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# Optical Photometry and Spectroscopy of the SN 1998bw-like Type Ic Supernova 2002ap

## 1 INTRODUCTION

Core-collapse supernovae (SNe) are classified by their spectral (e.g., Filippenko 1997) and photometric properties (e.g., Patat et al. 1993). There are overwhelming indications that the observational differences in these objects result from differences in their progenitor stars. Red supergiants with a full, massive hydrogen envelope collapse to form SNe of Type II plateau; the “plateau” refers to a period of relatively unchanged optical brightness after maximum brightness. SNe of Type Ib occur through the same core-collapse process as Type II, except the progenitors are stripped of their outer hydrogen layer by either stellar winds or transfer to a companion; thus, the resulting spectra lack hydrogen. If further stripping occurs to the point of removing the deeper helium layer, the SN is considered to be of Type Ic.

Recently, a subclass of SNe Ic has been identified as having unusually high-velocity early-time ejecta reaching velocities of $``$ 30,000 km s-1(Galama et al., 1998). Models indicate that these objects can have up to 10 times the kinetic energy per unit mass of normal core-collapse SNe (Iwamoto et al. 1998; see, however, Höflich et al. 1999 for a model in which this type of event is caused by an aspherical explosion with normal SN Ic energetics). Besides being among the most energetic events in the Universe, one particular example of this subclass, SN 1998bw, has been associated with a long-duration gamma-ray burst (GRB 980425; Galama et al. 1998). This discovery strongly supports the hypothesis that the physical process associated with long-duration GRBs (at least those of low gamma-ray luminosity, like GRB 980425) is linked to the core collapse of stripped stars. Very recently, the optical afterglow of another, more luminous GRB (GRB 030329) also exhibited weak spectral features closely resembling those of SN 1998bw; accordingly, it has been given a supernova designation (SN 2003dh; Garnavich et al. 2003; Chornock et al. 2003; Stanek et al. 2003).

SN 2002ap was discovered on 2002 January 29.4 (UT dates will be used throughout this paper) in the nearby spiral galaxy M74 by Y. Hirose (Nakano et al., 2002). Reaching a peak brightness of $`V12.4`$ mag, SN 2002ap was well observed. Spectra were quickly obtained, and SN 2002ap was identified as a SN Ic similar to SN 1998bw (Kinugasa et al., 2002; Meikle et al., 2002; Gal-Yam, Shemmer, & Dann, 2002; Filippenko & Chornock, 2002).

SN 2002ap has been closely followed in X-ray, radio, and optical bands. Specifically, Berger, Kulkarni, & Chevalier (2002) discovered synchrotron self-absorption at radio wavelengths and Sutaria et al. (2003) found inverse-Compton scattering in X-rays. At early times, SN 2002ap had an inferred intrinsic continuum polarization of $`1\%`$. When modeled in terms of the oblate, electron-scattering atmospheres of Höflich (1991) this implies an asymmetry of at least 20% (Leonard et al. 2002; see also Kawabata et al. 2002 and Wang et al. 2003).

Mazzali et al. (2002) modeled the light curve and spectrum of SN 2002ap using early-time data. This model predicts a kinetic energy of $``$ $`(410)\times 10^{51}`$ ergs, an ejected mass of $`2.55`$ $`M_{\mathrm{}}`$, and a synthesized 56Ni mass of $``$ 0.07 $`M_{\mathrm{}}`$. The model also predicts that the progenitor of SN 2002ap had a main-sequence mass of $`2025`$ $`M_{\mathrm{}}`$. Maeda et al. (2003) fit a two-component model to a bolometric light curve of SN 2002ap constructed from several optical and infrared data sets.

In this paper, we present both early and late-time optical photometry and spectroscopy of SN 2002ap. (Some preliminary results were discussed by Filippenko 2003.) Along with an analysis of these data and comparisons with other stripped core-collapse SNe, we calculate a model of the nebular spectra, complementing the early-time modeling of Mazzali et al. (2002). In Section 2, we present photometry in $`UBVRI`$ bands from the day after discovery and lasting for $``$ 10 months. In Section 3, we show 13 spectra ranging from 5 d to 386 d after $`B`$ maximum. Section 4 contains the results of our nebular modeling. We summarize our conclusions in Section 5.

## 2 Photometry

### 2.1 Photometric Observations and Data Reductions

On 2002 January 30, one day after the discovery of SN 2002ap, the Katzman Automatic Imaging Telescope (KAIT; Filippenko et al., 2001) at Lick Observatory began a $`UBVRI`$ monitoring program that lasted until 2002 March 9 when solar conjunction prevented further observations. After the SN became visible again in the morning skies, we obtained additional $`BVRI`$ photometry using the 1.0-m Nickel telescope at Lick Observatory and the 1.5-m Oscar Meyer telescope at Palomar Observatory.

KAIT obtained images of SN 2002ap (600 s in the $`U`$ band and 300 s in $`BVRI`$ bands) using an Apogee AP7 CCD camera, which has a back-illuminated SITe $`512\times 512`$ pixel CCD. At the $`f/8.2`$ Cassegrain focus of KAIT, the 24 $`\mu `$m pixel of the chip yields a scale of $`0\mathrm{}.8`$ pixel-1, making the total field of view of the camera $`6\mathrm{}.7\times 6\mathrm{}.7`$. The typical seeing at KAIT is $``$ 3$`\mathrm{}`$ full width at half maximum (FWHM), so the CCD images are well sampled.

For late-time observations, the camera at the Nickel telescope with a back-illuminated $`2048\times 2048`$ pixel Loral CCD was used in a 2$`\times `$2 binned mode, yielding a scale of $`0\mathrm{}.36`$ pixel-1 and a total field of view of $`6\mathrm{}.1\times 6\mathrm{}.1`$ (Li et al., 2001). The typical images from the Nickel telescope have FWHM $`2\mathrm{}`$, so once again the images are well sampled.

Late-time observations with the Palomar 1.5-m telescope were made with the thinned $`2048\times 2048`$ pixel “CCD 13” in the unbinned mode. Each pixel is 24 $`\mu `$m in size for a scale of $`0\mathrm{}.38`$ pixel-1. Observations were made near an airmass of 1.06 with exposure times 600 s and 300 s in Johnson $`BV`$ and Cousins $`RI`$ filters, respectively. The typical seeing for these data was $``$ $`1.1\mathrm{}`$, yielding well-sampled images.

For the KAIT images, dark-current subtraction and twilight-sky flatfielding were done automatically at the telescope. Since the KAIT camera is thermoelectrically cooled, the camera temperature is somewhat unstable, and thus the dark current is not always cleanly subtracted from each image. Consequently, there is a small dark-current residual which varies from night to night that must be removed manually by adding or subtracting fractions of a long-exposure dark image. Negligible uncertainties in the photometry are introduced by the manual removal of the dark-current residuals since the SN and comparison stars are rather bright (Li et al., 2001). Cosmic-ray removal was accomplished with the IRAF111IRAF (Image Reduction and Analysis Facility) is distributed by the National Optical Astronomy Observatories, which are operated by the Association of Universities for Research in Astronomy, Inc., under a cooperative agreement with the National Science Foundation. *cosmicray* procedure in the DAOPHOT package (Stetson, 1987). Reductions of the Lick Nickel and Palomar observations were routine, not necessitating manual adjustment of the dark-current image because the CCDs are cooled with liquid nitrogen.

Figure 1 shows a KAIT $`I`$-band image of SN 2002ap and 11 local standard stars taken on 2002 February 2.1. Absolute calibration of the field in $`BVRI`$ was accomplished with the Nickel telescope on 2002 June 11, June 12, and July 9 under photometric conditions. Calibrations for $`U`$ were obtained from Henden (2002). Table 1 shows photometry of the local standard stars acquired from those observations. Henden (2002) also provides $`BVRI`$ calibrations for the same stars which agree with our calibrations very well (within $``$ 0.02 mag of each other).

Since SN 2002ap is located about $`4.5\mathrm{}`$ from the nucleus of M74 and far from any bright spiral arms, we used simple aperture photometry to measure the instrumental magnitudes for SN 2002ap and the local standard stars in the KAIT images, when the SN was still bright. All local standard stars were measured except Stars 5 and 11, which usually had poor signal to noise ratio in the KAIT images. For the $`U`$, $`B`$, and $`V`$ observations of 2002 January 30, Stars 2, 3, and 6 were not included in the images and thus were not measured.

For the Lick 1.0-m Nickel and Palomar 1.5-m observations, we applied the point-spread-function (PSF) fitting technique to measure the instrumental magnitudes of SN 2002ap and the local standard stars, as the SN had already become quite faint in these images. The brightest stars (e.g., Stars 1, 6, 7, 8, and 9) are often saturated in these relatively deep images, and we used all the other unsaturated local standard stars to construct a PSF for each image. During the PSF-fitting process we also found that Stars 1 and 7 have nonstellar PSFs when they are not saturated, especially in the $`R`$ and $`I`$ bands, which are probably caused by the superimposition of some faint red background stars.

The instrumental magnitudes thus measured are converted to the standard Johnson-Cousins $`UBVRI`$ system using the following transformation equations:

$`u`$ $`=U+D_U(UB)+C_U`$
$`b`$ $`=B+D_B(BV)+C_B`$
$`v`$ $`=V+D_V(BV)+C_V`$
$`r`$ $`=R+D_R(VR)+C_R`$
$`i`$ $`=I+D_I(VI)+C_I.`$
Here, as in Modjaz et al. (2000), the lower-case bandpass letters signify our instrumental magnitudes and the upper-case bandpass letters denote magnitudes in the Johnson-Cousins system. The constants $`C_j`$ indicate differences between the zero points of the instrumental and standard systems, and the color-term coefficients $`D_j`$ for each telescope and setup are summarized in Table 2. Stars 1 and 7 were not used in the transformation due to their nonstellar profile as noted above.

During the transformation process, we found some peculiarities for the local standard Stars 2 and 3. When differential photometry was performed between SN 2002ap and these two stars for the KAIT images, the resulting magnitudes for SN 2002ap were systematically different (brighter by $`>3\sigma `$ and $`>10\sigma `$, respectively) from these derived from the other comparison stars. Yet, for the Lick 1.0-m and the Palomar 1.5-m images, both stars yielded measurements consistent with the other stars. We initially suspected that these were two variable stars, but their brightness remained the same during all the Nickel observations that spanned nearly 200 days. Another possible cause is that these two stars have peculiar colors, and when observed with CCD cameras of different quantum efficiency curves, their brightness may be systematically overestimated or underestimated, but the two stars seem to have quite normal colors compared to the other local standard stars. We were thus unable to find the cause of this inconsistency, and were forced to not use these two stars in the transformation. Fortunately, there are still enough local standard stars in the field that provide consistent measurements for the magnitudes of SN 2002ap, so we expect that our final photometry is not affected by this inconsistency.

Table 3 lists the final results from all of our $`UBVRI`$ observations of SN 2002ap, showing the early-time KAIT data and the late-time Nickel and Palomar data. Uncertainties, given in parentheses, were determined by combining in quadrature the errors given by the photometry routines in DAOPHOT with those introduced by the transformation of instrumental magnitudes onto the standard system. The uncertainties are dominated by the transformation errors at all times except for the very latest Nickel observations when SN 2002ap became fainter than 19 mag.

