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# Lonely adatoms in space

## Abstract

There is a close relation between the problems of second layer nucleation in epitaxial crystal growth and chemical surface reactions, such as hydrogen recombination, on interstellar dust grains. In both cases standard rate equation analysis has been found to fail because the process takes place in a confined geometry. Using scaling arguments developed in the context of second layer nucleation, I present a simple derivation of the hydrogen recombination rate for small and large grains. I clarify the reasons for the failure of rate equations for small grains, and point out a logarithmic correction to the reaction rate when the reaction is limited by the desorption of hydrogen atoms (the second order reaction regime).

Rate equations are a widely used tool for the mathematical description of kinetic phenomena. Despite successful applications in many different areas of science, however, there are instances where their predictions are known to be qualitatively incorrect. A prominent example are diffusion-controlled reactions in low dimensions . The purpose of this Rapid Communication is to point out the close relation between two kinetic problems, second layer nucleation in epitaxial crystal growth  and chemical reactions on dust grain surfaces in interstellar space , in which deviations from rate equation theory arise because the processes of interest take place in a spatially confined geometry.

In both cases one is concerned with the rate of a reaction confined to a finite surface region, onto which particles impinge and from which they leave again if no reaction takes place. In the case of second layer nucleation the confining region is the top terrace of a two-dimensional island, bounded by a step edge, while in the astrophysical context it is the (closed) surface of a small grain. In the first case the atoms leave the island by crossing the step, while in the second case they desorb from the grain surface***At high temperatures desorption plays a role also in epitaxial growth; see  for an analysis of two-dimensional nucleation in the presence of desorption..

The two problems also differ in that in second layer nucleation only the first nucleation event on the island is relevant – all atoms deposited after this event merely contribute to the growth of the second layer nucleus – whereas in the problem of grain surface reactions the reactants are usually assumed to desorb from the grain once they have formed, so that a steady state with a constant production rate is established. In this sense, second layer nucleation is a first passage problem , while grain surface kinetics deals with stationary processes.

For both problems it has been found that standard rate equation analysis fails when the mean number of particles present on the surface becomes small compared to unity (the *lonely adatom* limit of Ref.). In this fluctuation-dominated regime the reaction becomes a rare event which has to be treated statistically. Here I show how the time scale analysis developed in the context of second layer nucleation  can be applied to the problem of hydrogen recombination, one of the most important grain surface reactions of astrophysical interest. In this reaction two hydrogen atoms meet to form a H2 molecule, in analogy to the formation of a second layer nucleus in the case where dimers are stable (irreversible nucleation, critical nucleus size $`i^{}=1`$). I provide a simple derivation of the recombination rate in all three reaction regimes. I then discuss the reasons for the breakdown of the rate equation theory for small grains, and I point out the existence of a logarithmic correction to the recombination rate in the second order reaction regime, which was overlooked so far in the astrophysical context.

The notation follows that of . Atoms impinge on the grain surface at rate $`f`$ per adsorption site, they hop at rate $`a`$ and desorb at rate $`W`$. The number of adsorption sites on the grain is $`S`$, and the quantities $`F=fS`$ and $`A=a/S`$ refer to the whole grain. To make contact with the notation of  we introduce the lifetime $`\tau `$ of an atom on the grain,

$$\tau =1/W,$$
(1)
the diffusion time $`\tau _D`$ required for an atom to explore the whole grain,

$$\tau _DS/a=1/A,$$
(2)
and the mean time interval $`\mathrm{\Delta }t`$ between the arrival of two atoms on the grain,

$$\mathrm{\Delta }t=1/F.$$
(3)
The estimate (2) ignores a logarithmic correction arising from the distinction between the total number of sites visited by an adatom during its lifetime, $`𝒩_{\mathrm{all}}(\tau )`$, and the number $`𝒩_{\mathrm{dis}}(\tau )`$ of *distinct* sites visited; we will return to this point towards the end of the paper.

Following  we introduce the dimensionless quantities

$$s_{\mathrm{visit}}=a/W=S(\tau /\tau _D)$$
(4)
and

$$s_{\mathrm{vacant}}=W/f=S(\mathrm{\Delta }t/\tau ).$$
(5)
For large grains ($`S>s_{\mathrm{visit}}`$ and $`S>s_{\mathrm{vacant}}`$, respectively) $`s_{\mathrm{visit}}`$ is the number of sites visited by an atom during its lifetime, while $`s_{\mathrm{vacant}}`$ is the number of vacant sites surrounding a site occupied by an atom. If $`\tau >\tau _D`$ the atom has time to eplore the whole grain, so that the number of sites visited becomes equal to $`S`$, while for $`\tau <\mathrm{\Delta }t`$ the grain is typically occupied by zero or one atoms, so that an atom is surrounded by $`S`$ vacant sites; note that the mean number of atoms on the grain is equal to

$$\overline{n}=\tau /\mathrm{\Delta }t=F/W.$$
(6)
The relative ordering of the three dimensionless numbers $`S`$, $`s_{\mathrm{visit}}`$ and $`s_{\mathrm{vacant}}`$ defines six different regimes. It turns out, however, that the behavior of the reaction rate in a given regime depends only on which of the three numbers is the smallest. Thus we are left with three different regimes, which will be discussed in the following.

The fluctuation-dominated (lonely adatom) regime is characterized by the condition

$$S\mathrm{min}[s_{\mathrm{visit}},s_{\mathrm{vacant}}].$$
(7)
According to (4,5) this is equivalent to (i) $`\tau \mathrm{\Delta }t`$ and (ii) $`\tau \tau _D`$. The first condition simply implies that the mean number of atoms on the grain (6) is small compared to unity. In this limit, the probability that a freshly deposited atom participates in a recombination event is equal to the probability $`P_1`$ that a second atom is already present on the grain, times the *encounter probability* $`p_{\mathrm{enc}}`$ that the two atoms, once both present on the grain, will meet before one of them redesorbs. The first probability is given by  $`P_1=\tau /(\tau +\mathrm{\Delta }t)\tau /\mathrm{\Delta }t=F/W`$. Multiplying this with the number of atoms $`F=1/\mathrm{\Delta }t`$ arriving on the grain per unit time, we find that the total recombination rate (the number of molecules produced by the grain per unit time) is given by

$$R=\frac{\tau }{(\mathrm{\Delta }t)^2}p_{\mathrm{enc}}$$
(8)
whenever $`\overline{n}1`$. The second condition $`\tau \tau _D`$ implied by (7) means that, if two atoms are present simultaneously on the grain, they will meet with unit probability, because each atom spends enough time on the grain to visit all sites many times. Thus we have $`p_{\mathrm{enc}}=1`$ and

$$R=R_{\mathrm{lonely}}=\tau /(\mathrm{\Delta }t)^2=F^2/W.$$
(9)
In the small grain limit where (7) is satisfied, this expression is *exact*. The recombination efficiency defined by $`\eta =R/(F/2)`$ is then equal to $`2F/W`$, in agreement with the result obtained in  from the full solution of the master equation. In second layer nucleation, the lonely adatom regime is realized under typical experimental conditions when $`i^{}=1`$ .

In the remaining two regimes the finite grain size is irrelevant. These regimes can therefore be derived from standard rate equations . According to the scaling of the reaction rate with hydrogen flux, these two regimes will be referred to as the *first* and *second order* regimes (note that the lonely adatom regime is also of second order in this sense, see (9)).

The first order regime is characterized by the condition

$$s_{\mathrm{vacant}}\mathrm{min}[S,s_{\mathrm{visit}}].$$
(10)
In this regime the mean number of atoms on the grain is large compared to unity ($`\tau \mathrm{\Delta }t`$), and the number of sites visited by an atom during its lifetime ($`=\mathrm{min}[S,s_{\mathrm{visit}}]`$) is large compared to the number of vacant sites surrounding each atom. Hence each freshly deposited atom will certainly find a partner. In this case the recombination rate is

$$R=R_1=F/2$$
(11)
and the recombination efficiency is equal to unity. In the context of second layer nucleation, this regime corresponds to the nonstationary scaling regime I of , where the energy barriers at the step edges are so strong that $`\tau \mathrm{\Delta }t`$, and nucleation occurs as soon as a second atom is deposited onto the island.

It is easy to derive an interpolation formula connecting (9) and (11) under the assumption that the diffusion of the reactants, as well as the desorption of the hydrogen molecule, is very fast. Then the only possible values for the number of atoms on the grain is 0 or 1, since recombination occurs instantaneously as soon as a second atom is deposited. The probability $`P_1`$ for having one atom on the grain satisfies the master equation

$$dP_1/dt=FP_0(F+W)P_1=F(1P_1)(F+W)P_1$$
(12)
with the stationary solution $`P_1=F/(W+2F)`$. Since $`p_{\mathrm{enc}}=1`$, the recombination rate is

$$R=FP_1=\frac{F^2}{W+2F}.$$
(13)
The remaining, second order regime is characterized by the condition

$$s_{\mathrm{visit}}\mathrm{min}[S,s_{\mathrm{vacant}}].$$
(14)
The condition $`s_{\mathrm{visit}}S`$ (i.e., $`\tau \tau _D`$) has no clear analogue in the context of second layer nucleation, because there the lifetime of the atom is always at least as large as the diffusion time (the atom has to reach the island edge before it can leave the island). It is useful to distinguish the cases $`Ss_{\mathrm{vacant}}`$ (large grains) and $`Ss_{\mathrm{vacant}}`$ (small grains). In the first case many atoms are present on the grain simultaneously. The encounter probability for a freshly deposited atom to find a partner during its lifetime is equal to $`p_{\mathrm{enc}}=s_{\mathrm{visit}}/s_{\mathrm{vacant}}`$. Thus the recombination rate can be estimated as

$$R=R_2=Fp_{\mathrm{enc}}=F\frac{\tau ^2}{\tau _D\mathrm{\Delta }t}=\frac{f^2Sa}{W^2}$$
(15)
and the recombination efficiency is $`\eta =2af/W^2`$. For small grains the probability that a freshly deposited atom will undergo a reaction is the product of the probability $`P_1=F/W`$ that a second atom is present on the grain when it arrives, and the encounter probability, which now reads $`p_{\mathrm{enc}}=s_{\mathrm{visit}}/S`$ (note that the second atom occupies any site of the grain with equal probability). The recombination rate then becomes

$$R=\frac{F^2}{W}p_{\mathrm{enc}}=\frac{f^2Sa}{W^2},$$
(16)
which is *identical* to (15). Thus the second order result hold irrespective of whether the number of atoms on the grain is large compared to unity or not. This is similar to certain regimes of second layer nucleation with critical nucleus size $`i^{}>1`$ .

