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Journal of Physics B Atomic Molecular and Optical Physics

An algorithm for the nonlinear optical susceptibilities of dipolar molecules, and an application to third harmonic generation

Davıd L. Andrews, Luciana C. Dávila Romero, William J. Meath

Published Jan 1, 1999• 29 citations
Publisher

Abstract

It is well known that a simple transformation of the electric dipole interaction provides a convenient means for ascertaining the effects of permanent dipoles on the optical behaviour of systems with a response dominated by two energy levels. By establishing the general validity of the procedure for parametric processes such as harmonic generation, it is shown how the detailed structure of the optical susceptibilities associated with arbitrary forms of optical nonlinearity can be ascertained by an algorithmic method, based on a novel interpretation of the relevant quantum electrodynamical Feynman diagrams. Application of the algorithm to second and third harmonic generation illustrates its usefulness and simplicity, whilst also providing new results and revealing features, related to the role of permanent dipoles, which have not hitherto been apparent.

DOI
10.1088/0953-4075/32/1/003

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It is well known that a simple transformation of the electric dipole interaction provides a convenient means for ascertaining the effects of permanent dipoles on the optical behaviour of systems with a response dominated by two energy levels. By establishing the general validity of the procedure for parametric processes such as harmonic generation, it is shown how the detailed structure of the optical susceptibilities associated with arbitrary forms of optical nonlinearity can be ascertained by an algorithmic method, based on a novel interpretation of the relevant quantum electrodynamical Feynman diagrams. Application of the algorithm to second and third harmonic generation illustrates its usefulness and simplicity, whilst also providing new results and revealing features, related to the role of permanent dipoles, which have not hitherto been apparent.
Quantum electrodynamics furnishes a new type of representation for the characterisation of nonlinear optical processes. The treatment elicits the detailed role and interplay of specific quantum channels, information that is not afforded by other methods. Following an illustrative application to the case of Rayleigh scattering, the method is applied to second and third harmonic generation. Derivations are given of parameters that quantify the various quantum channels and their interferences; the results are illustrated graphically. With given examples, it is shown in some systems that optical nonlinearity owes its origin to an isolated channel, or a small group of channels.
This thesis employs molecular quantum electrodynamical theory to analyse the interactions between light and matter for four main processes. The first to be considered is Raman scattering, where the effect of the electrodynamic environment for the centre of spectroscopic interest is considered. This is achieved by engaging a retarded dipole-dipole interaction between the centre and a neighbouring molecule. Physically, this is explained by a virtual photon between the pair of centres. The results predict characteristic new lines on the Raman spectrum, for the species, arising from the engagement of selection rules not limited to those of a two-photon process. \nThe second process, is hyper-Rayleigh scattering, in which a single multipolar coupling is considered in place of the more familiar electric dipole. This modification to the theory subverts the standard selection rules for a three-photon process, which can allow for second-harmonic emission to be generated by a centre of high symmetry, such as a centrosymmetric molecule. \nThe third process offers another means of subverting the standard selection rules for second-harmonic generation, namely by incorporating six-wave mixing. First, the general mechanism is developed and pertinent results are expressed for the widely-deployed depolarisation ratio. Following this, structured light is considered and by utilising orbital angular momentum (OAM) conservation arguments, the pair of harmonic photons are found to display quantum entanglement. Moreover, the relative magnitudes of the possible emissions are found to correspond directly to that of the binomial coefficients. \nThis thesis concludes with a family of novel structures capable of directly generating OAM light. This work exploits symmetry characteristics for a delocalised excitonic structure that can allow for a more complex multipolar emission than that of any isolated centres. The phase of the exciton is shown to display an azimuthal phase progression, a vortex feature most commonly associated with Laguerre-Gaussian light.
