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# The self-organised phases of manganites

## 1 Introduction

The doped perovskite manganites are fascinating because they can readily be tuned between radically different phase states. Broadly speaking one has either a ferromagnetic metal, a charge-ordered insulator, or a paramagnetic polaron liquid. The spatial extent of these three types of phase is potentially unlimited — but so, according to a growing body of evidence, are the number of alternative phases that occur over mesoscopic length scales.

What is the basis for such richness and complexity? The answer is that the magnetic, electronic and crystal structures of any given manganite are intimately related. Thus one may parameterise any given phase in the manganites by the nature of the spin, charge, orbital and structural degrees of freedom; the degree to which these degrees of freedom are static or dynamic; and, of particular interest here, the length scales over which these degrees of freedom are homogeneous. Note that we do not consider any texture that only extends over microscopic (i.e. unit cell) length scales to be a phase. For example, one stripe in a stripe phase is not in itself a phase — because at least one dimension is too small for the object to be considered a thermodynamic entity.

At a microscopic level one can understand the strong interaction between the magnetic, electronic and crystal structures as follows. The electronic sub-lattice of a perovskite manganite consists of a cubic network of corner-sharing $`MnO_6`$ octahedra in which potential charge carriers arise in certain orbitals if, for example, the interstitial A-site cations comprise a mixture of trivalent and divalent species such that they act as a charge reservoir. This electronic sub-lattice is also the home of the magnetic sub-lattice since the magnetic structure arises primarily from the magnetic nature of the manganese atoms. Therefore the electronic and magnetic sub-lattices are one and the same such that they must interact strongly. The intimate connection with the crystal lattice arises both because $`Mn`$ is Jahn-Teller (JT) distorted by charge carriers, and also because the radius of the A-site cations is invariably less than ideal.

Several recent reviews provide colourful insights into the macroscopic and microscopic nature of the manganites . Here we concentrate on sub-micron mesoscopic length scales over which there is growing evidence for multi-phase coexistence. We argue that Landau theory will provide a natural explanation for these mesoscopic phenomena, and suggest a strategy that would enable self-organised structures to be generated in a controlled manner.

As a caveat we note that historically, evidence for phase separation in the manganites has come from several directions; an old reference known to us dates back to 1977 . The evidence we describe in this article is by no means complete. For example, we concentrate on the cubic manganites and neglect the Ruddlesden-Popper layered manganites in which phase separation has been seen .

## 2 Basic physics of manganites

$`La_{1x}Sr_xMnO_3`$ is a prototype for the broad class of cubic perovskite manganites, where with replacement of a trivalent rare earth by a divalent alkaline earth, the nominal valence of $`Mn`$ can be continuously tuned between $`3+`$ (corresponding to the Mn(III) configuration found at x=0) and $`4+`$ (corresponding to the Mn(IV) configuration found at x=1). The important physical ingredients can be seen by reference to Fig. 1.

In a cubic environment, the $`Mn`$ $`d`$ levels are crystal-field split into a low lying triplet of $`t_{2g}`$ symmetry and a doublet of $`e_g`$ symmetry. $`Mn`$ is a strongly correlated ion whereby double occupancy of the tightly bound $`d`$ orbitals is suppressed by Coulomb repulsion, and the direct on-site exchange interaction aligns the spins in the different $`d`$ orbitals. The $`t_{2g}`$ levels are strongly localised, whereas an electron in the higher lying $`e_g`$ state is potentially itinerant. At $`x=0`$, each $`e_g`$ level is singly occupied: double occupancy of these highest occupied $`e_g`$ levels is suppressed by Coulomb repulsion, and $`LaMnO_3`$ is an antiferromagnetic Mott insulator. At finite doping ($`x>0`$), there are some empty $`e_g`$ levels, and hence hopping is possible. The exchange (Hund’s rule) coupling $`J`$ between the spin of an itinerant carrier and each core spin is rather larger than the hopping matrix element $`t`$ between neighbouring $`e_g`$-levels. Consequently, each conduction electron is forced to align with the core spin texture (this may be viewed as a strong-coupling version of the RKKY interaction). Thus the effective hopping matrix element between $`Mn`$ sites is $`t\mathrm{cos}(\theta /2)`$, where $`\theta `$ is the relative angle between neighbouring core spins. Clearly, the kinetic energy of the conduction electrons is minimised (maximum bandwidth) if the core spins are parallel to one another, and this so-called double exchange is the fundamental mechanism  of metallic ferromagnetism at low temperatures in the doped manganites. At a sufficiently high temperature the energy of this ferromagnetic configuration is overwhelmed by the entropy gain available from a randomisation of the manganese spin system. Thus the system lowers its free energy by entering the paramagnetic state.

Another important feature of the manganites arises from the doubly-degenerate $`e_g`$ level in Fig. 1. This degeneracy may be broken by a Jahn-Teller (JT) distortion of the oxygen cage away from cubic symmetry that lowers the energy of the occupied $`e_g`$ level on the $`Mn^{3+}`$ ion. In pure $`LaMnO_3`$, there is an antiferrodistortive arrangement of the distorted octahedra , leading to a “doubled” unit cell. This is to be distinguished from an equivalent and simultaneous source of doubling of the unit cell due to rigid rotations of the octahedra, which are promoted by the small size of the A-site cations. (These rotations mainly affect O-Mn-O bond angles whereas the Jahn-Teller distortions mainly affect O-Mn-O bond lengths.) Since the $`e_g`$ level is progressively depopulated with increasing $`x`$, the tendency toward JT distortion is suppressed; the long-range-ordered antiferrodistortive phase disappears near $`x=0.2`$. It is important to note that the lattice displacements associated with the JT distortions are large and therefore the disappearance of the long-range order does not mean that (static or dynamic) JT fluctuations may not be pronounced. Such fluctuations have been discovered to be very prominent in the manganites.

On top of these JT fluctuations — be they static or dynamic — are the additional static distortions mentioned earlier that arise because the radii of the A-site cations are invariably less than the 1.30 $`\AA `$ required for the ideal manganese perovskite structure . Looking through the Attfield chemical window  one can see, for example, that at an electronic doping level that is particularly favourable for ferromagnetism (x=0.3), a high Curie temperature is achieved when the average A-site cation radius is large and the variance in this quantity is small — such that distortions and disorder are respectively minimised.

Both these JT fluctuations, and small A-site cations of varying radii, promote mixed-valent insulating phases of the manganites. The Mn (III) configuration will have a tendency to distort, whereas the Mn(IV) configuration will not. Because every electron in a local $`e_g`$ level carries around its own JT lattice distortion, this would appear to provide a recipe for insulating phases at any composition.

### 2.1 Low temperature ferromagnetic metallic phases (FMM)

If one is close to the ideal perovskite structure in the (x=0.3) Attfield chemical window then enough of the $`OMnO`$ bonds are sufficiently linear to make $`t`$ so large that the ground state is ferromagnetic by the means described above — whence the charge carriers are delocalised such that JT fluctuations are suppressed. One of these delocalised charge carriers is like the quantum-mechanical “particle in a box”: its energy is lowered when the box is made bigger, provided that any internal structure within the box can be ignored.

### 2.2 Charge-ordered insulating phases (COI)

Even when the JT fluctuations do indeed make for an insulating ground state, there can be order because the oxygen octahedra share corners; distortions about one $`Mn`$ site are anti-shared with a neighbour. Steric conflicts can be solved in ordered phases (such as undoped $`LaMnO_3`$), and in TEM it is common to observe “striped” phases consisting of diagonal arrays of Mn(III) and Mn(IV) . These striped phases predominate in $`x`$0.5 where the larger and asymmetric Mn(III) species are in the minority such that packing is easier. In these localised phases, the spin couplings are via superexchange, mostly antiferromagnetic, and naturally somewhat smaller than the ferromagnetic double exchange interactions in the metal.

In fact the term COI is used here to refer to a multiplicity of phases, including the parent antiferrodistortive ($`x`$=0) phase, and the striped phases that have been reported with several different periods that are commensurate with the lattice, especially periods of 2 (near $`x`$=1/2) and 3 (near $`x`$=2/3) . A naive counting of the ratio of Mn(III)/Mn(IV) would predict incommensurate phases with either one Mn(IV) stripe every $`(1/x)`$ in a Mn(III) environment (0$`<x`$0.5), or one Mn(III) stripe every $`1/(1x)`$ in a Mn(IV) environment (0.5$`x<`$1). However, there are undoubtedly strong commensurability effects that will stabilise the commensurate phases away from their “correct” nominal composition. The nature of the repeating units in stripe phases — be they commensurate or not — is not universally agreed upon. In the prevailing “bi-stripes” picture  the widths of the Mn(III) and Mn(IV) stripes are different. In the Wigner crystal model they are of equal width . There are also phases that may be charge-ordered, but not orbitally ordered — i.e. the orientation of the JT distortions are random, or strongly fluctuating locally . We shall suggest some other possibilities later.

### 2.3 The high temperature paramagnetic phase (PMI)

The recent burst of interest in the manganites was initially motivated by the discovery reported in 1994 of the bulk “colossal” magnetoresistive (CMR) effect in the paramagnetic phase at temperatures just around the Curie point . In situations and compositions (e.g. $`La_{0.7}Ca_{0.3}MnO_3`$) where a large CMR is achieved in this way, the paramagnetic state is found to be quasi-insulating (activated resistivity), and this has been tracked to the presence of large polaronic (JT) fluctuations in the paramagnetic insulator (PMI) which are strongly suppressed in the FMM . In this case, the high temperature competition for the FMM is not with the ordered mixed-valent insulator, but with something resembling a melted version of it — let us call this a “polaronic liquid”.

