期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 10, 期 13, 页码 3681-3687出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.9b01534
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资金
- National Key Research and Development Program of China [2018YFA0306303]
- Deutsche Forschungsgemeinschaft [ICRC TRR 160]
- National Natural Science Foundation of China [11374099, 11474097, 11727810, 61720106009]
- Science and Technology Commission of Shanghai Municipality [19ZR1414500, 16520721200]
- 111 project of China [B12024]
Coherent spin dynamics in colloidal CdSe quantum dots (QDs) typically show two spin components with different Larmor frequencies, whose origin is an open question. We exploit the photocharging approach to identify their origin and find that surface states play a key role in the appearance of the spin signals. By controlling the photocharging with electron or hole acceptors, we show that the specific spin component can be enhanced by the choice of acceptor type. In core/shell CdSe/ZnS QDs, the spin signals are significantly weaker. Our results exclude the neutral exciton as the spin origin and suggest that both Larmor frequencies are related to the coherent spin precession of electrons in photocharged QDs. The lower frequency is due to the electron confined in the middle of the QD, and the higher frequency to the electron additionally localized in the vicinity of the surface.
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