Article
Chemistry, Multidisciplinary
Liening Wei, Yang Li, Xuanyu Jiang, Pengcheng Wu, Xian Zhao, Lisong Zhang, Baoan Liu, Xiangxu Chai, Mingxia Xu, Xun Sun, Wei Hong
Summary: This study investigated the characteristics of potassium dihydrogen phosphate (KDP) crystals doped with Cr(NO3)3 at a level of approximately 10 ppm using UV-vis absorption spectrum, EPR spectroscopy, and first-principles calculations. The results show that Cr atoms substitute K atoms in KDP crystals, and charge compensation is achieved through two adjacent H vacancies.
Article
Multidisciplinary Sciences
Ryan T. Hannagan, Georgios Giannakakis, Romain Reocreux, Julia Schumann, Jordan Finzel, Yicheng Wang, Angelos Michaelides, Prashant Deshlahra, Phillip Christopher, Maria Flytzani-Stephanopoulos, Michail Stamatakis, E. Charles H. Sykes
Summary: The well-defined nature of single-atom-alloy catalysts allows for unambiguous theoretical modeling and precise surface science experiments, leading to the design of highly active, selective, and coke-resistant catalysts for low-temperature nonoxidative propane dehydrogenation.
Article
Chemistry, Physical
Lijing Wei, Feng Li, Shaoyuan Pang, Yinglong Wang, Jianxin Guo, Jianhui Chen
Summary: In this study, a simple, vacuum-free method was used to fabricate a polymer, Nafion, for passivating the outer-shell defects of Si nanowires (SiNWs). The results showed that the Nafion molecule could firmly adsorb on the surfaces of SiNWs, leading to a high stability of the Nafion-passivated SiNWs in a chemical environment. Additionally, the Nafion-passivated SiNWs exhibited a larger absorption coefficient and an equivalent quantum confinement effect compared to the H-passivated SiNWs.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Nanoscience & Nanotechnology
Zhi Li, Xianli Su, Xinfeng Tang
Summary: Among thermoelectrics, SnS is a promising candidate due to its low cost, abundance, and environmental friendliness. However, there are few theoretical studies on the charge and heat transport mechanism in SnS. This work reveals an abnormal optical-phonon-dominated L mode in SnS and highlights the essential role of optical phonons in charge transport. The findings suggest that SnS can achieve high thermoelectric performance without band engineering and identify dopants that effectively enhance the hole concentration.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Multidisciplinary
Peng Su, Han Ye, Naizhang Sun, Shining Liu, Hu Zhang
Summary: In this paper, the second harmonic generation (SHG) in Janus transition metal chalcogenide oxide monolayers was systematically investigated. The calculated results show that Janus MoSSe monolayer has comparable second-order nonlinear susceptibilities with other Janus MXO monolayers. The polarization-dependent responses of the MXO monolayers were demonstrated, and the effects of biaxial strain on band structures and SHG were further investigated.
Article
Chemistry, Multidisciplinary
Yanyan Zhan, Xuan Fang, Dengkui Wang, Dan Fang, Bobo Li, Jinhua Li, Xiaohua Wang
Summary: The band gap of lateral heterojunctions (LHSs) can be continuously tuned by changing the widths of their components. In this study, Sb/Bi LHSs based on monolayer Sb and Bi atoms with armchair and zigzag interfaces were constructed. It was found that these LHSs have adjustable band gaps and near-infrared absorption characteristics. These findings provide a new approach for the application of two-dimensional materials in near-infrared devices.
FRONTIERS IN CHEMISTRY
(2022)
Article
Nanoscience & Nanotechnology
Weijie Li, Xuan Fang, Dengkui Wang, Feng Tian, Haozhi Wang, Dan Fang, Jinhua Li, Xueying Chu, Hongbin Zhao, Dongbo Wang, Xiaohui Ma
Summary: This paper discusses the band structures and optical absorption properties of a seamless lateral heterostructure based on arsenene and antimonene along different interfaces. The study shows that the band gaps of heterostructure types are strongly influenced by atomic number, leading to unique optical absorption characteristics in the mid-infrared range.
PHYSICA E-LOW-DIMENSIONAL SYSTEMS & NANOSTRUCTURES
(2021)
Article
Chemistry, Physical
Zhihao Li, Xiucai Sun, Xiaoli Sun, Wan-Jian Yin, Zhongfan Liu
Summary: This study investigated the impact of substrate characteristics on the quality of graphene and found that the crystallographic orientation of the metal substrate, such as Cu (100), is crucial for producing high-quality and superclean graphene. The study also identified that low graphene defect density and high nucleation rate on the Cu(100) facet contribute to the suppression of amorphous carbon formation and facilitate rapid graphene synthesis.
