Article
Multidisciplinary Sciences
Liguo Ma, Phuong X. Nguyen, Zefang Wang, Yongxin Zeng, Kenji Watanabe, Takashi Taniguchi, Allan H. MacDonald, Kin Fai Mak, Jie Shan
Summary: This study demonstrates a strongly correlated two-dimensional excitonic insulator ground state in transition metal dichalcogenide semiconductor double layers, providing direct thermodynamic evidence for the state. Capacitance measurements show that the exciton fluid is compressible but charge-incompressible. An exciton phase diagram reveals both the Mott transition and interaction-stabilized quasi-condensation.
Article
Materials Science, Multidisciplinary
Itsuki Takahashi, Yuya Tanizaki
Summary: Using field-theoretic techniques, the study explores the SU(3) analog of antiferromagnetic Heisenberg spin model on the triangular lattice, revealing a low-energy effective theory with magnetic skyrmions and monopole instantons. The analysis of the Berry phase and Wess-Zumino term leads to insights on the valence-bond-solid phase and restrictions on perturbations by monopole operators. Furthermore, 't Hooft anomalies are computed to constrain possible phases, supporting a direct phase transition between Neel and VBS phases.
Article
Materials Science, Multidisciplinary
Antonio Picano, Jiajun Li, Martin Eckstein
Summary: Research focuses on the use of quantum Boltzmann equation to explain collective orders and photoinduced phase transitions in quantum matter. By utilizing a nonperturbative scattering integral, consideration of the separation of timescales is possible without assumptions on spectral function.
Article
Biochemistry & Molecular Biology
Peikun Zheng, Chenru Ji, Fuming Ying, Peifeng Su, Wei Wu
Summary: The paper revisits lambda-DFVB method and introduces lambda-DFVB(IS) scheme, which simplifies the calculation process by using NOONs as a function of parameter lambda. Lambda-DFVB(IS) demonstrates higher computational efficiency and robustness compared to lambda-DFVB(K), while maintaining accuracy comparable to high-level multireference wave function methods like CASPT2.
Article
Chemistry, Physical
Paul Andrew Johnson, A. Eugene DePrince III
Summary: The Richardson-Gaudin (RG) states are used as a variational wave function ansatz to describe strongly correlated isomers of H-4 and H-10. It is found that a single RG state can effectively describe the seniority-zero sector, while a configuration interaction in terms of RG states improves the model systematically.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Multidisciplinary
Slavko Radenkovic, Sason S. Shaik, Benoit Braida
Summary: The study investigates the bonding in the recently synthesized NaBH3- cluster using the high level Valence Bond BOVB method, revealing a split and polarized weakly coupled electron-pair mechanism for stabilization. The Na-B bond is not a standard polar-covalent bond, but rather a combination of (major) dipole-dipole electrostatic interaction and (secondary) resonant one-electron bonding mechanism. This analysis extends to similar clusters and unifies the previously published views on this exotic bond.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Daria Drwal, Pavel Beran, Micha Hapka, Marcin Modrzejewski, Adam Sokol, Libor Veis, Katarzyna Pernal
Summary: In this work, a new approach based on adiabatic connection is proposed to accurately describe the electronic structure, especially for systems with strong electron correlation. It is more efficient than existing ab initio multireference dynamic correlation methods.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Jerzy Cioslowski, Berthold-Georg Englert, Martin-Isbjoern Trappe, Jun Hao Hue
Summary: At the limit of infinite confinement strength, the ground state of a system containing two interacting fermions or bosons in harmonic confinement remains strongly correlated. The natural orbitals of this system exhibit peculiar properties, such as nonzero collective occupancies for all angular momenta and a relationship with eigenfunctions and eigenvalues of a zero-energy Schrodinger equation with an attractive Gaussian potential. These properties have implications for the decay behavior and energy contributions of the system.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Biochemistry & Molecular Biology
Sudip Pan, Gernot Frenking
Summary: Pauling's influence on the understanding of chemical bonding was significant, as he connected quantum theoretical description with Gilbert Lewis's classical bonding model. His introduction of the concept of resonance provided a consistent description for molecules, metals, and ionic crystals. However, his one-sided restriction to the valence bond method and rejection of the molecular orbital approach hindered further development of chemical bonding theory.
