Decrease of upper critical field with underdoping in ... · (see Supplementary Fig. S3 and Fig. 4c...

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ARTICLES PUBLISHED ONLINE: 12 AUGUST 2012 | DOI: 10.1038/NPHYS2380 Decrease of upper critical field with underdoping in cuprate superconductors J. Chang 1 , N. Doiron-Leyraud 1 , O. Cyr-Choinière 1 , G. Grissonnanche 1 , F. Laliberté 1 , E. Hassinger 1 , J-Ph. Reid 1 , R. Daou 1 , S. Pyon 2 , T. Takayama 2 , H. Takagi 2,3 and Louis Taillefer 1,4 * It is still unclear why the transition temperature T c of cuprate superconductors falls with underdoping. The doping dependence of the critical magnetic field H c2 is directly relevant to this question, but different estimates of H c2 are in sharp contradiction. We resolve this contradiction by tracking the characteristic field scale of superconducting fluctuations as a function of doping, via measurements of the Nernst effect in La 1.8-x Eu 0.2 Sr x CuO 4 . H c2 is found to fall with underdoping, with a minimum where stripe order is strong. The same non-monotonic behaviour is observed in the archetypal cuprate superconductor YBa 2 Cu 3 O y . We conclude that competing states such as stripe order weaken superconductivity and cause both H c2 and T c to fall as cuprates become underdoped. T wo paradigms have been proposed to account for the dome-like region of superconductivity in the temperature- doping phase diagram of cuprate superconductors 1 . In the first, the amplitude of the superconducting order parameter grows monotonically as the doping p is reduced, but its phase is increasingly disordered 2 , causing T c to fall at low p. The signature of this scenario is strong phase fluctuations and a superconducting gap above T c in the underdoped regime. In the second paradigm, the fall of T c at low p is due to the onset of a state that competes with superconductivity. The signature of this scenario is a small superconducting gap and a small H c2 in the underdoped regime. Whether strong phase fluctuations or a decrease in the pairing gap is causing T c to fall in underdoped cuprates is currently an open question. Different interpretations of photoemission data disagree on the evolution of the pairing gap 3–6 and different estimates of the upper critical field H c2 are in sharp contradiction 7,8 . The Nernst signal observed above T c in underdoped cuprates has been attributed to superconducting fluctuations 8–10 , and because it persists up to temperatures several times T c , it was deemed incompatible with the standard Gaussian fluctuations of the superconducting order parameter. It was attributed instead to vortex-like excitations in a phase-fluctuating superconductor 9,10 with a non-zero pairing amplitude above T c . The critical field H c2 deduced from the Nernst data on cuprates such as Bi 2 Sr 2 CaCu 2 O 8+δ (Bi-2212) was reported to increase with underdoping 8 , even though T c falls. As shown in Fig. 1a, this is in striking contrast to the rapid drop in H c2 deduced from a Gaussian analysis of fluctuations in the magneto-conductivity of YBa 2 Cu 3 O y (YBCO; ref. 7). Nernst effect in Eu–LSCO Here we re-examine the Nernst effect in cuprates with a study of La 1.8-x Eu 0.2 Sr x CuO 4 (Eu–LSCO), an underdoped cuprate in which the ratio of superconducting (N sc ) to quasiparticle (N qp ) contributions to the Nernst signal N is exceptionally large—at 1 Département de physique and RQMP, Université de Sherbrooke, Sherbrooke, Québec J1K 2R1, Canada, 2 Department of Advanced Materials, University of Tokyo, Kashiwa 277-8561, Japan, 3 RIKEN (The Institute of Physical and Chemical Research), Wako 351-0198, Japan, 4 Canadian Institute for Advanced Research, Toronto, Ontario M5G 1Z8, Canada. Present addresses: Institut de Physique de la Matière Complexe, École Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland & Paul Scherrer Institut, CH-5232 Villigen, Switzerland (J.C.); Laboratoire de Cristallographie et Sciences des Matériaux, CNRS (UMR6508), Caen 14050, France (R.D.). *e-mail:[email protected]. least 100 times larger than in previous studies of superconducting fluctuations in cuprates (see Supplementary Table S2). Because of its low T c , we could determine the quasiparticle background N qp (T ) in Eu–LSCO by fully suppressing superconductivity with a magnetic field (Fig. 2a). The large signal-to-background ratio allows us to reliably track N sc up to high temperature, namely up to a reduced temperature ε (T T c )/T c 5, compared to a typical upper limit of ε 0.5. As we shall see, this gives us access to a regime where the complicating effects of paraconductivity are negligible. In Fig. 3a, N sc is plotted versus magnetic field H for different temperatures above T c , for Eu–LSCO at a doping p = 0.11. N sc increases linearly at low H , peaks at a field H * and then decreases monotonically at high H , just as in the conventional superconductor Nb 0.15 Si 0.85 (refs 11,12; Supplementary Fig. S2). The peak field H * , also called the ‘ghost critical field’ (ref. 12), is plotted versus ε in Fig. 3b. It obeys H * = H * c2 ln(T /T c ) from ε 0.5 to ε 5, where H * c2 is a field scale whose relation to the T = 0 upper critical field H c2 is discussed below. Below ε 0.5, H * deviates from ln(T /T c ), and remains finite as ε 0. This is because N sc (ε) = α sc xy (ε)(ε) is the ratio of two quantities 13–16 —the off-diagonal Peltier coefficient from superconducting fluctuations α sc xy and the electrical conductivity σ —which both diverge as ε 0 (ref. 13). This causes N sc to saturate at low ε (Fig. 4). The deviation of H * from ln(T /T c ) coincides with the onset of paraconductivity below T 6K 1.5T c (see Supplementary Fig. S3 and Fig. 4c inset). Above ε 0.5, paraconductivity is negligible (Supplementary Fig. S4) and σ reaches its (field-independent) normal-state value, at which point N sc (H ) α sc xy (H ). We make use of H * in the latter regime only. H * also obeys H * = H * c2 ln(T /T c ) in our other Eu–LSCO samples (Supplementary Table S1 and Fig. S1), with p = 0.08, 0.10 and 0.125 (Fig. 3c). The value of H * c2 extracted from the fit at each doping is plotted in Fig. 5a. Our first and main finding is this: the field scale for superconductivity, H * c2 , decreases with underdoping, in a non-monotonic way, with a local minimum at p = 0.11. This NATURE PHYSICS | VOL 8 | OCTOBER 2012 | www.nature.com/naturephysics 751 © 2012 Macmillan Publishers Limited. All rights reserved.

