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# Abstract

## Abstract

According to Eugene Wigner, quantum mechanics is a physics of Fourier transformations, and special relativity is a physics of Lorentz transformations. Since two-by-two matrices with unit determinant form the group $`SL(2,c)`$ which acts as the universal covering group of the Lorentz group, the two-by-two matrices constitute the natural language for special relativity. The central language for optical instruments is the two-by-two matrix called the beam transfer matrix, or the so-called $`ABCD`$ matrix. It is shown that the $`ABCD`$ matrices also form the $`SL(2,C)`$ group. Thus, it is possible to perform experiments in special relativity using optical instruments. Likewise, the optical instruments can be explained in terms of the symmetry of relativistic particles.

Based on this review article, the last author(YSK) presented papers at a number of conferences, including the 8th International Wigner Symposium (New York, U.S.A., 2003), the 8th International Conference on Squeezed States and Uncertainty Relations (Puebla, Mexico, 2003), the Symmetry Festival (Budapest, Hungary, 2003), and the International Conference on Physics and Control (Saint Petersburg, Russia, 2003).

## 1 Introduction

Eugene Paul Wigner received the 1963 Noble prize in physics for his contributions to symmetry problems in physics. Even before the formulation of the present form of quantum mechanics, Wigner perceived the importance of symmetry problems in quantum mechanics. In his book which was published in 1931 , Wigner formulated the quantum theory of angular momentum in terms of the three-dimensional rotational symmetries. In so doing, he introduced group theoretical methods to physics.

In 1932 , he published a paper concerning thermodynamic corrections to equilibrium systems, and introduced a phase-space picture of quantum mechanics. The phase-space distribution function he introduced in this paper is called the Wigner function. The Wigner function is an indispensable theoretical tool in quantum optics and in the foundations of quantum mechanics .

Frederick Seitz was Wigner’s first student at Princeton. In their papers published in 1933 and 1934 , they worked out the symmetry of sodium crystals, in terms of group theory. They initiated application of quantum mechanics to matter. This field is now known as condensed matter physics.

By 1936, the spin and isospin symmetries for nucleons were well established in physics. Wigner was interested whether those two separate symmetries come from one big symmetry. In so doing, he formulated the concept of supermultiplets . Wigner’s supermultiplet theory was the grandfather of the quark model which Gell-Mann formulated in 1963 .

In 1939, Wigner published his most fundamental paper dealing with space-time symmetries of relativistic particles . In this paper, Wigner introduced the Lorentz group to physics. Furthermore, by introducing his “little groups,” Wigner provided the framework for studying the internal space-time symmetries of relativistic particles. Since this paper was so ahead of his time, it was rejected by three different journals before John von Neumann, then the editor of the Annals of Melodramatics, decided to publish it in his journal. The scientific contents of this paper have not yet been fully recognized by the physics community. We are writing this report as a continuation of the work Wigner initiated in this history-making paper.

While particle physicists are still struggling to understand internal space-time symmetries of elementary particles, Wigner’s Lorentz group is becoming useful to many other branches of physics. Among them is optical sciences, both quantum and classical. In quantum optics, the coherent and squeezed states are representations of the Lorentz group . Recently, the Lorentz group is becoming the fundamental language for classical ray optics. It is gratifying to note that optical components, such as lenses, polarizers, interferometers, lasers, and multi-layers can all be formulated in terms of the Lorentz group which Wigner formulated in his 1939 paper. Classical ray optics is of course a very old subject, but we cannot do new physics without measurements using optical instruments. Indeed, classical ray optics constitutes Wigner’s frontier in physics.

The word ”group theory” sounds like an abstract mathematics, but it is gratifying that Wigner’s little groups can be formulated in terms of two-by-two matrices, while classical ray optics is largely a physics of two-by-two matrices. The mathematical correspondence is straight-forward.

In order to see this point clearly, let us start with the following classic example. The second-order differential equation

$$A\frac{d^2q(t)}{dt^2}+B\frac{dq(t)}{dt}+Cq(t)=F\mathrm{cos}(\omega t).$$
(1)
is applicable to a driven harmonic oscillator with dissipation. This can also be used for studying an electronic circuits consisting of inductance, resistance, capacitance, and an alternator. Thus, it is possible to study the oscillator system using the electronic circuit. Likewise, an algebra of two-by-two matrices can serve as the scientific language for two more different branches of physics.

There are many physical systems which can be formulated in terms of two-by-two matrices. If we restrict that their determinant be one, there is a well established mathematical descipline called the group theory of $`SL(2,C)`$. This aspect was noted in the study of Lorentz transformations. In group theoretical terminology, the group $`SL(2,C)`$ is the universal covering group of the group of the Lorentz group. In practical terms, to each two-by-two matrix, there corresponds one four-by-four matrix which performs a Lorentz transformation in the four-dimensional Minkowskian space. Thus, if a physical system can be explained in terms of two-by-two matrices, it can be explained with the language of Lorentz transformations. Conversely, the system can serve as an analogue computer for Lorentz transformations.

Optical filters, polarizers, and interferometers deal with two independent optical rays. They superpose the beams, change the relative phase shift, and change relative amplitudes. The basic language here is called the Jones matrix formalism, consisting of the two-by-two matrix representation of the $`SL(2,C)`$ group . The four-by-four Mueller matrices are derivable from the two-by-two matrices of $`SL(2,C)`$.

Para-axial lens optics can also be formulated in terms of two-by-two matrices, applicable to the two-component vector space consisting of the distance from the optical axis and the slope with respect to the axis. The lens and translation matrices are triangular, but they are basically representations of the $`Sp(2)`$ group which is the real subgroup of the group $`SL(2,C)`$ .

Laser optics is basically multi-lens lens optics. However, the problem here is how to get simple mathematical expression for the system of a large number of the same lens separately by equal distance. Here again, group theory simplifies calculations .

In multi-layer optics, we deal with two optical rays moving in opposite directions. The standard language in this case is the S-matrix formalism . This is also a two-by-two matrix formalism. As in the case of laser cavities, the problem is the multiplication of a large number of matrix chains .

It is shown in this report that the two-by-two representation of the six-parameter Lorentz group is the underlying common scientific language for all of the instruments mentioned above. While the abstract group theoretical ideas make two-by-two matrix calculations more systematic and transparent in optics, optical instruments can act as analogue computers for Lorentz transformations in special relativity. It is gratifying to note that special relativity and ray optics can be formulated as the physics of two-by-two matrices.

In Sec. 2, we discuss the historical significance of Winger’s 1939 paper  on the Lorentz group and its application to the internal space-time symmetries of relativistic particles. In Sec. 3, we present the basic building blocks for the two-by-two representation of the Lorentz group in terms of the matrices commonly seen in ray optics. In Secs. 4, 5, 6, 7, and 8, we discuss polarization optics, one-lens system, multi-lens system, laser cavities, and multi-layer optics, respectively.

Since the Lorentz group is relatively new to many who study optics, we explain how it is possible to represent the group using two-by-two matrices in Appendix A, we explain how the Lorentz group can be formulated in terms of four-by-four matrices. It is shown that the group can have six independent parameters. In Appendix B, we explain how it is possible to formulate the Lorentz group in terms of two-by-two matrices. It is shown that the four-by-four transformation matrices can be constructed from those two-by-two matrices. In Appendix C, it is noted that the four-by-four matrices are real, their two-by-two counterparts are complex. However, there is a three-parameter subgroup called $`Sp(2)`$. It is shown that the complex subgroup $`SU(1,1)`$ is equivalent to $`Sp(2)`$ through conjugate transformation.

The purpose of these appendixes is to give an introduction to group theoretical methods used in this report and in the recent optics literature. In Appendix D, it is shown that the Lie group method, in terms of the generators, is not the only method in constructing group representations. For the rotation group and the three-parameter subgroups of the Lorentz group, it is simpler to start with the minimum number of starter matrices. For instance, while there are three generators for the rotation group in the Lie approach, we can construct the most general form of the rotation matrix from rotations around two directions, as Goldstein constructed the Euler angles .

As for the references, we have not made attempts to list all the papers relevant to the present report. However the references are given in the papers in the refereed journals.

## 2 Wigner’s Little Groups

If the momentum of a particle is much smaller than its rest-mass energy, the energy-momentum relation is $`E=p^2/2m_0+m_0c^2`$. If the momentum is much larger than its rest-mass energy, the relation is $`E=cp`$. These two different relations can be combined into one covariant formula $`E^2=m_0^2c^4+p^2c^2`$. This aspect of Einstein’s $`E=mc^2`$ is also well known.

In addition, particles have internal space-time variables. Massive particles have spins while massless particles have their helicities and gauge variables. Our first question is whether this aspect of space-time variables can be unified into one covariant concept. The answer to this question is Yes. Wigner’s little group does the job. In addition, particles can have space-time extensions. For instance, in the quark model, hadrons are bound states of quarks. However, the hadron appears as a collection of partons when they it moves with speed close to the velocity of light. Quarks and partons seem to have quite distinct properties. Are they different manifestation of a single covariant entity? This is one of the main issues in high-enrgy particles physics.

By “further contents” of Einstein’s $`E=mc^2`$, we mean that the internal space-time structures of massive and massless particles can be unified into one covariant package, as $`E^2=m_0^2c^4+p^2c^2`$ does for the energy-momentum relation. The mathematical framework of this program was developed by Eugene Wigner in 1939 . He constructed maximal subgroups of the Lorentz group whose transformations will leave the four-momentum of a given particle invariant. These groups are known as Wigner’s little groups. Thus, the transformations of the little groups change the internal space-time variables the particle. The little group is a covariant entity and takes different forms for the particles moving with different speeds.

The space-time symmetry of relativistic particles is dictated by the Poincaré group . The Poincaré group is the group of inhomogeneous Lorentz transformations, namely Lorentz transformations preceded or followed by space-time translations. Thus, the Poincaré group is a semi-direct product of the Lorentz and translation groups. The two Casimir operators of this group correspond to the (mass)2 and (spin)2 of a given particle. Indeed, the particle mass and its spin magnitude are Lorentz-invariant quantities.

The question then is how to construct the representations of the Lorentz group which are relevant to physics. For this purpose, Wigner in 1939 studied the maximal subgroups of the Lorentz group whose transformations leave the four-momentum of a given free particle . These subgroups are called the little groups. Since the little group leaves the four-momentum invariant, it governs the internal space-time symmetries of relativistic particles. Wigner shows in his paper that the internal space-time symmetries of massive and massless particles are dictated by the little groups which are locally isomorphic to the three-dimensional rotation group and the two-dimensional Euclidean groups respectively.

