Shriram Ramanathan

Correlated Perovskites as a New Platform for Super-Broadband-Tunable Photonics

We report strong and non-volatile optical modulation utilizing electron-doping induced phase change of a perovskite, SmNiO<inf>3</inf>. Broadband modulation (λ=400nm–17μm) is demonstrated using thin-film SmNiO<inf>3</inf>, and narrowband modulation is realized with metasurfaces integrated with SmNiO<inf>3</inf>.

Habituation based synaptic plasticity and organismic learning in a quantum perovskite

A central characteristic of living beings is the ability to learn from and respond to their environment leading to habit formation and decision making. This behavior, known as habituation, is universal among all forms of life with a central nervous system, and is also observed in single-cell organisms that do not possess a brain. Here, we report the discovery of habituation-based plasticity utilizing a perovskite quantum system by dynamical modulation of electron localization. Microscopic mechanisms and pathways that enable this organismic collective charge-lattice interaction are elucidated by first-principles theory, synchrotron investigations, ab initio molecular dynamics simulations, and in situ environmental breathing studies. We implement a learning algorithm inspired by the conductance relaxation behavior of perovskites that naturally incorporates habituation, and demonstrate learning to forget: a key feature of animal and human brains. Incorporating this elementary skill in learning boosts the capability of neural computing in a sequential, dynamic environment.Habituation is a learning mechanism that enables control over forgetting and learning. Zuo, Panda et al., demonstrate adaptive synaptic plasticity in SmNiO3 perovskites to address catastrophic forgetting in a dynamic learning environment via hydrogen-induced electron localization.

Strongly correlated perovskite lithium ion shuttles

Significance Designing solid-state ion conductors is of broad interest to energy conversion, bioengineering, and information processing. Here, we demonstrate a new class of Li-ion conducting quantum materials in the perovskite family. Rare-earth perovskite nickelate films of the chemical formula SmNiO3 are shown to exhibit high Li-ion conductivity while minimizing their electronic conductivity. This process occurs by electron injection into Ni orbitals when the Li ions are inserted from a reservoir. The mechanism of doping is studied by high-resolution experimental and first-principles theoretical methods to provide evidence for ion shuttling in the lattice and the atomistic pathways. The experiments are then extended to other small ions such as Na+, demonstrating the generality of the approach. Solid-state ion shuttles are of broad interest in electrochemical devices, nonvolatile memory, neuromorphic computing, and biomimicry utilizing synthetic membranes. Traditional design approaches are primarily based on substitutional doping of dissimilar valent cations in a solid lattice, which has inherent limits on dopant concentration and thereby ionic conductivity. Here, we demonstrate perovskite nickelates as Li-ion shuttles with simultaneous suppression of electronic transport via Mott transition. Electrochemically lithiated SmNiO3 (Li-SNO) contains a large amount of mobile Li+ located in interstitial sites of the perovskite approaching one dopant ion per unit cell. A significant lattice expansion associated with interstitial doping allows for fast Li+ conduction with reduced activation energy. We further present a generalization of this approach with results on other rare-earth perovskite nickelates as well as dopants such as Na+. The results highlight the potential of quantum materials and emergent physics in design of ion conductors.

Feature issue introduction: Optical Phase Change Materials

This Optical Materials Express feature issue presents a collection of twelve papers clustered around the general topic of optical phase-change materials. While the scientific study of phase-change materials has a long history, interest in these materials for optical as well as electronic applications has risen sharply in the last decade, and is now the subject of intense world-wide research efforts. In this set of feature papers, topics range from basic materials studies to applications of phase-change materials in metasurfaces, sensing, integrated optics, silicon photonics and polarization switching.

Low-voltage artificial neuron using feedback engineered insulator-to-metal-transition devices

We demonstrate a solid-state spiking artificial neuron based upon an insulator-to-metal (IMT) transition material element that operates at an unprecedented low voltage (0.8 V). We have developed a general coupled electrical-thermal device model for IMT based devices to accurately predict experimental outcomes. From the experiment and simulation, we show that voltage scalability to sub 0.3 V is possible by scaling of the IMT based neuron.

