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# Compositional analyses of a Reutlingen Bronze Age sword discovered at Giurgiu, Romania

## 1 Introduction

The compositional scheme of a Bronze Age sword, Fig. 1, recently discovered near Giurgiu, a town situated in the south of Romania on the Danube, has been studied using the method of particle-induced X ray emission (PIXE), at the Tandem accelerator of National Institute for Physics and Nuclear Engineering from Bucharest, Magurele, Romania. In order to have a comparative study of composition we have considered also the composition of 6 swords of the same type and from the same period from the south of Danube in Bulgaria, and some different copper-based alloy objects from Şpălnaca deposit, in Transylvania, dated also in the Bronze Age.

## 2 Archaeological considerations

### 2.1 Site of discovery of the sword

The sword has been discovered by Ion Cercel in 1981 in the Mihai Eminescu street of the city of Giurgiu, Romania, in the course of diggings related to the installation of underground electric cables. Since then the sword has been kept by Ion Cercel, who presently is retired, in his house from the Oinacu commune, district of Giurgiu, in southern Romania. In 1999, by a happy concurrence of events, this interesting artifact became available to us, and we take this opportunity to thank Ion Cercel who has been kind to render us the sword for study and analyses.

According to the author of the finding, the artifact has been found at a depth of approximately 1.1 m, no other bronze objects existing in its vicinity. Foundations of buildings from the late medieval period were known to exist in the area, but it seems that no such archaeological remains existed in the specific place where the sword has been found. It seems that the site where the sword has been discovered lies outside the medieval city, buildings being erected there only in the period after 1821.

### 2.2 Description of the sword

The sword is in a good state of conservation, being preserved almost entirely, and has the following dimensions: total length 39.5 cm, width at base 5.3 cm, width at the tip 2.9 cm, thickness at base 0.9 cm, thickness toward the tip 0.6 cm, length of the hilt with missing terminal part 9 cm, length of the blade 30.5 cm. On the blade of the sword one can observe, on both faces, channels situated at approximately 0.4 cm from the two edges, as shown in Fig. 1. The blade has a biconvex profile. In the zone of the hilt there are five orifices for the rivets of binding of the hilt and also three rivets still left in the orifices. It is possible that in the missing part of the hilt three more orifices should have existed for the binding of the hilt. The alloy is of a very good quality having a green-dark grey patina.

The sword belongs to the Reutlingen type defined by P. Schauer  and described, with a special view to artifacts attested on Romanian territory, by T. Bader.  Choosing as a criterion of classification in the first place the number of fixation orifices from the blade and the hilt, but also the shape of the nervure of the blade, the latter author distinguished several variants.  Due to the fact that the sword under consideration presents a large median nervure and which is slightly rounded, we think that it is most resembling to two fragmentary pieces belonging to the deposit of Drajna de Jos, district of Prahova, Romania, catalogued by T. Bader with numbers 188 and 189  and included in the Guşteriţa variant of the Reutlingen type. Moreover, the Giurgiu sword has much smaller dimensions, so that it could be rather considered a ”short sword” (Kurzschwert).

Artifacts of the Reutlingen type have been discovered over a very large area from the south of Scandinavia to Peloponesos and from the Rhine basin to the Black Sea,  and recently discoveries have been reported even in Anatolia.  However, the spreading is not uniform, existing some regions of concentration and others represented by much fewer discoveries. Among the latter, one counts the extra-Carpathian zone in Romania and the territory of Bulgaria and Greece.

It is however interesting that, in the Balkan area, the discoveries are concentrated mainly in the southern part of Romania, Wallachia, and in the north of Bulgaria, some of them just on the Danube line. In addition to the two pieces from Drajna de Jos, on the Romanian territory one finds specimens belonging to some variants in the ensemble of the Reutlingen type: Bălceşti and Mateeşti (district of Vâlcea), Techirghiol (district of Constanţa). On the territory of Bulgaria there are 10 discoveries of swords with tongues at the hilt, of which 7 to the north and 3 to the south of the Balkans.  The 7 specimens discovered on the territory between the Danube and the Balkans arise from Orjahovo (Orehovo),  Vărbica (deposit II), , Bajkal,  Kruševo,  Balkanski  and Vasil Levski,  to which one adds the specimen of smaller dimensions from the Razgrad Museum (inventory No. 117), discovered in the neighborhood.  Among these specimens the first two belong to the Reutlingen type.

The artifact from Giurgiu has very close analogues (except, of course, for the dimensions) just in the sword from Orjahovo and in the fragmentary artifact from Vărbica, both cited as belonging to the Guşteriţa variant by T. Bader.  These two specimens have been ascribed in the early horizon of the culture of the fields of urns (von Brunn stages I-III)  by B. Hänsel,  respectively in the subgroup I defined by I. Panayotov (the second horizon of deposits from Bulgaria: XIIIth century B.C.).  On the other hand, T. Bader dates, as a function of the synchronisms revealed by the various deposits, the great majority of the specimens belonging to the Reutlingen type discovered on the territory of Romania in the Cincu-Suseni period (HaA1, circa XIIth century B.C.), but ascribes three or four deposits (among which is also the one from Drajna de Jos) for the slightly earlier period Uriu-Domăneşti (Bronze D, circa XIIIth century B.C.)  Consequently, taking into account the analogies proposed by us with the specimens from Drajna de Jos, Orjahovo and Vărbica II, we favor a dating of the short sword from Giurgiu in the XIIIth century B.C., probably towards the end of the century; a date around 1200 B.C. is very likely.

## 3 Experimental

3 samples from the body of the sword: 1 sample from the tip of the sword and 2 samples from the hilt have been flatted and irradiated with protons of 3 MeV, in a irradiation chamber at the FN Tandem accelerator of National Institute for Physics and Nuclear Engineering from Bucharest, Magurele.

The beam current was kept below 10 nA to maintain a count rate of about 250 counts/s, which implies negligible dead-time and pile-up corrections. X-rays were detected with a HPGe (100 mm2mm) detector with 160 eV energy resolution at 5.9 keV. The X rays spectra have been recorded on a PC with a MCA interface. In the frame of the experimental conditions the following elements have been observed: As, Co, Cr, Cu, Fe, Ni, Pb, Sn and Zn.

The X ray spectra have been processed off line and then the concentrations of the elements have been calculated.

## 4 Results and Discussions

The results of PIXE analysis on the samples from the sword from Giurgiu are shown in the Table 1. The values of the concentrations are given in %. The instrumental errors are generally less than 15 %. We made corrections of the elemental concentrations so that the total value in the sample to be 100 %.

The composition of the 3 samples form the Giurgiu has been compared with the composition from similar 6 swords from Danubian regions from Bulgaria  and some different archaeological objects from the Bronze Age Şpălnaca deposit, Transylvania .

We present further, in the Table 2 the results of the analyses published by E. N. Černyh, for several of the swords with tongue at the hilt from Bulgaria.

1: Vărbica II (10945), category X
2: Orjahovo (9431), category X
3: Pavelsko (9220), category X
4: Bajkal (9432, analysis of the hilt; 9433, analysis of the blade), category X
5: Kričim (9210), category X
6: Vasil Levski (10892), category XI

For all specimens included in Table 2, the copper is the dominant element.

In Table 3 are shown the elemental composition for all considered objects: the Giurgiu sword, the swords from Bulgaria and different bronze objects from Transylvanian deposit at Şpălnaca. Ratios of concentrations are considered for interpretation of the results to avoid the errors in the absolute calculations of the concentrations. It has been reported value zero in the cases the value of concentrations has been under the limit of detection.

Fig. 2 presents the diagram of ratios of concentrations: Sn/Cu versus As/Sn for the analyzed samples in the present study, and also for Bulgarian and Transylvanian objects, analyzed by atomic spectroscopy and respectively neutron activation analysis.

One could remark that the sword from Giurgiu has a relative closer composition to the Bulgarian ones, especially for the elements: As, Cu, and Sn. The objects from Transylvania are situated relatively outside the cluster formed by the objects from Giurgiu and Bulgaria.

## 5 Conclusions

We could express the idea of an association of the sword from Giurgiu with the Bulgarian swords, having a close composition and also similitude in typology, geographic area and dating. Taking into account the analogies proposed by us with the Bulgarian specimens, Especially those of Drajna de Jos, Orjahovo and Vărbica II, we favor a dating of the short sword from Giurgiu in the XIIIth century B.C., probably towards the end of that century, around 1200 B.C.


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# Correlated radio:X-ray emission in the hard states of Galactic microquasars

## 1. Introduction

The (quasi) simultaneous observations of X-ray binaries in the radio and X-ray bands has led to the notion that the presence of radio jets is ubiquitous in sources with black holes or low magnetic field ($`10^9`$ G) neutron stars as compact objects (see Fender, 2001a; Fender & Kuulkers, 2001). Galactic X-ray binaries exhibiting radio jets (outflow of matter in a collimated beam), with both physical as well as temporal (variability) scale roughly at 6 orders of magnitude less than those of quasars, are termed as microquasars (Mirabel & Rodriguez, 1999).

Although superluminally moving radio jets are detected in several microquasars (Mirabel & Rodriguez, 1994; Tingay et al., 1995; Hjellming & Rupen, 1995), which are invariably associated with huge radio flares, only recently it has been realized that non-thermal radio emission is a common feature during relatively quiet phases. Fender (2001a, b) made a detailed calculation of the energetics during such quiet phases and argues that the non-thermal emission forms a substantial part (5%—50%) of the energy budget. Compact radio jets are indeed observed in the low-hard state of several microquasars viz. Cyg X-1 (Stirling et al., 2001), GRS 1915+105 (Dhawan et al., 2000), 1E 1740.7-2942 (Mirabel et al., 1992), and GRS 1758-258 (Rodriguez et al., 1992). Further, the spectral analysis of the radio emission from X-ray transient blackhole candidates, GS 2023+38, GRO J0422+32 and GS 1354-64 (Fender, 2001a) and two persistent X-ray blackhole candidates GX 339-4 (Corbel et al., 2000) and XTEJ 1550-564 (Corbel et al., 2001) are interpreted to originate from synchrotron emitting, compact conical jets. A comprehensive study of the association between radio and X-ray emission during the quiet phases of these sources is imperative for understanding the physical mechanism connecting the inflow and outflow of matter, a.k.a. the disk-jet connection, in such systems.

