Stangl, Thomas and Wilhelm, Philipp and Remmerssen, Klaas and Hoeger, Sigurd and Vogelsang, Jan and Lupton, John M. (2015) Mesoscopic quantum emitters from deterministic aggregates of conjugated polymers. PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 112 (41). E5560-E5566. ISSN 0027-8424,
Full text not available from this repository. (Request a copy)Abstract
An appealing definition of the term "molecule" arises from consideration of the nature of fluorescence, with discrete molecular entities emitting a stream of single photons. We address the question of how large a molecular object may become by growing deterministic aggregates from single conjugated polymer chains. Even particles containing dozens of individual chains still behave as single quantum emitters due to efficient excitation energy transfer, whereas the brightness is raised due to the increased absorption cross-section of the suprastructure. Excitation energy can delocalize between individual polymer chromophores in these aggregates by both coherent and incoherent coupling, which are differentiated by their distinct spectroscopic fingerprints. Coherent coupling is identified by a 10-fold increase in excited-state lifetime and a corresponding spectral red shift. Exciton quenching due to incoherent FRET becomes more significant as aggregate size increases, resulting in single-aggregate emission characterized by strong blinking. This mesoscale approach allows us to identify intermolecular interactions which do not exist in isolated chains and are inaccessible in bulk films where they are present but masked by disorder.
| Item Type: | Article |
|---|---|
| Uncontrolled Keywords: | SINGLE-MOLECULE; ENERGY-TRANSFER; BICHROMOPHORIC MOLECULES; ROOM-TEMPERATURE; FLUORESCENCE; CHROMOPHORES; LUMINESCENCE; SPECTROSCOPY; PHOTOPHYSICS; MACROCYCLES; photophysics; single-molecule spectroscopy; interchromophoric coupling; structure-property relations; organic electronics |
| Subjects: | 500 Science > 530 Physics |
| Divisions: | Physics > Institute of Experimental and Applied Physics > Chair Professor Lupton > Group John Lupton |
| Depositing User: | Dr. Gernot Deinzer |
| Date Deposited: | 13 May 2019 12:28 |
| Last Modified: | 13 May 2019 12:28 |
| URI: | https://pred.uni-regensburg.de/id/eprint/4622 |
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