The last observation shows that the failure of rate equation theory cannot generally be attributed to the fact that the number of reactants on the grain is small compared to unity. To clarify this issue, it is instructive to consider the amount by which the reaction rate is overestimated by the rate equation expressions when the condition (7) is satisfied. Two cases have to be distinguished. For $`s_{\mathrm{vacant}}s_{\mathrm{visit}}`$ we have to compare (9) to $`R_1`$, which yields

$$R_{\mathrm{lonely}}/R_1=F/W=\tau /\mathrm{\Delta }t.$$
(17)
This is precisely the mean number of atoms $`\overline{n}`$ on the grain. Thus in this case it is justified to say that the rate equations fail because $`\overline{n}1`$. On the other hand, for $`s_{\mathrm{visit}}s_{\mathrm{vacant}}`$ we have

$$R_{\mathrm{lonely}}/R_2=SW/a=S/s_{\mathrm{visit}}.$$
(18)
This ratio is not related to the mean number of atoms on the grain. Instead, it is equal to the ratio between the number of distinct sites visited by an adatom during its lifetime ($`𝒩_{\mathrm{dis}}=S`$) and the number of all sites visited ($`𝒩_{\mathrm{all}}=a/W=s_{\mathrm{visit}}`$). Castellano and Politi have emphasized that it is the distinction between $`𝒩_{\mathrm{dis}}`$ and $`𝒩_{\mathrm{all}}`$ which is responsible for the failure of rate equation theory in the case of second layer nucleation .

In the second order regime this distinction implies a logarithmic correction to the expression (15). The number of distinct sites visited by a two-dimensional random walk during time $`\tau `$ is given by $`𝒩_{\mathrm{dis}}(\tau )\pi a\tau /\mathrm{ln}(a\tau )`$ . The diffusion time should therefore be determined more accurately by $`𝒩_{\mathrm{dis}}(\tau _D)=S`$, and the expression (4) has to be replaced by $`s_{\mathrm{visit}}=𝒩_{\mathrm{dis}}(\tau )`$. Using this in the derivation of the reaction rate in the second order regime we find

$$R_2=\frac{f^2S}{W}s_{\mathrm{visit}}\frac{\pi f^2Sa}{W^2\mathrm{ln}(a/W)}.$$
(19)
The experimental estimates for the activation energies for H diffusion and desorption on amorphous carbon surfaces quoted in  show that the logarithmic factor in (19) is $`\mathrm{ln}(a/W)15`$ at a temperature of 10 K.

To go beyond the order of magnitude estimate (19) would require a detailed analysis of the random walk problem on the grain surface along the lines of . The master equation analysis of  is not sufficient for this purpose, because it keeps track only of the total number of atoms on the grain, thus ignoring the spatial aspects of the encounters between the atoms. As a first step in this direction, I present here a simple model calculation of the encounter probability $`p_{\mathrm{enc}}`$ for the case of small grains (in the sense of $`\overline{n}1`$), which allows to interpolate between the expressions (9) and (19); a similar approach has previously been applied in the context of second layer nucleation .

We take the grain surface to be a circular disk of radius $`L`$. One of the reacting atoms is assumed to be immobile, and is placed at the center of the large disk in the form of a small disk of radius $`l`$. In this way the problem becomes radially symmetric. The deposition, diffusion and desorption of the second atom is described by the stationary diffusion equation

$$D\left(\frac{^2}{r^2}+\frac{}{r}\right)n+\stackrel{~}{f}Wn=0$$
(20)
where $`n(r)`$ is the probability density for the second atom in polar coordinates, $`\stackrel{~}{f}`$ is the impingement flux per unit area, and the diffusion coefficient is $`D=al^2`$. The boundary conditions for (20) are reflecting at the outer boundary, $`n/r=0`$ at $`r=L`$, and absorbing at the inner boundary ($`n(r=l)=0`$). The encounter probability is then obtained as the ratio of the diffusion flux incident onto the inner boundary to the total deposition flux incident onto the surface,

$$p_{\mathrm{enc}}=\frac{2\pi lDn/r|_{r=l}}{\stackrel{~}{f}\pi L^2}.$$
(21)
The solution to this diffusion problem can be found in the thin film growth literature . In the limit where the atom radius $`l`$ becomes the smallest length in the problem, the encounter probability takes the form

$$p_{\mathrm{enc}}=\frac{4a}{SW}\left(\mathrm{ln}(a/W)+2K_1(\sqrt{SW/a})/I_1(\sqrt{SW/a})\right)^1,$$
(22)
where $`I_1`$ and $`K_1`$ are incomplete Bessel functions. For small arguments $`K_1(x)/I_1(x)2/x^2`$ and $`p_{\mathrm{enc}}1`$, while for large arguments $`K_1(x)/I_1(x)0`$ and (22) reduces to $`p_{\mathrm{enc}}4a/(SW\mathrm{ln}(a/W))`$. Inserting the second result into (8) we obtain an expression identical to (19), apart from the factor $`\pi `$ which is replaced by a factor 4.

To summarize, I have shown in this paper how recent results from the theory of second layer nucleation can be applied to the closely related problem of hydrogen recombination on dust grain surfaces. The expressions (9), (11) and (15) for the recombination rate have been obtained before , but the present derivation seems more straightforward. The analysis shows that the failure of the rate equation approach is not always related to the fact that the mean number of atoms $`\overline{n}`$ on the grain is small compared to unity. The logarithmic factor in the second order regime, Eq.(19), and the interpolation formulae (13) and (22) are new. The derivation of the encounter probability for realistic grain geometries using the methods of  seems like a promising problem for future studies.

*Acknowledgement:* I would like to thank Ofer Biham for useful correspondence.


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# Mutual composite fermions in double layer quantum Hall system

## Abstract

This paper was withdrawn and incorporated into section II of cond-mat/0310512


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# Magnetoelectric Jones Dichroism in Atoms

## Abstract

The authors suggest that atomic experiments measuring the interference between magnetic-dipole and electric-field-induced electric-dipole transition amplitudes provide a valuable system to study magnetoelectric Jones effects.

A recent letter roth00  reported the first observation of magnetoelectric Jones birefringence in liquids (see also Ref. rikken01 ). This observation helped to clarify some of the long-standing theoretical confusion surrounding Jones birefringence and the associated Jones dichroism (collectively known as Jones effects) graham83 ; ross89 . The interest in further understanding these effects has led to the investigation of other experimental systems which may exhibit Jones effects. These include the possibility of observing the effects through beam divergence in uniaxial crystals izdebski01  and possible observation in the quantum vacuum rikken00 . In this letter we point out that Jones dichroism can be studied in atomic systems under much less severe experimental requirements. In addition, these atomic systems are more amenable to theoretical analysis than the relatively complicated condensed-matter systems that have been studied to date. The simplicity of these systems may help to expand the understanding of the manifestation of Jones effects in general. We also point out that our recent experiment stalnaker02  measuring interference between magnetic-dipole and electric-field-induced electric-dipole transition amplitudes in atomic ytterbium constitutes a measurement of Jones dichroism in a simple atomic system.

The development of the Jones matrix calculus for describing the propagation of light led to the prediction of two distinct types of linear birefringence and dichroism jones48 . The two types of effects differ in the orientation of the birefringent and dichroic axes. The Jones formalism revealed that certain uniaxial media may exhibit birefringence and dichroism along axes which are at $`\pm 45^{}`$ relative to the axis of anisotropy. Birefringent and dichroic effects of this type are called Jones effects. They are distinct from the familiar birefringence and dichroism, which have axes parallel and perpendicular to the axis of anisotropy.

There has been theoretical discussion concerning the requirements for media that may exhibit Jones effects and what transition moments must be accounted for in order to describe it graham83 ; ross89 . In Ref. graham83 , it was shown that Jones effects may be induced in isotropic media by the application of parallel electric and magnetic fields. If the direction of light propagation is perpendicular to the electric and magnetic fields, the Jones effects are described by

$$\mathrm{\Delta }n_Jn_{+45^{}}n_{45^{}},$$
(1)
where $`n_{\pm 45^{}}`$ is the complex index of refraction for light polarized at $`\pm 45^{}`$ relative to the electric and magnetic fields. The real and imaginary parts of $`\mathrm{\Delta }n_J`$ describe Jones birefringence and dichroism, respectively. On a microscopic level, Jones dichroism may manifest itself as a difference between the rates with which atoms of the medium are transferred to the excited state in the presence of light polarized at $`\pm 45^{}`$ relative to the electric and magnetic fields given by

$$\mathrm{\Delta }\mathrm{\Gamma }_J\mathrm{\Gamma }_{+45^{}}\mathrm{\Gamma }_{45^{}}.$$
(2)
Jones effects generally occur in materials which exhibit the more familiar birefringence and dichroism. In addition, Jones effects are predicted to be significantly smaller than the usual birefringence and dichroism in most media. Consequently, magnetoelectric Jones birefringence has been observed only recently in molecular liquids under extreme experimental conditions roth00 ; rikken01 .

To our knowledge, the observation of Jones dichroism has not been reported as such. Here we point out that Stark-interference experiments bouchiat74  which utilize parallel electric and magnetic fields provide a simple atomic system which exhibits Jones dichroism. The experiment stalnaker02  measuring a highly forbidden magnetic-dipole transition amplitude in atomic ytterbium using this technique constitutes such a system and its results can be interpreted as an observation of magnetoelectric Jones dichroism.

