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Collisions of small ice particles under microgravity conditions (II): Does the chemical composition of the ice change the collisional properties? PDF

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Astronomy & Astrophysics manuscript no. does_the_chemical_composition_change_the_collisional_properties_arxiv_version ©ESO2015 January6,2015 Collisions of small ice particles under microgravity conditions (II): Does the chemical composition of the ice change the collisional properties? C.R.Hill1,D.Heißelmann2,3,J.Blum2,H.J.Fraser1 1 TheOpenUniversity,DepartmentofPhysicalSciences,WaltonHall,MiltonKeynes,MK76AA,UK e-mail:[email protected] 2 TechnischeUniversitätBraunschweig,InstitutfürGeophysikundextraterrestrischePhysik,Mendelssohnstraße3,38106Braun- schweig,Germany 3 International Max-Planck Research School, Max-Planck Institute of Solar System Research, Justus-von-Liebig-Weg 3, 37077 Göttingen,Germany 5 1 Received14November2014,Accepted23December2014 0 2 n ABSTRACT a J Context.Understandingthecollisionalpropertiesoficeisimportantforunderstandingboththeearlystagesofplanetformationand theevolutionofplanetaryringsystems.Simplechemicalssuchasmethanolandformicacidareknowntobepresentincoldprotostellar 5 regionsalongsidethedominantwaterice;theyarealsolikelytobeincorporatedintoplanetswhichforminprotoplanetarydisks,and planetaryringsystems.However,theeffectofthechemicalcompositionoftheiceonitscollisionalpropertieshasnotyetbeenstudied. ] P Aims.Collisionsof1.5cmicespherescomposedofpurecrystallinewaterice,waterwith5%methanol,andwaterwith5%formic acidwereinvestigatedtodeterminetheeffectoftheicecompositiononthecollisionaloutcomes. E Methods.Thecollisionswereconductedinadedicatedexperimentalinstrument,operatedundermicrogravityconditions,atrelative h. particleimpactvelocitiesbetween0.01and0.19m s−1,temperaturesbetween131and160Kandapressureofaround10−5mbar. p Results.Arangeofcoefficientsofrestitutionwerefound,withnocorrelationbetweenthisandthechemicalcomposition,relative - impactvelocity,ortemperature. o Conclusions.Weconcludethatthechemicalcompositionoftheice(atthelevelof95%watericeand5%methanolorformicacid) r doesnotaffectthecollisionalpropertiesatthesetemperaturesandpressuresduetotheinabilityofsurfacewettingtotakeplace.Ata t s levelof5%methanolorformicacid,thestructureislikelytobedominatedbycrystallinewaterice,leadingtonochangeincollisional a properties.Thesurfaceroughnessoftheparticlesisthedominantfactorinexplainingtherangeofcoefficientsofrestitution. [ Keywords. accretion,accretiondisks–astrochemistry–planetsandsatellites:formation–planetsandsatellites:rings–protoplan- 1 etarydisks v 0 3 81. Introduction (theso-calledbouncingbarrier)(Güttleretal.2010;Zsometal. 0 2010;Kotheetal.2013).Inrecentyears,thepresenceoficehas 0Water ice is abundant in the interstellar medium and has also been postulated as one possible solution to the bouncing bar- .been observed towards dense clouds, cloud cores, protostellar rier; it has been shown that ice particles have a larger adhesive 1 regionsandprotoplanetarydisks(Obergetal.2011a).Recentre- androllingfrictionforce(Gundlachetal.2011),ahigherstick- 0 5searchstudyingdeuterium-to-hydrogenenrichmentsinthesolar ing threshold (Gundlach & Blum 2014) and reduced elasticity 1system has shown that water ice was present in the solar neb- (Hertzsch 2002) compared to silicate dust particles which will :ula protoplanetary disk (Cleeves et al. 2014). Water ice is also increase the threshold velocity for sticking. In addition, recent v present in planetary ring systems such as the rings of Saturn model simulations have shown that ice condensation could en- i X(Cuzzi&Pollack1978;Cuzzietal.1980),whereitscollisional abledustgrainstogrowtodecimetresizesaroundthesnowline propertiesplayanimportantroleinthestructureanddynamical (Ros&Johansen2013)andeventoicyplanetesimalsiftheini- r aevolutionoftherings.Itisnotclearwhethertheseringsareold tialicegrainsweresubmicrometre-sized(Kataokaetal.2013). oryoung;intheformercase,theringswillberesiduesfromthe In the context of this paper, ring systems are also of inter- formation era. The presence of water ice across star and planet est. Until recently, rings had exclusively been known to exist formingregionsmaythereforeinfluencetheprocessesofplanet aroundthefouroutermostsolarsystemplanets,thoughwiththe formation. detection of two small dense rings around the Centaur (10199) It has been proposed that planets form from the dust in a Chariklo(Braga-Ribasetal.2014;Duffardetal.2014),itseems protoplanetary disk by a process of dust aggregation (Weiden- thatringsystemsarenotexclusivelypresentaroundgiantplan- schilling1977,1980).Whilethistheoryhasgainedwidespread