Article
Chemistry, Physical
Andrew M. Sand, Justin T. Malme, Erik P. Hoy
Summary: Single-molecule electronics have attracted research interest due to their small size and unique properties. A new approach, NEGF-MCPDFT, combining MCPDFT with NEGF, allows for efficient inclusion of electron correlations in the electronic structure description. The method was used to study alkane and benzyne junctions, showing agreement with DFT-NEGF results for alkane junctions and capturing additional electron correlation effects for benzyne junctions.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Moritz Bensberg, Johannes Neugebauer
Summary: In this study, a pair-selected multi-level DLPNO-CCSD (T-0) approach is proposed to accurately calculate the changes in correlation energy between orbital pairs in chemical reactions. This method is more robust than previous approaches and more efficient without adding complexity or sacrificing accuracy.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Matthew R. Hennefarth, Matthew R. Hermes, Donald G. Truhlar, Laura Gagliardi
Summary: Multiconfigurationpair-density functional theory (MC-PDFT) is a successful method for computing ground- and excited-state energies. However, it can lead to inaccurate potential energy surfaces near avoided crossings and conical intersections. In order to overcome this limitation and accurately describe molecular dynamics and Jahn-Teller instabilities, a new method called linearized PDFT (L-PDFT) is proposed. L-PDFT effectively recovers the correct potential energy surface topology and outperforms previous methods for predicting vertical excitations.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Multidisciplinary Sciences
Motoki Shimizu, Akiko Hirabuchi, Yu Sugihara, Akira Abe, Takumi Takeda, Michie Kobayashi, Yukie Hiraka, Eiko Kanzaki, Kaori Oikawa, Hiromasa Saitoh, Thorsten Langner, Mark J. Banfield, Sophien Kamoun, Ryohei Terauchi
Summary: Throughout their evolution, plant nucleotide-binding leucine-rich-repeat receptors (NLRs) have acquired widely divergent unconventional integrated domains that enhance their ability to detect pathogen effectors. However, the functional dynamics that drive the evolution of NLRs with integrated domains (NLR-IDs) remain poorly understood. Here, we reconstructed the evolutionary history of an NLR locus prone to unconventional domain integration and experimentally tested hypotheses about the evolution of NLR-IDs.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Article
Chemistry, Physical
Aleksandr O. Lykhin, Donald G. Truhlar, Laura Gagliardi
Summary: The dipole moment directly indicates molecular polarity, and the accuracy of computed dipole moments relies on the calculated electron density quality. The multiconfiguration pair-density functional theory (MC-PDFT) shows reasonable behavior in predicting dipole moments, especially for stretched geometries, and it significantly improves electron correlation compared to other methods. The recommended on-top density functionals and active space selection lead to more accurate predictions of dipole moments, with MC-PDFT and its hybrid extension (HMC-PDFT) showing comparable performance to other advanced methods.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2021)
Review
Chemistry, Physical
Prachi Sharma, Jie J. Bao, Donald G. Truhlar, Laura Gagliardi
Summary: Kohn-Sham density functional theory is less accurate for strongly correlated systems compared to weakly correlated systems. The available functionals for spin densities do not accurately predict energies for strongly correlated systems when using multiconfigurational wave functions with spin symmetry. Multiconfiguration pair-density functional theory overcomes these limitations by using a functional of the total density and on-top pair density, allowing efficient calculation of energy for strongly correlated systems.
ANNUAL REVIEW OF PHYSICAL CHEMISTRY, VOL 72
(2021)
Article
Physics, Fluids & Plasmas
Haidar Al-Naseri, Jens Zamanian, Gert Brodin
Summary: In this study, a system of coupled partial differential equations for the equal-time Wigner function in an arbitrary strong electromagnetic field was derived using the Dirac-Heisenberg-Wigner formalism. The research focused on two different cases: linearized wave propagation in a plasma and Schwinger pair production using the local density approximation. The dependence of the pair production rate on the perpendicular momentum was investigated and found to be related to the strength of the applied electric field in both cases.
