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B. Mroz et al- Elastic properties of Rb4LiH3(SO4)4 and K4LiH3(SO4)4 crystals

B. Mroz et al- Elastic properties of Rb4LiH3(SO4)4 and K4LiH3(SO4)4 crystals

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r.Phys.:Condens,Matter3(1991)5673-5684.PrintedintheUK
ElasticpropertiesofRb
4
LiH
3
(S04)4
andKaLiHlS0
4
)4
crystals
BMroz+,HKieftet,M
J
Clouterz
and
J
ATuszyriskij
.;.InstituteofPhysics.AMickiewiczUniversity,Grunwaldzka6.
6O-78U
Poznan.Poland
t
DepartmentofPhysics.MemorialUniversityofNewfoundland,SI.John's,Newfoundland.AlB3X7.Canada
*
DepartmentotPhysics.UniversityofAlberta,Edmonton.Alberta.T6G2J1.CanadaReceived3December1990,infinalform2April1991Abstract.High-resolutionBrillouinspectroscopywasusedtostudytheelasticpropertiesofRh"LiH,(SO~)+andK~LiH>(SO~)+crystals.Incontrasttoearlierstudiesoftheformercompound.thepresentresultsindicatethatthefcrroclasricphasetransition,whichoccursatapproximately115K,isofthe4_.2typeratherthan
4mm
---7
mm2
aspreviouslybelieved.Anappropriatetheoreticalmodelusingatwo-componentorderparameterfreeenergyexpansionhasbeenpresentedbasedontheLandautheory.K+LiH.,(SO+)~doesnotappear
to
beferroelasticinthetemperaturerangeexaminedandonlyexhibitsaslightchangeinslopeofthetemperatureplotsforelasticconstantsassociatedwithlongitudinalphonons.
1.Introduction
CrystalswiththegeneralformulaA4LiH
3
(B0
4
k
whereA
=
RborKandB0
4
=
S04orSe04,showtetragonalsymmetryatroomtemperatureandinmostofthecasesundergostructuralphasetransitions(Krajewski
eta/1988,
MingeandKrajewski1988,MrozandLaiho1989,PolomskaandSmutny1989).Fromrecentresults,itisknownthatRb4LiHj(S04)~
(RLHS)
undergoesafcrroelasticphasetransitionatabout130K.TheformulaforthiscrystalwasreportedbyWolejko
et
a/
(1988)andMroz
et
at
(19S8,1989a)asLiRbs(SO~)21.5H
2
S0
4;
however,recentchemicalanalyseshaveledtoitsnewformulaRb
4
LiH,(S04)4forwhichabetterfitofthemeasureddensityvaluetothatcalculatedfromthex-raystudieshasbeenobtained.Theferroclasticpropertiesweremanifestedbytheexistenceofadomainstructuresensitivetomechanicalstressandbytheacousticphononsofteningobservedinde-pendentlyinstudiesoftheelasticproperties,ofthiscrystal,bytheseriesimpedancemethod(Wolejko
eta/1988)
andbytheBrillouinscatteringtechnique(Mroz
etal1988,
1989a).Fromtheresultsoftheseinvestigations,theobservedphasetransitiontypeappearstobe
4mm
-?
mm2.
ItwasalsodemonstratedbyMroz
etal
(1989a)thatthecouplingterm,involvingthespontaneousstrainandthepolarization,appearstoexplaintheobservedincompletesofteningofthe
CflIi
elasticconstantduringthispseudo-propertransition.X-rayinvestigationscarriedoutbyPietruszkaantiLukaszewicz(1988),ontheotherhand,showedthe
RLHS
crystaltohavethesymmetryofthepointgroup4(spacegroups
0953-R9R4!91!305673
+
12$03.50
©
1991TOPPublishingLtd
5673
 
