Kumaki Fumitoshi, Nagasaka Masanari, Fukaya Ryo, Okano Yasuaki, Yamashita Shohei, Nozawa Shunsuke, Adachi Shin-Ichi, Adachi Jun-Ichi
Department of Materials Structure Science, School of High Energy Accelerator Science, SOKENDAI (The Graduate University for Advanced Studies), 1-1 Oho, Tsukuba, Ibaraki 305-0801, Japan.
Institute for Molecular Science, Myodaiji, Okazaki 444-8585, Japan.
J Chem Phys. 2023 Mar 14;158(10):104201. doi: 10.1063/5.0129814.
Operando time-resolved soft x-ray absorption spectroscopy (TR-SXAS) is an effective method to reveal the photochemical processes of metal complexes in solutions. In this study, we have developed the TR-SXAS measurement system for observing various photochemical reactions in solutions by the combination of laser pump pulses with soft x-ray probe pulses from the synchrotron radiation. For the evaluation of the developed TR-SXAS system, we have measured nitrogen K-edge x-ray absorption spectroscopy (XAS) spectra of aqueous iron phenanthroline solutions during a photoinduced spin transition process. The decay process of the high spin state to the low spin state in the iron complex has been obtained from the ligand side by N K-edge XAS, and the time constant is close to that obtained from the central metal side by time-resolved Fe K-edge XAS in the previous studies.
原位时间分辨软X射线吸收光谱（TR-SXAS）是揭示溶液中金属配合物光化学过程的有效方法。在本研究中，我们通过将激光泵浦脉冲与来自同步辐射的软X射线探测脉冲相结合，开发了用于观测溶液中各种光化学反应的TR-SXAS测量系统。为了评估所开发的TR-SXAS系统，我们在光致自旋转变过程中测量了水溶液中亚铁菲咯啉溶液的氮K边X射线吸收光谱（XAS）。通过N K边XAS从配体侧获得了铁配合物中高自旋态到低自旋态的衰减过程，其时间常数与先前研究中通过时间分辨Fe K边XAS从中心金属侧获得的时间常数相近。
