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# Stability and electronic structure in hexagonal 𝛽Al₉Mn₃Si and 𝜑Al₁₀Mn₃ crystals

## 1 Introduction

The almost isomorphic stable $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$  and metastable $`\phi \mathrm{Al}_{10}\mathrm{Mn}_3`$  phases are often present in alloys containing quasicrystals in Al(Si)-Mn systems. Although their diffraction features are different from those of quasicrystals, several correlations with quasiperiodic atomic structure have been shown. For instance, there is a strong resemblance of these phases with parts of the complex structures of $`\mu \mathrm{Al}_{4.12}\mathrm{Mn}`$  and $`\lambda \mathrm{Al}_4\mathrm{Mn}`$  which are related to quasicrystals. $`\beta `$ and $`\phi `$ are also almost isomorphic with $`\mathrm{Al}_5\mathrm{Co}_2`$  which is an approximant of decagonal quasicrystal with the shortest periodic stacking sequence along the tenfold axis .

Meta-stable icosahedral ($`i`$-) and decagonal ($`d`$-) quasicrystals have been found in the Al-Mn system . With the addition of few per cent of Si atoms, new stable phases are obtained: $`i`$-Al-Mn-Si , approximant $`\alpha \mathrm{Al}_9\mathrm{Mn}_2\mathrm{Si}`$  and $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$…The occurrence of stable complex structure in Al-Mn and Al-Mn-Si is a major question in the understanding of the stability of quasicrystals. For instance, the role of Si in stabilising the $`i`$-phase, is not yet understood. In this direction, investigations on relations between isomorphic stable $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ and meta-stable $`\phi \mathrm{Al}_{10}\mathrm{Mn}_3`$ phases represent a great interest. On another hand, these phases give a good example to analyse the effect of the position of transition metal (TM) atoms in stabilising complex structure related to quasiperiodicity.

In this paper, a first-principles (ab initio) study of the electronic structure in $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ and $`\phi \mathrm{Al}_{10}\mathrm{Mn}_3`$ phases is combined with a model approach in order to describe the interplay between the medium range order and the electronic structure. Results are compared between $`\beta `$, $`\phi `$, $`\mathrm{Al}_5\mathrm{Co}_2`$, $`\mu \mathrm{Al}_{4.12}\mathrm{Mn}`$, and $`\lambda \mathrm{Al}_4\mathrm{Mn}`$ phases. The stabilising role of Si and the origin of a large hole (vacancy) in both $`\beta `$ and $`\phi `$ phases are justified. The origin of a pseudogap is analysed in the frame of the Hume-Rothery stabilisation rule for sp-d electron phases . Besides, a real space approach in term of a realistic TM-TM pair interaction allows to understand the effect of Mn position. As these phases are related to quasiperiodic phases, such a study yields arguments to discuss the interplay between electronic structure and stability in quasicrystals.

The paper is organised as follows. In section 2, is presented a short review on Hume-Rothery mechanism in Al(rich)-TM phases that has often been proposed for the stabilisation of crystals and quasicrystals. The structures of $`\phi `$ and $`\beta `$ are presented in section 3 with a discussion on their relations with quasicrystals. First-principles (ab initio) study of the electronic structure is presented in section 4. Then the effect of the sp-d hybridisation is analysed in details through ab initio calculations for hypothetical structures. In section 5, these results are understood in term of a Friedel-Anderson sp-d hamiltonian that allows to find the “effective Bragg potential” for sp-d Hume-Rothery alloys. In section 6, a real space approach of the Hume-Rothery mechanism shows the strong effect of a medium range Mn-Mn pair interaction (up to $`5\mathrm{\AA }`$ and more). Magnetism is studied in section 7 and a short conclusion is given in section 8.

## 2 Hume-Rothery stabilisation in quasicrystals and related crystals

### 2.1 Near contact between Fermi sphere and pseudo-Brillouin zone

Since the 1950s, Al(rich)-TM crystals are considered by many authors as Hume-Rothery alloys  (for instance see Refs ). In these phases, the important parameter is the average number of electrons per atom, $`e/a`$. The valence of Al and Si are fixed without ambiguity (+3 and +4, respectively). Following classical theory , a negative valence is assigned to TM atom (typically, $`3`$ for Mn, $`2`$ for Fe, $`1`$ for Co and $`0`$ for Ni). For $`\phi \mathrm{Al}_{10}\mathrm{Mn}_3`$, $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ and $`\mathrm{Al}_5\mathrm{Co}_2`$, $`e/a`$ is equal to 1.61, 1.69 and 1.86, respectively. The occurrence of different compounds with similar structures is therefore to be explained by the fact that they are electron compounds with similar e/a ratio in spite of different atomic concentrations . Indeed, for these phases a band energy minimisation occurs when the Fermi sphere touches a pseudo-Brillouin zone (prominent Brillouin zone), constructed by Bragg vectors $`𝐊_p`$ corresponding to intense peaks in the experimental diffraction pattern. The Hume-Rothery condition for alloying is then $`2k_FK_p`$. Assuming a free electron valence band, the Fermi momentum, $`k_F`$, is calculated from $`e/a`$.

Soon after the discovery of quasicrystals, it has been pointed out that their stoechiometry appears to be governed by a Hume-Rothery rule (see for instance ). Indeed the $`e/a`$ ratio has been used for a long time to distinguish between Frank-Kasper type quasicrystals (sp quasicrystals) and Mackay type quasicrystals (sp-d quasicrystals) . Friedel and Dénoyer  have determined the pseudo-Brillouin zone in contact with the Fermi sphere for $`i`$-Al-Li-Cu. Gratias et al.  have shown that the Al-Cu-Fe icosahedral domain is located along a line in the phase diagram defined by the equation $`\mathrm{e}/\mathrm{a}1.86`$. Besides, Al-Cu-Fe alloys along an $`e/a`$-constant line have similar local electronic properties and local atomic order . Recently, a pseudo-Brillouin zone that touches the Fermi Sphere in 1/1 Al-Cu-Ru-Si and Al-Mg-Zn approximants has been identified . With the discovery of decagonal $`d`$-Al-Cu-Co and $`d`$-Al-Ni-Co by Tsai et al. , these authors  have determined that the value of $`e/a`$ ratio is about 1.7 in spite of wide composition range for quasicrystals in these systems. The importance of $`e/a`$ value in quasicrystals and their properties suggests that Hume-Rothery mechanism plays a significant role in their stabilisation.

### 2.2 Pseudogap in the density of states

The density of states (DOS) in sp Hume-Rothery alloys is well described by the Jones theory (for review see Refs ). The valence band (sp states) are nearly-free electrons, and the Fermi-sphere / pseudo-Brillouin zone interaction creates a depletion in the DOS, called “pseudogap”, near the Fermi energy, $`\mathrm{E}_\mathrm{F}`$. This pseudogap has been found both experimentally and from first-principles calculations in classical Hume-Rothery alloys (see for instance the recent theoretical study of archetypal system Cu-Zn ). It has also been found experimentally and theoretically in sp quasicrystals and related phases (for instance in Al-Li-Cu  and Al-Mg-Zn ). But, the treatment of Al(rich) alloys containing transition metal elements requires a new theory. Indeed, the d states of TM are not nearly-free states in spite of strong sp-d hybridisation. Thus a model for sp-d electron phases which combined the effect of the diffraction by Bragg planes with the sp-d hybridisation has been developped . It is shown that negative valence of TM atom results from particular effects of the sp-d hybridisation in Hume-Rothery alloys . Besides the TM DOS (mainly d states) depends strongly on TM atoms positions. For particular TM positions, one obtains a pseudogap near $`E_F`$ in total DOS and partial d DOS. This has been confirmed by ab initio calculations in a series of Al(rich)-TM crystals including $`\mathrm{Al}_5\mathrm{Co}_2`$ ,which is isomorphic with $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ and $`\phi \mathrm{Al}_{10}\mathrm{Mn}_3`$. The presence of a pseudogap in $`\mathrm{Al}_5\mathrm{Co}_2`$ DOS has also been confirmed by photoemission spectroscopy . For icosahedral sp-d quasicrystals and their approximants, a wide pseudogap at $`\mathrm{E}_\mathrm{F}`$ has been found experimentally  and from ab initio calculations . For instance in $`i`$-Al-Cu-Fe, $`i`$-Al-Pd-Mn and $`\alpha `$ Al-Mn-Si, the DOS at $`\mathrm{E}_\mathrm{F}`$ is reduced by $`1/3`$ with respect to pure Al (c.f.c.) DOS .

However, there are contradictory results about DOS in decagonal quasicrystals. Photoemission spectroscopy measurements in the photon-energy range 35-120 eV do not show any pseudogap  in $`d`$-$`\mathrm{Al}_{65}\mathrm{Co}_{15}\mathrm{Cu}_{20}`$ and $`d`$-$`\mathrm{Al}_{70}\mathrm{Co}_{15}\mathrm{Ni}_{15}`$, whereas ultrahigh resolution ultraviolet photoemission shows a depletion of the DOS at $`\mathrm{E}_\mathrm{F}`$ for the same compositions . From soft X-ray spectroscopy, DOS in $`d`$-$`\mathrm{Al}_{65}\mathrm{Co}_{20}\mathrm{Cu}_{15}`$ and $`d`$-$`\mathrm{Al}_{70}\mathrm{Co}_{15}\mathrm{Ni}_{15}`$, exhibits also a pseudogap in the Al-3p band . Recently a pseudogap, enhanced by sp-d hybridisation, has been found in the Al-p band of $`d`$-Al-Pd-Mn . There are also ab initio calculations performed for several atomic model approximants of $`d`$-Al-Cu-Co , $`d`$-Al-Co-Ni  and $`d`$-Al-Pd-Mn . The results show that an existence of pseudogap depends on the position of the TM atoms. Indeed, some TM atoms may “fill up” the pseudogap, via the sp-d hybridisation; whereas other TM positions enhance the pseudogap.

In summary, the importance of Hume-Rothery mechanism is now established for many Al-based quasicrystals with and without TM elements although the presence of a pseudogap near $`E_F`$ is still discussed for decagonal phases. Nevertheless, one can not ignore the possible Hume-Rothery stabilising effect on the origin of the quasiperiodicity. This is the reason why in this article ab initio results are analysed in the frame work of Hume-Rothery mechanism in order to test the importance of this mechanism.

## 3 Structures and relations with quasicrystals

### 3.1 General aspects

The unit cell dimensions of $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$  and $`\phi \mathrm{Al}_{10}\mathrm{Mn}_3`$  are similar, with a same space group $`\mathrm{P6}_3/\mathrm{mmc}`$. Atomic environment and interatomic distances are gathered in tables 1 and 2.

First atom neighbours of the Mn site correspond to 10 Al/Si + 2 Mn atoms situated at vertices of a distorted icosahedron. Such an icosahedron is considered in the structural representation of $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ (figure 1). The small Al(0)-TM, Al(1)-TM and Al(2)-TM distances suggest a strong effect of the sp-d hybridisation. Each Mn has two Mn first neighbours in Mn-triplet. Between Mn-triplets, Mn-Mn distances are about $`4.17\mathrm{\AA }`$. Similar Mn-triplets exist also in $`\mu \mathrm{Al}_{4.12}\mathrm{Mn}`$ (hexagonal, $`\mathrm{P6}_3/\mathrm{mmc}`$, $``$ 563 atoms / unit cell) . $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ and $`\phi \mathrm{Al}_{10}\mathrm{Mn}_3`$ have significant relations with the complex structures $`\mu \mathrm{Al}_{4.12}\mathrm{Mn}`$ and $`\lambda \mathrm{Al}_4\mathrm{Mn}`$ (hexagonal, $`\mathrm{P6}_3/\mathrm{m}`$, $``$ 568 atoms / unit cell)  that are related to quasicrystals. For instance, in figure 1 of Ref. , the outline of the repeated unit of $`\phi `$ phase on several parts of $`\mu `$ structure is shown. Kreiner and Franzen  showed that the I3-cluster, a structure unit of three vertex connected icosahedra, is the basic building block of a large number of intermetallic phases related to $`i`$-Al-Mn-Si such as $`\alpha \mathrm{Al}_9\mathrm{Mn}_2\mathrm{Si}`$, $`\mu \mathrm{Al}_{4.12}\mathrm{Mn}`$ and $`\lambda \mathrm{Al}_4\mathrm{Mn}`$. Note that the environment of Mn are also close to those found in $`\alpha `$ Al-Mn-Si approximant .