Note that nearer to the ideal perovskite structure in the (x=0.3) Attfield chemical window the dynamic polaronic fluctuations and hence CMR are suppressed in the paramagnetic phase. This is the case with $`La_{0.7}Sr_{0.3}MnO_3`$ above $`T_C`$ — which consequently has a metallic resistivity in that it rises with increasing temperature . In fact, there is no symmetry distinction between this paramagnetic metal (PMM) and the PMI, and the crossover (with varying composition) between these phases is generally smooth.

## 3 Competing phases

The three basic phases described above (COI, FMM and PMI) compete to be the stable thermodynamic phase. What can happen near the FMM/COI boundary is of particular interest in this article because there is no reason of symmetry why charge ordering and ferromagnetism cannot coexist. Instead it depends on the driving physics. This suggests that the transition between the two types of ordered phases will be first order — which seems to be the case (at least at low temperatures).

Below we argue that the spatial extent of a “phase” cannot be too small, and go on to describe some of the evidence for texture in the manganites that arises over length scales that are at least microscopic. We then consider the strong evidence for texture over longer length scales, i.e. “phase separation”.

### 3.1 Microscopic fluctuations

The PMM/FMM transition in $`La_{0.7}Sr_{0.3}MnO_3`$ described in Section 2.3 is continuous (second order) and smooth at the microscopic level as evidenced by ferromagnetic resonance measurements . The FMM/PMI transition (e.g. in $`La_{0.7}Ca_{0.3}MnO_3`$ as also described in Section 2.3) is also usually continuous . However more generally, a thermodynamically continuous (second order) transition is not necessarily smooth microscopically: it could be an order-disorder transition rather than a microscopically smooth “displacive” order-order transition. This order-disorder type of continuous (second order) transition can only be distinguished from a thermodynamically discontinuous (first order) transition if the length scale of the measuring probe is sufficiently long. Experimentally there is plenty of evidence to demonstrate the existence of at least short-range texture at the unit cell level, some of which we now describe below.

NMR studies in an applied magnetic field can probe both the ionisation state and the local magnetic environment of the $`{}_{}{}^{55}Mn`$ atoms. All around the phase diagram it is typical to find Mn(IV)/Mn(III) species coexisting with Mn species whose NMR signal is motionally narrowed . Such motional narrowing is indicative of the presence of metallic regions. However, in principle, motional narrowing can also arise if the energy levels accessible to a somewhat localised electron become blurred (e.g. due to thermal or interaction effects). Therefore, to be pedantic, we consider the existence of a motionally narrowed line to be good evidence rather than concrete proof for the existence of metallic phases. This technicality notwithstanding, NMR studies lead us to believe that there are metallic clusters in surprising places: above $`T_C`$ on the $`x<0.5`$ hole-doped side  and at 3 K on the $`x>0.5`$ electron-doped side where AF stripe phases predominate . A particularly interesting feature of NMR is that one can see whether or not the frequency of a motionally narrowed resonance will fall with the bulk magnetisation on increasing the temperature : if it does fall then we have a second order displacive transition; if it does not then we infer that the $`Mn`$ atoms are not all sitting in the same environment. However, since NMR is sensitive only to the local environment, this does not establish the existence of two thermodynamic phases: the disorder might only arise at the microscopic level.

Neutron data can reveal short-range order (as well as long-range order, discussed later). For example, in the $`La_{1x}Ca_xMnO_3`$ system when $`x=0.3`$, recent zero-field neutron spin echo studies of the low temperature FM phase have demonstrated inhomogeneity on a length scale of $`30\AA `$; and parallel muon studies suggest that the spin dynamics in the different regions are very different . Moreover, inelastic neutron scattering experiments have revealed that this low temperature FM phase contains soft zone boundary magnons and phonons .

Short-range order in $`x=0.3`$ systems has also been seen near $`T_C`$ using neutrons: the spin wave stiffness is found to remain finite  (c.f. the NMR evidence described above); and a superlattice with correlation length $`10\AA `$ is found to develop . This latter finding extends earlier studies near $`T_C`$ in which neutron pair distribution functions demonstrated the existence of JT distortions with short-range correlations . Similarly, early findings with SANS revealed the existence of local magnetic clusters with a length scale of $`12\AA `$ . There is similar evidence for these short-range correlations near $`T_C`$ from a recent high energy x-ray powder analysis ; and EXAFS studies in which the $`Mn`$ K-edge resonance is affected by local correlations .

Regarding short-range order at other doping densities: in the $`La_{1x}Ca_xMnO_3`$ system at $`x=0.15`$, the FMM ground state found at higher $`x`$ is replaced with a novel form of short-range orbital and charge order, according to bond valence sum calculations based on neutron powder diffraction data . It is around this doping density that canted spins  were originally postulated — effectively as an interpolation between the antiferromagnetic end member at $`x=0`$ and the FMM region at higher $`x`$. The evidence for novel short-range order presented in , and the presence of both “FM” and “AFM” peaks in NMR studies using an applied magnetic field , tend to rule out canting in favour of the postulated  microscopic texture. However the two scenarios are not mutually exclusive and in $`LaMnO_{3.02}`$ the 250 MHz NMR line displays a field-dependent slope that corresponds to half a gyromagnetic ratio; this indicates a canted state .

In $`x0.5`$ there is both neutron and TEM evidence for the so-called stripe phases that constitute the COI phase. We discuss this region of the phase diagram in the next section.

The experiments described above, and certain others, can be adduced as evidence for the existence in the manganites of inhomogeneities that arise over length scales that are comparable with unit cell dimensions. In some cases such experiments point to, but do not prove, the existence of inhomogeneities arising over somewhat longer length scales. These larger inhomogeneities form the subject of this review and in the next section we consider some of the strong and recent evidence for their existence. For now let us be clear: we reserve the term “phase separation” for the coexistence of mesoscopic and macroscopic thermodynamic phases.

### 3.2 Phase separation and coexistence

Whenever there is a first order phase boundary, there can be coexistence between phases. An unconstrained system in which there is a first order phase boundary should in principle be in one phase or the other at equilibrium. However in practice coexistence is liable to arise for several reasons.

Equilibrium coexistence of two thermodynamic phases generally occurs either because of disorder (where locally one phase is favoured over the other) or because of an imposed conservation law. The classic case of the latter is of the liquid/gas transition in a system of fixed volume, where the equilibrium fractions of the liquid and gas will adjust in order to fill the available space. When external parameters of the system are changed (e.g. temperature, volume), the two phases readjust in different proportions. If the readjustment is impeded, there will be hysteresis.

The phenomenon of hysteresis is often cited as evidence for phase coexistence. To be precise, it constitutes indicative but not conclusive evidence. For example, hysteresis loops of magnetisation versus applied magnetic field can arise in some rare-earth magnetic systems solely because the degree of saturation dictates the strength of the reverse field required to induce nucleation. In another example, hysteresis can be produced by supercooling, but this is a kinetic phenomenenon.

Electronic phase separation is often discussed in the context of the manganites . While it is no doubt a valid point of view to consider the mixed-valent charge-ordered phases as examples of microscopic electronic phase separation, the Coulomb energy associated with substantial charge density fluctuations on length scales longer than a few lattice constants is prohibitive. When we have coexistence between phases on long length scales, the electronic charge densities must be very nearly the same. We stress that in this and the subsequent sections of this article, we concern ourselves with phases that by definition (see section 3.1) extend over at least several unit cells.

A number of experiments have demonstrated that over wide ranges of compositions there can be coexistence between the FMM and COI phases (particularly period 2 or “1/2”-type). Perhaps the most visual and direct evidence for this type of coexistence comes from dark-field TEM images of $`La_{5/8y}Pr_yCa_{3/8}MnO_3`$ at 20 K . Sub-micron domains appear bright because they contain the extra periodicity associated with a COI phase, whereas the interspersed dark regions of similar size are inferred to be FMM through percolative resistivity measurements . Neutron powder data taken for compounds of similar compositions reveal the presence of both FM and AFM peaks, each with a different temperature dependence . This demonstrates directly the presence of two phase coexistence: each phase must extend over at least some hundreds of Angstroms in order to produce the neutron diffraction peaks. A more recent analysis estimates this distance to be not less than 500 $`\AA `$ and possibly even 1000 $`\AA `$ . A slightly more complicated phase separation arises hysteretically in $`Nd_{0.5}Sr_{0.5}MnO_3`$ powder samples below 145-175 K: the majority of the orthorhombic crystal, part of which is a FMM, undergoes a transition to a monoclinic COI phase, as evidenced by neutron diffraction and strain gauge data . Since a structural phase transition accompanies the appearance of the COI phase, one anticipates the eventuality of strain-driven phase separation in the manganites (see Section 4).

Further demonstrations of the FMM-COI interplay are found in sintered powder/thin film experiments. Sintered samples of the potentially COI material $`La_{0.5}Ca_{0.5}MnO_3`$ only develop a conducting path and a large magnetisation when the grain size is small, i.e. when there is a large amount of strained grain boundary material present . Similarly, a strained epitaxial film of $`La_{0.5}Ca_{0.5}MnO_3`$ was found to posess a FMM ground state , but this strain must be of the correct type . These experiments demonstrate the important role of strain, which is expanded upon below and in the next sections on Landau theory.

In the vicinity of the FMM/PMI phase boundary, Jaime et al.  argued some time ago that transport and thermodynamic data could be quantitatively described by a model of coexisting phases, rather than a homogeneous transition. There is also some very visual imaging evidence to support the strain-induced coexistence of the FMM and PMI phases in manganites. Scanning tunnelling microscopy scans suggest that a thin strained film of $`La_{0.7}Ca_{0.3}MnO_3`$ contains both metallic and insulating regions; and that the insulating sub-micron regions even persist at low temperatures and in high magnetic fields . Alternatively, temperature dependent magnetic force microscopy studies near an artificial grain boundary in a thin strained film of $`La_{0.7}Sr_{0.3}MnO_3`$ reveal that the FMM state persists within a micron of the boundary at temperatures above which the ferromagnetism in the rest of the film survives . Again, the most likely interpretation of these two experiments is that strain and strain relief respectively create the long-range inhomogeneity.

