Quantum Dots as an Active Reservoir for Longer Effective Lifetimes in GaAs Bulk

IF 5.3 2区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY ACS Applied Nano Materials Pub Date : 2024-07-04 DOI:10.1021/acsanm.4c01041
G. M. Jacobsen, H. Bragança, Yu. I. Mazur, M. E. Ware, G. J. Salamo, B. L. Liang, G. E. Marques, V. Lopez-Richard, M. D. Teodoro
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Abstract

AlInAs/AlGaAs quantum dots (QDs) have emerged as excellent emitters across the visible spectral range, showcasing highly tunable electronic properties through variations in composition and size. This versatility allows for diverse band alignments within the same system. In this study, we present compelling evidence for the coexistence of type-I indirect and direct emissions from QDs, supported by comprehensive analyses of their photoluminescence responses to excitation power, temperature, and time, along with band structure calculations. The high-density QD system exhibits signs of lateral coupling, facilitated by carrier transfer between dots, modulated by energy barriers and recombination times. Additionally, we can unequivocally prove that the QDs act as carrier reservoirs that progressively feed optically active states in the bulk GaAs at low temperatures─an attractive prospect for hot-carrier photovoltaics. Above certain temperatures, the bulk system reverts to the anticipated predominantly radiative recombination dynamics. Our theoretical framework, accounting for the coexistence of QD specimens with varying recombination times, successfully elucidates the optical response at different temperatures, emphasizing the pivotal role of QD excitation in enhancing the effective lifetime of carriers in the bulk.

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量子点作为活性储层,可延长砷化镓晶体的有效寿命
AlInAs/AlGaAs 量子点(QDs)已成为可见光谱范围内的优秀发光体,通过成分和尺寸的变化展现出高度可调的电子特性。这种多功能性允许在同一系统中实现不同的波段排列。在本研究中,我们通过全面分析 QD 对激发功率、温度和时间的光致发光响应以及带状结构计算,提出了 QD 同时存在 I 型间接和直接发射的有力证据。高密度 QD 系统显示出横向耦合的迹象,这种耦合是由载流子在点之间的转移促成的,并受到能量势垒和重组时间的调节。此外,我们还可以明确证明,QDs 可作为载流子贮存器,在低温条件下逐步为体砷化镓中的光学活性态提供载流子,这对于热载流子光伏技术来说是一个极具吸引力的前景。超过一定温度后,体质系统会恢复到预期的主要辐射重组动力学。我们的理论框架考虑了具有不同重组时间的 QD 试样共存的情况,成功地阐明了不同温度下的光学响应,强调了 QD 激发在提高体中载流子有效寿命方面的关键作用。
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来源期刊
CiteScore
8.30
自引率
3.40%
发文量
1601
期刊介绍: ACS Applied Nano Materials is an interdisciplinary journal publishing original research covering all aspects of engineering, chemistry, physics and biology relevant to applications of nanomaterials. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important applications of nanomaterials.
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