Emerging Design Principles for Enhanced Solar Energy Utilization with Singlet Fission

Gish, Melissa K.; Pace, Natalie A.; Rumbles, Garry; Johnson, Justin C.

doi:10.1021/acs.jpcc.8b10876

Title: Emerging Design Principles for Enhanced Solar Energy Utilization with Singlet Fission

Journal Article · 28 January 2019 · Journal of Physical Chemistry. C

DOI: https://doi.org/10.1021/acs.jpcc.8b10876 · OSTI ID:1496846

Gish, Melissa K. ^[1];

^[2];

^[1]

National Renewable Energy Lab. (NREL), Golden, CO (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)

Singlet fission (SF), the generation of two triplet excitons per the absorption of one photon, is a promising strategy for increasing the efficiency of solar cells beyond the theoretical Shockley-Queisser limit of 34%. Upon photon absorption by a SF molecule, the initially created singlet excited state (S1) interacts with a neighboring chromophore and is first transformed into a triplet pair (TT), which can be subsequently separated into independent triplet excitons (2T1). These independent triplet excitons can be harvested through triplet charge extraction or triplet energy transfer to an acceptor. Research on SF systems has revealed rates and efficiencies of triplet formation and triplet pair decorrelation that are strongly dependent on interchromophore coupling, which is dictated by molecular structure and the resulting geometrical arrangement of chromophores adopted in covalent (e.g., dimers) and noncovalent (e.g., films and crystals) systems. Incorporation of SF materials into realistic device architectures introduces a host of new challenges to consider regarding the efficient extraction of triplets generated through SF. In this Feature Article, we review our work that has led to some degree of understanding and control of inter- and intramolecular SF rates placed in the context of solar energy harvesting architectures, including dye-sensitized solar cells, conjugated polymer films, and ligand-exchanged quantum dots. We emphasize the importance of understanding and manipulating interactions between SF molecules with each other and with the charge or energy collectors across an interface in order to strike a kinetic balance that leads to efficient utilization of triplet excitons.

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Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1496846

Report Number(s):: NREL/JA--5900-72782

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 7 Vol. 123; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Striking the right balance of intermolecular coupling for high-efficiency singlet fission Pensack, Ryan D.; Tilley, Andrew J.; Grieco, Christopher Chemical Science, Vol. 9, Issue 29 https://doi.org/10.1039/C8SC00293B	journal	January 2018
The exciton dynamics in tetracene thin films Tayebjee, Murad J. Y.; Clady, Raphaël G. C. R.; Schmidt, Timothy W. Physical Chemistry Chemical Physics, Vol. 15, Issue 35 https://doi.org/10.1039/c3cp52609g	journal	January 2013
Solar conversion efficiency of photovoltaic and photoelectrolysis cells with carrier multiplication absorbers Hanna, M. C.; Nozik, A. J. Journal of Applied Physics, Vol. 100, Issue 7 https://doi.org/10.1063/1.2356795	journal	October 2006
Excited state dynamics in solid and monomeric tetracene: The roles of superradiance and exciton fission Burdett, Jonathan J.; Müller, Astrid M.; Gosztola, David The Journal of Chemical Physics, Vol. 133, Issue 14 https://doi.org/10.1063/1.3495764	journal	October 2010
The dependence of singlet exciton relaxation on excitation density and temperature in polycrystalline tetracene thin films: Kinetic evidence for a dark intermediate state and implications for singlet fission Burdett, Jonathan J.; Gosztola, David; Bardeen, Christopher J. The Journal of Chemical Physics, Vol. 135, Issue 21 https://doi.org/10.1063/1.3664630	journal	December 2011
Ultrafast dynamics of excitons in tetracene single crystals Birech, Zephania; Schwoerer, Markus; Schmeiler, Teresa The Journal of Chemical Physics, Vol. 140, Issue 11 https://doi.org/10.1063/1.4867696	journal	March 2014
Efficient singlet exciton fission in pentacene prepared from a soluble precursor Tabachnyk, Maxim; Karani, Arfa H.; Broch, Katharina APL Materials, Vol. 4, Issue 11 https://doi.org/10.1063/1.4968518	journal	November 2016
Singlet fission in pentacene dimers Zirzlmeier, Johannes; Lehnherr, Dan; Coto, Pedro B. Proceedings of the National Academy of Sciences, Vol. 112, Issue 17 https://doi.org/10.1073/pnas.1422436112	journal	April 2015
Multiple exciton generation in quantum dots versus singlet fission in molecular chromophores for solar photon conversion Beard, Matthew C.; Johnson, Justin C.; Luther, Joseph M. Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 373, Issue 2044 https://doi.org/10.1098/rsta.2014.0412	journal	June 2015
Ultrafast singlet and triplet dynamics in microcrystalline pentacene films Marciniak, Henning; Pugliesi, Igor; Nickel, Bert Physical Review B, Vol. 79, Issue 23 https://doi.org/10.1103/PhysRevB.79.235318	journal	June 2009
Enhanced Triplet Formation in Polycrystalline Tetracene Films by Femtosecond Optical-Pulse Shaping Grumstrup, Erik M.; Johnson, Justin C.; Damrauer, Niels H. Physical Review Letters, Vol. 105, Issue 25 https://doi.org/10.1103/PhysRevLett.105.257403	journal	December 2010
Origins of Singlet Fission in Solid Pentacene from an ab initio Green’s Function Approach Refaely-Abramson, Sivan; da Jornada, Felipe H.; Louie, Steven G. Physical Review Letters, Vol. 119, Issue 26 https://doi.org/10.1103/PhysRevLett.119.267401	journal	December 2017
Ultrafast Exciton Relaxation in Microcrystalline Pentacene Films Marciniak, H.; Fiebig, M.; Huth, M. Physical Review Letters, Vol. 99, Issue 17 https://doi.org/10.1103/PhysRevLett.99.176402	journal	October 2007
Direct observation of triplet energy transfer from semiconductor nanocrystals Mongin, C.; Garakyaraghi, S.; Razgoniaeva, N. Science, Vol. 351, Issue 6271 https://doi.org/10.1126/science.aad6378	journal	January 2016
Recent Advances in Singlet Fission Smith, Millicent B.; Michl, Josef Annual Review of Physical Chemistry, Vol. 64, Issue 1 https://doi.org/10.1146/annurev-physchem-040412-110130	journal	April 2013

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Modulating the Electronic and Solid‐State Structure of Organic Semiconductors by Site‐Specific Substitution: The Case of Tetrafluoropentacenes Geiger, Thomas; Schundelmeier, Simon; Hummel, Thorsten Chemistry – A European Journal, Vol. 26, Issue 15 https://doi.org/10.1002/chem.201905843	journal	March 2020
Lessons from intramolecular singlet fission with covalently bound chromophores Korovina, Nadezhda V.; Pompetti, Nicholas F.; Johnson, Justin C. The Journal of Chemical Physics, Vol. 152, Issue 4 https://doi.org/10.1063/1.5135307	journal	January 2020

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