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Spectral features of presolar diamonds in the laboratory and in carbon star atmospheres

Spectral features of presolar diamonds in the laboratory and in carbon star atmospheres

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A&A manuscript no.
(will be inserted by hand later)
Your thesaurus codes are:08.01.3 - 08.03.1 - 08.01.1 - 13.09.6
Spectral features of presolar diamonds in the laboratoryand in carbon star atmospheres
Anja C.Andersen
, Uffe Gr˚ae rgensen
, Flemming M.Nicolaisen
, Preben Gr˚ae rensen
, and Kris-tian Glejbøl
Astronomisk Observatorium, Juliane Maries Vej 30, DK–2100 Copenhagen, Denmark
Institute of Chemistry, Universitetsparken 5, DK–2100 Copenhagen, Denmark
Physics Institute, Technical University of Denmark, DK–2800 Lyngby, Denmark
NKT Research Center A/S, Sognevej 11, DK–2605 Brøndby, DenmarkReceived date; accepted date
Laboratory analyses on fine-grained diamondresidues from primitive meteorites have shown that nano-diamonds represent the most abundant form of presolardust preserved in meteoritic samples. The presolar di-amonds carry isotopic anomalies which indicate a verycomplex formation history. Several groups of diamondsmay exist with origin in different types of stars. In orderto identify the sites of formation observationally, we haveextracted presolar diamonds from the Allende meteoriteand measured the monochromaticabsorption coefficient ina form which is useful for stellar atmosphere calculations.The monochromatic absorption coefficient was measuredin the wavelength ranges 400–4000 cm
m) and12200–52600 cm
(190–820 nm). We have made iden-tical laboratory measurements on CVD diamonds as onthe meteoritic diamonds, in order to get a more solid ba-sis for the interpretation of the diamond spectrum. Themonochromatic absorption coefficient for the presolar dia-monds wasincorporatedin self-consistent carbon star pho-tospheric models. The main influence of the diamond dustin our photospheric models is a heating of the upper pho-tospheric layers and a reduction of the C
abundance.Due to the relatively small absorption coefficient of the di-amonds compared to other stellar dust grains, their spec-tral appearance is weak. However, the weak interactionof the diamonds with the radiation field may give theman important role in the dust nucleation process. The gaspressure will stay high and the gas will be much closerto hydrostatic equilibrium during possible diamond nu-cleation than is normally the case in dust forming stellarregions, and therefore allow ample time for the nucleationprocess.
Send offprint requests to
: Anja C.Andersen, email address:anja@astro.ku.dk
Key words:
Stars: atmospheres - Stars: carbon - Stars:abundances - Stars: infrared
1. Introduction
Until 1987, dust particles around stars had only beenrecognised by their appearance in stellar spectra, but thepossibility of studying unprocessed stellar condensates di-rectly in the laboratory has given important informationnot only about the Solar System formation, but has alsoprovided precise data for testing astrophysicalstellar mod-els.Presolar diamonds were the first grains to be isolatedfrom meteorites of the carbonaceous chondrite type, whichcould be shown to have originated from outside the So-lar System (Lewis et al. 1987). The identification of theirpresolar origin has been possible on the basis of isotopicanomalies that appear inconsistent with any known solarsystem process (Anders & Zinner 1993). Primitive me-teorites show the presence of two different components.One component consist of chondrules and other inclusionswhich have experienced various melting processes duringthe formation of the solar system. The other component,called the matrix, is fine grained and have experiencedlittle or no heating. It is in the matrix that the presolargrains are found. The presolar diamond content is verysimilar for all chondrite classes, around 500–1000 ppmof the matrix (Alexander et al. 1990; Huss 1990). Theirmedian grain size is about 2nm (Fraundorf et al. 1989),which means that each diamond contain only about onethousand carbon atoms. A large fraction of the atomsare therefore on the surface of the crystal, and the mete-oritic diamonds therefore consist of a mixture of diamondand hydrogenate amorphous carbon (a-C:H). The amor-phous part has been estimated to account for 0.46 the
