text:
# Continuum QRPA in the coordinate space representation

## I Introduction

The random phase approximation (RPA) has provided a convenient and useful method to describe excited states of many-fermion systems. There are a number of ways to formulate the RPA . In practical point of view, we particularly mention here a configuration space formalism and a response function formalism. The configuration space formalism diagonalizes a non-hermitian matrix denoted often by $`A`$ and $`B`$ matrices which are constructed in the model space of 1 particle-1 hole (1p-1h) states. In contrast, the response function formalism is based on the linear response theory and solves a Bethe-Salpeter equation for the response function, often in the coordinate space . The response function formalism can be formulated in various representations of basis states, and the connection between these two methods can be made by expressing response functions in the configuration space .

The response function formalism of RPA becomes particularly simple when the interaction is a zero-range contact force. In that case, the excitations to particle continuum states can be treated exactly by solving the single-particle Green function in the coordinate space. This method was first developed by Shlomo and Bertsch  and subsequently applied to self-consistent calculations of nuclear giant resonances with Skyrme interaction by Liu and Van Giai . Recently it has been extensively used by Hamamoto, Sagawa, and Zhang to discuss giant resonances of neutron-rich nuclei, where the continuum effects play an essential role due to a much lower threshold energy compared with $`\beta `$-stable nuclei . An extension to the three dimensional space has also been carried out recently by Nakatsukasa and Yabana for the study of atomic clusters . The coupling between particle-particle continuum was also studied in 11Li by Bertsch and Esbensen.

Although it has been well known that the pairing correlation plays an important role in the ground state of open-shell nuclei, it has been neglected in applying the response function formalism to describe excited states of atomic nuclei until very recently . So far a simple filling approximation has been employed in open-shell nuclei in order to simulate the pairing correlations. However, it is important to take into account the pairing effects consistently for the study of excited states of open-shell nuclei, and thus the quasi-particle RPA (QRPA) should be used instead of the RPA .

The aim of this paper is to generalize the formalism of Shlomo and Bertsch to the QRPA and discuss the effects of pairing correlations on excited states of open-shell nuclei. In this paper, we study only cases where the BCS approximation works well and thus all states in the pairing active space are bound, leaving out as a future work a self-consistent treatment of the pairing effects in the continuum using the Hartree-Fock-Bogoliubov + RPA theory . Our method is closely related to that in Ref. , although details are somewhat different. The paper is organized as follows. In Sec. II, we briefly review the formalism of Shlomo and Bertsch and extend it to the QRPA. In Sec. III, we apply the formalism to the isoscalar (IS) monopole, quadrupole, and octupole modes as well as the isovector (IV) dipole mode of excitation of the 120Sn nucleus and discuss the effects of pairing correlations on the excited states. A summary is given in Sec. IV.

## II Linear Response Theory for Open-shell Nuclei

We begin with the configuration space formalism of the RPA theory and then make a connection to the response function method. The RPA equation can be given in a compact form

$$\left(\begin{array}{cc}A& B\\ B^{}& A^{}\end{array}\right)\left(\begin{array}{c}X\\ Y\end{array}\right)=\omega \left(\begin{array}{c}X\\ Y\end{array}\right),$$
(1)
where $`X`$ and $`Y`$ are the forward and the backward amplitudes, respectively. For a residual interaction of delta-type contact force, $`v_{res}(𝒓_\mathrm{𝟏},𝒓_\mathrm{𝟐})=v((r_1+r_2)/2)\delta (𝒓_\mathrm{𝟏}𝒓_\mathrm{𝟐})`$, the matrix elements of $`A`$ and $`B`$ for the $`L`$-multipole mode read

$$A_{ph,p^{}h^{}}(ϵ_pϵ_h)\delta _{ph,p^{}h^{}}=B_{ph,p^{}h^{}}=I(php^{}h^{})j_pl_pY_Lj_hl_hj_p^{}l_p^{}Y_Lj_h^{}l_h^{}\frac{1}{2L+1},$$
(2)
where $`p`$($`h`$) denotes a particle (hole) state and $`jlY_Lj^{}l^{}`$ is the reduced matrix element. The radial integral $`I`$ is given by

$$I(php^{}h^{})=_0^{\mathrm{}}\frac{dr}{r^2}v(r)\varphi _p(r)\varphi _h(r)\varphi _p^{}(r)\varphi _h^{}(r),$$
(3)
where $`\varphi (r)`$ is a single-particle radial wave function. We have absorbed the overall factor $`(1)^L`$ in front of the $`B`$ matrix by redefining the sign of the backward $`Y`$ amplitudes.

The integral (3) can be computed by discretizing it as

$$I(php^{}h^{})\underset{k}{}\frac{\mathrm{\Delta }r}{r_k^2}v(r_k)\varphi _p(r_k)\varphi _h(r_k)\varphi _p^{}(r_k)\varphi _h^{}(r_k),$$
(4)
where $`\mathrm{\Delta }r`$ is the spacing of the radial coordinate. Since the interaction is then given as a sum of separable form, the RPA frequencies $`\omega `$ can be obtained by solving the generalized RPA dispersion relation $`det(1\mathrm{\Pi }_0(\omega )\chi )=0`$ , where the matrices $`\mathrm{\Pi }_0(\omega )`$ and $`\chi `$ are given by

