Molecular structure retrieval directly from laboratory-frame photoelectron spectra in laser-induced electron diffraction

Sanchez, A.; Amini, K.; Wang, S. -J.; Steinle, T.; Belsa, B.; Danek, J.; Le, A. T.; Liu, X.; Moshammer, R.; Pfeifer, T.; Richter, M.; Ullrich, J.; Gräfe, S.; Lin, C. D.; Biegert, J.

doi:10.1038/s41467-021-21855-4

Title: Molecular structure retrieval directly from laboratory-frame photoelectron spectra in laser-induced electron diffraction

Journal Article · Tue Mar 09 00:00:00 EST 2021 · Nature Communications

DOI:https://doi.org/10.1038/s41467-021-21855-4· OSTI ID:1817016

^[1]; Amini, K. ^[1]; Wang, S. -J. ^[2]; Steinle, T. ^[1];

^[1];

^[2]; Le, A. T. ^[3];

^[1]; Moshammer, R. ^[4];

^[4];

^[4]; Ullrich, J. ^[5]; Gräfe, S. ^[6];

^[3];

^[7]

The Barcelona Inst. of Science and Technology, Barcelona (Spain). ICFO-Institut de Ciencies Fotoniques
Kansas State Univ., Manhattan, KS (United States). Dept. of Physics, J. R. Macdonald Lab.
Kansas State Univ., Manhattan, KS (United States). Dept. of Physics, J. R. Macdonald Lab.; Missouri Univ. of Science and Technology, Rolla, MO (United States). Dept. of Physics
Max-Planck-Institut für Kernphysik, Heidelberg (Germany)
Max-Planck-Institut für Kernphysik, Heidelberg (Germany); Physikalisch-Technische Bundesanstalt, Braunschweig (Germany)
Friedrich-Schiller-Universität Jena (Germany). Inst. of Physical Chemistry. Abbe Center of Photonics
The Barcelona Inst. of Science and Technology, Barcelona (Spain). ICFO-Institut de Ciencies Fotoniques; Univ. Autonoma de Barcelona (Spain). Inst. Catalana de Recerca i Estudis Avancats (ICREA) and Inst. de Fisica d'Altes Energies (IFAE)

Ubiquitous to most molecular scattering methods is the challenge to retrieve bond distance and angle from the scattering signals since this requires convergence of pattern matching algorithms or fitting methods. This problem is typically exacerbated when imaging larger molecules or for dynamic systems with little a priori knowledge. Here, we employ laser-induced electron diffraction (LIED) which is a powerful means to determine the precise atomic configuration of an isolated gas-phase molecule with picometre spatial and attosecond temporal precision. We introduce a simple molecular retrieval method, which is based only on the identification of critical points in the oscillating molecular interference scattering signal that is extracted directly from the laboratory-frame photoelectron spectrum. The method is compared with a Fourier-based retrieval method, and we show that both methods correctly retrieve the asymmetrically stretched and bent field-dressed configuration of the asymmetric top molecule carbonyl sulfide (OCS), which is confirmed by our quantum-classical calculations.

View Accepted Manuscript (DOE)

Cite

Export

Save

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; Polish National Science Centre (NCN); Marie Sklodowska-Curie Foundation; European Research Council (ERC)

Grant/Contract Number:: FG02-86ER13491; 2016/20/W/ST4/00314; 641272; 772676

OSTI ID:: 1817016

Journal Information:: Nature Communications, Vol. 12, Issue 1; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

References (34)

