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Vibronic Dynamics of Photodissociating ICN from Simulations of Ultrafast X-Ray Absorption Spectroscopy
2020, Morzan, Uriel N., Videla, Pablo E., Soley, Micheline B., Nibbering, Erik T.J., Batista, Victor S.
Ultrafast UV-pump/soft-X-ray-probe spectroscopy is a subject of great interest since it can provide detailed information about dynamical photochemical processes with ultrafast resolution and atomic specificity. Here, we focus on the photodissociation of ICN in the 1Π1 excited state, with emphasis on the transient response in the soft-X-ray spectral region as described by the ab initio spectral lineshape averaged over the nuclear wavepacket probability density. We find that the carbon K-edge spectral region reveals a rich transient response that provides direct insights into the dynamics of frontier orbitals during the I−CN bond cleavage process. The simulated UV-pump/soft-X-ray-probe spectra exhibit detailed dynamical information, including a time-domain signature for coherent vibration associated with the photogenerated CN fragment. © 2020 The Authors. Published by Wiley-VCH GmbH
Filamentary pulse self-compression : the impact of the cell windows
2011, Brée, Carsten, Demircan, Ayhan, Bethge, Jens, Nibbering, Erik T.J., Skupin, Stefan, Bergé, Luc, Steinmeyer, Günter
Self-compression of multi-millijoule laser pulses during filamentary propagation is usually explained by the interplay of self-focusing and defocusing effects, causing a substantial concentration of energy on the axis of the propagating optical pulse. Recently, it has been argued that cell windows may play a decisive role in the self-compression mechanism. As such windows have to be used for media other than air their presence is often unavoidable, yet they present a sudden non-adiabatic change in dispersion and nonlinearity that should lead to a destruction of the temporal and spatial integrity of the light bullets generated in the self-compression mechanism. We now experimentally prove that there is in fact a self-healing mechanism that helps to overcome the potentially destructive consequences of the cell windows. We show in two carefully conducted experiments that the cell window position decisively influences activation or inhibition of the self-healing mechanism. A comparison with a windowless cell shows that presence of this mechanism is an important prerequisite for the exploitation of self-compression effects in windowed cells filled with inert gases.