$`\mathrm{\Pi }_0(i,j;\omega )`$ $`=`$ $`{\displaystyle \underset{ph}{}}D_{ph}(i)D_{ph}(j)\left({\displaystyle \frac{1}{ϵ_pϵ_h\omega i\eta }}+{\displaystyle \frac{1}{ϵ_pϵ_h+\omega i\eta }}\right),`$ (5)
$`\chi (i,j)`$ $`=`$ $`\chi (i)\delta _{i,j}={\displaystyle \frac{\mathrm{\Delta }r}{r_i^2}}v(r_i),`$ (6)
respectively, in the coordinate space representation. Here, $`\eta `$ is a infinitesimal real number, and $`D_{ph}`$ is given by

$$D_{ph}(i)=\varphi _p(r_i)\varphi _h(r_i)j_pl_pY_Lj_hl_h\frac{1}{\sqrt{2L+1}}.$$
(7)
Note that $`\mathrm{\Pi }_0(\omega )`$ is nothing but the unperturbed response function in the linear response theory. Here we introduce the RPA response function which obeys a Bethe-Salpeter equation

$$\mathrm{\Pi }_{RPA}=\mathrm{\Pi }_0+\mathrm{\Pi }_0\chi \mathrm{\Pi }_{RPA}.$$
(8)
This equation can be solved in the coordinate space by matrix inversion as

$$\mathrm{\Pi }_{RPA}(i,j;\omega )=\underset{k}{}(1\mathrm{\Pi }_0(\omega )\chi )_{i,k}^1\mathrm{\Pi }_0(k,j;\omega ).$$
(9)
The response of the system to an external field $`V_{ext}(𝒓)=V_{ext}(r)Y_{LM}(\widehat{𝒓})`$ is then given by

$$S(\omega )\underset{f}{}|f|V_{ext}|0|^2\delta (E_fE_0\omega )=\frac{1}{\pi }Im𝑑r_i𝑑r_jV_{ext}(r_i)\mathrm{\Pi }_{RPA}(i,j;\omega )V_{ext}(r_j).$$
(10)
The exact treatment of the continuum effects can be achieved by eliminating the sum of the particle states in the free response function (5) using the complete set of the wave function . This leads to

$`\mathrm{\Pi }_0(i,j;\omega )`$ $`=`$ $`{\displaystyle \underset{h}{}}\varphi _h(r_i)\varphi _h(r_j){\displaystyle \underset{j_pl_p}{}}j_pl_pY_Lj_hl_h^2{\displaystyle \frac{1}{2L+1}}`$ (12)
$`\times r_i\left|{\displaystyle \frac{1}{\widehat{h}ϵ_h\omega i\eta }}+{\displaystyle \frac{1}{\widehat{h}ϵ_h+\omega i\eta }}\right|r_j,`$
where $`\widehat{h}`$ is the single-particle Hamiltonian, and the single-particle Green function is given by

$$r\left|\frac{1}{\widehat{h}ϵ_h\pm \omega i\eta }\right|r^{}=\frac{2m}{\mathrm{}^2}\frac{u(r_<)w(r_>)}{W}.$$
(13)
Here, $`u`$ and $`w`$ are the regular and irregular solutions of the Hamiltonian $`\widehat{h}`$ at energy $`ϵ_h\omega `$, and $`W`$ is the Wronskian given by $`W=uw^{}wu^{}`$.

In the application of the formalism to nuclear systems, we use the proton-neutron formalism which can properly take into account the couplings between the IS and IV modes of excitation . The Bethe-Salpeter equation given by Eq. (8) is then generalized to be

$$\left(\begin{array}{c}\mathrm{\Pi }_{RPA}^{(p)}\\ \mathrm{\Pi }_{RPA}^{(n)}\end{array}\right)=\left(\begin{array}{c}\mathrm{\Pi }_0^{(p)}\\ \mathrm{\Pi }_0^{(n)}\end{array}\right)+\left(\begin{array}{cc}\mathrm{\Pi }_0^{(p)}\chi _{pp}& \mathrm{\Pi }_0^{(p)}\chi _{pn}\\ \mathrm{\Pi }_0^{(n)}\chi _{pn}& \mathrm{\Pi }_0^{(n)}\chi _{nn}\end{array}\right)\left(\begin{array}{c}\mathrm{\Pi }_{RPA}^{(p)}\\ \mathrm{\Pi }_{RPA}^{(n)}\end{array}\right).$$
(14)
For simplicity of the notation, we do not present below the formalism in the two-component form, although we indeed use it in the actual calculations given in the next section.

In the presence of paring correlations, the elementary excitation is a two quasi-particle excitation, rather than a particle-hole excitation. A generalization of the RPA to the QRPA is given in Ref.  together with relevant $`A`$ and $`B`$ matrices in the QRPA equation. A free response function in the QRPA in the configuration space representation can be constructed in a similar way to the RPA,

$$\mathrm{\Pi }_0(i,j;\omega )=\underset{\alpha \beta }{}D_{\alpha \beta }(i)D_{\alpha \beta }(j)\left(\frac{1}{E_\alpha +E_\beta \omega i\eta }+\frac{1}{E_\alpha +E_\beta +\omega i\eta }\right),$$
(15)
with

$$D_{\alpha \beta }(i)=\varphi _\alpha (r_i)\varphi _\beta (r_i)j_\alpha l_\alpha Y_Lj_\beta l_\beta \frac{u_\alpha v_\beta +()^Lv_\alpha u_\beta }{\sqrt{2L+1}}(1+\delta _{\alpha ,\beta })^{1/2},$$
(16)
where $`v_\alpha ^2`$ is the BCS occupation probability and $`u_\alpha ^2=1v_\alpha ^2`$. $`E_\alpha `$ is the quasi-particle energy given by $`E_\alpha =\sqrt{(ϵ_\alpha \lambda )^2+\mathrm{\Delta }_\alpha ^2}`$, where $`\lambda `$ and $`\mathrm{\Delta }_\alpha `$ are the chemical potential and the pairing gap, respectively. In the BCS approximation, $`\varphi _\alpha `$ is an eigenfunction of the single-particle Hamiltonian $`\widehat{h}`$ with an eigen-energy $`ϵ_\alpha `$. Since the quasi-particle energy $`E_\alpha `$ is not an eigenvalue of $`\widehat{h}`$ in general, it is not straightforward to introduce the single-particle Green function (13) in the QRPA free response function. However, when the pairing gap is zero for states $`k`$ outside the pairing active space, the quasiparticle energy becomes an eigenvalue of the single-particle Hamiltonian, i.e. $`E_k=ϵ_k\lambda ,v_k=0`$, and $`u_k`$=1. We therefore consider separately excitations among states within the pairing active space and those from the inside to the outside of the active space. To the latter model space, we apply the same procedure as the RPA response function. The free response function in the BCS approximation (15) thus becomes