### 3.2 Vacancies

The hexagonal structure of $`\mathrm{Al}_5\mathrm{Co}_2`$  is almost isomorphic with $`\beta `$ and $`\phi `$ where Co replace Mn and Va sites (table 1). These phases have similar atomic sites and first-neighbours distances (table 2). However, a major difference is that the site (2d) is empty (Va) in $`\beta `$ and $`\phi `$ whereas it is occupied by cobalt (Co(0)) in $`\mathrm{Al}_5\mathrm{Co}_2`$. It is thus interesting to understand why this vacancy is maintained in $`\beta `$ and $`\phi `$ crystals? As first-neighbour distances around Mn in $`\phi `$ and $`\beta `$ are similar to those around Co in $`\mathrm{Al}_5\mathrm{Co}_2`$, and that Va-Al distances in $`\beta `$ and $`\phi `$ are very close of Co(0)-Al distances a vacancy can not be explained from steric encumbering. The environment of Va forms a Tri-capped trigonal prism (3 Al(1) and 6 Al(2)).

The same environment is also found in $`\mu \mathrm{Al}_{4.12}\mathrm{Mn}`$  and $`\lambda \mathrm{Al}_4\mathrm{Mn}`$ . But in $`\mu `$ and $`\lambda `$, this site is occupied by a Mn atom (Mn(1) in (2b) in $`\mu \mathrm{Al}_{4.12}\mathrm{Mn}`$ and Mn(1) in (2d) in $`\lambda \mathrm{Al}_4\mathrm{Mn}`$). In $`\mu `$ and $`\lambda `$, the first-neighbour distances Mn(1)-Al are 2.35$``$2.48 $`\mathrm{\AA }`$, which are similar to Va-Al first-neighbour distances in $`\beta `$ and $`\phi `$.

In the following, it is shown that the presence (or not) of such a vacancy in $`\beta `$ and $`\phi `$ can be explained on account of the medium range atomic order because of strong Mn-Mn pair interaction up to medium range distances (more than 5 $`\mathrm{\AA }`$).

### 3.3 Role and position of Si atoms

The role of Si in Al based quasicrystals and related phases is known to have an important effect. Unstable quasicrystals are obtained in Al-Mn system, whereas stable quasicrystals are formed when a small proportion of Si is added . Similar stabilising effects occurs for $`i`$-Al-Cu-Cr-Si  and for approximants $`\alpha `$ Al-Mn-Si , 1/1 Al-Cu-Fe-Si , $`\alpha `$ Al-Re-Si . The number of valence electrons are 3 (4) per Al (Si) atom. With respect to a Hume-Rothery condition for alloying ($`2k_FK_p`$), it is possible that a substitution of a small quantity of Si increases the $`e/a`$ ratio in better agrement with $`2k_FK_p`$.

Experimentally Al and Si atoms have not been distinguished in $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$. However, Robinson  has proposed to consider Si in (2a) because the interatomic distances between an atom on sites (2a) and its six neighbouring Al atoms is less than between any other pairs of Al atoms in $`\beta `$ structure (table 2). But, from a comparison of $`\beta `$ and $`\phi `$, Taylor  has suggested that Si atoms should be preferentially in (12k) with Al atoms instead of (2a).

In section 4.2, we give arguments form ab initio calculations to understand the effect of Si on the Hume-Rothery stabilisation and to conclude that Si are likely in (2a).

## 4 First-principles calculations of the electronic structure

### 4.1 LMTO procedure, treatment of Si

Electronic structure determinations were performed in the frame-work of the local spin-density approximation (LSDA)  by using the ab initio Linear Muffin Tin Orbital method (LMTO) in an Atomic Sphere Approximation (ASA) . The space is divided into atomic spheres and interstitial region where the potential is spherically symmetric and flat, respectively. Sphere radii were chosen so that the total volume of spheres equals that of the solid. For vacancies (Va) empty spheres were introduced in (2d). The sphere radii are $`R_{Si/Al(0)}=1.37`$$`\mathrm{\AA }`$, $`R_{Al(1)}=R_{Al(2)}=1.53`$$`\mathrm{\AA }`$, $`R_{Mn}=1.34`$$`\mathrm{\AA }`$, $`R_{Va}=1.04`$$`\mathrm{\AA }`$ for $`\beta `$ phase, and $`R_{Al(0)}=1.38`$$`\mathrm{\AA }`$, $`R_{Al(1)}=R_{Al(2)}=1.55`$$`\mathrm{\AA }`$, $`R_{Mn}=1.35`$$`\mathrm{\AA }`$, $`R_{Va}=1.05`$$`\mathrm{\AA }`$ for $`\phi `$ phase. As these structures are metallic and rather compacts, it was found that a small change of the sphere radii does not modify significantly the results.

Neglecting the spin-orbit coupling, a scalar relativistic LMTO-ASA code, was used with combined corrections for ASA . The k integration in a reduced Brillouin zone was performed according to the tetrahedron method  in order to calculate the electronic density of states (DOS). The final step of the self-consistent procedure and the DOS calculation were performed with 4416 k points in the reduced Brillouin zone. With an energy mesh equals to $`\mathrm{\Delta }E=0.09`$ eV, calculated DOSs do not exhibit significant differences when the number of k points increases from 2160 to 4416. Thus, the structure in the DOS larger than 0.09 eV are not artefacts in calculations. Except in section 7, the LMTO DOSs calculations were performed without polarised spin (paramagnetic state).

The LMTO-ASA basis includes all angular moments up to $`l=2`$ and the valence states are Al (3s, 3p, 3d), Mn (4s, 4p, 3d), Co (4s, 4p, 3d), Si (3s, 3p, 3d) and Va (1s, 2p, 3d) 111In ASA approximation, orbitals are introduced in vacancies in order to yield a good expansion of the LMTO orbitals out of atomic spheres.. In order to analyse the position of Si atoms in the $`\beta `$ phase, we performed calculations for $`\beta (\mathrm{Al},\mathrm{Si})_{10}\mathrm{Mn}_3`$ where the Si atoms occupied randomly the Al sites. In this case an average atom named (Al,Si) was considered (virtual crystal approximation). In the LMTO-ASA procedure this atom is simulated with nuclear charge $`Z=(1c)Z_{Al}+cZ_{Si}`$, where $`c`$ is the proportion of Si atoms, and $`Z_{Al}=13`$, $`Z_{Si}=14`$ are the nuclear charge of Al, Si, respectively. Such a calculation can be justified as the main difference between Al and Si is the number of valence electrons. It was checked that the LMTO-ASA total energy of pure Al and pure Si are almost equal to this calculated with the average (Al,Si) atom with $`c=0.01`$ and $`c=0.99`$, respectively. Three possibilities were considered for the $`\beta `$ phase: (i) the phase named $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ where Si are on site (2a) and Al, on site (6h) and site (12k); (ii) the phase $`\beta \mathrm{I}`$-$`(\mathrm{Al},\mathrm{Si})_{10}\mathrm{Mn}_3`$ where Si atoms substitute for some Al (on sites (2a), (6h) and (12k)); (iii) the phase $`\beta \mathrm{II}`$-$`(\mathrm{Al},\mathrm{Si})_{10}\mathrm{Mn}_3`$ where Si atoms substitute for some Al(2) (site (12k)). Same sphere radii for these three cases were input.

### 4.2 General aspects of the density of states (DOS)

Total energy self-consistent calculations were performed for different volumes, with isotropic volume changes i.e. the ratio $`c/a`$ is constant and equal to the experimental value (table 1). The atomic positions were not relaxed. Minima of energy were obtained for a lattice parameter $`a`$ equal to 7.41 $`\mathrm{\AA }`$ for $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$, 7.41 $`\mathrm{\AA }`$ for $`\beta \mathrm{I}`$-$`(\mathrm{Al},\mathrm{Si})_{10}\mathrm{Mn}_3`$, 7.42 $`\mathrm{\AA }`$ for $`\beta \mathrm{II}`$-$`(\mathrm{Al},\mathrm{Si})_{10}\mathrm{Mn}_3`$, and 7.43 $`\mathrm{\AA }`$ for $`\phi \mathrm{Al}_{10}\mathrm{Mn}_3`$. These values correspond within $`1.5\%`$ to experimental values. Similar results have also been found in LMTO-ASA calculations for Al-TM alloys with small concentration of TM elements .

The total DOSs in $`\beta `$ and $`\phi `$ phases (figure 2), are very similar. Local DOSs in $`\beta `$ are also shown in figure 3. Except for low energies (less than $`10`$eV), the total DOS in $`\beta `$ does not depend on the Si position. The parabola due to the Al nearly-free states is clearly seen. The large d band from $`2`$ up to $`2`$ eV is due to a strong sp-d hybridisation in agreement with experimental results  and with first-principles calculations on Al-TM crystals and quasicrystals .

The sum of local DOSs on Al and Si atoms, shown in figure 4(a), is mainly sp DOS. As expected for a Hume-Rothery stabilisation, it exhibits a wide pseudogap near $`E_F`$ due to electron scattering by Bragg planes of a predominant pseudo-Brillouin zone (i.e. the pseudo-Brillouin zone close to the Fermi surface). Its width of about 1 eV is of the same order of magnitude to this found in Al-Mn icosahedral approximants . The large pseudogap in {Al $`+`$ Si} DOS is meanly characteristic of a p-band at this energy, but the pseudogap in the total DOS is narrower. Therefore, the d states of Mn atoms must fill up partially the pseudogap. Nevertheless, as it is shown in the following that the pseudogap in {Al $`+`$ Si} DOS results from Mn sub-lattice effect.

Spiky total DOS where obtained for the studied phases as it has been found in LMTO DOS of icosahedral small approximants (for instance $`\alpha `$Al-Mn-Si , 1/1 Al-Cu-Fe , 1/1 Al-Pd-Mn ). In fact this is a consequence of a small electron velocity (flat dispersion relations) which contributes to anomalous electronic transport properties . Such properties are not specific of quasicrystals as they are also observed in many crystal related to quasicrystals, therefore it does not only come from the long range quasiperiodicity. They are also associated with local and medium range atomic order that are related to quasiperiodicity. Indeed, it has been shown  that fine peaks in the DOS could come from electron confinement in atomic clusters characteristic  of the quasiperiodicity. This is not in contradiction with a Hume-Rothery mechanism because this tendency to localisation has a small effect on the band energy . Whether spiky DOSs exist in quasicrystals or not is however much debated experimentally  and theoretically (Ref  and references therein) and the present calculation does not give answer to this question for the case of quasicrystals. But, in case of $`\beta `$ and $`\phi `$ crystals, we checked that structures in the DOS with an energy scale larger than 0.09 eV are not artifacts in calculation as they do not depend on the non-physical parameters in the LMTO procedure (number of k points, see section 4.1).

### 4.3 Analysis of Si effect

From LMTO band energy calculated with fixed atomic positions and composition, the lowest band energy is obtain when Si atoms are in (2a) in $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$. The difference in band energy between $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ and $`\beta \mathrm{I}`$-$`(\mathrm{Al},\mathrm{Si})_{10}\mathrm{Mn}_3`$ is $`+5`$ eV / unit cell. The same order of magnitude is obtained between $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ and $`\beta \mathrm{II}`$-$`(\mathrm{Al},\mathrm{Si})_{10}\mathrm{Mn}_3`$. These ab initio results shows that Si are in (2a) and not mixed with Al. A comparison between the band energy of $`\beta `$ and $`\phi `$ phases cannot be made because their compositions are different.

In the vicinity of $`E_F`$, the total DOSs in $`\beta `$ and $`\phi `$ are very similar except $`E_F`$ positions (figure 2). At $`E_F`$, the DOS is $`5.6`$states$`/`$eV.cell in $`\beta `$, $`16.0`$states$`/`$eV.cell in $`\phi `$. The small amount of Si increases the average valence $`e/a`$ in $`\beta `$. In a rigid band like model, this $`E_F`$ shifts up to the minimum of the pseudogap, and in Hume-Rothery mechanism, the band energy is minimised. This difference allows one to understand why $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ phase is stable whereas $`\phi \mathrm{Al}_{10}\mathrm{Mn}_3`$ phase is metastable.

Differences between $`\beta (\mathrm{Al},\mathrm{Si})_{10}\mathrm{Mn}_3`$ where Si atoms are mixed with Al atoms, and $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ where Si atoms are in (2a) can also be understood from LMTO DOSs. Indeed, two bonding peaks are present at low energies ($`11.5`$ eV and $`10.3`$eV, figure 3) in the local Si DOS of $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$, which is no more nearly-free states (each Si atom has 6 Al(2) and 6 Mn first neighbours (table 2)). The close proximity between Si and Mn and the presence of a bonding peak in the partial Mn DOS suggest that the Si-Mn bond is rather covalent and thus increases the stability of $`\beta `$ phase when Si is on site (2a).

### 4.4 Effects of the d state of the transition-metal (TM) atoms

In this part the origin of the pseudogap is analysed from LMTO calculations for hypothetical phases derived from $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$. Three points are successively considered $`(i)`$ the strong effect of the sp-d hybridisation on the pseudogap, $`(ii)`$ the role of the Mn position which explains the origin of the vacancy (Va) in $`\beta `$ and $`\phi `$, $`(iii)`$ and the great effect of Mn-Mn medium range interaction up to $`5\mathrm{\AA }`$.