In the experiment stalnaker02 , we studied a highly forbidden transition between states of the same parity. In the absence of external fields and neglecting parity-nonconserving effects, the transition occurs only through a small magnetic-dipole amplitude ($`10^4\mu _B`$, where $`\mu _B`$ is the Bohr magneton). By applying a static electric field, an electric-dipole amplitude is induced through mixing of opposite-parity states. An atomic beam of ytterbium was excited with resonant laser light propagating perpendicularly to parallel electric and magnetic fields. The excitation light was polarized at an angle $`\theta `$ relative to the external fields. For the transition studied in our experiment (between a ground state with total angular momentum equal to zero and an excited state with total angular momentum equal to one), the electric field, $`𝐄`$, results in a Stark-induced electric-dipole transition amplitude to the $`M_J^{}`$ magnetic sublevel of the excited state given by bouchiat74

$$A\left(E1_{St}\right)=i\beta \left(𝐄\times 𝜺\right)_{M_J^{}},$$
(3)
where $`𝜺`$ is the electric-field amplitude of the laser light, $`(𝐄\times 𝜺)_{M_J^{}}`$ is the $`M_J^{}`$ component of the vector in the spherical basis, and $`\beta `$ is the vector transition polarizability note . The magnetic-dipole transition amplitude is given by

$$A(M1)=\mu (\widehat{𝐤}\times 𝜺)_{M_J^{}},$$
(4)
where $`\widehat{𝐤}`$ is the direction of propagation of the excitation light, $`\widehat{𝐤}\times 𝜺`$ is the magnetic-field amplitude of the light, and $`\mu `$ is the magnetic-dipole matrix element between the ground state and any of the $`M_J^{}`$ magnetic sublevels of the excited state. The transition rate is therefore

$$\begin{array}{cc}\hfill \mathrm{\Gamma }& \underset{M_J^{}}{}\left|A\left(E1_{St}\right)+A\left(M1\right)\right|^2\hfill \\ & \underset{M_J^{}}{}\left|A\left(E1_{St}\right)\right|^2+2\mathrm{R}\mathrm{e}\left[A\left(E1_{St}\right)A\left(M1\right)^{}\right]+\left|A\left(M1\right)\right|^2.\hfill \end{array}$$
(5)
As is discussed in Ref. stalnaker02 , the interference term in Eq. (5) is of opposite sign for the $`M_J^{}=+1`$ and $`M_J^{}=1`$ magnetic sublevels. It is therefore necessary to apply a magnetic field to resolve the different sublevels in order to observe the effect of this term. The signal due to the interference term is proportional to the rotational invariant

$$[(𝐄\times 𝜺)\times (\widehat{𝐤}\times 𝜺)]\widehat{𝐁},$$
(6)
which is also true in a more general case where $`𝐄`$ and $`𝐁`$ are not necessarily collinear.

We define the $`z`$ axis to be along the direction of the magnetic field, $`𝐁=B\widehat{𝐳}`$, and define the $`x`$ axis so that the electric field lies in the $`x`$-$`z`$ plane, $`𝐄=E_x\widehat{𝐱}+E_z\widehat{𝐳}`$. We assume that the light propagation is perpendicular to both fields, $`𝐤=k\widehat{𝐲}`$ and that the light is linearly polarized at an angle $`\theta `$ relative to the magnetic field, $`\widehat{\epsilon }=\mathrm{sin}\theta \widehat{𝐱}+\mathrm{cos}\theta \widehat{𝐳}`$ (Fig. 1).

The $`\left|A\left(E1_{St}\right)\right|^2`$ and $`\left|A\left(M1\right)\right|^2`$ terms in Eq. (5) are independent of the sign of the angle of polarization while the interference term is odd with $`\theta `$. Using expression (6) it is easily shown that the difference in transition rates for $`\pm \theta `$ results in a Jones dichroism given by

$$\mathrm{\Gamma }_{+\theta }\mathrm{\Gamma }_\theta E_z\mathrm{sin}\theta \mathrm{cos}\theta .$$
(7)
The factor $`E_z`$ in Eqn. (7) shows that

$$\mathrm{\Delta }\mathrm{\Gamma }_J𝐄\widehat{𝐁},$$
(8)
which is the predicted dependence of the magnetoelectric Jones effects on $`𝐄`$ and $`𝐁`$ graham83 . It is interesting to note that the transition rate depends on the magnitude of the magnetic field only for values of the magnetic field which do not fully resolve the magnetic sublevels. This is analogous to the change in magnetic-field dependence of the resonant Faraday rotation (see for example Ref. budker02 ).

Due to the weakness of the forbidden transition studied, we determined the transition rate by observing fluorescence in a decay branch of the excited state rather than detecting absorption. In our experiment the observed Jones dichroism is significantly smaller ($`5\times 10^3`$ at the electric fields used in the experiment) than the normal dichroism, which is dominated by the Stark-induced amplitude. As can be seen from Eq.(3), only the component of the light electric field that is perpendicular to $`𝐄`$ contributes to the transition rate. Thus, the dominant fluorescence signal is proportional to $`\mathrm{sin}^2\theta `$ and to $`\left|E\right|^2`$. These dependences were verified experimentally. The interference term responsible for Jones dichroism was isolated from the dominant signal by comparing the fluorescence spectra for opposite electric fields. In the data analysis we normalized the interference term to the dominant signal resulting in an asymmetry given by

$$\frac{\mathrm{\Gamma }(E_+)\mathrm{\Gamma }(E_{})}{\mathrm{\Gamma }(E_+)+\mathrm{\Gamma }(E_{})}=\frac{2M1}{\beta E}\frac{\mathrm{cos}(\theta )}{\mathrm{sin}(\theta )}M_J.$$
(9)
The dependence of the asymmetry on the electric field, magnetic field, and polarization angle was verified experimentally (see Ref. stalnaker02  for figure showing the interference term versus the magnitude of the electric field). Figure 2 shows the experimental fractional asymmetry \[Eq.(9)\] plotted versus the polarization angle. We have normalized the signal to the magnitude of the electric field in order to combine data taken a different electric fields and leave only the polarization angle dependence. Also shown is the expected angular dependence of the asymmetry. Most of the data was taken with light polarized at $`\theta =\pm 45^{}`$ relative to the electric field since the interference term is maximal at these values \[see Eq. (7)\]. The difference in the sign of the asymmetry for $`\theta =\pm 45^{}`$ clearly indicates a nonzero value of $`\mathrm{\Delta }\mathrm{\Gamma }_J`$, verifying the key signature of Jones dichroism.

We note that although the Jones dichroism was significantly smaller than the usual dichroism in our experiment, it is possible to significantly increase its size by using an allowed magnetic-dipole transition. In fact, it possible to have both the Jones dichroism and the regular dichroism of the same order as the overall absorption, which can be substantial in the case of an allowed magnetic-dipole transition.

Finally, we point out that atomic systems may be of use in measuring other types of magnetoelectric effects which are currently being studied in more complicated systems, such as more common forms of magnetoelectric linear birefringence roth02  and magnetoelectric directional anisotropy rikken02 . In fact, expression (6) shows that this system exhibits both of these effects. It is interesting to note that a polarization-dependent directional anisotropy is present for both parallel and perpendicular electric and magnetic fields. For the case of perpendicular electric and magnetic fields a component of the directional anisotropy is present even when averaged over the polarization angle.

The authors acknowledge their co-authors in Ref. stalnaker02 , D. P. DeMille, S. J. Freedman, and V. V. Yashchuk, and helpful discussions with D. F. Kimball, A.-T. Nguyen, A. O. Sushkov, S. M. Rochester, and E. D. Commins. This work has been supported by NSF, ONR, and the Miller Institute for Basic Research in Science.


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# A Search for Pulsars in Quiescent Soft X-Ray Transients. I.

## 1 Introduction

According to the current paradigm, millisecond pulsars (MSPs) are old neutron stars (NSs) recycled through accretion of matter and angular momentum from a mass-losing companion in a binary system (Alpar et al. 1982). Because the accretion process powers a copious X-ray emission, the progenitors of the millisecond pulsars are believed to form a subset of the population of the bright X-ray binaries (see e.g. Bhattacharya & Srinivasan 1995); namely, those classified as Neutron Star Low Mass X-ray Binaries (NS–LMXBs: see e.g. White, Nagase & Parmar 1995 for a review), in which a relatively light K or M star orbits a neutron star and overflows its Roche lobe with the mass transfer is mediated by a keplerian disk.

In a handful of these systems the spin frequency of the NS has been estimated from either coherent pulsations detected during type-I bursts or, indirectly, from the difference of the frequencies of the peaks of the kilohertz quasi periodic oscillations (kHz-QPOs) seen in the X-ray power spectrum of the source (e.g. van der Klis 2000 or Strohmayer 2001). In the latter case, the frequency difference $`\mathrm{\Delta }\nu `$ is interpreted as representative of the spin rate of the NS or of an overtone (Miller, Lamb & Psaltis 1998, but see Stella & Vietri 1998 for a different interpretation). A more accurate analysis has demonstrated that, at least in some cases, $`\mathrm{\Delta }\nu `$ is not constant (e.g. van der Klis et al. 1997; Mendez & van der Klis 1999); however, when both the kHz-QPOs and the coherent pulsations during type-I bursts can be observed, the inferred rotational periods are almost identical and cluster in the interval 1.8–3.8 ms for all the known sources. In the last few years, three transient sources (SAX J1808.4$``$3658, Wijnands & van der Klis 1998, 1751-305, Markwardt et al. 2002 and XTE 929-314, Galloway et al. 2002) have been discovered to emit coherent pulsations during the entire outburst event. These sources are the first examples of accretion-powered MSPs.

The spin rates inferred from all these sources can be coupled with other requirements imposed by the accretion process for constraining the NS magnetic moment (White & Zhang 1997; Burderi & King 1998; Psaltis & Chakrabarty 1999; Burderi et al. 2002), resulting in values spanning the interval $`10^{25}10^{27}`$ G cm$`^3.`$ In summary, all the available data strongly support the hypothesis that the NS–LMXBs host neutron stars spun up to millisecond periods and having surface magnetic field intensity in the range of those observed in the (spin-powered) MSPs.

