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PHYSICAL REVIEW B 79, 174403 2009

Néel and valence-bond crystal order on a distorted kagome lattice:

Implications for Zn-paratacamite

Erik S. Sørensen, ^{1}^{,} * Michael J. Lawler, ^{2}^{,}^{3} and Yong Baek Kim ^{4}

^{1} Department of Physics and Astronomy, McMaster University, Hamilton, Ontario, Canada L8S 4M1 ^{2} Department of Physics, Applied Physics, and Astronomy, Binghamton University, P.O. Box 6000, Binghamton, New York 13902-6000, USA ^{3} Department of Physics, Cornell University, Ithaca, New York 14853, USA ^{4} Department of Physics, University of Toronto, Toronto, Ontario, Canada M5S 1A7 Received 19 February 2009; published 4 May 2009

Zn-paratacamite is a rare spin-1/2 antiferromagnetic insulator with an ideal kagome lattice structure in part of its phase diagram. As a function of Zn doping, this material undergoes a structural distortion which relieves the frustration and introduces magnetic order in the ground state, though the precise nature of the order is not clear at this point. In this paper, we present strong evidence for Néel ordering in the strongly distorted phase of Zn-paratacamite through the application of quantum Monte Carlo techniques. These numerical results support a recent Schwinger-boson mean-ﬁeld theory of Zn-paratacamite. For weak distortion, close to the ideal kagome limit, our results indicate a regime with no Néel order but with broken glide-plane symmetry. For this model the glide-plane symmetry is broken by any valence-bond crystal. Hence, our results lend support to recent proposals P. Nikolic and T. Senthil, Phys. Rev. B 68 , 214415 2003 ; R. R. P. Singh and D. A. Huse, Phys. Rev. B 76, 180407 R 2007 of a valence-bond crystal ground state for the undistorted lattice. The phase transition between the two phases could be in the deconﬁned universality class if it is not a ﬁrst-order transition.

PACS number s : 75.10.Jm, 73.43.Nq, 75.40.Mg

I. INTRODUCTION

Recently, a number of spin-1/2 frustrated magnetic insu- lators have been discovered without any sign of magnetic order or structural distortions down to the lowest tempera- tures studied. ^{1}^{–}^{4} Among these materials, the Zn-doped- paratacamite family stands out for having a nearly control- lable degree of distortion allowing the amount of geometric frustration to be tuned directly by an experimentalist. As such, they are a promising place to look for new phases of matter while at the same time probe how these new phases may be related to more well understood phases. The control of the distortion is largely through the chemi- cal pressure induced by the substitution of Zn atoms for Cu atoms on the gray triangular lattice planes that live in be- tween kagome planes, as shown in Fig. 1. While Zn and Cu atoms are similar in size, Zn atoms ﬁt into these sites without disrupting their environment, unlike Cu atoms which distort the kagome planes given a high enough density. In particular, for less than 0.3 ﬁlling of Zn atoms greater than 0.7 ﬁlling of Cu atoms the lattice distorts in a remarkable bipartite structure and magnetic order is found in the ground state. ^{3}^{,}^{5}^{,}^{6} The spins are thus relatively unfrustrated at these low doping concentrations. For Zn doping larger than this threshold, the lattice has the undistorted ideal kagome form and for x 0.4 no magnetic ordering has been reported down to 50 mK despite an estimated spin exchange J 200 K. ^{5} A natural theoretical model of this material is the spin-1/2 Heisenberg model with two exchange parameters on a dis- torted kagome lattice ^{5}^{–}^{7} see Fig. 1 :

H = J _{} S _{i} · S _{j} + _{D} J _{} S _{i} · S _{j} .

i , j

ij

1

Here _{D} tunes the distortion on the next-nearest-neighbor bonds nnn with _{d} =1 the undistorted ideal kagome limit where nnn bonds are equivalent to nn bonds . This is an idealized model for several reasons: it assumes the coupling between planes and further neighbors is weak which seems reasonable ^{5}^{,}^{6} , it neglects Dzyaloshinsky-Moria interactions possibly important for the low-temperature susceptibility, ^{8}^{,}^{9}

FIG. 1. Color online The layered Zn-paratacamite magnetic lattice structure. Cu atoms live on the sometimes distorted kagome layer bronze atoms while Zn or Cu atoms occupy sites on a trian- gular lattice above the kagome plane gray atoms . Solid purple bonds represent nearest neighbors ij in Eq. 1 resulting in a “brick-wall” lattice, while transparent bronze bonds represent the next-nearest neighbors ij in Eq. 1 .

