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# Quasar Absorption Lines as a Function of Quasar Orientation Measures

## 1 Introduction

There is a wealth of classes of extragalactic radio sources. The idea that some or all of these sources come from the same parent population (i.e. the unified model) has been around for quite some time (Rowan-Robinson, 1977; Scheuer & Readhead, 1979). Specifically, it is thought that the classification of an object may have as much to do with our point of view as with the physics of the source. If the parent population is intrinsically non-spherically symmetric, then it is clear how such orientation effects might come about: sources drawn from the same parent population will look different depending on the observer’s vantage point.

For example, it has been suggested that type 1 and type 2 Seyfert galaxies differ only by orientation. The intrinsically non-spherical element in this model is a thick molecular torus that shields our view of Seyfert 2 broad line regions. This model gained widespread acceptance when Antonucci & Miller (1985) discovered hidden broad lines in NGC 1068’s polarized (scattered) light spectrum. Various models using beamed radio jet emission have been proposed to unify flat-spectrum radio quasars and steep-spectrum radio galaxies, but the jury is still out on the exact form this model must take (e.g., Orr & Browne, 1982; Padovani & Urry, 1992). For the purposes of this paper, it suffices that the average flat-spectrum quasar is probably viewed closer to the jet axis than the average steep-spectrum quasar, though such claims cannot be made for comparisons of individual objects.

The purpose of this paper is twofold. In the first part of the paper, we present new 3.5 and 20 cm VLA data (in the A configuration) taken for 120 of the sources from Richards et al. (1999, hereafter Paper I) and 24 sources from Richards (2000, hereafter Paper II). Using these new radio maps, we derive the core and the total spectral indices between 3.5 and 20 cm ($`\alpha _{3.5}^{20}`$), the core-to-lobe ratio (C)111The core-to-lobe ratio is denoted as $`C`$ rather than $`R`$ to avoid confusion with the use of $`R`$ as the radio-loudness parameter, and the ratio of the radio luminosity (at 20 cm) to the optical luminosity ($`R_V`$). Each of these parameters has been used as an indicator of the line-of-sight orientation of quasars. We discuss the utility of these parameters as such, with emphasis on testing the hypothesis that radio spectral indices correlate with the line-of-sight orientation of quasars.

The second part of the paper addresses the results of Paper I, where we found that the distribution of C IV absorption lines along the line of sight to QSOs may be a function of various QSO properties. This absorption line analysis in Paper I suffered from a number of inadequacies resulting from inhomogeneous radio data. The 6 and 20 cm radio data all were taken at different epochs and may be affected by variability. In addition, these data were taken from catalogs of data from both the Green Bank 6 and $`20\mathrm{cm}`$ surveys (Becker et al., 1991; White & Becker, 1992, respectively) and were mixed with $`20\mathrm{cm}`$ data from the NRAO VLA Sky Survey (NVSS; Condon et al. 1998). Furthermore, the flux density limit of the Green Bank surveys is such that only relatively bright radio sources have measured spectral indices. As a result, we felt it was necessary to reobserve some of the objects from Paper I at lower flux density limits, at higher spatial resolution, with a longer baseline, and simultaneously in two bands.

Utilizing this new radio data, we can confirm an apparent excess of narrow, apparently high-velocity C IV absorbers seen in flat-spectrum quasars as compared to steep-spectrum quasars. This result is surprising in that the vast majority of these absorption lines are thought to be caused by galaxies between the observer and the QSO: intrinsic QSO properties should not affect their distribution. Though we presume that the radio properties discussed herein are good indicators of quasar orientations, the results presented here do not depend on this assumption. It suffices that these radio properties are indicators of intrinsic differences in the quasars.

This paper is divided as follows. §2 describes the targets, the radio data and the reduction of said radio data. Quasar orientation measures are discussed in §3. §4 gives a discussion of both high-velocity and low-velocity C IV absorption lines systems as a function of the properties discussed in §3. Finally, §5 presents our conclusions.

## 2 The Data

The objects chosen for observations with the VLA in the A configuration were selected from the revised catalog of absorption line QSOs (York et al., 1991; Vanden Berk et al., 2000) as follows. First, we required that each object be detected by the low resolution Green Bank or NVSS Surveys, which had $`20\mathrm{cm}`$ flux density limits of $`19\mathrm{mJy}`$ and $`2.5\mathrm{mJy}`$, respectively. Since the primary goal of this work is to study the distribution of C IV absorbers in radio-detected quasars, we only observed objects with redshifts larger than $`1.5`$, so that C IV emission is observable in ground-based spectra. In addition, sources with declination less than -27.5 degrees declination were rejected. Though the VLA can observe further south than this limit, we chose not to observe such quasars so that followup spectroscopy could be conducted from the Northern Hemisphere.

Data were taken on 31 July and 9 August 1999, with the VLA222The VLA and NRAO are operated by Associated Universities, Inc., under cooperative agreement with the National Science Foundation. in the A-configuration. Snapshot observations (45 sec – 7.5 min, depending on expected source brightness) were performed sequentially on each target at both 1.4 and 8.4 GHz (20 and 3.5 cm). Absolute flux calibration was established with short observations of 3C286 and 3C147, respectively, on the two dates of observation. Phase calibrators were also observed periodically throughout both runs.

Data were reduced in the standard iterative manner using the 15APR98 version of the AIPS software package. The data were initially mapped, cleaned and self-calibrated using the task MAPIT; as warranted by these initial maps, some sources were further processed using the tasks IMAGR and CALIB. Clipping of especially bad data points was done as necessary on a source-by-source basis. Final source positions and peak fluxes were determined using the task JMFIT, whereas total flux densities were determined using the task TVSTAT to encircle all components associated with each radio source.

In Paper I there were 296 QSOs with measured radio spectral indices. Of these, 174 meet the redshift and declination limit for our present study. We observed 144 quasars during the course of this work, of which 120 were drawn from the sample of 174. The remaining 24 objects were drawn from Paper II. For 99 of these quasars, we obtained good 3.5 and 20 cm detections and were able to match the position of the radio core to the optical position such that we were able to determine the core spectral index. An additional 20 objects had good 20 cm detections (that coincided with the optical position) but no 3.5 cm detections. For those cases where we could not clearly identify the radio core, we still determined the total flux densities and total spectral indices.

The flux density limits of the original Green Bank data are such that only relatively bright radio sources have accurately measured radio spectral indices. The lack of fainter radio sources in our sample may constitute a bias in the data from Paper I. As such, we were careful in our new observations to include objects that are as faint as the flux density limit of the NVSS. The inclusion of fainter radio sources thus enables us to increase the number of quasars with accurate spectral indices, while helping to remove any bias incurred by the study of only the brightest sources. The total number of faint sources is still a significant minority; however, it is hoped that the inclusion of fainter objects will reduce any luminosity bias in the data.

These new data represent an additional significant improvement on that of Paper I in that we now have simultaneous data in two bands (eliminating the effects of source variability). In addition, these radio maps are of higher spatial resolution than the previous radio data. Since core spectral indices may be correlated with quasar orientation better than total (core+extended) spectral indices, it is hoped that these new radio data will solidify our absorption line analysis.

In Table 1 we present the observed properties of the quasars studied in this work. Given are 1) the name, 2) the right ascension in J2000 coordinates, 3) the declination, 4) the emission redshift, 5) an optical magnitude (often, but not always $`V`$), 6) the 6 cm Green Bank flux density (mJy) at low resolution, 7) the 20 cm Green Bank flux density (mJy) at low resolution. Also given are flux densities from the VLA in the A configuration including: 8) the peak 3.5 cm flux density, 9) the total 3.5 cm flux density, 10) the peak 20 cm flux density, and 11) the total 20 cm flux density. In addition to these quantities, we also determined an RMS error for each map and the uncertainty in the peak flux density measurements. Total errors on the peak flux density were determined by taking the sum in quadrature of the RMS noise in the map, the error in the fit as determined by JMFIT and 5% of the peak flux density. For the majority of the sources, this error will be dominated by last of these terms. The resolution of the VLA A configuration data is approximately $`0.7\mathrm{}`$ for the 20 cm (L band) measurements and $`0.1\mathrm{}`$ for the 3.5 cm (X band) measurements.

