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arXiv 2602.02064cond-mat.mes-hall
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半导体量子点中激子-声子耦合的原子论方法

Atomistic Approach to Exciton-Phonon Couplings in Semiconductor Quantum Dots

TU Dortmund(多特蒙德工业大学);Julius-Maximilians-Universität Würzburg(维尔茨堡朱利叶斯-马克西米利安大学)

Yasser Saleem, Moritz Cygorek

AI总结:

提出全原子论方法计算半导体量子点中激子-声子耦合,结合紧束缚模型与组态相互作用,揭示真实几何和原子波函数导致的高能偏差,并应用于模拟脉冲驱动量子点的发射亮度。

摘要:

我们提出了一种全原子论方法来处理半导体量子点中的激子-声子耦合,该方法将微观电子结构计算与非马尔可夫开放量子系统动力学联系起来。以嵌入InP矩阵中的InAsP量子点为例,我们使用从头参数化的紧束缚模型计算单粒子态,然后通过组态相互作用方法获得中性激子、双激子和带电三子的关联多体波函数。利用这些关联态,我们计算了激子-声子耦合矩阵元。将不同激子复合物的声子谱密度与广泛使用的解析超欧姆形式进行比较,揭示了由真实量子点几何和原子波函数引起的高能偏差,而组态混合仅起次要作用。此外,我们提取的辐射寿命与实验测量值相当。作为直接应用,我们模拟了脉冲驱动量子点的发射亮度,并证明与解析模型相比,原子论导出的谱密度显著拓宽了高效非共振激发区域。所提出的框架为模拟半导体量子点中的非马尔可夫开放量子动力学提供了一条几乎无参数路径。

英文摘要:

We present a fully atomistic approach to exciton-phonon coupling in semiconductor quantum dots that bridges microscopic electronic-structure calculations with non-Markovian open-quantum-system dynamics. On the example of an InAsP quantum dot embedded in an InP matrix, we compute single-particle states using an ab initio-parametrized tight-binding model, then obtain correlated many-body wave functions of neutral excitons, biexcitons, and charged trions via the configuration-interaction method. Using these correlated states, we compute the exciton-phonon coupling matrix elements. The resulting phonon spectral densities for different excitonic complexes are compared with the widely used analytical super-Ohmic form and reveal deviations at higher energies originating from the realistic dot geometry and atomistic wave functions, whereas configuration mixing is found to play only a minor role. Furthermore, we extract radiative lifetimes comparable to values experimentally measured. As a direct application, we simulate the emission brightness of a pulsed-driven quantum dot and demonstrate that the atomistically derived spectral density substantially broadens the region of efficient off-resonant excitation compared to the analytical model. The presented framework provides a nearly parameter-free route to simulate the non-Markovian open quantum dynamics in semiconductor quantum dots.

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