Showing 1–50 of 54 results for author: Toth, M

Finite temperature correlation functions of the sine--Gordon model

Authors: M. Tóth, J. H. Pixley, G. Takács, M. Kormos

Abstract: The sine-Gordon model serves as a foundational $1+1$-dimensional quantum field theory with numerous applications in condensed matter physics. Despite its integrability, characterizing its finite-temperature behavior remains a significant theoretical challenge. Here we use the previously developed Method of Random Surfaces (MRS) to evaluate two-point and higher-order correlation functions. We cross… ▽ More The sine-Gordon model serves as a foundational $1+1$-dimensional quantum field theory with numerous applications in condensed matter physics. Despite its integrability, characterizing its finite-temperature behavior remains a significant theoretical challenge. Here we use the previously developed Method of Random Surfaces (MRS) to evaluate two-point and higher-order correlation functions. We cross-check these results with known analytical limits, demonstrating that the MRS provides reliable, non-perturbative data in intermediate regimes where traditional form-factor expansions and semiclassical methods are inapplicable. Furthermore, we derive an exact result for arbitrary $N$-point functions satisfying an appropriate selection rule, providing a direct computational method for complex multi-point observables at finite temperature. We also characterize the non-Gaussianity of correlations and demonstrate that the results align with intuitive theoretical expectations. △ Less

Submitted 14 April, 2026; originally announced April 2026.

Comments: 7+5 pages, 4+3 figures

Twist-Controlled Modulation of Quantum Emitters in a Van der Waals Bilayer

Authors: Angus Gale, Seungjun Lee, Seungmin Park, Evan Williams, Helen Zhi Jie Zeng, James Liddle-Wesolowski, Young Duck Kim, Milos Toth, Tony Low, Igor Aharonovich

Abstract: Stacking and twisting two dimensional materials has garnered enormous attention across the condensed matter and the nanophotonic communities. The surge of interest stems from the emergence of novel photophysical phenomena that arise due to the interlayer coupling of the individual layers. Here, we demonstrate that the twist degree of freedom can modulate a single quantum emitter at room temperatur… ▽ More Stacking and twisting two dimensional materials has garnered enormous attention across the condensed matter and the nanophotonic communities. The surge of interest stems from the emergence of novel photophysical phenomena that arise due to the interlayer coupling of the individual layers. Here, we demonstrate that the twist degree of freedom can modulate a single quantum emitter at room temperature. We employ a van der Waals homobilayer of hexagonal boron nitride (hBN) and model the emission properties of quantum emitters as a function of the twist angle. Density functional theory results show that the embedded emitters are strongly influenced by the twist angle and the stacking of the top hBN layer. We consequently engineer these systems experimentally, and demonstrate in-situ tuning of embedded quantum emitters by mechanically twisting the top hBN layer, achieving tunability of over 30 nm (~ 100 meV). Our work demonstrates that mechanical twisting can be harnessed to modulate the embedded quantum emitters in a vdW material, marking a crucial step towards a programmable on-chip quantum circuitry. △ Less

Submitted 5 March, 2026; originally announced March 2026.

Quantum Emitters in Flux Grown hBN

Authors: Evan Williams, Angus Gale, Jake Horder, Dominic Scognamiglio, Milos Toth, Igor Aharonovich

Abstract: Hexagonal boron nitride (hBN) is an emerging material for use in quantum technologies, hosting bright and stable single photon emitters (SPEs). The B-center is one promising SPE in hBN, due to the near-deterministic creation methods and regular emission wavelength. However, incorporation of B-centers in high-quality crystals remains challenging, typically relying on additional post-growth methods… ▽ More Hexagonal boron nitride (hBN) is an emerging material for use in quantum technologies, hosting bright and stable single photon emitters (SPEs). The B-center is one promising SPE in hBN, due to the near-deterministic creation methods and regular emission wavelength. However, incorporation of B-centers in high-quality crystals remains challenging, typically relying on additional post-growth methods to increase creation efficiency. Here, we have demonstrated controlled carbon doping of hBN during growth, using a metal flux based method to increase the efficiency of B-center creation. Importantly, single B-centers with $g^{(2)}(0) < 0.5$ were able to be generated in the as-grown hBN when carbon additions during growth exceeded 2.5 wt.% C. Resonant excitation measurements revealed linewidths of 3.5 GHz with only moderate spectral diffusion present, demonstrating the applicability of the as-grown hBN as a host for high quality B-centers. △ Less

Submitted 20 February, 2025; originally announced February 2025.

Quantum Emitters in Rhombohedral Boron Nitride

Authors: Angus Gale, Mehran Kianinia, Jake Horder, Connor Tweedie, Mridul Singhal, Dominic Scognamiglio, Jiajie Qi, Kaihui Li, Carla Verdi, Igor Aharonovich, Milos Toth

Abstract: Rhombohedral boron nitride (rBN) is an emerging wide-bandgap van der Waals (vdW) material that combines strong second-order nonlinear optical properties with the structural flexibility of layered 2D systems. Here we show that rBN hosts optically-addressable spin defects and single-photon emitters (SPEs). Both are fabricated deterministically, using site-specific techniques, and are compared to the… ▽ More Rhombohedral boron nitride (rBN) is an emerging wide-bandgap van der Waals (vdW) material that combines strong second-order nonlinear optical properties with the structural flexibility of layered 2D systems. Here we show that rBN hosts optically-addressable spin defects and single-photon emitters (SPEs). Both are fabricated deterministically, using site-specific techniques, and are compared to their analogues in hexagonal boron nitride (hBN). Emission spectra in hBN and rBN are compared, and computational models of defects in hBN and rBN are used to elucidate the debated atomic structure of the B-center SPE in BN. Our results establish rBN as a monolithic vdW platform that uniquely combines second-order nonlinear optical properties, optically addressable spin defects, and high-quality SPEs, opening new possibilities for integrated quantum and nonlinear photonics. △ Less

Submitted 20 February, 2025; originally announced February 2025.

Quantum Optics Applications of Hexagonal Boron Nitride Defects

Authors: Aslı Çakan, Chanaprom Cholsuk, Angus Gale, Mehran Kianinia, Serkan Paçal, Serkan Ateş, Igor Aharonovich, Milos Toth, Tobias Vogl

Abstract: Hexagonal boron nitride (hBN) has emerged as a compelling platform for both classical and quantum technologies. In particular, the past decade has witnessed a surge of novel ideas and developments, which may be overwhelming for newcomers to the field. This review provides an overview of the fundamental concepts and key applications of hBN, including quantum sensing, quantum key distribution, quant… ▽ More Hexagonal boron nitride (hBN) has emerged as a compelling platform for both classical and quantum technologies. In particular, the past decade has witnessed a surge of novel ideas and developments, which may be overwhelming for newcomers to the field. This review provides an overview of the fundamental concepts and key applications of hBN, including quantum sensing, quantum key distribution, quantum computing, and quantum memory. Additionally, we highlight critical experimental and theoretical advances that have expanded the capabilities of hBN, in a cohesive and accessible manner. The objective is to equip readers with a comprehensive understanding of the diverse applications of hBN, and provide insights into ongoing research efforts. △ Less

Submitted 26 November, 2024; v1 submitted 10 October, 2024; originally announced October 2024.

Comments: 23 pages, 8 figures, 1 table

Journal ref: Adv. Optical Mater. 13, 2402508 (2025)

Sine-Gordon model at finite temperature: the method of random surfaces

Authors: M. Tóth, J. H. Pixley, D. Szász-Schagrin, G. Takács, M. Kormos

Abstract: We study the sine-Gordon quantum field theory at finite temperature by generalizing the method of random surfaces to compute the free energy and one-point functions of exponential operators non-perturbatively. Focusing on the gapped phase of the sine-Gordon model, we demonstrate the method's accuracy by comparing our results to the predictions of other methods and to exact results in the thermodyn… ▽ More We study the sine-Gordon quantum field theory at finite temperature by generalizing the method of random surfaces to compute the free energy and one-point functions of exponential operators non-perturbatively. Focusing on the gapped phase of the sine-Gordon model, we demonstrate the method's accuracy by comparing our results to the predictions of other methods and to exact results in the thermodynamic limit. We find excellent agreement between the method of random surfaces and other approaches when the temperature is not too small with respect to the mass gap. Extending the method to more general problems in strongly interacting one-dimensional quantum systems is discussed. △ Less

Submitted 16 August, 2024; originally announced August 2024.

Comments: 11+5 pages, 3+5 figures

Journal ref: Phys. Rev. B 111, 155112 (2025)

Electron Beam Restructuring of Quantum Emitters in Hexagonal Boron Nitride

Authors: Sergei Nedić, Karin Yamamura, Angus Gale, Igor Aharonovich, Milos Toth

Abstract: Hexagonal boron nitride (hBN) holds promise as a solid state, van der Waals host of single photon emitters for on-chip quantum photonics. The B-centre defect emitting at 436 nm is particularly compelling as it can be generated by electron beam irradiation. However, the emitter generation mechanism is unknown, the robustness of the method is variable, and it has only been applied successfully to th… ▽ More Hexagonal boron nitride (hBN) holds promise as a solid state, van der Waals host of single photon emitters for on-chip quantum photonics. The B-centre defect emitting at 436 nm is particularly compelling as it can be generated by electron beam irradiation. However, the emitter generation mechanism is unknown, the robustness of the method is variable, and it has only been applied successfully to thick flakes of hBN (>> 10 nm). Here, we use in-situ time-resolved cathodoluminescence (CL) spectroscopy to investigate the kinetics of B-centre generation. We show that the generation of B-centres is accompanied by quenching of a carbon-related emission at ~305 nm and that both processes are rate-limited by electromigration of defects in the hBN lattice. We identify problems that limit the efficacy and reproducibility of the emitter generation method, and solve them using a combination of optimized electron beam parameters and hBN pre- and post-processing treatments. We achieve B-centre quantum emitters in hBN flakes as thin as 8 nm, elucidate the mechanisms responsible for electron beam restructuring of quantum emitters in hBN, and gain insights towards identification of the atomic structure of the B-centre quantum emitter. △ Less

Submitted 14 April, 2024; originally announced April 2024.