$`\mathrm{\Pi }_0(i,j;\omega )={\displaystyle \underset{\alpha \beta }{}}D_{\alpha \beta }(i)D_{\alpha \beta }(j)\left({\displaystyle \frac{1}{E_\alpha +E_\beta \omega i\eta }}+{\displaystyle \frac{1}{E_\alpha +E_\beta +\omega i\eta }}\right)`$ (17)
$`{\displaystyle \underset{\alpha }{}}\varphi _\alpha (r_i)\varphi _\alpha (r_j)v_\alpha ^2{\displaystyle \underset{j_kl_k}{}}j_\alpha l_\alpha Y_Lj_kl_k^2{\displaystyle \frac{1}{2L+1}}`$ (18)
$`\times \{r_i|{\displaystyle \frac{1}{E_\alpha +\widehat{h}\lambda \omega i\eta }}+{\displaystyle \frac{1}{E_\alpha +\widehat{h}\lambda +\omega i\eta }}|r_j`$ (19)
$`{\displaystyle \underset{\beta }{}}\delta _{j_k,j_\beta }\delta _{l_k,l_\beta }\varphi _\beta (r_i)\varphi _\beta (r_j)({\displaystyle \frac{1}{E_\alpha +ϵ_\beta \lambda \omega i\eta }}+{\displaystyle \frac{1}{E_\alpha +ϵ_\beta \lambda +\omega i\eta }})\},`$ (20)
where the summations of $`\alpha `$ and $`\beta `$ are restricted to the states within the pairing active space. The last term in Eq. (20) is a correction for a double-counting of excitations within the pairing active space, which stems from the substitution of the completeness relation $`_k|\varphi _k\varphi _k|=1_\beta |\varphi _\beta \varphi _\beta |`$ in Eq. (15). Note that, without the pairing correlations, $`E_\alpha =\lambda ϵ_\alpha `$ and $`v_\alpha =1`$ for $`ϵ_\alpha <\lambda `$, and the BCS free response function (20) is identical to the corresponding response function (12) in the RPA. With this unperturbed response function (20), the QRPA response function is obtained again by solving the Bethe-Salpeter equation (8) as in the RPA theory.

## III Continuum QRPA Excitations in 120Sn

We now apply the continuum QRPA formalism to 120Sn and make a comparison between the QRPA and the RPA. We choose this system because it is a typical open-shell nucleus and also because it is a sub-shell closure nucleus where the RPA can be applied unambiguously without using the filling approximation for valence nucleons. The single-particle wave functions $`\varphi `$ and the single-particle energies $`ϵ`$ are obtained by solving the Shrödinger equation with a Woods-Saxon mean-field potential. As a residual interaction $`v_{res}`$, we use the $`t_0`$ and $`t_3`$ parts of the Skyrme residual interaction, which is obtained from the second derivative of the Skyrme energy functional with respect to the proton and the neutron densities. The ground state density to be used in the density-dependent $`t_3`$ part of the residual interaction is generated from the single-particle wave functions $`\varphi `$. We use the same parameters as those in Ref.  for the mean-field potentials and the residual interaction, i.e., $`t_0=`$1100 MeV fm3, $`t_3=`$16000 MeV fm6, $`x_0`$=0.5, $`x_3`$=1, and $`\gamma `$=1 in the standard notation of the Skyrme functional . Since this model is not self-consistent, we renormalize $`v_{res}`$ for the QRPA and the RPA calculations, respectively, so that the spurious IS dipole mode appears at zero excitation energy. The resultant renormalization factors are $`\kappa `$ = 0.638 and 0.660 for RPA and QRPA, respectively. For the pairing of neutrons, we use a schematic state-independent constant pairing gap $`\mathrm{\Delta }_\alpha =\mathrm{\Delta }=1.392`$ MeV, which is estimated from the experimental binding energies of neighboring nuclei. The pairing active space which we adopt includes the levels up to the $`N=50`$ major shell as well as the 1g7/2, 2d5/2, 2d3/2, 3s1/2, and 1h11/2 levels. The single-particle energy for the valence levels are shown in Table 1, together with the BCS occupation probabilities. The proton pairing gap is set to be zero due to the magic number $`Z=50`$.

Figs. 1–4 show the strength function $`S(\omega )`$ for the isoscalar (IS) monopole, IS quadrupole, IS octupole, and the isovector (IV) dipole modes of excitations, respectively. The external field $`V_{ext}(r)`$ for each modes is given by $`r^2`$, $`r^2`$, $`r^3`$, and $`r\tau _z`$, respectively. The lower panels show results of the QRPA calculations, while the upper panels show results of the RPA calculations without the pairing correlations as a comparison. For the latter, the levels up to 3s1/2 state are occupied with the occupation probability $`v^2`$ of 1, while those above 1h11/2 state are unoccupied with $`v^2=0`$ (see Table 1). Arrows indicate the positions of (Q)RPA states below the threshold, where the strength function has no width.

