Mapping and controlling ultrafast dynamics of highly excited H2 molecules by VUV-IR pump-probe schemes

Sturm, F. P.; Tong, X. M.; Palacios, A.; Wright, T. W.; Zalyubovskaya, I.; Ray, D.; Shivaram, N.; Martín, F.; Belkacem, A.; Ranitovic, P.; Weber, Th.

doi:10.1103/PhysRevA.95.012501

Title: Mapping and controlling ultrafast dynamics of highly excited $H_{2}$ molecules by VUV-IR pump-probe schemes

Journal Article · Mon Jan 09 00:00:00 EST 2017 · Physical Review A

DOI:https://doi.org/10.1103/PhysRevA.95.012501· OSTI ID:1379677

Sturm, F. P. ^[1]; Tong, X. M. ^[2]; Palacios, A. ^[3]; Wright, T. W. ^[4]; Zalyubovskaya, I. ^[4]; Ray, D. ^[4]; Shivaram, N. ^[4]; Martín, F. ^[5]; Belkacem, A. ^[4]; Ranitovic, P. ^[6]; Weber, Th. ^[4]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division; Univ. of Frankfurt (Germany). Inst. of Nuclear Physics
Univ. of Tsukuba (Japan). Center for Computational Sciences
Autonomous Univ. of Madrid (Spain). Dept. of Chemistry
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
Autonomous Univ. of Madrid (Spain). Dept. of Chemistry, Condensed Matter Physics Center (IFIMAC); Madrid Institute of Advanced Studies in Nanoscience (IMDEA-Nano), Madrid (Spain)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division; ETH Zurich (Switzerland). Labl of Physical Chemistry

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.

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

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

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1379677

Alternate ID(s):: OSTI ID: 1338632

Journal Information:: Physical Review A, Vol. 95, Issue 1; ISSN 2469-9926

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 10 works

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