Mesoscale coexistence of the COI phase with an insulating spin glass phase over (500-2000) $`\AA `$ has been observed in a powdered sample of $`Pr_{0.7}Ca_{0.3}MnO_3`$ using neutrons . This coexistence may be understood in terms of intragranular strain-driven segregation. The glassy phase melts into a metal under the influence of an applied magnetic field (c.f. melting the COI in $`Nd_{0.5}Sr_{0.5}MnO_3`$ ); and in a single crystal of similar composition $`(Pr_{0.63}Ca_{0.37}MnO_3)`$ there is found to be a large latent heat associated with a similar transition (i.e. thermodynamic evidence from calorimetry for first order behaviour) and a time-dependent specific heat in the coexistence regime that relaxes on a scale of tens of seconds . Relaxation phenomena have been observed elsewhere too, for example in ultra-thin strain films of $`La_{0.7}Ca_{0.3}MnO_3`$  and in $`Nd_{0.5}Ca_{0.5}Mn_{1y}Cr_yO_3`$ $`(0y0.1)`$ crystals .

Various other measurements of hysteresis , noise  and thermopower  also indicate two-phase coexistence; and various strategies for obtaining two-phase coexistence have been employed. For example, on the Mn(IV)-rich side of the $`La_{1x}Ca_xMnO_3`$ phase diagram near $`x=0.9`$ a cluster glass state develops and colossal magnetoresistance effects are seen . Similarly replacing 15% of the $`Mn`$ atoms with $`Cu`$ to produce $`La_{2/3}Ca_{1/3}Mn_{0.85}Cu_{0.15}O_3`$ appears to generate both FMM and COI regions as evidenced by transport and magnetisation measurements as a function of field and temperature .

Regarding the interpretation of the above examples (and many more), it is clear that the properties of a manganite are liable to be strongly dependent on the nature of the sample: the strain states and defects will vary between single crystals, powders, sintered powders and thin films. We note that from some perspectives, the propensity for twinning in the manganites reduces the value of single crystal studies in favour of free (non-sintered) powder samples since it is possible for each micron-sized grain to act like an untwinned single crystal. One is confident that the phase separation seen in neutron powder diffraction studies is not due to surface effects since, as mentioned five paragraphs ago, each phase must extend for hundreds of Angstroms to be seen at all with neutrons. Twinning may also be avoided by recourse to thin films.

Remarkably, the proportions of two coexisting phases can be easily “tweaked” by external parameters that include pressure , magnetic fields , temperature , these three parameters together , strain , electrical currents  and X-ray  or electron illumination .

We have argued elsewhere  that the equilibrium coexistence of two phases over a wide range of parameter space is most likely produced by the clamping effects of external and internally-generated strain fields. We must now ask what sets the length scale of the coexistence. We shall see that there is an intriguing possibility that the competing phases can self-organise over mesoscopic distances. Moreover, these self-organised structures may themselves constitute true thermodynamic phases.

## 4 Landau theory

It would be desirable, if possible, to construct a complete theory for the manganites from a fully microscopic basis. In fact, there is a good microscopic understanding of the homogeneous phases , and some evidence for texture near first order transitions . A full understanding of mesoscopic texture from a microscopic basis is a complex exercise because of the vast phase space to be explored. Moreover, such an exercise could turn out to be unnecessarily reductionist. Instead then, it may be useful, at least initially, to simplify the analysis by postulating a Landau theory for the various coupled order parameters (magnetism, charge-order, strain). Such an approach has turned out to be very valuable in the case of ferroelectric/ferroelastic transitions , and especially valuable for the case of incommensurate and commensurate phase charge-density wave systems . A full Landau theory for the case at hand is still very complicated and has not yet been fully explored . We shall restrict ourselves to a few simple scenarios. Of course, even with its simplifications, the Landau theory can only demonstrate possibilities, because the real physics lies in the values of the parameters of the theory, which we can only either guess at, or fit to experiment.

### 4.1 Strain effects in a commensurate striped phase

In a phase transition to a striped periodic phase, there is a development of an order parameter with a wavevector $`𝐐_i`$, where the subscript denotes one of the (several) directions of the possible stripes. Then we may write the full order parameter as

$$\rho _if(𝐐_i𝐫)$$
(1)
so that $`\rho _i`$ is the amplitude, and the function $`f`$ is a periodic function of its argument. The simplest Landau theory for the transition would then be contained in the following expansion of the free energy

$$_\rho =\underset{i}{}\left(\frac{1}{2}a(T)\rho _i^2+\frac{1}{4}b\rho _i^4+\frac{1}{6}c\rho _i^6+\mathrm{}\right)+\underset{i>j}{}b_{ij}\frac{1}{4}\rho _i^2\rho _j^2+\mathrm{}$$
(2)
For diagonal stripes, the sum must run over the possible equivalent $`\{110\}`$ directions (we index throughout with respect to the pseudo-cubic unit cell). For simplification we shall just consider the case when we may have one of the two $`(110)`$ (labelled $`i=1`$, say) and $`1\overline{1}0`$ $`(i=2)`$ directions in two dimensional symmetry.

It is conventional to assume that $`a(T)=a_o\times (TT_o)`$, so that the quadratic coefficient changes sign below a temperature $`T_o`$. Depending on the sign of the coefficient $`b`$, the model will predict a first order ($`b<0`$) or second order ($`b>0`$) transition. We shall need to choose $`b_{12}>0`$, so as to have a striped, rather than checkerboard phase as the lowest energy state.

Because the presence of the order parameters breaks the cubic symmetry, the order parameters must couple to shear strain $`s`$. This will lead to terms of the form

$$_s=\frac{1}{2}Ks^2+ds(\rho _1^2\rho _2^2),$$
(3)
where $`K`$ is the elastic constant and $`d`$ is another constant that describes the strength of the lowest order coupling term allowed by symmetry. Note that the sign of this coupling is opposite for the two order parameters, because the stripes run in orthogonal directions (we have picked axes for the tetragonal distortion along the $`(110)`$ and $`(1\overline{1}0)`$ directions).

Now imagine that we have a homogeneous situation, with $`\rho _10`$, and $`\rho _2=0`$, so that only one of the two kinds of stripes is present. We can determine the magnitude of the order parameter $`\rho _1`$, by looking for the minimum in the free energy. In the case where the strain is free to relax, we have from $`_s/s=0`$ that

$$s=\frac{d\rho _1^2}{K}.$$
(4)
As expected, a shear strain will accompany the stripe transition (c.f. the structural transition to a monoclinic COI phase described earlier ). Substituting this back into the free energy, which is now just a function of the single variable $`\rho _1`$, we have

$$(\rho ,s(\rho ))=_\rho \frac{d^2}{2K}\rho _1^4,$$
(5)
so that the strain relaxation makes the fourth-order coefficient more negative in the reduced free energy. This means that a transition that was already first order is made more strongly so such that $`T_o`$ is raised. It is also possible that initially $`b>0`$, but that $`b2d^2/K<0`$, so that a second-order transition — if the strain were clamped ($`s=0`$) — can be driven first order if the strain relaxes. Even more dramatically, if $`b`$ is sufficiently large and positive, the transition might in fact only occur at all if the strain is allowed to relax. Such phenomena are quite common in ferro-electric and ferro-elastic oxides .

In principle, we should also have a term $`_m`$, describing the magnetic free energy. In order not to complicate the discussion more than necessary, we shall not include it explicitly. Instead, we assume that the dominant terms are $`_\rho `$, and $`_s`$, and assert that (metallic) ferromagnetism will appear as the low temperature phase if the COI is suppressed — i.e. the ferromagnetism is slave to the absence of charge order.

In the manganites there is now a wide body of evidence to demonstrate that clamping the strain can produce pronounced effects. For example, as described earlier Section 3.2, compositions in which the equilibrium strain relaxed phase is the COI tend to adopt the FMM phase if the strain is clamped in the right way, either by imposed external stresses, or by internally generated stresses in multi-domain samples — such as micron-sized grains in free powders .

Strain-induced interactions are long-range, and can lead to pronounced kinetic effects, familiar in the martensites . Since the shear strain induced by two orthogonal striped domains is of opposite sign, the strain cancels at long distances such that the arrangement shown in Fig. 2a is favoured by nucleation in a bulk or clamped environment. However the strain fields are incompatible unless the two domains meet in a macroscopically strain-free fashion as shown in Fig. 2b. Either way there is the possibility of untransformed material between the two domains, which if sufficiently large we may expect to become a ferromagnetic metal.

### 4.2 Twin boundary between striped domains

In a $`90^{}`$ twin boundary (Fig. 2b), the interface between the two different stripe domains bisects the $`90^{}`$ angle between the domain orientations. Such a configuration potentially allows macroscopic strain relaxation for both domains (Fig. 2b). If there are indeed domains in a sample, such twins have the lowest strain energy. However, the domain boundary cannot be atomically abrupt, especially because we do not expect the different order parameters for each domain to overlap $`(b_{12}0)`$; neither, equally, do we expect these order parameters to jump abruptly to zero. More likely is the situation sketched in Fig. 3a, where the two order parameters decay over a length scale $`\xi _o`$ which is typically larger than a lattice constant (and even larger for smaller amplitude charge order modulations). If the coherence length $`\xi _o`$ is large enough, then it is clearly possible that the twin boundary itself is locally a ferromagnetic metal. Synchrotron x-ray diffraction evidence consistent with this scenario is found in single crystal $`La_{5/8y}Pr_yCa_{3/8}MnO_3`$ , but not, for example, in $`(Pr,Sr,Ca)MnO_3`$  implying that the proposed scenario is not universal.

