winer—logi™—l w—g—zineD eugust PHHSD †olF TW@RAD ppF RHQ±RPQ

„he ™hemistry of —ll—nite from

the h—i˜os—tsu €—ssD ‰—m—n—shiD t—p—n

ID I P I I I

wF ryƒrsxy BD wF uswe„e DxFxsƒrshe DeFu‰yxy DwFƒrsws exh ƒF „euse‡e

I

ho™tor—l €rogr—m in i—rth ivolution ƒ™ien™esD qr—du—te ƒ™hool of vife —nd invironment—l ƒ™ien™esD „he

niversity of „suku˜—D s˜—r—kiD QHSEVSUPD t—p—n

P

ghemi™—l en—lysis hivisionD ‚ese—r™h p—™ility gentre for ƒ™ien™e —nd „e™hnologyD „he niversity of „suku˜—D

s˜—r—kiD QHSEVSUUD t—p—n

efƒ„‚eg„

„he ™ryst—l stru™ture of —ll—nite from gr—niti™ pegm—titeD the h—i˜os—tsu €—ssD ‰—m—n—shiD t—p—nD h—s

˜een refined under the ™onstr—int of ™hemi™—l ™omposition determined ˜y ele™tron mi™ropro˜e —n—lysis

of r—re e—rth elementsF f—™kEs™—tteredEele™tron im—ges —nd ˆEr—y element m—ps of the —ll—nites show

th—t e—™h of their ™ryst—l gr—ins h—s ™hemi™—lly homogeneous distri˜ution of m—jor elementsF e typi™—l

formul— for the ™hemistry isX @g— 8 A @v— ge €r xd ƒm „h wn

HFWPH HFHVH ƒIFHHH HFPQV HFRRQ HFHRV HFIHH HFHIW HFHRP HFHHV

QC PC QC

8 A @el pe „i A @el A@pe pe wn wg A @ƒiy A@ƒi y Ay@yrAF HFIHP ƒIFHHH HFTHU HFHUT ƒIFHHH IFHHH HFHSS HFHQU ƒIFHHH R P U HFQIU HFSRQ HFQTS

Ê „he ™ryst—l stru™ture of —ll—niteD mono™lini™D — VFWHS @IAD ˜ SFUTHT @SAD ™ IHFIPQ @IA eD ˜ IIRFUVë@IAD

sp—™e group €P GmD  a PD h—s ˜een refined to —n unweighted ‚ f—™tor of QFRT7 for IRSW o˜served I

refle™tionsF elthough the r —tom position w—s not determined on the hifferen™eEpourier m—pD inspe™tion

of the ˜ond v—len™e sums demonstr—tes th—t the r —tom is uniquely lo™—ted —t the yIH —tom —nd involved

in — hydrogen ˜ond to yRF e system—ti™ ex—min—tion —s to ™ryst—l ™hemistry of —ll—nites suggests th—t the

isol—ted ƒiy tetr—hedron h—s the l—rgest distortion of three kinds of the tetr—hedron ™ont—ining ƒi y R P U

groups in the —ll—nite stru™tureF „his o˜serv—tion is ™ommon to the epidote group miner—lsD while the

l—rger distortion of eP sites ™—used ˜y o™™up—n™y ˜y ‚ii in —ll—nites ™ontr—sts with the sm—ller one of e

sites in other epidote group miner—lsF sn the —ll—nite groups the ˜ond —ngles ˜etween the yIHÿr ˜ond

—nd hydrogen ˜ond r•yR —re found to r—nge from IUH to IVHëF

gompil—tion of the ™hemi™—l ™ompositions of the title —ll—nite —nd the others from gr—niti™ ro™ksD t—p—nD

RC QC

whi™h reve—ls „hEin™orpor—tion —s the ™oupled su˜stitution of Q„h C 8 @v—™—n™yA b R‚ii D provides

—n expl—n—tion for the o˜serv—tion th—t higher „h ™on™entr—tions ™h—r—™terize —ll—nites from the isl—nd

—r™sF „he tern—ry el y Epe y Eƒ‚ii di—gr—m illustr—tes th—t —ll—nites —re groupedD —™™ording to their P Q P Q

originsD into three ™l—sses suggestive of te™toni™ ˜—™kgrounds for the ™ryst—lliz—tion lo™—litiesY

@IA intr—™ontinent—lD @PA isl—nd —r™ —nd @QA ™ontinent—l m—rginF

ui‰‡y‚hƒX —ll—niteD t—p—nD ™hemistryD te™toni™ settingD ™ryst—l stru™tureD iw€eF

—nd is found in gl—u™oph—ne s™hist @f—nnoD IWWQA sntrodu™tion

—nd g—rnet lherzolite —s well @‰—ng —nd in—miD vvexs„iD —n epidote group miner—l e

PHHQAF „here —re —lso —ll—nite pheno™rysts in —™id ‘e w ƒi y @yrAX e a g—D geY w a elD pe“D is P Q Q IP

vol™—ni™ ro™ks @eFgF w—hood —nd rildrethD IWVQY known —s — ™h—r—™teristi™ —™™essory miner—l in

ghesner —nd ittlingerD IWVWAF „he ™l—ssi®™—tion of gr—niteD gr—nodioriteD monzoniteD syeniteD sk—rns

ir™it @PHHPA permits —ll—nites to ˜e groupedD —nd gr—nite pegm—tite @eFgF heer et —lFD IWVTY

—™™ording to their m—jor ‚ii ™ontentsD into q—ines et —lFD IWWUY qiere —nd ƒorensenD PHHRAD

—ll—niteE@geAD —ll—niteE@v—A —nd —ll—niteE@‰AF wost

—ll—nites preferenti—lly in™orpor—te the r—dio—™tive

elements „h —nd D —s minor elements @heer et B iEm—ilX hossyUITd—rsi—FgeoFtsuku˜—F—™Fjp

—lFD IWVTAD —nd so —ll—nite often o™™urs in the hysX IHFIIVHGHHPTRTIHSTWRHPSW

5 PHHS „he winer—logi™—l ƒo™iety

wF ryƒrsxy i„ evF

x—g—shim—D IWTHAD ex™ept for gr—niti™ —ll—nite met—mi™t st—teF rowever — report ˜y roltst—m et

@ƒuzuki et —lFD IWWHA —nd met—morphi™ —ll—nite —lF @PHHQA ™on™luded th—t nonEmet—mi™t —nd

@ƒ—k—i et —lFD IWVRY f—nnoD IWWQAD were reported un—ltered ferri—ll—niteE@geA from the f—st—Ès

PC QC

˜efore initi—l use of iw€eF ƒever—l —uthors peEguE‚ii deposit in ƒwedenD geg—pe elpe

@€udovkin— —nd €y—tenkoD IWTSY holl—seD IWUIA @ƒiy A@ƒi y Ay@yrAD ™ont—ins neither „h nor F R P U

h—ve ™—rried out stru™tur—l determin—tions of nonE fe™—use of the very ™lose sp—™ing of the ˆEr—y

met—mi™t —ll—nites sin™e the ®rst re®nement of the lines in the v spe™tr— of the ‚iisD —™™ur—te

™ryst—l stru™ture of —ll—nite ˜y ed— @IWSSAF ele™tron mi™ropro˜e —n—lysis @iw€eA of ‚iiE

roweverD ˜e™—use of the l—™k of —™™ur—te iw€e ˜e—ring miner—ls is experiment—lly ™h—llenging

of ‚ii @‚eed —nd fu™kleyD IWWVY xishid— et —lFD @‚eed —nd fu™kleyD IWWVY xishid— et —lFD IWWWAF

IWWWAD stru™tur—l re®nements of —ll—nites h—ve not „he modi®ed methods devised through ™—reful

˜een —ttempted under the ®xed ™onstr—int of their me—surement of these ˆEr—y lines h—ve improved

™hemi™—l ™ompositionsF the qu—lity of the ‚ii d—t— ™olle™ted ˜y iw€e

„he —ims of this study —re @IA to determine @‚eed —nd fu™kleyD IWWVY xishid— et —lFD IWWWAD

—™™ur—te ™hemi™—l ™ompositionsD resolved ˜y where —™™eler—ting volt—ge of PS k† is —pproE

iw€eD of —ll—nites from gr—niti™ ro™ksD pri—te for qu—ntit—tive —n—lysis of ‚iiF €reviously

t—p—nese isl—nd —r™D @PA to de®ne ™ryst—l ™hemE pu˜lished ™ompositions of —ll—nites from t—p—n

istry ™h—r—™teristi™s of —ll—nitesD —nd @QA to provide @eFgF r—seg—w—D IWSUY x—g—shim— —nd

psqF IF y™™urren™es of —ll—nite in t—p—nF RHR

griwsƒ„‚‰ yp evvexs„i

geo™hemi™—l ˜—™kgrounds of te™toni™s on o™™urE

ren™es of —ll—nitesF

ixperiment—l methods

y™™urren™e —nd ™ryst—l inform—tion

„he h—i˜os—tsu €—ssD in northe—st ‰—m—n—shi

€refe™tureD t—p—nD ™omprises „erti—ry peliti™

hornfels @x—g—shim— —nd x—g—shim—D IWTHA

@pigF IAF ell—nite o™™urs —s — ™o—rseEgr—ined

˜l—™k prism—ti™ ™ryst—l in the gr—niti™ pegm—tite

intruding into those ro™ks together with qu—rtz

—nd — few pl—gio™l—ses @pigF PAF xe—r˜y dykes

™ont—in s™heeliteD epidote —nd ilmenite

@x—g—shim— —nd x—g—shim—D IWTHAF ƒome —ll—E

nites ™ompletely en™losed ˜y qu—rtzD presum—˜ly

less perme—˜le to ¯uidD tend to ˜e in — nonE—ltered

—nd nonEmet—mi™t st—teD ˜ut this gr—niti™ pegm—E psqF PF €hotogr—ph of the un—ltered —nd nonEmet—mi™t

tite is r—dio—™tiveD —s determined ˜y — qeigerE —ll—nite ™ryst—l in™luded in qu—rtz in gr—niti™ pegm—tite

wuller ™ounterF È from the h—i˜os—tsu €—ssF elX —ll—niteY zX qu—rtzY

„he —ll—nite ™ryst—ls r—nge in size from €lX pl—gio™l—seF

IHTIHTPS mm to PTPTSmmFpigureQ

shows the morphology of —ll—nites from the

™urrentF „he methods for sele™tion of the ‚ii h—i˜os—tsu €—ss —nd the intr—™ontinent—l region

pe—k position re™ommended ˜y xishid— et —lF @heer et —lFD IWVTAF „he intr—™ontinent—l morpholE

