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# DECORATION OF JOSEPHSON VORTICES BY PANCAKE VORTICES IN Bi2Sr2CaCu2O8+δ.

## I Introduction

In strongly anisotropic high-Tc superconductors, such as $`Bi_2Sr_2CaCu_2O_{8+\delta }`$ (BSCCO), different magnetic flux components are carried by different types of the magnetic vortices: pancake vortices residing in the cuprate planes are responsible for the perpendicular flux component and Josephson vortices centered between the cuprate planes present the in-plane flux . In the first approximation, these two types of vortices are not interacting and form crossing lattices when the external field is not very close to the ab-plane . In this state pancake vortices form a conventional hexagonal lattice which coexists with a stretched hexagonal lattice of Josephson vortices. Due to the large anisotropy $`\gamma `$ ($``$500 for BSCCO) the latter arranges into stacks of Josephson lines with large distances between the stacks along the cuprate planes and $`\gamma `$-times smaller inter-vortex separation in the perpendicular direction. It was predicted that the magnetic flux should lock into the $`ab`$ plane at smaller field angles (to be more precise, if the normal field component is small enough, $`H_z<H_{c1}^c`$) and form a lattice of tilted vortices when the field is far from the plane . However, the experiment revealed a more complicated picture that can not be explained neglecting the interactions between pancakes and Josephson vortices. An account of these interactions results in a rich phase diagram of various vortex states in inclined fields  where crossing lattices present the ground state of the superconductor in a wide range of field angles from orientations close to the $`ab`$ plane to those close to the $`c`$ axis .

Already in the early decoration experiments in BSCCO under inclined fields the formation of vortex rows along the in-plane field has been observed . They were initially treated as chains of tilted vortices in accordance with the theory for the moderately anisotropic superconductors . In such materials, unlike in the isotropic case, currents around vortices tilted from the anisotropy directions redistribute so that a magnetic field changes sign on one side of the tilted vortex at some distance from its axis. This field, although weak, attracts neighboring vortices in the tilt plane thus forming chains of inclined vortices. It turned out, however, that in HTS with a weak Josephson coupling between the cuprate layers the scenario is more intriguing. Calculations showed that pancakes and Josephson vortices coexisting in tilted fields attract each other and as a result pancake stacks decorate Josephson vortex stacks . A similar explanation of the observed vortex chains in BSCCO, although without supporting calculations, was first suggested in . This decoration effect allows to image otherwise invisible (on the $`ab`$ plane) Josephson vortices and study their arrangement and changes in layered superconductors (at least in the range of temperatures where the interaction between the Josephson vortices and pancakes is larger than pinning by defects). Recent vortex imaging using scanning Hall probe microscopy gave direct indication for this scenario and for different phases of the interpenetrating pancake and Josephson vortex systems . Also, formation of pancake vortex chains and enhanced mobility of pancakes along the Josephson vortices have been observed recently by the transmission electron microsopy

In the present study we utilize high-resolution magneto-optical imaging  to investigate the evolution of the coupled pancake (PV) / Josephson (JV) vortex system in dependence on temperature, applied field, and imperfections in single crystal BSCCO plates. It is revealed that PV/JV coupling is relatively strong and results in a joint motion of both vortex types under the direct action on either of them. We show that in addition to chains of pancake vortices on each JV line at small normal fields there can be superstructures with commensurate decoration patterns (each second JV stack occupied by PVs) as suggested in . Also, evidence for formation and motion of “dislocations”and “interconnects” in the Josephson lattice in increasing field is presented. A possibility of transitions between two JV lattice configurations resulting in steps on the field dependence of the JV stack period is discussed. We point out that the spacing of Josephson vortex stacks and their mobility is sensitive to the local density of pancakes and the defect structure in the sample. The latter results in spatial variations of the anisotropy and considerable bending of the JV lines.

## II Experiment and Discussion

The samples studied here were BSCCO single crystals with as grown flat surfaces and straight edges. $`T_c`$ of the samples was $``$ 90K as determined from the disappearance of the magneto-optical contrast at the sample edge. The fields parallel and perpendicular to the sample plane were produced by two separate sets of coils positioned outside the optical cryostat, which allowed varying the field components independently. For imaging the normal component of the magnetic induction on the sample surface the magnetic garnet indicators were used as described in a recent review . The indicator film was placed on a flat sample surface and variations of the normal field, $`B_z`$, were revealed as local changes of the image intensity in the polarized light microscope. The image intensity can be recalculated into magnetic field values using a calibration procedure. At uncrossed microscope polarizers an increased $`B_z`$ is revealed either as brighter or darker color of the image depending on the sign of $`B_z`$. The field resolution of the technique is of the order of a few tens of milliGauss.

Fig. 1 presents a set of images in the middle of a long BSCCO bar (3300$`\times `$850$`\times `$30 $`\mu m^3`$) observed in the increasing in-plane field at 85K. The in-plane field direction is indicated by the arrow. The images show dark lines that appear after the application of a small normal field $`H_z`$ = 2 Oe in the presence of the in-plane field. They represent enhanced values of the local magnetic induction and are the manifestation of Josephson vortex stacks decorated by pancake vortices. In small in-plane fields the decorated Josephson vortices are neither regularly spaced nor parallel to the applied field (Fig. 1 a, b). In Fig.1a there is also evidence for bifurcations of the pattern as discussed in more detail below. Such poor ordering in small in-plane fields is caused by the weak interaction between the distant Josephson vortex stacks. In some regions of the sample only segments of lines were revealed similar to the observations in  where 10 times different density of PVs along the same JVs was referred to transitions in PV states on a JV depending on $`H_z`$. Buzdin and Baladie  showed that PV stacks on a Josephson vortex have a long-range electromagnetic attraction due to their bending by JV currents. This attraction in balance with a short range repulsion provides an equilibrium distance between PV stacks $`a_{eq}2\lambda _{ab}\mathrm{𝑙𝑛}(1/ϵ)`$, with $`ϵ(\lambda _{ab}/\lambda _J)(B_x/H_o)^{1/4}`$ -a parameter characterizing the PV stack bending. Here, $`\lambda _{ab}`$ is the in-plane penetration depth, $`\lambda _J=\gamma s`$ is the JV core size, $`H_o=\mathrm{\Phi }_o/\gamma s^2`$, $`\mathrm{\Phi }_o`$ -the flux quantum, and s is the cuprate layer spacing. Above relation is valid if $`a_{eq}<\lambda _J`$. Note, that the equilibrium separation between PVs on a JV stack is controlled only by the in-plane field $`B_x`$ and this dependence is extremely weak. In small $`H_z`$ the available amount of pancakes is not sufficient to fill all JV stacks with the optimal PV density. In this case pancakes can gather (due to the long range character of attraction) into dense clusters where PVs are separated by $`a_{eq}`$ leaving the other parts of JV empty. This could explain our observations of segments of lines in the decoration patterns if to admit that the access of PVs is restricted in the areas where fragmented JV lines are revealed. In support of such situation we will show below that the inhomogeneous penetration of the normal field is a common feature revealed in all studied BSCCO crystals.

With increasing $`H_x`$ the pattern regularity improves. The PV lines orient along the field, become more periodic, and the period decreases as $`H_x`$ increases (Fig. 1c). At larger $`H_x`$ the MO contrast drops but the regularity of the JV stacks is well revealed at differences of images taken at $`H_z`$ =0 and 2 Oe in the same $`H_x`$ (Fig. 1d). Such a procedure reduces the optical noise and allows to observe much weaker features.

The improvement of the PV line pattern with $`H_x`$ can be explained by increasing the number of PV/JV intersections and the equilibrium density of PV stacks ($`1/a_{eq}`$). As it was calculated in  the intersection of a Josephson vortex and a pancake line produces a negative (attractive) contribution to the energy of both vortices due to the shift of PVs by the Lorentz force of JV currents. The main contribution to the crossing energy $`E_\times `$ comes from pancakes nearest to the JV and is given by

$`E_\times =2.1(\mathrm{\Phi }_o^2/4\pi ^2\gamma ^2s)\mathrm{ln}(3.5\lambda _J/\lambda _{ab})`$ (1)
Clearly the total gain of energy $`\mathrm{\Delta }E_{cr}`$ will increase with the number of intersections $`N1/d`$ where $`d=[2\mathrm{\Phi }_o/\gamma H_x]^{1/2}`$ is the distance between JVs in a stack along the c-axis. Thus the energy gain of the PV line crossing the JV stack compared to the energy of the noncrossing PV line $`E_{pv}=(\mathrm{\Phi }_o/4\pi \lambda _{ab})^2\mathrm{ln}(\lambda _{ab}/\xi _{ab})`$ will be

$`\mathrm{\Delta }E_{cr}/E_{pv}={\displaystyle \frac{8.4(\lambda _{ab}/\lambda _J)^2}{\mathrm{ln}(\lambda _{ab}/\xi _{ab})\mathrm{ln}(3.5\lambda _J/\lambda _{ab})}}(s/d)`$ (2)
(see also ). Taking for BSCCO $`\lambda _{ab}(T=0)=2000\AA `$, $`\xi _{ab}(0)=30\AA `$, $`s=15\AA `$, and $`\gamma =500`$, one gets $`|\mathrm{\Delta }E_{cr}|/E_{pv}=0.055(s/d)`$ at low T.

