# Probing Pairing Symmetry in Sr2RuO4

## Abstract

We study the spin dynamics in a p-wave superconductor at the nesting vector associated with $`\alpha `$ and $`\beta `$ bands in Sr<sub>2</sub>RuO<sub>4</sub>. We find a collective mode at the nesting vector in the superconducting phase identified as the odd-parity pairing state which breaks time reversal symmetry. This mode in the spin channel only exists in the p-wave superconductor, not in s- or d-wave superconductors. We propose that probing this mode would clarify the pairing symmetry in Sr<sub>2</sub>RuO<sub>4</sub>. The possibility of second superconducting phase transition is also discussed.

The nature of superconductivity discovered in Sr<sub>2</sub>RuO<sub>4</sub> has been the subject of intense theoretical and experimental activity. Although Sr<sub>2</sub>RuO<sub>4</sub> has the same layered perovskite structure as La<sub>2</sub>CuO<sub>4</sub>, the prototype of the cuprates, the behavior is remarkably different. At present, not much is known about any possible relation to the cuprates.

While it is clear that electron correlation effects are important in Sr<sub>2</sub>RuO<sub>4</sub>, the normal state is characterized as essentially a Fermi liquid below 50 K. The resistivities in all directions show $`T^2`$ behavior for $`T50K`$. The effective mass is about $`34m_{electron}`$ and the susceptibility is also about $`34\chi _0`$ where $`\chi _0`$ is the pauli spin susceptibility. In contrast to the conventional normal state (below 50 K), there are considerable evidences that the superconducting state (below about 1 K) is unconventional. The nuclear quadrupole resonance(NQR) does not show the Hebel-Slicheter peak . The transition temperature is very sensitive to non-magnetic impurities. The <sup>17</sup>O NMR knight shift experiment shows that the spin susceptibility has no change across $`T_c`$ but stays just the same as in the normal state for the magnetic field parallel to the RuO<sub>2</sub> plane.

Shortly after the discovery of the superconductivity in Sr<sub>2</sub>RuO<sub>4</sub>, it was proposed that the odd-pairity(spin triplet) Cooper pairs are formed in the superconducting state in analogy with <sup>3</sup>He. Further evidence favoring spin triplet pairing is the observation of the ferromagnetic metallic state in SrRuO<sub>3</sub> which is the three dimensional analogue of the layered Sr<sub>2</sub>RuO<sub>4</sub>. Since a weak coupling analysis of the spin triplet state implies nodeless gap, it is puzzling that the specific heat and NQR measurements show a large residual density of states (DOS), $`5060\%`$ of DOS of the normal state, in the superconducting phase. As a consequence, nonunitary superconducting state like <sup>3</sup>He A<sub>1</sub> phase, has been proposed. However, recent specific heat measurement shows that the residual DOS is about $`25\%`$ of the normal DOS, which indicates that the nonunitary state may not be stabilized.

An alternative explanation, so called, orbital dependent superconductivity was proposed. Since four $`4d`$ electrons in Ru<sup>4+</sup> partially fill the $`t_{2g}`$ band, the relevant orbitals are $`d_{xy}`$, $`d_{xz}`$, and $`d_{yz}`$ which determine the electronic properties. Using the quasi-two dimensional nature of the electronic dispersion, they show that there are two superconducting order parameters for two different classes of the orbitals. The gap of one class of bands is substantially smaller than that of other class of bands. The presence of gapless excitations for temperatures greater than the smaller gap would account for a residual DOS. The recent analysis of London penetration depth and coherence length led to the evidence for orbital dependent superconductivity identifying $`d_{xy}`$ as the orbital relevant for superconductivity. The possibility of the second superconducting phase transition was also discussed when the pairing symmetries are different for different classes of the bands.

