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Observation of a phonon bottleneck in copper-doped colloidal quantum dots
摘要： 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 1Pe hot electrons which is more than 30-fold longer than that in same-sized, undoped dots (~0.25 picosecond).
关键词： phonon bottleneck,electron-phonon scattering,hot electrons,colloidal quantum dots,copper-doped
更新于2025-09-16 10:30:52
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Fast Electron and Slow Hole Relaxation in InP-Based Colloidal Quantum Dots
摘要： Colloidal InP-based quantum dots are a promising material for light-emitting applications as an environment friendly alternative to their Cd-containing counterparts. Especially for their use in optoelectronic devices, it is essential to understand how charge carriers relax to the emitting state after injection with excess energy and if all of them arrive at this desired state. Herein, we report on time-resolved differential transmission measurements on colloidal InP/ZnS and InP/ZnSe core/shell quantum dots. By optically exciting and probing individual transitions, we are able to distinguish between electron and hole relaxation. This in turn allows us to determine how the initial excess energy of the charge carriers affects the relaxation processes. According to the electronic level scheme, one expects a strong phonon bottleneck for electrons, while holes should relax easier as their energy levels are more closely spaced. On the contrary, we find that electrons relax faster than holes. The fast electron relaxation occurs via an efficient Auger-like electron-hole scattering mechanism. On the other hand, a small wave function overlap between core and shell states slows the hole relaxation down. Additionally, holes can be trapped at the core/shell interface leading to either slow detrapping or nonradiative recombination. Overall, these results demonstrate that it is crucial to construct devices enabling the injection of charge carriers energetically close to their emitting states in order to maximize the radiative efficiency of the system.
关键词： InP,differential transmission spectroscopy,phonon bottleneck,charge carrier relaxation,trap states,electron-hole scattering,colloidal quantum dots
更新于2025-09-11 14:15:04