The energy of the electromagnetic coupling between PV lines at the equilibrium distance $`a_{eq}`$ on a JV stack  normalized to the energy of noninteracting lines gives

$`\mathrm{\Delta }E{\displaystyle \frac{2(s/d)[1/\mathrm{ln}(\lambda _{ab}/\xi _{ab})]}{\left[(\lambda _J/\lambda _{ab})\mathrm{ln}(\lambda _J/\lambda _{ab})\mathrm{ln}[\sqrt{s/d}(\lambda _J/2\lambda _{ab})\mathrm{ln}(\lambda _J/\lambda _{ab})]\right]^2}}`$ (3)
For comparison with $`\mathrm{\Delta }E_{cr}`$(at low T) we write this ratio in a similar form $`|\mathrm{\Delta }E_{em}|/E_{pv}0.0017(s/d)`$ at $`H_x`$=1 Oe and $`0.0039(s/d)`$ at $`H_x`$=100 Oe (the effect of $`(s/d)`$ under the $`\mathrm{ln}`$ is not large). This shows that the major gain of energy due to the decoration of JV stacks by pancakes is provided by $`\mathrm{\Delta }E_{cr}`$ and $`\mathrm{\Delta }E_{em}`$ gives only minor contribution. Formally it is clear from the ratio

$`\mathrm{\Delta }E_{em}/\mathrm{\Delta }E_{cr}{\displaystyle \frac{4(\lambda _{ab}/a_{eq})^2}{\mathrm{ln}(\lambda _J/\lambda _{ab})}}`$ (4)
As follows from the above formulas, the relative contribution of interactions in the PV line energy should strongly increase near $`T_c`$ due to the temperature dependence of $`\lambda _{ab}`$. Both $`E_\times `$ and $`E_{em}`$ are only weakly (logarithmically) dependent on $`\lambda _{ab}`$ and thus on T. However, the reference energy of a noninteracting PV line decreases near $`T_c`$ as $`\lambda _{ab}^2`$, which strongly increases the relative effects of $`E_\times `$ and $`E_{em}`$. Actually, these effects should logarithmically diverge at $`T_d`$=86.5K, where $`\lambda _{ab}(T)=\lambda _{ab}(0)/[1(T/T_c)^2]^{1/2}\lambda _J`$ (here $`T_c`$=90K). However, the theory is developed for $`\lambda _{ab}<\lambda _J`$ and it becomes inapplicable near $`T_d`$. We imaged decorated Josephson stacks in the temperature range from 60 K to 88 K. The patterns were poor at lower T and at T$`>`$87K, and the cleanest patterns were observed around 85 K. This is in accordance with the increasing role of $`E_\times `$ and $`E_{em}`$ at larger temperatures and successive instability of the crossing lattice configuration when $`\lambda _{ab}\lambda _J`$. Note that the MO contrast of the pattern should decrease with temperature due to the decrease of equilibrium decorating PV density $`1/a_{eq}1/\lambda _{ab}`$. Another factor that could facilitate in the formation of optimum pattern at $``$85K is the balance between pinning restricting the mobility of pancakes at lower temperatures and thermal disordering washing out the vortex lattices at higher temperature. We note that in HTS at high T effects of correlated pinning (on extended defects such as twins or columnar defects) become more effective. This would extend the limits of stability of the PV/JV decoration patterns. These patterns (although with a weak contrast and only at larger fields) have been revealed even at T=88K (see Fig.2c,d).

At a given field $`H_x`$ the only parameter controlling the period of the stacks of Josephson vortices is the anisotropy $`\gamma `$. This was used in  for extracting $`\gamma `$ from the decoration patterns observed in relatively small area ($``$25$`\times `$25 $`\mu m`$). Our observations in larger regions ($``$500$`\times `$500 $`\mu m^2`$) revealed that the period can vary across the sample even in high in-plane fields and well developed patterns as is shown in Fig. 2. This effect can have several reasons. First, there can be local changes of the anisotropy associated with compositional and structural variations in the sample. It is typically observed in BSCCO that irregularities of the crystal structure show up at relatively high temperatures due to ”balloons” of increased $`B_z`$ formed at them . We observed that at small normal fields $`B_z`$ inhomogeneities in our samples serve as seeding areas from which PVs spread along the JV stacks. Similar channeling of PVs along JVs was reported in . In the vicinity of the increased $`B_z`$ spots the decoration pattern showed smaller periods at all fields. This can be associated with compositional variations of the anisotropy (e.g. increased oxygen concentration should reduce $`\gamma `$  and thus the period). However, in some areas the difference in period compared to the neighboring regions was found to disappear at increasing field. This could be due to a possibility of two different JV configurations as shown in Fig.3, which have different relations for the stack periods ($`D`$) and distances between JVs in the stack ($`d`$): $`D_1=(\sqrt{3}\gamma \mathrm{\Phi }_o/2H_x)^{1/2}`$, $`d_1=(2\mathrm{\Phi }_o/\sqrt{3}\gamma H_x)^{1/2}`$, and $`D_2=(\gamma \mathrm{\Phi }_o/2\sqrt{3}H_x)^{1/2}`$, $`d_2=(2\sqrt{3}\mathrm{\Phi }_o/\gamma H_x)^{1/2}`$, respectively. Within the anisotropic London model such vortex configurations have the same energy when the field is along the $`ab`$ plane . This degeneracy, however, is lifted and the first configuration becomes preferential when the perpendicular field is applied . In the case of the layered systems in the crossing fields the difference in the energy of the configurations will be due to different number of PV/JV intersections. For one PV line intersecting a JV stack this difference will be $`\mathrm{\Delta }E_{cr}E_\times (1/d_11/d_2`$) which also gives preference to the first configuration ($`d_1<d_2`$). However, this preference is very small. Assuming the equilibrium distances between PV lines on JV stacks the total number of intersections per unit volume in each configuration will be $`N_{cr}1/d1/D1/a_{eq}`$. In this case the difference in the gain due to the crossing energy between them totally disappears ($`d_1D_1=d_2D_2`$). The average value of $`B_z`$ will be slightly different for the two configurations. However, due to the inhomogeneities in the samples tuning of the local $`B_z`$ can be easily realized. Therefore one can expect that these configurations could coexist in the samples and transform from one to another causing changes of the decoration pattern period. In the increasing in-plane field both distances between the stacks, D, and spacing between JVs along the $`c`$-axis, $`d`$, should decrease. For tuning $`D`$ Josephson vortices easily slide along the cuprate planes. However, to tune $`d`$ they have to traverse the planes which requires overcoming a considerable energetic barrier and makes this process much slower. It can be probably done only by formation of double kinks or kinks coming from the edges and their recession along the planes as in the case of dislocations moving from one crystal plane to another . It is reasonable to suggest that the system is not in the equilibrium state at all fields but transforms through a set of metastable states admitting a mixture of the above two possible JV configurations and transitions between them. A whole series of other JV configurations (with different D/d ratios) transforming from one to another in small $`H_x`$ were predicted for the situation when JV vortices can not move along the $`c`$ axis at all . Stepwise transitions between different JV configurations in higher fields were discussed recently in . A possible confirmation of the above scenario is the $`D^2(H_x)`$ dependence shown in Fig. 4. Minimum, maximum and average periods of the decoration pattern plotted on this graph were measured over a large area (500$`\times `$500 $`\mu m^2`$) in the middle of the crystal. The data definitely show a number of steps which can be associated with impeding of the JV system tuning and possibly transitions between different JV lattice configurations. At the same time, the overall changes of the decoration pattern period is well described by a linear dependence $`D^2`$ vs. $`H_x`$ and give reasonable values of the anisotropy from 570 to 700.

Another kind of variation of the pattern period was observed at moderate in-plane fields and at higher temperatures when areas showing the same anisotropy in larger $`H_x`$ unexpectedly reveal periods differing by a factor of two. Fig. 5a, b show such an area where the distance between decorated JV stacks increases with increasing field in contradiction to theory. However, the pattern in nearby areas (Fig. 5c) where the period decreases with increasing $`H_x`$ in a regular way displays half of the period seen in the anomalous areas. This indicates that the large period reveals only each second JV stack. The possibility of the formation of PV chains at integer numbers of JV periods was considered recently by Buzdin and Baladie . They show that the equilibrium density of PV lines decorating JV stack ($`1/a_{eq}`$) is practically field independent (it is a very weak function of $`H_x`$ only). So at low $`B_z`$ there are not enough pancakes to decorate all the JV stacks with this density and a superstructure of decorated and non-decorated stacks develops. With increasing $`B_z`$ the density of chains increases and finally all JV stacks become occupied with PV. In large $`B_z`$ pancakes start spreading into the volume between the JVs. Obviously, in our samples inhomogeneities of the PV concentration caused by crystal imperfections determine the domains where local conditions for superstructures are provided. We already exploited the argument of equilibrium PV spacing to explain the observation of segmented decoration lines. To explain the commensurate periodic patterns one has to account also for the long range repulsion between pancakes on different stacks. This could be due to the Pearl’s interaction  through the stray fields of pancakes at the sample surface. Although these interactions are long range but they are weak and their effect should be noticeable only in favorable conditions. Probably this is the reason why the superstructure was observed only at high temperatures and only in some parts of the sample.

The picture of the field transformations of the JV lattice discussed above suggests that there should be defects in the JV stack arrangement. In particular, we observed interconnects and “dislocations” in the regular decoration line arrays as illustrated in Fig.6. It is known that JV lines do not split or terminate inside a superconductor. Therefore, the decoration pattern reveals the migration of Josephson vortices between different stacks. A corresponding scheme of JV kinks visualized due to PV stacks of different length is shown at the bottom of Fig.6. The kinks can form at different depth from the surface and still they will be decorated by PV stacks if this depth is not too large. On the left scheme two possible variants of JV travelling between the stack is shown but only one of them corresponds to the pattern in Fig.6a. Note, that in either case the kinks in neighboring stacks are located between different cuprate planes. This means that defects in the decoration pattern reveal also defects in ordering of Josephson vortices in the stacks along the c-axis. Comparison of Fig.6b and c shows that JV kinks shift along the direction of $`H_x`$ at changing field. As a result the defects are removed from the decoration pattern at large in-plane fields.

Difference images presented in Figs.6b and c illustrate one more important feature of the JV behavior. The first picture corresponds to the increase of $`H_x`$ by 2 Oe and the second one to the increase of $`H_z`$ by the same 2 Oe. Old positions of JV stacks are revealed as brighter lines and new positions are seen as dark lines (the direction of motion is shown by arrow on the top). It is easy to see that at T$``$85K and $`H_x`$ 25 Oe the change of $`H_z`$ shifts JVs by nearly the same distance as a similar change of $`H_x`$. This is a direct evidence of the strong coupling between the two systems of vortices. It also reveals a possibility to move Josephson vortices either directly acting on them by the in-plane field or by shifting coupled to them pancake vortices by the normal field.