Sigrist et al proposed the following order parameter which is claimed to be compatible with all the present experimental data.

$$𝐝=\widehat{d}(k_1\pm ik_2),$$
(1)   
where $`\widehat{d}`$ is parallel to the $`\widehat{c}`$ axis and the gap is described as the tensor represented by $`𝐝`$ in the following way.

$$\widehat{\mathrm{\Delta }}(𝐤)=𝝈𝐝i\sigma _2,$$
(2)   
where $`𝝈`$ is the Pauli matrix. Here $`\widehat{d}`$ is the spin vector whose direction is perpendicular to the direction of the spin associated with the condensed pair. Notice that the direction of the order parameter vector is frozen along the $`\widehat{c}`$ direction due to the crystal field and there is a full gap on the whole Fermi surface.

The details of the Fermi surface have been observed by quantum oscillations . The Fermi surface consists of three nearly-cylindrical sheets, which is consistent to the electronic band calculations.  Three Fermi sheets are labeled by $`\alpha `$, $`\beta `$, and $`\gamma `$. While the $`\gamma `$ sheet of the Fermi surface can be attributed solely to the $`d_{xy}`$ Wannier function, the $`\alpha `$ and $`\beta `$ sheets are due to the hybridization of the $`d_{xz}`$ and $`d_{yz}`$ Wannier functions. Combining the orbital dependent superconductivity and experimental observation, the gap associated with $`\gamma `$ band is larger than that of $`\alpha `$ and $`\beta `$ bands. Therefore the $`\gamma `$ band, which is essentially quasi-isotropic two dimensional, is responsible for the existing superconductivity. On the other hand, $`\alpha `$ and $`\beta `$ sheets are quasi-one dimensional which can be visualized as a set of parallel planes separated by $`Q=2\pi /3`$ running both in $`k_x`$ and $`k_y`$ directions. Therefore, it is natural to expect a sizable nesting effects at the wave vector $`𝐐=(2\pi /3,2\pi /3)`$ originated from $`\alpha `$ and $`\beta `$ bands. In the normal state, one can see that there should be a collective mode in the spin channel due to the nesting, and has been shown by the numerical calculation on the static susceptibility. The neutron scattering experiment also shows a peak at the wave vector, $`(0.6\pi ,0.6\pi ,0)`$ close to the nesting vector, with energy transfer $`6.2meV`$. Mazin and Singh discussed the possibility of a competition between p-wave and d-wave superconductivity in Sr<sub>2</sub>RuO<sub>4</sub>. The experimental result also casts some doubt on the predominant role of ferromagnetic spin fluctuations in the mechanism of spin triplet superconductivity. Although it is generally accepted that the pairing symmetry in Sr<sub>2</sub>RuO<sub>4</sub> has the odd pairity, a direct theoretical prediction is still necessary to determine the pairing symmetry among the possible order parameters which have the odd pairity.

In this paper, we propose a way to probe the pairing symmetry in Sr<sub>2</sub>RuO<sub>4</sub>. We calculate the spin-spin correlation function at the nesting vector, $`𝐐=(2\pi /3,2\pi /3)`$, using the Green function method. It is important to include the coupling between the spin density and the vectorial order parameter fluctuation which is the unique property of p-wave superconductor. We find a collective mode in the spin channel in the superconducting state only in p-wave superconductor with the pairing symmetry which breaks time reversal symmetry. Since the position of the resonant peak is just below $`2\mathrm{\Delta }`$, this will also determine the size of the smaller gap related to $`\alpha `$ and $`\beta `$ bands which have the nesting. On the other hand, no observation of the mode will indicate that the pairing symmetry associated with $`\alpha `$ and $`\beta `$ bands is different from that with $`\gamma `$ band, assuming that the pairing symmetry in $`\gamma `$ band, which does not have any nesting effect on the Fermi surface, is the proposed one as Eq. (1). Therefore there must be a second superconducting phase transition at a rather low temperature.