#### (i) Role of the sp-d hybridisation on the pseudogap

Self-consistent LMTO calculation where performed without sp-d hybridisation by setting to zero the corresponding terms of the hamiltonian matrix . Such a calculation is physically meaningful because the d TM states are mainly localised in the TM sphere and the sp Al states are delocalised. In figure 3, local Mn DOS (mainly d states), is drawn for two cases: with sp-d hybridisation and without sp-d hybridisation. The comparison between these local DOSs shows that the sp-d hybridisation increases the width of d band. This confirms a strong sp-d hybridisation. The local {Al + Si} DOS (mainly sp DOS) is also strongly affected by a sp-d hybridisation. As a matter of fact the pseudogap disappears in the calculation without sp-d hybridisation (figure 4(b)).

For Hume-Rothery alloys containing TM elements, a stabilisation mechanism is more complex than in sp alloys because of a strong sp-d hybridisation in the vicinity of $`E_F`$. Al and Si atoms, which have a weak potential, scatter sp electrons by a potential $`V_B`$ almost energy independent. This leads to the so-called diffraction of electrons by Bragg planes in sp alloys. But the potential of Mn atoms depends on the energy. It is strong for energies around $`E_d`$, and creates a d resonance of the wave function that scatters also sp states. The effect is analysed in detail from a model hamiltonian in section 5. LMTO calculation was performed on hypothetical $`\beta \mathrm{Al}_9\mathrm{Al}_3\mathrm{Si}`$ constructed by putting Al in place of Mn in $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ in order to confirm (or not) the previous analysis. The resulting total DOS (mainly sp DOS) of the hypothetical phase has no pronounced pseudogap (figure 4(c)). But there are many small depletions that might come from diffractions by Bragg planes. It shows that classical diffractions by Bragg planes by a weak potential $`V_B`$ can not explain a pseudogap close to $`E_F`$ in $`\beta \mathrm{Al}_9\mathrm{Al}_3\mathrm{Si}`$ and $`\phi \mathrm{Al}_{10}\mathrm{Mn}_3`$.

#### (ii) Effect of the Mn position, origin of the vacancy

As explained in section 3, a particularity of $`\beta `$ and $`\phi `$ structures is a vacancy in (2d). This is the main difference with the $`\mathrm{Al}_5\mathrm{Co}_2`$ structure (table 1). The origin of a vacancy can not be explained from too short near-neighbour distances (section 3.2). Therefore, a LMTO calculation was performed including a new Mn atom, named Mn(0), on site (2d) in $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ phase using atomic sites and lattice parameters of $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ (table 1). This hypothetical phase is named $`\beta \mathrm{Al}_9\mathrm{Mn}_4\mathrm{Si}`$ and its total and {Al $`+`$ Si} DOSs are shown in figures 5 and 4(d), respectively. The absence of pseudogap in the total DOS results of a the great effect of Mn(0). In {Al $`+`$ Si} DOS the pseudogap created by the scattering of sp electrons by the sub-lattice of Mn in (6h) is still present. But a large peak at $`E_F`$ fills up partially the pseudogap. Consequently, $`E_F`$ is located in a peak due to sp(Al)-d(Mn(0)) hybridisation. This is in fact a good example where a sp-d hybridisation does not induce a pseudogap. A similar result was obtained with an hypothetical $`\phi \mathrm{Al}_{10}\mathrm{Mn}_4`$, built by putting a Mn atom in place of the vacancy in (2d).

Total and local DOSs of hypothetical $`\beta \mathrm{Al}_9\mathrm{Mn}_4\mathrm{Si}`$ and $`\mathrm{Al}_5\mathrm{Co}_2`$  are compared in figure 5. In spite of the near isomorphism between these structures, their DOSs are very different. As there is pseudogap in $`\mathrm{Al}_5\mathrm{Co}_2`$ and not in $`\beta \mathrm{Al}_9\mathrm{Mn}_4\mathrm{Si}`$, it indicates that Co(0) and Mn(0) act differently, thus justifying the existence of a vacancy in both $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ and $`\phi \mathrm{Al}_{10}\mathrm{Mn}_3`$ phases and not in $`\mathrm{Al}_5\mathrm{Co}_2`$.

Therefore, the similar Wyckoff sites lead to both anti-bonding or bonding peaks depending on the nature of the atom on the Wyckoff site (2d), either Mn(0) or Co(0) respectively. Since there is a great effect of the nature of the TM element, a further analysis is proposed in section 6, where cohesive energies are compared using realistic TM-TM pair interaction.

#### (iii) Effect of Mn-Mn medium range interaction

The Mn-Mn distances in $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ are reported in table 3. Mn are grouped together to form Mn-triplets (section 3.1). In order to determine the effect of a possible Mn-Mn medium range interaction on a pseudogap, a LMTO calculation was performed on a modified $`\beta `$ phase containing only one Mn-triplet per unit cell instead of two. In this case, $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ was transformed into $`\beta \mathrm{Al}_9\mathrm{Mn}_{1.5}\mathrm{Cu}_{1.5}\mathrm{Si}`$ by remplacing a Mn-triplet by a Cu-triplet. Mn environments remain identical up to $`4.17\mathrm{\AA }`$ (table 3).

As results, the local Cu DOS (mainly d states, figure 6(d)) at $`E_F`$ is very small; Cu having almost the same number of sp electrons as Mn, it has a minor effect near $`E_F`$. For the local Mn DOS the pseudogap disappears completely (figure 6(c)). For the total DOS, a small depletion below $`E_F`$ is still remaining (figure 6(a)), and for the local {Al + Si} DOS there is a pseudogap below $`E_F`$ (figure 6(b)), but less pronounced than for $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ (figure 4(a)). Therefore, such a disappearence of pseudogap proves the effect of Mn-Mn interactions over medium distances equal to 4.17, 4.96, 6.38 $`\mathrm{\AA }`$…(table 3).

## 5 Effective Bragg potential for sp states

### 5.1 Exitence of effective sp hamiltonian

As electrons are nearly-free electrons in Hume-Rothery sp crystals without TM atoms the hamiltonian writes ,

$`H_{sp}={\displaystyle \frac{\mathrm{}^2k^2}{2m}}+V_B.`$ (1)
$`V_B`$ is a weak potential (Bragg potential), and does not depend on an energy,

$`V_B(𝐫)={\displaystyle \underset{𝐊}{}}V_B(𝐊)\mathrm{e}^{i𝐊𝐫},`$ (2)
where the vectors $`𝐊`$ belong to the reciprocal lattice. However, for alloys containing TM atoms, the strong scattering of sp electrons by TM atoms can not be described from a weak potential. In this case, a generalised Friedel-Anderson hamiltonian  has been considered. In a non-magnetic case:

$`H=H_{sp}+H_d+H_{sp\text{-}d},`$ (3)
where sp states are delocalised nearly-free states (equation (1)) and d states are localised on d orbitals of TM atoms. $`H_d`$ is the energy of d states. The term $`H_{sp\text{-}d}`$ represents a sp-d coupling which is essential in this context. The eigenstates $`\psi `$ of $`H`$ can be decomposed in two terms:

$`|\mathrm{\Psi }=|\mathrm{\Psi }_{sp}+|\mathrm{\Psi }_d,`$ (4)
where $`\mathrm{\Psi }_{sp}`$ and $`\mathrm{\Psi }_d`$ are each linear combinations of sp states and linear combinations of d orbitals of all TM atoms. The classical tight-binding approximation $`\mathrm{\Psi }_{sp}|\mathrm{\Psi }_d=0`$ is made.

An “effective Bragg potential” for sp states, including effects of d orbitals of TM atoms, is calculated in order to analyse the effect of TM atoms. A projection of the Schrödinger equation, $`(HE)|\mathrm{\Psi }=0`$, on the sub-space generated by sp states allows one to write the effective hamiltonian for sp states:

$`H_{eff(sp)}={\displaystyle \frac{\mathrm{}^2k^2}{2m}}+V_{B,eff}\mathrm{with}V_{B,eff}=V_B+H_{sp\text{-}d}{\displaystyle \frac{1}{EH_d}}H_{sp\text{-}d},`$ (5)
and where $`V_B`$ is as given by equation (2). The second term of $`V_{B,eff}`$ depends on energy. In crystals and quasicrystals, $`V_{B,eff}`$ is an effective Bragg potential that takes into account the scattering of sp states by the strong potential of TM atoms.

### 5.2 Characteristic of effective Bragg potential

For the phases presently considered, there are a few pairs of Mn atoms that are near-neighbours. Indeed each Mn is surrounded by 10 Al (Si) and 2 Mn (section 3). Therefore, a direct hoping between two d orbitals can be neglected. Thus:

$`H_d={\displaystyle \underset{d,i}{}}E_{di}|d,id,i|,`$ (6)
where $`i`$ is a TM site index and $`d`$ the five d orbitals of each TM atom. Assuming that all TM atoms are equivalent, one has $`E_{di}=E_d`$. The Fourier coefficients of the effective Bragg potential $`V_{B,eff}`$ are calculated from $`H_{eff(sp)}`$ using the formula $`V_{B,eff}(𝐊)=𝐤|H_{eff(sp)}|𝐤𝐊`$. One obtains:

$`V_{B,eff}(𝐫)={\displaystyle \underset{𝐊}{}}\left(V_B(𝐊)+{\displaystyle \frac{|t_{𝐤,𝐊}|^2}{EE_d}}{\displaystyle \underset{i}{}}e^{i𝐊.𝐫_i}\right)e^{i𝐊.𝐫},`$ (7)
$`\mathrm{where}|t_{𝐤,𝐊}|^2={\displaystyle \underset{d=1}{\overset{5}{}}}𝐤|H_{sp\text{-}d}|d_0d_0|H_{sp\text{-}d}|𝐤𝐊,`$ (8)
where $`𝐫_i`$ is the position of TM(i) atoms. By convention a TM atom with orbital $`d_0`$ is on a site at $`𝐫_0=0`$. $`t_{𝐤,𝐊}`$ is a matrix element that couples sp states $`|𝐤`$ and $`|𝐤𝐊`$ via sp-d hybridisation. The expression (7) is exact providing that a direct d-d coupling is neglected.

The potential of TM atoms is strong and creates d resonance of the wave function in an energy range $`E_d\mathrm{\Gamma }EE_d+\mathrm{\Gamma }`$, where $`2\mathrm{\Gamma }`$ is the width of the d resonance. In this energy range, the second term of equation (7) is essential as it does represent the diffraction of the sp electrons by a network of d orbitals, i.e. the factor $`\left(_ie^{i𝐊.𝐫_{di}}\right)`$ corresponding to the structure factor of the TM atoms sub-lattice. As the d band of Mn is almost half filled, $`E_FE_d`$, this factor is important for energy close to $`E_F`$. Note that the Bragg planes associated with the second term of equation (7) correspond to Bragg planes determined by diffraction. For $`\beta `$ phase, it can be concluded that $`V_B`$ has no effect on a pseudogap and on a phase stabilisation because of absences of pseudogap for DOS calculated for $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ without sp-d hybridisation (figure 4(b)) and $`\beta \mathrm{Al}_9\mathrm{Al}_3\mathrm{Si}`$ without Mn atoms (figure 4(c)). Let us note however that the Hume-Rothery mechanism for alloying still minimizes the sp band energy due to a strong scattering of sp states by the Mn sub-lattice.

In summary, an analyse in term of effective Bragg potential allows one to interpret LMTO results as hybridisation-induced pseudogap in total and sp DOSs which comes from a diffraction of sp states by the sub-lattice of Mn atoms via the sp-d hybridisation. In this context the medium range distance between TM atoms might have important role.

## 6 Role of indirect Mn-Mn pair interaction

### 6.1 Medium range TM-TM interaction in Al based alloys

As a Hume-Rothery stabilisation is a consequence of oscillations of charge density of valence electrons with energy close to $`E_F`$ , a most stable atomic structure is obtained when distances between atoms are multiples of the wavelength $`\lambda _F`$ of electrons with energy close to $`E_F`$. Since the scattering of valence sp states by the Mn sub-lattice is strong, the Friedel oscillations of charge of sp electrons around Mn must have a strong effect on a stabilisation. Taking into account that stabilisation occurs for a specific Mn-Mn distance of 4.7 $`\mathrm{\AA }`$ . A Hume-Rothery mechanism in Al(rich)-TM compounds might be analysed in term of an indirect medium range TM-TM pair interaction resulting from a strong sp-d hybridisation. Zou and Carlsson  have calculated this interaction from an Anderson model hamiltonian with two impurities, using a Green’s function method. A calculation of an indirect TM-TM pair interaction, $`\mathrm{\Phi }_{TM\text{-}TM}`$, within a multiple scattering approach  yields a result in good agreement with this given in Ref.  (figure 7). Mn-Mn  and Co-Co  interactions have been used successfully for molecular-dynamics studies  of Al-Mn and Al-Co systems near the composition of quasicrystals.

