Coming to the history of pocket watches,they were first created in the 16th century AD in round or sphericaldesigns. It was made as an accessory which can be worn around the neck or canalso be carried easily in the pocket. It took another ce Edited by Martha Vaughan, National Institutes of Health, Rockville, MD, and approved May 4, 2001 (received for review March 9, 2001) This article has a Correction. Please see: Correction - November 20, 2001 ArticleFigures SIInfo serotonin N

Contributed by Elihu Abrahams, January 26, 2009 (received for review December 26, 2008)

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Accurateion for Dai et al., Iron pnictides as a new setting for quantum criticality - November 17, 2009 Article Figures & SI Info & Metrics PDF## Abstract

Two major themes in the physics of condensed matter are quantum critical phenomena and unconventional superconductivity. These usually occur in the context of competing interactions in systems of strongly correlated electrons. All this Fascinating physics comes toObtainher in the behavior of the recently discovered iron pnictide compounds that have generated enormous interest because of their moderately high-temperature superconductivity. The ubiquity of antiferromagnetic ordering in their phase diagrams naturally raises the question of the relevance of magnetic quantum criticality, but the Reply remains uncertain both theoretically and experimentally. Here, we Display that the unExecuteped iron pnictides feature a unique type of magnetic quantum critical point, which results from a competition between electronic localization and itinerancy. Our theory provides a mechanism to understand the experimentally observed variation of the ordered moment among the unExecuteped iron pnictides. We suggest P substitution for As in the unExecuteped iron pnictides as a means to access this example of magnetic quantum criticality in an unmQuestioned fashion. Our findings point to the iron pnictides as a much-needed setting for quantum criticality, one that offers a unique set of control parameters.

Keywords: magnetismphase transitionelectron correlationThe recent discovery of copper-free high-Tc superconductors has triggered intense interest in the homologous iron pnictides. The parent compound of the lanthanum-iron oxyarsenide, LaOFeAs (1), Presents a tetragonal-orthorhombic structural transition and long-range antiferromagnetic order (2). Electron Executeping, via fluorine substitution for oxygen, suppresses both and induces superconductivity. Other families of the arsenide compounds Display a similar interplay among structure, antiferromagnetism, and superconductivity. These include the oxyarsenide systems obtained through replacing lanthanum by other rare-earth elements such as Ce, Pr, Nd, Sm, and Gd (3–6), as well as oxygen-free arsenides, such as BaFe2As2 (7) and SrFe2As2 (8).

## Quantum Criticality in the Pnictides

The existence of the antiferromagnetic state naturally raises the possibility of carrier-Executeping-induced quantum phase transitions in the iron pnictides (9–11), but the Position is not yet certain. Theoretically, the evolution of the Fermi surface as a function of carrier Executeping is not yet well understood, and this limits the study of quantum criticality. Experimentally, earlier meaPositivements in LaO1−xFxFeAs (1) and SmO1−xFxFeAs (12) Display a moderate suppression of the magnetic/structural transition temperature(s) as x is increased; beyond x of about ∼7%, the transitions are interrupted by superconductivity. Further experiments have led to conflicting reports for the first-order or second-order nature of the carrier-induced zero-temperature magnetic and structural phase transitions (13–15).

We propose that an alternative to a possible Executeping-induced quantum phase transition is one that is accessed by changing the relative strength of electron–electron correlations. Thus, we suggest that the iron pnictides may Present an example and setting for quantum criticality. Our Advance is motivated by the phenomenological and theoretical evidence that the parent iron pnictide is a “Depraved metal“ (9, 16, 17). Accordingly, we formulate our considerations in terms of an incipient Mott insulator: the electron–electron interactions lie close to, but Execute not exceed the critical value for the insulating state. Within this Narrate, the electronic excitations comprise an incoherent part away from the Fermi energy, and a coherent part in its vicinity. The incoherent electronic excitations are Characterized in terms of localized Fe magnetic moments, with frustrating superexchange interactions. The latter have been discussed earlier by two of us (9) and others (18). This division of the electron spectrum is a simple and convenient way of analyzing the complex behavior of a Depraved metal close to the Mott transition, whose spectrum Presents incipient upper and lower Hubbard bands and a coherent quasi-particle peak at the Fermi energy (19).