ets.TheringsaroundSaturnarethemostwellstudiedandcon- acceptance,thereremainsaprobleminthatgrowthbetweencen- sist predominantly of small icy bodies (Cuzzi et al. 2010), be- timetreandkilometresizeshasnotbeendemonstrated,asthere tween1cmand10mdiameter,dominatedbywaterice(Zebker isacriticalvelocity,reducingwithparticlesize(Weidenschilling etal.1985).Theringdynamicsarecomplex,influencedbyper- 1977), beyond which particles tend to bounce rather than stick turbations by resonances between the ring particles and nearby Articlenumber,page1of8 A&Aproofs:manuscriptno.does_the_chemical_composition_change_the_collisional_properties_arxiv_version moons, which are counteracted by frequent inelastic collisions tutionwasthoughttobeduetothedifferenceinvelocityranges at low relative velocities. Typical collision velocities in the un- betweenthetwostudies. perturbed rings are well below 1 cm s−1 (Esposito 2002; Col- The range of coefficients of restitution and lack of depen- well et al. 2009), but gravitational perturbations may raise the denceonimpactvelocityandnormalisedimpactparameterisin averagecollisionspeedconsiderably.Thecollisionsdissipateki- contrast to previous studies of ice collisions which show a de- neticenergyfromtheringsandtherebydeterminethestabilityof creaseincoefficientofrestitutionwithincreasingimpactveloc- the rings (Salo et al. 2001; Schmidt et al. 2001); consequently, ity(Bridgesetal.(1984),Hatzesetal.(1988))andverylittleloss data pertaining to collisional properties and outcomes are vital ofkineticenergyforglancingcollisions(i.e.b/R∼1)(Supulver tomodeleffortswhichareusedtounderstandringinstabilities, et al. 1995). The reason for this was thought to be the differ- wakesandoverallstructure,includingtheverystronglyconfined enceinsurfaceroughness;whiletheicesurfacesintheworkof heights observed in Saturnian and other ring systems (Colwell Bridges et al. (1984), Hatzes et al. (1988) and Supulver et al. etal.2006,2007;Hedmanetal.2007;Thomsonetal.2007). (1995) were smooth, the ice surfaces in the studies of Heißel- While water is abundant in planet forming regions, many mannetal.(2010)andPaperIwereroughandanisotropic.This othermoleculeshavealsobeendetectedinprotostellarregions. explains the ranges of coefficient of restitution and the lack of Consequently, the icy mantles on dust grains in protoplanetary dependenceonimpactvelocityandnormalisedimpactparame- disks are likely to be composed of water dominated ices which ter and is in accordance with the work of Hatzes et al. (1988) mayalsocontainaplethoraof"contaminants",includingmany where both frost and roughened surfaces were found to reduce simple molecules such as CO, CO , CH OH, CH , NH and thecoefficientofrestitution.Forafullcomparisonoftheexper- 2 3 4 3 HCOOH (e.g. Pontoppidan et al. (2004), Aikawa et al. (2012), imentalconditionsinthesestudies,wereferthereadertoPaper Obergetal.(2011b),Nobleetal.(2013)).Recentworkhassug- I. gestedthatthemostabundantvolatilespeciesinplanetsofsolar Aninherentlimitationinthestudiesoficecollisionstodate composition are H O, CO, CO , CH OH and NH (Marboeuf (as related to planet formation and planetary ring systems) is 2 2 3 3 etal.2014).Itisalsopossiblethatsomeofthesespeciesmaybe theirfocusonpurewaterice.Itispossiblethatthepresenceof presentinplanetaryringssuchasthoseofSaturn.WhileSaturn’s otherchemicalsmightchangethecollisionalproperties;Bridges rings are composed of mainly water ice, there is evidence that etal.(1996)studiedthestickingforcesbetweenfrostcoatedwa- other species are present (Poulet et al. 2003; Cuzzi et al. 2009) ter ice at atmospheric pressure and temperatures between 110- anditisnotunreasonabletosupposethatsomeofthosemayin- 150Kanddiscoveredthatmethanolfrostshadstrongersticking clude the above molecules. This provides the main motivations forcesthanwaterfrosts.Themeltingpointofmethanolis176K forthispaper:firstlytostudytheeffectsofminorchemicalpol- atatmosphericpressuresoitispossiblethattheincreasedstick- lutantsoncollisionsbetweenicyparticlesatlowvelocities,and ing forces are due to surface melting. This is the same mecha- secondly to understand how the outcomes of these collisional nismthatleadstoiceaggregationinatmosphericclouds(Hobbs processes affect processes of planet formation and ring system 1965),leadingtoincreasedaggregationaroundthemeltingpoint evolution. of water (Hobbs et al. 1974). In protoplanetary disks and plan- The work on this paper builds on our previous publication etary rings, the temperatures and pressures are too low for this (Hill et al. (2015), henceforth Paper I) in which the collisions processtodominate.Bothmethanolandformicacidhavebeen of millimetre-sized ice particles (both spheres and irregularly detectedinprotostellarregionsinthesolidphase(Pontoppidan shaped fragments, diameters 4.7-10.8 mm) were studied under etal.