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# Impurity Effect on Ferromagnetic Transition in Double-Exchange Systems

## 1 Introduction

The double-exchange (DE) model has been studied intensively to explain ferromagnetic transition in colossal-magnetoresistance manganites.  The origin of the metallic ferromagnetism in these materials is well explained by the DE mechanism.  Recently, numerical calculations have demonstrated that fluctuations through the strong interplay between spin and charge degrees of freedom play a crucial role in this system.  Through precise calculations of the ferromagnetic transition temperature $`T_\mathrm{c}`$, the DE model is shown to give a quantitative description of the ferromagnetic transition in the typical material La1-xSrxMnO3 near $`x=0.3`$. This provides a well-established starting point toward comprehensive understanding of rich variety of physics in the manganites through quantitative comparisons between experiments and theories.

To this canonical DE ferromagnetic state, there are various perturbations in experiments, for instance, control of chemical compositions, external pressure and magnetic field.  It is important to clarify these effects theoretically in order to understand experiments where the perturbations may be entangled and act on in a complicated manner. Among them, we study effects of the randomness in this paper. Since mixed-valence manganites are synthesized as solid solutions, randomness is inevitably contained in these compounds. We discuss how the ferromagnetic transition is affected by the randomness.

The randomness effect for $`T_\mathrm{c}`$ in the DE system has been studied theoretically. Stability of the ferromagnetic state is studied by the coherent-potential approximation (CPA), and a decrease of $`T_\mathrm{c}`$ due to the randomness is predicted.  In this work, we go beyond the approximation and use a numerical technique which is essentially exact. Spatial random distribution of impurities is taken into account properly in this method. Since the spatial fluctuations which are neglected in the CPA are known to be important in the case without disorder,  the unbiased calculations are necessary also for the systems with disorder to discuss the quantitative change of $`T_\mathrm{c}`$.

This paper is organized as follows. The next section 2 introduces the DE model with disorder and describes the numerical methods briefly. In Sec. 3, the results for the approximately-estimated critical temperature are discussed for the cases with randomness in comparison with the results for the pure system. Sec. 4 is devoted to summary and concluding remarks.

## 2 Model and Method

In this work, we consider a simple model with a diagonal disorder in the framework of the DE model. The Hamiltonian is explicitly given by

$$H=t\underset{ij,\sigma }{}(c_{i\sigma }^{}c_{j\sigma }+\mathrm{h}.\mathrm{c}.)J_\mathrm{H}\underset{i}{}\stackrel{}{\sigma }_i\stackrel{}{S}_i+\underset{i\sigma }{}\epsilon _ic_{i\sigma }^{}c_{i\sigma },$$
(1)
where the first term denotes the nearest-neighbor hopping on the cubic lattice and the second term is for the Hund’s-rule coupling. The last term denotes the on-site randomness which modifies the one-body potential energy in each site. The potential $`\epsilon _i`$ takes $`\pm W_{\mathrm{imp}}/2`$ in equal probability in each site. The physical quantities are calculated by the random average for the quenched disorder. For simplicity, we consider the limits of $`J_H\mathrm{}`$ and $`|\stackrel{}{S}|\mathrm{}`$. In the following, we discuss the quarter-filled case which shows a maximum of $`T_\mathrm{c}`$ in the pure case.

We apply the Monte Carlo (MC) method to the model (1).  In this method, the MC weight to update a configuration of the localized moments are calculated quantum-mechanically by integrating out the fermion degrees of freedom. For large-size clusters, the difficulty of a rapid increase of the computational time has been solved by using the moment-expansion MC method.  The moment expansion as well as the random average is performed quite efficiently on parallel computer systems.

In the following, we use an energy unit $`W=6t=1`$ which is the half bandwidth for the pure system. For a given configuration of disorder, we have typically run $`1,000`$ MC samplings for measurements after $`1,000`$ MC steps for thermalization. The random average is taken for $`50`$ random configurations.

## 3 Results and Discussions

Before going to the cases with randomness, we review and discuss the ferromagnetic transition in the pure case ($`W_{\mathrm{imp}}=0`$).  Figure 1 shows the results for the temperature dependence of the magnetization for $`W_{\mathrm{imp}}=0`$. We present the data for finite-size clusters and those for the thermodynamic limit. The latter is obtained by the finite-size scaling analysis. From the onset of the magnetization in the thermodynamic limit, $`T_\mathrm{c}`$ is estimated as $`T_\mathrm{c}/W=0.023\pm 0.003`$.

Figure 1 indicates that in order to obtain the precise estimate of $`T_\mathrm{c}`$, a systematic study of the finite-size effects is crucial, which needs much computational effort. We note, however, that it is possible to define a characteristic temperature even for a fixed-size cluster. The temperature dependence of the magnetization for each finite-size cluster is a monotonic function and has an inflection point. We adopt this inflection point as the characteristic temperature $`T^{}`$. In Fig. 2, we plot the system-size dependence of $`T^{}`$ which is obtained from the numerical differentiation of the data in Fig. 1. Within the error bars, $`T^{}`$ is almost independent of the system size and agrees with $`T_\mathrm{c}`$ in the thermodynamic limit. Thus, $`T^{}`$ for a finite-size cluster is expected to give a good approximation for $`T_\mathrm{c}`$ in this pure case. We expect that this observation holds also for the systems with randomness below. Note that at least, since $`T^{}`$ must be an independent parameter to characterize the temperature scale for the ferromagnetic transition, it should be justified to discuss the stability of the ferromagnetism by $`T^{}`$.

Now we discuss the randomness effect. Figure 3 shows the magnetization curve for the system size of $`4\times 4\times 4`$ sites when we change the value of $`W_{\mathrm{imp}}`$. The magnetization decreases as the disorder strength $`W_{\mathrm{imp}}`$ increases. This indicates that the ferromagnetism is suppressed by the randomness. The decrease is the most significant near $`T_\mathrm{c}(W_{\mathrm{imp}}=0)`$. This is probably because near the critical point, the fluctuations are dominant and the coherence of the itinerant electrons becomes very sensitive to the randomness.

Based on the discussion in the pure case, we examine the stability of the ferromagnetism in the systems with randomness by $`T^{}`$. Figure 4 shows $`T^{}`$ as a function of $`W_{\mathrm{imp}}`$ which is estimated from the data in Fig. 3. As the critical temperature in the previous CPA results,  the approximated critical temperature $`T^{}`$ decreases as $`W_{\mathrm{imp}}`$ increases. Our MC data, however, show larger decrease in comparison with the CPA results: For instance, for $`W_{\mathrm{imp}}/W=0.5`$, our data show about $`35`$% decrease, while the CPA results show less than $`20`$% decrease. The CPA takes account of the randomness in an averaged way through the change of the density of states. In our MC study, the spatial distribution of the randomness as well as its effect on the coherence of electrons is included properly. Our data suggest that the spatial fluctuations are important and the suppression of $`T_\mathrm{c}`$ is stronger than expected from the band renormalization in the CPA.

## 4 Summary and Concluding Remarks

We have investigated the randomness effect on the ferromagnetic transition in the double-exchange model. We consider the model with on-site diagonal disorder. The spatial distribution of the randomness and large fluctuations inherent in this strongly-correlated system are taken into account properly by using the Monte Carlo method. The randomness suppresses the ferromagnetism of the double-exchange origin by reducing the coherence of the electron motion. Our results indicate that the suppression is significant in the critical region where the fluctuations are dominant. We have examined the characteristic temperature scale which is expected to give a good approximation for the critical temperature. The approximated critical temperature tends to be suppressed by the randomness as predicted by the coherent-potential approximation. Our Monte Carlo results, however, show a more rapid decrease than the previous results. This may be attributed to the spatial fluctuations by the randomness distribution which is included only in an averaged manner in the previous approximations.

The randomness effects are studied only for a small-size cluster in this paper. The estimated temperature $`T^{}`$ is an approximation for $`T_\mathrm{c}`$. Calculations for larger-size systems and more precise determination of the critical temperature including the finite-size scaling are under investigation. Different distribution of the randomness is also examined and will be reported elsewhere.

## Acknowledgement

The authors thank H. Nakata for helpful support in developing parallel-processing systems. The computations have been performed mainly using the facilities in the AOYAMA+ project (http://www.phys.aoyama.ac.jp/~aoyama+) and in the Supercomputer Center, Institute for Solid State Physics, University of Tokyo. This work is supported by “a Grant-in-Aid from the Ministry of Education, Culture, Sports, Science and Technology”.


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# References

hep-ph/0203209

RAL-TR-2002-008

21 Mar 2002

Symmetries and Generalisations of Tri-Bimaximal Neutrino Mixing.

P. F. Harrison

Physics Department, Queen Mary and Westfield College

Mile End Rd. London E1 4NS. UK 111E-mail:p.f.harrison@qmul.ac.uk

and

W. G. Scott

Rutherford Appleton Laboratory

Chilton, Didcot, Oxon OX11 0QX. UK 222E-mail:w.g.scott@rl.ac.uk

## Abstract

Tri-bimaximal mixing is a specific lepton mixing ansatz, which has been shown to account very successfully for the established neutrino oscillation data. Working in a particular basis (the ‘circulant basis’), we identify three independent symmetries of tri-bimaximal mixing, which we exploit to set the tri-bimaximal hypothesis in context, alongside some simple, phenomenologically interesting $`CP`$-conserving and $`CP`$-violating generalisations.

1. Introduction

Tri-bimaximal mixing  is a very successful lepton mixing ansatz, which has already attracted a degree of attention in the literature . In the standard parametrisation , tri-bimaximal mixing may be specified by: $`\theta _{12}=\mathrm{sin}^1(1/\sqrt{3})`$, $`\theta _{23}=\pi /4`$ and $`\theta _{13}=0`$, with no $`CP`$-violating phase. Tri-bimaximal mixing builds squarely on all of the most promising phenomenological ideas which have preceded it  and readily accounts for all of the best-established neutrino oscillation results to date   .

Despite these sucesses we have no reason to suppose that tri-bimaximal mixing will prove to be exactly right in every detail, and we seek therefore to generalise the original tri-bimaximal hypothesis, so as to parametrise possible deviations in simple and meaningful ways, which we hope will be useful in developing experimental tests. We begin by reviewing the symmetries inherent in the tri-bimaximal scheme, which will lead us to identify generic features which will form the basis of our generalisations.

2. Tri-Bimaximal Mixing and the Circulant Basis

Symmeties are usually thought to be best studied at the level of the mass-matrices, which are naturally referred to a ‘weak’ basis (ie. a basis which leaves the charged-current weak-interaction diagonal and universal). Furthermore, by restricting consideration to left-handed fields only, we may take our mass-matrices (squared) to be hermitian. Following Ref. , we will work in a particular weak basis in which the mass-matrix for the charged leptons takes the familiar $`3\times 3`$ ‘circulant’ form :

$$M_l^2=\left(\begin{array}{ccc}a& b& b^{}\\ b^{}& a& b\\ b& b^{}& a\end{array}\right)$$
(1)
where the constants $`a`$, $`b`$ and $`b^{}`$ encode the lepton masses as follows:

$`a={\displaystyle \frac{m_e^2}{3}}+{\displaystyle \frac{m_\mu ^2}{3}}+{\displaystyle \frac{m_\tau ^2}{3}}`$
$`b={\displaystyle \frac{m_e^2}{3}}+{\displaystyle \frac{m_\mu ^2\omega }{3}}+{\displaystyle \frac{m_\tau ^2\overline{\omega }}{3}}`$ (2)
$`b^{}={\displaystyle \frac{m_e^2}{3}}+{\displaystyle \frac{m_\mu ^2\overline{\omega }}{3}}+{\displaystyle \frac{m_\tau ^2\omega }{3}}`$
($`\omega =\mathrm{exp}(i2\pi /3)`$ and $`\overline{\omega }=\mathrm{exp}(i2\pi /3)`$ are complex cube roots of unity).

