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# Testing Leptonic 𝑆𝑈(2) Horizontal Symmetry Using Neutrino Mixings

## I Introduction

As the outline of the neutrino mixings pattern is beginning to emerge from recent solar and atmospheric neutrino experiments, understanding the neutrino mass matrix has become one of the central problems in theoretical particle physics. On the phenomenological side, while the mixings responsible for both solar and atmospheric neutrino oscillations seem to be fairly large (unlike quark mixings), the pattern of masses seem to remain undetermined. Three generic patterns that can be considered as equally acceptable at present are masses (i) with normal hierarchy i.e $`m_1m_2m_3`$; (ii) inverted hierarchy i.e. $`m_1m_2m_3`$ and (iii) degenerate i.e. $`m_1m_2m_3`$. Once some of the contemplated long baseline neutrino experiments and high precision searches for neutrinoless double beta decay are carried out***If the recent reports of a positive signal for $`\beta \beta _{0\nu }`$ are confirmed, the degenerate mass pattern will be picked as the unique choice and models of the type discussed here will be disfavored., the true mass pattern will be revealed. From a theoretical point of view, each pattern could be an indication of a different symmetry of physics beyond the standard model. Therefore, before those experiments are carried out, it is of interest in our opinion to explore the symmetry approach to understanding neutrino masses and isolate their tests. Combination of the future experimental results and the theoretical explorations can then decide the nature of physics beyond the standard model.

The key issues that need to be understood are: (i) the large atmospheric and solar mixing angles; (ii) the smallness of the ratio $`\mathrm{\Delta }m_{}^2/\mathrm{\Delta }m_A^2`$ and (iii) the smallness of the mixing $`U_{e3}`$.

One symmetry that predicts in zeroth order the correct mixing pattern i.e. large solar and atmospheric angles and zero $`U_{e3}`$ is the combination of the three leptonic symmetries of the standard model i.e. $`L_eL_\mu L_\tau `$; it picks the inverted hierarchy pattern and an exact bimaximal mixing. However in the symmetry limit it predicts that $`\mathrm{\Delta }m_{}^2=0`$ while $`\mathrm{\Delta }m_A^2`$ is predicted to be nonzero. This, therefore raises the possibility that, one may be able to understand the second puzzle in such models. In fact if one includes small breakings of the $`L_eL_\mu L_\tau `$ symmetry either radiatively or otherwise, it leads to quite interesting and testable neutrino mixing patterns. Because of this a great deal of attention has recently been focussed on it.

In order to have a deeper theoretical understanding of the inverted neutrino mass pattern with near bimaximal mixing or the $`L_eL_\mu L_\tau `$ symmetry, one approach would be to study it within a seesaw framework where the smallness of the neutrino masses is understood in a very simple manner. It appears that the most convenient way to arrive at the inverted pattern with two large mixings in a seesaw framework is to work with two heavy right handed neutrinos rather than three as is dictated by quark lepton symmetry. In a recent paper, we pointed out that if the standard model is extended by the inclusion of an $`SU(2)_H`$ symmetry acting on two lepton families, freedom from global anomalies require that there be two right handed neutrinos at the scale where $`SU(2)_H`$ symmetry is broken. We further showed that (i) the presence of the $`SU(2)_H`$ symmetry also helps in the understanding of the near bimaximal mixing pattern; (ii) the smallness of $`\mathrm{\Delta }m_{}^2/\mathrm{\Delta }m_A^2`$ is associated with a symmetry related to the horizontal symmetry. Needless to say that while it may appear that theory does not have quark lepton symmetry, it could be easily restored by including the third right handed neutrino and making it heavier than the seesaw scale. In this case the low energy theory near the horizontal symmetry breaking scale looks effectively like a theory with two right handed neutrinos.

It is the purpose of this paper to analyze this class of models in more detail and point out that in a specific supersymmetric realization of the model there is an experimentally interesting relation between the $`U_{e3}`$ parameter, the ratio $`\mathrm{\Delta }m_{}^2/\mathrm{\Delta }m_A^2`$ and the solar mixing angle $`\theta _{}`$ i.e. $`sin\theta _{}`$ as follows: $`U_{e3}^2cos2\theta _{}=\frac{\mathrm{\Delta }m_{}^2}{2\mathrm{\Delta }m_A^2}+O(U_{e3}^4,(m_e/m_\mu )^2)`$. Apart from being experimentally testable, this relation also provides a natural explanation of why the $`\mathrm{\Delta }m_{}^2`$ is so much smaller than $`\mathrm{\Delta }m_A^2`$.

We have organized this paper as follows: in section 2, we give arguments to suggest that within a seesaw framework for neutrino masses, normal or inverted hierarchical patterns prefer that one of the right handed neutrinos is much heavier than the others. In section 3, we present the basic ingredients of the model which is an $`SU(2)_H`$ extension of the minimal supersymmetric standard model (MSSM); in sec. 4, we discuss the predictions for neutrino mixings in the model and derive the main result of the paper, which is the relation between the neutrino oscillation parameters discussed above. Section 5 is devoted to some additional comments and in sec. 6, we give a summary of our results and conclusions.

## II Why $`SU(2)_H`$ ?

In this section, we will argue that for the normal or inverted hierarchy case, it is quite possible that two of the right handed neutrinos are lighter than the third one. This can be seen as follows. Let us assume that the smallness of the neutrino masses owes its origin to the seesaw mechanism:

$`_\nu =M_DM_R^1M_D^T`$ (1)
Inverting this relation with the assumption that the Dirac mass matrix is diagonal, one can express $`M_R`$ in terms of the neutrino mixing matrix elements and the neutrino masses $`m_i`$ and one has:

$`_{R,\alpha \beta }=m_{D,\alpha }\mu _{\alpha \beta }^1m_{D,\beta }`$ (2)
with

$`\mu _{\alpha \beta }^1={\displaystyle \underset{i}{}}U_{\alpha i}U_{\beta i}m_i^1`$ (3)
where $`𝐔`$ is the neutrino mixing matrix. Now observe that for both the normal and inverted hierarchy case, the lightest neutrino could have mass even equal to zero. Clearly as its mass gets closer to zero, the RH neutrino matrix takes the factorized form

$`M_R=m_1^1|11|`$ (4)
where $`|1=(U_{11}m_{D1}^2,U_{21}m_{D1}m_{D2},U_{31}m_{D1}m_{D3})`$ and clearly the smaller $`m_1`$ is, the heavier the heaviest right handed neutrino becomes. On the other hand the masses of the other two RH neutrinos are not free since they are linked to observed $`\mathrm{\Delta }m_{}^2`$ and $`\mathrm{\Delta }m_A^2`$. In this sense, we see that for both the normal and the inverted hierarchy case, it is quite likely that there is a separation of the RH neutrino levels. In fact, in the case of inverted hierarchy, the two “heavy” left handed neutrinos are nearly degenerate, the two lighter RH neutrinos are likely to be very close in mass, which then makes the case for a symmetry associated with it. In ref. we argued that the relevant symmetry is $`SU(2)_H`$ symmetry, which by group theory argument alone puts two of the RH neutrinos lighter than the third one. As discussed in ref., this happens because, when the local horizontal symmetry acts on the charged right handed leptons, freedom from global anomalies indeed requires that there be two RH neutrinos transforming as a doublet under $`SU(2)_H`$. Their mass after $`SU(2)_H`$ symmetry breaking then would be of order of the horizontal symmetry breaking scale. The third RH neutrino being unconstrained by this symmetry would have a much higher mass.

## III Details of the model and mass matrices for leptons

Our model is based on the gauge group $`G_{STD}\times SU(2)_H`$ with supersymmetry. In Table I the assignment of the leptons and Higgs superfields under the gauge group $`SU(3)_c\times SU(2)_L\times U(1)_Y\times SU(2)_HG_{STD}\times SU(2)_H`$ is given.

Table I

| Particles | $`G_{STD}\times SU(2)_H`$ |
| --- | --- |
|  | Quantum numbers |
| $`\mathrm{\Psi }(L_e,L_\mu )`$ | (1,2,-1,2) |
| $`L_\tau `$ | (1,2,-1,1) |
| $`E^c(\mu ^c,e^c)`$ | (1,1,-2, 2) |
| $`\tau ^c`$ | (1,1,-2, 1) |
| $`N^c(\nu _\mu ^c,\nu _e^c)`$ | (1,1,0,2) |
| $`\nu _\tau ^c`$ | (1,1,0,1) |
| $`\chi _H\left(\begin{array}{cc}\chi _1& \chi _2\end{array}\right)`$ | (1, 1, 0, 2) |
| $`\overline{\chi }_H(\overline{\chi }_1,\overline{\chi }_2)`$ | (1,1,0,2) |
| $`H_u`$ | (1,2,1,1) |
| $`H_d`$ | (1,2,-1,1) |
| $`\mathrm{\Delta }_H`$ | (1,1,0,3) |

Table caption: Representation content of the various fields in the model under the gauge group $`G_{STD}\times SU(2)_H`$.

Here $`L_{e,\mu ,\tau }`$ denote the left handed lepton doublet superfields. The quarks can transform as singlets or doublets of $`SU(2)_H`$ and are not mentioned since it does not mix affect the lepton masses which is the main focus of this paper. We arrange the Higgs potential in such a way that the $`SU(2)_H`$ symmetry is broken by $`<\chi _1>=v_{H1};<\chi _2>=v_{H2}`$ and $`<\mathrm{\Delta }_{H,3}>=v_H^{}`$, where $`v_H,v_H^{}v_{wk}`$. Note that we have used the $`SU(2)_H`$ symmetry to align the $`\mathrm{\Delta }_H`$ vev along the $`I_{H,3}`$ direction. At the weak scale, the neutral components of the fields $`H_u`$ and $`H_d`$ acquire nonzero vev’s and break the standard model symmetry down to $`SU(3)_c\times U(1)_{em}`$. We denote these vev’s as follows: $`<H_u^0>=\kappa _0`$ and $`<H_d^0>=\kappa _0cot\beta `$ ; Clearly $`\kappa _0`$ is expectd to have values in few to 100 GeV range. All the vev’s and couplings are taken to be real.

Note that $`<\mathrm{\Delta }_H>0`$ breaks the $`SU(2)_H`$ group down to the $`U(1)_{L_eL_\mu }`$ group which is further broken down by the $`\chi _H`$ vev. Since the renormalizable Yukawa interactions do not involve the $`\chi _H`$ field, this symmetry ($`L_eL_\mu `$) is also reflected in the right handed neutrino mass matrix and plays a role in leading to the bimaximal mixing pattern.

