Showing 1–20 of 20 results for author: Lynch, J

Reconfigurable, non-volatile control of optical anisotropy in ReS2 via ferroelectric gating

Authors: Mahfujur Rahaman, Seunguk Song, Aaliyah C. Khan, Bongjun Choi, Aaron M. Schankler, Kwan-Ho Kim, Wonchan Lee, Jason Lynch, Hyeon Suk Shin, Andrew M. Rappe, Deep Jariwala

Abstract: Electrically tunable linear dichroism (LD) with non-volatile properties represents a critical yet elusive feature for next-generation integrated photonic elements in practical device architectures. Here, we demonstrate record-breaking, non-volatile control of optical anisotropy in two-dimensional ReS2 via ferroelectric gating with aluminum scandium nitride (AlScN). Our ferroelectric field-effect t… ▽ More Electrically tunable linear dichroism (LD) with non-volatile properties represents a critical yet elusive feature for next-generation integrated photonic elements in practical device architectures. Here, we demonstrate record-breaking, non-volatile control of optical anisotropy in two-dimensional ReS2 via ferroelectric gating with aluminum scandium nitride (AlScN). Our ferroelectric field-effect transistors achieve near-unity (~95%) LD tunability of differential reflectance at room temperature--the highest reported for any electrically controlled 2D optical system. Crucially, the programmed optical states exhibit exceptional retention exceeding 12,000 seconds without applied bias, enabling true non-volatile optical memory. Through combined experimental characterization and ab initio calculations, we reveal that ferroelectric polarization switching induces substantial asymmetric charge transfer to ReS2, selectively populating conduction band states and triggering structural distortions that dramatically enhance optical anisotropy in the "up" polarization state while leaving the "down" state unperturbed. This ferroelectric-semiconductor coupling provides a universal platform for voltage-programmable, energy-efficient photonic devices with dynamic polarization control, addressing critical needs in integrated photonics as well as programmable far-field optics and telecommunications infrastructure. △ Less

Submitted 15 September, 2025; originally announced September 2025.

Comments: 5 main figures

Accelerating Domain-Aware Electron Microscopy Analysis Using Deep Learning Models with Synthetic Data and Image-Wide Confidence Scoring

Authors: Matthew J. Lynch, Ryan Jacobs, Gabriella Bruno, Priyam Patki, Dane Morgan, Kevin G. Field

Abstract: The integration of machine learning (ML) models enhances the efficiency, affordability, and reliability of feature detection in microscopy, yet their development and applicability are hindered by the dependency on scarce and often flawed manually labeled datasets and a lack of domain awareness. We addressed these challenges by creating a physics-based synthetic image and data generator, resulting… ▽ More The integration of machine learning (ML) models enhances the efficiency, affordability, and reliability of feature detection in microscopy, yet their development and applicability are hindered by the dependency on scarce and often flawed manually labeled datasets and a lack of domain awareness. We addressed these challenges by creating a physics-based synthetic image and data generator, resulting in a machine learning model that achieves comparable precision (0.86), recall (0.63), F1 scores (0.71), and engineering property predictions (R2=0.82) to a model trained on human-labeled data. We enhanced both models by using feature prediction confidence scores to derive an image-wide confidence metric, enabling simple thresholding to eliminate ambiguous and out-of-domain images resulting in performance boosts of 5-30% with a filtering-out rate of 25%. Our study demonstrates that synthetic data can eliminate human reliance in ML and provides a means for domain awareness in cases where many feature detections per image are needed. △ Less

Submitted 2 August, 2024; originally announced August 2024.