Despite all these clues, there is no direct proof of their being the MSP progenitors. Detection of radio signals pulsating at the rotational rate of the NS from some of these sources would provide this proof. A common requirement of the models of the radio emission mechanism from a rotating, magnetized NS is that a radio pulsar phase begins once the space surrounding the NS is free of external matter up to the light cylinder radius $`r_{lc}`$ (at which the speed of material rigidly rotating with the NS would be equal to the speed of light):

$$r_{lc}=4.8\times 10^6P_3\mathrm{c}m$$
(1)
where $`P_3`$ is the pulse period in ms. During the Roche-lobe overflow phase, the plasma spilling through the inner Lagrangian point of the binary system settles into an accretion disc, whose inner rim is located at the so-called magnetospheric radius $`r_m.`$ That radius results equal to a fraction $`\varphi 1`$ of the Alfvén radius, at which the pressure of the (assumed dipolar) NS magnetic field balances the ram pressure of the (assumed spherically) infalling matter:

$$r_m=1.0\times 10^6\varphi \mu _{26}^{4/7}\dot{m}_E^{2/7}m_1^{1/7}R_6^{2/7}\mathrm{c}m$$
(2)
Here $`\mu _{26}`$ is the magnetic moment in units of $`10^{26}`$ G cm3, $`\dot{m}_E`$ is the accretion rate in Eddington units (for a $`10^6`$ cm stellar radius the Eddington accretion rate is $`1.5\times 10^8`$ M yr-1 and scales with the radius of the compact object), $`m_1`$ is the NS mass in solar masses, and $`R_6`$ is the NS radius $`R`$ in units of $`10^6`$ cm. All these units are scaled to the parameters of a typical NS–LMXB, as inferred from the aforementioned observations and modeling. As long as $`r_m`$ is smaller than $`r_{lc},`$ the infalling plasma penetrates deeply in the NS magnetosphere and prevents the coherent emission of radio waves. Hence, bright NS–LMXBs showing steady X-ray luminosity are unsuitable targets for observing radio pulses.

However, among the NS–LMXBs known in the Galaxy, $`1/7`$ experience recurrent X-ray activity separated by longer phases of relative quiescence (Tanaka & Shibazaki 1996). They are known as Neutron Star Soft X-ray Transients (NS–SXTs), belonging to the larger class of the X-ray novae. The physical mechanism driving the transient behaviour of these objects is not fully understood yet (Tanaka & Shibazaki 1996), although a promising model invokes thermal disc instabilities coupled with the stabilizing effects of the illumination of the outer disc by the X-ray from the central source (King, Kolb & Burderi 1996; van Paradijs 1996).

During an outburst, the typical luminosity in the 0.5$``$10 keV band peaks between 1036 and 1039 erg/s (Chen, Shrader & Livio 1997) and the frequent observation of type-I bursts unambiguously indicate that massive accretion onto the NS surface is responsible. As a consequence, coherent radio emission cannot occur in this phase. More recently, also the 0.5$``$10 keV luminosity in quiescence has been detected, at levels ranging between 1031.5 and 1034 erg/s (Campana et al. 1998, Wijnands et al. 2001, Wijnands et al. 2002). Accretion of matter at a lower rate (van Paradijs et al. 1987; Yi et al. 1996) and shock emission from an enshrouded rapidly spinning pulsar (Stella et al. 1994) were originally proposed to account for this lower-luminosity emission. Detailed studies of the X-ray spectrum in quiescence (Rutledge et al. 2001) and of the thermal relaxation of the NS crust during this phase (Colpi et al. 2001) now suggest that the cooling of the periodically warmed up NS surface (Brown et al. 1998) is the more viable explanation for the bulk of the soft X-ray luminosity in quiescence. If this is the correct interpretation, during the X-ray quiescent phase $`\dot{m}_E0`$ and thus, plausibly

$$r_m>r_{lc}.$$
(3)
The time scale for the expansion of the magnetospheric radius beyond the light cylinder radius, in response to a sudden drop of the mass transfer rate, is much shorter (Burderi et al. 2001) than the typical duration ($``$ years) of a phase of quiescence in a NS–SXT, in principle allowing the radio pulsar to switch on. While inverse Compton scattering from the thermal photons of the quiescent X-ray emission could in principle play a role in absorbing the electrons of the primary beam (hence inhibiting radio emission) in the case of high magnetic field pulsars (Zhang, Qiao & Han 1997, Harding & Muslimov 2002), the same picture seems hardly appliable to the magnetosphere of millisecond pulsars (Supper & Trumper 2000).

With this picture in mind, we have undertaken a systematic deep search for millisecond pulsations at 1.4 GHz in six NS–SXTs during their phases of quiescence. Three of them had not been observed before, while we have significantly increased the sensitivity limits for the three sources (1455$``$314, 1908+005 and 1745$``$203) which had been already investigated with negative results (Kulkarni et al. 1992, Biggs & Lyne 1996). The observations and the method of analysis of the data are presented in §2, the results are reported in §3 and are discussed in §4. In §3.1 we discuss the limits introduced in our search by the orbital Doppler effect. The results of a fully accelerated search, which would further improve our limits, will be presented in paper II.

A pulsar binary system has been recently discovered (PSR J1740$``$5340, D’Amico et al. 2001a) in which the Roche-lobe overflow stage is apparently not yet ended (Ferraro et al. 2001). The MSP is already active and sweeps away the infalling matter preventing accretion onto its surface. This could be the first example of a binary in the radio-ejection phase (Burderi, D’Antona & Burgay 2002), believed to be common in many NS–SXTs when the transition from outburst to quiescence occurs (Burderi et al. 2001). Remarkably, the signal from PSR J1740$``$5340 is eclipsed for about 40% of the time at 1.4 GHz and often strongly disturbed at all orbit phases (D’Amico et al. 2001b), suggesting a bias against the detection of this kind of radio source. Thus, in §4.3 we speculate on the possible absorption of the radiopulsar signal from a NS–SXT when it travels through the plasma that the mass donor companion pours in the binary system also during the X-ray quiescent phase.

## 2 Observations and data analysis

In Table 1 we present our sample of NS–SXTs, listing the principal observational characteristics derived from X-ray and/or optical data.

Radio observations were made using the Parkes 64-m radio telescope with the central beam of the multibeam receiver at a central radio frequency of 1.4 GHz (cf. Manchester et al. 2001) on 1998 August 2 – 12. The nominal gain and system temperature of the system were 0.67 K/Jy and 22 K, respectively. After detection, the two orthogonally polarized signals are fed through a multichannel filterbank, in order to minimize the pulse broadening due to dispersion in the interstellar medium (ISM). The outputs from each channel are summed in polarisation pairs, integrated and 1-bit digitized every 0.125 ms. The resulting time series are stored on digital linear tapes for offline analysis. In general we used one of two filterbanks: the first splits the signal into 96 3 MHz$``$wide channels covering a total bandwidth of 288 MHz; the second has 256 channels, each 0.25 MHz wide, for a total bandwidth of 64 MHz. For the source KS 1731$``$260 (observed in March 2001) we used a filterbank with 512 0.5 MHz channels, giving a total band of 256 MHz, which became available recently.

The observations lasted $`16`$ hrs for each target; we have split the collected data in segments of different length, typically containing from $`2^{22}`$ to $`2^{24}`$ samples, corresponding to $`9`$ min and 35 min, respectively. Each segment has been analyzed with vlsa (Very Long Spectral Analysis, see http://tucanae.bo.astro.it/pulsar/vlsa/). In a first stage the data are de-dispersed according to 325 trial DM values ranging from 0.14 to 207.5 pc$`\mathrm{cm}^3`$ for the 96-channel filterbank, or 865 trial DM values in the interval between 0.56 and 2277.2 pc$`\mathrm{cm}^3`$ for the 256-channel filterbank, or 1731 trial values ranging from 0.16 to 1293.6 pc$`\mathrm{cm}^3`$ for the 512-channel filterbank. Lower and upper limits for the searched DMs correspond respectively to a broadening of 0.125 ms (i.e. equal to the sampling time) over the whole band and to a broadening of 2 ms in a single channel (above which the detection of a typical MSP becomes questionable).

Subsequently, each de-dispersed time series is transformed using a Fast Fourier Transform and the highest peaks in the power spectrum (and in the power spectra resulting from 5 steps of harmonic summing; see Manchester et al. 2001) are searched. In summary, for each investigated DM, we have selected periods ranging from 0.5 ms to 200 ms and with a spectral signal-to-noise ratio (S/N) greater than 7.0, storing a list of 640 candidates.

These lists are then sorted in order of decreasing S/N, rejecting, when possible, signals due to known interference. Finally, the time-domain data are folded in 128 subintegrations, using the period of each selected suspect, and the resulting subintegration arrays are searched for pulsed emission around the nominal period and dispersion measure. The parameters for final pulse profiles having S/N above a given threshold ($`\stackrel{>}{_{}}7.0`$) are displayed for visual inspection.

## 3 Results

No radio pulsation with period in the range $`0.5÷200`$ ms has been found in the six Soft X-ray Transients observed. In the following we present the flux density limits of our search. Moreover, we compare them with previous results, when available.

The equation that describes the minimum detectable flux density for a pulsar of period $`P`$ is (e.g. Manchester et al. 1996):

$$S_{min}=ϵn_\sigma \frac{T_{sys}+T_{sky}}{G\sqrt{N_p\mathrm{\Delta }t\mathrm{\Delta }\nu _{MHz}}}\sqrt{\frac{W_e}{PW_e}}\mathrm{mJy}$$
(4)
where $`n_\sigma `$ is the minimum S/N that we consider (in this case 7.0), $`T_{sys}`$ and $`T_{sky}`$ the system noise temperature and the sky temperature in K respectively, $`G`$ the gain of the radio telescope (in K/Jy), $`\mathrm{\Delta }t`$ the integration time in seconds, $`N_p`$ the number of polarizations and $`\mathrm{\Delta }\nu _{MHz}`$ the bandwidth in MHz. $`ϵ`$ is a factor $`1.4`$ accounting for sensitivity reduction due to digitization and other losses. $`W_e`$ is the effective width of the pulse:

$$W_e=\sqrt{W^2+\delta t^2+\delta t_{DM}^2+\delta t_{scatt}^2}$$
(5)
Its value depends on the intrinsic pulse width $`W`$, on the time resolution $`\delta t`$ of the receiver and on the broadening of the pulse introduced both by the dispersion of the signal in each channel ($`\delta t_{DM}`$) and by the scattering induced by inhomogeneities in the ISM ($`\delta t_{scatt}`$).

In Figure A Search for Pulsars in Quiescent Soft X-Ray Transients. I. we show the flux density limits as a function of pulse period for the segments containing $`2^{24}`$ samples, for all our targets but SAX J1808.4$``$3658, for which the period is known. The solid lines refer to the $`96\times 3`$ MHz filterbank, the dash-dotted lines refer to the $`256\times 0.25`$ MHz filterbank. For KS 1731$``$260 the curves refer to the $`512\times 0.5`$ MHz filterbank. Going towards short periods, the attained sensitivity depends strongly on the adopted DM value. So the lines related to each filterbank split below $`100`$ ms, representing the flux density limits for the nominal DM (i.e. the one inferred from the distance of the source and the ISM electron distribution model by Taylor & Cordes, 1993) and the upper DM value explored in the search, respectively.