(2004),Obergetal.(2011b),Aikawaetal.(2012),Schutte microgravityconditionsonaparabolicflight.Themainparam- et al. (1999), Zasowski et al. (2009)) at the 1-30% abundance eters studied were the coefficient of restitution, ε, and the im- levelrelativetowatericeformethanoland1-5%levelforformic pactparameter,b.Thecoefficientofrestitutionistheratioofthe acid (Boogert et al. 2008). We have therefore chosen to focus relativevelocitiesoftheparticlesafterandbeforethecollision, thisstudyonicyparticlesformedbyfreezingeitherpurewater whichisrelatedtothetranslationalkineticenergylostinthecol- or5%methanolorformicacidinwater,toinvestigatetheeffects lision: ofthechemicalcompositionoficeonitscollisionalproperties. Whiletheeventualaimistoinvestigatetheeffectsofthechem- v ε= a (1) icalcompositiononplanetformation,theformoficeusedhere v b (solidicespheres)ismorerelevanttoplanetaryringsystemsthan whereaandbdenoteafterandbeforethecollisionrespectively. protoplanetarydisks,wheretheiceislikelytobeintheformof The impact parameter is the distance of closest approach of porousagglomerates(e.g.Kataokaetal.(2013)).Thereforethe the two particles perpendicular to their relative velocity vector. results will be more immediately applicable to planetary rings, Henceforthweusethenormalisedimpactparameterb/R,which butitishopedthattheywillbeastartingpointfordiscussionof istheimpactparameter,b,normalisedtoR,thedistancebetween iceinprotoplanetarydisksaswell. thecentreofmassesofthetwoparticlesatthepointofcollision, i.e.thesumofthetworadiiforsphericalparticles. 2. Experimentaldetails The relative collision velocities ranged from 0.26 to 0.51 m s−1. The coefficients of restitution were spread evenly The experimental setup has previously been discussed in detail between 0.08 and 0.65 with no dependence of this property (Salter et al. (2009) and Paper I) and is summarised again here on either impact velocity or normalised impact parameter. The forcompleteness(seeFig.1).Theexperimentwasdesignedand spreadofcoefficientsofrestitutionwasattributedtothesurface built to carry out low velocity particle collisions on parabolic roughness of the particles. This corroborates previous work by flights. Prior to take off, the particles are loaded into a pre- Heißelmannetal.(2010),wherecollisionsof1.5cm(diameter) cooled(toaround77K)rotatingdoublehelixparticlereservoir, ice spheres were studied under microgravity conditions. In this orcolosseum(1).Thisisrotated(2)duringtheflighttolineup case,theimpactvelocitieswerebetween0.06and0.22m s−1and two diametrically opposed ice particles with motorised pistons thecoefficientofrestitutionwasspreadevenlybetween0.06and (3) which accelerate the particles to a pre-defined constant ve- 0.84.Thedifferencebetweentherangesofcoefficientsofresti- locitydirectedtowardsthecentreofthecollisionvolume,where Articlenumber,page2of8 C.R.Hill,D.Heißelmann,J.Blum,H.J.Fraser:Collisionsofsmalliceparticlesundermicrogravityconditions(II): surfaces.Thetargetwascomposedofpurecrystallinewaterice andwasplacedinthecentreofthechamberimmediatelypriorto evacuation.Thetargetwasplacedinadifferentorientationwith respecttothechamberforeachflight,givingaccesstodifferent normalisedimpactparameters. Thenormalisedimpact parame- ter is related to the angle of the target to the direction of travel (θ)bythefollowingequation: b/R=cos(θ) (2) On the first flight of this campaign, the target was at 90◦ to the direction of travel of the particles, giving b/R = 0 - completely headoncollisions.Thesecondflighthadthetargetat60◦tothe directionoftravel,givingb/R=0.5.Thethirdflighthadthetar- √ getmountedat30◦tothedirectionoftravel,givingb/R= 3/2. Fig. 1. Computer aided design schematic of the experimental setup Technicalproblemspreventedcollectionofdatainthisconfigu- (adapted from Salter et al. (2009). The particles are stored in an alu- rationandsoparticle-particlecollisionswereperformedinstead. minium colosseum (1) which is rotated (2) to line up two colosseum Itwasthereforenecessarytoopenthechamberduringtheflight holeswithtwodiametricallyopposedmotorisedpistons(3)whichcol- to remove the target. The particles remained within the sam- lidestheparticleseitherwitha52mmdiametericetarget(4)placedat plereservoirandhencetheirexposuretotheatmosphereofthe the centre of the collision volume or with each other when the target planewasminimal.Itisunlikelythatsignificantfrostformation isremoved.Thesystemispassivelycooledbypassingliquidnitrogen could occur on the particle surfaces under these conditions and