Radiohalos and Diamonds - CiteSeer

In A. A. Snelling (Ed.) (2008). Proceedings of theSixth International Conference on Creationism (pp. 323–334).Pittsburgh, PA: Creation Science Fellowship andDallas, TX: Institute for Creation Research.Radiohalos and Diamonds:Are Diamonds Really for Ever?Mark H. Armitage, M.S. Ed.S., Microspecialist, 587 Ventu Park Road 304, Thousand Oaks, CA 91320Andrew A. Snelling, Ph.D., Director of Research, Answers in Genesis, P.O. Box 510, Hebron, KY 41048AbstractRadiohalos were first reported in diamonds more than a decade ago. Since that time little workhas been done to locate other radiohalo-bearing diamonds, to explain the origin of the radiohalos,or evaluate their significance. We conducted a search for such diamonds secured from a variety ofsources and identified radiohalos containing one, three and four rings, as well as strange featuresin the form of twisted crystalline “tubes.” New data suggest a radiohalo annealing temperaturein diamond above 620 o C. We offer an explanation for the radiohalos and for the “tubes” in thesediamonds in terms of a hydrothermal fluid transport model for Po radiohalo formation.KeywordsRadiohalos, Diamonds, Diamond inclusions, Zircons, Polonium, Kimberlite, Hydrothermal fluids,CleavagesIntroductionDiamonds are probably the most intensely soughtafter of all the mineral gems known to man. Indiawas the earliest producer of diamonds in the sixthcentury, with monarchs as their primary customers.Diamonds remained very rare and only a privilegedfew had them, until the first commercial diamondmine was opened in the late 1860s in South Africa(Meyer, 1985). It was Marilyn Monroe who in 1953immortalized the phrase, “Diamonds are a girls’ bestfriend” in a song from the movie, “Gentlemen PreferBlondes”. Of course, it had already become acceptedpractice for a marriage proposal to be secured witha diamond ring. It was DeBeers, a privately ownedcommercial enterprise, and still the largest seller ofdiamonds in the world with revenues of US$65 billionin 2005 alone, who in 1947 launched the successful“A Diamond is Forever” marketing campaign(Wikipedia, 2007). The unmatched brilliance of thesparkle of diamonds, their sizes and colors make themdesirably attractive, but it is their unique hardnessand resistance to physical weathering that givethem their durability. Today, over 130 million carats(US$10–13 billion) of diamonds are mined annually(Wikipedia, 2007).Tiny, microscopic radioactive halos (or radiohalosfor short,) were first reported in diamonds only adecade ago (Armitage, 1993, 1995). This discoveryelicited some brief discussion (Armitage, 1998;Gentry, 1998; Wise, 1998), but little has been donesince to elucidate their enigma. The purpose of thisstudy was to find additional diamonds containingradiohalos and to investigate in greater depth howthey might have formed.DiamondsDiamonds are classified into two major categories—Type I, which contain nitrogen, and Type II, which donot (Meyer, 1985). There are four generally recognizedsub-categories based on the form and placement ofthe nitrogen, and the presence or absence of boron.Type Ia diamonds, for example, which may compriseover 98% of the world’s natural diamonds, containfrom 200 ppm up to a maximum of 5500 ppm nitrogendistributed in small clusters or aggregates of nitrogenatoms through the diamonds (Evans, 1992). Diamondsin this category are normally colorless, light yellow orbrown. Type Ib diamonds, which comprise around 1%of natural diamonds, are yellow and contain lesseratoms (150–600 ppm) of nitrogen in individual carbonsubstitution sites. Normal colors of this type rangefrom light to bright yellow or even amber. Type IIadiamonds comprise less than 1% of all diamonds andcontain very small concentrations of nitrogen atomsin the range of 4–40 ppm (undetectable or barelydetectable by infrared spectroscopy). These diamondsare generally colorless or brown. Some of the world’svery large diamonds are in this category. Type IIbdiamonds, the rarest and purest type, contain up toaround 20 ppm boron and even less nitrogen. Theseare usually blue or grey in color, and are electricallyconductive.The origin and formation of diamonds is not yetcompletely understood, but it is generally accepted

324that diamonds crystallized from a liquid melt in theearth’s upper mantle at depths of between 150 and300 km (Kirkley, Gurney, & Levinson, 1991). At thesedepths the temperatures range from 1100–2900° Cand the pressures range from 50–100 kilobars, ascalculated and confirmed by laboratory studies ofthe minerals in rock fragments brought up from theearth’s upper mantle with the diamonds in volcanicrocks (Mitchell, 1991). Some diamonds may even haveformed at depths of 450 km below the earth’s surface,because of the great temperatures and pressuresrequired for certain mineral inclusions in them toform (Meyer, 1987).Most natural diamonds so far discovered arethought to have crystallized between 1 and 3 billionyears ago in mantle rock containing relatively highconcentrations of magnesium and iron (Meyer, 1985;Stachel, Banas, Muehlenbachs, Kurszlaukis, &Walker, 2006). The processes of diamond formation areinferred on the basis of what is known of conditions inthe earth’s upper mantle at 150–300 km depth (Rice,2003; Shirey, Richardson, & Harris, 2004; Tappert,Stachel, Harris, Muehlenbachs, Ludwig, & Brey,2005). The origin of the carbon source for diamondsis also still very much debated (Banas, Stachel,Muehlenbachs, & McCandless, 2007; Gunn & Luth,2006; Rice, 2003). Once formed, the diamonds seemedto have resided for hundreds of millions up to 2 billionyears in the upper mantle beneath the Archeankeels of the continental Precambrian cratons. Thediamond phase of carbon, once crystallized, remainsstable there, because of the high temperatures andpressures.It is generally postulated that localized meltingof the mantle subsequently occurred to produce amagma rich in CO 2and H 2O, either a kimberlite orlamproite. This volatile-rich magma then began risingexplosively through the mantle areas containing thediamonds and transported the diamonds through thecrust to the earth’s surface at speeds of 10–30 kmper hour via propagating cracks in the mantle andthe crust above (Kelley & Wartho, 2000; Snelling,1994). The kimberlite and lamproite magmas cooledas they approached the earth’s surface and thereforehardened, so the resultant explosive eruptions oftenshattered the solidified magmas in what were coldvolcanic eruptions. What remained in the conduit andthe material that settled back into it after the eruptionscontains the diamonds in pipe-like structures. If thesekimberlite and lamproite magmas did not ascendcatastrophically from the upper mantle to the earth’ssurface within 8–24 hours, the diamond crystalswould have become unstable at the changing pressureand temperature conditions during their passageand would have reverted to graphite. At the earth’ssurface these kimberlite and lamproite pipes weatherM. H. Armitage & A. A. Snellingand are eroded so the diamonds are shed into alluvialdeposits in river systems, deltas and along coastlines.The diamonds that remain in the pipes may be mined,often from great depths. For some diamond depositsno formation process has been proposed (Banas et al,2007; DeStefano, Lefebvre, & Kopylova, 2006; Leost,Stachel, Brey, Harris, & Ryabchikov, 2003; Stachel,Viljoen, McDade, & Harris, 2004).Efforts to produce gem-grade synthetic diamonds,though intensive, have produced only meager results.In 1955 researchers at General Electric successfullysynthesized tiny industrial-grade diamonds overseveral weeks of extreme laboratory temperaturesand pressures over intervals of several weeks(Koskoff, 1981). Since then many small industrialgradediamonds have been produced (some estimatesare as high as 100,000 carats per year). In order toproduce these diamonds, carbon must be subjected tovery high pressures and temperatures in the presenceof transition metals (or some other “seed”) to get thereaction started (Gunn & Luth, 2006; Langenhorst,Poirier, & Frost, 2004; Zhou, Jia, Chen, Guo, & Li,2006). Although gem quality diamonds as large as5 carats have been produced, the cost of productiongenerally remains prohibitively high. DeBeers claimsthat their equipment can detect the difference betweensynthetic and natural diamonds; but that claim ishighly disputed. Synthetic gemstones larger than 1carat are not readily produced or available.Diamonds are mentioned in several places in theScriptures. A diamond was among the 12 gemstoneson the high priest’s breastplate representing the 12tribes of Israel before God (Exodus 20:18; 39:11).Diamonds were thus looked upon by God as things ofbeauty, purity and value. Indeed, in reference to the“anointed cherub” in Ezekiel 28:13–14, his coveringin “the garden of God” and “upon the holy mountainof God” was “every precious stone” including thediamond. This implies that diamonds, along withother gemstones, were present in and on the earthafter God created it, so if diamonds are really as “old”as claimed, then they may date back to the originalcreation. Their presence in the earth’s crust todayand at the earth’s surface may then largely be due tothe subsequently eruption of kimberlite and lamproitemagmas during the Flood. Diamonds and their originhave occasionally featured in creationist news reportsand literature (Baumgardner, 2005; Brown, 1997;Chaffin, 1986; DeYoung, 1982; Oard, 2004; Sarfati,2006; Snelling, 1994, 1996).Inclusions in DiamondsNatural diamonds (and many other crystallinematerials) often encase smaller grains or crystalsof other minerals within their crystalline matrices,and these are known as inclusions. Twenty to thirty

