Article
Chemistry, Multidisciplinary
Nawras Abidi, Kang Rui Garrick Lim, Zhi Wei Seh, Stephan N. Steinmann
Summary: Electrified interfaces play a crucial role in energy technologies, but understanding and modeling them at an atomistic level is challenging due to their structural complexity and the presence of electrochemical potential. Realistic relationships between potential and surface charge require consideration of solvent and counter charge. However, the descriptions of solvent and electrolyte are limited by computational power, leading to validation issues in both explicit and implicit methods.
WILEY INTERDISCIPLINARY REVIEWS-COMPUTATIONAL MOLECULAR SCIENCE
(2021)
Article
Chemistry, Physical
Akash Shah, Amit H. Munshi, Anthony P. Nicholson, Aanand Thiyagarajan, Umberto M. Pozzoni, Walajabad S. Sampath
Summary: Atomistic modeling based on Density Functional Theory coupled with surface Green's function was used to investigate energy band alignment in cadmium selenium telluride (CdSeTe) surfaces. Results showed differences in surface geometry and band alignment features between CdSeTe and CdTe surfaces, which may help explain the lower performance of CdSeTe-only solar cells compared to CdTe-only devices.
APPLIED SURFACE SCIENCE
(2021)
Article
Polymer Science
Wesley Michaels, Yan Zhao, Jian Qin
Summary: The study developed all-atom force fields for undoped and highly doped PEDOT systems, which showed significant improvements in simulating molecular structures and properties compared to GAFF. Meaningful differences were identified between undoped and highly doped PEDOT, with the optimized force fields capturing the finite size of charge carriers in doped PEDOT models.
Article
Nanoscience & Nanotechnology
Anthony P. Nicholson, Akash Shah, Ramesh Pandey, Amit H. Munshi, James Sites, Walajabad Sampath
Summary: This study employs a synergistic approach combining first-principles atomistic modeling with numerical device simulations to investigate the role of heterointerfaces in metal-chalcogenide-based photovoltaic technologies. The atomic-scale study of two interfaces in cadmium-telluride-based thin-film solar cells reveals the mechanisms contributing to device performance variations. Computational results show contrasting electronic structures and charge transport behavior between the Schottky barrier forming Al/CdTe interface and the Type I Te/CdTe heterojunction. The cadmium termination exhibits greater band bending features compared to the tellurium termination, leading to a 3.6% higher photovoltaic conversion efficiency for the cadmium termination. This research highlights the importance of atomic-scale interfacial properties for the performance of cadmium telluride solar cells.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Polymer Science
Wesley Michaels, Yan Zhao, Jian Qin
Summary: Poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) is a crucial conductive polymer complex in electronic devices. Density functional theory (DFT) and molecular dynamics (MD) studies have been used to investigate nanoscale details of this system, with different density functionals (DFs) showing varying accuracy in predicting properties of the system. Studies find that reducing Hartree-Fock exchange in DFs may lead to improved predictions of certain properties of the PEDOT:PSS system.
Article
Chemistry, Physical
Jonathan E. Moussa
Summary: Statistical model selection can be used to compare atomistic simulation methods with different costs, accuracies, transferabilities, and numbers of empirical parameters. These comparisons are helpful for developing new methods that balance cost and accuracy.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Review
Multidisciplinary Sciences
Aleksey Fedotov, Alexander Vakhrushev, Olesya Severyukhina, Anatolie Sidorenko, Yuri Savva, Nikolay Klenov, Igor Soloviev
Summary: This paper presents an analytical review of theoretical methods for modeling functional nanostructures, including the evolution of quantum-mechanical modeling and the basics of the electron density functional theory. It also introduces common approximations and approaches in quantum mechanics, as well as various options for describing the exchange-correlation energy.
Article
Chemistry, Multidisciplinary
Haiqing Wan, Xianbo Xiao, Yee Sin Ang
Summary: This study investigates the quantum transport properties of graphene nanoribbons (GNRs) with different edge doping strategies. The results show that boron and nitrogen edge doping on the electrodes region can significantly alter the electronic band structures and transport properties of the system. Remarkably, this edge engineering strategy transforms GNR into a molecular spintronic nanodevice with exceptional transport properties, such as dual spin filtering effect, spin rectifier, and negative differential resistance. These findings suggest a potential route for developing high-performance graphene spintronics technology using an electrode edge engineering strategy.
