Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume 123, Issue 30, Pages 18638-18645Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.9b04034
Keywords
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Funding
- National Natural Science Foundation of China [11774096, 21827814, 21573074, 21872053]
- Postdoctoral Science Foundation of China [2018 M640360]
- 111 project [B12024]
- JoRISS project
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It remains unclear whether the emission center of ligand-encapsulated metal nanoclusters (MNCs) is the surface ligands or the metal core. In this paper, we simultaneously observed metal-centered and ligand-centered emissions in Ag nanoclusters. The contributions of the surface ligands and the metal core were individually investigated to understand the nature of AgNC photoemission. A new ligand synergistic emission effect was observed. The amino correlated n pi* state provides a pivot to bridge the carboxyl correlated pi pi* and n pi* states to enhance the charge transfer efficiency between different surface electronic states. Consequently, the photoluminescence quantum yields were significantly improved (similar to 1 to similar to 10%). Transient absorption studies revealed that decreasing the pH could expand the potential energy curve and generate a conical intersection. This would facilitate the charge transfer and relaxation of excited electrons via a radiative pathway, thereby enhancing the emission intensity. These new insights into the photoemission mechanisms of MNCs should stimulate additional experimental and theoretical studies and could benefit the molecular-level design of luminescent MNCs for optoelectronics and other applications.
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