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Physica Scripta. Vol. 60, 277^282, 1999

Research of Electromagnetic Fields Arising at Interaction of Laser

Radiation with Ferroelectric Materials
V. V. Kolesov,2 Yu. V. Korobkin,1 * I. V. Romanov,1 V. B. Studenov1 and V. A. Davydov2
1
P. N. Lebedev Physics Institute, 117924 Leninsky prosp. 53, Moscow, Russia
2
Moscow Institute of Radioengineering, Electronics and Automation, 117454 Vernadsky prosp. 78, Moscow, Russia

Received December 30, 1998; accepted January 12, 1999

pacs ref: 77.70.+a

Abstract magnetic eld under a subnanosecond powerful laser pulse

In this paper we deal with electromagnetic radiation arising due to variation
of the dipole moment of a ferroelectric pattern as a result of its temperature
change. It is also shown here that, when the pattern is heated up with a power-
ful electromagnetic pulse, the total radiated energy is inversely related to the
pulse duration tp (at the same heating power). The radiation spectrum
has its maximum at the frequencies of the order of tp 1 and exponentially
abates if the frequency exceeds tp 1 The results of experimental investigation
of radio-frequency radiation from ferroelectric crystals when they are heated
with pulse laser radiation of nanosecond duration are touched upon below.
A numerical calculation of the magnetic component of the radio waveeld
has been performed for a laser pulse of a particular shape. A comparison
between the experimental results and the theory prediction is also available
here.
1. Introduction
In media whose properties are changed with time, electro-
magnetic radiation may be emitted by a system of steadystate
charges and currents. The radiation energy thereat is derived
from the source that provides with unsteady-state conditions
of the medium. A great number of works (see, e.g., Refs.
[1] and [2]) are devoted to the analysis of such radiation
processes. In the works the eld of those sources had usually
been accepted as a given (preset) one and the characteristics
of the radiation that had to appear under a denite depen-
has been registered.
In this paper we present both theoretical and experimental
treatment of the problem of electromagnetic radiation result-
ing from thermal changes of the dipole moment of a
ferroelectric. All experimental results have been obtained
by pulse heating of LiNbO3 crystals.
2. Radiation at an arbitrary time-temperature dependence
In what follows it is suggested that: (1) the temperature in a
pattern of the volume V is being changed homogeneously;
(2) the pattern is dened as a point dipole with the moment
PS V , which means, in particular, that the linear dimensions
of the pattern are much less than the radiation wavelength
and the distance to the point of observation. The angular dis-
tribution of the radiation instantaneous power in this case
is described by the known expression:
d 2W V 2 
2
P sin2 y; 1
dOdt 4pc3
(where y^ P;
d K K is the radiation wave vector), which can
be easily rewritten as
Z
d2 W V 2 4  2 2 1 1
dence of the medium permittivity on time (in some cases, o P o sin y; Po Pte iot dt: 2
on coordinates) had been considered. dO do 2c3 2p 1
Let us consider here the radiation that arises also in the Let us rst investigate the case when the temperature
event when there is no external eld available in the substance. change is much slower than the polarization relaxation to
The reason for such radiation in ferroelectrics might be the its equilibrium (at a given temperature) value of P e T . In this
pyroelectric eect, i.e. the temperature induced change in case the Pt dependence is fully dened by the T(t) function
the macroscopic dipole moment being conditioned by spon- and expressions (1) and (2) aquire respectively the form
taneous polarization. At temperatures T < TC (TC is the
ferroelectric phase transition temperature) the ferroelectric d2 W V 2 
2 2 2
d Pe _
2 dP e 
possess a spontaneous polarization P s PT . Variations Pe sin y; P e T T; 3
dOdt 4pc3 dT 2 dT
in temperature result in variations of the total dipole moment
of the crystal, that must cause the generation of electromag-
d2 W V 2 4  2
netic radiation, the intensity being proportional to jP s j (the 3
o P e o  sin2 y: 4
dots over the symbols from here on mean time derivatives). dOdo 4pc
As this takes place, thermal energy is partially transformed It should be noted that by non-linearity of the P e depen-
into radiation energy. It is essential that the analogous eect dence on time, radiation has to be emitted even for T 0:
in an unbounded homogeneous crystal is not available. This In this case the radiation power is
phenomenon is explained by a destructive interference of  
the radiation emitted by dierent areas of the crystal. d2 W V 2 dPe 2 _
4 2
T sin y: 5
Such radiation from ferroelectric crystals has been reported dOdt 4pc3 dT 2
in paper [3] where an electric component of a MW electro-
Hereafter for simplicity we restrict ourselves to the case of a
* e-mail: korobkin@sci.lpi.msk.su ferroelectric with one axis of spontaneous polarization.
# Physica Scripta 1999 Physica Scripta 60
278 V. V. Kolesov, Yu. V. Korobkin, I. V. Romanov, V. B. Studenoy and V. A. Davydov

