Si掺杂4,7-二(2-噻吩基)苯并噻二唑-3-辛基噻吩二炔在SnO_2(100)表面吸附的理论研究
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摘要
采用密度泛函理论与周期性平板模型相结合的方法,在GGA/PW91/DNP水平上研究了4,7-二(2-噻吩基)苯并噻二唑-3-辛基噻吩二炔(简称PTE-DTBT)和Si掺杂4,7-二(2-噻吩基)苯并噻二唑-3-辛基噻吩二炔(简称PTE-DTBT-Si)在SnO_2(100)表面的吸附.通过吸附前后化合物PTE-DTBT和PTE-DTBT-Si的Mulliken charge和前线轨道分析表明:当PTE-DTBT和PTE-DTBT-Si吸附在SnO_2(100)表面时,PTE-DTBT向SnO_2(100)表面转移了0.059 e电荷,SnO_2(100)表面向PTE-DTBTSi转移0.042 e电荷;同时前线轨道能隙变窄.通过吸附前后SnO_2(100)表面的能带和态密度分析表明:在SnO_2(100)表面吸附了化合物PTE-DTBT和PTE-DTBT-Si后,SnO_2中价带和导带间的禁带变窄或消失.且研究表明,PTE-DTBT掺杂一个Si原子后,电池材料光伏性更好.
The density functional theory and periodic slab model at the GGA / PW91 / DNP level are used to investigate the 3-octylthien-2,5-ylenediethynylene-co-benzo[c]-1',2',5'-thiadiazo-3,6-ylenedi( 2,5-thienylene)( PTE-DTBT for short) and silicon doping 3-octylthien-2,5-ylenediethynylene-co-benzo[c]-1',2',5'-thiadiazo-3,6-ylenedi( 2,5-thienylene)( PTE-DTBT-Si for short) adsorption on SnO_2( 100) Surface. The Mulliken charges and frontier orbitals of the PTE-DTBT and the PTE-DTBT-Si are also discussed. The results reveal that the charge of 0. 059 e transfers from the PTE-DTBT to the SnO_2( 100) surface,on the contrary,the charge of 0. 042 e transfers from the SnO_2( 100) surface to the PTE-DTBT-Si and the energy gap becomes narrow when the adsorption has occurred. The energy band structures and densities of states of the SnO_2( 100)-PTE-DTBT and the SnO_2( 100)-PTE-DTBT-Si are also discussed. The results reveal that the band gap becomes narrow or disappears when the adsorption has occurred. The results indicate that PTE-DTBT-Si has better activity of photovoltaic than PTE-DTBT.
The density functional theory and periodic slab model at the GGA / PW91 / DNP level are used to investigate the 3-octylthien-2,5-ylenediethynylene-co-benzo[c]-1',2',5'-thiadiazo-3,6-ylenedi( 2,5-thienylene)( PTE-DTBT for short) and silicon doping 3-octylthien-2,5-ylenediethynylene-co-benzo[c]-1',2',5'-thiadiazo-3,6-ylenedi( 2,5-thienylene)( PTE-DTBT-Si for short) adsorption on SnO_2( 100) Surface. The Mulliken charges and frontier orbitals of the PTE-DTBT and the PTE-DTBT-Si are also discussed. The results reveal that the charge of 0. 059 e transfers from the PTE-DTBT to the SnO_2( 100) surface,on the contrary,the charge of 0. 042 e transfers from the SnO_2( 100) surface to the PTE-DTBT-Si and the energy gap becomes narrow when the adsorption has occurred. The energy band structures and densities of states of the SnO_2( 100)-PTE-DTBT and the SnO_2( 100)-PTE-DTBT-Si are also discussed. The results reveal that the band gap becomes narrow or disappears when the adsorption has occurred. The results indicate that PTE-DTBT-Si has better activity of photovoltaic than PTE-DTBT.
引文
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[3]Huynh W U,Dittmer J J,Alivisatos A P.Hybrid nanorod-polymer solar cells[J].Science,2002,295:2425.