Table 2 gives parameters derived from those in Table 1. The columns are as follows: 1) the name, 2) the low resolution spectral index between 6 and 20 cm ($`\alpha _6^{20}`$)333Spectral indices are defined throughout according to $`f_\nu \nu ^\alpha `$, such that steep-spectrum sources have more negative spectral indices. as determined from columns 6 and 7 in Table 1, 3) the core spectral index between 3.5 and 20 cm ($`\alpha _{3.5}^{20}`$) using the values in columns 8 and 10 in Table 1, 4) the error in $`\alpha _{3.5}^{20}`$ (core), 5) the total ($`\alpha _{3.5}^{20}`$) spectral index as found from columns 9 and 11 in Table 1, 6) the ratio of the core radio luminosity to the optical luminosity ($`R_V`$), which is given by

$$R_V=\mathrm{log}(f_{20})(1.0+\alpha )\mathrm{log}(1.0+z)26.0+0.4(V+48.6),$$
(1)
where we have assumed an optical spectral index of $`1`$ and have not converted the 20 cm flux density to the more commonly used 6 cm flux density, 7) the core-to-lobe ratio at 20 cm (which we will label as “$`C_{20}`$”), given by

$$C_{20}=\left(f_{20hi}\left(1+z_{em}\right)^{\left(\alpha _{core}1\right)}\right)/\left(f_{20lo}f_{20hi}\right),$$
(2)
where we have taken the spectral index of the extended emission to be $`1`$, 8) the core 20 cm luminosity ($`\mathrm{ergs}\mathrm{s}^1\mathrm{Hz}^1`$), 9) the total 20 cm luminosity ($`\mathrm{ergs}\mathrm{s}^1\mathrm{Hz}^1`$), and 10) the absolute optical magnitude. For those quantities that are dependent upon cosmology, we have used $`q_\mathrm{o}=0.5`$ and $`H_\mathrm{o}=65\mathrm{km}\mathrm{s}^1\mathrm{Mpc}^1`$.

## 3 Quasar Orientation Measures

A number of parameters are currently being used as orientation indicators for radio-detected quasars and galaxies. The accuracy of a given parameter is typically evaluated by comparing to another such parameter — a process that is unappealing in its circularity. Barring more direct data that could only come from in situ inspection, it may not be possible to do much better. Fortunately, the purpose for which we need these orientation measures (comparing the absorption line velocity distribution between quasars with different intrinsic properties) does not depend on their being good orientation measures per se, but rather that they are correlated with apparent intrinsic differences projected along our line of sight.

Orientation measures include radio spectral indices (both core and total), core-to-lobe ratios, core-to-optical luminosity ratios, bend angles, core-hot spot distance ratios, etc. In this analysis, we will compare and contrast the use of core and total radio spectral indices along with $`R_V`$ and $`C_{20}`$ (the core-to-lobe ratio at 20 cm) as orientation indicators. The basis set for this study is the 144 $`z>1.5`$ quasars with known absorption line properties for which we now have 3.5 and 20 cm maps from the VLA in the A configuration.

One of the primary concerns that we had with our analysis in Paper I was the use of radio data taken at different epochs, meaning our analysis could have been influenced by variability in our data. Without simultaneous measurements, we were forced to assume that our data, on average, were unaffected by variability. With our new simultaneous 3.5 and 20 cm maps, we can now address this problem. Figure 1 shows the fractional difference between the total 20 cm flux density as measured by Green Bank or NVSS (the measurement used in Paper I) and our high resolution VLA maps. This difference is plotted against the log of the total 20 cm flux density from our new measurements. Large differences are indicative of either variability or resolution effects; large positive values on the y-axis indicate excess flux in the lower resolution data. The fact that most of our sources have differences less than about 20% means that variability should not strongly influence our results. However, it is clear that some sources have varied by 50% or more. The fact that the measurements were taken at different resolutions may contribute to these differences.

Since the A configuration data were taken simultaneously, we assume that the total spectral indices calculated from the VLA data are “correct”. Variability will then either conspire to yield incorrect spectral indices in the low resolution data (taken at different epochs), or will have no apparent effect if the low resolution observations happen to give the “correct” (or nearly correct) spectral index. Since flat-spectrum sources are more likely to be variable than steep-spectrum sources, we would expect that objects with flat core spectra (measured simultaneously at two frequencies) would exhibit indices that depart significantly from $`\alpha 0`$ when computed from non-simultaneous radio data. However, from Figure 2 it appears that this effect is not dramatic. Only 18 of the 45 objects with flat ($`0.4<\alpha <0.4`$)444The typical dividing line between steep- and flat-spectrum sources is $`\alpha =0.5`$. Here we use $`\alpha =0.4`$, since that is the median of our core spectral index sample. simultaneously-measured core spectral indices, have non-simultaneous (total flux) spectral indices that fall outside this range.

In Figure 2 (and similar graphs), open squares are those objects with 20 cm core-to-lobe ratios ($`C_{20}`$) less than unity. Filled squares are objects with core-to-lobe ratios greater than unity, whereas stars are those objects for which the core-to-lobe ratio is suspect or otherwise not available. Spectral indices were calculated according to $`f_\nu \nu ^\alpha `$ such that steep-spectrum sources have more negative spectral indices. Though it is possible that variability is the cause of the “outliers” described in the paragraph above, it must also be kept in mind that some of the “variability” observed in the data is likely a result of the different resolutions used to measure the core and total spectral indices. Note, in particular, that the objects with inverted core spectral indices and steep total spectral indices in the upper left hand side of Figure 2 are all lobe dominated, which is indicative of a resolution effect as opposed to a variability effect. Therefore, it seems likely that true radio variability is not a significant source of error in our previously published low resolution spectral data.

It is also important to realize that variability affects higher frequency data more than low frequency data, since the higher frequency observations are more sensitive to flat-spectrum sources, which are more likely to be variable. A comparison of flux densities of 20 cm data from different epochs should reveal less variability than a similar comparison at 6 cm. Therefore, the variability in Figure 1 is only a lower limit to the variability in the spectral indices.

Having addressed the effect that variability has on the measurement of radio spectral indices, we now turn to an analysis of their use as quasar orientation measures. Our new data allows the computation of spectral indices between 3.5 and 20 cm (at high resolution), whereas we used the 6 and 20 cm flux densities (at low resolution) in our previous analysis (Paper I). As such, it is worth making a comparison of the total (core+extended) spectral indices as determined from each data set; Figure 3 depicts this comparison. The spectral indices from the old and new data are roughly correlated; however, the slope of the correlation is not unity and the majority of the points are steeper in the high resolution data.

Nominally, one might expect that the core-dominated sources will have flat spectral indices independent of resolution. Similarly, the spectral indices of lobe-dominated sources would be steep both at low and high resolution, although less so in the A-configuration data because over-resolution would cause one to miss a significant fraction of the extended steep spectrum emission, thus flattening the overall spectrum. These naively expected trends are evident in the data, though there are exceptions. About a dozen of the core-dominated sources exhibit steep radio spectra (as measured by either index). These sources constitute a larger than expected fraction of core-dominated steep spectrum sources ($``$ 40% of the core-dominated sources in Figures 2 and 3 are steep-spectrum). Some of these sources may be Compact Steep Spectrum objects (CSS; O’Dea, 1998), although our division of core- vs. lobe-dominated (C20 less than or greater than unity) is not the same as is used to define CSS sources.

In addition to variability, we were also concerned that the resolution of our old (Paper I) radio data might bias our results. Since we chose to make our new radio maps at higher resolution (using the A configuration of the VLA), it is interesting to ask how much influence resolution has on spectral indices, especially how resolution affects the degree to which spectral indices correlate with the orientation angle of AGN. Figure 2 shows how the core spectral index (between the 3.5 and 20 cm) correlates with the total spectral index (between the 6 and 20 cm). There is a correlation, though it is not as strong as in Figure 3. Of particular interest are the lobe-dominated sources with flat cores located in the middle of the left hand side of the plot. If spectral indices are indeed a measure of the orientation of quasars, then it is clear that one or both are failing for these objects. For the most inverted-spectrum sources (both spectral indices greater than $`0.4`$) both the core and total spectral indices agree much better.