Transcript of Decrease of upper critical field with underdoping in ... · (see Supplementary Fig. S3 and Fig. 4c...

Page 1: Decrease of upper critical field with underdoping in ... · (see Supplementary Fig. S3 and Fig. 4c inset). Above "ˇ0:5; ... Nernst data on Nb 0:15Si 0:85 (refs 11,12) yield a peak

ARTICLESPUBLISHED ONLINE: 12 AUGUST 2012 | DOI: 10.1038/NPHYS2380

Decrease of upper critical field with underdopingin cuprate superconductorsJ. Chang1†, N. Doiron-Leyraud1, O. Cyr-Choinière1, G. Grissonnanche1, F. Laliberté1, E. Hassinger1,J-Ph. Reid1, R. Daou1†, S. Pyon2, T. Takayama2, H. Takagi2,3 and Louis Taillefer1,4*

It is still unclear why the transition temperature Tc of cuprate superconductors falls with underdoping. The doping dependenceof the critical magnetic field Hc2 is directly relevant to this question, but different estimates of Hc2 are in sharp contradiction.We resolve this contradiction by tracking the characteristic field scale of superconducting fluctuations as a function of doping,via measurements of the Nernst effect in La1.8−xEu0.2SrxCuO4. Hc2 is found to fall with underdoping, with a minimum wherestripe order is strong. The same non-monotonic behaviour is observed in the archetypal cuprate superconductor YBa2Cu3Oy.We conclude that competing states such as stripe order weaken superconductivity and cause both Hc2 and Tc to fall as cupratesbecome underdoped.

Two paradigms have been proposed to account for thedome-like region of superconductivity in the temperature-doping phase diagram of cuprate superconductors1. In the

first, the amplitude of the superconducting order parametergrows monotonically as the doping p is reduced, but its phaseis increasingly disordered2, causing Tc to fall at low p. Thesignature of this scenario is strong phase fluctuations and asuperconducting gap above Tc in the underdoped regime. In thesecond paradigm, the fall of Tc at low p is due to the onset of astate that competes with superconductivity. The signature of thisscenario is a small superconducting gap and a small Hc2 in theunderdoped regime.

Whether strong phase fluctuations or a decrease in the pairinggap is causing Tc to fall in underdoped cuprates is currently anopen question. Different interpretations of photoemission datadisagree on the evolution of the pairing gap3–6 and differentestimates of the upper critical fieldHc2 are in sharp contradiction7,8.The Nernst signal observed above Tc in underdoped cuprates hasbeen attributed to superconducting fluctuations8–10, and becauseit persists up to temperatures several times Tc, it was deemedincompatible with the standard Gaussian fluctuations of thesuperconducting order parameter. It was attributed instead tovortex-like excitations in a phase-fluctuating superconductor9,10with a non-zero pairing amplitude above Tc. The critical field Hc2deduced from theNernst data on cuprates such as Bi2Sr2CaCu2O8+δ(Bi-2212) was reported to increase with underdoping8, even thoughTc falls. As shown in Fig. 1a, this is in striking contrast to the rapiddrop inHc2 deduced from a Gaussian analysis of fluctuations in themagneto-conductivity of YBa2Cu3Oy (YBCO; ref. 7).

