@article{209499b1f769470582e758ac8e289b7b,
title = "Tuning Triplet-Pair Separation versus Relaxation Using a Diamond Anvil Cell",
abstract = "A tradeoff exists between triplet-pair separation versus relaxation that can limit the ability to utilize singlet fission for enhancing solar cell efficiency beyond the Shockley-Queisser limit. Here, we show that this tradeoff can be avoided in crystalline environments by studying a functionalized pentacene compressed in a diamond anvil cell. We demonstrate, using ultrafast transient absorption spectroscopy, that there is a “sweet spot” where the rate of triplet-pair separation can be accelerated by nearly an order of magnitude without causing fast excited state relaxation. X-ray diffraction and computational modeling allow us to quantify the corresponding increase of intermolecular coupling. Our findings suggest that increased coupling enhances excited state relaxation but that crystalline environments can suppress these relaxation processes in pentacene derivatives. The combination of these effects leads to the sweet spot and informs efforts to enhance triplet-pair separation rates in amorphous systems such as polymers.",
author = "Doucette, {Grayson S.} and Huang, {Haw Tyng} and Munro, {Jason M.} and Munson, {Kyle T.} and Changyong Park and Anthony, {John E.} and Timothy Strobel and Ismaila Dabo and Badding, {John V.} and Asbury, {John B.}",
note = "Funding Information: G.S.D. and J.B.A thank the U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences for support of this research through grant DE-SC0019349. K.T.M. is grateful for support from the National Science Foundation Graduate Research Fellowship Program under grant no. DGE-1255832. J.B.A. thanks Ryan D. Pensack and Christopher Grieco for helpful discussions. Any opinions, findings, and conclusions or recommendations expressed in this material are those of the author(s) and do not necessarily reflect the views of the National Science Foundation. T.S. gratefully acknowledges U.S. Army Research Laboratory under grant no. W911NF-17-1-0604. J.B. thanks salary support for H.T.-H. provided by DARPA under grant no. W31P4Q-13-1-0005. I.D. acknowledges support from the Soltis faculty support award and the Ralph E. Powe junior faculty award from Oak Ridge Associated Universities. J.E.A. thanks the National Science Foundation (CMMI-1255494) for supporting semiconductor synthesis. Portions of this work were performed at HPCAT (Sector 16), Advanced Photon Source (APS), Argonne National Laboratory. HPCAT operations are supported by DOE-NNSA's Office of Experimental Sciences. The Advanced Photon Source is a U.S. DOE Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under contract no. DE-AC02-06CH11357. Conceptualization, J.B.A. G.S.D. and H.-T.H.; Methodology, J.B.A. and G.S.D.; Validation, J.B.A. G.S.D. and H.-T.H.; Formal Analysis, J.B.A. G.S.D. H.-T.H. and J.M.M.; Writing – Original Draft, J.B.A. and G.S.D. Writing – Review and Editing, J.B.A. G.S.D. H.-T.H. J.M.M. K.T.M. C.P. T.S. and I.D.; Funding Acquisition, J.B.A.; Supervision, J.B.A. J.B.A. owns equity in Magnitude Instruments, which has an interest in this project. His ownership in this company has been reviewed by the Pennsylvania State University's Individual Conflict of Interest Committee and is currently being managed by the University. Funding Information: G.S.D. and J.B.A thank the U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences for support of this research through grant DE-SC0019349 . K.T.M. is grateful for support from the National Science Foundation Graduate Research Fellowship Program under grant no. DGE-1255832 . J.B.A. thanks Ryan D. Pensack and Christopher Grieco for helpful discussions. Any opinions, findings, and conclusions or recommendations expressed in this material are those of the author(s) and do not necessarily reflect the views of the National Science Foundation. T.S. gratefully acknowledges U.S. Army Research Laboratory under grant no. W911NF-17-1-0604 . J.B. thanks salary support for H.T.-H. provided by DARPA under grant no. W31P4Q-13-1-0005 . I.D. acknowledges support from the Soltis faculty support award and the Ralph E. Powe junior faculty award from Oak Ridge Associated Universities . J.E.A. thanks the National Science Foundation ( CMMI-1255494 ) for supporting semiconductor synthesis. Portions of this work were performed at HPCAT (Sector 16), Advanced Photon Source (APS), Argonne National Laboratory. HPCAT operations are supported by DOE-NNSA{\textquoteright}s Office of Experimental Sciences . The Advanced Photon Source is a U.S. DOE Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under contract no. DE-AC02-06CH11357 . Publisher Copyright: {\textcopyright} 2019 The Author(s)",
year = "2020",
month = jan,
day = "22",
doi = "10.1016/j.xcrp.2019.100005",
language = "English (US)",
volume = "1",
journal = "Cell Reports Physical Science",
issn = "2666-3864",
publisher = "Cell Press",
number = "1",
}