The Galactic blackhole candidate GX 339-4 exhibits canonical X-ray states typical for such binary systems. In its low-hard state the source shows very strong correlation between radio and both soft and hard X-ray emissions (Corbel et al., 2003), whereas in the high-soft state the radio emission is quenched (Corbel et al., 2000). For Cyg X-1, the archetypical blackhole binary system, Brocksopp et al. (1999) report that the radio flux is loosely correlated with both soft X-ray (2 – 12 keV, all-sky monitor \[ASM\]) and hard X-ray (20 – 100 keV, Burst and Transient Source Experiment \[BATSE\]) fluxes in the low-hard state of the source, with the soft (ASM) and hard (BATSE) X-ray flux being significantly correlated. The radio emission is suppressed in the high-soft state of this source. The enigmatic blackhole candidate GRS 1915+105 shows several variability classes, see Belloni et al. (2000) for the various classifications, of which the class $`\chi `$ with steady low X-ray flux has the closest association to the canonical low-hard state (Vadawale et al., 2001a). For this source, Rau & Greiner (2003) find no correlation between the radio emission and both soft X-ray emission and wide-band (1 - 200 keV) flux, but find an anti-correlation between hard X-ray (20 - 200 keV) flux and the radio emission. They also find that the slope of the hard power law spectrum correlates positively with the radio flux in this $`\chi `$ state. Thus, different types of radio and X-ray correlations have been reported for these sources and a clear and consistent picture of radio and X-ray flux correlation in the low-hard state for these black hole candidates is yet to emerge.

Recently, we have carried out a systematic analysis of correlation between radio, soft, and hard X-ray fluxes as well as a study of changes in wide band X-ray spectral behavior with radio flux in the steady quiescent X-ray state for Cyg X-3 (Choudhury et al., 2002, henceforth Paper 1), a suspected black hole candidate with strong radio emission from a jet (Mioduszewski et al, 2001; Marti et al., 2001). The X-ray emission of Cyg X-3 quite distinctively shows low and high states (Rajeev et al., 1994; Nakamura et al., 1993), which correspond to hard and soft states (Choudhury & Rao, 2002), distinguished by the shape of the X-ray spectra characterized, chiefly but not totally, by the presence (or absence) of multicoloured disk blackbody component and the power-law index (albeit with the individual model components more complicated than the canonical X-ray states of classical black hole candidates characterized, chiefly, by Cyg X-1, see, for eg. Tanaka & Lewin 1995). In Paper 1 we reported a strong and significant correlation between the radio and the soft X-ray emission (2 – 12 keV, \[RXTE-ASM\] in the hard state of Cyg X-3, while the hard X-ray (20 – 100 keV, CGRO-BATSE) anti-correlates with both the soft X-ray and the radio, the last anti-correlation was first reported by McCollough et al. (1999). The wide-band X-ray spectral analysis of the pointed RXTE observations in this hard state of the source at different radio flux levels show a definite pivoting of the spectrum around 12 keV correlated to the radio emission (see Figure 3 and Table 2 of Paper 1, ). As the interrelationship between radio and X-ray flux reported in Paper 1 has significant implications for connectivity between accretion disk and radio jet, we have explored other black hole candidates, for which similar radio and X-ray data are available, for radio and X-ray flux correlation analysis.

Here we present results of our analysis for the two persistent X-ray binaries, microquasars and black hole candidates, Cyg X-1 and GRS 1915+105 for which quasi-simultaneous radio and X-ray data are available from GBI, RXTE-ASM, and CGRO-BATSE. We select data during periods when there are no radio flares and the source is bright both in radio and hard X-rays. We examine radio X-ray correlations in such hard states and show that these correlations are similar to those found in the low-hard states of well studied sources like GX 339-4. We complement our analysis of this state by giving a qualitative self consistent picture of the steady X-ray non-flaring states of these sources, along with Cyg X-3 and GX 339-4, using the Two Component Advective Flow (TCAF) model of Chakrabarti (1996).

## 2. Data and Analysis

Fender & Kuulkers (2001) have compiled an extensive list of X-ray binaries, both neutron stars and black hole candidates, for which simultaneous X-ray and radio observations have been made. The Green Bank Interferometer, West Virginia, operated by NRAO, provides data for a number of X-ray sources that were monitored during its several years of operation. Collating these sources with those monitored by RXTE-ASM and CGRO-BATSE we found two X-ray binaries (black hole candidates) viz. Cyg X-1 and GRS 1915+105, along with Cyg X-3, which are persistent in radio, soft and hard X-ray bands and for which (quasi) simultaneous data from the three observatories are available.

Figure 1 and Figure 2 give the daily averaged light curves of GRS 1915+105 and Cyg X-1, respectively, in the soft X-ray (ASM, top panel), hard X-ray (BATSE, middle panel) and the radio (2.2 GHz, GBI, bottom panel) during the period when all the three instruments were simultaneously monitoring the sources. Analogous to our approach for testing the correlation among the radio, soft and hard X-ray emission from Cyg X-3 (Paper 1), we have used the Spearman Rank Correlation (SRC) test and adapted the method of partial rank correlation to test the influence of the third parameter (Macklin, 1982). The SRC coefficient gives the strength of the correlation between two variables and the corresponding D-parameter gives the confidence level, in terms of standard deviation, that the derived correlation is independent of the influence of the third parameter. Here we also give the results of the correlation analysis for data averaged over different time intervals viz., 1, 5 and 10 days as well as correlation between X-ray hardness ratio (ratio of observed BATSE count rate to that of ASM count rate) and radio (ASM count rate is taken as the third parameter) for the duration in which the respective sources were in a relatively long term steady quiescent hard state. Table 1 gives the complete result of the Spearman Rank Correlation (SRC) test for the correlation among 1) the radio, soft X-ray and hard X-ray, and 2) the hardness ratio in X-ray and radio (GBI) for GRS 1915+105 and Cyg X-1 along with Cyg X-3, during the steady quiescent hard state of X-ray emission, for fluxes in different bands averaged over 1, 5 and 10 days.

As in Paper 1 for Cyg X-3, a detailed wide band spectral analysis of GRS 1915+105 has been done using the pointed mode observations by RXTE Proportional Counter Array (PCA) and High Energy X-ray Timing Experiment (HEXTE) instruments available in RXTE archive during the period of radio monitoring of this source by GBI. For this purpose, two sets of X-ray data in the $`\chi `$ (hard) state of the source and corresponding to two extreme values of the radio flux, within the of precincts of this state, have been used for detailed spectral analysis following the method described in Paper 1. These representative observations, corresponding to the extreme behavior of the sources within the precincts of the respective low and hard states, are marked as inverted arrows in Figure 1 and some features of these observations are given in Table 2. Two unfolded spectra for GRS 1915+105 are overlaid on bottom panel of Figure 3 with top panel showing similar spectra for two extreme values of radio flux in the similar state for Cyg X-3 for comparison purpose (from Paper 1, ).

### 2.1. Cyg X-3

Cyg X-3 is one of the brightest radio sources associated with an X-ray binary. It exhibits radio flares reaching up to 20 Jy in intensity, with a steady emission in the range of 40 – 150 mJy during the quiescent state (Waltman et al., 1995). Table 1 gives the result of the Spearman Rank Correlation test for fluxes averaged over 1, 5 and 10 days, during the radio quiescent state (see Paper 1, Figure 1), also corresponding to X-ray quiescent and hard state. Though the value of the SRC coefficient increases with increasing bin time, it should be noted that the number of degrees of freedom decreases and hence the best correlation result is obtained for one day averaging (as seen by the value of the null hypothesis probability). Hence the correlation time scale is shorter than a day. The X-ray hardness ratio shows a very strong and significant anti-correlation with the radio emission. Interestingly this anti-correlation is stronger and more significant than the anti-correlation of the hard X-ray flux with radio (or soft X-ray). This suggests spectral bending being correlated with the radio emission, amply demonstrated in the top panel of Figure 3 (see also Figure 3 Paper 1, ). The pivoting of the spectrum around 12 keV, as obtained from pointed RXTE observations, explains the anti-correlation between the soft (2 – 10 keV, RXTE-ASM) and hard X-ray (20 – 100 keV CGRO-BATSE) emission.

We provide the X-ray wide band spectra following the same procedure as adapted in Paper 1 (see also Vadawale et al., 2001a). The X-ray spectra of black hole sources contain a thermal and a non-thermal part, which are conventionally modeled as a disk black body spectrum and a power-law (or cut-off power-law) or more realistic models incorporating Compton scattering from thermal as well as non-thermal electrons (Zdziarski et al., 2001). Since our aim is to make a wide band description of the spectra to understand the broad features, we have adopted an analytically simpler model consisting of a disk black-body and Comptonization from thermal electrons (Sunyaev & Titarchuk 1980 \- the CompST model), plus an additional power law component required to fit the spectra in the quiescent and hard state (Choudhury & Rao, 2002). For this source the X-ray spectra below 5 keV is dominated by the numerous photoionization emission lines (Paerels et al., 2000) originating in the hot gas, probably from the dense stellar wind of the Wolf-Rayet companion, engulfing the binary system (Nakamura et al., 1993). Therefore the continuum disk blackbody emission, contributing in the energy range below 5 keV is obscured and hence needs more rigorous analysis and better resolved spectra, which is beyond the scope of this paper. Therefore we present the spectra above 5 keV, modeled with the CompST and power law component. Vadawale et al. (2002) have shown that CompST model gives a functionally correct description of the more elaborate numerical codes, although with slightly different parameters. Moreover, such composite models have been used earlier for Cyg X-3 (Rajeev et al., 1994). Table 2 gives the results of the spectral fitting, along with the soft X-ray (ASM), hard X-ray (BATSE) and radio (2.2 & 8.3 GHz, GBI) flux, of two observations corresponding to the extreme behavior of the source within the precincts of the hard state.