We calculate the third-order nonlinear absorption and dispersion (self-phase-modulation and cross-phase modulation) of a homogeneously broadened two-level molecular system with permanent dipole moments interacting with (1) an optical field of frequency \ensuremath{\omega}, and (2) two optical fields of frequency ${\mathrm{\ensuremath{\omega}}}_{1}$ and ${\mathrm{\ensuremath{\omega}}}_{2}$, i.e., the susceptibilities ${\mathrm{\ensuremath{\chi}}}^{(3)}$(-\ensuremath{\omega};\ensuremath{\omega},-\ensuremath{\omega},\ensuremath{\omega}) and ${\mathrm{\ensuremath{\chi}}}^{(3)}$(-${\mathrm{\ensuremath{\omega}}}_{1}$;${\mathrm{\ensuremath{\omega}}}_{1}$,-${\mathrm{\ensuremath{\omega}}}_{2}$,${\mathrm{\ensuremath{\omega}}}_{2}$). Sharp features in the nonlinear absorption and dispersion appear whenever one- or two-photon resonance conditions are met. Only features corresponding to one-photon resonance arise if the difference between the permanent dipole moments of the levels, \ensuremath{\Delta}\ensuremath{\mu}, vanishes. The ${\mathrm{\ensuremath{\chi}}}^{(3)}$(-\ensuremath{\omega};\ensuremath{\omega},-\ensuremath{\omega},\ensuremath{\omega}) spectrum has two features, one at frequency ${\mathrm{\ensuremath{\omega}}}_{\mathit{b}\mathit{a}}$ dominated by contributions proportional to ${\mathrm{\ensuremath{\mu}}}_{\mathit{a}\mathit{b}}^{4}$, where ${\mathrm{\ensuremath{\mu}}}_{\mathit{a}\mathit{b}}$ is the transition dipole moment of the two levels with transition frequency ${\mathrm{\ensuremath{\omega}}}_{\mathit{b}\mathit{a}}$, and the other at frequency ${\mathrm{\ensuremath{\omega}}}_{\mathit{b}\mathit{a}}$/2 dominated by contributions proportional to (\ensuremath{\Delta}\ensuremath{\mu})2{)}^{2})2${\mathrm{\ensuremath{\mu}}}_{\mathit{a}\mathit{b}}^{2}$. Sharp features in ${\mathrm{\ensuremath{\chi}}}^{(3)}$(-${\mathrm{\ensuremath{\omega}}}_{1}$;${\mathrm{\ensuremath{\omega}}}_{2}$,-${\mathrm{\ensuremath{\omega}}}_{2}$,${\mathrm{\ensuremath{\omega}}}_{1}$) appear when ${\mathrm{\ensuremath{\omega}}}_{2}$ is near ${\mathrm{\ensuremath{\omega}}}_{\mathit{b}\mathit{a}}$,${\mathrm{\ensuremath{\omega}}}_{1}$,${\mathrm{\ensuremath{\omega}}}_{1}$+${\mathrm{\ensuremath{\omega}}}_{\mathit{b}\mathit{a}}$, and \ensuremath{\Vert}${\mathrm{\ensuremath{\omega}}}_{1}$-${\mathrm{\ensuremath{\omega}}}_{\mathit{b}\mathit{a}}$\ensuremath{\Vert}.
By means of a canonical transformation it is shown how it is possible to recast the equations for molecular nonlinear optics to completely eliminate ground-state static dipole coupling terms. Such dipoles can certainly play a highly important role in nonlinear optical response---but equations derived by standard methods, in which these dipoles emerge only as special cases of transition moments, prove unnecessarily complex. It has been shown that the elimination of ground-state static dipoles in favor of dipole shifts results in a considerable simplification in form of the nonlinear optical susceptibilities. In a fully quantum theoretical treatment the validity of such a procedure has previously been verified using an expedient algorithm, whose defense was afforded only by a highly intricate proof. In this paper it is shown how a canonical transformation method entirely circumvents such an approach; it also affords insights into the formulation of quantum field interactions.
We calculate the electric-field-induced second-harmonic-generation (EFISH) susceptibility of a homogeneously broadened two-level system with permanent dipole moments. This susceptibility has contributions from the second-harmonic-generation (SHG) susceptibility of the same system without the presence of a dc field and the four-wave-mixing (FWM) component of the susceptibility ${\ensuremath{\gamma}}_{\mathit{e}}$(-2\ensuremath{\omega};\ensuremath{\omega},\ensuremath{\omega},0). The magnitude and phase of the various contributions to EFISH arising from SHG and from FWM depend on the frequency of the fundamental optical field, the transition dipole moment ${\mathrm{\ensuremath{\mu}}}_{\mathit{a}\mathit{b}}$, the permanent dipole moment of the ground-state level ${\mathrm{\ensuremath{\mu}}}_{\mathit{a}\mathit{a}}$, and the difference of the ground- and excited-state dipole moments \ensuremath{\Delta}\ensuremath{\mu}. We present non-rotating-wave-approximation results for both the quasi-steady-state in systems where the dephasing time T2{\mathit{T}}_{2}T2​ is much shorter than the population decay time T1{\mathit{T}}_{1}T1​, so the polarization is in a steady state but the population is not, and for the complete steady state. Extraction of the SHG susceptibility from EFISH measurements is considered.
Starting with well known formulae for nth-order atomic susceptibilities, irreducible spherical tensor techniques and Racah algebra are used to put these in a form suitable for the treatment of complex nonlinear processes, e.g. where fine and hyperfine interactions can be included and the interacting fields can have quite general polarizations. By way of illustration the susceptibilities are calculated in detail for third harmonic generation and Raman scattering in alkali vapours, taking into account the effect of spin-orbit coupling.