Crossover from Thermal Activation to Quantum Interlayer Transport at the Superconducting Transition Temperature of Bi Sr CaCu O 2 2 2 8+δ ∗ S. O. Katterwe, A. Rydh, and V. M. Krasnov Department of Physics, Stockholm University, AlbaNova University Center, SE-10691 Stockholm, Sweden (Dated: February 2, 2008) Weperform adetailed studyof temperature,bias anddopingdependanceofinterlayertransport in the layered high temperature superconductor Bi2Sr2CaCu2O8+δ. We observe that the shape of 8 interlayer characteristics in underdoped crystals exhibit a remarkable crossover at the supercon- 0 ductingtransition temperature: from thermalactivation-typeatT >Tc,toalmost T−independent 0 quantum tunneling-type, at T < Tc. Our data indicates that the interlayer transport mechanism 2 may change with doping: from the conventional single quasiparticle tunneling in overdoped, to a progressively increasing Cooper pair contribution in underdoped crystals. n a PACSnumbers: 74.72.Hs74.45.+c74.50.+r74.25.Jb J 8 1 How does the high temperature superconductivity constrains on the nature of the c−axis pseudogap. In (HTSC) emerge with decreasing temperature? This the supplementaryinformation[15]wediscuss singleQP ] n highly debated question is crucial for understanding the characteristics, self-heating and clarify determination of o mechanism of HTSC. The superconducting transition in parameters. c HTSC appears to be unusual, with a seeming lack of We study two batches of crystals: the Y-doped Bi(Y)- - r changes in the quasiparticle (QP) density of states at 2212withthemaximumTc ≃94.5KandthepureBi-2212 p Tc and persistence of the normal state pseudogap above withthemaximumTc ≃86K.Detailsofmesafabrication u s Tc [1, 2]. However, there is no consensus about the and characterizationare described elsewhere [7, 8, 13]. . T−evolutionof the energy gap. Results obtained by dif- Figs. 1 a) and b) show the T− variation of I−V and at ferent experimental techniques range from complete T− dI/dV(V) curves for a Bi-2212 mesa, containing N = 7 m independence of the superconducting gap, ∆SG, in the intrinsic Josephson junctions, see Fig. 1 c). The follow- - whole T− range [3], to strong T−dependence at T =Tc ingcharacteristicfeaturesareseenindI/dV curves: The d [4, 5, 6, 7, 8, 9]. In some experiments, coexistence of sharp ”coherence” peak appears at T < T and is, in c n o the twoenergy scalesbelow Tc wasreported[7, 8, 9, 10]. analogy with conventional low-Tc junctions, attributed Theexistingcontroversyisoneofthemajorobstaclesfor to the sum-gap voltage V =2N∆ /e [7, 8, 11, 14]. A c g SG [ understanding HTSC andrequires further T−dependent broader hump is seen in the whole T− range and is at- studies. tributed to the c− axis pseudogap[7, 8, 11]. At elevated 1 Intrinsictunnelingspectroscopyutilizestheweakinter- T thedI/dV curvescrossinnearlyonepoint[8,14]. The v 1 layer (c−axis) coupling in layered HTSC. Unlike surface T−dependence of these features is plotted in Fig. 1 d) 2 probe techniques, it is perfectly suited for T−dependent Figure 2 a) shows dI/dV(V) curves (in a semi-log 9 studies and provides information about bulk electronic scale) for the most underdoped Bi(Y)-2212 mesa with 2 propertiesofHTSC.Inrecentyearsdifferentwaysofim- N = 34 junctions. The thin and thick lines in Fig. 2 a) 1. proving this technique were employed [7, 8, 11, 12, 13, represent dI/dV(V) curves below and above Tc, respec- 0 14]. Yet, interpretation of intrinsic tunneling character- tively. It is seen that the shape of interlayer characteris- 8 istics may not be free from misconceptions, associated tics exhibits a remarkable qualitative change at Tc: 0 bothwiththeproblemofself-heating[15]andthelackof (i)AboveT theslopeofln[dI/dV](V)curvesdecreases c : v completeunderstandingoftheinterlayertransportmech- withincreasingT,whilethevoltagescaleremainsalmost i anism. the same. The curves lean towards the horizontal line X Herewestudytemperature,biasanddopingdependen- dI/dV =σN, correspondingto the normalstate conduc- ar ciesofintrinsictunnelinginsmallBi2Sr2CaCu2O8+δ (Bi- tance, and cross almost in one point. 2212) mesa structures. We observe an abrupt crossover (ii) Below Tc the ln[dI/dV](V) curves have the same in the shape of current-voltage characteristics (IVC’s), T−independent slope. With increasing T the curves re- from thermal activation (TA) like at T > T , to main parallel and move towards the vertical axis V = 0 c T−independent quantum tunneling like at T < T . Our (i.e., the voltage scale decreases). c data indicates that the interlayer transport mechanism ExperimentalcurvesfromFig. 