Using the Nambu’s representation, the Green function can be written as 

$$G^1(\omega _n,𝐤)=i\omega _n\xi _𝐤\rho _3\sigma _3\mathrm{\Delta }\rho _1𝝈\widehat{d}i\sigma _2,$$
(3)   
where $`𝝆`$ and $`𝝈`$ are Pauli matrices which operate in the particle-hole and spin spaces, respectively. Here $`\xi _𝐤=k^2/(2m)\mu `$, where $`\mu `$ is the chemical potential. In the superconducting state, the bare susceptibility which represents the spin flip procedure can be written by using the Green functions. 

$$\chi ^{00}(\omega _\nu ,𝐪)=T\underset{n}{}\underset{𝐤}{}Tr[G(\omega _n,𝐤)\alpha _+G(\omega _n+\omega _\nu ,𝐤+𝐪)\alpha _{}],$$
(4)   
where $`\omega _n`$ is the Matubara frequency and the spin vertex $`𝜶`$ is given by

$$𝜶=\frac{1+\rho _3}{2}𝝈+\frac{1\rho _3}{2}\sigma _2𝝈\sigma _2,$$
(5)   
and $`\alpha _\pm =\alpha _1\pm i\alpha _2`$.

Since the gap order parameter fluctuation couples to the spin density, the susceptibility renormalized by order parameter fluctuations consists of two parts.

$$\chi ^0(\omega ,𝐪)=\chi ^{00}(\omega ,𝐪)\frac{V(\omega ,𝐪)g\overline{V}(\omega ,𝐪)}{1g\mathrm{\Pi }(\omega ,𝐪)},$$
(6)   
where the $`g`$ is the interaction strength and responsible for the superconductivity. Here $`V(\omega ,𝐪)`$ and $`\mathrm{\Pi }(\omega ,𝐪)`$ can be computed as follows.

$`V(\omega _\nu ,𝐪)`$ $`=`$ $`T{\displaystyle \underset{n}{}}{\displaystyle \underset{𝐤}{}}Tr[G(\omega _n,𝐤)\alpha _+G(\omega _n+\omega _\nu ,𝐤+𝐪)(\alpha _{}\rho _1\sigma _1)],`$ (7)   
$`\mathrm{\Pi }(\omega _\nu ,𝐪)`$ $`=`$ $`T{\displaystyle \underset{n}{}}{\displaystyle \underset{𝐤}{}}Tr[G(\omega _n,𝐤)(\alpha _+\rho _1\sigma _1)G(\omega _n+\omega _\nu ,𝐤+𝐪)(\alpha _{}\rho _1\sigma _1)].`$ (8)   
Using $`\xi _𝐤=\xi _{𝐤+𝐐}`$ for the nesting vector $`𝐐`$, we found the following results at $`T=0`$.