To double check our calibration of the SN 2002ap field and the final photometry of SN 2002ap, we compared our results with those reported in the literature. Our calibration of the SN 2002ap field is consistent (to within $`\pm `$ 0.02 mag) with those reported by Henden (2002), Gal-Yam, Ofek, & Shemmer (2002), and Yoshii et al. (2003), including Stars 2 and 3. Our $`BVRI`$ photometry of SN 2002ap is also generally consistent with that reported by Yoshii et al. (2003) to within $`\pm `$ 0.03 mag, although the difference in the $`U`$ band can be as large as 0.15 to 0.2 mag. Notice that Yoshii et al. (2003) used only one local standard star (Star 7 in Figure 1) which is probably contaminated by other stars as discussed above, but they adopted an aperture that is sufficiently large to include light in the whole system at all times.

### 2.2 Distance and Reddening

Schlegel, Finkbeiner, & Davis (1998) estimate the Galactic interstellar reddening in the direction of M74 to be $`E(BV)=0.071`$ mag. As shown in Section 3, this value is in agreement with the color excess derived from the narrow Na I D lines in our spectra. Reddening of SN 2002ap from the gas in M74 is estimated by Klose, Guenther, & Woitas (2002) to be $`E(BV)=0.008\pm 0.002`$ mag based on the Na I D1 absorption feature at the redshift of that galaxy in a spectrum of SN 2002ap. The total extinction of $`E(BV)=0.079`$ mag is clearly dominated by Galactic sources, which is to be expected in light of the projected distance of SN 2002ap from the nucleus of M74. The Galactic and host extinction in each band were then calculated using conversion factors in O’Donnell (1994), assuming a Galactic dust model for M74. The results of this procedure are summarized in Table 4.

Currently, there is no Cepheid distance to M74. Using photometry of the brightest red and blue stars in the system, Sharina, Karachentsev, & Tikhonov (1996) and Sohn & Davidge (1996) found distance moduli of 29.32 mag and 29.3 mag, respectively. This distance modulus corresponds to a distance of 7.3 Mpc. Earlier studies of M74 give distance moduli which span a range of about 5 mag, but the values from Sharina et al. and Sohn & Davidge are both in the middle of this range and very consistent with each other. The internal error given by Sharina et al. is 0.11 mag. Sharina et al. also determined that the mean distance modulus for the M74 group is 29.46 mag differing by 0.14 mag from their distance modulus for M74, resulting in a distance of 7.8 Mpc to the M74 group. We will adopt the difference between the distance modulus of M74 and its group (which is larger than the internal error reported by Sharina et al.) as the uncertainty in the distance modulus. The error in the distance modulus of $``$ 0.14 mag clearly overwhelms the uncertainty in the reddening ($``$ 0.01 mag) in any discussion of the absolute magnitude of SN 2002ap. The absolute magnitude of SN 2002ap derived from a distance modulus of 29.32 mag is presented in Table 4.

### 2.3 Optical Light Curves

Figure 2 displays our $`UBVRI`$ light curves of SN 2002ap. The maximum brightness and time of maximum brightness in each band were estimated by fitting polynomials to the data points. Since the light curves are well sampled near maximum, there is little uncertainty in our results. Table 4 lists the date and magnitude of peak brightness in each band as determined by the fits. All relative dates are normalized such that $`t=0`$ corresponds to $`B`$ maximum on 2002 Feb $`5.8\pm 0.5`$. Mazzali et al. (2002) indicate that the explosion occurred on Jan $`28.9\pm 0.5`$, $``$ 8 d before $`B`$ maximum and $``$ 0.5 d before discovery.

In the following sections, we discuss the behavior of SN 2002ap in each bandpass relative to the stripped core-collapse SNe 1994I (Richmond et al., 1996; Richmond, 2003), 1999ex (Stritzinger et al., 2002), 1998bw (Galama et al., 1998; Sollerman et al., 2002), 1997ef (Garnavich, 2003), and 1985F (Tsvetkov, 1986), when the data are available in that bandpass. In each of the comparison plots (Figures 3 through 7) the light curves have been normalized to the time of $`B`$ maximum for each supernova and to the same peak magnitude in the plotted band.

Since SN 2002ap exhibits unusually high expansion velocities in its spectra at early times similar to those of the GRB-associated SN 1998bw, we include the light curves of SN 1998bw for comparison in $`BVRI`$ . We also compare SN 2002ap to the prototypical SN Ic 1994I and the SN Ib/c 1999ex in $`UBVRI`$ . Because of limited available data, we display only the $`V`$-band light curve of the high-velocity SN Ic 1997ef, another peculiarly energetic event like SN 1998bw. Because of a lack of data in other bands, we only examine the $`B`$-band light curve of SN 1985F, which has a similar nebular-phase spectrum to that of SN 2002ap.

#### 2.3.1 $`U`$ Band

Figure 3 shows the $`U`$-band light curve of SN 2002ap with the light curves of SNe 1994I, 1999ex, and 1998bw. Before maximum at $`t=1.8`$ d, SN 2002ap rose more quickly than SN 1999ex. After maximum brightness, SN 1998bw declined slower than any of these, while SN 2002ap declined slightly faster than SN 1999ex until $`t=11`$ d when observations of SN 1999ex ceased. SN 1994I declined more quickly than all other SNe.

#### 2.3.2 $`B`$ Band

Figure 4 shows the $`B`$-band light curve of SN 2002ap with the light curves of SNe 1994I, 1999ex, 1998bw, and 1985F. Before maximum, SN 2002ap rises faster than SN Ib/c 1999ex and the high-velocity SN Ic 1998bw. It appears that SN 2002ap rises at the same rate as (or slower than) SN Ic 1994I, but this conclusion is not definitive because of a relatively late discovery of SN 1994I.

¿From maximum brightness until $`t7`$ d, SN 2002ap declines similarly to SN 1994I, and SNe 1998bw and 1999ex decline more slowly. After $`t9`$ d, the decline rate of SN 2002ap is relatively stable, while SN 1994I starts declining more rapidly. SN 2002ap follows SN 1998bw until around $`t=20`$ d (at a slightly fainter magnitude relative to the peak) when SN 1998bw begins its slower late-time decline phase. SN 1999ex closely follows SN 1998bw until $`t=12`$ d, after which it begins fading more rapidly to follow the light curve of SN 2002ap.

Notice that SN 1985F has an extremely wide $`B`$ light curve relative to even the energetic SNe 1998bw and 2002ap. The slow rise and decline of the light curve suggest high energetics and a large 56Ni mass as in SN 1997ef (Iwamoto et al. 2000; cf. the $`V`$ light curve of SN 1997ef in Section 2.3.3).

At late times, SN 2002ap declines at a mean rate of $`0.017\pm 0.001`$ and $`0.016\pm 0.001`$ mag day-1 at $`120<t220`$ d and $`220t<310`$ d, respectively. Data are only available at late times for SN 1998bw in $`B`$ until $`t190`$ d ($`0.014\pm 0.001`$ mag day-1) and after $`t320`$ d ($`0.015\pm 0.001`$ mag day-1). SN 2002ap seems to have faded more quickly than SN 1998bw at late times. We cannot conclude that SN 2002ap faded more quickly than SN 1998bw during the interval $`200300`$ d because of a lack of data. In addition, SN 1985F declines at a rate of about $`0.012\pm 0.002`$ mag day-1 at late times, much slower than SNe 1998bw and 2002ap, and at $`t300`$ d is still about 1.5 mag brighter than either of these SNe. However, the early data for SN 1985F are sparse, which may have resulted in a poor calculation of its peak magnitude.

#### 2.3.3 $`V`$ Band

We present the SN 2002ap $`V`$-band light curve along with other comparison curves in Figure 5. Before $`V`$ maximum at $`t3`$ d, SNe 2002ap and 1994I rise much more quickly than SNe 1999ex and 1999bw; as in $`B`$, however, SN 2002ap rises slightly more slowly than SN 1994I.

After maximum brightness ($`t=320`$ d), SNe 2002ap, 1999ex, and 1998bw decline in a similar manner. The decline occurs at a significantly slower rate than the rise, unlike for SN 1994I, which fades precipitously after maximum. At $`t>20`$ d, SN 1998bw fades at a slower rate as it enters its late-time decline phase; meanwhile SN 2002ap continues its rapid decline.

SNe 2002ap, 1998bw, and 1997ef also have similar peaks, being noticeably broader than that of SN 1994I. Such broad peaks seem to be a characteristic of the high-velocity SN Ic “hypernovae,” as noted for SN 1997ef by Iwamoto et al. (2000). However, as discussed by Clocchiatti & Wheeler (1997), SN Ib/c light curves are heterogeneous, consisting of both fast and slow decliners. Clocchiatti & Wheeler (1997) determined SN 1994I to be a fast decliner, while Stritzinger et al. (2002) established that SN 1999ex is a slow decliner. Most SNe Ic tend to be fast decliners, but SN 1990B is an example of a slow-declining SN Ic (Clocchiatti et al., 2001). This heterogeneity is apparent from the light curves presented here.

During times $`120220`$ d and $`220310`$ d, SN 2002ap fades at a mean rate of $`0.022\pm 0.001`$ and $`0.017\pm 0.001`$ mag day-1 (respectively) in the $`V`$ band. SN 1998bw, on the other hand, fades at a nearly constant rate of $`0.019\pm 0.001`$ mag day-1 during the interval $`50380`$ d, so SNe 2002ap and 1998bw decline at nearly the same rate here during the nebular phase. In the early nebular phase, $`70<t<140`$ d, SN 1997ef declines at a mean rate of $`0.012\pm 0.001`$ mag day-1, much slower than either of the other two SNe.

#### 2.3.4 $`R`$ Band

$`R`$-band light curves of SNe 2002ap, 1999ex, 1998bw, and 1994I are presented in Figure 6. For the first 6 days, $`t=7`$ to $`1`$ d, SNe 2002ap and 1994I rise very quickly compared with SNe 1998bw and 1999ex, although SN 2002ap rises at a rate somewhat intermediate to SNe 1994I and 1998bw. SN 1994I reaches $`R`$ maximum at $`t1.5`$ d past $`B`$ maximum, while SNe 2002ap, 1999ex, and 1998bw each reach $`R`$ maximum at $`t4`$ d.

After maximum, SNe 1998bw, 1999ex, and 2002ap decline together for 16 d ($`t=420`$ d). Thereafter, SN 1998bw declines more slowly, while SNe 2002ap and 1999ex continue their earlier decline. Compared with the other SNe, SN 1994I fades precipitously after $`R`$ maximum.

In the late phase, SN 2002ap ($`0.016\pm 0.001`$ mag day-1, $`120<t<310`$ d) fades at a mean rate slightly faster than SN 1998bw ($`0.015\pm 0.001`$ mag day-1, $`120<t<370`$ d).

#### 2.3.5 $`I`$ Band

The $`I`$-band light curves of SNe 2002ap, 1998bw, 1999ex, and 1994I are presented in Figure 7. As with the other bands, SNe 2002ap and 1994I rise quickly relative to SNe 1998bw and 1999ex before maximum, with SN 2002ap intermediate between the rest. SN 2002ap then reaches maximum later than all the other SNe, but is most nearly coincident with the maximum of SN 1999ex.

