Journal of the Korean Physical Society, Vol. 46, No. 1, January 2005, pp.

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Broad Doublet Spectra in SrTiO3

Mingqiu Tan, Yuhji Tsujimi and Toshirou Yagi
Research Institute for Electronic Science, Hokkaido University, Sapporo 060-0812, Japan (Received 5 August 2004) Broad doublet (BD) spectra have been investigated in quantum paraelectric SrTiO3 by a 180 Brillouin-scattering experiment. Spectral analyses suggest that the second-sound scenario seems to be unfavorable for explaining the physical origin of BD. We nd that the integrated intensity of BD shows quite strong anisotropy; the BD exists clearly around 27 K in the direction = 0.4 deviated from [001]c to [1 10]c , whereas the BD is almost absent in the direction = 21 . We also nd that the integrated intensity of the longitudinal acoustic mode decreases as increases, while that of the pure transverse acoustic mode increases. All these anisotropies can be explained by the conventional formula with Pockels tensor, signifying that the concept of antiphase-domain walls is not needed for such explanation.
PACS numbers: 77.84.Dy, 63.20.-e, 66.90.+r, 78.35.+c Keywords: Broad doublet, SrTiO3 , Brillouin scattering

I. INTRODUCTION SrTiO3 is a perovskite-type crystal exhibiting ferroelectric-transition-like features with decreasing temperature. The dielectric constant increases as the energy of the associated Brillouin zone center transverse optic (TO) mode decreases, following the classical CurieWeiss law. However, zero-point quantum uctuations prevent the condensation of the critical TO mode and the crystal remains paraelectric down to the lowest temperature. The material of this type is then called a quantum paraelectric (QPE) [13]. Of particular interest is the observation of an extra Brillouin-scattering doublet (BD: broad doublet) with a sound-like dispersion relation in QPE. This new excitation appears on top of the broad quasi-elastic central peak (CP) reported rstly by Lyons and Fleury [4]. The physical origin of BD was explained in terms of the second sound [5]. It was reported that the BD appears along [001]c , whereas it does not appear along [110]c . This anisotropy was attributed to antiphase-domain walls developing along [001]c [5]. However, much deeper studies are required to conrm the detailed features of this BD in various directions. In this report, the Brillouin scattering spectra on SrTiO3 along the directions between [001]c and [110]c were measured in the temperature range between 80 K and 15 K.

II. EXPERIMENTS

Brillouin-scattering experiments were performed on a commercial SrTiO3 single-crystal round specimen with diameter 10 mm and thickness 0.5 mm as shown in Figure 1. The crystal surfaces were perpendicular to the [001]c and [110]c directions. This orientation had enabled us to observe the light-scattering spectra in the 180 backscattering geometry with the scattering vector q spanned between [001]c and [110]c . In the setup, slight uniaxial pressure was applied perpendicular to the crystal surface, which made the c axis of the tetragonal domains formed below Ta = 105 K (cubicto-tetragonal phase transition temperature) prefer the orientation in the [001]c axis. The sample was mounted in a closed-cycle liquid-helium refrigerator. Brillouinscattering measurements were carried out in the temperature range from 15 K to 80 K with stability better than 0.1 K. For incident light, a longitudinal single-mode Ar+

Department

of Physics, Zhejiang University, Hangzhou 310027, P. R. China E-mail: yts@es.hokudai.ac.jp; Fax: +81-11-706-4965

Fig. 1. Schematic view of sample and measurement geometry for the Brillouin spectra of SrTiO3 . -97-

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Journal of the Korean Physical Society, Vol. 46, No. 1, January 2005

Fig. 2. Brillouin spectra for the broad doublet in SrTiO3 for = 0.4 (a), = 10.4 (b), and = 21 (c).

gas laser (SP BeamLok 2060) was used with a power of 70 mW at a wavelength of 514.5 nm. The polarization of the incident light was set along [110]c . The scattered light was collected and examined by a 3 + 3 pass tandem Fabry-P erot interferometer of Sandercock type. Polarization analysis was not made for the scattered light. The examined light was detected by a photomultiplier (Hamamatsu R585) and was stored in the memory of a multi-channel analyzer (ORTEC MCS-pci) as a spectrum after 3000-times accumulation. Figures 2(a), (b) and (c) show the temperature dependence of the Brillouin-scattering spectra of SrTiO3 with the scattering vector q pointed to the directions = 0.4 , = 10.4 , and = 21 , respectively. Here, is the angle measured from [001]c to [110]c on the (110)c plane. The BD peak around 20 GHz is clearly distinguished below 40 K in the spectra for = 0.4 and = 10.4 . However, in Figure 2(c) which corresponds to the spectra for = 21 we can not nd any obvious evidence of BD. This observation indicates that the BD is distributed within a very narrow angle around the [001]c axis, i.e., the BD is strongly anisotropic. In order to clarify the features in detail, we also performed Brillouin-spectra measurement at much higher angles, e.g., = 45 , and conrmed the disappearance of BD in this regime.

