Theoretical studies on spectroscopic properties of ruthenium sensitizers absorbed to TiO2 film surface with connection mode for DSSC
Theoretical studies on spectroscopic properties of ruthenium sensitizers absorbed to TiO2 film surface with connection mode for DSSC
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DOI：
10.1016/j.dyepig.2012.01.018
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发表时间：
2012-09
影响因子：
4.5
通讯作者：
Jie Chen;Fuquan Bai;Jian Wang;Li Hao;Zai-Feng Xie;Qingjiang Pan;Hong-Xing Zhang
中科院分区：
文献类型：
--
作者：
Jie Chen;Fuquan Bai;Jian Wang;Li Hao;Zai-Feng Xie;Qingjiang Pan;Hong-Xing Zhang
光激发发色团向介观半导体二氧化钛纳米粒子表面的电子注入是电子转移的关键过程之一。设计了一个合理可靠的二氧化钛表面模型(锐钛矿型(101)和金红石型(110)晶面模型)，用DFT方法研究了染料分子C101、J13和N749的吸附行为。根据计算结果，得到了详细的轨道组分和吸收跃迁，进而可以区分超快、激发态和发射电子注入。一般来说，二氧化钛的连接面和染料分子的去质子化程度都会对吸收光谱产生强烈的影响。我们的计算表明，效率较高的DSC应该对辅助配体或整个体系具有较大的共轭程度，这有利于从可见光到近红外区域的光子吸收。
Electron injection from a photoexcited chromophore into the surface of mesoscopic semiconductor TiO2nanoparticles is one of the key electron transfer processes for DSSC. A reasonable and reliable TiO2surface model (dropped down the anatase (101) and rutile (110) crystals a slab model) was designed, which was employed to investigate the absorption behavior of the adsorbed dye molecules such as C101, J13 and N749 under DFT method. According to the calculation results, the detailed orbital components and absorption transition are obtained; furthermore, the ultrafast, excited-state electron injection and emission electron injection can be discriminated. Generally, both the connecting surfaces of TiO2and degree of deprotonating dye molecules could influence absorption spectrum intensely. Our calculations show that the more efficient DSSCs should have larger conjugation degree for ancillary ligands or the whole system, which is beneficial to photon absorption from the visible to near-IR region.