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# On Aubry Sets and Mather’s Action Functional

## 1. Introduction

We start by recalling some facts about Aubry-Mather theory. Let $`M`$ be a smooth, closed, connected $`n`$-dimensional manifold and $`L`$ be a Lagrangian on the tangent bundle $`TM`$, that is, a $`C^r,r2`$ function on $`TM`$ which is convex and superlinear when restricted to any fiber. The Euler-Lagrange equation then defines a flow $`\mathrm{\Phi }_t`$ on $`TM`$, complete in the autonomous case. Throughout this paper we assume $`M`$ to be endowed with a fixed Riemann metric, with respect to which we evaluate distances and norms in the tangent bundle ; our results do not depend on the metric. Denote by $`\pi `$ the canonical projection $`TMM`$.

For $`x,yM`$ define $`h_t(x,y)`$ as the minimum, over all absolutely continuous curves $`\gamma :[0,t]M`$ with $`\gamma (0)=x,\gamma (t)=y`$, of $`_0^tL(\gamma ,\dot{\gamma })𝑑s`$. Then, by Fathi’s weak KAM theorem (\[Fa97a\]) there exists $`c(L)`$ such that $`lim\; inf_t\mathrm{}(h_t(x,y)+c(L)t)`$ is finite for every $`x,y`$. This $`lim\; inf`$, originally defined in \[Mr93\], is called the Peierls barrier and denoted $`h(x,y)`$ and $`c(L)`$ is Mañé’s critical value (see \[Mn97\]). The Aubry set $`𝒜_0`$ is then defined in \[Fa97b\] as the zero locus of $`h`$ restricted to the diagonal in $`M\times M`$. The canonical projection $`\pi `$ is a bi-Lipschitz homeomorphism between $`𝒜_0`$ and the set $`\stackrel{~}{𝒜}_0`$ of velocity vectors of orbits in $`𝒜_0`$ (Graph Property). Furthermore $`\stackrel{~}{𝒜}_0`$ is compact and $`\mathrm{\Phi }_t`$-invariant.

Fathi’s weak KAM theorem asserts that there exists a Lipschitz function $`u_+`$ (resp. $`u_{}`$) such that $`u_\pm (\gamma (t))u_\pm (\gamma (0))_0^t(L+c(L))(\gamma ,\dot{\gamma })𝑑s`$ for every absolutely continuous path $`\gamma :[0,t]M`$, which is written $`uL+c(L)`$ for short, and such that for every $`xM,t`$ there is a $`C^1`$ path $`\gamma :[0,t]M`$ with $`\gamma (0)=x`$ (resp. $`\gamma (t)=x`$) achieving equality. Such functions come in pairs, called conjugate pairs $`(u_+,u_{})`$ such that $`u_+u_{}`$ with equality on $`𝒜_0`$. Theorem 6 of \[Fa97b\] asserts that $`h(x,y)=sup\{u_{}(y)u_+(x)\}`$, where the supremum is taken over conjugate pairs of weak KAM solutions.

For every closed 1-differential $`\omega `$, $`L\omega `$ is a convex and superlinear Lagrangian, we sometimes denote $`𝒜_\omega `$ its Aubry set $`𝒜_0(L\omega )`$. Mather’s $`\alpha `$-function is defined in \[Mr90\] as

$$\alpha (\omega )=\mathrm{min}\{_{TM}(L\omega )𝑑\mu :\mu \}$$

where $``$ is the set of closed measures on $`TM`$, that is (see \[Ba99\]) the compactly supported probability measures $`\mu `$ on $`TM`$ such that $`𝑑f𝑑\mu =0`$ for every $`C^1`$ function $`f`$ on $`M`$. In other words, those are the measures with a well-defined homology class. The measures achieving the minimum are invariant by the Euler-Lagrange flow $`\mathrm{\Phi }_t`$ of $`L`$ (see \[Ba99\]). The quantity $`\alpha `$ defines a convex and superlinear function on $`H^1(M,)`$, twice the squareroot of which is also called stable norm when $`L`$ is a metric (see \[Mt97\] and the references therein). It is convex and superlinear and its Fenchel transform is Mather’s $`\beta `$-function on $`H_1(M,)`$, which is defined, for every real homology class $`h`$, as

$$\beta (h)=\mathrm{min}\{_{TM}(L)𝑑\mu :\mu ,[\mu ]=h\}.$$

Let $`\stackrel{~}{}_\omega `$ be the closure in $`TM`$ of the union of the supports of measures in $``$ achieving the minimum in the expression of $`\alpha `$. Such measures are called $`\omega `$-minimising measures, or just minimising measures if $`[\omega ]=0`$. We call Mather set of $`L`$ and $`\omega `$, and denote $`_\omega `$ the projection $`\pi (\stackrel{~}{}_\omega )`$ ; it is contained in $`𝒜_\omega `$ (\[Fa97a\]). In particular we call Mather set of $`L`$ the Mather set $`_0`$ corresponding to the zero cohomology class.

For every $`[\omega ]H^1(M,)`$ we call $`F_\omega `$ the maximal face of the epigraph $`\mathrm{\Gamma }_\alpha `$ of $`\alpha `$ containing $`[\omega ]`$ in its interior (see \[Mt97\]), and $`\text{Vect}F_\omega `$ the underlying vector space of the affine subspace generated by $`F_\omega `$ in $`H^1(M,)`$. Beware that $`\text{Vect}F_\omega `$ is not, unless $`F_\omega `$ contains the origin,, the vector space generated by $`F_\omega `$. Note that $`F_\omega =\{[\omega ]\}`$ if $`\alpha `$ is strictly convex at $`[\omega ]`$. The value of $`\alpha `$ at the null cohomology class is Mañé’s critical value $`c(L)`$.

In section 3 we relate the dimension of the faces of $`\mathrm{\Gamma }_\alpha `$ to the topological complexity of the complement of $`𝒜_\omega `$ in $`M`$, as follows. Let $`C_\omega (ϵ)`$ be the set of integer homology classes which are represented by a piecewise $`C^1`$ closed curve made with arcs contained in $`𝒜_\omega `$, except for a remainder of total length less than $`ϵ`$. Let $`C_\omega `$ be the intersection of $`C_\omega (ϵ)`$ over all $`ϵ>0`$, and let $`V_\omega `$ be the vector space spanned in $`H_1(M,)`$ by $`C_\omega `$. Note that $`V_\omega `$ is an integer subspace of $`H_1(M,)`$, that is, it has a basis of integer elements (images in $`H_1(M,)`$ of elements of $`H_1(M,)`$).

We denote

* by $`V_\omega ^{}`$ the vector space of cohomology classes of one-forms of class $`C^1`$ that vanish on $`V_\omega `$ .
* by $`G_\omega `$ the vector space of cohomology classes of one-forms of class $`C^1`$ that vanish in $`T_xM`$ for every $`x𝒜_\omega `$
* by $`E_\omega `$ the vector space of cohomology classes of one-forms of class $`C^1`$ , the supports of which are disjoint from $`𝒜_\omega `$.

