Sun Weiwei, Krajewska Chantalle J, Kaplan Alexander E K, Šverko Tara, Berkinsky David B, Ginterseder Matthias, Utzat Hendrik, Bawendi Moungi G
Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United States.
Nano Lett. 2023 Apr 12;23(7):2615-2622. doi: 10.1021/acs.nanolett.2c04895. Epub 2023 Mar 16.
Cesium lead halide perovskite nanocrystals (PNCs) have emerged as a potential next-generation single quantum emitter (QE) material for quantum optics and quantum information science. Optical dephasing processes at cryogenic temperatures are critical to the quality of a QE, making a mechanistic understanding of coherence losses of fundamental interest. We use photon-correlation Fourier spectroscopy (PCFS) to obtain a lower bound to the optical coherence times of single PNCs as a function of temperature. We find that 20 nm CsPbBr PNCs emit nearly exclusively into a narrow zero-phonon line from 4 to 13 K. Remarkably, no spectral diffusion is observed at time scales of 10 μs to 5 ms. Our results suggest that exciton dephasing in this temperature range is dominated by elastic scattering from phonon modes with characteristic frequencies of 1-3 meV, while inelastic scattering is minimal due to weak exciton-phonon coupling.
卤化铯铅钙钛矿纳米晶体(PNCs)已成为量子光学和量子信息科学中一种潜在的下一代单量子发射体(QE)材料。低温下的光学去相过程对量子发射体的质量至关重要,因此对相干损耗的机理理解具有根本意义。我们使用光子相关傅里叶光谱(PCFS)来获得单个PNCs的光学相干时间下限作为温度的函数。我们发现,20 nm的CsPbBr PNCs在4至13 K时几乎完全发射到一条狭窄的零声子线中。值得注意的是,在10 μs至5 ms的时间尺度上未观察到光谱扩散。我们的结果表明,在此温度范围内,激子去相主要由特征频率为1 - 3 meV的声子模式的弹性散射主导,而非弹性散射由于激子 - 声子耦合较弱而最小。