Pump and probe analysis of metal cluster dynamics

Andrae, K.; Dinh, Phuong Mai; Reinhard, P.‐G.; Suraud, E.

doi:10.1016/j.commatsci.2004.09.062

“…The x and y modes are nearly degenerate due to near axial symmetry of the total system. Pump and probe analysis of the time-dependent plasmon peaks thus provides worthwhile information about the shapes of the embedded cluster, which can be measured by probe pulse as explained in [12,59,14,15]. Note here that the experimental results obtained for Ag clusters in glass [23] are in qualitative agreement with our findings.…”

Section: Possible Pathways To Experimental Analysissupporting

confidence: 82%

“…Indeed, the plasmon couples strongly to light at very specific frequencies and these plasmon frequencies are uniquely related to the cluster shape. For free clusters, we have discussed a rather simple pump-and-probe setup which allows to map in a unique fashion the evolution of radial shape [12], of quadrupole deformations [59] and of elongation in a fission process [14,15]. We have computed that for the case considered here.…”

Section: Possible Pathways To Experimental Analysismentioning

confidence: 99%

“…It provides a strong coupling to photons in a very narrow frequency window which makes clusters an ideal laboratory for laser induced non-linear dynamics [9,10]. The plasmon also serves as a versatile handle for pump and probe experiments [11,12,13,14,15], and it provides the key mechanism in driving the hefty Coulomb explosion of clusters [16,17]. For a recent summary on this great variety of phenomena of the dynamics of free metal clusters, see [18,19].…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Embedded metal cluster in strong laser fields

Fehrer

¹

,

Dinh

²

,

Reinhard

³

et al. 2008

Computational Materials Science

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We discuss microscopic mechanisms of the violent dynamics following strong laser excitation of a metal cluster embedded in a rare gas matrix, taking as test case Na8@Ar434. This covers at least two aspects: first, it represents the typical experimental situation of metal clusters handled in raregas matrices or a finite drop of surrounding raregas material, and second, it serves as a generic test case for highly excited chromophores in inert surroundings addressing questions of energy transport and perturbation of the medium. We simulate the process up to 10 ps using a mixed quantum mechanical (for the electrons) and classical (ions and atoms) approach and analyze the emerging dynamics with respect to all basic constituents: cluster electrons, cluster ions, and matrix atoms. We find several stages of relaxation taking place with time scales from a few fs to over a few ps and much slower processes remaining for long after the simulation. A particularly interesting aspect is that the surrounding raregas material stabilizes a highly charged metal cluster which would otherwise explode without delay.

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“…Under these circumstances, we consider that it should be a reasonable choice to employ the ALDA to describe the Coulomb explosion phenomena. We note that the ALDA has often been employed in laser-atom and laser-molecule interactions in the literature [8,31,9,32,33]. We also note that the limitation of the KLI-SIC method had been pointed out recently, see [34].…”

Section: Choice Of the Exchange-correlation Potentialmentioning

confidence: 79%

Time-dependent density-functional theory simulation for electron–ion dynamics in molecules under intense laser pulses

Kawashita

¹

,

Nakatsukasa

²

,

Yabana

³

2009

J. Phys.: Condens. Matter

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We have developed a simulation method to describe three-dimensional dynamics of electrons and ions in a molecule based on the time-dependent density-functional theory. We solve the time-dependent Kohn-Sham equation for electrons employing the real-space and real-time method, while the ion dynamics are described in classical mechanics by the Ehrenfest method. For an efficient calculation in massively parallel computers, the code is parallelized dividing the spatial grid points. We apply the method to the Coulomb explosion of the H(2)S molecule under an intense and ultrashort laser pulse and investigate the mechanism of the process.

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“…It provides a strong cou-pling to photons in a very narrow frequency window which makes clusters an ideal laboratory for laser induced non-linear dynamics [9,10]. The plasmon also serves as a versatile handle for pump and probe experiments [11,12,13,14,15], and it provides the key mechanism in driving the hefty Coulomb explosion of clusters [16,17]. For a recent summary on this great variety of phenomena of the dynamics of free metal clusters, see [18,19].…”

Section: Introductionmentioning

confidence: 99%

Embedded metal cluster in strong laser fields

Fehrer,

Dinh,

Reinhard

et al. 2007

Preprint

Self Cite

0

View full text Add to dashboard Cite

We discuss microscopic mechanisms of the violent dynamics following strong laser excitation of a metal cluster embedded in a rare gas matrix, taking as test case Na8@Ar434. This covers at least two aspects: first, it represents the typical experimental situation of metal clusters handled in raregas matrices or a finite drop of surrounding raregas material, and second, it serves as a generic test case for highly excited chromophores in inert surroundings addressing questions of energy transport and perturbation of the medium. We simulate the process up to 10 ps using a mixed quantum mechanical (for the electrons) and classical (ions and atoms) approach and analyze the emerging dynamics with respect to all basic constituents: cluster electrons, cluster ions, and matrix atoms. We find several stages of relaxation taking place with time scales from a few fs to over a few ps and much slower processes remaining for long after the simulation. A particularly interesting aspect is that the surrounding raregas material stabilizes a highly charged metal cluster which would otherwise explode without delay.

show abstract

Pump and probe analysis of metal cluster dynamics

Cited by 5 publications

References 13 publications

Embedded metal cluster in strong laser fields

Embedded metal cluster in strong laser fields

Time-dependent density-functional theory simulation for electron–ion dynamics in molecules under intense laser pulses

Embedded metal cluster in strong laser fields

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