Single vibronic level fluorescence spectra from Hagedorn wavepacket dynamics

• URL: http://arxiv.org/abs/2403.00577v2
• Date: Wed, 15 May 2024 09:00:48 GMT
• Title: Single vibronic level fluorescence spectra from Hagedorn wavepacket dynamics
• Authors: Zhan Tong Zhang, Jiří J. L. Vaníček,
• Abstract summary: We develop an efficient algorithm to compute the overlaps between two Hagedorn wavepackets. We study the effects of displacement, distortion (squeezing), and Duschinsky rotation on SVL spectra.
• Score: 0.0
• License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
• Abstract: In single vibronic level (SVL) fluorescence experiments, the electronically excited initial state is also excited in one or several vibrational modes. Whereas computing all contributing Franck-Condon factors individually becomes impractical in large systems, a time-dependent formalism has not been applied to simulate emission from arbitrary initial vibrational levels. Here, we use Hagedorn functions, which are products of a Gaussian and carefully generated polynomials, to represent SVL initial states. In systems where the potential is at most quadratic, the Hagedorn functions are exact solutions to the time-dependent Schr\"{o}dinger equation and can be propagated with the same equations of motion as a simple Gaussian wavepacket. Having developed an efficient recursive algorithm to compute the overlaps between two Hagedorn wavepackets, we can now evaluate emission spectra from arbitrary vibronic levels using a single trajectory. We validate the method in two-dimensional global harmonic models by comparing it with quantum split-operator calculations. Additionally, we study the effects of displacement, distortion (squeezing), and Duschinsky rotation on SVL spectra. Finally, we demonstrate the applicability of the Hagedorn approach to high-dimensional systems on an example of displaced, distorted, and Duschinsky-rotated harmonic model with 100 degrees of freedom.

Related papers

• On-the-Fly Ab Initio Hagedorn Wavepacket Dynamics: Single Vibronic Level Fluorescence Spectra of Difluorocarbene [0.0]
  Hagedorn wavepackets have been used with local harmonic approximation to partially capture the anharmonic effects on single vibronic level (SVL) spectra in model potentials. We combine local harmonic Hagedorn wavepacket dynamics with on-the-fly ab initio dynamics. We show that, whereas global harmonic models are inadequate for CF$, spectra computed with the on-the-fly local harmonic Hagedorn wavepacket dynamics agree well with experimental data, especially for low initial excitations.
  arXiv  Detail & Related papers  (2024-09-03T13:04:44Z)
• Thawed Gaussian wavepacket dynamics with $Δ$-machine learned potentials [0.0]
  We develop a method for performing variable-width (thawed) Gaussian wavepacket (GWP) variational dynamics on machine-learned potentials. Instead of fitting the potential energy surface (PES), the anharmonic correction to the global harmonic approximation (GHA) is fitted using kernel ridge regression.
  arXiv  Detail & Related papers  (2024-04-30T20:53:05Z)
• Ab initio simulation of single vibronic level fluorescence spectra of anthracene using Hagedorn wavepackets [0.0]
  Single vibronic level (SVL) fluorescence spectroscopy contributes to the understanding of molecular vibrational structures and relaxation processes. Here, we present a practical method for computing SVL fluorescence spectra of polyatomic molecules from arbitrary initial vibrational levels.
  arXiv  Detail & Related papers  (2024-03-01T17:39:42Z)
• Third quantization of open quantum systems: new dissipative symmetries and connections to phase-space and Keldysh field theory formulations [77.34726150561087]
  We reformulate the technique of third quantization in a way that explicitly connects all three methods. We first show that our formulation reveals a fundamental dissipative symmetry present in all quadratic bosonic or fermionic Lindbladians. For bosons, we then show that the Wigner function and the characteristic function can be thought of as ''wavefunctions'' of the density matrix.
  arXiv  Detail & Related papers  (2023-02-27T18:56:40Z)
• Quantum emulation of the transient dynamics in the multistate Landau-Zener model [50.591267188664666]
  We study the transient dynamics in the multistate Landau-Zener model as a function of the Landau-Zener velocity. Our experiments pave the way for more complex simulations with qubits coupled to an engineered bosonic mode spectrum.
  arXiv  Detail & Related papers  (2022-11-26T15:04:11Z)
• 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)
• Visualizing spinon Fermi surfaces with time-dependent spectroscopy [62.997667081978825]
  We propose applying time-dependent photo-emission spectroscopy, an established tool in solid state systems, in cold atom quantum simulators. We show in exact diagonalization simulations of the one-dimensional $t-J$ model that the spinons start to populate previously unoccupied states in an effective band structure. The dependence of the spectral function on the time after the pump pulse reveals collective interactions among spinons.
  arXiv  Detail & Related papers  (2021-05-27T18:00:02Z)
• Tunable Anderson Localization of Dark States [146.2730735143614]
  We experimentally study Anderson localization in a superconducting waveguide quantum electrodynamics system. We observe an exponential suppression of the transmission coefficient in the vicinity of its subradiant dark modes. The experiment opens the door to the study of various localization phenomena on a new platform.
  arXiv  Detail & Related papers  (2021-05-25T07:52:52Z)
• 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)
• 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)
• Solving quantum trajectories for systems with linear Heisenberg-picture dynamics and Gaussian measurement noise [0.0]
  We study solutions to the quantum trajectory evolution of $N$-mode open quantum systems possessing a time-independent Hamiltonian, linear Heisenbergpicture dynamics, and measurement noise. To illustrate our results, we solve some single-mode example systems, with the POVMs being of practical relevance to the inference of an initial state.
  arXiv  Detail & Related papers  (2020-04-06T03:05:22Z)

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.