Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume 124, Issue 19, Pages 10408-10419Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.0c02382
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Funding
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-FG02-99ER14999]
- Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource [NSF ECCS-1542205]
- State of Illinois
- International Institute for Nanotechnology (IIN)
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Excited-state symmetry-breaking charge separation (SB-CS) can offer an efficient pathway to solar energy capture and conversion. We synthesized a series of 1,6,7,12-tetrakis(4-t-butylphenoxy)perylene(3,4:9,10)bis(dicarboximide) cyclophane dimers with m-xylylene, p-xylylene, and 4,4'-diyldimethane-1,1'-biphenyl spacers and studied them with steady-state and time-resolved optical spectroscopies. Photoinduced SB-CS occurs in all three cyclophanes in CH2Cl2, with the SB-CS rate decreasing as the interchromophore distance is increased. Time-resolved emission spectroscopy and kinetic modeling reveal that the chargeseparated state exists in pseudoequilibrium with the excited state prior to decay. Notably, the meta-spaced cyclophane also undergoes SB-CS in toluene within similar to 100 ps, despite the lack of charge stabilization by the low dielectric constant solvent. These results demonstrate that SB-CS can occur across long distances and in weakly polar environments, which offers the possibility of harnessing SB-CS for solar energy capture and conversion.
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