2a)haveacharacteris- inBi-2212changesinunderdopedBi-2212,togetherwith tic V-shape with voltage-independent slope. The overall development of the pseudogap. The observed simple TA shape of the curves at T >Tc closely resembles thermal behavior in the whole normal state region puts strong activationcharacteristics[16],whichcanbe describedby a simple expression [15]: dI n(T) U eV (T,V)∝ exp − TA cosh , (1) ∗Electronicaddress: [email protected] dV T (cid:20) k T(cid:21) (cid:20)2k T(cid:21) B B 2 FIG.1: (Coloronline). a)I−V andb)dI/dV(V)characteris- ticsforaBi-2212mesaatdifferentT. c)Periodicquasiparticle FIG.2: (coloronline). a)Asemi-logplotofdI/dV(V)curves branches. d)Temperaturedependenceofthepeak,humpand foranunderdopedBi(Y)-2212mesaatdifferentT. Notethat crossing voltages (perjunction). below Tc the curves maintain the same slope, while above Tc the slope changes progressively with T. A characteristic crossingpointofdI/dV(V)curvesatT >Tcismarkedbythe where n is the concentration of mobile charge carriers, arrow. b)Theeffectivetemperature,obtainedfromtheslopes ofthedI/dV(V)curvesatafinitebiasV/N =30mV [15]. A andU is the TAbarrier. Indeed, the cosh termrepro- TA remarkable crossover from the thermal activation, T =T, duces the rounded V-shape of ln[dI/dV](V) curves with eff the slope that monotonously increases as 1/T. to quantum,Teff =const,behavior occurs at Tc. InFig. S10[15]weshowthatthedatafromFig. 2a)in thewholenormalstate,T >T ,isverywelldescribedby c Eq.(1) with constantU ≃24meV andT−linearn(T). (the exp term in Eq.(1)). Experiments on small mesas TA It also reproduces the crossing point [16], which accord- provide a possibility to measure the small-bias QP re- ing to Eq.(1) occurs at eV ≃ 2U . Apparently, the sistance, RQP, in the superconducting state [11, 12, 19], TA TAbarriershouldbe associatedwiththec−axispseudo- whichisotherwiseshuntedbythesupercurrent[20]. This gap. Thus,theappearanceofthecrossingpointissimply isfacilitatedbythe largespecific capacitance(highqual- the consequence of a fairly T−independent c−axis pseu- ity factor) of intrinsic junctions [18], which causes the dogap [1, 3, 7, 8], while the crossing voltage represents pronounced hysteresis in the IVC’s and allows junctions the pseudogapenergy. Indeed, a correlationbetween the to remain in the resistive state even below the critical hump and the crossing voltages is seen from Fig. 1 d). current,seeFig. 1c). Therefore,biasyieldanadditional According to Eq.(1) the slope of the curves in Fig. parameter for our studies, which may render crucial for 2 a) should be proportional to the reciprocal temper- correct interpretation of the data. ature: d/dV(ln[dI/dV]) = (e/2k T)tanh(eV/2k T) ≃ Fig. 3a)showsthedc−resistanceR =V/I atdiffer- B B dc e/2k T. Fig. 2 b) shows the effective temperature, ent I for the same Bi-2212 meas as in Fig. 1. Measure- B T , obtained from the slopes at V/N =30mV [15]. It ments were done by first applying a large current, suffi- eff is seen that in the normal state T ≃ T, confirming cient for switching to the last QP branch, see Fig. 1 c), eff the TA nature of interlayer transport at T > T . How- and then ramping it back to the desired value. The R c dc ever, at T < T an abrupt saturation of T (T) oc- at the smallest current I = 5µA coincides with the con- c eff curs, typical for quantum tunneling transport [17, 18]. ventional ac− resistance, R . It drops at T < T , since ac c This is the central observation of this work. Remark- the finite quality factor of the junctions causes retrap- ably, the crossover is clearly distinguishable at T → T , ping to the superconducting branch at a finite current c althoughno other spectroscopicfeatures can be resolved [18]. From Fig. 3a) it is seen how non-linearity develops in dI/dV(V) curves. with decreasing both bias and T. At small I the curves So far we discussed dI/dV(V) at finite bias. Another approach an asymptotic, allowing a confident estimate straightforward way to investigate the TA behavior is of the zero-bias quasiparticle resistance, RQP, without a 0 to consider T−dependence of zero-bias resistance, R0, need for extrapolation. 3 1000 R QP UD(T=85K), c 0 OP(93K), 100 OD(92.5K). R K) TA / Ω ( Bi(Y)-2212 T 10 /0 2 OD(92.5) R A T R OP (93) 1 R/01 R ac UD (85) 0.01 0.02 0 0.03 0.04 50 100 150 200 1/T (K-1) T (K) FIG.4: (Coloronline). T−normalizedzero-biasquasiparticle resistance, R0QP,extrapolated from IVC’sat T <Tc andRac measured with a small ac-current for Bi(Y)-2212 mesas with FIG. 3: (Color online). a) T− dependence of the dc− resis- different doping. Dashed lines represent TA fits, Eq.(1), at tance at different bias currents for the same Bi-2212 mesa. T > Tc. Inset shows relative values of the excess QP resis- Panels b-d) show the asymptotic zero bias resistance: b) in tance with respect to theTA fit of thenormal state. A large the double-logarithmic scale; c) as a function of 1/T; and d) excess resistance appears below Tc in the overdoped mesa. normalized by T: a clear linear thermal activation behavior The excess resistance rapidly decreases with decreasing dop- (dashed line) is observed in the whole normal state region. ing and becomes negative in theunderdoped mesa. The RQP grows with decreasing T at T < T , and (OP)mesaandturns negative alreadyinmoderatelyun- 0 c is usually described either in terms of power-law depen- derdoped (UD) mesas. dence [20], inherent for single QP tunneling