To study the pattern of neutrino masses and mixings, let us first note that if we included $`\nu _{\tau R}`$ in the theory, a bare mass for the $`\nu _{\tau ,R}`$ field is allowed at the tree level unconstrained by any symmetries. This mass can therefore be arbitrarily large and $`\nu _{\tau ,R}`$ will decouple from the low energy spectrum. We will work in this limit of decoupled $`\nu _{\tau R}`$ and write down the gauge invariant Yukawa superpotential involving the remaining leptonic fields.

$`𝒲_Y=h_1(L_eH_u\nu _e^c+L_\mu H_u\nu _\mu ^c)+h_0L_\tau (\nu _\mu ^c\chi _2+\nu _e^c\chi _1)H_u/M`$ (5)
$`ifN^{cT}\tau _2\tau 𝚫_𝐇N^c+{\displaystyle \frac{h_1^{}}{M}}(L_e\chi _2L_\mu \chi _1)H_d\tau ^c`$ (6)
$`+{\displaystyle \frac{h_4^{}}{M}}L_\tau H_d(\mu ^c\chi _2+e^c\chi _1)+h_3^{}L_\tau H_d\tau ^c+h_2^{}(L_ee^c+L_\mu \mu ^c)H_d`$ (7)
$`<\mathrm{\Delta }_H^0>=v_H^{}`$ directly leads to the $`L_eL_\mu `$ invariant $`\nu _{eR}\nu _{\mu R}`$ mass matrix at the seesaw scale. The $`\chi _H`$ vev contributes to this mass matrix only through nonrenormalizable operators and we assume those contributions to be negligible. We also do not include any term where $`\mathrm{\Delta }_H`$ and $`\overline{\chi }_H`$ couple to light fields. Since in supersymmetric theories, the superpotential does not receive any loop induced corrections due to the nonrenormalization theorem, conclusions derived on the basis of the above potential are stable under radiative corrections. It must however be noted that even if such couplings were allowed, there would be no change in the predictions since the effects would be small. Similarly there will also be some small contributions from the $`\nu _{\tau R}`$ sector if we did not decouple it completely. We ignore these contributions in our analysis. Further, we define $`\kappa _{1,2}=\frac{<\chi _{1,2}>\kappa _0}{M}`$ taken to of order 10 GeV or so.

To study neutrino mixings, we write down the $`5\times 5`$ seesaw matrix for neutrinos:

$`M_{\nu _L,\nu _R}=\left(\begin{array}{ccccc}0& 0& 0& h_0\kappa _0& 0\\ 0& 0& 0& 0& h_0\kappa _0\\ 0& 0& 0& h_1\kappa _1& h_1\kappa _2\\ h_0\kappa _0& 0& h_1\kappa _1& 0& fv_H^{}\\ 0& h_0\kappa _0& h_1\kappa _2& fv_H^{}& 0\end{array}\right)`$ (13)
After seesaw diagonalization, it leads to the light neutrino mass matrix of the form:

$`_\nu =M_DM_R^1M_D^T`$ (14)
where $`M_D=\left(\begin{array}{cc}h_0\kappa _0& 0\\ 0& h_0\kappa _0\\ h_1\kappa _1& h_1\kappa _2\end{array}\right)`$; $`M_R^1=\frac{1}{fv_H^{}}\left(\begin{array}{cc}0& 1\\ 1& 0\end{array}\right)`$. The resulting light Majorana neutrino mass matrix $`_\nu `$ is given by:

$`_\nu ={\displaystyle \frac{1}{fv_H^{}}}\left(\begin{array}{ccc}0& (h_0\kappa _0)^2& h_0h_1\kappa _0\kappa _2\\ (h_0\kappa _0)^2& 0& h_0h_1\kappa _0\kappa _1\\ h_0h_1\kappa _0\kappa _2& h_0h_1\kappa _0\kappa _1& 2h_1^2\kappa _1\kappa _2\end{array}\right)`$ (18)
To get the physical neutrino mixings, we also need the charged lepton mass matrix defined by $`\overline{\psi }_L_{\mathrm{}}\psi _R`$. This is given in our model by:

$`_{\mathrm{}}=cot\beta \left(\begin{array}{ccc}h_2^{}\kappa _0& 0& h_1^{}\kappa _2\\ 0& h_2^{}\kappa _0& h_1^{}\kappa _1\\ h_4^{}\kappa _1& h_4^{}\kappa _2& h_3^{}\kappa _0\end{array}\right)`$ (22)
In order to study physical neutrino mixings, we must diagonalize the $`_\nu `$ and $`M_{\mathrm{}}`$ matrices. We discuss this in the next section.

## IV A relation between Neutrino mixings and smallness of $`\mathrm{\Delta }m_{}^2/\mathrm{\Delta }m_A^2`$

In order to discuss the physical neutrino mixings, we need to work in a basis where the charged lepton mass matrix is diagonal. Defining the matrices that diagonalize the charged lepton mass matrix as $`D_{\mathrm{}}=U_{\mathrm{}}^{(L)}M_{\mathrm{}}U_{\mathrm{}}^{(R)}`$, we get

$`U_{\mathrm{}}^{(L)}=\left(\begin{array}{ccc}s_1& c_1& 0\\ c_\beta c_1& c_\beta s_1& s_\beta \\ s_\beta c_1& s_\beta s_1& c_\beta \end{array}\right)`$ (26)
where $`tan2\beta 2\sqrt{\frac{h_1^{}}{h_4^{}}}\sqrt{m_\mu /m_\tau }`$ and $`sin\theta _1s_1=\frac{\kappa _1}{\sqrt{\kappa _1^2+\kappa _2^2}}`$. This matrix receives small corrections of order $`m_e/m_\mu `$, which are not important for our considerations.

In order to discuss neutrino mixings, we write down the orthogonal matrix $`U_\nu `$ that diagonalizes the $`_\nu `$ for $`\kappa _10`$. Defining two angles $`\theta _{1,2}`$:

$`sin\theta _1s_1={\displaystyle \frac{\kappa _1}{\sqrt{\kappa _1^2+\kappa _2^2}}}`$ (27)
$`sin\theta _2s_2={\displaystyle \frac{h_0\kappa _0}{\sqrt{h_0^2\kappa _0^2+h_1^2(\kappa _1^2+\kappa _2^2)}}}`$ (28)
the neutrino mass matrix can be written in terms of these angles as:

$`_\nu =\sqrt{\mathrm{\Delta }m_A^2}\left(\begin{array}{ccc}0& s_2^2& c_2s_2c_1\\ s_2^2& 0& c_2s_2s_1\\ c_2s_2c_1& c_2s_2s_1& 2c_2^2s_1c_1\end{array}\right)`$ (33)
The neutrino mass matrix $`_\nu `$ has a zero eigenvalue since one of the three right handed neutrinos was not protected by the $`SU(2)_H`$ symmetry and had decoupled. Identifying this with the third neutrino we have its mass $`m_3=0`$. The correspnding third-neutrino eigenvector is easy to evaluate exactly and is $`(c_2s_1,c_2c_1,s_2)`$.

The orthogonal matrix that diagonalizes $`_\nu `$ (i.e. $`U_\nu ^{}_\nu U_\nu =D_\nu `$) is given by

$`U_\nu =\left(\begin{array}{ccc}c_1c^{}s_1s_2s^{}& c_1s^{}+s_1s_2c^{}& c_2s_1\\ s_1c^{}c_1s_2s^{}& s_1s^{}+c_1s_2c^{}& c_2c_1\\ c_2s^{}& c_2c^{}& s_2\end{array}\right)`$ (37)
where $`s^{}=sin\theta ^{}`$ with $`\theta ^{}`$ given by $`tan2\theta ^{}=\frac{2s_2(c_1^2s_1^2)}{(1+s_2^2)2s_1c_1}`$. Note that as $`s_10`$, $`\theta ^{}\pi /4`$. Note that the third neutrino eigenvector is the third column of the above matrix.

The final physical neutrino mixing matrix is then given by $`𝐔=U_{\mathrm{}}^{(L)}U_\nu `$, where $`U_{\mathrm{}}^{(L)}`$ is defined in the previous section. Combining this with the neutrino mixing matrix $`U_\nu `$, we get the final physical neutrino mixing matrix $`U`$ to be

$`𝐔=\left(\begin{array}{ccc}s_2s^{}& s_2c^{}& c_2\\ (c^{}c_\beta +c_2s^{}s_\beta )& (c_\beta s^{}s_\beta c_2c^{})& s_2s_\beta \\ (c^{}s_\beta c_2s^{}c_\beta )& (c_2c^{}c_\beta +s^{}s_\beta )& s_2c_\beta \end{array}\right)`$ (41)
To see the consistency of the model, we first note that $`U_{e3}=c_20.16`$ from the reactor neutrino data. This implies $`s_21`$ and for $`\kappa _1\kappa _2\kappa _0`$, $`\frac{h_1\kappa _2}{h_0\kappa _0}0.16`$. To fit the atmospheric data, we then require, $`s_\beta 1/\sqrt{2}`$. This can be easily satisfied by requiring the Yukawa couplings to have a hierarchy $`h_4^{}/h_1^{}2\sqrt{\frac{m_\mu }{m_\tau }}`$.

The solar mixing angle $`(sin\theta _{}U_{e2})`$, for $`s_21`$ is given by

$`tan2\theta _{}tan2\theta ^{}cot2\theta _1`$ (42)
This implies that

$`sin2\theta _{}(c_1^2s_1^2)={\displaystyle \frac{\kappa _2^2\kappa _1^2}{\kappa _2^2+\kappa _1^2}}`$ (43)
Coming to neutrino masses $`m_1,m_2`$ and $`m_3`$, in the absence of $`\kappa _1\kappa _2`$ we have $`m_1=m_2=h_0\kappa _0`$ and $`m_3=0`$. The solar mass squared difference $`\mathrm{\Delta }m_{}^2=m_1^2m_2^2`$ is generated when $`\kappa _1`$ is turned on while the atmospheric mass squared difference $`\mathrm{\Delta }m_A^2m_1^2m_2^2h_0^2\kappa _0^2`$ gets a small correction. In the limit of $`s_21`$, one can write $`\mathrm{\Delta }m_{}^2`$ in terms of $`\kappa _i`$ as follows:

$`{\displaystyle \frac{\mathrm{\Delta }m_{}^2}{\mathrm{\Delta }m_A^2}}={\displaystyle \frac{4h_1^2\kappa _1\kappa _2}{\sqrt{h_0^2\kappa _0^2+h_1^2(\kappa _1^2+\kappa _2^2)}}}`$ (44)
It is then clear that if we choose $`\kappa _{1,2}\kappa _0`$ along with a mild hierarchy among the Yukawa parameters $`h_{1,0}`$, we can obtain the desired solar neutrino mass squared difference. This leaves the relative valus of $`\kappa _1`$ with respect to $`\kappa _2`$ unaffected. Appropriately choosing their relative values, we can get the solar mixing angle to be smaller than maximal as indicated by the central value for it.

