Formalism of collective electron excitations in fullerenes

We present a detailed formalism for the description of collective electron excitations in fullerenes in the process of the electron inelastic scattering. Considering the system as a spherical shell of a finite width, we show that the differential cross section is defined by three plasmon excitations, namely two coupled modes of the surface plasmon and the volume plasmon. The interplay of the three plasmons appears due to the electron diffraction of the fullerene shell. Plasmon modes of different angular momenta provide dominating contributions to the differential cross section depending on the transferred momentum.Comment: 11 pages, 2 figures; submitted to the special issue "Atomic Cluster Collisions: Structure and Dynamics from the Nuclear to the Biological Scale" of Eur. Phys. J.

Formalism for Multiphoton Plasmon Excitation in Jellium Clusters

We present a new formalism for the description of multiphoton plasmon excitation processes in jellium clusters. By using our method, we demonstrate that, in addition to dipole plasmon excitations, the multipole plasmons (quadrupole, octupole, etc) can be excited in a cluster by multiphoton absorption processes, which results in a significant difference between plasmon resonance profiles in the cross sections for multiphoton as compared to single-photon absorption. We calculate the cross sections for multiphoton absorption and analyse the balance between the surface and volume plasmon contributions to multipole plasmons.Comment: 29 pages, 1 figur

A Real-Space Full Multigrid study of the fragmentation of Li11+ clusters

We have studied the fragmentation of Li11+ clusters into the two experimentally observed products (Li9+,Li2) and (Li10+,Li) The ground state structures for the two fragmentation channels are found by Molecular Dynamics Simulated Annealing in the framework of Local Density Functional theory. Energetics considerations suggest that the fragmentation process is dominated by non-equilibrium processes. We use a real-space approach to solve the Kohn-Sham problem, where the Laplacian operator is discretized according to the Mehrstellen scheme, and take advantage of a Full MultiGrid (FMG) strategy to accelerate convergence. When applied to isolated clusters we find our FMG method to be more efficient than state-of-the-art plane wave calculations.Comment: 9 pages + 6 Figures (in gzipped tar file

Ab initio studies of structures and properties of small potassium clusters

We have studied the structure and properties of potassium clusters containing even number of atoms ranging from 2 to 20 at the ab initio level. The geometry optimization calculations are performed using all-electron density functional theory with gradient corrected exchange-correlation functional. Using these optimized geometries we investigate the evolution of binding energy, ionization potential, and static polarizability with the increasing size of the clusters. The polarizabilities are calculated by employing Moller-Plesset perturbation theory and time dependent density functional theory. The polarizabilities of dimer and tetramer are also calculated by employing large basis set coupled cluster theory with single and double excitations and perturbative triple excitations. The time dependent density functional theory calculations of polarizabilities are carried out with two different exchange-correlation potentials: (i) an asymptotically correct model potential and (ii) within the local density approximation. A systematic comparison with the other available theoretical and experimental data for various properties of small potassium clusters mentioned above has been performed. These comparisons reveal that both the binding energy and the ionization potential obtained with gradient corrected potential match quite well with the already published data. Similarly, the polarizabilities obtained with Moller-Plesset perturbation theory and with model potential are quite close to each other and also close to experimental data.Comment: 33 pages including 10 figure

Atomic structure and segregation in alkali-metal heteroclusters

The ground-state atomic and electronic distributions in NamCsn clusters with composition m=n and m=2n have been calculated by minimizing the total cluster energy using the density-functional formalism. The approximation is made by replacing the total external potential of the ions by its spherical average around the cluster center during the iterative process of solving the Kohn-Sham equations for each geometry tested. In the size range studied here (up to 90 atoms per cluster), the cluster is composed of well-separated homoatomic Na and Cs shells, the external one always being a Cs shell. We have also found that the cohesive energy goes rapidly to the bulk limit. An analysis of the geometries shows strong cluster reconstruction with increasing size. By comparing the geometry of pure Nan with that of the Nan core in NanCsn for clusters formed by only an inner Na layer and an outer Cs layer, we have observed that the Nan core adopts a geometry different in most cases from that of the free Nan cluster, and such that the number of faces of the polyhedron formed by the Nan core is as close as possible to the number of external Cs atoms, in order to accomodate these Cs atoms on top of the faces of the polyhedron

A far-ultraviolet-driven photoevaporation flow observed in a protoplanetary disk.

Most low-mass stars form in stellar clusters that also contain massive stars, which are sources of far-ultraviolet (FUV) radiation. Theoretical models predict that this FUV radiation produces photodissociation regions (PDRs) on the surfaces of protoplanetary disks around low-mass stars, which affects planet formation within the disks. We report James Webb Space Telescope and Atacama Large Millimeter Array observations of a FUV-irradiated protoplanetary disk in the Orion Nebula. Emission lines are detected from the PDR; modeling their kinematics and excitation allowed us to constrain the physical conditions within the gas. We quantified the mass-loss rate induced by the FUV irradiation and found that it is sufficient to remove gas from the disk in less than a million years. This is rapid enough to affect giant planet formation in the disk

PDRs4All IV. An embarrassment of riches: Aromatic infrared bands in the Orion Bar

(Abridged) Mid-infrared observations of photodissociation regions (PDRs) are dominated by strong emission features called aromatic infrared bands (AIBs). The most prominent AIBs are found at 3.3, 6.2, 7.7, 8.6, and 11.2 $\mu$m. The most sensitive, highest-resolution infrared spectral imaging data ever taken of the prototypical PDR, the Orion Bar, have been captured by JWST. We provide an inventory of the AIBs found in the Orion Bar, along with mid-IR template spectra from five distinct regions in the Bar: the molecular PDR, the atomic PDR, and the HII region. We use JWST NIRSpec IFU and MIRI MRS observations of the Orion Bar from the JWST Early Release Science Program, PDRs4All (ID: 1288). We extract five template spectra to represent the morphology and environment of the Orion Bar PDR. The superb sensitivity and the spectral and spatial resolution of these JWST observations reveal many details of the AIB emission and enable an improved characterization of their detailed profile shapes and sub-components. While the spectra are dominated by the well-known AIBs at 3.3, 6.2, 7.7, 8.6, 11.2, and 12.7 $\mu$m, a wealth of weaker features and sub-components are present. We report trends in the widths and relative strengths of AIBs across the five template spectra. These trends yield valuable insight into the photochemical evolution of PAHs, such as the evolution responsible for the shift of 11.2 $\mu$m AIB emission from class B$_{11.2}$ in the molecular PDR to class A$_{11.2}$ in the PDR surface layers. This photochemical evolution is driven by the increased importance of FUV processing in the PDR surface layers, resulting in a "weeding out" of the weakest links of the PAH family in these layers. For now, these JWST observations are consistent with a model in which the underlying PAH family is composed of a few species: the so-called 'grandPAHs'.Comment: 25 pages, 10 figures, to appear in A&