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# The very high state accretion disc structure from the galactic black hole transient XTE J1550-564

## 1 Introduction

Accreting black holes in our Galaxy show a large variety of X-ray properties, which can be classified into distinct spectral states (Tanaka & Lewin 1995; McClintock & Remillard 2003, hereafter MR03). In the high/soft state, typically seen at luminosities above $`510`$ per cent of Eddington, the energy spectrum is dominated by a soft thermal component of temperature 0.4– 1.5 keV. This is well described by the standard accretion model of emission from an optically thick and geometrically thin disc (Shakura & Sunyaev 1973, hereafter SS73). Where the source varies, the temperature and luminosity of this disc component change together in such a way as to indicate that the size of the emitting structure remains approximately constant i.e. $`LT^4`$ (Ebisawa et al.  1991; 1994; Kubota, Makishima & Ebisawa 2001; Kubota & Makishima 2004; hereafter KM04; Gierlinski & Done 2004; hereafter GD04). Excitingly, this gives an observable diagnostic of the mass and spin of the black hole, assuming that this constant size scale is set by the innermost stable orbit around the black hole.

These results are actually very surprising in the context of the SS73 disc equations. The predicted disc structure is violently unstable at such luminosities, where radiation pressure dominates, yet these disc dominated spectra show very little short time-scale variability. Also, the disc spectrum should not be a simple sum of blackbody spectra at these high temperatures, as electron scattering dominates over true absorption. In the X-ray band, this difference in spectral shape can be roughly described as a standard disc spectrum, but of a higher temperature than the effective (blackbody) temperature (Shimura & Takahara 1995; Merloni et al. 2000). However, this colour temperature correction factor can change with luminosity, so is not predicted to produce a simple $`LT^4`$ relation (GD04).

Real discs are then observed to be much simpler than the SS73 predictions, pointing to the inadequacies of the ad hoc $`\alpha `$ viscosity prescription and motivating further studies of the disc structure which results from the physical (magnetic dynamo) viscosity mechanism in radiative discs (e.g. Turner 2004). This observed simplicity is reserved only for the high/soft state data, where the disc spectrum is dominant. Accreting black holes can also show a rather different type of spectrum at high luminosities, the so-called very high state termed the steep power-law state by MR03), characterized by a very strong (roughly) power-law component (Miyamoto et al. 1991). This is normally steep, with photon spectral index $`\mathrm{\Gamma }>2.2`$, rather different to the standard low/hard state spectra seen usually at much lower luminosities (e.g. the reviews by Tanaka & Lewin 1995; MR03). In this very high state, the constant area inferred from the relation between observed temperature and disc luminosity breaks down (Ebisawa et al. 1994; Kubota et al. 2001; KM04; MR03).

To some extent this breakdown is expected. The strong high energy emission shows that a large fraction of the accretion energy is dissipated in some non-disc structure (corona/jet?), so the disc structure should be different to that seen when the emission is dominated by the thermal disc spectrum (e.g. Svensson & Zdziarski 1994). Also, the intense X-rays may illuminate the disc, again changing its structure (e.g. Nayakshin, Kazanas & Kallman 2000). However, Kubota et al (2001) showed that for very high state spectra where the high energy emission was less than $`50`$ per cent of the total flux (which they termed the anomalous spectra), then the constancy of disc area could be (approximately) recovered by careful modelling of the spectrum, and by correcting the observed disc luminosity to include the Compton scattered photons (KM04).

Here we investigate the extremely Comptonised very high state spectra from the 1998 outburst of XTE J1550-564, where the steep power law tail dominates the total emission. This source has a superluminal jet (Hannikainen et al. 2001) and is a confirmed black hole with mass of 8.4–11.2 $`M_{}`$, at a distance of 5 kpc and binary inclination angle of $`70^{}`$ (Orosz et al.  2002).

We show that these extremely Comptonised very high spectra are qualitatively and quantitatively different to the spectra with a weaker Comptonised tail. They are not easily compatible with a simple Comptonising corona above an untruncated disc, though such a geometry may be possible with a complex corona, with strong radial gradients in the optical depth. However, the simplest solution is that the disc in these Compton dominated spectra is truncated at larger radii than the minimum stable orbit around the black hole.

## 2 Spectral evolution of XTE J$`1550564`$ in the 1998 outburst

The transient black hole binary XTE J$`1550564`$ was discovered on 1998 September 7 by RXTE ASM (Smith 1998) and CGRO BATSE (Wilson et al. 1998). This source showed four subsequent outbursts since its discovery, but the first outburst was the brightest and best covered by RXTE pointing observations. The data were analyzed by many authors including Sobczak et al.  (1999; 2000ab), Wilson & Done (2001), Homan et al. (2001), and KM04.

Figure 1 shows the 1.5–12 keV light curve and hardness ratios of the first outburst, obtained with RXTE ASM, together with the frequency of the main QPO (where seen) from Remillard et al. (2002). Clearly the source hardness changes dramatically during the outburst, as does the QPO frequency. These are generally correlated, so that spectral states can be defined either from spectral or power spectral characteristics (van der Klis 2000; MR03).

Here we briefly summerise the main features of the source behaviour. The marked softening of the spectrum in the first 5-10 days after the source was detected is associated with a state transition from the low/hard state (first five days) into the very high state (Wilson & Done 2000; Cui et al. 1999; Sobczak et al. 1999). For about a month (between days 5–52: Fig. 1), the source showed strong QPOs and a strong hard spectral component (e.g., Sobczak et al. 2000a), so can be classified as in the very high state during the whole of this time. The QPO frequency changes quite dramatically during the first $``$ 40 days of the outburst, but then stabilizes from day 40-52. The type of QPO also changes at day 40 (from C/C’ to B: see Remillard et al.  2002).

After the day 52, the luminosity and hardness both decreased as the source made a transition to the classic high/soft disc dominated (termed thermal dominated: MR03) state. Generally the QPO is not seen, but when it is detected, it is of different type (A, very weak: Remillard et al. 2002) to that seen previously. Most of the time until the end of this first outburst, the source stayed in this disc dominated high/soft state as the luminosity changed, giving progressively higher/lower disc temperatures and so higher/lower hardness ratios. There is just one section (days 180-200) where the hard power law flux again increased relative to the disc emission to a level comparable to that seen towards the end of the first very high state (days 40-52) and where the QPOs (mainly type B) reappear. Hence Homan et al. (2001) identify these data as very high state.

The luminosity and temperature of the disc component from day 40 onwards is always consistent with optically thick material extending down to the last stable orbit around the black hole (KM04, see also Figs 4b-d). In this paper, we concentrate our discussion on the very high state spectra where the coronal luminosity is $`>`$ 50% of the total i.e. days 5–40 of the outburst. We will show that these data are most easily described if the inner disc does NOT extend down to the last stable orbit, as also indicated by the QPO frequency. Hereafter, we distinguish these data from the other very high states in which the power law component is weaker (days 40–52, 180–200), and call it the ”strong very high state”. In Table 1, we summarize the correspondence of the spectral states we used in this paper to the state defined in other literatures.

## 3 Data reduction

We used all the data from the first outburst except for the first 5 days where the source is in the low/hard state. Good PCA and HEXTE data were selected and processed, following the same procedures as in KM04 and WD01, respectively.

For the PCA data reduction we used top and mid layer from all available units, using standard exclusion criteria (target elevation less than $`10^{}`$ above the Earth’s limb, pointing direction was more than $`1^{}.2`$ from the target, data acquired within 30 minutes after the spacecraft passage through South Atlantic Anomaly). The standard dead time correction procedure was applied to the data. The PCA background was estimated for each observation, using the software package pcabackest (version 2.1e), supplied by the RXTE Guest Observer’s Facility at NASA/GSFC. The PCA response matrix was made for each observation by utilizing the latest version (8.0) of the software package pcarsp. In order to take into account the calibration uncertainties, 0.5% systematic errors are added to each bin of the PCA spectra. A more conservative 1% systematic error does not qualitatively change the results, but gives very small values of $`\chi ^2/\mathrm{dof}`$. The 3–20 keV data are used in this paper, since there is sometimes residual structure in the 20–35 keV range associated with the Xe-K edge at $``$30 keV.

The HEXTE consists of two independent clusters (Cluster 0 and 1) of four NaI(Tl)/CsI(Na) phoswich scintillation counters (Rothschild et al. 1998). The HEXTE data were selected in the same way as that of the PCA. Since one detector on Cluster 1 of the HEXTE has lost its spectral capability, we use only Standard mode data from Cluster 0. The HEXTE background was subtracted by sequential rocking of the two clusters on and off of the source position. We used the software package called hxtback for splitting the data and the background. The HEXTE data below $`30`$ keV were not used in the spectral fit because of response uncertainties associated with the Xe-K edge111 see http://mamacass.ucsd.edu/hexte/calib/README.hexte\_97mar20. Systematic errors of 0.5% are also added to each spectral bin of the HEXTE, though these are much smaller than statistical errors of the HEXTE data in the range of 30–200 keV so make no difference to the spectral fits. Figure 2 shows the range of spectral shapes seen by the PCA and HEXTE data over the course of the outburst, taken from days of 13, 17, 36, 46, and 65 as denoted by the up-arrows in Fig. 1.

ASCA observations of this source were performed three times, on 1998 September 12, 24, and 1999 March 17, as indicated with down arrows in Fig. 1. There are simultaneous RXTE observations corresponding to each ASCA observation. The first simultaneous observation was just on the boundary of the low and very high state, while the third one was in the weak very high state (days 180-200). In this paper we are most interested in the strong very high state, so we choose to use only the second ASCA observation. The ASCA GIS events were extracted from a circular region of $`6^{}`$ radius centered on the image peak, after selecting good time intervals in a standard procedure. A net exposure of 2.4 ks was obtained for this simultaneous pointing. Dead time fractions are determined from count rate monitor data (Makishima et al. 1996) as 85.6% for GIS2 and 87.3% for GIS3. Systematic errors of 1% are added to each spectral bin. We only use the GIS data since the SIS is strongly affected by pileup.

The well known difference in calibration between the GIS and the PCA has been fixed in the PCA response matrices in HEASOFT 5.2. Thus the data are fitted simultaneously in this paper.

