Disentangling conical intersection and coherent molecular dynamics in methyl bromide with attosecond transient absorption spectroscopy

Abstract

Attosecond probing of core-level electronic transitions provides a sensitive tool for studying valence molecular dynamics with atomic, state, and charge specificity. In this report, we employ attosecond transient absorption spectroscopy to follow the valence dynamics of strong-field initiated processes in methyl bromide. By probing the 3d core-to-valence transition, we resolve the strong field excitation and ensuing fragmentation of the neutral * excited states of methyl bromide. The results provide a clear signature of the non-adiabatic passage of the excited state wavepacket through a conical intersection. We additionally observe competing, strong field initiated processes arising in both the ground state and ionized molecule corresponding to vibrational and spin-orbit motion, respectively. The demonstrated ability to resolve simultaneous dynamics with few-femtosecond resolution presents a clear path forward in the implementation of attosecond XUV spectroscopy as a general tool for probing competing and complex molecular phenomena with unmatched temporal resolution.

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Document Details

Document Type
Technical Report
Publication Date
Jul 16, 2019
Accession Number
AD1088870

Entities

People

  • Daniel Neumark
  • Henry Timmers
  • Maurizio Reduzzi
  • Maximilian Hollstein
  • Mazyar Sabbar
  • Stephen R. Leone
  • Todd J. Martnez
  • Xiaolei Zhu
  • Yuki Kobayashi
  • Zheng Li

Organizations

  • University of California, Berkeley

Tags

Communities of Interest

  • Energy and Power Technologies

DTIC Thesaurus Topics

  • Absorption
  • Absorption Spectra
  • Dissociation
  • Electron Holes
  • Electrons
  • Energy Bands
  • Femtosecond Time
  • Gas Cells
  • Ground State
  • Ionization
  • Molecular Dynamics
  • Photoionization
  • Potential Energy
  • Simulations
  • Spectra
  • Spectroscopy
  • Spin-Orbit Interaction

Fields of Study

  • Physics

Readers

  • Molecular Photonics/Laser Physics
  • Quantum Dot Semiconductor Device Photonics and Graphene Optoelectronic Materials and THz Physics.

Technology Areas

  • Microelectronics
  • Space