Free energy surface of two- and three-dimensional transitions of Au 12 nanoclusters obtained by ab initio metadynamics

Gianluca Santarossa; rnAngelo Vargas; rnMarcella Iannuzzi; rnAlfons Baiker

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Free energy surface of two- and three-dimensional transitions of Au 12 nanoclusters obtained by ab initio metadynamics

机译：从头算动力学获得的Au 12纳米团簇的二维和三维跃迁的自由能表面

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The description of the conformational space generated by metal nanoparticles is a fundamental issue for the study of their physicochemical properties. In this investigation, an exhaustive exploration and a unified view of the conformational space of a gold nanocluster is provided using a Au 12 cluster as an example. Such system is characterized by coexisting planar/quasiplanar and tridimensional conformations separated by high-energy barriers. The conformational space of Au 12 has been explored by means of Born-Oppenheimer ab initio metadynamics, i.e., a molecular dynamics simulation coupled with a history dependent potential to accelerate events that might occur on a long time scale compared to the time step used in the simulations (rare events). The sampled conformations have complex, in general not intuitive topologies that we have classified as planar/quasiplanar or tridimensional, belonging to different regions of the free energy surface. Three conformational free energy basins were identified, one for the planar/quasiplanar and two for the tridimensional structures. At thermodynamic equilibrium, the planar/quasi-planar and tridimensional conformations were found to coexist, to be fiuxional and to be separated by high-free-energy barriers. The comparison between the free energy and the potential energy revealed the relevance of the entropic contribution in the equilibrium distribution of the conformations of the cluster.

机译：金属纳米颗粒产生的构象空间的描述是研究其物理化学性质的基本问题。在本研究中，以Au 12团簇为例，对金纳米团簇的构象空间进行了详尽的探索和统一观察。这种系统的特征是被高能垒隔开的平面/准平面和三维构象共存。 Au 12的构象空间已通过Born-Oppenheimer从头算动力学进行了探索，即分子动力学模拟与历史相关的潜力相结合，可以加速可能在较长时间尺度上发生的事件，而在时间尺度上使用模拟（罕见事件）。采样的构象具有复杂的，通常不是直观的拓扑，我们将其分类为平面/准平面或三维，属于自由能表面的不同区域。确定了三个构象自由能盆地，一个用于平面/准平面，两个用于三维结构。在热力学平衡下，发现平面/准平面和三维构象共存，处于通量状态并被高自由能垒隔开。自由能和势能之间的比较表明，熵的贡献与簇构型的平衡分布有关。

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来源
《Physical review》 |2010年第17期|P.174205.1-174205.10|共10页
作者
Gianluca Santarossa; rnAngelo Vargas; rnMarcella Iannuzzi; rnAlfons Baiker;
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作者单位

Institute for Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich, Hoenggerberg, HCI, 8093 Zurich, Switzerland;

rnInstitute for Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich, Hoenggerberg, HCI, 8093 Zurich, Switzerland;

rnInstitute of Physical Chemistry, University of Zurich, Winterthurerstrasse 190, 8057 Zurich, Switzerland;

rnInstitute for Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich, Hoenggerberg, HCI, 8093 Zurich, Switzerland;

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liquid metals and alloys; structural modeling: serial-addition models, computer simulation; computer simulation of liquid structure;

机译：液态金属和合金;结构建模：串行添加模型;计算机仿真;液体结构的计算机模拟;

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Free energy surface of two- and three-dimensional transitions of Au 12 nanoclusters obtained by ab initio metadynamics

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