Optically addressable spin defects coupled to bound states in the continuum metasurfaces

Authors: Luca Sortino, Angus Gale, Lucca Kühner, Chi Li, Jonas Biechteler, Fedja J. Wendisch, Mehran Kianinia, Haoran Ren, Milos Toth, Stefan A. Maier, Igor Aharonovich, Andreas Tittl

Abstract: Van der Waals (vdW) materials, including hexagonal boron nitride (hBN), are layered crystalline solids with appealing properties for investigating light-matter interactions at the nanoscale. hBN has emerged as a versatile building block for nanophotonic structures, and the recent identification of native optically addressable spin defects has opened up exciting possibilities in quantum technologie… ▽ More Van der Waals (vdW) materials, including hexagonal boron nitride (hBN), are layered crystalline solids with appealing properties for investigating light-matter interactions at the nanoscale. hBN has emerged as a versatile building block for nanophotonic structures, and the recent identification of native optically addressable spin defects has opened up exciting possibilities in quantum technologies. However, these defects exhibit relatively low quantum efficiencies and a broad emission spectrum, limiting potential applications. Optical metasurfaces present a novel approach to boost light emission efficiency, offering remarkable control over light-matter coupling at the sub-wavelength regime. Here, we propose and realise a monolithic scalable integration between intrinsic spin defects in hBN metasurfaces and high quality (Q) factor resonances leveraging quasi-bound states in the continuum (qBICs). Coupling between spin defect ensembles and qBIC resonances delivers a 25-fold increase in photoluminescence intensity, accompanied by spectral narrowing to below 4 nm linewidth facilitated by Q factors exceeding $10^2$. Our findings demonstrate a new class of spin based metasurfaces and pave the way towards vdW-based nanophotonic devices with enhanced efficiency and sensitivity for quantum applications in imaging, sensing, and light emission. △ Less

Submitted 6 March, 2024; v1 submitted 9 June, 2023; originally announced June 2023.

Comments: accepted version

Journal ref: Nature Communications, volume 15, Article number: 2008 (2024)

Manipulating the Charge State of Spin Defects in Hexagonal Boron Nitride

Authors: Angus Gale, Dominic Scognamiglio, Ivan Zhigulin, Benjamin Whitefield, Mehran Kianinia, Igor Aharonovich, Milos Toth

Abstract: Negatively charged boron vacancies ($\small{V_B^-}$) in hexagonal boron nitride (hBN) have recently gained interest as spin defects for quantum information processing and quantum sensing by a layered material. However, the boron vacancy can exist in a number of charge states in the hBN lattice, but only the -1 state has spin-dependent photoluminescence and acts as a spin-photon interface. Here, we… ▽ More Negatively charged boron vacancies ($\small{V_B^-}$) in hexagonal boron nitride (hBN) have recently gained interest as spin defects for quantum information processing and quantum sensing by a layered material. However, the boron vacancy can exist in a number of charge states in the hBN lattice, but only the -1 state has spin-dependent photoluminescence and acts as a spin-photon interface. Here, we investigate charge state switching of $\small{V_B}$ defects under laser and electron beam excitation. We demonstrate deterministic, reversible switching between the -1 and 0 states ($\small{V_B^- \rightleftharpoons V_B^0 + e^-}$), occurring at rates controlled by excess electrons or holes injected into hBN by a layered heterostructure device. Our work provides a means to monitor and manipulate the $\small{V_B}$ charge state, and to stabilize the -1 state which is a prerequisite for optical spin manipulation and readout of the defect. △ Less

Submitted 9 May, 2023; originally announced May 2023.

Framework for engineering of spin defects in hexagonal boron nitride by focused ion beams

Authors: Madeline Hennessey, Benjamin Whitefield, Angus Gale, John A Scott, Mehran Kianinia, Igor Aharonovich, Milos Toth

Abstract: Hexagonal boron nitride (hBN) is gaining interest as a wide bandgap van der Waals host of optically active spin defects for quantum technologies. Most studies of the spin-photon interface in hBN focus on the negatively charged boron vacancy (VB-) defect, which is typically fabricated by ion irradiation. However, VB- fabrication methods often lack robustness and reproducibility when applied to thin… ▽ More Hexagonal boron nitride (hBN) is gaining interest as a wide bandgap van der Waals host of optically active spin defects for quantum technologies. Most studies of the spin-photon interface in hBN focus on the negatively charged boron vacancy (VB-) defect, which is typically fabricated by ion irradiation. However, VB- fabrication methods often lack robustness and reproducibility when applied to thin flakes (less than 10 nm) of hBN. Here we identify mechanisms that both promote and inhibit VB- generation and optimize ion beam parameters for site-specific fabrication of optically active VB- centers. We emphasize conditions accessible by high resolution focused ion beam (FIB) systems, and present a framework for VB- fabrication in hBN flakes of arbitrary thickness for applications in quantum sensing and quantum information processing. △ Less

Submitted 9 November, 2023; v1 submitted 12 March, 2023; originally announced March 2023.

Comments: 11 pages, 5 figures

Ultralow-power cryogenic thermometry based on optical-transition broadening of a two-level system in diamond

Authors: Yongliang Chen, Simon White, Evgeny A. Ekimov, Carlo Bradac, Milos Toth, Igor Aharonovich, Toan Trong Tran

Abstract: Cryogenic temperatures are the prerequisite for many advanced scientific applications and technologies. The accurate determination of temperature in this range and at the submicrometer scale is, however, nontrivial. This is due to the fact that temperature reading in cryogenic conditions can be inaccurate due to optically induced heating. Here, we present an ultralow power, optical thermometry tec… ▽ More Cryogenic temperatures are the prerequisite for many advanced scientific applications and technologies. The accurate determination of temperature in this range and at the submicrometer scale is, however, nontrivial. This is due to the fact that temperature reading in cryogenic conditions can be inaccurate due to optically induced heating. Here, we present an ultralow power, optical thermometry technique that operates at cryogenic temperatures. The technique exploits the temperature dependent linewidth broadening measured by resonant photoluminescence of a two level system, a germanium vacancy color center in a nanodiamond host. The proposed technique achieves a relative sensitivity of 20% 1/K, at 5 K. This is higher than any other all optical nanothermometry method. Additionally, it achieves such sensitivities while employing excitation powers of just a few tens of nanowatts, several orders of magnitude lower than other traditional optical thermometry protocols. To showcase the performance of the method, we demonstrate its ability to accurately read out local differences in temperatures at various target locations of a custom-made microcircuit. Our work is a definite step towards the advancement of nanoscale optical thermometry at cryogenic temperatures. △ Less

Submitted 3 November, 2022; originally announced November 2022.

Suppression of surface roughening during ion bombardment of semiconductors

Authors: John A. Scott, James Bishop, Milos Toth

Abstract: Ion beams are used routinely for processing of semiconductors, particularly sputtering, ion implantation and direct-write fabrication of nanostructures. However, the utility of ion beam techniques is limited by crystal damage and surface roughening. Damage can be reduced or eliminated by performing irradiation at elevated temperatures. However, at these conditions, surface roughening is highly pro… ▽ More Ion beams are used routinely for processing of semiconductors, particularly sputtering, ion implantation and direct-write fabrication of nanostructures. However, the utility of ion beam techniques is limited by crystal damage and surface roughening. Damage can be reduced or eliminated by performing irradiation at elevated temperatures. However, at these conditions, surface roughening is highly problematic due to thermal mobility of adatoms and surface vacancies. Here we solve this problem using hydrogen gas, which we use to stabilize surface mass flow and suppress roughening during ion bombardment of elemental and compound semiconductors. We achieve smooth surfaces during ion-beam processing, and show that the method can be enhanced by radicalizing H2 gas using a remote plasma source. Our approach is broadly applicable, and expands the utility of ion beam techniques for the processing and fabrication of functional materials and nanostructures. △ Less

Submitted 19 September, 2022; v1 submitted 29 May, 2022; originally announced May 2022.

Comments: 14 pages, 5 figures

Real-time ratiometric optical nanoscale thermometry

Authors: Yongliang Chen, Chi Li, Tieshan Yang, Evgeny A. Ekimov, Carlo Bradac, Milos Toth, Igor Aharonovich, Toan Trong Tran

Abstract: All optical nanothermometry has become a powerful, noninvasive tool for measuring nanoscale temperatures in applications ranging from medicine to nanooptics and solid-state nanodevices. The key features of any candidate nanothermometer are sensitivity and resolution. Here, we demonstrate a real time, diamond based nanothermometry technique with sensitivity and resolution much larger than those of… ▽ More All optical nanothermometry has become a powerful, noninvasive tool for measuring nanoscale temperatures in applications ranging from medicine to nanooptics and solid-state nanodevices. The key features of any candidate nanothermometer are sensitivity and resolution. Here, we demonstrate a real time, diamond based nanothermometry technique with sensitivity and resolution much larger than those of any existing all optical method. The distinct performance of our approach stems from two factors. First, temperature sensors nanodiamonds cohosting two Group IV colour centers engineered to emit spectrally separated Stokes and AntiStokes fluorescence signals under excitation by a single laser source. Second, a parallel detection scheme based on filtering optics and high sensitivity photon counters for fast readout. We demonstrate the performance of our method by monitoring temporal changes in the local temperature of a microcircuit and a MoTe2 field effect transistor. Our work lays the foundation for time resolved temperature monitoring and mapping of micro, nanoscale devices such as microfluidic channels, nanophotonic circuits, and nanoelectronic devices, as well as complex biological environments such as tissues and cells. △ Less

Submitted 3 December, 2021; originally announced December 2021.