In the post-maximum decline, SN 2002ap behaves like SN 1998bw until $`t17`$ d, after which SN 1998bw begins declining slightly faster. This is the opposite of what is observed in $`R`$, where after this time, SN 2002ap begins to decline slightly faster than SN 1998bw. The light curve of SN 1999ex also exhibits a behavior similar to SNe 2002ap and 1998bw in its post-maximum decline, but at a slightly lower magnitude relative to the peak. After this epoch, the light curves of SNe 2002ap, 1998bw, and 1999ex begin to converge toward their late-time decline phases. As in the other bands, SN 1994I declines very quickly after maximum and is not similar to any of the other SNe during this time.

At late times, SNe 2002ap and 1998bw decline at mean rates of $`0.019\pm 0.001`$ and $`0.017\pm 0.001`$ mag day-1 during the intervals $`120310`$ d and $`120370`$ d, respectively. Again, as in the other bands, SN 2002ap fades slightly more quickly than SN 1998bw in the nebular phase.

### 2.4 Optical Color Curves

In Figures 8, 9, and 10 we respectively present ($`BV`$), ($`VR`$), and ($`VI`$) color curves of SN 2002ap and two comparisons, SNe 1998bw and 1994I. Since the reddenings for the comparison SNe are not well known, we present all the curves uncorrected for reddening.

The $`(BV)`$ color curves in Figure 8 show that the color evolution of SN 2002ap is similar to that of SN 1998bw, but significantly different from that of SN 1994I in the early post-maximum epoch. However, a lack of late-time data for SN 1994I prevents a late-time comparison with SN 2002ap.

All three SNe show an approximately linear increase in color at $`t=015`$ d, although their slopes differ somewhat. At later times, SN 2002ap and SN 1998bw both exhibit a linear decrease in color after $`t=15`$ d, until $`t=30`$ for SN 2002ap and until $`t180`$ d for SN 1998bw. The late-time ($`BV`$) data for SN 2002ap are sparse, but after $`t200`$ d SN 2002ap appears to reach a plateau phase of nearly constant color.

The ($`VR`$) color evolution of SN 2002ap differs dramatically from the ($`BV`$) evolution. SN 2002ap and SN 1998bw appear to show similarities in early decline rate from $`t10`$ d to $`t=0`$ d and in a linear increase in color between $`t=0`$ d and $`t30`$ d. SN 1994I also displays somewhat similar behavior during these days. After $`t30`$ d, SN 2002ap exhibits a dramatic change, by becoming increasingly redder to a maximum at $`t250`$ d, after which it appears to enter another plateau phase. This behavior is mimicked by SN 1998bw at these late times. This epoch is similar to the plateau phase in ($`BV`$).

Figure 10 shows the ($`VI`$) color evolution of the SNe. At early times, SN 2002ap shows more similarities to SN 1994I, increasing in a similar, linear way. Both SNe rise quite dramatically from $`t0`$ d to $`t30`$ d, while SN 1998bw has entered a plateau phase at this time. Both SNe 2002ap and 1994I have a larger change in ($`VI`$) color than SN 1998bw. At late times ($`t100300`$ d), SN 2002ap becomes redder at a minimal rate, slightly reversing this trend only in the last few days. SN 1998bw displays similar behavior, only decreasing $`50`$ d later.

### 2.5 Overall Photometric Results

In $`UBVRI`$ , SN 2002ap rises quickly like the normal SN Ic 1994I, while it declines slowly like the high-velocity SN Ic 1998bw and the SN Ib/c 1999ex, making its $`UBVRI`$ light curves distinctly broader than those of a “normal,” SN 1994-like SN Ic. At late times, SN 2002ap is again more photometrically similar to SN 1998bw than to a normal SN Ic.

Our photometric parameters listed in Table 4 agree reasonably well with those found by Pandey et al. (2003) and Yoshii et al. (2003). Pandey et al. report that there is a “flattening” of the optical light curves, where after $`t30`$ d the flux decline rates are $``$ 0.02 mag day-1 in all passbands until solar conjunction. However, we did not observe this flattening because our observations ceased approximately when Pandey et al. began to see this effect. Also, Yoshii et al. (2003) state that the rise rate before peak is almost independent of bandpass, while the post-maximum decline rate is steepest in $`U`$ and is progressively shallower through $`I`$. Our data show wavelength-dependent photometric evolution not only after maximum, but also before (Figure 2).

The color evolution of SN 2002ap is quite similar to the evolution of SN 1998bw and dissimilar from the evolution of SN 1994I. However, the ($`VI`$) colors of SNe 2002ap and 1994I are relatively similar.

## 3 SPECTROSCOPY

Our spectroscopic observations of SN 2002ap began on 2002 February 11.2, 5.4 d after $`B`$ maximum and 13.3 d after the time of explosion found by Mazzali et al. (2002). They were halted 2002 March 11 when the supernova was in solar conjunction, but resumed on 2002 June 8.5 on a semi-regular basis.

Data were obtained with the Kast double spectrograph (Miller & Stone, 1993) mounted on the Lick Observatory 3-m Shane telescope, the Low Resolution Imaging Spectrometer (LRIS; Oke et al. 1995) mounted on the 10-m Keck I telescope, and the Echellette Spectrograph and Imager (ESI; Sheinis et al. 2002) mounted on the 10-m Keck II telescope. The position angle of the slit was generally aligned along the parallactic angle to reduce differential light losses (Filippenko, 1982). Table 5 lists the journal of observations.

All data were reduced using standard techniques as described by Li et al. (2001) and references therein. Flatfields for the red CCD were taken at the position of the object to reduce near-IR fringing effects. The spectra were corrected for atmospheric extinction and telluric bands (Bessell, 1999; Matheson et al., 2000c), and then flux calibrated using standard stars observed at similar airmass on the same night as the SN. All spectra in this paper have been deredshifted by the NED222The NASA/IPAC Extragalactic Database (NED) is operated by the Jet Propulsion Laboratory, California Institute of Technology, under contract with the National Aeronautics and Space Administration. redshift of each SN’s host galaxy ($`z=0.002192`$ for SN 2002ap). The SN 2002ap spectra were dereddened by the overall reddening of $`E(BV)=0.079`$ mag as determined in Section 2.2. The zero-velocity Na I D lines in our ESI spectrum have an equivalent width of $``$ 0.4 Å. By the relationship proposed in Barbon et al. (1990), this corresponds to a Galactic reddening of $`E(BV)0.1`$ mag, which is consistent with the value we have determined. All other spectra were also dereddened by the appropriate Galactic value from Schlegel, Finkbeiner, & Davis (1998).

We display our early-time SN 2002ap spectra in Figure 11. Line identifications for the early-time and late-time spectra are shown in Figure 12. With a lack of hydrogen, helium, and strong $`6150`$ Å Si II features, SN 2002ap is classified as a SN Ic (Kinugasa et al., 2002; Meikle et al., 2002; Gal-Yam, Shemmer, & Dann, 2002). The high velocities present at early times indicate that the object produced an especially large energy per unit mass of the ejecta. The broad features at $``$ 4500 and $``$ 5400 Å resemble those in the spectra of SN 1998bw, the prototypical “hypernova” associated with GRB 980425 (Galama et al., 1998). The type Ic classification, large velocities, and spectral similarity to SN 1998bw caused many to classify SN 2002ap as a “hypernova.”

Mazzali et al. (2002) attributed the feature at $``$ 3800 Å in the early-time spectra of SN 2002ap (see Figure 12) to Ca II H & K. The broad feature from $``$ 4700 to $``$ 5400 Å is caused by an iron blend. The small feature at 5700 Å was attributed to either Na I or He I. However, for reasons discussed below, the progenitor of SN 2002ap probably had very little helium; hence, the feature is most likely Na I. The features from $``$ 6000 to $``$ 6400 Å, from $``$ 7400 to $``$ 8000 Å, and from $``$ 8100 to $``$ 8700 Å are Si II, O I, and Ca II, respectively.

In Figure 13, we present an early-time spectral comparison of SN 2002ap with the “hypernovae” SNe 1998bw and 1997ef as well as the normal SN Ic 1994I at early times. SN 2002ap is very similar to SN 1998bw, somewhat similar to SN 1997ef (over the very limited available wavelength range), and less similar to SN 1994I. Specifically, SN 1994I has narrower lines and much better-developed P-Cygni profiles for the Na I D and Ca II near-IR triplet lines, with very strong absorption components. The size of the Ca II triplet relative to other features can be used to identify the age of a SN Ic (Matheson et al., 2000c). This suggests that SN 2002ap evolved more slowly than SN 1994I.

Figure 13 also shows that certain spectral features are washed out with higher velocity. Specifically, SN 1994I has a significant dip in the spectra around 5400 Å. This feature is also present in the SN 2002ap spectrum, although not as prominent, but is not visible in the SN 1998bw spectrum. This washing out is indicative of higher energy per unit mass.

Comparisons of velocity widths of the O I $`\lambda 7774`$ line and the Ca II IR triplet for SNe 2002ap, 1998bw, and 1994I are shown in Figure 14. For SN 2002ap, Filippenko & Chornock (2002) measured a photospheric velocity from O I $`\lambda 7774`$ of $``$ 9000 km s-1 at 5 d after $`B`$ maximum. This is consistent with measurements from Gal-Yam, Ofek, & Shemmer (2002) and similar to SN 1998bw at the same epoch. The figure shows that SN 1998bw has a slightly lower photospheric velocity at 9 d after $`B`$ maximum than SN 2002ap at 5 d past $`B`$ maximum. Photospheric velocity decreases rapidly at early times, but slows about a week after maximum. The large photospheric velocity seen in SN 2002ap suggests that SN 2002ap is more energetic per unit mass of ejecta than normal SNe Ic such as SN 1994I.

¿From both the photometric light curves and the spectral comparisons, it is evident that SN 2002ap ages more quickly than SN 1998bw or SN 1997ef. The faster aging and the lower velocities derived from the line widths indicate that SN 2002ap is less energetic than SN 1998bw (Kinugasa et al., 2002). Likewise, the slower aging relative to SN 1994I suggests that SN 2002ap is more energetic than normal SN Ic (for energetic comparisons, see Table 7).

The nebular spectra of SN 2002ap shown in Figures 12 and 15 have incredibly strong \[O I\] $`\lambda \lambda 6300`$, 6364 and Mg I\] $`\lambda 4571`$ emission. The Mg I\] line grows over time with respect to the \[Ca II\] $`\lambda \lambda 7291`$, 7324 doublet and the \[O I\] doublet. In our latest spectrum (taken on 2003 February 27, 386 d past maximum), the Mg I\] integrated flux is 40% the \[O I\] integrated flux. Since we see farther into the core of the progenitor with time, we are probably peering directly into the Mg-O layer. It is expected that observations at later times will show an even larger Mg I\] to \[O I\] ratio.

As seen in Figure 16, the features of SNe 2002ap, 1998bw, 1997ef, 1985F, and 1994I are all similar, but the relative strengths of some emission lines differ. Relative to \[Ca II\] $`\lambda \lambda 7291`$, 7324, the Mg I\] $`\lambda 4571`$ emission is strongest in SN 2002ap, with the other SNe having about the same line strength. The other striking difference is the very strong O I $`\lambda 7774`$ and Ca IR triplet in the spectrum of SN 1997ef. In contrast, the \[O I\] $`\lambda \lambda 6300`$, 6364 and \[Ca II\] $`\lambda \lambda 7291`$, 7324 have about the same strength in SN 1997ef as in the other SNe. The stronger permitted lines relative to forbidden lines is likely due to denser radiating material in SN 1997ef. Indeed, the excess emission near 5400 Å may be Fe II emitted by dense clouds, as in SN 1987F (Filippenko, 1989).

