PHYSICAL REVIEW B VOLUME 55, NUMBER 14 1 APRIL 1997-II

Boundary-condition effects in anharmonic lattice dynamics: Existence criteria

for intrinsic localized modes from extended-mode properties
D. Bonart,* T. Rössler, and J. B. Page
Department of Physics and Astronomy, Arizona State University, Tempe, Arizona 85287-1504
~Received 20 August 1996; revised manuscript received 26 November 1996!
Recent theoretical studies of periodic one-dimensional anharmonic lattices with standard periodic boundary
conditions established fundamental connections between the existence of intrinsic localized modes ~ILM’s! and
the stability of the extended lattice modes into which they evolve with decreasing amplitude. While the
odd-order anharmonicity drops out of the equations of motion for the extended modes within these boundary
conditions, it nevertheless produces an amplitude-dependent period-averaged ‘‘dynamical stress’’ across the
supercell boundaries. Here, we allow the supercell length to adjust so as to eliminate this stress and find that
the frequency vs amplitude curves for the anharmonic extended modes are markedly changed for a variety of
realistic nearest-neighbor interactions, whereas highly localized ILM’s are little affected. Nevertheless, in all
cases ILM existence remains intimately connected to an instability of the associated extended mode. Further-
more, the use of zero-stress periodic boundary conditions now allows one to predict the spatial extent of an
ILM from extended-mode stability properties in lattices with odd-order anharmonicity. Most importantly, for
the zero-stress periodic boundary conditions we obtain an additional ILM existence criterion, based on simple
dynamical properties of the unperturbed related extended mode. Since well-localized ILMs are independent of
the specific choice of boundary conditions, our results yield promising tools for ILM predictions in real
systems. @S0163-1829~97!01014-X#

I. INTRODUCTION The studies of Ref. 6 used standard periodic boundary

In striking contrast to the familiar plane-wave vibrational
excitations in harmonic periodic lattices, it is known theoreti-
cally that lattices with nonlinear interactions can support
highly localized stationary vibrations.1,2 These so-called ‘‘in-
trinsic localized modes’’ ~ILM’s! can be centered on any site
and are optic-mode-like, in that adjacent particles move p
out of phase. In the low-amplitude limit, ILM’s broaden spa-
tially and for some cases reduce to stationary envelope soli-
tons of the sort described more than 20 years ago for weakly
anharmonic one-dimensional lattices,3,4 whereas such a de-
scription does not apply for large-amplitude highly localized
ILM’s.5 These unusual excitations have elicited numerous
studies over the last several years, most of which are focused
on one-dimensional ~1D! lattices and employ a mixture of
analytic techniques and direct numerical simulations. Vari-
ous aspects of ILM’s are surveyed in Ref. 2.
For the experimental establishment of ILM’s, it is impor-
tant to develop practicable existence criteria. Reference 6
obtained a fundamental connection between the existence of
ILM’s and the stability of the extended lattice modes
~ExM’s! into which they spatially broaden with decreasing
amplitude. Monatomic lattices were studied, for interactions
ranging from simple quadratic plus quartic nearest-neighbor
potentials (k 2 ,k 4 ) to realistic full potentials V(r), e.g., Born-
Mayer plus Coulomb, Lennard-Jones, etc. It was concluded
that for a given mode amplitude, ILM’s only exist when their
associated ExM’s are dynamically unstable with purely real
instability growth rates. The practical significance of this re-
sult is that the stability analysis is a linear problem and is
therefore simple to implement as a useful prelude to the
more difficult problem of direct numerical searches for
ILM’s.
conditions, in which the supercell length Na is fixed. Here
N is the number of particles and a is their equilibrium spac-
ing. These boundary conditions are ubiquitous in solid-state
physics and are convenient for ‘‘bulk’’ properties, i.e., those
which are independent of the detailed nature of the bound-
aries. This should hold for ILM dynamics, provided the
modes are highly localized relative to Na. However, the as-
sociated anharmonic ExM’s will be shown here to be af-
fected by the boundary conditions in a nontrivial manner, in
contrast to the situation in harmonic lattices, raising the
question of the role of boundary conditions in the ExM-ILM
interrelations detailed in Ref. 6. In the following we use
more general periodic boundary conditions to study these
connections, and we will show that the earlier results are
generalized in interesting and often unexpected ways. More-
over, we will obtain a second ILM existence criterion based
on properties of the ILM’s associated ExM. This criterion is
not based on stability properties and is complementary to the
first. It appears promising for the a priori prediction of ILM
existence in real systems.
To better motivate the generalized periodic boundary con-
ditions, we next outline some additional quantitative aspects
of the results of Ref. 6. Within specific models, it was shown
that the ExM stability analysis can go beyond ILM existence
prediction and yield quantitative information about ILM lo-
calization. For the monatomic lattices studied there, the rel-
evant ExM is the zone boundary mode ~ZBM!, in which
adjacent particles have equal and opposite displacements.
This mode’s spatial periodicity allows a Fourier decomposi-
tion of the instability perturbations, with the result that the
wave vector of the fastest-growing perturbation introduces a
characteristic length scale. For the simple case of nearest-
neighbor (k 2 ,k 4 ) interactions, the ZBM is unstable and

