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arXiv:0705.2541 · Physical Review Letters

Tailoring Optical Nonlinearities via the Purcell Effect

Peter A. Bermel, Alejandro W. Rodríguez, John D. Joannopoulos, Marin Soljacic A

Published Aug 3, 2007• 51 citations
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Abstract

We predict that the effective nonlinear optical susceptibility can be tailored using the Purcell effect. While this is a general physical principle that applies to a wide variety of nonlinearities, we specifically investigate the Kerr nonlinearity. We show theoretically that using the Purcell effect for frequencies close to an atomic resonance can substantially influence the resultant Kerr nonlinearity for light of all (even highly detuned) frequencies. For example, in realistic physical systems, enhancement of the Kerr coefficient by one to two orders of magnitude could be achieved.

DOI
10.1103/physrevlett.99.053601

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We predict that the effective nonlinear optical susceptibility can be tailored using the Purcell effect. While this is a general physical principle that applies to a wide variety of nonlinearities, we specifically investigate the Kerr nonlinearity. We show theoretically that using the Purcell effect for frequencies close to an atomic resonance can substantially influence the resultant Kerr nonlinearity for light of all (even highly detuned) frequencies. For example, in realistic physical systems, enhancement of the Kerr coefficient by one to two orders of magnitude could be achieved.
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We theoretically investigate the enhancement of Kerr nonlinearity through anisotropic Purcell factors provided by plasmon nanostructures. In a three-level atomic system with crossing damping, larger anisotropism of Purcell factors leads to more enhanced Kerr nonlinearity in electromagnetically induced transparency windows. While for fixed anisotropic Purcell factors, Kerr nonlinearity with orthogonal dipole moments increases with the decrease of its crossing damping, and Kerr nonlinearity with nonorthogonal dipole moments is very sensitive to both the value of crossing damping and the orientation of the dipole moments. We design the non-resonant gold nanorods array, which only provides subwavelength-confined anisotropic Purcell factors, and demonstrate that the Kerr nonlinearity of cesium atoms close to the nanorods array can be modulated at the nanoscale. These findings should have potential application in ultracompact quantum logic devices.
In earlier chapters we have considered in detail the susceptibility formalism of nonlinear optics, which is perhaps the most familiar approach and has a wide range of application. Starting from the constitutive relations of Chapter 2, the susceptibility formalism is quite general. In many practical applications, a particular phenomenon can be described accurately by a single order of nonlinearity, and the susceptibility then provides a useful and convenient description. However, this is not always the case. Some of the most interesting phenomena in nonlinear optics involve close resonance with the transition frequencies of the medium, and perhaps also the use of very intense optical fields. As remarked in §4.5, in these circumstances the resonant susceptibilities display mathematical divergences which are clearly unphysical. Strictly, these divergences occur only because higher-order nonlinearities have been neglected. Successive orders of nonlinearity take into account such effects as saturation, power broadening and level shifts (optical Stark effect). For intense fields or very close resonance, the contributions from several orders of nonlinearity may be comparable in magnitude. Therefore, despite its generality, the susceptibility formalism does not necessarily provide the most practical approach for the description of resonant processes. This chapter is concerned with the problem of deriving alternative and more manageable descriptions of resonant nonlinear processes, illustrated by examples. For much of the chapter, the nonlinear medium is treated as a two-level system (described in §6.2).