Another illustration of strong interactions between the two components of magnetic flux in BSCCO is the effect of $`B_z`$ inhomogeneities on bending JV stacks. Fig.7a-b presents two successive images taken at increasing $`H_z`$ from 5 to 8 Oe in a sample field cooled to 83K in $`H_x`$ =18.5 Oe. Dark spots on the pictures correspond to increased $`B_z`$ at structural imperfections of the crystal as discussed before. Dark lines are JV stacks decorated by PVs. Upon ramping $`H_z`$ up the increased $`B_z`$ region in the left bottom corner expands and shifts decorated JV stacks considerably bending them. Fig.7c shows that Josephson vortices can also strongly bend during their evolution in the in-plane field when they cross the $`B_z`$ inhomogeneities. This picture presents the difference of images at $`H_x`$ =12 and 14 Oe. A rounded area in the middle of the picture is the spot of increased $`B_z`$. It is not dark because at original images $`B_z`$ in this spot did not change. Here JV lines are not revealed because they did not move at changing $`H_x`$ being pinned by the large density of PVs. The break of angle of the Josephson vortices in this spot is well seen.

In general, the JV stacks in the crossing fields are clearly seen on the background of the inhomogeneous $`B_z`$ distribution as shown on a panoramic MO picture near the corner of a BSCCO crystal in Fig.8. They form an intricate pattern of curved lines (it straightens up at larger $`H_x`$ ) which can be a sensitive tool for studying crystal imperfections and spatial anisotropy variations.

## III Conclusions

We studied magneto-optically the behavior of the decoration of Josepshon vortices by pancake vortices in the single crystals of BSCCO. The decoration pattern turns out to be robust in a wide range of temperatures and fields. Simultaneous imaging of a large area accessible by the MO technique allows to observe interactions of the Josephson vortices with sample imperfections and through the measurements of JV stack periods to map spatial variations of the anisotropy of the sample. The experiment reveals a strong coupling between pancake and Josephson vortices which shows up through the motion of both flux components under the direct action on one of them and pinning and bending of JV lines at the inhomogeneities of the pancake density ($`B_z`$ ). At larger temperatures the quality of the decoration pattern improves which can be referred to (a) the relative increase of the energy of PV/JV interactions compared to the energy of noninteracting pancakes and (b) the increase of the role of correlated pinning of pancakes on the nearly 2D JV stacks. Possible evidences of the coexistence of two different JV lattice configurations are observed. Also intrinsic defects of the JV lattice like “interconnects” and “dislocations” are revealed that are associated with wandering of the Josephson vortices between neighboring stacks. At small fields commensurate patterns with each second JV stack decorated by pancakes are found in accordance with recent theoretical predictions.

## Acknowledgments

The authors thank A. I. Buzdin and S. Bending for stimulating discussions and presentation of his results prior to publication. The work was supported by the U.S.DOE, BES-Materials Sciences, under Contract #W-31-109-ENG-38.


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# Order to disorder transition in the XY-like quantum magnet 𝐂𝐬_𝟐𝐂𝐨𝐂𝐥_𝟒 induced by noncommuting applied fields

## I Introduction

A promising area for the study of zero-temperature quantum phase transitions is that of quantum spin systems in noncommuting applied magnetic fields sachdev99 . Such noncommuting terms introduce quantum fluctuations into the $`T=0`$ ground state which, for large enough fields, can completely disorder the system. Such a situation has been studied in considerable detail in the three-dimensional (3D) Ising ferromagnet LiHoF4 in a transverse magnetic field bitko96 . However, due to its high dimensionality, the system behaves in a mean-field like way. In this paper we consider a one-dimensional (1D) quantum magnet and the effects of a noncommuting field on its ground state.

The scenario that we investigate experimentally is that of the 1D spin-1/2 XXZ model ($`_{XXZ}(\mathrm{\Delta })`$) in a noncommuting field ($`_{APP}`$), given by the Hamiltonian,

$$=_{XXZ}(\mathrm{\Delta })+_{APP},$$
(1)
where,

$$_{XXZ}(\mathrm{\Delta })=J\underset{i}{}\left(S_i^xS_{i+1}^x+S_i^yS_{i+1}^y+\mathrm{\Delta }S_i^zS_{i+1}^z\right)$$
(2)
and

$$_{APP}=\underset{i}{}B^xS_i^x+B^zS_i^z,$$
(3)
and where $`J>0`$ is the antiferromagnetic (AF) exchange constant, and $`\mathrm{\Delta }<1`$ is the anisotropy parameter (a $`g_{x,z}\mu _B`$ factor is incorporated in the magnetic field $`B^{x,z}`$). The operators $`S^\alpha `$, where $`\alpha =x,y,z`$, are the usual spin operators for spin-1/2, and the applied field term does not commute with the exchange Hamiltonian $`[_{XXZ}(\mathrm{\Delta }),_{APP}]0`$ for $`\left|\mathrm{\Delta }\right|1`$ and $`B^x0`$. Indeed, the system we shall study, Cs2CoCl4, is an excellent realization of $`_{XXZ}(\mathrm{\Delta })`$ where $`\mathrm{\Delta }=0.25`$, and therefore should be well approximated by the famous XY model ($`\mathrm{\Delta }=0`$LSM .

The physics of the $`_{XXZ}(\mathrm{\Delta })`$ model at $`\mathrm{\Delta }=0`$ is well known in the absence of a magnetic field i.e. $`B^x=B^z=0`$. It is that of a 1D noninteracting Fermi gas as shown by the Jordan-Wigner transformation Jordan\_Wigner . The effect of a field along $`z`$, $`B^z0`$, (commuting) is trivial; it acts as a chemical potential and changes the filling level of the fermions in the chain inducing magnetization along $`z`$. Below a critical field, $`B_C^z`$, representing the field of complete saturation of the chain, the excitation spectrum remains gapless and the $`T=0`$ correlation functions fall algebraically as power laws. In contrast, the physics for the case of a field along $`x`$, $`B^x0,`$ $`B^z=0`$, is neither trivial nor widely known.

The action of noncommuting field $`B^x`$ on $`_{XXZ}(0)`$ has been considered theoretically by Kurmann et al. Kurmann81 ; Kurmann82 . From these studies it was found that the in-plane field has two effects: 1) it breaks the U(1) symmetry of the XY-model to a lower, Ising-like, symmetry which causes the ground state to long-range order (LRO) at $`T=0`$ into a spin-flop type Néel state. In fact at a special coupling, $`B^x=\sqrt{2}J`$ the spin-flop Néel state is the exact $`T=0`$ ground state. 2) The second effect is to introduce quantum fluctuations into the system. At high fields this causes a phase transition to occur where the fluctuations become large enough to destroy the LRO altogether. This disordering field is below that where the system reaches its saturation point. This phase transition is therefore a nontrivial quantum phase transition through a quantum critical point with the noncommuting field as a control parameter. Fig. 1 shows a schematic outline of the physics of the XY-model in a transverse field.

The theoretical studies Kurmann81 ; Kurmann82  suggest that this behavior is generic to a wide class of magnets in noncommuting fields, and a disordered spin-liquid (S.L.) phase is expected for all $`H_{XXZ}(|\mathrm{\Delta }|1)`$ in equation (1). Spin liquid phases such as this are generally gapped (evidenced by the exponentially decaying correlations in the zero-temperature ground state) and therefore robust against small perturbations. We therefore expect the effects of nonzero $`\mathrm{\Delta }`$ and interchain coupling to modify the transition fields in Fig. 1 but not to change its qualitative content.

In this paper we present a detailed study of the ground state ordering of the quasi-1D XY-like antiferromagnet $`\mathrm{Cs}_2\mathrm{CoCl}_4`$ in noncommuting fields from zero to well above saturation. The crystalline and magnetic properties of $`\mathrm{Cs}_2\mathrm{CoCl}_4`$ and the experimental tool of neutron diffraction will be introduced in Section II.

Section III presents the observed commensurate magnetic structure and its field dependence. The structure is that of magnetic chains which are ordered antiferromagnetically along their lengths with ordered moments lying in the ($`b`$,$`c`$) plane. The experimental results show that an applied field initially further stabilizes the ordered structure (spin-flop phase), but as the field increases fluctuations induced by field noncommutation cause a sharp transition to a new phase which we propose to be the spin-liquid phase discussed above. Study of the ferromagnetic component (III.4) confirms that the saturation field is higher still, and that the proposed spin liquid phase exists in the region $`2.10<H_{SL}<2.52`$ Tesla $``$$`a`$.

An extended discussion of our results is given in Section IV. The observation of commensurate order ($`𝒌`$=(0,1/2,1/2)) in $`\mathrm{Cs}_2\mathrm{CoCl}_4`$ is related to the effective Ising-type interchain coupling (IV.1) and compared with the quasi-elastic results of Yoshizawa et al.Yoshizawa  A microscopic study of the ordering is presented in IV.2 based on a mean-field analysis of the ground-state energy. The magnitude of the ordered moment is established in Section IV.3. Finally, in Section IV.4 the magnetization curve is critically examined and compared with known results for anisotropic spin chains in noncommuting applied fields.

## II Experimental Details

### II.1 Properties of $`\mathrm{𝐂𝐬}_\mathrm{𝟐}\mathrm{𝐂𝐨𝐂𝐥}_\mathrm{𝟒}`$

$`\mathrm{Cs}_2\mathrm{CoCl}_4`$ has been proposed as a spin-1/2 quasi-1D XY-like antiferromagnet with chains running along the $`b`$-direction. Heat-capacity measurementsAlgra  showed a broad maximum (characteristic of low-dimensional systems) around $`T0.9\mathrm{K}`$ and the overall temperature dependence agreed well with numerical predictionsKatsura  for a $`S`$=1/2 XY-like AF chain with exchange coupling $`J=0.23(1)\mathrm{meV}`$. A small lambda-type anomaly observed in the specific-heat at $`T_N=222\mathrm{mK}`$ was interpretedAlgra  as indicating a phase transition to a magnetically ordered phase caused by small couplings between chains. The in-plane magnetic susceptibility McElearney ; Duxbury  also indicated magnetic ordering below $`222\mathrm{mK}`$ and the temperature dependence between $`40\mathrm{mK}`$ and $`4.2\mathrm{K}`$ was in excellent agreement with numerical calculations for AF XXZ chains with $`\mathrm{\Delta }=0.25`$ in Eq 2.