Combining the above equations, we get for $`U_{e3}1`$,

$`U_{e3}^2cos2\theta _{}={\displaystyle \frac{\mathrm{\Delta }m_{}^2}{2\mathrm{\Delta }m_A^2}}+O(U_{e3}^4,(m_e/m_\mu )^2)`$ (45)
This equation is the major result of the paper and it is a direct consequence of the $`SU(2)_H`$ symmetry. It is interesting to note that the smallness of $`\mathrm{\Delta }m_{}^2/\mathrm{\Delta }m_A^2`$ is related to the smallness of $`U_{e3}`$. Furthermore this relation, Eq.(20) provides a test of the leptonic horizontal symmetry. In Fig. 1, we show the implications of this equation for the allowed parameter range in the case of the LMA solution to the solar neutrino problem. Inside of the quadrilateral is the allowed region for the parameters for the centarl value of the $`\mathrm{\Delta }m_A^2=2.5\times 10^3`$ eV2. Therefore, unless new solar neutrino data changes the current picture of neutrino mixings, long base line experiments such as the proposed JHF and NUMI Off-axis as well as KAMLAND experiments must yield points inside this allowed region, if this model is to describe nature. As is clear from the Fig. 1, taking the best fit values for the solar mixing angle i.e. $`0.22tan^2\theta _{}0.59`$ and $`2.2\times 10^5eV^2\mathrm{\Delta }m_{}^22\times 10^4eV^2`$ (at 99.7% c.l.), we find that, $`0.25cos2\theta _{}0.63`$, and using the above equation we get,

$`0.4U_{e3}0.083`$ (46)
Thus this model is testable in near future.

## V Comments and other tests of the model

(i) A characteristic test of the inverted hierarchy models is in its prediction for neutrinoless double beta decay. Generically in the exact bimaximal limit, the effective mass measured in neutrinoless double beta decay i.e. $`<m>_{\beta \beta }U_{ei}^2m_i=0`$, since we have $`<m>_{\beta \beta }=m_1U_{e1}^2+m_2U_{e2}^2`$ and $`m_1=m_2`$ and $`U_{e1}=U_{e2}=1/\sqrt{2}`$. The mass matrix in Eq. (8) however differs from this limit; nonetheless, the change in mass differences and the change in the mixing angles compensate each other to give zero. Therefore in the class of models we are discussing, the neutrinoless double beta decay is a probe of the structure of the leptonic mass matrix. In our case we predict $`<m>_{\beta \beta }(cos2\theta _{}\sqrt{\mathrm{\Delta }m_A^2})`$, which at 99.7% confidence level be as large as $`0.03`$ eV.

(ii) The model leads to the standard MSSM below the horizontal symmetry breaking scale.

(iii) In our model we imposed $`\overline{\chi }\overline{\chi }`$ discrete symmetry. This will leave the charge neutral Higgisnos corresponding to $`\chi `$ and $`\overline{\chi }`$ massless. However one may add a bilinear term of the form $`\overline{\chi }\chi `$ to the superpotential thereby breaking the discrete symmetry softly. This will then generate a mass for the corresponding horizontal Higgsino.

## VI Summary and conclusions

In conclusion, we have presented an extension of the minimal supersymmetric standard model where a local $`SU(2)_H`$ symmetry acts on both on the left and right handed charged leptons. Freedom from global anomalies then requires that a doublet of right handed neutrinos be included in the theory. This model provides a very natural way to understand two crucial features of the current neutrino oscillation data i.e. near bimaximal mixing pattern and a small $`\mathrm{\Delta }m_{}^2/\mathrm{\Delta }m_A^2`$. It also gives a relation between the neutrino observables $`U_{e3}`$, $`\mathrm{\Delta }m_{}^2/\mathrm{\Delta }m_A^2`$ and solar mixing angle $`sin^22\theta _{}`$. For the current fits to the latter two parameters, it predicts a lower bound on $`U_{e3}`$ which is quite accessible to long baseline experiments currently planned. We also present the complete range of allowed values for $`U_{e3}`$ and $`\mathrm{\Delta }m_{}^2/\mathrm{\Delta }m_A^2`$ predicted by our model.

The work of R. N. M. is supported by the National Science Foundation Grant No. PHY-0099544. We thank Luis Lavoura for a useful comment and Dragos Constantin for help with the figure.


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# Light Scattering in Transparent Glass Ceramics

## Abstract

Transparent glass ceramic materials, with microstructures comprised of dispersed nanocrystallites in a residual glass matrix, offer the prospect of nonlinear optical properties. However, good transparency requires low optical scattering and low atomic absorption. The attenuation of light due to scattering (turbidity) will depend upon the difference in refractive index of the two phases and the size and distribution of crystals in the glass. Here, we model the glass ceramic as a late-stage phase-separated structure, and compute scattering in this model. We find that the turbidity follows a $`k^8R^7`$ relationship, where $`k`$ is the wavevector of light in the glass ceramic and $`R`$ is the average radius of the crystals in the glass.

Glass ceramics are glasses containing nanometer to micron sized crystals embedded in a glass matrix. Glass ceramics are easier to manufacture into complex shapes than traditional ceramics, utilizing standard techniques developed for the glass industry Beall (1992). In addition, the embedded crystalline phase can enhance existing, or offer entirely new, properties from that of the parent glass. Recently, much attention has been paid to optically transparent glass ceramics Beall and Pinckney (1999); Tick et al. (1995); Tick (1998), which have greater thermal stability than their parent glasses. Transparent oxyflouride glass ceramics, for example, can be doped with optically active rare-earth cations, offering the possibility of numerous applications in nonlinear optics Tick et al. (1995). However, the understanding of the transparency of these nanophase glass ceramics is still relatively poor. Transparency has been found to occur in glasses with large volume fractions of crystals ($``$ 30-35 %) and nanoscale crystal sizes (1-15 nm). Application of the Mie theory of scattering to such a material, leads to an over-estimate of the attenuation due to scattering (turbidity) by many orders of magnitudeBeall and Pinckney (1999).

A more sophisticated approach is to use Rayleigh-Debye theory, which allows for the possibility of coherence and interference between scatterers. To describe the scattering, this theory requires a structure factor which depends on the distribution of scatterers in the medium. For example, Hopper Hopper (1985) has developed an approximate structure factor for glasses which have undergone late-stage microstructural phase separation via spinodal decomposition. Hopper’s structure factor has been used to describe the scattering in transparent glass ceramics Tick et al. (1995); Tick (1998) and gives a turbidity of

$$\tau 6.3\times 10^4(\frac{\mathrm{\Delta }n}{\overline{n}})^2k^4L^3$$
(1)
where $`k`$ is the wavevector of the incident light propagating in a medium with refractive index $`\overline{n}`$, $`\mathrm{\Delta }n`$ is the difference in refractive index between the glass and crystal phases, and $`L`$ is the mean distance between phases. This model improves on Mie theory, predicting turbidities that are somewhat closer to those measured for transparent glass ceramics.

Subsequent to Hopper’s work, there has been a considerable improvement in the understanding of late-stage structure factors in phase-separated media Langer (1992); Furukawa (1985, 1989a, 1989b). In particular, the small wave-number limit of the late-stage structure factor is now well characterized. We will apply this small wave-number structure factor to determine the attenuation due scattering in glass ceramics to improve on equation (1).

We consider the propagation of light in a medium with spatially varying dielectric constant $`ϵ(𝒓)`$. We define $`\eta (𝒓)`$ to be the fractional variation of the dielectric constant:

$$ϵ(𝒓)=\overline{ϵ}\left(1+\eta (𝒓)\right)$$
(2)
where $`\overline{ϵ}=ϵ`$ is the average dielectric constant in the medium and $`\eta =0`$. We also define the two-point correlation function for the fractional variation in dielectric constant as follows:

$$\varphi (𝒓)=\eta (𝒓+𝒓^{})\eta (𝒓^{}).$$
(3)
The structure factor, $`S(𝒌)`$, is just the Fourier transform of $`\varphi (𝒓)`$.

The Rayleigh-Debye approximation is valid in the scattering regime $`kL\mathrm{\Delta }ϵ1`$, where $`\mathrm{\Delta }ϵ`$ is the difference in dielectric constant between scatterer and background media Kerker (1969). For optical wavelengths, with phase sizes of several tens of nanometers and $`\mathrm{\Delta }ϵ0.3`$, this quantity is typically less than 0.1. This approximation also neglects multiple scattering, which may become significant if the depth of the media becomes comparable to the inverse turbidity.

In this approximation, the intensity of scattered light at an angle $`\theta `$ to unpolarized incident light, and the consequent turbidity, are given by:

$`{\displaystyle \frac{I(\theta )}{I_0}}`$ $`=`$ $`{\displaystyle \frac{k^4}{32\pi ^2r^2}}V\left(1+\mathrm{cos}^2\theta \right)S(2k\mathrm{sin}\theta /2),`$ (4)
$`\tau `$ $`=`$ $`{\displaystyle \frac{k^4}{16\pi }}{\displaystyle _0^\pi }𝑑\theta \mathrm{sin}\theta \left(1+\mathrm{cos}^2\theta \right)S(2k\mathrm{sin}\theta /2),`$ (5)
where $`I_0`$ is the intensity of the incident light, $`V`$ is the volume of the scattering media and $`r`$ is the distance from this media.