Article
Chemistry, Physical
B. B. Yin, J. S. Huang, W. M. Ji, K. M. Liew
Summary: Diamond nanothread (DNT) has been found to significantly improve frictional resistance of polymer composites. Atomistic simulations and density functional theory calculations reveal that DNT reduces the friction coefficient of the composites by enhancing interfacial interactions, and nitrogen-doped DNT further improves frictional resistance. The improvement is less significant at elevated temperatures due to decreased interfacial shear strength.
Article
Geochemistry & Geophysics
Eril Suhada Lanin, Hiroki Sone, Zheng Yu, Qitong Liu, Bu Wang
Summary: The study compares the elastic properties of biotites recovered by spherical nanoindentation with those predicted from density functional theory (DFT) simulations. Most of the nanoindentation modulus results are below the values inferred from the simulation results representing ideal defect-free minerals. Crystal defects, potentially ripplocations, are suggested to be the dominant cause of the lower indentation modulus recovered from nanoindentation compared to those inferred from DFT simulations.
JOURNAL OF GEOPHYSICAL RESEARCH-SOLID EARTH
(2021)
Article
Chemistry, Physical
Shujie Zhang, Kejiang Li, Yan Ma, Feng Guo, Chunhe Jiang, Zeng Liang, Yushan Bu, Jianliang Zhang
Summary: By conducting DFT calculations with various simulation parameters and pseudopotentials, the structures and properties of iron oxides were investigated. The strong coupling between O's 2p orbital and Fe's 3d orbital was found, and the Hubbard-U correction significantly improved the results. General principles for future DFT calculations of iron oxides were provided.
Article
Chemistry, Multidisciplinary
Matthias van den Borg, Daniel Gaissmaier, Donato Fantauzzi, Edwin Knobbe, Timo Jacob
Summary: The study identified negatively charged centers on metallic lithium surfaces as the origin of hydrogen formation, with strikingly low reaction barriers suggesting a self-supporting effect between hydrogen evolution and lithium degradation. Through periodic density functional theory calculations, the initial mechanisms for surface reactions of metallic lithium with water from the gas phase were investigated, focusing on the adsorption/absorption structures and diffusion and dissociation processes of hydrogen, OH, and H2O.
Review
Pharmacology & Pharmacy
Naike Ye, Zekai Yang, Yuchen Liu
Summary: This article reviews the recent advances in using density functional theory (DFT) in molecular modeling studies of COVID-19 pharmaceuticals. It provides an overview of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) drugs and targets, introduces the basic principles and application methods of DFT, discusses different approaches of applying DFT, and highlights important factors to consider when incorporating DFT in future drug modeling research.
DRUG DISCOVERY TODAY
(2022)
Article
Engineering, Chemical
Sungil Yun, Feiyang Ou, Henrik Wang, Matthew Tom, Gerassimos Orkoulas, Panagiotis D. Christofides
Summary: Atomistic simulations using density functional theory and a kinetic Monte Carlo method were used to investigate the area-selective atomic layer deposition (ASALD) process with the integration of small-molecule inhibitors (SMIs) for improved regioselectivity of thin-layer deposition. The simulation results were in good agreement with experimental findings.
CHEMICAL ENGINEERING RESEARCH & DESIGN
(2022)
Article
Engineering, Electrical & Electronic
Xi Ding, Ming Tao, Junhua Li, Mingyuan Li, Mengchao Shi, Jiashu Chen, Zhen Tang, Francis Benistant, Jie Liu
Summary: This paper proposes an efficient method using deep neural networks to model atomistic dopant migration, showing high accuracy and speed compared to traditional DFT-based methods through NEB simulations.
MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
(2022)
Article
Nanoscience & Nanotechnology
Pingzhi Zhang, Zhufeng Hou, Li Jiang, Jack Yang, Wissam A. Saidi, Oleg Prezhdo, Wei Li
Summary: The study reveals that higher temperatures enhance both inelastic and elastic electron-phonon interactions in quaternary Cu2ZnSnS4 (CZTS), leading to a more significant electron-phonon coupling. With increasing temperature, the enhanced inelastic electron-phonon scattering accelerates the loss of charge carrier lifetimes, deteriorating the performance of optoelectronic devices.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Physical
Peng Song, Zhufeng Hou, Pedro Baptista de Castro, Kousuke Nakano, Kenta Hongo, Yoshihiko Takano, Ryo Maezono
Summary: In this work, a global search for crystal structures of ternary MgScH hydrides (MgxScyHz) under high pressure was performed using the evolutionary algorithm and first-principles calculations. The thermodynamic convex hull and pressure-dependent phase diagram of MgxScyHz for a wide range of compositions were computed. No stable compounds were found in the hydrogen-rich range, while four thermodynamically stable compounds with superconductivity were identified in the hydrogen-middle range.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Multidisciplinary Sciences
Peng Song, Zhufeng Hou, Pedro Baptista de Castro, Kousuke Nakano, Yoshihiko Takano, Ryo Maezono, Kenta Hongo
Summary: Using crystal search and first-principle calculations, multiple high-pressure YMgHx phases were discovered, some of which exhibit high superconducting transition temperatures (Tc). It was found that H-rich phases have higher Tc due to larger H-driven electronic and phonon density of states, as well as larger electron-phonon coupling strength.
ADVANCED THEORY AND SIMULATIONS
(2022)
Article
Chemistry, Multidisciplinary
Jingjing Li, Wei Xia, Jing Tang, Yong Gao, Cheng Jiang, Yining Jia, Tao Chen, Zhufeng Hou, Ruijuan Qi, Dong Jiang, Toru Asahi, Xingtao Xu, Tao Wang, Jianping He, Yusuke Yamauchi
Summary: This study demonstrates the use of a special ultrathin nitrogen-doped graphene nanomesh as a scaffold for highly exposed Fe-N-4 active sites. By adjusting the pore sizes of the nanomesh, highly loaded single-atom catalysts can be synthesized, which exhibit superior performance in oxygen reduction reactions and fuel cell tests. This work provides a novel strategy for constructing highly exposed transition metals and nitrogen co-doped carbon materials catalysts.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Wei Xia, Zhufeng Hou, Jing Tang, Jingjing Li, Watcharop Chaikittisilp, Yena Kim, Koki Muraoka, Hongjuan Zhang, Jianping He, Buxing Han, Yusuke Yamauchi
Summary: In this work, materials informatics techniques were used to predict the properties of nanoporous carbon-based electrocatalyst. A suitable oxygen reduction reaction (ORR) catalyst was identified and fabricated as a single-atom catalyst with predictable structures. The results showed that the designed catalyst exhibited outstanding electrocatalytic activity, which is of great significance for the practice of inorganic synthetic chemistry.
Article
Chemistry, Multidisciplinary
Xiao-Hong Shi, Ya-Ping Wang, Xinrui Cao, Shunqing Wu, Zhufeng Hou, Zizhong Zhu
Summary: This study compares the charge compensation mechanisms in the delithiation processes of LiNi1/3Co1/3Mn1/3O2 (NCM111) using first-principles calculations. The results show that different sets of U values lead to different charge compensation mechanisms. Experimental charge compensation processes are crucial in evaluating theoretical calculations. The calculations also reveal better voltage platforms in the GGA+Ui methods (i = 1, 2, 3) compared to the GGA method. Additionally, the redox reactions and formation energies of oxygen vacancies are investigated, providing insights for improving the stability of lattice oxygen.
Article
Nanoscience & Nanotechnology
Ningjing Luo, Lianggang Feng, Huimin Yin, Andreas Stein, Shuping Huang, Zhufeng Hou, Donald G. Truhlar
Summary: This study investigates the effect of Mn substitution on the oxygen redox mechanism in Li-excess transition metal-oxide cathode materials and finds that Mn substitution effectively inhibits the formation of peroxo and superoxo species. The results provide important insights for the design of high-capacity lithium-ion battery cathode materials.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Multidisciplinary
Meiping Li, Qing Lv, Wenyan Si, Zhufeng Hou, Changshui Huang
Summary: Iron single-atom catalysts synthesized using graphdiyne as the carbon substrate exhibit excellent catalytic performance. The catalyst accelerates the reaction kinetics and enhances its oxygen reduction reaction (ORR) activity by regulating the electronic structure of iron atoms and optimizing the adsorption energy of ORR intermediates on the active sites. Furthermore, high power density and long-term performance are demonstrated in a zinc-air battery application.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Ningjing Luo, Zhufeng Hou, Guo-Liang Chai
Summary: This study systematically explores the catalytic activity of tungsten monocarbide (WC) by studying the methane dehydrogenation and C-C coupling processes on WC surfaces using density functional theory (DFT) calculations. The results indicate that the W-terminated WC(0001) surface is the most favorable exposed surface with a lower surface energy. Additionally, the Co(111), Ni(111), and W-terminated WC(0001) surfaces exhibit similar catalytic properties in methane dehydrogenation, and the rate-limiting step on the W-terminated WC(0001) surface is the dissociation of CH*. C-C coupling through CH* intermediates on the W-terminated WC(0001) surface favors the formation of C2H2 kinetically.