In the above basis (the ‘circulant basis’) the charged-lepton mass-matrix (Eq. 1) is clearly invariant under cyclic permutations of the three generation indices. Note, however, that invariance under odd permuations of the generation indices (ie. generation interchange) would require that odd permutations are performed simultaneously with a complex conjugation (see Section 3 below).

Thus far, we have simply chosen a basis, and it is the form of the neutrino mass matrix in this basis which determines the observable mixing. Since circulant matrices of identical order always commute, we cannot take the neutrino mass-matrix to be also a $`3\times 3`$ circulant and obtain non-trivial mixing. We were led therefore to postulate  a neutrino mass-matrix which is invariant under cyclic permutations of only two out of the three generations, ie. a $`2\times 2`$ circulant with one generation (which was taken to be generation 2 in this basis) isolated in the mass-matrix by four ‘texture zeroes’ , yielding the effective block-diagonal form:

$$M_\nu ^2=\left(\begin{array}{ccc}x& 0& y\\ 0& z& 0\\ y& 0& x\end{array}\right).$$
(3)
In Eq. 3 the constants $`x`$, $`y`$ and $`z`$ ($`y`$ negative) encode the neutrino masses as follows:

$`x={\displaystyle \frac{m_1^2}{2}}+{\displaystyle \frac{m_3^2}{2}}`$
$`y={\displaystyle \frac{m_1^2}{2}}{\displaystyle \frac{m_3^2}{2}}`$ (4)
$`z=m_2^2`$
Note that the neutrino mass matrix Eq. 3 is real and symmetric (as well as being, by construction, a $`2\times 2`$ circulant in the $`13`$ index subset). With $`y`$ real, the neutrino mass-matrix Eq. 3 is invariant under the odd permutation corresponding to the generation interchange $`13`$, performed with or without a complex conjugation (cf. Eq. 1 above).

The charged-lepton mass-matrix $`M_l^2`$ (Eq. 1) and the neutrino mass-matrix $`M_\nu ^2`$ (Eq, 3) are diagonalised by threefold maximal and twofold maximal unitary matrices $`U_l`$ and $`U_\nu `$, respectively . The MNS matrix  is then given by $`U_l^{}U_\nu =U`$ :

$`\begin{array}{ccc}\nu _1& \nu _2& \nu _3\end{array}\begin{array}{ccc}\nu _1& \nu _2& \nu _3\end{array}`$
$`\begin{array}{c}e\\ \mu \\ \tau \end{array}\left(\begin{array}{ccc}\frac{1}{\sqrt{3}}& \frac{1}{\sqrt{3}}& \frac{1}{\sqrt{3}}\\ \frac{\overline{\omega }}{\sqrt{3}}& \frac{1}{\sqrt{3}}& \frac{\omega }{\sqrt{3}}\\ \frac{\omega }{\sqrt{3}}& \frac{1}{\sqrt{3}}& \frac{\overline{\omega }}{\sqrt{3}}\end{array}\right)\left(\begin{array}{ccc}\sqrt{\frac{1}{2}}& 0& \sqrt{\frac{1}{2}}\\ 0& 1& 0\\ \sqrt{\frac{1}{2}}& 0& \sqrt{\frac{1}{2}}\end{array}\right)=\begin{array}{c}e\\ \mu \\ \tau \end{array}\left(\begin{array}{ccc}\sqrt{\frac{2}{3}}& \sqrt{\frac{1}{3}}& 0\\ \sqrt{\frac{1}{6}}& \sqrt{\frac{1}{3}}& \frac{i}{\sqrt{2}}\\ \sqrt{\frac{1}{6}}& \sqrt{\frac{1}{3}}& \frac{i}{\sqrt{2}}\end{array}\right)`$ (5)
which is tri-bimaximal mixing in a particular phase convention. Note that the tri-bimaximal mixing matrix (Eq. 5 \- RHS) has two rows (row 2 and row 3) which are complex conjugates of each other (so that corresponding elements are equal in modulus). This is readily traced to the fact that the matrix $`U_l^{}`$ (Eq. 5 \- LHS) has likewise two rows (row 2 and row 3) complex-conjugate, while the matrix $`U_\nu `$ is real. It will prove useful to observe (see Section 3) that the matrix $`U_l^{}`$ (Eq. 5 \- LHS) has also two columns (columns 1 and 3) complex conjugate.

3. CP-Conservation and Tri-Phi-Maximal Mixing

In the circulant basis (see Section 2, above) a number of generic features of tri-bimaximal mixing (Eq. 5) manifest themselves very simply in the form of the neutrino mass matrix (Eq. 3). Perhaps the most significant feature of tri-bimaximal mixing is the predicted absence of $`CP`$-violation in neutrino oscillations. If $`CP`$ is conserved, the MNS matrix is orthogonal (or may be taken111 The phases of the charged-lepton mass-eigenstates are entirely unphysical and may be re-defined at will. Also, the phases of the neutrino mass-eigenstates have no influence on the form of the neutrino mass-matrix (squared) $`M_\nu ^2`$ as defined here, ie. no influence on Eq. 6.  to be orthogonal). As remarked in Section 2, the unitary matrix $`U_l^{}`$ (Eq. 5 \- LHS) has two columns (columns 1 and 3) complex conjugates of each other. If the MNS matrix is orthogonal (ie. $`U=O`$), we have $`U_\nu =U_lO`$ which then gives $`U_\nu `$ with two rows (rows 1 and 3) complex conjugates of each other. Since $`M_\nu ^2=U_\nu \mathrm{diag}(m_1^2,m_2^2,m_3^2)U_\nu ^{}`$ this symmetry must then be manifest in the neutrino mass-matrix so that, in particular, a sufficiently general form for the neutrino mass matrix in the circulant basis, yielding no CP-violation in neutrino oscillations, may be written222 It should perhaps be said that the similarity of Eq. 6 of the present paper to Eq. 31 of Ref.  appears to be somewhat accidental. We remind the reader that we are working here in the ‘circulant basis’ (defined in Section 2, above) and not in the lepton flavour basis as in Ref. .:

$$M_\nu ^2=\left(\begin{array}{ccc}x& w& y^{}\\ w^{}& z& w\\ y& w^{}& x\end{array}\right).$$
(6)
The form Eq. 6 generalises Eq. 3, and also mirrors the circulant form Eq. 1 but with the $`2`$nd generation distinguished (when $`z=x`$ and $`y=w`$ Eq. 6 becomes circulant). The six real parameters correspond to the three masses and three real mixing angles. The important point however is that Eq. 6 exhibits the symmetry of Eq. 1 under the exchange of generations $`13`$ performed simutaneously with a complex conjugation. Indeed, in the circulant basis, it is the invariance of all the leptonic terms under this combined operation that ensures $`J_{CP}=0`$ (since Im $`det[M_l^2,M_\nu ^2]`$ changes sign).

Starting from Eq. 6, if we take $`w`$ and $`y`$ real, we immediately recover Altarelli-Feruglio mixing  with $`\mathrm{tan}2\theta =2\sqrt{2}(x+yzw)/(x+yz+8w)`$. If we consider only the combination $`w^2y`$ real (so that $`w`$ and $`y`$ have correlated phase, with $`w=|w|\mathrm{exp}(i\varphi )`$, $`y=|y|\mathrm{exp}(i2\varphi )`$ complex) we obtain a simple two parameter generalisation of Altarelli-Feruglio mixing with $`J_{CP}=0`$, but $`|U_{e3}|0`$ in general. Taking $`|w|0`$ (as required for tri-bimaximal mixing) but keeping $`y=|y|\mathrm{exp}(i2\varphi )`$ complex with a fixed phase-angle $`\varphi `$, we obtain a block-diagonal, complex neutrino mass-matrix, generalising Eq. 3, which will lead to ‘tri-$`\varphi `$maximal’ mixing (below):

$$M_\nu ^2=\left(\begin{array}{ccc}x& 0& y^{}\\ 0& z& 0\\ y& 0& x\end{array}\right).$$
(7)
The neutrino masses are given similarly to Eq. 4 (but with $`y`$ replaced by $`|y|`$):

$`x={\displaystyle \frac{m_1^2}{2}}+{\displaystyle \frac{m_3^2}{2}}`$
$`|y|={\displaystyle \frac{m_3^2}{2}}{\displaystyle \frac{m_1^2}{2}}`$ (8)
$`z=m_2^2`$
and we obtain the simple, one-parameter, $`CP`$-conserving generalisation of tri-bimaximal mixing (depending on the phase-angle $`\varphi `$) referred to here as ‘tri-$`\varphi `$maximal’ mixing:

$`\begin{array}{ccc}\nu _1& \nu _2& \nu _3\end{array}`$
$`U=\begin{array}{c}e\\ \mu \\ \tau \end{array}\left(\begin{array}{ccc}\sqrt{\frac{2}{3}}\mathrm{cos}\varphi & \frac{1}{\sqrt{3}}& \sqrt{\frac{2}{3}}\mathrm{sin}\varphi \\ \frac{\mathrm{cos}\varphi }{\sqrt{6}}\frac{\mathrm{sin}\varphi }{\sqrt{2}}& \frac{1}{\sqrt{3}}& \frac{\mathrm{cos}\varphi }{\sqrt{2}}\frac{\mathrm{sin}\varphi }{\sqrt{6}}\\ \frac{\mathrm{cos}\varphi }{\sqrt{6}}+\frac{\mathrm{sin}\varphi }{\sqrt{2}}& \frac{1}{\sqrt{3}}& \frac{\mathrm{cos}\varphi }{\sqrt{2}}\frac{\mathrm{sin}\varphi }{\sqrt{6}}\end{array}\right).`$ (9)
The phase angle $`\varphi `$ must satisfy $`|\mathrm{sin}\varphi |`$ $`\stackrel{<}{}`$ $`0.2`$ to fit the reactor data , while there is minimal impact on the fit to the atmospheric data . Tri-$`\varphi `$maximal mixing has $`U_{e3}0`$, but retains the symmetries $`|U_{e2}|=|U_{\mu 2}|=|U_{\tau 2}|`$ and $`J_{CP}=0`$. Note that in tri-$`\varphi `$maximal mixing the symmetry of two rows complex conjugate is sacrificed (compare Eq. 9 rows 2 and 3 with Eq. 5 \- RHS, rows 2 and 3). Clearly tri-$`\varphi `$maximal mixing reduces to tri-bimaximal mixng in the limit $`\varphi 0`$.

