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# Phase transitions induced by correlated hopping in the Falicov-Kimball model

## 1 Introduction

Recent theoretical studies of the Falicov-Kimball model (FKM)  showed that although this model is relatively simple, it can yield the correct physics for describing rare-earth and transition metal compounds . The model is based on the coexistence of two different types of electronic states in given materials: localized, highly correlated ionic-like states and extended, uncorrelated, Bloch-like states. The Hamiltonian of the model is given by sum of three terms

$$H=\underset{ij}{}t_{ij}d_i^+d_j+U\underset{i}{}d_i^+d_if_i^+f_i+E_f\underset{i}{}f_i^+f_i.$$
(1)
The first term of (1) is the kinetic energy corresponding to quantum mechanical hopping of the itinerant $`d`$ electrons between sites $`i`$ and $`j`$. Usually it is assumed that $`t_{ij}=t`$ if $`i`$ and $`j`$ are nearest neighbors and zero otherwise (the conventional FKM), however, in what follows we consider a much more realistic type of hopping, so for the moment we leave it as arbitrary. The second term represents the Coulomb interaction between $`f`$ electrons with density $`n_f=\frac{N_f}{L}=\frac{1}{L}_if_i^+f_i`$ and $`d`$ electrons with density $`n_d=\frac{N_d}{L}=\frac{1}{L}_id_i^+d_i`$, where $`L`$ is the number of lattice sites. The last term stands for the localized $`f`$ electrons whose sharp energy level is $`E_f`$.

One can see, that the interaction term in the conventional FKM includes only the local interactions and all nonlocal interactions are neglected. It is interesting to ask, however, if these nonlocal interactions are really unimportant and can be neglected or not. The possible improvement of the conventional FKM, which take into account also nonlocal interactions between nearest neighbors, is so-called correlated hopping term that describes how the occupancy of $`f`$ orbitals influences the hopping probability of $`d`$ electrons:

$$\stackrel{~}{t}_{ij}=t_{ij}+t_{ij}^{}(f_i^+f_i+f_j^+f_j).$$
(2)
The importance of the correlated hopping term has already been mentioned by Hubbard . Later Hirsch  pointed out that this term may be relevant in the explanation of superconducting properties of strongly correlated electrons. The effect of correlated hopping on the ground-state properties of the FKM has been examined recently by Gajek and Lemański in 1D  as well as Wojtkiewicz and Lemański in two dimensions . The same subject has been studied in our previous papers . Using finite-cluster diagonalization calculations we have showed that the picture of valence and metal-insulator transitions is dramatically changed if the term of correlated hopping is included. One of the most important results found for the one-dimensional FKM with correlated hopping was that the correlated hopping can induce the insulator-metal transition, even in the half-filled band case $`n_d=n_f=1/2`$ , where the ground state of the conventional FKM is insulating for all Coulomb interactions . In the present paper we go beyond this case and examine a more general point $`n_d+n_f=1`$, that is the point of the special interest for valence and metal-insulator transitions caused by promotion of electrons from localized $`f`$ orbitals $`(f^nf^{n1})`$ to the conduction band states.

Since in the spinless version of the FKM (1) with correlated hopping (2) the $`f`$ \- electron occupation number $`f_i^+f_i`$ of each site $`i`$ commutes with the Hamiltonian, the $`f`$-electron occupation number is a good quantum number, taking only two values: $`w_i=1`$ or 0, according to whether or not the site $`i`$ is occupied by the localized $`f`$ electron. Therefore the Hamiltonian of the FKM with correlated hopping can be rewritten as

$$H=\underset{ij}{}h_{ij}(w)d_i^+d_j+E_f\underset{i}{}w_i,$$
(3)
where $`h_{ij}(w)=\stackrel{~}{t}_{ij}(w)+Uw_i\delta _{ij}`$ and

$$\stackrel{~}{t}_{ij}(w)=t_{ij}+t_{ij}^{}(w_i+w_j).$$
(4)
Thus for a given $`f`$-electron configuration $`w=\{w_1,w_2,\mathrm{},w_L\}`$ the Hamiltonian (3) is the second-quantized version of the single-particle Hamiltonian $`h(w)`$, so the investigation of the model (3) is reduced to the investigation of the spectrum of $`h`$ for different configurations of $`f`$ electrons. This can be performed exactly (over the full set of $`f`$-electron configurations) or approximatively (over the incomplete set, but still kipping the high precision of calculations). Here we adopt the second method since it allows us to treat several times larger lattices and so to minimize finite-size effects.

## 2 The method

The method used in this paper to study effects of correlated hopping on ground-state properties of the FKM is a simple modification of the finite-cluster exact-diagonalization method. This method was used firstly by one of us to describe the ground-state phase diagram (in $`E_f`$ \- $`U`$ plane) of the conventional FKM in one and two dimensions . It was shown that the method is able to reproduce satisfactorily the exact results even after a relatively small number of iterations for both, one and two dimensions. The method is relatively simple and consists of the following steps: (i) Chose a trial configuration $`w=\{w_1,w_2,\mathrm{},w_L\}`$. (ii) Having $`w`$, $`U`$, $`t^{}`$ and $`E_f`$ fixed, find all eigenvalues $`\lambda _k`$ of $`h(w)=T+UW`$. (iii) For a given $`N_f=_iw_i`$ determine the ground-state energy $`E(w)=_{k=1}^{LN_f}\lambda _k+E_fN_f`$ of a particular $`f`$-electron configuration $`w`$ by filling in the lowest $`N_d=LN_f`$ one-electron levels. (iv) Generate a new configuration $`w^{}`$ by moving a randomly chosen electron to a new position which is chosen also at random. (v) Calculate the ground-state energy $`E(w^{})`$. If $`E(w^{})<E(w)`$ the new configuration is accepted, otherwise $`w^{}`$ is rejected. Then the steps (ii)-(v) are repeated until the convergence (for given $`U`$ and $`E_f`$ ) is reached.

Of course, one can move instead of one electron (in step (iv)) two or more electrons, the convergence of the method can thereby be improved. Indeed, tests that we have performed for a wide range of the model parameters showed that the latter implementation of the method, in which $`1pp_{max}`$ electrons ($`p`$ should be chosen at random) are moved to new positions, overcomes better the local minima of the ground-state energy. This also improves the accuracy of the method. Moreover, we have found that the method convergence depends sensitively on model parameters and selected values of $`p_{max}`$. Thus the first step in our numerical calculations was to find the optimum value of $`p_{max}`$ for the intermediate interactions, the case studied in this paper. In particular, we have tested the convergence of method for $`U=2`$ and four selected values of $`p_{max}`$, and namely, $`p_{max}=1,2,3`$ and $`N_f`$. The results of numerical calculations are summarized in Fig. 1, where the quantity $`M_0`$ (the minimal number of iterations for which the exact ground state for given $`L`$ is reached) is plotted as a function of $`1/L`$. It is seen, that selected $`p_{max}`$ strongly influence the method convergence, especially for large $`L`$, where the cases $`p_{max}=1`$ and $`p_{max}=N_f`$ need several times larger number of iterations than the cases $`p_{max}=2`$ and $`p_{max}=3`$. Therefore, we chose the case $`p_{max}=2`$ for the numerical calculations in the intermediate region.

## 3 Results and discussion

The main aim of this paper is to answer the question, how the correlated hopping influences ground-state properties of the one-dimensional FKM in the symmetric case ($`E_f=0,n_f+n_d=1`$). In particular, the influence of $`t^{}`$ on valence transitions and conducting properties of the model was studied. We present results for two selected values of the Coulomb repulsion interaction, namely $`U=1`$ and $`U=2`$. The value $`U=1`$ represents the typical behavior of the system for weak interactions and the value $`U=2`$ represents the behavior of the system for intermediate and strong interactions. The ground states were studied exactly on the finite clusters consisting of $`L=12,16,20`$ and $`24`$ lattice sites, while for larger lattices (up to $`L=120`$) the approximate method, discussed above, was used. It is well-known, that the $`f`$-electron density ($`n_f`$) for the symmetric FKM without correlated hopping is equal to $`1/2`$ and the system is an insulator for all $`U>0`$ . It is interesting to ask, if the non-zero correlated hopping can change this picture.
$`𝐔=\mathrm{𝟏}`$
To examine the influence of correlated hopping on the valence transition we have performed an exhaustive study of the model on finite clusters (up to $`L=60`$) for $`t^{}`$ ranging from $`2`$ to $`2`$ with step $`0.02`$. Results of numerical calculations are displayed in Fig. 2 for three selected clusters ($`L=24,48`$ and $`60`$) and they clearly demonstrate the strong effects of correlated hopping on the valence transitions. For each of these lattices $`n_f`$ exhibits the same characteristic features: (i) On the interval $`[0.38,0.4]`$ the $`f`$-electron concentration is equal to $`0.5`$ (like for the conventional FKM). (ii) Below $`t^{}=0.38`$ the $`f`$-electron occupation number increases. (iii) Above $`t^{}=0.4`$ the $`f`$-electron density rapidly falls down from $`n_f=0.5`$ to $`n_{f_{min}}0.25`$ and then gradually increases. Due to the fact that we have considered finite (although relatively large) lattices the valence transitions have a stair-case structure, which is gradually suppressed with increasing $`L`$, of course with the exception of the stair at $`t^{}=0.4`$ that seems to be independent of $`L`$. A detailed analysis showed (see Fig. 2d) that the valence transition from $`n_f=1/2`$ to $`n_{f_{min}}1/4`$ is not discontinuous, but it is realized through the consecutive intermediate-valence transitions (on the interval $`[0.4,0.44]`$) followed by continuous changes of $`n_f`$ ($`L\mathrm{}`$) for $`t^{}>0.44`$. The similar behavior was observed also for negative $`t^{}`$ ($`t^{}<0.38`$).