Electron Diffraction as a Tool of Structural Chemistry Schåfer, Lothar Applied Spectroscopy, Vol. 30, Issue 2 https://doi.org/10.1366/000370276774456381	journal	March 1976
Imaging CF ₃ I conical intersection and photodissociation dynamics with ultrafast electron diffraction Yang, Jie; Zhu, Xiaolei; Wolf, Thomas J. A. Science, Vol. 361, Issue 6397 https://doi.org/10.1126/science.aat0049	journal	July 2018
Ultrafast electron diffraction imaging of bond breaking in di-ionized acetylene Wolter, B.; Pullen, M. G.; Le, A. -T. Science, Vol. 354, Issue 6310 https://doi.org/10.1126/science.aah3429	journal	October 2016
Ab initio potential energy surfaces for excited states of the OCS ⁺ molecular ion Hirst, David M. Molecular Physics, Vol. 104, Issue 1 https://doi.org/10.1080/00268970500373304	journal	January 2006
Simultaneous observation of nuclear and electronic dynamics by ultrafast electron diffraction Yang, Jie; Zhu, Xiaolei; F. Nunes, J. Pedro Science, Vol. 368, Issue 6493 https://doi.org/10.1126/science.abb2235	journal	May 2020
The photochemical ring-opening of 1,3-cyclohexadiene imaged by ultrafast electron diffraction Wolf, T. J. A.; Sanchez, D. M.; Yang, J. Nature Chemistry, Vol. 11, Issue 6 https://doi.org/10.1038/s41557-019-0252-7	journal	April 2019
A new integral equation for treating high-intensity multiphoton processes Varró, S.; Ehlotzky, F. Il Nuovo Cimento D, Vol. 15, Issue 11 https://doi.org/10.1007/BF02451683	journal	November 1993
Influence of orbital symmetry on diffraction imaging with rescattering electron wave packets Pullen, M. G.; Wolter, B.; Le, A. -T. Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms11922	journal	June 2016
Atomic-resolution imaging of carbonyl sulfide by laser-induced electron diffraction Karamatskos, Evangelos T.; Goldsztejn, Gildas; Raabe, Sebastian The Journal of Chemical Physics, Vol. 150, Issue 24 https://doi.org/10.1063/1.5093959	journal	June 2019
Laser-induced electron diffraction: a new tool for probing ultrafast molecular dynamics Zuo, T.; Bandrauk, A. D.; Corkum, P. B. Chemical Physics Letters, Vol. 259, Issue 3-4 https://doi.org/10.1016/0009-2614(96)00786-5	journal	September 1996
Above threshold ionization beyond the high harmonic cutoff Schafer, K. J.; Yang, Baorui; DiMauro, L. F. Physical Review Letters, Vol. 70, Issue 11 https://doi.org/10.1103/PhysRevLett.70.1599	journal	March 1993
Imaging an aligned polyatomic molecule with laser-induced electron diffraction Pullen, Michael G.; Wolter, Benjamin; Le, Anh-Thu Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms8262	journal	June 2015
Electron diffraction in above-threshold ionization of molecules Lein, M.; Marangos, J. P.; Knight, P. L. Physical Review A, Vol. 66, Issue 5 https://doi.org/10.1103/PhysRevA.66.051404	journal	November 2002
Nonadiabatic dynamics: The SHARC approach Mai, Sebastian; Marquetand, Philipp; González, Leticia Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 8, Issue 6 https://doi.org/10.1002/wcms.1370	journal	May 2018
A correlated ab initio study of linear carbon-chain radicals CnH (n = 2−7) Woon, David E. Chemical Physics Letters, Vol. 244, Issue 1-2 https://doi.org/10.1016/0009-2614(95)00906-K	journal	September 1995
Effect of molecular bending on the photodissociation of OCS Sugita, Akihiro; Mashino, Michio; Kawasaki, Masahiro The Journal of Chemical Physics, Vol. 112, Issue 16 https://doi.org/10.1063/1.481324	journal	April 2000
Laser-Induced Electron Tunneling and Diffraction Meckel, M.; Comtois, D.; Zeidler, D. Science, Vol. 320, Issue 5882 https://doi.org/10.1126/science.1157980	journal	June 2008
Imaging ultrafast molecular dynamics with laser-induced electron diffraction Blaga, Cosmin I.; Xu, Junliang; DiChiara, Anthony D. Nature, Vol. 483, Issue 7388 https://doi.org/10.1038/nature10820	journal	March 2012
Imaging an isolated water molecule using a single electron wave packet Liu, Xinyao; Amini, Kasra; Steinle, Tobias The Journal of Chemical Physics, Vol. 151, Issue 2 https://doi.org/10.1063/1.5100520	journal	July 2019
Plasma perspective on strong field multiphoton ionization Corkum, P. B. Physical Review Letters, Vol. 71, Issue 13 https://doi.org/10.1103/PhysRevLett.71.1994	journal	September 1993