Within the framework of the Landau theory, the equilib- The radiation spectrum is described thereat by the
rium spontaneous polarization takes the form expressions

0 p; T > TC
2
Pes ; 6 d2 W S V2 P~ es
P~ es TC T ; T < TC
dOdo 32pc3 TC T0 3
h
 i2
where P~ es is a constant numerically equal to the magnitude of  T_
2
2TC T0 o2 T1o sin2 y; 11a
the spontaneous polarization at TC T 1K. in the case o

when there is a slight temperature change of the pattern, it

is reasonable to make use of a linear approximation of
Pes T far from TC : d2 W s V2 s 2
g To 2 o4 sin2 y; 11b
dOdo 2pc3
DPes
gs ; 7
DT
 
where gs is the pyroelectric coecient. The superscript s d2 W E V 2 zE 1
means that the pyroelectric coecient is dened at a constant 3
dOdo 2c 4p TC T 6
stress tension s 0; saying otherwise in the absence of any h 
 i2 
2 1; T > TC
mechanical coupling preventing from a free thermal  2 T_ jT TC jo2 T1o sin2 y  1 :
expansion of the pyroelectric [4]. o 4; T < TC
At the avalability of the electric eld E in the non-polar 11c
phase T > TC and also near by TC in the polar phase the
polarization obeys the Curie ^ Weiss law, The expressions (10^11) displayed above are valid for a
 temperature change which is slow enough and insignicant
zE T TC 1 ; T > TC : by its magnitude.
Pes 8
4p 1=2T TC 1 ; T < TC

Here z is the Curie constant. By substituting (6), (7), (8) into

(3) we shall get respectively: 3. Radiation at pulse heating: numerical evaluation

2 h In the case with pulse heating of a ferroelectric sample the

d2 W s V2 P~ es
2 i2 velocity of its temperature change is dened by the equation
3 3
T_ 2TC T T sin2 y; 9a
dOdt 64pc TC T
C T_ aLIt 12

d2 W s V 2 s
2 
2 2 where C is the heat capacity of the whole sample, It is the

g T sin y; 9b
dOdt 4pc3 incident radiation power, a is the absorption coecient, L
is the length of the area that absorbs (emits) the radiowaves.
  The volume V, which was met in Section 1, is equal to the
d2 W E V 2 zE 2 1 h
2 i2 product of L by the sectional area of the incident beam.
2 T_ jT TC jT sin2 y
dOdt 3
4pc 4p TC T 6 Equation (12) stems from the thermal balance equation if
 one ignores the heat emission through the border of the
1; T > TC
 1 : absorbing area (which can be done for a short pulse) and
4; T < TC
the radiation thermalization time [5].
9c Let us assume that the heating of the sample is performed
by a Gauss shape laser pulse whose intensity is dened by
Further we assume the pattern temperature to change the expression
insignicantly, that is: T T0 T1 t; jT1 j  jT0 TC j; so
that Eqs (9a) and (9c) correspondingly take the form
It I0 exp t2 =t2p ; 13
h