Article
Physics, Multidisciplinary
Jiayu Hu, Xuefeng Zhang, Cong Hu, Jian Sun, Xiaoqun Wang, Hai-Qing Lin, Gang Li
Summary: By analyzing and calculating, we discovered that monolayer Nb3Cl8 is a unique flat band system with short-range interactions. We proposed that it may be a molecular quantum spin liquid, providing a platform to explore its relation with other materials.
COMMUNICATIONS PHYSICS
(2023)
Article
Chemistry, Physical
Bei-Lei Liu, Yue-Chao Wang, Yu Liu, Hai-Feng Liu, Hai-Feng Song
Summary: We have developed a doubly screened Coulomb correction (DSCC) method for efficiently correcting the on-site Coulomb interaction in strongly correlated materials, and it can accurately simulate electronic and magnetic properties. Compared to hybrid functionals, DSCC has comparable accuracy but is an order of magnitude faster, and it can reflect the difference in the Coulomb interaction between metallic and insulating situations.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Koji Ando
Summary: Potential energy surfaces (ePES) for electron dynamics were constructed using a model of localized electron wave packets (eWP) with non-orthogonal valence-bond (VB) spin coupling. These ePES were then used to simulate quantum dynamics of high harmonic generation (HHG) spectra in hydrogen and helium atoms induced by intense laser pulses. The time-dependent Schrodinger equation was numerically solved to calculate the dynamics of the single electron on the ePES, and the results showed reasonable agreement with previous studies. Analysis of the electron wave function, dipole moment, and dipole acceleration revealed that the main part of the wave function remained near the nuclear position, while the smaller part that escaped the laser-induced potential barrier through quantum tunneling contributed significantly to HHG.
Article
Chemistry, Physical
Haodong Zhang, Jingxiang Zou, Xiaochuan Ren, Shuhua Li
Summary: The Anequation-of-motion block-correlated coupled cluster method based on the generalized valence bond wave function (EOM-GVB-BCCC) is proposed to describe low-lying excited states for strongly correlated systems. The EOM-GVB-BCCC2b method, which includes up to two-pair correlation, has been successfully implemented and tested for several strongly correlated systems. The results of EOM-GVB-BCCC2b for a water hexamer and four conjugated diradical species are consistent with the density matrix renormalization group (DMRG) results.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Materials Science, Multidisciplinary
Youngjae Kim
Summary: We used time-resolved transient absorption spectroscopy to investigate the ultrafast optical responses of condensed matter systems. We observed unconventional absorption spectra in Mott insulators that do not fully reflect the dynamical Franz-Keldysh effect, unlike in band insulators. These unconventional spectra, characterized by a negative difference absorption and a blueshift, are purely driven by electron correlations, as revealed by decomposed calculation.
Article
Materials Science, Multidisciplinary
A. Shchepetilnikov, A. R. Khisameeva, Yu A. Nefyodov, I. Kukushkin
Summary: The study investigates the spin relaxation of a strongly correlated electron system in a narrow AlAs quantum well near odd fillings of the integer quantum Hall effect. Results show that increasing tilt angle in the magnetic field leads to a significant decrease in relaxation time and alters the dependence of relaxation rate on filling factor at highest tilt angles. The observed effects are attributed to the renormalization of spin excitation spectra by strong electron-electron interactions.
