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# Quantum interference with distinguishable photons through indistinguishable pathways

## I Introduction

Quantum mechanical interference is observed when an event can occur by any of several alternate pathways. If an experiment is performed in which it is possible to determine which of the alternate pathways was actually taken, then the interference is lost feynman1 ; feynman2 . For two-photon interference, the existence of indistinguishable alternate pathways for a pair detection events leads to the interference. One of the best-known examples is the Hong-Ou-Mandel interferometer, in which two identical photons meet at a 50/50 beamsplitter and two single-photon detectors monitor the rate at which both detectors register photons (coincidence count) hong . A coincidence count may be recorded either when both photons are reflected (r-r) or when both are transmitted (t-t). If the photons reach the beamsplitter simultaneously, then these two pathways are indistinguishable and interference is observed in the form of a photon bunching effect: the photons exit the beamsplitter together, resulting in a null in the coincidence rate kim2 .

Although the photons reaching the beamsplitter in this example are identical, it is possible to observe interference even if the photons are distinguishable when they reach the beamsplitter. The key is to detect the photons in such a way that the distinguishable information is masked eraser . If, for example, the input photons are orthogonally polarized, no interference is expected, since the polarizations of the detected photons would make it possible to distinguish the r-r and t-t pathways. The interference is restored, however, simply by passing the photons through polarizers prior to detection. With their pass axes oriented halfway between the polarizations of the two input photons, the polarizers mask the polarization information shih ; eraser2 ; pittman . The same principles may be applied to distinguishing timing information. If the photons in one input port arrive earlier than their counterparts, then the r-r and t-t pathways are distinguishable by the photon arrival times and no interference is observed. Again, the interference may be restored by masking the distinguishing timing information pla . This may be accomplished, for example, by introducing alternate pathways into one of the exit ports pittman ; delay . The photon can reach the detector by one of two paths, leading to two different arrival times. If the delays are chosen properly, it is impossible to determine whether the photon left the beamsplitter first and took the longer path to the detector, or whether it left later and reached the detector via the shorter path. It is also possible mask the distinguishing timing information by using narrow-band spectral filters which increase inherent uncertainties associated with the differences in the photon pair arrival times at the beamsplitter kim1 ; filter .

These examples illustrate the role of indistinguishability in quantum interference. If the photons are not indistinguishable in all respects when they reach the beamsplitter, then elements must be introduced to mask the distinguishing information, in effect rendering the distinguishable photons indistinguishable. Here, we report an interference experiment in which the detected photons retain their distinguishing information. The photons approach the beamsplitter at different times, with different polarizations, and may even have different wavelengths. They propagate directly to the detectors without passing through compensating/masking elements and retain their distinguishing properties until being absorbed by the detectors. Nonetheless, interference is observed in the coincidence rate. We explain this counterintuitive result as the interference between two-photon wavepackets.

## II Experiment

An outline of the experimental setup is shown in Fig. 1. A 3 mm thick type-II BBO crystal is pumped by a train of ultrafast pulses with central wavelength of 390 nm and pulse duration of approximately 120 fsec. The crystal is oriented so that a small fraction of the pump photons are down-converted, via the process of spontaneous parametric down-conversion (SPDC), to orthogonally polarized signal and idler photons with center wavelengths of 780 nm. The down-converted photons are emitted into two distinct cones, one with extraordinary polarization (V-polarized) and the other with ordinary polarization (H-polarized). Here, we are interested in the intersections of the two light cones, where the polarizations of the single photons cannot be defined kwiat ; pulse ; kim3 . These two directions, defined by a set of apertures, make an angle of $`\pm `$ 3 degrees with respect to the pump propagation direction, see inset of Fig. 1. These two spatial modes are directed by mirrors to the two input ports of an ordinary non-polarizing beamsplitter. The output ports are monitored by single-photon counting detectors, D3 and D4. Broadband (20 nm at FWHM) spectral filters, F3 and F4, preceding the detectors help to reduce background noise. Polarization analyzers A3 and A4 are removable so that the interference effect can be studied both with and without the polarizers in place.

A set of quartz rods and quartz plates are inserted in each arm of the interferometer: QR1 and QR2 are 20 mm long quartz rods and QP1 and QP2 are 600 $`\mu `$m thick quartz plates. With their optic axes oriented vertically, these birefringent elements introduce a group delay of roughly 668 fsec between the V- and H-polarized photons in addition to the delay accumulated in the SPDC crystal. By tilting the quartz plates QP2 about their optic axes, it is possible to introduce an additional fine delay between the orthogonally polarized photons. The delay between the two arms of the interferometer is controlled by a trombone prism attached to a computer-controlled DC motor. The count rates of the two detectors, as well as the rate of coincidences, were recorded as a function of the delay between the two arms of the interferometer. The effective coincidence window used in this experiment was about 3 nsec, which is smaller than the pump pulse repetition period ($``$ 13 nsec).

Quantum interference is observed as the delay between the two arms is adjusted. This can be seen as the peak and dip shown in Fig. 2. The two different data sets correspond to two different phase settings, i.e., two different orientations of the quartz plates QP2. Tilting the quartz plates introduces a sub-wavelength delay between the orthogonally polarized modes in the lower arm. The peak-dip phase is associated with this additional birefringent delay. Tilting the quartz plates increases not only the relative delay, but also the total path length for the two different polarizations. This is reflected as an offset between the peak and dip.

We note here that the photon pairs approach the beamsplitter with very different properties: they are orthogonally polarized and approach at different times (one photon always reaches the beamsplitter 668 fsec earlier than the other). This time delay is larger than both the 120 fsec pump pulse duration and the 100 fsec single-photon wave-packet defined by the 20 nm (at FWHM) filter. It is somewhat surprising, then, that high visibility interference is observed even though the photons’ properties are not altered before the detection process, i.e., no elements are introduced after the beamsplitter to mask the distinguishing information. (For instance, $`45^{}`$ oriented polarizers and a group delay scheme could be used to ‘erase’ the polarization and temporal distinguishing information, respectively.)

To emphasize the fact that the quantum interference is indeed achieved with distinguishable photons, the experiment was repeated with polarizers A3 and A4 placed in front of the detectors. One of the polarizers was aligned to pass horizontally polarized light (A3 = $`90^{}`$), while the other was aligned to pass vertically polarized light (A4 = $`0^{}`$). The only photons that may be detected in such a set-up are emitted and detected with orthogonal polarizations and are orthogonally polarized at every point in the interferometer. Nevertheless, high visibility quantum interference is observed, as shown in Fig. 3. Although the overall count rate is lowered, the peak and dip features are still evident with no change in the visibility.