@IWWWA were —pplied to the present —n—lysisX the u ogies of —ll—nites @with some un™ert—inty in the

series of ˆEr—y spe™tr— w—s used for m—jor miner—l identi®™—tionA show t—˜ul—r h—˜it @rintzeD

elementsY the w series for „hY —nd the v series IVWUY h—n—D IWIIY qolds™hmidtD IWPHY „roÈgerD

for ‚iiF we—surements of the v— lines for ‰D v—D IWUIY heer et —lFD IWVTAD where—s —ll—nites from

ge —nd xd —nd the v˜ lines for €rD ƒmD qd —nd the h—i˜os—tsu €—ss —re regul—rly prism—ti™ —nd

hyD required no pe—kEoverl—p ™orre™tionsF „he euhedr—lF

present method for iw€e of ‚iiD ex™ept for xdD

h—s ˜een developed from th—t —dopted ˜y ‡ing et ghemi™—l ™omposition

—lF @PHHQAF

ilements dete™ted with qu—lit—tive —n—lyses ell—nites were —n—lysed for m—jor —nd minor

were me—sured ˜y qu—ntit—tive —n—lysesF ell—nite elements using the iw€e @tˆeEVTPIY tiyvA

gr—ins were —n—lysed qu—ntit—tively for m—jor equipped with three w—velengthEdispersive spe™E

elements @ƒiD „iD elD peD nD wnD wgD g—D „hA —t — trometersF u—lit—tive —n—lyses were m—de using

volt—ge of PS k†D ˜e—m ™urrent of IH neD —nd PS k† —™™eler—ting potenti—l —nd PSH ne ˜e—m

psqF QF worphology of —ll—nites from @—A isl—nd —r™ —nd @˜A intr—™ontinent—l settingsF RHS

wF ryƒrsxy i„ evF

„efvi IF ƒt—nd—rd m—teri—ls used for w—velength dispersive ele™tron

mi™ropro˜e —n—lysisF

ƒt—nd—rd ghemi™—l ™omposition

element @wtF7A

ƒi ƒiy @IHHFHA P

„i „iy @IHHFHA P

„h „hy @IHHFHA P

el el y @IHHFHA P Q

pe pe y @IHHFHA P Q

n ƒiy @QQFIIAD ny @TTFVWA P

wn wny @QHFUTAD pe y @TWFPRA P Q

wg wgy @IHHFHA

g— ƒiy @SIFUQAD g—y @RVFPUA P

‰ ƒiy @SRFQAD el y @IPFUAD g—y @PHFSAD ‰ y @IIFVA P P Q P Q

v— ƒiy @SRFQAD el y @IPFUAD g—y @PHFTAD v— y @IIFSA P P Q P Q

ge ƒiy @SRFPAD el y @IPFVAD g—y @PHFRAD ge y @IIFWA P P Q P Q

€r ƒiy @SRFHAD el y @IPFUAD g—y @PHFTAD €r y @IPFPA P P Q P Q

xd ƒiy @SRFRAD el y @IPFVAD g—y @PHFVAD xd y @IIFVA P P Q P Q

ƒm ƒiy @SRFVAD el y @IPFWAD g—y @PHFVAD ƒm y @IIFPA P P Q P Q

qd ƒiy @SRFVAD el y @IPFIAD g—y @PHFUAD qd y @IPFIA P P Q P Q

hy ƒiy @SRFUAD el y @IPFSAD g—y @PHFTAD hy y @IPFHA P P Q P Q

ground in —n —g—te pestle until their powders were ™ount times of PH sF gon™entr—tions of ‚ii were

judged to ˜e of — suf®™iently sm—ll gr—in size to me—sured —t PS k† with — SH ne ˜e—m ™urrentD

—nd ™ount times of PH sF foth ˜e—m ™urrents were

™orre™ted with the followingX

„efvi PF het—ils of d—t— ™olle™tion —nd re®nement of

—ll—nite from the h—i˜os—tsu €—ssF sntensity @spe™imenA

u ˆ 

sntensity @st—nd—rdA

fe—m ™urrent @st—nd—rdA

hiffr—™tometer inr—fExonius gehR 

fe—m ™urrent @spe™imenA

Ê

‡—velength woEu— r—di—tion @l a HFUIHTW eA

™omposition @st—nd—rdA

„emper—ture PWT u

gryst—l size HFITHFITHFI mm

„here were two types of me—surement for the

ƒ™—n mode oGPy

present —n—lyses ˜e™—use the —n—lyti™—l error

Ê — VFWHS@IA e

would ˜e gre—t if —ll elements were —n—lysed —t

Ê ˜ SFUTHT@SA e

the s—me ˜e—m ™urrent @ ™hiy—m— et —lFD IWUPAY — Ê ™ IHFIPQ@IA e

list of the st—nd—rds used in this study is presented ˜ IIRFUV@IAë

Q

Ê in „—˜le IY —nd —ll d—t— were ™orre™ted with — † RUHFU@PA e

ƒp—™e group €P Gm –ep9 m—trixE™orre™tion progr—mF I

 P

Py UH

m—x

ˆEr—y powder diffr—™tion „ot—l refle™tions SSSU

nique refle™tions IRWV

„he degrees of met—mi™tiz—tion for —ll—nites were

‚ v—lue HFHI int

ex—mined ˜y ˆEr—y powder diffr—™tion @€ˆ‚hA

nique p b IRSW

H

—n—lysisF ƒ—mples were ˆEr—yed with guEu—

I Rs@p A H

r—di—tion @RH k†D QH meA using — ‚ig—ku p@HHHA SRWFS

qeiger¯ex system with — ¯—t gr—phite monoE ‚ v—lue QFRT7

™hrom—tor —nd Ië divergen™e slitF ‡hole p—tterns ‚w v—lue IHFRW7

qoodness of fit IFPV

from S to TSëPy were s™—nned —t HFIëPy steps —nd

ÿI

m UFVU mm the re¯e™tions in the PRFSÿPTFH —nd QHFHÿQIFSëPy

r—nges —t HFHIëPy stepsF „he —ll—nite s—mples were RHT griwsƒ„‚‰ yp evvexs„i IFHHH ƒ A IP

H H H H HFHHH@IA HFHHR@IA HFHHI@IA H H H H H H H H H IFHHH ÿ ÿ ÿ ÿ ÿ ÿ ÿ ÿ ÿ ÿ ÿ ÿ ÿ ÿ ÿ ÿ ID @el w IQ for

IFHHH ƒ A HFHUT „i PQ

QC HFQIU HHHHFHHI@IAHFHHI@IA HFHHTU@VA HFHHI@IA HFHIH@IA HFHHUT@VA H HFHHW@IA HFHHTT@UA H HFHHT@IA HHH HFHHW@PA H HFHHV@PA H HFHII@PA HFHHU@PA HFHIR@PA HFHIH@PA HFHIH@PA H HFHHTW@SA HFHHHU@VA HFHHVQ@VA HFHHHW@VA HFHHHP@TA HFHHWR@TA HFHHHQ@TA HH HFHIPV@UA HFHHUS@PA pe AF ÿ ÿ ÿ ÿ ÿ ÿ ÿ ÿ ÿ ÿ ÿ ÿ ÿ ÿ ÿ ÿ ÿ ÿ P Ê HFTHU PD @el QQ e

for IFHHH ƒ A PP HFIHP

8 HFHHV wn HFHRP II

„h HFHIW ƒm HFIHH eq xd HFHRV €r QF HFRRQ w ge QF etomi™ ™oordin—tes —nd equiv—lent displ—™ement p—r—meters @e for HFPQV efvi IFHHH ƒ „ A ID @v— e HFHQU for wg yz IFHHH HFHSS ƒ A wn HFHVH QC HFQTS 8 pe HFWP x PC HFSRQ P —nd @pe w Q HFQHQH@IA HFPS HFPIQS@IA HFHPRS@QA HFHPII@TA HFHPQU@TA HFHPSU@TA P H H HFS HFHPHT@SA HFHIVR@WA HFHIW@IA HFHPR@IA I H H H HFHPRT@RA HFHPQI@VA HFHPQV@WA HFHPTH@VA

