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# Phase diagram of an asymmetric spin ladder

## Abstract

We investigate an asymmetric zig-zag spin ladder with different exchange integrals on both legs using bosonization and renormalization group. When the leg exchange integrals and frustration both are sufficiently small, renormalization group analysis shows that the Heisenberg critical point flows to an intermediate-coupling fixed point with gapless excitations and a vanishing spin velocity. When they are large, a spin gap opens and a dimer liquid is realized. Here, we find a continuous manifold of Hamiltonians with dimer product ground states, interpolating between the Majumdar-Ghosh and sawtooth spin-chain model.

PACS numbers: 75.10Jm, 75.10b, 71.10.Hf

The interplay of geometric frustration and quantum fluctuations, and eventually broken translational invariance, in low-dimensional spin systems gives rise to novel magnetic phases. Examples include: spin chains with interactions beyond nearest neighbors, spin ladders, triangular and Kagomé systems. Spin ladders in particular, have attracted much interest and several model problems are well understood, and highlight the role played by frustration. Spin-isotropic two-leg ladders with railroad geometry quite generally lead to a singlet ground state separated by a finite excitation gap from the first triplet states. Zig-zag ladders are more strongly frustrated and, depending on the ratio of the leg to rung exchange integrals, may have gapless spin liquid ground states or gapped dimer states. Compounds like $`Cu_2(C_5H_{12}N_2)_2Cl_4`$ and $`CuGeO_3`$ have been suggested to be described as railroad and zig-zag ladders, respectively .

Little work has been done on asymmetric spin ladders where the exchange integrals on both legs differ. Only the extreme case where one leg of a zig-zag ladder is missing entirely (sawtooth or $`\mathrm{\Delta }`$-chain) has been solved. The ground state of this model is a product of nearest-neighbor singlets and there is a spin gap, as in the Majumdar-Ghosh model. The properties of the excitations in both models are different, however. Sawtooth chains may describe the material $`YCuO_{2.5}`$ . Here, we perform a systematic study of asymmetric zig-zag spin ladders. Important questions concern possible new phases generated by the leg-asymmetry, their excitation spectra and their physical properties as well quantitative changes brought about by leg-asymmetry to the excitations in the more usual phases found on zig-zag ladders (spin liquid, Néel and dimer states).

We consider a Heisenberg model on the structure shown in Figure 1, and represent this as a chain with an alternating next-nearest-neighbor (NNN) exchange

$$H=\underset{l}{}\left\{J_1𝐒_l𝐒_{l+1}+\left[J_2+(1)^l\delta \right]𝐒_l𝐒_{l+2}\right\},$$
(1)
where $`J_11`$ and $`J_2\pm \delta `$ are the nearest-neighbor (NN) and alternating NNN coupling constants, respectively.

$`\delta =0`$ is the ordinary zig-zag ladder or frustrated spin chain, and fixing in addition $`J_2=\frac{1}{2}J_1`$ gives the exactly solved Majumdar-Ghosh (M-G) model . The sawtooth chain has $`\delta =J_2=\frac{1}{2}J_1`$.

Following the general approach to map the quantum spin model to a continuum field theory and using the standard dictionary of Abelian bosonization, we obtain an effective boson Hamiltonian $`H=H_0+H_1`$ with

$`H_0`$ $`=`$ $`{\displaystyle 𝑑x\frac{u}{2\pi }\left[K(\pi \mathrm{\Pi })^2+\frac{1}{K}(_x\mathrm{\Phi })^2\right]},`$ (2)
$`H_1`$ $`=`$ $`{\displaystyle 𝑑x\left[\frac{g_3}{2(\pi a)^2}\mathrm{cos}4\mathrm{\Phi }+\frac{g_1}{\pi ^2a}\left(_x\mathrm{\Phi }\right)\mathrm{cos}2\mathrm{\Phi }\right]}.`$ (3)
$`\mathrm{\Phi }(x)`$ is a bosonic phase field and $`\mathrm{\Pi }(x)`$ its canonically conjugate momentum. $`u`$ and $`K`$ are the effective spin velocity and coupling constants, including the effects of marginal interactions. $`a`$ is a short-distance cutoff, $`g_31J_2/J_{2c}`$ is the Umklapp-scattering amplitude and $`g_1\delta `$ is the amplitude of the alternating NNN field. In this paper, we only consider the case $`J_1/2J_2>\delta `$, while, for $`J_2>0.5J_1`$, quite different field theory treatments are required.

For $`\delta =0`$, the model (1) is well understood . Its elementary excitations are spinons which are gapless for $`J_2<J_{2c}=0.2412`$ when frustration is irrelevant and the ground state is unique, or gapped for $`J_2>J_{2c}`$ when frustration is relevant and the ground state is doubly degenerate. In the field theory (2), (3), this translates into the $`g_3`$ term being either marginally irrelevant, leading to the weak-coupling Heisenberg fixed point ($`K^{(H)}=1/2,g_3^{(H)}=0`$) , or relevant, yielding a strong-coupling dimer state. When the SU(2) spin symmetry is broken, a Néel state or an easy-plane spin liquid may form. Introducing dimerization, i.e. an alternating $`J_1`$, produces an effective confining potential between the spinons. The elementary excitations become a spin triplet and a spin singlet above the unique ground state. In the language of field theory, the external dimerization corresponds to a relevant term $`\mathrm{sin}2\mathrm{\Phi }`$ which lifts the double degeneracy of the dimer ground state.

Qualitative results on the influence of the new interaction ($`g_1`$) can be obtained from physical considerations alone. Firstly, the scaling dimensions of the Umklapp and nearest neighbor alternation terms $`g_3`$ and $`g_1`$ are

$$d_{g_3}=4K,d_{g_1}=K+1.$$
(4)
At the Heisenberg fixed point, $`g_3`$ is marginal with $`d_{g_3}=2`$, while the $`g_1`$-term with $`d_{g_1}=3/2`$ is relevant. We conclude that $`g_1`$ destabilizes the isotropic Heisenberg fixed point and the spin liquid ground state. On the other hand, there is no standard strong coupling theory for the $`g_1`$-term. Usually (e.g. $`g_3\pm \mathrm{}`$), the boson field $`\mathrm{\Phi }(x)`$ locks into a constant value with small fluctuations, and an associated excitation gap. Such a phase locking, however, is forbidden by the $`_x\mathrm{\Phi }`$-prefactor to the cos$`(2\mathrm{\Phi })`$-term in $`H_1`$. Secondly, the $`g_1`$-term, induced by the alternating NNN interaction, does not confine the spinons and plays a role very different from the external dimerization, as can be checked in the dimer state by comparing the sawtooth chain with the M-G model. Moreover, from differences in the size of the spin gaps in these two models, it follows that the $`g_1`$-term quite generally counteracts the Umklapp term while an external NN dimerization would cooperate.

That $`g_1`$ opens no spin gap despite being a relevant perturbation of the Heisenberg fixed point, is also corroborated by the absence of a magnetization plateau in our model in small magnetic fields. A necessary condition for the formation of a magnetization plateau in the absence of modulated external fields is an alternating component of the exchange integrals . For an alternating NN exchange, a magnetization plateau is observed in small magnetic fields, but alternating NNN exchange, it is only observed in high fields .

We now perform a perturbative renormalization group (RG) analysis by mapping the model on a modified (by $`g_1`$) classical 2D XY-model. Introducing the reduced variables $`y_3=g_3/\pi u`$ and $`y_1=g_1/\sqrt{2}\pi u`$, we obtain the linearized RG equations

$`{\displaystyle \frac{dK}{dl}}`$ $`=`$ $`y_3^2K^2+y_1^2K^4`$ (5)
$`{\displaystyle \frac{dy_3}{dl}}`$ $`=`$ $`(24K)y_3+K^2y_{1}^{}{}_{}{}^{2}`$ (6)
$`{\displaystyle \frac{dy_1}{dl}}`$ $`=`$ $`(1K)y_14K^2y_1y_3`$ (7)
$`{\displaystyle \frac{du}{dl}}`$ $`=`$ $`{\displaystyle \frac{1}{2}}uy_1^2(1+K)K^2.`$ (8)
under a change of length scale $`aae^{dl}`$. These equations, and our solutions to be discussed below, can also accommodate anisotropy in the NN and NNN exchange integrals. The RG equation for the spin velocity $`u`$ is a consequence of the anisotropy of the $`g_1`$-interaction in the classical 2D XY-model, i.e. its non-retarded but non-local character in the quantum field theory (3), and has been discussed before in the 1D electron-phonon problem. For $`y_1=0`$, one finds the three generic phases discussed earlier: (i) a weak-coupling spin liquid phase ($`g_3^{}=0,K^{}1/2`$) terminating at the isotropic Heisenberg fixed point $`K^{(H)}=1/2`$; (ii) a strong coupling Néel phase $`g_3^{}\mathrm{}`$; (iii) a strong coupling dimer phase $`g_3^{}\mathrm{}`$. Moreover, $`u`$ is not renormalized for $`y_1=0`$. Spin-rotation invariant models scale along the separatrix between Néel and spin liquid phases, or along its continuation into the dimer regime.

Taking $`y_1`$, the most relevant perturbation, finite, changes this simple picture. Quite generally, the corrections to the RG flow of $`K`$ and $`g_3`$ are positive, while those from $`g_3`$ are negative. In the spin liquid phase, close to the isotropic Heisenberg fixed point, the alternating NNN exchange will increase both $`K`$ and $`y_3`$, and therefore reverse the direction of the RG flow, compared to the $`y_1=0`$ situation. The sign of this effect agrees with the spin gap reduction in the dimer phase when going from the M-G to the sawtooth model. The magnitude of the effect is a direct consequence of the scaling dimension $`d_{g_1}`$. Figure 2 shows a family of solutions of the RG equations, projected on the $`y_3K`$-plane, which have been linearized for the purpose of the figure to accurately control spin-rotation invariance (cf. below).

The flow reversal is seen in much of the first quadrant. When $`K`$ is increased sufficiently by $`y_1`$, this perturbation becomes irrelevant, however, and the RG flow bends back to a weak coupling fixed line ($`K^{}1,y_3^{}=0,y_1^{}=0`$), describing a spin liquid with an increased easy-plane anisotropy. Its spin velocity $`u`$ is decreased but remains finite.

More interesting is the spin-rotation invariant line ($`y_3=4K2`$ in the linearized RG). While the initial flow towards the Heisenberg fixed point also reverses its direction under the influence of $`y_1`$, it reaches a new finite-coupling fixed point $`(K^{}0.578,y_3^{}0.315,y_1^{}\pm 0.544)`$, resp. $`(K^{}=0.6,y_3^{}=0.4,y_1^{}=\pm 0.8)`$ in the linearized RG. This fixed point is attractive for spin-rotation invariant systems, and repulsive otherwise with a flow into the spin liquid or Néel phases for easy plane (easy axis) anisotropy. At the fixed point, the renormalized spin velocity vanishes, $`u^{}=0`$. This conclusion follows from Eq. (8) and is independent of the exact value of the fixed point as long as it is located on the RG separatrix with $`1/2<K<\mathrm{}`$. Consequently, conformal invariance is broken, and we do not expect power-law decay of the correlation functions. Thermodynamic properties will be different from a Heisenberg chain: the specific heat will show nonlinear temperature dependence, and the magnetic susceptibility will depend on temperature. This state is significantly different from the Luttinger-type spin fluid state of the Heisenberg model. The fixed-point Hamiltonian can be rewritten as $`H^{}=u^{}(K^{},g_1^{},g_3^{})`$ where $``$ is independent of $`u^{}`$. It becomes trivial, $`H^{}=0`$, at the fixed point because $`u^{}=0`$. We interpret this as our spins effectively decoupling at the lowest energy scales, i.e. a kind of asymptotic freedom in this spin-rotation invariant ladder.

