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Reconfigurable Electronic Materials Inspired by Nonlinear Neuron Dynamics

Texas A&M University College of Engineering

Publications

Crystallographic variant mapping using precession electron diffraction data

Marcus Hansen, Ainiu Wang, Jiaqi Dong, Yuwei Zhang, Tejas Umale, Sarbajit Banerjee, Patrick Shamberger, Matt Pharr, Ibrahim Karaman, Kelvin Xie

Crystallographic variant mapping using precession electron diffraction data

July 4, 2023

In this work, we developed three methods to map crystallographic variants of samples at the nanoscale by analyzing precession electron diffraction data using a high-temperature shape memory alloy and a VO2 thin film on sapphire as the model systems. The three methods are (I) a user-selecting-reference pattern approach, (II) an algorithm-selecting-reference-pattern approach, and (III) a k-means approach. In the first two approaches, Euclidean distance, Cosine, and Structural Similarity (SSIM) algorithms were assessed for the diffraction pattern similarity quantification. We demonstrated that the Euclidean distance and SSIM methods outperform the Cosine algorithm. We further revealed that the random noise in the diffraction data can dramatically affect similarity quantification. Denoising processes could improve the crystallographic mapping quality. With the three methods mentioned above, we were able to map the crystallographic variants in different materials systems, thus enabling fast variant number quantification and clear variant distribution visualization. The advantages and disadvantages of each approach are also discussed. We expect these methods to benefit researchers who work on martensitic materials, in which the variant information is critical to understand their properties and functionalities.

Spontaneous Symmetry-Breaking of Nonequilibrium Steady–States Caused by Nonlinear Electrical Transport

Adelaide Bradicich, Timothy D. Brown, Sabyasachi Ganguli, R. Stanley Williams, Patrick J. Shamberger

Spontaneous Symmetry-Breaking of Nonequilibrium Steady–States Caused by Nonlinear Electrical Transport

June 25, 2023

Negative differential resistance (NDR) in certain materials has been attributed to spontaneous emergence of symmetry-breaking electrical current density localization from a previously homogeneous distribution, which is postulated to occur due to the nonequilibrium thermodynamic force of minimization of entropy production. However, this phenomenon has not been quantitatively predicted based on intrinsic material properties and an applied electrical stimulus. Herein an instability criterion is derived for localization of current density and temperature from a thermal fluctuation in a parallel conductor model of a thin film that is subject to Newton’s law of cooling. The conditions for steady–state electro-thermal localization is predicted, verifying a decrease in entropy production upon localization. Electro-thermal localization accompanied by a decrease of entropy production is confirmed in a multiphysics simulation of current flow in a thin film. The instability criterion predicts conditions for spontaneous current density localization, relating symmetry breaking fundamentally to dynamical instability via Local Activity theory.

Spontaneous Symmetry‐Breaking of Nonequilibrium Steady–States Caused by Nonlinear Electrical Transport

Adelaide Bradicich, Timothy Brown, Sabyasachi Ganguli, Stanley Williams, Patrick Shamberger.

Spontaneous Symmetry‐Breaking of Nonequilibrium Steady–States Caused by Nonlinear Electrical Transport

June 25, 2023

Negative differential resistance (NDR) in certain materials has been attributed to spontaneous emergence of symmetry-breaking electrical current density localization from a previously homogeneous distribution, which is postulated to occur due to the nonequilibrium thermodynamic force of minimization of entropy production. However, this phenomenon has not been quantitatively predicted based on intrinsic material properties and an applied electrical stimulus. Herein an instability criterion is derived for localization of current density and temperature from a thermal fluctuation in a parallel conductor model of a thin film that is subject to Newton’s law of cooling. The conditions for steady–state electro-thermal localization is predicted, verifying a decrease in entropy production upon localization. Electro-thermal localization accompanied by a decrease of entropy production is confirmed in a multiphysics simulation of current flow in a thin film. The instability criterion predicts conditions for spontaneous current density localization, relating symmetry breaking fundamentally to dynamical instability via Local Activity theory.

Protecting groups in insertion chemistry: Site-selective positioning of lithium ions in intercalation hosts

Joseph Handy, Wasif Zaheer, Ryan Albers, George Agbeworvi, Teak Boyko, Vladimir Bakhmoutov, Nattamai Bhuvanesh, Sarbajit Banerjee

Protecting groups in insertion chemistry: Site-selective positioning of lithium ions in intercalation hosts

February 21, 2023

The expanding toolbox of functionalization chemistries for selectively installing moieties on specific sites of a substrate underpins almost all modern organic and biochemical syntheses. Likewise, the installation of mobile guest ions in specific interstitial sites and their transport along specific diffusion pathways forms the basis of modern lithium (Li)-ion battery electrodes. Many insertion hosts afford a diverse range of accessible interstitial sites. However, site-selective positioning of cations with atomic precision remains almost entirely unexplored. Here, we show that by deciphering site preferences of co/pre-intercalated cations, we can position Li ions in four distinct sites within a 1D ζ-V2O5 insertion host. The use of topochemistry to effect single-crystal-to-single-crystal transformations enables atomic-resolution mapping of the selective positioning of Li ions through single-crystal X-ray diffraction. We image interstitial sites that are occupied at high depths of discharge, thereby obtaining unprecedented structural insight into “fully stuffed” frameworks critical for the realization of high-energy-density intercalation electrodes.

A reference-area-free strain mapping method using precession electron diffraction data

Dexin Zhao, Aniket Patel, Aaron Barbosa, Marcus Hansen, Ainiu Wang, Jiaqi Dong, Yuwei Zhang, Tejas Umale, Ibrahim Karaman, Patrick Shamberger, Sarbajit Banerjee, Matt Pharr, Kelvin Xie

A reference-area-free strain mapping method using precession electron diffraction data

February 10, 2023

In this work, we developed a method using precession electron diffraction data to map the residual elastic strain at the nano-scale. The diffraction pattern of each pixel was first collected and denoised. Template matching was then applied using the center spot as the mask to identify the positions of the diffraction disks. Statistics of distances between the selected diffracted disks enable the user to make an informed decision on the reference and to generate strain maps. Strain mapping on an unstrained single crystal sapphire shows the standard deviation of strain measurement is 0.5%. With this method, we were able to successfully measure and map the residual elastic strain in VO2 on sapphire and martensite in a Ni50.3Ti29.7Hf20 shape memory alloy. This approach does not require the user to select a “strain-free area” as a reference and can work on datasets even with the crystals oriented away from zone axes. This method is expected to provide a robust and more accessible alternative means of studying the residual strain of various material systems that complements the existing algorithms for strain mapping.

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Recent Publications

  • Intrinsic Nonlinearity Modulation in Two-Dimensional (Cu,Ag)InP2S6 for Selectorless Nonvolatile Memory Array
  • Alkali-Metal Interlocking of 2D V4O10 Sheets Defines Discretized Interlayer Shear Relationships
  • Low-cost calculation and analysis of 2D IR spectra of model diiron trinitrosyl complexes in the NO stretch region with vibrational perturbation theory
  • Magnetic and EPR Spectroscopic Studies of Thiolate Bridged Divalent Ni, Pd, and Pt Ions Capped with VO(N2S2) Metalloligands
  • Interlayer Exciton Polarons in Mesoscopic V2O5 for Broadband Optoelectronic Synapses

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