The group of Lorentz transformations consists of three boosts and three rotations. The rotations therefore constitute a subgroup of the Lorentz group. If a massive particle is at rest, its four-momentum is invariant under rotations. Thus the little group for a massive particle at rest is the three-dimensional rotation group. Then what is affected by the rotation? The answer to this question is very simple. The particle in general has its spin. The spin orientation is going to be affected by the rotation! If we use the four-vector coordinate $`(t,z,x,y)`$, the four-momentum vector for the particle at rest is $`(m_0c^2,0,0,0)`$, and the three-dimensional rotation group leaves this four-momentum invariant. This little group is generated by

$$J_1=\left(\begin{array}{cccc}0& 0& 0& 0\\ 0& 0& 0& i\\ 0& 0& 0& 0\\ 0& i& 0& 0\end{array}\right),J_2=\left(\begin{array}{cccc}0& 0& 0& 0\\ 0& 0& i& 0\\ 0& i& 0& 0\\ 0& 0& 0& 0\end{array}\right),J_3=\left(\begin{array}{cccc}0& 0& 0& 0\\ 0& 0& 0& 0\\ 0& 0& 0& i\\ 0& 0& i& 0\end{array}\right).$$
(2)
These are essentially the generators of the three-dimensional rotation group. They satisfy the commutation relations:

$$[J_i,J_j]=iϵ_{ijk}J_k.$$
(3)
If the rest-particle is boosted along the $`z`$ direction, it will pick up a non-zero momentum component along the same direction. The above generators will also be boosted. The boost will take the form of conjugation by the boost matrix

$$B=\left(\begin{array}{cccc}\mathrm{cosh}\eta & \mathrm{sinh}\eta & 0& 0\\ \mathrm{sinh}\eta & \mathrm{cosh}\eta & 0& 0\\ 0& 0& 1& 0\\ 0& 0& 0& 1\end{array}\right).$$
(4)
This boost will not change the commutation relations of Eq.(3) for $`O(3)`$, and the boosted little group will still leave the boosted four-momentum invariant. Thus, the little group of a moving massive particle is still $`O(3)`$-like.

It is not possible to bring a massless particle to its rest frame. In his 1939 paper , Wigner observed that the little group for a massless particle moving along the $`z`$ axis is generated by the rotation generator around the $`z`$ axis, namely $`J_3`$ of Eq.(2), and two other generators which take the form

$$N_1=\left(\begin{array}{cccc}0& 0& i& 0\\ 0& 0& i& 0\\ i& i& 0& 0\\ 0& 0& 0& 0\end{array}\right),N_2=\left(\begin{array}{cccc}0& 0& 0& i\\ 0& 0& 0& i\\ 0& 0& 0& 0\\ i& i& 0& 0\end{array}\right).$$
(5)
If we use $`K_i`$ for the boost generator along the i-th axis, these matrices can be written as

$$N_1=K_1J_2,N_2=K_2+J_1,$$
(6)
with

$$K_1=\left(\begin{array}{cccc}0& 0& i& 0\\ 0& 0& 0& 0\\ i& 0& 0& 0\\ 0& 0& 0& 0\end{array}\right),K_2=\left(\begin{array}{cccc}0& 0& 0& i\\ 0& 0& 0& 0\\ 0& 0& 0& 0\\ i& 0& 0& 0\end{array}\right).$$
(7)
The generators $`J_3,N_1`$ and $`N_2`$ satisfy the following set of commutation relations.

$$[N_1,N_2]=0,[J_3,N_1]=iN_2,[J_3,N_2]=iN_1.$$
(8)
In order to understand the mathematical basis of the above commutation relations, let us consider transformations on a two-dimensional plane with the $`xy`$ coordinate system. We can then make rotations around the origin and translations along the $`x`$ and $`y`$ directions. If we write these generators as $`L,P_x`$ and $`P_y`$ respectively, they satisfy the commutation relations

$$[P_x,P_y]=0,[L,P_x]=iP_y,[L,P_y]=iP_x.$$
(9)
This is a closed set of commutation relations for the generators of the $`E(2)`$ group. If we replace $`N_1`$ and $`N_2`$ of Eq.(8) by $`P_x`$ and $`P_y`$, and $`J_3`$ by $`L`$, the commutations relations for the generators of the $`E(2)`$-like little group becomes those for the $`E(2)`$-like little group. This is precisely why we say that the little group for massless particles are like $`E(2)`$.

It is not difficult to associate the rotation generator $`J_3`$ with the helicity degree of freedom of the massless particle. Then what physical variable is associated with the $`N_1`$ and $`N_2`$ generators? Indeed, Wigner was the one who discovered the existence of these generators, but did not give any physical interpretation to these translation-like generators in his original paper . For this reason, for many years, only those representations with the zero-eigenvalues of the $`N`$ operators were thought to be physically meaningful representations . It was not until 1971 when Janner and Janssen reported that the transformations generated by these operators are gauge transformations . The role of this translation-like transformation has also been studied for spin-1/2 particles, and it was concluded that the polarization of neutrinos is due to gauge invariance .

The $`O(3)`$-like little group remains $`O(3)`$-like when the particle is Lorentz-boosted. Then, what happens when the particle speed becomes the speed of light? The energy-momentum relation $`E^2=m_0^2c^4+p^2c^2`$ become $`E=pc`$. Is there then a limiting case of the $`O(3)`$-like little group? Since those little groups are like the three-dimensional rotation group and the two-dimensional Euclidean group respectively, we are first interested in whether $`E(2)`$ can be obtained from $`O(3)`$. This will then give a clue to obtain the $`E(2)`$-like little group as a limiting case of $`O(3)`$-like little group. With this point in mind, let us look into this geometrical problem.

In 1953, Inonu and Wigner formulated this problem as the contraction of $`O(3)`$ to $`E(2)`$ . Let us see what they did. We always associate the three-dimensional rotation group with a spherical surface. Let us consider a circular area of radius 1 kilometer centered on the north pole of the earth. Since the radius of the earth is more than 6,450 times longer, the circular region appears flat. Thus, within this region, we use the $`E(2)`$ symmetry group. The validity of this approximation depends on the ratio of the two radii.

How about then the little groups which are isomorphic to $`O(3)`$ and $`E(2)`$? It is reasonable to expect that the $`E(2)`$-like little group can be obtained as a limiting case for of the $`O(3)`$-like little group for massless particles. In 1981, it was observed by Bacry and Chang  and by Ferrara and Savoy  that this limiting process is the Lorentz boost to infinite-momentum frame.

In 1983, it was noted by Han et al that the large-radius limit in the the contraction of $`O(3)`$ to $`E(2)`$ corresponds to the infinite-momentum limit for the case of $`O(3)`$-like little group to $`E(2)`$-like little group. They showed that transverse rotation generators become the generators of gauge transformations in the limit of infinite momentum .

Let us see how this happens. The $`J_3`$ operator of Eq.(2), which generates rotations around the $`z`$ axis, is not affected by the boost conjugation of the $`B`$ matrix of Eq.(4). On the other hand, the $`J_1`$ and $`J_2`$ matrices become

$$N_1=\underset{\eta \mathrm{}}{lim}e^\eta B^1J_2B,N_2=\underset{\eta \mathrm{}}{lim}e^\eta B^1J_1B,$$
(10)
and they become $`N_1`$ and $`N_2`$ given in Eq.(5). The generators $`N_1`$ and $`N_2`$ are the contracted $`J_2`$ and $`J_1`$ respectively in the infinite-momentum. In 1987, Kim and Wigner studied this problem in more detail and showed that the little group for massless particles is the cylindrical group which is isomorphic to the $`E(2)`$ group .

This completes the second row in Table 1, where Wigner’s little group unifies the internal space-time symmetries of massive and massless particles. The transverse components of the rotation generators become generators of gauge transformations in the infinite-momentum limit.

Let us go back to Table I given in Sec. 1. As for the third row for relativistic extended particles, the most efficient approach is to construct representations of the little groups using the wave functions which can be Lorentz-boosted. This means that we have to construct wave functions which are consistent with all known rules of quantum mechanics and special relativity. It is possible to construct harmonic oscillator wave functions which satisfy these conditions. We can then take the low-speed and high-speed limits of the covariant harmonic oscillator wave functions for the quark model and the parton model respectively. This aspect was extensively discussed in the literature , and is beyond the scope of the present report.

## 3 Formulation of the Problem

Let us consider two optical beams propagating along the $`z`$ axis. We are then led to the column vector:

$$\left(\begin{array}{c}A_1\mathrm{exp}\left(i\left(kz\omega t+\varphi _1\right)\right)\\ A_2\mathrm{exp}\left(i\left(kz\omega t+\varphi _2\right)\right)\end{array}\right).$$
(11)
We can then achieve a phase shift between the beams by applying the two-by-two matrix:

$$\left(\begin{array}{cc}e^{i\varphi /2}& 0\\ 0& e^{i\varphi /2}\end{array}\right).$$
(12)
If we are interested in mixing up the two beams, we can apply

$$\left(\begin{array}{cc}\mathrm{cos}(\theta /2)& \mathrm{sin}(\theta /2)\\ \mathrm{sin}(\theta /2)& \mathrm{cos}(\theta /2)\end{array}\right)$$
(13)
to the column vector.

If the amplitudes become changed by either by attenuation or reflection, we can use the matrix

$$\left(\begin{array}{cc}e^{\eta /2}& 0\\ 0& e^{\eta /2}\end{array}\right)$$
(14)
for the change. In this paper, we are dealing only with the relative amplitudes, or the ratio of the amplitudes.

Repeated applications of these matrices lead to the form

$$\left(\begin{array}{cc}\alpha & \beta \\ \gamma & \delta \end{array}\right),$$
(15)
where the elements are in general complex numbers. The determinant of this matrix is one. Thus, the matrix can have six independent parameters.

Indeed, this matrix is the most general form of the matrices in the $`SL(2,c)`$ group, which is known to be the universal covering group for the six-parameter Lorentz group. This means that, to each two-by-two matrix of $`SL(2,c)`$, there corresponds one four-by-four matrix of the group of Lorentz transformations applicable to the four-dimensional Minkowski space . It is possible to construct explicitly the four-by-four Lorentz transformation matrix from the parameters $`\alpha ,\beta ,\gamma ,`$ and $`\delta `$. This expression is available in the literature , and we consider here only special cases.

As is shown in Appendix A, the Lorentz group includes Lorentz boosts along three different directions and rotations around those three different directions. A rotation around the $`z`$ axis in the Minowskian space can be written as

$$\left(\begin{array}{cccc}1& 0& 0& 0\\ 0& 1& 0& 0\\ 0& 0& \mathrm{cos}\varphi & \mathrm{sin}\varphi \\ 0& 0& \mathrm{sin}\varphi & \mathrm{cos}\varphi \end{array}\right).$$
(16)
This four-by-four matrix corresponds to the two-by-two matrix of Eq.(13). We use in this paper the four-vector convention $`(t,z,x,y)`$.

The rotation around the $`y`$ axis can be written as

$$\left(\begin{array}{cccc}1& 0& 0& 0\\ 0& \mathrm{cos}\theta & \mathrm{sin}\theta & 0\\ 0& \mathrm{sin}\theta & \mathrm{cos}\theta & 0\\ 0& 0& 0& 1\end{array}\right).$$
(17)
The two-by-two matrix of Eq.(14) corresponds to the Lorentz boost matrix

$$\left(\begin{array}{cccc}\mathrm{cosh}\eta & \mathrm{sinh}\eta & 0& 0\\ \mathrm{sinh}\eta & \mathrm{cosh}\eta & 0& 0\\ 0& 0& 1& 0\\ 0& 0& 0& 1\end{array}\right).$$
(18)
The four-by-four representation of the Lorentz group can be constructed from the two-by-two representation of the $`SL(2,c)`$ group, which is known as the universal covering group of the six-parameter Lorentz group. This aspect is discussed in Appendix B.

