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Renaud Papoular

Publications and source records attributed to Renaud Papoular.

At least 19 recordsLinked to original sources
arXiv2020

On the visible continuum and bands in the interstellar extinction curve II

Any distortion of a chemical structure causes new features to appear in the absorption spectrum of the structure, especially in the visible and near UV (see Paper I). Chemical modeling, using molecular orbital theory, showed that the continuum resulting from the accumulation of weak new bands in that range, correctly mimics the continuum measured in the laboratory on pure synthesized silicates, in the transparency spectral range, as well as in the InterStellar extinction curve in the same range. The present paper explores in more detail the strong discrete bands that emerge from the continuum due to distortion. It is found that different types of structure (linear or compact, carbon- or silicon-bearing) have each a limited number of strong, characteristic, bands at different wavelengths. Distortion is only one instance of ``defects'' that enrich the vis/UV absorption spectrum; others are: vacancies and voids, substitutions, inclusions in interstices, impurities, dangling bonds. The accumulation of these result in an ``amorphous'' structural state. Several examples of known amorphous materials, both carbon- and silicon-bearing, that have been analyzed in the laboratory, and simulated theoretically, are described below, thus extending the scope of this work. A final section lists several fields of astrophysics that have used, or may use, amorphous models of dust.

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arXiv2019

On the visible continuum and lines in the Interstellar Extinction Curve

This work purports to help understand the InterStellar Extinction Curve in and near the visible range. In this range, crystalline materials are known to be transparent, so amorphous dust is needed. Molecular modeling experiments are used to compute the electronic spectra of various, relatively large, carbon and silicate structures. Hardly any transition shows up beyond 0.4 mum when the structure is in its ground state (the lowest, most stable state, usually crystalline). This is no longer the case as soon as the structure is distorted in any way. Examples of simulated distortions (or ``defects'') are: angular or linear bond alteration, insertion of free radicals near the main structure, dangling bonds; their cumulative effects lead to the amorphous state. It is shown that, in this state, a structure bears a majority of weak transitions and a minority of strong ones. As the structure grows in size, the former ultimately form a weak continuum already detected experimentally, in the visible, on amorphous carbons and silicates. The stronger transitions will manage to emerge above the continuum, especially when they bunch together by chance near the same wavelength. Parallels are drawn between several properties of the computed continua and transitions and the observed continuum and Diffuse Interstellar Bands.

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arXiv2018

A new interpretation of Serkowski's polarization law

The basic tenets of the alternative interpretation to be presented here are that the spectral profiles of the star light polarization peaks observed in the visible and near IR are a result of the optical properties of silicate grains in the same spectral range, not of the grain size, provided it remains within the range of Rayleigh's approximation. The silicate properties are those obtained experimentally by Scott and Duley \cite{sco} for the non-iron bearing \bf amorphous \rm forsterite and enstatite. The whole range of observed Serkowski polarization profiles can be simulated with mixtures made of forsterite plus an increasing fraction (0 to 0.5) of enstatite as the spectral peak shifts from 0.8 to 0.3 $μ$m. Fits to individual observed polarization spectra are also demonstrated. The optical extinction of silicates in the vis/IR (the "transparency range") can be understood by analogy with the thoroughly studied amorphous hydrogenated carbons and amorphous silica. It is due to structural disorder (dangling bonds and coordination defects) and impurities, which give rise to electronic states in the forbidden gap of semi-conductors. Because they are partially localized, their extinction power is dramatically reduced and has been ignored or simply described by a low, flat plateau. As their number density depends on the environment, one expects variations in the ratio of optical extinction coefficients in the visible and mid-IR.

