J.

Phys.

France 50

(1989)

3181-3190

1er NOVEMBRE 1989,

3181

Classification Physics Abstracts 61.50E

Icosahedral

quasicrystals

with continuous

phasons

L. S. Levitov
L. D. Landau Institute for Theoretical

Physics,

Moscow

(Reu

le 5

juin 1989, accept le

juillet 1989)

Rsum.

2014

Des familles de modles de

quasi

cristaux

icosadriques

sont construites. Dans ces

modles, les atomes peuvent se dplacer continment sous laction des dplacements dans lespace des phasons R3* leurs distances mutuelles restant toujours plus grandes quun diamtre
de coeur dur h > 0. Ces modles possdent la symtrie de licosadre et leurs diffraction sont celles de structures parfaitement quasi priodiques.

proprits

de

A variety of models for icosahedral quasicrystals is constructed such that atoms move continuously under displacements along the phason space R3*,while their positions are separated by distances larger than some h > 0, a hard core diameter. The models exhibit icosahedral symmetry and the diffraction properties of perfect quasiperiodic structures.

Abstract.

2014

1. Introduction.

For one-dimensional quasiperiodic structures it is known that phasons can be either continuous or discontinuous, depending on the strength of the coupling [1]. These two regimes are separated by a line of analyticity breaking transition. In almost all incommensurate structures studied so far (Hg3 _ sAsF6, TTF-TCNQ, etc.) phasons are continuous. Are continuous phasons possible for quasicrystals ? All models constructed for an ideal quasicrystal structure [2-4] lead to discontinuous phasons, i.e. each atom jumps at certain value of phason shift. It was also suggested [5] that large symmetry groups of quasicrystals always forbid continuous phasons (theorems 1, 2 of Ref. [5]). However, a counterexample to these theorems was reported recently : an icosahedrally symmetric structure with continuous phason transformations [6]. Here 1 return to this problem and construct many other structures having continuous phasons. Results of reference [6] seem to be not completely satisfactory : a) The structure suggested in [6] looks as a very artificially designed, so one might suspect it is unique. b) The model [6] is constructed for only one of 11 possible icosahedral space groups [7-9], but the situation for other 10 groups is also of interest. c) The method of reference [6] refers strongly
Article published online by EDP Sciences and available at http://dx.doi.org/10.1051/jphys:0198900500210318100

3182

geometrical intuition, so for some people a more algebraic approach is desirable. Let us describe shortly the structure of the paper. Main results of this work are concentrated in sections 4, 5, 6. Models with continuous phasons are defined in section 2 as periodic families of non-intersecting continuous atomic surfaces. The contents of section 2 is not new, it almost entirely overlaps with references [5, 6]. Icosahedral symmetry groups are discussed in section 3. It is shown that for constructing continuous atomic surfaces for six of these groups one needs to do this for only one of them. In sections 4, 5 we derive conditions which are necessary for the existence of continuous atomic surfaces. A wide class of solutions of these conditions is found. In section 6 the solutions are used to construct continuous atomic surfaces. An important distinction of the structures constructed here and those described in reference [6] is that here we get straight linear atomic surfaces (hyperplanes in R 6) and periodic interpenetrating lattices of atoms in 1R3, while in reference [6] the atomic surfaces are curved and, thus, atomic positions in (iB3 form quasiperiodically modulated lattices.
Notation : trying to make the matter more transparent 1 almost everywhere use Gothic letters for algebraic objects (groups, (sub-)lattices, subspaces) in order to distinguish them from geometic ones (surfaces, hyperplanes, vectors). By the word hyperplane 1 denote linear manifolds not necessarily containing the origin, in contrast with subspaces that always contain 0-vector.

to the readers

2. Atomic

surfaces, lattices and subspaces.

Atomic surfaces describe the dependence of atoms positions on phason variables. For a ddimensional quasiperiodic structure with D = d + d incommensurate frequencies atomic R d is surfaces live in the space IRD = V 0153 V * (V = IR d represents the physical space, V * the phason space). The surfaces have dimension d. We denote them by si (i labels atoms of the structure). Three characteristic properties of atomic surfaces should be mentioned :
=

The family of the surfaces si is periodic and has D independent periods D-dimensional lattice 2 in RD. This periodicity in RD reflects quasiperiodicity in generating the physical space V. (ii) (conservation of atoms) Each atomic surface si has one-to-one projection on the phason space V *. Thus si can be described by a function fi: V * -+ V as a set of points ( f (y ), y) e RD where standard coordinates in RD are used : (x, y), x e V, y e V *. (iii) (hard core condition) Atoms cannot be closer to each other than by some constant h >- o. In terms of functions fi this restriction reads :1 fi (y ) - f j (y ) 1 >- h for all i,

