Raynaud C, Claude T, Borel A, Amara M R, Graf A, Zaumseil J, Lauret J-S, Chassagneux Y, Voisin C
Laboratoire de Physique, École Normale Supérieure, PSL, CNRS , Université de Paris, Sorbonne Université , 75005 Paris , France.
Institute for Physical Chemistry , Heidelberg University , 69120 Heidelberg , Germany.
Nano Lett. 2019 Oct 9;19(10):7210-7216. doi: 10.1021/acs.nanolett.9b02816. Epub 2019 Sep 11.
At cryogenic temperature and at the single emitter level, the optical properties of single-wall carbon nanotubes depart drastically from that of a one-dimensional (1D) object. In fact, the (usually unintentional) localization of excitons in local potential wells leads to nearly 0D behaviors such as photon antibunching, spectral diffusion, inhomogeneous broadening, etc. Here, we present a hyperspectral imaging of this spontaneous exciton localization effect at the single nanotube level using a super-resolved optical microscopy approach. We report on the statistical distribution of the trap localization, depth, and width. We use a quasi-resonant photoluminescence excitation approach to probe the confined quantum states. Numerical simulations of the quantum states and exciton diffusion show that the excitonic states are deeply modified by the interface disorder inducing a remarkable discretization of the excitonic absorption spectrum and a quenching of the free 1D exciton absorption.
在低温和单发射体水平下,单壁碳纳米管的光学性质与一维(1D)物体的光学性质有很大不同。实际上,激子在局部势阱中的(通常是无意的)局域化会导致近乎零维的行为,如光子反聚束、光谱扩散、非均匀展宽等。在此,我们使用超分辨光学显微镜方法,展示了在单纳米管水平下这种自发激子局域化效应的高光谱成像。我们报告了陷阱局域化、深度和宽度的统计分布。我们使用准共振光致发光激发方法来探测受限量子态。量子态和激子扩散的数值模拟表明,激子态因界面无序而被深度改变,导致激子吸收光谱出现显著离散化以及自由一维激子吸收的猝灭。