Re-entrant hidden order at a metamagnetic quantum critical end point N. Harrison1, M. Jaime1 and J. A. Mydosh2,3 1National High Magnetic Field Laboratory, LANL, MS-E536, Los Alamos, New Mexico 87545 2Kamerlingh Onnes Laboratory, Leiden University, NL-2300 RA Leiden, The Netherlands 3Max-Planck Institut for Chemical Physics of Solids, N¨othnitzer Str. 40, D-01187 Dresden, Germany 3 Magnetization measurementsofURu2Si2 inpulsedmagneticfieldsof44Trevealthatthehidden 0 orderphaseisdestroyedbeforeappearingintheformofare-entrantphasebetween≈36and39T. 0 Evidence for conventional itinerant electron metamagnetism at higher temperatures suggests that 2 there-entrant phaseis created in the vicinity of a quantumcritical end point. n a PACSnumbers: 71.45.Lr,71.20.Ps,71.18.+y J 6 1 Recent studies of itinerant electron magnetism in URu2Si2 can be explained by a scenario in which the strongly correlated d- and f-electron metals have shown magnetic field first destroys the HO phase before creat- ] that metamagnetism gives rise a new class of field- ing a new field-induced re-entrant phase [4] in the vicin- l e induced quantum phase transition [1, 2]. Sr3Ru2O7, ityofthemetamagnetictransition(seeFig.1foraphase r- CeRu2Si2andUPt3[3]areallconsideredexamplesofsys- diagram). IEM is accompanied by a pronounced asym- t tems that could posses a quantum critical end point, in metry between the occupancy of itinerant spin-up and s . which a notional line of first order phase transitions ter- spin-down f-electron states [15], brought on by the sud- t a minates at zero rather than finite temperature [1]. Here den population of the spin-up component as it sinks be- m we propose that URu2Si2 may be the first example of a low the Fermi energy εF at a magnetic field BM. Mag- - system in which thermodynamic instabilities associated netization measurements reveal that the magnetic field- d with the end point give rise to an ordered phase at high induced phase is accompanied by the opening of a gap n magneticfieldsandlowtemperatures[4]. Thisbehaviour in the spin-up f-electron band at BM. We argue that o is reminiscentofthe creationofsuperconductivity inthe sucha gapcouldbe compatible with a spin-singlet order c [ vicinityofanantiferromagneticquantumcriticalpointin parameter that breaks translational symmetry, of which zerofield[5]. Weshowthatthepresenceofmultiplemag- theorbitalantiferromagnetic(OAF)phase(recentlypro- 2 v netictransitionsinURu2Si2 atlowtemperatures[6,7,8] posed by Chandra et al. [9] to explain the origin of the can be ascribed to re-entrant phenomena arising from HO) is one such example. 4 4 the interplay between itinerant electron metamagnetism Figure 2a shows examples of the magnetization M 2 (IEM)andthehiddenorder(HO)parameterrecentlyat- 1 tributed to orbital antiferromagnetism [9]. of URu2Si2 measured in pulsed magnetic fields of up to 44 T at several different temperatures. The data 0 3 URu2Si2 belongs to a class of stronglycorrelatedmet- areobtainedusingawire-woundsample-extractionmag- 0 als in which f-electrons, rather than being localised and netometer in which the sample is inserted or removed / giving rise to magnetism, develop a distinctly itinerant from the detection coils in-situ. While the experimen- t a character[10]. Coulombinteractionscause the quasipar- tal curves in Fig. 2 appear similar to those measured m ticle effective masses to be heavily renormalised, mak- by other groups [6, 7, 8], the phase diagram obtained - ing the energetic rewards for forming ordered ground- in Fig. 1 upon extracting the positions of the maxima d n states substantially higher than in normal metals [11, in the differential susceptibility χ = µ0∂M/∂B|T at dif- 12]. Indeed, in addition to forming the HO phase at ferent temperatures is markedly different. In a recent o c To 17.5 K [9], URu2Si2 becomes superconducting at study, Jaime et al [4] noted that the magnetocaloric ef- ≈ : Tc 1.2 K [10]. The presence of an itinerant f-electron fect can cause severe variations in sample temperature v ≈ i Fermi surface [13, 14] also furnishes URu2Si2 with the in pulsed magnetic field experiments if the sample can- X essential preconditions for IEM [15], by which the f- not exchangeheat with the bath as the magnetic field B r electronsreverttoalocalisedbehaviourupontheiralign- changes. Thiseffectisparticularlyseriousifthesampleis