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# Spin Diffusion in Double-Exchange Manganites

## Abstract

The theoretical study of spin diffusion in double-exchange magnets by means of dynamical mean-field theory is presented. We demonstrate that the spin-diffusion coefficient becomes independent of the Hund’s coupling $`J_H`$ in the range of parameters $`J_HSWT`$, $`W`$ being the bandwidth, relevant to colossal magnetoresistive manganites in the metallic part of their phase diagram. Our study reveals a close correspondence as well as some counterintuitive differences between the results on Bethe and hypercubic lattices. Our results are in accord with neutron scattering data and with previous theoretical work for high temperatures.

Spin diffusion dominates the low-$`\omega `$, low-$`𝐤`$ excitation spectrum of a magnet in its paramagnetic state and contains important information about the spin dynamics. In the past, spin diffusion was studied intensively in Heisenberg systems and, recently, has been investigated both theoretically and experimentally for strongly-correlated itinerant magnets.Kopietz ; Bonca ; neutrons  The current growth of interest in spintronics requires understanding how local spins relax through their interactions mediated by itinerant charge carriers rather than through their direct interactions with each other.spintronics  Among such systems are the colossal magnetoresistive (CMR) manganites which are ferromagnetic metals in a large part of their phase diagram.Dagotto  Recent systematic neutron scattering experiments on the ferromagnetic CMR materials revealed a peak centered at $`\omega =0`$ associated with the spin diffusion. This peak was also seen below the ordering temperature indicating electronic inhomogeneity with regions having lower $`T_c`$’s.

In this Letter we present a comprehensive, self-consistent, microscopic calculation of spin diffusion applying dynamical mean-field theory (DMFT) to the double-exchange (DE) model. We demonstrate that the spin-diffusion coefficient $`𝒟_s`$ is related to the local single-particle Green’s function and can be evaluated as a function of doping and temperature. Our results agree quantitatively with neutron scattering data on manganites for a range of doping concentrations. Thus, our approach creates a framework for the self-consistent study of diffusive spin dynamics in many real materials, including magnetically doped semiconductors.

Following the general hydrodynamic arguments of Ref. hydro, , we write the generalized susceptibility of a paramagnet for low energies and long wavelengths as

$`\chi (𝐪,\omega )\chi (𝐪){\displaystyle \frac{𝒟_sq^2}{i\omega +𝒟_sq^2}},`$ (1)
which through the fluctuation-dissipation theorem gives the neutron-scattering dynamical structure factor $`𝒮(𝐪,\omega )2[n_B(\omega )+1]\text{Im}\chi (𝐪,\omega )`$, where $`\chi (𝐪)`$ is the static susceptibility at wave-vector $`𝐪`$ and $`n_B(\omega )=[e^{\omega /T}1]^1`$. We take $`\mathrm{}=k_B=1`$ throughout this paper. Further, the generalized susceptibility can be related to the spin current-current correlation function using the dispersion relationsMaleev  and the continuity equation $`S^\alpha (𝐫,t)/t=_ij_i^\alpha (𝐫,t)`$:

$`\chi (𝐪,\omega )={\displaystyle \frac{q^2a^2}{\omega ^2}}\left[\mathrm{\Pi }(𝐪,\omega )\mathrm{\Pi }(𝐪,0)\right],`$ (2)
where $`\mathrm{\Pi }_{ij}^{\alpha \beta }(𝐪,\omega )=i𝑑te^{i\omega t}\theta (t)[j_i^\alpha (𝐪,t),j_j^\beta (𝐪,0)]`$ is the retarded current-current correlation functionMahan , $`j_i^\alpha (𝐪,t)`$ is the $`i`$th component of the spin current for the $`\alpha `$-spin projection, $`i=1\mathrm{}d`$, $`d`$ is the dimensionality, and $`a`$ is the lattice constant. We use the isotropy of the spins above $`T_c`$ and assume the isotropy of real space to suppress the indices in $`\mathrm{\Pi }_{ij}^{\alpha \beta }(𝐪,\omega )=\mathrm{\Pi }(𝐪,\omega )\delta _{\alpha \beta }\delta _{ij}`$. Combining Eqs. (1) and (2) in the $`𝐪,\omega 0`$ limit, we write the Einstein relation between the spin-diffusion coefficient and the spin conductivity $`\sigma _s`$ (which in general is distinct from the particle conductivity) as

$`𝒟_s\chi =\sigma _s=a^2\underset{\omega 0}{lim}{\displaystyle \frac{\text{Im}[\mathrm{\Pi }(0,\omega )]}{\omega }},`$ (3)
where $`\chi =\chi (𝐪=0)`$. These expressions are general and do not depend on the microscopic model.

We now consider the DE model with Hamiltonian

$`=t{\displaystyle \underset{ij\sigma }{}}\left(c_{i\sigma }^{}c_{j\sigma }+\text{H.c.}\right)2J_H{\displaystyle \underset{i}{}}𝐒_i𝐬_i,`$ (4)
where $`t`$ is the nearest-neighbor kinetic energy, $`J_H`$ is the Hund’s coupling between the local Mn3+ $`S=3/2`$ spin and the electronic spin $`𝐬=c_\gamma ^{}\widehat{𝝈}_{\gamma \delta }c_\delta /2`$, and $`\widehat{𝝈}`$ are the Pauli matrices. To describe the multitude of phases in manganites requires that the orbital, phonon, or Jahn-Teller terms be included in the above model.Millis  However, the magnetic properties of these materials in the metallic part of their phase diagram, such as the magnetic excitation spectrum and the ferromagnetic transition temperature,Furukawa ; Golosov ; Bishop  are quantitatively well described by the model in Eq. (4). Therefore, such a model must be also capable of describing spin diffusion in these systems.remark2  Regardless of modifications of the DE model needed to describe a particular real system, elucidating the dynamic properties of this basic model of strongly-correlated itinerant magnets is an important task on its own.

Within the DE model there is no direct interaction between the local spins. Thus, the total on-site spin $`𝐒_l^{tot}=𝐒_l+𝐬_l`$ commutes with the exchange part of Eq. (4) and the spin current can be expressed in terms of electronic operators only:RF1  $`j_i^\alpha (𝐪)=_𝐤v_𝐤^ic_{𝐤,\gamma }^{}\widehat{\sigma }_{\gamma \delta }^\alpha c_{𝐤𝐪,\delta }/2`$, where $`v_𝐤^i=^i\epsilon _𝐤`$ and $`\epsilon _𝐤=2t_{i=1}^d\mathrm{cos}k_ia`$. This is simply another way of saying that electrons mediate the magnetic relaxation processes in an itinerant system.

The physical situation relevant to manganites corresponds to strong Hund’s coupling $`J_HSW`$. Since the characteristic relaxation time for the electronic spin is short and the spin relaxation is essentially local, perturbative approaches to the spin diffusionZou  are inapplicable. Therefore, we employ DMFT, which takes into account the local dynamics in strongly-correlated systems and has been successfully applied to a number of problems.DMFT\_review ; DMFT\_caution  Using DMFT also simplifies our problem significantly because the higher-order diagrams in the current-current correlation function of Eq. (3), often referred to as vertex corrections, are identically zero within this approach.DMFT\_review

Thus, to evaluate the spin-diffusion coefficient we apply the standard Matsubara formalism to Eq. (3) using the above definition of the spin current:

$`{\displaystyle \frac{𝒟_s\chi }{a^2}}={\displaystyle \frac{\pi }{2}}{\displaystyle \underset{𝐤}{}}(v_𝐤^i)^2{\displaystyle _{\mathrm{}}^{\mathrm{}}}𝑑\nu A_𝐤(\nu )^2\left({\displaystyle \frac{n(x)}{x}}|_{x=\nu }\right),`$ (5)
where $`𝐤`$ and $`\nu `$ are the internal momentum and frequency of the “bubble” diagram, respectively. Here $`v_𝐤^i=2t\mathrm{sin}k_ia`$, $`A_𝐤(\nu )=(1/\pi )\text{Im}G_𝐤(\nu )`$ is the electronic spectral function, $`n(\nu )=[e^{(\nu \mu )/T}+1]^1`$ is the Fermi function, and $`\mu `$ is the chemical potential.

The DMFT imposes a special form of the Green’s function in which the self-energy is $`𝐤`$-independent and is defined from a self-consistency condition specified below. Within the DMFT parameters of the model are rescaled such that $`\overline{t}=t\sqrt{z}`$ is finite as the dimensionality $`d\mathrm{}`$, where $`z=2d`$ is the number of nearest neighbors.DMFT\_review  In the following $`\sqrt{2}\overline{t}`$ is set to unity. Generally, the $`d=\mathrm{}`$ limit is well defined for Bethe and hypercubic lattice geometries. While the semicircular electronic density of states (DOS) of the Bethe lattice is convenient for calculations, the Bethe lattice itself lacks the translational invariance and inversion symmetry implicitly used to obtain Eq. (5). Thus, it is important to determine whether the results on the Bethe lattice are equivalent to the results on the hypercubic lattice, which is free from such deficiencies. Since many problems have been studied using the Bethe lattice,DMFT\_review  this comparison will have an even broader significance for the DMFT in general.