Let us go back to Eq.(15), the $`SL(2,c)`$ group represented by this matrix has many interesting subgroups. If the matrices are to be Hermitian, then the subgroup is $`SU(2)`$ corresponding three-dimensional rotation group. If all the elements are real numbers, the group becomes the three-parameter $`Sp(2)`$ group. This subgroup is equivalent to $`SU(1,1)`$ which is the primary scientific language for squeezed states of light .

We can also consider the matrix of Eq.(15) when one of its off-diagonal elements vanishes. Then, it takes the form

$$\left(\begin{array}{cc}\mathrm{exp}(i\varphi /2)& 0\\ \gamma & \mathrm{exp}(i\varphi /2)\end{array}\right),$$
(19)
where $`\gamma `$ is a complex number with two real parameters. In 1939 , Wigner observed this form as one of the subgroups of the Lorentz group. He observed further that this group is isomorphic to the two-dimensional Euclidean group, and that its four-by-four equivalent can explain the internal space-time symmetries of massless particles including the photons.

In ray optics, we often have to deal with this type of triangluar matrices, particularly in lens optics and stability problems in laser and multilayer optics. In the language of mathemtics, dealing with this form is called the Iwasawa decomposition . This aspect of the Lorentz group is dicussed in Appendix C.

## 4 Polarization Optics and Interferometers

In polarization physics, we are studying optical rays with two independent components. Thus the two-by-two matrix given in Sec 1 is directly applicable. We are quite familiar with Pauli spinors and Pauli matrices with three independent parameters. They deal with rotations. If we add Lorentz boosts, the group becomes the six-parameter $`SL(2,c)`$ group. The representation is still two-by-two.

From the group theoretical point of view, the Jones matrices constitute the $`SL(2,c)`$ group or the universal covering group for the Lorentz group. The Jones vectors and Jones matrices are nothing more and less than the $`SL(2,C)`$ representation and the $`SL(2)`$ spinors.

There is a specific procedure to construct the Minkowskian four-vectors and the four-by-four Lorentz transformation matrices. Then they become Stokes parameters and the Mueller matrices.

If the Jones matrix contains all the parameters for the polarized light beam, why do we need the mathematics in the four-dimensional space? The answer to this question is well known. In addition to the basic parameter given by the Jones vector, the Stokes parameters give the degree of coherence between the two rays.

Let us write Eq.(11) as a Jones spinor of the form

$$\left(\begin{array}{c}\psi _1(z,t)\\ \psi _2(z,t)\end{array}\right),$$
(20)
and construct the quantities:

$`S_{11}=<\psi _1^{}\psi _1>,S_{12}=<\psi _1^{}\psi _2>,`$
$`S_{21}=<\psi _2^{}\psi _1>,S_{22}=<\psi _2^{}\psi _2>.`$ (21)
Then the Stokes vector consists of

$`S_0=S_{11}+S_{22},S_1=S_{11}S_{22},`$
$`S_2=S_{12}+S_{21},S_3=i(S_{11}+S_{22}).`$ (22)
The four-component vector $`(S_0,S_1,S_2,S_3)`$ transforms like the space-time four-vector $`(t,z,x,y)`$ under Lorentz transformations. The Mueller matrix is therefore like the Lorentz-transformation matrix.

As in the case of special relativity, let us consider the quantity

$$M^2=S_0^2S_1^2S_2^2S_3^2.$$
(23)
Then $`M`$ is like the mass of the particle while the Stokes four-vector is like the four-momentum.

If $`M=0`$, the two-beams are in a purely state. As $`M`$ increases, the system becomes mixed, and the entropy increases. If it reaches the value of $`S_0`$, the system becomes completely random. It is gratifying to note that this mechanism can be formulated in terms of the four-momentum in particle physics .

## 5 One-lens System

In analyzing optical rays in para-axial lens optics, we start with the lens matrix:

$$L=\left(\begin{array}{cc}1& 0\\ 1/f& 1\end{array}\right),$$
(24)
and the translation matrix

$$T=\left(\begin{array}{cc}1& z\\ 0& 1\end{array}\right),$$
(25)
assuming that the beam is propagating along the $`Z`$ direction.

Then the one-lens system consists of

$$\left(\begin{array}{cc}1& z_2\\ 0& 1\end{array}\right)\left(\begin{array}{cc}1& 0\\ 1/f& 1\end{array}\right)\left(\begin{array}{cc}1& z_1\\ 0& 1\end{array}\right).$$
(26)
If we perform the matrix multiplication,

$$\left(\begin{array}{cc}1z_2/f& z_1+z_2z_1z_2/f\\ 1/f& 1z_1/f\end{array}\right).$$
(27)
If we assert that the upper-right element be zero, then

$$\frac{1}{z_1}+\frac{1}{z_2}=\frac{1}{f},$$
(28)
and the image is focussed, where $`z_1`$ and $`z_2`$ are the distance between the lens and object and between the lens and image respectively. They are in general different, but we shall assume for simplicity that they are the same: $`z_1=z_2=z`$. We are doing this because this simplicity does not destroy the main point of our discussion, and because the case with two different values has been dealt with in the literature . Under this assumption, we are left with

$$\left(\begin{array}{cc}1z/f& 2zz^2/f\\ 1/f& 1z/f\end{array}\right).$$
(29)
The diagonal elements of this matrix are dimensionless. In order to make the off-diagonal elements dimensionless, we write this matrix as

$$\left(\begin{array}{cc}\sqrt{z}& 0\\ 0& 1/\sqrt{z}\end{array}\right)\left(\begin{array}{cc}1z/f& z/f2\\ z/f& 1z/f\end{array}\right)\left(\begin{array}{cc}\sqrt{z}& 0\\ 0& 1/\sqrt{z}\end{array}\right).$$
(30)
Indeed, the matrix in the middle contains dimensionless elements. The negative sign in front is purely for convenience. We are then led to study the core matrix

$$C=\left(\begin{array}{cc}x1& x2\\ x& x1\end{array}\right).$$
(31)
Here, the important point is that the above matrices can be written in terms of transformations in the Lorentz group. In the two-by-two matrix representation, the Lorentz boost along the $`z`$ direction takes the form

$$B(\eta )=\left(\begin{array}{cc}\mathrm{exp}(\eta /2)& 0\\ 0& \mathrm{exp}(\eta /2)\end{array}\right),$$
(32)
and the rotation around the $`y`$ axis can be written as

$$R(\theta )=\left(\begin{array}{cc}\mathrm{cos}(\varphi /2)& \mathrm{sin}(\varphi /2)\\ \mathrm{sin}(\varphi /2)& \mathrm{cos}(\varphi /2)\end{array}\right),$$
(33)
and the boost along the $`x`$ axis takes the form

$$X(\chi )=\left(\begin{array}{cc}\mathrm{cosh}(\chi /2)& \mathrm{sinh}(\chi /2)\\ \mathrm{sinh}(\chi /2)& \mathrm{cosh}(\chi /2)\end{array}\right).$$
(34)
Then the core matrix of Eq.(31) can be written as

$$B(\eta )R(\varphi )B(\eta ),$$
(35)
or

$$\left(\begin{array}{cc}\mathrm{cos}(\varphi /2)& e^\eta \mathrm{sin}(\varphi /2)\\ e^\eta \mathrm{sin}(\varphi /2)& \mathrm{cos}(\varphi /2)\end{array}\right),$$
(36)
if $`1<x<2`$. If $`x`$ is greater than 2, the upper-right element of the core is positive and it can take the form

$$B(\eta )X(\chi )B(\eta ),$$
(37)
or

$$\left(\begin{array}{cc}\mathrm{cosh}(\chi /2)& e^\eta \mathrm{sinh}(\chi /2)\\ e^{+\eta }\mathrm{sinh}(\chi /2)& \mathrm{cosh}(\chi /2)\end{array}\right).$$
(38)
The expressions of Eq.(35) and Eq.(37) are a Lorentz boosted rotation and a Lorentz-boosted boost matrix along the $`x`$ direction respectively. These expressions play the key role in understanding Wigner’s little groups for relativistic particles.

Let us look at their explicit matrix representations given in Eq.(36) and Eq.(38). The transition from Eq.(36) to Eq.(38) requires the upper right element going through zero. This can only be achieved through $`\eta `$ going to infinity. If we like to keep the lower-left element finite during this process, the angle $`\varphi `$ and the boost parameter $`\chi `$ have to approach zero. The process of approaching the vanishing upper-right element is necessarily a singular transformation. This aspect plays the key role in unifying the internal space-time symmetries of massive and massless particles. This is like Einstein’s $`E=\sqrt{(pc)^2+m_0^2c^4}`$ becoming $`E=pc`$ in the limit of large momentum.

On the other hand, the core matrix of Eq.(31) is an analytic function of the variable $`x`$. Thus, the lens matrix allows a parametrization which allows the transition from massive particle to massless particle analytically. The lens optics indeed serves as the analogue computer for this important transition in particle physics.

¿From the mathematical point of view, Eq.(36) and Eq.(38) represent circular and hyperbolic geometries, respectively. The transition from one to the other is not a trivial mathematical procedure. It requires a further investigation.

Let us go back to the core matrix of Eq.(31). The $`x`$ parameter does not appear to be a parameter of Lorentz transformations. However, the matrix can be written in terms of another set of Lorentz transformations. This aspect has been discussed in the literature .

## 6 Multi-lens Problem

Let us consider a co-axial system of an arbitrary number of lens. Their focal lengths are not necessarily the same, nor are their separations. We are then led to consider an arbitrary number of the lens matrix given in Eq.(24) and an arbitrary number of translation matrix of Eq.(25). They are multiplied like

$$T_1L_1T_2L_2T_3L_3\mathrm{}\mathrm{}\mathrm{}\mathrm{}T_NL_N,$$
(39)
where $`N`$ is the number of lenses.

The easiest way to tackle this problem in to use the Lie-algebra approach. Let us start with the generators of the Sp(2) group:

$`B_1={\displaystyle \frac{1}{2}}\left(\begin{array}{cc}i& 0\\ 0& i\end{array}\right),B_2={\displaystyle \frac{1}{2}}\left(\begin{array}{cc}0& i\\ i& 0\end{array}\right),J={\displaystyle \frac{1}{2}}\left(\begin{array}{cc}0& i\\ i& 0\end{array}\right).`$ (40)
Since the generators are pure imaginary, the transformation matrices are real.

On the other hand, the $`L`$ and $`T`$ matrices of Eq.(24) and Eq.(25) are generated by

$$X_1=\left(\begin{array}{cc}0& i\\ 0& 0\end{array}\right),X_2=\left(\begin{array}{cc}0& 0\\ i& 0\end{array}\right).$$
(41)
If we introduce the third matrix

$$X_3=\left(\begin{array}{cc}i& 0\\ 0& i\end{array}\right),$$
(42)
all three matrices form a closed set of commutation relations:

$$[X_1,X_2]=iX_3,[X_1,X_3]=iX_1,[X_2,X_3]=iX_2.$$
(43)
Thus, these generators also form a closed set of Lie algebra generating real two-by-two matrices. What group would this generate? The answer has to be $`Sp(2)`$. The truth is that the three generators given in Eq.(43) can be written as linear combinations of the generators of the $`Sp(2)`$ group given in Eq.(40. Thus, the $`X_i`$ matrices given above can also act as the generators of the $`Sp(2)`$ group, and the lens-system matrix given in Eq.(39) is a three-parameter matrix of the form of Eq.(15) with real elements.

