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Preview Re-entrant hidden order at a metamagnetic quantum critical end point

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. Grigera, R. S. Perry, A. J. Schofield, M. Chiao, 287201 (2002). S. R. Julian, G. G. Lonzarich, S. I. Ikeda, Y. Maeno, [5] N.D.Marthur,F.M.Grosche,S.R.Julian,I.R.Walker, A. J. Millis and A. P. Mackenzie, Science 294, 329-332 D. M. Freye, R. K. W. Haselwimmer and G. G. Lon- (2001). zarich, Nature394, 39-43 (1998). [2] A. J. Millis, A. J. Schofield, G. G. Lonzarich and [6] A. de Visser, F. R. de Boer, A. A. Menovsky and S. A. Grigera, Phys. Rev. Lett. 88, 217204-1−217204-4 J.J.M.Franse,SolidStateCommun.64,527-530(1987). (2002). [7] T.SakakibaraandH.Amitsuka,JapaneseJournalofAp- [3] G. R. Stewart, Rev. Mod. Phys. 73, 797-855 (2001) and plied Physics Series 8, 240 (1993). references therein. [8] K. Sugiyama, M. Nakashima, H. Ohkuni, K. Kindo, [4] M.Jaime, K.H.Kim,G.Jorge, S.McCall, D.G.Hinks, Y. Haga, T. Honma, E. Yamamoto and Y. Onuki, J. A.A. Menovsky and J. A. Mydosh, Phys. Rev.Lett. 89 Phys. Soc. Japan 68, 3394-3401 (1999). 4 [16] T. E. Mason, W. J. L. Buyers, T. Petersen, A. A. Men- FIG. 1: The B > 30 T versus T phase diagram of URu2Si2 ovsky and J. D. Garret, J. Phys.: Condens. Matter 7, combinedwithacolourintensityplotofχmeasuredatmany 5089-5096 (1995). different temperatures. Square, triangle and circle symbols [17] R. S. Perry, L. M. Galvin, L. Capogna, A. J. Schofield, mark BM and transitions into and out of the HO and RHO A. P. Mackenzie, M. Chiao, S. R. Julian, S. I. Ikeda, hidden order (RHO) phases respectively. The curved dotted S. Nakatsuji, Y. Maeno and C. Pfleiderer, Phys. Rev. linesdepictthecontinuationofthephaseboundariesrevealed Lett. 86, 2661-26664 (2001). by specific heat and transport studies [4]. [18] K. Sugiyama, M. Nakashima, M. Futoh, H. Ohkuni, T.Inoue,K.Kindo,N.Kimura,E.Yamamoto,Y.Haga, T. Honma, R. Settai and Y. Onuki, Physica B 281 & FIG.2: a,M ofURu2Si2atseveraldifferenttemperaturesfor 282 244-246 (2000). B applied alongthec-axis. b,χin thevicinityofBM at sev- [19] P.H.FringsandJ.J.M.Franse,Phys.Rev.B31,4355- eraltemperaturesabovethere-entrantorderingtemperature. 4360 (1985). c χ at BM and at B≈ 34 T as a function of T. [20] J. Flouquet, P. Haen, S. Raymond, D. Aoki and G. Knebel, Physica B 319, 251-256 (2002). [21] P.Haen,J.Flouquet,F.Lapierre,P.Lejay,G.Remenyi, [9] P.Chandra,P.Coleman, J. A.Mydoshand V.Tripathi, J. Low Temp. Phys. 67, 391-419 (1987). Nature417, 881-884 (2002). [22] G.Gru¨ner,DensityWavesinSolids,FrontiersinPhysics [10] T. T. M. Palstra, A. A. Menovsky, J. van den Berg, 89 (Addison-Wesley Publishing Company, 1994). A. J. Dirkmaat, P. H. Kes, G. J. Nieuwenhuys and [23] S. Chakravarty, R. B. Laughlin, D. K. Morr and J. A. Mydosh,Phys. Rev.Lett. 55, 2727-2730 (1985). C.Nayak,Phys.Rev.B63,094503-1−094503-10 (2001). [11] A. C. Hewson, The Kondo Problem to Heavy Fermions, [24] W. Dieterich and P. Fulde, Z. Physik 265, 239-243 (Cambridge University Press, 1993). (1973). [12] G. R.Stewart, Rev.Mod. Phys. 56 755-787 (1984). [25] D. Zanchi, A. Bj´elis and G. Monatmbaux, Phys. Rev. B [13] H.Ohkuni,T.Ishida,Y.Inada,Y.Haga, E.Yamamoto, 53, 1240-1250 (1996). Y.OnukiandS.Takahashi,J.Phys.Soc.Japan66,945- [26] N. Harrison, Phys.Rev.Lett. 83, 1395-1398 (1999). 948 (1997). [27] S.A.M.Mentink,T.E.Mason,S.Su¨llow,G.J.Nieuwen- [14] N. Keller, S. A. J. Wiegers, J. A. A. J. Perenboom, huys,A.A.Menovsky,J. A.Mydosh,J. A.Mydosh and A. de Visser, A. A. Menovsky and J. J. M. Franse, J. J. A. A. Perenboom, Phys. Rev. B 53, R6014-R6017 Magn. Magn. Mater. 177, 298-299 (1998). (1996). [15] D. M. Edwards and A. C. M. Green, Z. Phys. B 103, 243-249 (1997). 5 FIG. 3: a-e Schematics of the evolution of the total DOS in URu2Si2 with B (as indicated) before (red lines) and after (black lines) formation of the HO or RHO phases. 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

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