### 4.3 Domain wall in the FMM

Competition between COI and FMM could also appear when the ferromagnetic phase is the stable ground state if we impose a magnetic domain wall, as in Fig. 3b. Usually magnetisation decays near a boundary over a long length scale determined by the (Heisenberg) exchange parameter and the magnetic anisotropy. One would therefore expect a negligibly small reduction in electronic bandwidth. If however, the suppression of the magnetisation at the FM domain wall were to lead to local charge order , this will produce a magnetic weak link akin to what is observed in fabricated magnetic tunnel junctions. Such effects may be responsible for the surprisingly large electrical resistance  of albeit apparently wide  magnetic domain walls in thin films.

### 4.4 Incommensurate striped and magnetic phases

In the case of the twin boundary and magnetic domain walls just described, we imagined that these configurations were imposed by external conditions. There is a further possibility, however, that such configurations may not be thus externally (or kinetically) imposed, but might also form long-period thermodynamic phases. To see how this might come about, we should understand how in the Landau theory we might incorporate the chemical tendency to match the period of the COI phases to the nominal Mn(III)/Mn(IV) ratio. Within the weak coupling approach of the Landau theory, one can allow for this by generalising the Landau theory to a complex order parameter

$$\psi _i=\rho _i(𝐫)e^{i(𝐐_i𝐫+\varphi _i(𝐫))},$$
(6)
where the physical charge density modulation is $`|\psi _i(𝐫)|`$. If we choose the period $`𝐐_i`$ to be commensurate with the lattice $`𝐐_i=𝐆_i/n`$, with $`n`$ an integer, and $`𝐆_i`$ a reciprocal lattice vector of the parent phase, then we can incorporate the possibility of structures with incommensurate periodicities by the phase variable $`\varphi (𝐫)`$. New terms in the free energy dependent upon the phase can have the following form

$$_\varphi =\xi _o^2|(iq)\psi _i|^2g\mathrm{}(\psi ^ne^{i𝐆_i𝐫})+\mathrm{}$$
(7)
The first term represents the preference for an incommensurate phase (where $`q`$ changes with concentration), and the second term is a commensurability (Umklapp) term that lowers the energy when the density wave lines up appropriately with the underlying lattice ($`g`$ is a constant and the operator $`\mathrm{}`$ returns the real part of its argument).

When the amplitude $`\rho _i`$ is stiff, these terms in the free energy can be simplified to give

$$_\varphi \xi _o^2\rho _i^2|\varphi q|^2g\rho _i^n\mathrm{cos}(n\varphi _i(𝐫)).$$
(8)
Here, we assume that the amplitude $`\rho _i(T)`$ is already fixed by the minimisation of (2) and (3). The minimisation of (8) produces the well-known sine-Gordon equation, and solutions which are solitons. Without discussing the details, notice that if the first term in (8) were dominant, then the phase will tend to “wind” with gradient $`q`$, whereas the second term suppresses the phase slips and prefers the commensurate phases $`\varphi =2\pi j/n`$. Arrays of solitons (“discommensurations”) arise at the minimum of the free energy intermediate between these limits. Furthermore, note that for $`n>2`$, the last term is of higher order in $`\rho _i(T)`$ than the first, so that there is generically the possibility of a transition from a commensurate to an incommensurate state with increasing $`T`$ (and reducing $`\rho _i`$), whereas no such transition is expected for $`n=2`$. This may help to account for the great stability of “1/2” type ordering in the manganites, which exists for a wide range of dopings. Incommensurate states are seen near $`x=2/3`$, however, and “frozen-in” discommensurations are sometimes visible in electron micrographs at low temperature in this region of doping .

That the phase and amplitude can be so cleanly separated is an approximation justified only in the weak coupling limit when $`\rho _i1`$, and $`\xi _o|𝐐_i|1`$. This is probably a poor approximation for the large amplitude distortions common to the manganites, in which case other potential long period phases may be favoured by the competition between the two principal order parameters, modulated by the imposed periodicity $`q`$ (note that $`q`$ acts like — and in fact couples to — a lattice strain). One speculation is the possibility of a novel incommensurate magnetic/CO phase, that can be made by a periodic arrangement of either of the configurations shown in Fig. 3. It is therefore possible that these types of configurations may not exist solely because they are externally imposed: they may be thermodynamically stable in their own right.

## 5 Manipulation of self-organised structures

We remarked near the end of Section 3.2 that it is not the coexistence of different phases in the manganites that is remarkable, but rather the fact that the proportions of these phases can readily adjust to small external forces. It seems therefore that the existing components are indeed in local equilibrium, and that their coexistence is not necessarily enforced because of strong hysteresis or pinning. The ideas framed in the Landau theory of the previous section allow for such a delicate balance, because of the pervasive effects of long-range strain fields.

Two (and perhaps more) broad possibilities allow for quasi-equilibrium coexistence. One is that the domain configurations are topologically frozen in. This is understandable because rearrangements that would remove large domains are kinetically disallowed. Nevertheless, local readjustments could easily be made — for example to the proportion of the FMM and COI phases in a frustrated configuration like the one sketched in Fig. 2a. Another class of possibilities is that one has not just the COI and FMM as stable thermodynamic phases, but in addition a host of incommensurate structures built out of periodic arrangements of these two basic subunits. This type of situation is certainly favoured by the natural tendency to incommensurability away from special doping values.

The potential range of self-organising structures in the manganites suggests that it should be possible to produce patterns in a controlled manner — in principle for the purpose of information storage. Strain templating is likely to be an effective means of achieving this because strain is so important in these materials — as discussed throughout this article. The possibility of x-ray lithography  and the use of currents  to pattern domains has already been suggested.

## 6 Conclusions

The mesoscale complexity that can arise in the manganites is reminiscent of the complexity that arises in the high temperature superconducting cuprates, or even organic systems. Because the crystal structure of a manganite interacts strongly with the corresponding magnetic and electronic structures, any imposed physical discontinuities in actual samples will likely create or destroy the delicate phase balances that we have described in this article. The challenge is therefore to better demonstrate the intrinsic nature of coexistence in the manganites, and to exploit this coexistence to produce self-organised structures over mesoscopic length scales.

## Acknowledgements

We thank for helpful discussions C.J. Adkins, J.P. Attfield, L. Brey, M.J. Calderón, C.H. Chen, S.-W. Cheong, Cz. Kapusta, P. Levy, A.J. Millis, D.V. Sheptyakov and B.B. van Aken. We also wish to thank M.G. Blamire, J.E. Evetts, M.-H. Jo, S.J. Lloyd, J.C. Loudon, P.A. Midgley and N.K. Todd for support and helpful discussions. We are grateful for the support of INTAS, the UK EPSRC, the Royal Society and Churchill College, Cambridge.


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# Hydro+Cascade, Flow, the Equation of State, Predictions and Data

## 1 Introduction

Relativistic Hydrodynamics provides a link between the Equation of State(EoS) of the excited nuclear matter and collective observables such as elliptic flow($`v_2`$-s) and radial flow($`T_{slope}`$-s). At the SPS, pure hydrodynamics calculations can fit the transverse mass spectra for almost any EoS by choosing the freezeout temperature $`T_f`$. However in non-central collisions, when $`v_2`$ was calculated for these same EoSs with the same $`T_f`$-s, $`v_2`$ was above the data by a factor of two. Bass and Dumitru removed the $`T_f`$ indeterminacy by injecting the particles into a microscopic transport model at a switching temperature $`T_{switch}T_c165MeV`$, and cascading the particles until they decoupled. With the freezeout parameter removed, the slope parameters for central PbPb collisions were calculated and found to agree with experimental values. The only parameter in this approach is the total multiplicity in the collision.

Later, elliptic flow was calculated in a similar Hydro+Cascade model and $`v_2`$ was only 20% above the data. Since at freezeout the viscosity is certainly important, it was not surprising that the introduction of a cascade reduced the elliptic flow. It $`was`$ surprising that Hydro+Cascade could simultaneously reproduce the elliptic $`and`$ radial flow for different particle species as a function of impact parameter. Furthermore, the combined analysis of radial and elliptic flow restricted possible EoSs since the freezeout temperature could no longer be adjusted to make any EoS fit any slope parameter. Roughly speaking, a soft EoS produced too little radial flow while a hard EoS produced too much elliptic flow.

Now, with the EoS roughly fixed from available SPS data, parameter free predictions were made for RHIC. A few of these predictions are: (a) an increase in $`v_2`$ by approximately 40% over the SPS and (b) a significant increase in the radial flow. (c) curved nucleon $`m_T`$ spectra. The preliminary data reported in this conference have been in agreement with these predictions .

Ideally, the cascade should provide a kind of dual description of the hydrodynamics. Although $`T_c`$ provides a natural place to switch to the cascade, the results (slope parameters and $`v_2`$-s, lifetimes, etc.) should be insensitive to the switching temperature $`T_{switch}`$. Unfortunately, Bass and Dumitru reported that the results were sensitive to the transition surface. By incorporating chemical freezeout into the hydrodynamic calculation, the sensitivity to $`T_{switch}`$ was much reduced although the elliptic flow at the SPS remained sensitive to $`T_{switch}`$.

If the preliminary data remain unchanged and further predictions are verified, the hydrodynamic description must be taken seriously and the equilibration times and transport cross sections estimated from binary, perturbative, classical parton cascades must be considered only a very coarse guide to the radiating, non-perturbative, quantum glue that makes up the initial state.

## 2 The EoS, Flow, Predictions and Data

Below a family of EoSs with a first order phase transition are studied and are labeled by the Latent Heat(LH). LH4, LH8, $`\mathrm{}`$ label EoSs with a latent heats of $`0.4GeV/fm^3`$, $`0.8GeV/fm^3`$, $`\mathrm{}`$. LH$`\mathrm{}`$ is studied as a limiting case. A Resonance Gas(RG) EoS (which does not have a phase transition) is also studied.

