Aqueous Solution Chemistry of Ammonium Cation in the Auger Time Window

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61388955%3A_____%2F17%3A00500331" target="_blank" >RIV/61388955:_____/17:00500331 - isvavai.cz</a>

Nalezeny alternativní kódy

RIV/60461373:22340/17:43914360

Výsledek na webu

<a href="http://dx.doi.org/10.1038/s41598-017-00756-x" target="_blank" >http://dx.doi.org/10.1038/s41598-017-00756-x</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1038/s41598-017-00756-x" target="_blank" >10.1038/s41598-017-00756-x</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Aqueous Solution Chemistry of Ammonium Cation in the Auger Time Window

Popis výsledku v původním jazyce

We report on chemical reactions triggered by core-level ionization of ammonium (NH4+) cation in aqueous solution. Based on a combination of photoemission experiments from a liquid microjet and high-level ab initio simulations, we identified simultaneous single and double proton transfer occurring on a very short timescale spanned by the Auger-decay lifetime. Molecular dynamics simulations indicate that the proton transfer to a neighboring water molecule leads to essentially complete formation of H3O+ (aq) and core-ionized ammonia (NH3+)* (aq) within the similar to 7 fs lifetime of the nitrogen 1s core hole. A second proton transfer leads to a transient structure with the proton shared between the remaining NH2 moiety and another water molecule in the hydration shell. These ultrafast proton transfers are stimulated by very strong hydrogen bonds between the ammonium cation and water. Experimentally, the proton transfer dynamics is identified from an emerging signal at the high-kinetic energy side of the Auger-electron spectrum in analogy to observations made for other hydrogen-bonded aqueous solutions. The present study represents the most pronounced charge separation observed upon core ionization in liquids so far.

Název v anglickém jazyce

Aqueous Solution Chemistry of Ammonium Cation in the Auger Time Window

Popis výsledku anglicky

We report on chemical reactions triggered by core-level ionization of ammonium (NH4+) cation in aqueous solution. Based on a combination of photoemission experiments from a liquid microjet and high-level ab initio simulations, we identified simultaneous single and double proton transfer occurring on a very short timescale spanned by the Auger-decay lifetime. Molecular dynamics simulations indicate that the proton transfer to a neighboring water molecule leads to essentially complete formation of H3O+ (aq) and core-ionized ammonia (NH3+)* (aq) within the similar to 7 fs lifetime of the nitrogen 1s core hole. A second proton transfer leads to a transient structure with the proton shared between the remaining NH2 moiety and another water molecule in the hydration shell. These ultrafast proton transfers are stimulated by very strong hydrogen bonds between the ammonium cation and water. Experimentally, the proton transfer dynamics is identified from an emerging signal at the high-kinetic energy side of the Auger-electron spectrum in analogy to observations made for other hydrogen-bonded aqueous solutions. The present study represents the most pronounced charge separation observed upon core ionization in liquids so far.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10403 - Physical chemistry

Projekt

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

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2017

Kód důvěrnosti údajů

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

Název periodika

Scientific Reports

ISSN

2045-2322

e-ISSN

—

Svazek periodika

7

Číslo periodika v rámci svazku

1

Stát vydavatele periodika

GB - Spojené království Velké Británie a Severního Irska

Počet stran výsledku

10

Strana od-do

—

Kód UT WoS článku

000398548500003

EID výsledku v databázi Scopus

2-s2.0-85018745578