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arXiv2017

On interstellar light polarization by diamagnetic silicate and carbon dust in the infrared

The motion of diamagnetic dust particles in interstellar magnetic fields is studied numerically with several different sets of parameters. Two types of behavior are observed, depending on the value of the critical number $R$, which is a function of the grain inertia, the magnetic susceptibility of the material and of the strength of rotation braking. If $R\leq10$, the grain ends up in a static state and perfectly aligned with the magnetic field, after a few braking times. If not, it goes on precessing and nutating about the field vector for a much longer time. Usual parameters are such that the first situation can hardly be observed. Fortunately, in the second and more likely situation, there remains a persistent partial alignment which is far from negligible, although it decreases as the field decreases and as $R$ increases. The solution of the complete equations of motion of grains in a field helps understanding the details of this behavior. One particular case of an ellipsoidal forsterite silicate grain is studied in detail and shown to polarize light in agreement with astronomical measurements of absolute polarization in the infrared. Phonons are shown to contribute to the progressive flattening of extinction and polarization towards long wavelengths. The measured dielectric properties of forsterite qualitatively fit the Serkowski peak in the visible.

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arXiv2017

Candidate dust structures for starlight polarization

Rotation damping and alignment are discussed as prerequisites for polarization power. An expression is derived from first principles, for the damping time of the rotation of a particle in a magnetic field, under the Faraday braking torque, provided its electrical properties are known. This makes it possible to describe mathematically, in great detail, the motion of the particle and determine its ultimate state of motion, if a steady state is possible at all. This work defines, first, the necessary condition for the Faraday braking to be effective: a) the net electronic charge distribution should not be uniform throughout; b) the number of vibration modes should exceed a few tens. Resonance of rotation frequency with any of these modes is not a requirement. For alignment to be possible, the ratio of gyroscopic and conservative magnetic to non-conservative (retarding) magnetic torques must be low. Either dia-, para- or ferro-magnetism can do, and a small susceptibility is enough and even preferable. This opens up a wide spectrum of possible candidates. A few examples are given.

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arXiv2016

On the dissipation of the rotation energy of dust grains in interstellar magnetic fields

A new mechanism is described, analyzed and visualized, for the dissipation of suprathermal rotation energy of molecules in magnetic fields, a necessary condition for their alignment. It relies upon the Lorentz force perturbing the motion of every atom of the structure, as each is known to carry its own net electric charge because of spatial fluctuations in electron density. If the molecule is large enough that the frequency of its lowest-frequency phonon lies near or below the rotation frequency, then the rotation couples with the molecular normal modes and energy flows from the former to the latter. The rate of this exchange is very fast, and the vibrational energy is radiated away in the IR at a still faster rate, which completes the removal of rotation energy. The energy decay rate scales like the field intensity, the initial angular velocity, the number of atoms in the grain and the inverse of the moment of inertia. It does not depend on the susceptibility. Here, the focus is on carbon-rich molecules which are diamagnetic. The same process must occur if the molecule is paramagnetic or bathes in an electric field instead. A semi-empirical method of chemical modeling was used extensively to illustrate and quantify these concepts as applied to a hydrocarbon molecule. The motion of a rotating molecule in a field was monitored in time so as to reveal the energy transfer and visualize the evolution of its orientation towards the stable configuration.

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arXiv2015

Molecular phonons and their absorption/emission spectra from the far IR to microwaves

Together with their fingerprint modes, molecules carry coherent vibrations of all their atoms (phonons). Phonon spectra extend from $\sim$20 to more than $10^{4}\,μ$m, depending on molecular size. These spectra are discrete but large assemblies of molecules of the same family, differing only by minor structural details, will produce continua. As such assemblies are expected to exist in regions where dust accumulates, they are bound to contribute to the observed continua underlying the Unidentified Infrared Bands and the 21-mum band of planetary nebulae as well as to the diffuse galactic emission surveyed by the Planck astronomical satellite and other means. The purpose of this work is to determine, for carbon-rich molecules, the intensity of such continua and their extent into the millimetric range, and to evaluate their detectability in this range. The rules governing the spectral distributions of phonons are derived and shown to differ from those which obtain in the solid state. Their application allow the extinction cross-section per H atom, and its maximum wavelength, to be determined as a function of molecular size and dimensionality. Chemical modeling of more than 15 large molecules illustrate these results. It is found that the maximum phonon wavelength of a 2D structure increases roughly as the square of its larger dimension. Spectral energy distributions were computed as far as 4000 mum, for molecules up to 50 A° in length.