4. CP-Violation and Tri-Chi-Maximal Mixing

In the circulant basis, it will be enough to require that the neutrino mass matrix be real (ie. symmetric, since our mass matrices are hermitian) to ensure that two rows of the MNS matrix have corresponding elements which are equal in modulus 333 In general, if the MNS matrix has two rows with corresponding elements equal in modulus, then by approriate re-phasings, the two rows may always be taken to be complex-congugate to each other, with the remaining row taken to be purely real., just as in Eq. 1 (rows 2 and 3 in this case). Such mixing matrices form an already interesting (two-parameter) generalisation of tri-bimaximal mixing, with a form of mu-tau universality. This time (cf. Section 3 above) the proof depends on the unitary matrix $`U_l^{}`$ (Eq. 5) having two rows (row 2 and row 3) complex-conjugate. The theorem follows immediately by noting that a real symmetric matrix may always be diagonalised by an orthogonal matrix (ie. $`U_\nu =O`$, with $`O`$ an orthogonal matrix) so that the resulting MNS matrix $`UU_l^{}U_\nu =U_l^{}O`$, is necessarily also of the form Eq. 5, with rows 2 and 3 complex-conjugate and row 1 purely real. Clearly the resulting mixing matrix is invariant under interchange of row 2 and row 3 performed simultaneously with a complex-conjugation. This form of mu-tau univesality implies strict mu-tau symmetry for $`CP`$-even observables (eg. disappearance probabilities), but has $`CP`$-odd observables (eg. asymmetries in appearance probabiliites) changing sign.

Of course, non-zero $`CP`$-violation means sacrificing the symmetry (Eq. 6) of the neutrino mass-matrix under $`13`$ interchange together with complex-conjugation. If we do this taking the neutrino mass-matrix to be real as discussed above, and again demanding effective block-diagonal form, just as for tri-bimaximal mixing, we are immediately led to the neutrino mass-matrix for ‘tri-$`\chi `$maximal’ mixing:

$$M_\nu ^2=\left(\begin{array}{ccc}x& 0& y\\ 0& z& 0\\ y& 0& w\end{array}\right)$$
(10)
The real constants $`x`$, $`y`$, $`z`$ and $`w`$ now encode the neutrino masses and one mixing angle $`\chi `$ as follows:

$`x={\displaystyle \frac{m_1^2+m_3^2}{2}}{\displaystyle \frac{m_3^2m_1^2}{2}}\mathrm{sin}2\chi `$
$`w={\displaystyle \frac{m_1^2+m_3^2}{2}}+{\displaystyle \frac{m_3^2m_1^2}{2}}\mathrm{sin}2\chi `$ (11)
$`z=m_2^2`$
where $`\mathrm{cot}2\chi =2y/(xw)`$, leading to our second simple one-parameter generalisation of tri-bimaximal mixing, called here ‘tri-$`\chi `$maximal’ mixing:

$`\begin{array}{ccc}\nu _1& \nu _2& \nu _3\end{array}`$
$`U=\begin{array}{c}e\\ \mu \\ \tau \end{array}\left(\begin{array}{ccc}\sqrt{\frac{2}{3}}\mathrm{cos}\chi & \frac{1}{\sqrt{3}}& \sqrt{\frac{2}{3}}\mathrm{sin}\chi \\ \frac{\mathrm{cos}\chi }{\sqrt{6}}i\frac{\mathrm{sin}\chi }{\sqrt{2}}& \frac{1}{\sqrt{3}}& i\frac{\mathrm{cos}\chi }{\sqrt{2}}\frac{\mathrm{sin}\chi }{\sqrt{6}}\\ \frac{\mathrm{cos}\chi }{\sqrt{6}}+i\frac{\mathrm{sin}\chi }{\sqrt{2}}& \frac{1}{\sqrt{3}}& i\frac{\mathrm{cos}\chi }{\sqrt{2}}\frac{\mathrm{sin}\chi }{\sqrt{6}}\end{array}\right)`$ (12)
Again, we have $`|\mathrm{sin}\chi |`$ $`\stackrel{<}{}`$ $`0.2`$ in order to fit the reactor data . Tri-$`\chi `$maximal mixing has non-zero $`U_{e3}=\sqrt{2/3}\mathrm{sin}\chi `$ and maximal $`CP`$-violation (for fixed $`|U_{e3}|`$) with the Jarlskog invariant  given by $`J_{CP}=\mathrm{sin}2\chi /(6\sqrt{3}`$). As expected, Eq. 12 has rows 2 and 3 complex conjugates of each other. Tri-$`\chi `$maximal mixing Eq.12 and tri-$`\varphi `$maximal mixing Eq. 9 are clearly very closely related (they are identical interchanging $`\chi \varphi `$, apart from the factors of $`i`$). Again, tri-$`\chi `$maximal mixing (Eq. 12) reduces to tri-bimaximal mixing in the limit $`\chi 0`$.

Finally, we note that there is always the possibility of specialising our mixings by imposing additional constraints. An amusing specialisation of tri-$`\chi `$maximal mixing would be to require $`y=z(x+w)/2`$, which leads immediately to: $`\mathrm{sin}\chi =\sqrt{\mathrm{\Delta }m_{21}^2/\mathrm{\Delta }m_{31}^2}0.13`$, certainly consistent with current experimental limits , and holding out the promise of observable $`CP`$-violation in future experiments .

5. Discussion

We have identified three symmetries of tri-bimaximal mixing. In the circulant basis (where the charged-lepton mass-matrix takes a simple $`3\times 3`$ circulant form) these symmetries may be (separately) implemented by taking the neutrino mass-matrix to be i) real, ii) invariant under $`13`$ interchange with complex conjugation and iii) effective block-diagonal in the $`1,3`$ index subset. At the level of the mixing matrix these symmetries correspond to the properties i) two rows (rows 2 and 3) complex conjugate (equal in modulus), ii) no CP-violation in neutrino oscillations ($`J_{CP}=0`$) and iii) trimaximal mixing for solar neutrinos, ie. $`|U_{e2}|=|U_{\mu 2}|=|U_{\tau 2}|=1/\sqrt{3}`$.

Together with the Altarelli-Feruglio hypothesis , tri-$`\varphi `$maximal and tri-$`\chi `$maximal mixing form the complete set of natural one-parameter generalisations of tri-bimaximal mixing, defined by dropping any one (or retaining any two) of the above three symmetries. Thus tri-$`\varphi `$maximal mixing (Eq. 9) retains ii) $`J_{CP}=0`$ and iii) $`|U_{e2}|=|U_{\mu 2}|=|U_{\tau 2}|=1/\sqrt{3}`$, but drops i) two-rows complex-conjugate, while tri-$`\chi `$maximal mixing (Eq. 12) retains i) two-rows complex-conjugate and iii) $`|U_{e2}|=|U_{\mu 2}|=|U_{\tau 2}|=1/\sqrt{3}`$, dropping ii) $`J_{CP}=0`$. Altarelli-Feruglio mixing  completes the set, dropping iii) $`|U_{e2}|=|U_{\mu 2}|=|U_{\tau 2}|=1/\sqrt{3}`$, but retaining i) two rows complex-conjugate (equal in modulus) and ii) $`J_{CP}=0`$. Of course, only tri-bimaximal mixing itself retains all three of the above symmetries (and is furthermore completely defined by them).

There is no implication here that the list of one-parameter generalisations of tri-bimaximal mixing is exhausted. For example, we have also considered $`CP`$-conserving and $`CP`$-violating analogues of Eq. 9 and Eq. 12 which leave unmodified the first column (rather than the second column) of the tri-bimaximal mixing matrix, altough we judge these somewhat less ‘natural’ than those presented above.

Clearly, less-constrained ansatze are obtained dropping two symmetries simultaneously, ie. retaining only one. The (three-parameter) set of all mixings with $`J_{CP}=0`$ (see Section 3) is obviously too unconstrained to be useful, and the two parameter mixing ansatz, having rows 2 and 3 of the MNS matrix complex-conjugate (equal in modulus) has already been discussed in Section 4. Our final, and perhaps our most useful, two-parameter generalisation of tri-bimaximal mixing drops i) two rows complex conjugate and ii) $`J_{CP}=0`$, but retains iii) $`|U_{e2}|=|U_{\mu 2}|=|U_{\tau 2}|=1/\sqrt{3}`$. This mixing ansatz is defined (in the circulant basis) simply by a neutrino mass-matrix with four off-diagonal ‘texture zeroes’  (ie. by a neutrino mass-matrix with effective block-diagonal form, cf. Eq. 3), and it interpolates smoothly between tri-$`\varphi `$maximal and tri-$`\chi `$maximal mixing. Appealing to the unitarity of the MNS matrix, one might even claim that the block-diagonal constraint (ie. the presence of the texture zeroes, Eq. 3) is enough to explain the solar data  and to explain near maximal mu-tau mixing at the atmospheric scale , given $`|U_{e3}|`$ small from reactors .

We do not know which (if any) of the above symmetries will survive as experiments become more refined. With $`CP`$-violation an established feature of quark mixing  , and $`CP`$-violation in the lepton-sector seen universally as a crucial goal experimentally , we are tempted to give most emphasis here to our one-parameter $`CP`$-violating ansatz ‘tri-$`\chi `$maximal’ mixing, Eq. 12, as our most interesting and predictive ansatz. In any case, however, in practical terms, tri-$`\varphi `$maximal mixing and tri-$`\chi `$maximal mixing represent the two extremes that one has necessarily to consider experimentally, and we have also made it clear how best to interpolate between them. Perhaps the most remarkable thing is that tri-bimaximal mixing itself (which adequately represents current experimental observation) comprises so many symmetries.

Acknowledgement

This work was supported by the UK Particle Physics and Astronomy Research Council (PPARC).


text:
# Adiabatic creation of entangled states by a bichromatic field designed from the topology of the dressed eigenenergies

## I Introduction

Entanglement is a key concept in various contemporary areas of active research in quantum physics. It explicitly demonstrates the non-local character of quantum theory, having potential applications in quantum communication, cryptography and computation . The preparation of an entangled state is of great interest for both fundamental and applied reasons. During the last few years various methods for preparation of entangled states of atomic systems have been proposed and some of them experimentally demonstrated .

Although a quantum system can be manipulated by tailored sequences of resonant pulses of precise area, in particular $`\pi `$ and $`\pi /2`$ pulses respectively for the complete inversion and the equal weight coherent superposition, deviations from the precise pulse area and from resonance can lead to significant errors. Adiabatic passage techniques provide much greater robustness against fluctuations in the interaction parameters. The stimulated Raman adiabatic passage (STIRAP) method  has been proposed for the creation of an entangled state of two three-level atoms in a QED cavity  and for $`\mathrm{\Lambda }`$ atomic systems .

In this paper we propose a simple method for entangling two subsystems driven by pulse shaped external fields. For definiteness we take these to be two identical spins interacting with each other and driven by radio-frequency fields. This system can be translated in a three-level ladder model with the intermediate level corresponding to the entangled state . The goal is to populate completely this entangled state at the end of the pulses. The most efficient couplings are obtained with two near one-photon resonant fields. We show that unlike in the STIRAP process, one- and two-photon detunings are required to populate most efficiently the intermediate level.

## II The model: Two spin system in external fields

We consider two spin-$`\frac{1}{2}`$ particles coupled by uniaxial exchange interaction in the $`z`$ direction . In a time-dependent magnetic field $`𝐁(t)=[B_x(t),B_y(t),B_z]`$, the Hamiltonian of this system reads ($`\mathrm{}=1`$)

$$\widehat{𝖧}(t)=\widehat{𝖧}_0+\mu 𝐁(t)\left(\widehat{𝐒}_1+\widehat{𝐒}_2\right),$$
(1)
where

$$\widehat{𝖧}_0=4\xi \widehat{S}_1^z\widehat{S}_2^z$$
(2)
is the part describing the exchange interaction, $`\mu `$ is the gyromagnetic ratio, $`\xi `$ is the exchange-interaction constant, and $`\widehat{𝐒}_k=[\widehat{S}_k^x,\widehat{S}_k^y,\widehat{S}_k^z]`$ is the $`k`$th spin operator $`(k=1,2)`$. We assume that the static magnetic $`B_z`$ field in the $`z`$ direction is strong enough ($`|\mu B_z||\xi |`$) so that the model with exchange interaction only in the $`z`$ direction is justified.