IP HFUSVS@PA HFSWQUS@TA HFUS HFUS HFISIS@PA HFRPWPR@SA HFHPIW@RA HFHPQQ@QA HFHPUP@WA HFHPIS@QA HFHIWH@VA HFHPSR@QA HFHPPI@VA HFHPIT@QA

ƒiIƒiPƒiQyI HFQQVT@PAyP HFTVTT@PAyQ HFIVVT@PA HFUSyR HFPQQH@SA HFPSyS HFQIQS@SA HFUSyT HFUWTT@SA HFWVUU@VAyU HFHSTS@VA HFHQSW@PA HFWUIV@VAyV HFHRWT@VA HFPUWV@PA HFHPRS@SA HFHIRU@UAyW HFHTUS@VA HFQPRS@PA HFQTSQ@SA HFPS HFHPIR@RAyIH HFSHWS@VA HFQQVI@RA HFUS HFHPIT@RA HFHPTV@VA HFSRIQ@VA HFUS HFHPIH@RA HFHPH@IA HFHPRQ@UA HFTHVR@VAƒite HFUS ™ontentsX HFHPH@IA HFHPTR@VA HFHVSI@UA HFHPQ@IA @g— HFIPWP@UA HFPS HFHIVW@WA HFHPQ@IA HFHPI@IA HFISIV@TA HFPS HFHPR@IA HFPS HFHPI@IA HFRIIV@TA HFHPI@IA HFHPS@IA HFHPI@IA HFIUVV@UA HFHPR@IA HFHPS@IA HFHPP@IA HFQQSS@UA HFHPI@IA HFHPR@IA HFHPQ@IA HFHQS@PA HFHPP@PA HFHPI HFIHIS@TA HFHPV@IA @IA HFRPVH@TA HFHPS@IA HFHPT@PA HFHQQ@IA HFHPW@PA HFHPS@PA HFHPV@IA HFHPT@PA HFHPR@IA HFHPT@PA HFHPU@PA HFHPT@PA HFHPI@PA HFHQH@PA HFHPT@PA HFHPR@PA HFHPS@PA HFHIW@PA HFHRV@RA HFHPT@PA HFHQV@QA HFHPP@IA HFHPW@QA HFHPU@QA HFHIT@PA HFHPS@QA w w etom e for e w RHU

wF ryƒrsxy i„ evF

Ê

„efvi RF fond lengths @eA —nd —ngles @ëAF

—˜ j

eIÿyQTP PFQQW@RA wIÿyRTP IFVTU@RA

kl

yU PFQRU@RA yITP IFWVS@RA

™d kl

yITP PFQTI@SA ySTP PFHIS@RA

e

yS PFSWI@UA we—n IFWST

e

yT PFWHS@UA

—

yWTP QFIPT@QA

we—n PFTII

mn

wPÿyQTP IFVTU@RA

H

yIHTP IFWHW@QA

kp

yTTP IFWIW@RA

ePÿyU PFQPQ@UA we—n IFVWV

fg

yPTP PFRUU@RA

h

yIH PFTHV@TA

i

yPTP PFTQI@RA

yQTP PFUWW@RA wQÿyV IFWSU@UA

yVTP QFHHU@PA yR IFWWR@TA

ik

we—n PFTUT yPTP PFIWS@RA

ik

yITP PFQHW@SA

we—n PFITH

ƒiIÿyU IFTHI@TA yIÿƒiIÿyUTP IIIFQ@PA

i

yITP IFTQV@SA yIÿƒiIÿyI IIQFS@QA

q

yW IFTRS@UA yIÿƒiIÿyWTP IHUFS@PA

we—n IFTQI yUÿƒiIÿyW IHSFQ@QA

ƒiPÿyV IFTIR@UA yQÿƒiPÿyV TP IHVFV@PA

˜

yQTP IFTQI@RA yQÿƒiPÿyQ IIPFR@QA

yW IFTRH@UA yWÿƒiPÿyV IIHFT@QA

we—n IFTPW yWÿƒiPÿyQ TP IHVFP@PA

i

ƒiQÿyPTP IFTQH@RA yPÿƒiQÿyP IHQFQ@QA

yT IFTST@TA yTÿƒiQÿyP TP IIQFI@PA

yS IFTTT@UA ySÿƒiQÿyP TP IIQFP@PA

we—n IFTRT ySÿƒiQÿyT IHIFQ@QA

— ˜

ƒymmetry tr—nsform—tions used to gener—te equiv—lent —tomsY xD yCID zY xD

™ d d f

ÿyCÝD zY ÿxCID yÿÝD ÿzY ÿxCID ÿyCPD ÿzY xCID yD zY ÿxCID ÿyCPD

g h i j

ÿzCIY ÿxCID yÿÝD ÿzCIY ÿxCID ÿyCID ÿzCIY xD ÿyCÅÙ D zY ÿxD ÿyD ÿzY

Ä

k l m n o

xD yÿID zY ÿxD ÿyCID ÿzY ÿxCID ÿyD ÿzCIY xÿID yD zY ÿxD ÿyD ÿzCIY

p q

ÿxD ÿyCID ÿzCIY ÿxCID ÿyCID ÿzF

pl—™ed on — ufr pl—teF i—™h spe™trum w—s —void pro˜lems —sso™i—ted with mi™roE—˜sorptionF

ÿI

me—sured in the TSHÿRHHH ™m ƒili™on met—l powder w—s used —s —n —ngleE regionD with —

ÿI

™—li˜r—tion intern—l st—nd—rd for —ngle diffr—™tionF I™m resolutionF

i—™h mixture of —ll—nite s—mple @Q gA —nd sili™on

powder st—nd—rd @HFQQQ gA w—s —pplied to the noE

ƒingle ™ryst—l ˆEr—y intensity me—surement

re¯e™tion qu—rtz pl—teF

ƒingle ™ryst—l ˆEr—yEdiffr—™tion intensities for the

h—i˜os—tsu —ll—niteE@geA were ™olle™ted with —n pourierEtr—nsform infr—red mi™rospe™tros™opy

—utom—ted diffr—™tometer @gehRY inr—fExonius

ÿ

„he @yr fF†FA with gr—phiteEmono™hrom—ted woEu— A presen™e —nd met—mi™tiz—tion in

r—di—tion from —n irregul—r fr—gment of dimenE —ll—nites were ™on®rmed ˜y t—nssen wi™ro

sions HFITHFITHFI mmF „wenty re¯e™tions pourierEtr—nsform infr—red spe™tros™opy @p„s‚Y

within the r—nge PHë R Py R QHë were ™entred t—s™oD sn™FAF ƒingle ™ryst—ls of —ll—niteD PH mm

su™h th—t unitE™ell dimensions @„—˜le PA ™ould ˜e thi™kD were ™hosen under — stereomi™ros™ope —nd RHV griwsƒ„‚‰ yp evvexs„i IFHHH vFuF ƒ IFWS IFVI PFHI IFVV IFWS IFVV IFUS IFWW P —nd ƒ A w HFHVH for 8 HFPS PFHH HFUS IFWU HFWP IFHHH ƒ A c IFHHH c c HFWV P ID @el HFVW HFWP T Y Y w for c IFHHH c c ƒ HFWV A P IFHQ HFWT T HFHUT „i c QC HFQIU pe c cY HFWT P HFTHU IFHU HFWS T Y PD @el e cY cY Q ƒiI ƒiP ƒiQ r c cY w for HFPP HFQH P P HFSI HFST T T IFHHH ƒ A c P HFIHP cY T P 8 w SF impiri™—l ˜ond v—len™e @vFuFABF HFST HFSH P P HFHHV T T wn efvi „ cY c cY P P P HFHRP cY T T T I „h w QD respe™tivelyF „he ˜ond v—len™e of the r —tom w—s —ssigned to ˜e in —™™ord—n™e with the in™ident HFRS HFTP HFRI HFRV P P P P HFHIW w T T T T Y Y Y ƒm for cY P HFIHH IFHHH cY c cY T ƒ P A xd cY cY e HFQP HFPI HFIQ HFHV P P P P HFHQU HFHRV T T T T HFRV HFPP Y Y Y Y Y Y €r wg c HFRRQ P HFHSS T c c ge I wn c c c e HFQP HFQR HFHR HFPQV P P P QC HFQTS T T T HFIU HFHU HFQQ Y Y Y Y Y Y pe ID @v— e PC HFSRQ

v— IFWU PFIV PFWT QFHV PFII QFWR QFWS QFUU IFHH

@pe yS ƒ B „he ˜ondEv—len™e ™onst—nts —re from frese —nd y9ueefe @IWWIAF fondEv—len™e sums —re weighted ˜y the —tomi™ r—tio for @g— yP yR yT yU yV yW yIH yQ for ˜ondEv—len™e requirements of the yR —nd yIH —tomsF yI RHW

wF ryƒrsxy i„ evF

„efvi TF ile™tron mi™ropro˜e —n—lysis @me—n —nd st—nd—rd devi—tion of U pointsA of