in the pres- Inset in Fig. 4 shows the magnitude of the excess QP ence of a d−wave gap (see Fig. S7 [15]), or in terms of resistance with respect to the TA fit, R , in the nor- TA TA [21]. The double-logarithmic plot, Fig. 3 b), demon- mal state (dashed lines). The quality of the fit could strates that R0(T) is not described by the power law in be judged from the flatness of the normal state region. any extended T−range for our mesas. Neither is it per- A progressive decrease of the excess QP resistance at fectly described by the Arrhenius law exp(UTA/kBT), T <Tc with decreasing doping is obvious. as demonstrated in Fig. 3 c). On the other hand, Fig. Westartdiscussionoftheobservedphenomenabyrec- 3 d) demonstrates that the ratio R0/T follows very ac- ollecting the expected T−variationfor conventionalsin- curately the Arrhenius law (dashed line) in the whole gle QP tunneling characteristics. As discussed in sec. I normal region, consistent with the TA expression Eq.(1) of the supplementary information, provided the physi- and with the finite bias behavior,Fig. 2 b). However,at cal requirement that ∆ and the quasiparticle lifetime SG T <T , RQP/T deviates downwardsfrom the Arrhenius increasewith decreasingT,allsingleQPtunneling char- c 0 law. This is consistent with saturation of the effective acteristics (including d−wave) exhibit the following uni- T (T < T ), as shown in Fig. 2 b). Therefore, it is a versal T−dependence: eff c consequence of the same crossover. A) Opening of the superconducting gap at T < T c In Fig. 4 we analyze doping dependence of R0(T)/T. leadstoappearanceofthelargeexcessQPresistancedue In the normal state, R0(T) varies in the TA manner for torapidfreezingoutofQP’supontheircondensationinto alldopinglevels. Inthesuperconductingstate,RQP also Cooper pairs (see inset in Fig. S7 [15]). 0 continues to grow with decreasing T, but the rate of the B)RQP continuestogrowwithdecreasingT bothdue 0 growth with respect to the TA behavior, RTA, (dashed tofreezing-outofthermalQP’sanddue togrowthofthe lines) strongly depends on doping: QPlifetime,whichdecreasesthenumberofavailablesub- For the overdoped (OD) mesa, RQP(T < T ) grows gap QP states. All this leads to a progressive growth of 0 c muchfasterthaninthenormalstate,i.e.,thereisasharp the slopeofdI/dV(V)characteristicswithdecreasingT. onset of the excess resistance at T = T . However, the The sudden appearance of excess resistance at T <T c c excess resistance at T < T decreases rapidly with un- in OD mesas indicates that the superconducting transi- c derdoping. Itbecomessmallinthenearoptimallydoped tionhereisconventional,inasensethatitisaccompanied 4 by opening of the superconducting gap, and is also con- shots in underdoped Bi-2212 could arise from doping- sistentwithsingleQPtunneling mechanismofinterlayer dependent nano-scale inhomogeneity, observed at the transport. surfaceofBi-2212[26,27], whichinthis caseshouldper- However, the superconducting transition in under- sists also in the bulk of Bi-2212 crystals. doped mesas is clearly abnormal. We emphasize again Such interpretation implies that not only the elec- thatappearanceofthenegativeexcessresistanceandthe tronicstructure,butalsothec−axistransportmechanism crossover to T−independent slope reflect the same phe- changeswithunderdoping: fromcoherentanddirectional nomenon at zero and finite bias, respectively. Therefore, [15] single QP tunneling in overdoped, to progressively any explanation of the observed unusual T−dependence increasingpaircontributioninunderdopedBi-2212. The must account for both zero and finite bias behavior. latter is apparent only in the phase coherent state at At the first glance, the lack of excess resistance at T <Tc,isalmostT−independent,andisconsistentwith T < T in UD mesas could be consistent with the pre- multiple Andreev reflection mechanism of the interlayer c cursor superconductivity scenario of the pseudogap [3], transport. according to which the gap does not open and QP’s do Finally we note that the reported amazingly trivial not start to pair at T , but at much higher T∗. Then thermalactivationbehaviorinthewholenormalstatere- c onecouldarguethatthe lackofexcessresistancereflects gion, puts strong constrains on the nature of the c−axis simply the lack of dramatic changes in the QP spectrum pseudogap. Even though, the similar TA-behavior can upon establishing of the global phase coherence at T . be ascribed to several processes (e.g., inelastic tunneling c However, the same argument would make it difficult to via the impurity [27, 28], or elastic tunneling via a reso- explain the abrupt crossover to T−independent slope. nant[29]stateinthetunnelbarrier,orCoulombblocking Furthermore, as we noted above, the slope of dI/dV(V) of tunneling [7]), it does not involve any gap, nor angu- should continue to increase with decreasing T for single lardependenceintheQPspectrum,butassumesinstead QP tunneling. Therefore, the observed crossover to con- thatthereissomeconstantblockingbarrierforinterlayer