Moreover, our numerical results showed that there are three critical values of $`t^{}`$ where $`n_f`$ changes its character. For negative values of correlated hopping $`t_{c_1}^{}0.38`$ was observed. For $`t^{}>0`$ two critical values of correlated hopping $`t_{c_2}^{}0.4`$ and $`t_{c_3}^{}0.54`$ were found. The numerical results showed that the ground state between $`t_{c_1}^{}`$ and $`t_{c_2}^{}`$ is the alternating configuration. For $`t^{}>t_{c_3}^{}`$ the ground states are the segregated configurations with different $`N_f`$. Between $`t_{c_2}^{}`$ and $`t_{c_3}^{}`$ a few configuration types are stable:

* The most homogeneous configurations with $`N_f<L/2`$.
* The mixtures of the alternating configuration ($`w_a`$) and the empty configuration ($`w_0`$).
* The mixtures of the empty configuration ($`w_0`$) and some periodic configurations ($`w_p`$) (e.g. $`w_{(L=20)}=\{11101110000000000000\}`$).
* Around the boundary of two configuration types $`w_A`$, $`w_B`$ mixtures $`w_A\&w_B`$ are observed.

The ground-state configurations for $`t^{}<t_{c_1}^{}`$ but near $`t_{c_1}^{}`$ are the most homogeneous configurations with $`N_f>L/2`$ and for smaller values of $`t^{}`$ there are the mixtures of the alternating configuration ($`w_a`$) and the fully occupied configuration ($`w_1`$). Lastly, mixtures of periodic configurations and the alternating configuration ($`w_p\&w_a`$) are observed.

Since the ground states of the FKM with correlated hopping consist of configurations which are different from the alternating configuration (that is the ground state for the conventional FKM) it is natural to expect that the correlated hopping will change also the conducting properties of the model. To verify this conjecture the energy gap ($`\mathrm{\Delta }=\lambda _{LN_f+1}\lambda _{LN_f}`$) at the Fermi level was calculated for different finite clusters. Fig. 3 shows the energy gap on the interval $`t^{}=[2,2]`$ for two clusters of $`L=36`$ and $`48`$ sites at $`U=1`$. In the region where the alternating phase is the ground state the gap $`\mathrm{\Delta }`$ has a finite value ($`\mathrm{\Delta }=U`$) independent of $`L`$, and so the system is an insulator. This conclusion is identical with the conventional FKM ($`t^{}=0`$). At $`t^{}0.4`$ the energy gap changes from $`\mathrm{\Delta }=U`$ to $`\mathrm{\Delta }U/2`$ for both examined lattices (the inset in Fig. 3). The detailed analysis showed that the most homogeneous configurations are the ground states for $`t^{}`$ between $`t^{}0.4`$ and $`t^{}0.44`$ where $`\mathrm{\Delta }U/2`$. The extrapolation of the finite-cluster results to the thermodynamic limit at $`t^{}=0.42`$ confirmed, that the energy gap has a finite value for $`L\mathrm{}`$ and the system is really an insulator in this region (Fig. 4). On Fig. 4 we plotted also extrapolated results for three other positive values of $`t^{}`$ ($`t^{}=0.5,0.55`$ and $`2`$). Their fits obviously converge to zero (the metallic state) indicating that the correlated hopping induces the insulator-metal transition at $`t^{}0.44`$. To find the complete picture of metal-insulator transitions in the FKM with correlated hopping we have performed also an exhaustive study of the model for a wide region of negative values of $`t^{}`$ ($`t^{}[2,0.38]`$). A similar behavior of the model has been observed. For $`t^{}`$ between $`t^{}0.5`$ and $`t^{}0.38`$, where the ground states are the most homogeneous configurations, the energy gap has a finite value $`\mathrm{\Delta }U/2`$, while for $`t^{}`$ between $`t^{}1`$ and $`t^{}0.5`$ the energy gap vanishes in the thermodynamic limit. This is illustrated in Fig. 5, where the energy gap $`\mathrm{\Delta }`$ is plotted for several values of $`t^{}`$ as a function of $`1/L`$. The comprehensive picture of insulator-metal transitions in the thermodynamic limit obtained from extrapolated behaviors is displayed in Fig. 6 and clearly demonstrates that the correlated hopping dramatically changes the conducting properties of the model. In addition to an insulating phase, which characterizes the conventional FKM, the large metallic phases are found for the FKM with correlated hopping. The metallic phases are observed for positive and also for negative $`t^{}`$. For $`t^{}>0`$ there exists the wide metallic region above $`t^{}0.44`$ and for $`t^{}<0`$ there exists the wide metallic region, between $`t^{}1`$ and $`t^{}0.5`$. For positive as well as negative $`t^{}`$ the transition from the insulating to metallic phase realizes through two discontinuous transitions. The first is the insulator-insulator transition from $`\mathrm{\Delta }=U`$ to $`\mathrm{\Delta }U/2`$ and the second is the insulator-metal transition from $`\mathrm{\Delta }U/2`$ to $`\mathrm{\Delta }=0`$. Unfortunately, we were not able to determine the type of transition (continuous or discontinuous) at $`t^{}1`$. The finite-size effects near this transition point are still large, and so it was very difficult to do definite conclusions concerning the transition type. Our results only indicate that the transition at $`t^{}1`$ is probably continuous.
$`𝐔=\mathrm{𝟐}`$
The same procedure as for $`U=1`$ has been used also for $`U=2`$. As was mentioned above this value represents the typical behavior of the system for intermediate and strong interactions. Again we have performed a study of the model on finite clusters (up to L = 60) for $`t^{}`$ running from $`2`$ to $`2`$ with step $`0.02`$. Fig. 7a shows the valence transition for the cluster with $`L=48`$ sites, which qualitatively describes $`n_f`$ for this interaction case. It is seen, that the valence transition has a similar character as for $`U=1`$. In particular, there exists the region (between $`t_{c_1}^{}0.78`$ and $`t_{c_2}^{}0.66`$), where the $`f`$-occupation number is constant and equal to $`1/2`$. Below $`t_{c_1}^{}`$ the $`f`$-electron occupation number increases from $`n_f=0.5`$, and above $`t_{c_2}^{}`$ the $`f`$-electron density rapidly falls down from $`n_f=0.5`$ to $`n_{f_{min}}0.42`$ and then gradually increases, similarly as for $`U=1`$. However, there is one important difference. The detailed analysis performed on finite clusters up to $`L=60`$ showed, that the valence transition at $`t_{c_2}^{}`$ changes discontinuously from $`n_f=0.5`$ to $`n_{f_{min}}0.42`$. Moreover, comparing the valence transitions for $`U=1`$ and $`U=2`$ one can see, that the stronger Coulomb interaction needs the larger $`t^{}`$ (in the absolute value) to change the ground state from $`n_f=1/2`$ to another $`n_f`$.

Also for this case, we have tried to describe the ground-state configurations. Although the phase diagram is very complex we were able to describe the basic configuration types. Between $`t_{c_1}^{}`$ and $`t_{c_2}^{}`$ the alternating configuration is the ground state for all investigated lattices. For $`t^{}>t_{c_2}^{}`$ the ground states are the segregated configurations with different $`N_f`$. Below $`t_{c_1}^{}`$ we were able to specify several configuration types with the significant stability regions. In particular:

* The most homogeneous configurations with different $`N_f>L/2`$.
* The mixtures of the alternating configuration ($`w_a`$) and the fully occupied configurations ($`w_1`$) of different length.
* The mixtures of the alternating configuration ($`w_a`$) and periodic configurations ($`w_p`$).

To calculate the energy gap for $`U=2`$ the same procedure, the extrapolation of finite-cluster calculations (up to $`L=120`$), was used. The extrapolated values of the energy gap are plotted in Fig. 7b as a function of $`t^{}`$. Comparing the energy gaps for $`U=1`$ and $`U=2`$ (Fig. 6 and Fig. 7b), one can see that they exhibit qualitatively same behaviors. In particular, there is the wide insulating region around $`t^{}=0`$, two wide metallic regions (one for positive and one for negative $`t^{}`$) and the insulating region below the metallic one for negative $`t^{}`$. On the other hand, the careful analysis showed one important difference between the case $`U=1`$ and $`U=2`$. Namely, for $`U=2`$ and $`t^{}>0`$ the system undergoes discontinuous insulator-metal transition from $`\mathrm{\Delta }=U`$ to $`\mathrm{\Delta }=0`$, while for $`U=1`$ the system undergoes two discontinuous transitions (the insulator-insulator transition from $`\mathrm{\Delta }=U`$ to $`\mathrm{\Delta }U/2`$ and the insulator-metal transition from $`\mathrm{\Delta }U/2`$ to $`\mathrm{\Delta }=0`$). Moreover, one can see that with increasing $`U`$ the metallic regions shift to larger values (in the absolute value) of correlated hopping.

Thus we can conclude that the correlated hopping $`t^{}`$ plays the crucial role in description of the ground-state properties of the spinless FKM in 1D. The non-zero values of $`t^{}`$ substantially change the valence transitions as well as the conducting properties of the model (in comparison with the conventional FKM). For the valence transitions it was found that the relatively small values of $`t^{}`$ can induce the large changes of $`n_f`$ and these changes can be continuous as well as discontinuous. However, the most important result is that the correlated hopping can induce the insulator-metal transitions in the FKM for both positive and negative values of $`t^{}`$. These results clearly show that the correlated hopping strongly influences the ground-state properties of the FKM and so it should not be neglected in the correct description of real materials with correlated electrons. Of course, to do a direct comparison with experimental measurements one has to study FKM with correlated hopping in large dimensions. Work on this subject is currently in progress.
Acknowledgments
This work was partially supported by the Slovak Grant Agency VEGA under Grant No. 2/3211/23 (P.F.) and the Science and Technology Assistance Agency under Grant APVT-20-021602 (H.C.). Numerical results were obtained using computational resources of the Computing Centre of the Slovak Academy of Sciences.

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# SN 2002lt and GRB 021211: a SN/GRB Connection at 𝑧=1

## 1 Introduction.

After long years of study, we have now some convincing evidence that long-duration gamma-ray bursts (GRBs) are produced by the death of a massive star. The earliest hint was the spatial and temporal coincidence between SN 1998bw and GRB 980425 (at $`z=0.0085`$; Galama98 ). However, this association was hardly representative of the whole class of GRBs: GRB 980425 was indeed a very dim event, its gamma-ray energy being lower than that of classical GRBs by $`4`$ orders of magnitude. SN 1998bw was also a peculiar event, belonging to the class of the so-called ‘hypernovæ’: it showed unusual expansion velocities and a very high luminosity, the latter being the effect of copious Nickel production (see e.g. Nomoto00 ).