In Paper 1, more spectral data were presented that showed a systematic change in the wide band spectrum correlated with the radio flux. The available spectra showed a pivoting behavior around 12 – 15 keV. This fact, coupled with the strong correlation between the soft X-ray and radio as well as that anti-correlation of the hard X-ray flux with radio (and soft X-ray flux) strongly suggest that the spectral shape governed by a pivoting behavior at around 12 keV is responsible for the observed correlations.

### 2.2. GRS 1915+105

The X-ray binary GRS 1915+105 was first detected in 1992 (Castro-Tirado et al., 1992), and has been observed in the X-ray, radio and infra-red bands since then (see Belloni et al., 2002, for a review). Muno et al. (2001) classify the radio emission into three classes, radio faint, radio steep and radio plateau, and find that radio emission is always present in the hard steady X-ray state. This source is extremely variable in nature and it has been classified into several variability classes (Belloni et al., 2000). The $`\chi `$ class is the closest analogue to the canonical low-hard states of Galactic black hole sources (Rao et al., 2000). Belloni et al. (2000) identify three stretches of long duration $`\chi `$ classes and two of them ($`\chi _2`$ and $`\chi _3`$) have simultaneous BATSE and GBI observations. These two periods are demarcated by numbers in the top panel of Figure 1, and are used for the correlation analysis. The results of the SRC test, given in Table 1 are similar to that of Cyg X-3. The radio and soft X-ray fluxes are well correlated. The anti-correlation of the hard X-ray flux with both radio and soft X-ray flux is not as strong as in the case of Cyg X-3. The correlation time scale, as can be concluded from the strength of the correlation, is one day or less. The correlation between the X-ray hardness ratio and radio flux again gives results similar to those of Cyg X-3, suggesting a spectral pivoting correlated to the radio emission. Hence, it is evident that the radio X-ray correlation behavior in the steady long term hard state of this source is similar to that of Cyg X-3.

Two unfolded spectra for GRS 1915+105 corresponding to GBI 8.3 GHz fluxes of 17 and 77 mJy respectively are overlaid in the bottom panel of Figure 3. Table 2 gives the details of the soft X-ray (ASM), hard X-ray (BATSE) and radio (2.2 & 8.3 GHz, GBI) flux along with the best fit parameters of the spectral fitting (Vadawale et al., 2001a). It is interesting to note that the wide-band spectra at extreme radio emissions shows a cross-over at higher energies (20 keV) compared to Cyg X-3 and, by association, we suggest that a spectral pivoting occurring at higher energies is responsible for the observed correlations. A possible reason for a weaker anti-correlation between hard X-ray (20 – 100 keV) flux and soft X-ray (2 – 12 keV) flux (and radio) compared to that in Cyg X-3 is that in the case of Cyg X-3 the soft X-ray (ASM) and hard X-ray (BATSE) energy ranges are, correspondingly, below and above the pivot energy of around 12 keV, whereas for GRS 1915+105, the pivot energy is at higher energies of around 20 keV, and the spectrum is relatively harder.

Rau & Greiner (2003) have made a detailed study of all the $`\chi `$ state observations of GRS 1915+105 based on the analysis of four years of pointed RXTE PCA and HEXTE observations. They find no correlation between radio and soft X-ray flux (1 – 20 keV), however, they find an anti-correlation between radio and hard X-ray (20-100 keV) flux, and also find that the slope of hard power law spectrum correlates positively with the radio flux in the low hard state of the source with observations during high radio emission showing a softer spectrum. The latter results agree with our findings presented here. Rau & Greiner (2003) also report spectral pivoting occurring between 20 – 30 keV in X-ray spectra in hard state of GRS 1915+105. The results of Rau & Greiner (2003) are consistent with our findings, except that the radio and soft X-ray fluxes are not correlated in their data, whereas we find a good correlation between radio and soft X-ray flux. Our results are based on the ASM data which is not very sensitive to X-rays above 10 keV, whereas Rau & Greiner (2003) use the flux up to 20 keV using a model fit to the joint PCA and HEXTE observations. The lack of correlation between radio:soft X-ray could be due to the spectral pivoting around 20 keV, because of which the soft X-ray flux from iRXTE PCA data will comprise of both correlated and anti-correlated fluxes thus weakening or averaging out the correlation.

### 2.3. Cyg X-1

Cyg X-1 (Bowyer, 1965) is the first Galactic black hole candidate (Herrerro et al., 1995) whose optical counterpart, O9.7Iab super giant HDE 226868, was among the earliest to be identified for an X-ray binary (Bolton, 1972; Webster & Murdin, 1972). A persistent source in X-ray, radio (Braes & Miley, 1971) and optical, it shows a binary modulation with a period of 5.6 days in all the bands (Pooley et al., 1999; Brocksopp et al., 1999). The radio emission is weak, generally around 15 mJy, varying between 10 to 25 mJy in the low-hard X-ray state getting considerably weaker in the high-soft state of X-ray emission (Brocksopp et al., 1999).

Figure 2 gives the combined light curve of Cyg X-1 in the soft X-ray (2 – 12 keV, ASM, top panel), hard X-ray (40 – 140 keV, BATSE, middle panel) and the radio (2.2 GHz, GBI, bottom panel). The region 1 as demarcated in the top panel of the figure denotes the period of the long term low-hard state of the X-ray emission. Since our emphasis is on the study of the long-term correlated radio: X-ray behavior of this source in low-hard state, we consider only this period for the SRC test. The results of the SRC test for Cyg X-1 are given in Table 1. The table shows that pattern of the correlation between X-ray and radio emission for Cyg X-1 seems to be different than for Cyg X-3 and GRS 1915+105. The soft X-ray and radio fluxes are not as well correlated as for the other two sources, specially for 1 day averages, being only 0.29 compared to 0.68 and 0.56 for Cyg X-3 and GRS 1915+105 respectively. Nevertheless, the correlation is significant at the level of about one part in 106. The anti-correlation of hard X-ray (40 – 140 keV, BATSE) flux with the soft X-ray (2 – 10 keV) as well as radio (2.2 GHz, GBI) fluxes found for Cyg X-3 and GRS 1915+105 is not present in Cyg X-1. Instead, the SRC test shows that the hard X-ray positively correlates with the both soft X-ray and radio emission. Also the X-ray hardness ratio does not show any correlation with radio flux in the case of Cyg X-1, unlike for Cyg X-3 and GRS 1915+105.

Brocksopp et al. (1999) report a value of the SRC coefficient for soft X-ray:radio flux correlation in low-hard state of 0.3 for 1 day average, after removing the mean orbital light curve, which is close to 0.29 found by us for the same correlation, without removal of the orbital modulation effects. Brocksopp et al. (1999) point out that loose correlation of radio and soft X-ray fluxes (for their 1 day averages) may be partly due to the possible offset between the radio and X-ray long period ($``$142 days) light curves. They also give the scatter plot of ASM, BATSE and radio fluxes.

The strength of the SRC between the radio and the both soft and hard X-ray are similar (Table 1), showing moderately strong correlation, whereas the soft and hard X-ray flux show a very strong positive correlation, the SRC coefficient being 0.70 for 1 day averages. Further, ASM and BATSE observations are at different times during the day implying that intra-day variability is relatively weak compared to variability on longer time scales as both fluxes are strongly correlated over longer time scales. Clearly, the similarity between hard X-ray:radio and soft X-ray: radio flux correlation is because of strong correlation between hard and soft X-ray fluxes. As mentioned earlier, the radio emission in Cyg X-1 is quite weak (around 15 mJy) varying between 10 and 25 mJy in the low-hard state. As the GBI observations have an error of nearly 4 mJy, a detailed wide-band spectral analysis for two extreme values of radio flux, for finding the relation between the shape of the X-ray spectra and the radio emission and the pivoting behavior and the pivot energy, as done for Cyg X-3 and GRS 1915+105, is difficult to be carried out for Cyg X-1.

Zdziarski et al. (2002) have shown that the long term variability of the X-ray emission from this source in hard state comprises of two types of spectral variability, one corresponds to the change in the shape of the spectra (with spectral shape pivoting around 80 keV) with change in soft X-ray flux and the other corresponds to the change in total flux, with the spectra simply moving up and down parallel to each other with a constant shape, in the whole X-ray broad band. This may explain the lack of correlation between the X-ray hardness ratio and the radio flux as well as the comparative weakness of the strength of the SRC correlation between ASM and radio flux. Zdziarski et al. (2002) have analyzed the various correlations among the fluxes of the three energy channels of ASM (1.5 – 3, 3 – 5 and 5 –12 keV) along with the 20 – 100 keV and 100 – 300 keV flux of BATSE and the corresponding specific spectral index of these bands. They conclusively show that in the low-hard state of the X-ray emission, over long periods, the change in the spectral shape occurs with a pivoting around 50 – 90 keV. This explains that the BATSE flux, being dominated by the lower energy photons is very strongly correlated to the ASM flux. The lack of anti-correlation between the X-ray flux hardness ratio and the radio emission may also be explained by this fact, as the lower energy of the BATSE flux, below the pivot point, is correlated to the radio emission along with the ASM flux.

## 3. Discussion

### 3.1. Comparison with earlier results

The results presented in this paper will be discussed along with similar results for GX 339-4 reported by Corbel et al. (2000, 2003). The compact object in GX 339-4 is also believed to be a black hole (Hynes et al., 2003). Corbel et al. (2000) find that for GX 339-4, the radio flux is strongly correlated with both soft and hard X-ray, covering the range 3-200 keV, in low-hard state, similar to the results obtained by us for Cyg X-1.

If we consider the results of the radio, soft X-ray and hard X-ray correlation analysis for these four sources, at first glance no consistent picture of the correlated variability pattern emerges. However, it is immediately noticeable that Cyg X-3 and GRS 1915+105 have similar overall correlation pattern. For both, the soft X-ray flux is correlated with the radio flux, and the hard X-ray flux is anti-correlated with the both radio and soft X-ray flux. Additionally, the hardness ratio is also strongly anti-correlated with the radio flux. Wide band X-ray spectral analysis in the hard state for both the sources at different radio flux levels suggests pivoting of the spectrum around 10 – 25 keV correlated with the radio emission.