Quasi-elastic neutron scattering experimentsYoshizawa  showed that between $`T=0.3`$ and $`0.6\mathrm{K}`$ the critical scattering of $`\mathrm{Cs}_2\mathrm{CoCl}_4`$ is sheet-like perpendicular to the $`b`$ axis, thus confirming the proposed quasi-1D character of the magnetic properties. Interestingly, the critical scattering is driven partly to incommensurate positions due to competing inter-chain interactions. Those earlier diffraction experiments Yoshizawa  concentrated on the critical scattering at temperatures above the ordering transition of $`0.22\mathrm{K}`$ inferred by macroscopic measurements. As the ordering in this material promises to have some unusual and challenging features, we undertook detailed neutron diffraction experiments to determine the magnetic structure and the behavior in applied noncommuting magnetic fields at temperatures much below the proposed ordering transition of $`0.22\mathrm{K}`$.

$`\mathrm{Cs}_2\mathrm{CoCl}_4`$ crystallizes in the orthorhombic (and nonsymmorphic) space group Pnma ($`D_{2h}^{16}`$, No. 62) Pnam . The crystal structure is shown schematically in Fig. 2. The lattice parameters at 0.3 K areFiggis\_Reynolds ; Yoshizawa  $`a=9.71`$Å , $`b=7.27`$Å and $`c=12.73`$Å. The magnetic ions, Co2+ with spin $`\stackrel{~}{S}=\frac{3}{2}`$, occupy site 4$`c`$ in the unit cell at positionsFiggis\_Reynolds ; Figgis\_Reynolds\_comment

$`(1):(0.235,0.25,0.422)`$
$`(2):(0.735,0.25,0.078)`$
$`(3):(0.765,0.75,0.578)`$
$`(4):(0.265,0.75,0.922)`$ $`.`$
Neighboring spins interact via a superexchange interaction involving a bridge of two Cl--ions with the path Co2+-Cl--Cl--Co2+. The shortest Cl--Cl- distance is between neighbors along the $`b`$-axis separated by $`3.63`$Å. As this is close to twice the ionic radius of Cl a sizeable overlap of electron wave-functions contributing to the exchange integral is expected.

Among other possible exchange paths are $`J_{ac}`$ between sites 1 and 2 ($`d_{\mathrm{Cl}^{}\mathrm{Cl}^{}}`$= 4.05 Å), $`J_{ab}`$ between sites 1 and 3 ($`d_{\mathrm{Cl}^{}\mathrm{Cl}^{}}`$= 4.04 Å), and $`J_{bc}`$ between sites 1 and 4 ($`d_{\mathrm{Cl}^{}\mathrm{Cl}^{}}`$=4.01 Å). Since the overlap of the electronic wave-functions decreases very rapidly (approximately exponentially) with distance, these exchange paths are expected to yield much smaller interactions than the coupling $`J`$ along $`b`$ such that $`\mathrm{Cs}_2\mathrm{CoCl}_4`$ can be regarded as a system of weakly-coupled spin chains along the $`b`$ axis.

Each Co2+ ion is tetrahedrally coordinated by Cl- ligands. Small distortions from a perfect tetrahedron lead to a splitting of the $`\stackrel{~}{S}`$=$`\frac{3}{2}`$ orbital singlet state into two Kramers doublets with a separation $`2D`$=1.3(1) meV. The magnetic exchange energy is much lower than the inter-doublet separation and therefore only the lowest-lying doublet states participate in the low-energy dynamics at low temperatures ($`TD`$). Projecting the Heisenberg exchange between the true spins onto the lowest-lying doublet of $`|\pm \frac{1}{2}`$ states gives an effective spin-1/2 Hamiltonian with XY-like exchange, $`_{XXZ}`$ in Eq. 2 with $`\mathrm{\Delta }`$=0.25.

Rotations of the CoCl4 tetrahedra in the unit cell lead to different orientations of the XY easy plane between sites (1,3) and (2,4) and give the $`b`$-axis as the only common in-plane direction for all sites. The main distortion of the CoCl4 unit from a perfect tetrahedron is due to one of the four Cl- ions being rotated by several degrees around the $`b`$-axis with respect to the central Co2+ ion and previous studiesFiggis  proposed that the normal to the XY easy plane ($`z`$-axis) bisects this large angle. This gives the $`z`$-axis direction ($`\mathrm{sin}\beta `$,0,$`\mathrm{cos}\beta `$) on sites (1,3) and ($`\mathrm{sin}\beta `$,0,$`\mathrm{cos}\beta `$) on sites (2,4) with $`\beta =38.8^{}`$. The shaded rectangular planes in Fig. 2 show the XY planes in this case. Another possibility is that the $`z`$ axis is along the vector connecting the central Co2+ ion with the Cl- ion rotated most and in that case $`\beta `$=+19.4.

### II.2 Experimental method

A high-quality $`6.45\mathrm{g}`$ single crystal of $`\mathrm{Cs}_2\mathrm{CoCl}_4`$ was grown from solution. The crystal was aligned with its $`(0,k,l)`$ plane in the horizontal scattering plane and was cooled to temperatures between $`T=80`$ and $`250\mathrm{mK}`$ using an Oxford Instruments dilution refrigerator insert placed inside a vertical 7 Tesla superconducting magnet.

Neutron diffraction measurements were made at the Hahn-Meitner Institut in Berlin, Germany. The two-axis crystal diffractometer E6 was employed with an incident energy of $`E_i`$=14.72 meV and with a pyrolytic graphite (PG) monochromator in double-focusing mode to increase the neutron flux at the sample position. The scattered neutrons were counted in a 20 wide BF3 detector bank with position sensitivity along the horizontal direction giving 200 channels. This gave an angular resolution of 0.1 in the total scattering angle $`2\mathrm{\Theta }`$. The intensities of nuclear and magnetic Bragg reflections were measured as a function of both $`2\mathrm{\Theta }`$ and the sample rotation angle $`\mathrm{\Psi }`$, thus constructing full two-dimensional (2D) maps of the scattering intensity in the ($`\mathrm{\Psi }`$, $`2\mathrm{\Theta }`$) plane. This allowed simultaneous coverage of both magnetic signal and background. Typical counting times were 5 minutes per 2D map to determine the total integrated intensity, and 40 seconds for a $`2\mathrm{\Theta }`$ scan at the peak center to extract the peak intensity. A two-dimensional Gaussian with adjustable rotation of the main axes of the ellipsoid gave a good account of the observed peak line shapes in both $`\mathrm{\Psi }`$ and $`2\mathrm{\Theta }`$ and the intensities of the Bragg reflections were obtained from least-square fits to the experimental data to reduce the sum of discrepancies $`\chi ^2`$.

## III Experimental results

### III.1 Magnetic order in zero field

Upon cooling below $`T_N`$=217 mK extra Bragg reflections were observed at the commensurate $`(0,n+0.5,m+0.5)`$ reciprocal lattice positions with $`n`$ and $`m`$ integers, indicating a transition to a magnetically long-range ordered state. Fig. 3 shows the temperature dependence of the $`(0,0.5,1.5)`$ AF reflection showing the onset of order below $`T_N`$. The extracted transition temperature $`T_N`$=217 mK is consistent with that inferred from specific-heat and susceptibility measurements.Algra ; Duxbury

The observed magnetic reflections are associated with a magnetic ordering wavevector $`𝒌=(0,1/2,1/2)`$. To determine the magnetic structure we first used group theory to identify the spin configurations consistent with the wavevector $`𝒌`$ for the given crystal symmetry, and second we compared the structure factor of possible spin configurations with the experimentally observed magnetic Bragg peak intensities.

The group theory analysis and determination of the symmetry-allowed basis vectors is presented in Appendix A. After comparison of the data with the possible eigenvectors, we find that the observed structure belongs to the $`\mathrm{\Gamma }^{10}`$ irreducible representation with eigenvector $`\varphi ^{10}`$ given in Eq. V.1. This eigenvector has 6 degrees of freedom corresponding to the three components of the moments $`𝒎_1`$ and $`𝒎_3`$. Using spherical coordinates these can be written as $`𝒎_1=M_1(\mathrm{sin}\vartheta _1,\mathrm{cos}\vartheta _1\mathrm{cos}\varphi _1,\mathrm{cos}\vartheta _1\mathrm{sin}\varphi _1)`$ and $`𝒎_3=M_3(\mathrm{sin}\vartheta _3,\mathrm{cos}\vartheta _3\mathrm{cos}\varphi _3,\mathrm{cos}\vartheta _3\mathrm{sin}\varphi _3)`$. For $`\vartheta _{1,3}=0`$ spins are in the ($`b,c`$) plane and $`\varphi `$ is the azimuthal angle with the $`b`$-axis.

Fig. 4(a) shows a pictorial representation of the $`\varphi ^{10}`$ eigenvector in Eq. V.1 in the special case of ordered spins contained in the ($`b,c`$) plane, making a small angle with the $`b`$-axis ($`\varphi _1=\varphi _3`$) and having equal magnitude on all sites ($`|𝒎_\mathrm{𝟏}|=|𝒎_\mathrm{𝟑}|`$). The structure can be described in terms of antiferromagnetic chains along $`b`$ with a certain ordering pattern between adjacent chains. Starting with the basic structure shown in Fig. 4(a) other distinct domains shown in Fig. 4(b)-(d) can be constructed by changing the sign of either the $`b`$\- or the $`c`$\- spin components, or the relative phase between chains 1 and 3 (for details see Appendix A).

We find that the measured Bragg intensities can be consistently described by an equal population of A and B domains of $`\mathrm{\Gamma }^{10}`$. The best fit of the model to the magnetic intensities (for details see Appendix) is shown in Fig. 5 and in Table 1, and gives a good description of the experimental data. A single-domain structure of either A- or B-type as defined in Appendix A and shown in Fig. 4 is unable to account for the results.

