Bulletin of the American Physical Society
APS March Meeting 2022
Volume 67, Number 3
Monday–Friday, March 14–18, 2022; Chicago
Session S10: Computational Modeling of Materials for Energy Applications IIRecordings Available
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Sponsoring Units: GERA Chair: Gabriel Landi, Instituto de F??sica da Universidade de Room: McCormick Place W-181A |
Thursday, March 17, 2022 8:00AM - 8:12AM |
S10.00001: Li doping effects on the electronic conductivity of WTe2 for energy storage devices: An ab initio investigation Aakash Kumar, Diana Y Qiu Transition metal dichalcogenides (TMDs) and other layered materials, also known as van der Waals (vdW) materials, are promising candidates as electrodes for solid-state battery applications. It is known that Li intercalation in these materials, e.g., MoS2, is accompanied by a semiconducting (2H) to metallic (1T) phase transition. Another TMD, WTe2 shows a unique opposite transition from a semi-metallic (Td) to a gapped (Td’) phase when Li is intercalated, a phenomenon only discovered very recently. These phase transitions lead to a change in the intrinsic electronic conductivity of TMDs, an important factor governing the rate-performance of the battery. Low electronic conductivity of the electrode impedes its ability to distribute the charge rapidly. Here, we employ ab initio density functional theory (DFT) and GW calculations to carefully examine the electronic structure of pristine and Li-doped bulk WTe2 to evaluate their applicability as electrodes in energy-storage devices, and the corresponding role of Li doping in the modification of its electronic bandstructure. We discuss the effective masses and carrier densities to elucidate the nature of the charge-transport in semi-metallic WTe2. Finally, we calculate the quasiparticle bandstructure of WTe2. |
Thursday, March 17, 2022 8:12AM - 8:24AM |
S10.00002: First-principles study of intra- and inter-valley scattering in thermoelectric materials Jesse Maassen, Vahid Askarpour A major goal of thermoelectric (TE) research is to develop materials with improved efficiencies. One strategy towards higher-performance TEs is band convergence, which seeks to align multiple electronic valleys within a narrow energy range. Theoretical modeling indicates that band convergence can lead to enhanced inter-valley scattering, which can reduce, or potentially offset, the benefits of this strategy. To help understand what controls the strength of inter-valley collisions, and their impact on TE properties, in this talk we present a density functional theory (DFT) study to characterize intra- and inter-valley electron-phonon scattering in six materials: three lead chalcogenides (PbS, PbSe, PbTe) and three half-Heuslers (ScNiBi, ScPbSb, ZrNiSn). The intra- and inter-valley scattering rates are analyzed by separating the contributions originating from the electron dispersion and from the electron-phonon coupling, to help elucidate the underlying factors that govern the scattering characteristics. We also propose a simple approach to estimate the inter-valley coupling strength, which is found to agree qualitatively with the rigorous results. These findings help guide our search of new and improved high-performance TEs. |
Thursday, March 17, 2022 8:24AM - 8:36AM |
S10.00003: Predicting Trends in the Bond Structure and Electronic Properties of Mixed-Transition-Metal Strontium Oxide Perovskites Francisco Marques dos Santos Vieira, Ismaila Dabo, Iurii Timrov, Matteo Cococcioni Solar radiation, the most abundant energy resource on Earth, can be converted to electricity using photovoltaic panels. For electrons to reach the absorber material, the top electrode of the device must be a transparent conductor (TC). The state-of-the-art material for this purpose is indium tin oxide. The availability of indium, a metal found in various ores at concentrations under 0.01%, limits the adoption of this technology, and has motivated the search for alternative TC. Cubic Sr-based perovskites SrMO3(M =V,Nb,Mo,W) show promise as technologically scalable TC if they can be stabilized against the formation of charge-compensating Sr vacancies [1,2]. Including multiple B cations may enable the Entropy stabilization [3] of this structure. To understand the effect of the coexistence of cations on the band structure and establish design rules for high entropy perovskites, the electronic properties of SrB1-xB’xO3 (B, B’={Ti,V,Cr,Nb,Mo,Ta,W} and x={0.25, 0.5, 0.75}) have been predicted from DFT+U calculations [4]. Four magnetic orderings of these systems were studied: the ferromagnetic, the antiferromagnetic phases with alternating planes of aligned spins in the [001], [110], and [111] directions. The effect of Sr deficiencies on the electronic properties are also investigated. |
Thursday, March 17, 2022 8:36AM - 8:48AM |