## 4 Analyses of the multiple RXTE data

### 4.1 Simple fits to the PCA data

In order to briefly characterize the spectral behavior throughout the outburst, we performed spectral fitting to the 3–20 keV PCA data with the canonical multicolour disc model (hereafter MCD model, diskbb in XSPEC; Mitsuda et al. 1984) plus a power-law model. The power-law component is modified by an absorption edge around 7–9 keV described by a smeared edge model (smedge in XSPEC; Ebisawa et al.  1994), and a narrow Gaussian is also added for the Fe-K line by constraining its central energy in the range 6.2–6.9 keV. The data of days 80–165 cannot constrain the power-law photon index so the index was fixed at 2.0, representing the mean HEXTE slope (Sobczak et al. 2000b; KM04). We fix the hydrogen column at $`N_\mathrm{H}=7\times 10^{21}\mathrm{cm}^2`$ as indicated by the ASCA data (see table 3), but otherwise the analysis is the same as in KM04.

Except for the data at the peak (day 13), this model fits the data adequately, and Table 2 gives the best fit parameters for the spectra shown in Fig. 2. Figure 3 shows the evolution of the spectral parameters as a function of time (as in Fig. 2 of KM04 but including the strong very high state data of the first 5–40 days as well). Panel (a) shows the bolometric luminosity of the disc, $`L_{\mathrm{disk}}`$, 1–100 keV power law luminosity, $`L_{\mathrm{pow}}`$ and total $`L_{\mathrm{tot}}L_{\mathrm{disk}}+L_{\mathrm{pow}}`$. Here, $`L_{\mathrm{disk}}`$ is calculated by referring to two parameters of the MCD model, inner disc temperature $`T_{\mathrm{in}}`$ (panel b) and an apparent inner disc radius $`r_{\mathrm{in}}`$ (panel c), as $`L_{\mathrm{disk}}=4\pi r_{\mathrm{in}}^2\sigma T_{\mathrm{in}}^4`$.

Figure 4a plots the derived disc luminosity against inner disc temperature for these fits. Clearly, $`L_{\mathrm{disk}}T_{\mathrm{in}}^4`$ in the standard high/soft state (magenta filled circles), indicating a constant area emitting region. Only the very lowest luminosity points deviate from this line, but the errors on these are fairly large as the low temperature disc is rather poorly covered by the PCA bandpass. When we fit these data points with a power-law, we obtain an index of $`3.9_{0.2}^{+0.1}`$ with a normalization at $`T_{\mathrm{in}}=1`$ keV of $`L_{\mathrm{disk}}=3.55\pm 0.08\mathrm{erg}\mathrm{s}^1`$. It is very tempting to identify the source of this markedly constant behaviour with the constant area defined by a disc extending down to the innermost stable orbit. When the apparent inner disc radius of $`r_{\mathrm{in}}=53`$ km derived from the fits is corrected for the stress–free inner boundary condition (Kubota et al. 1998) and colour temperature correction of 1.7 then this gives an estimate for the true inner disc radius of $`R_{\mathrm{in}}=63`$ km with a typical error of 10 %. This value is slightly smaller than 75–100 km, which is the innermost stable orbit for a non-spinning black hole of 8.4–11.2 $`M_{}`$. Therefore, XTE J$`1550564`$ is consistent with a moderately rotating black hole, while uncertainties of the source distance and determination of $`\kappa `$ can cancel this difference.

The behaviour of the disc component in the rest of the data is rather different. Fig. 4a shows that the strong very high state spectra (green open squares, days 5–30) have a much lower temperature disc than expected for the disc luminosity. Conversely the disc in the weak very high states has the disc at somewhat higher temperature than expected from its luminosity. In other words, the disc inner radius of the strong very high state appears at much larger values than that disc dominated regime, while that of the weak very high state is apparently found at smaller values. Inspection of Fig. 3(b)–(c) shows that this change in behaviour happens around day 30.

### 4.2 Fitting with the picture of the strong disc Comptonisation

The key characteristic of all the non high/soft state data is that the Comptonised tail is much more important in the spectrum (see Fig. 2), so details of how it is modeled become important. A power law approximation for the Comptonised spectrum is inadequate, as real Compton spectra show a low energy turnover close to the seed photon energy (KM04; Done, Zycki & Smith 2002). We replace the power law with a proper thermal Comptonisation model (thcomp777http://www.camk.edu.pl/~ptz/relrepr.html in XSPEC: Zdziarski, Johnson & Magdziarz 1996) which is parameterized by asymptotic power law index, $`\mathrm{\Gamma }_{\mathrm{thc}}`$, and electron temperature, $`T_\mathrm{e}`$. We assume that the seed photons are from the observed MCD component, so $`T_\mathrm{e}`$ is the only additional free parameter compared to the previous power law fits.

We use the PCA and HEXTE data in order to better constrain $`T_\mathrm{e}`$, but this broad bandpass shows that the spectra are rather more complex than a single thermal comptonisation component (and its reflected emission). While the data below 20 keV can be dominated by the disc and a cool thermal Compton component, the higher energy data show a quasi-power law tail (Gierlinski et al. 1999; Zdziarski et al. 2001; WD01; Kubota et al. 2001; Gierlinski & Done 2003; KM04). We follow KM04 and model this additional component as a power law with photon index $`\mathrm{\Gamma }`$ fixed at 2.0 which is the average index of the high energy emission in the standard high/soft state (e.g. fits to HEXTE data: Sobczak et al. 2000b), and fit all the PCA+HEXTE data with this three component continuum model; MCD plus thermal comptonisation (thcomp) plus power law, with the gaussian line and smeared edge to mimic reflection. All the model parameters are constrained to be the same between the PCA and the HEXTE data except for a normalization factor.

This three component model successfully reproduced all the spectra, and the electron temperature of the Comptonised component was found at 10–30 keV in all the very high state data, except for that at the peak (day 13) where the temperature is considerably higher at $`60`$ keV. This means that the thermal rollover in the spectrum is not so obvious in the PCA-HEXTE bandpass. Nonetheless, the complex continuum model (thermal plus non-thermal) is still strongly preferred by the data compared to a single Comptonised component. Thus it seems likely that the peak spectrum is simply a more extreme version of the surrounding very high state spectra. Alternatively it could contain an additional component such as an X-ray contribution from the jet, whose radio emission suddenly increased at this time (day 13), peaked on day 15, and decayed to quiescent level through day 18 (e.g., Wu et al.  2002).

Figure 5 shows the evolution of the spectral parameters with time, while the resulting luminosity/temperature diagram is shown in Fig. 4b. The change in derived disc parameters for spectra shown in Fig. 2 are given in Table 2. The disc temperature increases dramatically for the strong very high state spectra (days 5–30, green open squares), while for the weak very high state spectra (days 40–52 shown as blue open circles), it is the disc luminosity which increases. The net effect is to pull all the Comptonised spectra much closer to the constant radius behavior seen in the standard high/soft state (magenta filled circles: Fig. 4b). This looks very promising for models in which the disc structure remains rather stable in all the high state spectra, with constant apparent inner disc radius.

However, the Comptonised luminosity is indeed very large compared to that of the disc in the very high state, making it likely that the corona covers a fairly large fraction of the disc. In this case the corona is in the line of sight and intercepts some of the disc photons, so the observed disc luminosity underestimates the intrinsic disc luminosity, $`L_{\mathrm{disk}}^{\mathrm{int}}`$. The energy transfer by Compton scattering can be characterised by the Compton $`y`$ parameter, which is $`4\tau ^2kT_e/mc^2`$ (e.g., Rybicki & Lightman 1979). If this is small then $`L_{\mathrm{disk}}^{\mathrm{int}}`$ is roughly consistent with $`L_{\mathrm{disk}}+L_{\mathrm{thc}}`$ (Kubota et al. 2001; KM04). Figure 4c shows this luminosity plotted against $`T_{\mathrm{in}}`$. As shown by KM04 this puts the weak very high state (anomalous regime ; days 40–52) data onto the same constant radius line as the standard regime data, while the strong very high state lies significantly above these points.

For the strong very high state, the Compton energy boost is not negligible. Instead, we estimate $`L_{\mathrm{disk}}^{\mathrm{int}}`$ by conservation of photon number, as the photons in the Comptonised spectrum came originally from scattering of seed photons from the disc. Figure 6 shows two simple corona geometries for the very high state, a sphere and a slab, respectively, above an untruncated disc. The intrinsic number of disc photons, $`N_{\mathrm{disk}}^{\mathrm{int}}=N_{\mathrm{disk}}+aN_{\mathrm{thc}}`$, where values of $`a`$ are $`2\mathrm{cos}i`$ and 1, for spherical and slab geometries, respectively (KM04), assuming that the seed photons from the disc have the same disc blackbody spectrum as is observed. Thus, the intrinsic disc emission can be estimated by

$`L_{\mathrm{disk}}^{\mathrm{int}}`$ $`=`$ $`L_{\mathrm{disk}}N_{\mathrm{disk}}^{\mathrm{int}}/N_{\mathrm{disk}}`$ (1)
$`=`$ $`bT_{\mathrm{in}}N_{\mathrm{disk}}^{\mathrm{int}}`$ (2)
Here, the value of $`b`$ is defined as $`bT_{\mathrm{in}}N_{\mathrm{disk}}=L_{\mathrm{disk}}`$, and via equation (A1) in KM04, it is given as

$$b=1.31\times 10^9\frac{2\pi D^2}{\mathrm{cos}i}\mathrm{erg}\mathrm{keV}^1\mathrm{photons}^1\mathrm{cm}^2,$$
(3)
for the bolometric (0.01–100 keV) photon fluxes, $`N_{\mathrm{disk}}`$ and $`N_{\mathrm{thc}}`$.

Figure 4d shows this estimate for $`L_{\mathrm{disk}}^{\mathrm{int}}`$ (calculated for a spherical geometry) plotted against $`T_{\mathrm{in}}`$, while Fig. 5c shows the conversion of $`L_{\mathrm{disk}}^{\mathrm{int}}`$ into apparent inner disc radius. It is clear that the weak very high state (anomalous regime) data are now easily consistent with the same constant $`r_{\mathrm{in}}`$ seen in the standard high/soft data, but the strong very high state, where the Comptonised luminosity is more than $`50`$% of the total flux, are well above the line. This is highly unlikely to be due to a changing colour temperature correction, as it requires a smaller colour temperature correction than that in the standard high/soft state (see §6). Thus either the disc inner radius is increasing, or the corona is much more complex than modelled here.

