Journal
CHEM
Volume 5, Issue 12, Pages 3135-3150Publisher
CELL PRESS
DOI: 10.1016/j.chempr.2019.08.013
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Funding
- National Science Foundation [CHE 1836913, CHE 1800301]
- US Department of Energy, Office of Basic Energy Sciences [DE-FG02-07ER46454]
- US Department of Energy, Division of Materials Sciences and Engineering [DE-FG02-07ER46454]
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Excitonic organic materials owe their tunable optoelectronic properties to intricate microscopic configurations, challenging for conventional characterization methods to resolve, We generalize Kasha's model by incorporating the temperature (T)-dependent absorption peak shift, in addition to the monomer-aggregate absorption peak shift that defines J- and H-aggregates, to characterize the microscopic structures. We show that the short-range interactions dominate in determining the direction of the T-dependent peak shift, which accounts for previously observed T-dependent blueshifting J-aggregates (BJ-aggregates) that were not explained and predicts the existence of redshifting H-aggregates (RH-aggregates). This defines four types of excitonic aggregates: RJ-, BH-, BJ-, and RH-aggregates, where the latter two unconventional aggregates are possible because of the two dimensionality of excitonic systems and cannot be understood with the original Kasha's theory. Our conceptual framework is useful for elucidating structure-function relationships in molecular excitonic systems and is fully compatible with existing tools. Possible extensions to other spectroscopic observables and related systems are discussed.
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