2 Spectral features of nano-diamonds
volume fraction of the presolar diamonds (Bernatowicz etal. 1990).The size distribution of the presolar diamonds is log-normal rather than power-law, reflecting growth ratherthan fragmentation and suggesting a short interstellar res-idence time (Lewis et al. 1989). This size distribution issurprising, as interstellar dust normally shows a power-lawdistribution, which is the steady state form for fragmenta-tion. A log-normal distribution reflects either size-sortingor growth followed by partial conversion of small grainsto large ones (Lewis et al. 1989). The good fit for the sizedistribution obtained by Lewis et al. (1989) down to smallsizes suggests minimal contributions from processes thataffect small grains preferentially, such as fragmentation,sputtering and erosion. This suggests that the distribu-tion is young and unevolved.Various mechanisms have been proposed to account forthe production of diamond grains in space, but the mostlikely scenario appears to be that the nano-diamonds havecondensed directly from stellar outflows (Lewis et al. 1987;Jørgensen 1988; Clayton 1989; Clayton et al. 1995). Theconditions in cool stellar outflows are remarkably similarto those employed in industry to produce diamonds byChemical Vapour Deposition (CVD) (Angus & Hayman1988). The CVD mechanism makes use of the fact thethe free energy difference between diamond and graphiteis only around 1 kcal/mol. Almost any chemical reactionyielding graphite as the thermodynamically stable prod-uct can, in principle, yield diamond as a metastable prod-uct. The trick is to steer the kinetics so as to favour dia-mond over graphite. It has been suggested by Kr¨uger et al.(1996), that in circumstellar envelopes the surface growthprocesses on carbonaceous seed particles will take place atsp
bonded carbon atoms rather than at sp
bonded car-bon atoms, which suggest that the grain material formedin circumstellar envelopes will be amorphous diamond-likecarbon.For studies of radiative processes in stellar environ-ments, knowledge of opacities of the relevant atoms,molecules and grains are essential. In order for the grainsto be taken into account in stellar atmosphere compu-tations, knowledge of the spectral properties of the rele-vant grains are needed. Transmission spectroscopic mea-surements of presolar diamonds from the Allende mete-orite in the ultra-violet, the optical and the infrared re-gion are presented in this paper. The measurements weredesigned such that it has been possible to determine themonochromatic absorption coefficient. This coefficient isnecessary in order to include the nano-diamonds in modelatmosphere calculations and in synthetic spectrum calcu-lations. By use of the derived absorption coefficient, syn-thetic spectra of carbon stars with the nano-diamonds in-cluded have been calculated, under the assumption thatthe diamonds we have extracted have the same opticalproperties as they had when they formed in a stellar at-mosphere. Finally, we have performed similar laboratorymeasurements on CVD diamonds, in order to get a moresolid basis for understanding the spectral features of thepresolar diamonds.
2. Experiments
The presolar diamonds were extracted using the methoddescribed by Tang & Anders (1988). A 10.8g piece of theAllende meteorite was dissolved by alternating treatmentwith 10N HF–1N HCl and 6N HCl (10 ml/g meteorite)to remove the silicates. The sulfur was removed with aCS
treatment and the reactive kerogen was destroyed byoxidation with HNO
and HClO
. To separate the dia-monds the sample was dispersed by ultrasonification in0.1M NH
OH, producing a diamond colloid, which wasextracted after centrifugation.The CVD diamonds were prepared as a hetero-epitaxial diamond film on a silicon (100) substrate whichhad been polished with 0.25
g of diamond powder be-fore depositing the CVD diamonds. The CVD diamondswere deposited in a hot filament reactor with 8% CH
inthe H
source gas. The filament temperature was between2200
C and 2400
C, the substrate temperatures were be-tween 700
C and 900
C and the pressure was 5 mbar.This gives a growth rate of about 1
g/hour. The CVDdiamonds were scraped off from the silicon substrate witha diamond needle.
Fig. 1.
