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Anomalies of the temperature dependence of electrostriction in blue phases
V. Dolganov, O. Lourie, G. Heppke, H.-S. Kitzerow
To cite this version:
V. Dolganov, O. Lourie, G. Heppke, H.-S. Kitzerow. Anomalies of the temperature dependence of electrostriction in blue phases. Journal de Physique II, EDP Sciences, 1993, 3 (7), pp.1087-1096.
�10.1051/jp2:1993185�. �jpa-00247884�
J.
Phys.
II France 3 (1993) 1087-1096 JULY 1993, PAGE 1087Classification Physics Abstracts
61.30
Anomalies of the temperature dependence of electrostriction in
blue phases
V. K.
Dolganov II),
O. R. LourieII),
G.Heppke (2)
and H.-S. Kitzerow(2)
(')
Institute of Solid StatePhysics,
Russian Academy of Sciences, 142432,Chernogolovka,
Moscow distr., Russia
(2) Iwan-N.-Stranski-Institut, Sektretariat ER II, Technische Universitit Berlin, Strasse des 17. Juni 135, D-1000 Berlin 12,
Germany
(Received 29 October 1992, accepted in
final form
30 Maich 1993)Abstract. We investigated the field-induced Shift of the blue phase diffraction bands. The
temperature
dependence
of the electrostriction tensor components is determined for the first time.In the blue
phase
BPI at constant field strength E fl [001], a change of the temperture leads to achange
of both the unit cell volume and its shape. The deformation of the unit celldisplays
apretransitional
behaviour onapproaching
the BPI - BPIIphase
transition temperature.1. Introduction.
In the
liquid-crystalline
bluephases
BPI and BPII[I]
the localordering
of molecular orientation forms a 3Dperiodic
structure,having
the symmetry ofcrystals.
BPI exhibits abody
centered cubic lattice
O~,
while BPII is describedby
asimple
cubic structureO~.
Sofar,
essential progress has been achieved in the theoreticaldescription
andexperimental study
of bluephases.
In the framework of the Landautheory
onphase
transitions and of the disclination model[2-4]
it has been shown that for substances with a small cholestericpitch
the cubicstructures,
O~
andO~,
can bethermodynamically
stable between theisotropic liquid
and thecholesteric
phase.
The structures have been determinedexperimentally
and theiroptic
characteristics have been examined in detail.
A series of
electrooptic
effects associated with thechange
ofcrystal
orientation and local director in the lattice[5-9],
electrostriction[9-1Ii
andphase
transitions[10-15]
have been discovered in an electric field.Temperature dependences
of the cell parameters, the scalar order parameter s[16, 17],
and theoptical activity,
have been measured for the temperature range of bluephases.
It should be noted that these alterations do not exhibitpretransitional
behaviour for the BPI-BPII transition. For instance, e can be
regarded
as an orderparameter only
for the transition to theisotropic liquid,
I-e- the temperaturedependence
for ~ has nosingularities
in thevicinity
of the BPI-BPII transition. As yet,only
few attention has beendevoted to the temperature
dependence
of the electrostriction tensorf.
This tensor describes thedependence
of a field-induced strain k of the bluephase
lattice on theapplied
electric field E :Uij ~
Yijki l~t l~i II)
From the function y
ii
(T)
it has been concluded[18]
that the BPI lattice is not stable near the BPI-BPIIphase
transition.Here, we present for the first time the temperature
dependence
of all coefficients of the electrostriction tensor for BPI in two mixtures withnegative
dielectricanisotropy.
Bothmixtures
give
similar results. The temperaturedependence
off
differsdistinctly
for the orientations Efl [001
and Efl [01 ].
This indicates an essentialchange
in the electrostrictionanisotropy.
For both mixtures the deformation of the unit cell atEl [001] displays
apretransitional
behaviour uponreaching
the BPI-BPIIphase
transitiontemperature.
2.
Experimental.
Two separate mixtures, A and B, have been
investigated.