## 5 Simultaneous ASCA-PCA-HEXTE data

One obvious caveat of the spectral modelling is that the low temperatures inferred for the strong very high state mean that the disc spectrum is not well covered by the PCA bandpass which starts only at $``$3 keV. Hence we use the simultaneous ASCA GIS data to extend the soft energy response. We use the same three continuum component model and fitting conditions as above, except that the value of $`N_\mathrm{H}`$ is now a free parameter. Same as in §4.2, except for a normalization factor, all the model parameters are constrained to be the same between the GIS, the PCA and the HEXTE data. Table 3 shows the fitting results. Figure 8 shows the raw data and the residuals between the data and the model, and Fig. 8 shows an unfolded spectrum with the model. The model fits the simultaneous data very well with $`\chi ^2/\mathrm{dof}=150.4/186`$. The best fit value of $`T_{\mathrm{in}}=0.54\pm 0.02`$ keV is much more tightly constrained, and its central value is slightly shifted to lower temperature than $`0.65_{0.04}^{+0.08}`$ keV derived from the RXTE data alone.

In order to check the results with a more physical model, we replace the phenomenological line and smeared edge spectral features with the full reflection code included in the thcomp model (Zycki, Done & Smith 1998). We fix the inclination and iron abundance at $`70^{}`$ and solar abundance, respectively. These fit results are shown as model (b) in Table 3. The derived reflection parameters look somewhat unphysical, with a large amount of mostly neutral reflection. This is probably due to limitations of the reflection modelling for an ionized disc in thcomp, which is based on the pexriv reflected continuum calculations (Magzdiarz & Zdziarski 1995). These codes calculate the ionisation balance in a very simplistic way (Done et al. 1992), assumming it to be constant throughout the disc rather than varying as a function of height (Nayakshin et al. 2000; Ballantyne, Ross & Fabian 2001).

Another issue is that these models assume that Compton upscattering is negligible below 12 keV. However, for ionised material this can be very important in determining the iron line and edge structure observed (Ross, Fabian & Young 1999). While more accurate ionised reflection models are available for spectral fitting (Nayakshin et al. 2000; Ballantyne, Iwasawa & Ross 2001), they assume a very simple continuum form (power law, or power law with exponential cutoff) which means they cannot accurately describe the complex spectral shape observed in these very high state data. Instead, we estimate the impact of this uncertainty in the reflection modelling by removing the iron line and edge region (5–12 keV) and refitting the data with the thcomp reflected continuum with an ionization parameter, $`\xi `$, fixed at $`10^2`$, $`10^3`$ and $`10^4`$, (models (c), (d) and (e) respectively in Table 2).

The disc luminosities and temperatures derived from the series of models (a–e in Table 2) are plotted as filled black squares on the $`TL`$ plots (Fig. 4b–d). These show the range of systematic uncertainties present from the spectral modelling. However, all of the fits detailed in Table 2 have an even lower disc temperature than that derived from fits to the PCA+HEXTE data, but with a similar luminosity. These show even more clearly that the strongly Comptonised spectra are not easily consistent with an untruncated disc. For the simple corona geometries of Fig. 6, then in order to explain the high inferred intrinsic disc luminosity, $`L_{\mathrm{disk}}^{\mathrm{int}}2`$$`3\times 10^{38}\mathrm{erg}\mathrm{s}^1`$, with the same disc radius as seen in the standard high/soft state requires $`T_{\mathrm{in}}>`$ 0.85–0.9 keV. By contrast, the 99.9% upper limits ($`\chi ^2/\mathrm{dof}=1.35`$ for dof of 186–188) of the disc temperature from the ASCA-PCA-HEXTE data is $`<0.66`$ keV for all the models (a–e) in Table 2. Fixing $`T_{\mathrm{in}}=0.85`$ keV results in completely unacceptable fits ($`\chi ^2/\mathrm{dof}`$ =4.6–5.6).

More conservatively, even when the systematic errors of the PCA data and the HEXTE data increased to 1 %, the 99.9 % upper limit is still lower than 0.69 keV. Since deviations between the modeled and measured Crab spectrum do not exceed 1 % as noticed by many authors including Revnivtsev et al.  (2003), $`T_{\mathrm{in}}=0.69`$ keV can be considered as the securest upper limit of the disc inner temperature. It is clear that the low disc temperature derived in the strong very high state spectra from the PCA+HEXTE fits are not due to lack of PCA coverage of the disc spectrum, or the spectral modelling of the reflection emission.

## 6 Discussion

We have shown that the strong very high state spectra really do have a rather low temperature disc for its luminosity. These observations suggest that the disc is truncated at larger radii than the last stable orbit in the strong very high state. However, this is based on the assumptions that (1) the correction factor of color to effective temperature is kept approximately constant, and (2) the corona fully covers the disc as illustrated in Fig. 6

### 6.1 Change of color temperature correction

Figure 5c represents the time history of the apparent inner radius $`r_{\mathrm{in}}`$, as derived from the temperature and luminosity values given in Fig. 4d. The true inner radius $`R_{\mathrm{in}}`$ is related to $`r_{\mathrm{in}}`$ as $`R_{\mathrm{in}}\kappa ^2r_{\mathrm{in}}`$, where $`\kappa `$ is the colour temperature correction. For constant $`\kappa `$, the observed variability of $`r_{\mathrm{in}}`$ is just caused by change of the inner radius. However, a change in the colour temperature correction could be expected as a function of disc luminosity (Merloni et al. 2000; GD04; Kawaguichi 2003), and illumination of the upper layers of the disc (Nayakshin et al. 2000) and/or conductive heating could also lead to an increase in $`\kappa `$.

Close inspection of Fig. 4d shows that the data points corresponding to the weak very high state (anomalous regime) are slightly lower than the solid line denoting constant $`r_{\mathrm{in}}`$. Although this is not very significant, it could perhaps indicate a constant radius disc with slightly higher colour temperature correction. Conversely, the disc in the strong very high state requires a decrease in colour temperature correction by a factor of $`60`$% i.e. $`\kappa 1`$. This would imply that the observed colour temperature was the same as the effective disc temperature, which is only possible when true absorption opacity dominates over electron scattering. This cannot be the case at the observed $``$0.5 keV temperatures. Changing $`\kappa `$ cannot explain the strong very high state spectra with the disc with a constant radius.

The above discussion assumed that the disc spectrum can be described by a simple colour temperature correction. Plainly this may not be the case, and the disc spectrum could be completly distorted, for example if the inner disc colour temperature correction were much higher than at outer radii. The spectrum would then look like a low temperature disc with some fraction of the emission at much higher temperature. This is exactly what these strong very high state spectra look like, so we examine the effect of Comptonization as a function of radius on the disc spectrum below.

### 6.2 Geometry and energetics of the corona

So far, we assumed the corona fully covers the disc as illustrated in Fig. 6. However several other geometries can be considered, as illustrated in Fig. 9. If the corona is out of our line of sight to the disc e.g. a small inner region, perhaps physically representing an inner jet or bulk Comptonisation of the infalling material (see Fig. 9a and b), then the Compton scattering does not affect the observed disc flux, so the correction used above overestimates the intrinsic disc emission. The problem of such a geometry is that the Comptonising region would see many fewer disc photons than an observer, in conflict with the data (see Tables 2 and 3). Even without this problem, the best that such a geometry could do is reduce the estimated intrinsic disc luminosity to that observed (i.e. where none of the disc photons in our line of sight are intercepted). This puts us straight back to Fig. 4b, where the ASCA+PCA+HEXTE data show a much lower temperature disc than expected for its luminosity in the very high state.

Alternatively, the corona could be patchy (Fig. 9c), or cover only the inner disc (Fig. 9d). In both these geometries the corona is in the line of sight to the disc, so again this predicts that the Compton scattered photons we see are removed from the observed disc emission. The intrinsic disc emission should still be estimated as in Fig. 4d. While the patchy corona could take photons uniformly from the whole disc, the inner corona (Fig. 9d) would preferentially take only the inner disc (highest temperature) photons, perhaps leading to an underestimate of the disc temperature. This is analogous to having a variable colour temperature correction with radius (see above). We model this by switching the seed photons in thcomp to blackbody (rather than the MCD), and allow the temperatures of the observed inner disc and seed photons to be different. This gives a very strong upper limit on the seed photon temperature for the ASCA-PCA-HEXTE data of $`<0.6`$ keV, showing that the low disc temperature is not an artifact of the seed photon distribution assumed.

However, the existence of the corona changes the disc temperature structure. In the limit of a corona that covers the whole disc then this has little effect as both the disc luminosity and temperature are reduced (Svensson & Zdziarski 1994), but for an inner disc corona the behaviour is more complex. Only the inner disc temperature and luminosity are reduced, but these form the seed photons for the Compton scattering. For a fraction $`f`$ of the total accretion power dissipated in the corona, the inner disc temperature is reduced by a factor $`(1f)^{1/4}`$ (Svensson & Zdziarski 1994). This is an underestimate of the inner disc temperature as it intercepts and reprocesses a large fraction (up to a half) of the coronal flux. We will do more detailed modelling of this in a subsequent paper, but estimate that the size of this effect is not enough to make the temperature and luminosity consistent with the standard high/soft state radius disc.

## 7 A scenario for the disc evolution in the 1998 outburst of XTE J1550-564

### 7.1 A scenario derived by spectral studies

The discussion above shows that there are no easy alternatives to the conclusion that the inner disc is truncated in the strongly Comptonised very high state spectra. If so, then there must be some overlap between the inner hot region and the truncated disc in order for it to intercept enough seed photons, but the larger radius disc can trivially produce the lower observed disc temperature at high luminosity. This geometry is rather similar to the truncated disc/hot inner flow inferred for the low/hard state, so would give a physical basis for the well known similarities between the very high state spectra and the intermediate state spectra (seen towards the very end of the low/hard state; Belloni et al. 1996; Mendez et al. 1997). It could also explain the lower frequency QPO seen in the very high state (e.g. the review by van der Klis 2000; di Matteo & Psaltis 1999).

