Neutron beam from JRR-3M at JAERI was employed for reactor neutron-induced PGA. Fluctuation in neutron flux were monitored by a neutron counter and du

(1)

Proceedings or the Fifth International Symposium on

Advanced Nuclear Energy Research —NEUTRONS AS MICROSCOPIC PROBES—

410

REACTOR NEUTRON-INDUCED PROMPT GAMMA-RAY ANALYSIS AND INSTRUMENTAL NEUTRON ACTIVATION ANALYSIS OF ANCIENT GLASSWARE

T.TOMIZAWA', C.YONEZAWA2, Y.MINAI3, M.HOSHI2,

V.ITO4 and T.TOMINAGA3

1) Faculty of Literature, Keio University, Mita, Tokyo, Japan

2) Japan Atomic Energy Research Institute 3) School of Science, University of Tokyo,

Hongo, Tokyo, Japan

4) Research Center for Nuclear Science and Technology, University of Tokyo, Yayoi, Tokyo, Japan

ABSTRACT

Elemental composition of ancient glassware provides a clue to estimate provenance, source material, and manufacturing procedures. In determination of their compositions it is usually desirable to apply non destructive analytical techniques because even the shape of artifacts should be preserved as excavated for future studies. Reactor neutron-induced prompt gamma-ray analysis (PGA), instrumental neutron activation analysis (INAA), and X-ray fluorescence analysis (XRF) are simultaneous multielement

analytical methods providing information on elemental composition. Beside, both techniques are non destructive method, which are appropriate for studies of such artifacts. In this work we have reported the elemental composition of ancient glassware (from the Yayoi period to the Edo period) excavated from the ruins in Japan to estimate provenance, source material, and manufacturing procedures.

—

826-P-410

Pr，町田dingsof the Fifth International Symposium on

Advanced NucJear Energy R出国rch

NEUTRONS AS MICROSCOPIC

PROBES-REACTOR NEUTRON-IN臥JCEDPROMPT GA附A-RAVANALVSIS AND INSTRUMENTAL NEUTRON ACTIVATION ANALVSIS

o

r

ANCIENT GLASSWARE

T.T開IZAWA1

，

_C_._Y_O_N_E_Z_A_W_A₂

，

_Y_._附_NAP

阿

，

_._"_O_S_"₁₂

，

Y.IT04 and T.TOMINAGA3

1)Faculty of Literature

，

Keio University

，

Mita

，

Tokyo

，

japan

2)japan Atomic Energy Research Institute

3)Sc加01 of Scie恥e

，

University of Tokyo

，

Hongo

，

To

旬

。

，

japan

4 )

Research Center for Nuclear Science and Technology

，

University of Tokyo

，

Vayoi

，

Tokyo

，

Japan

ABSTRACT

Elemental c棚 positionof a舵 ientglass胤陀 providesa

clue to esti岡teprovenance

，

source material

，

and

manufacturi ng procedures. 1 n deter圃inationof their C叩positionsit is usually desirable

t

o

apply non -destructive analytical techniques because even the shape of artifacts sh凶Idbe preserved as excavated

for future studies. Reactor neutron-induced pro圃pt ganuna-ray anal拘is(PGA)

，

instru配ntal neutron

activation analysis (1 NAA)

，

and X-ray f luor，回田町e

analysis (XRF) are si刷 Ita町側S刷 Itiele聞ent

analytical岡ethodsproviding information on el明朗tal

co冊PQsition. Beside

，

both techniques are non

-destructive聞eth叫， which are appropriate for studies of such artifacts. In this work we have reported the ele舵ntal composition of ancient glassware (from the Yayoi period to the Edo period) excavated frOllthe ruins in japan to estimate provenance

，

sωrce material

，

and manufacturing procedures.

