Structural exploration of water, nitrate/water, and oxalate/water clusters with basin-hopping method using a compressed sampling technique.
Structural exploration of water, nitrate/water, and oxalate/water clusters with basin-hopping method using a compressed sampling technique.
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DOI：
10.1021/jp4109128
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发表时间：
2014-01
期刊：
影响因子：
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通讯作者：
Yirong Liu;Hui Wen;Teng Huang;Xiao Lin;Yanbo Gai;Chang‐jin Hu;Wei-Jun Zhang;Wei Huang
中科院分区：
文献类型：
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作者：
Yirong Liu;Hui Wen;Teng Huang;Xiao Lin;Yanbo Gai;Chang‐jin Hu;Wei-Jun Zhang;Wei Huang
探索原子或分子簇的低位结构仍然是纳米簇科学中的一个基本问题。盆地跳跃通常与随机运动结合使用，随机运动是局部最小结构的扰动。我们结合了“随机采样”和“压缩采样”两种不同的采样技术来探索分子团簇的势能面。我们使用该方法在 MP2/aug-cc-pVDZ 理论水平上研究了水、硝酸盐/水和草酸盐/水簇系统。具有3D结构的NO3(-)(H2O)3簇分子的异构体的能量低于平面结构，此前实验研究报道平面结构为能量最低的结构。发现NO3(-)(H2O)5和NO3(-)(H2O)7团簇的最低能量结构与纯(H2O)8和(H2O)10团簇的结构相似，这与Wang等人先前的实验结果相矛盾(J. Chem. Phys. 2002, 116, 561-570)。通过我们的计算，找到了 C2O4(2-)(H2O)5 和 C2O4(2-)(H2O)6 的新的最小能量结构。
Exploration of the low-lying structures of atomic or molecular clusters remains a fundamental problem in nanocluster science. Basin hopping is typically employed in conjunction with random motion, which is a perturbation of a local minimum structure. We have combined two different sampling technologies, "random sampling" and "compressed sampling", to explore the potential energy surface of molecular clusters. We used the method to study water, nitrate/water, and oxalate/water cluster systems at the MP2/aug-cc-pVDZ level of theory. An isomer of the NO3(-)(H2O)3 cluster molecule with a 3D structure was lower in energy than the planar structure, which had previously been reported by experimental study as the lowest-energy structure. The lowest-energy structures of the NO3(-)(H2O)5 and NO3(-)(H2O)7 clusters were found to have structures similar to pure (H2O)8 and (H2O)10 clusters, which contradicts previous experimental result by Wang et al.(J. Chem. Phys. 2002, 116, 561-570). The new minimum energy structures for C2O4(2-)(H2O)5 and C2O4(2-)(H2O)6 are found by our calculations.