[4]Sailor M J,Ginsburg E J,Gorman C B,et al.Thin films of n-Si/poly-(CH3)3Si-cyclooctatetraene:conducting-polymer solar cells and layered structures[J].Science,1990,249:1146.
[5]Avasthi S,Lee S,Loo Y L,et al.Role of majority and minority carrier barriers silicon/organic hybrid heterojunction solar cells[J].Adv.Mater.,2011,23:5762.
[6]Liu Q,Ono M,Tang Z,et al.Highly efficient crystalline silicon/zonyl fluorosurfactant-treated organic heterojunction solar cells[J].Appl.Phys.Lett.,2012,100:183901.
[7]Liu R,Lee S T,Sun B.13.8%efficiency hybrid Si/organic heterojunction solar cells with Mo O3film as antireflection and inversion induced layer[J].Adv.Mater.,2014,26:6007.
[8]Van Beek R,Zoombelt A P,Jenneskens L W.Side chain mediated electronic contact between a tetrahydro-4H-thiopyran-4-ylidene-appended polythiophene and Cd Te quanturn dots[J].Chem.Eur.,2006,12:8075.
[9]Advincula,R.C.Hybrid organic-inorganic nanomaterials based on polythiophene dendronized nanoparticles[J].Dalton Trans.,2006,23:2778.
[10]Liu C J,Tsai J H,Lee W Y,et al.New didecyloxyphenylene-acceptor alternating conjugated copolymers:synthesis,properties,and optoelectronic device applications[J].Macromolecules,2008,41:6952.
[11]Chen M H,Hou J H,Hong Z R,et al.Efficient polymer solar cells with thin active layers based on alternating polyfluorene copolymer/fullerene bulk heterojunctions[J].Adv.Mater,2009,21:4238.
[12]Blouin N,Michaud A,Leclerc M.A low-bandgap poly(2,7-carbazole)derivative for use in high-performance solar cells[J].Adv.Mater.,2007,19:2295.
[13]Song S,Jin Y,Kim S H,et al.Stabilized polymers with novel indenoindene backbone against photodegradation for LEDs and solar cells[J].Macromolecules,2008,41:7296.
[14]Zhou E,Cong J,Yamakawa S,et al.Synthesis of thieno[3,4-b]pyrazine-based and 2,1,3-benzothiadiazole-based donor-acceptor copolymers and their application in photovoltaic devices[J].Macromolecules,2010,43:2873.
[15]Liu Z Y,Li Y J,Huang P C.Synthesis and optical properties of a novel low band-gap conjugated polymer[J].Acta Chimica Sinica,2008,66:999[刘中义,李彦军,黄鹏程.一种新型低带隙共轭聚合物的合成及其光学性质[J].化学学报,2008,66:999]
[16]Zhang F L,Wan B J,Xu B H,et al.Theoretical study of synthesis mechanism and electronic structure for 3-octylthien-2,5-ylenediethynylene-cobenzo[c]-1',2',5'-thiadiazo-3,6-ylenedi(2,5-thienylene)[J].Acta Chimica Sinica,2012,70:721[张福兰,万邦江,徐伯华,等.4,7-二(2-噻吩基)苯并噻二唑-3-辛基噻吩二炔的合成机理和电子结构的理论研究[J].化学学报,2012,70:721]
[17]Zhang F L,Wu X F.Density functional theory study of3-octylthien-2,5-ylenediethynyl-ene-co-benzo[c]-1’,2’,5’-thiadiazo-3,6-ylenedi(2,5-thienylene)adsorption on Ti O2(100)surf-ace[J].J.At.Mol.Phys.,2012,29:927[张福兰,吴兴发.4,7-二(2-噻吩基)苯并噻二唑-3-辛基噻吩二炔在Ti O2(100)表面吸附的密度泛函理论研究[J].原子与分子物理学报,2012,29:927]
[18]Delley B.An all-electron numerical method for solving the local density functional for polyatomic molecules[J].J.Chem.Phys.,1990,92:508.
[19]Delley B.From molecules to solids with the DMol3approach[J].J.Chem.Phys.,2000,113:7756.