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Bifurcation of Excited-State Population Leads to Anti-Kasha Luminescence in a Disulphide-Decorated Organometallic Rhenium Photosensitiser

Title	Bifurcation of Excited-State Population Leads to Anti-Kasha Luminescence in a Disulphide-Decorated Organometallic Rhenium Photosensitiser
Authors	Julia Franz, Manuel Oelschlegel, J. Patrick Zobel, Shao-An Hua, Jan-Hendrik Borter, Lucius Schmid, Giacomo Morselli, Oliver S. Wenger, Dirk Schwarzer, Franc Meyer, Leticia González
Magazine	Journal of the American Chemical Society
Date	04/10/2024
DOI	10.1021/jacs.4c00548
Introduction	This study investigates a rhenium diimine photosensitiser featuring a disulphide unit on a bipyridine ligand, revealing anti-Kasha luminescence. Utilising steady-state and ultrafast spectroscopy paired with nonadiabatic dynamics simulations, the research details the excited-state dynamics. Post intersystem crossing, the complex transitions to two triplet states: a (S–Sbpy 4,4)-ligand-centred excited state (3LC) at lower energy and a metal-to-(bpy)-ligand charge transfer (3MLCT) state at higher energy with 90% and 10% yields, respectively. The 3LC state excites the disulphide group into the antibonding σ* orbital, elongating the S–S bond. Notably, the higher-lying 3MLCT state shows luminescence with a 270 ns lifetime, indicative of anti-Kasha behaviour. This finding suggests an energy barrier ≥ 0.6 eV or minimal electronic coupling, inhibiting reaction towards the 3LC state once the population is in the 3MLCT state. This work exemplifies the complex excited-state dynamics of transition-metal photosensitisers, decoded through experimental and computational methods. Disulphide functionalisation is proposed as a novel strategy for exploiting excess energy for potential electron or energy transfer reactions.
Quote	Julia Franz, Manuel Oelschlegel and J. Patrick Zobel et al. Bifurcation of Excited-State Population Leads to Anti-Kasha Luminescence in a Disulfide-Decorated Organometallic Rhenium Photosensitiser. J. Am. Chem. Soc. 2024. Vol. 146(16):11272-11288. DOI: 10.1021/jacs.4c00548
Element	Sulfur (S)
Materials	Chemical Compounds
Industry	Research & Laboratory

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