Effects of Self-Hybridized Exciton-Polaritons on WS2 Photovoltaics

Authors: Adam D. Alfieri, Tobia Ruth, Cheryl Lim, Jason Lynch, Deep Jariwala

Abstract: Excitonic semiconductors such as transition metal dichalcogenides (TMDCs) are attractive for next-generation photovoltaics (PVs) with low cost, light weight, and low material consumption. In WS2 and other TMDCs, the simultaneous large optical constants and strong exciton resonance can result in the primary photogenerated species being self-hybridized exciton-polaritons emerging from the strong cou… ▽ More Excitonic semiconductors such as transition metal dichalcogenides (TMDCs) are attractive for next-generation photovoltaics (PVs) with low cost, light weight, and low material consumption. In WS2 and other TMDCs, the simultaneous large optical constants and strong exciton resonance can result in the primary photogenerated species being self-hybridized exciton-polaritons emerging from the strong coupling of excitons and optical cavity modes formed by the WS2. We show that strong coupling can benefit photovoltaic performance, with external quantum efficiencies and power conversion efficiencies enhanced by an order of magnitude, approaching values of 55 and 2%, respectively. Thickness dependent device characterization is performed to study the polariton dispersion, revealing anomalous internal quantum efficiency and fill factor behavior that are attributed to polariton-modified exciton transport processes. Our results uncover a significant mechanism in the photoconversion process for PVs from high index, excitonic semiconductors and indicate the utility of strong coupling for optoelectronic devices. △ Less

Submitted 21 October, 2024; v1 submitted 18 June, 2024; originally announced June 2024.

Ultrastrong Light-Matter Coupling in 2D Metal-Chalcogenates

Authors: Surendra B. Anantharaman, Jason Lynch, Mariya Aleksich, Christopher E. Stevens, Christopher Munley, Bongjun Choi, Sridhar Shenoy, Thomas Darlington, Arka Majumdar, P. James Shuck, Joshua Hendrickson, J. Nathan Hohman, Deep Jariwala

Abstract: Hybridization of excitons with photons to form hybrid quasiparticles, exciton-polaritons (EPs), has been widely investigated in a range of semiconductor material systems coupled to photonic cavities. Self-hybridization occurs when the semiconductor itself can serve as the photonic cavity medium resulting in strongly-coupled EPs with Rabi splitting energies > 200 meV at room temperatures which rece… ▽ More Hybridization of excitons with photons to form hybrid quasiparticles, exciton-polaritons (EPs), has been widely investigated in a range of semiconductor material systems coupled to photonic cavities. Self-hybridization occurs when the semiconductor itself can serve as the photonic cavity medium resulting in strongly-coupled EPs with Rabi splitting energies > 200 meV at room temperatures which recently were observed in layered two-dimensional (2D) excitonic materials. Here, we report an extreme version of this phenomenon, an ultrastrong EP coupling, in a nascent, 2D excitonic system, the metal organic chalcogenate (MOCHA) compound named mithrene. The resulting self-hybridized EPs in mithrene crystals placed on Au substrates show Rabi Splitting in the ultrastrong coupling range (> 600 meV) due to the strong oscillator strength of the excitons concurrent with the large refractive indices of mithrene. We further show bright EP emission at room temperature as well as EP dispersions at low-temperatures. Importantly, we find lower EP emission linewidth narrowing to ~1 nm when mithrene crystals are placed in closed Fabry-Perot cavities. Our results suggest that MOCHA materials are ideal for polaritonics in the deep green-blue part of the spectrum where strong excitonic materials with large optical constants are notably scarce. △ Less

Submitted 21 August, 2023; originally announced August 2023.

Wafer-scale growth of two-dimensional, phase-pure InSe

Authors: Seunguk Song, Sungho Jeon, Mahfujur Rahaman, Jason Lynch, Pawan Kumar, Srikrishna Chakravarthi, Gwangwoo Kim, Xingyu Du, Eric Blanton, Kim Kisslinger, Michael Snure, Nicholas R. Glavin, Eric A. Stach, Roy H. Olsson, Deep Jariwala

Abstract: Two-dimensional (2D) indium monoselenide (InSe) has attracted significant attention as a III-VI two-dimensional semiconductor (2D) with a combination of favorable attributes from III-V semiconductors as well as van der Waals 2D transition metal dichalcogenides. Nevertheless, the large-area synthesis of phase-pure 2D InSe remains unattained due to the complexity of the binary In-Se system and the d… ▽ More Two-dimensional (2D) indium monoselenide (InSe) has attracted significant attention as a III-VI two-dimensional semiconductor (2D) with a combination of favorable attributes from III-V semiconductors as well as van der Waals 2D transition metal dichalcogenides. Nevertheless, the large-area synthesis of phase-pure 2D InSe remains unattained due to the complexity of the binary In-Se system and the difficulties in promoting lateral growth. Here, we report the first polymorph-selective synthesis of epitaxial 2D InSe by metal-organic chemical deposition (MOCVD) over 2 inch diameter sapphire wafers. We achieve thickness-controlled, layer-by-layer epitaxial growth of InSe on c-plane sapphire via dynamic pulse control of Se/In flux ratio. The layer-by-layer growth allows thickness control over wafer scale with tunable optical properties comparable to bulk crystals. Finally, the gate-tunable electrical transport suggests that MOCVD-grown InSe could be a potential channel material for back-end-of-line integration in logic transistors with field-effect mobility comparable to single-crystalline flakes. △ Less

Submitted 4 March, 2023; originally announced March 2023.

