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Shriram Ramanathan

Publications and source records attributed to Shriram Ramanathan.

At least 19 recordsLinked to original sources

Protonic Nickelate Device Networks for Spatiotemporal Neuromorphic Computing

Computation in biological neural circuits arises from the interplay of nonlinear temporal responses and spatially distributed dynamic network interactions. Replicating this richness in hardware has remained challenging, as most neuromorphic devices emulate only isolated neuron- or synapse-like functions. In this work, we introduce an integrated neuromorphic computing platform in which both nonlinear spatiotemporal processing and programmable memory are realized within a single perovskite nickelate material system. By engineering symmetric and asymmetric hydrogenated NdNiO3 junction devices on the same wafer, we combine ultrafast, proton-mediated transient dynamics with stable multilevel resistance states. Networks of symmetric NdNiO3 junctions exhibit emergent spatial interactions mediated by proton redistribution, while each node simultaneously provides short-term temporal memory, enabling nanoseconds scale operation with an energy cost of 0.2 nJ per input. When interfaced with asymmetric output units serving as reconfigurable long-term weights, these networks allow both feature transformation and linear classification in the same material system. Leveraging these emergent interactions, the platform enables real-time pattern recognition and achieves high accuracy in spoken-digit classification and early seizure detection, outperforming temporal-only or uncoupled architectures. These results position protonic nickelates as a compact, energy-efficient, CMOS-compatible platform that integrates processing and memory for scalable intelligent hardware.

cs.ET

Large tuning of the optical properties of nanoscale NdNiO3 via electron doping

We synthesized crystalline films of neodymium nickel oxide (NdNiO3), a perovskite quantum material, switched the films from a metal phase (intrinsic) into an insulator phase (electron-doped) by field-driven lithium-ion intercalation, and characterized their structural and optical properties. Time-of-flight secondary-ion mass spectrometry (ToF-SIMS) showed that the intercalation process resulted in a gradient of the dopant concentration along the thickness direction of the films, turning the films into insulator-metal bilayers. We used variable-angle spectroscopic ellipsometry to measure the complex refractive indices of the metallic and insulating phases of NdNiO3. The insulator phase has a refractive index of n ~ 2 and low absorption in the visible and near infrared, and analysis of the complex refractive indices indicated that the band gap of the insulating phase is roughly 3-4 eV. Electrical control of the optical band gap, with corresponding large changes to the optical refractive indices, creates new opportunities for tunable optics.

cond-mat.mtrl-sci

Hydrogen-doping mediated solid state thermal switch

Recent reports reveal that isothermal chemical doping of hydrogen in correlated complex oxides such as perovskite nickelates (e.g. NdNiO3) can induce a metal-to-insulator transition (MIT) without the need for temperature modulation. In this work, we interrogate the magnitude change in temperature dependence of thermal conductivity upon chemical doping of hydrogen, as any changes to the thermal properties upon doping offer a route to solid-state thermal switches as well as another potential signal to monitor in a diverse set of sensing, electronic, and optical applications. Using frequency-domain thermoreflectance, we demonstrate that a large concentration of hydrogen (~ 0.1 - 0.5 H/unit cell) completely suppresses the electronic contribution to thermal conductivity in NdNiO3 thin films and reduces the phononic contribution by a factor of 2. These results are critical for the design of next-generation solid-state thermal switches, sensors, extreme environment electronics and neuromorphic memory architectures.

cond-mat.mtrl-sci

Origin of discrete electrical switching in chemically heterogeneous vanadium oxide crystals

Electrically driven insulator-metal transitions in prototypical quantum materials such as VO2 offer a foundational platform for designing novel solid-state devices. Tuning the V: O stoichiometry offers a vast electronic phase space with non-trivial collective properties. Here, we report the discovery of discrete threshold switching voltages with constant threshold voltage difference between cycles in vanadium oxide crystals. The observed threshold fields over 10000 cycles are ~100X lower than that noted for stoichiometric VO2 and show unique discrete behaviour. We correlate the observed discrete memristor behaviour with the valence change mechanism and fluctuations in the chemical composition of spatially distributed VO2-VnO2n-1 complex oxide phases. Design of chemical heterogeneity in Mott insulators, therefore, offers an intriguing path to realizing low-energy neuromorphic devices.