We briefly sketch here the DMFT equations for the DE model.Furukawa ; Auslender  Since the self-energy is local, one can change $`G_𝐤(E)G_\epsilon (E)=[E\epsilon \mathrm{\Sigma }(E)]^1`$, and $`_𝐤𝑑\epsilon \rho _0(\epsilon )`$, where $`\epsilon =\epsilon _𝐤`$, and $`\rho _0^B(\epsilon )=\sqrt{2\epsilon ^2}/\pi `$ and $`\rho _0^H(\epsilon )=\mathrm{exp}(\epsilon ^2)/\sqrt{\pi }`$ are the bare DOS’s for Bethe and hypercubic lattices, respectively. The properties of the system are obtained from the local Green’s function:

$`g(E)={\displaystyle 𝑑\epsilon \frac{\rho _0(\epsilon )}{E\epsilon \mathrm{\Sigma }(E)}},`$ (6)
where the self-energy is defined from $`\mathrm{\Sigma }(E)=g_0^1(E)g^1(E)`$, reminiscent of the Dyson equation, where $`g_0^1(E)`$ is the “Weiss” function containing the dynamic influence of the environment on a given local site. The solution of the single-site problem provides a relation between $`g_0(E)`$ and $`\mathrm{\Sigma }(E)`$.Furukawa ; DMFT\_review  In the paramagnetic state and in the quasiclassical limit $`S1`$, such a relation is particularly simple:Furukawa  $`\mathrm{\Sigma }(E)=(J_HS)^2g_0(E)`$, which yields

$`g(E)={\displaystyle \frac{\mathrm{\Sigma }(E)}{(J_HS)^2\mathrm{\Sigma }(E)^2}}.`$ (7)
Together with Eq. (6), this gives a self-consistent condition for $`\mathrm{\Sigma }(E)`$ or $`g(E)`$.

We now compare the Bethe and hypercubic solution for the single-particle properties. Fig. 1 shows the evolution of the interacting DOS $`N(\omega )=(1/\pi )\text{Im}g(\omega )`$ for several values of $`J_HS`$. The band splits as $`J_H`$ increases and both lattice geometries exhibit the same qualitative behavior. Since the hypercubic DOS is expected to have in-gap states, one may ask whether the metal-insulator transition is well defined for a half-filled band. We find that the band splitting in the Bethe and hypercubic lattices happens at the same critical value $`(J_HS)_c=1/\sqrt{2}`$. At the transition, the imaginary part of the self-energy at $`\omega =0`$ vanishes and the real part diverges. As a result, $`N(\omega =0)`$ is exactly zero for $`J_H>J_H^c`$ and the metal-insulator transition for the half-filled band in the hypercubic geometry is well defined.Anokhin  At small energies, $`N(\omega )e^{(J_HS)^4/\omega ^2}`$ vanishes quite abruptly.remark3  In contrast, the “outer” tails of the upper and lower bands behave very similar to the “bare” Gaussian form. Note that for $`J_HS1`$, the form of $`N(\omega )`$ for each subband is rather insensitive to the further increase of $`J_H`$.

We now rewrite Eq. (5) for the spin-diffusion coefficient within the DMFT:

$`{\displaystyle \frac{𝒟_s\chi }{a^2}}={\displaystyle \frac{1}{2z}}{\displaystyle _{\mathrm{}}^{\mathrm{}}}𝑑\nu \left({\displaystyle \frac{n(x)}{x}}|_{x=\nu }\right)\left[{\displaystyle \frac{1}{b}}{\displaystyle \frac{}{b}}\right]\widehat{A}(\nu ),`$ (8)
where $`b=\text{Im}\mathrm{\Sigma }(\nu )`$ and $`\widehat{A}(\nu )=𝑑\epsilon \widehat{\rho }_0^\alpha (\epsilon )A_\epsilon (\nu )`$ with $`\widehat{\rho }_0^\alpha (\epsilon )`$ being the “current” DOS defined from the transformation $`_𝐤\mathrm{sin}^2k_ia𝑑\epsilon \widehat{\rho }_0(\epsilon )`$.Chardopathy  For the hypercubic lattice $`\widehat{\rho }_0^H(\epsilon )=\rho _0^H(\epsilon )/2`$ while for the Bethe lattice $`\widehat{\rho }_0^B(\epsilon )=(2\epsilon ^2)\rho _0^B(\epsilon )/3`$. To obtain Eq. (8) we used the relation $`A_\epsilon (\nu )^2=\left[1/b/b\right]A_\epsilon (\nu )/2\pi `$. Since the spin conductivity is proportional to the correlation function of two spin currents, each scaling as $`t1/\sqrt{z}`$, the prefactor in Eq. (8) contains $`1/z`$. This means that $`d𝒟_s\chi `$ is finite as $`d\mathrm{}`$, similar to the particle conductivity.Metzner

In the manganites, the Curie temperature $`T_c`$ is much smaller than either the Hund’s coupling or the bandwidth, in agreement with DMFT and Monte Carlo calculations for the DE model.Furukawa ; Furukawa1  Therefore, all realistic temperatures are much smaller than the bandwidth $`TW`$ and the derivative of the Fermi-function in the integrand of Eq. (8) should be replaced by a $`\delta `$-function at the chemical potential. Then, combining Eq. (8) with the specific form of the DOS’s for the Bethe and hypercubic lattices, one arrives at:

$`{\displaystyle \frac{𝒟_s\chi z}{a^2}}=\{\begin{array}{c}\frac{1}{6\pi }\left(2\frac{g^{\prime \prime }}{b}(22b^2f^2)fg^{}\right)_{\nu =\mu }^B,\\ \frac{1}{4\pi }\left(2\frac{g^{\prime \prime }}{b}(12b^2)2fg^{}\right)_{\nu =\mu }^H,\end{array}`$ (11)
where $`g^{}=\text{Re}g(\nu )`$, $`g^{\prime \prime }=\text{Im}g(\nu )`$, and $`f=\nu \text{Re}\mathrm{\Sigma }(\nu )`$. Thus, the spin-diffusion coefficient is expressed through the local electronic Green’s function and self-energy only. Fig. 2 presents $`𝒟_s\chi `$ as a function of the electronic concentration $`n`$ for several $`J_HS`$. As $`n`$ varies from 0 to 1, the chemical potential sweeps from $`\omega =\mathrm{}`$ to $`\omega =0`$ in Fig. 1. The results are very similar in both geometries and become independent of $`J_HS`$ as $`J_HS\mathrm{}`$ with the maximum located at $`n=0.5`$. In the limit $`J_HS1`$, Eq. (11) yields a numerical value for this maximum in $`𝒟_s\chi z/a^2`$: $`5/6\pi (=0.265)`$ and $`0.292`$ for the Bethe and hypercubic case, respectively. This demonstrates a close quantitative correspondence between the results in the Bethe and hypercubic lattices, which justifies the use of the former despite the concerns outlined earlier. An interesting feature appears in the results for the hypercubic lattice as $`n0`$. Instead of vanishing, the spin-diffusion coefficient tends to a finite limit $`𝒟_s\chi z/a^2=1/4\pi (J_HS)^2`$, shown by circles in Fig. 2.Remark4

In the high-temperature limit $`TJ_HS1`$ Eq. (8) yields the result $`𝒟_s\chi 1/T`$ obtained previously using a Tchebycheff bounds (TB) formalism.RF2  Numerically, $`(𝒟_s^{DMFT}/𝒟_s^{TB})_{Bethe}=40\sqrt{2}/9\pi ^{3/2}=1.13`$ agree very closely as well.

It is interesting to analyze our results in the context of CMR materials. The superexchange (SE) interaction is often discussedDagotto  as necessary to correct the DE model. Within DMFT, the SE coupling $`J^{SE}`$ must scale as $`1/z`$. Combining this with the result of Ref. Kopietz,  one finds that $`𝒟_s^{SE}1/z^{3/2}`$ is suppressed in comparison with the DE result $`𝒟_s1/z`$. This also serves as a demonstration that the DE model cannot be simply reduced to an effective Heisenberg model. In a real $`d=3`$ material the role of SE is further reduced by the smallness of $`J_{ij}^{SE}t^2/J_HS`$ in comparison with the kinetic energy $`xt`$. Therefore, the DE must dominate the spin diffusion and one can expect our results to be valid not only for the metallic part of the CMR phase diagram ($`x=\mathrm{0.22..0.5}`$ for La1-xCaxO3, $`n=1x`$ in Fig. 2) but also for the ferromagnetic insulating phase ($`x0.22`$).Remark5  Of course, in the limit $`x0`$ DE will diminish and the SE will dominate. Also, the critical scaling in the mixed phase $`0<x<0.12`$ (with a mixture of antiferromagnetic and ferromagnetic orders) can be strongly modified.Kiselev  These cases require separate consideration. At $`x0.5`$ charge ordering prevents the DE mechanism from being operative.

