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# From pseudomorphic to orthomorphic growth of Fe films on Cu3Au(001).

## Introduction

Very thin iron films, with physical properties at variance with the ordinary $`\alpha `$–Fe phase, can be grown on appropriately chosen substrates. Such ”artificial” phases represent an ideal ground in the investigation of the interplay between the structure and the magnetic properties of materials.  In this field, the Cu3Au(001) surface has been considered as a candidate for the stabilisation of a face–centered–cubic (fcc), expanded volume, high–spin Fe phase. For this substrate, a model of the so–called epitaxial lines of iron, calculated within the frame of linear elasticity theory, suggested the formation of a tetragonally strained phase, with some uncertainty on its body or face centered geometry. The calculations did not consider interdiffusion processes between the Fe deposit and surface atoms, but both intermixing at the interface and substrate segregation have been reported for Fe deposited at room temperature (RT) on Cu(001) and on Au(001).

In previous research on the magnetism of the Fe/Cu3Au(001) films, three regions of thickness of different properties were identified. At sub–monolayer coverage no hysteresis loops were detected. A second region was instead characterised by a magnetisation perpendicular to the surface. Then, at a critical thickness $`\mathrm{\Theta }_{sw}`$ of the order of a few monolayers and depending on the temperature of deposition, the magnetisation was found to switch to an in plane orientation ( spin reorientation transition, in brief SRO) as in ordinary $`\alpha `$–Fe.

In spite of an overall agreement on film magnetism, no general consensus has been reached about the film structure. Regarding room temperature (RT) growth, an early LEED study claimed the occurrence of a face–centered cubic phase up to 7 Mono–Layers (ML). In a more recent LEED I-V investigation the SRO transition ($`\mathrm{\Theta }_{sw}`$ $`4`$ ML) was tightly related to a transition from an fcc to a bcc–like phase; the LEED analysis was successively backed by an STM study in the coverage range of the SRO transition, pointing out a complex topography assigned to the coexistence of different phases. Another LEED I-V study, backed by dynamical calculations, proposed instead a body–centered–tetragonal (bct) structure down to $`\mathrm{\Theta }`$ = 3.3 ML with no apparent correlation between structural properties and the SRO transition.  In fact, the latter experiments must be carefully taken into consideration, since they were performed on substrates prepared by pre-depositing 2 ML of Fe at 150 K. For this temperature and thickness range, we have recently shown that the structure and morphology of of the growing film is driven by electronic mechanisms, whereas only strain and thermally activated processes drive the RT growth. Finally, in a recent electron scattering experiment (in the so–called Primary—beam Diffraction Modulated Electron Emission configuration, PDMEE)  an fcc–like structure was found for $`\mathrm{\Theta }`$ $`<`$ 4 ML; then in a region extending up to $``$ 23 ML, two different phases were detected. A unique phase of bct type was finally detected, at least within the outermost layers, for relatively thicker films, in agreement with results of Ref.. Ref. considered atomic exchange processes in some details, indicating the occurrence of a limited Au intermixing and segregation at the initial stages of growth.

The somewhat conflicting results demand for further investigation. Here we report on experiments of Fe/$`\mathrm{Cu}_3\mathrm{Au}(001)`$ RT growth performed at the ALOISA beamline at the Elettra Synchrotron (Trieste, Italy). Our investigation deals with a structural characterization of films in a thickness range of 3-36 Å, performed by means of X-ray induced photo– (and/or Auger–) electron Diffraction (from now on ED for brevity) in the so–called forward scattering condition. In this condition, the emission intensity is enhanced along the direction of interatomic axes by means of a focusing effect. The angular position of focusing peaks in polar ED scans is well known to provide ”simple”, chemically selected, short range information on the structure of the topmost layers of the films.  Furthermore, the availability of reliable calculations codes allows for a close comparison with experimental data and for quantitative analysis.

In our experimental approach,  ED data are backed by Grazing Incidence X-Rays Diffraction (GIXRD) measurements, supplying information about the in–plane lattice parameter of films  and about the film morphology. In the next section details on the experimental procedures are reported. Experimental data will be described in sect. II. A quantitative analysis of the data can be found in the sect. III. A discussion of the results obtained follows in sect. IV. A summary and the conclusions can be found in sect. V.

## I Experimental

The beamline ALOISA allows users to perform both electron spectroscopy and X-Ray surface diffraction measurements under the same experimental conditions. The sample is mounted on a 6–degrees–of–freedom manipulator, specially designed to select with great accuracy (0.01) the grazing angle of the beam electric field. The temperature of the sample, measured by thermocouples, can be varied by resistive heating and liquid nitrogen cooling. The UHV experimental chamber (base pressure in the 10-11 mBar range) hosts the hemispherical electron analysers and X-Ray detectors. The emission direction from the sample surface can be freely selected for any orientation of the surface. For the surface preparation, the sample is translated in the preparation chamber (base pressure of $`12\times 10^{10}`$ mBar) equipped with facilities for sputtering, evaporation cells, gas inlets and a RHEED system.

The surface preparation procedure was set up in previous He diffraction experiments. The procedure takes into account the particular thermodynamics of $`\mathrm{Cu}_3\mathrm{Au}(001)`$, that is characterized by a continuous order/disorder (O/D) phase transition at the surface with a critical temperature Tc = 663 K  and a bulk first order O/D transition at the same Tc. An ordered surface, displaying sharp $`c(2\times 2)`$ RHEED patterns typical of the Au-Cu termination, was obtained by sputtering and careful annealing procedures described in details elsewhere. The same sample was also used in a previous synchrotron experiment  and in the PDMEE experiment of Ref. .

At ALOISA, XPS surveys at grazing incidence (of the order of the critical angle) were used to check contamination of light adsorbates and Fe residuals after the sputtering removal of films. A preliminary ED characterization of the substrate, backed by multiple scattering calculations has been presented in a previous paper. Simulations taking into account the geometry for the Au-Cu termination available in literature  were found to be in excellent agreement with experimental results.

Iron was evaporated from a carefully outgassed electron bombardment cell (Omicron). A quartz microbalance allowed to tune the deposition flux (typically of the order of 1 layer per minute) prior to the deposition on the sample. The quartz microbalance was calibrated by X-ray reflectivity from the sample during and after deposition. Fig. 1 shows a typical deposition curve, measured at an incidence (tilt) angle $`\alpha _{in}`$ = 8.25 and a photon energy of 3500 eV during film deposition at room temperature. The interference between the waves reflected by the film-vacuum and the substrate-film interfaces yields an oscillatory evolution of the reflectivity as a function of the overlayer thickness. For the selected vertical momentum transfer $`k_z=2\frac{E}{\mathrm{}c}\mathrm{sin}\alpha _{in}`$, identical phase conditions occur after a thickness increase of $`\mathrm{\Delta }D=\frac{2\pi }{k_z}=12.35`$ Å, thus leading to an accurate calibration of the deposition rate.

The post growth GIXRD measurements consist of radial scans across the (200) and (220) peaks in the in–plane $`\mathrm{Cu}_3\mathrm{Au}(001)`$ reciprocal lattice. These measurements were taken scanning the photon energy in broad ranges under a suitable $`\theta `$-$`2\theta `$ scattering geometry. The observation of diffraction peaks in radial scans allows to determine the in-plane spacing $`d`$ through the Bragg condition $`2d\mathrm{sin}\theta =hc/E`$. Rocking curves of selected Bragg peaks, obtained by rotating the azimuthal angle at fixed energy, were measured to get additional information on the surface morphology.

A coverage estimate obtained by XPS measurements was found consistent with the reflectivity measurements within $`\pm 20\%`$. ED polar scans were measured by rotating the electron analyser in the plane defined by the surface normal and the beam axis, while keeping the grazing angle, the surface azimuthal orientation with respect to the beam axis and the polarization orientation fixed. We considered emission along the two main symmetry direction $`100`$sub and $`110`$sub of the substrate unit cell. The photon energy was set to about 900 eV in order to look at several photoelectron and Auger peaks of Fe, Cu and Au. Here we will focus on the Fe L2,3M23M45 line at a K. E. of 698 eV. The signal was collected at the maximum and at suitably chosen energies aside the peak, in order to allow an effective subtraction of the background of secondaries.

## II Results

### A GIXRD

Radial scans of the substrate diffraction peaks, taken on films of different thickness, are expected to show additional diffraction features arising from the Fe overlayers, if the film unit cell, although strained, is oriented parallel to the substrate, as reported in the literature. Upon deposition at room temperature, the first Fe-induced peak arises at a thickness of $``$ 8 $`\AA `$. The radial scans across the (200) and (220) substrate peaks are shown in Fig. 2 as a function of the substrate reciprocal lattice unit. The peaks labelled $`\gamma `$ mark the appearance of a new structure, i.e. the overcome of the limit for pseudomorphic growth. The corresponding lattices for the antiferromagnetic and ferromagnetic fcc Fe are also shown for comparison, as well as the lattice of a bcc(100) unit cell rotated by 45. Azimuthal scans taken on the $`\gamma `$ peaks (not shown) indicate this Fe phase to be oriented parallel to the substrate lattice.

The evolution of the Fe film structure as the thickness increases is shown in Fig. 3, where radial scans across the (200) substrate peak are shown from 3 up to 36 $`\AA `$. The peak $`\gamma `$ becomes more intense in the 10-17 Å range. A shoulder appears at the left hand side of peak $`\gamma `$ at $`\mathrm{\Theta }`$ 17 Å. For $`\mathrm{\Theta }`$ 25 Å this shoulder develops in the well defined peak $`\alpha `$, that gradually moves away from the (200) reflection.

The position $`1.93\pm 0.005`$ r.l.u. of the $`\gamma `$ peak in the 10 Å pattern of fig. 3, is the same of Fig. 2 at 8 Å and corresponds to a distance d100 =$`1.94\pm 0.01`$ Å along the $`001`$ direction of direct space, eventually leading to a square cell of side $`a_\alpha ^{}`$ =$`d\sqrt{2}`$ = 2.74 $`\pm `$ 0.01 Å. The position of the $`\alpha `$ peak at 36 Å thickness in Fig. 3 corresponds to a lattice parameter $`a_\alpha `$ = 2.830 $`\pm `$ 0.005 Å. The position of $`\alpha `$ is indeed close to the (220) reflection of a R45bcc structure. Further, reasonable arguments on the energetics of iron modifications and inspection of the so–called epitaxial lines calculated in Ref.  led us to consider the $`\alpha `$ peak incompatible with an fcc-like modification (fct phase). The $`\alpha `$ peaks were therefore assigned to tetragonally strained body centered ( R45bct ) structures.

The GIXRD measurements provided therefore valuable insight on the in–plane structure of the films; this information is relatively direct for those patterns presenting one dominant Fe–induced peak, as it is the case at very low ($``$ 8 Å) and very large coverages (36 Å). In an intermediate region between 10 and 20 Å, the patterns are more complex, likely reflecting the coexistence of more than one phase in the film. A full structural determination requires also the value of the vertical lattice constant of the various iron phases which forms at different thickness. We extracted this information by ED, in the forward focusing regime.

### B ED

ED polar scan measured on films of selected thickness for the Fe Auger line along the $`100_{sub}`$ and $`110_{sub}`$ directions, are reported in Figs. 4 and 5, respectively. The Fe films are the same of Fig. 3 at the corresponding thickness. The patterns were obtained after subtraction of the background of secondaries. The peak F is originated by the forward scattering effect along off–normal nearest–neighbour chains. The position of this peak provides a guess on the ratio between the in–plane and vertical lattice constants of the film. In this respect, the full vertical lines in Figs. 4 and 5 mark the position of the F peak expected in case of fcc and R45bcc geometry, respectively.

