Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 116, Issue 17, Pages 8173-8177Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1817465116
Keywords
structural dynamics; electron diffraction; attosecond wave packet; laser-induced electron diffraction; nonadiabatic dynamics
Categories
Funding
- Spanish Ministry of Economy and Competitiveness (MINECO), through the Severo Ochoa Programme for Centres of Excellence in RD [SEV-2015-0522]
- Centres de Recerca de Catalunya (CERCA) Programme/Generalitat de Catalunya
- European Research Council (ERC) for ERC [788218]
- MINECO for Plan Nacional [FIS2017-89536-P]
- Agencia de Gestio d'Ajuts Universitaris i de Recerca [EU-H2020 654148, 2017 SGR1639]
- Polish National Science Center within the project Symfonia [2016/20/W/ST4/00314]
- Marie Sklodowska-Curie Grant [641272]
- MINECO [MAT2017-88492-R]
- ERC [789104]
- ERC Consolidator Grant QUEMCHEM [772676]
- German Research Foundation [GR 4482/2]
- US Department of Energy [DE-FG02-86ER13491]
- Ministerio de Economia y Competitividad [FIS2016-79508-P FISICATEAMO, SGR 1341]
- CERCA Programme
- European Union's Horizon 2020 research and innovation programme FETPRO QUIC [641122]
- ERC
- European Research Council (ERC) [772676] Funding Source: European Research Council (ERC)
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Structural information on electronically excited neutral molecules can be indirectly retrieved, largely through pump-probe and rotational spectroscopy measurements with the aid of calculations. Here, we demonstrate the direct F structural retrieval of neutral carbonyl disulfide (CS2) in the (B) over tilde (1) B-2 excited electronic state using laser-induced electron diffraction (LIED). We unambiguously identify the ultrafast symmetric stretching and bending of the field-dressed neutral CS2 molecule with combined picometer and attosecond resolution using intrapulse pump-probe excitation and measurement.We invoke the Renner-Teller effect to populate the (B) over tilde (1) B-2 excited state in neutral CS2, leading to bending and stretching of the molecule. Our results demonstrate the sensitivity of LIED in retrieving the geometric structure of CS2, which is known to appear as a two-center scatterer.
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