Though radio spectral indices may be good orientation indicators, Wills & Brotherton (1995) claim that the ratio of core radio luminosity to optical luminosity ($`R_V`$) may be a better indicator of quasar orientation, particularly as compared to the ratio of core radio luminosity to extended radio luminosity ($`C`$, the core-to-lobe ratio). Their argument is that the extended radio flux is sensitively dependent upon interactions with the quasar environment, whereas the optical luminosity is correlated with the power available to the lobes and is not affected by the quasar environment. In Figure 4 we compare the total (low resolution) spectral index to this parameter ($`R_V`$). There is a reasonable correlation between the two parameters if one ignores the lobe-dominated steep (total) spectrum sources that have anomalously low values of $`R_V`$. These are the same outliers as in Figure 2. If both parameters are orientation measures, then one is clearly failing on these sources. Given that these objects have lobe-dominated morphologies and have total spectral indices that are consistent with this observation, it would seem that $`R_V`$ is the parameter in “error”.

For comparison, we also plot $`R_V`$ versus the core spectral index in Figure 5. Both of these parameters are ratios that contain the core 20 cm flux, so the correlation between the two is somewhat artificial. Nevertheless, we can see that objects with flat cores tend to have small values of $`R_V`$, whereas objects with steep cores tend to have larger values of $`R_V`$.

As a final test, we compare the total (low resolution) spectral indices against the core-to-lobe ratio (at 20 cm). Figure 6 gives the log of the core-to-lobe ratio versus the total (low resolution) spectral index. Open circles are those objects whose 20 cm maps are resolved into two or more sources. Closed circles are apparently unresolved point sources. Stars are objects that were difficult to classify as one or the other. There is a general (but not perfect) trend towards flatter spectral indices with more core-dominated sources. The most lobe-dominated sources ($`C_{20}<0.1`$) are steep-spectrum sources ($`\alpha <0.4`$), as expected.

One caveat with respect to Figure 6 is that the core-to-lobe ratio is best used as an indicator of relative orientation only among classes of objects that are believed to be intrinsically the same. Because this sample was chosen based on the presence of optical absorption properties, there is little reason to believe the radio engines are intrinsically the same in these objects. Specifically, the bulk jet Lorentz factors may vary significantly from object to object. This fact will adversely affect the core-to-lobe ratio as an orientation indicator since it implies two objects that are intrinsically the same in every respect except in jet speed, seen at identical lines of sight, will have significantly different core-to-lobe ratios. Finally, the fact that different classes of radio sources have different intrinsic amounts of core relative to lobe emission, may introduce a scatter into Figure 6. Core-to-lobe ratios are therefore best used as orientation measures when there is some reason to believe the radio sources in question are intrinsically the same and only appear different because of orientation. Again, this is not necessarily the case for this sample of quasars, selected by virtue of the presence of optical C IV absorption.

From an analysis of our new radio data in comparison to the radio data used in Paper I, we have addressed the usefulness of various radio properties as quasar orientation measures. Given the rough correlation between each of these properties, it is likely that all trace the orientation of quasars to some degree. However, it is clear that the correlation between these parameters is far from perfect and that these “orientation indicators” should be treated with a healthy amount of caution.

The primary purpose of using multiple orientation indicators in this study was to test the validity of the total flux radio spectral indices as an orientation indicator in Papers I and II. That the total flux radio spectral index is roughly correlated with the other properties presented herein is taken as justification for the use of this parameter. Even if the radio spectral indices are not the best measure of orientation per se, there is no doubt that they are probes of properties that are intrinsic to the quasars and therefore should not correlate in any way with any property not intrinsic to the quasar, such as intervening absorption systems. We now turn our analysis to this issue.

## 4 Absorption Line Analysis and Discussion

The purpose of obtaining this new radio data was to determine if our inhomogeneous radio data were biasing the results of our analysis from Paper I. At least three issues are involved here. First, the spectral indices in Paper I were determined from maps made at different epochs. Second, the old radio data are low resolution. Finally, only the brightest sources had spectral index measurements. With the new radio data presented above, we have alleviated each of these problems and we can now proceed with a re-analysis of the absorption line properties of quasars as a function of quasar orientation measures.

The new data seem to indicate that, but for a small number of sources, the total spectral indices are reasonably correlated with other intrinsic quasar properties that have traditionally been used as orientation measures. In particular, the total spectral indices taken nearly simultaneously and at high resolution agree well with the total spectral indices taken at different epochs and at low resolution. This being the case, we could stop here and claim that our results support the conclusions drawn in Paper I. However, it is worth discussing this and related issues in further detail.

The absorption line data is studied as a function of the intrinsic radio properties of six subsamples of data. The results from this analysis are presented in Figure 7 and Table 3. The samples are defined so as to allow for the splitting of the samples into two based on the orientation indicator that defines the sample. Sample A includes the C IV absorbers in quasars where the radio spectral index has been measured at low resolution between 6 and 20 cm. Sample B is a subset of sample A and includes only those quasars for which we have both low resolution spectral indices between 6 and 20 cm and also high resolution, core spectral indices between 3.5 and 20 cm. Sample C includes only those quasars for which we were able to measure high resolution, core spectral indices between 3.5 and 20 cm. Sample D combined both samples B and C by requiring not only that both high and low resolution spectral indices are measured, but also that both spectral indices are both either steep or flat. Sample E includes those objects for which we measured $`R_V`$, whereas Sample F includes the quasars that have measured values of $`C_{20}`$. The columns in Table 3 are as follows. Column 1 gives the sample and the orientation indicator (e.g. steep or flat spectrum). Columns 2-4 give values for absorbers with velocities within $`\pm 5000\mathrm{km}\mathrm{s}^1`$ of the quasar redshift, including 1) $`dN/d\beta `$, 2) the error in $`dN/d\beta `$, and 3) the number of absorbers. Columns 5-8 give values for absorbers with velocities larger than $`5000\mathrm{km}\mathrm{s}^1`$, but less than $`55,000\mathrm{km}\mathrm{s}^1`$, including 5) $`dN/d\beta `$, 6) the error in $`dN/d\beta `$, 7) the observed number of absorbers, and 8) the expected number of absorbers based on the average of the number of quasars studied.

### 4.1 Narrow, High-Velocity C IV Absorption

In Paper I we showed that there is a excess of high-velocity C IV absorbers in flat-spectrum quasars as compared to steep-spectrum quasars. We also showed that this effect is not apparently the result of some other bias in the steep-spectrum quasar sample (i.e. because they tend to be fainter or at lower redshift). In Figure 7 we show the apparent velocity distribution of C IV absorbers for a number of samples of QSOs with different observed radio properties. Here we assume that the redshifts of the absorbers are due to outflows from QSOs and are non-cosmological (we certainly do not propose that all C IV absorption is non-cosmological; however, in making this plot that is a fundamental assumption).

For sample A, we plot the number density of absorbers per unit velocity versus velocity for both steep- and flat-spectrum quasars. The spectral indices are the same as those used in Paper I, specifically the ratio of the 6 and 20 cm flux densities from Green Bank (or NVSS). A spectral index of -0.4 ($`f_\nu \nu ^\alpha `$), which is the median of this sample (as compared to -0.5, used in Paper I), serves as the dividing line between flat- and steep-spectrum sources. For sample A, the closed squares are the steep-spectrum data points, whereas the open squares are the flat-spectrum data points. On the far left of Figure 7, we include only those absorbers within $`\pm 5000\mathrm{km}\mathrm{s}^1`$ of the QSO redshift (sample A only); these are the so-called “associated” absorption systems (e.g., Foltz et al., 1986). For the remainder of the samples only higher velocity data points are given, where the low velocity edge of the bin is at $`5000\mathrm{km}\mathrm{s}^1`$, and the red edge is at $`55,000\mathrm{km}\mathrm{s}^1`$. This range is set so as to maximize the number of absorbers in the bin, but to avoid lines that are either too close to the QSO redshift or that are too close to the Lyman-$`\alpha `$ emission line. Except for the binning of the high velocity data (which is necessary for comparison for the samples that follow, since they have fewer absorption line systems), sample A represents a compression of the data in the top panel of Figure 4 in Paper I.