In the spin product state space $`\{|m_1|m_2\}`$ $`(m=,)`$, where the states $`|_k`$ and $`|_k`$ denote respectively the spin-down and spin-up states of the $`k`$th spin, a complete basis of orthonormalized eigenstates of $`\widehat{H}_0`$ is given by

$`|`$ $``$ $`|_1|_2,`$ (4)
$`|^+`$ $``$ $`{\displaystyle \frac{1}{\sqrt{2}}}\left[|_1|_2+|_1|_2\right],`$ (5)
$`|`$ $``$ $`|_1|_2,`$ (6)
$`|^{}`$ $``$ $`{\displaystyle \frac{1}{\sqrt{2}}}\left[|_1|_2|_1|_2\right].`$ (7)
In this basis, the Hamiltonian (1) can be expressed in the block-matrix form

$$𝖧(t)=\left[\begin{array}{cc}𝐇_c(t)& \mathrm{𝟎}\\ \mathrm{𝟎}& \xi \end{array}\right],$$
(8)
where

$$𝐇_\text{c}=\left[\begin{array}{ccc}\xi \beta _z& \frac{1}{\sqrt{2}}(\beta _x+i\beta _y)& 0\\ \frac{1}{\sqrt{2}}(\beta _xi\beta _y)& \xi & \frac{1}{\sqrt{2}}(\beta _x+i\beta _y)\\ 0& \frac{1}{\sqrt{2}}(\beta _xi\beta _y)& \xi +\beta _z\end{array}\right]$$
(9)
with $`\beta [\beta _x,\beta _y,\beta _z]=\mu 𝐁`$. The state $`|^{}`$ is thus decoupled from the other states; it describes the evolution of a spin$`0`$ singlet in a time-dependent magnetic field. This decoupling justifies our choice of the basis. The three other states $`|`$, $`|^+`$ and $`|`$ are coupled by the transverse $`(xy)`$ magnetic field. To complete the definition of the problem, we suppose that initially the two-spin system is in the unentangled state $`|`$. Our goal is to establish the conditions leading to the most efficient robust transfer into the entangled state $`|^+`$.

We consider the case when the spin system interacts with a constant magnetic field in the $`z`$ direction and two radio-frequency fields of respective frequencies $`\omega _1`$ and $`\omega _2`$ in the $`x`$ direction:

$`\beta _z`$ $`=`$ $`\text{const},`$ (11)
$`\beta _x`$ $`=`$ $`\mathrm{\Omega }_1\left(t\right)\mathrm{cos}\left(\omega _1t+\phi _1\right)+\mathrm{\Omega }_2\left(t\right)\mathrm{cos}\left(\omega _2t+\phi _2\right),`$ (12)
$`\beta _y`$ $`=`$ $`0.`$ (13)
The state vector $`\varphi (t)`$ is solution of the Schrödinger equation i$`\frac{d}{dt}\varphi (t)=𝖧_\text{c}(t)\varphi (t)`$ with the Hamiltonian $`𝖧_\text{c}(t)`$ (9) written in the basis $`\left\{\right|,|^+,|\}`$. When the radiofrequency fields are off ($`\beta _x=0`$), we have the following energies $`E_{}\xi \beta _z`$, $`E_^+\xi `$ and $`E_{}\xi +\beta _z`$. Without loss of generality we assume $`\xi <0`$ and $`\beta _z>0,`$ leading for $`\beta _z>2\left|\xi \right|`$ to a ladder configuration $`E_{}<E_^+<E_{}`$. We apply near resonant fields $`\omega _1E_^+E_{}`$, $`\omega _2E_{}E_^+`$, i.e. with the detunings $`\mathrm{\Delta }_1`$ and $`\mathrm{\Delta }_2`$:

$`\omega _1`$ $``$ $`2\left|\xi \right|+\beta _z\mathrm{\Delta }_1,`$ (15)
$`\omega _2`$ $``$ $`2\left|\xi \right|+\beta _z\mathrm{\Delta }_2.`$ (16)
According to the rotating wave approximation (RWA), one can neglect non resonant counterrotating terms under the conditions $`\omega _{1,2}\mathrm{\Omega }_1\left(t\right),\mathrm{\Omega }_2\left(t\right)`$. The RWA transformation

$$𝖱=\left[\begin{array}{ccc}e^{\text{i}E_{}t}& 0& 0\\ 0& e^{\text{i}\left(E_{}+\omega _1\right)t}& 0\\ 0& 0& e^{\text{i}\left(E_{}+\omega _1+\omega _2\right)t}\end{array}\right]$$
(17)
leads to the state vector $`\stackrel{~}{\varphi }(t)=𝖱^{}\varphi (t)`$ (whose coefficients have the same absolute values as the ones of $`\varphi `$), that satisfies the Schrödinger equation

$$\text{i}\frac{d}{dt}\stackrel{~}{\varphi }(t)=\stackrel{~}{𝖧}_\text{c}(t)\stackrel{~}{\varphi }(t),$$
(18)
with the Hamiltonian $`\stackrel{~}{𝖧}_\text{c}=𝖱^{}𝖧_\text{c}𝖱`$i$`\left(𝖱^{}/t\right)𝖱`$, where only the quasi-resonant terms have been kept:

$$\stackrel{~}{𝖧}_\text{c}=\frac{1}{2}\left[\begin{array}{ccc}0& \mathrm{\Omega }_1\left(t\right)+e^{\text{i}\delta t}\mathrm{\Omega }_2\left(t\right)& 0\\ \mathrm{\Omega }_1\left(t\right)+e^{\text{i}\delta t}\mathrm{\Omega }_2\left(t\right)& 2\mathrm{\Delta }_1& \mathrm{\Omega }_2\left(t\right)+e^{\text{i}\delta t}\mathrm{\Omega }_1\left(t\right)\\ 0& \mathrm{\Omega }_2\left(t\right)+e^{\text{i}\delta t}\mathrm{\Omega }_1\left(t\right)& 2\left(\mathrm{\Delta }_1+\mathrm{\Delta }_2\right)\end{array}\right].$$
(19)
The frequency

$$\delta \omega _1\omega _2=4\left|\xi \right|+\mathrm{\Delta }_2\mathrm{\Delta }_1$$
(20)
characterizes the coupling ambiguity . This Hamiltonian $`\stackrel{~}{𝖧}_\text{c}`$ allows indeed both fields to couple the two transitions when the field amplitudes $`\mathrm{\Omega }_1\left(t\right)`$ and $`\mathrm{\Omega }_2\left(t\right)`$ are not small compared to $`\delta `$. The competing coupling schemes are depicted in Fig. 1 with $`|1|,`$ $`|2|^+`$ and $`|3|`$. Two limit channels can thus be exhibited: the channel A (respectively B) corresponding to the absorptions of one $`\omega _1`$photon (respectively of one $`\omega _2`$photon) by the $`12`$ transition and of one $`\omega _2`$photon (respectively of one $`\omega _1`$photon) by the $`23`$ transition. We will study more precisely in Sections V and VI the various regimes that occur in this system. The problem of preparing the entangled state $`|2|^+`$ is thus reduced to the study of the population transfer of the intermediate level in the ladder system driven by the Hamiltonian $`\stackrel{~}{𝖧}_\text{c}`$ (19).

The populations given by the Schrödinger equation (18) are invariant under the following transformation $`𝒯`$

$`\mathrm{\Delta }_1`$ $``$ $`\mathrm{\Delta }_1+\delta ,`$ (22)
$`\mathrm{\Delta }_2`$ $``$ $`\mathrm{\Delta }_2\delta ,`$ (23)
$`\delta `$ $``$ $`\delta ,`$ (24)
$`\mathrm{\Omega }_1`$ $``$ $`\mathrm{\Omega }_2.`$ (25)
We indeed obtain $`\stackrel{~}{𝖱}^{}\left(𝒯\stackrel{~}{𝖧}_\text{c}\right)\stackrel{~}{𝖱}`$i$`\left(\stackrel{~}{𝖱}^{}/t\right)\stackrel{~}{𝖱}=\stackrel{~}{𝖧}_\text{c}`$, with the unitary transformation

$$\stackrel{~}{𝖱}=\left[\begin{array}{ccc}1& 0& 0\\ 0& e^{\text{i}\delta t}& 0\\ 0& 0& 1\end{array}\right].$$
(26)
## III Numerical results

Figures 2 and 3 display the population of the state $`|2`$ at the end of a sequence of delayed gaussian pulses of the same lengths and the same peak amplitudes

$`\mathrm{\Omega }_1\left(t\right)`$ $`=`$ $`\mathrm{\Omega }_0\mathrm{exp}\left[\left(t+\tau \right)^2/T^2\right],`$ (28)
$`\mathrm{\Omega }_2\left(t\right)`$ $`=`$ $`\mathrm{\Omega }_0\mathrm{exp}\left[\left(t\tau \right)^2/T^2\right],`$ (29)
for various normalized peak amplitudes $`\mathrm{\Omega }_0/\delta `$ and detunings $`\mathrm{\Delta }/\delta `$, where we have chosen

$$\mathrm{\Delta }\mathrm{\Delta }_1=\mathrm{\Delta }_2.$$
(30)
We have considered this restriction of the parameters because it gives preferentially large islands of good population transfer. This will be justified in Sections V and VI. Note that the case $`\mathrm{\Delta }_1=\mathrm{\Delta }_2`$ is irrelevant since it corresponds to a two-photon resonance between the product states $`|`$ and $`|`$. We could have considered equivalently the restriction $`\mathrm{\Delta }_2=\mathrm{\Delta }_1+2\delta `$ in accordance with the symmetry (II). The two different orderings of pulses have been considered: the sequence 1 of Fig. 2 (respectively the sequence 2 of Fig. 3) corresponds to the $`\omega _1`$pulse (respectively the $`\omega _2`$pulse) being switched on first, with the delay $`\tau =1.7T`$ (respectively $`\tau =1.7T`$). Global adiabaticity is ensured by the choice of a large pulse area $`\mathrm{\Omega }_0T=50`$.

One can distinguish three islands of robust high transfer (white regions). Specific parameters characterizing these islands are labelled by ($`a`$), ($`a^{}`$), ($`d`$), and ($`d^{}`$), with the subscript 1 or 2 respectively for the figures 2 or 3 \[except ($`a_2`$) which is outside the regions of high transfer\]. These islands of high transfer are analyzed in the following Sections by using the dressed Hamiltonian corresponding to $`\stackrel{~}{𝖧}_\text{c}`$ (19) and the adiabatic properties of the dynamics. We will characterize different regimes and associate them with different effective dressed Hamiltonians. We will show that the islands of good transfer can be understood from the topological properties of the appropriate effective dressed Hamiltonian.

We will show the following results:

(i) Regions (a) correspond to a STIRAP-like process associated to the channel A (see Fig. 1) that is perturbed (in the sense of non-resonant perturbation theory) by the channel B. Note that the restriction $`\mathrm{\Delta }_2=\mathrm{\Delta }_1+2\delta `$ would have given a STIRAP-like process associated to the channel B perturbed by the channel A;

(ii) Regions (d) (in the weak field regime, i.e. $`\mathrm{\Omega }_1,\mathrm{\Omega }_2<\delta `$) correspond to an effective two-level SCRAP-like (Stark chirped rapid adiabatic passage) process ;

(iii) Regions (d’) (in the strong field regime, i.e. $`\mathrm{\Omega }_1,\mathrm{\Omega }_2\delta `$) corresponds to an effective two-level bichromatic SCRAP process (with additional Stark shifts) as described in Ref. .

