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# HST Proper Motion confirms the optical identification of the nearby pulsar PSR 1929+101footnote 11footnote 1Based on observations with the NASA/ESA Hubble Space Telescope, obtained at the Space Telescope Science Institute, which is operated by AURA, Inc. under contract No NAS 5-26555

## 1 Introduction

PSR1929+10 is an old ($`310^6`$ yrs) radio pulsar. With a distance of $``$ 330 pc, determined from VLBA radio parallax measurements (Brisken et al. 2002), it is also one of the closest to the solar system. After the original X-ray detection with Einstein (Helfand 1983), pulsations at the radio period (227 ms) were discovered by ROSAT (Yancopulous et al. 1994) and later confirmed in ASCA data (Wang and Halpern 1997). The X-rays pulse profile exhibits a single, broad, peak markedly different from the sharp radio one. The X-ray spectrum can be described either by a blackbody ($`T3510^6K`$) produced from hot polar caps (Yancopulous et al. 1994; Wang and Halpern 1997) or by a power law with $`\alpha 1.27\pm 0.4`$ (Becker and Trümper 1997). A trail of diffuse X-ray emission originated from the pulsar and extending $``$ 10 arcmin to South East was discovered with the ROSAT/PSPC (Wang et al. 1993). A candidate optical counterpart to PSR1929+10 was identified with the HST/FOC by Pavlov et al. (1996) based on the positional coincidence ($`0\stackrel{}{\mathrm{.}}4`$) with the radio coordinates. Interestingly, the measured flux of the PSR1929+10 counterpart ($`U25.7`$) was found to deviate by 3 orders of magnitude from the values predicted from the X-ray spectra. This behaviour is markedly different from that of the middle aged pulsars PSR0656+14 (Pavlov et al. 1997), Geminga (Mignani et al. 1998) and PSR1055-52 (Mignani et al. 1997), where the optical data are not too far from the extrapolation of the X ray spectra. Confirming the optical identification of PSR1929+10 becomes a crucial step to settle a consistent scenario for the long term evolution of the optical luminosity of pulsars and to investigate possible turnovers in the emission physics. While young ($`10^310^4`$ yrs) objects are relatively bright, their optical throughput seems to decay on a timescale of few thousands years and progressively turn to a composite magnetospheric/thermal regime (Mignani 1998; Caraveo 2000). Although evidence for such a trend can be recognized in middle-aged objects ($`10^5`$ yrs), like PSR 0656+14 and Geminga, little is known on the optical emission at later stages of the pulsar lifetime.
Taking advantage of new HST observations, we use the pulsar proper motion to secure the PSR 1929+10 optical identification, thus adding an important piece of information on the optical behaviour of old pulsars. Observations and data reduction are described in §2, while the results are discussed in §3.

## 2 Observations

The field of PSR 1929+10 was observed with the STIS detector aboard HST in five different visits on August 28th 2001, September 11th, 15th, 21st 2001, October 20th 2001. The observations were performed after the reactivation of the STIS following problems with the power supply units occurred in May 2001. Owing to this malfunction, the observations could have been affected by a residual few percent increase of the dark current level. For each visit, the total integration time was 2 400 s, split in two exposures of 1 200 s each. Observations run smoothly apart from short gaps ($``$ 60 s) in the engineering telemetry occurred during visits #3 and #4. The NUV-MAMA detector, with a pixel size of $`0\stackrel{}{\mathrm{.}}024`$ ($`24\stackrel{}{\mathrm{.}}7\times 24\stackrel{}{\mathrm{.}}7`$ field of view), was used its TIME-TAG mode to obtain time-resolved images with a temporal resolution of $`125\mu `$s. To add spectral information in the NUV and to complement previous data obtained with the FOC at $`\mathrm{3\hspace{0.17em}400}\AA `$ by Pavlov et al. (1996), the exposures were taken through the F25QTZ filter ($`\lambda =2364\AA ,\mathrm{\Delta }\lambda 842\AA FWHM`$).
Our identification strategy was based on two independent and complementary approaches. Firstly, following the straightforward, but powerful, strategy successfully applied in the case of the identification of PSR 0656+14 (Mignani, De Luca and Caraveo 2000), we performed a proper motion measurement of the proposed counterpart to be compared with the known one of the radio pulsar, recently reassessed by Brisken et al. (2002) using the VLBA. Secondly, we used our time-resolved images to search for pulsations at the radio period from the candidate counterpart. The proper motion measurement is described in the following sections, while the results of the timing analysis are presented in a companion paper (Mignani et al. in preparation).

### 2.1 Data Analysis

As starting point for our proper motion measurement we used the FOC observations of Pavlov et al. (1996), collected on July 10th 1994. Images were taken in three different filters: F130LP ($`\lambda =3437.7\AA ,\mathrm{\Delta }\lambda 1965\AA FWHM`$), F342W ($`\lambda =3402\AA ,\mathrm{\Delta }\lambda 442\AA FWHM`$) and F430W ($`\lambda =3940\AA ,\mathrm{\Delta }\lambda 832\AA FWHM`$), with total integration times of 1221, 3310 and 596 s, respectively. The camera was operated at two different focal lenghts corresponding to a field of view of $`7\stackrel{}{\mathrm{.}}4\times 7\stackrel{}{\mathrm{.}}4`$ for the F130LP and F342W exposures and of $`14\stackrel{}{\mathrm{.}}8\times 14\stackrel{}{\mathrm{.}}8`$ for the F430W one. In both cases, the angular resolution was $`0\stackrel{}{\mathrm{.}}014`$ per pixel. The data were retrieved from the ST-ECF public archive after on-the-fly recalibration with the best reference files. As shown by Pavlov et al. (1996), the pulsar counterpart is detected only through the F130LP and the F342W filters (see their figures 2c and 3a).
The STIS images were retrieved from the STScI data archive after the default pipeline calibration. Each image has been corrected for the geometric distortion of the CCD using the DRIZZLE software distributed in the STSDAS package222stsdas.stsci.edu/STSDAS.html and applying the most recent coefficients of the cubic mapping of the NUV-MAMA field of view listed in the STIS Users’ Handbook333www.stsci.edu/hst/stis/documents/handbooks/cycle11/stis\_cy11\_ihbTOC.html. The two exposures taken during each visit were coadded after accounting for thiny shifts (of order 0.4 pixels) and differences in roll angle (of order 0.03) due to the spacecraft jitter. For each couple, the average coadditon accuracy was of $``$ 0.1 pixels in both $`x`$ and $`y`$.

Since the expected overall displacement of the pulsar counterpart ($``$ 15 mas, equivalent to 0.6 STIS pixels) in the epoch interval spanned by our observations (2001.65-2001.80) would be negligible with respect to the total displacement ($``$ 770 mas) predicted since the reference epoch (1994.52), we first combined all the five available STIS images to benefit of the higher $`S/N`$. Using as relative reference grid the coordinates of 7 to 10 common stars (the actual number depending on the telescope roll angle), all the frames were registered on the mid-epoch frame (i.e. the september 15th one) by fitting a linear coordinate transformation after aligning each frame in right ascension and declination according to the telescope roll angles. The final STIS image resulting from the combination of all the available frames is shown in Figure 1. As expected in the case of a moving object, the centering accuracy of the target in the combined image (0.3 pixels in RA and 0.15 pixels in Dec) appears degraded wrt to the values measured in each single single frame, for which we found accuracies of $``$ 0.1 pixels in both coordinates. To the error on the centroid determination we then added in quadrature the rms on the epoch-to-epoch coordinate transformation, which in all cases turned out to be within 0.2 pixels (per coordinate), plus the accuracy of the exposures coaddition in each visit (0.1 pixels). The final precision on the target position in the combined STIS image was thus 0.37 pixels in RA and 0.27 pixels in Dec.

Next step was to apply the STIS-to-FOC registration to evaluate the relative displacement of the pulsar counterpart over the $``$ 7.2 years interval spanned by the available observations. Although our target was clearly detected in the FOC/F130LP image (preferred to the F342W one because of its higher $`S/N`$), its $`7\stackrel{}{\mathrm{.}}4\times 7\stackrel{}{\mathrm{.}}4`$ field of view containes only one object in common with the wider STIS image ($`24\stackrel{}{\mathrm{.}}7\times 24\stackrel{}{\mathrm{.}}7`$). Thus, we decided to register both images on a common reference frame defined by the FOC/F430W image ($`14\stackrel{}{\mathrm{.}}8\times 14\stackrel{}{\mathrm{.}}8`$). This allowed us to use three bright reference objects for the FOC/130LP-to-FOC/430W superposition (accounting for shift and rotation for a resulting accuracy of 0.3 FOC pixels per coordinate) and 4 good reference objects for the STIS-to-FOC/430W superposition (rms of 0.55 FOC pixels per coordinate \- accounting for shift, rotation and scale factor). The overall accuracy in the final STIS-to-FOC/F130LP superposition was thus obtained by adding in quadrature all the uncertainties quoted above and turned out to be $``$ 0.6 FOC pixels per coordinate.

## 3 Results

### 3.1 Proper Motion

After registering both the FOC and the STIS images on a unique reference frame, we could evaluate the displacement of the pulsar candidate counterpart by simply measuring the difference in its relative coordinates. The overall uncertainty on such difference was estimated by adding in quadrature all the uncertainties derived from the different steps of our relative astrometry procedure. These include: the centering error of the counterpart in the combined five-epochs STIS image (0.37 STIS pixels in RA and 0.27 pixels in Dec) and in the FOC/130LP image ($``$ 0.1 FOC pixels per coordinate) plus the overall accuracy of the STIS-to-FOC/130LP superposition (0.6 FOC pixels per coordinate) as obtained by the two-step procedure described in the previous section. The difference in the relative coordinates is 48.7 $`\pm `$ 1.0 FOC pixels and 23.2 $`\pm `$ 1.0 FOC pixels along the RA and Dec directions, respectively. Such measurements represent a clear evidence for the object displacement over the $``$ 7.2 years time span between the FOC (1994.52) and the average STIS epoch (2001.731). The pulsar displacement can be appreciated in Figure 2, where the relative FOC position is overlayed on the STIS image. After applying the FOC plate scale of $`0\stackrel{}{\mathrm{.}}01435`$/pixel (with 0.5% uncertainty) to translate from pixel to sky coordinates, we computed the proper motion of the pulsar optical counterpart. This is $`\mu _\alpha cos(\delta )=+97\pm 2`$ mas yr-1 and $`\mu _\delta =+46\pm 2`$ mas yr-1, corresponding to a total yearly displacement in the plane of the sky of $`\mu =107.3\pm 1`$ mas yr-1 along a position angle (PA) of 64.6 $`\pm `$ 0.5. Although the FOC and STIS observations were taken at different times of the year, we did not apply any correction for the object’s parallax (Brisken et al. 2002) as the effect of the tiny parallactic displacement is well within our error budget.

As a further check, we have recomputed the pulsar displacement using the FOC/130LP image and, in turn, each of the five single-epoch STIS images. This allowed us to obtain five independent measures for five different epoch pairs (see Table 1) and thus to exclude the effects of unknown systematics in our procedure. In this case, for each STIS image the error on the target position was only due to the combination of the centering error ($``$ 0.1 pixels per coordinates) and the accuracy of the coaddition of the single exposures in each visit (0.1 pixels). The final precision on the target position in each of the five single-epoch STIS images was thus of the order of 0.15 pixels per coordinate. The strategy for the STIS-to-FOC/130LP registration was clearly the same described above. We computed the STIS-to-FOC/430W frame registrations (rms of 0.45 -0.65 FOC pixels per coordinate - accounting for shift, rotation and scale factor) with the same number of objects used in §2.1. The overall accuracy of the final STIS-to-FOC/130LP registrations turned out to be between 0.55 and 0.8 FOC pixels. As described above, the uncertainty on the target displacement is due to the combination of the centering error of the counterpart in the single STIS images (0.15 original STIS pixels in both RA and Dec) and in the FOC/130LP image (0.1 FOC pixels per coordinate) plus the overall STIS-to-FOC/130LP superposition accuracy (0.55-0.8 FOC pixels per coordinate).
The proper motions derived from the displacements computed for each of the five epoch pairs are listed in Table 1, where all the values are seen to be consistent with the proper motion obtained using the combined STIS image. A $`\chi ^2`$ fit to the values listed in Table 1 yields the best proper motion values: $`\mu _\alpha cos(\delta )=+97\pm 1`$ mas yr-1 and $`\mu _\delta =+46\pm 1`$ mas yr-1, corresponding to a yearly displacement $`\mu =107.35\pm 1`$ mas yr-1 along a position angle of 64.63 $`\pm `$ 0.55.
We can now compare our best proper motion value with the most recent radio measure obtained by Brisken et al. (2002), who give $`\mu _\alpha cos(\delta )=+94.82\pm 0.26`$ mas yr-1 and $`\mu _\delta =+43.04\pm 0.15`$ mas yr-1 (65.58 $`\pm `$ 0.09 PA). Although our value is somewhat less precise, we note that the optical proper motion is fully consistent with the radio one. Thus, our proper motion measurement provides a robust proof that the candidate proposed by Pavlov et al. (1996) is indeed the optical counterpart of PSR 1929+10.