stantslopecanhardlybeexplainedintermsofsingleQP hoping [16]. This may indicate that the ”large” c−axis tunneling [15]. pseudogapisnotapairinggap,whichwouldnaturallyex- plain it’s indifference to such classical depairing factors This conclusion brings us to one possible interpreta- tion of the observedphenomena. If the c−axistransport as temperature and magnetic field [7]. We are grateful to E.Silva for stimulating discussions inUDmesasisnotsolelyduetosingleQP’s,itmustalso and to A.Yurgens, T.Benseman and G.Balakrishnan for involve pairs. The corresponding multi-particle tunnel- providingBi(Y)-2212andBi-2212singlecrystals. Finan- ing [22, 23] and the multiple Andreev reflection [24, 25] processes are well studied for conventionallow−T junc- cial support from the K.&A. Wallenberg foundation and c tions. Bothprocessesaresimilar[25] andarealmostT− theSwedishResearchCouncilisgratefullyacknowledged. independent, becausetheydonotrelyonthepresenceof thermallyexcitedQP’s,butdirectlyinvolveCooperpairs I. SUPPLEMENTARY INFORMATION from the Fermi level. The multi-particle current occurs via elastic conversion (dissociation or recombination) of Cooper pairs into QP’s; while the multiple Andreev re- A. Nomenclature flectionprocessisduetotransmutationofaquasielectron into a quasihole with creation of a Cooper pair and can ARPES:angularresolvedphotoemissionspectroscopy, beuniversallydescribedintermsofinelastictunnelingin Bi-2212: Bi2Sr2CaCu2O8+δ, the presence of time-dependent phase difference due to Bi(Y)-2212: Y-doped Bi-2212, the ac-Josephsoneffect [25]. DoS: density of states, Importantly, the multi-particle processes result in al- ∆: energy gap, mostT−independentandV−exponentialsubgapcurrent ∆T: self-heating, [22, 23], which essentially coincides with the description Γ: depairing factor, reciprocal quasiparticle lifetime; of the observed crossover, see Fig. 2. Furthermore, the HTSC: high temperature superconductor, abruptness of the crossover at T , points towards the I: current, c coherent multiple Andreev reflection mechanism of the IJJ: intrinsic Josephson junction. interlayer current, because it requires the time-periodic IVC: Current-Voltage characteristic, ac-Josephson effect [25] and, consequently, abruptly dis- N: number of IJJ’s in the mesa, appears simultaneously with phase coherence at T . n: concentration of mobile charge carriers, c We may further speculate why the multiparticle pro- OD, OP, UD: overdoped, optimally doped, under- cesses become progressivelymore important with under- doped, respectively; doping. The multiparticle current decrease much faster QP: quasiparticle, than the single QP current with decreasing the interface R0: zero bias resistance (in the normal state), transparency [22, 25]. Therefore, the single QP domi- RQP: zero bias quasiparticle resistance in the super- 0 nates over multiparticle current, unless there are micro- conductingstate,isdifferentfromR0 becauseofthepro- shots in the tunnel barrier [23]. The required micro- nounced hysteresis in the IVC’s at T <T ; c 5 R : tunnel (normal) resistance, In Fig. S5 a) and b) we show numerically simulated n R : thermal resistance of a mesa, SIS characteristics for different single QP tunneling sce- th SIS: Superconductor-Insulator-Superconductor, narios. We assumed, t(ϕ1,ϕ2) =const for incoherent- SIN: Superconductor-Insulator-Normalmetal, nondirectional, t(ϕ1,ϕ2) ∝ δ(ϕ1 − ϕ2) for coherent- STM: scanning tunneling microscope, nondirectionalandt(ϕ1,ϕ2)∝[cos(kx)−cos(ky)]2δ(ϕ1− TA: thermal activation, ϕ2) for coherent-directional tunneling [31]. The simu- lations were made for ∆(ϕ = 0) = 35meV, at low T T : superconducting critical temperature, c and small depairing Γ ≪ ∆(0). Detailed discussion of U : thermal activation barrier, TA dI/dV characteristics can be found in Ref. [30]. Irre- V: voltage, spective of the scenario,the zero-biasresistancediverges Vg: the sum-gap voltage Vg =2N∆/e (the conductance tends to zero) at T → 0 and Γ = 0. ThecapitalM/Sinfrontofthefigureorequationnum- The divergence is removed by the finite Γ, see the inset berindicatesthatthereferenceismadetotheManuscript in Fig. S6 b). Therefore, dI/dV(V = 0,T → 0) pro- or the Supplementary information, respectively. videsthe informationaboutthe value ofΓ. We alsonote that dI/dV(V) characteristics exhibit a sharp peak at the sum-gap voltage V = 2∆/e ( except for the curve g B. Influence of the quasiparticle life time on dI/dV A). characteristics It is expected that interlayer QP tunneling in Bi-2212 single crystals should be predominantly coherent (pro- We have argued in the manuscript that the observed videdthatthe singlecrystalis pureenoughsothatthere crossovertoT−independentslopeandthecorrelatedap- isnomomentumscatteringupontunneling)andstrongly pearanceofthenegativeexcessresistanceareinconsistent directional,withdominatingantinodaltunneling[31,32]. with the single QP tunneling mechanism of the c−axis Indeed, the curve C in Fig. S5 resembles most closely transport. However, the