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Purcell factor engineering in plasmonic nanostructures for the enhanced generation of energy-time entangled states

Pavel Ginzburg, Alexander N. Poddubny, Pavel A. Belov, Anatoly V. Zayats, Yuri S. Kivshar

Published Jan 1, 2012• 0 citations
OpenAlex

Abstract

We summarize our studies of the plasmonic enhancements of the spontaneous two-photon emission. In particular, we draw attention to the rigorous investigation of quantum framework for the multi-photon spontaneous decay rates in an environment with arbitrary structure of electromagnetic modes. We demonstrate that nanostructured environment can be used for tailoring the basic characteristics of the two-photon emission such as spectrum, lifetime, and entanglement. Moreover, careful engineering of the two-photon Purcell enhancement may provide any desired spectral response and may serve as an ultimate route for designing light sources with novel properties.

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arXiv:1709.07028•Sep 20, 2017•0 citations
We summarize our studies of the plasmonic enhancements of the spontaneous two-photon emission. In particular, we draw attention to the rigorous investigation of quantum framework for the multi-photon spontaneous decay rates in an environment with arbitrary structure of electromagnetic modes. We demonstrate that nanostructured environment can be used for tailoring the basic characteristics of the two-photon emission such as spectrum, lifetime, and entanglement. Moreover, careful engineering of the two-photon Purcell enhancement may provide any desired spectral response and may serve as an ultimate route for designing light sources with novel properties.
The rate of spontaneous emission is known to depend on the environment of a emitter, and the enhancement of one-photon emission in a resonant cavity is known as the Purcell effect. Here we develop a theory of spontaneous two-photon emission for a general electromagnetic environment including inhomogeneous dispersive and absorptive media. This theory is used to evaluate the two-photon Purcell enhancement in the vicinity of metallic nanoparticles and demonstrates that the surface-plasmon resonances supported by these particles can increase the emission rate by more than two orders of magnitude. The control over two-photon Purcell enhancement given by tailored nanostructured environments could provide an emitter with any desired spectral response and may serve as an ultimate route for designing light sources with novel properties.
We present a novel photonic model that enables an efficient computation of the two-photon Purcell effect of a quantum emitter in the vicinity of an arbitrary photonic structure. Our framework is relevant for the plasmonic nanocavities used to enhance higher-order light-matter interactions, as it goes beyond the dipolar approximation. The computation of Purcell factors through classical electromagnetic simulations determines the influence of the environment without tedious analytic calculations. We demonstrate that placing a hydrogen-like emitter close to a silver nanodisk enhances the transition rate by 5 and 11 orders of magnitude via electric dipole and quadrupole two-photon transitions, respectively. This process has exciting implications for future research, including the potential for efficient entangled two-photon sources.
Frontier quantum engineering tasks require reliable control over light-matter interaction dynamics, which could be obtained by introducing electromagnetic structuring. Initiated by the Purcell's discovery of spontaneous emission acceleration in a cavity, the concept of electromagnetic modes' design have gained a considerable amount of attention due to development of photonic crystals, micro-resonators, plasmonic nanostructures and metamaterials. Those approaches, however, offer qualitatively different strategies for tailoring light-matter interactions and are based on either high quality factor modes shaping, near field control, or both. Remarkably, rigorous quantum mechanical description might address those processes in a different fashion. While traditional cavity quantum electrodynamics tools are commonly based on mode decomposition approach, few challenges rise once dispersive and lossy nanostructures, such as noble metals (plasmonic) antennas or metamaterials, are involved. The primary objective of this review is to introduce key methods and techniques while aiming to obtain comprehensive quantum mechanical description of spontaneous, stimulated and higher order emission and interaction processes, tailored by nanostructured material environment. The main challenge and the complexity here are set by the level of rigorousity, up to which materials should be treated. While relatively big nanostructured features (10 nm and larger) could be addressed by applying fluctuation–dissipation theorem and corresponding Green functions' analysis, smaller objects will require individual approach. Effects of material granularity, spatial dispersion, tunneling over small gaps, material memory and others will be reviewed. Quantum phenomena, inspired and tailored by nanostructured environment, plays a key role in development of quantum information devices and related technologies. Rigorous analysis is required for both examination of experimental observations and prediction of new effects.
The ability to harness light-matter interactions at the few-photon level plays a pivotal role in quantum technologies. Single photons-the most elementary states of light-can be generated on demand in atomic and solid state emitters. Two-photon states are also key quantum assets, but achieving them in individual emitters is challenging because their generation rate is much slower than competing one-photon processes. We demonstrate that atomically thin plasmonic nanostructures can harness two-photon spontaneous emission, resulting in giant far field two-photon production, a wealth of resonant modes enabling tailored photonic and plasmonic entangled states, and plasmon-assisted single-photon creation orders of magnitude more efficient than standard one-photon emission. We unravel the two-photon spontaneous emission channels and show that their spectral line shapes emerge from an intricate interplay between Fano and Lorentzian resonances. Enhanced two-photon spontaneous emission in two-dimensional nanostructures paves the way to an alternative efficient source of light-matter entanglement for on-chip quantum information processing and free-space quantum communications.
Single-photon and correlated two-photon sources are important elements for optical information systems. Nonlinear downconversion light sources are robust and stable emitters of single photons and entangled photon pairs. However, the rate of downconverted light emission, dictated by the properties of low-symmetry nonlinear crystals, is typically very small, leading to significant constrains in device design and integration. In this paper, we show that the principles for spontaneous emission control (i.e. Purcell effect) of isolated emitters in nanoscale structures, such as metamaterials, can be generalized to describe the enhancement of nonlinear light generation processes such as parametric down conversion. We develop a novel theoretical framework for quantum nonlinear emission in a general anisotropic, dispersive and lossy media. We further find that spontaneous parametric downconversion in media with hyperbolic dispersion is broadband and phase-mismatch-free. We predict a 1000-fold enhancement of the downconverted emission rate with up to 105 photon pairs per second in experimentally realistic nanostructures. Our theoretical formalism and approach to Purcell enhancement of nonlinear optical processes, provides a framework for description of quantum nonlinear optical phenomena in complex nanophotonic structures.