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arXiv:1507.07734 · Physical review. B./Physical review. B

Enhancement of four-wave mixing via interference of multiple plasmonic conversion paths

S. K. Singh, Musa Kurtuluş Abak, Mehmet Emre Taşgın

Published Jan 7, 2016• 50 citations
arXivHTMLPDF

Abstract

Recent experiments demonstrate that plasmonic resonators can enhance the four-wave mixing (FWM) process by several orders of magnitude, due to the localization of the incident fields. We show that, when the plasmonic resonator is coupled to two quantum emitters, a three orders of magnitude enhancement can be obtained on top of the enhancement due to the localization. We explicitly demonstrate---on an expression for the steady-state FWM amplitude---how the presence of a Fano resonance leads to the cancellation of nonresonant terms in a FWM process. A cancellation in the denominator gives rise to an enhancement in the nonlinearity. The explicit demonstration we present here guides one to a method for achieving even larger enhancement factors by introducing additional coupling terms. The method is also applicable to Fano resonances induced by all-plasmonic couplings, which are easier to control in experiments.

DOI
10.1103/physrevb.93.035410

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Recent experiments demonstrate that plasmonic resonators can enhance the four-wave mixing (FWM) process by several orders of magnitude, due to the localization of the incident fields. We show that, when the plasmonic resonator is coupled to two quantum emitters, a three orders of magnitude enhancement can be obtained on top of the enhancement due to the localization. We explicitly demonstrate---on an expression for the steady-state FWM amplitude---how the presence of a Fano resonance leads to the cancellation of nonresonant terms in a FWM process. A cancellation in the denominator gives rise to an enhancement in the nonlinearity. The explicit demonstration we present here guides one to a method for achieving even larger enhancement factors by introducing additional coupling terms. The method is also applicable to Fano resonances induced by all-plasmonic couplings, which are easier to control in experiments.
We show that, Four wave mixing (FWM) processes of grating can be controlled by the presence of interactions with a quantum dot or a molecule made by coupled quantum dots. By choosing the appropriate level spacing for the quantum emitter, one can either suppress or enhance the Four wave mixing process. We revel theoretically the underlying mechanism for this effect. (i) Suppression in FWM intensity occurs simply because induced Electromagnetic Induced Transparency does not allow the excitation at converted FWM frequency. (ii) Enhancement emerges since FWM process can be brought to resonance. Path interference effect cancels the nonresonant frequency terms. Furthermore, we have also shown that in case of coupled quantum dots enhancement increases significantly as compared to the case of a single quantum dot.
We propose and analyze an efficient way to enhance four-wave mixing (FWM) signals in a four-subband semiconductor quantum well via Fano-type interference. By using Schrödinger-Maxwell formalism, we derive explicitly analytical expressions for the input probe pulse and the generated FWM field in linear regime under the steady-state condition. With the aid of interference between two excited subbands tunneling to the common continuum, the efficiency to generate FWM field is found to be significantly enhanced, up to 35%. More interestingly, a linear growth rate in the FWM efficiency is demonstrated as the strength of Fano-type interference increases in presence of the continuum states, which can be maintained for a certain propagation distance (i.e., 50μm).
We study theoretically the quantum optical properties of hybrid molecules composed of an individual quantum dot and a metallic nanoparticle. We calculate the resonance fluorescence of this composite system. Its incoherent part, arising from nonlinear quantum processes, is enhanced by more than 2 orders of magnitude as compared to that of the dot alone. The coupling between the two systems gives rise to a Fano interference effect which strongly influences the quantum statistical properties of the scattered photons: a small frequency shift of the incident light field may cause changes in the intensity correlation function of the scattered field of orders of magnitude. The system opens a good perspective for applications in active metamaterials and ultracompact single-photon devices.
An influence of nonlinear interference processes at quantum transitions in strong resonance electromagnetic fields on absorption, amplification and refractive indices as well as on four-wave mixing processes is investigated. Doppler broadening of the coupled transitions, incoherent excitation, relaxation processes, as well as power saturation processes associated with the coupled levels are taken into account. Both closed (ground state is involved) and open (only excited states are involved) energy level configurations are considered. Common expressions are obtained which allow to analyze the optical characteristics (including gain without inversion and enhanced refractive index at vanishing absorption) for various V, (Lambda) and H configurations of interfering transitions by a simple substitution of parameters. Similar expressions for resonant four-wave mixing (FWM) in Raman configurations are derived too. Crucial role of Doppler broadening is shown. Theory is applied for numerical analysis of some recent and potential experiments.
When nonlinear four-wave mixing (FWM) is resonant with a Raman transition, it causes coupling between lightwaves separated by two Raman frequency shifts. This coupling is manifested in effects such as Raman gain suppression, higher-order Stokes generation, and coherent Raman spectroscopies (e.g., CARS). An understanding of these effects, however, has been impeded by a widespread misconception that Raman-resonant FWM does not transfer energy between the lightwaves and the medium. The equations for the photon densities at each light frequency show that, in actuality, two medium excitations are created or destroyed for each photon produced by FWM. This point may be further clarified by consideration of the driving nonlinear polarization and by comparisons with broadband Raman conversion and nonresonant FWM. The Raman gain suppression effect may be understood qualitatively in terms of destructive interference between FWM and the usual stimulated Raman process.
We consider effects which occur when four-wave sum frequency generation and multiphoton ionization are induced by lasers tuned near a three-photon resonance and simultaneously near or at a dipole allowed four-photon resonance. In studies with unfocused laser beams, if the phase mismatch of the generated four-wave-mixing field is large and the related two-photon resonance for the absorption of a four-wave-mixing photon and a laser photon results in strong absorption of the four-wave-mixing field, a coherent cancellation occurs between the pumping of the resonance by two- and four-photon processes. This interference effect occurs when the first laser is tuned on either side of the three-photon resonance and \ensuremath{\Vert}\ensuremath{\Delta}kr{\mathit{k}}_{\mathit{r}}kr​L\ensuremath{\Vert}\ensuremath{\gg}1, where \ensuremath{\Delta}kr{\mathit{k}}_{\mathit{r}}kr​ is the mismatch and L is the length of the path of the laser beams in the gas. With focused laser beams large differences occur between ionization with unidirectional beams and with counterpropagating laser beams when \ensuremath{\Vert}\ensuremath{\Delta}kr{\mathit{k}}_{\mathit{r}}kr​b\ensuremath{\Vert}\ensuremath{\gg}1, where b is the confocal parameter of the focused laser beams. Strong absorption of the four-wave-mixing field is shown not to be necessary for strong destructive interference with focused laser beams when the phase mismatch is large. This work also suggests an explanation for earlier experiments where the presence of a four-photon resonance enabled the generation of third-harmonic light in a positively dispersive wavelength region. We argue that this process can occur when the laser used to achieve the four-photon resonance is focused on the small z (z is the coordinate in the direction of propagation) side of the focal point of the laser responsible for the third-harmonic generation. In this way the absorption of the third-harmonic light on one side of the focal point is made much stronger than on the other side. Correspondingly, contributions to the third-harmonic field from the two sides of the focal point are unequal and cannot undergo complete destructive interference as would otherwise occur in a positively dispersive region.