5, 15-二(五氟苯基)-10-(2-氨基苯基)金属咔咯的二阶非线性光学性质

王健; 应晓; 刘海洋

doi:10.6054/j.jscnun.2020024

5, 15-二(五氟苯基)-10-(2-氨基苯基)金属咔咯的二阶非线性光学性质

王健¹,
应晓^1, ,,
刘海洋^2, ,

1.
华南理工大学应用物理系，广州 510641
2.
华南理工大学化学系//广东省燃料电池重点实验室，广州 510641

基金项目:

国家自然科学基金项目 21671068

详细信息

通讯作者:
应晓, 副教授, Email:yingxiao@scut.edu.cn

刘海洋, 教授, Email:chhyliu@scut.edu.cn

中图分类号: O641
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- 文章访问数: 2846
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出版历程
- 收稿日期: 2019-06-23
- 网络出版日期: 2021-03-21
- 刊出日期: 2020-04-24

Second-Order Nonlinear Optical Properties of 5, 15-Bis(pentafluorophenyl)-10-(2-aminophenyl) Metal Corrole

1.
Department of Applied Physics, South China University of Technology, Guangzhou 510641, China
2.
Department of Chemistry, South China University of Technology//The Guangdong Provincial Key Laboratory of Fuel Cell Technology, Guangzhou 510641, China

摘要

摘要: 运用密度泛函理论(DFT)研究了5, 15-二(五氟苯基)-10-(2-氨基苯基)咔咯(F₁₀Cor)及其金属(Mn、Cu、Ga)配位化合物的几何结构、电子吸收光谱和二阶非线性光学(NLO)性质.利用态求和的方法在CAM-B3LYP/aug-cc-pVDZ水平计算了咔咯配位化合物的二阶NLO系数(β₀).计算结果表明：F₁₀Cor及配位化合物的静态二阶NLO系数β₀的大小顺序为F₁₀CorCu(57.75×10^-30 esu)、F₁₀Cor(37.92×10^-30 esu)、F₁₀CorMn(27.10×10^-30 esu)、F₁₀CorGa(20.00×10^-30 esu)，这些咔咯配位化合物的二阶非线性光学响应主要源自于β_y分量的贡献. F₁₀CorCu的二阶NLO响应主要来源于β-HOMO-1→β-LUMO轨道跃迁，表现为2-氨基苯基与咔咯大环之间的配体内电荷转移(ILCT)跃迁.动态第一超极化率计算结果表明，在波长为1 907 nm入射光照下，F₁₀Cor及金属配位化合物均未表现出强的色散效应，其动态二阶NLO系数(β_{1 907 nm})约为静态值β₀的2倍，顺序为F₁₀CorCu(103.94×10^-30 esu)、F₁₀Cor (60.60×10^-30 esu)、F₁₀CorMn(48.75×10^-30 esu)、F₁₀CorGa(34.39×10^-30 esu).
- 金属咔咯 /
- 密度泛函理论 /
- 态求和 /
- 二阶非线性光学性质
Abstract: The geometric and electronic absorption spectra and second-order nonlinear optical (NLO) properties of 5, 15-bis(pentafluorophenyl)-10-(2-aminophenyl) corrole (F₁₀Cor) and metal corrole (Mn, Cu, Ga) complexes have been investigated with density functional theory (DFT) calculations. The second-order NLO coefficients (β₀) of corrole complexes were calculated on the CAM-B3LYP/aug-cc-pVDZ level using the sum-over-states (SOS) method. The calculated results showed that the static second-order NLO coefficients β₀ for F₁₀Cor and complexes followed an order of F₁₀CorCu(57.75×10^-30 esu), F₁₀Cor(37.92×10^-30 esu), F₁₀CorMn(27.10×10^-30 esu) and F₁₀CorGa(20.00×10^-30 esu), the second-order NLO responses of these compounds were mainly contributed by the β_y component. The second-order NLO responses of the F₁₀CorCu complex were derived from the β-HOMO-1 to β-LUMO transition, exhibiting intraligand charge transfer (ILCT) transition between 2-aminophenyl and corrole macrocycle. The calculations of the dynamic first hyperpolarizability indicated that F₁₀Cor and all metal complexes have not shown strong dispersion effect under the influence of incident wavelength of 1 907 nm. The dynamic second-order NLO coefficients (β_{1 907 nm}) were about twice as large as static β₀ values, following an order of F₁₀CorCu (103.94×10^-30 esu), F₁₀Cor (60.60×10^-30 esu), F₁₀CorMn(48.75×10^-30 esu) and F₁₀CorGa(34.39×10^-30 esu).
- metal corrole /
- density functional theory /
- sum-over-states /
- second-order nonlinear optical properties

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图 1 5, 15-二(五氟苯基)-10-(2-氨基苯基)咔咯(F₁₀Cor)及金属配位化合物(F₁₀CorM, M=Mn、Cu、Ga)的分子结构

Figure 1. The molecular structures of 5, 15-bis(pentafluorophenyl)-10-(2-aminophenyl) corrole (F₁₀Cor) and metal corrole (Mn, Cu, Ga) complexes

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图 2 F₁₀Cor及金属配位化合物的前线分子轨道

Figure 2. The frontier molecular orbitals of F₁₀Cor and metal complexes

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图 3 咔咯静态第一超极化率(β₀)与激发态数的收敛关系

Figure 3. The convergent behavior of static first hyperpolarizabilities (β₀) with the number of excited states for corroles

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图 4 咔咯中对静态第一超极化率(β₀)有重要贡献的激发态空穴(蓝色)和电子(绿色)分布

Figure 4. The hole (blue) and electron (green) distribution of major contribution excited states to static first hyperpolarizability (β₀) for corroles