(i) (periodicity)
a

je Z, y eV*.
Atomic surfaces define positions of atoms in the physical space as follows. Choose some V * (phason parameter) and consider a d-dimensional hyperplane Va consisting of all points (x, a) e IRD, i. e. the space V shifted by the vector (0, a). The hyperplane Va represents the physical space. Atoms positions are given by intersection points of the surfaces si and Va. A family of atomic surfaces satisfying conditions (i), (ii), (iii) together with the rule of finding atoms positions constitute the most general way of describing models for quasiperiodic arrangements of atoms. By varying the phason parameter a in the above given definition on obtains different configurations of atoms. If the space V and the lattice 2 are 0 ]), then all configurations of atoms incommensurate ( [incommensurability ] - [2 n V a are physically equivalent. In this case phason shifts are included in the produced by varying
a e
@
=

3183

group of Goldstone

equivalence

transformations of the structure

(like

translations for

ordinary crystals). It is important that

or

atoms positions as functions of phason shifts can be either continuous discontinuous. Since here we are interested in continuous phasons, let us introduce the

condition (iv) (continuity) All atomic surfaces si (and corresponding functions fi) are continuous. The continuity condition enables one to introduce lattices of periods of single atomic surfaces. For an atomic surface si its lattice li is defined as a sublattice ouf 2 consisting of all translations transforming si into itself. Simple analysis (presented in Ref. [5]) shows that dim (l i) d. Besidesi we need to introduce d-dimensional subspaces ri : ri is a real linear envelope of vectors of li. The subspace ri is parallel to si: si remains within a fixed distance of ri. Both lattices 1i and subspaces ri will be used below.
=

3. Icosahedral symmetry. Icosahedral group acts in (R6 = V (f) V* (V == (R3, V* = (R3*) according to its 3 + 3 representation (see [2-4]). Beginning from here we are interested only in icosahedrally symmetric structures, i. e. we demand that the symmetry group of the family of the atomic surfaces si coincides with one o f 11 icosahedral space groups. All possible icosahedral groups were found in [7-9] (our notation of symmetry groups and related objects coincides with that of Ref. [8]). There are 2 point groups ffi : Y (60 elements, inversion is not included) and YI (120 elements, inversion is present). Their 6-dimensional representations 3 + 3 are point

(thus, d = d 3). Three Bravais lattices are possible : DSC, Fcc, 2BCC. For each pair [0, 2], ((5 = Y, Y,, 2 = 2sc, Spcc. Bcc) two space groups exist symmorphic and non-symmorphic except for the case (5 YI, .2 = Spcc which yields only a symmorphic group. Thus get 11 groups.
symmetry groups of the
-

structures considered

For two groups

H1, h2

we

say that

h1

includes

H2 if H2 is isomorphic to
are

subgroup of

h1.
Proposition 1 : If
two space

symmetry groups

H1, H2

such that

for continuous atomic continuous atomic surfaces.

a) -51 includes H2 ; b) the group -51 allows

Proo f : family

surfaces, then the group

H2 also allows for

Given a family of atomic surfaces with the space symmetry group H1, one easily gets of surfaces with the symmetry group H2 by lowering the symmetry from to (this can be done by a proper continuous small deformation of the surfaces). H1 In what follows we work only with the symmorphic group .!5: (fj Y, L = sc, and construct continuous atomic surfaces for it. One can check that this group includes all groups (both symmorphic and non-symmorphic) with 6) Y, L = .2sc, .2Fcc, 2BCC (totally, 6 groups). According to Proposition 1, the existence of continuous atomic surfaces for these groups is guaranteed by the existence of such surfaces for the group H. Other 5 icosahedral groups (based on (fi YI) will not be discussed here. Due to the presence of inversion not all of them allow for continuous phasons (proof will be reported
a

H2

elsewhere).
4.

Non-transversality condition

and its solutions.