s 2 i2
d2 W s V2 Pe 2
3
T_ 1 2TC T0 T 1 sin2 y; where I0 is the maximum intensity, and t2p characterizes the
dOdt 64pc TC T0
3
pulse duration.
10a By using Eqs (13), (12), (9b), and (10a,c) one can easily nd
the radio-frequency radiation intensity
 
d2 W E V 2 zE 2 1
2
4
d2 W s V 2 P~ es T_ m
dOdt 4pc 4p TC T0 6
3

h i2  dOdt 64pc3 TC T 3

2 1; T > TC " #2
 2 T_ 1 jT0 TC jT 1 sin2 y  1 :
t TC T0
4; T < TC 2 2
t2 =t2P
 e 2t =tp 4
e sin2 y; 14a
10c tp T_ m tp

Physica Scripta 60 # Physica Scripta 1999

 Research of Electromagnetic Fields Arising at Interaction of Laser Radiation with Ferroelectric Materials 279

d2 W s V 2 s 2 _
2 t2 t2t2
2 dependence of the total irradiated energy on the pulse
g T m 4 e P ; 14b duration.
dOdt pc3 tp
Let us now estimate the pyroelectric radiation magnitude
for readily accessible experimental conditions. The radio
 
4 pulse energy substantially depends on the sample material.
d2 W E V 2 zE 2 T_ m
3 The lithium niobate single-domain crystal possesses one of
dOdt pc 4p TC T0 6 the highest values of spontaneous polarization Pes At
" #2
2 2 t TC T0 t2 =t2 T 300 K the value of Pes makes up 0.71 C/m2, the
 e 2t =tp
e P sin2 y pyroelectric coecient is gs 0.4
10 8 C/cm2 K. The typical
tp T_ m tp
 polarization relaxation time for such well studied ferroelectric
1; T > TC materials as (LiNbO3 , BaTiO3) is about tr  10 11 s. The
 1 :
4; T < TC 14c magnitude of the radio pulse eld increases proportionally

to the energy of the heating pulse. In this case the failure
Here T_ m aLI0 =C is the maximum velocity of the threshhold of the crystal is likely to be a limiting factor for
sample temperature variation. If the temperature change is the laser pulse intensity.
small, then, while calculating the total irradiated energy For LiNbO3 crystals this threshhold is 1:5
109 W/cm2
and the radiation spectrum one can ignore the rst term l 1:06 mm; tp  100 ps or 5.5
108 W/cm2 l 1:06 mm,
in the square brackets of Eqs (14a, c). So, for the total energy tp  5 ns). Let a LiNbO3 crystal with L 1 cm be radiated
one has by a laser pulse of duration tP  100 ps 10 10 s (this is

2
4 an optimum duration having regard to the condition of
dW s 1 V 2 P~ es T_ m 1 2 homogeneity of the crystal heating) and an energy equal to
p 3 sin y; 15a 0,1 J.
dO 16 2p c TC T0 tp
The heat capacity of LiNbO3 is Cp 3 J/cm3 K. The crystal

2
2 is kept at room temperature, T  300 K, whereas its phase
dW s 1 V 2 gs T_ m 1 2 transition temperature being TC 1483 K one can make
p 3
sin y; 15b use of Eq. (15b) to evaluate the pyroelectric radiation energy.
dO 4 2p pc t p
By considering that 10% of the laser pulse aL  0; 1 is

2 absorbed and supposing the beam diameter d to be of
  
dW E 1 V 2 zE 2 T_ m 1 2
2
1; T > TC 1 cm (V pd L=4), one nds for the radiation angle
p 3 sin y  :
dO 4 2p c 4p TC T0 4 tp
1
4; T < TC y p=2; dW s =dO  10 12 J/sr which corresponds to an
average power of tP 1 dW s =dO  10 2 W/sr.
15c
As this takes place, the main radiation energy is grouped
It should be noted that Eq. (3) as well as Eqs. (15) are true within a decimeter range of wavelengths of W  tp 1 
10 1
only at tp  tr ; where tr is the polarization relaxation time 10 s :
to its equilibrium, at a given temperature. Another indepen-
dent limitation for the use of formulae (15) is the condition 4. The experimental arrangement
ctp  L which provides with a homogeneous heating up
and the validity of the point dipole approximation. To investigate the dynamics of the radio wave generation pro-
The spectrum corresponding to Eqs (14a, b, c) has the form cess the ferroelectric sample was exposed to the eect of a
high intensity nanosecond laser pulse.