To develop a structure factor for the variation in dielectric constant in glass ceramics, we will assume that the material is a binary mixture which has undergone late-stage phase separation. Thus, the local composition can be specified by a single parameter $`\mathrm{\Phi }=\phi _A\phi _B`$, where $`\phi _{A(B)}`$ is the molar fraction of phase A (B). We also assume that the dielectric constant of the glass at any point is linearly related to the composition, $`ϵ=ϵ_A\phi _A+ϵ_B\phi _B`$. The fractional deviation $`\eta `$ of the dielectric constant is then given by

$$\eta (𝒓)=\frac{\mathrm{\Delta }ϵ}{2\overline{ϵ}}\left(\mathrm{\Phi }(𝒓)\mathrm{\Phi }\right)$$
(6)
where $`\mathrm{\Phi }`$ is the average value of $`\mathrm{\Phi }`$. Thus, the two-point correlation function (3), and hence the structure factor, is determined by the local composition, and will evolve as the composition evolves.

The dynamics of such a system undergoing phase separation can be described by the Cahn-Hilliard equation Cahn and Hilliard (1959):

$$\frac{\mathrm{\Phi }}{t}=\mathbf{}\left(D\mathbf{}\mu (\mathrm{\Phi })\right),$$
(7)
where $`\mu (\mathrm{\Phi })`$ is a generalized chemical potential for the two-phase system and $`D`$ is a diffusion coefficient. Some glass ceramics do phase separate via a spinodal mechanism (e.g. transparent mullite glass ceramics) while others nucleate homogeneously (e.g. transparent oxyflouride glass ceramics) Beall and Pinckney (1999). While equation (7) cannot immediately be applied to nucleationLanger (1992), at sufficiently late times the structure of the phase separated material will be independent of the initial separation mechanismFurukawa (1989a). Hence, the late-stage structure of systems that have phase separated via nucleation can be approximated by solutions of equation (7).

Figure 1 shows a numerical solution of equation (7) in one spatial dimension for spinodal decomposition. The early-stage spinodal instability produces a separation of phases from an initially homogeneous mixture. Late-stage coarsening leads to an increase in the size of the separated regions, as regions grow, evaporate and coalesce. This late-stage coarsening process, often called Ostwald ripening Ostwald (1900), occurs at late times in systems undergoing phase separation via both spinodal and nucleation mechanisms Voorhees (1992); Alkemper et al. (1999).

The structure factor for a system undergoing late-stage coarsening via equation (7), can be approximated in the small $`kR`$ limit by:

$$S(k)\phi (1\phi )R^d\left(kR\right)^4\left(\frac{\mathrm{\Delta }ϵ}{2\overline{ϵ}}\right)^2$$
(8)
where $`R`$ is the average crystal radius, $`d`$ is the number of spatial dimensions and $`\phi `$ the crystal volume fraction Langer (1992); Furukawa (1985, 1989a, 1989b). This form of the structure factor has been observed in late-stage phase separated systems in computer simulations Furukawa (1989b) and experiment Gaulin et al. (1987). Indeed, figure 2 shows the late-stage structure factor for a 1D numerical simulation, where the $`(kR)^4`$ dependence is evident for $`kR<1`$.

Assuming that (8) holds, we can now give the scattered intensity and turbidity for a glass ceramic, with mean crystalline volume fraction $`\phi `$, that has undergone late-stage coarsening:

$`{\displaystyle \frac{I(\theta )}{I_0}}`$ $``$ $`{\displaystyle \frac{Vk^8R^7}{2\pi ^2r^2}}\phi (1\phi )\left(1+\mathrm{cos}^2\theta \right)\mathrm{sin}^4\theta /2\left({\displaystyle \frac{\mathrm{\Delta }n}{\overline{n}}}\right)^2`$ (9)
$`\tau `$ $``$ $`{\displaystyle \frac{14}{15\pi }}\phi (1\phi )k^8R^7\left({\displaystyle \frac{\mathrm{\Delta }n}{\overline{n}}}\right)^2`$ (10)
where we have assumed $`\mathrm{\Delta }ϵ\overline{ϵ}`$. In figure 3, contours of turbidity for (10) are shown as a function of crystal volume fraction and radius. In addition, figure 4 compares the turbidity predicted by Mie theory, equation (1) and equation (10), for a fixed volume fraction ($`\phi =0.3`$). The strong $`R^7`$ dependence means that transparency is rapidly lost as R approaches $`2030`$ nm. The $`L^3`$ dependence of Hopper’s equation for turbidity (1) does not predict such a rapid transition.

Mie theory is expected to be valid only if there are no spatial correlations in composition on a length-scale comparable to the wavelength of the incident light i.e. for early stage growth in the dilute limit ($`LR`$). Equation (10) does not reduce to Mie theory in the dilute limit, as (10) assumes the presence of late-stage spatial correlations in composition. However, a theory of scattering that treats late-stage and early-stage structures via (7) will be sought in future work.

Finally, we make comparison with turbidity data given by Tick, Borrelli, Cornelius and Newhouse Tick et al. (1995). They report on transparent oxyflouride glass ceramics with crystal radii $`R15`$ nm, crystal volume fractions $`\varphi =0.3`$ and turbidities due to scattering of $`2\times 10^2`$ m-1 for a wavelength of $`\lambda _0=647`$ nm (in vacuum). Assuming a mean refractive index $`\overline{n}=1.7`$ and a refractive index difference $`\mathrm{\Delta }n=0.1`$, Mie theory predicts a turbidity of $`200`$ m-1, equation (1) predicts a turbidity of $`7`$ m-1 (using $`L2.6R`$), whereas equation (10) predicts a turbidity of $`0.2`$ m-1. Thus equation (10) represents a substantial improvement over (1) and Mie theory when applied to transparent glass ceramics.


text:
# Aging dynamics of ±𝐽 Edwards-Anderson spin glasses

## I INTRODUCTION

After more than twenty years of extensive research, the physics of spin glasses is still far from being completely understood. The inherent complexity of the physical scenario together with unsurmountable mathematical difficulties undermine even the simplest theoretical approaches that attempt to include basic realistic ingredients. Notwithstanding that a large amount of information could be extracted from the analysis of the mean field model (i.e. the Sherrington-Kirkpatrick modelmpv ; mprrz ), the extension of those results to finite dimensional spin glasses remains a matter of hard controversy in the statistical physics community droplet ; ns . In this context large scale numerical simulations emerged as a valuable aid in gaining physical insight into more realistic modelsrieger1 ; mpr ; however, they pose such a serious demand over existent computational capabilities that the study of the low temperature phases of these systems may be considered in many respects to be still in an exploratory state.

Regarding the out of equilibrium behavior of finite dimensional spin glasses, much attention has been devoted to models with continuous couplings distributions mpr ; bb . One important feature of these systems is that the ground state is unique. For Gaussian couplings, the aging behavior of models in $`3d`$ and $`4d`$ reported in the literature seems to be compatible with the simple aging or weak interrupted aging scenarios (to be defined below). These particular scenarios suggest a rather simple phase space structure with a unique relevant time scale, namely the age of the system. This apparently simple behavior could be a consequence of the existence of strongly separated temporal scales. Because of this during the time span of a simulation or experiment at very low temperatures the system could not be able to cross over between different time regimes and only one relevant time scale is probed.

One may wonder whether the relatively simple dynamical behavior observed in spin glasses with continuous distributions at very low temperatures can also be expected in systems with discrete couplings, which present a strong degeneracy of their ground states as well as a noticeable discretization of their low-energy spectrum. That might lead to very low temperature effects that could not be observable in continuous spin glasses.

It is known that at temperatures relatively close to $`T_c`$ there is no qualitative difference in the phenomenological characterization of aging rieger2  between the continuous and discrete couplings systems. However, at lower temperatures, effects deriving from the discrete nature of the energy spectrum as well as from the high degeneracy of the ground states may become apparent in discrete models.

Scaling properties contribute to a quantitative description of complex phenomena, even in cases where a general theory is lacking droplet ; bckm ; yohuta02 . In this respect, different dynamical universality classes may emerge for which similar scaling functions describe the dynamics of different systems. The knowledge of these scaling rules gives considerable insight into the nature of the underlying dynamical processes.

In this paper we present the results of an extensive numerical study of the aging dynamics and scaling properties of the two-time autocorrelation functions for the $`\pm J`$ Edwards-Anderson spin glasses in dimensions $`d=4`$ and $`d=6`$ at temperatures which cover the whole low temperature phases of the models.

Our results show important differences between the aging dynamics of the $`\pm J`$ models compared with the corresponding Gaussian models. At the very low temperatures $`T=0.07T_c`$ and $`T=0.15T_c`$ we find interrupted aging scenarios both in $`4d`$ and $`6d`$. In particular, for the lowest temperature we find a very small exponent indicative of a rapid relaxation to a stationary dynamics. At first sight this seems hard to reconcile with the expected very slow relaxation which takes place at these extremely low temperatures. Nevertheless this can be seen as a consequence of the discrete nature of energy levels which can produce some non trivial time dependent phenomena at very low temperatures at time scales roughly independent of the waiting time $`t_w`$. The systems simply do not have enough time to relax over barriers dependent on $`t_w`$. So this dynamics is completely different from the usual long time non-equilibrium relaxation but is not trivial due to the discreteness of the low lying energy levels. At $`T=0.5T_c`$ we observe some differences in the behavior in $`4d`$ and in $`6d`$. In $`4d`$ logarithmic scalings, which are compatible with dynamic ultrametricity, work very well even at this relatively high temperature. In $`6d`$ the scenario is less clear since we observe that although logarithmic scalings are very good it is also possible to scale the data with a super-aging scaling form. As $`d=6`$ is the upper critical dimension the relaxation dynamics should present some features of the infinite range model. We find insted that the behavior is more similar to that at lower dimensions than to the mean field model.

The paper is organized as follows: in section II we define the model studied and the observables measured; in section III and IV we analyze the results of the 4d and 6d models respectively. Finally the conclusions and a discussion are presented in section V.

## II MODEL AND METHOD

The system consists of a d-dimensional hypercubic lattice of Ising spins which interact according to the following Hamiltonian:

$$=\underset{i,j}{}J_{ij}S_iS_j,$$
(1)
where the symbol $`i,j`$ indicates that only first neighbor pairs $`i,j`$ are taken into account. The coupling constants $`J_{ij}`$ are binary random variables chosen from the following probability distribution:

$$\rho (J_{ij})=\frac{1}{2}\left(\delta (J_{ij}1)+\delta (J_{ij}+1)\right).$$
(2)
The time evolution of the model is governed by a standard heat-bath Monte Carlo process with sequential random update. The imposed boundary conditions were periodic in 4d and helical in 6d mc . In the practical implementation of the numerical algorithm a significant increase in speed was accomplished by using multi-spin coding mc  so each spin and coupling constant demand just one bit of information each for storage. In this way we can run many replicas at the same time at the cost of a single realization. In all cases the dynamics is initiated from a random configuration, simulating a sudden quench from infinite temperature into the spin glass phase.

