TY - JOUR
T1 - Third- And Fifth-Order Nonlinear Optical Response of a TICT/Stilbene Hybrid Chromophore
AU - Lou, Alexander J.T.
AU - Benis, Sepehr
AU - Gao, Munan
AU - Baev, Alexander
AU - Kim, David
AU - Van Stryland, Eric W.
AU - Hagan, David J.
AU - Marks, Tobin J.
N1 - Funding Information:
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.
Funding Information:
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.
Publisher Copyright:
Copyright © 2020 American Chemical Society.
PY - 2020/3/5
Y1 - 2020/3/5
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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U2 - 10.1021/acs.jpcc.9b11735
DO - 10.1021/acs.jpcc.9b11735
M3 - Article
AN - SCOPUS:85080082679
SN - 1932-7447
VL - 124
SP - 5363
EP - 5370
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
IS - 9
ER -