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Intramolecular Singlet Fission in Oligoacene Heterodimers

Journal Article · · Angewandte Chemie (Online)
 [1];  [1];  [1];  [1];  [2];  [1]
  1. Columbia Univ., New York, NY (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)

In this Communication we investigate singlet fission (SF) in heterodimers comprising a pentacene unit covalently bonded to another acene as we systematically vary the singlet and triplet pair energies. We find that these energies control the SF process, where dimers undergo SF provided that the resulting triplet pair energy is similar or lower in energy than the singlet state. In these systems the singlet energy is determined by the lower energy chromophore, and the rate of SF is found to be relatively independent of the driving force. However, triplet pair recombination in these heterodimers follows the energy gap law. The ability to tune the energies of these materials provides a key strategy to study and design new SF materials – an important process for third generation photovoltaics.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI ID:
1329779
Report Number(s):
BNL--112602-2016-JA; KC0403020
Journal Information:
Angewandte Chemie (Online), Journal Name: Angewandte Chemie (Online) Journal Issue: 10 Vol. 128; ISSN 1521-3757
Publisher:
German Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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Cited By (23)

A Direct Mechanism of Ultrafast Intramolecular Singlet Fission in Pentacene Dimers journal May 2016
New insights into the design of conjugated polymers for intramolecular singlet fission journal July 2018
Designing Singlet Fission Candidates from Donor-Acceptor Copolymers journal February 2020
Triplet Harvesting from Intramolecular Singlet Fission in Polytetracene journal September 2017
Liquid Crystallinity as a Self‐Assembly Motif for High‐Efficiency, Solution‐Processed, Solid‐State Singlet Fission Materials journal July 2019
Intramolecular Singlet Fission in an Antiaromatic Polycyclic Hydrocarbon journal July 2017
Revealing the Nature of Singlet Fission under the Veil of Internal Conversion journal December 2019
Intramolecular Singlet Fission in an Antiaromatic Polycyclic Hydrocarbon journal July 2017
Revealing the Nature of Singlet Fission under the Veil of Internal Conversion journal January 2020
Pentacene Dimers as a Critical Tool for the Investigation of Intramolecular Singlet Fission journal March 2018
High‐Yield Generation of Triplet Excited States by an Efficient Sequential Photoinduced Process from Energy Transfer to Singlet Fission in Pentacene‐Modified CdSe/ZnS Quantum Dots journal July 2018
Harnessing singlet exciton fission to break the Shockley–Queisser limit journal October 2017
Quintet multiexciton dynamics in singlet fission journal October 2016
Ultra-fast intramolecular singlet fission to persistent multiexcitons by molecular design journal August 2019
Picosecond timescale tracking of pentacene triplet excitons with chemical sensitivity journal June 2019
Photophysical characterization and time-resolved spectroscopy of a anthradithiophene dimer: exploring the role of conformation in singlet fission journal January 2017
Effects of aromatic substituents on the electronic structure and excited state energy levels of diketopyrrolopyrrole derivatives for singlet fission journal January 2018
Color-tunable upconversion emission from a twisted intramolecular charge-transfer state of anthracene dimers via triplet–triplet annihilation journal January 2019
Striking the right balance of intermolecular coupling for high-efficiency singlet fission journal January 2018
Annihilator dimers enhance triplet fusion upconversion journal January 2019
Singlet fission in a hexacene dimer: energetics dictate dynamics journal January 2020
Morphology independent triplet formation in pentalene films: Singlet fission as the triplet formation mechanism journal September 2019
Weakly coupled triplet pair states probed by quantum beating in delayed fluorescence in tetracene crystals journal October 2019

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