As was observed in Paper I there is an excess of high velocity C IV absorption between $`5000`$ and $`55,000\mathrm{km}\mathrm{s}^1`$ in flat-spectrum quasars as compared to steep-spectrum quasars. While the significance of this excess is not large and the numbers are small, the potential consequences for quasar absorption line studies justifies further analysis in attempt to confirm or reject this result. In addition to the tests presented herein and in Papers I and II, it would be extremely useful to conduct a similar study that focuses on bright steep-spectrum quasars since they tend to be fainter than flat-spectrum quasars (Orr & Browne, 1982), even though such a bias was ruled out in Paper I.

The first test we conduct using our new radio data is to ask if this result could be biased by variability of the radio measurements. Using only those quasars from sample A for which we have core spectral indices from our VLA A configuration data at 3.5 and 20 cm, we repeat the above experiment. This comparison is necessary to test that our selection of objects for followup radio observations is not biased with respect to the initial sample. Thus, in sample B (a subset of sample A) we show the difference in the number density of C IV absorbers between steep- (closed square) and flat-spectrum (open square) quasars, again using the low resolution spectral indices. That the steep/flat dichotomy is as strong or stronger in sample B as in sample A supports the notion that this dichotomy is neither due to variability or to a selection bias in the radio data.

Though there may be resolution and bandpass issues (our new high frequency datapoint is at 3.5 cm, instead of 6 cm) between the high resolution total spectral index and total spectral index measured at lower resolution, the new spectral indices are unaffected by source variability and were shown to correlate very well with the indices derived from the low resolution data (Figure 3). Thus, it would seem then that our initial result from Paper I is probably not the result of variability in the original radio data.

Since the results from both total spectral index measurements (non-simultaneous low resolution and simultaneous high resolution) agree well, we next look at the distribution of absorbers with respect to the core spectral index. If the core spectral index is a better orientation indicator than the total spectral index and if there is an orientation dependent population of absorbers, then we expect that this experiment will yield a more dramatic steep/flat dichotomy. Doing this experiment, we find that there is a difference in the velocity distribution of C IV absorbers between flat- and steep-spectrum sources when using core spectral indices; however, the difference is weaker than expected from our hypothesis. That this is the case can be seen in sample C of Figure 7.

One possible explanation for the observation that core spectral indices produce less of a dichotomy than total spectral indices is if there is a population of high-velocity intrinsic C IV absorbers, it could be located on scales much larger than the core radio flux. For the 20 cm data, this means that the absorbing material would have to be $`2\mathrm{kpc}`$ or more from the central engine of the quasar, where

$$d=\frac{2c}{H_\mathrm{o}}\frac{\left[(1+z)(1+z)^{1/2}\right]}{(1+z)^2}\theta ,$$
(3)
taking $`q_\mathrm{o}=0.5`$, $`H_\mathrm{o}=65\mathrm{km}/\mathrm{s}/\mathrm{Mpc}`$, $`z_{em}=2.5`$, and $`\theta =0.7\mathrm{}`$. If there are indeed narrow, ejected absorbers, such a distance may not be surprising. A velocity of $`1000\mathrm{km}\mathrm{s}^1`$ corresponds to $`10^3\mathrm{pc}\mathrm{yr}^1`$, such that material might be found out to a distance of $`100\mathrm{kpc}`$ during the expected lifetime of a quasar ($`10^8\mathrm{yrs}`$). Alternatively, it could be that for the sample of quasars studied here (selected originally by the presence of C IV absorption systems), core radio spectral indices are not as accurate a measure of either intrinsic or orientation-dependent differences as the spectral indices measured using the total flux.

One way to test these conclusions further is to require that both the low and high-resolution spectral indices be steep or flat (i.e. combine samples B and C). Cutting the data in this way has two effects. First, we are still using the low resolution spectral indices as an orientation indicator. Second, we remove any objects that might be affected by variability by requiring that the high resolution spectral index (which is derived from simultaneous data) be the “same” (either steep or flat spectra) as the low resolution spectral index. Sample D in Figure 7 shows the results of such an analysis. Even though the observed number of absorbers is quite small in this subsample, it is again clear that there are more absorbers in flat-spectrum quasars and fewer absorbers in steep-spectrum quasars as compared to each other (and to the expected, average, distribution).

A few comments regarding the distribution of C IV absorbers as a function of other orientation indicators ($`R_V,C_{20}`$) are necessary. Looking at Figure 4, we note that to divide the sample into two by the median of $`\alpha _6^{20}`$ produces completely different data sets than if the sample is divided by the median of $`R_V`$. It is worth asking if the C IV absorption dichotomy remains if the sample is delineated by “$`R_V`$”. In fact, it does not. High-$`R_V`$ and low-$`R_V`$ QSOs have nearly the same velocity distribution of C IV absorbers (see Sample E in Figure 7). Since $`R_V`$ is thought to be one of the better orientation measures, our hypothesis that there is a population of intrinsic C IV absorption line systems that are a function of QSO orientation seems to be in jeopardy. However, we reiterate our doubt that $`R_V`$ is a good orientation measure for our particular sample, since the $`R_V`$ values for lobe-dominated, steep-spectrum sources are clearly out of line with the expected values.

There is a similar effect with the core-to-lobe ratios, $`C_{20}`$. From Figure 6 we see that whereas lobe-dominated quasars ($`C_{20}1`$) are predominantly steep-spectrum sources, and core-dominated quasars ($`C_{20}>1`$) are typically flat-spectrum sources, there are exceptions. As with $`R_V`$, a division of the sample into two parts using $`C_{20}=1`$ as the dividing line yields little or no difference in the C IV absorber distribution between the two subsamples of sample F in Figure 7. This effect would also seem to rule against the conclusion that many high velocity C IV absorbers are actually intrinsic to the quasars. However, the range of spectral indices for core-dominated objects is large. There is a handful of core-dominated steep-spectrum sources and also a number of objects that are multiple or resolved to the eye, but have core-to-lobe ratios that suggest that they are core-dominated. Furthermore, both lobe- and core-dominated steep-spectrum sources show a dearth of absorbers. These issues need to be resolved in order for an analysis of the distribution of C IV absorbers as a function of core-to-lobe ratio to be meaningful.

While some measures of properties intrinsic to quasars (e.g., $`C_{20}`$ and $`R_V`$) do not show a statistically significant difference in the frequency of high velocity C IV absorbers, other indicators (e.g., various estimates of the radio spectral index) clearly show a statistical difference between flat- and steep-spectrum objects. This could be interpreted several ways. First, detection of high velocity C IV absorbers could correlate with quasar orientation (and therefore be intrinsic to the quasars themselves) and two common indicators of quasar orientation ($`R_V`$ and $`C_{20}`$) are simply not good orientation measures for this particular quasar sample for any number of reasons. Alternatively, it could be that the presence of high velocity C IV absorbers is not related to quasar orientation in any simple way, but is related to at least one intrinsic quasar property: the total (core+extended) radio spectral index. Either way, our main conclusion from Paper I is confirmed here: the frequency of narrow, high-velocity C IV absorption systems cannot all be due to intervening systems. At least some fraction of these systems must be intrinsic to the quasars themselves.

### 4.2 “Associated” Absorption

In the left panel of Figure 7, sample A represents those absorption lines that have redshifts within $`5000\mathrm{km}\mathrm{s}^1`$ of the QSO emission redshift. These absorption lines are the so-called “associated” absorption systems (Foltz et al., 1986). Clearly, there is little doubt that these systems are drawn from a population that is different from the systems observed at larger relative velocities. We confirm that these systems are atypically strong and tend towards steep-spectrum quasars. We also emphasize (as we did in Paper I) that the excess of low velocity absorbers in steep-spectrum quasars is made more evident by the dearth of high-velocity absorbers in the same. On the other hand, the flat-spectrum level appears to be more consistent as a function of velocity (c.f. Figure 7).