###### Theorem 1.

We have $`E_\omega \text{Vect}F_\omega G_\omega V_\omega ^{}`$. When $`M`$ is a closed, orientable surface all inclusions are equalities and furthermore $`\text{Vect}F_\omega `$ is an integer subset of $`H^1(M,)`$.

###### Theorem 2.

When $`M`$ is a closed, orientable surface the vector space $`\text{Vect}F_\omega `$ is lower semi-continuous with respect to the Lagrangian.

Theorem 1 means that when $`M`$ is a closed, orientable surface, the dimension of the face $`F_\omega `$ equals the number of homologically independant closed curves disjoint from $`𝒜_\omega `$.

As a corollary we get differentiability results for $`\beta `$. The idea here was given to the author by Albert Fathi.

Let $`h`$ be a homology class. A cohomology class $`\omega `$ is said to be a subderivative for $`\beta `$ at $`h`$ if $`<\omega ,h>=\beta (h)+\alpha (\omega )`$. The subderivatives for $`\beta `$ at $`h`$ form a face $`F_h`$ of $`\mathrm{\Gamma }_\alpha `$. By proposition 6 the Aubry (resp. Mather) sets for all the cohomology classes in the interior of this face coincide. We call that Aubry set (resp. Mather set), the Aubry set (resp. Mather set) of $`h`$, and denote it $`𝒜_h`$ (resp. $`_h`$).

Recall that the tangent cone to the epigraph of $`\beta `$ at $`h`$ is the smallest cone in $`H_1(M,)\times `$ with vertex $`(h,\beta (h))`$ and containing the epigraph of $`\beta `$. We say that the $`\beta `$-function is differentiable at $`h`$ in the direction $`d`$ if the tangent cone to the epigraph of $`\beta `$ at $`h`$ contains the affine subspace $`h+d`$.

Thus we say the $`\beta `$-function is differentiable in $`k`$ directions at a homology class $`h`$ if the tangent cone at $`h`$ to the epigraph of $`\beta `$ splits as a metric product of $`^k`$ and another cone which contains no straight line (affine subspace of dimension one).

We say a homology class $`h`$ is $`k`$-irrational if $`k`$ is the dimension of the smallest subspace of $`H_1(M,)`$ generated by integer classes and containing $`h`$. In particular $`1`$-irrational means “on a line with rational slope” and $`dimH_1(M,)`$-irrational means completely irrational. We call rational any homology class of the form $`1/nh`$ where $`n`$ is an integer and $`h`$ is the image in $`H_1(M,)`$ of an integer homology class. The integrality of $`\text{Vect}F_\omega `$ has the following consequence :

###### Corollary 3.

Let $`M`$ be a closed orientable surface, and $`L`$ be a Lagrangian on $`M`$. At a $`k`$-irrational homology class $`h`$ the $`\beta `$-function of $`L`$ is differentiable in at least $`k`$ directions.

This was conjectured, and proved in the torus case, by V. Bangert. A similar result was proved for twist maps of the annulus by J. Mather in \[Mr90\]. See also \[D93\].

In particular when $`M`$ is a closed, orientable surface, $`\beta `$ is differentiable in every direction at a completely irrational class. Rademacher’s theorem says a convex function is differentiable almost everywhere but does not provide an explicit set of differentiability points. In \[BIK97\] a $`C^r`$ metric is constructed on a torus of dimension $`8r+8`$, such that its stable norm is not differentiable in all directions at some completely irrational class.

On the other hand if $`\beta `$ is differentiable in one (resp. no) direction at some homology class $`h`$, then $`h`$ must be 1-irrational (resp. zero). Also note that at every non-zero class $`\beta `$ is differentiable in the radial direction.

In the next section we investigate generic properties of Lagrangian systems. We say a property is true for a generic Lagrangian if, given a Lagrangian $`L`$, there exists a residual (countable intersection of open and dense subsets) subset $`𝒪`$ of $`C^{\mathrm{}}(M)`$ such that the property holds for $`L+f,f𝒪`$. Mañé (\[Mn96, CDI97\]) proved that for a generic Lagrangian, there exists a unique minimising measure and put forth in \[Mn96\] the

###### Conjecture 4 (Mañé).

For a generic Lagrangian $`L`$ on a closed manifold $`M`$ there exist a dense open set $`U_0`$ of $`H^1(M,)`$ such that $`\omega U_0`$, $`_\omega (L)`$ consists of a single periodic orbit, or fixed point.

As an application of Theorems 1, 2, and the results of \[Mt97\] we prove this conjecture to be true when $`M`$ is a closed, orientable surface.

## 2. Preliminary results

Recall that by a theorem of Fathi (\[Fa00\], p. 104) there exists a pair of conjugate weak KAM solutions $`(u_+,u_{})`$ such that $`u_+`$ and $`u_{}`$ coincide only on $`𝒜_\omega `$. The main result of this section is

###### Proposition 5.

For every $`ϵ>0`$ there exists an integrable, non-negative function $`G_ϵ`$ on $`M`$ such that $`G_ϵ^1(0)=𝒜_0`$ and for every absolutely continuous arc $`\gamma :[0,t]M`$ we have

(1)
$$_0^t(L+c(L))(\gamma ,\dot{\gamma })𝑑tu_+(\gamma (t))u_+(\gamma (0))+_0^tG_ϵ(\gamma (t))𝑑tϵ.$$

###### Proof.

Since $`M`$ is compact and the functions $`h_t`$ are equilipschitz on $`M\times M`$ (\[Mr93\], see also \[Fa00\], p. 105), by Ascoli’s theorem, for every $`ϵ>0`$ there exists $`T>0`$ such that

$$x,yM,tTh_t(x,y)h(x,y)c(L)tϵ.$$

Take $`T(ϵ)`$ to be the infimum of such $`T`$’s.

Let $`\gamma :_+M`$ be a $`C^1`$ arc. Take $`ϵ>0`$. Let $`\chi _ϵ`$ be $`ϵ/\mathrm{max}(1,T(ϵ))`$ times the characteristic function of the closed set $`(u_{}u_+)^1([2ϵ,+\mathrm{}[)`$. We prove, for all positive $`t`$,

(2)
$$_0^t(L+c(L))(\gamma ,\dot{\gamma })(s)𝑑su_+(\gamma (t))u_+(\gamma (0))+_0^t\chi _ϵ(\gamma (s))𝑑sϵ.$$

The proposition follows by taking $`G_ϵ`$ to be the upper bound of the functions $`\chi _\delta `$ over all $`\delta ϵ`$.