Consider two atomic surfaces sl, s2 and find their lattices ll, l2 and corresponding subspaces rl, r2. Calculate the dimension of r1 p r2, the linear envelope of rl and r2. Note that

3184

= d 3, so if dim ( ri q) r2 ) = d + d 6, then the subspaces r, and i.e. they have only 0-vector in common. In this case the surfaces transversal, r2 si, S2 are also transversal : they intersect and, moreover, their intersection is topologically unremovable (see Refs. [6, 10]). But intersections of atomic surfaces are unphysical they cannot exist due to the hard core condition. Thus, we obtain
dim

( rl )

dim

( r2 )

are

Proposition
ri rj
are

2 :

For every two atomic surfaces si, sj the

corresponding subspaces

not transversal :

For moving further we need to write the non-transversality condition (4.1) in the coordinates (x, y), x e V, y E V *. But first let us see how the subspaces ri can be described using these coordinates. Since for any i e Z dim ( ri ) 3 and ri has one-to-one projection on V*, one can find a linear transformation i : V * - V such that all points of ri are given by (i (y), y), y e V *. After
=

bases

are

chosen in V and

V *, each subspace ri

is

given by

equations :

xa = At/3 y/3
03B2

(03B1, f3 = 1, 2, 3 ), where At/3 is a matrix corresponding to i. Note that x and y live in different spaces (V and V * respectively). Consequently, transformation rules for the matrix At{3 are non-standard : if coordinates are changed by (x, y ) _ (RI (x), R2 (y), then

(here R1, R2 are arbitrary 3 x 3 matrices). Non-transversality condition (4.1) means that ri and rj have a common nonzero vector. Let it be (i (y), y ) _ (j(Y), y). We obtain y y, i (y) j (y), that can be finally rewritten
= =

as

This is Now

geometric restriction (4.1). analysis of the action of the symmetry group -5 on the subspaces ri. Beginning from here we use only orthonormal bases in V and V *. Operations of the point group (5 are given by matrices 6 x 6:
an

algebraic

form of the

we turn

to the

G and Gare 3 x 3 orthogonal matrices of the representations 3 and 3 respectively, is 0-matrix. The set of subspaces ri is symmetric under the point group (4.4), since the surfaces si are symmetric under the space group .5 . Let i be a 3 x 3 matrix connected with ri as explained above. Symmetry implies that not only ri but also other subspaces of the orbit {Rg[ri]} are present. After applying transformation (4.4) to i and using (4.2) get R9 [i] Gi G-1. Non-transversality condition (4.3) thus reads
where
=

3185

Sixty equations (4.5) impose strong constraints on possible matrices i. One solution of equations (4.5) was found in reference [6]. Here we get many other solutions. Proposition 3 : The orthogonal matrices e SO (3 ) solve non-transversality equations (4.5).

Proof : If

SO (3 ) then det
=

det1

since

an

orthog-

1 always has at least one eigenvalue 1 (here is unit matrix). onal 3 x 3 matrix with det One could be interested whether there are other solutions of equations (4.5). Although the whole set of solutions is not known, one can mention a) matrices proportional to orthogonal : , where E R, E SO (3 ) ; b) matrices corresponding to the lattices laf3Y introduced in reference [6]. Probably, other solutions also exist. We are not looking for them here, since orthogonal matrices suffice for our needs.

5.

Rationality of

the

subspaces

ri.

We have constructed a wide class of solutions of non-transversality equations (4.5). However, besides non-transversality there exists another important restriction on the subspaces their rationality. Indeed, r1 is a linear envelope of li, a sublattice of 2. Thus, ri ri is rational, i.e. it is commensurate with 2 ( [rationality ] - [commensurability ] [dim (ri n ) = dim ( ri ) ] ). Let us study which of orthogonal matrices generate rational
-

subspaces.
For this study a special choice of bases in V and V * will be crucial. It turns convenient to work with a cubic coordinate system in which the axes are aligned along 3 perpendicular 2fold symmetry axes of the icosahedral group (for details see Ref. [11] where this system was elaborated upon). The bases in V and V* are chosen so that vectors of the lattice 2sc projected on V and V * have the form

Here h, h,
T
=

k, k,l, f

(J5 + 1 )/2.

are integers such that h + k, k + l Vectors commensurate with sc are given

h, h, k, k, f, f. It

turns convenient to

modify

h are even numbers ; by (5.1) with arbitrary rational representation (5.1) and write vectors of
+

and

R6

commensurate with

Ssc

as

where

(ai , a2, a3 ), b

(bl, b2, b3 ) E R3

have

rational

components : aa, ba

e
=

(a = 1, 2, 3 ). The connection of (5.2) and (5.1) is given by bi = h, b, = k, bi

Let
a
=

l,

explore rationality of ri using representation (5.2). Rationality (E1 (y ), y) means that equations
us

of

vector

can

be solved

simultaneously.