throughacoolingring(5)priortotakeoff.Theparticlesarekeptwithin comparisonwithpreviousparticle-particlecollisionsconducted the colosseum and protected from radiative heating by an aluminium under similar conditions (but without the opening of the cham- shield (6), and a 45 kg copper block (7) acts as a thermal reservoir, keepingthesystemcoolduringtheflight.Theentiresetupisenclosed ber)showsthatthisassumptioniscorrect(seeSection4.1fora withinavacuumchamber(8). comparison of our data with that of Heißelmann et al. (2010)). Fig.2showsanexamplecollisionofanicespherecontaining5% formicacidwiththeicetargetat90◦tothedirectionoftravel. theycollideinperfectfreefallconditionseitherwithatarget(4) Table1showsabreakdownofallthecollisionssuccessfully or with each other. The system is cryogenically cooled to tem- performedduringthiscampaign.Thenumbersofcollisionssuit- peraturesaround77Kbypassingliquidnitrogenthroughacool- ableforanalysisandunsuitableforanalysisaregiven.Residual ing ring (5) prior to take off and is kept cool during flight with acceleration of the plane (when the quality of microgravity is the use of a U-shaped aluminium heat shield (6) and a 45 kg poorandthecameramoveshorizontallywithrespecttothepar- copperblock(7)onwhichtheparticlereservoirsits.Thecopper ticlesasaresult)wasaparticularproblemontheseconddayof actsasbothathermalreservoirandacryo-pumpforanyresidual thecampaign(targetat60◦)andhenceonly8collisionssuitable gas. The entire set up is encased inside a vacuum chamber (8), foranalysiswereobtained.Poorqualityhamperedimageanaly- with a typical residual gas pressure of 10−5 mbar. The pistons siseffortsinafewcasesandtherewasonecaseoffragmentation. enter the collision volume through two differentially pumped Thisisthoughttoberelatedtothewayinwhichtheicespheres feedthroughs.Acollisionisinitiatedbyacceleratingthepistons areformedratherthanarealcollisionaloutcome.Table2shows (which are controlled by Labview software) to a maximum ve- abreakdownofthecollisionssuitableforanalysis,theresultsof locityofbetween0.01and0.1m s−1.Thepistonsmakecontact whicharepresentedinSection4.1. withtheparticles,arebroughttoasharpstopafewmillimetres later, and then are immediately retracted to their starting posi- Table 1. A break down of the collisional outcomes observed in this tions. The piston tips remain within the cooled region at rest, study.Theanglesrefertotheanglebetweenthetargetandthedirection meaning that they are at the same temperature as the particles oftraveloftheparticles.Thecollisionsthatweresuitableforanalysis are detailed in Section 4.1. The other collisions were excluded from anddonotinduceparticleheatingorsurfacemeltingduringcol- theanalysisduetoresidualacceleration(poorqualityofmicrogravity), lision.Ahighspeedcamerawithaframerateof107framesper poorimagequalityandfragmentation. secondwascombinedwithprismopticstocapturetwoviewsof thecollision48.8◦apart. Collisionaloutcome Numberofcollisions Theparticlesusedinthisexperimentwereicespheresof1.5 Targetat90◦ Suitableforanalysis 35 cmdiameter.Somewerecomposedofpure,distilledwater,and Residualacceleration 1 others were composed of a 5% solution of methanol or formic Poorquality 4 acidindistilledwater.Theparticleswereproducedusingspher- Fragmentation 1 ical moulds and a standard kitchen freezer. Making ice parti- Targetat60◦ Suitableforanalysis 8 clesinthiswayproducescrystallinehexagonalicewitharough, Residualacceleration 41 anisotropicsurface(Heißelmannetal.2010).Theparticleswere Poorquality 5 removed from the freezer and placed directly into a container Fragmentation 0 of liquid nitrogen situated within the chamber. Once the parti- Notarget Suitableforanalysis 15 cles had reached 77 K, they were individually loaded into the Residualacceleration 3 pre-cooledsamplereservoir.Surfacefrostingwasminimisedby Poorquality 7 pre-coolingtheparticlereservoirto∼77Kpriortoloadingand Fragmentation 0 evacuatingthechambertoabasepressureofaround10−5 mbar Total 120 immediately after loading while the ice particles were still out- gassingN ,therebypreventingfrostfromformingontheparticle 2 Articlenumber,page3of8 A&Aproofs:manuscriptno.does_the_chemical_composition_change_the_collisional_properties_arxiv_version 11..44 Pure water Target 0° 5% methanol Target 60° 11..22 5% formic acid No target ε Pure water (previous data) Previous data (no target) n, o 11..00 uti stit 00..88 e of r nt 00..66 e ci effi 00..44 o C 00..22 00..00 00..0000 00..0055 00..1100 00..1155 00..2200 00..2255 Relative impact velocity (m s−1) Fig. 3. Coefficient of restitution as a function of impact velocity for collisions of 1.5 cm (diameter) ice spheres with a target at 90◦ to the Fig.2.Imagesequenceofanicespherecontaining5%formicacidcol- direction of travel (b/R = 0, shown by crosses), a target at 60◦ to the lidingwithapureicetarget(indicated)at90◦tothedirectionoftravelat directionoftravel(b/R=0.5,shownbysquares)andnotarget(boththis avelocityof0.08m s−1.Theimageswerecapturedusingbeamsplitter data (shown by circles) and data previously reported by Heißelmann opticswiththeviewontheleftseparatedfromtheviewshownonthe etal.