### 3.2 Photometry

We have used our STIS images to measure the pulsar flux in the F25QTZ filter. In order to take advantage of the higher $`S/N`$, our photometry has been computed on the combined image (Figure 1). The source counts were extracted using an optimized aperture and the flux conversion was applied using the photometric zeropoint provided by the pipeline STIS flux calibration. We thus derived a flux of (5.4 $`\pm `$ 0.4) $`10^{31}`$ erg cm-2 s-1 Hz-1, corresponding to an ST-mag of 25.4 $`\pm 0.15`$. The attached error takes into account both the accuracy of our aperture photometry and the systematic uncertainty of $``$ 5% which affects the absolute flux calibration of the STIS/MAMA444www.stsci.edu/hst/stis/documents/handbooks/cycle11/stis\_cy11\_ihbTOC.html. The measured flux was then compared with the values obtained with the FOC in the 130LP and 342W filters. For consistency, we have independently reanalized the FOC datasets finding flux values virtually identical to the ones reported in Pavlov et al. (1996). This confirms that the optical points are definetely inconsistent with the extrapolations of the X-ray spectra which, depending on the assumed model (power law or polar caps), predict fluxes $``$ 3 orders of magnitude higher and lower, respectively. The comparison between the FOC and the STIS photometry is shown in Figure 3, where in the upper panel we plotted the measured values and in the lower panel we corrected for a likely upper limit on the extinction of $`E(BV)=0.1`$ (see Pavlov et al. 1996). While the data can not be accounted by a single blackbody function, a power law provides a more straightforward fit. For the two extreme values of the extinction the power law spectral index $`\alpha `$ varies between 1 and 0, respectively. Although the data could also be compatible with a composite model, any realistic spectral fit is hampered both by the few points available and by the limited spectral coverage.

## 4 Conclusions

Using images collected with the STIS camera aboard HST together with archived HST/FOC images taken 7.2 years apart we have measured a very significant angular displacement of the proposed optical counterpart tof PSR 1929+10. This yields a proper motion $`\mu _\alpha cos(\delta )=+97\pm 1`$ mas yr-1 and $`\mu _\delta =+46\pm 1`$ mas yr-1. These values agree with the ones derived from very recent VLBA radio measurements (Brisken et al. 2002), thus providing an unambiguous confirmation of the pulsar identification. Securing the identification of an old pulsar such as PSR 1929+10 is an important step to assess the pulsars’ optical behaviour as a function of their age. At variance with the phenomenology of middle aged objects, such as PSR 0656+14, Geminga and PSR 1055-52, the optical emission of PSR 1929+10 seems unrelated to the X-ray one, be it either of thermal pr non-thermal origin. Although the new STIS data seem to favour a power law rather than a blackbody, the paucity of flux values and the limited spectral coverage available do not allow us to put firmer constraints on the spectrum. More data, expecially at longer wavelengths, are required to better characterize the pulsar spectral shape and to unveil the possible presence of different spectral components. The detection of the optical timing signature will add an important piece of information to understand the optical behaviour of this old pulsar.

RM warmly thanks F. Patat for his help in the finalization of this observing program.


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# CMB limits on large-scale magnetic fields in an inhomogeneous universe

## 1 Introduction

Magnetic fields have been observed in the universe on a wide range of scales. Fields with strengths of a few $`\mu `$G are prolific in galaxies and galaxy clusters, extending well beyond the core regions of the latter, and have also been detected in high redshift Lyman-$`\alpha `$ objects. Magnetic fields in extragalactic structures are detected mainly via radio polarisation studies, X-ray emission and Faraday rotation measurements (see  for a comprehensive review). Magnetic fields in galaxies and galaxy clusters appear to be the result of the nonlinear amplification of weak seed fields, mainly via the galactic dynamo. However, the detection of ordered magnetic fields in high redshift objects (with $`z>2`$) poses a stiff challenge to the dynamo mechanism. As yet, there is no direct evidence of magnetic field presence on cosmological scales, corresponding to a significant fraction of the Hubble length. Clearly, any such field could not arise through structure formation physics, but it would have to be the remnant of a primordial field, redshifting with expansion:

$$B=B_0\left(\frac{a_0}{a}\right)^2,$$
(1)
where $`B_0`$ is the current field strength.

The strength of primordial, cosmological magnetic fields is limited by observed helium abundances and by the near-isotropy of the cosmic microwave background (CMB) (see  for recent reviews). Any magnetic field present at the time of cosmological nucleosynthesis inevitably affects the abundance of primordial Helium, since it provides an additional form of relativistic energy density. This, in turn, increases the expansion rate of the universe with the effect that the neutron-proton freeze out of weak interactions occurs at a higher temperature. The result is an increase in the synthesised abundance of primordial Helium. Hence, Helium-4 observations (extrapolated to zero metalicity) provide an upper limit of $`10^7G`$, in today’s values, on any primordial magnetic field present at nucleosynthesis .

Stronger limits are imposed from the observed high isotropy of the CMB photons. The COBE data place an upper bound on a homogeneous magnetic field present at the time of last scattering. In a recent analysis of a particular class of spatially homogeneous Bianchi universes, an upper bound of $`B_0\begin{array}{c}<\hfill \\ \hfill \end{array}10^9`$G was obtained . Here we generalize previous work to the case of inhomogeneous fields in an inhomogeneous almost-Friedmann universe. We also generalize the limits found in  by weakening some of their assumptions. It turns out that, if we do not assume a spatially homogeneous geometry, the limits imposed directly by CMB data on super-Hubble magnetic fields in an inhomogeneous universe are much weaker, $`B_0\begin{array}{c}<\hfill \\ \hfill \end{array}10^6`$G. A similar situation arises when considering the limits placed on the shear by CMB anisotropies, as pointed out in .

Recently it was proven  under quite general circumstances that a magnetic field is prohibited in spacetimes where exactly isotropic radiation is also present. Taking this as our starting point, small anisotropy allows for a weak magnetic field. We use the 1+3-covariant analysis of CMB temperature anisotropies  and of magnetic fields , in order to derive limits on large-scale fields as a function of coherence scale. Following the approach of , we use the radiation multipoles to derive limits which are model-independent, in the sense that they do not rely on assumptions about the (perturbed Friedmann) spacetime geometry.

In Sec. 2 we outline the general formalism for imposing limits on large-scale magnetic fields from observed CMB temperature anisotropies. In Sec. 3, we give our main results, which follow from a refinement of the method in . For convenience, we omit most of the calculational details, and give the key equations in Appendices A and B. We use units such that $`8\pi G=1=c`$. Our notation follows that of . In particular, $`\dot{X}_{a\mathrm{}b}=u^c_cX_{a\mathrm{}b}`$ and $`\mathrm{D}_a`$ is the covariant derivative in the rest space, i.e., $`\mathrm{D}_cX_{a\mathrm{}b}=h_c^dh_a^e\mathrm{}h_b^f_dX_{e\mathrm{}f}`$, where $`h_{ab}=g_{ab}+u_au_b`$ is the projection tensor. Angled brackets on indices denote the projected, symmetric and trace free (PSTF) part. The 3-divergence and 3-curl of PSTF tensors are $`\mathrm{𝖽𝗂𝗏}X_a=\mathrm{D}^bX_{ab}`$, $`\mathrm{}`$, and $`\mathrm{𝖼𝗎𝗋𝗅}X_a=\epsilon _{abc}\mathrm{D}^bX^c`$, $`\mathrm{𝖼𝗎𝗋𝗅}X_{ab}=\epsilon _{cd(a}\mathrm{D}^cX_{b)}^d`$, $`\mathrm{}`$.

## 2 CMB anisotropy induced by large-scale magnetic fields

In the 1+3-covariant analysis of CMB anisotropy , a physical choice of 4-velocity $`u^a`$ is made, usually the 4-velocity of cold dark matter (CDM), and all perturbative quantities are then covariant vectors or tensors in the rest-space of $`u^a`$, with direct geometrical or physical meaning. The fractional temperature fluctuation is expanded in covariant multipoles $`\tau _A_{\mathrm{}}`$ ($`A_{\mathrm{}}=a_1\mathrm{}a_{\mathrm{}}`$), which are PSTF tensors. These are limited directly by observations:

$$|\tau _A_{\mathrm{}}|\sqrt{\tau _A_{\mathrm{}}\tau ^A_{\mathrm{}}}<ϵ_{\mathrm{}}.$$
(2)
COBE data leads to the values

$`ϵ_2`$ $``$ $`1.1(\pm 0.8)\times 10^5,`$ (3)
$`ϵ_3`$ $``$ $`2.5(\pm 1.3)\times 10^5,`$ (4)
which we use here. The first moment $`\tau _a`$ is the dipole, which is usually attributed to our peculiar motion relative to the CMB frame. We assume this motion is corrected for by setting $`\tau _a=0=ϵ_1`$ for the bulk of the paper. However, it is possible that a residual dipole of cosmological origin exists (it would be frequency dependent, and thus could not be set to zero by a Lorentz boost), and we include it in our calculations for generality.

In addition to the observed bounds on the $`\tau _A_{\mathrm{}}`$, we need bounds on their temporal and spatial gradients, in order to find limits on geometrical and physical quantities that characterize the spacetime. We define the expansion-normalized, dimensionless $`ϵ`$-quantities

$`|\dot{\tau }_A_{\mathrm{}}|`$ $`<`$ $`3Hϵ_{\mathrm{}}^{},|\ddot{\tau }_A_{\mathrm{}}|<9H^2ϵ_{\mathrm{}}^{},\mathrm{},`$
$`|\mathrm{D}_a\tau _A_{\mathrm{}}|`$ $`<`$ $`3Hϵ_{\mathrm{}}^{},|\mathrm{D}_a\mathrm{D}_b\tau _A_{\mathrm{}}|<9H^2ϵ_{\mathrm{}}^{},\mathrm{},`$
$`|(\mathrm{D}_a\tau _A_{\mathrm{}})^{}|`$ $`<`$ $`9H^2ϵ_{\mathrm{}}^{},|(\mathrm{D}_a\mathrm{D}_b\tau _A_{\mathrm{}})^{}|<27H^3ϵ_{\mathrm{}}^{},\mathrm{},`$ (5)
where $`H`$ is the background Hubble rate.

Following , we can find upper bounds on all perturbative quantities in terms of the $`ϵ_{\mathrm{}},ϵ_{\mathrm{}}^{},ϵ_{\mathrm{}}^{}`$, etc. However, the derivative bounds $`ϵ_{\mathrm{}}^{},ϵ_{\mathrm{}}^{}\mathrm{}`$ are not directly measurable, as we are unable to move a cosmological time- or space-separation from our current spacetime event. Here we make the simple assumption that the time- and space-variations of the multipoles are governed respectively by the Hubble rate and the physical scale $`\lambda `$ of the perturbation, i.e.,

$$\left|\dot{\tau }_A_{\mathrm{}}\right|H|\tau _A_{\mathrm{}}|,\left|\mathrm{D}_a\tau _A_{\mathrm{}}\right|\frac{1}{\lambda }|\tau _A_{\mathrm{}}|.$$
(6)
This assumption implies

$`ϵ_{\mathrm{}}^{}{\displaystyle \frac{1}{3}}ϵ_{\mathrm{}},ϵ_{\mathrm{}}^{}{\displaystyle \frac{1}{9}}ϵ_{\mathrm{}},\mathrm{},`$ (7)
$`ϵ_{\mathrm{}}^{}{\displaystyle \frac{1}{3\beta }}ϵ_{\mathrm{}},ϵ_{\mathrm{}}^{}{\displaystyle \frac{1}{9\beta ^2}}ϵ_{\mathrm{}},\mathrm{}\text{where}\beta ={\displaystyle \frac{\lambda }{H^1}}.`$ (8)
The dimensionless parameter $`\beta `$ gives the coherence scale as a fraction of the Hubble length, with $`\beta \begin{array}{c}>\hfill \\ \hfill \end{array}O(1)`$ since we are considering large scales.

The magnetic field is ‘frozen’ into the baryonic fluid, which may be treated as an infinitely conducting medium. Here, we neglect the peculiar velocity of CDM relative to the baryons. The physical justification for doing so comes from the fact that we address the linear regime and consider large scales, where the velocity difference between the two components is expected to be minimal. On these grounds, we choose $`u^a`$ to be the 4-velocity of CDM-baryon fluid with total density $`\rho _\mathrm{M}`$. The kinematics of the pressure-free matter are characterized by the volume expansion $`\mathrm{\Theta }`$, rotation $`\omega ^a`$, acceleration $`A^a`$ and shear distortion $`\sigma _{ab}`$ of $`u^a`$. Note that, even in the absence of pressure gradients, the flow lines are generally non-geodesic (i.e. $`A_a0`$) due to the magnetic field presence. Here, however, we will assume an effectively force-free field (i.e. $`\epsilon _{abc}B^b\mathrm{curl}B^c=0`$), and ignore the acceleration to first order. This is a reasonable approximation, given that the field is too weak to affect the motion of the baryonic matter. It will also allow us to focus upon the purely anisotropic magnetic effects.

The energy-momentum tensor of the magnetized dust is

$$T_{ab}=(\rho _\mathrm{M}+\rho _\mathrm{B})u_au_b+p_\mathrm{B}h_{ab}+\mathrm{\Pi }_{ab},$$
(9)
where $`\rho _\mathrm{B}=B^2/8\pi `$ and $`p_\mathrm{B}=\rho _\mathrm{B}/3`$ are the magnetic energy density and isotropic pressure respectively. Also, $`\mathrm{\Pi }_{ab}=B_aB_b/4\pi `$ is the symmetric and trace free tensor that conveys the anisotropic magnetic effects. The radiation energy-momentum tensor is

$$𝒯_{ab}=\mu u_au_b+\frac{1}{3}\mu h_{ab}+2u_{(a}q_{b)}+\pi _{ab},$$
(10)
where $`\mu `$, $`q_a`$ and $`\pi _{ab}`$ are the photon energy density, momentum density and anisotropic stress. These are directly related to the temperature anisotropy multipoles by

$$q_a=\frac{4}{3}\mu \tau _a,\pi _{ab}=\frac{8}{15}\mu \tau _{ab}.$$
(11)
The photon energy momentum tensor involves only the first two multipoles, but we will require also the octupole

$$\xi _{abc}=\frac{8}{35}\mu \tau _{abc},$$
(12)
which appears in the evolution equation for $`\pi _{ab}`$, Eq. (27).