In fact, the peak-dip quantum interference is completely independent of the polarizer angles. With QP2 fixed for the coincidence peak (dip), the measurement was repeated for polarizer angles A3 $`=45^{}`$ and A4 $`=45^{}`$ (orthogonal polarizers) and A3 $`=45^{}`$ and A4 $`=45^{}`$ (parallel polarizers). These polarizer settings will typically change the coincidence peak (dip) into a coincidence dip (peak) shih ; eraser2 ; pittman . In this experiment, however, the peak structure remained, with no change in the visibility: only the overall count rates are reduced. Figure 4 shows the data for this set of measurements.

## III Theory

The experimental results make it clear that it is possible to observe high-visibility quantum interference, even when the detected photons have very different properties. The interference effect can be understood more clearly through a calculation of the coincidence rate at the two detectors. As described above, the photons leave the SPDC crystal in the paths corresponding to the overlap of the o- and e-polarized cones. The two-photon state may be written in this case as

$$|\mathrm{\Psi }=\frac{1}{\sqrt{2}}\left\{|\psi _{HV}+e^{i\varphi }|\psi _{VH}\right\}$$
(1)
where $`|\psi _{HV}`$ and $`|\psi _{VH}`$ represent the two ways in which a photon pair may be emitted into these directions and where $`\varphi `$ represents the phase between the two terms. Because the crystal is aligned for type-II SPDC and because it is pumped by a train of short pulses, a multi-mode treatment is required in order to reveal the subtle spectral and temporal characteristics of the two-photon state.

Although the state may be described in either the spectral or temporal domain, the analysis in this case is somewhat simpler in the temporal domain. Accordingly, the states $`|\psi _{HV}`$ and $`|\psi _{VH}`$ are

$`|\psi _{HV}={\displaystyle 𝑑t_o𝑑t_e𝒢_{HV}(t_o,t_e)\widehat{a}_{H1}^{}(t_o)\widehat{a}_{V2}^{}(t_e)|0},`$
$`|\psi _{VH}={\displaystyle 𝑑t_o𝑑t_e𝒢_{VH}(t_o,t_e)\widehat{a}_{V1}^{}(t_e)\widehat{a}_{H2}^{}(t_o)|0},`$
where the two photon amplitude is given by

$`𝒢_{HV}(t_o,t_e)=𝒢_{VH}(t_o,t_e)`$
$`=Ne^{i\overline{\omega }(t_o+t_e)}\xi (t_o,t_e)\mathrm{\Pi }[t_et_o;0,L(k_o^{}k_e^{})].`$
Here, $`N`$ is a normalization constant, $`\overline{\omega }`$ is the mean photon frequency, $`L`$ is the crystal length, and the function $`\mathrm{\Pi }[t;t_1,t_2]`$ is given by

$$\mathrm{\Pi }[t;t_1,t_2]=\{\begin{array}{c}1\text{for}t_1<t<t_2\hfill \\ 0\text{otherwise}.\hfill \end{array}$$
(2)
The function $`\xi (t_o,t_e)`$ is related to the pump field and the birefringent properties of the crystal. For a pump field proportional to $`\mathrm{exp}\{[(\omega 2\overline{\omega })/\sigma ]^2\}`$, $`\xi (t_o,t_e)`$ is

$$\xi (t_o,t_e)=\mathrm{exp}\left\{\frac{\sigma ^2}{4}\left[\left(\frac{k_p^{}k_e^{}}{k_o^{}k_e^{}}\right)t_o\left(\frac{k_p^{}k_o^{}}{k_o^{}k_e^{}}\right)t_e\right]^2\right\}$$

where $`k_p^{}=\frac{dk_p}{d\omega }|_{2\overline{\omega }}`$ and $`k_{o(e)}^{}=\frac{dk_{o(e)}}{d\omega }|_{\overline{\omega }}`$ are the inverse group velocities of the pump ($`p`$), o-polarized ($`o`$), and e-polarized ($`e`$) photons, respectively.

Expressed in this way, it is easy to see that the two-photon probability amplitude describes a pair of photons whose emission times are determined primarily by the temporal shape of the pump pulse, modified somewhat by the group velocity differences inside the crystal. The rectangle function $`\mathrm{\Pi }[t;t_1,t_2]`$ sets upper and lower bounds for the difference in emission times and reflects the fact that the o- and e-polarized photons will separate temporally as they propagate through the crystal. With a lower bound of zero (for a pair created at the exit face) and an upper bound of $`L\left(k_o^{}k_e^{}\right)`$ (for a pair created at the entrance face), it is evident that these expressions describe the two-photon states as they exit the crystal, i.e., before the photons pass through any birefringent elements.

After exiting the crystal, the photons propagate along paths 1 and 2, experiencing nearly identical birefringent delays (due to the quartz rods and quartz plates). They are then brought together at a beamsplitter, though the path lengths may be slightly different. To within a constant overall phase, the two-photon state at the input of the beamsplitter is simply the state given in Eq. (1) with the temporal arguments shifted as follows:

$`𝒢_{HV}(t_o,t_e)𝒢_{HV}(t_o,t_e\tau _2\tau )`$
$`𝒢_{VH}(t_o,t_e)𝒢_{VH}(t_o\tau ,t_e\tau _1)`$
Here, $`c\tau `$ is the difference in free-space path lengths between the upper and lower paths. The delays $`\tau _1`$ and $`\tau _2`$ represent the delays of the e-polarized photons with respect to the o-polarized photons in paths 1 and 2, respectively.

With no polarizers in place, the coincidence rate at detectors D3 and D4 is given by

$$R=𝑑t𝑑t^{}\{P_{HV}(t,t^{})+P_{VH}(t,t^{})\},$$
(3)
where $`P_{HV}(t,t^{})`$ \[$`P_{VH}(t,t^{})`$\] is the probability that a horizontally \[vertically\] polarized photon is detected at D3 at time $`t`$ and that a vertically \[horizontally\] polarized photon is detected at D4 at time $`t^{}`$. The expression should in general also include the terms $`P_{HH}(t,t^{})`$ and $`P_{VV}(t,t^{})`$, but since the photons emitted in type-II SPDC are orthogonally polarized, these are zero for the experiment described here.