Comments: MS + SI

Charge and Energy Transfer Dynamics of Hybridized Exciton-Polaritons in 2D Halide Perovskites

Authors: Surendra B. Anantharaman, Jason Lynch, Christopher E. Stevens, Christopher Munley, Chentao Li, Jin Hou, Hao Zhang, Andrew Torma, Thomas Darlington, Francis Coen, Kevin Li, Arka Majumdar, P. James Schuck, Aditya Mohite, Hayk Harutyunyan, Joshua R. Hendrickson, Deep Jariwala

Abstract: Excitons, bound electron-hole pairs, in Two-Dimensional Hybrid Organic Inorganic Perovskites (2D HOIPs) are capable of forming hybrid light-matter states known as exciton-polaritons (E-Ps) when the excitonic medium is confined in an optical cavity. In the case of 2D HOIPs, they can self-hybridize into E-Ps at specific thicknesses of the HOIP crystals that form a resonant optical cavity with the ex… ▽ More Excitons, bound electron-hole pairs, in Two-Dimensional Hybrid Organic Inorganic Perovskites (2D HOIPs) are capable of forming hybrid light-matter states known as exciton-polaritons (E-Ps) when the excitonic medium is confined in an optical cavity. In the case of 2D HOIPs, they can self-hybridize into E-Ps at specific thicknesses of the HOIP crystals that form a resonant optical cavity with the excitons. However, the fundamental properties of these self-hybridized E-Ps in 2D HOIPs, including their role in ultrafast energy and/or charge transfer at interfaces, remain unclear. Here, we demonstrate that > 0.5 um thick 2D HOIP crystals on Au substrates are capable of supporting multiple-orders of self-hybridized E-P modes. These E-Ps have high Q factors (> 100) and modulate the optical dispersion for the crystal to enhance sub-gap absorption and emission. Through varying excitation energy and ultrafast measurements, we also confirm energy transfer from higher energy upper E-Ps to lower energy, lower E-Ps. Finally, we also demonstrate that E-Ps are capable of charge transport and transfer at interfaces. Our findings provide new insights into charge and energy transfer in E-Ps opening new opportunities towards their manipulation for polaritonic devices. △ Less

Submitted 18 February, 2023; originally announced February 2023.

Comments: 5 figures plus supporting information

How Good Can 2D Excitonic Solar Cells Be?

Authors: Zekun Hu, Da Lin, Jason Lynch, Kevin Xu, Deep Jariwala

Abstract: Excitonic semiconductors have been a subject of research for photovoltaic applications for many decades. Among them, the organic polymers and small molecules based solar cells have now exceeded 19% power conversion efficiency (PCE). While organic photovoltaics (OPVs) are approaching maturity, the advent of strongly excitonic inorganic semiconductors such as two-dimensional transition metal dichalc… ▽ More Excitonic semiconductors have been a subject of research for photovoltaic applications for many decades. Among them, the organic polymers and small molecules based solar cells have now exceeded 19% power conversion efficiency (PCE). While organic photovoltaics (OPVs) are approaching maturity, the advent of strongly excitonic inorganic semiconductors such as two-dimensional transition metal dichalcogenides (TMDCs) has renewed interest in excitonic solar cells due to their high-optical constants, stable inorganic structure and sub-nm film thicknesses. While several reports have been published on TMDC based PVs, achieving power conversion efficiencies higher than 6% under one-sun AM1.5G illumination has remained challenging. Here, we perform a full optical and electronic analysis of design, structure and performance of monolayer TMDC based, single-junction excitonic PVs. Our computational model with optimized properties predicts a PCE of 9.22% in a superlattice device structure. Our analysis suggests that, while the PCE for 2D excitonic solar cells may be limited to < 10%, a specific power > 100 W g-1 may be achieved with our proposed designs, making them attractive in aerospace, distributed remote sensing, and wearable electronics. △ Less

Submitted 9 February, 2023; originally announced February 2023.

