RT info:eu-repo/semantics/article
T1 Are zinc clusters really amorphous? A detailed protocol for locating global minimum structures of clusters
A1 Aguado Rodríguez, Andrés
A1 Vega Hierro, Andrés
A1 Lebon, Alexandre
A1 von Issendorff, Bernd
K1 Zinc clusters
K1 Grupos de zinc
K1 Amorphism
K1 Amosfismo
AB We report the results of a conjoint experimental/theoretical effort to assess the structures of free-standing zinc clusters with up to 73 atoms. Experiment provides photoemission spectra for Zn􀀀N cluster anions, to be used as fingerprints in structural assessment, as well as mass spectra for both anion and cation clusters. Theory provides both a detailed description of a novel protocol to locate global minimum structures of clusters in an efficient and reliable way, and its specific application to neutral and charged zinc clusters. Our methodology is based on the well-known hybrid EP-DFT (empirical potential-density functional theory) approach, in which the approximate potential energy surface generated by an empirical Gupta potential is first sampled with unbiased basin hopping simulations, and then a selection of the isomers so identified is re-optimized at a first-principles DFT level. The novelty introduced in our paper is a simple but efficient new recipe to obtain the best possible EP parameters for a given cluster system,with which the first step of the EP-DFT method is to be performed. Our method is able to reproduce experimental measurements at an excellent level for most cluster sizes, implying its ability to locate the true global minimum structures; meanwhile, if exactly the same method is applied based on the existing Gupta potential (fitted to bulk properties), it leads to wrong predicted structures with energies between 1 and 2 eV above the correct ones. Opposite to what was claimed in the past, our work unequivocallydemonstrates that Zn clusters are not amorphous, and they rather adopt high symmetry structures for most sizes. We show that Zn clusters have a number of exotic, unprecedented structural and electronic properties which are not expected for clusters of a metallic element, and describe them in detail.
PB Royal Society of Chemistry
SN 2040-3372
YR 2018
FD 2018
LK http://uvadoc.uva.es/handle/10324/36720
UL http://uvadoc.uva.es/handle/10324/36720
LA eng
NO Nanoscale, 2018, n. 40. p. 19162-19181
NO Producción Científica
DS UVaDOC
RD 17-jul-2024