For the monopole excitation shown in Fig.1, the RPA does not show any low-lying mode, although the experimental second lowest $`0^+`$ state in the 120Sn nucleus is observed at the excitation energy 1.874 MeV, which is attributed to a paring vibration mode. The second lowest $`0^+`$ state in the QRPA is found at rather low energy 2.9 MeV, and may couple to the pairing vibrational mode. The IS giant monopole states are seen in the energy region 17$``$28 MeV in both the QRPA and RPA calculations. The transition densities for the IS monopole mode at two different energies, i.e., $`\omega `$ = 2.9 MeV and 21.6 MeV, are shown in Fig. 5. We find that the former shows a characteristic behaviour of the pairing vibration mode while the latter shows the compressional character. For the quadrupole mode shown in Fig. 2, the lowest RPA state is at 5.2 MeV, in comparison with the experimental value of 1.17 MeV. The transition strength is B(E2:0$`{}_{}{}^{+}2^+`$)= 0.031 $`e^2b^2`$ in the RPA calculation, while the experimental value is 0.2 $`e^2b^2`$. If one takes the pairing correlations into account, the low-lying 2+ RPA states goes substantially down and the lowest QRPA state appears at 2.3 MeV having the transition strength B(E2:0$`{}_{}{}^{+}2^+`$)= 0.107 $`e^2b^2`$, which is much closer to the experimental value. In both cases, the main peak of the IS giant quadrupole resonance (GQR) appears at around 13 MeV exhausting most of the sum rule strength. The experimental GQR is also observed at the excitation energy around 13MeV. As for the octupole mode of excitations in Fig. 3, the experimental value of the lowest $`3^{}`$ state is at 2.4 MeV, while the RPA and the QRPA lead to 1.4 MeV and 3.0 MeV, respectively. The experimental value for the corresponding transition rate is B(E3:0$`{}_{}{}^{+}3^{}`$)= 0.09 $`e^2b^3`$, while it is 0.159 $`e^2b^3`$ and 0.0771 $`e^2b^3`$ in the RPA and the QRPA, respectively. The RPA without pairing correlations underestimates the lowest $`3^{}`$ state energy and the QRPA is more satisfactory compared with the experimental value. We summarize in Table 2 the results of the RPA and the QRPA calculations together with the experimental data for the lowest 2+ and 3- states. Giant octupole resonances (GOR) are observed in Fig. 3 at the excitation energy 23 MeV in both cases. Results for the IV giant dipole resonance (GDR) are shown for RPA and QRPA in Fig. 4. As is the same as in Figs. 1–3, the structure of GDR is not much disturbed by the effect of the pairing.

Notice that the effect of the pairing on the low-lying quadrupole mode is opposite to that on the octupole mode. For the former, the energy of the lowest 2+ state becomes smaller due to the pairing, with enhancement of the B(E2) value. On the other hand, the QRPA raises the energy of the lowest 3- state and the B(E3) value is hindered. In both cases, the QRPA gives better agreement with the experimental values compared with the RPA. These features can be understood as follows. For excitations with even parity, such as the quadrupole excitations, transitions between the same levels are allowed in the presence of the pairing correlations. This enhances the collectivity of low-lying states, resulting in a smaller excitation energy and a larger transition strength. On the contrary, such excitations are not allowed for odd parity excitations, e.g., the octupole mode. In that case, the dominant excitation is from one major shell to another regardless of the pairing correlation. Since the particle-hole excitations are weakened by the factor $`v^2`$ in the presence of the pairing, the QRPA lowers the collectivity of low-lying collective excitations with odd parity.

In contrast to the low-lying modes of excitations, in general, high-lying modes are much less sensitive to the paring correlations. This is the case for all the modes of excitations shown in Figs. 1–4. This fact can be seen more transparently if one smears the strength functions with a finite width. We show in Figs. 6–9 the RPA and QRPA results with a finite value of $`\eta `$ =0.5MeV in Eq. (20). As one clearly sees, the two results resemble each other in the giant resonance region at energies above the threshold near 10 MeV. These results are natural consequences of the pairing correlations since the configurations outside the pairing active space are the main p-h configurations for the giant resonances and thus the pairing effects should play a minor role.

A conventional approximation to treat the continuum effect is to put a nucleus in a box and discretize the continuum states by imposing a boundary condition at the edge of the box. A model space of these states is usually truncated at the maximum single-particle energy $`ϵ_{max}`$. Since our continuum QRPA method can treat the coupling to the continuum exactly, it is interesting to compare our method with the box discretization approximation. Fig. 10 shows a convergence property of the box discretization method for the IS quadrupole response. We take the box size of $`R_{max}`$=10 fm, and smear the strength function with $`\eta `$=0.5 MeV for the representation purpose. We have checked that the results do not change significantly even if we use a larger value of $`R_{max}`$. The solid line is the result of the continuum QRPA method with the exact treatment of the continuum effect, which is the same as in Fig. 6. The dot-dashed, dashed, and thin solid lines are results of the box discretization method with truncation energy at $`ϵ_{max}`$= 10, 50, and 100 MeV, respectively. In the upper panel, we use the same residual interaction for all the calculations. As one can see, the convergence with respect to the maximum energy of continuum states is extremely slow: even with $`ϵ_{max}`$= 100 MeV the peak positions are not reproduced. The peak height for the lowest energy peak is not reproduced, either. We note that the truncation of the model space shfts the position of the spurious IS dipole state. It appears at 6.0, 4.4, and 3.7 MeV for $`ϵ_{max}`$= 10, 50, and 100 MeV, respectively. In the lower panel, the renormalized residual interaction is used for each value of $`ϵ_{max}`$ so that the IS dipole mode appears at zero energy. The renormalization factors are $`\kappa `$= 0.968, 0.776, and 0.732 for $`ϵ_{max}`$= 10, 50, and 100 MeV, respectively. This procedure drastically improves the convergence. In the case of the truncation energy $`ϵ_{max}`$= 50 MeV (dashed line), the exact solution is almost reproduced. The result converges at this energy and the shape of the strength function is not altered even when the states up to $`ϵ_{max}`$= 100 MeV are included. This study clearly indicates the importance of the self-consistency between the space truncation and the renormalization of the residual interaction. If this self-consistency is imposed, the box discretization method works well. It should be emphasized, however, that the escape width of resonances can be obtained only when the single-particle continuum states are treated exactly as we do in this article.