Comments: Manuscript plus supplement

Self-driving Multimodal Studies at User Facilities

Authors: Phillip M. Maffettone, Daniel B. Allan, Stuart I. Campbell, Matthew R. Carbone, Thomas A. Caswell, Brian L. DeCost, Dmitri Gavrilov, Marcus D. Hanwell, Howie Joress, Joshua Lynch, Bruce Ravel, Stuart B. Wilkins, Jakub Wlodek, Daniel Olds

Abstract: Multimodal characterization is commonly required for understanding materials. User facilities possess the infrastructure to perform these measurements, albeit in serial over days to months. In this paper, we describe a unified multimodal measurement of a single sample library at distant instruments, driven by a concert of distributed agents that use analysis from each modality to inform the direct… ▽ More Multimodal characterization is commonly required for understanding materials. User facilities possess the infrastructure to perform these measurements, albeit in serial over days to months. In this paper, we describe a unified multimodal measurement of a single sample library at distant instruments, driven by a concert of distributed agents that use analysis from each modality to inform the direction of the other in real time. Powered by the Bluesky project at the National Synchrotron Light Source II, this experiment is a world's first for beamline science, and provides a blueprint for future approaches to multimodal and multifidelity experiments at user facilities. △ Less

Submitted 22 January, 2023; originally announced January 2023.

Comments: 36th Conference on Neural Information Processing Systems (NeurIPS 2022). AI4Mat Workshop

Ultrathin Broadband Metasurface Superabsorbers from a van der Waals Semimetal

Authors: Adam D. Alfieri, Michael J. Motala, Michael Snure, Jason Lynch, Pawan Kumar, Huiqin Zhang, Susanna Post, Christopher Muratore, Joshua R. Hendrickson, Nicholas R. Glavin, Deep Jariwala

Abstract: Metamaterials and metasurfaces operating in the visible and near-infrared (NIR) offer a promising route towards next-generation photodetectors and devices for solar energy harvesting. While numerous metamaterials and metasurfaces using metals and semiconductors have been demonstrated, semimetals-based metasurfaces in the vis-NIR range are notably missing. Here, we experimentally demonstrate a broa… ▽ More Metamaterials and metasurfaces operating in the visible and near-infrared (NIR) offer a promising route towards next-generation photodetectors and devices for solar energy harvesting. While numerous metamaterials and metasurfaces using metals and semiconductors have been demonstrated, semimetals-based metasurfaces in the vis-NIR range are notably missing. Here, we experimentally demonstrate a broadband metasurface superabsorber based on large area, semimetallic, van der Waals PtSe2 thin films in agreement with electromagnetic simulations. Our results show that PtSe2 is an ultrathin and scalable semimetal that concurrently possesses high index and high extinction across the vis-NIR range. Consequently, the thin-film PtSe2 on a reflector separated by a dielectric spacer can absorb > 85 % for the unpatterned case and ~97 % for the optimized 2D metasurface in the 400-900 nm range making it one of the strongest and thinnest broadband perfect absorbers to date. Our results present a scalable approach to photodetection and solar energy harvesting, demonstrating the practical utility of high index, high extinction semimetals for nanoscale optics. △ Less

Submitted 28 August, 2022; originally announced August 2022.

Direct Nano-Imaging of Light-Matter Interactions in Nanoscale Excitonic Emitters

Authors: Kiyoung Jo, Emanuele Marino, Jason Lynch, Zhiqiao Jiang, Natalie Gogotsi, Thomas P. Darlington, Mohammad Soroush, P. James Schuck, Nicholas J. Borys, Christopher Murray, Deep Jariwala

Abstract: Strong light-matter interactions in localized nano-emitters when placed near metallic mirrors have been widely reported via spectroscopic studies in the optical far-field. Here, we report a near-field nano-spectroscopic study of the localized nanoscale emitters on a flat Au substrate. We observe strong-coupling of the excitonic dipoles in quasi 2-dimensional CdSe/CdxZnS1-xS nanoplatelets with gap… ▽ More Strong light-matter interactions in localized nano-emitters when placed near metallic mirrors have been widely reported via spectroscopic studies in the optical far-field. Here, we report a near-field nano-spectroscopic study of the localized nanoscale emitters on a flat Au substrate. We observe strong-coupling of the excitonic dipoles in quasi 2-dimensional CdSe/CdxZnS1-xS nanoplatelets with gap mode plasmons formed between the Au tip and substrate. We also observe directional propagation on the Au substrate of surface plasmon polaritons launched from the excitons of the nanoplatelets as wave-like fringe patterns in the near-field photoluminescence maps. These fringe patterns were confirmed via extensive electromagnetic wave simulations to be standing-waves formed between the tip and the emitter on the substrate plane. We further report that both light confinement and the in-plane emission can be engineered by tuning the surrounding dielectric environment of the nanoplatelets. Our results lead to renewed understanding of in-plane, near-field electromagnetic signal transduction from the localized nano-emitters with profound implications in nano and quantum photonics as well as resonant optoelectronics. △ Less

Submitted 20 August, 2022; originally announced August 2022.

