Article
Chemistry, Multidisciplinary
Pradeep Tanwar, Uttam Paliwal, K. B. Joshi, Jitendra Kumar
Summary: This paper investigates the structural, electronic, and vibrational properties of 3D bulk and 2D layer of TiS2 using density functional theory and van der Waals interaction. The calculated results agree well with experimental data. Both bulk and monolayer TiS2 are found to be semimetals with a small overlapping of bands near Fermi level. The band overlapping increases in bulk TiS2 under pressure, and the magnitude of phonon vibration frequencies also increases with pressure. The monolayer TiS2 becomes a metal under negative strain and opens an indirect bandgap under positive strain.
JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
(2023)
Article
Chemistry, Physical
Matthew Lawson, Elton Graugnard, Lan Li
Summary: This study utilized density functional theory to investigate the nucleation of MoF6 on various oxide surfaces, revealing that hydroxyl groups play a role in reducing the reaction barrier and promoting precursor chemisorption. The formation of highly ionic MFx bonds at oxide surfaces further supports this discovery, emphasizing the importance of surface chemistry in the process.
APPLIED SURFACE SCIENCE
(2021)
Article
Physics, Multidisciplinary
Hiroki Katow, Ryosuke Akashi, Yoshiyuki Miyamoto, Shinji Tsuneyuki
Summary: This letter proposes a technique of forming an optical dipole trap for excitons in graphane based on first-principles calculations. The huge exciton binding energy and large dipole moments in graphane enable the formation of a dipole trap with meV depth and nm width. This study opens a new way to control light-exciton interacting systems using numerically robust ab initio calculations.
PHYSICAL REVIEW LETTERS
(2022)
Article
Chemistry, Physical
Tahir Wahab, Yun Wang, Antonio Cammarata
Summary: In this study, the structural, opto-electronic, and photocatalytic properties of GeC-MX2 (M = Mo, W, X = S, Se) van der Waals heterostructures for photocatalysis were systematically investigated using first-principles computations. The results showed that the GeC-MX2 heterostructures could absorb visible light and allow for continuous separation of photogenerated electron-hole pairs. The induced electric field at the interface between the GeC and MX2 monolayers was essential for preventing the recombination of photogenerated charges. Additionally, the band-edge locations suggested that GeC-MX2 heterostructures could be utilized as a photocatalyst for water splitting. Overall, the opto-electronic properties of these novel GeC-MX2 heterostructures made them suitable for future photocatalysis applications.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
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
Chunyu Zhao, Dashuai Wang, Ruqian Lian, Dongxiao Kan, Yaying Dou, Chunzhong Wang, Gang Chen, Yingjin Wei
Summary: Through first-principles calculations based on density functional theory, it was found that monolayer TiSe2 and bulk TiSe2 exhibit distinct Li+ storage mechanisms and both undergo a two-stage redox process. Monolayer TiSe2 has higher theoretical capacity and lower Li+ diffusion barriers, indicating great potential as a high rate anode material for lithium-ion batteries.
APPLIED SURFACE SCIENCE
(2021)
Article
Nanoscience & Nanotechnology
Razieh Beiranvand
Summary: The MoX2 monolayers exhibit high absorption coefficients and broad absorption spectrum, making them promising materials for solar cells and optoelectronic applications. The wide band gap of TMDs, which is thickness dependent, also makes them potential candidates for optoelectronic devices.
PHYSICA E-LOW-DIMENSIONAL SYSTEMS & NANOSTRUCTURES
(2021)
Article
Chemistry, Multidisciplinary
Tran P. T. Linh, Nguyen N. Hieu, Huynh Phuc, Cuong Q. Nguyen, Pham T. Vinh, Nguyen Q. Thai, Nguyen Hieu
Summary: The study systematically examines the structural, mechanical, electronic, and optical properties of two-dimensional Janus CrXO monolayers, revealing their good stability, broad absorption spectrum, and varied behaviors in metallicity and semiconductor characteristics. The findings provide insight into these new materials and suggest potential applications in optoelectronic and nanoelectromechanical devices, encouraging further experimental research.
Article
Physics, Applied
Yong Li, Hengtao Li, Yuxian Wu, Xiang Kan, Yong Zhao, Yongliang Chen
Summary: Due to the spin-orbital coupling effects, we have discovered a series of novel structures in the Os-S system and predicted a potential superconductivity of I-4m2 phase at 3.6 K and 0 GPa. The superconductivity is associated with the soft phonon modes of Os. However, there is no superconducting transition temperature in the I-4m2 phase when the pressure reaches 50 GPa.
