Microscopic descriptions of solution phase photoacid-base reactions involve the concept of “tight” contact and “loose” solvent separated reaction pairs for the elementary steps of proton transfer. Typically one has to deal with multiple distributions of complexes with possible different configurations, that makes ultrafast experiments rather involved {1]. Even when only the dynamics on the...
We establish high-harmonic generation (HHG) in liquids as a powerful ultrafast probe for tracking spatial and temporal electron dynamics on attosecond time scales. Beyond the traditional three-step model, we uncover new nonlinear features such as multi-plateau structures and bandgap modification. These findings open pathways to attosecond-scale exploration of solvation dynamics, light–matter...
The excited state dynamics of ethylene following excitation into the energetically lowest lying absorption band, nominally understood as arising from the $\pi\pi^*$ and $\pi3s$ states, have been the focus of numerous theoretical and computational studies for many decades. Here, we present new quantum dynamics computations and spectroscopic simulations that indicate the non-adiabatic population...
Pulse shaping has long been used to tailor femtosecond laser pulses for studying and controlling the fragmentation of polyatomic molecules [1, 2]. We employed 80-bit binary spectral phase functions (BPs) to reduce the search space while maintaining the ability to generate essentially any arbitrary phase [3]. Analysis of the reduced search space allowed us to gain insight into which pulse...