interlayer tunneling in Bi-2212 the experimental characteristics (cf. with the curves at may depend on a number of parameters [30, 31, 32]: T = 13.4K from Fig. M1a and b), see also a discussion in Refs. [30, 34]. (i)TheQPlife time,1/Γ,which,accordingtoARPES data,hasasubstantialT−dependencecloseto T ,where In what follows, we will analyze the incoherent- c it increases roughly linearly with T; [9, 33] nondirectional single QP tunneling characteristics, rep- resenting an ”extreme” d−wave case with the weakest (ii)Momentumconservationupontunneling(coherent sum-gappeak. The conclusionswill, however,be univer- vs. incoherent tunneling); (iii) The directionality of c−axis tunneling, i.e., the sal for any single QP tunneling scenario. angular dependence of the tunneling matrix element NowweconsidertheeffectofT (pointiv)andΓ(point t(ϕ1,ϕ2), caused by a non-spherical Fermi surface [31, i) on dI/dV characteristics. It is clear that both param- 32]. eters will smoothen dI/dV(V) characteristics and fill-in the dip in conductance at V =0. However, they do this (iv) Temperature and (v) angular dependence of the in a slightly different manner. This is illustrated in Figs. gap in the DoS and the points (i-iii) above. Deviations from pure d−wave symmetry were reported in recent S6 and S7. ARPES experiments [9]. TheincreaseofΓ leadstosmearingofthe QPgapsin- gularity and simultaneous filling-in of the sub-gap states It may not be obvious that experimental data can not in DoS, Eq.(S2). This naturally leads to smearing of bedescribedbythesingleQPtunnelingwithafortunate the sum-gappeak and to filling-in of the zero-biasdip in combination of all those parameters. Therefore, below dI/dV, as shown in the inset in Fig. S6 b). we want to dwell upon this statement. TheincreaseofT leadstothedecreaseof∆. Bothfac- We start with considering the consequences of points torsresultintheincreasednumberofexcitedQP’sabove (ii, iii) and (v), i.e., coherence and directionality of tun- the gap, which leads to rapid filling-in of the zero bias neling and the symmetry of the order parameter. The dip in conductance. However, the increase of T (unlike single QP tunneling current is given by: Γ) keeps the gap singularity in DoS unchanged. From 2π 2π +∞ Fig. S7 it is seen that this leads not only to filling-in I(V)= dϕ1dϕ2dE (2) of the dip, but also to development of the maximum at Z0 Z0 Z−∞ V = 0, representing the so called zero-bias logarithmic t(ϕ1,ϕ2)ρ(E,ϕ1)ρ(E+eV,ϕ2)f(E)[1−f(E+eV)], singularity [35]. Theoriginofthesingularityisverysimple: atelevated where E is the energy of the QP with respect to the T thereisasubstantialamountofthermallyexcitedQP’s Fermisurface,ϕ1,2aretheanglesinthemomentumspace just above the gap. At V = 0 the partly filled gap sin- of the initial and the final state of the QP, and ρ(E,ϕ1) gularities in the two electrodes are co-aligned, causing a ρ(E+eV,ϕ2) are the corresponding QP DoS: largecurrentflowfromoneelectrodetoanother,whichis exactlycompensatedbythe counterflowfromthe second ρ(E,ϕ)=ℜ[(E−iΓ)/ (E−iΓ)2−∆(ϕ)2], (3) electrode. However,exactcancelationisliftedatanarbi- p 6 Incoherent, a) non-directional d-wave tunneling. V) 70 T = 5K, 0.5, m ∆(T) = 35 meV. 3.2, ( R n 5.8, I 35 Γ = 11.1 (meV) 21.6, 40.0, 63.7. 0 0 35V (m V) 70 n b) R V 1 d I/ d 1 T = 5K n R 0,1 (0) 0,1 Γ 1.36 V d I/0,01 Γ (meV) d 1 10 0,01 0 35 V (mV) 70 FIG. 5: (Color online). Simulated single QP characteris- FIG.6: (coloronline). Effectofthedepairingfactoronsingle tics for different tunneling scenarios. A: incoherent, non- QP characteristics. Shown are simulated characteristics at directional, d−wave; B: coherent, non-directional, d−wave; constantT and∆forvaryingΓ. IncreaseofΓtendstoreduce C: coherent, directional, d−wave; D: s−wave. Note that the theslopeofdI/dV characteristics. Insetinpanelb)indicates sharpsum-gappeakandthehalf-gapsingularityindI/dV are that filling-in of the zero bias dip with Γ occurs in a power inherent to most scenarios. law manner. trarysmallvoltageacrossthejunction,leadingtoasharp maximum in dI/dV. From Fig. S7 it is seen that the zero-bias maximum in d−wave junctions is pronounced even in the extreme case of weakest sum-gap peak. We havecheckedthatthezero-biaslogarithmicsingularityis inherent for single QP characteristics,irrespective of the It is impossible to maintain the slope under the physical tunneling scenario. requirements that Γ increases and ∆ decrease simulta- Interestingly, the experimental characteristics do not neously with increasing T because all of the three pa- exhibit the zero-bias logarithmic singularity, see Fig. rametersworkinthe samedirection-decreasetheslope. M2a). Within the single QP tunneling scenario this is The inset in Fig. S7 shows the calculated zero bias re- only possible if the depairing factor increases with T at sistance vs. 1/T for incoherent, non-directional,d−wave sucharate thatit smearsoutthe gapsingularityinDoS single QP tunneling and different Γ. It is seen that a and thus suppresses development of the