At the lowest coverage investigated ( patterns $`a`$ of Figs. 4 and 5), the forward focusing peak F is fairly pronounced in the $`100_{sub}`$ scan close to the fcc–like position . The F peak lays close to the fcc marker in the $`110_{sub}`$ direction as well, though its intensity is very weak. Note in both patterns the presence of the forward focusing peak N, related to close–packed chains along the surface normal. At 10 Å (pattern $`b`$ of Figs. 4 and 5) the F peaks move slightly from the fcc markers towards larger polar angles. The angular shift of the F peaks becomes more evident at $`\mathrm{\Theta }`$ = 20 Å (patterns $`c`$). Also the shape of the patterns shows evident variations with respect to lower coverages. In the spectra obtained on the film at $`\mathrm{\Theta }`$ = 36 Å (patterns $`d`$), the F peak becomes narrower and shifts towards the $`bcc`$ position.

We performed also ED measurements for the Auger lines of Cu and for the Au 4f7/2 photoemission line. The experimental data resulted in overall agreement with results of Ref. , obtained on the same sample and under similar experimental conditions of this paper. We address the reader to Ref.  for a careful discussion of the intermixing between iron and substrate species.

## III ED Data Analysis

In this section we present the structural models for the Fe film at different thickness, as obtained by comparison of the ED experimental data to multiple scattering calculations. In our computational approach the ED polar pattern $`I_{exp}(\theta )`$ is considered as a superposition of two contributions, according to the expression:

$$I_{exp}(\theta )=ISO_{exp}(\theta )(1+\chi _{exp}(\theta ))$$
(1)
where $`ISO_{exp}(\theta )`$ is a smooth, nearly isotropic background and the anisotropy term $`\chi _{exp(\theta )}`$ is the diffractive part of the pattern, carrying the information on the interatomic distances.

The $`ISO_{exp}`$ contribution is commonly obtained by interpolating $`I_{exp}(\theta )`$ to a polinomial and divided out in order to extract $`\chi _{exp}`$, which is then compared to calculated $`\chi _{calc(\theta )}`$. We have preferred to afford a calculation of the ISO term. Thus, the polar scans $`I_{exp}(\theta )`$ have been compared with calculations:

$$I_{calc}(\theta )=ISO_{calc}(\theta )(1+\chi _{calc}(\theta ))$$
(2)
For any given model the anisotropy term $`\chi _{calc}`$ has been calculated by means of the MSCD code package , while the ISO term has been written as the product of several factors. First, an emission factor accounts for the electron emission matrix element; it is determined by the polarization of the beam and by the initial and final states of the emitted electron. A second factor bears the information on the excited electron escape path through the Fe film; it depends on the thickness and the homogeneity of the film. A third factor accounts for the surface roughness. Finally, an instrumental factor accounts for the beam spot size on the sample and the angular acceptance of the detector. The calculation of the ISO part requires therefore reasonable estimates on the thickness and the surface roughness of the film and on the electronic mean free path.

Concerning MSCD calculations, the non structural input parameters, i.e. Multiple Scattering order = 6 and the inner potential = 10 eV have been fixed for all the simulations. Clusters of at least 180 atoms have been considered. The isotropic emission for the Auger electrons has been simulated by the transition from an initial p–level to an s (l-1) final–state level.

The value of the lattice parameter of the in–plane square cell $`a`$ has been obtained from the GIXRD measurement, while the ratio between the vertical spacing $`c`$ and $`a`$ , was first estimated by visual inspection of the angular position of the F peaks in the ED patterns. With these input parameters, the structural models have been refined by calculating $`\chi _{calc(\theta )}`$ as a function of $`a`$ and $`c`$.

### A Low Coverage: $`\mathrm{\Theta }<8`$ Å

The patterns of Figs. 4 and 5 force us to consider an fcc–like structure. Although results from Ref.  suggested a limited degree of mixing of Au in the first few layers, a reasonable fitting of the data was possible disregarding atomic exchange processes. The comparison between MSCD calculations and the experimental ED scans is reported in Figs. 4,5 (curves labelled $`a`$). Note that the same $`ISO_{calc}(\theta )`$ is used in both azimuthal directions.

The polar scans compare rather well with a simple three-layer Fe pseudomorphic fcc film ( $`a`$= 2.65 Å; $`c/a`$ = 1.41) built on an unrelaxed substrate extending three layers beneath. However, a slightly better agreement ) was found by admitting a slight tetragonal distortion with $`a_p`$ = 2.65 Å and $`c/a_p=`$ 1.38. The quality of the fit is observed to be slightly worst along the $`110_{sub}`$ direction. In fact, the ED polar scans are certainly affected by the film morphology (such as preferred step orientation), but we cannot exclude a structural origin related to a very slight zig-zag of the surface atom chains, which would smear the forward focussing features. In fact, a strong buckling was reported for the Fe on Cu(001) system, where this distortion is predicted to be precursor of the fcc(100) to bcc(110) martensitic transition,  however the latter transition is not observed on the present system.

### B Medium Coverage: 8 Å $`\mathrm{\Theta }`$ 20 Å

The $`\gamma `$ peak in the GIXRD patterns at $`\mathrm{\Theta }8`$ Å indicates a change of the growth mode. We first calculated the simulation for a homogeneous iron phase made of six complete layers, assuming the $`c/a`$ ratio of 1.32 estimated by simple inspection of the angular position of the maximum of the F peak in the polar pattern. This model yields a simulation of the ED data (not shown) definitely not adequate. GIXRD and ED evidences can be rationalized if the coexistence of the two phases is assumed: the majority fcc–like phase, as seen at low coverage, is accompanied by the nucleation of a new phase $`\gamma `$, minority phase at this stage.

The ED patterns for the 10 Å Fe film thickness (curve $`b`$ in Figs.4,5) have been compared to calculations performed on a crude model assuming the linear combination of two ”independent” phases:

$$I_{th}=AI_p+BI_\gamma ,$$
(3)
where

I$`{}_{p}{}^{}a_p`$ = 2.65 Å and $`c/a_p1.38`$

I$`{}_{\gamma }{}^{}a_\gamma `$ = 2.74 Å ( from GIXRD) and $`c/a_\gamma `$ to be determined.

$`c/a_\gamma ,`$ $`A`$ and $`B`$ were varied in order to find the best agreement with experimental data. Taking into account the estimated thickness of the film, we have modelled a film of about 5-6 layers. A good agreement was obtained with $`c/a_\gamma =1.22`$, $`A`$ = 0.6 and $`B`$ = 0.4 for both azimuthal directions (full line in polar scan $`b`$ of Figs. 4,5).

For comparison, we also calculated the simulation for a homogeneous iron phase made of six complete layers, assuming the $`c/a`$ ratio of 1.32 estimated by simple inspection of the angular position of the maximum of the F peak in the polar pattern. This model yields a simulation of the ED data (not shown) definitely worse than the mixed phases model.

At 20 Å the F peaks are clearly shifted, indicating a change of the $`c/a`$ ratio. Backed by GIXRD, a model considering the superposition of three phases was attempted:

$$I_{th}=AI_p+BI_\gamma +CI_\alpha $$
(4)
For simplicity, the parameters for the pseudomorphic and the $`\gamma `$ phases were fixed at the same values found at lower coverage:

I$`{}_{p}{}^{}a_p`$=2.65 Å, $`c/a_p`$ 1.38

I$`{}_{\gamma }{}^{}a_\gamma `$ = 2.74 Å, $`c/a_\gamma `$ = 1.22.

By taking A = 0.4, B = 0.4 and C = 0.2, a rather satisfactory agreement was found (curves labelled $`c`$ in Figs. 4,5) with the following set of parameters for the $`\alpha `$ phase,

I$`{}_{\alpha }{}^{}a_\alpha `$ = 2.80 Å, $`c/a_\alpha =1.05`$.

We note that a reasonable agreement was found also with a linear combination of the pseudomorphic phase ($`a_p`$=2.65 Å, $`c/a_p1.38`$) and the $`\gamma `$ phase ($`a_\gamma `$= 2.74 Å, $`c/a_\gamma =1.22`$) found at 10 Å. However, in this case, we have found rather different values of the $`A`$ and $`B`$ coefficients along the two azimuthal directions considered. Finally, the simulation for a homogeneous phase model assuming $`c/a=1.25`$, corresponding to the angular position of the F peak in the polar scan, gave a bad quality fit.

### C  High Coverage: $`\mathrm{\Theta }>`$ 25 Å

The in–plane lattice parameter of the $`\alpha `$ phase at 36 Å determined by GIXRD is $`a_\alpha =2.830\pm 0.005`$ Å. The value of $`c/a_\alpha `$ was determined by simulation of scattering from a free standing film consisting of a unique phase of 10 layers. The best fit yielded $`a_\alpha =2.83`$ Å and $`c/a_\alpha =1.03\pm 0.02`$. The best fit curves along $`100_{sub}`$ and $`110_{sub}`$ are reported in Figs. 4,5 (curves labelled $`d`$). We found an excellent agreeement along the $`100_{sub}`$ direction. The simulation reproduces rather accurately the angular position, intensity and width of the N and F peaks. The experimental data are not reproduced equally well along the $`110_{sub}`$ direction, possibly due to some morphological effect. A similar analysis, performed on the film of 30 Å thickness provided $`a_\alpha =2.810\pm 0.005`$ Å and $`c/a_\alpha =1.05\pm 0.02`$.

## IV Discussion

In Fig. 6, we report the comparison of our results and the other experimental data available in literature with the theoretical prediction for the structure of the bct and fct phases, the so called epitaxial curves (i.e. the curves where the Poisson ratio between the elastic constants for the given structure is conserved).

The single phase we found at the lower coverage represents the pseudomorphic phase predicted at initial stages of metal-on-metal epitaxy. The occurrence of a pseudomorphic phase at low coverage is also reported by other measurements on Cu3Au(001)  and Cu90Au10(001). As can be seen, this phase lies above the FM fcc epitaxial line and is locked by the substrate for a few layers before the appearance of the $`\gamma `$-phase at $`8`$ Å (for the pseudomorphic phase this thickness corresponds to 4.5 ML), which indicates that the limit for pseudomorphic growth has been overcome (in Fig. 6, we have reported the point at 10 Å for which the vertical spacing has been also determined by the ED analysis). These data are therefore consistent with the limit of 4 ML found in a recent experiment  and with the values obtained in earlier studies on this system .

A relevant exception to such general agreement on initial stages of growth, is provided by the accurate analysis of Wuttig and coworkers. As can be seen in Fig. 6, the films were found to lie on the bcc epitaxial line already at the coverage of 3.3 ML (i.e. $``$ 5 Å, according to the data in table I of Ref. ). This discrepancy could be possibly attributed to the different procedure for film deposition, since the authors of Ref.  deposited the first two monolayers at 150 K, while subsequent layers were deposited at 300 K. This procedure is expected to reduce both intermixing and surface segregation. In fact, a fraction of the order of 10% of a monolayer of Au atoms has been found to segregate for $`\mathrm{\Theta }`$ $`<`$ 4 ML upon deposition at RT and a few percents has been found within the Fe film. We may speculate that Au and Cu impurities are concurrent in the stabilization of the pseudomorphic phase. It is worth noting that a bcc-like structure has been recently suggested for 2-4 ML Fe films on Cu(001), where segregation is certainly much lower .

The morphology of the growing film is also affected by the deposition procedure. In fact, we previously found by He atom scattering that deposition of 1 layer equivalent at 150 K and subsequent annealing at 400 K yields the formation of an homogeneous pattern of three-layer height islands, whereas a much higher filling of the first layer (68 %) is obtained upon deposition of 1 ML at RT.

Whatever the effect of temperature on segregation, structure and morphology, our measurements do not support a direct relation between the SRO transition and the fct to bct one. In fact, the latter phase only appears at a thickness of 17 Å, i.e. well beyond the 2.5-3.5 ML range claimed in the literature for the SRO transition. On the basis of the present data, we cannot exclude a connection between the transition from the pseudomorphic phase to the fct $`\gamma `$-phase and the SRO transition.

