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Mechanisms enabling reconfigurability and long-term retention in vanadium oxide electrochemical memory

Journal Article · · Physical Review Materials
DOI:https://doi.org/10.1103/k616-d2q5· OSTI ID:2584903
 [1];  [1];  [1];  [1];  [2];  [3];  [3];  [4];  [5];  [1];  [2];  [2];  [2];  [1];  [1];  [6];  [2];  [1]
  1. Sandia National Lab. (SNL-CA), Livermore, CA (United States)
  2. Texas A&M University, College Station, TX (United States)
  3. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
  4. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
  5. University of Michigan, Ann Arbor, MI (United States)
  6. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Texas A&M University, College Station, TX (United States)
Phase coexistence in nanoscale electrochemical random-access memory (ECRAM) has recently been demonstrated to enable both information storage and extraordinary reconfigurability. These proof-of-principle demonstrations have left the mechanistic details of such a process unresolved. Particularly, the mechanisms that stabilize the multiple phases, and the underlying processes behind sustained memory retention, remain unclear, and are necessary to design such devices. Here we report microscale ECRAM devices composed of V⁢O𝑥, which enables us to directly probe the active region in an operando fashion using optical techniques. Using Raman mapping, we show the phase coexistence driven by the electrochemical injection of O vacancies to be spatially uniform (i.e., with no filaments). The stability was observed to be unusually long, with 1% loss over 14 years in ambient conditions. First-principles calculations of the oxygen vacancy formation energies in V⁢O𝑥 further support the thermodynamic coexistence of multiple V⁢O𝑥 phases and clarify the origin of the observed long-term retention in the ECRAM devices. Further, we demonstrate single devices that can be voltage programmed to exhibit synaptic, neuronal, and reconfigurable logic gate functionalities. Furthermore, we not only uncover the phase coexistence mechanism that may help device design, but also demonstrate the circuit-level applications of reconfigurability.
Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Sandia National Laboratories (SNL-CA), Livermore, CA (United States)
Sponsoring Organization:
USDOE; USDOE National Nuclear Security Administration (NNSA)
Grant/Contract Number:
AC05-00OR22725; NA0003525
OSTI ID:
2584903
Alternate ID(s):
OSTI ID: 2587458
Report Number(s):
SAND--2025-10447J; 1728750
Journal Information:
Physical Review Materials, Journal Name: Physical Review Materials Journal Issue: 8 Vol. 9; ISSN 2475-9953
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

References (59)

