Mapping wave packet bifurcation at a conical intersection in CH3I by attosecond XUV transient absorption spectroscopy

Chang, Kristina F.; Wang, Han; Poullain, Sonia M.; Prendergast, David; Neumark, Daniel M.; Leone, Stephen R.

doi:10.1063/5.0056299

Title: Mapping wave packet bifurcation at a conical intersection in CH₃I by attosecond XUV transient absorption spectroscopy

Journal Article · Tue Jun 15 00:00:00 EDT 2021 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/5.0056299· OSTI ID:1840946

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Univ. of California, Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. Complutense de Madrid (Spain)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Extreme ultraviolet (XUV) transient absorption spectroscopy has emerged as a sensitive tool for mapping the real-time structural and electronic evolution of molecules. Here, attosecond XUV transient absorption is used to track dynamics in the A-band of methyl iodide (CH₃I). Gaseous CH₃I molecules are excited to the A-band by a UV pump (277 nm, ~20 fs) and probed by attosecond XUV pulses targeting iodine I(4d) core-to-valence transitions. Owing to the excellent temporal resolution of the technique, passage through a conical intersection is mapped through spectral signatures of nonadiabatic wave packet bifurcation observed to occur at 15 ± 4 fs following UV photoexcitation. The observed XUV signatures and time dynamics are in agreement with previous simulations [H. Wang, M. Odelius, and D. Prendergast, J. Chem. Phys. 151, 124106 (2019)]. Furthermore, due to the short duration of the UV pump pulse, coherent vibrational motion in the CH₃I ground state along the C-I stretch mode (538 ± 7 cm^-1) launched by resonant impulsive stimulated Raman scattering and dynamics in multiphoton excited states of CH₃I are also detected.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1840946

Alternate ID(s):: OSTI ID: 1788285

Journal Information:: Journal of Chemical Physics, Vol. 154, Issue 23; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Mapping wave packet bifurcation at a conical intersection in CH3I by attosecond XUV transient absorption spectroscopy

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Title: Mapping wave packet bifurcation at a conical intersection in CH₃I by attosecond XUV transient absorption spectroscopy