Define a sequence in $`_+`$ by $`t_0=0`$ and $`t_{i+1}=`$

$$\mathrm{max}\{tt_i:tt_iT(ϵ)\text{ and Leb}([t_i,t]\gamma ^1(\text{supp}(\chi _ϵ)))T(ϵ)\}$$

where Leb denotes Lebesgue measure on $``$. Observe that $`\gamma (t_i)\text{supp}(\chi _ϵ)`$, that $`t_{i+1}t_iT(ϵ)`$, and that for all $`x`$ between $`t_i`$ and $`t_{i+1}`$

$$_{t_i}^x\chi _ϵ(\gamma )(s)𝑑sϵ\frac{\text{Leb}([t_i,x]\gamma ^1(\text{supp}(\chi _ϵ)))}{\mathrm{max}(1,T(ϵ))}ϵ.$$

We have, taking $`t_n`$ to be the last $`t_i`$ before $`t`$,

$$_0^t(L+c(L))(\gamma ,\dot{\gamma })(s)𝑑s=$$

$$\underset{t_{i+1}t}{}\left(_{t_i}^{t_{i+1}}L(\gamma ,\dot{\gamma })(s)𝑑s+c(L)(t_{i+1}t_i)\right)$$

$$+_{t_n}^tL(\gamma ,\dot{\gamma })(s)𝑑s+c(L)(tt_n)$$

thus, since $`u_\pm `$ are weak KAM solutions, and by the definitions of $`h_t`$, and $`T(ϵ)`$,

$`{\displaystyle _0^t}L(\gamma ,\dot{\gamma })(s)𝑑s+c(L)t`$ $``$ $`{\displaystyle \underset{t_{i+1}t}{}}h_{t_{i+1}t_i}(\gamma (t_i),\gamma (t_{i+1}))`$
$`+c(L)(t_{i+1}t_i)+u_+(\gamma (t))u_+(\gamma (t_n))`$
$``$ $`{\displaystyle \underset{t_{i+1}t}{}}\left(h(\gamma (t_i),\gamma (t_{i+1}))ϵ\right)+u_+(\gamma (t))u_+(\gamma (t_n))`$
$``$ $`{\displaystyle \underset{t_{i+1}t}{}}\left(u_{}(\gamma (t_{i+1}))u_+(\gamma (t_i))ϵ\right)+u_+(\gamma (t))u_+(\gamma (t_n))`$
$``$ $`{\displaystyle \underset{i=0}{\overset{n}{}}}\left(u_{}(\gamma (t_i))u_+(\gamma (t_i))ϵ\right)+u_+(\gamma (t))u_+(\gamma (0))`$
$``$ $`u_+(\gamma (t))u_+(\gamma (0))+ϵ\mathrm{}\{i/t_it\}`$
$``$ $`{\displaystyle \underset{i=1}{\overset{n}{}}}{\displaystyle _{t_{i1}}^{t_i}}\chi _ϵ(\gamma )(s))ds+u_+(\gamma (t))u_+(\gamma (0))`$
$``$ $`u_+(\gamma (t))u_+(\gamma (0))+{\displaystyle _0^t}\chi _ϵ(\gamma )(s)𝑑sϵ.`$
### 2.1. proof of Proposition 6

The next proposition enables us to speak of the Aubry set of a face of the epigraph of $`\alpha `$, and therefore, of the Aubry set of a homology class.

###### Proposition 6.

If a cohomology class $`[\omega _1]`$ belongs to the maximal face $`F_\omega `$ of $`\mathrm{\Gamma }_\alpha `$ containing $`[\omega ]`$ in its interior, then $`𝒜_\omega 𝒜_{\omega _1}`$. In particular, if $`[\omega _1]`$ belongs to the interior of $`F_\omega `$, then $`𝒜_\omega =𝒜_{\omega _1}`$. Conversely, if two cohomology classes $`\omega `$ and $`\omega _1`$ are such that $`\stackrel{~}{𝒜_\omega }\stackrel{~}{𝒜}_{\omega _1}\mathrm{}`$, then $`\alpha (\omega )=\alpha (a\omega +(1a)\omega _1)`$ for all $`a[0,1]`$, i.e. $`\mathrm{\Gamma }_\alpha `$ has a face containing $`\omega `$ and $`\omega _1`$.

###### Proof.

We can find $`\omega _2F_\omega `$ and $`a]0,1[`$ such that $`\omega =a\omega _1+(1a)\omega _2`$. By \[Fa98a\], the following property characterises $`𝒜_\omega `$:

$$x𝒜_\omega ,t_n+\mathrm{},\text{ and }\gamma _n:[0,t_n]M,\text{ such that }\gamma (0)=\gamma (t_n)=x$$

$$\text{ and }_0^{t_n}(L\omega )(\gamma _n,\dot{\gamma }_n)(s)𝑑s+\alpha (\omega )t0.$$

Now $`\omega =a\omega _1+(1a)\omega _2`$, and $`\alpha (\omega )=a\alpha (\omega _1)+(1a)\alpha (\omega _2)`$ since $`[\omega _1],[\omega _2]F_\omega `$. Therefore

$$a\left[_0^{t_n}(L\omega _1)(\gamma _n,\dot{\gamma }_n)(s)𝑑s+\alpha (\omega _1)t\right]$$

$$+(1a)\left[_0^{t_n}(L\omega _2)(\gamma _n,\dot{\gamma }_n)(s)𝑑s+\alpha (\omega _2)t\right]0.$$

Observe that both summands on the left are non-negative, for if $`u_{}`$ is a weak KAM solution for $`L\omega _i`$, $`i=1,2`$, we have

$`{\displaystyle _0^{t_n}}(L\omega _i)(\gamma _n,\dot{\gamma }_n)(s)𝑑s+\alpha (\omega _1)t`$ $``$ $`u_{}(\gamma (t_n))u_{}(\gamma (0))`$
$`=`$ $`u_{}(x)u_{}(x)=0`$
$$\text{hence }_0^{t_n}(L\omega _i)(\gamma _n,\dot{\gamma }_n)(s)𝑑s+\alpha (\omega _1)t0\text{ when }n\mathrm{}.$$

Conversely, let $`(\gamma ,\dot{\gamma })`$ be an orbit in $`\stackrel{~}{𝒜_\omega }\stackrel{~}{𝒜}_{\omega _1}`$. We have

$$_0^t[L\omega +\alpha (\omega )](\gamma ,\dot{\gamma })(s)𝑑s=u(\gamma (t))u(\gamma (0)),$$

$$_0^t[L\omega _1+\alpha (\omega _1)](\gamma ,\dot{\gamma })(s)𝑑s=u_1(\gamma (t))u_1(\gamma (0)),$$

where $`u`$ (resp. $`u_1`$) is a weak KAM solution for $`L\omega `$ (resp. $`L\omega _1`$). Therefore

$$_0^t[L(a\omega +(1a)\omega _1)+\alpha (a\omega +(1a)\omega _1)](\gamma ,\dot{\gamma })(s)𝑑s=$$

$$a[u(\gamma (t))u(\gamma (0))]+(1a)[u_1(\gamma (t))u_1(\gamma (0))]$$

$$+t[\alpha (a\omega +(1a)\omega _1)a\alpha (\omega )(1a)\alpha (\omega _1))].$$

The first two summands on the right are bounded below, hence for the sum to be bounded below, we must have $`\alpha (\omega )=a\alpha (\omega )+(1a)\alpha (\omega _1)=\alpha (a\omega +(1a)\omega _1)`$, since by convexity of $`\alpha `$, $`\alpha (a\omega +(1a)\omega _1)a\alpha (\omega )+(1a)\alpha (\omega _1)`$. ∎

## 3. Faces of the epigraph

Proof of $`G_\omega V_\omega ^{}`$.

