Classification of features in a scene typically requires conversion of the incoming photonic field int the electronic domain. Recently, an alternative approach has emerged whereby passive structured materials can perform classification tasks by directly using free-space propagation and diffraction of light. In this manuscript, we present a theoretical and computational study of such systems and establish the basic features that govern their performance. We show that system architecture, material structure, and input light field are intertwined and need to be co-designed to maximize classification accuracy. Our simulations show that a single layer metasurface can achieve classification accuracy better than conventional linear classifiers, with an order of magnitude fewer diffractive features than previously reported. For a wavelength λ, single layer metasurfaces of size 100λ x 100λ with aperture density λ-2 achieve ~96% testing accuracy on the MNIST dataset, for an optimized distance ~100λ to the output plane. This is enabled by an intrinsic nonlinearity in photodetection, despite the use of linear optical metamaterials. Furthermore, we find that once the system is optimized, the number of diffractive features is the main determinant of classification performance. The slow asymptotic scaling with the number of apertures suggests a reason why such systems may benefit from multiple layer designs. Finally, we show a trade-off between the number of apertures and fabrication noise.
Typical approaches to classify scenes from light convert the light field to electrons to perform the computation in the digital electronic domain. This conversion and downstream computational analysis require significant power and time. Diffractive neural networks have recently emerged as unique systems to classify optical fields at lower energy and high speeds. Previous work has shown that a single layer of diffractive metamaterial can achieve high performance on classification tasks. In analogy with electronic neural networks, it is anticipated that multilayer diffractive systems would provide better performance, but the fundamental reasons for the potential improvement have not been established. In this work, we present extensive computational simulations of two - layer diffractive neural networks and show that they can achieve high performance with fewer diffractive features than single layer systems.
This project aimed to identify the performance-limiting mechanisms in mid- to far infrared (IR) sensors by probing photogenerated free carrier dynamics in model detector materials using scanning ultrafast electron microscopy (SUEM). SUEM is a recently developed method based on using ultrafast electron pulses in combination with optical excitations in a pump- probe configuration to examine charge dynamics with high spatial and temporal resolution and without the need for microfabrication. Five material systems were examined using SUEM in this project: polycrystalline lead zirconium titanate (a pyroelectric), polycrystalline vanadium dioxide (a bolometric material), GaAs (near IR), InAs (mid IR), and Si/SiO 2 system as a prototypical system for interface charge dynamics. The report provides detailed results for the Si/SiO 2 and the lead zirconium titanate systems.
Classification of features in a scene typically requires conversion of the incoming photonic field into the electronic domain. Recently, an alternative approach has emerged whereby passive structured materials can perform classification tasks by directly using free-space propagation and diffraction of light. In this manuscript, we present a theoretical and computational study of such systems and establish the basic features that govern their performance. We show that system architecture, material structure, and input light field are intertwined and need to be co-designed to maximize classification accuracy. Our simulations show that a single layer metasurface can achieve classification accuracy better than conventional linear classifiers, with an order of magnitude fewer diffractive features than previously reported. For a wavelength λ, single layer metasurfaces of size 100λ × 100λ with an aperture density λ-2 achieve ∼96% testing accuracy on the MNIST data set, for an optimized distance ∼100λ to the output plane. This is enabled by an intrinsic nonlinearity in photodetection, despite the use of linear optical metamaterials. Furthermore, we find that once the system is optimized, the number of diffractive features is the main determinant of classification performance. The slow asymptotic scaling with the number of apertures suggests a reason why such systems may benefit from multiple layer designs. Finally, we show a trade-off between the number of apertures and fabrication noise.
Advanced GaN power devices are promising for many applications in high power electronics but performance limitations due to material quality in etched-and-regrown junctions prevent their widespread use. Carrier diffusion length is a critical parameter that not only determines device performance but is also a diagnostic of material quality. Here we present the use of electron-beam induced current to measure carrier diffusion lengths in continuously grown and etched-and-regrown GaN pin diodes as models for interfaces in more complex devices. Variations in the quality of the etched-and-regrown junctions are observed and shown to be due to the degradation of the n-type material. We observe an etched-and-regrown junction with properties comparable to a continuously grown junction.