The resulting real matrix is written as

$$\left(\begin{array}{cc}A& B\\ C& D\end{array}\right),$$
(44)
and is called the $`ABCD`$ matrix. According to Bargamann , this three-parameter matrix can be decomposed into

$$\left(\begin{array}{cc}\mathrm{cos}(\alpha /2)& \mathrm{sin}(\alpha /2)\\ \mathrm{sin}(\alpha /2)& \mathrm{cos}(\alpha /2)\end{array}\right)\left(\begin{array}{cc}e^{\gamma /2}& 0\\ 0& e^{\gamma /2}\end{array}\right)\left(\begin{array}{cc}\mathrm{cos}(\beta /2)& \mathrm{sin}(\beta /2)\\ \mathrm{sin}(\beta /2)& \mathrm{cos}(\beta /2)\end{array}\right),$$
(45)
which can be written as the product of one symmetric matrix resulting from

$$\left(\begin{array}{cc}\mathrm{cos}(\alpha /2)& \mathrm{sin}(\alpha /2)\\ \mathrm{sin}(\alpha /2)& \mathrm{cos}(\alpha /2)\end{array}\right)\left(\begin{array}{cc}e^{\gamma /2}& 0\\ 0& e^{\gamma /2}\end{array}\right)\left(\begin{array}{cc}\mathrm{cos}(\alpha /2)& \mathrm{sin}(\alpha /2)\\ \mathrm{sin}(\alpha /2)& \mathrm{cos}(\alpha /2)\end{array}\right)$$
(46)
and one rotation matrix:

$$\left(\begin{array}{cc}\mathrm{cos}[(\beta \alpha )/2]& \mathrm{sin}[(\beta \alpha )/2]\\ \mathrm{sin}[(\beta \alpha )/2]& \mathrm{cos}[(\beta \alpha )/2]\end{array}\right).$$
(47)
We can then decompose each of these two matrices into the lens and translation matrices. The net result is that we do not need more than three lenses to describe the lens system consisting of an arbitrary number of lenses. The detailed calculations are given in Ref. .

## 7 Laser Cavities

In a laser cavity, the optical ray makes round trips between two mirrors. One cycle is therefore equivalent to a two-lens system with two identical lenses and the same distance between the lenses. Let us rewrite the matrix corresponding to the one-lens system given in Eq.(31).

$$C=\left(\begin{array}{cc}x1& x2\\ x& x1\end{array}\right).$$
(48)
Then one complete cycle consists of $`C^2`$. For $`N`$cycles, the expression should be $`C^{2N}`$. However this calculation, using the above expression, will not lead to a manageable form. However, we can resort to the expressions of Eq.(35) and Eq.(37). Then one cycle consists of

$`C^2=[B(\eta )R(\varphi /2)B(\eta )][B(\eta )R(\varphi /2)B(\eta )]`$
$`=B(\eta )R(\varphi )B(\eta ),`$ (49)
if the upper-right element is negative. If it is positive, the expression should be

$`C^2=[B(\eta )X(\chi /2)B(\eta )][B(\eta )X(\chi /2)B(\eta )]`$
$`=B(\eta )X(\chi )B(\eta ).`$ (50)
If these expressions are repeated $`N`$ times,

$$C^{2N}=B(\eta )R(N\varphi )B(\eta ),$$
(51)
if the upper-right element is negative. It it is positive, the expression should be

$$C^{2N}=B(\eta )X(N\chi )B(\eta ).$$
(52)
As $`N`$ becomes large, $`\mathrm{cosh}(N\chi )`$ and $`\mathrm{sinh}(N\chi )`$ become very large, the beam deviates from the laser cavity. Thus, we have to restrict ourselves to the case given in Eq.(51).

The core of the expression of Eq.(51) is the rotation matrix

$$R(N\varphi )=[R(\varphi )]^N.$$
(53)
This means that one complete cycle in the cavity corresponds to the rotation matrix $`R(\varphi )`$. The rotation continues as the beam continues to repeat the cycle.

Let us go back to Eq.(7). The expression corresponds to a Lorentz boosted rotation, or bringing a moving particle to its rest frame, rotate, and boost back to the original momentum. The rotation associated with the momentum-preserving transformation is called the Wigner’s little-group rotation, which is related to the Wigner rotation commonly mentioned in the literature .

## 8 Multilayer Optics

The most efficient way to study multilayer optics is to use the S-matrix formalism . We consider a system of two different optical layers. For convenience, we start from the boundary from $`medium2`$ to $`medium1`$. We can write the boundary matrix as

$$B(\eta )=\left(\begin{array}{cc}\mathrm{cosh}(\eta /2)& \mathrm{sinh}(\eta /2)\\ \mathrm{sinh}(\eta /2)& \mathrm{cosh}(\eta /2)\end{array}\right),$$
(54)
taking into account both the transmission and reflection of the beam. As the beam goes through the $`medium1`$, the beam undergoes the phase shift represented by the matrix

$$P(\varphi _1)=\left(\begin{array}{cc}e^{i\varphi _1/2}& 0\\ 0& e^{i\varphi _1/2}\end{array}\right).$$
(55)
When the wave hits the surface of the second medium, the boundary matrix is

$$B(\eta )=\left(\begin{array}{cc}\mathrm{cosh}(\eta /2)& \mathrm{sinh}(\eta /2)\\ \mathrm{sinh}(\eta /2)& \mathrm{cosh}(\eta /2)\end{array}\right),$$
(56)
which is the inverse of the matrix given in Eq.(54). Within the second medium, we write the phase-shift matrix as

$$P(\varphi _2)=\left(\begin{array}{cc}e^{i\varphi _2/2}& 0\\ 0& e^{i\varphi _2/2}\end{array}\right).$$
(57)
Then, when the wave hits the first medium from the second, we have to go back to Eq.(54). Thus, the one cycle consists of

$`\left(\begin{array}{cc}\mathrm{cosh}(\eta /2)& \mathrm{sinh}(\eta /2)\\ \mathrm{sinh}(\eta /2)& \mathrm{cosh}(\eta /2)\end{array}\right)\left(\begin{array}{cc}e^{i\varphi _1/2}& 0\\ 0& e^{i\varphi _1/2}\end{array}\right)`$
$`\times \left(\begin{array}{cc}\mathrm{cosh}(\eta /2)& \mathrm{sinh}(\eta /2)\\ \mathrm{sinh}(\eta /2)& \mathrm{cosh}(\eta /2)\end{array}\right)\left(\begin{array}{cc}e^{i\varphi _2/2}& 0\\ 0& e^{i\varphi _2/2}\end{array}\right).`$ (58)
The above matrices contain complex numbers. However, it is possible to transform simultaneously

$$\left(\begin{array}{cc}\mathrm{cosh}(\eta /2)& \mathrm{sinh}(\eta /2)\\ \mathrm{sinh}(\eta /2)& \mathrm{cosh}(\eta /2)\end{array}\right)$$
(59)
to

$$\left(\begin{array}{cc}\mathrm{exp}(\eta /2)& 0\\ 0& \mathrm{exp}(\eta /2)\end{array}\right),$$
(60)
and transform

$$\left(\begin{array}{cc}e^{i\varphi _i/2}& 0\\ 0& e^{i\varphi _i/2}\end{array}\right)$$
(61)
to

$$\left(\begin{array}{cc}\mathrm{cos}(\varphi _i/2)& \mathrm{sin}(\varphi _i/2)\\ \mathrm{sin}(\varphi _i/2)& \mathrm{cos}(\varphi _i/2)\end{array}\right),$$
(62)
using a conjugate transformation. It is also possible to transform these expressions back to their original forms. This transformation property has been discussed in detail in Ref. .

As a consequence, the matrix of Eq.(8) becomes

$`\left(\begin{array}{cc}e^{\eta /2}& 0\\ 0& e^{\eta /2}\end{array}\right)\left(\begin{array}{cc}\mathrm{cos}(\varphi _1/2)& \mathrm{sin}(\varphi _1/2)\\ \mathrm{sin}(\varphi _1/2)& \mathrm{cos}(\varphi _1/2)\end{array}\right)`$
$`\times \left(\begin{array}{cc}e^{\eta /2}& 0\\ 0& e^{\eta /2}\end{array}\right)\left(\begin{array}{cc}\mathrm{cos}(\varphi _2/2)& \mathrm{sin}(\varphi _2/2)\\ \mathrm{sin}(\varphi _2/2)& \mathrm{cos}(\varphi _2/2)\end{array}\right).`$ (63)
In the above expression, the first three matrices are of the same mathematical form as that of core matrix for the one-lens system given in Eq.(35). The fourth matrix is an additional rotation matrix. This makes the mathematics of repetition more complicated, but this has been done .

As a consequence the net result becomes

$$B(\mu )R(N\alpha )B(\mu ),$$
(64)
or

$$B(\mu )X(N\xi )B(\mu ),$$
(65)
where the parameters $`\mu ,\alpha `$ and $`\xi `$ are to be determined from the input parameters $`\eta ,\varphi _1`$ and $`\varphi _2`$. Detailed calculations are given in Ref. .

It is interesting to note that the Lorentz group can serve as a computational device also in multilayer optics.

## 9 Concluding Remarks

We have seen in this report that the Lorentz group provides convenient calculational tools in many branches of ray optics. The reason is that ray optics is largely based on two-by-two matrices. These matrices also constitute the group $`SL(2,c)`$ which serves as the universal covering group of the Lorentz group.

The optical instruments discussed in this report are the fundamental components in optical circuits. In the world of electronics, electric circuits form the fabric of the system. In the future high-technology world, optical components will hold the key to technological advances. Indeed, the Lorentz group is the fundamental language for the new world.

It is by now well known that the Lorentz group is the basic language for quantum optics. Coherent and squeezed states are representations of the Lorentz group. It is challenging to see how the Lorentz nature of the above-mentioned optical components will manifest itself in quantum world.

The Lorentz group was introduced to physics by Einstein and Wigner to understand the space-time symmetries of relativistic particles and the covariant world of electromagnetic fields. It is gratifying to note that the Lorentz group can serve as the language common both to particle physics and optical sciences.