It can also be noticed that correlation among the radio, soft and hard X-ray fluxes for Cyg X-1 and GX 339-4 is similar. Both show a positive correlation among the radio, soft X-ray and hard X-ray fluxes. For Cyg X-1 the hardness ratio is not correlated with radio flux. Further, Zdziarski et al. (2002) find a pivoting of the X-ray spectrum of Cyg X-1 at higher energy of around 50-90 keV. Similarly, the wide band X-ray to gamma-ray spectral analysis of GX 339-4 (Wardzinski et al., 2002) has shown that there is a pivoting in the spectrum at energies $``$300 keV in the low-hard state of the source.

At this stage it will be worthwhile to note other similarities in the X-ray and radio emission characteristics of Cyg X-3 and GRS 1915+105 vis a vis Cyg X-1 and GX 339-4. Most notable are that the first two sources are the strongest and most variable radio sources amongst the Galactic X-ray binaries whereas both Cyg X-1 and GX 339-4 are amongst the comparatively weak and steady radio sources. On the other hand, both Cyg X-1 and GX 339-4 have a very hard X-ray spectrum compared to Cyg X-3 and GRS 1915+105.

Thus both X-ray sources with softer X-ray spectrum have a lower pivot energy and Cyg X-1 with a much harder X-ray spectrum has a much higher pivot energy, indicating that the pivot energy is directly related to spectral shape. The correlation between hard X-ray flux and radio and soft X-ray fluxes observed in Cyg X-1 and GX 339-4 can then be explained because hard X-ray flux (40 – 140 keV for Cyg X-1, 20-200 keV for GX 339-4) is around or below the pivot energy in these two sources and will, therefore, be correlated with the soft X-ray and thereby the radio fluxes. Thus, it is quite evident that X-ray fluxes below and above the pivot energy are anti-correlated for these X-ray sources and the reported differences between radio, soft X-ray and hard X-ray correlation amongst these X-ray sources is an instrumental artifact where the RXTE-ASM and CGRO-BATSE energy ranges are fixed and the pivot energy varies from source to source. This is supported by finding of Zdziarski et al. (2002) who report an anti-correlation between 1.5 – 3.0 keV and 100 – 300 keV flux and find a very weak correlation between 1.5 – 3.0 keV and 20 – 100 keV flux for Cyg X-1 in the low-hard state. Thus the X-ray – radio behavior of these X-ray sources are consistent in terms of correlation between soft X-ray, hard X-ray and radio emissions reported here.

### 3.2. The X-ray soft state and suppressed radio emission

In the previous sub-section we have shown that the X-ray radio emission characteristics in the hard states of the highly variable sources Cyg X-3 and GRS 1915+105 are similar to those seen in the low-hard states of the well studied black hole sources Cyg X-1 and GX 339-4, once we assume different pivot energy correlated to the radio emission. Here we explore whether the suppressed radio emission seen in the high-soft states of Cyg X-1 (Brocksopp et al., 1999) and GX 339-4 (Corbel et al., 2000) are seen in these two sources. We must caution that the identification of various spectral states using monitoring data is fraught with difficulties of flaring emissions which could be quite delayed in the various emission bands.

Corbel et al. (2000) show that with the X-ray state transition from low-hard to high-soft the radio emission evolves from a jet like synchrotron emission to quenched emission in GX 339-4. This state is generally preceded by a low-hard X-ray (with correlated radio emission) and followed by an X-ray off state (with radio off). For a comparative analysis we plot the radio (GBI, 2.2GHz) and soft X-ray (RXTE-ASM, 2-12 keV) scatter diagram in Figure 4 for Cyg X-3 (top panel), GRS 1915+105 (middle panel) & Cyg X-1 (bottom panel), for the non flaring states, which include hard as well as soft states. We have attempted to distinguish the high and low states by the soft X-ray flux and denoted them by open and filled symbols, respectively. For Cyg X-3 the major flares are excluded, and in the process we have excluded the (very low) quenched radio emission immediately preceding the major flares. For GRS 1915+105, too, the data for the radio flares are excluded. It is evident that even for these two sources the radio emission is suppressed in the high state, analogous to the canonical high-soft state. Cyg X-3 shows a very systematic behaviour, with the radio positively correlated to the soft X-ray in the hard state, until it transits to the soft state, where the radio emission is negatively correlated to the soft X-ray emission. For GRS 1915+105 the transition into the soft state with suppressed radio emission is not that drastic but definitely pronounced. Cyg X-1 shows a more scattered association between the radio and X-ray emission, but the suppression of the radio emission with higher ASM flux is evident. Hence, it can be comfortably claimed that the suppression of the radio emission with the X-ray state transition is a generally consistent feature of the X-ray binary systems (BHCs), irrespective of their individual spectral characteristics. Therefore a consistent picture of the accretion-ejection picture is emerging from the observational analysis of sources with apparently very diverse behavioural patterns.

### 3.3. A universal correlation and its origin

In the previous two sub-sections we have shown that the four sources, viz. Cyg X-3, GRS 1915+105, Cyg X-1 and GX 339-4, all show a consistent picture of accretion-ejection mechanism, with the radio emission correlated to the X-ray spectral pivoting in the low state and suppression of the radio emission in the high state following the X-ray state transition. The most notable feature, however, is the strong positive correlation between the radio and soft X-ray flux in the hard state of all the sources. This is similar to the correlation reported for GX 339-4 (Hannikainen et al., 1998; Corbel et al., 2000; Gallo et al., 2002) and V404 Cyg (Gallo et al., 2002)). We explore below whether the observed correlation is an universal phenomena among the Galactic black hole candidate sources.

In Figure 5, we show a scatter plot of the radio flux against the soft X-ray flux for Cyg X-1 (plus sign), Cyg X-3 (filled circles) and GRS 1915+105 (open circles), all in their corresponding low-hard and their analogous states. The data are normalized to a distance of 1 kpc, with the assumed distances of 2 kpc, 8.5 kpc & 12.5 kpc, respectively for the above three sources. For the soft X-ray flux (based on RXTE-ASM data) 75 ASM counts s-1 is taken as the observed Crab flux. Individual data points are the average value for a bin size of 5 days. Recently, Gallo et al. (2002) have detected a correlation between the radio flux (Sradio) and X-ray flux (SX) of the form Sradio = k S$`{}_{}{}^{+0.7}{}_{X}{}^{}`$ for GX 339-4 and V404 Cyg, all the way from the quiescent level to close to high-soft state transition. This relationship is also shown in Figure 5 as a dotted line (for GX 339-4) and dashed line (for V404 Cyg). The extents of the lines correspond to the data used for the fit in Gallo et al. (2002).

The remarkable feature of Figure 5 is that a simple relation seems to hold for all the black hole sources over close to 5 orders of magnitude variation in the luminosity, in the low-hard state. The data points for Cyg X-1 fall just below the correlation found for GX 339-4, whereas, the data points for GRS 1915+105 lie on the line extrapolated from the correlation derived for V404 Cyg. The data points for Cyg X-3 are parallel to those of GRS 1915+105. It should be noted here that Cyg X-3 shows a very strong orbital modulation which is most probably due to the obscuration of the accretion disk by a cocoon of matter surrounding the accretion disk. Hence the ‘true’ X-ray emission from the accretion disk should be larger than the observed one and the data points should move closer to the extrapolated line from GX 339-4 and V404 Cyg. Since Cyg X-3 is suspected to be a micro-blazar (Fender & Kuulkers, 2001), it is also quite possible that the radio emission is over-estimated due to strong beaming and Doppler boosting. It is also noteworthy that GRS 1915+105, the most massive stellar mass black hole known, has the highest intrinsic X-ray emission.

Fitting individual data points of the sources with a function of the form Sradio = k S$`{}_{}{}^{+0.7}{}_{X}{}^{}`$ gives the value of the constant term as 54 mJy, 235 mJy and 1376 mJy, respectively for Cyg X-1, GRS 1915+105 and Cyg X-3. These values should be compared to those obtained for GX 339-4 and V404 Cyg, 124 mJy and 254 mJy, respectively. The individual data points, however, are also consistent with a linear relation and the continuous line in the Figure 5 is a linear fit to the combined data of Cyg X-1 and GRS 1915+105.

Although we cannot completely rule out the possibility that the individual correlations of these sources may exist due to processes unrelated to one another, the fact that the data points for sources close to their ‘off’ states (GX 339-4 and V404 Cyg) occupy one extreme of observations while sources with repeated radio flares (Cyg X-3 and GRS 1915+105) occupy the other extreme strongly suggests of a common physical mechanism in operation in all the sources. One natural consequence to be explored is whether the radio and the X-ray emissions are emitted directly from the same source region. Since there are very strong observational evidences for the radio emission to be of synchrotron origin, it is tempting to assume that the X-ray emission too is emitted by the same process, but at the base of the jet. There are evidences for X-ray synchrotron emission being responsible for the X-ray spectrum of some black hole sources like XTE J1118+480 (Markoff et al., 2001) and part of the spectrum in sources like GRS 1915+105 (Vadawale et al., 2001a). However, for several black hole sources wide-band X-ray spectrum has been extensively studied and the spectral shape is inconsistent with a simple synchrotron emission. Further, the X-ray:radio correlation appears to be valid from ‘off’ state to low-hard and the associated analogous states, and all the way up to the intermediate state, and it is extremely unlikely that the bulk of the X-ray emission is due to synchrotron emission in all these states.

Recently Markoff et al. (2003) have suggested jet synchrotron emission as a possible way to explain the broadband (including X-ray) features of GX 339-4. To explain the observed correlation, their model predicts that the X-ray emission is mostly due to synchrotron emission (with a power-law spectral shape). Since the wide band hard X-ray/ low energy gamma-ray spectra of black hole sources in their hard states like GX 339-4 (Wardzinski et al., 2002), GRS 1915+105 (Zdziarski et al., 2001), and Cyg X-1 (Zdziarski, 2000) require thermal-Compton emission to explain the spectral shape, we explore below alternate models where the X-ray emission is primarily due to accretion disk emission.

