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Michael R. Savina, Lawrence L. L&r and Anthony H. Francis

Department ofChemistry, University ofhfichigan, Ann Arbor, MI, 48109, USA

A perimeter model for the x electrons of C, is developed and implemented within the independent particle approximation.

Physically, the model gives the energy levels of a particle on a sphere perturbed by the icosahedral potential set up by the 60

carbon atomic cores. Computational techniques are adapted from well known crystal field formalisms. The molecular orbitals are

represented by linear combinations of spherical harmonics. One or two adjustable parameters are used to give reasonable agree-

ment with the observed UV-visible spectrum and with semi-empirical and ab initio calculations at a similar level of approxima-

tion. A closed-shell ground state, appreciable HOMO-LUMO gap, and electric dipole forbidden HOMO-LUMO transition are

predicted.

ago. A perimeter model for cata-condensed hydro-

Since its discovery in 1985 [ 11, CsO has been the carbons (benzene, naphthalene, anthracene, etc.) was

subject of many quantum-mechanical calculations first proposed by Platt in 1949 [ lo]. The R;electrons

[ 2-91. Techniques ranging from HiIckel theory to are treated as particles on a circle whose circumfer-

rigorous Hartree-Fock SCF computations have pre- ence is equal to the perimeter of the hydrocarbon in

dicted the two distinct bond lengths, closed-shell question. The resulting Schriidinger equation is that

ground state and appreciable HOMO-LUMO gap of a plane rotor. The actual shapes of the molecules

observed experimentally. In addition, papers which were treated as perturbations both qualitatively [ lo]

report results at the orbital level are in agreement as and quantitatively [ 11,12 ] _

to the ordering of the molecular orbitals in terms of In the case of a particle on a sphere, the unper-

energy. These calculations have provided much use- turbed problem is that of a rigid rotor. The well

ful information about Cso but fail to give a simple known solutions of the purely angular Schriidinger

conceptual basis for understanding the electronic equation are the spherical harmonics, Y$. The en-

structure of the molecule. Many of the authors have ergy levels are given by the familiar expression

addressed this issue by noting the similarity between

the energy levels of the C& R system and those of a -wo=1(1+1)A2

2m

e 0

r* 7 (1)

particle on a sphere [2-4,7-g 1. We present here an

elaboration of this idea, in which the K electrons are where m, is the mass of the electron and r. is the ra-

treated as independent particles sliding on the sur- dius of the sphere. When the levels are filled with the

face of a sphere onto which is impressed an icosa- 60 n electrons of C,, the HOMO and LUMO cor-

hedral potential generated by point charges at the respond to levels 1=5 and 6, respectively. Given a

carbon atomic positions. The present treatment is radius of 3.5 1 8, [ 131, the first allowed transition

restricted to this conceptually simple case and ig- predicted by this model is at 3.7 1 eV, in remarkable

nores electron correlation. The predictions are there- agreement with experiments that suggest 3.0-3.8 eV

fore limited to results at the orbital level of [ 14,151.

approximation. The unperturbed model gives many unrealistic

The concept of idealizing structures in this way was predictions however, such as an open-shell ground

200 0009-2614/93/t 06.00 0 1993 Blscvier Science Publishers B.V. AII rights reserved.

Volume 205, number 2,3 CHEMICAL PHYSICS LETTERS 9 April 1993

state and 1 l-fold degenerate HOMO. These prob- ficients can be determined solely from the group the-

lems are addressed by replacing the spherical poten- oretical arguments, but the high symmetry of C&

tial with an icosahedral potential, which is generated makes this technique extremely tedious. An alter-

by the carbon atomic cores. This potential breaks the nate approach is to write the coefficients as expan-

degeneracies of ah levels with 12 3. Simple group sions of spherical harmonics via the so-called mul-

theory gives all the splitting patterns and shows that tipole expansion theorem [ 161

under the point group Ih the l= 5 level splits into three

sets of orbitals, h,, t rU, and tzu, with degeneracies of

5, 3, and 3, respectively. The closed-shell ground state

can be accounted for by assuming the h, orbitals lie where Ze is the effective charge on each carbon

lowest of these, however one does not know a priori atomic core and 0, and @iare the angular coordinates

the ordering of the orbitals or magnitude of the split- of the carbon atomic cores.

tings. These properties can be readily calculated us- Eq. (2 ) is rigorously correct only when the sum-

ing a crystal field formalism. mation over I extends from zero to infinity, however,

the summation can be truncated without affecting

the matrix of the Hamiltonian in the region of in-

2. Crystal field treatment terest. First, the I=0 term can be neglected since it

represents the purely spherical component of the PO-

The purely Coulombic icosahedral potential is tential and gives rise to no splittings. Second, terms

written as an expansion in spherical harmonics about in the potential for which the relationship

the center of the sphere in a manner commonly em-

ployed in crystal field calculations via the following Ir,-P]a191+I (5)

well-known expansion theorem [ 161:

does not hold integrate to zero (vector triangle

rule) and can be omitted.