physics.app-ph

High-speed sensing of RF signals with phase change materials

RF radiation spectrum is central to wireless and radar systems among numerous high-frequency device technologies. Here, we demonstrate sensing of RF signals in the technologically relevant 2.4 GHz range utilizing vanadium dioxide (VO2), a quantum material that has garnered significant interest for its insulator-to-metal transition. We find the electrical resistance of both stoichiometric as well as off-stoichiometric vanadium oxide films can be modulated with RF wave exposures from a distance. The response of the materials to the RF waves can be enhanced by either increasing the power received by the sample or reducing channel separation. We report a significant ~73% drop in resistance with a 5 μm channel gap of the VO2 film at a characteristic response time of 16 microseconds. The peak sensitivity is proximal to the phase transition temperature boundary that can be engineered via doping and crystal chemistry. Dynamic sensing measurements highlight the films' rapid response and broad-spectrum sensitivity. Engineering electronic phase boundaries in correlated electron systems could offer new capabilities in emerging communication technologies.

physics.app-ph

Hydrogen-induced tunable remanent polarization in a perovskite nickelate

Materials with field-tunable polarization are of broad interest to condensed matter sciences and solid-state device technologies. Here, using hydrogen (H) donor doping, we modify the room temperature metallic phase of a perovskite nickelate NdNiO3 into an insulating phase with both metastable dipolar polarization and space-charge polarization. We then demonstrate transient negative differential capacitance in thin film capacitors. The space-charge polarization caused by long-range movement and trapping of protons dominates when the electric field exceeds the threshold value. First-principles calculations suggest the polarization originates from the polar structure created by H doping. We find that polarization decays within ~1 second which is an interesting temporal regime for neuromorphic computing hardware design, and we implement the transient characteristics in a neural network to demonstrate unsupervised learning. These discoveries open new avenues for designing novel ferroelectric materials and electrets using light-ion doping.

cond-mat.str-el

Temporal credit assignment for one-shot learning utilizing a phase transition material

Design of hardware based on biological principles of neuronal computation and plasticity in the brain is a leading approach to realizing energy- and sample-efficient artificial intelligence and learning machines. An important factor in selection of the hardware building blocks is the identification of candidate materials with physical properties suitable to emulate the large dynamic ranges and varied timescales of neuronal signaling. Previous work has shown that the all-or-none spiking behavior of neurons can be mimicked by threshold switches utilizing phase transitions. Here we demonstrate that devices based on a prototypical metal-insulator-transition material, vanadium dioxide (VO2), can be dynamically controlled to access a continuum of intermediate resistance states. Furthermore, the timescale of their intrinsic relaxation can be configured to match a range of biologically-relevant timescales from milliseconds to seconds. We exploit these device properties to emulate three aspects of neuronal analog computation: fast (~1 ms) spiking in a neuronal soma compartment, slow (~100 ms) spiking in a dendritic compartment, and ultraslow (~1 s) biochemical signaling involved in temporal credit assignment for a recently discovered biological mechanism of one-shot learning. Simulations show that an artificial neural network using properties of VO2 devices to control an agent navigating a spatial environment can learn an efficient path to a reward in up to 4 fold fewer trials than standard methods. The phase relaxations described in our study may be engineered in a variety of materials, and can be controlled by thermal, electrical, or optical stimuli, suggesting further opportunities to emulate biological learning.

cond-mat.dis-nn

Infrared Nanoimaging of Hydrogenated Perovskite Nickelate Synaptic Devices

Solid-state devices made from correlated oxides such as perovskite nickelates are promising for neuromorphic computing by mimicking biological synaptic function. However, comprehending dopant action at the nanoscale poses a formidable challenge to understanding the elementary mechanisms involved. Here, we perform operando infrared nanoimaging of hydrogen-doped correlated perovskite, neodymium nickel oxide (H-NdNiO3) devices and reveal how an applied field perturbs dopant distribution at the nanoscale. This perturbation leads to stripe phases of varying conductivity perpendicular to the applied field, which define the macroscale electrical characteristics of the devices. Hyperspectral nano-FTIR imaging in conjunction with density functional theory calculations unveil a real-space map of multiple vibrational states of H-NNO associated with OH stretching modes and their dependence on the dopant concentration. Moreover, the localization of excess charges induces an out-of-plane lattice expansion in NNO which was confirmed by in-situ - x-ray diffraction and creates a strain that acts as a barrier against further diffusion. Our results and the techniques presented here hold great potential to the rapidly growing field of memristors and neuromorphic devices wherein nanoscale ion motion is fundamentally responsible for function.