Another prominent feature is the near-IR Ca II triplet. This blend decreases in strength over time relative to \[Ca II\]. Matheson et al. (2000b, c) found that the strength of the Ca II triplet depends heavily on age for SNe Ib/c, and should decrease in strength over time, consistent with our spectra.

The feature covering 5200 to 5600 Å is probably a mixture of Mg and Fe lines. From modeling, we have seen that the shoulder of the feature may be \[Fe II\], whereas the emission at 5190 Å is probably Mg I\]. In some SNe with very dense ejecta, however, Filippenko (1989, SN 1987F) suggests that Fe II lines dominate.

The line profiles of Mg I\] $`\lambda 4571`$ and \[O I\] $`\lambda \lambda 6300`$, 6364 seen in Figures 12 and 15 are very sharp. Figure 17 shows these lines in detail. The lines have a narrow component at $``$ 555 km s-1 relative to the systemic velocity of M74 on top of a slightly broader base, as first seen by Leonard et al. (2002). Our ESI spectrum has a high resolution of $``$ 75 km s-1, confirming the results of Leonard et al. (2002). These profiles can be caused either by low-velocity gas clouds near the center of the forming nebula or from material lost earlier or expelled by the progenitor that is now in the circumstellar environment of SN 2002ap (for example, SN 1999cq; Matheson et al., 2000a). The other strong emission lines (\[Ca II\] $`\lambda \lambda 7291`$, 7329; Ca II IR triplet) might weakly show this profile; however, this is uncertain due to line blending.

Table 6 lists the relative line strengths for each nebular epoch of SN 2002ap. To compute these values, first we fit a cubic spline to a local continuum around each line. After subtracting the continuum, we integrated the flux in the lines. Since the examined lines are rather broad, other lines may add significant flux to the wings (especially for the Ca II IR triplet; Filippenko & Sargent 1986 showed that \[C I\] $`\lambda 8727`$ contributes to this feature). Furthermore, to avoid obvious adjacent, close lines, we made somewhat arbitrary determinations of the endpoints of each line. Changing these boundaries by a few Å will change the integrated flux slightly. Although this method is somewhat inaccurate, it does show that the Mg I\] increases in strength and the near-IR Ca triplet decreases in strength over time relative to \[Ca II\]. SN 2002ap had a Mg/O ratio comparable to that of SN 1994I, but larger than that of SN 1998bw.

Comparisons to other SNe Ic at late times confirm that SN 2002ap has the strongest oxygen and magnesium lines of any SN yet published. The best comparison is to SN 1998bw, which has strong \[O I\] emission, but its Mg I\] line is much weaker relative to either \[O I\] or Ca II than in SN 2002ap.

## 4 MODELING

We modeled the nebular spectra of SN 2002ap using a non-LTE nebular code (Mazzali et al., 2001). (Preliminary results in agreement with those presented here are given by Mazzali et al. 2003.) The code computes $`\gamma `$-ray deposition in a nebula of constant density and homogeneous composition, and produces a synthetic spectrum by balancing the collisional heating resulting from the $`\gamma `$-ray deposition and the cooling via line emission. Emission is mostly in forbidden lines, but some permitted transitions (e.g., Ca II) are also strong if the conditions are favorable. The model is characterized by the outer velocity of the nebula, which is derived essentially by fitting the width of the emission lines; the mass of 56Ni, which provides the heating; and the masses of the various elements required to reproduce the observed emission lines. The mass of 56Fe is derived from the decay of 56Ni. Since Fe lines are observed, all masses can be determined uniquely for a given distance and reddening.

The nebular spectra of SN 2002ap are similar to those of SN 1998bw. The strongest feature is \[O I\] $`\lambda \lambda 6300`$, 6364. However, the blend of \[Fe II\] lines observed at $``$ 5200 Å is much weaker in SN 2002ap than in SN 1998bw. Qualitatively, this is a confirmation of the suggestion that SN 2002ap synthesized much less 56Ni than SN 1998bw. Unfortunately, this makes it difficult to determine the mass of 56Ni with high precision, as the \[Fe II\] feature is typically observed with a small signal-to-noise ratio and blends with other lines may affect the measured flux. Also, as noted above, the Mg I\] line is much stronger, relative to the \[O I\] line, in SN 2002ap.

In order to increase the accuracy of our diagnostics, we therefore modeled three spectra, observed at different epochs. For all spectra we find that the outer velocity of the nebula is $``$ 5500 km s-1, and the 56Ni mass is $``$ $`0.09M_{}`$. The ejecta mass contained within the outer velocity is $``$ $`1.5M_{}`$. This mass is consistent with the corresponding value derived from the explosion model used by Mazzali et al. (2002). The model ejecta extend to much larger velocities. However, material at the highest velocities is too thin to contribute to net emission. Hence, the estimated mass here is a lower limit to the total ejecta mass.

Approximately $`0.6M_{}`$ of the ejecta mass is O, while Si and S contribute a combined mass of $``$ $`0.5M_{}`$, and the mass of C is $``$ $`0.2M_{}`$. The Mg mass is relatively small, $``$ $`0.005M_{}`$, which is, however, sufficient to form a strong line, and the same holds for Ca.

The value of the 56Ni mass derived from these nebular models is slightly larger than that derived from fitting the peak of the light curve. This is required mainly to fit the peak of the emission lines of \[O I\] and Mg I\]. However, these peaks are distinctly narrower than the rest of the lines, as was the case for SN 1998bw. This may indicate the presence of an inner concentration of matter (O, Mg), a possible signature of an asymmetric explosion (Maeda & Nomoto, 2003).

Figure 18 shows a comparison of the nebular spectrum of SN 2002ap observed on 2002 July 11, and a synthetic spectrum computed with a NLTE, 1-zone code. The fiducial epoch of the spectrum is 163 days after explosion.

## 5 DISCUSSION AND CONCLUSIONS

The strong O and Mg emission, along with the lack of H and He, suggest that SN 2002ap is a core-collapse event, where the hydrogen, helium, and perhaps most of the carbon/oxygen layers are stripped. The high velocities in the early spectra further support this hypothesis since more massive outer layers generally decelerate the ejected material more than less massive outer layers. In addition, stripping the outer layers decreases the amount of ejecta, which in turn causes the kinetic energy per unit of ejecta mass to increase.

The photometric and spectroscopic data suggest that SNe 2002ap, 1998bw, 1997ef, and 1994I are all related events. However, SN 1994I is distinctly different photometrically and spectroscopically from the other three SNe. The results of modeling of the spectra of these SNe are presented in Table 7. These models suggest that SNe 2002ap, 1998bw, and 1997ef may be unusually energetic SNe Ic. Because of their higher 56Ni mass, the gamma-ray trapping for SNe 1998bw and 1997ef was greater, resulting in broad light curves, while the light curves of the normal SN Ic 1994I are narrower and fade more rapidly. However, the 56Ni mass of SN 2002ap is not significantly higher than that of SN 1994I, yet SN 2002ap has much broader light curves. In addition, SN 1999ex has broad light curves without showing the high-velocity ejecta characteristic of SNe 1998bw and 2002ap (for a discussion of fast and slow-declining SNe Ib/c, see Clocchiatti & Wheeler 1997). SNe 2002ap and 1994I produced a similar 56Ni mass, despite the slightly larger energy of the former. Therefore, 56Ni mass is not a sufficient indicator of a peculiar SN Ic event similar to SN 1998bw.

The lack of hydrogen and helium, along with the strong \[O I\] and Mg I\] lines in the nebular spectrum of SN 2002ap, suggest that the progenitor’s outermost layers were stripped.

The stripped nature of the progenitor of SN 2002ap can be further investigated by examining the levels of magnesium and oxygen in its nebular spectra. A more heavily stripped star should reveal more of the oxygen/magnesium/neon shell, and therefore less of the carbon/oxygen shell, resulting in more magnesium (relative to oxygen) present in the nebular spectrum. The large Mg/O ratio of SN 2002ap relative to other SNe Ic indicates that we are seeing deep into the core of the progenitor of SN 2002ap, suggesting that the progenitor’s carbon/oxygen layer was more stripped than the progenitors of most SNe Ic including SN 1998bw. However, since no strong neon transitions are seen in the nebular spectrum, it is inconclusive whether the carbon/oxygen layer of the progenitor was completely stripped, revealing the oxygen/neon/magnesium layer. Modeling suggests that no realistic star can contain enough neon to show a strong, unblended neon line in the nebular phase. In addition, mixing and excitation effects may play a significant role in nebular \[O I\] and Mg I\] lines. Perhaps if there were a strong unblended optical carbon line, one could see Mg I\] increase and the carbon line decrease with increased stripping.

It has been suggested that SN 1985F was of type SN Ib (Matheson, 2000). However, there are only late-time spectra of SN 1985F, starting $``$ 160 d past $`B`$ maximum. The similarity of the SN 1985F spectrum in Figure 16 to that of SN 2002ap (specifically the \[O I\]/\[Ca II\] ratio), coupled with the very broad $`B`$-band peak, suggests that SN 1985F was not a SN Ib and was probably a high-velocity SN Ic.

Currently, there is a debate over how SNe 1998bw, 1997ef, 2002ap, and their spectrally similar cousins should be classified (see Gal-Yam, Ofek, & Shemmer 2002 for a discussion). Many researchers have called SN 2002ap a “hypernova.” However, the explosion energy of SN 2002ap was probably only slightly higher than that of a normal SN Ic, unlike the case for the more powerful SN 1998bw. Also, SN 2002ap showed no evidence of relativistic ejecta at radio wavelengths (Berger, Kulkarni, & Chevalier, 2002). Moreover, the “hypernova” classification distracts casual readers of the literature from the physical process involved in an event like SN 2002ap. Since “hypernovae” are probably the result of the core-collapse of a massive star, we feel these events should still be classified as supernovae.

The second portion of the classification discussion centers around calling these events Type Ic, Ic-peculiar, or Id. Since the spectra of SN 2002ap-like events are quite different from prototypical SN Ic spectra (such as SN 1994I), these events should not be classified as normal Type Ic. However, the spectra of these events are not drastically different from those of normal SNe Ic.

This degree of similarity and heterogeneity is seen with peculiar SNe Ia. In particular, despite the fact that the premaximum spectrum of SN 1991T contained no Si II or Ca II, which are defining characteristics of a SN Ia, SN 1991T is considered a SN Ia and was not given its own classification of “Ix.” Furthermore, the spectrum of SN 1991bg contained strong Ti II features, deviating from a typical SN Ia spectrum, but SN 1991bg is still considered to be a SN Ia (see Filippenko 1997 for a review of these objects). To distinguish an object similar to the prototype SN 1991T (or SN 1991bg) from “normal” SNe Ia, we classify it as a SN 1991T-like (or a SN 1991bg-like) SN Ia.

Since SNe 2002ap, 1998bw, and 1997ef all have spectra similar to that of SN 1994I (a typical SN Ic), with the presence of high-velocity lines being the largest difference, we feel it is unnecessary to use the “SN Id” designation for these objects. Instead, by continuing the syntax established with peculiar SNe Ia, we propose that a SN with a spectrum similar to that of SN 1998bw be classified as a SN 1998bw-like SN Ic. Under this naming scheme, the correct classification for SN 2002ap is that of a “SN 1998bw-like SN Ic.”