## IV The dressed Hamiltonian

It is convenient to use the adiabatic Floquet theory in order to study the Hamiltonian $`\stackrel{~}{𝖧}_\text{c}`$ (19) since its time dependence contains a characteristic frequency $`\delta `$. The dressed Hamiltonian (or quasienergy Hamiltonian) corresponding to $`\stackrel{~}{𝖧}_\text{c}`$ is :

$$𝖪^{[\mathrm{\Omega }_1,\mathrm{\Omega }_2]}=\text{i}\delta \frac{}{\theta }+\frac{1}{2}\left[\begin{array}{ccc}0& \mathrm{\Omega }_1\left(t\right)+e^{\text{i}\theta }\mathrm{\Omega }_2\left(t\right)& 0\\ \mathrm{\Omega }_1\left(t\right)+e^{\text{i}\theta }\mathrm{\Omega }_2\left(t\right)& 2\mathrm{\Delta }_1& \mathrm{\Omega }_2\left(t\right)+e^{\text{i}\theta }\mathrm{\Omega }_1\left(t\right)\\ 0& \mathrm{\Omega }_2\left(t\right)+e^{\text{i}\theta }\mathrm{\Omega }_1\left(t\right)& 2\left(\mathrm{\Delta }_1+\mathrm{\Delta }_2\right)\end{array}\right].$$
(31)
This dressed Hamiltonian depends parametrically on the pulse shapes and the detunings. It acts in the Hibert space spanned on the three states $`\{|1,|2,|3\}`$ tensored by the photonic Hilbert space . The eigenstates of $`𝖪`$ are families of three states denoted $`|1;k,k`$, $`|2;k1,k`$ and $`|3;k1,k1`$ with $`k`$ a positive or negative integer. The corresponding eigenvalues $`\lambda _{1;k,k}`$, $`\lambda _{2;k1,k}`$ and $`\lambda _{3;k1,k1}`$ have the following periodicity property: $`\lambda _{n;k_1,k_2}=\lambda _{n;k_11,k_2+1}+\mathrm{}\delta `$, for $`n=1,2,3`$. The notation $`|n;k_1,k_2`$ characterizes (when the fields are off) the state $`|n`$ dressed by the field of $`k_1`$ $`\omega _1`$photons and of $`k_2`$ $`\omega _2`$photons. The integers $`k_1`$ and $`k_2`$ characterize thus relative photon numbers of the respective fields of frequency $`\omega _1`$ and $`\omega _2.`$ The initial state is denoted $`|1;0,0.`$ The problem can be formulated as follows: we look for robust adiabatic connections between the initial state $`|1;0,0`$ and the final state $`|2;k1,k`$ for some positive or negative integer $`k`$.

The possible connections depend on the topology of the eigenenergy surfaces of (31) as functions of the field envelopes $`\mathrm{\Omega }_1`$ and $`\mathrm{\Omega }_2`$ for given $`\mathrm{\Delta }_1`$ and $`\mathrm{\Delta }_2`$ . The topology is characterized by true crossings which occur generically when one of the fields is off. We will study in the following the topology of $`𝖪`$ using different effective dressed Hamiltonians corresponding to different regimes. These regimes will depend on the ranges of the detunings and of the field amplitudes.

We classify the different regimes and construct effective dressed Hamiltonians by determining in the Hamilonian $`𝖪`$ (31) which terms are resonant (or quasi-resonant) and which one are only perturbative. The resonant terms are treated by an adapted unitary transformation which allows an explicit diagonalization, whereas the perturbative terms can be treated by stationary pertubation theory. This technique has been presented in . Note that for a simple RWA two-level system of Rabi frequency $`\mathrm{\Omega }`$ and detuning $`\mathrm{\Delta }`$, the perturbative regime is such that $`\mathrm{\Omega }\left|\mathrm{\Delta }\right|`$ and the resonant regime such that $`\mathrm{\Omega }`$ $`\left|\mathrm{\Delta }\right|`$. We classify the different regimes as functions of the ranges of the field amplitudes and of the detunings. In the following, we have normalized all the quantities with respect to $`\delta .`$

## V Weak field regime

The weak field regime occurs when $`\mathrm{\Omega }_1\left(t\right),\mathrm{\Omega }_2\left(t\right)<\delta `$. Note that when one has $`\mathrm{\Delta }_1=\mathrm{\Delta }_2`$ additionally, this regime coincides with a strong spin coupling since we have then $`4\left|\xi \right|>\mathrm{\Omega }_1\left(t\right),\mathrm{\Omega }_2\left(t\right)`$. In this case of weak field regime, we can intuitively analyze the different regimes with respect to the range of the detunings using the diagram of linkage patterns (Fig. 1). Five relevant regimes (bounded by dashed lines) have been collected in Fig. 4, depending on the quasi-resonances:

($`A`$) The transition 1-2 is quasi-resonant with $`\omega _1`$ and perturbed by $`\omega _2`$, 2-3 is quasi-resonant with $`\omega _2`$ and perturbed by $`\omega _1`$;

($`B`$) 1-2 is quasi-resonant with $`\omega _2`$ and perturbed by $`\omega _1`$, 2-3 is quasi-resonant with $`\omega _1`$ and perturbed by $`\omega _2`$;

($`C`$) 1-2 and 2-3 are both quasi-resonant with $`\omega _2`$, and perturbed by $`\omega _1`$;

($`D`$) 1-2 is quasi-resonant with $`\omega _2`$ and perturbed by $`\omega _1`$, 2-3 is perturbed by $`\omega _2`$ and $`\omega _1`$;

($`\stackrel{~}{C}`$) 1-2 and 2-3 are both quasi-resonant with $`\omega _1`$, and perturbed by $`\omega _2`$;

($`\stackrel{~}{D}`$) 1-2 is quasi-resonant with $`\omega _1`$ and perturbed by $`\omega _2`$, 2-3 is perturbed by $`\omega _1`$ and $`\omega _2`$.

In the exact resonant cases, we have represented the regimes $`A`$, $`C`$ and $`D`$ in Fig. (5).

As shown schematically in Fig. 4, the above regimes can be roughly bounded by

$$\mathrm{\Delta }_1=\pm \delta /2,\mathrm{\Delta }_1=3\delta /2\mathrm{\Delta }_2=\pm \delta /2,\mathrm{\Delta }_2=3\delta /2.$$
(32)
By the symmetry (II), we recover the regime $`B`$ from the regime $`A`$, $`\stackrel{~}{C}`$ from $`C`$, $`\stackrel{~}{D}`$ from $`D`$ (exchanging additionally $`\mathrm{\Omega }_1`$ and $`\mathrm{\Omega }_2`$).

The regimes $`A`$ and $`B`$ are STIRAP-like regimes; $`D`$ and $`\stackrel{~}{D}`$ are SCRAP-like regimes.

We do not consider other regimes where the state $`|1`$ is almost not depopulated by adiabatic passage.

The line $`\mathrm{\Delta }=\delta /2`$ appears as a dashed line in Figs 2 and 3, where the restriction $`\mathrm{\Delta }_1=\mathrm{\Delta }_2`$ has been considered.

### A Regime A

When the transition 1-2 is quasi-resonant with the frequency $`\omega _1`$ and the transition 2-3 quasi-resonant with the frequency $`\omega _2`$, the process can be analyzed as the channel A perturbed (in the sense non-resonant perturbation theory) by the channel B. We refer to it as the regime A as shown in Figs 2 and 3, where it is roughly bounded by the dashed lines $`\mathrm{\Delta }=\delta /2`$, $`\mathrm{\Delta }=\delta /2`$ (not shown) and $`\mathrm{\Omega }_0=\delta `$. This regime is approximately characterized by the following effective Hamiltonian in the basis $`\{|1;0,0`$,$`|2;1,0`$,$`|3;1,1\}`$ :

$$\stackrel{~}{𝖧}_\text{c}^\text{A}=\frac{1}{2}\left[\begin{array}{ccc}\frac{\left[\mathrm{\Omega }_2\left(t\right)\right]^2}{2\left(\delta +\mathrm{\Delta }_1\right)}& \mathrm{\Omega }_1\left(t\right)& 0\\ \mathrm{\Omega }_1\left(t\right)& 2\mathrm{\Delta }_1+\frac{\left[\mathrm{\Omega }_2\left(t\right)\right]^2}{2\left(\delta +\mathrm{\Delta }_1\right)}+\frac{\left[\mathrm{\Omega }_1\left(t\right)\right]^2}{2\left(\delta \mathrm{\Delta }_2\right)}& \mathrm{\Omega }_2\left(t\right)\\ 0& \mathrm{\Omega }_2\left(t\right)& 2\left(\mathrm{\Delta }_1+\mathrm{\Delta }_2\right)\frac{\left[\mathrm{\Omega }_1\left(t\right)\right]^2}{2\left(\delta \mathrm{\Delta }_2\right)}\end{array}\right]$$
(33)
which corresponds to the Hamiltonian characterizing the channel A with additional time dependent Stark shifts (on the diagonal) induced by the channel B. Note that this effective Hamiltonian is less precise for bigger $`\mathrm{\Omega }_1`$ or $`\mathrm{\Omega }_2`$ approaching $`\delta `$.

Before analyzing the dynamics given by this Hamiltonian (33), we recall the results in the limit case of a very weak field $`\mathrm{\Omega }_1\left(t\right),\mathrm{\Omega }_2\left(t\right)\delta `$ obtained in Ref. . In this case the perturbative terms can be neglected and the Hamiltonian becomes

$$\stackrel{~}{𝖧}_\text{c}^\text{A}\frac{1}{2}\left[\begin{array}{ccc}0& \mathrm{\Omega }_1\left(t\right)& 0\\ \mathrm{\Omega }_1\left(t\right)& 2\mathrm{\Delta }_1& \mathrm{\Omega }_2\left(t\right)\\ 0& \mathrm{\Omega }_2\left(t\right)& 2\left(\mathrm{\Delta }_1+\mathrm{\Delta }_2\right)\end{array}\right].$$
(34)
This resulting effective Hamiltonian corresponds to the channel A alone. The topology of the energy surfaces of this Hamiltonian has been analyzed in . It has been shown that the adiabatic transfer to state $`|2`$ is topologically allowed for

$`\mathrm{\Delta }_1\mathrm{\Delta }_2>0.`$

The topological analysis shows moreover that for the sequence 1 the region of this process is bounded in the parameter space by the curves

$`\mathrm{\Omega }_0=2\sqrt{\mathrm{\Delta }_1\left(\mathrm{\Delta }_1+\mathrm{\Delta }_2\right)}`$

and for the sequence 2 by the curves

$`\mathrm{\Omega }_0=2\sqrt{\mathrm{\Delta }_1\left(\mathrm{\Delta }_1+\mathrm{\Delta }_2\right)}\text{and}\mathrm{\Omega }_0=2\sqrt{\mathrm{\Delta }_2\left(\mathrm{\Delta }_1+\mathrm{\Delta }_2\right)}.`$

Taking now into account the perturbation by the channel B \[Hamiltonian (33)\] leads to two kinds of topology as shown in Figs 6 and 7, where the surfaces of quasienergies as functions of the normalized Rabi frequencies $`\mathrm{\Omega }_1/\delta `$ and $`\mathrm{\Omega }_2/\delta `$ respectively for $`\mathrm{\Delta }=\mathrm{\Delta }_1=\mathrm{\Delta }_2=\delta /20`$ and $`\mathrm{\Delta }=\mathrm{\Delta }_1=\mathrm{\Delta }_2=\delta /4`$ have been displayed. The eigenvalues of (33) (not shown) fit these surfaces well except in Fig. 7 when $`\mathrm{\Omega }_1\delta `$ and $`\mathrm{\Omega }_2\delta `$ because of an additional dynamical resonance (i.e. a resonance occuring beyond a threshold of the field amplitudes)  which involves the surface connected with $`|3;0,2`$ (which corresponds to the surface connected to $`|3;1,1`$ and translated of $`\delta `$) and the surface right below.

