Resonant inelastic x-ray scattering at the N2 π* resonance: Lifetime-vibrational interference, radiative electron rearrangement, and wave-function imaging

L Kjellsson,C Såthe,M Guarise,H O Karlsson,A Nicolaou,C Hague,A Pietzsch,S G Chiuzbăian,J Lüning,M Agåker,J.-E Rubensson,V Ekholm,N Jaouen

doi:10.1103/physreva.103.022812

Abstract

Resonant inelastic x-ray scattering spectra excited at the ${\ensuremath{\pi}}^{*}$-resonance of the nitrogen molecule are presented. Well-resolved vibrational excitations in the electronic ground state, and in the $3{\ensuremath{\sigma}}_{g}^{\ensuremath{-}1}1{\ensuremath{\pi}}_{g}^{1}\phantom{\rule{4pt}{0ex}}{a}^{1}{\mathrm{\ensuremath{\Pi}}}_{g}$ state are observed. The spectra are analyzed within the Kramers-Heisenberg formalism, and the importance of lifetime-vibrational interference effects is highlighted. In addition, strongly dissociative multiply excited final states populated in radiative electron rearrangement are found in the valence ionization continua. The vibrational wave functions of the core-excited state are imaged on the strongly dissociative final state potentials.

Highlights

IntroductionN2, is arguably one of the most studied molecules
Nitrogen, N2, is arguably one of the most studied molecules
It is typically used as a showcase when new techniques are introduced, and it is ubiquitous in development of soft x-ray spectroscopy. On it was the first system where vibrational resolution was demonstrated in x-ray emission spectroscopy (XES) [1] and the vibrationally resolved x-ray absorption spectrum (XAS) is often used for determining the resolving power [2,3,4] and energy calibration of monochromators at synchrotron radiation facilities

Summary

Introduction

N2, is arguably one of the most studied molecules It is typically used as a showcase when new techniques are introduced, and it is ubiquitous in development of soft x-ray spectroscopy. On it was the first system where vibrational resolution was demonstrated in x-ray emission spectroscopy (XES) [1] and the vibrationally resolved x-ray absorption spectrum (XAS) is often used for determining the resolving power [2,3,4] and energy calibration of monochromators at synchrotron radiation facilities. Methodological developments still lead to the uncovering of new states and processes in the nitrogen molecule, e.g., in connection with double-core hole excitation dynamics at synchrotrons and [5] and free-electron lasers [6].

Methods

Results

Conclusion