One straightforward way to characterize the out of equilibrium dynamics of complex magnetic systems is through the analysis of the two-time autocorrelation function $`C(t,t^{})`$, which can exhibit history dependent features usually referred to as aging. A system that has attained thermodynamic equilibrium will show a stationary dynamics for which only time differences make physical sense, and therefore $`C(t,t^{})C(tt^{})`$. However, complex magnetic systems such as spin glasses show a much more complex behavior due to the presence of an extremely slow relaxational dynamics. These materials may be out of equilibrium for spans of time longer than any available time scale in the laboratory. In this circumstances insight into the ongoing processes can be obtained by studying the scaling properties of dynamical quantities like $`C(t_w+t,t_w)`$, where the waiting time, $`t_w`$, stands for the age of the system measured after a quench into the spin glass phase, and $`t`$ stands for the time measured since the age $`t_w`$.

In the numerical experiments we compute the quantity

$$C(t_w+t,t_w)=\left[\frac{1}{N}\underset{i=1}{\overset{N}{}}S_i(t_w+t)S_i(t_w)\right]_{av},$$
(3)
where we have denoted by $`[\mathrm{}]_{av}`$ an average taken over several realizations of the random couplings and thermal histories. An additive form for the autocorrelations was assumed:

$$C(t_w+t,t_w)=C_{st}(t)+C_{ag}\left(\frac{h(t_w+t)}{h(t_w)}\right).$$
(4)
The stationary part $`C_{st}(t)`$ is well described by an algebraic decay of the form $`C_{st}(t)=At^{x(T)}+q`$. There is no theoretical basis for determining the scaling function $`h(z)`$ appearing in the aging part of the autocorrelations. There have been proposed a couple of simple forms which work reasonably well for relaxations in the vicinity of simple aging, in the sense that the correct scaling variable is of the form $`t/t_w^\mu `$ with $`\mu 1`$ bb . In our case it was not possible to find a unique realization of the function $`h(z)`$ for the whole range of temperatures studied. In the scaling analysis we restricted ourselves to find the relevant scaling variables for the aging part of the autocorrelations.

## III d=4

The simulations of the four dimensional Edwards-Anderson model were done for systems of linear size $`L=12`$ $`(T=0.07T_c)`$ and $`L=10`$ imposing periodic boundary conditions. We recall that the critical temperature for this model has been estimated to be $`T_c2`$hu99 ; mazu99 .

### III.1 Very low temperatures: probing the discreteness of the lowest energy levels

In Figure 1 we show the behavior of the two-time autocorrelation function $`C(t_w+t,t_w)`$ at the temperature $`T=0.07T_c`$. The waiting times are $`t_w=2^k,k=14\mathrm{}19`$, and the simulation was run up to $`t=10^7`$ MCS. There is a weak dependence on the wainting time and the system relaxes to a stationary regime presenting a strong sub-aging behavior.

In Figure 2 we show the best scaling obtained for the long time behavior of the autocorelation function after subtraction of the stationary part:

$$C_{st}(T)=At^{x(T)}+q.$$
(5)
In this particular case, the best fit was obtained for $`x(T)=0.57`$ (a rather high value) and $`q0.93`$. In the (weakly) $`t_w`$ dependent region it is possible to distinguish two regimes: a first one when the system falls out of the quasi-equilibrium and a second regime at long times. Both are very well described by different interrupted or sub-aging scalings of the form:

$$C_{ag}(t_w+t,t_w)=𝒞\left(\frac{t}{t_w^\mu }\right).$$
(6)
For very long times, the best fit yields an exponent $`\mu 0.1`$ which characterizes a very strong sub-aging regime. It is also possible to collapse the data in the time window corresponding to the first out of equilibrium regime ($`tt_w`$) with the form given by Eq.(6) with an exponent $`\mu 0.27`$ as can be seen in figure 3. Note that the first sub-aging regime disappears gradually as $`t_w`$ grows and effectively, after the longest waiting time studied $`t_w510^5`$, these slow modes have practically equilibrated. After these very long waiting times the system evolves quickly to a stationary situation with a very short characteristic aging time $`t_w^{0.1}`$. The observation of these sub-aging regimes at this very low temperature is consequence of the discrete nature of the low lying energy levels. In fact the smallest time scale for activation in this energy landscape is of the order of $`\mathrm{exp}(2/T)1,610^6`$ which is approximately the time where the correlation leaves the quasi-equilibrium regime (see Figure 1). Up to this time scale the system relaxes effectively in the flat energy landscape defined by the sites with zero local field which are free to flip (besides a smaller group which can still contribute to lowering the energy). Note that the value of the correlation in the plateau $`C=q`$ in this regime does not correspond to the equilibrim order parameter $`q_{EA}`$ but instead to one minus the fraction of sites with zero field 111This was pointed to us by Federico Ricci-Tersenghi (private communication).. After a time of the order of $`\mathrm{exp}(1/0.07)`$ thermal activation begins to take place through the lowest lying barriers and the correlations decay to zero as the system expands its available phase space. As a further test for this interpretation we have performed a set of simulations in a microcanonical ensemble which are shown in the inset of Figure 1: for the three longest waiting times we have allowed the system to relax up to $`t_w`$ and from then on only flips of spins with zero local fields were allowed. In these conditions the correlations decayed only to the plateau suggesting that the long time decay in the canonical dynamics was produced by activation over low energy barriers. The scenario for this behavior is quite clear: after a long waiting time, the system diffuses further in a flat energy landscape surrounded by barriers of minimum height $`\mathrm{\Delta }E=2`$. At time scales of the order of $`\mathrm{exp}(2/T)`$ it can further relax by thermal activation over these low barriers. The next level is at $`\tau \mathrm{exp}(4/T)2,5610^{12}`$ and it is clearly unreachable. The simplicity of the landscape seen by the system at this temperature explains the presence of the rapidly interrupted aging which is observed.

In figure 4 we present the results of a simulation performed at a higher temperature (though still very low) $`T=0.15T_c`$. At this temperature in the time range of the simulation the system is able to probe activation over barriers of height $`\mathrm{\Delta }E=2`$ and $`\mathrm{\Delta }E=4`$. The waiting times are $`t_w=5000`$, $`10000`$, $`50000`$ and $`200000`$. The three curves for the shortest waiting times can still be well collapsed for large values of $`t`$ by the interrupted aging form (6), with an exponent $`\mu 0.3`$. However, the last curve ($`t_w=200000`$) clearly departs from this scaling, signaling a crossover to another regime. It is still possible to see an intermediate regime for the shortest $`t_w`$’s.

### III.2 Full aging dynamics

As the thermal energy is raised above the lowest lying levels the full ruggedness of the landscape should emerge and true aging dynamics should be restored. What happens when the thermal energy is enough to turn discrete energy levels undetectable? In figure 5 we see the autocorrelations for a temperature $`T=0.5T_c`$ for three waiting times $`t_w=10000,50000,100000`$. A fit to the quasi-equilibrium region gives $`x(T)=0.1`$ and $`q=0.62`$, indicating a very slow relaxation. This is due to the increasing complexity of the phase space visited at this temperature. The best scaling form obtained for the aging regime is presented in figure 6 and corresponds to the following logarithmic form:

$$C_{ag}(t_w+t,t_w)=𝒞\left(\frac{\mathrm{ln}t}{\mathrm{ln}t_w}\right).$$
(7)
Note that there is still an intermediate regime which is not well described by this logarithmic scaling but the corresponding time window is too small to try a reasonable collapse there. On the other side, in the long time regime the logarithmic scaling (7) works remarkably well. It is worth noting that this form of the scaling function is compatible with dynamical ultrametricity (see bertin ). This form is slightly different from that expected by a droplet like scenario, which takes the form $`\mathrm{ln}(t+t_w)/\mathrm{ln}(t_w)`$ and does not obey ultrametricity. This new evidence for a (weak) ultrametricity obtained directly from aging measurements is in agreement with recent results for the same model obtained from a quite different approach st01 . We have also done simulations at temperature $`T=0.75T_c`$ (not shown) and the results are compatible with the logarithmic scaling (7) although due to the strong noise at this rather high temperature the data is not so clean as at lower temperatures and the scaling of the curves is not so good. At high temperatures several time scales are mixed or superposed because of thermal noise and consequently it is difficult to obtain reliable scalings.

### III.3 d=6

We have done a similar analysis of data obtained for the $`d=6`$ Edwards-Anderson model. As this model is at the upper critical dimension we expected to see a behavior similar to the mean field or Sherrington-Kirkpatrick (SK) model cuku94 ; maparo98 ; motastca00 . The off equilibrium dynamics of the SK model is only poorly understood due to the complexity which emerges from the full replica symmerty breaking which is the central characteristic of that model. As a consequence of the complex ultrametric organization of time scales no simple scaling form can be found for the aging dynamics which might be described by a superposition of scaling regimes of the form cuku94 :

$$C_{ag}(t_w+t,t_w)=\underset{i}{}𝒞_i\left(\frac{h_i(t_w+t)}{h_i(t_w)}\right).$$
(8)
Nevertheless we have found a much simpler scenario which is in fact very similar to what is observed in $`d=3`$ and $`d=4`$. The transition to an SK like aging scenario seems to be very slow as the connectivity of the system grows.

All these simulations were carried out for systems with linear size $`L=5`$. It is worth noting that the computational time required for simulating these systems increases as $`L^6`$, making it much more difficult to use larger values of $`L`$. The critical temperature of this model was estimated in wayo93 ; be96  to be $`T_c3`$. Here again we start by considering the very low temperature case $`T=0.07T_c`$.

The overall behavior of the two-time autocorrelation function is similar to that described for dimension $`d=4`$. It is possible to identify two different sub-aging regimes within the time window of our simulation, which covers up to $`t=10^7`$. Both in the intermediate and in the asymptotic regimes the functions $`C(t_w+t,t_w)`$ can be very well collapsed by an interrupted aging scenario of the form (6). In Figure 7 we show the best scaling obtained for the long time behavior of the autocorrelation after subtraction of the stationary part. The plots correspond to the three longest waiting times: $`t_w=2^{15}`$, $`2^{17}`$ and $`2^{19}`$. The fitting in the quasi-equilibrium regime yielded $`x(T)=0.55`$ and $`q0.96`$, similar to those found for $`d=4`$ at the same temperature. The two regimes described above can be clearly identified in this graph. For the last regime, the best data collapse yields an exponent $`\mu 0.25`$ and in the intermediate regime $`\mu 0.9`$ (this figure is not shown).

