Observation of intermolecular Coulombic decay and shake-up satellites in liquid ammonia
The result's identifiers
Result code in IS VaVaI
<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61388963%3A_____%2F22%3A00559973" target="_blank" >RIV/61388963:_____/22:00559973 - isvavai.cz</a>
Alternative codes found
RIV/60461373:22340/22:43924772
Result on the web
<a href="https://doi.org/10.1063/4.0000151" target="_blank" >https://doi.org/10.1063/4.0000151</a>
DOI - Digital Object Identifier
<a href="http://dx.doi.org/10.1063/4.0000151" target="_blank" >10.1063/4.0000151</a>
Alternative languages
Result language
angličtina
Original language name
Observation of intermolecular Coulombic decay and shake-up satellites in liquid ammonia
Original language description
We report the first nitrogen 1s Auger-Meitner electron spectrum from a liquid ammonia microjet at a temperature of ∼223 K (-50 °C) and compare it with the simultaneously measured spectrum for gas-phase ammonia. The spectra from both phases are interpreted with the assistance of high-level electronic structure and ab initio molecular dynamics calculations. In addition to the regular Auger-Meitner-electron features, we observe electron emission at kinetic energies of 374-388 eV, above the leading Auger-Meitner peak (3a12). Based on the electronic structure calculations, we assign this peak to a shake-up satellite in the gas phase, i.e., Auger-Meitner emission from an intermediate state with additional valence excitation present. The high-energy contribution is significantly enhanced in the liquid phase. We consider various mechanisms contributing to this feature. First, in analogy with other hydrogen-bonded liquids (noticeably water), the high-energy signal may be a signature for an ultrafast proton transfer taking place before the electronic decay (proton transfer mediated charge separation). The ab initio dynamical calculations show, however, that such a process is much slower than electronic decay and is, thus, very unlikely. Next, we consider a non-local version of the Auger-Meitner decay, the Intermolecular Coulombic Decay. The electronic structure calculations support an important contribution of this purely electronic mechanism. Finally, we discuss a non-local enhancement of the shake-up processes.
Czech name
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Czech description
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Classification
Type
J<sub>imp</sub> - Article in a specialist periodical, which is included in the Web of Science database
CEP classification
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OECD FORD branch
10403 - Physical chemistry
Result continuities
Project
<a href="/en/project/GX21-26601X" target="_blank" >GX21-26601X: Probing and Transforming Matter by Electrons in Liquid Jets</a><br>
Continuities
I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace
Others
Publication year
2022
Confidentiality
S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů
Data specific for result type
Name of the periodical
Structural Dynamics
ISSN
2329-7778
e-ISSN
2329-7778
Volume of the periodical
9
Issue of the periodical within the volume
4
Country of publishing house
US - UNITED STATES
Number of pages
12
Pages from-to
044901
UT code for WoS article
000886075800001
EID of the result in the Scopus database
2-s2.0-85135461627