Potential energy surfaces of bound and metastable electron-attached states of N2O characterized by a joint experimental and theoretical study

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61388955%3A_____%2F25%3A00637617" target="_blank" >RIV/61388955:_____/25:00637617 - isvavai.cz</a>

Výsledek na webu

<a href="https://pubs.aip.org/aip/jcp/article/163/2/024120/3351962/Potential-energy-surfaces-of-bound-and-metastable" target="_blank" >https://pubs.aip.org/aip/jcp/article/163/2/024120/3351962/Potential-energy-surfaces-of-bound-and-metastable</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1063/5.0273585" target="_blank" >10.1063/5.0273585</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Potential energy surfaces of bound and metastable electron-attached states of N2O characterized by a joint experimental and theoretical study

Popis výsledku v původním jazyce

We report a combined experimental and theoretical investigation of electron scattering from nitrous oxide (N2O). Experimental two-dimensional electron energy loss spectra (EELS) provide information about vibrational states of a molecule and about potential energy surfaces of anionic resonances. This study reports the EELS measured at 2.5-2.6 eV incident energy. The calculations using complex-valued extensions of equation-of-motion coupled-cluster theory (based on the non-Hermitian quantum mechanics) facilitate the assignment of all major EELS features. Our simulations identified two broad and partially overlapping resonances-one of pi* and another of sigma* character-located at similar to 2.8 and 2.3 eV vertically at the equilibrium geometry of the neutral. Due to the Renner-Teller effect, the pi* resonance splits upon bending. The upper state, (2)Pi, remains linear. The lower state mixes with the sigma* configuration, giving rise to the (2)A ' resonance, which becomes strongly stabilized at bent geometries (alpha(NNO) = 134 degrees), resulting in very low adiabatic electron attachment energy. The calculations estimate the electron affinity of N2O to be0.140 eV. The (2)A ' state is predissociative, with the barrier for the N-O bond dissociation of 0.183 eV. The measured EELS feature sharp vibrational structures at low energy losses, followed by a linear (in logarithmic scale) tail extending to the maximum energy loss. The simulations attribute the sharp features at the low energy loss to the non-resonant excitations and contributions from the cold (2)Pi resonance. The tail is attributed to the vibrationally hot (2)A ' state, and its slope is determined by the excess energy available in this state.

Název v anglickém jazyce

Potential energy surfaces of bound and metastable electron-attached states of N2O characterized by a joint experimental and theoretical study

Popis výsledku anglicky

We report a combined experimental and theoretical investigation of electron scattering from nitrous oxide (N2O). Experimental two-dimensional electron energy loss spectra (EELS) provide information about vibrational states of a molecule and about potential energy surfaces of anionic resonances. This study reports the EELS measured at 2.5-2.6 eV incident energy. The calculations using complex-valued extensions of equation-of-motion coupled-cluster theory (based on the non-Hermitian quantum mechanics) facilitate the assignment of all major EELS features. Our simulations identified two broad and partially overlapping resonances-one of pi* and another of sigma* character-located at similar to 2.8 and 2.3 eV vertically at the equilibrium geometry of the neutral. Due to the Renner-Teller effect, the pi* resonance splits upon bending. The upper state, (2)Pi, remains linear. The lower state mixes with the sigma* configuration, giving rise to the (2)A ' resonance, which becomes strongly stabilized at bent geometries (alpha(NNO) = 134 degrees), resulting in very low adiabatic electron attachment energy. The calculations estimate the electron affinity of N2O to be0.140 eV. The (2)A ' state is predissociative, with the barrier for the N-O bond dissociation of 0.183 eV. The measured EELS feature sharp vibrational structures at low energy losses, followed by a linear (in logarithmic scale) tail extending to the maximum energy loss. The simulations attribute the sharp features at the low energy loss to the non-resonant excitations and contributions from the cold (2)Pi resonance. The tail is attributed to the vibrationally hot (2)A ' state, and its slope is determined by the excess energy available in this state.

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

2025

Kód důvěrnosti údajů

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

Název periodika

Journal of Chemical Physics

ISSN

0021-9606

e-ISSN

1089-7690

Svazek periodika

163

Číslo periodika v rámci svazku

2

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

14

Strana od-do

024120

Kód UT WoS článku

001528008300023

EID výsledku v databázi Scopus

2-s2.0-105010448958