1098-0121/2009/79 17 /174403 6

174403-1

©2009 The American Physical Society

∆

SØRENSEN, LAWLER, AND KIM

PHYSICAL REVIEW B 79, 174403 2009

and it replaces the effect of doping in the triangle lattice planes with the uniform distortion parameter _{D} . While it is possible that any of these approximations may be important for some properties of Zn-paratacamite, here we will focus on those properties which clearly belong to the phenomenol- ogy of this simpliﬁed model. In this paper, we study the ground-state properties of the Hamiltonian in Eq. 1 as a function of _{D} , extrapolating between a bipartite “brick-wall” lattice at _{D} =0 and the iso- tropic kagome lattice at _{D} =1. At _{D} =0, we show using valence-bond quantum Monte Carlo ^{1}^{0}^{,}^{1}^{1} that the ground state is magnetically ordered with the expected Néel pattern for this bipartite lattice and with a magnetization of m ^{†} =0.240 1 that is 22% smaller than the square lattice value. ^{1}^{2} For 0 _{D} 1 we study this model using exact diagonaliza- tion on ﬁnite-size clusters of size 12, 24, and 36 sites. By introducing symmetry breaking ﬁelds, we study the suscep- tibility of the ground state toward dimerization. Remarkably, we ﬁnd that for _{D} 0.8, a phase transition occurs toward a rotationally invariant state which prefers to have a broken glide-plane GP symmetry, consistent with the presence of a valence-bond crystal VBC order including the pin-wheel VBC pattern proposed by Ref. 7. This symmetry breaking survives up to the _{D} =1 ideal kagome limit. While it is difﬁcult to draw deﬁnitive conclusions on such small sys- tems, a broken glide-plane symmetry supports Refs. 13–15 proposal that the spin-1/2 kagome antiferromagnet has a VBC ground state. At the same time a broken glide-plane symmetry is not consistent with a spin-liquid phase, fre- quently supported by other exact diagonalization studies. ^{1}^{6} In addition, while we cannot rule out a ﬁrst-order transition from a VBC phase to the Néel phase in our model, it is also possible this quantum phase transition is in the deconﬁned universality class. ^{1}^{7}

II. RESULTS AT _{D} = 0

We ﬁrst discuss our results obtained at _{D} =0 where we have been able to study large system. As can be seen from Fig. 1, where the transparent bronze bonds are proportional to _{D} , the lattice formed by the remaining solid purple bonds is a bipartite “brick-wall” lattice with a coordination number of 3 on two thirds of the sites and of 2 on the re- maining sites. Due to the bipartite nature of the _{D} =0 lattice there is no frustration. A classical antiferromagnetic Néel state can be unambiguously assigned to the lattice. It is then possible to perform very efﬁcient quantum Monte Carlo simulations using the recently proposed ^{1}^{0}^{,}^{1}^{1} valence-bond quantum Monte Carlo VBQMC . For _{D} =0 there is no sign problem and extremely precise results can be obtained. VBQMC is a projection method where the T =0 ground state is projected out through the repeated application of the Hamiltonian, H , on a trial state, _{T} . In essence, _{G}

= − H ^{n} _{T} . In the limit where n → this becomes exact. In

a practical implementation n is kept ﬁxed at a high number

and the different terms in _{G} are sampled using Monte Carlo methods. For convergence, the relevant lattice size- independent expansion order is n / N _{b} , where N _{b} is the num- ber of terms in the Hamiltonian. N _{b} is equal to 4 / 3 N for the

0.040

0.035

0.030

0.025

0.020

0.015

0.010

0.005

0.000

n/N b =5

n/N b =7

n/N b =10

0

0.001

0.002

0.003

0.004

0.005

0.006

1/N

FIG. 2. Color online The singlet-triplet gap, , versus inverse system size 1 / N . The different curves correspond to different ex- pansion orders n , with the ratio n / N _{b} kept ﬁxed. Here, N _{b} is the number of bond operators in the Hamiltonian, N _{b} = 4 / 3 N . Results are shown for n / N _{b} =5 , n / N _{b} =7 , and n / N _{b} =10 . Error bars are shown but are typically smaller than the symbols.

