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Code as a Weapon: A Consensus-Labeled Prompt Bank for Measuring Coding-Model Compliance with Malicious-Code Requests
Authors:
Richard J. Young,
Gregory D. Moody
Abstract:
A general-purpose language model that answers a harmful question returns text; a coding model that complies with a malicious request can return a working weapon: a keylogger, ransomware, an exploit that runs as written. This asymmetry in the severity of a single act of compliance implies coding-specialized models should clear a higher refusal bar than general-purpose chat models, not a lower one,…
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A general-purpose language model that answers a harmful question returns text; a coding model that complies with a malicious request can return a working weapon: a keylogger, ransomware, an exploit that runs as written. This asymmetry in the severity of a single act of compliance implies coding-specialized models should clear a higher refusal bar than general-purpose chat models, not a lower one, yet the field cannot tell whether they do. Refusal benchmarks for malicious code are fragmented: they mix requests for executable software with requests for harmful security knowledge and report refusal rates over non-comparable corpora. This paper's central result is that the CODE-versus-KNOWLEDGE classification axis established in a prior four-corpus release remains stable under a substantially expanded corpus pool and an independently refreshed judge panel, evidence that it measures a real construct rather than an artifact of the prompts or judges. Eight corpora spanning diverse elicitation paradigms (direct, jailbreak-decorated, indirect, and agent/interpreter: ASTRA, CySecBench, AdvBench/harmful_behaviors, JailbreakBench, MalwareBench, RedCode, RMCBench, Scam2Prompt) are classified under a five-judge consensus protocol (6,675 prompts x 5 judges = 33,375 calls), reaching Fleiss' kappa = 0.767 [95% CI 0.755, 0.777] ("substantial"). Critically, the panel shares no judge with the prior release (five paid commercial APIs replaced by five open-weight models from five vendors), yet the two panels agree on 94.45% of the 3,133 shared prompts and reach Cohen's kappa = 0.952 [0.942, 0.963] on the 3,031-prompt binary overlap: the axis survives near-total panel replacement. The released bank comprises 4,748 consensus-CODE and 1,923 consensus-KNOWLEDGE prompts, a reliability-quantified benchmark whose central classification axis is shown stable across corpus expansion and judge-panel replacement.
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Submitted 15 June, 2026; v1 submitted 27 May, 2026;
originally announced May 2026.
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Refusal Evaluation in Coding LLMs and Code Agents: A Systematic Review of Thirteen Malicious-Code Prompt Corpora (2023-2025)
Authors:
Richard J. Young,
Gregory D. Moody
Abstract:
The evaluation of large language model refusal on malicious-coding tasks now spans at least thirteen publicly released prompt corpora (AdvBench, the CyberSecEval family, RMCBench, RedCode, MCGMark, JailbreakBench, CySecBench, MalwareBench, CIRCLE, MOCHA, ASTRA, Scam2Prompt / Innoc2Scam-bench, and JAWS-Bench), each constructed under a different protocol, released under different licensing terms, an…
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The evaluation of large language model refusal on malicious-coding tasks now spans at least thirteen publicly released prompt corpora (AdvBench, the CyberSecEval family, RMCBench, RedCode, MCGMark, JailbreakBench, CySecBench, MalwareBench, CIRCLE, MOCHA, ASTRA, Scam2Prompt / Innoc2Scam-bench, and JAWS-Bench), each constructed under a different protocol, released under different licensing terms, and validated (or not) against different inter-rater reliability standards. Existing surveys treat code security, jailbreak taxonomy, or vulnerability detection as the central object and mention these corpora only in passing. This paper reverses that framing: it treats the prompt datasets themselves as the unit of analysis. Following a PRISMA-style protocol, we specify a search strategy, screen the recent literature on coding-LLM refusal evaluation, apply a uniform extraction template to each in-scope corpus, and synthesize the resulting catalogue along construction methodology, prompt-construction taxonomy (modality, turn structure, elicitation style), reproducibility and licensing, and malware-category coverage. The synthesis surfaces three recurring methodological gaps: the absence of human-annotator baselines against which LLM-judge labels can be calibrated, the absence of cross-corpus comparability with refusal-rate statistics measuring non-equivalent constructs, and the fragmentation of malware-category taxonomies, with no canonical schema spanning the thirteen in-scope corpora. The review concludes with proposed methodological directions for next-generation corpora, including pre-registration of inclusion criteria, vendor-diverse multi-judge validation, Fleiss' kappa with bootstrap CI as the reliability baseline, and a candidate canonical taxonomy.
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Submitted 19 May, 2026;
originally announced May 2026.
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A Wafer-Scale Heterogeneous III-V-on-Silicon Nitride Quantum Photonic Platform
Authors:
Lillian Thiel,
Boqiang Shen,
Jasper R. Venneberg,
Melissa A. Guidry,
Nic Arnaud,
Adam Slater,
Lucas Wang,
Xuefeng Li,
Josh Castro,
Yiming Pang,
Max Meunier,
Sahil D. Patel,
Yang Shen,
Theodore Morin,
Igor Kudelin,
Bowen Song,
Kaustubh Asawa,
John E. Bowers,
Kerry Vahala,
Nergis Mavalvala,
Xinghui Yin,
Steven Bowers,
Minh A. Tran,
Tin Komljenovic,
Galan Moody
Abstract:
Heterogeneous integration of gain and strongly nonlinear materials with ultra-low-loss silicon nitride (SiN) photonics offers a route to scalable quantum circuits, but concurrent wafer-scale manufacturability, low interlayer loss, and high performance have been challenging to realize. Here we demonstrate a wafer-scale III-V-on-SiN quantum photonic platform that directly integrates III-V layers to…
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Heterogeneous integration of gain and strongly nonlinear materials with ultra-low-loss silicon nitride (SiN) photonics offers a route to scalable quantum circuits, but concurrent wafer-scale manufacturability, low interlayer loss, and high performance have been challenging to realize. Here we demonstrate a wafer-scale III-V-on-SiN quantum photonic platform that directly integrates III-V layers to foundry-fabricated SiN circuits. The SiN layer provides 200-300 nm thick waveguides with $<1$ dB/m loss and a mature passive photonics ecosystem, while III-V materials provide large $χ^{\left(2\right)}$ and $χ^{\left(3\right)}$ nonlinearities for parametric gain, frequency conversion and quantum light generation. Adiabatic interlayer couplers yield $<25$ mdB loss to InGaP waveguides and resonators with intrinsic quality factors exceeding $10^6$, enabling $15\times$ brighter entanglement sources and efficient nonlinear conversion on SiN. Integrated components--including low-loss beam splitters, waveguide crossers, and tunable interferometers--are complemented by III-V lasers and InP photodetectors with amplifiers achieving up to $99^{+1}_{-12}\%$ quantum efficiency and $3$ GHz bandwidth. This architecture unites ultra-efficient sources, nonlinear elements and detectors on a wafer-scale, low-loss platform, establishing a path toward large-scale, low-noise quantum photonic systems.
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Submitted 17 May, 2026;
originally announced May 2026.
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High-Efficiency InGaP-on-Insulator Microresonator Nonlinear Conversion and Entanglement Generation
Authors:
Xuefeng Li,
Lillian Thiel,
Yiming Pang,
Amalu Shimamura,
Lucas Wang,
Joshua Castro,
Max Meunier,
Nicholas Lewis,
John Bowers,
Kevin Silverman,
Richard Mirin,
Galan Moody
Abstract:
InGaP-on-insulator (InGaP-OI), with its intrinsically high $χ^{\left(2\right)}$ optical nonlinearity, has emerged as an efficient and bright integrated photonic platform for frequency conversion and on-chip entanglement generation, but high waveguide propagation loss in the visible wavelength range has limited its overall performance. Here, we identify the dominant loss mechanism through mode-prof…
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InGaP-on-insulator (InGaP-OI), with its intrinsically high $χ^{\left(2\right)}$ optical nonlinearity, has emerged as an efficient and bright integrated photonic platform for frequency conversion and on-chip entanglement generation, but high waveguide propagation loss in the visible wavelength range has limited its overall performance. Here, we identify the dominant loss mechanism through mode-profile analysis and effectively mitigate the loss using a surface treatment method. Statistical analysis of the resonator quality factor and propagation loss reveals the optimal ring radius that maintains a strong nonlinear interaction while suppressing significant bending related loss, resulting in loss as low as 0.49 dB/cm (4.31 dB/cm) at 1560 nm (780 nm). The method provides a 3.5--4$\times$ quality factor enhancement at 780 nm, enabling a second-harmonic generation efficiency of $3.01\times10^{5}$ \,\%/\textrm{W} and a degenerate photon-pair generation rate of $4.27\,\textrm{MHz}/μ\textrm{W}$ and coincidence-to-accidental ratio as high as 10,000. The quasi-phase matching condition is experimentally verified, and nonlinear conversion is systematically characterized across the entire parameter space. This work establishes a scalable pathway for classical and quantum photonics in a low-loss, highly nonlinear, and wafer-scale integration platform.
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Submitted 15 August, 2026; v1 submitted 14 May, 2026;
originally announced May 2026.
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Electronic and Photonic Integration of Single Quantum Emitters in 2D Materials
Authors:
Sahil D. Patel,
Sean Doan,
Luka Jevremovic,
Kamyar Parto,
Galan Moody
Abstract:
Single-photon sources that are bright, pure, and interference-ready are essential for quantum communication and photonic quantum information processing, but many solid-state platforms still rely on bulky optical excitation, careful alignment, and post-selection to achieve useful linewidth, stability, and brightness. Scalable quantum photonics instead requires turnkey quantum-light engines that can…
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Single-photon sources that are bright, pure, and interference-ready are essential for quantum communication and photonic quantum information processing, but many solid-state platforms still rely on bulky optical excitation, careful alignment, and post-selection to achieve useful linewidth, stability, and brightness. Scalable quantum photonics instead requires turnkey quantum-light engines that can be triggered on demand, stabilized against environmental noise, and efficiently interfaced with fibers or photonic circuits. This review surveys recent progress in electronic and photonic integration of single quantum emitters in two-dimensional materials, focusing on localized excitonic emitters in transition metal dichalcogenides and defect-based color centers in hexagonal boron nitride. On the electronic side, we discuss electrical injection, fast modulation, electrostatic stabilization, and Stark tunability as routes to suppress blinking, spectral wandering, and charge-noise-induced broadening. On the photonic side, we review waveguide and resonator platforms that funnel emission into well-defined optical modes and, in some cases, enhance radiative rates through the Purcell effect. We connect these integration strategies to key source metrics, including single-photon purity, brightness, spectral stability, and photon indistinguishability. We conclude that the next stage of progress will depend on co-designed electronic and photonic architectures that jointly optimize on-demand operation, stabilization, tunability, and packaging-compatible optical interfacing.
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Submitted 7 May, 2026;
originally announced May 2026.