As interaction magnitudes are larger for TM-TM than for Al-TM and Al-Al, $`\mathrm{\Phi }_{TM\text{-}TM}`$ has a major effect on the electronic energy. Because of the sharp Fermi surface of Al, it asymptotic form at large TM-TM distance ($`r`$) is of the form:

$`\mathrm{\Phi }_{TM\text{-}TM}(r){\displaystyle \frac{\mathrm{cos}(2k_Fr\delta )}{r^3}}.`$ (9)
The phase shift $`\delta `$ depends on the nature of the TM atom and varies from $`2\pi `$ to $`0`$ as the d band fills. Magnitude of the medium range interaction is larger for Mn-Mn than for other transition metal (Cr, Fe, Co, Ni, Cu), because the number of d electrons close to $`E_F`$ is the largest for Mn, and the most delocalised electrons are electrons with Fermi energy. From the figure 7 and equation (9), it is clear that distances corresponding to minima of $`\mathrm{\Phi }_{TM\text{-}TM}`$ depend also on the nature of TM atom.

### 6.2 Contribution of the medium range Mn-Mn interaction to total energy

The “structural energy”, $``$, of TM sub-lattice in Al(Si) host is defined as the energy needed to built the TM sub-lattice in the metallic host that simulates Al and Si atoms from isolated TM atoms in the metallic host. $``$ per unit cell is:

$`={\displaystyle \underset{i,j(jj)}{}}{\displaystyle \frac{1}{2}}\mathrm{\Phi }_{TM\text{-}TM}(r_{ij})e^{\frac{r_{ij}}{L}},`$ (10)
where $`i`$ and $`j`$ are index of TM atom and $`r_{ij}`$, TM(i)-TM(j) distances. $`L`$ is the mean-free path of electrons due to scattering by static disorder or phonons . $`L`$ depends on the structural quality and temperature and can only be estimated to be larger than 10 $`\mathrm{\AA }`$. Note that a similar exponential damping factor was introduced originaly in the treatment of RKKY interaction . In the following, the effects of TM-TM pairs over distances larger than first-neighbour distances is analysed. Therefore, an energy $`^{}`$ is calculated from equation (10) without including first-neighbour TM-TM terms in the sum. $`^{}`$ is the part of the structural energy of TM sub-lattice that only comes from medium range distances.

Structural energies, $`^{}`$, of the Mn sub-lattice are shown for $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ and $`\phi \mathrm{Al}_{10}\mathrm{Mn}_3`$ structures in figure 8, where they are compared to those of $`\mathrm{o}\mathrm{Al}_6\mathrm{Mn}`$  and $`\alpha `$ Al-Mn-Si approximants . $`^{}`$ are always negative with magnitudes less than $`0.1`$ eV $`/`$ TM atom, but strong enough to give a significant contribution to the band energy.

This result is in good agreement with an effect of Mn sub-lattice on the pseudogap as shown previously (sections 4.4 and 5). According to a Hume-Rothery mechanism, one expects that a pseudogap is well pronounced for a large value of $`|^{}|`$. Such a correlation is verified for the hypothetical $`\beta \mathrm{Al}_9\mathrm{Mn}_{1.5}\mathrm{Cu}_{1.5}\mathrm{Si}`$ (section 4.4) where the diminution of pseudogap in $`\beta \mathrm{Al}_9\mathrm{Mn}_{1.5}\mathrm{Cu}_{1.5}\mathrm{Si}`$ sp DOS (figure 6(b)) with respect to $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ sp DOS (figure 4(a)), corresponds to reduction of $`(|^{}|)`$ (figure 8).

### 6.3 Origin of the Vacancy

For structures containing serveral Mn Wyckoff sites, the TM-TM pair interaction mediated by conduction states allows one to compare the relative stability of TM atoms on different Wyckoff sites. Considering a phase with a structural energy of the TM sub-lattice equal to $``$, the variation, $`\mathrm{\Delta }_i`$, of $``$ is determined when one TM(i) atom is removed from the structure:

$`\mathrm{\Delta }_i={\displaystyle \underset{j(ji)}{}}\mathrm{\Phi }_{TM\text{-}TM}(r_{ij})e^{\frac{r_{ij}}{L}}.`$ (11)
TM atoms on different Wyckoff sites have different $`\mathrm{\Delta }_i`$ values that can be compared. The most stable Mn sites correspond to highest $`\mathrm{\Delta }_i`$ values. Moreover, the energy reference is a TM imputity in the Al(Si) matrix which does not depend on the structure. Therefore, it is possible to compare $`\mathrm{\Delta }_i`$ calculated for different structures. As previously, the energy $`\mathrm{\Delta }_i^{}`$ is calculated from equation (11) without the first-neighbour TM-TM contributions in order to analyse effects at medium range order.

Considering the hypothetical $`\beta \mathrm{Al}_9\mathrm{Mn}_4\mathrm{Si}`$ builted from $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ in which a Mn atom (Mn(0)) replaces a vacancy (Va) in (2d), it appears that $`\mathrm{\Delta }_{Mn(1)}^{}>\mathrm{\Delta }_{Mn(0)}^{}`$ (figure 9). Mn(0) in (2d) is therefore less stable than Mn in (6h) for hypothetical $`\beta \mathrm{Al}_9\mathrm{Mn}_4\mathrm{Si}`$, thus justifying that a vacancy exists in $`\beta `$ phase. A similar result was obtained for $`\phi \mathrm{Al}_{10}\mathrm{Mn}_3`$.

On opposite, for complex crystals $`\mu \mathrm{Al}_{4.12}\mathrm{Mn}`$  and $`\lambda \mathrm{Al}_4\mathrm{Mn}`$  containing a Mn site (Mn(1) in Refs ) with similar local environment as Va (or Mn(0)) in $`\beta `$ structure (section 3.2), the corresponding $`\mathrm{\Delta }_i^{}`$ values differs strongly from those of Mn(0) in hypothetical $`\beta \mathrm{Al}_9\mathrm{Mn}_4\mathrm{Si}`$. Thus Mn(1) in $`\mu `$ and $`\lambda `$ are more stable than an additional Mn atom replacing the vacancy in $`\beta `$ and $`\phi `$. Moreover, both $`\mathrm{\Delta }_{Mn(1)}^{}`$ in $`\mu `$ and $`\lambda `$ have the same order of magnitude as the $`\mathrm{\Delta }_i^{}`$ calculated for other Mn(i) atoms in $`\mu `$ and $`\lambda `$ ($`\mu `$ and $`\lambda `$ phases contain 10 and 15 Mn Wyckoff sites respectively ). Thus Mn(1) in $`\mu `$ and $`\lambda `$ is stable. Such a difference between $`\beta `$, $`\phi `$ and $`\mu `$, $`\lambda `$ can be interpreted in terms of medium range Mn-Mn distances with respect to the curve of figure 7: In $`\beta `$, $`\phi `$ phases, environment of Va contains two Mn at distance 3.8 Å (table 2), whereas the smallest Mn(1)-Mn distance is 4.8 Å in $`\mu `$ and $`\lambda `$ phases. 3.8 Å corresponds to an unstable Mn-Mn distance whereas 4.8 Å corresponds to a stable one (figure 7).

For $`\mathrm{Al}_5\mathrm{Co}_2`$ phase almost isomorphic of $`\beta `$ and $`\phi `$ phases, there is a Co site (Co(0)) corresponding to the vacancy of $`\beta `$ and $`\phi `$ (table 1). In this case $`\mathrm{\Delta }_{Co(0)}^{}`$, calculated with a Co-Co pair interaction, is almost equal to $`\mathrm{\Delta }_{Co(1)}^{}`$ (figure 10). As Co(0) in (2d) is as stable as Co(1) in (6h), it justifies why any vacancy does not exist in $`\mathrm{Al}_5\mathrm{Co}_2`$.

The present anaylsis on the origin of the vacancy in terms of TM-TM medium range interactions confirms the LMTO results (section 4.4). It shows the importance of TM-TM medium range indirect interaction on the atomic structure.

## 7  Magnetic properties

The presence of localised magnetic moments in quasicrystals and related phases containing Mn is much debated . Vacancies, Mn pairs, triplets, quadruplets, quintuplets, variation of first-neighbour distances around Mn are often invoked to explain magnetic moments . But in previous work , it has been shown that an extreme sensitivity of magnetic properties also comes from an effect of an indirect Mn-Mn interaction mediated by sp states. Consequently an analysis limited to first-neighbour environments is not sufficient to interpret magnetic properties.

The unit cell of $`\beta `$ and $`\phi `$ phases contains two Mn-triplets distant each other from from about $`5\mathrm{\AA }`$, and experimental measurements indicate that Mn-triplets are non-magnetic . LMTO electronic structures calculated with polarised spin confirms that Mn triplets are non-magnetic in $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ and $`\phi \mathrm{Al}_{10}\mathrm{Mn}`$. But from polarised spin LMTO calculation, performed on $`\beta \mathrm{Al}_9\mathrm{Mn}_{1.5}\mathrm{Cu}_{1.5}\mathrm{Si}`$ phase where a Cu-triplet replaces one Mn-triplet in each cell (section 4.4$`(iii)`$ and table 3), a magnetic moment equal to $`1\mu _\mathrm{B}`$ was found on each Mn in $`\beta \mathrm{Al}_9\mathrm{Mn}_{1.5}\mathrm{Cu}_{1.5}\mathrm{Si}`$ (i.e. 3 Mn in Mn-triplet are almost equivalent with a ferromagnetic spin orientation). The energy of formation of magnetic moments in $`\beta \mathrm{Al}_9\mathrm{Mn}_{1.5}\mathrm{Cu}_{1.5}\mathrm{Si}`$ is $`0.046\mathrm{eV}`$ per triplet. The Cu has no long range interaction as its d orbitals are full. Thus a medium range Mn-Mn interaction holds Mn-triplets in non-magnetic state whereas a Mn-triplet impurity in Al should be magnetic. It proves that a magnetic state of a Mn atom is very sensitive to surrounding Mn atoms at a medium range distance up to $`4.17\mathrm{\AA }`$ (table 3). The model of the spin polarised Mn-Mn interaction presented in Ref.  is in agreement with this LMTO result.

As explain in the literature , the occurrence of magnetic Mn can be related to a reduction of pseudogap in the local Mn paramagnetic DOS in $`\beta \mathrm{Al}_9\mathrm{Mn}_{1.5}\mathrm{Cu}_{1.5}\mathrm{Si}`$ (figure 6(c)) by comparison with the local Mn DOS in $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ (figure 3). However, the present study shows that a pseudogap in paramagnetic Mn DOS does not only depend on the local environment of Mn as it is also very sensitive to Mn-Mn medium range interaction (sections 4.4$`(iii)`$, 5.2 and 6.2).

## 8 Conclusion

From first-principles calculations combined with a model hamiltonian approach, it is shown that a detailed analysis of the electronic structure allows one to explain the following features of $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ and $`\phi \mathrm{Al}_{10}\mathrm{Mn}_3`$ structures:

* The small amount of Si in $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ stabilises its structure due to a shift of the Fermi energy toward the minimum of the pseudogap in the DOS. An ab initio study shows that, at 0 Kelvin, Si atoms are on a Wyckoff site different of those for Al atoms.
* $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ and $`\phi \mathrm{Al}_{10}\mathrm{Mn}_3`$ are sp-d Hume-Rothery phases. The transition metal (TM) elements have a crucial effect as sp electrons are scattered by an effective Bragg potential dominated by the effect of the Mn sub-lattice. Such a Bragg potential relates to an indirect Mn-Mn interaction which has a strong magnitude up to $`5\mathrm{\AA }`$ and more.
* An analysis in terms of medium range TM-TM interactions gives theoretical arguments to understand the origin of a large vacancy existing in $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ and $`\phi \mathrm{Al}_{10}\mathrm{Mn}_3`$, whereas similar sites are occupied by Mn in $`\mu \mathrm{Al}_{4.12}\mathrm{Mn}`$ and $`\lambda \mathrm{Al}_4\mathrm{Mn}`$, and by Co in $`\mathrm{Al}_5\mathrm{Co}_2`$.

Finally, in $`\beta \mathrm{Al}_9\mathrm{Mn}_3\mathrm{Si}`$ and $`\phi \mathrm{Al}_{10}\mathrm{Mn}_3`$, the Hume-Rothery minimization of band energy leads to a “frustration” mechanism which favours a complex atomic structure. The Mn sub-lattice appears to be the skeleton of the stucture via a medium range indirect interactions between Mn atoms in the Al matrix. As $`\beta `$ and $`\phi `$ structures are related to those of quasicrystals, it suggests that Hume-Rothery stabilisation, expressed in terms of Mn-Mn interactions, is intrinsically linked to the emergence of quasiperiodic structures in Al(Si)-Mn systems.

