4.8 Article

Extracting Kinetics and Thermodynamics of Molecules without Heavy Atoms via Time-Resolved Solvent Scattering Signals

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JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 14, 期 13, 页码 3103-3110

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AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.3c00041

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Time-resolved X-ray liquidography (TRXL) is a powerful technique for studying the structural dynamics of small molecules and macromolecules in liquid solutions. However, it has limited sensitivity for small molecules containing light atoms only, making the signal from solvent molecules dominate. This study presents an alternative approach using solvent temperature change to detect the dynamics of photoinduced reactions, allowing the identification of intermediates and reaction pathways in small molecules without heavy atoms.
Time-resolved X-ray liquidography (TRXL) has emerged as a powerful technique for studying the structural dynamics of small molecules and macromolecules in liquid solutions. However, TRXL has limited sensitivity for small molecules containing light atoms only, whose signal has lower contrast compared with the signal from solvent molecules. Here, we present an alternative approach to bypass this limitation by detecting the change in solvent temperature resulting from a photoinduced reaction. Specifically, we analyzed the heat dynamics of TRXL data obtained from p-hydroxyphenacyl diethyl phosphate (HPDP). This analysis enabled us to experimentally determine the number of intermediates and their respective enthalpy changes, which can be compared to theoretical enthalpies to identify the intermediates. This work demonstrates that TRXL can be used to uncover the kinetics and reaction pathways for small molecules without heavy atoms even if the scattering signal from the solute molecules is buried under the strong solvent scattering signal.

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