APPLIED PHYSICS EXPRESS
(2022)
Article
Nanoscience & Nanotechnology
Jinhan Shen, Dan Han, Bowen Zhang, Rongxing Cao, Yang Liu, Shu Zheng, Hongxia Li, Yuqi Jiang, Yuxiong Xue, Mengyun Xue
Summary: In this paper, the thermal transport properties of MoTe2 and WTe2 monolayers with different phases were investigated, showing different lattice thermal conductivities and phonon thermal transport characteristics. The findings suggest the potential applications of these monolayers in two-dimensional nanoelectronic devices.
PHYSICA E-LOW-DIMENSIONAL SYSTEMS & NANOSTRUCTURES
(2023)
Article
Chemistry, Multidisciplinary
Yongji Wang, Wei Zhai, Yi Ren, Qinghua Zhang, Yao Yao, Siyuan Li, Qi Yang, Xichen Zhou, Zijian Li, Banlan Chi, Jinzhe Liang, Zhen He, Lin Gu, Hua Zhang
Summary: 2D heterostructures are promising alternatives to conventional semiconductors. A facile method of chemical vapor deposition is reported to prepare vertical 1H/1T' MoS2 heterophase structures, which exhibit excellent rectification and photodetection properties.
ADVANCED MATERIALS
(2023)
Article
Materials Science, Multidisciplinary
Tran Yen Mi, Nguyen Duy Khanh, Rajeev Ahuja, Nguyen Thanh Tien
Summary: By using first-principles calculations, the study systematically investigated the structural and electronic properties of the buckled SiC2 pentagon-based nanoribbons. It was found that the SS-ribbon achieved the greatest thermal and dynamic stability, while the energy gaps were primarily influenced by competition in edge structures, finite size confinements, and asymmetry of chemical bonds.
MATERIALS TODAY COMMUNICATIONS
(2021)
Article
Chemistry, Multidisciplinary
Jeffrey D. Cain, Sehoon Oh, Amin Azizi, Scott Stonemeyer, Mehmet Dogan, Markus Thiel, Peter Ercius, Marvin L. Cohen, Alex Zettl
Summary: The study presents a vapor-phase synthesis method for ultranarrow TaS2 nanoribbons, achieving widths down to the nanoscale. By using carbon nanotubes as templates, the width and layer number of the nanoribbons can be controlled while maintaining stability, offering a new approach for the growth of ultranarrow TMD nanoribbons.
Article
Multidisciplinary Sciences
Nelson Naveas, Ruth Pulido, Carlo Marini, Jacobo Hernandez-Montelongo, Miguel Manso Silvan
Summary: Due to limitations in Fe-3d orbitals and self-interaction error of exchange-correlation functionals, approximate DFT fails to accurately describe the electronic structure and magnetic properties of iron oxides. Hybrid DFT or DFT + U can solve these problems, but are expensive or only consider on-site interactions. In this study, we used DFT + U + V, an extension that includes intersite interactions, to simulate the properties of alpha-Fe2O3. We found that DFT + U + V improves the description of structural, magnetic, and electronic properties compared to approximate DFT, with the accuracy depending on the type of atomic orbital projectors used.
Article
Materials Science, Multidisciplinary
Jie Yin, Yunhui Wang, Lan Bi, Shanling Ren, Gang Yan, Xin Huang, Zhihong Yang
Summary: The study focused on the structural stability, electronic, and magnetic properties of zigzag boron nitride nanoribbons (ZBNNRs) with single vacancy defects and doped with ten 3d transition metal (TM) species. It was found that vacancy defects significantly decreased the structural stability of ZBNNRs, with N-site defects being more stable than B-site defects. Among the ten different TM ions, Sc-, Ti-, and V-doping improved structural stability, while Cr-, Mn-, Fe-, Co-, Ni-, Cu-, and Zn-doping led to instability in ZBNNRs compared to pristine ones. The substitutional doping with 3d TM atoms exhibited a magnetic effect in non-magnetic ZBNNRs.
MATERIALS TODAY COMMUNICATIONS
(2021)
Article
Chemistry, Medicinal
Yufeng Liu, Zhenyu Li
Summary: Ionization energy is an important property of molecules, and it can be efficiently predicted using machine learning models. This study compares the performance of different machine learning models in predicting ionization energy for molecules with distinct functional groups. Support vector regression is the best conventional model, while AttentiveFP performs even better in graph-based models. These results provide high-performance models for ionization energy prediction and valuable guidance in choosing reliable QSPR models.