From standard arguments, we find that the elementary excitations in the fixed point, spinon and antispinon, are still gapless. One can also provide a variational argument, based on an effective Hamiltonian $`H_1`$, Eq. (3). Minimizing its energy directly produces pairwise kink and antikink solutions corresponding to the elementary excitations with energies proportional to $`g_3`$ resp. $`g_1`$. Including the quantum fluctuations from $`H_0`$ is expected to delocalize these kinks and reduce their energies further. Using now our fixed point properties $`g_{1,3}=y_{1,3}^{}u^{}`$, $`u^{}0`$ makes the excitation gap vanish at the fixed point. Also, the numerical results of Wiessner et al.,, indicate a paramagnetic susceptibility.

A natural question arises here: Is this intermediate fixed point stable against higher order perturbations? Our answer is positive although we do not attach any particular significance to the numerical values of the coupling constants, which may change as higher-order corrections are included. Its location on the RG separatrix between the Néel state and the easy-plane spin liquid is protected by spin-rotation invariance and it can be pushed neither back to the Heisenberg fixed point, nor to strong coupling, $`K\mathrm{}`$, by higher-order operators. The first option is inconsistent with the scaling dimensions, the second one would correspond, in the fermion language, to long-range pairing order which is excluded in 1D. Scaling into the dimer regime is inconsistent with the absence of a magnetization plateau.

Care should be taken when comparing these predictions to results, e.g., from exact numerical diagonalization on small clusters (size $`N`$). The finite system size will stop the RG flow at a scale $`l_N=\mathrm{ln}N`$, and the fixed point ($`l\mathrm{}`$) is not reached. However, Eqs. (5)–(8) predict a spin velocity decreased significantly by the alternating component of the NNN exchange, with an unusual size dependence which can be evaluated by integrating the RG equations up to $`l_N`$. Due to the scale dependence of the renormalization, the finite-size spectrum likely exhibits significant nonlinear corrections which, again, are size-dependent. The velocity renormalization also suggests a scale-dependence of the magnetic susceptibility. A direct solution of our model in a magnetic field is rather involved, however, because higher-order terms lead to a field-induced generation of new, relevant operators. This will be reported later.

Of course, when $`J_2`$ increases beyond a critical value $`J_{2c}(\delta )`$ now depending on the exchange alternation, the RG flows to a strong coupling fixed point, which corresponds to the quantum dimer phase. For $`y_1=0.001`$, this critical point is indicated in $`(K,y_3)`$-coordinates in Figure 2 by a star. For small $`\delta `$ and $`J_2>J_{2c}(\delta )`$, our RG equations show that the spin gap is decreased by increasing $`\delta `$, but the system will remain in the universality class of the dimer liquid.

However, we do not expect that the field theory description is very precise for $`J_2`$ near the M-G point $`J_2=0.5J_1`$. The main reason is that the correlation length, which is proportional to the inverse of the energy gap, decreases quickly when $`J_2`$ increases much beyond $`J_{2c}(\delta )`$. To access this limit, we now discuss the influence of NNN exchange alternation on the ground state and excitations of the Majumdar-Ghosh model. For the M-G model, the two linearly independent ground states, say, left or right dimer ground state, are products of nearest-neighborly singlets, respectively

$$\mathrm{\Phi }_L=\underset{l=odd}{}[l,l+1],\mathrm{\Phi }_R=\underset{l=even}{}[l,l+1],$$
(9)
where $`[i,j]=([]_i[]_j[]_i[]_j)/\sqrt{2}`$ denotes the singlet combinations of spin i and j. (9) also represents the degenerated ground state of the sawtooth model. How are these models connected? We notice that NNN exchange alternation does not modify the product states of nearest-neighbor singlets

$$H_\delta \mathrm{\Phi }_{L,R}=(1)^l\delta 𝐒_l𝐒_{l+2}\mathrm{\Phi }_{L,R}=0.$$
(10)
Furthermore, we can prove that introducing NNN exchange alternation into the M-G model, or changing it in the sawtooth chain, will not affect their ground states. There is thus an entire manifold of Hamiltonians, parameterized by $`\delta `$ with $`J_1=2J_2`$ fixed, with doubly degenerate NN-dimer product ground states $`|\mathrm{\Phi }_{L,R}`$. This kind of ground state attracted much attention recently for the experimental realization of $`SrCu_2(BO_3)_2`$ as 2D Shastry-Sutherland model.

While in these models, the focus is on the ground state, we also can characterize the elementary excitations as kinks and antikinks with finite excitation energies and different dispersions, in the dimer state of our ladder. Starting from the M-G model, the kinks can be thought of as domain walls separating the different dimer ground state configurations. From symmetry considerations, the kink and antikink properties are identical in the M-G model. With alternating NNN interaction, the symmetry between legs is broken, some properties will differ between kinks and antikinks, in particular the dispersions. However, they still survive as the elementary excitations of the asymmetric spin ladder system. The alternating NNN interaction does not serve as a confining potential for the kink and antikink, but changes the energy gap of the excitations. Based on the cluster variation method , our numerical estimates indicate that the gap decreases from $`0.234`$ in the M-G model to $`0.219`$ in the sawtooth chain with increasing $`\delta `$, while the ground state remains invariant. Particularly, for $`\delta =J_2`$, i.e. the sawtooth chain, the kink excitation is exactly a single spin on odd site and dispersionless, while an antikink is still a domain wall propagating with an effective mass.

The preceding results can also be understood from the point of view of the corresponding field model. The presence of $`g_1`$ term $`_x\mathrm{\Phi }\mathrm{cos}2\mathrm{\Phi }`$ does not lift the degeneracy of the dimer ground state, which is the constant solution minimizing the energy of the Hamiltonian with $`g_3`$ term. Near the strong coupling dimer fixed point, the $`g_3`$ term is much more relevant than the $`g_1`$ term. In this case, the soliton solutions of the $`\mathrm{cos}4\mathrm{\Phi }`$ sine-Gordon equation will survive. However, the $`g_1`$ term, although it is much less relevant than the $`g_3`$ term, gives different masses to the sine-Gordon kink and antikink solutions. This give us a rough explanation to the asymmetric kink and antikink excitations in the presence of alternating NNN coupling. The difference in (numerically determined) gap size between the M-G and sawtooth chains, is consistent with our RG results on the influence of $`\delta `$ for smaller $`J_2`$, on the spin gap magnitude.

Spin-isotropic, asymmetric zig-zag ladders are described, in the limit of weak frustration, by an intermediate-coupling fixed point with gapless excitations and a vanishing spin velocity, likely indicating a decoupling of the spins at low energy scales. For larger frustration, a more usual dimer liquid phase is realized whose spin gap decreases with increasing leg-asymmetry. A continuous manifold of Hamiltonians with the same singlet product ground state interpolates between the Majumdar-Ghosh model and the sawtooth spin chain. In addition, we find gapless spin liquid and gapped Néel states with easy-plane and easy-axis anisotropy. Extensions we currently consider include external fields and doping with charge carriers.

We are grateful to Prof. K. H. Mütter and Dr. M. Nakamura for fruitful discussions. This research was supported by Deutsche Forschungsgemeinschaft through grants no. VO436/6-2 (Heisenberg fellowship to J.V.) and VO436/7-1.


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# On the superluminal propagation of light-pulses in a ”transparent” dispersive medium

## Abstract

The mechanisms leading to a seemingly superluminal propagation of light in dispersive media are examined. The anomalous dispersion near an absorption line, involved in the first experiments displaying negative group velocity propagation, is shown to be not only simpler but also more efficient than the so-called transparent dispersion used in the later experiments of Wang et al. (Nature (London) 406, 277 (2000)) and of Dogariu et al. (Phys.Rev.A 63, 053806 (2001)). The modest pulse advances observed by these authors can in particular be reproduced with a better overall transmittance of the medium and the significant advances attained with a single-line arrangement would probably be unattainable with their gain-doublet arrangement.

Much ado was made about the late experimental evidence of superluminal propagation of light-pulses in an amplifying medium . The repeated statement that ”the peak of the pulse exits the cell before it even enters” is in part responsible for the hazardous speculations on ”superluminality” that appeared in the press. This excitement should not however hide the fact that the pulse advances reported by Wang et al.  and by Dogariu et al.  are modest (a few percent of the pulse width). More significant advances have been observed a long time ago by Chu and Wong  and by Ségard and Macke  in experiments exploiting the very large anomalous dispersion occurring near an absorption line. Astonishingly enough, Dogariu et al. hastily discard these experiments under the pretext that, due to the absorption, they ”resulted in controversies over the interpretations”  and even that the phenomenon was ”poorly understood”  ! We are not aware of the controversies alluded to by Dogariu et al. and everybody can appreciate the degree of physical understanding of the authors of Ref. and Ref.  by examining the corresponding papers. As shown hereafter, the physics underlying their experiments and those of Dogariu et al. is in fact the same but the dispersion mechanism is more efficient in the former that in the latter. Consequently the pulse advances observed by Dogariu et al. in a medium which is globally absorbing (transmittance 40%) can be reproduced with a better transmittance and the significant pulse advances obtained in Ref. and Ref. would be probably impossible to attain with their gain-doublet arrangement.

Both kinds of experiments discussed here involve negative group velocities. Garrett and McCumber  have been the first to recognise that, under suitable conditions, pulses of light can actually propagate at such velocities. A bell-shaped pulse then travels in the medium without significant alteration in such a manner that the peak of the pulse exits the medium while the signal is still increasing at its entrance. It is worth emphasising that this does not imply any breaking of the causality principle  since ”the $`t<0`$ envelope maximum seen by an observer at $`z>0`$ is not a direct reflection of the maximum of the input-pulse envelope, but arises from the action of the dispersive medium on the weak early components of that envelope” . From a spectral point of view, the phenomenon exclusively results from an interference between the different frequency components of the pulse in an anomalous dispersion region and not from a more or less selective amplification or absorption in the medium, as stated in Ref.. Variations in the transmittance of the medium with frequency have in fact detrimental effects : by privileging some frequency components, they result in dramatic distortions of the pulse and/or changes of its mean frequency, which increase rapidly with propagation distance. Unfortunately, the large anomalous dispersions required to attain significant effects are always associated with rapid variations in the transmittance of the medium with frequency. The best results are expected to be obtained when there exists a particular frequency for which the transmittance and the (negative) group velocity are simultaneously extremum, that is nearly constant in the vicinity of this frequency. This condition is fulfilled in both kinds of experiments underdiscussion . The working frequencies are indeed close to a minimum of transmittance, respectively a maximum of absorption  or a minimum of gain , coinciding with an extremum of the group velocity.

