Abstract
We present a setup combining a liquid flatjet sample delivery and a MHz laser system for time-resolved soft X-ray absorption measurements of liquid samples at the high brilliance undulator beamline UE52-SGM at Bessy II yielding unprecedented statistics in this spectral range. We demonstrate that the efficient detection of transient absorption changes in transmission mode enables the identification of photoexcited species in dilute samples. With iron(II)-trisbipyridine in aqueous solution as a benchmark system, we present absorption measurements at various edges in the soft X-ray regime. In combination with the wavelength tunability of the laser system, the set-up opens up opportunities to study the photochemistry of many systems at low concentrations, relevant to materials sciences, chemistry, and biology.
Highlights
More.5,22–31 Recent advances in liquid jet technology have enabled the possibility of forming liquid sheets with thicknesses small enough to allow for remaining transmission of incident light in the percentage range at soft X-ray photon energies.32 It has been shown that the principle of colliding two regular round jets abides the vacuum demands of X-ray spectroscopy methods and provides a complete sample substitution between laser pulses operated at a MHz repetition rate
We present a setup combining a liquid flatjet sample delivery and a MHz laser system for time-resolved soft X-ray absorption measurements of liquid samples at the high brilliance undulator beamline UE52-SGM at Bessy II yielding unprecedented statistics in this spectral range
We demonstrate that the efficient detection of transient absorption changes in transmission mode enables the identification of photoexcited species in dilute samples
Summary
More. Recent advances in liquid jet technology have enabled the possibility of forming liquid sheets with thicknesses small enough to allow for remaining transmission of incident light in the percentage range at soft X-ray photon energies. It has been shown that the principle of colliding two regular round jets abides the vacuum demands of X-ray spectroscopy methods and provides a complete sample substitution between laser pulses operated at a MHz repetition rate. We report on the unique combination of a flatjet sample delivery system with a laser-pump soft X-ray-probe setup yielding high signal-to-noise ratios (S/N) and a temporal resolution on the order of of 50 ps, located at the synchrotron BESSY II (Berlin, Germany). We present time-resolved NEXAFS data on iron(II)-trisbipyridine 1⁄2FeðbpyÞ23þ in aqueous solution, where the inter-system-crossing processes following a photo-excitation have been subject to various studies employing a wide range of spectroscopic methods, including X-ray absorption measurements at the ligand and metal center.. As all excitations induced within this study are at least partly of metal-to-ligand charge-transfer (MLCT) character and result in quintet formation within the 50 ps time resolution, the wavelength tunability of the laser system can be demonstrated. The results of our measurements highlight the excellent S/N achievable with the presented setup, thereby giving leeway to study the photochemistry of dilute systems down to sample concentrations of a few millimoles per liter
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