Deterministic fabrication of blue quantum emitters in hexagonal boron nitride

Authors: Angus Gale, Chi Li, Yongliang Chen, Kenji Watanabe, Takashi Taniguchi, Igor Aharonovich, Milos Toth

Abstract: Hexagonal boron nitride (hBN) is gaining considerable attention as a solid-state host of quantum emitters from the ultraviolet to the near infrared spectral ranges. However, atomic structures of most of the emitters are speculative or unknown, and emitter fabrication methods typically suffer from poor reproducibility, spatial accuracy, or spectral specificity. Here, we present a robust, determinis… ▽ More Hexagonal boron nitride (hBN) is gaining considerable attention as a solid-state host of quantum emitters from the ultraviolet to the near infrared spectral ranges. However, atomic structures of most of the emitters are speculative or unknown, and emitter fabrication methods typically suffer from poor reproducibility, spatial accuracy, or spectral specificity. Here, we present a robust, deterministic electron beam technique for site-specific fabrication of blue quantum emitters with a zero-phonon line at 436 nm (2.8 eV). We show that the emission intensity is proportional to electron dose and that the efficacy of the fabrication method correlates with a defect emission at 305 nm (4.1 eV). We attribute blue emitter generation to fragmentation of carbon clusters by electron impact and show that the robustness and universality of the emitter fabrication technique are enhanced by a pre-irradiation annealing treatment. Our results provide important insights into photophysical properties and structure of defects in hBN and a framework for deterministic fabrication of quantum emitters in hBN. △ Less

Submitted 26 November, 2021; originally announced November 2021.

Coupling spin defects in hexagonal boron nitride to monolithic bullseye cavities

Authors: Johannes E. Fröch, Lesley Spencer, Mehran Kianinia, Daniel Totonjian, Minh Nguyen, Vladimir Dyakonov, Milos Toth, Sejeong Kim, Igor Aharonovich

Abstract: Color centers in hexagonal boron nitride (hBN) are becoming an increasingly important building block for quantum photonic applications. Herein, we demonstrate the efficient coupling of recently discovered spin defects in hBN to purposely designed bullseye cavities. We show that the all monolithic hBN cavity system exhibits an order of magnitude enhancement in the emission of the coupled boron vaca… ▽ More Color centers in hexagonal boron nitride (hBN) are becoming an increasingly important building block for quantum photonic applications. Herein, we demonstrate the efficient coupling of recently discovered spin defects in hBN to purposely designed bullseye cavities. We show that the all monolithic hBN cavity system exhibits an order of magnitude enhancement in the emission of the coupled boron vacancy spin defects. In addition, by comparative finite difference time domain modelling, we shed light on the emission dipole orientation, which has not been experimentally demonstrated at this point. Beyond that, the coupled spin system exhibits an enhanced contrast in optically detected magnetic resonance readout and improved signal to noise ratio. Thus, our experimental results supported by simulations, constitute a first step towards integration of hBN spin defects with photonic resonators for a scalable spin photon interface. △ Less

Submitted 25 May, 2021; originally announced May 2021.

Bottom-Up Synthesis of Hexagonal Boron Nitride Nanoparticles with Intensity-Stabilized Quantum Emitters

Authors: Yongliang Chen, Xiaoxue Xu, Chi Li, Avi Bendavid, Mika T. Westerhausen, Carlo Bradac, Milos Toth, Igor Aharonovich, Toan Trong Tran

Abstract: Fluorescent nanoparticles are widely utilized in a large range of nanoscale imaging and sensing applications. While ultra-small nanoparticles (size <10 nm) are highly desirable, at this size range their photostability can be compromised due to effects such as intensity fluctuation and spectral diffusion caused by interaction with surface states. In this letter, we demonstrate a facile, bottom-up t… ▽ More Fluorescent nanoparticles are widely utilized in a large range of nanoscale imaging and sensing applications. While ultra-small nanoparticles (size <10 nm) are highly desirable, at this size range their photostability can be compromised due to effects such as intensity fluctuation and spectral diffusion caused by interaction with surface states. In this letter, we demonstrate a facile, bottom-up technique for the fabrication of sub-10-nm hBN nanoparticles hosting photostable bright emitters via a catalyst-free hydrothermal reaction between boric acid and melamine. We also implement a simple stabilization protocol that significantly reduces intensity fluctuation by ~85% and narrows the emission linewidth by ~14% by employing a common sol-gel silica coating process. Our study advances a promising strategy for the scalable, bottom-up synthesis of high-quality quantum emitters in hBN nanoparticles. △ Less

Submitted 27 January, 2021; originally announced January 2021.

Grain Dependent Growth of Bright Quantum Emitters in Hexagonal Boron Nitride

Authors: Noah Mendelson, Luis Morales, Chi Li, Ritika Ritika, Minh Anh Phan Nguyen, Jacqueline Loyola-Echeverria, Sejeong Kim, Stephan Gotzinger, Milos Toth, Igor Aharonovich

Abstract: Point defects in hexagonal boron nitride have emerged as a promising quantum light source due to their bright and photostable room temperature emission. In this work, we study the incorporation of quantum emitters during chemical vapor deposition growth on a nickel substrate. Combining a range of characterization techniques, we demonstrate that the incorporation of quantum emitters is limited to (… ▽ More Point defects in hexagonal boron nitride have emerged as a promising quantum light source due to their bright and photostable room temperature emission. In this work, we study the incorporation of quantum emitters during chemical vapor deposition growth on a nickel substrate. Combining a range of characterization techniques, we demonstrate that the incorporation of quantum emitters is limited to (001) oriented nickel grains. Such emitters display improved emission properties in terms of brightness and stability. We further utilize these emitters and integrate them with a compact optical antenna enhancing light collection from the sources. The hybrid device yields average saturation count rates of ~2.9 x106 cps and an average photon purity of ~90%. Our results advance the controlled generation of spatially distributed quantum emitters in hBN and demonstrate a key step towards on-chip devices with maximum collection efficiency. △ Less

Submitted 21 May, 2020; originally announced May 2020.

Optical Thermometry with Quantum Emitters in Hexagonal Boron Nitride

Authors: Yongliang Chen, Thinh Ngoc Tran, Ngoc My Hanh Duong, Chi Li, Milos Toth, Carlo Bradac, Igor Aharonovich, Alexander Solntsev, Toan Trong Tran

Abstract: Nanoscale optical thermometry is a promising non-contact route for measuring local temperature with both high sensitivity and spatial resolution. In this work, we present a deterministic optical thermometry technique based on quantum emitters in nanoscale hexagonal boron-nitride. We show that these nanothermometers exhibit better performance than that of homologous, all-optical nanothermometers bo… ▽ More Nanoscale optical thermometry is a promising non-contact route for measuring local temperature with both high sensitivity and spatial resolution. In this work, we present a deterministic optical thermometry technique based on quantum emitters in nanoscale hexagonal boron-nitride. We show that these nanothermometers exhibit better performance than that of homologous, all-optical nanothermometers both in sensitivity and range of working temperature. We demonstrate their effectiveness as nanothermometers by monitoring the local temperature at specific locations in a variety of custom-built micro-circuits. This work opens new avenues for nanoscale temperature measurements and heat flow studies in miniaturized, integrated devices. △ Less

Submitted 8 March, 2020; originally announced March 2020.

Identifying Carbon as the Source of Visible Single Photon Emission from Hexagonal Boron Nitride

Authors: Noah Mendelson, Dipankar Chugh, Jeffrey R. Reimers, Tin S. Cheng, Andreas Gottscholl, Hu Long, Christopher J. Mellor, Alex Zettl, Vladimir Dyakonov, Peter H. Beton, Sergei V. Novikov, Chennupati Jagadish, Hark Hoe Tan, Michael J. Ford, Milos Toth, Carlo Bradac, Igor Aharonovich

Abstract: Single photon emitters (SPEs) in hexagonal boron nitride (hBN) have garnered significant attention over the last few years due to their superior optical properties. However, despite the vast range of experimental results and theoretical calculations, the defect structure responsible for the observed emission has remained elusive. Here, by controlling the incorporation of impurities into hBN and by… ▽ More Single photon emitters (SPEs) in hexagonal boron nitride (hBN) have garnered significant attention over the last few years due to their superior optical properties. However, despite the vast range of experimental results and theoretical calculations, the defect structure responsible for the observed emission has remained elusive. Here, by controlling the incorporation of impurities into hBN and by comparing various synthesis methods, we provide direct evidence that the visible SPEs are carbon related. Room temperature optically detected magnetic resonance (ODMR) is demonstrated on ensembles of these defects. We also perform ion implantation experiments and confirm that only carbon implantation creates SPEs in the visible spectral range. Computational analysis of hundreds of potential carbon-based defect transitions suggest that the emission results from the negatively charged VBCN- defect, which experiences long-range out-of-plane deformations and is environmentally sensitive. Our results resolve a long-standing debate about the origin of single emitters at the visible range in hBN and will be key to deterministic engineering of these defects for quantum photonic devices. △ Less

Submitted 20 April, 2020; v1 submitted 2 March, 2020; originally announced March 2020.