In figure 8 we present the results of a similar simulation performed at $`T=0.15T_c`$. Here we note that the long times regime which had a smaller exponent (faster relaxation) has now disappeared. Actually the three curves can be very well collapsed by a unique interrupted scaling form with $`\mu =0.93`$. The main difference between this simulation and that performed for $`d=4`$ (see figure 4) is the fact that now it is not seen the crossover described in $`d=4`$ for the longest waiting time.

Note also that as $`T`$ increases the scaling form approaches the simple aging scaling law $`\mu 1`$.

At $`T=0.5T_c`$ the scenario is not so clear as in $`d=4`$. In figures 9 and 10 we present two different scalings. In 9 we use the expression (7) and in 10 the same scaling form used in the interrupted scenario. Nevertheless, it is important to stress that in this last case the exponent that produces the best collapse is $`\mu 1.2`$, indicating the possible existence of a super-aging regime. However, as can be concluded from these figures, it is difficult to decide which is the true scaling law. In summary, as mentioned at the beginning of this section the $`d=6`$ model presents an aging dynamics very similar to the $`d=4`$ case at corresponding temperatures and it seems to be still far from the limit of the mean field system studied in maparo98 ; motastca00 .

## IV DISCUSSION AND CONCLUSION

In this paper we have presented an extensive numerical study of the out of equilibrium dynamics of spin glasses with discrete couplings defined on hypercubic lattices in $`4`$ and $`6`$ dimensions, for very low temperatures $`T=0.07T_c`$, $`T=0.15T_c`$ and $`T=0.5T_c`$.

The relaxation behavior of the model with $`\pm J`$ couplings is different from that with continuous gaussian couplings. While the observed aging dynamics of the gaussian model is described in a wide range of temperatures and time scales by simple aging or weak interrupted aging scalings, the observed behavior of the $`\pm J`$ model seems to depart from that. At the lowest temperatures studied , that is for $`T=0.07T_c`$ and $`T=0.15T_c`$, the thermal energy is still not enough to permit activation over several scales and only the lowest lying energy levels are probed. As a consequence the system diffuses on a flat energy landscape surrounded by low barriers of height 2 or at most 4. It relaxes in this simple landscape presenting a kind of interrupted aging with a rapid relaxation to stationarity. In this sense these relaxations are practically independent of $`t_w`$ and true aging is restored only at higher temperatures. In order to see true aging at these very low temperatures we would have to wait for extremely long times. At $`T=0.5T_c`$ both in $`d=4`$ and $`d=6`$ the full aging is restored, no more signs of interrupted scalings are seen but a slower logarithmic scaling is observed. At this intermediate temperature range thermal energy is large compared with the low lying energy states which were important at the lower temperatures. Consequently the aging dynamics proceeds slowly but with the tendency of restoring ergodicity and equilibrium as $`t_w`$ grows. It is important to stress that for no one of the temperatures studied $`T=0.07T_c`$, $`T=0.15T_c`$, $`T=0.5T_c`$, and $`T=0.75T_c`$ simple aging scenarios were found, in contrast to what seems to be the rule for the gaussian spin glass model. Insted the logarithmic aging observed at $`T=0.5T_c`$ (and also at $`T=0.75T_c`$) points to a simple hierarchy of time scales with dynamical ultrametricity as observed in st01 . On the other hand, even for the model in $`d=6`$, which is at the upper critical dimension, the qualitative form of the aging curves and the scaling functions are very different from those found in the SK modelmaparo98  and in the Hopfield model motastca00  which are known to present full replica symmetry breaking and a consequently full hierarchical or ultrametric organization of time scalescuku94 . In this respect it is worth citing recent work by Yoshino, Hukushima and Takayama yohuta02  where they presented an extended version of the dynamical droplet theory. Two interesting new predicitions are the presence of a new dynamical order parameter $`q_D<q_{EA}`$ which should be observed in a particular lenght/time scaling regime and the distinction between the times at which time translation invariance and the Fluctuation-Dissipation Theorem are violated. The authors presented numerical results on the $`d=4`$ $`\pm J`$ spin glass to support their findings but clearly more precise measurements are needed in order to test the theoretical predictions. In particular, scaling functions depend on the growth law of the coherence lenght $`L(t)`$ which permits to see the crossover between critical to activated dynamics. Unfortunately this information is still not available for the temperatures and time scales reached in our simulations which we think are necessary in order to clearly see the separation of time regimes during aging dynamics. We expect new interesting results to come from these kind of analysis in the near future.

###### Acknowledgements.

We thank F. Ricci-Tersenghi for interesting comments on an earlier version of the manuscript. The work of D.A.S. was supported in part by Conselho Nacional de Desenvolvimento Cient fico e Tecnol gico (CNPq) and Fundaç o de Amparo Pesquisa do Estado do Rio Grande do Sul (FAPERGS), Brazil. M.A.M. acknowledges finacial support from the Secretary of Science and Technology (SeCYT) of the National University of C rdoba, Argentina.


text:
# 𝜇SR and SQUID Investigation of Superconductivity in (NH3)0.75NaK2C60

## I Introduction

In fullerene based superconductors ammonia intercalates as a neutral molecule, without interacting with the host electronic system and preserving the superconducting properties of the material. Since it acts simply as a molecular spacer, a change in lattice parameters and an increase of unit cell volume are often observedZhou et al. (1993). As a consequence, the $`t_{1u}`$ conduction band of the fullerene compound narrows and its density of states at the Fermi level increases, thus determining an increment in the superconducting transition temperature. An example of this mechanism has been reported for Na2CsC60Zhou et al. (1993) which gives (NH3)4Na2CsC60 after ammoniation, with a conspicuous increase in transition temperature from 10.5 to 29.6 K.

The intercalation of ammonia can also induce a metal-to-insulator transition as e.g. in NH3K3C60,Iwasa et al. (1996); Kitano et al. (2002) where the superconductivity of the ammoniated compound can be restored only after the application of external pressure.Zhou et al. (1995)

We will deal here with a family of fullerides such as (NH3)xNaK2C60 and (NH3)xNaRb2C60, whose precursors NaK2C60 and NaRb2C60 cannot exist as a single phase in normal conditions, but become stable only as ammoniated compounds.Shimoda et al. (1996) X-ray diffraction in these systems shows that the NH3-Na groups occupy the large octahedral sitesShimoda et al. (1996) with a consequent off-centering of the Na+ ions. Since their discovery, these compounds have revealed puzzling features concerning the relation between the superconducting transition temperature both with the lattice parameter as well as with the density of states at the Fermi level. Indeed, the progressive removal of NH3, accomplished by pumping on the sample above room temperature, results in a decrease of the lattice parameters accompanied by an increase of the superconducting transition temperature, a trend opposite to that observed in (NH3)4Na2CsC60. In addition, we have recently shownRiccò et al. (2001) that in a series of (NH3)xNaK2C60 compounds (with $`0.5<x<0.8`$) the Pauli-Landau spin susceptibility yields a lower density of states at the Fermi level in compounds having a higher $`T_c`$, in contrast with BCS or Migdal-Eliashberg predictions.

It is therefore interesting to ask whether these anomalies are related to essential differences in the nature of superconductivity in (NH3)0.75NaK2C60 with respect to most common superconducting fullerides. A possible non-conventional nature of the superconductivity in this system would manifest itself in the values of the critical parameters of its superconducting phase: the London penetration depth $`\lambda `$ and the lower and upper critical fields, $`H_{c1}`$ and $`H_{c2}`$ respectively. Such fundamental parameters have never so far been measured and we will tackle the problem by providing their values and discussing the implications.

From the available data in the literature, the other so-called “normal” fullerene based superconductors appear to be extreme type-II superconductorsHolczer et al. (1991); Sparn et al. (1992) characterized by $`\kappa =\lambda /\xi 1`$, where $`\kappa `$ is the Ginzburg-Landau parameter. Our results will be first analyzed in this framework and, in case of discrepancies, alternative suggestions will be offered.

When $`\lambda \xi `$, both of these fundamental lengths can be easily extracted from measurements of the lower ($`H_{c1}`$) and the upper ($`H_{c2}`$) critical magnetic fields or, more precisely, from their extrapolated values at zero temperature. Roughly speaking, $`H_{c2}`$, the field at which the transition from the superconducting to the normal state occurs, corresponds to the field at which one quantum of magnetic flux $`\mathrm{\Phi }_0=hc/2e2\times 10^7`$ G cm2 extends over the coherence area of an electron pair, so that:

$$H_{c2}(0)=\frac{\mathrm{\Phi }_0}{2\pi \xi ^2},$$
(1)
from which the Ginzburg-Landau coherence length $`\xi `$ can be determined. On the other hand, the knowledge of $`H_{c1}`$, the field at which the magnetic flux starts to penetrate the sample, allows the computation of the penetration depth $`\lambda `$ by using the well known equation (valid for $`\kappa 1`$):

$$H_{c1}(0)=\frac{\mathrm{\Phi }_0}{4\pi \lambda ^2}\mathrm{ln}\kappa .$$
(2)
In addition to independent measurements of $`H_{c1}`$ and $`H_{c2}`$, as obtained by standard SQUID magnetometry, we will provide also the value for $`\lambda `$, which yields a stringent check of the validity of eq. (1) and (2). Since $`\lambda `$ represents the transverse extension of the vortices in the Abrikosov intermediate phase, its value can be also determined from the local magnetic field distribution. It is well known that Muon Spin Rotation ($`\mu `$SR) gives reasonable estimates of $`\lambda `$, even for irregular flux line lattices. Details on SQUID and $`\mu `$SR measurements are given in the next experimental section.

## II Experimental

The samples were prepared following the procedures outlined in Ref. Shimoda et al., 1996. Stoichiometric amounts of alkali metals (Aldrich, 99.95%) and C60 (Southern Chem. 99.5%) were dissolved in anhydrous ammonia (Aldrich, 99.99+%) at 230 K. After the reaction had taken place, the temperature was slowly increased until the ammonia was completely evaporated. The successive pumping at 120C for 30 minutes yielded the compound (NH3)0.75NaK2C60; the sample was then annealed at 100C for 10 days. Its transition temperature was $`T_c=12`$ K and it showed a 20% superconducting fraction, indicative of bulk superconductivity. The ammonia concentration $`x=0.75`$ was determined from the superconducting transition temperature by interpolating the $`T_cx`$ data reported in Ref. Shimoda et al., 1996.