Electrical Conductivity of Semiconducting Tungsten Oxide Glasses journal June 2001
Electrochemically Triggered Metal-Insulator Transition between VO 2 and V 2 O 5 journal June 2018
Filament‐Free Bulk Resistive Memory Enables Deterministic Analogue Switching journal September 2020
Memory Devices: Filament‐Free Bulk Resistive Memory Enables Deterministic Analogue Switching (Adv. Mater. 45/2020) journal November 2020
ECRAM Materials, Devices, Circuits and Architectures: A Perspective journal November 2022
Electro‐Thermal Characterization of Dynamical VO2 Memristors via Local Activity Modeling journal November 2022
Nonvolatile Electrochemical Random‐Access Memory under Short Circuit journal November 2022
Electron beam modification of vanadium dioxide oscillators journal December 2016
Review of computational approaches to predict the thermodynamic stability of inorganic solids journal February 2022
Electronic Structure of Unsaturated V2O5(001) and (100) Surfaces: Ab Initio Density Functional Theory Studies journal May 2009
Numerical integration of the cartesian equations of motion of a system with constraints: molecular dynamics of n-alkanes journal March 1977
Crystal structure of vanadium suboxide V2O1±x journal July 1975
On the structural and morphological relationships between the VOx and β-vanadium suboxides in the two-phase system journal May 1970
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set journal July 1996
Nonvolatile electrochemical memory at 600°C enabled by composition phase separation journal December 2024
Recent progresses on physics and applications of vanadium dioxide journal October 2018
Electrical characterization of metal-oxide-high-k dielectric-oxide-semiconductor (MOHOS) structures for memory applications journal April 2007
Silicon nanocrystal non-volatile memory for embedded memory scaling journal April 2007
Reactivity at the Lithium–Metal Anode Surface of Lithium–Sulfur Batteries journal November 2015
TiO2 Polarons in the Time Domain: Implications for Photocatalysis journal January 2022
A Combined Car−Parrinello QM/MM Implementation for ab Initio Molecular Dynamics Simulations of Extended Systems:  Application to Transition Metal Catalysis journal October 1997
Artificially controlled nanoscale chemical reduction in VO2 through electron beam illumination journal July 2023
Thermodynamics of multi-sublattice battery active materials: from an extended regular solution theory to a phase-field model of LiMnyFe1-yPO4 journal August 2023
Energy-efficient Mott activation neuron for full-hardware implementation of neural networks journal March 2021
Dynamical memristors for higher-complexity neuromorphic computing journal April 2022
Subthreshold firing in Mott nanodevices journal May 2019
Growth dynamics and photoresponse of the Wadsley phase V6O13 crystals journal January 2020
Layered vanadium and molybdenum oxides: batteries and electrochromics journal January 2009
Improved tangent estimate in the nudged elastic band method for finding minimum energy paths and saddle points journal December 2000
A climbing image nudged elastic band method for finding saddle points and minimum energy paths journal December 2000
A density-functional model of the dispersion interaction journal October 2005
Optimization methods for finding minimum energy paths journal April 2008
Density functional theory study of rutile VO 2 surfaces journal October 2012
Commentary: The Materials Project: A materials genome approach to accelerating materials innovation journal July 2013
A metal-insulator transition study of VO2 thin films grown on sapphire substrates journal December 2017
Volatile and non-volatile behavior of metal–insulator transition in VO 2 through oxygen vacancies tunability for memory applications journal July 2020
Phase separation in amorphous tantalum oxide from first principles journal July 2020
Crystallization dynamics probed by transient resistance in phase change memory cells journal May 2024
Ab initio calculations of free-energy reaction barriers journal January 2008
Reconfigurable Mott electronics for homogeneous neuromorphic platform journal December 2023
Ab initiomolecular dynamics for liquid metals journal January 1993
Projector augmented-wave method journal December 1994
Structural Relaxation Made Simple journal October 2006
Evaluating optimal U for 3 d transition-metal oxides within the SCAN+ U framework journal April 2020
Comprehensive derivation of bond-valence parameters for ion pairs involving oxygen journal September 2015
SPICE Modeling of Insulator Metal Transition: Model of the Critical Temperature journal January 2019
Understanding Controlled Ion Doping Mechanism of Vertical Sensing Electrochemical Random Access Memory Using Ion-Permeable Graphene Electrodes journal July 2023
Selective area doping for Mott neuromorphic electronics journal March 2023
Suppression of Metal-Insulator Transition in VO2 by Electric Field-Induced Oxygen Vacancy Formation journal March 2013
Spatiotemporal characterization of the field-induced insulator-to-metal transition journal August 2021
Reconfigurable perovskite nickelate electronics for artificial intelligence journal February 2022
Monoclinic superstructure V14O6 of the tetragonal solid solution of oxygen in vanadium journal January 2008
Activation diffusion of oxygen under conditions of the metal-semiconductor phase transition in vanadium dioxide journal May 2017
Classical and Quantum Dynamics in Condensed Phase Simulations conference June 1998
First-Principles Studies for Optimal Model of the Ni/YSZ Triple Phase Boundary in Solid Oxide Cells journal May 2023
From Spiking Neuron Models to Linear-Nonlinear Models journal January 2011
Recent Advances in Lithium Iron Phosphate Battery Technology: A Comprehensive Review journal December 2024
A Review on the Properties and Applications of WO3 Nanostructure−Based Optical and Electronic Devices journal August 2021
Electron-beam modification and electrical property recovery dynamics of vanadium dioxide films in semiconducting and metallic phases journal April 2015