$`\mathrm{Re}\chi ^{00}(\omega ,𝐐)`$ $`=`$ $`\{\begin{array}{cc}g^1N_0\frac{|\omega |\mathrm{arcsin}|\omega |/2\mathrm{\Delta }}{2\sqrt{|\omega ^24\mathrm{\Delta }^2|}}\hfill & |\omega |<2\mathrm{\Delta }\hfill \\ g^1N_0\frac{|\omega |\mathrm{ln}\left(\frac{4\mathrm{\Delta }^2}{\omega ^24\mathrm{\Delta }^2}\right)}{2\sqrt{\omega ^24\mathrm{\Delta }^2}}\hfill & |\omega |>2\mathrm{\Delta }\text{,}\hfill \end{array}`$ (9)   
$`\mathrm{Im}\chi ^0(\omega ,𝐐)`$ $`=`$ $`\{\begin{array}{cc}0\hfill & |\omega |<2\mathrm{\Delta }\hfill \\ N_0\frac{\pi \omega }{2\sqrt{\omega ^24\mathrm{\Delta }^2}}\hfill & |\omega |>2\mathrm{\Delta }\text{,}\hfill \end{array}`$ (10)   
$`\mathrm{Re}V(\omega ,𝐐)`$ $`=`$ $`\{\begin{array}{cc}N_0\frac{\mathrm{\Delta }sgn(\omega )\mathrm{arcsin}|\omega |/2\mathrm{\Delta }}{\sqrt{|\omega ^24\mathrm{\Delta }^2|}}\hfill & |\omega |<2\mathrm{\Delta }\hfill \\ N_0\frac{\mathrm{\Delta }sgn(\omega )\mathrm{ln}\left(\frac{4\mathrm{\Delta }^2}{\omega ^24\mathrm{\Delta }^2}\right)}{\sqrt{\omega ^24\mathrm{\Delta }^2}}\hfill & |\omega |>2\mathrm{\Delta }\text{,}\hfill \end{array}`$ (11)   
$`\mathrm{Im}V(\omega ,𝐐)`$ $`=`$ $`\{\begin{array}{cc}0\hfill & |\omega |<2\mathrm{\Delta }\hfill \\ N_0\frac{\pi \mathrm{\Delta }}{\sqrt{\omega ^24\mathrm{\Delta }^2}}\hfill & |\omega |>2\mathrm{\Delta }\text{,}\hfill \end{array}`$ (12)   
$`\mathrm{Re}\mathrm{\Pi }(\omega ,𝐐)`$ $`=`$ $`\{\begin{array}{cc}N_0\frac{2\mathrm{\Delta }^2\mathrm{arcsin}|\omega |/2\mathrm{\Delta }}{|\omega |\sqrt{|\omega ^24\mathrm{\Delta }^2|}}\hfill & |\omega |<2\mathrm{\Delta }\hfill \\ N_0\frac{2\mathrm{\Delta }^2\mathrm{ln}\left(\frac{4\mathrm{\Delta }^2}{\omega ^24\mathrm{\Delta }^2}\right)}{|\omega |\sqrt{\omega ^24\mathrm{\Delta }^2}}\hfill & |\omega |>2\mathrm{\Delta }\text{,}\hfill \end{array}`$ (13)   
$`\mathrm{Im}\mathrm{\Pi }(\omega ,𝐐)`$ $`=`$ $`\{\begin{array}{cc}0\hfill & |\omega |<2\mathrm{\Delta }\hfill \\ N_0\frac{2\pi \mathrm{\Delta }^2}{\omega \sqrt{\omega ^24\mathrm{\Delta }^2}}\hfill & |\omega |>2\mathrm{\Delta }\text{,}\hfill \end{array}`$ (14)   
where $`N_0`$ is the DOS at the Fermi level. Using the above result, the renormalized susceptibility is obtained as follows for $`|\omega |<2\mathrm{\Delta }`$,

$`\mathrm{Re}\chi ^0(\omega ,𝐐)`$ $`=`$ $`g^1{\displaystyle \frac{N_0}{2}}{\displaystyle \frac{|\omega |\mathrm{arcsin}\frac{|\omega |}{2\mathrm{\Delta }}}{\sqrt{4\mathrm{\Delta }^2\omega ^2}}}+{\displaystyle \frac{N_0^2\mathrm{\Delta }^2|\omega |(\mathrm{arcsin}\frac{|\omega |}{2\mathrm{\Delta }})^2}{g^1|\omega |(4\mathrm{\Delta }^2\omega ^2)2N_0\mathrm{\Delta }^2\mathrm{arcsin}\frac{|\omega |}{2\mathrm{\Delta }}\sqrt{4\mathrm{\Delta }^2\omega ^2}}},`$ (15)   
$`\mathrm{Im}\chi ^0(\omega ,𝐐)`$ $`=`$ $`0.`$ (16)   
Including the effects of the exchange interaction within the random phase approximation(RPA), the full dynamical spin susceptibility is expressed as

$$\chi (\omega ,𝐪)=\frac{\chi ^0(\omega ,𝐪)}{1I_𝐪\chi ^0(\omega ,𝐪)},$$
(17)   
where the exchange interaction $`I_𝐐I`$ for $`𝐐`$. Since $`\mathrm{Im}\chi ^0=0`$ and $`\mathrm{Re}\chi ^0`$ diverges as $`\omega `$ approaches to $`2\mathrm{\Delta }`$, there exists a collective mode when $`I<g`$. The position of the mode is at