0163-1829/97/55~14!/8829~18!/$10.00 55 8829 © 1997 The American Physical Society

8830 D. BONART. T. RÖSSLER, AND J. B. PAGE
ILM’s exist at all amplitudes, and the ZBM instability length
scale matches the spatial width of the ILM having the same
frequency as the ZBM. Moreover, finite-time molecular dy-
namics ~MD! simulations showed that the unstable ZBM
evolves with time into a periodic array of localized excita-
tions having the same frequency as the original ZBM, but
larger amplitudes. Note that the finite-time MD simulations
justify making the above length-scale comparison at the
same ZBM and ILM frequency. This comparison is facili-
tated by the fact that the ZBM instability and the ILM exist
over identical frequency ranges.
Real interatomic potentials are dominated by cubic anhar-
monicities, and it was also shown in Ref. 6 that the addition
of nonzero k 3 changes the detailed manner in which the
above existence criterion is realized: in monatomic
(k 2 ,k 3 ,k 4 ) lattices with realistic parameter values, ZBM in-
stability and ILM existence occur above a finite threshold
amplitude, below which the ZBM is stable and ILM’s are not
found. The ZBM instability perturbation again introduces a
characteristic length scale, but quantitative comparisons with
the corresponding ILM length scales are now difficult, for
two reasons: ~1! for the standard periodic boundary condition
lattices studied in Ref. 6, the frequency ranges of the un-
stable ZBM’s and the corresponding ILM’s no longer fully
coincide and ~2! finite-time MD runs show that the unstable
ZBM’s again break up into periodic arrays of localized ex-
citations, but the frequencies as well as amplitudes change in
the process. The underlying cause of these differences from
the (k 2 ,k 4 ) case is the amplitude-dependent local static dis-
tortion which accompanies ILM’s in lattices with nonzero
k 3 ,7 and the effect is to prevent the simple length scale com-
parison outlined above.
Within the standard periodic boundary conditions of Ref.
6, the symmetry of the ZBM displacement pattern renders
the mode’s equation of motion independent of odd-order an-
harmonicity. Nevertheless, such anharmonicity strongly af-
fects the mode’s instability properties, owing to the symme-
try breaking introduced by the instability perturbations.
Moreover, even without an instability perturbation, the ZBM
in a lattice with odd-order anharmonicity sets up a ‘‘dynami-
cal stress,’’ i.e., a nonzero period-average force across any
imaginary plane perpendicular to the chain. Its presence in a
real lattice would drive a uniform expansion, dependent on
the ZBM amplitude, such that the dynamical stress vanishes.
The consequences of such a condition will be studied here,
by allowing the supercell length to change with mode ampli-
tude such that the dynamical stress remains zero. We will
call these boundary conditions ‘‘zero-stress periodic bound-
ary conditions’’ ~ZSPBC’s!, in contrast to the standard peri-
odic boundary conditions ~StdPBC’s! used earlier. Employ-
ing ZSPBC’s rather than free-end boundary conditions
preserves the simplicity of the ILM-related anharmonic
ExM’s, permitting both a meaningful comparison with the
StdPBC case and, more importantly, an extension of the
ExM instability/ILM length-scale comparisons outlined
above to the case of nonzero k 3 . Since the properties of
well-localized ILM’s are independent of the boundary con-
ditions, the use of numerical model studies of ExM’s within
the ZSPBC’s to predict ILM existence and properties tran-
scends these boundary conditions and is thus applicable to
real systems.
55
We will discuss 1D diatomic lattices with nearest-
neighbor potentials. Our numerical studies will be detailed
for the case of (k 2 ,k 3 ,k 4 ) interactions, with parameter val-
ues appropriate to realistic potentials. Results for other cases,
such as full potentials V(r), or the monatomic limit, will be
given at appropriate points. Several studies of ILM’s in 1D
diatomic lattices have been carried out ~see Refs. 8–10!.
Here, our focus is on the effects of boundary conditions on
ExM-ILM interrelations, and it turns out that the
(k 2 ,k 3 ,k 4 ) diatomic lattice offers a particularly fruitful
model system, exhibiting a richer variety of ExM-ILM be-
havior than does a model using full potentials. Indeed, the
results for full potentials are readily discussed within the
context of the results obtained here. In addition, we will see
that the (k 2 ,k 3 ,k 4 ) model studies reveal an interesting and
unexpected ILM spatial broadening behavior as the mode
amplitude is changed.
It is customary to classify ILM’s according to whether
their frequencies are above the maximum harmonic fre-
quency of the lattice or are within the gap between the acous-
tic and optic harmonic phonon bands. However, we will see
that for either of the periodic boundary conditions to be used
here, this classification is not clear cut, e.g., ILM’s can occur
within the harmonic phonon bands. We feel that the more
useful classification is in terms of the ILM’s associated ExM.
Thus we will discuss ‘‘optical zone center mode’’ ILM’s,
which broaden into an anharmonic ExM having the pattern
of the harmonic k50 optic phonon mode, and ‘‘optical zone
boundary mode’’ ILM’s, which broaden into an anharmonic
version of the harmonic k5 p /2a optical zone boundary
mode. These two classes exhibit quite different behaviors,
and it is important to consider them both. The results of Ref.
6 are recovered from the StdPBC results for the first class, in
the monatomic limit.
The following section describes our theoretical frame-
work, after which we discuss boundary conditions and define
dynamical stress. Our numerical results are detailed in Sec.
IV, which is split into two parts according to the ExM in-
volved. We first consider the anharmonic optical zone center
mode, discussing its dynamics, stability and related ILM be-
havior, after which the same topics are discussed for the
anharmonic optical zone boundary mode. Section V com-
prises a detailed discussion and synthesis, including the ad-
ditional existence criterion mentioned earlier. The paper is
concluded in Sec. VI, and two appendices provide additional
details.
II. THEORETICAL BASIS
We discuss longitudinal motion in a 1D lattice of particles
having anharmonic interactions V(r) between nearest neigh-
bors. For an infinite lattice, the Hamiltonian is
H5 (n F p 2n
2m n
G
1V ~ r n 2r n21 ! , ~1!
where $ m n % gives the masses and $ p n (t) % and $ r n (t) % are the
instantaneous momenta and positions. We will mainly con-
sider diatomic lattices of alternating masses m and M .m,
and V(r) is either a full potential such as Born-Mayer plus
55 BOUNDARY-CONDITION EFFECTS IN ANHARMONIC . . .
Coulomb ~BMC!: V(r)5le 2r/ r 2q 2 /r, or the corresponding
fourth-order Taylor series expansion:
1 1 1 is independent of the lattice site, i.e., F̄ n,n21 [F̄.
V ~ r ! 5V ~ a ! 1 k 2 ~ r2a ! 2 1 k 3 ~ r2a ! 3 1 k 4 ~ r2a ! 4 .
2 3 4
~2!
Here a is the static-lattice nearest-neighbor equilibrium sepa-
ration, obtained by minimizing the total potential energy. For
our assumption of nearest-neighbor interactions, a occurs at
the minimum of V(r).
To treat a finite lattice of N particles, we will use periodic
boundary conditions r n1N 5r n 1L, where L is the repeat
length; these are realized in Eq. ~1! by summing n from 1 to
N and defining r 0 [r N 2L. A major focus of this paper is on
the effects of dynamically induced changes of L in anhar-
monic lattices. Thus L will generally not be equal to its static
equilibrium value Na. In passing, we note that free-end
boundary conditions would correspond to r 0 [r 1 2a.
As discussed in previous work,2,6 the ‘‘rotating wave ap-
proximation’’ ~RWA! has proven convenient for giving ac-
curate stationary solutions to the equations of motion derived
from Eq. ~1!, for both spatially extended and localized an-
harmonic modes. In the RWA, the motion of particle n is
assumed to be of the form
r n ~ t ! 5c n cos~ v t ! 1b n 1na.
After inserting this ansatz into the equations of motion, we
multiply the resulting equations by either cos(vt) or unity
and average over a single period. This yields a system of
2N coupled nonlinear equations for the dynamic displace-
ments $ c n % and the static displacements $ b n % :
E
1 2p
05m n v 2 c n 2 d f cosf @ V 8 ~ r n 2r n21 !
p 0
2V 8 ~ r n11 2r n !# ,
052
1
2p
E0
2p
d f @ V 8 ~ r n 2r n21 ! 2V 8 ~ r n11 2r n !# ,
where f 5 v t and V 8 (r n 2r n21 )[(dV/dr) u r5r n 2r n21 . Once
the boundary conditions are specified, these equations can be
solved using standard numerical routines; the solutions in
conjunction with Eq. ~3! constitute the RWA. Wherever pos-
sible we will compare our RWA predictions with results ob-
tained by direct MD simulations of the full equations of mo-
tion for the Hamiltonian ~1!, using a fifth-order Gear
predictor-corrector method.11
For future reference we note that Eq. ~4b! can be rewritten
05F̄ n,n21 1F̄ n,n11 ,
where F n,m is the force on particle n due to particle m and
the overbar indicates a time average over a mode period.
This equation is actually independent of the RWA, as is eas-
ily seen: the right-hand side of Eq. ~5! is proportional to the
time-integral of the total force on a particle over one period,
and is thus proportional to the corresponding momentum
8831
change, which vanishes for any periodic motion. Moreover,
since F̄ n,n11 52F̄ n11,n , we see from Eq. ~5! that the time-
average force on a particle due to either one of its neighbors
The preceding discussion applies both to localized and
extended stationary modes. We now focus on ExM’s which
have the same dynamic displacement patterns with and with-
out anharmonicity present. In particular, for a diatomic lat-
tice we study the anharmonic versions of the harmonic
k50 optical zone-center mode ~OZCM! and the
k5 p /2a optical zone-boundary mode ~OZBM!. The
respective dynamic displacement patterns $ c n % are
A( . . . ,1,2m/M ,1,2m/M , . . . ) and A( . . . ,1,0,21,0,1,0,
21,0, . . . ), with A being the amplitude of the light particles
in each case. In some instances we will also give our OZCM
results for the case M 5m of a monatomic lattice; the static
equilibrium lattice constant is then a rather than 2a and the
mode is the monatomic lattice ZBM, with the dynamic dis-
placement pattern A( . . . ,1,21,1,21, . . . ).
With anharmonicity present, each of the above three ExM
dynamic displacement patterns can produce static displace-
ments consisting of just a simple uniform expansion of the
lattice, for a broad class of realistic potentials and a large
range of dynamic displacements. Indeed, we note that for all
three modes, the relative dynamic displacements
Dc n [c n 2c n21 between adjacent particles can be written as
~3! Dc n [(21) n 2Ã, where à is an effective mode amplitude,
given by (11m/M )(A/2), A/2, and A, for the diatomic
OZCM, the diatomic OZBM, and the monatomic ZBM, re-
spectively. Within the RWA we then obtain
F̄ ~ Ã ! 52
1
2p
E 2p
d f V 8 ~ 2Ãcosf 1Db n 1a ! , ~6!
0
where Db n [b n 2b n21 gives the relative static displace-
ments. Since we have seen that F̄ is independent of n, the
~4a! right-hand side of Eq. ~6! cannot depend on n. A simple
uniform expansion Db n [D satisfies this constraint. To
check for other possible static displacement patterns, we as-
sume that Db n is a continuous function of à and that the
~4b! interparticle potential V(r) has only a single minimum ~at
r5a). It can then be shown that for standard realistic poten-
tials ~e.g., BMC, Lennard-Jones!, the relative static displace-
ments Db n cannot be site dependent over a large range of
dynamic displacements; specifically, they are site indepen-
dent for 2Ã1D(Ã)<0.30a ~see Ref. 12!. Accordingly, we
will only consider uniform expansions a→â5a1D when
discussing the three ExM’s described above. The specific
functional dependence D(Ã) depends on the choice of
boundary conditions, as discussed in the following section.
~5! III. BOUNDARY CONDITIONS
AND DYNAMICAL STRESS
For bulk properties of lattices, it is traditional and conve-
nient to employ Born-von Karman periodic boundary condi-
tions. As noted above, we do this by requiring
r n1N 5r n 1L for an N-particle lattice, where L is the repeat
length. For purely harmonic vibrations, the repeat length is
8832 D. BONART. T. RÖSSLER, AND J. B. PAGE
just the static lattice value Na, but with anharmonicity
present, we will allow L to vary, contrasting the results so
obtained with those for L5Na.
A. Standard periodic boundary conditions
Standard periodic boundary conditions with L fixed at
Na are denoted as StdPBC’s, whether they are applied to
harmonic or anharmonic lattices. For the solution of Eqs. ~4!
within the RWA, these are realized by setting c n1N 5c n and
b n1N 5b n . StdPBC’s were employed throughout our earlier
study of the interrelations between ILM’s and ExM’s in Ref.
6.
As discussed in Sec. II, for an anharmonic lattice vibrat-
ing in any of the three ExM’s introduced there, the relative
static displacements Db n 5D are site independent. Hence for
StdPBC’s, D vanishes identically, and the period-average
separations of adjacent particles remain equal to the static
equilibrium value a, even with one of these ExM’s present.
An additional consequence of the StdPBC’s is that the
odd-order terms of the Taylor series of the interaction poten-
tial do not occur in the equations of motion for any of the
three ExM’s. This follows directly from Eq. ~4a! and the
symmetry of the mode patterns, as shown explicitly in Ap-
pendix A.
B. Dynamical stress and zero-stress periodic
boundary conditions
With vibrations present in our 1D system, and for the case