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A Validated Prompt Bank for Malicious Code Generation: Separating Executable Weapons from Security Knowledge in 1,554 Consensus-Labeled Prompts
Authors:
Richard J. Young,
Gregory D. Moody
Abstract:
Existing benchmarks of language-model refusal on malicious-coding tasks routinely conflate requests for executable malicious software with requests for harmful security knowledge. This conflation matters because the two request types plausibly trigger distinct refusal pathways in safety-aligned language models, and a single refusal-rate statistic computed over a mixture cannot isolate either. This…
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Existing benchmarks of language-model refusal on malicious-coding tasks routinely conflate requests for executable malicious software with requests for harmful security knowledge. This conflation matters because the two request types plausibly trigger distinct refusal pathways in safety-aligned language models, and a single refusal-rate statistic computed over a mixture cannot isolate either. This paper introduces a weapons-versus-knowledge classification axis, operationalized through a five-model consensus protocol, and applies it to 3,133 prompts drawn from four public benchmarks, yielding a 1,554-prompt consensus-CODE bank (the primary released artifact) and a 388-prompt consensus-KNOWLEDGE comparison set used by the companion benchmark paper. The consensus pipeline uses five large-language-model judges spanning four vendor families (Anthropic, OpenAI, Google, Zhipu AI, Alibaba), each issuing a binary CODE/KNOWLEDGE label per prompt under a three-of-five majority rule, with inter-rater reliability quantified by Fleiss' kappa with bootstrap 95% confidence intervals. Across all 3,133 prompts the five judges achieve kappa = 0.876 [95% CI: 0.862, 0.888], "almost perfect" agreement by the Landis & Koch convention, with 69.3% of prompts unanimous at five-of-five; all 3,133 prompts reached the 3-of-5 threshold, so the consensus pipeline produced zero ambiguity-excluded prompts. Whether the axis separates model behavior in practice is an empirical question this paper leaves to the companion benchmark study; the present contribution is the reliability-documented artifact and the case for treating the weapons-versus-knowledge distinction as the organizing axis of code-safety evaluation.
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Submitted 4 May, 2026;
originally announced May 2026.
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A Universal Quantum Information Preserving Photonic Switch for Scalable Quantum Networks
Authors:
Jiapeng Zhao,
Stéphane Vinet,
Amir Minoofar,
Michael Kilzer,
Lucas Wang,
Galan Moody,
Vijoy Pandey,
Ramana Kompella,
Reza Nejabati
Abstract:
Quantum networks are a keystone of the quantum internet. However, existing implementations remain largely confined to static point-to-point links due to the absence of a switching paradigm capable of dynamically routing fragile quantum entanglement without introducing decoherence. Here, we propose the Universal Quantum Switch, a foundational building block allowing on-demand, non-blocking, and enc…
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Quantum networks are a keystone of the quantum internet. However, existing implementations remain largely confined to static point-to-point links due to the absence of a switching paradigm capable of dynamically routing fragile quantum entanglement without introducing decoherence. Here, we propose the Universal Quantum Switch, a foundational building block allowing on-demand, non-blocking, and encoding-agnostic routing of quantum information, as well as seamless modality conversion between disparate quantum platforms. We develop a prototype in thin-film lithium niobate and experimentally demonstrate robust switching with $\le 4\%$ decoherence via thermo-optic modulation and high-speed electro-optic switching of arbitrary entangled states at 1 MHz. Moreover, we show that our platform can support reconfiguration speeds up to 1 GHz. To our knowledge, this work represents the first demonstration of multi-node dynamic entanglement distribution at these speeds. Complementing these experimental results, we project the architecture's scalability, showing dimension-independent decoherence, and provide a scalable, interoperable building block for heterogeneous quantum network fabrics.
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Submitted 23 April, 2026;
originally announced April 2026.
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Nonlinear integrated quantum photonics with AlGaAs
Authors:
F. Baboux,
G. Moody,
S. Ducci
Abstract:
Integrated photonics provides a powerful approach for developing compact, stable and scalable architectures for the generation, manipulation and detection of quantum states of light. To this end, several material platforms are being developed in parallel, each providing its specific assets, and hybridization techniques to combine their strengths are now possible. This review focuses on AlGaAs, a I…
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Integrated photonics provides a powerful approach for developing compact, stable and scalable architectures for the generation, manipulation and detection of quantum states of light. To this end, several material platforms are being developed in parallel, each providing its specific assets, and hybridization techniques to combine their strengths are now possible. This review focuses on AlGaAs, a III-V semiconductor platform combining a mature fabrication technology, direct band-gap compliant with electrical injection, low-loss operation, large electro-optic effect, and compatibility with superconducting detectors for on-chip detection. We detail recent implementations of room-temperature sources of quantum light based on the high second- and third-order optical nonlinearities of the material, as well as photonic circuits embedding various functionalities ranging from polarizing beamsplitters to Mach-Zehnder interferometers, modulators and tunable filters. We then present several realizations of quantum state engineering enabled by these recent advances and discuss open perspectives and remaining challenges in the field of integrated quantum photonics with AlGaAs.
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Submitted 11 February, 2026;
originally announced February 2026.
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High-Performance Near-Infrared Quantum Emission from Color Centers in hBN
Authors:
Sean Doan,
Sahil D. Patel,
Yilin Chen,
Jordan A. Gusdorff. Mark E. Turiansky,
Luis Villagomez,
Luka Jevremovic,
Nicholas Lewis,
Kenji Watanabe,
Takashi Taniguchi,
Lee C. Bassett,
Chris Van de Walle,
Galan Moody
Abstract:
Color centers hosted in hexagonal boron nitride have emerged as a highly promising platform for single-photon emission and spin-photon technologies relevant to quantum communication and quantum networking. As a wide-bandgap van der Waals material, hBN can host optically active quantum defects across a broad spectral range. Here, we demonstrate a simple and scalable oxygen-plasma process that repro…
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Color centers hosted in hexagonal boron nitride have emerged as a highly promising platform for single-photon emission and spin-photon technologies relevant to quantum communication and quantum networking. As a wide-bandgap van der Waals material, hBN can host optically active quantum defects across a broad spectral range. Here, we demonstrate a simple and scalable oxygen-plasma process that reproducibly creates single quantum emitters in hBN with blinking-free zero-phonon lines spanning the near-infrared from 700 up to 971 nm. These emitters combine MHz-level brightness, single-photon purity up to 99.9\%, and ultranarrow cryogenic linewidths down to 2.7~GHz under quasi-resonant excitation, placing them in a particularly attractive regime for quantum photonics. Photostability measurements further reveal resistance to photobleaching, sub-nm spectral stability over long timescales, and near-shot-noise-limited intensity fluctuations. Analysis of the phonon sidebands shows weak vibronic coupling and ZPL-dominated emission, with Debye--Waller factors approaching 50\%. Control experiments together with EDS elemental mapping support oxygen incorporation as a necessary ingredient in activating the NIR emitter population, while first-principles calculations identify O$_N$V$_N$ and O$_N$V$_N$H as the leading defect candidates. These results establish a high-performance NIR quantum-emitter platform in hBN for free-space quantum networking and future integrated quantum-photonic architectures.
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Submitted 23 April, 2026; v1 submitted 18 December, 2025;
originally announced December 2025.
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The Signalgate Case is Waiving a Red Flag to All Organizational and Behavioral Cybersecurity Leaders, Practitioners, and Researchers: Are We Receiving the Signal Amidst the Noise?
Authors:
Paul Benjamin Lowry,
Gregory D. Moody,
Robert Willison,
Clay Posey
Abstract:
The Signalgate incident of March 2025, wherein senior US national security officials inadvertently disclosed sensitive military operational details via the encrypted messaging platform Signal, highlights critical vulnerabilities in organizational security arising from human error, governance gaps, and the misuse of technology. Although smaller in scale when compared to historical breaches involvin…
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The Signalgate incident of March 2025, wherein senior US national security officials inadvertently disclosed sensitive military operational details via the encrypted messaging platform Signal, highlights critical vulnerabilities in organizational security arising from human error, governance gaps, and the misuse of technology. Although smaller in scale when compared to historical breaches involving billions of records, Signalgate illustrates critical systemic issues often overshadowed by a focus on external cyber threats. Employing a case-study approach and systematic review grounded in the NIST Cybersecurity Framework, we analyze the incident to identify patterns of human-centric vulnerabilities and governance challenges common to organizational security failures. Findings emphasize three critical points. (1) Organizational security depends heavily on human behavior, with internal actors often serving as the weakest link despite advanced technical defenses; (2) Leadership tone strongly influences organizational security culture and efficacy, and (3) widespread reliance on technical solutions without sufficient investments in human and organizational factors leads to ineffective practices and wasted resources. From these observations, we propose actionable recommendations for enhancing organizational and national security, including strong leadership engagement, comprehensive adoption of zero-trust architectures, clearer accountability structures, incentivized security behaviors, and rigorous oversight. Particularly during periods of organizational transition, such as mergers or large-scale personnel changes, additional measures become particularly important. Signalgate underscores the need for leaders and policymakers to reorient cybersecurity strategies toward addressing governance, cultural, and behavioral risks.
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Submitted 27 October, 2025; v1 submitted 8 September, 2025;
originally announced September 2025.
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Integrated magneto-optic based magnetometer: classical and quantum limits
Authors:
Paolo Pintus,
Heming Wang,
Sudharsanan Srinivasan,
Sergio Pinna,
Duanni Huang,
Yuya Shoji,
Caroline A. Ross,
John E. Bowers,
Galan Moody
Abstract:
Magnetic field sensors with high sensitivity and spatial resolution have profoundly impacted diverse applications ranging from geo-positioning and navigation to medical imaging, materials science, and space exploration. However, the use of high-precision magnetometers is often limited due to their bulky size or low energy efficiency. In this work, we present the design, modeling and an experimenta…
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Magnetic field sensors with high sensitivity and spatial resolution have profoundly impacted diverse applications ranging from geo-positioning and navigation to medical imaging, materials science, and space exploration. However, the use of high-precision magnetometers is often limited due to their bulky size or low energy efficiency. In this work, we present the design, modeling and an experimental demonstration of an all-optical magnetometer based on silicon integrated photonics heterogeneously integrated with a magneto-optic thin film. By bonding a thin cerium-yttrium iron garnet layer onto an integrated silicon photonic interferometer, small magnetic field fluctuations can be detected through the non-reciprocal phase shift in the sensor. This strategy enables more than 80 dB of dynamic range with better than 40~pT/$\sqrt{\text{Hz}}$ sensitivity at room temperature. Importantly, by leveraging silicon photonics, the core platform is scalable through foundry manufacturing, and the ultra-low power requirements enable complete system integration with on-chip lasers, detectors, and quantum elements for enhanced sensitivity. This work provides a path to realizing a compact, scalable, room temperature magnetometer based on integrated photonic systems, opening new opportunities for ultra-sensitive and ultra-efficient magnetic field detectors.
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Submitted 21 August, 2025;
originally announced August 2025.