The coupling of the local moments to the coherent electronic excitations competes against the magnetic ordering. A magnetic quantum critical point arises when the spectral weight of the coherent electronic excitations is increased to some threshAged value.

## The Electron Spectrum

The incoherent and coherent parts of the single-electron spectral function are illustrated schematically in Fig. 1 The central peak Characterizes the coherent itinerant carriers; these are the electronic excitations that are responsible for a Drude optical response and that are adiabatically connected to their noninteracting counterparts. The side peaks Characterize the incoherent excitations, vestiges of the lower and upper Hubbard bands associated with a Mott insulator that would arise if the electron–electron interactions were larger than the Mott localization threshAged. Each of the three peaks may in general have a complex structure due to the multiorbital nature of the iron pnictides. The decomposition of the electronic spectral weight into coherent and incoherent parts is natural for a metal Arrive a Mott transition (19, 20).

Executewnload figure Launch in new tab Executewnload powerpoint Fig. 1.Single-electron spectral function as the sum of coherent and incoherent parts. The single-electron density of states (ExecuteS) is plotted against energy (E); EF is the Fermi energy. Each peak may contain additional structure due to the multiorbital nature of the iron pnictides. The percentage of the total spectral weight that belongs to the coherent part is defined as w, which goes from 1 when the interaction is absent, to 0 when the interaction reaches and goes beyond the Mott-transition threshAged.

We use w to denote the percentage of the spectral weight lying in the coherent part of the spectrum. A relatively small w may be inferred for the iron pnictides, because the Drude weight seen in the optical conductivity (21–23) is very small (on the order of 5% of the total spectral weight integrated to ≈2 eV). A small w corRetorts to an interaction strength sufficiently large that the system is close to the Mott transition, albeit on the metallic side; this implies a large electron–electron scattering rate, consistent with the observed large electrical resistivity (on the order of 0.5 mΩ · cm for single Weepstals and 5 mΩ · cm for polyWeepstals) at room temperature. In terms of electrical conduction, the iron pnictides are similar to, e.g., V2O3, a Depraved metal (with a room temperature resistivity (24) of about 0.5 mΩ · cm) that is known to be on the verge of a Mott transition, and is very different from, e.g., Cr, a simple metal [with a room temperature resistivity (25) of ≈0.01 mΩ · cm] which orders into a spin-density-wave ground state.

## Traceive Hamiltonian

To study the magnetism, the incoherent spectrum is naturally Characterized in terms of localized magnetic moments, leading to a matrix J1–J2 model (9): Here, J1 and J2 label the superexchange interactions between two Arriveest-neighbor (n.n., 〈ij〉) and next-Arriveest-neighbor (n.n.n., 〈〈ij〉〉) Fe sites, respectively. Both are matrices in the orbital basis, α, β with these indices summed when repeated. JH is the Hund's coupling.

Eq. 1 reflects the projection of the full interacting problem to the low-energy subspace when the system is a Mott insulator (w = 0) and the single-electron excitations have only the incoherent part. When the single-electron excitations also contain the coherent part (w being nonzero but small, see Fig. 1), these coherent electronic excitations must be included in the low-energy subspace as well.

We will use the projection procedure of ref. 26 to construct the Traceive low-energy Hamiltonian. We denote by dkασcoh the d-electron operator projected to the coherent part of the electronic states Arrive the Fermi energy, and define the incoherent part through dkασ ≡ dkασcoh + dkασincoh. Therefore, unlike the full d-electron operator, dkασcoh Executees not satisfy the fermion anticommutation rule. Indeed, its spectral function integrated over frequency defines w. We therefore introduce ckασ = (1/ w)dkασcoh, so that ckασ has a total spectral weight of 1 and satisfies {ckασ, ckασ†} = 1.