Single-photon detectors have typically consisted of macroscopic materials where both the photon absorption and transduction to an electrical signal happen. Newly proposed designs suggest that large arrays of nanoscale detectors could provide improved performance in addition to decoupling the absorption and transduction processes. Here we study the properties of such a detector consisting of a nanoscale superconducting (SC) transport channel functionalized by a photon absorber. We explore two detection mechanisms based on photoinduced electrostatic gating and magnetic effects. To this end we model the narrow channel as a one-dimensional atomic chain and use a self-consistent Keldysh-Nambu Green's function formalism to describe nonequilibrium effects and SC phenomena. We consider cases where the photon creates electrostatic and magnetic changes in the absorber, as well as devices with strong and weak coupling to the metal leads. Our results indicate that the most promising case is when the SC channel is weakly coupled to the leads and in the presence of a background magnetic field, where photoexcitation of a magnetic molecule can trigger a SC-to-normal transition in the channel that leads to a change in the device current several times larger than in the case of a normal-phase channel device.
The III-nitride semiconductors have many attractive properties for field-emission vacuum electronics, including high thermal and chemical stability, low electron affinity, and high breakdown fields. Here, we report top-down fabricated gallium nitride (GaN)-based nanoscale vacuum electron diodes operable in air, with record ultralow turn-on voltages down to ∼0.24 V and stable high field-emission currents, tested up to several microamps for single-emitter devices. We leverage a scalable, top-down GaN nanofabrication method leading to damage-free and smooth surfaces. Gap-dependent and pressure-dependent studies provide new insights into the design of future, integrated nanogap vacuum electron devices. The results show promise for a new class of high-performance and robust, on-chip, III-nitride-based vacuum nanoelectronics operable in air or reduced vacuum.
Terahertz (THz) technology has shown promise for several applications, but limitations in sources and detectors have prevented broader adoption. Existing THz detectors are rigid, planar, and fabricated using complex technology, making it difficult to integrate into systems. Here we demonstrate THz detectors fabricated by inkjet printing on submicrometer thick, ultraflexible substrates. By developing p- and n-type carbon nanotube inks, we achieve optically thick p–n junction and p-type devices, enabling antenna-free pixels for THz imaging. By further designing and folding the printed devices, we realize origami-inspired architectures with improved performance over single devices, achieving a noise-equivalent power of 12 nW/Hz1/2 at room temperature with no voltage bias. Our approach opens avenues for nonplanar, foldable, deployable, insertable, and retractable THz detectors for applications in nondestructive inspection.
A number of applications in basic science and technology would benefit from high-fidelity photon-number-resolving photodetectors. While some recent experimental progress has been made in this direction, the requirements for true photon number resolution are stringent, and no design currently exists that achieves this goal. Here we employ techniques from fundamental quantum optics to demonstrate that detectors composed of subwavelength elements interacting collectively with the photon field can achieve high-performance photon number resolution. We propose a new design that simultaneously achieves photon number resolution, high efficiency, low jitter, low dark counts, and high count rate. We discuss specific systems that satisfy the design requirements, pointing to the important role of nanoscale device elements.
Recent years have seen an explosion in research efforts discovering and understanding novel electronic and optical properties of topological quantum materials (TQMs). In this LDRD, a synergistic effort of materials growth, characterization, electrical-magneto-optical measurements, combined with density functional theory and modeling has been established to address the unique properties of TQMs. Particularly, we have carried out extensive studies in search for Majorana fermions (MFs) in TQMs for topological quantum computation. Moreover, we have focused on three important science questions. 1) How can we controllably tune the properties of TQMs to make them suitable for quantum information applications? 2) What materials parameters are most important for successfully observing MFs in TQMs? 3) Can the physical properties of TQMs be tailored by topological band engineering? Results obtained in this LDRD not only deepen our current knowledge in fundamental quantum physics but also hold great promise for advanced electronic/photonic applications in information technologies. ACKNOWLEDGEMENTS The work at Sandia National Labs was supported by a Laboratory Directed Research and Development project. Device fabrication was performed at the Center for Integrated Nanotechnologies, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science. We are grateful to many people inside and outside Sandia for their support and fruitful collaborations. This report describes objective technical results and analysis. Any subjective views or opinions that might be expressed in the paper do not necessarily represent the views of the U.S. Department of Energy or the United States Government. Sandia National Laboratories is a multimission laboratory managed and operated by National Technology & Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International Inc., for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-NA0003525.
