Femtosecond Time‐Resolved Geometry Relaxation and Ultrafast Intramolecular Energy Redistribution in Ag<sub>2</sub>Au

Bernhardt, Thorsten M.; Hagen, Jan; Socaciu, Liana D.; Mitrić, Roland; Heidenreich, Andreas; Roux, Jean-Michel; Popolan, Denisia; Vaida, Mihai E.; Wöste, L.; Bonačić‐Koutecký, Vlasta; Jortner, Joshua

doi:10.1002/cphc.200400454

Cited by 36 publications

(37 citation statements)

References 39 publications

(61 reference statements)

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“…Fig. 1a) indicates that in this case the IVR process induced by the internal collision between the terminal Ag and Au atoms has been observed (18). It should be pointed out that, for the probe pulse energy of 6.1 eV, the contribution of the continuum is negligible and therefore NeNePo-ZEKE and NeNePo simulated signals are very close to each other (cf.…”

Section: Ag 3o2supporting

confidence: 57%

“…The experimental setup for temperature-controlled ultrafast NeNePo spectroscopy is described in ref. 18, and here only the main features will be outlined. The charged clusters formed in a sputtering process are steered into a helium-filled quadrupole where clusters are thermalized.…”

Section: Methodsmentioning

confidence: 99%

“…Therefore, the identification of different ultrafast processes such as geometric relaxation, internal vibrational relaxation (IVR), different photoionization pathways, fragmentation, etc. becomes attainable (13)(14)(15)(16)(17)(18)(19). Moreover, optimization of the laser fields permits one to manipulate these processes by favoring or suppressing some of the chosen channels.…”

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confidence: 99%

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Ultrafast dynamics in atomic clusters: Analysis and control

Bonačić‐Koutecký

Mitrić

Werner

et al. 2006

Proc. Natl. Acad. Sci. U.S.A.

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We present a study of dynamics and ultrafast observables in the frame of pump-probe negative-to-neutral-to-positive ion (NeNePo) spectroscopy illustrated by the examples of bimetallic trimers Ag2Au ؊ ͞Ag2Au͞Ag2Au ؉ and silver oxides Ag3O 2 ؊ ͞Ag3O2͞Ag3O 2 ؉ in the context of cluster reactivity. First principle multistate adiabatic dynamics allows us to determine time scales of different ultrafast processes and conditions under which these processes can be experimentally observed. Furthermore, we present a strategy for optimal pump-dump control in complex systems based on the ab initio Wigner distribution approach and apply it to tailor laser fields for selective control of the isomerization process in Na3F2. The shapes of pulses can be assigned to underlying processes, and therefore control can be used as a tool for analysis.ultrafast ab initio dynamics ͉ NeNePo spectroscopy ͉ optimal control I nvestigation of femtosecond dynamical processes in elemental clusters and their control by tailored laser fields are of fundamental importance for learning how the interplay of size, structures, and laser fields can be used to manipulate optical properties and reactivity of these species (1). This research area involving combination of laser-selective femtochemistry (2-5) with the functionality of nanostructures opens new perspectives for basic research and numerous technical applications. In particular, exploration of clusters in the size regime in which each atom counts is attractive, because in this regime structures and the numbers of atoms directly determine size-selective properties (6-12). Another important aspect is that the study of ultrafast dynamics in clusters with finite densities of states allows for separation of time scales of nuclear motion (1). Therefore, the identification of different ultrafast processes such as geometric relaxation, internal vibrational relaxation (IVR), different photoionization pathways, fragmentation, etc. becomes attainable (13-19). Moreover, optimization of the laser fields permits one to manipulate these processes by favoring or suppressing some of the chosen channels. In both contexts, the role of theory is essential from conceptual as well as from predictive point of view.Theory not only determines time scales of different processes and predicts ultrafast observables, but also finds conditions under which they can be experimentally realized (13). Moreover, the analysis of shaped laser pulses and the comparison with experimentally optimized laser fields allows us to identify the underlying processes and therefore to use optimal control (20-23) as the tool for analysis (1,23).In this contribution we address both aspects by showing what we can learn (i) from the pump-probe signals and (ii) from the optimized pulse shapes. We also wish to show that for accurate simulations of pump-probe signals and for developing new control strategies for complex systems, the semiclassical limit of the Liouville formulation of quantum mechanics offers a suitable theoretical approach (1,14,15,23)....