### 3.4. X-ray spectral shape as the “driver” of the radio emission

The wide band X-ray spectral shapes of Galactic X-ray binaries with black holes as compact objects show a systematic and predictable behavior, particularly in well studied sources like Cyg X-1 (Zdziarski, 2000) and GX 339-4 (Wardzinski et al., 2002), where, in the low-hard state, the spectral energy distribution peaks at $``$ 100–300 keV, with the emission being dominated by thermal-Compton emission from a population of hot electrons. For sources which go to the ‘off’ state the X-ray spectrum is quite similar to the low-hard state, but at a very low intensity. In the intermediate state the soft X-ray flux increases and in the high-soft state the spectrum is dominated by thermal emission from the accretion disk. Although it is quite convenient to assume that the mass accretion rate is responsible for such systematic changes, there is no strong evidence for this (see Homan et al., 2001, for a different behaviour of XTE J1550-654). Nevertheless, one can safely conclude that some unspecified ‘accretion parameters’ causally affect the wide band X-ray spectral shape of black hole X-ray binaries.

The evidences presented in this paper strongly suggests that the very same ‘accretion parameters’ must be causally responsible for the radio emission, rather than the amount of soft X-ray emission, provided they account for the suppressed radio emission in the soft state. Such a hypothesis neatly explains the behavior of Cyg X-3, which is quite bright in all the three energy ranges and hence the observational uncertainty is quite low. It can also be noticed from Table 1 that the most significant correlation for Cyg X-3 is between the radio emission and the ratio of hard X-ray flux to soft X-rays. Though such an explanation is not very clear in other sources, all the available observations are consistent with this. Since the radio emission too shows increasing emission from ‘off’ state to low-hard state (in GX 339-4 and V404 Cyg), correlated behavior in low-hard state (the above two sources and Cyg X-1), and high radio emission in an intermediate state very close to the high state (in GRS 1915+105 and Cyg X-3) and suppressed radio emission in the high state (Cyg X-3, GRS 1915+105, Cyg X-1 & GX 339-4), we speculate that the soft X-ray intensity determines the spectral shape and the accretion disc condition in these sources, which in turn determines the amount of radio emission (in the X-ray quiescent hard state of these sources). The transition of the systems (Cyg X-3 & GRS 1915+105) into flaring state and their corresponding behavior in the radio as well as X-ray bands is an issue not discussed here.

### 3.5. The TCAF model for the X-ray:radio correlation

Though there are models describing the accretion disk emission (Zdziarski, 2000) or jet emission (Markoff et al., 2003), there are very few models which self-consistently solve the accretion and ejection phenomena seen in black hole sources. Since our findings suggest a close connection between these two phenomena, we attempt below to qualitatively explain the X-ray radio association using one such model: the Two Component Advective Flow (TCAF) model of Chakrabarti (1996). According to this model, the Compton scattered X-rays in a black hole source originates from a region close to the compact object, confined within the Centrifugal Boundary Layer (CENBOL). The X-ray spectral shape in various ‘states’ of the source essentially depends on the location of the CENBOL and a detailed description can be found in Chakrabarti & Titarchuk (1995) and Ebisawa et al. (1996). At low accretion rates, the CENBOL is far away from the compact object and the X-ray spectrum is dominated by a thermal-Compton spectrum, originating from the high temperature region within the CENBOL. In the transition state, the CENBOL comes closer to the compact object and the CENBOL can sometimes give rise to radial shocks, causing intense quasi-periodic oscillations, as seen in GRS 1915+105. In the high state, the increased accretion rate produces copious photons in the accretion disc which cool the Compton region, giving rise to very intense disk blackbody emission along with bulk motion Comptonization (a power-law in hard X-rays with a photon index of $``$2.5). At some critical accretion rates, the state transitions could be oscillatory as seen in GRS 1915+105 (Chakrabarti & Manickam, 2000).

The behavior of TCAF disks and the outflow has been studied in detail in Das & Chakrabarti (1998). The outflow rate is found to be a monotonic function of the compression ratio, R, of the gas at the shock region. In this scenario, at low accretion rates, the CENBOL is far away from the compact object, and a weak shock can form with low compression ratio, giving low and steady outflow. If this outflow gives rise to radio emission, one can expect a relation between the radio emission and the X-ray emission. In this state (off state to low-hard state), an increased accretion rate increases the overall amount of energy available to the Comptonizing region and hence increasing the X-ray emission. The CENBOL location would be pushed inward, increasing the compression ratio (and hence increasing the radio emission) and also can increase the temperature and optical depth of the Comptonizing region, thus giving rise to a pivoting behavior at hard X-rays (50 – 90 keV) as seen in Cyg X-1 and GX 339-4. At increased accretion rate, the CENBOL can come closer to the compact region, giving the spectral and radio properties as seen in GRS 1915+105 and Cyg X-3. For a given accretion rate the compression ratio, after reaching a critical value (with the shock region coming correspondingly closer to the event horizon), causes the source to transit into the high-soft state state, for which the radio emission is progressively suppressed (Chakrabarti, 1999). This model qualitatively explains all the observed X-ray spectral and radio properties of Galactic black hole sources presented here.

## 4. Summary and conclusions

A complete understanding of the accretion-ejection physics in Galactic microquasars demands proper interpretation and modeling of all the varied states of X-ray and radio emission, encompassing the various flaring and steady emissions covering all ranges of time scales. In this paper we have taken a first step in this direction by attempting to understand the long term variation of the (non flaring) radio emission associated with the X-ray emission in the steady hard and soft states. We have analyzed the (quasi) simultaneous observations on GRS 1915+105 and Cyg X-1 using the RXTE-ASM, CGRO-BATSE and GBI data and made a detailed study of correlation between radio and X-ray fluxes. Based on this analysis along with discussion of earlier published results on Galactic microquasars we find that:

* A correlation exists between the soft X-ray and radio emission of GRS 1915+105 based on the data during the long $`\chi `$ state (associated to the low-hard state). The hard X-ray emission is anti-correlated with both radio and soft X-rays. There is a spectral pivoting at around 20 keV, correlated with the radio flux.
* Comparing these results with those of Rau & Greiner (2003) who found a strong correlation between radio emission and the X-ray spectral index in the $`\chi `$ states, we conclude that the X-ray and radio emission characteristics of GRS 1915+105 are similar to those of Cyg X-3 (Paper 1). The only difference lies in the values of the pivot energy of the X-ray spectra, which is around $``$12 keV in Cyg X-3 and around $``$20 keV in GRS 1915+105.
* A three way correlation among soft X-ray, hard X-ray and radio emission has been found in the low-hard state of Cyg X-1, confirming the results of Brocksopp et al. (1999). Comparing this result with those of Zdziarski et al. (2002) who have found that soft X-ray and hard X-ray above 100 keV are anti-correlated and also that there is a spectral pivoting at around 50 – 90 keV, we conclude that the X-ray:radio behavior of Cyg X-1 is similar to that of Cyg X-3 and GRS 1915+105, but for the fact that the pivoting energy is at a higher value.
* The X-ray:radio properties of Cyg X-1 are quite similar to that of GX 339-4, where a 3-way correlation between soft X-ray, hard X-ray and radio emission has been reported (Corbel et al., 2000, 2003). Though an anti-correlation between soft X-ray/radio with hard X-rays has not been reported in this source, we note that the X-ray spectrum during low-hard state too shows a pivoting behavior at high energies $``$300 keV (Wardzinski et al., 2002).
* The radio emission is suppressed for Cyg X-1 & GX 339-4 in their high-soft state and similarly for Cyg X-3 and GRS 1915+105 in their high states (with associated softer spectra). Therefore, all these four sources with apparent diverse X-ray and radio properties show very similar behavioural pattern encompassing the long term steady non-flaring state.
* Compiling the soft X-ray and radio observations of the above sources (GRS 1915+105, Cyg X-3, and Cyg X-1) with the published correlation in GX 339-4 and V404 Cyg (Gallo et al., 2002), we find that all the sources show a monotonic increase of radio emission with the soft X-ray emission, spanning a 5 orders of magnitude variation in their intrinsic luminosities. Cyg X-3 deviates from a single relation by about an order of magnitude which can be reconciled if 1) the observed X-ray intensity is an under-estimate because of obscuration and/or 2) the observed radio intensity is an over-estimate because of beaming and Doppler boosting.
* If a common physical phenomena is responsible for such an uniform relation spanning across ‘off’ state to intermediate state, we argue that both radiations (X-ray and radio) are unlikely to be originating from a single mechanism like synchrotron emission.
* Finally, we invoke a Two Component Advective Flow (TCAF) model (Chakrabarti, 1996) to explain the accretion-ejection behaviour in these systems in the steady hard as well as soft states.

## Acknowledgements

This research has made use of data obtained through the HEASARC Online Service, provided by the NASA/GSFC, and the Green Bank Interferometer, a facility of the National Science Foundation operated by the NRAO in support of NASA High Energy Astrophysics Programs. The authors thank the anonymous referee for the extensive and insightful comments. MC and SVV have been partially supported by the Kanwal Rekhi Scholarship for Career Development. AKJ is grateful to P. S. Goel, Director, ISAC and K. Kasturirangan, Chairman, ISRO, for their constant encouragement and support during the course of this work.


text:
# Giant Helium Dimers Produced by Photoassociation of Ultracold Metastable Atoms

Permanent address: \]Calvin College, Grand Rapids, MI, USA. Permanent address: \]FOM instituut voor plasmafysica Rijnhuizen, and University of Twente, The Netherlands. Present address: \]Institut für Quantenoptik, Universität Hannover, Germany.

## Abstract

We produce giant helium dimers by photoassociation of metastable helium atoms in a magnetically trapped, ultracold cloud. The photoassociation laser is detuned red of the atomic $`2^3S_12^3P_0`$ line and produces strong heating of the sample when resonant with molecular bound states. The temperature of the cloud serves as an indicator of the molecular spectrum. We report good agreement between our spectroscopic measurements and our calculations of the five bound states belonging to a $`0_u^+`$ purely long-range potential well. These previously unobserved states have classical inner turning points of about 150 $`a_0`$ and outer turning points as large as 1150 $`a_0`$.

