Development of a Time Correlation Spectroscopy for Liquid Phase Reactions using a Liquid Micro Jet in Combination with a Synchrotron Radiation

本研究的目的是为辐射损伤的产生和修复的新方面开发一种新的光谱学，它试图通过分别在气相原子和分子光谱学以及湿体系中辐射与生物分子的辐射相互作用方面弥合首席研究人员和主要合作研究人员的不同背景。我们希望通过真空中的液体微喷射结合单色同步辐射激发的电子能谱来观察生物功能分子的结构和能量状态，这些结构和能量状态是由水溶液中的水化网络确定的。这有望有助于选择性地观察分子相对于原子元素的初始(完整)结构和能量、特定原子的成键位置，以及通过分析抛射光电子的动能来与它们水合。这种电子的射出是初级辐射相互作用的位置发生弛豫到最终固定损伤的标志。通过使用质谱学和光学光谱学来确定在修复损害的过程中特别出现的中间物种。因此，在目前的工作中，我们开发了一种产生液体微喷流的技术，以保持和稳定高真空光电子能谱中的液体样品。这是通过改进微射流源和真空系统来实现的。我们还研制了反射式高分辨率飞行时间质谱仪和光电子能量分析的可见光至紫外光时间相关光谱光学探测系统。还对光电子能谱系统进行了改进，以实现高精度的测量。

The objective of the present research has been the development of a new spectroscopy for a new aspect of production and restoration of radiation damage, which has been attempted by bridging the different background of the head investigator and the main collaborating investigator in atomic and molecular spectroscopy in gas phase and the radiation interaction with bio-molecules in wet systems, respectively. We have intended the observation of the structures and the energy states of bio-functional molecules, which are determined by the hydration network surrounding them in water solution, by means of a liquid micro jet in vacuum in combination with an electron spectroscopy for chemical analysis employing a monochromatic synchrotron radiation excitation. This has been expected to facilitate the selective observation of initial (intact) structures and energies of the molecules with respect to the atomic elements, bonding site of particular atoms, and hydration with them by analyzing the kinetic energies of ejected photoelectrons. Ejection of such electrons is the signature of the site of the primary radiation interaction undergoing to relaxation to the final fixed damage. The intermediate species emerging specifically in particular time domains on the way to fixed damage are specified by the use of a mass spectrometry and an optical spectroscopy.1. Thus, in the present work, we have developed the technique of generating a liquid micro jet to retain and stabilize liquid samples for a photoelectron spectroscopy in high vacuum. This has been achieved by improving the micro jet source and vacuum system.2. We have also achieved development of both a reflectron type high-resolution time-of-flight mass spectrometer and an optical detection system in the visible to ultraviolet range for a time correlation spectroscopy with the photoelectron energy analysis. Improvement of the system of photoelectron spectroscopy for high precision measurement is also made in advance.