# Ultrafast Dynamics And Electronic State – Lifetime Interferences In Chlorine-Containing Molecules

G Goldsztejn, T Marchenko, R Guillemin, L Journel, R K Kushawaha, R

Püttner, D Céolin, M N Piancastelli, Marielle Simon

► To cite this version:

G Goldsztejn, T Marchenko, R Guillemin, L Journel, R K Kushawaha, et al.. Ultrafast Dynamics And Electronic State – Lifetime Interferences In Chlorine-Containing Molecules. Journal of Physics: Conference Series, 2015, 635 (11), pp.112092 10.1088/1742-6596/635/11/112092 . hal-01265948

HAL Id: hal-01265948

https://hal.sorbonne-universite.fr/hal-01265948

Submitted on 1 Feb 2016

HAL is a multi-disciplinary open access
archive for the deposit and dissemination of sci-
entific research documents, whether they are pub-
lished or not. The documents may come from
teaching and research institutions in France or
abroad, or from public or private research centers.

L'archive ouverte pluridisciplinaire HAL, est
destinée au dépôt et à la diffusion de documents
scientifiques de niveau recherche, publiés ou non,
émanant des établissements d'enseignement et de
recherche français ou étrangers, des laboratoires
publics ou privés.

<figure><img src="image_1.png" /></figure>

Distributed under a Creative Commons Attribution 4.0 International License
Ultrafast Dynamics And Electronic State – Lifetime Interferences In Chlorine-Containing
Molecules

This content has been downloaded from IOPscience. Please scroll down to see the full text.

2015 J. Phys.: Conf. Ser. 635 112092

(http://iopscience.iop.org/1742-6596/635/11/112092)

View the table of contents for this issue, or go to the journal homepage for more

Download details:

IP Address: 134.157.80.136

This content was downloaded on 01/02/2016 at 16:48

Please note that terms and conditions apply.
# Ultrafast Dynamics And Electronic State - Lifetime Interferences In Chlorine-Containing Molecules

G. Goldsztejn<fnref n="1" />,<fnref n="2" />*, T. Marchenko<fnref n="1" />,<fnref n="2" />, R. Guillemin<fnref n="1" />,<fnref n="2" />, L. Journel<fnref n="1" />,<fnref n="2" />, R.K. Kushawaha<fnref n="1" />,<fnref n="2" />, R. Püttner<fnref n="3" />, D. Céolin<fnref n="4" />, M.N. Piancastelli<fnref n="1" />,<fnref n="2" />,<fnref n="5" /> and M. Simon<fnref n="1" />,<fnref n="2" />,<fnref n="4" />

**Synopsis** In order to have access to fine phenomena such as ultrafast nuclear dynamics and electronic state - lifetime interferences (ELI) at high energies (few keV), one has to rely on great experimental resolution. The new experimental HAXPES endstation at the GALAXIES beamline of the French synchrotron SOLEIL provides photons in the 2-12 keV energy range along with a total instrumental resolution below 500 meV. In this work we show experimental evidences of ultrafast nuclear dynamics and ELI on HCl and CH₃Cl excited around the Cl 1s resonance. We show also simulations that allow to disentangle the contribution of nuclear dynamics and ELI in our experimental spectra.

Ultra-fast photodissociation in chlorine-
containing molecules has been known for more than
twenty years [1,2].

While the first observations were made after
photoexcitation of the Cl L shell, the study of nu-
clear motion in these molecules has been recently
extended to deep shells by means of Resonant Ine-
lastic X-ray Scattering (RIXS) in the tender x-ray
region (2–12 keV) [3,4,5].

A new experimental station [6] dedicated to HArd X-ray PhotoElectron Spectroscopy (HAXPES), has been mounted on the GALAXIES beamline of the synchrotron SOLEIL.

Using this setup, we have studied the electronic
relaxation of HCl and CH3Cl [7] after Cl 1s excita-
tion under resonant Raman conditions, i.e. with to-
tal instrumental resolution below the natural line
width of the decay features.

In particular, we were able to observe nuclear
dynamics on the 1-femtosecond time scale using the
'core-hole clock approach' [8].

These measurements also allowed us to unravel
subtle phenomena as electronic state-lifetime

interferences, which were also observed in
RIXS [9] and in Argon using HAXPES [10].
We present a 'simple model' simulation, initial-
ly based on a theoretical model [11], which re-
produces well the electronic state-lifetime inter-
ferences in both HCl and CH3Cl.

References

[1] H. Aksela, et al 1990, Phys. Rev. A, 41 6000

[2] O. Bjorneholm et al 1997, Phys. Rev. Lett., 79 3150

[3] M. Simon et al 2006 Phys. Rev. A, 020706

[4] T. Marchenko et al 2011, J. Chem. Phys., 144308

[5] L. El Khoury et al 2012, J. Chem. Phys, 024319

[6] D. Céolin et al 2013, J. of Elect. Spectro. and Rel. Ph., 190 188

[7] M. N. Piancastelli et al 2014, J. Phys. B, 47 124031

[8] F. Gel'mukhanov et al 1999, Phys. Rep., 312 87

[9] M. Kavčič et al 2010, Phys. Rev. Lett., 105 113004

[10] D. Céolin et al.2015, Phys. Rev. A, 91 022502

[11] G. B. Armen et al 1996, Phys. Rev. A, 53 772

<footnote n="1">¹ CNRS, UMR 7614, Laboratoire de Chimie Physique-Matière et Rayonnement, F-75005, Paris, France</footnote>

<footnote n="2">² Sorbonne Universités, UPMC Univ Paris 06, UMR 7614, Laboratoire de Chimie Physique-Matière et Rayonnement, F-75005, Paris, France</footnote>

<footnote n="3">³Institut für Experimentalphysik, Freie Universität Berlin, Arnimallee 14, D-14195 Berlin, Germany</footnote>

<footnote n="4">⁴Synchrotron SOLEIL, l'Orme des Merisiers, F-91192, Gif-sur-Yvette Cedex, France</footnote>

<footnote n="5">⁵Department of Physics and Astronomy, Uppsala University, SE-75120, Uppsala, Sweden</footnote>

<footnote>* E-mail: gildas.goldsztejn@upmc.fr</footnote>