Global Optimization of Li and Na Clusters: Application of a Modified Embedded Atom Method

Huwig, Kai; Grigoryan, Valeri G.; Springborg, Michael

doi:10.1007/s10876-019-01685-7

Cited by 6 publications

(5 citation statements)

References 71 publications

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“…The ionization potential and polarizability values were calculated at MP2/6-311G(d) level of theory for the pure Li clusters and they found a good agreement with the experimental results. Huwig et al [35] identified low-energy Li x and Na x isomers with x = 2-150 using a two-step global structure optimization procedure. The authors determined the magic clusters with enhanced stability compared to other studies already reported, but the structures with x = 74, 83, 87, 95, 104, 131, and 137 atoms were not identified.…”

Section: Introductionmentioning

confidence: 99%

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Application of a quantum genetic algorithm and QTAIM analysis in the study of structural and electronic properties of neutral bimetallic clusters NaxLiy (4 ≤ x + y ≤ 10)

et al. 2020

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Alloy clusters of Na x Li y (4 ≤ x + y ≤ 10) are studied by exploring the potential energy surface in the ab initio MP2 level with the support of a quantum genetic algorithm (QGA). In some cases, the structures have been also refined with DFT and coupledcluster methods. The general trends of sodium-lithium structures are in line with previous studies. The ionization potentials and polarizabilities to all structures were calculated with MP2 method and the average error between these two properties compared with experimental data was 6% and 13%, respectively. The topological analysis based on quantum theory of atoms in molecules (QTAIM) showed that by increasing the cluster size of the diatomic system there was a decrease of atomic interaction energies. The degree of degeneracy from D3BIA aromaticity index and the analysis of the atomic charges showed the influence (by charge transfer) of the chemical element in lower quantity in the cluster with respect to the other atoms. Our achievements of comparing our theoretical results with available experimental data have demonstrated that our approach can also predict satisfactorily quantum atomic and alloy clusters properties, at least, for low nuclearities.

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Section: Introductionmentioning

confidence: 99%

“…Ionization potential and polarizability of some selected structures of Na x Li y (MP2/ LANL2DZ). Experimental ionization potential was measured by Benichou et al[35] and…”

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confidence: 99%

Application of a quantum genetic algorithm and QTAIM analysis in the study of structural and electronic properties of neutral bimetallic clusters NaxLiy (4 ≤ x + y ≤ 10)

et al. 2020

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“…In order to obtain an estimate for the IE we need to know the ground state structure of Na 13 . The neutral Na 13 cluster has been the subject of many studies [17,18,20,22,[33][34][35][36]. A careful analysis of these reports reveals that the 3:3 capped PBP structure of Poteau and Spiegelmann with doublet spin state seems to be the ground state configuration of this neutral cluster.…”

Section: Computational Detailsmentioning

confidence: 99%

On the three lowest spin states of Na13+: Hybrid Density Functional Theory and benchmark CASSCF(12,12)+CASPT2 studies

Alanís‐Manzano

Ramı́rez-Solı́s

2022

Int J of Quantum Chemistry

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The three lowest spin states (S = 0,1,2) of 12 representative Na13+ isomers have been estudied using both, KS‐DFT via three hybrid density functionals, and benchmark multireference CASSCF and CASPT2 methods with a couple of Dunning's correlation consistent basis sets. CASSCF(12,12) geometry optimizations were carried out. Since 12 electrons in 12 active orbitals span the chemically‐significant complete valence space, the results of the present study provide benchmarks for Na13+. The CASPT2(12,12)/cc‐pVTZ* lowest energy structures are three nearly degenerate singlets (S = 0): an isomer formed from two pentagonal bipyramids fused together (PBPb), a capped centered‐squared antiprism [CSAP‐(1,3)] and an optimum tetrahedral OPTET(II) structure, the last two lying 0.88 and 1.63 kcal/mol above the first, respectively. The lowest triplet (S = 1) and quintet (S = 2) states lie 4.33 and 3.77 kcal/mol above the singlet global minimum, respectively. The latter is a deformed icosahedron while the former is a CSAP‐(1,3). The flatness of the potential energy surface of this cluster suggests a rather strong dynamical character at finite temperature. Prediction of the lowest energy structures and electronic properties is crucially sensitive both to non‐dynamical and dynamical electron correlation treatment. The CASPT2 vertical ionization energy is 3.66 eV, in excellent agreement with the 3.6 ± 0.1 eV experimental figure. All the isomers are found to have a strong multireference character, thus making KS density functional theory fundamentally inappropriate for these systems. Only large multiconfigurational CASSCF wavefunctions provide a reliable zeroth‐order description; then the dynamic correlation effects must be properly taken into account for a truly accurate account of the structural and energetic features of alkali‐metal clusters.