of general two-body interactions, we define the dynamical
stress across an imaginary plane to be the period-average
force on the particles on one side due to the particles on the
other side. For the present case of interactions restricted to
nearest neighbors, this quantity is just the period-average
force on a particle due to one of its nearest neighbors. Note
that in addition to the forces between particles that move, our
definition of dynamical stress includes the forces between
particles which are essentially at rest, e.g., between adjacent
particles far from the center of a highly localized ILM. If the
interaction potential contains only positive terms of even or-
der, there are no static displacements and no dynamical
stresses, and the StdPBC’s are appropriate for ILM’s and the
ExM’s we are treating. However, for realistic full potentials,
e.g., BMC, Lennard-Jones, or Morse, the odd-order terms are
important, and they result in nonzero dynamical stress across
the supercell boundary for StdPBC’s. For the case of highly
localized ILM’s, this stress vanishes in the N→` limit of a
large number of particles, but for the ExM’s, it does not.
Accordingly, with odd-order anharmonicity present, we
modify the StdPBC’s by allowing the periodicity length L to
vary such that the dynamical stress vanishes across the su-
percell boundary. As a result L is changed from its static
equilibrium value Na to a value which depends on the am-
plitude and nature of the mode ~ILM or ExM!. As noted in
the introduction, these zero-stress periodic boundary condi-
tions are abbreviated ZSPBC’s. For the solution of Eqs. ~4!
within the RWA, they are implemented by setting
c n1N 5c n and b n1N 5b n 1L2Na.
With one of our three ExM’s present, the ZSPBC’s deter-
mine D(Ã) and hence the nearest-neighbor distance as a
55
function of the mode amplitude: â(Ã)5a1D(Ã), with the
functional form depending on the particular mode. Such
changes in the lattice constant for the case of small-
amplitude ExM’s in monatomic (k 2 ,k 3 ,k 4 ) lattices have
been included in Refs. 4 and 13. Here, we will show that the
ZSPBC’s alter the interrelations between ILM’s and ExM’s,
compared with the StdPBC results obtained in Ref. 6.
In Appendix B, it is shown that the ZSPBC’s follow from
minimizing the period-average supercell potential energy.
Thus they are a dynamical analog to the use of periodic
boundary conditions in computing the equilibrium lattice
constant, where one would minimize the static potential en-
ergy of the supercell.
Similar to a lattice with ZSPBC’s, a lattice having free
ends would allow for a relaxation of the dynamical stress by
static distortion. However, the presence of free ends breaks
the periodicity, so that the simplicity of the ExM mode pat-
terns is lost, preventing a straightforward comparison of the
ExM-ILM interrelations for zero and nonzero dynamical
stress. Moreover, we find that the lack of a common ampli-
tude range for the free-end ExM’s and ILM’s prevents us
from obtaining useful ExM-ILM results of the sort obtained
here using ZSPBC’s. Nevertheless, in the limit of highly
localized ILM’s, the ZSPBC’s and free-end boundary condi-
tions become equivalent. Hence the latter can be used in MD
simulations of these modes, allowing one to avoid the diffi-
cult task of implementing the zero-stress condition in MD.
IV. RESULTS
We have studied the interrelations between ILM’s and the
anharmonic ExM’s introduced in Sec. II, as a function of the
periodic boundary conditions and for a wide variety of inter-
actions in diatomic lattices. Many of the results are qualita-
tively similar for realistic full potentials and their
(k 2 ,k 3 ,k 4 ) series expansions. Moreover, the latter case often
allows one to proceed further analytically, and it yields a
more diverse range of ExM-ILM behavior. Since the results
for full potentials are easily described within the context of
the (k 2 ,k 3 ,k 4 ) results, we will detail the latter case, pointing
out important differences and similarities for full potentials.
Unless explicitly stated otherwise, we take k 3 a/k 2 5210,
k 4 a 2 /k 2 550, and m/M 51/4. These force constant ratios are
appropriate for realistic potentials and were used in our ear-
lier studies for StdPBC’s in monatomic systems.6 Further-
more, the corresponding (k 2 ,k 3 ,k 4 ) potential function has
only a single minimum, as is the case for realistic full poten-
tials. Frequencies will be given in terms of the k50 har-
monic frequency v max 5 A2k 2 mM /(m1M ).
A. Optical zone center mode and related ILM’s
1. Dynamics of the OZCM
a. Standard periodic boundary conditions. As shown in
Appendix A, k 3 plays no role in the dynamics of the OZCM
within StdPBC’s, owing to the symmetry of the dynamic
displacement pattern. The RWA frequency is determined by
S D
v StdPBC 2 k4
5113 Ã 2 , ~7!
v max k2
55 BOUNDARY-CONDITION EFFECTS IN ANHARMONIC . . .
FIG. 1. Frequency vs amplitude curves for the optical zone-
center mode ~OZCM! and the related intrinsic localized mode
~OZCM-ILM! in a 40-particle diatomic (k 2 ,k 3 ,k 4 ) lattice, for the
parameter values given in the text. The frequency and amplitude are
scaled to the maximum harmonic lattice frequency v max and the
static lattice nearest-neighbor distance a, respectively. The solid
curves ~a! and ~a 8 ) are for the OZCM with standard periodic
boundary conditions ~StdPBC’s! and zero-stress periodic boundary
conditions ~ZSPBC’s!, respectively. The dashed curves ~b! and
~b 8 ) are for the OZCM-ILM’s under the same two boundary con-
ditions. For these ILM curves the plotted amplitudes are those of
the mode’s central particle, which is a light mass. The thin horizon-
tal lines locate the top and bottom of the harmonic optical phonon
band, indicated by the vertical bar. The top of the harmonic acoustic
band is at v 50.45v max , below the range of the graph. The crosses
and open circles are the results of MD measurements of mode fre-
quencies for StdPBC’s and free-end boundary conditions,
respectively—for well-localized ILM’s, free ends should give the
same results as ZSPBC’s, and our MD measurements and RWA
predictions differ by 2% at most. The two diamonds give the pre-
dicted thresholds above which the OZCM is unstable for each of the
two periodic boundary conditions. Note that these thresholds are
also the points where the two ILM curves join the OZCM curves.
where Ã5(11m/M )(A/2) and A is the amplitude of a light
mass. Hence for StdPBC’s, the OZCM frequency increases
monotonically with amplitude starting from v max , as shown
by the solid line ~a! in Fig. 1. This curve is the diatomic
lattice version of the solid curve in Fig. 8 of Ref. 6, which is
for a monatomic (k 2 ,k 3 ,k 4 ) lattice—recall that in the mon-
atomic limit the diatomic OZCM becomes the monatomic
ZBM. For the case of realistic full potentials, the OZCM
v (A) curve exhibits the same qualitative behavior.
b. Zero-stress periodic boundary conditions. In contrast,
when ZSPBC’s are used, the OZCM produces a changed
period-average nearest-neighbor distance â(Ã)5a1D(Ã).
The requirement of vanishing dynamical stress yields an
equation for D(Ã):
D1
k3 2 k4 3
k2
D 1 D 12Ã 2
k2
k3
k2
k4
S
13 D 50.
k2 D ~8!
Since we do not consider double-well potentials, the only
solution of this equation for Ã50 is D50. One can show
analytically that with increasing amplitude, D remains
8833
FIG. 2. Fractional lattice constant change D/a vs normalized
amplitude A/a of the OZCM for the 40-particle diatomic lattice of
Fig. 1, with ZSPBC’s. The dashed line corresponds to the large-
amplitude asymptotic value D ` 52k 3 /3k 4 . This graph also applies
to the optical zone boundary mode ~OZBM!, provided the abscissa
values are multiplied by (11m/M ); the value of D ` is the same for
both modes.
unique. For the k 3 ,0 case considered here, D increases
monotonically, eventually saturating at an asymptotic value
given by D ` 52k 3 /3k 4 . This behavior is shown in Fig. 2.
Relative to the new equilibrium positions, the force constants
are renormalized according to k̂ 2 [k 2 12k 3 D13k 4 D 2 ,
k̂ 3 [k 3 13k 4 D and k̂ 4 [k 4 . Note that k̂ 3 goes to zero as D
approaches its saturation value. An earlier study14 showed
that the application of static external stress of the right mag-
nitude to a finite diatomic (k 2 ,k 3 ,k 4 ) lattice can produce a
static strain which eliminates cubic anharmonicity. The lat-
tice constant change predicted there is just D ` , which is
produced here by the presence of a large-amplitude OZCM.
Equation ~7! for the OZCM also applies for ZSPBC’s,
provided the force constants are replaced by their renormal-
ized versions given above. Thus the RWA squared frequency
for ZSPBC’s can be expressed as
S D
v ZSPBC 2 k̂ 2 k̂ 4 k3 k4
5 13 Ã 2 5112 D13 ~ D 2 1Ã 2 ! ,
v max k2 k2 k2 k2
~9!
which, of course, can also be derived directly. From Eq. ~8!,
we find that D522Ã 2 k 3 /k 2 for small amplitudes. The cor-
responding limit for the squared frequency is
( v ZSPBC / v max) 2 511(3k 4 /k 2 ) @ 124k 23 /(3k 2 k 4 ) # Ã 2 ~see
Ref. 15!. We can thus distinguish two kinds of small-
amplitude behavior: for 4k 23 /(3k 2 k 4 ),1 the frequency in-
creases with amplitude, while for 4k 23 /(3k 2 k 4 ).1 it de-
creases. For our force constants, this quantity is equal to
8/3, and we will thus focus on the second case, although
some pertinent results for the first case will be summarized
in Sec. V. For small amplitudes, then, the frequency of the
OZCM moves downward into the harmonic optical phonon
band, as shown by curve ~a 8 ) in Fig. 1. With increasing
amplitude, the positive term 3(k 4 /k 2 )(D 2 1Ã 2 ) in Eq. ~9!
gains importance, and at A50.063a the frequency reaches a
8834 D. BONART. T. RÖSSLER, AND J. B. PAGE
minimum value of v 50.91v max , beyond which it increases
monotonically. In contrast, for realistic full potentials V(r),
the presence of higher-order terms is found to prevent this
bottoming out, and the OZCM frequency descends through
the harmonic optical phonon band into the phonon gap.
Comparing the solid curves ~a! and ~a 8 ) in Fig. 1, we see
that the relaxation of the dynamical stress lowers the OZCM
frequency for a given amplitude. Furthermore, the zero-stress
OZCM has the lower energy at a given amplitude, as ex-
pected since the ZSPBC’s follow from minimizing the
period-average potential energy at a fixed amplitude ~Appen-
dix B!.
2. Stability of the OZCM
We have examined the stability properties of the
(k 2 ,k 3 ,k 4 ) OZCM using the RWA stability analysis de-
scribed in Refs. 6 and 16, with the result that the qualitative
stability properties are the same for the two types of periodic
boundary conditions. The stability analysis assumes infini-
tesimal displacement and phase perturbations having expo-
nential time dependence exp(lt), leading to an eigenvalue
problem for the growth rates $ l % . Instabilities correspond to
l’s with positive real parts, and whenever these are found,
we consider only the fastest-growing instability, associated
with the eigenvalue l max having the maximum positive real
part. In Ref. 6, it was shown that for the ZBM in a mon-
atomic (k 2 ,k 4 ) or (k 2 ,k 3 ,k 4 ) lattice with StdPBC’s, the oc-
currence of instabilities with growth rates l max which are
purely real is intimately connected with the existence of
ILM’s. Following Ref. 6, we term such instabilities ‘‘ILM
related,’’ and in the remainder of this paper we will only
discuss ExM instabilities of this type.17
For the small-amplitude OZCM with either StdPBC’s or
ZSPBC’s, we do not find purely real l max’s, implying by
analogy with the monatomic StdPBC studies of Ref. 6 that
related ILM’s do not exist at small amplitudes. However, for
both periodic boundary conditions, we find that a finite
threshold amplitude A thresh exists, above which the RWA sta-
bility analysis predicts a purely real l max . The upper panel
of Fig. 3 plots our predicted maximum growth rate as a func-
tion of the OZCM amplitude for StdPBC’s. The diamonds
give the results of MD measurements based on the ‘‘projec-
tion’’ method of Ref. 6, for a 40-particle lattice. The agree-
ment between the predicted and measured values is within
7%. By decomposing the instability perturbation into its
plane-wave Fourier components, we can obtain the wave
vector (k p ) max of the fastest-growing component, as dis-
cussed in Ref. 6 for the monatomic lattice ZBM. The lower
panel of Fig. 3 plots (k p ) max as a function of the OZCM
amplitude for StdPBC’s. At the instability threshold ampli-
tude A thresh50.120a, (k p ) max vanishes, and it increases to its
maximum allowed value of p /2a over a restricted range of
amplitudes. The corresponding wavelength 2 p /(k p ) max in-
troduces a preferred instability length scale at each ampli-
tude, similar to that for the monatomic ZBM in Ref. 6. As
the amplitude of the OZCM increases from A thresh , the insta-
bility length scale decreases from infinity, attaining a maxi-
mum value of 4a, after which it remains constant for in-
creasing amplitude. Finite-time MD simulations of unstable
OZCM’s in lattices with StdPBC’s reveal that the instability
55
FIG. 3. Upper panel: The solid curve gives the predicted RWA
maximum instability growth rate of the OZCM as a function of the
normalized amplitude, for a diatomic (k 2 ,k 3 ,k 4 ) lattice with
StdPBC’s. The parameter values are given in the text. The dia-
monds give growth rate measurements obtained from MD simula-
tions for a 40-particle lattice. Lower panel: Wave vector of the
fastest-growing Fourier component of the instability perturbation as
a function of the normalized amplitude. To achieve good resolution,
the stability analysis for both panels was based on a wave vector
