Exciton Optical Absorption in Self-Similar Aperiodic Lattices

Exciton optical absorption in self-similar aperiodic one-dimensional systems is considered, focusing our attention on Thue-Morse and Fibonacci lattices as canonical examples. The absorption line shape is evaluated by solving the microscopic equations of motion of the Frenkel-exciton problem on the lattice, in which on-site energies take on two values, according to the Thue-Morse or Fibonacci sequences. Results are compared to those obtained in random lattices with the same stechiometry and size. We find that aperiodic order causes the occurrence of well-defined characteristic features in the absorption spectra which clearly differ from the case of random systems, indicating a most peculiar exciton dynamics. We successfully explain the obtained spectra in terms of the two-center problem. This allows us to establish the origin of all the absorption lines by considering the self-similar aperiodic lattices as composed of two-center blocks, within the same spirit of the renormalization group ideas.Comment: 16 pages in REVTeX 3.0. 2 figures on request to F. D-A ([email protected]

Band-theoretical prediction of magnetic anisotropy in uranium monochalcogenides

Magnetic anisotropy of uranium monochalcogenides, US, USe and UTe, is studied by means of fully-relativistic spin-polarized band structure calculations within the local spin-density approximation. It is found that the size of the magnetic anisotropy is fairly large (about 10 meV/unit formula), which is comparable with experiment. This strong anisotropy is discussed in view of a pseudo-gap formation, of which crucial ingredients are the exchange splitting of U 5f states and their hybridization with chalcogen p states (f-p hybridization). An anomalous trend in the anisotropy is found in the series (US>>USe<UTe) and interpreted in terms of competition between localization of the U 5f states and the f-p hybridization. It is the spin-orbit interaction on the chalcogen p states that plays an essential role in enlarging the strength of the f-p hybridization in UTe, leading to an anomalous systematic trend in the magnetic anisotropy.Comment: 4 pages, 5 figure

Orientational self-sorting in cuboctahedral Pd cages

Cuboctahedral coordination cages of the general formula [Pd12L24]24+ (L = low-symmetry ligand) were analyzed theoretically and experimentally. With 350 696 potential isomers, the structural space of these assemblies is vast. Orientational self-sorting refers to the preferential formation of particular isomers within the pool of potential structures. Geometric and computational analyses predict the preferred formation of cages with a cis arrangement at the metal centers. This prediction was corroborated experimentally by synthesizing a [Pd12L24]24+ cage with a bridging 3-(4-(pyridin-4-yl)phenyl)pyridine ligand. A crystallographic analysis of this assembly showed exclusive cis coordination of the 3- and the 4-pyridyl donor groups at the Pd2+ ions

Trace and antitrace maps for aperiodic sequences, their extensions and applications

We study aperiodic systems based on substitution rules by means of a transfer-matrix approach. In addition to the well-known trace map, we investigate the so-called `antitrace' map, which is the corresponding map for the difference of the off-diagonal elements of the 2x2 transfer matrix. The antitrace maps are obtained for various binary, ternary and quaternary aperiodic sequences, such as the Fibonacci, Thue-Morse, period-doubling, Rudin-Shapiro sequences, and certain generalizations. For arbitrary substitution rules, we show that not only trace maps, but also antitrace maps exist. The dimension of the our antitrace map is r(r+1)/2, where r denotes the number of basic letters in the aperiodic sequence. Analogous maps for specific matrix elements of the transfer matrix can also be constructed, but the maps for the off-diagonal elements and for the difference of the diagonal elements coincide with the antitrace map. Thus, from the trace and antitrace map, we can determine any physical quantity related to the global transfer matrix of the system. As examples, we employ these dynamical maps to compute the transmission coefficients for optical multilayers, harmonic chains, and electronic systems.Comment: 13 pages, REVTeX, now also includes applications to electronic systems, some references adde