4 2 In order to receive nanosecond light pulses a phosphate
2 s ~ s 2 2 T _ t
d W P V m p 2 2
e 3 o2 e o tp =2 sin2 y; 16a glass laser (l 1:06 mm) was used together with a
dO do 32pc TC T0
Fabry ^ Perot resonator working in the mode of modulation
durability performed by a saturating absorber of LiF with
d2 W s V 2 s 2 _
2 2 2 o2 t2p =2 2 dyeing centra. A generator output pulse of 30 ns duration
g T m tp o e sin y; 16b was used for the formation of a light pulse with the duration
dO do 2pc3
tf 6 ns and with the fronts tf 1 ns. After preliminary

4  amplication (by 10 times) and telescopic expansion of
d2 W E V 2 zE 2 T_ m t2p 2 o2 t2p =2 2 1; T > TC the light beam the light pulse was directed into two-path
o e sin y  1 :
dO do 24pc3 TC T0 4 4; T < TC and three-path ampliers. The maximum energy of the light
16c pulse at the laser system output reached 4.5 J for a beam
cross-section diameter of 15 mm and with an angular diver-
One can see thatpthe spectrum (16) has its maximum at the gence equal to  10 3 rad.
1 The time response of the laser beam is shown in Fig. 1a.
frequency om 2tp and exponentially dies away at
o  tp .
With the change of tp the spectrum is expanding and the
5. Estimation of the magnetic component of SHF wave eld
contribution to the total energy from the high frequencies
2
exceeds ``the losses'' caused by the decrease of d W =dOdo Let us dene the shape of the radio pulse expected in our
at the ``previous'' frequency values. One can say that the experiment. As the size of the investigated crystal is essentially
decrease in tp reduces the role of destructive interference less than the distinctive wavelength of the emitting radio pulse
``cutting o '' the spectrum at high frequencies. And this very (l 30 cm at tf  1 ns) usage could be made of the dipole
fact explains the highlighted above (not a quite common) approximation to calculate the radiation. Let the X-axis
# Physica Scripta 1999 Physica Scripta 60
280 V. V. Kolesov, Yu. V. Korobkin, I. V. Romanov, V. B. Studenoy and V. A. Davydov

electromotive force induced in the turn is

 
S P P
ei ; 19
c2 R0 c R20

where S is the area of the turn. From Eq. (7) far away from
the Curie point at small temperature changes the time-
temperature dependence of the dipole moment os dened as
_ ; t gs T_ t:
PT 20

By dierentiating sequentially Eqs (19) and (12) and sub-

stituting the result obtained into Eq. (18) we may write down
the ei dependence on the laser pulse intensity as
S s aL 1 

ei g IR0 =c I_ ; 21
c2 Cv R20

where Cv is the specic heat of the sample.

So the radio signal shape in the loop is dened by the part in
brackets in Eq. (21) and essentially depends on
the distance
R0 : The calculated dependences of IR  0 =c I_ correspond-
ing to the light pulse (Fig. 1a) for R0 2; 5 cm; R0
20 cm are demonstrated in Fig. lb. It can be easily seen that
at R0 2; 5 cm the signal shape is dened by the second item
in Eq. (21) corresponding to the nearest radiation zone which
exceeds the rst (wave) item by a factor of 10.
In the case of R0 20 cm the wave item becomes essential.

