Transient Absorption Microscopy with Spatiotemporal Resolution in the “µ’s” – Microsecond and Micrometer – Reveal Heterogeneity in Carbon Nitride (CNx) Photocatalyst Particles
Sutripto Khasnabis a, Robert Godin a
a The University of British Columbia, 2036 Main Mall, Vancouver, BC, Canada
International Conference on Hybrid and Organic Photovoltaics
Proceedings of International Conference on Hybrid and Organic Photovoltaics (HOPV23)
London, United Kingdom, 2023 June 12th - 14th
Organizers: Tracey Clarke, James Durrant and Trystan Watson
Oral, Robert Godin, presentation 126
DOI: https://doi.org/10.29363/nanoge.hopv.2023.126
Publication date: 30th March 2023

Polymeric photocatalysts made of Earth-abundant elements have been extensively developed over the past decade to take advantage of their synthetic tunability.[1] Within this family, carbon nitrides (CNx) are emerging as exciting photocatalysts because of their high photocatalytic performance combined with good stability and facile synthesis. However, significant gaps remain in our knowledge of the photophysical properties of these organic polymeric materials. Determining the pathways and mechanism of photoinduced processes will greatly aid our efforts to engineer better CNx photocatalysts for solar fuel production.

Time-resolved spectroscopies, particularly transient absorption spectroscopy (TAS), enable us to determine the nature of short lived photoexcited states and determine the kinetics of competing processes. For example, our previous combined TAS and time-resolved photoluminescence (tr-PL) study of CNx provided important insight into the role of charge trapping on timescales ranging from femtoseconds to seconds.[2]

We are taking the next step to develop a full picture of the charge carrier dynamics by expanding our spectroscopic capabilities to transient absorption microscopy (TAM). Notably, our first-of-its-kind TAM system monitors the microsecond – second timescales relevant to the complex multi electron redox reactions that occur to produce solar fuels. Spatial mapping of the charge carrier dynamics on the micron scale provides novel insights into the heterogeneity in individual CNx particles. These new insights into the heterogeneity of charge carrier dynamics in CNx particles can push the field into uncovering the optimal structure and local environment in defect-rich organic semiconductors such as CNx.

This work was carried out while on the unceded and traditional territory of the Syilx People of the Okanagan Nation on the land now known as British Columbia, Canada. We are grateful for financial support from the Natural Sciences and Engineering Research Council of Canada (NSERC) and the Canada Foundation for Innovation (CFI).

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