A systematic neutron scattering study of the metallic manganites recently focused on spin diffusion.neutrons  The width of the observed peak in $`𝒮(𝐪,\omega )`$ centered at $`\omega =0`$ scales as $`\mathrm{\Lambda }q^2`$, where $`\mathrm{\Lambda }=2𝒟_s`$. Experimental results taken at $`T^{exp}(x)1.1T_c(x)`$, where $`T_c(x)`$ is the Curie temperature for a given hole concentration $`x`$, give $`\mathrm{\Lambda }=1530`$ meVÅ2. To compare our results to experiments we use $`z=6`$ and $`a=3.87`$ Å. But keep in mind that spin diffusion persists below the transition point and that, at least for the experimentally accessible wave-vectors, the correlation length saturates at about 20 Å. This implies that local magnetic correlations are suppressed by electronic inhomogeneities, which are probably associated with the local charge ordering.neutrons  So for simplicity, we take the susceptibility in the Curie form $`\chi ^{exp}=S^{}(S^{}+1)/3T^{}`$, where $`S^{}(x)=S+(1x)/2`$ is an average on-site spin and $`T^{}=T^{exp}(x)`$ is known from Ref. neutrons, . Fig. 3 shows the theoretical data for $`𝒟_s\chi /a^2`$ for $`J_HS1`$ from Eq. (11) as a function of $`x`$ together with experimental $`𝒟_s^{exp}\chi ^{exp}/a^2`$. We note here, that the theoretical curves in Fig. 3 are virtually independent of the actual value of $`J_HS`$ for $`J_HS1`$. This figure demonstrates a remarkable agreement between the experimental and theoretical results, which contains no fitting parameters. Further improvement of the agreement can be sought, for example, from taking into account the second $`e_g`$ band which would effectively reduce $`J_H/W`$.remark2

Since various other experiments also indicate the presence of local inhomogeneities in CMR systems,Adams  we propose the following analysis. As $`𝐪`$ decreases, long-range magnetic correlations must dominate $`\chi (𝐪)`$ and the magnetic correlation length must eventually exceed the size of the local polaronic distortions. So at a fixed temperature close to $`T_c`$, $`\chi ^{exp}(𝐪)`$ will increase and there will be a systematic decrease in the observed value of $`𝒟_s^{exp}1/\chi `$. This set of measurements would provide further information about magnetic correlations within the inhomogeneities in CMR systems.

In conclusion, we have presented a self-consistent study of the spin-diffusion in the double-exchange magnets within the framework of DMFT. This non-perturbative approach allows us to calculate the spin-diffusion coefficient at any temperature down to a transition point. A good agreement with the experiments in the ferromagnetic CMR manganites and earlier work is found. Altogether, this provides a new insight into the dynamics of strongly-correlated itinerant magnets.

We would like to acknowledge valuable discussions with A. H. Castro Neto, P. Dai, J. Fernandez-Baca, M. Jarrell, M. N. Kiselev, V. Perebeinos, and A. G. Yashenkin. This research was supported by ORNL, managed by UT-Battelle, LLC, for the U.S. DOE under contract DE-AC05-00OR22725.


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# Understanding Paramagnetic Spin Correlations in the Spin-Liquid Pyrochlore Tb2Ti2O7

## Abstract

Recent elastic and inelastic neutron scattering studies of the highly frustrated pyrochlore antiferromagnet Tb2Ti2O7 have shown some very intriguing features that cannot be modeled by the local $`111`$ classical Ising model, naively expected to describe this system at low temperatures. Using the random phase approximation to take into account fluctuations between the ground state doublet and the first excited doublet, we successfully describe the elastic neutron scattering pattern and dispersion relations in Tb2Ti2O7, semi-quantitatively consistent with experimental observations.

The search for the physical realization of a spin liquid in three dimensions has been a long quest for the condensed matter community. Recently, geometrically frustrated magnetic systems have been the focus of intensive experimental and theoretical studies because it is believed that geometrical frustration can inhibit the formation of long-range order, thus enabling the system to remain paramagnetic down to low temperatures. Among three-dimensional systems, the pyrochlore lattice of corner-sharing tetrahedra have been studied extensively. It has been shown theoretically and numerically Villain (1979); Reimers (1992); Moessner and Chalker (1998) that for classical Heisenberg spins with nearest-neighbor antiferromagnetic (AF) exchange, there is no transition to long-range magnetic order at finite temperature. This makes AF materials based on the pyrochlore lattice excellent candidates to search for the low-temperature spin liquid state. A number of experimental studies on insulating pyrochlore materials have been carried out. Interestingly, most materials either develop long-range Néel order, such as Gd2Ti2O7 Ramirez (2002) and Er2Ti2O7 Champion et al. , or reveal spin-glass behavior, such as Y2Mo2O7 Keren and Gardner (2001). The “spin ice” materials, Ho2Ti2O7 Harris et al. (1997); Bramwell et al. (2001) and Dy2Ti2O7 Ramirez et al. (1999); den Hertog and Gingras (2000) exhibit low-temperature thermodynamic properties reminiscent of Pauling’s “water ice model” Bramwell and Gingras (2002). In these systems, an effective ferromagnetic interaction is frustrated due to the single-ion $`111`$ Ising anisotropy Bramwell and Harris (1998); Bramwell and Gingras (2002). The behavior of these systems can be quantitatively described by the $`111`$ Ising spin model with nearest-neighbor exchange and long-range dipolar interactions den Hertog and Gingras (2000); Bramwell et al. (2001); Bramwell and Gingras (2002).

Tb2Ti2O7 shows, however, very different and intriguing behavior. It is believed that Tb2Ti2O7 belongs to the same family of $`111`$ Ising systems as Dy2Ti2O7 and Ho2Ti2O7 but with an effective nearest neighbor AF interaction Gardner et al. (1999); den Hertog and Gingras (2000); Gingras et al. (2000); Gingras and den Hertog (2002); Gardner et al. (2001). The same spin model that very successfully described the spin-ice systems predicts it to have a noncollinear Néel $`𝐐=0`$ order, with all spins pointing into or out of each tetrahedron, at about 1 K den Hertog and Gingras (2000). In dramatic contrast, Tb2Ti2O7 remains a spin liquid, or “cooperative paramagnet”, down to 70mK Gardner et al. (1999, 2001). In addition, recent paramagnetic neutron scattering studies show that the scattering pattern for this material is not consistent with a $`111`$ Ising model, while a Heisenberg spin model Gardner et al. (2001); Enjalran and Gingras  or some level of relaxation away from the $`111`$ Ising model Yasui et al. (2002) can better describe the observed neutron scattering pattern. These results suggest that the restoration of spin isotropy in the system, despite its expected Ising-like nature at low temperature Gingras et al. (2000); Siddharthan et al. (1999); Rosenkranz et al. (2000); Rosenkranz , is essential in understanding the paramagnetic spin correlations. Inelastic neutron scattering studies have also been performed on this system and partial softening of the magnetic excitations at an energy of about 20 K has been observed Gardner et al. (1999, 2001); Kanada et al. (1999). This has been attributed to a (spin) roton-like mode, as in liquid 4He Gardner et al. (1999, 2001); Feynman (1955), which further indicates a more isotropic nature of the spins. Given the ensemble of evidences, it would appear that one needs a more isotropic spin model to understand the paramagnetic spin correlations in this system. More importantly, such a “restoration” of spin isotropy may also be the key to understanding why Tb2Ti2O7 fails to order down to low temperatures. In this paper, we employ the random-phase approximation (RPA) Jensen and Mackintosh (1991) to take into account the fluctuations between the ground state doublet and the first excited doublet. We successfully describe the observed paramagnetic spin correlations in Tb2Ti2O7, without any assumptions regarding the nature of the spins, while we still obtain the $`𝐐=0`$ Néel order at low temperatures. This result makes the fact that Tb2Ti2O7 fails to order even more puzzling.

