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# Correlation gap in the heavy-fermion antiferromagnet UPd2Al3

## I Introduction

More than twenty years after the discovery of superconductivity in heavy-fermion (HF) compounds, the nature of the superconducting ground state is still under debate. In particular the discovery of the coexistence of antiferromagnetic (AF) ordering and superconductivity in some of these materials has reinforced the interest to study the interplay between electronic and magnetic degrees of freedom in these correlated electron systems. Instead of the conventional electron-phonon interaction, the electron-magnon correlations have been proposed to cause the pairing in HF superconductors. Heavy fermions are intermetallic compounds containing elements with $`f`$ electrons which show a large enhancement of the quasiparticle effective mass. The wavefunctions of the atomic and conduction electrons mix (hybridization), and the strong interaction of the quasi-free conduction-band electrons with nearly localized $`f`$ electrons leads to a so-called Abrikosov-Suhl resonance, i.e. an enhanced density of states at the Fermi energy.  The main idea of understanding this state of matter is the competition between Kondo and Ruderman-Kittel-Kasuya-Yosida (RKKY) interactions. The RKKY interaction leads to a magnetic ground state while the dominance of the Kondo interaction causes hybridization between localized $`f`$-electron states and delocalized conduction electrons. Due to the arrangement of the $`f`$ orbitals on a regular lattice, the hybridization with the itinerant states leads to the opening of a charge gap at the Fermi energy; hence if not fully developed at least a pseudogap should show up in the electronic excitation spectrum.

The common feature of the HF systems is the crossover from an incoherent state, where the scattering of the charge carriers on magnetic moments can be described in the frame of the single-particle Kondo model, to a many-body ground state (Kondo lattice) on cooling below the coherence temperature $`T^{}`$. Above $`T^{}`$ the optical conductivity exhibits a broad Drude behavior

$$\widehat{\sigma }(\omega )=\sigma _1(\omega )+i\sigma _2(\omega )=\frac{\sigma _{dc}}{1+i\omega \tau }$$
(1)
which characterizes normal metals; the dc conductivity is given by $`\sigma _{dc}=ne^2\tau /m`$ with $`n`$ the concentration of conduction electrons, $`e`$ and $`m`$ the electronic charge and mass, and $`1/\tau =\mathrm{\Gamma }`$ the scattering rate, which is typically a few hundred wavenumbers for usual metals. The area under the conductivity spectrum is the spectral weight:

$$\sigma _1(\omega )d\omega =\frac{\pi ne^2}{2m}=\frac{\omega _p^2}{8}$$
(2)
and determines the plasma frequency $`\omega _p=\sqrt{4\pi ne^2/m}`$.

Below the coherence temperature $`T^{}`$, however, the increase in the density of electronic states (DOS) at low energies is commonly described by the formation of a narrow Drude peak with a renormalized effective mass $`m^{}`$ and scattering rate $`\mathrm{\Gamma }^{}`$ of charge carriers:

$$\widehat{\sigma }(\omega )=\frac{(\omega _p^{})^2}{4\pi }\frac{1}{\mathrm{\Gamma }^{}+i\omega }.$$
(3)
Because $`m^{}\mathrm{\Gamma }^{}=m\mathrm{\Gamma }`$, the dc conductivity $`\sigma _{dc}=ne^2/(m^{}\mathrm{\Gamma }^{})`$ is not affected by the renormalization. The spectral weight $`\omega _p^2/8=\pi ne^2/(2m^{})`$, however, decreases as $`m^{}`$ increases; typically $`m^{}`$ can reach several hundred times the free electron mass $`m`$. The enhancement of the effective mass is connected to the hybridization of $`s`$ and $`f`$-orbitals which leads to a narrow band with a high DOS at the Fermi energy and to the strong coupling of the charge carriers to the local magnetic moments. In HF compounds which do not order magnetically, a scaling relation

$$\left(\frac{\mathrm{\Delta }}{T^{}}\right)^2=\frac{m^{}}{m}$$
(4)
between the hybridization gap $`\mathrm{\Delta }`$ and the enhancement of the effective mass $`m^{}/m`$ is found theoretically  and experimentally. With $`T^{}`$ in the order of 10 to 100 K the hybridization gap is normally observed in the far-infrared range of frequency.

The antiferromagnetic ordering reveals itself in rather different ways for the various HF compounds. For instance, UPt3 does not show any appreciable anomaly of the specific heat or resistivity at the Néel temperature $`T_N=5`$ K while in URu2Si2 and UPd2Al3 the transition into a magnetically ordered state is accompanied by clear anomalies of these quantities. However, URu2Si2 shows a remarkable resistivity increase at $`T_N`$, typical for a spin-density-wave (SDW) system, while in UPd2Al3 only a kink in the $`\rho (T)`$ due to freezing-out of the spin-flip-scattering is observed. This already indicates that in contrast to the former system with itinerant antiferromagnetism, UPd2Al3 is an antiferromagnet with localized spins. In both UPt3 and URu2Si2, but also in UCu5, the progressive development of a gap (or pseudogap) in the optical spectra is observed in connection with the ordering of the magnetic moments, whereas for UPd2Al3 no effect of magnetic ordering on the optical response at frequencies above 30 cm-1 has been detected in the first infrared investigations.

In the heavy fermion superconductor UPd2Al3, on which we want to focus in this paper, a maximum of the resistivity occurs at temperaturea around 80 K which is often related to the onset of coherence; the values cited for the coherence temperature $`T^{}`$ range from 20 K to 60 K depending on the experimental method used for determination. The magnetic susceptibility $`\chi (T)`$ shows appreciably different behaviors for field directions parallel and perpendicular to the hexagonal $`c`$-axis; in the $`ab`$-plane $`\chi (T)`$ is Curie-Weiss like above 40 K with a maximum at around 35 K. Below this temperature, AF correlations develop, and UPd2Al3 shows a metamagnetic behavior. When cooling down even further, a commensurate AF order develops below $`T_N=14`$ K; superconductivity finally sets in below 2 K. For $`2\mathrm{K}<T<14`$ K the specific heat shows a $`C/TT^2`$ dependence; the effective mass of the charge carriers is estimated as $`m^{}/m50`$.

In the superconducting state of UPd2Al3 two low-energy modes at 1.5 meV and 0.4 meV have been observed by inelastic neutron scattering experiments at $`𝐪=\frac{1}{2c}(0,0,1)`$; it was suggested that they are associated with magnetic excitons and superconductivity, respectively. An important feature of UPd2Al3 is that – compared with other HF antiferromagnets – it has a rather large magnetic moment (0.85 $`\mu _B`$) which is localized predominantly on the U-site. Based on this experimental evidence, it has been suggested that UPd2Al3 can be described as a local-moment magnet, and hence the magnetic ordering should have only a minor influence on the electronic DOS. However, theoretical calculations of the Fermi surface  as well as de Haas-van Alphen experiments  also indicate an itinerant character of $`5f`$-electrons, and therefore one can expect in UPd2Al3 to find appreciable correlations between electronic states and magnetic ordering. Besides the interesting interplay of magnetic ordering and superconductivity, these correlations make UPd2Al3 one of the most studied HF systems in recent years; they are the main subject of our investigation.