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“…7 Generally, the precise configuration of small-sized clusters (typically containing 100 atoms or less) is more conveniently predicted by theoretical calculations. 8,9 The optimal (most stable) structure of a cluster is considered to be the global minimum on its potential energy surface (PES). 10 However, the number of local minima on the PES usually increases exponentially with increasing cluster size.…”

Section: Introductionmentioning

confidence: 99%

“…Metallic clusters, as an intermediate transition state from the individual atom to bulk matter, have attracted growing attention due to their unique properties and numerous promising applications in catalysis, energy, information storage, and biological medicine. − Since their properties rely heavily on cluster sizes and structures, it is crucial to determine the stable structures of the clusters with different sizes and to deduce the pattern of their structural evolution, thereby shedding light on the structure–function relationship. − Meanwhile, gaining a deep understanding of geometrical structure is the essential step toward bridging cluster physics and chemistry from fundamental science to manufacturing technology . Generally, the precise configuration of small-sized clusters (typically containing 100 atoms or less) is more conveniently predicted by theoretical calculations. , The optimal (most stable) structure of a cluster is considered to be the global minimum on its potential energy surface (PES) . However, the number of local minima on the PES usually increases exponentially with increasing cluster size.…”

Section: Introductionmentioning

confidence: 99%

Structural Determination and Hierarchical Evolution of Transition Metal Clusters Based on an Improved Self-Adaptive Differential Evolution with Neighborhood Search Algorithm

Yang,

Yu,

Huang

et al. 2023

J. Chem. Inf. Model.

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Determining the optimal structures and clarifying the corresponding hierarchical evolution of transition metal clusters are of fundamental importance for their applications. The global optimization of clusters containing a large number of atoms, however, is a vastly challenging task encountered in many fields of physics and chemistry. In this work, a high-efficiency self-adaptive differential evolution with neighborhood search (SaNSDE) algorithm, which introduced an optimized cross-operation and an improved Basin Hopping module, was employed to search the lowest-energy structures of Co N , Pt N , and Fe N (N = 3–200) clusters. The performance of the SaNSDE algorithm was first evaluated by comparing our results with the parallel results collected in the Cambridge Cluster Database (CCD). Subsequently, different analytical methods were introduced to investigate the structural and energetic properties of these clusters systematically, and special attention was paid to elucidating the structural evolution with cluster size by exploring their overall shape, atomic arrangement, structural similarity, and growth pattern. By comparison with those results listed in the CCD, 13 lower-energy structures of Fe N clusters were discovered. Moreover, our results reveal that the clusters of three metals had different magic numbers with superior stable structures, most of which possessed high symmetry. The structural evolution of Co, Pt, and Fe clusters could be, respectively, considered as predominantly closed-shell icosahedral, Marks decahedral, and disordered icosahedral-ring growth. Further, the formation of shell structures was discovered, and the clusters with hcp-, fcc-, and bcc-like configurations were ascertained. Nevertheless, the growth of the clusters was not simply atom-to-atom piling up on a given cluster despite gradual saturation of the coordination number toward its bulk limit. Our work identifies the general growth trends for such a wide region of cluster sizes, which would be unbearably expensive in first-principles calculations, and advances the development of global optimization algorithms for the structural prediction of clusters.

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Global Optimization of Li and Na Clusters: Application of a Modified Embedded Atom Method

Cited by 6 publications

References 71 publications

Application of a quantum genetic algorithm and QTAIM analysis in the study of structural and electronic properties of neutral bimetallic clusters NaxLiy (4 ≤ x + y ≤ 10)

Application of a quantum genetic algorithm and QTAIM analysis in the study of structural and electronic properties of neutral bimetallic clusters NaxLiy (4 ≤ x + y ≤ 10)

On the three lowest spin states of Na13+: Hybrid Density Functional Theory and benchmark CASSCF(12,12)+CASPT2 studies

Structural Determination and Hierarchical Evolution of Transition Metal Clusters Based on an Improved Self-Adaptive Differential Evolution with Neighborhood Search Algorithm

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