Bulletin of the American Physical Society
APS March Meeting 2022
Volume 67, Number 3
Monday–Friday, March 14–18, 2022; Chicago
Session Q10: Computational Modeling of Materials for Energy Applications IRecordings Available
|
Hide Abstracts |
Sponsoring Units: GERA Chair: Benjamin Paren, Massachusetts Institute of Technology Room: McCormick Place W-181A |
Wednesday, March 16, 2022 3:00PM - 3:12PM |
Q10.00001: Ab initio Studies of the Electrochemical Properties of Zn and ZnO in Rechargeable Zn/MnO2 Batteries Birendra Ale Magar, Nirajan Paudel, Timothy N Lambert, Igor Vasiliev Zn has long been recognized as a promising anode material for aqueous rechargeable batteries because of its high theoretical capacity, low redox potential, high stability in ambient environments, non-toxicity, abundance, and low cost. However, Zn anodes have demonstrated low utilization and poor rechargeability in alkaline electrolytes due to the problems associated with surface passivation and dendrite growth. The electrochemical performance of Zn anodes in rechargeable alkaline Zn/MnO2 batteries is influenced by the structure and composition of the ZnO layer formed on the surface of metal Zn during the battery discharge. The crystal structure of ZnO formed in Zn anodes is known to contain defects and impurities, such as Zn and O vacancies, interstitial hydrogen, and alkali metal ions (Li, Na, K). We apply ab initio computational methods based on density functional theory to study the structural and electrochemical properties of Zn and ZnO in rechargeable Zn/MnO2 batteries. Our calculations show that the formation energies of charged defects and impurities in ZnO are strongly affected by the position of the Fermi level and the applied anode potential. The existence of Zn and O vacancies changes the band structure and optical properties of ZnO. The results of our study suggest that the presence of defects and impurities in ZnO has a significant impact on the electrochemical properties of Zn anodes. |
Wednesday, March 16, 2022 3:12PM - 3:24PM |
Q10.00002: Magnetic structure, mechanical stability and thermoelectric properties of Quaternary Heusler Alloys: First-principles calculations Hind Alqurashi, Bothina Hamad First-principal calculations were performed to investigate the structural, thermodynamic, dynamical, mechanical, electronic, magnetic, and thermoelectric (TE) properties of quaternary-Heusler alloys (QHAs) with the chemical formula of XX′YZ. Here the X, X′, and Y are transition metal atoms, while Z is a main group element. Several alloys were found to have a half-metallic ferromagnetic structure with indirect band gaps, which is promising for future spintronic applications. They also show good TE properties and appreciable figure-of-merit (ZT) values that suggest them as good candidates for future thermoelectric applications. The TE properties of these quaternary alloys were found to exceed the values of the state-of-the-art thermoelectric materials. An example is the ZT value for a quaternary compound was found to be on the order of 1.0 as compared to that of Bi2Te3, which is less than 1 at its optimum temperature. |
Wednesday, March 16, 2022 3:24PM - 3:36PM |
Q10.00003: Origin of Rashba Spin Splitting and Strain Tunability in Ferroelectric Bulk CsPbF3 Preeti Bhumla, Saswata Bhattacharya Spin–orbit coupling (SOC) in conjunction with broken inversion symmetry acts as a key ingredient for several intriguing quantum phenomena, viz., persistent spin textures, topological surface states and Rashba–Dresselhaus (RD) effect. The coexistence of spontaneous polarization and the RD effect in ferroelectric (FE) materials enables the electrical control of spin degrees of freedom. Here, we explore the FE lead halide perovskite CsPbF3 as a potential candidate in the field of spintronics by employing state-of-the-art first-principles-based methodologies, viz., density functional theory (DFT) with semilocal and hybrid functional (HSE06) combined with SOC and many-body perturbation theory (G0W0). For a deeper understanding of the observed spin splitting, the spin textures are analyzed using the k.p model Hamiltonian. We find there is no out-of-plane spin component indicating that the Rashba splitting dominates over Dresselhaus splitting. Owing to the presence of Pb-6p orbital in conduction band, the large value of Rashba coefficient (αR) at conduction band minimum (CBm) is noticed in comparison to that of at the valence band maximum (VBM). We also observe that the strength of Rashba spin splitting can be substantially tuned on application of uniaxial strain (±5%). More interestingly, we notice reversible spin textures by switching the FE polarization in CsPbF3 perovskite, making it potent for perovskite-based spintronic applications. |