A transmission electron microscope bright-field micro-graph showing a cluster of presolar nm-sized diamond crystal-lite. Each cluster consists of about 1000 diamonds. The cor-responding diffraction pattern is shown indicating the (111),(220), (311) and (400) spacings for diamond crystallite (d =2.065 (2.06), 1.281 (1.26), 1.035 (1.0754) and 0.8892 (0.8916)˚A, respectively, with the table values in parenthesis).
Transmission electron microscopy (TEM) was carriedout on both the presolar diamonds and the CVD dia-monds, using a Philips EM 430 transmission electron mi-croscope operated at 300 keV (Fig.1). With this instru-ment we performed conventional imaging, electron diffrac-tion and energy-dispersive X-ray spectroscopy (EDS) witha sensitivity down to Boron. We estimated that the sizesof the CVD diamonds are between 1.4 nm and 14 nm,from visual inspection of the TEM images. The CVD di-
Spectral features of nano-diamonds 3
amonds are hence, approximately three times bigger thanthe meteoritic diamonds.The spectral measurements were carried out in the in-frared (400–4000 cm
; 2.5–25
m) and in the UV/VIS(12200–52600 cm
; 190–820 nm) region.The UV/VIS spectra of the presolar and CVD dia-monds were taken on a very dilute solution of 350
g dia-monds in distilled water. The spectra were obtained witha HP 8452A Diode-Array Spectrophotometer, which is asingle-beam microprocessor-controlled spectrophotometerwith a deuterium lamp as the light source giving 190 nm –820 nm wavelength range. The wavelength accuracy was
2 nm. The sample cell was a small quartz containerwith dimensions 40 mm
10 mm
1 mm. During themeasurements, a reference spectrum of distilled water wasused. The difference of the signals obtained for the quartzcontainer filled with distilled water and the one filled withdiamonds in distilled water was attributed to the absorp-tion of the diamonds.The infrared spectra of the presolar and CVD dia-monds were obtained with a FT-IR Perkin Elmer 1760Infrared Spectrometer. The spectrometer operates in theregion 400–5000cm
. The instrument operation is drivenby a computer station which allowed us to record the spec-tra in digital form. All measurements were performed with64 scans and a resolution of 1–2cm
. For sample prepara-tion the KBr technique was used, where small quantities of the sample are mixed throughly with powdered KBr (300mg). Because of the softness of KBr and its bulk trans-parency between 40 and 0.2
m, the KBr and particlemixture can be pressed into a clear pellet (diameter = 13mm) (Colthup et al. 1990). Around 300
g of presolar di-amonds was added to the KBr as a suspension in ethanol.The diamonds were suspended in order to separate them,so that they would not be stuck in big clumps, because thediamonds are likely to have formed individually, not in ag-glomeration in stellar atmospheres. By suspending themwe therefore expect to obtain a spectrum which comparebest with the possible stellar spectrum. Around 200
g of CVD diamonds was added to the KBr in the same wayand the KBr for the reference pellets were also suspendedin ethanol. The ethanol was removed by pumping on thesample before pressing the tablet. Despite this, we stillhad traces of ethanol in our spectra, so it was necessaryto compensate for this by the use of the reference spectra.
3. Interpretation of the experimental spectra
3.1. The UV/VIS spectra of the diamonds
The UV/VIS spectra of our presolar and CVD diamondsamples are very similar to one another, showing strongabsorption in the UV, with a distinct band at 217 nm(46000 cm
), a flat maximum around 270 nm (37000cm
) and declining absorption towards the visual endof the spectrum (Fig.2). These absorption characteristicsare also typical for terrestrial diamond containing pairs of nitrogen atoms (Davies 1984). These bulk UV/VIS fea-tures deviate significantly from the results by Lewis et al.(1989), but correspond well with the measurements ob-tained by Mutschke et al. (1995) on presolar diamondsfrom the Murchison meteorite, except that the strengthof the flat maximum around 270 nm seem to be muchstronger for the Murchison presolar diamonds.The position of the band around 217 nm coincides withthat of the interstellar extinction bump at 217.5 nm, asit has also been found by Mutschke et al. (1995) for theMurchison meteorite.
Fig. 2.
The UV/VIS absorbance spectrum of the presolar andthe CVD diamonds, respectively.

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