We thank the Lick Observatory and Keck Observatory staffs for their assistance; Aaron Barth, Saurabh Jha, and Ed Moran also helped with some of the observations. The W. M. Keck Observatory is operated as a scientific partnership among the California Institute of Technology, the University of California, and NASA; the observatory was made possible by the generous financial support of the W. M. Keck Foundation. The work of A.V.F.’s group at the University of California, Berkeley, is supported by National Science Foundation grant AST-9987438, as well as by the Sylvia and Jim Katzman Foundation. Additional funding is provided by NASA through grants GO-9114, GO-9155 and GO-9428 from the Space Telescope Science Institute, which is operated by the Association of Universities for Research in Astronomy, Inc., under NASA contract NAS 5-26555. KAIT was made possible by generous donations from Sun Microsystems, Inc., the Hewlett-Packard Company, AutoScope Corporation, Lick Observatory, the National Science Foundation, the University of California, and the Katzman Foundation. P.M.’s work has been supported in part by the Grant-in-Aid for Scientific Research (14047206, 14540223, 15204010) of the Ministry of Education, Science, Culture, Sports, and Technology in Japan.


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# Coexistence or Separation of the Superconducting, Antiferromagnetic, and Paramagnetic Phases in Quasi One-Dimensional (TMTSF)2PF6 ?

## I Introduction

The interplay (co-existence, segregation, or competition) of the magnetic spin ordering and the superconducting pairing of electrons is in the focus of the broad research interest. These effects are of the key importance for understanding the rich physics of high $`T_c`$ superconductors, heavy fermion compounds and also organic conductors . Indeed, for these materials, having low-dimensional electron systems, the phase diagrams are surprisingly similar on the plane “pressure”$`P`$ \- temperature $`T`$ (here by “pressure” we mean either externally applied pressure or internal “chemical pressure”, i.e. dopant concentration)- see Fig. 1a. The phase diagrams for these materials include a magnetically ordered phase, metallic, and superconducting phases .

The origin of the superconducting phase in (TMTSF)2PF6 remains puzzling; there are experimental and theoretical results pointing at a triplet mechanism of electron pairing . Therefore, the issue of the character of the phase border and the origin of the transitions between magnetic, superconducting, and paramagnetic phases (caused. e.g. by pressure changes) become of the fundamental importance . The most general approach to the problem was suggested by a symmetry theory, which incorporates descriptions of the magnetic and superconducting phases by introducing a superspin, whose three components correspond to magnetic- and two others to superconducting- order parameters . In the frameworks of this SO(5) symmetry theory, at a certain intermediate pressure there might exist a state in which all components of the superspin (magnetic and superconducting) are nonzero. Such a “microscopically” mixed state possesses magnetic ordering in the superconducting state. There are indeed experimental indications for the existence of a local magnetic order in the high temperature superconductors . Recently, the microscopically mixed state was experimentally found in the heavy fermion compound CeRhIn5 .

On a different footing, the microscopically mixed state has been suggested in Ref.  to occur in (TMTSF)2PF6 due to lacking of the complete nesting over the entire Fermi surface. On the $`PT`$ phase diagram, the mixed state should occupy a narrow strip of pressures just below the critical $`P_{SDW}`$ value. At temperature $`T=1.4`$ K, this region should be about 4% wide on the pressure scale.

One should admit an alternative possibility, where in the vicinity of the phase border, a macroscopically inhomogeneous state may arise; this state incorporates inclusions of the minority phase embedded in the majority phase. As an example, it is well known, that the two-dimensional Mott type insulators tend to the formation of phase-inhomogeneous states . It is also known that martensitic transformations  concomitant with phase segregated states take place in such materials, where the free energy of electron system (including the magnetic energy of spin ordering) depends linearly on lattice deformation. If the inhomogeneous state with spatially separated phases emerged on the border of the magnetic and superconducting states (see Fig. 1a), it would have demonstrated simultaneously magnetic and superconducting properties, similarly to those of the heterophase mixed state.

The mixed state, as well as the state with spatial phase-separation, are expected to exhibit similar purely superconducting or purely magnetic properties far away from the phase boundary, so that their behaviors are indistinguishable. However, in the close vicinity of the phase boundary $`(T_0,P_0)`$, properties of these two types of states are different. In principle, one may distinguish these two possibilities, if the system is forced to cross the phase border by varying pressure at constant temperature, along the vertical trajectory in Fig. 1 a. In particular, for the inhomogeneous state with inclusions of the minority phase, one might expects such effects as pre-history and hysteresis: the properties of the system at a given point of the $`PT`$ phase diagram may depend on the pathway which the system has arrived at this point, due to a path-dependent concentration of segregated phases. In contrast, there is no reason to expect history effects for the mixed state.

Straightforward performing such experiment represents a hard technical task. Nevertheless, such measurements of $`R(T)`$ at fixed pressure values have been described recently in Ref. , where the $`R(T)`$-dependence was studied for a number of pressure values $`P_i`$ in the vicinity of $`P_0`$. The authors of Ref.  observed hysteresis effects within the AF phase and fitted the set of the measured $`R(T,P_i)`$ curves using a simple percolation model (which modeled the inclusions of one phase into another one). It was concluded that the observed hysteresis in the $`R(T)`$-dependences reflects a macroscopically inhomogeneous state, i.e. a mixture of the two phases. We note, however, that the identification of the AF and metallic phases is not trivial; at zero magnetic field the signature of the AF state is the onset of the $`R(T)`$ rise with cooling. Under circumstances when the system may contain a new phase with apriory unknown conduction, such procedure may be potentially ambiguous; therefore, the conclusions made in Ref.  require additional verification.

In the current paper, we applied a different experimental approach. Using the magnetic field dependence of the $`TP`$ phase border for this compound, we swept the magnetic field at a number of fixed pressure values in the vicinity of $`(T_0,P_0)`$; the magnetic field caused changes of the phase boundary and the corresponding phase transitions between the AF and PM states. Thus, the magnetic field was used in our experiment for both, driving the system through the phase transition (instead of pressure), and for reliable identifying the phase content.

We observed strong prehistory effects in the resistivity (in the presence of magnetic field), similar to those reported in Ref.  for the $`B=0`$ case. Besides, we found prehistory effects also in the character of the magnetic field dependence $`R(B)`$, which occur when the system crosses the phase boundary. These results evidence for the macroscopically inhomogeneous heterophase state in the vicinity of the AF-PM border. Depending on the direction of the magnetic field sweeping, the minority phase extended across the phase border, deep into the majority phase. Observation of the hysteresis and prehistory effects is not consistent with the model of the microscopically mixed (coexisting) antiferromagnetic and paramagnetic states. Thereby, in the current paper we have unambiguously determined that the transition from the AF insulating to PM metallic phase takes place through emergence of a macroscopically inhomogeneous state with spatially separated phases. Thus, our results obtained by independent technique, are in agreement with the preceding data by Vuletić et al. .

## II The idea of the experiment

For the quasi-one dimensional compound (TMTSF)2PF6 at zero magnetic field, there is a narrow pressure range in the vicinity of $`P0.6`$ GPa, where the two electronic phase transitions take place as temperature decreases. Firstly, there is a transition from the paramagnetic PM metallic phase  to the insulating AF phase (spin density wave state), and further, from the AF state to the superconducting (SC) state. Figure 1 a shows the corresponding phase diagram , which incorporates the domains of the AF, PM, and SC phases. A vertical trajectory $`P=0.54`$ GPa on the phase diagram corresponds to the temperature dependence of resistance $`R(T)`$, shown in the inset to Fig. 1 a. Crossings of the phase boundaries are marked with dots on the vertical trajectory (Fig. 1 a) and on the measured $`R(T)`$ dependence.

### A Traditional approach: varying $`P`$ and $`T`$

In order to explore the character of the transition, one has to be able to unambiguously identify the phase character and component content in the vicinity of the phase boundary. Observation of the absolute resistivity solely at zero field can hardly provide the required information, for the resistance changes smoothly and insignificantly in the vicinity of the second order transition. To identify the pure homogeneous PM and AF states, one could, in principle, make use of the temperature dependence of conduction, which has an activated character in the AF phase and diffusive character with the “metallic” sign $`d\sigma /dT<0`$ in the PM phase. In practice, however, this would require $`R(T)`$ measurements over a broad temperature range, which is inaccessible in the AF phase. Indeed, for the most interesting regime in the vicinity of the contiguity of the three phases, $`T_0=1.3`$ K and $`P_0=0.61`$ GPa, the temperature range of the existence of the AF phase is limited both, from the high and low-side (see Fig. 1 a). Besides, direct studies of such transition by changing the pressure in situ (i.e. along horizontal trajectories in Fig. 1 a) at low temperatures represent a very hard technical task.

### B Alternative approach: varying $`P_0`$ and $`T_0`$

According to our measurements in magnetic field and the earlier results (see, e.g., Ref. , the AF/PM border $`T(P)`$ shifts to higher temperatures as magnetic field grows. Figure 1 b shows schematically the changes of the border with magnetic field. Due to the smooth and monotonic dependence of $`T_0`$ on magnetic field, this dependence may be used for varying $`T_0`$. Thus, the system may be forced to cross the border by varying the magnetic field at fixed values of pressure and temperature. Figure 1 b shows that when the initial $`P`$ and $`T`$ values (at zero field) are chosen in the vicinity but bigger than $`P_0`$, $`T_0`$, the phase trajectory of the system (trajectory 2) will cross the phase border with magnetic field growth. Thus, crossing the border occurs due to the changes in $`T_0(B)`$ and $`P_0(B)`$ at fixed $`T`$ and $`P`$ values. Besides, crossing the border in the presence of magnetic field causes qualitative changes in the behavior of magnetoresistance, which are used in the current work for identifying the phase state and phase content of the system.

## III Experimental

Two samples - (TMTSF)2PF6 single crystals have been grown using a conventional electrochemical technique; the typical sample sizes were $`2\times 0.8\times 0.3`$ mm3, along the crystal directions a, b, and c, correspondingly. The two nominally equivalent samples showed qualitatively similar behavior and had slightly different resistivity value at low temperature. Measurements were made by four probe ac lock-in technique at 32 Hz frequency. For electrical contacts, four $`25\mu `$m Pt-wires were attached by a graphite conductive paint to the sample along the most conducting direction a at the a-c plane. The sample and a manganin pressure gauge were placed inside a nonmagnetic pressure cell  filled with Si-organic (polyethilenesiloxane) PES-1 pressure transmitting liquid; a required pressure was created at room temperature. The Ohmic character of the contacts to the sample was confirmed by the negligibly small out-of phase component of the measured voltage drop between the contacts.

The pressure cell was mounted in a cryostat in the bore of a 16 T superconducting magnet. Measurements at temperatures $`T1.4`$ K were done in the cryostat with 4He pumping. For all measurements, the magnetic field was applied along the least conducting direction, c, of the crystal and current was applied along a. Temperature of the pressure cell was measured using the RuO2 resistance thermometer, and heat contact of the sample to the liquid helium (or mixture) bath was provided with Pt-wires. In order to implement the idea of measurements with crossing the phase border for the account of magnetic field changes, the pressure value has to be set in the interval $`0.620.64`$ GPa at $`T1.4`$ K.