(2)

Neutron beam from JRR-3M at JAERI was employed for reactor neutron-induced PGA. Fluctuation in neutron flux were monitored by a neutron counter and duplicate PGA measurements of a titanium foil. Triga II reactor at Rikkyo University was used for conventional INNA. Some standard reference materials were employed as analytical standard for quantitative analysis purpose.

Concentrations of several elements (e.g., chlorine) determined by PGA were compared with the concentrations obtained by INAA. The analytical results obtained by either method were in good

agreement with each other if the analytical precisions were given in terms of counting statistics of the corresponding photo peak.

Elemental composition of the ancient glassware determined by PGA and INAA varied largely with the age of manufacturing and the location of the ruin,

indicating history and provenance of the source materials used for manufacturing of the glassware. Some elements were expected to be added on purpose to color the glassware of the basis of the determinations.

1. Introduction

Reactor neutron-induced prompt gamma-ray analysis (PGA), instrumental neutron activation analysis (INAA), and X-ray fluorescence analysis (XRF) are rapid non-destructive simulta neous multielement analytical methods on elemental composition of archaeological artifacts. These methods have been applied to determine the major and trace elements of glassware. 2. Experimental procedures

2.1 X-ray fluorescence analysis

A 100 HtCi Z 4 1A m source was employed to induce fluorescen

ce X-rays from the glass samples. The fluorescence X-rays were detected and analyzed by means of a Si(Li) X-ray detector coupled with a 2048 channel pulse hight analyzer. The typical measuring time was 3000 seconds.

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2.2 Neutron activation analysis

About 30 mg of samples were weighed into polyethlene seet sealed before irradiation. Capsules containing of such samples were irradiated in the Triga II reactor at the nuclear research institute of Rikkyo University for 3 minutes (thermal neutron flux : 1.5 x 10 1 2 n« cm ~2 • sec"1 ) and 18 hours

(thermal neutron flux : 1.5 x 10 l 2 n « c m ~2

•sec"')-The gamma-ray detection system used in this study consisted of 50 cm3 Iiturn drifted germanium detector coupled

to a 4096 channel pulse hight analyzer. After neutron irradiation the samples and standard were made three measure ments. The short lived radioactive species were measured for 5 minutes after a cooling period of 5 minutes to allow the

2 8A I activity to decay. The second counting of sample was

made after a cooling period of 1 week for 3000 seconds and 4 weeks later for 20000 seconds.

After the counting all peak areas w^re corrected for decay and counting losses and compared with those obtained from weighed samples and standards. All samples and standards were irradiated and measured in the similar manner.

2.3 Reactor neutron-induced prompt gamma-ray analysis Neutron beam from JRR-3M at JAERI was used for reactor neutron-induced PGA. Fluctuation in neutron flux were monitored by a neutron counter and duplicate PGA measurements of a titanium foil.

Samples were sealed into fluorinated ethylenepropylene resin film (FEP, 2 5 # m in thickness). The samples were set on the sample chamber from which the air was purged with the flow of He gas. The sample chamber was made of polytetra-fluoroethylene (PTFE, Teflon). The gamma-ray spectrometer consists of a high purity Ge detector, and BG0 ( bisumuth germanate,8uGe30i2) shielding detector coupled with a 8192 channel pulse hight analyzer".

In measurements we have used the following spectrometer system, which can measure simultaneously the prompt gamma-ray energy (0 - 12 MeV). A single mode, a Compton suppression mode, and a pair mode were performed. The thermal neutron flux was determined to be 2.4 x 10 7 n• cm ~2 • sec"1 and the cold

neutron flux was found to be 1.1 x 10 8 r>«cm ~2 - s e c "1) . The

-828-2

.

