TY - JOUR
T1 - Femtosecond photoexcitation dynamics inside a quantum solvent
AU - Thaler, Bernhard
AU - Ranftl, Sascha
AU - Heim, Pascal
AU - Cesnik, Stefan
AU - Treiber, Leonhard
AU - Meyer, Ralf
AU - Hauser, Andreas W.
AU - Ernst, Wolfgang E.
AU - Koch, Markus
PY - 2018/12/1
Y1 - 2018/12/1
N2 - The observation of chemical reactions on the time scale of the motion of electrons and nuclei has been made possible by lasers with ever shortened pulse lengths. Superfluid helium represents a special solvent that permits the synthesis of novel classes of molecules that have eluded dynamical studies so far. However, photoexcitation inside this quantum solvent triggers a pronounced response of the solvation shell, which is not well understood. Here, we present a mechanistic description of the solvent response to photoexcitation of indium (In) dopant atoms inside helium nanodroplets (HeN), obtained from femtosecond pump–probe spectroscopy and time-dependent density functional theory simulations. For the In–HeN system, part of the excited state electronic energy leads to expansion of the solvation shell within 600 fs, initiating a collective shell oscillation with a period of about 30 ps. These coupled electronic and nuclear dynamics will be superimposed on intrinsic photoinduced processes of molecular systems inside helium droplets.
AB - The observation of chemical reactions on the time scale of the motion of electrons and nuclei has been made possible by lasers with ever shortened pulse lengths. Superfluid helium represents a special solvent that permits the synthesis of novel classes of molecules that have eluded dynamical studies so far. However, photoexcitation inside this quantum solvent triggers a pronounced response of the solvation shell, which is not well understood. Here, we present a mechanistic description of the solvent response to photoexcitation of indium (In) dopant atoms inside helium nanodroplets (HeN), obtained from femtosecond pump–probe spectroscopy and time-dependent density functional theory simulations. For the In–HeN system, part of the excited state electronic energy leads to expansion of the solvation shell within 600 fs, initiating a collective shell oscillation with a period of about 30 ps. These coupled electronic and nuclear dynamics will be superimposed on intrinsic photoinduced processes of molecular systems inside helium droplets.
UR - http://www.scopus.com/inward/record.url?scp=85054087841&partnerID=8YFLogxK
U2 - 10.1038/s41467-018-06413-9
DO - 10.1038/s41467-018-06413-9
M3 - Article
C2 - 30275442
AN - SCOPUS:85054087841
SN - 2041-1723
VL - 9
JO - Nature Communications
JF - Nature Communications
IS - 1
M1 - 4006
ER -