singularity. We prominentexcessresistanceappearseveninthisextreme estimate that the corresponding Γ at T = Tc should be d−wave case and even for very large Γ. The dashed line in the range 2-5 meV, somewhat smaller than deduced shows that the excess resistance grows approximately as from ARPES [9, 33]. T−2 in this case. The abrupt appearance of the excess Now we can substantiate our statement. In Fig. S8 QP resistance is a mere reflection of the abrupt opening we show the attempt of maintaining the same slope of of the superconducting gap at T . Therefore, the ob- c lndI/dV(V)curvesforprogressivelydecreasing∆. Since served T−independent slope and the absence of excess increaseofbothΓandT leadstofilling-inofthezerobias resistance, observed for UD mesas, are inconsistent with dip, i.e., to decrease of the slope, the slope can be main- the single QP tunneling and points towards the doping- tained only if Γ and T move in the opposite directions. dependentchangeintheinterlayertransportmechanism. 7 where P = IV is the dissipated power and R is the th effective thermal resistance of the junctions, which is T−dependent and, therefore, bias dependent [36]. The 1 influence of self-heating on IVC’s of our mesa structures n IVRd/d 0,1 2.0 K,RR / 0n10 Γ25(0,T ,0c )1.1(0m, eV)= waFiadgsi.stc3huofsrrsooiomungRholfeyfs.cs[7atu]l)idn.igedofinIVRCe’fss.i[n34th,e36in,s3e7t,o3f8F]i(gs.ee1aalnsdo Despite relative simplicity of the phenomenon, discus- 24.8 K, T -2 0,01 47.6 K, sionofself-heatinginintrinsictunnelingspectroscopyhas 62.8 K, 1 causedaconsiderableconfusion,alargepartofwhichhas 78.0 K, 0,00 10/,T02 (K-10),04 been caused by a series of publications by V.Zavaritsky 1E-3 93.2 K. [39], in which he ”explained” the non-linearity of intrin- 0 35 70 V (mV) sictunneling characteristicsbyassumingthatthereisno intrinsic tunneling. The irrelevance of this model to our subject was discussed in Ref.[38]. A certain confusion might be also caused by a large spread in R , reported by different groups [14, 36, 40, th FIG. 7: (color online). Effect of T and ∆(T) variation on 41, 42]. For the sake of clarity it should be empha- single QP characteristics. Calculations were made for inco- sized that those measurements were made on samples herent, non-directional, d−wave tunneling, the experimental of different geometries. It is clear that R depends ∆(T) dependence and linear Γ(T). Note that increase of T th strongly on the geometry [36, 37], e.g., R can be anddecreaseof∆leadsnotonlytosmearingofdI/dV charac- th teristics, butalsotheappearanceofthelogarithmiczero-bias much larger in suspended junctions with poor thermal singularity. Inset shows the zero bias resistance vs. 1/T for link to the substrate [42] than in the case when both different values of Γ(Tc). It is seen that the excess QP resis- top and bottom surfaces of the junctions are well ther- tance rapidly develops at T <Tc even in thed−wavecase. mally anchored to the heat bath [14]. For mesa struc- tures similar to those used in this study (a few µm in- plane size, containing N ≃ 10 IJJ), there is a consensus that R (4.2K) ∼ 30−70K/mW (depending on bias) th [36, 41] and R (90K)∼5−10K/mW [36]. Larger val- th ues R > 100K/mW claimed by some authors [40] are th 1 unrealisticforourmesasbecausetheycanwithstanddis- Incoherent, sipatedpowersinexcessof10mW withoutbeingmelted. n R non-directional Yet,wenotethattalkingaboutatypicalvalueofR is Vd d-wave tunneling. equallysenselessastalkingaboutatypicalvalueofacthon- I/ Γ =1, ∆=35 (meV), T= 59K; tact (Maxwell) electrical resistance: both depend on the d Γ =2, ∆=35 (meV), T=55.2K; geometry. Therefore, reduction of mesa sizes provides Γ =5, ∆=35 (meV), T= 36.2K; a simple way for reduction of self-heating [37]. Conse- 0,1 Γ =5, ∆=17.5 (meV), T= 32.4K; quently,variationofdI/dV characteristicswiththejunc- Γ =7, ∆=10 (meV), T= 0.1K. tion size and geometry provides an unambiguous way of 0 35V (mV) 70 discriminating artifacts of self-heating from the spectro- scopic features [36]. How self-heating can distort the IVC’s of Josephson junctions is obvious: since self-heating rises the effective T it may affect the IVC only via T−dependent parame- FIG. 8: (Color online). An attempt to maintain the slope of ters. There are three such parameters: the quasiparticle single QP characteristics at different T. It is seen that the resistance,thesuperconductingswitching[18,43]current slope can be maintained only under the un-physical require- andthe superconducting gap. They will affect the IVC’s ment that Γ increases and ∆ decreases with decreasing T. of Bi-2212 mesas, containing several stacked Josephson junctions, in the following manner: The consecutive increase of T upon sequential switch- C. Analysis of self-heating and non-equilibrium ing of IJJ’s from the superconducting to the resis- phenomena tive state will distort the periodicity of quasiparticle branches. Each consecutive QP branch will have a Self-heating can distort IVC’s of Josephson junctions smallerQPresistance(smallerV