—ll—nite from the h—i˜os—tsu €—ss used for the stru™ture re®nementF nit formul—e

norm—lized toIPFS oxygensF

yxide @wtF7A me—n sFdF —FpFfFuF me—n sFdF

QHFRW HFHP ƒi QFHHH HFHHR ƒiy P

„iy IFHT HFHQ „i HFHUT HFHHU P

„hy IFWI HFHI „h HFHRP HFHHS P

el y IRFPU HFHP el IFTHU HFHHS

P Q

QC

pe y WFHH HFHP pe HFTVP HFHHT P Q

v— y TFUR HFHP v— HFPQV HFHHS P Q

ge y IQFPV HFHQ ge HFRRQ HFHHS P Q

€r y IFQW HFHS €r HFHRV HFHHV P Q

xd y PFWQ HFHI xd HFIHH HFHHQ P Q

ƒm y HFSW HFHS ƒm HFHIW HFHHU

P Q

PC

pey UFIT HFHP pe HFSRQ HFHHT

wny HFUV HFHR wn HFHTQ HFHHT

wgy HFPT HFHP wg HFHQU HFHHS

g—y VFWW HFHP g— HFWPH HFHHS

„ot—l WVFVS HFHQ „ot—l UFVIV HFHHT

ghemi™—l formul—X

@g— 8 A @v— ge €r xd ƒm „h wn 8 A

HFWPH HFHVH ƒIFHHH HFPQV HFRRQ HFHRV HFIHH HFHIW HFHRP HFHHV HFIHP ƒIFHHH

QC PC QC

@el pe „i A @el A@pe pe wn wg A @ƒiy A@ƒi y Ay@yrAF HFQIU HFSRQ HFQTS HFTHU HFHUT ƒIFHHH IFHHH HFHSS HFHQU ƒIFHHH R P U

8 st—nds for — defe™tF

es™—pes iw€e dete™tionF por ™—l™ul—tion of re®ned ˜y le—stEsqu—res from the result—nt setting

PC QC

pe —nglesF sntensity d—t— were ™olle™ted in oEPy s™—nE Gpe in —ll—nite formul—D ir™it @PHHPA h—s

mode —t — ®xed s™—nEr—te of IFHëPyG minF sn —llD suggested th—t the method ˜—sed on T @wC„A

SSSU re¯e™tions were me—sured within the r—nge ™—tions —nd IP @yA C I@yrA per formul— is

of Rë R Py R THëF €siEs™—n d—t— were me—sured superiorF roweverD his ™—l™ul—tion of the —ll—nite

on ®ve re¯e™tions —t in™rements of IHë —˜out the formul— w—s suggested ˜—sed on the ™hemi™—l

diffr—™tion ve™torY —˜sorption ™orre™tion w—s ™ompositions ˜efore est—˜lishment of the

—pplied using the semiEempiri™—l method @xorth improved iw€e method for —™™ur—te ‚ii

et —lFD IWTVAF h—t— were ™orre™ted for vorentzD dete™tion @‚eed —nd fu™kleyD IWWVY xishid— et

pol—riz—tion —nd ˜—™kground effe™tsD —ver—ged —nd —lFD IWWWAF „hus it is —ssumed th—t ƒi is Q —s — ˜—sis

redu™ed to stru™ture f—™torsF „he result—nt IRSW of norm—liz—tionD whi™h h—s ˜een —pplied in

unique re¯e™tions were ™onsidered —s o˜served ™ryst—l stru™ture re®nements of ‚iiE˜e—ring

‘p epidote group miner—ls @holl—seD IWUIY €e—™or aRs@p A“F pin—l —tomi™ position—l —nd H H

—nd hunnD IWVVY ‚ouse —nd €e—™orD IWWQAF equiv—lent displ—™ement p—r—meters —re given in

„hereforeD stru™tur—l formul—e were ™—l™ul—ted „—˜le QF „—˜le R shows sele™ted inter—tomi™

˜—sed on IPFS oxygensD —fter norm—liz—tion of dist—n™es —nd —nglesF „—˜le S presents ˜ond

™hemi™—l d—t— to Q ƒi —toms per formul— unitF v—len™e —n—lysisF

„—˜le T lists —ssignments of ™—tions ˜—sed on

™h—rge ˜—l—n™eF ell—nites from gr—niti™ ro™ks of

‚esults

r—guriD ymiy—d—niD h—i—nD ƒuishoy—m—D

ghemi™—l ™omposition pukud—y—m— —nd ƒhimoEono in t—p—nD were —lso

—n—lysed ˜y iw€eF „he lo™—tion of these s—mples „he present iw€e demonstr—tes th—t ge is

—re shown in pigF IF ell of these —ll—nites proved predomin—nt over other ‚ii in —ll —n—lysed

to ˜e of — ge typeF „—˜les U —nd V list ™hemi™—l —ll—nite gr—ins from the h—i˜os—tsu €—ssD whi™h

™ompositions of these —ll—nites in ™omp—rison were identi®ed —s —ll—niteE@geA @„—˜le TAF „his

with th—t of the re®ned —ll—nite from the —ll—nite is ™h—r—™terized ˜y — n—rrow r—nge of

h—i˜os—tsu €—ss @„—˜le TAF ™omposition—l v—ri—tion —nd its ™hemi™—l zoning RIH

griwsƒ„‚‰ yp evvexs„i

„efvi UF ile™tron mi™ropro˜e —n—lysis @me—n —nd st—nd—rd devi—tion of IH pointsA of —ll—nites from r—guriD

ymiy—d—ni —nd h—i—n in t—p—nF nit formul—e norm—lized to IPFS oxygensF

yxide @wtF7A r—guriEh r—guriEf ymiy—d—niEh ymiy—d—niEf h—i—nEh h—i—nEf

me—n sFdF me—n sFd me—n sFdF me—n sFdF me—n sFdF me—n sFdF

ƒiy QIFRR HFHS QIFPQ HFHU QQFRV HFHS QQFUU HFHQ QPFQH HFHQ QPFIR HFHS P

„iy HFHH HFHH HFHH HFHH IFIT HFHP HFRP HFHS IFSU HFHP IFRW HFHU P

„hy IFUT HFHU IFRV HFHR IFIQ HFHR IFPT HFHP QFTH HFHI QFPH HFHS P

el y ISFWT HFHS ISFVQ HFHQ IUFUQ HFHR IUFUP HFHQ ITFUQ HFHR ISFQP HFHR P Q

pe y VFSI HFHV VFUH HFHS TFSS HFHQ UFPU HFHQ UFPS HFHS UFRT HFHP P Q

‰ y IFWQ HFHR IFWH HFHI HFHH HFHH HFHH HFHH HFUS HFHQ HFWI HFHQ P Q

v— y PFPV HFHQ PFPT HFHP SFVW HFHU SFWW HFHT RFRR HFHP SFHP HFHR P Q

ge y TFTS HFHP TFTT HFHP VFQQ HFHS VFUR HFHS UFVP HFHR VFHV HFHR P Q

€r y IFRV HFHQ IFSP HFHQ IFIT HFHS IFIW HFHV IFQP HFHR IFQU HFHP P Q

xd y TFPH HFHR TFPT HFHP QFRQ HFHR RFHP HFHS QFWV HFHS RFQI HFHI P Q

ƒm y PFVU HFHP PFVV HFHR HFSH HFHP HFSR HFHR HFWV HFHP HFIU HFHS P Q

qd y PFHV HFHS PFPI HFHS IFHP HFHQ IFHS HFHR IFHI HFHI IFHT HFHR P Q

hy y HFVT HFHQ HFVR HFHQ HFHH HFHH HFHH HFHH HFSP HFHI HFTI HFHP P Q

pey UFVQ HFHV VFPS HFHP TFIP HFHQ TFVP HFHQ TFUI HFHS TFUS HFHP

ny HFHH HFHH HFHH HFHH HFSQ HFHR HFQP HFHR HFHH HFHH HFHH HFHH

wny TFTI HFHR UFQI HFHS HFSR HFHS HFTS HFHP IFHI HFHR IFHS HFHI

wgy HFHH HFHH HFHH HFHH HFVS HFHR HFSH HFHR HFRT HFHQ HFSS HFHR

g—y QFIQ HFHR PFQQ HFHI IIFPI HFHQ WFVI HFHS UFVV HFHR WFQI HFHR

„ot—l WWFSV HFHS WWFTT HFHQ WWFTQ HFHR WWFPW HFHR WVFQQ HFHQ WVFVH HFHR

ell—nites from r—guriD ymiy—d—ni —nd h—i—n h—ve two kinds of d—rk @hA —nd light @fA dom—insD o˜served on the