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图 5 计算所得咔咯动态第一超极化率β_w的色散行为

Figure 5. Calculated dispersion behavior of dynamic first hyperpolarizability β_w for corroles

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图 6 咔咯动态第一超极化率(β_{1 907} _nm)与激发态数目之间的收敛关系

Figure 6. The convergent behavior of dynamic first hyperpolarizabilities (β_{1 907} _nm) with the number of excited states for corroles

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表 1 F₁₀Cor和F₁₀CorM(M =Mn, Cu, Ga)的几何结构参数及Mulliken电荷

Table 1 The geometric structure parameters of F₁₀Cor and F₁₀CorM(M =Mn, Cu, Ga) and Mulliken charge

参数	F₁₀Cor	F₁₀CorMn	F₁₀CorCu	F₁₀CorGa
M—N₁键长/nm	-	0.190 5	0.192 1	0.192 4
M—N₂键长/nm	-	0.191 5	0.192 4	0.191 0
M—N₃键长/nm	-	0.191 5	0.192 4	0.191 1
M—N₄键长/nm	-	0.190 6	0.192 2	0.192 5
C₁—C₁₉键长/nm	0.142 5	0.142 3	0.145 4	0.143 0
∠C_2-1-19-18/(°)	17.624	5.684	4.243	3.715
金属电荷数(e)	-	1.153	0.541	1.026
配体电荷数(e)	-	-1.153	-0.541	-1.026

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表 2 计算所得咔咯最大吸收波长(λ_max)、振子强度(f)、基态与激发态偶极矩之差(Δμ)、跃迁能(ΔE)和主要跃迁形式

Table 2 The calculated maximum absorption wavelength (λ_max/nm), oscillator strengths (f), difference in dipole moments between ground and excited state(Δμ), transition energy (ΔE) and major transition forms of corroles

化合物	λ_max/nm	f	Δμ/D	ΔE/eV	β₀	主要跃迁方式
F₁₀Cor	370	1.136	1.006	3.350	2.082	HOMO-1→LUMO+1(62%), HOMO→LUMO(21%)
F₁₀CorMn	349	0.481	0.812	3.552	0.596	β-HOMO→β-LUMO+5(24%), α-HOMO→α-LUMO+1(16%)
F₁₀CorCu	347	0.422	0.960	3.577	0.601	β-HOMO→β-LUMO+2(64%), α-HUMO→α-LUMO+1(14%)
F₁₀CorGa	362	1.216	0.080	3.421	0.164	HOMO-1→LUMO+1(64%), HOMO→LUMO(30%)
注：β₀表示双能级模型计算值(×10^-30 esu)，α和β指分子轨道的α和β自旋态.

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表 3 咔咯的基态偶极矩(μ₀)及其分量

Table 3 The ground state dipole moments (μ₀) and components of corroles

化合物	偶极矩/D
化合物	μ_x	μ_y	μ_z	μ₀
F₁₀Cor	1.53	2.15	-0.79	2.75
F₁₀CorMn	0.90	0.75	0.71	1.37
F₁₀CorCu	0.99	1.21	0.54	1.65
F₁₀CorGa	0.90	1.14	0.68	1.60

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表 4 咔咯的静态极化率α₀及其分量

Table 4 The static polarizabilities α₀ and components of corroles

化合物	极化率/(×10^-25 esu)
化合物	α_xx	α_yy	α_zz	α₀	Δα
F₁₀Cor	588	394	18	333(348)	502
F₁₀CorMn	440	329	2	256(270)	394
F₁₀CorCu	428	372	3	268(280)	400
F₁₀CorGa	493	372	16	293(305)	430
注：括号中的数据是动态极化率α_{1 907 nm}.

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表 5 咔咯静态第一超极化率β₀及其分量

Table 5 The static first hyperpolarizability β₀ and corresponding components of corroles

化合物	第一超极化率/(×10^-30 esu)
化合物	β_x	β_y	β_z	β₀	β_0(CPKS)
F₁₀Cor	-6.02	37.35	2.61	37.92(60.60)	23.45
F₁₀CorMn	-2.30	27.00	0.70	27.10(48.75)	20.89
F₁₀CorCu	-7.45	57.27	0.39	57.75(103.94)	33.89
F₁₀CorGa	-2.33	19.86	0.16	20.00(34.39)	16.15
注：括号中的数据是动态第一超极化率β_{1 907 nm}；β_0(CPKS)采用CPKS方法在CAM-B3LYP/aug-cc-pVDZ水平下计算.

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表 6 计算所得咔咯主要激发态序号、组态系数、主要贡献和对应分子轨道跃迁

Table 6 The calculated major excited states, configuration coefficients, contribution and corresponding MO transitions of corroles

化合物	激发态序号	组态系数	主要贡献率/%	分子轨道跃迁
F₁₀Cor	3	0.526 52	55	HOMO→LUMO+1
		0.410 93	34	HOMO-1→LUMO
F₁₀CorMn	22	0.593 16	35	β-HOMO-2→β-LUMO
	23	0.489 71	24	β-HOMO→β-LUMO+5
	24	0.449 63	20	β-HOMO-2→β-LUMO
	25	0.465 16	22	β-HOMO-2→β-LUMO+1
	26	0.611 33	37	β-HOMO-2→β-LUMO+1
F₁₀CorCu	6	0.703 04	49	β-HOMO-1→β-LUMO
	21	0.313 66	10	α-HOMO-3→α-LUMO+1
	26	0.802 22	64	β-HOMO→β-LUMO+2
F₁₀CorGa	3	0.565 36	64	HOMO-1→LUMO+1
		0.385 72	30	HOMO→LUMO

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