Abstract
Antiferromagnetic materials can host spinwaves with polarizations ranging from circular to linear depending on their magnetic anisotropies. Until now, only easyaxis anisotropy antiferromagnets with circularly polarized spinwaves were reported to carry spininformation over long distances of micrometers. In this article, we report longdistance spintransport in the easyplane canted antiferromagnetic phase of hematite and at room temperature, where the linearly polarized magnons are not intuitively expected to carry spin. We demonstrate that the spintransport signal decreases continuously through the easyaxis to easyplane Morin transition, and persists in the easyplane phase through current induced pairs of linearly polarized magnons with dephasing lengths in the micrometer range. We explain the long transport distance as a result of the low magnetic damping, which we measure to be ≤ 10^{−5} as in the best ferromagnets. All of this together demonstrates that longdistance transport can be achieved across a range of anisotropies and temperatures, up to room temperature, highlighting the promising potential of this insulating antiferromagnet for magnonbased devices.
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Introduction
The ultrafast magnetization dynamics of antiferromagnets (AFMs) are complex due to the multiple sublattices involved, and have so far been studied mostly by neutron scattering experiments^{1,2}. The development of THz spectroscopy combined with the burgeoning field of antiferromagnetic spintronics^{3,4} has recently generated exciting predictions and first results on the potential exotic dynamics of antiferromagnetic magnons have emerged. Antiferromagnetic magnons can exhibit the full range of circular to linear polarization in collinear antiferromagnets^{5}, and a finite magnon Hall angle is predicted in chiral antiferromagnets^{6}. Theoretical work has also predicted the interaction between antiferromagnetic magnons and spintextures^{7,8}, by respective changes of their polarization and of the local Néel order. Ballistic^{9}, diffusive^{10} and spinsuperfluid regimes through magnon condensation^{11,12} have been predicted, and electrical signatures by spin–orbit coupling effects are expected^{13,14,15}.
Experimental observations of these rich physics have started to emerge, with recent reports of longdistance spintransport near room temperature in the easyaxis phase of hematite^{8,16} and at low temperatures in antiferromagnetic quantum Hall graphene^{17}. However, the complex spintransport features in collinear antiferromagnets are generally not indicative of the coherent transport regime although signatures have recently been claimed^{18}. Furthermore, while the transport in easyaxis AFMs that is expected from the circular polarization of the magnons has been clearly observed^{16}, the possibility to propagate longdistance spincurrents in the widespread class of collinear easyplane antiferromagnets remains an open question in the emerging field of antiferromagnetic magnonics^{10}. Finally, achieving longdistance room temperature spintransport has not been achieved yet which is a prerequisite to integrate antiferromagnets in spintronic and magnonic devices.
Hematite, αFe_{2}O_{3}, is a model system to investigate the spintransport regime of easyaxis antiferromagnets as we recently reported^{8,16} but the easyaxis phase is only present at low temperatures. Above the Morin temperature (T_{Morin} = 260 K), undoped hematite single crystals undergo a transition from an easyaxis to an easyplane AFM, due to a change of sign of its anisotropy field H_{A}^{19}, with a small sublattice canting due to its internal Dzyaloshinskii–Moriya interaction (DMI)^{20}. One must notice that the Morin transition can disappear due to size effects in thin films and be recovered through doping^{21}. A similar transition towards a canted easyplane phase can be obtained at lower temperatures for sufficiently high fields in the spinflop state^{20,22}. In order to realize room temperature spintransport, one needs to demonstrate the transport in the easyplane phase. Hematite therefore represents a model system to simultaneously address and compare the origins of the magnonic transport in easyaxis and canted easyplane antiferromagnets by making use of temperature and field cycling.
In this paper, we demonstrate that the easyplane phase of the antiferromagnet hematite can transport spininformation over long distances at room temperature. As a function of temperature, the spintransport length scale drops continuously. When going across the Morin transition there is no abrupt change but rather the transport length scale continuously changes with temperature. We associate this surprising behavior with currentinduced correlated magnon pairs with a small difference of k vectors in combination with the ultralow magnetic damping of hematite that we measure using electron paramagnetic resonance at frequencies of hundreds of gigahertz. Altogether we can explain the longdistance transport present in both the easyaxis and easyplane phases and at elevated temperatures as required for applications.