It amounts to showing that a one-form in $`G_\omega `$ vanishes on $`V_\omega `$. Let $`\omega G_\omega `$ and let $`h`$ be represented as in the definition of $`V_\omega `$ for some $`ϵ>0`$. Call $`S`$ the part of the curve representing $`h`$ which consists in segments of $`𝒜_\omega `$, and $`R`$ the remainder. Now $`<[\omega ],h>=_S\omega +_R\omega `$ where the first summand is zero, and the second summand can be bounded by $`Cϵ`$, where $`C`$ depends on $`L`$ and $`\omega `$ only. The conclusion follows since $`ϵ`$ is arbitrarily small. ∎

Proof of $`\text{Vect}F_\omega G_\omega `$.

Take $`\omega _1,\omega _2F_\omega `$. By Proposition 6 the Aubry sets for $`L\omega _1`$ and $`L\omega _2`$ coincide with $`𝒜_\omega `$. The weak KAM solutions $`(u_+,u_{})`$ are differentiable at every point of $`𝒜_{(u^+,u^{})}`$ (see \[Fa97a\]) with derivative the Legendre transform of the (well defined) tangent vector. This derivative is Lipschitz and furthermore (see \[Fa00\], p. 92) we have

(3)
$$|u_\pm (\varphi (y))u_\pm (\varphi (x))\frac{L\omega }{v}(\varphi (x),\dot{\gamma }(0))D_x\varphi (yx)|Kyx^2$$

where $`\varphi `$ is a local chart on $`M`$, $`x`$ and $`y`$ are two points in the inverse image of $`𝒜_\omega `$ by the chart, $`\dot{\gamma }(0)`$ is the tangent vector to $`𝒜_\omega `$ at $`\varphi (x)`$, and $`K`$ only depends on the chart. So Whitney’s extension theorem (\[Fe69\], theorem 3.1.14) allows us to take $`\stackrel{~}{u}_1,\stackrel{~}{u}_2`$ two $`C^1`$ functions, the derivatives of which coincide with that of $`u_+^1`$ and $`u_+^2`$ respectively along $`𝒜_\omega `$. Replace $`\omega _2`$ by $`\omega _2+d\stackrel{~}{u}_1d\stackrel{~}{u}_2`$. This one-form coincides with $`\omega _1`$ in the tangent space to every point of $`𝒜_\omega `$ hence the cohomology class $`[\omega _1\omega _2]`$ belongs to $`G_\omega `$. ∎

Proof of $`E_\omega \text{Vect}F_\omega `$

Assume, replacing if necessary $`L`$ by $`L\omega `$, that $`\omega =0`$. We actually prove a slightly stronger statement. Call $`\stackrel{~}{𝒯}_0`$ the intersection with $`𝒜_0`$ of the union of Hausdorff limits, when $`\eta `$ tends to $`0`$, of supports of $`L\eta `$-minimising measures, and call $`𝒯_0`$ its projection to $`M`$. Let $`\eta `$ be supported away from $`𝒯_0`$.

For starters we prove that there exists $`\delta >0`$ such that for all $`L+\delta \eta `$-minimising measure $`\mu `$, for all $`(x,v)`$ in $`\text{supp}(\mu )`$, we have $`\delta |\eta _x(v)|G_1(x)`$ where $`G_1`$ comes from Proposition 5.

Indeed, assume otherwise. Then there exists a sequence $`\delta _n0`$, $`L+\delta _n\eta `$-minimising measures $`\mu _n`$, and points $`(x_n,v_n)`$ in $`\text{supp}(\mu _n)`$ such that for all $`n`$, we have

(4)
$$\delta _n|\eta _{x_n}(v_n)|>G_1(x_n).$$

The sequence $`(x_n,v_n)`$ is bounded in $`TM`$ because the measures $`\mu _n`$ sit in the energy levels $`\alpha (\delta _n[\eta ])`$. So we may assume $`(x_n,v_n)(x,v)`$. Then we have $`G_1(x_n)0`$ so by construction of $`G_1`$, $`G_1(x)=0`$ and $`x𝒜_0`$. Besides, $`(x,v)`$ belongs to a Hausdorff limit point of the sequence of compact sets $`\text{supp}(\mu _n)`$ so $`x𝒯_0`$. But then for $`n`$ large enough, since $`\eta `$ is supported outside $`𝒯_0`$, we should have $`\eta _{x_n}(v_n)=0`$ which contradicts Equation 4 since $`G_1`$ is non-negative.

Therefore we see that for every orbit $`\gamma `$ in the support of an $`L+\delta \eta `$-minimising measure $`\mu `$, by Equation 1 we have

$$_0^t(L+c(L)\pm \delta \eta )(\gamma ,\dot{\gamma })(s)𝑑s$$

$$u_+(\gamma (t))u_+(\gamma (0))+_0^t(G_1\pm \delta \eta )(\gamma ,\dot{\gamma })(s)𝑑s1$$

so , by averaging and letting $`t`$ go to infinity,

$$c(L\pm \delta \eta )(G_1\pm \delta \eta )𝑑\mu c(L)$$

whence, since $`G_1\pm \delta \eta `$ is non-negative on the support of $`\mu `$,

$$\alpha (0)=c(L)c(L\pm \delta \eta )=\alpha (\pm \delta \eta ).$$

By convexity of $`\alpha `$, we have $`2\alpha (0)\alpha (\delta \eta )+\alpha (\delta \eta )`$ so we get $`\alpha (0)=\alpha (\pm \delta \eta )`$ which implies that $`\pm \delta [\eta ]`$ belong to $`F_0`$. ∎

### 3.1. The two-dimensional case

We prove that when $`M`$ is a closed surface, $`V_\omega ^{}E_\omega `$, thus proving all inclusions to be equalities. Since $`V_\omega `$ is an integer subset of $`H_1(M,)`$ this implies that $`\text{Vect}F_\omega `$ is an integer subset of $`H^1(M,)`$.

To that end we prove that there exists a neighborhood $`U`$ of $`𝒜_\omega `$ such that every closed curve contained in $`U`$ has its homology class in $`V_\omega `$. First let us show how this implies the equality. If a 1-form $`\alpha `$ vanishes on every element of $`V_\omega `$, then there exists a function $`f`$ defined on $`U`$ such that the restriction of $`\alpha `$ to $`U`$ is equal to $`df`$. Extend $`f`$ to $`M`$, now $`\alpha df`$ is cohomologous to $`\alpha `$ and supported away from $`U`$.