For Cen X$``$4, Aql X$``$1 and 1745$``$203 we compare in Fig. A Search for Pulsars in Quiescent Soft X-Ray Transients. I. our results with those of Kulkarni et al. (1992) and of Biggs & Lyne (1996). We have drawn with dotted lines their flux density limits, extrapolated at 1.4 GHz using the $`S_{min}`$ reported by the authors and assuming a typical spectral index 1.7 for the millisecond pulsars. The range of DMs is the same used for plotting our results. We note that our sensitivity limits are significantly better (from 3 to 10 times, depending also on the period) than any previous result.

For those sources for which the pulse period is well known (SAX J1808.4$``$3658) or for which an indication of the pulse period exists (Aql X$``$1 and 1731$``$260), we also plotted (see Figure A Search for Pulsars in Quiescent Soft X-Ray Transients. I.) the flux density limit as a function of the DM, at constant $`P`$. The vertical dashed line indicates the nominal DM.

The upper limits on the flux density (for nominal DM and using either the known pulse period or a standard value $`P=3`$ ms) are listed in the second column of Table 2 for 35 min long integrations.

Given various uncertainties on the parameters of our apparatus which enter eqs. 4 and 5, we estimate a residual systematic uncertainty of $``$25% in the absolute values of the flux densities reported in Table 2 (Camilo et al. 2000).

### 3.1 Effects of the orbital motion

Because a full acceleration code was not available when the observations were analysed, we now discuss the effects of the orbital motion.

For a binary pulsar, the time of arrival of the pulses (and in turn the observed pulse phase) is affected by the orbital motion. This results in a broadening of the integrated pulse profile and hence in a sensitivity loss during a blind periodicity search. In this case, the effective pulse width can be written as:

$$W_{e\mathrm{\_}bin}=\sqrt{W_e^2+\delta t_{bin}^2}.$$
(6)
The extra term $`\delta t_{bin}`$ accounts for the pulse broadening introduced by the Doppler effect due to the orbital motion:

$$\delta t_{bin}=\frac{1}{8c}a\mathrm{\Delta }t^2$$
(7)
where $`c`$ is the speed of light and $`a`$ is the line-of-sight component of the acceleration of the NS, supposed constant during the integration time $`\mathrm{\Delta }t.`$ As $`\delta t_{bin}`$ approaches the pulse period $`P,`$ the pulsating signal is smeared, preventing the discovery of MSPs in strongly accelerated binary systems (cf. Johnston & Kulkarni 1991; Camilo et al. 2000; Jouteux et al. 2002).

For an assigned value of $`a`$, $`\delta t_{bin}`$ can be significantly decreased only reducing $`\mathrm{\Delta }t.`$ All the NSs in our sample belong to binary systems: thus, in addition to the standard segments containing $`2^{24}`$ samples, we analysed also shorter time series of $`2^{22}`$ samples (corresponding to $`9`$ min), implying a reduction of $`\delta t_{bin}`$ of at least a factor 16. In Figure A Search for Pulsars in Quiescent Soft X-Ray Transients. I. we show the sensitivity loss due to the orbital motion for the case of an integration time of $`9`$ min. The solid line represents the sensitivity to an isolated pulsar, while long-dashed, short-dashed and dotted lines are for a pulsar in a binary system, subjected to a constant acceleration of 5, 15 and 30 m s-2 respectively. These values of $`a`$ span the range of the instantaneous accelerations along the line-of-sight that are experienced by the known millisecond pulsars detected in binary systems.

However, each pulsar undergoes a change of the sign of the line-of-sight acceleration twice a orbit, namely at orbital phases 0.00 and 0.50, when it is in quadrature with the companion star. If a segment of the observation brackets one of these phases and the integration time $`\mathrm{\Delta }t`$ is a small fraction of the orbital period, the Doppler effect does not significantly affect the detectability of the pulsar in that segment of data. Whenever the total observing time covers at least half a orbit of a binary system, a good segment can always be selected.

According to these considerations, we have listed in Table 2, the minimum pulse period that our search could have detected for the NS–SXTs whose orbital period is known. In particular, we have assumed that the minimum detectable period corresponds to $`\delta t_{bin}=2W_e`$, which is $`0.3P`$ for a duty cycle of $`15\%.`$ The value in the fourth column refers to the most favorable situation in which, during a $`9`$ min observation, the NS experiences the minimum line-of-sight acceleration along its (assumed circular) orbit (i.e. when the NS centripetal acceleration is almost perpendicular to the line of sight). The probability that one of the segments in which we have split the observations just coincides with this favorable condition is listed in the fifth column. The value in the last column refers to the worst case, in which the NS apparent motion is almost perpendicular to the line of sight.

For SAX J1808.4$``$3658, for which we know both the (short) orbital period and the pulse period, and for which our observations covered twice the entire orbit, we analysed segments containing only $`2^{21}`$ samples corresponding to 4.4 min. With this choice we are sure that there are at least four segments of the observation where the maximum acceleration along the line-of-sight is $`\stackrel{<}{_{}}3`$ m s-2 implying a negligible broadening of the pulse $`\stackrel{<}{_{}}0.1`$ ms.

From Table 2 we see that, with a modest penalty in term of limiting flux density (about a factor 2), our search had a good probability of detecting a millisecond pulsar signal in these binary systems, at least where an indication of the orbital period is available.

It is worth noting that the pulse periods in the sixth column are absolute upper limits: since a significant fraction of the orbit has been always covered by our observations, the line-of-sight acceleration in the best of our segments is certainly less than the maximum possible acceleration. Moreover, if a millisecond pulsar is bright enough, its signal can appear in a portion of the subintegration array of the folded data even if it is badly smeared by the binary motion over the whole observation. Such a feature would certainly have been recognised.

## 4 Why a null result ?

Although a full acceleration analysis might improve our detection limit, we have reached sensitivities significantly better than any similar previous search on these six targets, yet we have no detections. We see three possible expanations for this within the framework of the recycling model. These are examined in turn.

### 4.1 No coherent radio emission in quiescence

A first interpretation is that the simple model presented in §1 fails to predict when the radio emission mechanism switches on in a fast-rotating magnetized neutron star. In particular the condition of equation (3) could be necessary but not sufficient: maybe the conditions for establishment of coherent radio emission require a time longer than the typical time between two accretion phases. On this hypothesis, the class of the NS–SXTs displaying the longest times of quiescence should be preferentially selected for the search of radio pulses.

Another possibility is that the mechanism of accretion contributes to the X-ray luminosity also during quiescence. In this case, the condition (3) is fulfilled if

$$\frac{\dot{m}_{quiesc}}{\dot{m}_{outb}}=\left[\frac{r_m(outb)}{r_m(quiesc)}\right]^{7/2}\stackrel{<}{}\left[\frac{r_m(outb)}{r_{lc}}\right]^{7/2}$$
(8)
where $`\dot{m}_{quiesc},`$ $`\dot{m}_{outb},`$ $`r_m(quiesc)`$ and $`r_m(outb)`$ are the mass transfer rates toward the NS and the magnetospheric radii during the quiescence and during an X-ray outburst. When an approximate value of the spin rate of the NS is available, the rightmost term in equation (8) can be estimated. On the contrary, the leftmost term in equation (8) is usually difficult to estimate because the efficiency $`\eta `$ of conversion of the accretion flow into observed X-ray luminosity depends on the regime at which the bulk of the accretion energy is released (Campana et al. 1998). Actually, accretion directly onto the surface of a spinning, magnetized NS is centrifugally inhibited once the magnetospheric radius is outside the corotation radius $`r_{co},`$ at which the Keplerian angular frequency of the orbiting matter equals the NS angular speed:

$$r_{co}=1.5\times 10^6P_3^{2/3}m_1^{1/3}\mathrm{c}m.$$
(9)
The light cylinder is always outside the corotation radius, their ratio being $`r_{lc}/r_{co}=3.2P_3^{1/3}m_1^{1/3}>1`$ for reasonable values of the parameters. When a NS settles in the so-called propeller stage (i.e. $`r_{co}<r_m<r_{lc}`$), $`\eta `$ depends on uncertain factors (Illarionov & Sunyaev 1975) and hence the observed reduction in the X-ray luminosity during the decline from an outburst cannot unequivocally lead to the conclusion that equation (3) is satisfied. Similar caveats hold if the inner part of the accretion disk is bloated, allowing some of the matter to overcome the centrifugal barrier, accreting onto the NS polar caps.

### 4.2 Geometry and luminosity biases

Even if a radio pulsar is active, its signal could be too weak for being detected at the distance of the Earth and/or the radio beams could miss our line-of-sight. In this section we try to quantify the probability that such geometrical and luminosity factors prevent the detection of radio pulsations at 1.4 GHz from all our six targeted sources.

The average value $`f(\rho )`$ of the fraction of the sky swept by two conal radio beams of half-width $`\rho `$ is

$$f(\rho )=_0^{\pi /2}f(\rho ,\alpha )\mathrm{sin}\alpha d\alpha =(1\mathrm{cos}\rho )(\rho \frac{\pi }{2})\mathrm{sin}\rho $$
(10)
where $`\alpha `$ is the angle (supposed randomly distributed) between the magnetic axis (aligned with the radio beams) and the rotational axis and $`f(\rho ,\alpha )=\mathrm{cos}[max(0,\alpha \rho )]\mathrm{cos}[min(0,\alpha +\rho )]`$ (Emmering & Chevalier 1989).

As a population, the MSPs display wider beams than the longer-period pulsars, but the measured opening angles do not follow the same $`P^{1/2}`$ scaling law of the normal pulsars (Kramer et al. 1998). On the contrary, they are spread over a large range of angles for similar values of $`P`$. Conservatively assuming the average value $`<\rho >=25^o`$ derived from profile widths measured at 10% intensity by Kramer et al. (1998), we get $`f(\rho )=0.57`$. Hence, the probability that the radio beams of all the six targeted sources are missing our line-of-sight is $`0.006`$.

