Over the past several years, a new generation of quantum simulations has greatly expanded our understanding of charge density wave phase transitions in Hamiltonians with coupling between local phonon modes and the on-site charge density. A quite different, and interesting, case is one in which the phonons live on the bonds, and hence modulate the electron hopping. This situation, described by the Su-Schrieffer-Heeger (SSH) Hamiltonian, has so far only been studied with quantum Monte Carlo in one dimension. Here we present results for the 2D SSH model, show that a bond ordered wave (BOW) insulator is present in the ground state at half filling, and argue that a critical value of the electron-phonon coupling is required for its onset, in contradistinction with the 1D case where BOW exists for any nonzero coupling. We determine the precise nature of the bond ordering pattern, which has hitherto been controversial, and the critical transition temperature, which is associated with a spontaneous breaking of Z_{4} symmetry.
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http://dx.doi.org/10.1103/PhysRevLett.126.017601 | DOI Listing |
J Chem Theory Comput
January 2025
Center for Computational Quantum Physics, The Flatiron Institute, 162 Fifth Avenue, New York, New York, 10010, United States.
We present a generalization of the phaseless auxiliary-field quantum Monte Carlo (AFQMC) method to cavity quantum-electrodynamical (QED) matter systems. The method can be formulated in both the Coulomb and the dipole gauge. We verify its accuracy by benchmarking calculations on a set of small molecules against full configuration interaction and state-of-the-art QED coupled cluster (QED-CCSD) calculations.
View Article and Find Full Text PDFJ Chem Theory Comput
January 2025
Max-Planck-Institute for Solid State Research, Heisenbergstraße 1, 70569 Stuttgart, Germany.
A new method to perform complete active space second-order perturbation theory on top of large active spaces optimized with full configuration quantum Monte Carlo is presented. Computing the three- and Fock-contracted four-particle density matrix from imaginary-time-averaged wave functions is found to resolve fermionic positivity violations and to ensure numerical stability. The protocol is applied to [NiFe]-hydrogenase, [CuO]-oxidase and Fe-porphyrin model systems up to 26 electrons in 27 orbitals and benchmarked against DMRG-CASPT2.
View Article and Find Full Text PDFJ Chem Theory Comput
January 2025
Department of Chemistry, Rice University, Houston, Texas 77005-1892, United States.
Generalized Hartree-Fock (GHF) is a long-established electronic structure method that can lower the energy (compared to spin-restricted variants) by breaking physical wave function symmetries, namely and . After an exposition of GHF theory, we assess the use of GHF trial wave functions in phaseless auxiliary field quantum Monte Carlo (ph-AFQMC-G) calculations of strongly correlated molecular systems including symmetrically stretched hydrogen rings, carbon dioxide, and dioxygen. Imaginary time propagation is able to restore symmetry and yields energies of comparable or better accuracy than CCSD(T) with unrestricted HF and GHF references, and consistently smooth dissociation curves─a remarkable result given the relative scalability of ph-AFQMC-G to larger system sizes.
View Article and Find Full Text PDFBiomed Opt Express
January 2025
Department of Electronic Engineering, Shanghai Jiao Tong University, Shanghai 200240, China.
Optical coherence tomography angiography (OCTA) offers unparalleled capabilities for non-invasive detection of vessels. However, the lack of accurate models for light-tissue interaction in OCTA jeopardizes the development of the techniques to further extract quantitative information from the measurements. In this manuscript, we propose a Monte Carlo (MC)-based simulation method to precisely describe the signal formation of OCTA based on the fundamental theory of light-tissue interactions.
View Article and Find Full Text PDFJ Phys Chem A
January 2025
Université Paris-Saclay, CNRS, Institut des Sciences Moléculaires d'Orsay UMR 8214, 91405 Orsay, France.
This study deals with the understanding of hydrogen atom scattering from graphene, a process critical for exploring C-H bond formation and energy transfer during atom surface collision. In our previous work [Shi, L.; 2023, 159, 194102], starting from a cell with 24 carbon atoms treated periodically, we have achieved quantum dynamics (QD) simulations with a reduced-dimensional model (15D) and a simulation in full dimensionality (75D).
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