Very recently, however, SN 2003dh was discovered associated with GRB 030329 (Stanek03 ; Hjorth03 ; Matheson03 ). An intensive spectral monitoring showed a strict similarity between SN 2003dh and SN 1998bw, thereby conclusively proving that hypernovæ can generate classical GRBs. SN 2003dh was however somewhat fainter than SN 1998bw (Mazzali03 ).

We present here photometric and spectroscopic observations highlightening the association between GRB 021211 and SN 2002lt (DV03 ). GRB 021211 (Crew03 ) was a rather dim event, its total (isotropic) gamma-ray energy being $`E_{\mathrm{iso}}=(6\pm 0.5)\times 10^{51}`$ erg, at the low end of the energy distribution of GRBs (Frail01 ). Prompt optical observations allowed an early discovery of the optical afterglow, just few minutes after the GRB onset (e.g. Li03 ; Fox03 ). The afterglow also turned out to be quite faint, about 3 magnitudes in the $`R`$ optical band. The redshift was determined to be $`z=1.006`$ (Vreeswijk02 ). Optical/NIR colors showed little or no extinction local to the host galaxy. The intrinsic faintness of the afterglow made this event a good candidate for searching a supernova component.

## 2 Data and analysis

We observed the optical afterglow of GRB 021211 with the ESO VLT–UT4 equipped with the FORS 2 instrument, during the period January – March 2003 (20 – 100 days after the GRB). Low-resolution spectroscopy was performed on Jan 8.27 UT.

Photometric data show a rebrightnening of the afterglow starting $`15`$ days after the burst (Fruchter02 ) and reaching the maximum, $`R24.5`$, during the first week of January. The contribution of the host galaxy, estimated from our late-epoch images, is $`R=25.22\pm 0.10`$. Therefore, the intrinsic magnitude of the bump was $`R=25.24\pm 0.38`$. The significance of the rebrightening is at the 4-$`\sigma `$ level. At the time of the maximum, the afterglow contribution, extrapolated from earlier epochs, is smaller than $`5\%`$ under the most conservative assumptions. This suggests that the bump is powered by some different component.

To investigate the nature of the rebrightening, we obtained a spectrum with VLT+FORS 2. The reduced spectrum covered the range of wavelengths $`(60009000)`$ Å at an acceptable S/N ($`>3`$). The resolution was about 19 Å, and the integration time was $`4\times 1`$ h with a seeing of $`0^{\prime \prime }.6`$$`1^{\prime \prime }.4`$. We confirm the detection of the emission line at $`\lambda =7472.9`$ Å (Vreeswijk02 ), which may be interpreted as \[O II\] 3727 Å in the rest frame, leading to a determination of the redshift $`z=1.006`$.

Fig. 2 shows our spectrum smoothed and cleaned from the emission line \[O II\]. The spectrum of the afterglow is characterized by broad low-amplitude undulations blueward and redward of a broad absorption, the minimum of which is measured at $`3770`$ Å (in the rest frame of the GRB), whereas its blue wing extends up to $`3650`$ Å. The absorption feature in our spectrum is a characteristic signature of the SN ejecta (see SN 1991bg and SN 1994I in Fig. 2) and it is due to Ca II H+K absorption lines. The blueshifts corresponding to the minimum of the absorption and to the edge of the blue wing imply velocities of $`v\mathrm{14\hspace{0.17em}400}`$ km/s and $`v\mathrm{23\hspace{0.17em}000}`$ km/s respectively. The more convincing resemblance is found with SN 1994I, a prototypical type-Ic event, 9 days after its $`B`$-band maximum (Filippenko95 ). It is difficult to explain such broad absorption feature in terms of other components. It was argued that the telluric absorption at $`7600`$ Å can contaminate, by chance, the absorption feature. Fig. 3 shows that even in the case that the subtraction of the telluric line was not effective (which is not the case), its profile cannot reproduce the broad and double-structured deep in the spectrum. Also in Fig. 3 the position of the rest-frame Ca H+K absorption lines is marked (crosses), showing that no contamination comes from the host galaxy.

## 3 Implications

The spectroscopic features observed during the rebrightening of the afterglow of GRB 021211 and the similarity of its lightcurve with the one of SN 1994I indicate that the bump was indeed powered by a supernova. This is therefore the third GRB (second in chronological order) for which a SN association was spectroscopically confirmed. The IAU dubbed this event SN 2002lt (DV03b ). SN 2001ke and GRB 011121 are another possible case of SN/GRB association, although no ‘typical’ SN features have been detected in the spectrum (Garnavich03 ).

Supernova dating. Using SN 1994I as a template, our photometric and spectroscopic data allow us to estimate the time at which the SN exploded, and to compare it with the GRB onset time. Due to the limited wavelength coverage and to the lack of multi-time spectroscopic observations, our spectrum yields only a shallow contrain, suggesting that the SN went off between $``$50 and 0 days before the GRB (see Fig. 4).

Information from the photometry yields more stringent limits. After assuming SN 1994I as a template, the best match is achieved if the SN and the GRB exploded simultaneously or separated, at most, by a few days. We stress however that also in this case the dataset is not rich enough to set firm bounds. Moreover, this result also depends upon the assumed rising time of the template SN, which was quite short ($``$12 days) for SN 1994I (Iwamoto94 ).

GRB progenitor. It is also interesting to note that SN 1994I, the spectrum of which provides the best match to that observed in GRB 021211, is a typical type-Ic event rather than an exceptional 1998bw-like object, as the one proposed for association with GRB 980425 and GRB 030329 (Galama98 ; Stanek03 ; Hjorth03 ). If the SN associated with GRB 021211 indeed shared the properties of SN 1994I, this would open the interesting possibility that GRBs may be associated with standard type-Ic SNe, and not only with the more powerful events known as ‘hypernovæ’. However, we should note that the recently studied SN 2002ap (Mazzali02 ) showed significantly broader lines than our case and this difference vanished after maximum, such that it may be not easy to distinguish between the two types of SNe.


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# Orbital and Spin contributions to the 𝑔-tensors in metal nanoparticles

## I Introduction

The difference in energy between the eigenvalues for the two spin states of an isolated electron in an external magnetic field $`B`$ is $`g_0\mu _\mathrm{B}B`$, where $`\mu _\mathrm{B}`$ is the Bohr magneton and $`g_0`$ is the so-called $`g`$-factor for an isolated electron. If we ignore quantum electrodynamical corrections, it follows from the one-particle Dirac equation that $`g_0=2`$. In an infinite crystal in the absence of external magnetic fields, time-reversal symmetry dictates that each electron Bloch state, labeled by $`𝐤`$, is doubly degenerate (Kramer’s degeneracy), provided that the crystal has inversion symmetryKittel (1987). This degeneracy is lifted by a magnetic field $`B\widehat{B}`$, and the energy difference between the two states can be expressed by means of a symmetric, $`3\times 3`$, “$`g`$-tensor”, $`𝒢_𝐤`$Slichter (1963)

$$\mathrm{\Delta }ϵ_𝐤=\mu _\mathrm{B}B\left(\widehat{B}^T𝒢_𝐤\widehat{B}\right)^{1/2}.$$
(1)
The tensor $`𝒢_𝐤`$ is related to the total magnetic moment of the state $`𝐤`$ (see below)

$$\mu _\mathrm{B}\stackrel{}{\mu }_𝐤=\mu _\mathrm{B}\stackrel{}{L}_𝐤+\mu _\mathrm{B}g_0\stackrel{}{S}_𝐤.$$
(2)
Here $`\mu _\mathrm{B}\stackrel{}{L}`$ and $`\mu _\mathrm{B}g_0\stackrel{}{S}`$ are the orbital and spin magnetic moments. The brackets $`\mathrm{}_𝐤`$ denote the expectation value in the $`𝐤`$-state. In the absence of spin-orbit interactions, the orbital angular momentum is quenched, and only the spin magnetic moment contributes to the level splitting. In this case the Kramer doublet is composed of two (opposite) pure spin states and the tensor $`𝒢_𝐤`$ is isotropic, $`(𝒢_𝐤)_{ij}=4\delta _{ij}`$. It follows that the $`g`$-factor for a magnetic field in the $`z`$ direction, defined as the square root of the tensor element $`(𝒢_𝐤)_{zz}`$, is equal to the free electron $`g_0`$. The effect of spin-orbit coupling is fourfold: (i) because the states forming a Kramer doublet are no longer pure spin states, their average spin is less than $`1/2`$, which tends to decrease the typical $`g`$-factor; (ii) the orbital angular momentum is no longer quenched and the corresponding magnetic moment can contribute to the level splitting, either by decreasing or increasing $`g`$; (iii) the tensor structure of $`𝒢`$ is non-trivial (i.e. the response to a magnetic field is anisotropic and does not in general lead a moment aligned with the field); (iv) $`𝒢_𝐤`$ can vary strongly with $`𝐤`$. In bulk metals direct measurement of electron $`g`$-factors can be obtained only via conduction electron spin resonance (CESR) experiments. CESR involves transitions between states of the electron continuum. The two quantities measured in these experiments are the position of a resonance line, that is the average $`g`$-factor of the conduction electrons, over the Fermi surface, $`g_{\mathrm{av}}`$, and the linewidth, corresponding to the spin relaxation time $`\tau _{\text{so}}`$. In case of weak spin-orbit interaction the $`g`$-factor shift $`\mathrm{\Delta }gg_{\mathrm{av}}g_0`$ can be evaluatedElliott (1954) perturbatively in the spin-orbit coupling constant $`\xi `$, $`\mathrm{\Delta }g\xi /W`$, where $`W`$ is the band width. Since $`W>>\xi `$, the effect of spin-orbit interaction on bulk $`g`$-factors is expected to be small, even for heavy elements like gold. Indeed experimentally $`g_{\mathrm{av}}`$ in Al is essentially equal to $`g_0`$, while for Au $`g_{\mathrm{av}}=2.1`$. When evaluated perturbatively, the spin relaxation time $`\tau _{\text{so}}`$ can be related to $`\mathrm{\Delta }g`$ and to the “resistivity” relaxation time $`\tau _r`$ through the Elliott relationElliott (1954), $`\frac{1}{\tau _{\text{so}}}=\frac{\mathrm{\Delta }g^2}{\tau _r}`$. This relation shows that scattering off impurities, surfaces, and phonons, which determine $`\tau _r`$, affects indirectly $`\tau _{\text{so}}`$, although the mechanism responsible for the spin relaxation is the spin-orbit interaction, which is essentially atomic in character.