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Microscopic Theory of Squeezed Light in Quantum Dot Systems
Authors:
Sahil Patel,
Sean Doan,
Chen Shang,
Frederic Grillot,
Frank Jahnke,
John Bowers,
Galan Moody,
Weng Chow
Abstract:
We present a cavity-QED theory for generating squeezed light from semiconductor quantum dots (QDs) integrated in microcavities. We formulate equations of motion for an inhomogeneously broadened QD ensemble that is incoherently pumped and simultaneously driven by a coherent seed field, solve for steady states, and compute the output-field quadrature variances. The analysis identifies operating cond…
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We present a cavity-QED theory for generating squeezed light from semiconductor quantum dots (QDs) integrated in microcavities. We formulate equations of motion for an inhomogeneously broadened QD ensemble that is incoherently pumped and simultaneously driven by a coherent seed field, solve for steady states, and compute the output-field quadrature variances. The analysis identifies operating conditions that yield amplitude-quadrature squeezing, with photon-number fluctuations reduced below the coherent-state limit and squeezing levels as large as 5 dB attainable with presently accessible QD and cavity parameters using only ~ 1 uW pump power. We further show that quantum correlations originating from four-wave mixing play a dual role: they both shape the gain spectrum and generate squeezing. These correlations constitute the quantum counterpart of the mean-field (semiclassical) mechanisms responsible for self-mode-locking in QD lasers and the ultra-narrow lasing linewidths achieved under self-injection locking.
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Submitted 20 August, 2025;
originally announced August 2025.
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Increasing single-photon production with cavity-QED
Authors:
Chen Shang,
Weng W. Chow,
Galan Moody,
John E. Bowers
Abstract:
A study was performed to determine the extent cavity enhancement may increase single-photon production while maintaining single-photon purity. It was found that certain combinations of cavity lifetime and light-matter coupling strength can lead to carrier-photon correlations that increase single-photon generation rate while maintaining low 2nd order photon correlation. This study provides guidance…
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A study was performed to determine the extent cavity enhancement may increase single-photon production while maintaining single-photon purity. It was found that certain combinations of cavity lifetime and light-matter coupling strength can lead to carrier-photon correlations that increase single-photon generation rate while maintaining low 2nd order photon correlation. This study provides guidance for future emitter-cavity design to achieve high purity and ultrafast single photon generation.
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Submitted 26 June, 2025;
originally announced June 2025.
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Characterization of Chromium Impurities in $β$-Ga$_2$O$_3$
Authors:
Mark E. Turiansky,
Sai Mu,
Lukas Razinkovas,
Kamyar Parto,
Sahil D. Patel,
Sean Doan,
Ganesh Pokharel,
Steven J. Gomez Alvarado,
Stephen D. Wilson,
Galan Moody,
Chris G. Van de Walle
Abstract:
Chromium is a common transition-metal impurity that is easily incorporated during crystal growth. It is perhaps best known for giving rise to the 694.3 nm (1.786 eV) emission in Cr-doped Al$_2$O$_3$, exploited in ruby lasers. Chromium has also been found in monoclinic gallium oxide, a wide-bandgap semiconductor being pursued for power electronics. In this work, we thoroughly characterize the behav…
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Chromium is a common transition-metal impurity that is easily incorporated during crystal growth. It is perhaps best known for giving rise to the 694.3 nm (1.786 eV) emission in Cr-doped Al$_2$O$_3$, exploited in ruby lasers. Chromium has also been found in monoclinic gallium oxide, a wide-bandgap semiconductor being pursued for power electronics. In this work, we thoroughly characterize the behavior of Cr in Ga$_2$O$_3$ through theoretical and experimental techniques. $β$-Ga$_2$O$_3$ samples are grown with the floating zone method and show evidence of a sharp photoluminescence signal, reminiscent of ruby. We calculate the energetics of formation of Cr from first principles, demonstrating that Cr preferentially incorporates as a neutral impurity on the octahedral site. Cr possesses a quartet ground-state spin and has an internal transition with a zero-phonon line near 1.8 eV. By comparing the calculated and experimentally measured luminescence lineshape function, we elucidate the role of coupling to phonons and uncover features beyond the Franck-Condon approximation. The combination of strong emission with a small Huang-Rhys factor of 0.05 and a technologically relevant host material render Cr in Ga$_2$O$_3$ attractive as a quantum defect.
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Submitted 31 December, 2024;
originally announced January 2025.
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A Versatile Chip-Scale Platform for High-Rate Entanglement Generation using an AlGaAs Microresonator Array
Authors:
Yiming Pang,
Joshua E. Castro,
Trevor J. Steiner,
Liao Duan,
Noemi Tagliavacche,
Massimo Borghi,
Lillian Thiel,
Nicholas Lewis,
John E. Bowers,
Marco Liscidini,
Galan Moody
Abstract:
Integrated photonic microresonators have become an essential resource for generating photonic qubits for quantum information processing, entanglement distribution and networking, and quantum communications. The pair generation rate is enhanced by reducing the microresonator radius, but this comes at the cost of increasing the frequency mode spacing and reducing the quantum information spectral den…
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Integrated photonic microresonators have become an essential resource for generating photonic qubits for quantum information processing, entanglement distribution and networking, and quantum communications. The pair generation rate is enhanced by reducing the microresonator radius, but this comes at the cost of increasing the frequency mode spacing and reducing the quantum information spectral density. Here, we circumvent this rate-density trade-off in an AlGaAs-on-insulator photonic device by multiplexing an array of 20 small-radius microresonators each producing a 650-GHz-spaced comb of time-energy entangled-photon pairs. The resonators can be independently tuned via integrated thermo-optic heaters, enabling control of the mode spacing from degeneracy up to a full free spectral range. We demonstrate simultaneous pumping of five resonators with up to $50$ GHz relative comb offsets, where each resonator produces pairs exhibiting time-energy entanglement visibilities up to 95$\%$, coincidence-to-accidental ratios exceeding 5,000, and an on-chip pair rate up to 2.6 GHz/mW$^2$ per comb line -- more than 40 times improvement over prior work. As a demonstration, we generate frequency-bin qubits in a maximally entangled two-qubit Bell state with fidelity exceeding 87$\%$ (90$\%$ with background correction) and detected frequency-bin entanglement rates up to 7 kHz ($\sim 70$ MHz on-chip pair rate) using $\sim 250$ $μ$W pump power. Multiplexing small-radius microresonators combines the key capabilities required for programmable and dense photonic qubit encoding while retaining high pair-generation rates, heralded single-photon purity, and entanglement fidelity.
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Submitted 20 December, 2024;
originally announced December 2024.
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Photon pair generation via down-conversion in III-V semiconductor microrings: modal dispersion and quasi-phase matching
Authors:
Samuel E. Fontaine,
Colin Vendromin,
Trevor J. Steiner,
Amirali Atrli,
Lillian Thiel,
Joshua Castro,
Galan Moody,
John Bowers,
Marco Liscidini,
J. E. Sipe
Abstract:
We explore how III-V semiconductor microring resonators can efficiently generate photon pairs and squeezed vacuum states via spontaneous parametric down-conversion by utilizing their built-in quasi phase matching and modal dispersion. We present an analytic expression for the biphoton wave function of photon pairs generated by weak pump pulses, and characterize the squeezed states that result unde…
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We explore how III-V semiconductor microring resonators can efficiently generate photon pairs and squeezed vacuum states via spontaneous parametric down-conversion by utilizing their built-in quasi phase matching and modal dispersion. We present an analytic expression for the biphoton wave function of photon pairs generated by weak pump pulses, and characterize the squeezed states that result under stronger pumping conditions. Our model includes loss, and captures the statistics of the scattered photons. A detailed sample calculation shows that for low pump powers conversion efficiencies of 10$^{-5}$, corresponding to a rate of $39$ MHz for a pump power of 1 $μ$W, are attainable for rudimentary structures such as a simple microring coupled to a waveguide, in both the continuous wave and pulsed excitation regimes. Our results suggest that high levels of squeezing and pump depletion are attainable, possibly leading to the deterministic generation of non-Gaussian states.
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Submitted 10 February, 2025; v1 submitted 12 September, 2024;
originally announced September 2024.
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Integrated Mode-Hop-Free Tunable Lasers at 780 nm for Chip-Scale Classical and Quantum Photonic Applications
Authors:
Joshua E. Castro,
Eber Nolasco-Martinez,
Paolo Pintus,
Zeyu Zhang,
Boqiang Shen,
Theodore Morin,
Lillian Thiel,
Trevor J. Steiner,
Nicholas Lewis,
Sahil D. Patel,
John E. Bowers,
David M. Weld,
Galan Moody
Abstract:
In the last decade, remarkable advances in integrated photonic technologies have enabled table-top experiments and instrumentation to be scaled down to compact chips with significant reduction in size, weight, power consumption, and cost. Here, we demonstrate an integrated continuously tunable laser in a heterogeneous gallium arsenide-on-silicon nitride (GaAs-on-SiN) platform that emits in the far…
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In the last decade, remarkable advances in integrated photonic technologies have enabled table-top experiments and instrumentation to be scaled down to compact chips with significant reduction in size, weight, power consumption, and cost. Here, we demonstrate an integrated continuously tunable laser in a heterogeneous gallium arsenide-on-silicon nitride (GaAs-on-SiN) platform that emits in the far-red radiation spectrum near 780 nm, with 20 nm tuning range, <6 kHz intrinsic linewidth, and a >40 dB side-mode suppression ratio. The GaAs optical gain regions are heterogeneously integrated with low-loss SiN waveguides. The narrow linewidth lasing is achieved with an extended cavity consisting of a resonator-based Vernier mirror and a phase shifter. Utilizing synchronous tuning of the integrated heaters, we show mode-hop-free wavelength tuning over a range larger than 100 GHz (200 pm). To demonstrate the potential of the device, we investigate two illustrative applications: (i) the linear characterization of a silicon nitride microresonator designed for entangled-photon pair generation, and (ii) the absorption spectroscopy and locking to the D1 and D2 transition lines of 87-Rb. The performance of the proposed integrated laser holds promise for a broader spectrum of both classical and quantum applications in the visible range, encompassing communication, control, sensing, and computing.
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Submitted 22 July, 2024;
originally announced July 2024.