Radiohalos and Diamonds: Are Diamonds Really for Ever?different minerals have been described as inclusionsinside natural diamonds, along with 58 different typesof impurities, including uranium and thorium (Meyer,1987). Synthetic diamonds also suffer from inclusions,but these are mostly metal fragments introducedin the manufacturing process (Langenhorst et al,2004). In the case of the natural diamonds, theseincluded minerals must have been present at thetime the diamonds formed to be incorporated withinthe diamond matrix. As far as has been ascertained,diamonds are almost completely chemically inert andextremely resistant to any contamination or chemicalexchange within their crystal lattice. This means theywould have traveled from the earth’s upper mantleand through the crust to the earth’s surface carryingthese inclusions completely intact and unchangedduring the 150–300 km ascent (Baumgardner, 2005;Dobrzhinetskaya, Green, Bozhilov, Mitchell, &Dickerson, 2003; Meyer, 1985; Promprated, Taylor,Anand, Floss, Sobolev, & Pokhilenko, 2004; Tappertet al., 2005). Therefore, these inclusions represent tiny“capsules” of mantle materials captured under mantleconditions that have been safely delivered from theupper mantle to the earth’s surface. Yet there are someas yet unexplained mysteries concerning the typesof inclusions found in diamonds. For example, it iswell known that sulfides represent the most commoninclusions in diamonds, implying that these sulfidesformed in the mantle. Yet many mantle xenolithsbrought from the upper mantle to the earth’s surfaceby volcanic eruption contain only small quantities ofsulfides (Westerlund, Guknhy, Caklson, Shirey, Hauri,& Richardson, 2004). Furthermore, it is puzzling asto how saline liquids and water, plus gases, are oftenencapsulated as fluid inclusions within diamonds atsuch depths (and pressures).Inclusions consist of, but are not limited to, apatite,calcite, carbonates, chromite, smaller diamonds,garnet, hematite, iron, mica, pyrite, pyroxene,silicates, sulfides, zircon, and, as mentioned, liquids(such as liquid CO 2, water and even brine) and gases(Anonymous, 2001, 2003; Bizzarro & Stevenson,2003; Jacob, Kronz, & Viljoen, 2004; Klein-BenDavid,Izraeli, Hauri, & Navon, 2007; Navon, Izraeli, & Klein-BenDavid, 2003; Promprated et al., 2004; Stachel etal., 2004, Tappert et al., 2005; Tomlinson, Jones, &Harris, 2006; Westlund & Gurney, 2004).Frequently mineral inclusions contain radioactivenuclides such as uranium or thorium incorporatedwithin the crystalline lattice of the inclusion. Theseradioactive nuclides eject alpha particles as a normalpart of the radioactive decay process. Alpha-particlestravel some distance in the mineral (and then intothe surrounding host) depending on the energy atwhich they were ejected from the nucleus of thenuclide as well as the characteristics of the crystalline325material(s). The crystalline lattice structure ofinclusions, including zircons, may tend to becomesomewhat amorphous over time if sufficient selfirradiationtakes place (Nasdala, Wenzel, Andrut,Wirth, & Blaum, 2001; Nasdala, Wildner, Wirth,Groschopf, Pal, & Moller, 2006).The presence of zircons in diamonds is consideredrare, but they have been previously reported (Kinney& Meyer, 1993, 1994). It may be that few reports ofzircon inclusions have appeared because zircons arenot expected to be at depths in the mantle wherediamonds are thought to form (Meyer, 1985). Theconsensus is that zircons exist predominately in theearth’s crust. Because of their extreme hardness, itis unlikely that diamonds can incorporate zirconsfrom the crust during their ascent from the mantleto the earth’s surface (J. Baumgardner, personalcommunication, April 2, 2007). Nevertheless, zirconinclusions occur within diamonds and have beenreported (Kinney & Meyer, 1993, 1994). Furthermore,there have even been reports of diamond inclusionswithin zircons (Dobrzhinetskaya et al., 2003; Kinneyand Meyer, 1994; Menneken, Nemchin, Geisler,Pidgeon & Wilde, 2007), but these are microdiamondsformed under ultrametamorphic conditions in theearth’s crust (Dobrzhinetskaya et al., 1995; Snelling,1996).Zircons are known to contain radioactive nuclides(such as described above) and they are also well knownin their role as radiocenters for 238 U radiohalos, whichhave been observed in biotite, chlorite, cordierite,fluorite, sapphire, quartz and other minerals(Coenraads, Sutherland, & Kinney, 1990; Gentry,1973; Ion, Ion-Mihai, Ion, & Sandru, 2003; Nasdalaet al., 2001, 2006; Pal, 2004; Snelling, 2000, 2005a).One well-known researcher commented, however, thathe was not aware of any report describing uraniumin diamond (K. N. Bozhilov, personal communication,June 16, 2006). Nevertheless, zircon inclusions insapphires are known to contain uranium, the parentradionuclide for polonium (Coenraads, Sutherland,& Kinney, 1990) and others have described suchradioactive elements in other rocks from diamondbearingkimberlites (Kramers, 1979).Radiohalos are minute circular areas (in crosssection)of discoloration and darkening caused bydamage from α-particle radiation emanating from atiny central inclusion containing radioactive elementssuch as U and Th (Gentry, 1973; Snelling, 2000). Thedamage is mostly from point vacancies produced in thecrystal lattice of the host mineral by the α-particles.The identity of the isotopic species responsible for agiven ring in the darkened region can be determinedfrom the ring’s diameter, which is proportional tothe energy of the alpha particles emitted by theisotopic species. The rare element polonium (Po) is

