Fan Zhaochuan, Koster Rik S, Wang Shuaiwei, Fang Changming, Yalcin Anil O, Tichelaar Frans D, Zandbergen Henny W, van Huis Marijn A, Vlugt Thijs J H
Process and Energy Department, Delft University of Technology, Leeghwaterstraat 39, 2628 CB Delft,The Netherlands.
Debye Institute for Nanomaterials Science and Center for Extreme Matter and Emergent Phenomena, Utrecht University, Princetonplein 5, 3584 CC Utrecht, The Netherlands.
J Chem Phys. 2014 Dec 28;141(24):244503. doi: 10.1063/1.4904545.
A transferable force field for the PbSe-CdSe solid system using the partially charged rigid ion model has been successfully developed and was used to study the cation exchange in PbSe-CdSe heteronanocrystals [A. O. Yalcin et al., "Atomic resolution monitoring of cation exchange in CdSe-PbSe heteronanocrystals during epitaxial solid-solid-vapor growth," Nano Lett. 14, 3661-3667 (2014)]. In this work, we extend this force field by including another two important binary semiconductors, PbS and CdS, and provide detailed information on the validation of this force field. The parameterization combines Bader charge analysis, empirical fitting, and ab initio energy surface fitting. When compared with experimental data and density functional theory calculations, it is shown that a wide range of physical properties of bulk PbS, PbSe, CdS, CdSe, and their mixed phases can be accurately reproduced using this force field. The choice of functional forms and parameterization strategy is demonstrated to be rational and effective. This transferable force field can be used in various studies on II-VI and IV-VI semiconductor materials consisting of CdS, CdSe, PbS, and PbSe. Here, we demonstrate the applicability of the force field model by molecular dynamics simulations whereby transformations are initiated by cation exchange.
利用部分带电刚性离子模型成功开发了一种适用于PbSe-CdSe固体体系的可转移力场，并用于研究PbSe-CdSe异质纳米晶体中的阳离子交换[A. O. 亚尔钦等人，“外延固-固-气生长过程中CdSe-PbSe异质纳米晶体阳离子交换的原子分辨率监测”，《纳米快报》14, 3661 - 3667(2014年)]。在这项工作中，我们通过纳入另外两种重要的二元半导体PbS和CdS来扩展此力场，并提供有关该力场验证的详细信息。参数化结合了巴德电荷分析、经验拟合和从头算能量表面拟合。与实验数据和密度泛函理论计算相比，结果表明使用此力场可以准确再现块状PbS、PbSe、CdS、CdSe及其混合相的广泛物理性质。功能形式和参数化策略的选择被证明是合理且有效的。这种可转移力场可用于对由CdS、CdSe、PbS和PbSe组成的II-VI和IV-VI半导体材料的各种研究。在此，我们通过分子动力学模拟证明了力场模型的适用性，其中转变由阳离子交换引发。
