Heterobinuclear unit light absorbers consisting of chemically dissimilar transition metals can serve as light absorbers for nanoscale artificial photosystems. TiOCo and ZrOCo units on silica nanoparticles were coupled with 2,2’-bipyridine (bipy) as a luminescent electron acceptor, with TiOCo observed as a negative control. The synthesis steps were confirmed using FT-IR and the geometries of the heterobinuclear unit-bipy diads were modeled using DFT. The particles were pressed into pellets and then placed into a home-built 3D printed gas cell. Time-correlated single photon counting (TCSPC) and time-resolved emission spectroscopy (TRES) data were collected under argon and oxygen atmospheres to measure the relaxation of the excited state. The quenching of emission in the presence of oxygen supports that the long-lived excited state of the ZrOCo-bipy system is due to a change in spin state.

Time-resolved photoluminescence spectroscopy of charge transfer states in ZrOCo and TiOCo heterobinuclear units

ACS Spring 2022

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