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Register a new userCollective dipole excitations in sodium clusters
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Added by
Apolodor Aristotel Raduta
Publication date
2011
fields
Physics
and research's language is
English
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Some properties of small and medium sodium clusters are described within the RPA approach using a projected spherical single particle basis. The oscillator strengths calculated with a Schiff-like dipole transition operator and folded with Lorentzian functions are used to calculate the photoabsorbtion cross section spectra. The results are further employed to establish the dependence of the plasmon frequency on the number of cluster components. Static electric polarizabilities of the clusters excited in a RPA dipole state are also calculated. Comparison of our results with the corresponding experimental data show an overall good agreement.
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Photoionization studies of Na20 and Na92 clusters are carried out in a framework of linear response density functional theory. Cross sections show substantial spillover of plasmon resonances to the near-threshold ionization energies which are in reasonable agreements with measurements. The analysis of the oscillator strength, consumed by the cross section, lends further insights. The many-body interaction induced self-consistent field from density fluctuations suggests the existence of an attractive force. This may cause time-delayed plasmonic photoemissions in ultrafast measurements. At the waning end of the plasmon structure, a strong minimum in the cross sections from a correlation-driven coherence effect is predicted which can possibly be observed by the photoelectron spectroscopy.
Cryogenic cluster beam experiments have provided crucial insights into the evolution of the metallic state from the atom to the bulk. Surprisingly, one of the most fundamental metallic properties, the ability of a metal to efficiently screen electric fields, is still poorly understood in small clusters. Theory has predicted that many small Na clusters are unable to screen charge inhomogeneities and thus have permanent dipole moments. High precision electric deflection experiments on cryogenically cooled Na$_N$ ($N<200$) clusters show that the electric dipole moments are at least an order of magnitude smaller than predicted, and are consistent with zero, as expected for a metal. The polarizabilities of Na clusters also show metal spheroid behavior, with fine size oscillations caused by the shell structure.
The fission of highly charged sodium clusters with fissilities X>1 is studied by {em ab initio} molecular dynamics. Na_{24}^{4+} is found to undergo predominantly sequential Na_{3}^{+} emission on a time scale of 1 ps, while Na_{24}^{Q+} (5 leq Q leq 8) undergoes multifragmentation on a time scale geq 0.1 ps, with Na^{+} increasingly the dominant fragment as Q increases. All singly-charged fragments Na_{n}^{+} up to size n=6 are observed. The observed fragment spectrum is, within statistical error, independent of the temperature T of the parent cluster for T leq 1500 K. These findings are consistent with and explain recent trends observed experimentally.
The induced polarization of a beam of polar clusters or molecules passing through an electric or magnetic field region differs from the textbook Langevin-Debye susceptibility. This distinction, which is important for the interpretation of deflection and focusing experiments, arises because instead of acquiring thermal equilibrium in the field region, the beam ensemble typically enters the field adiabatically, i.e., with a previously fixed distribution of rotational states. We discuss the orientation of rigid symmetric-top systems with a body-fixed electric or magnetic dipole moment. The analytical expression for their adiabatic-entry orientation is elucidated and compared with exact numerical results for a range of parameters. The differences between the polarization of thermodynamic and adiabatic-entry ensembles, of prolate and oblate tops, and of symmetric-top and linear rotators are illustrated and identified.
Collective plasma excitations in moire flat bands display unique properties reflecting strong electron-electron interactions and unusual carrier dynamics in these systems. Unlike the conventional two-dimensional plasmon modes, dispersing as $sqrt{k}$ at low frequencies and plunging into particle-hole continuum at higher frequencies, the moire plasmons pierce through the flat-band continuum and acquire a strong over-the-band character. Due to the complex structure of the moire superlattice unit cell, the over-the-band plasmons feature several distinct branches connected through zone folding in the superlattice Brillouin zone. Using a toy Hubbard model for the correlated insulating order in a flat band, we predict that these high-frequency modes become strongly dipole-active upon the system undergoing charge ordering, with the low-frequency modes gapped out within the correlated insulator gap. Strong dipole moments and sensitivity to charge order make these modes readily accessible by optical measurements, providing a convenient diagnostic of the correlated states.
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