Ultrafast Hot-Electron Dynamics Observed in<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:msubsup><mml:mrow><mml:mi>Pt</mml:mi></mml:mrow><mml:mrow><mml:mn>3</mml:mn></mml:mrow><mml:mrow><mml:mspace/><mml:mo>−</mml:mo></mml:mrow></mml:msubsup></mml:mrow></mml:math>Using Time-Resolved Photoelectron Spectroscopy

Pontius, N.; Ps, Bechthold; Neeb, M.; Eberhardt, W.

doi:10.1103/physrevlett.84.1132

Cited by 54 publications

(40 citation statements)

References 27 publications

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“…Similar relaxation times have also been observed for Pd and Au nanoparticles [3]. Even the smallest transition metal clusters of Pt, Pd, and Ni show electron relaxation times of about 100 fs [4,5]. Thermalization between the electronic and vibrational system is usually slower ranging to the ps regime.…”

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Photon-Induced Thermal Desorption of CO from Small Metal-Carbonyl Clusters

et al. 2002

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Thermal CO desorption from photoexcited free metal-carbonyl clusters has been resolved in real time using two-color pump-probe photoelectron spectroscopy. Sequential energy dissipation steps between the initial photoexcitation and the final desorption event, e.g., electron relaxation and thermalization, have been resolved for Au 2 ͑CO͒ 2 and Pt 2 ͑CO͒ 5 2 . The desorption rates for the two clusters differ considerably due to the different numbers of vibrational degrees of freedom. The unimolecular CO-desorption thresholds of Au 2 ͑CO͒ 2 and Pt 2 ͑CO͒ 5 2 have been approximated by means of a statistical Rice-Ramsperger-Kassel calculation using the experimentally derived desorption rate constants. DOI: 10.1103/PhysRevLett.88.076102 PACS numbers: 68.43.Vx, 33.80.Eh, 36.40. -c, 42.65.Re Thermal desorption of a molecule from an equilibrated surface takes place due to statistical energy fluctuations among all degrees of freedom. There is a certain probability that energy is accumulated in a specific chemisorptive bond that exceeds the desorption threshold of an adsorbed molecule. As thermal desorption is a statistical process, which is usually described in terms of stochastic time evolution of the energy content of the dissociative mode [1], the desorption rate depends first of all on the desorption threshold and the total number of degrees of freedom. In isolated particles, the energy cannot simply be released to the surrounding by diffusion or heat transport as in solids. Therefore in small metal-adsorbate clusters a finite probability exists to release the energy by thermal electron emission (thermionic emission) or thermal desorption of a ligand molecule after reaching thermal equilibrium. The energy redistributes either into a particular degree of freedom, i.e., a particular electronic state having one electron less, or a dissociative final state.For photon-induced desorption processes, many dissipation steps are involved between the initial energy absorption and final ligand evaporation. Energy dissipation in photoexcited systems proceeds via electron relaxation and vibrational relaxation where the former process is usually faster than electron-vibrational coupling. Inelastic electron-electron scattering with time constants much less than 100 fs have been observed in optically excited bulk metals [2]. Similar relaxation times have also been observed for Pd and Au nanoparticles [3]. Even the smallest transition metal clusters of Pt, Pd, and Ni show electron relaxation times of about 100 fs [4,5]. Thermalization between the electronic and vibrational system is usually slower ranging to the ps regime.Transition metal-carbonyl clusters such as Pt n ͑CO͒ m 2 are excellent candidates to study photon-induced thermal desorption processes. In these clusters decarbonylation thresholds are smaller than both the electron affinity (thermionic emission threshold) and the metal-metal dissociation energy [6,7]. Besides fluorescence, evaporation of a ligand molecule should thus be the only process by which energy can be rele...

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confidence: 50%

Photon-Induced Thermal Desorption of CO from Small Metal-Carbonyl Clusters

et al. 2002

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“…These ideas have motivated a series of TRPES experiments on transition metal cluster anions by Pontius and coworkers. [246][247][248][249][250] For example, Pt 3 -was studied with TRPES using pump and probe pulses with photon energies of 1.5 eV. 248 Near time zero, two-photon photoemission (2PPE) closely matches the contours of a one-photon photoelectron spectrum taken at 3.0 eV, reflecting a relatively constant density of states among unoccupied levels within the excitation window.…”

Section: Anion Intramolecular Electronic Relaxation Dynamicsmentioning

confidence: 99%

Femtosecond Time-Resolved Photoelectron Spectroscopy

2004

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“…Experimentally, time-resolved two-photon photoemission (TR 2PPES) has been applied to measure the electronic lifetimes in metallic nanoparticles and clusters. [11][12][13][14][15][16] Measurements for internal electron thermalization times in silver nanoparticles embedded in a matrix show that the electron relaxation rate increases with decreasing particle size when the particle radius is less than 5 nm.…”

Section: Introductionmentioning

confidence: 99%

Quasiparticle lifetimes in magnesium clusters modeled by self-consistentGWΓcalculations

Zeng

2011

Phys. Rev. B

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Quasiparticle (QP) lifetimes in magnesium clusters are calculated using many-body Green's function theory. We analyze the effect of the self-consistency of the one-particle Green's function G on the calculations and demonstrate the necessity of the implementation of such a self-consistency. Based on hot electron and hot hole lifetimes in Mg40 calculated by the GW Γ method, we find that in the low energy excitation regime, the QP lifetimes are longer than those in the free electron gas with the electron density rs = 2.66 (3s 2 of the bulk Mg) due to the lack of states available for transitions. In the high excitation energy regime, scaled lifetimes of hot electrons converge to the range of 21 to 24 fs eV 2 . Scaled lifetimes of hot holes in this regime are shorter than those of hot electrons and decrease with increasing excitation energies.

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Ultrafast Hot-Electron Dynamics Observed inPt3−Using Time-Resolved Photoelectron Spectroscopy

Cited by 54 publications

References 27 publications

Photon-Induced Thermal Desorption of CO from Small Metal-Carbonyl Clusters

Photon-Induced Thermal Desorption of CO from Small Metal-Carbonyl Clusters

Femtosecond Time-Resolved Photoelectron Spectroscopy

Quasiparticle lifetimes in magnesium clusters modeled by self-consistentGWΓcalculations

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