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Interchain conductivity of coupled Luttinger liquids and organic conductors Antoine Georges1,2, Thierry Giamarchi2,1, Nancy Sandler3 1CNRS UMR 8549- Laboratoire de Physique Th´eorique, Ecole Normale Sup´erieure, 24 Rue Lhomond 75005 Paris FRANCE 2 Laboratoire de Physique des Solides, CNRS-UMR 8502, Batiment 510, Universit´e de Paris-Sud, 91405 Orsay, FRANCE 3 Laboratoire de Physique de la Matiere Condens´ee, Ecole Normale Sup´erieure, 24 Rue Lhomond 75005 Paris FRANCE (February 1, 2008) We reconsider the theory of dc and ac interchain conductivity in quasi-one dimensional systems. 0 0 Ourresultsareingoodagreementwiththemeasuredc-axisopticalconductivityof(TMTSF)2ClO4 0 and suggest that the c-axis dc-conductivity of (TMTSF)2PF6 in the 150K < T < 300K range 2 is dominated by precursor effects of Mott localization. The crossover from a Luttinger liquid at highenergytoaFermiliquidatlowenergyisalsoaddressed,withinadynamicalmean-fieldtheory. n Implicationsfortheinter-chainresistivityandDrudeweightintheFermiliquidregimearediscussed. a J Inter-chain(orinter-plane)coherenceis akeyissuefor temperature scale than the early estimates based on the 6 the physicsofanisotropicstronglycorrelatedsystems. It NMR.Furthermore,itisclearfromthe opticaldatathat isofspecialimportanceforthequasi-onedimensionalor- another important energy scale is present in these com- ] l ganic conductors TMTSF X and TMTTF X which are pounds,associatedwithaMottgapsignaledbytheonset e 2 2 - systems of weakly coupled chains [1]. Since the one di- of optical absorption at 100cm−1 150K. Transverse r mensional (1D) interacting electron gas has non Fermi hoppingisactuallyrespo∼nsibleforth≃e metalliccharacter t s liquid (Luttinger liquid) properties [2], one expects in of the (TMTSF) X compounds, which otherwise would . 2 t these compounds a crossover from Luttinger liquid be- be Mott insulators [11,15]. These findings raise a num- a m havior to a coherent behavior as the temperature or fre- ber of important and largely unanswered questions such quency is lowered. The latter can be either a metallic as the precise nature of the dimensional crossover, the - d three-dimensional conductor (presumably Fermi-liquid origin of the anomalies observed for 10K < T < 100K n like), or a phase with long-range order. (calling in particular for a reinterpretation of the NMR o Although there is general agreement on this qualita- in this range), and the actual range of the LL behavior. c [ tive scenario, there is considerable debate on how pre- Inthisletter,wefocusoninter-chaintransportandop- cisely this crossover takes place [3–7]. As was pointed ticalresponse,whichareidealprobesofthese issues. We 1 outearlyon[8],theinteractionsrenormalizetheeffective first reconsider the theoretical analysis of the ω and T- v 3 interchain hopping of weakly-coupled Luttinger chains. dependence of the inter-chain conductivity for the sim- 6 This leads to a crossover scale E∗ t(t⊥/t)1/(1−α) = plest case of weakly coupled metallic Luttinger liquids. ∝ 0 t (t /t)α/(1−α) for the onset of coherence along one of We findapowerlawofthetemperatureorthe frequency ⊥ ⊥ 1 the transverse directions with interchain hopping t . In σ (T,ω) (T,ω)2α−1. Theexponentisatvariancewith ⊥ ⊥ 0 ∝ this expression, t is the intra-chain hopping and α previous theoretical predictions [6,16,14], but is in rea- 0 ≡ 0 41(Kρ +1/Kρ)− 21 is the Fermi surface exponent. The sonable agreement with recent measurements of c-axis t/ scale E∗ can be much smaller than the bare interchain optical conductivity of the (TMTSF)2ClO4 compound a hopping t . With this idea in mind, analysis