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Broadband Entangled-Photon Pair Generation with Integrated Photonics: Guidelines and A Materials Comparison
Authors:
Liao Duan,
Trevor J. Steiner,
Paolo Pintus,
Lillian Thiel,
Joshua E. Castro,
John E. Bowers,
Galan Moody
Abstract:
Correlated photon-pair sources are key components for quantum computing, networking, and sensing applications. Integrated photonics has enabled chip-scale sources using nonlinear processes, producing high-rate entanglement with sub-100 microwatt power at telecom wavelengths. Many quantum systems operate in the visible or near-infrared ranges, necessitating broadband visible-telecom entangled-pair…
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Correlated photon-pair sources are key components for quantum computing, networking, and sensing applications. Integrated photonics has enabled chip-scale sources using nonlinear processes, producing high-rate entanglement with sub-100 microwatt power at telecom wavelengths. Many quantum systems operate in the visible or near-infrared ranges, necessitating broadband visible-telecom entangled-pair sources for connecting remote systems via entanglement swapping and teleportation. This study evaluates broadband entanglement generation through spontaneous four-wave mixing in various nonlinear integrated photonic materials, including silicon nitride, lithium niobate, aluminum gallium arsenide, indium gallium phosphide, and gallium nitride. We demonstrate how geometric dispersion engineering facilitates phase-matching for each platform and reveals unexpected results, such as robust designs to fabrication variations and a Type-1 cross-polarized phase-matching condition for III-V materials that expands the operational bandwidth. With experimentally attainable parameters, integrated photonic microresonators with optimized designs can achieve pair generation rates greater than ~1 THz/mW$^2$.
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Submitted 5 July, 2024;
originally announced July 2024.
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Wafer-Scale Fabrication of InGaP-on-Insulator for Nonlinear and Quantum Photonic Applications
Authors:
Lillian Thiel,
Joshua E. Castro,
Trevor J. Steiner,
Catherine L. Nguyen,
Audrey Pechilis,
Liao Duan,
Nicholas Lewis,
Garrett D. Cole,
John E. Bowers,
Galan Moody
Abstract:
The development of manufacturable and scalable integrated nonlinear photonic materials is driving key technologies in diverse areas such as high-speed communications, signal processing, sensing, and quantum information. Here, we demonstrate a novel nonlinear platform -- InGaP-on-insulator -- optimized for visible-to-telecommunication wavelength $χ^{\left(2\right)}$ nonlinear optical processes. In…
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The development of manufacturable and scalable integrated nonlinear photonic materials is driving key technologies in diverse areas such as high-speed communications, signal processing, sensing, and quantum information. Here, we demonstrate a novel nonlinear platform -- InGaP-on-insulator -- optimized for visible-to-telecommunication wavelength $χ^{\left(2\right)}$ nonlinear optical processes. In this work, we detail our 100-mm wafer-scale InGaP-on-insulator fabrication process realized via wafer bonding, optical lithography, and dry-etching techniques. The resulting wafers yield 1000s of components in each fabrication cycle, with initial designs that include chip-to-fiber couplers, 12.5-cm-long nested spiral waveguides, and arrays of microring resonators with free-spectral ranges spanning 400-900 GHz. We demonstrate intrinsic resonator quality factors as high as 324,000 (440,000) for single-resonance (split-resonance) modes near 1550 nm corresponding to 1.56 dB cm$^{-1}$ (1.22 dB cm$^{-1}$) propagation loss. We analyze the loss versus waveguide width and resonator radius to establish the operating regime for optimal 775-to-1550 nm phase matching. By combining the high $χ^{\left(2\right)}$ and $χ^{\left(3\right)}$ optical nonlinearity of InGaP with wafer-scale fabrication and low propagation loss, these results open promising possibilities for entangled-photon, multi-photon, and squeezed light generation.
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Submitted 26 June, 2024;
originally announced June 2024.
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Rational Design of Efficient Defect-Based Quantum Emitters
Authors:
Mark E. Turiansky,
Kamyar Parto,
Galan Moody,
Chris G. Van de Walle
Abstract:
Single-photon emitters are an essential component of quantum networks, and defects or impurities in semiconductors are a promising platform to realize such quantum emitters. Here we present a model that encapsulates the essential physics of coupling to phonons, which governs the behavior of real single-photon emitters, and critically evaluate several approximations that are commonly utilized. Emis…
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Single-photon emitters are an essential component of quantum networks, and defects or impurities in semiconductors are a promising platform to realize such quantum emitters. Here we present a model that encapsulates the essential physics of coupling to phonons, which governs the behavior of real single-photon emitters, and critically evaluate several approximations that are commonly utilized. Emission in the telecom wavelength range is highly desirable, but our model shows that nonradiative processes are greatly enhanced at these low photon energies, leading to a decrease in efficiency. Our results suggest that reducing the phonon frequency is a fruitful avenue to enhance the efficiency.
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Submitted 13 February, 2024;
originally announced February 2024.
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Continuous Entanglement Distribution from an AlGaAs-on-Insulator Microcomb for Quantum Communications
Authors:
Trevor J. Steiner,
Maximilian Shen,
Joshua E. Castro,
John E. Bowers,
Galan Moody
Abstract:
Using an aluminum gallium arsenide microring resonator, we demonstrate a bright quantum optical microcomb with $>300$ nm bandwidth and more than 20 sets of time-energy entangled modes, enabling spectral demultiplexing with simple, off-the-shelf commercial telecom components. We report high-rate continuous entanglement distribution for two sets of entangled-photon pair frequency modes exhibiting up…
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Using an aluminum gallium arsenide microring resonator, we demonstrate a bright quantum optical microcomb with $>300$ nm bandwidth and more than 20 sets of time-energy entangled modes, enabling spectral demultiplexing with simple, off-the-shelf commercial telecom components. We report high-rate continuous entanglement distribution for two sets of entangled-photon pair frequency modes exhibiting up to $20$ GHz/mW$^2$ pair generation rate. As an illustrative example of entanglement distribution, we perform a continuous-wave time-bin quantum key distribution protocol with 8 kbps raw key rates while maintaining less than 10$\%$ error rate and sufficient two-photon visibility to ensure security of the channel. When the $>$20 frequency modes are multiplexed, we estimate $>$100 kbps entanglement-based key rates or the creation of a multi-user quantum communications network. The entire system requires less than 110 $μ$W of on-chip optical power, demonstrating an efficient source of entangled frequency modes for quantum communications. As a proof of principle, a quantum key is distributed across 12 km of deployed fiber on the UCSB campus and used to transmit a 21 kB image with $<9\%$ error.
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Submitted 21 October, 2023;
originally announced October 2023.
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Heterogeneous integration of superconducting thin films and epitaxial semiconductor heterostructures with Lithium Niobate
Authors:
Michelle Lienhart,
Michael Choquer,
Emeline D. S. Nysten,
Matthias Weiß,
Kai Müller,
Jonathan J. Finley,
Galan Moody,
Hubert J. Krenner
Abstract:
We report on scalable heterointegration of superconducting electrodes and epitaxial semiconductor quantum dots on strong piezoelectric and optically nonlinear lithium niobate. The implemented processes combine the sputter-deposited thin film superconductor niobium nitride and III-V compound semiconductor membranes onto the host substrate. The superconducting thin film is employed as a zero-resisti…
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We report on scalable heterointegration of superconducting electrodes and epitaxial semiconductor quantum dots on strong piezoelectric and optically nonlinear lithium niobate. The implemented processes combine the sputter-deposited thin film superconductor niobium nitride and III-V compound semiconductor membranes onto the host substrate. The superconducting thin film is employed as a zero-resistivity electrode material for a surface acoustic wave resonator with internal quality factors $Q \approx 17000$ representing a three-fold enhancement compared to identical devices with normal conducting electrodes. Superconducting operation of $\approx 400\,\mathrm{MHz}$ resonators is achieved to temperatures $T>7\,\mathrm{K}$ and electrical radio frequency powers $P_{\mathrm{rf}}>+9\,\mathrm{dBm}$. Heterogeneously integrated single quantum dots couple to the resonant phononic field of the surface acoustic wave resonator operated in the superconducting regime. Position and frequency selective coupling mediated by deformation potential coupling is validated using time-integrated and time-resolved optical spectroscopy. Furthermore, acoustoelectric charge state control is achieved in a modified device geometry harnessing large piezoelectric fields inside the resonator. The hybrid quantum dot - surface acoustic wave resonator can be scaled to higher operation frequencies and smaller mode volumes for quantum phase modulation and transduction between photons and phonons via the quantum dot. Finally, the employed materials allow for the realization of other types of optoelectronic devices, including superconducting single photon detectors and integrated photonic and phononic circuits.
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Submitted 30 April, 2023; v1 submitted 6 February, 2023;
originally announced February 2023.
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Surface Acoustic Wave Cavity Optomechanics with WSe$_2$ Single Photon Emitters
Authors:
Sahil D. Patel,
Kamyar Parto,
Michael Choquer,
Sammy Umezawa,
Landon Hellman,
Daniella Polishchuk,
Galan Moody
Abstract:
Surface acoustic waves (SAWs) are a versatile tool for coherently interfacing with a variety of solid-state quantum systems spanning microwave to optical frequencies, including superconducting qubits, spins, and quantum emitters. Here, we demonstrate SAW cavity optomechanics with quantum emitters in 2D materials, specifically monolayer WSe$_2$, on a planar lithium niobate SAW resonator driven by s…
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Surface acoustic waves (SAWs) are a versatile tool for coherently interfacing with a variety of solid-state quantum systems spanning microwave to optical frequencies, including superconducting qubits, spins, and quantum emitters. Here, we demonstrate SAW cavity optomechanics with quantum emitters in 2D materials, specifically monolayer WSe$_2$, on a planar lithium niobate SAW resonator driven by superconducting electronics. Using steady-state photoluminescence spectroscopy and time-resolved single-photon counting, we map the temporal dynamics of modulated 2D emitters under coupling to different SAW cavity modes, showing energy-level splitting consistent with deformation potential coupling of 30 meV/%. We leverage the large anisotropic strain from the SAW to modulate the excitonic fine-structure splitting on a nanosecond timescale, which may find applications for on-demand entangled photon-pair generation from 2D materials. Cavity optomechanics with SAWs and 2D quantum emitters provides opportunities for compact sensors and quantum electro-optomechanics in a multi-functional integrated platform that combines phononic, optical, and superconducting electronic quantum systems.
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Submitted 28 November, 2022;
originally announced November 2022.
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Cavity-Enhanced 2D Material Quantum Emitters Deterministically Integrated with Silicon Nitride Microresonators
Authors:
Kamyar Parto,
Shaimaa I. Azzam,
Nicholas Lewis,
Sahil D. Patel,
Sammy Umezawa,
Kenji Watanabe,
Takashi Taniguchi,
Galan Moody
Abstract:
Optically active defects in 2D materials, such as hexagonal boron nitride (hBN) and transition metal dichalcogenides (TMDs), are an attractive class of single-photon emitters with high brightness, room-temperature operation, site-specific engineering of emitter arrays, and tunability with external strain and electric fields. In this work, we demonstrate a novel approach to precisely align and embe…
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Optically active defects in 2D materials, such as hexagonal boron nitride (hBN) and transition metal dichalcogenides (TMDs), are an attractive class of single-photon emitters with high brightness, room-temperature operation, site-specific engineering of emitter arrays, and tunability with external strain and electric fields. In this work, we demonstrate a novel approach to precisely align and embed hBN and TMDs within background-free silicon nitride microring resonators. Through the Purcell effect, high-purity hBN emitters exhibit a cavity-enhanced spectral coupling efficiency up to $46\%$ at room temperature, which exceeds the theoretical limit for cavity-free waveguide-emitter coupling and previous demonstrations by nearly an order-of-magnitude. The devices are fabricated with a CMOS-compatible process and exhibit no degradation of the 2D material optical properties, robustness to thermal annealing, and 100 nm positioning accuracy of quantum emitters within single-mode waveguides, opening a path for scalable quantum photonic chips with on-demand single-photon sources.
