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Canadian Journal of Physics

Tutorial/Article didactique: Angular momenta dynamics in magnetic and electric field: Classical and quantum approach

Marcis P. Auzinsh

Published Dec 12, 1997• 13 citations
Publisher

Abstract

A standard description of the angular momentum in atomic or molecular physics is based on quantum mechanics. However, especially at large angular-momentum limit in molecules, sometimes a classical approach greatly simplifies problems that are extremely complicated from a quantum-mechanical viewpoint. The aim of this paper is to examine the relationship between the classical and quantum descriptions of the angular-momentum distribution in an ensemble of particles. At first glance, quantum and classical approaches appear to be absolutely different and have very little in common. In this paper this relationship is analyzed. It is shown that similarities can be found between the precession of angular momentum in the external field and the influence of this field upon the wave-function phase of a microparticle. The importance of wave function phases is stressed even for stationary conditions, and some examples of coherent superposition of quantum states are presented. The general method of how to pass from the quantum approach to a classical one is formulated. Results are visualized in the form of 3D distribution functions. This approach allows a graphical interpretation and thus results in a better understanding, sometimes at first glance, of counterintuitive quantum results. As an example the phenomenon of alignment- orientation transition is considered. Rather than presenting only formal derivations, the emphasis is on the instructional aspects, and on illustrating the general approach.

