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Physica B 292 (2000) 47}53

Systems with icosahedral clusters: Direct links between atoms


in cluster-recursion methods and DOS spectral "ne structure
H. Solbrig*, C.V. Landauro
Technische Universita( t Chemnitz, Institut fu( r Physik, D-09107 Chemnitz, Germany
Received 21 January 2000; received in revised form 13 March 2000; accepted 13 March 2000

Abstract

The origin of narrow pseudogaps close to the Fermi energy is examined in two model systems: a-AlMn(Si) and
i-AlCuFe (1/1). We show that long-range electronic interferences in the Mn/Fe sub-systems give rise to such narrow
spectral features which are highly important for the electronic transport. Besides the ASA-LMTO and the TB-LMTO
recursion method we employ a cluster-recursion method within the mu$n-tin scattered wave concept which reveals
interference results on arbitrary length scales. We conclude that certain properties of quasicrystals are due to the physics
in chemically de"ned sub-systems.  2000 Elsevier Science B.V. All rights reserved.

PACS: 61.44.#p; 71.10.#x; 71.20.!b

Keywords: Quasicrystals; Density of states; Pseudogaps; Recursion method

1. Introduction a cluster which are electronically active at e should


$
be linked in each recursion step. Otherwise, links to
In the cluster approach to quasicrystals (QC) and adjacent clusters may predominate, and the three-
approximants (AP) [1] certain atomic aggregates diagonalizing basis is driven towards a subspace
(clusters) are treated as building blocks. This im- where cluster interaction has too large a weight.
plies that the properties of QC/AP depend mark- Transition metal atoms with d resonances close to
edly on the cluster electronic structure close to the e are electronically active in this respect.
$
Fermi energy e . Electronic and vibrational prop- Current RM for the electronic density of states
$
erties of such systems are calculated by means of (DOS) of QC/AP [2,3] employ the hamiltonian of
recursion methods (RM) where numerical feasibil- the tight-binding linear mu$n-tin orbital method
ity is achieved upon truncating direct links between (TB-LMTO [4]). The structure constants are
atoms at certain distances. Truncation must be screened, i.e. they suppress direct links to atoms
critical if there are clusters, because all atoms inside beyond roughly 20}40 neighbors (2}3 R ), and,
51
for numerical e$ciency, the hamiltonian should
not be more expanded than e #h!hoh#hohoh.
J
In systems with MacKay icosahedra Al Mn
* Corresponding author. Tel.: #49-371-531-3209; fax: #49-  
371-531-3143. (MI), however, it takes about 250 neighbors for
E-mail address: solbrig@physik.tu-chemnitz.de (H. Solbrig). a Mn atom to `see directlya the other 11 Mn atoms

0921-4526/00/$ - see front matter  2000 Elsevier Science B.V. All rights reserved.
PII: S 0 9 2 1 - 4 5 2 6 ( 0 0 ) 0 0 4 8 9 - 0
48 H. Solbrig, C.V. Landauro / Physica B 292 (2000) 47}53