Strain Engineering of Quantum Emitters in Hexagonal Boron Nitride

Authors: Noah Mendelson, Marcus Doherty, Milos Toth, Igor Aharonovich, Toan Trong Tran

Abstract: Quantum emitters in hexagonal boron nitride (hBN) are promising building blocks for the realization of integrated quantum photonic systems. However, their spectral inhomogeneity currently limits their potential applications. Here, we apply tensile strain to quantum emitters embedded in few-layer hBN films and realize both red and blue spectral shifts with tuning magnitudes up to 65 meV, a record f… ▽ More Quantum emitters in hexagonal boron nitride (hBN) are promising building blocks for the realization of integrated quantum photonic systems. However, their spectral inhomogeneity currently limits their potential applications. Here, we apply tensile strain to quantum emitters embedded in few-layer hBN films and realize both red and blue spectral shifts with tuning magnitudes up to 65 meV, a record for any two-dimensional quantum source. We demonstrate reversible tuning of the emission and related photophysical properties. We also observe rotation of the optical dipole in response to strain, suggesting the presence of a second excited state. We derive a theoretical model to describe strain-based tuning in hBN, and the rotation of the optical dipole. Our work demonstrates the immense potential for strain tuning of quantum emitters in layered materials to enable their employment in scalable quantum photonic networks. △ Less

Submitted 10 January, 2020; v1 submitted 18 November, 2019; originally announced November 2019.

Low-temperature electron-phonon interaction of quantum emitters in hexagonal Boron Nitride

Authors: Gabriele Grosso, Hyowon Moon, Christopher J. Ciccarino, Johannes Flick, Noah Mendelson, Milos Toth, Igor Aharonovich, Prineha Narang, Dirk R. Englund

Abstract: Quantum emitters based on atomic defects in layered hexagonal Boron Nitride (hBN) have emerged as promising solid state 'artificial atoms' with atom-like photophysical and quantum optoelectronic properties. Similar to other atom-like emitters, defect-phonon coupling in hBN governs the characteristic single-photon emission and provides an opportunity to investigate the atomic and electronic structu… ▽ More Quantum emitters based on atomic defects in layered hexagonal Boron Nitride (hBN) have emerged as promising solid state 'artificial atoms' with atom-like photophysical and quantum optoelectronic properties. Similar to other atom-like emitters, defect-phonon coupling in hBN governs the characteristic single-photon emission and provides an opportunity to investigate the atomic and electronic structure of emitters as well as the coupling of their spin- and charge-dependent electronic states to phonons. Here, we investigate these questions using photoluminescence excitation (PLE) experiments at T=4K on single photon emitters in multilayer hBN grown by chemical vapor deposition. By scanning up to 250 meV from the zero phonon line (ZPL), we can precisely measure the emitter's coupling efficiency to different phonon modes. Our results show that excitation mediated by the absorption of one in-plane optical phonon increases the emitter absorption probability ten-fold compared to that mediated by acoustic or out-of-plane optical phonons. We compare these measurements against theoretical predictions by first-principles density-functional theory of four defect candidates, for which we calculate prevalent charge states and their spin-dependent coupling to bulk and local phonon modes. Our work illuminates the phonon-coupled dynamics in hBN quantum emitters at cryogenic temperature, with implications more generally for mesoscopic quantum emitter systems in 2D materials and represents possible applications in solid-state quantum technologies. △ Less

Submitted 4 October, 2019; originally announced October 2019.

Photonic devices fabricated from (111) oriented single crystal diamond

Authors: Blake Regan, Sejeong Kim, Anh Tu Huy Ly, Aleksandra Trycz, Kerem Bray, Kumaravelu Ganesan, Milos Toth, Igor Aharonovich

Abstract: Diamond is a material of choice in the pursuit of integrated quantum photonic technologies. So far, the majority of photonic devices fabricated from diamond, are made from (100)-oriented crystals. In this work, we demonstrate a methodology for the fabrication of optically-active membranes from (111)-oriented diamond. We use a liftoff technique to generate membranes, followed by chemical vapour dep… ▽ More Diamond is a material of choice in the pursuit of integrated quantum photonic technologies. So far, the majority of photonic devices fabricated from diamond, are made from (100)-oriented crystals. In this work, we demonstrate a methodology for the fabrication of optically-active membranes from (111)-oriented diamond. We use a liftoff technique to generate membranes, followed by chemical vapour deposition of diamond in the presence of silicon to generate homogenous silicon vacancy colour centers with emission properties that are superior to those in (100)-oriented diamond. We further use the diamond membranes to fabricate high quality microring resonators with quality factors exceeding ~ 3000. Supported by finite difference time domain calculations, we discuss the advantages of (111) oriented structures as building blocks for quantum nanophotonic devices. △ Less

Submitted 9 September, 2019; originally announced September 2019.

Charge transition levels of quantum emitters in hexagonal boron nitride

Authors: Zai-Quan Xu, Noah Mendelson, John A. Scott, Chi Li, Igor Aharonovich, Milos Toth

Abstract: Quantum emitters in layered materials are promising candidates for applications in nanophotonics. Here we present a technique based on charge transfer to graphene for measuring the charge transition levels ($\rm E_t$) of fluorescent defects in a wide bandgap 2D material, and apply it to quantum emitters in hexagonal boron nitride (hBN). Our results will aid in identifying the atomic structures of… ▽ More Quantum emitters in layered materials are promising candidates for applications in nanophotonics. Here we present a technique based on charge transfer to graphene for measuring the charge transition levels ($\rm E_t$) of fluorescent defects in a wide bandgap 2D material, and apply it to quantum emitters in hexagonal boron nitride (hBN). Our results will aid in identifying the atomic structures of quantum emitters in hBN, as well as practical applications since $\rm E_t$ determines defect charge states and plays a key role in photodynamics. △ Less

Submitted 30 June, 2019; originally announced July 2019.

Room Temperature Initialisation and Readout of Intrinsic Spin Defects in a Van der Waals Crystal

Authors: Andreas Gottscholl, Mehran Kianinia, Victor Soltamov, Carlo Bradac, Christian Kasper, Klaus Krambrock, Andreas Sperlich, Milos Toth, Igor Aharonovich, Vladimir Dyakonov

Abstract: Optically addressable spins in widebandgap semiconductors have become one of the most prominent platforms for exploring fundamental quantum phenomena. While several candidates in 3D crystals including diamond and silicon carbide have been extensively studied, the identification of spindependent processes in atomically thin 2D materials has remained elusive. Although optically accessible spin state… ▽ More Optically addressable spins in widebandgap semiconductors have become one of the most prominent platforms for exploring fundamental quantum phenomena. While several candidates in 3D crystals including diamond and silicon carbide have been extensively studied, the identification of spindependent processes in atomically thin 2D materials has remained elusive. Although optically accessible spin states in hBN are theoretically predicted, they have not yet been observed experimentally. Here, employing rigorous electron paramagnetic resonance techniques and photoluminescence spectroscopy, we identify fluorescence lines in hexagonal boron nitride associated with a particular defect, the negatively charged boron vacancy and determine the parameters of its spin Hamiltonian. We show that the defect has a triplet ground state with a zero field splitting of 3.5 GHz and establish that the centre exhibits optically detected magnetic resonance at room temperature. We also demonstrate the spin polarization of this centre under optical pumping, which leads to optically induced population inversion of the spin ground state a prerequisite for coherent spin manipulation schemes. Our results constitute a leap forward in establishing two dimensional hBN as a prime platform for scalable quantum technologies, with extended potential for spin based quantum information and sensing applications, as our ODMR studies on hBN NV diamonds hybrid structures show. △ Less

Submitted 9 June, 2019; originally announced June 2019.

Journal ref: Nature Materials (2020)

Direct Measurement of Quantum Efficiency of Single Photon Emitters in Hexagonal Boron Nitride

Authors: Niko Nikolay, Noah Mendelson, Ersan Özelci, Bernd Sontheimer, Florian Böhm, Günter Kewes, Milos Toth, Igor Aharonovich, Oliver Benson

Abstract: Single photon emitters in two-dimensional materials are promising candidates for future generation of quantum photonic technologies. In this work, we experimentally determine the quantum efficiency (QE) of single photon emitters (SPE) in few-layer hexagonal boron nitride (hBN). We employ a metal hemisphere that is attached to the tip of an atomic force microscope to directly measure the lifetime v… ▽ More Single photon emitters in two-dimensional materials are promising candidates for future generation of quantum photonic technologies. In this work, we experimentally determine the quantum efficiency (QE) of single photon emitters (SPE) in few-layer hexagonal boron nitride (hBN). We employ a metal hemisphere that is attached to the tip of an atomic force microscope to directly measure the lifetime variation of the SPEs as the tip approaches the hBN. This technique enables non-destructive, yet direct and absolute measurement of the QE of SPEs. We find that the emitters exhibit very high QEs approaching $(87 \pm 7)\,\%$ at wavelengths of $\approx\,580\,\mathrm{nm}$, which is amongst the highest QEs recorded for a solid state single photon emitter. △ Less

Submitted 17 April, 2019; originally announced April 2019.

