Geometric and Electronic Structures of Silicon Oxide Clusters

Chu, Tianshu; Zhang, and R. Q.; Cheung, Ho-Fai

doi:10.1021/jp002046k

Cited by 106 publications

(153 citation statements)

References 18 publications

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“…DF calculations have accurately reproduced the properties of silica clusters obtained from both experimental studies and other high-level calculations [8,9]. Cluster geometries were optimized at the AM1 semiempirical level and then further at the B3LYP=6-31G level, imposing no symmetry constraints.…”

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confidence: 86%

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Fully Coordinated Silica Nanoclusters:(SiO2)NMolecular Rings

2003

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A new form of finite silica with edge-sharing SiO 2 units connected in a ring is proposed. High-level density-functional calculations for SiO 2 N , N 4-14, show the rings to be energetically more stable than the corresponding SiO 2 N linear chains for N > 11. The rings display frequency modes in remarkable agreement with infrared bands measured on dehydrated silica surfaces indicating their potential as models of strained extended silica systems. Silica rings, if synthesized, may also be useful precursors for new bulk-silica polymorphs with tubular or porous morphologies.

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confidence: 86%

“…1. For N 1-6, SiO 2 N chains are predicted to be the most thermodynamically stable form of silica, being energetically favored over all other such stoichiometric silica clusters [8,9]. For larger N, two-ring chains of arbitrary length may be formed in the high temperature synthesis of fibrous silica-w [10].…”

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confidence: 99%

Fully Coordinated Silica Nanoclusters:(SiO2)NMolecular Rings

2003

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“…Song and Choi 20 compared the stability of elongated and compact SiO 2 clusters with 12-46 molecules using plane-wave density-functional theory ͑DFT͒ and provided a very good discussion about effects of size, morphology, and different types of silica rings and their electronic and optical properties. Nayak et al 21 studied structure and properties of ͑SiO 2 ͒ n ͑n =1-6͒ and Si 3 O n ͑n =1,3,4͒ employing ab initio methodology, while Zhang et al 19 and Chu et al 22 provided a detailed theoretical study of structures of Si n O m ͑n , m =1-8͒ by the DFT-B3LYP ͑Ref. 23͒ method.…”

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confidence: 99%

Theoretical prediction of atomic and electronic structure of neutral Si6Om (m=1–11) clusters

Caputo

Oña

Ferraro

2009

The Journal of Chemical Physics

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In this paper we found the most stable structures of silicon-oxide clusters of Si 6 O m ͑m =1-11͒ by using the genetic algorithm. In this work the genetic algorithm uses a semiempirical energy function, MSINDO, to find the best cluster structures of Si 6 O m ͑m =1-11͒. The best structures found were further optimized using the density functional theory. We report the stable geometries, binding energies, lowest unoccupied molecular orbital-highest occupied molecular orbital gap, dissociation energies for the most favorable fragmentation channels and polarizabilities of Si 6 O m ͑m =1-11͒. For most of the clusters studied here we report structures not previously found using limited search approaches on common structural motifs.

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“…For DFT calculations the B3LYP hybrid exchangecorrelation functional [12] with a 6 -31G(d) basis set was used, employing no symmetry constraints. This level of theory has been shown in numerous previous studies to be suitable for calculating accurate structures and energies of SiO 2 nanoclusters [13,14]. The GAMESS-UK [15] code was used for all DFT calculations.…”

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Columnar-to-Disk Structural Transition in Nanoscale(SiO2)NClusters

Bromley

Flikkema

2005

Phys. Rev. Lett.

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Extensive large-scale global optimizations refined by ab initio calculations are used to propose SiO 2 N N 14-27 ground states. For N < 23 clusters are columnar and show N-odd-N-even stability, energetically and electronically. At N 23 a columnar-to-disk structural transition occurs reminiscent of that observed for Si N . These transitions differ in nature but have the same basis, linking the nanostructural behavior of an element (Si) and its oxide (SiO 2 ). Considering the impact of devices based on the nanoscale manipulation of Si=SiO 2 the result is of potential technological importance. DOI: 10.1103/PhysRevLett.95.185505 PACS numbers: 61.46.+w, 36.40.Ei, 36.40.Mr, 68.65.2k The technological importance of nanoscale silica (SiO 2 ) can hardly be overstated considering its established utilization in microelectronics, catalysis, and composite materials and its promise in the emerging field of photonics. Although much experimental and theoretical work has focused upon the stabilities and structures of the many silica bulk polymorphs and their surfaces, the low energy structures and potential energy surface (PES) of nanoscale SiO 2 clusters is relatively unknown. In this Letter we provide the beginnings of an energetic baseline of the complex PES of nanoscale SiO 2 by finding the lowest energy forms of silica for SiO 2 N N 14-27 providing new limits on the stability of this centrally important material in the physical, chemical, and geophysical sciences. The clusters we study all have at least one dimension between 1 and 2.5 nm and are all substantially lower in energy than any previously reported. Our results strongly indicate that one-dimensional columnar structures are energetically favored up to a length scale of at least 2 nm where upon a transition to two-dimensional trigonal disklike structures occurs at N 23. The transition is characterized by sharp changes in measures of the structural form, electronic structure, and bonding topology of the cluster series, but appears smooth with respect to cluster energies. The structural transition in SiO 2 N clusters is compared to that known for clusters of its parent element Si N [1]. In both cases for N 23-25 a structural transition from elongated to more compact forms appears to occur in the thermodynamically preferred clusters [2]. Usually oxides and their parent elements display different but complementary physical and chemical properties and typically bear little structural relation to one another. Our finding that, at the nanoscale, the size-dependent structural behavior of SiO 2 and its parent element follow a similar general pattern is at once relatively unexpected and fundamentally suggests an inherent link between the two materials. Because of the immense dependence on the combined structural and physical properties of both nanoscale Si and SiO 2 in electronic and optical devices, our demonstration of such a connection is of potential significant technological importance.Although relatively small, M 20 homogeneous clusters of low atomic weight atoms are...

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Geometric and Electronic Structures of Silicon Oxide Clusters

Cited by 106 publications

References 18 publications

Fully Coordinated Silica Nanoclusters:(SiO2)NMolecular Rings

Fully Coordinated Silica Nanoclusters:(SiO2)NMolecular Rings

Theoretical prediction of atomic and electronic structure of neutral Si6Om (m=1–11) clusters

Columnar-to-Disk Structural Transition in Nanoscale(SiO2)NClusters

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