Results
Spin transport through the Morin transition
To study the role of the antiferromagnetic symmetry and anisotropy in the transport of antiferromagnetic magnons, we performed nonlocal measurements on a crystal of the antiferromagnet hematite using platinum stripes, parallel to the projection of the inplane projection of the easyaxis (along the xaxis, sketch in Fig. 1a). To measure magnon transport, we inject a charge current through the Pt injector, which generates a transverse spincurrent due to the spinHall Effect (SHE). An electron spinaccumulation builds up at the Pt/αFe_{2}O_{3} interface (along y) resulting in the excitation of spinpolarized magnons for a parallel alignment of the antiferromagnetic order and the interfacial electron spinaccumulation. This nonequilibrium magnon population then diffuses away from the injector and is then absorbed by an electrically isolated Pt detector some distance away (0.5 to 10 μm). It is then converted to a charge current via the inverse SHE. This spinbias signal can then be expressed as a nonlocal voltage V_{el} as previously established^{16}.
While transport has so far been confined to the low temperature easyaxis phase, here we investigate the temperature dependence of the spintransport signal through the Morin transition as shown in Fig. 1b. As we previously reported^{16}, we observe at all temperatures below the Morin temperature (T_{M} = 260 K) a peak of the spintransport signal at the spinflop field when the applied field leads to the Néel vector reorientation (n // y) and the softening of the magnetic systems closes the magnon gap. This divergence is less pronounced at lower temperatures for which the magnetic susceptibility and the spinflop field are larger (about 8 T at 150 K^{22}). The absence of detectable signal below 75 K indicates a diffusive transport process dominated by thermal magnons and no dominating spin superfluidity. At temperatures above T_{M}, in the easyplane phase, the peak is less pronounced and the amplitude of the signal decreases as seen in Fig. 1c.
In parallel, we also measure a reduction of the magnon spindiffusion length λ as the temperature increases. This decrease is in contrast to the increase with temperature observed in ferrimagnet YIG^{23}. We detect a spintransport signal for distances larger than 500 nm between the injector and the detector up to 320 K allowing us to determine that the spintransport length scales even above room temperature are still in the range of μm. These features highlight the change of the spintransport properties of diffusive magnons between the easyplane and easyaxis antiferromagnetic phases.
Spin transport in the canted easyplane phase
To characterize the detailed magnon transport properties above the Morin temperature, and in particular identify whether the spin current is carried by the Néel vector or the weak canted moment, which are orthogonal to one another, we present in Fig. 2 the angular and field dependences of the spin signal in the canted easyplane phase (sketch of Fig. 2a). When we apply a field along the x or the zaxis, the Néel vector smoothly reorients within the easyplane and orients perpendicular to the Pt stripes, i.e., along y, and saturates at a field of about 0.4 T. This small spinflop field in the easyplane arises from magnetoelastic interactions, which emerge above the Morin temperature^{24}. This spinflop field, associated with a 6^{th} order anisotropy term, leads to a threefold symmetry in the easyplane and to a nonzero frequency gap^{22}. Such threefold symmetry prevents a full compensation of the anisotropy fields, and is detrimental to achieve potential spinsuperfluid regimes in linear response^{12}.
Above the spinreorientation transition, the amplitude of the spin signal smoothly decreases when the field is applied along the x and zaxes. If instead, the field is applied perpendicular to the stripes, the Néel order orients perpendicular to the electron spinaccumulation and no signal is observed (red curve in Fig. 2b). This indicates that the spin information is transported along the Néel order direction and not by the weak canted moment; the transport is thus of antiferromagnetic nature as found previously for the easyaxis phase. The moment due to the canting of the sublattices plays no significant role here. We confirm these observations using the angular dependence in the (xy), (yz), and (xz) planes as shown in Fig. 2c–e. The transport signal shows a maximum for H parallel to either x or z, while a minimum is observed for a magnetic field applied along y. At 0.5 T, the signal is nearly always maximal in the γplane (Fig. 2e) except at γ = −35 ± 5° (mod. 180°) for which the field is applied perfectly along the hardaxis (caxis). In this latter case, the condition n parallel to the current polarization y is not fulfilled and no spincurrent propagates. Considering the angular dependence of the signals shown in Fig. 2c–e, one can see that the easyplane symmetry plays a crucial role in the properties of the spintransport signal^{25}. In the (xy) and (yz) planes, the oscillations keep their shape at 8 T but their amplitude strongly decreases as expected from the measurements using a singlefield direction shown in Fig. 2b. The increase of the externally applied magnetic field has two main effects: first, the increasing field enhances the magnon gap, indicating that low energy magnons with small k vectors dominate the spintransport signal. Second, it modifies the magnon polarization; above the Morin transition, the ellipticity of the magnons near the center of the Brillouin zone^{5}, evolves towards a linear polarization with increasing temperature (due to the continuous increase in the hardaxis anisotropy).