Femtosecond electron diffraction: heralding the era of atomically resolved dynamics Sciaini, Germán; Miller, R. J. Dwayne Reports on Progress in Physics, Vol. 74, Issue 9 https://doi.org/10.1088/0034-4885/74/9/096101	journal	August 2011
Direct Imaging of Transient Molecular Structures with Ultrafast Diffraction Ihee, H. Science, Vol. 291, Issue 5503 https://doi.org/10.1126/science.291.5503.458	journal	January 2001
Femtosecond gas-phase mega-electron-volt ultrafast electron diffraction Shen, X.; Nunes, J. P. F.; Yang, J. Structural Dynamics, Vol. 6, Issue 5 https://doi.org/10.1063/1.5120864	journal	September 2019
Diffractive Imaging of $C_{60}$ Structural Deformations Induced by Intense Femtosecond Midinfrared Laser Fields Fuest, Harald; Lai, Yu Hang; Blaga, Cosmin I. Physical Review Letters, Vol. 122, Issue 5 https://doi.org/10.1103/PhysRevLett.122.053002	journal	February 2019
Molcas 8: New capabilities for multiconfigurational quantum chemical calculations across the periodic table : Molcas 8 Aquilante, Francesco; Autschbach, Jochen; Carlson, Rebecca K. Journal of Computational Chemistry, Vol. 37, Issue 5 https://doi.org/10.1002/jcc.24221	journal	November 2015
High average power and single-cycle pulses from a mid-IR optical parametric chirped pulse amplifier Elu, Ugaitz; Baudisch, Matthias; Pires, Hugo Optica, Vol. 4, Issue 9 https://doi.org/10.1364/OPTICA.4.001024	journal	January 2017
Imaging the Renner–Teller effect using laser-induced electron diffraction Amini, Kasra; Sclafani, Michele; Steinle, Tobias Proceedings of the National Academy of Sciences, Vol. 116, Issue 17 https://doi.org/10.1073/pnas.1817465116	journal	April 2019
Interatomic contributions to high-energy electron-molecule scattering McCaffrey, P. D.; Dewhurst, J. K.; Rankin, D. W. H. The Journal of Chemical Physics, Vol. 128, Issue 20 https://doi.org/10.1063/1.2928806	journal	May 2008
Carbonyl sulphide under strong laser field: Time-dependent density functional theory Bilalbegović, G. The European Physical Journal D, Vol. 49, Issue 1 https://doi.org/10.1140/epjd/e2008-00137-8	journal	July 2008
Strong-field rescattering physics—self-imaging of a molecule by its own electrons Lin, C. D.; Le, Anh-Thu; Chen, Zhangjin Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 43, Issue 12 https://doi.org/10.1088/0953-4075/43/12/122001	journal	June 2010
4d Ultrafast Electron Diffraction, Crystallography, and Microscopy Zewail, Ahmed H. Annual Review of Physical Chemistry, Vol. 57, Issue 1 https://doi.org/10.1146/annurev.physchem.57.032905.104748	journal	May 2006
Nonadiabatic bending dissociation in 16 valence electron system OCS Suzuki, Toshinori; Katayanagi, Hideki; Nanbu, Shinkoh The Journal of Chemical Physics, Vol. 109, Issue 14 https://doi.org/10.1063/1.477200	journal	October 1998
An Atomic-Level View of Melting Using Femtosecond Electron Diffraction Siwick, Bradley J.; Dwyer, Jason R.; Jordan, Robert E. Science, Vol. 302, Issue 5649 https://doi.org/10.1126/science.1090052	journal	November 2003
Sub-250-mrad, passively carrier–envelope-phase-stable mid-infrared OPCPA source at high repetition rate Thai, A.; Hemmer, M.; Bates, P. K. Optics Letters, Vol. 36, Issue 19 https://doi.org/10.1364/OL.36.003918	journal	January 2011

Similar Records

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

Journal Article · Mon Oct 25 00:00:00 EDT 2021 · Journal of Chemical Physics · OSTI ID:1817016

Wang, Su-Ju; Daněk, Jiří; Blaga, Cosmin I; +3 more

Above-threshold ionization in multicenter molecules: The role of the initial state

Journal Article · Thu Mar 29 00:00:00 EDT 2018 · Physical Review A · OSTI ID:1817016

Suárez, Noslen; Chacón, Alexis; Pisanty, Emilio; +6 more

Bound state dynamics in the long-range spin-12 XXZ model

Journal Article · Wed Dec 22 00:00:00 EST 2021 · Physical Review. B · OSTI ID:1817016

Macrì, Tommaso; Lepori, Luca; Pagano, Guido; +2 more

Related Subjects

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS
atomic and molecular physics
optical techniques

Title: Molecular structure retrieval directly from laboratory-frame photoelectron spectra in laser-induced electron diffraction

Citation Formats

References (34)

Similar Records

Related Subjects