Wednesday, March 16, 2022 3:36PM - 3:48PM |
Q10.00004: Development of a universal machine learning descriptor from density functional theory data of ion adsorption and diffusion properties on Sulfer-functionalized MXenes for battery applicatations Gracie Chaney, Akram Ibrahim, Deniz Cakir, Can Ataca Two-dimensional materials composed of transition metal carbides and nitrides (MXenes) are hopeful candidates for energy storage devices, such as ion batteries and supercapacitors, on account of their high capacity and high-power capabilities. Additionally, adding Sulfur terminations decreases the diffusion energy barrier for some ions, increasing the devices’ efficiencies. In this work, we developed a database of adsorption energy and diffusion barriers for various adatoms (Li, Ca, Mg, Na, Al, and Zn) on nine M2CS2 monolayers (M: Cr, Hf, Mo, Nb, Ta, Ti, B, W, Zr). We found that Ca binds the most strongly to all of the MXenes, and that Zn binds the weakest in dilute concentrations. Our database also consists of coverage dependent formation energies and open-circuit voltages (OCVs) derived through cluster expansion. Finally, we go one step further and develop a machine learning descriptor from our data set to predict binding energy, adsorption geometry, charge transfer. This universal descriptor is trained to work successfully on multilayer M2CS2s and their heterostructures as well. |
Wednesday, March 16, 2022 3:48PM - 4:00PM |
Q10.00005: Predicting Lithium Transport Mechanisms Using Solvent Metrics With Experimentally-Validated Classical Molecular Dynamics Simulations Emily J Crabb, Graham A Leverick, Ryan Stephens, Yang Shao-Horn, Jeffrey C Grossman Lithium-oxygen batteries have higher energy densities than traditional lithium-ion batteries but are not yet commercially viable due to poor efficiency, high charging voltages, and low cycle lifetimes. These issues could be addressed with a deeper fundamental understanding of the atomistic behavior of these batteries, especially how different factors impact lithium transport behavior. We have used classical molecular dynamics (MD) simulations to examine lithium transport behavior in different solvents. We have validated our classical force fields by experimentally measuring the densities, viscosities, and ionic conductivities of our solvent–LiTFSI systems for comparison. However, our classical MD simulations have allowed us to investigate properties that are more difficult to access experimentally, such as the residence time of solvent molecules in the lithium solvation shell. Our atomistic simulations also allow us to examine whether a vehicular or solvent exchange mechanism is the dominant lithium transport mechanism in different solvents. Our goal in this work is to develop solvent metrics based on easily measured solvent properties that can be used to predict the microscopic lithium transport behavior in the solvent. |
Wednesday, March 16, 2022 4:00PM - 4:12PM |
Q10.00006: Thermoelectric properties of ternary Zintl-phase XAgP (X= Sr, Ag) compounds Rakshanda Dhawan, Hem C Kandpal, Tashi Nautiyal Rising need for inexhaustible energy sources has been a pressing factor for seeking effective thermoelectric (TE) materials. In this work, we examine the ABC-type compounds resulting from the combination of elements belonging to groups 2, 11, and 15 of the periodic table. Since semiconductors are usually good TE materials, we investigated the band structure of these compounds for existence of a band gap. Thus, we shortlisted two ternary Zintl compounds XAgP (X= Sr and Ba), which crystallize in the hexagonal structure with space group P63/mmc, and investigated these thoroughly. The TE performance was studied within the Boltzmann transport theory. At room temperature, SrAgP exhibits (mainly due to a large phonon group-velocity) slightly higher lattice thermal conductivity than for BaAgP. However, balanced values of other transport coefficients for SrAgP help raise its power factor and |
Wednesday, March 16, 2022 4:12PM - 4:24PM |
Q10.00007: Multi-mechanistic Strategies for Novel Solid Electrolytes with Superior Properties Hong Fang, Purusottam Jena Despite a wide range of solid electrolyte phases, most of them only exist at high temperatures. The challenge is to tailor the chemical compositions of solid electrolyte materials that yield high ionic conductivities and low activation energies at ambient temperature. This is crucial for the development of all-solid-state batteries that are both powerful and safe. Here, we report our recent works to meet this challenge by utilizing multiple mechanistic principles and clusters as the building blocks. We show that the atomic-level interactions that govern the fast-ion conduction can be optimized by incorporating polyanion dynamics, non-stoichiometry, point defects and strong ionic correlations. Specifically, two case studies of Li/Na solid electrolytes will be covered, including lithium solid electrolytes (SE) with record-high ionic conductivities at room temperature (over 100 mS/cm) and sodium SE with record-low activation energies (< 0.1 eV). |