The first one(A)
is a mixture of thechiral
compound
S811(Merck, Germany,
30 fbby weight)
with the nematic mixture EN18(Chisso Corp. Japan,
70wt.-%).
The second one(B)
is a mixtureanalogous
to that used earlier[18]
a chiral-nematic mixture with the chiralcompound
BNX-16(Vilnius University,
Lithuania
(81
wt.-fb))
and the nematicliquid crystal
1650DII
8.9 wt.-fb).
Both mixtures havenegative
dielectricanisotropy.
The mixture A forms the three bluephases BPI,
BPII, and BPIII[19], showing
thefollowing temperature
ranges. BPI 41.80-42.12°C,
BPII 42.12-42.29 °C,BPIII : 42.29-42.4 °C. The mixture B forms the blue
phases
BPI and BPII. Thetemperature
ranges are for BPI : 37.64-38.025 °C, for BPII 38.025-38.47 °C.
The
sample
was contained between twoglass
slides coated with a transparentconducting layer. Mylar
spacers of 17 ~Lm thickness were used. The temperature was controlled with an accuracy of ± 0.005 °C. In order toinvestigate
the behaviour of bluephases
in an electricfield,
sinusoidalvoltages
with afrequency
of 4 kHz were utilized. Diffraction lines were measured in thelight
transmissionspectrum.
Samples
with[001]
and[0
II directions normal to theglass plates
wereprepared. Samples
of BPI with the cell
plane parallel
to theglass plates
were obtainedby applying
sinusoidalvoltage (m
45 V ) to thesample.
After a slow decrease of thefield,
a uniform[001
orientationwas obtained. A
[011]
orientation in BPIsamples
was achievedby
slowcooling
from BPII.The orientation
[011] fl
E is not stable andeventually
thesample
mayacquire
the orientation[001 fl
E. The time constant of reorientationdepends
on theapplied
fieldstrength
and on thetemperature.
At U ~ 40 V and T~ T ~ 0.03°C,
the orientation[011]
fl E was stable for several hours. At ahigher
temperature, the reorientation time decreaseddrastically,
and it was notpossible
to make measurements for the lattice orientation[011]
fl E in the closevicinity
of the BPI-BPIIphase
transitiontemperature.
3. Results.
Beyond
thesample absorption region
the BPI transmission spectrum for the[001]
facesparallel
to theglass plates
ispresented by
asingle
bandA~.
The band involves one reflection(002)
and four reflectionsloll ),
coincidijin wavelengths
for abody
centered cubic latticeO~ (Aw~
= d n sin @,=
90 °;
A~jj
=
2 d n sin @,
= 45° ;
Aw~
=A~jj ).
Without anelectric field the
spectral position
of reflections shows atemperature dependence
which istypical
for bluephases (Figs.
la,2a)
: ashort-wavelength
shift of reflections(compression
of the unitcell)
is observed withincreasing
temperature. Deformation of the cubic structure of bluephases
in an electric field(electrostriction)
leads tosplitting
of the bands A~~~ andN° 7 ANOMALIES OF THE TEMPERATURE DEPENDENCE OF ELECTROSTRICTION 1089
11
~
b
I,
nlT
~~~
~
4 I
~
+ .
u '
~ ~ @
~
D
D
@ D
-20
~ ~h
~ mm
42.0
42.1 42.042.I
Fig. I.-a)
spectrum : (.) Ao
~
(A
o~~ + 2 A ~j j )/3;
b) emperature ependence do~~do~~ 2 d~~ ( *),
U
= 39 ixture .
1-O
,, a
I
') ,"'~~'"',
","' /~
°
$
i J i ," / °I j II
/
'o o
z~ , I I
l$°'~
j
l~
' , o °i ' ,
j II
o o
4i ~
,' ~
~ 3
a o
' 2
16 on° 4
14
400 450 500
Wa~ekngth, n3n
Fig.
