First-Principles Interatomic Potential of Silica Applied to Molecular Dynamics

Tsuneyuki, Shinji; Tsukada, Masaru; Aoki, Hideo; Matsui, Yoshito

doi:10.1103/physrevlett.61.869

Cited by 595 publications

(389 citation statements)

References 15 publications

Supporting

Mentioning

367

Contrasting

Unclassified

Order By: Relevance

“…However, existing force fields for silica 34,35,36,37 were parameterized to describe primarily its bulk physical properties correctly, and then refined to reproduce the geometry of the silica surface, 38 but the force fields were not validated to describe interactions with biopolymers in aqueous solution. Furthermore, the fuctional form for the potential energy in available force fields is not compatible with the water models used in biomolecular simulations, i.e., TIP3P 39 or SPC.…”

Section: Introductionmentioning

confidence: 99%

Water−Silica Force Field for Simulating Nanodevices

2006

View full text Add to dashboard Cite

Amorphous silica is an inorganic material that is central for many nanotechnology appplications, such as nanoelectronics, microfluidics, and nanopore technology. In order to use molecular dynamics (MD) simulations to study the behavior of biomolecules with silica, we developed a force field for amorphous silica surfaces based on their macroscopic wetting properties that is compatible with the CHARMM force field and TIP3P water model. The contact angle of a water droplet with silica served as a criterion to tune the intermolecular interactions. The resulting force field was used to study the permeation of water through silica nanopores, illustrating the influence of the surface topography and the intermolecular parameters on permeation kinetics. We find that minute modeling of the amorphous surface is critical for MD studies, since the particular arrangement of surface atoms controls sensitively electrostatic interactions between silica and water.

show abstract

Section: Introductionmentioning

confidence: 99%

Water−Silica Force Field for Simulating Nanodevices

2006

View full text Add to dashboard Cite

show abstract

“…Force field studies have focused on quartz, 68,457,473,499,542,587,588,[590][591][592][593]619,620 and cristobalite. 559,594 De Leeuw et al studied the -(0001) hydroxylated quartz-water interface.…”

Section: Crystalline Silicas-liquid Water Interfacementioning

confidence: 99%

Silica Surface Features and Their Role in the Adsorption of Biomolecules: Computational Modeling and Experiments

et al. 2013

View full text Add to dashboard Cite

show abstract

“…Such factors, especially when considering a real material, make it particularly crucial that a well-parameterized potential set be employed to accurately represent the complex PES. For nanoscale silica we have found that commonly used bulk-parameterized potentials [5,6] are less accurate for small cluster systems [7]. The reason for this nanoscale breakdown is mainly due to the occurrence of defect states in nanocale SiO 2 not commonly found in bulk silica (e.g., Si 2 O 2 two-rings, Si --O terminations).…”

mentioning

confidence: 99%

“…The reason for this nanoscale breakdown is mainly due to the occurrence of defect states in nanocale SiO 2 not commonly found in bulk silica (e.g., Si 2 O 2 two-rings, Si --O terminations). In order to more accurately represent the PES of small silica clusters we have thus developed our own specifically parameterized potential set [7] which retains the two-body Buckingham form complemented with electrostatics, as successfully used in bulk parameterized SiO 2 potentials [5,6]. Although our potential has been instrumental in successfully obtaining ground state candidates for SiO 2 N N 6-12 [8] and for identifying the structures of magic SiO 2 8 -based magic clusters observed in laser ablation experiments [9]-for the significantly larger SiO 2 N N 14-27 clusters studied herein we also used the bulk-parameterized potential from Ref.…”

mentioning

confidence: 99%

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

Bromley

Flikkema

2005

Phys. Rev. Lett.

View full text Add to dashboard Cite

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...

show abstract

First-Principles Interatomic Potential of Silica Applied to Molecular Dynamics

Cited by 595 publications

References 15 publications

Water−Silica Force Field for Simulating Nanodevices

Water−Silica Force Field for Simulating Nanodevices

Silica Surface Features and Their Role in the Adsorption of Biomolecules: Computational Modeling and Experiments

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

Contact Info

Product

Resources

About