In the purely long-range molecules first proposed by Stwalley et al. Stwalley , the binding potential depends only on the long-range part of the atom-atom interaction, and the internuclear distance is always large compared with ordinary chemical bond lengths. Theoretical description of these molecules involves only the leading $`C_3/R^3`$ terms of the electric dipole-dipole interaction and the fine structure inside each atom. These well-known interactions allow precise calculation of potential wells and rovibrational energies. Previous experimental studies of such spectra in alkali atoms have utilized the technique of laser-induced photoassociation (PA) in a magneto-optical trap (MOT) Lett ; Cline . In addition to testing calculations of molecular structure, that work has produced precise measurements of excited-state lifetimes Mcalexander ; Jones ; Wang ; Gutterres  and has led to accurate determinations of s-wave scattering lengths for alkali systems, which are of interest for studies of Bose Einstein condensates (BECs)Abraham ; Gardner .

This letter reports novel spectroscopic measurements and calculations for extraordinarily long-range molecules that are produced when two 4He atoms in the metastable $`2^3S_1`$ state absorb laser light tuned close to the $`2^3S_12^3P_0`$ ($`D_0`$) atomic line at $`\lambda =1083`$ nm. As compared with the alkali dimers considered previously, the potential wells are shallower, and molecules are much more tenuous, with an internuclear distance reaching values as large as $`1150a_0`$ ($`a_00.53\AA `$, the Bohr radius). At such large distances, retardation clearly influences the dipole-dipole interaction. Moreover, these purely long-range molecular states of metastable helium are distinctive in that each atom carries a high internal energy (the $`2^3S_1`$ state lies 20 eV above the ground state). While one normally expects Penning ionization to destabilize such energetic molecules, we note that purely long-range interactions might rather suppress this process, since the atoms are effectively held apart by the same potential that binds them together. The absence of purely long-range resonances in recent PA experiments in Utrecht, which monitored ion production rates in a MOT, is consistent with this reasoning PrivateCom .

The present experiment differs significantly from reported PA measurements with 4He in a MOT Herschbach . Our atomic cloud is confined in a magnetic trap and cooled nearly to the BEC transition Pereira101 ; Robert . The phase space density is typically six orders of magnitude higher than in a MOT, so the PA process is much more efficient Pillet . In addition, our magnetically trapped atoms are spin-polarized in a single Zeeman sublevel of the $`2^3S_1`$ state, so the initial quasi-molecular state is $`{}_{}{}^{5}\mathrm{\Sigma }_{g}^{+}`$. Therefore, only ungerade excited states are accessible. Finally, whereas previous PA experiments have monitored only ions or trap losses, we use absorption imaging to detect heating effects in the atomic cloud. Molecular resonances that produce no ions or very little trap loss can still be detected with our method.

Fig. 1 shows the only two potentials that can be excited in our experiment in the vicinity of the $`D_0`$ atomic line. The photoassociation experiment consists in driving the transition from free pairs of $`2^3S_1`$ atoms to bound states in the purely long-range $`0_u^+`$ well connected to the $`2^3S_1+2^3P_0`$ asymptote. Measurements of the bound-state spectrum proceed as follows. About $`10^9`$ atoms are trapped in a MOT before being transferred into an Ioffe-Pritchard magnetostatic trap. An evaporative cooling sequence that utilizes RF-induced spin flips cools the atoms to 2-30 $`\mu `$K. The critical temperature for Bose-Einstein condensation is in the range 1 to 4 $`\mu `$K, depending on the density Pereira101 ; Pereira2 .

After cooling, the cloud is illuminated for a few ms by light from a “PA laser” beam containing all polarization components relative to the magnetic field axis. Just after this PA pulse, the cloud is released and then detected by means of destructive absorption imaging after ballistic expansion. The number of atoms, the peak optical density, and the temperature are thereby measured as functions of the PA laser frequency. Fig. 3 shows the optical density after contributions from atomic ($`D_0`$) absorption have been subtracted. For this broad scan, the PA laser is a temperature-controlled diode laser with a 3-MHz spectral width. A Fabry-Perot cavity is used to measure the frequency relative to a reference laser frequency locked to the $`2^3S_12^3P_2`$ atomic line. The accuracy of the PA frequency in this case is 10 MHz.

More accurate spectroscopy is performed with a PA beam derived from a cavity-stabilized laser (width 0.3 MHz) locked to the $`D_0`$ line. The PA beam is tuned to the molecular lines by acousto-optic modulators. Its intensity is set between 0.01 and 1 mW/cm2, and the exposure time between 0.1 and 10 ms. With this technique we can reach and zoom in on the four highest (v=1 to v=4) lines in the $`0_u^+`$ well. Fig. 4 shows typical experimental data for the line v=4. Figs. 4a) and 4b) demonstrate that the peak optical density drops significantly when the PA beam is resonant with a molecular line, even if trap loss is weak. This situation is explained by the strong heating indicated in Fig. 4c. The temperature increase provides a very sensitive diagnostic for resonances that produce little loss. Assuming that the heat deposited in the cloud is proportional to the number of molecules produced, we fit the frequency dependence of the temperature to a Lorentzian curve. The FWHM of the molecular lines is measured at low intensities to be 3.0(3) MHZ, within the expected range for the molecular radiative width ($`\mathrm{\Gamma }_{mol}2\mathrm{\Gamma }`$).

The heating mechanism that produces our signals can be roughly understood as follows. After absorbing a photon near the outer turning point, the molecular system can decay radiatively into two fast metastable atoms, each with a non-zero probability of being in the trapped state. Since the trap depth is 15 mK, fast atoms can remain trapped and heat up the whole cloud. This reasoning is supported by the fact that we can convert the heating into trap loss if, during a 10 ms thermalization time after the PA pulse, we apply an RF “knife” that removes fast atoms from the trap. The simultaneous measurement of small trap loss and significant temperature increase suggests that each molecular excitation heats the sample considerably. This is the reason why the temperature probe is so sensitive.

We measure the detuning $`\delta <0`$ of the PA laser relative to the $`D_0`$ atomic line. The initial $`2^3S_1`$ pair undergoes an inhomogeneous Zeeman effect due to the trapping potential. Additionally, the relative kinetic energy of the pair is characterized by a non-zero temperature $`T`$. Each of these effects contributes a $`\frac{3}{2}k_BT`$ Boltzmann term to the initial average energy of a pair. Hence, the binding energy $`hb<0`$ of a given vibrational state is $`hb=h\delta +2\mu B_0+3k_BT`$, where $`2\mu B_0>0`$ is the Zeeman shift for a $`2^3S_1`$ pair at the center of the trap. Additional recoil and mean-field shifts of order 10 kHz are neglected because they are much smaller than our experimental uncertainty. Each line is probed in different conditions of $`T`$ (2 - 30 $`\mu `$K), $`B_0`$ (300 mG - 10 G) and density ($`10^{12}`$ \- $`5\times 10^{13}`$ cm-3). Within the accuracy of our experiment we finally find no density or magnetic-field dependence of the binding energies, and for each line we estimate an uncertainty of $`\pm 0.5`$ MHz. Given this uncertainty and the range of magnetic field explored, we can infer an upper limit for the $`0_u^+`$ magnetic moment of $`0.04`$ Bohr magnetons 111Since pure $`0_u^+`$ states are not degenerate, only molecular rotation gives rise to a magnetic moment, which is therefore expected to be of the order of the nuclear magneton..

In order to interpret the experimental frequency spectrum quantitatively, we calculate the coupling between the atomic orbitals of one atom in the $`2^3S_1`$ state and another in the $`2^3P_{J=0,1,2}`$ state, which involves 54 molecular potentials. This coupling is constructed as a perturbative Hamiltonian in the basis of fine-structure-free atomic states. At large internuclear distances $`R`$, the lowest-order term of the electromagnetic interaction is the retarded dipole-dipole interaction Dashevskaya ; Meath , which is fully determined by the coefficient $`C_3=(3/4)\mathrm{}\mathrm{\Gamma }/k^3`$, where $`\mathrm{\Gamma }=2\pi \times 1.6248`$ MHz Drake  is the atomic linewidth, and $`k=2\pi /\lambda `$ is the wave number. This interaction includes no coupling between electronic orbital and spin angular momenta ($`\stackrel{}{L}`$ and $`\stackrel{}{S}`$) and is diagonal in the molecular Hund’s case (a) basis.

In the absence of $`\stackrel{}{L}`$-$`\stackrel{}{S}`$ coupling, the potential curves resulting from dipole-dipole interaction are purely attractive or repulsive and have a single asymptote. When we include the atomic fine structure in the Hamiltonian MovrePichler , the coupling gives rise to three distinct asymptotes and to anti-crossings between attractive and repulsive curves, leading to purely long-range potential wells 222The absence of hyperfine structure in 4He leads to relatively simple molecular potentials.. We construct the fine-structure coupling phenomenologically from $`2^3P`$ splittings that have been measured accurately FineStructSplit1 ; FineStructSplit2 . If there is no rotation, only the projection $`\mathrm{\Omega }`$ of the total electronic angular momentum on the molecular axis remains a good quantum number. Our experiment probes the $`0_u^+`$ purely long-range well plotted in Fig. 1.

We also consider how the rotation of the molecule can couple electronic states ($`\mathrm{\Delta }\mathrm{\Omega }=0,\pm 1`$), an effect that will leave $`\mathrm{\Omega }=0`$ and $`0_u^+`$ as only approximate labels. Ultimately, only the total angular momentum $`J`$ remains a good quantum number. Our final addition to the Hamiltonian is the operator $`\stackrel{}{\mathrm{}}^2/(2\mu R^2)`$ Hougen , where $`\stackrel{}{\mathrm{}}=\stackrel{}{J}\stackrel{}{L}\stackrel{}{S}`$ is the nuclear angular momentum operator. In the s-wave scattering regime, the initial ($`2^3S_1+2^3S_1`$) pair exists only in the $`J=2`$ state. Elementary group theory and Bose-Einstein statistics for the nuclei Hougen  dictate that $`J`$ in the excited state must be odd, namely 1 or 3. What is more, the Condon radius at which the transition occurs is so large that the excited molecule is in almost the same quantum state as a non-interacting pair of atoms in the $`2^3S_1+2^3P_0`$ state (Hund’s case (c)). Therefore $`J=1`$ is dominant.