APPLIED SURFACE SCIENCE
(2022)
Article
Chemistry, Physical
Ruikuan Xie, Zhufeng Hou, Guo-Liang Chai
Summary: This study investigates the potential of Heusler alloys as catalysts for electrochemical CO2 reduction reactions (ECO2RR) using density functional theory calculations. It breaks the linear scaling relationship between adsorption energies of CHO (and COOH) and CO intermediates, allowing for regular tuning of overpotential. Cu2ZnAl is found to be the most active catalyst, with 41% improvement in energy efficiency compared to pure Cu electrode. The study also encourages further exploration in this research area by suggesting the search for promising candidates among the thousands of Heusler alloys discovered experimentally.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Energy & Fuels
Rong Guo, Zhufeng Hou, Jianshan Chen, Yeyan Qin, Guoliang Chai, Yuangen Yao
Summary: This study reveals the effect of NaY zeolite support on Pd-based catalysts in the CO2 carbonylation reaction with MN through experiments and theoretical simulations. The experimental results show that the activity of the catalysts increases when the Si/Al molar ratio of NaY zeolite is increased within the range of 1.37 to 1.75, but decreases when the Si/Al ratio reaches 2.33. The theoretical simulations indicate that the CO adsorption strength is influenced by both the Si/Al ratio and the distribution pattern of Al substitutions.
Article
Chemistry, Physical
Pingzhi Zhang, Bojun Chang, Ting Xue, Rui-Xue Ding, Chuan-Jia Tong, Zhufeng Hou, Wei Li
Summary: This study investigates the electron-vibration interaction and the dependence on anion composition in CZTSSe materials using computational simulations. The results show that CZTSSe alloy has smaller electron-phonon coupling strength, potentially leading to better charge transport. The study also explores the interplay between disordered structures and S/Se stoichiometry.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Multidisciplinary
Ningjing Luo, Zhufeng Hou, Chensheng Lin, Guo-Liang Chai
Summary: The stable ordered phases of W2C are determined by the attractive interaction of carbon vacancies in the L3-type lattice, while the disordered phase is stabilized by its configuration entropy. The phase transformation between different structures of W2C is facilitated by the migration of carbon atoms through a sequential intralayer mechanism.
CRYSTAL GROWTH & DESIGN
(2023)
Article
Chemistry, Physical
Meiping Li, Zhufeng Hou, Xiaodong Li, Changshui Huang, Qing Lv
Summary: Single-atom metal-N-x sites show excellent catalytic properties and have gained increasing attention. Typically, these metal atoms depend heavily on N atoms for anchoring to the carbon substrate. However, the low content of N due to post-treatments limits the construction of diverse efficient single-atom active sites. In this study, hydrogen-substituted graphdiyne (HsGDY) is used as a carbon substrate to construct a cobalt atom electrocatalyst (Co-HsGDY) for the oxygen reduction reaction (ORR). The Co-HsGDY exhibits comparable catalytic activity to Pt/C and shows outstanding performance in a rechargeable zinc-air battery with high power density and superior long-term stability.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Xun Liu, Dabao Lu, Zhufeng Hou, Kenji Nagata, Bo Da, Hideki Yoshikawa, Shigeo Tanuma, Yang Sun, Zejun Ding
Summary: This study applies a machine learning method to predict electron inelastic mean free paths (IMFPs) for 42 inorganic compounds, and finds that machine learning is efficient and convenient for completing surface analysis databases.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