Optical experiments have in general proven to be sensitive to the formation of heavy quasiparticles; the relevant features show up at the lower end of the infrared spectral range which is commonly accessible. In order to extend our earlier investigations  to lower frequencies, in the present work we have carried out optical experiments on UPd2Al3 films in the spectral range from microwaves up to the far infrared. First results have partially been reported in Refs. .

## II Experimental Methods

The highly $`c`$-axis oriented, epitaxial thin ($`150`$ nm) film of UPd2Al3 was prepared on (111) oriented LaAlO3 substrate (thickness $`0.924`$ mm) by electron-beam co-evaporation of the constituent elements in a molecular-beam epitaxy system. The phase purity and structure of the film were investigated by X-ray and reflection high-energy electron diffraction. The high quality of the film is seen in dc resistivity data displayed in Fig. 1 which are in excellent agreement with measurements of bulk crystals. At $`T=300`$ K the resistivity is $`\rho =172\mu \mathrm{\Omega }`$cm, the residual resistivity ratio $`\rho _{300\mathrm{K}}/\rho _{2\mathrm{K}}=23`$, the Néel temperature $`T_N=14`$ K; our film shows a sharp superconducting transition at $`T_c=1.75`$ K.

For the measurements in the millimeter and sub-millimeter spectral range ($`501400`$ GHz, $`1.240`$ cm-1, $`0.25`$ meV) a coherent source spectrometer was employed  utilizing a set of different backward wave oscillators as monochromatic and continuously tunable sources. The spectrometer includes an interferometric setup in a Mach-Zehnder arrangement which allows for measuring both the amplitude $`T_F`$ and the phase $`\varphi _t`$ of the signal transmitted through the plane-parallel sample, which in our case is a film on a substrate. These two quantities are used to evaluate the complex refractive index $`\widehat{N}=n+ik`$ \[or alternatively the complex conductivity $`\widehat{\sigma }(\omega )`$\] of the film using Fresnel’s formulas for a two-layer system  without assuming any particular model. In general, the complex transmission coefficient $`\widehat{t}_{1234}=\sqrt{T_F}e^{i\varphi _t}`$ of a two-layer system (layers which we index with 2 and 3) separating two media (indices 1 and 4) is given by

$`\widehat{t}_{1234}=\widehat{t}_{12}\widehat{t}_{23}\widehat{t}_{34}\mathrm{exp}\left\{i(\delta _2+\delta _3)\right\}[1+\widehat{r}_{12}\widehat{r}_{23}\mathrm{exp}\left\{2i\delta _2\right\}`$ (5)
$`+\widehat{r}_{23}\widehat{r}_{34}\mathrm{exp}\left\{2i\delta _3\right\}+\widehat{r}_{12}\widehat{r}_{34}\mathrm{exp}\left\{2i(\delta _2+\delta _3)\right\}]^1`$ (6)
where the complex angles are $`\delta _2=\omega d_2(n_2+ik_2)/c`$ for the film and $`\delta _3=\omega d_3(n_3+ik_3)/c`$ for the substrate; $`c=3.010^{10}`$ cm/s is the velocity of light in vacuum. The transmission coefficients at each interface are evaluated by the standard equation $`\widehat{t}_{ij}=(\widehat{N}_i\widehat{N}_j)(\widehat{N}_i+\widehat{N}_j)^1`$; where $`\widehat{N}_1=\widehat{N}_4=1`$ correspond to vacuum. The optical parameters of the LaAlO3 substrate ($`n_3`$ and $`k_3`$) are determined beforehand by performing the experiments on a blank substrate. The large size of the sample (approximately $`10\times 10`$ mm2) allowed us to extend the measurements to very low frequencies, from $`\omega /(2\pi c)=40`$ cm-1 down to 1.15 cm-1.

For the infrared range and higher frequencies we used the reflectivity results obtained on bulk samples and published previously.

In addition, at the frequencies of 10, 24, and 34 GHz enclosed resonators were developed and the sample was measured by cavity perturbation technique. The cylindrical TE011 copper cavities – quality factors around 15 000 – were operated by Gunn diode oscillators with sufficient tuning range; two waveguides couple to the cavity by holes on the half height of the opposite side walls. A small slice of a sample (typically 3 $`\times `$ 3 mm2) was placed in the electrical field maximum. The transmitted power was detected by a diode, amplified and processed by fitting a Lorentzian in order to determine the central frequency $`f_0`$ and the width $`\mathrm{\Gamma }_0`$. From the shift in frequency $`\mathrm{\Delta }f`$ and change in width $`\mathrm{\Delta }\mathrm{\Gamma }`$ upon introduction of the sample, the surface resistance $`R_S`$ and the surface reactance $`X_S`$ which determine the surface impedance $`\widehat{Z}_S=R_S+iX_S`$ are calculated as follows:

$$R_S=Z_0\frac{\mathrm{\Delta }\mathrm{\Gamma }}{2f_0\zeta }\mathrm{and}X_S=Z_0\frac{\mathrm{\Delta }f}{f_0\zeta },$$
(7)
where $`Z_0=4\pi /c=4.1910^{10}`$ s/cm is the impedance of free space ($`Z_0=377\mathrm{\Omega }`$ in SI units). The resonator constant $`\zeta `$ can be calculated from the geometry of the cavity and the sample when the dielectric properties of the substrate are known. The complex conductivity $`\widehat{\sigma }`$ can be evaluated from the surface impedance using $`\widehat{Z}_S=Z_0\sqrt{\omega /4\pi i\widehat{\sigma }}`$, and the absorptivity $`A`$ (sometimes simply called the absorption) is given by the relation

$$A=1R=\frac{4R_S}{Z_0}\left(1+\frac{2R_S}{Z_0}+\frac{R_S^2+X_S^2}{Z_0^2}\right)^1,$$
(8)
where $`R`$ is the reflectivity. In the limit $`R_S,|X_S|Z_0`$, the last equation reduces to

$$A4R_S/Z_0.$$
(9)
While at 10 GHz the two components of the complex surface impedance could be measured and therefore both the conductivity and the dielectric constant were calculated, in our higher frequency experiments at 24 and 34 GHz – because of the large influence of the substrate – we were not able to determine the frequency shift accurately enough to evaluate the dielectric properties of the film; hence we only utilize the surface resistance $`R_S`$. By using Eq. (9), however, it was possible to combine these millimeter wave cavity data with all of the higher frequency optical data, i.e. the transmission results through the films obtained in the submillimeter wave range and the reflectivity  measured on bulk samples in the infrared, visible and ultraviolet spectral range. The reflection coefficient is a complex function $`\widehat{r}(\omega )=|r(\omega )|e^{i\varphi _r(\omega )}`$ with the measured bulk reflectivity $`R=|\widehat{r}|^2`$. In order to obtain the phase $`\varphi _r`$ we performed a Kramers-Kronig analysis on the reflectivity spectra:

$$\varphi _r(\omega )=\frac{\omega }{\pi }_0^{\mathrm{}}\frac{\mathrm{ln}[R(\omega ^{})]\mathrm{ln}[R(\omega )]}{\omega ^2(\omega ^{})^2}d\omega ^{},$$
(10)
where the $`\mathrm{ln}[R(\omega )]`$ term has been added to the standard form in order to remove the singularity at $`\omega ^{}=\omega `$. It has no effect on the integral because $`_0^{\mathrm{}}[\omega ^2(\omega ^{})^2]^1d\omega ^{}=0`$. Because this integral extends from zero to infinity, it is necessary to make suitable high and low frequency extrapolations to the measured reflectivity data. We have chosen to use a power law \[$`R(\omega )1/\omega ^4`$\] at high frequencies above $`10^6`$ cm-1 and a Hagen-Rubens extrapolation

$$R(\omega )=1\left(\frac{2\omega }{\pi \sigma _{\mathrm{dc}}}\right)^{1/2}$$
(11)
below 0.3 cm-1. From $`R(\omega )`$ and $`\varphi _r(\omega )`$ it is then possible to calculate the complex optical conductivity $`\widehat{\sigma }(\omega )`$.