Physical nature of critical wave functions in Fibonacci systems

We report on a new class of critical states in the energy spectrum of general Fibonacci systems. By introducing a transfer matrix renormalization technique, we prove that the charge distribution of these states spreads over the whole system, showing transport properties characteristic of electronic extended states. Our analytical method is a first step to find out the link between the spatial structure of these critical wave functions and the quasiperiodic order of the underlying lattice.Comment: REVTEX 3.0, 11 pages, 2 figures available upon request. To appear in Phys. Rev. Let

Towards Space Deployment of the NDSA Concept for Tropospheric Water Vapour Measurements

A novel measurement concept specifically tuned to monitoring tropospheric water vapour's vertical distribution has been demonstrated on a theoretical basis and is currently under development for space deployment. The NDSA (Normalised Differential Spectral Attenuation) technique derives the integrated water vapour (IWV) along the radio link between a transmitter and a receiver carried by two LEO satellites, using the linear correlation between the IWV and a parameter called spectral sensitivity. This is the normalised incremental ratio of the spectral attenuation at two frequencies in the Ku and K bands, with the slope of the water vapour absorption line at 22.235 GHz. Vertical profiles of WV can be retrieved by inverting a set of IWV measurements acquired in limb geometry at different tangent altitudes. This paper provides a comprehensive insight into the NDSA approach for sounding lower tropospheric WV, from the theoretical investigations in previous ESA studies, to the first experimental developments and testing, and to the latest advancements achieved with the SATCROSS project of the Italian Space Agency. The focus is on the new results from SATCROSS activities; primarily, on the upgrading of the instrument prototype, with improved performance in terms of its power stability and the time resolution of the measurements. Special emphasis is also placed on discussing tomographic inversion methods capable of retrieving tropospheric WV content from IWV measurements, i.e., the least squares and the external reconstruction approaches, showing results with different spatial features when applied to a given atmospheric scenario. The ultimate goal of deploying the NDSA measurement technique from space is thoroughly examined and conclusions are drawn after presenting the results of an Observing System Simulation Experiment conducted to assess the impact of NDSA data assimilation on environmental model simulations

Cross-architecture tuning of silicon and SiGe-based quantum devices using machine learning

The potential of Si and SiGe-based devices for the scaling of quantum circuits is tainted by device variability. Each device needs to be tuned to operation conditions and each device realisation requires a different tuning protocol. We demonstrate that it is possible to automate the tuning of a 4-gate Si FinFET, a 5-gate GeSi nanowire and a 7-gate Ge/SiGe heterostructure double quantum dot device from scratch with the same algorithm. We achieve tuning times of 30, 10, and 92 min, respectively. The algorithm also provides insight into the parameter space landscape for each of these devices, allowing for the characterization of the regions where double quantum dot regimes are found. These results show that overarching solutions for the tuning of quantum devices are enabled by machine learning

Highly Conducting pi-Conjugated Molecular Junctions Covalently Bonded to Gold Electrodes

We measure electronic conductance through single conjugated molecules bonded to Au metal electrodes with direct Au-C covalent bonds using the scanning tunneling microscope based break-junction technique. We start with molecules terminated with trimethyltin end groups that cleave off in situ resulting in formation of a direct covalent sigma bond between the carbon backbone and the gold metal electrodes. The molecular carbon backbone used in this study consist of a conjugated pi-system that has one terminal methylene group on each end, which bonds to the electrodes, achieving large electronic coupling of the electrodes to the pi-system. The junctions formed with the prototypical example of 1,4-dimethylenebenzene show a conductance approaching one conductance quantum (G0 = 2e2/h). Junctions formed with methylene terminated oligophenyls with two to four phenyl units show a hundred-fold increase in conductance compared with junctions formed with amine-linked oligophenyls. The conduction mechanism for these longer oligophenyls is tunneling as they exhibit an exponential dependence of conductance with oligomer length. In addition, density functional theory based calculations for the Au-xylylene-Au junction show near-resonant transmission with a cross-over to tunneling for the longer oligomers.Comment: Accepted to the Journal of the American Chemical Society as a Communication