$$\omega =2\mathrm{\Delta }\frac{\pi ^2}{4}\frac{g^2I^2}{(gI)^2}\mathrm{\Delta }N_0^2.$$
(18)   
Here we have assumed that the $`\mathrm{arcsin}|\omega |/2\mathrm{\Delta }\pi /2`$ consistent with the result, and $`g,I<1/N_0`$. Notice that the position of the mode is very close to $`2\mathrm{\Delta }`$. The intensity of the peak is

$$\frac{\pi ^2}{2}\frac{g^3I}{(gI)^3}\mathrm{\Delta }N_0^2.$$
(19)   
If the coupling between the spin density and the order parameter fluctuation, $`g`$, is rather large, then there are two solutions which satisfy the condition, Re $`\chi _0(\omega )=1/I`$, for $`g<I`$. However, the separation between two modes is $`\frac{\pi ^2g^3}{4(gI)^2}\sqrt{g8Ig+8I^2}\mathrm{\Delta }N_0^2`$ which is very tiny so that we expect to observe only one mode at

$$\omega =2\mathrm{\Delta }\frac{\pi ^2g^2(g2I)^2}{8(gI)^2}\mathrm{\Delta }N_0^2.$$
(20)   
Now, let us investigate the case of the spin singlet superconductors, such as s- or d-wave superconductor. In the case of the spin singlet superconductor, the bare spin-spin correlation function can be obtained through the following expression.

$$\chi ^{00}(\omega ,𝐐)=\underset{𝐤}{}\left(1\frac{\xi _𝐤\xi _{𝐤+𝐐}+\mathrm{\Delta }_𝐤\mathrm{\Delta }_{𝐤+𝐐}}{E_𝐤E_{𝐤+𝐐}}\right)\left(\frac{1}{\omega E_𝐤E_{𝐤+𝐐}}\frac{1}{\omega +E_𝐤+E_{𝐤+𝐐}}\right).$$
(21)   
For s-wave superconductor, i.e., $`\mathrm{\Delta }_𝐤=\mathrm{\Delta }_{𝐤+𝐐}=\mathrm{\Delta }`$, one can obtain the following results for $`|\omega |<2\mathrm{\Delta }`$.

$`\mathrm{Re}\chi ^0(\omega ,𝐐)`$ $`=`$ $`N_0\mathrm{ln}({\displaystyle \frac{\sqrt{|\omega ^24\mathrm{\Delta }^2|}}{\mathrm{\Delta }}}+{\displaystyle \frac{\sqrt{|\omega ^23\mathrm{\Delta }^2|}}{\mathrm{\Delta }}})+\mathrm{ln}(C),`$ (22)   
$`\mathrm{Im}\chi ^0(\omega ,𝐐)`$ $`=`$ $`0,`$ (23)   
where $`C`$ is a constant. This implies that one needs enomously large interaction $`I`$ to get the collective mode, i.e., $`I1/N_0`$, which is practically impossible.

Let us study the possibility of having the resonance peak in the d-wave superconductor at the nesting vector $`𝐐=(2\pi /3,2\pi /3)`$. Assuming that the superconducting phase is described by the conventional BCS superconductor with d-wave pairing symmetry, $`\mathrm{\Delta }(𝐤)=\frac{\mathrm{\Delta }}{2}[cos(k_x)cos(k_y)]`$, we use the same expression as Eq. (21) for the bare spin-spin correlation function. Due to the coherence factor, there is a collective mode at $`𝐐=(\pi ,\pi )`$ even without the nesting in the electronic dispersion. However, in the case of $`𝐐=(2\pi /3,2\pi /3)`$, we do not have simple relation as that for $`𝐐=(\pi ,\pi )`$. In fact, $`\mathrm{\Delta }_𝐤`$ is equal to $`\mathrm{\Delta }_{𝐤+𝐐}`$ for the line from $`𝐤=(2\pi /3,0)`$ to $`(0,2\pi /3)`$, which makes the coherence factor $`O(1)`$, but $`\mathrm{\Delta }_𝐤`$ and $`\mathrm{\Delta }_{𝐤+𝐐}`$ have the linear dispersion in $`(k_x,k_y)`$ so it does not produce any singularity in the spin susceptibility. If the momentum lies near the node, then we have the same dispersion relation for the $`𝐐=(\pi ,\pi )`$ and it was found that there is no singularity in spin channel if $`𝐤`$ and $`𝐤+𝐐`$ are near the nodes. Therefore we do not expect any collective mode in either s- or d-wave superconductor at the wave vector $`𝐐=(2\pi /3,2\pi /3)`$.