## IV The results of measurements

The magnetic field dependence of the resistance is qualitatively different for three different trajectories (1, 2, 3) in the $`BPT`$ phase space, depicted on Fig. 1 b.

### A Trajectory 1

Figure 2 a shows a typical example of the magnetic field dependence of the resistivity, corresponding to the trajectory 1 on Fig. 1 b. For such trajectory, which entirely belongs to the AF domain, changes in the resistivity are not accompanied with hysteresis. Resistance increases monotonically with magnetic field; in strong field, the so called “Rapid oscillations” (RO) appear on the background of the monotonic $`R(B)`$ growth ; such $`R(B)`$ dependence is typical for the AF phase . The oscillations can be more clearly seen in the derivative $`dR(B)/dB`$, shown in the inset to Fig. 2 a. As pressure increases (but still remains less than the critical $`P_0(B)`$ value), the resistance magnitude decreases, whereas $`R(B)`$ dependence does not change qualitatively.

### B Trajectory 3

When the initial $`T,P`$ values are chosen essentially larger than $`T_0,P_0`$, the trajectory 3 of the system (Fig. 1 b) lies entirely in the PM domain over all range of the magnetic field changes. Figure 2 b shows that the magnetoresistance in this case has a character qualitatively different from that discussed above for the AF phase. As magnetic field increases, the smooth growth of $`R(B)`$ transforms into step-like changes, which are related to the developing cascade of transitions between the states with different nesting vector . In strong fields and at low temperatures, the transitions between the states with different nesting vector have a character of the 1st order phase transitions . Correspondingly, the step-like changes of $`R(B)`$ in strong fields are accompanied with hysteresis in $`R(B)`$ . Such hysteresis may be noticed in $`R(B)`$ traces in strong fields, presented in Fig. 2 b.

The inset to Fig. 2 b shows on the $`BT`$ plane the corresponding phase diagram, which includes different sub-phases of the field-induced spin density waves . On Figure 2 b, the $`R(B)`$ curve at $`T=Const`$ corresponds to the isothermal trajectory on the $`BT`$ phase diagram (shown in the inset to this figure) which sequentially crosses different sub-phases. The corresponding jumps in $`R(B)`$ are periodic in $`1/B`$  and well correspond to the phase boundaries on the known $`BT`$ phase diagram of the FISDW-regime (see inset to Fig. 2 b) .

Each individual subphase has its own nesting vector and the quantized Hall resistance value . Indices $`N`$ for different subphases in Fig. 2 b correspond to the number of filled Landau levels in the quantum Hall effect, and, simultaneously, determine quantized changes of the nesting vector . When pressure $`P`$ decreases (but still remans bigger than the critical $`P_0`$ value), the resistance magnitude smoothly increases whereas $`R(B)`$ dependence does not change qualitatively. The resistance jumps related to the phase transitions persist and monotonically shift to lower fields, thus indicating the shift of the phase boundaries .

### C Trajectory 2

When the initial $`P,T`$ values are chosen in the vicinity but slightly bigger than $`P_0,T_0`$, one can expect the phase trajectory 2 to cross the border with increasing magnetic field, as discussed above. The inset to Fig. 3 a shows the $`R(T)`$ dependence measured at $`B=0`$; it evidences for the true metallic initial state of the sample at $`P=0.64`$ GPa (which is close to the critical value $`P_00.61`$ GPa). When magnetic field increases, the resistance changes insignificantly up to $`B7`$ T (see Fig. 3a). Upon further increase of $`B`$ up to 16 T, the resistance sharply grows by 3 orders of magnitude. This growth indicates the transition from the metallic PM to insulating AF phase. On the background of the growing monotonic resistivity component, one can note the appearance of non-monotonic periodic variations of resistance (starting from $`B8`$ T), which are absolutely untypical for the AF phase.

As magnetic field is swept down (i.e. decreases from 16 T to 7 T), a strong hysteresis ($`20\%`$) is revealed in the resistance (Fig. 3 a), whereas the non-monotonic component of $`R`$ practically disappears. The $`R(B)`$ hysteresis and the appearance and disappearance of the non-monotonic component of resistance depend only on the absolute magnetic field value and do not depend on its direction (compare $`R(B)`$ and $`R(B)`$ in Fig. 3 a). The magnitude of hysteresis grows with magnetic field. Upon repeated magnetic field sweeps from 0 to 16 T, the described above $`R(B)`$ dependence reproduces fully. The non-monotonic component of the resistance is more clearly seen in the $`dR/dB`$ derivative shown in Fig. 3 b. It is worthy of note that the non-monotonic component is observed only when magnetic field is increased and is practically invisible when magnetic field is decreased from 16 T.

Vertical arrows in Fig. 3 b depict the locations of the FISDW phase boundaries, which were experimentally determined in Ref.  from the jumps in $`R(B)`$ versus field in the FISDW area of the pure PM phase. The location of peaks in $`dR/dB`$ in Fig. 3 b coincides well with the arrows (i.e. with the anticipated borders of the FISDW phases). The inset to Fig. 3 b demonstrates that these peaks are equidistant in $`1/B`$. For these two reasons, we may identify the observed peaks in $`dR/dB`$ with crossing the borders between the FISDW phases with $`N=65`$, $`54`$, $`43`$, and $`32`$, correspondingly, on the phase diagram Fig. 2 b upon isothermal sweeping the field.

We wish to stress once more that the existence of the peaks and their periodicity in $`1/B`$ would be quite natural for the PM state, but is absolutely unexpected for the AF state. On the $`dR/dB`$ dependence, the next peak ($`N=21`$) at $`B14`$ T is not seen, despite the peak amplitude is known to strengthen with decreasing $`N`$ . The absence of this peak indicates almost complete disappearance of the PM phase and the onset of the homogeneous AF state at the field of $`B=14`$ T. As an additional confirmation of this conclusion, we note that in stronger fields $`B>14`$ T rapid oscillations may be seen in Fig. 3 b; these RO oscillations are characteristic for the AF phase .

Magnetic field dependences of the derivative $`dR/dB`$ are shown in Fig. 4 for different temperatures. One can see that the hysteresis of $`R(B)`$ in fields sweeping up and down disappears as temperature increases. Note that at low temperature, the hysteresis reveals itself not only in the magnitude of $`R(B)`$ (and $`dR/dB`$) but also in the qualitatively different character of the $`R(B)`$ dependence. When the field is swept up, the $`R(B)`$ dependence exhibits jumps (marked by arrows in fields $`B=812`$ T). The jumps are characteristic for the FISDW phase transitions in the PM phase, whereas the system passed transformation to the AF phase starting from field $`B6`$ T; the strong growth of resistance in Fig. 3 a and the appearance of RO evidence for this transformation. When the magnetic field is swept down, these anomalous jumps are almost invisible and one can see only the anticipated RO oscillations .

## V Discussion of the results

The most essential results of our studies are as follows:
1) As expected, when the field increases (decreases) along the trajectory 2 (see Fig. 1 b), the system exhibits the phase transition. The steep, a factor of $`10^3`$, raise (fall) of the resistance at $`B6`$ T evidence for this phase transformation.
2) At the transition from the PM to AF phase, rather far away from the phase border, the magnetoresistance continues to exhibit residual signatures of the metallic (minority) phase. When the field grows, the signatures of the minority phase almost disappear and are not restored when the system approaches back to the same phase border (i.e. as field decreases). In other words, at such transition, a strong hysteresis is observed both, in the magnitude of $`R`$ and in the character of $`R(B)`$ dependence.
3) Upon return transformation from the AF to PM phase (with decreasing field), a hysteresis in the magnitude of $`R`$ is observed: at the transition, the resistance is noticeably higher than that for the pure metallic PM phase (or than the resistance value measured as the field grows from $`B=0`$). The “true” value of $`R`$ is restored only when the field is decreased to zero.

In view of the complicated character of the magnetoresistance behavior, which exhibits signatures of both phases, the experimental determination of the AF and PM phases becomes of the principle importance. According to the existing theory , the SDW-PM transition is expected to be either of the second, or weak first order. Experimental data are in agreement with this conclusion . In the vicinity of the critical pressure the SDW gap $`\mathrm{\Delta }`$, in general, might be small as compared to the antinesting parameter $`t_b^{}`$ . In this case, the pseudo-activated $`R(T)`$ dependence in the SDW phase would have a semi-metallic character and would be indistinguishable from the “metallic” $`R(T)`$ dependence, thus making the identification of the two phases difficult. However, for the specific 2D tight binding case in (TMTSF)2PF6, $`\mathrm{\Delta }`$ does not depend on pressure in the vicinity of the critical pressure and is not small at the transition . This agrees with experimental observations , where $`R(T)`$ was shown to have a pseudo-activated character with rather big gap in the vicinity of the critical pressure. We use therefore, the sharp growth of $`R(T)`$ (starting from $`B7`$T in Fig. 3 a) as a firm indication of the onset of the SDW phase.

### A Inhomogeneous state: phase separation or phase mixing ?

Manifestly, our experimental results do not fit the behavior, anticipated for a microscopically mixed state made of the two coexisting phases. For such a state, the hysteresis effects and the dependence of the phase content on the prehistory, should not occur. The behavior described above is also not typical for a homogeneously “overheated” or “overcooled” phases at the first order phase transitions, for the minority phase disappears smoothly with no sharp jumps in $`R`$. Besides, for the 2nd order transition in a homogeneous system, neither hysteresis nor “overheating/overcooling” should take place. In the domain of the phase space, where only PM or AF phase should exist, clear signatures of the opposite phase are observed beside the “correct” phase. Therefore, the appearance of the hysteresis and the distinct signatures of the presence of both phases in the same domain of the phase space, both evidence that the phase content of the system becomes inhomogeneous. From a theoretical viewpoint, the cascade of transitions could also exist in the AF phase (accompanied with a corresponding jumps in $`R(B)`$ . However, such cascade has never been observed experimentally in the AF phase. Furthermore, even if the cascade of transitions occurs, as a homogeneous state, it would not give raise to pre-history effects such as observed in our experiment.

The phase-inhomogeneous state is not a consequence of the inhomogeneity of the sample or of the external pressure. The experimental results which prove this are as follows:
1. The phase-inhomogeneous state was observed on two different samples; the hysteresis and prehistory effects were qualitatively similar in both samples (compare Figs. 3 b and 4).
2. The existence of the prehistory in the appearance of the phase-inhomogeneous state contradicts the assumption of the inhomogeneity of the sample or external pressure. Indeed, if such inhomogeneities exist, they would manifest always, and would not disappear at the field sweeping through the border of the 2nd order transition; therefore, the prehistory effects would not take place.
3. Hysteresis in the character of $`R(B)`$ dependence arises only at pressure and temperature values in the vicinity of the phase border ($`T_0,P_0`$). No history effects are observed when the system is moved away from the phase boundary in either pressure or temperature axes. This may be seen, e.g. in Fig. 4, where in strong fields $`B>12`$ T, rapid oscillations  have the same magnitude and phase for the field sweeping up and down.
4. Low residual value of the resistivity, $`60\times 10^6`$ Ohm$``$cm (see Fig. 3 a), evidences for high quality of the samples.