Comments: manuscript + supporting information

Tutorial: Exciton resonances for atomically-thin optics

Authors: Jason Lynch, Ludovica Guarneri, Deep Jariwala, Jorik van de Groep

Abstract: Metasurfaces enable flat optical elements by leveraging optical resonances in metallic or dielectric nanoparticles to obtain accurate control over the amplitude and phase of the scattered light. While highly efficient, these resonances are static and difficult to tune actively. Exciton resonances in atomically thin 2D semiconductors provide a novel and uniquely strong resonant light-matter interac… ▽ More Metasurfaces enable flat optical elements by leveraging optical resonances in metallic or dielectric nanoparticles to obtain accurate control over the amplitude and phase of the scattered light. While highly efficient, these resonances are static and difficult to tune actively. Exciton resonances in atomically thin 2D semiconductors provide a novel and uniquely strong resonant light-matter interaction, which presents a new opportunity for optical metasurfaces. Their resonant properties are intrinsic to the band structure of the material and do not rely on nanoscale patterns and are highly tunable using external stimuli. In this tutorial, we present the role that excitons resonances can play for atomically-thin optics. We describe the essentials of metasurface physics, provide a background on exciton physics, as well as a comprehensive overview of excitonic materials. Excitons demonstrate to provide new degrees of freedom and enhanced light-matter interactions in hybrid metasurfaces through coupling with metallic and dielectric metasurfaces. Using the high sensitivity of excitons to the medium's electron density, the first demonstrations of electrically-tunable nanophotonic devices and atomically-thin optical elements are also discussed. The future of excitons in metasurfaces looks promising, while the main challenge lies in large-area growth and precise integration of high-quality materials. △ Less

Submitted 24 June, 2022; originally announced June 2022.

Journal ref: Journal of Applied Physics 132, 091102 (2022)

Cavity-Enhanced Raman Scattering from 2D Hybrid Perovskites

Authors: Aditya Singh, Jason Lynch, Surendra B. Anantharaman, Jin Hou, Simrjit Singh, Gwangwoo Kim, Aditya D. Mohite, Rajendra Singh, Deep Jariwala

Abstract: Two-dimensional (2D) hybrid organic-inorganic perovskites (HOIPs) are promising candidates for optoelectronic applications due to their efficient light emission properties, and strong dielectric confinement effects. Raman spectroscopy is a versatile, non-contact and often non-destructive technique, widely used to characterize crystalline materials. However, the inherently weak phonon scattering, s… ▽ More Two-dimensional (2D) hybrid organic-inorganic perovskites (HOIPs) are promising candidates for optoelectronic applications due to their efficient light emission properties, and strong dielectric confinement effects. Raman spectroscopy is a versatile, non-contact and often non-destructive technique, widely used to characterize crystalline materials. However, the inherently weak phonon scattering, strong background, and complex nature of the Raman signals from HOIPs present challenges in obtaining reliable signals. Further, the fragile nature of the 2D HOIP crystals results in rapid degradation upon exposure to heat, light and moisture, which presents further difficulty in enhancing Raman scattered photon signals. Herein, we report a novel approach to enhance the weak Raman scattering signals in Ruddlesden-Popper (RP) phase HOIPs by introducing an open-cavity comprising HOIP crystals on a gold substrate. We observe 15x enhancement of the Raman signals due to the Purcell effect inside the high-index HOIP crystals. Our simple approach can be extended to enhance the study of phonon scattering in other HOIP and van der Waals layered crystals. △ Less

Submitted 8 March, 2022; originally announced March 2022.