Selective Defect Formation in Hexagonal Boron Nitride

Authors: Irfan H. Abidi, Noah Mendelson, Toan Trong Tran, Abhishek Tyagi, Minghao Zhuang, Lu-Tao Weng, Barbaros Ozyilmaz, Igor Aharonovich, Milos Toth, Zhengtang Luo

Abstract: Luminescent defect-centers in hexagonal boron nitride (hBN) have emerged as a promising 2D-source of single photon emitters (SPEs) due to their high brightness and robust operation at room temperature. The ability to create such emitters with well-defined optical properties is a cornerstone towards their integration into on-chip photonic architectures. Here, we report an effective approach to fabr… ▽ More Luminescent defect-centers in hexagonal boron nitride (hBN) have emerged as a promising 2D-source of single photon emitters (SPEs) due to their high brightness and robust operation at room temperature. The ability to create such emitters with well-defined optical properties is a cornerstone towards their integration into on-chip photonic architectures. Here, we report an effective approach to fabricate hBN single photon emitters (SPEs) with desired emission properties in two isolated spectral regions via the manipulation of boron diffusion through copper during atmospheric pressure chemical vapor deposition (APCVD)--a process we term gettering. Using the gettering technique we deterministically place the resulting zero-phonon line (ZPL) between the regions 550-600 nm or from 600-650 nm, paving the way for hBN SPEs with tailored emission properties across a broad spectral range. Our ability to control defect formation during hBN growth provides a simple and cost-effective means to improve the crystallinity of CVD hBN films, and lower defect density making it applicable to hBN growth for a wide range of applications. Our results are important to understand defect formation of quantum emitters in hBN and deploy them for scalable photonic technologies. △ Less

Submitted 24 February, 2019; v1 submitted 21 February, 2019; originally announced February 2019.

Suppression of Spectral Diffusion by Anti-Stokes Excitation of Quantum Emitters in Hexagonal Boron Nitride

Authors: Toan Trong Tran, Carlo Bradac, Alexander S. Solntsev, Milos Toth, Igor Aharonovich

Abstract: Solid-state quantum emitters are garnering a lot of attention due to their role in scalable quantum photonics. A notable majority of these emitters, however, exhibit spectral diffusion due to local, fluctuating electromagnetic fields. In this work, we demonstrate efficient Anti-Stokes (AS) excitation of quantum emitters in hexagonal boron nitride (hBN), and show that the process results in the sup… ▽ More Solid-state quantum emitters are garnering a lot of attention due to their role in scalable quantum photonics. A notable majority of these emitters, however, exhibit spectral diffusion due to local, fluctuating electromagnetic fields. In this work, we demonstrate efficient Anti-Stokes (AS) excitation of quantum emitters in hexagonal boron nitride (hBN), and show that the process results in the suppression of a specific mechanism responsible for spectral diffusion of the emitters. We also demonstrate an all-optical gating scheme that exploits Stokes and Anti-Stokes excitation to manipulate spectral diffusion so as to switch and lock the emission energy of the photon source. In this scheme, reversible spectral jumps are deliberately enabled by pumping the emitter with high energy (Stokes) excitation; AS excitation is then used to lock the system into a fixed state characterized by a fixed emission energy. Our results provide important insights into the photophysical properties of quantum emitters in hBN, and introduce a new strategy for controlling the emission wavelength of quantum emitters. △ Less

Submitted 10 February, 2019; originally announced February 2019.

Effects of microstructure and growth conditions on quantum emitters in Gallium Nitride

Authors: Minh Nguyen, Tongtong Zhu, Mehran Kianinia, Fabien Massabuau, Igor Aharonovich, Milos Toth, Rachel Oliver, Carlo Bradac

Abstract: Single-photon emitters in gallium nitride (GaN) are gaining interest as attractive quantum systems due to the well-established techniques for growth and nanofabrication of the host material, as well as its remarkable chemical stability and optoelectronic properties. We investigate the nature of such single-photon emitters in GaN with a systematic analysis of various samples produced under differen… ▽ More Single-photon emitters in gallium nitride (GaN) are gaining interest as attractive quantum systems due to the well-established techniques for growth and nanofabrication of the host material, as well as its remarkable chemical stability and optoelectronic properties. We investigate the nature of such single-photon emitters in GaN with a systematic analysis of various samples produced under different growth conditions. We explore the effect that intrinsic structural defects (dislocations and stacking faults), doping and crystal orientation in GaN have on the formation of quantum emitters. We investigate the relationship between the position of the emitters (determined via spectroscopy and photoluminescence measurements) and the location of threading dislocations (characterised both via atomic force microscopy and cathodoluminescence). We find that quantum emitters do not correlate with stacking faults or dislocations; instead, they are more likely to originate from point defects or impurities whose density is modulated by the local extended defect density. △ Less

Submitted 28 November, 2018; originally announced November 2018.

Fabrication of photonic nanostructures from hexagonal boron nitride

Authors: Johannes E. Fröch, Yongsop Hwang, Sejeong Kim, Igor Aharonovich, Milos Toth

Abstract: Growing interest in devices based on layered van der Waals (vdW) materials is motivating the development of new nanofabrication methods. Hexagonal boron nitride (hBN) is one of the most promising materials for studies of quantum photonics and polaritonics. Here, we report in detail on a promising nanofabrication processes used to fabricate several hBN photonic devices using a hybrid electron beam… ▽ More Growing interest in devices based on layered van der Waals (vdW) materials is motivating the development of new nanofabrication methods. Hexagonal boron nitride (hBN) is one of the most promising materials for studies of quantum photonics and polaritonics. Here, we report in detail on a promising nanofabrication processes used to fabricate several hBN photonic devices using a hybrid electron beam induced etching (EBIE) and reactive ion etching (RIE) technique. We highlight the shortcomings and benefits of RIE and EBIE and demonstrate the utility of the hybrid approach for the fabrication of suspended and supported device structures with nanoscale features and highly vertical sidewalls. Functionality of the fabricated devices is proven by measurements of high quality cavity optical modes (Q~1500). Our nanofabrication approach constitutes an advance towards an integrated, monolithic quantum photonics platform based on hBN and other layered vdW materials. △ Less

Submitted 20 September, 2018; originally announced September 2018.

Hexagonal boron nitride cavity optomechanics

Authors: Prasoon K. Shandilya, Johannes E. Fröch, Matthew Mitchell, David P. Lake, Sejeong Kim, Milos Toth, Bishnupada Behera, Chris Healey, Igor Aharonovich, Paul E. Barclay

Abstract: Hexagonal boron nitride (hBN) is an emerging layered material that plays a key role in a variety of two-dimensional devices, and has potential applications in nanophotonics and nanomechanics. Here, we demonstrate the first cavity optomechanical system incorporating hBN. Nanomechanical resonators consisting of hBN beams with predicted thickness between 8 nm and 51 nm were fabricated using electron… ▽ More Hexagonal boron nitride (hBN) is an emerging layered material that plays a key role in a variety of two-dimensional devices, and has potential applications in nanophotonics and nanomechanics. Here, we demonstrate the first cavity optomechanical system incorporating hBN. Nanomechanical resonators consisting of hBN beams with predicted thickness between 8 nm and 51 nm were fabricated using electron beam induced etching and positioned in the optical nearfield of silicon microdisk cavities. A 160 fm/$\sqrt{\text{Hz}}$ sensitivity to the hBN nanobeam motion is demonstrated, allowing observation of thermally driven mechanical resonances with frequencies between 1 and 23 MHz, and mechanical quality factors reaching 1100 at room temperature in high vacuum. In addition, the role of air damping is studied via pressure dependent measurements. Our results constitute an important step towards realizing integrated optomechanical circuits employing hBN. △ Less

Submitted 16 December, 2018; v1 submitted 11 September, 2018; originally announced September 2018.

Comments: Revised version

A random laser based on diamond nanoneedles

Authors: Ngoc My Hanh Duong, Blake Regan, Milos Toth, Igor Aharonovich, Judith M Dawes

Abstract: Random lasers use radiative gain and multiple scatterers in disordered media to generate light amplification. In this study, we demonstrate a random laser based on diamond nanoneedles that act as scatterers in combination with fluorescent dye molecules that serve as a gain medium. Random lasers realized using diamond possess high spectral radiance with angle-free emission and thresholds of 0.16 mJ… ▽ More Random lasers use radiative gain and multiple scatterers in disordered media to generate light amplification. In this study, we demonstrate a random laser based on diamond nanoneedles that act as scatterers in combination with fluorescent dye molecules that serve as a gain medium. Random lasers realized using diamond possess high spectral radiance with angle-free emission and thresholds of 0.16 mJ. The emission dependence on the pillar diameter and density is investigated, and optimum lasing conditions are measured for pillars with spacing and density of 336 nm and ~ 2.9x10^10 cm-2. Our results expand the application space of diamond as a material platform for practical, compact photonic devices and sensing applications. △ Less

Submitted 30 August, 2018; originally announced August 2018.

