Center for Nanoscale Materials, Argonne National Laboratory , Argonne, Illinois 60439, United States.
Department of Chemistry and James Franck Institute, University of Chicago , Chicago, Illinois 60637, United States.
ACS Nano. 2017 Sep 26;11(9):9119-9127. doi: 10.1021/acsnano.7b03943. Epub 2017 Sep 5.
Quasi-two-dimensional nanoplatelets (NPLs) possess fundamentally different excitonic properties from zero-dimensional quantum dots. We study lateral size-dependent photon emission statistics and carrier dynamics of individual NPLs using second-order photon correlation (g(τ)) spectroscopy and photoluminescence (PL) intensity-dependent lifetime analysis. Room-temperature radiative lifetimes of NPLs can be derived from maximum PL intensity periods in PL time traces. It first decreases with NPL lateral size and then stays constant, deviating from the electric dipole approximation. Analysis of the PL time traces further reveals that the single exciton quantum yield in NPLs decreases with NPL lateral size and increases with protecting shell thickness, indicating the importance of surface passivation on NPL emission quality. Second-order photon correlation (g(τ)) studies of single NPLs show that the biexciton quantum yield is strongly dependent on the lateral size and single exciton quantum yield of the NPLs. In large NPLs with unity single exciton quantum yield, the corresponding biexciton quantum yield can reach unity. These findings reveal that by careful growth control and core-shell material engineering, NPLs can be of great potential for light amplification and integrated quantum photonic applications.
准二维纳米板(NPL)具有与零维量子点根本不同的激子特性。我们使用二阶光子相关(g(τ))光谱和光致发光(PL)强度相关寿命分析来研究单个 NPL 的横向尺寸依赖性光子发射统计和载流子动力学。通过 PL 时间轨迹中的最大 PL 强度周期可以得出 NPL 的室温辐射寿命。它首先随 NPL 横向尺寸减小,然后保持恒定,偏离电偶极近似。对 PL 时间轨迹的进一步分析表明,NPL 中的单激子量子产率随 NPL 横向尺寸减小而减小,并随保护壳厚度增加而增加,表明表面钝化对 NPL 发射质量的重要性。单个 NPL 的二阶光子相关(g(τ))研究表明,双激子量子产率强烈依赖于 NPL 的横向尺寸和单激子量子产率。在具有单位单激子量子产率的大 NPL 中,相应的双激子量子产率可以达到 1。这些发现表明,通过仔细的生长控制和核壳材料工程,NPL 具有很大的潜力用于光放大和集成量子光子应用。