## IV Summary and Discussions

We proposed a QRPA model in the coordinate space to take into account the continuum effects. It is a generalization of the formalism of Shlomo and Bertsch for the continuum RPA to the QRPA. We treated separately the p-h excitations within the pairing active space and those between the active space and the non-active space. For the former, we explicitly used the two quasiparticle configurations in the response function in the coordinate space, while for the latter we use the single-particle Green function in the coordinate space representation taking into account the coupling to the particle continuum properly. We applied the formalism to 120Sn and showed that the pairing correlations enhance the collectivity of the positive parity low-lying states, while that of the negative parity low-lying states are hindered. We found that the QRPA is more satisfactory in reproducing the experimental data of the energy of low-lying modes of excitation, while the giant resonances are not much affected by the pairing correlations. We would like to point out that these results however do not justify the RPA model without the pairing correlations for the study of giant resonances in open-shell nuclei, especially near the drip-lines. Since the single-particle energies and wave functions could be different in principle due to the density dependence of the mean-field, the response properties even in the giant resonance region might be affected by the pairing correlations. We therefore advocate to use the QRPA all through the excitation region in open-shell nuclei.

There are many possible applications of the continuum QRPA method presented in this paper. One of them is a neutrino-nucleus scattering, e.g. 12C($`\nu ,\nu ^{}`$)12C  and 12C($`\nu _e,e^{}`$)12N , where the RPA and the QRPA have been one of the standard methods for theoretical investigations. Another application will be the excitations of drip-line nuclei. Because of a low energy threshold, the responses would be very sensitive to the pairing correlations. In these cases, the pairing active space includes particle continuum states and the BCS approximation should be carefully examined. Also, the residual interaction in the particle-particle channel, which we neglected in this paper, might have to be taken into account. A more sophisticated treatment of the pairing interaction is provided by the Hartree-Fock-Bogoliubov (HFB) theory, which consistently describes couplings between the particle-hole and the particle-particle channels. It would be an interesting future work to develop a continuum QRPA theory based on the HFB approximation.

## Acknowledgment

We are grateful to the Institute for Nuclear Theory at the University of Washington, where this work was initiated during the INT program INT-00-3 on “Nuclear structure for the 21st century”. We thank its hospitality and a partial financial support for this work. We thank also K. Matsuyanagi and Nguyen Van Giai for useful and stimulating discussions and Baha Balantekin for discussions on the RPA approach to neutrino-nucleus reactions. This work is supported in part by the Ministry of Education, Science, Sports and Culture in Japan by Grant-In-Aid for Scientific Research under the program number (C(2)) 12640284.


format: text

text:
# Electrical Transport Properties of Single Crystal "Sr"₃"Ru"₂"O"₇: The Possible Existence of an Antiferromagnetic Instability at Low Temperatures

## I INTRODUCTION

The discovery of superconductivity in the layered perovskite Sr2RuO4 , which appears to posses a $`p`$-wave spin-triplet pairing , has renewed interest in the magnetic properties of related compounds, such as SrRuO3 and Sr3Ru2O7. Understanding the magnetic properties of these compounds may provide clues to the mechanism leading to $`p`$-wave pairing in Sr2RuO4.

SrRuO3, the three-dimensional (3D), cubic perovskite in the Ruddlesden-Popper (R-P) series (Srn+1RunO3n+1, with $`n=\mathrm{}`$), is an established ferromagnet with $`T_c`$ = 160 K . For Sr3Ru2O7, the n=2 member in the R-P series, has been the subject of controversy regarding its magnetic properties . In the original work of Cava et al on phase-pure, polycrystalline $`\text{Sr}_3\text{Ru}_2\text{O}_7`$ , the magnetic susceptibility $`\chi `$ was found to show a peak around 15 K, accompanied by a Curie-Weiss behavior at high temperatures, $`\chi =\text{C}/(T\theta _{\text{CW}})`$, where C is the Curie constant, $`T`$ is the temperature, and $`\theta _{\text{CW}}`$ is the Curie temperature, yielding negative $`\theta _{\text{CW}}`$ 15 K and a large moment of 2.5 $`\mu _\text{B}`$/Ru.

In a subsequent study, using single crystals of Sr3Ru2O7 prepared by flux method, Cao et al  reported a ferromagnetic (FM) ordering at 104 K under ambient pressure. This result was in sharp contrast with the neutron diffraction results on polycrystalline $`\text{Sr}_3\text{Ru}_2\text{O}_7`$, which did not reveal any long-range magnetic ordering down to 1.6 K . Recently, Ikeda et al.  reported the magnetic susceptibility ($`\chi (T)`$) data of Sr3Ru2O7 obtained on crystals prepared by the FZ method, which shows a peak at about 17 K but no ferromagnetic ordering. This result is different from Cao’s result, but consistent with earlier results obtained in polycrystals. It has been suggested that the FM ordering observed in flux crystals was induced by contamination from impurities of the flux, the crucible, or a combination of both .

