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NIMS Award Symposium 2026

HOME > Profile > SHIGEMITSU, Hajime

External affiliations

  • 九州大学 工学府 応用化学専攻 准教授 (NIMS連携大学院)

Research

Keywords

Supramolecular Photochemistry, Aggregation Photochemistry, Photoinduced Charge Separation, Aggregation-Induced Charge Separation (AICS), Photodynamic Therapy (PDT), Photoredox Chemistry, Radical Photochemistry, Chiral Photophysics, Circularly Polarized Luminescence (CPL), Self-Assembly Energy Conversion

Research fields: Photochemistry, Supramolecular Chemistry, Functional Molecular Materials, Photomedicine, Solar Energy Conversion My research focuses on the creation, mechanistic understanding, and application of novel photofunctions that emerge from the self assembly of organic dye molecules. In particular, I study supramolecular assemblies formed by ionic pi conjugated molecules in water, where intermolecular electronic interactions induce photoinduced charge separation and unusual excited state dynamics. When molecules assemble, new photochemical pathways can emerge that are not accessible in isolated molecules. These processes often lead to long lived charge separated states and radical reactions, resulting in new forms of photochemistry. In this context, I have proposed the concept of Aggregation Induced Charge Separation (AICS), in which charge separation is generated through molecular aggregation. My research aims to elucidate the general principles underlying this phenomenon by combining spectroscopic analysis, theoretical calculations, and molecular design. Building on these supramolecular photochemical principles, I am also developing applications in photodynamic therapy (PDT) and solar energy conversion materials. In particular, I am working on supramolecular photosensitizers capable of sustained radical generation through charge separation, which may overcome the limitations of conventional photomedicine under hypoxic conditions. More broadly, my research integrates supramolecular photochemistry with biomedical and energy related applications. By combining experimental chemistry with AI and robotic technologies for materials discovery, I aim to accelerate the development of next generation photofunctional molecular materials.

researchPicture

有機色素の分子集合や空間配置を精密に制御することで、非発光性の暗状態(Dark States)と発光状態(Bright States)の双方を活用し、新しい光機能の創出を目指しています。
左図では、水中でのイオン性色素の自己集合によって分子間電荷分離を促進し、従来は発光消光の原因と考えられてきた暗状態をラジカル光化学反応に利用する研究を示しています。これらの研究を基盤として、光触媒反応や光線力学療法(PDT)への応用を進めています。
右図では、シクロデキストリンなどのキラルな分子足場上に複数の発光団を集積し、励起状態相互作用やエキシマー形成を制御することで、高輝度の円偏光発光(CPL)を実現する研究を示しています。さらに、分子認識機能との融合によるセンシングやバイオイメージングへの展開を目指しています。

PublicationsNIMS affiliated publications since 2004.

Presentations

    Society memberships

    日本化学会, 光化学協会, シクロデキストリン学会

    Funds

    • 科学技術振興機構(JST) 戦略的創造研究推進事業 さきがけ (2026)
    • 防衛装備庁 安全保障技術研究推進制度(タイプA) (2026)
    • 日本学術振興会(JSPS) 科学研究費助成事業 基盤研究(B) (2026)
    • 文部科学省 科学研究費助成事業 学術変革領域研究(A)「π分子複雑性の追究が紡ぐ機能科学」(公募研究) (2026)
    Research Center for Macromolecules and Biomaterials
    Title

    Supramolecular Photochemistry: Engineering Excited States and Emerging Photofunctions through Molecular Assembly

    Keywords

    Supramolecular Photochemistry, Molecular Self-Assembly, Excited-State Engineering, Photoinduced Charge Separation, Aggregation-Induced Charge Separation, Photodynamic Therapy, Circularly Polarized Luminescence, Photocatalysis

    Overview

    Molecules can exhibit markedly different photophysical and photochemical properties when they assemble and interact with one another. Our research aims to create new excited states and photofunctions by precisely controlling the self-assembly and spatial arrangement of organic chromophores. A central focus is aggregation-induced charge separation (AICS), in which molecular aggregation promotes photoinduced charge separation and opens photochemical pathways that are inefficient or inaccessible in isolated molecules. By exploiting these processes, we seek to transform molecular aggregation, often regarded as detrimental to photofunctional performance, into a strategy for driving radical photochemistry. We also investigate the control of circularly polarized luminescence (CPL) through the chiral spatial organization of chromophores. By establishing fundamental principles of supramolecular excited-state engineering, we aim to develop photofunctional materials for photodynamic therapy (PDT), photocatalysis, and energy conversion.