grid appropriate to a 2000-particle lattice.
leads to a breakup of the mode into a periodic array of lo-
calized excitations whose spacing is very close to the pre-
ferred instability length.
For ZSPBC’s, the qualitative features of the curves of Fig.
3 are retained, but the ILM-related instability threshold am-
plitude is different for the two periodic boundary conditions.
In the limit of an infinite lattice and StdPBC’s, A thresh can be
obtained analytically, following an argument analogous to
that given in Ref. 6 for the case of a ZBM in a monatomic
(k 2 ,k 3 ,k 4 ) lattice. For the OZCM in an infinite diatomic
(k 2 ,k 3 ,k 4 ) lattice with StdPBC’s, we find that the instability
threshold criterion is
3L 4 1
9
2S D
11
m
M
2
L 24 >4L 23 , ~10!
where L 3 [k 3 A/k 2 and L 4 [k 4 A 2 /k 2 . The use of the renor-
malized force constants in place of (k 2 ,k 3 ,k 4 ) in Eq. ~10!
yields the corresponding instability threshold criterion for the
ZSPBC version of the OZCM. However, due to the ampli-
tude dependence of the renormalized force constants, this
criterion is not straightforward to solve analytically for
A thresh , in contrast to the StdPBC case. Nevertheless, a rather
lengthy analytic calculation shows that A thresh for the OZCM
in the infinite lattice with ZSPBC’s coincides exactly with
the minimum of this mode’s frequency vs amplitude curve.
The instability thresholds computed numerically for a 40-
particle lattice with both boundary conditions are shown by
the diamonds on curves ~a! and ~a 8 ) in Fig. 1; for
StdPBC’s the threshold is at (A thresh /a, v / v max)
55 BOUNDARY-CONDITION EFFECTS IN ANHARMONIC . . .
FIG. 4. Dynamic ~circles! and static ~squares! displacements for
an odd-parity OZCM-ILM in the 40-particle diatomic lattice of Fig.
1, with ZSPBC’s. The small ~large! symbols represent
the light ~heavy! masses, respectively. Upper panel: At
(A/a, v / v max)5(0.194,1.40) the mode is highly localized, with the
particles away from the mode center being essentially at rest and
having constant static displacements. Lower panel: At
(A/a, v / v max)5(0.099,0.95) the dynamic displacement pattern ex-
hibits an OZCM-like extended background. Note the accompanying
lattice constant change away from the ILM center.
5(0.120,1.36), while for ZSPBC’s the values are
(0.063,0.91). The differences between the 40-particle thresh-
old amplitudes and their infinite lattice counterparts are un-
observable on the scale of this figure.
No MD runs showing the finite-time evolution of either
the unstable OZCM or the unstable OZBM for ZSPBC’s are
reported here, since the implementation of the zero-stress
condition in MD is difficult, particularly when dealing with
the spatial inhomogeneities introduced by the ExM instabili-
ties or the presence of ILM’s.
3. OZCM-related ILM’s
Next, we consider ILM’s that are related to the OZCM in
our diatomic lattice, in a sense which will become clear be-
low. Since the dynamic displacement pattern of the OZCM is
odd under reflection in a site, we restrict our attention to
ILM’s with this parity. These ILM’s are just the diatomic
versions of the known odd-parity ILM’s in monatomic
(k 2 ,k 3 ,k 4 ) lattices. The upper panel of Fig. 4 shows the
dynamic and static displacements for such an ILM in a 40-
particle lattice with ZSPBC’s. For this ILM, v 51.40v max .
In Fig. 1, the frequency of this odd-parity ILM in a 40-
particle diatomic lattice is shown as a function of the ampli-
tude of the mode’s central particle. The dashed curves ~b!
and ~b 8 ) are for ILM’s in lattices with StdPBC’s and
ZSPBC’s, respectively. It can be seen that for amplitudes
greater than A'0.15a, the ILM curves for the two different
periodic boundary conditions are nearly coincident. Inspec-
tion of the corresponding displacement patterns in this range
shows that the dynamic displacements are likewise almost
identical. At such amplitudes, the modes are highly localized
8835
for both boundary conditions, i.e., the particles away from
the mode center are essentially at rest, as shown in the upper
panel of Fig. 4 for the ZSPBC case. The slight difference
between the two ILM curves of Fig. 1 in this range arises
from the different static displacements away from the mode
center for the two types of periodic boundary conditions. For
StdPBC’s, the total length L of the lattice is held fixed at its
static equilibrium value, and a highly localized ILM pro-
duces dynamical stress, resulting in static displacements
$ b n % which decrease uniformly to zero at the supercell
boundaries; thus there is a constant static strain away from
the ILM center. The magnitude of this strain and the corre-
sponding dynamical stress decrease with increasing number
of particles N and vanish only in the infinite lattice limit. On
the other hand, for a finite lattice with ZSPBC’s, the dynami-
cal stress set up by the ILM is relieved by allowing the
supercell length to increase. As a result, a highly localized
ILM in a ZSPBC lattice produces zero strain away from the
mode center, even for a finite lattice ~see top panel of Fig.
4!—the lattice on each side of the ILM simply moves out
uniformly. Thus when the ILM localization is much smaller
than the total number of particles, as in the upper panel of
Fig. 4, the ILM properties should be very similar for
StdPBC’s and ZSPBC’s. This is the case in Fig. 1, for ILM
amplitudes greater than A'0.15a.
However, the situation is very different for these ILM’s at
smaller amplitudes. As the amplitude is decreased from the
highly localized case discussed above, the ILM frequencies
for the two periodic boundary conditions decrease together
in Fig. 1, approaching v max from above. Further decrease of
the amplitude leads to a separation of the two ILM curves:
the ZSPBC ILM curve continues down into the harmonic
optical phonon band until it merges with the curve for the
ZSPBC OZCM at (A/a, v / v max)5(0.063,0.91). This point
corresponds almost exactly to the minimum of the OZCM
curve. On the other hand, with StdPBC’s, the ILM frequency
never enters the harmonic optical phonon band. Instead,
shortly before v max is reached, the frequency vs amplitude
curve has a sharp minimum ~‘‘knee’’! and the frequency
rises over a very small amplitude range, until the ILM curve
merges with the StdPBC OZCM curve at
(A/a, v / v max)5(0.120,1.36).
This clearly distinct behavior with decreasing amplitudes
can be understood from the nature of the dynamic displace-
ment patterns. When the frequency is above v max , the ILM
remains localized and the particles away from the mode cen-
ter behave like particles in a harmonic lattice which is driven
above its maximum frequency v max , i.e., they vibrate with
very small amplitudes that die away rapidly with distance
from the mode center. As the ILM frequency decreases to
become resonant with v max , the entire lattice responds, and
the ILM dynamic displacement pattern acquires a small-
amplitude extended background away from the mode center.
For StdPBC’s, this occurs slightly above v max , whereas for
ZSPBC’s, it occurs at v max . In each case, the background
pattern is just that of the corresponding small-amplitude
OZCM having the same frequency as the ILM.18 Hence, for
StdPBC’s, the extended background amplitude and fre-
quency correspond to a point in Fig. 1 on the OZCM curve
~a! just above v max , whereas for ZSPBC’s, they correspond
to a small-amplitude point just below v max on the OZCM
8836 D. BONART. T. RÖSSLER, AND J. B. PAGE
curve ~a 8 ). For a further decrease of the ILM amplitude, the
extended background amplitude grows relative to the local-
ized portion of the ILM; comparing curves ~a! and ~a 8 ), we
see that for StdPBC’s, the background OZCM amplitude can
grow only if the mode frequency increases, whereas for
ZSPBC’s, an increase in the background OZCM amplitude
corresponds to a frequency decrease. Thus the different be-
havior of the two ILM curves in Fig. 1 results from the
different frequency vs amplitude behavior of the corre-
sponding extended background portions. In either case, the
extended background amplitude grows as the ILM amplitude
decreases, until the ILM becomes the OZCM for the particu-
lar periodic boundary condition. We will refer to these
ILM’s as ‘‘OZCM-ILM’s,’’ to distinguish them from the
OZBM-related ILM’s to be discussed in the next section.
The lower panel of Fig. 4 illustrates an OZCM-ILM in a
ZSPBC 40-particle lattice for v 50.95v max , well inside the
harmonic optical phonon band. The mode’s extended back-
ground is readily apparent. ILM’s with an extended back-
ground were discussed briefly in Ref. 6, for a monatomic
(k 2 ,k 3 ,k 4 ) lattice with StdPBC’s.
Finally, we emphasize that for each periodic boundary
condition, the point in Fig. 1 where the OZCM-ILM fre-
quency vs amplitude curve merges with the corresponding
OZCM curve and where we have seen that the OZCM-ILM
actually becomes the OZCM, agrees exactly with the OZCM
instability threshold amplitude in our 40-particle lattice,
shown in the figure as a diamond. Furthermore, for ampli-
tudes below A thresh , we find no OZCM-ILM’s in either case.
It is interesting to note from Fig. 1 that with ZSPBC’s, the
frequency range of the unstable OZCM and the OZCM-ILM
are the same, whereas this is seen not to be the case for
StdPBC’s. This mismatch of the frequency ranges of the un-
stable ExM and its related ILM for StdPBC’s was briefly
discussed in the introduction in the context of the ZBM in a
monatomic (k 2 ,k 3 ,k 4 ) lattice, and we will return to this
point later.
For either periodic boundary condition, changing the par-
ticle number N does not affect our qualitative results, such as
the junction between the OZCM and OZCM-ILM frequency
vs amplitude curves and the nature of the evolution of the
OZCM-ILM displacement patterns along the curves.
B. Optical zone boundary mode and related ILM’s
1. Dynamics of the OZBM
a. Standard periodic boundary conditions. For these
boundary conditions, the OZBM dynamics are not affected
by cubic anharmonicity, just as for the OZCM ~see Appendix
A!. The RWA frequency of the OZBM is determined by
S D S D S D
21
v StdPBC 2 m k4 2
5 11 113 Ã , ~11!
v max M k2
where à is now A/2 rather than the OZCM value
(11m/M )(A/2), with A again being the amplitude of a light
mass. The frequency of the OZBM thus increases monotoni-
cally with increasing amplitude, starting from the corre-
harm 5 v max / A11m/M and
sponding harmonic frequency v OZBM
moving up through the harmonic optical phonon band. This
55
is illustrated by the solid curve ~a! in Fig. 5. When realistic
full potentials are used, the OZBM v (A) curve exhibits the
same qualitative behavior.
b. Zero-stress periodic boundary conditions. For these
boundary conditions, the OZBM produces a lattice constant
change D(Ã) which is given by Eq. ~8!, but with Ã5A/2.
Thus Fig. 2 applies to the OZBM, provided the abscissa
values are multiplied by (11m/M ). The expressions for the
renormalized force constants in terms of D are the same as
those given below Eq. ~8!, and they lead to the RWA squared
frequency
S D S DS
v max
2
v ZSPBC
5 11
m
M
21
k̂ 2
k2
k̂ 4
13 Ã 2
k2
D
S DF
5 11
m
M
21
112
k3
k2
k4
G
D13 ~ D 2 1Ã 2 ! ,
k2
~12!
from which we compute the solid curve ~a 8 ) of Fig. 5. Com-
paring Eqs. ~11! and ~12! with their OZCM counterparts Eqs.
~7! and ~9!, we observe that the only differences are the
constant prefactor (11m/M ) 21 in Eqs. ~11! and ~12! and
the definitions of the effective mode amplitude Ã. Therefore,
the OZBM frequency vs amplitude curves for the two peri-
odic boundary conditions exhibit the same qualitative behav-
ior as those for the OZCM, and the discussion given in Sec.
IV A 1 below Eq. ~9! applies here as well. Note, however,
that the minimum of our OZBM ZSPBC frequency vs am-
plitude curve occurs within the harmonic phonon gap, at
(A/a, v / v max)5(0.078,0.81), rather than within the har-
monic optical phonon band as for the OZCM. For realistic
full potentials the OZBM frequency has no minimum, de-
scending instead through the phonon gap.
2. Stability of the OZBM
Although the frequency vs amplitude curves for the
OZBM and the OZCM are very similar, we find that these
modes’ ILM-related stability properties differ markedly and
are, in fact, complementary: whereas the OZCM is stable for
amplitudes below an instability threshold, the OZBM is
stable above a critical amplitude. The two types of periodic
boundary conditions only affect the details of this behavior,
analogous to the situation for the OZCM. More specifically,
for both StdPBC’s and ZSPBC’s, the RWA stability analysis
predicts the OZBM to have an ILM-related instability, i.e.,
an instability with a purely real growth rate l max , only for
amplitudes from zero up to a critical threshold value
A thresh . The upper panel of Fig. 6 shows our predicted
growth rate as a function of the OZBM amplitude for
StdPBC’s. Measured growth rates for MD simulations of the
OZBM in a 40-particle lattice are indicated by diamonds,
and the agreement with the RWA prediction is to within less
than 3% except for the point at the largest amplitude, where
the deviation is 10%. For our force constants the RWA
instability threshold occurs at (A thresh /a, v / v max)
5(0.149,1.21).
In the lower panel of Fig. 6 we plot the wave vector
(k p ) max of the fastest-growing Fourier component of the
RWA instability perturbation as a function of the OZBM
55 BOUNDARY-CONDITION EFFECTS IN ANHARMONIC . . .
FIG. 5. Same as Fig. 1, but for the OZBM and its associated ILM. The inset magnifies a portion of the figure near the minimum of the
curve for the ZSPBC OZBM. The solid circle, square and upward-pointing triangle correspond to specific mode patterns discussed in the
text.
