American Mineralogist, Volume 63, pages l7-27, 1978

of quartzfibers'
Characters
CLrprono FnoNorI-
Department of GeologicalSciences,Haruard Uniuersity
Cambridge,Massachusetts02 138

Abstract

X-ray and piezoelectrictechniquesconfirm that the common direction of elongation of

microscopic quartz fibers is along a polar (l 120)direction. The fibers have a preferredpolar
orientation to the interfaceat which crystallizationinitiated, in which the attachedpole is that
acquiring a negativepiezoelectriccharge on axial compression.This descriptionis independ-
ent of the enantiomorph involved. The same polar orientation is shown by macroscopic
twisted quartz crystalselongatedalong [ 120]
Both quartz fibers and singlecrystalselongatedalong |1201 are twisted around this axis.
The twist senseis stereospecific: opposite to the morphological chirality of the quartz struc-
ture. The observedvaluesofthe twist period rangecontinuouslyabout 5 orders ofmagnitude,
from roughly 20 microns to over 300 cm. Both the incidenceof twisting and the twist period
appear to be temperature-dependent, the former decreasingand the latter increasingwith
increasing temperature of crystallization. Twisting is typical of fibers and rare in single
crystals.Twisting around [0001] also occurs in singlecrystalsbut is much lessfrequent than
around !1201.
Right- and left-handed twisted quartz fibers appear to be equally abundant, although
seedingeffectsmay locally give rise to a large preponderanceof one enantiomorph. Data on
27,043quartz singlecrystalsalso indicatethat the two enantiomorphsare equally abundant.
The dimensional elongation of quartz fibers and single crystals along one direction of a
three-fold symmetry-equivalentset, (1120), and the associatedstereospecifictwisting, are
ascribedto screwdislocationswith their Burgersvector along [l 120].The polar orientation is
believed to be an associatedrate-of-growtheffect deriving from different core structuresof
screw dislocationspropagatedin opposite sensesalong [120].
It is suggestedthat the general occurrenceof quartz as microscopicfibers in low-temper-
ature environments,and as macroscopiceuhedralor anhedral crystalsin higher temperature
environments,arisesin factors determiningthe incidence,density,and orientation of disloca-
tions in a quartz matrix rather than through the crystallizationkineticsof the solution itself

Introduction cilitating the study of the fibers in an experimental

Among the more common types of occurrenceof sense,this condition is essentialto the recognition of
fibrous quartz are sedimentary rocks (chert), con- fiber characterssuch as polar orientation to the site of
cretionary masses(flint), replacementand alteration nucleation and stereospecific twisting.
bodies in rocks, and varied creviceand cavity fillings
Non-centricpropertiesof quartz
such as crustiform aggregates,geodes, and agates.
The latter occurrencesgenerallypassunder the name With regard to pertinent aspectsof the crystallog-
chalcedony.What is primarily of interesthere are the raphy of quartz, the structural polarity of the two-
charactersof quartz fibers that have nucleatedfrom f o l d s y m m e t r ya x e s ,o r ( 1 1 2 0 )d i r e c t i o n s i. s m a n i -
solution at an interface,as upon a planar surfaceor fested by piezoelectriceffectsand by unlike rates of
the wall of a spheroidal cavity, to form parallel- s o l u t i o n ( M e y e r a n d P e n f i e l d ,1 8 9 0 ;G i l 1 , 1 8 9 3 )a n d
fibrous or radially-fibrousaggregates.Aside from fa- of growth (Brown et al ., 1952)in opposite senses.In
the conventional description, compression along
[1 120]producesa negativeelectrostaticchargeat that
' M i n e r a l o g i c a lc o n t r i b u t i o n n o 4 9 9 pole terminated by faces of the positive trigonal
ooo3-004x/78loI o2-00| 7so2oo t7
l8 FRONDEL, QUARTZ FIBERS