Given that the so-called associated absorption systems tend to be “associated” with steep-spectrum quasars, it might be interesting to look at the other orientation measures for QSOs with associated absorption. We find that the average $`\alpha _6^{20}`$ (total, low resolution) for QSOs from Paper I with C IV absorption within $`3000\mathrm{km}\mathrm{s}^1`$ of the emission redshift is $`0.76`$. Unfortunately, our new sample only included a half-dozen or so of these quasars, so it is difficult to do a complete analysis of the other orientation measures; however, we can calculate the mean values. We find that the average associated absorption quasar has $`\alpha _{3.5}^{20}`$ (core, high resolution) $`=0.49`$, $`\alpha _{3.5}^{20}`$ (total, high resolution) $`=1.07`$, $`R_V=2.55`$, $`\alpha _6^{20}`$ (total, low resolution) $`=0.82`$, while the $`C_{20}`$ values are intermediate. Curiously, both of the “total” spectral indices (high and low resolution) are very steep, whereas the core, high resolution spectral index is near the dividing line. $`R_V`$ and $`C_{20}`$ are also right near the dividing line.

It is interesting that the associated systems are found so predominantly in steep-spectrum sources, yet their other orientation measures are more intermediate. This situation is similar to what we observe for the narrow, high-velocity absorbers: the excess of absorbers only occurs for comparisons of total spectral indices, but not other orientation measures. That this behavior occurs in a sample of systems that are accepted as being associated and not intervening lends credence to the possibility that there may be a population of narrow, high-velocity C IV absorbers that are related to the QSO and are distributed as a function of the total radio spectral index. Further work is clearly needed to fully understand the associated absorbers; however, a detailed analysis is beyond the scope of this work.

### 4.3 Orientation versus Intrinsic Indicators

Throughout this work we refer to a number of radio properties of quasars as “orientation indicators”. The reader may agree or disagree that these measurements do indeed correlate with the line-of-sight orientation of quasars in a statistical sample. However, it is important to stress that it is not very important to this work that these parameters be good orientation indicators. All that is required is that they are good indicators of something intrinsic to the quasar itself. That is, the radio properties are all intrinsic to the quasars even if they are not good orientation measures; the fact that these properties are intrinsic and not that they are orientation indicators are what make them ideal for studying intrinsic absorption in quasars. For example, the excess of C IV absorbers at low velocities in steep-spectrum quasars is an empirical fact. Whether or not the spectral indices are also a good orientation indicator is not entirely relevant; the total radio spectral index need not delineate the location of the jet or the axis of the disk so long as it tells us something about the physical location and distribution of the hypothesized absorbing material. However, it is true that in terms of producing a model that explains such effects, it would be surprising if the spectral index was not a good orientation indicator. As such, our discussion leans towards the assumption that these intrinsic radio properties of quasars are indicators of the orientation of the quasars.

In terms of intrinsic absorption, whether or not the spectral indices are also orientation indicators depends significantly on the location of the absorbing material with respect to the material that is producing the radio emission. Since quasars are observed to have extended radio emission, it is possible that the absorbing material could be located anywhere from about 1 pc (the scale of the accretion disk) to hundreds of kiloparsecs (the scale of a large radio lobe). If intrinsic absorbers, whether they be the accepted type, such as the “associated” absorbers, or the high-velocity type postulated herein, are formed far from the central engine of the quasar, such as at the boundary where the radio lobes interact with the IGM, then it would not be surprising to find that there is a correlation between intrinsic absorption properties and total spectral index, but not quasar orientation. This is because the spectral index will have been profoundly influenced by the IGM material (which is why Wills & Brotherton (1995) proposed using $`R_V`$ as an orientation measure in the first place), and also because precession of the central source during the lifetime of the lobes may produce a significant offset. As such, we too caution against the blind used of radio properties as orientation measures, but we stress that their use as such is not explicitly required for our analysis.

## 5 Conclusions

We have presented new radio measurements at both 3.5 and 20 cm using the VLA in the A configuration for 144 quasars with known C IV absorption line properties. These measurements are used to determine radio properties that are often used as quasar orientation measures, particularly the total radio spectral index as determined from non-simultaneous data in two bandpasses.

Our results can be summarized as follows:

1) Total, low-resolution spectral indices (between 6 and 20 cm) computed from data taken at different epochs are not significantly corrupted by variability. Furthermore, they are reasonably well correlated with total spectral indices computed between 3.5 and 20 cm that were taken simultaneously at much higher resolution.

2) $`R_V`$ is correlated with $`\alpha _6^{20}`$ (total, low resolution), except for some lobe-dominated sources, which appear to have “incorrect” values of $`R_V`$.

3) We confirm the excess of narrow, high-velocity C IV absorbers found in flat-spectrum quasars as compared to steep-spectrum quasars that was reported by Richards et al. (1999). This excess is not caused by variability or a radio luminosity bias.

4) The steep/flat dichotomy is less pronounced for core spectral indices. If there is indeed a population of narrow, high-velocity intrinsic absorbers, this fact may indicate that the location of these systems is beyond the extent of the resolution of the VLA in the A configuration ($`2\mathrm{kpc}`$).

5) Other orientation measures do not show the same dichotomy. However, there is reason to believe that these measures are flawed as good orientation indicators for our particular sample. Furthermore, the dichotomy need not be strictly an orientation effect, but rather an intrinsic effect.

6) Associated absorption systems are preferentially found in quasars with total spectral indices that are very steep. However, the mean values of other orientation measures are more moderate.

RHB and SLM acknowledge support from the NSF (grants AST-98-02791 and AST-98-02732) and the Institute of Geophysics and Planetary Physics (operated under the auspices of the U.S. Department of Energy by the University of California Lawrence Livermore National Laboratory under contract No. W-7405-Eng-48). We thank an anonymous referee for suggestions that improved the paper.


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# Electron and Nuclear Spin Dynamics in Antiferromagnetic Molecular Rings

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## Abstract

We study theoretically the spin dynamics of antiferromagnetic molecular rings, such as the ferric wheel Fe10. For a single nuclear or impurity spin coupled to one of the electron spins of the ring, we calculate nuclear and electronic spin correlation functions and show that nuclear magnetic resonance (NMR) and electron spin resonance (ESR) techniques can be used to detect coherent tunneling of the Néel vector in these rings. The location of the NMR/ESR resonances gives the tunnel splitting and its linewidth an upper bound on the decoherence rate of the electron spin dynamics. We illustrate the experimental feasibility of our proposal with estimates for Fe10 molecules.

\]

Magnetic molecular clusters have been the subject of intense research in recent years, because they offer the possibility of observing macroscopic quantum phenomena . Ring systems such as the antiferromagnetic (AF) ferric wheels, Fe6 and Fe10 , also allow one to study the transition from microscopic magnetism to one-dimensional bulk magnetism. In ferromagnetic clusters such as Fe8 and Mn12, incoherent tunneling of the $`S=10`$ magnetic moment is observed directly in magnetization and susceptibility measurements . The AF ferric wheels are candidates for the observation of macroscopic quantum coherence (MQC) in the form of coherent tunneling of the Néel vector . Although quantum effects in antiferromagnets are expected to be more pronounced than in ferromagnets , the detection of quantum behavior is experimentally more challenging . The reason for this is that magnetization and susceptibility measurements probe only the total spin of the molecule which, by symmetry, remains unaffected upon tunneling of the Néel vector $`𝐧`$. At low temperatures, the dynamics of $`𝐧`$ is determined by two characteristic frequencies, the tunneling rate $`\mathrm{\Delta }/\mathrm{}`$ and the electron spin decoherence rate $`\mathrm{\Gamma }_S`$. In Fe10, $`\mathrm{\Delta }`$ can be tuned from $`0`$ to $`2`$K by varying the magnetic field . Although the tunnel splitting $`\mathrm{\Delta }`$ enters thermodynamic quantities such as magnetization and specific heat, no conclusive results revealing the characteristic functional dependence $`\mathrm{\Delta }(B)`$ have yet been obtained . Measuring $`\mathrm{\Gamma }_S`$ is of central importance for the characterization of the quantum tunneling, since coherent quantum tunneling requires $`\mathrm{\Gamma }_S\mathrm{\Delta }`$. An estimate of $`\mathrm{\Gamma }_S`$ can be obtained from the typical energy scales of various interactions leading to decoherence. Spin-phonon interactions are frozen out at low $`T`$. Nuclear dipolar ($`0.1`$mK) and hyperfine ($`1`$mK) interactions are significantly smaller than interring electron spin dipolar interactions (some $`10`$mK). These numbers indicate that, in Fe10, tunneling of $`𝐧`$ is coherent for a wide range of $`\mathrm{\Delta }`$.