    Novelty and originality

    Conventional design strategies for organic photofunctional materials have generally focused on suppressing aggregation-caused quenching (ACQ), which often reduces luminescence efficiency. In contrast, our research seeks to exploit aggregation-induced changes in excited-state dynamics and redirect nonemissive excited states toward productive photochemical reactions. In particular, we have demonstrated a supramolecular strategy in which the assembly of ionic organic dyes promotes intermolecular charge separation and enables Type I photosensitization through radical-generating pathways. We have also developed chiral molecular architectures in which multiple chromophores are spatially organized on scaffolds such as cyclodextrins, enabling the control of excitonic interactions and excimer formation to achieve bright circularly polarized luminescence. The originality of our approach lies in treating intermolecular interactions and three-dimensional molecular organization, rather than molecular structure alone, as fundamental design parameters for controlling excited states and generating new photofunctions.

    Details

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    Exploring New Photochemical Reactivity through Aggregation-Induced Charge Separation (AICS) and Dark-State Engineering Molecular aggregation of organic dyes generally causes luminescence quenching and excited-state energy loss. However, such nonemissive excited states, often referred to as dark states, do not necessarily represent unproductive energy dissipation. By appropriately controlling intermolecular electronic interactions, charge-separated states unique to molecular assemblies can be generated, opening new pathways for photochemical reactions. We have investigated self-assembly-induced changes in excited-state properties and radical-generating photochemical reactions in aqueous environments using ionic organic dyes, including rhodamines, cyanines, and fluoresceins. In particular, we focus on aggregation-induced charge separation (AICS), aiming to harness dark states, traditionally associated with luminescence quenching, as productive intermediates for driving photochemical reactions. In fluorescein derivatives, we demonstrated that molecular aggregation enables a switch from conventional Type II to Type I photosensitization, resulting in photodynamic therapeutic effects against cancer cells. Our current research focuses on elucidating the relationships among intermolecular interactions, assembly structures, and excited-state dynamics, with the ultimate goal of establishing the fundamental principles of Dark-State Engineering, in which the formation and reactivity of nonemissive excited states are controlled through molecular assembly.
    Emergent Photofunctions through Chromophore Organization on Chiral Molecular Scaffolds The three-dimensional spatial organization of molecules plays a crucial role in determining their absorption and emission properties. In particular, the precise organization of multiple chromophores on chiral molecular scaffolds enables control over intermolecular electronic interactions and excited-state properties, giving rise to photofunctions that are difficult to achieve with isolated molecules. We investigate the controlled organization of aromatic chromophores on chiral molecular scaffolds, including cyclodextrins, to regulate excitonic interactions and excimer formation. In particular, we have developed cyclodextrin derivatives bearing multiple pyrene units and demonstrated bright circularly polarized luminescence (CPL) through the interplay between chromophore interactions and chiral spatial organization. Our ongoing research focuses on understanding how the number, distance, orientation, and molecular dynamics of chromophores influence excited-state behavior and CPL properties, with the aim of establishing molecular design principles for precise control of photofunctions. Furthermore, by integrating chiral molecular recognition and host–guest interactions with luminescent properties, we aim to develop molecular sensing systems capable of optically detecting specific molecules and changes in their chemical environments.

    Summary

    Our research aims to create new photophysical properties and photochemical reactivity by precisely controlling the molecular assembly and spatial organization of organic chromophores and exploiting intermolecular interactions in their excited states. Our major research directions include Dark-State Engineering, which seeks to harness nonemissive excited states traditionally associated with luminescence quenching for productive photochemical reactions, and the control of luminescent properties through the precise organization of chromophores on chiral molecular scaffolds. Through these studies, we seek to establish fundamental principles governing excited-state behavior in molecular assemblies and translate these insights into applications such as photodynamic therapy (PDT), photocatalysis, and molecular sensing. By assembling and spatially organizing molecules, we aim to create unprecedented photofunctions and open new frontiers in supramolecular photochemistry.
    この機能は所内限定です。
    この機能は所内限定です。

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