Comments: 4 figures + supporting

Scalable synthesis of 2D van der Waals superlattices

Authors: Michael J. Motala, Xiang Zhang, Pawan Kumar, Eliezer F. Oliveira, Anna Benton, Paige Miesle, Rahul Rao, Peter R. Stevenson, David Moore, Adam Alfieri, Jason Lynch, Guanhui Gao, Sijie Ma, Hanyu Zhu, Zhe Wang, Ivan Petrov, Eric A. Stach, W. Joshua Kennedy, Shiva Vengala, James M. Tour, Douglas S. Galvao, Deep Jariwala, Christopher Muratore, Michael Snure, Pulickel M. Ajayan , et al. (1 additional authors not shown)

Abstract: Heterostructure materials form the basis of much of modern electronics, from transistors to lasers and light-emitting diodes. Recent years have seen a renewed focus on creating heterostructures through the vertical integration of two-dimensional materials, including graphene, hexagonal boron nitride, and transition metal dichalcogenides (TMDCs). However, fundamental challenges associated with mate… ▽ More Heterostructure materials form the basis of much of modern electronics, from transistors to lasers and light-emitting diodes. Recent years have seen a renewed focus on creating heterostructures through the vertical integration of two-dimensional materials, including graphene, hexagonal boron nitride, and transition metal dichalcogenides (TMDCs). However, fundamental challenges associated with materials processing have limited material quality and impeded scalability. We demonstrate a method to convert sub-nanometer metal films deposited on silicon and sapphire into TMDC heterostructures through vapor-phase processing. The resulting heterostructures and superlattices exhibit novel properties compared with stand-alone TMDCs, including reduced bandgap, enhanced light-matter coupling, and improved catalytic performance. This robust and scalable synthetic method provides new opportunities to generate a wide range of artificially stacked 2D superlattices with controlled morphology and composition. △ Less

Submitted 4 November, 2021; originally announced November 2021.

Self-Hybridized Polaritonic Emission from Layered Perovskites

Authors: Surendra B. Anantharaman, Christopher E. Stevens, Jason Lynch, Baokun Song, Jin Hou, Huiqin Zhang, Kiyoung Jo, Pawan Kumar, Jean-Christophe Blancon, Aditya D. Mohite, Joshua R. Hendrickson, Deep Jariwala

Abstract: Light-matter coupling in excitonic materials has been the subject of intense investigation due to emergence of new excitonic materials. Two-dimensional layered hybrid organic/inorganic perovskites (2D HOIPs) support strongly bound excitons at room-temperatures with some of the highest oscillator strengths and electric loss tangents among the known excitonic materials. Here, we report strong light-… ▽ More Light-matter coupling in excitonic materials has been the subject of intense investigation due to emergence of new excitonic materials. Two-dimensional layered hybrid organic/inorganic perovskites (2D HOIPs) support strongly bound excitons at room-temperatures with some of the highest oscillator strengths and electric loss tangents among the known excitonic materials. Here, we report strong light-matter coupling in Ruddlesden-Popper phase 2D-HOIPs crystals without the necessity of an external cavity. We report concurrent occurrence of multiple-orders of hybrid light-matter states via both reflectance and luminescence spectroscopy in thick (> 100 nm) crystals and near-unity absorption in thin (< 20 nm) crystals. We observe resonances with quality factors > 250 in hybridized exciton-polaritons and identify a linear correlation between exciton-polariton mode splitting and extinction coefficient of the various 2D-HOIPs. Our work opens the door to studying polariton dynamics in self-hybridized and open cavity systems with broad applications in optoelectronics and photochemistry. △ Less

Submitted 13 May, 2021; originally announced May 2021.

Journal ref: Nano Letters 2021

Current Overview of Statistical Fiber Bundles Model and Its Application to Physics-based Reliability Analysis of Thin-film Dielectrics

Authors: James U. Gleaton, David Han, James D. Lynch, Hon Keung Tony Ng, Fabrizio Ruggeri