(2010)(shownbystars)).Thechemicalcompositionofthespheres rightby48.8◦.Theimagesaretaken4/107sapart. areindicatedwithcolours(blackforwater,redformethanol,bluefor formicacidandgreyforthepreviousdata).Therectangles(blackfor Table2.Abreakdownofanalysedcollisionsintermsofchemicalcom- purewater,redfor5%methanolinwaterandbluefor5%formicacid position.Theanglesrefertotheanglebetweenthetargetandthedirec- inwater)showthedataencompassedbyonestandarddeviationofthe tionoftraveloftheparticles.Theicesphereswerecomposedofpure mean. hexagonalcrystallinewaterice,5%methanolinwaterand5%formic acidinwater. resultsofHeißelmannetal.(2010)whichwereforcollisionsof Collisiontype Purewater 5% 5% Total purewatericespheresofidenticalsize.Apartfromtwooutliers methanol formicacid around 0.01 m s−1, the data in the current study lies virtually Targetat90◦ 7 10 18 35 within the range of the previous data. The two distinct veloc- Targetat60◦ 8 0 0 8 ity groupings in our data are because of the different relative Notarget 2 8 5 15 velocities obtained by colliding a particle with a stationary tar- Total 58 get(thelowervelocityregion)andcollidingaparticlewithan- othermovingparticle(thehighervelocityregion).Thevelocity range is similar for both studies (0.05-0.19 m s−1 for the cur- 3. Analysismethodology rent study (disregarding the two outliers around 0.01 m s−1)) Thedataanalysiswasperformedasfollows.Theparticleswere and 0.06-0.22 m s−1 for the previous study). The values of ε manually tracked frame by frame in both views of the colli- arespreadbetween0.08and0.81forourdataandbetween0.02 sion; the co-ordinates from the two views were combined us- and 0.84 for the previous data; the range is virtually identical ing a transformation algorithm to give orthogonal (x, y, z) co- forthecurrentandpreviousresults.Thereisnoapparentdiffer- ordinates. Linear fits in each dimension yielded particle trajec- encebetweenthecollisionalpropertiesofthedifferentchemical tories from which velocities before and after the collision and compositions. The similarity of the target data with the previ- hence coefficients of restitution were calculated. The velocities ousparticle-particlecollisiondatashowsthatcollidingasphere wereresolvedintocomponentsnormalandtangentialtothecol- withalargerbodyhasthesameeffectascollidingitwithanother lidingsurfacestogivenormalandtangentialcoefficientsofresti- sphere, aresult whichis notsurprising consideringthe similar- tution.Fortheparticle-particlecollisions,normalisedimpactpa- ities in contact area during collision in both cases. Finally, the rameters (b/R) were also calculated from particle trajectories. similarity of these particle-particle collisions with the previous Where errors are shown, they were calculated using standard work reiterates the fact that the brief opening of the chamber methodsforthepropagationoferrors. duringtheflighttoremovethetargetdidnotaffecttheresults;if significant frosting of the particle surfaces had occurred during this time, the coefficients of restitution would be lower (Hatzes 4. Resultsanddiscussion etal.1988). Where there was sufficient data, rectangles have been plot- 4.1. Coefficientofrestitution tedtoshowhowmanypointslaywithinonestandarddeviation Bouncing was the only collisional outcome observed in this ofthemean(ignoringanyoutliers).Theserectangleshavebeen study, corroborating previous results in Paper I and also those plottedindependentlyforeachexperimentalsetup.Forthetarget of Heißelmann et al. (2010). If ice particles have a critical ve- at90◦andforparticle-particlecollisions,thereisagoodoverlap locityfortheonsetofbouncing,itwillbebelow0.01m s−1(the betweentherectangles,demonstratingthatthereisnostatistical lowestvelocitycollisioninthecurrentstudy)forparticlesofthis differencebetweenthedatasets.Wethereforeconcludethatthe size.Fig.3showsthecoefficientsofrestitution(ε)asafunction presenceofmethanolandformicacidintheiceatalevelof5% ofrelativeimpactvelocityforthisstudycomparedtheprevious does not change the coefficient of restitution. For the target at Articlenumber,page4of8 C.R.Hill,D.Heißelmann,J.Blum,H.J.Fraser:Collisionsofsmalliceparticlesundermicrogravityconditions(II): 60◦, technical difficulties prevented the capture of useful colli- targetat90◦(b/R=0)andthedataforparticle-particlecollisions