Nernst effect in Eu–LSCOHere we re-examine the Nernst effect in cuprates with a studyof La1.8−xEu0.2SrxCuO4 (Eu–LSCO), an underdoped cuprate inwhich the ratio of superconducting (Nsc) to quasiparticle (Nqp)contributions to the Nernst signal N is exceptionally large—at

1Département de physique and RQMP, Université de Sherbrooke, Sherbrooke, Québec J1K 2R1, Canada, 2Department of Advanced Materials, University ofTokyo, Kashiwa 277-8561, Japan, 3RIKEN (The Institute of Physical and Chemical Research), Wako 351-0198, Japan, 4Canadian Institute for AdvancedResearch, Toronto, Ontario M5G 1Z8, Canada. †Present addresses: Institut de Physique de la Matière Complexe, École Polytechnique Fédérale de Lausanne(EPFL), CH-1015 Lausanne, Switzerland & Paul Scherrer Institut, CH-5232 Villigen, Switzerland (J.C.); Laboratoire de Cristallographie et Sciences desMatériaux, CNRS (UMR6508), Caen 14050, France (R.D.). *e-mail: [email protected].

least 100 times larger than in previous studies of superconductingfluctuations in cuprates (see Supplementary Table S2). Because ofits lowTc, we could determine the quasiparticle backgroundNqp(T )in Eu–LSCOby fully suppressing superconductivitywith amagneticfield (Fig. 2a). The large signal-to-background ratio allows us toreliably track Nsc up to high temperature, namely up to a reducedtemperature ε≡ (T–Tc)/Tc≈ 5, compared to a typical upper limitof ε≈ 0.5. As we shall see, this gives us access to a regime where thecomplicating effects of paraconductivity are negligible.

In Fig. 3a, Nsc is plotted versus magnetic field H for differenttemperatures above Tc, for Eu–LSCO at a doping p = 0.11.Nsc increases linearly at low H , peaks at a field H ∗ and thendecreases monotonically at high H , just as in the conventionalsuperconductor Nb0.15Si0.85 (refs 11,12; Supplementary Fig. S2).The peak field H ∗, also called the ‘ghost critical field’ (ref. 12), isplotted versus ε in Fig. 3b. It obeysH ∗=H ∗c2ln(T/Tc) from ε≈ 0.5to ε≈ 5, whereH ∗c2 is a field scale whose relation to the T = 0 uppercritical fieldHc2 is discussed below.

Below ε ≈ 0.5, H ∗ deviates from ln(T/Tc), and remains finiteas ε → 0. This is because Nsc(ε) = αsc

xy(ε)/σ (ε) is the ratioof two quantities13–16—the off-diagonal Peltier coefficient fromsuperconducting fluctuations αsc

xy and the electrical conductivityσ—which both diverge as ε→ 0 (ref. 13). This causes Nsc tosaturate at low ε (Fig. 4). The deviation of H ∗ from ln(T/Tc)coincides with the onset of paraconductivity below T ≈ 6K≈ 1.5Tc(see Supplementary Fig. S3 and Fig. 4c inset). Above ε ≈ 0.5,paraconductivity is negligible (Supplementary Fig. S4) and σ

reaches its (field-independent) normal-state value, at which pointNsc(H )∼αsc

xy(H ).Wemake use ofH ∗ in the latter regime only.H ∗ also obeysH ∗=H ∗c2ln(T/Tc) in our other Eu–LSCO samples

(Supplementary Table S1 and Fig. S1), with p=0.08, 0.10 and 0.125(Fig. 3c). The value of H ∗c2 extracted from the fit at each dopingis plotted in Fig. 5a. Our first and main finding is this: the fieldscale for superconductivity, H ∗c2, decreases with underdoping, ina non-monotonic way, with a local minimum at p = 0.11. This

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ARTICLES NATURE PHYSICS DOI: 10.1038/NPHYS2380

Prior analysis

New analysis

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Figure 1 |Doping dependence of the upper critical field Hc2 in cupratesuperconductors. a, Upper critical field Hc2 of cuprate superconductorsversus doping p extracted from magneto-conductivity data on YBCO (ref. 7,blue circles; left axis) and from Nernst data on Bi-2212 (ref. 8, red circles;left axis). These two studies of superconducting fluctuations above Tc ledto contradictory conclusions on how the superconducting pairing strengthin cuprates varies with doping. The superconducting Tc of YBCO is alsoshown (ref. 34, grey dome; right axis). b, Two different definitions of theupper critical field Hc2 extracted from Nernst data on the same material,Bi-2201, lead to opposite doping dependencies. When Hc2 is defined as thefield H where N versus H at T= Tc extrapolates to zero (filled black circlesand error bars, from ref. 8), one finds that Hc2 increases with underdoping.The same increase is found for the peak field H∗ in N versus H (see Fig. 3a)when taken at T= Tc (open black circles; from Fig. 7,×10). By contrast, adecrease is found if the peak field H∗ is taken at T≈ 1.65Tc (ε≈0.65),outside the region of strong paraconductivity (open red circles; from Fig. 7,×1.9). The latter result is independent of any theory. Equivalently, Hc2 maybe obtained as H∗c2 in a fit of the peak field H∗ to H∗c2ln(T/Tc) (see Fig. 3b),as done in Fig. 7 (filled red circles), again yielding an Hc2 that decreaseswith underdoping. This is true whether H∗ is obtained from Nernst data(away from the region of strong paraconductivity) or from diamagnetism(Fig. 7). The error bars on the filled red circles reflect the uncertainty infitting the H∗ data points in Fig. 7 to the relation H∗c2ln(T/Tc). Error bars onopen circles (red and black) reflect the uncertainty in determining H∗ fromthe data in refs 10,20 (see Fig. 7).