2

Neutron activation analysis Ab側t30剛gof sa圃pleswere weig恥d into polyethler昭総et sealed before irradiation. Capsules containing of such samples were irradiated in the Triga11 reactor at the nuclear research institute of Rikkyo University for3 mi~比四 (thermal neutron flux 1.5x 1012 n. c圃 -2. sec-I ) and18hou同 (thernl附utronflux 1.5x 1012 n

・

c剛ーしsec-I). The ga棚a-raydetection syste.used in this study consisted of 50 c棚aI i tu圃driftedger，同niulIdetector coupled to a 4侠渇channel凹lsehight analyzer. After neutron irradiation t加 samplesand standard~re .ade three.e3sure -ments. The short lived radioactive species were measur剖 for 5 minutes after a cooling period of 5削削除sto al low the 28AI activity to decay. The民自condcount i ng of sa即 lewas made after a cooling period of1 week for 3叩O鈴印刷sand 4 weeks later for2(削

o

seconds. After the count i ng a"問akareasWC!re corrected for decayand c側nting loss四 andco欄paredwith those obtained f rOlI we i ghed sa即l四 andstandards. AII sa聞pl四 andstandards 同reirradiated and嗣easu陀d in the si聞ilar聞ann巴r.

2 .

3

Reactor neutron-i nduced pr，冊ptg3llma-ray analysis N凹tronbe畑 fr帽 JRR-訓 atJAERI胤su田dfor reactor n閃tron-inducedPGA. fluctuation in聞 Jtronf lux were monitored by a r剛 tronc叫 nterand dupl icate PGA

闘

"

sure.ents of a titaniu. foil. Sa剛pleswere se剖ed into fluorinated ethylenepropylene resin fil. (fEP

，

25μm in thickness). The sallples were set on t加S3IIpI e Chall加rfrOllwhich t恥 airwas附rgedw i th the flow of He gas. The sa即lechailber was腕deof polytetra -fluoroethyle附 (PTfE

，

Teflon). The ga欄鴎・rayspectr柵eter consists of a high凹

r

i tyGedetec旬r

，

and Bω( bisu刷th germanate

，

Bi4GeaOI2) shielding detector coupled川tha 8192 chanr時l仰l艶 hightanalyzerl). In鯛easure柵ents間隔veused t加 followingspectro舵ter syste欄， which can llleasure si刷 lta問。uslythe prOllpt g繍鵬-ray energy (0・12門eV). A single聞叫e

，

a Co欄ptonsuppression 冊。de

，

and a pair111叫ewere perforll剖.The t恥r嗣Ineutron flux was deterll i ned to加2.4x 107 n. c剛-2• sec-I and t恥 cold 間utronflux was f叫ndto be1.1x 108 r

・

C闇句2

・

sec-t). The -828ー

(4)

samples were measured for about 3000 seconds for the cold neutron bean.

3. Results and discussions

Glass is one of the oldest nan-made materials and the most important artifacts in the world. The prehistoric period of Japan is divided into the Jomon period (before ca.300 B.C.) and the Vayoi period (ca. 300 B.C.-ca. 300 A.D.).

No glass has been found in the Jomon period. In the Yayoi period, glassware has been found in several sites. In Kofun period (Tumulus period, from ca. third century A.D. to the seventh century), glass beads have been excavated in several tombs. In that period, most of the glass beads were made of mixed-alkali glass.

Glass are obtained by the fusion of silica and some metal oxides. They are mixtures of the following components: silica (Si02), alumina ( A l203) , lime (CaO), magnesia (Mg20),

soda (Na20), potash (K20),manganese oxide (MnO), ferric oxide

( F ea03) , tin oxide (Ti02), and lead oxide (Pb20). The propor

tions of soda and potash (alkalin oxide) vary widely. Table 1 lists some of the most common metal ions used by ancient glass makers to color glass. The color of glass is determined by the presence of various metallic oxides, usually in small amounts. Iron is the almost universal coloring agent of ancient glasses. Iron is usually present in glass as a mixture of ferrous ions (Fe2*), which color the glass blue. And ferr

ic ions (Fe3*) gives it yellow. Many ancient glasses were

colored by the presence of oxidized cobalt and copper; cobalt ions (Co2*) give glass dark blue color and cupric ions (Cu2*)

bright blue

color-About two thousand samples of ancient Japanese glass were analyzed X-ray fluorescence analysis2'. The results revealed

the existence of four compositional groups as shown in Table 2. The lead-barium glass beads are known to have been made in ancient China (Pre-Han and Han dynasty (202 B.C. -220 A.D.))