From

(5.3)

find

R (b ),

where

Rationality of the subspace

implies that R is a rational matrix (all its matrix

3186

elements

matrix :

are rational numbers). Another important observation is R E SO (3). This is a direct consequence of two facts : a) Rand commute, hence they have common eigenvectors ;
z -

that

is

an

orthogonal

b) Function into itself.

Thus,
rational

(T 2 Z + 1 )/ (z + T 2) transforms the circle[ z1

to

= 1 in the

complex z-plane

we come

Proposition 4 : Orthogonal matrices generating rational subspaces orthogonal matrices R :

are

parametrized by

large is the set (5.5) of allowed matrices Proposition 5 : Matrices of the form (5.5) are dense in the For the proof of Proposition 5 we need to prove
In order to
see

how

we

prove

group
are

SO (3 ).

Lemma :

Rational

orthogonal
Each matrix

matrices

so (3) f1 GL3(Q)
can

dense in the group

SO (3 ).
Proof of Lemma :
R
E

SO(3)

be written

using

Euler

parametrization

(y, z ) by an angle a (f3, y ). The matrix elements of Tx( a), Ty(f3), Tz( 1) are 1, 0, cos (a ), sin (a ), cos (13 ), sin (f3), cos (y ), sin (y ). It is well known that the angles a for which cos (a ) and sin (a ) are rational numbers are dense in the interval [0, 2 7T] (this is an easy consequence of the existence of infinitely many Pithagoras triplets a, b, c E Z such that az+ bz C2). Since the matrix product (5.6) is continuous as a function of a, /3, y, rational matrices can be found in any vicinity of any matrix of SO (3 ).
Here
a
x
=

TX (a ) (T y ({3 ), T z ( l

is

matrix of rotation around the axis

Proof o f Proposition
R

5 :

Consider

transformation

p :

Applying

the method used above

SO (3) --+ SO (3 ), p () to prove orthogonality

of

we find that p is a continuous one-to-one transformation. From Lemma we know that rational matrices are dense in SO (3 ). But continuous one-to-one image of a dense set is a dense set. Thus we found a wide class (5.5) of orthogonal matrices yielding orbits of non-transversal rational subspaces. Matrices (5.5) will be used in section 6 for constructing a family of icosahedrally symmetric continuous atomic surfaces.

6. Continuous atomic surfaces.

The atomic surfaces discussed here are always linear, i.e. they are hyperplanes. Thus we use the words surface and hyperplane without distinguishing between them. We begin with describing our Basic construction. Choose an orthogonal matrix satisfying (5.5) and a vector a = (xo, yo ) E V # V *. We consider an atomic surface

3187

and apply all surfaces

operations

of the space

group .5 = ffi Q) 2 = Y ffi t sc to s. We get a family of

The main result of this paper

can

be formulated
=

as
an

and the vector a (xo, yo) are appropriately chosen, then icosahedrally symmetric family of surfaces (6.2) satisfies conditions (i), (ii), (iii), (iv)
Theorem : If the matrix
section 2.

of

Proof : Properties (i), (ii), (iv) need no attention, since for all and a the surfaces (6.2) are obviously periodic, continuous and have one-to-one projection on V*. Hence, only the hard core condition (iii) needs special investigation. We perform it in two steps.

(parallel surfaces). For this part of the proof we have to make use of a simple result subspaces : Lemma : Given a subspace r commensurate with the lattice E, one can find a positive constant ho 0 such that for any q E 2 the distance from the point q to the subspace r is either
Step
1
on

commensurate

0 or > h. We leave this easy Lemma without proof. Consider a subgroup of -5 consisting of pure translations belonging to translations to the hyperplane s and get a family of parallel hyperplanes

Esc. Apply

these

We have to prove that the minimal distance. Notation : Denote

hyperplanes (6.3)

either coincide

or are

separated by

constant

by so the hyperplane (6.1) with xo 0, yo 0. Since so contains 0, it is not only a hyperplane but also a subspace of R6. Two hyperplanes s + ql, s + q2 coincide if and only if ql - q2 E so. The lattice 1 [s ] = so n S has dimension 3, since so is commensurate with 2. Elements of factor-group /l [s] label non-identical elements of the family (6.3). Separation of parallel hyperplanes s + ql, s + q2 is equal to the distance between the point ql - q2 and the subspace so. Using the Lemma we find that the hard core condition is true
=

for the surfaces

orbit

(6.3).