## Acknowledgments

I am very grateful to D. Mayou with whom many ideas of this work have been developed. I thank also F. Hippert, D. Nguyen-Manh, R. Bellissent, V. Simonet and J. J. Préjean for fruitful discusions. My thanks to M. Audier from stimulating discussions and carefull reading of this paper.

## References


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# On the Dual Cascade in Two-Dimensional Turbulence

## 1 Introduction

Since Kraichnan , Batchelor , and Leith  (referred to as KLB) adapted Kolmogorov’s theory of self-similarity in three-dimensional turbulence to two-dimensional (2D) fluids, the conventional wisdom for decades has been that 2D turbulence simultaneously exhibits a direct cascade of enstrophy to large wavenumbers, up to a dissipation wavenumber $`k_\nu `$, and an inverse cascade of energy to small wavenumbers, down to wavenumber $`k=0`$. In the limit of small viscosity, the inverse cascade is thought to proceed indefinitely in time to ever-larger scales, transferring virtually all of the energy input to wavenumber zero. The direct cascade is thought to come into balance with viscosity, transferring virtually all of the enstrophy input to $`k_\nu `$, where it will then be dissipated. In the long-time limit, a quasi-steady state is reached, in which two inertial ranges are established. According to the KLB theory, the energy range, which is only quasi-steady, scales as $`k^{5/3}`$. The enstrophy range, which is in absolute equilibrium, should scale as $`k^3`$.

The idea of a dual cascade was first suggested by Fjørtoft , who examined nonlinear transfer by individual interacting wavenumber triads. A later study by Merilees and Warn  provides more quantitative detail. They showed that roughly 70% (60%) of triads containing a given intermediate wavenumber $`k`$ predominantly exchange energy (enstrophy) with lower (higher) wavenumbers. These analyses of nonlinear transfer, although carried out at the triad level, provide only a necessary basis for the KLB theory. The theory requires all triads to work collectively such that virtually all of the energy (enstrophy) input gets transferred to the large (small) scales; this is neither suggested nor implied by . Nevertheless, a dual cascade from a spectrally localized initial spectrum is consistent with  and has been well confirmed by numerical simulations with various resolutions (e.g. Borue ; Frisch and Sulem ; Lilly ; Smith and Yakhot ). In particular, the inverse energy cascade is observed in the laboratory experiments of Dubos et al.  and Paret and Tabeling .111The inverse energy cascade and the $`k^{5/3}`$ range are also seen to be robust in many numerical simulations, at least until the energy reaches the lower spectral boundary; however, the evidence for a direct enstrophy cascade is inconclusive (see the discussion in Paret and Tabeling  and references therein). What has not been established beyond doubt is the realization of the inertial spectral scaling $`k^3`$. In fact, there exist other theories that propose very different spectral slopes (Moffatt ; Saffman ; Sulem and Frisch ).

Numerical simulations, aiming to verify the KLB picture, face a number of formidable tasks. First, the simulations are performed for fluids in a rectangular box instead of an infinite domain. This turns out to be a serious shortcoming, as the equilibrium dynamics of a fluid in a doubly periodic domain differs considerably from that of an unbounded fluid in the KLB picture (see Constantin, Foias, and Manley ; Tran and Shepherd ). In particular, the $`k^3`$ range and the direct enstrophy cascade have been shown to be unrealizable in a bounded domain. The main reason seems to be that in the bounded case, where an absolute equilibrium will be reached, there is no analogue of a persistent upscale flow of energy that eventually evades viscous dissipation altogether. To mimic the inverse cascade, one needs to introduce a dissipation that removes energy at the large scales (cf. ). Linear Ekman drag (proportional to $`k^0`$ and restricted to a few low wavenumbers) and inverse viscosity ($`\nu _\mu k^{2\mu }`$, with $`\mu <0`$) have often been used for that purpose. Unfortunately, the inverse energy cascade, subject to this large-scale dissipation, carries with it a significant fraction of the enstrophy (in contrast to the asymptotic KLB inverse cascade, which carries no enstrophy). Moreover, there is no guarantee that the large-scale dissipation will absorb virtually all of the energy input. This is crucial in the KLB picture, as any fraction of the energy input that gets reflected would ultimately be trapped in the inertial ranges. The trapped energy, being in a virtually inviscid region, would then considerably change the dynamics and the slopes of the inertial ranges. Second, testing the theory requires the achievement of high Reynolds numbers, but current computers are only able to resolve relatively low Reynolds numbers. To overcome these resolution limitations, researchers often resort to introducing a hyperviscosity $`\nu _\mu k^{2\mu }`$, where the degree of viscosity $`\mu `$ is greater than one. This numerical device helps to compress the dissipation range, allowing simulations to be performed at relatively low resolutions. It is hoped that the effect of this modification on the inertial-range dynamics is negligible. However, a significant dissipation of energy at the small scales is inevitable in all numerical schemes.

In this study, we establish a theoretical basis highlighting the dynamical differences between bounded and unbounded 2D turbulence. The consequences for numerical simulations that aim to verify the KLB theory will be addressed. In particular, we argue that instead of the familiar inertial-range spectral scalings $`k^{5/3}`$ and $`k^3`$ conjectured by KLB, one would expect steeper scalings, such as $`k^3`$ and $`k^5`$, respectively, in these ranges for bounded systems in equilibrium. In fact, it is shown in  that the enstrophy range must be steeper than $`k^5`$; the physical implication is that no direct enstrophy cascade is possible. This result is easily generalized, using the Poincaré inequality, to turbulence in semi-unbounded 2D fluids, i.e. fluids confined to unbounded channels with a periodic boundary condition in the across-channel direction. Moreover, we investigate the effectiveness of using a large-scale dissipation to obtain a dual cascade in a bounded fluid. This information should be particularly useful for numerical simulations.

In Section 2, we summarize the KLB theory and contrast it to the dynamics of a bounded fluid. We also show that the theory does not apply to a fluid in an infinite channel with a periodic boundary condition in the across-channel direction. In Section 3, we review a result in  related to the unrealizability of a direct enstrophy cascade and discuss the fundamental differences between the dynamics of bounded fluids in equilibrium and that of unbounded fluids (or bounded fluids in transient phase) in the KLB picture. In Section 4, we derive a new constraint on the spectral slope of the energy range for bounded fluids in equilibrium and a condition for a persistent inverse energy cascade for unbounded fluids. In Section 5, we point out some effects of including a large-scale dissipation and the implications for numerical simulations attempting to verify the KLB picture. We conclude with some remarks in the final section. Further estimates on spectral slopes are given in the appendices.

## 2 KLB picture for unbounded 2D fluids

The evolution of the ensemble-averaged energy spectrum $`E(k)`$, which represents the energy density associated with the wavenumber $`k`$, is governed by (see Frisch  and Kraichnan )

$`{\displaystyle \frac{d}{dt}}E(k)`$ $`=`$ $`T(k)2\nu k^2E(k)+F(k).`$ (1)
Here $`T(k)`$ and $`F(k)`$ are, respectively, the ensemble-averaged energy transfer and energy input rate and $`\nu `$ is the kinematic viscosity coefficient. Since waves of the same scale do not nonlinearly interact, $`T(k)`$ is linear in the modal component corresponding to wavenumber $`k`$. Moreover, $`T(k)`$ satisfies, by virtue of energy and enstrophy conservation,

$`{\displaystyle _0^{\mathrm{}}}T(k)𝑑k`$ $`=`$ $`{\displaystyle _0^{\mathrm{}}}k^2T(k)𝑑k=0.`$ (2)
For a fluid in a doubly periodic domain, which for convenience we call a bounded fluid, the integral in (2) and elsewhere in this section should be replaced by a discrete sum over all wavenumbers. This constraint on $`T(k)`$ imposes certain restrictions on its distribution and is thought to give rise to the dual cascade, believed to be a distinct feature of 2D turbulence.

We multiply (1) by $`k^2`$ and integrate both the original and resulting equations over all wavenumbers, noting from (2) that the nonlinear terms drop out, to obtain evolution equations for the total energy density $`E=_0^{\mathrm{}}E(k)𝑑k`$ and enstrophy density $`Z=_0^{\mathrm{}}k^2E(k)𝑑k`$,

$`{\displaystyle \frac{d}{dt}}E`$ $`=`$ $`2\nu Z+ϵ,`$ (3)
$`{\displaystyle \frac{d}{dt}}Z`$ $`=`$ $`2\nu P+\eta ,`$ (4)
in terms of the energy and enstrophy injection rates $`ϵ=_0^{\mathrm{}}F(k)𝑑k`$ and $`\eta =_0^{\mathrm{}}k^2F(k)𝑑k`$, respectively, and the palinstrophy density $`P=_0^{\mathrm{}}k^4E(k)𝑑k`$. We assume that the forcing is spectrally localized to a wavenumber interval $`[k_{\mathrm{min}},k_{\mathrm{max}}]`$ in the sense that

$`0k_{\mathrm{min}}^2ϵ\eta k_{\mathrm{max}}^2ϵ.`$ (5)
This hypothesis is employed in . This is a classical (although not exclusive) scenario for the KLB theory (cf. Kraichnan , p. 1421b; Pouquet et al. , p. 314; and Lesieur , p. 291), and is furthermore a common setup in numerical simulations of forced 2D turbulence (cf. Lilly ; Basdevant et al. ; Shepherd ). This assumption seems plausible for time-independent or white-noise forcing over $`[k_{\mathrm{min}},k_{\mathrm{max}}]`$, given the assemble-averaged nature of $`ϵ`$ and $`\eta `$. In particular, a monoscale forcing at a wavenumber $`s`$ satisfies (5) with $`k_{\mathrm{min}}=k_{\mathrm{max}}=s`$ for each individual realization. Another example of such a forcing over $`[k_{\mathrm{min}},k_{\mathrm{max}}]`$ is described in ; in each realization it yields time-independent energy and enstrophy injection rates $`ϵ`$ and $`\eta `$ such that $`\eta =s^2ϵ`$, where $`s^2`$ is the mean of $`k^2`$ over $`[k_{\mathrm{min}},k_{\mathrm{max}}]`$. A similar forcing was used by Shepherd  in a study of 2D turbulence in a large-scale zonal jet on the so-called beta-plane. In these examples, the characteristic forcing wavenumber $`s`$ is constant in time.

The dual cascade scenario can be best appreciated if one examines the evolution equation

$`s^2{\displaystyle \frac{d}{dt}}E{\displaystyle \frac{d}{dt}}Z`$ $`=`$ $`2\nu (Ps^2Z),`$ (6)
obtained from (3) and (4). Here $`s`$ is the forcing wavenumber $`\sqrt{\eta /ϵ}`$ (for $`ϵ>0`$), which according to hypothesis (5), must lie in the interval $`[k_{\mathrm{min}},k_{\mathrm{max}}]`$. If $`ϵ=0`$, then $`\eta =0`$ and we take $`s`$ to be any wavenumber in $`[k_{\mathrm{min}},k_{\mathrm{max}}]`$. A direct enstrophy cascade requires that the characteristic enstrophy dissipation wavenumber $`\sqrt{P/Z}`$ be much larger than the forcing wavenumber $`s`$; hence, the right-hand side of (6) must be positive. The positiveness of $`Ps^2Z`$ implies the positiveness of the left-hand side of (6) as well. If, in accord with the quasi-steady KLB theory, the total enstrophy reaches a steady state, we deduce that $`dE/dt`$ must be positive. Equation (6) reflects the fact that the total energy must increase without limit, due to the inverse energy cascade toward wavenumber zero. (In a bounded domain, Tran and Shepherd  showed that $`P=s^2Z`$ and concluded from this that no direct cascade is possible.)

Equation (6) satisfies $`P/Zs^2`$ not only for the KLB scaling $`k^{5/3}`$ and $`k^3`$ but also for a rich variety of spectra. This condition only requires an energy spectrum shallower than $`k^5`$ for a sufficiently wide range of wavenumbers $`k>s`$, provided that the energy spectrum for $`ks`$ is shallower than $`k^3`$. (In Section 4, it is shown that the quantity $`Ps^2Z`$ can be positive even if the energy spectrum for $`k>s`$ is steeper than $`k^5`$. This allows for the possibility of an inverse energy cascade in the absence of a direct enstrophy cascade.) However, the KLB theory insists on the specific scalings $`k^{5/3}`$ and $`k^3`$ (with a logarithmic correction proposed by Kraichnan  and further investigated by Bowman ), respectively, for the energy and enstrophy inertial ranges. The $`k^{5/3}`$ scaling is analogous to the Kolmogorov spectrum for 3D turbulence; the $`k^3`$ scaling implies that successive octaves in the enstrophy range contain equal amounts of enstrophy, so that the enstrophy grows logarithmically with dissipation wavenumber $`k_\nu `$. There exist a number of predictions for the numerical value of the enstrophy inertial range slope $`\beta `$ in the literature. Saffman  proposes $`\beta =4`$, while Moffat  favours a slightly smaller value: $`\beta =11/3`$. Sulem and Frisch  instead propose the upper bound $`\beta 11/3`$.