physics.app-ph

Electrically tunable VO2-metal metasurface for mid-infrared switching, limiting, and nonlinear isolation

We demonstrate an electrically controlled metal-VO2 metasurface for the mid-wave infrared that simultaneously functions as a tunable optical switch, an optical limiter with a tunable limiting threshold, and a nonlinear optical isolator with a tunable operating range. The tunability is achieved via Joule heating through the metal comprising the metasurface, resulting in an integrated optoelectronic device. As an optical switch, the device has an experimental transmission ratio of ~100 when varying the bias current. Operating as an optical limiter, we demonstrated tunability of the limiting threshold from 20 mW to 180 mW of incident laser power. Similar degrees of tunability are also achieved for nonlinear optical isolation, which enables asymmetric (nonreciprocal) transmission.

physics.optics

Efficient Probabilistic Computing with Stochastic Perovskite Nickelates

Probabilistic computing has emerged as a viable approach to solve hard optimization problems. Devices with inherent stochasticity can greatly simplify their implementation in electronic hardware. Here, we demonstrate intrinsic stochastic resistance switching controlled via electric fields in perovskite nickelates doped with hydrogen. The ability of hydrogen ions to reside in various metastable configurations in the lattice leads to a distribution of transport gaps. With experimentally characterized p-bits, a shared-synapse p-bit architecture demonstrates highly-parallelized and energy-efficient solutions to optimization problems such as integer factorization and Boolean-satisfiability. The results introduce perovskite nickelates as scalable potential candidates for probabilistic computing and showcase the potential of light-element dopants in next-generation correlated semiconductors.

cond-mat.mtrl-sci

Tuning carrier density and phase transitions in oxide semiconductors using focused ion beams

We demonstrate spatial modification of the optical properties of thin-film metal oxides, zinc oxide and vanadium dioxide as representatives, using a commercial focused ion beam (FIB) system. Using a Ga+ FIB and thermal annealing, we demonstrated variable doping of a band semiconductor, zinc oxide (ZnO), achieving carrier concentrations from 10^18 cm-3 to 10^20 cm-3. Using the same FIB without subsequent thermal annealing, we defect-engineered a correlated semiconductor, vanadium dioxide (VO2), locally modifying its insulator-to-metal transition (IMT) temperature by range of ~25 degrees C. Such area-selective modification of metal oxides by direct writing using a FIB provides a simple, mask-less route to the fabrication of optical structures, especially when multiple or continuous levels of doping or defect density are required.

cond-mat.mtrl-sci

Nanoscale Thermal Imaging of VO$_2$ via Poole-Frenkel Conduction

We present a method for nanoscale thermal imaging of insulating thin films using atomic force microscopy (AFM), and we demonstrate its utility on VO$_2$. We sweep the applied voltage $V$ to a conducting AFM tip in contact mode and measure the local current $I$ through the film. By fitting the $IV$ curves to a Poole-Frenkel conduction model at low $V$, we calculate the local temperature with spatial resolution better than 50 nm using only fundamental constants and known film properties. Our thermometry technique enables local temperature measurement of \textit{any} insulating film dominated by the Poole-Frenkel conduction mechanism, and can be extended to insulators that display other conduction mechanisms.

cond-mat.str-el

Quantum materials for energy-efficient neuromorphic computing

Neuromorphic computing approaches become increasingly important as we address future needs for efficiently processing massive amounts of data. The unique attributes of quantum materials can help address these needs by enabling new energy-efficient device concepts that implement neuromorphic ideas at the hardware level. In particular, strong correlations give rise to highly non-linear responses, such as conductive phase transitions that can be harnessed for short and long-term plasticity. Similarly, magnetization dynamics are strongly non-linear and can be utilized for data classification. This paper discusses select examples of these approaches, and provides a perspective for the current opportunities and challenges for assembling quantum-material-based devices for neuromorphic functionalities into larger emergent complex network systems.

cs.ET

Wavelength-by-wavelength temperature-independent thermal radiation utilizing an insulator-metal transition