The film evolution in the 10-20 Å coverage range is the most interesting one since up to three different phases are seen to co-exist. The $`\gamma `$ phase is seen to fall on the epitaxial line for FM fcc Fe. Its lattice parameter at 8-10 Å, $`a_\gamma =2.74\pm 0.01`$ Å, seems to be the maximum allowed strain for this fct phase; in fact, when the third phase $`\alpha `$ appears at higher coverage, $`a_\gamma `$ rather shrinks (see Fig. 3). This suggests that the appearance of the $`\alpha `$ phase partially relieves the strain of the fct film. The $`\alpha `$ phase, when appearing at 17 Å, has already a lateral lattice spacing of 2.80 Å, which, together with the vertical spacing determined by MSCD analysis, brings the new phase directly on the bcc epitaxial line. No diffraction features are observed for lateral lattice spacings ranging from 2.74 Å up to 2.80 Å. Upon further deposition, the ”asymptotic” orthomorphic $`\alpha `$ phase evolves along the bcc epitaxial line. The structure of this phase is seen to be fully consistent with previous data reported in the literature for thick films. From our data, the transition path between the fct and bct structure can be traced at the value of maximum tensile strain $`a_\gamma =2.74`$ of the $`\gamma `$ phase. The observation of a bct phase with the same lateral lattice constant was not possible, in fact the appearance of the $`\alpha `$ phase is accompanied by a partial relief of strain as witnessed by the slight decrease of $`a_\gamma `$, which corresponds to a volume decrease of the $`\gamma `$ unit cell towards the predicted Fe fcc equilibrium point. On the other hand, the limit value for the bct stability was appearently reached by the group of Wuttig. By following a different preparation procedure, they stabilized the bct phase down to four monolayers, with a corresponding lateral lattice constant in excellent agreement with the 2.74 Å value, we found for the limit of stability of the fct phase (see Fig. 6).

It is interesting to compare this system with the Fe/Cu(100) one. In the latter case, Fe is also seen to grow with an fcc pseudomorphic structure for at least 4 ML, at higher coverage the magnetic properties change and the formation of buffer layers with anti-ferromagnetic fcc structure is proposed. An fcc(100) to bcc(110) transition takes place at about 10 ML, (which is also accompanied by an SRO transition) but, in this case, the whole film is observed to deconstruct, i.e. a martensitic phase transition takes place. This is not observed for Fe on Cu3Au(001), where the $`\gamma `$ phase is still detectable at a thickness of 20 Å. In any case the formation of the bct phase is accompanied by a significant amount of surface roughness, possibly leading to the exposure of the layers closer to the Fe/substrate interface (which are still probed by ED at 20 Å, see section III.B). This is consistent with a quantitative evaluation of the bct domain size obtained by the width of the diffracted $`\alpha `$ peaks. The profiles of the R45 bct (110) and R45bct (100) peaks, obtained with an azimuthal scan at fixed photon energy (not shown), yielded a mean domain size of $``$ 150 Å for the 36 Å film thickness. This high level of morphological disorder is consistent with the experimental findings for homoepitaxial deposition of Fe on Fe(001) at RT, where, in absence of surfactant species, the growth is seen to proceed in a three-dimensional fashion, resulting in the formation of pyramidal mound-like structures.

## V Conclusions

We have presented a combined GIXRD-ED study of the growth of thin films of Fe on Cu3Au(001). We observed the formation of different phases as a function of the film thickness. The main conclusions of this investigation can be summarized as follows:

i. A single pseudomorphic phase of nearly fcc character was observed below 8 Å thickness. This conclusion is consistent with most of the previous works in the literature whereas it seems in apparent contrast with the analysis of Ref.  that reports a bct phase down to $`5`$ Å. In this respect, we suggested that exchange processes at the interface  may concur to the stabilization of the pseudomorphic phase and we speculate that the different results of Ref.  are due to a lower influence of intermixing obtained during the deposition of the first two layers at 150 K.

ii. On a 8 Å Fe thickness film, a neat Fe induced peak, clearly illustrating the overcoming of the thickness limit for pseudomorphic growth, has been observed from the in–plane GIXRD measurements. Above this limit the film is characterized by the coexistence of phases: the pseudomorphic phase, most likely in inner layers, and a second strained phase $`\gamma `$. The latter phase is seen to lie on the ferromagnetic fcc epitaxial line.

iii. At $`\theta `$ 17 Å, we clearly observed the nucleation of a third strained phase, $`\alpha `$, which becomes the dominating structure at $`\theta `$ 25 Å. The $`\alpha `$ phase is characterized by a body centered, tetragonally strained structure, whose unit cell is rotated of 45 with respect to the fcc substrate. The strain is progressively relieved with the increasing film thickness, in close agreement with the results of Ref. . The experimentally determined lattice constants of $`\alpha `$ are in strict quantitative agreement with the epitaxial curves for bcc Fe.

## Acknowledgements

Maurizio Canepa, Silvana Terreni and Lorenzo Mattera are very grateful to Fernando Tommasini for his continuous support to this experiment. The authors are then grateful to P. Cantini, G. Boato, S. Valeri and A. Di Bona for stimulating discussions on the Fe/Cu3Au system. The authors thank G. Gazzadi for discussions on the MSCD calculations and C. Mannori and S. Prandi for helpful assistance at various stages of the experiment.

Funding from INFM and from the Italian Ministero dell’Università e Ricerca Scientifica ( Cofin 990211848) are gratefully acknowledged.


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# Comment on Neutrino Masses and Oscillations in an 𝑆𝑈(3)_𝐿×𝑈(1)_𝑁 Model with Radiative Mechanism

## Abstract

We discussed how neutrino masses and oscillations are radiatively generated in an $`SU(3)_L`$ $`\times `$ $`U(1)_N`$ gauge model with a symmetry based on $`L_eL_\mu L_\tau `$ ($``$$`L^{}`$). The model is characterized by lepton triplets $`\psi ^i=(\nu ^i,\mathrm{}^i,E^i)`$, where $`E^i`$ are negatively charged heavy leptons, an $`SU(3)_L`$ triplet Higgs scalar $`\xi `$ and a singlet Higgs scalar $`k^{++}`$. These Higgs scalars can be interpreted as a Zee’s and Zee-Babu’s scalar for radiative mechanisms. We demonstrated that the mass hierarchy of $`\mathrm{\Delta }m_{atm}^2`$ $``$ $`\mathrm{\Delta }m_{}^2`$ arise as a consequence of the dynamical hierarchy between $`L^{}`$-conserving one-loop effects and $`L^{}`$-violating two-loop effects, and our model is relevant to yield quasivacuum solution for solar neutrino problem.

There is definitive evidence for neutrino oscillations from atmospheric and solar neutrino observations. For the atmospheric neutrino oscillations, the recent SuperKamiokande (SK) data indicates that the observed deficit of $`\nu _\mu `$ is due to the $`\nu _\mu `$ $``$ $`\nu _\tau `$ oscillation , while for the solar neutrino oscillations , the SK, Homestake , SAGE , GALLEX  and GNO  data indicate the $`\nu _e`$ $``$ $`\nu _\mu ,\nu _\tau `$ oscillation. The existence of these neutrino oscillations implies the neutrinos are massive particles . The mass squared differences for atmospheric oscillations $`\mathrm{\Delta }m_{atm}^2`$ is measured as $`\mathrm{\Delta }m_{atm}^2`$ $``$ $`3\times 10^3`$ eV2 . On the other hand, there are some solutions to explain the observed solar neutrino oscillation data as (1) $`\mathrm{\Delta }m_{}^2`$ $``$ $`10^5`$ eV2 for the LMA solution, (2) $`\mathrm{\Delta }m_{}^2`$ $``$ $`10^6`$ eV2 for the SMA solution, (3) $`\mathrm{\Delta }m_{}^2`$ $``$ $`10^7`$ eV2 for the LOW solution, (4) $`\mathrm{\Delta }m_{}^2`$ $``$ $`10^{10}`$ eV2 for the VO solution and recently proposed (5) $`\mathrm{\Delta }m_{}^2`$ $``$ $`10^9`$ eV2 for the quasi-VO (QVO) solution . To sum up, we have $`\mathrm{\Delta }m_{atm}^2`$ $``$ $`10^3`$ eV2 and $`\mathrm{\Delta }m_{}^2`$ $`\stackrel{<}{}`$ $`10^5`$ eV2 indicating the hierarchy of $`\mathrm{\Delta }m_{atm}^2`$ $``$ $`\mathrm{\Delta }m_{}^2`$ exist. In the theoretical view, this mass hierarchy suggests that the neutrino mass matrix has bimaximal structure .

Recently, radiative mechanisms to generate tiny neutrino masses and oscillations in $`SU(3)_L`$ $`\times `$ $`U(1)_N`$ gauge models  with the $`L^{}`$ symmetry have been extensively studied . Here $`L^{}`$ $``$ $`L_eL_\mu L_\tau `$ is a new lepton number and the conservation of this quantum number is one of the possibilities of the origin of the bimaximal structure . Three $`SU(3)_L`$ $`\times `$ $`U(1)_N`$ gauge models are used to accomodate such radiative mechanisms. Each of the $`SU(3)_L`$ $`\times `$ $`U(1)_N`$ models can be distinguished by the lepton triplets $`\psi ^i`$ ($`i=1,2,3`$) in the models: (a) $`\psi ^i`$ = $`(\nu ^i,\mathrm{}^i,\omega ^{0i})`$ model , (b) $`\psi ^i`$ = $`(\nu ^i,\mathrm{}^i,\kappa ^{+i})`$ model The model with $`\psi ^i`$ = $`(\nu ^i.\mathrm{}^i,\mathrm{}^{+i})`$ has been lately examined to yield tiny neutrino masses and observed neutrino oscillations .  and (c) $`\psi ^i`$ = $`(\nu ^i,\mathrm{}^i,E^i)`$ model , where $`\omega ^{0i}`$, $`\kappa ^{+i}`$ and $`E^i`$ are denoted by electrically neutral heavy leptons, positively charged heavy leptons and negatively charged heavy leptons, respectively. In the model (a) and the model (b), the atmospheric neutrino oscillations are generated by a one-loop radiative mechanism with $`L^{}`$-conserving interactions , and the solar neutrino oscillations are induced from a two-loop rediative mechanism with $`L^{}`$-violating interactions . Consequently, the mass hierarchy of $`\mathrm{\Delta }m_{atm}^2`$ $``$ $`\mathrm{\Delta }m_{}^2`$ is explained as a result of the smallness of the two-loop effects compared with one-loop effects . On the other hand, in the model (c), there is no one-loop interaction and both of the atmospheric and solar neutrino oscillations come from two-loop radiative effects . The mass hierarchy of $`\mathrm{\Delta }m_{atm}^2`$ $``$ $`\mathrm{\Delta }m_{}^2`$ is related to the dynamical hierarchy of the $`L^{}`$-conserving and $`L^{}`$-violating two-loop interaction effects.

In this article, we show that it is possible to construct the other $`SU(3)_L\times U(1)_N`$ model with lepton triplets $`\psi ^i`$ = $`(\nu ^i,\mathrm{}^i,E^i)`$ . The model has similar particle content to the model (c); however, one-loop interactions also exist and neutrino masses are induced by the $`L^{}`$-conserving one-loop radiative mechanism as well as the $`L^{}`$-violating two-loop radiative mechanism.