In this paper we focus on the $`g`$-factors for electrons confined inside a metal grain of nanometer size, where the quantum energy spectrum is discrete and its individual quasiparticle energy levels $`ϵ_n`$ can be directly observed at low temperatures. By replacing the Bloch index $`𝐤`$ with the discrete quasiparticle orbital index $`n`$, equations (1) and (2) describe how a Kramer doublet splits in a magnetic field. In contrast to the bulk case, the effects on the spin-orbit interaction on $`g`$ – summarized in (i)-(iv) above – is expected to be enhanced, since the relevant energy scale with which the spin-orbit coupling strength $`\xi `$ should be compared is not $`W`$ but the much smaller single-particle mean-level spacing $`\delta `$. In fact quantum finite-size effects on $`g`$-factors in ensembles of metal nanoparticles have been investigated in the past experimentally via CESR. (For a review see Ref. Halperin, 1986 and references therein.) To the best of our knowledge though, these experiments are riddled with many puzzling features, which make their comparison with proposed theoriesKawabata (1970); Buttet et al. (1982) very difficult. Furthermore in none of these experiments is there sufficient detail to extract information concerning statistical distribution of $`g`$-factors (see point (iii) above ). On the other hand, two groupsSalinas et al. (1999); Davidovic and Tinkham (2000); Petta and Ralph (2001, 2002), using tunneling spectroscopy in single-electron transistors, have recently succeeded in measuring $`g`$-factors of individual quasiparticle levels of a single metal nanoparticle. Measured $`g`$-factors ranged from 0.1 to 2, depending on material, grain size and doping; $`g`$-factors displayed large level-to-level fluctuations and strong dependence on the orientation of the applied magnetic field. Clearly $`g`$-factors in small metal grains measured by single-electron spectroscopy have little in common with bulk $`g`$-factors measured by CESR.

The statistical properties and mesoscopic fluctuations of $`g`$-factors measured experimentally in Refs. Salinas et al., 1999; Davidovic and Tinkham, 2000; Petta and Ralph, 2001, 2002 are well described by theoretical distributions based on Random Matrix Theory (RMT), derived by two independent groupsBrouwer et al. (2000); Matveev et al. (2000); Adam et al. (2002). There is however a longstanding puzzle in the comparison between this theory and experiment. The $`g`$-tensor distributions obtained from RMT are normalized to the average $`(g^2)^{1/2}`$, which has to be evaluated by independent arguments. In the regime of strong spin-orbit interaction, the two theoretical modelsMatveev et al. (2000); Adam et al. (2002) predict $`g^2`$ to have contributions from both spin and orbital magnetic moments

$$g^2=\frac{3}{\pi \mathrm{}}\tau _{\text{so}}\delta +\alpha \frac{l}{R},$$
(3)
where $`l`$ is the elastic mean free path, $`R`$ is the size of the particle and $`\alpha `$ is a constant of order 1111In Ref. Adam et al., 2002 Eq. (3) was derived by including explicitly a phenomenological orbital term in the RMT Hamiltonian; whereas in Ref. Matveev et al., 2000 this equation was derived by expressing $`g^2`$ and the energy absorption in a time-dependent magnetic field in terms of the same phenomenological RMT parameter.. In the limit of strong spin-orbit scattering $`\tau _{\text{so}}\delta 0`$, the spin contribution vanishes and only the orbital contribution $`\alpha (l/R)(L_z)^2`$ survives. The nanoparticles studied in Refs. Petta and Ralph, 2001, 2002 are not disordered and therefore $`lR`$. Thus Eq. (3) predicts that $`g^2`$ should never be much less than 1. In noble-metal nanoparticles, however, the measured values of $`g^2`$ are typically between 0.05 and 0.1.

RMT is a phenomenological approach which assumes that the statistical properties of interest depend only on the symmetry of the Hamiltonian. This assumption, although appealing and reasonable, is usually difficult to justifies rigorously. This fact, together with the discrepancy between theoryMatveev et al. (2000); Adam et al. (2002) and experiment mentioned above, motivates the theoretical study of $`g`$-factors in metal nanoparticles presented here. Our investigation is based on a semi-realistic microscopic tight-binding model that we solve numerically.

From the comparison between RMT and our microscopic theory we are able to shed some light on the discrepancy between the experimental measurements of $`g^2`$ and the value predicted in Refs. Matveev et al., 2000; Adam et al., 2002. The results of our model are in agreement with most of the RMT conclusions as to the functional form of the $`g`$-tensor distribution and its dependence on the spin-orbit coupling strength. In particular we find that $`g`$-tensors are strongly anisotropic when the nanoparticle shape is not perfectly symmetric, and that this anisotropy originates from mesoscopic quantum fluctuations of the nanoparticle wavefunctions. However, we are able to go beyond RMT, in that our more detailed analysis allows us to clarify the role played by the orbital motion and demonstrate that its contribution to the average $`g`$-factor is very sensitive to the character of the quasiparticle wavefunctions. Based on these results we conclude that the small value of $`g^2`$ measured experimentally can be understood if the orbital angular momentum of the tunneling states, in contrast to the RMT assumptions, is still partially quenched.

The paper is organized as follows. In Sec. II we introduce and discuss our model, with particular emphasis on the coupling between orbital motion and external field. In Sec. III we illustrate our numerical results, we compare them with RMT predictions, and we discuss their implications for the interpretation of the tunneling spectroscopy experiments. A summary and concluding remarks are presented in Sec. IV.

## II Model

We model the nano-particle as a truncated fcc crystal lattice with $`N_a`$ atoms. The shape of the system can be arbitrarily varied to simulate the variability of realistic nanoparticles. A $`spd`$ tight-binding-model is used with 18 orbitals at each atomic site, including the spin degrees of freedom.

The Hamiltonian,

$$=_{\mathrm{band}}+_{\text{so}}+_{\mathrm{Zee}},$$
(4)
has been introduced in a study of the quasiparticle properties in ferromagnetic metal nanoparticlesCehovin et al. (2002). Here we give only a brief description of the terms in Eq.(4).

The first term $`H_{\mathrm{band}}`$ is an orbital part,

$$_{\mathrm{band}}=\underset{i,j}{}\underset{s}{}\underset{\mu _1,\mu _2}{}t_{\mu _1,\mu _2,s}^{i,j}c_{i,\mu _1,s}^{}c_{j,\mu _2,s}^{}$$
(5)
involving the Slater-Koster parameters Slater and Koster (1954), $`t_{\mu _1,\mu _2,s}^{i,j}`$. Atomic sites are labeled by $`i,j`$, and $`t^{i,j}`$ couples up to second nearest-neighbors. The indices $`\mu _1,\mu _2`$ label the nine distinct atomic orbitals (one $`4s`$, three $`4p`$ and five $`3d`$). The spin degrees of freedom, labeled by the index $`s`$, double the number of orbitals at each site.

The second term describes a spin-orbit interaction, essentially atomic in character

$$_{\text{so}}=\xi \underset{i}{}\underset{\mu ,\mu ^{},s,s^{}}{}i,\mu ,s|\stackrel{}{L}\stackrel{}{S}|i,\mu ^{},s^{}c_{i,\mu ,s}^{}c_{i,\mu ^{},s^{}}^{},$$
(6)
reflecting the fact that relativistic effects are important only when the electron is close to the nucleus. In spite of the local nature of these interaction, the effect of $`_{\text{so}}`$ on the spin-orbit relaxation time $`\tau _{\text{so}}`$, compared to non-disordered infinite systems, is strongly enhanced by the destruction of crystal symmetry due to the nanoparticle surface. This is, to a certain extent, similar to the mechanism described by the Elliott relation.

A quantitative measure of the relative strength of the spin-orbit interaction is given by the dimensionless parameter $`\lambda `$Brouwer et al. (2000)

$$\lambda ^2=\pi \frac{\mathrm{}}{\tau _{\text{so}}\delta }.$$
(7)
The spin-orbit scattering is strong if $`\lambda >>1`$ and weak if $`\lambda <<1`$. In the limit of weak spin-orbit interaction $`\tau _{\text{so}}`$ can be calculated perturbatively by Fermi golden rule. Here, however, we use a more pragmatic approach: we define $`\tau _{\text{so}}`$ in terms of the average spin-orbit quasiparticle energy shiftCehovin et al. (2002)

$$\mathrm{}\tau _{\text{so}}^1|ϵ_nϵ_n^0|,$$
(8)
where $`ϵ_n`$ and $`ϵ_n^0`$ is the $`n`$-th eigenvalue with and without spin-orbit interaction respectively and the average $`\mathrm{}`$ is performed over the spectrum of the nanoparticle222In the limit of weak spin-orbit scattering, this definition is equivalent to the Fermi golden rule result..

Since $`\tau _{\text{so}}`$ decreases weakly with particle size $`L`$, while $`\delta `$ varies as $`L^3`$, the effective strength of the spin-orbit interaction decreases with decreasing particle size. In the experiments of Ref. Petta and Ralph, 2001, 2002, containing up to several thousand atoms, $`\lambda `$ can be as large as $`10`$ for Au nanoparticles. In our theoretical studies we are able to deal numerically with nanoparticles containing only up to a few hundred atoms, which would yield $`\lambda <<1`$ for a realistic value of $`\xi 100`$ meV. In order to achieve larger $`\lambda `$ values we therefore artificially increase the spin-orbit coupling strength $`\xi `$. For a disordered dot of a generic shape our numerical results depend on the value of $`\lambda `$ but only weakly on the separate values of $`\xi `$ and $`\delta `$.