where ID , D , and D are the integrated intensity, damping constant, and natural frequency, respectively. The broad peak of CP and the sharp peaks of the LA, TA1 and TA2 phonons were also included in the tting. Here, LA means a longitudinal acoustic mode, and TA1 and TA2 mean transverse acoustic modes with displacement along [001]c and (001)c , respectively (TA1 is the pure mode and TA2 is the forbidden mode in the present scattering geometry). The spectral shape of BD has been tted reasonably well. The frequency BD is related to D and D via the following simple formalism: BD =
2 D

2 D . 2

Now we estimate the mean free path (MFP) of BD at 27 K. According to Hehlen et al. [5], the dispersion of BD is linear, i.e., vBD = BD , qBD

where vBD is the velocity, and qBD is the wave vector, which can be calculated from the measurement geometry and the wavelength of the laser beam, . In the backscattering geometry, qBD is related to = 514.5 nm and the index n = 2.47 of SrTiO3 directly: qBD = 4n ,

III. NUMERICAL FITTING AND ANALYSIS For a quantitative analysis of the BD spectra, a damped-harmonic-oscillator model was employed, which describes the line shape of BD as I ( ) =
2 ID D D , 2 2 ( D )2 + ( D )2

and the velocity vBD is therefore calculated to be 2500 m/s. The MFP of BD is evaluated as BD = vBD BD = vBD 2 51(nm). D

The observation wavelength O must fulll the window condition for second-sound excitation; N O R

Broad Doublet Spectra in SrTiO3 Mingqiu Tan et al.

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IV. CONCLUSIONS A 180 Brillouin-scattering experiment has been performed in order to investigate the broad doublet (BD) in SrTiO3 . In the paper of Hehlen et al. [5], more than two possible candidates for a theory of the mechanism of BD have been proposed. Among these candidates, the most hopeful ones are the second-sound model and the model of the two-phonon dierence scattering process on the TA sheet. We examine the window condition necessary for second-sound excitation from the spectral analyses. The second-sound scenario seems to be unfavorable for explaining the appearance of BD. We nd that the integrated intensity of BD shows a quite strong anisotropy. Moreover, it is found that the integrated intensity of the LA mode decreases as increases, while that of the pure TA1 mode increases. All these anisotropic features can be explained simply by the conventional formula with Pockels tensor. Therefore, the concept of antiphasedomain walls is unnecessary. Our results do not conict with the model of the two-phonon dierence scattering process.

Fig. 3. Ratio of integrated intensity of BD to that of LA as a function of angle at T 30 K and T 40 K.

[6]. Here, N and R are the MFPs of normal (momentum conserving) and resistive (momentum nonconserving) relaxations, respectively. O = 2/qBD is 104 nm in the present experiment, and R corresponds to BD = 51 nm. Second sound has been detected in NaF [7]. U was expected to be 10 m at 30 K in this material. If the value of U is applicable for SrTiO3 , N is estimated to be 110 nm by the formula N = U 1/2 [8], where is the dielectric susceptibility (8000 at 30 K). Clearly, the window condition cannot be fullled, meaning that our result seems to be unfavorable for the second-sound scenario. We nd that the integrated intensities of LA (ILA ) and BD (IBD ) have a tendency to decrease as increases. However, as for their angular dependences, the data are scattered. This is caused by the fact that the intensity measurement is aected by many factors (such as sample surface condition, interferometer adjustment, and so on). In order to remove this eect, the relative integrated intensity IBD /ILA is calculated near 30 K and 40 K. Figure 3 shows dependence of IBD /ILA . It seems that in the present experimental range, this ratio remains almost constant. We can say roughly that the angular dependence of ILA can be understood by a conventional formula taking Pockels tensor into account [9]. Thus, the anisotropy of IBD can be explained simply by this formula, which is evidence against an early suggestion that the anisotropy of BD originates from antiphasedomain walls aligned along [001]c . Moreover, our results indicate that the angular dependence of the integrated intensity of TA1 (IT A1 ) increases with an increase in and almost follows the conventional formula [A sin(2)]2 (Pockels tensor components appear in a proportional constant A). This is also evidence against the early suggestion. If the antiphase-domain walls reduce ILA and IBD as increases, they must also reduce IT A1 . However, this is against our result.

ACKNOWLEDGMENTS The authors express their appreciation to Mr. Tatsuji Meike for his regular improvement of the sample cell and for his technical advice. The present work has been supported in part by a Grant-in-Aid for Scientic Research (B) from the Ministry of Education, Science, Sports and Culture of Japan, No. 14340086.

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