326momentarily produced as three isotopes in the 238 Udecay chain— 218 Po, 214 Po and 210 Po. Whereas a 238 Uradiohalo consists of eight rings, radiohalos are alsofound with only three, two and one rings, resultingfrom, respectively, the α-decay of these three Poisotopes. Such 218 Po, 214 Po, and 210 Po radiohalos hadto have been produced with the respective Po isotopesexclusively present in their radiocenters. It has beenestimated that each radiohalo requires between 500million and 1 billion α-particles to form it (Gentry,1988).Doubts have been raised concerning whetherradiohalos interpreted as polonium radiohalos havebeen correctly identified. For example, Moazed,Spector, and Ward (1973) and Moazed, Overbey,and Spector (1975) claim that single, double, tripleand quadruple ring radiohalos can clearly andunambiguously be shown to have been generatedby the 238 U and 232 Th decay chains, rather thanby “parentless” polonium isotopes as proposed byGentry (1974, 1984, 1986, 1988). This claim is basedpartly on the issue of potential uncertainties in theion microprobe analyses of the halo radiocenters.However, Gentry (1974, 1986) and Gentry, Hulett,Cristy, McLaughlin, McHugh, and Bayard (1974)have refuted this claim, demonstrating that due carewas taken in these analyses, and other techniqueswere employed for comparison to rule out suchuncertainties. Furthermore, most of the many othersthat disagree with Gentry’s model for the formationof these polonium radiohalos have accepted theircorrect identification (for example, Damon, 1979;Dutch, 1983; Wakefield, 1988; Wilkerson, 1989;York, 1979). Indeed, Collins (1992) goes furtherand specifically includes the Moazed, Overbey, andSpector (1975) claim in his list of attempts to explainGentry’s conundrum that are not fully satisfactory. Inany case, Meier and Hecker (1976) have conclusivelyshown that polonium radiohalos are sometimesassociated with polonium bands generated by thepolonium being transported by hydrothermal fluidsalong fractures. Thus the overwhelming consensusis that the polonium radiohalos have been correctlyidentified.The formation of Po radiohalos has thus beensomewhat enigmatic, given the short half-lives of thethree Po isotopes—3.1 minutes, 164 microsecondsand 138 days, respectively. Conventionally the Poradiohalos have been called “a very tiny mystery”without further explanation (Dalrymple, as quotedby Gentry, 1988, p. 122). The mystery in question ishow these polonium isotopes could have been derivedand separated from a nearby source of 238 U to thenbe concentrated in radiocenters to produce the Poradiohalos, all within ten half-lives of these Po isotopes,corresponding to their effective life-spans (1.64M. H. Armitage & A. A. Snellingmilliseconds in the case of 214 Po). Therefore, Gentry(1974, 1984, 1986, 1988) proposed that the poloniumhad to have been primordial, created in place in theradiocenters and then nearly instantaneously producethe Po radiohalos. Furthermore, he maintained, if thePo was primordial, then the host crystals and rocks(for example, biotite flakes and their host granites)also had to have been created at the same time.However, as pointed out by Wise (1989) and Snelling(2000), many granites that contain Po radiohalosappear from their geologic contexts to have beenformed during the Flood, and therefore cannot havebeen primordial (that is, created) granites. Thisin turn implies that the Po which generated the Poradiohalos in those granites could not have beenprimordial Po. Indeed, Snelling and Armitage (2003)studied three specific Po-radiohalo-bearing graniteplutons that they demonstrated had to have beengenerated and formed during the Flood. Therefore,Snelling and Armitage (2003) and Snelling (2005a)proposed a hydrothermal fluid transport model forPo radiohalo formation, which has been tested andverified by subsequent studies (Snelling, 2005b, 2006,2008; Snelling & Gates, 2008).Mendelssohn, Milledge, Vance, Nave, and Woods(1979) reported finding radiohalos on the outer surfacesof opaque diamonds using cathodoluminescence.Armitage (1993, 1995), however, was the first to reportoptically-visible, multi-ringed internal radiohalos ina Type Ia diamond. Despite the fact that exact sizematching with the radiohalos observed in biotiteswas difficult because of the greater density of thediamond’s carbon structure reduces the penetrationdistance of the α-particles, these radiohalo rings werenevertheless identified as produced by 218 Po, 214 Po,210Po, and 222 Ra. Furthermore, these radiohalos werefound along rod-like structures and at the terminiof strange hollow tubes that were bent repeatedlyat right angles within the diamond. Wise (1998)suggested that these structures represented fluidconduits along which the radioisotopes responsible forparenting these radiohalos had been transported intothe diamond, but both Armitage (1998) and Gentry(1998) maintained that this interpretation was notviable due to the diamond’s unfractured internalcrystal structure. They insisted instead that the shorthalf-lives of the radioisotopes responsible for the ringsin the radiohalos suggested a primordial origin for theradioisotopes and thus the diamond. Nevertheless,Vicenzi, Heaney, Snyder, and Armstrong (2002)reported radiation halos 25 micrometers in diameterin alluvially deposited polycrystalline diamonds(carbonados) from the Central African Republic, whichthey maintained were generated as a result of uraniumdeposition from a single pulse of fluids infiltrating thediamonds following their formation. Furthermore,