Fig. 6 shows that the two conical intersections, one occuring for $`\mathrm{\Omega }_1=0`$, the other one for $`\mathrm{\Omega }_2=0`$, bound the adiabatic connection between the initial state $`|1;0,0`$ and the target state $`|2;1,0`$. More precisely, for the sequence 1, the conical intersection occuring for $`\mathrm{\Omega }_1=0`$ is favorable for this adiabatic connectivity. The path denoted $`a_1`$ (also corresponding to the cross $`a_1`$ of Fig. 2) is an example for the complete transfer. On the other hand, for the sequence 2, the conical intersection occuring for $`\mathrm{\Omega }_1=0`$ is also favorable but the one occuring for $`\mathrm{\Omega }_2=0`$ is detrimental since it makes $`|1;0,0`$ connect with $`|3;1,1`$. The path denoted $`a_2`$ is an example for the complete transfer to $`|3;1,1`$ (also corresponding to the cross $`a_2`$ of Fig. 3).

For a bigger detuning (in absolute value), the topology is different as shown in Fig. 7. The previous conical intersection occuring for $`\mathrm{\Omega }_2=0`$ has now disappeared and another one involving the surfaces connected to $`|1;0,0`$ and $`|3;0,2`$ has appeared. The two conical intersections, the one occuring for $`\mathrm{\Omega }_1=0`$ and the other one for $`\mathrm{\Omega }_2=0`$, are involved for the adiabatic connection between the initial state $`|1;0,0`$ and the target state $`|2;1,0`$. More precisely, for the sequence 1, these two conical intersections bound this adiabatic connection; the path denoted $`a_1^{}`$ (also corresponding to the cross $`a_1^{}`$ of Fig. 2) is an example for the complete transfer. On the other hand, for the sequence 2 only the conical intersection occuring for $`\mathrm{\Omega }_1=0`$ bounds now the adiabatic connection; the path denoted $`a_2^{}`$ is an example for the complete transfer (also corresponding to the cross $`a_2^{}`$ of Fig. 3).

Using the effective Hamiltonian (33), the position of the previous conical intersections, for $`\mathrm{\Omega }_1=0`$ and $`\mathrm{\Omega }_2=0`$ respectively, lead to the three boundaries for the sequence 1

$`\mathrm{\Delta }`$ $`=`$ $`{\displaystyle \frac{\mathrm{\Omega }_2}{16\delta }}\left(5\mathrm{\Omega }_2\pm \sqrt{9\left(\mathrm{\Omega }_2\right)^2+32\delta ^2}\right),`$ (36)
$`\mathrm{\Omega }_1`$ $`=`$ $`\sqrt{2(\delta \mathrm{\Delta })\left[2\left(\delta +\mathrm{\Delta }\right)\sqrt{2\left(\delta +\mathrm{\Delta }\right)}\right]}.`$ (37)
The delay between the pulses has been chosen sufficiently large such that it is a good approximation to consider that the adiabatic connectivity is quite well described by the value of the peak amplitudes. Thus we have displayed these boundaries in Fig. 2 as full lines, with $`\mathrm{\Omega }_0=\mathrm{\Omega }_2`$ for (36) and with $`\mathrm{\Omega }_0=\mathrm{\Omega }_1`$ for (37). They globally bound the lower and upper part of the island of good transfer of the regime A observed in the numerical computation. This island is crossed by the line of resonance $`\mathrm{\Delta }=0`$ around which the transfer to $`|2`$ depends on the pulse areas, as shown by small oscillating islands.

For the sequence 2, the conical intersections involved give the following boundaries

$`\mathrm{\Delta }`$ $`=`$ $`{\displaystyle \frac{\mathrm{\Omega }_2}{16\delta }}\left(5\mathrm{\Omega }_2\sqrt{9\left(\mathrm{\Omega }_2\right)^2+32\delta ^2}\right),`$ (39)
$`\mathrm{\Omega }_1`$ $`=`$ $`\sqrt{(\delta \mathrm{\Delta })\left[4\mathrm{\Delta }+\delta \pm \sqrt{\delta \left(\delta +8\mathrm{\Delta }\right)}\right]},\text{for }\mathrm{\Delta }<0.`$ (40)
These curves are displayed in fig. 3, with $`\mathrm{\Omega }_0=\mathrm{\Omega }_2`$ for (39) and with $`\mathrm{\Omega }_0=\mathrm{\Omega }_1`$ for (40). They give a good prediction of the island of good transfer of the regime A observed numerically.

For the two sequences, the islands of good transfer to the state $`|2`$ of the regime A occur with absorption of one $`\omega _1`$photon.

### B Regime B

This regime is characterized by the transition 1-2 quasi-resonant with the frequency $`\omega _2`$ and the transition 2-3 quasi-resonant with the frequency $`\omega _1`$. This process can be analyzed as the channel B perturbed (in the sense of non-resonant perturbation theory) by the channel A and is described by the effective Hamiltonian $`\stackrel{~}{𝖧}_\text{c}^\text{B}=𝒯\stackrel{~}{𝖧}_\text{c}^\text{A}`$:

$$\stackrel{~}{𝖧}_\text{c}^\text{B}=\frac{1}{2}\left[\begin{array}{ccc}\frac{\left[\mathrm{\Omega }_1\left(t\right)\right]^2}{2\mathrm{\Delta }_1}& \mathrm{\Omega }_2\left(t\right)& 0\\ \mathrm{\Omega }_2\left(t\right)& 2\left(\mathrm{\Delta }_1+\delta \right)+\frac{\left[\mathrm{\Omega }_1\left(t\right)\right]^2}{2\mathrm{\Delta }_1}\frac{\left[\mathrm{\Omega }_2\left(t\right)\right]^2}{2\mathrm{\Delta }_2}& \mathrm{\Omega }_1\left(t\right)\\ 0& \mathrm{\Omega }_1\left(t\right)& 2\left(\mathrm{\Delta }_1+\mathrm{\Delta }_2\right)+\frac{\left[\mathrm{\Omega }_2\left(t\right)\right]^2}{2\mathrm{\Delta }_2}\end{array}\right].$$
(41)
The regions of high transfer efficiency to the state $`|2`$ are bounded in the same manner as in the regime A by the lines (V A) and (V A) to which we apply the transformation $`𝒯`$ (II).

### C Regime C

The regime $`C`$ is characterized by a mixture of regimes $`A`$ and $`B`$ for which the transitions 1-2 and 2-3 are both quasi-resonant with the same frequency $`\omega _2`$. As long as the $`\omega _1`$field is perturbative for both transitions, we have the following effective Hamiltonian

$$\stackrel{~}{𝖧}_\text{c}^\text{C}=\frac{1}{2}\left[\begin{array}{ccc}\frac{\left[\mathrm{\Omega }_1\left(t\right)\right]^2}{2\mathrm{\Delta }_1}& \mathrm{\Omega }_2\left(t\right)& 0\\ \mathrm{\Omega }_2\left(t\right)& 2\left(\mathrm{\Delta }_1+\delta \right)+\frac{\left[\mathrm{\Omega }_1\left(t\right)\right]^2}{2\mathrm{\Delta }_1}\frac{\left[\mathrm{\Omega }_1\left(t\right)\right]^2}{2(\mathrm{\Delta }_2\delta )}& \mathrm{\Omega }_2\left(t\right)\\ 0& \mathrm{\Omega }_2\left(t\right)& 2\left(\mathrm{\Delta }_1+\mathrm{\Delta }_2+\delta \right)+\frac{\left[\mathrm{\Omega }_1\left(t\right)\right]^2}{2(\mathrm{\Delta }_2\delta )}\end{array}\right],$$
(42)
in the basis $`\{|1;0,0`$,$`|2;0,1,|3;0,2\}`$. No efficient transfer is observed in this regime.

### D Regime D

This regime is such that the only quasiresonance is between the states 1 and 2 with $`\omega _2`$. In this case, in the basis $`\{|1;0,0`$,$`|2;0,1`$,$`|3;0,2\}`$ we can construct an effective Hamiltonian from the previous one \[Eq. (42)\] considering that the $`\omega _2`$field is perturbative for the transistion 2-3:

$$\stackrel{~}{𝖧}_\text{c}^\text{D}=\frac{1}{2}\left[\begin{array}{ccc}\frac{\left[\mathrm{\Omega }_1\left(t\right)\right]^2}{2\mathrm{\Delta }_1}& \mathrm{\Omega }_2\left(t\right)& 0\\ \mathrm{\Omega }_2\left(t\right)& 2\left(\mathrm{\Delta }_1+\delta \right)+\frac{\left[\mathrm{\Omega }_1\left(t\right)\right]^2}{2\mathrm{\Delta }_1}\frac{\left[\mathrm{\Omega }_1\left(t\right)\right]^2}{2(\mathrm{\Delta }_2\delta )}\frac{\left[\mathrm{\Omega }_2\left(t\right)\right]^2}{2\mathrm{\Delta }_2}& 0\\ 0& 0& 2\left(\mathrm{\Delta }_1+\mathrm{\Delta }_2+\delta \right)+\frac{\left[\mathrm{\Omega }_1\left(t\right)\right]^2}{2(\mathrm{\Delta }_2\delta )}+\frac{\left[\mathrm{\Omega }_2\left(t\right)\right]^2}{2\mathrm{\Delta }_2}\end{array}\right].$$
(43)
We can remark that this Hamiltonian is valid for the field amplitude $`\mathrm{\Omega }_2`$ below the position of the resonance occuring between the transition 2-3 and the $`\omega _2`$ field that can be estimated by

$$\mathrm{\Omega }_2^\text{r}2\sqrt{\mathrm{\Delta }_2\left(\mathrm{\Delta }_1+\mathrm{\Delta }_2+\delta \right)}\text{and }\mathrm{\Delta }_1+2\mathrm{\Delta }_2+\delta 0.$$
(44)
This limit is represented as the bent dashed line crossing the figure horizontally in Figs 2 and 3 (with $`\mathrm{\Omega }_0=\mathrm{\Omega }_2^\text{r}`$). Below this limit, one is allowed to decouple the states $`|2;0,1`$ and $`|3;0,2`$ from the Hamiltonian (42). A more detailed analysis of this regime shows that a dynamical resonance between the transition 1-2 and the $`\omega _1`$field, induced by the $`\omega _2`$field occurs approximately for

$$\mathrm{\Omega }_2=\mathrm{\Omega }_2^{\text{dr}}\sqrt{\mathrm{\Delta }_1\left(\mathrm{\Delta }_1+2\delta \right)}.$$
(45)
It is obtained when the difference of the dressed eigenvalues connected to $`|1;0,0`$ and $`|2;0,1`$ (calculated without the Stark shifts) compensates the difference of the frequencies $`\delta `$. This additional resonance is described as dynamical since it occurs beyond a threshold of the $`\omega _2`$field amplitude. It is represented as the bent dashed line crossing the figure vertically (which separates the regimes $`D`$ and $`D^{}`$) in Figs 2 and 3 with $`\mathrm{\Omega }_0=\mathrm{\Omega }_2^{\text{dr}}`$. The Hamiltonian (43) is thus approximately valid before the dynamical resonance (45).