3. Transmission spectrum in an electric field for the orientation El [001]. (1), (2), (3) BPI. (I) T= 41.99 °C, (2) T
=
42.07 °C, (3) T
=
42.12 °C, (4) BPII. Mixture A.
(short-wavelength
band inFig. 3),
which is in agreement with thetetragonal
symmetry of thecell
[19]
in an electric fieldEl [001].
The temperaturedependences
forA~~~(T)
andA~jj
(T)
differconsiderably (Figs.
la,2a).
To separate the effects related to electrostriction and temperature variation we haveplotted
the shifts of the(002)
and(0
II reflections relative totheir
positions
without a field infigures16,
2b (A~~~ =A~~~(E)
A~;A~jj
=A~jj(E)
A~).
To calculate A~~~ andA~ij
for T ~ T~(Fig. 4)
the value of A~ was determinedby
linearextrapolation
of thetemperature dependence Ao(T).
The lattice constants of the deformed lattice aregiven by dwj(E)
=
d + a,
dj~~(E)
=
d + b, where d is the lattice constant of the undisturbed cubic lattice d~~j and
dim
are the lattice constantsparallel
andperpendicular
to the field direction. The shift of the(002)
reflection is causedby
achange
of theinterplanar spacing
d~~j~ °°2 =
~~
+ ~ n(2~
The shift of the
(011)
reflections occurs due to variations of both the lattice constantd~jj
and the diffractionangle
@ojjdoll
~) Ii
+~~i~ (3)
Sin 0011
-) Ii ~i~~ (4)
A ojj = 2
dojj
n sin @ojj =(d
+b)
n~
dim
n(5)
For the field direction
[001
the shift of the(002
reflection isproportional
to thechange
of the lattice parameterparallel
to the fielddirection,
the shift ofAoii
isproportional
to thechange
of the latticeparameter
normal to the field direction. If the volume of the unit cell ispreserved (a
= 2
b)
we get fromequations (2)
and(5)
:~002
" ~ ~011(6)
In this case, the sum
(Aw~
+ 2 Aojj
)/3
should be constant (= Ao),
I-e- Aoo~ + 2Aoj
j = 0.
Figures
I and 2present
the values of(Aw~
+ 2Aojj )/3
andAw~
+ 2Aojj
obtained from theexperimental
values of Aoo~ and A
oj j.
Proceeding
from the data offigures
I and2,
we concludethat within the
experimental
accuracy of our measurements the deformation of the unit cell does not affect its volume.N° 7 ANOMALIES OF THE TEMPERATURE DEPENDENCE OF ELECTROSTRICTION 1091
Tuming
to the electrostrictioncoefficients,
ourexperimental
observation of the functionsA~~i(E)
=
fj~~ijE~ yields
effective coefficientsfj~~ij
which are linear combinations of the componentsy,~~~
defined inequation (I).
yjiij =
f
joojj can be calculated either from the shift of the
(002) reflection, f
joey = Aoo~/Ao
E~,
or(due
to the constant volume of the unitcell)
from thesplitting
between the reflection bands A= Aoo~
Aojj, fjoojj
= ~ ~~
(Figs. 5, 6).
The 3Ao
Eloo
u
6,
oomm
BPI BAIT
50
[
~ A~6
Do 6
a
~ T~
0
42.0 42.I
T,°C
Fig. 4. -Temperature
dependence
of thesplitting
A between the two reflections (002) and (011), in BPI : (o) U 42 V, (D) U=
39 V, (/L) U
=
30 V. Mixture A.
o
~~~ ,' '',
~
~
l
0"I
~'~
,,~
°~
~~~~~
~ p
j',
B pj jm'~l~
10 ''>, ° 0.1 75
j o_o
1' ,~
0. I BPI~'i (
BPIIa DO
~ ~
~~*~,
~ °~ '
'i,y
o_o
~''
0.0 ~
' ''
'
~ +
i
+ +/~
~+ ,
~ ~
* *, ~ ~
*
l
*"0* '#
»j
0 *-10. 0
42.0 42.I T,°C 37.9 38.0
T,°C
Fig.5. Fig.