Wednesday, March 16, 2022 4:24PM - 4:36PM |
Q10.00008: Simulating streaming current output of water evaporation driven carbon nanogenerator. Lassi Hällström, Tomi Koskinen, Camilla Tossi, Taneli Juntunen, Ilkka Tittonen Electricity generation from streaming current induced by water evaporation in nanostructured carbon material was first demonstrated in 2017[1]. Since then, the phenomenon has been demonstrated for a variety of different materials and the efficiency improved by modifying the nanoscale structure of the active material. We present a multiphysics simulation of power generation by water evaporation in a nanostructured porous film generator. A finite element model is used to compute the dynamics of the water flow in the device, simultaneously solving for both the liquid and vapor phase. |
Wednesday, March 16, 2022 4:36PM - 4:48PM |
Q10.00009: Exploring low lattice thermal conductivity materials using chemical bonding principles Jiangang He, Yi Xia, Wenwen Li, Koushik Pal, Yizhou Zhu, Mercouri G Kanatzidis, Christopher M Wolverton Semiconductors with very low lattice thermal conductivities are highly desired for applications relevant to thermal energy conversion and management, such as thermoelectrics and thermal barrier coatings. Although the crystal structure and chemical bonding are known to play vital roles in shaping heat transfer behavior, material design approaches of lowering lattice thermal conductivity using chemical bonding principles are uncommon. In this talk, we present an effective strategy of weakening interatomic interactions and therefore suppressing lattice thermal conductivity based on chemical bonding principles and develop a high-efficiency approach of discovering low κL materials by screening the local coordination environments of crystalline compounds. The followed first-principles calculations uncover 30 hitherto unexplored compounds with (ultra)low lattice thermal conductivities from thirteen prototype crystal structures contained in the inorganic crystal structure database. Furthermore, we demonstrate an approach of rationally designing high-performance thermoelectrics by additionally incorporating cations with stereochemically active lone-pair electrons. Our results not only provide fundamental insights into the physical origin of the low lattice thermal conductivity in a large family of copper-based compounds but also offer an efficient approach to discovery and design materials with targeted thermal transport properties. |
Wednesday, March 16, 2022 4:48PM - 5:00PM |
Q10.00010: Vacancy assisted oxygen redox stability in Na-cathode Kuan H Hsu Battery cathode material has been an increasingly popular research area due to the increasing demand for electric cars and energy storage solutions. However, designing a battery that has high energy density and high reversibility remains a challenge in modern research. Oxygen-redox active cathodes provide a promise for higher capacity than conventional cathodes, such as LiCoO2, but are prone to voltage hysteresis and capacity fading during charging cycles. However, recent studies showed an exceptional reversibility and low-voltage hysteresis of oxygen-redox active cathode, Na2Mn3O7 (NMO). In this work, we utilize ground state and excited state calculation to determine the redox mechanism of different sodium-based cathode material and investigate how defect structures can impact the stability of different cathode materials. |
Wednesday, March 16, 2022 5:00PM - 5:12PM |
Q10.00011: Theoretical Insights of Excitonic Effect in Lead Bromide Perovskites Manjari Jain, Saswata Bhattacharya Exciton binding energy is an important factor in photovoltaics as the formation of excitons influences the charge separation in solar cells. However, a detailed theoretical study of excitonic properties is rather demanding due to huge computational cost. We have systematically applied several state-of-the-art advanced first-principles based methodologies, viz., hybrid density functional theory combined with Spin–Orbit Coupling (SOC), Many Body Perturabtion Theory (MBPT), model-BSE, Wannier–Mott, and Density Functional Perturbation Theory (DFPT) approaches, to understand the excitonic properties by taking a prototypical model system of lead bromide perovskites, viz., APbBr3 [A=CH3NH3+ (MA), HC(NH2)2+ (FA), Cs+]. We show that via conventional procedure using GW/BSE approach along with SOC effect, it is very challenging to converge the BSE calculation to obtain the correct position of the excitonic peak to compute the exciton binding energy (EB) accurately. Therefore, we have employed Wannier–Mott and DFPT approaches to compute EB, where we find that the contribution of ionic dielectric screening is essential. In addition, we have calculated the exciton lifetime, which is in agreement with the trend observed (FAPbBr3 > MAPbBr3 > CsPbBr3) for electron–phonon coupling. The role of cation “A” for achieving the long-lived exciton lifetime is also explained and well understood. |