Beyond electrostatic modification: design and discovery of functional oxide phases via ionic-electronic doping

ABSTRACT A new research field of functional materials and device physics is rising that combines ionic transport with charge carrier modulation to realize emergent physical properties and discovery of metastable phases. The paradigm for enabling function extends far beyond carrier accumulation or depletion in band semiconductors or simply moving ions through an insulating electrolyte. Rather, by carefully selecting electronically or structurally fragile materials, one can collapse or open band gaps via extreme ionic dopant concentration, or reconfigure their entire crystal structure to create new phases. Electron–electron and electron–lattice interactions can be coupled or controlled independently in such systems via electric fields without thermal constraints by use of ionic dopants. The unifying theme across these studies is to introduce ions and electrons via electric fields through interfaces, with electrochemistry playing a dominant role. In this review, we briefly summarize this nascent field of iontronics and discuss principal results to date with examples from binary and complex oxides as well as selected 2D materials systems. We conclude the review by highlighting gaps in fundamental scientific understanding and prospects for the use of such novel devices in future electronic, photonic and energy technologies. Graphical Abstract

Thermally tunable VO2-SiO2 nanocomposite thin-film capacitors

We present a study of co-sputtered VO2-SiO2 nanocomposite dielectric thin-film media possessing continuous temperature tunability of the dielectric constant. The smooth thermal tunability is a result of the insulator-metal transition in the VO2 inclusions dispersed within an insulating matrix. We present a detailed comparison of the dielectric characteristics of this nanocomposite with those of a VO2 control layer and of VO2/SiO2 laminate multilayers of comparable overall thickness. We demonstrated a nanocomposite capacitor that has a thermal capacitance tunability of ∼60% between 25 °C and 100 °C at 1 MHz, with low leakage current. Such thermally tunable capacitors could find potential use in applications such as sensing, thermal cloaks, and phase-change energy storage devices.We present a study of co-sputtered VO2-SiO2 nanocomposite dielectric thin-film media possessing continuous temperature tunability of the dielectric constant. The smooth thermal tunability is a result of the insulator-metal transition in the VO2 inclusions dispersed within an insulating matrix. We present a detailed comparison of the dielectric characteristics of this nanocomposite with those of a VO2 control layer and of VO2/SiO2 laminate multilayers of comparable overall thickness. We demonstrated a nanocomposite capacitor that has a thermal capacitance tunability of ∼60% between 25 °C and 100 °C at 1 MHz, with low leakage current. Such thermally tunable capacitors could find potential use in applications such as sensing, thermal cloaks, and phase-change energy storage devices.

Optical power diodes based on phase-transition materials (Conference Presentation)

We present several designs and experimental implementations of optical power diodes – devices that are designed to be transparent from one direction, but opaque from the other, when illuminated by a beam with sufficient intensity. Optical power diodes can be used to protect optical devices that both detect and transmit light. Our designs are based on phase-change material vanadium dioxide (VO2), which undergoes an insulator-to-metal transition (IMT) that can be triggered thermally or optically. Here, VO2 films serve as nonlinear elements that can be transformed from transparent to opaque by intense illumination. We build thin-film metallic structures on top of the VO2 films such that the optical absorption becomes asymmetric – light impinging from one direction is absorbed at a higher rate than from the other direction, triggering the transition, and turning the device opaque. This results in asymmetric transmission. The designs are optimized with finite-difference time-domain (FDTD) simulations, using optical constants of VO2 extracted using ellipsometry, and are shown to be scalable across the near- and mid-infrared. Our initial experimental results using a simple design comprised of metal and VO2 films on sapphire, designed for an operating wavelength of 1.35µm, show a transmission asymmetry ratio of ~2, and experiments with superior designs are ongoing. Future work will include the use of defect-engineered VO2 to engineer the intensity threshold of optical power diodes.