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Submitted 29 June, 2022;
originally announced June 2022.
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Expanding the Quantum Photonic Toolbox in AlGaAsOI
Authors:
Joshua E. Castro,
Trevor J. Steiner,
Lillian Thiel,
Alex Dinkelacker,
Corey McDonald,
Paolo Pintus,
Lin Chang,
John E. Bowers,
Galan Moody
Abstract:
Aluminum gallium arsenide-on-insulator (AlGaAsOI) exhibits large $χ^\left(2\right)$ and $χ^\left(3\right)$ optical nonlinearities, a wide tunable bandgap, low waveguide propagation loss, and a large thermo-optic coefficient, making it an exciting platform for integrated quantum photonics. With ultrabright sources of quantum light established in AlGaAsOI, the next step is to develop the critical bu…
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Aluminum gallium arsenide-on-insulator (AlGaAsOI) exhibits large $χ^\left(2\right)$ and $χ^\left(3\right)$ optical nonlinearities, a wide tunable bandgap, low waveguide propagation loss, and a large thermo-optic coefficient, making it an exciting platform for integrated quantum photonics. With ultrabright sources of quantum light established in AlGaAsOI, the next step is to develop the critical building blocks for chip-scale quantum photonic circuits. Here we expand the quantum photonic toolbox for AlGaAsOI by demonstrating edge couplers, 3-dB splitters, tunable interferometers, and waveguide crossings with performance comparable to or exceeding silicon and silicon-nitride quantum photonic platforms. As a demonstration, we demultiplex photonic qubits through an unbalanced interferometer, paving the route toward ultra-efficient and high-rate chip-scale demonstrations of photonic quantum computation and information applications.
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Submitted 13 May, 2022;
originally announced May 2022.
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Prospects and challenges of quantum emitters in 2D materials
Authors:
Shaimaa I. Azzam,
Kamyar Parto,
Galan Moody
Abstract:
The search for an ideal single-photon source has generated significant interest in discovering novel emitters in materials as well as developing new manipulation techniques to gain better control over the emitters' properties. Quantum emitters in atomically thin two-dimensional (2D) materials have proven very attractive with high brightness, operation under ambient conditions, and the ability to b…
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The search for an ideal single-photon source has generated significant interest in discovering novel emitters in materials as well as developing new manipulation techniques to gain better control over the emitters' properties. Quantum emitters in atomically thin two-dimensional (2D) materials have proven very attractive with high brightness, operation under ambient conditions, and the ability to be integrated with a wide range of electronic and photonic platforms. This perspective highlights some of the recent advances in quantum light generation from 2D materials, focusing on hexagonal boron nitride and transition metal dichalcogenides (TMDs). Efforts in engineering and deterministically creating arrays of quantum emitters in 2D materials, their electrical excitation, and their integration with photonic devices are discussed. Lastly, we address some of the challenges the field is facing and the near-term efforts to tackle them. We provide an outlook towards efficient and scalable quantum light generation from 2D materials towards controllable and addressable on-chip quantum sources.
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Submitted 14 April, 2021;
originally announced April 2021.
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Roadmap on Integrated Quantum Photonics
Authors:
Galan Moody,
Volker J. Sorger,
Daniel J. Blumenthal,
Paul W. Juodawlkis,
William Loh,
Cheryl Sorace-Agaskar,
Alex E. Jones,
Krishna C. Balram,
Jonathan C. F. Matthews,
Anthony Laing,
Marcelo Davanco,
Lin Chang,
John E. Bowers,
Niels Quack,
Christophe Galland,
Igor Aharonovich,
Martin A. Wolff,
Carsten Schuck,
Neil Sinclair,
Marko Lončar,
Tin Komljenovic,
David Weld,
Shayan Mookherjea,
Sonia Buckley,
Marina Radulaski
, et al. (30 additional authors not shown)
Abstract:
Integrated photonics is at the heart of many classical technologies, from optical communications to biosensors, LIDAR, and data center fiber interconnects. There is strong evidence that these integrated technologies will play a key role in quantum systems as they grow from few-qubit prototypes to tens of thousands of qubits. The underlying laser and optical quantum technologies, with the required…
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Integrated photonics is at the heart of many classical technologies, from optical communications to biosensors, LIDAR, and data center fiber interconnects. There is strong evidence that these integrated technologies will play a key role in quantum systems as they grow from few-qubit prototypes to tens of thousands of qubits. The underlying laser and optical quantum technologies, with the required functionality and performance, can only be realized through the integration of these components onto quantum photonic integrated circuits (QPICs) with accompanying electronics. In the last decade, remarkable advances in quantum photonic integration and a dramatic reduction in optical losses have enabled benchtop experiments to be scaled down to prototype chips with improvements in efficiency, robustness, and key performance metrics. The reduction in size, weight, power, and improvement in stability that will be enabled by QPICs will play a key role in increasing the degree of complexity and scale in quantum demonstrations. In the next decade, with sustained research, development, and investment in the quantum photonic ecosystem (i.e. PIC-based platforms, devices and circuits, fabrication and integration processes, packaging, and testing and benchmarking), we will witness the transition from single- and few-function prototypes to the large-scale integration of multi-functional and reconfigurable QPICs that will define how information is processed, stored, transmitted, and utilized for quantum computing, communications, metrology, and sensing. This roadmap highlights the current progress in the field of integrated quantum photonics, future challenges, and advances in science and technology needed to meet these challenges.
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Submitted 22 September, 2021; v1 submitted 5 February, 2021;
originally announced February 2021.
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Ultra-bright entangled-photon pair generation from an AlGaAs-on-insulator microring resonator
Authors:
Trevor J. Steiner,
Joshua E. Castro,
Lin Chang,
Quynh Dang,
Weiqiang Xie,
Justin Norman,
John E. Bowers,
Galan Moody
Abstract:
Entangled-photon pairs are an essential resource for quantum information technologies. Chip-scale sources of entangled pairs have been integrated with various photonic platforms, including silicon, nitrides, indium phosphide, and lithium niobate, but each has fundamental limitations that restrict the photon-pair brightness and quality, including weak optical nonlinearity or high waveguide loss. He…
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Entangled-photon pairs are an essential resource for quantum information technologies. Chip-scale sources of entangled pairs have been integrated with various photonic platforms, including silicon, nitrides, indium phosphide, and lithium niobate, but each has fundamental limitations that restrict the photon-pair brightness and quality, including weak optical nonlinearity or high waveguide loss. Here, we demonstrate a novel, ultra-low-loss AlGaAs-on-insulator platform capable of generating time-energy entangled photons in a $Q$ $>1$ million microring resonator with nearly 1,000-fold improvement in brightness compared to existing sources. The waveguide-integrated source exhibits an internal generation rate greater than $20\times 10^9$ pairs sec$^{-1}$ mW$^{-2}$, emits near 1550 nm, produces heralded single photons with $>99\%$ purity, and violates Bell's inequality by more than 40 standard deviations with visibility $>97\%$. Combined with the high optical nonlinearity and optical gain of AlGaAs for active component integration, these are all essential features for a scalable quantum photonic platform.
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Submitted 28 September, 2020;
originally announced September 2020.
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Irradiation of Nanostrained Monolayer WSe$_2$ for Site-Controlled Single-Photon Emission up to 150 K
Authors:
Kamyar Parto,
Kaustav Banerjee,
Galan Moody
Abstract:
Quantum-dot-like WSe$_2$ single-photon emitters have become a promising platform for future on-chip scalable quantum light sources with unique advantages over existing technologies, notably the potential for site-specific engineering. However, the required cryogenic temperatures for the functionality of these sources have been an inhibitor of their full potential. Existing strain engineering metho…
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Quantum-dot-like WSe$_2$ single-photon emitters have become a promising platform for future on-chip scalable quantum light sources with unique advantages over existing technologies, notably the potential for site-specific engineering. However, the required cryogenic temperatures for the functionality of these sources have been an inhibitor of their full potential. Existing strain engineering methods face fundamental challenges in extending the working temperature while maintaining the emitter's fabrication yield and purity. In this work, we demonstrate a novel method of designing site-specific single-photon emitters in atomically thin WSe$_2$ with near-unity yield utilizing independent and simultaneous strain engineering via nanoscale stressors and defect engineering via electron-beam irradiation. Many of these emitters exhibit exciton-biexciton cascaded emission, purities above 95%, and working temperatures extending up to 150 K, which is the highest observed in van der Waals semiconductor single-photon emitters without Purcell enhancement. This methodology, coupled with possible plasmonic or optical micro-cavity integration, potentially furthers the realization of future scalable, room-temperature, and high-quality van der Waals quantum light sources.
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Submitted 15 September, 2020;
originally announced September 2020.
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Fast phase cycling in non-collinear optical two-dimensional coherent spectroscopy
Authors:
Maria F. Munoz,
Adam Medina,
Travis M. Autry,
Galan Moody,
Mark E. Siemens,
Alan D. Bristow,
Steven T. Cundiff,
Hebin Li
Abstract:
As optical two-dimensional coherent spectroscopy (2DCS) is extended to a broader range of applications, it is critical to improve the detection sensitivity of optical 2DCS. We developed a fast phase-cycling scheme in a non-collinear optical 2DCS implementation by using liquid crystal phase retarders to modulate the phases of two excitation pulses. The background in the signal can be eliminated by…
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As optical two-dimensional coherent spectroscopy (2DCS) is extended to a broader range of applications, it is critical to improve the detection sensitivity of optical 2DCS. We developed a fast phase-cycling scheme in a non-collinear optical 2DCS implementation by using liquid crystal phase retarders to modulate the phases of two excitation pulses. The background in the signal can be eliminated by combining either two or four interferograms measured with a proper phase configuration. The effectiveness of this method was validated in optical 2DCS measurements of an atomic vapor. This fast phase-cycling scheme will enable optical 2DCS in novel emerging applications that require enhanced detection sensitivity.
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Submitted 18 August, 2020;
originally announced August 2020.