trapezohedrons,such as x {516-l} or the trigonal pyra- tion. The general effect presumably results from di-
m i d s { l 1 2 1 } ,a n d a c o r r e s p o n d i n gp o s i t i v ec h a r g ea t rected strain associatedwith the initial dislocation
the opposite pole. This descriptionis independentof ( E s h e l b y ,1 9 5 3 ;G o m e r , 1 9 5 8 )i n t h e n u c l e a rc r y s t a l
the chirality. Tension reversesthe effect.Temperature that destroys the formal crystallographic equiva-
gradientsproduce internal stressesand thus also pro- lences.
duce charges (pyroelectricity); on cooling, the
charges correspond to those of compression. The Polar orientation
rates of solution and growth as measuredon spheres Since the [ 120] direction is polar, the question
or on platescut perpendicularto [ 120]are greaterin ariseswhether there is a preferredpole of attachment
the axial direction away from the pole which becomes of the fibers to the site at which crystallizationiniti-
n e g a t i v eo n c o m p r e s s i o n . ated. In the technique used here, thin plates were
Structurally, the Si and O ions are arranged in sawn at right anglesto the fiber elongation,electrodes
special positions in the enantiomorphous space were plated on, and the piezoelectriccharges pro-
groups C3r2 and C3r2. The enantiomorphism arises duced by axial compressionwere identified. Exami-
in helical arrangementsof the Si and O ions along the nation of several hundred parallel-fibrousand radi-
[0001]direction.This arrangementand the associated ally-fibrous crusts, geodes,and agates from world-
optical activity are lost when the structure is dis- wide localitiesestablishedthat a preferredorientation
solvedor melted. The chirality of quartz as described is commonly present.The attached pole is that one
by conventional morphological and optical rotatory becoming negatively charged on compression.This
criteria is opposite to that of the crystal structure. description is independent of the quartz enan-
tiomorph involved. The same polar orientation is
Fiber elongation shown by large quartz single crystals, describedbe-
The common direction of fiber elongationas deter- y o n d , t h a t a r e e l o n g a t e da l o n g [ 1 1 2 0 ] .A n o r i e n t e d
mined by X-ray diffraction and piezoelectrictech- piezoelectricresponsewas weak or absentin many of
niquesis along one of the polar (l 120)directions.The the fibrous specimens examined, notably in cha[-
earlier X-ray work and the general literature on fi- cedony crusts from hydrothermal veins, closely
b r o u s q u a r t z a r e s u m m a r i z e d b y B r a i t s c h ( 1 9 5 7 ) . banded or deeply pigmented agates,and material in
Quartz fibers also occur elongated along the non- which the fibers have a feathery character or are in
polar [0001] direction but are rare and appear to be the submicron range of size.The angular divergence
typical of particular geochemicalenvironments(Folk of the fibers is also a factor. More or less equal
and Pittman,l97l). mixtures of fibers of opposite polarity also would be
In the formation of fibrous quartz, the direction of representedhere.
elongation as predicted by periodic bond-chain the- The microscopic fibers that constitute chert and
o r y ( H a r t m a n a n d P e r d o k , 1 9 5 5 ;H a r t m a n , 1 9 7 3 )i s flint are randomly arranged as seen in thin section.
related to chains of strong Si-O-Si bonds running Platescut from such aggregatesdid not give a piezoe-
through the crystal structure.The strongestof these lectric response. Optically the flbers generally are
chains are in the ( I 120)and [0001]directions.A prob- length-fast; they hence are elongated in the (0001)
l e m a r i s e sh e r e i n t h a t t h e ( l 1 2 0 ) d i r e c t i o n sc o m p r i s e plane, but the identity of the specificdirection therein
a three-fold symmetry-equivalentset. The growth is not known.
rates henceshould be equal in each of the equivalent The polar orientation is viewed as a rate-of-growth
directions,as shown by the equant cross-sectionnor- effect connected with the dislocations to which the
mally seen across (0001) in single crystals.The ob- fiber elongation itself is ascribed. It is believed to
serveddimensional elongation of quartz fibers along derive from the different core structure of screw dis-
one of the three equivalentdirections(hereafterdes- locations propagated in opposite sensesalong [ 120]
i g n a t e d t 1 1 2 0 1 )i s b e l i e v e dt o b e c o n t r o l l e d b y d i s - (Ashbee, 1973),resulting in different growth rates as
locations implanted during nucleation and growth. the dislocationsare emergentat oppositefiber poles.
The same feature of dimensional elongation along When the faces terminating the fibers can be dis-
one direction of a symmetry-equivalentset is shown cernedthey are found to belong to either {1010}or to
by whisker crystals (Doremus et al., 1958 Webb e/ a { 1 0 1 1 }o r { 0 l l l } r h o m b o h e d r o n I. t m a y b e n o t e d
a l . , 1 9 5 7 R i e b l i n g a n d W e b b , 1 9 5 7 )o f v a r i o u s s u b - that fibers terminated by these or other non-polar
stances, and derives from screw-dislocationswith forms, if free from dislocations,would have identical
their Burgers vector along the direction of elonga- growth ratesregardlessofthe polar senseofthe axis.
 FRONDEL,QUARTZFIBERS

Solubility control has been suggestedby Becke

( 1 8 8 9 ) a n d H o l z n e r ( 1 9 2 1 ) f o r e x a m p l e so f p o l a r
orientation in hemimorphite and other crystals.Dur-
ing the random nucleation of a polar substanceupon
an interface, those nuclei that by chance have their
greater rate-of-solutisn'polar vector suppressedby
attachment at the interface would have, in effect, a
lower bulk solubility. They henceshould nucleate
first and yield a preferred orientation. This mecha-
nism seemsunlikely in quartz, sincethe greaterpolar
rate of solution vector comprises a three-fold set.
Solubility control also has beensuggestedby Johnson
(1907) for crystals twinned by reflection across the
plane perpendicularto a polar axis. Here, as a general
rule, the polar vectors of greater rate of solution in
the twinned parts point toward the surfaceof junc-
ture. Dauphind twinning in quartz appearsto follow F i g I O p t i c a l e x t i n c t i o n b a n d i n g i n a p a r a l l e l a g g r e g a t eo f
this relation. q u a r t z f i b e r s ;c r o s s e dn i c o l s .T h e t w i s t p e r i o d i s a p p r o x i m a t e l y2 5 0
Whatever the mechanisminvolved,the polar orien- m i c r o n s . T h e f i b e r e l o n g a t i o n i s f r o m l o w e r r i g h t t o u p p e r l e f t .
tation of quartz fibers is a physical effect that is
independentof the chemical or structural nature of produced in fibers by the rotation of uniaxial and
the interface itself. In this it differs from the polar biaxial indicatrices in both twisted and helical ar-
orientation of elongate organic moleculesand long- rangements.Quartz normally is uniaxial, but some-
chain biopolymerscontaining hydrophilic and hydro- times shows an anomalous biaxial character.In such
p h o b i c s u b s t i t u e ngt r o u p sa t o p p o s i t ep o l e s .A r e v i e w i n s t a n c e sa, s e a r l i e rn o t e d b y J o n e s( 1 9 5 2 )a n d o t h e r s ,
o l t h i s s u b j e c ti s g i v e n b y T a n f o r d ( 1 9 7 3 ) .A l t h o u g h the obtuse bisectrix X is along the fiber length, with
the opposite ends of polar quartz fibers are chem- 2V variable 10" to 30o.
ically identical, their adsorptive behavior, such as The twist period in quartz fibers, based on the
with regard to (OH) and H+, may be different. measurement of several hundred examples, ranges
from about 20 to 700 microns. Longer twist periods,
Stereospecifictwisting in the mm to cm range, apparently occur, but could
not be measuredoptically either becausethe fiber was
Twisting around fl l20l in fibers too short or extended outside the area of the thin
The orderly twisting of quartz fibers was first no- section. Over 100 successivetwists have been ob-
ticed and explained optically by Michel-L6vy and servedalong a single fiber. The twist period ordinar-
M u n i e r - C h a l m a s( 1 8 9 2 ) ,a n d t h e r e a r e n u m e r o u si n - ily is uniform along the fiber length. A variation is
cidental observations in later literature. The main occasionallynoted close to the point where crystalli-
study of twisting in fibers generally, however, has zation initiated. Here the twist period may rapidly
been in connection with the so-calledbanded spheru- increase to larger values. An abrupt variation also
lites of organic high-polymers(Bernauer, 1929;Geil, has been noted at the terminal end (Fig. 2). In some
1 9 6 3 ;P r i c e , 1 9 5 9 ;K e l l e r , 1 9 5 5 ) ,a n d i n w h i s k e rc r y s - instancestwisting along the fiber length may be inter-
tals of metals and other substances. rupted by one or more untwisted zones. The twist
In parallel-fibrousand radially-fibrous quartz ag- senseof the fibers is found to be either to the right or
gregates,as examined in thin section cut parallel to left. It can be determined by the technique of Ber-
the fiber elongation,the twisting appearsin polarized nauer ( 1926),involving rotating the fiber in polarized
light as a successionof zero birefringence optical light on a universal stagein a prescribedmanner.
extinction bands extending along the fiber length The thicknessof the fibers as determined by elec-
(Fig. l). The bands representthe identity period of tron microscopy is in the range from about 0.05 to 1
the twist that brings the optic axis (at right anglesto micron in most parallel-fibrousand radially-fibrous
the fiber elongation) parallel to the microscopeaxis. aggregates.The range is somewhat smaller in chert
General treatmentshave been given by Keller (1959) and flint. The thicknessextendsup to 10 microns or
and by Keith and Padden( 1959)of the optical effects more in some hydrothermal vein fillings and crusti-
20 FRONDEL QUARTZ FIBERS