a ment in strong magnetic fields. IEM is considered to ac- too large, a poor thermal diffusivity isolates the sample, countfortheincreaseinthemagnetizationby 1µBper or if the field is swept too rapidly. Adequate isothermal ≈ U atom at magnetic fields between 35 T and 40 T, equilibrium in pulsed magnetic fields could, however, be ≈ ≈ although the existence of multiple magnetic transitions achieved by using a long-pulse magnet (with a field de- has remained controversial[6, 7, 8]. Recent observations cay constant of 0.25 s) combined with a sample thick- ≈ that local moment antiferromagnetism occurs within a ness of 150 µm [4]. It is by making such provisions in ≃ minority phase that is destroyed by fields in excess of the present study that we obtain a phase diagram that 15 T [9, 16] call for a re-examination of the bulk high agrees more closely with specific heat measurements in magnetic field phenomena in URu2Si2. static magnetic fields [4]. In this paper, we show that multiple transitions in TheexistenceofIEMofasimilartypetothatobserved 2 in Sr3Ru2O7 [17], UPt3 [18, 19] and CeRu2Si2 [20, 21] is itinerantf-electronband is shifted by the Zeeman inter- evidencedattemperaturesabove 6KinFig.2bbythe actiontoenergiesjustbelowεF atBM (seeFig.3),caus- ≈ presence of a single broad maximum in χ . The dashed ingM toundergoadramaticincreasebyasmuchas1µB lineinFig.1indicatesthatthelocationofthisfeatureat per f-electron atom [15]. As a result, f-electrons that BM 37.9Tdoesnotchangesignificantlywithtempera- were mostly itinerant below BM become mostly aligned ≈ ture. The rapid increase in the χ at BM with decreasing and localised at fields above BM. The field BM corre- temperature, shown in Fig. 2c (filled squares), implies sponds to a situation where the Fermi energy εF inter- that the jump in M sharpens with decreasing tempera- sectsthemiddleofthespin-upf-electronbandcausingit ture. Suchbehaviourisconsistentwiththeexistenceofa tobehalfoccupied. Thisleadstoanapproximatelytem- firstordercriticalendpointatafieldBMattemperatures perature independent M at BM (see Fig. 2a) but with χ wellbelow6Kthatisbroadenedbythermalfluctuations increasing dramatically with decreasing temparture (see athighertemperatures[2]. Ratherthandivergingindefi- Fig. 2c). The continuation of the temperature indepen- nitely,however,themaximuminχvanishesbelow 6K dence of M at BM below 6 K, accompanied by an ≈ ≈ on entering the field-induced ordered phase recently in- abrupt reduction in χ, indicates that the field-induced dentifiedinspecificheatmeasurements[4]. Thefactthat orderedphase stabilisesa situationwhereapproximately BM occurs within the field-induced ordered phase im- half of the 5f-electrons become localised while the other plies that fluctuations associatedwiththe metamagnetic halfremainitinerant. Thistype ofbehaviourimplies the critical end-point [1] could play a role in its formation. existence of a charge gap in the spin-up itinerant 5f- Strong fluctuations in the vicinity of quantum critical electron band at εF, at BM. points can cause metals to become highly susceptible to The formation of a charge gap in the spin-up 5f- orderas a means of loweringenergy [1, 2]. A wellknown electron band is consistent with the existence of a spin- exampleisprovidedbythecreationofsuperconductivity singlet order parameter that breaks translational sym- in the vicinity of an antiferromagnetic quantum critical metry. Orderparametersof the charge-densitywave[22] point [5]. andOAF[9]typebothpossessthisessentialproperty;the The intense magnetic fields combined with formation latteralsobreakstimereversalsymmetry. Theybothin- ofthe field-inducedphasebelow 6 KinURu2Si2 make volve singlet pairing of quasiparticles at a characteristic ≈ the process of identifying whether the critical end point translational wavevector Q, where Q is determined by would otherwise terminate at T = 0 less certain than details of the Fermi surface topology [9, 22, 23]. In fact, with Sr2Ru3O7 [1], UPt3 [18, 19] or CeRu2Si2 [20, 21]. regardlessofthe pairingsymmetry,any singletorderpa- This normallyrequires evidence for non-Fermiliquid be- rameterthatinvolvesspatialvariationsinchargedensity, havior. Fortunately, the transitionin the specific heat C orrelativechargedensities betweenone