Two-Dimensional nonlinear optical switching materials: molecular engineering toward high nonlinear optical contrasts

Combining photochromism and nonlinear optical (NLO) properties of molecular switches-functionalized self-assembled monolayers (SAMs) represents a promising concept toward novel photonic and optoelectronic devices. Using second harmonic generation, density functional theory, and correlated wave funct...

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Bibliographic Details
Main Authors: Hänsel, Marc (Author) , Tegeder, Petra (Author)
Format: Article (Journal)
Language:English
Published: October 16, 2018
In: The journal of physical chemistry. C, Energy, materials, and catalysis
Year: 2018, Volume: 122, Issue: 44, Pages: 25555-25564
ISSN:1932-7455
DOI:10.1021/acs.jpcc.8b08212
Online Access:Verlag, Volltext: https://doi.org/10.1021/acs.jpcc.8b08212
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Author Notes:Marc Hänsel, Christoph Barta, Clemens Rietze, Manuel Utecht, Karola Rück-Braun, Peter Saalfrank, and Petra Tegeder

MARC

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520 |a Combining photochromism and nonlinear optical (NLO) properties of molecular switches-functionalized self-assembled monolayers (SAMs) represents a promising concept toward novel photonic and optoelectronic devices. Using second harmonic generation, density functional theory, and correlated wave function methods, we studied the switching abilities as well as the NLO contrasts between different molecular states of various fulgimide-containing SAMs on Si(111). Controlled variations of the linker systems as well as of the fulgimides enabled us to demonstrate very efficient reversible photoinduced ring-opening/closure reactions between the open and closed forms of the fulgimides. Thus, effective cross sections on the order of 10-18 cm-2 are observed. Moreover, the reversible switching is accompanied by pronounced NLO contrasts up to 32%. Further molecular engineering of the photochromic switches and the linker systems may even increase the NLO contrast upon switching. 
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