Article
Chemistry, Physical
Javed Rehman, Xiaofeng Fan, M. K. Butt, Amel Laref, Van An Dinh, W. T. Zheng
Summary: Research on 2D materials like SnSe2 for Na and K ion batteries has shown promising results, with strong adsorption, conductive behavior, low activation barriers, and high theoretical capacity, making them potentially productive for commercialization.
APPLIED SURFACE SCIENCE
(2021)
Article
Chemistry, Physical
Manushi J. Patel, Dhara Raval, Sanjeev K. Gupta, P. N. Gajjar
Summary: The DFT analysis of cubic phase CsPbCl3 perovskite shows that both bulk and monolayer structures are dynamically stable. Doping with Mn and Nb results in shifted absorption edges towards lower photon energy, leading to improved efficiency in solar cells. The Nb-doped monolayer achieves a J(sc) of 655.45 A/m(2) and an efficiency of 15.68%, while the Mn-doped monolayer shows a J(sc) of 525.68 A/m(2) and a high efficiency of 26.88%, making it a promising candidate for solar cell applications.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Materials Science, Multidisciplinary
Yiming Ren, Yonghong Hu, Zhenglong Hu, Li Xue
Summary: The effects of Zn atoms on the electronic and optical properties of CuGaSe2 were investigated through first-principles calculations. It was found that the participation of Zn can improve the optical properties of solar cells.
RESULTS IN PHYSICS
(2021)
Article
Chemistry, Physical
Bakhtiar Ul Haq, M. M. Alsardia, I. B. Khadka, R. Ahmed, S. AlFaify, Faheem K. Butt, Zulfiqar Ali Shah, Se-Hun Kim
Summary: In this article, the physical behavior of Ti2SnX (X: C, N) compounds from the 211-MAX phases was reported, and a detailed analysis of their structural parameters, electronic structures, and optical spectra was provided in comparison with available literature. The calculations were based on the FP-LAPW method within the DFT. The compounds showed metallic properties with a considerable density of states over the Fermi level, symmetrical electronic structures, and negligible magnetic moments. The predicted structural and electronic properties were well-matched with the literature. The compounds exhibited static refractive indices and comprehensive discussions on light reflection and absorption were provided.
Article
Energy & Fuels
Mukaddar Sk, Saurabh Ghosh
Summary: This article systematically investigates the structural, electronic, optical, and thermoelectric properties of Cs2Tl(As/Sb)I-6, and predicts its potential as photovoltaic and thermoelectric materials.
INTERNATIONAL JOURNAL OF ENERGY RESEARCH
(2022)
Article
Biochemistry & Molecular Biology
Luca Sementa, Mauro Stener, Alessandro Fortunelli
Summary: A computational study was conducted on the optical absorption processes of Ag-20 and Au-20 clusters on the magnesium oxide (100) facet, with regular and point defect configurations. The interaction between the substrate and clusters induced broadening and red-shift of the excited states, which were further enhanced by the presence of oxygen vacancies.
Article
Chemistry, Physical
Ying Wei, Anwen Tang, Xiaojie He, Hong Chen, Huimin Yin, Yi Li, Yongfan Zhang, Shuping Huang
Summary: The potassium storage performance of UiO-66 derivatives was investigated using density functional theory calculations. The results showed that modifying the metal atoms in the UiO-66 nodes can affect the band gap and charge transfer processes. Proper modification can improve the electronic and ionic conductivity of UiO-66 when used as an anode material in potassium ion batteries.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Materials Science, Ceramics
Thomas Schwab, Hasan Razouq, Korbinian Aicher, Gregor A. Zickler, Oliver Diwald
Summary: Ion exsolution is crucial for engineering intergranular regions in ceramic microstructures. BaO admixtures trapped inside MgO grains undergo annealing-induced exsolution to generate photoluminescent surface and interface structures. The effects of BaO admixtures on grain coarsening and powder densification were compared using spectroscopy measurements and in-depth structure characterization.