when the twist axis is held vertically'zis stereospecific.

It is always opposite to the chirality of the crystalsas
defined by their morphology. The twist period, or
length correspondingto a complete 180oturn around
[ 120], varies widely. The twist period in all of the
known instancesis greater than the actual length of
the crystal. The largest turn observed is about 50o
over a 12 cm length.
Direct measurementof the pitch of 228 crystals
examined in various museum collections are in the
range from 8.5o to 0.50o per cm. Thesevaluescorre-
spond to calculated twist periods of 21 to 360 cm.
Values in this range also have been reported in the
Fig 2. Optical extinction banding with a twist period of 140 literature. Some crystals apparently have twist peri-
m i c r o n s ( l e f t ) , a t e r m i n a l z o n e o f l a r g e r t w i s t p e r i o d ( c e n t e r ) ,a n d ods extending to 500 cm or more, but the measure-
t h e f i n a l d e p o s i t i o n o f a m o s a i c o f q u a r t z c r y s t a l s( r i g h t ) ; c r o s s e d
ment of very small pitches by optical goniometry
nicols Growth direction left to risht
becomesuncertain becauseof surfaceirregularities.
Twisted single crystals occur as euhedral individ-
form types formed at relatively high temperatures. uals, more or lesselongatedalong [ 120],that project
The twist period tends to increasewith increasing from the walls of an opening (Fig. 3). They usually
fiber thickness although, as noted beyond, the pri- have a smoky color. The pole of attachment almost
mary control appearsto be the temperatureof crys- always can be identifiedvisually from morphological
tallization. features, and corresponds to that pole acquiring a
The fiber length ranges up to severalcm in some negative piezoelectriccharge on axial compression
geodesand agates.The individual fibers usually are (Fig. a). This orientation also has been identified by
grouped into bundles from a few microns to over 50 L e m m l e i n ( 1 9 3 7 ) . l t i s i d e n t i c a lw i t h t h e p o l a r o r i e n -
microns in thickness. Occasionally the bundles ap- tation of quaftz fibers elongatedalong [120].
pear to be helically twisted on a coarse scale. This
'A different convention has been used by some authors, in
f e a t u r ea l s o h a s b e e n n o t e d b y R e i s ( 1 9 1 6 ) .
w h i c h t h e s e e m i n gd i r e c t i o n o f r o t a t i o n o f t h e t e r m i n a l p r i s m e d g e ,
The zig-zag appearance of the twist extinction a s s e e nw h e n t h e c r y s t a l i s v i e w e d a l o n g t h e p o l a r 1 2 0 ]a x i s w i t h
Il
bands is mainly causedby a slight angular divergence t h e p o s i t i v e - o n - c o m p r e s s i opno l e i n f r o n t , i s d e s c r i b e da s c l o c k w i s e
or a slight lengthwisedisplacementbetweenadjacent o r c o u n t e r c l o c k w i s e A c l o c k w i s e t u r n c o r r e s p o n d s t o a l e f t -
fiber bundles. If these differencesare large, the twist handedaxial twist
extinction has a mosaic or blotchy appearanceor it
may be obliterated. Identical featuresare shown by
the banded spherulitesof organic high-polymers.The
twist extinction bands are relativelypoorly developed
in crustiform types from hydrothermal veins, and
generally are not observedin the individual fibers of
random or featheryaggregates.It is difficult to decide
in many instanceswhether twisting is absent or if it
has been obscured. In any case, twisting is a very
common character of quartz fibers elongated along
I r r2 0 ] .
Twisting around ft I20l in single crystals
Large twisted quartz crystalswere first noticed by
Weiss (1836) and there are numerous later descrip-
t i o n s , n o t a b l y b y T s c h e r m a k( 1 8 9 4 ) ,R o s i c k j '( 1 9 3 3 ) ,
F r i e d l a e n d e r( 1 9 5 1 ) ,a n d L e m m l e i n ( 1 9 3 6 ,1 9 3 7 ) .I n Fig. 3. Twisted single crystal Closed type. Right-handed
large quartz single crystals, the sense of the twist q u a r t z , l e f t - h a n d e dt w i s t . S w i t z e r l a n d C r y s t a l a b o u t 5 c m l o n g .
around [1120], to the right or left, viewed as a screw Attached oole to left.
 FRONDEL QUARTZ FIBERS 2l

