Quantum confinement and ultrafast dephasing dynamics in InP nanocrystals

Abstract

The electronic level structure and dephasing dynamics of InP nanocrystals in the strong quantum-confinement regime are studied by two complementary techniques: nanosecond hole burning and the femtosecond three-pulse photon echo. Hole burning yields the homogeneous electronic level structure while the photon echo allows the extraction of the linewidth of the band-gap transition. The congestion of electronic levels observed close to the band-edge transition in the hole-burning experiments gives rise to a pulse-width-limited initial decay in the photon-echo signal. The level structure is calculated and assigned using a model which includes valence-band mixing. The homogeneous linewidth of the band-edge transition is approximately 5 meV at 20 K and is broadened considerably at higher temperatures. The temperature dependence of the linewidth is consistent with an intrinsic dephasing mechanism of coupling to low-frequency acoustic modes mediated by the deformation potential. Quantum-confinement effects in III-V semiconductor InP are compared to those of the prototypical CdSe II-VI semiconductor nanocrystal system.