result comes directly from the Nernst data, free of any model ortheory. In fact, the evolution of H ∗c2 may be directly read off theraw N versusH isotherms: it is simply proportional to the fieldH ∗at which N peaks for a given reduced temperature, say T = 1.5Tc(Supplementary Fig. S5).

9 T28 T

/T (

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Figure 2 |Quasiparticle and superconducting contributions to the Nernstsignal in Eu–LSCO. a, Temperature dependence of the Nernst coefficientν≡N/H of Eu–LSCO at p=0.125, plotted as ν/T versus T, for twomagnetic fields as indicated. ν(T) is independent of H for T> 35 K, andhence ν(T)≈ νqp(T) above 35 K (ref. 32). In the range 35–70 K, ν/T islinear, so that νqp/T= a−bT (solid black line). Application of a field of 28 T(open squares) to suppress superconductivity such that νsc� νqp showsthat the linear T dependence of νqp(T) persists as T→0. We therefore takeNqp= νqpH= (a−bT)TH to be our estimate of the quasiparticlecontribution used to extract Nsc(T,H)=N(T,H)−Nqp(T). The sameprocedure is applied to the data at p=0.08, 0.10 and 0.11, with parametersa and b that are only slightly different. The dashed lines are the upper andlower bounds on the uncertainty in νqp(T). These translate into error bars inthe determination of H∗ plotted in Fig. 3b,c (see panels below). b,c, Nernstsignal N= νH (black) measured in Eu–LSCO at p=0.11 and quasiparticlecontribution Nqp= νqpH (dashed blue line), for two temperatures asindicated. The difference Nsc=N−Nqp (red) is the contribution ofsuperconducting fluctuations. In b, where ε < 1, Nqp is small compared withthe measured Nernst signal and hence the extraction of the peak field H∗,defined as the field where Nsc versus H is maximal, is essentially unaffectedby the subtraction of Nqp. By contrast for ε > 1 (c), Nqp is large andsubtraction is necessary to obtain an accurate determination of H∗.

Nernst data on Nb0.15Si0.85 (refs 11,12) yield a peak field inagreement with H ∗ = H ∗c2ln(T/Tc) up to at least 5 Tc (Fig. 3c).Pourret et al. point out that H ∗ separates a low-H regimecontrolled by the temperature-dependent coherence length ξ(T )=ξ0/(ln(T/Tc))1/2 and a high-H regime controlled by the magneticlength lB= (h/2eH )1/2 (ref. 17) where ξ0 is the T =0 superconduct-ing coherence length, h is Planck’s constant, and e is the electroncharge. They argue thatH ∗ is the field where ξ(T )= lB(H ∗), so thatH ∗ = (80/2πξ 20 )ln(T/Tc), where 80 = h/2e is the flux quantum.

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NATURE PHYSICS DOI: 10.1038/NPHYS2380 ARTICLES

H∗

Tc = 3.86 K

3.9 K4.8

19.0

5.56.78.2

10.213.1

0 5 10 15

H (T)

= (T¬Tc)/Tcε

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¬1 )

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c2

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00

Nb0.15Si0.850.1250.110.100.08

Figure 3 | Peak field H∗ in the superconducting Nernst signal above Tc.a, Superconducting Nernst signal Nsc of Eu–LSCO plotted as a function ofmagnetic field H at p=0.11, for different values of the temperature T asindicated. A quasiparticle background Nqp is subtracted from the raw dataof N versus H in Supplementary Fig. S1 (see Fig. 2). The arrows mark themaximum value of Nsc=N−Nqp for each isotherm, which defines the peakfield H∗ (also called the ‘ghost critical field’). b, Temperature dependence ofH∗ extracted from the data in a plotted versus reduced temperatureε≡ (T−Tc)/Tc. The solid line is a fit to H∗=H∗c2ln(T/Tc), which provides amodel-free field scale, H∗c2, equal to 6.2 T for this doping. c, Peak field H∗ inEu–LSCO at p=0.08, 0.10, 0.11 and 0.125, and in the conventionalsuperconductor Nb0.15Si0.85 (from ref. 11), plotted as H∗/H∗c2 versus ε, withH∗c2 obtained as in b for each sample. The values of H∗c2 are given inSupplementary Table S1 and plotted in Fig. 5a. Error bars on H∗ in b and ccome from the uncertainty in Nqp (Fig. 2).