atgivenI)andsmaller atlargebias. The temperature rise due to self-heating is switchingcurrent,seethediscussioninRefs. [7,38]. This given by a simple expression type of distortion of the QP branches becomes clearly visible (at base T =4.2K) when ∆T &20K [37, 38]. ∆T =PR (T), The T−dependence of ∆ may lead to appearance of th 8 of self-heating the ”measured” gap vanishes at T = T , c i.e., simultaneously with the true gap. Thus trivial self- T(K)=90,80,70,50,30,4.2 T(K)=90,80,70,50,30,4.2 heating simply can not ”hide” the qualitative ∆(T) de- V) 80 without V)80 0 with pendence. Forexample,thereisnowayinwhichonecan m 60 self-heating m60 self-heating get the vanishing ”measured” (self-heating affected) gap R (N40 R (N40 ifthetruegapisT−independent. Therefore,thediscrep- I I ancy in the measured strong T−dependence of the gap 20 a) 20 b) at T in intrinsic tunneling (and recent ARPES [9]), or c 0 0 completeT−independenceinSTMmeasurements[3]can 0 20 40 60 80 0 20 40 60 80 V (mV) V (mV) not be attributed to self-heating. 60 To quantitatively analyze the significance of self- T(K)=90,80,70,50,30,4.2 d) 120 0 V)50 heatinginourmesas,weprovidevaluesofthedissipation T (K) 4800 e∆2/ (m234000 w withitho ut gBpaoi(pwYep)r-e2Pa2k1=2isImV0e.s8af2omratWthTe. s=tFur4do.i9meKdtmhdeeisssapispr:eavtFiiooornustahtaentanhleeyasrsi-usOmoP-f c) 10 self-heating the size dependence of V for similar mesas [36] it was g 0 0 observed that V becomes size-independent, and there- g 0 20 40 60 80 100 0 20 40 60 80 V (mV) T (K) fore not affected by self-heating, for small mesas with P(V )<1mW. Allthe mesasstudiedinthismanuscript g fall into this category. All of them exhibit perfect pe- riodicity of quasiparticle branches [7] and none of them exhibit back-bending at any T, which according to Fig. FIG.9: (Coloronline). Simulateddistortion ofSIStunneling S9, implies that self-heating at V is less than T /2 at characteristics by strong self-heating. a) Undistorted IVC’s g c T = 4.2K. This is consistent with previous in-situ mea- at different T. Simulations weremade fortypicalparameters of ourmesas, T−dependentthermalconductivityof Bi-2212, surements[36],Rth(T =4.2K,V =Vg)≃30−40K/mW. andforcoherent,directional,d−wavetunneling. b)distorted Therestofthedatapresentedinthemanuscriptisnot IVC’s at the same base temperatures; c) The mesa tempera- affected by self-heating for the following reasons: tureasafunctionofbias. d)Temperaturedependenceofthe The effective T in Fig. M2b) was obtained at eff genuinesuperconductinggap(solidline)andthe”measured” V/N = 30meV at which the dissipation power was only gapobtainedfromdistortedIVC’s(dashedcurve). Notethat P ≃ 3.8µW at T = 5.5K (for comparison, P(V ) = even strong self-heating (T reaches Tc/2 at Vg at 4.2K) does g 0.21mW for the same curve). Therefore, self-heating not cause considerable distortion of the measured gap. Data from Ref.[34] here is negligible (sub-Kelvin). Besides, as arguedin the manuscript, the slope of lndI/dV(V) in Fig. M2 is ap- parently V and P independent, therefore the same data back-bending of the IVC at the sum-gap knee. Fig. S9 couldbeobtainedatmuchsmallerorlargerP. Thedata reproduces the results of numerical simulation of such inFigs. M3b-d)andM4isfreefromself-heatingbecause the distortion, made specifically for the case of Bi-2212 it was obtained at zero bias. mesa with the corresponding T−dependent parameters Finally, it is important to emphasize that the concept (see Ref.[34] for details). Fig. S9 a) shows a set of simu- of heat diffusion is inapplicable for small Bi-2212 mesas latedundistortedIVC’satdifferentT forcoherent,direc- containing only few atomic layers. The phonon trans- tional,d−wavetunnelingwitha∆(T),shownbythesolid port in this case is ballistic [36, 45] and the energy flow line in Fig. S9 d). Panels b) and c) show the distorted from the mesa is determined not by collisions between IVC’s and the actual junction temperature, respectively. the tunneled non-equilibriumQPwith thermalphonons, The dashed line in panel d) represents the ”measured” but by spontaneous emission of a phonon upon relax- gapobtainedfromthepeakindistorteddI/dV character- ationofthe non-equilibriumQP[13]. Thisprocessisnot istics. Remarkably, the deviation from the true ∆(T) is hinderedatT =0. Therefore,theeffectiveR (andself- th marginal,despite largeself-heating,∆T ≃T /2at4.2K! heating)canbemuchsmallerbecauseitisnotlimitedby c The robustness of the measured gap with respect to poor thermal conductivity at T = 0, but is determined self-heating is caused by a flat T−dependence of the su- by the fast, almostT−independent, non-equilibrium QP perconducting gap at T < T /2. If self-heating reaches relaxationtime. Theconceptofself-heatingbecomesad- c T at the sum-gap knee, an acute back-bending appears equate only inthe bulk ofthe Bi-2212crystal,where the c in the IVC’s, however even this does not cause princi- dissipation power density and the temperature rise are ple changes in the ”measured” ∆(T). In experiments on much smaller due to the much larger area of the crystal. large mesas [40] or suspended structures [42], in which FormoredetailsseethediscussioninRef. [36]. Thenon- acute self-heating was reported, no clear Ohmic tunnel- equilibriumenergytransferchannelis specific for atomic ing resistance could be observed at high bias, in stark scaleintrinsicJosephsonjunctionsmadeofperfectsingle contrast to our mesas, see Fig. M1a, and Refs.