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Title: Mapping and controlling ultrafast dynamics of highly excited H 2 molecules by VUV-IR pump-probe schemes

Journal Article · · Physical Review A
 [1];  [2];  [3];  [4];  [4];  [4];  [4];  [5];  [4];  [6];  [4]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division; Univ. of Frankfurt (Germany). Inst. of Nuclear Physics
  2. Univ. of Tsukuba (Japan). Center for Computational Sciences
  3. Autonomous Univ. of Madrid (Spain). Dept. of Chemistry
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
  5. Autonomous Univ. of Madrid (Spain). Dept. of Chemistry, Condensed Matter Physics Center (IFIMAC); Madrid Institute of Advanced Studies in Nanoscience (IMDEA-Nano), Madrid (Spain)
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division; ETH Zurich (Switzerland). Labl of Physical Chemistry
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Here, we used ultrashort femtosecond vacuum ultraviolet (VUV) and infrared (IR) pulses in a pump-probe scheme to map the dynamics and nonequilibrium dissociation channels of excited neutral H2 molecules. A nuclear wave packet is created in the B1Σ$$+\atop{u}$$ state of the neutral H2 molecule by absorption of the ninth harmonic of the driving infrared laser field. Due to the large stretching amplitude of the molecule excited in the B1Σ$$+\atop{u}$$ electronic state, the effective H2+ ionization potential changes significantly as the nuclear wave packet vibrates in the bound, highly electronically and vibrationally excited B potential-energy curve. We probed such dynamics by ionizing the excited neutral molecule using time-delayed VUV-or-IR radiation. We identified the nonequilibrium dissociation channels by utilizing three-dimensional momentum imaging of the ion fragments. We also found that different dissociation channels can be controlled, to some extent, by changing the IR laser intensity and by choosing the wavelength of the probe laser light. Furthermore, we concluded that even in a benchmark molecular system such as H2*, the interpretation of the nonequilibrium multiphoton and multicolor ionization processes is still a challenging task, requiring intricate theoretical analysis.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1379677
Journal Information:
Physical Review A, Journal Name: Physical Review A Journal Issue: 1 Vol. 95; ISSN PLRAAN; ISSN 2469-9926
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

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Cited By (2)

The quantum chemistry of attosecond molecular science journal July 2019
H 2 : the benchmark molecule for ultrafast science and technologies journal January 2018

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74 ATOMIC AND MOLECULAR PHYSICS