This makes the field scaleH ∗c2 equal to the T = 0 upper critical fieldHc2 ≡80/2πξ 20 . In Supplementary Fig. S6, we use resistivity dataon Nd–LSCO, a material very similar to Eu–LSCO, to show thatthe field H res

c2 needed to suppress superconductivity in Nd–LSCOat p= 0.12 and T = Tc/20 is roughly equal to H ∗c2 in Eu–LSCO atp=0.125 (Fig. 5a). This confirms experimentally thatH ∗c2≈Hc2.

Comparison to Gaussian theoryWe now compare our data against the theory of Gaussianfluctuations13–15. The calculated curve of αsc

xy versus H (ref. 15) is

in excellent agreement with the measured curve of Nsc versus H(Fig. 6). The peak field in αsc

xy versus H increases with temperatureroughly asH ∗∼ ln(T/Tc) (Supplementary Fig. S7), with a prefactorthat is proportional to 1/ξ 20 (Supplementary Fig. S7). In the H = 0limit, theory predicts14,15: νsc σ =αsc

xy/H∼ξ20 /T ln(T/Tc). In Fig. 4a,

the Nernst coefficient ν(≡ N/H ) of Eu–LSCO at p = 0.11 isplotted versus H for different temperatures above Tc. Its valuein the H = 0 limit, ν0 ≡ ν(H → 0), is plotted in Fig. 4b as afunction of ε. In Fig. 4d, the data are seen to follow the theoreticaltemperature dependence precisely, from 1.02 Tc up to at least 5Tc, as previously found14,15 in Nb0.15Si0.85 (refs 11,12). As shown inFig. 6 (and explained in the Supplementary Information), the dataalso follow the theoretical dependence on magnetic field, both atT < Tc and at T > Tc. We conclude that our Nernst data on Eu–LSCO are consistent with several non-trivial features of Gaussiantheory. This validates the earlier use of Gaussian theory to analyseconductivity data7 in YBCO (in a context of much smaller signal-to-background ratio; Supplementary Table S2), discussed below.Note that the quantum oscillations observed in YBCO at p∼ 0.1(ref. 18) are consistent with Fermi-liquid theory19, the frameworkon which Gaussian theory is based. Agreement with Gaussiantheory and consistency of the different measures of Hc2 indicatethat the superconducting fluctuations in this cuprate are controlledentirely by the coherence length, and there is only one temperaturescale, Tc, and one field scale, Hc2, for superconductivity. Thefluctuations seem to be no different from those of conventionalsuperconductors, and there is no need to invoke unusual vortex-likeexcitations8–10,16,20,21, at least for p=0.08 and above.

Nernst effect and diamagnetism in Bi-2201Wang et al.8 extracted a field scale from their raw Nernst data onthe cuprates Bi-2212 and Bi2Sr2−yLayCu2O6 (Bi-2201), and foundit to increase with underdoping (Fig. 1). However, because theyused Nernst data at T = Tc, their analysis was contaminated byparaconductivity. Our analysis of their data8 away from Tc yieldsa field scale that decreases with underdoping, in agreement withdiamagnetism data20 on Bi-2201 (Fig. 7). TheH dependence ofMd,the diamagnetic component of magnetization, is very similar tothat of Nsc (ref. 21), as expected theoretically16,22. Magnetizationdata on an underdoped sample of Bi-2201 with Tc= 12K (ref. 20)yield a peak value H ∗d that obeys H ∗c2ln(T/Tc) all the way fromT ≈ Tc to T ≈ 4Tc (Fig. 7), with H ∗c2 ≈ 19 T. Applying the same fitto published Nernst data on a Bi-2201 sample of the same doping8yields the same value of H ∗c2 (Figs 1b and 7). In summary, bothdiamagnetic and Nernst signals in the cuprate Bi-2201 obey therelationH ∗=H ∗c2ln(T/Tc) (Fig. 7), from which the same field scalecan be reliably extracted, and this field scale (proportional to Hc2)decreases with underdoping (Fig. 1b). This resolves the apparentcontradiction highlighted in Fig. 1a.

Critical field Hc2 in YBCOIn YBCO, a cuprate with Tc ≈ 60K at p= 0.11, the effect of su-perconducting fluctuations on the in-plane electrical conductivityσ was analysed up to ε ≈ 1 for a range of dopings7, using theAslamazov–Larkin theory of Gaussian fluctuations. The only fitparameter in the theory is ξ0, plotted in Fig. 5a as Hc2 =80/2πξ 20versus p. Hc2 is seen to have a minimum at p = 0.11, just as inEu–LSCO. In Fig. 5b, we show that this value of Hc2 (obtainedfrom fluctuations above Tc) is in good agreement with the valueof H res

c2 measured at T � Tc directly by high-field transport23,24.H res

c2 is defined as the field where ρ or the Hall coefficient RH orthe Seebeck coefficient S has reached its normal-state value23,24.For example, in YBCO at p= 0.11, S versus H at T = 2K yieldsH res

c2 ≈25 T (ref. 24). A third, independent estimate of the coherencelength ξ0 is the vortex core radiusmeasured bymuon spin relaxationdeep in the vortex state (at low H and T � Tc). In YBCO at