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Twist Angle Dependent Interlayer Exciton Lifetimes in van der Waals Heterostructures
Authors:
Junho Choi,
Matthias Florian,
Alexander Steinhoff,
Daniel Erben,
Kha Tran,
Dong Seob Kim,
Liuyang Sun,
Jiamin Quan,
Robert Claassen,
Somak Majumder,
Jennifer A. Hollingsworth,
Takashi Taniguchi,
Kenji Watanabe,
Keiji Ueno,
Akshay Singh,
Galan Moody,
Frank Jahnke,
Xiaoqin Li
Abstract:
In van der Waals (vdW) heterostructures formed by stacking two monolayers of transition metal dichalcogenides, multiple exciton resonances with highly tunable properties are formed and subject to both vertical and lateral confinement. We investigate how a unique control knob, the twist angle between the two monolayers, can be used to control the exciton dynamics. We observe that the interlayer exc…
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In van der Waals (vdW) heterostructures formed by stacking two monolayers of transition metal dichalcogenides, multiple exciton resonances with highly tunable properties are formed and subject to both vertical and lateral confinement. We investigate how a unique control knob, the twist angle between the two monolayers, can be used to control the exciton dynamics. We observe that the interlayer exciton lifetimes in $\text{MoSe}_{\text{2}}$/$\text{WSe}_{\text{2}}$ twisted bilayers (TBLs) change by one order of magnitude when the twist angle is varied from 1$^\circ$ to 3.5$^\circ$. Using a low-energy continuum model, we theoretically separate two leading mechanisms that influence interlayer exciton radiative lifetimes. The shift to indirect transitions in the momentum space with an increasing twist angle and the energy modulation from the moiré potential both have a significant impact on interlayer exciton lifetimes. We further predict distinct temperature dependence of interlayer exciton lifetimes in TBLs with different twist angles, which is partially validated by experiments. While many recent studies have highlighted how the twist angle in a vdW TBL can be used to engineer the ground states and quantum phases due to many-body interaction, our studies explore its role in controlling the dynamics of optically excited states, thus, expanding the conceptual applications of "twistronics".
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Submitted 26 January, 2021; v1 submitted 29 July, 2020;
originally announced July 2020.
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Efficient second harmonic generation in nanophotonic GaAs-on-insulator waveguides
Authors:
Eric J. Stanton,
Jeff Chiles,
Nima Nader,
Galan Moody,
Nicolas Volet,
Lin Chang,
John E. Bowers,
Sae Woo Nam,
Richard P. Mirin
Abstract:
Nonlinear frequency conversion plays a crucial role in advancing the functionality of next-generation optical systems. Portable metrology references and quantum networks will demand highly efficient second-order nonlinear devices, and the intense nonlinear interactions of nanophotonic waveguides can be leveraged to meet these requirements. Here we demonstrate second harmonic generation (SHG) in Ga…
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Nonlinear frequency conversion plays a crucial role in advancing the functionality of next-generation optical systems. Portable metrology references and quantum networks will demand highly efficient second-order nonlinear devices, and the intense nonlinear interactions of nanophotonic waveguides can be leveraged to meet these requirements. Here we demonstrate second harmonic generation (SHG) in GaAs-on-insulator waveguides with unprecedented efficiency of 40 W$^{-1}$ for a single-pass device. This result is achieved by minimizing the propagation loss and optimizing phase-matching. We investigate surface-state absorption and design the waveguide geometry for modal phase-matching with tolerance to fabrication variation. A 2.0 $μ$m pump is converted to a 1.0 $μ$m signal in a length of 2.9 mm with a wide signal bandwidth of 148 GHz. Tunable and efficient operation is demonstrated over a temperature range of 45 $^{\circ}$C with a slope of 0.24 nm/$^{\circ}$C. Wafer-bonding between GaAs and SiO$_2$ is optimized to minimize waveguide loss, and the devices are fabricated on 76 mm wafers with high uniformity. We expect this device to enable fully integrated self-referenced frequency combs and high-rate entangled photon pair generation.
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Submitted 14 February, 2020; v1 submitted 27 December, 2019;
originally announced December 2019.
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Optimization of photoluminescence from W centers in silicon-on-insulator
Authors:
Sonia M. Buckley,
Alex N. Tait,
Galan Moody,
Stephen Olson,
Joshua Herman,
Kevin L. Silverman,
Satyavolu Papa Rao,
Sae Woo Nam,
Richard P. Mirin,
Jeffrey M. Shainline
Abstract:
W centers are trigonal defects generated by self-ion implantation in silicon that exhibit photoluminescence at 1.218 $μ$m. We have shown previously that they can be used in waveguide-integrated all-silicon light-emitting diodes (LEDs). Here we optimize the implant energy, fluence and anneal conditions to maximize the photoluminescence intensity for W centers implanted in silicon-on-insulator, a su…
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W centers are trigonal defects generated by self-ion implantation in silicon that exhibit photoluminescence at 1.218 $μ$m. We have shown previously that they can be used in waveguide-integrated all-silicon light-emitting diodes (LEDs). Here we optimize the implant energy, fluence and anneal conditions to maximize the photoluminescence intensity for W centers implanted in silicon-on-insulator, a substrate suitable for waveguide-integrated devices. After optimization, we observe near two orders of magnitude improvement in photoluminescence intensity relative to the conditions with the stopping range of the implanted ions at the center of the silicon device layer. The previously demonstrated waveguide-integrated LED used implant conditions with the stopping range at the center of this layer. We further show that such light sources can be manufactured at the 300-mm scale by demonstrating photoluminescence of similar intensity from 300 mm silicon-on-insulator wafers. The luminescence uniformity across the entire wafer is within the measurement error.
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Submitted 19 May, 2020; v1 submitted 4 November, 2019;
originally announced November 2019.
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Multi-functional integrated photonics in the mid-infrared with suspended AlGaAs on silicon
Authors:
Jeff Chiles,
Nima Nader,
Eric J. Stanton,
Daniel Herman,
Galan Moody,
Jiangang Zhu,
J. Connor Skehan,
Biswarup Guha,
Abijith Kowligy,
Juliet T. Gopinath,
Kartik Srinivasan,
Scott A. Diddams,
Ian Coddington,
Nathan R. Newbury,
Jeffrey M. Shainline,
Sae Woo Nam,
Richard P. Mirin
Abstract:
The microscale integration of mid- and longwave-infrared photonics could enable the development of fieldable, robust chemical sensors, as well as highly efficient infrared frequency converters. However, such technology would be defined by the choice of material platform, which immediately determines the strength and types of optical nonlinearities available, the optical transparency window, modal…
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The microscale integration of mid- and longwave-infrared photonics could enable the development of fieldable, robust chemical sensors, as well as highly efficient infrared frequency converters. However, such technology would be defined by the choice of material platform, which immediately determines the strength and types of optical nonlinearities available, the optical transparency window, modal confinement, and physical robustness. In this work, we demonstrate a new platform, suspended AlGaAs waveguides integrated on silicon, providing excellent performance in all of these metrics. We demonstrate low propagation losses within a span of nearly two octaves (1.26 to 4.6 $μ$m) with exemplary performance of 0.45 dB/cm at $λ= 2.4$ $μ$m. We exploit the high nonlinearity of this platform to demonstrate 1560 nm-pumped second-harmonic generation and octave-spanning supercontinuum reaching out to 2.3 $μ$m with 3.4 pJ pump pulse energy. With mid-IR pumping, we generate supercontinuum spanning from 2.3 to 6.5 $μ$m. Finally, we demonstrate the versatility of the platform with mid-infrared passive devices such as low-loss 10 $μ$m-radius bends, compact power splitters with 96 $\pm$ 1% efficiency and edge couplers with 3.0 $\pm$ 0.1 dB loss. This platform has strong potential for multi-functional integrated photonic systems in the mid-IR.
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Submitted 3 May, 2019;
originally announced May 2019.
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Dephasing of InAs quantum dot p-shell excitons using two-dimensional coherent spectroscopy
Authors:
Takeshi Suzuki,
Rohan Singh,
Galan Moody,
Marc Aßmann,
Manfred Bayer,
Arne Ludwig,
Andreas D. Wieck,
and Steven T. Cundiff
Abstract:
The dephasing mechanisms of p-shell and s-shell excitons in an InAs self-assembled quantum dot ensemble are examined using two-dimensional coherent spectroscopy (2DCS). 2DCS provides a comprehensive picture of how the energy level structure of dots affects the exciton dephasing rates and recombination lifetimes. We find that at low temperatures, dephasing of s-shell excitons is lifetime limited, w…
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The dephasing mechanisms of p-shell and s-shell excitons in an InAs self-assembled quantum dot ensemble are examined using two-dimensional coherent spectroscopy (2DCS). 2DCS provides a comprehensive picture of how the energy level structure of dots affects the exciton dephasing rates and recombination lifetimes. We find that at low temperatures, dephasing of s-shell excitons is lifetime limited, whereas p-shell excitons exhibit significant pure dephasing due to scattering between degenerate spin states. At elevated temperatures, quadratic exciton-phonon coupling plays an important role in both s-shell and p-shell exciton dephasing. We show that multiple p-shell states are also responsible for stronger phonon dephasing for these transitions
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Submitted 22 August, 2018;
originally announced August 2018.
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Microsecond Valley Lifetime of Defect-Bound Excitons in Monolayer WSe$_2$
Authors:
Galan Moody,
Kha Tran,
Xiaobo Lu,
Travis Autry,
James M. Fraser,
Richard P. Mirin,
Li Yang,
Xiaoqin Li,
Kevin L. Silverman
Abstract:
In atomically thin two-dimensional semiconductors such as transition metal dichalcogenides (TMDs), controlling the density and type of defects promises to be an effective approach for engineering light-matter interactions. We demonstrate that electron-beam irradiation is a simple tool for selectively introducing defect-bound exciton states associated with chalcogen vacancies in TMDs. Our first-pri…
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In atomically thin two-dimensional semiconductors such as transition metal dichalcogenides (TMDs), controlling the density and type of defects promises to be an effective approach for engineering light-matter interactions. We demonstrate that electron-beam irradiation is a simple tool for selectively introducing defect-bound exciton states associated with chalcogen vacancies in TMDs. Our first-principles calculations and time-resolved spectroscopy measurements of monolayer WSe2 reveal that these defect-bound excitons exhibit exceptional optical properties including a recombination lifetime approaching 200 ns and a valley lifetime longer than 1 $μ$s. The ability to engineer the crystal lattice through electron irradiation provides a new approach for tailoring the optical response of TMDs for photonics, quantum optics, and valleytronics applications.
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Submitted 10 July, 2018;
originally announced July 2018.
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Moiré Excitons in Van der Waals Heterostructures
Authors:
Kha Tran,
Galan Moody,
Fengcheng Wu,
Xiaobo Lu,
Junho Choi,
Akshay Singh,
Jacob Embley,
André Zepeda,
Marshall Campbell,
Kyounghwan Kim,
Amritesh Rai,
Travis Autry,
Daniel A. Sanchez,
Takashi Taniguchi,
Kenji Watanabe,
Nanshu Lu,
Sanjay K. Banerjee,
Emanuel Tutuc,
Li Yang,
Allan H. MacDonald,
Kevin L. Silverman,
Xiaoqin Li
Abstract:
In van der Waals (vdW) heterostructures formed by stacking two monolayer semiconductors, lattice mismatch or rotational misalignment introduces an in-plane moiré superlattice. While it is widely recognized that a moiré superlattice can modulate the electronic band structure and lead to novel transport properties including unconventional superconductivity and insulating behavior driven by correlati…
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In van der Waals (vdW) heterostructures formed by stacking two monolayer semiconductors, lattice mismatch or rotational misalignment introduces an in-plane moiré superlattice. While it is widely recognized that a moiré superlattice can modulate the electronic band structure and lead to novel transport properties including unconventional superconductivity and insulating behavior driven by correlations, its influence on optical properties has not been investigated experimentally. We present spectroscopic evidence that interlayer excitons are confined by the moiré potential in a high-quality MoSe2/WSe2 heterobilayer with small rotational twist. A series of interlayer exciton resonances with either positive or negative circularly polarized emission is observed in photoluminescence, consistent with multiple exciton states confined within the moiré potential. The recombination dynamics and temperature dependence of these interlayer exciton resonances are consistent with this interpretation. These results demonstrate the feasibility of engineering artificial excitonic crystals using vdW heterostructures for nanophotonics and quantum information applications.