3 - 4 1. In Figure 1 a typical X-ray fluorescence spectrum of

lead-alkali glass bead is shown: the Cu X-ray K a line, Ba K a lines,Sn K a line, Fe K a line, Hn K a line,and Pb L lines can be seen.

Neutron activation analysis was applied to the glass beads

sup 1 es were_四suredfor about 3似JOseconds for t加 cold neutron陸棚 . 3.町田ultsand dis凶ssio附 Glass is 0陪 ofthe oldest Man-闘denterials and the 鵬sti剛portantartifacts in the world. The prehistoric period of Japan is divided into the Jo網開問riod(before ca.300 B.C.) and the Vayoi period (ca. 3

∞

B.C.・四.初

o

A.D.). No glass h師陣enf凶ndin the J欄onperiod.1 n t加 Vayoi peri凶， glassware has加enf凶 ndin several sites. In Kofun 閃ri叫 (Tu刷 lusperiod

，

fro欄ca. third century A.D. to the seventh cen1ury)

，

glass beads have been excavated in several to耐s. In that陀ri叫， .ost of the glass beads were made of 聞ixed-al陥liglass. Glass are obtained by t恥 fusionof silica and so

.

e

附

tal oxides. They are剛ix1uresof the following c欄ponents: silica (Si02)， alu聞ina(AI203)， 1 i

.

e

(臼0)，闘sr悶 ia(問g20)， soda (Na20)， potash (K20)，JRanga即seoxide 側副)， ferric oxide (Fe203)

，

tin oxide (Ti02)

，

and lead oxide (Pb20). The prqpor -tions of:;叫aand potash (al陥linoxide) vary widely. Table 1 1 ists so欄eof t加開時t0側鵬n圃etal io隔 U舵dby ancient glass .akers 10 color glass. T加 colorof glass is determined by the pr田町問。fvarious附句11ic oxides

，

usually i n湖all a聞ωnts. Iron is the al冊。stuniversal coloring agent of ancient glass四 .Iron is u釦allypresent in glass as a聞ixture of ferrous io悶 (Fe2+)

，

which color t加 glassblue. And ferr ic ions (Fe3

つ

givesi t yellow. Hanyancient glasses田re colored by the prese舵eof oxid ized cobal t and co仰er;cobalt ions (C02

つ

giveglass dark blue color a咽 cupricions (Cu2

つ

bright blue color. About t同 t加usandsa聞plesof a舵 ientJapanese glass同re analyzed X-ray fluor回田町eanalysis21 • The re;剤lt渇 revealed the ex i stence of f叫rc帽P回itionalgr，側psas shown in Table 2. The lead-bariu剛glassbeads are known to have民間間.dein ar陀ientChina (P問・Hanand Han dynasty (却2B.C. -220 A.D.)) ト山 . In Figure1 a typical X-ray fluoresoe舵es陀ctru聞of lead-alkali glass bead is shown: t加印 X-rayKαline

，

Ba Kα

li問s，SnKαli附， Fe Kαline， Hn Kαli問，andPbL 1 i問scan

be seen.

(5)

of the Edo period. Results of the analysis of the major and trace components are presented in Table 3. Glass beads are of lead glass type, except for the blue bead, which is of soda-Iime type.

A typical prompt gamma-ray spectrum of glass beads (potash-Iime glass bead, the Edo period, excavated at the Kaneiji Temple in Tokyo ) is shown in Figure 2- Elements such as boron, sodium, potasium, chlorine, and silicon can be measured in high sensitivity at the thermal neutron beam. The content of boron indicates of the difference in raw materials for manufacturing glass. Boron content was in the 20 - 80 ppm range.