of NMR [17]. We then show that understanding the observed ⊥ m data [9,10] led to believe that the 1D Luttinger liquid T-dependence of c-axis transport in (TMTSF) PF re- 2 6 - (LL) to Fermi liquid (FL) crossover took place in the quires to take into account the physics associated with d (TMTSF) Xfamilyatalowtemperature,oftheorderof theMottgapapparentinopticalmeasurements. Finally, n 2 10 15K. This scale seemed consistent with the above we consider a dynamical mean-field theory (DMFT) for o − c estimate of E∗ since the interchain hopping along the b- the description of the dimensional crossover, and draw : axis is t 300K, an order of magnitude smaller than someconsequencesfortheinter-chainconductivityinthe v b ∼ i the hopping ta along the chains. Recent analysis of the low-temperature FL regime. X transport and optical properties [11] have led to a re- We consider the hamiltonian of coupled chains: r examination of this commonly accepted view. Measure- a ment of the optical conductivity along the chains agrees H = H1(mD)− t⊥ (c+imσcim′σ +h.c) (1) withaLLpictureathighenoughfrequencyandprovides Xm hmX,m′i Xiσ a determination of the LL exponent K [12,13](of order ρ K 0.23). This value is consistent with the temper- in which H(m) stands for each individual chain m, and ρ 1D ≃ ature dependence of ρa(T) in the 100K 300K range the inter-chain hopping t⊥ will be first considered, for − (suitably corrected for thermal expansion [1]). However, simplicity, to be identical for all transverse directions. these studies andmostnotably the recentmeasurements UsingtheDMFT approachdetailedbelow,ageneralfor- of the interchain dc conductivity [14] revealed that the mula(Eq.6)forthetransverseconductivitycanbeestab- 1D regime only extends down to 100K, a much higher lished. When the inter-chain hopping t⊥ can be treated ∼ in perturbation theory to lowest order, this formula re- 1 ducestothatestablishedinRef.[14]withinthetunneling relevant. This suggests that if the transverse hopping approximation [18]: was entirely suppressed in these compounds, they would actually be one-dimensional (quarter filled) Mott insu- Reσ (ω,T)pert t2 dx dω′A (x,ω+ω′) lators. Fortunately, optical experiments extend to high ⊥ ∝ ⊥Z Z 1D × frequencies compared to the Mott gap. Thus the com- A (x,ω′)f(ω′)−f(ω′+ω) (2) plications associated with the proximity to the Mott in- 1D × ω sulating state can be treated perturbatively, making the comparison to Eq.(3) relevant. Recently, optical stud- where A (x,ω) is the one-electron spectral function of 1D iesof(TMTSF) ClO havebeenperformed[17],andthe asinglechain,andf the Fermifunction. Letusconsider 2 4 high-frequencyopticalconductivityσ (ω)alongthe least firstthe simplest casein whicheachdecoupledchainis a c conducting c-axis was found to be a broad, very slowly LuttingerliquidcharacterizedbyagivenvalueofK ,and ρ increasing function of frequency in the range 50cm−1 < all intra-chain umklapp processes can be neglected. For ω <105cm−1. Thisslowlyincreasingcontinuumisessen- thevaluesofK ofinteresthere,thetransversehoppingis ρ tially independent of temperature for 10K< T < 300K, thenarelevantperturbationintherenormalizationgroup andis ingoodagreementwithourresultσ (ω) ω2α−1. sense, so that it is legitimate to treat it perturbatively c ∝ The exponent 2α 1 = (K + 1/K )/2 2 depends only at sufficiently high energy or temperature. Eq. (2) − ρ ρ − quite sensitively on the value of K (2α 1 = 0.12 for thus applies only when kT E∗ or h¯ω E∗, where ρ − ≫ ≫ K = 0.25 and 2α 1 = 0.6 for K = 0.2). The latter E∗ = t(t⊥/t)1/(1−α) is the single-particle crossover scale ρ − ρ value 2α 1 0.6 provides a reasonable fit to the