The two-time detection probabilities are given by

$$P_{ij}(t,t^{})=\left|\widehat{a}_{i3}(t)\widehat{a}_{j4}(t^{})|\mathrm{\Psi }\right|^2,$$

where $`i`$ and $`j`$ are the polarization labels which can be $`H`$ or $`V`$ depending on the polarization state of the photon in a given spatial mode. To within a constant phase factor, the annihilation operators at the detectors are related to the input operators by

$`\widehat{a}_{i3}(t)={\displaystyle \frac{1}{\sqrt{2}}}[\widehat{a}_{i2}(t)+i\widehat{a}_{i1}(t)],`$
$`\widehat{a}_{i4}(t)={\displaystyle \frac{1}{\sqrt{2}}}[\widehat{a}_{i1}(t)+i\widehat{a}_{i2}(t)].`$
Using the expressions given above, the coincidence count rate $`R`$ given in eq. (3) is found to be

$`R`$ $`=`$ $`R_0\{1\mathrm{cos}[\varphi \overline{\omega }(\tau _2\tau _1)](1{\displaystyle \frac{|2\tau +\tau _2\tau _1|}{L(k_o^{}k_e^{})}})`$ (4)
$`\times \mathrm{exp}[{\displaystyle \frac{\sigma ^2}{8}}[\left({\displaystyle \frac{2k_p^{}k_o^{}k_e^{}}{k_o^{}k_e^{}}}\right)\tau +\left({\displaystyle \frac{k_p^{}k_o^{}}{k_o^{}k_e^{}}}\right)(\tau _2\tau _1)]^2]\mathrm{\Pi }[2\tau +\tau _2\tau _1;L(k_o^{}k_e^{}),L(k_o^{}k_e^{})]\},`$
where $`R_0`$ is a constant. While this expression is a bit cumbersome, it simplifies greatly for $`\tau =0`$ (equal path lengths) and $`\tau _1\tau _20`$ (nearly identical birefringent delays), in which case the expression becomes

$$RR_0\{1\mathrm{cos}[\varphi \overline{\omega }(\tau _2\tau _1)]\}.$$
(5)
In this form, it is clear that the coincidence count rate can be made to vanish for the appropriate birefringent delays and, likewise, that it can be raised to twice the background rate with a small phase shift. \[Recall that $`\varphi `$ is the unknown fixed phase term from eq. (1).\] It is these two settings that were used to generate the data shown in Figs. 2 $``$ 4. As described above, the phase shift in $`\tau _1\tau _2`$ was introduced in our experiment by tilting QP2. This type of adjustment introduces slightly different path length increases for the two polarizations, but also increases the overall length of the lower arm (of the interferometer) so that the trombone prism must be adjusted to compensate. This is the origin of the offset between the coincidence peak and the coincidence dip observed in the figures.

## IV Discussions

A couple of results from the above analysis invite further comment. First, the interference features are independent of the presence of polarizers or, if polarizers are in place, of their orientations. This is in contrast to previous experiments, where the relative orientations of the polarizers determine the phase between the interfering terms and whether the interference is constructive or destructive. The inclusion of polarizers in the above analysis changes the overall rate of coincidence detection, but the peak/dip features persist. Thus, photon polarization has absolutely no bearing on the interference effect and there is no need to mask differences between the photons polarizations.

Another result worth noting is that the photons may reach the beamsplitter at very different times pla . Recall that the photons are emitted with orthogonal polarizations and, therefore, travel at different speeds through the birefringent elements. By adjusting the birefringent delays, it is possible to change the arrival times for the orthogonally polarized photons. For maximum visibility, $`\tau _1`$ and $`\tau _2`$ must be nearly identical, but the constraint is on their difference, not on the individual delays. Thus, interference can be observed for arbitrary amounts of birefringent delay, as long as the delays in the two arms are nearly identical. These results stand in contrast to previous works involving similar configurations where interference could be observed only if there were no distinguishing timing or polarization information, or if such information were erased before detection shih ; eraser2 ; pittman ; pulse ; delay ; filter . Here, such information seems not to matter.

The difference between those experiments and the one reported here is the input state. Whereas the previous experiments involved single two-photon states, the input state for our experiment is the superposition state of Eq. (1). This seemingly subtle change to the input state is critical to the observed interference effect, for this superposition now provides two pathways for a given detection outcome. Suppose, for example, that detector D3 registers a horizontally polarized photon, while D4 registers a vertically polarized photon. There are two ways that this may happen: the photons may be emitted as $`|H_1|V_2`$ and be reflected at the beamsplitter; or they may be emitted as $`|V_1|H_2`$ and be transmitted. As long as the interferometer is properly adjusted, these two pathways will be indistinguishable, even though the photons themselves may have very different properties (see $`\mathrm{\Psi }_1`$ and $`\mathrm{\Psi }_4`$ in Fig. 5).

The relationships between the various detection pathways are shown in the two-photon Feynman diagrams of Fig. 5. The four diagrams leading to coincident detection correspond to two possible outcomes (both photons reflected, r-r, or transmitted, t-t, at the beamsplitter) for each of the two possible emission states ($`|H_1|V_2`$ or $`|V_1|H_2`$). The four cases are pairwise indistinguishable: $`\mathrm{\Psi }_1`$ and $`\mathrm{\Psi }_4`$ correspond to H at D3 and V at D4, while $`\mathrm{\Psi }_2`$ and $`\mathrm{\Psi }_3`$ correspond to V at D3 and H at D4. Note, also, that the horizontally polarized photon is always detected first, a consequence of the birefringent delays. As long as the delays are identical, the amplitudes remain pairwise indistinguishable.

Returning to the comparison with previous two-photon interference experiments, it is clear that indistinguishability still plays an important role, even when the photons, themselves are distinguishable. While the detected photons may be different, it is critical that the r-r and t-t pathways be indistinguishable. Typically, this condition could be satisfied only if the photons were identical as they entered the beamsplitter or if they were detected in such a way that they appeared to be identical. Here, the indistinguishability is found in the ambiguity of the input to the beamsplitter. For example, a photon with a particular set of properties may be detected at a given detector, with a second photon having a distinct set of properties at the other detector. The r-r and t-t pathways remain indistinguishable, however, because there are two ways that these two photons may be emitted into the set-up.

