Article
Materials Science, Multidisciplinary
Alejandro Lopez-Bezanilla
Summary: Design principles are used to create dynamically stable transition metal, lanthanide, and actinide-based low-dimensional borides, predicting complex covalent heterostructures hosting Dirac states. Layered borides can be stacked in a layer-by-layer fashion to explore new physical properties and materials, with multiple Dirac states, highly dispersive electronic bands, and decoupled acoustic-optical phonon branches being studied.
PHYSICAL REVIEW MATERIALS
(2021)
Article
Materials Science, Multidisciplinary
Aurash Karimi, Michael Auinger
Summary: This study systematically investigates the diffusion of nitrogen in Ferrite and Austenite using a robust multiscale model combining Density Functional Theory and Kinetic Monte Carlo. Quantitative predictions are made for nitrogen diffusion in vacancy-rich iron crystals, providing valuable insights for nitriding manufacturers. The enhanced diffusion models may play a crucial role in improving existing processes and avoiding common manufacturing problems.
Review
Chemistry, Multidisciplinary
Edward Ditler, Sandra Luber
Summary: Vibrational spectroscopy is an important experimental technique for characterizing molecules and materials, but the interpretation of experimental results can be challenging. Computational studies using molecular dynamics simulations provide a valuable tool for understanding and predicting experimental results. This review article summarizes the field of vibrational spectroscopy using first-principles molecular dynamics and highlights recent advances in simulation techniques.
WILEY INTERDISCIPLINARY REVIEWS-COMPUTATIONAL MOLECULAR SCIENCE
(2022)
Article
Chemistry, Physical
Huijun Zheng, Yang-Yang Zhang, Tiantong Wang, Shuai Jiang, Wenhui Yan, Chong Wang, Ya Zhao, Han-Shi Hu, Jiayue Yang, Weiqing Zhang, Guorong Wu, Dongxu Dai, Gang Li, Jun Li, Xueming Yang, Ling Jiang
Summary: In this study, size-specific infrared spectra of neutral water nonamer (H2O)9 were obtained using threshold photoionization and a tunable vacuum ultraviolet free-electron laser. The spectra revealed distinctive OH stretch vibrational fundamentals, providing unique spectral signatures for the formation of an unprecedented (H2O)9 structure. This structure coexists with five previously identified structures, shedding light on the formation and growth mechanism of hydrogen-bonding networks in condensed-phase water.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Rocio Sanchez-de-Armas, Nicolas Montenegro-Pohlhammer, Aysegul Develioglu, Enrique Burzuri, Carmen J. Calzado
Summary: This study investigates the integration of SCO molecules on active nanodevices through quantum chemistry calculations, focusing on the encapsulation of Fe(ii) spin-crossover complexes in single-walled carbon nanotubes. The research reveals that the applied external electric field affects the spin-transition, and the local conditions of the substrate impact the transport properties.
Article
Chemistry, Physical
Mian Azmat, Abdul Majid, Mohammad Alkhedher, Sajjad Haider, Muhammad Saeed Akhtar
Summary: The prospect of using two-dimensional tetragonal samarium nitride (t-SmN) in photo-catalytic applications is being reported. First principles calculations were performed to study its structural, electronic, thermal, and photocatalytic properties. The material was found to be dynamically stable, thermally stable up to 1000 K, chemically inert at room temperature, and suitable for electrochemical reduction of water splitting. It also showed good light-harvesting ability from visible and ultraviolet regions of the solar spectrum.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Materials Science, Multidisciplinary
Nikola Koutna, Alexander Brenner, David Holec, Paul H. Mayrhofer
Summary: The study employs high-throughput density functional theory calculations to develop design guidelines for nanolaminates combining cubic transition metal nitride and/or carbide ceramics, identifying several top candidates for novel superlattice films. Key factors promoting interface-induced enhancement of hardness and/or fracture toughness include lattice parameter and shear modulus mismatch of the layer components.