In the long-time limit, the KLB inverse energy cascade (or any inverse energy cascade with a spectral scaling shallower than $`k^3`$ near $`k=0`$) carries no enstrophy with it. Therefore, the enstrophy necessarily approaches an absolute equilibrium in a quasi-steady state. As a consequence, (6) reduces to

$`s^2{\displaystyle \frac{d}{dt}}E`$ $`=`$ $`2\nu (Ps^2Z).`$ (7)
This equation indicates a simple and interesting fact about the KLB theory for unbounded 2D turbulence: in a quasi-steady state (for which $`dZ/dt=0`$), the strength of an inverse energy cascade (the rate of the energy growth), if realizable, is primarily determined by the rate $`2\nu P`$ of enstrophy dissipation.

Besides the simultaneous conservation of energy and enstrophy, other essential features of 2D turbulence that underly the KLB theory are the scale-selectivity of the molecular viscosity and the unboundedness of the domain (in both directions). Together, they give rise to an infinite reservoir of energy in the vicinity of $`k=0`$ that allows for the possibility of the KLB inverse energy cascade (which contains no enstrophy if the spectrum near $`k=0`$ is shallower than $`k^3`$). The theory breaks down when either the scale-selectivity of the dissipation or the unboundedness of the domain is absent. We demonstrate the former case and the semi-bounded case below. The case of a fluid in a doubly periodic domain is studied in  and will be reviewed in the next section.

Consider (1) with the viscous dissipation term $`\nu k^2`$ replaced by a constant $`\sigma >0`$; this scale-neutral frictional dissipation is often called Ekman drag in geophysical contexts. Equations (3) and (4) become

$`{\displaystyle \frac{d}{dt}}E`$ $`=`$ $`2\sigma E+ϵ,`$ (8)
$`{\displaystyle \frac{d}{dt}}Z`$ $`=`$ $`2\sigma Z+\eta ,`$ (9)
which, for bounded injection rates $`ϵ`$ and $`\eta `$, implies that both the energy and enstrophy are bounded. This simple fact precludes the KLB type of inverse energy cascade. (As argued below, an inverse energy cascade dissipated by the friction at the large scales is not possible either.) Moreover, upon applying (5), we find

$`{\displaystyle \frac{d}{dt}}(k_{\mathrm{min}}^2EZ)`$ $``$ $`2\sigma (k_{\mathrm{min}}^2EZ),`$ (10)
$`{\displaystyle \frac{d}{dt}}(k_{\mathrm{max}}^2EZ)`$ $``$ $`2\sigma (k_{\mathrm{max}}^2EZ).`$ (11)
Hence, in the limit $`t\mathrm{}`$ the following holds

$`k_{\mathrm{min}}^2EZ0k_{\mathrm{max}}^2EZ,`$ (12)
or equivalently,

$`k_{\mathrm{min}}^2{\displaystyle \frac{Z}{E}}k_{\mathrm{max}}^2.`$ (13)
Equation (13) implies that the redistribution of energy and enstrophy obeys exactly the same constraint as that imposed on the energy and enstrophy injection rates. Now, the boundedness of energy (enstrophy) prohibits an infinitely wide range of wavenumbers $`k<k_{\mathrm{min}}`$ ($`k>k_{\mathrm{max}}`$) in which the energy spectrum can scale as $`k^1`$ ($`k^3`$), as this would imply a logarithmic divergence of the energy (enstrophy) as $`k0`$ ($`k\mathrm{}`$). In fact, an energy spectrum $`k^1`$ ($`k^3`$) or steeper (shallower) on the large (small) scales is inconsistent with (13). Spectra consistent with (13) require that the energy and enstrophy be primarily dissipated near the region of forcing; hence no inverse (direct) energy (enstrophy) cascade is possible.

Besides the boundedness of the energy density in the present case, the spectral distribution of energy and enstrophy obeying (13) is profoundly different from that of the classical picture. The energy range is seen to be much shallower than $`k^{5/3}`$ for a friction that acts uniformly on all scales. What seems curious is that the slopes of the enstrophy range in both cases do not differ by much. In fact, one could argue that a $`k^3`$ enstrophy-range spectrum with a logarithmic correction is consistent with the constraint (13), provided that the spectrum in the energy range scales as $`k^1`$ (with a similar correction). Nevertheless, we see that the scale-selectivity of the molecular viscosity plays an important role in the dual cascade picture. Perhaps, instead of studying the 2D Navier–Stokes dual cascade, one could replace the molecular dissipation $`\nu k^2`$ in (1) by another scale-selective dissipation $`\nu _\mu k^{2\mu }`$ (with $`\mu >0`$) and examine the realizability of a dual cascade in this hypothetical unbounded system.

Finally, it is interesting to note that the KLB picture is not realizable for a 2D Navier–Stokes fluid confined to an unbounded channel with a periodic boundary condition in the across-channel direction ($`0yL`$) and vanishing velocity (and derivatives thereof) at $`x=\pm \mathrm{}`$. This system is also furnished with the zero-mean flow condition

$`{\displaystyle _0^L}𝒖(x,y,t)𝑑y`$ $`=`$ $`\mathrm{𝟎},`$ (14)
where $`𝒖(x,y,t)`$ is the fluid velocity. To see why the dynamics of this system are incompatible with the KLB picture, consider the Poincaré inequality for this domain: there exists a constant $`\lambda >0`$ such that

$`\lambda {\displaystyle _0^{\mathrm{}}}k^\mu E(k)𝑑k`$ $``$ $`{\displaystyle _0^{\mathrm{}}}k^{2+\mu }E(k)𝑑k,`$ (15)
where $`\mu 0`$. The optimal value of the constant $`\lambda `$ depends on $`L`$. Now, the energy equation (3) and enstrophy equation (4) can be bounded via (15) as follows

$`{\displaystyle \frac{d}{dt}}E`$ $``$ $`2\nu \lambda E+ϵ,`$ (16)
$`{\displaystyle \frac{d}{dt}}Z`$ $``$ $`2\nu \lambda Z+\eta .`$ (17)
These inequalities render the boundedness of both energy and enstrophy. The boundedness of the energy rules out the persistent inverse cascade needed for the positiveness of $`Ps^2Z`$; rather, an absolute equilibrium is more plausible for this system. This result is quite physically reasonable: if one visualizes the inverse cascade as a result of the coalescence of same-sign vortices to form ever-larger ones, the system will tend toward equilibrium as the radii of the vortices approach the channel width $`L`$. This dynamical behaviour is observed by Rutgers  in an experiment of turbulence in a long channel, where, as equilibrium is approached, the vortices grow until the channel width is reached.

Now, if an equilibrium is achieved, (6) necessarily reduces to

$`Ps^2Z`$ $`=`$ $`0.`$ (18)
This equation, which also applies to the case of bounded fluids in equilibrium considered in the next section, implies that the dissipation of enstrophy mainly occurs in the forcing region and admits much steeper spectra than the KLB spectrum.

Remark 1. Some theoretical studies of the 2D Navier–Stokes equations in unbounded domains make an a priori assumption that the Poincaré inequality holds (e.g. Rosa ; see also Temam , p. 307). Such studies automatically exclude the possibility of the KLB dynamics.

## 3 Dynamics of bounded fluids in equilibrium

In bounded systems, the energy is also in absolute equilibrium for arbitrary (but positive) viscosity coefficient $`\nu `$, so that (18) holds in equilibrium. This implies that $`P/Z=s^2`$, ruling out the existence of an enstrophy inertial range, as argued in . Moreover, the energy spectrum for $`k>k_{\mathrm{max}}`$ is steeper than $`k^5`$. This constraint clearly indicates a dramatic departure from the KLB theory. It is consistent with numerous numerical results, in which large-scale vortices, known as coherent structures, are observed (see for example Borue ; McWilliams ; Santangelo, Benzi, and Legras ; Smith and Yakhot ); these are often blamed for causing spectra steeper than those predicted by KLB. Although the mechanism behind these structures is not fully understood, we argue that it is the steepness of the spectrum (steeper than $`k^5`$) that allows coherent structures to form, rather than the other way around. There is no need to invoke coherent structures to explain steep spectra: the steepness arises merely as a consequence of global conservation laws, molecular viscosity, and a spectrally localized forcing. As a matter of fact, a small-scale spectrum steeper than $`k^5`$ implies that the large scales carry virtually all of the system’s enstrophy. Hence, dynamics exhibiting strong large-scale structures on a much weaker turbulent background of noise are consistent with . It should be noted that the small-scale spectrum only needs to be steeper than $`k^3`$ for most of the enstrophy to reside in the large scales. Hence, large-scale structures may also be observed in simulations where a slope between $`3`$ and $`5`$ in the enstrophy range can be achieved, using a large-scale dissipation (see next section). Also, if the spectrum on the large scales is shallower than $`k^3`$, one may expect vortices comparable in size to the forcing scale to form, because most of the system’s enstrophy is then distributed in that spectral region. This has previously been noted by Paret and Tabeling .

In Section 4, we show that (18), which may be rewritten as

$`{\displaystyle \underset{k<s}{}}(s^2k^2)k^2E(k)`$ $`=`$ $`{\displaystyle \underset{k>s}{}}(k^2s^2)k^2E(k),`$ (19)
implies the spectral exponents satisfy $`\beta >5`$ and $`\alpha +\beta 8`$, where $`\alpha `$ ($`\beta `$) is the asymptotic slope of the range of wavenumbers lower (higher) than the forcing wavenumber (in the usual case where the forcing wavenumber is no greater than the geometric mean of the integral and dissipation wavenumbers). For example, if the small-scale spectrum is approximately $`k^5`$, then the large-scale spectrum should scale as $`k^3`$. This would be consistent with the observed $`k^3`$ spectrum for the large-scale dynamics of the atmosphere (Lilly ). Now, a large-scale $`k^3`$ spectrum means that the enstrophy scales as $`k^1`$; each octave in this range contains approximately the same amount of enstrophy. Therefore, the dissipation of energy is uniformly distributed among successive octaves in the energy range, so that no inverse energy cascade is possible. Nevertheless, a spectrum steeper than $`k^3`$ on the large scales is allowed by (19). This is more likely to occur if the small-scale spectrum is only marginally steeper than $`k^5`$ (see Section 4). Unlike the KLB inverse cascade, which carries virtually all of the injected energy to ever-larger scales, this inverse cascade, if realizable, would only carry a fraction of the energy input to the largest scales.

The dynamics of a bounded fluid in equilibrium is characteristically different from the quasi-steady KLB picture. There is an infinite energy reservoir at $`k=0`$ in unbounded systems that is forever available to collect the energy transfer; this feature is absent in bounded fluids (and in unbounded fluids satisfying the Poincaré inequality). Hence, the departure should not come as a surprise. What seems ironic is that the enstrophy is only weakly dissipated in bounded fluids at high Reynolds numbers but strongly dissipated in the unbounded KLB case: in the bounded case the result $`P/Z=s^2`$  implies that the enstrophy dissipation rate $`2\nu P/Z`$ becomes $`2\nu s^2`$, while in the KLB theory it is approximately $`\nu k_\nu ^2/\mathrm{ln}(k_\nu /s)`$, which is much greater than $`2\nu s^2`$ since $`k_\nu s`$.

There appears to be no simple generalization from the dynamics of a bounded fluid in absolute equilibrium to that of its unbounded classical counterpart and vice versa. The familiar reconciliation found in the literature is that the $`k^{5/3}`$ range is modified or disrupted at the large scales when the inverse cascade reaches the lowest available wavenumber. If the KLB picture applies to non-equilibrium dynamics in a bounded system, v.z. before the inverse cascade gets reflected by the spectral boundary,222In a finite system, an inverse energy cascade carries a non-negligible amount of enstrophy. If an inverse energy cascade carrying virtually all of the energy input rate $`ϵ`$, reaches a wavenumber $`k_{}`$, it would transfer enstrophy at the rate $`k_{}^2ϵ`$ to wavenumber $`k_{}`$. Hence, the ratio of the enstrophy accompanying the inverse energy cascade to the enstrophy input is approximately given by $`k_{}^2/s^2`$, independent of the viscosity $`\nu `$. then a dramatic adjustment of the spectrum has to occur as an equilibrium is approached (see Smith and Yakhot  for a discussion of the so-called finite-size effects). We have not yet investigated in detail how this adjustment takes place; however, it seems plausible that as the inverse cascade hits the spectral boundary and gradually loses its strength ($`dE/dt0`$), a substantial amount of the energy gets bounced back to the forcing scale. As there is little dissipation at the large scales, growth of the energy spectrum in the energy range is inevitable. This growth proceeds until the large-scale energy spectrum is sufficiently excited so that the enstrophy dissipation occurs mainly in the vicinity of the forcing scale, whereupon a forced-dissipative equilibrium is reached. As $`dE/dt0`$, the enstrophy cascade (if initially present) ceases since the quantity $`Ps^2Z`$ on the right-hand side of (6) decreases to zero. As a consequence, a gradual steepening of the enstrophy-range spectrum takes place (whatever the spectral slope of the enstrophy range during the transient phase). In Section 4 and Appendix A, we establish that the sum of the steady-state spectral exponents in the energy and enstrophy ranges must asymptotically approach $`8`$.