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arXiv2014

Some optical properties of graphite from IR to millimetric wavelengths

Far infrared(FIR) data on the optical properties of graphite are presently lacking. An important step towards filling this gap was taken by Kuzmenko et al. (2008) who measured, on HOPG (Highly Oriented Pyrolitic Graphite) at normal incidence and from 10 to 300 K, the in-plane dielectric functions from 0.3 to 200 mum, and the reflectance between 0.3 and about 300 mum. We show here how, using recent developments of the electron theory of graphene, extended to graphite, it is possible to properly extrapolate the data farther even than 1000 mum, in effect all the way to Direct Current. The plasma frequency as well as the scattering rate of free electrons are shown to both decrease with T, but level off near 0 K, in agreement with theory. Along the way, we noticed significant discrepancies with the well-known and often used derivation of Philipp (1977) at room temperature, and also with previous data on temperature dependence and absorbance of graphitic material samples in different physical forms. Possible reasons for these discrepancies are discussed. Finally, the absorption efficiency of small graphitic spheres is deduced for the spectral range from 0.3 to 10000 mum. This may contribute to the discussion on model dust candidates for recently observed astronomical far infrared emissions.

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arXiv2014

On the carriers of the 3.4-micrometer absorption and emission bands, and their evolution

Based on the results of chemical analysis and simulation of kerogens and immature coals, a large number of chemical structures carrying the 3.4-mum feature were studied by means of computer simulation codes. Further selection criteria were the integrated strength of the absorption lines in the aliphatic stretchings wavelength band, weak IR activity in the aromatic stretching band and absence of notable activity outside the astronomical UIBs (Unidentified Infrared Bands). Most of the structures that were retained can be classed as branched, short and oxygen-bridged CH_{2} chains, and naphtenic chains. Combinations of their absorption spectra deliver spectra comparable to those observed in the sky. Absorption spectra were derived from Normal Mode Analysis. Emission spectra of the same structures were computed by monitoring their overall dipole moment as they vibrate freely in vacuum after excitation. These spectra were then combined in suitable proportions, together with those of aromatic structures, so as to simulate various typical near IR emission spectra observed in the sky.

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arXiv2014

The contribution of CHONS particles to the diffuse high Galactic latitude IR emission

This work purports to model the far infrared gray-body emission in the spectra of high-Galactic-latitude clouds. Several carbonaceous laboratory materials are tested for their fitness as carriers of this modified-black-body emission which, according to data delivered by the Planck satellite, and others before, is best fit with temperature 17.9 K and spectral index beta=1.78. Some of these materials were discarded for insufficient emissivity, others for inadequate beta. By contrast, CHONS clusters (beta=1.4, T=19 K) combine nicely with magnesium silicate (beta=2, T=18.7 K) to give a spectrum which falls well within the observational error bars (total emission cross-section at 250 mum: 8.6 10^{-26} cm^{2} per H atom). Only 15 % of all Galactic carbon atoms are needed for this purpose. The CHONS particles that were considered and described have a disordered (amorphous) structure but include a sizable fraction of aromatic rings, although they are much less graphitized than a-C:H/HAC. They can be seen as one embodiment of ``astronomical graphite" deduced earlier on from the then available astronomical observations. Grain heating by H atom capture is proposed as a contributor to the observed residual emissions that do not follow the dust/HI correlation.

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arXiv2013

On the carbonaceous carriers of IR plateau and continuum emission

This study explores the molecular origins of plateaus and continuum underlying IR and FIR bands emitted by compact nebulae, especially proto-planetary nebulae. Computational organic chemistry codes are used to deliver the vibrational integrated band intensities of various large, typical carbonaceous structures. These spectra are composed of a rather continuous distribution of weak modes from which emerge the fingerprints. The 6 to 18-mu region is interspersed with a great many weak lines, to which the plateaus are assigned. Similarly, the far IR spectrum is ascribed to the phonon (skeletal) spectrum which is readily identified beyond 18 mu. The absorptivities and absorption cross-sections per interstellar H atom deduced from these spectra are comparable with those of laboratory dust analogs and astronomical measurements, respectively. Moreover, the 5-35 mu spectra of two typical Proto-Planetary Nebula were reasonably well simulated with combinations of molecules containing functional groups which carry the 21- and 30-mu bands, and molecules devoid of these but carrying strong phonon spectra. These results may help understand the emergence of plateaus, the origin of continua underlying FIR bands, as well as the composition of circumstellar dust.

