Article
Physics, Multidisciplinary
Fangzhou Zhao, Mark E. Turiansky, Audrius Alkauskas, Chris G. Van de Walle
Summary: Trap-assisted Auger-Meitner recombination is highlighted as a dominant nonradiative process in wide-band-gap materials, and a first-principles methodology is presented to determine the rates of this process in semiconductors or insulators due to defects or impurities.
PHYSICAL REVIEW LETTERS
(2023)
Article
Chemistry, Physical
Yang Zhong, Zhenpeng Hu, Tongqing Sun, Yongfa Kong, Jingjun Xu
Summary: In this study, the crystal structures and optical properties of MAlBO3F (M = K, Rb, Cs) were systematically investigated using first-principles method, predicting 16 different crystal structures with potential applications in deep ultraviolet nonlinear optical crystals. The maximum birefringence and second-harmonic generation coefficients were found to be comparable or higher than those of known nonlinear optical crystals, providing useful clues for the search of new materials with desired optical properties.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Physics, Condensed Matter
Andrew J. Stollenwerk, Lukas Stuelke, Lilit Margaryan, Timothy E. Kidd, Pavel Lukashev
Summary: Metal/transition metal dichalcogenide interfaces are actively researched due to their potential for interplay of electronic and magnetic properties. Results from first principles calculations on Ni/WSe2 and Ni/MoS2 interfaces in thin-film geometry show metallic transition in layers adjacent to Ni, inducing moderate spin-polarization, while the electronic and magnetic properties of Ni remain largely unaffected. These findings provide a reference for experimental efforts on metal/dichalcogenide heterostructures with potential applications in modern magnetic storage devices.
JOURNAL OF PHYSICS-CONDENSED MATTER
(2021)
Article
Chemistry, Multidisciplinary
Haohong Song, De-en Jiang
Summary: This study investigated the interfacial chemistry between water and defected Ti3C2O2 MXene using first principles molecular dynamics simulations. The results showed that water molecules can repair the surface O vacancies by dissociating to hydroxide and hydronium. F terminal groups cannot effectively block water chemisorption, while Ti vacancies behave as a spectator species with respect to interaction with water.
Article
Chemistry, Multidisciplinary
Haohong Song, De-en Jiang
Summary: This study investigates the interfacial chemistry between water and defected Ti3C2O2 MXene using first principles molecular dynamics simulations. The results show that water molecules can repair surface defects, while F terminal groups cannot effectively block water adsorption on the Ti surface.
Article
Multidisciplinary Sciences
Alex M. Ganose, Junsoo Park, Alireza Faghaninia, Rachel Woods-Robinson, Kristin A. Persson, Anubhav Jain
Summary: The authors developed a computationally efficient method for calculating carrier scattering rates of semiconductors, which shows similar accuracy to state-of-the-art methods but at a much lower computational cost. This approach enables high-throughput computational workflows for accurate screening of carrier mobilities, lifetimes, and thermoelectric power.
NATURE COMMUNICATIONS
(2021)
Article
Multidisciplinary Sciences
Mohammad Bagheri, Hannu-Pekka Komsa
Summary: Raman spectroscopy is a widely-used non-destructive method for characterizing materials and determining their atomic structure and chemical composition. This study presents an optimized workflow for efficiently calculating Raman spectra using existing material databases. The workflow was validated by comparing the calculated spectra with experimental results, and high-throughput calculations were performed for a large number of materials from various classes, resulting in a comprehensive database of Raman spectra that agree well with experiments.