of the icosahedral shell where it belongs. We believe 2. Models and methods


that direct links at least between the 12 Mn atoms
of each MI are necessary to obtain characteristic We deal with systems where atomic d states close
DOS features close to e . One can even not exclude to e arise from transition metal atoms in icosahed-
$ $
that all links between active atoms must be con- ral clusters. They are called the active atoms, and
sidered. The absence of spectral "ne structure in the we focus on the local DOS at just these atoms.
TB-LMTO RM indicates that the interference of The Elser}Henley model (EHM [9]) describes
direct waves from many distant sources is missing. a-AlMnSi as a BCC-MI lattice with glue atoms.
The range of inter-atomic couplings is also re- 12 Mn atoms occupy the second icosahedral shell
lated to the question whether an atom carries of each MI. There is only one kind of active Mn
a magnetic moment or not. Such issues have been atoms, and they form compact sub-clusters. We
examined for several Al}Mn phases [5,6] by means reduce to two components (unit cell: 114 Al, 24
of the atomic-sphere approximation to the linear Mn). The voids in the EHM are eliminated by
mu$n-tin orbital method (ASA-LMTO [7]) and Monte-Carlo relaxation of the Al glue at 3000
the TB-LMTO RM as well. It turned out that the K (pair potentials [10]). AS radii are calculated by
magnetic moments of Mn atoms depend on rather means of a Voronoi tessellation.
extended environments (radius 5}10 As [6]). This The situation is slightly di!erent with i-AlCuFe
is beyond the scope of the TB-LMTO RM. The (1/1). The Cockayne model [11] is an FCC lattice
present work deals with the origin of narrow of overlapping icosahedral Bergman clusters (BI)
pseudogaps about e . We are necessarily con- with glue (unit cell: 80 Al, 32 Cu, 16 Fe). There are
$
fronted with both the above termination problems, two kinds of active Fe atoms: Each BI has 3 Fe
direct links and continued fractions. Our models atoms inside (the b-Fe), and 4 Fe atoms per unit cell
are hypothetical (1/1) AP of icosahedral QC in the belong to the glue (the g-Fe). A rather open struc-
Al}Mn}Si system and the Al}Cu}Fe system. We ture is thus formed by the active Fe atoms } tri-
proceed as follows: (i) Application of the ASA- angles of b-Fe which are connected by g-Fe.
LMTO. This provides DOS curves to be con- However, in both the above models the active
sidered `correcta for a large system. Moreover, the atoms occupy sets of planes with Fibonacci-like
self-consistent e!ective atomic spheres (AS) are ob- spacings (LSL), and this has proved important in
tained for subsequent use. (ii) Application of the view of the electronic transport [12,13].
TB-LMTO RM. The potential parameters are With the k-space treatment in the ASA-LMTO
transferred from the ASA-LMTO. (iii) Application we rely on reduced simple-cubic special k sets [14].
of an RM within the mu$n-tin scattered wave We employ the set n"3 which includes
(MT-SW) approach [8]. The same AS are em- 2L(2L#2)(2L#4)/48"20 non-equivalent weighted
ployed, but they are now characterized by energy- special k points in the irreducible wedge of the
dependent scattering phase shifts g (e). Structure cubic Brillouin zone. The physical meaning of such
J
constants are long-range in this approach which restrictions is clearly revealed within the Green's-
allows for arbitrary linking schemes. One can in- function approach to the state density: Spurious
crease the range of direct inter-atomic couplings features of the AS DOS in a central unit cell are
which must reveal the critical environments where caused by open scattering paths from beyond a sur-
certain DOS features "rst appear. rounding (cubical) shell of [2(2L!1)#1]!1"
Section 2 outlines the employed models and 3374 unit cells. This means for a-AlMnSi that an
methods. The following two sections present results undistorted periodic environment about the central
with related discussions. We show (Section 3) that unit cell includes 3374;138"4 65 612 atoms,
extended resonances exist in the BCC lattice of much more than both RM can manage with realis-
icosahedral Mn shells in a-AlMn(Si). The corre- tic atoms. The DOS curves thus supplied by the
sponding resonances in i-AlCuFe (1/1) are due to ASA-LMTO can be considered as `correct refer-
the co-operation of two types of Fe atoms (Section ence curvesa. Gaussian broadening (20 meV) of the
4). Conclusions are drawn in Section 5. one-particle energies provides smooth DOS curves.
H. Solbrig, C.V. Landauro / Physica B 292 (2000) 47}53 49

Our implementation of the TB-LMTO RM With respect to the scattering in the cluster, late
works with the expanded hamiltonian H"e # patterns are thus very distant from "02. This is the
J
h!hoh# hohoh where the potential parameters physical reason why the continued fraction (3) can
are transferred from the ASA-LMTO. Local atomic be terminated. Note the di!erence from common
environments are terminated at 3. R which in- TB RM which separate the local physics. The
51
cludes about 42 neighbors. For d-type states, 10 C and the C C in (3) can be calculated
LL L L> L> L
recursion steps are considered with the Beer}Petti- from the moments [8], i.e. the chain vectors are
for terminator [15]. More extended recursion does hidden. Terminators are not employed in the cur-
not improve the spectral "ne structure. rent implementation. The moments become large,
As yet, the DOS of QC/AP has not been cal- especially if the linking scheme is ill-de"ned. Poly-
culated by means of MT-SW RM. A possible ver- nomial-based access to the parameters of the con-
sion [8] calculates the partial DOS of the tinued fraction is thus required.
embedded AS (site R), We present DOS curves at the active atoms
which are obtained from the three approaches men-