A plot of K20 (Wtt) vs Na20 (WtX) indicates that there

may indeed be three compositional type. The groups can be characterized according to the concentration of three oxides: lead (PbO), sodium (Na20) and potassium ( K20 ) . Variation in

the concentrations of soda and potash are probably due to the compositional variation of the raw materials used in

manufacture. 4. Conclusions

PGA, INAA and XRF can be successfully applied to ancient glass beads because of their ability of rapid non-destructive simultaneous multielement analyses. The methods have been found to be applicable to archaeological samples in general. Because of these advantages it may be applicable to other precious objects of cultural property. The analysis of samples provides a clue to estimate provenance, raw materals, and manufacturing procedures. Based on the contents of boron, sodium, potasium, chlorine, silicon, barium, and lead, ancient Japanese glass beads colud be characterized.

REFERENCES

1) C.YONEZAUA, A.K.HAJI WOOD, M.HOSHI, V.ITO and E.TACHIKAWA (1993) (in press).

2) T.TOMIZAWA, T.TOHINAGA and Y.KOIZUMI (1993) "Azumazaka Kofun"; ed. by the school board of Atsugi city in Kanagawa prefecture, pp.105-117.

3) H.C.BECK and C.G.SELIGMAN (1934) Nature, 133, 982. 4) C.G.SELIGMAN, P.D.RITCHIE and H.C.BECK0936) Nature,

138, 721.

-830-of the Edo period. Results of the analysis of the major and

trace co冊ponentsare presented in Table 3. Glass beads are

of lead glass type

，

except for the blue bead

，

which is of soda-I i聞etype. A typical pr棚 ptga酬a-rayspectru冊。fglass beads (potash -lime glass bead

，

the Edo period

，

excavat剖 att加 Kaneiji Te冊plein Tokyo ) is shown in~igure 2. Ele欄entssuch as boron

，

sodiu

，

聞

potasiu

，

闘

chlori

閑

，

and silicon can be Measured in high sensitivity at the ther.al聞 Jtronbea聞. The content of boron indicates of the difference in raw materials for m附facturingglass. Boron content w路 inthe 20・80ppm range. A plot of K20 (Wt%) vs Na20 (Wt%) indicates that there may i ndeed be three cornpos i t i ona I type. The groups can be characterized accordingωt恥 concentrationof three oxides: lead (附0)

，

s叫ium(Na20) and potassium (K20). Variation in

the concentrations of soda and potash are probably due 旬 the

co冊positional variation of the raw Materials used in 圃a附fac加re. 4. Cor陀lusior隠 PGA

，

INAA andXR~ can加 successfullyapplied to ancient glass加ads民団useof t加irability of rapid non-destructive simultane側 S刷 1tielement analyses. The meth叫shave been f倒Jndto be applicable to archa凹 logical sa四plesin駅前ral. Because of these advantages it聞aybe applicable to other precious objects of cultural property. Tt陪 analysisof sa冊ples provides a clue to estimate provena舵:e

，

raw lllateral s

，

and manufacturing pr舵edures. 8ased on t加 contentsof加ron

，

sodiu

，

剛

potasiu

，

聞

chlorine

，

silicon

，

bariu

，

圃

and lead

，

ancient Japanese glass beads colud be characteriz'剖 . RE~ERENC回 1) C. YONEZAWA

，

A.K.HAJ 1 W

∞

D

，

肌

H05HI

，

Y.ITO and E.TACHIKAWA (1993) (in pr目的. 2) 1.'1'倒1 IZAWA

，

T.TOf1INAGA and Y.KOIZlX11 (1993) "A剖lIazaka Kofun"; ed. by the sc加01加ardof At剖gi city in Kanagawa prefecture

，

pp.l05-117. 3) H.C.BECK and C.G.SELIGMAN (1934) Na加re

，

133

，

982.

