Molecular dynamics simulations of the solvent- and thermal history-dependent structure of the PCBM fullerene derivative
Molecular dynamics simulations of the solvent- and thermal history-dependent structure of the PCBM fullerene derivative
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PCBM 富勒烯衍生物的溶剂和热历史依赖性结构的分子动力学模拟
DOI：
10.1039/c2jm16142g
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发表时间：
2012
影响因子：
--
通讯作者：
Guido Raos
中科院分区：
文献类型：
--
作者：
F. Frigerio;M. Casalegno;C. Carbonera;Tommaso Nicolini;S. Meille;Guido Raos
富勒烯衍生物PCBM（[6，6]phenyl-C61-butyric acid methyl ester）是迄今为止用于溶液加工有机光伏器件的最佳电子受体之一。这种成功的原因部分取决于其有利的电子性质，部分取决于其在常见有机溶剂中的溶解度，并且还可能取决于通过沉积后处理（溶剂或热退火）优化其结构和形态的可能性。后一个特征在很大程度上仍然是推测的问题，因为实验验证的器件内PCBM分子组织的结构模型仍然不可用。这种结构表征是不平凡的，考虑到有序性差的PCBM纳米晶体和无定形域似乎经常共存于基于该系统的本体异质结膜中。在这里，我们使用分子动力学（MD）模拟来解决其中的一些问题。我们的出发点是仅有的两种已发表的PCBM晶体结构，它们是通过oDCB（邻二氯苯）和MCB（一氯苯）结晶获得的。两者都含有特定溶剂的客体分子。我们模拟了它们的热行为，从室温到它们的表观熔点。另外的MD模拟涉及通过从这些共晶结构中去除溶剂分子获得的模型晶体。模型，可以适用于非晶相或纳米晶样品已获得通过冷却熔融PCBM，在模拟中的不同阶段去除溶剂后。它们的密度接近实验值，并且它们呈现出富勒烯部分的良好互连网络，其中每个富勒烯部分平均有七个近邻可用于电荷跳跃。在有机太阳能电池生产和主客体系统动力学的框架内讨论了前和后熔化结构特征，如分子间对分布函数。
The fullerene derivative PCBM ([6,6]phenyl-C61-butyric acid methyl ester) is one of the best electron acceptors used so far in solution-processed organic photovoltaic devices. The reasons for this success depend partly on its favourable electronic properties, partly on its solubility in common organic solvents and plausibly also on the possibility to optimize its structure and morphology by post-deposition treatments (solvent or thermal annealing). The latter feature is still largely a matter of speculation, as experimentally validated structural models of PCBM molecular organization within the devices are still unavailable. This structural characterization is non-trivial, given that poorly ordered PCBM nanocrystals and amorphous domains appear to often coexist in bulk-heterojunction films based on this system. Here we address some of these issues using molecular dynamics (MD) simulations. Our starting points are the only two published PCBM crystal structures, which were obtained by crystallization from oDCB (ortho-dichlorobenzene) and MCB (monochlorobenzene). Both contain guest molecules of the specific solvent. We simulated their thermal behavior, from room temperature up to their apparent melting points. Additional MD simulations involved model crystals obtained by removing solvent molecules from these co-crystal structures. Models that can apply to the amorphous phase or to nanocrystalline samples have been obtained by cooling molten PCBM, after removing the solvent at different stages in the simulation. Their densities are close to the experimental values and they present a well interconnected network of fullerene moieties, where each of them has an average of seven close neighbours available for charge hopping. Pre- and post-melting structural features such as intermolecular pair distribution functions are discussed in the framework of organic solar cell production and host–guest system dynamics.
影响因子：
5.5
作者：
R. Beal;A. Stavrinadis;J. Warner;Jason M. Smith;H. Assender;A. Watt
通讯作者：
R. Beal;A. Stavrinadis;J. Warner;Jason M. Smith;H. Assender;A. Watt
影响因子：
5.5
作者：
Ruehle, Victor;Lukyanov, Alexander;May, Falk;Schrader, Manuel;Vehoff, Thorsten;Kirkpatrick, James;Baumeier, Bjoern;Andrienko, Denis
通讯作者：
Andrienko, Denis
影响因子：
4.4
作者：
MacKenzie, Roderick C. I.;Frost, Jarvist M.;Nelson, Jenny
通讯作者：
Nelson, Jenny