First in Fig. 1(a), the measured slope parameters at the SPS are compared to model predictions for different EoSs. LH8 gives the best description of the available spectra. LH4 is too stiff (the slope parameters are too high) and LH16 is too soft (the slope parameters are too low). The $`T_{slope}`$-s for a RG EoS are comparable to LH4, and the $`T_{slope}`$-s for LH$`\mathrm{}`$ are comparable to LH16.

Although LH8 gives the best fit to SPS spectra, the model-data discrepancy for the other EoSs is not large. As the collision energy is increased from the SPS to RHIC the slope parameters all increase (see e.g. ). Since at high energies the importance of the QGP phase increases, the differences between these EoSs are magnified during the systems evolution. In Fig. 1(b), the model predictions at RHIC collision energies are shown for different EoSs. Note, the spectra are curved and the parameterization in terms of slope parameters is only schematic. LH$`\mathrm{}`$, with no QGP push, generates only small slope parameters. The differences between the EoSs is clear in the flow of the $`\mathrm{\Omega }`$.

With these predictions, a comparison to the first RHIC data is made in Fig. 2. The $`M_T`$ spectra are curved (see ) and therefore the STAR and PHENIX collaborations measure quite different slope parameters. The STAR collaboration fits the observed spectra in a low $`M_T`$ range and measures large slopes, while the PHENIX collaboration fits in a high $`M_T`$ range and measures small slopes. The best agreement with the proton and anti-proton slope parameters of both collaborations is found between LH8 and LH16 . LH$`\mathrm{}`$ has too much flow at small $`M_T`$ and too little flow at high $`M_T`$ and therefore fails to reproduce the curvature of the $`M_T`$ spectra seen in the data. The slope parameters reported in this conference implicate a strong transverse expansion.

Now, elliptic flow is studied as a function of impact parameter. In Fig. 3(a) and (b), the elliptic flow of pions/charged particles at the SPS and RHIC is shown for different EoSs. Notice that elliptic flow increases by approximately $`40\%`$ from the SPS to RHIC. This prediction was borne out by the first STAR measurements. At the SPS, EoSs without or only a very weak phase transition (e.g. RG or LH4) produce far too much elliptic flow. At the SPS, LH8 and LH16 give approximately the same elliptic flow since the contribution to $`v_2`$ of the pure QGP phase is small. At RHIC, the $`v_2`$-s of LH4, LH8 and LH16 begin to separate as the QGP phase becomes increasingly significant.

Acknowledgements. P. Kolb is thanked for critically reading this manuscript. This work is partly supported by US DOE grant No. DE-FG02-88ER40388 and grant No. DE-FGO2-87ER 40331.


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# Nonlinear vertical oscillations of a particle in a sheath of a rf discharge

## Abstract

A new simple method to measure the spatial distribution of the electric field in the plasma sheath is proposed. The method is based on the experimental investigation of vertical oscillations of a single particle in the sheath of a low-pressure radio-frequency discharge. It is shown that the oscillations become strongly nonlinear and secondary harmonics are generated as the amplitude increases. The theory of anharmonic oscillations provides a good qualitative description of the data and gives estimates for the first two anharmonic terms in an expansion of the sheath potential around the particle equilibrium.

There are various experimental methods on the plasma sheath diagnostic in low-pressure gas discharges (see, e.g.,  and references therein). Most of the methods are based on optical emission spectroscopy and temporally resolved probe measurements and are rather complicated technically. We propose an “alternative” simple method to measure the spatial distribution of the electric field in the plasma sheath based on investigation of “large-amplitude” vertical oscillations of micron sized particles.

So far, investigation of the particle oscillations in the sheath of a radio-frequency (rf) discharge  was one of the methods used to determine the particle charge . This method is based on the assumption that the vertical distribution of the sheath potential is known and can be approximated by a parabolic profile , so that the oscillations are always harmonic. This assumption is reasonable for sufficiently high gas pressure, when the mean free path of ions is much less than the vertical spatial scale of the sheath field : For example, the model of a parabolic rf sheath in an argon plasma can be applied for pressures above $`20`$ Pa. But for $`p10`$ Pa the sheath profile might deviate strongly from a parabolic one. In this case, the oscillations are harmonic only if their amplitude is very small.

In this Letter, we report experimental and theoretical investigations of nonlinear (large-amplitude) vertical oscillations of a single particle in the sheath of a low-pressure rf discharge. We compare the experimental results with the theory of anharmonic oscillations and estimate the first two anharmonic terms in an expansion of the sheath potential around the particle equilibrium height. Thus, the study of large-amplitude particle oscillations allows us to reconstruct the distribution of the vertical electric field in wide region of the sheath.

Experimental setup and results — The experiments are performed in a so-called Gaseous Electronic Conference (GEC) rf reference cell  with the electrode system modified as shown in Fig. 1. The lower aluminum electrode, 230 mm in diameter, is capacitively coupled to a rf generator providing a peak-to-peak voltage $`70`$ V (rf power $`2`$ W). A ring-shaped upper grounded electrode with an outer diameter of 200 mm and a thickness of 10 mm is located 50 mm above the lower electrode. A 2 mm thick copper ring with a 40 mm inner diameter is placed on the lower electrode to confine the particle above the center. Argon gas at a pressure 0.5 Pa is used for the discharge. For this pressure, a self-bias voltage $`33`$ V on the lower electrode provides the sheath with a (visible) thickness of $`20`$ mm and causes a spherical polystyrene particle (density $`1.05`$ g/cm3, diameter $`7.6\pm 0.1\mu `$m) to levitate $`14`$ mm above the electrode.

At a height 8 mm above the lower electrode a horizontal wire of 0.5 mm diameter and 80 mm length is placed directly below the levitated particle. A low-frequency sinusoidal voltage of amplitude $`U_{\mathrm{ex}}`$ is applied to this wire to excite the vertical oscillations of the particle. The frequency $`\omega /2\pi `$ of the voltage could be varied from 0.1 Hz up to 40 Hz and back in 0.1 Hz steps. To determine the oscillation amplitude at each step, we illuminated the particle with a vertical laser sheet of $`140\mu `$m thickness and imaged it from the side by an external digital CCD camera (max. field rate is 50 fields/s, resolution is $`768\times 576`$ pixels).

For relatively small values of the excitation voltage ($`U_{\mathrm{ex}}30`$ mV), we observed the usual linear (harmonic) oscillations: The dependence of the oscillation amplitude on the frequency has a single symmetric narrow maximum at the resonance frequency $`\omega _0/2\pi 17.0`$ Hz (primary resonance). However, for larger $`U_{\mathrm{ex}}`$ the dependence clearly exhibits nonlinearity of the oscillations (see, e.g., ). Figure 2 shows that the maximum of the primary resonance shifts to the left, as the excitation voltage increases. When $`U_{\mathrm{ex}}`$ exceeds some critical value, a hysteresis appears. To illustrate this phenomenon, we can compare Figs. 2(a) and 2(b) ($`U_{\mathrm{ex}}=100`$ mV and 200 mV). When the frequency increases \[Fig. 2(a)\], the amplitude grows continuously until a certain frequency ($`\omega _+`$) is reached, then it “jumps” upward and thereafter decreases monotonically as $`\omega `$ is further increased. On the “way back” \[Fig. 2(b)\], the amplitude grows continuously until another frequency ($`\omega _{}`$) is reached. Then it spontaneously “jumps” downward and continuous to decrease slowly as the frequency is reduced further. We found that $`\omega _+`$ is always larger, than $`\omega _{}`$. Outside this “hysteresis zone”, the experimental points obtained for increasing and decreasing frequencies practically overlap. The shift of the maximum, as well as the width of the “hysteresis zone” rapidly increase with $`U_{\mathrm{ex}}`$.

Another peculiarity of the oscillations are the secondary resonances – two maxima at $`\omega \frac{1}{2}\omega _0`$ and $`\omega 2\omega _0`$, which are observed for sufficiently high excitation voltage. Figure 3 shows the peak in the vicinity $`\omega \frac{1}{2}\omega _0`$ (superharmonic resonance) for different values of $`U_{\mathrm{ex}}`$. We see that the dependence has a finite offset with some slope (marked by the dashed line), which represents the low-frequency tail of the primary resonance. The shape of the peaks resembles that of the primary resonance: As $`U_{\mathrm{ex}}`$ increases, the maximum shifts to lower $`\omega `$ and the hysteresis appears. In contrast, for the subharmonic resonance at $`\omega 2\omega _0`$ (Fig. 4) the dependence is qualitatively different. When $`U_{\mathrm{ex}}`$ is below a certain threshold, we see only the offset – the high-frequency tail of the primary resonance – but when $`U_{\mathrm{ex}}`$ exceeds this threshold, the amplitude increases abruptly. When $`\omega `$ is increased \[Fig. 4(a)\], the amplitude decreases very slowly along the offset line up to some point. Then the amplitude jumps upward and subsequently decreases rapidly until the resonance branch crosses the offset line. At higher frequencies the dependence again follows the offset. When $`\omega `$ is decreased \[Fig. 4(b)\], the amplitude varies approximately as in the case of increasing frequency, but there is no readjustment downward anywhere. The amplitude increases until the particle is ejected from the sheath. Both the height and the width of the peak rapidly increase with $`U_{\mathrm{ex}}`$.

It is worth noting that the amplitude of oscillations both for primary and secondary resonances is always much smaller than the sheath thickness ($`20`$ mm).

