Solution-based intramolecular singlet fission in cross-conjugated pentacene dimers

Zirzlmeier J, Casillas R, Reddy R, Coto PB, Lehnherr D, Chernick E, Papadopoulos I, Thoss M, Tykwinski R, Guldi DM (2016)

Publication Type: Journal article

Publication year: 2016

Journal

Nanoscale Royal Society of Chemistry

Book Volume: 8

Pages Range: 10113-10123

Journal Issue: 19

DOI: 10.1039/C6NR02493A

Abstract

We show unambiguous and compelling evidence by means of pump-probe experiments, which are complemented by calculations using ab initio multireference perturbation theory, for intramolecular singlet fission (SF) within two synthetically tailored pentacene dimers with cross-conjugation, namely XC1 and XC2. The two pentacene dimers differ in terms of electronic interactions as evidenced by perturbation of the ground state absorption spectra stemming from stronger through-bond contributions in XC1 as confirmed by theory. Multiwavelength analysis, on one hand, and global analysis, on the other hand, confirm that the rapid singlet excited state decay and triplet excited state growth relate to SF. SF rate constants and quantum yields increase with solvent polarity. For example, XC2 reveals triplet quantum yields and rate constants as high as 162 $±$ 10% and (0.7 $±$ 0.1) $\times$ 1012 s-1, respectively, in room temperature solutions.

Authors with CRIS profile

Johannes Zirzlmeier Lehrstuhl für Physikalische Chemie I Ruben Casillas Pacheco Lehrstuhl für Physikalische Chemie I Pedro Brana Coto Professur für Theoretische Physik mit dem Schwerpunkt Molekulare Materialien Erin Chernick Sonderforschungsbereich 953/3 Synthetische Kohlenstoffallotrope Ilias Papadopoulos Lehrstuhl für Physikalische Chemie I Michael Thoss Professur für Theoretische Physik mit dem Schwerpunkt Molekulare Materialien Rik Tykwinski Lehrstuhl für Organische Chemie I Dirk Michael Guldi Lehrstuhl für Physikalische Chemie I

Additional Organisation(s)

Exzellenz-Cluster Engineering of Advanced Materials

Involved external institutions

University of Alberta CA Canada (CA)

How to cite

APA:

Zirzlmeier, J., Casillas, R., Reddy, R., Coto, P.B., Lehnherr, D., Chernick, E.,... Guldi, D.M. (2016). Solution-based intramolecular singlet fission in cross-conjugated pentacene dimers. Nanoscale, 8(19), 10113-10123. https://dx.doi.org/10.1039/C6NR02493A

MLA:

Zirzlmeier, Johannes, et al. "Solution-based intramolecular singlet fission in cross-conjugated pentacene dimers." Nanoscale 8.19 (2016): 10113-10123.

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