brick-wall lattice, with N as the number of sites in the lattice. Typically we use n / N _{b} =3–10 and an extrapolation to n / N _{b} = can then be performed. We have performed systematic VBQMC studies of _{D} =0 brick-wall lattices with number of sites N =12 m ^{2} for

m =1,

10 ^{6} –10 ^{7} Monte Carlo steps were performed for a range of values of n / N _{b} =3,5,7,10. All error bars were calculated using standard binning techniques. A very natural question to ask is if the _{D} =0 brick-wall lattice has a nonzero singlet to triplet gap, . A particularly appealing feature of VBQMC is that it allows for a direct estimator ^{1}^{0}^{,}^{1}^{1} of this gap independent of the estimators for the ground-state singlet and excited triplet energies. Due to a cancellation of errors it is then possible to calculate this gap with a precision signiﬁcantly exceeding that which could have been obtained by separately calculating the ground and excited state energies. Our results for at _{D} =0 are shown in Fig. 2. Data are shown for three different values of n / N _{b} =5 , n / N _{b} =7 , n / N _{b} =10 versus inverse system size 1 / N . At N =1200, n / N _{b} =10 the gap is =0.0059 1 J and minimal dependence on the expansion or- der n / N _{B} is seen. From the results shown in Fig. 2 we con- clude that the gap vanishes in the thermodynamic limit. For the two-dimensional square lattice antiferromagnetic Heisenberg model it is well known ^{1}^{8} that the antiferromag- netic order exists at T =0 with m ^{†} =0.30743 1 Ref. 12 . The square lattice has a coordination number of 4 whereas the brick-wall lattice has a mixed coordination of 2 and 3. We therefore expect m ^{†} to be smaller or possibly zero for the brick-wall lattice. As usual, we deﬁne

,10 using periodic boundary conditions. Typically,

S q _{c} =

2

1

N

x

, y

^{˜} S ^{z} x , y _{} ^{2} _{} ,

2

where q _{c} is the wave vector of the staggered magnetization

˜

and S ^{z} x , y is given by

174403-2

NÉEL AND VALENCE-BOND CRYSTAL ORDER ON A…

0.10

0.08

0.06

0.04

0.02

0.00

0.00

0.05

0.10

0.15

0.20

0.25

S(q c )

N -1/2

FIG. 3. Color online The structure factor, S q , versus inverse linear system size 1 / N . Results are shown for n / N _{b} =10. Error bars are shown but are typically smaller than the symbols. Results for n / N _{b} =7 are indistinguishable from the n / N _{b} =10 results shown and have been left out for clarity.

c

˜ 1

S ^{z} x , y = _{2} _{x} _{,} _{y} ^{z} x , y ,

3

with

point x , y belongs to. Hence we have ^{1}^{8}

^{} x , y

equal to +1 or −1 depending on what sublattice the

˜

m ^{†} = S ^{z} = lim

i

L →

3 S q _{c} .

4

Our results for S q _{c} for n / N _{b} =10 are shown in Fig. 3. It is

expected

form 1 / N and a ﬁt to this form yields S q _{c} =0.0192 5 and consequently

m ^{†} = 0.240 3 .

As expected, this value is reduced with respect to the square lattice result, but is clearly nonzero, indicating a well- established antiferromagnetic order at _{D} =0.

5

18 that the leading ﬁnite-size corrections are of the

III. RESULTS AT _{D} Å 0

We now turn to a discussion of our results for 0 _{D} 1. In this case it is no longer possible to perform VBQMC calculations due to a sign problem that appears rather severe as soon as _{D} 0 and reliable numerical results are therefore much harder to obtain. In light of the strong sign problem we have performed exact diagonalization studies for 0 1 on ﬁnite-size systems employing periodic boundary condi- tions. Our goal is to study generalized bond susceptibilities with respect to symmetry breaking ﬁelds. We focus on C _{2} and GP symmetry breaking ﬁelds shown in Fig. 4 where the dimers indicate bonds where the strength is modiﬁed J _{} = J . The C _{2} symmetry corresponds to a rotation by and clearly the ﬁeld shown in Fig. 4 a breaks this symmetry. The GP symmetry ^{7} is somewhat more exotic and corresponds to a translation along the rails where the dimers are sitting fol- lowed by a reﬂection around one of these rails. We note that the GP ﬁeld does not break the C _{2} symmetry and likewise the