The field equations $`G_{ab}=T_{ab}+𝒯_{ab}`$, the Ricci identities and the Bianchi identities may be split into a set of evolution (along $`u^a`$) and constraint equations. The evolution of the magnetic field is determined by Maxwell’s equations. The reader is referred to Appendix A for the necessary equations.

## 3 The limits

We first present the CMB limits on inhomogeneous magnetic fields as a function of coherence scale, $`\lambda `$; then we discuss the homogeneous case.

### 3.1 Inhomogeneous universe

Our procedure to find constraints on the magnetic field strength $`\rho _\mathrm{B}`$, or equivalently $`|\mathrm{\Pi }_{ab}|`$, is a generalization of the non-magnetized analysis in . Briefly, we manipulate the field equations to express $`\mathrm{\Pi }_{ab}`$ in terms only of the radiation quantities $`\mu ,q_a,\pi _{ab},\xi _{abc}`$. This is facilitated by the appearance of the shear in Eq. (27), which, in the absence of acceleration, is the only coupling of the radiation to the first-order kinematical quantities. The main aspects of this calculation are in Appendix B, and the key result is Eq. (47).

Neglecting the dipole moment and the energy density of the radiation $`\mathrm{\Omega }_\mathrm{R}`$, and restoring units, Eq. (47) gives

$`B_0`$ $`<`$ $`\mathrm{max}(B)\left({\displaystyle \frac{3}{2}}\right)^{3/4}{\displaystyle \frac{cH_0}{\sqrt{G}}}\{{\displaystyle \frac{1}{4}}\mathrm{\Omega }_\mathrm{M}(5ϵ_2^{}+{\displaystyle \frac{45}{7}}ϵ_3^{})+\mathrm{\Omega }_\mathrm{\Lambda }(ϵ_2^{}+{\displaystyle \frac{9}{7}}ϵ_3^{})`$ (13)
$`+`$ $`2ϵ_2^{}+{\displaystyle \frac{15}{2}}ϵ_2^{}+{\displaystyle \frac{9}{2}}ϵ_2^{}+3ϵ_2^{}+{\displaystyle \frac{9}{2}}ϵ_2^{}+{\displaystyle \frac{81}{10}}ϵ_2^{}`$
$`+`$ $`{\displaystyle \frac{18}{7}}ϵ_3^{}+{\displaystyle \frac{135}{14}}ϵ_3^{}+{\displaystyle \frac{81}{14}}ϵ_3^{}+{\displaystyle \frac{81}{14}}ϵ_3^{}\}^{1/2},`$
where the $`ϵ`$’s are evaluated at the current time. The function $`\mathrm{max}(B)`$ gives upper limits on large-scale magnetic fields, coherent on a given scale $`\lambda `$, imposed by CMB temperature anisotropies. This upper limit is given directly in terms of CMB multipoles and their derivatives, and is model-independent, i.e., no assumptions have been made about the spacetime geometry.

For a numerical estimate, we need to use the simple assumptions of Eqs. (7) and (8), in order to evaluate the derivative-$`ϵ`$’s. Then we find, in terms of the observable quantities $`ϵ_2,ϵ_3`$, that

$`\mathrm{max}(B)`$ $`=`$ $`\left({\displaystyle \frac{3}{2}}\right)^{3/4}{\displaystyle \frac{cH_0}{\sqrt{G}}}\{ϵ_2[{\displaystyle \frac{5}{12}}\mathrm{\Omega }_\mathrm{M}+{\displaystyle \frac{1}{3}}\mathrm{\Omega }_\mathrm{\Lambda }+{\displaystyle \frac{5}{3}}+{\displaystyle \frac{1}{2}}\beta ^2+{\displaystyle \frac{1}{10}}\beta ^4]`$ (14)
$`+ϵ_3[{\displaystyle \frac{1}{7}}({\displaystyle \frac{5}{4}}\mathrm{\Omega }_\mathrm{M}+\mathrm{\Omega }_\mathrm{\Lambda }+5)\beta ^1+{\displaystyle \frac{3}{14}}\beta ^3]\}^{1/2}.`$
This is our main result. Using the limits in Eqs. (3) and (4), we can evaluate max($`B`$), which is plotted in Fig. 1. One of the main features of the plot is that uncertainty in $`ϵ_2`$ and $`ϵ_3`$ from COBE data produces a far greater uncertainty than the uncertainty in the cosmological parameters.

On the largest scales, $`\beta \mathrm{}`$, Eq. (13) simplifies to give

$$\mathrm{max}(B)|_\beta \mathrm{}=\left(\frac{3}{2}\right)^{3/4}\frac{cH_0}{\sqrt{G}}\left\{\frac{5}{12}\mathrm{\Omega }_\mathrm{M}+\frac{1}{3}\mathrm{\Omega }_\mathrm{\Lambda }+\frac{5}{3}\right\}^{1/2}ϵ_210^6\mathrm{G}.$$
(15)
### 3.2 Spatially homogeneous universe

The upper limit on $`B_0`$ on the largest scales in the general case of an inhomogeneous universe, as given by Eq. (15), is much weaker than the limit that can be imposed if we assume that the universe is spatially homogeneous to first order. Homogeneity implies that we can set to zero the $`ϵ`$’s that involve gradients, as we did in deriving Eq. (15).555Note that homogeneous radiation multipoles, i.e. $`\mathrm{D}_a\tau _A_{\mathrm{}}=0`$, imply a Bianchi spacetime to first order . However, it is not only the radiation multipoles that are homogeneous to first order, but the whole spacetime, leading to a Bianchi model. The special dynamics of Bianchi models then leads to a tighter constraint on $`B_0`$. A similar situation arises when deriving limits on the shear $`\sigma _{ab}`$ .

It follows from  that the spatial 3-curvature vanishes to first order, $`_{ab}==0`$. In addition the shear becomes, from Eq. (27),

$$\sigma _{ab}=\dot{\tau }_{ab}.$$
(16)
Thus the shear evolution equation becomes, using Eq. (38),

$$\mathrm{\Pi }_{ab}=\ddot{\tau }_{ab}+\mathrm{\Theta }\dot{\tau }_{ab}+\frac{8}{15}\mu \tau _{ab}.$$
(17)
The magnetic field acts as a forcing term for the quadrupole. The particular solution associated with this forcing term is

$$\mathrm{\Pi }_{ab}=\frac{8}{15}\mu \tau _{ab},$$
(18)
with $`\dot{\tau }_{ab}=0`$ for the particular solution. The solution to the (non-magnetic) homogeneous part oscillates (at frequency $`\sqrt{8\mu /15}`$), while being suppressed with a damping scale of the Hubble time. Thus a conservative upper limit is given by Eq. (18); using Eq. (4) and $`\mathrm{\Omega }_\mathrm{R}2.5h^2\times 10^5\mathrm{\Omega }_\mathrm{M}`$, we find that

$$B_0<6.2_{3.0}^{+1.9}\times 10^9\sqrt{\mathrm{\Omega }_\mathrm{M}}G.$$
(19)
With $`\mathrm{\Omega }_\mathrm{M}=0.3`$, Eq. (19) gives

$$B_0<3.4_{1.6}^{+1.0}\times 10^9G.$$
(20)
This confirms the value found in , and is derived under slightly weaker assumptions; the spacetime is not chosen as a specific exact Bianchi model, but is homogeneous to first order, and turns out to be Bianchi I if we start with a flat Friedmann background. Furthermore, we include both the radiation energy density and the cosmological constant. In the set of Bianchi models which admit a pure magnetic field (types I, II, III, IVo, VIIo), they are all of the same genericity; therefore we may consider this more general than , where the geometry is assumed to be type VIIh.

## 4 Conclusions

For large-scale magnetic fields in an inhomogeneous almost-Friedmann universe, we have found upper limits on the field strength directly in terms of the CMB temperature multipoles and their derivatives, as given by Eqs. (13) and (14). On super-Hubble scales, this upper limit is very weak:

$$B_0\begin{array}{c}<\hfill \\ \hfill \end{array}2\times 10^6\mathrm{G}$$

for the concordance model, as shown by Eq. (15) and Fig. 1.

When the almost-Friedmann universe is assumed to be homogeneous to first order, i.e. a Bianchi spacetime, the upper limit is much stricter, as given by Eq. (19). This generalizes the result of , by including a cosmological constant and removing initial assumptions of a choice of model.

These limits have been derived in a covariant and gauge invariant way using the 1+3 formalism. A major feature of our approach is that our limits are largely model-independent, being derived from properties of the Einstein-Boltzmann equations. Our main assumptions are imposed on the $`ϵ`$-quantities that bound the derivatives of radiation multipoles, which are in principle observable but in practice are not measurable.

It is also possible to find limits on the inhomogeneity of the magnetic field, as given by the gradient of the magnetic energy density $`\mathrm{D}_a\rho _\mathrm{B}`$. The result is given in Appendix B by Eq. (51).

CAC was supported by NSERC (at Dalhousie) and NRF (at Cape Town). AAC acknowledges funding from NSERC. RM was supported by PPARC. CGT was supported by PPARC (at Portsmouth) and Sida/NRF (at Cape Town). RM and CGT thank Dalhousie University for hospitality while part of this work was done.

## Appendix A The linearized equations

We assume that CDM and baryons share the same 4-velocity, which coincides with that of the fundamental observers. Also, confining ourselves to times after last scattering, we may treat the magnetized dust and the radiation fluid as independently conserved entities (i.e., $`^bT_{ab}=0=^b𝒯_{ab}`$). Then we arrive at the following linearized evolution equations for the magnetised dust (see )

$`\dot{\rho }_\mathrm{M}+\mathrm{\Theta }\rho _\mathrm{M}`$ $`=`$ $`0,`$ (21)
$`\rho _\mathrm{M}A_a+{\displaystyle \frac{1}{3}}\mathrm{D}_a\rho _\mathrm{B}+\mathrm{𝖽𝗂𝗏}\mathrm{\Pi }_a`$ $`=`$ $`0,`$ (22)
$`\dot{\rho }_\mathrm{B}+{\displaystyle \frac{4}{3}}\mathrm{\Theta }\rho _\mathrm{B}`$ $`=`$ $`0,`$ (23)
$`\dot{\mathrm{\Pi }}_{ab}+{\displaystyle \frac{4}{3}}\mathrm{\Theta }\mathrm{\Pi }_{ab}`$ $`=`$ $`0,`$ (24)
and

$`\dot{\mu }+{\displaystyle \frac{4}{3}}\mathrm{\Theta }\mu +\mathrm{𝖽𝗂𝗏}q`$ $`=`$ $`0,`$ (25)
$`\dot{q}_a+{\displaystyle \frac{4}{3}}\mathrm{\Theta }q_a+{\displaystyle \frac{4}{3}}\mu A_a+{\displaystyle \frac{1}{3}}\mathrm{D}_a\mu +\mathrm{𝖽𝗂𝗏}\pi _a`$ $`=`$ $`0,`$ (26)
$`\dot{\pi }_{ab}+{\displaystyle \frac{4}{3}}\mathrm{\Theta }\pi _{ab}+{\displaystyle \frac{8}{15}}\mu \sigma _{ab}+2\mathrm{D}_aq_b+\mathrm{𝖽𝗂𝗏}\xi _{ab}`$ $`=`$ $`0,`$ (27)
for the photons (see ). Note that in deriving Eq. (22) we have used the linear relation $`\epsilon _{abc}B^b\mathrm{𝖼𝗎𝗋𝗅}B^c=\frac{1}{6}\mathrm{D}_aB^2+\mathrm{D}^b\mathrm{\Pi }_{ab}`$ (recall that $`\mathrm{D}^aB_a=0`$). To first order, the kinematic evolution is given by

$`\dot{\mathrm{\Theta }}+{\displaystyle \frac{1}{3}}\mathrm{\Theta }^2+{\displaystyle \frac{1}{2}}(\rho _\mathrm{M}+2\mu +2\rho _\mathrm{B})\mathrm{𝖽𝗂𝗏}A\mathrm{\Lambda }`$ $`=`$ $`0,`$ (28)
$`\dot{\sigma }_{ab}+{\displaystyle \frac{2}{3}}\mathrm{\Theta }\sigma _{ab}+E_{ab}{\displaystyle \frac{1}{2}}\pi _{ab}{\displaystyle \frac{1}{2}}\mathrm{\Pi }_{ab}\mathrm{D}_aA_b`$ $`=`$ $`0,`$ (29)
$`\dot{\omega }_a+{\displaystyle \frac{2}{3}}\mathrm{\Theta }\omega _a+{\displaystyle \frac{1}{2}}\mathrm{𝖼𝗎𝗋𝗅}A_a`$ $`=`$ $`0,`$ (30)
$`q_a{\displaystyle \frac{2}{3}}\mathrm{D}_a\mathrm{\Theta }+\mathrm{𝖽𝗂𝗏}\sigma _a\mathrm{𝖼𝗎𝗋𝗅}\omega _a`$ $`=`$ $`0,`$ (31)
$`\mathrm{𝖽𝗂𝗏}\omega `$ $`=`$ $`0,`$ (32)
where $`A_a`$ is given by Eq. (22). Finally, the spacetime geometry is determined by

