title: Intramolecular Singlet Fission in Oligoacene Heterodimers.
abstract: 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.
authors.affiliation: Department of Chemistry, Columbia University, 3000 Broadway, MC3124, New York, NY, 10027, USA.
authors.forename: Samuel N
authors.initials: SN
authors.lastname: Sanders
authors.affiliation: Department of Chemistry, Columbia University, 3000 Broadway, MC3124, New York, NY, 10027, USA.
authors.forename: Elango
authors.initials: E
authors.lastname: Kumarasamy
authors.affiliation: Department of Chemistry, Columbia University, 3000 Broadway, MC3124, New York, NY, 10027, USA.
authors.forename: Andrew B
authors.initials: AB
authors.lastname: Pun
authors.affiliation: Department of Chemistry, Columbia University, 3000 Broadway, MC3124, New York, NY, 10027, USA.
authors.forename: Michael L
authors.initials: ML
authors.lastname: Steigerwald
authors.affiliation: Center for Functional Nanomaterials, Brookhaven National Laboratory, Building 735, Upton, NY, 11973, USA.
authors.forename: Matthew Y
authors.initials: MY
authors.lastname: Sfeir
authors.affiliation: Department of Chemistry, Columbia University, 3000 Broadway, MC3124, New York, NY, 10027, USA. lcampos@columbia.edu.
authors.forename: Luis M
authors.initials: LM
authors.lastname: Campos
keywords: conjugated materials; heterodimers; organic electronics; photophysics; singlet fission