玻璃基质中 CuCl 纳米晶内载流子的 Landé g 因子与自旋动力学
Landé g-factors and spin dynamics of charge carriers in CuCl nanocrystals in a glass matrix
AI总结：
该研究结合多种磁光光谱与六带价带理论，测量并建模玻璃基质中不同尺寸 CuCl 纳米晶的载流子 g 因子、激子跃迁及自旋动力学。
摘要：
本文通过实验和理论研究了在玻璃基质中结晶、尺寸不同（半径从 1.8 nm 到 28 nm）的 CuCl 半导体纳米晶（NCs）中受限载流子的自旋性质。利用光致发光、自旋翻转拉曼散射、时间分辨法拉第椭圆率以及时间分辨差分透射技术，在 1.6–120 K 温度范围、最高 8 T 的磁场下进行测量，获得了关于 Landé g 因子以及布居和自旋动力学的全面信息。自旋信号来自受限电子，其 g 因子接近 2，并随 NC 尺寸减小（即电子受限能增加）而表现出微弱上升。为描述 CuCl NCs 中 Z3 和 Z1,2 激子能量的尺寸依赖性，我们在六带价带模型内重新审视了球形 NCs 中激子受限的整体理论。理论上证明，Z1,2 能量跃迁随半径减小而更强地增加，可归因于激子中强重空穴–轻空穴混合所导致的激发激子态的强吸收。通过比较计算与实验得到的激子跃迁尺寸依赖性，估算了同时描述激子和空穴动能的六带哈密顿量参数。本文还建立了一个理论模型，用于描述价带具有负自旋轨道分裂的半导体球形 NCs 中受限电子和空穴的尺寸依赖 Landé g 因子。
英文摘要：
The spin properties of charge carriers confined in CuCl semiconductor nanocrystals (NCs) of different sizes (radius from 1.8 nm up to 28 nm) crystallized in a glass matrix are studied experimentally and theoretically. By means of photoluminescence, spin-flip Raman scattering, time-resolved Faraday ellipticity, and time-resolved differential transmission performed at temperatures in the range of $1.6 - 120$ K at magnetic fields up to 8 T, comprehensive information on the Landé $g$-factors as well as the population and spin dynamics is received. The spin signals are contributed by confined electrons with a $g$-factor close to 2, which shows a weak increase with decreasing NC size, i.e. increasing electron confinement energy. We revisit the theory of exciton confinement as a whole in spherical NCs within the six-band valence band model in order to describe the size dependence of the $Z_3$ and $Z_{1,2}$ exciton energies in CuCl NCs. We demonstrate theoretically that the stronger increase of the $Z_{1,2}$ energy transitions with decreasing radius can be explained by the strong absorption from the excited exciton state caused by strong heavy hole-light hole mixing in the exciton. The parameters of the six-band Hamiltonian describing both the exciton and hole kinetic energies are estimated from the comparison of the calculated and experimental size dependences of the exciton transitions. A theoretical model of the size-dependent Landé $g$-factors for electron and hole confined in spherical NCs of semiconductors with negative spin-orbit splitting of the valence band is developed.
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