P band intermediate state (PBIS) tailors photoluminescence emission at confined nanoscale interface

Autor: Kun Zhang, Songqiu Yang, Fang Huang, Bing-Qian Shan, Peng Wu, Bo Peng, En-Hui Yuan, Tai-Qun Yang
Rok vydání: 2019
Předmět:
Zdroj: Communications Chemistry, Vol 2, Iss 1, Pp 1-11 (2019)
ISSN: 2399-3669
DOI: 10.1038/s42004-019-0233-1
Popis: The availability of a range of excited states has endowed low dimensional quantum nanostructures with interesting luminescence properties. However, the origin of photoluminescence emission is still not fully understood, which has limited its practical application. Here we judiciously manipulate the delicate surface ligand interactions at the nanoscale interface of a single metal nanocluster, the superlattice, and mesoporous materials. The resulting interplay of various noncovalent interactions leads to a precise modulation of emission colors and quantum yield. A new p-band state, resulting from the strong overlapping of p orbitals of the heteroatoms (O, N, and S) bearing on the targeting ligands though space interactions, is identified as a dark state to activate the triplet state of the surface aggregated chromophores. The UV-Visible spectra calculated by time-dependent density functional theory (TD-DFT) are in quantitative agreement with the experimental adsorption spectra. The energy level of the p-band center is very sensitive to the local proximity ligand chromophores at heterogeneous interfaces. The basic principles behind the optoelectronic properties of metal nanoclusters are still not fully understood. Here the authors manipulate the surface ligand interactions on single metal nanoclusters, within self-assembled superlattices, and in confined nanopores to achieve precise modulation of emission colors and quantum yields.
Databáze: OpenAIRE