Motivated by these numbers, in this paper we study the quantum spin dynamics of the ferric wheel. We show that the tunnel dynamics of $`𝐧`$ enters the correlation functions of a single electron spin. As indicated in  for a bulk AF system, a nuclear spin coupled to a single electron spin acts as a local spin probe. We show that in small AF rings in which $`𝐧`$ itself has additional coherent dynamics, the correlation functions of the nuclear spin exhibit signatures of the tunneling of $`𝐧`$. In particular, we discuss the coherent dynamics of one nuclear spin coupled to one of the electron spins of the ferric wheel and show that both the tunnel splitting $`\mathrm{\Delta }`$ and the electron spin decoherence rate can be obtained from NMR and ESR spectra.

The ferric wheels Fe6 and Fe10 are well characterized . The $`s=5/2`$ Fe III ions are arranged on a ring, with an AF nearest-neighbor exchange coupling $`J>0`$ and a weak, easy-axis anisotropy directed along the ring axis $`𝐞_z`$. The minimal Hamiltonian for the system is

$$H_0=J\underset{i=1}{\overset{N}{}}𝐬_i𝐬_{i+1}+𝐡\underset{i=1}{\overset{N}{}}𝐬_ik_z\underset{i=1}{\overset{N}{}}s_{i,z}^2,$$
(1)
where $`N=10`$ or $`6`$ and $`𝐬_{N+1}𝐬_1`$, $`𝐡=g\mu _B𝐁`$, with $`𝐁`$ the external magnetic field and $`g=2`$ the electron spin $`g`$-factor. For Fe10, $`J=15.56\mathrm{K}`$ and $`k_z=0.0088J`$. For Fe6, the values for $`J`$ and $`k_z`$ vary appreciably depending on the central alkali metal atom: for Na:Fe6, $`J=32.77\mathrm{K}`$ and $`k_z=0.0136J`$, whereas for Li:Fe6, $`J=20.83\mathrm{K}`$ and $`k_z=0.0053J`$ .

For $`k_z=0`$, the eigenstates of $`H_0`$ are also eigenstates of the operator of total spin, $`𝐒=_{i=1}^N𝐬_i`$, with $`E_{S,S_x}=(2J/N)S(S+1)+hS_x`$ . For $`k_z2J/(Ns)^2`$, the anisotropy can be taken into account in perturbation theory in $`k_z`$. The scenario changes drastically for $`k_z2J/(Ns)^2`$, when $`𝐧`$ (staggered magnetization) is localized along $`\pm 𝐞_z`$. We label the states with $`𝐧`$ oriented along $`\pm 𝐞_z`$ by $`|`$ and $`|`$. In a semiclassical description, the low-energy sector of the ferric wheel consists of two states, a ground state, $`|g=(|+|)/\sqrt{2}`$, and a first excited state, $`|e=(||)/\sqrt{2}`$. The static equilibrium properties of a system described by Eq. (1) are discussed in detail in Ref. . With $`𝐁𝐞_x`$, i.e. in the plane of the ring, the system exhibits interesting spin dynamics: In the high field regime, $`h_x\mathrm{}\omega _0`$, $`𝐧`$ is confined to the $`(y,z)`$-plane and tunneling takes place through the potential barrier of height $`Nk_zs^2`$. In particular, $`\mathrm{\Delta }=\mathrm{\Delta }_0|\mathrm{sin}(\pi Nh_x/4J)|`$, with $`\mathrm{\Delta }_0=8\mathrm{}\omega _0\sqrt{𝒮/2\pi \mathrm{}}e^{𝒮/\mathrm{}}`$, $`\omega _0=s\sqrt{8Jk_z}/\mathrm{}`$, and $`𝒮/\mathrm{}=Ns\sqrt{2k_z/J}`$, shows oscillatory behavior as a function of $`h_x`$ . We restrict our considerations henceforth to the geometry $`𝐁𝐞_x`$. For Fe10, $`\mathrm{\Delta }_02.18`$K is much larger than in, e.g., Mn12  or Fe8.

Spin susceptibilities. - We consider first the standard ac. spin susceptibility and ESR measurements, in which an infinitesimal magnetic probing field couples to the total spin $`𝐒=_{i=1}^N𝐬_i`$ of the ferric wheel. We will show that these experimental techniques are insufficient to detect coherent tunneling of $`𝐧`$ in a system described by $`H_0`$ alone. In an effective-action description for the system (1) with Lagrangian density $`L_E[𝐧]`$ , we find $`𝐒=\frac{N}{4J}[i𝐧\times \dot{𝐧}𝐡+𝐧(𝐧𝐡)]`$. In high magnetic fields $`h_x\mathrm{}\omega _0`$, the spin susceptibility, $`\chi _{\alpha \alpha }(\omega )=_0^\beta \mathrm{}d\tau T_\tau \widehat{S}_\alpha (\tau )\widehat{S}_\alpha e^{i\omega _n\tau }|_{i\omega _n\omega +i0}`$, with $`\alpha =x,y,z`$, $`\beta =1/k_BT`$, and $`T_\tau `$ the imaginary time ordering operator, may be evaluated using spin path integrals. For $`\omega ,k_BT/\mathrm{}\omega _0,h_x/\mathrm{}`$, up to corrections $`𝒪(e^{𝒮/\mathrm{}})`$,

$$\chi _{\alpha \alpha }(\omega )=\frac{N}{4J}f_\alpha ,$$
(2)
with $`f_x=1𝒪(\pi ^2N\mathrm{\Delta }/8J)`$ and $`f_yf_z1`$. It is clear from eq. (2) that the susceptibilities $`\chi _{\alpha \alpha }(\omega )`$ for the ring (1) do not exhibit resonances at $`\omega =\pm \mathrm{\Delta }/\mathrm{}`$. The main conclusion we draw from eq. (2) is that a uniform magnetic field cannot drive transitions from $`|g`$ to $`|e`$. Starting from the rigid rotor Hamiltonian of the ferric wheel , this result can also be shown to hold for an arbitrary direction of $`𝐁`$.

We consider next the correlation function of a single spin, $`T_\tau \widehat{s}_{i,\alpha }(\tau )\widehat{s}_{i,\alpha }s^2T_\tau n_\alpha (\tau )n_\alpha `$, for $`h_x4Js`$, with $`i=1,\mathrm{},N`$. In contrast to the correlations of $`𝐒`$ discussed above, $`T_\tau \widehat{s}_{i,\alpha }(\tau )\widehat{s}_{i,\alpha }`$ indeed exhibits signatures of coherent tunneling of $`𝐧`$. To evaluate the correlation function, we use an effective two-state description for the ferric wheel and introduce a pseudospin $`\mathrm{}𝝈/2`$, with $`|`$ and $`|`$ being eigenstates of $`\sigma _z`$. The tunneling dynamics of the Néel vector $`𝐧`$ is then generated by the pseudo-Hamiltonian $`\mathrm{\Delta }\sigma _x/2`$. Because $`T_\tau n_z(\tau )n_zT_\tau \sigma _z(\tau )\sigma _z`$ in the low-energy sector, we obtain immediately

$$T_\tau \widehat{s}_{i,z}(\tau )\widehat{s}_{i,z}(\tau ^{})s^2\frac{\mathrm{cosh}[(\beta 2|\tau \tau ^{}|)\mathrm{\Delta }/2]}{\mathrm{cosh}[\beta \mathrm{\Delta }/2]}.$$
(3)
After analytic continuation, the real-time correlation function exhibits the $`e^{\pm i\mathrm{\Delta }t/\mathrm{}}`$ time dependence characteristic of coherent tunneling. We conclude that local spin probes allow the observation of the Néel vector dynamics. Nuclear spins which couple (predominantly) to a given $`𝐬_i`$ are ideal candidates for such probes, as we shall discuss next.