[7, 8, 44]. crystals. It can explain a remarkably low self-heating at SimulationsasinFig. S9clearlyshowthatirrespective very high bias [13]. 9 that for strongly UD mesas it is R0 (circles in Fig. S10 b), rather than R0/T, that is more accurately described by the Arrhenius law (dashed line). From comparison of Figs. M2a) and S10a) it is seen that Eq.(M1) does provide a good fit to experimental data at T > T , including the crossing point. Simulta- c neously a dramatic discrepancy is seen below T . This c indicates that the slopes of dI/dV(V) curves in the su- perconducting state are not determined by the real T, but by some constant effective temperature, as shown in Fig. M2 b). Fig. S10 b) shows the slope of experimental curves from Fig. M2a) at V/N = 30mV (red squares) and the logarithm of zero bias resistance (green circles) as a function of 1/T. Clear linear dependence of both at T > T indicates that the IVC’s in the normal state c have thermal activation nature both at zero and finite bias, consistent with Eq.(M1). According to Eq.(M1) theeffectivetemperaturecanbeexplicitlyobtainedfrom the slope d/dV[ln(dI/dV)] = (e/2k T)tanh(eV/2k T) B B ≃ e/2k T. Here there are two slight obstacles: First, B the tanh term deviated from unity at high T leading to eventual saturation of the slope at 1/T → 0. The exact T−depensence according to Eq.(M1) is shown by the solid (magenta) line in Fig. S10 b). We emphasize that there are no fitting parameters in this curve. It is seen that Eq.(M1) reproduces quite well T−dependence FIG. 10: (Color online). a) Simulated dI/dV characteristics of the slopes, except for a small offset. This additional according to Eq.(M1) for the same T as in Fig. M2 a). It is offset is caused by the fact that the slope of experimen- seen that at T > Tc they provide a good fit to experimental tal curves becomes negative at large T [8]. The simple data, including the crossing point. b) The slope of experi- mentalcharacteristics from Fig. M2a) atV/N =30mV (red TA expression, Eq.(M1), does not reproduce this nega- squares, left axis) and the logarithm of zero bias resistance tive slope. However, more advanced TA simulations do (green circles, right axis) vs. 1/T. It is seen that both fol- reproduce the negative slope and, in fact, all the details low the TA behavior at T > Tc and simultaneously deviate of experimental dI/dV characteristics at T >Tc [16]. downwards in the superconducting state, indicating that ap- It should be noted that TA-like behavior is quite uni- pearanceofthenegativeexcessresistanceandthecrossoverto versal for many process. Except for pure thermal ac- quantumc−axistransportarecorrelated. Thedashed-dotted tivation over the finite barrier without the gap in the linerepresentstheslope ofresonant tunnelingcharacteristics electronic DoS [16], it may appear in pure tunneling (shown for comparison). characteristics in the presence of the gap in electronic DoS, due to TA-like behavior of the Fermi factor (even D. Thermal activation analysis though this would require a very specific correlation be- tween T−dependent factors mentioned in sec.I); as a re- sultofinelastictunnelingviatheimpurity[28],orelastic The TA current is given by a simple expression: tunneling via a resonant state [29] in the tunnel barrier. U eV Abrikosov has shown that the later scenario can quanti- I ∝n(T)exp − TA cosh , (4) TA tativelyreproducetheinterlayercharacteristicsofHTSC (cid:20) k T(cid:21) (cid:20)2k T(cid:21) B B inthenormalstate[29]. Thebluedash-dottedlineinFig. from which follows Eq.(M1). S10 b) represents the slope d/dV[ln(dI/dV)] in the case Fig. S10 a) shows the dI/dV(V) characteristics in a of resonanttunneling with the appropriate energy of the semi-log scale calculated from Eq.(M1) for the same T resonant state. It follows the simple linear TA behavior and scale as in Fig. M2 a), in order to facilitate the di- at k T lower than the resonant energy and saturates at B rectcomparison. Simulationsweremadeforconstantσ higher T. Comparison with the resonant tunneling cal- N and U = 24meV, which were adjusted to obtain sim- culation shows that the saturation of the slope at high TA ilar R0(T) values as in the experimental data from Fig. T results in appearance of a negative offset in the linear M2 a) at T >T ; and for n(T)∝T. Considerable grows d/dV[ln(dI/dV)] vs 1/T dependence at 1/T → 0. Be- c of mobile carrier concentrationn(T) with T in UD crys- low the saturation temperature, the actual temperature tals was reported in Hall effect measurements [46]. 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