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- M. Korek, A.R. Allouche and S.N. Abdul Al- Potential curves and rovibrational energies for electronic states of the molecular ion KCs^+
- Jan Clausen- Auf dem Weg zur Synthese des [17]Annulenkations
- R. González-Férez and P. Schmelcher- Electric-field-induced adiabaticity in the rovibrational motion of heteronuclear diatomic molecules
- Frederic Mila, Charles Stafford and Sylvain Capponi- Persistent currents in a Moebius ladder: A test of interchain coherence of interacting electrons
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- Joseph N. Stember and Gregory S. Ezra- Fragmentation kinetics of a Morse oscillator chain under tension
- Gregory S Ezra and Stephen Wiggins- Impenetrable barriers in phase space for deterministic thermostats
- Joseph N. Stember and Gregory S. Ezra- Isomerization kinetics of a strained Morse oscillator ring
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- Nan Zhao et al- Observable Topological Effects of Mobius Molecular Devices
- Gregory S. Ezra and Stephen Wiggins- Phase space barriers and dividing surfaces in the absence of critical points of the potential energy
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- Sarin A. Deshpande and Gregory S. Ezra- Quantum state reconstruction for rigid rotors
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number 6

CHEhlICAL PHYSICS LETTERS

27 July 1984

A SIMPLE METHOD FOR DETERMINING THE NUMBER OF ISOLATING INTEGRALS IN MULTIDIMENSIONAL SYSTEMS: COMPUTATION OF THE POINTWISE DIMENSION Craig C. MARTENS and Gregory S. EZRA

Received 7 Ilarch 1984; in final form 4 hlay 1984 The point~vise dimension is calculated for trajectories of two- and three-dimensional Hamiltonians. enabling the number of isolating integrals to be determined directly. Results for the H&on-Heiles system are in agreement with recent calculations of the fractal and information dimensions by Stine and Noid.

1. Introduction There is considerable current interest in the nature of the coexistence of regular (quasi-periodic) and irregular (chaotic, stochastic) motions in the phase space of generic classical Hamiltonian systems [ 1,2], especially the transition from predominantly regular to global chaotic behaviour found at high energies [ 1,2] _These ideas are widely recognized to be of fundamental importance for chemistry [3], insofar as classical dynamics provides an accurate description of intramolecular dynamics. The classical mechanics of two-dimensional model potential surfaces has been intensively studied in recent years [2,3] _ In particular, the Poincare surface of section has been found to be a useful diagnostic for regularity or irregularity of a trajectory [3] _By contrast. very little is known at present concerning the detailed classical dynamics of multidimensional systems described by realistic potential surfaces (for recent work, cf. refs. [4--71). Surface of section methods are difficult to apply for (IV > 3)dimensional systems, so that emphasis must be placed on intrinsic indicators of dynamical behaviour, such as the appearance of coordinate power spectra, or rate of divergence of nearby trajectories (cf. refs. [ 1,3] )_ An important characteristic of any trajectory is the number of isolating integrals associated with it (in addition to the ener,v). This number determines the dimension of the trajectory, where a generalized notion of dimension such as the fractal dimension [8] must in general be used. The importance of the fractal dimension 0 00$2614/84/S (North-Holland 03.00 OElsevier Physics Publishing Science Publishers Division) B-V.

in this context has recently been emphasized by Reinhardt [9]_ There are indications that for (N= 3)dimensional coupled oscillator systems, for example, the chaotic re8ion of phase space is divided at intermediate energies into disjoint “stochastic seas”, each of which is characterized by a particular number of isolating integrals [lo] _ These disjoint regions then merge at higher energy into a single “big sea”. It is clearly important for understanding the structure of chaos in multidimensional systems to have efficient methods for direct computation of the dimension of the trajectory in phase space. Stine and Noid [ 11,12] have recently described methods for calculating both the fractal [ 1 l] and the so-called information dimension [ 121 of a trajectory [ 13]_ These are summarized in section 2. Both techniques rely on computationally intensive bin-counting and sorting operations. In this letter we apply a conceptually and computationally simple approach for determining the pointwise dimension [ 131 of trajectories in two- and three-dimensional Hamiltonian systems. This method has previously been used by Guckenheimer [ 141 to characterize attractors. The defiiition [ 131 of the pointwise dimension (cf. section 3) relies on the existence of both a metric and a probability measure (density of points) in phase space. For Hamiltonian systems, the pointwise dimension is expected to be equal to both the information and the fractal dimension [ 13,13]_ We have confirmed this result for the particular two- and three-dimensional potentials treated below. 573