Because of poor statistics and observational biases, the luminosity function of MSPs is difficult to assess. Therefore, in Figure A Search for Pulsars in Quiescent Soft X-Ray Transients. I. we have plotted the distribution (binned in logarithmic units) of the pseudo-luminosity $`S_{1400}\times d^2`$ for 58 MSPs detected in the Galactic disk and in globular clusters, where $`S_{1400}`$ is the measured flux density in mJy at 1400 MHz and $`d`$ is the distance of the source, generally inferred from the dispersion measure, given a model for the distribution of the interstellar ionized matter (Taylor & Cordes 1993). When available, we have used the values of $`S_{1400}`$ quoted in literature, otherwise we have scaled the 400 MHz flux densities using an average spectral index for the MSPs, $`\alpha =1.7`$ (Kramer et al. 1998). Comparing the obtained distribution with our sensitivity limits (indicated in Fig. A Search for Pulsars in Quiescent Soft X-Ray Transients. I. with an arrow for each observed object) we have roughly estimated for each source the probability that its pseudo-luminosity is too faint for detection in our experiment. These probabilities are shown in Fig. A Search for Pulsars in Quiescent Soft X-Ray Transients. I.. Combining these results with the beaming factor, there is a probability of $`20`$% that the pulsed emission from all the objects in our list would be unobservable at 1.4 GHz. This is not negligible, but can be reduced with deeper searches and/or a larger sample.

### 4.3 Absorption in the plasma surrounding the binary

It is well known that absorption (see e.g. Thompson et al. 1994 for a review) is a viable mechanism for explaining the absence of observable radio signals from a source surrounded by ionized gas: here we will investigate this hypothesis for the case of a radio pulsar in a NS–SXT.

It has been recently suggested (Burderi et al. 2001) that during their X-ray quiescent phase, most NS–SXTs show the so-called radio–ejection phenomenon. During the transition from outburst to quiescence, the mass transfer rate suddenly drops from $`\dot{m}_{outb}`$ (which determines the X-ray luminosity during the outburst) to a value below $`\dot{m}_{switch}`$, at which the condition (3) is satisfied and the NS becomes a source of relativistic particles and magneto-dipole emission. The released energy both (i) sweeps the environment of the neutron star, allowing coherent radio emission to be switched on (Shvartsman 1970) and (ii) expels the gas still leaving the companion star through the inner Lagrangian point of the binary, thus preventing further accretion (Ruderman, Shaham & Tavani 1989).

As pointed out by Burderi et al. (2001), a moderate resurgence of the mass transfer rate $`\dot{m}`$ to a value just above $`\dot{m}_{switch}`$ is not sufficient to cause accretion to resume. To quench the radio pulsar, $`\dot{m}`$ must be restored to at least the outburst value $`\dot{m}_{outb}`$. This means that, during the X-ray quiescent phase of a NS–SXT, the mass loss rate from the companion can be quite large (almost equal to the mass transfer rate during the outburst, $`\dot{m}_{outb}`$), but nevertheless the matter overflowing the Roche lobe of the companion is swept away by the radiation pressure of the pulsar and leaves the system in the form of a wind.

The possible occurrence of large values of $`\dot{m}`$ during quiescence suggests that a surrounding wind may be responsible for absorption of the radio emission at any orbital phase. A hydrodynamical simulation of the flow of the plasma from the inner Lagrangian point to the surroundings of the binary is beyond the scope of this paper. Here we are interested in an order-of-magnitude estimate, to verify that absorption of the radio signal by the ejected plasma can occur for reasonable values of NS–SXT parameters. We adopt the simple hypotheses of free-free absorption in a spherically symmetric outflow (Rasio et al. 1989).

For a system seen edge–on, the minimum electron column density $`n_e`$ occurs when the NS is in front of the secondary. In this case $`n_e=\gamma _{R_{L1}}^DN_e𝑑r=\gamma _{R_{L1}}^D\rho _{wind}(X+0.5Y)/m_p𝑑r`$, where $`N_e`$ is the electron density (in cm-3), $`R_{L1}`$ is the radius of the inner Langrangian point, $`D`$ is the distance of the system, $`\gamma `$ is the fraction of ionized gas, $`X0.7`$ and $`Y0.3`$ are the hydrogen and helium fractions respectively, and $`m_p`$ is the proton mass. The density of the swept wind $`\rho _{wind}`$ is given by the continuity equation $`4\pi r^2\rho _{wind}v_{wind}=\dot{m},`$ where $`v_{wind}`$ is the speed of the wind and $`\dot{m}`$ the mass loss rate from the secondary. The free-free optical depth can be computed from

$`\tau _{ff}=0.018g_{ff}T^{3/2}\nu ^2{\displaystyle _{R_{L1}}^D}N_e^2𝑑r`$ (11)
where $`\nu `$ is the observation frequency, $`T`$ is the temperature of the gas surrounding the NS and $`g_{ff}`$ is the Gaunt factor. This term can be written as (Tucker 1975)

$`g_{ff}={\displaystyle \frac{\sqrt{3}}{2\pi }}\mathrm{ln}\left[{\displaystyle \frac{4}{\xi ^{5/2}}}\left({\displaystyle \frac{KT}{h\nu }}\right)\left({\displaystyle \frac{KT}{Z^2R_y}}\right)\right]`$ (12)
where $`\xi 1.82`$, $`Z`$ is the atomic number and $`R_y`$ is the Rydberg constant. Expressing the radius of the inner Lagrangian point in term of the binary parameters $`P_{b,h}`$ (the orbital period in hours), $`m_1`$ and $`m_2`$ (the masses of the NS and of the companion) and neglecting the term depending on the inverse of the distance (because $`DR_{L1}`$), it follows that:

$`\tau _{ff}=1.63\times 10^{22}{\displaystyle \frac{\dot{m}^2(X+0.5Y)^2\lambda _{21}^2\mathrm{ln}(\chi T_4^2\lambda _{21}Z^2)}{T_4^{3/2}v_8^2(m_1+m_2)P_{b,h}^2f_{orb}^3}}`$ (13)
where $`\chi =8.3\times 10^3`$ and $`f_{orb}=[10.462m_2/(m_1+m_2)]`$. $`\dot{m}`$ is in units of Myr-1, $`v_8`$ is the velocity of the wind in units of $`10^8`$ km s-1 (order of magnitude of the escape velocity from the system), $`\lambda _{21}`$ is the wavelength in units of 21 cm and $`T_4`$ is the gas temperature in units of $`10^4`$ K. Indeed $`T_4=1`$ is compatible with the kinetic energy of a plasma escaping the binary, but also $`T_4=10`$ could be appropriate, considering that the radiation of the pulsar should heat the surrounding gas. It is useful to write the mass loss from the donor star as a fraction $`g1`$ of the mass transfer $`\dot{m}_{switch}`$ (Burderi et. al 2001)

$`\dot{m}=g\dot{m}_{switch}=1.3\times 10^{12}g\mu _{26}^2P_3^{7/3}m_1^{1/2}.`$ (14)
The equations (13) and (14) allow us to compute the value of the parameter $`g`$ that gives an optical depth $`\tau _{ff}>1`$ (thus causing absorption at all orbital phases)

$`g>6.03P_{b,h}{\displaystyle \frac{T_4^{3/4}v_8(m_1+m_2)^{1/2}f_{orb}^{3/2}P_3^{7/3}m_1^{1/2}}{\mu _{26}^2(X+0.5Y)\lambda _{21}[\mathrm{ln}(\chi T_4^2\lambda _{21}Z^2)]^{1/2}}}.`$ (15)
For the NS–SXT to be in quiescence, $`g`$ must also satisfy

$`g<\dot{m}_{outb}/\dot{m}_{switch}9.07\times 10^2{\displaystyle \frac{L_{37}^{outb}R_6m_1^{3/2}}{\mu _{26}^2P_3^{7/3}}}.`$ (16)
Adopting $`\gamma =1,`$ $`v_8=1,`$ $`\lambda _{21}=1,`$ $`Z=1,`$ $`T_4=110,`$ the outburst luminosity $`L_{37}^{outb}=1`$ and assuming that the other parameters are those supposed typical of the NS–SXTs ($`m_1=1.4`$ M, $`m_2=0.6`$ M, $`\mu _{26}=1`$ and $`P_3=3`$, implying $`\dot{m}_{switch}=7.2\times 10^{14}`$ M yr-1), there is a large interval of values of $`g`$ ($`10\stackrel{<}{}g\stackrel{<}{}1000`$) which fulfill both the inequalities (15) and (16), provided the orbital period is not too long, $`P_{b,h}\stackrel{<}{}24`$. In summary, complete absorption of the radio signal at 1.4 GHz should be a common phenomenon during the quiescent phase of most NS–SXTs.

In particular, using the available values (see Table 1) of $`P_{b,h},`$ $`P_3`$ and $`L_{37}^{outb}`$ derived from X-ray and/or optical observations (holding the other unknown parameters at the reference values), the inequalities (15) and (16) are satisfied for the sources in our list. Hence, absorption in the gas engulfing the NS–SXTs during quiescence can explain the null result of our search at 1.4 GHz.

In this case, the most favorable moment for detecting a radio pulsar in a SXT would be just at the beginning of the quiescent phase, immediately after the ignition of the radio pulsar emission. At this point, the rate of infall should be a minimum. Later on, during the X-ray quiescent phase, the secondary star would resume a much higher rate of mass loss, not enough for restarting accretion on the NS surface, but enough to completely absorb the radio pulsar signal.

#### 4.3.1 Dispersion smearing

A pulsating signal from a pulsar can become undetectable not only due to absorption, but also if the pulse profile is broadened due to a variation of the dispersion measure during the observation. However, in the following we show that the dispersion smearing alone can hardly explain our results.

Assuming as in §4.3 a fully ionized spherically symmetric isothermal gas leaving the binary, the additional $`\mathrm{DM}_{\mathrm{loc}}`$ introduced by the local matter is

$`\mathrm{DM}_{\mathrm{loc}}={\displaystyle _{R_{cav}}^{R_{out}}}n_e𝑑r={\displaystyle _{R_{cav}}^{R_{out}}}{\displaystyle \frac{\rho (r)(X+0.5Y)}{m_p}}𝑑r`$ (17)
where $`R_{cav}`$ is the internal radius of the cavity that the pulsar energetic flux creates in the surrounding gas and $`R_{out}`$ is the external radius of this cavity, where the density of the gas $`\rho `$ becomes equal to the ISM density $`\rho _{ISM}2\times 10^{24}`$ g cm-3.

