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Title: Imaging an isolated water molecule using a single electron wave packet

Abstract

Observing changes in molecular structure requires atomic-scale Ångstrom and femtosecond spatio-temporal resolution. We use the Fourier transform (FT) variant of laser-induced electron diffraction (LIED), FT-LIED, to directly retrieve the molecular structure of H2O+ with picometer and femtosecond resolution without a priori knowledge of the molecular structure nor the use of retrieval algorithms or ab initio calculations. We identify a symmetrically stretched H2O+ field-dressed structure that is most likely in the ground electronic state. We subsequently study the nuclear response of an isolated water molecule to an external laser field at four different field strengths. We show that upon increasing the laser field strength from 2.5 to 3.8 V/Å, the O–H bond is further stretched and the molecule slightly bends. The observed ultrafast structural changes lead to an increase in the dipole moment of water and, in turn, a stronger dipole interaction between the nuclear framework of the molecule and the intense laser field. Our results provide important insights into the coupling of the nuclear framework to a laser field as the molecular geometry of H2O+ is altered in the presence of an external field.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [1];  [1];  [1];  [1];  [3];  [4];  [5];  [5];  [6];  [7];  [3];  [3]; ORCiD logo [8]
+ Show Author Affiliations
  1. Barcelona Institute of Science and Technology (BIST), Tarragona (Spain). ICFO—Institut de Ciencies Fotoniques
  2. Barcelona Institute of Science and Technology (BIST), Tarragona (Spain). ICFO—Institut de Ciencies Fotoniques; Univ. of Warsaw (Poland)
  3. Friedrich Schiller Univ., Jena (Germany)
  4. Missouri Univ. of Science and Technology, Rolla, MO (United States)
  5. Max Planck Inst. fuer Kernphysik, Heidelberg (Germany)
  6. Max Planck Inst. fuer Kernphysik, Heidelberg (Germany); Physikalisch-Technische Bundesanstalt (PTB), Braunschweig (Germany)
  7. Univ. of Warsaw (Poland)
  8. Barcelona Institute of Science and Technology (BIST), Tarragona (Spain). ICFO—Institut de Ciencies Fotoniques; Univ. Autonoma de Barcelona (Spain). Inst. Catalana de Recerca i Estudis Avancats (ICREA)
Publication Date:
Research Org.:
Kansas State Univ., Manhattan, KS (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); China Scholarship Council; European Research Council (ERC)
OSTI Identifier:
1610038
Grant/Contract Number:  
FG02-86ER13491
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 151; Journal Issue: 2; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
Chemistry; Physics

Citation Formats

Liu, Xinyao, Amini, Kasra, Steinle, Tobias, Sanchez, Aurelien, Shaikh, Moniruzzaman, Belsa, Blanca, Steinmetzer, Johannes, Le, Anh-Thu, Moshammer, Robert, Pfeifer, Thomas, Ullrich, Joachim, Moszynski, Robert, Lin, C. D., Gräfe, Stefanie, and Biegert, Jens. Imaging an isolated water molecule using a single electron wave packet. United States: N. p., 2019. Web. doi:10.1063/1.5100520.
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Liu, Xinyao, Amini, Kasra, Steinle, Tobias, Sanchez, Aurelien, Shaikh, Moniruzzaman, Belsa, Blanca, Steinmetzer, Johannes, Le, Anh-Thu, Moshammer, Robert, Pfeifer, Thomas, Ullrich, Joachim, Moszynski, Robert, Lin, C. D., Gräfe, Stefanie, & Biegert, Jens. Imaging an isolated water molecule using a single electron wave packet. United States. https://doi.org/10.1063/1.5100520
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Liu, Xinyao, Amini, Kasra, Steinle, Tobias, Sanchez, Aurelien, Shaikh, Moniruzzaman, Belsa, Blanca, Steinmetzer, Johannes, Le, Anh-Thu, Moshammer, Robert, Pfeifer, Thomas, Ullrich, Joachim, Moszynski, Robert, Lin, C. D., Gräfe, Stefanie, and Biegert, Jens. Thu . "Imaging an isolated water molecule using a single electron wave packet". United States. https://doi.org/10.1063/1.5100520. https://www.osti.gov/servlets/purl/1610038.
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@article{osti_1610038,
title = {Imaging an isolated water molecule using a single electron wave packet},
author = {Liu, Xinyao and Amini, Kasra and Steinle, Tobias and Sanchez, Aurelien and Shaikh, Moniruzzaman and Belsa, Blanca and Steinmetzer, Johannes and Le, Anh-Thu and Moshammer, Robert and Pfeifer, Thomas and Ullrich, Joachim and Moszynski, Robert and Lin, C. D. and Gräfe, Stefanie and Biegert, Jens},
abstractNote = {Observing changes in molecular structure requires atomic-scale Ångstrom and femtosecond spatio-temporal resolution. We use the Fourier transform (FT) variant of laser-induced electron diffraction (LIED), FT-LIED, to directly retrieve the molecular structure of H2O+ with picometer and femtosecond resolution without a priori knowledge of the molecular structure nor the use of retrieval algorithms or ab initio calculations. We identify a symmetrically stretched H2O+ field-dressed structure that is most likely in the ground electronic state. We subsequently study the nuclear response of an isolated water molecule to an external laser field at four different field strengths. We show that upon increasing the laser field strength from 2.5 to 3.8 V/Å, the O–H bond is further stretched and the molecule slightly bends. The observed ultrafast structural changes lead to an increase in the dipole moment of water and, in turn, a stronger dipole interaction between the nuclear framework of the molecule and the intense laser field. Our results provide important insights into the coupling of the nuclear framework to a laser field as the molecular geometry of H2O+ is altered in the presence of an external field.},
doi = {10.1063/1.5100520},
journal = {Journal of Chemical Physics},
number = 2,
volume = 151,
place = {United States},
year = {Thu Jul 11 00:00:00 EDT 2019},
month = {Thu Jul 11 00:00:00 EDT 2019}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1063/1.5100520
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Cited by: 16 works
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Figures / Tables:

FIG. 1 FIG. 1: FT-LIED extraction. Two-dimensional map of the longitudinal, Pl, and transverse, Pt, momenta given in atomic units (a.u.). The return momentum, kr, at the instance of rescattering is obtained by subtracting the vector potential, Ar, from the detected rescattering momentum, kresc, given by kr = kresc− Ar. The energy-dependentmore » interference signal is extracted at various different vector potential kicks (see white, yellow, and green arrows along Pt = 0) by integrating the area indicated by a block arc. A schematic is drawn at the top of the figure relating kresc (black arrow), kr (blue arrows), Ar (red arrow), and the integrated area indicated by the gray shaded block arc corresponding to a small range of rescattering angles and momenta, ∆θ and ∆k, respectively. We use ∆θr and ∆kr values of 10○ and 0.2 a.u., respectively. The dotted black lines represent the detection acceptance angle of the reaction microscope.« less
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