A schematic picture for the whole disc evolution during the 1998 outburst of XTE J$`1550564`$ is shown in Fig. 10. The outburst starts in the low/hard state, with a truncated disc, and hot inner flow (panel a). The increase in mass accretion rate increases the optical depth of the inner flow before the inner disc has time to form, leading to an optically thick, cooler inner flow and truncated disc (the strongly Comptonised very high state, panel b) on $``$day 5 (WD01). During days 5–30, the fraction of energy dissipated in the corona to that from the disc is kept almost constant (Fig. 5f), while $`T_\mathrm{e}`$ and $`\mathrm{\Gamma }_{\mathrm{thc}}`$ of the corona changed with time (Fig. 5d and e). Through this period, the X-ray flux reached at the peak (day 13). The radio flare was observed at this time with a continuance of 5 days, and VLBA image showed evolving structure (Hannikainen et al.  2001).

During days 30–40 the inner disc is able to form at progressively smaller radii, perhaps due to the correlated decrease in fractional power dissipated in the corona (see Fig. 5f) which reduces the coronal heating/irradiation. The disc finally reaches the last stable orbit at around day 40, causing a noticeable change in disc temperature behaviour despite little change in luminosity (Fig. 5b). The power dissipated in the corona continues to drop, leading to more weakly Comptonised spectra above the untruncated disc (the weak very high state, anomalous regime; days 40-52). This eventually becomes a small ($`<`$ 20%) fraction of the total power, giving the standard high/soft state (after day 52, panel e). This is similar to the geometry for the spectral states proposed by Esin et al. (1997), except that the strongly Comptonised very high state spectra corresponds here to a truncated disc.

While this gives a good overall description of the properties of XTE J$`1550564`$ during its outburst, the remaining problem is what makes the truncated disc with the strong Compton corona. Advection dominated accretion flows cannot be maintained at such high luminosities (e.g. Esin et al. 1997), although these are only an approximation to the complex nature of the optically thin, hot flow which is predicted from numerical simulations (Hawley & Balbus 2002). Physically, such truncation could arise from disc overheating (Beloborodov 1998), or by strong conduction/irradiative heating from the corona, or, perhaps most attractively, by disruption of the inner disc by jet formation. However, the total mass accretion rate cannot be the trigger for this behaviour since (apart from the peak) the very high state spectra have total luminosity which is similar to that in the disc dominated regime seen in days 100–180. Therefore some other parameters are required to drive the structural changes in the disc (see e.g. van der Klis 2001; Homan et al.  2001; MR03)

### 7.2 Consistency with the QPO behavior

The type of QPO seen is roughly consistent with the changes in geometry shown in Fig. 10, and with the spectral state (Table 1) as suggested by Homan et al.  (2001) based on the spectral hardness ratio. Since the QPO frequencies are thought to reflect the size of the Comptonising region and the disc inner radii, it is meaningful to compare evolution of the QPO frequencies with that of disc inner radii estimated by the spectral analyses. As we can see in Fig. 1, through day 18–30, the frequency of the low-frequency QPO increased from $`2.7`$ Hz, and after the day 30, it was almost kept constant at $`6`$ Hz. This is very consistent with the decrease in $`r_{\mathrm{in}}`$ derived from the spectra through days 5–40 as shown in Fig. 5c. Indeed, Homan et al.  2001 suggested almost the same scenario of evolution of the accretion disc based on the QPO behavior.

However, there is some inconsistency between the timing and the spectral behavior before day 18. On one hand, the low-frequency QPO increased to $`10`$ Hz around the peak (day 13). This frequency is higher than the $`6`$ Hz which was observed after days 30–40, suggesting that the disc extends closer to the black hole during the peak. Yet the X-ray spectra imply that the disc extends down to the last stable orbit during days 30–40 and truncates at larger radii during the peak(Fig. 5c). Moreover, the high-frequency QPO which is sometimes seen in the very high state data (Fig. 1) shows rather different behaviour. In Fig. 4, we marked the data points which have high-frequency QPOs with big open diamonds. Some green open squares showed both the characteristics of large inner radius by the spectral fits and the high frequency of the QPOs. Therefore, the QPO and the spectral behavior are not easily consistent, pointing either to a lack of understanding of how QPOs and/or disc spectra relate to the inner radius.

As a brief comment, the strong very high state data with high frequency QPO and the low-frequency QPOs of the higher frequencies may be considered to be relate to the jet ejection. As described in § 4.2, the radio flux was observed to increase suddenly at day 13, the peak of X-ray flux (Wu et al.  2002), and the extending radio jet was reported on day 15 by Hannikainen et al.  (2001). In Fig.4, the data points which show strong radio emission were also marked with big circle plus cross. Thus, the data with high-frequency QPO can be understood to have some relation to the jet ejection.

## 8 Summary and Conclusions

The disc dominated high/soft state of Galactic black holes can be well modelled by a disc of constant inner radius and colour temperature correction. This most probably indicates that the disc extends down to the innermost stable orbit around the black hole. This is clearly seen in the 1998 outburst of XTE J$`1550564`$. However, the strongly comptonised very high state spectra seen at the start of the outburst do not follow this trend. Careful modelling of these spectra show that the disc temperature is somewhat lower than expected for the observed disc luminosity for a constant radius disc. Correcting the disc luminosity for the effects of Compton scattering in a disc-corona geometry make this discrepancy much more marked. We discuss the effects of changing colour temperature corrections, and different geometries, but none of these can convincingly reproduce the observed disc temperatures and luminosities. We will model the effects of a more complex coronal geometry (e.g. one with strong radial gradients in optical depth: Fig. 9d) in a subsequent paper, but the simplest solution is that the inner disc is truncated in the strong very high state.

### Acknowledgements

The authors would like to thank an anonymous referee for his/her detailed comments. The present work is supported in part by a Sydney Holgate fellowship in Grey College, University of Durham, JSPS Postdoctoral Fellowship for Young Scientists, and by JSPS grant of No.13304014. A.K. is supported by special postdoctoral researchers program in RIKEN.


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# Search for a Θ⁺⁺ Pentaquark State

## 1 The search for the $`\mathrm{\Theta }^{++}`$

The constituent quark model does not exclude pentaquark systems. Until recently, only bound triplet-quark and quark-antiquark systems have been found. A possible candidate for a pentaquark system is the $`\mathrm{\Theta }^+`$, with strangeness S=+1. Recent experimental evidence  may suggest the existence of such a pentaquark system, previously predicted by the chiral soliton approach to hadron dynamics . Thus the search is on for a family of pentaquark systems. Theoretical predictions of a family, including $`\mathrm{\Theta }^{}`$, $`\mathrm{\Theta }^0`$, $`\mathrm{\Theta }^+`$, $`\mathrm{\Theta }^{++}`$, and $`\mathrm{\Theta }^{+++}`$, have been published, for instance .

In 2000, we analyzed the CLAS g1a data  and searched for the $`\mathrm{\Theta }^{++}`$ in an exclusive measurement of the reaction $`\gamma `$p$``$K+K-p, as a by-product of a hyperon-resonance analysis . The $`\mathrm{\Theta }^{++}`$ may be found in the reaction $`\gamma `$p$``$K$`{}_{}{}^{}\mathrm{\Theta }_{}^{++}`$ with an assumed strong decay $`\mathrm{\Theta }^{++}`$K+p. Thus, we require the exclusive identification of all three particles in the final state, namely, p, K+, and K-. We searched for a structure in the mass distribution between 1.5 GeV/c2 and 1.6 GeV/c2. The range is based on theoretical predictions. The only structure that we found in this mass region was at 1.59 GeV/c2 which we label “$`\mathrm{\Theta }^{++}`$”. We then tried to understand the origin of this structure. After evidence for a $`\mathrm{\Theta }^+`$ was found and the physics community was more interesting in the $`\mathrm{\Theta }^{++}`$, we received several requests that encouraged us to present the result of this analysis in light of recent findings.

The photon beam energy range of the g1a data set is Eγ = 0.5 GeV to 2.4 GeV. The threshold for the reaction $`\gamma `$p$``$K$`{}_{}{}^{}\mathrm{\Theta }_{}^{++}`$ is Eγ = 1.85 GeV, assuming a mass $`m_{\mathrm{\Theta }^{++}}=1.59`$ GeV/c2. Here we take the peak center position of the $`\mathrm{\Theta }^{++}`$ mass distribution which we find below. In the first iteration, no cut was applied on Eγ, but for the final analysis only events above the threshold are selected. Even if the $`\mathrm{\Theta }^{++}`$ mass were to differ by a few tens of MeV, because we cover a wide energy range up to about 0.5 GeV above the threshold, the effect on the mass distributions shown in this paper is negligible. For the search for the $`\mathrm{\Theta }^{++}`$, the energy range covered by the measurement presented in this paper is most interesting, because the cross section for the reaction $`\gamma `$p$``$K$`{}_{}{}^{}\mathrm{\Theta }_{}^{++}`$ would very likely reach its maximum within this range. We discuss the $`\mathrm{\Theta }^{++}`$ mass below.

Figure 1 shows the missing mass $`m_X`$ from $`\gamma `$p$``$K-X versus the invariant mass $`m_{(K^+,p)}`$ from $`\gamma `$p$``$K-K+p for the selected events. The same distribution is presented in Fig. 2 lego plot format. The X– and Y–projection of this distribution are shown in Fig. 3 and 4. Notice that the missing mass $`m_X`$ in Fig. 4 comes from the p and $`K^+`$ since both particles are required by the event selection although they are not used for the calculation of $`m_X`$. A bump can be seen at about 1.59 GeV/c2 in Fig. 1, 3 and 4. The missing mass distribution contains a flat background, wherein some events have an occasional missing mass $`m_X`$ below the total of m$`_\mathrm{K}^{}`$ \+ m$`_{\mathrm{K}^+}`$ \+ mp. These events most likely arise from particle misidentification. We can also see these event in Fig. 2 below the diagonal. There are two groups of background reactions, namely $`\gamma `$p$`\pi ^{}`$K+p from $`\mathrm{\Lambda }`$ and $`\mathrm{\Sigma }^0`$ production and $`\gamma `$p$`\pi ^{}\pi ^+`$p. The cross sections for these reactions are significantly larger than the cross section for double-kaon production. Thus, the result is not surprising. This is the most important reason to make an exclusive measurement and not to rely on the missing mass distribution only.

