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Basic studies toward ultrafast soft x-ray photoelectron diffraction; its application to probing local structure in iodobenzene molecules

Ultrafast x-ray photoelectron diffraction (UXPD) for free molecules has a promising potential to probe the local structures of the molecules in an element-specific fashion. Our UXPD scheme consists of three steps: (1) near-infrared laser (NIR) with ns pulse duration aligns sample molecules, (2) ultr...

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Autores principales: Teramoto, T., Minemoto, S., Majima, T., Mizuno, T., Mun, J. H., Yagishita, A., Decleva, P., Tsuru, S.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Crystallographic Association 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9050171/
https://www.ncbi.nlm.nih.gov/pubmed/35496382
http://dx.doi.org/10.1063/4.0000141
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author Teramoto, T.
Minemoto, S.
Majima, T.
Mizuno, T.
Mun, J. H.
Yagishita, A.
Decleva, P.
Tsuru, S.
author_facet Teramoto, T.
Minemoto, S.
Majima, T.
Mizuno, T.
Mun, J. H.
Yagishita, A.
Decleva, P.
Tsuru, S.
author_sort Teramoto, T.
collection PubMed
description Ultrafast x-ray photoelectron diffraction (UXPD) for free molecules has a promising potential to probe the local structures of the molecules in an element-specific fashion. Our UXPD scheme consists of three steps: (1) near-infrared laser (NIR) with ns pulse duration aligns sample molecules, (2) ultra-violet laser with fs pulse duration pumps the aligned molecules, and (3) soft x-ray free-electron laser (SXFEL) with fs pulse duration probes the molecules by measuring x-ray photoelectron diffraction (XPD) profiles. Employing steps of (1) and (3), we have measured I 3d XPD profiles from ground state iodobenzene aligned by the NIR laser with the SXFEL. Then, we have intensively calculated I 3d XPD profiles with density functional theory, taking degrees of alignments of the molecules into account, to extract a distance between C and I atoms in iodobenzene from the experimental I 3d XPD profiles. Although we have failed to determine the distance from the comparison between the experimental and theoretical results, we have succeeded in concluding that the degeneracies of the initial state eliminate the sensitivity on molecular structure in the I 3d XPD profiles. Thus, the observation of fine structures in the XPD profiles could be expected, if a nondegenerate molecular orbital is selected for a probe of UXPD. Finally, we have summarized our criteria to perform UXPD successfully: (1) to use SXFEL, (2) to prepare sample molecules with the degree of alignment higher than 0.8, and (3) to select a photoemission process from a nondegenerate inner-shell orbital of sample molecules.
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spelling pubmed-90501712022-04-29 Basic studies toward ultrafast soft x-ray photoelectron diffraction; its application to probing local structure in iodobenzene molecules Teramoto, T. Minemoto, S. Majima, T. Mizuno, T. Mun, J. H. Yagishita, A. Decleva, P. Tsuru, S. Struct Dyn ARTICLES Ultrafast x-ray photoelectron diffraction (UXPD) for free molecules has a promising potential to probe the local structures of the molecules in an element-specific fashion. Our UXPD scheme consists of three steps: (1) near-infrared laser (NIR) with ns pulse duration aligns sample molecules, (2) ultra-violet laser with fs pulse duration pumps the aligned molecules, and (3) soft x-ray free-electron laser (SXFEL) with fs pulse duration probes the molecules by measuring x-ray photoelectron diffraction (XPD) profiles. Employing steps of (1) and (3), we have measured I 3d XPD profiles from ground state iodobenzene aligned by the NIR laser with the SXFEL. Then, we have intensively calculated I 3d XPD profiles with density functional theory, taking degrees of alignments of the molecules into account, to extract a distance between C and I atoms in iodobenzene from the experimental I 3d XPD profiles. Although we have failed to determine the distance from the comparison between the experimental and theoretical results, we have succeeded in concluding that the degeneracies of the initial state eliminate the sensitivity on molecular structure in the I 3d XPD profiles. Thus, the observation of fine structures in the XPD profiles could be expected, if a nondegenerate molecular orbital is selected for a probe of UXPD. Finally, we have summarized our criteria to perform UXPD successfully: (1) to use SXFEL, (2) to prepare sample molecules with the degree of alignment higher than 0.8, and (3) to select a photoemission process from a nondegenerate inner-shell orbital of sample molecules. American Crystallographic Association 2022-04-27 /pmc/articles/PMC9050171/ /pubmed/35496382 http://dx.doi.org/10.1063/4.0000141 Text en © 2022 Author(s). https://creativecommons.org/licenses/by/4.0/All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) ).
spellingShingle ARTICLES
Teramoto, T.
Minemoto, S.
Majima, T.
Mizuno, T.
Mun, J. H.
Yagishita, A.
Decleva, P.
Tsuru, S.
Basic studies toward ultrafast soft x-ray photoelectron diffraction; its application to probing local structure in iodobenzene molecules
title Basic studies toward ultrafast soft x-ray photoelectron diffraction; its application to probing local structure in iodobenzene molecules
title_full Basic studies toward ultrafast soft x-ray photoelectron diffraction; its application to probing local structure in iodobenzene molecules
title_fullStr Basic studies toward ultrafast soft x-ray photoelectron diffraction; its application to probing local structure in iodobenzene molecules
title_full_unstemmed Basic studies toward ultrafast soft x-ray photoelectron diffraction; its application to probing local structure in iodobenzene molecules
title_short Basic studies toward ultrafast soft x-ray photoelectron diffraction; its application to probing local structure in iodobenzene molecules
title_sort basic studies toward ultrafast soft x-ray photoelectron diffraction; its application to probing local structure in iodobenzene molecules
topic ARTICLES
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9050171/
https://www.ncbi.nlm.nih.gov/pubmed/35496382
http://dx.doi.org/10.1063/4.0000141
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