论文标题
皮秒时期分辨的抗挑战测量纳米级激子运动，歼灭和真实数量的发色团
Picosecond time-resolved antibunching measures nanoscale exciton motion, annihilation, and true number of chromophores
论文作者
论文摘要
在单量子系统的荧光光子统计中，光的粒子样性质变为光子抗激素。在多颗粒系统中，激子扩散和随后的歼灭发生。这些过程还产生了光子抗挑战，但不能可靠地解释。在这里，我们开发了Picsecond Time Crasolvice Antibunching（PSTRAB），以识别和解码此类过程。我们使用PSTRAB来测量定义明确的多颗粒DNA-Origami结构上的发色团的真实数量，并精确地确定了激子之间歼灭的距离依赖性速率。此外，PSTRAB使我们能够测量介质H和J型共轭聚合物聚集体中的激子扩散。我们在激发后的不同时间区分一维的链和三维链激发子扩散，并确定依赖障碍依赖性扩散长度。我们的方法提供了一种新的晶状体，可以通过该镜头在单粒子水平上研究激子，从而使改进的激子探针（例如超亮荧光纳米颗粒）的合理设计以及用于光电设备的材料。
The particle-like nature of light becomes evident in the photon statistics of fluorescence of single quantum systems as photon antibunching. In multichromophoric systems, exciton diffusion and subsequent annihilation occurs. These processes also yield photon antibunching but cannot be interpreted reliably. Here, we develop picosecond time-resolved antibunching (psTRAB) to identify and decode such processes. We use psTRAB to measure the true number of chromophores on well-defined multichromophoric DNA-origami structures, and precisely determine the distance-dependent rates of annihilation between excitons. Further, psTRAB allows us to measure exciton diffusion in mesoscopic H- and J-type conjugated-polymer aggregates. We distinguish between one-dimensional intra-chain and three-dimensional inter-chain exciton diffusion at different times after excitation and determine the disorder-dependent diffusion lengths. Our method provides a new lens through which excitons can be studied at the single-particle level, enabling the rational design of improved excitonic probes such as ultra-bright fluorescent nanoparticles, and materials for optoelectronic devices.