We utilize four-momentum conservation as an additional event selection criterion. Because this is an exclusive measurement, it is possible to look at the missing mass $`m_X`$ as well as the invariant mass $`m_{(K^+,p)}`$ without fixing the mass of the $`\mathrm{\Theta }^{++}`$. We merely require that the missing mass and invariant mass be identical within some reasonable range. This is achieved by a cut on $`|m_Xm_{(K^+,p)}|35`$ MeV/c2. In Fig. 1 and 2, which show $`m_X`$ plotted against $`m_{(K^+,p)}`$, this would be a 35 MeV/c2 broad diagonal cut. This cut removes the background which does not conserve the four-momentum and is not on the diagonal. No cut on the particle momentum or any other kinematic cut has been applied.

The result of the cut $`|m_Xm_{(K^+,p)}|35`$ MeV/c2 is shown in Fig. 5. The dashed line shows the invariant mass $`m_{(K^+,p)}`$ distribution from Fig. 3, while the solid line represents the distribution after we apply the cut. The peak at $`m=`$ 1.59 GeV/c2 is our “$`\mathrm{\Theta }^{++}`$ signal”, which is in good agreement with the prediction of . The signal-to-background ratio has been improved. The number of events, however, is small. From a fit to the $`\mathrm{\Theta }^{++}`$ signal with a normal distribution plus a constant offset as background, we get a mass $`m_{\mathrm{\Theta }^{++}}=m_{(K^+,p)}`$ of 1.59 GeV/c2 with a width $`\sigma _m`$ of 0.01 GeV/c2, $`\mathrm{\Gamma }_m`$ is about 0.025 GeV/c2.

This analysis of the reaction $`\gamma `$p$``$K$`{}_{}{}^{}\mathrm{\Theta }_{}^{++}`$ preceded the recent experimental discoveries of the $`\mathrm{\Theta }^+`$ by some three years. The $`\mathrm{\Theta }^+`$ mass shows a wide spread between 1.527 GeV/c2 and 1.555 GeV/c2 with a width of up to 0.032 GeV/c2 . The current average of the $`\mathrm{\Theta }^+`$ mass from all experiments is about 1.54 GeV/c2. The width $`\mathrm{\Gamma }_m`$ of 0.025 GeV/c2 for the $`\mathrm{\Theta }^{++}`$ is well within the range seen by other CLAS experiments for the $`\mathrm{\Theta }^+`$ . The range of 1.5 GeV/c2 to 1.6 GeV/c2 for the $`\mathrm{\Theta }^++`$ search may be too broad, compared to recent experimental results for the $`\mathrm{\Theta }^+`$ mass, but we also need to take into consideration that the isospin mass splitting for a pentaquark system with strangeness S=+1 is currently unknown.

## 2 The origin of the $`\mathrm{\Theta }^{++}`$ signal

We now must evaulate the question whether this “$`\mathrm{\Theta }^{++}`$ signal” is real or an artifact. It is unlikely that the peak is the result of an enhancements caused by a combination of the momentum spectra from two particles because of the large acceptance of CLAS and the fact that we apply only basic cuts. No special cut on the particle momentum is applied. But CLAS does cut off low-momentum particles. The minimum momentum for particle identification is $`p`$ $`\stackrel{>}{}`$ 0.2 GeV/c.

Figure 1 shows that the signal is far away from most of the mass distributions where the data might be severely affected by the experimental acceptance and limited total energy. But the mass distributions may be slightly shifted by a few MeV/c2, due to the momentum-dependent acceptance of CLAS.

Particle misidentification is always an issue. In particular, the separation of pions and kaons with CLAS is difficult. However, the exclusive measurement and the lack of any missing particle significantly reduce the likelihood of particle misidentification. A pion misidentified as a kaon would result in a violation of the four-momentum conservation, and there is little phase space left to make up the difference because of the lack of any undetected heavy particle. If we had, for example, a reaction in which there was a missing neutron in the final state, then the large missing mass and uncertainty of the momentum measurement would increase the probability that a particle misidentification remains undetected. Analyses where a kinematical fit is used to constrain the particle momentum are especially susceptible to such misidentification. This is yet another reason that we chose an exclusive measurement instead of an inclusive measurement with better statistics.

For this analysis, we do not have to deal with complicated production mechanisms either. There is no spectator and no scattering of a final-state particle on a spectator or on any other particle. Also Fermi motion is of no concern for this analysis, because the target is a free proton instead of a deuteron.

But we do have to identify possible reflections from other reactions; there are various reactions possible with a p, K+, and K- in the final state. The obvious candidates are $`\gamma `$p$``$K$`{}_{}{}^{+}\mathrm{\Lambda }(1520)`$, $`\gamma `$p$``$K$`{}_{}{}^{+}\mathrm{\Lambda }(1670)`$ with $`\mathrm{\Lambda }^{}`$K-p and $`\gamma `$p$`\varphi `$p with $`\varphi `$K+K- .

First, we search for $`\varphi `$ production in the events within the $`\mathrm{\Theta }^{++}`$ signal. The invariant mass $`m_{(K^+,p)}`$ versus the invariant mass $`m_{(K^+,K^{})}`$ is shown in Fig. 6. The Y– and X–projection of Fig. 6 are shown in Fig. 7 and 8 respectively. We cut on the $`\mathrm{\Theta }^{++}`$ peak, select the corresponding events below the peak and require $`m_{(K^+,K^{})}^2>0`$. The selected events are indicated by the dashed line in Fig. 7. We then look at the invariant mass $`m_{(K^+,K^{})}`$, shown in Fig. 8. Figure 6, 7, and 8 indicate that there is a substantial fraction of $`\varphi `$ production in the group of “$`\mathrm{\Theta }^{++}`$” events.

To consider hyperon resonance production, the test is also applied the other way around. It turns out that the $`\mathrm{\Lambda }(1670)`$ is of no importance for this test. Only the results for $`\mathrm{\Lambda }(1520)`$ are shown in Fig. 9 and 10. We apply two cuts, namely $`|m_Xm_{(K^{},p)}|<35`$ MeV/c2 for $`\gamma `$p$``$K+X and $`|m_Xm_{(K^+,p)}|<35`$ MeV/c2 for $`\gamma `$p$``$K-X. In Fig. 9 and 10 we compare the $`\mathrm{\Theta }^{++}`$ signal in $`m_{(K^+,p)}`$ for $`\mathrm{\Lambda }(1520)`$ production events and the rest. The “$`\mathrm{\Theta }^{++}`$” peak in Fig. 9 from $`\mathrm{\Lambda }(1520)`$ production is very small. Most of the “$`\mathrm{\Theta }^{++}`$” signal in 10 comes from events which were not identified as $`\mathrm{\Lambda }(1520)`$ production.

## 3 How much of the “$`\mathrm{\Theta }^{++}`$” signal is left

We select events from $`\varphi `$, $`\mathrm{\Lambda }(1520)`$ and $`\mathrm{\Lambda }(1670)`$ production as described before and remove these events from the “$`\mathrm{\Theta }^{++}`$” mass distribution. Then we compare the distributions.

The top (solid) line in Fig. 11 is again the mass distribution $`m_{(K^+,p)}`$ as seen in Fig. 5 with the cut $`|m_Xm_{(K^+,p)}|35`$ MeV/c2. The middle (dashed) line is the $`m_{(K^+,p)}`$ distribution from either $`\varphi `$, $`\mathrm{\Lambda }(1520)`$, or $`\mathrm{\Lambda }(1670)`$ production. The difference between the top and middle distribution plotted as the bottom (dash-dotted) line of the “$`\mathrm{\Theta }^{++}`$” signal, is comparable with a flat line. The signal at 1.59 GeV/c2 is gone. There is no peak in the range between 1.5 GeV/c2 and 1.6 GeV/c2, in particular not at 1.54 GeV/c2 or 1.59 GeV/c2. The absence of a $`\mathrm{\Theta }^{++}`$ indicates that the $`\mathrm{\Theta }^+`$ state is an isospin-0 isosinglet, in agreement with the conclusions of .

## 4 Summary

A peak can be seen in the correlated invariant and missing mass distributions, suggesting a signal from a $`\mathrm{\Theta }^{++}`$ candidate. However, our analysis shows that this peak can be dismissed as a reflection mainly from $`\varphi `$ production and a smaller contribution from hyperon-resonance production. Our findings agree with recent results of a $`\mathrm{\Theta }^{++}`$ search in the existing K+-p scattering data in the W range of 1.520 to 1.560 GeV, which show that there is no evidence for $`\mathrm{\Theta }^{++}`$ with a width greater than 1 MeV/c2 . This suggests that the $`\mathrm{\Theta }^+`$ state is an isospin-0 isosinglet.


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# Magnetic-field induced spin-Peierls instability in strongly frustrated quantum spin lattices

## Abstract

For a class of frustrated antiferromagnetic spin lattices (in particular, the square-kagomé and kagomé lattices) we discuss the impact of recently discovered exact eigenstates on the stability of the lattice against distortions. These eigenstates consist of independent localized magnons embedded in a ferromagnetic environment and become ground states in high magnetic fields. For appropriate lattice distortions fitting to the structure of the localized magnons the lowering of magnetic energy can be calculated exactly and is proportional to the displacement of atoms leading to a spin-Peierls lattice instability. Since these localized states are present only for high magnetic fields, this instability might be driven by magnetic field. The hysteresis of the spin-Peierls transition is also discussed.

frustrated antiferromagnets, spin-Peierls instability

Antiferromagnetically interacting spin-$`\frac{1}{2}`$ systems on geometrically frustrated lattices have attracted much attention during last years. Such systems have rich phase diagrams exhibiting a number of unusual quantum phases 01 ; 02 . A striking example is the kagomé lattice antiferromagnet having a liquid-like ground state with a gap for magnetic excitations and a huge number of singlet states below the first triplet state (see e.g. Ref. waldtmann98,  and references therein). Another intriguing example is the structural phase transition in spin systems driven by magnetoelastic coupling (spin-Peierls instability) observed, e.g., in CuGeO3 CuGeO . Frustrating interactions may also provide a route to generating fractional phases in two dimensions which manifest itself in the dynamic correlations probed by inelastic neutron scattering experiments 03 .