JOURNAL OF CHEMICAL INFORMATION AND MODELING
(2023)
Article
Chemistry, Physical
Xinbo Ma, Wenjun Chu, Youxi Wang, Zhenyu Li, Jinlong Yang
Summary: Photocatalytic water splitting is a potential way to utilize solar energy. In this study, a new photocatalytic water splitting model based on intermediate bands (IBs) is proposed, which significantly increases the solar-to-hydrogen efficiency compared to conventional single-band gap systems. First-principles calculations reveal that N-doped TiO2, Bi-doped TiO2, and P-doped ZnO have suitable IBs, with corresponding STH efficiency limits of 10.0%, 12.0%, and 19.0% respectively. This study opens a new avenue for the design of photocatalytic water splitting systems.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Zhenjie Liu, Jiale Ma, Xiangjian Liu, Haiyang Wu, Dianlun Wu, Bin Chen, Peng Huang, Yang Huang, Lei Wang, Zhenyu Li, Shulei Chou
Summary: In this study, a dimethyl sulfoxide (DMSO)-H2O hybrid electrolyte containing polyacrylonitrile (PAN) additives (PAN-DMSO-H2O) was proposed to improve the electrical field and ion transport of the Zn anode, effectively inhibiting dendrite growth. PAN preferentially adsorbs on the Zn anode surface and provides abundant zincophilic sites, enabling a balanced electric field and lateral Zn plating. DMSO regulates the solvation structure of Zn2+ ions and enhances ion transport, leading to a dendrite-free Zn anode surface during plating/stripping. Zn-Zn symmetric and Zn-NaV3O8 center dot 1.5H(2)O full batteries with this PAN-DMSO-H2O electrolyte exhibit enhanced coulombic efficiency and cycling stability.
Article
Chemistry, Multidisciplinary
P. Prabhu, Viet-Hung Do, Chun Kuo Peng, Huimin Hu, San-Yuan Chen, Jin-Ho Choi, Yan-Gu Lin, Jong-Min Lee
Summary: Here, we report a high-performance electrocatalyst, atomically thin rhodium metallene incorporated with oxygen-bridged single atomic tungsten (Rh-O-W), for pH-universal hydrogen evolution reaction. The Rh-O-W metallene exhibits remarkable electrocatalytic HER performance in pH-universal electrolytes, with low overpotentials, high mass activities, excellent turnover frequencies, and stability, outperforming benchmark catalysts such as Pt/C, Rh/C, and other precious-metal HER catalysts. The promoting effect of -O-W single atomic sites is understood through characterization and calculations, which show fine-tuning of density of states and electron localization at Rh active sites, leading to near-optimal hydrogen adsorption for HER.
Article
Chemistry, Multidisciplinary
Wei Li, Cong Liu, Chenkai Gu, Jin-Ho Choi, Song Wang, Jun Jiang
Summary: In this study, single-atom catalysis on two-dimensional graphene and electride heterostructures was investigated using first-principles calculations. The electron gas in the electride layer facilitated a significant transfer of electrons to the graphene layer, which could be controlled by the choice of electride. The charge transfer effectively modified the d-orbital electron occupancy of a single metal atom, leading to enhanced catalytic activity for hydrogen evolution and oxygen reduction reactions. The strong correlation between adsorption energy and charge transfer suggested that interfacial charge transfer is a crucial catalytic descriptor for heterostructure-based catalysts. The polynomial regression model demonstrated the importance of charge transfer and accurately predicted the adsorption energy of ions and molecules. This study offers a strategy for obtaining high-efficiency single-atom catalysts using two-dimensional heterostructures.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Multidisciplinary Sciences
Zhenqi Gu, Jiale Ma, Feng Zhu, Ting Liu, Kai Wang, Ce-Wen Nan, Zhenyu Li, Cheng Ma
Summary: In this study, the role of space-charge layers in Li0.33La0.56TiO3, a solid electrolyte, was investigated through experimental and computational methods. Contrary to previous assumptions, it was found that the actual space-charge layers are Li-excess instead of Li-deficient. The efficient ion transport in these Li-excess layers excluded them as potential bottlenecks, identifying Li-depleted grain-boundary cores as the major cause of the large resistance.
NATURE COMMUNICATIONS
(2023)
Article
Materials Science, Multidisciplinary
Huimin Hu, Jin-Ho Choi
Summary: In this study, we investigate the catalytic properties of single-atom doped graphene as electrocatalysts for hydrogen evolution reactions (HERs) using first-principles calculations. The findings show that all the considered doped graphene, except for As-doped graphene, can be highly active for HER, with hydrogen adsorption free energies (Delta G (H*)) close to the optimal value (Delta G (H*) = 0), ranging from -0.19 to 0.11 eV.
Article
Quantum Science & Technology
Honghui Shang, Yi Fan, Li Shen, Chu Guo, Jie Liu, Xiaohui Duan, Fang Li, Zhenyu Li
Summary: Quantum computing is advancing towards commercial applications in chemical and biomedical sciences, but the lack of quantum resources in the current noisy intermediate-scale era hinders these explorations. Emulating quantum computing on classical computers is valuable for developing quantum algorithms and validating quantum hardware, yet existing simulators often face memory limitations, making large-scale quantum chemistry calculations challenging.