Article
Chemistry, Physical
Sergey Yu. Ketkov, Sheng-Yuan Tzeng, Elena A. Rychagova, Anton N. Lukoyanov, Wen-Bih Tzeng
Summary: Metallocenes, including methylcobaltocene, play important roles in various fields of chemistry. The ionization energy and vibrational structure of (Cp ')(Cp)Co can be influenced by introducing methyl substituents. The mass-analyzed threshold ionization spectrum and DFT calculations provide accurate information about the properties and transformations of (Cp ')(Cp)Co.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Review
Chemistry, Physical
Qifeng Mu, Jian Hu
Summary: Polymer mechanochemistry has experienced a renaissance due to the rapid development of mechanophores and principles governing mechanochemical transduction or material strengthening. It has not only provided fundamental guidelines for converting mechanical energy into chemical output, but also found applications in engineering and smart devices.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Da Hye Yang, Francesco Ricci, Fredrik L. Nordstrom, Na Li
Summary: Through systematic evaluation of the oiling-out behavior of procaine, we identified both stable and metastable liquid-liquid phase separation, and established phase diagrams to assist in rational selection of crystallization strategies.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Vikki Anand Varma, Simmie Jaglan, Mohd Yasir Khan, Sujin B. Babu
Summary: Designing engineering structures like nanocages, shells, and containers through self-assembly of colloids is a challenging problem. This work proposes a simple model for the subunit, which leads to the formation of monodispersed spherical cages or containers. The model with only one control parameter can be used to design cages with the desired radius.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Hainan Jiang, Yaolong He, Xiaolin Li, Zhiyao Jin, Huijie Yu, Dawei Li
Summary: The cycling lifespan and coulombic efficiency of lithium-ion batteries are crucial for high C-rate applications. The Li-ion concentration plays a crucial role in determining the mechanical integrity and structural stability of electrodes. This study focuses on graphite as the working electrode and establishes an experimental system to investigate the mechanical properties of composite graphite electrode at different C-rates. Considering the effect of Li-ion concentration in stress analysis is found to be significant.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Zhiye Wang, Yunchuan Li, Mingjun Sun
Summary: This study investigates the influence of intramolecular pi-pi interactions on the electronic transport capabilities of molecules. By designing and analyzing three pi-conjugated molecules, the researchers observe that different pi-conjugated structures have varying effects on electron transport. The findings provide a theoretical foundation for designing single-molecule electronic devices with multiple electron channels based on intramolecular pi-pi interactions.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Yuandong Xu, Haoyang Feng, Chaoyang Dong, Yuqing Yang, Meng Zhou, Yajun Wei, Hui Guo, Yaqing Wei, Jishan Su, Yingying Ben, Xia Zhang
Summary: Hollow MoS2 cubes and spheres were successfully synthesized using a one-step hydrothermal method with the hard template method. The hollow MoS2 cubes exhibited higher specific capacitance and energy density compared to the hollow MoS2 spheres. The symmetrical supercapacitors assembled with these hollow structures showed good performance and high capacity retention after multiple cycles. These findings suggest that controlling the pore structure and surface characteristics of MoS2 is crucial for enhancing its electrochemical properties.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Ainhoa Oliden-Sanchez, Rebeca Sola-Llano, Joaquin Perez-Pariente, Luis Gomez-Hortiguela, Virginia Martinez-Martinez
Summary: The combination of photoactive molecules and inorganic structures is important for the development of advanced materials in optics. In this study, bulky dyes were successfully encapsulated in a zeolitic framework, resulting in emission throughout the visible spectrum.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Miaomiao Zhang, Cunyuan Pei, Qiqi Xiang, Lintao Liu, Zhongxu Dai, Huijuan Ma, Shibing Ni