## Appendix

## Appendix A Lorentz Transformations

Let us consider the space-time coordinates $`(t,z,x,y)`$. Then the rotation around the $`z`$ axis is performed by the four-by-four matrix

$$\left(\begin{array}{cccc}1& 0& 0& 0\\ 0& 0& 0& 0\\ 0& 0& \mathrm{cos}\theta & \mathrm{sin}\theta \\ 0& 0& \mathrm{sin}\theta & \mathrm{cos}\theta \end{array}\right).$$
(66)
This transformation is generated by

$$J_3=\left(\begin{array}{cccc}0& 0& 0& 0\\ 0& 0& 0& 0\\ 0& 0& 0& i\\ 0& 0& i& 0\end{array}\right).$$
(67)
Likewise, we can write down the generators of rotations $`J_1`$ and $`J_2`$ around the $`x`$ and $`y`$ axes respectively.

$$J_1=\left(\begin{array}{cccc}0& 0& 0& 0\\ 0& 0& 0& i\\ 0& 0& 0& 0\\ 0& i& 0& 0\end{array}\right),J_2=\left(\begin{array}{cccc}0& 0& 0& 0\\ 0& 0& i& 0\\ 0& i& 0& 0\\ 0& 0& 0& 0\end{array}\right).$$
(68)
These three generators satisfy the closed set of commutations relations

$$[J_i,J_j]=iϵ_{ijk}J_k.$$
(69)
This set of commutation relations is for the three-dimensional rotation group.

The Lorentz boost along the $`z`$ axis takes the form

$$\left(\begin{array}{cccc}\mathrm{cosh}\eta & \mathrm{sinh}\eta & 0& 0\\ \mathrm{sinh}\eta & \mathrm{cosh}\eta & 0& 0\\ 0& 0& 1& 0\\ 0& 0& 0& 1\end{array}\right),$$
(70)
which is generated by

$$K_3=\left(\begin{array}{cccc}0& i& 0& 0\\ i& 0& 0& 0\\ 0& 0& 0& 0\\ 0& 0& 0& 0\end{array}\right).$$
(71)
Likewise, we can write generators of boosts $`K_1`$ and $`K_2`$ along the $`x`$ and $`y`$ axes respectively, and they take the form

$$K_1=\left(\begin{array}{cccc}0& 0& i& 0\\ 0& 0& 0& 0\\ i& 0& 0& 0\\ 0& 0& 0& 0\end{array}\right),K_2=\left(\begin{array}{cccc}0& 0& 0& i\\ 0& 0& 0& 0\\ 0& 0& 0& 0\\ i& 0& 0& 0\end{array}\right).$$
(72)
These boost generators satisfy the commutation relations

$$[J_i,K_j]=iϵ_{ijk}K_k,[K_i,K_j]=iϵ_{ijk}J_k.$$
(73)
Indeed, the three rotation generators and the three boost generators satisfy the closed set of commutation relations given in Eq.(69) and Eq.(73). These three commutation relations form the starting point of the Lorentz group. The generators given in this Appendix are four-by-four matrices, but they are not the only set satisfying the commutation relations. We can construct also six two-by-two matrices satisfying the same set of commutation relations. The group of transformations constructed from these two-by-matrices is often called $`SL(2,c)`$ or the two-dimensional representation of the Lorentz group. Throughout the present paper, we used the two-by-two transformation matrices constructed from the generators of the $`SL(2,c)`$ group.

## Appendix B Spinors and Four-vectors in the Lorentz Group

In Appendix A, we have noted that there are four-by-four and two-by-two representations of the Lorentz group. The four-by-four representation is applicable to covariant four-vectors, while the two-by-two transformation matrices are applicable to two-component spinors which in the present case are Jones vectors. The question then is whether we can construct the four-vector from the spinors. In the language of polarization optics, the question is whether it is possible to construct the coherency matrix  from the Jones vector.

With this point in mind, let us start from the following form of the Pauli spin matrices.

$$\sigma _1=\left(\begin{array}{cc}1& 0\\ 0& 1\end{array}\right),\sigma _2=\left(\begin{array}{cc}0& 1\\ 1& 0\end{array}\right),\sigma _3=\left(\begin{array}{cc}0& i\\ i& 0\end{array}\right).$$
(74)
These matrices are written in a different convention. Here $`\sigma _3`$ is imaginary, while $`\sigma _2`$ is imaginary in the traditional notation. Also in this convention, we can construct three rotation generators

$$J_i=\frac{1}{2}\sigma _i,$$
(75)
which satisfy the closed set of commutation relations

$$[J_i,J_j]=iϵ_{ijk}J_k.$$
(76)
We can also construct three boost generators

$$K_i=\frac{i}{2}\sigma _i,$$
(77)
which satisfy the commutation relations

$$[K_i,K_j]=iϵ_{ijk}J_k.$$
(78)
The $`K_i`$ matrices alone do not form a closed set of commutation relations, and the rotation generators $`J_i`$ are needed to form a closed set:

$$[J_i,K_j]=iϵ_{ijk}K_k.$$
(79)
The six matrices $`J_i`$ and $`K_i`$ form a closed set of commutation relations, and they are like the generators of the Lorentz group applicable to the (3 + 1)-dimensional Minkowski space. The group generated by the above six matrices is called $`SL(2,c)`$ consisting of all two-by-two complex matrices with unit determinant.

In order to construct four-vectors, we need two different spinor representations of the Lorentz group. Let us go to the commutation relations for the generators given in Eqs.(76), (78) and (79). These commutators are not invariant under the sign change of the rotation generators $`J_i`$, but are invariant under the sign change of the squeeze operators $`K_i`$. Thus, to each spinor representation, there is another representation with the squeeze generators with opposite sign. This allows us to construct another representation with the generators:

$$\dot{J}_i=\frac{1}{2}\sigma _i,\dot{K}_i=\frac{i}{2}\sigma _i.$$
(80)
We call this representation the “dotted” representation. If we write the transformation matrix $`L`$ of Eq.(15) in terms of the generators as

$$L=\mathrm{exp}\left\{\frac{i}{2}\underset{i=1}{\overset{3}{}}\left(\theta _i\sigma _i+i\eta _i\sigma _i\right)\right\},$$
(81)
then the transformation matrix in the dotted representation becomes

$$\dot{L}=\mathrm{exp}\left\{\frac{i}{2}\underset{i=1}{\overset{3}{}}\left(\theta _i\sigma _ii\eta _i\sigma _i\right)\right\}.$$
(82)
In both of the above matrices, Hermitian conjugation changes the direction of rotation. However, it does not change the direction of boosts. We can achieve this only by interchanging $`L`$ to $`\dot{L}`$, and we shall call this the “dot” conjugation.

Likewise, there are two different set of spinors. Let us use $`u`$ and $`v`$ for the up and down spinors for “undotted” representation. Then $`\dot{u}`$ and $`\dot{v}`$ are for the dotted representation. The four-vectors are then constructed as

$`u\dot{u}=(xiy),v\dot{v}=(x+iy),`$
$`u\dot{v}=(t+z),v\dot{u}=(tz)`$ (83)
leading to the matrix

$$C=\left(\begin{array}{cc}u\dot{v}& u\dot{u}\\ v\dot{v}& v\dot{u}\end{array}\right)=\left(\begin{array}{c}u\\ v\end{array}\right)\left(\begin{array}{cc}\dot{v}& \dot{u}\end{array}\right),$$
(84)
where $`u`$ and $`\dot{u}`$ are one if the spin is up, and are zero if the spin is down, while $`v`$ and $`\dot{v}`$ are zero and one for the spin-up and spin-down cases. The transformation matrix applicable to the column vector in the above expression is the two-by-two matrix given in Eq.(15). What is then the transformation matrix applicable to the row vector $`(\dot{v},\dot{u})`$ from the right-hand side? It is the transpose of the matrix applicable to the column vector $`(\dot{v},\dot{u})`$. We can obtain this column vector from

$$\left(\begin{array}{c}\dot{v}\\ \dot{u}\end{array}\right),$$
(85)
by applying to it the matrix

$$g=i\sigma _3=\left(\begin{array}{cc}0& 1\\ 1& 0\end{array}\right).$$
(86)
This matrix also has the property

$$g\sigma _ig^1=\left(\sigma _i\right)^T,$$
(87)
where the superscript $`T`$ means the transpose of the matrix. The transformation matrix applicable to the column vector of Eq.(85) is $`\dot{L}`$ of Eq.(82). Thus the matrix applicable to the row vector $`(\dot{v},\dot{u})`$ in Eq.(84) is

$$\left\{g^1\dot{L}g\right\}^T=g^1\dot{L}^Tg.$$
(88)
This is precisely the Hermitian conjugate of $`L`$.

In optics, this two-by-two matrix form appears as the coherency matrix, and it takes the form

$$C=\left(\begin{array}{cc}<E_x^{}E_x>& <E_y^{}E_x>\\ <E_x^{}E_y>& <E_y^{}E_y>\end{array}\right),$$
(89)
where $`<E_i^{}E_j>`$ is the time average of $`E_i^{}E_j`$. This matrix is convenient when we deal with light waves whose two transverse components are only partially coherent. In terms of the complex parameter $`w`$, the coherency matrix is proportional to

$$C=\left(\begin{array}{cc}1& re^{i\delta }\\ re^{i\delta }& r^2\end{array}\right),$$
(90)
if the $`x`$ and $`y`$ components are perfectly coherent with the phase difference of $`\delta `$. If they are totally incoherent, the off-diagonal elements vanish in the above matrix.

Let us now consider its transformation properties. As was noted by Opatrny and Perina , the matrix of Eq.(89) is like

$$C=\left(\begin{array}{cc}t+z& xiy\\ x+iy& tz\end{array}\right),$$
(91)
where the set of variables $`(x,y,z,t)`$ is transformed like a four-vector under Lorentz transformations. Furthermore, it is known that the Lorentz transformation of this four-vector is achieved through the formula

$$C^{}=LCL^{},$$
(92)
where the transformation matrix $`L`$ is that of Eq.(15). The construction of four-vectors from the two-component spinors is not a trivial task . The two-by-two representation of Eq.(91) requires one more step of complication.

## Appendix C Conjugate Transformations

The core matrix of Eq.(31) contains the chain of the matrices

$$W=\left(\begin{array}{cc}e^{i\varphi }& 0\\ 0& e^{i\varphi }\end{array}\right)\left(\begin{array}{cc}\mathrm{cosh}\eta & \mathrm{sinh}\eta \\ \mathrm{sinh}\eta & \mathrm{cosh}\eta \end{array}\right)\left(\begin{array}{cc}e^{i\xi }& 0\\ 0& e^{i\xi }\end{array}\right).$$
(93)
The Lorentz group allows us to simplify this expression under certain conditions.

For this purpose, we transform the above expression into a more convenient form, by taking the conjugate of each of the matrices with

$$C_1=\frac{1}{\sqrt{2}}\left(\begin{array}{cc}1& i\\ i& 1\end{array}\right).$$
(94)
Then $`C_1WC_1^1`$ leads to

$$\left(\begin{array}{cc}\mathrm{cos}\varphi & \mathrm{sin}\varphi \\ \mathrm{sin}\varphi & \mathrm{cos}\varphi \end{array}\right)\left(\begin{array}{cc}\mathrm{cosh}\eta & \mathrm{sinh}\eta \\ \mathrm{sinh}\eta & \mathrm{cosh}\eta \end{array}\right)\left(\begin{array}{cc}\mathrm{cos}\xi & \mathrm{sin}\xi \\ \mathrm{sin}\xi & \mathrm{cos}\xi \end{array}\right).$$
(95)
In this way, we have converted $`W`$ of Eq.(93) into a real matrix, but it is not simple enough.