Volume 108, nunlber 6

**CHEMICAL PlIYSICS LETTERS dimensions: methods
**

versus In IV should give a straight

**27 July 1981
**

line of slope 211 -k

9,. The fractal and information of Stine and Noid

The idea for computing the fractal dimension of a trajectory [I I] or attractor [13,15] is very simple: Phase space is divided into a large number of hypercubes (bins). The trajectory is then run for a time long enough to ensure that the number of bins visited by the trajectory converges to a constant value (no note is taken of the number of times a particular bin is visited by the trajectory). Plotting the log of the number or bins visited versus the log of the inverse size of the bin gives a straight line whose slope is the fractal dimension of the trajectory. Thus, let fV be the number of bins in each direction of phase space, 212 the dimension of phase space. and N,,,k,Uc the number of unique bins visited by the trajectory. We then have [ 1 I] :

In IV unique = (212 -- kj IIl N + COIlSt31lt, (1)

[12]. The above methods have been applied by Stine and Noid to calculate the number of isolating integrals k for quasi-periodic and chaotic trajectories of the 2D H&on-Heiles system. Both approaches yield values k = 2 (quasi-periodic) and k = 1 (chaotic) within reasonable error limits. These results are expected on the basis of surface-of-section studies [2,3] _ Nevertheless, both methods used by Stine and Noid rely on time-consuming bin-sorting operations. This

**factor becomes increasingly important for (fV> 3)-d&
**

mensional systems. We have therefore applied a much simpler approach to determine the so-called pointwise dimension of a trajectory- This method. due to Guckenheimer [ 141 and described in the next section. has minimal sorting and storage requirements yet yields values in agreement wit11 those of Stine and Noid for both two- and three-dimensional systems. We note also the recent calculation of the so-called correlation exponent for attractors by Grassberger and Procaccia [ 161. For the systems treated here the correlation exponent is identical with the pointwise dimension, but is computed using a different and (we found) more time-consuming algorithm.

where 212 -k is the fractal dimension of the trajectory with k the effective number of isolating integrals. There are several drawbacks to this approach. For iargc M (correspcnding to a large numberN2” of bins, ncccssary for accurate results) the trajectory must be run for a very long time to ensure that the number of unique hypcrcubes visited has reached its asymptotic value. In orher words. the trajectory may tend to fill phase spw2 wry IIon-uniforlnly.wlii~i~ slows conver!$ncc of A’,,niclI,L’ The method also requires nluch com-

3. Computation

of the pointwise

dimension

putationally intensive bookkeeping to be done keeping track of bin occupations. Finally_ all counting and sorting has IO bc done for a scrics of bin sized in order to

detcrminc k. mentioned above, Srine and Noid developed a method for calculating the iIiforniaIion dimension of a trajectory. In this proce-

To ~llcviatc the first problem

Jurc. bins tllat arc visited frequently by the trajectory arc ivzighlcd more st rorigly than those visited less frequently. It is therefore possible to attain convergence

with a sliortcr trajectory icmgtll than for the fractal dimension. In addition to a metric in phase space, a probability mcasurc (number of trajectory points in :I given biII/Iotal number of points 011 trajectory) is required. ifgi is Ilic probabili(y of accessing hypcrcubc i, ZIplot

Suppose we have a probability measure ~1(density of points on a trajectory) in phase space. The pointwise dimension d,, is then the exponent with which the total probability contained in a region (sphere) around a given point decreases as the radius of the sphere decreases [ I;]_ hlorc precisely, if S, (x0) is a sphere of a radiuss centered at point x0 on the trajectory, then

(3) If d,, (x0) is independent

‘I,, = d, (x-0) is called

ofxo for almost all x0, then the poitltwise dimension.