We begin with the model spin Hamiltonian,

$$=\frac{1}{2}\underset{i,j,\alpha ,\beta ,a,b}{}S_{i,a}^\alpha 𝒥_{ab}^{\alpha \beta }(i,j)S_{j,b}^\beta +\underset{i,a}{}_{\mathrm{CF}}(i,a),$$
(1)
where $`i,j`$ are indices of the Bravais lattice vectors for the FCC lattice, $`a,b`$ are indices of sublattice basis vectors and $`\alpha ,\beta `$ are indices for the spatial coordinates. $`_{\mathrm{CF}}`$ is the single-ion crystal field (CF) Hamiltonian. The spin-spin interaction matrix $`𝒥`$, including both exchange and long-range dipolar interactions, reads

$$𝒥_{ab}^{\alpha \beta }(i,j)=J_1\delta ^{\alpha \beta }\delta _{nn}+D_{dd}\left[\frac{\delta ^{\alpha \beta }}{|𝐑_{ij}^{ab}|^3}\frac{3R_{ij}^{ab,\alpha }R_{ij}^{ab,\beta }}{|𝐑_{ij}^{ab}|^5}\right],$$

where $`\delta _{nn}`$ refers to nearest-neighbor interaction, and $`R_{ij}^{ab,\alpha }`$ denotes the $`\alpha `$ component of the interspin vector $`𝐑_{ij}^{ab}`$ that connects spins $`𝐒_{i,a}`$ and $`𝐒_{j,b}`$. The nearest-neighbor exchange for Tb2Ti2O7 is given by $`J_10.167`$ K exc , and $`D_{dd}=(g\mu _B)^2\mu _0/4\pi `$, where $`\mu _B`$ is the Bohr magneton, $`\mu _0`$ the magnetic permeability, and $`g=3/2`$ for Tb3+.

The single-ion susceptibility is given by Jensen and Mackintosh (1991)

$`\chi _a^{0,\alpha \beta }(\omega )`$ $`=`$ $`{\displaystyle \underset{\mu ,\nu }{\overset{E_\mu E_\nu }{}}}{\displaystyle \frac{M_{\nu \mu ,a}^\alpha M_{\mu \nu ,a}^\beta }{E_\mu E_\nu \mathrm{}(\omega +i0^+)}}(n_\nu n_\mu )`$ (2)
$`+{\displaystyle \frac{\delta (\omega )}{k_BT}}{\displaystyle \underset{\mu ,\nu }{\overset{E_\mu =E_\nu }{}}}M_{\nu \mu ,a}^\alpha M_{\mu \nu ,a}^\beta n_\nu ,`$
where $`n_\nu `$ is the thermal occupation fraction for state $`\nu `$. The matrix elements for the single-ion states are given by $`M_{\nu \mu ,a}^\alpha =_{\overline{\alpha }}\nu |S^{\overline{\alpha }}|\mu u_{\overline{\alpha },a}^\alpha `$, where $`u_{\overline{\alpha },a}^\alpha `$ is the rotation matrix from the local ($`\overline{\alpha }`$) frame defined on sublattice $`a`$ to the global ($`\alpha `$) frame. The spin operator $`S^{\overline{\alpha }}`$ acts on the CF states defined along the local quantization axis Gingras et al. (2000). The local wave function structure has been obtained from both experimental measurements and theoretical calculations Gingras et al. (2000); Rosenkranz et al. (2000); Rosenkranz . The primary components are $`J_z`$ eigenstates $`|\pm 4`$ for the ground state doublet and $`|\pm 5`$ for the first-excited state doublet. The doublets are separated by an anisotropy gap $`\mathrm{\Delta }20`$ K, which is comparable with the Curie-Weiss temperature $`\theta _{\mathrm{CW}}19`$ K Gingras et al. (2000).

The RPA equation which takes into account the two-ion interaction contribution to the full susceptibility Jensen and Mackintosh (1991) is given by

$$\chi _{ab}^{\alpha \beta }(𝐪,\omega )+\underset{\gamma ,\delta ,c}{}\chi _a^{0,\alpha \gamma }(\omega )𝒥_{ac}^{\gamma \delta }(𝐪)\chi _{cb}^{\delta \beta }(𝐪,\omega )=\delta _{ab}^{}\chi _a^{0,\alpha \beta }(\omega ),$$

where $`𝒥(𝐪)`$ is the Fourier transformation of the interaction matrix $`𝒥(i,j)`$. The slowly converging, infinite lattice sum of the dipolar interaction is handled using Ewald summation techniques Born and Huang (1968); Enjalran and Gingras . We solve for $`\chi _{ab}^{\alpha \beta }(𝐪,\omega )`$ numerically using LAPACK routines.

The elastic and dynamical neutron cross-sections are related to the spin susceptibilities by summing over the sublattice contributions and taking the transverse components of $`𝐒`$ perpendicular to $`𝐐`$ Jensen and Mackintosh (1991),

$`S_{\mathrm{el}}(𝐐)`$ $``$ $`{\displaystyle \frac{|F(𝐐)|^2}{k_BT}}{\displaystyle \underset{\alpha ,\beta ;a,b}{}}(\delta _{\alpha \beta }\widehat{Q}_\alpha \widehat{Q}_\beta )`$ (3a)
$`\times `$ $`\mathrm{exp}\left[i(𝐫^a𝐫^b)𝐆\right]\text{Re}\chi _{ab}^{\alpha \beta }(𝐪);`$
$`S_{\mathrm{dyn}}(𝐐,\omega )`$ $``$ $`{\displaystyle \frac{|F(𝐐)|^2}{1\mathrm{exp}(\mathrm{}\omega /k_BT)}}{\displaystyle \underset{\alpha ,\beta ;a,b}{}}(\delta _{\alpha \beta }\widehat{Q}_\alpha \widehat{Q}_\beta )`$ (3b)
$`\times `$ $`\mathrm{exp}\left[i(𝐫^a𝐫^b)𝐆\right]\text{Im}\chi _{ab}^{\alpha \beta }(𝐪,\omega ),`$
where $`𝐐=𝐆+𝐪`$, $`𝐆`$ is a reciprocal lattice vector of the FCC lattice, and $`𝐪`$ is a primitive vector in the first Brillouin zone. $`𝐫^a`$ is the sublattice basis vector and $`F(𝐐)`$ is the magnetic form factor for Tb3+.

Figure 1a shows the experimental scattering pattern in the $`(h,h,l)`$ plane at 9 K Gardner et al. (2001). Note that there is a strong intensity maximum around $`(0,0,2)`$. Figure 1b shows the $`S(𝐐)`$ calculation using the $`111`$ Ising model, i.e., the anisotropy gap $`\mathrm{\Delta }\mathrm{}`$. It is clear that this model fails to reproduce the correct neutron scattering pattern as observed experimentally, as there is only weak non-critical intensity around $`(0,0,2)`$. It has been shown that in the $`111`$ Ising model, the intensity at $`(0,0,2)`$ and $`(0,0,0)`$ are exactly correlated, and vanishes for Tb2Ti2O7 Enjalran and Gingras ; Gardner et al. (2001); Gingras et al. (2000). Using a more realistic doublet-doublet model for Tb2Ti2O7, we are able to qualitatively reproduce the experimentally observed scattering pattern (Fig. 1c). It captures most details of the experimental pattern, such as the intensity maximum around $`(0,0,2)`$, the minima around $`(0,0,0)`$, $`(2,2,2)`$ and $`(0,0,4)`$. This excellent agreement between theory and experiment indicates that to properly understand the spin correlations in Tb2Ti2O7, the fluctuations out of the ground state doublet to the first excited doublet, originating from the first term in Eq. (2), are important. It should be noted that this result is obtained from the simple level scheme described above with no other assumptions about the nature of the spin or the details of the wave functions.

Line scans in reciprocal space along three high-symmetry directions $`(0,0,l)`$, $`(h,h,0)`$ and $`(h,h,h)`$ at $`T=`$4 K are plotted in Fig. 2. Open symbols are the data points for $`S(𝐐)`$. Filled symbols are the dispersion relations $`E(𝐐)`$ for the lowest-energy band of magnetic excitations at 4 K. The dispersion relations show good semi-quantitative agreement with the experimental dispersion observed in single crystal Tb2Ti2O7 reported in Fig. 9 of Ref. Gardner et al., 2001. We also find that the minimum in $`E(𝐐)`$ corresponds to the maximum in $`S(𝐐)`$ in all symmetry directions, as is observed in the experiment. The sharp jumps in dispersions, e.g., near $`(0,0,1)`$ and $`(0,0,3)`$, correspond to shifts of spectral maximum between different branches, since the experiment and current calculation track only the maximum peaks in the energy spectra. In principle, there should be four branches of magnetic excitations with different intensities due to the four sublattice structure. Higher resolution experiments need to be performed to map out the dispersion relations of these branches.

To study the temperature effects on the dispersion relations of the lowest three bands of magnetic excitations, we use the wave functions obtained from crystal field calculations in the point charge approximation and in the fixed $`J=6`$ manifold for Tb3+ Gingras et al. (2000). This gives the CF level scheme with two low-lying doublets as described above, and two higher-energy singlets Gingras et al. (2000); Gardner et al. (2001). The energy levels are given as 0, 24.6, 113.9 and 132.7K, consistent with experiments. The two higher singlets have large $`|\pm 3`$ contributions and some mixing with other $`|J,M_J`$ components Gingras et al. (2000). All the excited states are connected to the ground state doublet through the $`S^+`$ and $`S^{}`$ operations and the excitations are visible via neutron spectroscopy Gardner et al. (2001). Figure 3 shows the dispersion relations of the three lowest-lying magnetic excitations along $`(h,h,h)`$ at 12 K and 30 K at the same energy scale. The lowest band becomes more dispersive as the temperature is lowered, while the higher two bands do not show much change with temperature.