$`\dot{E}_{ab}+\mathrm{\Theta }E_{ab}\mathrm{𝖼𝗎𝗋𝗅}H_{ab}+{\displaystyle \frac{1}{2}}(\rho _\mathrm{M}+{\displaystyle \frac{4}{3}}\mu )\sigma _{ab}+`$
$`{\displaystyle \frac{1}{2}}\dot{\pi }_{ab}+{\displaystyle \frac{1}{6}}\mathrm{\Theta }\pi _{ab}{\displaystyle \frac{1}{2}}\mathrm{\Theta }\mathrm{\Pi }_{ab}+{\displaystyle \frac{1}{2}}\mathrm{D}_aq_b=0,`$ (33)
$`\dot{H}_{ab}+\mathrm{\Theta }H_{ab}+\mathrm{𝖼𝗎𝗋𝗅}E_{ab}{\displaystyle \frac{1}{2}}\mathrm{𝖼𝗎𝗋𝗅}\pi _{ab}{\displaystyle \frac{1}{2}}\mathrm{𝖼𝗎𝗋𝗅}\mathrm{\Pi }_{ab}=0,`$ (34)
$`H_{ab}\mathrm{𝖼𝗎𝗋𝗅}\sigma _{ab}\mathrm{D}_a\omega _b=0,`$ (35)
$`\mathrm{𝖽𝗂𝗏}E_a+{\displaystyle \frac{1}{2}}\mathrm{𝖽𝗂𝗏}\pi _a+{\displaystyle \frac{1}{2}}\mathrm{𝖽𝗂𝗏}\mathrm{\Pi }_a{\displaystyle \frac{1}{3}}\mathrm{D}_a(\rho _\mathrm{M}+\mu +\rho _\mathrm{B})+{\displaystyle \frac{1}{3}}\mathrm{\Theta }q_a=0,`$ (36)
$`\mathrm{𝖽𝗂𝗏}H_a+{\displaystyle \frac{1}{2}}\mathrm{𝖼𝗎𝗋𝗅}q_a(\rho _\mathrm{M}+{\displaystyle \frac{4}{3}}\mu )\omega _a=0,`$ (37)
$`_{ab}+{\displaystyle \frac{1}{3}}\mathrm{\Theta }\sigma _{ab}{\displaystyle \frac{1}{2}}\pi _{ab}{\displaystyle \frac{1}{2}}\mathrm{\Pi }_{ab}E_{ab}=0,`$ (38)
$`2(\rho _\mathrm{M}+\mu +\rho _\mathrm{B})+{\displaystyle \frac{2}{3}}\mathrm{\Theta }^22\mathrm{\Lambda }=0,`$ (39)
where $`_{ab}`$ and $``$ are respectively the projected Ricci tensor and Ricci scalar. To proceed further we now assume that the fluid flow remains geodesic (i.e. $`A_a=0`$) despite the magnetic presence. In other words, we impose the force-free condition on the magnetic field (i.e. $`\epsilon _{abc}B^b\mathrm{curl}B^c=0=\frac{1}{3}\mathrm{D}_a\rho _\mathrm{B}+\mathrm{𝖽𝗂𝗏}\mathrm{\Pi }_a`$).

## Appendix B Calculating the limits

Our method provides a small refinement of , allowing us to get slightly stronger limits (by about a factor of about two). In , limits on $`\sigma _{ab}`$ were calculated in the following way: First, Eq. (27) is solved for $`\sigma _{ab}`$, and then the separate limits in Eqs.(7)–(22) of  were inserted to give the following limit:

$$\frac{|\sigma _{ab}|}{\mathrm{\Theta }}<\frac{8}{3}ϵ_2+ϵ_2^{}+5ϵ_1^{}+\frac{9}{7}ϵ_3^{}.$$
(40)
However, if, after solving Eq. (27) for $`\sigma _{ab}`$, we use Eq. (41) of  to convert $`\pi _{ab}\tau _{ab}`$ etc. (i.e., $`\tau _a3q_a/4\mu `$, $`\tau _{ab}15\pi _{ab}/8\mu `$…), and then use Eqs. (1)–(4) of  (after expanding all derivatives, and using the relevant evolution equations), some terms cancel, and we get the tighter limit:

$$\frac{|\sigma _{ab}|}{\mathrm{\Theta }}<ϵ_2^{}+5ϵ_1^{}+\frac{9}{7}ϵ_3^{}.$$
(41)
This gives simpler limits than using the method in . As a further example, consider the limits on $`E_{ab}`$ in the case of no magnetic field (including cosmological constant):

$$\frac{|E_{ab}|}{\mathrm{\Theta }}<H\left\{10ϵ_1^{}+15ϵ_1^{}+2ϵ_2^{}+3ϵ_2^{}+\frac{18}{7}ϵ_3^{}+\frac{27}{7}ϵ_3^{}\right\}+\frac{4}{15}H\mathrm{\Omega }_\mathrm{R}ϵ_2,$$
(42)
which is less than the corresponding limit in Eq. (28), .

### B.1 Magnetic field strength

Our first problem is to find limits on $`\mathrm{\Pi }_{ab}`$. In the absence of magnetic fields, limits on $`E_{ab}`$ may be found directly from Eq. (29), using Eq. (27). However, with magnetic fields present, this will give limits on the combination $`|E_{ab}\frac{1}{2}\mathrm{\Pi }_{ab}|`$, so we have to find separate equations for $`E_{ab}`$ and $`\mathrm{\Pi }_{ab}`$. We can do this by solving Eq. (33)and the time derivative of Eq. (29), which gives

$`\mathrm{\Pi }_{ab}`$ $`=`$ $`{\displaystyle \frac{3}{2\mathrm{\Theta }}}\ddot{\sigma }_{ab}{\displaystyle \frac{5}{2}}\dot{\sigma }_{ab}+\mathrm{\Theta }\sigma _{ab}\left({\displaystyle \frac{2}{3}}+2{\displaystyle \frac{\mu }{\mathrm{\Theta }^2}}+{\displaystyle \frac{5}{4}}{\displaystyle \frac{\rho _\mathrm{M}}{\mathrm{\Theta }^2}}+2{\displaystyle \frac{\rho _\mathrm{B}}{\mathrm{\Theta }^2}}{\displaystyle \frac{\mathrm{\Lambda }}{\mathrm{\Theta }^2}}\right)`$ (43)
$`+{\displaystyle \frac{3}{2\mathrm{\Theta }}}\dot{\pi }_{ab}+\pi _{ab}+{\displaystyle \frac{3}{4\mathrm{\Theta }}}\mathrm{D}_aq_b{\displaystyle \frac{3}{2\mathrm{\Theta }}}\mathrm{𝖼𝗎𝗋𝗅}H_{ab},`$
with a similar equation for $`E_{ab}`$. We have used Eq. (24). In the linear regime, we can drop the angled brackets on time derivatives of PSTF tensors. Decoupling these quantities has introduced extra uncertainty into our equations, in the form of $`\ddot{\sigma }_{ab}`$. In Eq. (43), all the shear terms may be found in terms of the $`\tau _A_{\mathrm{}}`$ simply by taking appropriate derivatives of Eq. (27) and using Eqs. (11) and (12), followed by (5). The only term left to worry about is the $`\mathrm{𝖼𝗎𝗋𝗅}H_{ab}`$ term; however, we may use $`\mathrm{D}_c`$ of Eq. (35), given that

$$|\mathrm{D}_cH_{ab}|<|\mathrm{D}_a\mathrm{D}_b\sigma _{cd}|+|\mathrm{D}_a\mathrm{D}_b\omega _c|.$$
(44)
Limits on the second gradient of the shear may be found from Eq. (27):

$$|\mathrm{D}_a\mathrm{D}_b\sigma _{cd}|<\frac{9}{7}H^3\left\{105ϵ_1^{}+14ϵ_2^{}+21ϵ_2^{}+27ϵ_3^{}\right\}.$$
(45)
The rotation term may be found using $`\omega _a=\mathrm{𝖼𝗎𝗋𝗅}\mathrm{D}_a\mu /2\dot{\mu }=\epsilon _{abc}\mathrm{D}^b\mathrm{D}^c\mu /8H\mu `$ and Eq. (26):

$$|\mathrm{D}_a\mathrm{D}_b\omega _c|<\frac{81}{10}H^3\left\{5ϵ_1^{}+5ϵ_1^{}+6ϵ_2^{}\right\}.$$
(46)
So we finally have

$`{\displaystyle \frac{|\mathrm{\Pi }_{ab}|}{\mathrm{\Theta }}}`$ $`<`$ $`H\{{\displaystyle \frac{1}{4}}\mathrm{\Omega }_\mathrm{M}[25ϵ_1^{}+5ϵ_2^{}+{\displaystyle \frac{45}{7}}ϵ_3^{}]`$ (47)
$`+`$ $`\mathrm{\Omega }_\mathrm{R}\left[9ϵ_1^{}+{\displaystyle \frac{8}{15}}ϵ_2+{\displaystyle \frac{6}{5}}ϵ_2^{}+{\displaystyle \frac{18}{7}}ϵ_3^{}\right]+\mathrm{\Omega }_\mathrm{\Lambda }\left[5ϵ_1^{}+ϵ_2^{}+{\displaystyle \frac{9}{7}}ϵ_3^{}\right]`$
$`+`$ $`10ϵ_1^{}+{\displaystyle \frac{75}{2}}ϵ_1^{}+{\displaystyle \frac{45}{2}}ϵ_1^{}+2ϵ_2^{}+{\displaystyle \frac{15}{2}}ϵ_2^{}+{\displaystyle \frac{9}{2}}ϵ_2^{}+{\displaystyle \frac{18}{7}}ϵ_3^{}+{\displaystyle \frac{135}{14}}ϵ_3^{}+{\displaystyle \frac{81}{14}}ϵ_3^{}`$
$`+`$ $`{\displaystyle \frac{117}{4}}ϵ_1^{}+{\displaystyle \frac{27}{4}}ϵ_1^{}+3ϵ_2^{}+{\displaystyle \frac{9}{2}}ϵ_2^{}+{\displaystyle \frac{81}{10}}ϵ_2^{}+{\displaystyle \frac{81}{14}}ϵ_3^{}\};`$
$`{\displaystyle \frac{|E_{ab}|}{\mathrm{\Theta }}}`$ $`<`$ $`H\{{\displaystyle \frac{1}{8}}\mathrm{\Omega }_\mathrm{M}[25ϵ_1^{}+5ϵ_2^{}+{\displaystyle \frac{45}{7}}ϵ_3^{}]+\mathrm{\Omega }_\mathrm{R}[{\displaystyle \frac{9}{2}}ϵ_1^{}+{\displaystyle \frac{3}{5}}ϵ_2^{}+{\displaystyle \frac{9}{7}}ϵ_3^{}]`$ (48)
$`+`$ $`{\displaystyle \frac{1}{2}}\mathrm{\Omega }_\mathrm{\Lambda }\left[5ϵ_1^{}+ϵ_2^{}+{\displaystyle \frac{9}{7}}ϵ_3^{}\right]`$
$`+`$ $`15ϵ_1^{}+{\displaystyle \frac{135}{4}}ϵ_1^{}+{\displaystyle \frac{45}{4}}ϵ_1^{}+3ϵ_2^{}+{\displaystyle \frac{27}{4}}ϵ_2^{}+{\displaystyle \frac{9}{4}}ϵ_2^{}+{\displaystyle \frac{27}{7}}ϵ_3^{}+{\displaystyle \frac{243}{28}}ϵ_3^{}+{\displaystyle \frac{81}{28}}ϵ_3^{}`$
$`+`$ $`{\displaystyle \frac{117}{8}}ϵ_1^{}+{\displaystyle \frac{27}{8}}ϵ_1^{}+{\displaystyle \frac{3}{2}}ϵ_2^{}+{\displaystyle \frac{9}{4}}ϵ_2^{}+{\displaystyle \frac{81}{20}}ϵ_2^{}+{\displaystyle \frac{81}{28}}ϵ_3^{}\}.`$
Comparing Eq. (48) with the limits found in the absence of a magnetic field, Eq. (42), reveals the extra complexity and uncertainty involved in having just one additional field.