 
1 tioned. The "gures are organized as follows: Two
nR (e)"nR (e) 1# Re ¹R R , (1)
J J 2l#1 * * panels on the top show results of the ASA-LMTO
K
(left) and the TB-LMTO RM (right). The panels
from the bare-AS DOS, nR (e), and the diagonal
J arrays below are obtained by means of the MT-SW
back-scattering amplitudes of the environment,
RM. We show the total DOS together with the
¹R "e ERl 1R¸"(I!PF)\P"R¸2e ERl . (2) partial p- and s-DOS curves. Spectral "ne struc-
* R* tures of the ASA-LMTO curves are obviously miss-
¸"(l, m) is the angular momentum. The gR (e) are ing in the TB-LMTO RM. In the array, the panel in
J
the AS scattering phase shifts. F means the bare-AS the nth line of the mth column will be referred to as
scattering matrix of the whole cluster in the P(n, m). Each panel has labels. R10 means that 10
atomic-site angular-momentum representation. recursion levels are included for each partial DOS.
P is the corresponding matrix of the vacuum The other pairs of numbers characterize the linking
propagators. The ¹R R are related to the scatter- schemes. If there is only one pair, such as (5000
Y*Y *
ing-path operator [16]. With C,PF and above 60), a spherical cluster with 5000 atoms
"R¸2,"02 the key inversion problem of multiple about a central atom is considered. Each atom
scattering in (2) can be solved upon three-diagonal- receives waves from its "rst 60 neighbors in this
izing C, cluster. The label (945 above 944) indicates thus
a cluster with 945 atoms where each atom receives
10"(I!C)\C"02 waves from all other atoms. This cluster is com-
1 pletely linked. Two pairs of numbers, such as (600
" above 1000) separated from (4400 above 60), indi-
C C
1!C !   cate that the cluster has again 5000 atoms. How-
 1!C !C C /1!C !2
    ever, in a central sphere with 600 atoms, each atom
!1. (3) receives waves from its "rst 1000 neighbors in the
cluster while the other 4400 atoms in the shell have
In each case, we have C "0, because propaga- only 60 emitter atoms.

tion guides to other atoms. The matrix C is non-
hermitian which means that a two-sided chain
model is required. In detail, a sequence of non- 3. Extended resonances: a-AlMn(Al)
orthogonal incident-"eld patterns is generated to-
gether with the corresponding dual sequence. The The "rst two panels lines of the array in Fig. 1
nth pattern appears after n scattering-propagation belong to systems where all links between atoms
steps, and it contributes for the "rst time to are considered. P(1,1) resembles the TB-LMTO
¹R R (2) after 2n scattering-propagation steps. RM (top right). There is no spectral structure
* *
50 H. Solbrig, C.V. Landauro / Physica B 292 (2000) 47}53

except for d band splitting in pairs of Mn atoms


which are next-nearest neighbors to one another.
Extended recursion, P(2,1), does not supply the
missing "ne structure, cf. ASA-LMTO (top left).
P(1,2) shows how spectral features beyond simple
pair e!ects appear. In the cluster with 250 atoms
the icosahedral Mn shell is completely linked. Res-
onances are generated on this length scale which
gets more pronounced with many recursion steps,
P(2,2). However, even clusters with 945 atoms,
P(1,3), cannot produce the spectral signature of the
interaction between many icosahedral Mn shells as
seen in the ASA-LMTO, because, most shells are
not complete. Deep recursion, P(2,3), or a large
system where long inter-atomic links are omitted,
P(3,1-3), both do not improve the results.
Recently, we have examined the electronic trans-
port in a-AlMn(Al) by means of the Landauer}BuK t-
tiker method [12]. It turned out that the electronic
multiple scattering in the sub-system of Mn atoms
gives rise to narrow, high-resistivity peaks close to
e . Let us try the following generalization: Signi"-
$
cant spectral "ne structure about the Fermi level is
caused by scattering paths which include only Mn
atoms. Scattering paths with Al atoms re-de"ne the
vacuum potential for the multiple scattering in the
Mn sub-system. For proof we omit all Al atoms.
The P(4,1-3) of Fig. 1 present the Mn DOS in such
BCC arrays of icosahedral Mn shells. Note that the
Mn scattering phase-shifts are those of the self-
consistent AS in the ASA-LMTO. In P(4,3) we have
thus the exact contribution made by pure Mn scat-
tering paths in a completely linked system with
138*945/24"5433 atoms. Note also that the
amount of interacting complete icosahedral Mn
shells will be less than 945/12"78 but larger than
in P(1-2,3), of course. The trend towards a single,
narrow pseudogap above e is clearly indicated.
$
Scattering paths with Al shift the band down and
promote the decay of this narrow pseudogap, cf.
ASA-LMTO. The DOS curves in the P(4,1-3) are
Fig. 1. The DOS at Mn in a-AlMn(Al). Top: ASA-LMTO (left), smooth, no spiky features are seen in the complete
TB-LMTO (right). Below: MT-SW recursion method, labels multiple scattering in the large system of icosahed-
explained in Section 2. Panels in (line): all atoms, all links (1-2), ral Mn shells. P(5,1-3) shows how the narrow
all atoms, short links (3), only Mn, all links (4), only Mn, short pseudogap decays if long vacuum-propagation
links (5).
steps are omitted.
Summarizing, we stress that the Mn d orbitals
in a-AlMn(Si) combine and create extended
H. Solbrig, C.V. Landauro / Physica B 292 (2000) 47}53 51

resonances close to e . The electronic transport


$
depends critically on the existence of such small-
scale spectral features [12,13,17].