S10.00004: Descriptors to identify asymmetric conduction bipolar materials with ultra-high thermoelectric power factors Neophytos Neophytou, Patrizio Graziosi Low bandgap thermoelectric materials suffer from bipolar effects at high temperatures, with increased electronic thermal conductivity and reduced Seebeck coefficient, leading to reduced power factor and low ZT figure of merit. However, the presence of strong conduction asymmetries between the conduction and valence bands can allow high-phonon limited electronic conductivity at finite Seebeck coefficient values, leading to largely enhanced power factors. The power factors that can be achieved are significantly larger compared to their maximum unipolar counterparts, allowing for doubling of the ZT figure of merit. Using both advanced electronic Boltzmann transport calculations for realistic bandstructures as well as simplified parabolic electronic bands, including all relevant energy dependencies of scattering rates, we develop a series of descriptors which can guide machine learning studies in identifying such classes of materials with extraordinary power factors at nearly undoped conditions. For this we test more than 1500 analytical bandstructures and their features, and more than 60 possible descriptors, to identify the most promising ones that contain: i) only bandstructure features for easy identification from material databases, and ii) bandstructure and transport parameters that provide much higher correlations, but are somewhat more difficult to find parameters for. We validate the descriptors in cases from the half-Heusler material family and identify possible candidates. |
Thursday, March 17, 2022 8:48AM - 9:00AM |
S10.00005: Solid-liquid structure of Cu2S: Theoretical acanthite-like model for electronic and transport properties investigations. Ho Ngoc Nam, Katsuhiro Suzuki, Tien Quang Nguyen, Akira Masago, Hikari Shinya, Tetsuya Fukushima, Kazunori Sato Cu2S has long been studied for its potential applications in the field of photovoltaic solar cells and, most recently, thermoelectricity (TE) [1]. The interesting properties of this material are mainly driven by the liquid-like behavior of the Cu atoms, which is also a barrier that confuses us in determining their atomic positions and electronic properties [2]. In this work, using a theoretical model called the acanthite-like phase, we confirm the appearance of electronic structure with the indirect bandgap as observed experimentally before [3]. The formation of point defects and their influence on the conductive properties are also discussed. Finally, the use of the electron-phonon scattering approximation allows us to estimate the electron energy relaxation time, thereby reproducing the reasonable results of transport property compared to experimental observation. Therefore, demonstrating that the acanthite-like model is ideally suitable and can be used for computational design of TE material related to the low-temperature phase of Cu2S. |
Thursday, March 17, 2022 9:00AM - 9:12AM Withdrawn |
S10.00006: Microscopic mechanism of unusual lattice thermal transport in TlInTe2: Roles of anharmonic renormalization and wave-like tunneling of phonons Koushik Pal, Yi Xia, Christopher M Wolverton TlInTe2 represents a class of chain-like crystalline semiconductors (InTe, TlSe, TlGaTe2) that exhibit ultralow lattice thermal conductivity (κl). Here, we investigate the microscopic mechanism of the ultralow-κl in TlInTe2 using an advanced theory of lattice heat transport that considers contributions arising from the particle-like propagation as well as wave-like tunneling of phonons. While we evaluate the former term using the Peierls-Boltzmann transport equation, the latter quantity has been determined by calculating the off-diagonal (OD) components in the heat-flux operator using density functional theory. At each temperature, T, we anharmonically renormalize the phonon frequencies using the self-consistent phonon theory including quartic anharmonicity and utilize them to calculate κl. With the combined inclusion of the particle-like and OD contributions, and additional grain boundary scatterings, our calculations successfully reproduce available experimental results. Our analysis shows that the presence of the large quartic anharmonicity (a) strongly hardens the rattling phonon branches, (b) diminishes the three-phonon scattering processes at finite T, and (c) recovers the correct T-dependence of κl that deviates from T-1 behavior found in weakly anharmonic solids. |
Thursday, March 17, 2022 9:12AM - 9:24AM |