Article
Chemistry, Multidisciplinary
Ruinian Xu, Ning Liu, Chengna Dai, Yan Li, Jie Zhang, Bin Wu, Gangqiang Yu, Biaohua Chen
Summary: By introducing H2O molecules on Cu-BEA zeolites, the selectivity, productivity, and long-term stability of direct oxidation of methane to methanol can be significantly improved.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Abdelazim M. Mebed, Muhammad Mushtaq, Muhammad Faizan, Riadh Neffati, Amel Laref, Sumegha Godara, Sana Maqbool
Summary: In this study, the adsorption of CO molecule on the (001) surface of Heusler alloy CrCoIrGa was investigated using DFT+U calculations. It was found that the surface retained the bulk atomic positions with no surface reconstruction, but had more spin-polarization and atomic moments due to the presence of unsaturated bonds. The most favorable adsorption configuration was found to be with the CO molecule adsorbed on the top of the Ir atom. This indicates a strong interaction (chemisorption) between the (001) surface and CO gas molecule, suggesting potential applications in gas sensing.
Article
Materials Science, Multidisciplinary
Xi Zhang, Sergiy Divinski, Blazej Grabowski
Summary: In this study, ab initio density-functional-theory calculations were used to investigate the vacancy formation and migration energies in HCP Al-Hf-Sc-Ti-Zr high entropy alloys (HEAs) and their subsystems. The temperature-dependent formation Gibbs energies and averaged atomic environments were obtained using the special quasi-random structure approach and statistical analysis. It was found that the temperature-dependent vacancy formation Gibbs energy had a negative configurational entropy contribution. The local cluster expansion technique was applied to explore extended vacancy migration phase spaces.
Article
Chemistry, Physical
David Ochoa-Resendiz, Antonio Gamboa-Suarez, Ramon Hernandez-Lamoneda
Summary: This article presents a detailed theoretical characterization of the structure and interactions in dichlorine clathrate hydrate cages, including the influence of halogen bonding and rotational motion. Monte Carlo simulations and energy decomposition analysis are used to further understand these effects.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Environmental Sciences
Ilya S. Sosulin, Vladimir Feldman
Summary: Difluoromethane is a potential environmentally friendly alternative to ozone depleting compounds. The formation of complexes between difluoromethane and water can suppress the radiation-induced degradation of difluoromethane.
Article
Chemistry, Physical
Juan J. J. Aucar, Alejandro F. F. Maldonado, Juan I. I. Melo
Summary: In this work, relativistic corrections to the electric field gradient (EFG) are presented, including spin-dependent corrections for the first time. The results show that these new corrections significantly improve the performance of the existing method and are in close agreement with calculations at the four-component Dirac-Hartree-Fock (4c-DHF) level. The accuracy of the EFG values obtained with this new method allows for the analysis of the electronic origin of relativistic effects using well-known nonrelativistic operators.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Materials Science, Multidisciplinary
Kirill N. Boldyrev, Vadim S. Sedov, Danny E. P. Vanpoucke, Victor G. Ralchenko, Boris N. Mavrin
Summary: The vibrational behavior of the germanium-vacancy (GeV) in diamond has been studied using photoluminescence spectrum and first-principles modeling. Two localized modes associated with the GeV center and neighboring carbon atoms have been identified, corresponding to the observed features in the photoluminescence spectrum.
DIAMOND AND RELATED MATERIALS
(2022)
Article
Materials Science, Coatings & Films
Petr Rehak, Jakub Ceska, Miroslav Cerny
Summary: Using a first-principles approach, the effect of oxygen as a substitutional impurity on the cohesion of three transition metal nitride multilayers was investigated. It was found that oxygen prefers to replace nitrogen atoms in interfacial planes and does not reduce the multilayer cohesion. In fact, in the AlN/TiN system, the presence of oxygen was found to increase the cohesion of the interface.
SURFACE & COATINGS TECHNOLOGY
(2023)
Article
Engineering, Environmental
Abhishek Meena, Pandiarajan Thangavel, Arun S. Nissimagoudar, Aditya Narayan Singh, Atanu Jana, Da Sol Jeong, Hyunsik Im, Kwang S. Kim
Summary: The self-supported oxovanadate-doped cobalt carbonate (VCoCOx@NF) on nickel foam (NF) is a high-performance catalyst for overall water splitting in alkaline-anionexchange-membrane-water-electrolyzer (AAEMWE). It shows excellent activity for both hydrogen and oxygen evolution reactions, reducing overpotentials and achieving overall water splitting at low cell voltages. The doping of V species enhances the HER and OER at the Co site, providing potential for large-scale hydrogen production utilizing V- and Co-based bimetallic oxide materials.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Materials Science, Multidisciplinary
In Young Choi, Sung-Doo Baek, Ashkan Vakilipour Takaloo, Seung Yong Lee, Amir Hajibabaei, Kwang S. Kim, Jae-Min Myoung
Summary: This study demonstrates a highly efficient pure-blue light-emitting diode (PeLED) by using a novel nanocomposite perovskite film as an emissive layer. The nanocomposite effectively reduces nonradiative recombination and enhances luminescence efficiency. The optimized nanocomposite layer also possesses a shallower valence band maximum, which is advantageous for hole injection in device operation.