5674B
Mroz
etal
P4
1
orP4
3),
atroomtemperature.Forsuchaprototypesymmetry,thetheoryofferroelasticsecond-orderphasetransitions(Toledano
etal
1983)requiresthatthelow-temperaturephasebymonoclinic2.Atthesametime,however,PietraszkoandLukaszewicz(1988)suggestthepresenceoforthorhombicdistortioninthelow-tem-peraturephase.Veryrecentresults,fromx-rayinvestigations(Zuniga
eta/1990),
showthat
RLHS
isbuiltupoflayerscharacterizedbyoppositesignsinopticalactivityandbelongingtothespacegroupsP4
1
andP4
3
Consequently,althoughthemorereliablex-rayresultsareinconsistentwiththeoryandotherpreviousworkdiscussedabove(especiallythoseconcerningthelow-tem-peraturephase),thestructuraltransitionsequence4
--,0
2willbeassumedintheprsentpaper.SuchaphasetransitionmodelalsoappliedtoK4LiH3(S04)4
(KI.HS)
whichisisomorphousto
RLHS.
Elasticpropertiesof
KLHS
werestudiedusingtheseriesimpedancemethodandtheBrillouinscatteringtechnique(Mr6zandLaiho1989).Theseinves-tigations.however,didnotrevealcompleteacousticphononsoftening.
It
wasfoundthatthetemperaturedependenceoftheBrillouinshiftsrelatedtothelongitudinalphononsexhibitedonlychangesintheirslopeat
To
=
115K.Due
to
ahighlevelofnoise.itwasnotpossibletoobserveanytemperaturechangesinthevelocitiesoftransversephonons,whichcouldbedirectlyrelatedtoaposiblesoftacousticmode.Thus,theaimhereistoreexaminethepreviousBrillouinscatteringresults(Mroz
et
at
1988.1989a)in
RLHS
usingthenewlypostulatedphasesequence4
--,0
2.Suchatransitionshouldbeaccompaniedbytheappearanceofasoftacousticmodeofamorecomplicatedform(Boccara19(4)incomparisonwiththe
C66
elasticconstant(inthecaseof
4mm
--,0
mm2).
The4
--,0
2transitionalsoinvolvessomechangesinthetheoreticalmodelgivenbyMroz
et
at
(19S9a)andwillbediscussedinsection4.AnothergoalofthepresentworkistocompletetheBrillouinscatteringinvestigationof
KLIIS,
namelythetemperature-dependenceofthevelocitiesofthetransversephononssincethenecessaryconditionforthecrystaltobeferroclastic(namelyachangeofthecrystalsystem)isfulfilled.
2.Experimentalprocedure
Crystalsof
RLHS
and
KJ.HS
weregrownisothermallyat310Kbythedynamicmethodfromanacidaqueoussolution(pH~I)oftheappropriateinitialsalts(pureforanalysis)instoichiometricproportionsintheCrystalPhysicsLaboratory(InstituteofPhysics,AMickiewiczUniversity,Poznan,Poland).Theaccuracyofthesamplecutwasbetterthan0.15°.Samplesofseveraldifferentorientationswerepreparedintheformofcubes(5x5x5mm
3)
tomeasurethesoundvelocitiesalongthecrystallographicaxesandthebisectorsoftheseaxes.Samplesof
RLHS,
forangulardependencemeasurementsofthesoftacousticmode,werealsopreparedtoverifytheeffectofincompletesofteningofthetransverseacousticphonons,observedinthepreviousBrillouinscatteringinvestigations(Mroz
eta/1989b)
andintheultrasonicmeasurements(Hempel
eta/1988,
Breczewski
etaI1990).
TheBrillouinspectrometerhasbeendescribedindetailinpreviouspapers(Mroz
et
at
1989b).Theincidentlightwasprovidedbyastabilizedsingle-modeargon-ionlaser(SpectraPhysics2020)operatingat514.5nm.Thescatteredlightwasanalysedat
fJ
=
90°withapiezoelectricallyscannedtriple-passFabry-Perotinterferometer(BurleighRC-llO).Thefinessewas50andthemeasuredcontrastratiowasabout10
6.
 
ElasticpropertiesofALiH
3
(S04)4
crystals
5675
Tablel,Somephysicalpropertiesdescribing
4mm
-->
mm2
and4~2Ierroelastictransitions.OldNewTransition
4mm-->mm2
4~2
Orientationof
+y
Y'$~X
rystallographicaxes
~__x
z
He
-e,+c
-
Softelasticconstant
pv;
C(.t.
V'(C
11-
C'2-
en,')"
+
!kl.]
Ci,k!
%
a
forthe
ell'CJJ.C-1-l
el.
c~~.
C4.:hC66
prototypephase
eM.
ell.
Cl.~
ell.CLhCHI
Spontaneousstrain
e,
et-
e]_
and
en
Softmodedirection
[100J
=
lOlOJ[11OJ
Thesoundvelocities
[J
werefoundfromthemeasuredfrequencyshifts
L\v
usingtheBrillouinequation:
v
=
AL\v(nr
+
n~-Zn.n;
cos8)-1/2
(1)
where}.isthewavelengthoftheincidentlightand
n;
and
fl,
aretherefractiveindicesfortheincidentandscatteredlight,respectively.Refractiveindicesof
RLHS
werefound
by
comparingthecrystalsampleswithseveralliquids(CargilleLabs)ofknownrefractiveindices.
It
wasfoundthat
nx"'"
fly
=
1.462and
n
z
=
1.468.For
KLHS
itwasfoundthat
n,
=
It,
=
1.46and
n,
=
1.44usingamicroscopicmethod.Theelasticconstantsofthecrystalswerefoundusingsolutionsoftheequationofmationforthethreeacousticwavespropagatinginthedirection
Q
asgivenby:
Iciiklqiqk-pv2
1
=
0(2)where
qj'qk
arethedirectioncosinesof
Q,
p
isthedensityofthecrystal
(2.81
gem
-3
for
RLHS
and2.3gcm
3
for
KLHS
usingthex-raydataofPietraszkoandLukaszewicz,1988)and
C'jki
areelasticstiffnesstensorcomponents.
3.Experimentalresults
3.1.
RLHS
Inordertoclarifythedifferencesimposedbythenewlypostulatedtypeofphasetransitionin
RLHS,
severalpropertiesdescribingthe'old'
(4mm-mm2)
and'new'(4---;.2)transitions,havebeencollectedintable1.Asisevidentfromthistable,thesoftelasticconstant(forpointgroup4),whichvanisheswhen
T---;.T
c'
hasamorecomplicatedformincomparisontothe
Ctih
elasticconstantforpointgroup
4mm.
Thisisrelatedtotheformofspontaneousstrainforthe4-2transition,namely
a(e
t-
e2)
+
{3e6
andthecorrespondingeigenvaluesoftheelasticconstantmatrix,givenintheform(Boccara1964):
1
ell-el2
C]612C]6C66
Theexpressionsfor
pu"
asafunctionoftheelasticconstantsforpointgroup4are

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