ex- mentionedabove[8,3,19]. Inthishigh-temperature/high- − ≃ perimental data of [17]. Note that values of K in the energy regime, the system can be considered to be quasi ρ 0.2-0.25range are quite consistent with the other exper- one-dimensional. Using knownproperties of the spectral imental findings discussed above. In contrast, the ω2α functions in a Luttinger liquid, we then obtain from (2): law advocated in [6,16,14] would require K 0.35 to ρ ≃ t 2 T 2α−1 ω explain these data, a value quite inconsistent with that Reσ⊥(ω,T)pert ⊥ Fα (3) obtained from the longitudinal optical conductivity. Fi- ∝(cid:18) t (cid:19) (cid:18)t (cid:19) (cid:16)T(cid:17) nally, an important issue in view of the success of this In this expression, F is a scaling function such that simple theory is whether it can also account for the be- α F (0) = const and F (x 1) x2α−1. Thus, we find havioroftheopticalconductivityalongtheb-axis. Since α α ≫ ∼ Reσ (T ω) T2α−1 for kT E∗, while at high- t /t 0.1,anincoherentregimeshouldalsoapplythere ⊥ b a ≫ ∝ ≫ ≃ frequency (h¯ω E∗), we obtain σ (ω T) ω2α−1. atthosehighfrequencies. Preliminaryanalysis[20]ofthe ⊥ ≫ ≫ ∝ This behavior of σ (T) differs from the conclusions σ data of[17]seems in agreementwith sucha behavior, ⊥ b ofpreviousauthors. In[6], the authorsuseda somewhat but more detailed comparison with the data is needed. differentapproachthanthedirectKuboformulaandcon- We now discuss the measurements of the c-axis trans- cluded that σ (T) T2α. In [14], it was noted that this portin(TMTSF) PF [14,21]. Becauseofthelargether- ⊥ 2 6 ∝ temperature dependence also results from (2) provided malexpansion,thesewereperformedatseveralpressures that the spatial integral is cutoff at a scale of the order so that a volume correction could be made. This yields of the lattice spacing. According to these authors, this data for the c-axis resistivity ρ (T) which can be inter- c cutoff is justified by the incoherent nature of the propa- preted as corresponding to a compound with constant gationof a physicalelectron within each chain (in which latticeparameters. Thisvolume-correctedρ (T)displays c the true quasiparticles are spinons and holons). In our a marked increase by more than a factor of 3 upon cool- opinion however, this information is already encoded in ing from T = 350K down to T = 100K (followed by a the spectral function of the physical electron A (x,ω) rapid downturn at lower temperature which presumably 1D and no extra cutoff has to be introduced in (2). This marks the onset of inter-chain coherence). Such a large conclusion would of course be changed in the presence variationofρ (T)cannot be explainedbythedependence c ofspecificformsofintra-chaindisordersuchasarandom ρ 1/T2α−1 found above with acceptable values of K c ρ ∝ forwardscattering,whichwouldspoilmomentumconser- (which correspond to rather small values of 2α 1). In − vation and bring in a natural cutoff of the order of the [14],itwasfittedtoa1/T1.4powerlaw,whichhappensto mean-free path. Note however that more realistic forms be in reasonable agreement with the 1/T2α dependence of disorder would be signaled by localisation effects. advocated by these authors. However, the temperature We now turn to a comparison with experiments on rangeinwhichthesedataareobtainedissuchthatkT is (TMTSF) X. Itisincreasinglyrecognizedthattheprop- never significantly larger than the “would-be” 1D Mott 2 erties ofthese compounds resultfromthe commensurate gap which can be extracted from the optical measure- quarter-fillingoftheband[11,13,14]. Transportandopti- ments (100 200cm−1) leading to transport gaps (half − calmeasurementsleadto consistentvalues ofthe