It is the superposition of the two two-photon states before they reach the beamsplitter, therefore, that is essential to the interference effect. Indeed, this type of arrangement was originally proposed by Braunstein and Mann as a means of distinguishing one of the four polarization Bell states braunstein ; bellmeasure . It is interesting to note that the interference effect persists even when $`|\mathrm{\Psi }`$ exhibits little or no polarization entanglement. It is well documented that a pure polarization-entangled state may be generated only when the two photons in a particular path are distinguishable only by their polarizations. Differences in spectral properties and/or time of arrival tend to blur the entanglement pulse ; kim3 ; kim4 . In this experiment, however, the interference effect is observed even when the photons may be distinguished by their arrival times. Since the photon pairs are generated in an ultrafast-pulse-pumped type-II crystal, they also posses distinguishing spectral information pulse ; kim3 ; kim4 ; grice . Even so, the visibility is much higher, 100% in principle, than would be expected if this spectral information were to play a role. This suggests that it is not even necessary that the photons have the same center wavelengths.

In conclusion, we have demonstrated a two-photon quantum interference effect in which the detected individual photons have very different properties. Unlike other interference experiments, in which the photons themselves must be indistinguishable upon detection, the individual photons here have different polarization states, different arrival times, and different spectra. Indistinguishability still plays a critical role for quantum interference to occur, however, and comes in the form of the input state: for each detection event, there are essentially two possible sources (or quantum mechanical amplitudes) for the photon pair.

## Acknowledgements

This research was supported in part by the National Security Agency, the Advanced Research & Development Activity, and the LDRD program of The Oak Ridge National Laboratory, managed for the U.S. DOE by UT-Battelle, LLC, under contract No. DE-AC05-00OR22725.


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# Ferromagnetic Kondo-Lattice Model

## 1 Introduction

The Kondo-lattice model (KLM), being also denoted as s-f or s-d model or, in its strong-coupling regime, as double exchange model, is today surely one of the most prominent models in solid state theory, and that mainly because of its great variety of important applications to rather hot topics in the wide field of collective magnetism. It refers to magnetic materials which get their magnetic properties from a system of localized magnetic moments being indirectly coupled via an interband exchange $`J`$ to itinerant conduction electrons. Many characteristic properties of such materials can be traced back to this interband exchange.

There are a lot of important applications of the KLM, first of all to the classical systems of magnetic semiconductors such as EuO and EuS  and magnetic metals such as Gd  ($`J>0`$, weak to intermediate coupling). All these materials have strictly localized moments because of the half-filled $`4f`$ shell of the rare earth ion (Eu2+, Gd3+). The striking temperature-dependence of the unoccupied (!) conduction bandstates in the EuX  manifesting itself, e. g., in the well-known red shift effect , and the effective moment coupling in Gd via a conduction electron spin polarization (RKKY)  can be understood only by the existence of the interband exchange $`J`$.

Other candidates are the intensively investigated diluted magnetic semiconductors such as Ga1-xMnxAs with probably negative $`J`$ (strong coupling). The Mn2+ ion creates simultaneously an $`S=\frac{5}{2}`$ spin and an itinerant hole in the GaAs valence band . The latter takes care for an indirect coupling between the randomly distributed magnetic moments that leads already for very small $`x`$ to a ferromagnetic order with a maximum $`T_\mathrm{C}`$ of $`110`$ K for $`x=0.053`$ .

Another hot topic because of great potential for engineering applications are the colossal magnetoresistance (CMR) materials  such as La1-x(Ca,Sr)xMnO3 which show up a very rich magnetic phase diagram. For $`0.2x0.4`$ the originally antiferromagnetic and insulating parent compound LaMnO3 changes into a ferromagnetic metal. This is ascribed to a homogeneous valence mixing (Mn$`{}_{}{}^{3+}{}_{1x}{}^{}`$ Mn$`{}_{}{}^{4+}{}_{x}{}^{}`$). The three $`3d_{t_{2g}}`$ electrons in Mn3+ are considered more or less localized forming an $`S=\frac{3}{2}`$ moment while the additional $`3d_{e_g}`$ electron is itinerant. Again, the local moment-itinerant electron exchange is made responsible for many typical features of the CMR materials ($`J>0`$, strong coupling).

We derive in the next section the multiband-Hamiltonian of the Kondo-lattice model which is combined in Section 4 with an “ab initio” bandstructure calculation to get the temperature-dependent electronic structure of the prototype ferromagnets EuO and EuS. To understand the physics of the KLM we present in Section 3 for the nondegenerate case an analysis of the magnetic and electronic model properties.

## 2 Multiband Kondo-Lattice Model

The system under consideration consists of quasi-free electrons in rather broad conduction bands (d bands) and localized electrons with extremely flat dispersions (f levels). While there is no contribution of the f electrons to the kinetic energy, the part of the d electrons reads

$$H_d=\underset{ijm\overline{m}\sigma }{}T_{ij}^{m\overline{m}}c_{im\sigma }^+c_{j\overline{m}\sigma }$$
(1)
The hopping process from site $`𝐑_i`$ to site $`𝐑_j`$ may be accompanied by an orbital change ($`m\overline{m}`$). $`T_{ij}^{m\overline{m}}`$ are the respective hopping integrals. $`c_{jm\sigma }^+`$ ($`c_{jm\sigma }`$) is the creation (annihilation) operator for a Wannier electron at site $`𝐑_j`$ in the orbital m with spin $`\sigma `$ ($`\sigma =`$, $``$).

When applying the model study to real local-moment materials, intended as our final goal, we have to require that the single-electron energies do not only account for the kinetic energy and the influence of the lattice potential, but also for all those interactions which are not explicitly covered by the model Hamiltonian. That means that the hopping integrals are to be taken from a proper “ab initio” band calculation. We exemplify the procedure in Sect. 4 for the special case of the ferromagnetic europium chalcogenides. In particular we show how to avoid the well-known double-counting problem of important interactions.

The Coulomb interaction is restricted to intraatomic terms. Furthermore, we assume that only two subbands are involved in the scattering process. Then the interaction part can be written as

$$H_c=H_{dd}+H_{ff}+H_{df}$$
(2)
In an obvious manner the Coulomb interaction may be split into three different parts depending on whether both interacting particles stem from a conduction band $`H_{dd}`$, or both from a flat band $`H_{ff}`$, or one from a flat band and the other from a conduction band $`H_{df}`$. The first term refers to electron correlations in the conduction bands, not explicitly taken into account by the KLM. As mentioned, our procedure for describing real materials accounts for such correlations by a proper renormalization of the single particle energies.