Fig. 1. (a) The response of laser pulse. (b) The calculated dependences
 0 =c I)
(IR _ in arbitrary units. The solid line corresponds to R0 2; 5 cm,
the dashed line to R0 20 cm. (c) The time response of the magnetic
component of SHF waves is registered at R0 2; 5 cm.
6. Experimental procedure
The geometry of the experiment is illustrated in Fig. 2. The
direction of the spontaneous polarization axis of the
ferroelectric crystal was perpendicular to the light beam
direction. The crystal aperture was completely packed with
the light beam volume. In order to investigate the process
of SHF wave generation using materials with high absorption
coecients in the visible spectrum range provision was made
for the transformation of the basic radiation of the laser into
the second harmonic with l 0:53 mm with the aid of a
KDP crystal. The transformation coeicient was 15%. Regis-

coincide with the laser beam direction and the Z-axis be

parallel to the spontaneous polarization. The expression for
the intensity of the magnetic eld in the spherical coordinate
system combined with the Cartesian one (the polar angle y
is counted o from the Z-axis) has the following form [6]:

1 _
Pt R0 =c
H r H y 0; H j rot ; 17
c R0

where P P S V is the dipole moment of the sample, R0 is the

distance from the sample to the point of observation (the centre
of a small loop). Then the magnetic eld in the centre of the
loop will be equal to
 
1 P P_
H sin y sin a : 18
c R0 c R20

For simplicity hereinafter we reason that y 90 (the centre

of the loop lies in the plane (X ; Y ; Z; 0)).We think that the
angle a between H and n (between the normal and the plane Fig. 2. The geometry of the experiment: the crystal-(1); the loop-(2); the
of the loop turn) equals zero. For a small enough loop the coaxial cable for the SHF output-(3); the light beam-(4); the metal cavity-(5).