˜—™ks™—ttered ele™tron im—geF

ghemi™—l formul—

r—guriEhX

PC

@g— wn 8 A @‰ v— ge €r xd ƒm qd hy „h pe 8 A

HFHRT HFQPI HFSQT HFIRQ ƒIFHHH HFHWV HFHVI HFPQQ HFHSP HFPIP HFHWS HFHTT HFHPT HFHQV HFHSQ ƒIFHHH

QC PC QC

@el pe A @el A@pe pe A @ƒiy A@ƒi y A y@yrAF HFIWU HFSSH HFRSH HFVHQ ƒIFHHH IFHHH ƒIFHHH R P U

r—guriEfX

PC

@g— wn 8 A @‰ v— ge €r xd ƒm qd hy „h pe 8 A

HFHVS HFPQW HFSWS HFITT ƒIFHHH HFHWU HFHVH HFPQS HFHSQ HFPIS HFHWS HFHUH HFHPT HFHQP HFHIP ƒIFHHH

QC PC QC

@el pe A@el A@pe pe A @ƒiy A@ƒi y A y@yrAF HFPHU HFSVS HFRIS HFUWQ IFHHH ƒIFHHH R P U

ymiy—d—niEhX

PC QC

@g— A@v— ge €r xd ƒm qd „h g— pe 8 A @el „i pe A

HFHRH HFHRW IFHHH HFIWS HFPTI HFHQV HFIIH HFHIS HFHQH HFHPQ HFHUT HFPIP ƒIFHHH HFVUQ HFHUV ƒIFHHH

PC QC

@el A @pe pe wg wn n A @ƒiy A@ƒi y A y@yrAF IFHHH ƒIFHHH HFIIQ HFHRI HFHQS ƒIFHHH R P U HFRIV HFQWQ

ymiy—d—niEfX

PC

@g— 8 A @v— ge €r xd ƒm qd „h pe 8 A

HFWSS HFHRS ƒIFHHH HFPHI HFPUU HFHQW HFIQI HFHIU HFHQP HFHPT HFHRR ƒIFHHH HFHVP

QC PC QC

@el pe „i A @el A@pe pe wg wn n A @ƒiy A@ƒi y A y@yrAF HFVWW HFHPW ƒIFHHH IFHHH HFHTV HFHSH HFHPI ƒIFHHH R P U HFHUP HFRQT HFRPS

h—i—nEhX

PC

@g— 8 A @‰ v— ge €r xd ƒm qd hy „h pe 8 A

HFIIP HFUVR HFPIT ƒIFHHH HFHQU HFISP HFPSR HFHRS HFIQP HFHQI HFHQI HFHIT HFHUT HFIIR ƒIFHHH

QC QC PC

@el „i pe A @el A@pe pe wn wg A @ƒiy A@ƒi y A y@yrAF HFHSW HFRRV HFRHW HFVQI HFIIH ƒIFHHH IFHHH HFHUW HFHTR ƒIFHHH R P U

h—i—nEfX

PC

@g— 8 A @‰ v— ge €r xd ƒm qd hy „h pe 8 A

HFHHI HFWQI HFHTW ƒIFHHH HFHRS HFIUQ HFPTQ HFHRU HFIRR HFHHS HFHQQ HFHIV HFHTV HFPHQ ƒIFHHH

QC PC QC

@el pe „i A @el A@pe pe wn wg A @ƒiy A@ƒi y A y@yrAF HFPIH HFSPT HFQIR HFTVS HFIHS ƒIFHHH IFHHH HFHVQ HFHUU ƒIFHHH R P U

8 st—nds for — defe™tF

TD U —nd VAD —pproxim—tely ™onsistent with the „he present —ll—nites h—ve only moder—te wn

™ompiled d—t— for ™hemi™—l ™ompositions of ™ontentsD ˜ut the —ll—nites from r—guri —nd

—ll—nite @qiere —nd ƒorensenD PHHRAF „his ƒuishoy—m— h—ve —ppre™i—˜le wn ™ontents

in™orpor—tion ™ontr—sts with v—ri—tions in „h @~U wtF7 wnyAD equiv—lent to m—ng—no—n —ll—E

™ontent ˜etween gr—ins within — single thin nite ™ont—ining TFUR wtF7 of wny @ruttonD

se™tion of —ll—nite in gr—nite from t—p—n IWSIAF woreoverD „hy ™ontents in the —n—lysed P

@r—y—seD IWSRAF rowever the me™h—nisms of —ll—nites —re in the r—nge IFIQÿQFTH wtF7 @„—˜les RII

wF ryƒrsxy i„ evF

„efvi VF ile™tron mi™ropro˜e —n—lysis @me—n —nd st—nd—rd devi—tion of IH pointsA of —ll—nites from

ƒuishoy—m—D pukud—y—m— —nd ƒhimoEono in t—p—nF nit formul—e norm—lized toIPFS oxygensF

yxide @wtF7A ƒuishoy—m— pukud—y—m— ƒhimoEono

me—n sFdF me—n sFdF me—n sFdF

ƒiy QHFSR HFHT QPFII HFIU QIFQU HFPU P

„iy HFHH HFHH HFHH HFHH IFRH HFHP P

„hy IFIU HFHR PFVI HFHQ QFRQ HFHW P

el y IQFSS HFHS ITFQT HFIP IQFTT HFIH P Q

pe y VFRU HFHR VFSS HFHT UFWT HFII P Q

Ī y HFIW HFHI HFPR HFHH HFHH HFHH P Q

‰ y IFQT HFHW PFUU HFHR IFRS HFHR P Q

v— y QFTP HFIQ PFIR HFHS PFQP HFHU P Q

ge y VFQT HFIR RFTV HFIP SFQU HFIU P Q

€r y IFUW HFHQ IFPI HFHP IFRS HFHQ P Q

xd y SFSI HFHS RFPP HFHR SFTU HFHS P Q

ƒm y IFWU HFHR PFRS HFHS PFPS HFHR P Q

qd y IFST HFHT PFSS HFHI IFWI HFHP P Q

hy y IFIH HFHP IFSS HFHR IFHV HFHR P Q

pey UFWT HFHR UFSQ HFHT VFQP HFII

wny TFUH HFIV PFVQ HFHR QFWP HFHS

wgy HFHH HFHH HFHH HFHH HFPU HFHH

g—y RFVI HFII UFRQ HFHR UFVP HFHT

„ot—l WVFTT HFIW WWFRQ HFQS WWFTS HFTI

ghemi™—l formul—

ƒuishoy—m—X

@g— wn A @ƒ™ ‰ v— ge €r xd ƒm qd hy „h 8 A

HFSHV HFRPI ƒIFHHH HFHIT HFHUP HFIQP HFQHP HFHTR HFIWR HFHTU HFHSI HFHQS HFHPT HFHRP ƒIFHHH

QC PC QC

@el pe A @el A@pe pe wn A @ƒiy A@ƒi y A y@yrAF HFSUS ƒIFHHH IFHHH HFIQW ƒIFHHH R P U HFRPS HFTPQ HFPQV

pukud—y—m—X

@g— wn 8 A @ƒ™ ‰ v— ge €r xd ƒm qd hy „h

HFURV HFPPS HFHPU ƒIFHHH HFHP HFIQW HFHUR HFITI HFHRI HFIRP HFHUW HFHUW HFHRU HFHTH

PC QC PC QC

pe 8 A @el pe A @el A@pe pe wn wg A @ƒiy A@ƒi y A y@yrAF HFHIH HFPHU HFSVS HFRIS HFIRV ƒIFHHH HFUWQ ƒIFHHH IFHHH HFHVP HFHQV ƒIFHHH R P U

ƒhimoEonoX

@g— wn A @‰ v— ge €r xd ƒm qd hy „h wn 8 A

HFVHQ HFIWU ƒIFHHH HFHUR HFHVP HFIVV HFHSI HFIWR HFHUR HFHTI HFHQQ HFHUS HFHQW HFIPW ƒIFHHH

QC PC QC

@el pe „i A @el A@pe pe wn wg A @ƒiy A@ƒi y Ay@yrAF HFQSU HFTQP HFPRV HFSRP HFIHI ƒIFHHH IFHHH HFHVP HFHQV ƒIFHHH R P U

8 st—nds for — defe™tF

h—i˜os—tsu €—ssD ƒuishoy—m—D pukud—y—m— —nd ™oupled su˜stitutions responsi˜le for „h in™orE

ƒhimoEonoD respe™tivelyD —re ™omp—red in „—˜le W por—tion —re ™omplex —nd spe™ul—tive @qiere —nd

—nd pigF RF „he pro™ess of met—mi™tiz—tion of ƒorensenD PHHRAF „he most distin™tive fe—ture of

—ll—nite gre—tly in¯uen™es intensities —nd d sp—E —ll—nites from gr—niti™ ro™ks of the t—p—nese

™ings of its ˆEr—y powder diffr—™tion lines @eFgF isl—nd —r™ is th—t no w—s dete™ted ˜y iw€e

ed—D IWSUY €ell—sD IWTIAF ‡ith de™re—sing even though „h is present in —ll the s—mplesF heer

degree of l—tti™e orderingD diffr—™tion pe—ks et —lF @IWVTA did suggest th—t „h —nd —re present

—ppe—r to ˜e™ome less intense —nd less sh—rpF es in the m—jority of —ll—nitesF rowever some reports

is evident from „—˜le W —nd pigF RD with @eFgF r—seg—w—D IWTHY ƒuzuki et —lFD IWWHA

in™re—sing —morphiz—tionD the ˆ‚h pe—ks ™on™luded th—t —ll—nites from gr—niti™ ro™ks in

de™re—se in ˜oth sh—rpness —nd intensityD ˜ut t—p—n often ™ont—in less th—n HFI7 F „hE

their shift tow—rds lower Py @iFeF l—rger d sp—E p—rtitioning ˜etween —ll—nite —nd melt @or

™ingsA is not distin™tive ˜e™—use of the v—riety of solutionA will ˜e dis™ussed in more det—il l—terF

™hemi™—l ™omposition of the investig—ted —ll—E

nitesD —nd ®n—lly they f—de —w—yX the degree of

ˆEr—y powder diffr—™tion

met—mi™tiz—tion in™re—ses in the orderX

h—i˜os—tsu €—ssD ƒuishoy—m—D pukud—y—m— —nd sntensities of two ˆEr—y powder diffr—™tion linesD

