Origin of Two Larmor Frequencies in the Coherent Spin Dynamics of Colloidal CdSe Quantum Dots Revealed by Controlled Charging

Abstract

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.

arXiv comment35 pages, 16 figures

References in corpus (7)

• Quantum Computation with Quantum Dots
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• Spin dynamics in semiconductor nanocrystals
• Spin coherence of a two-dimensional electron gas induced by resonant excitation of trions and excitons in CdTe/(Cd,Mg)Te quantum wells
• Effect of the Surface on the Electron Quantum Size Levels and Electron g-Factor in Spherical Semiconductor Nanocrystals
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Cited by in corpus (2)

• Effective Landé factors of electrons and holes in lead chalcogenide nanocrystals
• Electron, hole and exciton effective g-factors in semiconductor nanocrystals