Radiohalos and Diamonds: Are Diamonds Really for Ever?whereas J. W. Harris (personal communication,May, 2007) has claimed, “over decades of looking atmillions of diamonds I have only once seen a green setof haloes inside a stone,” jewelers and gemologists insouthern California testify to having regularly seenradiohalo inclusions in diamonds and other gemstones(Armitage, personal communications with jewelers insouthern California, April, 2007; May, 2007).Diamonds ExaminedSixty-nine small diamonds and diamond chips fromdiamond mines in Kimberley (South Africa), Jwaneng(Namibia), and Orapa (Botswana), and from alluvialdiamond deposits in Namibia and Guinea, wereexamined for radiohalos. These diamonds were in thepossession of Dr. John Baumgardner at the Institutefor Creation Research in Santee, California. The twodiamonds with radiohalos in them examined in thisstudy were on loan from the Gemological Instituteof America laboratory (GIA), Carlsbad, California,courtesy of Dr. John Koivula and Thor Strom. Thefirst of these diamonds was a 0.06 carat, faceted stonefrom an unknown source. The other was described asa 0.11 carat diamond macle (or oddly shaped crystal)from the Diamantina mines, Gerias, Brazil.The diamonds of interest were photographed withfilm on a Zeiss Jena dissecting light microscopeconfigured with multiple fiber optic illuminators andan Olympus SLR film camera body. Illumination ofradiohalos proved difficult particularly since bothspecimens had been carbon-coated for examinationwith scanning electron microscopy (SEM), butSEM was not performed in this study. Prints of thenegatives made were digitally scanned.Twenty different jewelry stores in three countiesin southern California were visited over a period ofseveral weeks. Jewelers and gemologists at thosestores were interviewed. Half of the proprietorsstated that they had seen such radiohalo inclusionsin diamonds and other gemstones previously butFigure 1. Small inclusions in diamond from Orapa mine,Africa. Magnification 250×. Scale bar = 300 microns.327none of the twenty had any gemstones available forexamination.ResultsNo radiohalos were found in any of the Africandiamonds. However, large numbers of variousinclusions (including possible zircons) were foundin them and some in the Orapa diamond werephotographed (Figure 1).Radiohalos with one, three, and four rings werefound in the GIA diamonds. The round brilliant cut0.06 carat diamond from an unknown source containeddozens of radiohalos and “etch trails” (Figures 2–4).Documentation was provided with this diamond. Itdescribed “etch trails” which intersected with theradiocenters of each halo sharply bent at differingangles (see Figure 4). These “etch trails” did notextend to the surface. Therefore, the diamond girdlewas ground away by GIA personnel until contactwith the etch trails was made (see ground girdle onFigures 4–5). The text stated that inclusions weresolid (crystalline?) and that “they appear to have ahexagonal outline.” These radiohalos (both 3 and4 ring varieties) were measured with a calibratedocular micrometer to 50 micrometers diameter.The diamond macle (oddly shaped crystal) fromBrazil (Figures 7–8) contained dozens of radiohalos,but only of the single ring variety. This documentationsupplied with this specimen stated “this 0.11 caratdiamond macle is from Diamantina mines, Gerais,Brazil. Its radiation spots with central ‘cores’ arefrom some unknown substance. These spots startedout green and changed to brownish orange when thediamond was heated to 620 °C. The first change in spotcolor was noticed at 590–600 °C.” These radiohalos(single ring only) were measured with a calibratedocular micrometer to 30 micrometers diameter.DiscussionThe crucial factor in the occurrence of the radiohaloswithin these two diamonds is the temperature atwhich radiohalos are annealed. At the annealingtemperature the vibrations of the atoms in the crystalstructure have increased sufficiently to repair thepoint vacancies caused by the previous α-particlebombardment, such that the darkening, and thusthe radiohalos, are erased. In biotites, radiohalosare erased above 150 °C (Laney & Laughlin, 1981).This annealing temperature was determined usingsamples taken from a drill-hole in which present insitu temperatures had been measured, and so could beinterpreted as having been determined under naturalconditions. In contrast, Armitage and Back (1994)placed biotite flakes containing radiohalos in an oven,heating them at temperatures up to 700 °C for up tofive hours. They found erasure of radiohalos occurred