### B.2 Inhomogeneity of the field

To find limits on the inhomogeneity, we need to find limits on $`\mathrm{D}_a\rho _\mathrm{B}=3\mathrm{𝖽𝗂𝗏}\mathrm{\Pi }_a`$. \[Note that solving $`\mathrm{D}_a`$ of Eqs. (28) and (36) for $`\mathrm{D}_a\rho _\mathrm{B}`$ does not work since it does not separate gradients of $`\rho _\mathrm{B}`$ and $`\rho _\mathrm{M}`$.\] First we take $`\mathrm{D}^a`$ of Eq. (43), and note that

$$\mathrm{𝖽𝗂𝗏}\mathrm{𝖼𝗎𝗋𝗅}H_a=\frac{1}{2}\mathrm{𝖼𝗎𝗋𝗅}\mathrm{𝖽𝗂𝗏}H_a=\frac{1}{4}\mathrm{𝖼𝗎𝗋𝗅}\mathrm{𝖼𝗎𝗋𝗅}q_a+\frac{1}{2}\left(\rho _\mathrm{M}+\frac{4}{3}\mu \right)\mathrm{𝖼𝗎𝗋𝗅}\omega _a,$$
(49)
so

$$|\mathrm{𝖽𝗂𝗏}\mathrm{𝖼𝗎𝗋𝗅}H_a|<\frac{1}{4}|\mathrm{D}_a\mathrm{D}_bq|+\frac{1}{2}\left(\rho _\mathrm{M}+\frac{4}{3}\mu \right)|\mathrm{D}_a\omega _b|.$$
(50)
Hence we find that

$`{\displaystyle \frac{|\mathrm{D}_a\rho _\mathrm{B}|}{H^3}}`$ $`<`$ $`{\displaystyle \frac{\mathrm{max}|\mathrm{D}_a\rho _\mathrm{B}|}{H^3}}\mathrm{\Omega }_\mathrm{M}\left\{{\displaystyle \frac{2511}{4}}ϵ_1^{}+{\displaystyle \frac{243}{8}}ϵ_1^{}+54ϵ_2^{}+162ϵ_2^{}+{\displaystyle \frac{729}{20}}ϵ_2^{}+{\displaystyle \frac{2187}{14}}ϵ_3^{}\right\}`$ (51)
$`+`$ $`\mathrm{\Omega }_\mathrm{\Lambda }\left\{{\displaystyle \frac{405}{2}}ϵ_1^{}+81ϵ_2^{}+{\displaystyle \frac{243}{2}}ϵ_2^{}+{\displaystyle \frac{729}{14}}ϵ_3^{}\right\}`$
$`+`$ $`\mathrm{\Omega }_\mathrm{R}\left\{972ϵ_1^{}+{\displaystyle \frac{81}{2}}ϵ_1^{}+{\displaystyle \frac{513}{5}}ϵ_2^{}+{\displaystyle \frac{2187}{10}}ϵ_2^{}+{\displaystyle \frac{243}{5}}ϵ_2^{}+{\displaystyle \frac{3645}{14}}ϵ_3^{}\right\}`$
$`+`$ $`{\displaystyle \frac{3645}{2}}ϵ_1^{}+{\displaystyle \frac{8505}{2}}ϵ_1^{}+{\displaystyle \frac{3645}{2}}ϵ_1^{}+54ϵ_2^{}+567ϵ_2^{}+972ϵ_2^{}`$
$`+`$ $`{\displaystyle \frac{729}{2}}ϵ_2^{}+{\displaystyle \frac{6561}{14}}ϵ_3^{}+{\displaystyle \frac{2187}{2}}ϵ_3^{}+{\displaystyle \frac{6561}{14}}ϵ_3^{}.`$


text:
# Nucleon strangeness and spin crisis?

## I. Quark Valence Picture

Given that pions are composed of $`\overline{q}q`$ nonstrange ($`NS`$) quarks and (static) nucleons are composed of $`qqq`$ $`NS`$ quarks $`uud`$ and $`ddu`$, the strangeness-antistrangeness quantum numbers appear when e.g. $`\pi ^{}p\mathrm{\Lambda }K^0`$. The static nonrelativistic quark model then requires the SU(6) valence ($`V`$) values for the axial-vector quark spin component ($`\mathrm{\Delta }qN\left|\overline{q}\gamma _\mu \gamma _5q\right|NS^\mu `$) matrix elements of the nucleon to be

$$\mathrm{\Delta }u_V=\frac{4}{3},\mathrm{\Delta }d_V=\frac{1}{3},\mathrm{\Delta }s_V=0.$$
$`(1)`$
This quark valence picture (1) was first tested using the Sachs form factor for on-shell nucleons $`\mathrm{\Gamma }_\mu =G_E(q^2)P_\mu /m_N+G_M(q^2)r_\mu /4m_N^2`$, where $`P=(p^{}+p)/2`$, $`q=p^{}p`$, $`r_\mu =2\epsilon _{\mu \alpha \beta \gamma }q^\alpha P^\beta \gamma ^\gamma \gamma _5`$ and $`G_M(q^2=0)=\mu _N`$ is the nucleon total magnetic moment. The corresponding proton and neutron magnetic moments expressed in terms of the valence quark spins of (1) are .

$$\mu _p=\mu _u\mathrm{\Delta }u_V+\mu _d\mathrm{\Delta }d_V+\mu _s\mathrm{\Delta }s_V,$$
$`(2a)`$
$$\mu _n=\mu _d\mathrm{\Delta }u_V+\mu _u\mathrm{\Delta }d_V+\mu _s\mathrm{\Delta }s_V,$$
$`(2b)`$
where $`\mu _p`$, $`\mu _n=2.793`$, $`1.913`$ are scaled to nucleon magnetons $`e/2m_N`$ and the corresponding quark magnetons are in the ratio of quark charges and constituent quark masses as

$$\mu _u/\mu _de_u/e_d=2,\mu _s/\mu _d=e_sm_d/e_dm_s\frac{2}{3},$$
$`(2c)`$
because in the latter relation one expects the inverse mass ratio to be $`m_s/m_d1.5`$ . Then substituting the quark valence spin values (1) and the first quark magneton ratio of (2c) into the quark spin versions of the nucleon magnetic moment valence expressions (2a, b), one obtains the predicted ratio .

$$\frac{\mu _p}{\mu _n}=\frac{\left(\frac{\mu _u}{\mu _d}\frac{\mathrm{\Delta }u_V}{\mathrm{\Delta }d_V}\right)+1+0}{\frac{\mathrm{\Delta }u_V}{\mathrm{\Delta }d_V}+\frac{\mu _u}{\mu _d}+0}=\frac{9}{6}=1.50,$$
$`(2d)`$
very close to the observed magnetic moment ratio  $`\mu _p/\mu _n1.460`$.

Also subtracting or adding the nucleon magnetic moment relations (2a,b) leads to quite reasonable values of the nonstrange $`(NS)`$ constituent quark mass ($`m_u=m_d=\widehat{m}`$) when the valence values in (1) are again used:

$$\mu _p\mu _n=(\mu _u\mu _d)(\mathrm{\Delta }u_V\mathrm{\Delta }d_V)4.71(e/2m_N)$$
$`(2e)`$
$$\mu _p+\mu _n=(\mu _u+\mu _d)(\mathrm{\Delta }u_V+\mathrm{\Delta }d_V)+2\mu _s\mathrm{\Delta }s_V0.88(e/2m_N)$$
$`(2f)`$
Equations (2e,f) require $`\widehat{m}332`$ MeV, 356 MeV, respectively. Such an average NS constituent quark mass as 340 MeV can be obtained in many other ways as well  and is compatible with many data sets.

Furthermore, the magnetic moment quark valence expressions of the $`\mathrm{\Sigma }^{+,}`$ baryons in analogy with eqs. (2a,b) for $`\mathrm{\Sigma }^+=uus`$ and $`\mathrm{\Sigma }^{}=dds`$ are

$$\mu _{\mathrm{\Sigma }^+}=\mu _u\mathrm{\Delta }u_V+\mu _s\mathrm{\Delta }d_V+\mu _d\mathrm{\Delta }s_V$$
$`(3a)`$
$$\mu _\mathrm{\Sigma }^{}=\mu _d\mathrm{\Delta }u_V+\mu _s\mathrm{\Delta }d_V+\mu _u\mathrm{\Delta }s_V.$$
$`(3b)`$
Then the measured difference of magnetic moments  $`\mu _{\mathrm{\Sigma }^+}2.458`$, $`\mu _\mathrm{\Sigma }^{}1.160`$ in units of nuclear magnetons combined with the nucleon magnetic moment difference from (2a,b) both computed in the quark valence picture of (1) predicts the magnetic moment ratio

$$\frac{\mu _{\mathrm{\Sigma }^+}\mu _\mathrm{\Sigma }^{}}{\mu _p\mu _n}=\frac{\mathrm{\Delta }u_V\mathrm{\Delta }s_V}{\mathrm{\Delta }u_V\mathrm{\Delta }d_V}=\frac{\frac{4}{3}}{\frac{5}{3}}=0.80.$$
$`(3c)`$
This ratio (3c) is likewise close to the measured ratio 0.77.

It is clear that the above quark valence picture cannot be the whole story, however, because the nonstrange $`\lambda _3`$ isovector difference of quark spins determined by neutron $`\beta `$ decay ,

$$\mathrm{\Delta }u\mathrm{\Delta }d=g_A=1.2670\pm 0.0035,$$
$`(4)`$
is 25% less than the valence value in (1); i.e. $`\mathrm{\Delta }u_V\mathrm{\Delta }d_V=\frac{5}{3}`$. Moreover, the $`\lambda _8`$ component of the nucleon axial-vector current found from the various hyperon semileptonic weak decays

$$\mathrm{\Delta }u+\mathrm{\Delta }d2\mathrm{\Delta }s=g_A\left[\frac{3fd}{f+d}\right]_A0.58$$
$`(5)`$
for the empirically determined  ratio $`(d/f)_A1.74`$ (or equivalently $`(f/d)_A0.58`$), is 40% less than the valence $`\lambda _8`$ prediction $`\mathrm{\Delta }u_V+\mathrm{\Delta }d_V2\mathrm{\Delta }s_V=1`$. However, these more dynamical quark-spin difference SU(3) relations, (4) and (5) have more dynamical significance. Adding and subtracting these quark spin relations (4) and (5) lead to two more (equivalent) quark spin SU(3) relations

$$\mathrm{\Delta }u\mathrm{\Delta }s0.92,\mathrm{\Delta }d\mathrm{\Delta }s0.34.$$
$`(6)`$
For example, the ratio of the first difference in (6) to the $`\lambda _3`$ difference in (4) gives

$$\frac{\mathrm{\Delta }u\mathrm{\Delta }s}{\mathrm{\Delta }u\mathrm{\Delta }d}=\left[\frac{2f}{f+d}\right]_A0.73,$$
$`(7)`$
instead of the ratio in (3c), which in turn predicts the sigma to nucleon magnetic moment difference to be 0.73, also close to the experimental ratio of 0.77 .

However, these more dynamical quark spin differences (4)–(6) do a poor job when combined with the (static) nucleon magnetic moment difference from (2a,b), predicting instead

$$\mu _p\mu _n=(\mu _u\mu _d)(\mathrm{\Delta }u\mathrm{\Delta }d)(e/2m_d)g_A4.71(e/2m_N),$$
$`(8)`$
or a smaller-than-expected constituent quark mass of $`m_d253\text{MeV}`$.

## II. Dynamical QCD Models

To apply these four quark spin difference relations in (4), (5) and (6) to more dynamical problems, one must introduce a (chiral) model to set the overall quark spin scale. In QCD the gluon spin $`\mathrm{\Delta }g`$ must also be accounted for via the helicity sum rule resulting in the spin $`\frac{1}{2}`$ nucleon:

$$s_N=\frac{1}{2}=\frac{1}{2}\mathrm{\Delta }\mathrm{\Sigma }+\mathrm{\Delta }g+\mathrm{\Delta }L_Z,$$
$`(9a)`$
where $`\mathrm{\Delta }L_Z`$ is the orbital angular momentum of the constituent quarks and $`\mathrm{\Delta }\mathrm{\Sigma }=\mathrm{\Delta }u+\mathrm{\Delta }d+\mathrm{\Delta }s`$ is the total quark spin of the nucleon ($`\mathrm{\Delta }\mathrm{\Sigma }_V=1`$ in the valence picture of (1)). The SLAC scaling experiments of 1970  suggest at a 1 GeV scale $`\mathrm{\Delta }L_Z=k_{}r_c1.3`$ for $`k_{}300\text{MeV}`$ and a proton transverse radius of $`r_c0.85\text{fm}`$ (the proton charge radius)111The fact that $`\mathrm{\Delta }g>0`$ (and $`\mathrm{\Delta }L_Z<0`$) is compatible with finding more positive helicity gluons emitted by quarks inside a positive helicity proton.. Then the helicity sum rule (9a) at a 1 GeV scale reduces to

$$\frac{1}{2}\mathrm{\Delta }\mathrm{\Sigma }+\mathrm{\Delta }g1.8.$$
$`(9b)`$
On the other hand , $`\mathrm{\Delta }q\mathrm{\Delta }q(\alpha _s\mathrm{\Delta }g)/2\pi `$ in QCD, but the gluon spin does not affect the SU(3) quark spin difference relations (4)–(6) because $`\mathrm{\Delta }g`$ is flavor-independent. However, $`\mathrm{\Delta }g`$ does enter spin singlet-dependent relations such as the EMC measurement  of the polarized proton structure function integral at $`q^210\text{GeV}^2`$:

$$_0^1𝑑xg_1^p(x)=\frac{1}{2}\left[\frac{4}{9}\mathrm{\Delta }u+\frac{1}{9}\mathrm{\Delta }d+\frac{1}{9}\mathrm{\Delta }s\right]\frac{1}{3}\left(\frac{\alpha _s\mathrm{\Delta }g}{2\pi }\right)0.126.$$
$`(10)`$
Here the combination $`\alpha _s\mathrm{\Delta }g`$ is an approximate renormalization group invariant, as are the quark spins, which we compute at a 1 GeV scale where the reduced helicity sum rule (9b) containing $`\mathrm{\Delta }g`$ is obtained, and it is known  that $`\alpha _s(1\text{GeV}^2)0.50`$. Then substituting $`\mathrm{\Delta }g`$ from (9b) together with $`\alpha _s0.50`$ into the EMC result (10), one obtains a pure quark spin scale (including $`U(3)`$ singlet components)

$$4\mathrm{\Delta }u+\mathrm{\Delta }d+\mathrm{\Delta }s+0.24\mathrm{\Delta }\mathrm{\Sigma }3.13.$$
$`(11)`$
The solution of the quark spin difference relations (4)–(6) together with the EMC-deduced quark spin scale (11) leads to the unique solution

$$\mathrm{\Delta }u=0.87,\mathrm{\Delta }d=0.40,\mathrm{\Delta }s=0.05,\mathrm{\Delta }\mathrm{\Sigma }=0.42.$$
$`(12)`$
Then $`\mathrm{\Delta }\mathrm{\Sigma }=0.42`$ from (12) in turn fixes the gluon spin in the reduced helicity sum rule (9b) to be $`\mathrm{\Delta }g1.59`$ at a renormalization scale of 1 GeV. This latter $`\mathrm{\Delta }g`$ depends only on the $`\mathrm{\Delta }L_Z`$ as modeled from SLAC scaling data together with the less model-dependent SU(3) quark spin difference relations (4)–(6) .