Explicit expressions of the advance of the pulse and of its distortion are conveniently derived from the transfer function which links the Fourier transforms of the complex envelopes of the input and output fields. By using the retarded time $`t^{}`$ ($`t^{}=tz/c`$ in a dilute sample), this transfer function may be written $`H(u)=\mathrm{exp}\left[G(u)\right]`$ where $`G(u)`$ is the complex gain and $`u=(\omega \omega _0)`$ is the deviation of the frequency $`\omega `$ from the central frequency $`\omega _0`$ of the pulse spectrum, taken as origin. When the anomalous dispersion originates from an ensemble of $`n`$ homogeneously broadened lines, the complex gain simply reads :

$$\mathrm{\Gamma }(u)=\underset{i=1}{\overset{n}{}}\left(\frac{G_i}{1+iu/\gamma +i\delta _i/\gamma _i}\right)$$
(1)
with $`\delta _i=(\omega _0\omega _i)`$ and where $`\omega _i`$, $`G_i`$ and $`\gamma _i`$ are respectively the frequency, the amplitude gain and the relaxation rate of (or corresponding to) the $`i^{th}`$ line. $`G_i=g_iL/2`$, where $`g_i`$ is the intensity gain coefficient on resonance (negative for an absorption line) and L is the medium thickness. Eq.1 is obtained by assuming that the pulse bandwidth and all $`\delta _i`$ and $`\gamma _i`$ are small with respect to $`\omega _0`$ and that all $`g_i`$ are small compared to the wavenumber $`\omega _0/c`$ (slowly varing amplitude and phase approximation). Note that the poles (singularities) of $`\mathrm{\Gamma }(p)`$ and then of the transfer function $`H(p)`$ with $`p=iu`$ are located in the left part of the complex plane. This ensures that the impulse response $`h(t^{})=_{\mathrm{}}^+\mathrm{}H\left(u\right)\mathrm{exp}(iut^{})𝑑u/2\pi `$ of the medium is null for $`t^{}<0`$ and, $`t^{}`$ indicating here the retarded time, that superluminal propagation of information is forbidden . A general study of the systems described by Eq. 1 will be presented in a forthcoming paper. The analysis is here restricted to the cases where the anomalous dispersion originates either from a single absorption line as in the experiments of Chu and Wong  and of Ségard and Macke  or from a doublet of two identical amplifying lines as in the experiments of Dogariu et al. . The detunings $`\delta _i`$ are chosen such that the real and imaginary parts of the complex gain are respectively even and odd functions of $`u=(\omega \omega _0)`$. This warrantees that the medium transmittance and the group velocity will be both extremum for $`\omega =\omega _0`$ and is achieved for $`\delta _1=0`$ in the single-line case $`(n=1)`$ and for $`\delta _1=\delta _2`$ in the gain-doublet case $`(n=2)`$. The complex gains, respectively $`\mathrm{\Gamma }_1`$ and $`\mathrm{\Gamma }_2`$, take then the simple forms given below.

$$\mathrm{\Gamma }_1(u)=\frac{Z}{1+iu/\gamma }$$
(2)
where Z is the optical thickness of the medium ($`Z=\alpha L/2=G_1>0`$, $`\alpha `$ being the intensity absorption coefficient on resonance).

$$\mathrm{\Gamma }_2(u)=\frac{G}{1+iu/\gamma i\mathrm{\Delta }}+\frac{G}{1+iu/\gamma +i\mathrm{\Delta }}$$
(3)
where $`G_1=G_2=G>0`$ and $`\mathrm{\Delta }=\delta _1/\gamma =+\delta _2/\gamma >0`$. If the pulse spectrum is very narrow with rapidly decreasing wings, the complex gain may be approximated by its first order expansion in ($`u/\gamma `$). The transfer functions $`H_1(u)`$ and $`H_2(u)`$ can then be written under the general form $`H_n(u)=H_n(0)\mathrm{exp}\left(iua_n\right)`$ with

$$a_1=Z/\gamma >0$$
(4)
$$H_1(0)=\mathrm{exp}\left(Z\right)=\mathrm{exp}\left(\gamma a_1\right)<1$$
(5)
$$a_2=\frac{2G}{\gamma }\frac{\mathrm{\Delta }^21}{\left(\mathrm{\Delta }^2+1\right)^2}$$
(6)
$$H_2(0)=\mathrm{exp}\left(\frac{2G}{1+\mathrm{\Delta }^2}\right)=\mathrm{exp}\left(\gamma a_2\frac{\mathrm{\Delta }^2+1}{\mathrm{\Delta }^21}\right)>1$$
(7)
$`H_n(0)`$ and $`a_n`$ being real  for $`n=1`$ or 2, the effect of the medium on the complex envelope of the pulse is to change its amplitude by the factor $`H_n(0)`$ and to shift it in time by $`a_n`$. The time-shift is easily identified with the advance of the pulse having propagated in the medium at the group velocity on the same pulse having covered the same distance in vacuum. $`a_2`$ is positive (true advance) only if $`\mathrm{\Delta }>1`$ and attains its maximum value $`G/4\gamma `$ for $`\mathrm{\Delta }=\sqrt{3}`$. As indicated before, the amplitude transmittance of the medium $`\left|H_n(u)\right|`$ is minimum for $`u=0`$. It is an absolute minimum for $`\left|H_1(u)\right|`$ and a relative minimum between two maximums for $`\left|H_2(u)\right|`$ when $`a_2>0`$ (see Fig.5 of Ref.). The essential point is that the larger are the aimed advances the more the transmittances depart from unity, downwards in the single-line case and upwards in the gain-doublet case (see Eq.5 and Eq.7). It is thus impossible to obtain advances without change of the pulse amplitude, unless one associates amplification and absorption. This has been simply achieved in the experiments  by compensating the absorption (resp. the amplification) by a suitable broadband, i.e. non-dispersive, amplification (resp. absorption). The device achieving the required amplification (resp. absorption) should be considered as an integral part of the systems under investigation (denoted $`S_1`$ and $`S_2`$ in the following). Absorption and amplification appear then to be tightly coupled in both kinds of experiments which, from this point of view, only differ by the implementation of the dispersion, associated either to the absorption stage  or to the amplification stage .

The pulse advances should naturally be referred to the pulse duration $`\tau _p`$ (hereafter the half-width at $`1/e`$ of the amplitude profile) and the relative merits of the systems $`S_1`$ and $`S_2`$ are suitably evaluated by comparing the pulse distortion they generate for the same value of the relative advance $`A=a/\tau _p`$, where $`a`$ indicates $`a_1`$ or $`a_2`$. This distortion can be derived from the exact form of the transfer functions of the above-defined global systems $`S_1`$ and $`S_2`$. The transfer function $`H_1^{}`$ of $`S_1`$ can be expressed in terms of the dimensionless quantities $`A`$, $`Z`$ and $`\mathrm{\Omega }=(\omega \omega _0)\tau _p`$. One gets:

$$H_1^{}(\mathrm{\Omega })=\mathrm{exp}\left(\frac{i\mathrm{\Omega }A}{1+i\mathrm{\Omega }A/Z}\right)$$
(8)
with $`A=Z/\gamma \tau _p`$. The equivalent expression of the transfer function $`H_2^{}(\mathrm{\Omega })`$ of $`S_2`$ is somewhat complicated in the general case but only its particular form for $`\mathrm{\Delta }=\sqrt{3}`$ (leading to the maximum advance) is needed for the following discussion. It reads :

$$H_2^{}(\mathrm{\Omega })=\mathrm{exp}\left(i\mathrm{\Omega }A\frac{12i\mathrm{\Omega }A/G}{1+2i\mathrm{\Omega }A/G4\mathrm{\Omega }^2A^2/G^2}\right)$$
(9)
where $`A=G/4\gamma \tau _p`$. Note that $`H_1^{}(\mathrm{\Omega })`$ and $`H_2^{}(\mathrm{\Omega })`$ both tend towards a constant when $`\mathrm{\Omega }\mathrm{}`$ . The corresponding impulse response $`h_1^{}(\theta )`$ and $`h_2^{}(\theta )`$ with $`\theta =t^{}/\tau _p`$ are then proportional to the Dirac function $`\delta (\theta )`$ and this means that the propagation of temporally localised features (involving high frequency components) is luminal. Advances are obtained in the opposite limit $`\mathrm{\Omega }0`$ and the distortion of the pulse envelope, if it is not too large, mainly originates from the second order term in the expansion of the complex gain in powers of $`\mathrm{\Omega }`$. The transfer functions $`H_1^{}(\mathrm{\Omega })`$ and $`H_2^{}(\mathrm{\Omega })`$ can then be written under the common form.

$$H_n^{}\left(\mathrm{\Omega }\right)\left(1+\epsilon _n\mathrm{\Omega }^2/2\right)\mathrm{exp}\left(i\mathrm{\Omega }A\right)$$
(10)
with $`\epsilon _1=2A^2/Z`$ and $`\epsilon _2=8A^2/G`$. The transcription of Eq.10 in the time domain  leads to :

$$E(L,\theta )E(0,\theta +A)\frac{\epsilon }{2}\frac{d^2}{d\theta ^2}E(0,\theta +A)$$
(11)
where $`E(L,\theta )`$ and $`E(0,\theta )`$ are respectively the complex envelopes of the output and input pulses and where $`\epsilon `$ indicates $`\epsilon _1`$ or $`\epsilon _2`$. The last term of Eq.11 is obviously responsible for the pulse distortion which, for a given pulse shape, is fully characterised by the parameter $`\epsilon `$. Although superluminal propagation is not specific to gaussian pulses , these pulses are suitable for simple calculations . Putting $`E(0,\theta )=\mathrm{exp}(\theta ^2)`$ in Eq.11, it is easily shown that the alteration of the pulse simply consists of a magnification of the amplitude profile by the factor $`\beta =(1+\epsilon )`$ and its narrowing by the same factor, in agreement with the area theorem for the field envelope . The intensity profile is also narrowed by the factor $`\beta `$ but magnified by the factor $`\beta ^2`$. The narrowing is in particular responsible for the difference between the advances $`a_{}`$ and $`a_{}`$ on the fall and the rise of the pulse. Such a difference is particularly apparent on Fig.6 of Ref.. Dogariu et al. claim that ”the front edges and the trailing edges of the pulse are shifted forward by the same amount”. A simple inspection of the insets in their figure shows on the contrary that $`a_{}`$ and $`a_{}`$ are dramatically different, roughly in the proportion of 3 to 2. Quite generally, $`a_{}=a+\tau _a(1\frac{1}{\beta })`$ and $`a_{}=a\tau _a(1\frac{1}{\beta })`$, where $`\tau _a`$ indicates the half-width of the pulse at the amplitude or intensity used to determine $`a_{}`$ and $`a_{}`$. The difference ($`a_{}`$ \- $`a_{}`$) is suitably characterised by the ”contrast” $`\xi `$ :

$$\xi =\frac{a_{}a_{}}{a_{}+a_{}}\frac{a_{}a_{}}{2a}\frac{\epsilon \tau _a}{a}$$
(12)
The parameter $`\xi `$ has the advantage of referring the distortion to the relative advance.

Since the pulse advances observed with the gain-doublet arrangement  are one order of magnitude smaller than those attained with the single-line scheme , the direct comparison of the absolute distortions is meaningless. These distortions indeed increase as the square of the advances. It is obviously more relevant to examine the potentialities of each experiment for a same pulse advance and a same level of distortion ($`A`$ and $`\epsilon `$ given) or, more precisely, to determine in what conditions each system would be able to reproduce the results obtained with the other. This is easily achieved by remarking that, $`A`$ being fixed, the same level of distortion is attained in both arrangements when $`Z=G/4`$ (see the expressions of $`\epsilon `$).