328M. H. Armitage & A. A. SnellingFigure 2. Round, brilliant cut diamond. Note radiohalosat 12 o’clock position. Scale bar = 0.3 mmFigure 3. Radiohalos in round diamond. Magnification80×. Scale bar = 450 micrometers.Figure 4. Radiohalos in round diamond. Note right andsharp angles made by crystalline tubes. Magnification80×. Scale bar = 450 micrometers.Figure 5. Radiohalos in round diamond. Magnification100×. Scale bar = 160 micrometers.Figure 6. Radiohalos in round diamond. Magnification200×. Scale bar = 75 micrometers.after only an hour of heating at temperatures of250–550 °C. However, it is not known whetherradiohalos in diamonds are annealed at 150–250 °C.The Brazilian macle diamond was reported to havebeen heated to 620 °C without complete loss ofradiohalos. This would seem to imply that theannealing temperature of radiohalos in diamonds isFigure 7. Radiohalos in macle diamond from Brazil.Magnification 200×. Scale bar = 1 mm.higher than 620 °C.The temperatures at the 150–300 km depthsin the upper mantle where diamonds are inferredto have formed are 1100–2900 °C. Of course, anyradiohalos would only be generated in diamonds afterthe diamonds formed at those temperatures. If theannealing temperature of radiohalos in diamonds is

Radiohalos and Diamonds: Are Diamonds Really for Ever?Figure 8. Radiohalos in macle diamond. Magnification90×. Scale bar = 0.5 mm.higher than 620 °C, there is a greater temperaturewindow (compared with the 150 °C annealingtemperature of radiohalos in biotites) in whichmagmatic and hydrothermal fluids could transport238U and its decay products into and within diamonds.This assumes that 238 U, its decay products, or tinycrystals of a mineral such as zircon hosting them,had not been included in diamonds when they formed.Zircon inclusions in diamonds are considered to berare, but at the upper mantle temperatures at whichdiamonds have supposedly resided for hundredsof millions of years, before transport to the earth’ssurface by kimberlite and lamproite magmas, it ishighly unlikely radiohalos would have formed aroundany zircon inclusions.Instead, it is far more likely that 238 U and its decayproducts infiltrated the diamonds during and aftertheir ascent to the earth’s upper crust. However, whilekimberlite and lamproite magmas are volatile-rich,particularly with respect to CO 2, they contain verylittle water and so produce dry volcanic eruptions.Thus, as water is the likely transporter of 238 U and itsdecay products, the infiltration of water transporting238U and its decay products to form the radiohalos indiamonds would need to occur after the emplacementof the host kimberlite or lamproite at and near theearth’s surface. Indeed, even though the kimberliteand lamproite magmas are considered dry, they arenonetheless very hot (>1,000 °C) when emplaced,and their interaction with the ground waters in theimmediately surrounding intruded strata wouldgenerate in situ hydrothermal fluids (Snelling &Woodmorappe, 1998). That such fluids are generatedis confirmed by the ubiquitous hydrothermallyproduced minerals such as serpentine in kimberlitesand lamproites. Such fluids would scavenge, dissolve,and concentrate 238 U and its decay products from boththe intruded strata and the congealed, rapidly cooled,and explosively fragmented intruding magmas.The next question has to be whether magmatic and329hydrothermal fluids can infiltrate into diamonds. BothArmitage (1998) and Gentry (1998) insisted that fluidinfiltration was not possible due to the unfractured,tight internal crystal structure of diamonds. However,Vicenzi et al (2002) maintained the radiohalosthey found in alluvially deposited carbonados weregenerated as a result of uranium deposition froma single pulse of fluids having infiltrated thosemicrocrystalline diamonds after their formation. Thecrystal structure of diamonds is cubic, and even thoughdiamonds fracture conchoidally, they exhibit cleavagein four directions (octahedral) with one perfect cubiccleavage {111} (Mason & Berry, 1968). As in the caseof the radiohalos in the diamond documented byArmitage (1994), many of the radiohalos in one ofthe diamonds in our study are centered along thindarkened straight lines within the diamond. Theselines appear to follow the directions of the cleavages(Figures 3–5). Other radiohalos are at the termini ofstrange darkened tubes that turn and twist at rightangles (Figure 4). Wise (1998) interpreted all thesefeatures as conduits along which fluids must havetransported the 238 U and its decay products responsiblefor the radiohalos. This interpretation is supported bythe observations made by Armitage and Back (1994)and in our study that the darkening along theselinear features and twisted tubes is due to radiationstaining. Furthermore, these linear features and thelinear sections of the twisted tubes appear to followthe perfect cleavages within the diamonds. Thesecleavages are the