The terminal prism edgeat the free end often has a

slight S-shapedinflection to the right or left in the
same senseas the twist. Trigonal trapezohedralfaces Screw
sense
usually are present and are of relatively large size.
The perfection of the crystals varies considerably.
'\ f

;\,
The surfaces of some are smooth and continuous
z
(Tschermak's closed type); other crystals are com-
posite, and composed of partly merged individuals
(open type). In thin section the most perfect crystals
r),ro.. I
show undulose extinction, and afford X-ray single F i g 4 S c h e m a t i cd r a w i n g s h o w i n g t h e r e l a t i o n b e t w e e nt w i s t
crystal photographs with uniformly stretched-outre- s e n s e ,h a n d a n d p o l a r a t t a c h m e n t i n q u a r t z s i n g l e c r y s t a l s a n d
fibers elongatedalong [120] The free end is that acquiring a
flections.As with the fibers,there is a rough tendency
positive piezoelectric charge on axial compression.
for the twist period to increasewith increasingcrystal M o r p h o l o g i c a l l y r i g h t - h a n d e dc r y s t a l .T h e t w i s t s e n s ei s r e v e r s e d
size. Most of the known occurrencesare in hydro- i n a l e f t - h a n d e dc r y s t a l .
thermal quartz veins, cavity deposits of the Alpine
type, and pegmatites. cavity fillings formed in rhyolitic flows and welded
tuffs and in basaltic flows, gash veins in sandstone
Twisting around [0001] and quartzites,cavity and vein fillings ofthe so-called
Quartz fibers elongatedalong [0001]are rare. They Alpine type, quartz veinscontaining silicatesand sul-
can be identifiedoptically (length-slow),but the pres- fidic minerals of moderate to high temperatureaffili-
ence of twisting around [0001] cannot be recognized ations, pegmatites,and miarolitic cavitiesin granitic
optically in the uniaxial case. A few instances of rocks. In a general way, the twist period and the
twisting around [0001] in large single crystals have crystal size increase and the incidence of twisting
b e e n n o t e d b y T s c h e r m a k( 1 8 9 4 ) , L e m m l e i n ( 1 9 3 6 , decreasesin the order given. The range of temper-
1937), Frondel (1936, 1962), and Sadanaga and ature representedfor the crystallizationof the quartz
Bunno (1974\.Ten additional instanceswere found in in these occurrencesis conjectural. Study of liquid
the course of the present study. The twist sensehas inclusions in the twisted crystalswould be informa-
been reported as in the same senseor the opposite tive of the actual temperatureof crystallization.
senseas the morphological hand. Nearly all instances It is not known if the twist period is a linear or
are of the latter type. Identification of the twist sense more complex function of temperature,or if the rela-
sometimesis ambiguous becauseof the presenceof tion is directly with the temperature or with some
twinning. The twist period, in terms of a 120' turn, is characterof the crystallizingsolution that is temper-
variable. In the specimensexamined here it ranged ature dependent.
from about 54 to 800 cm. The maximum turn ob- There is also a marked variation in the incidenceof
served was about 45o over a length of 2l cm. The twisting around [1 120] over the observed range of
occurrencesare all from high temperature environ- temperature. Twisting is quite general in fibrous
ments. The crystals usually are relatively elongate quartz formed at low temperaturesand is quite un-
along [0001]. common in crystals formed at higher temperatures.
Probably less than 1500 examples of twisted single
Origin crystals are preserved in Museum collections. The
The [1120] twist period in fibers and singlecrystals twisted single crystals occur as isolated individuals
varies continuously from about 20 microns to over associatedwith quartz crystalsof normal habit elon-
300 cm. There is a small gap in this range,from a few gated along [0001] and of contemporaneousforma-
cm up to about 20 cm, in which only a few doubtful tion. Single crystals twisted around [0001] are ex-
measurementsare available.On either side there are tremely rare-probably less than 50 examples are
several hundred measurementsthat are rather uni- known-and seem to be typical of crystallizationat
formly distributed. high temperatures.
The types of occurrenceinclude geodalconcretions The twisting of quartz is believed to derive from
and crusts produced in the meteoric circulation and screwdislocationswith their Burgersvector along the
by weatheringprocesses, cavity fillings formed during direction of elongation and twisting. The primary slip
the chloritic and zeolitic stagesof post-magmatichy- systemsin quartz have Burgers vectors along (1120),
drothermal action in basic igneous flow rocks, gas [ 0 0 0 1 ] ,a n d ( l 1 2 0 ) + [ 0 0 0 1 ] .T h e y h a v e b e e ni n v e s t i -
22 FRONDEL QUARTZ FIBERS

, n d L e m m l e i n( 1 9 3 6 ,
B i l l o w s ( 1 9 0 9 ) ,R o s i c k j ' ( 1 9 3 3 ) a
1937), but the observed relation is very crude. It is
often found, for example,that separatecrystalsof the
same thickness or overall dimensions will vary in
twist period by a factor of 2 or more. The degreeof
supersaturationseemsa more likely control for both
the crystal size and the twist period. It influencesthe
rate of nucleation, or ultimate averagecrystal size,
and as found by Kozlovskii (1962) the step height of
screw dislocations increaseswith decreasingsuper-
saturatlon.