JOURNAL OF THE AMERICAN CERAMIC SOCIETY
(2023)
Article
Materials Science, Ceramics
Hasan Razouq, Gregor A. Zickler, Thomas Berger, Nicola Huesing, Oliver Diwald
Summary: By mixing MgO nanoparticles with polyvinylalcohol (PVA), fiber structures with layered Mg(OH)2 nanosheets can be produced. Upon high-temperature calcination, the Mg(OH)2 nanosheets undergo dehydration, along with the removal of the polymer, resulting in staggered MgO nanoparticle ensembles in the fibers. Using methanol as a solvent in polyvinylpyrrolidone (PVP) fibers, the crys-tallinity and structure of MgO nanoparticles are preserved, forming nanoparticle threads with a cylindrical profile and particle size gradient after calcination.
CERAMICS INTERNATIONAL
(2023)
Article
Chemistry, Multidisciplinary
Ellie Neige, Thomas Schwab, Maurizio Musso, Thomas Berger, Gilles R. Bourret, Oliver Diwald
Summary: The fate of photogenerated charges within ferroelectric metal oxides is studied, focusing on the contributions of tetragonal distortion and point defects on charge separation and recombination in BaTiO3 (BTO) nanocrystals. The results show that BTO nanocrystals have significantly enhanced charge separation compared to TiO2 anatase nanocrystals, highlighting the beneficial effect of the BTO perovskite nanocrystal lattice. However, charge separation is hindered within BTO nanoparticles with higher annealing temperatures due to the formation of Ba-O divacancies.
Article
Chemistry, Physical
Henry W. Sprueill, Jenna A. Bilbrey, Qin Pang, Peter V. Sushko
Summary: Neural network potentials (NNPs) can accelerate atomistic simulations and allow broader sampling of structural outcomes and transformation pathways. In this study, an active sampling algorithm is demonstrated to train an accurate NNP for microstructural evolutions. The NNP is then used with a perturbation scheme to stochastically sample structural and energetic changes caused by shear-induced deformation, revealing a range of possible intermixing and vacancy migration pathways. The code for the active learning strategy and NNP-driven shear simulations is openly available.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Shashank G. G. Mehendale, Bo Peng, Niranjan Govind, Yuri Alexeev
Summary: The unitary coupled-cluster (UCC) ansatz is a commonly used chemically inspired approach in variational quantum computing. However, the standard UCC ansatz has an unfavorable scaling of the number of parameters with respect to the system size, which hinders its practical use on near-term quantum devices. This paper explores the parameter redundancy in the preparation of the unitary coupled-cluster singles and doubles (UCCSD) ansatz and proposes techniques to reduce the number of parameters and improve convergence time. Experimental results on small molecules demonstrate significant cost reduction and faster convergence compared to conventional UCCSD-VQE simulations. The potential application of machine learning techniques in further exploring parameter redundancy is also discussed as a future direction for research.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Physical
Michael J. Elser, Ellie Neige, Thomas Berger, Mario Chiesa, Elio Giamello, Keith McKenna, Thomas Risse, Oliver Diwald
Summary: Particle attachment and neck formation in TiO2 nanoparticle networks play a crucial role in determining the performance of materials in sensing, photo-electrochemistry, and catalysis. This study investigates a point defect that traps electrons and is predominantly found in aggregated TiO2 nanoparticle systems. The presence of this defect is explained by the incorporation of residual carbon atoms into the lattice during particle neck formation. This study provides important insights into the relationship between dopants, defects, and microstructural features in oxide nanomaterials.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Soumen Ghosh, Shaul Mukamel, Niranjan Govind
Summary: This letter investigates the predictive ability of multiconfiguration pair-density functional theory (MC-PDFT) for X-ray absorption spectra (XAS) by calculating the metal K pre‑edge features of aquated 3d transition metal ions in common oxidation states. It is found that MC-PDFT provides quantitatively accurate results for all excited states with significantly lower computational cost compared to restricted active-space second-order perturbation theory (RASPT2) and time-dependent density functional theory (TDDFT).
