Relaxation of Electronically Excited Hydrogen Peroxide in Liquid Water: Insights from Auger-Electron Emission

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F60461373%3A22340%2F13%3A43895775" target="_blank" >RIV/60461373:22340/13:43895775 - isvavai.cz</a>

Výsledek na webu

<a href="http://dx.doi.org/10.1021/jp401569w" target="_blank" >http://dx.doi.org/10.1021/jp401569w</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/jp401569w" target="_blank" >10.1021/jp401569w</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Relaxation of Electronically Excited Hydrogen Peroxide in Liquid Water: Insights from Auger-Electron Emission

Popis výsledku v původním jazyce

Autoionization electron spectroscopy is applied to study nonradiative relaxation processes of hydrogen peroxide aqueous solution irradiated by soft X-rays. The high kinetic energy part of the oxygen Is H2O2(aq) Auger-electron spectrum reveals dicationicfinal states with considerably lower energy than for neat liquid water. Assisted by quantum chemical calculations, it is argued that such lower-energy states arise from two fundamentally different relaxation processes. One is (local) Auger decay, yielding (H2O2)2+(aq) species, and here the low final-state energy arises from charge delocalization across the molecular O-O bond. Alternatively, nonlocal dicationic states can form, corresponding to a charge-separated complex comprising H2O2 and a neighboringwater molecule. Different charge-separation mechanisms, depending on whether or not proton dynamics of the core-level excited or ionized H2O2 molecule is involved, are discussed. We also present for the first time the partial electron yi

Název v anglickém jazyce

Relaxation of Electronically Excited Hydrogen Peroxide in Liquid Water: Insights from Auger-Electron Emission

Popis výsledku anglicky

Autoionization electron spectroscopy is applied to study nonradiative relaxation processes of hydrogen peroxide aqueous solution irradiated by soft X-rays. The high kinetic energy part of the oxygen Is H2O2(aq) Auger-electron spectrum reveals dicationicfinal states with considerably lower energy than for neat liquid water. Assisted by quantum chemical calculations, it is argued that such lower-energy states arise from two fundamentally different relaxation processes. One is (local) Auger decay, yielding (H2O2)2+(aq) species, and here the low final-state energy arises from charge delocalization across the molecular O-O bond. Alternatively, nonlocal dicationic states can form, corresponding to a charge-separated complex comprising H2O2 and a neighboringwater molecule. Different charge-separation mechanisms, depending on whether or not proton dynamics of the core-level excited or ionized H2O2 molecule is involved, are discussed. We also present for the first time the partial electron yi

Druh

J_x - Nezařazeno - Článek v odborném periodiku (Jimp, Jsc a Jost)

CEP obor

CF - Fyzikální chemie a teoretická chemie

OECD FORD obor

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Projekt

<a href="/cs/project/GA13-34168S" target="_blank" >GA13-34168S: Ab initio simulace rentgenové fotodynamiky a spektroskopie ve vodných roztocích</a><br>

Návaznosti

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

Rok uplatnění

2013

Kód důvěrnosti údajů

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

Název periodika

Journal of Physical Chemistry C

ISSN

1932-7447

e-ISSN

—

Svazek periodika

117

Číslo periodika v rámci svazku

43

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

8

Strana od-do

22268-22275

Kód UT WoS článku

000326608200015

EID výsledku v databázi Scopus

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