In the presence of an external magnetic field frustrated quantum spin systems exhibit a number of unusual properties. In particular, plateaus and jumps can be observed in the zero-temperature magnetization curve for such models 01 ; 04 . The theoretical investigation of exotic magnetization curves has been additionally stimulated by the experimental observation of plateaus e.g. in CsCuCl3 nojiri88  or SrCu2(BO3)2 kageyama99 .

Though the treatment of quantum spin systems often becomes more complicated if frustration is present, in some exceptional cases frustration is crucial to find simple ground states of product form majumdar\_ghosh ; ivanov\_richter . Recently, for a wide class of frustrated spin lattices exact eigenstates consisting of independent localized magnons in a ferromagnetic environment have been found 05 . They may become ground states if a strong magnetic field is applied and lead to a macroscopic jump in the zero-temperature magnetization curve just below saturation.

In the present paper we examine the stability of antiferromagnetic spin lattices hosting independent localized magnons with respect to lattice distortions through a magnetoelastic mechanism. We are able to present rigorous analytical results completed by large-scale exact diagonalization data for lattices up to $`N=54`$ sites. We discuss the field-tuned changes of the ground-state properties owing to a coupling between spin and lattice degrees of freedom.

The effect of a magnetoelastic coupling in frustrated antiferromagnets is currently widely discussed. First of all the investigation of the Peierls phenomena in frustrated 1D spin systems is in the focus (see, for instance, Ref. 07,  and references therein). But also in 2D and 3D quantum spin systems lattice instabilities breaking the translational symmetry are reported. The frustration-driven structural distortions in the spin-$`\frac{1}{2}`$ square-lattice $`J_1`$-$`J_2`$ Heisenberg antiferromagnet studied in Ref. 08,  might be relevant for Li2VOSiO4 and VOMoO4 08 ; 09 . For 3D frustrated antiferromagnets containing corner-sharing tetrahedra one discusses several examples for lattice distortions. Inelastic magnetic neutron scattering on ZnCr2O4 revealed that a lattice distortion can lower the energy driving the spin system into an ordered phase 10 . NMR investigation of the three-dimensional pyrochlore antiferromagnet Y2Mo2O7 gives evidence for discrete lattice distortions which reduce the energy 11 . A lifting of a macroscopic ground-state degeneracy of frustrated magnets through a coupling between spin and lattice degrees of freedom in pyrochlore antiferromagnets was studied in Refs. 12, ; 13, , which may have relevance to some antiferromagnetic compounds with pyrochlore structure 13 .

In all those studies the lattice instability is discussed at zero field. As pointed out already in the late seventies gross  a magnetic field may act against the spin-Peierls transition and might favor a uniform or incommensurate phase. In contrast to those findings, in the present paper we discuss magnetic systems for which the magnetic field is essential for the occurrence of the lattice instability.

To be specific, we consider two geometrically frustrated lattices, namely, the square-kagomé lattice (Fig. 1, left)

and the kagomé lattice (Fig. 1, right). The ground state and low-temperature thermodynamics for the Heisenberg antiferromagnet on both lattices are subjects of intensive discussions (see e.g. Refs. 01, ; 02, ; waldtmann98, ; 14, ; tomczak, ). The Hamiltonian of $`N`$ quantum ($`s=\frac{1}{2}`$) spins reads

$`H={\displaystyle \underset{(nm)}{}}J_{nm}\left({\displaystyle \frac{1}{2}}\left(s_n^+s_m^{}+s_n^{}s_m^+\right)+\mathrm{\Delta }s_n^zs_m^z\right)hS^z.`$ (1)
Here the sum runs over the bonds (edges) which connect the sites (vertices) occupied by spins for the lattice under consideration, $`J_{nm}>0`$ are the antiferromagnetic exchange constants between the sites $`n`$ and $`m`$, $`\mathrm{\Delta }0`$ is the anisotropy parameter (in most cases throughout this paper $`\mathrm{\Delta }=1`$), $`h`$ is the external magnetic field and $`S^z=_ns_n^z`$ is the $`z`$-component of the total spin. We assume that all bonds in the lattice without distortion have the same length and hence all exchange constants have the same value $`J`$.

From Ref. 05,  we know that independent localized one-magnon states embedded in a ferromagnetic background are exact eigenstates of the Hamiltonian (1) for the considered models. More specifically, by direct computation one can check05  that

$`|1`$ $`=`$ $`{\displaystyle \frac{1}{2}}{\displaystyle \underset{\stackrel{i=1}{isquare}}{\overset{4}{}}}(1)^is_i^{}|FM,`$ (2)
$`|1`$ $`=`$ $`{\displaystyle \frac{1}{\sqrt{6}}}{\displaystyle \underset{\stackrel{i=1}{ihexagon}}{\overset{6}{}}}(1)^is_i^{}|FM`$ (3)
are the one-magnon eigenstates of the Hamiltonian (1) on the square-kagomé and kagomé lattices, where $`|FM`$ stands for the embedding fully polarized ferromagnetic environment. The corresponding energies ($`h=0`$) of the one-magnon states (2) and (3) are

$`J+J+\left(2N12\right){\displaystyle \frac{1}{4}}J,`$ (4)
$`{\displaystyle \frac{1}{2}}J+2J+\left(2N18\right){\displaystyle \frac{1}{4}}J.`$ (5)
The magnons (2) or (3) are trapped (localized) on a square or on a hexagon, respectively. We separate explicitly in (4), (5) the contributions to the energy from those bonds which form a magnon trapping cell (first terms), from the bonds connecting this cell with the environment (second terms) and from the ferromagnetic environment (third terms). One can proceed to fill the lattices with $`n>1`$ localized magnons; the state with maximum filling (“magnon crystal”) has $`n=n_{\mathrm{max}}`$ independent localized magnons with $`n_{\mathrm{max}}=\frac{1}{6}N`$ and $`\frac{1}{9}N`$ for the square-kagomé and kagomé lattices, respectively 05 . Since $`S^z`$ commutes with the Hamiltonian (1), the energy in the presence of an external field $`h0`$, $`E(S^z,h)`$, can be obtained from the energy without field, $`E(S^z)`$, through the relation $`E(S^z,h)=E(S^z)hS^z.`$ Since each magnon carries one down spin, a localized magnon state with $`n`$ independent magnons has $`S^z=\frac{1}{2}Nn`$ and consequently Eqs. (4), (5) give $`E(S^z=\frac{1}{2}N1)`$ for the corresponding systems.

Under quite general assumptions it was proved 15  that these localized magnon states have lowest energies in the corresponding sector of total $`S^z`$. As a result, these states become ground states in a strong magnetic field. More specifically, the ground-state energy in the presence of a field is given by $`E_0(h)=E_{\mathrm{min}}(S^z)hS^z`$ and the ground-state magnetization $`S^z`$ is determined from the equation $`h=E_{\mathrm{min}}(S^z)E_{\mathrm{min}}(S^z1)`$. Since for $`S^z=\frac{1}{2}N,\mathrm{},\frac{1}{2}Nn_{\mathrm{max}}`$ (i.e., $`0nn_{\mathrm{max}}`$) the localized magnon states are the lowest states, one has

$`E_{\mathrm{min}}(S^z)={\displaystyle \frac{1}{2}}NJ3nJ=NJ+3JS^z`$ (6)
for both models. Due to the linear relation between $`E_{\mathrm{min}}`$ and $`S^z`$ one has a complete degeneracy of all localized magnon states at $`h=h_1`$, i.e. the energy is $`NJ`$ at $`h=h_1`$ for all $`\frac{1}{2}Nn_{\mathrm{max}}S^z\frac{1}{2}N`$, where $`h_1=3J`$ is the saturation field (identical for both models). Consequently, the zero-temperature magnetization $`S^z`$ jumps between the saturation value $`\frac{1}{2}N`$ and the value $`\frac{1}{3}N`$ ($`\frac{7}{18}N`$) for the square-kagomé (kagomé) lattice. The effects of the localized magnon states become irrelevant if the spins become classical ($`s\mathrm{}`$).

We want to check the lattice stability of the considered systems with respect to a spin-Peierls mechanism. For this purpose we assume a small lattice deformation which preserves the symmetry of the cell which hosts the localized magnon (in this case the independent localized magnon states remain the exact eigenstates) and analyze the change in the total energy (which consists of the magnetic and elastic parts) to reveal whether the deformation is favorable or not. To find a favorable deformation one needs optimal gain in magnetic energy. For that we use the circumstance that due to the localized nature of the magnons we have an inhomogeneous distribution of nearest-neighbor (NN) spin-spin correlations $`𝐬_i𝐬_j`$ 05 . In case that one magnon is distributed uniformly over the lattice the deviation of the NN correlation from the ferromagnetic value, $`𝐬_i𝐬_j\frac{1}{4}`$, is of the order $`\frac{1}{N}`$. On the other hand for a localized magnon (3) \[(2)\] we have along the hexagon \[square\] hosting the localized magnon actually a negative NN correlation $`𝐬_i𝐬_j=\frac{1}{12}[\frac{1}{4}]`$ and all other correlations are positive. Hence a deformation with optimal gain in magnetic energy shall lead to an increase of antiferromagnetic bonds on the square (hexagon) and to a decrease of the bonds on the attaching triangles. The corresponding deformations are shown in Fig. 1. For the square-kagomé lattice (Fig. 1, left) the deformations lead to the following changes in the exchange interactions: $`J\left(1+\sqrt{2}\delta \right)J`$ (along the edges of the square) and $`J\left(1\frac{1}{4}\sqrt{2}\left(\sqrt{3}1\right)\delta \right)J`$ (along the two edges of the triangles attached to the square), where the quantity $`\delta `$ is proportional to the displacement of the atoms and the change in the exchange integrals due lattice distortions is taken into account in first order in $`\delta `$. For the kagomé lattice (Fig. 1, right) one has $`J\left(1+\delta \right)J`$ (along the edges of the hexagon) and $`J\left(1\frac{1}{2}\delta \right)J`$ (along the two edges of the triangles attached to the hexagon). The magnetic energies (4) and (5) are lowered by distortions and become $`\frac{1}{2}NJ3J\frac{1}{4}\sqrt{2}\left(3+\sqrt{3}\right)\delta J`$ and $`\frac{1}{2}NJ3J\frac{3}{2}\delta J`$, respectively. This is in competition with the increase of the elastic energy, which is given in harmonic approximation by $`2\left(6\sqrt{3}\right)\alpha \delta ^2`$ (square-kagomé) and by $`9\alpha \delta ^2`$ (kagomé). The parameter $`\alpha `$ is proportional to the elastic constant of the lattice. The change of total energies due to distortions read

$`{\displaystyle \frac{1}{4}}\sqrt{2}\left(3+\sqrt{3}\right)\delta J+2\left(6\sqrt{3}\right)\alpha \delta ^2,`$ (7)
$`{\displaystyle \frac{3}{2}}\delta J+9\alpha \delta ^2,`$ (8)
where for $`n`$ independent localized magnons with $`n`$ related distortions these results have to be multiplied by $`n`$. Minimal total energy is obtained for $`\delta =\delta ^{}=\frac{\sqrt{2}\left(3+\sqrt{3}\right)}{16\left(6\sqrt{3}\right)}\frac{J}{\alpha }`$ for the square-kagomé and $`\delta =\delta ^{}=\frac{1}{12}\frac{J}{\alpha }`$ for the kagomé lattice.