Remark 2. It should be emphasized that the possibility of a direct enstrophy cascade in a bounded fluid during the non-equilibrium phase cannot be ruled out (not to say, however, that it actually occurs). For the case of a monoscale time-independent forcing, it is shown in Tran and Shepherd  that a direct enstrophy cascade is not realizable on average, whether the average be taken on a chaotic trajectory, limit cycle, or on the entire global attractor. This result leaves only the possibility of a direct enstrophy cascade in a neighborhood of the resulting monoscale stationary solution, on its unstable manifold. In this region one simultaneously has $`Ps^2Z>0`$ and $`s^2EZ>0`$ (see Tran and Shepherd  and also Tran, Shepherd, and Cho ); the former inequality prevents one from ruling out a direct enstrophy cascade. More quantitative determination of the quantity $`Ps^2Z`$ (which is viscosity-dependent, see ) in this region will help assess the existence of the enstrophy cascade (and how this would depend on the viscosity) as a monoscale basic flow loses its stability.

It is interesting to note that a $`k^3`$ spectrum (or slightly steeper), subject to experimental error, is observed in the laboratory experiments of Paret, Jullien, and Tabeling , and Rutgers . In these experiments, mechanical friction at the bottom and top boundaries (in particular with the air, as noted in ) of the fluid could be sufficiently strong to outplay viscosity, so that Ekman drag alone is essentially responsible for dissipation. This might explain the observed spectra, according to the discussion in the previous section. Moreover, the analysis of  suggests that a combination of strong Ekman drag and weak viscosity allows for such a shallow spectrum to be realizable. Thus, there is no contradiction between the observed spectra and the predicted $`k^5`$ spectrum for a Navier–Stokes fluid in equilibrium.

## 4 Constraints on constant spectral slopes

We now derive constraints on the spectral slopes for bounded fluids in equilibrium and for a dual cascade in unbounded fluids, particularly for a persistent inverse energy cascade. We assume that the quasi-steady (steady) spectrum for the unbounded (bounded) case can be approximated by

$`E(k)`$ $`=`$ $`\{\begin{array}{cc}ak^\alpha \hfill & \text{if }k_0<k<s\text{,}\hfill \\ bk^\beta \hfill & \text{if }s<k<k_\nu \text{,}\hfill \end{array}`$ (20)
where $`a,b,\alpha ,\beta `$ are constants, $`k_0`$ is the lowest wavenumber in the energy range ($`k_00`$ as $`t\mathrm{}`$ for the unbounded case), and $`k_\nu `$ is the highest wavenumber in the enstrophy range, beyond which the spectrum is supposed to be steeper than $`k^\beta `$. In Appendix A, we show that the arguments below can even be extended to the more realistic case, where the inertial-range slopes depend on wavenumber.

The quantity $`Ps^2Z`$ can then be estimated as

$`{\displaystyle _{k_0}^{\mathrm{}}}(k^2s^2)k^2E(k)𝑑k`$ $``$ $`a{\displaystyle _{k_0}^s}(k^2s^2)k^{2\alpha }𝑑k+b{\displaystyle _s^{k_\nu }}(k^2s^2)k^{2\beta }𝑑k`$
$`=`$ $`as^{5\alpha }{\displaystyle _{k_0/s}^1}(\kappa ^21)\kappa ^{2\alpha }𝑑\kappa +bs^{5\beta }{\displaystyle _{s/k_\nu }^1}(1\kappa ^2)\kappa ^{\beta 6}𝑑\kappa `$
$`=`$ $`as^{5\alpha }\left({\displaystyle _{k_0/s}^1}(1\kappa ^2)\kappa ^{2\alpha }𝑑\kappa +{\displaystyle _{s/k_\nu }^1}(1\kappa ^2)\kappa ^{\beta 6}𝑑\kappa \right),`$
where the inequality results from dropping the spectral contribution beyond $`k_\nu `$ (which is considerable if $`\beta 5`$), the second line is obtained by the respective changes of variables $`\kappa =k/s`$ and $`\kappa =s/k`$ in the two integrals on the right-hand-side of the first line, and the third line is obtained using the continuity relation $`as^\alpha =bs^\beta `$.

In the bounded case the left-hand side of (4) vanishes. Therefore,

$`{\displaystyle _{k_0/s}^1}(1\kappa ^2)\kappa ^{2\alpha }𝑑\kappa `$ $``$ $`{\displaystyle _{s/k_\nu }^1}(1\kappa ^2)\kappa ^{\beta 6}𝑑\kappa .`$ (22)
For a strong forcing at a relatively low wavenumber $`s`$, it is reasonable to assume that $`k_0/ss/k_\nu `$. This requires $`2\alpha \beta 6`$, as the integrals in (22) decrease if the corresponding powers of $`\kappa `$ ($`\beta 6`$ and $`2\alpha `$) increase. That is, $`\alpha +\beta 8.`$

On the other hand, the convergence of the right-hand integral in (22), as $`s/k_\nu 0`$, requires also that $`\beta >5`$. This result was derived in , on the basis that the dissipation of enstrophy mainly occurs in the vicinity of the forcing scale. Now if $`\beta =5+\delta `$, where it may be plausible that $`0<\delta 1`$ for high Reynolds numbers, then $`\alpha 3\delta `$. It thus seems possible to obtain $`\alpha 3`$. In the limits $`k_0/s0`$ and $`s/k_\nu 0`$, as is usual for high-Reynolds-number turbulence, the inequality $`\alpha +\beta 8`$ approaches an equality.

Remark 3. We caution that replacing the molecular viscosity $`\nu k^2`$ by a general viscosity $`\nu _\mu k^{2\mu }`$ ($`\mu 0`$) in the previous argument leads to the result $`\alpha +\beta 4+4\mu `$. The significant dependence on $`\mu `$ of this constraint suggests that the introduction of a hyperviscosity could seriously alter the expected steady-state spectral slopes.

We now derive a condition for a persistent inverse energy cascade in the unbounded case. We assume $`\alpha <3`$, in accord with the realization of an inverse cascade toward wavenumber $`k=0`$ that carries no enstrophy with it. In the limits $`k_0/s0`$ and $`s/k_\nu 0`$, the condition $`Ps^2Z>0`$ is guaranteed if $`2\alpha >\beta 6`$ and $`\alpha <3`$, or equivalently, $`\alpha +\beta <8`$ and $`\alpha <3`$. These constraints admit a variety of spectra for a quasi-steady state in which an inverse energy cascade to wavenumber zero, carrying with it virtually no enstrophy, and a direct enstrophy cascade to the dissipation wavenumber $`k_\nu `$, carrying with it virtually no energy, are allowed. Note that the inverse cascade scenario cannot be ruled out even if $`\beta >5`$, i.e, in the absence of a direct enstrophy cascade, provided that the inequality $`\alpha +\beta <8`$ holds. For the KLB energy-range spectrum $`k^{5/3}`$, it is interesting to note that this condition requires only $`\beta <19/3`$. We therefore suggest that an inverse energy cascade in the absence of a direct enstrophy cascade can be realizable for a wide range of (modest) Reynolds numbers.

Remark 4. If the molecular viscosity $`\nu k^2`$ is replaced by a hyperviscosity $`\nu _\mu k^{2\mu }`$ for $`\mu >1`$ in an unbounded fluid, the condition for a persistent inverse energy cascade $`Ps^2Z>0`$ is replaced by $`_0^{\mathrm{}}(k^2s^2)k^{2\mu }E(k)𝑑k>0`$. This leads to $`\alpha +\beta <4+4\mu `$. Of course, the condition $`\alpha <3`$ is required for a zero-enstrophy-carrying inverse energy cascade.

## 5 Large-scale dissipation

In this section, we examine how a large-scale dissipation could be used to obtain a dual cascade, and in particular, a direct enstrophy cascade. Consider (1) in the bounded case, with a general dissipation:

$`{\displaystyle \frac{d}{dt}}E(k)`$ $`=`$ $`T(k)D(k)E(k)+F(k),`$ (23)
where $`D(k)`$ is a non-negative function of $`k`$. Systems for which $`D(k)`$ vanishes in the intermediate wavenumber range, including the forcing region, and for which the boundedness of energy is not guaranteed (Eyink ) have previously been studied in the literature.

For a general $`D(k)`$, (6) becomes

$`s^2{\displaystyle \frac{d}{dt}}E{\displaystyle \frac{d}{dt}}Z`$ $`=`$ $`{\displaystyle \underset{k}{}}(k^2s^2)D(k)E(k),`$ (24)
which, in equilibrium, reduces to the balance equation

$`{\displaystyle \underset{k}{}}(k^2s^2)D(k)E(k)`$ $`=`$ $`0.`$ (25)
A slightly different form of this equation is derived in . Equation (25) implies that the energy-range spectrum is related to the enstrophy-range spectrum in an intimate manner. For a given $`D(k)`$, an increase of the energy in one range requires an increase of the energy in the other. Thus, a steeper (shallower) energy-range spectrum corresponds to a shallower (steeper) enstrophy-range spectrum, for fixed $`E(s)`$. Another obvious consequence of (18) is that a nontrivial equilibrium is not possible if $`D(k)`$ vanishes for all $`k<s`$.

We are interested in an expression for $`D(k)`$ that retains the usual molecular viscosity and includes a large-scale dissipation. Thus, we consider $`D(k)=D_{\mathrm{}}(k)+2\nu k^2`$, where $`D_{\mathrm{}}(k)`$ is a non-negative function of $`k`$. This dissipation includes the physically relevant case in which $`D_{\mathrm{}}(k)`$ is a positive constant representing friction from the planetary boundary layer in the geophysical context. Equation (25) then becomes

$`2\nu (Ps^2Z)`$ $`=`$ $`{\displaystyle \underset{k}{}}(s^2k^2)D_{\mathrm{}}(k)E(k).`$ (26)
The left-hand side of (26) is the familiar term due to viscosity, which would vanish in the absence of the large-scale dissipation. It can now become positive since the right-hand side can be made positive in a variety of ways. Two popular forms of $`D_{\mathrm{}}(k)`$ used in numerical simulations are the inverse viscosity $`D_{\mathrm{}}(k)=2\nu _\mu k^{2\mu }`$, for $`\mu <0`$, and mechanical friction restricted to the largest scales (say $`k<k_{\mathrm{}}`$): $`D_{\mathrm{}}(k)H(k_{\mathrm{}}k)`$, where $`H(k_{\mathrm{}}k)`$ is the Heaviside step function (see Maltrud and Vallis , for example). To facilitate the formation of an enstrophy cascade, one might try to maximize the right-hand side of (26). However, since we have no a priori control over $`E(k)`$ for different $`D_{\mathrm{}}(k)`$, it is not known how to maximize the product $`D_{\mathrm{}}(k)E(k)`$ for $`k<s`$. Nevertheless, restricting $`D_{\mathrm{}}(k)`$ to $`k<s`$ by setting $`D_{\mathrm{}}(k)=0`$ for $`ks`$ is reasonable since any non-zero contribution to the right-hand side of (26) beyond $`s`$ is negative.

If a positive value for the right-hand side of (26) can be achieved, the quantity $`Ps^2Z`$ will be large for sufficiently small $`\nu `$. This may help break the constraint that the enstrophy range slope must be steeper than $`k^5`$ and allow for a direct enstrophy cascade. An inverse cascade should be realizable, as we expect most of the energy dissipation to occur at the large scales. Thus, a dual cascade is possible. However, this cannot be achieved without a cost, as $`D_{\mathrm{}}(k)`$, which dissipates energy at the rate $`_kD_{\mathrm{}}(k)E(k)`$, also dissipates enstrophy on the large scales at the rate $`_kD_{\mathrm{}}(k)k^2E(k)`$. But

$`k_0^2{\displaystyle \underset{k}{}}D_{\mathrm{}}(k)E(k)`$ $``$ $`{\displaystyle \underset{k}{}}D_{\mathrm{}}(k)k^2E(k),`$ (27)
where $`k_0`$ is the lowest wavenumber corresponding to the system size. Hence, if $`_kD_{\mathrm{}}(k)E(k)`$ is comparable to the energy injection rate (which is ideally sought after in the spirit of the KLB theory), then the ratio of the enstrophy dissipation rate at the large scales to the enstrophy injection rate is greater than $`k_0^2/k_{\mathrm{max}}^2`$. This fraction of the enstrophy dissipation at the large scales may be small, but not negligible. By allowing the enstrophy to be transferred to the large scales, a non-negligible amount of enstrophy may be trapped in the forcing region. If this is the case, then the spectrum in the forcing region has to adjust dramatically (since $`\nu `$ is small and the large-scale dissipation is assumed to be weak around the forcing scale) to balance the trapped enstrophy. In Appendix B, we emphasize the difficulty of obtaining an enstrophy-range spectrum shallower than $`k^5`$ with a large-scale dissipation that is well separated from the forcing region.