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Submitted 10 July, 2018;
originally announced July 2018.
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Demonstrating sub-3 ps temporal resolution in a superconducting nanowire single-photon detector
Authors:
B. A. Korzh,
Q-Y. Zhao,
S. Frasca,
J. P. Allmaras,
T. M. Autry,
E. A. Bersin,
M. Colangelo,
G. M. Crouch,
A. E. Dane,
T. Gerrits,
F. Marsili,
G. Moody,
E. Ramirez,
J. D. Rezac,
M. J. Stevens,
E. E. Wollman,
D. Zhu,
P. D. Hale,
K. L. Silverman,
R. P. Mirin,
S. W. Nam,
M. D. Shaw,
K. K. Berggren
Abstract:
Improving the temporal resolution of single photon detectors has an impact on many applications, such as increased data rates and transmission distances for both classical and quantum optical communication systems, higher spatial resolution in laser ranging and observation of shorter-lived fluorophores in biomedical imaging. In recent years, superconducting nanowire single-photon detectors (SNSPDs…
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Improving the temporal resolution of single photon detectors has an impact on many applications, such as increased data rates and transmission distances for both classical and quantum optical communication systems, higher spatial resolution in laser ranging and observation of shorter-lived fluorophores in biomedical imaging. In recent years, superconducting nanowire single-photon detectors (SNSPDs) have emerged as the highest efficiency time-resolving single-photon counting detectors available in the near infrared. As the detection mechanism in SNSPDs occurs on picosecond time scales, SNSPDs have been demonstrated with exquisite temporal resolution below 15 ps. We reduce this value to 2.7$\pm$0.2 ps at 400 nm and 4.6$\pm$0.2 ps at 1550 nm, using a specialized niobium nitride (NbN) SNSPD. The observed photon-energy dependence of the temporal resolution and detection latency suggests that intrinsic effects make a significant contribution.
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Submitted 18 April, 2018;
originally announced April 2018.
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All-silicon light-emitting diodes waveguide-integrated with superconducting single-photon detectors
Authors:
Sonia Buckley,
Jeffrey Chiles,
Adam N. McCaughan,
Galan Moody,
Kevin L. Silverman,
Martin J. Stevens,
Richard P. Mirin,
Sae Woo Nam,
Jeffrey M. Shainline
Abstract:
We demonstrate cryogenic, electrically-injected, waveguide-coupled Si light-emitting diodes (LEDs) operating at 1.22 $μ$m. The active region of the LED consists of W centers implanted in the intrinsic region of a $p$-$i$-$n$ diode. The LEDs are integrated on waveguides with superconducting nanowire single-photon detectors (SNSPDs). We demonstrate the scalability of this platform with an LED couple…
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We demonstrate cryogenic, electrically-injected, waveguide-coupled Si light-emitting diodes (LEDs) operating at 1.22 $μ$m. The active region of the LED consists of W centers implanted in the intrinsic region of a $p$-$i$-$n$ diode. The LEDs are integrated on waveguides with superconducting nanowire single-photon detectors (SNSPDs). We demonstrate the scalability of this platform with an LED coupled to eleven SNSPDs in a single integrated photonic device. Such on-chip optical links may be useful for quantum information or neuromorphic computing applications.
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Submitted 6 July, 2017;
originally announced August 2017.
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Trion Valley Coherence in Monolayer Semiconductors
Authors:
Kai Hao,
Lixiang Xu,
Fengcheng Wu,
Philipp Nagler,
Kha Tran,
Xin Ma,
Christian Schüller,
Tobias Korn,
Allan H. MacDonald,
Galan Moody,
Xiaoqin Li
Abstract:
The emerging field of valleytronics aims to exploit the valley pseudospin of electrons residing near Bloch band extrema as an information carrier. Recent experiments demonstrating optical generation and manipulation of exciton valley coherence (the superposition of electron-hole pairs at opposite valleys) in monolayer transition metal dichalcogenides (TMDs) provide a critical step towards control…
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The emerging field of valleytronics aims to exploit the valley pseudospin of electrons residing near Bloch band extrema as an information carrier. Recent experiments demonstrating optical generation and manipulation of exciton valley coherence (the superposition of electron-hole pairs at opposite valleys) in monolayer transition metal dichalcogenides (TMDs) provide a critical step towards control of this quantum degree of freedom. The charged exciton (trion) in TMDs is an intriguing alternative to the neutral exciton for control of valley pseudospin because of its long spontaneous recombination lifetime, its robust valley polarization, and its coupling to residual electronic spin. Trion valley coherence has however been unexplored due to experimental challenges in accessing it spectroscopically. In this work, we employ ultrafast two-dimensional coherent spectroscopy to resonantly generate and detect trion valley coherence in monolayer MoSe$_2$ demonstrating that it persists for a few-hundred femtoseconds. We conclude that the underlying mechanisms limiting trion valley coherence are fundamentally different from those applicable to exciton valley coherence. Based on these observations, we suggest possible strategies for extending valley coherence times in two-dimensional materials.
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Submitted 10 November, 2016;
originally announced November 2016.
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Neutral and Charged Inter-Valley Biexcitons in Monolayer MoSe$_2$
Authors:
Kai Hao,
Lixiang Xu,
Judith F. Specht,
Philipp Nagler,
Kha Tran,
Akshay Singh,
Chandriker Kavir Dass,
Christian Schüller,
Tobias Korn,
Marten Richter,
Andreas Knorr,
Xiaoqin Li,
Galan Moody
Abstract:
In atomically thin transition metal dichalcogenides (TMDs), reduced dielectric screening of the Coulomb interaction leads to strongly correlated many-body states, including excitons and trions, that dominate the optical properties. Higher-order states, such as bound biexcitons, are possible but are difficult to identify unambiguously using linear optical spectroscopy methods alone. Here, we implem…
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In atomically thin transition metal dichalcogenides (TMDs), reduced dielectric screening of the Coulomb interaction leads to strongly correlated many-body states, including excitons and trions, that dominate the optical properties. Higher-order states, such as bound biexcitons, are possible but are difficult to identify unambiguously using linear optical spectroscopy methods alone. Here, we implement polarization-resolved two-dimensional coherent spectroscopy to unravel the complex optical response of monolayer MoSe$_2$ and identify multiple higher-order correlated states. Decisive signatures of neutral and charged inter-valley biexcitons appear in cross-polarized two-dimensional spectra as distinct resonances with respective ~20 meV and ~5 meV binding energies--similar to recent calculations using variational and Monte Carlo methods. A theoretical model taking into account the valley-dependent optical selection rules reveals the specific quantum pathways that give rise to these states. Inter-valley biexcitons identified here, comprised of neutral and charged excitons from different valleys, offer new opportunities for creating exotic exciton-polariton condensates and for developing ultrathin biexciton lasers and polarization-entangled photon sources.
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Submitted 7 September, 2016;
originally announced September 2016.
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Optical amplitude and phase modulation dynamics at the single-photon level in a quantum dot ridge waveguide
Authors:
Galan Moody,
Corey McDonald,
Ari Feldman,
Todd Harvey,
Richard P. Mirin,
Kevin L. Silverman
Abstract:
The amplitude and phase of a material's nonlinear optical response provide insight into the underlying electronic dynamics that determine its optical properties. Phase-sensitive nonlinear spectroscopy techniques are widely implemented to explore these dynamics through demodulation of the complex optical signal field into its quadrature components; however, complete reconstruction of the optical re…
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The amplitude and phase of a material's nonlinear optical response provide insight into the underlying electronic dynamics that determine its optical properties. Phase-sensitive nonlinear spectroscopy techniques are widely implemented to explore these dynamics through demodulation of the complex optical signal field into its quadrature components; however, complete reconstruction of the optical response requires measuring both the amplitude and phase of each quadrature, which is often lost in standard detection methods. Here, we implement a heterodyne-detection scheme to fully reconstruct the amplitude and phase response of spectral hole-burning from InAs/GaAs charged quantum dots. We observe an ultra-narrow absorption profile and a corresponding dispersive lineshape of the phase, which reflect the nanosecond optical coherence time of the charged exciton transition. Simultaneously, the measurements are sensitive to electron spin relaxation dynamics on a millisecond timescale, as this manifests as a magnetic-field dependent delay of the amplitude and phase modulation. Appreciable amplitude modulation depth and nonlinear phase shift up to 0.09$\timesπ$ radians (16$°$) are demonstrated, providing new possibilities for quadrature modulation at faint photon levels with several independent control parameters, including photon number, modulation frequency, detuning, and externally applied fields.
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Submitted 26 August, 2016;
originally announced August 2016.
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Coherent and Incoherent Coupling Dynamics between Neutral and Charged Excitons in Monolayer MoSe2
Authors:
Kai Hao,
Lixiang Xu,
Philipp Nagler,
Akshay Singh,
Kha Tran,
Chandriker Kavir Dass,
Christian Schüller,
Tobias Korn,
Xiaoqin Li,
Galan Moody
Abstract:
The optical properties of semiconducting transition metal dichalcogenides are dominated by both neutral excitons (electron-hole pairs) and charged excitons (trions) that are stable even at room temperature. While trions directly influence charge transport properties in optoelectronic devices, excitons may be relevant through exciton-trion coupling and conversion phenomena. In this work, we reveal…
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The optical properties of semiconducting transition metal dichalcogenides are dominated by both neutral excitons (electron-hole pairs) and charged excitons (trions) that are stable even at room temperature. While trions directly influence charge transport properties in optoelectronic devices, excitons may be relevant through exciton-trion coupling and conversion phenomena. In this work, we reveal the coherent and incoherent nature of exciton-trion coupling and the relevant timescales in monolayer MoSe2 using optical two-dimensional coherent spectroscopy. Coherent interaction between excitons and trions is definitively identified as quantum beating of cross-coupling peaks that persists for a few hundred femtoseconds. For longer times up to 10 ps, surprisingly, the relative intensity of the cross-coupling peaks increases, which is attributed to incoherent energy transfer likely due to phonon-assisted up-conversion and down-conversion processes that are efficient even at cryogenic temperature.
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Submitted 26 May, 2016;
originally announced May 2016.