The Hamiltonian including retarded dipole-dipole interaction, fine structure, and nuclear rotation is diagonalized numerically. The $`0_u^+`$ well cited above is found to remain almost pure; that is, the couplings to other $`\mathrm{\Omega }`$ subspaces are very small. It is 2 GHz deep and contains 5 bound states (see Fig. 1). The inner turning points of these bound states are around $`150a_0`$ and the outer turning point is as large as $`1150a_0`$ for the v=4 vibrational state. From the discussion above, it is clear that even the repulsive, inner part of the potential has purely long-range character; this fact distinguishes these dimers from those bound by usual chemical interactions. The large internuclear distance is also the reason why the next-order term in $`C_6/R^6`$ of the electromagnetic interaction is negligible 333We estimate the $`C_6/R^6`$ correction is at least 4 orders of magnitude smaller than $`C_3/R^3`$ for an internuclear distance larger than $`150a_0`$.. More detail about the theoretical approach will be given in a forthcoming paper 444The calculation exhibits two other ungerade purely long-range wells connected to the $`2^3S_1+2^3P_1`$ asymptote. They are even shallower and support fewer bound states than the well examined here. Their inner turning points are over 300 $`a_0`$..

Measured and calculated binding energies in the $`0_u^+`$ well are presented in Table 1. The measured spectrum agrees very well with the predicted J=1 progression, except for v=1, for which the 2 MHz discrepancy remains unexplained. Although it is too weak to be observed, the $`J=3`$ progression has been calculated to illustrate the expected rotational splitting. Finally, comparison with calculated results for a non-retarded dipole-dipole interaction demonstrates the significant influence of retardation. We note that our measurement confirms the assumed value of $`C_3`$ to within $`0.3\%`$.

In related work, we have measured other molecular lines, not belonging to purely long-range potentials, to the red of $`2^3S_1+2^3P_2`$. Their identification is under way. Additionally, an accurate measurement of the heat deposited in the cloud by decaying long-range molecules is in development; this could lead to a quantitative “calorimetric” method of measuring PA rates and thermal transport properties in the sample. Finally, this letter provides a foundation for a two-color, stimulated Raman experiment that would prepare molecules in the most weakly bound state of the $`{}_{}{}^{5}\mathrm{\Sigma }_{g}^{+}`$ potential shown in Fig. 1, with the $`0_u^+`$, v=0 state as an intermediate state. The corresponding Franck-Condon factor of $`0.1`$ suggests that the transition rate should be high. The lifetime of these atypical dimers formed from two $`2^3S_1`$ metastable atoms is unknown. Moreover, an accurate measurement of the s-wave elastic scattering length of $`2^3S_1`$ helium should follow directly from the measured binding energy Abraham .

Acknowledgements : The authors thank Peter van der Straten (Utrecht), the Cold Atoms and Molecules group at Laboratoire Aimé Cotton and the Cold Atoms group at Laboratoire Kastler Brossel for fruitful discussions. The work of APM is part of the research program of Stichting voor Fundamenteel Onderzoek der Materie (FOM) which is financially supported by Nederlandse Organisatie voor Wetenschappelijk Onderzoek (NWO). MW was partly funded by National Science Foundation Grant PHY-0140135, and TM by the Procope exchange program.


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# Detection of XY behaviour in weakly anisotropic quantum antiferromagnets on the square lattice

## Abstract

We consider the Heisenberg antiferromagnet on the square lattice with $`S=1/2`$ and very weak easy-plane exchange anisotropy; by means of the quantum Monte Carlo method, based on the continuous-time loop algorithm, we find that the thermodynamics of the model is highly sensitive to the presence of tiny anisotropies and is characterized by a crossover between isotropic and planar behaviour. We discuss the mechanism underlying the crossover phenomenon and show that it occurs at a temperature which is characteristic of the model. The expected Berezinskii-Kosterlitz-Thouless transition is observed below the crossover: a finite range of temperatures consequently opens for experimental detection of non-critical 2D XY behaviour. Direct comparison is made with uniform susceptibility data relative to the $`S=1/2`$ layered antiferromagnet Sr2CuO2Cl2.

Predictions of the Berezinskii-Kosterlitz-Thouless (BKT) theory BKT  for topological ordering with zero order parameter have been verified in many real systems, such as superfluid or superconducting films Mooij94  and Josephson junction arrays FaziodZ01 . However, despite the BKT theory being originally formulated as referred to 2D planar magnets, evidences of XY behaviour in real magnets are weak and limited to very peculiar cases BKTexp . On the other hand, for $`S=1/2`$ there exist several cuprous oxides that, besides being excellent realizations of 2D antiferromagnets, are known Johnston97  to display a weak exchange easy-plane (EP) anisotropy: unambiguous observations of XY critical behaviour in such systems are not easy to achieve, due to both the weakness of the anisotropy and the existence of finite inter-layer coupling. As for the former point, the EP anisotropy observed in real magnets is usually $`10^4÷10^3`$ times the isotropic exchange coupling, and the signatures of BKT critical behaviour are often either too weak to be extracted from the isotropic thermodynamics or too close to the critical temperature to be experimentally accessible. The residual inter-layer coupling, even if orders of magnitudes smaller than the intra-layer one, drives the system towards a 3D transition, which is actually triggered by the divergence of 2D intra-layer spin correlations. Therefore purely 2D critical behaviour of diverging quantities is most often masked by the onset of 3D long-range order.

In this work we show that several non-diverging quantities are sensitive to the presence of EP anisotropy and display an evident and detectable crossover between isotropic and XY behaviour above the expected BKT transition. Such crossover occurs at a temperature which is characteristic of the model and is marked by peculiar features in the temperature dependence of non-critical observables. In particular, we present quantum Monte Carlo (QMC) data for the uniform susceptibility, the finite-size staggered out-of-plane magnetization, the specific heat and the density of in-plane vortices.

We consider the $`S=1/2`$ easy-plane antiferromagnet on the square lattice described by the Hamiltonian

$$\widehat{}=\frac{J}{2}\underset{𝒊,𝒅}{}\left(\widehat{S}_𝒊^x\widehat{S}_{𝒊+𝒅}^x+\widehat{S}_𝒊^y\widehat{S}_{𝒊+𝒅}^y+(1\mathrm{\Delta })\widehat{S}_𝒊^z\widehat{S}_{𝒊+𝒅}^z\right)$$
(1)
where $`𝒊=(i_1,i_2)`$ runs over the sites of a square lattice, $`𝒅`$ connects each site to its four nearest neighbours, $`J>0`$ is the antiferromagnetic exchange coupling and $`\mathrm{\Delta }(0,1]`$ is the EP anisotropy parameter. We use the reduced temperature $`t=T/J`$.

The above model is studied by means of QMC simulations based on the continuous-time loop algorithm Beard ; Evertz02 ; CRTVVprb02  for $`\mathrm{\Delta }`$ = 0.001, 0.02, and 1, and on lattice sizes from $`L=64`$ to $`L=200`$. Each MC run consists of $`10^4`$ thermalization steps, followed by $`1÷1.5\times 10^5`$ MC steps for measurements. Whenever possible, we implement improved estimators Evertz02  for the quantities of interest.

The class of EP antiferromagnets described by Eq. (1) is characterized by the possibility for the model to support non-linear topological excitations in the form of in-plane vortices (V) and antivortices (AV). Such excitations play a fundamental role in determining the thermodynamics and critical behaviour of the system, as described by the BKT theory relative to the classical planar rotator model. When both quantum and out-of-plane fluctuations are present, the BKT behaviour persists even in strongly quantum ($`S=1/2`$) nearly isotropic ($`\mathrm{\Delta }10^3`$) models CRTVVprb02 .

Nevertheless, there exist significant differences between the standard BKT phenomenology and the XY behaviour actually observed in quantum nearly isotropic antiferromagnets, where the out-of-plane spin component plays an essential role above the transition.

Let us consider a strongly anisotropic EP model ($`\mathrm{\Delta }1`$): At high temperatures the system, despite being disordered, already supports topological excitations in the form of well separated V and AV in the easy plane. As $`t`$ decreases V and AV attract each other, till V-AV pairs begin to form and a maximum in the specific heat is correspondingly observed. At the critical temperature $`t_{_{\mathrm{BKT}}}`$ V and AV are all paired and the topological transition occurs.

In the nearly isotropic case ($`\mathrm{\Delta }1`$), the picture is modified as follows. At high temperature the system is isotropically disordered. When $`t`$ decreases the EP anisotropy becomes effective enough to stabilize planar configurations and allow for V and AV to appear in the easy plane. This phenomenon, occurring at a temperature hereafter indicated as $`t_{\mathrm{co}}`$, may be thought of as a crossover between the isotropic and a more genuine XY behaviour, and suggests the temperature range $`t_{_{\mathrm{BKT}}}<t<t_{\mathrm{co}}`$ as the most appropriate for experimental observations.

We consider the dimensionless uniform susceptibility $`\chi _\mathrm{u}^{\alpha \alpha }`$, defined as

$$\chi _\mathrm{u}^{\alpha \alpha }=\frac{J}{L^2}\underset{𝒊𝒋}{}_0^\beta 𝑑\tau \widehat{S}_𝒊^\alpha (0)\widehat{S}_𝒋^\alpha (\tau ).$$
(2)
Fig. 1 shows its temperature dependence, which we find strongly characterized by the appearence of a minimum in the $`zz`$ component. A similar minimum has been indeed experimentally observed in Sr2CuO2Cl2 and suggested to be related to the onset of 2D XY behaviour Vakninetal97 .