Nuclear susceptibility. - NMR techniques have been widely used to study molecular magnets . In the following we show that nuclear spins can also be used as a local probe to detect coherent tunneling of $`𝐧`$. For simplicity, we restrict our considerations to interactions of the form $`H^{}=A𝐬_1𝐈`$, which includes both the hyperfine contact interaction and the direction-independent part of the magnetic dipolar interaction. For 57Fe, the dominant coupling to the electron spin is by a hyperfine contact interaction, $`A_{\mathrm{Fe}}s3.3`$mK . In contrast, the interaction of a 1H nuclear spin with the electron spins is dipolar, with a direction-independent term $`_iA_i𝐬_i𝐈`$. For AF order, the sum yields an effective coupling $`A_\mathrm{H}s𝐧𝐈`$, where, for Fe10, the coefficient $`A_\mathrm{H}=_i(1)^{i+1}A_i`$ depends strongly on the site of the proton spin $`𝐈`$. For many of the inequivalent sites, however, $`A_H`$ is of order $`0.1`$mK . With $`N_{\mathrm{Fe}}`$ and $`N_\mathrm{H}`$ the numbers of NMR-active 57Fe and proton nuclei, as long as $`N_{\mathrm{Fe}}A_{\mathrm{Fe}}+N_\mathrm{H}A_\mathrm{H}\mathrm{\Delta }`$, the effect of the nuclear spins on the electron spin dynamics remains small. We define the decoherence rates $`\mathrm{\Gamma }_I`$ and $`\mathrm{\Gamma }_S`$ of the nuclear and electronic spins as the decay rates of $`I_y(t)I_y`$ and $`n_z(t)n_z`$, respectively. For time scales $`t<1/\mathrm{\Gamma }_S`$, the electron spin produces a coherently oscillating effective magnetic field with frequency $`\mathrm{\Delta }/\mathrm{}`$ at the site of the nucleus.

In order to show that this field affects the nuclear spin dynamics, we now consider a single, NMR-active 57Fe or 1H nucleus (inset of Fig. 1). For $`k_BT\mathrm{}\omega _0`$, we may restrict our considerations to the Hilbert space spanned by $`\{|g,|e\}`$. By using the decomposition $`𝐬_i=(1)^{i+1}s𝐧+𝐒/N`$ of a single spin into staggered magnetization $`\pm s𝐧`$, $`𝐧^2=1`$, and fluctuations $`𝐒𝐧`$ around the Néel ordered state, we obtain $`H^{}=A𝐬_1𝐈As𝐧𝐈`$. We show now that, due to $`e|n_z|g0`$ , the tunneling dynamics of $`𝐧`$ can be obtained from the nuclear spin correlation functions $`I_\alpha (t)I_\alpha `$. With $`e|n_z|g=𝒪(1)`$, the dominant term in $`H^{}`$ is $`Asn_zI_z`$, or in the pseudospin notation introduced above,

$$H^{}Asn_zI_zAs\sigma _zI_z.$$
(4)
NMR experiments measure via power absorption the imaginary part of the nuclear spin susceptibility, $`\chi _{I,\alpha \alpha }^{\prime \prime }(\omega )`$, and by pulsed techniques the nuclear spin correlation functions $`I_\alpha (t)I_\alpha `$ in the time domain . From expanding $`I_\alpha (t)I_\alpha `$ in $`H^{}`$,

$`I_\alpha (t)I_\alpha I_\alpha (t)I_\alpha _0A^2s^2/\mathrm{}^2{\displaystyle _{\mathrm{}}^t}dt^{}{\displaystyle _{\mathrm{}}^0}dt^{\prime \prime }`$ (5)
$`\times [I_z(t^{}),I_\alpha (t)][I_z(t^{\prime \prime }),I_\alpha ]_0n_z(t^{})n_z(t^{\prime \prime })_0,`$ (6)
it is evident that the dynamics of $`𝐧`$ enters $`\chi _{I,\alpha \alpha }^{\prime \prime }(\omega )`$.

To evaluate eq. (5), we diagonalize the Hamiltonian

$$H=\frac{\mathrm{\Delta }}{2}\sigma _x+\gamma _IB_xI_x+AsI_z\sigma _z,$$
(7)
with $`\gamma _I`$ the nuclear gyromagnetic ratio, which describes the ferric wheel in the low-energy sector with a single nuclear spin $`𝐈`$ coupled to $`𝐬_1`$, eq. (4). We assume thermal equilibrium for both electron and nuclear spins. For Fe10 in the high field regime, the results may be derived by expansion to leading order in $`As/\mathrm{\Delta }`$ and $`\gamma _IB_x/\mathrm{\Delta }`$, because $`\mathrm{\Delta }_0\gamma _IB_x,As`$, for both 57Fe and 1H nuclei, and $`B_x10\mathrm{T}`$. For $`I=1/2`$, $`\chi _{I,zz}^{\prime \prime }(\omega )`$ displays the unperturbed emission and absorption peaks at $`\omega \pm \gamma _IB_x/\mathrm{}`$, although these are slightly shifted if the hyperfine term $`A𝐒𝐈/N`$ is taken into account. $`\chi _{I,xx}^{\prime \prime }(\omega )`$, however, displays resonant absorption and emission of small intensity at $`\omega =\pm (\mathrm{\Delta }\pm \gamma _IB_x)/\mathrm{}`$. Finally,

$`\chi _{I,yy}^{\prime \prime }(\omega )={\displaystyle \frac{\pi }{4}}[\mathrm{tanh}\left({\displaystyle \frac{\beta \gamma _IB_x}{2}}\right)\delta (\omega \gamma _IB_x/\mathrm{})`$ (8)
$`+\left({\displaystyle \frac{As}{\mathrm{\Delta }}}\right)^2\mathrm{tanh}\left({\displaystyle \frac{\beta \mathrm{\Delta }}{2}}\right)\delta (\omega \mathrm{\Delta }/\mathrm{})][\omega \omega ]`$ (9)
exhibits satellite resonances at the tunnel splitting $`\mathrm{\Delta }`$ of the electron spin system. Their physical origin is readily understood in terms of a classical vector model. For $`A=0`$, $`𝐈(t)`$ precesses around the static magnetic field $`𝐁=B_x𝐞_x`$. For $`A0`$, the coherent tunneling of $`𝐧`$ leads to an additional ac hyperfine field $`A𝐬_1(t)As\mathrm{cos}(\mathrm{\Delta }t/\mathrm{})𝐞_z`$ at the site of the nucleus. In contrast to a static hyperfine field which induces a change in precession frequency and axis, the rapidly oscillating hyperfine field in Fe10 leads only to a small deviation $`\delta 𝐈(t)=𝒪(As/\mathrm{\Delta })`$ from the original precession. In particular, $`\delta I_y(t)(As/\mathrm{\Delta })\mathrm{sin}(\mathrm{\Delta }t/\mathrm{})`$ also oscillates at frequency $`\mathrm{\Delta }/\mathrm{}`$ and hence gives rise to the second term in eq. (8).

We restricted the above analysis to the low-energy sector of the ferric wheel. To check this approximation, we have performed exact numerical diagonalization (ED) on a small AF ring with one nuclear spin of $`I=1/2`$ coupled to one of the electron spins. For the small systems accessible by ED, in this case $`N=4`$, $`s=3/2`$, and $`k_z=0.2J`$, the field range for which the theoretical framework is applicable becomes rather small: $`2Jh_x6J`$. However, the numerical results (Fig. 1) for $`e|I_y|g`$ indicate that our analytical value $`|e|I_y|g|=As/2\mathrm{\Delta }`$ entering eq. (8) is a good approximation. For our parameters, the analytical value tends to overestimate $`e|I_y|g`$ by $`30`$% which results from the neglect of $`n_y`$ in eq. (4).

We turn next to a discussion of the experimental feasibility of measuring $`\mathrm{\Delta }`$ by NMR. Because $`As/\mathrm{\Delta }1`$, the intensity of the satellite peaks at $`\omega =\pm \mathrm{\Delta }/\mathrm{}`$ (8) is small compared to that of the main peaks at $`\omega =\pm \gamma _IB_x/\mathrm{}`$. However, this satellite peak intensity may be increased significantly by tuning $`B_x`$ close to one of the critical values $`B_x^c`$ at which the magnetization of the ferric wheel jumps and $`\mathrm{\Delta }(B_x=B_x^c)=0`$. Note, however, that our theory only applies to high magnetic fields, $`B_x>7.7`$T for Fe10. Coherent tunneling of the Néel vector $`𝐧`$ requires $`\mathrm{\Delta }\mathrm{\Gamma }_S`$. From the estimates for the decoherence rate $`\mathrm{\Gamma }_S`$ given in the introduction we conclude that this condition can be satisfied even for a large range of $`\mathrm{\Delta }/\mathrm{\Delta }_01`$.