Below this dynamical resonance, this Hamiltonian (43) is very similar to the one describing the process named SCRAP (acronym for Stark chirped Rapid adiabatic passage) between the states $`|1;0,0`$ and $`|2;0,1`$ . The pump of this process is here $`\mathrm{\Omega }_2`$ and the Stark pulse $`\mathrm{\Omega }_1`$. We have here $`\mathrm{\Omega }_2`$ acting additionally as a Stark pulse.

It is important to note that when $`\mathrm{\Delta }_1=\delta `$, the field $`\omega _2`$ is exactly in resonance with the transition 1-2, and it cannot induce any complete population transfer from $`|1`$ to $`|2`$. Below this boundary (plotted as a full line in Figs 2 and 3), i.e. for $`\mathrm{\Delta }_1<\delta `$, the topology does not allow the transfer from $`|1`$ to $`|2`$. Above this aboudary ($`\mathrm{\Delta }_1>\delta `$), the transfer is possible as shown by the surfaces of quasienergies (for $`\mathrm{\Delta }=\mathrm{\Delta }_1=\mathrm{\Delta }_2=9\delta /10)`$ in Fig. 8. The eigenvalues of (43) (not shown) fit well these surfaces below the dynamical resonances $`\mathrm{\Omega }_2<\mathrm{\Omega }_2^r.`$ Fig. 8 shows that the conical intersection for $`\mathrm{\Omega }_2=0`$ between the surfaces connected to $`|1;0,0`$ and the target state $`|2;0,1`$ bound the adiabatic connection between these states. This characterizes a transfer to the state $`|2`$ with absorption of one $`\omega _2`$photon. This boundary is calculated from the effective Hamiltonian (43):

$`\mathrm{\Omega }_1=2\sqrt{\mathrm{\Delta }{\displaystyle \frac{\mathrm{\Delta }^2\delta ^2}{2\delta \mathrm{\Delta }}}}.`$

It is plotted in Figs 2 and 3 as a full line in the region $`D`$ and bounds the upper island of good transfer of this region.

The cases beyond the dynamical resonance are studied in the next section.

## VI Strong field regimes

The strong field regime occurs when $`\mathrm{\Omega }_1\left(t\right),\mathrm{\Omega }_2\left(t\right)\delta `$. For $`\mathrm{\Delta }_1=\mathrm{\Delta }_2`$, this corresponds to a weak spin coupling since one has then $`4\left|\xi \right|\mathrm{\Omega }_1\left(t\right),\mathrm{\Omega }_2\left(t\right)`$. More resonances occur in this case and the previous effective Hamiltonians are no more valid. We will study in detail the interesting regime $`D^{}`$ which gives quite large areas of transfer to state $`|2`$.

This regime is located below the resonance (44) and beyond the dynamical resonance (45), when the transition 1-2 is quasi-resonant with both the $`\omega _1`$ and $`\omega _2`$fields and when the transition 2-3 is not resonant with either the $`\omega _1`$field or the $`\omega _2`$field. This regime is thus characterized by the effective dressed Hamiltonian

$$𝖪^{\text{D’}}=\text{i}\delta \frac{}{\theta }+\frac{1}{2}\left[\begin{array}{ccc}0& \mathrm{\Omega }_2\left(t\right)+e^{\text{i}\theta }\mathrm{\Omega }_1\left(t\right)& 0\\ \mathrm{\Omega }_2\left(t\right)+e^{\text{i}\theta }\mathrm{\Omega }_1\left(t\right)& 2\left(\mathrm{\Delta }_1+\delta \right)\frac{\left[\mathrm{\Omega }_1\left(t\right)\right]^2}{2(\mathrm{\Delta }_2\delta )}\frac{\left[\mathrm{\Omega }_2\left(t\right)\right]^2}{2\mathrm{\Delta }_2}& 0\\ 0& 0& 2\left(\mathrm{\Delta }_1+\mathrm{\Delta }_2+\delta \right)+\frac{\left[\mathrm{\Omega }_1\left(t\right)\right]^2}{2(\mathrm{\Delta }_2\delta )}+\frac{\left[\mathrm{\Omega }_2\left(t\right)\right]^2}{2\mathrm{\Delta }_2}\end{array}\right].$$
(46)
It is equivalent to a two-level system driven by a bichromatic field  with additional Stark shifts. The surfaces of quasienergies as functions of the normalized Rabi frequencies $`\mathrm{\Omega }_1/\delta `$ and $`\mathrm{\Omega }_2/\delta `$ (for $`\mathrm{\Delta }=\mathrm{\Delta }_1=\mathrm{\Delta }_2=7\delta /5`$) are displayed in Fig. 9. This figure shows that the two conical intersections, one for $`\mathrm{\Omega }_1=0`$ and one for $`\mathrm{\Omega }_2=0`$, bound the adiabatic connection between the initial state $`|1;0,0`$ and the target state $`|2;1,2`$. We calculate the boundaries using the effective Hamiltonian (46), which are plotted as full lines in Figs 2 and 3:

$`\mathrm{\Omega }_1`$ $`=`$ $`2\sqrt{(\mathrm{\Delta }\delta )\left[2\delta \mathrm{\Delta }2\sqrt{\delta \left(2\delta \mathrm{\Delta }\right)}\right]},`$
$`\mathrm{\Omega }_2`$ $`=`$ $`2\sqrt{\mathrm{\Delta }\left[\delta \mathrm{\Delta }\sqrt{\delta \left(\delta 4\mathrm{\Delta }\right)}\right]}.`$
This process corresponds to a multiphoton transfer to the state $`|2`$, with absorption of two $`\omega _2`$photons and emission of one $`\omega _1`$photon.

The analysis of the topology allows to improve the transfer efficiency. It shows indeed that a $`\omega _1`$field amplitude larger than the $`\omega _2`$field amplitude is better in this regime since the conical intersection for $`\mathrm{\Omega }_1=0`$ occurs for a larger value than the one for $`\mathrm{\Omega }_2=0`$.

This process of a two-level system driven by a bichromatic field studied in Ref  shows that the transfer can still occur for a stronger field (i.e. for a weaker spin coupling), but with absorption of more than two $`\omega _2`$photons and emission of more than one $`\omega _1`$photon. This result is shown in Fig. 10 where strong field white islands can be observed. The lower white islands correspond to good population transfer to the entangled state $`|2;k1,k`$, with $`k=1,2,3,4`$ from left to right.

## VII Conclusion

We have shown that a system of two interacting spins in an external bichromatic field is equivalent to a three level problem. We have determined the choices of laser pulses which can give a maximal final population in the entangled state. The proposed strategies are robust with respect to the external parameters. We have found that in the parameter space it is possible to find large islands where the quantum system can be transferred to the entangled state with a high efficiency. These islands of good transfer have been characterized by the topology of the surfaces of dressed states as functions of the parameters.

The methods employed here are quite general and can be applied for a large variety of systems. We anticipate interesting applications of this method in quantum computing and quantum communication.

## Acknowledgments

We acknowledge supports by INTAS 99-00019 and the Conseil Régional de Bourgogne. S.G. thanks support from a CNRS project ”jeunes chercheurs”. RU thanks support by the Alexander Von Humboldt Foundation and l’université de Bourgogne for kind hospitality. The authors thank N. Vitanov for usefull discussions.


text:
# Abstract

### Abstract

Precise calorimetric measurements have been carried out in the 7 - 300 K temperature range on two ceramic samples of thulium 123 cuprates TmBa2Cu3O6.92 and TmBa2Cu3O6.70. The temperature dependence of the heat capacity was analyzed in the region where the pseudogap state (PGS) takes place. The lattice contribution was subtracted from the experimental data. The PGS component has been obtained by comparing electronic heat capacities of two investigated samples because the PGS contribution for the 6.92 sample is negligible. The anomalous behavior of the electronic heat capacity near the temperature boundary of PGS was found. It is supposed that this anomaly is due to peculiarities in $`N(E)`$ function where $`N`$ is the density of electronic states and $`E`$ is the energy of carriers of charge.

PACS: 74.25.Bt, 74.72.Jt

Introduction

Last years a number of articles devoted to research of features of various properties, connected with so called pseudogap state (PGS), have appeared in periodicals. The PGS arises in underdoped yttrium 1-2-3 and lanthanum 2-1-4 superconductors in the temperature region above the line of superconducting transition ($`T_c<`$ $`T<`$ $`T`$\*) and at concentrations of carriers of charge, smaller than the critical value $`p_c`$ appropriate to the point of optimal doping (POD) (Fig. 1).

Hundreds publications were devoted to studying of unusual manifestations of the PGS in various properties. The most convincing proofs of existence of the PGS were received by direct methods - photoemission with the angular resolution (ARPES) and methods of electronic tunneling \[1-3\]. These data make evident an appreciable decrease of the density of electronic states in the field of PGS. The density of electronic states near the Fermi level has V-shaped minimum. If temperature increases and gets over a boundary line $`T`$*$`(p)`$, this minimum disappears and the system goes out of the PGS.

At first the line $`T`$\*($`p)`$ was perceived as a boundary of the region where NMR spin-lattice relaxation deviates significantly from the Korringa rule . Later it has been shown that experimental investigations of different physical properties determine different standings of the boundary of this state . The border derived from the NMR measurements of the Knight shift or from the measurements of spin-lattice relaxation is marked in Fig. 1 with $`T_{cr}(p)`$. It is situated at higher temperatures, than the border derived from thermodynamic and kinetic properties $`T`$\*($`p)`$. Such a discrepancy allows several researchers to suggest that there are two regions on the phase diagram, corresponding to weak and strong PGS . Discussing the problem, we use the notations of ref.  throughout the work. The upper temperature boundary denoted by $`T_{cr}`$, is defined as a border of crossover phenomena in NMR experiments. The lower boundary is denoted traditionally by $`T^{}(p)`$.

Two probable mechanisms of the PGS formation are discussed in the literature:

1. The Cooper pairs exist above the temperature of superconducting phase transition forming the incoherent paired states. The number of the pairs increases with decreasing temperature and at the temperature $`T_c`$ the incoherent pairing transforms into the correlated superconducting state .

2. The charge carriers interact with the fluctuations of magnetic or charge short-range order (spin or charge density waves) \[9-11\]. Such an interaction can yield the V-shaped minimum in the density of electron states near the Fermi level .

It is difficult to recognize what mechanism of PGS formation is actual. Many authors suppose the second mechanism to be more plausible, than first .