S10.00007: First-Principles Study of the Surface Properties of ZnO Anode Material in Rechargeable Zn/MnO2 Batteries Nirajan Paudel, Birendra A Magar, Krishna Acharya, Timothy N Lambert, Igor Vasiliev Zinc electrodes show promise for grid-scale energy storage systems because of their high theoretical capacity, stability, non-toxicity, and low cost. The performance of zinc anodes in aqueous alkaline batteries is affected by the structure and composition of a solid-state layer of ZnO grown on the surface of metal Zn. Recent studies have shown that the crystal structure of ZnO formed in zinc anodes could contain a large number of defects and impurities, such as O and Zn vacancies and interstitial hydrogen. The presence of defects and impurities in the structure of ZnO has a significant impact on the electrochemical properties and rechargeability of zinc anodes. We apply ab initio density functional computational methods to investigate the mechanisms of defect formation in the bulk and on the surface of ZnO. Our calculations show that the formation energies of O and Zn vacancies near the surface of ZnO are significantly lower than those in the bulk ZnO. The energies of hydrogen atoms attached to the surface of ZnO are found to be approximately 0.7 – 1.4 eV lower than the energies of hydrogen atoms inserted into the bulk ZnO. The results of our study suggest that the surface regions of ZnO have a strong influence on the electrochemical properties of zinc anodes. |
Thursday, March 17, 2022 9:24AM - 9:36AM |
S10.00008: The interaction of lithium with a monolayer of graphene monoxide Danylo Radevych, Marija Gajdardziska-Josifovska, Carol J Hirschmugl, Michael Weinert The interaction of Li atoms with a graphene monoxide (GmO) monolayer in various LixCyOy structures is investigated to determine if a monolayer of GmO can bind Li atoms and to predict the maximum theoretical capacity of this potentially new anode material for Li-ion batteries. Ab initio DFT calculations show that Li atoms are adsorbed on GmO by attaching to the O atoms and that Li atoms tend to repel during lithiation. An isolated Li atom prefers adsorption at the hollow site of the C sublattice, although the hollow site of the O sublattice, which is close in energy, may be preferable for multilayer systems. At the highest Li concentration, Li2C6O6 configuration for GmO is energetically stable and has the theoretical capacity of 957 mAh/g, which is 2.6 times higher than capacity of LiC6 in graphite. Analysis of the band structure and density of states show that the Li donates a large fraction of its valence electron to GmO, although there is also the formation of covalent Li-O bonds, thus facilitating the formation of Li+ ions when leaving the GmO monolayer. These characteristics are desirable for the battery anode material and suggest that GmO, especially in multilayer form, is a promising candidate. |
Thursday, March 17, 2022 9:36AM - 9:48AM |
S10.00009: Deep Learning Method to Accelerate Discovery of Effective Doping in Sr1-xRxFe1-yMyO3-δ Oxygen Carriers for Chemical Looping Air Separation Ali Ramazani, Eric J Popczun, Sittichai Natesakhawat, Jonathan W Lekse, Yuhua Duan Design and discovery of high-performance oxygen carrier materials play a crucial role in the energy applications (i.e. oxide fuel cells, cleaner fossil fuel combustion, etc.). Perovskite-type ABO3-δ oxides as oxygen carriers are receiving much attention recently due to their high thermal stability, good mechanical properties, and ability to reversibly and rapidly uptake and release oxygen. Furthermore, the flexibility in choosing the elemental composition of the A and B sites allows for the synthesis of many different perovskite-structured materials with inherently distinct oxygen storage properties. SrFeO3 is a promising oxygen carrying material due to its effectiveness and the low cost of iron. In the current work, the dopant chemical space in Sr1-xRxFe1-yMyO3-δ (R= La, K, Rb, Cs, Ca, Ba, Pd, Cu, Ag, Au, Cd, Hg, Tl, Pb, M= Co, Ni, Mn, Mo, Ti, Cu, Zn, x, y = 0, 0.125, 0.25, 0.375, 0.5, and δ = 0, 0.0625) is systematically explored using density functional theory (DFT) computations in combination with machine learning (ML) methods. We study a range of cationic dopants including alkali, alkaline earth metals, 3d, 4d, and 5d transition metal elements with and without an adjacent O vacancy. The effect of A and B site doping, both individually and in combination, on the oxygen ion diffusion considering oxygen vacancy formation energy is investigated utilizing DFT calculations. A linear programming approach is used to determine the energetically most favorable decomposition pathway (or products) and the corresponding decomposition energy. The dopants are then assessed based on the resistance of the doped oxide to decomposition, the tendency of O vacancy formation, and the site preference based on the decomposition energy. At the end, a predictive machine learning (ML) model is developed based on the data from DFT calculations and experiments for rational materials design and discovery by establishing a relationship between dopant features and the oxygen formation energy. |
Thursday, March 17, 2022 9:48AM - 10:00AM |