Let us take another conjugate with

$$C_2=\frac{1}{\sqrt{2}}\left(\begin{array}{cc}1& 1\\ 1& 1\end{array}\right).$$
(96)
Then the conjugate $`C_2C_1WC_1^1C_2^1`$ becomes

$$\left(\begin{array}{cc}\mathrm{cos}\varphi & \mathrm{sin}\varphi \\ \mathrm{sin}\varphi & \mathrm{cos}\varphi \end{array}\right)\left(\begin{array}{cc}e^\eta & 0\\ 0& e^\eta \end{array}\right)\left(\begin{array}{cc}\mathrm{cos}\xi & \mathrm{sin}\xi \\ \mathrm{sin}\xi & \mathrm{cos}\xi \end{array}\right).$$
(97)
The combined effect of $`C_2C_1`$ is

$$C=C_2C_1=\frac{1}{\sqrt{2}}\left(\begin{array}{cc}e^{i\pi /4}& e^{i\pi /4}\\ e^{i\pi /4}& e^{i\pi /4}\end{array}\right),$$
(98)
with

$$C^1=\frac{1}{\sqrt{2}}\left(\begin{array}{cc}e^{i\pi /4}& e^{i\pi /4}\\ e^{i\pi /4}& e^{i\pi /4}\end{array}\right).$$
(99)
After multiplication, the matrix of Eq.(97) will take the form

$$V=\left(\begin{array}{cc}A& B\\ C& D\end{array}\right),$$
(100)
where $`A,B,C,`$ and $`D`$ are real numbers. If $`B`$ and $`C`$ vanish, this matrix will become diagonal, and the problem will become too simple. If, on the other hand, only one of these two elements become zero, we will achieve a substantial mathematical simplification and will be encouraged to look for physical circumstances which will lead to this simplification.

Let us summarize. we started in this section with the matrix representation $`W`$ given in Eq.(93). This form can be transformed into the $`V`$ matrix of Eq.(97) through the conjugate transformation

$$V=CWC^1,$$
(101)
where $`C`$ is given in Eq.(98). Conversely, we can recover the $`W`$ representation by

$$W=C^1VC.$$
(102)
For calculational purposes, the $`V`$ representation is much easier because we are dealing with real numbers. On the other hand, the $`W`$ representation is of the form for the S-matrix we intend to compute. It is gratifying to see that they are equivalent.

Let us go back to Eq.(97) and consider the case where the angles $`\varphi `$ and $`\xi `$ satisfy the following constraints.

$$\varphi +\xi =2\theta ,\varphi \xi =\pi /2,$$
(103)
thus

$$\varphi =\theta +\pi /4,\xi =\theta \pi /4.$$
(104)
Then in terms of $`\theta `$, we can reduce the matrix of Eq.(97) to the form

$$\left(\begin{array}{cc}(\mathrm{cosh}\eta )\mathrm{cos}(2\theta )& \mathrm{sinh}\eta (\mathrm{cosh}\eta )\mathrm{sin}(2\theta )\\ \mathrm{sinh}\eta +(\mathrm{cosh}\eta )\mathrm{sin}(2\theta )& (\mathrm{cosh}\eta )\mathrm{cos}(2\theta )\end{array}\right).$$
(105)
Thus the matrix takes a surprisingly simple form if the parameters $`\theta `$ and $`\eta `$ satisfy the constraint

$$\mathrm{sinh}\eta =(\mathrm{cosh}\eta )\mathrm{sin}(2\theta ).$$
(106)
Then the matrix becomes

$$\left(\begin{array}{cc}1& 0\\ 2\mathrm{sinh}\eta & 1\end{array}\right).$$
(107)
This aspect of the Lorentz group is known as the Iwasawa decomposition , and has been discussed in the optics literature .

The matrices of the form is not so strange in optics. In para-axial lens optics, the translation and lens matrices are written as

$$\left(\begin{array}{cc}1& u\\ 0& 1\end{array}\right),and\left(\begin{array}{cc}1& 0\\ u& 1\end{array}\right),$$
(108)
respectively. These matrices have the following interesting mathematical property ,

$$\left(\begin{array}{cc}1& u_1\\ 0& 1\end{array}\right)\left(\begin{array}{cc}1& u_2\\ 0& 1\end{array}\right)=\left(\begin{array}{cc}1& u_1+u_2\\ 0& 1\end{array}\right),$$
(109)
and

$$\left(\begin{array}{cc}1& 0\\ u_1& 1\end{array}\right)\left(\begin{array}{cc}1& 0\\ u_1& 1\end{array}\right)=\left(\begin{array}{cc}1& 0\\ u_1+u_2& 1\end{array}\right).$$
(110)
We note that the multiplication is commutative, and the parameter becomes additive. These matrices convert multiplication into addition, as logarithmic functions do.

## Appendix D Euler versus Lie Representations

In this paper, we restricted ourselves to the algebra of two-by-two matrices and avoided as much as possible group theoretical languages. In order to explain where those algebraic tricks came from, we give in this Appendix A group theoretical interpretation of what we did in this paper.

The group $`SL(2,c)`$ consists of two-by-two unimodular matrices whose elements are complex. There are therefore six independent parameters, and thus six generators of the Lie algebra. This group is locally isomorphic to the six-parameter Lorentz group or $`O(3,1)`$ applicable to the Minkowskian space of three space-like directions and one time-like direction.

Like the Lorentz group, the $`SL(2,c)`$ has a number of interesting subgroups. The subgroup most familiar to us is $`SU(2)`$ which is locally isomorphic to the three-dimensional rotation group. In addition, this group contains three subgroups which are locally isomorphic to the group $`O(2,1)`$ applicable to the Minkowskian space of two space-like and one time-like dimensions.

One of the subgroups of $`SL(2,c)`$ is $`SL(2,r)`$ consisting of matrices with real elements. This subgroup is also called the $`Sp(2)`$ group which we used in this paper in order to carry out the Iwasawa decomposition. Another interesting subgroup is the one we used for computing the $`S`$ matrix, which starts with the boundary matrix of Eq.(54) and the phase-shift matrix of Eq.(55). This group is called $`SU(1,1)`$. The present paper exploits the isomorphism between $`Sp(2)`$ and $`SU(1,1)`$. While the physical world is describable in terms of $`SU(1,1)`$, we carry out the Iwasawa decomposition in the $`Sp(2)`$ regime.

Indeed, the conjugate transformation of Eq.(93) to Eq.(95) is from $`SU(1,1)`$ to $`Sp(2)`$, while the transition from Eq.(95) to Eq.(97) is within the $`Sp(2)`$ group. Thus, the transition from Eq.(93) to Eq.(97) is a conjugate transformation from the $`SU(1,1)`$ subgroup to the subgroup $`Sp(2)`$ of $`SL(2,r)`$.

In this paper, we are concerned with the decomposition of the $`Sp(2)`$ and $`SU(1,1)`$ matrices. Unlike the traditional approach to group theory which starts from the generators of the Lie algebra, we used in this paper an approach similar to what Goldstein did for the three-dimensional rotation group in terms of the Euler angles . There are three-generators for the rotation group, but Goldstein starts with rotations around the $`z`$ and $`x`$ directions. Rotations around the $`y`$ axis and the most general form for the rotation matrix can be constructed from repeated applications of those two starting matrices. Let us call this type of approach the “Euler construction.”

There are three basic advantages of this approach. First, the number of “starter” matrices is less than the number of generators. For example, we need only two starters for the three-parameter rotation group. In our case, we started with two matrices for the three-parameter group $`Sp(2)`$ and also for $`SU(1,1)`$. Second, each starter matrix takes a simple form and has its own physical interpretation.

The third advantage can be stated in the following way. Repeated applications of the starter matrices will lead to a very complicated expression. However, the complicated expression can decomposed into the minimum number of starter matrices. For example, this number is three for the three-dimensional rotation group. This number is also three for $`SU(2)`$ and $`Sp(2)`$. We call this the Euler decomposition. The present paper is based on both the Euler construction and the Euler decomposition.

Among the several useful Euler decompositions, the Iwasawa decomposition plays an important role in the Lorentz group. We have seen in this paper what the decomposition does to the two-by-two matrices of $`Sp(2)`$, but it has been an interesting subject since Iwasawa’s first publication on this subject . It is beyond the scope of this paper to present a historical review of the subject. However, we would like to point out that there are areas of physics where this important mathematical theorem was totally overlooked.

For instance, in particle theory, Wigner’s little groups dictate the internal space-time symmetries of massive and massless particles which are locally isomorphic to $`O(3)`$ and $`E(2)`$ respectively . The little group is the maximal subgroup of the Lorentz group whose transformations do not change the four-momentum of a given particle . The $`E(2)`$-like subgroup for massless particles is locally isomorphic to the subgroup of $`SL(2,c)`$ which can be started from one of the matrices in Eq.(108) and the diagonal matrix of Eq.(55). Thus there was an underlying Iwasawa decomposition while the the $`E(2)`$-like subgroup was decomposed into rotation and boost matrices , but the authors did not know this. One of those authors is one of the authors of the present paper.

In optics, there are two-by-two matrices with one vanishing off-diagonal element. It was generally known that this has something to do with the Iwasawa effect, but Simon and Mukunda  and Han et al.  started treating the Iwasawa decomposition as the main issue in their papers on polarized light.

In para-axial lens optics, the matrices of the form given in Eq.(108) are the starters , and repeated applications of those two starters will lead to the most general form of $`Sp(2)`$ matrices. It had been a challenging problem since 1985  to write the most general two-by-two matrix in lens optics in terms the minimum number of those starter matrices. This problem has been solved recently , and the central issue in the problem was the Iwasawa decomposition.


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# Close-Packing of Clusters: Application to Al100

## I Introduction

Formation of atomic clusters can lead to close-packed (CP) structures under some conditions. The shape of such clusters is determined by the balance of surface area, surface energy, and internal strain. In small metal clusters also the self-deformation of the valence electron density can play an important role. Other common packing patterns in clusters include often icosahedral and decahedral motifs with internal twin boundaries.martin96  Metals such as Na, Mg and Cu show icosahedral magic numbers.martin96 ; reinhard97  The motivation to study FCC and other close-packed clusters is the fact that some elements, for example Al, are found to form FCC clusters of octahedral shape.martin92  Moreover, at certain cluster sizes pair potentials (e.g. Lennard-Jones) also yield FCC-based structures as the most stable isomers.

Generally, the search for the lowest energy isomer of a cluster is a difficult problem due to the vast number of isomers which correspond to local minima on a complex potential energy surface. The energy differences between the isomers are caused by the surface energy,Wul01  strain energy due to structural defects such as twin boundaries,Ino69  and in metals also the electronic shell structure.hakkinen97  For example, if one uses classical or ab initio molecular dynamics (MD) one usually needs an appropriate initial configuration in order to save computation time. hakkinen95 ; rytkonen00 ; kumar91 ; delaly92 ; akola99  One purpose of this work is to apply the Monte Carlo method to look for the most stable isomers of hard sphere clusters, to be used as starting geometries for MD simulations.

