Title: Two-dimensional retrieval methods for ultrafast imaging of molecular structure using laser-induced electron diffraction

Abstract

Molecular structural retrieval based on electron diffraction has been proposed to determine the atomic positions of molecules with sub-angstrom spatial and femtosecond temporal resolutions. Given its success on small molecular systems, in this work, we point out that the accuracy of structure retrieval is constrained by the availability of a wide range of experimental data in the momentum space in all molecular systems. To mitigate the limitations, for laser-induced electron diffraction, here we retrieve molecular structures using two-dimensional (energy and angle) electron momentum spectra in the laboratory frame for a number of small molecular systems, which have previously been studied with 1D methods. Compared to the conventional single-energy or single-angle analysis, our 2D methods effectively expand the momentum range of the measured data. Besides utilization of the 2D data, two complementary methods are developed for consistency check on the retrieved results. The 2D nature of our methods also offers a way of estimating the error from retrieval, which has never been explored before. Comparing with results from prior experiments, our findings show evidence that our 2D methods outperform the conventional 1D methods. Paving the way to the retrieval of large molecular systems, in which their tunneling ionization rates are challengingmore » to obtain, we estimate the error of using the isotropic model in place of including the orientation-dependent ionization rate.« less

Authors:

Wang, Su-Ju  ^[1];

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Daněk, Jiří  ^[1];

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Blaga, Cosmin I ^[1]; DiMauro, Louis F.  ^[2];

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Biegert, Jens  ^[3];

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Lin, C. D.  ^[1]

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• Search DOE PAGES for ORCID "0000-0003-4847-8938"
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+ Show Author Affiliations

1. Kansas State Univ., Manhattan, KS (United States)
2. The Ohio State Univ., Columbus, OH (United States)
3. Barcelona Institute of Science and Technology (BIST), Barcelona (Spain); Univ. Autonoma de Barcelona (Spain). Inst. Catalana de Recerca i Estudis Avancats (ICREA)

Publication Date:

2021-10-25

Research Org.:

Kansas State Univ., Manhattan, KS (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; European Research Council (ERC); Ministry of Economic Affairs and Digital Transformation of Spain (MINECO); Polish National Science Centre (NCN); USDOE

OSTI Identifier:

1832244

Alternate Identifier(s):

OSTI ID: 1827460; OSTI ID: 1832245

Grant/Contract Number:  

FG02-86ER13491; FG02-04ER15614; 788218; 840010; 829153; 899794; 654148; FIS2017-89536-P; 2017 SGR 1639; SEV-2015-0522; 2016/20/W/ST4/00314

Resource Type:

Accepted Manuscript

Journal Name:

Journal of Chemical Physics

Additional Journal Information:

Journal Volume: 155; Journal Issue: 16; Journal ID: ISSN 0021-9606

Publisher:

American Institute of Physics (AIP)

Country of Publication:

United States

Language:

English

Subject:

74 ATOMIC AND MOLECULAR PHYSICS; Photoelectron spectroscopy; Molecular geometry; Molecular structure; Scattering theory; Elastic electron scattering; Electron diffraction; Lasers