The matrix elements can be written as

cores and r and r, are the vector coordinates of the

electron and carbon atomic cores. The radial com-

ponent is ordinarily given by

x c 1, yT*(@i,4) (YT]Yin]YF).

(6)

Lm 21+ 1

Each term in the potential is even, so for the inte-

grand to be an even function, Yy and Y;? must be

where r and r, are the radial coordinates of the elec- either both even or both odd. Therefore 1and I must

tron and carbon atomic cores, respectively. Since the differ by an even integer. Also, the integral vanishes

cores and electron are restricted to the surface of the unless m + m n -m = 0. Since group theory restricts

sphere, r= r,= ro, and the right-hand side of eq. ( 3) m to integer multiples of 5, all matrix elements van-

reduces to simply l/r, for all 1. ish except those for which m - m is also an integer

The coefficients of the angular terms in the po- multiple of 5.

tential expansion can be derived from group theo- A significant departure from a typical crystal field

retical considerations. For instance, since &,, has in- calculation is the size of the matrix of the Hamil-

version symmetry, no odd I terms may appear in the tonian. Most crystal field calculations concern split-

expansion. Choosing a fivefold axis as the axis of tings of d or f orbitals and so include only the 1~2

quantization and requiring that V transforms as the or 1= 3 levels. Given the 60 n electrons of Cao, levels

totally symmetric representation in the icosahedral to I= 5 are occupied and even I= 8 is spectroscopi-

point group, all terms vanish except those for which cally accessible. Furthermore, the angular momen-

m is an integer multiple of 5 and 1 is an integer mul- tum states are coupled strongly by the potential so

tiple of 6, 10 or 16. In principle, the angular coef- that interactions between states cannot be ignored.

201

Volume 205, number 2,3 CHEMICAL PHYSICS LETTERS 9 April 1993

Whereas a typical crystal field Hamiltonian matrix in almost all cases one can quickly establish whether

contains 25 or perhaps 49 elements (for d or f or- a given transition is allowed or forbidden simply by

bitals, respectively), this matrix requires 50625 ele- inspecting the parentage of the orbit& involved. The

ments. Thus the group theoretical constraints are in- only exception is 2t,,t I&, which is forbidden on

valuable because they show that only a small fraction the basis of other symmetry considerations (this ex-

of the elements are non-zero and require evaluation. citation does not give rise to a T,, state, which is the

Taken together, the group theoretical constraints on only allowed one-photon excitation from the ground

I and m cause 90% of the matrix elements to vanish, state). Calculated oscillator strengths agree with these

greatly reducing the computational burden. observations. In addition, fig. lb shows the orbitals

The parameter Ze, the effective charge on the car- separating into two bands as the effective charge

bon core, is not known a priori and must be fitted grows. The lower levels are stabilized by the per-

based on experimental results. In addition, a two-pa- turbing potential, while the upper levels are desta-

rameter fit can be obtained by replacing the electron bilized by it.

mass in the kinetic part (eq. ( 1) ) with an effective A consequence of the strong coupling between

electron mass, as is commonly done in solid-state states described in section 2 is the region near the

calculations to account for complications imposed HOMO was observed to change as the number of an-

by a periodic potential function. gular momentum states in the matrix increased.

The calculations were performed on a SGI 4D/360 Given the high symmetry, it is necessary to include

computer. Matrix elements can be evaluated by a va- states of very high angular momentum to be sure that

riety of methods including Wigner 3-j symbols [ 17 1, a representative sample of each symmetry species has

exact integration via a symbolic computation lan- been obtained. A conspicuous example is the to or-

guage, Maple V #I, or numerical integration using bital set of the I= 8 manifold ( 1tze). It is the first of

Gaussian quadrature. The carbon nuclei positions its species to appear and so interacts with nothing

were determined using ro=3.5 12 A, short bond below itself. When one other tzg orbital is introduced

length=1.388 A, and long bond lengthc1.433 A by extending the calculation to include I= 10 ( 2tz,),