## III Results and Analysis

### A Transmission Spectra

In Fig. 2 we present the low-frequency transmission spectra for the UPd2Al3 film on the substrate for two selected temperatures (100 K and 2 K); they already illustrate clearly our main finding. The fringes in the spectra are due to multi-reflection of the radiation within the plane-parallel substrate acting as a Fabry-Perot resonator for our monochromatic radiation. The frequency spacing between two peaks is mainly determined by the thickness and refractive index of the substrate; their amplitude (minima to maxima), however, is governed by the parameters of the film. At temperatures above 25 K, the transmission spectra basically do not change. For $`T20`$ K the overall transmission is found to be strongly reduced below $`10\mathrm{cm}^1`$ due to absorption within the film. At lower frequencies, $`\nu =\omega /(2\pi c)<3.5\mathrm{cm}^1`$, the transmitted signal increases again, indicating an absorption edge. It is worth to note, that our preliminary study of a 136 nm thick UPd2Al3 film showed the same features in the optical response.

This feature appears below the temperature where the magnetic susceptibility has a maximum – when the AF correlations develop. Therefore we checked whether the observed transmission minimum could be due to some magnetic absorption. We tried to fit the observed behavior by modelling the complex permeability $`\widehat{\mu }(\omega )`$ with a magnetic oscillator (Lorentzian):

$$\widehat{\mu }(\omega )=1+\frac{\mathrm{\Delta }\mu _1\omega _0^2}{\omega _0^2\omega ^2+i\omega \mathrm{\Gamma }}$$
(12)
where $`\omega _0`$ and $`\mathrm{\Gamma }`$ are the center frequency and the width of the oscillator, respectively, and $`\mathrm{\Delta }\mu \omega _0^2`$ denotes the spectral weight. Alternatively we can satisfactorily describe the transmission spectra by using a dielectric oscillator

$$\widehat{ϵ}(\omega )=ϵ_1(\omega )+iϵ_2(\omega )=1+\frac{\mathrm{\Delta }ϵ_1\omega _0^2}{\omega _0^2\omega ^2+i\omega \mathrm{\Gamma }}.$$
(13)
Here $`\mathrm{\Delta }ϵ_1\omega _0^2`$ describes the oscillator strength (spectral weight), $`\omega _0`$ and $`\mathrm{\Gamma }`$ denote the center frequency and the width of the harmonic oscillator. The results of the least-square fit of the transmitted signal using a Drude–Lorentz model in combination with a magnetic or with a dielectric oscillator are shown in the lower two panels of Fig. 2. The parameters of the magnetic oscillator are $`\mathrm{\Delta }\mu _1=1.001`$, $`\omega _0/(2\pi c)=5.45`$ cm-1, $`\mathrm{\Gamma }/(2\pi c)=4.08`$ cm-1; and for the dielectric oscillator we used accordingly $`\mathrm{\Delta }ϵ_1=\omega _p^2/\omega _0^2=2.1410^5`$, $`\omega _0/(2\pi c)=3.86`$ cm-1, $`\mathrm{\Gamma }/(2\pi c)=2.13`$ cm-1. One can immediately see that, no satisfactory fit is possible with a magnetic oscillator term. Second, the $`\mathrm{\Delta }\mu _1`$ value (which denotes the strength of the magnetic contribution) is much higher than expected from the static magnetic susceptibility measurements. Third, the frequency dependence of the transmission is only described satisfactorily using the dielectric model. Thus we conclude that the observed feature is not due to a pure magnetic excitation and proceed with the analysis of our data along the lines of the complex dielectric constant $`\widehat{ϵ}(\omega )=ϵ_1(\omega )+iϵ_2(\omega )`$, or complex conductivity $`\widehat{\sigma }=\widehat{ϵ}\omega /(4\pi i)`$, respectively.

### B Optical Conductivity

To discuss our findings on the temperature and frequency dependent transport in UPd2Al3, let us first turn back to Fig. 1. Below $`T_N`$ the temperature dependence of the dc resistivity of the film can be described using the expression for an antiferromagnet with an energy gap $`E_g^{}`$:

$$\rho (T)=\rho _0+aT^2+bT\left(1+\frac{2k_\mathrm{B}T}{E_g^{}}\right)\mathrm{exp}\left\{\frac{E_g^{}}{k_\mathrm{B}T}\right\}.$$
(14)
Here $`\rho _0`$ gives the residual resistivity and the second term describes the electron-electron scattering (Fermi liquid). A fit of the dc curve (dotted line in Fig. 1) by Eq. (14) yields the gap value $`E_g^{}=1.9`$ meV, which corresponds to the one reported in Ref. .

From early tunneling measurements on UPd2Al3 a rather large spin-gap energy up to 12.4 meV was first suggested. Using thin films of this compound, recent tunneling experiments in the superconducting and normal state clearly demonstrate that there remains a reduced DOS at zero-bias up the temperature range of 7 K with a gap value of 1.0 meV while the superconducting gap is at 0.235 meV. The existence of a gap in either the electronic DOS or in the magnon spectrum was opposed by Caspary et al.  and on grounds of infrared measurements by Degiorgi et al.  In the light of the low-energy measurements presented in this paper, the arguments will be reconsidered below.

The real parts of the low-frequency optical conductivity $`\sigma _1(\omega )`$ and of the dielectric constant $`ϵ_1(\omega )`$ of UPd2Al3 are plotted in Fig. 3 for some temperatures. Except for the dc conductivity on the left axis of the upper frame and the results of the microwave impedance measurements at 0.3 cm-1, all the data points plotted are obtained directly from the transmitted power and phase shift in our transmission experiments. Within our accuracy both quantities are frequency independent for $`T25`$ K, but show a strong dispersion for lower temperatures. In addition, the response of the Drude model \[Eq. (3)\] is shown (solid line) which matches the dc conductivity $`\sigma _{dc}=1.2810^5(\mathrm{\Omega }\mathrm{cm})^1`$ at 2 K and the far-infrared roll-off around 10 cm-1; it is obvious that the observed optical response of UPd2Al3 differs from that of a renormalized Drude metal. As a result, the simple Hagen-Rubens extrapolation – in general used  to extrapolate the far-infrared reflectivity below 30 cm-1 – totally misses the following two features in our millimeter and sub-millimeter range. First, the optical conductivity $`\sigma _1(\omega )`$ clearly shows the development of a gap-like minimum below 3 cm-1 at $`T<20`$ K; it corresponds to a pronounced increase of the dielectric constant $`ϵ_1(\omega )`$ which is a direct measure of the gap. This feature gradually disappears with increasing temperature and is not seen above 30 K. Second, at frequencies below approximately 1.5 cm-1 the conductivity increases for $`\omega 0`$ towards considerably higher dc values leading to a very narrow peak at zero frequency.