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ARTICLES NATURE PHYSICS DOI: 10.1038/NPHYS2380

0.2 2H (T)

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Figure 4 | Temperature dependence: comparison to Gaussian theory. a, Nernst coefficient ν of Eu–LSCO at p=0.11 as a function of magnetic field H,plotted on a log–log scale for various values of the temperature T as indicated. b, Temperature dependence of the Nernst coefficient in the H=0 limit, ν0,plotted versus reduced temperature ε on a log–log scale. The solid line is the quasiparticle background νqp obtained in Fig. 2. c, Zero-field conductivityσ (=1/ρ) from Supplementary Fig. S3. The dashed line shows the temperature dependence expected from Gaussian fluctuation theory close to Tc (ref. 13).Inset: zoom on the resistivity near the transition. The lower vertical dashed line marks Tc= 3.86 K; the upper vertical dashed line marks T= 1.5Tc.d, Product of ν0 in b and σ in c. Open circles show the effect of subtracting νqp from ν0, to obtain νsc(B→0)= ν0−νqp. The solid line is the theoreticalexpectation for the Peltier coefficient in the B→0 limit, αsc

xy ∼ νscσ , from Gaussian fluctuations of the order parameter in a 2D superconductor14,15. Thedashed line is the expected limiting behaviour close to Tc (ref. 13).

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a b

Figure 5 |Doping dependence of Hc2 in YBCO and Eu–LSCO. a, Upper critical field Hc2 obtained from the superconducting fluctuations above Tc, plottedas a function of hole doping p. For YBCO (blue symbols; left axis), Hc2 is defined via the relation Hc2≡80/2πξ2

0 , in terms of the zero-temperaturecoherence length ξ0 obtained from a Gaussian analysis of the fluctuation magneto-conductivity (ref. 7). For Eu–LSCO (red symbols; right axis), Hc2 is takento be H∗c2 in the fit of the peak field H∗ to H∗=H∗c2ln(T/Tc) (Fig. 3). Error bars on H∗c2 correspond to the uncertainty in fitting to the H∗ data points in Fig. 3c.The red square marks the value of Hc2 obtained directly from resistivity measurements at T→0 on Nd–LSCO, a material very similar to Eu–LSCO(Supplementary Fig. S6). b, Comparison of Hc2 in YBCO determined in two different ways: from ξ0 above Tc (circles), as in a, and from high-field transportmeasurements23,24 (squares) that suppress superconductivity at low temperature (T� Tc). The two measures of Hc2 are in reasonable agreement; inparticular, they both have a minimum at p = 0.11, where Hc2≈ 30 T. The doping dependence of the zero-field Tc is shown for comparison (grey dome, rightaxis; ref. 34).

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NATURE PHYSICS DOI: 10.1038/NPHYS2380 ARTICLES

H/H∗c2

H/H∗c2

/max

()

νν

T = 2 K < Tc

Nsc

(nV

1 )

1 3 5

0 1 2 3 4 50.0

0.5

1.0N

sc/N

sc (

H∗

)

H/H∗

0.100.11Gaussian theory

0

250

500

750

T = 1.5 Tc

0 0.5 1.0 1.5 2.0 2.50.0

0.5

1.0

a

b

Figure 6 | Field dependence: comparison to Gaussian theory. a, Nernstsignal N of Eu–LSCO at p=0.10 (blue; Tc= 5.0 K) and p=0.11 (red;Tc= 3.86 K) as a function of H/H∗, for a temperature T= 1.5Tc. At thistemperature, the peak field H∗, at which Nsc versus H is maximal, isH∗=4.0 T and 3.0 T, respectively. The solid line is a theoretical calculationof αsc

xy (=Nscσ ), as in ref. 15, for a diffusion constant D=0.178 cm2 s−1

(K. Michaeli, personal communication). Note that the experimental σ atT= 1.5Tc is essentially independent of H so that the H dependences of Nsc

and αscxy are the same. The theoretical curve is independent of D when

normalized at H∗, for a wide range of D values (K. Michaeli, personalcommunication; Supplementary Fig. S7). b, Nernst coefficient of Eu–LSCOat p=0.10 (blue) and p=0.11 (red), for a temperature T=2 K<Tc, plottedversus H/H∗c2, where H∗c2 is obtained from the peak field H∗=H∗c2ln(T/Tc)(Fig. 3c). The fact that the data for different dopings collapse on the samecurve when normalized by H∗c2 for both T< Tc and T> Tc (see alsoSupplementary Fig. S8) shows that H∗c2 is the relevant field scalethroughout the H–T phase diagram. Inset: Nsc versus H/H∗c2 for p=0.11 atthe high-field end (up to 34 T), compared against the limiting behaviourexpected theoretically14,15 for αxy =Nscσ at H�Hc2, namelyαxy ∼ 1/Hln(H/Hc2) (solid line).

p ≈ 0.11, the vortex core radius is ≈3 nm, so that Hc2 ≈ 30 T(ref. 25). The fact that three very different measures of Hc2 agreeis compelling evidence that the correct value of Hc2 has beenreached in underdoped YBCO, with a minimum of Hc2 ≈ 30 T atp = 0.11. The agreement also confirms the validity of Gaussiantheory. We conclude that the upper critical field Hc2 of cupratesdecreases with underdoping, in the same non-monotonic fashionin Eu–LSCO and YBCO.