Article
Astronomy & Astrophysics
Orkash Amat, Li-Na Hu, Mamat Ali Bake, Melike Mohamedsedik, B. S. Xie
Summary: The effect of spatially oscillating field on Schwinger pair production is studied using numerical and analytical methods. The results show that under large spatial scale, the characteristics of the position and momentum distribution of created pairs can be explained using the tunneling picture for the Dirac vacuum. Additionally, the Dirac-Heisenberg-Wigner formalism can be simplified using alternative methods when the spatial scale is large in a certain number of spatial oscillating cycles. The validity of these alternative methods is also discussed, and the results show that the maximum reduced particle number is about 5 times higher compared to the maximum number in a nonoscillating inhomogeneous field.
Article
Astronomy & Astrophysics
Li-Na Hu, Orkash Amat, Li Wang, Adiljan Sawut, Hong-Hao Fan, B. S. Xie
Summary: The study revisits spiral structures in multiphoton pair production induced by two counterrotating fields with time delay, revealing new findings for fields of different cycles. It is shown that subcycle fields can still generate a remarkable spiral structure in the momentum spectrum even with a large time delay, while the supercycle case requires a small time delay for easier generation. Additionally, critical polarization values exist for the appearance of spirals corresponding to different cycle numbers. The relative phase difference between the fields not only breaks the symmetry of momentum spectra and spirals, but also alters the shape and number of spiral arms.
Article
Chemistry, Physical
Riddhish Pandharkar, Matthew R. Hermes, Christopher J. Cramer, Donald G. Truhlar, Laura Gagliardi
Summary: This study introduces a new localized-active-space PDFT method, which uses LAS wave function to compute spin-state energies and gaps, and compares them to CAS-PDFT values for validation.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2021)
Article
Biophysics
Anh Thi Viet Nguyen, Bao Tuan Duong, Hyun Park, Seon-Ju Yeo
Summary: A novel peptide pair-based flow immunochromatographic test strip was developed to detect Zika virus (ZIKV) with a limit of detection of 2 x 10^4 TCID50/mL, and the test could distinguish ZIKV from Dengue virus (DENV) with high stability and performance in human sera and urine. This study demonstrates the potential of using in silico modeling to develop rapid diagnostic tests for detecting ZIKV.
BIOSENSORS & BIOELECTRONICS
(2022)
Article
Physics, Nuclear
T. Settlemyre, H. Zheng, A. Bonasera
Summary: Electron-positron pairs can be produced through the Schwinger mechanism in strong electric fields. These pairs can provide information about the dynamics of fission and alpha-decay processes, as their energy distribution is related to the relative distance and velocity of the daughter nuclei. The use of a neck model of nuclear fission illustrates how these pairs can serve as probes of the dynamics.
Article
Physics, Multidisciplinary
Clifton C. Sluss, Jace Pittman, Donald M. Nicholson, David J. Keffer
Summary: Evaluation of entropy from molecular dynamics simulation remains challenging. A recent study demonstrated a functional based on pair correlation function that can accurately determine excess entropy. This research explores the general applicability of this method and applies it to three different materials.
Article
Physics, Multidisciplinary
Ian M. Hayes, Nikola Maksimovic, Gilbert N. Lopez, Mun K. Chan, B. J. Ramshaw, Ross D. McDonald, James G. Analytis
Summary: Many unconventional superconductors exhibit strange metal properties characterized by anomalous charge transport, with measurements showing that quantum criticality is involved in driving Hall effect and correlated with superconductivity, suggesting a possible link between the three.