Assuming spin moments confined to the ($`b,c`$) plane ($`\vartheta _1=\vartheta _3=0`$) and equal ordered moments on all sites ($`|𝒎_1|=|𝒎_3|`$) the best fit results are $`\varphi _1=15(5)^{}`$, $`\varphi _3=15(5)^{}`$ and fraction of A-domain $`\alpha =0.48(3)`$ with the sum of discrepancies $`\chi ^2=2.55`$. The obtained value for $`\alpha 1/2`$ demonstrates that domains A and B occupy the sample in equal parts. It will be shown in Section IV.2 that those two domains have the same mean-field exchange energy and are thus expected to occur with the same probability. Taking $`𝒎_1`$ out of the ($`b,c`$) plane by choosing a series of non-zero values for the out-of-plane angle $`\vartheta _1`$ and fitting $`\vartheta _3`$ leads to worse agreement with the observed intensities, so within the accuracy of the experiment it was concluded that magnetic moments are mostly contained in the ($`b,c`$) plane.

Fig. 6 compares the temperature dependence of the reduced intensity $`I/I_{T=80\mathrm{m}\mathrm{K}}`$ of three AF reflections. Here $`I_{T=80\mathrm{m}\mathrm{K}}`$ is the observed intensity at base temperature $`T=80\mathrm{mK}`$. The three reflections have essentially the same temperature dependence, indicating that the magnetic structure is unchanged between 80 mK and $`T_N`$.

### III.2 Magnetic order in applied field

The effect of an applied field on the magnetic order was investigated for fields along $`a`$. A spin-flop phase arises (spins cant out of the ($`b,c`$) plane towards the field axis) evidenced by a perpendicular antiferromagnetic order coexisting with a ferromagnetic moment along the field direction. Fig. 7 shows the field dependence of the $`(0,0.5,1.5)`$ reflection measuring the antiferromagnetic component. The intensity increases with increasing field, reaches a maximum around $`H1.4\mathrm{T}`$ and then it abruptly drops to zero at $`H_c=2.10(4)\mathrm{T}`$ in a sharp, near-first order phase transition. Throughout the spin-flop phase ($`0<H<H_c`$) the ordering wave-vector was constant at the commensurate position $`(0,1/2,1/2`$).

The transition at $`H_c`$ was measured both with increasing and decreasing field, and no measurable hysteresis effect was observed as shown in Fig. 7. At $`3\mathrm{T}`$, no AF or incommensurate reflections were observed along symmetry direction in the ($`b,c`$) plane with an intensity larger than $`1.5\%`$ of the zero-field intensity of the strong $`(0,0.5,1.5)`$ reflection, equivalent to half the average background level. The absence of magnetic Bragg peaks in the ($`b,c`$) plane suggests that the phase immediately above the critical field $`H_c`$ is a disordered phase (no LRO) stabilized by the applied magnetic fields c.f. the disordered SL phase in Fig. 1.

Fig. 8 compares the field dependence of the reduced intensity $`I/I_0`$ of three AF reflections at $`T=80\mathrm{mK}`$, where $`I_0`$ is the zero-field integrated intensity. The field dependence coincides showing that the magnetic structure formed by the antiferromagnetic moments in the $`(b,c)`$ plane is unchanged throughout the spin flop phase up to the critical field $`H_c`$. Furthermore, it shows that the initial increase in the AF Bragg peak intensities is not due to a rearrangement of the moments in a different spin configuration but arises from an increase in the magnitude of the antiferromagnetically ordered moment. This effect is attributed to the suppression of zero-point quantum fluctuations by the applied field which allows more of the available spin moment to order.

The effect of the applied field initially suppressing fluctuations and stabilizing the antiferromagnetic order is even more pronounced at elevated temperatures where the zero-field moment value is further reduced by thermal fluctuations. Fig. 9 shows that the antiferromagnetic moment increases significantly in applied field to reach a maximum around 1.4 T and only at much higher fields it collapses in a sharp transition at $`H_c`$=2.10(4) T (nearly $`T`$-independent up to 195 mK=0.9 $`T_N`$).

Consistent with the above observation, scans in temperature at intermediate fields (below $`H_c`$) observe that the transition temperature is higher than in zero field, as expected for a structure with an increased ordered moment (stabilized by the field) that has a larger mean-field energy and is thus more stable against thermal fluctuations. This is shown in Fig. 10 by measurements of (0,0.5,-1.5) peak intensity in a field of $`H`$=1.9 T. The intensity decreases slower with increasing temperature than in zero field \[see Fig. 3\] and the order is stable beyond the zero-field transition temperature $`T_N`$=217(5) mK and disappears only at a much higher temperatures above the range covered by this experiment, extrapolated to $`T_N(H`$=1.9 T$`)`$ $``$ 300(20) mK. The long-range coherence of the structure is unchanged in the whole measured temperature range as evidenced by the same angular width of $`2\mathrm{\Theta }`$ scans at the two extreme temperatures shown in the inset of Fig. 10.

### III.3 Temperature-field phase diagram

In Fig. 11 we show an ($`Ha`$,$`T`$) phase diagram of $`\mathrm{Cs}_2\mathrm{CoCl}_4`$ based on the measurements described above. At zero field, $`\mathrm{Cs}_2\mathrm{CoCl}_4`$ orders below $`T_N`$=217(5) mK with a commensurate wave-vector $`𝒌=(0,1/2,1/2)`$. The chains are ordered antiferromagnetically along their length and the moments are contained in the ($`b,c`$) plane at a small angle with the $`b`$-axis. Magnetic fields applied along the $`a`$-axis initially stabilize the antiferromagnetic order by suppressing fluctuations. This is directly observed both in the increase of the perpendicular antiferromagnetic moment in applied field (see Figs. 8-9) and also in the increase in the transition temperature at finite field (compare Figs. 3 and 10). At higher fields the order becomes unstable and above $`H_c`$=2.10(4) T$``$ $`a`$ it collapses in a sharp, near-first order transition to a phase with no long-range magnetic order in the ($`b,c`$) plane, possibly a spin-liquid phase. Based on 1) the absence of order in the ($`b,c`$) plane, 2) nonsaturation of the magnetization, see Section III.4, and 3) the expected order-disorder transition driven by the large fluctuations arising from field noncommutation, we identify the phase above the critical field $`H_c`$ with the spin-liquid (S.L.) state predicted to occur below saturation in Fig. 1.

### III.4 Ferromagnetic moment as a function of field

The ferromagnetically-ordered moment was determined from the intensity of the (011) reflection. The resulting magnetization curve at $`T`$=80 mK is shown in Fig. 12. The ferromagnetic moment increases over the whole range of the measurements up to 6.4 T and two regimes can be identified: a low- and a high-field region separated by a cross-over around $`H_m`$=2.52$`\pm `$0.06 T above which the rate of increase of the magnetization is significantly reduced. This cross-over is best illustrated in a plot of the differential susceptibility ($`\chi =M/H`$) in Fig. 13(b) which shows significantly reduced values above $`H_m`$ (of order 4$`\pm `$1 compared to zero field). This cross-over behavior is typical of spin-3/2 systems with two energetically-separated Kramers doublets (for details see Section IV.4): in applied field the lower-lying doublet is saturated first at a field $`H_m`$ above which the magnetization curve shows a large decrease in susceptibility as only higher-doublet states can still be polarized.

The cross-over field $`H_m`$ (defined experimentally as the field where the magnetization is within less than 5$`\%`$ of the linear high-field behavior) is plotted in Fig. 11 (open symbols). Note that the antiferromagnetic order in the ($`b,c`$) plane is suppressed at $`H_c`$=2.10(4) T much below the lower-doublet saturation field identified with $`H_m`$=2.52$`\pm `$0.06 T ($`T`$=80 mK). The absence of long-range order for $`H_c<H<H_m`$ is not due to thermal fluctuations as this field range remains finite after extrapolation to $`T`$=0 as shown in Fig. 11. This region is thus a quantum disordered phase induced by the applied field and is thus consistent with the proposed spin-liquid phase in the schematic phase diagram in Fig. 1.

## IV Discussion

In the previous section we have established the magnetic structure of Cs2CoCl4 and the effects of a noncommuting field on its ground state. Here we discuss relevant microscopic mechanisms that may give rise to the observed ordered structure and find that a simple (nearest neighbor) mean-field picture can not explain all observed features. We then estimate the ordered moment and find a significant reduction from the available moment, indicating the presence of strong quantum fluctuations. Finally, we relate the observed magnetic phase diagram to the minimal model of the XY-chain in a noncommuting field.

### IV.1 Commensurate vs. incommensurate order

The observed ordering wave-vector condenses out of the diffuse scattering measured by Yoshizawa et al.Yoshizawa  in the disordered phase at 0.3 K just above $`T_N`$ (inset of Fig. 5), consistent with the expectation that order should arise at wavevectors where paramagnetic fluctuations are strong. The measured diffuse scatteringYoshizawa  showed systematic incommensurate modulations along the chain direction attributed to competing interchain interactions. In isotropic systems, a mean-field picture for such frustrated couplings would predict incommensurate, spiral spin order along the chains Yoshizawa . The observed order however occurs at the commensurate, antiferromagnetic wavevector $`𝒌`$=(0,1/2,1/2) where interchain frustration effects cancel out and chains behave as decoupled.

In Cs2CoCl4 the tendency to form spiral order is suppressed because XY planes of neighboring chains are not parallel but make a large relative angle 2$`\beta `$ resulting in an Ising-like frustrated interchain coupling between the XY-like 1D chains. Considering only chains 1 and 4 in the chemical unit cell with XY spins the energy of a helical order in the easy planes of the two chains at a pitch to minimize frustration for the $`b`$-axis spin components is $`E_{helix}=S^2[J|\mathrm{cos}2\beta |J_{bc}^2/(2J)]`$. This spiral structure becomes degenerate with the simple AF Néel order (spins along $`b`$) in the limit of orthogonal easy planes $`2\beta `$=90 (close to the actual situation in Cs2CoCl4). In the proximity of this limit of small effective frustration other effects may stabilize the observed commensurate Néel-type order and possibilities include: (1) zero-point quantum fluctuations could introduce non-linear terms in the free-energy expansion which may lift the classical degeneracy and promote ordering at the decoupling point $`𝒌`$=(0,1/2,1/2), (2) further neighbor couplings such as between sites 1 and 5, or 1 and 6, although believed to be small could potentially stabilize the antiferromagnetic order, and (3) other effective Ising-type anisotropies arising from spin-orbit coupling or crystal field effects may favor spin ordering close to the $`b`$-axis with the lowest energy achieved for an antiferromagnetic-type arrangement (constant moment on each site) as opposed to other incommensurate structures. We have also considered dipolar couplings and found an increased energy by 10-5 meV per spin for the observed order compared to a ferromagnetic-type arrangement along the $`c`$-axis and thus it was concluded that dipolar effects could not explain the observed structure.