In the experiment of Dogariu et al. , $`G`$, $`a`$ and the full width at half maximum of the intensity profile of the pulse are respectively 0.7, 63 ns and 2.4 $`\mu s`$. This leads to $`\tau _p=2.04\mu s`$ (half-width at $`1/e`$ of the corresponding amplitude profile, assumed to be gaussian), $`A=0.031`$ and $`\epsilon =0.011`$. The value $`\mathrm{\Delta }=\sqrt{3}`$, used to establish the relation $`\epsilon =8A^2/G`$, is consistent with the contrast $`\xi `$ deduced from Fig.6 of Ref. ($`\xi 0.2`$) and with the separation of the two maximums of gain shown in Fig.5. The same relative advance and distortion would be obtained in the single-line case with an optical thickness $`Z=G/4`$ and the intensity transmittance of the medium would be $`\mathrm{exp}(G/2)0.7`$. It is amazing to note that the transmittance of this ”absorbing” medium is better than that of the ”transparent” medium used by Dogariu et al. (only 0.4, due to the presence of reverse-pumped atoms).

On an other hand one may wonder whether it would be possible to observe the large advances attained in the single-line case  with a gain-doublet arrangement. For the sake of definiteness, the data of the Fig.2 of Ref. are considered. $`Z`$, $`a`$ and the half-width at half-maximum of the amplitude profile of the pulse are respectively 5.25, 2 $`\mu s`$ and 4 $`\mu s`$. This leads to $`\tau _p=4.8\mu s`$, $`A=0.42`$, $`\epsilon =0.067`$ and $`\xi =0.13`$. The extended system $`S_1`$ under consideration consists of the medium of amplitude transmittance $`e^Z`$ and an amplifier of amplification factor $`e^Z`$ ($``$46dB). Assuming again $`\mathrm{\Delta }=\sqrt{3}`$, the same relative advance and distortion would be obtained in the gain-doublet case with $`G=4Z=21`$. The maximum of $`Re(\mathrm{\Gamma }_2)`$ is $`G/(4\sqrt{3}6)1.08G`$ whereas its minimum (at $`\mathrm{\Omega }=0`$) is $`G/2`$. The maximum of the field amplification factor of the global system $`S_2`$ would then be $`e^{0.58G}2.10^5`$ $`(106dB)`$. Even if it would be feasible (?) a system having such an optical gain at some frequency would be unstable. It is obviously possible to reduce the optical gain by a broadband absorber overcompensating the gain at $`\mathrm{\Omega }=0`$ and to use a post-amplifier (as it is actually done in the experiments of Dogariu et al.). However the amplification factor of the required post-amplifier would be considerably larger than that of the amplifier used in the single-line arrangement and this could raise serious problem of signal to noise ratio.

In conclusion, the propagation of light pulses at a negative group velocity in a medium whose dispersion originates from a single absorption line is a phenomenon which has been well understood for a long time and now pertains to classical physics . The physics underlying the experiments where the dispersion results from a doublet of two amplifying lines is quite similar. Indeed both kinds of experiments involve tightly coupled amplification and absorption and, in principle, only differ by the stage where the dispersion is implemented. However, the single-line arrangement appears, in practice, to be more efficient that the gain-doublet scheme. A study of other arrangements is in progress. It appears possible in particular to cancel the second order distortion (prevailing in the experiments discussed above) by using a doublet of absorption lines. In all cases, obtaining significant advances with moderate distortion requires the association of very large amplification and absorption. Otherwise said, Mother Nature resists to any transgression of her laws, even when this trangression is only apparent as in the experiments of superluminal propagation.

The authors thank J. C. Garreau and A. Walters for a critical reading of the manuscript. The Laboratoire de Physique des Atomes, Lasers et Molécules is ”Unité Mixte de Recherche de l’Université de Lille 1 et du CNRS (UMR 8523)”. The Centre d’Etudes et de Recherches Lasers et Applications (CERLA) is supported by the Ministère chargé de la Recherche, the Région Nord-Pas de Calais and the Fonds Européen de Développement Economique des Régions.


text:
# Magnetic- field -induced structural changes in the electron doped manganites CaxSm1-xMnO3 (x = 0.8, 0.85)

## I INTRODUCTION

In spite of extensive investigations on the hole doped, Mn3+: t$`{}_{}{}^{3}{}_{2g}{}^{}`$e$`{}_{}{}^{1}{}_{g}{}^{}`$ rich manganites there are scarcely few reports on the electron doped, Mn4+:t$`{}_{}{}^{3}{}_{2g}{}^{}`$e$`{}_{}{}^{0}{}_{g}{}^{}`$ rich compounds. Recently electron-doped CaMnO3 compounds regained experimental2-9 and theoretical interests10 motivated by the following facts:.1. The compounds x $`>`$0.5 in the series RE$`{}_{}{}^{3+}{}_{1x}{}^{}`$Ca$`{}_{}{}^{2+}{}_{x}{}^{}`$MnO3 (RE = La, Nd, Pr, etc.,) are antiferromagnetic insulators and the antiferromagnetic state is insensitive to the external magnetic field of $`\mu _0`$H = 5-7 T normally employed in many laboratories. However, magnetoresistance of about 82 % was first reported by Mahendiran et al in La0.1Ca0.9MnO3 (Mn4+ = 85 %) around the Neel temperature (TN). 2. Investigations by Chiba et al on Bi1-xCaxMnO3 and by Maignan et al on RE1-xCaxMnO3 (RE = Nd, Sm Gd, etc.,) revealed that magnetoresistance exists over a wide range (0.96 $``$ x $``$ 0.8) and the maximum magnetoresistance was again obtained for Mn4+ $``$ 85 %. In contrast to the hole-doped (rich in Mn3+:t$`{}_{}{}^{3}{}_{2g}{}^{}`$e$`{}_{}{}^{1}{}_{g}{}^{}`$) compounds whose resistivity ($`\rho `$) becomes insensitive to a fixed external magnetic field as size of the rare earth ion decreases, a large magnetoresistance independent of the rare earth ion is observed in the electron doped manganites. 3. Magnetization of the electron doped compounds for 0.85 $`<`$ x $`<`$ 1 surprisingly increases below TN whose origin is attributed to the formation of ferromagnetic clusters and their growth with x in the G-type antiferromagnetic background although canted antiferromagnetic structure for certain x value cannot be completely ruled out. Interestingly $`\rho `$ also exhibits a maximum around TN in compounds (x = 0.97-0.88) which have higher magnetization . 4. Electron-doped manganites serve as a laboratory to study the dynamics of excess electrons (eg electrons of Mn3+:t$`{}_{}{}^{3}{}_{2g}{}^{}`$e$`{}_{}{}^{1}{}_{g}{}^{}`$) in an antiferromagnetic matrix with compositionally tunable Jahn-Teller interactions and model to verify electronic phase separation proposed theoretically. When intersite Jahn-Teller interactions becomes dominant the G-type simple two sublattice antiferromagnetic order in Sm1-xCaxMnO3 (x = 1) changes to the C-type antiferromagnet (ferromagnetic linear chains with inter chain antiferromagnetic coupling) for x = 0.87-0.8 without charge ordering and with charge ordering for 0.8 $`<`$x $`<`$0.6. The composition x = 0.5 is generally a CE-type antiferromagnet (zig-zag ferromagnetic chains with inter chain antiferromagnetic coupling) with charge and cooperative Jahn-Teller ordering occurring at T $`>`$TN. Most of the existing studies have attributed the large magnetoresistance in manganites to the magnetic field induced ferromagnetic alignment of the t$`{}_{}{}^{3}{}_{2g}{}^{}`$ core spins either from the antiferromagnetic or the paramagnetic state although few investigations suggest that magnetically tunable lattice distortion could play an important role. However, the sign of lattice deformations either in zero or non zero magnetic field is not predicted theoretically so far and the existing experimental results are mostly on the hole doped (x $`<`$0.5) or x = 0.5 compounds. The purpose of this paper is to investigate the nature of the lattice distortion in absence and in presence of a external magnetic field in the electron doped Sm1-xCaxMnO3.series (x = 0.85, 0.8) which undergo simultaneous magnetic (paramagnetic to a C-type antiferromagnetic) and structural transitions (orthorhombic to monoclinic) with lowering temperature.

## II EXPERMENT

We measured magnetization of polycrystalline samples of CaxSm1-xMnO3 (x = 0.85, 0.8) using a commercial vibrating sample magnetometer up to 12 T and zero field four probe resistivity was also measured in the temperature range 5K $`<`$T $`<`$300 K. The structural characterization of our samples was already reported . Linear thermal expansion ($`\mathrm{\Delta }`$L/L) in zero magnetic field was measured for 20 K $`<`$T $`<`$300 K using the strain gauge technique. The volume thermal expansion was calculated using $`\mathrm{\Delta }`$V/V = 3$`\mathrm{\Delta }`$L/L. Magnetostriction by the strain gauge method was measured in a pulsed magnetic field up to 14 T with the magnetic field parallel and perpendicular to the measuring direction. The volume magnetostriction of randomly oriented polycrystallites was calculated through $`\mathrm{\Delta }`$V/V = $`\lambda _{par}`$+2$`\lambda _{per}`$ where $`\lambda _{par}`$ and $`\lambda _{per}`$ are parallel and perpendicular magnetostrictions. The anisotropic magnetostriction was found to be negligible and not presented in this paper. Neutron powder diffraction spectra at T = 100 K in 0 T and 6 T on Ca0.85Sm0.15MnO3 with Sm154 isotope were carried out in the high resoultion spectrometer (D2B instruement ) at Institue Laue-Langvein (ILL),Grenoble using the wavelength of 1.594 Angstrom.

