First principles electron-correlated calculations of optical absorption in magnesium clusters

Shinde, Ravindra; Shukla, Alok

doi:10.1140/epjd/e2017-80356-6

Cited by 14 publications

(19 citation statements)

References 30 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…This optical behaviour is somewhat different from the case of Ag where only a red-shift is observed when the particle size is increased. 15 The excitation spectrum of the smallest Mg nanoparticle shows similarities with very small nanoclusters between 2-5 and ∼ 10-100 metallic atoms previously studied by correlated wavefunction theory 59 and time-dependent DFT, 36,37 respectively.…”

Section: Optical Absorption Spectra and Hot-carrier Distribution On Mg Nanoclustersmentioning

confidence: 62%

Plasmonic enhancement of molecular hydrogen dissociation on metallic magnesium nanoclusters

2021

View full text Add to dashboard Cite

show abstract

Section: Optical Absorption Spectra and Hot-carrier Distribution On Mg Nanoclustersmentioning

confidence: 62%

Plasmonic enhancement of molecular hydrogen dissociation on metallic magnesium nanoclusters

2021

View full text Add to dashboard Cite

show abstract

“…This optical behaviour is somewhat different from the case of Ag where only a red-shift is observed when the particle size is increased. 15 The excitation spectrum of the smallest Mg nanoparticle shows similarities with very small nanoclusters between 2-5 and ∼ 10-100 metallic atoms previously studied by correlated wavefunction theory 56 and time-dependent DFT, 36,37 re-spectively.…”

Section: A Optical Absorption Spectra and Hot-carrier Distribution On...mentioning

confidence: 63%

Plasmonic enhancement of molecular hydrogen dissociation on metallic magnesium nanoclusters

Douglas-Gallardo,

Box,

Maurer

2021

Preprint

View full text Add to dashboard Cite

Light-driven plasmonic enhancement of chemical reactions on metal catalysts is a promising strategy to achieve highly selective and efficient chemical transformations. The study of plasmonic catalyst materials has traditionally focused on late transition metals such as Au, Ag, and Cu. In recent years, there has been increasing interest in the plasmonic properties of a set of earth-abundant elements such as Mg, which exhibit interesting hydrogenation chemistry with potential applications in hydrogen storage. This work explores the optical, electronic, and catalytic properties of a set of metallic Mg nanoclusters with up to 2057 atoms using time-dependent density functional tight-binding and density functional theory calculations. Our results show that Mg nanoclusters are able to produce highly energetic hot electrons with energies of up to 4 eV. By electronic structure analysis, we find that these hot electrons energetically align with electronic states of physisorbed molecular hydrogen, occupation of which by hot electrons can promote the hydrogen dissociation reaction. We also find that the reverse reaction, hydrogen evolution, can potentially be promoted by hot electrons, but following a different mechanism. Thus, from a theoretical perspective, Mg nanoclusters display very promising behaviour for their use in light promoted storage and release of hydrogen.

show abstract

“…In order to compute the optical absorption spectra, we utilized the ab initio MRSDCI approach, as implemented in the computer program MELD, [23] and described in recent works on the optical properties of clusters. [18,19,20,21] For the purpose, we utilized the geometries of the isomers (quasi-planar, double ring, and chain) presented in Fig. 1, and the cc-pVDZ basis set, which was also used for geometry optimization.…”

Section: Optical Absorption Spectrummentioning

confidence: 99%

“…This process is continued until the calculated absorption spectrum has converged within reasonable limits. [18,19,20,21] We make a few brief comments about the line width γ occurring in the expression for the optical absorption spectrum (see Eq. 2 above).…”

Section: Isomermentioning

confidence: 99%

“…Geometry optimization was carried out using the coupled-cluster-singles-doubles (CCSD) approach, while the optical absorption spectra of various isomers were computed using the multi-reference singles-doubles configuration interaction (MRSDCI) approach, which has been extensively utilized in the group of one of us to study optical properties of conjugated polymers, [11,12,13,14,15] graphene quantum dots, [16,17] along with atomic clusters such as those of boron, [18] aluminium, [19] sodium, [20] and magnesium. [21] 2. Theoretical approach and Computational details…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

First principles study of structural and optical properties of B12 isomers

Bhattacharyya

Boustani

Shukla

2019

Journal of Physics and Chemistry of Solids

Self Cite

View full text Add to dashboard Cite

In this work we undertake a comprehensive numerical study of the ground state structures and optical absorption spectra of isomers of B 12 cluster. Geometry optimization was performed at the coupledcluster-singles-doubles (CCSD) level of theory, employing cc-pVDZ extended basis sets. Once the geometry of a given isomer was optimized, its ground state energy was calculated more accurately at the coupled-cluster-singles-doubles along with perturbative treatment of triples (CCSD(T)) level of theory, employing larger cc-pVTZ basis sets. Thus, our computed values of binding energies of various isomers are expected to be quite accurate. Our geometry optimization reveals eleven distinct isomers, along with their point group, and electronic ground state symmetries. We also performed vibrational frequency analysis on the three lowest energy isomers, and found them to be stable. Therefore, we computed the linear optical absorption spectra of these isomers of B 12 , employing large-scale multi-reference singles-doubles configuration-interaction (MRSDCI) approach, and found a strong structure-property relationship. This implies that the spectral fingerprints of the geometries can be utilized for optical detection, and characterization, of various isomers of B 12 . We also explored the stability of the isomer with with the structure of a perfect icosahedron, with I h symmetry. In bulk boron icosahedron is the basic structural unit, but, our vibrational frequency analysis reveals that it is unstable in the isolated form. We speculate that this instability could be due to Jahn-Teller distortion because five-fold degenerate HOMO orbitals in I h structure are unfilled. academic and practical importance. Thereupon, the mass spectra of alkali-metal, non-metal, carbon and boron clusters were investigated as well as the related magic numbers were determined.[1] For example, among the allotropes of carbon, all sp 2 -types are closely related and have been extensively studied: graphene (flat monoatomic sheet of graphite), spherical fullerenes, and nanotubes.[2] Also for boron, carbon's left neighbor in the periodic table, the landscape of fullerene-like possibilities is just beginning to emerge: from small quasi-planar clusters, spherical cages and nanotubes [3], then to borophene (single atom-thin monolayer sheet of boron atoms) [4].However, the development of non crystalline boron beyond the icosahedral arrangements began in the late eighties with theoretical and experimental studies on small boron clusters. Anderson group [5] carried out the first experimental and theoretical study of bonding and structures in boron cluster ions B n + for (n ≤ 13) in comparison with the well known closo boron hydrides. Further important study on boron clusters was carried out by Kawai and Weare [6] using Car-Parrinello ab initio molecular dynamics simulation. They found that an open 3D structure is more stable than the icosahedral boron. However, Kato et al. [7] investigated boron clusters B n for (n=8-11) using ab initio molecular orbital theory, a...

show abstract

First principles electron-correlated calculations of optical absorption in magnesium clusters

Cited by 14 publications

References 30 publications

Plasmonic enhancement of molecular hydrogen dissociation on metallic magnesium nanoclusters

Plasmonic enhancement of molecular hydrogen dissociation on metallic magnesium nanoclusters

Plasmonic enhancement of molecular hydrogen dissociation on metallic magnesium nanoclusters

First principles study of structural and optical properties of B12 isomers

Contact Info

Product

Resources

About