The term $`H_{ff}`$ describes interactions between electrons from the flat bands which interest us only with respect to the fact that they form permanent magnetic moments (spins):

$$𝐒_i=\underset{f}{}𝝈_f$$
(3)
$`𝝈_f`$ is the spin operator of an electron in subband f. If it is necessary to consider a (super)exchange interaction between the local spins then $`H_{ff}`$ is chosen to be a Heisenberg Hamiltonian, possibly with a symmetry-breaking single-ion anisotropy $`D`$:

$$H_{ff}=\underset{ij}{}J_{ij}𝐒_i𝐒_jD\underset{i}{}\left(S_i^z\right)^2$$
(4)
The third term in (2) $`H_{df}`$ refers to the interaction between a localized and an itinerant electron. Neglecting unimportant spin-independent contributions it can be written as an intraatomic exchange, i. e. a local interaction between the conduction electron spin $`𝝈_{jm}`$ and the local moment spin $`𝐒_j`$  :

$$H_{df}=J\underset{jm}{}𝝈_{jm}𝐒_j$$
(5)
Here $`m`$ denotes the conduction electron orbital. $`J`$ is the exchange coupling constant being assumed to be identical for all df pairs. Using second quantization for the itinerant electron spin ($`n_{jm\sigma }=c_{jm\sigma }^+c_{jm\sigma }`$), this interaction reads:

$$H_{df}=\frac{1}{2}J\underset{jm}{}\left(S_j^z\left(n_{jm}n_{jm}\right)+S_j^+c_{jm}^+c_{jm}+S_j^{}c_{jm}^+c_{jm}\right)$$
(6)
We see that the first term describes an Ising-like interaction of the two spin operators while the two others provide spin exchange processes between localized moment and itinerant electron. In particular the two latter terms are responsible for many typical properties of the Kondo-lattice materials. Spin exchange may happen in three different elementary processes: magnon emission by an itinerant $``$ electron, magnon absorption by an $``$ electron and formation of a quasiparticle (magnetic polaron). The latter can be understood as a propagating electron dressed by a virtual cloud of repeatedly emitted and reabsorbed magnons corresponding to a depolarization of the immediate localized spin neighbourhood.

The total Hamiltonian of the multiband-Kondo lattice is composed of (1), (2) and (6)

$$H=H_d+H_{ff}+H_{df}$$
(7)
An important model parameter is of course the effective coupling constant $`\frac{J}{W}`$ where $`W`$ is the Bloch-bandwidth. Especially the sign of $`J`$ is decisive. Other parameters are the local spin $`S`$, the lattice structure, and above all the band occupation $`n=_{m\sigma }n_{m\sigma }`$. In case of a nondegenerate band $`n`$ is a number in between 0 and 2.

## 3 Magnetic and Electronic Model Properties

The many-body problem of the KLM is not exactly solvable for the general case even for the nondegenerate case, for which we can remove the orbital dependence and which shall exclusively be tackled in this section:

$$H=\underset{ij\sigma }{}T_{ij}c_{i\sigma }^+c_{j\sigma }J\underset{j}{}𝐒_j𝝈_j=H_0+H_1$$
(8)
However, there exists a non-trivial, very illustrative limiting case which is rigorously tractable and nevertheless exhibits all the above-mentioned elementary excitation processes . It refers to a single electron in an otherwise empty conduction band coupled to a ferromagnetically saturated moment system, e. g. EuO at $`T=0`$. In this case the $``$ spectrum is simple, because the $``$ electron cannot exchange its spin with

the parallel aligned spin system. Only the Ising-type interaction in (5) and (6) takes care for a rigid shift of the total spectrum by $`\frac{1}{2}JS`$. The spectral density is a $`\delta `$-function at $`ϵ(𝐤)\frac{1}{2}JS`$ where $`ϵ`$ is the free Bloch energy, the Fourier transform of the hopping integral $`T_{ij}`$. Real correlation effects appear, however, in the $``$ spectrum. Fig. 1 shows the energy dependence of the $``$-spectral density for some symmetry points. For weak couplings the spectral density consists of a single pronounced peak. The finite width points to a finite quasiparticle lifetime due to first spinflip processes, but the quasiparticle bandstructure, being read off from the peak positions, is still very similar in shape to the Bloch dispersion.

This changes drastically already for rather moderate effective exchange couplings $`JS/W`$. One observes in certain parts of the Brillouin zone, for a strongly coupled system even in the whole Brillouin zone, that the excitation energy splits into two parts. The sharp high-energy peak belongs to the magnetic polaron while the broader low-energy part consists of scattering states due to magnon emission. As long as the polaron peak is above the scattering spectrum the quasiparticle has even an infinite lifetime. The scattering spectrum is in general rather broad because the emitted magnon can carry away any wave-vector from the first Brillouin zone. Because of the concomitant spinflip, magnon emission can happen only if there are $``$ states within reach. Therefore, the scattering part extends just over that energy region where $`\rho _{}0`$ ($`\rho _\sigma `$: quasiparticle density of states (Q-DOS)).

For the general case (finite temperature, finite band occupation) the many-body problem of the KLM cannot be solved exactly. Approximations must be tolerated. The central quantity is the selfenergy, for which we use the Green function procedure developed in . This non-perturbational theory can be considered a “moment conserving decoupling approximation” (MCDA) which interpolates between exact limiting cases as, e. g., the above discussed example. In more detail, the method decouples the hierarchy of equations of motion by expressing certain “higher” Green functions as linear combination of “lower” functions, already involved in the procedure. The ansatz is motivated by exact special cases as the atomic limit, ferromagnetic saturation, local spin $`S=1/2`$, full or empty band, and so on. Free parameters in the ansatz are eventually fitted to rigorous spectral moments. As other methods, too, e. g. the interpolating selfenergy approaches in refs., it leads to the following structure of the selfenergy:

$$\mathrm{\Sigma }_{𝐤\sigma }(E)=\frac{1}{2}Jz_\sigma S^z+J^2D_{𝐤\sigma }(E)$$
(9)
Restriction to the first term, only, yields the mean-field approach to the KLM, which is correct for sufficiently weak couplings $`J`$. It is due to the Ising-part in Eq. (5) ($`z_\sigma =\delta _\sigma \delta _\sigma `$). Without the second part of the selfenergy it would give rise to a spin-polarized splitting of the conduction band. The term $`D_{𝐤\sigma }(E)`$ is more complicated being predominantly determined by the spin exchange processes. It is a complicated functional of the selfenergy itself, i. e. (9) is an implicit equation for $`\mathrm{\Sigma }_{𝐤\sigma }(E)`$ and not at all an analytical solution. $`D_{𝐤\sigma }(E)`$ depends, further on, on mixed spin correlations such as $`S_i^zn_{i\sigma }`$,$`S_i^+c_i^+c_i`$, …, built up by combinations of localized-spin and itinerant-electron operators. Fortunately, all these mixed correlations can rigorously be expressed via the spectral theorem by any of the Green functions involved in the hierarchy of the MCDA.