S10.00010: Rashba Spin-Splitting and Anomalous Spin Textures in the Bulk Ferroelectric Oxide Perovskite KIO3 Sajjan Sheoran, Saswata Bhattacharya The momentum-dependent Rashba and Dresselhaus spin-splitting has gained much attention for its highly promising applications in spintronics. Non-centrosymmetric structure and presence of spin-orbit coupling (SOC), lead to momentum-dependent spin-splitting of degenerate bands at non-time-reversal-invariant k-points. This lifts the Kramer’s degeneracy leading to Rashba and Dresselhaus splitting. In search of new ferroelectric Rashba semiconductors, here we present ferroelectric oxide perovskite KIO3, where the presence of heavy element (I), significant SOC and inversion asymmetric nature induce interesting band splitting. By employing state-of-the-art density functional theory (DFT) with semi-local and hybrid functional (HSE06) combined with SOC, we find non-negligible spin-splitting effect at conduction band minimum (CBm) and valence band maximum (VBM) for R3m and R3c phases. For a deeper understanding of the observed spin-splitting, we have analyzed the spin textures within the combined framework of DFT and k.p model Hamiltonian. Linear Rashba terms successfully explain the splitting at VBM. However, cubic terms become important in realizing spin-orientation near CBm. In R3c phase, four-band k.p model Hamiltonian including the pure orbital-degree of freedom coupled with the spin-degree of freedom is needed to completely understand the anomalous nature of the spin textures, which is beyond the conventional linear Rashba and Dresselhaus splitting. In a nonmagnetic system without SOC, all symmetry-protected degenerate levels are referred to as PODF. Our results show the enhancement in Rashba parameters on tuning the epitaxial strain. Further, we have observed reversal of spin-orientation on switching the direction of polarization. |
Thursday, March 17, 2022 10:00AM - 10:12AM Withdrawn |
S10.00011: Estimation of the Binary Interaction Parameters of the aNRTL Model using Molecular Simulations Rajasi Shukre, Rajesh Khare, Chau-Chyun Chen The adsorption Non-Random Two-Liquid (aNRTL) model captures the non-idealities in the adsorbed phase for mixed gas adsorption equilibria. The underlying premise of the model is based on the dominance of adsorbate-adsorbent interactions in the adsorbed phase. It regresses the binary interaction parameter which is used to calculate the adsorbed phase mole fractions and the activity coefficients. The binary interaction parameter is a measure of competitive adsorption of a binary gas mixture. This model requires regression of model parameters using experimental data. Unavailability or unreliability of experimental datasets in terms of missing uncertainties and fewer data points affects the regression process, thus impacting the model output. Therefore, it is extremely important to develop a methodology to estimate such parameters that do not make use of experimental adsorption data. Such an approach has been developed for the estimation of binary interaction parameters of the NRTL model using molecular dynamics simulations. In this study, we follow a similar approach to estimate the binary interaction parameters for a pair of adsorbate molecules in zeolites and MOFs using Monte Carlo and Molecular Dynamics Simulations. We derived equations relating the binary interaction parameters to the molecular parameters of the adsorbate-adsorbent interactions in the first coordination shell of each distinct adsorption site. The binary interaction parameters computed from molecular simulations gave an accurate prediction of the binary adsorption equilibria for the systems that were studied. |
Thursday, March 17, 2022 10:12AM - 10:24AM |
S10.00012: Thermoelectric behaviour of CuFeS2 from DFT simulations Vikram Vikram, Frances Towers-Tompkins, Sahil Tippireddy, Anthony V Powell, Umesh V Waghmare, Ricardo Grau-Crespo We will present a density functional theory (DFT) study of the electronic structure and thermoelectric behaviour of CuFeS2. Using Hubbard U corrections and Grimme’s dispersion corrections, we find values of bandgaps and cell parameters in good agreement with experiment. The electronic structure suggests significant covalent character of the Cu-S bonding and a more ionic Fe-S bonding in the lattice. We calculate electronic transport coefficients based on the Boltzmann’s transport equation with the relaxation time approximation. A model for energy- and temperature-dependent carrier relaxation time, based on the electronic density of states (DOS), gives a significant improvement over the constant relaxation time approximation (CRTA), giving a better fit to the electrical conductivities and a better estimate of the Seebeck coefficients. Lattice thermal conductivities (κL) calculated from DFT also compare well with the experimental values. We predict that nanostructuring would be an effective way to reduce κL in this material, although the effect is much less pronounced at the high temperatures of interest for applications, than at room temperature. We show that a figure of merit (zT) as high as 0.44 can be reached for the bulk sample at 673 K at a carrier concentration of 5×1020 cm-3. With the reduction of the particle size, a significant enhancement of the ZT values is predicted (up to zT ≈ 1.5 at 673 K and optimal carrier concentration). |
