Femtosecond symmetry breaking and coherent relaxation of methane cations via x-ray spectroscopy-Reference-Cited by-同舟云学术

Femtosecond symmetry breaking and coherent relaxation of methane cations via x-ray spectroscopy

Published:2023-05-19 Issue:6646 Volume:380 Page:713-717
ISSN:0036-8075
Container-title:Science
language:en
Short-container-title:Science

Author:

Ridente Enrico¹²^ORCID,Hait Diptarka¹²^ORCID,Haugen Eric A.¹²^ORCID,Ross Andrew D.¹²^ORCID,Neumark Daniel M.¹²^ORCID,Head-Gordon Martin¹²^ORCID,Leone Stephen R.¹²³^ORCID

Affiliation:

1. Department of Chemistry, University of California, Berkeley, CA 94720, USA.

2. Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.

3. Department of Physics, University of California, Berkeley, CA 94720, USA.

Abstract

Understanding the relaxation pathways of photoexcited molecules is essential to gain atomistic-level insight into photochemistry. We performed a time-resolved study of ultrafast molecular symmetry breaking through geometric relaxation (Jahn-Teller distortion) on the methane cation. Attosecond transient absorption spectroscopy with soft x-rays at the carbon K-edge revealed that the distortion occurred within 10 ± 2 femtoseconds after few-femtosecond strong-field ionization of methane. The distortion activated coherent oscillations in the asymmetric scissoring vibrational mode of the symmetry-broken cation, which were detected in the x-ray signal. These oscillations were damped within 58 ± 13 femtoseconds because vibrational coherence was lost with the energy redistributing into lower-frequency vibrational modes. This study completely reconstructs the molecular relaxation dynamics of this prototypical example and opens avenues for exploring complex systems.

Publisher

American Association for the Advancement of Science (AAAS)

Subject

Multidisciplinary

Link

https://www.science.org/doi/pdf/10.1126/science.adg4421

Reference64 articles.

1. Stability of polyatomic molecules in degenerate electronic states - I—Orbital degeneracy

2. Modern Aspects of the Jahn−Teller Effect Theory and Applications To Molecular Problems

3. H. C. Longuet-Higgins in Advances in Spectroscopy H. W. Thompson Ed. (Interscience Publishers 1961) pp. 429–472.

4. Structure of Jahn–Teller distorted solvated copper(ii) ions in solution, and in solids with apparently regular octahedral coordination geometry

5. Interplay of Jahn–Teller and pseudo‐Jahn–Teller vibronic dynamics in the benzene cation

Cited by 19 articles. 订阅此论文施引文献订阅此论文施引文献，注册后可以免费订阅5篇论文的施引文献，订阅后可以查看论文全部施引文献

1. Benchmark Study of Core-Ionization Energies with the Generalized Active Space-Driven Similarity Renormalization Group;Journal of Chemical Theory and Computation;2024-09-13

2. Measurement of coherent vibrational dynamics with X-ray Transient Absorption Spectroscopy simultaneously at the Carbon K- and Chlorine L2,3- edges;Communications Physics;2024-09-13

3. Estimating vertical core-excitation energies from Møller–Plesset theory with spin projection;Molecular Physics;2024-09-04

4. The presence of triple degeneracy in molecular potential energy surfaces can now be modelled using newly found analytical function;Molecular Physics;2024-09-04

5. Prediction of photodynamics of 200 nm excited cyclobutanone with linear response electronic structure and ab initio multiple spawning;The Journal of Chemical Physics;2024-06-24