Fiber enantiomorphism
F i g . 5 P e r i o d i c s t r i a t i o n s i n a p a r a l l e l a g g r e g a t eo f t w i s t e d
quartz fibers. Striation spacing approximately 2.4 mrcrons.
If the nucleation of quartz as right or left enan-
C r o s s e dn i c o l s , s h o w i n g o p t i c a l e x t i n c t i o n b a n d i n g .tiomorphs is a matter of chance,the two enantiom-
rophs should be equally frequent.This appearsto be
gated especiallyin connection with the plastic defor- the case.The chirality of 27,043large quartz crystals
mation of quartz at elevatedtemperaturesand pres- has been determined by morphological, optical ro-
s u r e s( C h r i s t i ee t q \ . , 1 9 6 4 ;C h r i s t i ea n d G r e e n , 1 9 6 4 : tatory, or etching techniques:13,481are left-handed
B a E t aa n d A s h b e e ,1 9 6 9 ;M c l a r e n e t a I . , 1 9 6 7 :M i u s - and 13,5'72are right-handed. The data have been
k o v e t a | . , 1 9 1 1 ) . T h e s l i p v e c t o r sa r e i n f l u e n c e db y drawn from studies by Gross (1972), Lemmlein
temperatureand the presenceof water in the quartz (1944), Heritsch (1952), Bussiereand Maisonneuve
s t r u c t u r e( B l a c i c , 1 9 7 4 ) . ( 1 9 7 1 ) ,C . S . H u r l b u t ( p r i v a t ec o m m u n i c a t i o n ,1 5 4 9
A structural model for the propagation of screw left- and 1551right-handed),and other sourcescited
d i s l o c a t i o n sa l o n g [ 1 1 2 0 ]h a s b e e nd e s c r i b e db y A s h - by Frondel (1962). Becauseof presumedseedingef-
b e e ( 1 9 7 3 ) . T h e p a r t i c u l a r o r i e n t a t i o n a n d s t e r e o - fects some local quartz populations in igneousrocks
specificrelation taken by the screw dislocations in- are predominantly right or left (Heritsch, 1952;Bus-
volves choices (as described for morphologically s i e r ea n d M a i s o n n e u v e ,l 9 7 l ) . O f 3 0 1 s i n g l ec r y s t a l s
right-handed quartz) between the rectangular and t w i s t e d a r o u n d [ 1 1 2 0 ] f o r w h i c h d a t a a r e a v a i l a b l e ,
h e x a g o n a lc h a n n e l sa l o n g [ 1 2 0 ] , d e f i n e d b y r i g h t - 1 4 9w e r e l e f t - a n d 1 5 2r i g h t - h a n d e d .
handed and left-handed helicesof (SiO,) tetrahedra It is found that most aggregatesof twisted fibers
respectively,and the triangular and hexagonalchan- are more or less equal mixtures of the two enan-
nels along [0001], defined by left-handed and right- tiomorphs. In some instances, however, sizeable
handed helicesrespectively.The energeticsinvolved areasof fibrous geodesand agates,as seenin section,
include the sign of the Burgers vector along [ 120]. are all of the same hand, right or left. Occasionally
Whisker crystals of centrosymmetric substances theseobjectsapparentlyare wholly of the samehand.
show twisting to the right or the left dependingon the
c h a n c es e n s eo f t h e i n i t i a l d i s l o c a t i o n .T h e s e n s eo f
the twist or stressfield produced is opposite to the
screw senseof the controlling dislocation.In twisted
whisker crystalsthe twist period has beenobservedto
vary from small to immeasureablylarge valuesin the
same substance.Featuressuch as the temporary ces-
sation of twisting along the whisker axis, such as seen
in quartz fibers, also have been observed.
The twisting of whisker crystals and of planar or-
ganic spherulitefibers apparentlyis primarily a func-
t i o n o f t e m p e r a t u i e( G e i l , 1 9 6 3 ;K e l l e r , 1 9 5 9 ) , a l -
though fiber or crystal thickness and the degree of
supersaturation have been discussed in this con-
nection. A relation between crystal size and twist
period in quartz single crystals has been sought by Fig 6 Samefield as Fig. 5, in ordinary light.
 FRONDEL: OUART-Z FIBERS z-)

A sectoral distribution of enantiomorphs has been

observed in some planar organic spherulites(Keith
a n d P a d d e n ,1 9 5 9 ) .