AlGaN-channel high electron mobility transistors (HEMTs) were operated as visible- and solar-blind photodetectors by using GaN nanodots as an optically active floating gate. The effect of the floating gate was large enough to switch an HEMT from the off-state in the dark to an on-state under illumination. This opto-electronic response achieved responsivity > 108 A/W at room temperature while allowing HEMTs to be electrically biased in the offstate for low dark current and low DC power dissipation. The influence of GaN nanodot distance from the HEMT channel on the dynamic range of the photodetector was investigated, along with the responsivity and temporal response of the floating gate HEMT as a function of optical intensity. The absorption threshold was shown to be controlled by the AlN mole fraction of the HEMT channel layer, thus enabling the same device design to be tuned for either visible- or solar-blind detection.
Photodetection plays a key role in basic science and technology, with exquisite performance having been achieved down to the single-photon level. Further improvements in photodetectors would open new possibilities across a broad range of scientific disciplines and enable new types of applications. However, it is still unclear what is possible in terms of ultimate performance and what properties are needed for a photodetector to achieve such performance. Here, we present a general modeling framework for photodetectors whereby the photon field, the absorption process, and the amplification process are all treated as one coupled quantum system. The formalism naturally handles field states with single or multiple photons as well as a variety of detector configurations and includes a mathematical definition of ideal photodetector performance. In conclusion, the framework reveals how specific photodetector architectures introduce limitations and tradeoffs for various performance metrics, providing guidance for optimization and design.
HKUST-1 or Cu3BTC2 (BTC = 1,3,5-benzenetricarboxylate) is a prototypical metal-organic framework (MOF) that holds a privileged position among MOFs for device applications, as it can be deposited as thin films on various substrates and surfaces. Recently, new potential applications in electronics have emerged for this material when HKUST-1 was demonstrated to become electrically conductive upon infiltration with 7,7,8,8-tetracyanoquinodimethane (TCNQ). However, the factors that control the morphology and reactivity of the thin films are unknown. Here, we present a study of the thin-film growth process on indium tin oxide and amorphous Si prior to infiltration. From the unusual bimodal, non-log-normal distribution of crystal domain sizes, we conclude that the nucleation of new layers of Cu3BTC2 is greatly enhanced by surface defects and thus difficult to control. We then show that these films can react with methanolic TCNQ solutions to form dense films of the coordination polymer Cu(TCNQ). This chemical conversion is accompanied by dramatic changes in surface morphology, from a surface dominated by truncated octahedra to randomly oriented thin platelets. The change in morphology suggests that the chemical reaction occurs in the liquid phase and is independent of the starting surface morphology. The chemical transformation is accompanied by 10 orders of magnitude change in electrical conductivity, from <10-11 S/cm for the parent Cu3BTC2 material to 10-1 S/cm for the resulting Cu(TCNQ) film. The conversion of Cu3BTC2 films, which can be grown and patterned on a variety of (nonplanar) substrates, to Cu(TCNQ) opens the door for the facile fabrication of more complex electronic devices.
Detection of low intensity light down to a few photons requires photodetectors with high gain. A new photodetector is reported based on C60-sensitized aligned carbon nanotube (CNT) transistors with an extremely high responsivity of 108 A W−1 (gain > 108) in the ultraviolet and visible range, and 720 A W−1 (gain = 940) in the infrared range. In contrast to most sensitized phototransistors that operate on the photogating effect, the new photodetector operates on the modulation of the electrons scattering in the CNTs, leading to negative photoconductivity. Comparison with similar photodetectors using random CNT networks shows the benefit of using aligned CNTs. At room temperature, the aligned CNT photodetectors are demonstrated to detect a few tens of photons per CNT.
Quantum-size-controlled photoelectrochemical (QSC-PEC) etching, which uses quantum confinement effects to control size, can potentially enable the fabrication of epitaxial quantum nanostructures with unprecedented accuracy and precision across a wide range of materials systems. However, many open questions remain about this new technique, including its limitations and broader applicability. In this project, using an integrated experimental and theoretical modeling approach, we pursue a greater understanding of the time-dependent QSC-PEC etch process and to uncover the underlying mechanisms that determine its ultimate accuracy and precision. We also seek to broaden our understanding of the scope of its ultimate applicability in emerging nanostructures and nanodevices.