Assume the surface has genus greater than one, the genus one case being treated by Bangert in \[Ba94\], and assume our reference metric $`g`$ has negative curvature. By \[BG99\] every minimising orbit stays within finite distance, in the universal cover $`\stackrel{~}{M}`$ of $`M`$, of a $`g`$-geodesic. In particular one can define the ends of a minimiser in the boundary at infinity of $`\stackrel{~}{M}`$. Call $`\lambda `$ the geodesic lamination obtained from $`𝒜_\omega `$ by replacing each orbit by the corresponding geodesic.

From \[CB88\], we know that each boundary component of a connected component of the complementary set of $`\lambda `$ in $`M`$ is either a closed leaf of $`\lambda `$, or a finite sequence of non-closed leaves $`\delta _1,\mathrm{}\delta _n`$ such that $`\delta _i`$ and $`\delta _{i+1}`$ are asymptotic ($`i`$ being in $`/n`$).

Therefore each boundary component of a connected component of the complementary set of $`𝒜_\omega `$ in $`M`$ is either a closed orbit in $`𝒜_\omega `$, or a finite sequence of non-closed orbits $`\delta _1,\mathrm{}\delta _n`$ such that $`\delta _i`$ and $`\delta _{i+1}`$ are asymptotic ($`i`$ being in $`/n`$).

Hence for each boundary component $`\delta `$ of a connected component $`R`$ of the complementary set of $`𝒜_\omega `$ in $`M`$ there exists a neighborhood $`V`$ of $`\delta `$ in $`R`$ such that every arc contained in $`V`$, with its end on $`\delta `$, is homotopic, with fixed ends, to an arc consisting of portions of $`\delta `$ and a remainder of length arbitrarily small (or no remainder at all if $`\delta `$ is a closed leaf). Now we just need to take $`U`$ such that $`UM𝒜_\omega `$ is contained in the union over all boundary components of $`R`$, and over all connected component of the complementary set of $`𝒜_\omega `$ in $`M`$, of such neighborhoods. ∎

Proof of Corollary 3.

Let $`h`$ be a $`k`$-irrational homology class. Then the set of subderivatives to $`\beta `$ at $`h`$ form a face $`F_h`$ of $`\mathrm{\Gamma }_\alpha `$. Furthermore $`\beta `$ is differentiable in $`(dimH_1(M,)dimF_h)`$ directions. Take $`\omega `$ in the interior of the face$`F_h`$. We have $`F_hF_\omega `$ so $`dimG_\omega dimF_h`$.

Then for every $`\omega ^{}G_\omega `$ we have $`<\omega ^{},h>=0`$. Note that $`\{hH_1(M,):<\omega ^{},h>=0\omega ^{}G_\omega \}`$ is an integer subset of $`H_1(M,)`$, of dimension $`dimH_1(M,)dimG_\omega `$.

Since $`h`$ is $`k`$-irrational this implies $`dimH_1(M,)dimG_\omega k`$ whence $`dimH_1(M,)dimF_hk`$ which proves Corollary 3. ∎

Proof of Theorem 2

Assume a sequence of Lagrangians $`L_n`$ converges, in the $`C^2`$-topology, to a $`C^2`$ Lagrangian $`L`$.

Let $`(u_n^+,u_n^{})`$ be conjugate pair of weak KAM solutions for $`L_n`$. By \[Fa00\], p. 88 the functions $`(u_n^+,u_n^{})`$ are equi-Lipschitz. By Ascoli’s theorem we may assume that $`(u_n^+,u_n^{})`$ converges to a pair $`(u^+,u^{})`$ of Lipschitz functions. Furthermore $`u^\pm L+c(L)`$. Take $`xM`$ and $`t_+`$. For every $`n`$ there exists a $`C^1`$ path $`\gamma _n:[0,t]M`$ such that $`\gamma _n(0)=x`$ (resp. $`\gamma _n(t)=x`$) and

$$u_n^\pm (\gamma _n(t))u_n^\pm (\gamma _n(0))=_0^t(L_n+c(L_n))(\gamma _n,\dot{\gamma }_n)𝑑s.$$

Take $`vT_xM`$ a limit point of $`\dot{\gamma }_n(0)`$ (resp. $`\dot{\gamma }_n(t)`$). Then the extremal trajectory $`\gamma :[0,t]M`$ of the Lagrangian, with $`\gamma (0)=x`$ and $`\dot{\gamma }(0)=v`$ (resp. $`\gamma (t)=x`$ and $`\dot{\gamma }(t)=v`$)is a uniform limit of $`\gamma _n`$ and so

$$u^\pm (\gamma (t))u^\pm (\gamma (0))=_0^t(L+c(L))(\gamma ,\dot{\gamma })𝑑s.$$

This shows that $`(u^+,u^{})`$ are weak KAM solutions for $`L`$. Then for every neighborhood $`U`$ of $`\{xM:u^+(x)=u^{}(x)\}`$ there exists an $`N`$ such that $`nN,\{xM:u_n^+(x)=u_n^{}(x)\}U`$. Hence there exists an $`N`$ such that $`nN,E_0(L)E_0(L_n)`$. ∎

## 4. On Generic Lagrangians

From now on we assume $`M`$ to be a closed orientable surface. We begin with a

###### Lemma 7.

Let $`L`$ be a Lagrangian on a closed orientable surface. The set $`S(L)`$ of subderivatives to $`\beta `$ at 1-irrational homology classes is dense in $`H^1(M,)`$.

###### Proof.

Assume there exists an open set $`U`$ in $`H^1(M,)`$ such that $`US(L)=\mathrm{}`$. We may assume $`U`$ to be convex. Then the set $`V=\{hH_1(M,):\omega U,<\omega ,h>=\alpha (\omega )+\beta (h)\}`$ is also convex. Call $`H`$ the vector space $`V`$ generates in $`H_1(M,)`$. Then, since $`V`$ does not contain any 1-irrational class, the codimension of $`H`$ is at least one. Now $`U=_{hV}F_h`$ so there exists $`hV`$ such that $`dimF_h1`$. Such an $`h`$ is at most $`(dimH_1(M,)1)`$-irrational by Corollary 3. Take $`\omega `$ in the interior of $`F_h`$ ; we have $`\text{Vect}F_\omega =E_\omega `$ so there exists a closed curve $`\gamma `$, such that $`𝒜_\omega `$ is disjoint from $`\gamma `$. Furthermore, by semi-continuity of $`\text{Vect}F_\omega =E_\omega `$, there exists a convex neighborhood $`U_1`$ of $`\omega `$ in $`U`$ such that for all $`\omega ^{}`$ in $`U_1`$, $`𝒜_0(L\omega ^{})`$ is disjoint from $`\gamma `$. In particular $`H`$ is contained in the integer subspace defined by the equation $`\text{Int}([\gamma ],.])=0`$.

