Spin polarized electron dynamics enhance water splitting efficiency by yttrium iron garnet photoanodes: a new platform for spin selective photocatalysis.

This work presents a spectroscopic and photocatalytic comparison of water splitting using yttrium iron garnet (YFeO, YIG) and hematite (α-FeO) photoanodes. Despite similar electronic structures, YIG significantly outperforms widely studied hematite, displaying more than an order of magnitude increase in photocurrent density. Probing the charge and spin dynamics by ultrafast, surface-sensitive XUV spectroscopy reveals that the enhanced performance arises from (1) reduced polaron formation in YIG compared to hematite and (2) an intrinsic spin polarization of catalytic photocurrents in YIG.

On the electronically nonadiabatic decomposition dynamics of furazan and triazole energetic molecules.

The combined results of ab initio electronic-structure calculations, nonadiabatic molecular dynamics simulations using ab initio multiple spawning, and previous spectroscopic investigations of jet-cooled molecules provide strong evidence of a (π,σ)-mediated decomposition mechanism for the furazan and triazole energetic molecules. The importance of dissociative excited states formed by electron promotion from a π molecular orbital to a σ molecular orbital is explored for the furazan and triazole energetic molecules. Dissociative (π,σ) states of furazan and triazole energetic molecules can be populated by nonadiabatic surface jump from the (π,π) or the (n,π) state.

Sub-500 fs electronically nonadiabatic chemical dynamics of energetic molecules from the S excited state: Ab initio multiple spawning study.

Energetic materials store a large amount of chemical energy. Different ignition processes, including laser ignition and shock or compression wave, initiate the energy release process by first promoting energetic molecules to the electronically excited states. This is why a full understanding of initial steps of the chemical dynamics of energetic molecules from the excited electronic states is highly desirable.