ADVANCED OPTICAL MATERIALS
(2022)
Article
Chemistry, Physical
Muhammad Umer, Sohaib Umer, Mohammad Zafari, Miran Ha, Rohit Anand, Amir Hajibabaei, Ather Abbas, Geunsik Lee, Kwang S. Kim
Summary: This study highlights a new perspective for the rational design of transition metal single-atom catalysts (SACs) using density functional theory (DFT) and machine learning (ML) approaches. By embedding single atoms of 3d/4d/5d transition metals in different substrates, the electronic properties of 364 catalysts were tuned. Machine learning analysis identified stable and high-performance catalysts for hydrogen evolution reaction (HER) based on various descriptors. The study provides a fundamental understanding for the efficient rational design of TM-SACs for H-2 production through water-splitting.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)
Article
Chemistry, Physical
Abhishek Meena, Pandiarajan Thangavel, Da Sol Jeong, Aditya Narayan Singh, Atanu Jana, Hyunaik Im, Duc Anh Nguyen, Kwang S. Kim
Summary: Developing low-cost, efficient, and stable electrocatalysts are crucial for industrial high-purity hydrogen production. This study introduces an active pre-electrocatalyst that achieves high current density at low overpotential, meeting the commercial requirements for oxygen evolution reaction. Additionally, by combining with a non-noble metal-based HER catalyst, complete water-splitting is achieved in a highly corrosive alkaline environment, and an economically viable alkaline-anion-exchange-membrane water-electrolyzer is fabricated.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Physics, Condensed Matter
Amir Hajibabaei, Muhammad Umer, Rohit Anand, Miran Ha, Kwang S. Kim
Summary: This study applies on-the-fly machine learning potentials (MLPs) and sparse Gaussian process regression (SGPR) algorithm to optimize atomic structures quickly. The acceleration achieved is significant even for a single local optimization. It is found that, while MLPs have limited accuracy and may require switching to another algorithm for finding the exact local minimum, the algorithm is highly suitable for global optimization methods such as random or evolutionary structure searching or basin hopping, particularly due to the highly transferable MLPs.
JOURNAL OF PHYSICS-CONDENSED MATTER
(2022)
Article
Chemistry, Physical
Miran Ha, Amir Hajibabaei, Dong Yeon Kim, Aditya Narayan Singh, Jeonghun Yun, Chang Woo Myung, Kwang S. Kim
Summary: This study investigates the anion redox reaction in high-energy-density cathode materials using density functional theory and machine learning methods. The voltage/capacity fadings are suppressed by Al-doping, which enhances the structural stability and diminishes safety concerns. This research contributes to the design of stable reversible layered cathode materials.
ADVANCED ENERGY MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Bangaru Bhaskararao, Madeline E. Rotella, Dong Yeon Kim, Jung-Min Kee, Kwang Soo Kim, Marisa C. Kozlowski
Summary: Cooperative dual catalysis is a powerful strategy to achieve unique reactivity by combining catalysts with orthogonal modes of action. In this study, quantum mechanical calculations are used to reveal the mechanism of γ-butyrolactone formation using N-heterocyclic carbene organocatalyst and iridium catalyst. The calculated pathways agree with experimental findings, demonstrating the stereochemical features of the reaction.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Chang Woo Myung, Amir Hajibabaei, Ji-Hyun Cha, Miran Ha, Junu Kim, Kwang S. Kim
Summary: Metal halide perovskite (MHP) shows promising properties for various applications, but there is a gap between its applications and theoretical understanding. Machine learning approaches are proposed as a tool to overcome the theoretical obstacles in MHPs, highlighting ab initio ML potentials, materials design/optimization models, and data mining strategies.