Summary: The design of a solid electrolyte interphase (SEI) plays a crucial role in improving the electrochemical performance of anode materials. In this study, lithium difluoro(oxalate)borate (LiDFOB) is used as an electrolyte additive to form a protective SEI film on Li3VO4 (LVO) anodes. The addition of LiDFOB results in a dense, uniform, stable, and LiF-richer SEI, which enhances the Li-ion storage kinetics. The generated SEI also prevents further decomposition of the electrolyte and maintains the morphology of LVO anodes during charge/discharge processes. This work demonstrates the effectiveness of LiDFOB as a multi-functional additive for LiPF6 electrolytes and provides insights into SEI construction for high-performance LVO anodes.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
B. V. Andryushechkin, T. V. Pavlova, V. M. Shevlyuga
Summary: The atomic structure of the Ag(111)-p(4 x 4)-O phase was reexamined and two phases with the same periodicity were discovered. It was demonstrated that the accepted Ag6 model is incompatible with high-resolution oxygen-sensitive STM images.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
S. L. Romo-Avila, D. Marquez-Ruiz, R. A. Guirado-Lopez
Summary: In this study, we used density functional theory (DFT) calculations to investigate the interaction between model graphene oxide (GO) nanostructures and chlorine monoxide ClO. We aimed to understand the role of this highly oxidizing species in breaking C-C bonds and forming significant holes on GO sheets. Our results showed that C-C bonds in a single graphene oxide sheet can be broken through a simple mechanism involving the dissociation of two chemically attached ClO molecules. The formation of carbonyl groups and holes on the GO surface was also observed. This study provides important insights into the degradation of carbon nanotubes and the stability of GO during the myeloperoxidase (MPO) catalytic cycle.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Alberto Garcia-Fernandez, Birgit Kammlander, Stefania Riva, Hakan Rensmo, Ute B. Cappel
Summary: In this study, the X-ray stability of five different lead halide perovskite compositions (MAPbI3, MAPbCl3, MAPbBr3, FAPbBr3, CsPbBr3) was investigated using photoelectron spectroscopy. Different degradation mechanisms and resistance to X-ray were observed depending on the crystal composition. Overall, perovskite compositions based on the MA+ cation were found to be less stable than those based on FA+ or Cs+. Metallic lead formation was most easily observed in the chloride perovskite, followed by bromide, and very little in MAPbI3. Multiple degradation processes were identified for the bromide compositions, including ion migration, formation of volatile and solid products, as well as metallic lead. CsBr was formed as a solid degradation product on the surface of CsPbBr3.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Timofei Rostilov, Vadim Ziborov, Alexander Dolgoborodov, Mikhail Kuskov
Summary: The shock-loading behavior of nanomaterials is investigated in this study. It is found that shock compaction waves exhibit a distinct two-step structure, with the formation of faster precursor waves that travel ahead of the main compaction waves. The complexity of the shock Hugoniot curve of the tested nanomaterial is described, and the effect of initial porosity on the compressed states is demonstrated.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Sergey S. Nikitin, Alexander D. Koryakov, Elizaveta A. Antipinskaya, Alexey A. Markov, Mikhail V. Patrakeev
Summary: The stability of La1/3Sr2/3Fe1-xMnxO3-delta, a perovskite-type oxide, under reducing conditions is dependent on the manganese content. Increasing the manganese content leads to a decrease in stability. The behavior of iron and manganese in the oxide shows distinct differences, which can be attributed to the difference in the enthalpy of oxidation reactions. Additionally, the change in the La/Sr ratio affects the concentration of iron and manganese ions.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Mosayeb Naseri, Shirin Amirian, Mehrdad Faraji, Mohammad Abdur Rashid, Maicon Pierre Lourenco, Venkataraman Thangadurai, D. R. Salahub
Summary: Inspired by the successful transfer of freestanding ultrathin films of SrTiO3 and BiFeO3, this study assessed the structural stability and investigated the electronic, optical, and thermoelectric properties of a group of two-dimensional perovskite-type materials called perovskenes. The findings revealed that these materials are wide bandgap semiconductors with potential application in UV shielding. Moreover, they exhibit better electrical and thermal conductivity at high temperatures, enabling efficient power generation in thermoelectric devices.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)