The Zeeman part $`_{\mathrm{Zee}}`$ in Eq. (4) is conveniently divided into two terms,

$$_{\mathrm{Zee}}=\mu _\mathrm{B}\underset{i}{}\stackrel{}{B}\left\{\underset{\mu ,\mu ^{},s,s^{}}{}i,\mu ,s|g_s\stackrel{}{S}+\stackrel{}{L}|i,\mu ^{},s^{}c_{i,\mu ,s}^{}c_{i,\mu ^{},s^{}}^{}\right\}+_{\mathrm{Zee}}^{\mathrm{NLOC}}$$
(9)
The first term of Eq. (9) is the usual atomic contribution already considered in our earlier paper Cehovin et al. (2002), arising from the space dependence of the vector potential on an atomic length scale. In addition to this, there is a second term, a non-local orbital contribution arising from the magnetic flux encompassed by closed loops describing the paths of an electron hopping from site to site. Only the latter term is accounted for in the RMT approach, whereas the former term has a larger importance in many respects. We discuss this contribution in detail in the next section.

### II.1 Non-Local Orbital Contribution (NLOC)

The NLOC originates from delocalized electrons in an external magnetic field. The coupling to an external magnetic field in tight-binding theory is accomplished by the introduction of the Peierls phases Peierls (1933); Luttinger (1951); Graf and Vogl (1995),

$$\mathrm{exp}(i\mathrm{\Theta }_{i,j})=\mathrm{exp}\left[\frac{ie}{\mathrm{}c}_{\stackrel{}{R}_i}^{\stackrel{}{R}_j}\stackrel{}{A}(x)𝑑\stackrel{}{x}\right]\mathrm{exp}\left[\frac{ie}{\mathrm{}c}\frac{(\stackrel{}{R}_j\stackrel{}{R}_i)(\stackrel{}{A}(\stackrel{}{R}_j)+\stackrel{}{A}(\stackrel{}{R}_i))}{2}\right],$$
(10)
modifying the Slater-Koster parameters so that,

$`_{\mathrm{Zee}}^{\mathrm{NLOC}}={\displaystyle \underset{i,j}{}}{\displaystyle \underset{s}{}}{\displaystyle \underset{\mu _1,\mu _2}{}}(\mathrm{exp}(i\mathrm{\Theta }_{i,j})1)t_{\mu _1,\mu _2,s}^{i,j}c_{i,\mu _1,s}^{}c_{j,\mu _2,s}^{}.`$ (11)
The non-trivial approximation of Eq. (10), replacing the contour integral with a simple line integral has been justified by Ismail-Beigi et al. Ismail-Beigi et al. (2001).

Choosing the vector potential in the symmetric gauge,

$$\stackrel{}{A}=\frac{1}{2}\stackrel{}{r}\times \stackrel{}{B},$$
(12)
the Peierls phases can be conveniently rewritten in a form suitable for perturbation theory purposes,

$$\mathrm{\Theta }_{i,j}=\frac{2\pi }{4\varphi _0}\left[(\stackrel{}{R}_j\stackrel{}{R}_i)\times (\stackrel{}{R}_i+\stackrel{}{R}_j)\right]\stackrel{}{B}.$$
(13)
The phase factor of Eq. (10) is expanded to first order in $`\stackrel{}{B}`$,

$$\mathrm{exp}(i\mathrm{\Theta }_{i,j})=1i\mu _B\stackrel{}{L}^{NLOC}\stackrel{}{B}+O(B^2),$$
(14)
where $`\stackrel{}{L}^{NLOC}`$ is defined as

$$i,\mu ,s|\stackrel{}{L}^{NLOC}|j,\mu ^{},s^{}=\frac{2\pi }{4\mu _B\varphi _0}\left[(\stackrel{}{R}_j\stackrel{}{R}_i)\times (\stackrel{}{R}_i+\stackrel{}{R}_j)\right].$$
(15)
This expansion allows one to write Eq. (9) to first order in (small) $`\stackrel{}{B}`$ in the familiar form

$`_{\mathrm{Zee}}`$ $`\mu _B`$ $`\stackrel{}{\mu }\stackrel{}{B}`$ (16)
$``$ $`\mu _\mathrm{B}`$ $`{\displaystyle \underset{i}{}}\left\{{\displaystyle \underset{\mu ,\mu ^{},s,s^{}}{}}i,\mu ,s|g_s\stackrel{}{S}+\stackrel{}{L}|i,\mu ^{},s^{}c_{i,\mu ,s}^{}c_{i,\mu ^{},s^{}}^{}\right\}\stackrel{}{B}`$ (17)
$``$ $`\mu _\mathrm{B}`$ $`{\displaystyle \underset{i,j}{}}\left\{{\displaystyle \underset{\mu ,\mu ^{},s,s^{}}{}}i,\mu ,s|\stackrel{}{L}^{NLOC}|j,\mu ^{},s^{}c_{i,\mu ,s}^{}c_{j,\mu ^{},s^{}}^{}\right\}\stackrel{}{B}.`$ (18)
We have explicitly checked that the Zeeman splitting due to the non-local interaction is gauge invariant in our numerical calculations, although the definition presented above is obviously for a particular gauge choice.

### II.2 Wannier states

The basis set, $`|j,\mu ,s`$, is to be interpreted as a set of Wannier orbitals, extracted Slater and Koster (1954) from bulk properties. The Slater-Koster parameters, $`t_{\mu _1,\mu _2,s}^{i,j}`$, are Hamiltonian matrix elements of $`|j,\mu ,s`$. Application of $`t_{\mu _1,\mu _2,s}^{i,j}`$ to a nano-particle relies on their transferability, the assumption of local electronic environmental insensitivity to the boundaries of the system. The success of this procedure depends on the nature of the states involved . In noble metals the electronic density of the $`sp`$-bands is delocalized, and very different from a simple sum of atomic densities. The corresponding Wannier orbitals lose their atomic-like character in this limit, and the transferability is expected to be less robust, since the boundary conditions play an increasingly important role. The orbitals, $`|j,\mu ,s`$, of $`sp`$-symmetry will thus have large hopping elements, a property expected to remain the same in any transferable tight-binding treatment of these states. The $`d`$-orbitals originate from bands of a different nature, with rather localized electronic densities around the atomic sites. The corresponding Wannier orbitals remain atomic-like and hopping parameters are small.

From these arguments it is immediately clear that the contribution from $`_{\mathrm{Zee}}^{\mathrm{NLOC}}`$ becomes increasingly important in the limit of extended Wannier states with large hopping parameters.

The eigenstates of this model are in general a mixture of all basis orbitals, $`|j,\mu ,s`$. An approximate separation of the eigenspectrum into bands of specific symmetries can still be made. For this purpose it is useful to define the projection operators, $`P_s,P_p`$ and $`P_d`$.

$`P_s`$ $`=`$ $`{\displaystyle \underset{i}{}}{\displaystyle \underset{s}{}}{\displaystyle \underset{\mu _s}{}}|i,\mu _s,si,\mu _s,s|,`$ (19)
$`P_p`$ $`=`$ $`{\displaystyle \underset{i}{}}{\displaystyle \underset{s}{}}{\displaystyle \underset{\mu _p}{}}|i,\mu _p,si,\mu _p,s|,`$ (20)
$`P_d`$ $`=`$ $`{\displaystyle \underset{i}{}}{\displaystyle \underset{s}{}}{\displaystyle \underset{\mu _d}{}}|i,\mu _d,si,\mu _d,s|,`$ (21)
with

$$P_s+P_p+P_d=1.$$
(22)
These operators project onto the subspaces of $`s`$, $`p`$ or $`d`$-symmetry. As an example, in Fig. (1) we plot the expectation values of these projection operator in the eigenstates $`|n`$ of the Hamiltonian of Eq. (4). The calculations are done for a 143 gold atom nanoparticle with hemispherical shape, from which 5 atoms have been removed to break the rotational symmetry. It is seen that states in the middle of the occupied band have well-defined $`d`$-character, with the exception of some states around $`n=700`$, which have mixed $`spd`$-components and low-energy states, which have mainly $`s`$-character. High-energy states far above the Fermi level have dominant $`p`$-character. States around the Fermi level are rather strongly mixed with the $`d`$-component decreasing sharply with eigenvalue number.

### II.3 $`g`$-tensor

In the absence of an external magnetic field, a nano-particle will have a doubly degenerate eigenspectrum, $`ϵ_n`$, reflecting the formation of Kramer pairs in a time-reversal symmetric system. In the presence of spin-orbit interaction, the Zeeman splittings, $`ϵ_nϵ_n\pm \delta ϵ_n`$, show anisotropic dependence on the direction of the applied field, $`\stackrel{}{B}`$. For small $`\stackrel{}{B}`$ this is conveniently described in terms of the $`g`$-tensor Slichter (1963),

$`\delta ϵ_n^2(\stackrel{}{B})`$ $`=`$ $`\left({\displaystyle \frac{\mu _B}{2}}\right)^2\stackrel{}{B}𝒢_n\stackrel{}{B}`$ (23)
$`𝒢_n`$ $`=`$ $`G_n^TG_n.`$ (24)
By using standard degenerate perturbation theory in $`_{\mathrm{Zee}}`$, the $`G_n`$ matrices can be related to the matrix elements of the (dimensionless) magnetic moment operator $`\stackrel{}{\mu }`$,

$`(G_n)_{1,j}+i(G_n)_{2,j}`$ $`=`$ $`2T\psi _n|\mu _j|\psi _n`$ (25)
$`(G_n)_{3,j}`$ $`=`$ $`2\psi _n|\mu _j|\psi _n.`$ (26)
Here $`|\psi _n`$ and $`|T\psi _n`$ are the time-reversed pair of eigenstates of $``$ in the absence of $`\stackrel{}{B}`$, corresponding to the eigenvalue $`ϵ_n^2`$. The diagonalization of $`𝒢_n`$, or in other words a suitable choice of coordinate system for the external field $`\stackrel{}{B}`$, allows one to write $`\delta ϵ_n(\stackrel{}{B})`$ in terms of the 3 eigenvalues $`g_j^2`$, $`j=1,2,3`$, of $`𝒢`$

$`\delta ϵ_n(\stackrel{}{B})={\displaystyle \frac{\mu _B}{2}}\sqrt{g_1^2B_1^2+g_2^2B_2^2+g_3^2B_3^2},`$ (27)
where $`B_j`$, $`j=1,2,3`$, are the components of the magnetic field along the “principal axis”, $`\widehat{e}_1,\widehat{e}_2,\widehat{e}_3`$, defined by the three normalized eigenstates of $`𝒢`$. We refer to $`g_j,j=1,2,3`$ as the principal $`g`$-factorsBrouwer et al. (2000). The Zeeman splittings, $`\delta ϵ_n(\stackrel{}{B})`$, can also be obtained from direct numerical diagonalization of the Hamiltonian for a given direction of $`\stackrel{}{B}`$. This approach is of course time demanding, but served as a check of the correctness of the perturbative approach, since the two methods should give identical results for small $`\stackrel{}{B}`$.