amplitude for StdPBC’s. We find that (k p ) max decreases from
p /2a at small amplitudes to a minimum of 0.25p /2a at
A50.084a and then increases back to p /2a at A thresh . With
an instability perturbation of wave vector (k p ) max present,
the spatial modulation of an ExM of wave vector k is deter-
mined by Dk5 u k2(k p ) maxu , so that the ExM’s preferred in-
stability length scale is 2 p /Dk. Note that for the OZCM
discussed earlier, k50 and Dk5(k p ) max , whereas for the
FIG. 6. Same as Fig. 3, but for the OZBM.
8837
OZBM Dk5 u p /2a2(k p ) maxu . Hence the minimum in the
(k p ) max vs amplitude curve of Fig. 6 corresponds to a maxi-
mum of Dk and hence to a minimum preferred instability
length scale. Finite-time MD simulations of unstable
OZBM’s for StdPBC’s reveal that the instability causes the
mode to break up into a periodic array of localized excita-
tions whose spacing is close to the preferred instability
length.
Replacing the StdPBC’s by ZSPBC’s, we obtain qualita-
tively similar results. For these boundary conditions, the
RWA instability threshold is at (A thresh /a, v / v max)
5(0.078,0.81), which coincides exactly with the minimum
in the ZSPBC OZBM frequency vs amplitude curve ~a 8 ) of
Fig. 5. Furthermore, (k p ) max attains its minimum value
0.57p /2a at A50.054a. In Fig. 5, the computed OZBM in-
stability thresholds for both periodic boundary conditions in
a 40-particle lattice are shown by diamonds.
3. OZBM-related ILM’s
Finally, we discuss the ILM’s which are related to the
OZBM in our diatomic lattice in the same sense that the
OZCM-ILM’s discussed in Sec. IV A 3 are related to the
OZCM. Provided the amplitude is not too high, the frequen-
cies of these ‘‘OZBM-ILM’s’’ turn out to be in the harmonic
phonon gap. Regarding the symmetry of these ILM’s, we
first note that the dynamic displacement pattern of the
OZBM is odd under reflection in a light mass site and even
under reflection in a heavy mass site. Gap ILM’s having one
or the other of these symmetry properties have been consid-
ered in Refs. 9 and 10. Here, we will focus on gap ILM’s that
are odd under reflection in a light mass site. These are the
8838 D. BONART. T. RÖSSLER, AND J. B. PAGE
FIG. 7. Dynamic ~circles! and static ~squares! displacements for
an odd-parity OZBM-ILM in the 40-particle diatomic lattice of Fig.
1, with ZSPBC’s. The small ~large! symbols represent the light
~heavy! masses, respectively. Upper panel: Displacements for
(A/a, v / v max)5(0.017,0.89). Middle panel: At (A/a, v / v max)
5(0.067,0.85), the mode has its smallest spatial width. Lower
panel: At (A/a, v / v max)5(0.097,0.83), the ILM has spatially
broadened by acquiring a central ‘‘core’’ of 17 particles having an
OZBM-like dynamic displacement pattern.
most localized gap ILM’s for a given amplitude, and the
maximum dynamic displacement occurs for the light mass at
the mode center. The central panel of Fig. 7 shows the dy-
namic and static displacements of such a gap ILM in a 40-
particle lattice with ZSPBC’s. The frequency is
v 50.85v max , and the ILM is highly localized.
In Fig. 5, the dashed curves ~b! and ~b 8 ) give the fre-
quency of the odd-parity gap ILM as a function of the
central-particle amplitude for StdPBC’s and ZSPBC’s, re-
spectively, in our 40-particle lattice. For StdPBC’s the ILM
frequency eventually moves up into the harmonic optical
phonon band, while for ZSPBC’s it remains in the gap. For
both boundary conditions, however, the ILM curves merge
with the corresponding OZBM curves at both small and large
amplitudes, and we will thus henceforth refer to these ILM’s
as OZBM-ILM’s, rather than as gap ILM’s.
The amplitude vs frequency behavior of the OZBM-
ILM’s in Fig. 5 is more complex than the previously dis-
cussed OZCM-ILM behavior shown in Fig. 1. A striking
feature of the ILM curves of Fig. 5 is their oscillatory nature
for amplitudes greater than A'0.08a. For ZSPBC’s, this is
shown more clearly in the inset. The oscillations are inti-
mately related to the manner in which the spatial width of the
OZBM-ILM changes along the curves, as will now be de-
tailed. In Sec. V we will discuss this behavior in terms of a
simplified model and will give conditions under which it is
likely to occur.
55
To discuss the results of Fig. 5 in more detail, we now
focus on the ZSPBC case and will later simply point out the
differences for StdPBC’s. As we follow the OZBM-ILM
curve ~b 8 ) from small amplitudes to its large-amplitude
junction with curve ~a 8 ), the mode’s spatial width changes
from delocalized ~small-amplitude OZBM! to highly local-
ized and then again to delocalized ~large-amplitude OZBM!.
The mode shown in the middle panel of Fig. 7 is, in fact, the
minimum-width OZBM-ILM for our 40-particle lattice, and
the upper and lower panels of this figure show the mode for
smaller and larger amplitudes, respectively. To quantify the
broadening, we introduce a convenient measure of the ILM’s
spatial width as
N
u c nu
s5 (
n51 A
, ~13!
where N is the total number of particles in the lattice. With
this definition, more highly localized modes have smaller
values of s . For the OZBM-ILM, the maximum value of s
is obtained when the mode broadens to become the OZBM;
this gives s max5N/2, since the heavy masses are at rest and
all of the light masses have the same amplitude. For the three
OZBM-ILM patterns of Fig. 7, the values of s / s max are 0.47
for the upper and lower panels and 0.12 for the middle panel.
The two panels of Fig. 8 give our results for s / s max as a
function of the OZBM-ILM amplitude or frequency, respec-
tively, for our 40-particle lattice with ZSPBC’s. For an infi-
nite lattice, the small-amplitude OZBM-ILM exists down to
A50, corresponding to the frequency v 5 v OZBM harm , the bot-
tom of the harmonic optical phonon band. However, because
our lattice is finite, there is a very small threshold amplitude
A50.008a for OZBM-ILM existence, as seen in the left-
hand panel of Fig. 8. The corresponding threshold frequency
is seen in the right-hand panel to be slightly below v OZBM harm ,
shown by the thin vertical line. For amplitudes just above the
threshold, the dynamic displacement pattern is essentially
that of a small-amplitude OZBM, but with the dynamic dis-
placements gradually rising a small amount as one moves
from the ends of the lattice towards the center. For this de-
localized pattern s / s max'1. With increasing amplitude, the
frequency decreases within the harmonic gap ~Fig. 5!, and
the mode’s spatial width decreases smoothly, as does
s / s max . The smallest width is reached at (A/a, v / v max)
5(0.069,0.85), where s / s max has its minimum value of
0.12, giving the mode pattern shown in the middle panel of
Fig. 7. This most localized OZBM-ILM in our lattice is seen
to be strongly dominated by the motion of the central par-
ticle. The solid circles in Fig. 5 and in both panels of Fig. 8
correspond to this mode.
Increasing the ILM amplitude beyond this point, we find
that the spatial width of the ILM begins to increase. How-
ever, as seen in Fig. 8, this increase is now accompanied by
‘‘oscillations’’ of both the ILM amplitude and frequency; as
a function of s / s max , their period is close to 0.1. The oscil-
lations indicate that the ILM’s width is now changing by a
less continuous process than at small amplitudes, where no
oscillations are seen. Detailed inspection of the mode pattern
reveals that after the first of these oscillations, the amplitudes
of the two light masses on either side of the center of the
highly localized mode shown in the middle panel of Fig. 7
55 BOUNDARY-CONDITION EFFECTS IN ANHARMONIC . . .
FIG. 8. Normalized spatial width parameter s / s max @Eq. ~13!#
for the OZBM-ILM as a function of the normalized amplitude ~left
panel! and frequency ~right panel!, for the 40-particle diatomic lat-
tice of Fig. 1, with ZSPBC’s. The downward-pointing triangle, the
circle, and the square correspond to the modes whose patterns are
given in the top, middle and lower panels of Fig. 7, respectively.
The upward-pointing triangle corresponds to the similarly marked
point in Fig. 5. Crosses represent MD measurements of the OZBM-
ILM frequency for the case of free-end boundary conditions. The
MD measurements and RWA predictions differ by 1% at most. The
thin vertical line denotes the bottom of the harmonic optical phonon
band.
have grown to become almost equal with that of the central
particle, whereas the other amplitudes have changed only
slightly. The additional two large amplitudes increase s by
approximately 2, so that s / s max grows by about 0.1 for our
40-particle lattice. During the next oscillation period of
A/a and v / v max , the amplitudes of two additional light
masses increase until they closely match that of the central
particle, and so on. The lower panel of Fig. 7 shows the
dynamic and static displacements for (A/a, v / v max)
5(0.097,0.83) and s / s max50.47. It is seen that a ‘‘core’’ of
17 particles exhibits an OZBM-like displacement pattern,
while the rest of the lattice barely vibrates. Note that for this
type of broadening, N s / s max gives an approximate measure
of the number of particles in the core. The locations of this
ILM on the curves of Figs. 5 and 8 are shown by squares.
As the width of the OZBM-like core region grows by the
addition of pairs of light masses, the dynamical behavior
near the mode center approaches that of the full lattice
OZBM having the same amplitude as the OZBM-ILM’s cen-
tral particle. This is seen in the inset of Fig. 5, where the
oscillations in the OZBM-ILM amplitude vs frequency curve
~b 8 ) eventually parallel a portion of the OZBM amplitude vs
frequency curve ~a 8 ). Indeed, the later oscillations cannot be
resolved from each other or from the OZBM curve, and the
square denoting the location of the mode shown in the lower
panel of Fig. 7 is actually removed from the OZBM curve
~a 8 ) by approximately five oscillations.
Clearly, in a finite lattice only a finite number of the os-
cillations can occur, since the number of particles in the
mode’s OZBM-like core cannot exceed the total number N.
The limiting situation is approached when the core encom-
passes almost the entire lattice, and since we are using peri-
odic boundary conditions, the mode pattern then looks like a
8839
‘‘hole’’ in the full-lattice OZBM. Indeed, if the site labels are
all shifted by N/2, the pattern appears as if one had simply
subtracted from the OZBM a highly localized OZBM-ILM,
centered in the lattice. One can develop this ‘‘anti’’-ILM
point of view to give a completely equivalent description of
the OZBM-ILM, although we will not do so here.
The final amplitude and frequency oscillations for our 40-
particle lattice are marked in Figs. 5 and 8 by upward-
pointing triangles. Further decrease in the OZBM-ILM am-
plitude is accompanied by a decrease in the frequency, which
then tracks very closely the OZBM frequency vs amplitude
curve ~a 8 ) in Fig. 5 downward, until the minimum is reached
at the diamond, marking the OZBM instability threshold. At
this point the OZBM-core fills the entire lattice, i.e., the
OZBM-ILM has become the OZBM.
Turning now to the StdPBC case, we find the same quali-
tative behavior for the OZBM-ILM dynamic displacement
pattern as we follow curve ~b! in Fig. 5, starting from small
amplitudes and ending at its large-amplitude junction with
the OZBM curve ~a!: the mode first changes smoothly from
delocalized ~small-amplitude OZBM! to highly localized, af-
ter which it delocalizes with accompanying amplitude and
frequency oscillations. The mode becomes a large-amplitude
OZBM at the upper diamond, corresponding to the OZBM
instability threshold for our 40-particle StdPBC lattice. The
differences between the OZBM-ILM curves ~b! and ~b 8 ) re-
sult from the presence of nonzero dynamical stress produced
by the ILM in the StdPBC case; this effect is necessarily
absent for ZSPBC’s. Note that the presence of dynamical
stress renders the mode frequency at a given amplitude
higher for StdPBC’s than for ZSPBC’s in our 40-particle
lattice. Even so, we see that for amplitudes from zero to
A'0.08a, the effect is not large and curve ~b! approximately
follows curve ~b 8 ). At this point the mode for either bound-
ary condition is beyond its maximum localization ~see the
middle panel of Fig. 7! and has begun to broaden by devel-
oping an OZBM-like central core, as detailed above for the
ZSPBC case. This broadening continues, with its attendant
frequency and amplitude oscillations, until the size of the
OZBM-like core is such as to produce enough dynamical
stress in the StdPBC case to markedly affect the mode dy-
namics. For our 40-particle lattice this occurs above
A'0.08a, and the curves ~b! and ~b 8 ) in Fig. 5 become very
different. The difference just reflects the strong influence of
nonzero dynamical stress on the pure OZBM curve for
StdPBC’s, as is evidenced by comparison of curves ~a!
and ~a 8 ). As the large-amplitude OZBM-ILM for each peri-
odic boundary condition broadens to become the correspond-
ing OZBM, the accompanying oscillations in its frequency
vs amplitude curve parallel and approach the OZBM curve to
which it eventually attaches.
Finally, for either of our periodic boundary conditions,
changing the particle number N does not affect our qualita-
tive results, such as the existence of two junctions between
the OZBM and OZBM-ILM frequency vs amplitude curves,
the appearance of an OZBM-like ‘‘core’’ in the OZBM-ILM
with its accompanying frequency and amplitude oscillations,
and the nature of the evolution of the ILM displacement
patterns along the frequency vs amplitude curves.
8840 D. BONART. T. RÖSSLER, AND J. B. PAGE 55

