Auger Recombination Lifetime Scaling for Type I and Quasi-Type II Core/Shell Quantum Dots.,The Journal of Physical Chemistry Letters

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Auger Recombination Lifetime Scaling for Type I and Quasi-Type II Core/Shell Quantum Dots.
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2020-06-08 , DOI: 10.1021/acs.jpclett.0c01460
John P Philbin ₁ , Eran Rabani _{1,

2,

3}

Affiliation

Having already achieved near-unity quantum yields, with promising properties for light-emitting diode, lasing, and charge separation applications, colloidal core/shell quantum dots have great technological potential. The shell thickness and band alignment of the shell and core materials are known to influence the efficiency of these devices. In many such applications, improving the efficiency requires a deep understanding of multiexcitonic states. Herein, we elucidate the shell thickness and band alignment dependencies of the biexciton Auger recombination lifetime for quasi-type II CdSe/CdS and type I CdSe/ZnS core/shell quantum dots. We find that the biexciton Auger recombination lifetime increases with the total nanocrystal volume for quasi-type II CdSe/CdS core/shell quantum dots and is independent of the shell thickness for type I CdSe/ZnS core/shell quantum dots. To perform these calculations and compute Auger recombination lifetimes, we developed a low-scaling approach based on the stochastic resolution of identity. The numerical approach provided a framework for studying the scaling of the biexciton Auger recombination lifetimes in terms of the shell thickness dependencies of the exciton radii, Coulomb couplings, and density of final states in quasi-type II CdSe/CdS and type I CdSe/ZnS core/shell quantum dots.

中文翻译：

I型和准II型核/壳量子点的俄歇复合寿命标度。

胶体核/壳量子点已经实现了近统一的量子产率，并在发光二极管，激光和电荷分离应用方面具有令人鼓舞的特性，具有巨大的技术潜力。已知壳和芯材料的壳厚度和带取向会影响这些装置的效率。在许多此类应用中，提高效率需要深入了解多激子态。在本文中，我们阐明了准II型CdSe / CdS和I CdSe / ZnS核/壳量子点的双激子俄歇复合寿命的壳厚度和能带排列依赖性。我们发现准准II CdSe / CdS核/壳量子点的双激子俄歇复合寿命随总纳米晶体体积的增加而增加，并且与I型CdSe / ZnS核/壳量子点的壳厚度无关。为了执行这些计算并计算俄歇复合寿命，我们基于身份的随机分辨率开发了一种低尺度方法。数值方法提供了一个框架，用于研究准激子IId CdSe / CdS和Id CdSe / ZnS中激子半径的壳厚度依赖性，库仑耦合以及最终态密度，从而研究了双激子俄歇复合寿命的尺度。核/壳量子点。我们基于身份的随机解析开发了一种低规模的方法。数值方法提供了一个框架，用于研究准激子II CdSe / CdS和I CdSe / ZnS的激子半径的壳厚度依赖性，库仑耦合以及最终态的密度，从而研究了双激子俄歇复合寿命的尺度。核/壳量子点。我们基于身份的随机解析开发了一种低规模的方法。数值方法提供了一个框架，用于研究准激子II CdSe / CdS和I CdSe / ZnS的激子半径的壳厚度依赖性，库仑耦合以及最终态的密度，从而研究了双激子俄歇复合寿命的尺度。核/壳量子点。

更新日期：2020-07-02

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