In the limit of zero spin-orbit interactions the three principal $`g`$-factors are identically equal to 2. In this case the Kramer pairs are pure spin states and the angular momentum is quenched. With the introduction of spin-orbit interaction spin characters mix, and non-zero orbital contributions Kravtsov and Zirnbauer (1992) to $`g_i`$ are expected. At weak spin orbit strength the spin character mixing is weak and the orbital contribution to $`g_i`$ is small. For large $`\lambda `$ the spin character mixing is strong, while orbital contributions are expected to increase.

## III Results and Discussion

In this section we present results of numerical calculations of $`g`$-tensors for $`Au`$-nanoparticles containing 143 atoms. Similar results, not shown here, were obtained for larger and smaller sizes. We first consider the distribution of principal-axis directions. Fig.(2a) shows calculated principal axis directions for a perfect hemisphere. The direction of $`\widehat{e}_i`$ is strongly dependent on the symmetry of the nanoparticle, with one axis always along the normal of the base plane. Due to the crystal fcc symmetry and the hemispherical truncation, the two remaining $`g`$-factors will be degenerate and two principal axes can be arbitrarily chosen within the base plane. This is shown in Fig.(2a), where we plot the direction of the principal axis directions on the unit sphere for all the quasiparticle orbitals of the nanoparticle. The situation changes dramatically with a small distortion of the shape obtained by removing five atoms from the hemispherical truncation. This slight breaking of the spherical symmetry produces a completely random distribution of principal axis, no longer preferentially aligned along crystalline or shape directions, as clearly seen in Fig. (2b). A random distribution of the principal axis directions was originally predicted by RMTBrouwer et al. (2000). Recent experiments Petta and Ralph (2002) measuring principal $`g`$-factors find random spatial orientation of the corresponding axis directions, $`\widehat{e}_i`$. The measurements were performed on Cu nanoparticles with approximately hemispherical shape. The results demonstrates that small irregularities in the boundaries in an otherwise ordered sample are enough to produce completely randomized directions, exactly as happens in our model.

Once the perfect axial symmetry of the hemispherical nanoparticle is broken, for example by removing a few atoms, we find that the numerical results depend weakly on the particle shape: nanoparticles with shapes that are even less symmetric display qualitatively similar distributions of principal $`g`$-factors. It turns out that the dimensionless spin-orbit strength $`\lambda `$, defined in Eqs. (7)-(8), is the crucial parameter that controls the distributions. A meaningful evaluation of $`\lambda (\xi )`$ for a given value of $`\xi `$ is however made complicated by the fact that states of different orbital character, as determined by the projection operators discussed above, yield very different values of $`\lambda `$ for the same $`\xi `$. Therefore we divide the eigenstates into two groups of states, which we refer to $`d`$\- and mixed states. An eigenstate is operationally considered a $`d`$-state if $`n|P_d|n>0.7`$; it is a mixed state otherwise. We will use this distinction extensively below. For a given value of $`\xi `$, the parameter $`\lambda `$ is then calculated separately for these two group of states. This procedure turns out to be very useful in the interpretation of our numerical results. A first example of this is shown in Fig. (3). In Fig. (3a) we plot $`\lambda (\xi )`$ as a function of $`\xi `$ for these two groups of states for a given nanoparticle. In both cases $`\lambda `$ increases approximately linearly with $`\xi `$, but the slope is much larger for the $`d`$-states. In Fig. (3b) we plot relative differences of the $`\lambda `$ for two nanoparticles with the same number of atoms ($`N_a=143`$) but very different shapes, again separating $`d`$\- and mixed states. Here $`\lambda _A`$ refers to a nanoparticle with hemispherical shape with 5 atoms removed; $`\lambda _B`$ refers to a nanoparticle with a strongly disordered shape. It is seen that $`\lambda `$ for the $`d`$ states is essentially the same for both nanoparticles for all values of $`\xi `$. On the other hand mixed states give a value of $`\lambda `$ that is more sensitive on the shape of the nanoparticle, although the relative difference is always less than $`10\%`$. It follows that the two nanoparticles will have very similar $`g`$-factor distributions, with a stronger shape dependence of the $`g`$-factor of mixed character states.

We now come to the discussion of the main results of our paper and to the comparison with RMT predictions. A very useful quantity for this comparison is the average of the sum of the squares of the principal $`g`$-factors

$$g^2=\frac{1}{3}g_1^2+g_2^2+g_3^2.$$
(28)
In Fig. 4 we plot $`g^2`$ as a function of $`\lambda `$ for a Au hemispherical nanoparticle with 5 atoms removed, separating again the contribution from $`d`$\- and mixed states. The results in Fig. 4(a) are for the case in which the spin term and both orbital terms are included in the magnetic moment of Eq. (2). As expected, $`g^24`$ in the limit $`\lambda 0`$ of zero spin-orbit coupling and decreases monotonically with increasing $`\lambda `$. In the limit of strong spin-orbit coupling, $`\lambda >>1`$, $`g^2`$ tends to a constant value, which is relatively small ($`0.3`$) for $`d`$-states but is of order 2 for mixed states. This saturation value in the strong spin-orbit scattering limit comes almost entirely from the non-local orbital contribution (NLOC) to the magnetic moment. Indeed Fig. 4(b) shows that that the saturation value is negligible when the NLOC is not included; in this case the $`g^2`$ vs. $`\lambda `$ for $`d`$\- and mixed states fall on the same curve which goes to zero like $`1/\lambda ^2`$ for large $`\lambda `$. Note that the large saturation value for mixed states, when the NLOC is present, is consistent with the fact that $`d`$-states are linear combination of atomic orbitals with small hopping parameters, whereas mixed states tend to be more free-electron like.

We found that the calculated $`g^2(\lambda )`$ could always be fit to

$$g^2(\lambda )=\frac{4\nu (\lambda )}{1+\lambda ^2}+6\eta ^2$$
(29)
in the entire range of $`\lambda `$. Here $`\eta `$ is a constant independent of $`\lambda `$, whereas $`\nu (\lambda )`$ is a function weakly dependent on $`\lambda `$ such that $`\nu (\lambda =0)=6\eta ^2`$ and $`\nu (\lambda )1`$ for $`\lambda >>1`$. In practice a reasonable fit (shown in the figure) is obtained by fixing $`\nu =6\eta ^2`$. Remembering the relationship between $`\lambda `$ and $`\tau _{\text{so}}`$ given in Eq. (7), we can see that Eq. (29) is perfectly consistent with the RMT predictionMatveev et al. (2000); Adam et al. (2002) in the strong spin-orbit scattering limit given in Eq. (3). The first term in Eq. (29) comes essentially from the spin contribution to the magnetic moment. The second term originates from orbital contributions and it has been written in this specific way to make contact with the the RMT phenomenological parameter $`\eta `$ that describes its coupling of the magnetic field to the orbital angular momentumAdam et al. (2002). The RMT parameter $`\eta ^2`$ can be estimated for specific physical systems by computing $`n|L_z^2|n`$ in the absence of spin-orbit couplingMatveev et al. (2000); Adam et al. (2002). For a ballistic sphere with diffusive boundary conditions one gets $`\eta ^2=1/8`$Matveev et al. (2000); Adam et al. (2002). Thus for no disorder RMT predicts for $`g^2`$ a saturation value $`1`$, which according to our model would correspond to the case of mixed states.

We can further analyze the relationship between RMT and our microscopic model by comparing the distribution of the three individual principal $`g`$-factors in different regimes of the spin-orbit coupling strength. In Fig. 5 and Fig. 6 we plot the distribution of $`g_1`$, $`g_2`$, and $`g_3`$ for $`d`$ and mixed states respectively. Translating into RMT language, Fig. 5 and Fig. 6 correspond to small and large orbital contribution respectively. The sub-cases (a), (b), (c) in each figure correspond to the regimes of weak, intermediate and strong spin-orbit scattering respectively. The values of $`\lambda `$ are chosen to compare with the cases considered in Refs. Brouwer et al., 2000; Adam et al., 2002. For weak spin-orbit interaction, we find that typically $`g_1g_2<2`$ and $`g_32`$ when the spin contribution to the $`g`$ tensor dominates (i.e. $`\eta <<\lambda `$ as in Fig.5(a) ). On the other hand, when the orbital contribution dominates the $`g`$-tensor ($`\eta >>\lambda `$ as in Fig.6(a) ), $`g_1<1`$, $`g_22`$, $`g_3>2`$. Both cases are in remarkable agreement with RMT predictionsBrouwer et al. (2000); Adam et al. (2002)

The trends of our numerical distributions for the cases of intermediate and strong spin-orbit scattering also agree with the RMT scenarioBrouwer et al. (2000). In particular in the strong spin-orbit scattering regime and for weak orbital contribution (see Fig. 5(c) ), all three principal $`g`$-factors are peaked at values smaller than 0.5. In this case, typical values of $`g`$ are always much smaller than the free electron value $`g_0=2`$.

