Abstract
The recent development of liquid jet and liquid leaf sample delivery systems allows for accurate measurements of soft X-ray absorption spectra in transmission mode of solutes in a liquid environment. As this type of measurement becomes increasingly accessible, there is a strong need for reliable theoretical methods for assisting in the interpretation of the experimental data. Coupled cluster methods have been extensively developed over the past decade to simulate X-ray absorption in the gas phase. Their performance for solvated species, on the contrary, remains largely unexplored. Here, we investigate the current state of the art of coupled cluster modeling of nitrogen K-edge X-ray absorption of aqueous ammonia and ammonium based on quantum mechanics/molecular mechanics, where both the level of coupled cluster calculations and polarizable embedding are scrutinized. The results are compared to existing experimental data as well as simulations based on transition potential density functional theory.
Highlights
The recent development of liquid jet and liquid leaf sample delivery systems allows for accurate measurements of soft X-ray absorption spectra in transmission mode of solutes in a liquid environment
Knowledge of how the electronic structure of solutions is affected by hydration interactions has been gained through photoelectron spectroscopy and X-ray spectroscopy.[1−4] X-ray absorption (XA) spectroscopy[2,5,6] is very sensitive to hydration, in particular hydrogen bonding, because the underlying core-excited states often involve extended unoccupied orbitals that are very sensitive to slight geometric changes
Because X-ray spectroscopy reaches the core levels, the photon energy of the incident X-rays can be tuned to specific element edges to give element selectivity, and the local electronic structure of a solute can be probed in a complex environment
Summary
The recent development of liquid jet and liquid leaf sample delivery systems allows for accurate measurements of soft X-ray absorption spectra in transmission mode of solutes in a liquid environment. We will investigate whether the shortcomings of the transition potential DFT (TP-DFT) methods in the description of the post-edge region of the nitrogen K-edge spectra of the solutes can be overcome.[13]
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