In a first approach we describe the narrow peak at $`\omega =0`$ by the Drude model and use a phenomenological gap model  for the higher frequencies:

$`\sigma _1(\omega )={\displaystyle \frac{\sigma _{dc}(\mathrm{\Gamma }_D^{})^2}{\omega ^2+(\mathrm{\Gamma }_D^{})^2}}+(1\mathrm{\Theta }){\displaystyle \frac{\mathrm{\Sigma }_g}{\omega ^2+\mathrm{\Gamma }_g^2}}\sqrt{\omega \omega _g}`$ (15)
where $`\mathrm{\Theta }=1`$ for $`\omega \omega _g`$ and $`\mathrm{\Theta }=0`$ above the gap frequency $`\omega _g`$. Here $`\mathrm{\Gamma }_D^{}`$ is the damping of the narrow $`\omega =0`$ mode and $`E_g=\mathrm{}\omega _g`$ corresponds to the gap energy. The parameters $`\mathrm{\Sigma }_g`$ and $`\mathrm{\Gamma }_g`$ depend on the concentration, the effective mass, and the scattering rate of the charge carriers above the gap. By performing a Kramers-Kronig integration of Eq. (15) we have also obtained an analytical expression for the dielectric constant which was used in the fitting procedures. The assumed model (15) describes very well the experimental results of $`\sigma _1(\omega )`$ and $`ϵ_1(\omega )`$ for temperatures $`T20`$ K; as an example, the fit of the 2 K data is shown in Fig. 4. The temperature dependence of the gap energy $`\mathrm{}\omega _g`$ as obtained by this fit is displayed in the inset (solid squares corresponding to the left axis). The gap value $`E_g0.22`$ meV is essentially temperature independent, which does not correspond to the well-known BCS-like temperature behavior obtained by mean-field theory; instead, the gap feature becomes more and more pronounced as the temperature is lowered.

While the above analysis was solely based on direct measurements of the optical conductivity and dielectric constant without applying the Kramers-Kronig analysis, we now want to combine all the absorption data available in the entire range of frequency. In Fig. 5a the frequency dependence of the absorptivity $`A(\omega )=1R(\omega )`$ is plotted over a wide spectral range and for different temperatures. From the measured dc conductivity the absorptivity is calculated in the Hagen-Rubens limit assuming Eq. (11). The full symbols are the results of the microwave cavity measurements of the surface resistance $`R_S`$, using Eq. (9). In the range from 1 cm-1 to 40 cm-1, the absorptivity is evaluated from our optical experiments using the transmission coefficient and the phase shift (open circles; only 2 K data are plotted for clarity reasons). Above 30 cm-1 up to $`10^6\mathrm{cm}^1`$ we also utilized the data from bulk reflectivity measurements (solid lines) published previously. For even higher frequencies we extrapolated by $`R(\omega )\omega ^4`$. The lines represent the input we used for performing the Kramers-Kronig analysis in order to calculate the optical conductivity. It was obtained by simultaneously fitting the absorptivity results and the directly measured conductivity. Obviously, the low-temperature data exhibit significant deviations from the $`A(\omega )\omega ^{1/2}`$ Hagen-Rubens behavior for frequency above 0.1 cm-1.

The lower panel of Fig. 5 shows the corresponding optical conductivity $`\sigma _1(\omega )`$ as obtained by a Kramers-Kronig analysis of the absorptivity just described; in addition we again display the directly measured conductivity data which were also taken into account for the absorptivity fit, as mentioned above. The agreement is very good considering the error bars for each measurement technique. The main features can be summarized as follows: (i) At high temperatures $`T>50`$ K, we observe a broad conductivity spectrum as expected for a metal according to Eq. (1). Following Ref. , the plasma frequency from the evaluation of the entire spectral weight of all free charge carriers is $`\omega _p/(2\pi c)=4.410^4\mathrm{cm}^1`$. (ii) As the temperature decreases below $`T^{}`$, a renormalized Drude peak \[Eq. (3)\] develops due to the gradual enhancement of the effective mass $`m^{}`$. The renormalized plasma frequency $`\omega _p^{}/(2\pi c)`$ 4350 cm-1, which will be obtained by the procedure discussed in Subsection III C, corresponds to $`m^{}100m`$. This behavior is typical for heavy fermions  and was discussed in detail by Degiorgi, Dressel and coworkers  for the case of UPd2Al3. At the same time, a gap-like feature develops around 100 cm-1 as expected from the hybridization of the localized $`5f`$ electrons and the conduction electrons; this value is in good agreement with the scaling relation (4). (iii) Lowering the temperature further, magnetic ordering sets in at $`T_N=14`$ K and leads to distinct signatures in the optical spectrum. We observe a well pronounced pseudogap below 2 cm-1 which we assign to magnetic correlations between the localized and delocalized charge carriers. At even lower frequencies, an extremely narrow mode centered zero-frequency remains which is eventually responsible for superconductivity below $`T_c=2`$ K. The analysis and understanding of this low-temperature ($`T_c<TT_N`$) and low-frequency ($`\nu <50`$ cm-1) behavior is the main point of this paper.

For the analysis of our low-frequency data we introduce a complex frequency dependent scattering rate $`\widehat{\mathrm{\Gamma }}(\omega )=\mathrm{\Gamma }_1(\omega )+i\mathrm{\Gamma }_2(\omega )`$ into the standard Drude form of Eq. (3). If we define the dimensionless quantity $`\lambda (\omega )=\mathrm{\Gamma }_2(\omega )/\omega `$, the complex conductivity can be written as

$$\widehat{\sigma }(\omega )=\frac{(\omega _p^{})^2}{4\pi }\frac{1}{\mathrm{\Gamma }_1(\omega )i\omega (m^{}(\omega )/m)}$$
(16)
where $`m^{}/m=1+\lambda (\omega )`$ is the frequency dependent enhanced mass. $`\omega _p^{}/(2\pi c)=9.510^3\mathrm{cm}^1`$ corresponds to the fraction of electrons which participate in the many body state which develops below $`T^{}`$ as discussed in the following subsection. By rearranging Eq. (16) we can write expressions for $`\mathrm{\Gamma }_1(\omega )`$ and $`m^{}(\omega )`$ in terms of $`\sigma _1(\omega )`$ and $`\sigma _2(\omega )`$ as follows:

$$\mathrm{\Gamma }_1(\omega )=\frac{(\omega _p^{})^2}{4\pi }\frac{\sigma _1(\omega )}{|\widehat{\sigma }(\omega )|^2}$$
(17)
$$\frac{m^{}(\omega )}{m}=\frac{(\omega _p^{})^2}{4\pi }\frac{\sigma _2(\omega )}{|\widehat{\sigma }(\omega )|^2}\frac{1}{\omega }.$$
(18)
Due to causality,  $`\mathrm{\Gamma }_1(\omega )`$ and $`m^{}(\omega )`$ are related through the Kramers-Kronig integrals.  Such analysis allows us to look for interactions which would lead to energy dependent renormalization effects as the frequency dependent scattering rate and effective mass are related to the real and imaginary parts of the frequency dependent self-energy of the electrons. Such analysis has been used before in studying the response of HF compounds  and high temperature superconductors.  In the lower frames of Fig. 6 the frequency dependence of the scattering rate $`\mathrm{\Gamma }_1(\omega )`$ and of the effective mass $`m^{}(\omega )`$ are displayed for different temperatures; for comparison we plot $`\sigma _1(\omega )`$ and $`ϵ_1(\omega )`$ in Fig. 6a and b. As expected for a Drude metal, at $`T>T^{}`$ the spectra of $`\mathrm{\Gamma }_1(\omega )`$ and $`m^{}(\omega )`$ are nearly frequency independent. As the temperature is lowered we observe a peak in the energy dependent scattering rate at the hybridization gap, as can be nicely seen in the $`T=30`$ K data of Fig. 6c. The existence of HF quasi-particles is confirmed by a low-frequency plasmon characterized by the zero-crossing in the spectra of the dielectric constant $`ϵ_1(\omega )`$ shown in Fig. 6b. The decrease of $`\mathrm{\Gamma }_1(\omega )`$ to lower frequencies corresponds to an increase of $`m^{}(\omega )`$. At these intermediate temperatures, $`T_N<T<T^{}`$, the effective mass $`m^{}/m`$ already reaches a value of 35.

The question remains how the optical response at very low frequencies can be described, i.e. for excitations of the zero-frequency mode; whether it is simply a renormalized Drude behavior. The Landau Fermi-liquid theory  predicts that the scattering rate due to electron–electron interactions in three dimensions should be quadratic both in temperature and frequency.  In order to examine the shape of the zero-frequency peak observed in the data, we have adopted the following phenomenological forms of $`\mathrm{\Gamma }_1(\omega )`$ and $`m^{}(\omega )`$, used by Sulewski et al. in their study of the Fermi liquid behavior of the heavy fermion compound UPt3:

$$\mathrm{\Gamma }_1(\omega )=\mathrm{\Gamma }_0+\frac{\lambda _0\alpha \omega ^2}{1+\alpha ^2\omega ^2}$$
(19)
and

$$\frac{m^{}(\omega )}{m}=1+\frac{\lambda _0}{1+\alpha ^2\omega ^2},$$
(20)
where $`\mathrm{\Gamma }_0`$ and $`\lambda _0`$ are the zero-frequency scattering rate and mass enhancement, respectively. $`1/\alpha `$ is a characteristic frequency (energy) of the process. These expressions obey the Kramers-Kronig relation and have the proper Fermi-liquid frequency dependence. The comparison of the low-frequency behavior of $`\mathrm{\Gamma }_1(\omega )`$ at $`T=30`$ K to the fit by Eq. (19) (inset of Fig. 6) confirms the main features: as the frequency increases, $`\mathrm{\Gamma }_1(\omega )`$ grows and then saturates around 100 cm-1. The present set of data, however, does not allow to conclude whether UPd2Al3 can be satisfactorily described within a Fermi-liquid formalism or not. These questions remain the subject of further investigations at lower frequencies.

The scattering rate drops more than one order of magnitude below 15 K. This can be explained by the freezing-out of spin-flip scattering below $`T_N`$. As was recently pointed out  in the context of high temperature superconductors, the energy dependent scattering rate is related to the electronic DOS. In fact, a sum-rule was suggested similar to Eq. (2). In the case of UPd2Al3 we can distinguish two gap structures with an enhanced DOS at the edges, as it is known from superconductors and low-dimensional semiconductors. Again, it would be of great interest to determine $`\mathrm{\Gamma }_1(\omega )`$ of this narrow zero-frequency mode which remains in the AF state. Due to the influence of magnetic correlations it might be well distinct from the behavior at $`T>T_N`$ plotted in the inset of Fig. 6. The related experiments are currently in progress.

Decreasing the temperature below $`T_N`$ results in a second peak of $`\mathrm{\Gamma }_1(\omega )`$ and a strong increase of the effective mass around 1 cm-1. Already seen at $`T=15`$ K, this effect becomes stronger as the temperature is lowered to 2 K. The effective mass $`m^{}/m`$ levels off below this frequency and nicely matches the values obtained by thermodynamic methods  which are indicated by the point at $`\omega =0`$ in Fig. 6d. Note, that due to the few data points, the features below 1 cm-1 are not significant; this range demands further studies. The important finding of our study is, that the magnetic ordering significantly changes the energy dependence $`m^{}(\omega )`$: the strong increase of the effective mass does not occur at the hybridization gap at 10 meV, but mainly below the energy range which corresponds to the correlation gap at 0.2 meV. This infers that the magnetic correlations are of superior importance for the mass enhancement.

### C Spectral Weight

According to Eq. (2), the area under the conductivity spectrum is related to the density and the mass of the charge carriers. Well above the coherence temperature $`T^{}`$, optical spectra of UPd2Al3 simply follow the Drude behavior of a normal metal with an unrenormalized plasma frequency of $`\omega _p/(2\pi c)=4.410^4\mathrm{cm}^1`$ as evaluated previously. Assuming $`m=m`$, the free electron mass, we estimate a charge carrier density $`n=1.110^{22}\mathrm{cm}^3`$. From experimental  and calculated  de Haas–van Alphen spectra we know that only approximately 35 % of the electrons contribute to the HF state; qualitatively we observe this fact also in our optical spectra. The plasma frequency which corresponds to those electrons (concentration $`n^{}`$) which are affected by the formation of the HF state  is $`\omega _p^{}/(2\pi c)=9.510^3`$ cm-1. Our analysis further infers that these carriers have a band mass $`m^{}=7m`$. This also means, that a large fraction of the carriers is unaffected by the HF ground state and will not be considered in our further analysis.

Typical for a HF compound, below 100 cm-1 a narrow conductivity mode develops due to electronic correlations at lower temperatures. For $`T>20`$ K but below $`T^{}`$, the spectral weight of this contribution does not change significantly; the renormalized plasma frequency is $`\omega _p^{}/(2\pi c)4350`$ cm-1. A similar result of a temperature independent $`\omega _p^{}`$ was obtained from our fit of the directly measured conductivity as displayed in the inset of the Fig. 4 by the open diamonds.

Assuming that the total number of charge carriers $`n^{}`$ remains unchanged, sum-rule arguments give $`\omega _p^{}/\omega _p^{}=\sqrt{m^{}/m^{}}`$. Thus we obtain $`m^{}/m30`$ which is in good agreement with the value obtained by thermodynamic methods of specific heat and susceptibility ($`m^{}/m=4166`$)  and is somewhat smaller than the estimate from infrared measurements ($`m^{}/m=85`$). Analyzing our data by the generalized Drude model (16), we have obtained the energy dependence of the effective mass as plotted in Fig. 6d. For $`T=2`$ K we find an enhancement of $`m^{}(\omega )/m=45`$, in excellent agreement with the above estimates of the spectral weight.

