Tracking Exciton Diffusion and Exciton Annihilation in Single Nanoparticles of Conjugated Polymers by Photon Correlation Spectroscopy

Schedlbauer, Jakob and Streicher, Sabrina and Forster, Michael and Scherf, Ullrich and Vogelsang, Jan and Lupton, John M. (2022) Tracking Exciton Diffusion and Exciton Annihilation in Single Nanoparticles of Conjugated Polymers by Photon Correlation Spectroscopy. ADVANCED OPTICAL MATERIALS, 10 (14): 2200092. ISSN 2195-1071,

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Abstract

A fundamental question relating to the nature of light emission and absorption in organic semiconductors is the dimension of the domain within a bulk material responsible for the interaction of light and matter. How large can a nanoparticle become to retain the quantized nature of light emission? Excitons are only a few nanometers in size, but because they diffuse in space, they probe a much larger volume than the single molecule. When excitons meet, they may decay non-radiatively by singlet-singlet or singlet-triplet annihilation (SSA or STA). Fluorescence photon statistics reveal whether single photons are emitted (photon antibunching) or arrive in randomly spaced packets (photon bunching), offering direct insight into excitonic mobility. Single multichain nanoparticles of ladder-type poly(para-phenylene) (LPPP) are examined. The effect of SSA and STA is seen in the photon antibunching and bunching, respectively, which both decrease in fidelity as the size of the nanoparticle increases. Time resolving the photon correlation measurement yields microscopic annihilation rates for SSA and STA in agreement with values obtained from bulk LPPP films. Even though triplets in LPPP are known to be highly mobile, the results show that, on the timescale of the singlet exciton lifetime, triplet diffusion is not of significance in the STA process.

Item Type: Article
Uncontrolled Keywords: ENERGY-TRANSFER; LADDER POLYMER; TRIPLET; FLUORESCENCE; CHROMOPHORES; EMISSION; RECOMBINATION; POLY(3-HEXYLTHIOPHENE); PHOSPHORESCENCE; DISSOCIATION; conjugated polymers; exciton annihilation; exciton diffusion; photon statistics; single-particle spectroscopy
Subjects: 500 Science > 530 Physics
Divisions: Physics > Institute of Experimental and Applied Physics
Physics > Institute of Experimental and Applied Physics > Chair Professor Lupton > Group John Lupton
Depositing User: Dr. Gernot Deinzer
Date Deposited: 12 Dec 2023 09:30
Last Modified: 12 Dec 2023 09:30
URI: https://pred.uni-regensburg.de/id/eprint/56998

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