Center for Integrated Nanotechnologies, Materials Physics and Applications Division, ‡Theoretical Division, and §Physical Chemistry and Applied Spectroscopy Group, Chemistry Division, Los Alamos National Laboratory , Los Alamos, New Mexico 87545, United States.
ACS Nano. 2014 Oct 28;8(10):10613-20. doi: 10.1021/nn504138m. Epub 2014 Sep 30.
We study temporal evolution of photoluminescence (PL) spectra from individual single-walled carbon nanotubes (SWCNTs) at cryogenic and room temperatures. Sublinear and superlinear correlations between fluctuating PL spectral positions and line widths are observed at cryogenic and room temperatures, respectively. We develop a simple model to explain these two different spectral diffusion behaviors in the framework of quantum-confined Stark effect (QCSE) caused by surface charges trapped in the vicinity of SWCNTs. We show that the wave function properties of excitons, namely, localization at cryogenic temperature and delocalization at room temperature, play a critical role in defining sub- and superlinear correlations. Room temperature PL spectral positions and line widths of SWCNTs coupled to gold dimer nanoantennas on the other hand exhibit sublinear correlations, indicating that excitonic emission mainly originates from nanometer range regions and excitons appear to be localized. Our numerical simulations show that such apparent localization of excitons results from plasmonic confinement of excitation and an enhancement of decay rates in the gap of the dimer nanoantennas.
我们研究了单个单壁碳纳米管(SWCNT)在低温和室温下的光致发光(PL)光谱的时间演化。在低温和室温下,分别观察到PL 光谱位置和线宽的波动之间的次线性和超线性相关性。我们在由 SWCNT 附近捕获的表面电荷引起的量子限制斯塔克效应(QCSE)框架内,开发了一个简单的模型来解释这两种不同的光谱扩散行为。我们表明,激子的波函数性质,即在低温下的局域化和在室温下的离域化,在定义次线性和超线性相关性方面起着关键作用。另一方面,与金二聚体纳米天线耦合的 SWCNT 的室温 PL 光谱位置和线宽表现出次线性相关性,表明激子发射主要源自纳米级区域,并且激子似乎局域化。我们的数值模拟表明,这种激子的明显局域化是由于激子的等离子体限制和二聚体纳米天线间隙中衰减率的增强所致。