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arXiv2012

Simulation of UIB spectra with IR emission from CHONS molecules

The present work purports to identify candidate carriers of the UIBs. This requires a procedure for the computation of the emission spectrum of any given candidate. The procedure used here consists in exciting the carrier into a state of internal vibration, waiting until the system has reached dynamic equilibrium and, then, monitoring the time variations of the overall electric dipole moment associated with this vibration. The emission spectrum is shown to be simply related to the FT of these variations. This procedure was applied to more than 100 different chemical structures, inspired by the exhaustive experimental and theoretical analyses of Kerogens, the terrestrial sedimentary matter, which is known to be mainly composed of C, H, O, N and S atoms. From this data base, 21 structures were extracted, which fall in 4 classes, each of which contributes preferentially to one of the main UIBs. Summing their adequately weighted spectra delivers an emission spectrum which indeed exhibits the main UIB features (allowing for computational errors inherent in the chemical simulation code). By changing the weights, it is possible to change the relative band intensities so as to mimic the corresponding (moderate) changes observed in the sky. The defects of the present simulation are discussed, and directions for improvement are explored.

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arXiv2011

Excitation of Unidentified Infrared Bands by H atom impact

A model was developed for the excitation of the UIBs by H atom impacts in the Interstellar Medium. It builds upon the fact that, in the presence of far UV radiation and hydrocarbon grains, the hydrogen gas will be partially dissociated and the grain surface will be partially hydrogenated and partially covered with free carbon bonds. Under such a statistical equilibrium, H atoms from the gas will recombine with C atoms at the grain surface at some rate. At each recombination, the H atom deposits an energy of about 5 eV in the grain. Half of this is directly converted into vibrational excitation, always distributed in the same way among the most tightly coupled vibration modes of the grain. Absent frequent grain-grain collisions, the only outlet for this energy is IR reemission, part of it in the UIBs, provided the chemical structure of the grains is adequate, and the other part in the continuum. The partition only depends upon the grain size, all grains being assumed to have the same constitution. Only a fraction, about 0.25, of the grains (among the smallest ones) will contribute significantly to the UIBs. It is shown quantitatively that H impacts are generally more efficient excitation agents than UV absorption because of the overwhelming abundance of hydrogen relative to UV photons. Only very close to young bright stars is this no longer true because photon flux then largely exceeds H atom flux. Thus H impacts and FUV absorption are both necessary to understand the variety of observed UIB spectra. The model translates into a small number of equations enabling a quantitative comparison of its predictions with available astronomical observations, which have become exquisitely rich and accurate in the last two decades.

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arXiv2011

Candidate carriers and synthetic spectra of the 21- and 30-mu protoplanetary nebular bands

Computational chemistry is used here to determine the vibrational line spectrum of several candidate molecules. It is shown that the thiourea functional group, associated with various carbonaceous structures (mainly compact and linear aromatic clusters), is able to mimic the 21-$μ$m band emitted by a number of proto-planetary nebulae. The combination of nitrogen and sulphur in thiourea is the essential source of emission in this model: the band disappears if these species are replaced by carbon. The astronomical 21-$μ$m feature extends redward to merge with another prominent band peaking between 25 and 30 $μ$m, also known as the 30-$μ$m band. It is found that the latter can be modelled by the combined spectra of aliphatic chains, made of CH$_{2}$ groups, oxygen bridges and OH groups, which provide the 30-$μ$m emission. The absence of oxygen all but extinguishes the 30-$μ$m emission. The emission between the 21- and 30-$μ$m bands is provided mainly by thiourea attached to linear aromatic clusters. The chemical software reveals that the essential role of the heteroatoms N, S and O stems from their large electronic charge. It also allows to determine the type of atomic vibration responsible for the different lines of each structure, which helps selecting the most relevant structures. A total of 22 structures have been selected here, but their list is far from being exhaustive; they are only intended as examples of 3 generic classes. When background dust emission is added, model spectra are obtained, which are able to satisfactorily reproduce recent observations of proto-planetary nebulae. The relative numbers of atomic species used in this model are typically H:C:O:N:S=53:36:8:2:1.