Abstract: In this paper, we present a critical overview of statistical fiber bundles models. We discuss relevant aspects, like assumptions and consequences stemming from models in the literature and propose new ones. This is accomplished by concentrating on both the physical and statistical aspects of a specific load-sharing example, the breakdown (BD) for circuits of capacitors and related dielectrics. For… ▽ More In this paper, we present a critical overview of statistical fiber bundles models. We discuss relevant aspects, like assumptions and consequences stemming from models in the literature and propose new ones. This is accomplished by concentrating on both the physical and statistical aspects of a specific load-sharing example, the breakdown (BD) for circuits of capacitors and related dielectrics. For series and parallel/series circuits (series/parallel reliability systems) of ordinary capacitors, the load-sharing rules are derived from the electrical laws. This with the BD formalism is then used to obtain the BD distribution of the circuit. The BD distribution and Gibbs measure are given for a series circuit and the size effects are illustrated for simulations of series and parallel/series circuits. This is related to the finite weakest link adjustments for the BD distribution that arise in large series/parallel reliability load-sharing systems, such as dielectric BD, from their extreme value approximations. An elementary but in-depth discussion of the physical aspects of SiO$_2$ and HfO$_2$ dielectrics and cell models is given. This is used to study a load-sharing cell model for the BD of HfO$_2$ dielectrics and the BD formalism. The latter study is based on an analysis of Kim and Lee (2004)'s data for such dielectrics. Here, several BD distributions are compared in the analysis and proportional hazard regression models are used to study the BD formalism. In addition, some areas of open research are discussed. △ Less

Submitted 25 January, 2023; v1 submitted 9 April, 2021; originally announced April 2021.

Comments: The majority of the materials in the paper has been published as a book

Light-Matter Coupling in Scalable Van der Waals Superlattices

Authors: Pawan Kumar, Jason Lynch, Baokun Song, Haonan Ling, Francisco Barrera, Huiqin Zhang, Surendra B. Anantharaman, Jagrit Digani, Haoyue Zhu, Tanushree H. Choudhury, Clifford McAleese, Xiaochen Wang, Ben R. Conran, Oliver Whear, Michael J. Motala, Michael Snure, Christopher Muratore, Joan M. Redwing, Nicholas R. Glavin, Eric A. Stach, Artur R. Davoyan, Deep Jariwala

Abstract: Two-dimensional (2D) crystals have renewed opportunities in design and assembly of artificial lattices without the constraints of epitaxy. However, the lack of thickness control in exfoliated van der Waals (vdW) layers prevents realization of repeat units with high fidelity. Recent availability of uniform, wafer-scale samples permits engineering of both electronic and optical dispersions in stacks… ▽ More Two-dimensional (2D) crystals have renewed opportunities in design and assembly of artificial lattices without the constraints of epitaxy. However, the lack of thickness control in exfoliated van der Waals (vdW) layers prevents realization of repeat units with high fidelity. Recent availability of uniform, wafer-scale samples permits engineering of both electronic and optical dispersions in stacks of disparate 2D layers with multiple repeating units. We present optical dispersion engineering in a superlattice structure comprised of alternating layers of 2D excitonic chalcogenides and dielectric insulators. By carefully designing the unit cell parameters, we demonstrate > 90 % narrowband absorption in < 4 nm active layer excitonic absorber medium at room temperature, concurrently with enhanced photoluminescence in cm2 samples. These superlattices show evidence of strong light-matter coupling and exciton-polariton formation with geometry-tunable coupling constants. Our results demonstrate proof of concept structures with engineered optical properties and pave the way for a broad class of scalable, designer optical metamaterials from atomically-thin layers. △ Less

Submitted 25 March, 2021; originally announced March 2021.

Comments: 4 figures + supporting

Nanosheet-stabilized emulsions: ultra-low loading segregated networks and surface energy determination of pristine few-layer 2D materials

Authors: Sean P. Ogilvie, Matthew J. Large, Adam J. Cass, Aline Amorim Graf, Anne C. Sehnal, Marcus A. O'Mara, Peter J. Lynch, Jonathan P. Salvage, Marco Alfonso, Philippe Poulin, Alice A. K. King, Alan B. Dalton

Abstract: A framework is developed to allow emulsification to be used to fabricate functional structures from, and study the properties of, pristine layered nanosheets. Liquid-exfoliated few-layer graphene and MoS2 are demonstrated to stablize emulsions which exhibit system-scale electrical conductivity at ultra-low nanosheet volume fractions. When deposited on a substrate, the controlled drying dynamics of… ▽ More A framework is developed to allow emulsification to be used to fabricate functional structures from, and study the properties of, pristine layered nanosheets. Liquid-exfoliated few-layer graphene and MoS2 are demonstrated to stablize emulsions which exhibit system-scale electrical conductivity at ultra-low nanosheet volume fractions. When deposited on a substrate, the controlled drying dynamics of these emulsions facilitates their application as inks where the lack of any coffee ring effect allows manual deposition of high conductivity films. In order to broaden the range of compositions and subsequently applications, an understanding of emulsion stability and orientation in terms of surface energy of the three phases is developed. Importantly, this model facilitates determination of the surface energies of the nanosheets themselves and subsequently allows design of emulsions. Finally, emulsification by surfactant-exfoliated nanosheets and emulsion inversion using basic solution are demonstrated to allow water-based processing where composition and orientation can be tailored to enable applications. △ Less

Submitted 13 May, 2020; originally announced May 2020.