111’tlic infoIniaIion

s =

entropy

(2)

A practical procedure for computingd,(xo) is as rollows [ 141: (i) Choose an initial point x0 = (qo, po) in phase space. (ii) Run a trajectory to obtain a series of points S(tj = (q(t), p(f)) with x(r = 0) =x0_ The trajectory

Volume

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CHEMICAL

PHYSICS

LETTERS

27 July

1984

must be run for a time long enough to accumulate an appreciable density of points in the vicinity ofxo.This turns out to be quite feasible for two- and three-dimensional systems examined below. but is of course a major limitation of the method as applied to higher dimension problems, since it necessitates accurate integration over long times of trajectories having possible stochastic character. (iii) At each point on the trajectory, calculate D(t) = 11x(t) -x011, the distance of the point x(t) from the reference point x0_ For a perturbed oscillator Hamiitonian of the foml H(q_p) = If0 + V(q)_ wliere (4

the straight line plots shown in section 4. Keeping track of the distance along the trajectory from each reference point requires very little extra computational effort. The assumption that dp(xO) is constant over rhe whole trajectory allows us to improve statistics by averaging over a set of {x0}_ Examination of log-log plots for individual values of x0 indicates that this assumption is valid for the trajectories shown in section 4, which have well defined regular or chaotic character. It would however be of great interest to study the variation of d,(xo) with phase space point xo for a trajectory corresponding to a ‘patchy” torus, as suggested by Reinhardt [9] _ Such a trajectory would presumably have local regions corresponding to different pointwise dimensions.

a natural

metric in phase space is: II

**4. Results 4.1. T~c’oifirltctuiorralH&m--Hcilcs
**

We have

potential

For all the systems treated below Wi = 1 (i= I. 3 and 3). so that the metric (6) reduces to the Cartesian distance in phase space. We have also verified that the precise form of the metric adopted is not crucial for computation of the pointwise dimension. For example, taking 0.5 wf instead of of in the metric (6) has no effect on the calculated value ofdt,. (iv) As the trajectory is run. the pointsx(f) are binned according to the value of the distanceD(r). At the end of the run, this discrete distance distribution is integrated to give a binned distribution of the total number of points on the trajectory within a given distance of the reference point x0_ Note that no large-scale sorting operations are involved, regardless of the length of the trajectory or the dimension of phase space. (v) The log of the number of points within a given distance is then plotted against the log of the distance. The slope of the straight line portion of the graph at small distances (see section 4) is d,(xo). (vi) Assuming that $,(x0) is the same for all points x0 on the trajectory, the pointwise dimension d, can be defined as the average of d,,(x,) over a set of reference points {x0). We have used sets of 10 reference points (chosen by taking points at every 100th timestep at the beginning of a trajectory run; 100 timesteps is approximately 0.5 characteristic periods) to obtain

applied the method described in the previsection to calculate the pointwise dimension of trajectories for the standard degenerate two-dimensional H&on-Heiles Hamiltonian:

ous

H =+ <p; +pS) +(q;+-

&

+ (+?a

-f

&.