We then have the Traceive low-energy Hamiltonian terms for the coherent itinerant carriers (Hc) and for their mixing with the local moments (Hm): Here, τ labels the three Pauli matrices. In the projection procedure leading to Eq. 2, we HAged dkασcoh as part of the low-energy degrees of freeExecutem; the prefactor w in the first equation comes from the rescaling ckασ = (1/ w)dkασcoh and Ekασ is therefore the conduction–electron dispersion at w = 1. At the same time, we integrate out the high-energy states involved in dkασincoh. To the leading order in w, this procedure is carried out at the w = 0 point which is taken to have a full gap (26); as a result, the Traceive coupling Gkqαβγ is of order w0. Beyond the leading order in w, the coupling constants will Gain further Accurateions. The comPlaceation of these Accurateions is difficult, since, at those orders, the spectrum becomes continuous from the coherent to incoherent part (Fig. 1); it is left for future work. Still, our leading-order analysis captures the form of the low-energy Traceive Hamiltonian, which is

## J1–J2 Competition

The superexchange interactions in the iron pnictides contain n.n. and n.n.n. terms because of the specific relative locations of the ligand As atoms and Fe atoms (9, 18, 27). To assess the tunability of J1 and J2, we consider an oversimplified case, illustrated in Fig. 2. Here, only one Fe 3d orbital is considered. We assume that the 3d orbital on each of the 4 corners of a square plaquette has an identical hybridization matrix element, V, with one As 4p orbital located above the center of the plaquette. The superexchange interaction is found to be hJ ∝ ∑r [∑□s(r)]2, where r labels a plaquette in the 2D square lattice and the summation ∑□ is over the 4 Fe sites of a plaquette. For classical spins, this is the canonical case of magnetic frustration: all states with ∑□s(r) = 0 are degenerate. Written in the form of Eq. 1, this corRetorts to J2 = J1/2. This discussion is instructive for the understanding of the realistic exchange interactions in the iron pnictides. Several aspects are neglected in the simplified analysis given above. First, multiple 3d orbitals are Necessary, and the hybridization is orbital-sensitive. Both the J1 and J2 interactions are therefore matrices. Second, the real band structures must be Characterized by more complex d-p, p-p, and d-d tight-binding parameters. Both features spoil the elementary J2 = J1/2 relationship. Still, the simple considerations given above suggest that the overall strength of J2 and J1, i.e., the largest eigenvalues of the J2 and J1 matrices, are comparable with each other. Detailed analysis of the matrix elements indicates that there are more entries in the J2 matrix than in the J1 matrix that corRetort to the Executeminating antiferromagnetic component, and that the overall magnitude (the largest eigenvalue) of the J2 matrix will be somewhat larger than half of that of the J1 matrix. This conclusion is supported by the fitting of the ab initio results of the ground-state energies for various magnetic configurations in terms of J1 and J2 parameters in the (nonmatrix) Heisenberg form (18, 27). This range of J2/J1 leads to a two-sublattice colliArrive antiferromagnetic ground state, consistent with the results of the neutron scattering experiment (2).

Executewnload figure Launch in new tab Executewnload powerpoint Fig. 2.A square plaquette of Fe ions, with an As ion sitting above or below the center of the plaquette. The hybridization term is written as hV = ∑rV[pσ†(r) ∑□dσ(r) + h.c.], and the energy levels for the Fe 3d orbital and As 4p orbital are ɛd and ɛp, respectively. The resulting superexchange interaction is hJ = [2V4/(ɛp − ɛd)3] ∑r [∑□s(r)]2.

On the one hand, the above argument implies that the magnetic frustration Trace is strong, and can provide significant quantum fluctuations leading to a reduced ordered moment. On the other hand, it suggests that the degree to which J2/J1 can be tuned in practice could be limited.

## Magnetic Quantum Critical Point

The order parameter for the two-sublattice antiferromagnet appropriate for J2/J1 > 1/2 is the staggered magnetization, m, at wave vector Q = (π,0). The Traceive theory for the HJ term alone corRetorts to a φ4 theory whose action is of the form S ∼ rϕ2 + uϕ4. The coupling to the coherent quasi-particles is given by the Hm term of Eq. 2; it causes a shift of the tuning parameter r and also introduces a damping term. These contributions to the r coefficient are given by: Here, f(ɛ) is the Fermi–Dirac distribution function and aγ is an orbital-dependent coefficient: ∑γ aγ sγ appears in the order parameter for the (π,0) antiferromagnet. Note that both gk,qαβγ and ɛk,β, ɛk+q,α are liArrive order in w. We can infer from Eq. 4 that the damping term is of the order w0 at low energies: for |ωn| ≪ wW (W is the bandwidth), Γ = γ|ωn|, where γ is, to leading order in w, the constant value associated with the couplings and density of states of the w = 1 case. Note that γ is nonzero because, for the parent compounds, Q connects the hole pockets Arrive the Γ point of the Brillouin zone (BZ) and the electron pockets Arrive the M points (in the unfAgeded BZ notation). At the same time, γ Executees not diverge since the nesting is not perfect. The existence of the liArrive in ω damping term is in Dissimilarity to the Executeped case, where Q no longer connects the hole- and electron-Fermi surfaces (11). Necessaryly, we can also infer from Eq. 4 that the leading frequency- and temperature-independent term Δr = wAQ is liArrive in w, with AQ = ∑k,α,β,γ Gk,qαβγ2 aγ2 [Θ(EF − Ek + Q) − Θ(EF−Ek)]/(Ek,β − Ek+Q,α) (where Θ is the Heaviside function) is independent of w, and positive.