One could assume that the phase-inhomogeneous state arises due to a positive surface energy at the border between AF and PM phases, and therefore, the two phases are spatially separated. On the contrary, the microscopic coexistence of the two phases would require a negative surface energy. However, the existence of a noticeable surface energy would mean that this transition is of the well-pronounced 1st order; such assumption seems to disagree with theoretical predictions for the SDW phase transition  and experimental data .

### B Prehistory effects

The prehistory effect is the most unexpected among the results obtained, even more unexpected than the hysteresis. This phenomenon is illustrated on Fig. 5 b, where four different dependences $`dR(B)/dB`$ are compared; these dependences correspond to 4 trajectories ($`AB,BC,CD`$, and $`DE`$) shown in Fig. 5 a. When the system crosses the PM-AF phase border (at $`B6`$ T) and moves deep into the AF domain along the trajectory $`AB`$, the derivative $`dR(B)/dB`$ exhibits peaks (marked with vertical arrows). These peaks correspond well to the resistance jumps observed in the PM phase at crossing the borders between the FISDW sub-phases $`43`$, and $`32`$ ; correspondingly, the peaks have nothing in common with the AF phase in which the system is supposed to be for the given $`P,B,T`$ values. The existence of these peaks evidence that, at least, a part of the sample did not transform into the insulating AF phase and remains in the metallic PM phase. In the field $`B15`$ T, instead of the next anticipated peak (which would correspond to the FISDW transition $`21`$), one can see only weak oscillations reminiscent of the RO oscillations in the AF phase. This points out at almost complete disappearance of the PM phase and the onset of the homogeneous AF state.

### C Phase separation at zero magnetic field

In the described above experiments, the presence of the magnetic field was not of a principle importance. The role of the magnetic field was to produce a qualitative difference between the $`R(B)`$ dependences in the AF and PM phases; this is necessary to identify crossing the border and to reveal the phase content of the inhomogeneous state. In our view, the phase-inhomogeneous state with inclusions of minority phase imbedded into the majority phase must also arise in the transition from PM to AF phase with decreasing temperature (see the phase diagram in Fig. 1a). In this case, however, the resistance changes are anticipated to be weak and of a quantitative rather than qualitative character. Such measurements have been already undertaken in Ref. , and our task was to test or confirm these results for same samples in which we have determined the character of the transition in non-zero magnetic field.

For the experiment we have chosen the pressure $`P=0.5`$ GPa, which is less than the critical value. The results are represented in Fig. 6. For this pressure and $`B=0`$, the system transforms from the metallic to AF state as temperature decreases below $`T=7`$ K . At the transition, the resistance sharply raises and further grows with decreasing the temperature; this behavior corresponds to the onset of the insulating state (spin density wave). The variations of the resistance with temperature along the trajectory $`AB`$ are shown in Fig. 6 a. The final resistance value at point $`B`$ corresponds to the minimal temperature 4.2 K in this experiment.

According to the above assumption, at point $`B`$ the system has a spatially inhomogeneous phase content: beyond the majority insulating AF phase, it contains also inclusions of the minority metallic PM phase. The following experiment was done in order to check this assumption: the magnetic field was increased from 0 to 16 T; according to the above results, such strong field should destroy completely the inclusions of the minority phase. Figure 6 b shows resistance changes with increase (trajectory BC) and subsequent decrease (trajectory CD) of the magnetic field. After magnetic field is decreased to zero, the system returns to a state (point $`D`$) similar to the initial (point $`B`$). However, magnifying the data in the inset to Fig. 6 b reveals a small ($`5\%`$) increase in the resistance at point $`D`$ as compared to that at the initial point $`B`$. This minor difference evidences for decreasing the share of the well-conducting metallic phase. The observed hysteresis is weak, therefore its interpretation could hardly be done without preliminary studies of much stronger hysteresis effects in magnetic field. The hysteresis in our $`R(T,B=0)`$ measurements is essentially weaker than that in Ref. . The reasons for this might be related to a somewhat smaller deviation of the pressure from the critical $`P_0`$ value in Ref.  than in our studies. Indeed, the lower transition temperature $`T_{\mathrm{SDW}}=2.5`$ K in Ref.  as compare to $`T_{\mathrm{SDW}}=7`$ K in our studies (see Fig. 6 a) indirectly indicates for such difference.

As the field varies repeatedly from $`D`$ to $`C`$ and back, no irreversible changes in the resistance are observed; we conclude the inclusions of the metallic phase disappeared. Upon further increase of temperature at zero field, the resistance varies along the trajectory $`DA`$. Repeated coolings reproduce the trajectory $`AB`$ within 1% accuracy, the result which evidences for restoring the phase-inhomogeneous state.

## VI Conclusion

The experiments described above reveal hysteresis in the magnitude of the resistance and the character of its variation with magnetic field, which develop at the transition from metallic to antiferromagnetic insulator state. Furthermore, we found that the behavior of the resistance with magnetic field becomes prehistory dependent. These results evidence unambiguously for the occurrence of the inhomogeneous state in the vicinity of the phase boundary between the PM and AF phases; we conclude that this state consists of inclusions of the minority phase imbedded into the majority phase. No data are available yet on the spatial arrangement of the two-phase state. The conclusions we drawn, do not depend on any model assumptions about the spatial arrangement of the two-phase state, because for identifying the phase content we used qualitative difference in the magnetoresistance behavior in AF and PM states. Our results are in a good agreement with previous data , obtained in a different way.

The observed phenomena of the phase separation at the second order transitions are similar to those typically seen in martensitic transformations. If this analogy is not accidental, it suggests that the free energy of the electron system depends linearly on the charge or SDW distortion. This conclusion requires experimental verification.

The minority phase inclusions can be eliminated completely as the system moves far away from the boundary, deep in the majority phase domain. The hysteresis in the magnitude and in the field dependence of the resistance does not depend on time; it is a stationary and well reproducible effect. The most striking evidence for the heterophase content was obtained from experiments in finite magnetic fields. However, similar phase-inhomogeneous state has been also observed in zero field, for the transition from metallic to antiferromagnetic insulator (SDW)-state. These observations confirm that the magnetic field does not play an essential role in the occurrence of the heterophase state. Extending this analogy to the superconducting transition, we note an interesting possibility that the transition from the antiferromagnetic insulator to superconductor state might also occur via superconducting transition in inclusions of the minority metallic phase, rather than between the two homogeneous AF and SC states. This suggestion also requires an additional experimental verification.

## VII Acknowledgements

The authors are grateful to V. Kiryukhin, V. Podzorov, S. Brazovski, A. G. Lebed, and V. Yakovenko for discussions. The work was partially supported by INTAS, RFBR, NWO, Russian Federal Programs “Quantum macrophysics”, “Strongly correlated electrons”, ”High temperature superconductivity”, “Integration of high education and academic research”, “The State support of the leading scientific schools”, and COE Research in Grant-in-Aid for Scientific Research, Japan.

Figure captions

Fig. 1. a) The $`PT`$ phase diagram for (TMTSF)2PF6 in the absence of magnetic field. Difference phases are designated as follows: PM - paramagnetic metal, AF - antiferromagnetic insulator, SC - superconductor. Vertical line shows the isobaric trajectory $`P=0.54`$ GPa, which crosses the PM - AF and AF - SC phase borders. The inset shows the temperature dependence of the resistance at $`P=0.54`$ GPa, which corresponds to the vertical trajectory at the main panel. Two bold dots at the $`R(T)`$ curve and at the trajectory mark two corresponding phase transitions, from the metallic PM to the insulating AF state, and from AF to the superconducting SC state. b) Schematic $`PBT`$ phase diagram for the nonsuperconducting phase space ($`T1.14`$ K).

Fig. 2. a) Variation of the resistance with magnetic field in the AF state, which corresponds to the motion along the trajectory 1 in Fig. 1 b. In the inset, on the derivative $`dR/dB`$, one can see the RO oscillations, which are typical for the AF phase. b) Variation of the resistance with magnetic field in the PM state, (trajectory 3 in Fig. 1 b). In high fields, one can see jumps in $`R(B)`$, which are typical for the PM state and correspond to crossing the boundaries between the FISDW phases with different nesting vector. The inset shows the corresponding phase diagram for the FISDW region, experimentally determined in Ref. .

Fig. 3. a) Variation of the resistance with magnetic field for the case of crossing the PM-AF boundary (trajectory 2 in Fig. 1 b). The inset shows $`R(T)`$ changes in the initial state at $`B=0`$, characteristic for the PM metal ($`dR/dT>0`$). The sharp growth of $`R(B)`$ at $`B7`$ T corresponds to the PM $``$ AF transition. b) Magnetic field dependence of the derivative $`dR/dB`$, which corresponds to the $`R(B)`$ curves in Fig. 3 a upon increasing and decreasing field. The vertical arrows show the borders between the FISDW phases, depicted from the experimentally determined phase diagram (see  and the inset to Fig. 2 b). The inset demonstrates the periodicity of the $`dR/dB`$ peaks in $`1/B`$. Sample #1.

Fig. 4. Magnetic field dependence of the derivative $`dR/dB`$ for four temperatures. The curves show rapidly disappearing hysteresis as temperature grows, and a characteristic nonmonotonic temperature dependence of the rapid oscillations. Sample #2.

Fig. 5. History effects developing in $`R(B)`$ (panel a) and in $`dR/dB`$ (panel b) as magnetic field varies along the trajectories AB, BC, CD, and DE. Two arrows mark the peaks in $`dR/dB`$ corresponding to the FISDW transitions in the PM phase; these peaks are missing as field decreases.

Fig. 6. a) History effects in the temperature dependence $`R(T)`$ at zero field when the trajectory crosses the PM-AF phase boundary; b) Re-establishing the homogeneous state by sweeping the magnetic field to 16 T and back to zero. Pressure is $`P=0.5`$ GPa.


text:
# Unusual magnetic field-induced phase transition in the mixed state of superconducting NbSe2

## Abstract

The thermal conductivity $`\kappa `$ in the basal plane of single-crystalline hexagonal NbSe2 has been measured as a function of magnetic field $`H`$, oriented both along and perpendicular to the $`c`$-axis, at several temperatures below $`T_c`$. With the magnetic field in the basal plane and oriented parallel to the heat flux we observed, in fields well below $`H_{c2}`$, an unexpected hysteretic behavior of $`\kappa (H)`$ with all the generic features of a first order phase transition. The transition is not manifest in the $`\kappa (H)`$ curves, if $`H`$ is still in the basal plane but oriented perpendicularly to the heat-flux direction. The origin of the transition is not yet understood.

The layered hexagonal compound NbSe2 has been of interest to researchers for some time, mainly because of the relatively strong anisotropy of its superconducting properties. Pure samples exhibit a superconducting critical temperature $`T_c7.2`$ K, and the upper critical fields for $`H`$ along and perpendicular to the hexagonal $`c`$-axis are $`H_{c2}^c=40`$ kOe and $`H_{c2}^{ab}=140`$ kOe,Woollam76  respectively. The anisotropy of the electron system is also reflected in the charge density wave (CDW) transition at $`T_{\mathrm{CDW}}=34\mathrm{K}`$ (in pure NbSe2), interesting by itself and also in view of the competition between the CDW formation and superconductivity. Sooryakumar80  Another important feature of NbSe2 is the existence of a variety of vortex matter related phenomena, such as a pronounced peak effect and various phase transitions and instabilities (see, e.g., Refs. Banerjee99\_Dis, ; Marchevsky01, ; Paltiel00\_Ins,  and references therein).