Assuming a simple density profile $`\rho r^2`$ and using the continuity equation for normalizing $`\rho `$ at its value at $`R_{out},`$ from integration of eq (17) it turns out:

$`\mathrm{DM}_{\mathrm{loc}}={\displaystyle \frac{\dot{m}(X+0.5Y)}{4\pi v_{wind}m_p}}\left({\displaystyle \frac{1}{R_{cav}}}{\displaystyle \frac{1}{R_{out}}}\right)=g\mathrm{\hspace{0.33em}1.2}\times 10^{18}{\displaystyle \frac{\mu _{26}^2P_3^{7/3}m_1^{1/2}}{v_8a_{ls}}}\mathrm{cm}^2`$ (18)
where $`a_{ls}`$ is the orbital separation in light seconds and the other quantities as in §4.3. The right hand of eq (18) has been calculated neglecting the $`1/R_{out}`$ term, writing $`\dot{m}=g\times \dot{m}_{switch}`$ (like already done in §4.3) and assuming $`R_{cav}`$ equal to the orbital separation. Adopting $`a_{ls}=1`$ and using the reference values of §4.3 for the other parameters, we derive

$`\mathrm{DM}_{\mathrm{loc}}=g\mathrm{\hspace{0.33em}0.025}\mathrm{pc}\mathrm{cm}^3`$ (19)
On one hand, this estimate ensures that our search has not been limited by additional dispersion due to matter released by the targeted systems: at most one can expect that $`g1000`$ (higher values would imply the occurrence of a new phase of accretion which would quench the pulsar radio emission, see previous section), and hence $`\mathrm{DM}_{\mathrm{loc}}\stackrel{<}{}25`$ pc cm-3, well within the range of our searched values of DM.

On the other hand, eq (15) shows that a true absoprtion of the signal can be avoided only for $`g\stackrel{<}{}10P_{b,h},`$ hence for $`\mathrm{DM}_{\mathrm{loc}}\stackrel{<}{}0.25P_{b,h}`$ pc cm-3. Given the total bandwidth of our observations, the latter inequalitie corresponds to a dispersive smearing of the pulse $`\mathrm{\Delta }t_{sm}\stackrel{<}{}0.2P_{b,h}`$ ms over the entire orbit. The segments of observations that we analysed, anyway, cover only a fraction of the total orbital period, lasting from $`\mathrm{\Delta }t_{sm}^{seg}4`$ to $`35`$ min. Hence, the expected smearing produced on every segment is typically of the order:

$`\mathrm{\Delta }t_{sm}^{seg}\mathrm{\Delta }t_{sm}{\displaystyle \frac{\mathrm{\Delta }t_{seg,h}}{P_{b,h}}}\stackrel{<}{}0.3\mathrm{\Delta }t_{seg,h}\stackrel{<}{}0.2\mathrm{ms}`$ (20)
where $`\mathrm{\Delta }t_{seg,h}`$ is the segment lenght in hours. Such values of $`\mathrm{\Delta }t_{seg,h}`$ (in agreement with what we obtain using the $`deltaDM`$ formula from Rasio et al. 1991) are not an obstacle for detecting the pulsating signal. In summary, the dispersion smearing can become a treath for recognizing the pulsating nature of the radio signal from our systems only for values of $`g`$ for which the signal is already strongly weakened by the free-free absorption. The role of the dispersion smearing could only be enhanced by the presence of strong time-variable clumping and inhomogeneities of the matter at all the orbital phases at which we have observed. In this unlikely case, observations in the continuum would be preferable.

## 5 Conclusion

We have searched for millisecond pulsations at 1.4 GHz in six neutron-star soft X-ray transient sources during their phases of quiescence. Despite the significant improvement of the sensitivity threshold compared to any similar previous experiment, no pulsed signal was detected.

If coherent radio emission from the rapidly rotating magnetized neutron star occurs in these systems, the probability of having missed it due to its weakness or beaming is only about 25%. Free-free absorption offers a viable alternative interpretation of our null result. We have shown that, during the quiescent phase, the companion to a NS–SXT can lose an amount of gas insufficient to quench the radio emission, but sufficient to completely absorb the radio signal.

N.D’A., A.P. and L.B. are supported by the Ministero della Ricerca Scientifica e Tecnologica (MURST). The Parkes radio telescope is part of the Australia Telescope which is funded by the Commonwealth of Australia for operation as a National Facility


text:
# Superconductivity and Field-Induced Magnetism in Pr2-xCexCuO4 Single Crystals

## Abstract

We report muon-spin rotation/relaxation ($`\mu `$SR) measurements on single crystals of the electron-doped high-$`T_c`$ superconductor Pr2-xCexCuO4. In zero external magnetic field, superconductivity is found to coexist with Cu spins that are static on the $`\mu `$SR time scale. In an applied field, we observe a $`\mu ^+`$-Knight shift that is primarily due to the magnetic moment induced on the Pr ions. Below the superconducting transition temperature $`T_c`$, an additional source of static magnetic order appears throughout the sample. This finding is consistent with antiferromagnetic (AFM) ordering of the Cu spins in the presence of vortices. We also find that the temperature dependence of the in-plane magnetic penetration depth $`\lambda _{ab}`$ in the vortex state resembles that of the hole-doped cuprates at temperatures above $`0.2`$ $`T_c`$.

While there now exists a large body of convincing experimental work on high-$`T_c`$ superconductors with hole-type carriers, the intrinsic properties of the electron-doped cuprates $`R_{2x}`$CexCuO4 ($`R`$ La, Pr, Nd, Sm or Eu) have remained very elusive. Part of the problem stems from the difficulty of preparing single phase superconducting samples. An additional complication is the presence of both Cu and rare-earth ($`R`$) moments. The interplay between these two magnetic sublattices has been studied extensively in the undoped parent compounds $`R_2`$CuO4 Sachi:97 . In Ce-doped samples, there is the possibility that the magnetic exchange interactions involving the CuO2 planes play an important role in superconductivity. There is also some uncertainty about the symmetry of the superconducting order parameter. Although, recent phase sensitive Tsuei:00  and angle-resolved photoemission Armitage:01  experiments are consistent with $`d`$-wave pairing symmetry, measurements of thermodynamic quantities such as the in-plane magnetic penetration depth $`\lambda _{ab}`$, generally do not show the expected linear temperature dependence at low $`T`$ that is characteristic of a “clean” superconductor. Many of the early results for $`\lambda _{ab}(T)`$ in electron-doped cuprates were obtained in the Meissner phase of Nd2-xCexCuO4 (NCCO) thin films and single crystals. While these results favored $`s`$-wave symmetry Wu:93 ; Andreone:94 ; Anlage:94 , it has since been recognized that the paramagnetism of the Nd ions strongly affects the low-$`T`$ behavior of $`\lambda _{ab}(T)`$ Cooper:96 ; Alff:99 ; Prozorov:00a ; Kokales:00 . Consequently, attention has shifted primarily to the Pr2-xCexCuO4 (PCCO) system, where crystal electric field (CEF) splitting of the Pr3+ $`J=4`$ manifold results in a nonmagnetic singlet ground state. Unfortunately, more recent measurements of $`\lambda _{ab}(T)`$ in PCCO thin films and crystals using a variety of techniques have not yielded consistent results Alff:99 ; Kokales:00 ; Prozorov:00a ; Ku:01 ; Skinta:02a ; Skinta:02b ; Biswas:02 .

To avoid extrinsic effects related to the sample surface, we have utilized the $`\mu `$SR technique. $`\mu `$SR is a local probe of the bulk and is one of the few techniques that can measure $`\lambda _{ab}(T)`$ in the vortex state — sensitive to the supercurrents circulating around the vortex cores, rather than the screening currents which flow near the sample surface. Attempts to accurately measure $`\lambda _{ab}(T)`$ in NCCO by $`\mu `$SR have been precluded by the considerable Nd-moment contribution to the muon-spin depolarization rate Luke:97 . In this Letter, we report on the first $`\mu `$SR study of superconducting PCCO single crystals.

We studied three single crystals of PCCO grown by a directional solidification technique in Al2O3 crucibles using a CuO-based flux Peng:91 . Reduction of oxygen to induce superconductivity was achieved by encapsulating each single crystal in polycrystalline PCCO in the presence of flowing Ar at 900-1000 C (Ref. Brinkmann:96 ). Here we report on representative data from one of the single crystals, noting that qualitatively similar results were obtained in a partial $`\mu `$SR study of the other two. The crystal was 0.07 mm thick, having an $`\widehat{a}`$-$`\widehat{b}`$ plane surface area of $`6.5`$ mm2 and a mass of 3.74 mg. Although resistivity measurements indicate a $`T_c`$ value of 25(1) K, bulk susceptibility $`\chi ^{}`$ measurements show that the diamagnetic signal assumes a constant value below $`16`$ K (see Fig. 1 inset).

The measurements were carried out on the M15 and M20B positive muon ($`\mu ^+`$) beam lines at TRIUMF, Canada. In a $`\mu `$SR experiment the spin of the implanted $`\mu ^+`$ precesses at a frequency $`\omega _\mu =\gamma _\mu B_\mu `$, where $`B_\mu `$ is the local field at the $`\mu ^+`$ site and $`\gamma _\mu =13.5534`$ kHz G-1 is the muon gyromagnetic ratio. The PCCO single crystals are the smallest samples studied to date by conventional $`\mu `$SR. Consequently, a special arrangement of scintillator detectors inside a He gas-flow cryostat was needed to eliminate the contribution from muons that did not stop in the sample. Unfortunately, this setup is not possible in a dilution refrigerator, so 2.3 K is the lowest temperature that could be reached. Measurements were taken both in zero external field (ZF) and in a transverse field (TF) geometry with $`H`$ directed perpendicular to the CuO2 planes.

In ZF, the muon-spin polarization $`P(t)`$ is relaxed by magnetic moments of electronic and nuclear origin. As shown in Fig. 1, the relaxation rate of the ZF-$`\mu `$SR signal in PCCO increases with decreasing $`T`$. The absence of discrete frequency oscillations indicates that there is no onset of spontaneous magnetic order at temperatures above 2.3 K. Additional measurements carried out in a longitudinal-field geometry indicate that the muon spin is depolarized by randomly oriented internal fields which are static on the $`\mu `$SR time scale. Since the Pr ions have a nonmagnetic singlet ground state and the nuclear contribution to $`P(t)`$ is small, we attribute the source of the magnetism to disordered Cu spins.