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arXiv2010

Synthetic spectra of UIBs (2 to 40 mu)

Computational chemistry is used here to build a set of carbonaceous structures whose combined spectra approximately mimic typical UIB (Unidentified Infrared Band) spectra. A large number of relatively small hydrocarbon structures, containing traces of heteroatoms (oxygen, nitrogen and sulfur) were considered, including aliphatic chains, compact and concatenated hexagonal and pentagonal rings. Their ir (infrared) spectra were computed using standard chemistry software. Those which exhibited at least a few lines falling within one of the UIBs, and no significantly strong line outside the observed bands, were retained: in all 35 structures, grouped in 8 families and totalling about 6000 vibrational modes together. Each family exhibits a characteristically different spectrum. Guided by the IRS spectra of the Spitzer satellite, each of the 8 families was given a weight, which was tailored so that the concatenation of all 35 weighted spectra resembled UIB spectra. A typical chemical composition is found to be C:H:O:N:S=1:1.15:0.064:0.0026:0.013. The present procedure allows each structural family to be preferentially assigned to an observed UIB, which helps figuring out the structure of interstellar dust. The essential role of heteroatoms is apparent.

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arXiv2010

An enduring puzzle: the width variations of the 2175 Angstrom extinction band

Graphene, a single infinite, planar, sheet of graphite, has the same dielectric resonances as bulk graphite, but solid state theory indicates that its features are about half as wide. Based on this theory, the dielectric functions of mono- and multi-layer graphenes are deduced and compared with those of terrestrial graphite. The resonance width of an ordered stack of graphenes is found to increase with the number of layers while the central frequency stays constant. This is the basis of the polycrystalline model of the carrier of the 2175 Angstrom interstellar extinction band. In this model, the carrier dust grains derive from parent hydrocarbon grains. As a grain ages in the IS medium, the light atoms are expelled, hexagonal carbon rings lump together into compact planar clusters, which then assemble into stacks of parallel, equidistant, graphene-like layers. This so-called graphitization is well known to occur in the earth or under strong heating. As the number of layers in each stack increases and their relative orientational order improves, the pi resonance width increases asymptotically towards that of terrestrial graphite. Because of the initial random structure of the parent grains, many randomly oriented stacks may coexist in the same grain. Calculations of the dielectric response of this composite medium show that, for such a grain, the width of the extinction efficiency peak follows the same trend as the pi resonance of the average stack, and thus covers the observed range of IS feature widths, at very nearly constant peak frequency.

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arXiv2009

A polycrystalline graphite model for the 2175 Angstrom interstellar extinction band

A random, hydrogen-free, assembly of microscopic sp2 carbon chips, forming a macroscopically homogeneous and isotropic solid, is proposed as a model carrier for the UV interstellar extinction band . The validity of this model is based on the calculation of the Bruggeman average dielectric function of a mixture of the known parallel and perpendicular dielectric functions of graphite. The pi absorption feature of Rayleigh-sized spheres of this mixture falls near 4.6 mu-1 (2175 Angstroms), but its width is 1.5 mu-1, somewhat larger than the astronomically observed average, 1 mu-1. This is confirmed by measurements of the reflectance of an industrial material, polycrystalline graphite. A better fit to the IS feature position and width is obtained with a hypothetical material, having the same dielectric functions as natural graphite, except for less extended wings of the pi resonance. Physically, this could result from changes in the electronic band structure due to previous thermal histories. On this model, the Frolich feature central wavelength depends only on the pi resonance frequency, while its width depends only on the damping constant of the same resonance. This explains the range of observed feature widths at constant feature wavelength.

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