In this paper, we present the observation of an unexpected hysteretic behavior of the thermal conductivity in external magnetic fields $`\kappa `$ with the characteristic features of a first order phase transition. Several anomalies associated with the transition are yet to be explained.

The single crystal used in the experiments was grown by employing the iodine vapor transport method as described in Ref. Levy83, . Two bar-shaped samples with dimensions of $`4.4\times 0.88\times 0.42\mathrm{mm}^3`$ and $`2.8\times 0.51\times 0.50\mathrm{mm}^3`$, were cut from the crystal. Very detailed measurements of $`\kappa (T,H)`$ were done on one of the samples and the other specimen was used to ascertain that the observed effects described below are indeed sample-independent. The thermal conductivity was measured by employing the standard uniaxial heat flux method in an experimental setup that was also used in our recent study of $`\kappa (T,H)`$ in MgB2.Sologubenko02\_Tem ; Sologubenko02\_The  The heat flux $`\dot{𝐐}`$ was kept in the basal plane and along the longest lateral dimensions of the sample. The temperature difference $`\mathrm{\Delta }T`$ along the specimen was kept to about 3 - 5 % of the average sample temperature. The zero-field superconducting transition temperature $`T_c=7.2`$ K was determined via four-contact $`dc`$ resistivity measurements and from the results of measurements of the magnetic susceptibility, employing a commercial Quantum Design SQUID magnetometer.

Fig. 1 shows $`\kappa (H)`$ at $`T=0.85`$ K for all three orientations of the magnetic field that we have explored. Similar results were obtained at other temperatures in the interval between 0.38 K and $`T_c`$. The data for $`Hc`$ are in good agreement with the recent results presented by Boaknin et al..Boaknin03  The main features of $`\kappa (T,H)`$ can readily be understood by considering that the total thermal conductivity consists of two components, namely the phonon contribution $`\kappa _{\mathrm{ph}}`$ and the quasiparticle (electron) contribution $`\kappa _e`$. The normal electronic excitations in the cores of the vortices in the mixed state considerably reduce the phonon mean free path, but they also add positively to the heat transport. Hence when the external magnetic field is enhanced to above the lower critical field $`H_{c1}`$, $`\kappa _{\mathrm{ph}}(H)`$ is efficiently reduced but, simultaneously, $`\kappa _e(H)`$ starts to increase. The result is a minimum in the $`\kappa (H)`$ curve in a magnetic field slightly exceeding $`H_{c1}`$. These features may be seen in Figs. 1 and 2(b). In the normal state, above the upper critical field $`H_{c2}`$, the thermal conductivity varies only weakly with $`H`$. It reflects the field induced positive variation of the electrical resistivity of NbSe2 in the normal state, which also affects the electronic contribution $`\kappa _e`$ to $`\kappa `$.

This general behavior of $`\kappa (H)`$ is observed for all orientations of the magnetic field, but, with $`Hc`$ and parallel to the heat-flux direction, a pronounced hysteretic behavior in $`\kappa (H)`$, as shown in Fig 2, is observed. This feature, emphasized in Fig. 2 (a), is a clear manifestation of some kind of phase transition, most likely of first order. As we discuss in detail below, some details are not compatible with a conventional first order transition, however.

Inspecting the data presented in Fig 2, it is clear that two different $`\kappa (H)`$ regimes have to be distinguished. They correspond to two different modifications or phases of the mixed state, one of which is stable in low fields ($`l`$-phase) and the other ($`h`$-phase) corresponds to the equilibrium state in high magnetic fields. In the following we shall use $`\kappa ^{(l)}(H)`$ and $`\kappa ^{(h)}(H)`$ to denote the thermal conductivities of the $`l`$\- and $`h`$-phases of the mixed state, respectively (see Fig. 2(a) for the definitions of $`\kappa ^{(l)}`$, $`\kappa ^{(h)}`$ and the corresponding characteristic fields). While the $`l`$-phase is stable up to $`H=H_2`$, the high-field modification remains stable down to $`H=H_1<H_2`$. Also note that the transition from one modification to the other is rather narrow upon field reduction, whereas the transition in increasing field is more than twice as wide, with $`\kappa (H)`$ being almost constant in the transition region. All the features shown in Fig. 2 were confirmed to be reproducible and they were observed for both investigated samples.

The hysteresis is completely absent if the magnetic field, while still parallel to the basal plane, is rotated to be perpendicular to the heat flux direction (see Fig 2(b)). This disappearance of the hysteresis is quite unexpected because, considering the hexagonal symmetry of the crystal structure of NbSe2, no anisotropy is expected in the basal plane. It may also be seen that $`\kappa (H)`$ is notably higher if the magnetic field is oriented perpendicularly to the heat flux.

Another unusual feature of this transition is the considerable width of the hysteresis loop with $`H_2^{}/H_1^{}1.7`$. It turns out that both $`H_1^{}`$ and $`H_2^{}`$ increase with increasing temperature (see Fig.3 (a)). Considering that all critical fields of a superconductor usually decrease with increasing temperature, this is again an unexpected observation.

The magnetic field ranges $`H_2<H<H_2^{}`$ in increasing and $`H_1^{}<H<H_1`$ in decreasing fields, respectively, correspond to transition regions where the $`l`$\- and the $`h`$-phase coexist. Because both $`\kappa ^{(l)}(H)`$ and $`\kappa ^{(h)}(H)`$ may quite well be approximated by parallel straight lines, the volume ratio between the two phases for each point in the transition regions can easily be evaluated from the experimental data.

Partial hysteresis loops, as shown in Fig. 4, are also unusual. If a reduction of the magnetic field is started from the transition region between $`H_2`$ and $`H_2^{}`$ (Fig. 4 (a)), the measured $`\kappa (H)`$ curve is practically parallel to $`\kappa ^{(l)}(H)`$ and $`\kappa ^{(h)}(H)`$ until $`H_1`$ is reached. Roughly the same feature emerges if the magnetic field is enhanced from the transition region $`H_1>H>H_1^{}`$ (see Fig. 4(b)). These observations imply that in the limited field range between the vertical broken lines in Fig. 4, the volume ratio between the $`l`$\- and the $`h`$-phase in the sample is independent of the applied magnetic field and can only be changed if the magnetic field exceeds $`H_2`$ (in increasing field) or is reduced to below $`H_1`$ (in decreasing field). This behavior is rather difficult to understand in terms of a common first order phase transition. Indeed, in conventional first order transitions, the main reason for a hysteresis is the inertia toward generating a sufficiently large nucleus of a new phase. Once the nucleus exists, the transition usually happens in a rather narrow range of fields or temperatures. Here we have a completely different situation. Two different phases coexist in fixed amounts over an extended field region and it needs to be understood why the transformation from one phase to the other does not happen upon varying the applied magnetic field within the limits mentioned above.

We also tested the stability of $`\kappa `$ at fixed values of the magnetic field in the transition regions and at constant temperature. As may be seen in Fig. 5, there are no observable changes of $`\kappa `$ with time. This observation provides again clear evidence that the transformation of one phase into the other cannot happen as easily as it usually does in the case of common first order phase transitions. In an extended range of the magnetic field both the $`l`$\- and the $`h`$-phase are present and stable in the sample. Taking into account that near the edges of the hysteresis loop only one of them represents the equilibrium, the stability of the described situation implies that some potential barrier seems to prevent the completion of the transition from one equilibrium phase to the other.

Before we discuss the situation further, we note that at temperatures as low as 0.38 K, the phonon contribution $`\kappa _{\mathrm{ph}}`$ to the thermal conductivity in the mixed state is small compared to $`\kappa _e`$, certainly in fields beyond the $`\kappa (H)`$ minima (see Figs. 1 and 2). Because we are mainly interested in low magnetic fields $`H0.1H_{c2}`$, no overlap of vortex cores needs to be considered and each vortex line is expected to contribute to the heat transport individually. If the magnetic field is perpendicular to the heat flux, the vortex motion along the heat flux, induced by a temperature gradient $`T`$, also contributes to $`\kappa `$, but this contribution is not expected to be significant (see Ref. Freimuth03,  and references therein).

The results presented above clearly imply the existence of a phase transition in the mixed state of our NbSe2 samples with the following main features:

(i) A very large difference $`\mathrm{\Delta }\kappa =\kappa ^{(l)}\kappa ^{(h)}`$ between the thermal conductivities in the low and the high field phase. If we assume that $`\mathrm{\Delta }\kappa `$ is only due to a change of the vortex density, we have to assume an unrealistically large variation of the magnetic induction $`\mathrm{\Delta }B3`$ kG (see Fig. 2 (a)).

(ii) A very large width of the hysteresis loop with $`H_2^{}/H_1^{}=1.7`$.

(iii) The coexistence of the $`l`$\- and the $`h`$-phase of the mixed state in an extended range of magnetic fields. The adopted volume ratio is practically independent of $`H`$ in this range (Fig. 3). This particular feature is incompatible with a conventional first order transition.

(iv) A completely different behavior of $`\kappa (H)`$, if the magnetic field is oriented perpendicularly to the heat flux, exhibiting no visible signs of a phase transition (Fig. 2 (b)).

(v) A shift of the transition to higher fields with increasing temperature (Figs. 2 (b) and 3 (a)).

Although the phase transition manifests itself by a rather prominent feature in the $`\kappa (H)`$ curves, we could not find a reasonable scenario which would explain all the different features of the transition. Below we briefly consider several possible phase transitions in the mixed state of type-II superconductors and discuss their relevance for our experimental observations.

1. The well known vortex-lattice melting transition explains neither the magnitude of the observed difference $`\mathrm{\Delta }\kappa =\kappa ^{(l)}\kappa ^{(h)}`$, nor the vanishing of the transition for $`H\dot{𝐐}`$. Quite unlikely are other vortex ordering transitions considered in the literature, because all of them invoke only small changes of the vortex density. We also recall that the vortex lattice melting is a typical first order transition and therefore it is incompatible with the partial hysteresis loops shown in Fig. 4.

2. It was pointed out that in superconductors with other ordering phenomena, a first order phase transition may occur due to the competition between superconductivity and the additional ordering phenomenon. Kurin94  As an example of additional ordering, the authors of Ref. Kurin94,  considered a charge density wave formation. This matches exactly the case for NbSe2 but, because the assumed transition is of first order, it is not clear how the coexistence of two mixed state phases and the dependence of the $`\kappa (H)`$ feature on the orientation of the magnetic field can be explained.

3. The first order transition discussed in Ref. Paltiel00\_Ins,  was observed for $`Hc`$ and therefore seems not to be relevant to our case. The same applies to other reports of instabilities of the mixed state of NbSe2 which were observed either close to $`H_{c2}`$ or for other field orientations.Banerjee99\_Dis ; Marchevsky01

4. The possible phase transition discussed in Ref. Landau02,  is expected to occur in fields rather close to $`H_{c2}`$ and therefore is a priori considered as unlikely to be the reason for our observation.

In conclusion, measurements of the thermal conductivity in external magnetic fields revealed an unusual phase transition in the mixed state of NbSe2. The origin and the nature of this transition is not yet understood and further experiments are needed to clarify the situation.

###### Acknowledgements.

This work was financially supported in part by the Schweizerische Nationalfonds zur Förderung der Wissenschaftlichen Forschung. A.B. acknowledges financial support from the Swiss Federal Commission for Foreign Students.