However, there are also pure local-moment correlations of the form $`S_i^z`$, $`S_i^\pm S_i^{}`$, $`\left(S_i^z\right)^3`$, …, which also have to be expressed by the selfenergy (9). For this purpose we use the modified RKKY theory of  which exploits a mapping of the interband exchange (5) to an effective Heisenberg model,

$$H_f=\underset{ij}{}\widehat{J}_{ij}𝐒_i𝐒_j$$
(10)
by averaging out the conduction electron degrees of freedom:

$$J\underset{j}{}𝐒_j𝝈_jJ\underset{j}{}𝐒_j𝝈_j^{(c)}H_f$$
(11)
In the last analysis this means to determine the expectation value $`c_{𝐤+𝐪\sigma }^+c_{𝐤\sigma ^{^{}}}^{(c)}`$. We use again a Green-function procedure  which eventually leads to effective exchange integrals in (10):

$`\widehat{J}_{ij}={\displaystyle \frac{J^2}{4\pi N^2}}{\displaystyle \underset{\mathrm{𝐤𝐪}\sigma }{}}e^{i𝐪(𝐑_i𝐑_j)}`$ $`{\displaystyle _{\mathrm{}}^+\mathrm{}}dEf_{}(E)\text{Im}[(Eϵ(𝐤)+i0^+)`$ (12)
$`\times (Eϵ(𝐤+𝐪)\mathrm{\Sigma }_{𝐤+𝐪\sigma }(E))]^1`$
$`f_{}(E)`$ denotes the Fermi function. The effective exchange integrals are decisively influenced by the conduction electron selfenergy $`\mathrm{\Sigma }_\sigma `$ which brings a distinct band occupation and temperature dependence to the $`\widehat{J}_{ij}`$. Neglecting $`\mathrm{\Sigma }_\sigma `$ leads to the “conventional” RKKY formula with $`J_{ij}J^2`$ as a result of second order perturbation theory. Via $`\mathrm{\Sigma }_\sigma `$ higher order terms of the electron spin polarization enter the modified RKKY being therefore not restricted to weak couplings, only. Note that at the right-hand side of Eq. (12) the product of two propagators appear. From the equation of motion method in  it follows directly that one of them is dressed by a selfenergy, the other not.

To get from the effective operator (10) the magnetic properties of the KLM we apply the standard Tyablikov-approximation which is known to yield convincing results in the low as well as in the high temperature region . All the above-mentioned local-moment correlations are then expressed by the electronic selfenergy. We therefore end up with a closed system of equations that can be solved self-consistently for all entities of interest.

Fig. 2 shows the temperature dependence of the

quasiparticle bandstructure (Q-BS), derived as density plot from the spectral density, and the quasiparticle density of states (Q-DOS) $`\rho _\sigma (E)`$ for a typical parameter set from the moderate coupling regime ($`J=0.2`$ eV, $`W=1`$ eV, $`n=0.2`$, $`S=\frac{7}{2}`$, sc lattice). In this case the self-consistently calculated Curie temperature $`T_\mathrm{C}`$ amounts to $`238`$ K. At $`T=37`$ K the local-moment magnetization is $`3.4`$ and therewith very close to saturation. The theory reproduces, in spite of the finite carrier concentration, the same features as for the exact $`(n=0,T=0)`$-case exhibited in Fig. 1. The $``$ dispersion as well as the QDOS $`\rho _{}`$ are practically identical to the respective “free” Bloch functions. The $``$ spectrum, however, is more complicated. The scattering states take away a substantial part of the spectral weight near the $`\mathrm{\Gamma }`$ point while near the $`R`$ point the polaron state clearly dominates. With increasing temperature (decreasing $`S^z`$) a finite magnon density appears allowing for scattering states in the $``$ spectrum, too, because of magnon absorption and simultaneous spinflip by the $``$ electron. Furthermore, polaron and scattering states separate, where, surprisingly, the rather broad scattering spectrum is in wide wave-vector regions bunched to a prominent peak. At $`T=T_\mathrm{C}`$ the spin asymmetry is removed but there remains a correlation-caused splitting of the spectrum into two branches and two subbands, respectively, due to the interband exchange coupling $`J`$. Because of the possibility of mutual spin exchange $`\rho _{}`$ and $`\rho _{}`$ are occupying for finite temperatures always the same energy regions.

The key-quantity of ferromagnetism is the Curie temperature $`T_\mathrm{C}`$. A finite $`T_\mathrm{C}`$ comes out as a consequence of an indirect coupling between the local moments, mediated by a polarization of the conduction electron

spins. Therefore, $`T_\mathrm{C}`$ exhibits a strong carrier-concentration dependence which is plotted in Fig. 3. The effective exchange integrals have been taken into account up to 25th neighbours. Ferromagnetism appears for low electron (hole) concentrations, while being excluded in the region around half-filling ($`n=1`$). Around $`n=1`$ we expect an antiferromagnetic phase, however, not explicitly calculated here. A similar $`n`$-dependence of $`T_\mathrm{C}`$ has been found in Ref. . It is interesting to compare the results with those of the conventional RKKY, given by $`\mathrm{\Sigma }_\sigma 0`$ in Eq. (12). A corresponding curve is inserted in Fig. 3. The maximal $`T_\mathrm{C}`$ values are higher, but ferromagnetism exists only in a very narrow region of low electron (hole) concentrations where this region turns out to be independent of $`J`$.