### IV.2 Mean-field analysis

To identify the exchange couplings involved in stabilizing the observed magnetic structure we calculate its energy in the mean-field approximation. We find simple energetic arguments to explain: 1) why the observed magnetic structure belongs to the $`\mathrm{\Gamma }^{10}`$ irreducible representation, 2) why the ordered moments are confined to the ($`b,c`$) plane and 3) why a multi-domain structure occurs.

We first assume an isotropic Heisenberg exchange such that the three spin components along $`x`$, $`y`$ and $`z`$ ($`a`$-, $`b`$\- and $`c`$-directions) could be treated separately. The observed ordering wave-vector $`𝒌`$=(0,1/2,1/2) indicates a doubling of the unit cell along the $`b`$ and $`c`$ axes leading to 16 different magnetic sublattices in the magnetic unit cell, as shown in Fig. 4(a). Using this extended unit cell we calculated the interaction matrix $`\eta `$ in the mean-field approximation; the eigenvectors of $`\eta `$ are basis vectors of the magnetic ordering and the eigenvalues are the corresponding energy levels. Diagonalization of $`\eta `$ gives the two lowest energy levels $`\lambda _\pm =J\pm J_{ac}`$, assuming weakly-coupled AF chains running along the $`b`$-axis ($`J>0`$ and $`JJ_{ab},J_{ac},J_{bc}`$). For AF exchange between spins 1 and 2 ($`J_{ac}>0`$) the ground state has energy $`\lambda _{}=JJ_{ac}`$ and there are 3 degenerate eigenvectors: (1) ordering of the $`y`$($`b`$) spin components in the irreducible representation $`\mathrm{\Gamma }^{10}`$ (Eq. V.1), (2) ordering of the $`z`$($`c`$)-components also in $`\mathrm{\Gamma }^{10}`$ or (3) ordering of the $`x`$($`a`$)-components in $`\mathrm{\Gamma }^9`$ (Eq. V.1).

Upon including anisotropy effects this three-fold degeneracy is lifted favoring ordering along the $`b`$-axis ($`b`$ is a common easy axis for all spins as shown by paramagnetic susceptibility measurementsDuxbury ; Pnam ). The determined magnetic structure shown in Fig. 4 is indeed in the $`\mathrm{\Gamma }^{10}`$ representation with the largest spin moment along the easy $`b`$-axis and a small moment along $`c`$, also in $`\mathrm{\Gamma }^{10}`$. The observed confinement of the ordered moments to the ($`b,c`$) plane can also be understood on energetic grounds: according to Eq. V.1 ordering of spins along $`a`$ in $`\mathrm{\Gamma }^{10}`$ would have parallel spins on sites 1 and 2, which would be energetically unfavored by the AF interchain couplings $`J_{ac}`$ (the ordering of the $`a`$ components can not belong to another representation, say $`\mathrm{\Gamma }^9`$, because the full Hamiltonian including all anisotropy terms respects the symmetry of the crystal structure and therefore does not mix spin orderings from different irreducible representations).

For a magnetic ordering of the $`b`$ and $`c`$ spin components in the $`\mathrm{\Gamma }^{10}`$ representation the spin configuration is not unique, but instead four distinct domains are possible, all with the same mean-field exchange energy. Those four domains are shown in Fig. 4 and the degeneracy arises because the $`\mathrm{\Gamma }^{10}`$ representation of the $`b`$ and $`c`$ components is two-dimensional (sites 1 and 3 and independent).

Interestingly, at the mean-field level the ground-state energy does not depend on the couplings between sublattices (1,2) and (3,4). This is a general result for any antiferromagnetic ordering along $`b`$, i.e. $`𝒌`$=(0,1/2,$`l`$) as can be easily seen by inspecting Fig. 4(a): each spin on the second group of sublattices interacts with pairs of antiparallel spins from the first group such that the net interactions cancel out. For example, spin 4 interacts through $`J_{bc}`$ with the pair of antiparallel spins 1 and 9 (5 and 13). Similarly, spin 4 at $`x`$$``$ 0.25 interacts through $`J_{ab}^{}`$ with the pair of antiparallel spins 6 and 14 at $`x`$$``$0.75 ($`J_{ab}`$ with antiparallel spins type 6 and 14 at $`x`$$``$$`0.25`$).

The observed ordering at $`𝒌`$=(0,1/2,1/2) thus consists of two interpenetrating magnetic lattices that are non-interacting at the mean-field level. One lattice containing atoms $`1,\mathrm{\hspace{0.17em}2},\mathrm{\hspace{0.17em}5},\mathrm{\hspace{0.17em}6},\mathrm{\hspace{0.17em}9},\mathrm{\hspace{0.17em}10},\mathrm{\hspace{0.17em}13},\mathrm{\hspace{0.17em}14}`$, and the other has atoms $`3,\mathrm{\hspace{0.17em}4},\mathrm{\hspace{0.17em}7},\mathrm{\hspace{0.17em}8},\mathrm{\hspace{0.17em}11},\mathrm{\hspace{0.17em}12},\mathrm{\hspace{0.17em}15},\mathrm{\hspace{0.17em}16}`$ in the magnetic unit cell. Since those two global lattices are related by inversion symmetry ($`\overline{1}`$ at the center of the chemical unit cell) the intra-sublattice interactions are identical and so the ordered magnetic moment is expected to be the same for both, as assumed in the analysis of the magnetic Bragg peaks in Section III that gave good agreement with the experiment.

The observed small alternating tilt $`\varphi =\pm `$15(5) of the magnetic moments away from the $`b`$-axis indicates an effective local spin anisotropy. We do not have an explanation for its origin but propose that it may arise when the Heisenberg interchain exchange between sites with rotated XY planes (such as $`J_{ac}`$ between spins 1 and 2 in Fig. 2) is projected onto the lower-lying Kramers doublet of effective spin-1/2.

### IV.3 Absolute magnitude of the ordered moment

The magnitude of the ordered moment at $`T=80\mathrm{mK}`$ was determined by comparing the nuclear and the AF Bragg peak intensities (see Appendix C). Using $`A_{\mathrm{exp}}`$ and Eq. 11 the resulting ordered moment at $`T=80\mathrm{mK}`$ is $`m_0=1.7(4)\mu _B`$ (zero field).

The lower-lying Kramers doublet of Co2+ ions with effective spin-1/2 has anisotropic $`g`$-values, $`g_{x,y}=2g`$ and $`g_z=g`$. Here $`g`$=2.4 is the isotropic $`g`$-value of the underlying spin-3/2 and was determined from high-temperature paramagnetic susceptibility measurements Smit ; McElearney ; Figgis . This implies that the available moment in the XY plane is $`g_{x,y}\mu _B/2`$=2.4 $`\mu _B`$. From the present diffraction experiments the estimated ordered moment along the in-plane axis $`b`$ common to all spins is $`m_0\mathrm{cos}\varphi `$=1.6(4) $`\mu _B`$, clearly smaller than the available full moment in the XY plane (the ordered moment along the $`c`$-axis is very small and is a mixture between longitudinal and transverse parts). The reduction of the ordered moment from the full available value indicates strong zero-point fluctuations in the ground state.

### IV.4 Magnetization curve

In this section we consider a minimal magnetic Hamiltonian consistent with the crystal field and magnetization data on Cs2CoCl4 and relate the observed magnetic phase diagram to the phenomenology of anisotropic magnets in noncommuting fields. We analyze the magnetization curve in terms of a spin-3/2 Hamiltonian appropriate for the Co2+ ions and identify the observed crossover at $`H_m`$ with near-saturation of the lower-lying spin doublet. We then estimate the lower-doublet magnetization curve (Fig. 14) and discuss it in terms of an effective $`S`$=1/2 XXZ Hamiltonian in noncommuting field.

#### IV.4.1 Full Hamiltonian

A minimal Hamiltonian for the spin $`\stackrel{~}{S}`$=3/2 Co2+ ions that includes the 1D exchange and crystal field effects is

$$\stackrel{~}{}=\underset{i}{}I\stackrel{~}{𝑺}_i\stackrel{~}{𝑺}_{i+1}+D\left(\stackrel{~}{S}_i^z\right)^2g\mu _BH_z\stackrel{~}{S}_i^zg\mu _BH_x\stackrel{~}{S}_i^x,$$
(4)
where $`I`$ is the nearest-neighbor (isotropic) exchange interaction along the 1D chains and $`D`$ is the easy-plane anisotropy energy (perpendicular to the local $`z`$-axis). The last two terms in Eq. 4 are the Zeeman energy in longitudinal ($`H_z=H\mathrm{sin}\beta `$) and transverse ($`H_z=H\mathrm{sin}\beta `$) fields, where $`\beta `$ is the angle between the field direction and the XY plane (for $`H`$$``$$`a`$ this is equal to the angle between the local $`z`$-axis and the $`c`$-axis in Fig. 2).

In the absence of magnetic fields ($`H=0`$) and in the limit of large local anisotropy ($`DI`$) only the lower-lying doublet $`|\pm \frac{1}{2}`$ contributes to the low-energy dynamics and in this subspace the degrees of freedom can be describedAlgra  by an effective spin $`S`$=1/2 XXZ Hamiltonian (Eq. 2) with exchange $`J=4I`$ and anisotropy parameter $`\mathrm{\Delta }`$=0.25.