As the temperature decreases below $`T_N`$, a pseudogap develops in the optical spectra around 1.8 cm-1 (i.e. 0.2 meV) with important implications on the spectral weight. At low temperatures the optical weight consists of two contributions, the narrow $`\omega `$=0 centered resonance and the charge carriers excited across the gap of energy $`\mathrm{}\omega _g`$

$$_0^{\omega _c}\sigma _1(\omega )d\omega =_0^{\omega _g}\sigma _1(\omega )d\omega +_{\omega _g}^{\omega _c}\sigma _1(\omega )d\omega .$$
(21)
Here we integrated up to a cut-off frequency $`\omega _c/(2\pi c)100`$ cm-1 which lies above the features associated to correlation effects but well below the interband transitions. The zero-frequency response contains only 10% of the overall spectral weight, the major contribution comes from the excitations across the gap. This agrees well with the above discussion of the peak in the DOS right above the gap. The temperature dependences of both components as well as their sum are presented in the inset of Fig. 4 (right axis). The contribution of the $`\omega =0`$ response increases as the temperature decreases (open triangles in inset of Fig. 4); within our accuracy, this however, does not lead to a significant change of the overall spectral weight with temperature (open diamonds). The observed behavior can be taken as an indication that these two modes correspond to charge carriers localized at different parts of the Fermi surface. The coexistence of two different electronic subsystems in UPd2Al3 has also been suggested in Ref..

The most interesting question is the relation between the AF ordering and the pseudogap origin. The fact that we also see the gap-like feature slightly above $`T_\mathrm{N}`$ up to 20 K or more does not rule out its connection to the magnetic ordering since an incommensurate phase was also observed up to $`T20`$ K by neutron diffraction experiments.

## IV Discussion

Since the development of the HF state in UPd2Al3 and the corresponding hybridization gap, which we observe around 100 cm-1, was already discussed in Ref.  extensively, we concentrate now on the newly discovered feature at lower energies. Four possible explanations for the origin of the correlation gap at 0.2 meV will be considered: (i) the pseudogap in the optical response may be related to spin-wave excitations, (ii) the formation of a SDW ground state may lead to the opening of an energy gap, (iii) due to interaction the hybridization gap is shifted to low energies, and (iv) magnetic correlations in the AF ground state influence the electronic DOS spectra.

(i) From torque magnetization measurements Süllow et al.  found evidence of a gap in the spin-wave spectrum of the order of $`E_g0.4`$ meV, which is about the value of the pseudogap we see in the optical spectra. For $`T>T_c=2`$ K inelastic neutron scattering experiments found a Lorentzian-shaped line around 1.5 meV which is ascribed to magnetic excitations.  Another gap observed at 0.4 meV was associated with superconductivity. All of these modes exhibit a strong temperature and q-dependence.  Besides the resistivity $`\rho (T)`$ discussed above, the fall of $`C(T)`$ was also interpreted as the opening of a gap in the magnetic excitation spectrum.  Typically magnetic excitations, however, lead to a much smaller response in the optical properties. As it was shown above in Sec. III A, we were not able to obtain a reasonable fit of the observed features by a magnetic absorption process (cf. Fig. 2). Moreover, in our preliminary experiments in magnetic field  we have not seen any clear evidence in favor of the magnetic nature of the observed gap feature. We also think that the dielectric constant $`ϵ_1(\omega )`$ would show a stronger influence of the magnetic field if the features were related to an AF resonance; in particular the frequency of the excitation would shift.

(ii) Below $`T_N`$ a commensurate ordering of the rather large magnetic moments (0.85 $`\mu _B`$) occurs in UPd2Al3; also in the HF antiferromagnet URu2Si2 a commensurate structure develops but the ordered moment only amounts to 0.02 $`\mu _B`$. Soon after the discovery of UPd2Al3 it was debated whether also in this compound the antiferromagnetic ordering is due to the SDW ground state like in URu2Si2. In contrast to URu2Si2, the resistivity of UPd2Al3 does not increase right below $`T_N`$, but the low temperature decrease can be well described by an activated behavior \[Eq. (14)\]. We do not think that the so-obtained gap value $`E_g`$=1.9 meV indicates the formation of a SDW state ; it is much larger than the value obtained from our optical results (Fig. 4). The pseudogap feature we see in UPd2Al3 is not as clearly developed as the energy gap in URu2Si2 or UCu5  and about a factor of five below the frequency one would expect from mean-field theory $`E_g=3.5k_BT_N`$. The opening of a SDW gap can be seen in the temperature dependent NMR relaxation rate of URu2Si2  yielding a reduction of the electronic density of states by a factor of three. A very similar behavior has been detected by 27Al-NQR experiments  in UPd2Al3. Indications for a SDW behavior in isostructural UNi2Al3 have been reported by Y. Dalichaouch et al.  and by Uemura et al.  Recent 105Pd-NMR and NQR experiments, however, speak against the SDW model for the UPd2Al3; the observed divergence in $`1/T_1`$ at $`T_N`$ can be explained by a localized moment picture of uranium.

(iii) Another possible mechanism of the pseudogap formation at these low energies is the change of the electronic DOS due to the coherence of screening conduction electrons in the Kondo lattice (so-called hybridization gap ). The coherence temperature $`T^{}`$ is usually of the same order of magnitude as the single particle Kondo temperature $`T_K`$,  below which local moments are screened and a local Fermi-liquid picture applies. According to different experiments,  the coherence temperature of UPd2Al3 lies in the range from 20 K to 60 K, i.e. the hybridization gap should be approximately 1.9 to 5 meV. This is in excellent agreement with the 100 cm-1 gap (124 meV) we observe and hence assign to the hybridization gap following Eq. (4). However, there might be scenarios which also relate the low-frequency gap at 0.2 meV to the hybridization:
(a) The strong anisotropy in UPd2Al3 may lead to an anisotropic hybridization gap, and optical measurements see an “effective” value, which can be lower than the single-particle Kondo coupling energy. We want to recall a similar discussion for high-temperature superconductors where a complicated gap symmetry is made responsible for ‘states in the gap’ and a distinct optical response.  However, such a situation is only realized for $`f^1`$ or $`f^3`$ configurations of the U-ions, due to the absence of the Kondo screening for $`f^2`$ state. On the other side many experiments indicate U4+ oxidation state ($`f^2`$-configuration) in UPd2Al3,  but the electronic configuration of the U is not determined unambiguously.
(b) By means of analytical and numerical calculations  the ratio $`T_K/T^{}`$ should be less than unity in case of a low density of screening electron (exhausting regime). It leads to a decrease of the coherence temperature $`T^{}`$, which is a measure of the hybridization gap. In this case our Kondo-system would have single-particle excitations with an energy of the order $`k_BT_K`$1.9 meV \[it corresponds to the energy of the mode (1.5 meV), observed in the inelastic neutron scattering experiments \] and a collective resonance in the heavy particle assembly with about ten times lower energy. In favor of this hypothesis speaks the high magnetic moment of U (low concentration of the screening electrons) and also the fact that we observe the pseudogap up to $`T20`$ K: as the numerical calculations in the periodic Anderson model indicate, the Kondo resonance in the exhausting regime shows a much weaker temperature dependence and can be seen up to temperature $`T10T^{}`$, in full agreement with our experimental observation.