Å Å ƒhimoEonoF woreoverD ™l—y miner—ls were not s@PIIA—nds@IIQAD for —ll—nites from the RIP

griwsƒ„‚‰ yp evvexs„i

psqF RF €ˆ‚h p—tterns of four —ll—nites @h—i˜os—tsu €—ssD ƒuishoy—m—D pukud—y—m— —nd ƒhimoEonoA representing the

Å Py r—nges suggestive of r—di—tion d—m—geD from well ™ryst—llized to fully met—mi™t st—tesF @—A €ro®les of @PIIA pe—kF

Å @˜A €ro®les of @IIQA pe—kF

pourierEtr—nsform infr—red mi™rospe™tros™opy

dete™ted in these —ll—nitesD whi™h shows th—t these

ÿ

„he @yr —ll—nites were not —lteredF „hereforeD the de™re—se A spe™trum of un—ltered —nd nonE

in ™ryst—llinity of the ex—mined —ll—nites is found met—mi™t —ll—nite from the h—i˜os—tsu €—ss

to result from met—mi™tiz—tion onlyF „hereforeD ™onsists of two m—in stret™hing ˜—nds —t

ÿI ÿI

the h—i˜os—tsu —ll—nite is — suit—˜le s—mple for QIVU ™m —nd QQSS ™m @pigF SAF „his o˜serE

™ryst—l stru™ture re®nementF v—tion entirely ™onforms with the yrEstret™hing RIQ

wF ryƒrsxy i„ evF

„efvi WF „he d sp—™ingD full width —t h—lf m—ximum @p‡rwA intensity —nd

Å intensity for fr—gg —nd diffuse s™—ttering ™omponents of the @PIIA —nd

Å @IIQA re¯e™tions of —ll—nites from gr—niti™ pegm—tites in t—p—nF

ƒ—mple d p‡rw sntensity

Ê @eA @ëPyA @™ountsGmgAB

Å PII refle™tion

h—i˜os—tsu €—ss QFSIT HFIRW QUFT

ƒuisyoy—m— QFSPH HFPQT IPFH

pukud—y—m— QFSIS HFPRU UFT

ƒhimoEono nFdFBB nFdF nFdF

Å IIQ refle™tion

h—i˜os—tsu €—ss PFWHS HFIVT VSFT

ƒuisyoy—m— PFWIP HFPUV QQFT

pukud—y—m— PFWIT HFQPI IQFT

ƒhimoEono nFdF nFdF nFdF

B sntensity of investig—ted —ll—nites is norm—lized to the —mount of s—mple

mounted on —n ˆEr—y nonEre¯e™tion qu—rtz holderF

BB nFdFX not dete™tedF

Ï re®nement led to ™—l™ul—tion of — threeEdimenE ˜—nds in epidote @ge™h et —lFD IWUPAF yn the other

sion—l differen™eEpourier m—pD where the hydrogen h—ndD the spe™tr— of met—mi™t —ll—nites from

—tom position w—s not determinedF gr—niti™ ro™ks from ƒuishoy—m—D pukud—y—m—

purther re®nement w—s ™—rried out with only ƒi —nd ƒhimoEono show rel—tively ˜ro—d —˜sorption

ÿI

—ssigned to tetr—hedr—l sitesD —s re®ned with only pe—ks —t ~QPPSD QPIV —nd QPHW ™m D respe™E

ƒi o™™upying three tetr—hedr—l sites for epidote tively @pigF SAD very different from those in the

group miner—ls @eFgF holl—seD IWUIY ‚ouse —nd h—i˜os—tsu —ll—niteF sn —dditionD the ƒiyE

ÿI

€e—™orD IWWQY fon—zzi et —lFD IWWTAF porm f—™tors stret™hing ˜—nd —t IHQS ™m of the h—i˜os—tsu

for g— —nd @‚ii C „h C wnA were —ppliedD —ll—nite shifted tow—rds the lower w—venum˜ers

ÿI

respe™tivelyF y™™up—n™ies of g— in eI —nd @‚ii @~IHPID IHIU —nd IHHR ™m A with the in™re—sing

C „h C wnA in eP were re®ned together with met—mi™t st—te ™h—r—™teristi™ of the other —ll—nites

™oordin—tes —nd isotropi™ temper—ture f—™tors to @pigF SAF ƒimil—r shifts were o˜served in the

determine the distri˜ution of g— —nd @‚ii C„hC ™orresponding spe™tr— of —ll—niteD zir™on —nd

wnA in eI —nd eP sites of —ll—niteF porm f—™tors their met—mi™t equiv—lents @t—ne™zek —nd i˜yD

for wID wP —nd wQ sites were modeled with IWWQY h—ng —nd ƒ—ljeD PHHIAF „hereforeD the yrE

QC QC QC

@HFTHUel —nd ƒiyEstret™hing ˜—nds m—y serve —s indi™—tors C HFQIUpe C HFHUT„iAD el —nd

PC QC

of met—mi™tiz—tionF @HFSRQpe C HFQTSpe C HFHSSwn C HFHQUwgAD

respe™tivelyD ˜—sed on ™onsider—tions of ™h—rge

˜—l—n™eD the ™ryst—lE™hemi™—l d—t— for other

ƒtru™ture ref|nement

epidote group miner—ls @holl—seD IWUIY uvi™k et

„he progr—m ƒrivˆvEWU @ƒheldri™kD IWWUA w—s —lFD IWVVY ‚ouse —nd €e—™orD IWWQAD —nd known

used throughout this workF ‚e®nement of the inter—tomi™ dist—n™es in —ll—nites @holl—seD IWUIAF

QC

present stru™ture under the ™onstr—ints of the sn p—rti™ul—rD eI h—s — strong preferen™e for wP

™hemi™—l ™ompositionD whi™h is signi®™—ntly in epidote stru™turesD where—s ™l—rifying —ny

different from th—t est—˜lished ˜y holl—se @IWUIAD —m˜iguity in the distri˜ution of other ™—tions

w—s ™—rried out in the sp—™e group €P through re®nement is dif®™ult ˜e™—use of the GmDwith I

simil—rity in respe™tive form f—™tors of el —nd stru™tur—l p—r—meters given ˜y holl—se @IWUIAF

wgD —nd pe —nd wnF „hereforeD ™—tionEo™™up—nE ‚e®nement of the position—l p—r—meters —nd

™ies for wI —nd wQ sites were ®xed —t the isotropi™ displ—™ement p—r—meters ™onverged to

represent—tive iw€e v—lue @„—˜le TAF por th—t —n ‚ index of QFVR7F „he —nisotropi™ displ—™ement

re—sonD st—rting o™™up—n™y f—™tors ™—n ˜e tested modelD together with re®nement of —ll p—r—metersD

˜y ™omp—ring expe™ted me—n ˜ond lengths for the suggested —n ‚ index of QFRT7F „his st—ge of RIR

griwsƒ„‚‰ yp evvexs„i

QC PC

pe EyD „iEyD wn Ey —nd wgEy from the survey

of f—ur @IWVIAD with the o˜served me—n ˜ond

lengths @„—˜le RAF es shown in „—˜le IHD

simil—rity ˜etween the predi™ted —nd o˜served

me—ns is ™onsidered to ˜e suf®™ient ˜e™—use

differen™es in wI —nd wP sites —re no more th—n

Ê ÔHFHI eF „he error in me—surements of ˜ond

lengths of the wQ site is l—rger th—n those of the

wI —nd wP sitesD —nd is ™onsidered to result from

PC

˜oth the t—hnE„eller effe™t of pe in wQ site

@usenofontov et —lFD IWVSA —nd deform—tion of wQ

polyhedr— sh—ring edges with distorted ‚iiE

˜e—ring eP polyhedr— @pigF TAF gon™erning the

presen™e of v—™—n™ies @8A in the e sitesD €eterson

—nd w—™p—rl—ne @IWWQA reported the defe™t

r—nging from HFHS to HFRHD while re®nement of

the ™ryst—l stru™ture of khristoviteE@geA @ƒokolov—

et —lFD IWWIA suggested th—t there —re 8 —t the HFPH

eI site —nd 8 —t ePF ell —ll—nite gr—ins HFHU

—n—lysed in this study —lso ret—in the defe™t in e

sites r—nging from HFHRP to HFQQH @„—˜les TD U —nd

VAF fesidesD the result of the stru™tur—l re®nement

for the present —ll—nite s—mple from the

h—i˜os—tsu €—ss showed th—t eI —nd eP sites

h—ve HFHVH —nd HFIHP v—™—n™iesD respe™tivelyF

„his model is supported ˜y ˜ondEv—len™e

QC

™onsider—tionsX gre—ter ™h—rge ™—tions @‚ii D

RC

„h A prefer ePD —nd the ˜ondEv—len™e ™ontri˜uE

tions from the WE™oordin—ted ™—tion —t eI to its

™oordin—ting —nions —re mu™h less th—n those from

the IHE™oordin—ted ™—tion —t eP@„—˜leSAF

„hereforeD the v—™—n™ies —t the eI —nd eP sites

determined ˜y the ™hemi™—l ™omposition —nd

™ryst—l stru™ture re®nement for the h—i˜os—tsu

—ll—nite will ®nd gener—l —™™ept—n™e with the

™ryst—l ™hemistry of —ll—niteF

his™ussion

gryst—l ™hemistry of —ll—nite

„he ™oordin—tion polyhedr— —re where ‚iis —re

known to ˜e distorted in inorg—ni™ l—nth—nide

„efvi IHF gomp—rison ˜etween the me—n

˜ond lengths ™—l™ul—ted —nd o˜served for

w sitesF

psqF SF s‚ d—t— for nonEmet—mi™t —ll—nites from the

h—i˜os—tsu €—ssD —nd for met—mi™t —ll—nites from

g—l™ul—ted y˜served

ƒuishyoy—m—D pukud—y—m— —nd ƒhimoEonoF

wI IFWS IFWT

wP IFWI IFWH

w sitesD ™—l™ul—ted using the proportions of elD peD

wQ PFHW PFIT

„iD wn —nd wg from the re®nement —nd the me—n

PC

of —ll me—surements v—lues for elEyD pe EyD RIS

wF ryƒrsxy i„ evF

psqF TF „he stru™ture of epidote group miner—ls with edge sh—ring eP polyhedr—D wQ o™t—hedr— —nd ƒiQ tetr—hedr— ˜y