The particle content in our $`SU(3)_L\times U(1)_N`$ gauge model is summarized as follows:

$`\psi _L^{i=1,2,3}=(\nu ^i,\mathrm{}^i,E^i)_L^T:(\text{3},2/3),\mathrm{}_R^{1,2,3}:(\text{1},1),E_R^{1,2,3}:(\text{1},1),`$ (1)
in the lepton sector, where we have denoted $`E^i`$ by $`E^i`$,

$`Q_L^1=(u^1,d^1,d^1)_L^T:(\text{3},0),Q_L^{i=2,3}=(d^i,u^i,u^i)_L^T:(\text{3}^{},1/3),`$ (2)
$`u_R^{1,2,3}:(\text{1},2/3),d_R^{1,2,3}:(\text{1},1/3),u_R^{2,3}:(\text{1},2/3),d_R^1:(\text{1},1/3),`$ (3)
in the quark sector, and

$`\eta =(\eta ^0,\eta ^{},\overline{\eta }^{})^T:(\text{3},2/3),\rho =(\rho ^+,\rho ^0,\overline{\rho }^0)^T:(\text{3},1/3),`$ (4)
$`\chi =(\chi ^+,\overline{\chi }^0,\chi ^0)^T:(\text{3},1/3),\xi =(\xi ^{++},\overline{\xi }^+,\xi ^+)^T:(\text{3},4/3),`$ (5)
$`k^{++}:(\text{1},2),`$ (6)
in the Higgs sector, where the quantum numbers are specified in the parentheses by $`(SU(3)_L,U(1)_N)`$. Let $`N/2`$ be the $`U(1)_N`$ quantum number, then the hypercharge ($`Y`$) and electric charge ($`Q_e`$) are given by $`Y=\lambda ^8/\sqrt{3}+N`$ and $`Q_e=(\lambda ^3+Y)/2`$, respectively, where $`\lambda ^a`$ is the $`SU(3)`$ generator with Tr($`\lambda ^a\lambda ^b`$) = $`2\delta ^{ab}`$ ($`a,b`$ = $`1,\mathrm{},8`$). Three Higgs triplets $`\eta ,\rho `$ and $`\chi `$ are the minimal set to generate masses of quarks and leptons in $`SU(3)`$ $`\times `$ $`U(1)_N`$ models. An additional Higgs triplet $`\xi `$ is introduced as a triplet version of the Zee scalar to realize the one-loop radiative mechanism  and an additional Higgs singlet $`k^{++}`$ is introduced to realize the two-loop radiative mechanism .

Here, we introduce two constraints to obtain the relevant Yukawa interactions. The first is the $`L^{}`$ $``$ $`L_eL_\mu L_\tau `$ conservation imposed on our interactions to reproduce the observed atmospheric neutrino oscillations as mentioned. The $`L^{}`$ assignment is shown in Table I. The second is the discrete symmetry based on $`Z_4`$ to suppress unwanted flavor-changing-neutral-currents (FCNC) interactions in the quark sector and the lepton sector. In the quark sector, there are quarks with the same charge, thus, quark mass terms can be generated by $`\rho `$ and $`\chi `$ between $`Q_L^1`$ and down-type quarks and by $`\rho ^{}`$ and $`\chi ^{}`$ between $`Q_L^{2,3}`$ and up-type quarks. FCNC is induced from these interactions . Also, in the lepton sector, $`\mathrm{}^i`$ and $`E^i`$ ($`i=1,2,3`$) has the same chage and the similar FCNC problem can occur. To avoid such interactions, Yukawa interactions must be constrained such that a quark (lepton) flavor gains a mass from only one Higgs scalar . These situations can be realized by introducing the following $`Z_4`$ symmetry into the model: $`\psi _L^{1,2,3}i\psi _L^{1,2,3}`$, $`\mathrm{}_R^{1,2,3}\mathrm{}_R^{1,2,3}`$, $`E_R^{1,2,3}iE_R^{1,2,3}`$, $`Q_L^1iQ_L^1`$, $`Q_L^{2,3}iQ_L^{2,3}`$, $`u_R^{1,2,3}u_R^{1,2,3}`$, $`d_R^{1,2,3}d_R^{1,2,3}`$, $`u_R^{2,3}iu_R^{2,3}`$, $`d_R^1id_R^1`$, $`\eta i\eta `$, $`\rho i\rho `$, $`\chi \chi `$, $`\xi \xi `$, and $`k^{++}ik^{++}`$.

With these constraints, the Yukawa interactions are given by

$`_Y`$ $`=`$ $`ϵ^{\alpha \beta \gamma }{\displaystyle \underset{i=2,3}{}}f_{[1i]}\overline{\left(\psi _{\alpha L}^1\right)^c}\psi _{\beta L}^i\xi _\gamma +{\displaystyle \underset{i=1,2,3}{}}\overline{\psi _L^i}\left(f_{\mathrm{}}^i\rho \mathrm{}_R^i+f_E^i\chi E_R^i\right)`$ (9)
$`+{\displaystyle \underset{i,j=2,3}{}}f_k^{ij}\overline{(\mathrm{}_R^i)^c}E_R^jk^{++}+\overline{Q_L^1}\left(\eta U_R^1+\rho D_R^1+\chi D_R^1\right)`$
$`+{\displaystyle \underset{i=2,3}{}}\overline{Q_L^i}(\eta ^{}D_R^i+\rho ^{}U_R^i+\chi ^{}U_R^i)+(h.c.),`$
where $`f`$’s are Yukawa couplings with the relation $`f_{[ij]}=f_{[ji]}`$ demanded by the Fermi statics, and right-handed quarks are denoted by $`U_R^i=_{j=1}^3f_{uj}^iu_R^j`$, $`D_R^i=_{j=1}^3f_{dj}^id_R^j`$, $`U_R^i=f_{u^{}2,3}^iu_R^{2,3}`$ and $`D_R^1=f_{d^{}1}^1d_R^1`$. For simplicity, we have assumed diagonal mass terms for the leptons. Note that there is no term which can induce FCNC interactions such as $`\overline{Q_L^1}\chi D_R^1`$, $`\overline{Q_L^1}\rho D_R^1`$, $`\overline{Q_L^{2,3}}\chi ^{}U_R^{2,3}`$, $`\overline{Q_L^{2,3}}\rho ^{}U_R^{2,3}`$, $`\overline{\psi _L^i}\chi \mathrm{}_R^i`$ and $`\overline{\psi _L^i}\rho E_R^i`$.

The Higgs interactions are given by self-Hermitian terms of $`\varphi _\alpha \varphi _\beta ^{}`$ ($`\varphi `$ = $`\rho `$, $`\eta `$, $`\chi `$, $`\xi `$, $`k^{++}`$), and two types of non-self-Hermitian Higgs potentials:

$`V_0`$ $`=`$ $`\lambda _0ϵ^{\alpha \beta \gamma }\eta _\alpha \rho _\beta \chi _\gamma +\lambda _1(\eta ^{}\rho )(\xi ^{}\chi )+\lambda _2(\eta ^{}\chi )(\xi ^{}\rho )+(h.c.),`$ (10)
$`V_b`$ $`=`$ $`\mu _b\xi ^{}\eta k^{++}+(h.c.),`$ (11)
where $`\lambda _{0,1,2}`$ stands for $`L^{}`$-conserving coupling constants and $`\mu _b`$ denotes the $`L^{}`$-violating mass scale. The interaction of the $`\eta \rho \chi `$ type in Eq.(11) is a guarantee of the orthogonal choice of vacuum expectation values (VEVs) for three Higgs scalars, $`\eta `$, $`\rho `$ and $`\chi `$ as $`0|\eta |0=(v_\eta ,0,0)^T`$, $`0|\rho |0=(0,v_\rho ,0)^T`$, and $`0|\chi |0=(0,0,v_\chi )^T`$, respectively.

We note that there are two main differences between the model (c) discussed in Ref. and the model in this article (current model). The first is the absence of an $`SU(3)_L`$ singlet Higgs scalar $`k^{++}`$ in the current model. The model (c) has two Zee-Babu type Higgs scalars called $`k^{++}`$ and $`k^{++}`$, which are needed to realize $`L^{}`$-conserving and $`L^{}`$-violating two-loop interactions. However, in the current model, only one Higgs $`k^{++}`$ is introduced and no additional singlet Higgs is needed because $`L^{}`$-conserving one-loop effects will serve as the $`L^{}`$-violating two-loop effects in the model (c). The second is the different implementation of the discrete symmetry into the models. The discrete symmetry based on $`Z_2`$ is required in model (c) to avoid the FCNC interactions and to prevent the realization of the one-loop effects. Meanwhile, in the current model, the discrete symmetry based on $`Z_4`$ is introduced and the one-loop effects are allowed.

Now, let us demonstrate how radiative corrections induce neutrino masses in our model. The Yukawa interaction denoted by $`_Y`$ and $`L^{}`$-conserving Higgs potential $`V_0`$ work together to generate one-loop interactions as shown in Fig. 1, also $`_Y`$ and $`L^{}`$-violating Higgs potential $`V_b`$ yield two-loop interactions as shown in Fig. 2. From the one-loop diagrams, we obtained the following Majorana neutrino masses:

$`m_{1i}^{(1)}`$ $`=`$ $`f_{[1i]}[\lambda _1{\displaystyle \frac{m_\mathrm{}^i^2F(m_\mathrm{}^i^2,m_{\xi ^+}^2,m_{\rho ^+}^2)m_e^2F(m_e^2,m_{\xi ^+}^2,m_{\rho ^+}^2)}{v_\rho ^2}}`$ (13)
$`+\lambda _2{\displaystyle \frac{m_{E^i}^2F(m_{E^i}^2,m_{\overline{\xi }^+}^2,m_{\chi ^+}^2)m_{E^1}^2F(m_{E^1}^2,m_{\overline{\xi }^+}^2,m_{\chi ^+}^2)}{v_\chi ^2}}]v_\eta v_\rho v_\chi ,`$
where

$`F(x,y,z)`$ $`=`$ $`{\displaystyle \frac{1}{16\pi ^2}}[{\displaystyle \frac{x\mathrm{ln}x}{(xy)(xz)}}+{\displaystyle \frac{y\mathrm{ln}y}{(yx)(yz)}}+{\displaystyle \frac{z\mathrm{ln}z}{(zy)(zx)}}],`$ (14)
and, from the two-loop diagrams, we obtain:

$`m_{11}^{(2)}`$ $`=`$ $`2{\displaystyle \underset{i,j=2,3}{}}\lambda _2f_{[1i]}f_{[1j]}f_k^{ij}\mu _bm_\mathrm{}^im_{E^j}v_\rho v_\chi I^{(2)}`$ (15)
with

$`I^{(2)}`$ $`=`$ $`{\displaystyle \frac{G(m_\mathrm{}^i^2,m_{\xi ^+}^2)\left[G(m_{E^j}^2,m_{\overline{\eta }^{}}^2)G(m_{E^j}^2,m_{\overline{\xi }^+}^2)\right]}{m_k^2\left(m_{\overline{\eta }^{}}^2m_{\overline{\xi }^+}^2\right)}},`$ (16)
$`G(m_a^2,m_b^2)`$ $`=`$ $`{\displaystyle \frac{1}{16\pi ^2}}{\displaystyle \frac{m_a^2\mathrm{ln}(m_a^2/m_k^2)m_b^2\mathrm{ln}(m_b^2/m_k^2)}{m_a^2m_b^2}},`$ (17)
where the relation of $`m_k`$ (masses of other particle) has been used. The outline of the derivation of the two-loop integral, Eq.(17), is shown in the Appendix of Ref..