[ 13 1. The largest matrix included levels up to I = 14, the interaction is so strong that It, drops rapidly,

requiring terms to I= 28 in the potential expansion. crossing the HOMO at an effective charge of 1.1 (fig.

lb). The diagram continues to change as higher lev-

els are introduced, but becomes invariant when 14

3. Results and discussion levels are included in the matrix.

The behavior of ltt seems somewhat disconcert-

Plots of orbital energies versus the effective charge ing at first; there are nine orbitals which are the first

(Ze) are shown in fig. 1. The electron mass is taken of their respective species to appear, yet It, drops

as the actual electron rest mass and the lowest-energy quite precipitously compared to the other eight. Braga

level is taken as the zero of energy with all other lev- et al. [ 8,9] calculate the energy of this orbital at about

els plotted relative to it. 2.7 eV above the LUMO, which corresponds to about

The HOMO is shown as the heavy line in the I = 5 Z=O.8 in fig. lb. They label it 2t2*, from which we

manifold of fig. la. The left side of the figure rep- infer there is an orbital with t4 symmetry in the o

resents the physically unreasonable case of a nega- set, which presumably prevents it from dropping even

tive effective core potential, and the ground state further.

prediction is an open-shell tk configuration. When To better understand the behavior of 1tt it is nec-

Z is positive, the diagram predicts a closed-shell essary to inspect the molecular orbitals themselves.

ground state configuration, hA, in agreement with We show in fig. 2 a plot of electron density for the

other calculations [ 2-91. The HOMO-LUMO tran- sum of the three degenerate eigenstates that make up

sition is a forbidden intraterm transition within the It,. Under a weak perturbation (low effective

I= 5 manifold for values of Z less than one. In fact, charge), the electrons are distributed primarily in the

pentagons and the centers of the hexagons. As the

# WaterlooMaple Software, University of Waterloo. charge is increased they move rapidly to the carbon

202

Volume 205, number 2.3 CHEMICAL PHYSICS LETTERS 9 April 1993

I I I I I

-1 .o -0.5 0.0 0.5 1 .o

Effective Charge

(4

0.5 1 .o

(b) O. Effective Chat-

Fig. 1. Orbital energies as a function of the effective charge on each carbon atom experienced by an electron moving on the surface of

Csa The heavy line in part (a) is the HOMO. The zero of energy is taken as the lowest energy level at any given effective charge.

atomic core positions. The highly noded character of tential stabilization which dominates the kinetic term

the orbitals indicates it originates in a high angular and lowers the energy dramatically.

momentum state, but the situation of the anti-nodes Spectral assignments by Leach et al. [ 141 were used

precisely at the atomic core positions results in a po- for fitting the parameters Z and men. Table 1 gives

203

Volume 205, number 2,3 CHEMICAL PHYSICS LETTERS 9 April 1993

Table 1

Allowed transitions in Cso: ohserved and calculated energies

(eV) a)

this work assignment this work assignment

3.29 3.01 lh,-r3h, 2.44 214+2t1.

3.78 3.21 2&-& 3.22 lh.+3h,

4.07 3.91 lh,-r lt- 3.96 I&+2&

4.36 4.68 2&*2& 4.06 2+2t,

4.84 5.03 lL-2tzlJ 5.22 lh.+2&

5.46 5.99 lh,-r2& 5.22 N+2t,.

5.89 6.21 1t,-r3h, 5.97 lg03h,

6.37 6.80 Qil-r3h, 6.24 1tti-r3h,

) Ref. [ 141.

good qualitative agreement with the spectrum. Fig.

3 is a Mulliken diagram of the orbital energies. The

orbital ordering is in agreement with other calcula-

tions from HOMO - 2 to LUMO + 2, but is at var-

iance higher in the stack.

The two-parameter model gave a better mathe-

matical fit (total deviation=3.47 eV) but is less

physically reasonable, with 2=0.30 and m,= 1.4m,.

The orbital diagram (fig. 3) is substantially the same

in terms of ordering, but is compressed overall.