Bottom up engineering of near-identical quantum emitters in atomically thin materials

Authors: Noah Mendelson, Zai-Quan Xu, Toan Trong Tran, Mehran Kianinia, Carlo Bradac, John Scott, Minh Nguyen, James Bishop, Johannes Froch, Blake Regan, Igor Aharonovich, Milos Toth

Abstract: Quantum technologies require robust and photostable single photon emitters (SPEs) that can be reliably engineered. Hexagonal boron nitride (hBN) has recently emerged as a promising candidate host to bright and optically stable SPEs operating at room temperature. However, the emission wavelength of the fluorescent defects in hBN has, to date, been shown to be uncontrolled. The emitters usually disp… ▽ More Quantum technologies require robust and photostable single photon emitters (SPEs) that can be reliably engineered. Hexagonal boron nitride (hBN) has recently emerged as a promising candidate host to bright and optically stable SPEs operating at room temperature. However, the emission wavelength of the fluorescent defects in hBN has, to date, been shown to be uncontrolled. The emitters usually display a large spread of zero phonon line (ZPL) energies spanning over a broad spectral range (hundreds of nanometers), which hinders the potential development of hBN-based devices and applications. We demonstrate bottom-up, chemical vapor deposition growth of large-area, few layer hBN that hosts large quantities of SPEs: 100 per 10x10 μm2. Remarkably, more than 85 percent of the emitters have a ZPL at (580{\pm}10)nm, a distribution which is over an order of magnitude narrower than previously reported. Exploiting the high density and uniformity of the emitters, we demonstrate electrical modulation and tuning of the ZPL emission wavelength by up to 15 nm. Our results constitute a definite advancement towards the practical deployment of hBN single photon emitters in scalable quantum photonic and hybrid optoelectronic devices based on 2D materials. △ Less

Submitted 4 June, 2018; originally announced June 2018.

Effects of high energy electron irradiation on quantum emitters in hexagonal boron nitride

Authors: Hanh Ngoc My Duong, Minh Anh Phan Nguyen, Mehran Kianinia, Hiroshi Abe, Takeshi Ohshima, Kenji Watanabe, Takashi Taniguchi, James H. Edgar, Igor Aharonovich, Milos Toth

Abstract: Hexagonal Boron Nitride (hBN) mono and multilayers are promising hosts for room temperature single photon emitters (SPEs). In this work we explore high energy (~ MeV) electron irradiation as a means to generate stable SPEs in hBN. We investigate four types of exfoliated hBN flakes - namely, high purity multilayers, isotopically pure hBN, carbon rich hBN multilayers and monolayered material - and f… ▽ More Hexagonal Boron Nitride (hBN) mono and multilayers are promising hosts for room temperature single photon emitters (SPEs). In this work we explore high energy (~ MeV) electron irradiation as a means to generate stable SPEs in hBN. We investigate four types of exfoliated hBN flakes - namely, high purity multilayers, isotopically pure hBN, carbon rich hBN multilayers and monolayered material - and find that electron irradiation increases emitter concentrations dramatically in all samples. Furthermore, the engineered emitters are located throughout hBN flakes (not only at flake edges or grain boundaries), and do not require activation by high temperature annealing of the host material after electron exposure. Our results provide important insights into controlled formation of hBN SPEs and may aid in identification of their crystallographic origin. △ Less

Submitted 10 May, 2018; originally announced May 2018.

Photonic Crystal Cavities from Hexagonal Boron Nitride

Authors: Sejeong Kim, Johannes E. Fröch, Joe Christian, Marcus Straw, James Bishop, Daniel Totonjian, Kenji Watanabe, Takashi Taniguchi, Milos Toth, Igor Aharonovich

Abstract: Development of scalable quantum photonic technologies requires on-chip integration of components such as photonic crystal cavities and waveguides with nonclassical light sources. Recently, hexagonal boron nitride (hBN) has emerged as a promising platform for nanophotonics, following reports of hyperbolic phonon-polaritons and optically stable, ultra-bright quantum emitters. However, exploitation o… ▽ More Development of scalable quantum photonic technologies requires on-chip integration of components such as photonic crystal cavities and waveguides with nonclassical light sources. Recently, hexagonal boron nitride (hBN) has emerged as a promising platform for nanophotonics, following reports of hyperbolic phonon-polaritons and optically stable, ultra-bright quantum emitters. However, exploitation of hBN in scalable, on-chip nanophotonic circuits, quantum information processing and cavity quantum electrodynamics (QED) experiments requires robust techniques for the fabrication of monolithic optical resonators. In this letter, we design and engineer high quality photonic crystal cavities from hBN. We employ two approaches based on a focused ion beam method and a minimally-invasive electron beam induced etching (EBIE) technique to fabricate suspended two dimensional (2D) and one dimensional (1D) cavities with quality (Q) factors in excess of 2,000. Subsequently, we show deterministic, iterative tuning of individual cavities by direct-write, single-step EBIE without significant degradation of the Q-factor. The demonstration of tunable, high Q cavities made from hBN is an unprecedented advance in nanophotonics based on van der Waals materials. Our results and hBN processing methods open up promising new avenues for solid-state systems with applications in integrated quantum photonics, polaritonics and cavity QED experiments. △ Less

Submitted 13 January, 2018; originally announced January 2018.

Single crystal diamond membranes for nanoelectronics

Authors: K. Bray, H. Kato, R. Previdi, R. Sandstrom, K. Ganesan, M. Ogura, T. Makino, S. Yamasaki, A. P. Magyar, M. Toth, I. Aharonovich

Abstract: Single crystal, nanoscale diamond membranes are highly sought after for a variety of applications including nanophotonics, nanoelectronics and quantum information science. However, so far, the availability of conductive diamond membranes remained an unreachable goal. In this work we present a complete nanofabrication methodology for engineering high aspect ratio, electrically active single crystal… ▽ More Single crystal, nanoscale diamond membranes are highly sought after for a variety of applications including nanophotonics, nanoelectronics and quantum information science. However, so far, the availability of conductive diamond membranes remained an unreachable goal. In this work we present a complete nanofabrication methodology for engineering high aspect ratio, electrically active single crystal diamond membranes. The membranes have large lateral directions, exceeding 500x500 um2 and are only several hundreds of nanometers thick. We further realize vertical single crystal p-n junctions, made from the diamond membranes that exhibit onset voltages of ~ 10V and a current of several mA. Moreover, we deterministically introduce optically active color centers into the membranes, and demonstrate for the first time a single crystal nanoscale diamond LED. The robust and scalable approach to engineer the electrically active single crystal diamond membranes, offers new pathways for advanced nanophotonics, nanoelectronics and optomechanics devices employing diamond. △ Less

Submitted 17 October, 2017; originally announced November 2017.

Single Photon Emission from Plasma Treated 2D Hexagonal Boron Nitride

Authors: Zai-Quan Xu, Christopher Elbadawi, Toan Trong Tran, Mehran Kianinia, Xiuling Li, Daobin Liu, Timothy B. Hoffman, Minh Nguyen, Sejeong Kim, James H. Edgar, Xiaojun Wu, Li Song, Sajid Ali, Mike Ford, Milos Toth, Igor Aharonovich

Abstract: Artificial atomic systems in solids are becoming increasingly important building blocks in quantum information processing and scalable quantum nanophotonic networks. Yet, synthesis of color centers that act as single photon emitters which are suitable for on-chip applications is still beyond reach. Here, we report a number of plasma and thermal annealing methods for the fabrication of emitters in… ▽ More Artificial atomic systems in solids are becoming increasingly important building blocks in quantum information processing and scalable quantum nanophotonic networks. Yet, synthesis of color centers that act as single photon emitters which are suitable for on-chip applications is still beyond reach. Here, we report a number of plasma and thermal annealing methods for the fabrication of emitters in tape-exfoliated hexagonal boron nitride (hBN) crystals. A two-step process comprised of Ar plasma etching and subsequent annealing in Ar is highly robust, and yields a seven-fold increase in the concentration of emitters in hBN. The initial plasma etching step generates emitters that suffer from blinking and bleaching, whereas the two-step process yields emitters that are photostable at room temperature and have an emission energy distribution that is red-shifted relative to that of pristine hBN. An analysis of emitters fabricated by a range of plasma and annealing treatments, combined with a theoretical investigation of point defects in hBN indicates that single photon emitters characterized by a high degree of photostability and emission wavelengths greater than ~700 nm are associated with defect complexes that contain oxygen. This is further confirmed by generating the emitters by annealing hBN in an oxidative atmosphere. Our findings advance present understanding of the structure of quantum emitter in hBN and enhance the nanofabrication toolkit that is needed to realize integrated quantum nanophotonics based on 2D materials. △ Less

Submitted 19 October, 2017; originally announced October 2017.

Photophysics of GaN single photon sources in the visible spectral range

Authors: Amanuel M. Berhane, Kwang-Yong Jeong, Carlo Bradac, Michael Walsh, Dirk Englund, Milos Toth, Igor Aharonovich

Abstract: In this work, we present a detailed photophysical analysis of recently-discovered optically stable, single photon emitters (SPEs) in Gallium Nitride (GaN). Temperature-resolved photoluminescence measurements reveal that the emission lines at 4 K are three orders of magnitude broader than the transform-limited widths expected from excited state lifetime measurements. The broadening is ascribed to u… ▽ More In this work, we present a detailed photophysical analysis of recently-discovered optically stable, single photon emitters (SPEs) in Gallium Nitride (GaN). Temperature-resolved photoluminescence measurements reveal that the emission lines at 4 K are three orders of magnitude broader than the transform-limited widths expected from excited state lifetime measurements. The broadening is ascribed to ultra-fast spectral diffusion. Continuing the photophysics study on several emitters at room temperature (RT), a maximum average brightness of ~427 kCounts/s is measured. Furthermore, by determining the decay rates of emitters undergoing three-level optical transitions, radiative and non-radiative lifetimes are calculated at RT. Finally, polarization measurements from 14 emitters are used to determine visibility as well as dipole orientation of defect systems within the GaN crystal. Our results underpin some of the fundamental properties of SPE in GaN both at cryogenic and RT, and define the benchmark for future work in GaN-based single-photon technologies. △ Less

Submitted 30 August, 2017; originally announced August 2017.

