Hybridization and de-hybridization between the locally-excited (LE) state and the charge-transfer (CT) state: a combined experimental and theoretical study

被引：134

作者：

Gao, Yu ^{[1
,2
]}

Zhang, Shitong ^{[1
,2
]}

Pan, Yuyu ^{[1
,2
]}

Yao, Liang ^{[1
,2
]}

Liu, Haichao ^{[1
,2
]}

Guo, Yachen ^{[1
,2
]}

Gu, Qiang ^{[2
]}

Yang, Bing ^{[1
,2
]}

Ma, Yuguang ^{[3
]}

机构：

[1] Jilin Univ, State Key Lab Supramol Struct & Mat, Changchun 130012, Peoples R China

[2] Jilin Univ, Coll Chem, Changchun 130012, Peoples R China

[3] South China Univ Technol, Inst Polymer Optoelect Mat & Devices, State Key Lab Luminescent Mat & Devices, Guangzhou 510640, Guangdong, Peoples R China

来源：

PHYSICAL CHEMISTRY CHEMICAL PHYSICS | 2016年 / 18卷 / 35期

基金：

美国国家科学基金会;

关键词：

LIGHT-EMITTING-DIODES; BLUE FLUORESCENT EMITTERS; HIGHLY EFFICIENT; ELECTRON; MODEL; THERMOCHEMISTRY; OLIGOFLUORENES; PROPORTION; DESIGN;

D O I：

10.1039/c6cp02778d

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Excited state properties play a key role in the photoluminescence (PL) and electroluminescence (EL) performance of organic light-emitting diode (OLED) materials. The solvatochromic effects were observed in a series of triphenylamine (TPA)-phenanthroimidazole (PI) derivatives with the increase of solvent polarity, accompanied by the transformation of an excited state character from the locally-excited (LE) state to the charge-transfer (CT) state in the emission spectra. The excited state properties were systematically investigated in these donor-acceptor systems using time-dependent density functional theory (TD-DFT). The hybridization and de-hybridization processes between LE and CT states were resolved with an increasing number of phenyls along horizontal and vertical directions, respectively. We provide a novel insight into the fine modulation of the excited-state characters and compositions in the donor-acceptor system for the new-generation, low-cost and high-efficiency fluorescent OLED materials.

引用

页码：24176 / 24184

页数：9

共 44 条

[1] DENSITY-FUNCTIONAL THERMOCHEMISTRY .3. THE ROLE OF EXACT EXCHANGE [J].

BECKE, AD .

JOURNAL OF CHEMICAL PHYSICS, 1993, 98 (07) :5648-5652

[2] Asymptotic correction approach to improving approximate exchange-correlation potentials: Time-dependent density-functional theory calculations of molecular excitation spectra [J].

Casida, ME ;

Salahub, DR .

JOURNAL OF CHEMICAL PHYSICS, 2000, 113 (20) :8918-8935

[3] Solvent Effects on the Optical Spectra and Excited-State Decay of Triphenylamine-thiadiazole with Hybridized Local Excitation and Intramolecular Charge Transfer [J].

Fan, Di ;

Yi, Yuanping ;

Li, Zhendong ;

Liu, Wenjian ;

Peng, Qian ;

Shuai, Zhigang .

JOURNAL OF PHYSICAL CHEMISTRY A, 2015, 119 (21) :5233-5240

[4]

Frisch M.J., 2016, Gaussian, V16

[5] Structural changes accompanying intramolecular electron transfer: Focus on twisted intramolecular charge-transfer states and structures [J].

Grabowski, ZR ;

Rotkiewicz, K ;

Rettig, W .

CHEMICAL REVIEWS, 2003, 103 (10) :3899-4031

[6] INHOMOGENEOUS ELECTRON-GAS [J].

RAJAGOPAL, AK ;

CALLAWAY, J .

PHYSICAL REVIEW B, 1973, 7 (05) :1912-1919

[7] Closely Stacked Oligo(phenylene ethynylene)s: Effect of π-Stacking on the Electronic Properties of Conjugated Chromophores [J].

Jagtap, Subodh P. ;

Mukhopadhyay, Sukrit ;

Coropceanu, Veaceslav ;

Brizius, Glen L. ;

Bredas, Jean-Luc ;

Collard, David M. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (16) :7176-7185

[8]

Koch W., 2001, CHEM GUIDE DENSITY F

[9] SELF-CONSISTENT EQUATIONS INCLUDING EXCHANGE AND CORRELATION EFFECTS [J].

KOHN, W ;

SHAM, LJ .

PHYSICAL REVIEW, 1965, 140 (4A) :1133-&

[10] Coupled Oscillators for Tuning Fluorescence Properties of Squaraine Dyes [J].

Lambert, Christoph ;

Scherpf, Thorsten ;

Ceymann, Harald ;

Schmiedel, Alexander ;

Holzapfel, Marco .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2015, 137 (10) :3547-3557

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