Article
Physics, Multidisciplinary
William J. Huggins, Kianna Wan, Jarrod McClean, Thomas E. O. ' Brien, Nathan Wiebe, Ryan Babbush
Summary: This Letter addresses the task of estimating the expectation values of multiple observables in quantum algorithms. The authors propose an approach that utilizes a quantum gradient estimation algorithm to achieve efficient estimation. They demonstrate that this approach provides optimal scaling in the high-precision regime and showcases its flexibility.
PHYSICAL REVIEW LETTERS
(2022)
Article
Materials Science, Multidisciplinary
Alexander B. Shick, Shin-ichi Fujimori, Warren E. Pickett
Summary: Correlated band theory based on density functional theory with exact diagonalization was applied to UTe2, revealing its physical properties at different U values, including a transition to a semimetallic state at U = 3 eV. Predictions were made for the Kondo temperature of UTe2 and the electric field gradient difference between uranium and tellurium sites, consistent with experimental observations.
Article
Multidisciplinary Sciences
Alexander Muller, Gauthier J-P Deblonde, Peter Ercius, Steven E. Zeltmann, Rebecca J. Abergel, Andrew M. Minor
Summary: In this work, the authors utilize transmission electron microscopy to characterize highly-radioactive compounds of berkelium and californium, requiring only small amounts of the elements. They find that berkelium exhibits unexpectedly weak spin-orbit coupling, while californium follows a jj coupling scheme.
NATURE COMMUNICATIONS
(2021)
Article
Physics, Applied
Ling Chen, Shanshan Sheng, Bowen Sheng, Tao Wang, Liuyun Yang, Baoqing Zhang, Jiajia Yang, Xiantong Zheng, Zhaoying Chen, Ping Wang, Weikun Ge, Bo Shen, Xinqiang Wang
Summary: We demonstrate a high electron mobility of similar to 4850 cm(2) V(-1)s(-1) in nearly-dislocation-free hexagonal InN at room temperature using Hall-effect measurement. These high-quality InN crystals were achieved through droplet-assisted epitaxy on a GaN/sapphire template by molecular beam epitaxy. The achievement of such high-mobility InN opens up promising opportunities for the fabrication of high-speed electronic devices.
APPLIED PHYSICS EXPRESS
(2022)
Article
Chemistry, Physical
Subhasish Mandal, Kristjan Haule, Karin M. Rabe, David Vanderbilt
Summary: Systematic investigation using first principles calculations reveals that the computed bandwidths of nearly free-electron metals can be well described by the local approximation to the self-energy, providing a good agreement with angle-resolved photoemission experiments.
NPJ COMPUTATIONAL MATERIALS
(2022)
Article
Physics, Multidisciplinary
S. Sasikumar, Huiqing Fan, Weijia Wang, T. K. Thirumalaisamy, S. Saravanakumar, P. Diana, D. Sivaganesh
Summary: A series of novel lead-free ceramics were fabricated and studied for their dielectric and microstructural properties. With increasing BSN content, the average grain size decreased and dielectric anomalous behavior became more pronounced.
Article
Materials Science, Multidisciplinary
D. Potorochin, R. Kurleto, O. J. Clark, E. D. L. Rienks, J. Sanchez-Barriga, F. Roth, V. Voroshnin, A. Fedorov, W. Eberhardt, B. Buechner, J. Fink
Summary: This study presents a high-resolution angle-resolved photoemission (ARPES) investigation of the nearly free-electron metal sodium, revealing a slightly smaller mass enhancement compared to previous studies. The observed lifetime broadening highlights the need for theories beyond the random phase approximation. Contrary to the proposed strong enhancement of scattering rates due to coupling to spin fluctuations, our results do not support this hypothesis. Additionally, comparison with earlier electron energy-loss data suggests a significant reduction in the mass enhancement of dipolar electron-hole excitations compared to monopole hole excitations, as measured by ARPES.
Article
Chemistry, Multidisciplinary
Xiaoran Shi, Hongsheng Liu, Ziyu Hu, Jijun Zhao, Junfeng Gao
Summary: In the search for high mechanical strength and flexibility, ultrahigh semiconducting speed is crucial for the next generation of microelectronic and wearable electronics. Two 2D graphene-like macrocyclic complex carbon-based monolayers, g-MC-A and g-MC-B, with high mechanical strength and semiconducting properties, are proposed. These monolayers also exhibit excellent inherent conductivity and anisotropic characteristics. Moreover, simulation predicts that these metal-free monolayers will have high thermoelectric performance. Therefore, these C-based metal-free layers have promising applications in mechanical enhancement, microelectronics, wearable electronics, and thermoelectric devices.
Article
Chemistry, Multidisciplinary
Maria Grazia Betti, Ernesto Placidi, Chiara Izzo, Elena Blundo, Antonio Polimeni, Marco Sbroscia, Jose Avila, Pavel Dudin, Kailong Hu, Yoshikazu Ito, Deborah Prezzi, Miki Bonacci, Elisa Molinari, Carlo Mariani
Summary: By exposing fully free-standing nanoporous samples of graphene to atomic hydrogen in ultrahigh vacuum, the researchers achieved an unprecedented level of hydrogenation, converting conductive graphene into a wide gap semiconductor. The experimental results confirmed the theoretical predictions of a stable, double-sided fully hydrogenated configuration without pi states.