6.Fig. 5.-
Temperature dependence
of the electrostriction coefficients in BPI : yjii "ijooii,
(o) U=
42 V, ID) U 39 V, (/L) U 30 V ; (.) y
j~ii (+)
fjoii
j, U 39 V (*) y2323. BPII : (Q) yii ii, U
= 39 V, mixture A.
Fig. 6.-
Temperature dependence
of the electrostriction coefficients in BPI: yjii "ijooii,
lo) U=
45 V, (D) U
= 39 V, (.)
y/j(j
(+) fjoi~~, U 39 V (*) y2323. BPII (Q ) yjiti, U= 39 V,
mixture B.
electrostriction coefficient
§jojjj, characterizing
the variation of theinterplanar spacing doj
j for the orientation Efl [011 ],
was determined in BPI from the shift of the diffraction bandAojj
in the transmissionspectrum
:fjojjj
= AA
ojj/Aojj E~ (Figs. 5, 6).
The electrostriction coefficientfjoojj
in BPII was found from the shift of the diffraction bandAwj
insamples
with the orientation[001] fl
E(Figs. 5, 6).
4. Discussion.
The most remarkable feature of the data obtained is a drastic increase in the
splitting
A(Fig. 4)
and in yii
(Figs.
5,6)
onapproaching
thephase
transition temperature. There is an essential difference in the behaviour offjoojj
andfjojjj.
The electrostriction coefficientfjoojj diverges
close to the transition temperature, while
f
joyj
depends only slightly
on temperature. Since the volume of the unit cell ispreserved (yjj~~
= yj ii j
), only
two of the three electrostriction 2tensor
components (in
cubic structures yjjjj, yjj~~ and y~~~~) areindependent
yjjjj=
fjoojj,
y~~~~=
fjojjj fjoojj [20].
Ananomalously
drastic increase of yjii
IT)
occursonly
4
in BPI. At the
phase
transition BPI-BPII, thesign
of yj ii
changes
and its absolute value above the transition temperature is smaller. ForBPII,
yiij does not
depend
on the temperature. The shift of the diffraction bands in a substance with alarge
cholestericpitch,
observed in paper[21],
islikely
to be associated with thechange
of electrostriction. The values ofy~~~~
presented
infigures 5,
6 were obtained from the relation y~~~~ =fjojjj fjo~jj.
In 4contrast to yj ii j, y~~~~ does not exhibit a critical behaviour close to the BPI-BPII transition.
This result indicates that the lattice becomes soft with respect to field-induced deformations
along
the axes of the cubic lattice(which
are describedby
yjjjj),
but remains stable as far asshear deformations are concemed
(which
are describedby
theoff-diagonal
elements ofk).
The difference in the behaviour of yj jjj and y~~~~
(Figs. 5, 6)
results in astrong change
ofthe electrostriction
anisotropy
1~ =
(yj
iii
yjj~~)/2
y~~~~ in BPI(Figs.
7,8).
The absolute value of1~ increases on
approaching
thephase
transition temperature.o-o
xx
_~_~ ~ x~~ xx
~
~§
-l.0~
~ x
x
~
~~'°
'~
~~n~ ~x
-2.0 ~
42.0 42.I
T,°C
37.9 38.0T,°C
Fig
7Fig.
8.Fig.
7.- Temperaturedependence
of the electrostrictionanisotropy (yjjjj yjj~~)/2
y~~~~ in BPI.Mixture A.
Fig. 8. -Temperature dependence of the electrostriction
anisotropy
(yjjjj-yjj~~)/2 y~~~~ in BPI.Mixture B.
N° 7 ANOMALIES OF THE TEMPERATURE DEPENDENCE OF ELECTROSTRICTION 1093
For both mixtures the
dependence
yjjii
(T)
can be describedby
the function yjiii
(T)
=
A(T* T)~ '.