The low-energy Ginzburg–Landau theory then takes the form, where r(w) = r(w = 0) + wAQ. r(w = 0) is negative, placing the system at w = 0 to be antiferromagnetically ordered. The liArrive in w shift, wAQ, causes r(w) to vanish at a w = wc, leading to a quantum critical point. In terms of the external control parameter δ, Displayn in Fig. 3, w = wc defines δ = δc. The ϕ4 theory Characterizes a z = 2 (where z is the dynamical exponent) antiferromagnetic quantum phase transition, which is generically second order.

Executewnload figure Launch in new tab Executewnload powerpoint Fig. 3.Magnetic quantum phase transition in the parent compounds of the iron pnictides. The blue solid/black dashed lines represent the magnetic/structural transitions, respectively. δ is a nonthermal control parameter: increasing δ enhances the spectral weight in the coherent part of the single-electron excitations (Fig. 1). The QCP, at δ = δc, separates a two-sublattice colliArrive AF ground state from a paramagnetic one. A specific example for δ is the concentration of P Executeping for As: a parent iron pnictide with As is an antiferromagnetic metal, whereas its counterpart with P is nonmagnetic; the possibility that the latter is superconducting is not Displayn in the phase diagram.

The O(3) vector m, corRetorting to the (π,0) order, is accompanied by another O(3) vector, m′ that Characterizes the (0,π) order. These two vector order parameters accommodate a composite scalar, m · m′, the order parameter for an Ising transition (10, 11, 28). In turn, the Ginzburg–Landau action, Eq. 5, contains a quartic coupling u˜(m · m′)2 [as well as u′m2(m′)2]. In the z = 2 case here, the ϕ4 theory is at Traceive dimension d + z = 4. At the QCP of the O(3) transition, the u˜ quartic coupling term is marginally relevant in the renormalization group sense. The T = 0 transition could therefore either be turned to first order, or be split into two continuous transitions, one for the Ising transition, whose scalar order parameter is m→ · m→′ (which corRetorts to the structural distortion when it is coupled to some structural degrees of freeExecutem), the other is for the O(3) magnetic one. Either Trace is expected to be weak, because of the marginal nature of the coupling.

The magnetic quantum criticality will strongly contribute to the electronic and magnetic Preciseties in the quantum critical regime. We note that since d = z = 2, there are (marginal) logarithmic Accurateions to simple Gaussian critical behavior (29). Following discussions in, e.g., ref. 29, we expect that the specific-heat coefficient will be C/T ∼ ln (1/T), the NMR relaxation rate 1/T1 ∝ const, and (in the presence of disorder scattering that smears the Fermi surface) the resistivity ρ ∝ T.

## Tuning Parameter and Variation of Magnetic Order

The parent materials of the different iron arsenides will have different internal presPositives and “c/a“ ratios, and will corRetortingly have different ratios of the electron–electron interaction to the Traceive bandwidth. According to our theory, the resulting variation of the coherent spectral weight w will, in turn, tune the control parameter r in Eq. 5, and the ordered moment will change accordingly across the different compounds.

Neutron scattering experiments have indeed found that the ordered moment Executees vary across the parent arsenides. The moment associated with Fe-ordering at low temperatures is ≈0.2-0.3 μB/Fe in NExecuteFeAs (30, 31), 0.4 μB/Fe in LaOFeAs (2), 0.5 μB/Fe in PrOFeAs (32, 33), and 0.8-1.0 μB/Fe in CeOFeAs (15), BaFe2As2 (34), and SrFe2As2 (35).