We have considered only a special class of lattice deformations (under which the independent localized one-magnon states survive). Although we are not able to prove rigorously that these lattice deformations are the most favorable, we have presented above nonrigorous arguments that these deformations take advantage of the localized magnons in an optimal way. However, we have rigorously shown that there exist lattice deformations which yield a gain in the total energy for large values of $`S^z`$ leading to a spin-Peierls instability of the lattice for an appropriate (large) magnetic field $`h_1`$.

To discuss the scenario of spin-Peierls instability more specifically we consider a magnetic field above the saturation field $`h_1`$. For the corresponding fully polarized ferromagnetic state a lattice distortion is not favorable. Decreasing $`h`$ till $`h_1`$ the homogeneous ferromagnetic state transforms into the “distorted magnon crystal”; this transformation is accompanied by the aforementioned magnetization jump. On the basis of general arguments 17 ; 18  we expect that the “magnon crystal” state has gapped excitations and the system exhibits a magnetization plateau between $`h_1`$ and $`h_2<h_1`$ at $`S^z=\frac{1}{2}Nn_{\mathrm{max}}`$. To support this statement we calculate the plateau width $`\mathrm{\Delta }h=h_1h_2`$ for finite systems of $`N=27,36,45,54`$ (kagomé) and $`N=24,30,48,54`$ (square-kagomé) for the undistorted lattice, where $`h_2`$ is obtained by $`h_2=E_{\mathrm{min}}(S^z=\frac{1}{2}Nn_{\mathrm{max}})E_{\mathrm{min}}(S^z=\frac{1}{2}Nn_{\mathrm{max}}1)`$. Using a $`\frac{1}{N}`$ finite-size extrapolation we find indeed evidence for a finite $`\mathrm{\Delta }h=0.07J`$ ($`\mathrm{\Delta }h=0.33J`$) for the kagomé (square-kagomé) lattice in the thermodynamic limit. This plateau width might be enlarged by distortions (see below).

Now the question arises whether the lattice distortion under consideration is stable below this plateau, i.e., for $`S^z<\frac{1}{2}Nn_{\mathrm{max}}`$. We are not able to give a rigorous answer but can discuss the question again for finite systems of size $`N=24,30,48,54`$ (square-kagomé) and $`N=18,27,36,45,54`$ (kagomé) with $`n_{\mathrm{max}}`$ distorted squares/hexagons. We calculate the magnetic energy for zero and small distortion parameter $`\delta `$ for different values of $`S^z`$. Adopting for the magnetic energy the ansatz

$`E_{\mathrm{min}}(S^z,\delta )=E_{\mathrm{min}}(S^z,0)+A\delta ^p`$ (9)
and taking $`\delta `$ of the order of $`10^4`$ we can estimate the exponent $`p`$ from the numerical results. Evidently, the lattice may become unstable if $`p<2`$ (and, of course, $`A<0`$) whereas $`p2`$ indicates lattice stability.

Of course, the numerical results reproduce the analytical findings reported above for $`S^z=\frac{1}{2}Nn_{\mathrm{max}}`$. More interesting is the sector of $`S^z`$ just below, i.e. $`S^z=\frac{1}{2}Nn_{\mathrm{max}}1`$. Remarkably both lattices behave differently as $`h`$ becomes smaller than $`h_2`$. For the finite square-kagomé lattices considered we find $`p=1.001,\mathrm{\hspace{0.33em}1.000},\mathrm{\hspace{0.33em}1.000},\mathrm{\hspace{0.33em}1.000}`$ for $`N=24,30,48,54`$, respectively, if $`S^z=\frac{1}{2}Nn_{\mathrm{max}}1`$. Moreover, $`p`$ remains equal to 1 for smaller $`S^z`$. Therefore, we conclude that the distorted square-kagomé lattice remains stable for $`S^z<\frac{1}{2}Nn_{\mathrm{max}}`$. On the other hand, for finite kagomé lattices we obtain $`p=2.000,\mathrm{\hspace{0.33em}1.002},\mathrm{\hspace{0.33em}2.000},\mathrm{\hspace{0.33em}1.998},\mathrm{\hspace{0.33em}2.055}`$ for $`N=18,27,36,45,54`$, respectively, if $`S^z=\frac{1}{2}Nn_{\mathrm{max}}1`$. The “outrider” for $`N=27`$ may be attributed to finite-size effects, indeed we have $`p=1.994`$ for the next lower $`S^z=\frac{1}{2}Nn_{\mathrm{max}}2`$. Moreover, $`p`$ remains about 2 for smaller $`S^z`$. We interpret small deviations from 2 also as finite-size effects and conclude that the spin-Peierls instability in the kagomé lattice (within the adopted ansatz for the lattice deformation) is favorable only for $`\frac{1}{2}Nn_{\mathrm{max}}S^z<\frac{1}{2}N`$ and the distortion disappears for $`h<h_2`$.

The origin for the different behavior of the square-kagomé and the kagomé lattice below $`h_2`$ can be attributed to the circumstance, that the square-kagomé lattice has non-equivalent NN bonds (namely bonds belonging to triangles and bonds belonging to squares) which carry different NN spin-spin correlations, but the kagomé lattice has not. This difference in the NN spin-spin correlations leads to a special affinity of the magnetic system to the considered lattice distortions.

Let us now briefly discuss the influence of the lattice distortion on the saturation field $`h_1`$. Since the fully polarized ferromagnetic state is not distorted, $`h_1`$ is shifted to higher values according to $`\frac{h_1(\delta ^{})}{J}=3+\frac{3\left(2+\sqrt{3}\right)}{32\left(6\sqrt{3}\right)}\frac{J}{\alpha }`$ for the square-kagomé and $`\frac{h_1(\delta ^{})}{J}=3+\frac{1}{16}\frac{J}{\alpha }`$ for the kagomé lattice, i.e. the “distorted magnon crystal” remains stable until $`h_1(\delta ^{})>h_1`$. On the other hand, starting at large magnetic fields $`h>h_1`$ the fully polarized ferromagnetic state remains (meta)stable until $`h_1=3J`$. Consequently, we have a hysteresis phenomenon in the vicinity of saturation field.

We mention that our considerations basically remain unchanged for the anisotropic Hamiltonian (1) with $`\mathrm{\Delta }1`$. The presence of anisotropy leads only to quantitative changes in our results. For the sectors of $`S^z`$ below the localized magnon states we have checked that numerically for $`N=18`$ (kagomé) and $`N=24`$ (square-kagomé). For the sectors of $`S^z`$ with localized magnon states it becomes obvious from the change in magnetic energy of a localized magnon state due to distortions given by $`\left(\sqrt{2}+\frac{1}{4}\sqrt{2}\left(\sqrt{3}1\right)\mathrm{\Delta }\right)\delta J`$ (square-kagomé) and $`\left(1+\frac{1}{2}\mathrm{\Delta }\right)\delta J`$ (kagomé), where these expressions for $`\mathrm{\Delta }=1`$ transform to the first terms in Eqs. (7) and (8), respectively.

From the experimental point of view the discussed effect should most spectacularly manifest itself as a hysteresis in the magnetization and the deformation of kagomé-lattice antiferromagnets or the kagomé-like magnetic molecules in the vicinity of the saturation field.

We wish to stress that the predicted spin-Peierls instability in high magnetic fields may appear in a whole class of frustrated quantum magnets in one, two and three dimensions hosting independent localized magnons provided it is possible to construct a lattice distortion preserving the symmetry of the localized-magnon cell. Moreover, the effect is not restricted to $`s=\frac{1}{2}`$ and to isotropic Heisenberg systems05 ; 15 . We mention, that we have checked explicitly that our results are valid for e.g. the kagomé-like chain of Ref. wksme,  or the dimer-plaquette chain (see Ref. schul02,  and references therein). This fact certainly increases the chance to observe the predicted spin-Peierls instability.

There is an increasing number of synthesized quantum frustrated kagomé magnetsramirez00dd ; 19 ; 20 ; bono04 . Though these available materials do not fit perfectly to an ideal kagomé Heisenberg antiferromagnet the physical effects based on localized magnon states may survive in non-ideal geometries, see Ref. entropy, . Furthermore one needs comparably small exchange constants $`J`$ to reach experimentally the saturation field where the structural instability occurs. A simple calculation leads to the relation $`h_{sat}`$/Tesla $`2.23`$ $`J`$/K for a spin-$`\frac{1}{2}`$ kagomé Heisenberg antiferromagnet. As a candidate for an experimental study at saturation field may serve the novel spin-$`\frac{3}{2}`$ kagomé like material Ba2Sn2ZnCr7pGa10-7pO22bono04  with a comparably small exchange constant of about $`J37\mathrm{}40`$K leading to a saturation field accessible with today available high-end experimental equipment. We may expect that further such materials will be synthesized and with our work we are pointing out that the efforts in this direction are worthwhile also because of a new effect: the spin-Peierls instability in a strong magnetic field.

To summarize, we have reported a spin-Peierls instability in strong magnetic fields for several frustrated Heisenberg antiferromagnets hosting independent localized magnons. This spin-Peierls instability may or may not survive for smaller fields in dependence on details of lattice structure. In particular, for the Heisenberg antiferromagnet on the kagomé lattice we have found evidence that the spin-Peierls instability breaking spontaneously the translational symmetry of the kagomé lattice appears only in a certain region of the magnetic field. The field dependence of the magnetization and the deformation in the vicinity of saturation displays a hysteresis.