We conclude this section by attempting a comparison between the results of our model and the experimental results of Ref. Petta and Ralph, 2002. In Table 1 we have summarized: (i) the experimental measurements of the average values of $`g_i,i=1,2,3`$, for two Cu nanoparticles–raws labelled by “Exp”; (ii) the RMT results, including spin contribution only–raws labelled by “RMT”; and (iii) the results of our calculations for $`d`$-states, including both spin and orbital contributions –raws labelled by “Here”333The calculations presented here are done on gold nanoparticles. Gold was one of the materials used in earlier $`g`$-factor experimentsPetta and Ralph (2001), which showed the same qualitative behavior for all noble-metal nanoparticles. Since all noble metals have similar electronic structures at the Fermi level, we expect our model to produce similar results for all them (Au, Ag and Cu), provided that we compare noparticles with the same relative spin-orbit interaction strength. As we explained in Sec.II, this strength is controlled by the parameter $`\lambda `$, which depends on the intrinsic spin-orbit coupling strength $`\xi `$ and the volume-dependent single-particle mean-level spacing. Here we use $`\xi `$ as a free parameter to generate different values of $`\lambda `$ and mimick particles of different sizes.. The procedure to extract these numbers is the following. First the value of $`\lambda `$ corresponding to a particular nanoparticle is obtainedPetta and Ralph (2002) by matching the RMT value of $`g^2`$ with the same quantity measured experimentally. Given this $`\lambda `$, the average values of the principal $`g`$-factors $`g_1`$, $`g_2`$, and $`g_3`$ can then be calculated theoretically by RMT. This was done in Ref. Petta and Ralph, 2002 and the results are reported in Table I. We can also compute the averages of $`g_i`$ within our microscopic model by choosing the parameter $`\xi `$ for a given nanoparticle so that the value of $`\lambda `$ obtained from Eqs. 7-8 is equal to the value extracted from the experiment using RMT. The averages predicted by the two theories (RMT and our macroscopic model) can then be compared with each other and with the values measured experimentally.

From the table one can see that RMT – with orbital contributions neglected – predicts average values of $`g_i`$ in good agreement with the experiments for two different $`\lambda `$’s corresponding to two different nanoparticles. The message that we want to convey here is that the average $`g`$ values of $`d`$-states predicted by our microscopic model, at the same nominal values of $`\lambda `$ defined through Eqs. 7-8, are also in good agreement with RMT and the experiments, even when the orbital contributions are included444In fact, RMT seems to agree even better with experiment than our theory. One possible reason is that the definition of $`\lambda `$ used in our model – see Eqs. 7-8– might differ by a constant factor from the RMR $`\lambda `$. Specifically in the two cases considered in Table I, our model would give a better agreement with experiment if we used a slightly smaller $`\lambda `$.. Thus our resuls suggests a scenario, namely $`g`$-factor distributions of states of mainly $`d`$ character, which, if realized, would solve the puzzle posed by the comparison between RMT and experiment. Note that RMT is based on a picture of single-particle wavefunctions essentially ergodic in space and it is therefore unable to capture the nature of wavefunctions more localized around atomic cores or defects, which instead are naturally described within our tight binding model.

The problem with the scenario proposed here is that the Fermi level for noble-metal nanoparticles lies near states of both $`d`$-like and mixed-like character, (see Fig. 1 ) and therefore the latter ones most likely play a very relevant role in the tunneling experiments. However if we use the procedure described above and compute $`g`$-factor averages including mixed states, we find values that are too large in comparison with experiment.

As possible solutions, we consider the following: (i) electrons are, in fact, tunneling into states of pure $`d`$ character. (ii) Electrons are tunneling into states of mixed characters, but the nature of these delocalized states is strongly affected by the surface and therefore their characteristics, including their orbital angular momentum, are profoundly modified. This is an effect which is clearly not included in our model, and most likely it is more important for mixed states than for $`d`$-states. (iii) electron-electron interaction beyond the simple mean-field approximation incorporated in the SK parameters could also modify the electronic states and partially quench their orbital angular momentum. This effect is also not included in our model. Note that recent studiesVoisin et al. (2000) have demonstrated a sharp increase of electron-electron interaction due to surface induced reduction of screening. At the moment we find the occurrence of explanation (i) problematic: apart from the fact that in our calculations all states of pure $`d`$-character are below the Fermi level and therefore not available for tunneling, states of $`s`$ character have much larger tunneling probabilities than $`d`$-states, when (as in the present case) the barriers separating the grain from the electrodes are made of aluminum oxide. Explanations (ii) or (iii) or a combination of the two seem more compelling and alluring. However pursuing these lines requires theoretical modeling beyond the scopes of the present work.

## IV Conclusions

In summary, we have presented a theoretical study of the statistical properties of $`g`$-tensors for individual quasiparticle energy levels of metal nanoparticles, based on numerical calculations for a simplified but realistic model that treats spin-orbit interactions microscopically. Our theory of the $`g`$-tensors includes both spin and orbital contributions to the magnetic moment. We have shown that even small deviations from a perfectly symmetric nanoparticle shape cause random fluctuations in the quasiparticle wavefunctions, which, in turn, are the source of strong anisotropies of the $`g`$-tensors and strong level-to-level fluctuations both in the principal $`g`$-factor values and in the directions of their principal axis. A dimensionless parameter measuring the strength of the spin-coupling controls the $`g`$-tensor distributions for nanoparticles of generic shape, in excellent agreement with the prediction of random matrix theory. Our work sheds light on the relative importance of the spin vs orbital contributions to the $`g`$-factors and the strong dependence of the latter on the orbital character of the wave-functions. The presence near the Fermi energy of states of both $`d`$-like and $`sp`$-like character is responsible for aspects of the $`g`$-factor physics that are not captured by Random Matrix Theory. The small values of $`g`$-factors measured experimentally suggest that the orbital angular momentum of the tunneling states near the Fermi energy is most likely still partially quenched, even in the presence of strong spin-orbit scattering. Our calculations demonstrate that angular momentum quenching cannot be due simply to the strong $`d`$-orbital hybridization of states near the Fermi energy. Non-trivial changes in electronic structure might be responsible, perhaps due to irregularly shaped nanoparticle boundaries that produce orbitals more localized at the surface than those in the model that we have studied. Enhanced correlation effects near the surface, could also play a role. If surface imperfections are the main source of orbital localization, large $`g`$-factors should be observable in nanoparticles with very regularly shaped boundaries in which all orbitals are extended across the entire particle.

## V Acknowledgments

We would like to thank Dan Ralph for several explanations of his experimental results, and Piet Brouwer, Mandar Deshmukh and Leonid Glazman for stimulating discussions. This work was supported in part by the Swedish Research Council under Grant No:621-2001-2357, by the faculty of natural science of Kalmar University, and in part by the National Science Foundation under Grants DMR 0115947 and DMR 0210383. Support from the Office of Naval Research under Grant N00014-02-1-0813 is also gratefully acknowledged.


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# Circular dichroism and bilayer splitting in the normal state of underdoped (Pb,Bi)2Sr2(CaxY1-x)Cu2O8+δ and overdoped (Pb,Bi)2Sr2CaCu2O8+δ.

## Abstract

We report an ARPES investigation of the circular dichroism in the first Brillouin zone (BZ) of under- and overdoped Pb-Bi2212 samples. We show that the dichroism has opposite signs for bonding and antibonding components of the bilayer-split CuO-band and is antisymmetric with respect to reflections in both mirror planes parallel to the c-axis. Using this property of the energy and momentum intensity distributions we prove the existence of the bilayer splitting in the normal state of the underdoped compound and compare its value with the splitting in overdoped sample. In agreement with previous studies the magnitude of the interlayer coupling does not depend significantly on doping. We also discuss possible origins of the observed dichroism.

It is hard to overestimate the role of magnetic interactions in the high-temperature superconducting cuprates. While the spin fluctuations Chubukov  remain a reasonable candidate as a mediator of the pairing itself, the orbital currents form the basis of the approaches which seem to be promising in the explanation of the enigmatic pseudogap state.Chakravarty ; Wen  Angle-resolved photoemission spectroscopy (ARPES) has proven to be a successful technique to study related feedback effects in the electronic spectrum.NormanPRL\_97 ; Johnson ; Gromko1 ; BorisPRL\_03 ; KimPRL\_03  To be directly sensitive to magnetism, ARPES experiment needs to resolve the spins of photoelectrons. Such an attractive opportunity to measure spin, momentum and energy simultaneously and with the same efficiency requires further improvement of the apparatus for ”complete” photoemission - high spin resolution today still implies lower energy or/and momentum resolutions. To go around this problem one can suggest an alternative to a conventional explicit spin analysis. When using circularly polarized light as an excitation source, and in certain cases, the photoemission intensity itself may depend explicitly on the spin state of the excited electrons.OepenPRL ; Garbe  Explained in terms of spin-dependent diffraction through the surface, this effect suggests a possibility to study spin-dependent processes with conventional spin integrating electron analyzers. On the other hand, circularly polarized excitation can also be used to test the time-reversal invariance of the electronic system which is broken in the presence of the orbital currents.Varma ; Kaminski ; Boris\_condmat\_03  Up to now, however, only a small part of the Brillouin zone of Bi2Sr2CaCu2O8+δ (Bi2212) in the close vicinity of the ($`\pi `$, 0)-point was the focus of attention in the studies using circularly polarized light.Kaminski ; Boris\_condmat\_03  In addition, already the geometry of both experiments assumed a strong dichroic component, expected from a purely general consideration of the problem.Varma

Here we extend our studies to the whole Brillouin zone. We reduce the ”handedness” of our experiments, keeping the vectors of incidence, emission and the normal to the sample surface coplanar. In spite of this we clearly observe a strong (up to $`18\%`$) dichroism which turns out to be of opposite sign for bonding and antibonding components and which is odd upon reflections in all mirror planes. We use this effect to prove the existence of the bilayer splitting in the normal state of an underdoped sample. This is in direct contradiction with recent claims that the bilayer splitting is absent already in the optimally doped Bi2212.Kaminski\_noBS  Quantitative estimates give comparable results for the under- and overdoped samples implying the constancy of the bilayer splitting with doping in agreement with previous studies.Chuang ; KordPRB\_02