## III RESULTSÅ

Fig. 1(a) show temperature dependence of the inverse magnetic susceptibility (H/M.) for x = 0.85 and 0.8 while cooling from 300 K. The arrows mark the onset of C-type antiferromagnetic ordering (TNC = 112 K for x = 0.85 and 150 K for x = 0.8). The paramagnetic to a C-type antiferromagnetic transitions are accompanied by orthorhombic ($`\mathrm{𝑃𝑛𝑚𝑎}`$ space group) to monoclinic (P21/m) structural transitions. The magnetic transition in these compounds are hysteretic as shown already. Earlier neutron diffraction study on x = 0.85 showed that in addition to the C-type ordering in the monoclinic phase, another antiferromagnetic ordering of G-type also sets in orthorhombic phase around TG = 118 K and its phase fraction increases from 5% at 100 K to 9 % at 10 K. Due to its smaller phase fraction and closeness of TG to TC, its signature is not very clear in the magnetic measurements. The Curie-Weiss fit (dark lines) for T $`>`$TNC gives Curie-Weiss temperatures $`\theta _p`$ =119 K ( x = 0.85) and 135 K (x = 0.8). The experimentally determined effective moments Peff = 4.386$`\mu _B`$ (x = 0.85), 4.238$`\mu _B`$ (x = 0.8) are slightly higher than the theoretical values Peff = 4.162 $`\mu _B`$ for x = 0.85 and 4.215 $`\mu _B`$ for x = 0.8. The x = 0.8 composition is expected to undergo a paramagnetic to a C-type antiferromagnetic transition below TNC = 150 K without coexistence of phases at low temperature based on the measurements on similar compounds

Fig. 1(b) shows the zero field resistivity $`\rho `$(T) of x = 0.85 and x =0.8 while cooling from 300 K to 5 K and warming back to 300 K. We clearly see hysteresis in resistivity around TNC. The crystallographic transition accompanying magnetic transition are marked. At 300 K, $`\rho `$(x = 0.8) $`>`$ $`\rho `$(x = 0.85). In contrast to the insulating behavior of $`\rho `$(T) in the paramagnetic phase of hole-doped compounds, $`\rho `$(T) of these two electron-doped compounds decreases as the temperature decreases from 300 K and shows a broad minimum at Tmin = 155 K ( x = 0.85), 210 K (x = 0.8) as shown in the inset and then jumps at TNC ( $`<`$Tmin). In between TN and 5 K, $`\rho `$(T) increases by four orders of magnitude in x = 0.85 and eight orders of magnitude in x = 0.8. The resistivity minimum above TNC can be recaptured in non adiabatic polaronic picture when the thermal and polaron activation energies are equal. We were able to fit the data using the relation $`\rho `$(T) = $`\rho _0`$T1.5exp(Ea/kBT) with Ea = 0.017 eV and Ea = 0.023 eV. With increasing content of the the rare earth ion, Tmin shifts to much higher temperatures

Fig. 1(c) shows the volume thermal expansion ($`\mathrm{\Delta }`$V/V) with respect to V value at 300 K. As T decreases from 300 K, the lattice shrinks in the paramagnetic region and then shows a rapid increase at TNC. In the entire temperature range (300 K- 20 K), the over all change in $`\mathrm{\Delta }`$V/V is larger for x = 0.85 than x = 0.8. However, around TNC the volume of x = 0.8 increases by 0.35 % which is five times larger than in x = 0.85 ( $`\mathrm{\Delta }`$V/V $``$ 0.07 % around TNC). These differences are intimately tied to the degree of localization of charges (for example, resistivity of x = 0.8 at 5 K is 5 orders of magntidue higher than x = 0.8), the strength of antiferromagnetic exchange interactions and structural distortions. Here, it should be mentioned that the magnitude of $`\mathrm{\Delta }`$V/V in x = 0.85 is very senstive to the stoichiometry. All previous studies on manganites undergoing transition either from a paramagnetic insulator to a ferromagnetic metal or from a ferromagnetic metal to a charge-ordered antiferromagnetic insulator showed that volume contracts at the transition temperature  in contrast to the volume expansion behavior seen here.

Figs. 2(a)-(d) illustrate the influence of external magnetic fields on the spin and lattice degrees of freedom. The field dependence of the magnetization and the magnetostriction data were taken after zero field cooling to a predetermined temperature. At 12 K (T $`<`$$`<`$TNC) M(H) of x = 0.85 \[Fig. 2(a)\] shows a rapid increase at low fields ( $`\mu _0`$H $`<`$0.5 T), gradually increases up to 2.5 T and then shows a rapid, but a smooth increase until the maximum field of $`\mu _0`$H = 12 T. The trend of the high field data suggest that M(H) can increase even beyond $`\mu _0`$H = 12 T. Upon decreasing H, M(H) exhibits a huge hysteresis. The low field behavior is caused by the presence of ferromagnetic regions in antiferromagnetic phase as suggested previously. The rapid increase of M(H) above 2.5 T is due to the field induced transition from the C-type AF to ferromagnetic state. It should be noted that the maximum magnetic moment at 12 K even at a field as high as 12 T is 1.45 $`\mu _B`$ which is much less than 3.1 $`\mu _B`$ expected for a fully ferromagnetic alignment of Mn spins. This means only a part of the sample transforms into ferromagnetic state and the rest remaining in antiferromagnetic state. We will touch upon this aspect in the later part of the paper. As T increases the width of hysteresis decreases and finally at 175 K and 225 K, M(H) is linear in H as expected for a paramagnet. Fig. 2(b) shows M(H) of x = 0.8 very close but below TN. First we note that the ferromagnetic like low field behavior seen in x = 0.85 is absent in x = 0.8. Second, the metamagnetic transition is rather sharp and the width of the hysteresis loop is nearly same (= 1.5 T) for T = 140 K and 145 K. The magnetic moment even at a field as high as 12 T is $``$ 1.2 $`\mu _B`$ (see 145 K data) which is far below the value of 3.2 $`\mu _B`$ expected for a fully ferromagnetic alignment of Mn3+ and Mn4+ spins. The critical field HC for the metamagnetic transition, as determined from the inflection point of the rapidly increasing part of M(H) in the field-up mode increases rapidly from 8 T to 11 T as the temperature decreases by 5 K from 145 K.

The field-induced metamagnetic transition is also accompanied by a dramatic change in volumes. The volume magnetostriction ($`\omega `$) isotherms in Fig. 2(b) and 2(d), for x = 0.8 and x = 0.85 respectively, show that the lattice volume contracts upon transition from the antiferromagnetic to the metamagnetic state. The reverse transition is hysteretic. The maximum volume change at 13.7 T is -0.135 % at 25 K for x = 0.85 and decreases to -0.085 % at 100 K. As like the magnetization, the hysteresis in $`\omega `$ also decreases with increasing temperature. At 120 K, $`\omega `$ is positive and is 0.0185 %. The volume change is negligible for x = 0.8 at 12 K. An appreciable magnetostriction in x = 0.8 appears only in between 120 K and 150 K. The maximum value of magnetostriction ($`\mathrm{\Delta }`$V/V)max increases with H, reaches a maximum at 135 K and then decreases again. Fig. 3 is complementary to Figs. 2(c) and (d) and it compares the values of the volume magnetostriction at the maximum field $`\mu _0`$H = 13.7 T for x = 0.85 and 0.8.as a function of temperature. The ($`\mathrm{\Delta }`$V/V)max is zero far away from TNC and at very close but above TNC it has smaller positive value and, a rapid increase occurs just below TNC. The peak in ($`\mathrm{\Delta }`$V/V)max for x = 0.8 is due to the fact that the maximum available field is insufficient to induce a complete antiferromagnetic to ferromagnetic transition.

## IV Discussion

Now we turn attention to the origin of the volume contraction under a magnetic field. The paramagnetic to C-type AF transition in the electron doped compounds under investigation is accompanied by orthorhombic ($`Pnma`$) \- monoclinic (P21/m) structural transition. The C-type antiferromagnetism is coupled to polarization of the d$`_{z^2r^2}`$ orbitals of Mn3+ sites along the c-axis. The x = 0.85 composition exhibits multiple phase separation. It was found that about 9 % of the G-AF phase in $`\mathrm{𝑃𝑛𝑚𝑎}`$ structure also coexists with the C-phase (P21/m structure) at 10 K in zero field in x = 0.85. In addition, a third phase which is ferromagnetic also appears to be present in x = 0.85. But the volume fraction of the ferromagnetic phase is extremely sensitive to sample preparation. The ferromagnetic phase is in $`\mathrm{𝑃𝑛𝑚𝑎}`$ structure, if one extrapolates the trend seen in x = 0.9 compound. When H is increased from 0 T, the magnetic contribution due to domain wall displacement in ferromagnetic phase dominates at low fields. As H increases further above 5 T at 12 K, a metamagnetic transition takes place and a portion of the C- AF phase is converted into a ferromagnetic phase. Since, the magnetic moment does not saturate even at the highest field of 12 T, ferromagnetic phase and antiferromagnetic phase coexists in between 4 T and 12 T at 12 K. Because of the strong coupling between the C-type AF and d$`_{z^2r^2}`$ orbitals, the destruction of the C-type AF is accompanied by disordering of d$`_{z^2r^2}`$ which drives $`P2_1/m`$ to $`Pnma`$ structural transition. Since the P21/m phase higher volume than the $`Pnma`$ phase, the field induced monoclinic to orthorhommbic transition leads to a volume contraction as seen in the magnetostriction data (Fig. 2(c)). If this is to true, we can expect to see an increase in the $`Pnma`$ phase fraction above at high fields. This is what indeed found in the neutron diffraction study. While small angle neutron scattering study and elaborate powder neutron diffraction study in Ca0.85Sm0.15MnO3 will be published by some of us elsewhere, we show the result most relevant to this work. Fig. 4 shows the schematic diagram of the nuclear phases of x = 0.85 at 100 K in absence of a magnetic field and in presence of H = 6 T. The $`P2_1/m`$ phase (C-AF) which is 91 % at 0 T reduces to 44 % at 6 T and correspondingly the $`Pnma`$ phase (G-AF) increases from 9 % at 0 T to 56 % at 6 T. A large ferromagnetic component of = 1.7 $`\mu _B`$ is also found in the $`Pnma`$ phase. We believe that similar field induced structural transition also takes place in x = 0.8 compound.

## V SUMMARY

In summary, we have shown that the paramagnetic to the C-type antiferromagnetic transition in the electron doped manganites CaxSm1-xMnO3 (x = 0.80, 0.85) is accompanied by an abrupt volume expansion ($`\mathrm{\Delta }`$V/V = 0.07 % in x = 0.85, 0.35 % in x = 0.8) and orthorhombic (Pnma) to monoclinic (P21/m) structural transitions. The x = 0.85 compound is magnetically and structurally phase separated with two types of antiferromagnets ,G-(Pnma) and C- (P21/m) and a minority ferromagnetic phase (Pnma) coexisting together. Magnetization study shows that metamagnetic transiton (C-AF to ferromagnetic) field increases from 5 T in x = 0.85 to more than 12 T in x = 0.8 at 12 K. Isothermal magnetostriction measurements shows high volume to low volume transition under a magnetic field which has been suggested to structural transition ($`P2_1/m`$ to $`Pnma`$ ) under a field. The driving factor for this structural transition is the strong coupling between the C-type antiferromagnetic order and the d$`_{3z^2r^2}`$ orbital order. The field induced structural transition in x = 0.85 compound is supported by neutron diffraction study.

## VI Acknowledgments

R. M thanks MENRT (France) and Ministerio de Ciencia Y Cultura (Spain) for financial assistance and acknowledges discussions with Prof. T. V. Ramakrishnan and Dr.Venkatesh Pai on electron doped manganites

Figure captions

Temperature dependence of the inverse susceptibility (H/M) measured under $`\mu _0`$H = 0.01 T in CaxSm1-xMnO3 (x = 0.8, 0.85). G- and C-type antiferromagnetic phases coexist down to the lowest temperature in x = 0.15. PM -paramagnetic phase. (b). Temperature dependence of the zero field resistivity of x = 0.85 and x = 0.8 while cooling and warming. The inset shows the resistivity minimum in the paramagnetic state (c). Temperature dependence of the spontaneous volume thermal expansion of x = 0.8 and x = 0.85. The structural transitions are also marked.

Magnetization isotherms of (a) x = 0.85 and (b) x = 0.8. Volume magnetostriction isotherms of (c) x = 0.15 and (d) x = 0.8.

Temperature dependence of the volume magnetostriction ($`\mathrm{\Delta }`$V/V) of x = 0.85 and 0.8 at the the maximum field $`\mu _0`$H = 13.7 T.