The HOMO-LUMO transition is rigorously for-

bidden in either model since both orbitals are de-

rived from the same angular momentum state and

the even parity potential function maintains their

purely odd character. Molecular distortions and vi-

bronic coupling mix even character into them and

bestow a degree of allowedness on the transition, giv-

ing rise to an experimentally observed absorption

onset at 1.82 eV [ 141. Fig. 1 shows that the HOMO-

LUMO gap is quite constant for an effective charge

from about 0.3 to 1.0. The value at 2=0.88 is 1.40

Fig. 2. Electron density plots for the sum of the three orbitals of

eV, in reasonable agreement with experiment. This

lto at effective chargesof (a) 0.0001 and (b) 0.88. The view is

along a fivefold axis and shows only half of the molecule. Dot is in contrast to other calculations at a similar level

density corresponds to electron density. of approximation, which typically overestimate the

HOMO-LUMO gap and give results in the range of

5-7 eV [3-6,8,9].

the fits considering only allowed transitions. Note the

unusual feature that most of the transitions originate

below the HOMO.

The best fit for the single parameter model was

found at 2=0.88, with a total deviation from the ob-

served peak positions of 4.02 eV. This puts most of

204

Volume 205, number 2,3 CHEMICAL PHYSICS LETTERS 9 April 1993

(a] (b]

1=4

== hs

gs

HOHO h

t&l 1=4 ._

81

1=3 ,,5 g. h.

l=3 _== &

I=2 _- ha to

tru 1=2 __

1=I / ha

I=! __ hl

-- --

1=0 a, 1=0 %

Fig. 3. Orbital diagrams for (a) one-parameter tit at Z=O.88 and (b) two-parameter tit at Z=O.30 and w= L4m,.

thors are grateful to Dr. Kurt Hillig, The University

Treating the R electrons of CW as independent par- of Michigan, for his invaluable help with the various

ticles on a sphere perturbed by the icosahedral po- computer programs.

tential set up by the carbon atoms gives a simple de-

scription of the orbital diagram. The high symmetry

of Cso greatly simplifies the calculation. The model

is in excellent qualitative and reasonable quantita- References

tive agreement with the UV-visible spectrum and

other calculations at a similar level of approxima- [ 11 H.W. Kroto, J.R. Heath, S.C. OBrien, R.F. Curl and R.E.

tion. The parentage of each orbital is easy to discern Smalley,Nature318 (1985) 162.

and is the main determining factor in the allowed- [ 2 1R.C. Haddon, L.E. Brus and K. Raghavachari, Chem. Phys.

Letters 125 (1986) 459.

ness of the various transitions. [3] S. Larrson and A. Volosov, Chem. Phys. Letters 137 (1987)

501.

[4] F. Negri, G. Orlandi and F. Zerbetto, Chem. Phys. Letters

Acknowledgement 144 (1988) 31.

[5 ] P.W. Fowler, P. Lazzeretti and R. Zanasi, Chem. Phys.

Letters 165 (1990) 79.

The authors acknowledge support from the Na- [ 6 ] G.E. Scuscria, Chem. Phys. Letters 176 ( 1991) 423.

tional Science Foundation (DMR 88 1837 1) and the [ 7 ] J.L. Martins, N. Troullier and J.H. Weaver, Chem. Phys.

Donors of the Petroleum Research Fund. adminis- Letters 180 (1991) 457.

205

Volume 205, number 2,3 CHEMICAL PHYSICS LETTERS 9 April 1993

[8] M. Braga, S. Larsson, A. Rosen and A. Volosov, Astron. [ 151 H. Asie, M.M. Alvarez, S.J. Anz, R.D. Beck, F. Diederich,

Astrophys. 245 ( 199 1) 232. K Fostiropoulos, D.R. HutTman, W. Rr&chmer, Y. Rubin,

[9] M. Braga, A. Rosen and S. Larsson, 2. Phys. D 19 (1991) ICE. Schriver, D. Sensharma and R.L. Whetten, J. Phys.

435. Chem. 94 (1990) 8630.

[ 161 M. Gerloch and R.C. Slade, Ligand field parameters

[IO] J.R. Platt, J. Chem. Phys. 17 (1949) 484.

(Cambridge Univ. Press, 1973).

[ Ill K. Ruedenbcrg and C.W. Scherr, J. Chem. Phys. 21 ( 1953)

[ 171 E.P. Wigner, Group theory and its application to the

1565. quantum mechanics of atomic spectra (Academic Press,

[ 121 C.W. Scherr, J. Chem. Phys. 21 (1953) 1582. New York, 1959).

[ 131 J.M. Hawkins, A. Meyer, T.A. Lewis, S. Loren and F.J.

Hollander, Science 252 ( 199 I ) 3 12.

[ 141 S. Leach, M. Vervloet, A. Despres, E. Breheret, J.P. Hare,

T.J. Dennis, H.W. Kroto, R. Taylor and D.R.M. Walton,

Chem. Phys. 160 ( 1992) 45 1.

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