An alternative QCD-dependent determination of the various quark spins follows from exploiting the Bjorken sum rule  as it pertains to QCD beyond leading order . Using the recent EMC  and SMC data  for proton structure functions and SLAC E142 data  for neutron structure functions, the Bjorken sum rule (BSR)

$$_0^1\left[g_1^p(x)g_1^n(x)\right]𝑑x=\frac{1}{6}g_A\left[1\alpha _s(Q^2)/\pi \right]$$
$`(13)`$
is shown to be valid to within 12% . Given this BSR (13), perturbative QCD corrections calculated up to $`𝒪\left[\left(\alpha _s/\pi \right)^3\right]`$ and estimated through $`𝒪\left[\left(\alpha _s/\pi \right)^4\right]`$ lead to the quark spin relations  (including higher twist effects)

$$\begin{array}{cc}\mathrm{\Delta }u=0.85\pm 0.03,\hfill & \mathrm{\Delta }d=0.41\pm 0.03\hfill \\ \mathrm{\Delta }s=0.08\pm 0.03,\hfill & \mathrm{\Delta }\mathrm{\Sigma }=0.37\pm 0.07.\hfill \end{array}$$
$`(14)`$
Also to order $`𝒪\left[\left(\alpha _s/\pi \right)^4\right]`$, ref.  finds $`\alpha _s(2.5\text{GeV}^2)=0.375\stackrel{+0.062}{_{0.081}}`$ (compatible with $`\alpha _s(1\text{GeV}^2)0.50`$ in ref. ), corresponding to $`\alpha _s(M_Z^2)=0.122\pm 0.007`$ as found in the PDG tables  due to averaging data of PEP/PETRA, TRISTAN, LEP, SLC, CLEO.

We stress that the BSR structure (but without the $`\alpha _s`$ QCD factor in (13)) already follows by subtracting the polarized neutron structure function analog of (10) but with $`ud`$ quarks from the proton version (10) along with using the $`\lambda _3`$ isovector difference of quark spins $`\mathrm{\Delta }u\mathrm{\Delta }d=g_A`$ of eq. (4). The flavor-independent gluon spin factor $`\alpha _s\mathrm{\Delta }g`$ in (10) then cancels out in the BSR relation (13), yet the BSR plus the higher order dynamical QCD renormalization scheme “knows” about the second SU(3) $`d/f`$-type of quark spin difference (5) (or (6)) and knows about the singlet-type of helicity sum rule (HSR) (9b) coupled with the EMC proton polarized structure function scale (10) or the (singlet-included) quark spin U(3) scale (11). We draw this conclusion because of the close agreement between the SU(3) quark spin differences (4)–(6) plus the dynamical HSR determination of the EMC measurement (10) leading to the quark spins of eqs. (12). The latter roughly numerically match the dynamically driven QCD analysis of the BSR (13) resulting in the quark spins of eqs. (14).

## III. Dynamical Tadpole Leakage

A third scheme to estimate the quark axial-vector spins $`\mathrm{\Delta }u`$, $`\mathrm{\Delta }d`$, $`\mathrm{\Delta }s`$ which naturally links up to the quark-valence picture of Sec. I is due to axial-vector tadpole graphs. For simplicity we shall label the axial-vector hadronic states $`f_1(1285)`$ and $`f_1(1420)`$ by their early names, $`D`$ and $`E`$ respectively. Then we use the nonstrange $`(NS)`$ and strange $`(S)`$ hadronic axial-vector basis to write

$$|D=\mathrm{cos}\varphi _A|A_{NS}\mathrm{sin}\varphi _A|A_S,|E=\mathrm{sin}\varphi _A|A_{NS}+\mathrm{cos}\varphi _A|A_S,$$
$`(15)`$
where $`|A_{NS}=|\overline{u}u+\overline{d}d/\sqrt{2}`$ and $`|A_S=|\overline{s}s`$ . The axial-vector mixing angle in (15) is determined by the present decay rate ratio — the branching fraction for $`DK\overline{K}\pi `$ is 9% and we take 50% for $`EK\overline{K}\pi `$ since this mode together with $`EK\overline{K}^{}+`$ c.c. are both dominant :

$$\frac{\mathrm{\Gamma }_{DK\overline{K}\pi }}{\mathrm{\Gamma }_{EK\overline{K}\pi }}\mathrm{tan}^2\varphi _A\frac{2.16\text{MeV}}{27.75\text{MeV}}0.078,\varphi _A16^{}.$$
$`(16)`$
Given eqs. (15) and (16), the quark spin $`\mathrm{\Delta }s`$ is found from Fig. 1a as

$$\mathrm{\Delta }s=\left[\frac{1}{m_D^2}\frac{1}{m_E^2}\right]\mathrm{cos}\varphi _A\mathrm{sin}\varphi _A0\left|\overline{s}\gamma _\mu \gamma _5s\right|A_SA_{NS}N|N^\mu .$$
$`(17a)`$
To link up with Sec. I, SU(2) symmetry is assumed conserved at the lower vertex in Fig. 1a so that $`A_{NS}N|N^\mu =1S^\mu `$, where $`S^\mu `$ is the spin 1 polarization four vector, along with $`0\left|\overline{s}\gamma _\mu \gamma _5s\right|A_S=S_\mu m_{A_S}^2`$ (with $`m_{A_S}^2=m_D^2\mathrm{sin}^2\varphi _A+m_E^2\mathrm{cos}^2\varphi _A2\text{GeV}^2)`$. Then the tadpole equation (17a) requires

$$\mathrm{\Delta }s=\left[\frac{1}{m_D^2}\frac{1}{m_E^2}\right]\mathrm{cos}16^{}\mathrm{sin}16^{}m_{A_S}^20.06,$$
$`(17b)`$
since  $`m_D1282\text{MeV}`$ and $`m_E1426\text{MeV}`$.

Encouraged by the proximity of (17b) to our earlier determinations in (12) and in (14) for $`\mathrm{\Delta }s`$, we extend this analysis to the tadpole graph of Fig. 1b in order to estimate the quark spin $`\mathrm{\Delta }u`$ in nucleons, leading to

$$\mathrm{\Delta }u=\left[\frac{\mathrm{cos}^2\varphi _A}{m_D^2}+\frac{\mathrm{sin}^2\varphi _A}{m_E^2}\right]0\left|\overline{u}\gamma _\mu \gamma _5u\right|A_{NS}A_{NS}N|N^\mu .$$
$`(18a)`$
The first two terms in brackets in (18a) sum to 0.6 GeV-2, while the second factor is $`0\left|\overline{u}\gamma _\mu \gamma _5u\right|A_{NS}=\frac{1}{\sqrt{2}}0\left|\overline{u}\gamma _\mu \gamma _5u\right|\overline{u}u`$ and the latter up flavor matrix element is $`0\left|\overline{u}\gamma _u\gamma _5u\right|\overline{u}u=S_\mu 2\text{GeV}^2`$ in the SU(3) conserving limit as above (17b). Then the tadpole version of $`\mathrm{\Delta }u`$ in (18a) becomes

$$\mathrm{\Delta }u0.6\text{GeV}^22\text{GeV}^2/\sqrt{2}0.85,$$
$`(18b)`$
again close to $`\mathrm{\Delta }u`$ in (12) and in (14).

Finally we compute the quark spin $`\mathrm{\Delta }d`$ in this tadpole picture driven again by $`D`$ and $`E`$ spin $`1^+`$ poles. Since they too simulate the axial-vector current, we can invoke the $`\lambda _3`$ axial current quark spin difference relation found from neutron $`\beta `$ decay, $`\mathrm{\Delta }u\mathrm{\Delta }d=g_A`$. This latter relation was used in part to fix the quark spins in (12) and it was also needed to derive the Bjorken sum rule (13) which in turn led to the quark spins in (14). So assuming the tadpole-driven $`\mathrm{\Delta }u0.85`$ in (18b), the tadpole-driven $`\mathrm{\Delta }d`$ is

$$\mathrm{\Delta }d=\mathrm{\Delta }ug_A0.851.27=0.42.$$
$`(19)`$
Collecting the tadpole-driven quark spins of (17b), (18b) and (19), we have

$$\mathrm{\Delta }u0.85,\mathrm{\Delta }d0.42,\mathrm{\Delta }s0.06,\mathrm{\Delta }\mathrm{\Sigma }0.37.$$
$`(20)`$
## IV. Conclusion

We have reviewed the static SU(3) valence picture of the constituent quark model while focusing on nucleon magnetic moments in Sec. I. We slightly modified this picture in Sec. II in the context of QCD dynamical models, first obtaining in eqs. (12) the strangeness and total quark spins due to the helicity sum rule and EMC data

$$\mathrm{\Delta }s=0.05,\mathrm{\Delta }\mathrm{\Sigma }=\mathrm{\Delta }u+\mathrm{\Delta }d+\mathrm{\Delta }s=0.42.$$
$`(21)`$
Also in Sec. II we reviewed the Bjorken sum rule in QCD, resulting in analog quark spins in eqs. (14),

$$\mathrm{\Delta }s=0.08\pm 0.03,\mathrm{\Delta }\mathrm{\Sigma }=0.37\pm 0.07.$$
$`(22)`$
Finally in Sec. III we estimated the tadpole leakage due to $`D`$$`E`$ mixing. This led to eqs. (20) with strangeness and total quark spins

$$\mathrm{\Delta }s0.06,\mathrm{\Delta }\mathrm{\Sigma }0.37.$$
$`(23)`$
The consistent pattern of the above three dynamical schemes giving (21), (22) and (23) makes us question whether such a compatible picture is really a quark spin “crisis”. While it is true that the quark spin $`\mathrm{\Delta }s`$ in (21)–(23) is a nonvanishingly small (and negative) 5%–8% of the valence values in (1), $`\mathrm{\Sigma }_V=1`$, $`\mathrm{\Delta }s_V=0`$, the momentum distribution of strange quarks in nucleons was observed by the Columbia-Chicago-Fermi-Rochester collaboration  to be a similar small 6% fraction. Moreover the SLAC scaling experiments of the 1970s found that the overall momentum distribution was about 50% due to quarks and presumably 50% due to QCD gluons. In like manner, the total quark spin $`\mathrm{\Delta }\mathrm{\Sigma }`$ in (21)–(23) is about 40% and implied gluon spin $`\mathrm{\Delta }g`$ is about 60% of the nucleon spin. Even as a crisis, the above quark spins always form an orderly pattern.

The notion of crisis here asks why the quarks in (nonstrange) nucleons are not all nonstrange and why they do not always carry 100% of the nucleon’s spin, as the quark-valence picture requires. We have suggested in Sec. II that about 6% of the nucleon’s spin (and also its momentum) are due to strange quarks. Moreover, about 40% of the nucleon’s total spin (and also its momentum) are due to quarks, with the other 60% presumably generated by QCD gluons. An analogous picture likewise emerges in Sec. III based on tadpole leakage of quark spins, assuming the (axial-vector) $`D`$ and $`E`$ tadpole propagators couple to nucleons in an SU(3) and spin-conserving manner. In the latter case, the empirical $`D`$$`E`$ mixing can also be understood via OZI-violating quark-annihilation graphs coupling to QCD gluons .

We conclude that in all three of the above quark spin analyses in Secs. II and III QCD glue is needed to resolve the quark strangeness and spin crisis in nucleons. In a similar fashion, one must be cautious when applying these dynamical quark spin differences (4)–(6) to (static) magnetic moment problems such as in eq. (8). This too should not be considered a crisis, but instead is a mixture of dynamical quark spins set in a static quark framework.

Acknowledgement: LB appreciates support from NSF. MDS is grateful for 1997 summer support at TRIUMF.


text:
# Molecular Dynamics in grafted layers of poly(dimethylsiloxane) (PDMS)

## I Introduction

The glass transition and related dynamics of both, polymers DutcherACS99 ; ForrestACIS01 ; ForrestPSITF00 ; DKBuch1102  and low molar mass glass-forming liquids ArndtPRL97 ; HuwePRL99 ; DKBuch602  under the constraint of spatial confinement have been studied extensively by a variety of experimental techniques. The idea of these studies is to prove the existence of a characteristic, temperature dependent length scale $`\xi `$ for the glass transition, i.e. the size of cooperatively rearranging regions as introduced by Adam and Gibbs AdamJCP65 . Thus, the dynamics related to the glass transition is expected to deviate from that of the bulk when the increase of $`\xi `$ is hindered by the confinement.

In case of polymers the confinement can be conveniently realized by preparation of thin films via spin coating, grafting or Langmuir-Blodgett (LB-) techniques. Plenty of experimental investigations has been dedicated to the determination of the glass transition temperature $`T_\mathrm{g}`$ in thin supported or freely standing spin coated films by several techniques since the pioneering ellipsometric experiments by Keddie and co-workers KeddieEPL94 . A good review of this topic is given in ForrestPSITF00 . There are only a few experiments which examine the dynamics related to the glass transition ($`\alpha `$-relaxation) in thin polymer films in addition to a mere determination of $`T_\mathrm{g}`$. Due to its broad frequency and temperature range, dielectric relaxation spectroscopy DKBuch1102 ; BlumADVM95 ; FukaoEPL99 ; FukaoPRE200 ; FukaoPRE301 ; FukaoPRE401 ; HartmannMRC00 ; HartmannEPJE01  has turned out to deliver comprehensive information on the changes of the $`\alpha `$-relaxation but also of secondary relaxations FukaoPRE401  when the film thickness is reduced. For the investigation of finite size effects in thin polymer films it is up to now the only technique which probes directly molecular fluctuations. Since the capacitance as measurand can be tailored by variation of the dimensions of the sample capacitor, dielectric spectroscopy does not suffer sensitivity losses when it is applied to thin polymer films. In some cases dielectric relaxation spectroscopy can be combined with thermal expansion spectroscopy FukaoPRE301  to extend the accessible frequency range. Moreover, second harmonic generation reveals a broadening of the relaxation time distribution in thin supported polymer films HallMM97 . Photon correlation spectroscopy indicates a reduction of the $`\alpha `$-relaxation time in thin freely standing films of polystyrene ForrestPRE98 .

