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Abstract
Phonon-assisted up-conversion photoluminescence can boost energy of an emission photon to be higher than that of the excitation photon by absorbing vibration energy (or phonons) of the emitter. Here, up-conversion photoluminescence power-conversion efficiency (power ratio between the emission and excitation photons) for CdSe/CdS core/shell quantum dots is observed to be beyond unity. Instead of commonly known defect-assisted up-conversion photoluminescence for colloidal quantum dots, temperature-dependent measurements and single-dot spectroscopy reveal the up-conversion photoluminescence and conventional down-conversion photoluminescence share the same electron-phonon coupled electronic states. Ultrafast spectroscopy results imply the thermalized excitons for up-conversion photoluminescence form within 200 fs, which is 100,000 times faster than the radiative recombination rate of the exciton. Results suggest that colloidal quantum dots can be exploited as efficient, stable, and cost-effective emitters for up-conversion photoluminescence in various applications.
Up-conversion photoluminescence in colloidal quantum dots is generally believed to be mediated by thermal activation from defect states. Here, the authors reveal that highly-efficient up-conversion photoluminescence instead is related to electron-phonon coupling.
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1 Zhejiang University, Key Laboratory of Excited-State Materials of Zhejiang Province, Department of Chemistry, Hangzhou, China (GRID:grid.13402.34) (ISNI:0000 0004 1759 700X)
2 Zhejiang University, Key Laboratory of Excited-State Materials of Zhejiang Province, Department of Chemistry, Hangzhou, China (GRID:grid.13402.34) (ISNI:0000 0004 1759 700X); Zhejiang University, College of Information Science and Electronic Engineering, Hangzhou, China (GRID:grid.13402.34) (ISNI:0000 0004 1759 700X)
3 Najing Technology Corporation LTD, Hangzhou, China (GRID:grid.13402.34)