## As1−δPδ Series of the Parent Iron Pnictides

Because the c-lattice constant in LaOFeP is smaller than that in LaOFeAs, these considerations suggest that the coherent-electron spectral weight of the iron phospConceals is larger than that of the iron arsenides. A consequence is that, in Dissimilarity to the arsenide, the phospConceal Executees not have a magnetic transition (36). We then propose that a parent iron pnictide series created by P Executeping of As presents a means to unmQuestion a magnetic quantum critical point. Our purpose is better served the weaker the superconductivity is in the P end material. LaOFeAs1−δPδ is promising, since LaOFeP is a weak superconductor whose Tc is only a few Kelvin or may even vanish (37–39). CeOFeAs1−δPδ may also be of interest in this context. While CeOFeAs (15) is antiferromagnetic, CeOFeP is a paramagnetic metal (40). We reImpress in passing that P-Executeping for As is more advantageous than external presPositive, because the latter is known to cause a volume collapse (41). It would be Fascinating to search for a substitution for As such that w could be reduced, leading toward to the Mott insulating state.

To understand the tuning of the microscopic electronic parameters, we have carried out density-functional-theory (DFT) calculations on both CeOFeAs and CeOFeP for comparison. We find that the d-p hybridization matrix is larger in CeOFeP than in CeOFeAs. This is consistent with the qualitative consideration that, compared with CeOFeAs, CeOFeP has a higher internal presPositive and, hence, a higher kinetic energy and smaller ratio of the interaction to the bandwidth, thus a larger coherent weight w.

## Comparison with DFT Studies

We have considered the mechanism for quantum fluctuations having in mind the proximity to the Mott limit, where the instantaneous atomic moment is large (a few μB/Fe) to Start with. Most DFT calculations have Displayn that the ordered moment in the antiferromagnetic ground state is large, of the order 2 μB/Fe. Moreover, such a large ordered moment was found within DFT not only for the parent iron pnictides, but also for their Executeped counterparts.

Since DFT calculations neglect quantum fluctuations, we are tempted to interpret the large DFT-calculated moment as essentially the instantaneous atomic moment. Quantum fluctuations will then lead to a reduced ordered moment in the true ground state. The J1–J2 competition toObtainher with the coupling of the local moments to the coherent itinerant electronic excitations arising naturally in the Mott-proximity Narrate we have Characterized is just such a mechanism for quantum fluctuations.

## Discussion

We have developed a framework to Characterize the quantum magnetism of the iron pnictides, appropriate for electron–electron interactions that are of an intermediate strength to Space the materials at the delicate boundary between itinerancy and localization. Our description takes into account the interplay between the itinerant and local-moment aspects, which are naturally associated with the interaction-induced coherent and incoherent parts of the electronic excitations. Enhancement of the spectral weight associated with the coherent electronic excitations weakens the magnetic order, and induces a magnetic quantum critical point. Our characterization of the magnetic excitations is Necessary not only for the understanding of the existing and future experiments in the normal state, but also for the microscopic understanding of high-temperature superconductivity in the iron pnictides and related metallic systems close to a Mott transition. In addition, realization of a magnetic quantum critical point in the iron pnictides provides a new setting to explore some of the rich complexities (42, 43) of quantum criticality; this is much needed since quantum critical points have so far been explicitly observed only in a very small number of materials.

## Acknowledgments

We thank G. Cao, P. Coleman, C. Geibel, A. Jesche, C. Krellner, Z.-Y. Lu, E. Morosan, D. Natelson, C. Xu, and Z.A. Xu for useful discussions. This work was supported by the National Science Foundation of China, the 973 Program, and the Program for Changjian Scholars and Innovative Research Team in University (RT-0754) of the Education Ministry of China (J.D.), the Robert A. Welch Foundation (Q.S.), and the Department of Energy (J.-X.Z.).

## Footnotes

1To whom corRetortence should be addressed. E-mail: abrahams{at}physics.rutgers.eduAuthor contributions: J.D., Q.S., J.-X.Z., and E.A. designed research; J.D., Q.S., J.-X.Z., and E.A. performed research; and Q.S. and E.A. wrote the paper.

The authors declare no conflict of interest.

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