Ikeda et al. also studied the magnetic properties of Sr3Ru2O7 under hydrostatic pressure. Clear evidence for FM ordering was found. The FM transition temperature, $`T_c`$, was found to be 70 K at 1.1 GPa. Therefore the authors argued that Sr3Ru2O7 is a nearly FM Fermi liquid. They furtherfore suggested that the maximum behavior in $`\chi (T)`$ might be due to the critical spin fluctuations found close to a quantum critical point, as in the case of (Ca,Sr)2RuO4  and MnSi .

To further clarify the nature of the magnetic fluctuations in Sr3Ru2O7, we have carried out Hall coefficient ($`R_\mathrm{H}`$) and magnetoresistance (MR) measurements using Sr3Ru2O7 single crystals grown by the FZ method. In this article, we will present the results of our measurements and discuss their physical implications.

## II EXPERIMENTAL METHODS

Single crystals of $`\text{Sr}_3\text{Ru}_2\text{O}_7`$ used in this study were grown by the floating-zone method. $`X`$-ray diffraction measurements confirmed a crystal structure of

the $`n`$=2 R-P compound, showing no impurity phases. For in-plane MR and Hall measurements, we used two rectangular-shaped single crystals with dimensions around $`0.5\times 0.1\times 0.1`$ and $`0.8\times 0.3\times 0.15\text{mm}^3`$, respectively. For each sample, two current contacts covering the opposite ends and four voltage contacts on the two sides of the crystal were prepared. All $`\text{RuO}_2`$ layers were electrically shorted along the c-axis to ensure a homogeneous current distribution. The c-axis transverse ($`HI`$) MR measurements were carried out in a single crystal with dimensions around $`0.8\times 0.4\times 0.2`$ mm3. Two ring-shaped current contacts were prepared on the opposite $`ab`$ faces. The two voltage contacts were point-like positioned in the center of the rings.

Electrical measurements were carried out in a 3He and dilution refrigerator. The temperature was measured using a Lakeshore Cernox 1030 thermometer with relative temperature corrections (due to the applied magnetic field, typically 0.15% at 4.2 K and 5.9% at 2K and 8.0T). For transverse and longitudinal MR measurements, the magnetic field $`H`$ was applied perpendicular and parallel to the injected current $`I`$, respectively. In order to exclude the Hall contribution to the MR, only the symmetric part of $`\mathrm{\Delta }\rho _{ab}(H)=\rho _{ab}(H)\rho _{ab}(0)`$ under field reversal was included. For Hall measurements, the magnetic field was applied parallel to the $`c`$-axis with a current bias applied along the $`ab`$-plane. The Hall voltage $`V_\mathrm{H}`$, which contains only the asymmetric contributions under field reversal, was found to vary linearly with $`H`$ up to 4 T over the whole temperature region. By fitting $`V_\mathrm{H}(H)`$ data using $`V_\mathrm{H}=R_\mathrm{H}HI/d`$ ($`d`$ is the thickness of the sample along the $`c`$-axis), the Hall coefficient $`R_\mathrm{H}`$ was obtained.

## III EXPERIMENTAL RESULTS AND DISCUSSIONS

Figure 1 shows the temperature dependence of electric resistivity for in- and out-of-plane directions of the Sr3Ru2O7 crystals (denoted by $`\rho _{ab}`$ and $`\rho _c`$ respectively). The overall shape of these data are similar to those reported in Ref.10. Both $`\rho _{ab}(T)`$ and $`\rho _c(T)`$ are metallic in the whole temperature region. The sharp drop in $`\rho _c(T)`$ below 50 K has been attributed to the suppression of thermal scattering between quasi-particles and phonons . Interestingly, both $`\rho _{ab}`$ and $`\rho _c`$ were found to show an apparent slope change around 17 K (see the inset of Fig. 1). This temperature is close to that below which the magnetic susceptibility drops sharply, indicating that magnetic fluctuations have strong influence on the electrical transport properties.

The temperature dependence of the Hall coefficient $`R_\mathrm{H}`$ is shown in Fig. 2. $`R_\mathrm{H}`$ is positive over the entire temperature region studied (0.30-300K), reaching a maximum at the same temperature (=17 K) where both $`\rho _{ab}(T)`$ and $`\rho _c(T)`$ show a slope change ($`T`$* will be used to denote this characteristic temperature). These observations agree well with a previous report  in which $`R_\mathrm{H}`$ was measured on single crystals prepared by the FZ method as well.

The temperature dependence of $`R_\mathrm{H}(T)`$ is strikingly similar to that of $`\chi (T)`$ . Such a behavior was observed previously in heavy fermion compounds such as in UPt3  and ferromagnetic metals . It was found that $`R_\mathrm{H}`$ can be fit by

$$R_\text{H}=R_\text{0}+R_\text{s}\times 4\pi \chi (T).$$
(1)
$`R_\text{0}`$ and $`R_\text{s}`$ are referred to as the normal and anomalous Hall coefficients respectively. Such behavior of $`R_\mathrm{S}`$ can be understood in the picture of a skew scattering that involves competition between spin-orbit coupling and spin-flip scattering .