natural weaknesses of the diamondcrystal lattice along which infiltrating fluids might beexpected to flow.This interpretation raises several issues. Again, theintact crystal structure of diamonds, without clearlydeveloped fracture surfaces along cleavages, wouldseem not to be capable of providing open avenues forfluid infiltration. However, this concern is based onobservations of diamonds at ambient temperatures.By contrast, at the temperatures of 300–400 °C atwhich magmatic and hydrothermal fluids might haveinfiltrated, the heat would likely have expanded thediamond crystal structure, thus opening cleavageplanes to provide the necessary pathways for thesefluids. Yet how are these darkened linear featuresand “tubes” produced by fluid infiltration whencleavage planes are two-dimensional surfaces? Giventhat the diamond crystal structure is normally tight(close-packed), if the cleavages within it are openedby heat and fluid pressures, the easiest, most open,pathways for fluids to infiltrate would be at the linearintersections of cleavage planes. It then follows thatbecause there are essentially five cleavage planes indiamonds, the lines of intersection between them runin numerous directions, which would account for thetwisted tubes.

330It would also be precisely because of the tightcrystal structure of diamonds that some of thesetubes are twisted at right angles. Because all thecleavages are at varying angles only a few right angleswould seem possible, but the cubic cleavage plane isregarded as perfect (Mason & Berry, 1968). Armitage(1998) described these strange twisted tubes as solidinclusions, rather than being hollow as previouslythought (Armitage, 1994). A few of these twisted tubeswere found to extend to the surface of the diamond(Armitage, 1994), and not all of them terminated at aradiohalo. Furthermore, in both the Armitage (1994)diamond and the cut diamond in our study, both thedarkened linear tubes with radiohalos centered alongthem, and the twisted tubes terminating in radiohalos,usually do not reach the surfaces of these facetedstones. This would seem to argue against these tubeshaving been formed by fluid infiltration. However,the character of these tubes, and their containmentof solid mineral inclusions, suggest their formation asmineral inclusions via precipitation from infiltratingfluids. These would have to have been trapped in thediamond crystal structure long enough for the mineralmatter dissolved in them to precipitate.It is thus envisaged that with the emplacementof the host kimberlite pipe, connate water in thesurrounding intruded strata was heated by thecooling kimberlite, and the hydrothermal fluidsthus generated infiltrated the still warm diamondswithin the kimberlite, carrying 238 U and its decayproducts scavenged from the intruded strata. Heateddiamonds expanded sufficiently to facilitate fluidinfiltration along cleavage planes; but because of thetight diamond crystal structure, where the fluidsmet resistance within the diamonds because thecleavages would not open further, the fluids insteadexploited any weakness along the intersectionsbetween other cleavage directions. Thus some of thelinear fluid pathways became twisted repeatedly atright angles as the fluids infiltrated where cleavageintersections were sufficiently open to them. As thediamonds first cooled at their outer surfaces, thecleavages infiltrated by the fluids would contract andclose first at their outer surfaces, locking the fluidsinto those cleavages where the contained elementsand minerals then precipitated. Because 238 U and itsdecay products were dissolved in these infiltratingfluids, α-radiation tracks would be left along thecleavage pathways traversed by the fluids. The 238 Udecay products in the fluids apparently becameconcentrated in nucleation or precipitation centers,where trace atoms such as Cl (present in diamonds)chemically attracted Po. These precipitated Po atomsthen “parented” the now observed radiohalos. Thehalf-lives of these radioisotopes are short ( 210 Po 138days, 218 Po 3.1 minutes, and 214 Po 164 microseconds);M. H. Armitage & A. A. Snellingbut isolated 214 Po radiohalos may be accounted forby retention in the infiltrating fluid of the 27-minutehalf-life parent 214 Pb and the 20-minute half-lifeparent 214 Bi. Similarly, isolated 210 Po radiohalos maybe accounted for by retention of the 22-year half-lifeparent 210 Pb and the 5-day half-life parent 210 Bi. Asatisfactory explanation for the observed densityratios of polonium radiohalos awaits further study.The single ring radiohalos in the Brazilianmacle diamond, most probably 210 Po radiohalos, aredispersed randomly and sometimes apparently inclusters, and do not seem to be along any radiationstainedlinear features (Figures 7–8). This doesnot mean the 210 Po was not transported into thisdiamond by fluid infiltration along cleavages. Rather,it suggests that the 210 Po transport was so rapidthere was insufficient time for radiation stainingto develop along the cleavages infiltrated by thefluids. Furthermore, the oddly