Both the magnitude and spectrum of the blackbody-radiation distribution change with temperature. Here, we designed the temperature-dependent spectral emissivity of a coating to counteract all the changes in the blackbody-radiation distribution over a certain temperature range, enabled by the nonhysteretic insulator-to-metal phase transition of SmNiO3. At each wavelength within the long-wave infrared atmospheric-transparency window, the thermal radiance of our coating remains nearly constant over a temperature range of at least 20 °C. Our approach can conceal thermal gradients and transient temperature changes from infrared imaging systems, including those that discriminate by wavelength, such as multispectral and hyperspectral cameras.

physics.optics

Low-temperature emergent neuromorphic networks with correlated oxide devices

Neuromorphic computing which aims to mimic the collective and emergent behavior of the brain's neurons, synapses, axons, dendrites offers an intriguing, potentially disruptive solution to society's ever-growing computational needs. Although much progress has been made in designing circuit elements that mimic the behavior of neurons and synapses, challenges remain in designing networks of elements that feature a collective response behavior. We present simulations of networks of circuits and devices based on superconducting and Mott-insulating oxides that display a multiplicity of emergent states that depend on the spatial configuration of the network. Our proposed network designs are based on experimentally known ways of tuning the properties of these oxides using light ions. We show how neuronal and synaptic behavior can be achieved with arrays of superconducting Josephson junction loops, all within the same device. We also show how a multiplicity of synaptic states could be achieved by designing arrays of devices based on hydrogenated rare-earth nickelates. Together, our results demonstrate a new research platform that utilizes the collective macroscopic properties of quantum materials to mimic the emergent behavior found in biological systems.

physics.app-ph

Proton distribution visualization in perovskite nickelate devices utilizing nanofocused X-rays

We use a 30-nm x-ray beam to study the spatially resolved properties of a SmNiO$_3$-based nanodevice that is doped with protons. The x-ray absorption spectra supported by density-functional theory (DFT) simulations show partial reduction of nickel valence in the region with high proton concentration, which leads to the insulating behavior. Concurrently, x-ray diffraction reveals only a small lattice distortion in the doped regions. Together, our results directly show that the knob which proton doping modifies is the electronic valency, and not the crystal lattice. The studies are relevant to on-going efforts to disentangle structural and electronic effects across metal-insulator phase transitions in correlated oxides.

cond-mat.mtrl-sci

First Demonstration of Robust Tri-Gate \b{eta}-Ga2O3 Nano-membrane Field-Effect Transistors Operated Up to 400 °C

Nano-membrane tri-gate beta-gallium oxide (\b{eta}-Ga2O3) field-effect transistors (FETs) on SiO2/Si substrate fabricated via exfoliation have been demonstrated for the first time. By employing electron beam lithography, the minimum-sized features can be defined with a 50 nm fin structure. For high-quality interface between \b{eta}-Ga2O3 and gate dielectric, atomic layer-deposited 15-nm-thick aluminum oxide (Al2O3) was utilized with Tri-methyl-aluminum (TMA) self-cleaning surface treatment. The fabricated devices demonstrate extremely low subthreshold slope (SS) of 61 mV/dec, high drain current (IDS) ON/OFF ratio of 1.5 X 109, and negligible transfer characteristic hysteresis. We also experimentally demonstrated robustness of these devices with current-voltage (I-V) characteristics measured at temperatures up to 400 °C.

physics.app-ph

Effective reduction of PdCoO2 thin films via hydrogenation and sign tunable anomalous Hall effect

PdCoO2 , belonging to a family of triangular oxides called delafossite, is one of the most conducting oxides. Its in-plane conductivity is comparable to those of the best metals, and exhibits hydrodynamic electronic transport with extremely long mean free path at cryogenic temperatures. Nonetheless, it is nonmagnetic despite the presence of the cobalt ion. Here, we show that a mild hydrogenation process reduces PdCoO2 thin films to an atomically-mixed alloy of PdCo with strong out-of-plane ferromagnetism and sign-tunable anomalous Hall effect. Considering that many other compounds remain little affected under a similar hydrogenation condition, this discovery may provide a route to creating novel spintronic heterostructures combining strong ferromagnetism, involving oxides and other functional materials.

cond-mat.mtrl-sci