The possible Cooper pairing states were classified according to the irreducible representation of the tetragonal point group D<sub>4h</sub> which include four one-dimensional and one two-dimensional representations for both even and odd parity. Assuming that the order parameter associated with $`\alpha `$($`\beta `$) band has the odd parity with a different pairing symmetry from Eq. (1), we also study the existence of the resonance peak with the following order parameters classified as the odd-parity pairing.

$$𝐝=\{\begin{array}{cc}\widehat{x}k_1+\widehat{y}k_2\hfill & \\ \widehat{x}k_1\widehat{y}k_2\hfill & \\ \widehat{x}k_2+\widehat{y}k_1\hfill & \\ \widehat{x}k_2\widehat{y}k_1.\hfill & \end{array}$$
(24)   
Due to the coherence factor, we found that the spin-spin correlation function behaves as in Eq. 23. However, once the fluctuation effect gets strong, one might get a collective mode with the other order parameters as in Eq. 24. Since the coupling between the spin density and the fluctuation of the order parameter should not destabilize the ground state, one needs careful investigation of the values such as $`\mathrm{\Delta }N_0`$, $`gN_0`$ and $`I_𝐐N_0`$ which would determine the possibility of the resonance peak due to the fluctuation effect. . Therefore, we conclude that the collective mode at the nesting vector only exits with the proposed order parameter as in Eq. (1) unless there is unusually strong coupling between the spin density and the order parameter fluctuation. Notice that only the order parameter which breaks the time reversal symmetry shows the resonance peak at the nesting vector.

In conclusion, we studied the spin dynamics in p-wave superconductor at the nesting vector associated with $`\alpha `$ and $`\beta `$ bands in Sr<sub>2</sub>RuO<sub>4</sub>. We found that there is a collective mode at the frequency just below $`2\mathrm{\Delta }`$ where $`\mathrm{\Delta }`$ is a smaller gap according to the orbital dependent superconductivity. We show that this mode exists only in p-wave superconductor, not in s- or d-wave superconductor. We also presented that the other odd pairing states do not produce the collective mode unless there is unusually strong coupling between the spin density and the order parameter fluctuation. Therefore we suggest that probing this mode will determine the pairing symmetry in Sr<sub>2</sub>RuO<sub>4</sub> which breaks time reversal symmetry assuming that all bands favor the same pairing symmetry. This will clarify the controversial situation about the possibility of having s- or d-wave superconductor in Sr<sub>2</sub>RuO<sub>4</sub>. Moreover, no observation of this mode will indicate that the order parameter associated with $`\alpha (\beta )`$ band is different from the proposed order parameter as in Eq. (1). This implies that there must be a second superconducting phase transition at rather low temperature. The observation of the strong pinning of the vortex about $`50mK`$ might be an indication of second superconducting phase transition, although we believe that second superconducting phase is described as one of the possible p-wave pairing states.

###### Acknowledgements.

I thank S. Chakravarty, Yong Baek Kim, Kazumi Maki, and especially M. Sigrist for helpful discussions. This work was conducted under the auspices of the Department of Energy, supported (in part) by funds provided by the University of California for the conduct of discretionary research by Los Alamos National Laboratory.