Article
Chemistry, Physical
Lihong Zhang, Shunqing Wu, Jianwei Shuai, Zhufeng Hou, Zizhong Zhu
Summary: The study investigated the formation energies of an oxygen vacancy (V-O) in bulk Pnma-Li2FeSiO4 using first-principles calculations, indicating that fully ionizing the oxygen vacancy in Li2FeSiO4 is energetically favorable. The presence of V-O results in a distinct redistribution of electronic charge densities around Fe and Si ions adjacent to the O-vacancy site.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Song Yu, Zenghua Cai, Deyan Sun, Yu-Ning Wu, Shiyou Chen
Summary: Defect types in layered semiconductors can be identified by matching STEM images with first-principles simulations. MoS2 antisite is dominant in PVD-grown MoS2 monolayer, and MoS may be mistaken as MoS2 due to similar structural distortion and ionization. Previous studies have overlooked the ionization and structural distortion of MoS. Considering defect ionization and associated structural distortion is necessary in STEM identification of defects in layered semiconductors.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Song Yu, Zenghua Cai, Deyan Sun, Yu-Ning Wu, Shiyou Chen
Summary: The defect types in layered semiconductors can be determined by comparing scanning transmission electron microscopy (STEM) images with first-principles simulations. The Mo-S2 antisite is found to be the dominant defect in PVD-grown MoS2 due to its matching structure in STEM images. However, MoS can also be mistaken for Mo-S2, as both have similar structural distortion and can be easily ionized under electron irradiation. The overlooked radiation-induced ionization and structural distortion of Mo-S highlight the necessity of considering these factors in STEM identification of defects in layered semiconductors.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Materials Science, Multidisciplinary
Wuzhang Fang, K. D. Belashchenko
Summary: Spin-orbit torques in a Mn2Au/heavy-metal bilayer, such as W or Pt, were calculated using the nonequilibrium Green's function technique. It was found that interfaces with W or Pt generate parallel dampinglike torques of opposite signs and antiparallel fieldlike and dampinglike torques that can penetrate deep into Mn2Au. The efficiency of the dampinglike torque depends strongly on the termination of the interface and the presence of spin-orbit coupling in Mn2Au.
Article
Chemistry, Physical
Xiaohang Lin, Anchen Shao, Minghao Hua, Xuelei Tian
Summary: The structural, electronic, and vibrational properties of water layers on Ag(100) and Ag(511) surfaces have been studied using first-principles calculations and ab initio molecular dynamics simulations. The most stable water structures and their vibrational spectra have been obtained. The results show that the water layer on the stepped Ag surface has high stability and crystal-like structure with long-range ordering at 140 K. The temperature increase from 140 K to 300 K leads to a red-shift in the vibrational spectra on Ag(100) due to changes in the number of H-bonded hydrogen. On Ag(511), a three-fold splitting of the O-H stretch mode is observed, which can be explained by the unique water structure on the stepped Ag surface.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Materials Science, Multidisciplinary
Da -Wei Wu, Yong -Bo Yuan, Shuang Liu, Meng-Qiu Long, Yun-Peng Wang
Summary: In this study, first-principles calculations were performed on NiBr2 monolayer, and it was found that the electric polarization is related to the spin-orbital coupling effect, with the Br atomic orbitals strongly hybridized with Ni orbitals being the major contributor to the polarization.
Article
Materials Science, Multidisciplinary
Banasree Sadhukhan, Anders Bergman, Yaroslav O. Kvashnin, Johan Hellsvik, Anna Delin
Summary: The study finds that low-dimensional magnets are more sensitive to atomic displacement and phonons due to thermal fluctuations. The spin-lattice coupling in the 2D ferromagnet CrI3 is investigated using relativistic first-principles study, and it is found to be significantly larger than in bulk systems. The magnetic interactions depend on both in-plane and out-of-plane motion of atoms, and the magnetic pair interactions change sign for specific atomic displacements.
Article
Chemistry, Multidisciplinary
Duy Khanh Nguyen, Chu Viet Ha, Le Hong Gam, J. Guerrero-Sanchez, D. M. Hoat
Summary: The effects of doping with alkaline earth metals (AEMs) on the structural, electronic, and magnetic properties of indium nitride (InN) monolayers are investigated. The results show that AEMs doping induces local structural distortion and half-metallicity, which have potential applications in the preparation of 2D spintronic materials.
