Nuclear tunneling effects of charge transport in rubrene, tetracene, and pentacene

被引:260
作者
Nan, Guangjun [1 ]
Yang, Xiaodi [1 ]
Wang, Linjun [1 ]
Shuai, Zhigang [1 ,2 ]
Zhao, Yi [3 ,4 ]
机构
[1] Chinese Acad Sci, Inst Chem, BNLMS, Key Lab Organ Solids, Beijing 100190, Peoples R China
[2] Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
[3] Xiamen Univ, State Key Lab Phys Chem Solid Surfaces, Xiamen 361005, Peoples R China
[4] Xiamen Univ, Dept Chem, Xiamen 361005, Peoples R China
关键词
ab initio calculations; hole mobility; hopping conduction; organic semiconductors; random processes; ELECTRON-TRANSFER REACTIONS; SINGLE-CRYSTAL PENTACENE; ORGANIC SEMICONDUCTORS; MOLECULAR-CRYSTALS; TRANSFER INTEGRALS; HOLE TRANSFER; MOBILITY; TRANSISTORS; PARAMETERS; DYNAMICS;
D O I
10.1103/PhysRevB.79.115203
中图分类号
T [工业技术];
学科分类号
08 ;
摘要
The mechanism of charge transport in organic materials is still controversial from both experimental and theoretical perspectives. At room temperature, molecular deformations interact strongly with the charge carrier both through intermolecular and intramolecular phonons, suggesting a thermally activated hopping mechanism as described by the Marcus electron transfer theory. However, several experimental measurements have indicated that the electronic transport behaves in a "bandlike" manner, as indicated by a decrease in mobility with increasing temperature, in contradiction to the Marcus description. Bandlike first-principles calculations based on the Holstein-Peierls model tend to overestimate the charge mobility by about 2 orders of magnitude. Here, a hopping model is derived that not only quantitatively describes the charge mobility but also explains the observed bandlike behavior. This model uses the quantum version of charge-transfer theory coupled with a random-walk simulation of charge diffusion. The results bridge the gap between the two extreme mechanisms. This first-principles method predicts the room-temperature hole mobilities to be 2.4, 2.0, and 0.67 cm(2)/V s, for rubrene, pentacene, and tetracene, respectively, in good agreement with experiment.
引用
收藏
页数:9
相关论文
共 51 条
[41]   Elastomeric transistor stamps: Reversible probing of charge transport in organic crystals [J].
Sundar, VC ;
Zaumseil, J ;
Podzorov, V ;
Menard, E ;
Willett, RL ;
Someya, T ;
Gershenson, ME ;
Rogers, JA .
SCIENCE, 2004, 303 (5664) :1644-1646
[42]   Charge-transport regime of crystalline organic semiconductors: Diffusion limited by thermal off-diagonal electronic disorder [J].
Troisi, A ;
Orlandi, G .
PHYSICAL REVIEW LETTERS, 2006, 96 (08)
[43]   Dynamics of the intermolecular transfer integral in crystalline organic semiconductors [J].
Troisi, A ;
Orlandi, G .
JOURNAL OF PHYSICAL CHEMISTRY A, 2006, 110 (11) :4065-4070
[44]   The hole transfer in DNA: calculation of electron coupling between close bases [J].
Troisi, A ;
Orlandi, G .
CHEMICAL PHYSICS LETTERS, 2001, 344 (5-6) :509-518
[46]   Effect of electronic polarization on charge-transport parameters in molecular organic semiconductors [J].
Valeev, Edward F. ;
Coropceanu, Veaceslav ;
da Silva Filho, Demetrio A. ;
Salman, Seyhan ;
Bredas, Jean-Luc .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2006, 128 (30) :9882-9886
[47]   Roles of inter- and intramolecular vibrations and band-hopping crossover in the charge transport in naphthalene crystal [J].
Wang, L. J. ;
Peng, Q. ;
Li, Q. K. ;
Shuai, Z. .
JOURNAL OF CHEMICAL PHYSICS, 2007, 127 (04)
[48]   Effects of pressure and temperature on the carrier transports in organic crystal: A first-principles study [J].
Wang, L. J. ;
Li, Q. K. ;
Shuai, Z. .
JOURNAL OF CHEMICAL PHYSICS, 2008, 128 (19)
[49]   Influences of crystal structures and molecular sizes on the charge mobility of organic semiconductors: Oligothiophenes [J].
Yang, Xiaodi ;
Wang, Linjun ;
Wang, Caili ;
Long, Wei ;
Shuai, Zhigang .
CHEMISTRY OF MATERIALS, 2008, 20 (09) :3205-3211
[50]   Theoretical modelling of carrier transports in molecular semiconductors: molecular design of triphenylamine dimer systems [J].
Yang, Xiaodi ;
Li, Qikai ;
Shuai, Zhigang .
NANOTECHNOLOGY, 2007, 18 (42)