Characteristics of mass and nuclear charge distributions of229th(nth,f). implications for fission dynamics

The mass and nuclear charge distributions of fission fragments from²²⁹Th(n_{th, f}) have been measured at several kinetic energies with the mass spectrometer Lohengrin (ILL-Grenoble). The average proton e-o effect, which reaches 41%, induces large oscillations in the parameters of the isotopic charge distribution. A comparison of the data from different fissile nuclei shows the importance of the last stage of the process for intrinsic excitations.     

New far infrared measurements of the rotational spectrum of cyanoacetylene HC3N

Several rotational lines of cyanoacetylene in the ground state and the first excited state v7=1 have been measured between 580 and 1100 GHz with a new FIR laser sidebands spectrometer. A global analysis which takes into account the previous measurements on this molecule is performed.     

On the Brownian motion of a massive sphere suspended in a hard-sphere fluid. I. Multiple-time-scale analysis and microscopic expression for the friction coefficient

The Fokker-Planck equation governing the evolution of the distribution function of a massive Brownian hard sphere suspended in a fluid of much lighter spheres is derived from the exact hierarchy of kinetic equations for the total system via a multiple-time-scale analysis akin to a uniform expansion in powers of the square root of the mass ratio. The derivation leads to an exact expression for the friction coefficient which naturally splits into an Enskog contribution and a dynamical correction. The latter, which accounts for correlated collisions events, reduces to the integral of a time-displaced correlation function of dynamical variables linked to the collisional transfer of momentum between the infinitively heavy (i.e., immobile) Brownian sphere and the fluid particles.     

Theoretical and experimental studies of CH3X-Y2 rotational line shapes for atmospheric spectra modelling: application to room-temperature CH3Cl-O2

The case of symmetric tops CH(3)X (X = Br, Cl, F, …) perturbed by non-polar diatoms Y(2) (Y = N(2), O(2), …) is analysed from the viewpoint of theoretical collisional broadening of their rotational lines observed in atmospheric spectra. A semi-classical approach involving an exponential representation of the scattering operator and exact trajectories governed by the isotropic potential is presented. For the first time the active molecule is strictly treated as a symmetric top and the atom-atom interactions are included in the intermolecular potential model. It is shown for the CH(3)Cl-O(2) system that these interactions contribute significantly to the line width for all values of the rotational quantum numbers J and K. Additional testing of modifications required in the semi-classical formalism for a correct application of the cumulant expansion is performed and it is shown that the use of the cumulant average on the rotational states of the perturbing molecule leads to entirely negligible effects for the not very strongly interacting CH(3)Cl-O(2) system. In order to check the theoretical predictions and to extend the scarce experimental data available in the literature to higher values of the rotational quantum numbers, new measurements of room-temperature O(2)-broadened CH(3)Cl rotational lines are carried out by a photomixing continuous-wave terahertz spectrometer. The experimental line widths extracted with a Voigt profile model demonstrate an excellent agreement with theoretical results up to very high J-values (J = 31, 37, 40, 45, 50).     

STM and chemistry: a qualitative molecular orbital understanding of the image of CO on a Pt surface

Theoretical calculations of STM images for isolated carbon monoxide on Pt(111) have been performed. These simulations are directly comparable to experimental data from Eigler's group. They also confirm a strong site dependence of the STM molecular contrast and assign the two experimental STM forms of CO with two distinct binding sites (the top and the bridge sites) which have already been well-characterised by other surface techniques. Moreover, the approach used here allows a detailed understanding of the electronic origin of the STM molecular pattern. Hence, we demonstrate that the CO STM pattern results from the superposition, with interference effects, of two current contributions. The direct through space tunneling process between the tip and the metal surface is decreased by the presence of the adsorbate molecule, but this depression in the current is more or less compensated, depending on the binding site, by the tunnel current mediated by the molecular levels of the adsorbate. The frontier π orbitals of CO have a small contribution to the current and the σ framework has the major influence with the 5σ lone pair (HOMO of CO) and also the low-lying 3σ. These two MO contributions, however, show a destructive interference effect, and this, together with the absence of π current, is responsible for the weak amplitude of the CO STM image.     

Ultimate sensitivity of heterodyne spectrometers

Low noise heterodyne receivers are now used in a large variety of instruments such as radiotelescopes, far infrared laser side bands spectrometers, supersonic nozzle beams Fourier transform spectrometers, lidars or plasmas diagnostics devices. Numerous papers have been devoted to the analysis of heterodyne receivers in the attempt to reach ultimate performances. These previous papers usually retain the restrictive hypothesis of vanishingly small signal powers. Such a condition occurs only in a restrictive number of applications, radioastronomic systems being probably among the most representative examples. Spectroscopic instruments operate usually in a different regime. The signal to be detected consists of a small variation in the source power. The absolute value of this source power largely depends on the available technology in the spectral range of interest. The purpose of this paper is to analyze the behavior of heterodyne detection in the general case. The results apply to a large category of systems including spectroscopic instruments. The influence of crucial parameters such as source power and predetection bandwidth is analysed in details. The theory is experimentally tested on an example of ultra low noise receiver designed for far infrared laser side bands spectroscopy. Some numerical calculations are proposed, illustrating methods for an optimal sizing of receiver's predetection bandwidth and the estimation of ultimate sensitivity of spectrometers.     

Rotational spectroscopy and dynamics of carbonyl sulphide studied by terahertz free induction decays signals

A terahertz time domain spectroscopy experiment is used to study the coherent re-emission after exciting more than 60 energy rotational states of OCS molecules in gas phase. Due to the regular structure of the absorption spectrum of such linear molecules, a set of subsequent pulses separated by 82.6 ps is re-radiated from the vapour and recorded up to 450 ps. A model based on a linear response of the gas and by use of “Maxwell-Bloch” equations has permitted the re-emitted free induced decay to be investigated. Spectroscopic parameters, such as rotational constant, centrifugal distortion coefficient and relaxation times are responsible for the temporal shape and so can be evaluated. The influence of the optical thickness to access the relaxation times is discussed.     

Friction tensor for a pair of Brownian particles: Spurious finite-size effects and molecular dynamics estimates

In this work, we show thatin any finite system, the binary friction tensor for two Brownian particlescannot be directly estimated from an evaluation of the microscopic Green-Kubo formula, involving the time integral of force-force autocorrelation functions. This pitfall is associated with a subtle inversion of the thermodynamic and long-time limits and leads to spurious results for the estimates of the friction matrix based on molecular dynamics simulations. Starting from a careful analysis of the coupled Langevin equations for two interacting Brownian particles, we derive a method to circumvent these effects and extract the binary friction tensor from the correlation function matrix of the instantaneous forces exerted by the bath particles on the fixed Brownian particles, and from the relaxation of the total momentum of the bath in afinite system. The general methodology is applied to the case of two hard or soft Brownian spheres in a bath of light particles. Numerical estimates of the relevant correlation functions and of the resulting self and mutual components of the matrix of friction tensors are obtained by molecular dynamics simulations for various spacings between the Brownian particles. This paper is dedicated to B. Jancovici on the occassion of his 65th birthday.