Two features dominate the $`J`$-dependence of the Curie temperature plotted in part (b) of Fig. 3. The first is the appearance of a critical $`J`$ for band occupations for which the conventional RKKY does not allow ferromagnetism ($`n0.13`$). This is in accordance with the fact that for $`J0`$ the modified RKKY reproduces the conventional RKKY. The second fact is that $`T_\mathrm{C}`$ runs into a saturation for strong couplings $`J`$, where the saturation value depends on the band occupation $`n`$. These results are far beyond conventional RKKY which can work of course only in the weak coupling regime.

It is interesting to observe (see Fig. 4) that in the weak coupling RKKY region $`T_\mathrm{C}`$ scales with the effective

coupling constant $`\frac{J}{W}`$ and in the strong coupling double exchange region with the kinetic energy, i. e. $`W`$. In part (b) of Fig. 4 the change from RKKY behaviour (small $`\frac{J}{W}`$) to double exchange behaviour (large $`\frac{J}{W}`$) is clearly to be seen.

Fig. 5 shows a typical example of a spin-wave dispersion, which obtains via the effective exchange integrals (12) a distinct temperature dependence. Upon heating the dipersion relation

uniformly softens, disappearing above $`T_\mathrm{C}`$. This agrees qualitatively with neutron scattering data on manganites .

## 4 Application to ferromagnetic EuO and EuS

In the last step we want to demonstrate how the model analysis can be used to describe real magnetic materials. We exemplify the method with respect to the classical local-moment ferromagnets EuO and EuS. These are ferromagnetic semiconductors which crystallize in the fcc-rocksalt structure with lattice constants $`a=5.142`$ Å(EuO) and $`a=5.95`$ Å(EuS), respectively. The physics of these materials is mainly determined by localized and half-filled 4f levels, on the one hand, and, on the other hand, by extended, at low temperature empty, 5d band states. In accordance to Hund’s rule, the Eu2+-4f shell produces a maximum spin moment $`S=\frac{7}{2}`$.

To investigate real materials such as EuO and EuS one has to exploit the multiband version of the KLM developed in Section 1. As already explained, the hopping integrals $`T_{ij}^{m\overline{m}}`$ in (1) have not only to incorporate the kinetic energy of the band electrons plus the influence of the

periodic lattice potential but also as realistically as possible all those interactions which are not directly covered by the model Hamiltonian. For this purpose we performed a bandstructure calculation based on density functional theory, using the Andersen scheme  of a tight-binding linear muffin-tin orbital (TB-LMTO) ansatz. LDA-typical difficulties arise with the strongly localized character of the 4f levels. A normal LDA calculation for EuO produces a metal with the 4f levels lying well within the conduction band. To circumvent the problem we considered the 4f electrons as core electrons, since our main interest is focused on the temperature-reaction of the (empty) conduction bands. In our study the 4f levels appear only as localized spins (moments) in the sense of $`H_{ff}`$ in Eq. (4). Fig. 6 shows the so-derived spin-dependent bandstructure of EuS without the 4f levels. The low-energy part belongs to S-3p states, we are not interested in here, because only $`fd`$ excitations shall be in the focus. The conduction band region is dominated by Eu-5d states, to which we have restricted the investigation by our combined many-particle, first principles procedure. For comparison we have also performed an LDA+U calculation which indeed is able to put the respective bands into better positions. On the other hand, the results, which we are interested in, do not differ too strongly from those of LDA with the 4f electrons in the core. So we have chosen the much simpler LDA calculation, since our study mainly aims at overall correlation and temperature effects. The extreme details of the band structure are not so important.

The many-body treatment of the multiband KLM follows exactly the same line as for the single-band case, no need to create new approaches. However, we have to fix the only parameter of our procedure, the interband exchange $`J`$. It is generally assumed that an LDA treatment of ferromagnetism is quite compatible with a mean-field picture, so that the $`T=0`$-shift of the $``$ and $``$ dispersions in Fig. 6 should amount to $`\mathrm{\Delta }=JS`$. However, it can be seen that the assumption of a rigid shift is too simple. A certain energy dependence of the exchange splitting is found by LDA, too. We decided to use the splitting of the 5d-band centre of gravity to fix the $`J`$ for EuS at $`0.23`$ eV . Averaging over prominent features in the Q-DOS of EuO yields a similar value of $`J=0.25`$ eV .

Another important issue concerns the renormalized single-particle input, because a double counting of the decisive interband exchange, once by the LDA input and once more explicitly in the model-Hamiltonian (5), might produce rather misleading results. The most direct solution of this problem would be to switch off the interband exchange $`H_{df}`$ in the LDA code, which turns out to be impossible. However we can elegantly exploit the exact limiting case, discussed at the beginning of Section 3. For zero temperature and zero band occupation the $``$ spectrum of the single- as well as multiband-KLM is only rigidly shifted towards lower energies by the amount of $`\frac{1}{2}JS`$. Thus we can use without any manipulation the $``$ dispersions of the LDA calculation ($`T=0!`$) for the empty 5d bands as input for the single-electron Hamiltonian (1). There is no need to switch off $`H_{df}`$ because in this special case it leads only to an unimportant rigid shift. Note that this holds only for the $``$ part, the $``$ spectrum is even at $`T=0`$ strongly influenced by correlation effects (see Fig. 1). Therewith it is guaranteed, on the one side, that all those interactions, which are not directly covered by the KLM, are implicitly taken into account by the LDA-renormalized single-particle energies. On the other side, a double counting of any decisive interaction, which usually occurs when combining first-principles and many-body model calculations, is definitely avoided.

Because of the empty conduction bands a self-consistent justification of the EuO (EuS) ferromagnetism via the modified RKKY-treatment of Section 3 is not possible. The magnetic properties of the insulators EuO and EuS are exclusively due to the partial operator $`H_{ff}`$ (4). Its exchange integrals between nearest ($`J_1`$) and next-nearest ($`J_2`$) neighbours have been derived by a neutron scattering spin wave analysis : $`J_1/k_\mathrm{B}=0.625(0.221)`$ K, $`J_2=0.125(0.100)`$ K for EuO (EuS). The single-ion anisotropy constant $`D`$ does not play a decisive role as long as the bulk bandstructure and its temperature dependence is aimed at. However, when treating systems of lower dimensionality (films, surfaces) as done for EuO in Refs. , then a finite $`D`$ is necessary to overcome the Mermin-Wagner theorem  for getting a collective magnetic order of the moment system. $`D`$ has been chosen in such a way that the experimental $`T_\mathrm{C}`$ value is correctly reproduced (see Fig. 3 in Ref. . The temperature-dependence of the 4f moment system leads to a remarkable induced temperature behaviour of the (unoccupied!) 5d spectrum. The evaluation of the effective Heisenberg model (4) is done by a Tyablikov decoupling of the equation of motion of a poperly chosen spin Green function. Details are given in .