Classical molecular dynamics have been extensively used to study the lowest energy structures of small clusters. However, finding the correct ground state geometry of a small cluster ($`N100`$) is a difficult optimization task even with classical pair potentials.Wil85  For historical reasons, the Lennard-Jones potential is the best studied,Hoa83 ; doye98 ; doye99 ; leary99  but other pair potentialsdoye01b ; doye00 ; doye01  as well as many-atom potentialsbaletto00 ; baletto02 ; valkealahti92 ; cleveland97  have been used. Nearly all give an icosahedral geometry for the 13 and 55 atom clusters. The behavior of the binding energy as a function of cluster size is, however, quite different for different potentials. While $`N=13`$ is seen as an exceptionally stable size, the second complete icosahedron ($`N=55`$) is not a clear local minimum for most of the potentials studied. For example, the 38 atom FCC structure (Wulff’s polyhedron) depends less on the model potential than does the 55 icosahedron.

In this article, we present results for the lowest energy isomers of close-packed clusters in the size range $`N110`$. Our model, which uses the hard sphere packing as a starting point, does not include icosahedral and decahedral motifs as well as any other structures with varying bond lengths and angles. This makes our approach extremely efficient in finding lowest energy structures of CP clusters. The cluster energy is determined using either a pairwise nearest neighbor interaction or a many-atom potential based on the tight-binding model. For many sizes, the lowest energy structure found includes stacking faults, making the cluster a mixture of FCC and HCP phases.

For a cluster with 100 aluminum atoms we use a density functional (DF) method to relax the atomic positions of the low energy isomers obtained with the simple model. Our goal is to study the applicability of our classical energy expression in a realistic cluster, where the true electronic structure is present. The cluster size $`N=100`$ is particularly interesting because the experimental photoelectron spectrum of the anion has a large energy gap between the highest and lower-lying occupied orbitals.Wang98  Our calculations show that many of the low energy isomers have such an energy gap, but the absolute value of the theoretical gap is still smaller than the experimental result.

The plan of this article is the following. In Section 2, the theoretical hard sphere model and the DF method used are outlined. The results for the lowest energy structures of the close-packed clusters and their relations to the cluster shapes are presented in Section 3, and the DF calculations for Al100 and the corresponding photoelectron spectra are presented in Section 4. The conclusions are given in Section 5.

## II Simulation methods

### II.1 Monte Carlo method for hard sphere clusters

The lowest energy geometries of hard sphere clusters are computed using the Monte Carlo (MC) method with a Metropolis algorithm. This is described in our earlier work where the role of stacking faults in small hard sphere clusters was studied.kmanninen02  Similar algorithm was earlier used by Akola et al. for making pure FCC clusters.akola00  A dense lattice is generated inside a spherical volume in such a way that atoms occupying these lattice sites can form an FCC or HCP lattice or any combination of these two, including stacking faults in all possible directions. The lattice sites are then randomly populated with $`N`$ atoms, such that the minimum distance between any atom pair is twice the hard sphere radius, i.e., the nearest neighbor distance in the FCC lattice. After this, a Monte Carlo procedure is used together with the cluster binding energy to change the lattice site occupations leading to a “clustering” of atoms. The simulation is started at a high temperature that is gradually decreased to zero to obtain the low energy isomers. This optimization procedure, including millions of steps, is repeated typically at least 1000 times for each cluster size. During the optimization, we record not only the most stable geometry but also many other low energy isomers.

Two simple models, a pair-potential (PP) and a tight-binding based potential (TB), are used as a contact interaction between the hard spheres. In the former the energy is calculated as

$$E_{\mathrm{PP}}=\frac{V}{2}\underset{i}{\overset{N}{}}C_i=VN_{\mathrm{bonds}}$$
(1)
where $`C_i`$ is the coordination number of the atom $`i`$ and $`V`$ is the strength of the interaction ($`V`$ determines the energy scale) and $`N_{\mathrm{bonds}}`$ is the total number of bonds (contacts between the hard spheres). The second model is derived from tight-binding theory,gupta81 ; finnis84  and it has a simple square root dependence on the coordination number

$$E_{\mathrm{TB}}=\frac{V}{2}\underset{i}{\overset{N}{}}\sqrt{C_i}.$$
(2)
In practice, Eq.(2) has shown to be a good approximation for the true TB energy of small clusters.hakkinen91  Nevertheless, this model cannot describe effects related to the details of the electronic structure, such as Jahn-Teller deformation, and the geometries obtained from Eq.(2) should not be confused with the most stable geometries determined with the true tight-binding method.wang87 ; yoshida94

The Monte Carlo simulations are performed using the PP model energy expression Eq.(1), which leads in many cases to several different geometries with the same energy. The TB interaction is more practicable here, since it is more sensitive in separating the energy of different isomers. In most cases, it removes the degeneracy of lowest energy isomers of the PP model. The TB model favors geometries where each atom has a similar coordination, whereas the PP model is insensitive to the bond distribution.

### II.2 Electronic structure calculations

The DF calculations of Al100 isomers are performed using the Car-Parrinello molecular dynamics (CPMD) code,CPMD  where the electron-ion interaction is described by an ionic pseudopotential, TM91  and the generalized gradient correction approximation of Perdew, Burke, and Ernzerhof (PBE) is applied to the exchange correlation energy of the electron density.PBE96  The basis set is taken to be plane waves with a cut-off energy of 15.4 Ry. In contrast to many Car-Parrinello simulations, we do not enforce periodicity in the system, i.e., calculations are performed in an isolated cubic box of 25.4 Å. We also do not employ the Car-Parrinello algorithm for the coupling of ionic and electronic solutions during geometry optimization, and the electronic Hamiltonian is rediagonalized after each geometry optimization step. The metal clusters studied show systematically small energy gaps between the occupied and unoccupied molecular orbitals (HOMO-LUMO gaps). In order to converge the electron density, a finite temperature functional ($`T=300`$ K) is used for the the Kohn-Sham (KS) orbital occupancies. The ionic positions are optimized according to a conjugate gradient method until all the nuclear gradient components are below $`1\times 10^4`$ au.

## III Results

### III.1 Lowest energy geometries of the hard sphere clusters

Tables 1, 2, 3, and 4 give the energies of the lowest energy isomers found with the PP and TB potentials. For each size, we show the energy of the most stable FCC isomer together with the lowest energy isomer with one or more stacking faults (SF). In addition, the occupation numbers of parallel (111) layers in the FCC isomer are also shown (this is not done for the SF clusters, since these cannot generally be described by parallel (111) layers). Examples of the isomers obtained are shown in Figures 1, 2, and 3. The results for the most stable isomers of small clusters $`N=458`$ agree with those published earlier, kmanninen02  except for some TB energies. The lowest energy structures obtained using the PP model are similar to the results by Doye and Wales doye95  except for $`N=33`$, 49, 50, 51, 68, 69, 82, 107, and 108, where we have found a more stable geometry (for 33, 49, 51, 69, 82, 107 our results have one additional bond, for 50, 68, 108 two bonds more than those of Doye and Wales).

The total number of bonds in the most stable geometry is the same in both the PP and TB models for all $`N`$. The difference between the two energy formulas appears only in separation between different isomers with the same number of bonds. For each cluster size we have determined the lowest energy FCC geometry, but the most stable geometry with at least one stacking fault is determined only for those clusters where a stacking fault does not decrease the number of bonds (as in the sizes 4, 38, 39, 40, 86, 88, 102, 104). For the other sizes (see Tables I-IV), the TB model gives lower energies for SF structures in many cases. A detailed discussion of the structure evolution of small hard sphere clusters has been given earlier,kmanninen02  and we concentrate on clusters with more than 60 atoms in the following.

Clusters with $`N=58`$, 59, and 60 are based on a truncated 31-atom tetrahedron with all four overlayers in stacking fault locations. We denote such isomers with tetrahedral symmetry as SFS (see also $`N=100`$). Both the PP and TB models give a large energy difference between the most stable FCC geometry and the SFS lowest energy isomer. For $`62N64`$, the clusters consist mainly of four (111) layers, three of them being in an FCC arrangement and the fourth being either FCC or HCP. For each size, the most stable FCC and SF structures have the same number of atoms in the layers. The lowest energy SF structure of $`N=67`$ resembles closely an HCP cluster. It consists of five layers, four of them forming an HCP-lattice and the fifth in a stacking fault position (layer-packing ABABC, which can be seen as two connected FCC subunits). SF clusters with $`N=68`$, 69, and 73 have similar structures, whereas the cluster sizes 70, 72 and 74 atoms show four parallel FCC layers, and the fifth layer is displaced in a stacking fault position. The lowest energy structure of 71 atoms consists of two FCC subdomains (layer-packing ABCBA).

In the size range 75–80, the lowest energy isomers are FCC structures according to the TB potential with a very small energy difference to SF structures. This applies also for $`N=79`$, where the FCC construction gives a complete truncated octahedron (TO). The corresponding SF isomer (two FCC units connected) also has large (111) facets, which explains the low energy. Similar kinds of SF clusters with a stacking fault layer inside the cluster are found in $`N=8192`$, and 94, while $`N=81`$, 83, and 92 are better than FCC for both potentials. The clusters with 86 and 88 atoms have a nondegenerate FCC energy minimum in the PP model. These isomers are based on the FCC-79 with one (111) overlayer. For $`N=87`$, the FCC structure is still lower in TB energy, but there are SF structures with the same number of bonds (PP energy). The lowest energy isomers of $`N=93`$ and 95 consist of four FCC layers, with the fifth being in HCP position (with respect to the two lower layers). The clusters with $`N=9698`$ atoms do not have stacking faults according to the TB model.

The most stable isomers for 99 or 100 atoms have an SFS structure based on a truncated FCC tetrahedron with stacking faults at each of the four surfaces. The 100 atom cluster has the same structural motif as SFS-59, whereas in the case of 99 (101) atoms, one surface atom is removed (added). The lowest-lying TB geometries for $`101N104`$, $`N=106`$, 109, and 110 are FCC structures with five (111) layers. They all are related to FCC-102, which is an elongated TO having a full atom shell (similar to FCC-52). Clusters with $`N=105`$, 107 and 108 prefer stacking faults in the TB model, and SF-105 has the largest number of bonds in its class.

### III.2 Magic numbers

The most stable cluster sizes (magic numbers) reflect the stability of the cluster with respect to the neighboring sizes. In order to see also the possible regions of increased stability, it is convenient to subtract a smooth size dependence from the energy. This can be obtained by fitting the total energies to a “mass formula” $`E_{\mathrm{ave}}=E_{\mathrm{coh}}N+bN^{2/3}+cN^{1/3}`$, where $`b`$ and $`c`$ are fitting parameters and $`E_{\mathrm{coh}}`$ is the cohesion energy of the model in question ($`E_{\mathrm{coh}}=6V`$ for the PP model and $`V\sqrt{3}`$ for the TB model).Wei35 ; Per91  Figure 4 shows the deviation of energy from this function. Clusters with $`N=12`$, 26, 38, 50, 59, 61, 68, 75, 79, 86, 100, and 102 are the most pronounced local minima, but there are several weaker local minima, and the results show odd-even alternation in some regions. However, since this behavior is not of electronic origin,manninen94  the minima can be for $`N`$ even (around 38) or odd (around 61).