Evaluation of the granulometry of the samples was performed using a scanning electron microscope (SEM), whose micrographs indicate an average size of the particles $`d2`$ $`\mu `$m.

DC magnetometry measurements were performed with a Quantum Design SQUID magnetometer equipped with a home built Helmholtz cube which surrounded the whole instrument body, thus allowing a reduction of the residual field on the sample to less than 2 mG. The SQUID superconducting magnet was cooled from RT to liquid He temperature in zero external field. For a good thermal contact even at low temperatures the sample was sealed in a long quartz tube under 1 mbar of He atmosphere. The sample was suspended in the middle of the tube, whose length was so chosen as to have always a tube portion face the SQUID coils, even when the sample had to move in and out of them during the magnetic moment measurement. This expedient allowed an accurate subtraction of the quartz diamagnetic contribution.

$`\mu `$SR, which measures the spin precession of implanted muons, is very sensitive to local magnetic fields and therefore it constitutes a valuable technique for our purposes. Indeed, when the applied transverse field exceeds $`H_{c1}`$, the field distribution of the flux line lattice will damp the muon spin precession signal, hence the penetration depth can be readily extractedMacFarlane et al. (1998) from the damping rate.

In common metals and superconductors all the implanted muons usually sit interstitially and, being screened by conduction electrons, they will not form any paramagnetic bound state (muonium). Hence, their precession frequency in an external magnetic field remains that of a free particle (diamagnetic muon). In C60 based superconductors, besides this major component there is an additional part of implanted muons (typically 10–20%) which will form endohedral muonium (located inside a C60 molecule), whose precession frequency is much higher than that of diamagnetic muon. Here we are interested only in the majority of muons that come at rest in the fcc lattice interstices (the precise location is not well known) and precess as diamagnetic muons, i.e. with a gyromagnetic ratio $`\gamma _\mu =13.55`$ kHz/G.

When a superconductor is in the intermediate state, i.e. $`\mu _0H_{c1}<B<\mu _0H_{c2}`$, the muon precession signal will be damped by the inhomogeneous magnetic field distribution of the vortices. The expected damping profile (or the corresponding lineshape in Fourier space) in the case of a triangular flux-line lattice has been computedBrandt (1988) and, for single crystals, also successfully measured. Unlike single crystals, polycrystalline or powder materials exhibit a smeared out magnetic field distribution, with the consequence that the $`\mu `$SR line will assume a Gaussian shape ($`\sigma _{\text{sc}}0.1`$–0.6 $`\mu `$s-1 for fullerides) below $`T_c`$.MacFarlane et al. (1998) The established relation between the $`\mu `$SR damping rate $`\sigma _{\text{sc}(0)}`$ and the internal field rms deviation $`\mathrm{\Delta }B`$ is given by $`\mathrm{\Delta }B=\sigma _{\text{sc}}(0)/2\pi \gamma _\mu `$. Once $`\mathrm{\Delta }B`$ is known from an experiment that measures $`\sigma _{\text{sc}}(0)`$ in the appropriate intermediate field range $`\mu _0H_{c1}<B<\mu _0H_{c2}`$, the penetration depth $`\lambda `$ is given by:Brandt (1988)

$$\lambda 3.71\times 10^3\left[\frac{\mathrm{\Phi }_0^2}{(\mathrm{\Delta }B)^2}\right]^{1/4}.$$
(3)
$`\mu `$SR experiments were performed on the EMU spectrometer of the ISIS Facility (Rutherford Laboratory, UK). The pulsed nature of the muon beam sets an upper frequency cut-off that prevents the direct observation of high muonium frequencies. Nevertheless, the interesting fraction of diamagnetic muons will precess well within the pass-band of the spectrometer and therefore could be readily measured. In our case, the sample ($`500`$ mg) was pressed inside an air tight aluminum cell equipped with a thin (75 $`\mu `$m) Kapton window. A pure silver foil was put both directly behind the sample and around the cell window to make it easy to subtract the signal coming from the sample holder.

## III SQUID Measurements

### III.1 Lower critical field

In spite of many previous measurements of the lower critical field by SQUID magnetometry in fullerides,Sparn et al. (1992); Politis et al. (1992a, b); Holczer et al. (1991); Buntar et al. (1992, 1995); Buntar (1995); Buntar et al. (1996, 1997, 1998) its precise determination is still controversial due to considerable experimental difficulties. The simplest way to measure $`H_{c1}`$ consists in observing the field at which the $`M=M(H)`$ curve starts to deviate from linearity. Unfortunately data on fullerides never show a good linearity and this brings to an overestimate of the $`H_{c1}`$ value. Alternative methods based on Bean’s critical state modelBean (1962) give quite different values.Buntar et al. (1995) Recently it was shownBuntar et al. (1996) that the measurement of the trapped magnetization in the intermediate phase yields a more reliable determination of $`H_{c1}`$. The procedure is as follows: first the sample is cooled in zero field from above $`T_c`$ and its initial magnetic moment ($`M_1`$) is measured (ideally it should be zero, but a residue always exists). Then a magnetic field $`H`$ is applied for at least 30 s and, after switching it off, the final moment ($`M_2`$) is measured. When the applied field exceeds a threshold value $`H_{\text{thr}}`$ the magnetic flux is trapped inside the sample. This trapped magnetization, given by the difference $`M_2M_1`$, is then plotted against the applied field $`H`$, as shown in Figure 1 for measurements on (NH3)0.75NaK2C60 performed at 7 K. The increase of the trapped magnetization above $`H_{\text{thr}}`$, which follows a linear behavior at all the investigated temperatures, allows a much more precise determination of $`H_{c1}`$ than alternative procedures. The fitted value for trapping onset (0.51 G for the linear fit shown in Figure 1) is related to the lower critical field value by $`H_{c1}=H_{\text{thr}}/(1n)`$, where $`n`$ is the demagnetization factor. Preliminary measurements on powdered samples gave essentially the same results, although the trapped magnetization values were rather scattered around the (same) fit line (see Figure 1). The use of (weakly compressed) pellets remarkably reduced the spread without an appreciable change in $`H_{\text{thr}}`$, confirming that the demagnetization factor of a set of independent spheres ($`n=1/3`$), correctly adopted for powders,Buntar et al. (1996) is appropriate also for pellets.

The results of several $`H_{c1}`$ measurements at different temperatures are illustrated in Figure 2. The zero temperature value $`H_{c1}(0)=0.87`$ G was then extrapolated from a parabolic fit (BCS weak coupling gave a similar result and experimental errors do not allow to distinguish between the different behaviors).

The striking feature about the $`H_{c1}(0)`$ is its low value with respect to that of other fullerides, shown in Table 1 for a comparison. Even an unphysical linear fit of the data would at most yield an extrapolated value $`H_{c1}(0)1.2`$ which still is one order of magnitude smaller than $`H_{c1}(0)`$ for the quoted fullerides. The obvious suspicion that the powdered nature of the sample affects the measured values was addressed in a previous experiment, reported in Ref. Buntar et al., 1996, where a powdered RbCs2C60 sample and a single crystal were compared and found to have the same lower critical field value. Hence, the measured low $`H_{c1}`$ value given here will be considered an intrinsic feature of the compound.

### III.2 Upper critical field

The upper critical field $`H_{c2}`$ can be determined from the temperature dependence of the field cooled magnetization.Buntar et al. (1995) In this case the sample is cooled in an externally applied field $`H`$ (0.5 T $`<H<`$ 5.5 T) starting from $`T>T_c`$ and its magnetic moment is measured. The value of the external field corresponds to $`H_{c2}`$ when the temperature equals the relative $`T_c`$. Figure 3 shows an example of such a measurement in a 3 T magnetic field.

The data above $`T_c`$ were fitted to a Curie behavior coming from paramagnetic impurities, to which one must add a temperature independent component resulting from Pauli, Landau and core contributions to susceptibility (upper part of the figure).Riccò et al. (2001) After subtraction of all these contributions the curve shown in the lower part of Figure 3 is obtained. $`T_c`$ was estimated as the temperature at which the linear interpolation of the data in the superconducting state intersects the normal state baseline. The observed superconducting transition temperature $`T_c(H)`$ decreases on increasing $`H_{\text{appl}}`$. In Figure 4 we report the dependence of the critical temperature on $`H_{\text{appl}}`$.

Unfortunately, the maximum field available in our conventional SQUID magnetometer ($`H_{\text{max}}=5.5`$ T) does not allow us to investigate the full range of $`T_c=T_c(H_{\text{appl}})`$ dependence so that we have to resort to extrapolation. The extrapolated field value at zero temperature (relevant for $`\xi `$ calculation) is usually extracted from the slope of the observed linear behavior using the Werthamer-Helfand-Hohenberg (WHH) formula:Werthamer et al. (1966)

$$H_{c2}(0)=0.69T_c\frac{H_{c2}}{T}|_{T=T_c}.$$
(4)
The value for the derivative is $`5.0\pm 0.3`$ T/K and from eq. (4) we find $`H_{c2}(0)=40\pm 2`$ T. If we use eq. 1, we can extract a coherence length $`\xi =2.86(8)`$ nm. Both of these values, although different, do not appear to be inconsistent with those of other C60 based superconductors.Baenitz et al. (1995)

Similarly to the measurement of $`H_{c1}`$ it is important to examine possible factors that could affect the estimated value for $`H_{c2}`$:
a) According to analogous measurements on K3C60Boebinger et al. (1988) the parabolic $`H_{c2}(T)`$ dependence predicted by the WHH theoryWerthamer et al. (1966) was not observed: the use of such theory to extract $`H_{c2}(0)`$ was shown to produce an underestimated value. By guessing from Ref. Boebinger et al., 1988 a plausible enhancement factor of 2 in our datum, we point out that eq. (1) would predict a still smaller $`\xi `$ ($`2`$ nm), which has an important role in the discussion that will follow.
b) It is known that sample granularity enhances the measured $`H_{c2}(0)`$ values due to the onset of 0-D fluctuations, as detected in conductivity measurements in K3C60.Hou et al. (1994) This effect is expected to become dramatic when the grain size $`d`$ becomes comparable to $`\xi `$. Indeed, also conventional superconductors like Al, in a suitable fine granular form, can have an upper critical field nearly two orders of magnitude larger than that of bulk samples.Abeles et al. (1967) The granularity of the material we have investigated, however, involves an average particle size of $`2`$ $`\mu `$m, which is more than three orders of magnitude larger than any estimate for $`\xi `$, thus allowing us to definitely exclude any appreciable $`H_{c2}`$ enhancement effect due to granularity.

