Third- And Fifth-Order Nonlinear Optical Response of a TICT/Stilbene Hybrid Chromophore

Alexander J.T. Lou; Sepehr Benis; Munan Gao; Alexander Baev; David Kim; Eric W. Van Stryland; David J. Hagan; Tobin J. Marks

doi:10.1021/acs.jpcc.9b11735

Third- And Fifth-Order Nonlinear Optical Response of a TICT/Stilbene Hybrid Chromophore

Alexander J.T. Lou, Sepehr Benis, Munan Gao, Alexander Baev, David Kim, Eric W. Van Stryland, David J. Hagan, Tobin J. Marks^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

11 Scopus citations

Abstract

Twisted intramolecular charge transfer (TICT) chromophores exhibit a promising third-order nonlinear optical (NLO) response, γ, which is potentially useful for all-optical switching. Here we explore the third- and fifth-order NLO response of a newly synthesized chromophore, TMC-3′, which incorporates both stilbene and TICT motifs with optical function. Solution Z-scan measurements in CH₂Cl₂ reveal modest two-photon absorptions (2PA) at 1100 and 800 nm (σ_2PA > 80 GM), and two contributions to the nonlinear refraction. The first component is attributed to the third-order bound-electronic response, while the second is assigned to a fifth-order process involving 2PA induced excited state refraction (2PA-ESR). Quantum computation suggests that the differences between the present work and previous studies lie primarily in the addition of the stilbene related states, as well as the increase in ground state dipole moment. This work yields insight into the third- and fifth-order NLO response of TICT chromophores and demonstrates that subtle structural modifications significantly impact their functionality.

Original language	English (US)
Pages (from-to)	5363-5370
Number of pages	8
Journal	Journal of Physical Chemistry C
Volume	124
Issue number	9
DOIs	https://doi.org/10.1021/acs.jpcc.9b11735
State	Published - Mar 5 2020

Funding

We thank AFOSR Grant FA9550_12_1_0119 and MURI Grant FA9550_14_1_0040 for support of this research. A.J.-T.L. thanks the NDSEG for a graduate research fellowship. S.B, M.G, E.W.V.S, and D.J.H thank the Army Research Lab (W911NF-15-2-0090) for support. We thank AFOSR Grant FA9550_12_1_0119 and MURI Grant FA9550_14_1_0040 for support of this research. A.J.-T.L. thanks the NDSEG for a graduate research fellowship. S.B, M.G, E.W.V.S, and D.J.H thank the Army Research Lab (W911NF-15-2-0090) for support.

ASJC Scopus subject areas

Electronic, Optical and Magnetic Materials
General Energy
Physical and Theoretical Chemistry
Surfaces, Coatings and Films

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abstract = "Twisted intramolecular charge transfer (TICT) chromophores exhibit a promising third-order nonlinear optical (NLO) response, γ, which is potentially useful for all-optical switching. Here we explore the third- and fifth-order NLO response of a newly synthesized chromophore, TMC-3′, which incorporates both stilbene and TICT motifs with optical function. Solution Z-scan measurements in CH2Cl2 reveal modest two-photon absorptions (2PA) at 1100 and 800 nm (σ2PA > 80 GM), and two contributions to the nonlinear refraction. The first component is attributed to the third-order bound-electronic response, while the second is assigned to a fifth-order process involving 2PA induced excited state refraction (2PA-ESR). Quantum computation suggests that the differences between the present work and previous studies lie primarily in the addition of the stilbene related states, as well as the increase in ground state dipole moment. This work yields insight into the third- and fifth-order NLO response of TICT chromophores and demonstrates that subtle structural modifications significantly impact their functionality.",

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AU - Marks, Tobin J.

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N2 - Twisted intramolecular charge transfer (TICT) chromophores exhibit a promising third-order nonlinear optical (NLO) response, γ, which is potentially useful for all-optical switching. Here we explore the third- and fifth-order NLO response of a newly synthesized chromophore, TMC-3′, which incorporates both stilbene and TICT motifs with optical function. Solution Z-scan measurements in CH2Cl2 reveal modest two-photon absorptions (2PA) at 1100 and 800 nm (σ2PA > 80 GM), and two contributions to the nonlinear refraction. The first component is attributed to the third-order bound-electronic response, while the second is assigned to a fifth-order process involving 2PA induced excited state refraction (2PA-ESR). Quantum computation suggests that the differences between the present work and previous studies lie primarily in the addition of the stilbene related states, as well as the increase in ground state dipole moment. This work yields insight into the third- and fifth-order NLO response of TICT chromophores and demonstrates that subtle structural modifications significantly impact their functionality.

AB - Twisted intramolecular charge transfer (TICT) chromophores exhibit a promising third-order nonlinear optical (NLO) response, γ, which is potentially useful for all-optical switching. Here we explore the third- and fifth-order NLO response of a newly synthesized chromophore, TMC-3′, which incorporates both stilbene and TICT motifs with optical function. Solution Z-scan measurements in CH2Cl2 reveal modest two-photon absorptions (2PA) at 1100 and 800 nm (σ2PA > 80 GM), and two contributions to the nonlinear refraction. The first component is attributed to the third-order bound-electronic response, while the second is assigned to a fifth-order process involving 2PA induced excited state refraction (2PA-ESR). Quantum computation suggests that the differences between the present work and previous studies lie primarily in the addition of the stilbene related states, as well as the increase in ground state dipole moment. This work yields insight into the third- and fifth-order NLO response of TICT chromophores and demonstrates that subtle structural modifications significantly impact their functionality.

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Third- And Fifth-Order Nonlinear Optical Response of a TICT/Stilbene Hybrid Chromophore

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