Periodic fiber striations

A poorly understood feature occasionallyseenin
qvartz fibers is a uniformly spacedseriesof striations
at right angles to the elongation of the fiber aggre-
gates.The striationsand the associatedoptical effects
w e r e f i r s t d e s c r i b e db y J o n e s( 1 9 5 2 ) .T h e s t r i a t i o n s
appear dark in both ordinary and polarized light
(Figs. 5 and 6). A similar effecthas been describedby
K e i t h a n d P a d d e n ( 1 9 5 8 ) i n s p h e r u l i t e so f o r g a n i c
high-polymers. Fig 7. Periodic striations showing a complex sequence
The striationsapparentlyrepresentinternal bound- (. . .DDFFFFDDFFFFDD ) . S t r i a t i o n s p a c i n g2 . 2 m i c r o n s .
aries of different optical density at which light is in
part scatteredand totally reflectedand acrosswhich tions and the twist period. The ratio of the two was
c r y s t a l l o g r a p h i cc o n t i n u i t y i s m a i n t a i n e d . W h a t i s found to vary betweenabout 30 to I and 120 to I in
seenis the optical effect and not the boundary itself. about 30 measuredexamplesfrom various localities.
Examination by both transmissionand scanningelec- In some but not all instances,gaps in the striation
tron microscopy and, in the caseof very broad stria- sequenceare accompaniedby gaps in the twisting.
tions, by optical microscopy does not clearly indicate The feature has been observedonly in closed sys-
t h e n a t u r e o f t h e b o u n d a r i e s .M i n u t e i n c l u s i o n so f tems, that is, where fibrous quartz has beendeposited
f o r e i g n m a l . e r i aal r e s e e ni n s o m e i n s t a n c e s . by solutions infiltrating closed cavitiesto form radi-
The spacingof the striationsusually is about I to 3 ally-fibrous geodes or agates.As with the twist ex-
microns, but ranges down to the limit of optical tinction bands, the striations have a zig-zag appear-
r e s o l u t i o na n d u p w a r d s t o 1 0 0 m i c r o n s o r m o r e . I t ance when traced across adjoining fibers or fiber
often is constant over long sequences. In one instance bundles and have proportionally the same off-set.
over 8,000successive striationsspacedapproximately The uniformity of the spacingover long sequences
2 microns apart were observed.When the fiber length would seem to preclude periodic variation in some
is in the plane of a relatively thick section the regu- gross character of the solution, such as temperature
larly spaced striations act as optical phase gratings or pH, that is recordedon the fibers.Fiber participa-
and produce strongly polarized diffraction colors in tion must be involved to the extent of modulating
transmitted light (Raman and Jayaraman, 1953, some external factor. Possiblypyroelectricchargesat
1 9 5 5 ;J a y a r a m a n ,1 9 5 3 ) .S o - c a l l e di r i s a g a t ei s o f t h i s the growing tips of the fibers, generatedby thermal
nature. The effect is diminished and the striations strain attendingdiffusion ofthe latent heat ofcrystal-
appeardiffusewith increasinginclination of the fibers lization away from the interface,have influencedthe
to the plane of the section. The striations also may growth mechanism.Rapid growth under non-equilib-
appear bordered by a bright line, dependingon their rium conditionswould then seemrequisite.Torsional
a t t i t u d ea n d t h e m a n n e r o f i l l u m i n a t i o n . strain associatedwith screw-dislocationsalso might
The optical density or apparent width of the stria- excite piezoelectriccharges. Periodic interaction of
tions is a function of the scattering power of the growing fiber tips charged by adsorptive processes
b o u n d a r y .I t u s u a l l yi s q u i t e c o n s t a n t ,b u t s o m e t i m e s with oppositely-chargedcolloidal particlesof foreign
varies without changing the center-to-centerspacing material in the solution, such as hydrous iron oxide,
of the striations. A lengthy sequencemay then in- is another possibility.
volve orderly alternations of dark (D) and faint (F) Etched sectionsof quartz single crystalsoccasion-
striations such as DFDF ally show irregularly spacedsequences of thin growth
DFFFDFFFD..., or ...DDFFFFDDFFFFDD... bands that differ in their content of (OH) and in their
(Fig. 7). Sequencesalso may be interrupted by gaps, indices of refraction (Bambauer, l96l; Bambauer el
the gaps either uniformly spaced or varying in size al.,1961; Kats, 1962',Bambauer et a|.,1969). Infrared
along the fiber length. In twisted fibers there is no a n d t h e r m a ls t u d i e so f c h a l c e d o n y( P e l t o ,1 9 5 6 ; B r u n -
apparent relation between the spacing of the stria- ner et al.. 1959)show that the small amountsof water
 FRONDEL: QUARTZ FIBERS

Examination under the microscopeof thin sections

cut acrossthe interface of inwardly radial aggregates
(chieflygeodesand agates)and parallel-fibrouscrusts
shows that crystallizationgenerallybeginsnot as iso-
lated fibers, although this sometimesappears to be
the case, but as minute, hemispherical,divergently
fibrous spherulitesscatteredover the interface (Fig.
8). As the spherulitesgrow in size they abut and
interfere laterally, with those fibers more nearly per-
pendicular to the interfacesurviving competition. At
a planar interfacethe end result is a crust offibers in
approximately parallel array perpendicularto the in-
terface(Fig. 9,A, B). In the spheroidalcasethe fibers
F i g 8 S p h e r u l i t e sa t a n i n t e r f a c e ,s h o w i n g a b a n d o f i n c l u d e d becomeradial (Fig. 9C). In neither casedoesthe final
Ibreign material. Crossed nicols, showing one isogyre of the arrangement resemble a spherulite, especially in
s p h e r u l i t i cc r o s s F i e l d w i d t h 4 0 0 m i c r o n s .
agateswith a central cavity, but the processof nucle-
generallypresentinclude (OH), together with molec- ation is spherulitic.
ular water, although the site or sites in which it is In the spheroidal case,the surfacesofjuncture of
located are uncertain. Zoning in terms of (OH) con- adjoining spherulitesalso convergeinwardly, often in
tent along the fiber length thus also comes into ques- complex patterns,as seenin cross-section, depending
tion here. on the actual shapeof the cavity and the number and
Periodic phenomena also appear in single crystals arrangementof the sites of nucleation (Figs. l0 and
of the amethyst variety of quartz. Here alternating I l). This gives rise to the turtleback structureseenin
bands of right- and left-handedquartz twinned on the
Brazil law, of uniform thicknessin the micron range
of size,extend over long sequences. Sincethe striated
fibers are found to have a uniform piezoelectricre-
sponse, the suggestion that they are polysynthetic
twins on the Japan law (Raman and Jayaraman,
1955)or on the Dauphin6 or Brazil laws can not
apply. These laws reversethe polarity in the succes-
s i v ep a r t s a l o n g [ 1 2 0 ] .

