Large second-order optical nonlinearity in a ferroelectric molecular crystal of croconic acid with strong intermolecular hydrogen bonds

被引：14

作者：

Sawada, R. ^{[1
]}

Uemura, H. ^{[1
]}

Sotome, M. ^{[1
]}

Yada, H. ^{[1
]}

Kida, N. ^{[1
]}

Iwano, K. ^{[2
]}

Shimoi, Y. ^{[3
]}

Horiuchi, S. ^{[3
,4
]}

Okamoto, H. ^{[1
,4
]}

机构：

[1] Univ Tokyo, Dept Adv Mat Sci, Chiba 2778561, Japan

[2] Grad Univ Adv Studies, Inst Mat Struct Sci, High Energy Accelerator Res Org KEK, Tsukuba, Ibaraki 3050801, Japan

[3] Natl Inst Adv Ind Sci & Technol, Tsukuba, Ibaraki 3058562, Japan

[4] Japan Sci & Technol Agcy JST, CREST, Tokyo 1020075, Japan

来源：

APPLIED PHYSICS LETTERS | 2013年 / 102卷 / 16期

关键词：

Intermolecular hydrogen bonds - Molecular dipole moment - Near infrared region - Nonlinear optical response - Photoexcited state - Second harmonic generation spectroscopies - Second order optical nonlinearity - Second-order nonlinear susceptibility;

D O I：

10.1063/1.4802727

中图分类号：

O59 [应用物理学];

学科分类号：

摘要：

Linear and nonlinear optical responses in a molecular crystal, croconic acid, showing electronic-type ferroelectricity were studied by reflection and second harmonic generation spectroscopy. The second-order nonlinear susceptibility chi((2)) was very large, exceeding 10(-6) esu in the near-infrared region. The enhancement of chi((2)) was attributed to the large dipole moment of the lowest pi-pi* transition and the large difference between the molecular dipole moments for the ground state and the photoexcited state. We deduced the molecular orbitals (MOs) and dipole moments responsible for the large chi((2)) by comparing the experimental optical parameters and MO calculation results based upon density functional theory. (C) 2013 AIP Publishing LLC [http://dx.doi.org/10.1063/1.4802727]

引用

页数：4

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