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Dissecting the Triplet-State Properties and Intersystem Crossing Mechanism of the Ligand-Protected Au Superatom. | LitMetric
Icosahedral Au nanoclusters are among the most typical superatoms and are of great interest as promising building blocks for nanocluster-assembled materials. Herein, the key parameters involved in the intersystem crossing (ISC) process of [Au(dppe)Cl] (; dppe = 1,2-bis(diphenylphosphino)ethane) were characterized. Quenching experiments using aromatic compounds revealed that the T energy of is 1.63 eV. An integrative interpretation of our experimental results and the relevant literature uncovered important facts concerning the Au superatom: the ISC quantum yield is unity due to the ultrafast ISC (∼10 s), the lowest absorption band includes contributions of direct singlet-triplet transitions, and there exists a large S-T gap of 0.73 eV. To explain the efficient ISC, the El-Sayed rule was applied to the superatomic orbitals corresponding to the excited-state hole/electron distributions obtained from theoretical calculations. The strong spin-orbit coupling between the S and T-T states offers a reasonable explanation for the ultrafast ISC.
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