。

C.G.SELI側AN

，

P.D.RITCHIE and H.C.BECK(1936) Nature

，

旦~， 721. -830ー

(6)

Table 1 Glass-coloring ions

Color of glass Mettal ions

Blue Cupric(Cu2*) CobalKCo2*) Green Cupric(Cu2*) Ferrous(Fe2 +) Amber Ferric(Fe3*) Ye I low UraniumW*) Cadniun(Cd2+) Red Cuprous(Cu2 t) Violet Manganous(Mn2+)

Table 2 Chemical composition of Japanese glass beads

Period Cobalt blue Blue Grrcen Yellow Brown V h i l e

Vayoi period

(B.C.3C~-3C>

Soda-potash-line glass B a l i i n M e a d glass

Soda-potash-1 iHe glass Soda-|>oLash-l imp. *lass Lead glass

Sal i n - load glass

l.e*d glass

Kofun period ( 4 0 - 7 C )

S o d a - p o U s h - l i K glass l e a d - a l k a l i glass

Soda-potash-live glass Soda-potash-lime glass

Lead glass

Baliiw-lead glass

Lead glass

Hetan period Lead glass Lead glass Lead glass Lead glass Lead glass

Edo period ( 1 6 0 3 - 1 8 7 6 )

Lead glass Soda-potash-li*e glass Lead glass Lead glass Lead glass Lead glass Table 1 Glass-coloring ions Color of glass Mettal ions Blue Cupric(Cu2_・_〉 Cobal t(C02

つ

Green Cupric(Cu2₊₎ F 'errous(F'e2₊₎ Amber F'erric(F'e3φ〉 Vellow Uraniu冊(U4+) Cadniu聞(Cd2+) Red Cuprous(Cu2₊₎ Violet 臨時an側s(Mn2+) Table 2 Chemical composition of Japanese glass加ads p.，，，吋 (0回日.，.. 81ue Grr.en Yell<柑 8，剛" ¥lhlt.e VaYOI問 " 岬 Soda-凹U胡-lillleslass SOOo-同t.a...h-II・("tlass S剖Ja"，IOLash-11闘，1.田 1.目dnla田 (8.C.3(-3C) 8.1...・leadslass l.ead Xlas宮 8aliu.-1四d1¥1.田 Kofun問riod S叫.-凹".h・lille，Iass S咽0-田tash-Ij~ &Ia'田島由・凹l&sh-lillezla由 u割引ass (4C-1I:) 担割-alkali &1&由 U叫.，.田 8.li岨・1四dtlass

tfeian問円吋 Lead &1.田 I.ead 31as宮 Lead .r:lass I.ead .1世諸 I.ead &Ia田〈百・-1191)

回operi剖国"_d8₁_&_S_S SOOo-同U曲・1;・esla田 lead，Ia開

lc副，10田

L

一a一一d一g一'一日s I Lead &Ia田

I

〈描田問16)

(7)

AKA7-380. SPC 89/09'l4 TIME= 4000 SEC GREEN

m

Pb

0 1 0 2 0

ENERGKkeV)

Figure 1 X-ray fluorescence spectrum

2000 4000 6000

Channel Number

SOOO

Figure 2 Prompt gamma-ray spectrum

— 832 — TI恒 4邸犯 SEC 僚任N 向KA7-初日.S陀 89..-00/14

L u

n r

P

b

S

n

=

ー

- 岳ー-~

=

~凶ヨ

ー

=

-30

20 、

.

，

a ' ' u " u p h H b

ι

巴_R ，，， . ‘ ‘ ‘ HUE-n z H M W R u a n n h v u M m H n h r u

1

0

。

X-ray fluorescen明 Spectrull Figure 1 ー

-

l

自000

﹁

!