The neutrino mass matrix is composed of these Majorana masses as

$$M_\nu =\left(\begin{array}{ccc}m_{11}^{(2)}& m_{12}^{(1)}& m_{13}^{(1)}\\ m_{12}^{(1)}& 0& 0\\ m_{13}^{(1)}& 0& 0\end{array}\right),$$
(18)
from which we find the following relations for the neutrino oscillations in our $`SU(3)_L`$ $`\times `$ $`U(1)_N`$ model

$`\mathrm{\Delta }m_{atm}^2=m_{12}^{(1)2}+m_{13}^{(1)2}(m_\nu ^2),\mathrm{\Delta }m_{}^2=2m_\nu |m_{11}^{(2)}|.`$ (19)
The bimaxmal structure of $`M_\nu `$ is realized by requiring that $`|m_{12}^{(1)}||m_{13}^{(1)}|`$, thereby, leading to $`m_{E^2}m_{E^3}`$ or $`m_{E^2,E^3}m_{E^1}`$ because the charged lepton contributions are to be neglected in our case. We assume that $`m_{E^2}m_{E^3}`$ in our analysis.

In order to see that our result, Eq.(19), really regenerates the observed neutrino oscillations, we make the following assumptions on relevant free parameters in the same way as those in Ref.: (1) $`v_\eta =v_w/20`$, $`v_\rho =v_w`$ and $`v_\chi =10v_w`$, where $`v_w=(2\sqrt{2}G_F)^{1/2}=`$174 GeV, (2) $`m_\xi m_\rho =v_w`$, $`m_{\chi ,k}=10v_w`$, $`m_{E^2,E^3}=ev_\chi `$ to enhance the bimaximal mixing and $`m_{E^1}=0.9m_{E^2,E^3}`$ to contribute to $`\mathrm{\Delta }m_{atm}^2`$, where $`e`$ stands for the electromagnetic coupling, (3) $`f_{[1i]}10^7`$, $`\lambda _1=\lambda _2=f_k^{ij}=1`$ and $`\mu _b=ev_\chi `$, where $`f_{[1i]}`$ is determined by $`\mathrm{\Delta }m_{atm}^2`$ = $`m_{12}^{(1)2}+m_{13}^{(1)2}`$ = $`3.0\times 10^3`$ eV2. From numerical calculations of Eq.(19), we find $`f_{[1i]}=0.93\times 10^7`$ eV2, which reproduce $`\mathrm{\Delta }m_{atm}^2=3.0\times 10^3`$ eV2 and $`\mathrm{\Delta }m_{}^2=0.91\times 10^9`$ eV2. As a result, the mixing angle $`\vartheta `$ for atmospheric neutrinos defined by $`\mathrm{cos}\vartheta =m_{12}^{(1)}/m_\nu `$ is computed to yield $`\mathrm{sin}^22\vartheta =0.93`$, where the charged lepton contributions to $`\mathrm{\Delta }m_{atm}^2`$ give the deviation form $`\mathrm{sin}^22\vartheta =1`$ for the bimaximal mixing case. The estimated $`\mathrm{\Delta }m_{}^2`$ lies in the allowed region of the QVO solution to the solar neutrino problem.

Summarizing our discussion, we have constructed an $`SU(3)_L`$ $`\times `$ $`U(1)_N`$ gauge model with lepton triplets $`\psi ^i=(\nu ^i,\mathrm{}^i,E^i)`$, where $`E^i`$ are negatively charged heavy leptons. This model has a triplet version of the Zee scalar $`\xi `$ and a singlet as the Zee-Babu scalar $`k^{++}`$. Owing to the existence of these scalars, our $`SU(3)_L\times U(1)_N`$ model is capable of generating tiny neutrino masses by the radiative mechanism. The atmospheric neutrino oscillation is related to $`L^{}`$-conserving one-loop interactions, while the solar neutrino oscillation is related to $`L^{}`$-violating two-loop interactions, where $`L^{}L_eL_\mu L_\tau `$. As a result, the bimaximal structure of the neutrino mass matrix is enhanced by the approximate degeneracy between masses of heavy leptons of $`E^2`$ and $`E^3`$. The observed mass hierarchy of $`\mathrm{\Delta }m_{atm}^2`$ $``$ $`\mathrm{\Delta }m_{}^2`$ is explained by the difference between one-loop and two-loop effects. From our numerical estimate, our model reproduces the observed neutrino oscillation data $`\mathrm{\Delta }m_{atm}^2=3.0\times 10^3`$ eV2 with $`\mathrm{sin}^2\vartheta =0.93`$ and $`\mathrm{\Delta }m_{}^2=0.91\times 10^9`$ eV2. Our model is, thus, relevant to yield quasivacuum solution for solar neutrino problem.

The author would like to thank Prof. M.Yasuè for many helpful suggestions, useful comments and a careful reading of this article.

Table Captions

Figure Captions

TABLE I. $`L`$ and $`L^{}`$ quantum number.


text:
# Critical behaviour near the metal-insulator transition of a doped Mott insulator

## 1 Introduction

The Mott-Hubbard metal-insulator transition (MIT) is an important but difficult many-body problem which has been studied extensively Mott . Significant progress has been achieved in recent years through the application of dynamical mean-field theory (DMFT) Georges1  to generic microscopic models, such as the single-band Hubbard model. In this approach the lattice problem is mapped onto an impurity problem where a correlated impurity site is embedded in an effective uncorrelated medium that has to be determined self-consistently. The mapping can be shown to be exact for certain models with local interactions in the limit of infinite dimensions Metzner , and constitutes an approximate method for finite-dimensional models. Several techniques have been applied to deal with the effective impurity problem, including iterated perturbation theory Georges1 , non-crossing approximation Pruschke , projective self-consistent method (PSCM) Fisher , quantum Monte Carlo (QMC) Jarrell , exact diagonalization (ED) Caffarel  and numerical renormalization group (NRG) Sakai ; Bulla1  techniques. These methods have different strengths and limitations, and apparent discrepancies between some of the results have led to a controversial discussion on the nature of the MIT in the infinite-dimensional Hubbard model at low temperatures Schlipf ; Rozenberg ; Noack ; Bulla2 ; Krauth . Recently, however, most of these differences have been resolved Bulla3 .

However, not all aspects of the transition have been investigated thoroughly. In particular, the critical behaviour of the doped Mott insulator has not received so much attention as it is more difficult to solve the model off half-filling using purely numerical methods. Iterated perturbation theory, which provides a reasonable description of the MIT at half-filling Georges1 , is less suitable for calculations in the doped case since ad hoc modifications of the approach become necessary away from half-filling KK .

Recently, we have shown Bulla ; Ono  that a linearized form of the DMFT provides a simple and attractive technique to obtain approximate but analytical results for the critical regime. Using this approach for the single- and for the two-band Hubbard model, it has been demonstrated that the predictions for the critical coupling of the MIT are in very good agreement with most accurate numerical estimates.

Here we show that the linearized DMFT can be extended to the non-symmetric case. This allows for a comprehensive analytical investigation of the critical behaviour as a function of doping. In particular, we have calculated the discontinuity in the chemical potential on changing from hole to electron doping. The analytic result is in good agreement with the results of numerical methods, NRG as well as ED. It also agrees well with the result of PSCM Fisher . In addition, we have analytically determined the compressibility, the quasiparticle weight, the double occupancy and the local spin susceptibility near half-filling as functions of the on-site Coulomb interaction and the doping. These are difficult to calculate using the numerical methods mentioned above.

## 2 Linearized dynamical mean-field theory

We consider the single-band Hubbard model at zero temperature on the Bethe lattice Bethe  with infinite connectivity $`q\mathrm{}`$

$`H={\displaystyle \underset{<i,j>,\sigma }{}}t_{i,j}(c_{i\sigma }^{}c_{j\sigma }+h.c.)+U{\displaystyle \underset{i}{}}n_in_i.`$ (1)
The nearest-neighbor hopping is scaled as usual: $`t_{i,j}=\frac{t}{\sqrt{q}}`$ Metzner . For the single-band Hubbard model on the Bethe lattice, the DMFT self-consistency equation is simply given by Georges1

$$𝒢_0(z)^1=z+\mu t^2G(z),$$
(2)
where $`G(z)`$ is the local Green’s function of the Hubbard model and $`𝒢_0(z)=(z\epsilon _f\mathrm{\Delta }(z))^1`$ is the non-interacting Green’s function of an effective single-impurity Anderson model defined by the hybridization function $`\mathrm{\Delta }(z)`$. The DMFT self-consistency cycle starts with a guess for the hybridization function DMFT . The solution of the corresponding impurity model yields the impurity Green’s function $`G(z)`$ to be identified with the on-site Green’s function of the lattice model. From the self-consistency equation (2) $`𝒢_0(z)`$ and thus a new hybridization function $`\mathrm{\Delta }(z)`$ can be calculated. The cycles have to be repeated until self-consistency is achieved.

The application of numerical methods for solving the effective impurity problem (see ref. Bulla2 , for example) have established that at moderate coupling the density of states in the metallic phase is characterized by a three-peak structure consisting of the lower and the upper Hubbard bands and a quasiparticle resonance near the Fermi energy in addition. The quasiparticle peak is more or less isolated from the Hubbard bands. On approaching the Mott-insulating state with increasing interaction strength, the quasiparticle peak becomes extremely narrow and finally vanishes for $`U=U_c`$.

The linearized dynamical mean-field theory Bulla ; Ono  focuses on this critical regime close to the transition. Here, the quasiparticle peak is approximated by a single pole at the Fermi level, i. e. $`G(z)=\frac{Z}{z}`$ near the Fermi level with a small weight $`Z0`$ as $`UU_c`$. Correspondingly, the hybridization function $`\mathrm{\Delta }(z)`$ is a one-pole function $`\mathrm{\Delta }(z)=\frac{V^2}{z}.`$ This effectively represents an approximate mapping of the model (1) onto a two-site or zero-bandwidth Anderson model Hewson

$`H_{2\mathrm{site}}`$ $`=`$ $`\epsilon _f{\displaystyle \underset{\sigma }{}}f_\sigma ^{}f_\sigma +Uf_{}^{}f_{}f_{}^{}f_{}`$ (3)
$`+`$ $`\epsilon _c{\displaystyle \underset{\sigma }{}}c_\sigma ^{}c_\sigma +V{\displaystyle \underset{\sigma }{}}(f_\sigma ^{}c_\sigma +c_\sigma ^{}f_\sigma )`$
with $`\epsilon _c=0`$ and $`\epsilon _f=\mu `$. The hybridization strength $`V`$ has be determined from the self-consistency equation which takes the simple form

$`t^2Z=V^2.`$ (4)
For a more detailed discussion and for an extension of the approach to the two-band model see refs. Bulla ; Ono .

Now we calculate the critical value of $`U`$ for the MIT at half-filling. In this case, the chemical potential is fixed to $`\mu =\frac{U}{2}`$ due to particle-hole symmetry. Close to the MIT $`V`$ is small, and $`V0`$ for $`UU_c`$. The weight $`Z`$ can be calculated from the impurity spectral function and is given by Hewson  (see also Appendix A)

$`Z=36{\displaystyle \frac{V^2}{U^2}},`$ (5)
up to second order in $`V`$. From eqs. (4,5), we obtain the critical value

$`U_c=6t.`$ (6)
This result is in good agreement with the best numerical estimates of NRG ($`U_c=5.88t`$) Bulla2  and ED ($`U_c=5.87t`$) Ono  as well as PSCM ($`U_c=5.84t`$) Georges1 .

When we solve the self-consistency equation (4) by iteration, $`V^2`$ increases exponentially with iteration number for $`U<U_c`$. In this case, the single-pole approximation for $`\mathrm{\Delta }(z)`$ breaks down. On the other hand, for $`U>U_c`$, the hybridization strength $`V^2`$ decreases exponentially to give the self-consistent value $`V^2=0`$ corresponding to the insulating solution.