Journal ref: Phys. Rev. B 97, 165202 (2018)

Resonant Excitation of Quantum Emitters in Hexagonal Boron Nitride

Authors: Toan Trong Tran, Mehran Kianinia, Minh Nguyen, Sejeong Kim, Zai-Quan Xu, Alexander Kubanek, Milos Toth, Igor Aharonovich

Abstract: Quantum emitters in layered hexagonal boron nitride (hBN) have recently attracted a great attention as promising single photon sources. In this work, we demonstrate resonant excitation of a single defect center in hBN, one of the most important prerequisites for employment of optical sources in quantum information application. We observe spectral linewidths of hBN emitter narrower than 1 GHz while… ▽ More Quantum emitters in layered hexagonal boron nitride (hBN) have recently attracted a great attention as promising single photon sources. In this work, we demonstrate resonant excitation of a single defect center in hBN, one of the most important prerequisites for employment of optical sources in quantum information application. We observe spectral linewidths of hBN emitter narrower than 1 GHz while the emitter experiences spectral diffusion. Temporal photoluminescence measurements reveals an average spectral diffusion time of around 100 ms. On-resonance photon antibunching measurement is also realized. Our results shed light on the potential use of quantum emitters from hBN in nanophotonics and quantum information. △ Less

Submitted 29 August, 2017; originally announced August 2017.

First principles investigation of quantum emission from hBN defects

Authors: Sherif Abdulkader Tawfik, Sajid Ali, Marco Fronzi, Mehran Kianinia, Toan Trong Tran, Catherine Stampfl, Igor Aharonovich, Milos Toth, Michael J. Ford

Abstract: Hexagonal boron nitride (hBN) has recently emerged as a fascinating platform for room-temperature quantum photonics due to the discovery of robust visible light single-photon emitters. In order to utilize these emitters, it is necessary to have a clear understanding of their atomic structure and the associated excitation processes that give rise to this single photon emission. Here we perform dens… ▽ More Hexagonal boron nitride (hBN) has recently emerged as a fascinating platform for room-temperature quantum photonics due to the discovery of robust visible light single-photon emitters. In order to utilize these emitters, it is necessary to have a clear understanding of their atomic structure and the associated excitation processes that give rise to this single photon emission. Here we perform density-functional theory (DFT) and constrained DFT calculations for a range of hBN point defects in order to identify potential emission candidates. By applying a number of criteria on the electronic structure of the ground state and the atomic structure of the excited states of the considered defects, and then calculating the Huang-Rhys (HR) factor, we find that the CBVN defect, in which a carbon atom substitutes a boron atom and the opposite nitrogen atom is removed, is a potential emission source with a HR factor of 1.66, in good agreement with the experimental HR factor. We calculate the photoluminescence (PL) line shape for this defect and find that it reproduces a number of key features in the the experimental PL lineshape. △ Less

Submitted 13 June, 2017; v1 submitted 16 May, 2017; originally announced May 2017.

Atomic Engineering of Single Photon Sources in 2D Boron Nitride Zai-Quan

Authors: Zai-Quan Xu, Christopher Elbadawi, Toan Trong Tran, Mehran Kianinia, Timothy B. Hoffman, James H. Edgar, Milos Toth, Igor Aharonovich

Abstract: Artificial atomic systems in solids such as single photon emitters are becoming increasingly important building blocks in quantum information processing and scalable quantum nanophotonic networks. Here, we report on a controllable way to engineer emitters in two-dimensional (2D) hexagonal boron nitride (hBN) crystals using plasma processing. The method is robust, and yields a 7-fold increase in th… ▽ More Artificial atomic systems in solids such as single photon emitters are becoming increasingly important building blocks in quantum information processing and scalable quantum nanophotonic networks. Here, we report on a controllable way to engineer emitters in two-dimensional (2D) hexagonal boron nitride (hBN) crystals using plasma processing. The method is robust, and yields a 7-fold increase in the density of emitters in hBN, which is promising for their deployment in practical devices. While as-fabricated emitters suffer from blinking and bleaching, a subsequent annealing step yields photo-stable emitters. The presented process is the first step towards controllable placement of quantum emitters in hBN for integrated on-chip quantum nanophotonics based on 2D materials. △ Less

Submitted 8 May, 2017; v1 submitted 17 April, 2017; originally announced April 2017.

Comments: manuscript will be updated later

Room temperature single photon emission from oxidized tungsten disulphide multilayers

Authors: Toan Trong Tran, Sumin Choi, John A. Scott, Zai-quan Xu, Changxi Zheng, Gediminas Seniutinas, Avi Bendavid, Michael S. Fuhrer, Milos Toth, Igor Aharonovich

Abstract: Two dimensional systems offer a unique platform to study light matter interaction at the nanoscale. In this work we report on robust quantum emitters fabricated by thermal oxidation of tungsten disulphide multilayers. The emitters show robust, optically stable, linearly polarized luminescence at room temperature, can be modeled using a three level system, and exhibit moderate bunching. Overall, ou… ▽ More Two dimensional systems offer a unique platform to study light matter interaction at the nanoscale. In this work we report on robust quantum emitters fabricated by thermal oxidation of tungsten disulphide multilayers. The emitters show robust, optically stable, linearly polarized luminescence at room temperature, can be modeled using a three level system, and exhibit moderate bunching. Overall, our results provide important insights into understanding of defect formation and quantum emitter activation in 2D materials. △ Less

Submitted 30 December, 2016; originally announced January 2017.

Emergent pattern formation in an interstitial biofilm

Authors: Cameron Zachreson, Christian Wolff, Cynthia B. Whitchurch, Milos Toth

Abstract: Collective behavior of bacterial colonies plays critical roles in adaptability, survivability, biofilm expansion and infection. We employ an individual-based model of an interstitial biofilm to study emergent pattern formation based on the assumptions that rod-shaped bacteria furrow through a viscous environment, and excrete extracellular polymeric substances which bias their rate of motion. Becau… ▽ More Collective behavior of bacterial colonies plays critical roles in adaptability, survivability, biofilm expansion and infection. We employ an individual-based model of an interstitial biofilm to study emergent pattern formation based on the assumptions that rod-shaped bacteria furrow through a viscous environment, and excrete extracellular polymeric substances which bias their rate of motion. Because the bacteria furrow through their environment, the substratum stiffness is a key control parameter behind the formation of distinct morphological patterns. By systematically varying this property (which we quantify with a stiffness coefficient γ), we show that subtle changes in the substratum stiffness can give rise to a stable state characterized by a high degree of local order and long-range pattern formation. The ordered state exhibits characteristics typically associated with bacterial fitness advantages, even though it is induced by changes in environmental conditions rather than changes in biological parameters. Our findings are applicable to broad range of biofilms and provide insights into the relationship between bacterial movement and their environment, and basic mechanisms behind self-organization of biophysical systems. △ Less

Submitted 15 December, 2016; v1 submitted 13 November, 2016; originally announced November 2016.

Comments: 14 pages, 8 figures, 2 movies

Journal ref: Phys. Rev. E 95, 012408 (2017)

Robust Solid State Quantum System Operating at 800 K

Authors: Mehran Kianinia, Sherif Abdulkader Tawfik, Blake Regan, Toan Trong Tran, Michael J. Ford, Igor Aharonovich, Milos Toth

Abstract: Realization of Quantum information and communications technologies requires robust, stable solid state single photon sources. However, most existing sources cease to function above cryogenic or room temperature due to thermal ionization or strong phonon coupling which impede their emissive and quantum properties. Here we present an efficient single photon source based on a defect in a van der Waal… ▽ More Realization of Quantum information and communications technologies requires robust, stable solid state single photon sources. However, most existing sources cease to function above cryogenic or room temperature due to thermal ionization or strong phonon coupling which impede their emissive and quantum properties. Here we present an efficient single photon source based on a defect in a van der Waals crystal that is optically stable and operates at elevated temperatures of up to 800 K. The quantum nature of the source and the photon purity are maintained upon heating to 800 K and cooling back to room temperature. Our report of a robust high temperature solid state single photon source constitutes a significant step to-wards practical, integrated quantum technologies for real-world environments. △ Less

Submitted 9 November, 2016; originally announced November 2016.

Comments: 9 pages

Bright Room-Temperature Single Photon Emission from Defects in Gallium Nitride

Authors: Amanuel M. Berhane, Kwang-Yong Jeong, Zoltán Bodrog, Saskia Fiedler, Tim Schröder, Noelia Vico Triviño, Tomás Palacios, Adam Gali, Milos Toth, Dirk Englund, Igor Aharonovich

Abstract: Single photon emitters play a central role in many photonic quantum technologies. A promising class of single photon emitters consists of atomic color centers in wide-bandgap crystals, such as diamond silicon carbide and hexagonal boron nitride. However, it is currently not possible to grow these materials as sub-micron thick films on low-refractive index substrates, which is necessary for mature… ▽ More Single photon emitters play a central role in many photonic quantum technologies. A promising class of single photon emitters consists of atomic color centers in wide-bandgap crystals, such as diamond silicon carbide and hexagonal boron nitride. However, it is currently not possible to grow these materials as sub-micron thick films on low-refractive index substrates, which is necessary for mature photonic integrated circuit technologies. Hence, there is great interest in identifying quantum emitters in technologically mature semiconductors that are compatible with suitable heteroepitaxies. Here, we demonstrate robust single photon emitters based on defects in gallium nitride (GaN), the most established and well understood semiconductor that can emit light over the entire visible spectrum. We show that the emitters have excellent photophysical properties including a brightness in excess of 500x10^3 counts/s. We further show that the emitters can be found in a variety of GaN wafers, thus offering reliable and scalable platform for further technological development. We propose a theoretical model to explain the origin of these emitters based on cubic inclusions in hexagonal gallium nitride. Our results constitute a feasible path to scalable, integrated on-chip quantum technologies based on GaN. △ Less

Submitted 15 October, 2016; originally announced October 2016.