(iv) The itinerant antiferromagnetism of a SDW is at odds with the formation of local moment magnetism deduced from susceptibility  and neutron scattering. On the other hand, using self-consistent density functional calculations in the local approximation the magnetic structure and the size of the ordered moment of UPd2Al3 have been well described within a purely itinerant electron picture. It was suggested  that two different electronic subsystems coexist in UPd2Al3. One of them is a rather localized uranium $`5f`$ state responsible for the magnetic properties, the other is delocalized and determines the heavy fermion and superconducting properties. From the London penetration depth  $`\lambda _L(0)`$=450 nm we calculate  the plasma frequency of the superconducting carriers $`(2\pi \lambda _L(0))^1=3540`$ cm-1 and find a good agreement with $`\omega _p^{}/(2\pi c)=4350`$ cm-1 obtained from the spectral weight of our low-frequency conductivity spectrum just above $`T_c`$ (cf. inset of Fig.4). This has the following implications:
(a) In order to recover the spectral weight $`\rho ^s`$ of the $`\delta `$-peak in the superconducting state (as determined from the penetration depth) according to the Tinkham-Ferrell sum rule,  we have to integrate the normal state conductivity $`\sigma _1^n(\omega )`$ up to a cut-off frequency $`\omega _c^s/(2\pi c)=100\mathrm{cm}^1`$ (assuming that the conductivity decreases to zero up to this frequency) which is well above the frequency $`2\mathrm{\Delta }/(hc)=4\mathrm{cm}^1`$ at which the superconducting gap was observed by tunneling spectroscopy. In conventional superconductors a change in the optical properties upon entering the superconducting state can be observed only up to approximately three times the gap frequency. A similar discrepancy of spectral weight was found in high-temperature superconductors  and gave argument to a change of the kinetic energy $`\mathrm{\Delta }K`$ associated with the superconducting transition:

$$\rho ^s=_{0+}^{\omega _c^s}\left[\sigma _1^n(\omega )\sigma _1^s(\omega )\right]d\omega +\mathrm{\Delta }K.$$
(22)
Our results indicate that also for UPd2Al3 there is a loss of kinetic energy in the superconducting state. Since we were not yet able to probe the superconducting state and determine the superconducting gap by optical means, we do not want to further speculate on the violation of the Tinkham-Ferrell sum rule and possible implications.
(b) All electrons seen in our low-energy spectra are in the HF ground state and eventually undergo the superconducting transition below $`T_c`$. We can definitely rule out an assignment of the gap to the localized carriers of the AF ordered states with the delocalized carriers contributing only to the narrow feature around $`\omega =0`$ because with a plasma frequency of 1500 cm-1 at low temperatures, this feature contains only 18 % of the carriers which become superconducting. The small spectral weight below the correlation gap implies that the excitations above the gap stem from the delocalized states and that the pseudogap observed in our conductivity spectra is either inherent to the heavy-quasiparticle state or it is related to exchange correlations of the second subsystem.

Recently Sato et al.  argued that the magnetic excitations seen by neutron scattering produce effective interactions between itinerant electrons, and therefore are responsible for superconductivity. Similar conclusions where drawn from tunneling measurements on UPd2Al3 films. Our results now indicate that already in the normal state electronic and magnetic excitations interact in the energy range which is relevant for superconductivity in UPd2Al3. From the frequency dependence of the effective mass $`m^{}(\omega )`$ we can conclude that also the mass enhancement in the metallic state is strongly influenced by the magnetic correlations. Thus as magnetic excitons are supposed to be responsible for the superconductivity , we suggest that the localized magnetic excitations also influence the properties of the normal state which were commonly assigned to the heavy-fermion ground state. We propose that the magnetic order in these compounds is the pre-requisite to the formation of the heavy quasiparticles and eventually of superconductivity.

It is expected that the temperature dependence of the quasiparticle formation, as observed in the enhancement of the effective mass, goes hand in hand with the energy dependence of the correlation effects, as probed by the f requency dependence of $`m^{}`$; however, only very few experiments on heavy fermion systems have been performed in this regard. From Fig. 6d we see a moderate enhancement of $`m^{}(\omega ,T=0)`$ for frequencies below the hybridization gap and a larger one below the gap due to magnetic correlations. Accordingly, $`m^{}(\omega =0,T)`$ increases only slightly below $`T^{}`$ and shows a large enhancement below $`T_N`$. The latter behavior should also be observed in thermodynamic measurements of $`m^{}`$.

## V Outlook

If our explanation the optical properties of UPd2Al3 is valid, it may also apply to other heavy fermion compounds, in particular to UPt3 which exhibits a similar behavior in many regards . For UPt3 the effective mass of the quasiparticles is larger ($`m^{}/m200`$) and the relevant energy scales are lower. The coherence temperature $`T^{}30`$ K, fluctuating short-range magnetic order occurs at $`T_N=5`$ K, and superconductivity sets in at $`T_c=0.5`$ K.  Although the magnetic moment ($`0.02\mu _B`$) is much smaller, recent bandstructure calculations  infer the existence of localized as well as delocalized $`5f`$-electrons in UPt3 very much similar to UPd2Al3. It was suggested that the observed enhancement of the quasiparticle mass results from the local exchange interaction of two localized $`5f`$-electrons with the remaining delocalized ones.

Millimeter wave experiments on UPt3 crystals  which show a peak in the conductivity at 6 cm-1 for temperatures below 5 K indicate a similar scenario. We reanalyzed the optical properties of UPt3 shown in Fig. 7a in the same way as described above (Sec. III B) and obtain similar features.  When the coherent ground state builds up ($`T<T^{}`$), the optical conductivity increases for frequencies below 30 cm-1 (Fig. 7b). As the temperature drops below $`T_N=5`$ K, magnetic ordering occurs and an energy gap progressively develops at about $`3\mathrm{cm}^1`$ which is assigned to magnetic correlations.  In full analogy to the case of UPd2Al3, the frequency dependence of the effective mass of UPt3 displayed in Fig. 7d clearly shows that only a marginal increase of $`m^{}`$ is observed around 30 cm-1, while below the energies related to the magnetic correlations the mass is drastically enhanced. Thus for UPt3 we also find that, as for UPd2Al3, the coupling of the localized and delocalized $`5f`$-electrons causes the heavy quasiparticles in UPt3; these magnetic excitations are very likely to be responsible for superconductivity. More detailed electrodynamic studies on UPt3 and on the superconducting state in general have to be performed since they seem to be the appropriate method to probe the energy dependence of the correlation effects which are the key issue for understanding the nature of the heavy quasiparticles. It remains to be seen how far our findings have implications on non-magnetic heavy fermions with a large effective mass. Of further interest would be the study of Ce compounds for which comparable band structure calculations do not yet exist.

## VI Conclusion

In conclusion, the electrodynamic response of UPd2Al3 in the low-energy range from 0.04 meV to 5 meV (0.33 cm-1 to 40 cm-1) exhibits a behavior at low temperatures ($`T20K`$) which cannot be explained within the simple picture of a renormalized Fermi liquid. At around 12 meV a hybridization gap develops below $`T^{}`$ which is characteristic for heavy fermions. The lower-frequency response shows the well-known renormalized behavior only above the magnetic ordering; below $`T_N=14`$ K, however, additional features were discovered. Besides an extremely narrow (less than 1 cm-1) zero-frequency response, we observe a pseudogap of about 0.22 meV. The experiments yield indications that this pseudogap is not a simple SDW gap or some excitation in the local magnetic moments system, but rather is connected to magnetic correlations on the delocalized charge carriers. We have argued, that this gap at extremely low energies is due to the influence of the localized magnetic moments on the itinerant electrons and this interaction is mainly responsible for the enhanced mass $`m^{}`$. It appears that the formation of the heavy quasiparticles relies on the establishment of antiferromagnetic order rather than competition of the coherent singlet formation and the magnetic order.