sions for any other material than pure water, meaning that the (b/R=0.00-0.33)bothhaveasmallcomponentoftangentialim- effectofchemicalcompositioncannotbetestedforthisflight. pactvelocitycomparedtothenormalcomponent(Fig.4a,b,e, At this point it is instructive to consider why the inclusion f),whichistobeexpectedforheadon(ornearlyheadon)col- ofmethanol andformicaciddoes notnoticeablyaffectthe col- lisions.Thetangentialcoefficientsofrestitutionarespreadfrom lisional properties of the ice spheres. As mentioned in the in- around0.1to1.3andfromaround0.2to1.1forparticle-particle troduction, methanol frosts are much stickier than water frosts collisions. The spread for the normal coefficients of restitution between 110 and 150 K at atmospheric pressure (Bridges et al. is much less, from around 0 to 0.6 for the target at 90◦, and 1996); this is most likely because of surface wetting near the fromaround0to0.7forparticle-particlecollisions.Thisshows melting point. However, surface wetting is not possible at the thatheadoncollisionscanresultinbothscatteringandrebound, lowpressureswithinourchamberforeithermethanolorformic withmoreenergygoingintoscatteringthanreboundonaverage. acid.Itisalsousefultoconsiderwherethemethanolislocated For the target at 60◦ (b/R=0.5), there is a much larger tangen- within our ice spheres. Considering the methanol-water phase tialcomponenttotheimpactvelocitythanforthetargetat90◦, diagram (Takaizumi & Wakabayashi (1997), Deschamps et al. although the normal component to the impact velocity is still (2010)),at255K(thetemperatureofastandardkitchenfreezer), larger(Fig.4candd).Thespreadsoftangentialandnormalco- thewaterwillhavefrozenbutthemethanolwillremainasaliq- efficientsofrestitutionareverysimilarinthiscase,botharound uid.Asthefreezingprocesswillfreezefromtheoutsidein,itis 0.3-0.7. This demonstrates that for b/R=0.5, the distribution of possiblethatallofthemethanolisatthecentreoftheicesphere energyintoreboundandscatteringisroughlyequal.Inallcases, due to exclusion from the water ice as it freezes, meaning that thechemicalcompositionoftheicedoesnotaffectthedistribu- thesurfaceisessentiallypurewatericewhichwouldexplainthe tionoftranslationalkineticenergy. similarity in collisional properties. Formic acid freezes at 282 Considering the highest value of ε obtained in this study, a K, which is higher than the freezing point of water, although it minimum of 29% of the particles’ translational kinetic energy is likely that the presence of the water will depress the freez- (1−ε2 with ε = 0.84) is lost in the collision. From the image ingpointofformicacid.Ataconcentrationof5%,wespeculate sequences of the collisions, it is clear that some of the energy thattheformicacidwillbedistributedthroughouttheicesphere isconvertedintorotationalenergy.Abreakdownoftheparticle due to the similarity in freezing points. Regardless of where in rotation is shown in Table 3. The overall values are given but thespheresthemethanolandformicacidispresent,atalevelof dividing the spheres by chemical composition does not signif- 5%,theoverallstructureislikelytobedominatedbycrystalline icantly alter the proportions. Due to the spherical shape of the waterice.Itislikelyforthisreasonthatthecollisionalproperties particles(andhencethelackofdistinguishingmarks),itwasnot shownodependenceonthecompositionoftheice. possibletoextractmorequantitativerotationalinformation. To determine the strength of any correlation between the variables, the linear Pearson correlation coefficient was com- Table3.Thepercentageofparticlesthatrotateanddonotrotatebefore puted: andafterthecollision. (cid:80)n (y −y¯)(x −x¯) Rotates(%) Doesnotrotate(%) Unclear(%) r= (cid:112)(cid:80)n (iy=0−iy¯)2(cid:112)(cid:80)ni (x −x¯)2 (3) Before 4 89 7 i=0 i i=0 i After 71 10 19 The number of points is given by n and the mean values of x andyaregivenby x¯andy¯ respectively.Thisgivesameasureof The majority of the particles were fired from the pistons thestrengthofcorrelationbetweentwovariables,xandy,witha withoutanyobservablerotation(89%).Themajorityofthepar- valueof1/-1indicatingperfectpositive/negativecorrelationand ticles did rotate after the collision (71%) but 10% did not. It is avalueof0indicatingnocorrelation.Thevaluereturnedisonly clearfromthisandpreviousresultsinPaperIthatrotationcan- significantwherethereisasignificantnumberofdatapointsand notaccountforalloftheparticles’energyloss.Acomputational soonlycasesthatmeetthisconditionwillbediscussed.Forthe study by Zamankhan (2010) showed that most translational ki- targetat90◦,thedataforpurewater,methanolandformicacid netic energy in icy grain collisions is dissipated due to surface shows no correlation between coefficient