Fluctuations between the doublets are important in understanding the experimentally observed scattering pattern. These fluctuations originate in the first term of Eq. (2), where the anisotropy gap $`\mathrm{\Delta }=E_1E_0`$ enters the formulation algebraically, instead of exponentially as in the elastic (second) term through the thermal occupation fraction. If the two-ion interaction, characterized by $`\theta _{\mathrm{CW}}`$, is comparable with $`\mathrm{\Delta }`$, then the effect of this term is large and part of the isotropic response is restored. By setting $`\mathrm{\Delta }\mathrm{}`$ or the matrix element between two doublets to zero, this term is eliminated, and the scattering pattern is reduced to that of the $`111`$ Ising model Enjalran and Gingras . This explains why the $`111`$ Ising model works so well in describing the spin correlations in spin ice materials den Hertog and Gingras (2000); Bramwell et al. (2001), since in these systems $`\mathrm{\Delta }200300`$ K Rosenkranz et al. (2000); Rosenkranz  and $`\theta _{\mathrm{CW}}0.52`$ K den Hertog and Gingras (2000); Bramwell et al. (2001); Ramirez et al. (1999), so the effects of the fluctuations out of the ground state doublet are negligible. To understand the different temperature dependencies of the dispersion for the three lowest-lying magnetic excitations, we inspect the thermal factor $`n_{\nu \mu }=n_\nu n_\mu `$ in the first term of Eq. (2). For temperatures much lower than $`\mathrm{\Delta }`$, only the ground state doublet is populated, and this factor is almost the same for all three bands. When the temperature reaches a value $`T\mathrm{\Delta }`$, the first excited state doublet begins to be populated, therefore reducing the factor $`n_{01}=n_0n_1`$, while those for the two higher levels remain essentially unchanged. This change in thermal occupation factor results in a large temperature dependence of the dispersion in the lowest band.

The low temperature ground state of our model in RPA is the noncollinear “all-in” or “all-out” $`𝐐=0`$ Néel state den Hertog and Gingras (2000) with $`T_c1.8`$K. Exact $`T_c`$ value depends on the details of the crystal field wave functions. Suprisingly, this value is very close to the $`T_c`$ obtained recently in hydrostatic pressure measurements for pressure greater than 1 GPa Mirebeau et al. (2002). By standard Holstein-Primakoff expansion aroud this ground state we obtain the spin-wave excitation spectrum with a large gap and the reduction of the staggered magnetization due to quantum fluctuations $`\mathrm{\Delta }m/m<10^4`$Del Masetro and Gingras . This result should be taken only as an indicator, though, since the ground state doublet ($`M_J=\pm 4`$) is not at its saturation value $`M_J=\pm 6`$ due to the crystal field interaction. The magnetic ground state doublet is a non-Kramers doublet, and the states are time-conjugate of each other, so there exist no matrix elements between them Abragam and Bleaney (1970), indicating that any quantum fluctuations causing spins to flip result from a higher-order virtual process via excited crystal field levels.

In conclusion, with a simple level scheme and the RPA to include the fluctuations between the ground state and the first excited state doublets, we are able to describe semi-quantitatively the experimentally observed neutron scattering pattern and the energy dispersion in Tb2Ti2O7. Our results indicate that the crystal field effects are important in this system due to the fact that the anisotropy gap and the two-ion interaction are comparable, and that some isotropy is present in the response. The ground state of our model, however, is still the “all-in” or “all-out” $`𝐐=0`$ Néel state den Hertog and Gingras (2000) with $`T_c1.8`$K, which is stable against the lowest order quantum fluctuations. These results indicate that a mechanism that may restore more isotropy and thus increase the quantum fluctuations leading to the suppression of $`T_c`$, requires further detailed study.

We thank B. Buyers, B. Canals, B. Gaulin, J. Gardner and S. Rosenkranz for useful and stimulating discussions. This work is supported by the NSERC of Canada, Research Corporation and the Province of Ontario.


text:
# Magnetically mediated superconductivity: Crossover from cubic to tetragonal lattice

## I Introduction

One can expect that the effective interaction between quasiparticles in strongly correlated electron systems to be very complex. The interaction will depend obviously on the charge, but also more generally on the spin and current carried by the quasiparticles. On the border of long-range magnetic order it is plausible that the dominant interaction channel is of magnetic origin and depends on the relative spin orientations of the interacting quasiparticles.

It has been shown that this magnetic interaction treated at the mean field level can produce anomalous normal state properties and superconducting instabilities to anisotropic pairing states. It correctly predicted the symmetry of the Cooper state in the copper oxide superconductors and is consistent with spin-triplet p-wave pairing in superfluid $`{}_{}{}^{3}He`$ \[for a recent review see, e.g., ref. \]. One also gets the correct order of magnitude of the superconducting and superfluid transition temperature $`T_c`$ when the model parameters are inferred from experiments in the normal state of the above systems. There is growing evidence that the magnetic interaction model may be relevant to other materials on the border of magnetism.

Thus far the magnetic interaction model has been explored in very simple cases. The most extensively investigated example is that of a nearly half-filled single-band in a square or cubic lattice. These studies have revealed a number of interesting features that are quite in contrast to those expected for conventional phonon mediated pairing. In the latter case, the interaction is local in space, but non-local in time, whereas on the border of magnetism, one expects the interaction to be strongly non-local in both space and time. For nearly antiferromagnetic metals the magnetic interaction is oscillatory in space and superconductivity depends on the ability of the electrons in a Cooper pair state to sample mainly the attractive regions of these oscillations. Because of the strong retardation in time, the relative wavefunction of the Cooper pair must be constructed from Bloch states with wavevectors close to the Fermi surface. Furthermore, the allowed symmetries of the Cooper pair wavefunction are restricted by the crystal structure. The possibility of constructing a Cooper pair state with maximum probability in the attractive regions of the magnetic interaction can be severely constrained by these requirements. Therefore, one expects that the robustness of magnetic pairing to be very sensitive to details of the electronic and lattice structures.

On the border of ferromagnetism, one is not hampered by the oscillatory nature of the magnetic interaction which in the simplest model is attractive everywhere in space and time in the spin-triplet channel. At first sight this would seem to be the most favourable case for magnetically mediated superconductivity. However, the results of the numerical calculations presented in ref.  indicate that the highest mean field $`T_c`$ for the cases considered is obtained for d-wave pairing in the nearly antiferromagnetic state in a quasi-2D tetragonal lattice. In this particular case, as explained in ref. , it turns out to be possible to ideally match the Cooper pair state to the attractive regions of the magnetic interaction.

On the border of ferromagnetism, magnetic pairing in the spin-triplet state has the disadvantage that only the exchange of magnetic fluctuations polarised along the direction of the interacting spins, i.e., longitudinal fluctuations, contribute to the quasiparticle interactions. For a spin-rotationally invariant system, both longitudinal and transverse fluctuations contribute to pairing only for a spin-singlet state.

Another disadvantage of being on the border of ferromagnetism is that for otherwise similar conditions the suppression of $`T_c`$ due to the self interaction arising from the exchange of magnetic fluctuations is stronger than in the corresponding case on the border of antiferromagnetism. This disadvantage can be mitigated in systems with strong magnetic anisotropy in that the effect of the transverse magnetic fluctuations on the self interaction would be suppressed while the strength of the pairing interaction arising from the longitudinal magnetic fluctuations need not be reduced. This may apply in systems with strong spin-orbit interactions or in the spin-polarised state close to the border of ferromagnetism.

These arguments  have stimulated a new search for evidence of superconductivity on the border of itinerant electron ferromagnetism in cases where spin anisotropy is expected to be pronounced, such as $`UGe_2`$. This search has proved fruitful because it led to the first observation of the coexistence of superconductivity and itinerant electron ferromagnetism in $`UGe_2`$ and shortly thereafter in $`ZrZn_2`$ and $`URhGe`$.

The prediction of the simple model presented in ref.  that magnetic pairing is more robust in the quasi-2D square lattice than in the cubic structure seems to have been borne out by recent experiments. Namely, one finds an order of magnitude increase in the maximum $`T_c`$ and in the range in pressure where superconductivity is observed on the border of metallic antiferromagnetism when the simple cubic lattice of $`CeIn_3`$ is stretched along one principal axis by the insertion of non-magnetic layers to form the tetragonal compounds $`CeMIn_5`$ ($`M`$ is $`Co`$, $`Rh`$ or $`Ir`$).

These systems, albeit quite anisotropic, would not normally be considered to be quasi-two dimensional and it is not clear at first sight that the model calculations carried out in ref.  are directly relevant. The purpose of this paper is to show that for comparable model parameters, the robustness of magnetic pairing increases gradually as one goes from a cubic structure to a more and more anisotropic structure on the border of metallic antiferromagnetism and ferromagnetism. This behaviour of the mean field transition temperature is in stark contrast to that of the ”one-loop” fluctuations corrections to $`T_c`$. The latter corrections typically depend logarithmically on the degree of anisotropy and would be expected to be negligible for materials such as $`CeMIn_5`$.

