Picosecond time-resolved photon antibunching measures nanoscale exciton motion and the true number of chromophores.

ABSTRACT: The particle-like nature of light becomes evident in the photon statistics of fluorescence from 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 to identify and decode such processes. We use this method 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, this 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

SUBMITTER: Hedley GJ 

PROVIDER: S-EPMC7910429 | biostudies-literature | 2021 Feb

REPOSITORIES: biostudies-literature