Low-lying excited states in crystalline perylene

Organic materials are promising candidates for advanced optoelectronics and are used in light-emitting diodes and photovoltaics. However, the underlying mechanisms allowing the formation of excited states responsible for device functionality, such as exciton generation and charge separation, are ins...

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Bibliographic Details
Published in:Proceedings of the National Academy of Sciences - PNAS 2018-01, Vol.115 (2), p.284-289
Main Authors: Rangel, Tonatiuh, Rinn, Andre, Sharifzadeh, Sahar, da Jornada, Felipe H., Pick, André, Louie, Steven G., Witte, Gregor, Kronik, Leeor, Neaton, Jeffrey B., Chatterjee, Sangam
Format: Article
Language:English
Subjects:
ATOMIC AND MOLECULAR PHYSICS
Bethe-Salpeter equation
Crystal structure
Crystallinity
Crystals
excited states
First principles
Light emitting diodes
many-body perturbation theory
molecular crystals
Optoelectronics
Organic light emitting diodes
Organic materials
Perturbation theory
Photovoltaic cells
Photovoltaics
Physical Sciences
Polaritons
Polymorphism
Sample preparation
Single crystals
Solar cells
Spectroscopy
Spectrum analysis
Thin films
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Summary:Organic materials are promising candidates for advanced optoelectronics and are used in light-emitting diodes and photovoltaics. However, the underlying mechanisms allowing the formation of excited states responsible for device functionality, such as exciton generation and charge separation, are insufficiently understood. This is partly due to the wide range of existing crystalline polymorphs depending on sample preparation conditions. Here, we determine the linear optical response of thin-film single-crystal perylene samples of distinct polymorphs in transmission and reflection geometries. The sample quality allows for unprecedented high-resolution spectroscopy, which offers an ideal opportunity for judicious comparison between theory and experiment. Excellent agreement with first-principles calculations for the absorption based on the GW plus Bethe–Salpeter equation (GW-BSE) approach of many-body perturbation theory (MBPT) is obtained, from which a clear picture of the low-lying excitations in perylene emerges, including evidence of an exciton–polariton stopband, as well as an assessment of the commonly used Tamm–Dancoff approximation to the GW-BSE approach. Our findings on this well-controlled system can guide understanding and development of advanced molecular solids and functionalization for applications.
ISSN:0027-8424
1091-6490
DOI:10.1073/pnas.1711126115