Review
Chemistry, Multidisciplinary
Constantine Tsounis, Priyank Kumar, Hassan Masood, Rutvij Pankaj Kulkarni, Gopalakrishnan Sai Gautam, Christoph R. Mueller, Rose Amal, Denis A. Kuznetsov
Summary: MXenes, with their tailorable chemistry and favorable physical properties, have great potential in electrocatalytic energy conversion reactions. Further advances specific to electrocatalysis are required to fully exploit their potential. This review discusses the recent advances in performance, stability, compositional discovery and synthesis of MXenes, as well as their prospects in large scale synthesis and solution processing techniques.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Yishen Liu, Meijia Gu, Qihang Ding, Zhiyun Zhang, Wanxia Gong, Yuncong Yuan, Xiaofei Miao, Huili Ma, Xuechuan Hong, Wenbo Hu, Yuling Xiao
Summary: We developed efficient heavy-atom-free photosensitizers in the near-infrared (NIR) range using a facile approach. By modifying the thiopyrylium-based NIR-II dyads, our study showed that a sterically bulky and electron-rich moiety enhanced the intersystem crossing and electron excitation characteristics, resulting in significantly elevated reactive oxygen species (ROS) quantum yield. Our optimized lung-targeting nanoparticles enabled real-time NIR-II lung imaging and guided effective pulmonary coronavirus inactivation.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Smobin Vincent, Jin Hyun Chang, Pieremanuele Canepa, Juan Maria Garcia-Lastra
Summary: Rechargeable Mg-S batteries are attractive due to their high energy density and low costs. The poor cycling performance of Mg-S batteries is linked to the formation of insulating discharge products, but our research suggests that by controlling the oxidation process, the batteries can be improved.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
S. Swathilakshmi, Reshma Devi, Gopalakrishnan Sai Gautam
Summary: In this study, we evaluated the accuracy and computational efficiency of the recently developed metaGGA functional r(2)SCAN in transition metal oxide systems and compared it with SCAN. We assessed various properties of binary 3d TMOs calculated by r(2)SCAN, including oxidation enthalpies, lattice parameters, magnetic moments, and band gaps, and compared them with SCAN calculations and experimental values. Our results showed that including the U-correction with r(2)SCAN improved the description of TMOs' ground state properties with better computational efficiency than SCAN. The overall computational time required for r(2)SCAN(+U) was lower than SCAN(+U).
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Multidisciplinary
Zhaoqiang Zhang, Zeyu Deng, Hayden A. Evans, Dinesh Mullangi, Chengjun Kang, Shing Bo Peh, Yuxiang Wang, Craig M. Brown, John Wang, Pieremanuele Canepa, Anthony K. Cheetham, Dan Zhao
Summary: The exclusive capture of carbon dioxide (CO2) from hydrocarbon mixtures is crucial in the petrochemical industry. A new study introduces a ultramicroporous material, ALF, which can selectively capture CO2 from hydrocarbon mixtures with high capacity and efficiency. The material's unique pore chemistry allows for molecular recognition of CO2 by hydrogen bonding, while rejecting other hydrocarbons.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Stephanie C. C. van der Lubbe, Ziliang Wang, Damien K. J. Lee, Pieremanuele Canepa
Summary: Sodium vanadium fluorophosphate (NVPF) is a promising intercalation electrode material with high operation voltage, large capacity, and long cycle life. However, the high voltage plateau and reduced sodium-ion diffusivity limit its energy density. This study investigates the potential substitution of vanadium with other transition metals to address these issues and improve the energy density of NVPF.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Hengning Chen, Zeyu Deng, Yuheng Li, Pieremanuele Canepa
Summary: Niobate and tantalate coating materials can mitigate the interfacial reactivities in Li-ion and all-solid-state batteries by forming stable native defects and enhancing Li-ion transport. The multiphasic nature of Li-Nb-O and Li-Ta-O coatings, containing mixtures of LiNbO3 and Li3NbO4 or of LiTaO3 and Li3TaO4, was revealed through first-principles calculations.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Hayden A. Evans, Taner Yildirim, Peng Peng, Yongqiang Cheng, Zeyu Deng, Qiang Zhang, Dinesh Mullangi, Dan Zhao, Pieremanuele Canepa, Hanna M. Breunig, Anthony K. Cheetham, Craig M. Brown
Summary: This study demonstrates the remarkable hydrogen storage performance of aluminum formate at non-cryogenic temperatures and low pressures. The findings suggest that aluminum formate has potential for use in safe storage systems serving fuel cells.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Stephanie C. C. van der Lubbe, Pieremanuele Canepa
Summary: Understanding the thermodynamic properties of electrolyte solutions is crucial for various physiological and technological applications. By combining molecular dynamics and density functional theory, we can predict the static permittivity and ion size of a solution, enabling the application of relevant equations to electrolytes of any concentration and temperature.