PHYSICAL REVIEW B 79, 174403 2009

(a)

(b)

FIG. 4. Color online a The glide-plane symmetry breaking ﬁeld. b C _{2} symmetry breaking ﬁeld. Solid dimers denote bonds

where the coupling strength is modiﬁed to J _{} .

C _{2} ﬁeld preserves the GP symmetry. The pin-wheel VBC discussed in Ref. 7 would break the GP symmetry but not the C _{2} symmetry where as the columnar VBC Ref. 7 would break both. If we by b , b _{C} _{2} _{,}_{G}_{P} denote the ground-state expec- tation value S _{i} · S _{j} for the bond b and its partner under the

symmetry operation b _{C} _{2} _{,}_{G}_{P} , we can deﬁne the generalized bond susceptibility as follows:

_{C} _{2} _{,}_{G}_{P} = lim

→ 0

with

b _{C} _{2} _{,}_{G}_{P} J _{} = J + − b _{C} _{2} _{,}_{G}_{P} J _{} = J −

2

^{,}

6

b _{C} _{2} _{,}_{G}_{P} = b J _{} − b _{C} _{2} _{,}_{G}_{P} J . 7

Clearly, if b goes to zero linearly with the generalized bond susceptibility is a constant independent of system size and the associated symmetry is not spontaneously broken. On the other hand, a bond susceptibility diverging with sys- tem size signals that the associated symmetry is spontane- ously broken in the thermodynamic limit. When performing exact diagonalization studies of small systems the choice of the ﬁnite cluster is crucial since the smaller clusters will reduce the point group symmetry of the inﬁnite lattice. For the isotropic kagome lattice, _{D} =1, the plane group is p 6 mm . This symmetry group implies that for the isotropic kagome lattice all bonds are equivalent. Our choice of ﬁnite clusters are shown in Fig. 5 for N =12,24,36. Only the N =36 cluster has the full symmetry point group symmetry of the kagome lattice. However, for all clusters do we ﬁnd that all bonds are equivalent at _{D} =1. For 0 _{D} 1 only two different types of bonds occur for these clusters. These are the only clusters we have found with these properties. For the bond susceptibilities to yield mean- ingful information about the thermodynamic limit this is very important since we want to make sure that the presence of a reduced point group symmetry does not explicitly break the C _{2} or GP symmetry. This is not the case for the clusters shown in Fig. 5. Using the clusters from Fig. 5 we can now study _{G}_{P} and _{C} _{2} as a function of _{D} for the different clusters. Our results are shown in Figs. 6 and 7, respectively. We have used

174403-3

_{C}_{2}

χ

_{G}_{P}

χ

SØRENSEN, LAWLER, AND KIM

PHYSICAL REVIEW B 79, 174403 2009

FIG. 5. Color online The 12-, 24-, and 36-site lattices.

0.001 small enough that , Eq. 6 , is almost completely independent of . We begin by discussing _{G}_{P} shown in Fig. 6. For _{D} less than roughly 0.8 do we ﬁnd that _{G}_{P} is almost independent of N . In the inset is shown 1 / _{G}_{P} as a function of 1 / N for =0.3 indicating a ﬁnite value in the thermodynamic limit. This is consistent with the GP symme- try not being broken. However, for _{D} greater than 0.8 pronounced size dependence occurs. At _{D} =1, 1 / _{G}_{P} as a function of 1 / N is shown in the inset. In this case it seems reasonable to conclude that _{G}_{P} diverges with N and hence that the GP symmetry is spontaneously broken in the ther- modynamic limit. A natural interpretation of this result is that a quantum phase transition occurs at 0.8 between a state with antiferromagnetic order, which does not break the GP symmetry, to a new phase where the GP symmetry is broken. Finally, in Fig. 7 we show our results for _{C} _{2} . Again we see that for _{D} smaller than roughly 0.8 there is very little N dependence. In the inset of Fig. 7 is shown 1 / _{C} _{2} as a function of 1 / N at _{D} =0.3. Clearly the results extrapolate to