Theory and discussion — The particle oscillations are determined by the spatial distribution of the electrostatic potential, $`\varphi (z)`$, in the sheath. In the absence of excitation, a particle is levitated in the minimum of the potential well (at the height $`z=0`$), where the gravitational force, $`Mg`$, is balanced by the electrostatic force, $`Q(0)E(0)Q_0E_0`$. We assume that the equilibrium particle charge, $`Q(z)`$, changes weakly with $`z`$ \[compared to the electric field of the sheath, $`E(z)`$\], so that we can set $`QQ_0=`$ const. The particle collision experiments  in Ar discharge at pressures $`p1`$ Pa confirm this assumption: Typically, the spatial scale of the field change is approximately one order smaller than that of the charge change . The electrostatic energy of the particle, $`𝒰=Q\varphi `$, can be expanded around $`z=0`$ in the series,

$$𝒰(z)=𝒰_0^{^{}}z+\frac{1}{2}𝒰_0^{^{\prime \prime }}z^2+\frac{1}{6}𝒰_0^{^{\prime \prime \prime }}z^3+\frac{1}{24}𝒰_0^{(4)}z^4+O(z^5).$$
(1)
Using the condition of equilibrium $`Mg=QE_0𝒰_0^{^{}}`$ and the definition of the resonance frequency, $`M\omega _0^2=QE_0^{^{}}𝒰_0^{^{\prime \prime }}`$, we rewrite it as follows:

$$𝒰(z)M\left(gz+\frac{1}{2}\omega _0^2z^2+\frac{1}{3}\alpha z^3+\frac{1}{4}\beta z^4\right),$$
(2)
where $`\alpha =𝒰_0^{^{\prime \prime \prime }}/2M`$ and $`\beta =𝒰_0^{(4)}/6M`$ are the anharmonic coefficients. We keep only the first two anharmonic coefficients, because in practice they are sufficient to describe all major peculiarities of a nonlinear oscillator .

Introducing the damping rate due to neutral gas friction, $`\gamma `$, and using Eq. (2), we can write the following equation for the particle oscillation:

$$\ddot{z}+2\gamma \dot{z}+\omega _0^2z+\alpha z^2+\beta z^3=\frac{F(z)}{M}\mathrm{cos}\omega t.$$
(3)
Here $`F`$ is the excitation force acting from the wire below the particle. This force presumably depends on the vertical position of the particle, and we expand it up to quadratic terms,

$$F(z)F_0+F_0^{^{}}z+\frac{1}{2}F_0^{^{\prime \prime }}z^2.$$
(4)
First, let us consider the primary resonance $`\omega \omega _0`$. Nonlinear effects are stronger when the oscillation amplitude is larger, and therefore we are interested in a narrow region $`ϵ=\omega \omega _0`$ around the resonance frequency, where $`|ϵ|\omega _0`$. This approach is normally valid in the limit $`\gamma \omega _0`$ and is justified for our case: From the expression for the neutral friction force  we evaluate $`\gamma /2\pi 0.068`$ Hz which is much less than the measured $`\omega _0/2\pi 17.0`$ Hz. Then, we obtain from Eq. (3),

$$\ddot{z}+2\gamma \dot{z}+\omega _0^2z+\alpha z^2+\beta z^3=\omega _0^2A\mathrm{cos}(\omega _0+ϵ)t,$$
(5)
where $`A=F_0/M\omega _0^2kU_{\mathrm{ex}}`$ and $`k`$ is a “scale factor” of the oscillation amplitude, normalized to the excitation voltage. In Eq. (5) we omit the terms of higher order in $`F(z)`$, because for the primary resonance they are not important when the inequality $`A|F_0^{^{}}/F_0|1`$ is satisfied (this condition always holds in our case). In accordance with the method of successive approximations for anharmonic oscillations , the first term in the solution of Eq. (5) is $`z(t)a\mathrm{cos}\left(\omega _0+ϵ\right)t`$, and the dependence of the amplitude $`a`$ on $`ϵ`$ and $`A`$ (frequency-response equation) is given by

$$a^2\left[(ϵ\kappa a^2)^2+\gamma ^2\right]=\frac{1}{4}\omega _0^2A^2,$$
(6)
where the constant $`\kappa `$ characterizes a nonlinear shift of the primary resonance frequency,

$$\kappa =\frac{3\beta }{8\omega _0}\frac{5\alpha ^2}{12\omega _0^3}.$$
(7)
The least-squares fit of the experimental points for the low-amplitude (linear) primary resonance gives us the following values: the resonance frequency $`\omega _0/2\pi =17.0`$ Hz, the damping rate $`\gamma /2\pi =0.067`$ Hz, and the amplitude scale factor $`k=0.042`$ mm/V (note that the fitted damping rate is very close to $`\gamma /2\pi =0.068`$ Hz evaluated from the theory ). Using these values, we fit the points for the nonlinear oscillations in Fig. 2 to the function $`a(ϵ,A)`$ from Eq. (6). The solid lines represent the least-squares fit with $`\kappa /2\pi =0.96`$ Hz/mm2. If each curve is fitted independently, this value varies within $`5\%`$. The hysteresis appears on the curves, when $`A`$ exceeds the critical value: $`A_{\mathrm{cr}}^2=\frac{32}{3\sqrt{3}}(\gamma ^3/|\kappa |\omega _0^2)(2.4\times 10^3\mathrm{mm})^2`$, which corresponds to $`U_{\mathrm{ex}}60`$ mV.

For the superharmonic resonance $`\omega \frac{1}{2}\omega _0`$, we set $`ϵ=\omega \frac{1}{2}\omega _0`$. The solution of Eq. (3) is approximately a sum of the first- and second-order terms , $`z(t)z_1(t)+z_2(t)`$. The first (linear) term is $`z_1(t)=a_1\mathrm{cos}(\frac{1}{2}\omega _0+ϵ)t`$, where

$$a_1\frac{4}{3}\left(1+\frac{4}{3}ϵ/\omega _0\right)A,$$
(8)
represents the amplitude offset (dashed line in Fig. 3), and $`z_2`$ describes the resonance peak due to nonlinearity. Substituting the expression for $`z_1(t)`$ together with Eq. (4) in Eq. (3), we get the resonance terms $`z_1^2\mathrm{cos}(\omega _0+2ϵ)t`$ in the resulting equation (see Ref. ). Retaining these terms, we obtain,

$$\ddot{z}_2+2\gamma \dot{z}_2+\omega _0^2z_2+\alpha z_2^2+\beta z_2^3=\frac{8}{9}\alpha _{(\omega /2)}A^2\mathrm{cos}\left(\omega _0+2ϵ\right)t,$$
(9)
where $`\alpha _{(\omega /2)}=\alpha \frac{3}{4}\omega _0^2/\mathrm{}`$ and $`\mathrm{}=F_0/F_0^{^{}}<0`$ is the spatial scale of change of the excitation force. In Eq. (9) we omit the small terms $`O(A^2/\mathrm{}^2)`$. Formally, the derived equation for the superharmonic resonance is similar to that for the primary resonance \[see Eq. (5)\], and therefore shapes of the corresponding curves are qualitatively the same. Assuming $`z_2(t)a_2\mathrm{cos}\left(\omega _0+2ϵ\right)t`$, we obtain the following frequency-response equation for the superharmonic resonance:

$$a_2^2\left[(2ϵ\kappa a_2^2)^2+\gamma ^2\right]=\frac{16}{81}\left(\frac{\alpha _{(\omega /2)}}{\omega _0}\right)^2A^4.$$
(10)
The independent least-squares fit of the experimental points in Fig. 3 using Eq. (10) gives for each curve values of $`\omega _0`$ and $`\gamma `$, which are nearly the same as those for the primary resonance (deviation within $`0.5\%`$), $`\kappa /2\pi =1.0\pm 5\%`$ Hz/mm2, and $`|\alpha _{(\omega /2)}|/(2\pi )^2=32\pm 10\%`$ Hz2/mm. The critical value of $`A`$ for the hysteresis: $`A_{\mathrm{cr}}^4=\frac{9\sqrt{3}}{2}(\gamma ^3\omega _0^2/|\kappa |\alpha _{(\omega /2)}^2)(4.5\times 10^2\mathrm{mm})^4`$, which corresponds to $`U_{\mathrm{ex}}3.5`$ V.

Next, for the subharmonic resonance $`\omega 2\omega _0`$, we set $`ϵ=\omega 2\omega _0`$. The first-order term is $`z_1(t)=a_1\mathrm{cos}(2\omega _0+ϵ)t`$ with the amplitude offset

$$a_1\frac{1}{3}\left(1\frac{4}{3}ϵ/\omega _0\right)A.$$
(11)
Retaining the necessary terms (see Ref. ), we derive from Eq. (3) the equation for $`z_2`$,

$$\ddot{z}_2+2\gamma \dot{z}_2+\omega _0^2\left[1\frac{2}{3}\left(\alpha _{(2\omega )}A/\omega _0^2\right)\mathrm{cos}\left(2\omega _0+ϵ\right)t\right]z_2+\alpha z_2^2+\beta z_2^3=0,$$
(12)
where $`\alpha _{(2\omega )}=\alpha +\frac{3}{2}\omega _0^2/\mathrm{}`$. We see that Eq. (12) is an equation of a nonlinear parametric oscillator, and therefore the subharmonic resonance increases due to a parametric instability . Putting $`z_2(t)a_2\mathrm{cos}(\omega _0+\frac{1}{2}ϵ)t`$, we get the frequency-response equation,