###### Acknowledgements.

We acknowledge helpful discussions of our findings with F. Andres, A.A. Dolgov, A.V. Goltsev, G. Grüner, A. Muramatsu, A. Schwartz, F. Steglich, and G. Zwicknagl. We thank D.N. Basov for his attempt on the low-temperature measurements. The work was partially supported by the Deutsche Forschungsgemeinschaft (DFG) via Dr228/9 and SFB 252.


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# Ubiquitous column density variability in Seyfert 2 Galaxies

## 1 Introduction

Strong obscuration is observed in the hard (2-10 keV) X-ray spectra of Type 2 Active Galactic Nuclei, where a photoelectric cut-off at energies E $`>`$ 1-2 keV indicates the presence of a column density of absorbing gas N$`{}_{H}{}^{}>10^{22}`$ cm-2.

The simplest geometry for this gas surrounding the nucleus is that of a torus covering $``$ 80% of the solid angle (in order to reproduce the 4:1 observed ratio between unobscured and obscured AGN, Maiolino & Rieke 1995). One of the unsolved questions about this putative torus is its typical dimensions. Detailed models have been proposed for both a 100 pc-scale torus (Granato et al. 1997) and for a parsec-scale one (Pier & Krolik 1992). Both models are supported by observational evidence, so it is likely that both the components could be present in AGN. Here we investigate the variability of the X-ray absorbing column density in X-ray defined Seyfert 2s having column densities higher than $`10^{22}`$ cm-2, but less than 1024 cm-2 (in order to have a measurement of the photoelectric cut-off in the 2-10 keV band). We collected all the data available in the literature for Seyfert 2s and we complemented them with the analysis of unpublished data in the ASCA and BeppoSAX public archives. In the following Sections we show the results and we show that they can be explained within a consistent physical picture only assuming that the absorber is located at a distance from the center typical of the Broad Emission Line Region (BELR).

## 2 Results

We found that a sample of 25 sources were observed at least twice in the hard X-rays. Out of these 25 sources, 22 show NH variability on timescales from a few months to years (Fig. 1).

The full detailed analysis of the 139 observations of these 25 sources is described in Risaliti et al. 2001.

There are two physical reasons that can explain the variability of the absorbing column density: variation in the ionization state of the absorber, due to variations in the ionizing continuum, and variations of the amount of gas along the line of sight. We ruled out the first possibility, since the NH variations are not correlated with the flux variations (see Risaliti et al. 2001 for details). The second scenario -motions in a clumpy medium- is the only one that can account for the observations.

However, the results on the ubiquity of NH variability in Seyfert 2s, together with the short (from 2 months to a few years) variability timescales, pose severe problems for the standard torus model. We can idealize the situation by assuming the typical timescale of variation, $`t`$, to be the crossing time of a discrete cloud across the line of sight. Assuming that the absorption is due to spherical clouds moving with Keplerian velocities, the distance from the central black hole of mass $`M_{}`$ is given by:

$$R3\times 10^{16}\frac{M_{}}{10^9M_{}}(\frac{\rho }{10^6\mathrm{cm}^3})^2(\frac{t}{5\mathrm{Msec}})^2(\frac{N_H}{10^{22}\mathrm{cm}^2})^2\mathrm{cm}$$
(1)
where $`\rho `$ is the density of the cloud. The black hole mass and the cloud density have been normalized to extreme values for a putative torus in order to obtain the greatest distance.

The distance we obtained is typical for the BELR. Even if many parameters are poorly constrained, it is not possible to obtain a value of $`R>10^{18}`$ cm within a consistent physical scenario. Therefore, the parsec-scale torus model is not able to explain our data. An alternative scenario, within the standard AGN model (Antonucci 1993), is that the X-ray absorber is located in the BELR, much nearer to the central black hole than the standard torus. If we assume that the broad line clouds are responsible for the absorption in the X-rays, we can find a consistent combination of the parameters in the previous equations, with higher cloud densities ($`\rho 10^9cm^3`$) and shorter variability timescales ($`t3`$ days). We note that such timescales are not ruled out by our data, since we cannot investigate variations shorter than the time interval between two observations of the same source.

An absorber which is very compact (as required by our data) and axisymmetric (as required by the arguments supporting the unified schemes) can be easily obtained by extending the wind model by Elvis (2000, and these proceedings). In this model most of the phenomenology of type 1 AGNs is explained through a two-phase wind arising from the accretion disc. The cold phase of the wind is formed by the Broad Emission Line Clouds (BELC). A simple extension of this model could be that in type 2 AGNs the wind is thicker, and the BELC cover all lines of sight through the wind, as illustrated in Fig. 2. The external part of the wind can well be cold enough for dust to survive, therefore this absorber can also explain the optical properties of Seyfert 2s. Interestingly, the average dust-to-gas ratio predicted by this model, assuming that the external part of the wind has a standard ISM composition, is lower than Galactic, in agreement with recent findings (Maiolino et al. 2001, Risaliti et al. 2001)

## 3 Conclusions, and future work

Variability of X-ray absorbing column density appears to be an ubiquitous property in Seyfert 2 galaxies. Variation timescales can be as short as a few months. We have shown that these data rule out an X-ray absorber on a parsec scale. Instead, we propose that the Broad Emission Line Clouds, in an axisymmetric distribution, like in the model of Elvis (2000) are responsible for X-ray absorption. If this is the case, variations in NH are expected on timescales of days. Our variability study is limited by the shortest time between two observations of the same source. However, our work can be significantly improved looking for NH variations inside single, long observations of the brightest sources in our sample. This work is still in progress. However we can show some preliminary,promising results. In Fig. 3 we plot 3 light curves for three different energy intervals of a BeppoSAX observation of the Seyfert 2 ESO 103-G35.

The intervals are chosen is order to have the photoelectric cut-off at the separation energy between the first two lightcurves. Therefore, in case of variations of NH, we expect that one of the first two light curves varies, while the other two remain constant (the third energy interval is little affected by small NH variations). Instead, if we have a flux variation, we expect both the second and third light curve vary, while the first remains constant, since the emission at energies lower that the cutoff is mainly due to an extended/reprocessed component. It is clear from Fig. 3 that in the interval between 40 and 60 ks the light curves vary in a way suggesting NH variability. To check if this is indeed the case, we extracted two spectra, one in the 40-60 ks interval, and the other in the remaining time intervals. We performed a careful fit of these spectra, and concluded that the NH measurements differ by $`3\times 10^{22}`$ cm-2, at a 5$`\sigma `$ level of confidence. This NH variation on a timescale of $``$ 20 ks strongly suggests that the X-ray absorber is very close to the central black hole, in agreement with the model we have proposed.

This work was supported in part by NASA grant NAG5-4808.

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