(7)

Initial conditions were chosen to give three trajectories whose configuration-space prqiections are shown in fig. l_ They are of “precessing” quasi-periodic, “Iibrating” quasi-periodic, and chaotic type, respectively. Hamilton’s equation of motion were integrated using Gear’s hybrid 6th order method [I 71, which has proved exceptionally stable for integration of long irregular trajectories [IS] _ For the calculations reported here a constant time step At = 0.05 was used for trajectory integration. and x(t) computed for every point. Retaining a smaller fraction of points on the trajectory for the calculation of the pointwise dimension (for example, 1 point out of every IO) leaves the value of d, essentially unchanged_ We therefore keep all points on the trajectory in order to obtain better statistics for a given trajectory length. A plot of the number of points within a given distance Li versus log D is shown in fig. 2 for the precessing trajectory of fig. 1a. The trajectory was run for 1 X 1 O5

Volume

108. number

6

CHEhIICAL

PIiYSICS

LITERS

‘4

0

‘7 July

1984

a

Tb

a

-49

O-0

I

1:;::. I. Contiguration

-li.s cg 05

i

spxe

projections

of tlm tluee

twodi-

1

mcnsional IICncm-licilcs trajectoriss cxaminetl: (:~)‘Trmxsin~:’ quasi-periodic. (II) “Iibrating” quasipcriodic, (c) cliaotic.

rirnc srcps. In this plot the distance D cxtcnds all the way to its maximum relevant vnlue D,,,;,, , i.e. the size of Lhc whole triijcctory in phase space, 3s cm be seen iron1 111~ saturation of the number of points at large D. A well defined straight line portion of the plot is apparent at small values of D up to ~0.1 Dlllily, and rbr slope of this section defines the pointwise dimension (I,,. Regions of the plot for larger D up to D,,,,, contain information on the global phase space structure of the torus, but are not analysed any further here. AH plots shown from IIOW o11 extend only up to D 50.1

fig. 1 are shown in fig. 3. The plot of fig. 3a has leastsquares slope 2.00, so that to the nearest integer value the pointwise dimension of the precessing quasi-periodic trajectory is 2. This corresponds to X-=4-2 =2, so that there is one isolating integral in addition to the energy, as expected for a quasi-periodic trajectory on an invariant torus. The straight line portion of the

curve for the librating trajectory does not extend as far as for the precessing case. Since the librating trajec-

D 111,,\~

Log-log 576

plots for each of the three trajectories

of

tory corresponds to a “long thin torus”, this is a result of large local curvature of the trajectory manifold in phase space. The plot of fig. 3b corresponds to 2.5 X 1O5 points, and has least-squares slope 2.03. The librat-

Volunw IO& nurnbcr 6

CI1EMICAL PHYSICS LETTERS

27 July 1964

JO

10

8.0

30

LN(D)

I:@. 2. 1’101 log (number of trajcrlory points within 3 disol’ tmcc D of rckrcncc point) versus log fl for 111s:r;~jcctory of fig. la, nvcragcd over ;I set of 10 rcfcrence poin1s.D extends tlic masimmn cstcnt of the trujcstory a11IllC w3y to D,,,,,. in phase spncc. Note the well defined str:lighl line portion nt small D. and the mluration at large D. The poillL!visc dimcnsion is the slope of the plot at small D.

ing trajectory therefore also has 2 isolating integrals. The plot for the chaotic trajectory is shown in fig. 3c (5 X IO5 points) and has least-squares slope 2.98. The chaotic trajectory therefore has k = 1, and no isolating integrals in addition to the energy. 4.2. nlrec-di~nensional model porerlfiul To test the applicability of the method for threedimensional systems, we follow ref. [ 1I] and introduce an additional degree of freedom: H’=H++ (p; + C&J’s), 0)

LX(D)

where we take w3 = 1.0. Although the third degree of freedom is uncoupled, it serves to increase the dimensionality of phase space. Trajectories were run for the three-dimensional system of eq. (8) with initial conditions for modes 1 and 2 identical with those of the trajectories of fig. 1; for mode 3. we set q3 = 0.0, p3 = 0.3. All trajectories were run for 1.O X IO6 time steps. Log-log plots for the three trajectories run are shown in fig. 4. Least-squares values of d, are 3.06. 2.99, and 3.94, corresponding to integer k values 3,3, and 2, respectively. These values are just those expect-

Fig. 3. Log (number of points) versus IosD for the tr3jectories of fig. I. The msGrnutn value of D shown is _<O.l Do,,,. (a) Precessing quasi-periodic: least-squares slope = 3.00, (b) librating quasi-periodic: lcast-squmx slope = 2.03, (c) chaotic: least-squares slope = 2.98.