4. Two types of active atoms: i-AlCuFe-(1/1)

We demonstrate (i) that Fe-based extended res-


onances are formed with all consequences de-
scribed in the former section, and (ii) that this is
accomplished by the co-operation between b-Fe
and g-Fe. The resonances exist on the whole Fe
network.
In Fig. 2 (b-Fe) and Fig. 3 (g-Fe) the spectral
curves are shown. There are many di!erences be-
tween b-Fe and g-Fe, even with respect to the Cu
signature at Fe atoms which is much stronger at
b-Fe (Fig. 2). Among its "rst 12 neighbors
each b-Fe has 4 Cu whereas g-Fe has none in this
shell.
Typical spectral "ne structures of the ASA-
LMTO curves appear in the MT-SW RM quite
continuously between 120 and 150 atoms per clus-
ter, P(1,1-3), because there are no compact Fe sub-
clusters in the present case. Provided the system is
large enough and all links are considered, the
curves can be improved by extended recursion,
P(2,1-3). The P(3,1-3) show results for large systems
without including long inter-atomic links: No nar-
row psudogaps are seen at e , but a trend towards
$
spurious features is to be noted, most pronounced
on the low-energy side of the Fe d band where the
coupling with the Cu sub-system must be strong,
P(3,2) of Fig. 2. The situation resembles a-AlMn(Si)
where Mn resonances extend throughout the sys-
tem above e . The corresponding can be proved
$
valid with the Fe sub-system. P(4,1-3) of Figs. 2,
3 belong to systems where both Al and Cu are
omitted. Particularly at the b-Fe, the narrow
pseudogap slightly above e is very deep. Again,
$
this kind of pseudogap decays if long inter-atomic
links are not considered (cf. a-AlMn(Si), Fig. 1, Fig. 2. The DOS at b-Fe in i-AlCuFe (1/1). Top: ASA-LMTO
P(5,1-3)). The question remains if the resonances (left), TB-LMTO (right). Below: MT-SW recursion method,
are really supported by both kinds of Fe atoms, i.e. labels explained in Section 2. Panels in (line): all atoms, all links
the whole Fe network. We prove it in P(5,1-3) of (1-2), all atoms, short links (3), only Fe, all links (4), only b-Fe, all
links (5).
Figs. 2 and 3 where only the b-Fe and the g-Fe,
respectively, participate. The narrow pseudogaps
are clearly missing.
52 H. Solbrig, C.V. Landauro / Physica B 292 (2000) 47}53

Summarizing, we state that the resonance is nei-


ther a b-Fe resonance nor a g-Fe resonance. The
`quasi-gapa of P(4,3) indicates that the driving force
of the resonance process may be localized at the
b-Fe, but the links via g-Fe are required to become
really an extended resonance on the Fe network.

5. Conclusions

We examine narrow pseudogaps close to the


Fermi energy in the one-particle electronic spec-
trum of two model systems (a-AlMn(Al) [9], i-Al-
CuFe (1/1) [11]). Three methods are employed, the
ASA-LMTO super-cell method, the TB-LMTO re-
cursion method, and a recursion method within the
mu$n-tin scattered-wave approach. Only the latter
one is capable of revealing narrow spectral features
in large, non-periodic clusters. It turns out that
transition metals with e!ective-atom resonances
close to the Fermi energy give rise to resonances
which extend throughout the system. Active atoms
in this respect form arrays of separate clusters (Mn
in a-AlMn(Si)) or rather open networks (Fe in i-
AlCuFe (1/1)). Pseudogaps below the 1 eV scale in
the state density curves at active atoms are caused
by scattering paths which include only active
atoms. Other components such as Al promote the
decay of the resonances in the active sub-systems
and re-de"ne the vacuum level. All this has conse-
quences for the electronic transport in distorted
quasicrystals where the Fermi energy can be shifted
away from the self-consistent position in the ideal
system towards such narrow pseudogaps. The main
conclusion is that emphasis should be put on chem-
ical aspects. Certain properties of quasicrystals may
arise from electronic processes in sub-systems.

Acknowledgements

This work is supported by the Deutsche For-


Fig. 3. The DOS at g-Fe in i-AlCuFe (1/1). Top: ASA-LMTO schungsgemeinschaft.
(left), TB-LMTO (right). Below: MT-SW recursion method,
labels explained in Section 2. Panels in (line): all atoms, all links
(1-2), all atoms, short links (3), only Fe, all links (4), only g-Fe, all
links (5). References

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