Now assume by induction we have proved that for some $`2kdimH_1(M,)2`$ there exist $`\omega _k`$ in $`U`$, a convex neighborhood $`U_k`$ of $`\omega _k`$ in $`U`$, and closed curves $`\gamma _1:=\gamma ,\mathrm{}\gamma _k`$ such that for all $`\omega ^{}`$ in $`U_k`$, $`𝒜_0(L\omega ^{})`$ is disjoint from $`\gamma _1:=\gamma ,\mathrm{}\gamma _k`$. Likewise define $`V_k`$ to be the set of homology classes at which elements of $`U_k`$ are subderivatives, and $`H_k`$ to be the vector space generated by $`V_k`$. Then $`H_k`$ is contained in the integer subspace defined by the equations $`\text{Int}([\gamma _i],.])=0`$ for $`i=1,\mathrm{}k`$ and the codimension of $`H_k`$ is at least $`k`$. Assume the codimension of $`H_k`$ is exactly $`k`$ ; then as previously $`H_k`$ is an integer subspace. Any open (in the induced topology) subset of such a subspace contains a 1-irrational class, an impossibility. So the codimension of $`H_k`$ is at least $`k+1`$. Then, as previously, there exists $`h_kV_k`$ such that $`dimF_{h_k}k+1`$. Such an $`h_k`$ is at most $`(dimH_1(M,)k1)`$-irrational by Corollary 3. Take $`\omega _{k+1}`$ in the interior of $`F_{h_k}`$ ; we have $`\text{Vect}F_{\omega _{k+1}}=E_{\omega _{k+1}}`$ so there exists a closed curve $`\gamma _{k+1}`$ homologically independent from $`\gamma _1:=\gamma ,\mathrm{}\gamma _k`$, such that $`𝒜_{\omega }^{}{}_{k+1}{}^{}`$ is disjoint from $`\gamma _1,\mathrm{}\gamma _{k+1}`$. Furthermore, by semi-continuity of $`\text{Vect}F_\omega =E_\omega `$, there exists a convex neighborhood $`U_{k+1}`$ of $`\omega _{k+1}`$ in $`U_k`$ such that for all $`\omega ^{}`$ in $`U_{k+1}`$, $`𝒜_0(L\omega ^{})`$ is disjoint from $`\gamma _1,\mathrm{}\gamma _{k+1}`$.

By induction we prove that $`U`$ contains a $`(dimH_1(M,)k)`$-irrational class, for all $`k=1,\mathrm{}dimH_1(M,)1`$, a contradiction. ∎

By \[Mt97\], Proposition 5, any minimizing measure with a rational homology class must be supported on a union of periodic orbits, or fixed points.

By \[Mn96\], Theorem D, for a given homology class $`h`$, there exists a residual subset $`𝒪_h`$ of $`C^{\mathrm{}}(M)`$ such that for all $`\varphi 𝒪_h`$ there exists a unique closed measure in $`_h(L+\varphi )`$.

Then for all $`h`$ with rational direction, for all $`\varphi 𝒪_h`$ there exists a unique closed measure $`\mu _{h,\varphi }`$ in $`_h(L+\varphi )`$, supported on a union of periodic orbits $`\gamma _{h,\varphi }`$. Every such periodic orbit is minimising in its homology class. Then by \[Mn96\], Theorem D, we may assume that $`\gamma _{h,\varphi }`$ consists of pairwise non homologous periodic orbits. For any given $`K`$ only a finite number of integer homology classes have their $`L`$-action $`K`$ so then $`\gamma _{h,\varphi }`$ actually consists of a finite number of periodic orbits $`\gamma _{h,\varphi ,i}`$. For each of those orbits there exists a closed one-form $`\omega _i`$ such that $`\gamma _{h,\varphi ,i}`$ is the unique $`L\omega _i`$-minimising measure (cf. \[Mt97\], Theorem 8). Then by \[CI99\], Theorem D, we may assume $`\gamma _{h,\varphi }`$ to be hyperbolic in its energy level.

Next we prove that, for all $`\varphi 𝒪_h`$, there exists $`ϵ(h,\varphi )>0`$, such that for any $`\lambda ]1ϵ(h,\varphi ),1+ϵ(h,\varphi )[`$, there exists a unique closed measure $`\mu _{\lambda ,\varphi }`$ in $`_{\lambda h}(L+\varphi )`$, supported on a union of periodic orbits $`\gamma _{\lambda ,\varphi }`$, homotopic to $`\gamma _{h,\varphi }`$.

Indeed, fix $`\varphi 𝒪_h`$, and consider a sequence $`\lambda _n`$ of real numbers converging to one. Let $`\mu _n`$ be $`\lambda _nh`$-minimising measures. The sequence of measures $`\mu _n`$ converge to an $`h`$-minimising measure, and the only possibility is that it is supported on $`\gamma _{h,\varphi }`$. The latter being hyperbolic, a topological conjugacy argument proves our claim.

The set of 1-irrational homology classes is a countable union of lines. Choose a countable dense subset $`h_i,i`$. Call $`𝒪`$ the intersection over all $`i`$ of $`𝒪_{h_i}`$ ; this is a countable intersection of residual sets, hence residual. Now for all $`\varphi 𝒪`$, there exists an open and dense subset $`U(\varphi )`$ of the subset of 1-irrational homology classes, such that for any $`hU(\varphi )`$, there exists a unique closed measure $`\mu _{h,\varphi }`$ in $`_h(L+\varphi )`$, supported on a union of periodic orbits $`\gamma _{h,\varphi }`$.

If $`M`$ has genus $`2`$, by Theorems 7 and 8 of \[Mt97\], every subderivative to $`\beta `$ at a 1-irrational homology class is contained in a face of codimension one, whether on the boundary or in the interior. By Corollary 3, if a cohomology class is contained in a face of codimension one (resp. zero), then it must be subderivative to $`\beta `$ at a 1-irrational (resp. zero) homology class.

The same is true if $`M`$ is a torus and $`\varphi 𝒪`$ ; for in that case, in every 1-irrational homology class $`h`$, there exists a unique minimising measure. Such a measure is supported on one periodic orbit, hence $`\beta `$ is not differentiable at $`h`$ (\[Ba94\]).

Hence when $`\varphi 𝒪`$ $`S(L+\varphi )`$ equals the set of cohomology class contained in a face of codimension one or zero.

Now consider the set $`S^{}(L+\varphi )`$ of cohomology classes contained in the interior of a face of codimension one or zero, and subderivative to $`\beta `$ at a point of $`U(\varphi )`$. By Theorem 2 $`S^{}(L+\varphi )`$ is open in $`H^1(M,)`$ for any Lagrangian $`L`$. Besides, since the interior of any face is dense in that face, and the $`h_i`$ are dense in $`H_1(m,)`$, $`S^{}(L)`$ is dense in $`S(L)`$, hence in $`H^1(M,)`$. Note that for all $`\omega S^{}(L+\varphi )`$, $`_\omega `$ consists of periodic orbits with the same homology class, or fixed points. Indeed if $`_\omega `$ contained two homologically distinct periodic orbits, then $`V_\omega `$ would contain their homology classes and its dimension would be at least two, so $`\omega `$ could not lie in the the interior of a face of codimension one or zero.

In particular for for all $`\varphi 𝒪`$, $`\omega S^{}(L+\varphi )`$, $`_\omega (L+\varphi )`$ consists of one periodic orbit or fixed point. This proves Conjecture 4 for surfaces.