NPJ QUANTUM INFORMATION
(2023)
Article
Chemistry, Physical
Juntao Lai, Yi Fan, Qiang Fu, Zhenyu Li, Jinlong Yang
Summary: In this work, analytical calculations of atomic forces based on the Hellmann-Feynman theorem within the framework of the variational quantum eigensolver were achieved. The accuracy of the approach is demonstrated by comparing the calculated atomic forces with values obtained from full configuration interaction calculations. The results show that the analytical approach has a significant accuracy advantage and is feasible for practical quantum chemistry simulations.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Yi Fan, Jie Liu, Zhenyu Li, Jinlong Yang
Summary: As shown in the DMRG method, approximating many-body wave function of electrons using a matrix product state (MPS) is a promising approach for solving electronic structure problems. The expressibility of an MPS is determined by the bond dimension, which can be very large in quantum chemistry simulations. In this study, the ground state energies of molecular systems are calculated using a variational optimization of the quantum circuit MPS (QCMPS) method with a relatively small number of qubits. Results show that QCMPS can achieve similar accuracy as DMRG with a large bond dimension by carefully choosing circuit structure and orbital localization scheme. QCMPS simulation of a linear hydrogen molecular chain with 50 orbitals reaches chemical accuracy using only 6 qubits at a moderate circuit depth. These findings suggest that QCMPS is a promising wave function ansatz in the variational quantum eigensolver algorithm for molecular systems.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Physical
Shirui Weng, Wenjun Chu, Huaze Zhu, Junxiang Li, Ronglu Dong, Rui Niu, Jun Yang, Changjin Zhang, Zhenyu Li, Liangbao Yang
Summary: In this study, a new approach based on the coupling effect of neighboring electron orbitals is proposed to elucidate the electromagnetic field enhancement mechanism of single-atom-layer Au clusters embedded in 2H-TaS2 for SERS sensing. Experimental results confirmed the insertion of Au atoms into the 2H-TaS2 interlayer, leading to a 2 orders of magnitude enhancement in SERS signal compared to pure 2H-TaS2. XPS and micro-UV/vis-NIR spectra revealed the overlap and migration of outer electrons between neighboring Au and 2H-TaS2. First-principles calculations demonstrated strong electronic coupling between Au and 2H-TaS2. This study provides valuable insights into SERS enhancement in nonprecious metal compounds and offers guidance for the development of new SERS substrates.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Yi Fan, Changsu Cao, Xusheng Xu, Zhenyu Li, Dingshun Lv, Man-Hong Yung
Summary: This work proposes a strategy to reduce the circuit depth of quantum algorithms for large chemical systems by employing an energy-sorting strategy. By prescreening subsets of excitation operators based on their contribution to the total energy, the method effectively reduces the number of operators while maintaining the accuracy.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Multidisciplinary Sciences
Lv Hu, Jinzhu Wang, Kai Wang, Zhenqi Gu, Zhiwei Xi, Hui Li, Fang Chen, Youxi Wang, Zhenyu Li, Cheng Ma
Summary: To enable the development of all-solid-state batteries, an inorganic solid-state electrolyte with high ionic conductivity (>1 mS cm(-1) at 25℃), compressibility (>90% density under 250-350 MPa), and cost-effectiveness (<$50/kg) is required. Here, the authors report the development and preparation of Li1.75ZrCl4.75O0.5 oxychloride solid-state electrolyte that meets these requirements, with an ionic conductivity of 2.42 mS cm(-1) at 25℃, a compressibility enabling 94.2% density under 300 MPa, and an estimated raw material cost of $11.60/kg.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Huan Ma, Jie Liu, Honghui Shang, Yi Fan, Zhenyu Li, Jinlong Yang
Summary: Exploration of potential applications of quantum computers in material design and drug discovery has gained significant attention. However, the current resource requirements for quantum simulations in these areas exceed the capabilities of near-term quantum devices. This study proposes a multiscale quantum computing approach that integrates multiple computational methods at different resolution scales to simulate complex systems. By efficiently implementing most methods on classical computers and leaving critical computations to quantum computers, the simulation scale of quantum computing can be expanded. The proposed algorithm has demonstrated decent accuracy in simulating systems with hundreds of orbitals on classical simulators. This work should encourage further research on quantum computing for practical material and biochemistry problems.
Article
Chemistry, Physical
Wenjun Chu, Xinbo Ma, Zhenyu Li
Summary: In this study, the intrinsic defect properties of Cs2AgPdBr5 are investigated from first principles. It is found that Cs2AgPdBr5 has a small thermodynamic stable region, requiring careful control of growth conditions. P-type Cs2AgPdBr5 can be obtained under Ag-poor conditions, while Pd-i(2+) and Pd-Ag(1+) are the only two deep-level recombination centers.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)