'

∞

一閃 -F 自 L ' h u m u N -D l

﹁

∞

- e -4 m 一同 ↑ c r

∞

- n u 同町 ζ ω μ c コ o u Pro側ptgaII鵬・rayspectru聞 -832ー Figu陀 2

(8)

Tabic 3 Analyses of Japanese glass beads

Edo pcriod(1603~187G),Beads

Colour White Brown Green Blue Blue

Type Lead glass Lead glass Lead glass Lead glass Polash-Lime

Wei gilt GO.O(mg) 35.4(mg) 37.2(mg) 50.0(ms) 43.9(mg)

A l203« ) Na20 K20 CaO Ti02 NgO MnO Fe203 1.03 0.1G 5.9 n.d. n.d. n.d. n.d. 0.13 0.84 0.14 G.3 n.d. n.d. n.d. 0.005 3.78 0.89 0.15 8.0 n.d. n.d. n.d. 0.001 0.19 1.51 0.27 8.8 n.d. n.d. 0.29 0-523 0.24 2.71 3.1 13.4 9.2 0.14 n.d. 0.005 0.24 Sc(i)pm) V Cr Co Cu As Ag Rb SI) Ba La Ce Sm Eu Tb Yb Lu llf 1.3 n.d. n.d. 9.1 190 n.d. 89 35 500 n.d. 0.14 n.d. n.d. n.d. n.d. n.d. n.d. n.d. 2.9 n.d. n.d. 0.10 430 n.d. 210 47 140 n.d. 0.72 n.d. 0.07 n.d. n.d. 0.45 n.d. n.d. 2.7 n.d. n.d. 1.2 9500 n.d. 19 43 220 n.d. 0.24 n.d. n.d. n.d. n.d. n.d. n.d. n.d. 1.5 10 51 390 C30 n.d. 150 120 3200 n.d. 1.3 82 0.13 n.d. n.d. 0.87 0.38 0.87 O.GO 7.8 n.d. 3.9 0500 17 3.3 n . d . 15 n . d . 7.0 19 0.96 0.25 0.11 n.d. n.d. 0.87 TalJlc 3 Analyscs ofJapan~e glass beads Edo[lcriod(l603-187G)，scads Coloul \~hi te sI"OIII1 Grccn sluc sluc Typc Lcad glass .lcad glass L巴adglass Lcad glass 1'0Lash-Lirn巴 ¥ .leighL 60.0(lI1g) 35.11(1111:) 37.2(1111;) 50.0(lI1g) ~3.9(1I11:) A 1203(%) 1.03 0.81' 0.89 1.51 2.71 Na20 0.1G 0.11' 0.15 0.27 3.1 K20 5.9 G.3 8.0 8.8 13.~ CaO n.d. n.d. l1.d. n.d. 9.2 Ti02 n.d. n・d. n.d. n.d. 0.11' NgO n.d. n.d. n.d. 0.29 n.d. トlnO l1.d. ().005 0.001 0.523 0.()05 fC203 0.13 3.78 0.19 0.24 0.211 Sc(mlsl) 1.:l 2.a 2. -( 1.5 0.60 n.(/. n.d. n.d. 10 7.8 Cr n.d. n.d. Il.d. 51 n.【1. Co 9.1 0.10 1.2 390 3.9 Cu 190 ~30 9500 630 6500 As n.o. n.d. n.d. n.d. 17 Ag 89 21() 19 150 3.3 Rb 35 1'7 ~3 120 Il.d. Sb 500 11'0 220 3200 15 sa l1.d. n.cl. n.d. l1.d. l1.d. La 0.111 0.72 0.21' 1.3 7.0 Cc n.d. n.d. n.d. 82 19 Sm n.d. 0.07 n.d. 0.13 0.96 Eu n.d. n.d. n.d. n.d. 0.25 Tb n.d. n.d. n.d. n.d. 0.11 Yb n.d_ 0-'15 n.d. 0.87 n.d. Lu n.cI. n.d. n.d. 0.38 n.d. IIf n.d. n.d. n.d. 0.87 0.87