shaped nature of thismacle diamond has two other implications. First, itscontraction accompanying cooling after emplacementwould have been very rapid due to its likely less orderlycrystalline structure; and thus fluid infiltration toproduce these 210 Po radiohalos also needed to be veryrapid. And second, the packing of its crystal structurewould mean that its cleavages are not as well defined,and the infiltrating fluids would have more readilydispersed around the constituent components ofits crystal lattice rather than along cleavages. Thisis consistent with its distribution pattern of 210 Poradiohalos. However, since only 210 Po radiohalos arepresent in this macle diamond, the infiltrating fluidslikely only transported 210 Po scavenged from the hostkimberlite and the intruded strata. The fluids whichinfiltrated the other diamond we studied had to havecarried radioisotopes higher up the 238 U decay chain,at least up to 1,000 year half-life 226 Ra, which isreadily soluble in most fluids.All these considerations indicate time limits onthe fluid infiltration process to generate the poloniumradiohalos is the order of hours or weeks. This isconsistent with the evidence of the rapid speed(within hours) at which diamond-bearing kimberlitepipes are explosively emplaced. Additionally, onceemplaced, complete cooling of the fragmentedcongealing kimberlite magma is also rapid (withindays or weeks) at the surface, and in the near-surfaceenvironment beneath where heated meteoric waterscontaining Ra, Rn, and Po scavenged from the hoststrata would rapidly penetrate into the kimberliteand mix with any magmatic and hydrothermal fluids.Rapid hydrothermal fluid transport of 210 Po in thenatural environment has been documented (Snelling,2000). Hussain, Church, Luther, and Moore (1995)found that the residence time of 210 Po in hydrothermalfluids venting on the ocean floor was of the order of

Radiohalos and Diamonds: Are Diamonds Really for Ever?only a few minutes, and that the residence time of thehot fluids in the hydrothermal system was no morethan 30 days. Furthermore, the hydrothermal fluidsin geothermal and mid-ocean ridge vent systemsare estimated to circulate through rock volumes ofseveral cubic kilometers over distances of severalkilometers (Lowell, Rona, & Von Herzen, 1995;Nicholson, 1994), transporting 210 Po within 20–30days. Given the explosive emplacement of the hotkimberlite pipes and the rapid penetration into themof hydrothermal fluids transporting Ra, Rn, and Po,infiltration of hydrothermal fluids carrying Po intothe diamonds within the hot fragmented kimberlitewould have needed to be rapid to deposit the Po intime to generate the Po radiohalos before the wholesystem cooled rapidly, the diamond cleavages “closed,”and hydrothermal fluid circulation ceased.ConclusionsEven though the available data suggest theerasure temperature of radiohalos in diamondsmay be above 620 °C, the 1100–2900 °C conditionsin the mantle where diamonds form would be toosevere for radiohalos to form there. Furthermore,the temperature of the kimberlite and lamproitemagmas that transported diamonds to the uppercrust, the short transit times, and the lack of water totransport radioisotopes into diamonds, would militateagainst radiohalos being formed during the ascent ofdiamonds from the mantle. Thus the radiohalos in thediamonds examined in this study must have formedafter emplacement of their host kimberlite/lamproitepipes at or near the earth’s surface.The emplacement of the hot, dry kimberlite/lamproite magmas in pipes would result in heatingof the connate water in the surrounding intruded(host) strata. The hydrothermal fluids thus producedwould then scavenge and concentrate trace amountsof 238 U and its decay products, transporting them intothe kimberlite/lamproite pipes via convective flow.Due to expansion of the still hot diamonds, thesefluids would have infiltrated the diamonds alongthe cleavages within them. Where resistance wassometimes encountered because of the diamonds’tight crystal structure, the fluids exploited othercleavage directions, resulting in fluid pathways, whichtwisted repeatedly at right angles. The α-decay of theradioisotopes in the fluids often left dark radiationstains along these linear and twisted fluid pathways.Contraction of the outer surfaces of the diamondswould have closed termination of cleavages there,thus trapping the infiltrated fluids to precipitatethe mineral matter that forms the observed tubes.Precipitation of 238 U decay products in nucleationcenters along, and sometimes at the end of, these fluidinfiltrated cleavages where chemical conditions were331conducive produced concentrations that generatedthe observed polonium radiohalos. All considerationsindicate severe time limits on the fluid infiltrationprocess—on the order of hours or weeks.Radiohalos in diamonds can be explained by thehydrothermal fluid transport model for Po radiohaloformation; but they cannot answer the question: arediamonds really for ever? 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