The general profile of the energy curve is related to the total number of bonds. This is natural in our model which totally neglects the internal strain. In all cases, the lowest PP and TB structures have the same number of bonds and qualitatively similar energy curves. Note that from the magic sizes only those with 38, 75, 79, 86, and 102 atoms are pure FCC clusters, while others have stacking faults. Doye and Wales have used a pair-wise Morse potential in the size range $`20N80`$ to study the effect of potential range on the magic numbers.doye97  For the hardest potential studied, they found magic numbers 26, 38, 50, 55, 59, 61, 68, and 79, which are present in our results except the size 55, which is an icosahedron. These results seem to indicate that the internal strain is not important in clusters which do not have twin boundaries.

### III.3 Moments of inertia

The overall shape of clusters is studied by calculating the three moments of inertia for the principal axis, and the normalized average moment of inertia

$$I=\frac{1}{N^{5/3}}\underset{i}{\overset{N}{}}(𝐑_i𝐑_{\mathrm{cm}})^2,$$
(3)
where $`𝐑_i`$ is the atom position and $`𝐑_{\mathrm{cm}}`$ the center of mass (in units of the FCC lattice constant). The factor $`1/N^{5/3}`$ is chosen because the moment of inertia is proportional to $`N^{5/3}`$ for a spherical cluster. The normalized moments of inertia are shown in Figure 5(a), and the similarity between Figures 4 and 5(a) is obvious. The minima in moments of inertia are present also in the energy curve except for $`N=15`$, 19, and 107.

It is also interesting to resolve the cluster deformation on the basis of moments of inertia, since for a sphere (or a cube, etc.) all the principal components of inertia are equal. Figure 5(b) shows the difference of the maximum and minimum components as a function of cluster size. Many of the magic clusters ($`N=38`$, 59, 68, 79, 100) have high symmetry, but some, e.g. 50, 86, and 102 have a marked deformation. The large (111) facets compensate the increase in surface area (deformation) in such cases.

### III.4 Electronic structure calculations of Al100 isomers

In order to test the applicability of our classical energy expressions for Al clusters we have chosen an MC-generated test set of 15 low energy isomers for $`N=100`$ together with the corresponding icosahedral and decahedral isomers, which we optimized using the DF method. The results for total energies, bond lengths, deformation, and HOMO-LUMO gaps ($`E_g`$) of KS orbitals are presented in Table 5. The corresponding cluster geometries are shown in Figure 6. The FCC isomers are all based on the same structural motif, which leads to a full atomic shell of an elongated TO at cluster size 102 (notice the two missing atoms in Figure 6). The higher degree of freedom in the case of clusters with stacking faults results in a variety of different structures. Among the 11 different geometries chosen from this class, five of them (SF2, SF3, SF6, SF7, and SF8) have the same structure of two connected FCC subdomains with two external atoms changing their positions on the surface, and we show the most stable geometry SF2. As representatives of CP clusters, the SFS isomers T1 and T2 have stacking faults in all four  directions. The perfect symmetry of T1 is broken in T2 (not shown) via a surface atom displacement. The icosahedral and decahedral isomer structures are obtained from the Cambridge Cluster Database,walesco  where ICO corresponds to the most stable icosahedral configuration found with a model potential, and DECA is based on the Mark’s decahedron for 101 atoms (one atom is removed).

The isomers in Table 5 are ordered according to the DF total energy. The FCC isomers have lowest energy, followed by other CP structures, and the DECA and ICO isomers are significantly higher due to the internal strain within these geometries. This is in agreement with a previous study of Al clusters, akola00  which showed that Al tends to form FCC geometries at a relatively early stage ($`N55`$). In contrast to the classical potentials, DF calculations give a higher total energy for T1 than for the other CP clusters (except for T2). The highly symmetric geometry of T1 results in degeneracies of electronic levels (see Figure 7), and one of them occurs at the Fermi energy, leading to an energetically unstable situation. The cluster undergoes a small Jahn-Teller deformation, which can be seen as a finite HOMO-LUMO gap in Table 5, but there are no changes in the overall shape. We presume that a deformation of the T1 shape should lower the total energy, especially when the other structures show marked deformations (see Table 5). This is related to the self-deformation of valence electron density in the jellium model,Bra93  a phenomenon that lowers total energy. Taking this effect into account, we have modified our expression for the classical energy:

$$E_{\mathrm{TB}}^{\mathrm{DEF}}=E_{\mathrm{TB}}+\frac{1}{2}K(DD_0)^2,$$
(4)
where $`K`$ is a coupling constant and $`D_0`$ corresponds to the minimum energy deformation, defined as $`D=(I_{\mathrm{max}}I_{\mathrm{min}})/I_{\mathrm{ave}}`$ where $`I`$’s are the moments of inertia in the principal axis presentation. The value of $`K`$ is calibrated using the DF results for FCC1 and T1 (difference in binding energy), assuming that FCC1 represents an ideal deformation. The results for the new classical energy in Table 5 now correlate better with DF calculations, but SF2 and structures related to it remain close to the lowest energy isomer, indicating that other contributions (such as surface and strain energy) must also be considered.

Density functional calculations show that the CP isomers lie within a very narrow energy range of 1.13 eV (Table 5), corresponding to 90 K when converted to vibrational energy.tvib  Moreover, the energy difference between the most stable (FCC1) and next higher (SF1) isomers is negligible, which emphasizes that one cannot claim that FCC clusters are more stable than SF structures. The nearest neighbor distances reveal, however, some minor deviations: in FCC clusters the average bond length is slightly smaller, and the related distribution width is narrow. The FCC isomers are evidently relatively strain-free, which partially explains the energetic trend in the CP data set (see also ICO and DECA). As discussed above, the electronic structure contributes to the total energy, as shown by the HOMO-LUMO gap, which is maximized via a self-deformation process whenever possible. It is shown in Table 5 that the HOMO-LUMO gaps of Al100 clusters are in the range of 0.02-0.21 eV, and that the most stable structures FCC1 and SF1 also have significant values. Nevertheless, there is no clear trend among the clusters studied.

The electronic density of states (DOS) of FCC1 and T1 clusters is shown in Figure 7. The DOS of T1 is highly peaked due to the electron level degeneracies whereas FCC1 shows a gradually increasing DOS with less fine structure. The latter applies basically to all the other CP isomers that have no symmetry in the cluster geometry. In order to compare our results with the spherical jellium model (SJM), we have labeled the main peaks present in the T1 spectrum according to the related number of valence electrons (KS orbitals). Apart from $`N_{el}=56`$, the system corresponds fully with the magic numbers of SJM up to 198 valence electrons, after which the exact details in the cluster shape and structure start to contribute. The T1 cluster actually has a $`T_d`$ symmetry, but a corner truncation has brought it apart from a perfect tetrahedron, and no magic numbers related to the tetrahedral external potential can be observed.Rei97  The last electron shell in the T1 spectrum is only partially filled, and there is no shell closing at $`N_{el}=300`$ (Fermi energy).

The experimental photoelectron spectrum (PES) of AlN ($`N=100112`$) cluster anions Wang98  shows a marked gap at the threshold region. Based on our earlier experience with Al clusters,akola99 ; akola00  we have compared the DOS of close-packed Al$`{}_{}{}^{}{}_{100}{}^{}`$ isomers (not shown) with the experimental PES. As indicated by the sizable HOMO-LUMO gaps of neutral clusters, qualitatively correct features can be observed in the DOS of lowest energy isomers (FCC1 and SF1). However, the separation of the first peak in the theoretical DOS is far too small (0.2 eV), and the corresponding electron detachment energy is 3.2 eV, whereas it is 3.4 eV in the experiments. This suggests that the experimental spectrum is dominated by an electronically stable isomer that is not considered in the present study. Presumably, the long thermal tail in the experimental PES (starting from 3.1 eV) is caused by the presence of other isomers – such as FCC1 and SF1.

## IV Conclusion

Close-packed geometries are important structures present in a small cluster size regime, and we have studied the structures of hard sphere clusters up to $`N=110`$ atoms using two types of classical potentials. The total energy is minimized using the Monte Carlo method. For most sizes, the discrete PP model leads to several isomers with the same total energy (number of bonds). Only for $`N=4`$, 38–40, 86, 88, 102, and 104 does the FCC geometry have more bonds than any of the geometries with stacking faults. On the other hand, for $`N=5`$, 11, 12, 26–28, 33, 35, 49–51, 58–60, 81, 83, 92, 99–100, 105 the most stable PP isomer does not have an FCC structure. Clusters with $`N=5860`$ and $`N=99100`$ atoms have a tetrahedral symmetry and stacking faults on all surface facets. An inclusion of the TB model yields qualitatively same results, the only effect being in the separation of the isomers having the maximal coordination.

The energy as a function of the cluster size shows that clusters with $`N=12`$, 26, 38, 50, 59, 61, 68, 75, 79, 86, 100, and 102 have the most pronounced energy minima. Of these only the 38, 75, 79, 86, and 102 atom clusters have an FCC structure. The moments of inertia correlate well with the energy curve, showing that most of the magic clusters have also a compact geometry, i.e., the overall shape of clusters is not deformed. There exist, however, structures such as FCC-102 where the deformation is compensated by the large (111) facets. Such a behavior becomes increasingly important as the cluster size increases, leading to an epitaxial growth pattern.Val95

The connection between the model potential and DF calculations has been studied in the case of Al100. The DF calculations show that the strain-free CP structures are lower in total energy than the corresponding icosahedral and decahedral isomers. In CP regime the total energy differences are very small (supposing that the coordination number of the cluster is close to the maximum), and the electronic structure becomes important. As illustrated by the isomer T1, the valence electron density of Al100 clusters prefers deformation, and this criterion is fulfilled by almost all the CP isomers presented. None of the structures reported reproduces the experimental PES.Wang98  The exceptional shape of the experimental curve and the high electron detachment energy indicate that the underlying isomer must be electronically very stable. We speculate that perhaps an elongated (or otherwise deformed) T1 isomer, where the degeneracy at the Fermi energy is removed, can reproduce this feature. A simple geometry optimization is not enough to investigate this possibility, and ab initio MD simulations will be necessary.

CP clusters with stacking faults are potential candidates for the most stable isomer in some occasions, and we have demonstrated this for Al100, where the energetic difference between the FCC and SF clusters is negligible. Therefore, these structural motifs are competitive even at relatively large cluster sizes ($`N100`$). Experiments indicate that the octahedral FCC isomers start to dominate the Al mass-spectrum at $`N200`$ due to formation of large (111) facets that minimize the surface energy. martin92 ; martin96

## V Acknowledgments

This work has been supported by the Academy of Finland under the Finnish Centre of Excellence Programme 2000-2005 (Project No. 44875, Nuclear and Condensed Matter Programme at JYFL). J.A. has been supported by the Bundesministerium für Bildung und Forschung (BMBF), Bonn, within the Kompetenzzentrum Materialsimulation, 03N6015. We thank L.-S. Wang for providing us the experimental PES of Al$`{}_{}{}^{}{}_{100}{}^{}`$, and R.O. Jones for a critical reading of the manuscript.