We attribute this non-monotonic weakening of supercon-ductivity to the competing effect of stripe order. Stripe orderis present in Eu–LSCO above p = 0.08 (ref. 26). In YBCO,stripe order was recently inferred from Seebeck measurements ofFermi-surface reconstruction24 and confirmed by high-field NMRmeasurements27. This scenario of phase competition is akin to thatfound in iron-based, heavy-fermion and organic superconductors,

ε = (T¬Tc)/Tc

ε = (T¬Tc)/Tc

ε = (T¬Tc)/Tc

H∗ (

T)

H∗ (

T)

H∗ (

T)

OverdopedH∗c2 = 28 T

UnderdopedH∗c2 = 19 T

Optimally dopedH∗c2 = 24 T

Magnetization

Nernst

a

b

c

30

25

20

15

10

5

00.0 0.5 1.0 1.5 2.0 2.5 3.0

30

25

20

15

10

5

00.0 0.5 1.0 1.5 2.0 2.5 3.0

30

25

20

15

5

0

10

0.0 0.5 1.0 1.5 2.0 2.5 3.0

Figure 7 | Peak field H∗ in Bi-2201. Peak field H∗, plotted versusε= (T−Tc)/Tc, obtained from published data10,20 on the cuprate Bi-2201,for three different dopings: a, overdoped (Tc= 22 K for Nernst10 andTc= 20 K for magnetization20), b, optimally doped (Tc= 28 K for Nernst10

and Tc= 30 K for magnetization20), and c underdoped (Tc= 12 K for bothNernst10 and magnetization20). H∗ is extracted from Nernst data10, as thepeak in N versus H (filled red circles), and H∗d is extracted frommagnetization data20, as the peak in the diamagnetic signal—|Md| versus H(blue squares). In the overdoped and optimally doped samples, where thequasiparticle term Nqp is very small10, H∗ agrees well with H∗d (aboveε≈0.2). In the underdoped sample (Tc= 12 K), however, a large positiveNqp must be subtracted to get a meaningful H∗, as in underdoped Eu–LSCO(Fig. 2). The open red circles are obtained assuming the same Nqp as inunderdoped Eu–LSCO (Fig. 2a); they agree well with the magnetizationdata (blue squares). The solid lines are fits of the Nernst data to theexpression H∗=H∗c2 ln(T/Tc), giving values of H∗c2 as indicated, with errorbars of±5 T. The fits reveal that H∗c2 decreases with decreasing p. Theopposite conclusion would be reached if, as done previously8, the focuswere placed on the Nernst data at T≈ Tc (Fig. 1b), where contamination byfield-dependent paraconductivity is maximal (Supplementary Fig. S4). Theerror bars reflect the uncertainty in determining H∗ from the data of refs 10and 20.

where the competing phase in these cases is spin-density-waveorder. In YBCO at lower doping (p < 0.08), the rapid drop inTc and Hc2 (Fig. 5b) may be due to other phases, such as spin-density-wave order below p≈0.08 (ref. 28) and antiferromagnetismbelow p≈ 0.05. At low doping, the approach to the Mott insulatormay also play a role.

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ARTICLES NATURE PHYSICS DOI: 10.1038/NPHYS2380

MethodsNernst effect. TheNernst effect29 is the development of a transverse electric field Ey

across the width (y axis) of a metallic sample when a temperature gradient ∂T/∂x isapplied along its length (x axis) in the presence of a perpendicular magnetic fieldH(along the z axis). The Nernst signal is N = Ey/(∂T/∂x) and the Nernst coefficientν =N/H . Two mechanisms can give rise to a Nernst signal: superconductingfluctuations, which give a positive signal Nsc, and charge carriers (quasiparticles),which give a signalNqp that may be of either sign. The measured signal is their sum:N =Nsc+Nqp (see Supplementary Information). The superconducting term Nsc

is strongly dependent on the field strengthH , whereas the quasiparticle term Nqp isessentially linear in field (that is, νqp is constant).