Dynamics and structure of an aging binary colloidal glass

Authors: Jennifer M. Lynch, Gianguido C. Cianci, Eric R. Weeks

Abstract: We study aging in a colloidal suspension consisting of micron-sized particles in a liquid. This system is made glassy by increasing the particle concentration. We observe samples composed of particles of two sizes, with a size ratio of 1:2.1 and a volume fraction ratio 1:6, using fast laser scanning confocal microscopy. This technique yields real-time, three-dimensional movies deep inside the co… ▽ More We study aging in a colloidal suspension consisting of micron-sized particles in a liquid. This system is made glassy by increasing the particle concentration. We observe samples composed of particles of two sizes, with a size ratio of 1:2.1 and a volume fraction ratio 1:6, using fast laser scanning confocal microscopy. This technique yields real-time, three-dimensional movies deep inside the colloidal glass. Specifically, we look at how the size, motion and structural organization of the particles relate to the overall aging of the glass. Particles move in spatially heterogeneous cooperative groups. These mobile regions tend to be richer in small particles, and these small particles facilitate the motion of nearby particles of both sizes. △ Less

Submitted 23 August, 2008; v1 submitted 3 July, 2008; originally announced July 2008.

Comments: 7 pages; submitted to Phys. Rev. E. Revised with 1 new figure, improved text

Journal ref: Phys. Rev. E 78, 031410 (2008)

Differential Charge Sensing and Charge Delocalization in a Tunable Double Quantum Dot

Authors: L. DiCarlo, H. J. Lynch, A. C. Johnson, L. I. Childress, K. Crockett, C. M. Marcus, M. P. Hanson, A. C. Gossard

Abstract: We report measurements of a tunable double quantum dot, operating in the quantum regime, with integrated local charge sensors. The spatial resolution of the sensors is sufficient to allow the charge distribution within the double dot system to be resolved at fixed total charge. We use this readout scheme to investigate charge delocalization as a function of temperature and strength of tunnel cou… ▽ More We report measurements of a tunable double quantum dot, operating in the quantum regime, with integrated local charge sensors. The spatial resolution of the sensors is sufficient to allow the charge distribution within the double dot system to be resolved at fixed total charge. We use this readout scheme to investigate charge delocalization as a function of temperature and strength of tunnel coupling, showing that local charge sensing allows an accurate determination of interdot tunnel coupling in the absence of transport. △ Less

Submitted 7 February, 2004; v1 submitted 13 November, 2003; originally announced November 2003.

Comments: related papers at http://marcuslab.harvard.edu

Journal ref: Phys. Rev. Lett. 92, 226801 (2004)

The Low-Temperature Fate of the 0.7 Structure in a Point Contact: A Kondo-like Correlated State in an Open System

Authors: S. M. Cronenwett, H. J. Lynch, D. Goldhaber-Gordon, L. P. Kouwenhoven, C. M. Marcus, K. Hirose, N. S. Wingreen, V. Umansky

Abstract: Besides the usual conductance plateaus at multiples of 2e2/h, quantum point contacts typically show an extra plateau at ~ 0.7(2e2/h), believed to arise from electron-electron interactions that prohibit the two spin channels from being simultaneously occupied. We present evidence that the disappearance of the 0.7 structure at very low temperature signals the formation of a Kondo-like correlated s… ▽ More Besides the usual conductance plateaus at multiples of 2e2/h, quantum point contacts typically show an extra plateau at ~ 0.7(2e2/h), believed to arise from electron-electron interactions that prohibit the two spin channels from being simultaneously occupied. We present evidence that the disappearance of the 0.7 structure at very low temperature signals the formation of a Kondo-like correlated spin state. Evidence includes a zero-bias conductance peak that splits in a parallel field, scaling of conductance to a modified Kondo form, and consistency between peak width and the Kondo temperature. △ Less

Submitted 31 January, 2002; originally announced January 2002.

Journal ref: Phys. Rev. Lett. 88, 226805 (2002).