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%\title{Femtosecond photoexcitation dynamics of dimers solvated in helium nanodroplets: vibrational wave packets and predissociation}

\title{FEMTOSECOND PHOTOEXCITATION DYNAMICS OF DIMERS SOLVATED IN HELIUM NANODROPLETS: VIBRATIONAL WAVEPACKETS AND PREDISSOCIATION}

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\author{\underline{\FirstName W. E. \LastName ERNST},
  \FirstName M. \LastName STADLHOFER, \FirstName M. \LastName KOCH}
\address{Institut f\"ur Experimentalphysik,
Technische Universit\"at Graz,
Petersgasse 16,
8010 Graz}

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\fancyhead[C]{{\footnotesize \textit{HRMS, 28th Colloquium, Dijon, France,
  Aug. 28 - Sept. 1, 2023}}}
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\category {11,12}
\begin{document}

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\noindent
Ultrafast pump-probe photoionization experiments were conducted on dimers solvated inside liquid helium nanodroplets ($\mathrm{He_N}$) to gain insights into the influence of the quantum solvent on nuclear and electronic dynamics. 
We first present coherent vibrational wave packet dynamics of Al$_2$ inside $\mathrm{He_N}$, where coherence is preserved for tens of picoseconds, in analogy to  our previous work on In$_2$~$^[$\footnote{
\href{http://dx.doi.org/10.1103/physrevlett.124.115301}{doi:10.1103/physrevlett.124.115301},
B. Thaler, M. Meyer, P. Heim, and M. Koch,\\
Phys.~Rev.~Lett.~\textbf{124},~115301 (2020)}$^]$
.  The short revival time of $\sim30$\,ps of Al$_2$ will allow us to investigate the influence of additional solvent molecules on the wavepacket motion.
%Aluminum dimers within the nanodroplets showed vibrational coherence in the excited state, which persisted for up to 130 ps with a wavepacket revival time of 31 ps. The temporal position and amplitude of the second wavepacket revival exhibited a clear dependence on the chirp of the pump pulse. The short revival time, combined with long nuclear coherence, will allow for the investigation of the influence of additional solvated species on the wavepacket motion.

\noindent
Time-resolved photoion spectroscopy  of In$_2$ revealed the detachment of $\mathrm{InHe_N^+}$ ions from the helium droplet following probe-pulse ionization~$^[$\footnote{
\href{http://dx.doi.org/10.1039/d2cp03571e}{doi:10.1039/d2cp03571e},
M. Stadlhofer, B. Thaler and M. Koch,\\
Phys.~Chem.~Chem.~Phys.~\textbf{24},~24727-24733 (2022) }$^]$. Detection of the ion fragments, which are typically trapped inside the droplet, is enabled by electronic excitation of the ion during the ionization process.  The excess energy provides the ion fragments with sufficient kinetic energy to overcome the attractive $\mathrm{He_N}$ potential. Ion detection enables electron-ion correlation spectroscopy within liquid helium droplets, which provides deeper insight into reaction pathways, particularly in cases where significant kinetic energy is released during fragmentation.

\noindent
Time-resolved photoion spectroscopy was furthermore employed to investigate iodine molecules inside $\mathrm{He_N}$. Excitation to the bound B-state did not yield wave packet oscillation, as observed in the gas phase, but instead exhibited immediate ground-state bleach. With velocity map imaging, we observe $\mathrm{IHe_N^+}$ fragments appearing after 1~ps and remaining at least up to 150~ps.  
Comparison with A-state dissociation of gas-phase I$_2$ suggests rapid and efficient predissociation of the molecule from the B-state via droplet-mediated internal conversion.
Large velocities partially exceeding those of Coulomb explosion of gas phase iodine indicate that the fragment iodine atoms are confined within the droplet after dissociation.



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