$$a_2^2\left[(\frac{1}{2}ϵ\kappa a_2^2)^2+\gamma ^2\right]=\frac{1}{36}\left(\frac{\alpha _{(2\omega )}}{\omega _0}\right)^2A^2a_2^2.$$
(13)
Solution of Eq. (13) has the following peculiarities : If $`A`$ is less than the threshold value $`A_{\mathrm{th}}=6\gamma \omega _0/|\alpha _{(2\omega )}|`$, then Eq. (13) has only the zero solution $`a_2=0`$, and thus just the offset $`a_1(\omega )`$ can be observed in experiments. For sufficiently high $`U_{\mathrm{ex}}`$ ($`A>A_{\mathrm{th}}`$), a non-zero solution exists for $`ϵ_{\mathrm{b1}}<ϵ<ϵ_{\mathrm{b2}}`$, where $`ϵ_{\mathrm{b1},2}=2\gamma \sqrt{A^2/A_{\mathrm{th}}^21}`$. If the frequency increases, $`a_2`$ jumps upward from zero at $`ϵ_{\mathrm{b1}}`$ and then continuously decreases to zero at $`ϵ_{\mathrm{b2}}`$. On the “way back”, $`a_2`$ starts from zero at $`ϵ_{\mathrm{b2}}`$ and then grows monotonically. The least-squares fit of the points in Fig. 4 ($`U_{\mathrm{ex}}=2.0`$ V) with Eq. (13) gives us $`\kappa /2\pi =0.95`$ Hz/mm2 and $`|\alpha _{(2\omega )}|/(2\pi )^2=320`$ Hz2/mm. Thus, $`A_{\mathrm{th}}0.02`$ mm, which corresponds to $`U_{\mathrm{ex}}0.5`$ V. The fit for the center $`ϵ=0`$ yields $`34.85`$ Hz, which is $`2\%`$ larger than the double value of the resonance frequency obtained for the primary and superharmonic resonance.

Now we can finally reconstruct the sheath potential, $`\varphi (z)`$. Using the fitted values $`|\alpha _{(\omega /2)}|=|\alpha \frac{3}{4}\omega _0^2/\mathrm{}|(2\pi )^2\times 30`$ Hz2/mm and $`|\alpha _{(2\omega )}|=|\alpha +\frac{3}{2}\omega _0^2/\mathrm{}|(2\pi )^2\times 320`$ Hz2/mm, we evaluate the first anharmonic coefficient and the spatial scale of the excitation force: $`\alpha /(2\pi )^2130`$ Hz2/mm and $`\mathrm{}2`$ mm. Substituting this value for $`\alpha `$ and putting $`\kappa /2\pi =0.95`$ Hz/mm in Eq. (7), we estimate the second anharmonic coefficient: $`\beta /(2\pi )^220`$ Hz2/mm2. Then, using the series Eq. (2) we evaluate the potential energy of a particle in the sheath field ($`z`$ in mm),

$$𝒰(z)M\omega _0^2\left(0.9z+\frac{1}{2}z^2\frac{1}{3}0.5z^3+\frac{1}{4}0.07z^4\right)\varphi (z).$$
(14)
We see that in our case at least the first anharmonic term results in a significant deviation of the sheath potential from a parabolic one, and therefore the oscillations become strongly nonlinear when the amplitude reaches a few tenths of mm, or more. At the same time the obtained coefficients of the series converge rapidly ($`\beta /\alpha 0.15`$ mm-1), so that for $`|z|2`$ mm we can limit ourselves to expansion (1). Thus, Eq. (14) provides convenient analytical expression for the electric field in rather wide vicinity of the equilibrium particle position.

Other experiments performed with different particle sizes and discharge conditions (Ar and Kr, $`p17`$ Pa) confirm that the sheath potential contains considerable anharmonic terms at low pressures. We have also investigated, how strongly the sheath potential is perturbed by the wire below the particle. Experiments with a wire at the same level with a particle (horizontal separation $`11`$ mm) show results, which are very similar to those reported here.

In this Letter, we have presented one example of nonlinear particle oscillations in the sheath of a low-pressure rf discharge and its quantitative analysis. The proposed simple method opens a possibility to retrieve the profile of the electric field in the whole pre-sheath and upper part of the sheath region, using particles of different masses (and thus levitating at different heights). Analysis for each particle allows us to reconstruct the electric field in a range of a few mm, and therefore it is sufficient to use just a few different particles to get rather precise field distribution in the whole sheath range. Hence, we believe that experiments with excitation of nonlinear oscillations might be an effective way to study the sheath distribution.


text:
# Influence of vortices on the magnetic resonance in cuprate superconductors

## Abstract

We investigate several theoretical possibilities for the suppression in a c-axis magnetic field of the magnetic resonance recently observed in inelastic neutron scattering experiments on YBa2Cu3O6.6. We find that neither the Doppler shift of the quasiparticle states caused by supercurrents outside the vortex core, nor an assumed spatially uniform suppression of the coherence factors or spectral gap due to the applied field, can account for the observed effect. In contrast, suppressing the gap or the coherence factors in the vortex core to zero is consistent with the data. We demonstrate that an even simpler description of the data can be achieved by assuming that the resonance is not supported within an effective radius $`\xi _{eff}`$ around each vortex, where $`\xi _{eff}`$ is the sum of the superconducting and spin-spin correlation lengths. We use this simple idea to predict the doping dependence of the field suppression.

One of the more intriguing developments in the field of high temperature cuprate superconductivity has been the observation by inelastic neutron scattering (INS) experiments of a sharp magnetic resonance in the superconducting state. Recently, it was found that a c-axis magnetic field suppressed the intensity of this resonance, as predicted from an analysis of specific heat data. Since the same effect was not observed for in-plane fields, this indicates that the resonance is sensitive to the presence of Abrikosov vortices, and thus intimately connected to the nature of the superconducting ground state. This has obvious implications for microscopic theories of the resonance.

In this paper, we consider a model where the resonance is treated as a particle-hole bound state in a $`d`$-wave superconductor, with calculations performed within linear response theory (RPA). Several effects of the vortices are considered. First, we calculate the influence of the supercurrents circulating around the vortices on the resonance. We find that this only leads to a broadening of the resonance in energy; the integrated weight remains the same, in conflict with experiment. Second, we study the effect of a spatially uniform suppression of the $`\mathrm{\Delta }_𝐤\mathrm{\Delta }_{𝐤+𝐐}`$ correlator which enters the coherence factors of the spin susceptibility (where $`𝐐`$ is the antiferromagnetic wave vector at which the resonance is peaked). Such a suppression is speculative, but could be a result of dephasing of the pairing in a c-axis field due to the vortices, as observed in Josephson plasma resonance experiments. We find that although this does lead to a suppression of the integrated weight as observed experimentally, the effect causes the resonance to shift to higher energy, in conflict with experiment. Third, an assumed (field induced) spatially uniform suppression of the gap magnitude causes the resonance to shift to lower energy, also in conflict with experiment.

This leads us to consider the effect of the vortex cores themselves. We observe that if the resonance is not supported in the vortex cores, then the resulting field dependence is in reasonable agreement with experiment. We consider three possibilities for the suppression of the resonance in the vortex core regions: (a) the suppression of the gap magnitude in the core, (b) the suppression of the $`\mathrm{\Delta }\mathrm{\Delta }`$ correlator in the core, and (c) the absence of quasiparticles in the core. Any of these three possibilities give a good account of the data. We use case (c) to estimate the doping dependence of the field suppression effect.

To calculate the influence of the supercurrents around the vortices on the resonance in the spin-spin correlation function, we approximate the superflow by a circular flow around the vortex center. The corresponding local supermomentum, $`𝐩_s`$, is proportional to the gradient of the phase, $`𝐩_s=\mathrm{}𝐞_\varphi /2r`$. This is a good approximation for the experiments considered here, where the intervortex spacing is smaller than the penetration depth and large compared to the coherence length.

In the intervortex regions, the variation of the order parameter and of the superflow occurs on a scale large compared to the spin-spin correlation length, which amounts to only a few lattice constants as determined from the momentum width of the resonance. Consequently, we determine the RPA susceptibility in the intervortex region at each point of the unit cell of the vortex lattice in the presence of the local superflow,

$$\chi (\omega ,𝐐,𝐩_s)=\frac{\chi _0(\omega ,𝐐,𝐩_s)}{1J_𝐐\chi _0(\omega ,𝐐,𝐩_s)}.$$
(1)
The bare susceptibility $`\chi _0(\omega ,𝐐,𝐩_s)`$, is determined as

$`\chi _0(\omega ,𝐐,𝐩_s)`$ $`=`$ $`{\displaystyle \underset{𝐤}{}}{\displaystyle \underset{\mu ,\nu =\{\pm \}}{}}{\displaystyle \frac{A_𝐤^\mu A_{𝐤+𝐐}^\nu +\alpha C_𝐤^\mu C_{𝐤+𝐐}^\nu }{\omega +E_𝐤^\mu E_{𝐤+𝐐}^\nu +i\mathrm{\Gamma }}}`$ (3)
$`\times \left(f(E_𝐤^\mu )f(E_{𝐤+𝐐}^\nu )\right)`$
where the excitation spectrum in the presence of a superflow with momentum $`𝐩_s`$ is given by

$`E_𝐤^\pm `$ $`=`$ $`\pm \sqrt{\overline{\xi }_𝐤^2+|\mathrm{\Delta }_𝐤|^2}+\delta \xi _𝐤`$ (4)
with $`\delta \xi _𝐤=(\xi _{𝐤+𝐩_s}\xi _{𝐤𝐩_s})/2`$, $`\overline{\xi }_𝐤=(\xi _{𝐤+𝐩_s}+\xi _{𝐤𝐩_s})/2`$, and

$`A_𝐤^\pm ={\displaystyle \frac{1}{2}}\pm {\displaystyle \frac{\overline{\xi }_𝐤}{E_𝐤^+E_𝐤^{}}}C_𝐤^\pm =\pm {\displaystyle \frac{\mathrm{\Delta }_𝐤}{E_𝐤^+E_𝐤^{}}}`$ (5)
as coherence factors. The factor $`\alpha `$ (1 in the current case) will be discussed later. The spatial average of the Doppler shifted susceptibility over the intervortex region of the vortex lattice unit cell is then calculated, $`\chi (\omega ,𝐐)=<\chi (\omega ,𝐐,𝐩_s(𝐑))>_𝐑`$. We evaluated Eq. (3) for a $`512\times 512`$ grid of $`𝐤`$-points and perfomed the spatial average over 320 $`𝐑`$-points. Note we use a normalization equal to the intervortex area, not the total area. The contribution from the vortex cores will be discussed later in the paper.

