Theoretical study of the finite temperature spectroscopy in van der Waals clusters. III Solvated Chromophore as an effective diatomics

The absorption spectroscopy of calcium-doped argon clusters is described in terms of an effective diatomics molecule Ca-(Ar_n), in the framework of semiclassical vertical transitions. We show how, upon choosing a suitable reaction coordinate, the effective finite-temperature equilibrium properties can be obtained for the ground- and excited-surfaces from the potential of mean force (PMF). An extension of the recent multiple range random-walk method is used to calculate the PMF over continuous intervals of distances. The absorption spectra calculated using this single-coordinate description are found to be in good agreement with the spectra obtained from high-statistics Monte Carlo data, in various situations. For CaAr$_{13}$, we compare the performances of two different choices of the reaction coordinate. For CaAr_37, the method is seen to be accurate enough to distinguish between different low-energy structures. Finally, the idea of casting the initial many-body problem into a single degree of freedom problem is tested on the spectroscopy of calcium in bulk solid argon.Comment: 8 pages, 9 figure

Theoretical study of finite temperature spectroscopy in van der Waals clusters. II Time-dependent absorption spectra

Using approximate partition functions and a master equation approach, we investigate the statistical relaxation toward equilibrium in selected CaAr$_n$ clusters. The Gaussian theory of absorption (previous article) is employed to calculate the average photoabsorption intensity associated with the 4s^2-> 4s^14p^1 transition of calcium as a function of time during relaxation. In CaAr_6 and CaAr_10 simple relaxation is observed with a single time scale. CaAr_13 exhibits much slower dynamics and the relaxation occurs over two distinct time scales. CaAr_37 shows much slower relaxation with multiple transients, reminiscent of glassy behavior due to competition between different low-energy structures. We interpret these results in terms of the underlying potential energy surfaces for these clusters.Comment: 10 pages, 9 figure

Theoretical study of finite temperature spectroscopy in van der Waals clusters. I. Probing phase changes in CaAr_n

The photoabsorption spectra of calcium-doped argon clusters CaAr_n are investigated at thermal equilibrium using a variety of theoretical and numerical tools. The influence of temperature on the absorption spectra is estimated using the quantum superposition method for a variety of cluster sizes in the range 6<=n<=146. At the harmonic level of approximation, the absorption intensity is calculated through an extension of the Gaussian theory by Wadi and Pollak [J. Chem. Phys. vol 110, 11890 (1999)]. This theory is tested on simple, few-atom systems in both the classical and quantum regimes for which highly accurate Monte Carlo data can be obtained. By incorporating quantum anharmonic corrections to the partition functions and respective weights of the isomers, we show that the superposition method can correctly describe the finite-temperature spectroscopic properties of CaAr_n systems. The use of the absorption spectrum as a possible probe of isomerization or phase changes in the argon cluster is discussed at the light of finite-size effects.Comment: 17 pages, 9 figure

Manipulation of single-photon states encoded in transverse spatial modes: possible and impossible tasks

Controlled generation and manipulation of photon states encoded in their spatial degrees of freedom is a crucial ingredient in many quantum information tasks exploiting higher-than-two dimensional encoding. Here, we prove the impossibility to arbitrarily modify $d$-level state superpositions (qu$d$its) for $d>2$, encoded in the transverse modes of light, with optical components associated to the group of symplectic transforms (Gaussian operations). Surprisingly, we also provide an explicit construction of how non-Gaussian operations acting on mode subspaces do enable to overcome the limit $d=2$. In addition, this set of operations realizes the full SU(3) algebra.Comment: Published in PR

Spin and Orbital angular momentum propagation in anisotropic media: theory

This paper is devoted to study the propagation of light beams carrying orbital angular momentum in optically anisotropic media. We first review some properties of homogeneous anisotropic media, and describe how the paraxial formalism is modified in order to proceed with a new approach dealing with a general setting of paraxial propagation along uniaxial inhomogeneous media. This approach is suitable for describing the space-variant-optical-axis phase plates

Uniform non-stoichiometric titanium nitride thin films for improved kinetic inductance detector array

We describe the fabrication of homogeneous sub-stoichiometric titanium nitride films for microwave kinetic inductance detector (mKID) arrays. Using a 6 inch sputtering target and a homogeneous nitrogen inlet, the variation of the critical temperature over a 2 inch wafer was reduced to <25 %. Measurements of a 132-pixel mKID array from these films reveal a sensitivity of 16 kHz/pW in the 100 GHz band, comparable to the best aluminium mKIDs. We measured a noise equivalent power of NEP = 3.6e-15 W/Hz^(1/2). Finally, we describe possible routes to further improve the performance of these TiN mKID arrays.Comment: 7 pages, 4 figures, submitted to Journal of low temperature physics, Proceedings of LTD-1

Measuring two-photon orbital angular momentum entanglement

We put forward an approach to estimate the amount of bipartite spatial entanglement of down-converted photon states correlated in orbital angular momentum and the magnitude of the transverse (radial) wave vectors. Both degrees of freedom are properly considered in our framework, which only requires azimuthal local linear optical transformations and mode selection analysis with two fiber detectors. The coincidence distributions predicted by our approach give an excellent fit to the distributions measured in a recent experiment aimed to show the very high-dimensional transverse entanglement of twin photons from a down-conversion source. Our estimate for the Schmidt number is substantially lower but still confirms the presence of high-dimensional entanglement.Comment: Extended paper of a published version in PRA, with some extra appendice