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Daniel Mejia-Rodriguez, Edoardo Apra, Jochen Autschbach, Nicholas P. Bauman, Eric J. Bylaska, Niranjan Govind, Jeff R. Hammond, Karol Kowalski, Alexander Kunitsa, Ajay Panyala, Bo Peng, John J. Rehr, Huajing Song, Sergei Tretiak, Marat Valiev, Fernando D. Vila
Summary: This paper provides an overview of the recent developments in the NWChem computational chemistry suite, including the functionality in the current stable release (NWChem 7.2.0) and the ongoing developments in the master development branch. It highlights the interfaces to quantum computing simulators, external libraries, the NWChem github repository, and containerization of NWChem executable images.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Physical
Rosa Di Felice, Maricris L. Mayes, Ryan M. Richard, David B. Williams-Young, Garnet Kin-Lic Chan, Wibe A. de Jong, Niranjan Govind, Martin Head-Gordon, Matthew R. Hermes, Karol Kowalski, Xiaosong Li, Hans Lischka, Karl T. Mueller, Erdal Mutlu, Anders M. N. Niklasson, Mark R. Pederson, Bo Peng, Ron Shepard, Edward F. Valeev, Mark van Schilfgaarde, Bess Vlaisavljevich, Theresa L. Windus, Sotiris S. Xantheas, Xing Zhang, Paul M. Zimmerman
Summary: The sustainability and interoperability of computational chemistry software development are pressing issues. A flexible forward strategy is needed to take full advantage of existing and forthcoming computational resources and provide unique computational tools for next-generation science problems and scientific discoveries.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Multidisciplinary
Victor M. Freixas, Jeïreïmy R. Rouxel, Yeonsig Nam, Sergei Tretiak, Niranjan Govind, Shaul Mukamel
Summary: Chirality is a fundamental property of molecules that has significant implications in biophysics and drug design. Optical circular dichroism (OCD) and X-ray circular dichroism (XCD) are two important spectroscopic probes that can detect global and local molecular chirality, respectively.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Hasan Razouq, Thomas Berger, Nicola Huesing, Oliver Diwald
Summary: The spatial arrangement of metal oxide nanoparticles plays a crucial role in their chemical utilization. In this study, we successfully created metal oxide nanoparticle-based networks by dispersing vapor phase-grown TiO2 and ZnO nanoparticles in an aqueous polyvinyl alcohol solution. Electrospinning and subsequent calcination resulted in self-supported nanoparticle-based nanofibers, with particle coarsening observed for both TiO2 and ZnO nanoparticles.
MONATSHEFTE FUR CHEMIE
(2023)
Article
Chemistry, Multidisciplinary
Guangdong Liu, Yang He, Zhixiao Liu, Hui Wan, Yaobin Xu, Huiqiu Deng, Hui Yang, Ji-Guang Zhang, Peter V. V. Sushko, Fei Gao, Chongmin Wang, Yingge Du
Summary: By using in situ transmission electron microscopy and density functional theory calculations, the influence of planar defects on the diffusion pathways and transport kinetics of Li ions in a tungsten trioxide lattice is revealed. It is found that planar defects disrupt the continuity of ion conduction channels by altering the charge distribution and lattice spacing, leading to a significant increase in energy barrier for Li diffusion. This atomic-level understanding has important implications for rational interface design in solid-state batteries and solid oxide fuel cells.
Article
Materials Science, Multidisciplinary
Matthew Chrysler, Judith Gabel, Tien-Lin Lee, Zihua Zhu, Tiffany C. Kaspar, Mark Bowden, Peter V. Sushko, Scott A. Chambers, Joseph H. Ngai
Summary: Charge redistribution across heterojunctions influences the functionality of materials systems. The composition of the terminating surface affects charge transfer across a Si/SrTiO3 heterojunction. Surface depletion in Si causes itinerant electrons to migrate across the interface and modify the interfacial dipole. This leads to a change in band alignment, which can be weakened by capping the SrTiO3 surface.
PHYSICAL REVIEW MATERIALS
(2023)
Article
Nanoscience & Nanotechnology
Hasan Razouq, Kerstin Neuhauser, Gregor Zickler, Thomas Berger, Oliver Diwald
Summary: Transformations of nanoparticle-based ferroelectric components in aqueous environments raise stability issues that are important for various applications. This study investigates the dissolution and crystallization behavior of BaTiO3 nanoparticles in water and shows that the nanoparticles undergo incongruent Ba2+ dissolution, resulting in the formation of crystalline BaCO3 needles. The size, crystallinity, surface contaminants, and surface passivation with polymers are found to play critical roles in the stability of these nanoparticle-based composites.
ACS APPLIED NANO MATERIALS
(2023)
Article
Multidisciplinary Sciences
Prescott E. Evans, Yang Wang, Peter V. Sushko, Zdenek Dohnalek
Summary: This study investigates the deposition of palladium (Pd) on WTe2(001) and finds that Pd nucleation is driven by the interaction with excess tellurium (Te) atoms. The formation of Pd-Te clusters is not affected by surface defects and remains stable at elevated temperatures. These findings are important for the manufacturing of novel quantum and microelectronics devices and catalytically active nano-alloy centers.