TABLE I. Results relating ExM properties and ILM existence for specific model lattices: ~a! diatomic
(k 2 ,k 3 ,k 4 ) lattice with 4k 23 /(3k 4 k 2 ).1, ~b! diatomic (k 2 ,k 3 ,k 4 ) lattice with 0<4k 23 /(3k 4 k 2 ),1, ~c! di-
atomic lattice with full BMC potential. Column 3 gives a range for the mode amplitude A of both the ExM
specified in column 2 and the ExM’s related ILM’s of column 7. The quantity A thresh denotes the threshold
amplitude for the ILM-related instability of the ExM. The ExM stability behavior of column 4 as well as the
signs of the ExM quantities v 9 (k) and v ZSPBC 8 (A) defined in Sec. V A 2 apply to the entire amplitude range
of column 3. Column 7 indicates whether ILM’s related to the ExM of column 2 exist with amplitudes within
this range, and if so, of which type they are. The various ILM types are described in Sec. V. Entries in
columns 4 and 7 are valid for both StdPBC’s and ZSPBC’s, although the corresponding A thresh may differ.

ExM ~also gives Amplitude ILM-related ExM-related

Model m→M limit! range ExM stability v 9 (k) 8
v ZSPBC (A) ILM’s

OZCM~→ZBM! A,A thresh stable ,0 ,0 no ILM’s

A.A thresh unstable ,0 .0 type ~1!

~a!
A,A thresh unstable .0 ,0 types ~2!, ~3!
OZBM
A.A thresh stable .0 .0 type ~3!

OZCM ~→ZBM! A.0 unstable ,0 .0 type ~2!

~b!
OZBM A.0 stable .0 .0 no ILM’s

OZCM (→ZBM! A.0 stable ,0 ,0 no ILM’s

~c!
OZBM A.0 unstable .0 ,0 type ~2!