A sound argument in favour of this interpretation is the following. An infinitesimal uniform magnetic field causes a finite response in an antiferromagnet via the canting mechanism: adjacent spins antialigned in the plane perpendicular to the field cant out of such plane and give rise to a net magnetization, while a negligible response comes from spins anti-aligned along the field direction. On this basis, we interpret Fig. 1. At high temperature, $`\chi _\mathrm{u}^{zz}`$ and $`\chi _\mathrm{u}^{xx}`$ behave in the same way and decrease upon decreasing $`t`$ as antiferromagnetic coupling gets more effective and canting consequently harder. As $`t`$ is further lowered, the anisotropy starts to play a role, and most of the spins antialign in the easy plane: therefore, compared to the isotropic case, the number of spins responding to a field applied in the plane (along $`z`$) decreases (increases). As a consequence, $`\chi _\mathrm{u}^{xx}`$ decreases faster, while $`\chi _\mathrm{u}^{zz}`$ slows down its decrease; the further reduction of out-of-plane fluctuations is eventually responsible for the low-temperature increase of $`\chi _\mathrm{u}^{zz}`$. A clear minimum consequently appears and marks the crossover to XY behaviour at the temperature $`t_{\mathrm{co}}`$, where the out-of-plane component of the antiferromagnetic coupling becomes irrelevant. No particular feature is instead seen at the transition.

In order to check the direct relation between the crossover phenomenon and the out-of-plane fluctuations, we consider our data relative to finite-size out-of-plane staggered magnetization, $`m_{\mathrm{s},\mathrm{L}}^z`$ ; such quantity, which obviously vanishes at all temperatures in the thermodynamic limit, is quite useful when local spin configurations are under analysis, as in our case. In the inset of Fig. 1 we show data for different lattice sizes and $`\mathrm{\Delta }=0.02`$. By lowering $`t`$, $`m_{\mathrm{s},\mathrm{L}}^z`$ increases (as expected in the isotropic behaviour) above $`t_{\mathrm{co}}`$, and decreases (as expected in XY behaviour) below $`t_{\mathrm{co}}`$: a stable maximum is seen at $`t_{\mathrm{co}}`$. From the above evidences we obtain the estimates $`t_{\mathrm{co}}(\mathrm{\Delta }=0.02)=0.30(1)`$ and $`t_{\mathrm{co}}(\mathrm{\Delta }=0.001)=0.225(10)`$. Signatures of the crossover are also present in the staggered out-of-plane susceptibility and out-of-plane correlation length (shown in Ref. CRTVVprb02, ), displaying a maximum at a temperature quite close to $`t_{\mathrm{co}}`$.

The above results suggest that the crossover phenomenon is peculiar to the system and is due to the suppression of out-of-plane fluctuations. In particular, $`t_{\mathrm{co}}`$ is the temperature below which the weakly anisotropic system behaves like a planar rotator model with a spin length effectively reduced by out-of-plane fluctuations. Other authors have referred to such crossover as due to a ”spin-dimensionality reduction”, meaning the loss of one spin component Vakninetal97 .

By the semiclassical reasoning in Appendix B of Ref.CRTVVprb02,  we can predict $`t_{\mathrm{co}}`$ to depend on the anisotropy parameter $`\mathrm{\Delta }`$ according to

$$t_{\mathrm{co}}\frac{4\pi \rho __\mathrm{S}/J}{\mathrm{ln}(C/\mathrm{\Delta })},$$
(3)
where $`\rho __\mathrm{S}`$ is the renormalized spin stiffness of the quantum isotropic model, and $`C`$ is a constant. A logarithmic fit to our data, shown in Fig. 2, gives $`C=160`$ and $`\rho __\mathrm{S}=0.214J`$, which compares well with the known value Beard  $`\rho __\mathrm{S}=0.180J`$.

The onset of XY behaviour below $`t_{\mathrm{co}}`$ is further supported by the temperature dependence of the specific heat $`c`$. In the planar rotator model such quantity displays a maximum well above the BKT transition. Fig. 3 shows our data for the weakly anisotropic model with $`\mathrm{\Delta }=0.02`$: an embryonic peak, out of the isotropic component, is seen at $`t=0.29(1)`$, slightly below $`t_{\mathrm{co}}`$. To clarify the actual meaning of such peak, we have also considered the density of in-plane vortices with unitary vorticity, defined as Bettsetal81

$$\rho __\mathrm{V}=\frac{1}{8}18\widehat{S}_𝒊^x\widehat{S}_𝒍^x+16\widehat{S}_𝒊^x\widehat{S}_𝒋^y\widehat{S}_𝒍^x\widehat{S}_𝒎^y,$$
(4)
where $`(𝒊,𝒋,𝒍,𝒎)`$ defines a plaquette of the square lattice (indices are ordered counterclockwise). Choosing $`z`$ as quantization axis, the above quantity is off-diagonal. The estimator of the bilinear term in Eq. (4) can be found in Ref. Evertz02, . In the same spirit we introduce the estimator for the quartic term in the context of the loop algorithm Roscilde02 .

By considering QMC data for $`\mathrm{\Delta }=1`$, shown in the inset of Fig. 3, we observe that the temperature derivative of $`\rho __\mathrm{V}`$ displays a maximum where the specific heat exhibits its peak. Both features mark therefore the onset of the formation of V-AV pairs. In Fig. 3 we show that this picture is fully reproduced by our data for $`\mathrm{\Delta }=0.02`$, thus confirming the XY character of our weakly anisotropic system.

From the experimental point of view, the above findings may be firstly used to easily characterize the anisotropy of the layered antiferromagnets: if a minimum in the out-of-plane component of the uniform susceptibility is observed above the transition, this is a signature of EP anisotropy (while a minimum at the transition suggests an easy-axis anisotropy, as shown in Ref. CRTVVprb02, ). Once $`t_{\mathrm{co}}`$ has been experimentally determined, Eq. (3) allows one to get an independent estimate of the bare anisotropy parameter $`\mathrm{\Delta }`$ of Eq. (1). As shown below, this is quite an essential point for interpreting the experimental data.

We now consider the layered cuprate Sr2CuO2Cl2, whose intra-layer spin-spin coupling of the Cu2+ ions has been proposed Grevenetal95  to be governed by the Hamiltonian (1) with $`J=1450`$ K. As for the anisotropy parameter $`\mathrm{\Delta }`$, the experimental analysis Grevenetal95  hands us the renormalized value $`\mathrm{\Delta }^{\mathrm{exp}}=0.00014`$, extracted from low-temperature measurements of the spin gap in the out-of-plane branch of the 2D spin waves propagating in the Cu-layers, by means of the approximated expression $`G=4JSZ_c\sqrt{2\mathrm{\Delta }^{\mathrm{exp}}}`$, where $`Z_c`$ is the zero-temperature value of the spin-wave velocity renormalization coefficient of the isotropic Heisenberg system Igarashi92 . The above $`\mathrm{\Delta }^{\mathrm{exp}}`$ is not hence the bare value appearing in Eq. (1), as it already contains quantum renormalizations. In fact, a more refined self-consistent spin-wave-theory calculation Roscilde02  leads to the expression $`G=4JSZ_c\sqrt{2Z_\mathrm{\Delta }\mathrm{\Delta }}`$ with $`Z_\mathrm{\Delta }=0.099`$, and hence $`\mathrm{\Delta }=\mathrm{\Delta }^{\mathrm{exp}}/Z_\mathrm{\Delta }0.0014`$.

Experimental data relative to the uniform susceptibility of Sr2CuO2Cl2 (from Refs. Vakninetal97,  and Vakninetal90, ) are shown in Fig. 4 together with our results for $`\mathrm{\Delta }=0.001`$; a constant offset for the experimental data has been introduced in order to take into account spurious temperature-independent contributions Miller02  to the measured values of $`\chi _\mathrm{u}^{\alpha \alpha }`$. The agreement is excellent for both the in-plane and the out-of-plane component; considering that no adjustment has been introduced for the temperature axis, the position of the minimum of $`\chi _\mathrm{u}^{zz}`$ is nicely reproduced, and a crossover temperature $`t_{\mathrm{co}}0.227`$ for the real compound is determined. When the critical region is approached, experimental data deviate from the theoretical predictions due to the fact that a purely 2D model is no longer sufficient to capture the thermodynamic behaviour of the real magnet, which is in fact characterized by an experimentally observed Néel transition at $`t__\mathrm{N}=0.176`$. Such transition temperature compares remarkably with the BKT transition temperature of the purely 2D model, $`t_{_{\mathrm{BKT}}}=0.175(10)`$: this confirms that the 3D ordering is induced by the incipient intra-layer BKT transition.

From our analysis we conclude that the experimental observation of a minimum in the transverse uniform susceptibility at a temperature which is well above the critical region, is a signature of EP character neatly detectable in real compounds even with very weak anisotropy. To this respect, we notice that the bare anisotropy value, needed for a quantitative comparison between experimental and theoretical results, significantly differs from the (measured) renormalized value, due to the relevance of quantum effects. Finally, two distinct regimes, separated by the crossover, can be identified in the disordered phase: an isotropic regime for $`t>t_{\mathrm{co}}`$ and a disordered XY regime for $`t__\mathrm{N}<t<t_{\mathrm{co}}`$. It is relevant that the crossover temperature can be obtained by measuring non-diverging quantities above the critical region, which is an experimentally feasible task.

In summary, by means of quantum Monte Carlo simulations we have shown that two-dimensional $`S=1/2`$ square-lattice antiferromagnets with a weak easy-plane anisotropy display a crossover from a high-temperature isotropic behaviour to a genuinely 2D XY behaviour at a temperature $`t_{\mathrm{co}}`$ which stays around 30$`\%`$ above the critical temperature $`t_{_{\mathrm{BKT}}}`$. We have moreover shown that Sr2CuO2Cl2 realizes these predictions, and therefore stands as a very clean example of weakly planar quasi-2D antiferromagnet. This represent a clear evidence of non-critical XY behaviour in a real layered antiferromagnet. Other evidences for an isotropic-to-XY crossover in Sr2CuO2Cl2 come from neutron scattering Vakninetal97  and NMR Suhetal96  experiments, and enforce our conclusions. Further work on such crossover effect in the above compound, as well as in other layered antiferromagnets with easy-plane anisotropy (as, e.g., Pr2CuO4), opens the perspective for a systematic investigation of the vortex phase in purely magnetic systems.

We thank D. Vaknin, L. L. Miller and V. Tognetti for fruitful discussions and correspondence. This work has been partially supported by the COFIN2000-MURST fund and the INFM Advanced Parallel Computing Project.