A schematic diagram of the volume phase fractions of nuclear phases in 0 T and 6 T at 100 K in Ca0.85Sm0.15MnO3.


text:
# Ripple and kink dynamics

## I Introduction

The formation of ripples due to the wind blowing across a sand bed  is a complex phenomenon involving various mechanisms such as air turbulence, non-linear fluxes of sand, saltation, grain ejection threshold, creeping and avalanches.

Different models  for ripple formation have been proposed. Some of those models consider both hopping and rolling of grains, and they are able to reproduce travelling ripple structures. Simulations  have also considered various additional effects like the screening of crests, the grain reptation and the existence of a grain ejection threshold.

The Nishimori-Ouchi (NO) model  is able to reproduce a wide variety of different eolian structures: ripples, star dunes, barkhanic dunes, etc… The main advantage of such a numerical model is that all parameters can be easily tuned and the dynamics can be deeply investigated. In a recent work , we have shown that the NO model reproduces the complex labyrinthic patterns created in some experiments . However, the NO model leads to unrealistic features. Among others, a cube of sand can be stable within the NO model. It is possible to create aeolian structures with an infinite height. In fact, the existence of a critical angle is lacking in the NO model.

In the next section, we will propose a modification of the NO model in order to impose a more realistic constraint to granular surfaces. In section 3, we will study how the ripple formation depends on the various parameters of the model. In section 4, the dynamics of the new model will be studied and will be confronted to various situations. Finally, a summary of our findings will be given in section 5.

## II Models

In this section, we present two 2-dimensional models of granular landscape evolution.

### A Nishimori-Ouchi (NO)

In the Nishimori-Ouchi model , two modes of granular transport are considered: (i) saltation and (ii) reptation. The saltation process acts along the $`x`$ axis. It takes grains from a site $`(x\mathrm{},y)`$ and add these grains to a site $`(x,y)`$. The value of the saltation length $`\mathrm{}(x,y)`$ depends on the local slope of the landscape at $`(x,y)`$. In this model, the saltation grains are captured by the surface when they touch it. The granular flux $`Q_{salt}`$ due to the saltation process can be written as

$$Q_{salt}=A_x\mathrm{}^xN(x^{},y)dx^{},$$
(1)
where $`N(x,y)`$ is the amount of sand per time unit and surface unit at the position $`(x,y)`$. $`A`$ is a dimensionless constant parameter.

The NO model also considers a 2-dimensional diffusion process, i.e. the reptation. The amount of sand displaced at $`(x,y)`$ is supposed to be proportional to the local curve of the surface at that position. The flux $`Q_{rept}`$ due to the reptation reads

$$Q_{rept}=Dh,$$
(2)
with a kind of diffusion coefficient $`D`$. The mass conservation imposes

$$\frac{h}{t}=Q,$$
(3)
where $`Q=Q_{salt}+Q_{rept}`$. Therefore, the temporal evolution of the height $`h`$ of sand at the position $`(x,y)`$ reads

$`{\displaystyle \frac{h(x,y,t)}{t}}`$ $`=`$ $`A\left[N(x\mathrm{},y)\left(1{\displaystyle \frac{\mathrm{}(x,y)}{x}}\right)N(x,y)\right]`$ (4)
$`+`$ $`D\mathrm{\Delta }h.`$ (5)
As in the NO model , we have assumed that the local slope (along the $`x`$ direction) mainly controls the sand flux $`Q_{salt}`$. Experimentally , one observes that the wind is stronger on the crests. As a consequence, the amount of displaced sand is larger around the crests. This effect can be included in the NO model by assuming

$$\frac{Q_{salt}}{x}=\delta \left(1+\mathrm{tanh}\frac{h}{x}\right)\left(1+\epsilon \mathrm{tanh}\frac{h}{x}\right)$$
(6)
where the parameters $`\delta `$ and $`\epsilon `$ give respectively the scale factor of the saltation flux and the non-zero asymptotic quantity of sand displaced when $`h/x>0`$. The saltation length $`\mathrm{}`$ is represented by the factor $`(\mathrm{tanh}(\frac{h}{x})+1)`$. This assumes that $`\mathrm{}`$ is maximum on the crest and that small saltation jumps take place on the downstream part of the ripple.

We have numerically solved the NO model on two-dimensionnal square lattices starting from an initially plane landscape. At each time step, a randomly chosen site is submitted to both saltation and reptation processes (Eqs.(4) and (5)). Figure 1 shows the maximum height $`h_{max}`$ reached by the profile as a function of time $`t`$. Time is expressed in numerical steps (iterations).

One observes that : (i) the growth of the maximum height $`h_{max}`$ is linear and (ii) there is no saturation. This means that ripples become infinitely high! This unrealistic behavior comes from the right hand side of Eq.(4). Indeed, when the first term becomes larger, the sand deposit becomes more important than the relaxation. As time goes on, a net growth of the profile is thus recorded. This situation will remain unchanged since the ratio between deposit and relaxation is fixed once by the values of $`\delta `$, $`\epsilon `$ and $`D`$. Consequently, $`h_{max}`$ grows ad infinitum. One should note that this pathology implies the possibility of making cubes of sand since nothing prohibits vertical walls. In order to get a more realistic situation, an additional term should be included in the NO model.

### B Saltation-Creep-Avalanche (SCA)

Granular materials are characterized by the angle of repose $`\theta _r`$ . If the slope of a granular pile exceeds $`\mathrm{tan}(\theta _r)`$, an avalanche is created and stabilizes the surface. The angle of repose depends on the grain characteristics: size distribution, shape, rugosity, and density. Typically, this angle $`\theta _r`$ is about $`37^{}`$ for sand . Since it is an intrinsic property of the granular material, the relevant parameter $`\theta _r`$ should be considered in numerical models.

Let us consider a square lattice with discrete spatial variables $`x`$ and $`y`$. The stability condition with respect to the angle of repose $`\theta _r`$ reads

$`\left|h_xh_{x+1}\right|`$ $`<`$ $`\mathrm{tan}(\theta _r)`$ (7)
$`\left|h_yh_{y+1}\right|`$ $`<`$ $`\mathrm{tan}(\theta _r)`$ (8)
where the left hand side is the discrete counterpart of the spatial derivative of the height of sand $`h`$ at the position $`(x,y)`$. If Eq.(7) is not verified for a specific direction ($`x`$ or $`y`$), an avalanche occurs as illustrated in Figure 2. In this case, the excess of sand $`E=\mathrm{tan}(\theta )\mathrm{tan}(\theta _r)`$ (with $`\mathrm{tan}(\theta )=\frac{h}{i}`$, with $`i=x`$ or $`i=y`$ depdending on which condition (7) is not verified) is supposed to be equitably distributed between $`x`$ and $`x+1`$ if the avalnche occure in that direction. The same applies for the $`y`$ direction. Taking those considerations into account, Eq.(4) becomes

$`{\displaystyle \frac{h(x,y,t)}{t}}`$ $`=`$ $`A\left[N(x\mathrm{},y)\left(1{\displaystyle \frac{\mathrm{}(x,y)}{x}}\right)N(x,y)\right]`$ (9)
$`+`$ $`\mathrm{\Theta }(E){\displaystyle \frac{E}{2}}+D\mathrm{\Delta }h,`$ (10)
where $`\mathrm{\Theta }`$ is the Heavyside step function and

$$E=\left|h\right|\mathrm{tan}(\theta _r).$$
(11)
The new model is called the Saltation-Creep-Avalanche (SCA) model. It will be investigated in the present paper and numerical results will be compared with respect to NO landscapes. One should note that we have numerically solved Eq.(9) using the same flux law (6) as in the original NO model.

## III Ripple formation

In this section, we investigate the influence of the four parameters $`\delta `$, $`\epsilon `$, $`D`$ and $`\theta _r`$ on the formation of the ripples in the SCA model. All the simulations presented herebelow are made on $`150\times 150`$ square lattices. The evolution of the landscape is typically stopped after $`10^7`$ iterations. The default parameter values are $`\delta =12.5`$, $`\epsilon =0.3`$, $`D=0.4`$ and $`\theta _r=37^{}`$.

### A Flux parameter $`\delta `$

The saltation process obeys Eq.(6) in which the parameter $`\delta `$ controls the flux $`Q_{salt}`$. A small arbitrary value of $`\delta `$ implies that small amounts of sand are displaced along small saltation lengths, while larger values of $`\delta `$ lead to a more important transport of sand over long distances. Experimentally , one observes that the ripple wavelength (the distance between two consecutive crests) grows with the saltation length $`\mathrm{}`$.

We have performed simulations varying $`\delta `$ from 1 to 100. For very small values of the parameter ($`\delta <7`$), no ripple appears and the surface remains irregular. This threshold is not encountered in the NO model and is certainly due to the angle of repose. For small values of the flux parameter, not enough sand is displaced and the surface is continuously smoothed by avalanches.

Above this threshold $`\delta 7`$, a set of several ripples appears. The density of ripples depends on $`\delta `$. The larger $`\delta `$ is, the smaller is the density of ripples. For example, after $`\mathrm{5\; 10}^6`$ iterations, the density of ripples is 0.04 for $`\delta =10`$, while there is only a single ripple (density of 0.006) if $`\delta =85`$. The SCA model is thus in good agreement with observations: the wavelength of the ripple pattern grows with the saltation length $`\mathrm{}`$. In the case of the NO model, the density of ripples grows non-linearly with $`\delta `$ in opposition with experimental observations.

### B Asymmetry parameter $`\epsilon `$

In the SCA model, we have assumed a non-zero value for the flux of sand $`Q_{salt}`$ displaced on the stoss slopes (which are upstream) of the ripples (see Eq.(6)). This hypothesis is supported by numerical results . If the parameter $`\epsilon `$ is non zero, the saltation flux becomes asymmetric (see Figure 3). Sand is always taken from the stoss slope, while $`Q_{salt}`$ tends to zero on the lee slope. This comes from the fact that sand on the lee slope is confined in wind vortices.

Practically, we have considered values of $`\epsilon `$ ranging from 0 to 2. Our observations are: (i) no ripple appears if $`\epsilon =0`$. (ii) for small values of $`\epsilon `$ (typically $`0<\epsilon <0.2`$), ondulations appear in the landscape. (iii) As $`\epsilon `$ becomes larger, the number of ripples present in the system grows (from $`5`$ at $`\epsilon =0.5`$ to $`11`$ for $`\epsilon =1.8`$). Moreover, ripples are more asymmetric (windward slopes smaller than downstream slopes) for large values of $`\epsilon `$. We will study this asymmetry in section 4.

In the case of the NO model we observe that: (i) if $`\epsilon =0`$ very small ripples appear. (ii) when the parameter reaches a threshold $`\epsilon 0.2`$ larger ripples appear. Note that the wavelength of the ripples does not depend on $`\epsilon `$ above that threshold. The fact that ripples appear for $`\epsilon =0`$ in the NO model and do not appear within the SCA model is due to the existence of an angle of repose. Indeed, avalanches tend to smooth the landscape.

In summary, the flux $`Q_{salt}`$ should be asymmetric in order to create ripples. For positive slopes, a minimum value of this flux is required.