All these studies have revealed deviations of $`T_\mathrm{g}`$ in thin films from the bulk value. However, the sign and the amount of these deviations depend strongly on the interaction with the underlying substrate GrohensLMR98 ; FryerMM00  as it is consistently found for small molecules in untreated pores GorbatschowEPL96 . Thus, the conclusion from the observed shifts of $`T_\mathrm{g}`$ to the existence of $`\xi `$ and the estimation of its value can be done unambiguously only in case of freely standing polymer films for molecular weights which are sufficiently small to exclude effects of chain confinement MattsonPRE00 . Moreover, it was emphasized recently ReiterEPJE01  that spin coated films have to be considered as a highly metastable form of matter and it was argued in particular, if alterations of $`T_\mathrm{g}`$ can be related to metastable states of spin coated films. This conjecture suggests to measure the glass transition temperature or to investigate the dynamics in thin polymer films prepared by other techniques than spin coating such as grafted films or LB-films. Publications concerning this point are sparse. Optical waveguide spectroscopy yields an identical decrease of $`T_\mathrm{g}`$ for thin films of poly(methyl methacrylate) prepared by spin coating, grafting and by the LB-technique, respectively PruckerMMCP98 . For grafted films of hydroxy terminated polystyrene and poly(4-hydroxystyrene) increases of $`T_\mathrm{g}`$ of 50 K for a film thickness of 100 nm are reported FryerJCP01 .

In the limit of high molecular weights for freely standing films an additional ”sliding motion” of the polymer chains along their own contour was proposed which leads to an increased chain mobility and hence to a reduction of $`T_\mathrm{g}`$ deGennesEPJE00 . For thin polymer films the shift of $`T_\mathrm{g}`$ is considered as indication of an underlying distribution of glass transition temperatures, $`T_\mathrm{g}(d)`$. This distribution is described by models which assume the film to be composed of layers whose mobility is enhanced, reduced or equal to that of the bulk. Dielectric experiments allow to determine the thickness of these layers in thin supported films FukaoPRE200 . Moreover, they reveal that the distribution $`T_\mathrm{g}(d)`$ in thin films is associated with an increase of the width of the $`\alpha `$-relaxation, a reduction of its dielectric strength and a shift of its relaxation rate.

In this paper, we use dielectric relaxation spectroscopy to investigate the dynamics in thin grafted films of PDMS and to prove, if effects known from supported spincoated films hold as well for films obtained by different preparation techniques. The range of film thicknesses covers values above and below the radius of gyration. Evaluation of the isochronal dielectric loss allows to determine the relaxation rates of the $`\alpha `$\- and the cold crystallization ($`\alpha _\mathrm{c}`$-relaxation), respectively. While the former is related to the glass transition of amorphous PDMS, the latter originates from the amorphous fraction after a partial crystallization has occurred. Thus, from temperature dependence of relaxation rates the Vogel temperature and the thermal expansion coefficient of free volume are obtained for films of various film thickness and for the bulk material.

## II Experimental

Bulk properties of poly(dimethylsiloxane) (PDMS), such as the glass transition temperatures, the relaxation processes and their dependence on thermal history have been studied extensively ClarsonPolym85 ; ClarsonPolym96 ; KirstCPS94 ; AdachiJPS79 . The preparation of end-grafted layers of PDMS and the characterization of their structure by small-angle neutron scattering is reported in previous publications AuroyMM90 ; AuroyPRL91 ; AuroyMM91 ; LegerAPS99 ; MarzolinMM01 . In order to form dense end-grafted layers, at first the aluminium surface of the electrodes has to be chemically modified to prevent the adsorption of monomers while still keeping the possibility of end-grafting. This modification is accomplished by vapor deposition of a chemically attached monolayer of short PDMS oligomers (four SiO units) which is terminated by a SiH group. This modified surface is subsequently incubated with a melt of mono vinyl end terminated PDMS at 120 0C in presence of platinum as a catalyst. The melt is a mixture of long and short PDMS chains (see Tab. 1) where the latter serve to prevent adsorption of the long chains. Finally, the grafting of the PDMS chains is achieved by a hydrosililation reaction between the vinyl end groups and the SiH groups of the monolayer. Thus, the long chains are end attached, but not adsorbed. The grafting density in this procedure is controlled by the concentration of long chains in the mixture LegerAPS99 . Chains that have not reacted are rinsed away by toluene, subsequently the layers were dried. Prior to evaporation of the upper electrodes, the samples have been stored at room temperature for one day in the vacuum system of the evaporation source. Cast films from a solution of the polymer in toluene with a thickness of some ten microns were prepared in order to compare the dynamic behaviour of bulk PDMS to that of the grafted polymer. The solution cast films were dried at ambient temperature in a vacuum system prior to dielectric measurements.

The thickness ($`d_{\mathrm{diel}})`$ of the grafted samples has been determined from the capacitance of the sample condenser at the lowest temperature of 120 K and at a frequency of the electric field of 105 Hz. The value for the real part $`\epsilon ^{}`$ of the dielectric function required for this thickness determination was obtained from measurements on PDMS bulk samples of a known sample geometry. For some samples the thickness has been measured independently by ellipsometry ($`d_{\mathrm{ellip}}`$) on dried grafted layers. However, the accuracy of this technique is limited because of the small difference in the refractive indices of PDMS and the substrate. The knowledge of the thickness of grafted layers allows to estimate the grafting density $`\sigma `$ and the distance $`b`$ between grafting sites by use of relations derived previously AuroyMM91 . Values of characteristic quantities of grafted samples are given in Table 1.

Please insert Table 1

Measurements of the dielectric loss $`\epsilon ^{^{\prime \prime }}`$ were performed in the frequency range from $`110^1`$ Hz to $`10^7`$ Hz at temperatures between 120 K and ambient temperature. A Solartron-Schlumberger frequency response analyzer FRA 1260 with a Novocontrol active sample cell BDC-S was used. Further details on the application of dielectric spectroscopy to study the dynamics in thin polymer films and on the experimental setup can be found elsewhere FukaoPRE301 ; HartmannEPJE01 . In the isothermal representation of dielectric loss an artifact occurs at high frequencies ($`\nu 510^4`$ Hz) due to the finite resistance of electrodes BlumADVM95 .

Since PDMS is known for its tendency to crystallize, the first measurement on each PDMS sample consisted in recording the dielectric spectra at constant temperatures after the sample has been quenched in liquid nitrogen and subsequently stored for 30 min at 120 K. The cooling rate of $``$50 K min-1 obtained during the quenching procedure is known to be sufficient to avoid crystallization in bulk samples of PDMS KirstCPS94 ; AdachiJPS79 . Therefore, this procedure should allow to monitor the $`\alpha `$-relaxation in the amorphous polymer. For some samples dielectric spectra were subsequently recorded during a slow cooling of the sample.

## III Results and Discussion

Figure 1(a) displays the dielectric loss at $`T`$=153 K and $`T`$= 146 K, respectively as obtained for the bulk and for thin films of $`d`$=41 nm ($`d>R_\mathrm{g}`$) and $`d`$=11 nm ($`d<R_\mathrm{g}`$) of PDMS ($`M_\mathrm{w}`$=170000 g mol-1). Spectra were taken during a heating run of samples which were at first quenched in liquid nitrogen. Additionally, for $`d`$=41 nm data are shown which were taken during a slow cooling of the sample. The lines in Fig. 1(a) represent fits according to the equation of Havriliak and Negami HavNeg67  (HN-equation):

$$\epsilon ^{^{\prime \prime }}(\omega ;T=const.)=\frac{\sigma _0}{\epsilon _0}\frac{a}{\omega ^s}\mathrm{Im}\left[\frac{\mathrm{\Delta }\epsilon }{(1+(i\omega \tau )^\alpha )^\gamma }\right].$$
(1)
In this notation, $`\mathrm{\Delta }\epsilon `$ is the dielectric strength and $`\sigma _0`$ the DC conductivity. $`\alpha `$ and $`\gamma `$ describe the symmetric and asymmetric broadening of the relaxation peak. The exponent $`s`$ equals one for Ohmic behavior, deviations ($`s<1`$) are caused by electrode polarization. $`a`$ is a factor having the dimension $`[\mathrm{s}]^{(1s)}`$. In Fig. 1(a) at high frequencies an artifact is observed which is treated in the fits as the low frequency wing of a relaxation process.

Please insert Figure 1

Figure 1(a) reveals that in case of quenched samples the $`\alpha `$-relaxation of the amorphous PDMS in a film of 41 nm thickness (i.e. a film thickness above the radius of gyration) resembles the $`\alpha `$-relaxation in the bulk with respect to the dielectric strength $`\mathrm{\Delta }\epsilon `$, the shape of loss peak and its width. However, its maximum position is shifted by about one decade to lower frequencies with respect to the bulk data. The comparison of the loss peaks of grafted PDMS ($`d`$=41 nm) recorded during a heating run after quenching the sample and during a cooling run shows that in case of the latter the loss peak is again shifted to lower frequencies and that its dielectric strength has decreased. These findings are due to a partial crystallization of PDMS during the slow cooling which immobilizes a part of dipoles in crystalline regions and restricts the mobility of those which still contribute to the $`\alpha `$-relaxation. The loss peak corresponding to the $`\alpha `$-relaxation in a grafted PDMS-film with a thickness of $`d`$=11 nm (i.e. $`d<R_\mathrm{g}`$) clearly differs from that of the thicker film. Fits according to Eq. (1) reveal that its maximum is shifted to higher frequencies by more than 1 decade, the dielectric strength is reduced and its width is increased with respect to the bulk and the thicker film. However, the analysis of isothermal data as shown in Fig. 1(a) suffers, in particular for thin films, from the drawback that the relaxation processes can be traced only in a limited temperature range due to restrictions given by the conductivity at low frequencies and the artifact process at high frequencies, respectively. Therefore, the analysis has been extended by use of the isochronal representation of dielectric loss, i.e. its representation versus temperature at constant frequencies (Fig. 1(b)) FukaoEPL99 . Hence, the dielectric loss can be described as a superposition of up to three Gaussian functions and a term taking account of the conductivity. The latter is obtained from the conductivity contribution in Eq. 1 under the following assumptions: (i) the temperature dependence of the DC-conductivity $`\sigma _0`$ obeys the Vogel-Fulcher-Tammann(VFT)-equation (Eq. 3) and (ii) the exponent $`\mathrm{s}`$ depends linearly on temperature. Thus, the dielectric loss in the isochronal representation can be described by:

$$\epsilon ^{^{\prime \prime }}(T;\omega =const.)=\underset{i=1}{\overset{3}{}}a_\mathrm{i}\mathrm{exp}\left(\frac{(TT_\mathrm{i}^{\mathrm{max}})^2}{w_\mathrm{i}}\right)+\frac{\sigma _{\mathrm{}}}{\epsilon _0\omega ^{(\mathrm{m}\mathrm{T}+\mathrm{n})}}\mathrm{exp}\left(\frac{B}{TT_0}\right)+\lambda ,$$
(2)
where $`a_\mathrm{i}`$ and $`T_\mathrm{i}^{\mathrm{max}}`$ denote the amplitude and the maximum position of the Gaussian functions. $`w_\mathrm{i}`$ corresponds to the width of peak when it has decreased to $`1/e`$ of its maximum. $`\sigma _{\mathrm{}}`$, $`B`$ and $`T_0`$ are the parameters describing the VFT-dependence of the conductivity, $`m`$ and $`n`$ are used to describe the linear dependence of the exponent $`\mathrm{s}`$ on the temperature, $`\omega =2\pi \nu `$ is the angular frequency of the electric field and $`\lambda `$ is an offset. Note that Eq. (2) is used only to obtain the maximum position of peaks and hence the activation plot (Fig. 2, $`\tau =1/(2\pi \nu )`$). The results of both fitting procedures coincide at temperatures for which an analysis according to Eq. 1 is possible.

Examples for fits according to Eq. (2) are given in Fig. 1(b) as obtained for the same data sets of quenched samples as in Fig. 1(a) at a frequency of 0.55 Hz. The inset exemplifies the decomposition of the fit into three peaks and the conductivity contribution for the grafted film of $`d`$=11 nm. For the quenched bulk sample the isochronal representation of dielectric loss $`\epsilon ^{^{\prime \prime }}`$ is characterized by two relaxation processes: a symmetric and narrow peak corresponding to the $`\alpha `$-relaxation of the amorphous PDMS and a peak corresponding to the $`\alpha `$-relaxation of the amorphous fraction in the partial crystalline sample ($`\alpha _\mathrm{c}`$-relaxation) which rises above the crystallization temperature of 162 K. The increase at high temperatures for a frequency of 0.55 Hz is due to the conductivity. This situation holds also for the grafted film with a thickness of 41 nm being larger than $`R_\mathrm{g}`$ of the polymer. In contrast, for the film with $`d`$=11 nm, the two processes are no longer well separated in temperature, but the $`\alpha _\mathrm{c}`$-relaxation appears as shoulder of the $`\alpha `$-relaxation. The latter is broadened also in the isochronal representation with respect to the $`\alpha `$-process in the bulk. Consistently to Fig. 1(a), in the isochronal representation the $`\alpha `$-relaxation in the grafted film of a thickness of 11 nm is reduced in the maximum of dielectric loss and it is shifted to lower temperatures with respect to the bulk.

