Abstract
Chemical reaction dynamics in liquids and at interfaces are central themes in the materials, energy, and environmental sciences. Ultrafast photoelectron spectroscopy of liquids enables unprecedented access to the electronic dynamics of transient chemical species, providing deeper insights into nonadiabatic reaction dynamics in aqueous solutions, which are strongly coupled with solvation dynamics.
Highlights
A combination of molecular beam techniques and laser mass spectrometry led them to the celebrated discovery of C60.2 the successful marriage of molecular beam methods and laser spectroscopy in the past four decades resulted in a number of breakthroughs in gas-phase studies of molecular structures and reaction dynamics
Ultrafast spectroscopy has captured the decisive moments of chemical reactions at the transition state and at the conical intersection of potential energy surfaces,3 and crossed molecular beam scattering with laser-spectroscopic detection of products enabled clear identification of quantum mechanical (Feshbach) resonances4 in elementary bimolecular reactions
Experiments indicate that the effective attenuation length of an electron flux in liquid water is several nm in the kinetic energy region less than 20 eV, and this is sufficiently large for photoelectron spectroscopy to probe the bulk properties of aqueous solutions with large dielectric constants
Summary
The 1974 paper by Smalley et al demonstrated that the highly congested electronic spectrum of NO2 at room temperature is drastically simplified by adiabatic cooling in a supersonic jet expansion. Later, a combination of molecular beam techniques and laser mass spectrometry led them to the celebrated discovery of C60.2 the successful marriage of molecular beam methods and laser spectroscopy in the past four decades resulted in a number of breakthroughs in gas-phase studies of molecular structures and reaction dynamics. Ultrafast spectroscopy has captured the decisive moments of chemical reactions at the transition state and at the conical intersection of potential energy surfaces, and crossed molecular beam scattering with laser-spectroscopic detection of products enabled clear identification of quantum mechanical (Feshbach) resonances in elementary bimolecular reactions.. Ultrafast spectroscopy has captured the decisive moments of chemical reactions at the transition state and at the conical intersection of potential energy surfaces, and crossed molecular beam scattering with laser-spectroscopic detection of products enabled clear identification of quantum mechanical (Feshbach) resonances in elementary bimolecular reactions.5–7 These studies have extended to research in attosecond electron dynamics, cold molecular collisions, and many other new frontiers. We offer a brief overview of the current status of ultrafast photoelectron spectroscopy of aqueous solutions.
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