The temperature T* is in closevicinity
of thephase
transition temperature :T* T~ m 0.05-0.08 °C, which is
by
an order ofmagnitude
less than thecorresponding
value for thephase
transition from a nematic or cholestericphase
to theisotropic liquid.
Note that T* determined in this way indicates thehigh-temperature
limit ofdivergence
for yj ii j, since the latter may have atemperature-independent
part. In this case, the difference T* T~ will be of a smaller value.Therefore,
the temperature variation of yjj ii indicates apretransitional
behaviour for the BPI-BPII transition in both mixtures.
Since the electrostriction is the result of a
competition
between electric and elasticforces,
letus consider the connection between these
properties
in more detail in thefollowing paragraph.
In
general,
thedependence
of the free energy on an extemal field E and on deformations k of the bluephase
lattice is describedby [22]
AF
=
A,~a
u,~ u~i x,~~iE,
E~ E~Et
p~~~i E~ E~ u~i(7)
Here,
the elastic constant tensorI
characterizes the stiffness of the lattice,I
is the non-linear dielectricsusceptibility
tensor, and theelasto-optic
tensor#
describesa
coupling
term which connects the free energy to both k and E. The electrostriction tensorf
which isinvestigated
inour paper is connected to these
macroscopic properties by [22]
Yi jki ~
( 7r ~,j,in, ~'nmti (8)
where
(
is the tensor ofelasticity
or
compliance coefficients,
I-e- thereciprocal
tensor toI. Physically, equation (8)
means that themagnitude
of the electrostrictive effect islarge
if the lattice ismechanically
soft and/or if thecoupling
between the electric field and the strain in the free energyexpansion (I.e.
the third term inEq. (7))
islarge.
In order toexplore
these relations in moredetail,
we have to express the individual components of the electrostriction tensorby
the components of the
elasto-optic
tensor and the elastic constant tensor. For cubic structures, the tensors(
and#
have threeindependent
components, which can be used forexpressing
Y I, Y 122, ~fld Y2323
Yllll
"~ (~llll~'llll
+~~l122~'l122), (9)
Yl122 "
) (~llll ~'l122 +~l122~'llll +~l122~'l122), (10)
Y2323 ~)
~2323 ~'2323The
splitting
between thereflections,
A= A
w~ A
~jj =
(a
b n,depends
on the difference between the electrostriction components A = y j j yj j~~) E~
Ao. For
(
yj j j y ~~
)
weobtain the
simple
relation :Yllll Yl122 "
) (~'till ~~'l122)(~llll ~~l122). (l~)
The tensor
(
isreciprocal
to the elastic constant tensorI.
Thus, fora cubic structure the
relation between the
independent
components of the tensors(
andI
has the form:
~~~~~
(~
II IIl~~~)~~~l~~~~
~ ~ l122)
~~~~
~~~~~
(~llll
~122~~~~~ll
+ ~
~l122)
~~~~
s ~~~
l
(15)
~ 4 ~2323
From
(12)-(14)
thefollowing
relation must be fulfilled :Yiiii-yjj~~=
I
_~'nil-Pj122
~~ ~~~~l
~l122 (16)
The relation yj ii j =
2 y
j j~~
imposes
limitations on the components of theelasto-optic
tensorfi.
It follows fromequations (9), (10)
and from the relation yjjjj=-2yjj~~,
thatPi
jjj = 2 Pjj~~. This relation leads to the electrostriction coefficients :
Yllll ~
£~'till(~llll ~~l122) (17)
From
equations (11), (13)-(15), (17)
and(18)
we can obtain the components of the electrostriction tensor~llll ~
~
~[ill
~~~~~~~
~ ~~~~~(i~~
Yl122 ~
~llll
~~
"~~~~~i ~i122) ~20)
y~~~~ =
~~~~~
(21)
~ "~
2323
Equations
similar to(19)-(21)
have been obtainedpreviously by
Stark and Trebin[23] using
theassumption
that an electric field causesonly
achange
of the orientational order(P
ii j = 2 Pj~~
).