For the samples E, F and G at high temperatures an additional relaxation process is observed. It is assigned to segmental fluctuations of low molecular weight PDMS chains ($`M_\mathrm{w}`$=5000 g mol-1) which are used in the preparation to decouple the high molecular weight polymers from the surface of the substrate. Compared to any relaxation process in bulk PDMS this relaxation is by orders of magnitude slowed down presumably due to adhesion to the surface. The question why such a process is not observed in sample D with $`d>R_\mathrm{g}`$ and a grafting density of $`\sigma `$=0.14 remains open and requires further studies in dependence on the grafting density. It fits to the interpretation given above that this segmental fluctuation depends strongly on the thermal history of the sample.

Please insert Figure 2

Figure 2 displays the activation plot obtained from fits in the isochronal representation for both molecular weights under study ((a) $`M_\mathrm{w}`$=170000 g mol-1, (b) ($`M_\mathrm{w}`$=96000 g mol-1) and for different thermal histories of samples as described above. For each molecular weight data for the three relaxation processes introduced above are shown: the $`\alpha `$-relaxation, the $`\alpha _\mathrm{c}`$-relaxation and a process related to the dynamics in the interface layer of low molar weight PDMS. Solid lines in Fig. 2 are fits according to the VFT-equation:

$$\mathrm{log}(1/\tau )=\mathrm{log}(1/\tau _{\mathrm{}})\frac{B}{TT_0},$$
(3)
where $`\tau _{\mathrm{}}`$ denotes the relaxation time at high temperatures, $`B`$ is related to the expansion coefficient of free volume, $`\alpha _\mathrm{f}`$, via $`\alpha _\mathrm{f}=B^1`$ and $`T_0`$ is the Vogel temperature.

The main result in Fig. 2 is a shift of the $`\alpha `$-relaxation to shorter relaxation rates $`\tau `$ for films with a thickness distinctly smaller than the radius of gyration. Independent of the sample thickness, the $`\alpha `$-relaxation is slightly slowed down in samples which were cooled slowly compared to samples which were quenched prior to a heating run. However, this effect due to a different thermal history is small in comparison to the shift of $`\tau `$ when the film thickness is reduced to values below $`R_\mathrm{g}`$ of the polymer. In contrast to these findings, the $`\alpha `$-relaxation in the film with $`d=41\mathrm{nm}>R_\mathrm{g}`$ is slowed down with respect to the bulk (open and full circles in Fig. 2(a)). This effect is even more pronounced when the sample is cooled slowly. The $`\alpha _\mathrm{c}`$-relaxation shows no dependence on the film thickness which could be separated from influence of thermal history of the samples. Thus, the results indicate that for films in the regime of chain confinement (i.e. $`d<R_\mathrm{g}`$) the $`\alpha `$-relaxation is distinctly faster than in the bulk, whereas for films with $`d>R_\mathrm{g}`$ the dynamics resembles well to that in the bulk. The observed slowing down of the $`\alpha `$-relaxation in thick films is attributed to interactions with the electrode which prevail the confinement effect at this film thickness. In films with $`d>R_\mathrm{g}`$, the transition between the $`\alpha `$\- and $`\alpha _\mathrm{c}`$-relaxation occurs, as in the bulk, at a well defined temperature ($`T162`$ K), whereas no such sharp transition can be found in films with thicknesses below $`R_\mathrm{g}`$. In these films the $`\alpha _\mathrm{c}`$-relaxation appears as a shoulder of the $`\alpha `$-relaxation whose maximum is poorly defined. Thus, it can be only stated that the transition temperature between the $`\alpha `$\- and $`\alpha _\mathrm{c}`$-relaxation is the same for all films with an uncertainty of $`\pm 5K`$.

Please insert Figure 3

Figure 3 displays the dielectric strength $`\mathrm{\Delta }\epsilon `$ as obtained from fits of Eq. 1 to isothermal data. For quenched bulk samples, $`\mathrm{\Delta }\epsilon `$ of the $`\alpha `$-relaxation is characterized by a gradual decrease when the temperature approaches the phase transition at 162 K from below. Due to partial crystallization, $`\mathrm{\Delta }\epsilon `$ of the $`\alpha _\mathrm{c}`$-relaxation is notedly reduced with respect to the $`\alpha `$-relaxation. For bulk samples which were cooled slowly, the temperature dependence of $`\mathrm{\Delta }\epsilon `$ is given by a steady decrease when the temperature is lowered. The same situation as in the bulk is found for the grafted film of 41 nm thickness with the only difference that $`\mathrm{\Delta }\epsilon `$ of the $`\alpha _\mathrm{c}`$-relaxation increases with increasing temperature after the sample has been quenched. Here, the determination of $`\mathrm{\Delta }\epsilon `$ is complicated due to the separation of the high frequency artifact especially at the highest temperatures.

In thin films with a thickness smaller than $`R_\mathrm{g}`$ of the polymer a reduction of the dielectric loss $`\epsilon ^{^{\prime \prime }}`$ has been detected as shown in Fig. 1(a). This leads to a decrease of $`\mathrm{\Delta }\epsilon `$ of the $`\alpha `$-relaxation by about 50% to 60%. The dielectric strength of the $`\alpha _\mathrm{c}`$-relaxation can not be determined from HN-fits according to Eq. (1) since this process is too weak and appears only as a shoulder of the $`\alpha `$-relaxation in isochronal representation of dielectric loss (Fig. 1(b)). The decrease of $`\mathrm{\Delta }\epsilon `$ occurs also in grafted layers after they were quenched ruling out crystallization as the cause for this reduction. It is instead assumed that the reduction of the dielectric strength of the $`\alpha `$-relaxation in films with $`d<R_\mathrm{g}`$ is due to a restriction of cooperative fluctuations or a partial immobilization of dipoles in interfaces near the electrodes FukaoPRE301 ; HartmannEPJE01 .

Please insert Figure 4

Figure 4 displays the dependence of the Vogel temperature $`T_0`$ and of the thermal expansion coefficient of free volume, $`\alpha _\mathrm{f}=1/B`$ as obtained from fits of Eq. 3 to the temperature dependence of the relaxation time $`\tau `$. For the fits $`\tau _{\mathrm{}}`$ was fixed to the value obtained from bulk measurements ($`log(\tau _{\mathrm{}})=14.5`$). Thus, only $`B`$ and $`T_0`$ were adjusted to reproduce the observed values FukaoPRE301 . Alternatively, fits were carried out by adjustment of all three parameters. The tendencies given in Fig. 4 are independent of the chosen fitting procedure. It is found that both, the Vogel temperature $`T_0`$ and the thermal expansion coefficient $`\alpha _\mathrm{f}`$ of the free volume decrease when the film thickness is reduced. Table 2 summarizes the values for both, $`T_0`$ and $`\alpha _\mathrm{f}`$ for various samples. Additionally, values for the glass transition temperature $`T_\mathrm{g}`$ as the temperature where the relaxation rate is equal to 100 s are given.

Please insert Table 2

In the framework of the free volume theory by Cohen and Turnbull CohenTurn59  the relaxation time $`\tau _\alpha `$ of the $`\alpha `$-relaxation is given by:

$$\tau _\alpha =\tau _{\mathrm{}}\mathrm{exp}(\frac{b}{f}),$$
(4)
where $`b`$ is a constant and $`f`$ is the fractional free volume. For any film thickness $`d`$, the latter is related to the Vogel temperature $`T_0`$ and the expansion coefficient $`\alpha _\mathrm{f}`$ via:

$$f(d;T)=\alpha _\mathrm{f}(d)(TT_0(d)).$$
(5)
Recently, Fukao and co-workers FukaoPRE200  reported that the $`\alpha `$-relaxation in thin spincast films of polystyrene is faster than in the bulk. In frame of the free volume theory, the decrease of both, $`\alpha _\mathrm{f}`$ and $`T_0`$ in thin grafted films leads to two competing trends concerning the relaxation time $`\tau _\alpha `$: while the former tends to slow down the $`\alpha `$-relaxation, the latter can be regarded as an increase of the relaxation rate of the $`\alpha `$-process. From these considerations it was concluded that for sufficiently high temperatures the relaxation dynamics in thin films should become slower than in the bulk. In the present study this crossover temperature could be estimated to be around 180 K. Since this value is above the temperature of crystallization, for thin films of amorphous PDMS only a faster $`\alpha `$-relaxation than that in the bulk is to be expected.

Qualitatively, the glass transition temperature $`T_\mathrm{g}`$ should behave similar to the Vogel temperature $`T_0`$ (see Tab. 2). It has been reported recently that $`T_\mathrm{g}`$ in thin grafted films of polystyrene increases for films much thicker than the radius of gyration FryerJCP01 . This result resembles to our finding for the film with $`d>R_\mathrm{g}`$, where the $`\alpha `$-relaxation is slowed down and $`T_\mathrm{g}`$ is consequently increased with respect to the bulk. However, in FryerJCP01  no results for $`T_\mathrm{g}`$ are given for the case $`d<R_\mathrm{g}`$ as it is investigated in the present study and where a decrease of $`T_\mathrm{g}`$ is found. The opposed findings of an increase and decrease of $`T_\mathrm{g}`$, respectively may be due to differences of the investigated polymers. While polystyrene has rather stiff chains, poly(dimethylsiloxane) is characterized by a high chain flexibility.

## IV Conclusions

The dynamics of the $`\alpha `$\- and $`\alpha _\mathrm{c}`$-relaxation of PDMS in the bulk and as grafted films have been investigated by use of dielectric relaxation spectroscopy. The results of this study can be summarized as follows:

1. The evaluation of the temperature dependence of the $`\alpha `$-relaxation strongly suggests that its dynamics in grafted films of PDMS depends on the ratio of the film thickness $`d`$ to the radius of gyration $`R_\mathrm{g}`$ (chain confinement). In case of the $`\alpha `$-relaxation, this dependence of the molecular dynamics on the film thickness can be well distinguished from the dependence on the thermal history of the samples.
2. In films with $`d<R_\mathrm{g}`$ the relaxation rate of the $`\alpha `$-relaxation increases by up to two orders of magnitude compared to the bulk.
3. For films with a thickness larger than $`R_\mathrm{g}`$ the relaxation rate of the $`\alpha `$-relaxation is slowed down by one order of magnitude compared to that of the bulk. This slowing down is considered as a prevailing of interactions between the polymer and the substrate over the influence of spatial (chain) confinement.
4. While the dielectric strength $`\mathrm{\Delta }\epsilon `$ of the $`\alpha `$-relaxation in films with $`d>R_\mathrm{g}`$ is comparable to that of the bulk, it is reduced by up to 60% in the thinner films. This decrease is explained by a partial immobilization of chain segments.
5. The Vogel temperature $`T_0`$ is decreased by up to 20 K in films with $`d<R_\mathrm{g}`$, whereas it is slightly increased in films with $`d>R_\mathrm{g}`$.
6. Within the framework of free volume theory, the thermal expansion coefficient of free volume $`\alpha _\mathrm{f}`$ is found to decrease in films of a thickness below $`R_\mathrm{g}`$.
7. For the $`\alpha _\mathrm{c}`$-relaxation which is related to the dynamics of the amorphous fraction of PDMS in partial crystalline samples, any possible effect of the confinement is outweighed by the dependence of this relaxation process on the thermal history of the samples.

Qualitatively, the finding concerning the relaxation time of the $`\alpha `$-relaxation in grafted films with $`d<R_\mathrm{g}`$ (Fig. 2) is in accord with results for small molecules confined to pores or channels with a diameter of 0.5 nm to 10 nm: with decreasing thickness, $`\tau _\alpha `$ is shifted to smaller values. Moreover, the results 2. and 3. lead to the conjecture of the existence of a critical thickness $`d_\mathrm{c}`$ at which the dynamics of the $`\alpha `$-relaxation changes from that in the bulk to that in thin films. In case of confined small molecules, this result could be explained unambiguously by an interference of the size of confinement with a growing correlation length $`\xi `$ (in the order of 1…10 nm) inherent to the glass transition ArndtPRL97 . However, in case of grafted PDMS deviations from the $`\alpha `$-relaxation time in the bulk appear already at film thicknesses of 15 nm (Fig. 2), whereas the molecular dynamics in films of 40 nm thickness resembles well to that of the bulk except a slight decrease of the relaxation rate. From dielectric and temperature modulated calorimetric (TMDSC) measurements on PDMS ($`M_\mathrm{w}`$=1400 g mol-1) confined to nanoporous sol-gel glasses with pore diameters ranging from 2.5 nm to 20 nm the length scale for cooperative fluctuations is estimated to be between 5 nm and 7.5 nm at the glass transition temperature DKBuch602 . But also in pores of a diameter of 20 nm an increased relaxation rate of the $`\alpha `$-relaxation of PDMS is observed with respect to that of the bulk. This is in agreement to our findings for films of a comparable film thickness, i.e. $`d<R_\mathrm{g}`$, whereas the slowing down of the $`\alpha `$-relaxation in thicker films is attributed to adsorption. From these results it has to be concluded that the onset of confinement effects for the $`\alpha `$-relaxation appears at sizes of the confinement well above the length scale for cooperative fluctuations.

## Acknowledgement

We gratefully acknowledge support of the DFG within Sonderforschungsbereich 294, TP G6.