D respe™tivelyF „he other y —toms —re shown —s BF yP —nd yV —tomsF yP —nd yV —toms —re shown —s T —nd

stru™tureF „he o˜serv—tion th—t distortion of the ™ompounds with ™omplex —nions @‡i™klederD

ƒiQ tetr—hedron is —lw—ys the l—rgest is ™ommon to PHHPAF sn ‚iisD ele™trons —re removed from the

epidote group miner—ls @„—˜le IIAF holl—se lo™—lized Rf st—teF e™™ording to the expl—n—tion ˜y

@IWUIA indi™—ted th—t the ƒiQ tetr—hedron is furdett @IWWSAD wh—t h—ppens is the ™re—tion of —

somewh—t distorted pro˜—˜ly due to the f—™t th—t sm—ll pol—ronD — region —sso™i—ted with — lo™—l

geometri™—l distortion —round the site where one

‚ii —tom h—s lost ele™tronsF „hereforeD in —ll—nite

the polyhedr— with the eP sites o™™upied ˜y ‚ii

tend tow—rds distortionF

„he o˜serv—tion of h Gh `I@hX the ˜ulk „h

solid p—rtition ™oef®™ients for —nd „hA in —ll—nite

h—s often ˜een reported @eFgF y˜erli et —lFD IWVID

PHHRAF „he su˜stitution me™h—nism responsi˜le for

„h in™orpor—tion in the present —ll—nites @„—˜les TD

U —nd VA ™—n ˜e expl—ined ˜y the following

RC QC

rel—tionX Q„h C 8 @v—™—n™yA b R‚ii Dwhi™h

w—s demonstr—ted in pigF UF „his rel—tionship

RC

me—ns th—t ™ryst—l ™hemi™—l properties of „h

QC

—nd ‚ii ™—tions h—rmonize with —n ePsitein

RC RC

—ll—niteF e site preferen™e of „h r—ther th—n

in the —ll—nite stru™ture is ™onsidered to ˜e due to

l—rgeD ‚ii eP l—tti™e sitesD more f—vour—˜le to the

Ê

in™orpor—tion of the l—rger „h ion @IFHS e in

RC

Ê †sssEfold ™oordin—tionA th—n @IFHH eAF

„etr—hedr—l distortions for ƒiy —nd ƒi y of R P U psqF UF €lot illustr—ting potenti—l ™oupled su˜stitution in

epidote group miner—ls were ™—l™ul—ted following —ll—nite in gr—niti™ ro™ks from t—p—nF „he ™omposition of

the method of ‚o˜inson et —lF @IWUIAF pigure T s—mple ymiy—d—niEh in „—˜le U shows it is from — littleE

illustr—tes the polyhedr—l link—ge of three ƒi —ltered rim of — single —ll—nite ™ryst—lF „hereforeD the

ymiy—d—niEh s—mple is not shown in pigF UF tetr—hedr—D eI—ndeP sites in the —ll—nite RIT griwsƒ„‚‰ yp evvexs„i IWVVA ell—nite @IWUIABF @this studyA holl—seiteE@geA @€e—™or —nd hunnD et —lF ell—nite r—n™o™kite @holl—seD IWUIA @holl—seD IWUIA D D et —lF et —lF IWWHA PHHQA @fon—zzi a perri—ll—niteE@geA @u—rt—shov ƒtrontiopiemontite ./. D D 109 47 5 et —lF et —lF i () 1 IWVWA IWWTA 6 = i ∑ €iemontite @ƒiQA of epidote group miner—ls ™—l™ul—ted —fter ‚o˜inson Eri™h piemontite =−° R @perr—ris @fon—zzi 2 ‚ii tet () θ σθ D D IWVVA et —lF et —lF IWWTA ipidote endrositeE@v—A @fon—zzi @ƒiI —nd ƒiPA —nd ƒiy U @uvi™k y P D IWUQA et —lF IWWQA ipidote h—iss—kisiteE@geA @q—˜e @‚ouse —nd €e—™orD D et —lF IIF „etr—hedr—l distortions for ƒi IWWIA ipidote @holl—seD IWUIA efvi uhristoviteE@geA @ƒokolov— „

ƒiIƒiPƒiQ PFWU IFVU RFSH QFPP PFPH RFTU QFIV IFVQ QFWW PFWQ IFUQ RFQI PFWW IFWW RFRW PFUS IFRQ QFQS QFUV PFIH SFSR ƒiIƒiPƒiQ QFPRB IFTW histortion for ƒi tetr—hedr— SFPQ ™—l™ul—ted —™™ording to the formul— of PFVW PFHU SFRQ QFSI IFUW SFQP QFHV IFTT RFUH QFQH IFVW SFVR PFVU PFHH SFVH QFIP IFUH SFTR RIU

wF ryƒrsxy i„ evF

—ver—ge ˜ond lengths following the modi®ed it sh—res —n edge with the eP polyhedron —nd the

method of ‚o˜inson et —lF @IWUIAF „he dotted opposite edge with the eI polyhedronF „he eP

lines in pigF V indi™—te th—t the eEsite distortions sites of epidote group miner—ls h—ve the following

of ‚iiE˜e—ring epidote group miner—ls @—ll—nite o™™up—n™iesX @g— A—nd@g— wn Ain IFHH HFWV HFHP

zoneA —re l—rger th—n those of the other epidote epidote @holl—seD IWUIY q—˜e et —lFD IWUQY uvi™k

group miner—ls @nonE—ll—nite zoneAF „he l—rger et —lFD IWVVAD @g— ƒr A in piemontite @perr—ris HFVR HFIT

distortion of e sites in —ll—nites is ™—used ˜y et —lFD IWVWAD @ƒr g— A —nd @ƒr g— Ain HFSW HFRI HFUQ HFPU

o™™up—n™y of ‚ii —t eP sitesF „he ˜ond v—len™e strontiopiemontite @fon—zzi et —lFD IWWHAD

sum w—s ™—l™ul—ted to est—˜lish the ™redi˜ility of @€˜ ƒr @g—DwnA A in h—n™o™kite @holl—seD HFS HFPS HFPS

the re®ned ™ryst—l stru™tureF „he ™—l™ul—tion w—s IWUIAF yn the other h—ndD the eP sites of —ll—nites

™—rried out —s ˜y frown —nd elterm—tt @IWVSA in™orpor—te ‚iiD „h —nd wnF „his in™orpor—tion

with p—r—meters given ˜y frese —nd y9ueeffe indi™—tes th—t there is — disordered distri˜ution of

@IWWIAF fond v—len™es of yP —nd yV —re these ™—tions —t eP sitesF sn—smu™h —s the distorted

unders—tur—ted in ™omp—rison with the ide—l eP polyhedron —™™ommod—ting ‚ii sh—res one

˜ond v—len™eD PFHHD for —n y —tom @„—˜le SAF yPÿyP edge with the ƒiQ tetr—hedron @pigF TAD it

„he ˜ond v—len™e model does not ne™ess—rily give is re—son—˜le th—t ƒiQ distortion of —ll—nite is

—n un—m˜iguous des™ription for — defe™t environE gre—ter th—n th—t of the other epidote group

ment @frownD PHHPAF woreoverD unders—tur—tion miner—lsF

of ˜ond v—len™e sums for yP —nd yV —re pigure V shows th—t distortions of —ver—ged e

interpreted —s the effe™t of defe™t —t the eP siteF —nd w sites of —ll—nite from the h—i˜os—tsu €—ss

yn the other h—ndD the ˜ond v—len™e sums for yR ™—n ˜e distinguished from those of other epidote

—nd yIH —re IFUQ —nd IFPP vFuFD respe™tivelyD group miner—lsX they were ™—l™ul—ted from

psqF VF ‚el—tionship ˜etween —ver—ged distortions of e —nd w sites in epidote group miner—lsF „he dotted line

represents the ˜ound—ry ˜etween —ll—nites —nd the other epidote group miner—lsF „he modi®ed method of ‚o˜inson et

@IWUIA is —s followsX

—lF λλ 9 10

AA12+ = 2 = 2 D where for eID for the eP siteF e sitesX @IA iqu—tion for distortion of ∑()//9 ∑()//10 λ A= λ Ai10ll λ Ai20ll 2 i=1 i=1