V. DISCUSSION
In this section, we use our diatomic (k 2 ,k 3 ,k 4 ) lattice
results of Sec. IV, together with findings for other model
lattices, to obtain basic interrelations between ILM’s and
their associated ExM’s. In Sec. IV, we encountered three
qualitatively different ways for the dynamic displacement
pattern of an ILM to change as one moves along its fre-
quency vs amplitude curve: ~1! For the OZCM-ILM’s dis-
cussed in Sec. IV A 3, the pattern begins as a localized re-
gion of increased displacements ‘‘on top’’ of a finite-
amplitude background OZCM ~e.g., lower panel of Fig. 4!
and evolves with increasing amplitude into a highly localized
mode without background ~e.g., upper panel of Fig. 4!. ~2!
For the OZBM-ILM discussed in Sec. IV B 3, the mode
evolves from a very small-amplitude OZBM with dynamic
displacements gradually rising towards the mode center ~e.g.,
upper panel of Fig. 7! to a highly localized mode ~e.g.,
middle panel of Fig. 7!. Further increase in the amplitude
leads to a very different behavior, as follows. ~3! The
OZBM-ILM of ~2! evolves from being highly localized to a
mode having a broad and sharply delineated OZBM-like
core ~e.g., lower panel of Fig. 7!. The width of the core
increases with increasing amplitude by the addition of pairs
of particles to its ends until it becomes the OZBM, and this
process is accompanied by unusual frequency and amplitude
‘‘oscillations,’’ seen in Figs. 5 and 8. Our results show that if
one of these three ILM behaviors occurs for the ZSPBC’s, it
also occurs for StdPBC’s and vice versa, although the de-
tailed amplitude ranges may differ.
Various examples of these three types of ILM spatial be-
havior are encountered in monatomic and diatomic lattices
for diverse interparticle potentials. For some systems, type-
~2! behavior turns out to encompass all amplitudes, i.e., type-
~3! broadening is absent. Moreover, type ~2! is the only one
found to exist with realistic full potentials V(r), where it
occurs for OZBM-ILM’s in diatomic lattices at all ampli-
tudes; we thus regard type ~2! as the ‘‘generic’’ ILM behav-
ior. All three types will play roles in the remainder of this
section.
A. Existence criteria for type-„1… and type-„2… ILM’s
Table I collects some pertinent ExM-ILM interrelations
that we have obtained for several model lattices, for both
StdPBC’s and ZSPBC’s. The models are: ~a! the diatomic
(k 2 ,k 3 ,k 4 ) lattice for 4k 23 /(3k 4 k 2 ).1, which is discussed in
detail in this paper, ~b! the same lattice, but with
0<4k 23 /(3k 4 k 2 ),1, and ~c! a diatomic lattice with full
BMC potential. Moreover, the table includes the results for
the monatomic limit of these lattices. For each model, it lists
the relevant ExM’s, a studied amplitude range, whether or
not the ExM exhibits an ILM-related instability in this range,
and dynamical properties of the ExM to be discussed in de-
tail in Sec. V A 2. Most importantly, the last column de-
scribes whether or not ILM’s related to the ExM exist with
amplitudes within the studied range ~but not necessarily cov-
ering the entire range!, and if they exist, which of the three
ILM types they are.
1. Criterion based on extended mode stability
The results of columns 4 and 7 in Table I provide com-
prehensive numerical evidence that, independent of the
choice of periodic boundary conditions, ILM’s of types ~1!
and ~2! exist only for ILM amplitudes where the related ExM
55 BOUNDARY-CONDITION EFFECTS IN ANHARMONIC . . .
FIG. 9. Dashed curve: Preferred instability length scale vs fre-
quency for the OZBM in a 2000-particle diatomic (k 2 ,k 3 ,k 4 ) lat-
tice, for the parameter values given in the text and ZSPBC’s. This
quantity is the wavelength corresponding to the difference
u p /2a2(k p ) maxu between the wave vector of the OZBM and the
wave vector (k p ) max of the fastest-growing Fourier component of
the instability perturbation. Diamonds: Spatial extent of the OZBM-
ILM vs frequency in the corresponding 40-particle lattice. This
quantity is 2N s / s max .
is unstable. This generalizes the findings of Ref. 6, which
were for StdPBC’s, to a wider variety of model systems and
to the ZSPBC’s.
In addition, we now present another quantitative connec-
tion between an ILM and stability properties of its associated
ExM, for the case of ZSPBC’s. As discussed in Secs. IV A 2
and IV B 2 for the OZCM and OZBM with
StdPBCs, the wavelength corresponding to the difference be-
tween the wave vector of the ExM and that of the fastest-
growing Fourier component of its instability perturbation in-
troduces a preferred instability length scale. Following the
analysis of Ref. 6 @which was for the ZBM in a monatomic
(k 2 ,k 4 ) lattice with StdPBC’s#, we now compare the ZSPBC
OZBM instability length scale with the spatial extent of the
type-~2! OZBM-ILM having the same frequency in our di-
atomic (k 2 ,k 3 ,k 4 ) lattice with 4k 23 /(3k 4 k 2 ).1. The motiva-
tion for comparing at equal frequencies is discussed in Ref.
6: there, MD simulations of the ZBM in simple (k 2 ,k 4 )
monatomic lattices, where the StdPBC’s and ZSPBC’s are
identical since there is no dynamical stress, revealed that the
unstable ZBM decays into a periodic array of localized ex-
citations having larger amplitudes than the original ZBM, but
having the same frequency. Here, as a measure for the spatial
extent of the OZBM-ILM we use 2N s / s max , where s and
s max are defined in Sec. IV B 3. The comparison is made in
Fig. 9, and the good agreement seen there strongly implies
that the preferred instability length scale is just the spatial
extent of the ILM, in complete analogy to the (k 2 ,k 4 ) case
considered in Ref. 6. Note that a similar comparison is not
possible here for the StdPBC case, since the corresponding
unstable OZBM and type-~2! OZBM-ILM do not share a
common frequency range. Furthermore, finite-time MD
simulations reveal that the unstable OZBM for StdPBC’s
decays into a periodic array of localized excitations having a
frequency different than that of the original OZBM, just as
8841
for the ZBM in a monatomic (k 2 ,k 3 ,k 4 ) lattice reviewed in
the introduction.
For all the other model lattices that exhibit ILM’s of types
~1! or ~2! as listed in Table I, we find similar results for the
match between the preferred instability length scale of an
ExM and the spatial extent of its related ILM at the same
frequency with ZSPBC’s ~after subtracting any ExM-like
background which exists, e.g., that of the lower panel of Fig.
4!. Previously this connection was only shown for the much
simpler case of (k 2 ,k 4 ) lattices with StdPBC’s. In that case,
there is no dynamical stress, and the StdPBC’s are equivalent
to the ZSPBC’s. With odd-order potentials, however, the use
of StdPBC’s generally results in a mismatch of the frequency
ranges of the unstable ExM’s and their related ILM’s, ren-
dering impossible the length scale comparisons at a fixed
frequency. The use of ZSPBC’s now allows a confirmation
of this important ExM-ILM connection for lattices with odd-
order anharmonicity, including those with full BMC nearest-
neighbor potentials.
Studies of anharmonic ExM stability can thus provide
valuable information about the range over which ILM’s exist
in model lattices and, for ZSPBC’s, can also yield informa-
tion about their spatial extent. Such studies form a useful
prelude to direct searches for ILM’s—the stability analysis is
a linear problem and hence is much simpler than searching
for the ILM itself.
2. Criterion based on extended mode dynamics
We now propose a practical, additional existence criterion
for ILM’s of types ~1! and ~2!, which involves both the an-
harmonic and harmonic dynamical properties of the ILM-
related ExM’s. The criterion is based on our numerical stud-
ies for the ZSPBC’s, and it is as follows: for ZSPBC’s, type-
~1! or type-~2! ILM’s related to a given ExM only exist for
amplitudes A where
8
v ZSPBC~ A ! v 9 ~ k ! ,0 ~14!
8
for that ExM. Here, v ZSPBC (A)[d v ZSPBC /dA is the slope of
the frequency vs amplitude curve of the anharmonic ExM for
ZSPBC’s, and v 9 (k)[d 2 v /dk 2 is the curvature of the har-
monic dispersion curve at the wave vector of the ExM. Table
I gives the signs of these quantities for the models listed.
Note from Figs. 1 and 5 that for our diatomic nearest-
neighbor (k 2 ,k 3 ,k 4 ) model lattice of Sec. IV, for both the
OCZM and the OZBM, v ZSPBC 8 (A) is negative for small am-
plitudes and then becomes positive at the mode’s instability
threshold A thresh . Moreover, the curvature v 9 (k) of the har-
monic dispersion is negative for the OZCM (k50) and posi-
tive for the OZBM (k5 p /2a). Hence for the OZCM, the
criterion is met only for amplitudes from the ZSPBC insta-
bility value A thresh50.063a onward, precisely the same range
where we have seen that type-~1! OZCM-ILM’s exist for
ZSPBC’s. On the other hand, for the OZBM in this lattice,
the criterion is satisfied only over the amplitude range from
zero to the ZSPBC instability point for the OZBM, at
A thresh50.078a. This is the amplitude range within which we
have seen that type-~2! OZBM-ILM’s exist for ZSPBC’s.
Although the criterion applies specifically to ZSPBC’s,
we have already remarked that if ILM’s related to an ExM of
a given type ~1!, ~2!, or ~3! exist in a given lattice for one of
8842 D. BONART. T. RÖSSLER, AND J. B. PAGE
our periodic boundary conditions, they also exist for the
other, albeit over a possibly different range of amplitudes.
Moreover, when the ILM’s are highly localized, we have
seen that their properties become essentially independent of
the boundary conditions, as is obvious physically. Accord-
ingly, the existence criterion given here can give useful
information on ILM existence beyond the context of the
ZSPBC’s.
This criterion has been found to hold for every model
system we have studied, as is seen by inspection of columns
5, 6, and 7 of Table I. Moreover, previous ILM studies for
full potentials V(r) other than the BMC interaction included
in the table are also consistent with the criterion. For a di-
atomic lattice with nearest-neighbor full potentials of the
Toda, Morse, or Lennard-Jones forms, v ZSPBC 8 (A),0 for
both the OZCM and the OZBM at all nonzero amplitudes,
and the criterion predicts ILM’s for the latter but not for the
former. Consistent with this, OZBM-ILM’s are found in the
harmonic phonon gap for all amplitudes9 ~until the harmonic
acoustic phonon band is approached19!, whereas OZCM-
ILM’s have not been reported. In the monatomic limit, the
OZCM becomes the ZBM, and no ZBM-ILM’s were found.6
Note that our criterion argues against a speculation offered in
Ref. 20 that ILM’s ‘‘on top’’ of an extended ZBM back-
ground mode @i.e., type-~1! ILM’s# might exist for a Toda
chain.
The specific lattice models discussed so far have been
restricted to nearest-neighbor interactions. Since the inclu-
sion of interactions beyond nearest neighbors can markedly
affect the harmonic dispersion relation, it is interesting and
important to study their effect on the above ILM criterion.
Accordingly, we added a second-neighbor harmonic force
constant k (2nn)
2 /k 2 50.2 to our diatomic (k 2 ,k 3 ,k 4 ) lattice.
The effect is to increase the harmonic OZBM frequency be-
yond the harmonic OZCM frequency and to change the signs
of v 9 (k) for these two modes. On the other hand, the quali-
tative features of their frequency vs amplitude curves are not
altered by this added second-neighbor harmonic interaction.
Equation ~14! thus predicts the opposite behavior from the
case without second-neighbor interactions: OZCM-ILM’s
should now exist below a finite amplitude threshold, whereas
OZBM-ILM’s should exist above a threshold. We have in-
deed verified these predictions.
The above ILM existence criterion is not limited to small
amplitudes. However, in the limit of vanishingly small am-
plitudes we can put it on a rigorous basis in terms of the
mathematical properties of continuous nonlinear dynamical
systems. It is well known3,4,21 that small-amplitude localized
modes in anharmonic 1D lattices, so-called envelope soli-
tons, can be described in terms of an extended carrier mode
having a modulated envelope whose spatial and temporal
variations are slow compared with those of the carrier. In
general, these are propagating solutions for any wave vector,
but for particular wave vectors, e.g., at the zone boundary,
they become stationary envelope solitons and connect with
the small-amplitude versions of the ILM’s studied in this
paper. Moreover, this approach has proven very useful be-
yond the context of 1D lattices, e.g., as a starting point for
theoretical studies of localized anharmonic edge and surface
modes in crystals.22 For the simplest case of a monatomic
55
(k 2 ,k 4 ) lattice, the dynamics of the envelope c (x,t) are de-
scribed by the nonlinear Schrödinger equation ~NLSE!
]c ] 2c
i 1 P 2 2Q u c u 2 c 50, ~15!
]t ]j
where t [ e 2 t and j [ e (x2 v g t) are the slowly varying time
and space variables describing the variation of the envelope
and v g [d v /dk is the group velocity of the carrier wave.23
The coefficients P and Q are, up to positive numerical fac-
tors, equal to v 9 (k) and limA→0 @ v 8 (A)/A # for the carrier
wave, respectively. The sign of their product determines both
the type of solutions of Eq. ~15!, and the stability properties
of the associated anharmonic extended modes, i.e., the car-
rier wave. For PQ.0, Eq. ~15! does not admit spatially
localized solutions having vanishing displacements far from
the mode center, and the corresponding extended carrier
mode is stable against infinitesimal amplitude and phase per-
turbations. For PQ,0, however, localized solutions exist
and the extended carrier mode is unstable.23
For a lattice with cubic anharmonicity, a static distortion
corresponding to the $ b n % in our RWA solutions accompa-
nies envelope solitons.4 This leads to a pair of coupled equa-
tions for the envelope functions which describe the static and
dynamic components of the particle displacements. These
can be combined to yield an equation of the form of Eq. ~15!,
but with different coefficients P̃ and Q̃. Although these
quantities still determine the properties of localized and ex-
tended modes, Q̃ is in general no longer simply proportional
to limA→0 @ v 8 (A)/A # . We suspect that unawareness of this
fact may be the reason that Ref. 4 gives what we believe to
be an incorrect frequency v (A,k) for small-amplitude anhar-
monic ExM’s of general wave vector in monatomic
(k 2 ,k 3 ,k 4 ) lattices.15 At any rate, it can be shown for these
lattices that the simple relation Q̃}limA→0 @ v 8 (A)/A # holds
only for the ZBM, and then only under ZSPBC’s.
Consequently, the existence criterion obtained from the
NLSE approach for the ZBM in (k 2 ,k 4 ) and (k 2 ,k 3 ,k 4 )
monatomic lattices is that for limA→0 @ v 8 (A,k5 p /a)/A #
3 v 9 (k5 p /a),0 the ILM exists and the ZBM is unstable,
whereas if this quantity is positive the ILM does not exist
and the ZBM is stable, all for ZSPBC’s. For the case of the
(k 2 ,k 4 ) lattice the ZBM introduces no dynamical stress, so
the ZSPBC’s and StdPBC’s are equivalent. These small-
amplitude existence results from the NLSE agree with our
more general RWA-based existence criterion of Eq. ~14!,
which applies for arbitrary amplitudes.
We re-emphasize that the NLSE analysis is based on the
assumption of slow spatial and temporal variations of the
envelope as well as small amplitudes, so that its range of
validity is much more restricted than that of our RWA ap-
proach. This is reflected by the fact that the detailed dynami-
cal behavior within these two approaches deviates markedly
for large amplitudes. For instance, the above NLSE analysis
cannot predict the switchover between ILM nonexistence
and ILM existence at a finite threshold amplitude, as we have
encountered in Sec. IV A 3. Furthermore, the unusual large-
amplitude frequency and amplitude oscillations which ac-
company type-~3! broadening and are discussed further in
the following section, cannot be described within the NLSE
approach. Nevertheless, the results of our studies strongly
55 BOUNDARY-CONDITION EFFECTS IN ANHARMONIC . . .
imply that our ILM existence and ExM instability criterion
8
based on the sign of v ZSPBC (A) v 9 (k) is a general property
which applies well beyond the range of validity of the NLSE
approach.
B. Unusual large-amplitude behavior: type-„3… ILM’s
Finally, we return briefly to the unusual amplitude and
frequency oscillations observed in our model studies for the
type-~3! broadening of the OZBM-ILM beyond its point of
highest localization. The oscillations are seen in Figs. 5 and
8, and they occur at large amplitudes. It will be recalled that
the type-~3! broadening is characterized by the presence of
an OZBM-like ‘‘core’’ ~e.g., lower panel of Fig. 7!, whose
width increases by the addition of particles to its ends, two at
a time.
We find similar oscillations for ILM’s in a monatomic
(k 2 ,k 4 ,k 6 ) lattice with k 2 and k 4 positive and negative k 6 ;
hence the essential aspect of their origin is not the presence
of odd-order anharmonicity or a harmonic phonon gap. In-
stead, we feel that the relevant aspects of the model for this
behavior are that small-amplitude ILM’s exist, and that the
frequency vs amplitude behavior of the ExM core which ap-
pears in type-~3! broadening possesses an extremum, so that
the ExM core at a given frequency can occur with two dif-
ferent amplitudes. These features hold for both the mon-
atomic (k 2 ,k 4 ,k 6 ) lattice mentioned above and for our di-
atomic (k 2 ,k 3 ,k 4 ) lattice with ZSPBC’s. For the latter case,
this is evident from curves ~a 8 ) and ~b 8 ) in Fig. 5. The
situation for StdPBC’s, where the oscillations also occur in
our lattice, is more complicated, and its discussion will be
deferred until the ZSPBC case is treated. For our model, the
situation is simplified by the rather large mass discrepancy,
which results in the heavy masses having essentially no dy-
namic displacement. This means that, to a good approxima-
tion, each light particle added to the core has an individual
frequency vs amplitude behavior which mimics that of the
core itself, i.e., possesses a minimum. We incorporate these
features into a highly simplified model consisting of two
anharmonic oscillators having identical frequency vs ampli-
tude curves which possess a minimum. The oscillators are
then weakly coupled. We make the RWA and start from a
displacement pattern in which one oscillator ~representing
the OZBM-like core! has a large amplitude, while the second
oscillator ~representing a light mass to be added to the core!
has a small amplitude, at the same frequency for each oscil-
lator. A continuum of solutions is then found, such that a
smooth transition can occur to a displacement pattern where
the amplitude of both oscillators is the same as the initial
large amplitude of the first oscillator. In terms of this model,
the core has added one light particle. During this transition,
the amplitudes of the two oscillators approach each other by
moving towards the minimum of the frequency vs amplitude
curve until they match, and the oscillators’ frequencies shift
together. From the minimum point, the amplitudes and fre-
quencies increase together, until both oscillators attain the
initial large amplitude of the ‘‘core’’ oscillator. In this tran-
sition, the core oscillator has gone through a single period of
the frequency and amplitude oscillations observed for the
type-~3! OZBM-ILM’s in our diatomic lattice.
For the case of StdPBC’s, our diatomic (k 2 ,k 3 ,k 4 ) lattice
also yields small-amplitude OZBM-ILM’s @curve ~b! in Fig.
8843
5# with type-~3! broadening and associated amplitude and
frequency oscillations. On the other hand, it is at first sight