Article
Nanoscience & Nanotechnology
Mahmoud Mohamed Saad Abdelnabi, Elena Blundo, Maria Grazia Betti, Gianluca Cavoto, Ernesto Placidi, Antonio Polimeni, Alessandro Ruocco, Kailong Hu, Yoshikazu Ito, Carlo Mariani
Summary: Graphane is formed by bonding hydrogen (and deuterium) atoms to carbon atoms in the graphene mesh, with modification from the pure planar sp(2) bonding towards an sp(3) configuration. The non-destructive H- (and D-) NPG chemisorption is very stable at high temperatures up to about 800 K, with complete healing and restoring of clean graphene above 920 K, opening up possibilities for advanced detectors and semiconducting graphane.
Article
Chemistry, Physical
Lei Wang, Jia Hang, Qinqin Yuan, Wenjin Cao, Xiaoguo Zhou, Shilin Liu, Xue-Bin Wang
Summary: In this study, the electron affinity and electronic structure of hexafluoroacetone (HFA) were investigated using negative ion photoelectron (NIPE) spectroscopy and quantum chemistry calculations. The results showed a singlet ground state with a large singlet-triplet energy difference, providing important insights into the physicochemical properties of HFA. The determined electron affinity and singlet-triplet energy difference of HFA were found to be EA=1.42+/-0.02 eV and Delta E-S(T)=-3.01 eV, respectively.
JOURNAL OF PHYSICAL CHEMISTRY A
(2021)
Article
Quantum Science & Technology
Matthew Thibodeau, Bryan K. Clark
Summary: Solving for quantum ground states is crucial for understanding quantum many-body systems, and quantum computers are well-suited for this task. Recent research has proposed an optimal scheme for preparing ground states on a quantum computer for generic Hamiltonians, whose query complexity scales inversely with their normalized gap. This study focuses on the ground state preparation problem for a special subset of Hamiltonians called nearly-frustration-free. An algorithm with better dependence on the gap is presented, scaling inversely as the gap to the power of y/2-1, which is optimal up to logarithmic factors. Examples of physically motivated Hamiltonians in this subclass are provided, and an extension of the method for excited states is described.
Article
Chemistry, Physical
Huijuan Wang, Xiaole Zheng, Xinxin Li, Linxin He, Jiasen Guo, Ying Chen, Hua Lin, Jianfeng Tang, Chunmei Li
Summary: Photocatalytic water splitting is a promising solution to the energy crisis and environmental problems. Graphene's practical application is limited due to its zero gap, while graphane shows potential with a wider band gap. In this work, the electronic structure of graphane is modulated through structural modifications and heterojunctions, enhancing its photocatalytic efficiency.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Roberto Costantini, Alessio Giampietri, Dario Marchiani, Maria Grazia Betti, Samuel Jeong, Yoshikazu Ito, Alberto Morgante, Martina Dell'Angela, Carlo Mariani
Summary: The effects of optical excitation on fully hydrogenated free-standing nanoporous graphene have been studied, showing partial dehydrogenation of graphane and providing an estimation of its thermal conductivity. Furthermore, the dynamics of the C 1s core level under optical excitation display distinctive features.
APPLIED SURFACE SCIENCE
(2024)
Article
Chemistry, Inorganic & Nuclear
Weiqi Huang, Xiaolong Wu, Belal Ahmed, Yanqiang Li, Yang Zhou, Han Wang, Yipeng Song, Xiaojun Kuang, Junhua Luo, Sangen Zhao
Summary: We report a novel lead-free hybrid pseudo-perovskite layered structure of MLASnCl(4) with large birefringence. The observed birefringence is generated from the delocalized pi-conjugations of melamine cations and stereochemically active lone pair electrons on the Sn2+ cations of highly distorted SnCl4 tetrahedra.
INORGANIC CHEMISTRY FRONTIERS
(2023)
Review
Physics, Atomic, Molecular & Chemical
Xiongzhi Zeng, Wei Hu, Xiao Zheng, Jin Zhao, Zhenyu Li, Jinlong Yang
Summary: Computational simulation plays a crucial role in accurately characterizing the structure and properties of nanosystems. Various methods, such as electronic structure calculations, scanning tunneling microscopy image simulation, hierarchical equation solving, and excited state dynamics simulation, have been developed to provide electronic structure information and experimentally comparable data. Additionally, multiscale simulation methods are essential for characterizing the atomic details of nanosystems involved in chemical processes.
CHINESE JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Lanlan Chen, Yanan Zhou, Yifei Rao, Mingxin Qin, Bingbing Gong, Wenhua Zhang, Zhenyu Li
Summary: Fe atom-decorated MoS2 has been found to be a stable and noble-metal-free catalyst for nitrogen reduction reaction (NRR) at ambient conditions. The synergetic effect between a single Fe atom and the directly bonded oxygen atoms in the Mo-edge of MoS2 is responsible for the high-performance of NRR, and moderate charge transfer between Fe and the support greatly promotes the NRR activity and selectivity.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Yan Xu, Jiale Ma, Taoli Jiang, Honghe Ding, Weiping Wang, Mingming Wang, Xinhua Zheng, Jifei Sun, Yuan Yuan, Mingyan Chuai, Na Chen, Zhenyu Li, Hanlin Hu, Wei Chen
Summary: Tuning the solvation structures of Al3+ cations in concentrated aqueous electrolytes can prevent their intercalation into the MnO2 cathode, ensuring high reversibility and improving the performance of MnO2 cathode in aqueous batteries. This approach opens up new possibilities for the development of highly reversible MnO2 cathodes in multivalent metal/MnO2 batteries.
ENERGY STORAGE MATERIALS
(2022)
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
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
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)
