Observation of site-selective chemical bond changes via ultrafast chemical shifts.
Journal
Nature communications
ISSN: 2041-1723
Titre abrégé: Nat Commun
Pays: England
ID NLM: 101528555
Informations de publication
Date de publication:
22 11 2022
22 11 2022
Historique:
received:
21
01
2022
accepted:
02
11
2022
entrez:
24
11
2022
pubmed:
25
11
2022
medline:
26
11
2022
Statut:
epublish
Résumé
The concomitant motion of electrons and nuclei on the femtosecond time scale marks the fate of chemical and biological processes. Here we demonstrate the ability to initiate and track the ultrafast electron rearrangement and chemical bond breaking site-specifically in real time for the carbon monoxide diatomic molecule. We employ a local resonant x-ray pump at the oxygen atom and probe the chemical shifts of the carbon core-electron binding energy. We observe charge redistribution accompanying core-excitation followed by Auger decay, eventually leading to dissociation and hole trapping at one site of the molecule. The presented technique is general in nature with sensitivity to chemical environment changes including transient electronic excited state dynamics. This work provides a route to investigate energy and charge transport processes in more complex systems by tracking selective chemical bond changes on their natural timescale.
Identifiants
pubmed: 36418902
doi: 10.1038/s41467-022-34670-2
pii: 10.1038/s41467-022-34670-2
pmc: PMC9684563
doi:
Substances chimiques
Carbon Monoxide
7U1EE4V452
Types de publication
Journal Article
Research Support, Non-U.S. Gov't
Langues
eng
Sous-ensembles de citation
IM
Pagination
7170Informations de copyright
© 2022. The Author(s).
Références
J Chem Theory Comput. 2019 Nov 12;15(11):5925-5964
pubmed: 31509407
Science. 1982 Jul 9;217(4555):111-21
pubmed: 17770242
Science. 2014 Oct 17;346(6207):336-9
pubmed: 25324385
Annu Rev Phys Chem. 2013;64:101-27
pubmed: 23245522
Science. 2012 Jun 8;336(6086):1287-91
pubmed: 22679093
Nat Commun. 2014 Apr 30;5:3762
pubmed: 24781868
Faraday Discuss. 2021 May 27;228(0):519-536
pubmed: 33575691
Angew Chem Int Ed Engl. 2000 Aug 4;39(15):2586-2631
pubmed: 10934390
J Chem Theory Comput. 2017 Apr 11;13(4):1723-1736
pubmed: 28240892
J Synchrotron Radiat. 2015 May;22(3):492-7
pubmed: 25931058
J Phys Chem Lett. 2019 Nov 7;10(21):6536-6544
pubmed: 31589459
Nat Commun. 2016 May 23;7:11652
pubmed: 27212390
Phys Rev Lett. 2020 Aug 14;125(7):073203
pubmed: 32857563
Phys Rev Lett. 2002 Jul 22;89(4):043001
pubmed: 12144479