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2022 Fiscal Year Final Research Report

Development and Application of Multi-Pulse Ultrafast Spectroscopy to Reveal Essential Characteristics of Reacting Molecules

Research Project

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Project/Area Number 21K18943
Research Category

Grant-in-Aid for Challenging Research (Exploratory)

Allocation TypeMulti-year Fund
Review Section Medium-sized Section 32:Physical chemistry, functional solid state chemistry, and related fields
Research InstitutionInstitute of Physical and Chemical Research

Principal Investigator

Tahara Tahei  国立研究開発法人理化学研究所, 開拓研究本部, 主任研究員 (60217164)

Co-Investigator(Kenkyū-buntansha) 松崎 維信  国立研究開発法人理化学研究所, 開拓研究本部, 研究員 (70830165)
Project Period (FY) 2021-07-09 – 2023-03-31
Keywords超高速分光 / フェムト秒 / 反応ダイナミクス / 構造不均一性 / 非調和性
Outline of Final Research Achievements

We took on the challenge of realizing ultrafast "action" spectroscopy by adding "change" pulses to traditional time-resolved spectroscopy that only uses pump and probe pulses. First, the newly developed transient two-dimensional electronic spectroscopy was performed on hydrated electrons. As a result, a spectral hole indicating inhomogeneity was clearly observed immediately after the excitation. This is the first experimental evidence of the inhomogeneous broadening of the broad absorption of hydrated electrons. We also observed the disappearance of the hole due to spectral diffusion, revealing the time scale of the structural fluctuation of hydrated electrons. Fifth-order time-domain Raman spectroscopy was also performed on myoglobin and CO-bound myoglobin, and two-dimensional spectra were obtained, but the low S/N indicates that further investigation is needed.

Free Research Field

物理化学

Academic Significance and Societal Importance of the Research Achievements

本研究で挑戦した2つの超高速分光は、いずれも世界に先駆けて我々が実現したものであり、またそこから得ることができる分子の構造不均一性と非調和性の知見は、極めて本質的でありながら未だにほとんど理解されていない。それを実行し、特に、長い間謎とされていた水和電子の不均一性の存在に対して明確な実験的な証拠を得たことには極めて高い学術的意義がある。一般に分光計測は、理学と工学、基礎研究と応用研究の違いを問わず大変広く用いられており、広範な科学・技術の基盤になっている。本研究で行った研究はその最先端をさらに進めるもので、分光計測の新しい可能性を拓くものであると言える。

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Published: 2024-01-30  

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