Ultrafast isomerization in acetylene dication after carbon K-shell ionization

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61389021%3A_____%2F17%3A00508743" target="_blank" >RIV/61389021:_____/17:00508743 - isvavai.cz</a>

Nalezeny alternativní kódy

RIV/68378271:_____/17:00487226

Výsledek na webu

<a href="https://www.nature.com/articles/s41467-017-00426-6" target="_blank" >https://www.nature.com/articles/s41467-017-00426-6</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1038/s41467-017-00426-6" target="_blank" >10.1038/s41467-017-00426-6</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Ultrafast isomerization in acetylene dication after carbon K-shell ionization

Popis výsledku v původním jazyce

Ultrafast proton migration and isomerization are key processes for acetylene and its ions. However, the mechanism for ultrafast isomerization of acetylene [HCCH](2+) to vinylidene [H2CC](2+) dication remains nebulous. Theoretical studies show a large potential barrier (> 2 eV) for isomerization on low-lying dicationic states, implying picosecond or longer isomerization timescales. However, a recent experiment at a femtosecond X-ray free-electron laser suggests sub-100 fs isomerization. Here we address this contradiction with a complete theoretical study of the dynamics of acetylene dication produced by Auger decay after X-ray photoionization of the carbon atom K shell. We find no sub-100 fs isomerization, while reproducing the salient features of the time-resolved Coulomb imaging experiment. This work resolves the seeming contradiction between experiment and theory and also calls for careful interpretation of structural information from the widely applied Coulomb momentum imaging method.

Název v anglickém jazyce

Ultrafast isomerization in acetylene dication after carbon K-shell ionization

Popis výsledku anglicky

Ultrafast proton migration and isomerization are key processes for acetylene and its ions. However, the mechanism for ultrafast isomerization of acetylene [HCCH](2+) to vinylidene [H2CC](2+) dication remains nebulous. Theoretical studies show a large potential barrier (> 2 eV) for isomerization on low-lying dicationic states, implying picosecond or longer isomerization timescales. However, a recent experiment at a femtosecond X-ray free-electron laser suggests sub-100 fs isomerization. Here we address this contradiction with a complete theoretical study of the dynamics of acetylene dication produced by Auger decay after X-ray photoionization of the carbon atom K shell. We find no sub-100 fs isomerization, while reproducing the salient features of the time-resolved Coulomb imaging experiment. This work resolves the seeming contradiction between experiment and theory and also calls for careful interpretation of structural information from the widely applied Coulomb momentum imaging method.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10305 - Fluids and plasma physics (including surface physics)

Projekt

Výsledek vznikl pri realizaci vícero projektů. Více informací v záložce Projekty.

Návaznosti

P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)

Rok uplatnění

2017

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

Nature Communications

ISSN

2041-1723

e-ISSN

—

Svazek periodika

8

Číslo periodika v rámci svazku

September

Stát vydavatele periodika

GB - Spojené království Velké Británie a Severního Irska

Počet stran výsledku

7

Strana od-do

453

Kód UT WoS článku

000409458000007

EID výsledku v databázi Scopus

2-s2.0-85028911375