Finite-temperature, anharmonicity, and Duschinsky effects on the two-dimensional electronic spectra from ab initio thermo-field Gaussian wavepacket dynamics

• URL: http://arxiv.org/abs/2101.12251v3
• Date: Fri, 19 Mar 2021 11:52:30 GMT
• Title: Finite-temperature, anharmonicity, and Duschinsky effects on the two-dimensional electronic spectra from ab initio thermo-field Gaussian wavepacket dynamics
• Authors: Tomislav Begu\v{s}i\'c and Ji\v{r}\'i Van\'i\v{c}ek
• Abstract summary: We use the concept of thermo-field dynamics to derive an exact finite-temperature expression that lends itself to an intuitive wavepacket-based interpretation. An efficient method for computing finite-temperature two-dimensional spectra is obtained by combining the exact thermo-field dynamics approach with the thawed Gaussian approximation for the wavepacket dynamics.
• Score: 0.0
• License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
• Abstract: Accurate description of finite-temperature vibrational dynamics is indispensable in the computation of two-dimensional electronic spectra. Such simulations are often based on the density matrix evolution, statistical averaging of initial vibrational states, or approximate classical or semiclassical limits. While many practical approaches exist, they are often of limited accuracy and difficult to interpret. Here, we use the concept of thermo-field dynamics to derive an exact finite-temperature expression that lends itself to an intuitive wavepacket-based interpretation. Furthermore, an efficient method for computing finite-temperature two-dimensional spectra is obtained by combining the exact thermo-field dynamics approach with the thawed Gaussian approximation for the wavepacket dynamics, which is exact for any displaced, distorted, and Duschinsky-rotated harmonic potential but also accounts partially for anharmonicity effects in general potentials. Using this new method, we directly relate a symmetry breaking of the two-dimensional signal to the deviation from the conventional Brownian oscillator picture.

Related papers

• Nonlinear dynamical Casimir effect and Unruh entanglement in waveguide QED with parametrically modulated coupling [83.88591755871734]
  We study theoretically an array of two-level qubits moving relative to a one-dimensional waveguide. When the frequency of this motion approaches twice the qubit resonance frequency, it induces parametric generation of photons and excitation of the qubits. We develop a comprehensive general theoretical framework that incorporates both perturbative diagrammatic techniques and a rigorous master-equation approach.
  arXiv  Detail & Related papers  (2024-08-30T15:54:33Z)
• Thermalization and Criticality on an Analog-Digital Quantum Simulator [133.58336306417294]
  We present a quantum simulator comprising 69 superconducting qubits which supports both universal quantum gates and high-fidelity analog evolution. We observe signatures of the classical Kosterlitz-Thouless phase transition, as well as strong deviations from Kibble-Zurek scaling predictions. We digitally prepare the system in pairwise-entangled dimer states and image the transport of energy and vorticity during thermalization.
  arXiv  Detail & Related papers  (2024-05-27T17:40:39Z)
• Finite-temperature vibronic spectra from the split-operator coherence thermofield dynamics [0.0]
  We present a numerically exact approach for evaluating vibrationally resolved electronic spectra at finite temperatures. We show that the finite-temperature spectra obtained with the coherence thermofield dynamics in a Morse potential agree exactly with those computed by Boltzmann-averaging the spectra of individual vibrational levels.
  arXiv  Detail & Related papers  (2023-11-16T16:33:36Z)
• Photoinduced prethermal order parameter dynamics in the two-dimensional large-$N$ Hubbard-Heisenberg model [77.34726150561087]
  We study the microscopic dynamics of competing ordered phases in a two-dimensional correlated electron model. We simulate the light-induced transition between two competing phases.
  arXiv  Detail & Related papers  (2022-05-13T13:13:31Z)
• Applicability of the thawed Gaussian wavepacket dynamics to the calculation of vibronic spectra of molecules with double-well potential energy surfaces [0.0]
  We show that a semiclassical wavepacket approach is more robust and to provide more accurate spectra than the conventional harmonic approximation. The method is efficient and requires only a single classical ab initio molecular dynamics trajectory.
  arXiv  Detail & Related papers  (2022-01-14T20:30:41Z)
• Rotating Majorana Zero Modes in a disk geometry [75.34254292381189]
  We study the manipulation of Majorana zero modes in a thin disk made from a $p$-wave superconductor. We analyze the second-order topological corner modes that arise when an in-plane magnetic field is applied. We show that oscillations persist even in the adiabatic phase because of a frequency independent coupling between zero modes and excited states.
  arXiv  Detail & Related papers  (2021-09-08T11:18:50Z)
• Adiabatic Sensing Technique for Optimal Temperature Estimation using Trapped Ions [64.31011847952006]
  We propose an adiabatic method for optimal phonon temperature estimation using trapped ions. The relevant information of the phonon thermal distributions can be transferred to the collective spin-degree of freedom. We show that each of the thermal state probabilities is adiabatically mapped onto the respective collective spin-excitation configuration.
  arXiv  Detail & Related papers  (2020-12-16T12:58:08Z)
• On-the-fly ab initio semiclassical evaluation of third-order response functions for two-dimensional electronic spectroscopy [0.0]
  We use the single-trajectory semiclassical thawed Gaussian approximation to evaluate two-dimensional electronic spectra. We find that in this molecule, the anharmonicity effects are weak, whereas the Duschinsky rotation and the changes in the mode frequencies must be included in accurate simulations.
  arXiv  Detail & Related papers  (2020-10-06T21:29:11Z)
• Probing eigenstate thermalization in quantum simulators via fluctuation-dissipation relations [77.34726150561087]
  The eigenstate thermalization hypothesis (ETH) offers a universal mechanism for the approach to equilibrium of closed quantum many-body systems. Here, we propose a theory-independent route to probe the full ETH in quantum simulators by observing the emergence of fluctuation-dissipation relations. Our work presents a theory-independent way to characterize thermalization in quantum simulators and paves the way to quantum simulate condensed matter pump-probe experiments.
  arXiv  Detail & Related papers  (2020-07-20T18:00:02Z)
• On-the-fly ab initio semiclassical evaluation of vibronic spectra at finite temperature [0.0]
  ab initio extended thawed Gaussian approximation used to compute vibrationally resolved spectra at zero temperature. New approach allows for a clear distinction among finite-temperature, anharmonicity, and Herzberg-Teller effects on spectra.
  arXiv  Detail & Related papers  (2020-05-18T22:54:10Z)

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.