#### IV.4.2 XXZ chain in a longitudinal (commuting) field

The physics of the XXZ model (Eq. 2) is well understood in the limit $`\mathrm{\Delta }`$=0 when it is equivalent to a 1D free fermion gas. Longitudinal fields ($`Hz`$) act as chemical potential filling up the quasiparticle band. The magnetization is directly related to the filling factor and at finite temperature $`T`$ is given by Katsura

$$M(H,T)=\frac{M_{1z}}{\pi }_0^\pi 𝑑\omega \mathrm{tanh}\frac{g_z\mu _B(HH_{1z}\mathrm{cos}\omega )}{2k_BT},$$
(5)
with the $`T`$=0 result $`M(H)=2M_{1z}\mathrm{sin}^1\left(H/H_{1z}\right)/\pi `$, $`HH_{1z}`$. Fig. 14 shows a typical magnetization curve plot at $`T`$=0 (dashed curve) and finite $`T`$ (solid line) where the approach to saturation is rounded off by thermal fluctuations. The saturation magnetization $`M_{1z}=g_z\mu _B/2`$ (per spin) is reached at the critical field (for finite $`\mathrm{\Delta }`$) $`H_{1z}=J(1+\mathrm{\Delta })/g_z\mu _B`$. The zero-field, $`T=0`$ longitudinal susceptibility is reduced compared to the semi-classical value due to quantum fluctuations and for $`\mathrm{\Delta }`$=0.25 is calculated as Muller84  $`\chi _z(0)`$$``$0.237$`g_z^2\mu _B^2/J`$. Using the proposed values for the exchange interactions in Cs2CoCl4, $`J`$=0.23(1) meV, $`g_z`$=2.4 the longitudinal critical field is estimated as $`H_{1z}`$=2.1(1) T.

#### IV.4.3 XXZ chain in a transverse (noncommuting) field

Transverse fields ($`H||x`$) have a very different effect compared to longitudinal fields because they : (1) break the spin rotational symmetry from U(1) to Ising, and (2) do not commute with the exchange terms. In low fields this produces perpendicular long-range antiferromagnetic order (spin-flop phase) Kurmann81 ; Kurmann82 . The non-commutation of the field introduces fluctuations that become strong enough above a critical field to suppress the antiferromagnetic order and induce a transition to a spin liquid state where the spin moment is not yet saturated along the field and the finite perpendicular spin components have exponentially-decaying correlations. A typical ground state phase diagram is shown in Fig. 1. The critical disordering field is estimated Kurmann82  at $`H_{1x}^{}J(3+\mathrm{\Delta })/2g_x\mu _B`$ whereas exact diagonalizations of finite chainsKurmann81  suggest that near-saturation of the magnetization occurs at much higher fields, similar to the classical saturation value $`H_{1x}=2J/g_x\mu _B`$. For Cs2CoCl4 those estimates give $`H_{1x}^{}`$ $``$1.3(1) T and $`H_{1x}`$=1.7(1) T. The zero-field, $`T=0`$ susceptibility is again reduced compared to the semiclassical value due to quantum fluctuations and for the XY chain is calculated as Muller84  $`\chi _x(0)0.075g_x^2\mu _B^2/J`$.

#### IV.4.4 Full Hamiltonian in a longitudinal field

For the $`\stackrel{~}{S}`$=3/2 Hamiltonian in Eq. 4 with well-separated energy scales for the lower $`|\pm \frac{1}{2}`$ and higher $`|\pm \frac{3}{2}`$ doublets a cross-over in behavior is expected in applied magnetic field from a low-field region where only the lower doublet participates (or both doublets depending on the field direction) to a higher field region where the lower doublet is saturated and only the higher-doublet contributes to the magnetization.

Longitudinal fields ($`Hz`$) do not mix higher-doublet states until very large fields of the order the inter-doublet separation energy $`H_{2z}2D/g_z\mu _B`$. At low fields only the lower-doublet states contribute and the physics is that of the XXZ model in longitudinal fields. Above the lower-doublet saturation at $`H_{1z}`$ the magnetization shows a plateaux at $`M_{1z}=g_z\mu _B/2`$ (per spin) stable up to fields around $`H_{2z}`$ when the magnetization increases again by mixing in states from the higher-lying doublet $`|\pm \frac{3}{2}`$ to finally reach the full spin value of $`3/2g\mu _B`$. The upper longitudinal critical field for Cs2CoCl4 is estimated at $`H_{2z}`$=9(1) T.

#### IV.4.5 Full Hamiltonian in a transverse field

Transverse fields ($`H`$ $``$ $`x`$) in Eq. 4 have finite matrix elements between the two doublets and thus mix higher-doublet states into the ground state (of order $`g\mu _BH/2D`$) at any finite field.Smit  Both doublets participate at low fields (large susceptibility) and above a cross-over field the lower doublet is near saturated and only the higher doublet contributes (small susceptibility). Such a behavior is evident in earlier magnetization measurementsSmit ; Pnam  on Cs2CoCl4 in fields along the $`b`$-axis (entirely transverse) where the magnetization increases rapidly at low fields with a large susceptibility then crosses over above $``$3 T to a region where the magnetization increases much slower to approach saturation (3.6 $`\mu _B`$) at fields $`>`$16 T.

#### IV.4.6 Comparison with the observed (total) magnetization

The $`a`$-axis magnetization shown in Fig. 12 is in broad agreement with the expected behavior for mixed longitudinal and transverse fields on the full $`\stackrel{~}{S}`$=3/2 Hamiltonian in Eq. 4: a rapid increase is observed at small fields (both doublets contribute) followed by a cross-over to a much slower increase at higher fields (only higher-doublet states contribute). The cross-over field $`H_m`$=2.52$`\pm `$0.06 T ($`T`$=80 mK) is identified with near-saturation of the lower doublet. This field appears to be larger than the estimated near- or full-saturation fields for purely transverse $`H_{1x}`$ or purely longitudinal fields $`H_{1z}`$, possibly due to either the approximations used in estimating $`H_{1x}`$ solving Eq. 4 assuming decoupled lower and higher doublets, or other terms in the Hamiltonian, such as interchain exchanges not included explicitly here.

Fig. 14 shows the partial lower-doublet magnetization assuming the contribution to the magnetization from the higher doublet states can be approximated by a constant susceptibility (as shown in Fig. 12). This assumption is consistent with calculations in the single-site approximation following Ref. Smit, , which predict that the higher-doublet susceptibility for fields tilted at $`\beta `$=45 is relatively small (compared to $`\chi _{x,z}(0)`$ of the lower doublet) and decreases smoothly by only $``$25$`\%`$ between zero and 5 T. Putting the magnetization values in Fig. 14 on an absolute scale gives a lower-doublet saturation moment $`M_s`$=1.7(4) $`\mu _B`$, consistent with typical values expected for fields applied at an angle to the $`z`$-axis $`M_s=\sqrt{g_x^2\mathrm{cos}^2\beta +g_z^2\mathrm{sin}^2\beta }\mu _B/2`$1.9 $`\mu _B`$ for $`\beta `$=45.

#### IV.4.7 (Partial) magnetization of the XXZ chain

Since no detailed predictions are available for the magnetization curve of XXZ chains in mixed longitudinal and transverse fields we compare the results with the generic analytic form given in Eq. 5. This is valid strictly only for XY chains in longitudinal fields, but it provides a simple analytic form to parametrize the data and extract an effective saturation field $`H_s`$, the saturation magnetization and an effective “temperature” $`\stackrel{~}{T}`$, which is a measure of the fluctuations causing the rounded approach to saturation.

The extracted saturation field $`H_s`$=2.37(3) T (80 mK$`<`$$`T`$$`<`$ 250 mK) is significantly larger than the critical field $`H_c`$=2.10(4) T where the antiferromagnetic order disappears, giving further support for the existence of an intermediate phase between the antiferromagnetic order and the nearly fully-polarized phase as indicated in the phase diagram in Fig. 11. The fitted “temperatures” $`\stackrel{~}{T}`$ are systematically larger than the true measuring temperatures $`T`$ ($`\stackrel{~}{T}`$=200(50) mK for the $`T`$=80 mK data, fit shown by solid line in Fig. 14) indicating more fluctuations in the system than can be accounted for by temperature alone. A source of those fluctuations can be the noncommuting fields that create disorder effects at large fields. At small noncommuting fields the dominant effect is breaking the spin rotational symmetry which has the consequence of promoting long-range order in a spin-flop phase. This is also in agreement with the experiments, which observed that low fields stabilize the perpendicular antiferromagnetic order.

### IV.5 Further studies

The measurements presented here have highlighted a potentially very significant field induced phase transition in Cs2CoCl4. The field dependence of the order correlates well with the expectations of a quantum magnet driven through a quantum critical point by a noncommuting field. Essential to this picture is the identification of the disordered phase with a gapped spin liquid state. Further studies using NMR, magnetic susceptibility, and heat capacity are called for to investigate whether a spin gap really does open above the critical field of 2.10 T. It would also be very interesting to look for any evidence of spin glass behavior induced by the field. Inelastic neutron scattering measurements of the excitations in a field should be particularly revealing and we plan to make such measurements in the near future.

## V Conclusions

In conclusion, single-crystal neutron diffraction was used to determine the magnetic ordering as a function of noncommuting applied field in the quasi-1D spin-1/2 XY-like antiferromagnet Cs2CoCl4. In zero field long-range order with wavevector $`𝒌`$=(0,1/2,1/2) was found below $`T_N`$=217(5) mK. The magnetic structure was determined using group theory and has spins ordered antiferromagnetically along the chains with moments confined to the ($`b,c`$) plane. A domain structure was found with adjacent chains in different phases. Possible mechanisms promoting this commensurate order were discussed. The observed reduction in the ordered moment was attributed to zero-point fluctuations in the ground state.

Magnetic fields applied along the $`a`$-axis were found to initially stabilize the perpendicular AF order and form a spin-flop phase. This structure becomes unstable at high fields where a transition occurs to a phase with no LRO in the ($`b,c`$) plane. Measurements of the ferromagnetic component found that near-saturation of the moments occurs only at much higher fields. The phase in-between the spin-flop and saturated phases $`2.10<H_{SL}<2.52`$ T $``$ $`a`$ has been proposed to be a spin liquid state disordered by the strong quantum fluctuations arising from the applied field noncommutability with the exchange Hamiltonian.

###### Acknowledgements.

We would like to thank R. A. Cowley, F. H. L. Essler and M. Meissner for stimulating discussions. Preliminary work for the characterization of single crystals was performed at Chalk River Laboratories in Canada. Financial support for the experiments was provided by the EPSRC and by the EU through the Human Potential Programme under IHP-ARI contract HPRI-CT-1999-00020. ORNL is managed for the U.S. D.O.E. by UT-Battelle, LLC, under Contract No. DE-AC05-00OR22725. One of the authors (M.K.) was supported by the Swiss National Science Foundation under Contract No. 83EU-053223.