577

Volume

108, number

6

CHEhlICAL

PHYSICS LET2-ERS

27 July 1984

ed for the addition of an uncoupled degree of freedom to the two-dimensional system treated above.

These results establish the practicability of the meth. od for three-dimensional Hamiltonian systems, and open the way for application to more realistic molecular potentials.

5. Conclusion

We have applied a conceptually and computationally simple method to calculate the pointwise dimension of trajectories of two- and three-dimensional Hamiltonian systems. The method provides the number of isolating integrals for the trajectory directly. Our calculations for the H&on-Heiles potential confirm expec-

00

is

LX(D)

tations

based

agreement [I 1 ,13]_ We have also established

on surface of section studies, and are in with the recent results of Stine and Noid

the applicability of the method for N=3 systems_ Work in progress is concerned with computation of the pointwise dimension for trajectories of realistic three-dimensional surfaces.

Acknowledgement

Acknowledgement petroleum Research is made to the donors of the Fund, administered by the

American

Chemical Society,

for support

of this research.

References

A.J. Licbtcnbcrg and M.A. Lieberman. Repulxr and stochtistic motion (Springer. Berlin. 1963). 51. Tabor, Advan. Chom. Phys. 46 (198 1) 73; P. Brumer, Advan. Chcm. Phys. 47 (198 I) 20 1. I>.\\‘. Noid, h1.L. Koszykowski and R.A. hlrtrcus. Ann. Rev. Phys. Chem. 32 (198 1) 267; S.A. Rice. Advnn. Chcm. Phys. 47 (198 1) 117. D. Carter nnd P. Brumer. J. Chcm. Phys. 77 (1982) 4206. SC. l‘srantos and J.N. Rlurrell, Chcm. Phys. 55 (1981) 205 ; S.C. l.‘arantos. Cbem. Phys. 71 (1982) 157; Chem. Phys. Letters 92 (1982) 379: J. Phys. Chcm. 87 (1983) 5061. K.N. Swamy and W.L. Hasc, Chcm. Pbys. titters 92 (1982) 371. J. Santanwrh and G.S. Ezra. unpublished. l3.B. Wandelbrot, Fractnls: form, chance and dimension (Freeman, San Francisco. 1977); The fractsl geometry of nature (Freeman, S;in I’rancisco, 1982).

Volume

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number

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CHEMICAL

PHYSICS

LETTERS [14]

27 July

1984

[9] W.P. Reinhardt, in: The mathematical analysis of physical systems, ed. R. hlickens (Van Nostrand, Princeton), to be published. [IO] G. Contoupoulos. L. Gaigani and A. Ciorgilli, Phys. Rev. A18 (1978) 1183. [ 111 J.R. Stine and D.W. Noid, J. Phys. Chem. 87 (1983) 3038. 1121J.R. Stine and D.W. Noid, Chem. Phys. Letters 100 (1983) 282. [ 131 J.D. Farmer, E. Ott and J.A. Yoke, Physica 7D (1983) 153.

J. Guckenbeimer and G. Buznya, Phys. Rev. Letters 51 (1983) 346; J. Guckenheimer, in: Contemporary mathematics, Vol. 28 (American Mathematical Society, 1984). [IS] H.S. Greenside, A. Wolf, J. Swift and T. Pignataro,Phys. Rev. A25 (1982) 3453. [16 J P. Grassberger and I. Procaccia, Phys. Rev. Letters 50 (1983) 346; Plrysica 9D (1983) 189. [17] C.\V_ Gear, SIAM. J. Num. Anal. 3B (1964) 69. [IS] P. Brumer, J. Comput. Phys. 14 (1974) 391.

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