Observation of electron-transfer-mediated decay in aqueous solution

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F60461373%3A22340%2F17%3A43914361" target="_blank" >RIV/60461373:22340/17:43914361 - isvavai.cz</a>

Výsledek na webu

<a href="https://www.nature.com/articles/nchem.2727" target="_blank" >https://www.nature.com/articles/nchem.2727</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1038/NCHEM.2727" target="_blank" >10.1038/NCHEM.2727</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Observation of electron-transfer-mediated decay in aqueous solution

Popis výsledku v původním jazyce

Photoionization is at the heart of X-ray photoelectron spectroscopy (XPS), which gives access to important information on a sample&apos;s local chemical environment. Local and non-local electronic decay after photoionization-in which the refilling of core holes results in electron emission from either the initially ionized species or a neighbour, respectively-have been well studied. However, electron-transfer-mediated decay (ETMD), which involves the refilling of a core hole by an electron from a neighbouring species, has not yet been observed in condensed phase. Here we report the experimental observation of ETMD in an aqueous LiCl solution by detecting characteristic secondary low-energy electrons using liquid-microjet soft XPS. Experimental results are interpreted using molecular dynamics and high-level ab initio calculations. We show that both solvent molecules and counterions participate in the ETMD processes, and different ion associations have distinctive spectral fingerprints. Furthermore, ETMD spectra are sensitive to coordination numbers, ion-solvent distances and solvent arrangement.

Název v anglickém jazyce

Observation of electron-transfer-mediated decay in aqueous solution

Popis výsledku anglicky

Photoionization is at the heart of X-ray photoelectron spectroscopy (XPS), which gives access to important information on a sample&apos;s local chemical environment. Local and non-local electronic decay after photoionization-in which the refilling of core holes results in electron emission from either the initially ionized species or a neighbour, respectively-have been well studied. However, electron-transfer-mediated decay (ETMD), which involves the refilling of a core hole by an electron from a neighbouring species, has not yet been observed in condensed phase. Here we report the experimental observation of ETMD in an aqueous LiCl solution by detecting characteristic secondary low-energy electrons using liquid-microjet soft XPS. Experimental results are interpreted using molecular dynamics and high-level ab initio calculations. We show that both solvent molecules and counterions participate in the ETMD processes, and different ion associations have distinctive spectral fingerprints. Furthermore, ETMD spectra are sensitive to coordination numbers, ion-solvent distances and solvent arrangement.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10403 - Physical chemistry

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

2017

Kód důvěrnosti údajů

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

Název periodika

Nature Chemistry

ISSN

1755-4330

e-ISSN

—

Svazek periodika

9

Číslo periodika v rámci svazku

7

Stát vydavatele periodika

GB - Spojené království Velké Británie a Severního Irska

Počet stran výsledku

7

Strana od-do

708-714

Kód UT WoS článku

000404056800019

EID výsledku v databázi Scopus

2-s2.0-85021291785