We do not expect some of the results of ref.  to be generic properties of the magnetic interaction model. We have already stressed that even in simple cases, the robustness of magnetic pairing can be very sensitive to certain details of the lattice and electronic structure. Even in the single band problem, many such structures have not yet been extensively studied theoretically. Furthermore, we expect that the range of possibilities to be greatly expanded in the presence of more than one partially filled electronic band.

Most known materials on the border of magnetism crystallise in other than simple cubic or tetragonal structure and have more than one band crossing the Fermi level. For these more complex systems, one would not expect the model of ref.  to be directly relevant. For example, the observation of spin-triplet rather than spin-singlet d-wave pairing in some multi-band materials with strongly enhanced antiferromagnetic spin fluctuations, such as $`UPt_3`$ and $`Sr_2RuO_4`$, may not be inconsistent with the idea of magnetic pairing. A detailed study of magnetic pairing in multi-band systems for a range of crystal structures would shed light on the possible forms of superconductivity and the conditions most favorable for their observation.

The simple model calculations suggest that anisotropic forms of superconductivity should be a generic property of systems on the border of metallic magnetism. It may seem surprising therefore that there are still so few observations of this phenomenon. In many cases, the multiplicity of bands and, for example, magnetic fluctuations in the non-bipartite lattice may weaken magnetic pairing to such an extent that quenched disorder may completely suppress superconductivity. An illustration of this point is the dramatic collapse of the spin-triplet superconducting transition temperature in $`Sr_2RuO_4`$ in the presence of $`Al`$ impurity concentrations as low as 0.1%.

At first sight, the magnetic interaction model is mathematically analogous to the conventional electron-phonon problem with the generalised magnetic susceptibility playing the role of the phonon propagator. One would therefore expect that a simple analytic expression similar to that proposed by McMillan could be used to represent approximately the $`T_c`$ calculated numerically via the Eliashberg equations. Our attempts in this direction have not, however, proved successful. A recent study suggests that there may be a fundamental reason for inapplicability of the McMillan-style expression for $`T_c`$. On the border of long-range magnetic order, the incoherent part of the electron Green function, which is ignored in the simplest treatment, plays a major role in the formation of the Cooper pair condensate. The traditional picture in which superconductivity arose from pairing of well defined (weakly damped) quasiparticles appears inadequate on the border of metallic magnetism even in the mean field Eliashberg treatment.

We note that in our model the coupling of the quasiparticles to the magnetic fluctuations is a phenomenological constant to be inferred from normal state properties that formally includes that part of the vertex correction which is local in space and time. Calculations have shown that the neglect of vertex corrections that are non-local in space and time is justified at least in some cases of physical interest. When the magnetic correlation length becomes sufficiently large, however, these neglected non-local vertex corrections (including superconducting phase fluctuations) may become important. Their effect on $`T_c`$ and the normal state properties are as yet incompletely understood.

## II Model

We consider quasiparticles in a simple tetragonal lattice described by a dispersion relation

$`ϵ_𝐩`$ $`=`$ $`2t(\mathrm{cos}(p_x)+\mathrm{cos}(p_y)+\alpha _t\mathrm{cos}(p_z))`$ (1)
$``$ $`4t^{}(\mathrm{cos}(p_x)\mathrm{cos}(p_y)+\alpha _t\mathrm{cos}(p_x)\mathrm{cos}(p_z)+\alpha _t\mathrm{cos}(p_y)\mathrm{cos}(p_z))`$ (2)
with hopping matrix elements $`t`$ and $`t^{}`$. $`\alpha _t`$ represents the electronic structure anisotropy along the z direction. $`\alpha _t=0`$ corresponds to the quasi-2D limit while $`\alpha _t=1`$ corresponds to the 3D cubic lattice. For simplicity, we measure all lengths in units of the respective lattice spacing. In order to reduce the number of independent parameters, we take $`t^{}=0.45t`$ and a band filling factor $`n=1.1`$ as in our earlier work.

The effective interaction between quasiparticles is assumed to be isotropic in spin space and is defined in terms of the coupling constant $`g`$ and the generalised magnetic susceptibility which is assumed to have a simple analytical form consistent with the symmetry of the lattice.

$$\chi (𝐪,\omega )=\frac{\chi _0\kappa _0^2}{\kappa ^2+\widehat{q}^2i\frac{\omega }{\eta (\widehat{q})}}$$
(3)
where $`\kappa `$ and $`\kappa _0`$ are the correlation wavevectors or inverse correlation lengths in units of the lattice spacing in the basal plane, with and without strong magnetic correlations, respectively. Let

$$\widehat{q}_\pm ^2=(4+2\alpha _m)\pm 2(\mathrm{cos}(q_x)+\mathrm{cos}(q_y)+\alpha _m\mathrm{cos}(q_z))$$
(4)
where $`\alpha _m`$ parameterises the magnetic anisotropy. $`\alpha _m=0`$ corresponds to quasi-2D magnetic correlations and $`\alpha _m=1`$ corresponds to 3D magnetic correlations.

In the case of a nearly ferromagnetic metal the parameters $`\widehat{q}^2`$ and $`\eta (\widehat{q})`$ in Eq. (3) are defined as

$`\widehat{q}^2`$ $`=`$ $`\widehat{q}_{}^2`$ (5)
$`\eta (\widehat{q})`$ $`=`$ $`T_{sf}\widehat{q}_{}`$ (6)
where $`T_{sf}`$ is a characteristic spin fluctuation temperature. Note that our definition of $`T_{sf}`$ may differ from the characteristic spin fluctuation temperature scales used by other authors.

In the case of a nearly antiferromagnetic metal, the parameters $`\widehat{q}^2`$ and $`\eta (\widehat{q})`$ in Eq. (3) are defined as

$`\widehat{q}^2`$ $`=`$ $`\widehat{q}_+^2`$ (7)
$`\eta (\widehat{q})`$ $`=`$ $`T_{sf}\widehat{q}_{}`$ (8)
As in our previous work, the band structure and generalized magnetic susceptibility are modeled independently. This choice may be inconsistent when all of the contributions to $`\chi (𝐪,\omega )`$ come from the chosen band. However, it allows us, in principle, to deal with the case where there are other important contributions to the generalized magnetic susceptibility. It has been argued that the latter case is of relevance to the ruthenates, and most likely the heavy-fermion systems.

A complete description of the model, the Eliashberg equations for the superconducting transition temperature and their method of solution can be found in the appendix.

We note that the model is fully defined by the phenomenological parameters describing the electronic structure $`ϵ_𝐩`$, the generalised magnetic susceptibility $`\chi (𝐪,\omega )`$ and the interaction vertex $`g`$. In principle, these parameters can be estimated from experimental studies of the normal state. In particular, the resistivity can be used to estimate the dimensionless coupling parameter $`g^2\chi _0/t`$ the value of which is between 10 and 20 for the simplest RPA model for the magnetic interaction.

## III Results

### A Solution of the Eliashberg Equations for $`T_c`$

The dimensionless parameters at our disposal are $`g^2\chi _0/t`$, $`T_{sf}/t`$, $`\kappa _0`$ and $`\kappa `$. For comparison with the results of our earlier work, we take $`T_{sf}=\frac{2}{3}t`$ and $`\kappa _0^2=12`$. In 2D, this $`T_{sf}`$ corresponds to about $`1000^{}K`$ for a bandwidth of 1 eV while our choice of of $`\kappa _0^2`$ is a representative value.

The results of our numerical calculations of the mean field critical temperature $`T_c`$ as a function of the electronic and magnetic anisotropy parameters $`\alpha _t`$ and $`\alpha _m`$, respectively, are shown in Figs 1 and 2 for representative values of the parameters $`\kappa ^2`$ and $`g^2\chi _0/t`$. Figures 1a-c illustrate the results for a nearly anti-ferromagnetic metal and figures 2a-c for a nearly ferromagnetic metal. Note that our previous calculations correspond to the quasi-2D case $`\alpha _t=\alpha _m=0`$ and to 3D case $`\alpha _t=\alpha _m=1`$.

A glance at figure 1 reveals a clear pattern in the variation of $`T_c`$ with both anisotropy parameters $`\alpha _t`$ and $`\alpha _m`$. We notice that $`T_c`$ increases gradually and monotonically as the system becomes more and more anisotropic in either the electronic structure or in the magnetic interaction. In going from 3D to quasi-2D, $`T_c/T_{sf}`$ is found to increase by up to an order of magnitude for otherwise fixed parameters of the model. The increase becomes least pronounced as for small $`\kappa ^2`$ and large $`g^2\chi _0/t`$.