## 3 Critical behaviour of the single-band Hubbard model

### 3.1 Physical quantities

For more extensive studies of the critical region of the Mott MIT, we need the result for the quasiparticle weight up to fourth order in $`V`$ (see Appendix A),

$`Z=V^2F(U,\mu )V^4G(U,\mu ),`$ (7)
where

$`F(U,\mu )`$ $`=`$ $`{\displaystyle \frac{5}{2\mu ^2}}+{\displaystyle \frac{4}{\mu (U\mu )}}+{\displaystyle \frac{5}{2(U\mu )^2}},`$ (8)
$`G(U,\mu )`$ $`=`$ $`{\displaystyle \frac{29}{2\mu ^4}}+{\displaystyle \frac{24}{\mu ^3(U\mu )}}+{\displaystyle \frac{22}{\mu ^2(U\mu )^2}}`$ (9)
$`+{\displaystyle \frac{24}{\mu (U\mu )^3}}+{\displaystyle \frac{29}{2(U\mu )^4}}.`$
To determine the doping dependence, we also calculate the impurity occupation number up to second order in $`V`$ (see Appendix A)

$`n=1+V^2D(U,\mu ),`$ (10)
where

$`D(U,\mu )={\displaystyle \frac{2}{(U\mu )^2}}{\displaystyle \frac{2}{\mu ^2}}.`$ (11)
We note that, for $`\mu \stackrel{\stackrel{_>}{_=}}{_<}\frac{U}{2}`$, $`D\stackrel{\stackrel{_>}{_=}}{_<}0`$ and thus $`n\stackrel{\stackrel{_>}{_=}}{_<}1`$. The double occupancy $`d=\widehat{n}_{}\widehat{n}_{}`$ is given by (see Appendix A)

$`d={\displaystyle \frac{2V^2}{(U\mu )^2}},`$ (12)
up to second order in $`V`$. We also calculate the static local spin susceptibility, $`\chi _0\chi _{ii}(0)`$, with

$`\chi _{ii}(\omega )={\displaystyle _{\mathrm{}}^{\mathrm{}}}dt\mathrm{e}^{\mathrm{i}\omega t}\mathrm{i}\theta (t)[\widehat{S_i}^{}(t),\widehat{S_i}^+],`$ (13)
where $`\widehat{S_i}^\pm `$ are the spin raising and lowering operators at the same site $`i`$ and where we set $`(g\mu _B)^2/2=1`$. At $`T=0`$, $`\chi _0`$ is given by

$`\chi _0={\displaystyle \underset{n}{}}{\displaystyle \frac{|E_n|\widehat{S}^+|E_0|^2+|E_n|\widehat{S}^{}|E_0|^2}{E_nE_0}},`$ (14)
where $`|E_n`$ are the eigenstates with the eigenenergies $`E_n`$, and $`|E_0`$ is the ground state. By using the results for the 2-site Anderson model in eq.(14), we obtain (see Appendix A)

$`\chi _0={\displaystyle \frac{1}{2V^2\left(\frac{1}{\mu }+\frac{1}{U\mu }\right)}}\left(1+O(V^2)\right).`$ (15)
We now invoke the self-consistency equation (4) and substitute $`V^2`$ from eq.(4) into eqs.(7,10,12,15). This yields

$`Z(U,\mu )`$ $`=`$ $`\left(F(U,\mu ){\displaystyle \frac{1}{t^2}}\right){\displaystyle \frac{1}{t^2G(U,\mu )}},`$ (16)
$`n(U,\mu )`$ $`=`$ $`1+Z(U,\mu )t^2D(U,\mu ),`$ (17)
$`d(U,\mu )`$ $`=`$ $`2t^2Z(U,\mu )/(U\mu )^2,`$ (18)
$`\chi _0(U,\mu )`$ $`=`$ $`\mu (U\mu )/\left(2Ut^2Z(U,\mu )\right).`$ (19)
### 3.2 Critical behaviour at half-filling

First we discuss the critical behaviour near the Mott MIT at half-filling Bulla . The chemical potential is fixed to $`\mu =\frac{U}{2}`$ due to particle-hole symmetry. In fact, eq.(10) yields $`n(U,\frac{U}{2})=1`$ for all $`U`$ as $`D(U,\frac{U}{2})=0`$ from eq.(11). Substituting $`\mu =\frac{U}{2}`$ into eqs.(16,18,19), we obtain

$`Z(U)`$ $`=`$ $`{\displaystyle \frac{18}{11}}\left(1{\displaystyle \frac{U}{U_c}}\right),`$ (20)
$`d(U)`$ $`=`$ $`{\displaystyle \frac{4}{11}}\left(1{\displaystyle \frac{U}{U_c}}\right),`$ (21)
$`\chi _0(U)`$ $`=`$ $`{\displaystyle \frac{11}{24t}}\left(1{\displaystyle \frac{U}{U_c}}\right)^1,`$ (22)
near $`U_c`$ for $`U<U_c`$. The result for $`Z`$, eq.(20), has already been obtained by Bulla and Potthoff Bulla . Using eq.(17) the compressibility, $`\kappa =(\frac{n}{\mu })__U`$, is given by

$`\kappa (U)=t^2Z(U){\displaystyle \frac{D(U,\mu )}{\mu }}|_{\mu =\frac{U}{2}},`$ (23)
at half-filling for $`U<U_c`$. Substituting eqs.(11,20) into eq.(23), we obtain

$`\kappa (U)={\displaystyle \frac{16}{33t}}\left(1{\displaystyle \frac{U}{U_c}}\right),`$ (24)
near $`U_c`$ for $`U<U_c`$.

Due to local charge fluctuations the double occupancy is finite even in the insulating phase with $`d(U)0`$ only for $`U\mathrm{}`$. The linearized DMFT, however, predicts a vanishing double occupancy for $`UU_c`$. This indicates that the approach misses these local fluctuations. We nevertheless believe that the trends in the metallic phase are correct on the mean-field level. This situation may be analogous to the mean-field theory of ferromagnetism in the Heisenberg model, where the fluctuations in the magnetization and short-range order cannot be taken into account. We also note that the local spin susceptibility diverges in the limit of the MIT $`UU_c`$. Even in this limit, however, the uniform spin susceptibility is finite due to the effect of the super-exchange interaction $`J=2t^2/U`$ Georges1 .

### 3.3 Discontinuity in the chemical potential

For $`U<U_c`$ the chemical potential $`\mu `$ as a function of $`n`$ is continuous at $`n=1`$. For $`U>U_c`$, on the other hand, $`\mu (n)`$ has a discontinuity at $`n=1`$: At half-filling the system is a Mott insulator for $`\mu _{}<\mu <\mu _+`$ where $`\mu _{}=\mu _{}(U)`$, $`\mu _+=\mu _+(U)`$, and $`\mu _{}(U)<\mu _+(U)`$ for $`U>U_c`$. The jump $`\mathrm{\Delta }\mu =\mu _+\mu _{}`$ can be calculated within the linearized DMFT exploiting the fact that the MIT is characterized by a vanishing quasiparticle weight. Setting $`Z=0`$ in eq.(16), we obtain an equation to determine the MIT point:

$`F(U,\mu )={\displaystyle \frac{1}{t^2}}.`$ (25)
In Fig. 1, $`F(U,\mu )`$ is plotted as a function of $`\mu `$ for several values of $`U`$. When $`U<U_c`$, $`F(U,\mu )>\frac{1}{t^2}`$ for all $`\mu `$, and the system is metallic. When $`U>U_c`$, $`F(U,\mu )=\frac{1}{t^2}`$ for $`\mu =\mu _\pm `$ ($`\mu _+>\mu _{}`$), and the system is insulating for $`\mu _{}<\mu <\mu _+`$ while it is metallic for $`\mu <\mu _{}`$ and $`\mu >\mu _+`$. We notice that, for $`U=U_c`$, $`F(U,\mu )`$ as a function of $`\mu `$ is at its minimum for $`\mu =\frac{U}{2}`$ consistent with the considerations in ref. Ono .

Using eq.(8) we can solve eq.(25) to get the explicit $`U`$ dependence of $`\mu _\pm `$ for $`U>U_c`$

$`\mu _\pm ={\displaystyle \frac{U}{2}}\pm {\displaystyle \frac{U}{2}}\left(1+{\displaystyle \frac{1}{18u^2}}\sqrt{{\displaystyle \frac{10}{9u^2}}+\left({\displaystyle \frac{1}{18u^2}}\right)^2}\right)^{\frac{1}{2}},`$ (26)
where $`u\frac{U}{U_c}>1`$. For the discontinuous jump $`\mathrm{\Delta }\mu =\mu _+\mu _{}`$ we obtain

$`\mathrm{\Delta }\mu =U\left(1+{\displaystyle \frac{1}{18u^2}}\sqrt{{\displaystyle \frac{10}{9u^2}}+\left({\displaystyle \frac{1}{18u^2}}\right)^2}\right)^{\frac{1}{2}}.`$ (27)
Note that we have $`n1`$ with $`n<1`$ ($`n>1`$) from eq.(17) for $`\mu \mu _{}`$ ($`\mu \mu _+`$) from the metallic side. For $`U>U_c`$ close to $`U_c`$, eq.(27) yields

$`\mathrm{\Delta }\mu ={\displaystyle \frac{6}{\sqrt{38}}}U_c\sqrt{{\displaystyle \frac{U}{U_c}}1}.`$ (28)
In Fig. 2 we have plotted $`\mathrm{\Delta }\mu `$, as given by eq.(27), as a function of $`U`$.

We have also calculated $`\mathrm{\Delta }\mu `$ numerically by using the NRG and the ED method. We solved the full DMFT equation numerically and obtained the occupation number $`n`$ as a function of $`\mu `$. When $`\mu `$ approaches $`\mu _+`$ ($`\mu _{}`$) from above (below), $`n`$ approaches unity from above (below) and $`n=1`$ for $`\mu _{}<\mu <\mu _+`$. We also confirmed that, at $`\mu =\mu _\pm `$, the groundstate changes from singlet ($`\mu <\mu _{}`$ or $`\mu >\mu _+`$) to doublet ($`\mu _{}<\mu <\mu _+`$). The ED calculations were done for finite cluster sizes $`n_s`$ up to $`n_s=11`$. An extrapolation of the results yields the $`n_s\mathrm{}`$ extrapolated value of $`\mathrm{\Delta }\mu `$ as shown in the inset of Fig. 2.

As can be seen from Fig. 2, the result from the linearized DMFT is in good agreement with the results of the NRG and the ED. It also agrees well with the result from the PSCM Fisher . We note that the result for $`\mu _\pm `$ from the linearized DMFT seems to be less satisfying for the strong-coupling limit $`UU_c`$. This may be explained by the fact that here $`\mu _\pm `$ is very close to the edge of the lower or upper Hubbard band, respectively, and that the effect of the bandwidth, which is neglected in the linearized DMFT Bulla , becomes important Uc .

In the case of half-filling, as $`U`$ approaches $`U_c`$ from below, we have the picture of well separated lower and upper Hubbard bands with a quasiparticle peak in between. The quasiparticle peak disappears at $`U=U_c`$ leaving an insulator with a finite gap. For $`U>U_c`$, Fisher et al. Fisher  give a similar picture for the slightly doped case in terms of quasiparticle in-gap states. The jump $`\mathrm{\Delta }\mu `$ from hole to electron doping tends to zero as $`UU_c`$ from above, so the Fermi level in the slightly hole-doped case must lie within the quasiparticle peak which in turn lies within the Mott-Hubbard gap. The same applies to the slightly electron-doped case. This interpretation is confirmed by more extensive NRG and ED calculations.