Thursday, March 17, 2022 10:24AM - 10:36AM |
S10.00013: Modeling Li Dendrite Formation in All-solid-state Lithium-ion Batteries Zhuolin Xia, Dilip Gersappe Li metal is considered as an ideal candidate for anode material of high energy all-solid-state Lithium-ion-batteries(ASS LIBs). Theoretically, using solid-state electrolytes(SSEs) with good mechanical strength is able to suppress Li dendrite growth. The dendrite problems still exist in ASS LIBs with Li anode as demonstrated in many studies. We present a 3D meso-scale model of ASS LIBs using the Lattice Boltzmann Method(LBM) that incorporates ion transport in the SSEs based on the Nernst-Planck equation and reaction kinetics at the electrode/electrolyte interface using modified Butler-Volmer equation. The porous geometries of the SSEs were included and their effects on the maximal transport ability of the system were studied. The results show that diffusion-limited current decreases as porosity increases or transport parameter decreases. The model was applied to simulate galvanostatic charge processes of ASS LIBs under various charge conditions. Using this approach, we obtained Li ion concentration in the electrolyte and captured the Li dendrite formation behavior. The dendrite growth and morphology which are attributed to inhomogeneous ion activities are not only dependent on the charge current and transport parameter but also associated with porous nature of the SSEs. |
Thursday, March 17, 2022 10:36AM - 10:48AM |
S10.00014: Novel Two dimensional MA2N4 (M=transition metal, A=Si, Ge) Materials for Renewable Energy Applications Asha S Yadav In the present work, based on first-principles calculations we explored members of the recently proposed new two-dimensional MA2Z4 (M=Ti, Zr, Hf, V, Nb, Ta, Cr, Mo, W; A= Si, Ge) family and classified them for different applications. Furthermore, electronic structure accurate hybrid HSE functionals and detailed descriptor property calculation of these compounds scrutinize the best possible compounds. Among these materials, MoGe2N4 and HfSi2N4 exhibit a reasonably high optical absorption coefficient and optical transition strength from the valence band to conduction band confirm its suitability for solar harvesting applications. However, the two-dimensional nature of both MoGe2N4 and HfSi2N4 reveal strong excitonic effects, as confirmed by GW+BSE calculations. Thickness-dependent spectroscopic limited maximum efficiency of MoGe2N4 turns out to be around 15.40 %, thus proposing the possibility to be a potential candidate for photovoltaic application. On the other hand, a suitable band edge position with respect to CO2 reduction potential and effective CO2 activation on HfSi2N4 recommend it for photocatalytic CO2 reduction. Interestingly, NbSi2N4 exclusively exhibits a recently proposed bipolar magnetic character and enables its active use for spin transport-based applications. |
Thursday, March 17, 2022 10:48AM - 11:00AM Withdrawn |
S10.00015: Stability limits and Mechanical Behaviors of Methane Gas Hydrates for use in Greenhouse Gas Mitigation Technologies Xiaodan Zhu, Alejandro Rey, Phillip Servio With the increasing crises of global warming phenomenon, Carbon dioxide (CO2) sequestration is an inevitable component during greenhouse gas mitigation. It aims to capture and store the CO2 gases in the atmosphere. Gas hydrates are potential material for CO2 sequestration due to their excellent storage capacity. The CO2 sequestration process is based on SI methane gas hydrates; methane is replaced by carbon dioxide. The pressures and temperatures surrounding the gas hydrates change during this process, making the hydrate structure unstable. This contribution will present the pressure stability limits of monocrystal defect-free methane gas hydrates, using accurate density functional theory (DFT) to simulate the hydrate's performance under varying pressure. The effects of pressure on this guest-host crystal's geometric and atomic bonding features are presented and analyzed using various atomic angle and bond length distribution functions. Comprehensive characterization of the elastic properties with pressure is presented and related to the crystal geometry changes. Taken together, these results contribute to understanding the methane gas hydrate stability under a great range of pressures and provide a comprehensive prediction of the hydrate's performance during CO2 sequestration. |
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