of restitution and im- fracturing. We cannot confirm or refute this here because such pact velocity (values of 0.21, 0.06 and 0.05 respectively). The surface fracturing would not be visible in our images. It is also sameistrueforpurewaterwiththetargetat60◦(correlationco- possiblethatenergyisconvertedintoheatleadingtodesorption efficientof0.13)andformethanolwithnotarget(correlationco- ofsurfacematerial,whichagainisnotdetectableinourexperi- efficientof0.47);therestofthedatasetscontainaninsufficient mentandisbeyondthescopeofthispaper. number of points for any correlation to be statistically signifi- cant.Thesevaluesindicatethatthecoefficientofrestitutiondoes 4.2. Effectoftemperature not depend significantly on impact velocity which corroborates ourpreviousworkinPaperIandtheworkofHeißelmannetal. Duetoparabolicflightrestrictions,itisnotpossibletocoolthe (2010).Here,asbefore,thesurfaceroughnessislikelytobethe chamberwithliquidnitrogenduringflight.Theflowofnitrogen most important factor in explaining the range of coefficients of mustbestoppedpriortotakeoff,relyingonthecopperintheex- restitution. perimenttoactasaheatsink.Thechambertemperatureslowly Fig.4showsthecoefficientsofrestitutiontangentialandnor- increasesduringtheflight,givingusanopportunitytostudythe maltothecollidingsurfacesasafunctionoftangentialandnor- effect of temperature on coefficient of restitution. The data for malimpactvelocityrespectively.Calculatingthesegivesfurther the third flight of this campaign have been excluded due to the information about the distribution of energy after the collision. possibilityofadditionalwarmingwhenthechamberwasopened Thenormalcoefficientofrestitutiongivesinformationaboutthe toremovethetarget.Thetemperaturerangedfrom131to160K, reboundoftheparticlesandthetangentialcoefficientofrestitu- increasingatarateof22.5Kh−1 forthefirst20minutesandat tiongivesinformationaboutparticlescattering.Thedataforthe arateof7.0Kh−1 fortheremainderoftheflight.Fig.5shows Articlenumber,page5of8 A&Aproofs:manuscriptno.does_the_chemical_composition_change_the_collisional_properties_arxiv_version 11..44 11..44 εII Pure water Pure water ential coefficient of restitution, 0001100011..........4680246802 55%% mfoermthica naoclid εmal coefficient of restitution, ⊥ 0001100011..........4680246802 55%% mfoermthica naoclid ang 00..22 Nor 00..22 T 00..00 00..00 00..0000 00..0022 00..0044 00..0066 00..0088 00..1100 00..1122 00..0000 00..0022 00..0044 00..0066 00..0088 00..1100 00..1122 Tangential relative impact velocity (m s−1) Normal relative impact velocity (m s−1) 11..44 11..44 εII Pure water Pure water ential coefficient of restitution, 0001100011..........4680246802 εmal coefficient of restitution ,⊥ 0001100011..........4680246802 ang 00..22 Nor 00..22 T 00..00 00..00 00..0000 00..0022 00..0044 00..0066 00..0088 00..1100 00..1122 00..0000 00..0022 00..0044 00..0066 00..0088 00..1100 00..1122 Tangential relative impact velocity (m s−1) Normal relative impact velocity (m s−1) 11..44 11..44 εII Pure water Pure water ential coefficient of restitution, 0001100011..........4680246802 55%% mfoermthica naoclid εmal coefficient of restitution, ⊥ 0001100011..........4680246802 55%% mfoermthica naoclid ang 00..22 Nor 00..22 T 00..00 00..00 00..0000 00..0055 00..1100 00..1155 00..2200 00..0000 00..0055 00..1100 00..1155 00..2200 Tangential relative impact velocity (m s−1) Normal relative impact velocity (m s−1) Fig. 4. Coefficients of restitution normal and tangential to the colliding surfaces as a function of the normal and tangential impact velocity respectively.Thechemicalcompositionsareindicatedbydifferentcoloursandsymbols:blackplussymbolsforpurewaterice,redcrossesfor 5%methanolinwater,andbluecirclesfor5%formicacidinwater.a.Tangentialcoefficientofrestitutionforthetargetat90◦tothedirectionof travel(b/R=0).b.Normalcoefficientofrestitutionforthetargetat90◦tothedirectionoftravel(b/R=0).c.Tangentialcoefficientofrestitution forthetargetat60◦tothedirectionoftravel(b/R=0.5).d.Normalcoefficientofrestitutionforthetargetat60◦tothedirectionoftravel(b/R= 0.5).e.Tangentialcoefficientofrestitutionforparticle-particlecollisions(b/R=0.00-0.33).f.Normalcoefficientofrestitutionforparticle-particle collisions(b/R=0.00-0.33). the coefficient of restitution as a function of temperature. The would be required (around 250 K and a few mbar, considering dataforthesecondflight(targetat60◦)isatlowertemperatures the phase diagram of water (Ehrenfreund et al. 2003)). In this thanthedataforthefirstflight(targetat90◦)becausetheavail- temperature and pressure regime, we would expect to see a re- ablecollisionsfromthisflightalltookplaceearlierintheflight duction in coefficient of restitution with increasing temperature thanthoseonthefirstflight.Thereisnocorrelationbetweenthe owingtogreaterstickingforcesathighertemperatures,asseen parameters(acorrelationcoefficientof-0.06)andhencewecon- bySupulveretal.