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

Abstract

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.

Authors:
 [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
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1379677
Alternate Identifier(s):
OSTI ID: 1338632
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review A
Additional Journal Information:
Journal Volume: 95; Journal Issue: 1; Journal ID: ISSN 2469-9926
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS

Citation Formats

Sturm, F. P., Tong, X. M., Palacios, A., Wright, T. W., Zalyubovskaya, I., Ray, D., Shivaram, N., Martín, F., Belkacem, A., Ranitovic, P., and Weber, Th. Mapping and controlling ultrafast dynamics of highly excited H2 molecules by VUV-IR pump-probe schemes. United States: N. p., 2017. Web. doi:10.1103/PhysRevA.95.012501.
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. Mapping and controlling ultrafast dynamics of highly excited H2 molecules by VUV-IR pump-probe schemes. United States. https://doi.org/10.1103/PhysRevA.95.012501
Sturm, F. P., Tong, X. M., Palacios, A., Wright, T. W., Zalyubovskaya, I., Ray, D., Shivaram, N., Martín, F., Belkacem, A., Ranitovic, P., and Weber, Th. Mon . "Mapping and controlling ultrafast dynamics of highly excited H2 molecules by VUV-IR pump-probe schemes". United States. https://doi.org/10.1103/PhysRevA.95.012501. https://www.osti.gov/servlets/purl/1379677.
@article{osti_1379677,
title = {Mapping and controlling ultrafast dynamics of highly excited H2 molecules by VUV-IR pump-probe schemes},
author = {Sturm, F. P. and Tong, X. M. and Palacios, A. and Wright, T. W. and Zalyubovskaya, I. and Ray, D. and Shivaram, N. and Martín, F. and Belkacem, A. and Ranitovic, P. and Weber, Th.},
abstractNote = {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.},
doi = {10.1103/PhysRevA.95.012501},
journal = {Physical Review A},
number = 1,
volume = 95,
place = {United States},
year = {Mon Jan 09 00:00:00 EST 2017},
month = {Mon Jan 09 00:00:00 EST 2017}
}

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Works referencing / citing this record:

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