Antiferromagnetic resonance and magnetic damping of hematite
Having established the possibility of spin transport in both the easyaxis and easyplane phase of hematite, we need to understand the origin of the record spintransport distances found in hematite. A key parameter of the magnon decay length in both the easyaxis and easyplane antiferromagnetic phases is the magnetic damping. To obtain information about the magnetization dynamics of hematite and on this key parameter, we investigate the magnetization dynamics on a single crystal of hematite using magnetic resonance measurements from 120 GHz to 380 GHz^{26}. From the dynamics of the probed uniform mode, we can extract information about the low k magnons which dominate the spin transport. In Fig. 3a, b, we show the frequency and linewidth dependence of the low frequency mode. The frequency dependence of the mode can be fitted using our calculations^{27}. Owing to a wavelength smaller than the thickness of the crystal at high frequencies, we observe a broad peak at low magnetic field and multiple resonance peaks at higher magnetic fields (see inset of Fig. 3a). At magnetic fields below 4 T, the presence of magnetostatic modes leads to additional linewidth broadening that prevents us from extracting the magnetic damping (see “Methods”). Above this value, we can extract the resonance linewidth by measuring the average peaktopeak distance of the resonances. This technique leads to large error bars as shown in Fig. 3b, but the results are in agreement with previous measurements using neutron^{2}, terahertz^{28} and electron paramagnetic resonance^{29,30} spectroscopy. The results cannot be fitted well with the existing simple theories of antiferromagnetic resonances^{31}, but we can deduce a magnetic damping with an upper limit of 10^{−5}. This indicates that the magnetic damping of hematite α is of the same order as for YIG, the ferromagnetic material with so far the lowest reported magnetic damping of any magnetic compound.
We also performed magnetic resonance measurements for a fixed excitation frequency of 127 GHz as a function of temperature as shown in Fig. 3c. First, we observe that the linewidths at 200 K and 300 K are of similar order of magnitude showing that the magnetic damping is low in both the easyplane and easyaxis phases. We also observe a small increase of the linewidth around T_{M}, indicative of stronger dissipation processes at the transition which could arise from the minimum anisotropy at the Morin transition^{31}.
Discussion
To understand the observed spin transport resulting from the magnon properties in hematite, we develop a simple phenomenological model of magnon transport which defines a phase diagram with two regions (see Fig. S1 in Supplementary Information). Below the critical field H_{cr}(T) for the spinflop, the equilibrium orientation of the Néel vector \({\mathbf{n}}^{\left( 0 \right)}\left( {\mathbf{H}} \right)\) varies depending on the magnetic field H (inset in Fig. S1 in Supplementary Information). In this region (both above and below the Morin transition), the magnon modes are polarized parallel or antiparallel to the equilibrium orientation of the Néel vector. Spin transport in this region is similar to spin transport of uniaxial antiferromagnets discussed in refs. ^{9,16}. Above the critical field H_{cr}(T), the Néel vector \({\mathbf{n}}^{\left( 0 \right)}\left( {\mathbf{H}} \right)\mathbf{ y} \bot {\mathbf{H}}\) is oriented perpendicular to the magnetic field, the magnon eigenmodes in the absence of a spin current are linearly polarized. So, to understand the observed spintransport signal, we need to discuss the magnon spin transport in antiferromagnets with linearly polarized magnon modes.
