2021
DOI: 10.1002/chem.202102766
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Elucidating Inner Workings of Naturally Sourced Organic Optoelectronic Materials with Ultrafast Spectroscopy

Abstract: Recent advances in sustainable optoelectronics including photovoltaics, light‐emitting diodes, transistors, and semiconductors have been enabled by π‐conjugated organic molecules. A fundamental understanding of light‐matter interactions involving these materials can be realized by time‐resolved electronic and vibrational spectroscopies. In this Minireview, the photoinduced mechanisms including charge/energy transfer, electronic (de)localization, and excited‐state proton transfer are correlated with functional … Show more

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Cited by 7 publications
(18 citation statements)
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“…This analysis hints at a possible coherence between the “jiggling and wiggling” of atoms and the electronic change enabled by an ultrafast ESIPT reaction starting from PA* with excess energy by a bluer pump, and the apparent 750 fs time constant could have contributions from characteristic vibrational cooling, ,, which may result in better charge/energy transfer for optoelectronic applications in the redder-light-absorbing region (see Section ). , An alternative interpretation could be that a sequential or concerted ESIDPT occurs on this time scale, which will be the subject of theoretical calculations as follows (e.g., PA* ↔ PS* occurs on the sub-ps time scale).…”
Section: Resultsmentioning
confidence: 99%
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“…This analysis hints at a possible coherence between the “jiggling and wiggling” of atoms and the electronic change enabled by an ultrafast ESIPT reaction starting from PA* with excess energy by a bluer pump, and the apparent 750 fs time constant could have contributions from characteristic vibrational cooling, ,, which may result in better charge/energy transfer for optoelectronic applications in the redder-light-absorbing region (see Section ). , An alternative interpretation could be that a sequential or concerted ESIDPT occurs on this time scale, which will be the subject of theoretical calculations as follows (e.g., PA* ↔ PS* occurs on the sub-ps time scale).…”
Section: Resultsmentioning
confidence: 99%
“…With a bevy of equilibrium and nonequilibrium insights, an informed design of Draconin Red should be able to improve its functional properties and application potentials through strategic substitution(s) of the methoxy groups to stronger electron withdrawing/donating groups at opposite ends of the chromophore to incur more directionality of a CT state. , This engineering feat may enhance the intramolecular CT character of the pigment that is nearly ubiquitous for many high-performance optoelectronic molecules as we recently demonstrated for xylindein and its derivatives. ,,,, In particular, the exciton transport between chromophores with minimal energy loss (like in photosynthetic systems) , represents a crucial step to replicating and optimizing charge generation in designed organic electronics (e.g., donor–acceptor bulk heterojunction solar cells). However, the facile crystallization of Draconin Red from solution processing (Section ) needs to be addressed before its effective use as a donor.…”
Section: Resultsmentioning
confidence: 99%
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“…Proton transfer is among the most abundant and fundamental processes in organic, inorganic, and biological systems which can occur between molecules and solvents (intermolecular), leading to a change of the protonation state; or within the molecule itself (intramolecular), resulting in the formation of a constitutional (structural) isomer. Excited-state proton transfer (ESPT) and excited-state intramolecular proton transfer (ESIPT) represent functional processes with distinct underlying mechanisms that have powered broad applications from research labs to industrial settings and from biological to energy fields, which include bioimaging and materials advances. , Recently, there have been extensive studies into the potential of ESIPT reactions from optoelectronic devices, fluorescence sensors, organic light-emitting diodes, lasers, and optical data storages to displays, among others. , Many of the molecules possessing ESPT or ESIPT capabilities are naturally occurring, such as the green fluorescent protein (GFP) from Aequorea victoria, , a blue-green pigment xylindein from the fungi Chlorociboria aeruginosa, and a red pigment Draconin red from the fungi Scytalidium cuboideum . The fundamental knowledge and insights obtained that delineate the proton transfer mechanisms in various natural systems have since inspired rational design inquiries and targeted molecular engineering endeavors.…”
Section: Introductionmentioning
confidence: 99%