### 3.4 Doping dependence

Finally, we discuss the critical behaviour of the doped metallic system for $`U>U_c`$ close to the Mott insulating phase. Substituting eq.(26) into eq.(17), we obtain the doping dependence of the quasiparticle weight for $`n1`$ and $`U>U_c`$

$`Z(U,n)=C(U)|n1|,`$ (29)
where the coefficient $`C(U)`$ is given by

$`C(U)^1=t^2|D(U,\mu _\pm )|=32t^2{\displaystyle \frac{U\mathrm{\Delta }\mu }{[U^2(\mathrm{\Delta }\mu )^2]^2}}.`$ (30)
Due to particle-hole symmetry we obtain the same result for both, $`n<1`$ and $`n>1`$.

Eliminating $`Z`$ from eqs.(16,17), the occupation number can be expressed as a function of $`U`$ and $`\mu `$. For $`U>U_c`$ and close to the MIT we have

$`n(U,\mu )=1+\left(F(U,\mu ){\displaystyle \frac{1}{t^2}}\right){\displaystyle \frac{D(U,\mu )}{G(U,\mu )}}.`$ (31)
This also yields the compressibility in the limit $`n1`$ for $`U>U_c`$

$`\kappa (U)={\displaystyle \frac{D(U,\mu _\pm )}{G(U,\mu _\pm )}}{\displaystyle \frac{F(U,\mu )}{\mu }}|_{\mu =\mu _\pm }.`$ (32)
Again, due to particle-hole symmetry, the result eq.(32) for $`\kappa `$ is the same for both, $`n<1`$ and $`n>1`$.

Substituting eqs.(26,29) into eq.(18), the double occupancy is obtained as a function of $`U`$ and $`n`$ for $`n1`$ and $`U>U_c`$

$`d(U,n)=\alpha _\pm (U)|n1|,`$ (33)
where

$`\alpha _\pm (U)^1={\displaystyle \frac{16(U\mu _\pm )^2U\mathrm{\Delta }\mu }{[U^2(\mathrm{\Delta }\mu )^2]^2}},`$ (34)
and where $`+`$ and $``$ stand for $`n>1`$ and $`n<1`$, respectively. For a given interaction strength $`U`$ we find $`\alpha _+>\alpha _{}`$. This means that when doping the system away from half-filling, the increase of the double occupancy for $`n>1`$ is stronger than its decrease for $`n<1`$. As mentioned before, there is a finite double occupancy even for $`n=1`$ and $`U>U_c`$ in contrast to the result eq.(33) from the linearized DMFT. Nevertheless, we believe that the trend in the metallic state, i.e. the coefficient $`\alpha _\pm `$, is physically significant.

Substituting eqs.(26,29) into eq.(19), the local spin susceptibility is obtained as a function of $`U`$ and $`n`$ for $`n1`$ and $`U>U_c`$

$`\chi _0(U,n)=\beta (U)|n1|^1,`$ (35)
where

$`\beta (U)={\displaystyle \frac{4\mathrm{\Delta }\mu }{U^2(\mathrm{\Delta }\mu )^2}}.`$ (36)
In Fig. 3, $`C^1`$, $`\kappa `$, $`\alpha _\pm ^1`$ and $`\beta `$, as given by eqs.(30,32, 34,36), are plotted as functions of $`U`$. To see the critical properties near $`U_c`$, we substitute eq.(28) into eqs.(30,32,34, 36), and obtain for $`U>U_c`$

$`C(U)^1`$ $`=`$ $`{\displaystyle \frac{16}{3\sqrt{38}}}\sqrt{{\displaystyle \frac{U}{U_c}}1},`$ (37)
$`\kappa (U)`$ $`=`$ $`{\displaystyle \frac{32}{33t}}\left({\displaystyle \frac{U}{U_c}}1\right),`$ (38)
$`\alpha _\pm (U)^1`$ $`=`$ $`{\displaystyle \frac{24}{\sqrt{38}}}\sqrt{{\displaystyle \frac{U}{U_c}}1},`$ (39)
$`\beta (U)`$ $`=`$ $`{\displaystyle \frac{4}{\sqrt{38}t}}\sqrt{{\displaystyle \frac{U}{U_c}}1}.`$ (40)
The critical properties near $`U_c`$ as resulting from the linearized DMFT are similar to those of the Brinkman-Rice approach Vollhardt ; Vollhardt2 . However, the coefficients are different.

## 4 Conclusion and discussion

We have shown that analytical calculations of the critical behaviour in the parameter region close to the Mott MIT can be carried out by using a simple linearized version of the DMFT. This approach gives rather reliable estimates for the critical parameters at the transition point. Considering the single-band Hubbard model, we have calculated the discontinuity in the chemical potential $`\mu `$ for the change from hole to electron doping. The analytical result is in good agreement with the numerical estimates from the PSCM, the NRG and the ED. The results for small hole and electron doping and for $`U>U_c`$ can be interpreted in terms of quasiparticle in-gap states which lie within the Mott-Hubbard gap. We have also made predictions for the compressibility, the quasiparticle weight, the double occupancy and the local spin susceptibility near half-filling as functions of $`U`$ and the doping. It would be interesting to see whether these predictions can be confirmed by some of the more comprehensive numerical realizations of DMFT, and whether there is any experimental evidence in support of them Imada .

The simplicity of our approach should also enable similar calculations to be made for more general models, such as multi-band Hubbard-type models, where we can have both Mott-Hubbard type and charge-transfer type metal-insulator transitions Ono1 . Even for more complex multi-band models one might obtain analytical expressions as has been demonstrated recently for the five critical parameters in the two-band Hubbard model Ono . This makes the linearized DMFT a powerful technique for exploring general trends and phase diagrams within a high-dimensional parameter space. An interesting question to examine would be the role of in-gap states in the two-band Hubbard model (equivalent to the $`d`$-$`p`$ model) near the MIT. In this parameter regime the results of the model should be relevant for a description of the behaviour of weakly doped high-$`T_c`$ materials.

## 5 Acknowledgments

We gratefully acknowledge the support of the Grant-in-Aid for Scientific Research from the Ministry of Education, Science, Sports and Culture, and also by CREST (Core Research for Evolutional Science and Technology) of Japan Science and Technology Corporation (JST) (YŌ); the Deutsche Forschungsgemeinschaft, through the Sonderforschungsbereich 484 (RB) and 290 (MP); and the EPSRC, through research grant (GR/J85349) (ACH). We also wish to thank the Newton Institute in Cambridge for providing facilities and support for this work during their six month programme on ‘Strongly Correlated Electron Systems’.

## Appendix A ppendix A

Here we discuss the two-site Anderson model eq.(3) Hewson  in the limit $`V0`$. We assume that the conduction level is between the atomic $`f`$-level and the upper Hubbard level $`\epsilon _f<\epsilon _c<\epsilon _f+U.`$ Then we define

$`\mathrm{\Delta }`$ $``$ $`\epsilon _c\epsilon _f>0,`$ (41)
$`W`$ $``$ $`\epsilon _f+U\epsilon _c>0.`$ (42)
The one-electron eigenstates

$`|E_\pm =a_\pm f_\sigma ^+|0+b_\pm c_\sigma ^+|0,`$ (43)
correspond to the eigenenergies

$`E_\pm ={\displaystyle \frac{1}{2}}\left(\epsilon _c+\epsilon _f\pm \sqrt{(\epsilon _c\epsilon _f)^2+4V^2}\right).`$ (44)
For small hybridization strength $`V^2\mathrm{\Delta }`$, eq.(44) is simplified as

$`E_+`$ $`=`$ $`\epsilon _c+{\displaystyle \frac{V^2}{\mathrm{\Delta }}}{\displaystyle \frac{V^4}{\mathrm{\Delta }^3}},`$ (45)
$`E_{}`$ $`=`$ $`\epsilon _f{\displaystyle \frac{V^2}{\mathrm{\Delta }}}+{\displaystyle \frac{V^4}{\mathrm{\Delta }^3}},`$ (46)
to fourth order in $`V`$, with the corresponding eigenstates

$`|E_+=\alpha \left\{{\displaystyle \frac{V}{\mathrm{\Delta }}}\left(1{\displaystyle \frac{V^2}{\mathrm{\Delta }^2}}\right)f_\sigma ^++c_\sigma ^+\right\}|0,`$ (47)
$`|E_{}=\alpha \left\{f_\sigma ^+{\displaystyle \frac{V}{\mathrm{\Delta }}}\left(1{\displaystyle \frac{V^2}{\mathrm{\Delta }^2}}\right)c_\sigma ^+\right\}|0,`$ (48)
where

$`\alpha ^2=1{\displaystyle \frac{V^2}{\mathrm{\Delta }^2}}+3{\displaystyle \frac{V^4}{\mathrm{\Delta }^4}}.`$ (49)
Similarly, we obtain the three-electron (one-hole) eigenenergies

$`\overline{E}_\pm ={\displaystyle \frac{1}{2}}\left(3\epsilon _c+3\epsilon _f+U\pm \sqrt{(\epsilon _f+U\epsilon _c)^2+4V^2}\right).`$ (50)
For small hybridization strength $`V^2W`$, eq.(50) is simplified as

$`\overline{E}_+`$ $`=`$ $`\epsilon _c+2\epsilon _f+U+{\displaystyle \frac{V^2}{W}}{\displaystyle \frac{V^4}{W^3}},`$ (51)
$`\overline{E}_{}`$ $`=`$ $`2\epsilon _c+\epsilon _f{\displaystyle \frac{V^2}{W}}+{\displaystyle \frac{V^4}{W^3}},`$ (52)
to fourth order in $`V`$. The corresponding eigenstates are

$`|\overline{E}_+`$ $`=`$ $`\overline{\alpha }\left\{{\displaystyle \frac{V}{W}}\left(1{\displaystyle \frac{V^2}{W^2}}\right)f_\sigma +c_\sigma \right\}|4,`$ (53)
$`|\overline{E}_{}`$ $`=`$ $`\overline{\alpha }\left\{f_\sigma +{\displaystyle \frac{V}{W}}\left(1{\displaystyle \frac{V^2}{W^2}}\right)c_\sigma \right\}|4,`$ (54)
where

$`\overline{\alpha }^2=1{\displaystyle \frac{V^2}{W^2}}+3{\displaystyle \frac{V^4}{W^4}},`$ (55)
and $`|4=f_{}^+f_{}^+c_{}^+c_{}^+|0.`$

The two electron states can be classified as singlets or triplets. In the triplet state, the spatial part of the wavefunction is antisymmetric and the interaction $`U`$ has no effect. Then the total energy of the triplet state is given by $`E_++E_{}=\epsilon _c+\epsilon _f.`$ There are three possible singlet states which can be written by the linear combination of the states,

$`|\varphi _1`$ $`=`$ $`{\displaystyle \frac{1}{\sqrt{2}}}(c_{}^+f_{}^+c_{}^+f_{}^+)|0,`$ (56)
$`|\varphi _2`$ $`=`$ $`c_{}^+c_{}^+|0,`$ (57)
$`|\varphi _3`$ $`=`$ $`f_{}^+f_{}^+|0.`$ (58)
The eigenenergies are given by the solutions of the equation,

$`\left|\begin{array}{ccc}E\epsilon _c\epsilon _f& \sqrt{2}V& \sqrt{2}V\\ \sqrt{2}V& E2\epsilon _c& 0\\ \sqrt{2}V& 0& E2\epsilon _fU\end{array}\right|=0.`$ (62)
To fourth order in $`V`$, the ground state eigenenergy is

$`E_0=\epsilon _c+\epsilon _f2V^2\left({\displaystyle \frac{1}{\mathrm{\Delta }}}+{\displaystyle \frac{1}{W}}\right)\left(1{\displaystyle \frac{2V^2}{\mathrm{\Delta }^2}}{\displaystyle \frac{2V^2}{W^2}}\right),`$ (63)
and the corresponding singlet ground state is