The behavior in the nearly ferromagnetic case, figure 2, though broadly similar to that of the nearly antiferromagnetic metal, shows some interesting differences. In some cases, the minimum $`T_c`$ occurs for 3D electronic structure, but quasi-2D magnetic interaction. Also, in all cases considered the maximum $`T_c`$ is obtained for a quasi-2D electronic structure and strongly anisotropic, but not 2D magnetic interactions.

### B Mass renormalisation and interaction parameter

In order to make a comparison with the corresponding electron-phonon problem it is instructive to define a mass renormalization parameter $`\lambda _Z`$ and interaction parameter $`\lambda _\mathrm{\Delta }`$. We define

$`\lambda _Z`$ $`=`$ $`{\displaystyle \frac{_{\mathrm{}}^+\mathrm{}\frac{d\omega }{\pi }<\frac{1}{\omega }ImV_Z(𝐩𝐩^{},\omega )>_{FS(𝐩,𝐩^{})}}{<1>_{FS(𝐩)}}}`$ (9)
$`\lambda _\mathrm{\Delta }`$ $`=`$ $`{\displaystyle \frac{_{\mathrm{}}^+\mathrm{}\frac{d\omega }{\pi }<\frac{1}{\omega }ImV_\mathrm{\Delta }(𝐩𝐩^{},\omega )\eta (𝐩)\eta (𝐩^{})>_{FS(𝐩,𝐩^{})}}{<\eta ^2(𝐩)>_{FS(𝐩)}}}`$ (10)
where

$$V_Z(𝐪,\omega )=g^2\chi (𝐪,\omega )$$
(11)
and

$`V_p(𝐪,\omega )`$ $`=`$ $`{\displaystyle \frac{g^2}{3}}\chi (𝐪,\omega )`$ (12)
$`\eta (𝐩)`$ $`=`$ $`\mathrm{sin}(p_x)`$ (13)
for p-wave spin triplet pairing $`(\mathrm{\Delta }p)`$ while

$`V_d(𝐪,\omega )`$ $`=`$ $`g^2\chi (𝐪,\omega )`$ (14)
$`\eta (𝐩)`$ $`=`$ $`\mathrm{cos}(p_x)\mathrm{cos}(p_y)`$ (15)
in the case of d-wave spin-singlet pairing $`(\mathrm{\Delta }d)`$. The Fermi surface averages are given by

$`<\mathrm{}>_{FS(𝐩)}`$ $`=`$ $`{\displaystyle \frac{d^dp}{(2\pi )^d}\mathrm{}\delta (ϵ_𝐩\mu )}`$ (16)
$`<\mathrm{}>_{FS(𝐩,𝐩^{})}`$ $`=`$ $`{\displaystyle \frac{d^dp}{(2\pi )^d}\frac{d^dp^{}}{(2\pi )^d}\mathrm{}\delta (ϵ_𝐩\mu )\delta (ϵ_𝐩^{}\mu )}`$ (17)
In practice, we compute the Fermi surface average with a discrete set of momenta on a cubic or tretragonal lattice and we replace the delta function by a finite temperature expression

$`{\displaystyle \frac{d^dp}{(2\pi )^d}}`$ $``$ $`{\displaystyle \frac{1}{N}}{\displaystyle \underset{𝐩}{}}`$ (18)
$`\delta (ϵ_𝐩\mu )`$ $``$ $`{\displaystyle \frac{1}{T}}f_𝐩(1f_𝐩)`$ (19)
where $`f_𝐩`$ is the Fermi function. Note that $`\frac{1}{T}f_𝐩(1f_𝐩)\delta (ϵ_𝐩\mu )`$ as $`T0`$. We have used $`T=0.1t`$ and $`N=128^d`$ in all of our calculations. The finite temperature effectively means that van Hove singularities will be smeared out.

Note that the Fermi surface average that appears in $`\lambda _Z`$, Eq. (9) plays a role similar to that of $`\alpha ^2F(\omega )/\omega `$ in the case of phonon mediated superconductivity. From the definitions of the parameters $`\lambda _{Z,\mathrm{\Delta }}`$ Eqs. (9), (10) and our model for $`\chi (𝐪,\omega )`$ Eq. (3), we see that $`\lambda _{Z,\mathrm{\Delta }}`$ are directly proportional to the dimensionless factor $`g^2\chi _0\kappa _0^2/t`$. Thus we will consider the quantities

$$\lambda _{Z,\mathrm{\Delta }}^{}\lambda _{Z,\mathrm{\Delta }}/(g^2\chi _0\kappa _0^2/t)$$
(20)
which are functions only of $`n`$, $`t^{}/t`$ and $`\kappa ^2`$.

In figures 3 and 4 we show $`\lambda _Z^{}`$, $`\lambda _\mathrm{\Delta }^{}`$ and the ratio $`\lambda _\mathrm{\Delta }/\lambda _Z`$ for a representative value of $`\kappa ^2`$ in the case of a nearly antiferromagnetic metal and nearly ferromagnetic metal, respectively.

The trends in both cases are the same. $`\lambda _Z^{}`$ and $`\lambda _\mathrm{\Delta }^{}`$ are seen to increase gradually and monotonically in going from 3D to quasi-2D. However, $`\lambda _\mathrm{\Delta }^{}`$ grows faster than $`\lambda _Z^{}`$ so the ratio $`\lambda _\mathrm{\Delta }/\lambda _Z`$ also increases in going from 3D to quasi-2D. This qualitative trend in the ratio is consistent with the behavior of $`T_c`$ obtained from the numerical solution of the Eliashberg equations. In the ferromagnetic case, however, it fails to reproduce the fact that the minimum $`T_c`$ is not necessary for a fully 3D system and that the maximum $`T_c`$ is obtained for strongly anisotropic yet not quasi-2D systems.

## IV Discussion

The results of the calculations for both the nearly ferromagnetic and nearly antiferromagnetic metals show that the robustness of magnetic pairing increases gradually as one goes from a cubic to a more and more anisotropic structure with parameters other than $`\alpha _m`$ and $`\alpha _t`$ left unchanged. These results are consistent with our previous findings  and with the calculations for $`\alpha _m=\alpha _t=0`$ and $`\alpha _m=\alpha _t=1`$ presented in ref. . In an earlier study, Nakamura et al.  found that $`T_c`$ could increase by up to a factor of three in going from 3D to 2D for their choice of model parameters. The effect of anisotropy on $`T_c`$ for nearly ferromagnetic and nearly antiferromagnetic metals is qualitatively similar. This phenomenon arises from the increase with growing anisotropy of the density of states of both the quasiparticles and of the magnetic fluctuations that mediate the quasiparticle interaction. This effect could be further enhanced in the case of a nearly antiferromagnetic metal by the change in the pattern of the oscillations of the magnetic interaction.

It can be seen from figure 5 that the strength of the interaction in the repulsive sites outside of the nodal plane of the $`d_{x^2y^2}`$ state gets reduced while crucially the attraction in the basal plane gets enhanced as one goes from the cubic to a more and more anisotropic tetragonal lattice. This enhancement is the consequence of the increase of the phase space of soft magnetic fluctuations as one goes from a cubic to a quasi-two dimensional structure. Since our model potential varies smoothly with the tetragonal distortion, parameterised by $`\alpha _m`$ in figures 1 and 2, it is clear that these effects occur gradually with increasing separation between the basal planes.

The calculations assume that the maximum magnetic response for a nearly antiferromagnetic metal occurs at the commensurate wavevector defined by $`Q_x=Q_y=\pi /a`$ and $`Q_z=\pi /c`$, where $`a`$ and $`c`$ are the lattice constants in the basal plane and along the tetragonal axis respectively, reintroduced here for clarity. The oscillations in the magnetic interaction potential along the tetragonal axis obviously depend on the value of $`Q_z`$. However, the enhancement of the attraction in the basal plane and the reduction of the interaction elsewhere as one goes from a cubic to a more and more anisotropic lattice do not depend on the particular value of $`Q_z`$. Therefore, we expect the qualitative conclusions of this paper to be independent of $`Q_z`$.

The robustness of the pairing is further enhanced by the gradual change in the electronic band from a 3D to a quasi-2D form (see Eq. (2)). The reduced hopping along the distortion axis, parameterised by $`\alpha _t`$ in figures 1 and 2, implies a reduced electronic bandwidth and hence increased density of electronic states. Our calculations show that this too leads to a gradual increase in $`T_c`$ with increasing distortion of the lattice.

In a nearly ferromagnetic metal, one again benefits from the reduction of the electronic band width and the increase of the interaction in the basal plane as one goes from a cubic to a tetragonal lattice (see figure 6). However, the suppression of the interaction between the basal planes has a less dramatic effect on the border of ferromagnetism than antiferromagnetism because in the latter case one suppresses key repulsive regions of the interaction (figure 5).