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Exciton Dynamics in Monolayer Transition Metal Dichalcogenides
Authors:
Galan Moody,
John Schaibley,
Xiaodong Xu
Abstract:
Since the discovery of semiconducting monolayer transition metal dichalcogenides, a variety of experimental and theoretical studies have been carried out seeking to understand the intrinsic exciton population decay and valley relaxation dynamics. Reports of the exciton decay time range from hundreds of femtoseconds to ten nanoseconds, while the valley depolarization time can exceed one nanosecond.…
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Since the discovery of semiconducting monolayer transition metal dichalcogenides, a variety of experimental and theoretical studies have been carried out seeking to understand the intrinsic exciton population decay and valley relaxation dynamics. Reports of the exciton decay time range from hundreds of femtoseconds to ten nanoseconds, while the valley depolarization time can exceed one nanosecond. At present, however, a consensus on the microscopic mechanisms governing exciton radiative and non-radiative recombination is lacking. The strong exciton oscillator strength resulting in up to 20% absorption for a single monolayer points to ultrafast radiative recombination. However, the low quantum yield and large variance in the reported lifetimes suggest that non-radiative Auger-type processes obscure the intrinsic exciton radiative lifetime. In either case, the electron-hole exchange interaction plays an important role in the exciton spin and valley dynamics. In this article, we review the experiments and theory that have led to these conclusions and comment on future experiments that could complement our current understanding.
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Submitted 14 February, 2016;
originally announced February 2016.
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Electronic Coherence Control in a Charged Quantum Dot
Authors:
Galan Moody,
Corey McDonald,
Ari Feldman,
Todd Harvey,
Richard P. Mirin,
Kevin L. Silverman
Abstract:
Minimizing decoherence due to coupling of a quantum system to its fluctuating environment is at the forefront of quantum information science and photonics research. Nature sets the ultimate limit, however, given by the strength of the system's coupling to the electromagnetic field. Here, we establish the ability to electronically control this coupling and $\textit{enhance}$ the coherence time of a…
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Minimizing decoherence due to coupling of a quantum system to its fluctuating environment is at the forefront of quantum information science and photonics research. Nature sets the ultimate limit, however, given by the strength of the system's coupling to the electromagnetic field. Here, we establish the ability to electronically control this coupling and $\textit{enhance}$ the coherence time of a quantum dot excitonic state. Coherence control is demonstrated on the positively charged exciton transition (an electron Coulomb-bound with two holes) in quantum dots embedded in a photonic waveguide by manipulating the electron and hole wavefunctions through an applied lateral electric field. With increasing field up to 15 kV cm$^{-1}$, the coherence time increases by a factor of two from $\sim1.4$ ns to $\sim2.7$ ns. Numerical calculations reveal that longer coherence arises from the separation of charge carriers by up to $\sim6$ nm, which leads to a $30\%$ weaker transition dipole moment. The ability to electrostatically control the coherence time and transition dipole moment opens new avenues for quantum communication and novel coupling schemes between distant qubits.
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Submitted 19 October, 2015;
originally announced October 2015.
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Direct Measurement of Exciton Valley Coherence in Monolayer WSe$_2$
Authors:
Kai Hao,
Galan Moody,
Fengcheng Wu,
Chandriker Kavir Dass,
Lixiang Xu,
Chang-Hsaio Chen,
Ming-Yang Li,
Lain-Jong Li,
Allan H. MacDonald,
Xiaoqin Li
Abstract:
In crystals, energy band extrema in momentum space can be identified by their valley index. The internal quantum degree of freedom associated with valley pseudospin indices can act as a useful information carrier analogous to electronic charge or spin. Interest in valleytronics has been revived in recent years following the discovery of atomically thin materials such as graphene and transition met…
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In crystals, energy band extrema in momentum space can be identified by their valley index. The internal quantum degree of freedom associated with valley pseudospin indices can act as a useful information carrier analogous to electronic charge or spin. Interest in valleytronics has been revived in recent years following the discovery of atomically thin materials such as graphene and transition metal dichalcogenides. However, the valley coherence time, a key quantity for manipulating the valley pseudospin, has never been measured in any material. In this work, we use a sequence of laser pulses to resonantly generate a coherent superposition of excitons (Coulomb-bound electron-hole pairs) in opposite valleys of monolayer WSe$_2$. The imposed valley coherence persists for approximately one hundred femtoseconds. We propose that the electron-hole exchange interaction provides an important decoherence mechanism in addition to exciton population decay. Our work provides critical insight into the requirements and strategies for optical manipulation of the valley pseudospin for future valleytronics applications.
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Submitted 29 September, 2015;
originally announced September 2015.
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Trion Formation Dynamics in Monolayer Transition Metal Dichalcogenides
Authors:
Akshay Singh,
Galan Moody,
Kha Tran,
Marie Scott,
Vincent Overbeck,
Gunnar Berghäuser,
John Schaibley,
Edward J. Seifert,
Dennis Pleskot,
Nathaniel M. Gabor,
Jiaqiang Yan,
David G. Mandrus,
Marten Richter,
Ermin Malic,
Xiaodong Xu,
Xiaoqin Li
Abstract:
We report charged exciton (trion) formation dynamics in doped monolayer transition metal dichalcogenides (TMDs), specifically molybdenum diselenide (MoSe2), using resonant two-color pump-probe spectroscopy. When resonantly pumping the exciton transition, trions are generated on a picosecond timescale through exciton-electron interaction. As the pump energy is tuned from the high energy to low ener…
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We report charged exciton (trion) formation dynamics in doped monolayer transition metal dichalcogenides (TMDs), specifically molybdenum diselenide (MoSe2), using resonant two-color pump-probe spectroscopy. When resonantly pumping the exciton transition, trions are generated on a picosecond timescale through exciton-electron interaction. As the pump energy is tuned from the high energy to low energy side of the inhomogeneously broadened exciton resonance, the trion formation time increases by ~ 50%. This feature can be explained by the existence of both localized and delocalized excitons in a disordered potential and suggests the existence of an exciton mobility edge in TMDs. The quasiparticle formation and conversion processes are important for interpreting photoluminescence and photoconductivity in TMDs.
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Submitted 16 December, 2015; v1 submitted 16 July, 2015;
originally announced July 2015.
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Intrinsic Exciton Linewidth in Monolayer Transition Metal Dichalcogenides
Authors:
Galan Moody,
Chandriker Kavir Dass,
Kai Hao,
Chang-Hsiao Chen,
Lain-Jong Li,
Akshay Singh,
Kha Tran,
Genevieve Clark,
Xiaodong Xu,
Gunnar Bergauser,
Ermin Malic,
Andreas Knorr,
Xiaoqin Li
Abstract:
Monolayer transition metal dichalcogenides feature Coulomb-bound electron-hole pairs (excitons) with exceptionally large binding energy and coupled spin and valley degrees of freedom. These unique attributes have been leveraged for electrical and optical control of excitons for atomically-thin optoelectronics and valleytronics. The development of such technologies relies on understanding and quant…
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Monolayer transition metal dichalcogenides feature Coulomb-bound electron-hole pairs (excitons) with exceptionally large binding energy and coupled spin and valley degrees of freedom. These unique attributes have been leveraged for electrical and optical control of excitons for atomically-thin optoelectronics and valleytronics. The development of such technologies relies on understanding and quantifying the fundamental properties of the exciton. A key parameter is the intrinsic exciton homogeneous linewidth, which reflects irreversible quantum dissipation arising from system (exciton) and bath (vacuum and other quasiparticles) interactions. Using optical coherent two-dimensional spectroscopy, we provide the first experimental determination of the exciton homogeneous linewidth in monolayer transition metal dichalcogenides, specifically tungsten diselenide (WSe2). The role of exciton-exciton and exciton-phonon interactions in quantum decoherence is revealed through excitation density and temperature dependent linewidth measurements. The residual homogeneous linewidth extrapolated to zero density and temperature is ~1.5 meV, placing a lower bound of approximately 0.2 ps on the exciton radiative lifetime. The exciton quantum decoherence mechanisms presented in this work are expected to be ubiquitous in atomically-thin semiconductors.
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Submitted 12 October, 2014;
originally announced October 2014.
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Homogeneous Linewidth Narrowing of the Charged Exciton via Nuclear Spin Screening in an InAs/GaAs Quantum Dot Ensemble
Authors:
G. Moody,
M. Feng,
C. McDonald,
R. P. Mirin,
K. L. Silverman
Abstract:
In semiconductor quantum dots, the electron hyperfine interaction with the nuclear spin bath is the leading source of spin decoherence at cryogenic temperature. Using high-resolution two-color differential transmission spectroscopy, we demonstrate that such electron-nuclear coupling also imposes a lower limit for the positively charged exciton dephasing rate, γ, in an ensemble of InAs/GaAs quantum…
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In semiconductor quantum dots, the electron hyperfine interaction with the nuclear spin bath is the leading source of spin decoherence at cryogenic temperature. Using high-resolution two-color differential transmission spectroscopy, we demonstrate that such electron-nuclear coupling also imposes a lower limit for the positively charged exciton dephasing rate, γ, in an ensemble of InAs/GaAs quantum dots. We find that the dephasing rate is sensitive to the strength of the hyperfine interaction, which can be controlled through the application of an external magnetic field in the Faraday configuration. At zero applied field, strong electron-nuclear coupling induces additional dephasing beyond the radiative limit and γ= 230 MHz (0.95 μeV). Screening of the hyperfine interaction is achieved for an external field of ~1 T, resulting in γ= 172 MHz (0.71 μeV) limited only by spontaneous recombination. On the other hand, application of a Voigt magnetic field mixes the spin eigenstates, which increases the dephasing rate by up to 75%. These results are reproduced with a simple and intuitive model that captures the essential features of the electron hyperfine interaction and its influence on γ.
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Submitted 29 September, 2014;
originally announced September 2014.
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Coherent Electronic Coupling in Atomically Thin MoSe2
Authors:
Akshay Singh,
Galan Moody,
Sanfeng Wu,
Yanwen Wu,
Nirmal J. Ghimire,
Jiaqiang Yan,
David G. Mandrus,
Xiaodong Xu,
Xiaoqin Li
Abstract:
We report the first direct spectroscopic evidence for coherent electronic coupling between excitons and trions in atomically thin transition metal dichalcogenides, specifically monolayer MoSe2. Signatures of coupling appear as isolated cross-peaks in two-color pump-probe spectra, and the lineshape of the peaks reveals that the coupling originates from many-body interactions. Excellent agreement be…
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We report the first direct spectroscopic evidence for coherent electronic coupling between excitons and trions in atomically thin transition metal dichalcogenides, specifically monolayer MoSe2. Signatures of coupling appear as isolated cross-peaks in two-color pump-probe spectra, and the lineshape of the peaks reveals that the coupling originates from many-body interactions. Excellent agreement between the experiment and density matrix calculations suggests the formation of a correlated exciton-trion state due to their coupling.
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Submitted 9 January, 2014;
originally announced January 2014.