To address this, we first analyze the magnon spectrum in the presence of spinpolarized currents emerging from the current distribution in the Pt injector electrode. Below the critical field H_{cr}(T) where the eigenmodes have an elliptical polarization, i.e., carry spin information, the currentinduced antidamping torque suppresses (enhances) the damping of the magnons polarized parallel (antiparallel) to the spin of current^{32}. According to the fluctuation dissipation theorem^{33}, this can be interpreted as a splitting of the effective temperature T_{±} for spinup and spindown magnons^{34} and lead to the creation of a nonequilibrium spinaccumulation of magnons (see the details on the analytical modelling in the Supplementary Information):
where \({\mathbf{H}}_{{\mathbf{curr}}}\) is the effective field parallel to the electron spinaccumulation and proportional to the current density j, f is the equilibrium BoseEinstein distribution function and \(\omega _ \pm\) is the magnon frequency. The spin polarization of the magnon mode \(0 \le s_ \pm \le 1\) is related to its ellipticity^{5,32}, and depends on the magnetic field: \(s_ \pm \propto {\mathbf{H}} \cdot {\mathbf{n}}^{\left( 0 \right)}\). The nonmonotonic field dependence of the voltage \(V\left( H \right) \propto \mu _y\) shown in Fig. 1b. is thus explained by a fieldinduced variation of the ellipticity \(s_ \pm\) and the rotation of the Néel vector. This model also predicts the growth of the V(H) maximum with temperature once the temperature dependence of the magnetic easyaxis anisotropy \(H_{{\mathrm{an}}}(T)\)^{27} is taken into account, as shown in the top panel of Fig. 1c. by the gray line.
Above the critical field H_{cr}(T), below and above the Morin transition, the situation changes completely: the magnon modes are linearly polarized and the currentinduced torques establish correlations between the linearly polarized magnon modes with orthogonal polarizations^{35}. The pairs of two linearly polarized magnons with different frequencies, though coupled by current, carry no spinangular momentum and do not contribute to spin transport. However, the pairs, whose wave vectors k satisfy the energy conservation relation, \(\omega _1^2 + c^2{\mathbf{k}}_1^2 = \omega _2^2 + c^2{\mathbf{k}}_2^2\), (see Fig. 4), generate a net nonequilibrium magnon spinaccumulation (1) with \(\omega _ + \to \sqrt {\omega _1^2 + c^2{\mathbf{k}}_1^2}\), \(s_ + = 1\), \(s_  = 0\), where \(H_{{\mathrm{curr}}}\left( {{\mathbf{k}}_1  {\mathbf{k}}_2} \right)\) corresponds to the space Fourier component of the current j(k_{1} – k_{2}), ω_{1,2} to the gaps (k = 0) of the high frequency and low frequency magnon branches, c is the limiting velocity of magnons. These pairs thus carry spin information, which explains the presence of a nonzero spintransport signal above the spinflop field and in the easyplane phase above the Morin transition.
Below the Morin transition, the spinpropagation length λ of magnons was measured at the spinflop field, i.e., at the phase boundary H_{cr}(T) where the signal \(V_{{\mathrm{el}}}\) reaches a maximal value (Fig. 1b). The corresponding temperature dependence can be well fitted with the law \(\lambda \propto \sqrt {H_{{\mathrm{an}}}\left( T \right)/T}\), which correlates with the magnon spindiffusion length \(\lambda _T \propto 1/\sqrt T\)^{9} as shown in the bottom panel of Fig. 1c. The additional factor \(\sqrt {H_{{\mathrm{an}}}\left( T \right)}\) can be attributed to the effect of the magnetic field, which stabilizes elliptically polarized states and whose value at the phase boundary H_{cr}(T) scales with \(H_{{\mathrm{an}}}\).