These simple arguments explain how the pairing effects of the interaction are strengthened by a tetragonal distortion in our model. However, the same effects also contribute to an enhanced self-interaction which acts to suppress $`T_c`$. The relative importance of the pair forming and pair breaking effects of the magnetic interaction cannot be inferred by the above physical picture alone. The numerical calculations show that for most cases considered here the pair forming effects dominate. The balance is particularly delicate on the border of ferromagnetism where the suppression of $`T_c`$ brought about by the self-interaction is pronounced. A physical interpretation of this suppression of $`T_c`$ is given in ref. . The same interpretation may explain, for example, why the maximum of $`T_c/T_{sf}`$ in the nearly ferromagnetic case is for a strongly anisotropic yet not quasi-2D pairing potential (figure 2).

A most striking manifestation of the interplay between the pair-forming and pair-breaking tendency of the magnetic interaction is the breakdown of the McMillan-style expression for $`T_c`$ in terms of the parameters $`\lambda _\mathrm{\Delta }`$ and $`\lambda _Z`$ (see Eqs. (9,10). This was noted in ref.  and has been interpreted in ref.  in terms of the important role played by the incoherent part of the Green function which is ignored in the simplest treatments, but is included in the present and earlier work where the full momentum and frequency dependence of the self energy is taken into account.

## V Outlook

The calculations show that the lattice anisotropy may increase the robustness of magnetic pairing in the mean-field approximation. Superconducting phase fluctuations which are not included in this approximation may be expected to suppress $`T_c`$ in the 2D limit. Therefore, in practice, one would think that the most favorable case for magnetic pairing is that of strong but not extreme anisotropy.

As noted in the introduction and in the previous two sections, the robustness of magnetic pairing can be very sensitive to certain details of the magnetic interaction and electronic structure. Therefore, one should exercise caution in making quantitative comparisons between the results of our calculations and experiment. For instance, one would expect all of the parameters of the model (not solely $`\alpha _m`$ and $`\alpha _t`$) to change simultaneously with increasing lattice anisotropy. The changes brought about in going from a cubic to a tetragonal lattice may even be much more complex than considered here. In particular, the number of partially filled bands may itself change. As also mentioned in the introduction, this could have in some cases even more dramatic consequences on superconductivity than the effects taken into account in our simple one-band model.

The theoretical framework developed for systems on the border of magnetism can be translated to describe systems on the border of other types of instabilities, such as charge density wave or ferroelectric instabilities. The above given phase space argument to explain the increased robustness of magnetic pairing with increasing lattice anisotropy should carry over in part to these other pairing mechanisms, at least at the one-loop mean-field level (see, e.g., ref. ).

While some understanding of the properties of the magnetic interaction model has been gained over the last few years (e.g., the conditions for robust pairing of electrons), there are many cases where the predictions of the model have not been worked out. Of particular importance is the role of the multiplicity of partially filled bands which may be expected to be the key to understanding exotic superconductivity observed in nearly magnetic materials such as $`UPt_3`$ and $`Sr_2RuO_4`$.

## VI Acknowledgments

We would like to thank A.V. Chubukov, P. Coleman, S.R. Julian, P.B. Littlewood, A.J. Millis, A.P. Mackenzie, D. Pines, D.J. Scalapino and M. Sigrist for discussions on this and related topics. We acknowledge the support of the EPSRC, the Newton Trust and the Royal Society.

## VII Appendix

We consider quasiparticles on a cubic or tetragonal lattice. We assume that the dominant scattering mechanism is of magnetic origin and postulate the following low-energy effective action for the quasiparticles:

$`S_{eff}`$ $`=`$ $`{\displaystyle \underset{𝐩,\alpha }{}}{\displaystyle _0^\beta }𝑑\tau \psi _{𝐩,\alpha }^{}(\tau )\left(_\tau +ϵ_𝐩\mu \right)\psi _{𝐩,\alpha }(\tau )`$ (22)
$`{\displaystyle \frac{g^2}{6N}}{\displaystyle \underset{𝐪}{}}{\displaystyle _0^\beta }𝑑\tau {\displaystyle _0^\beta }𝑑\tau ^{}\chi (𝐪,\tau \tau ^{})𝐬(𝐪,\tau )𝐬(𝐪,\tau ^{})`$
where $`N`$ is the number of allowed wavevectors in the Brillouin Zone and the spin density $`𝐬(𝐪,\tau )`$ is given by

$$𝐬(𝐪,\tau )\underset{𝐩,\alpha ,\gamma }{}\psi _{𝐩+𝐪,\alpha }^{}(\tau )\sigma _{\alpha ,\gamma }\psi _{𝐩,\gamma }(\tau )$$
(23)
where $`\sigma `$ denotes the three Pauli matrices. The quasiparticle dispersion relation $`ϵ_𝐩`$ is defined in Eq. (2), $`\mu `$ denotes the chemical potential, $`\beta `$ the inverse temperature, $`g^2`$ the coupling constant and $`\psi _{𝐩,\sigma }^{}`$ and $`\psi _{𝐩,\sigma }`$ are Grassmann variables. In the following we shall measure temperatures, frequencies and energies in the same units.

The retarded generalized magnetic susceptibility $`\chi (𝐪,\omega )`$ that defines the effective interaction, Eq. (22), is defined in Eq. (3).

The spin-fluctuation propagator on the imaginary axis, $`\chi (𝐪,i\nu _n)`$ is related to the imaginary part of the response function $`Im\chi (𝐪,\omega )`$, Eq. (3), via the spectral representation

$$\chi (𝐪,i\nu _n)=_{\mathrm{}}^+\mathrm{}\frac{d\omega }{\pi }\frac{Im\chi (𝐪,\omega )}{i\nu _n\omega }$$
(24)
To get $`\chi (𝐪,i\nu _n)`$ to decay as $`1/\nu _n^2`$ as $`\nu _n\mathrm{}`$, as it should, we introduce a cutoff $`\omega _0`$ and take $`Im\chi (𝐪,\omega )=0`$ for $`\omega \omega _0`$. A natural choice for the cutoff is $`\omega _0=\eta (\widehat{q})\kappa _0^2`$. We have checked that our results for the critical temperature are not sensitive to the particular choice of $`\omega _0`$ used.

The Eliashberg equations for the critical temperature $`T_c`$ in the Matsubara representation reduce, for the effective action Eq. (22), to

$$\mathrm{\Sigma }(𝐩,i\omega _n)=g^2\frac{T}{N}\underset{\mathrm{\Omega }_n}{}\underset{𝐤}{}\chi (𝐩𝐤,i\omega _ni\mathrm{\Omega }_n)G(𝐤,i\mathrm{\Omega }_n)$$
(25)
$$G(𝐩,i\omega _n)=\frac{1}{i\omega _n(ϵ_𝐩\mu )\mathrm{\Sigma }(𝐩,i\omega _n)}$$
(26)
$`\mathrm{\Lambda }(T)\mathrm{\Phi }(𝐩,i\omega _n)`$ $`=`$ $`\left[{\displaystyle \genfrac{}{}{0pt}{}{\frac{g^2}{3}}{g^2}}\right]{\displaystyle \frac{T}{N}}{\displaystyle \underset{\mathrm{\Omega }_n}{}}{\displaystyle \underset{𝐤}{}}\chi (𝐩𝐤,i\omega _ni\mathrm{\Omega }_n)|G(𝐤,i\mathrm{\Omega }_n)|^2\mathrm{\Phi }(𝐤,i\mathrm{\Omega }_n)`$ (27)
$`\mathrm{\Lambda }(T)`$ $`=`$ $`1T=T_c`$ (28)
where $`\mathrm{\Sigma }(𝐩,i\omega _n)`$ is the quasiparticle self-energy, $`G(𝐩,i\omega _n)`$ the one-particle Green’s function and $`\mathrm{\Phi }(𝐩,i\omega _n)`$ the anomalous self-energy. The chemical potential is adjusted to give an electron density of $`n=1.1`$, and $`N`$ is the total number of allowed wavevectors in the Brillouin Zone. In Eq. (28), the prefactor $`g^2/3`$ is for triplet pairing while the prefactor $`g^2`$ is appropriate for singlet pairing. Only the longitudinal spin-fluctuation mode contributes to the pairing amplitude in the triplet channel. Both transverse and longitudinal spin-fluctuation modes contribute to the pairing amplitude in the singlet channel. All three modes contribute to the quasiparticle self-energy.

The momentum convolutions in Eqs. (25,28) are carried out with a Fast Fourier Transform algorithm on a $`48\times 48\times 48`$ lattice. The frequency sums in both the self-energy and linearized gap equations are treated with the renormalization group technique of Pao and Bickers. We have kept between 8 and 16 Matsubara frequencies at each stage of the renormalization procedure, starting with an initial temperature $`T_0=0.6t`$ and cutoff $`\mathrm{\Omega }_c30t`$.The renormalization group acceleration technique restricts one to a discrete set of temperatures $`T_0>T_1>T_2\mathrm{}`$. The critical temperature at which $`\mathrm{\Lambda }(T)=1`$ in Eq. (28) is determined by linear interpolation.