LL pa- the optical gap) in the range ∆ 75 150K. As a re- ≃ − rameterK 0.23. NotethatK <0.25isthecondition sult,theproximitytotheincipientMottinsulatorcannot ρ ρ ∼ upon which the quarter-filled umklapp process becomes be neglected, and we propose that this effect is the one 2 responsiblefortheincreaseofρ (T). Indeed,wehaveat- formulate a controlledDMFT of strongly-correlatedsys- c tempted a phenomenologicalfit by an activated behavior tems [24,25]. We consider eachone-dimensionalchain to ρ (T) 1/T2α−1exp∆/T. and found that it provides be coupled to z nearest neighbor ones, with the c ⊥ ∝ → ∞ a fit of the data of Ref. [14,21] which is as satisfactory transverse hopping scaled as t = t /√z , so that the ⊥ ⊥ ⊥ as the power-law fit used in [14]. The value of ∆ used non-interacting density of states in the transverse direc- e in this fit is of the same order of magnitude than the tionD(ǫ ) δ[ǫ ǫ(k )] remains well-defined. It ⊥ ≡ k⊥ ⊥− ⊥ Mott gap seen in optical measurements. The discrep- is easily shownPthat in this limit the self-energy becomes ancybetweenthetheoreticalresult,Eq.(3)andtheexper- independent of transverse momentum k : Σ=Σ(k,iω ) ⊥ n imentally observed behavior of ρ (T) is, in our opinion, (k is the momentum along the chains). Furthermore, c a strong indication that an explanation based on inco- the calculation of Σ reduces to the solution of an effec- herent tunneling between LL chains in a purely metallic tive one-dimensional problem specified by the effective regimeis insufficient andthat the physics ofMottlocali- action: sation plays an important role in the temperature range β 150K<T <300K. S = dτdτ′ c+(τ) −1(i j,τ τ′)c (τ′) A more refined theory of the interplay between inter- eff −Z Z0 Xij,σ iσ G0 − − jσ chain hopping and Mott localisation is clearly needed, β including both the transverse hopping and the quarter- + dτHint[ c ,c+ ] (4) Z 1D { iσ iσ} filling umklapp scattering [22]. Due to the umklapp, the 0 effective Kρ will be renormalized towards smaller values whereHint is the interactingpartofthe on-chainhamil- 1D as temperature is decreased, hence leading to larger val- tonian in (1), while is an effective bare propaga- 0 ues of ρ , as expected. The main issue is whether the G c tor which is determined from a self-consistency con- intra-chain resistivity is also strongly affected by these dition. The latter imposes that the Green’s function renormalizations. Indeed,nosignofanupturninρa(T)is G(i j,τ τ′) c(i,τ)c+(j,τ′) calculated from eff observed experimentally for the TMTSF X compounds. − − ≡ −h i 2 S coincides with the on-chain Green’s function of the eff Sdienccreeaρsae(Tin)K∝g12is/4aTlm16oKsρt−c3o[m11p]e,nitsaistecdonbcyeivaanbalesstohcaitatthede originalproblem,withaself-energyΣ=G0−1−G−1. This ρ condition reads: decrease of the effective g due to t . This however, 1/4 ⊥ D(ǫ ) remains to be verified and is probably the most chal- ⊥ G(k,iω )= dǫ (5) n ⊥ lenging issue for the picture that we propose. Transport Z iωn+µ ǫk Σ(iωn,k) ǫ⊥ − − − in the TMTTF X family is interesting in this respect. 2 The DMFT equations (4,5) fully determine the self- ThesecompoundsareinsulatorswitharatherlargeMott energy and Green’s function of the coupled chains. Fur- gap, and indeed both ρ (T) and ρ (T) display an acti- a c thermore, inter-chain transport properties simplify in vated behavior at low temperature. Above some tem- thisapproach. Becausethecurrentvertexisanoddfunc- perature scale however, ρ (T) becomes metallic, while a tionofthetransversemomentum,vertexcorrectionsdrop ρ (T) still displays insulating behaviour (albeit slower c out of the inter-chain conductivity, which reads: than