ormoreelectron at 5 K [4] appears to be first order (being of 0.25 K channels, will lead to such a gap. Order parameters of ≈ ≈ in width, albeit without observable hysteresis),implying thistypearealsoamenabletothepossibilityofre-entrant that the region above 6 K is free from thermal fluc- behaviour (see below). Evidence that the HO and field- ≈ tuations of the field-induced HO parameter. This region induced HO phases have a common origin may be pro- cantherefore be investigatedfor non-Fermiliquid effects videdbythefieldandtemperaturedependenceofχ. The associated with IEM [3]. Transport studies are thus far transitionintotheHOphaseisdevoidofanypronounced incomplete, presently yeilding only a broadmaximum in features in the temperature and field dependence of χ at the magnetoresistanceatBM [4]. Thestronglydivergent fields below 34 T, while those into the field induced ≈ behaviour of χ above 6 K in Fig. 2c together with the phase exhibit similar behaviour over a narrow interval ≈ approximately linearly decreasing variation in C/T with between 36.8 and 37.1 T (see Fig. 1). Furthermore, all T [4] at 38 T could, nevertheless, be possible indi- transitions into (or out of) both phases evolve into ones ≈ cations of non-Fermi liquid behaviour. Similar types of that are first order in the limit T 0, although actual → behaviourinotherf-electronsystemshavebeenascribed magnetic hysteresis remains undetected [4]. First order to the presence of a non-Fermi liquid [3]. transitions give rise to pronounced maxima in χ and/or magnetocaloricheatingasthefieldisswept[4]. Somede- ChangesinthevalueofM throughthetransitionspro- greeofsimilaritybetweenthelowandhighmagneticfield vides clues as to the nature of the ordered phase. For B < 25 T, M is weakly dependent on temperature, ex- phasesisalsoapparentinthetemperaturedependenceof hib∼iting a predominantly Pauli paramagnetic response the χ in Fig. 2c at 34.0 T and 37.9 T respectively. typical of heavy Fermi liquids [11, 12]. This, together In order to understand how re-entrance of the HO pa- withspecificheatmeasurementsabovetheorderingtem- rameter can occur, it is instructive first to consider the perature [4] and de Haas-van Alphen measurements be- density of electronic states (DOS) within the ordered low the ordering temperature [13, 14], unambiguously phase for B < 35 T, which has received most atten- establishes the existence of a heavy Fermi liquid with an tion thus far [1, 9]. Figures 3a-e show a schematic of effective Fermi energy of order 10 meV. In the itinerant the evolution of the total DOS with B with (black lines) f-electronpicture,aheavyFermiliquidresultsfrommix- and without (red lines) ordering. At B = 0 (Fig. 3a ing of the f-electrons with regular conduction electron red line), the spin-up and and spin-down Fermi surfaces states [11]. When IEM occurs, the spin-up component are degenerate. The introduction of a periodic charge 3 potential V(r Q0) within the HO phase must therefore developsinthevicinityofBM,enablingtherealisationof · resultintheindependentformationofbandgapsforboth a re-entrant hidden order (RHO) phase with a modified spins (black line). This process is only efficient at min- translationalvectorQ . Strong magnetic fluctuations at ↓ imising the energy of the systems if a significant part BM can be associated with the vanishingly small energy of the DOS is gapped at εF. The introduction of B in thatseparatesspin-upelectronsinlocalisedanditinerant Fig. 3b, however, causes the energies of the spin-up and states at εF [2]. This, combined with the weak disper- spin-down bands to split, leading to spin-up and spin- sion of the spin-up f-electron band, makes the system down Fermi surfaces of different sizes. The efficiency by especially vulnerable to forming an ordered phase. Or- which V(r Q0) can gap both spins therefore becomes deringisespeciallyeasytorealiseiftheperiodicpotential · progressively worsened as B is increased, leading to the V(r Q ) becomes comparable to the bandwidth of the ↓ · weakening of the gap and, eventually, to its destruction spin-up f-electrons, because it will succeed at gapping inamanneranalogoustothatofreachingthePaulilimit the entire spin-up density of f-electron states regardless ofasingletsuperconductor[24, 25,26]. Apreviousmag- of the value of Q and regardless of the