For Sr3Ru2O7, it has been shown that $`\chi (T)`$ satisfies the Curie-Wiess law  at high temperatures. We have attempted to fit our $`R_\mathrm{H}`$ data shown in Fig.2 using the following equation,

$$R_\text{H}=R_\text{0}+R_\text{s}^{}/(T\theta _{\text{CW}}),$$
(2)
with three fitting parameters. The best fit (see the solid line in Fig. 2) was obtained at $`R_0=1.4\times 10^{10}`$ m3/C, $`\theta _{\mathrm{CW}}`$ = -102 K, and $`R_\mathrm{S}^{}`$ = 1.7$`\times 10^7`$ m3/C. The absolute value of $`\theta _{\mathrm{CW}}`$ so obtained is higher than that obtained by fitting $`\chi (T)`$ curves (around -15 K for polycrystals and -40 K for single crystals), but has the same sign as that found from magnetic susceptibility measurements. $`R_0`$ was found to be negative, which means that the normal Hall effect is dominated by electrons. This is consistent with our expectation since band structure calculations reveal that in Sr3Ru2O7 there are four electron- and two hole-like bands crossing the Fermi surface . These observations suggest that skew scattering is a reasonable picture for understanding our $`R_\mathrm{H}(T)`$ result.

As pointed out in Ref. 19, a negative $`\theta _{\mathrm{CW}}`$ does not mean that the magnetic fluctuations are necessarily anti-ferromagnetic (AFM) in nature, as frequently assumed in literature. In fact, we found that $`V_\mathrm{H}`$ as a function of magnetic field deviated from linear behavior above $`T`$* (see inset of Fig. 2) in a manner characteristic of ferromagnetic behavior, consistent with the argument of nearly FM behavior in Ref.10. However, below $`T`$\*, $`V_\mathrm{H}`$ becomes linear with $`H`$.

Figure 3 shows the transverse in-plane MR, $`\mathrm{\Delta }\rho _{ab}^{}/\rho _{ab}`$ ($`HI`$), between 0 and 7.3 T at various temperatures. At high temperatures, $`\mathrm{\Delta }\rho _{ab}^{}/\rho _{ab}`$ is negative and small, varying monotonically with $`H`$. The magnitude of $`\mathrm{\Delta }\rho _{ab}^{}/\rho _{ab}`$ increases with decreasing temperature down to 30 K. As $`T`$ approaches $`T`$* from high temperatures, the opposite tendency is observed. The value of $`\mathrm{\Delta }\rho _{ab}^{}/\rho _{ab}`$ eventually becomes positive with $`T<T`$* (=17 K). Another striking feature is that, below $`T`$\*, $`\mathrm{\Delta }\rho _{ab}^{}/\rho _{ab}`$ shows a non-monotonic field-dependence. With increasing $`H`$, $`\mathrm{\Delta }\rho _{ab}^{}/\rho _{ab}`$ initially increases then decreases after reaching a maximum at $`H_{\mathrm{max}}`$, which appears to increase with decreasing temperature. This non-monotonic behavior of $`\mathrm{\Delta }\rho _{ab}^{}/\rho _{ab}`$($`H`$) persists to the lowest temperature measured.

We also measured the longitudinal in-plane MR, $`\mathrm{\Delta }\rho _{ab}^{}/\rho _{ab}`$, of Sr3Ru2O7. As shown in Fig. 4, $`\mathrm{\Delta }\rho _{ab}^{}/\rho _{ab}`$ exhibits similar features as $`\mathrm{\Delta }\rho _{ab}^{}/\rho _{ab}`$. In particular, it also shows a sign reversal at temperatures slightly lower than $`T`$\*. A more pronounced non-monotonic field-dependence was also found for $`\mathrm{\Delta }\rho _{ab}^{}/\rho _{ab}`$ for $`T<`$15 K.

We would like to point out another important feature in Fig. 3 and 4: The magnitude of $`\mathrm{\Delta }\rho _{ab}^{}/\rho _{ab}`$ is greater than that of $`\mathrm{\Delta }\rho _{ab}^{}/\rho _{ab}`$ at the same magnetic field below approximately 10 K. Since the current is not subject to the Lorentz force in the longitudinal configuration, it reflects mostly the contribution of spins. Therefore, this observation, together with that of the skew scattering, suggests that spin scattering has a strong influence on the electrical transport in Sr3Ru2O7.

Figure 5 shows the transverse $`c`$-axis MR ($`\mathrm{\Delta }\rho _c^{}/\rho _c`$) of Sr3Ru2O7 at different temperatures. It is clear that $`\mathrm{\Delta }\rho _c^{}/\rho _c`$ exhibits all the features observed in the in-plane MR. The only obvious difference is that the negative-to-positive sign reversal in $`\mathrm{\Delta }\rho _c^{}/\rho _c`$ was found at a slightly lower temperature(10 K).

It is remarkable that a maximum in $`\chi (T)`$ and $`R_\mathrm{H}(T)`$, a slope change in $`\rho _{ab}(T)`$ and $`\rho _c(T)`$, a deviation from linear magnetic field dependence in $`V_\mathrm{H}`$, and a sign change in longitudinal and transverse MR, were all found at approximately the same temperature. These observations suggest that in Sr3Ru2O7, instead of continuing its trend to move closer to FM ordering as temperature is lowered, as one would naturally expect, the system is side tracked to a different behavior below $`T`$\*. This qualitative change in the dynamics of the system has to be magnetic in origin.

Physical insight may be obtained from the (Ca2-xSrx)RuO4 solid solution system . For $`x<0.2`$, (Ca2-xSrx)RuO4 is antiferromagnetic. For $`0.2x0.5`$, this material system is near a FM instability. In particular, at $`x0.5`$, it is nearly ferromagnetic,

evolving from paramagnetic Sr2RuO4 through band narrowing. Between $`0.2x<0.5`$, it changes into a state with short-range AFM ordering below a characteristic temperature $`T_\mathrm{P}`$ ($`T_\mathrm{P}`$, which is about 10 K at $`x=0.2`$, decreases continuously to zero at $`x=0.5`$). Below $`T_\mathrm{P}`$, $`\rho _{ab}(T)`$ shows a change of slope. MR shows a negative-positive sign reversal and non-monotonic behavior in field dependence. In addition, both $`\chi (T)`$ and $`R_\mathrm{H}`$ show a maximum at $`T_\mathrm{P}`$.