Physica Scripta 60 # Physica Scripta 1999

 Research of Electromagnetic Fields Arising at Interaction of Laser Radiation with Ferroelectric Materials
tration of the magnetic component of the SHF wave was
performed by a loop with the area S 2 cm2, from which
the signal was enhanced by an amplier and then detected
by a high-speed oscillograph started up by a light pulse with
the help of a coaxial photocell. In the oscillograph in use
the rise time of the transition characteristic makes up 0.8
ns/point, and that allows us with a certain assurance to inves-
tigate pulses with fronts  0:8 ns. The voltage transfer
coecient of the receiving channel at the frequency
f 1 GHz was 10, the channel consisting of the loop, the
amplier, the delay line of the oscillograph. External
screening was used to protect the SHF pulse registration
system from electromagnetic interference arising during
the work of the laser arrangement. The emitter (the crystal)
and the loop were located in closed metal cavities of dierent
shapes and sizes and with a hole to inlet the light beam into
a crystal. In this case the interference level by voltage was
approximately 25 times reduced.
7. Experimental results
The LiNbO3 monodomain crystal containing 0,03% of Fe2O3
and measuring X 13 mm, Y 16 mm, Z 14 mm was
heated with a light pulse of the driving generator wavelength
and its second harmonic. A cylindrical cavity with H1
8 cm and R1 4:5 cm was used as a jamproong shield.
The loop was located at the angles y 90 ; a 0 and
according to the theoretical reasoning that corresponded
to a maximum amplitude of the signal. The distance from
the crystal to the centre of the loop was R0 2:5 cm. The
signal registered is displayed in Fig. 1c. The voltage
signal-to-noise ratio made up 5. There is a good correlation
between calculated and measured time characteristics of
the radio signal. With the crystal dipole moment inversion
(to do this it is enough to rotate the sample through 180 )
the signal polarity changed to the opposite one at constant
amplitude. The change of y and a angles caused the signal
to decrease considerably.
The measurements of the output signal amplitude showed
its linear dependence on the light pulse energy (from 0.3
to 1 J), that corresponded to theoretical concepts.
The shielding was carried out also with the aid of cylindri-
cal (with the dimensions: H2 6 cm, R2 3:25 cm) and
rectangular (X 21 cm; Y 28 cm, Z 30 cm) cavities
to investigate the inuence of a shield on the shape and
magnitude of a SHF pulse.
The estimation of the lowest eigenfrequencies of cylindrical
and rectangular resonators (see, for instance, Ref. [6]) showed
that in the case of cylindrical shields those frequencies were
3.5 GHz but in the case with the rectangular ones they were
equal to  1 GHz which correspond to the characteristic
duration of the radio signal.
So, the rectangular cavity is a resonator for the central fre-
quency of the radio pulse oscillation which was registered
in the experiment. Namely, a sequence of decaying pulses with
their total duration equal to 35 ns was observed. When a
smaller cylindrical screen was used, the signal amplitude
increased by a factor of 1.5, the signal shape did not change,
as one can see in Fig. 1c. The signal increase can be qualitat-
ively explained with the use of the method of images (see, e.g,
Ref. [6]). The ``image''of the emitting dipole creates in the loop
# Physica Scripta 1999
281
an electromotive force of the same sign which the sample itself
has.
Similar experiments were carried out with pure LiNbO3
crystals of the same size and they showed analogous results
with the exception of the signal amplitude which was approxi-
mately 3 times less when we had a pure crystal. This may be
explained by the fact that the light absorption coecients
for pure and doped crystals are dierent. The spectrophoto-
metric measurements showed that the portions of the
absorbed radiation in LiNbO3 were equal to 15.6% at
l 1:06 mm and 18.2% at l 0:53 mm; in LiNbO3 with
Fe2O3 they were 38% and 99%, respectively. With due regard
to the conversion coecient of the base radiation into the
second harmonic there is no diculty to calculate that the
summary absorption in a pure crystal makes up 16% and
in a modied one it is 47%.
Let us estimate the radio signal amplitude. The specic
heat of LiNbO3with Fe2O3 is Cv 3 J/cm2 K, the
pyroelectric coecient at T 300 K is
gs 0:4
10 8 C/cm2 K. The irradiation is performed by a
laser pulse of 6 ns duration, with fronts of 1ns and energy
equal to 0.8 J. The summary portion of the absorbed radiation
for a modied crystal makes up 47%. The distance from the
crystal to the centre of the loop is R0 2.5 cm, the loop area
is S 2 cm2. After nding and I and I_ from the time charac-
teristics of the laser pulse (Fig. 1a), one can use Eq. (21) to
dene the magnitude ei  0:03V. Then the oscillograph signal
should be about U  0.3 V and that practically coincides with
the registered one.
8. Conclusions
1. The experiments described in the present paper made it
apparent that in good coincidence with the theory the
pulse heating of a ferroelectric induces electromagnetic
radiation.
2. The radio pulse energy increases with the decrease of the
front duration of the heating pulse as it is examplied
by the joint analysis of the results given in Ref. [3] and
the present work.
3. The radio pulse power can reach considerable values.
Further increase of the radiation power is possible when
the working temperature of a crystal approaches its Curie
temperature Tc. In this case, however, one should con-
stantly keep in mind that the relaxation time also
increases and that fact in turn might cause a decrease
of their radiated power. Therefore it is necessary to select
an optimum of the working temperature of the crystal
and this is one of the directions of our further
investigations.
4. It is assumed in this work that the only reason for the
change of the dipole moment is the heating of the sample.
However, the heating results in a hydrostatic presure jump
pt, that might inuence the polarization value [5,7] due
to striction and, consequently, on the radio pulse power.
5. The power of the signal from LiNbO3 with Fe2O3 can be
increased due to the inner conversion into the second
harmonic of the warming radiation within it with
l 1; 06 mm:
6. On the basis of the experimental results stated in this
work, it should be noted that the registration of the signal
might be conducted in the nearest zone and in the wave
Physica Scripta 60
282 V. V. Kolesov, Yu. V. Korobkin, I. V. Romanov, V. B. Studenoy and V. A. Davydov
zone as well. From this fact it is apparent that it is possible
to perform remote measurements of rapid temperature
drops and to use the above stated eect for the generation
of pulse SHF signals with time resolution dened by the
receiving channel, whereas the resolution of the tra-
ditional pyroelectric sensors depends on their electric
capacitance.
Acknowledgements
The research described in this report was made possible in part by RFFI
Grant No. 98-02-17386-a.
Physica Scripta 60
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# Physica Scripta 1999