TF-$`\mu `$SR and magnetization measurements were carried out under both field-cooled (FC) and zero-field cooled (ZFC) conditions. Typical asymmetry spectra are shown in the inset of Fig. 2. In the ZFC case, pinning at the sample edges prevents flux from entering the bulk at $`T=2.3`$ K and $`H<300`$ Oe. Thus, the ZFC time spectrum in Fig. 2 resembles that observed in ZF. We note that this is also the case in high-quality YBa2Cu3O7-δ single crystals. Above 300 Oe, flux fully penetrates the sample at $`T=2.3`$ K, but pinning centers prevent the formation of an equilibrium vortex lattice configuration. On the other hand, a well-ordered vortex lattice is achieved in the FC procedure. Fast Fourier transforms (FFT) of the corresponding muon-spin precession signals at $`H=91`$ Oe are shown in Fig. 2. The FFT provides an approximate picture of the internal magnetic field distribution $`n(B)`$ Sonier:00 . Above $`T_c`$, the linewidth is due to the electronic and nuclear magnetic moments. Below $`T_c`$, the lineshape is further broadened and becomes asymmetric as a result of the inhomogeneous field distribution created by a lattice of vortices. Because the contribution of the magnetic moments to the width of $`n(B)`$ increases with increasing $`H`$, we have restricted the current study to low magnetic fields.

The stopping site of the $`\mu ^+`$ has previously been identified in the related undoped parent compound Nd2CuO4 as near an O atom midway between adjacent CuO2 layers Luke:90 . Consistent with this site assignment, the TF-$`\mu `$SR signal in PCCO shows a single well resolved signal with an average frequency shifted relative to the Larmor precession frequency of $`\mu ^+`$ in vacuum. The corresponding $`\mu ^+`$-Knight shift is

$$K_\mu ^{}=\frac{B_0\mu _0H}{\mu _0H}4\pi \left(\frac{1}{3}N\right)\rho _{\mathrm{mol}}\chi ^{},$$
(1)
where $`B_0`$ is the average internal field sensed by the muons, the second term is a correction for Lorentz and bulk demagnetization fields, $`\rho _{\mathrm{mol}}=0.01744`$ mol/cm3 is the molar density of PCCO, and $`N1`$ is the demagnetization factor for a thin plate-like crystal. Figure 3 shows that $`K_\mu ^{}`$ scales linearly with $`\chi ^{}`$ above $`T_c`$, indicating that the relative frequency shift is not induced by the $`\mu ^+`$. In the normal state there are several contributions to $`K_\mu ^{}`$. Susceptibility measurements have established that the field-induced moment on the Pr ions dominates the magnetic response of PCCO, which depends little on Ce-doping Hundley:89 . Furthermore, as shown in the inset of Fig. 3, $`\chi `$ is highly anisotropic due to strong crystalline electric-field (CEF) effects. For $`𝐇𝐜`$, there are smaller contributions to $`\chi ^{}`$ from the tilting of the Cu moments out of the $`\widehat{a}`$-$`\widehat{b}`$ plane, Cu2+-O2--Pr3+ superexchange interactions and from the polarization of the conduction electrons Foldeaki:94 . The Pauli paramagnetic susceptibility $`\chi _0`$ of the conduction electrons gives rise to a $`T`$-independent Knight shift, $`K_0=A_0\chi _0`$, where $`A_0`$ is the contact hyperfine coupling constant. The field induced moment on the Pr ions results in a $`T`$-dependent Knight shift $`K_f^{}`$ consisting of two contributions: (i) the dipole-dipole interaction between the localized Pr $`4f`$-moments and the $`\mu ^+`$, and (ii) an indirect Rudermann-Kittel-Kasuya-Yosida (RKKY) interaction, producing a spin polarization of the conduction electrons at the $`\mu ^+`$ site. Assuming the Cu-moment contributions to be negligible, $`K_\mu ^{}`$ at the axial symmetric $`\mu ^+`$-site is given by

$$K_\mu ^{}K_0+K_f^{}=K_0+(A_\mathrm{c}+A_{\mathrm{dip}}^{zz})\chi _f^{},$$
(2)
where $`A_\mathrm{c}`$ and $`A_{\mathrm{dip}}^{zz}`$ are the contact hyperfine and dipolar coupling constants, respectively, and $`\chi _f^{}\chi ^{}\chi _0`$. At the $`\mu ^+`$ site we calculate $`A_{\mathrm{dip}}^{zz}=663.6`$ Oe/$`\mu _B`$. The solid line in Fig. 3 is a fit to Eq. (2), yielding $`A_\mathrm{c}=3231`$ Oe/$`\mu _B`$ and $`K_0>4480`$ ppm.

Below $`T_c`$, there is a substantial increase of $`B_0`$ that nearly coincides with the increase of the diamagnetic signal under FC conditions (see Fig. 4). This cannot be explained by the reduction of $`\chi _0`$ that arises from the formation of Cooper pairs. We first considered the possibility that the increased field is a manifestation of the so-called paramagnetic Meissner effect Sigrist:95 , but the diamagnetic response observed in both the FC and ZFC magnetization does not support this interpretation. A second possible origin, thought to be responsible for magnetorestriction enhancements Zieglowski:88  and large diamagnetic shifts of $`B_0`$ Lichti:91  in the superconducting state of the $`R`$Ba2Cu3O7-δ system, is the $`R`$-moments induce screening currents in the CuO2 layers. However, here the Pr-moment is induced by the applied field, and thus is reduced below the normal-state value in regions well beyond the vortex cores. This is inconsistent with the FFTs in Fig. 2, which imply that all muons stopping in the sample see an increase in the local field. A third possible origin is that the vortices nucleate static Cu-spin order, as has been observed in the superconducting state of underdoped La2-xSrxCuO4 Lake:02 . We note that while the difference between $`B_0`$ in the superconducting and normal states is reduced with increasing $`H`$, this does not imply that the additional source of field below $`T_c`$ weakens. For example, the solid curve in Fig. 4 is a fit assuming $`B_0(T)=[(B_0^\mathrm{N})^2+(B_{})^2]^{1/2}`$, where $`B_0^\mathrm{N}`$ is the average internal field in the normal state and $`B_{}43`$ G and 28 G, at 5 K and 10 K, respectively. This indicates that the additional field $`B_{}`$ that appears at the $`\mu ^+`$-site is primarily directed in the $`\widehat{a}`$-$`\widehat{b}`$ plane. Calculations show that this is consistent with the La2NiO4 spin-structure that has been observed with $`\mu `$SR in the parent compound Nd2CuO4 at low $`T`$ Luke:90 . Thus, long-range order of the Cu spins appears to be stabilized in PCCO by a low density of vortices, perhaps due to the close proximity of the superconducting and AFM phases.

The in-plane magnetic penetration depth $`\lambda _{ab}`$ can be determined from the TF-$`\mu `$SR time spectra as described in Ref. Sonier:00 . In the normal state, the muon-spin precession signal is well described by the polarization function $`P(t)=e^{(\sigma t)^K}\mathrm{cos}(\omega _\mu t+\varphi )`$, where $`\beta 1.6`$ and $`\sigma `$ is the temperature-dependent depolarization rate. The TF-$`\mu `$SR time spectra below $`T_c`$ were well fit to

$$P(t)=e^{(\sigma _\mathrm{v}t)^\beta }n_\mathrm{v}(B)\mathrm{cos}(\gamma _\mu Bt+\varphi )𝑑B,$$
(3)
where $`n_\mathrm{v}(B)`$ is the field distribution of an hexagonal vortex lattice derived from Ginzburg-Landau theory, and $`\sigma _\mathrm{v}`$ is the depolarization rate due primarily to the effects of the magnetic moments — which occur on a length scale that is 103 times smaller than $`\lambda _{ab}`$. Fits at low $`T`$ which explicitly included a variable transverse field component $`B_{}`$, gave $`\beta 1.2`$ and a diamagnetic shift for the $`c`$-axis component of field. However, $`\lambda _{ab}(T)`$ could not be reliably obtained in this manner due to the decreased sensitivity to $`B_{}`$ with increasing $`T`$ and the competition with other fitting parameters. Our analysis using Eq. (3) shows that $`\sigma _\mathrm{v}`$ scales as $`1/(T\theta )`$, where $`\theta =18(5)`$ K. At low $`H`$, only a small fraction of the implanted muons stop near the vortex cores. As a result, the analysis is not very sensitive to the value of the coherence length $`\xi _{ab}`$. For example, increasing $`\xi _{ab}`$ from 30 Å to 60 Å changes $`\lambda _{ab}(0)`$ by less than 2 %. Figure 5 shows the temperature dependence of $`\lambda _{ab}^2`$. The absence of data below $`T=2.3`$ K forbids an accurate determination of the limiting temperature dependence of $`\lambda _{ab}^2(T)`$. However, above this $`\lambda _{ab}^2(0)/\lambda _{ab}^2(T)`$ shows reasonable agreement with that determined by $`\mu `$SR in the hole-doped systems La2-xSrxCuO4 and YBa2Cu3O7-δ. The solid curve in the inset of Fig. 5 is a fit of the PCCO data to $`\lambda _{ab}^2(T)=\lambda _{ab}^2(0)[1(T/T_c)^2]`$, yielding $`T_c=15.9(2)`$ K and $`\lambda _{ab}(0)=3369(73)`$ Å. The values of $`T_c`$ and $`\lambda _{ab}(0)`$ indicate that the bulk of our sample is primarily underdoped. For example, Meissner state measurements in Ref. Skinta:02b  on an underdoped PCCO film reported $`\lambda _{ab}=3100`$ Å. This same study showed evidence for a crossover from $`s`$-wave to $`d`$-wave behavior in the underdoped regime.

In conclusion, we have observed the onset of static magnetic order in the superconducting state of underdoped PCCO single crystals with a field applied perpendicular to the CuO2 plane. This result is consistent with vortex-induced AFM ordering of the Cu spins throughout the sample. In addition, our measurements of $`\lambda _{ab}^2(T)`$ in the vortex state appear consistent with hole-doped cuprates down to $`0.2`$ $`T_c`$. However, a unique determination of the low-temperature behavior by $`\mu `$SR awaits the availability of larger single crystals.

We are especially grateful to R.F. Kiefl for technical assistance and insightful discussions. This work was supported by the Natural Sciences and Engineering Research Council of Canada, and in the United States by National Science Foundation Grant DMR 01-02350.