We thank A. Honecker, J. Schnack, S. L. Drechsler and D. Ihle for discussions and comments. The present study was supported by the DFG (project 436 UKR 17/17/03).

Postal addresses:
Prof. Dr. Johannes Richter
Institut für Theoretische Physik, Universität Magdeburg,
P.O. Box 4120, D-39016 Magdeburg, Germany
Tel: +49 391 6718841
Fax: +49 391 6711217
E-mail: johannes.richter@physik.uni-magdeburg.de
Dr. Oleg Derzhko
Institute for Condensed Matter Physics, National Academy of Sciences of Ukraine,
1 Svientsitskii Street, L’viv-11, 79011, Ukraine
Tel: (0322) 76 19 78
Fax: (0322) 76 11 58
E-mail: derzhko@icmp.lviv.ua
Dr. Jörg Schulenburg
Universitätsrechenzentrum, Universität Magdeburg,
P.O. Box 4120, D-39016 Magdeburg, Germany
Tel:
Fax:
E-mail: Joerg.Schulenburg@URZ.Uni-Magdeburg.DE


text:
# Raman studies of polycrystalline CaCu3Ti4O12 under high-pressure

## Abstract

We report a Raman scattering study of polycrystalline CaCu3Ti4O12 (CCTO) under pressure up to 5.32 GPa. The pressure dependence of several Raman modes was investigated. No anomalies have been observed on the phonon spectra thereby indicating that the Th (Im$`\overline{3}`$) structure remains stable for pressures up to 5.32 GPa. The pressure coefficients for the observed modes were determined. This set of parameters was used for evaluating the stress developed in CCTO thin films.

The complex perovskite CaCu3Ti4O12 (CCTO) has been recently reported as a material having the largest dielectric constant (16000-18000) ever measured in the laboratory.subramanian00 ; ramirez00 ; homes01  In addition to this striking property, the dielectric constant is nearly constant over a wide temperature range (from 100 to 600 K). Explaining the anomalous dielectric constant has been an intriguing issue and many models have been proposed. Some authors have attributed the high values to extrinsic factors such as defects and grain boundaries.cohen03 ; sinclair02  By performing first principle calculations, the Vanderbilt’s group has suggested that the source of such giant dielectric constant should be related to extrinsic effects since the contribution of the lattice effects was estimated to be about 60.he02 ; he03  This value is extremely smaller than what has been found in the experiments (105). Recently, homogeneous CCTO thin films epitaxially grown were found to exhibit a low-frequency permittivity of $``$100.tselev03  This experimental result supports the hypothesis that the giant dielectric constant obtained for bulk CCTO comes from extrinsic effects. Owing to these remarkable properties, CCTO is being considered as a very promising material for application in microelectronics, mainly in capacitive elements. With the miniaturization of the devices and having in view the large and prompt integration with the current technology, CCTO thin films are the most likely systems to be used in CCTO-based devices. Such systems have been investigated and several reports on growth,lin02 ; fang03 ; jha03  dielectrics,tselev03 ; zhao031  dc and ac electrical resistivity,chen03  and optical propertieslitvinchuk03  have already been reported.

Thin films are expected to exhibit built-in stress due to the grain boundary, reduced dimensionality, and the lattice mismatch with the various substrate used for growing them. The residual stress affects the mechanical, electrical and optical properties of the films. Therefore, it is important to investigate the stress developed in the films in order to improve the growth methods and to tailor desired physical properties. Raman spectroscopy has been established as a powerful and versatile technique (non-destructive, contact-less and non-invasive) for investigating the stress in films by monitoring the phonon frequency shifts of the films relative to their bulk counterparts. For carrying out such analysis, the knowledge of the pressure dependence of the Raman spectra of polycrystalline CCTO can be the basis for probing and interpreting built-in stress in CCTO films.

So far, the Raman modes of CCTO have been measured in ceramicsalmeida02 , single crystals,kolev02 ; koitzsch02 , and thin films.litvinchuk03 . These investigations have been devoted to study the polarization and temperature dependence of the Raman spectra.kolev02 ; koitzsch02  In this work we report the effects of pressure on the Raman spectra of polycrystalline CCTO. We found that the mode frequencies exhibit a linear behavior with pressure. No anomalies have been observed from ambient pressure up to 5.32 GPa thus indicating the absence of structural instabilities (phase transitions) in this pressure range. The modes are sensitive to the applied pressure. The pressure coefficients $`\alpha =\omega /P`$ were determined and these values will be useful for calculating the Grüneisen parameters. Finally, we used our set of pressure coefficients along with the Raman data available in the literature litvinchuk03  for evaluating the stress in CCTO thin films.

Commercial oxides Ca(OH)2 (Vetec, 97% with 3% of CaCO3), CaCO3 (Aldrich, 99%), TiO2 (Aldrich, 99%), and CuO (Aldrich, 99%) were used for preparing CCTO ceramics. The CCTO samples were prepared by the conventional powder-sintering technique. The starting materials were weighted according to the stoichiometric ratios and mixed thoroughly in an agate mortar. The mixed powder was calcined at 900oC for 12 h, and the resulting samples were sintered in air at 1050oC for 24 h. High-pressure Raman experiments were performed using a diamond anvil cell (DAC) with 4:1 methanol : ethanol mixture as the transmitting fluid. The pressure calibration was achieved by using the well known pressure shift of the ruby luminescence lines. The pressure dependent Raman spectra were obtained with a triple-grating spectrometer (Jobin Ivon T64000) equipped with a N2 cooled charge coupled device (CCD) detection system. The line 514.5 nm of an argon ion laser was used as excitation. An Olympus microscope lens with a focal distance f$`=20.5`$ nm and numeric aperture N.A.$`=0.35`$ was employed to focus the laser beam on the sample surface.

Before discussing our results we briefly summarize some properties of CCTO. This material has a body-center cubic primitive cell containing 20 atoms and belonging to the centrosymmetric Th(Im$`\overline{3}`$) group. Standard group theory analysis predicts that the Raman active modes are distributed among the irreducible representation as 2Ag+2Eg+4Fg.kolev02  The lower trace in Fig. 1 shows the Raman spectrum of CCTO at ambient pressure and room temperature. CCTO is a weak scatter and only five of the eigth predicted modes are observed at around 444, 453, 510, 576 and 761 cm-1. Based on lattice dynamics studieshe02 ; he03  and polarized Raman measurements, kolev02  the mode symmetries are identified as Ag(1)(444 cm-1), Fg(2)(453 cm-1), Ag(2)(510 cm-1), Fg(3)(576 cm-1) and Fg(4)(761 cm-1). Following lattice dynamics calculations the 444, 453, and 510 cm-1 are TiO6 rotationlike modes. The peak at 576 cm-1 is assigned to the Ti-O-Ti anti-stretching mode of the TiO6 octahedra.kolev02  The Fg(4) mode has been predicted to be observed at about 710 cm-1. We have assigned the mode 761 cm-1 to the symmetric stretching breathing of the TiO6 octahedra. Its low intensity is typical of the structures containing shared units where the neighbors octahedra underdamp the symmetric vibrations. First-principle calculationshe02  predict this breathing mode to be observed at 739 cm-1. This value is much more close to 761 cm-1 we have observed than the prediction of classical lattice dynamics.kolev02

Upon increasing pressure, it is evident from the spectra (see Fig.1), that the material remains in its initial configuration up to the maximum pressure we have reached in our experiments. In order to discuss in detail the pressure effects on CCTO phonon frequencies we have constructed the frequency ($`\omega `$) vs. pressure (P) plots. The results for both compression (solid circles) and decompression (open circles) experiments are shown in Fig. 2. All peaks exhibit a linear behavior $`\omega (P)`$=$`\omega _0+\alpha P`$ and both frequency intercepts ($`\omega _0`$) and pressure coefficients ($`\alpha `$) are listed in Table 1. Note, that all modes are sensitive to pressure and large $`\alpha `$ values were observed. For the breathing mode $`\omega /P<`$0, indicating a possible structural instability that might lead to a structural phase transition at higher pressures. Finally, the pressure-dependent data also reveal that the linewidths change slightly with pressure. This result suggests that the pressure does not induce any disorder in CCTO.

Provided the pressure coefficients we have the ground knowledge for discussing the Raman scattering results in CCTO thin films. Litvinchuk et al.litvinchuk03  report the Raman scattering studies of CCTO thin films prepared by pulsed laser deposition on a (001) LaAlO3 substrate. When compared with bulk CCTO, these authors have observed the Raman modes in the film are shifted toward higher frequency by an amount of 4-7 cm-1. Similarly to spectra of bulk CCTO, the Ag(2) mode is the most intense mode measured in CCTO films. It was observed at 517 cm-1 which is 7 cm-1 higher than in CCTO bulk. We attribute this upshift to the stress developed during the growth process. The pressure behavior of the Ag(2) mode has been determined as $`\omega (P)=510+3.6P`$, being $`\omega `$ and $`P`$ in units of cm-1 and GPa, respectively. By using this equation and the value of $`\omega `$ measured in the CCTO film we calculate that the stress developed in the CCTO film reported in ref. litvinchuk03  is 1.94$`\pm `$0.3 GPa.

Summarizing, we studied polycrystalline CCTO under high pressure. No evidence for pressure-induced phase transition was found in the 0-5.32 GPa pressure range. The frequencies of all Raman modes exhibit a linear dependence on pressure. We also determined the pressure coefficients $`\alpha =\omega /P`$ for all modes. This set of parameters was used for evaluating the built-in stress in CCTO thin films prepared by pulsed laser deposition. The $`\alpha `$ values would be also useful for calculating the Grüneisen parameters for CCTO as the Young s modulus become available. Finally, this work improves the characterization data of CCTO that will be useful for feeding back theoretical models and allowed to improve the understanding of the Raman spectra properties of CCTO thin films.

D.V. and A.G.S.F. acknowledge financial support from the Brazilian agencies CNPq and CAPES (PRODOC grant No. 22001018), respectively. The authors acknowledge Dr. I. Guedes for a critical reading of the manuscript and partial support from Brazilian agencies CNPq, FUNCAP and FAPESP.