Along with direct examinations of features of electronic states in PGS of 1-2-3 and 2-1-4 cuprate HTSC by the methods of ARPES and electronic tunneling, the studying of thermodynamic properties of these substances can make a considerable contribution to the insight into the subject. The investigation of unusual peculiarities in thermodynamic properties of 1-2-3 and 2-1-4 cuprate HTSC was started by Junod and co-workers in the early 90s . Main investigations were carried out by Loram and co-workers after the middle of 90s \[16-20\] and are prolonged now. Such investigations are of great interest because of many problems in the theoretical interpretation of the phenomena observed. Another problem is the separation of the electronic contribution to the heat capacity. For the normal state above $`T_c`$, the electronic contribution $`C_{el}`$ is not greater than 2 - 3 % of total heat capacity. Change of $`C_{el}`$ connected with PGS formation is significantly less, namely 0.2 - 0.3 % of total heat capacity. Thus, even minor error in the separation of lattice, electronic, and magnetic contributions can lead to a significant error in the values describing electronic properties of cuprate HTSC.

To determine the electronic contribution at the PGS in yttrium cuprates YBCO6+X, Loram and co-workers used the lattice heat capacity $`C_{lat}`$ of dielectric YBCO6 as a reference value. Probable differences between the values for a reference substance and substance under investigation were corrected using the sum of Einstein functions. The parameters in the functions were derived from the fitting of experimental data at low temperatures. The extrapolation of these components into field of PGS has allowed authors to separate electronic heat capacity $`C_{el}`$ of the cuprates investigated. This way of calculation yields the value of $`C_{el}`$ containing also the differences in magnetic and anharmonic contributions. The approximation of the difference by Einstein functions and its extrapolation in the field of PGS can produce significant errors in the electronic contribution calculated.

The aim of this work is to use the experimental results for the sample close to the optimal doping as the reference data. We think that this way of calculation of electronic contribution in the PGS is more correct.

Experimental

The calorimetric measurements of TmBa2Cu3O6.92 and TmBa2Cu3O6.70 were carried out using automatic low-temperature vacuum adiabatic calorimetric system. The equipment was described elsewhere  but only one exception: the calorimeter we used was made of copper and covered with silver instead of that made of pure nickel . Internal volume of the calorimeter was about 6 cm3. Heat capacity of empty calorimeter was measured in the temperature range 6 - 310 K. The accuracy of the calorimetric results was tested using the standard reference sample - benzoic acid. Our results agree with reliable data for benzoic acid taken from the literature \[22-24\] within the limits of $`\pm `$2 % over the temperature range 6 - 10 K, 0.5 % for 10 - 30 K, 0.2 % for 30 - 60 K, and 0.1 % above 60 K. During the measurements, temperature increase at the heat pulse was 1 to 2 K at $`T<`$ 30 K and 3 - 5 K over the temperature range 30 - 300 K. The average deviation of the experimental values from the smoothed curve was about 0.02 % at temperatures 100 – 300 K. The deviation increased with decreasing temperature, growing up to 1 % at 10 K. A total of 300 - 400 experimental points were performed for each sample.

Ceramic TmBa2Cu3OX was synthesized in the solid-state reaction according to the standard procedure using high-purity oxides Tm2O3, BaO, and CuO. Before the synthesis, the oxides Tm2O3 and CuO were annealed at 750oC and 700oC, respectively, to remove volatile impurities. The synthesis was performed in a corundum crucible in the temperature range from 800 to 900oC, step by step with an interval of 25oC, for 25 hours each. Before each step, the sample was thoroughly ground in an agate mortar. To receive the sample with optimal oxygen content $`X`$ = 6.92, the heating was performed in an atmosphere with excess amount of oxygen. The sample with $`X`$ = 6.7 was prepared from the sample with $`X`$ = 6.92 which was annealed in air at $`T`$ = 590oC, then quenched into liquid nitrogen and annealed at 100oC for two days.

Thulium cuprates were chosen for the investigation instead of yttrium cuprates because aluminum impurity in thulium cuprate after the synthesis in a corundum crucible was several tens lower than in yttrium cuprate. $`X`$-ray powder diffraction showed ceramics TmBa2Cu3OX to be nearly monophase and to contain the impurities of Tm2BaCuO5 and BaCuO2. Total amount of these phases was not greater than 2-3 %. The analysis showed that the amount of impurities did not change when the oxygen content decreased from 6.92 to 6.70. The analysis of structural factors sensing to homogeneity of oxygen distribution (orthorhombicity and broadening of basal reflections) has shown a high degree of homogeneity both in the sample with $`X`$ = 6.92 and with $`X`$ = 6.70.

Results and Discussion

Heat capacity $`C_p`$ is the sum of several contributions

$`C_p=C_{harm}+C_{anh}+C_{el}+C_{magn}`$, (1)

where $`C_{harm}`$ is the contribution from harmonic vibrations in a lattice, $`C_{anh}`$ is that from anharmonicity, $`C_{el}`$ and $`C_{magn}`$ are the electronic and magnetic contributions, respectively. $`C_{el}`$ contains the contribution from the heat capacity of ordinary Fermi particles ($`C_s)`$ that constitutes the major portion of $`C_{el}`$ for the sample 1 with X = 6.92. Besides $`C_s`$, $`C_{el}`$ in the sample 2 with $`X`$ = 6.70 contains the contribution from the PGS ($`C_{PGS})`$. In the sample with $`X`$ = 6.92, a very small contribution of $`C_{PGS}`$ can also be, since the PGS in 1-2-3 cuprates disappears at $`X`$ 6.97.

The lattice contribution $`C_{harm}`$ was calculated by fitting the experimental data to the sum of Debye and Einstein functions according to the procedure described in . The fitting was performed at low temperatures. The sum of the electronic, magnetic, and anharmonic terms $`\gamma _{anh+el+magn}`$ = ($`C_{anh}+C_{el}+C_{magn})`$/T for the samples investigated is shown in Fig. 2 as a function of temperature over the temperature range 100 - 300 K. We suppose that the anharmonic and magnetic contributions to the heat capacity for both samples are nearly identical. At least, we state with certainty that the difference between those contributions is much greater for YBCO6 and YBCO6+X, compared by Loram \[16-20\], than for TmBa2Cu3O6.7 and TmBa2Cu3O6.92. The reason is the difference in structure and in magnetic order between the compared yttrium cuprates.

Our experimental data were treated in the following way. After substraction of lattice contribution from total heat capacity, the function $`f(T)`$ was derived:

$`f(T)`$ = {$`C_{anh}(X`$=6.92) / $`T+\gamma _{el}(X`$=6.92) + $`C_{magn}(X`$=6.92)/$`T`$} –

{$`C_{anh}(X`$=6.70)/ $`T+\gamma _{el}(X`$=6.70) + $`C_{magn}(X`$=6.70)/$`T`$ }. (2)

The function $`f(T)`$ is shown in Fig. 3. If the anharmonic and magnetic contributions are nearly the same, the difference is

$`f(T)=\mathrm{\Delta }\gamma _s\gamma _{PGS}(X`$=6.70). (3)

The first term is positive and increases slightly with increasing temperature . Function $`\mathrm{\Delta }\gamma _s(T)`$ has no extremum. Hence, the wavy anomalies in the Fig. 3 are caused by the second term in equation 3. The minimum of the $`f(T)`$ is the result of the maximum of the function $`\gamma _{PGS}(X`$ = 6.70) that exists in the temperature range 200 - 250 K. The $`f(T)`$ tends to zero as temperature increases up to 300 K indicating that the PGS transforms into other state.

Moca and Janko  have analyzed the experimental data on electronic heat capacity measured by Loram and co-workers. The analysis was based on the first point of view mentioned above: the incoherent Cooper pairs exist in the PGS. Moca and Janko supposed that $`\gamma _{el}`$ consists of two contributions:

$`\gamma _{el}(T)=\gamma _s(T)+\gamma _p(T)`$, (4)

where $`\gamma _s(T)`$ is the single-particle contribution from Fermi particles. This contribution is similar to the first term in Eq. 3. It increases slightly and monotonically with increasing temperature. The second term in Eq.4, $`\gamma _p(T)`$ is the contribution from the formation of the incoherent Cooper pairs. According to Ref. , $`\gamma _p(T)`$ depends on temperature like ($`T`$\*/$`T)^3`$exp(-2$`T`$\*/$`T)`$ with a maximum near $`T=T`$\*. According to analysis of the data reported by Loram et al., the authors  suppose the position of maximum of $`\gamma _{el}(T)`$ to shift to lower temperatures when the oxygen content increases. For the cuprate with $`X`$ = 6.7, the maximum of function $`\gamma _{el}(T)`$ was estimated to be within the temperature range 120 to 130 K . The experimental results in Fig. 3 clearly show that there is no maximum over the temperature range 120 - 130 K.

If there is a systematic error in the separation of harmonic and anharmonic contributions, the error in the electronic contribution can be as high as tens percent. Such an error in the calculations is equivalent to the experimental error of 0.1 - 0.2 % in the total heat capacity. It means that we analyze the function $`C_p(T)`$ in trying to recognize its peculiarities comparable with an accuracy of the experiments. This illustrates how complicate is to extract the electronic heat capacity and correctly determine its features.

It is possible to assume, that observed anomalies are related to impurities in samples. In fact, copper oxide is a starting material for the synthesis and it undergoes two phase transitions, at $`T`$ = 212.6 K and $`T`$ = 229.5 K . Nevertheless, to produce such an effect in heat capacity, the samples have to contain at least 4 or 5 % of copper oxide. We carefully investigated the samples by means of X-ray powder diffraction with a limit of detection about 2 - 3 % in searching for the copper oxide impurity. No traces of CuO were found. Besides, the effect observed in Fig. 3 is in the difference between heat capacities of two samples. The sample with $`X`$ = 6.70 was received after gentle heat treatment (at 590oC) of the sample with $`X`$ = 6.92. Copper oxide starts to decompose at 1061oC and it means that both of the samples contain the same amount of CuO. The probable effect of the phase transitions in copper oxide should be eliminated in the evaluation of the $`f(T)`$ function (Eq. 2). Thus, the copper oxide impurity cannot explain the anomalous behavior of the heat capacity. The amplitude of the anomalous heat capacity, by our data, decreases as the sample composition approaches the point of optimal doping. These facts lead us to the conclusion that the peculiarities observed are connected with the transformation of the samples into the PGS.

Recent theoretical investigations examined the electronic systems interacting with charge or spin short-range fluctuations . The interaction is shown to be responsible for the formation of pseudogap structure near the Fermi level. The evaluations based on the mean field approximation fail to describe correctly the properties of the system. At proper consideration of the fluctuations in the PGS it is found that, besides V-shaped minimum, the sharp peaks in the density of electronic states can form . It would appear reasonable that the effective value $`N(E)`$ near the Fermi level can be very complex and sensitive to the changes in the system near the PGS. In that case the transformation into the PGS can go with complex anomalous behavior of various physical properties. First of all, these are the properties connected with the density of states of charge carriers. We suppose that the observed anomalous behavior of the electronic heat capacity is the result of the transformation. Probably, the same phenomenon is responsible for unusual function $`C_p(T)`$ for lanthanum 2-1-4 cuprates described in . We assume that our experimental data for thulium cuprates, together with the results on the heat capacity of lanthanum 2-1-4 cuprates , can be qualitative confirmation of the theoretical calculations of Sadovskiy et al.

The work was supported in part by the Russian Foundation for Basic Researches (grant N.00-02-17914), by Scientific Programs ”High-temperature Superconductivity” (grant 98009) and ”Universities of Russia” (grant 1785), and by the FAP ”Integration” (grant 274).

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Figures

Fig. 1. Schematic phase diagram for the cuprates

Fig. 2. Electronic, anharmonic, and magnetic contributions to the heat capacity of thulium cuprates

Fig. 3. Function $`f(T)`$