Let us now select some typical results found for the archetypal ferromagnetic semiconductors EuO and EuS. We have no intention to be complete in this overview, rather to demonstrate the possibilities of our combined many-body/ab initio

method. Fig. 7 and 8 show the quasiparticle density of states (Q-DOS) for EuO and EuS, respectively, for five different 4f magnetizations, i. e. five different temperatures. Not surprisingly, the Q-DOS of EuO (Fig. 7) and EuS (Fig. 8) are qualitatively rather similar. Since we have taken into account the full bandstructure of the Eu-5d conduction bands, the symmetry of the different 5d orbitals is preserved. The 5d bands can therefore be decomposed into $`t_{2g}`$ and $`e_g`$ subbands, where the $`t_{2g}`$ bands are substantially broader ($`7`$ eV (EuS), $`9`$ eV (EuO)) than the $`e_g`$ bands ($``$ 4 eV (EuS), $``$ 6 eV (EuO)). A remarkable temperature-dependence shows up for both ferromagnets, manifesting itself, e. g., in a shift of the lower edge of the $``$ Q-DOS to lower energies upon cooling from $`T=T_\mathrm{C}`$ to $`T=0`$. This explains the famous red shift of the optical absorption edge for the electronic $`4f5d_{t_{2g}}`$ transition, in the meantime observed for all ferromagnetic local-moment systems . The temperature behaviour do not comply with the simple Stoner picture of an energy-independent induced exchange splitting of the spectra. The reason for the observed more complicated behaviour as a function of temperature is that in our theory correlation is treated in a way distinctly beyond mean-field.

While the Q-DOS refers to the spin resolved but angle averaged, direct or inverse photoemission experiment, the $`𝐤`$ dependent spectral density is the angle resolved counterpart. Prominent peaks of the spectral density as a function of energy determine the $`E(𝐤)`$ quasiparticle bandstructure (Q-BS). As an example, Fig. 9 represents the EuO-spectral density as a density plot for some symmetry directions and

three different temperatures. The degree of blackening is a measure of the magnitude of the spectral density. For $`T=0`$ ($`S_z=S`$) the $``$ spectral density agrees, except for a constant shift, with the LDA result, being therefore a $`\delta `$-function at the excitation energy, corresponding to a quasiparticle with infinite lifetime. The $``$ spectral density, however, exhibits already at $`T=0`$ a broadening of the dispersion curves, most notably around the $`\mathrm{\Gamma }`$-point, which indicates finite quasiparticle lifetimes due to correlation effects. For intermediate temperatures ($`S_z=0.5S`$) a broadening sets in also for the $``$ dispersions because the $``$ electron, too, can now exchange its spin with the no longer saturated local moment system. In the $``$ spectrum correlation effects increase leading to further quasiparticle damping. Simultaneously, both spin spectra are shifted towards each other reducing therewith the effective exchange splitting. At $`T=T_\mathrm{C}`$ ($`S_z=0`$) $``$ and $``$ dispersions conincide. Very similar behaviour is found for EuS .

As mentioned, the Q-BS has been derived from the spectral density. To give an insight into the temperature behaviour of the spectral density we have plotted in Fig. 10 for two $`𝐤`$-points from the first Brillouin zone ($`\mathrm{\Gamma }`$, W) the energy dependence of the spectral density for the same three 4f magnetizations as in Fig. 9, but now for EuS. For the $`\mathrm{\Gamma }`$-point (Fig. 10 (a)) we have to expect two structures according to the twofold degenerate ($`e_g`$) and threefold degenerate ($`t_{2g}`$) dispersions. Well defined quasiparticle peaks appear, spin split below $`T_\mathrm{C}`$. The spin splitting, induced via the interband coupling to the magnetically active 4f system, collapses for $`TT_\mathrm{C}`$. One speaks of a Stoner-type behaviour. Quasiparticle damping, that scales with the peak width, obviously increases with temperature. At the W-point (Fig. 10 (b)) four sharp peaks show up in the $``$ spectrum, and, though already strongly damped, the same peak sequence appears in the $``$ part, too (compare with the Q-BS in Fig. 9). The reduction of the spin splitting with increasing temperature leads to a strong overlap of the two upper peaks, which are then no longer distinguishable.

Altogether, the 5d spectral densities of the ferromagnetic semiconductors EuS and EuO (not shown here) exhibit drastic temperature-dependencies, what concerns the positions and the widths of the quasiparticle peaks. The driving force is the interband (4f-5d) exchange interaction, the investigation of which was the main aim of the presented study.

## 5 Summary

We have demonstrated how the (multiband) Kondo-lattice model can be used for a realistic description of the strikingly temperature-dependent electronic excitation spectrum of local-moment ferromagnets. For this purpose we have combined a many-body evaluation of the KLM with a first principles bandstructure calculation (TB-LMTO) for the ferromagnetic semiconductors EuO and EuS.

In the first step we inspected an exactly solvable, non-trivial limiting case of the KLM to learn about the fundamental elementary excitations. In addition, this limiting case provides a weighty testing criterion for unavoidable approximations in the case of the not exactly solvable general case.

By use of a self-consistent approach we found out the electronic as well as magnetic properties of the KLM as functions of decisive model parameters such as band occupation and interband exchange coupling. By inspecting the Curie temperature we could demonstrate the transition from a weak-coupling RKKY behaviour to a strong-coupling double exchange scenario. It appears remarkable that both features are simultaneously involved in our theory.

Using a straightforward multiband version of the KLM with identical theoretical approaches we have worked out the influence of the localized magnetic 4f moments of the Eu2+ ion on the 5d conduction bands in EuO and EuS, respectively. The normally empty bands exhibit a distinct and unconventional (”not Stoner-like”) temperature-dependent exchange splitting induced by the interband exchange coupling to the 4f levels. As a special detail we observe the famous red shift effect in EuO as well as EuS.

Financial support by the SFB 290 of the “Deutsche Forschungsgemeinschaft” is gratefully acknowledged.