DOI
10.1139/p97-034

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A standard description of the angular momentum in atomic or molecular physics is based on quantum mechanics. However, especially at large angular-momentum limit in molecules, sometimes a classical approach greatly simplifies problems that are extremely complicated from a quantum-mechanical viewpoint. The aim of this paper is to examine the relationship between the classical and quantum descriptions of the angular-momentum distribution in an ensemble of particles. At first glance, quantum and classical approaches appear to be absolutely different and have very little in common. In this paper this relationship is analyzed. It is shown that similarities can be found between the precession of angular momentum in the external field and the influence of this field upon the wave-function phase of a microparticle. The importance of wave function phases is stressed even for stationary conditions, and some examples of coherent superposition of quantum states are presented. The general method of how to pass from the quantum approach to a classical one is formulated. Results are visualized in the form of 3D distribution functions. This approach allows a graphical interpretation and thus results in a better understanding, sometimes at first glance, of counterintuitive quantum results. As an example the phenomenon of alignment- orientation transition is considered. Rather than presenting only formal derivations, the emphasis is on the instructional aspects, and on illustrating the general approach.
Anisotropy of angular momenta: ideas and methods The fundamental idea forming the basis of early quantum theory was the quantization of the angular momentum of the atom, which, at a later stage, assumed the form of the Bohr–Sommerfeld quantization rule [360], namely ∲ pdq = n ℏ where p and q are the generalized momentum and coordinate. This concept has retained its physical meaning in modern-day quantum mechanics [371, 372]. In the course of the further development of quantum mechanical concepts it became increasingly clear that in the theory of atoms and molecules the angular momentum is a ‘dominant’ notion, the fundamental significance of which is in no small degree connected with its dimension of action, which coincides with that of Planck's constant ℏ. In the interaction between particles and a directed beam of photons the angular momentum of the system is conserved, thus forming the basis for the optical method of producing spatial anisotropy of the distribution of the angular momenta of the ensemble of particles, i.e. its optical polarization . In terms of quantum concepts, spatial anisotropy means that in an ensemble of particles a non-equilibrium population of magnetic sublevels m j of angular momenta is created. We make a distinction between the alignment of momenta, for instance in the absorption of linear polarized light, when there is no difference between the population of ± m j -sublevels, and orientation , when such a difference exists. Anisotropic distribution of angular momenta in an excited state, as produced in absorption, manifests itself directly in the polarization of fluorescence. It is rather likely that understanding of the anisotropic distribution of the angular momenta of atoms was enhanced by Hanle's [184] discovery in 1924.
Abstract Angular momentum in classical mechanics is given by a vector. The plane perpendicular to this vector, in accordance to central field theory, determines the space in which particle motion takes place. No such simple picture exists in quantum mechanics. The states of a particle in a central field are proportional to spherical harmonics which do not define any plane of motion. In the first part of this paper we discuss the angular distribution of particle position and compare it to the classical probabilistic approach. In the second part, the matter of addition of angular momenta is discussed. In classical mechanics this means addition of vectors, while in quantum mechanics Clebsch–Gordan coefficients have to be used. We have found classical approximations to quantum coefficients and the limit of their applicability. This analysis gives a basis for the so-called ‘vector addition model’ used in some elementary textbooks on atomic physics. It can help to better understand the addition of angular momenta in quantum mechanics.
We have recently reported a derivation of the relationship between the quantum and classical descriptions of angular momentum polarization [M. P. de Miranda and F. Javier Aoiz, Phys. Rev. Lett. 93, 083201 (2004)]. This paper presents a detailed account of the derivation outlined in that paper, and discusses the implications of the new results. These include (i) a new expression of the role of the uncertainty principle in the broadening of angular momentum distributions, (ii) the attribution of azimuthal fluctuations of angular momentum distributions to spatial quantum beats, (iii) the definition of a new Fourier transform of the density matrix, distinct from those suggested in the past, that provides an alternative view of how the quantum description of angular momentum polarization approaches the classical one in the correspondence principle limit, (iv) a prescription for the determination of a quasiclassical angular momentum distribution function that does not suffer from problems encountered with its purely classical counterpart, and (v) a description of how angular momentum distributions commonly visualized with recourse to the classical vector model can be depicted with exact and well-defined quantum mechanics.
The Wigner representation of angular-momentum orientation in the classical limit on $J\ensuremath{\gg}1$ has been used to derive an equation of angular-momentum motion in the case of a closed two-level system interacting with an arbitrary polarized radiation. This equation enables us to carry out a theoretical analysis of angular-momentum motion and consider final states of the quantum system for all types of dipole transitions. We have found that in the case of a zero magnetic field in the final state of the system with $\stackrel{\ensuremath{\rightarrow}}{J}J$ or $\stackrel{\ensuremath{\rightarrow}}{J}J+1$ optical transition, the angular momentum is directed along or opposite to the wave vector of the radiation depending on the sign of the polarization ellipsity, while for a linear polarization the angular momentum is isotropically distributed on the plane orthogonal to the polarization vector. For the $\stackrel{\ensuremath{\rightarrow}}{J}J\ensuremath{-}1$ transition two directions of angular momentum are possible in the final state. These directions are determined by the ellipsity of polarization. The spatial size of the final distribution of the angular momentum has been defined by the quantum uncertainty, 1/J,1/\sqrt{J},1/J​, of the angular-momentum orientation. In the case of the $\stackrel{\ensuremath{\rightarrow}}{J}J\ensuremath{-}1$ or $\stackrel{\ensuremath{\rightarrow}}{J}J,$ transition particles come into ``dark'' states while for the $\stackrel{\ensuremath{\rightarrow}}{J}J+1$ transition they occupy the ``brightest'' state. In the presence of a nonzero magnetic field, particles with $\stackrel{\ensuremath{\rightarrow}}{J}J$ transition have in the final state only one angular-momentum orientation, i.e., along or opposite to the direction of the magnetic field depending on the polarization ellipsity sign. For the $\stackrel{\ensuremath{\rightarrow}}{J}J+1$ transition both directions are possible, i.e., along and opposite to the magnetic field. In the case of the $\stackrel{\ensuremath{\rightarrow}}{J}J\ensuremath{-}1$ transition the directions of the angular momentum form a cone around the magnetic field.
In this paper, a coherent superposition of angular-momentum states created by absorption of polarized light by molecules is analyzed. Attention is paid to the time evolution of wave packets representing the spatial orientation of the internuclear axis of a diatomic molecule. Two examples are considered in detail. Molecules absorbing light in a permanent magnetic field experiencing the Zeeman effect and molecules absorbing light in a permanent electric field experiencing the quadratic Stark effect. In a magnetic field, we have a wave packet that evolves in time exactly as a classical dipole oscillator in a permanent magnetic field (classical-physics picture of the Zeeman effect). In the second case, we have a wave packet that goes through periodical changes of shape of the packet with revivals of the initial shape. This is pure quantum behavior. The classical motion of angular momentum in an electric field in the case of a quadratic Stark effect is known to be a periodic. Solutions obtained for wave packet evolution are briefly compared with Rydberg-state coherent wave packets and harmonic-oscillator wave packets. Zeeman and Stark effects in small molecules continuously attract the attention of researchers, theoreticians, as well as experimentalists. These investigations allow us to obtain a deeper understanding of the interaction of molecules with stationary external fields and also can be used as a practical tool to measure different molecular characteristics, such as permanent electric or magnetic dipole moments, intramolecular perturbations, etc. It is worthwhile analyzing these effects as an evolution of wave packets. All this motivates a comparison of the quantum and classical picture of Zeeman and Stark effects in molecules.PACS No.: 33.55.Be