$`|E_0=\alpha _0\{|\varphi _1{\displaystyle \frac{\sqrt{2}V}{\mathrm{\Delta }}}(1{\displaystyle \frac{2V^2}{\mathrm{\Delta }^2}}{\displaystyle \frac{2V^2}{\mathrm{\Delta }W}})|\varphi _2`$
$`{\displaystyle \frac{\sqrt{2}V}{W}}(1{\displaystyle \frac{2V^2}{W^2}}{\displaystyle \frac{2V^2}{\mathrm{\Delta }W}})|\varphi _3\},`$ (64)
with

$`\alpha _0^2`$ $`=`$ $`12V^2\left({\displaystyle \frac{1}{\mathrm{\Delta }^2}}+{\displaystyle \frac{1}{W^2}}\right)`$ (65)
$`+`$ $`4V^4\left({\displaystyle \frac{3}{\mathrm{\Delta }^4}}+{\displaystyle \frac{2}{\mathrm{\Delta }^3W}}+{\displaystyle \frac{2}{\mathrm{\Delta }^2W^2}}+{\displaystyle \frac{2}{\mathrm{\Delta }W^3}}+{\displaystyle \frac{3}{W^4}}\right).`$
Now we calculate the $`f`$-electron Green’s function of this model. When a $`f,`$ electron is removed from the ground state $`|E_0`$, there are two possible final states: $`|E_+`$ and $`|E_{}`$. Correspondingly, there are two possible single-hole excitations with excitation energies,

$`E_+E_0`$ $`=`$ $`\epsilon _f+V^2\left({\displaystyle \frac{3}{\mathrm{\Delta }}}+{\displaystyle \frac{2}{W}}\right)`$ (66)
$``$ $`V^4\left({\displaystyle \frac{5}{\mathrm{\Delta }^3}}+{\displaystyle \frac{4}{\mathrm{\Delta }^2W}}+{\displaystyle \frac{4}{\mathrm{\Delta }W^2}}+{\displaystyle \frac{4}{W^3}}\right)`$
$``$ $`\epsilon _1,`$
$`E_{}E_0`$ $`=`$ $`\epsilon _c+V^2\left({\displaystyle \frac{1}{\mathrm{\Delta }}}+{\displaystyle \frac{2}{W}}\right)`$ (67)
$``$ $`V^4\left({\displaystyle \frac{3}{\mathrm{\Delta }^3}}+{\displaystyle \frac{4}{\mathrm{\Delta }^2W}}+{\displaystyle \frac{4}{\mathrm{\Delta }W^2}}+{\displaystyle \frac{4}{W^3}}\right)`$
$``$ $`\epsilon _2,`$
to fourth order in $`V`$. The matrix elements for these transitions are

$`E_+|f_{}|E_0`$ $`=`$ $`{\displaystyle \frac{\alpha \alpha _0}{\sqrt{2}}}\{1{\displaystyle \frac{2V^2}{\mathrm{\Delta }W}}`$
$`\times (1{\displaystyle \frac{V^2}{\mathrm{\Delta }^2}})(1{\displaystyle \frac{2V^2}{W^2}}{\displaystyle \frac{2V^2}{\mathrm{\Delta }W}})\},`$
$`E_{}|f_{}|E_0`$ $`=`$ $`{\displaystyle \frac{\alpha \alpha _0}{\sqrt{2}}}\{{\displaystyle \frac{V}{\mathrm{\Delta }}}(1{\displaystyle \frac{V^2}{\mathrm{\Delta }^2}})`$
$``$ $`{\displaystyle \frac{2V}{W}}(1{\displaystyle \frac{2V^2}{W^2}}{\displaystyle \frac{2V^2}{\mathrm{\Delta }W}})\},`$
which yield the transition probabilities:

$`|E_+|f_{}|E_0|^2`$ $`=`$ $`{\displaystyle \frac{1}{2}}{\displaystyle \frac{V^2}{2}}\left({\displaystyle \frac{3}{\mathrm{\Delta }^2}}+{\displaystyle \frac{4}{\mathrm{\Delta }W}}+{\displaystyle \frac{2}{W^2}}\right)+{\displaystyle \frac{V^4}{2}}`$ (68)
$`\times `$ $`\left({\displaystyle \frac{17}{\mathrm{\Delta }^4}}+{\displaystyle \frac{24}{\mathrm{\Delta }^3W}}+{\displaystyle \frac{22}{\mathrm{\Delta }^2W^2}}+{\displaystyle \frac{24}{\mathrm{\Delta }W^3}}+{\displaystyle \frac{12}{W^4}}\right)`$
$``$ $`w_1,`$
$`|E_{}|f_{}|E_0|^2`$ $`=`$ $`{\displaystyle \frac{V^2}{2}}\left({\displaystyle \frac{1}{\mathrm{\Delta }^2}}+{\displaystyle \frac{4}{\mathrm{\Delta }W}}+{\displaystyle \frac{4}{W^2}}\right){\displaystyle \frac{V^4}{2}}`$ (69)
$`\times `$ $`\left({\displaystyle \frac{5}{\mathrm{\Delta }^4}}+{\displaystyle \frac{16}{\mathrm{\Delta }^3W}}+{\displaystyle \frac{22}{\mathrm{\Delta }^2W^2}}+{\displaystyle \frac{32}{\mathrm{\Delta }W^3}}+{\displaystyle \frac{24}{W^4}}\right)`$
$``$ $`w_2,`$
to fourth order in $`V`$.

When a $`f,`$ electron is added to the ground state $`|E_1`$, possible final states are $`|\overline{E}_{}`$ and $`|\overline{E}_+`$. Correspondingly, there are two possible single-particle excitations with excitation energies,

$`\overline{E}_{}E_0`$ $`=`$ $`\epsilon _c+V^2\left({\displaystyle \frac{2}{\mathrm{\Delta }}}+{\displaystyle \frac{1}{W}}\right)`$ (70)
$``$ $`V^4\left({\displaystyle \frac{4}{\mathrm{\Delta }^3}}+{\displaystyle \frac{4}{\mathrm{\Delta }^2W}}+{\displaystyle \frac{4}{\mathrm{\Delta }W^2}}+{\displaystyle \frac{3}{W^3}}\right)`$
$``$ $`\epsilon _3,`$
$`\overline{E}_+E_0`$ $`=`$ $`\epsilon _f+U+V^2\left({\displaystyle \frac{2}{\mathrm{\Delta }}}+{\displaystyle \frac{3}{W}}\right)`$ (71)
$``$ $`V^4\left({\displaystyle \frac{4}{\mathrm{\Delta }^3}}+{\displaystyle \frac{4}{\mathrm{\Delta }^2W}}+{\displaystyle \frac{4}{\mathrm{\Delta }W^2}}+{\displaystyle \frac{5}{W^3}}\right)`$
$``$ $`\epsilon _4,`$
to fourth order in $`V`$. The matrix elements for these transitions are

$`\overline{E}_{}|f_{}|E_0`$ $`=`$ $`{\displaystyle \frac{\overline{\alpha }\alpha _0}{\sqrt{2}}}\{{\displaystyle \frac{V}{W}}(1{\displaystyle \frac{V^2}{W^2}})`$
$`+`$ $`{\displaystyle \frac{2V}{\mathrm{\Delta }}}(1{\displaystyle \frac{2V^2}{\mathrm{\Delta }^2}}{\displaystyle \frac{2V^2}{\mathrm{\Delta }W}})\},`$
$`\overline{E}_+|f_{}|E_0`$ $`=`$ $`{\displaystyle \frac{\overline{\alpha }\alpha _0}{\sqrt{2}}}\{1{\displaystyle \frac{2V^2}{\mathrm{\Delta }W}}`$
$`\times (1{\displaystyle \frac{V^2}{W^2}})(1{\displaystyle \frac{2V^2}{\mathrm{\Delta }^2}}{\displaystyle \frac{2V^2}{\mathrm{\Delta }W}})\},`$
which yield the transition probabilities:

$`|\overline{E}_{}|f_{}|E_0|^2`$ $`=`$ $`{\displaystyle \frac{V^2}{2}}\left({\displaystyle \frac{4}{\mathrm{\Delta }^2}}+{\displaystyle \frac{4}{\mathrm{\Delta }W}}+{\displaystyle \frac{1}{W^2}}\right){\displaystyle \frac{V^4}{2}}`$ (72)
$`\times `$ $`\left({\displaystyle \frac{24}{\mathrm{\Delta }^4}}+{\displaystyle \frac{32}{\mathrm{\Delta }^3W}}+{\displaystyle \frac{22}{\mathrm{\Delta }^2W^2}}+{\displaystyle \frac{16}{\mathrm{\Delta }W^3}}+{\displaystyle \frac{5}{W^4}}\right)`$
$``$ $`w_3,`$
$`|\overline{E}_+|f_{}|E_0|^2`$ $`=`$ $`{\displaystyle \frac{1}{2}}{\displaystyle \frac{V^2}{2}}\left({\displaystyle \frac{2}{\mathrm{\Delta }^2}}+{\displaystyle \frac{4}{\mathrm{\Delta }W}}+{\displaystyle \frac{3}{W^2}}\right)+{\displaystyle \frac{V^4}{2}}`$ (73)
$`\times `$ $`\left({\displaystyle \frac{12}{\mathrm{\Delta }^4}}+{\displaystyle \frac{24}{\mathrm{\Delta }^3W}}+{\displaystyle \frac{22}{\mathrm{\Delta }^2W^2}}+{\displaystyle \frac{24}{\mathrm{\Delta }W^3}}+{\displaystyle \frac{17}{W^4}}\right)`$
$``$ $`w_4,`$
to fourth order in $`V`$.

From eqs.(66-73), we obtain the $`f`$-electron Green’s function which has four poles:

$`G_\sigma (z)={\displaystyle \underset{i=1}{\overset{4}{}}}{\displaystyle \frac{w_i}{z\epsilon _i}}.`$ (74)
In the limit $`V0`$, high-energy poles at $`\epsilon _1\epsilon _f`$ and $`\epsilon _4\epsilon _f+U`$ have large residues $`w_1w_2\frac{1}{2}`$, while low-energy poles merge together at $`\epsilon _2\epsilon _30`$ with small total weight $`Zw_2+w_3`$:

$`Z`$ $`=`$ $`V^2\left({\displaystyle \frac{5}{2\mathrm{\Delta }^2}}+{\displaystyle \frac{4}{\mathrm{\Delta }W}}+{\displaystyle \frac{5}{2W^2}}\right)`$
$``$ $`V^4\left({\displaystyle \frac{29}{2\mathrm{\Delta }^4}}+{\displaystyle \frac{24}{\mathrm{\Delta }^3W}}+{\displaystyle \frac{22}{\mathrm{\Delta }^2W^2}}+{\displaystyle \frac{24}{\mathrm{\Delta }W^3}}+{\displaystyle \frac{29}{2W^4}}\right),`$
to fourth order in $`V`$. The number of $`f`$ electrons, $`n=2(w_1+w_2)`$, is given by

$`n=1`$ $``$ $`2V^2\left({\displaystyle \frac{1}{\mathrm{\Delta }^2}}{\displaystyle \frac{1}{W^2}}\right)`$
$`+`$ $`4V^4\left({\displaystyle \frac{3}{\mathrm{\Delta }^4}}+{\displaystyle \frac{2}{\mathrm{\Delta }^3W}}{\displaystyle \frac{2}{\mathrm{\Delta }W^3}}{\displaystyle \frac{3}{W^4}}\right),`$
to fourth order in $`V`$. By using eq.(64), we obtain the double occupancy, $`d=E_0|\widehat{n}_f\widehat{n}_f|E_0,`$ to fourth order in $`V`$

$`d={\displaystyle \frac{2V^2}{W^2}}\left\{1V^2\left({\displaystyle \frac{2}{\mathrm{\Delta }^2}}+{\displaystyle \frac{4}{\mathrm{\Delta }W}}+{\displaystyle \frac{6}{W^2}}\right)\right\}.`$