The phenomena seen in (Ca2-xSrx)RuO4 are clearly similar to those of Sr3Ru2O7. Furthermore, (Ca2-xSrx)RuO4 and Sr3Ru2O7 have comparable electronic specific heat coefficients and Wilson ratios. All these similarities suggest that the magnetic correlations in Sr3Ru2O7 show a qualitative change below $`T`$\*. At high temperatures, FM spin fluctuations dominate because of the close proximity to the FM instability, while at low temperatures (below $`T`$\*) they cross over to AFM fluctuations.

In the magnetization ($`M`$) vs. field ($`H`$) curve obtained on Sr3Ru2O7 poly-crystals , $`M(H)`$ shows a convex character at low fields below $`T`$\*. This is a characteristic feature of AFM correlations. Above $`T`$\*, $`M(H)`$ shows a concave feature, typical of FM correlations. This further supports the observation that as the temperature decreases, Sr3Ru2O7 at ambient pressure moves away from an FM, but closer to an AFM magnetic instability. This scenario seems to be capable of explaining all features seen in the electrical transport in Sr3Ru2O7 described above.

In (Ca2-xSrx)RuO4, the change of magnetic correlations is driven by a structural phase transition at temperature above $`T_\mathrm{P}`$ . In Sr3Ru2O7, although neutron diffraction measurements did not reveal any structural transition , an unusual change in structural details at low temperature, i.e., a negative thermal expansion along the $`c`$-axis, was observed. This might be responsible for the change of magnetic coupling at low temperatures.

We note, however, that the anisotropy in $`\chi (T)`$ between the in- and out-of-plane directions in Sr3Ru2O7 single crystals  is quite small. In addition, $`\chi (T)`$ was found to saturate below roughly 6 K. How do we explain these observations in the picture of AFM fluctuations below $`T`$\*?

This apparent difficulty may be solved if we assume that the spins aligned anti-ferromagnetically in Sr3Ru2O7 are canted to the $`c`$-axis. A small net ferromagnetic component in the c-axis in the canted AFM can explain the slight hysteresis observed in the $`MH`$ curve on poly-crystals Sr3Ru2O7 . The saturation of $`\chi (T)`$ below 6 K is likely to imply that the crossover from FM to AFM is incomplete, probably because Sr3Ru2O7 does not undergo a structural phase transition as in (Ca2-xSrx)RuO4. That might also be the reason why neutron diffraction did not detect any sizable magnetic ordering.

For (Ca2-xSrx)RuO4, the magnetic instability in the $`0.2x0.5`$ region leads to non-Fermi liquid behavior. Its $`\rho _{ab}(T)`$ shows a $`T^{1.4}`$ dependence. For Sr3Ru2O7, our resistivity data exhibit a similar behavior. Both $`\rho _{ab}(T)`$ and $`\rho _c(T)`$ clearly deviate from $`T`$-squared dependence. The best fit is $`T^{1.4}`$ for $`\rho _{ab}(T)`$ and $`T^{1.2}`$ for $`\rho _c(T)`$, as shown in Fig. 6. However, we note that the residual resistivity $`\rho _0`$ estimated from Fig. 1 is about 19.0 (2.8) $`\mu \mathrm{\Omega }`$cm for $`\rho _{ab}`$ ($`\rho _c`$). It is about five times (for $`\rho _{ab}`$) and two times (for $`\rho _c`$) greater than that reported by Ikeda in Ref.10, suggesting that our FZ crystals may contain slightly more impurities and defects than theirs. As a result, it is natural to ask whether the observed non-$`T^2`$ behavior is intrinsic to Sr3Ru2O7. In Ref.10, it was argued that Sr3Ru2O7 is a Fermi liquid with $`\rho _{ab}(T)T^2`$. However, their $`T`$-squared fitting for resistivities, especially for $`\rho _{ab}(T)`$, appears to be less than the best fit. A deviation from the $`T`$-squared dependence in $`\rho _{ab}(T)`$ is clearly visible even below 6 K. This deviation suggests an intrinsic deviation from Fermi liquid behavior in Sr3Ru2O7, most probably due to the system being close to an AFM instability.

The non-monotonic field-dependence of MR observed in Sr3Ru2O7 below $`T`$* can be easily understood in the crossover scenario as discussed above, in which the MR should contain both negative and positive terms. The negative term must have originated from the development of FM spin fluctuations as the field increases.

## IV CONCLUSION

In summary, we have studied the transport properties of Sr3Ru2O7 under magnetic field using single crystals prepared by the FZ method. The temperature dependence of the in-plane Hall coefficient has been found to resemble that of the magnetic susceptibility, showing a maximum at $`T`$\*. The field dependence of $`V_\mathrm{H}`$ was found to deviate from linear behavior above $`T`$\*. Both $`\rho _{ab}(T)`$ and $`\rho _c(T)`$ exhibit a slope change at about $`T`$\*. Furthermore, we found that the longitudinal in-plane MR is larger than the transverse. Both the in-plane and $`c`$-axis MR show a negative-to-positive sign reversal below $`T`$\*. All these observations support our assessment that the magnetic correlations in Sr3Ru2O7 are dominated by FM fluctuations above $`T`$\*, but cross over to AFM behavior blow $`T`$\*. Finally, the ground state may deviate from the conventional Fermi-liquid behavior.

We acknowlege useful discussions With Prof. Y. Maeno and Dr. S-I Ikeda. Y. Liu has benefited from communications with Dr. G. Cao. This work is supported by NSF through grants DMR-9702661 and ECS-9705839 at Penn State and DMR-9808941 at Princeton.