## Appendix

### V.1 Group theory analysis

Using the space group symmetry of the crystal structure we identify allowed basis vectors for a magnetic structure with the observed wavevector $`𝒌`$=(0,1/2,1/2). This is done by determining the irreducible representations and eigenvectors of the little group $`G_𝒌`$ of symmetry operations that leave the wavevector $`𝒌`$ invariant.

We start by considering the symmetry elements of the Pnma space group of $`\mathrm{Cs}_2\mathrm{CoCl}_4`$:

$$\{1,\overline{1},\mathrm{\hspace{0.33em}2}_x,\mathrm{\hspace{0.33em}2}_y,\mathrm{\hspace{0.33em}2}_z,m_{xy},m_{xz},m_{yz}\},$$
(6)
where $`1`$ is the identity operator, $`\overline{1}`$ is the inversion at the origin, $`2_\alpha `$ denotes a 180 screw axis along direction $`\alpha =x,y`$ or $`z`$ (180 rotation followed by a translation with half a unit cell along axis $`\alpha `$) and where throughout this group-theory section the axes $`x`$, $`y`$ and $`z`$ refer to the crystallographic directions $`a`$, $`b`$ and $`c`$. $`m_{\alpha \beta }`$ is a glide plane containing axes $`\alpha `$ and $`\beta `$. The group is nonsymmorphic because the group elements $`\{R|𝒂\}`$ consist of an operation $`R`$ followed by a translation $`𝒂`$ equal to half a direct lattice vector. The experimentally observed ordering wave-vector $`𝒌=(0,1/2,1/2)`$ is invariant under all these operations such that the little group $`G_𝒌`$ contains all of the above elements.

The representations of the little group $`G_𝒌`$ are given by $`\mathrm{exp}(i𝒌𝒂)\mathrm{\Gamma }^\alpha (R_𝒌)`$. The ordering in $`\mathrm{Cs}_2\mathrm{CoCl}_4`$ is a special case because the crystal symmetry is nonsymmorphic and the ordering wave-vector lies on the Brillouin zone boundary. The representations of elements $`R_𝒌`$ of the space group with subsequent translation $`𝒕=(0,n,m)`$ such that $`n+m=\mathrm{odd}`$ have a different sign to those of operations $`R_𝒌`$ alone, and this leads to additional irreducible representations. They can be found by adding new group elements to the little group $`G_𝒌`$,Heine  which are the original elements with an additional translation $`𝒕`$. We call the additional translations

$$\{1^t,\overline{1}^t,\mathrm{\hspace{0.33em}2}_x^t,\mathrm{\hspace{0.33em}2}_y^t,\mathrm{\hspace{0.33em}2}_z^t,m_{xy}^t,m_{xz}^t,m_{yz}^t\}.$$
(7)
Thus the little group $`G_𝒌`$ consists of a total of $`16`$ elements. We determined the classes and the character table of this group and these are shown in Table 2. The group consists of $`10`$ different classes and therefore has $`10`$ irreducible representations. Only two of the representations fulfill the necessary condition that $`\chi (1)=\chi (\overline{1}^t)`$ (this condition follows directly from the prefactor of the representation which changes sign under a translation by $`𝒕`$). The experimentally observed ordered magnetic structure is thus associated with one of these two representations.

The eigenvectors $`\varphi ^\lambda `$ of the irreducible representations $`\mathrm{\Gamma }^\lambda `$ were determined using the projector method.Heine  They are given by

$$\varphi ^\lambda =\underset{g}{}\chi ^\lambda (g)g(\varphi ),\lambda =1\mathrm{}10,$$
(8)
where $`g`$ is an element of the little group and $`\varphi `$ is any vector of the order parameter space. For $`𝒌`$=(0,0.5,0.5) the magnetic unit cell is doubled along the $`b`$ and $`c`$ axes, and the order parameter space is a $`48`$-dimensional axial vector because the magnetic unit cell contains $`16`$ magnetic moments as indicated in Fig. 4)(a) and each has three space components. We obtain

$`\varphi ^9=(m_{1x},m_{1y},m_{1z},m_{1x},m_{1y},m_{1z},`$
$`m_{3x},m_{3y},m_{3z},m_{3x},m_{3y},m_{3z},`$
$`𝒎_1,𝒎_2,𝒎_3,𝒎_4,`$
$`𝒎_1,𝒎_2,𝒎_3,𝒎_4,`$
$`𝒎_1,𝒎_2,𝒎_3,𝒎_4)`$ (9)
for representation $`\mathrm{\Gamma }^9`$. $`m_{i\alpha }`$ is the component $`\alpha `$ of the magnetic moment $`i`$ with $`1i16`$. For better readability, in the above equation the individual components of the magnetic moments 5 to 16 were omitted and the magnetic moments were written as vectors, i.e. $`𝒎_5=𝒎_1=(m_{1x},m_{1y},m_{1z})`$. For representation $`\mathrm{\Gamma }^{10}`$ we obtain

$`\varphi ^{10}=(m_{1x},m_{1y},m_{1z},m_{1x},m_{1y},m_{1z},`$
$`m_{3x},m_{3y},m_{3z},m_{3x},m_{3y},m_{3z},`$
$`𝒎_1,𝒎_2,𝒎_3,𝒎_4,`$
$`𝒎_1,𝒎_2,𝒎_3,𝒎_4,`$
$`𝒎_1,𝒎_2,𝒎_3,𝒎_4).`$ (10)
The ordered magnetic structure is thus doubly degenerate in each of the three spin components given by the dimension 2 of these two representations.

A magnetic structure in the $`\mathrm{\Gamma }^{10}`$ irreducible representation can occur in several different domains. Assume spins are confined to the ($`b,c`$) plane in a typical configuration shown in Fig.4(a) called domain A1. One can construct domain A2 in Fig.4(c) by reversing the $`b`$($`y`$)-components of all spins and keeping the $`c`$($`z`$)-components unchanged. Domain B1 in Fig.4(b) is obtained from domain A1 by reversing the spins on sites 3, 4 (and 7, 8, 11, 12, 15, 16) and using the same rule one transforms domain A2 in Fig.4(c) into B2 in Fig.4(d). Domains A1 and A2 are indistinguishable from each other in a neutron scattering experiment because they have the same magnetic structure factor and domains B1 and B2 are also indistinguishable. However, an A-type domain (either A1 or A2) has a different structure factor from a B-type (either B1 or B2) domain.

### V.2 Zero-field magnetic structure

The integrated intensity of magnetic Bragg peaks is related to the structure factor of the magnetic ordering through Squires

$$I(𝑸)=\left(\frac{\gamma r_0}{2\mu _B}\right)^2N_m\frac{(2\pi )^3}{V_{m0}}\mathrm{\Phi }\frac{|f(𝑸)|^2}{\mathrm{sin}(2\mathrm{\Theta })}|𝑭_{}(𝑸)|^2,$$
(11)
where $`f(𝑸)`$ is the magnetic form factor for Co2+ ions IntTables . $`\mathrm{\Phi }`$ is the flux of incident neutrons, $`N_m`$ and $`V_{m0}`$ are the number and the volume of the magnetic unit cells, $`\gamma =1.913`$ and $`r_0=2.81810^{15}\mathrm{m}`$. $`I(𝑸)`$ is the total integrated intensity of a Bragg reflection measured in the ($`\mathrm{\Psi }`$,$`2\mathrm{\Theta }`$) plane and $`1/\mathrm{sin}(2\mathrm{\Theta })`$ is the Lorentz correction factor that arises because intensity is measured as a function of angular coordinates. $`𝑭_{}(𝑸)`$ is the component of the magnetic structure factor perpendicular to the scattering wave vector and is defined as

$$𝑭_{}(𝑸)=𝑭(𝑸)(𝑭(𝑸)\widehat{𝑸})\widehat{𝑸},$$
(12)
where $`\widehat{𝑸}`$ is the normalized wave-vector transfer.

The magnetic structure factor is defined as

$$𝑭(𝑸)=\underset{i=1}{\overset{16}{}}𝒎_i\mathrm{exp}(\mathrm{i}𝑸𝒅_i)$$
(13)
where $`𝑸`$ is the wave-vector transfer in the experiment, $`𝒅_i`$ are the positions of the Co2+-ions and the sum is over all $`16`$ magnetic ions in the magnetic unit cell. For a two-domain structure (A + B type) the magnetic Bragg peak intensity can be written as

$$𝑰(𝑸)=\alpha 𝑰_A(𝑸)+(1\alpha )𝑰_B(𝑸),$$
(14)
where $`\alpha `$ is the population of the A-domain and $`(1\alpha )`$ is the population of the B-domain.

### V.3 Absolute magnitude of the ordered moment

The magnitude of the ordered moment at $`T=80\mathrm{mK}`$ was determined by comparing the nuclear and the AF Bragg peak intensities. The intensity of a nuclear Bragg peak is given as

$$I(𝑸)=N\frac{(2\pi )^3}{V_0}\mathrm{\Phi }\frac{|F_N(𝑸)|^2}{\mathrm{sin}(2\mathrm{\Theta })},$$
(15)
where $`N`$ and $`V_0`$ are the number and the volume of the unit cells. $`F_N(𝑸)`$ is the nuclear structure factor and given asSquires

$$F_N(𝑸)=\underset{i}{}b_i\mathrm{exp}(\mathrm{i}𝑸𝒅_i),$$
(16)
where the sum runs over all elements in the nuclear unit cell and $`b_i`$ is the elastic scattering lengthIntTables  of atom $`i`$ in the unit cell. The nuclear peaks used for calibration were (02$`\overline{2}`$), (033), (022) and (03$`\overline{3}`$) and their observed relative integrated intensities were consistent with the calculated structure factors to within 15$`\%`$. Multiple scattering and extinction corrections were assumed to be negligible. The measured nuclear intensities gave the overall scale factor for the intensities $`A_{\mathrm{exp}}=N\frac{(2\pi )^3}{V_0}\mathrm{\Phi }`$ in Eq 15. The magnitude of the ordered magnetic moment was determined using $`A_{\mathrm{exp}}`$ and Eq. 11. The resulting ordered moment at $`T=80\mathrm{mK}`$ in zero field is $`m_0=1.7(4)\mu _B`$.