Plasmon response of a quantum-confined electron gas probed by core-level photoemission

We demonstrate the existence of quantized "bulk" plasmons in ultrathin magnesium films on Si(111) by analyzing plasmon-loss satellites in core-level photoemission spectra, recorded as a function of the film thickness d. Remarkably, the plasmon energy is shown to vary as 1/d2 all the way down to three atomic layers. The loss spectra are dominated by the n=1 and n=2 normal modes, consistent with the excitation of plasmons involving quantized electronic subbands. With decreasing film thickness, spectral weight is gradually transferred from the plasmon modes to the low-energy single-particle excitations. These results represent striking manifestations of the role of quantum confinement on plasmon resonances in precisely controlled nanostructures.     

Plasmon satellites in X-ray photoemission spectra

Controversy exists whether plasmon-satellite structure observed in core-level photoemission spectra arises from so-called intrinsic or extrinsic plasmo     

Calorimetry at surfaces using high-resolution core-level photoemission

We have developed a method to measure simultaneously the internal energy of bulk and the first layer atoms of a crystal. The internal energy of bulk and the surface atoms of lithium (110) have been evaluated from 22 K up to above the melting transition, applying the Debye model to the thermal broadening of the respective 1s photoemission lines. Our measurements clearly reveal two phase changes: the known liquid to solid transition and the surface melting, occurring 50 K below the bulk melting point.     

Revisiting the valence-band and core-level photoemission spectra of NiO

We have reexamined the valence-band (VB) and core-level electronic structure of NiO by means of hard and soft x-ray photoemission spectroscopies. The spectral weight of the lowest energy state was found to be enhanced in the bulk sensitive Ni 2p core-level spectrum. A configuration-interaction model including a bound state screening has shown agreement with the core-level spectrum and off- and on-resonance VB spectra. These results identify the lowest energy states in the core-level and VB spectra as the Zhang-Rice (ZR) doublet bound states, consistent with the spin-fermion model and recent ab initio calculations within dynamical mean-field theory. The results indicate that the ZR character first ionization (the lowest hole-addition) states are responsible for transport properties in NiO and doped NiO.     

Splitting of core-level lines in photoemission spectra of transition metal compounds

The multiplet structure of core-electron binding energies in Cr 3s, Cr 3p and Cr 2p levels of CrCl₃ and CrBr₃ compounds has been investigated by X-ray photoelectron spectroscopy. The Cr 3s levels show a doublet splitting (about 4.3?eV) for the main emission in both halides. Satellites features are observed in Cr 3s, 3p and 2p levels at higher binding energies. In the Cr 3s spectrum, the main emission is assigned to unscreened intra-atomic multiplet splittings with correlation-induced satellites. The Cr 3p and 2p spectra can be better explained by the multiplet splitting arising from the interaction between valence band 3d electrons and core p holes in the crystal field. Final state screening (charge-transfer) effects do not play a major role in Cr 3s main emission nor do they affect the satellite structures in a relevant way. This explains why the Cr 3s exchange splitting in chromium halides is proportional to the local magnetic moment.     

Calculated oxygen 1s core-level photoemission spectra from cuprate superconductors

The observed O 1s X-ray photoemission spectra of the cuprate superconductors often exhibit a satellite at a higher binding energy to the main peak. The origin of this satellite is not fully understood. We have done model cluster calculations to investigate the origin of this satellite using the configuration interaction approach. The calculated spectra for the divalent and superconducting cuprates essentially exhibit a single peak. On distorting the cluster in-plane, the peak shifts to higher binding energies. This substantiates a deterioration of the surface leading to the observed satellite structure in the O 1s core-level photoemission spectra of the cuprate superconductors.     

Valence band and core-level photoemission spectra of black phosphorus single crystals

Valence band structures of black phosphorus have been measured by synchrotron-radiation photoemission spectroscopy. The excitation photon-energy dependence of the spectra has provided information about the 3s-3p hybridization. As for inner core-levels, binding energies of 2p and 2s core-levels, $\text{2p}{}_{\mathrm{<mtext>1</mtext><mtext>2</mtext>}}\text{?2p}{}_{\mathrm{<mtext>3</mtext><mtext>2</mtext>}}$ splitting, and the bulk plasmon energy are estimated from X-ray photoemission spectroscopy.     

Plasmon loss structure in synchrotron radiation photoemission from Mg films

Synchrotron radiation excitation has been used to vary the kinetic energy of electrons photoemitted from the 2p core level of polycrystalline magnesium films and the energy-dependence of the accompanying plasmon loss structure has been observed. Difficulties associated with background subtraction are discussed, and it is shown that the method of background subtraction profoundly affects the conclusions drawn from such an experiment on the relative importance of plasmon and single particle excitation mechanisms for electron scattering. Very thin films of Mg have also been studied in an attempt to separate the intrinsic and extrinsic modes of plasmon creation. Although the plasmon loss structure is dependent on film thickness implying a considerable contribution from extrinsic processes, we are not able to observe plasmons excited in the thin film by electrons originating in the substrate core level. The implications of these results are discussed and further experiments suggested.     

Bulk and surface plasmon excitation in X-ray photoemission

A quantitative theory of bulk and surface plasmon excitation by X-ray photoelectrons in thin metallic films is presented. The shape and strength of inelastic peaks in energy spectra are calculated. Their dependence on the point of primary excitation, energy and direction of the outgoing electron is discussed in the case of X-ray photoemission from aluminium.     

Plasmon excitation in the x ray absorption process

A simple approach is developed to study the excitation of a plasmon due to valence electronic correlations in the x ray absorption process. Assuming a complete separation between the core and the valence electrons, we introduce the plasmons in the system Hamiltonian externally according to the Bohm-Pines collective formalism and carry out the corresponding canonical transformations to separate the x ray photonplasmon-electron term. According to our calculations, the relative intensity of the plasmon process with respect to the main absorption, which represents single particle excitations is 0·12 times the interelectronic separation measured in Bohr radii. The theoretical estimates of the plasmon intensity agree satisfactorily with the experimental values for the Mn K and the Re L_III absorption discontinuities. The shape of the plasmon absorption band resembles the main absorption edge, if the wave vector dependence of the plasmon frequency is neglected. The intensity of the second plasmon harmonic is about 3 per cent of the first plasmon satellite spectrum. The electron plasmon interaction modifies the shape of the plasmon spectrum.