Wednesday, March 16, 2022 5:12PM - 5:24PM |
Q10.00012: Tuning Ionic Conductivity and Stability of Li10SnP2S12 Solid-State Electrolyte Santosh KC, Dirar Mashaleh Solid-State Electrolytes (SSEs) play a critical role in conducting ions between the cathode and anode materials in batteries. Unfortunately, most of the SSEs have not matched the ionic conductivity of their liquid counterparts. But, recent research of new materials has shown SSE can conduct ions at an equivalent or even higher rate. Using density functional theory (DFT), crystal structure, electronic and ionic properties of tin-based superionic conductors are investigated. The systematic study of compositional variation, phase stability, defects chemistry, and the impact on ionic conductivity is performed. This study provides significant insights into the ion conduction mechanism and strategy that can tune the ionic conductivity and stability. |
Wednesday, March 16, 2022 5:24PM - 5:36PM |
Q10.00013: Kinetics of CdTe(100) sublimation Indiras Khatri, Jacques G Amar One of the processes involved in the deposition of CdTe solar cells is closed-space sublimation. While a few first-principles calculations of the binding energies of Cd and Te atoms and/or CdxTey clusters have been carried out, the relevant desorption barriers and prefactors are still not known. In addition, experimental measurements of the temperature-dependent sublimation rate from the (100) CdTe surface have led to two significantly different values for the effective activation energy, depending on which experimental technique was used. Here we present the results of accelerated molecular dynamics simulations of Cd atom, Te atom, and Te2 dimer desorption for a variety of different configurations of the Cd-terminated and Te-terminated (100) surface which we have used to obtain key barriers and prefactors. Based on a steady-state assumption we find surprisingly good quantitative agreement between the temperature-dependent sublimation rate estimated from our simulations and experimental results. Our results also provide quantitative support for a previous suggestion that the sublimation rate is determined by a competition between two processes: vacancy nucleation and step-flow, each of which corresponds to a different activation barrier and turns on at different temperatures. |
Wednesday, March 16, 2022 5:36PM - 5:48PM |
Q10.00014: Ab initio study of Cs-containing uranium oxides Eunja Kim, Eduardo Montoya We have investigated Cs-containing uranium-oxides using density functional theory (DFT) in order to understand spent nuclear fuel (SNF) in long-term storage conditions. Predicting the chemical arrangement of molecular or crystal structures allows researchers a unique insight into the chemical behavior of many atomic frameworks. Those that have been studied extensively use empirical findings as a form of validation, tweaking and improving on the methodology for close accuracy and efficiency. These improvements are important for work on atomic systems that have yet to have been investigated experimentally due to legitimate safety concerns associated with radioisotopes. DFT is a tool used to investigate the ground state of an atomic system and is utilized in this research. The structure and physicochemical properties of pristine and Cs-containing uranium-oxides are the main focused of the study. There is yet any experimental data that can be used to validate our ongoing experimental results, so this research aims at providing it as well. Validity of both theory and experiment will be confirmed using various characterization methods, such as x-ray diffraction (XRD) or scanning electron microscopy (SEM). |
Follow Us |
Engage
Become an APS Member |
My APS
Renew Membership |
Information for |
About APSThe American Physical Society (APS) is a non-profit membership organization working to advance the knowledge of physics. |
© 2024 American Physical Society
| All rights reserved | Terms of Use
| Contact Us
Headquarters
1 Physics Ellipse, College Park, MD 20740-3844
(301) 209-3200
Editorial Office
100 Motor Pkwy, Suite 110, Hauppauge, NY 11788
(631) 591-4000
Office of Public Affairs
529 14th St NW, Suite 1050, Washington, D.C. 20045-2001
(202) 662-8700