NPJ COMPUTATIONAL MATERIALS
(2023)
Article
Chemistry, Physical
Thorben Boeger, Tim Bernges, Yuheng Li, Pieremanuele Canepa, Wolfgang G. Zeier
Summary: Solid electrolytes and solid-state batteries are gaining attention as a potential alternative to lithium-ion batteries, with increased energy density and safety. However, little is known about the thermal transport properties of solid electrolytes. This study reports the thermal properties of electrolytes in the argyrodite family and Li10GeP2S12 at different temperatures and porosities, finding that the thermal conductivities of solid electrolytes are similar to liquid electrolytes.
ACS APPLIED ENERGY MATERIALS
(2023)
Article
Materials Science, Multidisciplinary
Ziliang Wang, Tara P. Mishra, Weihang Xie, Zeyu Deng, Gopalakrishnan Sai Gautam, Anthony K. Cheetham, Pieremanuele Canepa
Summary: The development of high-performance sodium ion batteries requires improved electrode materials. The energy and power densities of NaSICON electrode materials show promise for large-scale energy storage applications. However, practical issues such as limited sodium extraction in low Na content NaSICONs present a challenge. Therefore, it is important to quantify the Na-ion mobility in a wide range of NaSICON electrodes.
ACS MATERIALS LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Chen Sun, Zeyu Deng, Zhiyuan Li, Zhongwei Chen, Xuanyu Zhang, Jian Chen, Haipeng Lu, Pieremanuele Canepa, Rui Chen, Lingling Mao
Summary: Hybrid organic-inorganic antimony halides with high photoluminescence quantum yield (PLQY) have gained attention for their non-toxicity and stability. Five pairs of antimony halides with different structures were synthesized and characterized to investigate the factors contributing to high PLQY. The antimony halides with square pyramidal geometry exhibited near-unity PLQY, while those with seesaw dimmer geometry showed PLQY close to 0%. The longer Sb center dot center dot center dot Sb distances in the square pyramidal structures and other factors such as Sb-Cl distance and stability of antimony chlorides may influence PLQY. The findings provide valuable insights for the precise design of highly emissive materials in optoelectronic applications.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Kamal Choudhary, Brian Decost, Lily Major, Keith Butler, Jeyan Thiyagalingam, Francesca Tavazza
Summary: Classical force fields based on machine learning methods have shown great potential for large scale simulations of solids. However, existing models are usually limited to specific systems. In this study, a unified atomistic line graph neural network-based force field model is developed, which can model structurally and chemically diverse solids with any combination of 89 elements from the periodic table. The model is trained and validated using a large dataset, demonstrating its accuracy and applicability.
Article
Chemistry, Physical
Aaron Jue Kang Tieu, Eunike Mahayoni, Yuheng Li, Zeyu Deng, Francois Fauth, Jean-Noel Chotard, Vincent Seznec, Stefan Adams, Christian Masquelier, Pieremanuele Canepa
Summary: The demand for cheaper and safer rechargeable batteries has led to a race to develop energy storage systems, with sodium-ion batteries emerging as a competitive alternative to lithium-ion batteries. By engineering the quantity of zirconium precursors, researchers have successfully synthesized zirconia-free Na SuperIonic CONductors (NZSP) as solid electrolytes, with impressive ionic conductivity and improved performance. These findings pave the way for further optimization of impurity-free complex solid electrolytes, which are crucial for the commercialization of solid-state batteries.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Materials Science, Multidisciplinary
Juefan Wang, Abhishek A. Panchal, Pieremanuele Canepa
Summary: Ion transport in materials plays an important role, but the variability in reported experimental results introduces challenges for accurate prediction. Machine-learned potentials have the potential to overcome these challenges, but their capabilities need to be critically assessed. This study evaluates the quality of a machine-learning potential based on the moment tensor potential formulation for ion transport in materials, highlighting the importance of high-quality training sets and considering intrinsic defects in solid electrolytes. The limitations posed by short-time and high-temperature simulations for predicting room-temperature properties are also demonstrated.