Calculations were performed using a model quasiparticle dispersion in the superconducting state motivated by photoemission measurements. Similar dispersions were found to give a good description of the zero field INS data, including the incommensurate structure observed at energies below resonance . A $`d`$-wave superconducting gap proportional to $`\mathrm{cos}(k_xa)\mathrm{cos}(k_ya)`$ was assumed, with a maximum value of $`\mathrm{\Delta }=`$ 29 meV as determined from recent STM measurements. A broadening factor, $`\mathrm{\Gamma }`$, of 2 meV was employed, and a temperature of 13 K.

In Fig. 1 we show our results for the effect of the circulating supercurrents on the resonance. The exchange coupling, $`J_𝐐`$, is fixed to give a resonance at 34 meV for zero magnetic field. For the spatial average we assumed a lower cut-off at the value $`\xi =2a`$ (vortex core radius) and an upper cut-off at the value $`R=25a`$ (radius for enclosing one flux quantum at 7 T), where $`a`$ is the Cu-Cu distance. The results are insensitive to the lower cutoff. As Fig. 1 shows, the supercurrent has three effects: (a) it shifts the position of the resonance to slightly lower energy, (b) it broadens the resonance, and (c) it reduces the magnitude of the resonance at the peak energy. Also shown are the energy integrated susceptibilities, which demonstrate that the integrated weight between 0 and $`2\mathrm{\Delta }`$ is conserved. These findings are in apparent contradiction with the experimental facts, which are that the resonance does not shift, nor broaden, and that the integrated weight is reduced by about 15% at 7 T \[Ref. \]. We have also tested a number of other dispersions , and a variety of assumed values for $`\mathrm{\Delta }`$ and $`J`$. Although the amount of broadening is somewhat sensitive to these details, we find that the integrated weight is always approximately conserved. An example is given in the right panel of Fig. 1, where we find virtually no effect of the Doppler shift on the susceptibility.

We also checked if an assumed field induced (spatially uniform) reduction of the gap magnitude accounts for the observed effect. Our result is shown as the dotted line in Fig. 2 compared to the zero field result (full line). The integrated weight is suppressed in this case (the left panel of Fig. 4 shows the reduction of the integrated weight versus $`\mathrm{\Delta }^2(H)/\mathrm{\Delta }^2(0)`$). To obtain the observed 15%

reduction in weight at 7 T would require reducing the gap from 29 to 20 meV. This reduction is substantially larger than would be indicated by the upper critical field (45 T), and the reduction appears to have the wrong functional dependence on $`H`$. Moreover, this gap reduction shifts the resonance to considerably lower energy, in contradiction with experiment.

As a third mechanism, we studied a (spatially uniform) suppression of the $`\mathrm{\Delta }_𝐤\mathrm{\Delta }_{𝐤+𝐐}`$ correlator in the $`C_𝐤C_{𝐤+𝐐}`$ coherence factors (by reducing $`\alpha `$ to less than 1 in Eq. 3). The motivation for this is that phase fluctuations induced by the vortices are known to lead to a dephasing of the layers, and the resonance will be sensitive to this since it involves c-axis coupling (it is peaked at $`k_z=\pi /d`$, where $`d`$ is the separation of nearest neighbor CuO layers). The observed decoupling inferred from the field dependence of the Josephson plasmon , though, is probably due to the weaker bilayer-bilayer coupling, which is also consistent with small mesa experiments . Therefore, at the current time, it is not known whether the two layers within a bilayer are dephased or not (though this could be determined from the field dependence of c-axis infrared conductivity measurements, where a feature is seen attributed to an optical Josephson plasmon ). For now, though, we will assume that this is a possibility, and test its consequences .

In Fig. 3, we compare the zero field result to the same result, but with the correlator reduced by 15% ($`\alpha =0.85`$). This leads to a large reduction of the integrated weight, as seen experimentally (in Fig. 4, we plot the integrated weight versus $`\alpha `$). We note that the

experimental suppression goes like $`1H/H^{}`$, where $`H^{}`$ is a number not much lower than $`H_{c2}`$, the upper critical field . Based on quantum Ginzburg-Landau theory, a reduction of the $`\mathrm{\Delta }\mathrm{\Delta }`$ correlator proportional to $`1H/H_{c2}`$ is expected. Therefore, it is reasonable to suppose that the relative experimental suppression goes like $`\alpha `$. This suppression is in good agreement with the calculation, as can be seen in Fig. 4. We note, however, that the position of the resonance shifts to higher energies, in disagreement with the data. It would be coincidental if this energy shift was exactly canceled by an assumed shift of the superconducting gap to lower energies by the field.

Let us now consider the effect of the vortex cores. The fact that the experimental suppression goes like $`1H/H^{}`$ is highly suggestive of a vortex core effect, as originally noted by Dai et al. . Therefore, we assume that the resonance is not supported in the region of the vortex core. This assumption is based on five facts: a) the considerable momentum width of the resonance shows that the corresponding spin excitations have a decay length of only two lattice constants, which is smaller than the coherence length; thus the resonance will be sensitive to variations of the order parameter on the coherence length scale; b) the resonance at zero field only exists in the superconducting state, and disappears in the normal state; c) coherence peaks in the single particle density of states at the gap edge were not found in the core region in STM measurements ; this would modify the $`2\mathrm{\Delta }`$-edge in $`\chi _0^{\prime \prime }`$ (Eq. 3) and suppress the resonance; d) in underdoped materials, missing subgap states point towards a loss of quasiparticle weight due to a pseudogap in the vortex core;  e) the dip feature in the tunneling density

of states, thought to be due to the coupling of quasiparticles to the resonance , is not observed in the vortex core region .

In Figs. 2 and 3, we show in the insets the susceptibility for zero $`\mathrm{\Delta }`$, and for zero $`\mathrm{\Delta }\mathrm{\Delta }`$ correlator. In both cases, the resonance is strongly suppressed. In the main panels, we show as dashed curves the results for the case when we use the curves in the insets for the vortex core regions, and the full curves (zero field results) for the intervortex regions. The latter is justified since we found above that the Doppler shift has a negligible effect on the integrated intensity. In both cases, the resulting curves, calculated for a 15% reduction in total integrated weight, reproduce very well the experimental finding of no shift or broadening of the resonance. One problem is that the observed weight suppression would require a vortex core region filling 24% of the total area for the first case, and 20% for the second case. Both values are somewhat larger than what one would expect at 7 T, as discussed below, especially for the first case.

There is a way of testing whether either of these two scenarios is correct. In the case where the gap is reduced in the cores, then extra weight would show up at lower energies, whereas for the case where the correlator is reduced in the cores, extra weight would show up at higher energies. Although our calculations indicate that the corresponding changes between 0 and 7 T are perhaps within experimental error bars, we encourage experimentalists to look for extra weight, both in the region around 20 meV and around 50 meV.

We note that our formalism assumes the presence of quasiparticle states, and thus we do not expect a resonance to exist if quasiparticles do not exist. A simpler idea to those discussed in the previous two paragraphs is to simply assume that the weight is zero in the considered energy range, consistent with a spin gap of $``$ 50 meV inside the cores. From this, we can estimate the effective radius of the core, $`\xi _{eff}`$, from the ratio of the INS weight to that at zero field. Since the ratio of the vortex core area to the total area is equal to $`B\pi \xi _{eff}^2/\mathrm{\Phi }_0`$, to obtain an effect of 15% at 7 T in underdoped YBa2Cu3O7-δ, we need a $`\xi _{eff}`$ of 37-38 Å. This is somewhat larger than the estimated coherence length of 27 Å ($`H_{c2}`$ of 45 T), but it should be noted that $`\xi _{eff}`$ should approximately be the sum of the superconducting and magnetic correlation lengths. The latter is approximately 10 Å (as measured by the momentum width of the resonance), so the two estimates are in agreement.

For optimally doped compounds, both coherence lengths are shorter. Assuming $`\xi _{eff}`$20-24 Å, our prediction for this case is that the suppression of the total weight at 7 T will only be 4-6%. Going further to the overdoped regime, the superconducting coherence length increases, leading to an increase of the sensitivity of the resonance with magnetic field again. Further underdoping, though, should lead to an even more dramatic reduction, as both coherence lengths are expected to increase as the doping is reduced. In fact, we would argue that the field dependence of the resonance at various dopings would be a good measure of the doping dependence of the superconducting coherence length, and it would be of great interest to correlate STM and INS measurements on the same samples.

We wish to conclude this paper with the following speculation, motivated by the above results. As documented by angle-resolved photoemission measurements , quasiparticle-like peaks in the spectral functions are present only below $`T_c`$, the onset temperature of phase coherence. The superconducting phase is singular at the vortex core, and therefore the phase correlations are strongly suppressed between points close to the core region (this was a motivation for the $`\alpha <1`$ calculations). We suggest that this may lead to a destruction of quasiparticle excitations in the vortex core region similar to what happens in the pseudogap state. The absence of quasiparticle peaks as well as the neutron resonance in the core region is consistent with the notion that both these spectral features require substantial local phase correlations. While this conjecture is at this stage admittedly speculative, we believe it deserves further experimental and theoretical investigation.

This work was supported by the U.S. Dept. of Energy, Office of Science, under Contract No. W-31-109-ENG-38.