Samples. Single crystals of La1.8−xEu0.2SrxCuO4 (Eu–LSCO) were grown by thetravelling floating zone method in Tokyo. The hole doping p is taken to be thenominal Sr concentration x . The characteristics of our four samples are listedin Supplementary Table S1. The superconducting transition temperature Tc wasdetermined as the temperature below which the resistivity ρ= 0. For each sample,three pairs of silver epoxy contacts were diffused into the surface. Contacts used tomeasure the temperature gradient were separated by a distance L and the transversecontacts used to measure the Nernst voltage were separated by a distance w . Theratio L/w was typically in the range 0.5–3.

Single crystals of La1.6−xNd0.4SrxCuO4 (Nd–LSCO) used for determining Hc2

from the resistivity (Supplementary Fig. S6) were described in ref. 30; their Tc andHc2 values are given in Supplementary Table S1.

Electrical resistivity. A standard four-probe method was used to measure theresistivity ρ in zero field. In Supplementary Fig. S3, we show ρ versus T for our fourEu–LSCO samples. Both temperature and doping dependences of the resistivity areconsistent with published data31, as is the magnitude just above Tc (ρ≈ 1m� cm).The resistivity of Nd–LSCO samples is shown in Supplementary Fig. S6.

Nernst measurements. The Nernst effect was measured using a one-heater two-thermometer setup, as described in refs 32 and 33. Themagnetic field, applied alongthe c axis, was swept between−15 and+15 T at a rate of 0.4 Tmin−1 or slower. Also,for Eu–LSCO samples with p=0.10 and 0.125 (p=0.11), the Nernst coefficient wasmeasured up to 28 T (34 T) at the high-field laboratory in Grenoble LaboratoireNational des Champs Magnétiques Intenses (LNCMI). Heat was appliedhorizontally in the ab plane and the temperature gradient dT =1T/Lwas obtainedby measuring the temperature difference 1T between two contacts separated bythe length L, using two uncalibrated Cernox chips referenced to a third calibratedchip. The Nernst voltage Vy =Ey/w across two transverse contacts separated by thelengthw wasmeasured using a nanovolt preamplifier and a nanovoltmeter.

The Nernst signal N is, as the Hall signal, anti-symmetric in field, so thatby taking the difference

N ={(Vy (H )−Vy (−H ))/dT }(L/2w)

any symmetric component is eliminated. For example, contamination from theSeebeck effect due to slightly misaligned contacts is removed in this fashion. Aconstant background coming from themeasurement circuit is also eliminated.

Received 12 April 2012; accepted 26 June 2012; published online12 August 2012; corrected online 28 August 2012

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AcknowledgementsWe thank H. Aubin, K. Behnia, A.M. Finkel’stein, V. Galitski, S. A. Kivelson, K. Michaeli,A. J. Millis, M. R. Norman, M. Serbyn, M. A. Skvortsov, A-M. Tremblay, D. van derMarel, A. Varlamov, and S. Weyerneth for fruitful discussions. We thank S. Y. Li for theresistivity data onNd–LSCO (Supplementary Fig. S6) and J. Corbin for his assistance withthe experiments. We thank K. Michaeli for her unpublished calculations in Fig. 6 andSupplementary Fig. S7.We thank the LNCMI for access to a high-fieldmagnet allowing usto get data up to 28 T (Fig. 2) and 34 T (Fig. 6). J.C. was supported by Fellowships from theFonds de recherche duQuébec—Nature et technologies (FQRNT) and the Swiss NationalFoundation. E.H.was supported by a Fellowship from the FQRNTand a Junior Fellowshipfrom the Canadian Institute for Advanced Research (CIFAR). L.T. acknowledges supportfrom CIFAR and funding from the Natural Sciences and Engineering Research Council ofCanada, FQRNT, theCanada Foundation for Innovation, and aCanadaResearchChair.

Author contributionsJ.C. initiated the project; J.C., N.D-L., O.C-C., F.L., E.H., J-Ph.R. and R.D. performedthe Nernst measurements in Sherbrooke; J.C., N.D-L., F.L., O.C-C. and G.G. performedthe Nernst measurements at the LNCMI in Grenoble; S.P., T.T. and H.T. prepared theEu–LSCO samples and measured their resistivity; J.C., N.D-L. and L.T. analysed the data;J.C., N.D-L. and L.T. wrote themanuscript; L.T. supervised the project.

Additional informationSupplementary information is available in the online version of the paper. Reprints andpermissions information is available online at www.nature.com/reprints. Correspondenceand requests for materials should be addressed to L.T.

Competing financial interestsThe authors declare no competing financial interests.

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In the version of this Article originally published online, the unit on the y axis of Fig. 4c should have read (mΩ–1 cm–1). This error has been corrected in the HTML and PDF versions of the Article.

Decrease of upper critical field with underdoping in cuprate superconductorsJ. Chang, N. Doiron-Leyraud, O. Cyr-Choinière, G. Grissonnanche, F. Laliberté, E. Hassinger, J-Ph. Reid, R. Daou, S. Pyon, T. Takayama, H. Takagi and Louis Taillefer

Nature Physics 8, http://dx.doi.org/10.1038/nphys2380 (2012); published online 12 August 2012; corrected online 28 August 2012.

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