Тип публикации: статья из журнала
Год издания: 2022
Идентификатор DOI: 10.1039/d1cp05499f
Аннотация: We study vibrationally-resolved resonant Auger (RAS) spectra of ammonia recorded in coincidence with the NH2+ fragment, which is produced in the course of dissociation either in the core-excited 1s(-1)4a1(1) intermediate state or the first spectator 3a(-2)4a1(1) final state. Correlation of the NH2+ ion flight times with electron kiПоказать полностьюnetic energies allows directly observing the Auger-Doppler dispersion for each vibrational state of the fragment. The median distribution of the kinetic energy release E-KER, derived from the coincidence data, shows three distinct branches as a function of Auger electron kinetic energy E-e: E-e + 1.75E(KER) = const for the molecular band; E-KER = const for the fragment band; and E-e + E-KER = const for the region preceding the fragment band. The deviation of the molecular band dispersion from E-e + E-KER = const is attributed to the redistribution of the available energy to the dissociation energy and excitation of the internal degrees of freedom in the molecular fragment. We found that for each vibrational line the dispersive behavior of E(KER)vs. E-e is very sensitive to the instrumental uncertainty in the determination of E-KER causing the competition between the Raman (E-KER + E-e = const) and Auger (E-e = const) dispersions: increase in the broadening of the finite kinetic energy release resolution leads to a change of the dispersion from the Raman to the Auger one. We study vibrationally-resolved resonant Auger (RAS) spectra of ammonia recorded in coincidence with the NH2+ fragment, which is produced in the course of dissociation either in the core-excited 1s-14a11 intermediate state or the first spectator 3a-24a11 final state. Correlation of the NH2+ ion flight times with electron kinetic energies allows directly observing the Auger-Doppler dispersion for each vibrational state of the fragment. The median distribution of the kinetic energy release EKER, derived from the coincidence data, shows three distinct branches as a function of Auger electron kinetic energy Ee: Ee + 1.75EKER = const for the molecular band; EKER = const for the fragment band; and Ee + EKER = const for the region preceding the fragment band. The deviation of the molecular band dispersion from Ee + EKER = const is attributed to the redistribution of the available energy to the dissociation energy and excitation of the internal degrees of freedom in the molecular fragment. We found that for each vibrational line the dispersive behavior of EKERvs. Ee is very sensitive to the instrumental uncertainty in the determination of EKER causing the competition between the Raman (EKER + Ee = const) and Auger (Ee = const) dispersions: increase in the broadening of the finite kinetic energy release resolution leads to a change of the dispersion from the Raman to the Auger one. We study vibrationally-resolved resonant Auger (RAS) spectra of ammonia recorded in coincidence with the NH2+ fragment, which is produced in the course of dissociation either in the core-excited 1s-14a11 intermediate state or the first spectator 3a-24a11 final state. Correlation of the NH2+ ion flight times with electron kinetic energies allows directly observing the Auger-Doppler dispersion for each vibrational state of the fragment. The median distribution of the kinetic energy release EKER, derived from the coincidence data, shows three distinct branches as a function of Auger electron kinetic energy Ee: Ee + 1.75EKER = const for the molecular band; EKER = const for the fragment band; and Ee + EKER = const for the region preceding the fragment band. The deviation of the molecular band dispersion from Ee + EKER = const is attributed to the redistribution of the available energy to the dissociation energy and excitation of the internal degrees of freedom in the molecular fragment. We found that for each vibrational line the dispersive behavior of EKERvs. Ee is very sensitive to the instrumental uncertainty in the determination of EKER causing the competition between the Raman (EKER + Ee = const) and Auger (Ee = const) dispersions: increase in the broadening of the finite kinetic energy release resolution leads to a change of the dispersion from the Raman to the Auger one.
Журнал: PHYSICAL CHEMISTRY CHEMICAL PHYSICS
Выпуск журнала: Vol. 24, Is. 10
Номера страниц: 5842-5854
ISSN журнала: 14639076
Место издания: CAMBRIDGE
Издатель: ROYAL SOC CHEMISTRY