### C Reptation coefficient $`D`$

The parameter $`D`$ plays the role of a diffusion coefficient for smoothing the irregularities along the surface. We have considered values of $`D`$ ranging from 0 to 1. Once again, no ripple appears for very small values of that parameter. Ripple appearance is allowed in the interval $`0.1D0.5`$. If $`D<0.1`$ the surface remains irregular. There is nearly no interaction between the cells because of the small diffusion coefficient. Note that the same behavior is observed in the NO model. As $`D`$ becomes larger, the ripple wavelength increases. Finally, for $`D>0.5`$ the diffusion coefficent becomes too large and the surface remains smooth and flat. For the NO model, no ripple appears when $`D>1.8`$, a larger value than in the case of the SCA model.

### D Angle of repose $`\theta _r`$

Parameters $`D`$ and $`\theta _r`$ are intrinsic parameters of the granular material, while $`\delta `$ and $`\epsilon `$ should be related to the wind. At each iteration, the reptation acts and moves grains. On the other hand, an avalanche occurs if and only if the local slope of the surface exceeds the angle of repose. The role played by both $`D`$ and $`\theta _r`$ parameters is thus different: $`D`$ is a diffusion coefficient, which controls the flow of sand between neighboring cells, while the angle of repose $`\theta _r`$ governs the local slope of the granular surface.

We considered typical values of $`\theta _r`$ between $`20^{}`$ and $`40^{}`$. For ripples of the same wavelength, we have noted that small angles of repose imply small ripple heights. The angle of repose is thus responsible of the value of the ratio $`h_{max}/\lambda `$, where $`\lambda `$ is the ripple wavelength. Indeed, a slope larger than $`\mathrm{tan}(\theta _r)`$ is reduced to a value $`\mathrm{tan}(\theta _r)`$ by avalanches. We have also noted the appearance of ripples for all tested values of $`\theta _r`$.

## IV Ripple dynamics

In this section, we investigate the dynamics of the SCA model. Three different aspects will be considered: the ripple height, the ripple shape and the formation of kinks. Again, the default parameters values are $`\delta =12.5`$, $`\epsilon =0.3`$, $`D=0.4`$ and $`\theta _r=37^{}`$.

### A Ripple amplitude $`h_{max}`$

Figure 4 presents the temporal evolution of the maximum ripple height $`h_{max}`$ in the case of the SCA model. One should note the saturation of $`h_{max}`$ for long times. This figure should be compared with Figure 1.

In Figure 4, many gaps can be observed in the early stages of evolution. Those gaps come from the absorption of small ripples by the largest ones. Since a small ripple travels faster than a large one , the large ripple tends to absorb the small. Figure 5 presents the evolution of a part of the lattice for different stages of the simulation. For each picture, a transverse view of the landscape is shown. One should note that the merge occurs as follows: first, the small ripple climbs on the larger one. The arrival of the small ripple on the crest causes an avalanche. A part of the small ripple falls in the avalanche, while the remainder feeds the larger one. It results in a fast growth of the largest ripple even it moves slowly.

Asymptotically, only one ripple occupies the whole lattice, and the time needed for a global merge becomes larger as $`\delta `$ decreases. If $`\delta `$ is large, the initial density of ripples is small. In this case, the global merge is obtained after a small number of collapses. In opposition, a large number of merges is necessary for small values of $`\delta `$. If one assumes that ripple collapses is a size independent process, one can understand that the global merge is faster when $`\delta 1`$.

The main characteristics of $`h_{max}(t)`$ are (i) gaps in the early stages of ripple formation, and (ii) a saturation for long times. Looking for details in Figure 4, one could see that gaps are allways followed by the same kind of growth. Indeed, the maximum ripple height evolves according to an exponential growth law

$$h_{max}=ab\mathrm{exp}\left(\frac{t}{c}\right),$$
(12)
where $`a`$, $`b`$ and $`c`$ are fitting parameters. This law is shown in Figure 4. One should see that the fit has been performed after the primary gaps, e.g. for $`t>10^7`$ iterations.

In summary, we have seen that, contrary to the NO model, the SCA model naturally leads to a non-linear evolution of $`h_{max}`$. Note that this kind of behavior has been experimentally observed in . Moreover, the SCA model predicts a saturation of $`h_{max}`$ after a finite time, as expected and observed. The saturation value depends essentially on $`\theta _r`$. The larger is $`\theta _r`$, the higher are the ripples.

### B Ripple aspect ratio $`\sigma `$

Under a non-oscillating wind, a ripple has generally an asymmetric shape . The stoss slope is indeed smaller than the lee slope. In Figure 6, the profile of the ripples is shown for both NO and SCA models. Ripples are more symmetric in the NO model than in the SCA model.

In order to measure the aspect ratio $`\sigma `$ of a ripple, we have measured the ratio of the horizontal projections of both sides of the ripples. Let us call $`x_s`$ the projection of the stoss slope on the horizontal $`x`$ axis, and $`x_l`$ the projection of the lee slope. The apect ratio of a ripple is defined as

$$\sigma =\frac{x_s}{x_l}.$$
(13)
The measure of $`\sigma `$ is averaged over all the ripples of the landscape. If $`\sigma =1`$ the ripples are symmetric, while $`\sigma 1`$ implies an asymmetry.

In Figure 7, the temporal evolution of $`\sigma `$ for both NO and SCA models are reported. Typical values of $`\sigma `$ range between 1 and 5 in the SCA model. In the NO model, $`\sigma `$ remains close to 1.

In the case of the SCA model, one should note that $`\sigma `$ grows linearly with time, and then remains close to a saturation value. The appearence of a saturation seems coherent since only one ripple occupies the whole lattice after a finite time. The angle of repose limits the height of that ripple and its morphology.

In order to compare the four parameter dependencies on $`\sigma `$, we have considered a reference situation which corresponds to the default parameters. Varying the value of a parameter while keeping constant the others allows us to define the influence of that parameter on the temporal evolution of the aspect ratio. Herebelow, we describe the results obtained for each of the four parameters $`\delta `$, $`\epsilon `$, $`D`$ and $`\theta _r`$. One should note that in all cases, the temporal evolution of $`\sigma `$ begins with a quasi-linear law, followed by a saturation.

The aspect ratio increases with the parameter $`\delta `$. Since the ripple wavelength directly depends on $`\delta `$, that result means that small ripples are less asymmetric than large ones. This result is in good agreement with observations .

Figure 8 presents the temporal evolution of the aspect ratio $`\sigma `$ for different values of $`\epsilon `$. One can see that small ripples (for small $`\epsilon `$ values) are less asymmetric. Indeed, $`\sigma `$ is larger for $`\epsilon =1`$ than for $`\epsilon =0.3`$. We have seen in Section III.B. that the ripple wavelength becomes larger as $`\epsilon `$ increases. One should also note that $`\sigma `$ saturates more rapidly when $`\epsilon `$ is small. This is consistent with the fact that the time needed for a global merge is shorter in the case of large ripples.

As observed for $`\delta `$ and $`\epsilon `$, the aspect ratio follows any variation of $`D`$. This results is in agreement with those observed previously in this section. Indeed, we have seen in Section III.D. that the ripple wavelength increases as $`D`$ becomes larger.

We have taken realistic values of $`\theta _r`$ between 30 and 40. The aspect ratio $`\sigma `$ is found to be independant of the value of $`\theta _r`$. This result is outside the scope of this paper and will be studied in the future.

### C Kink dynamics

Although the wind blows in a single direction, the resulting ripples are not strictly perpendicular to the wind direction. There are defects. Two different classes of defects can be found: kinks which are fusion points of two crests, and antikinks which are endings of crests. In Ref., we have studied in the NO model how defects modify a landscape morphology when a brutal change occurs in the wind direction. We have also shown in Ref. that under a constant wind direction, the density of defects decreases as time goes on. In the present section, we will focus on the processes leading to this decrease in the SCA model.

After extensive simulations, we conclude that some kinks can propagate during very long times, while others disappear quite rapidly.

The disappearance of a defect mainly occurs when a ripple is splitted into two inequitably parts (see an example in Figure 9). The small branch moves faster than the larger one and climbs on it following the merging dynamics described in section IV.A. Reaching the crest, the small branch creates an avalanche. The sand rolling on the lee slope may be captured. If the amount of sand escaped from this avalanche is small, the defect disappears and the small branch vanishes. After this process, the number of defects is reduced. If all defects show this kind of behavior the defect density will rapidly tend to zero. However, this is not the case .

The propagation of a kink takes place when a sufficient amount of sand escapes from the avalanche. This is the case when the branches are quite long. In the emphasized part of Figure 10, one can see the ending of a small ripple. The extremity of the ripple moves faster than the main part. The merge (second image) is accompanied by an avalanche. As seen in the previous paragraph, sand is expelled out of the avalanche. But here, the amount of sand is sufficient to create a new ripple. The merging/propagation process is thus repeated on the next ripple.

Let us consider a branch of length $`\mathrm{}_b`$. The merge of this branch with a larger ripple causes the decrease of the branch length since a part of the branch has been owned by the ripple. When a second meeting occurs, $`\mathrm{}_b`$ is once again reduced. As a consequence, the initial length of the branch is a relevant parameter in order to predict the life-time of a defect. For example, a kink of initial length $`\mathrm{}_b=65`$ can typically propagate during $`9.5\times 10^5`$ iterations, while a kink of initial length $`\mathrm{}_b=23`$ has a life expectancy of $`2.5\times 10^5`$ iterations. One should note that those life-times mainly depend on the diffusion coefficient $`D`$ and the avalanche process.

In Ref., we have found a non zero asymptotic value for the defect density. The existence of propagating kinks gives a picture of this behavior. The relevant ingredient for kink disappearance being the length of the branch.

## V Summary

We have introduced new ingredients in the Nishimori-Ouchi (NO) model: the existence of an angle of repose $`\theta _r`$ and subsequent avalanches when the local slope $`\theta `$ is larger than $`\theta _r`$. The new model reproduces realistic features of aeolian ripples such as a non-linear evolution of the ripple amplitude $`h_{max}`$. The origin of this behavior has been explained by the merge of ripples traveling at different speeds. Increasing the saltation length, we have observed a grows of the ripple wavelength, in agreement with observations. In the case of a constant wind orientation, natural ripples are asymmetric. This feature has also been reproduced by the new model.

Studying the kink dynamics, we have shown the coexistence of two kinds of kink evolution: propagation and disappearance. The defect initial length has been proposed as a relevant parameter in order to predict the life-time of that defect. From this result, the existence of a non-zero asymptotic value of the kink density has been explained.

## Acknowledgements

HC is financially supported by the FRIA, Belgium. This work is also supported by the Belgian Royal Academy of Sciences through the Ochs-Lefebvre prize.


text:
# H-atom laser without inversion (LWI) in space: a possible explanation for the intense, narrow-band, H(𝛼) emission frequently observed in reddened early-type stars

## 1 Introduction

The introduction of an entirely new concept to explain a class of observed phenomena in any field of science would seem to be a redundant activity, if the phenomena can reasonably be accounted for with use of existing theories and models. However, in the cases of certain astronomical observations of H($`\alpha `$) emission, standard explanations appear to be inadequate. This letter focusses specifically on recorded observations of intense H($`\alpha `$) emission in reddened early-type stars. It will be shown below that enough spectral information exists for such stars to suggest strongly that a new paradigm is here needed. One that appears to be quite suitable for explaining the H($`\alpha `$) emission data was recently developed in the field of quantum electronics and is termed ‘laser without inversion (LWI)’. The LWI concept is itself inseparably tied to another recently developed quantum electronics concept, that of ‘electromagnetically induced transparency (EIT)’. In the present letter a novel astrophysical model based upon LWI/EIT is introduced that appears to be fully capable of explaining the most intense and spectrally narrowest H($`\alpha `$) emissions seen in reddened early-type stars.