absence of well ↓ netoresistancestudy hasprovidedexperimentalevidence definedspin-upmomentumquantumnumbers. Asignifi- for weakening of the gap in fields of 25 T [27]. Ulti- cantamountofenergyisgainedbyopeningsuchagapat ≈ mately,theorderedphasemustbe destroyedatacritical εF, and this wouldthen accountfor the observednarrow field Bc BM, whereupon the spin-up and spin-down gap in the spin-up f-electron band (see Fig. 3d). The ≤ Fermisurfacesbecomeextremelyasymmetric. Theeffect value of Q need only be optimised to match the topol- ↓ ofB ontranslationalsymmetry-breakingspinsinglet or- ogy of the spin-down Fermi surface, which continues to derparametershasbeenextensivelymodeledusingmean be present at BM. Once B > BM, ordinary Fermi liq- field theory [24, 25, 26]. One possibility is that the tran- uid behaviour is expected to be restored, but with the sition evolves into one that is first order that terminates spin-up f-electrons being fully polarized as depicted in at a critical field Bc = ∆0/√2σgµB. Figure 3c depicts Fig. 3e. The pronounced asymmetry between spins in the density of electronic states at Bc where the spin-up theFermiliquidmakestheformationofanorderedphase andspin-downf-electronsstateshavebecomeclearlyre- unlikely, enabling the emergence of a Schottky anomaly solved and singlet gap formation is no longer favoured. in the specific heat [4]. Upon estimating the size of the order parameter using In summary, we presentM data which shows that the the BCS relation 2∆0 = 3.52kBTo [24, 26] and inserting HOparameteris firstdestroyedby Zeemansplitting ina free electron parameters for the spin σ = 1 and g-factor magneticfieldbutthenrestoredinare-entrantphase[4]. 2 g = 2,we obtainBc 32 T.This is of comparableorder The T and B dependence of χ reveals that IEM plays a ≈ to the first order-like transition at 35 T [4] obtained role in its re-entrance,possibly indicating that HO is re- ≈ fromthecurrentmeasurements(seeFig.1)aswellasspe- storedinresponsetomagneticfluctuationsinthevicinity cific heat[4]. Giventhat the product σgµB in f-electron of a metamagnetic quantum critical end point [1, 2]. If systems candepartfromthe free electronvalue [11], this true, this could be the first observation of the creation agreement may be merely circumstantial. However, a of an ordered phase in the vicinity of a magnetic field- further prediction of mean field theory is that both the induced quantum critical end point. We propose the ex- transitiontemperatureTo(B)asafunctionofB [24]and istenceofseparateHOandRHOphasescharacterisedby the critical field Bc(T) as a function of T [26] intersect a common spin-singlet translational symmetry-breaking the axesina perpendicularmanner,andbothcanbe ex- order parameter with slightly different translationalvec- panded in series of even powers of B and T respectively. tors Q0 and Q↓. A plot of T2 versus B2 should therefore yield a line that This work is supported by the National Science Foun- o intercepts both axes in an approximately linear fashion. dation,theDepartmentofEnergyandFloridaState. We This is confirmed in Fig. 3f upon making such a plot thankChristianBatista,Kee-HoonKim,GregBoebinger with actual URu2Si2 data. An interesting situation then and John Singleton for useful discussions. [1] S. A. 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Prior to ordering, mixing between conduction electron states and f-electron states gives rise to a large “Abrikosov-Suhl resonance”-like feature [11]. f A plot of the transition tem- perature squared To2 versus the magnetic field squared B2 taken from specific heat and transport data in Reference [4]. 3.5E-2 B 10 URu Si B || [001] M 2 2 itinerant localised c f-electrons f-electrons 2.0E-2 ) K 5 ( B T c HO RHO QCEP? 0 0 30 40 B (T) Figure 1 of Harrison et al. B (T) 0 10 20 30 40 1.5 a URu Si B || [001] 0.46 K 2 2 ) U 1.0 / B 7 K m( 0.5 8 K M B B c M 0.0 B B b 7 K c M -2 d 1x10 8 K B ~34 T / M 9 K -2 1x10 d 0 -3 5x10 11 K m = c B M c 0 0 35 40 0 10 B (T) T (K) Figure 2 of Harrison et al a b B = 0 0 < B < B c f-electrons ) ) f-electrons e( e( n n broaden HO gap gap narrows e e e e F F c d B = B < B B = B c M M ) (HO destroyed) ) e( e( n n RHO gap e e e e F F e B > B 300 f M ) (RHO destroyed) e( n ) 200 B 2 K M ( B 2 o100 c T 0 e e 0 500 1000 1500 F 2 2 B (T ) Figure 3 of Harrison et al