Swift Michael W, Efros Alexander L, Erwin Steven C
Center for Computational Materials Science, Naval Research Laboratory, Washington, DC, USA.
Nat Commun. 2024 Sep 4;15(1):7737. doi: 10.1038/s41467-024-51842-4.
Semiconductor nanoplatelets are atomically flat nanocrystals which emit light with high spectral purity at wavelengths controlled by their thickness. Despite their technological potential, efforts to further sharpen the emission lines of nanoplatelets have generally failed for unknown reasons. Here, we demonstrate theoretically that the linewidth is controlled by surface chemistry-specifically, inhomogeneities in the ligand layer on the nanoplatelet surface lead to a spatially fluctuating potential that localizes excitons. This localization leads to increased scattering and optical broadening. Importantly, localization also reduces the rate of radiative emission. Our model explains the observed linewidth and predicts that a more uniform ligand layer will sharpen the lines and increase the emission rates. These findings demonstrate that light emission from nanoplatelets can be controlled by optimizing their surface chemistry, an important advantage for their eventual use in optical technologies.
半导体纳米片是原子级平整的纳米晶体,其在由厚度控制的波长处发射具有高光谱纯度的光。尽管它们具有技术潜力,但由于未知原因,进一步锐化纳米片发射线的努力通常都失败了。在这里,我们从理论上证明,线宽由表面化学控制——具体而言,纳米片表面配体层的不均匀性会导致空间波动的势,从而使激子局域化。这种局域化会导致散射增加和光学展宽。重要的是,局域化还会降低辐射发射率。我们的模型解释了观察到的线宽,并预测更均匀的配体层将使谱线锐化并提高发射率。这些发现表明,纳米片的发光可以通过优化其表面化学来控制,这对于它们最终在光学技术中的应用是一个重要优势。