(1997). cludethattemperaturehasnoeffectoncoefficientofrestitution overthistemperaturerange.Thiscorroboratesourpreviouswork in Paper I and again we conclude that this is due to the lack of 5. Astrophysicalimplications surfacemeltingatthesetemperaturesandpressures.Inorderfor It appears that inclusion of methanol and formic acid at a level surfacemeltingtotakeplace,highertemperaturesandpressures of 5% has no impact on the collisional properties. However, Articlenumber,page6of8 C.R.Hill,D.Heißelmann,J.Blum,H.J.Fraser:Collisionsofsmalliceparticlesundermicrogravityconditions(II): 1. Sticking does not occur as a collisional outcome. Universal 11..44 bouncing was observed, demonstrating that the critical ve- Pure water Target 0° locity for the onset of bouncing of ice particles of this size ε 11..22 55%% mfoermthica naoclid Target 60° (1.5cmdiameter)islessthan0.01m s−1. on, 11..00 2. Nodifferencewasobservedbetweenthecoefficientsofresti- uti tutionforpurecrystallinewaterice,waterwith5%methanol estit 00..88 and water with 5% formic acid. The presence of methanol of r and formic acid in the ice does not affect the collisional ent 00..66 behaviour in our experiments. We postulate that this is be- ci effi 00..44 causeallsampleshavesurfacestructuresthataredominated Co bycrystallinewaterice.Asinpreviousstudies(PaperIand 00..22 Heißelmannetal.(2010)),thesurfaceroughnessisthedom- 00..00 inantfeatureoftheparticles,nottheirchemicalcomposition. 113300 113355 114400 114455 115500 3. A broad range of coefficients of restitution was found with Temperature (K) no correlation between this and impact velocity, replicating Fig.5.Coefficientofrestitutionasafunctionoftemperature.Thereis theresultsofpreviousstudies(PaperIandHeißelmannetal. nocorrelationbetweenthetwoparameters.Thechemicalcompositions (2010)). As before, this is thought to be due to the rough, areindicatedbydifferentcolours:blackforpurewaterice,redfor5% anisotropicsurfacesoftheiceparticles. methanolinwater,andbluefor5%formicacidinwater.Thesymbols 4. Atleast29%oftheparticles’initialtranslationalkineticen- indicatetheorientationofthetarget;aplussymbolforthetargetat90◦to ergyislostinthecollision.Someofthisenergyisconverted thedirectionoftravel,andasquareforthetargetat60◦tothedirection into rotational energy but this cannot account for all of the oftravel. energyloss. 5. Temperaturedidnotaffectcoefficientofrestitutionoverthe rangemeasured(131to160K). methanolfreezeoutinplanetaryringsandprotoplanetarydisks willhappenatlowertemperaturesthanthoseatwhichourfreez- Acknowledgements. We thank the Deutsches Zentrum für Luft- und Raum- ingprocesstookplace,whichcouldleadtoatrulymixedice.In fahrt (DLR) for providing us with the parabolic flights and for financial aid thisscenario,methanolmayhaveagreatereffectoncollisional throughgrantnos.50WM0936and50WM1236.WethanktheEuropeanSpace properties, particularly if it is present in higher concentrations Agency(ESA)forprovidinguswiththeICAPShigh-speedcamerasystemdur- neartheicesurface.However,formicacidhasnotbeendetected ingtheparabolicflightcampaign.D.HeißelmannwassupportedbytheDeutsche Forschungsgemeinschaft(DFG)throughgrantno.BL298/11-1.Wewouldlike abovethe5%levelandislikelytobeevenlydistributedthrough- tothanktheEuropeanCommunity’sSeventhFrameworkProgrammeLASSIE outouricesample,leadingustoconcludethattheinclusionof FP7/2007-2013(LaboratoryAstrochemicalSurfaceScienceinEurope)forfund- formicacidwillnotaffectthecollisionalpropertiesoftheices. ingH.J.FraserandC.R.Hill’sparticipationinthedataanalysisandinterpre- Therefore, it seems unlikely that the inclusion of other species tationfromthiswork,undergrantagreementno.238258.C.R.HillthanksThe onthelevelof5%willaffectthecollisionaloutcomesoficypar- OpenUniversityforaPhDstudentship;H.J.FraserthanksSUPA(ScottishUni- versitiesPhysicsAlliance)andTheUniversityofStrathclydeforsupportingthe ticlesinringsystemsorprotoplanetarydisks. originalexperimentalwork.Last,butnotleast,wethankallparabonauts(Katha- Boththepureicespheresandtheicespherescontaining5% rinaBairlein,EikeBeitz,RenéWeidlingandMartinUhrin)whoparticipatedin methanol or formic acid yielded a broad range of coefficients theparabolic-flightcampaignfortheirhelpinexecutingtheexperimentsandBob Dawsonforhisassistanceduringthecampaign. ofrestitution.ThiscorroboratespreviousresultsbyHeißelmann etal.(2010)andPaperI.Historically,thecoefficientsofrestitu- tion determined by Bridges et al. 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