However, in the present paper theequations (17)-(21)
have been derived from the condition of conservationofthe
unit cell volume under its deformation in an electric field. It should be noted that the relation(16)
is valid without the condition of constant unit cellvolume,
whereas the relations(19), (20)
are validonly
under the condition yjjjj=
~ Yl122, °~
~'II
II ~ ~
~'l122.
Using
theequations (19)-(21),
we can now discuss how the electrostriction coefficients are affectedby
the components offi
andI.
The relationyj iij =
2 y
jj~~ leads to a
relationship
between the
elasto-optic
coefficients(P
ii11 = 2 P
jj~~), but it does not lead to a
relationship
between the
elasticity
tensorcomponents. Signs
and values A,~~i areonly
limitedby
thecrystal stability
condition. Thecrystal
deformation energy A~~~i u~~ u,t should bepositive
at anyvalues of
u~~. This
imposes
certain restrictions on A~~~i~2323~0, ~llll*~l122~°, ~llll +~~l122~°' (~~)
Electrostriction tensor
components
have been calculatednumerically by
means of the Landau- de Gennestheory [23, 24]. However,
a numericalcomparison
of absolute values of A~~a with theexperimental
values cannot be done, since the final results obtained in[23, 24]
involve Landau
coefficients,
for which no exact data are available at present. The theoreticalN° 7 ANOMALIES OF THE TEMPERATURE DEPENDENCE OF ELECTROSTRICTION 1095
calculations neither
predict
thesign
of the temperaturedependence
of f noryield
inquantitative
values for the temperature coefficients off.
A decrease off
withincreasing
temperature[24],
or an increase of f with temperature[23]
have beenpredicted
in BPI and BPII. In conclusion, the theoretical considerations available as yetgive
no hints how toexplain
the unusual temperature
dependence
of the electrostriction tensor observed in ourexperiments especially,
it has not been discussed whether yj ii j may growanomalously
invicinity
of theBPI-BPII
phase
transition temperature.However,
inpreviously published experimental
works[25-27]
the temperaturedependence
of the shear modulus has been measured for blue
phases [25-27].
The variation of the shearmodulus in BPI near the BPI
- BPII
phase
transitiontemperature
amountsapproximately
30 fb (T~ T m 0.15
°C) [27].
y~~~~(Figs. 5, 6)
ischanged by
about the samemagnitude.
One may thus suppose that the basic contribution to thetemperature dependence
off
comes from the temperaturedependence I IT). According
toequation II 9),
an increase of yjii j, while
approaching
thephase
transition temperature(Figs. 5, 6),
can be associated with adecreasing
value of the difference A
jjjj A
jj~~. It is
important
to note that this difference is involved inthe conditions for elastic
stability
of thecrystal (see
relations(22)).
As Ajii A
jj~~ tends to zero, the
O~ (BPI)
lattice becomes unstable relative to spontaneous deformations. Estimates of the mean-square fluctuation values of the cubic lattice near the BPI-BPII transition temperature[18]
are in agreement with such aninterpretation
of the cause for the BPI- BPII
phase
transition. There are other evidences of temperature
dependent dynamical
processes in BAIT[28, 29]
as the transition to BPIII isapproached.
5. Conclusion.
We have determined the temperature
dependence
for all the threeindependent
components ofthe electrostriction tensor, y~~~i, for two mixtures with the
negative
dielectricanisotropy.
The temperaturedependences
for yjjjj and y~~~~ in BPI differessentially
which leads todeformation of the unit cell with
varying
temperature. The coefficient yiiii and theelectrostriction
anisotropy
1~
display
apretransitional behavior,
whenapproaching
the BPI- BPIIphase
transition temperature. Such a behaviour may beexplained by
the temperaturebehaviour of the
elasticity
module,and,
as a result, the BPI lattice may become unstablerelative to spontaneous deformations. In this case, the BPI- BPII
phase
transition andpretransitional
behaviour can be describedusing
the components of the elastic constant tensorI
as an order parameter.References
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