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Section: Ag 3o2supporting

confidence: 57%

Section: Methodsmentioning

confidence: 99%

mentioning

confidence: 99%

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Ultrafast dynamics in atomic clusters: Analysis and control

Bonačić‐Koutecký

Mitrić

Werner

et al. 2006

Proc. Natl. Acad. Sci. U.S.A.

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“…16 Moreover, an anion photoelectron spectroscopy study on Au m Ag n (2 k ¼ m þ n 4) clusters is available only recently. 17 The stability of cationic gold clusters doped with one transition metal atom was investigated by a mass spectrometric analysis of fragments resulting from high fluence irradiation of a cluster beam and the abundance patterns were related to the magic numbers of the electronic shell model for clusters.…”

Section: Introductionmentioning

confidence: 99%

Growth format, electronic architecture, magnetic, and optical properties of aromatic cyclo‐Cu₃Au₃ homotops

Tsipis¹,

Depastas²,

Kefalidis³

2007

J Comput Chem

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Bimetallic Cu(3)Au(3) clusters have been investigated using electronic structure calculation techniques (DFT) to understand their electronic, magnetic, and optical properties as well as the geometrical structures. The most stable homotop is the planar cyclo-[Cu(3)(micro-Au)(3)] form consisting of a triangular positively charged Cu(3) structural core with negatively charged Au atoms occupying exposed positions. This structure is characterized by the maximum number of heterobonds and peripheral positions of Au atoms. Possible growth formats of the cyclo-[Cu(3)(micro-Au)(3)] homotops have been explored following both the edge-capping and the stepwise metal atom substitution mechanism. The bonding pattern along with the density of states (DOS) plots of the cyclo-[Cu(3)(micro-Au)(3)] homotop are thoroughly analyzed and compared with those of the pure cyclo-[Cu(3)(micro-Cu)(3)] and cyclo-[Au(3)(micro-Au)(3)] clusters. Particular attention was paid on the stability of these bimetallic clusters in relation with the ring-shaped electron density distribution (aromaticity). It was found that all 3-membered metal rings exhibit significant aromatic character, which was verified by a number of established criteria of aromaticity, such as structural, energetic, magnetic (NICS profiles), and out-of-plane ring deformability criteria. The NICS (1) values correlate well with the out-of-plane ring deformation energy. Finally, a comprehensive analysis of the optical spectra of the CuAu, Cu(2), and Au(2) diatomics and the cyclo-[Cu(3)(micro-Au)(3)], cyclo-[Cu(3)(micro-Cu)(3)], and cyclo-[Au(3)(micro-Au)(3)] clusters placed the electronic assignments of the optical transitions on a firm footing.

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“…These different electrostatic properties can be used to select one or the other conformer in the logic schemes discussed in Section 3.2 below (see also discussion in Appendix). The alternation Z ⇒ Z' can be achieved either by using different metallic supporters or/and applied voltage, [39][40][41][42] by the optical 'negative ion -to neutral -to positive ion', NeNePo experimental setup [43][44][45][46], or by resonant photoionization. [47] For Z = 0, conformer I has one anchoring Au-N 1 bond and one conventional intermolecular Table 1, that allow to uniquely characterize each conformer.…”

Section: Introductionmentioning

confidence: 99%

Implementation of simple logic gates on gold–ammonia bonding patterns in different charge states

Kryachko

Remacle

2008

Molecular Physics

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Femtosecond Time‐Resolved Geometry Relaxation and Ultrafast Intramolecular Energy Redistribution in Ag₂Au

Cited by 36 publications

References 39 publications

Ultrafast dynamics in atomic clusters: Analysis and control

Ultrafast dynamics in atomic clusters: Analysis and control

Growth format, electronic architecture, magnetic, and optical properties of aromatic cyclo‐Cu₃Au₃ homotops

Implementation of simple logic gates on gold–ammonia bonding patterns in different charge states

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Femtosecond Time‐Resolved Geometry Relaxation and Ultrafast Intramolecular Energy Redistribution in Ag2Au

Cited by 36 publications

References 39 publications

Ultrafast dynamics in atomic clusters: Analysis and control

Ultrafast dynamics in atomic clusters: Analysis and control

Growth format, electronic architecture, magnetic, and optical properties of aromatic cyclo‐Cu3Au3 homotops

Implementation of simple logic gates on gold–ammonia bonding patterns in different charge states

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Product

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Femtosecond Time‐Resolved Geometry Relaxation and Ultrafast Intramolecular Energy Redistribution in Ag₂Au

Growth format, electronic architecture, magnetic, and optical properties of aromatic cyclo‐Cu₃Au₃ homotops