8 1/χ GP

λ

D =1

6

1

4

2

λ

D =0.30

0

0

0.05

1/N

0.1

N=12

N=24

N=36

0

0

0.1

0.2

0.3

0.4

0.5

0.6

0.7

0.8

0.9

1

1.2

0.8

0.6

0.4

0.2

^{λ} D

FIG. 6. Color online The glide-plane susceptibility, _{G}_{P} as a

function of _{D} for the different system sizes, N =12,24,36. The circles represent results for N =36, _{D} =0.3. The inset shows _{G}_{P}

versus 1 / N at _{D} =0.3,1.0.

−1

20

18

N=12

1

N=24

λ

D =0.30

N=36

16

0.8

14

0.6

12

0.4

10

λ

D =1

0.2

8

0

0

0.05

0.1

6

1/N

4

2

0

0

0.1

0.2

0.3

0.4

0.5

0.6

0.7

0.8

0.9

1

1/χ C2

^{λ} D

FIG. 7. Color online The C _{2} susceptibility _{C} _{2} as a function of _{D} for the different system sizes, N =12,24,36. The circles repre- sent results for N =36, _{D} =0.3. The inset shows _{C} _{2} versus 1 / N at _{D} =0.3,1.0.

a ﬁnite value in the thermodynamic limit consistent with the absence of C _{2} symmetry breaking as would be the case for an antiferromagnetic phase. As before, we ﬁnd that for _{D} greater than roughly 0.8 pronounced ﬁnite-size effects oc- cur consistent with a quantum phase transition. However, in this case, as can be seen in the inset of Fig. 7 at _{D} =1, the susceptibility does not diverge but rather tends to a ﬁnite, possibly very small value in the thermodynamic limit. There- fore, in the new phase occurring for _{D} greater than 0.8 the C _{2} symmetry is not broken. It is important to realize that several ﬁnite cluster effects are present in Figs. 6 and 7. First, the abrupt change in _{G}_{P} for N =12 in Fig. 6 is due to a level crossing that does not occur for N =24,36. The presence of such level crossings for small clusters is not surprising. Second, even though we be- lieve that we can reliably detect the divergence of _{G}_{P} , the eventual ordering occurring for _{D} 0.8 may not be compat- ible with the N =12,24 clusters. For example, the N =12,24 sized systems do not possess the translational symmetry of the large unit cell expected for the MZ state of Fig. 8 a . This could explain the relatively different appearance of the re- sults for N =24,36 in Fig. 6.

IV. DISCUSSION

Given these results, we may draw several conclusions. At _{D} =0, we have demonstrated that the spin gap vanishes and that the ground state has a ﬁnite staggered magnetization that is 22% smaller than the square lattice value. We ﬁnd this surprising given that each site has either two or three neigh- bors with 2.67 neighbors on average and that this network

is not far from the one-dimensional chain model which is disordered. It appears that this form of dimensional reduction does not easily suppress magnetic order. While we could only study very small system sizes for _{D} 0, ﬁnite-size effects seem to be small all the way out to _{D} 0.8. As a result, the antiferromagnetic order is quite

174403-4

NÉEL AND VALENCE-BOND CRYSTAL ORDER ON A…

(a)

(b)

FIG. 8. Color online a The Marston and Zeng MZ dimer pattern Ref. 19 on the kagome lattice and b the pin-wheel state on the distorted kagome lattice Ref. 7 . The MZ pattern arises by maximizing the number of dimers around each hexagon. Notice how the dimers on the two highlighted hexagons can be rotated by 180 about the center of the hexagon without needing to alter the rest of the dimer pattern. This benzenelike resonance suggests that ro- tational symmetry may be only very weakly broken if this is the ground state. The pin-wheel pattern, on the other hand, maximizes dimers around each rhombus and is manifestly C _{2} rotationally sym- metric about each hexagon.