Numerical simulations of 2D turbulence can resolve up to a certain wavenumber, say $`k_T`$. Therefore, there is always a finite amount of energy dissipation at the small scales. This is analogous to the dissipation of enstrophy at the large scales previously considered, due to the finite size of the domain. If $`D_h(k)`$ represents the small-scale dissipation coefficient, the enstrophy and energy dissipations on the small scales are respectively given by $`_kD_h(k)k^2E(k)`$ and $`_kD_h(k)E(k)`$. These quantities satisfy

$`{\displaystyle \underset{k}{}}D_h(k)k^2E(k)`$ $``$ $`k_T^2{\displaystyle \underset{k}{}}D_h(k)E(k).`$ (28)
Hence, if the dissipation of enstrophy by $`D_h(k)`$ is comparable to the enstrophy injection rate (which is ideally sought after in the spirit of the KLB theory), then the ratio of the energy dissipation rate at the small scales to the energy injection rate is greater than $`k_{\mathrm{min}}^2/k_T^2`$. This is true for any $`D_h(k)0`$, including a hyperviscosity of arbitrary degree.

Intuitively, if a large-scale dissipation is extended to $`s`$, one would expect it to absorb the reflected energy and keep the spectrum in the forcing region from growing as $`\nu 0`$. For a strong forcing and strong large-scale dissipation $`D_{\mathrm{}}(k)`$ (confined to $`ks`$), it may be hypothesized that the value of the right-hand side of (26) is unaffected as $`\nu 0`$, given all else fixed. If this is the case, the quantity $`Ps^2Z`$ grows as $`\nu ^1`$ and the ratio $`P/Z`$ is given by

$`{\displaystyle \frac{P}{Z}}`$ $`=`$ $`s^2+{\displaystyle \frac{1}{2\nu Z}}{\displaystyle \underset{k}{}}(s^2k^2)D_{\mathrm{}}(k)E(k).`$ (29)
This makes $`P/Z\mathrm{}`$ as $`\nu 0`$, a favorable limit for a direct enstrophy cascade, with a spectrum shallower than $`k^5`$. However, the resulting cascade would not have the physical significance of the KLB theory since the direct enstrophy cascade (regardless of the spectral slope) might only be marginal, with a significant fraction of the enstrophy dissipated in the energy range ($`ks`$) due to the strong large-scale dissipation, contrary to the classical theory.

## 6 CONCLUSION

In this paper we have analysed the classical dual cascade theory of 2D turbulence in unbounded fluids formulated by Kraichnan , Leith , and Batchelor . The main feature of the theory—the dual cascade—is contrasted to the behaviour of 2D turbulence in a region that satisfies the Poincaré inequality, such as a doubly periodic domain. It is shown that the dual cascade picture, if realizable, would strictly be an unbounded-system phenomenon. This important point is not adequately stressed and has often led to confusion in the literature. The familiar qualitative argument that the $`k^{5/3}`$ range is modified or disrupted at the large scales when the inverse energy cascade reaches the largest available scale in a bounded system (assuming the applicability of the dual-cascade dynamics to the transient phase) is inadequate. Two-dimensional turbulence either in a doubly periodic domain or in an unbounded channel with a periodic boundary condition on the across-channel dimension does not behave in the manner predicted by KLB. In particular, the spectral slopes in such systems are found to satisfy $`\beta >5`$ and $`\alpha +\beta 8`$, where $`\alpha `$ ($`\beta `$) is the slope of the range of wavenumbers lower (higher) than the forcing wavenumber. This result is well supported by numerical simulations, which consistently find enstrophy-range spectra steeper than the KLB prediction and dynamically dominant large-scale structures (McWilliams ; Santangelo, Benzi, and Legras ). It may even explain the observed large-scale $`k^3`$ spectrum in the atmosphere (Lilly , Boer and Shepherd ).

We have shown that a dual cascade in unbounded fluids is possible if $`\beta `$ satisfies $`3<\beta <5`$; this includes both the classical $`\beta =3`$ scaling as an extreme limit, and also the theories of Saffman , Moffat , and Sulem and Frisch , which propose $`\beta =4`$, $`\beta =11/3`$, and $`\beta 11/3`$, respectively. Moreover, in the absence of a direct enstrophy cascade ($`\beta >5`$), an inverse energy cascade, corresponding to flows with low Reynolds numbers (which should be relatively easy to simulate) cannot be ruled out.

The fundamental difference between bounded and unbounded fluids is that there is an infinite energy reservoir in the unbounded case, which allows a persistent inverse energy cascade to ever-larger scales to form, so that the energy eventually evades viscous dissipation altogether. Provided that the spectrum near $`k=0`$ is shallower than $`k^3`$, the inverse cascade asymptotically carries no enstrophy. This luxury is a consequence of both the unboundedness of the domain (in both directions) and the scale-selectivity of the molecular viscosity. In addition to the simultaneous conservation of energy and enstrophy, these properties constitute the basic building blocks of the KLB theory. Another important hypothesis is the existence of a quasi-steady state. As long as an inverse cascade is realizable and a quasi-steady state can be established in an unbounded system, the cascade dynamics are fundamentally distinct from what occurs in a bounded fluid in equilibrium. There appears to be no sound basis for extending the results from one case to the other. Of course, in an unbounded fluid it is quite possible for an inverse energy cascade to exist without a corresponding direct enstrophy cascade; in this case, there might then be certain similarities between the dynamics of the bounded and unbounded systems.

The dissipation operator plays an important role in the spectral distribution of energy. This is especially apparent in the balance equation (25) for a fluid in a doubly periodic domain: the product of the energy spectrum and the spectral dissipation function in the energy and enstrophy ranges are intimately related. This information is important for numerical 2D turbulence simulations, where various dissipation mechanisms are employed: it should help researchers rule out certain spectral distributions and anticipate possible outcomes for a given dissipation mechanism. Finally, we showed that a large-scale dissipation could give rise to a direct enstrophy cascade since the quantity $`Ps^2Z`$ could grow as $`1/\nu `$, until $`P/Zs^2`$.

## Appendix A Constraints on general spectral slopes

Strictly speaking, the spectrum (20) is too simplistic; actual spectral slopes will tend to vary monotonically with wavenumber (particularly in the enstrophy range, as one approaches the onset of the dissipation range). The arguments of Section 4 can be readily extended to more general spectra. Normalizing all wavenumbers so that $`s=1`$, we express the energy spectrum as

$`E(k)=a\{\begin{array}{cc}k^{\alpha (k)}\hfill & \text{if }k_0<k<1\text{,}\hfill \\ k^{\beta (k)}\hfill & \text{if }1k<k_1\text{,}\hfill \\ k^{\gamma (k)}\hfill & \text{if }k_1kk_T\text{,}\hfill \end{array}`$ (30)
with $`\beta (k_1)=\gamma (k_1)`$, where $`k_0`$ is the lower spectral cutoff wavenumber (determined by the domain size), $`k_1`$ is the highest wavenumber in the enstrophy range, and $`k_T`$ is the highest retained (truncation) wavenumber. Equation (18), or equivalently (25), then appears as

$`{\displaystyle _{k_0}^1}(1k^2)k^{2\alpha (k)}𝑑k`$ $`=`$ $`{\displaystyle _1^{k_1}}(k^21)k^{2\beta (k)}𝑑k+{\displaystyle _{k_1}^{k_T}}(k^21)k^{2\gamma (k)}𝑑k.`$ (31)
The change of variable $`\kappa =1/k`$ in the integrals on the right-hand side yields

$`{\displaystyle _{k_0}^1}(1\kappa ^2)\kappa ^{2\alpha (\kappa )}𝑑\kappa `$ $`=`$ $`{\displaystyle _{1/k_1}^1}(1\kappa ^2)\kappa ^{\beta (1/\kappa )6}𝑑\kappa +ϵ_\nu ,`$ (32)
where $`ϵ_\nu =_{1/k_T}^{1/k_1}(1\kappa ^2)\kappa ^{\gamma (1/\kappa )6}𝑑k0`$. For bounded turbulence, we restrict our attention to the usual case where $`k_11/k_0`$. Since $`_{1/k_1}^1(1\kappa ^2)\kappa ^\theta 𝑑\kappa `$ is a strictly decreasing function of $`\theta `$, we find that the maximum slopes $`\overline{\alpha }=\underset{k}{sup}\alpha (k)`$ and $`\overline{\beta }=\underset{k}{sup}\beta (k)`$ satisfy

$`{\displaystyle _{1/k_1}^1}(1\kappa ^2)\kappa ^{2\overline{\alpha }}𝑑\kappa `$ $``$ $`{\displaystyle _{1/k_1}^1}(1\kappa ^2)\kappa ^{2\alpha (\kappa )}𝑑\kappa {\displaystyle _{k_0}^1}(1\kappa ^2)\kappa ^{2\alpha (\kappa )}𝑑\kappa `$
$``$ $`{\displaystyle _{1/k_1}^1}(1\kappa ^2)\kappa ^{\beta (1/\kappa )6}𝑑\kappa {\displaystyle _{1/k_1}^1}(1\kappa ^2)\kappa ^{\overline{\beta }6}𝑑\kappa .`$
Hence $`2\overline{\alpha }\overline{\beta }6`$; that is, $`\overline{\alpha }+\overline{\beta }8.`$

One can also obtain estimates for the minimum slopes $`\underset{¯}{\alpha }=\underset{k}{inf}\alpha (k)`$ and $`\underset{¯}{\beta }=\underset{k}{inf}\beta (k)`$, assuming $`\gamma (k)\underset{¯}{\beta }`$:

$`{\displaystyle _{k_0}^1}(1\kappa ^2)\kappa ^{2\underset{¯}{\alpha }}𝑑\kappa `$ $`{\displaystyle _{k_0}^1}(1\kappa ^2)\kappa ^{2\alpha (\kappa )}𝑑\kappa ={\displaystyle _{1/k_1}^1}(1\kappa ^2)\kappa ^{\beta (1/\kappa )6}𝑑\kappa +ϵ_\nu `$ (33)
$`{\displaystyle _{1/k_T}^1}(1\kappa ^2)\kappa ^{\underset{¯}{\beta }6}𝑑\kappa .`$
In the asymptotic limit as $`k_00`$ and $`k_T\mathrm{}`$, we deduce $`\underset{¯}{\alpha }+\underset{¯}{\beta }8.`$

It is instructive to specialize these results to the case of constant slopes, where $`\underset{¯}{\alpha }=\overline{\alpha }=\alpha `$ and $`\underset{¯}{\beta }=\overline{\beta }=\beta `$ (e.g. if $`k_1k_\nu `$). For a bounded fluid satisfying $`k_11/k_0`$, we then see that $`lim_{k_00}\alpha +\beta =8`$.

## Appendix B Spectral slopes for a system with an inverse viscosity

It was suggested in Section 4 that a large-scale dissipation, well separated from the forcing scale, may not give rise to the desired direct enstrophy cascade and the corresponding $`k^3`$ spectrum. To demonstrate this point, we consider the special form $`D(k)=2\nu ^{}k^2+2\nu k^2`$, with $`\nu ^{}s^2=\nu s^2`$, so that at the forcing scale, the inverse viscosity and the usual molecular viscosity have the same strength. Equation (25) becomes

$`{\displaystyle \underset{k}{}}(k^2s^2)(\nu ^{}k^2+\nu k^2)E(k)`$ $`=`$ $`0.`$ (34)
Assume the spectral scaling (20) and follow the steps leading to (22), we obtain

$`{\displaystyle _{k_0/s}^1}(1\kappa ^2)(\kappa ^2+\kappa ^2)\kappa ^\alpha 𝑑\kappa `$ $``$ $`{\displaystyle _{s/k_\nu }^1}(1\kappa ^2)(\kappa ^2+\kappa ^2)\kappa ^{\beta 4}𝑑\kappa .`$ (35)
In the case $`k_0/ss/k_\nu `$ it follows that $`\alpha +\beta 4`$. In the limit $`s/k_\nu 0`$, we still require $`\beta >5`$. For the KLB enstrophy-range spectrum to be realizable it is necessary that $`\alpha 1`$; moreover, $`s/k_\nu `$ cannot be much smaller than $`k_0/s`$. The former condition does not seem to be plausible in the presence of an inverse viscosity, while the latter condition requires an unphysically narrow enstrophy range for a forcing at relatively small wavenumbers.

Acknowledgements

We would like to thank two anonymous referees for their constructive comments, which helped us clarify and improve the manuscript. This work was supported by the Natural Sciences and Engineering Research Council of Canada. CVT was also supported by a Pacific Institute for the Mathematical Sciences Postdoctoral Fellowship.