not clear that the frequency vs amplitude behavior of the
OZBM-ILM’s core for StdPBC’s would exhibit a minimum,
as needed for the above simple model to apply. However, we
have already stressed that the differences between the type-
~3! OZBM-ILM frequency vs amplitude curves for StdPBC’s
and ZSPBC’s in Fig. 5 arise from the dynamical stress
present with StdPBC’s. The dynamical stress depends on the
finite size of our lattice; for an OZBM-ILM having a fixed-
width core, it decreases as the size of the lattice is increased,
vanishing in the infinite lattice limit. In this limit, the lack of
dynamical stress would result in the core behaving dynami-
cally exactly like the OZBM-like core of the same spatial
width for ZSPBC’s in a finite lattice and thus having a mini-
mum in its frequency vs amplitude behavior. Hence, the ba-
sic physics underlying type-~3! ILM frequency and ampli-
tude oscillations is the same for ZSPBC’s and StdPBC’s, but
its details are significantly complicated by the presence of
dynamical stress and finite-size effects in the latter.
VI. SUMMARY AND CONCLUSION
In this paper we have studied boundary condition effects
on the properties of extended lattice modes and intrinsic lo-
calized modes and their interrelations in periodic 1D anhar-
monic lattices. In contrast to the more familiar situation of
harmonic or weakly anharmonic lattices, where the boundary
conditions play a passive role in determining bulk dynamical
properties, we have seen that strongly anharmonic dynamical
behavior is markedly affected by the boundary conditions.
Specifically, for lattices with odd-order interparticle anhar-
monicity, the use of standard periodic boundary conditions,
which keep the length of the supercell constant, generally
results in nonzero ‘‘dynamical stress’’ whenever an ExM or
ILM is present. Accordingly, we have studied the effects of
‘‘zero-stress periodic boundary conditions,’’ which allow the
supercell length to adjust such that the dynamical stress van-
ishes.
Within a rotating wave approximation, we have investi-
gated a variety of models. Our results have been illustrated in
detail via calculations for a diatomic lattice with harmonic,
cubic and quartic (k 2 ,k 3 ,k 4 ) nearest-neighbor interactions,
this model serving to illustrate a wide range of interesting
phenomena. For the anharmonic ExM’s studied, we have
seen that the frequency at a given amplitude is reduced when
the StdPBC’s are replaced by ZSPBC’s. For both the optical
zone center mode and the optical zone boundary mode in our
diatomic (k 2 ,k 3 ,k 4 ) lattice, the frequency increases mono-
tonically with the mode amplitude for StdPBC’s, while it
exhibits a minimum when ZSPBC’s are used. A stability
analysis reveals that the qualitative stability properties of
these ExM’s are the same for both periodic boundary condi-
tions: the OZCM is unstable above a critical amplitude,
while the OZBM is unstable below a critical amplitude, with
the critical amplitude differing for the two types of boundary
conditions. Remarkably, for ZSPBC’s the critical amplitudes
for both ExM’s occur exactly at the minimum of their fre-
quency vs amplitude curves.
Within each type of periodic boundary condition, the
properties of the ExM-related ILM’s were explored; these
8844 D. BONART. T. RÖSSLER, AND J. B. PAGE
are the ILM’s which spatially broaden to become the ExM as
the amplitude is reduced. Just as for the ExM’s, the ILM
frequency at a given amplitude is reduced when ZSPBC’s
are used rather than StdPBC’s. For amplitude ranges where
the ILM’s are highly localized compared to the extent of the
lattice, the ILM frequency vs amplitude curves are rather
insensitive to the choice of periodic boundary conditions, as
expected. However, the portions of these curves which de-
scribe the ILM’s as they spatially broaden to become the
associated ExM are strongly affected.
For both periodic boundary conditions, we have found
three qualitatively different types of ILM’s, characterized by
the way their dynamic displacement patterns change as one
follows their v (A) curves. These types are described in the
first paragraph of Sec. V and are represented by the mode
patterns shown in Fig. 4 @type ~1!#, the upper two panels of
Fig. 7 @type ~2!#, and the lower panel of Fig. 7 @type ~3!#.
ILM’s of type ~3! are unusual, in that they exhibit a central
‘‘core’’ which is essentially just a finite-length OZBM. With
increasing amplitude, the core broadens until it becomes the
OZBM, and this process is accompanied by frequency and
amplitude oscillations. Insight into these oscillations was ob-
tained via a simple model of two coupled anharmonic oscil-
lators. Type-~2! ILM’s exist from zero amplitude, where they
are broad. With increasing amplitude, they become localized
but may convert to type-~3! broadening at a finite amplitude,
as in our diatomic (k 2 ,k 3 ,k 4 ) lattice, or they can remain
localized and of type ~2!. The ILM’s for realistic full poten-
tials V(r) exhibit the latter behavior, remaining of type ~2!
for all amplitudes.
Connecting the ExM and ILM results, we found that for
both periodic boundary conditions, ILM’s of types ~1! and
~2! exist only at amplitudes for which their related ExM’s are
unstable, generalizing earlier qualitatively similar results for
monatomic (k 2 ,k 3 ,k 4 ) lattices with StdPBC’s.6 Further-
more, for ZSPBC’s we have seen that the unstable ExM’s
introduce preferred length scales which match the spatial ex-
tent of the ExM’s related ILM at the same frequency. For
lattices with odd-order anharmonicity, such an analysis is not
generally possible with StdPBC’s, because the frequency
ranges of the unstable ExM and its related ILM differ due to
the nonzero dynamical stress. However, the analysis is
straightforward when ZSPBC’s are used. Most importantly,
the ZSPBC’s have led to a useful second criterion @Eq. ~14!#
for the existence of ILM’s of types ~1! and ~2!, complement-
ing the above criterion based on ExM instability. This addi-
tional criterion involves just two relatively simple properties
of the ILM’s associated ExM, namely the curvature v 9 (k) of
the harmonic dispersion at the ExM wave vector and the
8
slope v ZSPBC (A) of the anharmonic ExM frequency vs am-
plitude curve. In the limit of vanishing amplitudes for type-
~2! ILM’s, this criterion reduces to earlier results for lattice
envelope solitons obtained by means of a nonlinear Schrö-
dinger equation ~NLSE! approach. However, our criterion
applies for finite amplitudes, well beyond the range where
the NLSE approximation breaks down, and it includes type-
~1! ILM’s.
Although the use of periodic boundary conditions which
require the dynamical stress to vanish might seem esoteric
from the point of view of harmonic or weakly anharmonic
lattice dynamics, our studies of its effects on strongly anhar-
55
monic lattice dynamics have yielded clarifying insights into
the fundamental connections between ILM’s and ExM’s.
Moreover, we have obtained promising tools for future ILM
investigations. The ILM existence criterion @Eq. ~14!# re-
quires only knowledge of two basic ExM properties: the cur-
vature of the ExM harmonic dispersion relation, which is
readily available for most real crystals, and the slope
v 8 (A) for the anharmonic ExM under ZSPBC’s, which can
be computed via nonlinear potential models or first-
principles techniques.24 The most attractive situation would
be for materials whose relevant ExM’s can be treated for-
mally within a 1D analysis such as that used here. With a
prediction of ILM existence in hand, one can then study the
stability of the ExM within the ZSPBC’s to obtain a priori
information on the spatial extent of the ILM displacement
patterns.
Realistic interparticle potentials have strong odd-order an-
harmonicity, and we have seen that with such anharmonicity
present, both of the above modeling steps require the use of
ZSPBC’s. Of course, once such ExM studies have been used
to predict ILM’s in a given lattice, the ILM properties for the
highly localized cases will be independent of the specific
boundary conditions, as long as the ILM’s spatial extent is
small compared with the length of the supercell. Thus, be-
sides yielding fundamental insights into the nature of
strongly anharmonic lattice dynamics, the use of ZSPBC’s
provides an appealing practical framework for predicting
ILM’s in real crystals.
ACKNOWLEDGMENTS
This work was supported by NSF Grant No. DMR-
9510182. D. Bonart acknowledges the support of Deutsche
Forschungsgemeinschaft Grant No. Ma 1074/5-1 during a
portion of this work.
APPENDIX A: BOUNDARY CONDITIONS AND THE
DEPENDENCE OF THE EXTENDED MODE DYNAMICS
ON ODD-ORDER POTENTIAL TERMS
As discussed in Sec. II, the relative dynamic displace-
ments for the three ExM’s introduced there are given by
Dc n 5(21) n 2Ã, and the corresponding relative static dis-
placements are Db n 5D. Within the StdPBC’s, D50, and
we can write Eq. ~4a! for the RWA dynamic displacements
as
m nv 2c n5
1
p
E
0
2p
d f cosf $ V 8 @~ 21 ! n 2Ãcosf 1a #
2V 8 @~ 21 ! n11 2Ãcosf 1a # % ~A1!
or
E
2 ~ 21 ! n 2p
m nv 2c n5 d f cosf V 8 ~ 2Ãcosf 1a ! ,
p 0
~A2!
where the latter form is obtained by shifting the integration
variable by p . Expanding V 8 about a, we get
55 BOUNDARY-CONDITION EFFECTS IN ANHARMONIC . . .
m nv c n5
2
2 ~ 21 ! n
p m50
`
~ 2Ã ! m V ~ m11 ! ~ a !
( m!
E
0
2p
d f cos m11
f,
~A3!
where V (m11) (a)[d m11 V(r)/dr m11 u r5a . The integral van-
ishes for m11 odd, so that only the even-order terms in the
expansion of the potential energy affect the dynamics of our
ExM’s.
Note that an analogous result also follows for the
ZSPBC’s, provided the potential is expanded about the
period-average nearest-neighbor distance â(Ã)5a1D(Ã).
In this case, the harmonic and anharmonic coefficients are
renormalized from their static equilibrium values, and only
the even-order renormalized coefficients $ V (m) (â) % are in-
volved in the dynamics of the ExM’s. However, to avoid
confusion, we always use the unrenormalized coefficients
$ V (m) (a) % appropriate to the static equilibrium lattice when
expanding the potential. Then both the even and the odd
potential terms contribute to our ExM’s within the
ZSPBC’s, but not for the StdPBC’s, as we have shown.
APPENDIX B: MINIMIZATION OF THE
PERIOD-AVERAGE POTENTIAL ENERGY
AND VANISHING DYNAMICAL STRESS
We show that the condition of zero dynamical stress
across the supercell boundary follows from requiring that the
period-averaged potential energy of the periodic boundary
condition supercell is minimized. We consider an
N-particle 1D lattice, where particles n and n2l interact via
an assumed central potential V l (r n 2r n2l ), with
l51, . . . ,L int . Here, L int,N/2 restricts the range of the in-
teraction. This is more general than the nearest-neighbor in-
teractions case considered in the main text, reducing to it for
L int51. In addition, we generalize the assumed time depen-
dence for the particle motion, given by Eq. ~3!, to
r n (t)5c n f (t)1b n 1na, where f (0)51 and f (t) is periodic
with period T, but has no zero-frequency Fourier component.
Within the RWA of Eq. ~3! we would have f (t)5cos(vt).
The instantaneous potential energy is given by
N L int N L int
U~ t !5 (( V l ~ r n 2r n2l ! 5 ( ( V l @~ c n 2c n2l ! f ~ t !
n51 l51 n51 l51
1 ~ b n 2b n2l ! 1la # . ~B1!
Since the interaction only depends on relative positions, we
can rewrite Eq. ~B1! in terms of relative dynamic and static
displacements between adjacent particles Dc n [c n 2c n21
and Db n [b n 2b n21 . Thus c n 2c n2l 5c n 2c n21
1c n21 2•••2c n2l11 1c n2l11 2c n2l 5 ( l21 k50 Dc n2k and
similarly for b n 2b n2l . The period-average total potential
energy is
*Also at Institute for Theoretical Physics, University of Regens-
burg, D-93040 Regensburg, Germany.
1
A. S. Dolgov, Fiz. Tverd. Tela 28, 1641 ~1986! @Sov. Phys. Solid
State 28, 907 ~1986!#; A. J. Sievers and S. Takeno, Phys. Rev.
Lett. 61, 970 ~1988!; J. B. Page, Phys. Rev. B 41, 7835 ~1990!.
8845
Ū5
1
T
E
0
T
dt
N L int
( ( V l k50
n51 l51
H l21
( @ Dc n2k f ~ t ! 1Db n2k 1a # J .
~B2!
Imposing periodic boundary conditions by defining
Dc n1N [Dc n and Db n1N [Db n , we ensure that all terms in
this sum are well defined.
Now we assume an arbitrary given relative dynamic dis-
placement pattern $ Dc n % and require ] Ū/ ] Db m 50 for all
mP $ 1, . . . ,N % , which is a necessary condition for the mini-
mization of Ū with respect to the set $ Db n % . Note that the
$ Db n % constitute a set of N independent variables as long as
we do not constrain the total length L of the supercell. We
then have
E
N L int l21
1 T ] V l ~ r n 2r n2l !
T 0
dt ((
n51 l51 ]rn ( k50
d n2k,m
L int l21
5 ((
l51 k50
F̄ m1k,m1k2l 50, ~B3!
where F̄ i, j is the period-average force on particle i due to
particle j. Inspection of this equation reveals that the double
sum involving F̄ is just the sum over all the period-average
interparticle forces acting from one side across an imaginary
plane separating particles m and m21. This is exactly the
definition of the period-average dynamical stress across that
plane as given in the main text. Thus we have shown that the
minimization of the period-average potential energy in the
supercell leads to vanishing period-average dynamical stress
across an imaginary plane separating any pair of adjacent
particles in the supercell, including the supercell boundary.
Note, however, that our argument does not require the sec-
ond derivative of Ū with respect to the set $ Db n % to be
positive and is therefore not reversible; it applies whenever
Ū is an extremum. Although we have not proven in general
that the zero dynamical stress condition is equivalent to a
minimization, we have evidence that this is indeed the case:
for the parameter values of the diatomic (k 2 ,k 3 ,k 4 ) lattice
studied in Sec. IV, it is easy to show analytically that Ū is a
minimum for any mode pattern. Moreover, for any physi-
cally reasonable values of (k 2 ,k 3 ,k 4 ) ~i.e., k 2 .0 and
k 4 .0), it can be shown analytically within the RWA that
this quantity is a minimum for both types of diatomic ExM’s
studied in this paper. Finally, numerical checks for ILM’s in
such lattices also yielded a minimum.
Furthermore, we can show that if we require the period-
average dynamical stress to vanish across an imaginary plane
separating any particular pair of adjacent particles in the su-
percell, it will vanish for all other pairs of adjacent particles,
irrespective of the range of the interaction.
2
A.J. Sievers and J.B. Page, in Dynamical Properties of Solids,
edited by G.K. Horton and A.A. Maradudin ~North Holland,
Amsterdam, 1995!, Vol. 7, p. 137.
3
A. M. Kosevich and A. S. Kovalev, Zh. Éksp. Teor. Fiz. 67, 1793
~1974! @Sov. Phys. JETP 40, 891 ~1974!#.
8846 D. BONART. T. RÖSSLER, AND J. B. PAGE
4
A. Tsurui, Prog. Theor. Phys. 48, 1196 ~1972!.
5
Y. A. Kosevich, Phys. Lett. A 173, 257 ~1993!.
6
K. W. Sandusky and J. B. Page, Phys. Rev. B 50, 866 ~1994!.
7
S. R. Bickham, S. A. Kiselev, and A. J. Sievers, Phys. Rev. B 47,
14 206 ~1993!.
8
M. Aoki, J. Phys. Soc. Jpn. 61, 3024 ~1992!; O. A. Chubykalo
and Y. S. Kivshar, Phys. Rev. E 48, 4128 ~1993!; M. Aoki, S.
Takeno, and A. J. Sievers, J. Phys. Soc. Jpn. 62, 4295 ~1993!;
M. Aoki and S. Takeno, ibid. 64, 809 ~1995!; A. Franchini, V.
Bortolani, and R. F. Wallis, Phys. Rev. B 53, 5420 ~1996!.
9
S. A. Kiselev, S. R. Bickham, and A. J. Sievers, Phys. Rev. B 48,
13 508 ~1993!.
10
S. A. Kiselev, S. R. Bickham, and A. J. Sievers, Phys. Rev. B 50,
9135 ~1994!.
11
See, for instance, M. P. Allen and D. J. Tildesley, Computer
Simulations of Liquids ~Clarendon, Oxford, 1987!.
12
The assumption of two distinct relative static displacements
Db n yielding the same time-average force F̄(Ã) at a given Ã
leads to imaginary RWA frequencies, as long as the particle
motion is restricted to relative displacements r at which the
fourth derivative of V(r) is positive. This encompasses relative
displacements deviating from the static equilibrium nearest-
neighbor separation a by as much as 30% for a Lennard-Jones
potential and 50% for the BMC potentials considered in this
work; moreover, it obviously imposes no restriction on the mo-
tion for a (k 2 ,k 3 ,k 4 ) potential with k 4 .0, such as used here.
13
S. C. Lowell, Proc. R. Soc. London, Ser. A 318, 93 ~1970!.
14
S. Wang, Phys. Lett. A 191, 261 ~1994!.
15
In the monatomic limit the OZCM becomes the ZBM with
Ã5A. We can compare this case with the results obtained for
small-amplitude anharmonic ExM’s in monatomic (k 2 ,k 3 ,k 4 )
lattices in Refs. 13 and 4. Setting k5 p /a in Eq. ~43! of Ref. 13
yields v (A) for the ZBM in agreement with our small-amplitude
limit. However, when Eqs. ~44! and ~45! of Ref. 13 are com-
bined, the resulting v (A) disagrees with our result. We have
therefore rederived Eq. ~44! from Eq. ~43! and find that the
quantity f c appearing in the former equation is given by
@ 4 (11 2 ba 22 ) # 2 (1/2), rather than the expression given by Eq.
3 1
~45! in Ref. 13. The corrected version of Eq. ~44! for k5 p /a
then agrees with our small-amplitude limit for v (A) of the
ZBM. In Ref. 4, Eq. ~5.2! gives the v (A) behavior of small-
amplitude anharmonic ExM’s, but it is not derived. For
k5 p /a we find agreement with our small-amplitude limit for
55
the ZBM. However, Eq. ~5.2! of Ref. 4 and the corrected Eq.
~44! of Ref. 13 disagree with each other for kÞ p /a. We have
therefore rederived Eq. ~5.2! of Ref. 4 using Eqs. ~4.1!, ~4.2!,
and ~5.1! of that paper and obtain V5 v $ 11 @ 2 q v 2 1 p 2 (4
3
23 v ) # u f 61 u e % , in complete agreement with the corrected
2 2 2
Eq. ~44! of Ref. 13.
16
K. W. Sandusky, J. B. Page, and K. E. Schmidt, Phys. Rev. B 46,
6161 ~1992!.
17
As in Ref. 6, we also find complex instability growth rates
l max , for both StdPBC’s and ZSPBC’s, over a range of OZCM
amplitudes. The imaginary parts of these growth rates are com-
parable with the mode frequencies, so that these instabilities are
not well described within the approximations of the RWA sta-
bility analysis. In Ref. 6, such instabilities were investigated via
an exact ‘‘Floquet analysis,’’ and were found to be unrelated to
the question of ILM existence for the systems studied there.
18
More precisely, in our finite lattice with StdPBC’s, the ILM’s
background pattern away from the mode center corresponds to a
small-amplitude OZCM having the frequency of the ILM, but
differing from the pure OZCM by the presence of a constant
strain. This ILM-induced strain renormalizes the force constants
such that the frequency of the background OZCM as a function
of its amplitude is raised slightly compared with the pure OZCM
curve ~a! of Fig. 1, while retaining the same qualitative behav-
ior. The effect of this strain is small in our 40-particle lattice and
vanishes in the infinite lattice limit. With ZSPBC’s, such strain
is completely removed by the supercell length change, for any
size lattice.
19
For completeness, we note that in diatomic lattices with realistic
potentials, at large amplitudes the frequency of the OZBM-ILM
eventually enters the acoustic band and the mode changes its
character, exhibiting an acoustic ZBM-like extended mode back-
ground, as mentioned in Ref. 10.
20
S. Flach, Physica D 91, 223 ~1996!.
21
N. Flytzanis, St. Pnevmatikos, and M. Remoissenet, J. Phys. C
18, 4603 ~1985!; St. Pnevmatikos, N. Flytzanis, and M. Remois-
senet, Phys. Rev. B 33, 2308 ~1986!; C. Tchawoua, T. C. Ko-
fane, and A. S. Bokosah, ibid. 50, 4189 ~1994!.
22
D. Bonart, A. P. Mayer, and U. Schröder, Phys. Rev. Lett. 75,
870 ~1995!; U. Schröder, D. Bonart, and A. P. Mayer, Physica B
219, 390 ~1996!.
23
M. Remoissenet, Waves Called Solitons ~Springer, Berlin, 1994!.
24
R. Car and M. Parrinello, Phys. Rev. Lett. 55, 2471 ~1985!; O. F.
Sankey and D. Niklewski, Phys. Rev. B 40, 3979 ~1989!.