Fiber aggregates
In the manifold varietiesof fibrous quartz the two
main modes of aggregation are either random or
spherulitic. Random orientation of essentiallyiso-
lated fibers is characteristic of chert and flint, al-
though some degree of organiza'i.ionaround the site
of nucleation is shown by the occurrenceof sheaf-
l i k e , f a n - l i k e ,s u b - r a d i a l a
, n d o c c a s i o n a l l ys p h e r u l i t i c
forms. In fibrous quaftz aggregatesthat have formed
by crystallization from solution at an interface, the
fiber organizationgenerallyis not random. The three
casescommonly observedare, in idealizedform: nu-
cleation at a single point on the interface, usually
giving rise to a hemispherical, divergently-fibrous
spherulite; nucleation at many points on a planar
interface, usually affording a parallel-fibrouscrust;
and nucleation at many points on the walls of a F i g 9 D i a g r a m s i l l u s t r a t i n gt h e f o r m a t i o n o f a p a r a l l e l - f i b r o u s
spheroidal cavity, usually forming an inwardly con- crust at a planar surface (A, B) and of an inwardly-convergent
vergent radial aggregate. f i b r o u s a r r a y i n a s p h e r o i d a lc a v i t y ( C ) .
 FRONDEL'QUARTZ FIBERS 25

cross-sectionsof some agates.When distinct twist

e x t i n c t i o nb a n d s a n d p e r i o d i c s t r i a t i o n sa r e p r e s e n t
t h e y a r e c o n t i n u o u st h r o u g h o u t t h e v a r i o u s s e c t o r s
( F i g . l 2 ) . I n i t i a l l y t h e y a r e c o n c e n t r i ca r o u n d t h e
various sites of spherulitic nucleation, but as growth
c o n t i n u e st h e y u l t i m a t e l ya p p e a ra s s h e l l sc o n c e n t r i c
to the walls of the cavity. The degreeto which these
featuresare, so to speak,in phasein adjoining sectors
or fiber bundles,giving a more or lesszig-zagappear-
a n c e ,m u s t d e p e n do n t h e t i m i n g i n t h e f o r m a t i o n o f
t h e i n i t i a l s p h e r u l i t e sI.f t h e f i b e r si n a d j o i n i n gs e c t o r s
are inclined at differentanglesto the plane of the thin
s e c t i o nt h e c o n t i n u i t y o f t h e t w i s t b a n d s i s b r o k e n ,
and at large angular differencesthey may seem to F i g . I I S p h e r u l i t e s e c t o r ss h o w i n g b a n d s o f i n c l u d e d f o r e i g n
stop at the boundary. Sometimesfinely disseminated m a t e r i a l , c r o s s e dn i c o l s . F i e l d w i d t h 7 0 0 m i c r o n s .

foreign material becomesincluded during the growth

of the fibers, giving thin pigmented bands that serve microscopic fibers to coarse euhedral crystalsin the
a s m a r k e r h o r i z o n s( F i g s . 8 a n d l l ) . I t s h o u l d b e final stageof cavity filling has been attributed to the
added that agateshave many additional features,not final influx of solutions at a much higher temper-
wholly relevantto the presentmatters,such as succes- a t u r e .I t s e e m si m p r o b a b l et h a t t h i s s h o u l d b e a g e n -
sive generationsor bands offibers not in crystallogra- eral condition. It can hardly apply to occurrences
p h i c c o n t i n u i t yw i t h o t h e r b a n d s . such as the crystal-linedfibrous geodesfound in the
T a m p a f o r m a t i o n i n F l o r i d a ( L u n d , 1 9 6 0 )t h a t h a v e
Quartz crystals in geodesand agates formed at very shallow depths in the ground water
A quite general feature of fibrous-quartz cavity c i r c u l a t i o n .A c h a n g ei n a p a r a m e t e ro f t h e s o l u t i o n
fillings, found in all types of occurrence,is the pres- such as degreeof supersaturation,rather than tem-
ence of a central opening that is crusted by or filled perature, seems more likely. The observations of
with macroscopicquartz crystals.Thb crystalsrange Oehler (1914) on the hydrothermal crystallizationof
up to a cm or more in size and are characterizedby silica gel initially into fibers and then to euhedral
the small developmentor absenceof prism facesand c r y s t a l ss u p p o r t st h i s v t e w .
t h e d o m i n a n c eo f { l 0 l 1 } o v e r { 0 1I 1 } . A l t h o u g h s e e d - T h i s m a t t e r p o i n t s u p a m o r e g e n e r a lq u e s t i o n .
i n g b y t h e [ 1 1 2 0 ]f i b e r si s s o m e t i m e so b s e r v e di n t h i n Quartz tends to crystallizein low-temperatureenvi-
s e c t i o n s ,a f e a t u r e a l s o n o t e d b y L e m m l e i n ( 1 9 4 6 ) , ronments as microscopic fibers, to form chert, flint,
the large crystalsare generallyrandomly arrangedor and the varied forms of chalcedony, and in high-
have [0001] essentiallyradial. The transition from temperature environments to form macroscopiceu-
hedral or anhedralsinglecrystals.Two differentchar-

F i g . l 0 I n t e r s e c t i o no f t h r e e s p h e r u l i t i cs e c t o r si n a n a g a t e T h e
t w i s t e d I i b e r si n t h e t h r e e s e c t o r sa r e a t d i f f e r e n ta n g l e st o t h e p l a n e Fig l2 Periodic striations crossing a spherulite sector
o f t h e s e c t i o n .c r o s s e dn i c o l s . F i e l d w i d t h 7 0 0 m i c r o n s b o u n d a r y . S t r i a t i o n s p a c i n g3 m i c r o n s . O r d i n a r y l i g h t .
 zo FRONDEL QUARTZ FIBERS

acters are involved. One is the differencein size, to B l a c i c , J D ( 1 9 7 5 ) P l a s t i c m e c h a n i s m si n q u a r t z : t h e e f f e c t o f