In the region above H_{cr}(T) and above the Morin transition, the characteristic decay length of the magnon is dominated by the dephasinginduced attenuation of the signal. This is also illustrated in Fig. 2b, which shows the field dependence V(H) at a fixed distance x from the injector electrode. Formally, the spatial dependence of the attenuated signal in the presence of dephasing follows the same exponential decay \(V\left( y \right) \propto {\mathrm{exp}}\left( {  \frac{y}{L}} \right)\) as in the case of diffusion. However, the characteristic length L depends on the difference \(\left {{\mathbf{k}}_1  {\mathbf{k}}_2} \right\) and, correspondingly, on the difference of magnon frequencies. We thus establish that the expression of the characteristic dephasing length is:
where we assumed that Δk_{z }≪ k_{y}. One can notice that the magnetic field increases the splitting between the frequencies \(\omega _1^2  \omega _2^2\), which explains how V(H) diminishes together with L(H). Furthermore, close to the Morin transition temperature, the values of the inplane (\(H_{{\mathrm{an}} \bot }\)) and outofplane magnetic anisotropies (H_{an}) are of the same order of magnitude. As a consequence, \(\omega _1^2  \omega _2^2 \propto H_{{\mathrm{an}}}  H_{{\mathrm{an}} \bot }\) is relatively small and L is relatively large (in the μm range). It should however be noted that \(H_{{\mathrm{an}} \bot }\) strongly increases above the Morin transition whilst H_{an} remains nearly constant^{29}. Far above the Morin transition, the frequency splitting is so strong even in absence of the magnetic field, that the dephasing length is below the experimental resolution. This result highlights the importance of having inplane and outofplane anisotropies of the same order to propagate spin information, which makes cubic antiferromagnets potential candidates in this purpose if they exhibit magnetic damping as low as hematite.
This longdistance spintransport in both easyaxis and, in particular, easyplane antiferromagnets and the observed ultralow magnetic damping are remarkable features. Our findings broaden the class of materials in which one can use to propagate spin information^{36}. Not only easyaxis antiferromagnets with intrinsic circularly polarized magnon modes can carry spin information, but also in easyplane antiferromagnets one can electrically generate pairs of linearly polarized spin waves, which carry an effective circular polarization and thus a spin information. The dephasing length of these magnon pairs is strongly dependent on the difference of their k vectors and thus on the magnetic anisotropies of the antiferromagnet. One can also control the Δk of the two magnon branches by applying a magnetic field or by varying the temperature. Secondly, the combined transport and antiferromagnetic resonance measurements highlight the high potential of low damping antiferromagnetic insulators, both with easyaxis and easyplane anisotropies, for their integration into magnonic and spintronic devices. Our findings potentially open the transport also to hematite thin films, which are intrinsically mostly in the easy plane phase^{37}. Significant further advances in the fabrication of highquality thin films with large domains are necessary to realize future devices^{8}. More generally, insulating antiferromagnets can have magnetic damping as low as the best ferromagnets and can also transport spin information at room temperature over large length scales, which are both key features for magnonic devices.
Methods
Hematite crystal
Hematite crystals (5 × 5 × 0.5 mm) orientated such that the sample plane is (1\(\bar 1\)02), also known as rplane, were commercially obtained. Before patterning the devices, the crystals were cleaned with acetone, isopropanol, and deionised water to remove any organic surface residues. The Morin temperature was obtained by magnetometry measurements using a superconducting quantum interference device and detecting the emerging canted moment at high temperatures.
Magnetotransport measurements
We patterned the nonlocal devices using electron beam lithography and the deposition of a 7 nm platinum layer by direct current sputtering in an Ar atmosphere to form the wires. The electrical contacts were patterned also by electron beam lithography and the deposition of a bilayer of Cr(6 nm)/Au(32 nm). The length of the Pt wires is 160 μm and their width is 350 nm wide. The separations between the wires range from 500 nm–10 μm. The sample was mounted to a piezorotating element in a superconducting magnet capable of fields up to 12 T and a temperature range from 10–320 K. Below 260 K, the resistivity of hematite is sufficiently large to avoid any leakage current between the platinum electrodes. At larger temperature, we performed rotation measurements to extract the spin signal and remove any small leakage current. The measured voltage was detected in the platinum detector wires using a nanovoltmeter, owing to the inverse spinHall effect creating a charge flow. This voltage was recorded as a function of the spatial separation, external field, applied bias current and angle between the charge current and the field. Electrical current polaritydependences were used to disentangle the contribution of the injected spin current from that of the thermally induced spin current.