Acknowledgements : the author thanks Albert Fathi for patiently explaining his theory, Victor Bangert for his kind invitation to Freiburg where part of this work was done, John Mather for pointing out a mistake in an early version, Renato Iturriaga and Hector Sanchez for the invitation to the workshop on Lagrangian Systems at CIMAT, and David Théret, as well as Patrick Bernard, for useful conversations.

CIMAT, Guanajuato, Gto., Mexico, and
GTA, UMR 5030, CNRS, Université Montpellier II, France
e-mail : massart@cimat.mx


text:
# Total-energy-based prediction of a quasicrystal structure

## Abstract

Quasicrystals are metal alloys whose noncrystallographic symmetry and lack of structural periodicity challenge methods of experimental structure determination. Here we employ quantum-based total-energy calculations to predict the structure of a decagonal quasicrystal from first principles considerations. We employ Monte Carlo simulations, taking as input the knowledge that a decagonal phase occurs in Al-Ni-Co near a given composition, and using a few features of the experimental Patterson function. The resulting structure obeys a nearly deterministic decoration of tiles on a hierarchy of length scales related by powers of $`\tau `$, the golden mean.

Al-Ni-Co forms thermodynamically stable and highly perfect decagonal quasicrystalline samples over a range of compositions . Of special interest is the composition Al0.70Ni0.21Co0.09 for which the structure is periodic along the z axis with a period of $`c=4.08`$ Å, and quasiperiodic perpendicular to this axis with a characteristic length (termed a “quasilattice constant”) of $`a_0=2.45`$ Å . This “basic Ni” composition is well suited for theoretical modeling because it should be the simplest structure, lacking the quasiperiodic modulation and $`c`$-axis doubling observed at other compositions. Numerous attempts to determine the structure of this compound start from experimental data  but do not predict a structure on the basis of total energy.

The transition metals Ni and Co (generically denoted “TM”) play similar chemical roles in Al-transition metal quasicrystals, and they are not distinguished by ordinary X-ray or electron diffraction. Our model predicts distinct sites for Ni and Co near the “basic” composition.

Our total energy calculations employ quantum-based pair-potentials derived from the generalized pseudopotential theory (GPT) . GPT expands the total energy in a series of volume-, pair- and many-body-potentials. The volume term exerts no force and may be neglected at fixed volume and composition. The many-body terms are small except among clusters of neighboring transition-metal atoms, and we incorporate their influence with modified short-ranged TM-TM pair interactions constrained by full ab initio calculations.

We identify four salient properties of the computed oscillatory potentials : (1) V$`{}_{\mathrm{AlAl}}{}^{}(r)`$ has a broad shoulder starting around $`r=2.9`$ Å and is repulsive at shorter distances; (2) V$`{}_{\mathrm{AlCo}}{}^{}(r)`$ and V$`{}_{\mathrm{AlNi}}{}^{}(r)`$ exhibit deep first minima near $`r=2.5`$ Å and second minima near $`r=4.5`$ Å; (3) The VAlCo well is significantly deeper than the VAlNi well; (4) The modified $`V_{\mathrm{TMTM}}(r)`$ have shallow minima near r=2.6 Å.

The following features of the $`d`$(AlNiCo) structures are evident in the experimentally determined Patterson function  which contains a peak at every interatomic vector $`𝐫`$: (A) All atoms lie on or nearly on layers separated by $`c/2=2.04`$ Å; (B) The vector from an atom to a nearest neighbor (with a tolerance of $`0.1`$ Å) belongs to a small, discrete basis set of “linkage” vectors; (C) The in-plane components of linkage vectors are $`\pm a_0𝐞_i`$ (see Fig. 1) or simple sums of such vectors.

We construct trial quasicrystal structures that achieve low total energy while satisfying the above experimental constraints. To enforce constraints (B) and (C) we limit atomic positions to a collection of discrete sites (Fig. 1), located at vertices of a two-dimensional tiling of rhombi with edge $`a_0`$ and acute angles $`36^{}`$ or $`72^{}`$. To enforce constraint (A) we stack two independent tilings above each other. As the tiles can be placed in many ways, and atoms distributed randomly among the sites, these minimal constraints permit a great variety of structures, including all reasonable quasicrystal structures. After we discover favorable low energy motifs consistent with the minimal constraints, we remove unnecessary degrees of freedom, effectively defining highly constrained models.

A Metropolis Monte Carlo annealing yields low energy structures. Two kinds of Monte Carlo steps are employed: (i) swaps between nearby atoms of different species in either layer, including hops of one atom to an empty ideal site nearby; (ii) “flips” which reshuffle the three rhombi in a fat or thin hexagon, in one layer. (see Fig. 1) Due to the hexagon flips, our ensemble is an “equilibrium random tiling” allowing phason disorder , but the system is free to find a quasiperiodic state if that is favored by the potentials. Our simulations are performed with periodic boundary conditions using cell sizes chosen to best approximate the quasiperiodic structure.

In our initial simulation with minimal constraints, we employ a cell of size $`12.22\times 14.37\times 4.08`$ Å3 and composition Al34Ni12Co4. This cell contains 72 ideal sites, 36 in each layer with the $`c`$-axis periodicity enforced. Slow cooling identifies a unique minimum energy configuration illustrated in Fig. 2a.

The optimal configuration can be described simply in terms of a new highly constrained model (see Fig. 2b) that obeys the following rules: (i) the entire plane is tiled by three compound tiles called “hexagon”, “boat”, and “star”, outlined by heavy edges and built respectively of three, four, and five rhombi (this is called the “HBS” tiling ). (ii) The optimal decoration of the HBS tiles is virtually unique. Minimally constrained simulations with larger cells support these rules.

We can understand this decoration in terms of the salient features of the potential we enumerated at the start. In view of features (1) and (2), the minimum-energy structure must maximize the number of Al-Co and Al-Ni bonds. In view of feature (3), every Co ought to have purely Al neighbors, which is geometrically feasible just up to $``$10 % Co, which is the “basic” composition. Thus, all TM-TM neighbors must be Ni-Ni. Every Ni has mostly Al neighbors but cannot escape having two or three Ni neighbors, since $``$30 % of all atoms are transition metals.

Let us check which ideal-site separations are favorable for which atom pairs. Within the same layer, the tile edge length $`r_2`$=2.45 Å is unfavorable for Al-Al or TM-TM bonds, but highly favorable for Al-TM bonds. However, because of the high density of Al atoms, we find a small number of Al-Al bonds do take this length. The short diagonal of a fat rhombus is $`r_3=2.88`$ Å, which is an acceptable Al-Al distance. Hence the $`72^{}`$ Al-TM-Al isosceles triangle (half a fat rhombus) is highly favored within a layer.

