Resonance Raman intensity analysis of photoactive metal-organic frameworks

Author:

Brennan Joe1ORCID,Choi Tae Hoon2ORCID,Soilis Zoe M.3ORCID,Rosi Nathaniel L.23ORCID,Johnson J. Karl2ORCID,Frontiera Renee1ORCID

Affiliation:

1. Department of Chemistry, University of Minnesota 1 , Minneapolis, Minnesota 55455, USA

2. Department of Chemical and Petroleum Engineering, University of Pittsburgh 2 , Pittsburgh, Pennsylvania 15260, USA

3. Department of Chemistry, University of Pittsburgh 3 , Pittsburgh, Pennsylvania 15261, USA

Abstract

Metal-organic frameworks (MOFs) are promising candidate materials for photo-driven processes. Their crystalline and tunable structure makes them well-suited for placing photoactive molecules at controlled distances and orientations that support processes such as light harvesting and photocatalysis. In order to optimize their performance, it is important to understand how these molecules evolve shortly after photoexcitation. Here, we use resonance Raman intensity analysis (RRIA) to quantify the excited state nuclear distortions of four modified UiO-68 MOFs. We find that stretching vibrations localized on the central ring within the terphenyl linker are most distorted upon interaction with light. We use a combined computational and experimental approach to create a picture of the early excited state structure of the MOFs upon photoactivation. Overall, we show that RRIA is an effective method to probe the excited state structure of photoactive MOFs and can guide the synthesis and optimization of photoactive designs.

Funder

Defense Threat Reduction Agency

National Science Foundation

Publisher

AIP Publishing

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