Periodic Reporting for period 1 - DTIMM (Dynamic Through-Space Interactions Driven by Molecular Motors)
Okres sprawozdawczy: 2024-01-01 do 2025-12-31
Distinct from the well-established paradigm of through-bond conjugation, through-space interaction (TSI) has emerged as a fundamental electronic phenomenon. Nevertheless, leveraging TSI for the rational design of organic functional materials remains a significant challenge, hindered by difficulties in conformational control and the absence of clear structure–property relationships.
This project seeks to systematically investigate the photophysical and electronic properties, dynamic behaviors, and operational mechanisms of noncovalent TSI, utilizing light-driven molecular motors as a versatile platform. The work is structured around three core objectives: i) Developing a novel class of molecular motors powered by noncovalent conformational locks; ii) Achieving dynamic through-space charge transfer and multistate luminescent switching systems; iii) Constructing single-molecule junctions featuring tunable through-space interactions. These objectives are pursued through an integrated experimental and theoretical methodology, bridging multidisciplinary techniques and knowledge domains. Furthermore, the project advances theoretical studies on excited-state processes in molecular motors and photoclick reactions, thereby strengthening the photochemical research portfolio of the host group.
Beyond scientific outputs, the project incorporates a comprehensive pathway to impact. Results are disseminated through peer-reviewed publications, international conferences, and social media, ensuring engagement with both academic and non-academic audiences. Building on the complementary expertise of the researcher and host institution, a two-way knowledge transfer is facilitated through tailored training, public outreach activities, and career development initiatives, enhancing the researcher’s professional trajectory and long-term employability within the European and worldwide research landscape.
This project seeks to systematically investigate the photophysical and electronic properties, dynamic behaviors, and operational mechanisms of noncovalent TSI, utilizing light-driven molecular motors as a versatile platform. The work is structured around three core objectives: i) Developing a novel class of molecular motors powered by noncovalent conformational locks; ii) Achieving dynamic through-space charge transfer and multistate luminescent switching systems; iii) Constructing single-molecule junctions featuring tunable through-space interactions. These objectives are pursued through an integrated experimental and theoretical methodology, bridging multidisciplinary techniques and knowledge domains. Furthermore, the project advances theoretical studies on excited-state processes in molecular motors and photoclick reactions, thereby strengthening the photochemical research portfolio of the host group.
Beyond scientific outputs, the project incorporates a comprehensive pathway to impact. Results are disseminated through peer-reviewed publications, international conferences, and social media, ensuring engagement with both academic and non-academic audiences. Building on the complementary expertise of the researcher and host institution, a two-way knowledge transfer is facilitated through tailored training, public outreach activities, and career development initiatives, enhancing the researcher’s professional trajectory and long-term employability within the European and worldwide research landscape.
Following the proposed research plan, a series of experimental and theoretical investigations were conducted, yielding significant scientific progress. The main work performed, and key achievements are summarized as follows: i) Synthesis and photophysical study of a pyrene-functionalized molecular motor: A novel artificial molecular motor incorporating pyrene luminogens was successfully synthesized. This system exhibits efficient photoisomerization and displays distinct fluorescent signals in its single-molecule versus aggregated states. This tunable emission is attributed to modulations in through-space interactions (TSI) between the pyrene units upon conformational change. ii) Development of a molecular motor with an intramolecular noncovalent lock: A new molecular motor architecture was designed and synthesized, featuring an intramolecular noncovalent interaction that serves as a conformational lock. This design provides a precise means to control molecular geometry and probe the influence of constrained TSI on motor function. iii) Theoretical analysis of photophysical processes: A detailed theoretical study was performed to elucidate the electronic factors governing photoisomerization and photoluminescence in artificial molecular motors. Analyses included computations of electron-cloud redistribution, charge-transfer strength, and molecular skeleton reorganization during photoexcitation, establishing clear structure–property relationships. iv) Mechanistic investigation of a photoclick reaction: The excited-state mechanism of the photoclick reaction involving 9,10-phenanthrenequinone was elucidated, with a focus on how electronic effects dictate the reaction pathway and efficiency.
Main achievements: the primary scientific output to date is an open-access publication in the Journal of the American Chemical Society (J. Am. Chem. Soc. 2025, 147, 35903). Additionally, two further manuscripts are currently in preparation, detailing the other core findings of the project. In addition to promoting the research communications and career development, the researcher also attended several international conferences, including ArtMoMa_Final Conference Groningen, The 18th International Symposium on Macrocyclic and Supramolecular Chemistry, Molecular Nanotour Symposium 2024, as well as ACS Fall 2024. In recognition of the research excellence, the researcher was awarded the ACS PHYS Young Investigator Award (American Chemical Society) during the project period, which is a global accolade granted to only four researchers worldwide each year.
Main achievements: the primary scientific output to date is an open-access publication in the Journal of the American Chemical Society (J. Am. Chem. Soc. 2025, 147, 35903). Additionally, two further manuscripts are currently in preparation, detailing the other core findings of the project. In addition to promoting the research communications and career development, the researcher also attended several international conferences, including ArtMoMa_Final Conference Groningen, The 18th International Symposium on Macrocyclic and Supramolecular Chemistry, Molecular Nanotour Symposium 2024, as well as ACS Fall 2024. In recognition of the research excellence, the researcher was awarded the ACS PHYS Young Investigator Award (American Chemical Society) during the project period, which is a global accolade granted to only four researchers worldwide each year.
This project has successfully established a proof-of-concept for manipulating photophysical properties and molecular conformation through dynamic through-space interactions (TSI). Key results include the development of two novel light-driven molecular motor systems with stimulus-responsive fluorescence and a locked conformation, and two mechanistic understandings of photophysical processes of molecular motors and photoclick reactions of 9,10-phenanthrenequinone, supported by a foundational theoretical framework.
Potential impacts and key needs for further uptake are: i) for further research: extending the molecular library and integrating motors into functional assemblies or prototype devices (e.g. sensors, optical switches). ii) for commercialisation & IPR: patenting the novel molecular designs is essential to attract funding and enable eventual commercial application. iii) for collaboration & internationalization: partnering with experts in device engineering, single-molecule physics, or industrial chemistry will accelerate translational development. iv) for standardization: as the field advances, contributing to standardized performance metrics will support broader adoption and reliability. These steps will help transition the fundamental advances made here into applicable technologies with long-term scientific and societal impact.
Potential impacts and key needs for further uptake are: i) for further research: extending the molecular library and integrating motors into functional assemblies or prototype devices (e.g. sensors, optical switches). ii) for commercialisation & IPR: patenting the novel molecular designs is essential to attract funding and enable eventual commercial application. iii) for collaboration & internationalization: partnering with experts in device engineering, single-molecule physics, or industrial chemistry will accelerate translational development. iv) for standardization: as the field advances, contributing to standardized performance metrics will support broader adoption and reliability. These steps will help transition the fundamental advances made here into applicable technologies with long-term scientific and societal impact.