期刊
ACS NANO
卷 15, 期 4, 页码 6499-6506出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.0c09244
关键词
semiconductor nanocrystals; lead-halide perovskites; homogeneous line broadening; multidimensional coherent spectroscopy; electron-phonon coupling; excitation-induced dephasing
类别
资金
- Department of Energy [DE-SC0015782]
- Brazilian National Council for Scientific and Technological Development (CNPq)
- FAPESP [2019/22576-8, 2018/15574-6]
- LNNano/CNPEM/MCTIC
- U.S. Department of Energy (DOE) [DE-SC0015782] Funding Source: U.S. Department of Energy (DOE)
Using multidimensional coherent spectroscopy, it was found that the line broadening mechanisms of perovskite nanoplatelets depend on platelet geometry, with decreasing thickness resulting in reduced line widths. Additionally, homogeneously broadened exciton resonances were observed in two-layer, but not necessarily three-layer, nanoplatelets at room temperature.
Perovskite nanoplatelets possess extremely narrow absorption and emission line widths, which are crucial characteristics for many optical applications. However, their underlying intrinsic and extrinsic line-broadening mechanisms are poorly understood. Here, we apply multidimensional coherent spectroscopy to determine the homogeneous line broadening of colloidal perovskite nanoplatelet ensembles. We demonstrate a dependence of not only their intrinsic line widths but also of various broadening mechanisms on platelet geometry. We find that decreasing nanoplatelet thickness by a single monolayer results in a 2-fold reduction of the inhomogeneous line width and a 3-fold reduction of the intrinsic homogeneous line width to the sub-millielectronvolts regime. In addition, our measurements suggest homogeneously broadened exciton resonances in two-layer (but not necessarily three-layer) nanoplatelets at room-temperature.
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