The experiments were performed at the 4.2R beamline ”Circular Polarization” at the ELETTRA storage ring using approximately 70$`\%`$ circularly polarized (CP) light from the elliptical wiggler-undulator. Spectra were collected in the angle-multiplexing mode of the SCIENTA SES-100 electron-energy analyzer. The overall average resolution in (k, $`\omega `$)-space was set to 0.01 Å-1 x 0.02 Å-1 x 30 meV. An essential advantage of this experimental setup is that no mechanical movement is involved in the process of switching the helicity of the incoming radiation. Only the direction of the current in the coils of the wiggler-undulator needs to be reversed which takes approximately 30 seconds. This enables the successive recording of the spectra using the light of both polarizations with the other experimental parameters remaining unchanged. The excitation energy was $`h\nu `$=25 eV. High-quality single crystals of 5x1-superstructure-free, underdoped Y-Pb-Bi2212 ($`T_c`$=80 K) and overdoped ($`T_c`$=72 K) Pb-Bi2212 were mounted on the three-axis stepper motor driven cryo-manipulator allowing a precise (0.1) positioning of the sample with respect to the analyzer’s entrance slit. Underdoping of the Pb-Bi2212 single crystals was done by partial substitution of calcium atoms by yttrium, which is known to be a good alternative to the de-oxygenation and is successfully investigated in different studies Y-doping . Measurement temperatures of the overdoped and underdoped samples were 105 K and 120 K respectively. Fermi surface maps were recorded at room temperature from the same single crystals using mostly unpolarized light as reported earlier.KordPRB\_02

In Fig. 1 we present the results of the routinely performed measurements which are considered by us as an essential constituent of the sample characterization. Local maxima on the momentum distribution maps measured near the Fermi level correspond to the Fermi surface. The area of the Fermi surface seen in Fig. 1 as rounded squares directly corresponds to the number of charge carriers in the system, i.e. its doping level. One can easily notice the difference in sizes of the ”barrels” even without any quantitative analysis. Moreover, the intensity near ($`\pi `$, 0)-point is much lower in case of the underdoped sample indicating the possible influence of the pseudogap. Comparison with the similar data for an optimally doped sample (not shown) together with these two observations clearly establishes the considerable difference in doping levels of the studied samples and their under- and overdoped characters respectively.KordPRB\_02

Energy distribution maps (EDM) and their difference taken in the nodal direction (cut 5) of the overdoped sample using the CP light are shown in Fig. 2(a-c). A difference EDM is obtained by subtraction of the raw data shown in panel (b) from the data shown in panel (a) taking into account corresponding values of the storage ring current. The resultant grey scale image does not show any significant variations of the intensity upon the change of helicity. We note that the grey scale is the same for the panels (c) and (f) and ranges from -45000 counts (black) to +45000 counts (white) resulting in the grey background if the difference is negligible. Cut 6 crosses the Fermi surface along a direction which makes an angle of 11 with the $`\mathrm{\Gamma }`$-($`\pi `$, $`\pi `$) line. One expects here a crossing of two bands originating from the c-axis bilayer splitting, the latter having been observed now by a number of photoemission groups in overdoped samples. In this case the dichroic signal is remarkably strong ($`\pm 8\%`$) and has a well-defined structure (Fig. 2 f). One would expect such a pattern if there are two closely separated dispersing features with the corresponding dichroism having the opposite sign for each of them. To check this we fitted the MDCs of panels (d), (e) and their sum with two Lorentzians. The fit appeared to be stable within the rather narrow energy interval ($`\pm `$ 40 meV) where an apparently asymmetric MDC’s line shape was observed. The results are shown in Fig. 2(g, h). The extracted dispersions prove the presence of two bands split by 0.032(7) Å-1, though the position of the weaker (in terms of intensity) bonding component is defined with larger errors as seen from Fig. 2(h). More importantly, the ratio of the spectral weights corresponding to the bonding and antibondig bands is systematically higher for the spectra taken with right-hand circularly polarized light. The presented data thus confirm the selective character of the excitation from the bonding and antibonding bands when using light of different helicity. A qualitatively similar picture is observed for other cuts through the FS within the irreducible octant of the first BZ (not shown).

The absence of dramatic changes of this picture in the underdoped regime as compared to the overdoped case is evident from Fig. 3. There we show difference EDMs for the directions 1 and 2 (see Fig. 1). The pattern is easily recognizable and qualitatively similar to the one shown in Fig. 2(f). Regardless of the origin of the dichroism, already on the basis of the visual comparison with the overdoped case, one can immediately conclude that the bilayer splitting is also present in the normal state of the underdoped sample, contrary to what is stated in Ref.Kaminski\_noBS, . Results of the fit for the direction 1 are nearly identical to those shown in Fig. 2: antibonding/bonding ratios are also of the order of 3 and 2 for the right- and left-hand CP light respectively and the size of the bilayer splitting is 0.037(5) Å-1 implying the constancy of this value with doping.Chuang  We note that the obtained values of the splitting in this direction of the BZ are larger than expected using the formula $`t_{}(\mathrm{cos}k_xa\mathrm{cos}k_ya)^2/2`$ (Ref. Andersen, ) and estimated in Ref. KordPRB\_03,  tight binding parameters . This is in agreement with our recent findings as for the finite nodal splitting.Kord\_nodal

Another characteristic feature of the momentum distribution of the dichroic signal is its antisymmetry with respect to the reflections in the crystal mirror planes. This is seen by comparing, for instance, the difference spectra presented in Fig. 4 (a-d). The spectra taken with circularly polarized light of positive helicity on one side of the mirror plane (e.g. cut 7) essentially agree with the ones recorded using the light of negative helicity and measured on the other side (e.g. cut 8) and vice versa. As seen from the Fig. 4 (a-d) this holds for both under- and overdoped samples. Qualitatively similar picture is observed for the $`\mathrm{\Gamma }`$ \- ($`\pi `$, $`\pi `$) mirror plane and at room temperature (not shown, see Ref.Boris\_condmat\_03, ).

Before going into the discussion of what could be the reason for such intensity variations we briefly summarize here three experimental results that follow from the presented and previously published data: (i) dichroism is observed everywhere in (k, $`\omega `$)-space except along the high symmetry lines, at different temperatures and in under- and overdoped samples of Pb-Bi2212; (ii) the sign of the dichroic signal changes upon reflection in all crystal mirror planes parallel to the c-axis; (iii) within the irreducible octant of the BZ the dichroism on the bonding and antibonding bands has the opposite sign. This is schematically illustrated in Fig. 4 (f).

We consider three possible candidates which could be responsible for the dichroism in the studied samples. An interference effect, known in the literature as circular dichroism in the angular distribution (CDAD), can be observed in nonchiral systems only if the experimental setup has a definite chirality.Westphal  As mentioned above, our experimental arrangement is such that all three vectors (incidence, emission and normal to the surface) are always kept within the same plane. This rules out a purely geometric origin of the dichroism.Geometry

The second possibility is the traditional magnetic circular dichroism in photoemission which requires the combination of spin-orbit coupling and exchange interaction in the initial or final state. It was demonstrated that the excitation with CP light under certain conditions results in optical spin orientation originating from the spin dependence of the dipole matrix elements.Woehlecke  The process becomes possible because the spin character of a given state is coupled to a wave function of certain spatial symmetry if one takes into account the spin-orbit interaction. In other words, the electrons excited from spin-orbit split bands could be spin-polarized in a final state due to relativistic symmetry selection rules when using circularly polarized light Orientation . Further, to detect this spin-polarization using a conventional analyzer the diffraction through the surface should be spin-dependent. This seems to be the case in Bi2212 since exactly Bi-O layers are the topmost after cleavage and Bi atoms are heavy enough to act as a natural ”spin-filter”. Moreover, within this scenario also the observed mirror plane antisymmetry of the dichroism is robustly understood. Both the photon spin and the spin polarization are axial vectors, so that they behave like angular-momentum vectors under a mirror operation. Taking this into account it is easy to show Garbe  that such antisymmetry would mean the flipping of the vector of spin-polarization upon reversal of the helicity. This last condition, in turn, is fulfilled for centrosymmetric crystals assuming that the time reversal symmetry is not broken.Garbe  To clarify the interplay between the bilayer splitting and spin-orbit interaction we have carried out relativistic band structure calculations of Bi2212. The basal plane-projected Fermi surface is shown in Fig. 4 (e). Inclusion of relativistic terms into the computational scheme results in the two split bands, but only near ($`\pi `$, 0) they are split by the spin-orbit interaction and only due to large admixture of the Bi-states which are thus actively involved in the formation of the Fermi surface. This, however, is in contradiction with the generally accepted views as for the non-metallicity of the Bi-O layers. The so called ”Bi-O pockets” have never been experimentally observed. In addition, presented experimental results clearly suggest that the effect persists all along the Fermi surface.

The third option is that the observed dichroism could also be attributed to orbital currents flowing in real space and thus breaking time-reversal symmetry. Naturally, the symmetry of the dichroism in reciprocal space requires that the order imposed by the orbital currents has to adequately reflect this symmetry. This condition limits the number of possible patterns. For instance, the pattern of currents suggested in Ref.Varma,  implies the breaking of the reflection symmetry in the $`\mathrm{\Gamma }`$ \- ($`\pi `$, 0) mirror plane and requires a considerable value of the dichroism in this mirror plane, which is apparently not the case, also in the present study. On the other hand, the arrangement of elementary currents expected in the ”d-density wave” approach Chakravarty  would be in agreement with our results. In order to account for the different sign of the dichroism for bonding and antibonding components one could order these currents in neighboring planes antiferromagnetically. In any case, our observations rule out a clear relation of the dichroism to the pseudogap regime as it was detected over significant portion of the phase diagram of Bi2212. This in turn reduces the chances of the orbital currents to be a solution of the given problem.

While at present it is not exactly clear what the origins of the reported dichroic effects in Bi2212 are, it definitely opens up a promising possibility to differentiate between the bonding and antibonding bands in future ARPES studies. Such a possibility seems to be urgently needed to help disentangle true many-body effects from mere features of the band structure.

We are grateful to H. Eschrig, A. Lichtenstein and N. Plakida for the stimulating discussions and to R. Hübel for technical support. We acknowledge the support of the European Community - Access to Research Infrastructure action of the Improving Human Potential Programme. HB is grateful to the Fonds National Suisse de la Recherche Scientifique, and MSG to FOM. MS and RC are supported by the DFG through SFB 484.