## 2 H($`\alpha `$) emissions in reddened early-type stars

In Rawlings et al. (rawlings (2000)) new optical spectroscopy for 45% of an older catalog (Stephenson stephenson (1992)) of $``$440 reddened stars was performed in an attempt to isolate reddened stars which are also early-type. The spectra between 6100 Å and 6900 Å of all the stars studied are shown in Rawlings et al. (rawlings (2000)). Only fifteen of the stars surveyed could be classified as early-type stars. With regard to H($`\alpha `$), the spectra of these early-type stars show tremendous variations. Some (Fig. 1a) show H($`\alpha `$) only in absorption. Others (Figs. 1b, 1c, 1d) show H($`\alpha `$) strongly in emission, with an intensity completely disproportionate to all other absorption features present. Yet the spectral types of these stars are all apparently roughly comparable. In the spectra of all the cooler stars surveyed by Rawlings et al. (rawlings (2000)), H($`\alpha `$), if present at all, appears only in absorption.

Much spectral data exists for the star, HD 44179, that powers the fascinating Red Rectangle nebula. We here consider an apertured line-of-sight that includes just the star, not the nebula. In such a line-of-sight, one sees (Cohen et al. cohen (1975)) that all Balmer lines, with the notable exception of H($`\alpha `$), appear as broad absorptions against the star’s blackbody continuum. No emissions are present in the blue-green spectral region. However, H($`\alpha `$) appears as a strong, narrow, emission line centrally placed in a broad absorption. A recent STIS scan showing H($`\alpha `$) emission in HD 44179 is shown in Fig. 2.

In view of the enormous variations in H($`\alpha `$) spectral width and intensity observed in lines-of-sight to reddened stars of roughly the same spectral type, a non-stellar origin for this emission is strongly suggested. Hence - at least in the most singular cases - this emission must originate from H atoms located outside the photosphere of the illuminating star. If the H($`\alpha `$) emissions resulted from electron impact excitation occurring in compact H II regions about the stars, one would expect also to detect emissions at the wavelengths of H($`\beta `$), H($`\gamma `$), H($`\delta `$), etc.. At least in the case of HD 44179, these are not observed. H($`\alpha `$) emission could reasonably be produced via linear photoexcitation of H atoms located in neutral regions bordering H II regions. However, as discussed below, this would generally result in broadened H($`\alpha `$) emission-line profiles, and cannot account for the extreme $`\delta `$-function-like profiles observed in some lines-of-sight. In essence, then, the nonlinear photoexcitation model introduced here will attempt to explain why some reddened early-type stars show H($`\alpha `$) emissions that are comparatively broad, particularly at the base, while others (e.g. Fig. 1b) display ones that are much sharper, more intense, and more singular-looking (i.e. unaccompanied by a significant pedestal).

## 3 Electromagnetically induced transparency (EIT)

To understand the concept of LWI, one must first understand that of EIT, since the former is built upon the latter. A good introductory review describing some of the recent exciting developments in EIT is Harris (harris (1997)). The particular LWI/EIT model being considered in the present letter involves the so-called three-level $`\mathrm{\Lambda }`$ scheme shown in Fig. 3. Transitions 1$``$3 and 2$``$3 are allowed; the total radiative decay rate of quantum level $`|3`$ is $`\mathrm{\Gamma }_3`$. Transition 1$``$2 is assumed to be basically forbidden. For H atoms, $`|2`$ decays radiatively to $`|1`$ via spontaneous two-photon emission at a rate $``$ 8 sec-1. This degree of metastability qualifies the H-atom 2s level to be level $`|2`$ in a $`\mathrm{\Lambda }`$-type EIT scheme.

When a nearly monochromatic laser beam (the EIT ‘coupling beam’), tuned to the center frequency $`\omega _{23}`$ of the 2$``$3 transition, is applied to a gas of three-level atoms, a sharp dip in absorption in the vicinity of the 1$``$3 transition occurs (Fig. 4). This cancellation in the imaginary part of the linear susceptibility (absorption is proportional to Im $`\chi ^{(1)}`$) can be shown to arise from quantum interference. For the ideal case $`\mathrm{\Gamma }_2`$=0, there is perfect transparency at the minimum. The width of the transparency hole varies as $`\mathrm{\Omega }_{23}`$, the so-called Rabi frequency, which is itself proportional to the square root of the laser power ($`\mathrm{}\mathrm{\Omega }`$= $`\mu E`$, where $`\mu `$ is the dipole matrix element and $`E`$ is the optical field).

If another nearly monochromatic laser beam (the EIT ‘probe beam’), tuned to the center frequency $`\omega _{13}`$ of the 1$``$3 transition, is applied to the same gas of atoms, the system will quickly adjust itself so that there is also no absorption about the line center of the 2$``$3 transition. This occurs independently of the ratio of Rabi frequencies $`\mathrm{\Omega }_{13}`$/$`\mathrm{\Omega }_{23}`$. The two laser beams rapidly drive all atoms of the system into a stable ‘coherently trapped population state’. In this state, the wavefunction of all the atoms in the gas becomes an antisymmetric linear combination of the unperturbed wavefunctions of levels $`|1`$ and $`|2`$. In this state, no atoms are present in level $`|3`$. One of the earliest experiments in which coherent trapping of atomic populations was realized is described in Gray et al. (gray (1978)). Atoms coherently trapped by this method are also commonly referred to as ‘coherently phased’ atoms. The coherently trapped state is sometimes denoted by NC, standing for ‘non-coupled’, because Im $`\chi ^{(1)}`$ $`=0`$ at the line centers of the two transitions 1$``$3 and 2$``$3. Once all the atoms of a gas have been driven to the NC state, light at the two applied laser frequencies can continue to pass over the atoms without being attenuated. There is a state orthogonal to the NC state in which the wavefunction of the atoms is a symmetric linear combination of the unperturbed wavefunctions of levels $`|1`$ and $`|2`$. Because Im $`\chi ^{(1)}`$ $`0`$ at the two allowed transitions for atoms in this state, it is sometimes referred to as the C (‘coupled’) state.

## 4 Laser without inversion (LWI); pumping via hyper-Raman scattering (HRS)

Consider a $`\mathrm{\Lambda }`$-type system with all atoms maintained in the NC state via the EIT process described above. If, through some separate means, some of these atoms can be excited to level $`|3`$, then these atoms can fluoresce at both 1$``$3 and 2$``$3 line centers via allowed transitions to the two C states shown in Fig. 3. Since the EIT mechanism rapidly and continually transfers all atoms from the C state to the NC state, true population inversions can exist between level $`|3`$ and both C states. Gain can therefore be present on these transitions, and stimulated emission (i.e. laser action) can result. This scenario is termed a ‘laser without inversion’, because there are many more atoms in each of the two NC levels than in level $`|3`$. An LWI demonstrated by the group of M.O. Scully (Padmabandu et al. padmabandu (1996)) works by combining optical pumping and EIT.

In considering mechanisms that could pump an H-atom LWI in space, one first should analyze simple linear photoexcitation of NC atoms via absorption of far-ultraviolet (FUV) continuum light from the star in the spectral vicinity of Ly-$`\beta `$. Typical H-atom densities in cold, neutral clouds surrounding bright stars are 104-105 cm-3, implying collision rates $``$10-8-10-7 sec-1. Such media should therefore be regarded as being virtually collisionless. In a collisionless regime, FUV light in the vicinity of Ly-$`\beta `$ \- but offset enough from it to avoid the $`\chi ^{(1)}`$ minimum (Fig. 4) - will either be elastically scattered by NC atoms or will undergo spontaneous resonant Raman scattering. In the latter process, an atom becomes excited to the NC $`|2`$ level, and a photon slightly offset from H($`\alpha `$) is simultaneously emitted. However, no excitation of level $`|3`$ occurs (Loudon loudon (2000)). Linear photoexcitation would therefore be an ineffective pumping mechanism for LWI in space, but it could perhaps account for the presence of spectrally broad H($`\alpha `$) emissions seen from some reddened early-type stars.

Harris et al. (harris90 (1990)) were the first to show that, while EIT makes a material system transparent to resonant laser radiation, it nonetheless allows a large nonlinear resonant process to occur with high probability. We propose that one such process, resonant hyper-Raman scattering (HRS), might be a viable mechanism for pumping an H-atom LWI in space. In the unit HRS pumping process (Fig. 5), a pair of FUV photons, with frequencies lying very close to Ly-$`\beta `$ but offset from it by equal amounts to high and low energies, are absorbed from the star’s blackbody continuum, a photon at Ly-$`\beta `$ line center is emitted, and an NC atom is excited to level $`|3`$ \- with all events in this energy conserving process occurring simultaneously. This HRS mechanism would be an efficient H-atom LWI pump, since, in the unit process, both a Ly-$`\beta `$ photon at line center is generated, and an NC atom is excited to the desired 3p level. An important feature of LWI excitation occurring via this mechanism is that the rate of pumping is itself proportional to the intensity of the radiation present at Ly-$`\beta `$ line center.

## 5 H-atom LWI associated with a reddened, early-type star

One would expect an H-atom LWI associated with a reddened early-type star to occur in a thin shell of neutral gas located just outside an ionized hydrogen (H II) region. For a B0 III star, the radius $`R_S`$ of such a region would typically be $``$0.01 pc. At 1000 Å, the FUV continuum flux at $`R_S`$ propagating outward from the star would be $``$3 x 1010 photons per cm2 per sec per wavenumber. This flux could be additionally enhanced several hundred times around the wavelength of Ly-$`\beta `$ via photoprocesses occurring in the H II region. It is also possible that nonlinear elastic scattering by H atoms of the two LWI narrow-band emissions generated would lead to additional intensity enhancement of these emissions in the active region via the effect of decreased spatial diffusion. This, in turn, would increase the rate of pumping.

From Fig. 4, one predicts a telling signature of LWI/EIT to be extremely narrow-band emission observed at both the H($`\alpha `$) and Ly-$`\beta `$ line centers. The HRS pumping process should be manifest by symmetrical absorption of continuum light around Ly-$`\beta `$ in a pattern that might superficially resemble the one shown in Fig. 2. (In Fig. 2, however, the apparent absorption dip has a stellar origin, as was noted above.)

An LWI/EIT mechanism can reasonably explain certain other intense, extremely narrow emission lines recorded by astronomers, examples being the sodium D-line doublet appearing in HD 44179, or the powerful O VI (1032 Å, 1037 Å) emission doublet that dominates the FUV spectra of symbiotic stars such as RR Tel. In both these cases, LWI/EIT would have to occur via the so-called ‘V’ scheme, which incidentally is the easiest one to excite in the presence of significant thermal Doppler broadening (Boon et al. boon (1999)). However, the environments existing in cold, collisionless neutral clouds surrounding H II regions are generally favorable for all LWI/EIT schemes.

M.O. Scully has coined the word $`phaseonium`$ to describe an ensemble of coherently phased atoms. An LWI based upon such a medium, he suggests, might appropriately be termed a $`phaser`$. Should the occurrence of LWI/EIT in space ever become substantiated, widespread usage of these terms in astronomy might follow.