robust and appears to be the ground state with a large basin of stability. The ground state for 0.8 _{D} 1 appears to break the glide-plane symmetry while remaining invariant under C _{2} rotations. While larger systems would be required to make deﬁnitive conclusions, this evidence is in stark contrast to the prediction that the kagome lattice ground state is a spin liquid. ^{1}^{9}^{,}^{2}^{0} Remarkably, on this lattice all valence-bond crystals break the glide-plane symmetry the most glide-plane symmetric conﬁguration of Fig. 4 b still breaks glide-plane symmetry if the missing dimers are added to the picture . So the break- ing of glide-plane symmetry strongly supports recent proposals ^{1}^{3}^{–}^{1}^{5} that the ground state may be a VBC. Candi- date such states include the Marston and Zeng 36-site unit cell dimer spin singlet pattern MZ ^{1}^{9} and the pin-wheel pattern in the presence of distortion see Fig. 8 . One may argue that the MZ pattern should also break C _{2} rotational symmetry. However, such a symmetry may naturally be re- stored by benzenelike resonances on the three dimer hexa-

PHYSICAL REVIEW B 79, 174403 2009

gons. One should note that whether the recent ED results ^{1}^{6} are disfavoring the MZ VBC state as well as other proposed VBC states ^{1}^{3}^{,}^{2}^{1} or not, is a subject of intense debate. ^{1}^{5} Since any VBC will have a diverging glide-plane suscep- tibility the results presented here are not very sensitive to transitions between different VBC’s as long as they conserve C _{2} symmetry. For example, a transition from the MZ pattern at _{D} =1 to the pin-wheel pattern at _{D} 1 is certainly pos- sible. For 0.8 _{D} we can therefore not exclude the presence of several different C _{2} symmetric VBC phases although the rate of divergence of _{G}_{P} could potentially be quite different for different phases. In fact, one might speculate that the cusp in _{G}_{P} for N =36 and in _{C} _{2} for N =24,36 in both cases at _{D} =0.98 is a signature of a phase transition between dif- ferent valence-bond crystals. A phase transition near _{D} 0.8 was also found in the large-N study of Ref. 7. Thus both large-N and exact diago- nalization methods predict the existence of a quantum phase transition at a value of _{D} away from the ideal kagome limit. If we assume that the spin gap is nonzero at _{D} =1 and van- ish approximately linearly with the deviation of _{D} from 1, then this value for the quantum critical point is also roughly consistent with the vanishing of the spin gap which, from exact diagonalizations, is estimated to be rather small but ﬁnite ^{2}^{0}^{,}^{2}^{2} in the thermodynamic limit and has a value of 0.1848J at _{D} =1 for the 36-site cluster . Given the apparent glide-plane symmetry breaking for _{D} 0.8, this phase tran- sition then appears to be between two phases with unrelated orders. It may therefore fall into the deconﬁned universality class ^{1}^{7} if it is not a ﬁrst-order transition.

c

ACKNOWLEDGMENTS

We thank Young Lee and Seung-Hun Lee for useful dis- cussions. This work was supported by the Natural Sciences and Engineering Research Council of Canada E.S.S. and

Y.B.K. , the Canadian Foundation for Innovation E.S.S. , the Canadian Institute for Advanced Research and the

E.S.S. gratefully

acknowledges the hospitality of the Department of Physics at the University of Toronto where part of this work was carried out. This work was made possible by the facilities of the

Canada Research Chair Program

Shared Hierarchical Academic Research Computing Net- work SHARCNET:www.sharcnet.ca .

*sorensen@mcmaster.ca ^{1} Y. Shimizu, K. Miyagawa, K. Kanoda, M. Maesato, and G. Saito, Phys. Rev. Lett. 91, 107001 2003 . ^{2} Z. Hiroi, M. Hanawa, N. Kobayashi, M. Nohara, and H. Takagi, J. Phys. Soc. Jpn. 70, 3377 2001 . ^{3} J. S. Helton, K. Matan, M. P. Shores, E. A. Nytko, B. M. Bartlett, Y. Yoshida, Y. Takano, A. Suslov, Y. Qiu, J.-H. Chung, D. G. Nocera, and Y. S. Lee, Phys. Rev. Lett. 98, 107204 2007 . ^{4} Y. Okamoto, M. Nohara, H. Aruga-Katori, and H. Takagi, Phys. Rev. Lett. 99, 137207 2007 . ^{5} S.-H. Lee, H. Kikuchi, Y. Qiu, B. Lake, Q. Huang, K. Habicht,

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