We consider first 57Fe, with $`\gamma _I=0.18\mu _N`$ . For $`T2`$K and $`B_x10`$T, the relative intensity of the satellite peak at $`\mathrm{\Delta }=\mathrm{\Delta }_0=2.18`$K, is $`(As/\mathrm{\Delta })^2\mathrm{tanh}(\beta \mathrm{\Delta }/2)/\mathrm{tanh}(\beta \gamma _IB_x/2)0.007`$. This intensity, however, increases by a factor of 10 (100) for $`\mathrm{\Delta }=0.1\mathrm{\Delta }_0`$ ($`\mathrm{\Delta }=0.01\mathrm{\Delta }_0`$). For 1H with $`\gamma _I=5.59\mu _N`$ , and a typical value $`As0.1`$mK, the relative peak intensity is $`2.05\times 10^7`$ ($`\mathrm{\Delta }=\mathrm{\Delta }_0`$), $`2.25\times 10^6`$ ($`\mathrm{\Delta }=0.1\mathrm{\Delta }_0`$), and $`2.25\times 10^5`$ ($`\mathrm{\Delta }=0.01\mathrm{\Delta }_0`$). However, the number of protons in the ring is much larger than that of NMR-active 57Fe nuclei, $`10N_\mathrm{H}/N_{\mathrm{Fe}}100`$, depending on the doping with 57Fe. Taking into account that the sensitivity of proton NMR is larger than that of Fe NMR by a factor of $`3\times 10^4`$ , 57Fe and proton NMR appear to be similarly appropriate for detecting the coherent tunneling of $`𝐧`$. The observation of the satellite peak in (8) is feasible, but still remains a challenging experimental task. The experiment must be conducted with single crystals of Fe10 (or a Fe6 system with sufficiently large $`k_z>2J/(Ns)^2`$) at high, tunable fields ($`10`$T) and low temperatures ($`2`$K). Moreover, because $`B_x^c`$ depends sensitively on the relative orientation of $`𝐁`$ and the easy axis , careful field sweeps are necessary to ensure that $`\mathrm{\Delta }/\mathrm{\Delta }_01`$ is maintained . Note that the NMR experiment suggested here could be more easily realized with nuclear spins exhibiting higher NMR sensitivity than 57Fe.

We show now that, from NMR spectra, also an upper bound for $`\mathrm{\Gamma }_S`$ can be extracted. The NMR resonance lines are broadened by the decoherence of the nuclear spin, with width $`\mathrm{\Gamma }_I`$ at $`\pm \gamma _IB_x/\mathrm{}`$. The NMR resonances at $`\omega =\pm \mathrm{\Delta }/\mathrm{}`$ also involve correlation functions of $`𝐧`$, see (5). Thus the decoherence of the electron spin, $`\mathrm{\Gamma }_S`$, adds to the linewidth, and the width of the satellite peak, $`\delta `$, is bounded by $`\mathrm{\Gamma }_I+\mathrm{\Gamma }_S<\delta `$. Measurement of $`\delta `$ then provides an upper bound for $`\mathrm{\Gamma }_S`$. Further, $`\mathrm{\Gamma }_S\mathrm{\Delta }`$ marks the transition from coherent to incoherent tunneling dynamics. Hence, if $`\delta <\mathrm{\Delta }`$ this would indicate unambigously that quantum tunneling of $`𝐧`$ is coherent. Note that the maximum peak height of a Lorentzian resonance line is $`𝒪(1/\delta )`$, so a large $`\mathrm{\Gamma }_S`$ ($`<\mathrm{\Delta }`$) would make detection of the satellite peak increasingly difficult.

ESR measurements in the presence of hyperfine interaction. - We show now that, in the presence of a hyperfine coupling $`H^{}`$, the electron spin susceptibility of the ring, $`\chi _{\alpha \alpha }(\omega )`$, also exhibits the signature of a coherent tunneling of $`𝐧`$. This results from the fact that integration over the initial and final nuclear spin configurations causes the matrix elements $`e|𝐒|g`$ occurring in the spectral representation of $`\chi _{\alpha \alpha }(\omega )`$ (eq. (2)) to become finite. In the high field limit $`h_x\mathrm{}\omega _0`$, the matrix elements become $`|e|S_y|g|(As/2h_x)(\mathrm{\Delta }_0𝒮/4Nk_zs^2)|\mathrm{cos}(\pi Nh_x/4J)|`$ and $`|e|S_z|g|As/2h_x`$. For a small system ($`N=4`$, $`s=3/2`$), we have again confirmed the qualitative features of these results by ED. It follows that $`\chi _{\alpha \alpha }^{\prime \prime }(\omega \mathrm{\Delta }/\mathrm{})=\pi |e|S_\alpha |g|^2\mathrm{tanh}(\beta \mathrm{\Delta }/2)\delta (\omega \mathrm{\Delta }/\mathrm{})`$ exhibits resonances at $`\mathrm{\Delta }/\mathrm{}`$. A qualitative understanding of this result may be obtained by noting that a nuclear spin polarized along $`𝐁`$ results in an effective magnetic field $`𝐞_xA/2g\mu _B`$ acting only on $`𝐬_1`$. In a classical description this hyperfine field causes $`𝐒`$ to acquire a component $`𝐧As/2h_x`$ along $`𝐧`$, and the coherent tunneling of $`𝐧`$ now also results in an oscillation of the total spin $`𝐒`$. Again, the decoherence rate of these oscillations, and hence the linewidth of the ESR resonance, is bounded by $`\mathrm{\Gamma }_S`$. Note that $`As/2h_x=1.2\times 10^4`$ for a single 57Fe nucleus with $`B_x=10`$T, so the ESR signal is very weak in this case.

However, our calculations apply to any impurity spin $`𝐣`$, which interacts with a single electron spin only, $`H^{}=A𝐬_1𝐣`$. In particular, for an electronic $`𝐣`$, $`A`$ is typically $`10^3`$ times larger than for a nuclear spin, and ESR techniques become a valuable tool for detecting the tunneling of $`𝐧`$. One advantage of this technique is that it is no longer necessary to have $`\mathrm{\Delta }/\mathrm{\Delta }_01`$ to obtain a large signal intensity, and thus the complete range of tunnel frequencies could be explored experimentally . Our calculations also apply to situations in which several impurity spins $`𝐣_i`$ produce different net magnetic fields for the two sublattices of the AF ring. For illustration, we discuss two simple scenarios. We consider $`N/2`$ impurity spins $`𝐣_i`$ ($`j_i=1/2`$) coupled to $`𝐬_1`$, $`𝐬_3`$, …, $`H^{}=A_{i=1}^{N/2}𝐣_{2i1}𝐬_{2i1}`$. For $`h_xAs,k_BT`$, all $`𝐣_i`$ align with the magnetic field $`𝐁`$. Since they all couple to one sublattice only, their net magnetic fields acting on $`𝐬_i`$ add up, $`|e|S_z|g|(N/2)As/2h_x`$, leading to a $`(N/2)^2`$-fold enhancement of the ESR-signal of a single impurity. In contrast, a single impurity $`𝐣`$ coupled to both $`𝐬_1`$ and $`𝐬_2`$, $`H^{}=A𝐣(𝐬_1+𝐬_2)`$, results in the same net magnetic field acting on both sublattices, $`e|S_z|g=0`$.

Conclusions - We have shown that NMR and ESR techniques can be used to measure both the tunnel splitting $`\mathrm{\Delta }`$ and the decoherence rate $`\mathrm{\Gamma }_S`$ in the ferric wheel. For Fe10, we showed that our proposal is within experimental reach. Our considerations apply to any AF ring system described by $`H_0`$, eq. (1), with some impurity spin coupled to one of the electron spins. Hence, the proposed scheme may prove useful for a wide class of molecular magnets.

This work was supported by the European Network MolNanoMag, grant number HPRN-CT-1999-00012, the BBW Bern, and the Swiss NSF. We are grateful to A. Cornia, A. Lascialfari, M. Leuenberger, S. Meier, and B. Normand for stimulating discussions. We are particularly indebted to A. Lascialfari for useful discussions on the experimental realization.