Step 2 (elimination of intersections). The family .5 [s 1 (6.2) can be viewd as a 60-element generated by the group Y applied to the family of parallel surfaces (6.3) :

(here
zero

R. has the form (4.4)). For each g e Y the family i?[R9(s)] satisfies the
our

hard

core

condition, whatever and a are chosen in (6.1) (see above). Thus,

goal is to provide non-

separation

of different elements of the orbit

(6.4) :

However, due
one :

to the

periodicity of the family-5

[s ] condition (6.5) can be replaced by a weaker

3188

easily that (6.6) combined with periodicity yields (6.5). Thus we have to choose that the intersections of hyperplanes h (s ) of the family (6.2) are absent. For some satisfying (5.5) we take a 0. Obviously, in this case intersections are present. Try to remove them by varying a. Let two different surfaces si , so belonging to

and
a so
=

One checks

intersect :
above
cannot

Then
a, then

where, according

to the

discussion, gl =F g2. Change

be removed

The intersection

if

We will

see that condition (6.7) has a more convenient representation in terms of the subspace Wl , orthogonal complement to W12. We find

But,

Hence,

W2

has dimension -- 1, it is

spanned by

all vectors

where vectors

u E

are

such that
an

always
reads :
or

has

solution since
au of the form

is

orthogonal 3 x 3 matrix). Rewritten

in terms of vectors

(6.10),

condition

(6.7)

for all au

W 2 given by (6.10).
Taking

Since for all

au from

condition
and

(6.10)

R9n1
or,

and

(6.11) is true (see (b.7)), we obtain from (4.4) get Gi 1 (u ) - GZ 1 (u ) 0 finally,

=
-

Clearly,
are

implies
axes

so

conditions

(6.12)

mean

that both

and

of the icosahedral group Y in the spaces V and symmetry * V of its representations 3 and 3 respectively. Each of these representations has 15 2-fold axes, 10 3-fold axes and 6 5-fold axes totally, 31 symmetry axes. We introduce unit vectors aligned along the axes (a = 1,..., 31 ). We impose the
-

following,restrictions

on

If

(6.13)

g1 =P 92

one can

is true, then (d.l2.i) is not compatible with (6.12.ii) and, hence, for all choose a such that (6.11) is not true. This, in its turn, makes condition (6.7)

3189

false for all gl, 92 (g1 # g2). Thus, all intersections can be removed by a proper choice of a if satisfies (6.13). Note that, due to periodicity, no new intersections will appear if a is sufficiently small. Each of 2 x 312 restrictions (6.13) erases a 1-dimensional curve from the group SO (3), where lives. This is not crucial, since SO (3) is a 3-dimensional manifold and, thus, the forbidden regions have zero measure. We see that, although important, conditions (6.13) are not very restrictive. They enable
one

to choose

so

that all intersections

an

can

be eliminated
matrix

results, orthogonal surfaces (6.1) (6.2) if it satisfies conditions (5.5), (6.13). Then hard core guaranteed by periodicity. The set of good matrices is dense in SO (3 ).
can

To summarize the

properly chosen vector a. generate non-intersecting atomic

by
a

condition is

7. Discussion.

We have constructed a variety of models with continuous phasons for icosahedral tals. The main features of the obtained structures are the following.

quasicrys-

In the physical space V (R3 each family of parallel surfaces (hyperplanes) (6.3) generates atoms positions arranged in a 3-dimensional periodic lattice. The whole family of surfaces (6.2) yields 60 interpenetrating lattices of atomic positions.

(i)

(ii) Diffraction properties of these structures coincide with those of conventional discontinuous models : icosahedral symmetry + perfect 3-peaks. (iii) By lowering the symmetry of the atomic surfaces one can get a structure symmetric under any of 6 icosahedral space groups having point groups (5 Y. The main distinction between continuous and discontinuous atomic surfaces is in the character of phason modes. Phasons exhibit massless diffusive dynamics in the continuous case (observed by scattering of neutrons in Hg3 _ sAsFb and other incommensurate structures). Probably, in the discontinuous case phasons are pinned and give contribution only to statistics but not to dynamics (at least at low temperatures). The results of this work show that both discontinuous and continuous phasons are possible for icosahedral quasicrystals. This enables one to conclude that an analyticity breaking transition between these regimes must exist.
=

Acknowledgements.
1
am

grateful

to P.A.

Kalugin

for his interest and discussions.

3190

References

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