The interlayer spacing $`c/2`$=2.04 Å is too short for any pair. Sites in adjacent layers, spaced by $`\tau ^1a_0`$ in-plane (e.g., the short diagonal of the thin rhombus), are separated by $`r_1^{}=2.54`$ Å which is favorable for Al-TM or TM-TM bonds. Finally, sites in adjacent layers separated by $`a_0`$ in-plane have a total separation of $`r_2^{}=3.19`$ Å which is an acceptable Al-Al distance.

Given this understanding of chemical bond lengths we can easily justify the decoration of the HBS tiles. Each tile is bounded by Al atoms of alternating heights at separation $`r_2^{}`$. Interior sites of the hexagon tile are too close to the Al border for Al atoms. Since it must hold two TM atoms, it holds a pair of Ni atoms at distances $`r_1^{}`$ and $`r_2`$ from the border Al and mutual separation $`r_1^{}`$. Four of the border Al atoms form a rectangle with edges $`r_2^{}`$ and $`r_3`$ lying in a plane that is nearly the perpendicular bisector of the Ni-Ni bond. This fragment of the hexagon tile is thus a slightly distorted region of B2 (CsCl) structure .

The interior vertex of the boat and star tiles are at the ideal TM distance $`r_2`$ from border Al atoms. Since this is a point of high Al coordination, it is occupied by Co. The boat and star tiles have room for two additional interior Al atoms at separation $`r_3`$. In an isolated star tile this interior Al pair can lie in any of five symmetry-related configurations. The structure surrounding the star generally breaks this degeneracy by means of long-range interactions.

In the decoration just described, an Al atom on an HBS tiling vertex is often at the center of a small cluster which was an important motif of earlier models . This cluster appears in Fig. 2b wherever hexagons join at their tips. This cluster consists of a pentagon of mixed Al and Ni atoms in the same layer as the vertex Al, and additional pentagons in the adjacent layers above and below. These adjacent pentagons contain only Al atoms and are rotated by 36$``$ with respect to the middle pentagon. This cluster exhibits interlayer Al-Ni separations of 2.54 Å and 4.46 Å, precisely at the first and second minima of V$`\mathrm{AlNi}`$.

Since the HBS tile corners are all multiples of $`72^{}`$, edges emanating from the HBS corner atoms in one layer can only point in the five directions $`+𝐞_i`$ while those within the other layer point in the directions $`𝐞_i`$. Statistically, the layers are equivalent but related by a screw axis. Allowing for the reflection planes normal to the layers, and in the absence of further symmetry-breaking, the HBS decoration implies a space group $`10_5`$/mmc, consistent with experiment.

For the next level of modeling, we take the highly constrained HBS tiles as fundamental objects. Tile-tile interactions are defined implicitly as the sum of the pair potentials between atoms decorating the tiles. The allowed “flips” (Monte Carlo moves) of the HBS tiling are called “bow tie flips” as the tile edges before and after the flip outline a bow tie shape . The bow tie flips are generated by fat hexagon flips of the underlying rhombus tiling. Additionally the Al pair inside the star can rotate among its five allowed orientations. The reduced degrees of freedom make the highly constrained HBS tiling much faster to simulate at low temperatures than the minimally constrained rhombus tiling.

The ensemble of random HBS tilings contains a variable tile frequency ratio H:B:S because HS pairs interchange with BB pairs by bow tie flips. Highly constrained simulations forbid this flip because it alters the chemical composition, given our ideal tile decoration. There is a particular “golden” ratio H:B:S=$`\sqrt{5}\tau :\sqrt{5}:1`$ that is obtained, for example, by removing double-arrow edges from a Penrose tiling. Decorating such a tiling deterministically yields an ideal composition Al0.700Ni0.207Co0.093 and atomic volume 14.16 Å3. Both composition and atomic volume are consistent with experiment.

Large-scale simulations (see Fig. 3) reveal a “supertile” ordering in which hexagons connect tip-to-tip. Each hexagon tip becomes a vertex of a “supertiling”, with longer edges of length $`\tau ^2a_0`$ along the midline of every hexagon. Since orientations of adjoining hexagons differ by multiples of $`72^{}`$ degrees, the same is true for their midlines, hence the “supertile” edges differ by $`72^{}`$ angles and form mainly HBS tiles (as well as a new “defect” tile).

The supertile atomic structure is mechanically stable. Under relaxation of the structure shown in figure 2 (which consists of two large scale hexagons), the average Co and Ni displacement is just 0.10 Å. The average Al displacement is 0.17 Å except for the two Al atoms located slightly off-center in the large-scale hexagons which displace 1.13 Å to the symmetric points at the hexagon centers.

The “defect” tile breaks the connectivity of the small-hexagon chain, introducing a new tile shape which we call a “bow tie”. To understand the role of the bow tie and its low symmetry decoration, consider the energetics of the large scale HBS tilings. Because the large-scale HBS tile decoration is essentially deterministic, we may replace the actual interatomic interactions with effective interactions between tiles. We find a single parameter dominates the energetics: an energy cost is associated with 72 junctions between tile edges decorated with Ni atom pairs, because the resulting high density of Ni atoms reduces the number of favorable Al-Ni bonds. Defect tiles enter only when they reduce the number of 72 junctions. They accomplish this reduction by interchanging a NiNi pair with a nearby AlCo pair.

An alternate means of reducing the frequency of 72 angles between tile edges decorated with Ni atom pairs is to alter the chemical composition. To accommodate the new composition we must relax certain constraints in our simulation. We keep the small scale HBS tiles with Al fixed on their boundaries, but allow arbitrary chemical occupancy of the interior sites. Replacing 20 % of NiNi pairs with AlCo pairs eliminates all defects from the minimum energy configuration and leads to chemical composition Al0.720Ni0.166Co0.114, still within the limits of the basic Ni composition. The low energy configurations consist entirely of HBS tiles decorated as found previously, but now many tile edges that participate in two 72 junctions get decorated with an AlCo pair rather than a NiNi pair (see Fig. 3b).

We compare our model with experimental Z-contrast electron microscope imagery . This experimental method images atomic columns proportionally to the mean square atomic number of the column, so the images translate quite directly into TM positions. A key feature of the experimental data is the occurrence of decagonal rings with a 20 Å diameter. These rings exhibit up to 10 TM doublets around the perimeter, an interior ring of 10 TM singlets, and a central triangular core . This characteristic structure is in excellent agreement with our model, where two hexagons and a boat frequently coalesce into a decagonal cluster (see center of Fig. 3b). The triangular core of this cluster, which breaks decagonal symmetry, is recognized as the sail of the boat tile. Full ab-initio calculations  recently verified energetic favorability of this particular core structure.

Our study began with interatomic potentials plus a minimum of experimental information. We derived structural models starting with a minimally constrained lattice gas on a fluctuating rhombus tiling. Systematically removing unnecessary degrees of freedom yielded a nearly deterministic decoration of HBS tiles at a length scale $`\tau ^2`$ times larger than the initial rhombus tiling, a model consistent with Z-contrast electron microscopy. This procedure can be repeated to identify yet larger characteristic atomic clusters providing a novel example of multiscale modeling which might be applicable to other quasicrystals.

This research was supported by the National Science Foundation and the Department of Energy.