In conclusion we can state that the coherence length we find from $`H_{c2}`$ measurements is accurate and, due to its inverse square-root dependence from $`H_{c2}`$, even large uncertainties in the determination of the latter would not appreciably affect the $`\xi `$ value.

## IV Muon Spin Rotation Measurements

As briefly described in Sec. II, $`\mu `$SR damping rate measurements yield a reasonable value for the penetration depth $`\lambda `$, even for an irregular flux-line configuration, typical for powders or polycrystalline samples. In our experiment the sample was field-cooled in an external transverse field of 50 G from above $`T_c`$ and the muon precession histograms measured at fixed $`T`$. The presence of two precessing signals at all temperatures indicated that a fraction of the total muons came at rest in the sample holder while the other in the sample. The two components could be easily singled out thanks to their differences not only in amplitude, but mainly in their precession frequency (diamagnetic shift due to superconducting material) and damping rate (internal field second moment due to flux-line lattice). In accounting for the whole expected signal, a missing fraction was detected: it is well known that this fraction is entirely due to the formation of endohedral muonium — i.e. muonium atoms at rest within the C60 cage — while the formation of muonium adduct radicals is inhibited in C$`{}_{}{}^{n}{}_{60}{}^{}`$ compounds. This fraction is “missing” because, at the applied field of 50 G, its characteristic frequency is too high to be observable at the ISIS facility. In passing, it must be pointed out that this missing muonium fraction is not interesting for the present experiment, where we look for the information yielded by the unbound muons in the material’s interstitial sites.

The signal due to the sample shows a Gaussian decay with a decay rate $`\sigma `$, which was fitted using the function $`\mathrm{sin}(\omega t+\varphi )\mathrm{exp}(\sigma ^2t^2/2)`$. Figure 5 shows the fitted values for $`\sigma `$ in the temperature range 4 $`<T<`$ 15 K. The temperature independent residual value as observed above $`T_c`$ is due to the magnetic field distribution of the randomly oriented nuclear dipoles (1H, 14N, 23Na, 39,40,41K, 13C).

The additional broadening below $`T_c`$, due to the flux-line lattice formation, is smaller than the nuclear term and much smaller than that found in similar fullerides such as Rb3C60 and K3C60.MacFarlane et al. (1998) The superconducting contribution and the normal state nuclear dipole broadening add in quadrature, hence the former ($`\sigma _{\text{sc}}`$) can be extracted. The temperature dependence of $`\sigma _{\text{sc}}`$ was fitted to the phenomenological temperature dependence: $`\sigma _{\text{sc}}(T)=\sigma _{\text{sc}}(0)[1(T/T_c)^\alpha ]`$, which yields $`\sigma _{\text{sc}}(0)=5.510^2`$ $`\mu s^1`$ and $`\alpha =2.55`$. The same experiment was repeated applying a 100 G transverse field; in this case no significant increase in $`\sigma _{\text{sc}}`$ was observed. The value for the London penetration depth $`\lambda `$ can be extracted from eq. (3) which gives $`\lambda =1.40`$ $`\mu `$m. This value is more than two times larger than that of other superconducting fullerides. In thinking of effects that could enhance the measured $`\lambda `$ a possible candidate is the granulometry of the sample, when the particles size is not much larger than $`\lambda `$. But this is just our case, where being $`d\lambda `$, we do expect strong surface effects which tend to increase the measured $`\lambda `$ value with respect to that of a bulk sample. Although we have no means to implement a quantitative correction to the measured value, we can definitely state that it represents an upper limit for the real penetration depth, which certainly cannot be larger than 1.4 $`\mu `$m.

## V Discussion

In the previous section we described the independent measurements of $`H_{c1}`$, $`H_{c2}`$, and $`\lambda `$ and anticipated that they would be used within the framework of the GL-Abrikosov equations (1) and (2). In principle, the knowledge of $`H_{c1}`$ and $`H_{c2}`$ values is sufficient to extract the coherence length $`\xi `$ and the penetration depth $`\lambda `$. The additional experimental value of $`\lambda `$ from $`\mu `$SR measurements helps in checking the internal consistency. From eq. (1) the experimental value of $`H_{c2}=40`$ T yields $`\xi =2.86(8)`$ nm; with this value and the experimental result for $`H_{c1}=0.87`$ G eq. (2) yields $`\lambda =3.82`$ $`\mu `$m. If only $`H_{c1}`$ and $`H_{c2}`$ were measured, the values for $`\xi `$ and $`\lambda `$ (although the latter seems considerably larger than the value found in other superconducting fullerides) would appear acceptable for an extreme type-II superconductor.

The picture appears inconsistent, however, since we must account for the measured value of $`\lambda =1.4`$ $`\mu `$m, which is nearly three times smaller than that predicted by eq. (1) and (2). Such a discrepancy is by no means trivial because, in order to weaken it, one has to make unphysical assumptions on the other measured parameters, i.e. the two critical fields. Indeed, as can be seen from eq. (1) and (2), even quite a small variation in $`\lambda `$ will determine orders of magnitude variations in the critical fields.

As an additional check for the observed discrepancy we have also used some approximate analytical solutions of the GL equations. Specifically, we compute the muon spin depolarization rate $`\sigma _{\text{sc}}`$, which can easily be compared with the experimental value. The calculation requires a numerical solution of the GL equations which was performed using the efficient algorithm developed in Ref. Brandt, 1997. This fast iterative variational procedure, which minimizes the free energy density $`f`$, gives as an output the local magnetic field distribution $`B=B(x,y)`$. The second moment of the local fields, $`\mathrm{\Delta }B`$, yields the damping rate ($`\sigma _{\text{sc}}`$) of the $`\mu `$SR.

The results of this calculation are shown in Fig. 6 which reports the dependence of $`\sigma _{\text{sc}}`$ on the coherence length $`\xi `$ as predicted by the GL equations for a fixed $`H_{c1}=0.87`$ G. The different curves refer to different values of the applied field in the range 5 G $`<B<100`$ G. It appears evident that the maximum predicted value for the muon decay rate at the applied field of 50 G is $`910^3`$ $`\mu `$s-1, much smaller than the measured value of $`5510^3`$ $`\mu `$s-1 and, in any case, too small to be measured. This confirms that the $`H_{c1}`$, $`H_{c2}`$ and $`\lambda `$ values measured in (NH3)0.75NaK2C60 cannot be representative of a superconducting system described by the Ginzburg-Landau theory. In addition, the fact that a series of samples with different ammonia content have critical temperatures inversely proportional to the density of states at the Fermi level, as recalled in the Introduction, is consistent with this conclusion.

Even though the phonon-mediated superconductivity in fullerides is well established, we suggest that polaron-based theories of superconductivity can correctly describe some of these systems, such as those considered in this work. Unlike the BCS or Migdal-Eliashberg alternatives, the polaronic approach does not require the phonon energy scale to be much smaller than that of electrons. In fullerides, indeed, typical phonon energies involved in the superconducting coupling are or the order of 0.15 eV, due to the intra-molecular $`H_\text{g}`$ modes of C60.Gunnarsson (1997) According to the early predictions of N.L. Bulaevskii and co-workersBulaevskii et al. (1984) for the superconducting properties of systems with local pairs, critical fields and critical length values are expected to be significantly different from those of ordinary BCS superconductors; in particular, the lower critical field $`H_{c1}`$ is expected to be much smaller and the penetration depth $`\lambda `$ much larger than the respective BCS counterparts. More recently, a polaron-based analysis has been formulated, with the inclusion of non adiabatic effects in the Migdal-Eliashberg theory, in order to better predict transition temperatures and photoelectron spectra of fullerides.Alexandrov and Kabanov (1996) The presence of charge instabilities or fluctuations (charge disproportion, charge density waves etc.) predicted in polaronic systems manifests itself, indirectly, in superconducting fullerides in the following circumstances: a) the NMR detection of a spin gap in the Na2CsC60 superconductor as due to the presence of Jahn-Teller distorted C$`{}_{}{}^{(2,4)}{}_{60}{}^{}`$ originating from a dynamic charge disproportion;Brouet et al. (2000) and b) the existence of a non-magnetic insulating phase in (NH3)2NaK2C60,Riccò et al. (2002) interpreted in terms of a possible (dynamic) charge disproportion. Polaronic instabilities are in general expected at high values of the electron-phonon coupling constant ($`\lambda _c1.5`$–2).Paci et al. (2002) In the case of fullerides, though, the coupling values suggested by different experimental techniques (even though still under debateGunnarsson and Han (2001)) settle in a $`0.5<\lambda _c<1.2`$ range. The closeness of the upper limit of this range to that of the previously mentioned polaronic superconductivity boundary could suggest a possible role played by polarons in these systems.

## VI Conclusions

In this work we have shown that the magnetic properties of the fullerene based superconductor (NH3)0.75NaK2C60 are quite different from those of other fullerides, namely it displays a very small $`H_{c1}`$ associated with very large $`H_{c2}`$ and $`\lambda `$ values. These results cannot be explained within the framework of the Ginzburg-Landau (GL) theory. It is suggested that the system considered here represents a border-line case, in which the nature of superconducting coupling begins to switch from a phonon-mediated to a polaronic character.

Indeed, electron-phonon interaction could be sufficiently large in general to make it possible for some systems, like (NH3)xNaK2C60, to exhibit an enhancement of the coupling which, in turn, favours the development of polaronic instabilities. In the present situation, specific quantitative predictions for measurable superconducting quantities are needed in order to understand the experimental results and clarify the essential nature of superconductivity in fullerides.

###### Acknowledgements.

We thank Prof. E. H. Brandt who kindly provided us with the simulation code for muon spin depolarization calculations and Dr G. Salviati with Dr N. Armani who performed the SEM granulometry measurements.
We acknowledge the financial support by the EU Improvement of Human Potential (IHP) programme, which sponsored part of our $`\mu `$SR experiments at ISIS facility (UK).