Article
Multidisciplinary Sciences
Qingzhen Wang, Sebastiaan L. D. ten Haaf, Ivan Kulesh, Di Xiao, Candice Thomas, Michael J. Manfra, Srijit Goswami
Summary: By coupling two quantum dots via a superconductor-semiconductor hybrid region, the authors achieve efficient splitting of Cooper pairs and measure large triplet correlations using a perpendicular magnetic field. This is the first demonstration of Cooper pair splitting in a semiconductor two-dimensional electron gas (2DEG). The exceptionally large spin-orbit interaction in their 2DEGs allows for a strong triplet component in the splitting process. This demonstration provides a credible route for studying on-chip entanglement and topological superconductivity.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Iakov Polyak, Gareth W. Richings, Scott Habershon, Peter J. Knowles
JOURNAL OF CHEMICAL PHYSICS
(2019)
Article
Chemistry, Physical
David A. Kreplin, Peter J. Knowles, Hans-Joachim Werner
JOURNAL OF CHEMICAL PHYSICS
(2020)
Article
Chemistry, Physical
Hans-Joachim Werner, Peter J. Knowles, Frederick R. Manby, Joshua A. Black, Klaus Doll, Andreas Hesselmann, Daniel Kats, Andreas Koehn, Tatiana Korona, David A. Kreplin, Qianli Ma, Thomas F. Miller, Alexander Mitrushchenkov, Kirk A. Peterson, Iakov Polyak, Guntram Rauhut, Marat Sibaev
JOURNAL OF CHEMICAL PHYSICS
(2020)
Article
Optics
Lamia Aissaoui, Peter J. Knowles, Moncef Bouledroua
EUROPEAN PHYSICAL JOURNAL D
(2020)
Article
Chemistry, Physical
Marat Sibaev, Iakov Polyak, Frederick R. Manby, Peter J. Knowles
JOURNAL OF CHEMICAL PHYSICS
(2020)
Article
Chemistry, Physical
Thomas Dresselhaus, Callum B. A. Bungey, Peter J. Knowles, Frederick R. Manby
JOURNAL OF CHEMICAL PHYSICS
(2020)
Article
Chemistry, Physical
Peter J. Knowles
Summary: This paper introduces a new general approach for defining the optimum zero-order Hamiltonian in Rayleigh-Schrodinger perturbation theory. Instead of directly deriving the operator from a model problem, it is constructed to be the best fit to the exact Hamiltonian in any desired functional form. When applied to many-body perturbation theory for electrons, significantly improved convergence is observed in cases where the conventional Fock Hamiltonian leads to divergence or slow convergence.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Multidisciplinary
Peter J. Knowles
Summary: The new approach presented in this study assigns a point group to a molecule by minimizing symmetry breaking in a coordinate frame. This measure is calculated efficiently as a simple function of molecular coordinates and point group specifications.
JOURNAL OF MATHEMATICAL CHEMISTRY
(2022)
Article
Chemistry, Physical
Marta L. Vidal, Frederick R. Manby, Peter J. Knowles
Summary: This study introduces a new computational framework that treats photons and electrons using coupled-cluster theory, focusing on the coupling between the first electronically excited state of carbon monoxide and an optical cavity. It investigates how the interaction with the photonic mode changes the vibrational spectroscopic signature of the electronic state.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Andreas Hesselmann, Hans-Joachim Werner, Peter J. Knowles
Summary: A systematic study on the accuracy and efficiency of various quadrature schemes for molecular Kohn-Sham Density-Functional Theory (DFT) revealed significant differences in accuracies among different approaches, with the new adaptive grid scheme performing the best. Integration errors are shown to be mostly independent of basis sets, with meta-GGA functionals requiring larger integration grids for the same level of accuracy compared to GGA functionals.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Optics
Yu Wang, P. J. Knowles, Jian Wang
Summary: A linear relation is discovered between Jaynes entropy and the correlation energy in a correlated molecular system, demonstrated in H-2 and water molecule. This relation modifies the Collins conjecture and may vary slightly with different basis sets. The correlation energy is found to be extensive and offers a convenient way to construct an approximate energy functional in reduced density-matrix-functional theory.
Article
Optics
Yu Wang, Feng Wang, Xiaowei Sheng, Yafei Yu, P. J. Knowles, Jian Wang
Summary: Collins conjecture is examined in dissociating molecules of H-2 and N-2, revealing a proportionality between correlation energy and entropy near equilibrium bond length, as well as between kinetic energy and entropy. In addition, the study shows a correlation between potential energy difference and entropy at larger nuclear distances, suggesting a method for estimating energy from entropy. Furthermore, the entropy from the eigenvalue spectrum of the 2-matrix is discussed.
Article
Physics, Multidisciplinary
Uliana Mordovina, Callum Bungey, Heiko Appel, Peter J. Knowles, Angel Rubio, Frederick R. Manby
PHYSICAL REVIEW RESEARCH
(2020)
Article
Physics, Atomic, Molecular & Chemical
Bridgette Cooper, Maria Tudorovskaya, Sebastian Mohr, Aran O'Hare, Martin Hanicinec, Anna Dzarasova, Jimena D. Gorfinkiel, Jakub Benda, Zdenek Masin, Ahmed F. Al-Refaie, Peter J. Knowles, Jonathan Tennyson
Article
Optics
Oleg V. Gritsenko, Jian Wang, Peter J. Knowles