Time-dependent Hole States in Multiconfigurational Time-Dependent Hartree-Fock Approaches: A Time-Domain Generalization of Extended Koopmans' Theorem

• URL: http://arxiv.org/abs/2505.11290v1
• Date: Fri, 16 May 2025 14:24:34 GMT
• Title: Time-dependent Hole States in Multiconfigurational Time-Dependent Hartree-Fock Approaches: A Time-Domain Generalization of Extended Koopmans' Theorem
• Authors: Zhao-Han Zhang, Yang Li, Himadri Pathak, Takeshi Sato, Kenichi L. Ishikawa, Feng He,
• Abstract summary: We introduce a time-domain generalization of the extended Koopmans' theorem within the framework of the multiconfigurational time-dependent Hartree-Fock theory.<n>This formulation naturally yields well-defined time-dependent hole states formed by removing one electron from the multielectron system.<n>We develop a systematic approach to extract hole-resolved observables directly from the time-dependent textitab initio wavefunctions.
• Score: 3.1101644254432896
• License: http://creativecommons.org/licenses/by/4.0/
• Abstract: We introduce a time-domain generalization of the extended Koopmans' theorem within the framework of the multiconfigurational time-dependent Hartree-Fock (MCTDHF) theory. This formulation naturally yields well-defined time-dependent hole states formed by removing one electron from the multielectron system, enabling the instantaneous construction of reduced density matrices for the photofragments during MCTDHF simulations with negligible computational overhead. Leveraging this foundation, we derive the equation of motion for the time-dependent Dyson orbitals and develop a systematic approach to extract hole-resolved observables directly from the time-dependent \textit{ab initio} wavefunctions, such as channel-resolved photoelectron momentum distributions. The proposed method is universally applicable to both projection-based and flux-based schemes, offering a powerful tool for disentangling correlated electron-hole dynamics in ultrafast multichannel ionization processes.

Related papers

• Time-dependent Hole States in Multiconfigurational Time-Dependent Hartree-Fock Approaches: Applications in Photoionization of Water Molecule [3.1101644254432896]
  We study the single-photon ionization process of a body-fixed water molecule driven by attosecond pulses.<n>We present a full-dimensional implementation of the MCTDHF method based on one-center expansions.<n>We explore the ultrafast control of attosecond coherence between electronic states of $mathrmHO+$.
  arXiv  Detail & Related papers  (2025-05-16T14:42:37Z)
• Time-dependent Neural Galerkin Method for Quantum Dynamics [42.81677042059531]
  We introduce a classical computational method for quantum dynamics that relies on a global-in-time variational principle.<n>Our scheme computes the entire state trajectory over a finite time window by minimizing a loss function that enforces the Schr"odinger's equation.<n>We showcase the method by simulating global quantum quenches in the paradigmatic Transverse-Field Ising model in both 1D and 2D.
  arXiv  Detail & Related papers  (2024-12-16T13:48:54Z)
• Information scrambling and entanglement dynamics in Floquet Time Crystals [49.1574468325115]
  We study the dynamics of out-of-time-ordered correlators (OTOCs) and entanglement of entropy as measures of information propagation in disordered systems.
  arXiv  Detail & Related papers  (2024-11-20T17:18:42Z)
• A Path Integral Treatment of Time-dependent Dunkl Quantum Mechanics [0.0]
  We reformulated the path integral to develop an explicit expression for the propagator. This formalism is applied to specific cases, including a Dunkl-harmonic oscillator with time-dependent mass and frequency.
  arXiv  Detail & Related papers  (2024-10-27T17:53:08Z)
• Krylov Subspace Methods for Quantum Dynamics with Time-Dependent Generators [0.0]
  We introduce a generalization valid for driven quantum systems governed by a time-dependent Hamiltonian.<n>This representation is used to establish a novel class of fundamental limits to the quantum speed of evolution and operator growth.<n>We also discuss generalizations of the algorithm, adapted to discretized time evolutions and periodic Hamiltonians, with applications to many-body systems.
  arXiv  Detail & Related papers  (2024-08-15T19:00:24Z)
• Diagrammatic representation and nonperturbative approximation of exact time-convolutionless master equation [0.0]
  We provide a general framework to model non-Markovian dynamics of an open quantum system with a time-local generator. A truncation of the perturbation expansion leads to the perturbative time-convolutionless quantum master equations.
  arXiv  Detail & Related papers  (2023-10-18T05:59:15Z)
• Faster spectral density calculation using energy moments [77.34726150561087]
  We reformulate the recently proposed Gaussian Integral Transform technique in terms of Fourier moments of the system Hamiltonian. One of the main advantages of this framework is that it allows for an important reduction of the computational cost.
  arXiv  Detail & Related papers  (2022-11-01T23:57:58Z)
• Real-Space, Real-Time Approach to Quantum-Electrodynamical Time-Dependent Density Functional Theory [55.41644538483948]
  The equations are solved by time propagating the wave function on a tensor product of a Fock-space and real-space grid. Examples include the coupling strength and light frequency dependence of the energies, wave functions, optical absorption spectra, and Rabi splitting magnitudes in cavities.
  arXiv  Detail & Related papers  (2022-09-01T18:49:51Z)
• Time Dependent Hamiltonian Simulation Using Discrete Clock Constructions [42.3779227963298]
  We provide a framework for encoding time dependent dynamics as time independent systems. First, we create a time dependent simulation algorithm based on performing qubitization on the augmented clock system. Second, we define a natural generalization of multiproduct formulas for time-ordered exponentials.
  arXiv  Detail & Related papers  (2022-03-21T21:29:22Z)
• Fast Thermalization from the Eigenstate Thermalization Hypothesis [69.68937033275746]
  Eigenstate Thermalization Hypothesis (ETH) has played a major role in understanding thermodynamic phenomena in closed quantum systems. This paper establishes a rigorous link between ETH and fast thermalization to the global Gibbs state. Our results explain finite-time thermalization in chaotic open quantum systems.
  arXiv  Detail & Related papers  (2021-12-14T18:48:31Z)
• Heisenberg treatment of multiphoton pulses in waveguide QED with time-delayed feedback [62.997667081978825]
  We propose a projection onto a complete set of states in the Hilbert space to decompose the multi-time correlations into single-time matrix elements. We consider the paradigmatic example of a two-level system that couples to a semi-infinite waveguide and interacts with quantum light pulses.
  arXiv  Detail & Related papers  (2021-11-04T12:29:25Z)
• Fast and differentiable simulation of driven quantum systems [58.720142291102135]
  We introduce a semi-analytic method based on the Dyson expansion that allows us to time-evolve driven quantum systems much faster than standard numerical methods. We show results of the optimization of a two-qubit gate using transmon qubits in the circuit QED architecture.
  arXiv  Detail & Related papers  (2020-12-16T21:43:38Z)

This list is automatically generated from the titles and abstracts of the papers in this site.

This site does not guarantee the quality of this site (including all information) and is not responsible for any consequences.