Switching from molecular to bulklike dynamics in electronic relaxation of a small gold cluster

Stanzel, J.; Neeb, M.; Eberhardt, W.; Lisinetskaya, Polina G.; Petersen, Jens; Mitrić, Roland

doi:10.1103/physreva.85.013201

Cited by 19 publications

(29 citation statements)

References 25 publications

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“…Electronic decay times in small particles are of the order of some 100 fs, e.g. Ag − N [41], Pd − N [42], Al − N [43] and Au − 7 [44], which is close to our result. But all those studies exhibit strong size dependence, in contrast to our measurements which give the same value τ = 350 fs for all products.…”

Section: Discussionsupporting

confidence: 91%

Time-resolved studies on the collapse of magnesium atom foam in helium nanodroplets

et al. 2013

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Magnesium atoms embedded in superfluid helium nanodroplets have been identified to arrange themselves in a metastable network, referred to as foam. In order to investigate the ionization dynamics of this unique structure with respect to a possible light-induced collapse, the femtosecond dual-pulse spectroscopy technique is applied. Around zero optical delay a strong feature is obtained which represents a direct probe of the foam response. We found that upon collapse, ionization is reduced. A particular intensity ratio of the pulses allows us to address either direct ionization or photoactivation of the neutral complexes, thus affecting reaction pathways. A simplified scheme visualizes possible excitation scenarios in accordance with the experimental observations. Contents

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Section: Discussionsupporting

confidence: 91%

Time-resolved studies on the collapse of magnesium atom foam in helium nanodroplets

et al. 2013

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“…The above presented FISH method is suitable for the simulation and control of laser-induced processes, [37,43,54,55] as well as for the simulation of spectroscopic observables such as timeresolved photoelectron spectra [53,56,57] or harmonic emission.…”

Section: Field-induced Surface-hopping (Fish) Methodsmentioning

confidence: 99%

Nonlinear Absorption Dynamics Using Field‐Induced Surface Hopping: Zinc Porphyrin in Water

et al. 2013

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We wish to present the application of our field-induced surface-hopping (FISH) method to simulate nonlinear absorption dynamics induced by strong nonresonant laser fields. We provide a systematic comparison of the FISH approach with exact quantum dynamics simulations on a multistate model system and demonstrate that FISH allows for accurate simulations of nonlinear excitation processes including multiphoton electronic transitions. In particular, two different approaches for simulating two-photon transitions are compared. The first approach is essentially exact and involves the solution of the time-dependent Schrödinger equation in an extended manifold of excited states, while in the second one only transiently populated nonessential states are replaced by an effective quadratic coupling term, and dynamics is performed in a considerably smaller manifold of states. We illustrate the applicability of our method to complex molecular systems by simulating the linear and nonlinear laser-driven dynamics in zinc (Zn) porphyrin in the gas phase and in water. For this purpose, the FISH approach is connected with the quantum mechanical-molecular mechanical approach (QM/MM) which is generally applicable to large classes of complex systems. Our findings that multiphoton absorption and dynamics increase the population of higher excited states of Zn porphyrin in the nonlinear regime, in particular in solution, provides a means for manipulating excited-state properties, such as transient absorption dynamics and electronic relaxation.

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“…By measuring the kinetic energy of the photoelectron the information on the current excited state energy is obtained and by adjusting the time delay the temporal evolution of the excited state can be investigated. This method has successfully been applied to a large variety of systems ranging from organic molecules and bio-chromophores [20,21] to metallic and molecular clusters [22][23][24][25][26][27].…”

Section: Introductionmentioning

confidence: 99%

“…Recently, the field-induced surface hopping (FISH) method has been developed [28,29] and implemented in the frame of the linear-response time-dependent density functional theory (TDDFT). This allowed for simulation of TRPES [25,30,31] and time-resolved harmonic generation signals in metal clusters [7].…”

Section: Introductionmentioning

confidence: 99%

Excited state nonadiabatic dynamics of bare and hydrated anionic gold clusters Au₃⁻[H₂O]_n (n = 0–2)

Lisinetskaya

Braun

Proch

et al. 2016

Phys. Chem. Chem. Phys.

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We present a joint theoretical and experimental study of the excited state dynamics in pure and hydrated anionic gold clusters AuWe employ mixed quantum-classical dynamics combined with femtosecond time-resolved photoelectron spectroscopy in order to investigate the influence of hydration on excited state lifetimes and the photo-dissociation dynamics.Gradual decrease of the excited state lifetime with the number of adsorbed water molecules as well as gold cluster fragmentation quenching by two or more water molecules are observed both in experiment and in simulations. Non-radiative relaxation and dissociation in excited states are found to be responsible for the excited state population depletion. Time constants of these two processes strongly depend on the number of water molecules leading to the possibility to modulate excited state dynamics and fragmentation of the anionic cluster by adsorption of water molecules.

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Switching from molecular to bulklike dynamics in electronic relaxation of a small gold cluster

Cited by 19 publications

References 25 publications

Time-resolved studies on the collapse of magnesium atom foam in helium nanodroplets

Time-resolved studies on the collapse of magnesium atom foam in helium nanodroplets

Nonlinear Absorption Dynamics Using Field‐Induced Surface Hopping: Zinc Porphyrin in Water

Excited state nonadiabatic dynamics of bare and hydrated anionic gold clusters Au₃⁻[H₂O]_n (n = 0–2)

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Switching from molecular to bulklike dynamics in electronic relaxation of a small gold cluster

Cited by 19 publications

References 25 publications

Time-resolved studies on the collapse of magnesium atom foam in helium nanodroplets

Time-resolved studies on the collapse of magnesium atom foam in helium nanodroplets

Nonlinear Absorption Dynamics Using Field‐Induced Surface Hopping: Zinc Porphyrin in Water

Excited state nonadiabatic dynamics of bare and hydrated anionic gold clusters Au3−[H2O]n (n = 0–2)

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Excited state nonadiabatic dynamics of bare and hydrated anionic gold clusters Au₃⁻[H₂O]_n (n = 0–2)