Magnetic resonance measurements
We characterized the magnetic resonance of a 0.5 mm thick single crystal of hematite using a setup that combines variable temperatures (5–290 K), strong magnetic fields (0–16 T) and high frequencies (127, 254, and 381 GHz)^{26}. The measurement setup consists of a continuouswave electron paramagnetic resonance spectrometer, the principle of which is based on a quasioptical propagation of microwaves generated by solid sources (95–130 GHz) associated with multipliers. The radiation is propagated with mirrors and polarizers outside a cryostat, whereas a corrugated waveguide is used inside. The derivative of the absorption of the wave, obtained with the help of a field modulation, is detected by a bolometer. The applied continuous magnetic field is applied in the sample plane and the microwave field is at 45° from the surface normal. The low frequency measurements (below 50 GHz) were performed using coplanar waveguides and 40 GHz radiofrequency source in a Quantum Design 9 T superconducting magnet.
Analyzing the shape of the antiferromagnetic resonance measurements requires one to carefully disentangle the contribution from magnetostatic modes. In ferromagnetic crystals, the observation of magnetostatic modes in resonance measurements is a common feature that appears in materials with low magnetic damping like YIG^{38}. At low magnetic fields, the magnetostatic modes lead to an artificial broadening of the FMR peak and large magnetic fields are required to resolve each peak individually. The situation is similar in antiferromagnetic crystals with an internal DMI field or in presence of external magnetic field^{39}. The field difference ΔH_{m} between the difference magnetostatic modes can be expressed as:
With f_{m} a fraction of several tenths^{39}. In hematite, we evaluate ΔH_{m} to be around 2 mT at H = 0 and 10 mT at H = 4 T for the separation between the lowest magnetostatic modes. In order to resolve the intrinsic linewidth of hematite ΔH_{res}, one requires ΔH_{m }≫ H_{res} or ΔH_{m }≪ H_{res} This condition is fulfilled only at high fields in the case of hematite. Then, resonance linewidths and fields were extracted by measuring the average peaktopeak distance and center of the resonances.
Data availability
The data that support the findings of this study are available from the corresponding authors upon reasonable request. Correspondence and requests for materials should be addressed to R.L. or M.K.
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Acknowledgements
R.L. acknowledges the European Union’s Horizon 2020 research and innovation program under the Marie SkłodowskaCurie grant agreements FAST number 752195. R.L., A.R. and M.K. acknowledge support from the Graduate School of Excellence Materials Science in Mainz (MAINZ) DFG 266, the DAAD (Spintronics network, Project No. 57334897), the ERC Synergy Grant 3D MAGIC No. 856538 and all groups from Mainz acknowledge that this work was funded by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) SFB TRR 173 –268565370 (projects A01, A03, A11, B02, B11 and B12). R.L. and M.K. acknowledge financial support from the Horizon 2020 Framework Program of the European Commission under FETOpen grant agreement no. 863155 (sNebula). R.L., A.R., and M.K. acknowledge support from the DFG project number 423441604. O.G. and J.S. acknowledge the Alexander von Humboldt Foundation, the ERC Synergy Grant SC2 (No. 610115). This work was also supported by the Max Planck Graduate Center (MPGC). A.Q, A.B., M.K. were supported by the Research Council of Norway through its Centers of Excellence funding scheme, project number 262633 “QuSpin”. V.B. acknowledges financial support from the French national research agency (ANR) (Grant Number ANR15CE24001501) and the bottomup exploratory program of the CEA (Grant Number PE18P31ELSA).
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R.L. and M.K. proposed and supervised the project. R.L. and A.R. performed the transport experiments. R.L., U.E., V.B., and A.L.B. performed the magnetic resonance measurements. A.R. patterned the samples. R.L., O.G., A.R. analyzed the data. O.G. performed the analytical calculations with inputs from R.L., M.K., A.Q., J.S., and A.B., R.L., O.G., A.R., and M.K. wrote the paper. All authors commented on the manuscript.
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Lebrun, R., Ross, A., Gomonay, O. et al. Longdistance spintransport across the Morin phase transition up to room temperature in ultralow damping single crystals of the antiferromagnet αFe_{2}O_{3}. Nat Commun 11, 6332 (2020). https://doi.org/10.1038/s41467020201557
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DOI: https://doi.org/10.1038/s41467020201557
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