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Optical-field driven charge-transfer modulations near composite nanostructures.

ABSTRACT: Optical activation of material properties illustrates the potentials held by tuning light-matter interactions with impacts ranging from basic science to technological applications. Here, we demonstrate for the first time that composite nanostructures providing nonlocal environments can be engineered to optically trigger photoinduced charge-transfer-dynamic modulations in the solid state. The nanostructures explored herein lead to out-of-phase behavior between charge separation and recombination dynamics, along with linear charge-transfer-dynamic variations with the optical-field intensity. Using transient absorption spectroscopy, up to 270% increase in charge separation rate is obtained in organic semiconductor thin films. We provide evidence that composite nanostructures allow for surface photovoltages to be created, which kinetics vary with the composite architecture and last beyond optical pulse temporal characteristics. Furthermore, by generalizing Marcus theory framework, we explain why charge-transfer-dynamic modulations can only be unveiled when optic-field effects are enhanced by nonlocal image-dipole interactions. Our demonstration, that composite nanostructures can be designed to take advantage of optical fields for tuneable charge-transfer-dynamic remote actuators, opens the path for their use in practical applications ranging from photochemistry to optoelectronics.

SUBMITTER: Lee KJ

PROVIDER: S-EPMC7708636 | biostudies-literature | 2020 Dec

REPOSITORIES: biostudies-literature

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Optical-field driven charge-transfer modulations near composite nanostructures.

Lee Kwang Jin KJ Beyreuther Elke E Jalil Sohail A SA Kim Sang Jun SJ Eng Lukas M LM Guo Chunlei C André Pascal P

Nature communications 20201201 1

Optical activation of material properties illustrates the potentials held by tuning light-matter interactions with impacts ranging from basic science to technological applications. Here, we demonstrate for the first time that composite nanostructures providing nonlocal environments can be engineered to optically trigger photoinduced charge-transfer-dynamic modulations in the solid state. The nanostructures explored herein lead to out-of-phase behavior between charge separation and recombination ...[more]

PMID: 33262344

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Project description:In dipolar organic π-conjugated molecules, variable photophysical properties can be realized through efficient excited-state intramolecular charge transfer (ICT), which essentially depends on the π-conjugation patterns. Herein, we report a controllable regioselective strategy for synthesis and optical properties of two donor-acceptor (DA)-type 1,3,5,9-tetraarylpyrenes (i.e., 1,3-A/5,9-D (4b) and 1,3-D/5,9-A (4c)) by covalently integrating two phenyl rings and two p-OMe/CHO-substituted phenyl units into the 2-tert-butylpyrene building block, in which the two phenyl rings substituted at the 1,3-positions act as acceptors for 4b or as donors for 4c and the two p-OMe or p-CHO-substituted phenyl moieties substituted at the K-region of 5,9-positions act as donors for 4b or as acceptors for 4c, respectively. Density functional theory calculations on their frontier molecular orbitals and UV-vis absorption of S0 → S1 transition theoretically predicted that the change of π-conjugation directions in the two DA pyrenes could be realized through a variety of substitution patterns, implying that the dissimilar ground-state and excited-state electronic structures exist in each molecule. Their single-crystal X-ray analysis reveal their highly twisted conformations that are beneficial for inhibiting the π-aggregations, which are strikingly different from the normal 1,3,5,9-tetraphenylpyrenes (4a) and related 1,3,6,8-tetraarylpyrenes. Indeed, experimental investigations on their optical properties demonstrated that the excited-state ICT pathways can be successfully controlled by the change of π-conjugation directions through the variety of substitution positions, resulting in the modulations of emission color from deep-blue to green in solution. Moreover, for the present DA pyrenes, highly fluorescent emissions with moderate-to-high quantum yields both in the thin film and in the doped poly(methyl methacrylate) film were obtained, suggesting them as promising emitting materials for the fabrication of organic light-emitting diodes.

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Optical-field driven charge-transfer modulations near composite nanostructures.

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Optical-field driven charge-transfer modulations near composite nanostructures.

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