activated). Studies of the transport properties of thesecompoundsoveramoreextendedrangeofpressure dk Reσ (ω,T) t2 dǫ D(ǫ ) dω′A(ǫ ,k,ω′) and temperature (and in particular a detailed compari- ⊥ ∝ ⊥Z ⊥ ⊥ Z 2π Z ⊥ son of the energy scales appearing in σa(ω), ρa(T) and f(ω′) f(ω′+ω) ρc(T)) would certainly prove very interesting. ×A(ǫ⊥,k,ω+ω′) −ω (6) Letusfinallyaddresstheissueofthecrossoverbetween a Mott-Luttinger liquid at highenergy/temperatureand Here, A(ǫ ,k,ω) = 1ImG(ǫ ,k,ω) is the single- ⊥ −π ⊥ acoherent(presumablyFermi-liquid)stateatlowenergy. particle spectral function of the coupled chains system. Themaintheoreticaldifficultyisthatthiscrossoverisas- Eq.(6) has a much wider range of applicability than its sociated with the breakdown of perturbative expansions small-t limit, Eq.(2),sinceitholdsallthe wayfromthe ⊥ int . Ontheotherhand,perturbativeapproachesinthe LL to the FL regime. ⊥ interactionstrengthcould be usedin the FL regime, but Solvingquantitativelythese DMFT equationsisstill a fail in the LL regime. The necessity of treating t in a challenging problem however. In the single-site DMFT ⊥ non-perturbativemannerwasrecentlynotedbyArrigoni (corresponding to the usual d = limit [24]) the map- ∞ [23],whousedalimitofinfinitetransversedimensionality pingisontoasingle-impurityAndersonmodelwithaself- as a guidance for resumming the perturbation series in consistent bath, and severaltechniques have been devel- t . Here, we show that this limit provides a generalized opedtohandlethisproblem. Herehowever,themapping ⊥ dynamicalmean-fieldtheory(DMFT) frameworkforthe is onto a self-consistent 1D-chain, and the problem is an description of the crossover, and we draw some conse- order of magnitude more difficult. Nevertheless, several quencesforinter-chainconductivity. Thelimitofinfinite conclusionscanbe drawnfromthe aboveequations even dimensions has been used extensively in recent years to in the absence of a full solution. We shall consider again 3 the simplest case of metallic 1D LL chains, neglecting WethankD.Jerome,J.Moser,L.Degiorgi,G.Gru¨ner, umklappscatteringandMott physics. Inthe 1Dregime, andV.Vescoliforsharinganddiscussingtheir datawith the self-energy behaves as Σ t((ω,k)/t)1/(1−α). From us. Discussions with M. Gabay and A. M Tremblay are ∝ (5), it is clear that the inter-chain hopping becomes rel- also acknowledged. A.G. and T.G. would like to thank evant when t > Σ, and we recover the crossover scale the ITP, Santa Barbara for support (under NSF grant ⊥ E∗ t(t /t)1/(1−α). At energies smaller than E∗, the No. PHY94-07194) and hospitality during part of this ⊥ ∝ DMFT approach leads to Fermi-liquid behavior. This is work. clearfromviewingthe effective 1Dmodelas asetofAn- dersonimpuritymodelscoupledtogetherbythenon-local part of the “bare” propagator . Each of the decou- 0 G pledAndersonmodelisaFermi-liquidatlow-energyand the non-local hybridization is a smooth perturbation on the FL ground state. In other words, the physics below [1] D. Jerome, in Organic Superconductors: From E∗ is smoothly connected from small t /t to large t /t. ⊥ ⊥ (TMTSF)2PF6 to Fullerenes (Marcel DekkerInc.,1994), When t t and for energy scales much smaller than ⊥ Chap. 10, p. 405. ≪ the bandwidth (of order t), all single-particle quantities [2] H. J. Schulz, in Mesoscopic quantum physics, Les shouldobeyascalingbehaviorinthevariablesω˜ =ω/E∗, Houches LXI, edited by E. Akkermans et al. (Elsevier, x˜ = xE∗/t, T˜ = T/E∗. In particular tΣ(x,ω,T) = Amsterdam, 1995). E∗t Σ˜(x˜,ω˜,T˜), tG(x,ω,T) = (E∗/t )G˜(x˜,ω˜,T˜) with [3] C. Bourbonnais and L. G. Caron, Int. J. Mod. Phys. B ⊥ ⊥ Σ˜ and G˜ universal scaling functions associated with the 5, 1033 (1991). crossover. Alow-frequencyexpansionofthescalingform [4] X. G. Wen,Phys. Rev.B 42, 6623 (1990). [5] S.BrazovskiiandV.Yakovenko,J.dePhys.