Engineering and localization of quantum emitters in large hexagonal boron nitride layers

Authors: Sumin Choi, Toan Trong Tran, Christopher ElBadawi, Charlene Lobo, Xuewen Wang, Saulius Juodkazis, Gediminas Seniutinas, Milos Toth, Igor Aharonovich

Abstract: Hexagonal boron nitride (hBN) is a wide bandgap van der Waals material that has recently emerged as promising platform for quantum photonics experiments. In this work we study the formation and localization of narrowband quantum emitters in large flakes (up to tens of microns wide) of hBN. The emitters can be activated in as-grown hBN by electron irradiation or high temperature annealing, and the… ▽ More Hexagonal boron nitride (hBN) is a wide bandgap van der Waals material that has recently emerged as promising platform for quantum photonics experiments. In this work we study the formation and localization of narrowband quantum emitters in large flakes (up to tens of microns wide) of hBN. The emitters can be activated in as-grown hBN by electron irradiation or high temperature annealing, and the emitter formation probability can be increased by ion implantation or focused laser irradiation of the as-grown material. Interestingly, we show that the emitters are always localized at edges of the flakes, unlike most luminescent point defects in 3D materials. Our results constitute an important step on the road map of deploying hBN in nanophotonics applications. △ Less

Submitted 14 August, 2016; originally announced August 2016.

Robust multicolor single photon emission from point defects in hexagonal boron nitride

Authors: Toan Trong Tran, Christopher ElBadawi, Daniel Totonjian, Charlene J Lobo, Gabriele Grosso, Hyowon Moon, Dirk R. Englund, Michael J. Ford, Igor Aharonovich, Milos Toth

Abstract: Hexagonal boron nitride (hBN) is an emerging two dimensional material for quantum photonics owing to its large bandgap and hyperbolic properties. Here we report a broad range of multicolor room temperature single photon emissions across the visible and the near infrared spectral ranges from point defects in hBN multilayers. We show that the emitters can be categorized into two general groups, but… ▽ More Hexagonal boron nitride (hBN) is an emerging two dimensional material for quantum photonics owing to its large bandgap and hyperbolic properties. Here we report a broad range of multicolor room temperature single photon emissions across the visible and the near infrared spectral ranges from point defects in hBN multilayers. We show that the emitters can be categorized into two general groups, but most likely possess similar crystallographic structure. We further show two approaches for engineering of the emitters using either electron beam irradiation or annealing, and characterize their photophysical properties. The emitters exhibit narrow line widths of sub 10 nm at room temperature, and a short excited state lifetime with high brightness. Remarkably, the emitters are extremely robust and withstand aggressive annealing treatments in oxidizing and reducing environments. Our results constitute the first step towards deterministic engineering of single emitters in 2D materials and hold great promise for the use of defects in boron nitride as sources for quantum information processing and nanophotonics. △ Less

Submitted 31 March, 2016; originally announced March 2016.

Quantum Emission from Defects in Single Crystal Hexagonal Boron Nitride

Authors: Toan Trong Tran, Cameron Zachreson, Amanuel Michael Berhane, Kerem Bray, Russell Guy Sandstrom, Lu Hua Li, Takashi Taniguchi, Kenji Watanabe, Igor Aharonovich, Milos Toth

Abstract: Bulk hexagonal boron nitride (hBN) is a highly nonlinear natural hyperbolic material that attracts major attention in modern nanophotonics applications. However, studies of its optical properties in the visible part of the spectrum and quantum emitters hosted by bulk hBN have not been reported to date. In this work we study the emission properties of hBN crystals in the red spectral range using su… ▽ More Bulk hexagonal boron nitride (hBN) is a highly nonlinear natural hyperbolic material that attracts major attention in modern nanophotonics applications. However, studies of its optical properties in the visible part of the spectrum and quantum emitters hosted by bulk hBN have not been reported to date. In this work we study the emission properties of hBN crystals in the red spectral range using sub-bandgap optical excitation. Quantum emission from defects is observed at room temperature and characterized in detail. Our results advance the use of hBN in quantum nanophotonics technologies and enhance our fundamental understanding of its optical properties. △ Less

Submitted 7 March, 2016; originally announced March 2016.

Comments: In press in Physical Review Applied

Localization of narrowband single photon emitters in nanodiamonds

Authors: Kerem Bray, Russell Sandstrom, Christopher Elbadawi, Martin Fischer, Matthias Schreck, Olga Shimoni, Charlene Lobo, Milos Toth, Igor Aharonovich

Abstract: Diamond nanocrystals that host room temperature narrowband single photon emitters are highly sought after for applications in nanophotonics and bio-imaging. However, current understanding of the origin of these emitters is extremely limited. In this work we demonstrate that the narrowband emitters are point defects localized at extended morphological defects in individual nanodiamonds. In particul… ▽ More Diamond nanocrystals that host room temperature narrowband single photon emitters are highly sought after for applications in nanophotonics and bio-imaging. However, current understanding of the origin of these emitters is extremely limited. In this work we demonstrate that the narrowband emitters are point defects localized at extended morphological defects in individual nanodiamonds. In particular, we show that nanocrystals with defects such as twin boundaries and secondary nucleation sites exhibit narrowband emission that is absent from pristine individual nanocrystals grown under the same conditions. Critically, we prove that the narrowband emission lines vanish when extended defects are removed deterministically using highly localized electron beam induced etching. Our results enhance the current understanding of single photon emitters in diamond, and are directly relevant to fabrication of novel quantum optics devices and sensors. △ Less

Submitted 18 January, 2016; originally announced January 2016.

Emergent formation of dynamic topographic patterns in electron beam induced etching

Authors: Aiden A. Martin, Alan Bahm, James Bishop, Igor Aharonovich, Milos Toth

Abstract: Spontaneous formation of geometric patterns is a fascinating, ubiquitous process that provides fundamental insights into the roles of symmetry breaking, anisotropy and nonlinear interactions in emergent phenomena. Here we report dynamic, highly ordered topographic patterns on the surface of diamond that span multiple length scales and have a symmetry controlled by the chemical species of a precurs… ▽ More Spontaneous formation of geometric patterns is a fascinating, ubiquitous process that provides fundamental insights into the roles of symmetry breaking, anisotropy and nonlinear interactions in emergent phenomena. Here we report dynamic, highly ordered topographic patterns on the surface of diamond that span multiple length scales and have a symmetry controlled by the chemical species of a precursor gas used in electron beam induced etching (EBIE). This behavior reveals an underlying etch rate anisotropy and an electron energy transfer pathway that has been overlooked by existing EBIE theory. We present an etch rate kinetics model that fully explains our results and is universally applicable to EBIE. Our findings can be exploited for controlled wetting, optical structuring and other emerging applications that require nano and micro-scale surface texturing. △ Less

Submitted 19 September, 2015; originally announced September 2015.

Facile Self-Assembly of Quantum Plasmonic Circuit Components

Authors: Toan Trong Tran, Jinghua Fang, Hao Zhang, Patrik Rath, Kerem Bray, Russell Sandstrom, Olga Shimoni, Milos Toth, Igor Aharonovich

Abstract: Efficient coupling between solid state quantum emitters and plasmonic waveguides is important for the realization of integrated circuits for quantum information, communication and sensing. However, realization of plasmonic circuits is still scarce, particularly due to challenges associated with accurate positioning of quantum emitters near plasmonic resonators. Current pathways for the constructio… ▽ More Efficient coupling between solid state quantum emitters and plasmonic waveguides is important for the realization of integrated circuits for quantum information, communication and sensing. However, realization of plasmonic circuits is still scarce, particularly due to challenges associated with accurate positioning of quantum emitters near plasmonic resonators. Current pathways for the construction of plasmonic circuits involve cumbersome and costly methods such as scanning atomic force microscopy or mechanical manipulation, where individual elements are physically relocated using the scanning tip. Here, we introduce a simple, fast and cost effective chemical self-assembly method for the attachment of two primary components of a practical plasmonic circuit: a single photon emitter and a waveguide. Our method enables coupling of nanodiamonds with a single quantum emitter (the nitrogen-vacancy (NV) center) onto the terminal of a silver nanowire, by simply varying the concentration of ascorbic acid (AA) in a reaction solution. The AA concentration is used to control the extent of agglomeration, and can be optimised so as to cause preferential, selective activation of the tips of the nanowires. The nanowire-nanodiamond structures show efficient plasmonic coupling of fluorescence emission from single NV centers into surface plasmon polariton (SPP) modes, evidenced by a more than two-fold reduction in fluorescence lifetime and an increase in fluorescence intensity. △ Less

Submitted 1 August, 2015; originally announced August 2015.

Comments: Published in Advanced Materials on 2 June 2015

Journal ref: Adv. Mater. 2015, 27, 4048