The study of simple metal clusters has burgeoned in the last decade, motivated by the growing interest in the evolution of physical properties from the atom to the bulk solid, a progression passing through the domain of atomic clusters. On the experimental side, the rapid development of new techniques for producing the clusters and for probing and detecting them has resulted in a phenomenal increase in our knowledge of these systems. For clusters of the simplest metals, the alkali and noble metals, the electronic structure is dominated by the number of valence electrons, and the ionic cores are of secondary importance. These electrons are delocalized, and the electronic system exhibits a shell structure that is closely related to the well-known nuclear shell structure. In this article the results from a broad range of experiments are reviewed and compared with theory. Included are the behavior of the mass-abundance spectra, polarizabilities, ionization potentials, photoelectron spectra, optical spectra, and fragmentation phenomena.

The physics of simple metal clusters: experimental aspects and simple models

The jellium model of simple metal clusters has enjoyed remarkable empirical success, leading to many theoretical questions. In this review, we first survey the hierarchy of theoretical approximations leading to the model. We then describe the jellium model in detail, including various extensions. One important and useful approximation is the local-density approximation to exchange and correlation effects, which greatly simplifies self-consistent calculations of the electronic structure. Another valuable tool is the semiclassical approximation to the single-particle density matrix, which gives a theoretical framework to connect the properties of large clusters with the bulk and macroscopic surface properties. The physical properties discussed in this review are the ground-state binding energies, the ionization potentials, and the dipole polarizabilities. We also treat the collective electronic excitations from the point of view of the cluster response, including some useful sum rules.

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The physics of simple metal clusters: self-consistent jellium model and semiclassical approaches

A proper account of core-polarization with pseudopotentials: single valence-electron alkali compounds

Modern aspects of the Jahn-Teller effect theory and applications to molecular problems.

Laser excitation of nanometer-sized atomic and molecular clusters offers various opportunities to explore and control ultrafast many-particle dynamics. Whereas weak laser fields allow the analysis of photoionization, excited-state relaxation, and structural modifications on these finite quantum systems, large-amplitude collective electron motion and Coulomb explosion can be induced with intense laser pulses. This review provides an overview of key phenomena arising from laser-cluster interactions with focus on nonlinear optical excitations and discusses the underlying processes according to the current understanding. A general survey covers basic cluster properties and excitation mechanisms relevant for laser-driven cluster dynamics. Then, after an excursion in theoretical and experimental methods, results for single-photon and multiphoton excitations are reviewed with emphasis on signatures from time- and angular-resolved photoemission. A key issue of this review is the broad spectrum of phenomena arising from clusters exposed to strong fields, where the interaction with the laser pulse creates short-lived and dense nanoplasmas. The implications for technical developments such as the controlled generation of ion, electron, and radiation pulses will be addressed along with corresponding examples. Finally, future prospects of laser-cluster research as well as experimental and theoretical challenges are discussed.

Laser-driven nonlinear cluster dynamics

Absorption spectra of lithium clusters containing four to eight atoms have been measured using depletion spectroscopy. Few intense transitions are observed, always located in two predominant spectral regions, ∼480 and 680 nm. The spectra are interpreted using ab initio configuration interaction (CI) calculations, leading to a complete characterization of the excited states and a straightforward determination of the ground state geometrical structure. Intense transitions are explained by interference effects in the transition amplitude and symmetry considerations. Comparisons with semiclassical models, in which an effective mass correction is introduced, are also presented.

Evolution of the electronic structure of lithium clusters between four and eight atoms

Electric-field-hindered vibrational autoionization in molecular Rydberg states.

The nd Rydberg series of the Na2 molecule have been excited by optical-optical double resonance. The experimental spectra are analysed in the framework of the multichannel quantum defect theory including rotational and vibrational channels. The rovibrational interactions in the Rydberg series are calculated and good agreement with experimental energy levels is obtained. The dynamical aspect of the autoionization process is theoretically investigated and interference effects are discussed for Δν=2 autoionization. The autoionization lifetimes are experimentally measured. Agreement between theory and experiment is only qualitative because the autoionization lifetime of the Δν=2 process depends drastically on the variation of the quantum defects with the intemuclear distance. Moreover, the lifetimes are found to be very sensitive to an external electric field.

MQDT analysis of rovibrational interactions and autoionization in Na2 Rydberg states

The optical-absorption spectrum of Lib has been observed by depletion spectroscopy in the 400-700-nm range. The experimental results are compared with theoretical spectra calculated for the three Li 6 structures in competition and we have been able to unambiguously determine the most stable Li 6 geometry as being the C 2υ tripyramidal geometry

Competition between planar and nonplanar structure in alkali hexamers: The example of Li6.

The optical absorption spectrum of small lithium clusters has been measured up to Li8. In Li3 high resolution Two Photon Ionization (TPI) spectra have been recorded allowing us to determine the geometry and potential surfaces of the ground and excited states. In larger clusters, the excited states are dissociative and the absorption spectra have been obtained by Depletion Spectroscopy. Vibronic resolution is still achieved in Li4, but not in larger clusters. The measured spectra exhibit a rather small number of transitions to electronically excited states. In Li7, only one intense band is observed in the blue region, while in Li8, an intense band is also observed in the blue region and a much weaker band in the red region. All the obtained results are in very good agreement with the ab initio calculation of Bonacic-Koutecky et al. This demonstrates that molecular effects are always present in these small clusters. The semi-classical models of surface plasma resonances are also discussed.

High resolution spectroscopy of small metal clusters

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