(Paris)Lett. ofΣintheFLregimeyieldsafinitequasiparticuleresidue Z ∝ (t⊥/t)1−αα ∝ E∗/t⊥ (shown in [23] to have only 4(169,9L2)1.11 (1985); V. M. Yakovenko, JETP Lett. 56, 510 weak k-dependence along the Fermi surface). Z can be [6] D. G. Clarke, S. P. Strong, and P. W. Anderson, Phys. much smaller than unity, while the effective mass (spe- Rev. Lett.72, 3218 (1994). cific heat) ratio m∗/m does not become large because [7] H. J. Schulz, in Correlated fermions and transport in ∂Σ/∂ω and ∂Σ/∂k scale in the same manner. Using the mesoscopic systems, editedbyT.Martin etal.(Editions FL form of Σ in (6), we obtain the T = 0 inter-chain fronti`eres, Gif sur Yvette,France, 1996). conductivityas: σ (ω,T =0)= ωD2⊥δ(ω)+σreg(ω)with [8] C.Bourbonnaiset al.,J.dePhys.(Paris)Lett.45,L755 ⊥ 8 ⊥ (1984). ω 2/8 Z2t2/t = t(t /t)2/(1−α). The total spectral D⊥ ∝ ⊥ ⊥ [9] C. Bourbonnais, J. de Phys.I 3, 143 (1993). weight dωσ (ω)=ω2 /8 is, from the f-sum rule, pro- ⊥ P⊥ [10] P. Wzietek et al.,J. dePhys. I 3, 171 (1993). portionRal to the inter-chain kinetic energy, and hence to [11] T. Giamarchi, Physica B 230-232, 975 (1997). t2/t, so that the relative weight carried by the Drude ⊥ [12] M. Dressel, A. Schwartz, G. Gru¨ner, and L. Degiorgi, peak is small, of order ωD2⊥/ωP2⊥ ∝(t⊥/t)2α/(1−α) =Z2 Phys. Rev.Lett. 77, 398 (1996). This is in reasonableagreementwith the opticaldata on [13] A. Schwartz et al.,Phys. Rev.B 58, 1261 (1998). the b-axis reflectivity of (TMTSF) PF [26], for which a [14] J. Moser et al.,Eur. Phys. J. B 1, 39 (1998). 2 6 Drudepeakisseenatlowtemperature,withω2 /ω2 [15] V. Vescoli et al.,Science 281, 1191 (1998). D⊥ P⊥ ≃ 0.03 (while t /t 0.1). Scaling considerations also lead [16] P. W. Anderson, T. V. Ramakrishnan, S. Strong, and b a toaninter-chainr≃esistivityρ (T)/ρ =(t/E∗)R(T/E∗), D. G. Clarke, Phys.Rev. Lett. 77, 4241 (1996). with R(x 1) x1−2α , ⊥R(x 01) x2 and ρ = [17] W. Henderson et al.,Eur. Phys.J. B 11, 365 (1999). 0 ≫ ∼ ≪ ∼ [18] Transverse conductivities are given in the units of hV /(e2a2) [18]. This implies that ρ /ρ =A(T/t)2 in m ⊥ ⊥ 0 e2a2⊥/(hVm),witha⊥ theinter-chainspacingandVmthe the FL regime, with an enhanced value of the coefficient volume of the unit cell, and the on-chain lattice spacing 3 A (t/t⊥)1−α. Note that ρ⊥ is typically much bigger is normalized to unity. ∝ than the Mott limit ρ0, as observed experimentally. [19] D.Boies,C.Bourbonnais,andA.-M.S.Tremblay,Phys. In conclusion, we have reconsidered in this paper the Rev. Lett.74, 968 (1995). theory of interchain conductivity in quasi-1D systems. [20] L. Degiorgi, privatecommunication. When applied to organic compounds, good agreement is [21] J. Moser, Ph.D. thesis, Paris XI University,1999. found with the frequency dependence of σ (ω). while c- [22] S.Florens,A.Georges,andT.Giamarchi,inpreparation. c axisdctransportappearstobedominatedbytheproxim- [23] E. Arrigoni, Phys. Rev. Lett. 83, 128 (1999), ; see also cond-mat/9910114. ity ofthe Mott gap∆. This calls for additionaltheoreti- [24] A.Georges,G.Kotliar,W.Krauth,andM.J.Rozenberg, calworkinthe regimewhereE∗ t(t /t)1/(1−α) <∆< ∝ ⊥ Rev. Mod. Phys. 68, 13 (1996). t⊥. It would also be valuable to see whether the regime [25] T.Pruschke, M.Jarrell, and J.Freericks, Adv. Phys. 42, ∆ < E∗, which is simpler to analyze theoretically, can 187 (1995). be realized experimentally in some family of compounds [26] V. Vescoli, phDthesis, unpublished. (e.g by applying uniaxial stress to TMTTF X). 2 4

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