Isomer identification and resolution in small gold clusters

Huang, Wei; Pal, Ranjan; Wang, Lei Ming; Zeng, Xiao Cheng; Wang, Lai Sheng

doi:10.1063/1.3299292

Cited by 88 publications

(112 citation statements)

References 46 publications

Supporting

Mentioning

101

Contrasting

Unclassified

Order By: Relevance

“…2(b) has been obtained by superposing the spectra of isomers 1 and 2 with equal weights since both isomers are energetically degenerate [25]. The overall agreement between theoretical and experimental TRPES is very good.…”

Section: Resultsmentioning

confidence: 91%

Switching from molecular to bulklike dynamics in electronic relaxation of a small gold cluster

et al. 2012

View full text Add to dashboard Cite

We have investigated the ultrafast electronic relaxation of Au − 7 using time-resolved photoelectron spectroscopy combined with first-principles simulations of the excited-state dynamics. Unlike previous findings, which have demonstrated molecularlike excited-state relaxation in Au − 7 at low excitation energy (1.56 eV), we show here that excitation with 3.12 eV leads to bulklike electronic relaxation without a considerable change of geometry. The experimental findings are fully supported by theoretical simulations, which reveal a bulklike electron-hole relaxation mechanism in a far band-gap cluster. Our findings demonstrate that small gold clusters in the sub-nm size range can exhibit either molecularlike or bulklike properties, depending on the excitation energy.

show abstract

Section: Resultsmentioning

confidence: 91%

Switching from molecular to bulklike dynamics in electronic relaxation of a small gold cluster

et al. 2012

View full text Add to dashboard Cite

show abstract

“…In addition, several heteroatomic clusters have been studied using BH-DFT. Generally, FP-BH studies have been used to investigate the influence of a single main-group element, [176] transition metal, [177,208]22 or a few sulfur [175] atoms on the geometric and electronic structure of Au clusters. A little different and, from a chemical point of view, more instructive, is the case study by Gao et al [174] moiety.…”

Section: Basin Hoppingmentioning

confidence: 99%

Global optimization of clusters using electronic structure methods

Heiles

Johnston

2013

Int J of Quantum Chemistry

198

191

View full text Add to dashboard Cite

Over the past decade, there has been a significant growth in the development and application of methods for performing global optimization (GO) of cluster and nanoparticle structures using first-principles electronic structure methods coupled to sophisticated search algorithms. This has in part been driven by the desire to avoid the use of empirical potentials (EPs), especially in cases where no reliable potentials exist to guide the search toward reasonable regions of configuration space. This has been facilitated by improvements in the reliability of the search algorithms, increased efficiency of the electronic structure methods, and the development of faster, multiprocessor high-performance computing architectures. In this review, we give a brief overview of GO algorithms, though concentrating mainly on genetic algorithm and basin hopping techniques, first in combination with EPs. The major part of the review then deals with details of the implementation and application of these search methods to allow exploration for global minimum cluster structures directly using electronic structure methods and, in particular, density functional theory. Example applications are presented, ranging from isolated monometallic and bimetallic clusters to molecular clusters and ligated and surface supported metal clusters. Finally, some possible future developments are highlighted.

show abstract

“…Because of the strong relativistic effects of the gold atom, the spin orbit (SO) coupling effect [74] also must be considered for heavy atoms such as gold. The PBE0/CRENBL level and SO effects were carefully selected for the gold atom to achieve quantitative agreement between the experimental and theoretical PES spectra [64,[75][76][77][78][79].…”

Section: Theoretical Methodsmentioning

confidence: 99%

“…The basin-hopping (BH) global search method [62][63][64][65][66] coupled with DFT was employed to search for low-lying isomers of phosphorus-doped clusters of the type Au n P À 2 (n = 1-8). The original BH algorithm fundamentally combined the Metropolis random sampling technique and local optimization procedures.…”

Section: Theoretical Methodsmentioning

confidence: 99%

Probing the structures and electronic properties of dual-phosphorus-doped gold cluster anions (AunP2-, n= 1–8): A density

Huang

Liu

et al. 2015

Chemical Physics

Self Cite

View full text Add to dashboard Cite

a b s t r a c tThe geometries of gold clusters doped with two phosphorus atoms, Au n P À 2 (n = 1-8), were investigated using density functional theory (DFT) methods. Various two-dimensional (2D) and three-dimensional (3D) structures of the doped clusters were studied. The results indicate that the structures of dualphosphorus-doped gold clusters exhibit large differences from those of pure gold clusters with small cluster sizes. In our study, as for Au 6 P À 2 , two cis-trans isomers were found. The global minimum of Au 8 P À 2 presents a similar configuration to that of Au À 20 , a pyramid-shaped unit, and the potential novel optical and catalytic properties of this structure warrant further attention. The higher stability of Au n P À 2 clusters relative to Au À nþ2 (n = 1-8) clusters was verified based on various energy parameters, and the results indicate that the phosphorus atom can improve the stabilities of the gold clusters. We then explored the evolutionary path of Au n P À 2 (n = 1-8) clusters. We found that Au n P À 2 clusters exhibit the 2D-3D structural transition at n = 6, which is much clearer and faster than that of pure gold clusters and single-phosphorus-doped clusters. The electronic properties of Au n P À 2 (n = 1-8) were then investigated. The photoelectron spectra provide additional fundamental information on the structures and molecular orbitals shed light on the evolution of Au n P À 2 (n = 1-8). Natural bond orbital (NBO) described the charge distribution in stabilizing structures and revealed the strong relativistic effects of the gold atoms.

show abstract

Isomer identification and resolution in small gold clusters

Cited by 88 publications

References 46 publications

Switching from molecular to bulklike dynamics in electronic relaxation of a small gold cluster

Switching from molecular to bulklike dynamics in electronic relaxation of a small gold cluster

Global optimization of clusters using electronic structure methods

Probing the structures and electronic properties of dual-phosphorus-doped gold cluster anions (AunP2-, n= 1–8): A density

Contact Info

Product

Resources

About