Observation of a phonon bottleneck in copper-doped colloidal quantum dots.

Wang, Lifeng; Chen, Zongwei; Liang, Guijie; Li, Yulu; Lai, Runchen; Ding, Tao; Wu, Kaifeng · Nat Commun · 2019

basic_science · Level V

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Abstract

Hot electrons can dramatically improve the efficiency of solar cells and sensitize energetically-demanding photochemical reactions. Efficient hot electron devices have been hindered by sub-picosecond intraband cooling of hot electrons in typical semiconductors via electron-phonon scattering. Semiconductor quantum dots were predicted to exhibit a "phonon bottleneck" for hot electron relaxation as their quantum-confined electrons would couple very inefficiently to phonons. However, typical cadmium selenide dots still exhibit sub-picosecond hot electron cooling, bypassing the phonon bottleneck possibly via an Auger-like process whereby the excessive energy of the hot electron is transferred to the hole. Here we demonstrate this cooling mechanism can be suppressed in copper-doped cadmium selenide colloidal quantum dots due to femtosecond hole capturing by copper-dopants. As a result, we observe a lifetime of ~8.6 picosecond for 1P<sub>e</sub> hot electrons which is more than 30-fold longer than that in same-sized, undoped dots (~0.25 picosecond).