Single-photon detectors have achieved impressive performance and have led to a number of new scientific discoveries and technological applications. Existing models of photodetectors are semiclassical in that the field-matter interaction is treated perturbatively and time-separated from physical processes in the absorbing matter. An open question is whether a fully quantum detector, whereby the optical field, the optical absorption, and the amplification are considered as one quantum system, could have improved performance. Here we develop a theoretical model of such photodetectors and employ simulations to reveal the critical role played by quantum coherence and amplification backaction in dictating the performance. We show that coherence and backaction lead to trade-offs between detector metrics and also determine optimal system designs through control of the quantum-classical interface. Importantly, we establish the design parameters that result in a ideal photodetector with 100% efficiency, no dark counts, and minimal jitter, thus paving the route for next-generation detectors.
V-telluride superlattice thin films have shown promising performance for on-chip cooling devices. Recent experimental studies have indicated that device performance is limited by the metal/semiconductor electrical contacts. One challenge in realizing a low resistivity contact is the absence of fundamental knowledge of the physical and chemical properties of interfaces between metal and V-telluride materials. This study presents a combination of experimental and theoretical efforts to understand, design, and harness low resistivity contacts to V-tellurides. Ab initio calculations are used to explore the effects of interfacial structure and chemical compositions on the electrical contacts, and an ab initio based macroscopic model is employed to predict the fundamental limit of contact resistivity as a function of both carrier concentration and temperature. Under the guidance of theoretical studies, an experimental approach is developed to fabricate low resistivity metal contacts to V-telluride thin film superlattices, achieving a 100-fold reduction compared to previous work. Interfacial characterization and analysis using both scanning transmission electron microscopy and energy-dispersive X-ray spectroscopy show unusual interfacial morphology and the potential for further improvement in contact resistivity. Finally, the improved contacts are harnessed to realize an improved high-performance thermoelectric cooling module.
The family of three-dimensional topological insulators opens new avenues to discover novel photophysics and to develop novel types of photodetectors. ZrTe5 has been shown to be a Dirac semimetal possessing unique topological, electronic, and optical properties. Here, we present spatially resolved photocurrent measurements on devices made of nanoplatelets of ZrTe5, demonstrating the photothermoelectric origin of the photoresponse. Because of the high electrical conductivity and good Seebeck coefficient, we obtain noise-equivalent powers as low as 42 pW/Hz1/2, at room temperature for visible light illumination, at zero bias. We also show that these devices suffer from significant ambient reactivity, such as the formation of a Te-rich surface region driven by Zr oxidation as well as severe reactions with the metal contacts. This reactivity results in significant stresses in the devices, leading to unusual geometries that are useful for gaining insight into the photocurrent mechanisms. Our results indicate that both the large photothermoelectric response and reactivity must be considered when designing or interpreting photocurrent measurements in these systems.
Metal organic frameworks (MOFs) are extended, nanoporous crystalline compounds consisting of metal ions interconnected by organic ligands. Their synthetic versatility suggest a disruptive class of opto - electronic materials with a high degree of electrical tunability and without the property - degrading disorder of organic conductors. In this project we determined the factors controlling charge and energy transport in MOFs and evaluated their potential for thermoelectric energy conversion. Two strategies for a chieving electronic conductivity in MOFs were explored: 1) using redox active 'guest' molecules introduced into the pores to dope the framework via charge - transfer coupling (Guest@MOF), 2) metal organic graphene analogs (MOGs) with dispersive band structur es arising from strong electronic overlap between the MOG metal ions and its coordinating linker groups. Inkjet deposition methods were developed to facilitate integration of the guest@MOF and MOG materials into practical devices.
Dynamic wavelength tunability has long been the holy grail of photodetector technology. Because of its atomic thickness and unique properties, graphene opens up new paradigms to realize this concept, but so far this has been elusive experimentally. Here we employ detailed quantum transport modeling of photocurrent in graphene field-effect transistors (including realistic electromagnetic fields) to show that wavelength tunability is possible by dynamically changing the gate voltage. We reveal the phenomena that govern the behavior of this type of device and show significant departure from the simple expectations based on vertical transitions. We find strong focusing of the electromagnetic fields at the contact edges over the same length scale as the band-bending. Both of these spatially-varying potentials lead to an enhancement of non-vertical optical transitions, which dominate even in the absence of phonon or impurity scattering. We also show that the vanishing density of states near the Dirac point leads to contact blocking and a gate-dependent modulation of the photocurrent. Several of the effects discussed here should be applicable to a broad range of one-and two-dimensional materials and devices.