which attention usually is drawn, and the other is w aler. Tectonophysics, 27, 27 | -292
crystallographic.The latter comprisethe dimensional B r a i t s c h ,O ( 1 9 5 7 )U b e r d i e n a t i i r l i c h e nF a s e r -u n d A g g r e g a t i o n s -
t y p e n b e i m S i o r , i h r e V e r w a c h s u n g s f o r m e nR , ichtungsstatistik
e l o n g a t i o na l o n go n e d i r e c t i o no f a s y m m e t r y - e q u i v a -
und Doppelbrechung Beitr. Mineral. Petrogr., 5, 331-372.
lent set to form a fiber in the first place, the polar Brown, C S., R. C Kell, L. A Thomas, N. Wooster and W. A
orientation, and the general occurrence of stereo- W o o s t e r ( 1 9 5 2 ) T h e g r o w t h a n d p r o p e r t i e so f l a r g e c r y s t a l s o f
specifictwisting. Thesefeaturesindicatethe pervasive synthetic quartz Mineral Mag , 29,858-874
role of dislocationsin the fibers.The spheruliticman- Brunner, G O, H Wondratschekand F Laves (1959)Uber die
Uftrarotabsorption des Quarzes. NaturwissenschaJien, 24, 661.
ner of crystallizationof the fibers, to the extent that
B u s s i e r e ,P a n d J M a i s o n n e u v e ( 1 9 7 1 ) R e p a r t i t i o n d e s v a r i e t e s
this derives from imperfectionsin the initial crystal e n a n t r o m o r p h e sd u q u a r t z d a n s l e s g r a n i t e sd e l a T e f e d e s t ,A l -
n u c l e u s ,a l s o m a y b e c o n t r o l l e db y d i s l o c a t i o n sT. h e gerie Trau. Lab. Gbol Mineral , Uniu Clermont Ferrand, 18,
u n l i k e m o d e s o f c r y s t a l l i z a t i o ni n t h e t w o t e m p e r - t-24
ature regimes may arise in factors determining the C h r i s t i e , J M . a n d H . W . G r e e n ( 1 9 6 4 ) S e v e r a ln e w s l i p m e c h a -
nisms in quaftz. Trans Am Geophys Union,45, lO3
i n c i d e n c e d, e n s i t y ,a n d o r i e n t a t i o no f d i s l o c a t i o n si n _, D . T . G r i g g s a n d N . L . C a r t e r ( 1 9 6 4 ) E x p e r i m e n t a le v i _
a quartz matrix, rather than wholly through the crys- d e n c eo f b a s a l s l i p i n q u a r t z . J G e o l , 7 2 , 7 3 4 - 7 5 6
tallization kinetics of the solution itself. Doremus, R. H , B. W. Roberts and D Turnbull (1958) Growth
and PerJectionof Crystals. Wiley, New York.
Acknowledgments E s h e l b y , J . D . ( 1 9 5 3 ) S c r e w d i s l o c a t i o n si n t h i n r o d s . J A p p l
A c c e s st o s t u d y m a t e r i a l w a s k i n d l y f a c i l i t a t e db y P e t e r E m b r e y Phys , 24, 176-179
and A A Moss of the British Museum (Natural History), Paul F o l k , R L a n d J S . P i t t m a n ( 1 9 7 1 ) L e n g t h - s l o w c h a l c e d o n y :a
D e s a u t e l so f t h e S m i t h s o n i a n I n s t i t u t i o n . V i n c e n t M a n s o n o f t h e new testament for vanished evaporites J. Sed. Petrol., 41,
A m e r i c a n M u s e u m o f N a t u r a l H i s t o r y , H . A . S t a l d e ro f t h e N a t u - I045-I 058
r a l H i s t o r y M u s e u m , B e r n e ,a n d E r i c W e l i n o f t h e N a t u r a l H i s t o r y F r i e d l a e n d e r ,C ( 1 9 5 1 ) U n t e r s u c h u n g i i b e r d i e E i g n u n g A l p i n e r
Museum, Stockholm. Peter Keller of the Los Angeles County Quarze fiir piezoelektrische Zwecke Beitr. Geol. Schweiz,
M u s e u m a n d E r l e C o l l i n s , S a n F r a n c i s c o ,s u p p l i e d m a n y a g a t e Ceotechn,Serie, 29, l-98.
s p e c i m e n sM u c h o f t h e m a t e r i a l e x a m i n e dc a m e f r o m t h e H a r v a r d F r o n d e l , C ( 1 9 3 6 ) T w i s t e d c r y s t a l so f p y r i t e a n d s m o k y q u a r t z
University Mineralogical Museum. Appreciation also is expressed Am Museum Nat Hist , NoDitates, no 829
to Harold Thompson and Maurice Campot of the Department of - (1962) Silica Minerals, Dana's System of Mineralogy, Yol.
C e o l o g i c a l S c i e n c e sH , arvard University, for aid in the prepara- 3. Wiley, New York
t i o n o f t h i n s e c t i o n sa n d i n m a k i n g p i e z o e l e c t r i cm e a s u r e m e n t s Geif , P H. (1963) Polymer Single Crystals. Wiley-lnterscience,
S t e v e nR i c h a r d s o no f t h e S m i t h s o n i a nA s t r o p h y s i c a lO b s e r v a t o r y , New York
Cambridge, contributed to the X-ray studies.The writer is in- G i l l , A . C . ( 1 8 9 3 ) B e i t r i i g ez u r K e n n t n i s s d e s Q u a r z e s .Z . K r i s t a l -
d e b t e d t o J o h n M . C h r i s t i e ,U n i v e r s i t y o f C a l i f o r n i a , L o s A n g e l e s , logr., 22, 91-128
I b r d i s c u s s i o n so f d i s l o c a t i o n t h e o r y G o m e r , R ( 1 9 5 8 ) F i e l d e m i s s i o nf r o m m e r c u r y w h i s k e r s .J C h e m
Phys , 28,457-464
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