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Angle-dependent strong-field ionization of halomethanes

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.5121711· OSTI ID:1802356
 [1];  [2];  [3];  [1];  [4];  [4];  [3];  [2];  [3];  [1]
  1. Univ. of Virginia, Charlottesville, VA (United States). Dept. of Physics
  2. Louisiana State Univ., Baton Rouge, LA (United States). Dept. of Chemistry
  3. Louisiana State Univ., Baton Rouge, LA (United States). Dept. of Physics and Astronomy
  4. The Ohio State Univ., Columbus, OH (United States). Dept. of Physics
+ Show Author Affiliations
We study, experimentally and theoretically, the ionization probability of singly halogenated methane molecules, CH3Cl and CH3Br, in intense linearly polarized 800 nm laser pulses as a function of the angle between the molecular axis and the laser polarization. Experimentally, the molecules are exposed to two laser pulses with a relative time delay. The first, weaker pulse induces a nuclear rotational wave packet within the molecules, which are then ionized by the second, stronger pulse. The angle-dependent ionization yields are extracted from fits of the measured delay-dependent ionization signal to a superposition of moments of the rotational wave packet’s angular distribution. Angle-dependent strong-field ionization (SFI) yields are also calculated using time-dependent density functional theory. Good agreement between measurements and theory is obtained. Interestingly, we find a marked difference between the angle-dependence of the ionization yields for these two halomethane species despite the similar structure of their highest occupied molecular orbitals. Calculations reveal that these differences are a result of multichannel (CH3Cl) vs single-channel (CH3Br) ionization and of increased hole localization on Br vs Cl. By adding calculations for CH3F, we can discern clear trends in the ionization dynamics with increasing halogen mass. These results are illustrative, as chemical functionalization and molecular alignment are likely to be important parameters for initiating and controlling charge migration dynamics via SFI.
Research Organization:
Louisiana State Univ., Baton Rouge, LA (United States)
Sponsoring Organization:
USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0012462
OSTI ID:
1802356
Alternate ID(s):
OSTI ID: 1607571
Journal Information:
Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 19 Vol. 151; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English

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