Molecular movie of ultrafast coherent rotational dynamics
Evangelos T. Karamatskos, Sebastian Raabe, Terry Mullins, Andrea Trabattoni, Philipp Stammer, Gildas Goldsztejn, Rasmus R. Johansen, Karol Długołęcki, Henrik St… 展开作者
Evangelos T. Karamatskos, Sebastian Raabe, Terry Mullins, Andrea Trabattoni, Philipp Stammer, Gildas Goldsztejn, Rasmus R. Johansen, Karol Długołęcki, Henrik Stapelfeldt, Marc. J. J. Vrakking, Sebastian Trippel, Arnaud Rouzée, Jochen Küpper
Recording molecular movies on ultrafast timescales has been a longstanding goal for unravelling detailed information about molecular dynamics. We present the direct experimental recording of very-high-resolution and -fidelity molecular movies over more than one-and-a-half periods of the laser-induced rotational dynamics of carbonylsulfide (OCS) molecules. Utilising the combination of single-quantum-state selection and an optimised two-pulse sequence to create a tailored rotational wavepacket, an unprecedented degree of field-free alignment, $\langle \cos^{2}{θ_{2D}}\rangle=0.96$ ($\langle \cos^{2}θ\rangle=0.94$) was achieved, exceeding the theoretical limit for single-pulse alignment. The very rich experimentally observed quantum dynamics is fully recovered by the angular probability distribution obtained from solutions of the time-dependent Schrödinger equation with parameters refined against the experiment. The populations and phases of rotational states in the retrieved time-dependent three-dimensional wavepacket rationalised the observed very high degree of alignment.
Ultrafast X-ray Spectroscopy of Intersystem Crossing in Hexafluoroacetylacetone: Chromophore Photophysics and Spectral Changes in the Face of Electron Withdrawing Groups