ADVANCED ENERGY MATERIALS
(2022)
Article
Engineering, Environmental
Sandeep Kajal, Jaeki Jeong, Jongdeuk Seo, Rohit Anand, YeonJu Kim, Bangaru Bhaskararao, Chan Beom Park, Jiwoo Yeop, Anders Hagdfeldt, Jin Young Kim, Kwang S. Kim
Summary: Despite the recent increase in efficiency, perovskite solar cells (PSCs) still suffer from surface defects and ion migration, affecting their stability. In this study, we synthesized new materials with high binding energy and investigated their effects on defect passivation, ion migration, and device stability. The passivation treatment significantly improved the power conversion efficiency of PSCs, reduced hysteresis, and enhanced long-term stability, even without encapsulation.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Physical
Haiyan Jin, Miran Ha, Min Gyu Kim, Jong Hoon Lee, Kwang S. Kim
Summary: In this study, a novel atomically dispersed catalyst Pt@VNC consisting of Pt single atoms, Pt-Pt/V dual atoms, and small clusters supported on a vanadium and nitrogen co-doped carbon (VNC) surface is synthesized. By introducing atomically dispersed V sites and V2O5 clusters, the coordination structures of Pt atoms are modulated, showing extraordinary activity for the hydrogen evolution reaction. The synergistic effect of single atoms and clusters contributes to the low charge transfer resistance, fast reaction kinetics, superior catalytic efficiency, and robust durability of Pt@VNC.
ADVANCED ENERGY MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Miran Ha, Pandiarajan Thangavel, Ngoc Kim Dang, Dong Yeon Kim, Siraj Sultan, Jae Sung Lee, Kwang S. Kim
Summary: Researchers have developed a high-quality catalyst for chlorine evolution reaction (ClER) with near 100% selectivity, long-term durability, significant chlorine production, and vastly improved mass activity compared to industrial electrodes. The catalyst, composed of single platinum atoms dispersed in N-doped graphene, also exhibits ultra-low overpotential at typical operating temperatures in the chlor-alkali industries, consistent with theoretical calculations.
Article
Chemistry, Physical
Sandeep Kajal, Hyungsu Jang, Rohit Anand, Yun Seop Shin, Jung Geon Son, Jae Woong Jung, Jin Young Kim, Kwang S. Kim
Summary: Poor crystallization and nonradiative recombination are challenges faced by mixed-halide perovskite solar cells. Passivation is needed to suppress surface defects and improve charge carrier lifetime, but it must be done without disrupting the 3D symmetry. By using secondary amine passivation, the bulk phase of the perovskite material can be stabilized, leading to improved performance.
ACS APPLIED ENERGY MATERIALS
(2023)
Article
Chemistry, Physical
Rohit Anand, Babu Ram, Muhammad Umer, Mohammad Zafari, Sohaib Umer, Geunsik Lee, Kwang S. Kim
Summary: Designing efficient bifunctional and multifunctional catalysts is crucial for the development of clean and renewable energy technologies. By incorporating non-noble metal atoms onto the surface of MXenes, their properties can be modified. Using machine learning and density functional theory, we systematically screened and investigated different MXene combinations to explore their catalytic abilities.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)
Article
Chemistry, Multidisciplinary
Atanu Jana, Chang Woo Myung, Vijaya Gopalan Sree, Kwang S. Kim
Summary: In this study, non-toxic, zero-dimensional bulk organic-inorganic hybrid materials were developed, which exhibited upconversion and multiexciton generation along with a long lifetime. The multiexciton generation in these materials contributed to a high photoluminescence quantum yield, the highest among any other materials. This research provides a pathway for designing and synthesizing lead-free materials with upconversion and multiexciton generation properties, thus improving the performance of optoelectronic devices.
MATERIALS CHEMISTRY FRONTIERS
(2022)
Article
Chemistry, Physical
Miran Ha, Amir Hajibabaei, Saeed Pourasad, Kwang S. Kim
Summary: Universal machine learning interatomic potentials for saturated, olefinic, and aromatic hydrocarbons are generated using the Sparse Gaussian process regression algorithm. These potentials combine previously trained systems and cross-terms between new systems. The ML-IAPs, trained using density functional theory, accurately predicted various molecular structures and energies in testing.
ACS PHYSICAL CHEMISTRY AU
(2022)