Electronic decay process spectra including nuclear degrees of freedom

• URL: http://arxiv.org/abs/2102.06040v3
• Date: Thu, 8 Aug 2024 13:40:32 GMT
• Title: Electronic decay process spectra including nuclear degrees of freedom
• Authors: Alexander Riegel, Elke Fasshauer,
• Abstract summary: We explore the ultra-rapid electronic motion spanning attoseconds to femtoseconds, demonstrating that it is equally integral and relevant to the discipline. The advent of ultrashort attosecond pulse technology has revolutionized our ability to directly observe electronic rearrangements in atoms and molecules.
• Score: 49.1574468325115
• License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
• Abstract: In the field of chemistry, where nuclear motion has traditionally been a focal point, we now explore the ultra-rapid electronic motion spanning attoseconds to femtoseconds, demonstrating that it is equally integral and relevant to the discipline. The advent of ultrashort attosecond pulse technology has revolutionized our ability to directly observe electronic rearrangements in atoms and molecules, offering a time-resolved insight into these swift processes. Prominent examples include Auger-Meitner decay and Interparticle Coulombic Decay (ICD). However, the real challenge lies in interpreting these observations, where theoretical models are indispensable. Building upon the analytical framework introduced in Phys. Rev. A 101, 043414 (2020), which analyzed the spectra of electrons emitted during electronic decay processes from a purely electronic perspective, our paper represents a significant advancement. We extend this theoretical base to include nuclear dynamics, utilizing the Born-Oppenheimer approximation to deepen our understanding of the intricate interaction between electronic and nuclear motion in these processes. We illustrate the impact of incorporating nuclear degrees of freedom in several theoretical cases characterized by different numbers of vibrational bound states in both the electronic resonance and the electronic final state. This approach not only clarifies complex spectral features and unusual peak shapes but also demonstrates a method for extracting the energy differences between multiple vibrational resonance states through their distinctive interference patterns.

Related papers

• Imaging coupled vibrational, rotational, and electronic wave packet dynamics in a triatomic molecule [3.7196648549871205]
  We show how the interplay between vibrational, rotational, and electronic degrees of freedom governs the evolution of molecular wave packets. Our results suggest that multi-coincident CEI represents an efficient experimental tool for characterizing coupled electronic and nuclear motion in polyatomic molecules.
  arXiv  Detail & Related papers  (2024-08-15T06:13:04Z)
• Effective light-induced Hamiltonian for atoms with large nuclear spin [0.0]
  Coupling with off-resonance light is an essential tool to selectively and coherently manipulate the nuclear spin states. We present a systematic derivation of the effective Hamiltonian for the nuclear spin states of ultra-cold fermionic atoms due to such an off-resonance light.
  arXiv  Detail & Related papers  (2024-04-18T18:00:01Z)
• Periodically driven open quantum systems with vibronic interaction: Resonance effects and vibrationally mediated decoupling [2.2022550150705804]
  We study the interplay between the driving field and vibronic states and its overall influence on the electronic system. Specifically, we observe an effective decoupling of the electronic system from the periodic driving at specific frequencies. These insights hold promise for efficient charge current control.
  arXiv  Detail & Related papers  (2023-09-11T16:05:43Z)
• Driving Force and Nonequilibrium Vibronic Dynamics in Charge Separation of Strongly Bound Electron-Hole Pairs [59.94347858883343]
  We study the dynamics of charge separation in one, two and three-dimensional donor-acceptor networks. This allows us to identify the precise conditions in which underdamped vibrational motion induces efficient long-range charge separation.
  arXiv  Detail & Related papers  (2022-05-11T17:51:21Z)
• Ab initio simulation of laser-induced electronic and vibrational coherence [0.0]
  We show that ensemble-averaging with initial configurations from a nuclear quantum distribution remedies many shortcomings of single-trajectory RT-TDDFT+Ehrenfest. The explicit inclusion of a time-dependent pulse in the simulations makes this method a prime advance for first-principles studies of coherent nonlinear spectroscopy.
  arXiv  Detail & Related papers  (2021-12-21T10:30:41Z)
• Relativistic aspects of orbital and magnetic anisotropies in the chemical bonding and structure of lanthanide molecules [60.17174832243075]
  We study the electronic and ro-vibrational states of heavy homonuclear lanthanide Er2 and Tm2 molecules by applying state-of-the-art relativistic methods. We were able to obtain reliable spin-orbit and correlation-induced splittings between the 91 Er2 and 36 Tm2 electronic potentials dissociating to two ground-state atoms.
  arXiv  Detail & Related papers  (2021-07-06T15:34:00Z)
• Demonstration of electron-nuclear decoupling at a spin clock transition [54.088309058031705]
  Clock transitions protect molecular spin qubits from magnetic noise. linear coupling to nuclear degrees of freedom causes a modulation and decay of electronic coherence. An absence of quantum information leakage to the nuclear bath provides opportunities to characterize other decoherence sources.
  arXiv  Detail & Related papers  (2021-06-09T16:23:47Z)
• Controlled coherent dynamics of [VO(TPP)], a prototype molecular nuclear qudit with an electronic ancilla [50.002949299918136]
  We show that [VO(TPP)] (vanadyl tetraphenylporphyrinate) is a promising system suitable to implement quantum computation algorithms. It embeds an electronic spin 1/2 coupled through hyperfine interaction to a nuclear spin 7/2, both characterized by remarkable coherence.
  arXiv  Detail & Related papers  (2021-03-15T21:38:41Z)
• Time-Dependent Self Consistent Harmonic Approximation: Anharmonic nuclear quantum dynamics and time correlation functions [0.0]
  We derive an approximate theory for the quantum time evolution of lattice vibrations at finite temperature. We apply perturbation theory around the static SCHA solution and derive an algorithm to compute efficiently quantum dynamical response functions.
  arXiv  Detail & Related papers  (2020-11-30T16:56:50Z)
• Theoretical methods for ultrastrong light-matter interactions [91.3755431537592]
  This article reviews theoretical methods developed to understand cavity quantum electrodynamics in the ultrastrong-coupling regime. The article gives a broad overview of the recent progress, ranging from analytical estimate of ground-state properties to proper computation of master equations. Most of the article is devoted to effective models, relevant for the various experimental platforms in which the ultrastrong coupling has been reached.
  arXiv  Detail & Related papers  (2020-01-23T18:09:10Z)

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.