++ 6 2

λλλMM123 M = D where for e—™h w siteF w sitesX

@PA iqu—tion for distortion of = λ ∑()//6

λ M Mill0 3 i=1 RIV

griwsƒ„‚‰ yp evvexs„i

„hereforeD this unique in™orpor—tion of „h h—s —n implying th—t the yIH —tom is the donor oxygen

impli™—tion for the ™ryst—lliz—tion me™h—nism of for the r —tom @„—˜le SAF e ®rm ™hemi™—l ˜ond

—ll—nite in gr—niti™ ro™ksF roweverD some reports exists ˜etween r —nd yIHF „he ™hemi™—l ˜ond

@eFgF r—seg—w—D IWTHY ƒuzuki et —lFD IWWHA ˜etween yIH —nd r in —ll—nite is ™onsistent with

™on™luded th—t —ll—nites from gr—niti™ ro™ks in those in ferri—ll—niteE@geA @u—rt—shov et —lFD PHHPA

t—p—n often ™ont—in `HFI7 F st is r—re for —ll—nite —nd in epidote @uvi™k et —lFD IWVVAF „—˜le IP

to ™ont—in more th—n „h @qiere —nd ƒorensenD topologi™—lly summ—rizes ™on®gur—tions of

PHHRAD eFgF in the met—som—ti™—lly formed ™ryst—ls hydrogen ˜onds for epidote group miner—lsF „he

from E‚ii sk—rn @w——s et —lFD IWVUA —nd in the yRÿyIH dist—n™e of the present —ll—nite is

Ê ™ryst—ls o™™urring in ˜lues™hists from the o˜served to ˜e PFWQ eF por th—t re—sonD if

ƒ—n˜—g—w— ˜elt of t—p—n @f—nnoD IWWQAF „hese yIHÿr —nd yR•r dist—n™es —re presumed to

Ê o˜serv—tions ™on®rm th—t the —ll—nites in gr—niti™ ˜e HFWT —nd IFWU eD respe™tivelyD then the ˜ond

ro™ks from the t—p—nese isl—nd —r™ h—ve experiE —ngle of yIHÿr•yR will ˜e IVHëF „he estim—ted

Ê en™ed neither met—som—tism nor met—morphismF yRÿr dist—n™eD IFWU eD ™losely ™oin™ides with

Ê sn™orpor—tion of light ‚ii —nd „h into —ll—nites the IFWT e o˜served in epidote @uvi™k et —lFD

o™™urs in v—rious ro™ksD h—ving geo™hemi™—l IWVVAF es shown in „—˜le IPD the yIHÿr•yR

impli™—tions for their petrogenesis @heer et —lFD —ngle ™—l™ul—ted for the present —ll—nite is

IWVTAF „he present @„—˜les TD U —nd VA —nd other estim—ted to ˜e pr—™ti™—l for the —ll—nite stru™tureF

studies @eFgF r—seg—w—D IWTHY heer et —lFD IWVTA

suggest th—t —ll—nites from the t—p—nese isl—nd —r™ ell—nite —s —n indi™—tor of te™toni™ setting

—re „hE˜e—ringF purthermoreD they ™ont—in more

„h th—n —ll—nites from the other te™toni™ settings „he present interest in —ll—nites from gr—niti™

@heer et —lFD IWVTAF ixley @IWVHA —lso reported ro™ks of the t—p—nese isl—nd —r™ origin—ted from

v—lues of up to RFVV wtF7 „hy the f—™t th—t „h is present in —ll the s—mples in —ll—nites of the P

despite the f—™t th—t no w—s dete™ted ˜y iw€eF ƒkye gr—nite of „erti—ry ™ontinent—l m—rgin

„efvi IPF gomp—risons of inter—tomi™ dist—n™es —nd —ngles for hydrogen ˜onding in epidote group miner—lsF

ipidote ipidote €iemontite ƒtrontiopiemontite

@q—˜e et —lFD IWUQA @uvi™k et —lFD IWVVA @perr—ris et —lFD IWVWA @fon—zzi et —lFD IWWHA

yIHÿr HFVW HFWV HFWU HFVW

r•yR PFHP IFWT PFHH PFIU

yIHÿyR PFWH PFWP PFWT PFWV

yIHÿr•yR IUQFU ITTFW ITVFI IRWFW

holl—seiteE@geA uhristoviteE@geA h—iss—kisiteE@geA endrositeE@v—A

@€e—™or —nd hunnD @ƒokolov— et —lFD @‚ouse —nd €e—™orD @fon—zzi et —lFD IWWTA

IWVVA IWWIA IWWQA

yIHÿr HFWT HFWI HFUU HFVV

r•yR IFVV IFWU PFIR PFHV

yIHÿyR PFVQ PFVU PFWH PFWR

yIHÿr•yR IUHFP ITWFU IUUFS ITSFW

‚iiEri™h piemontite perri—ll—niteE@geA ell—nite

@fon—zzi et —lFD IWWTA @u—rt—shov et —lFD @this studyA

PHHPA

yIHÿr HFVS HFUI HFWT @™onstr—inedA

r•yR PFIH PFIV IFWU @—ssumedA

yIHÿyR PFWR PFVW PFWQ @o˜servedA

yIHÿr•yR ITUFU IUUFQ IVHFH @™—l™ul—tedA RIW

wF ryƒrsxy i„ evF

n—tive interpret—tion of pigF W might suggest th—t originF „he present o˜serv—tion th—t —ll—nites from

the oxygen fug—™ity of gr—nites in the ™ontinent—l the t—p—nese isl—nd —r™ —re ri™h in „h gre—tly

m—rgin —re— is lower th—n th—t in the isl—nd —r™ reinfor™es the weight of rerm—nn9s @PHHPA

—re—F „he est—˜lishment of these three groups h—s ™on™lusion th—t —ll—nite h—s the potenti—l to ˜e —

impli™—tions for the different oxygen fug—™ities m—jor ™—rrier of light ‚ii —nd „h in su˜du™ted

in¯uen™ing the pe ™rust—l m—teri—lsF y ™ontent for —ll—nite ™ryst—lE P Q

„his study ™omp—res the tern—ry el liz—tionF „hereforeD su™h — dis™rimin—tion di—gr—m y Epe y E P Q P Q

is expe™ted to ˜e useful in trying to underst—nd the ƒ‚ii ™ompositions of —ll—nites in gr—niti™ ro™ks

origin of gr—niti™ m—gm—s yielding —ll—nites —nd from t—p—n with those of previously pu˜lished

trying to infer te™toni™ settings for their host d—t—D ™l—rifying the te™toni™ settings for —ll—nite

ro™ksF ™ryst—lliz—tionF w—ny —ll—nites from gr—niti™ ro™ks

were plotted in the tern—ry di—gr—m in pigF WF

ell—nites from the isl—nd —r™ zone —re plotted in

gon™lusions

one P ˜etween the ™ontinent—l m—rgin zone

@one QA —nd the intr—™ontinent—l one @one IAF f—sed on ™ryst—l ™hemistry of the present —ll—nites

„his zoning depends on different pe —nd stru™ture re®nement of the —ll—nite under the y ™ontents P Q

™onstr—int of its ™hemi™—l ™ompositionD the of —ll—nitesF sn gener—lD oxygen fug—™ities for

following ™on™lusions ™—n ˜e dr—wnX intr—™ontinent—lD isl—nd —r™ —nd ™ontinent—l m—rgin

@IA ell—nites o™™urring in the present gr—niti™ zones set the following trendF wost €roterozoi™

ro™ks from the t—p—nese isl—nd —r™ were identi®ed —norogeni™ gr—nites from erizon— —nd neighE

—s —ll—niteE@geAF ˜ouring g—liforni— —nd xev—d— @intr—™ontinent—lA

@PA qlo˜—l te™toni™ settings for —ll—nite ™ryst—lE —ppe—r to h—ve ™ryst—llized with oxygen fug—™ity

ÿISFV ÿIRFS

liz—tion —re impli™it in their pe @f A in the r—nge IH ÿIH ˜—r —t UHHëg y ™ontent

y P Q P

@enderson —nd fenderD IWVWAF yn the other h—ndD differen™esX three zones on the tern—ry el y E P Q

the f pe of gret—™eous gr—niti™ ™omplexes from y Eƒ‚ii di—gr—m signify intr—™ontinent—lD

y P Q

P

ÿIU

wyokenEz—n —nd ro˜enz—nD ƒ‡ t—p—n is IH isl—nd —r™D —nd ™ontinent—l m—rgin zones in order

of de™re—sing pe ˜—r —t UHHëg @„—k—gi —nd xurekiD IWWRY y F P Q

x—k—shim—D IWWTAF „hereforeD the division into @QA ell—nite is the import—nt host for light ‚ii

three zones in pigF W is ™onsistent with petroloE —nd „h in tr—™e element ˜udgets of su˜du™tion

gi™—l d—t— for the intr—™ontinent—l —nd isl—nd —r™ zone pro™essesF

—re—sF xeverthelessD there h—s ˜een no report @RA „wo s‚ —˜sorption ˜—nds —t QQSS —nd

ÿI

™on™erning the oxygen fug—™ity of gr—nites from QIVU ™m —nd the shift tow—rds the lower

™ontinent—l m—rgin —re—sF purthermoreD —n —lterE w—venum˜er of the ƒiyEstret™hing ˜—nd o˜served

psqFWFely Epe y Eƒ‚ii di—gr—m of —ll—nitesF „he d—shed lines indi™—te the three groups of different kinds of P Q P Q

o™™urren™e of —ll—niteF RPH

griwsƒ„‚‰ yp evvexs„i

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