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arXiv:1201.5072 · Physical Review B

Single-photon nonlinear optics with Kerr-type nanostructured materials

Sara Ferretti, Dario Gerace

Published Jan 10, 2012• 112 citations
arXivHTMLPDF

Abstract

We employ a quantum theory of the nonlinear optical response from an actual solid-state material possessing an intrinsic bulk contribution to the third-order nonlinear susceptibility (Kerr-type nonlinearity), which can be arbitrarily nanostructured to achieve diffraction-limited electro-magnetic-field confinement. By calculating the zero-time-delay second-order correlation of the cavity field, we set the conditions for using semiconductor or insulating materials with near-infrared energy gaps as an efficient means to obtain single-photon nonlinear behavior in prospective solid-state integrated devices, alternative to ideal sources of quantum radiation such as, e.g., single two-level emitters.

DOI
10.1103/physrevb.85.033303

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We employ a quantum theory of the nonlinear optical response from an actual solid-state material possessing an intrinsic bulk contribution to the third-order nonlinear susceptibility (Kerr-type nonlinearity), which can be arbitrarily nanostructured to achieve diffraction-limited electro-magnetic-field confinement. By calculating the zero-time-delay second-order correlation of the cavity field, we set the conditions for using semiconductor or insulating materials with near-infrared energy gaps as an efficient means to obtain single-photon nonlinear behavior in prospective solid-state integrated devices, alternative to ideal sources of quantum radiation such as, e.g., single two-level emitters.
The authors demonstrate here the nonlinear optical response of epsilon-near-zero (ENZ) nanostructures at the single-photon level using fully nonperturbative quantum theory of open systems with indium tin oxide materials and Kerr-type nonlinearity. Closed-form analytical results obtained for spherical nanoparticles are numerically validated and extended to geometries that can be fabricated using state-of-the-art electron-beam lithography, establishing a rigorous benchmark for understanding quantum nonlinear effects in ENZ nanostructures with optical losses. These results are important to emerging quantum technology, including on-chip single-photon nondemolition detection, sensing, and spectroscopy.
We propose the use of weakly nonlinear passive materials for prospective applications in integrated quantum photonics. It is shown that strong enhancement of native optical nonlinearities by electromagnetic field confinement in photonic crystal resonators can lead to single-photon generation only exploiting the quantum interference of two coupled modes and the effect of photon blockade under resonant coherent driving. For realistic system parameters in state of the art microcavities, the efficiency of such a single-photon source is theoretically characterized by means of the second-order correlation function at zero-time delay as the main figure of merit, where major sources of loss and decoherence are taken into account within a standard master equation treatment. These results could stimulate the realization of integrated quantum photonic devices based on non-resonant material media, fully integrable with current semiconductor technology and matching the relevant telecom band operational wavelengths, as an alternative to single-photon nonlinear devices based on cavity quantum electrodynamics with artificial atoms or single atomic-like emitters.
We propose the use of nanostructured photonic nanocavities made of ${\ensuremath{\chi}}^{(2)}$ nonlinear materials as prospective passive devices to generate strongly sub-Poissonian light via single-photon blockade of an input coherent field. The simplest scheme is based on the requirement that the nanocavity be doubly resonant, i.e., possess cavity modes with good spatial overlap at both the fundamental and second-harmonic frequencies. We discuss the feasibility of this scheme with state-of-the art nanofabrication technology and the possibility to use it as a passive single-photon source on demand.
The recent advent of optical metasurfaces, ultra-thin structures composed of nanoresonators facilitating strong light concentration [1–3], opens the path towards efficient \nfrequency conversion [4–7] in a material thousand times thinner than a human hair [8]. \nThere is a remarkable capacity to individually shape each nanoresonator of the metasurface to spatially and spectrally control the conversion process with unprecedented \nnanoscale resolution, facilitating an ultimate flexibility to selectively convert, focus, \nand image different colours with a single metasurface. The strong enhancement of the \nnonlinear processes in dielectric nanoresonators is largely due to the absence of material \nabsorption and the excitation of Mie-type bulk resonances [2]. The highest conversion \nefficiency to date has been achieved employing III-V semiconductor nanostructures, \nsuch as AlGaAs which is a non-centrosymmetric material with high quadratic nonlinear \nsusceptibility. In particular, second-harmonic generation efficiencies up to 10−4 have \nbeen recently demonstrated [8–12], six orders of magnitude higher than in plasmonics. \nSuch capabilities can make an immense fundamental and practical impact, including \nthe quantum state generation in nonlinear metasurfaces as we discuss in this chapter. \nThe quantum state of correlated photon-pairs is the essential building block for photon entanglement [13, 14], which underpins many quantum applications, including secure networks, enhanced measurement and lithography, and quantum information processing [15]. One of the most versatile techniques for the generation of correlated photons is the process of spontaneous parametric down-conversion (SPDC) [16, 17], see \nFig. 1. It allows for an arbitrary choice of energy and momentum correlations between \nthe generated photons, robust operation at room temperature, as well as for spatial and \ntemporal coherence between simultaneously pumped multiple SPDC sources. Alternative approaches based on atom-like single photon emitters, such as solid-state fluorescent atomic defects [18], quantum dots [19, 20], and 2D host materials [21, 22], have \nreached a high degree of frequency indistinguishability, purity and brightness [19, 20]. \nHowever, this comes with the expense of operation at cryogenic temperatures and lack \nof spatial coherence between multiple quantum emitters. These features might limit \npossible applications and reduce the potential for device scalability. Furthermore, the \nsmall size of the atomic sources often requires complex schemes aimed at coupling to \noptical nanoantennas and improving the photon extraction efficiency [21]. \nThe miniaturization of SPDC quantum-light sources to micro and nanoscale dimensions is a continuing quest, as it enables denser integration of functional quantum \ndevices. Traditionally, bulky cm-sized crystals were utilized for SPDC, entailing the \ndifficulty of aligning multiple optical elements after the SPDC crystal, while offering \nrelatively low photon-pair rates [17]. As a first step of miniaturization, SPDC was \nrealized in low-index-contrast waveguides, which allowed confining light down to several square micrometers transversely to the propagation direction, significantly enhancing the conversion efficiency [23]. However, this approach still requires centimetres \nof propagation length, which makes the on-chip integration with other elements challenging [24]. The introduction of high-index contrast waveguides and ring resonators \nallowed for shrinking the sizes necessary for SPDC to millimetres [25], and to tens \nof micrometers [26]. However, further miniaturisation down to the metasurfaces composed of nanoresonators requires conceptually different approaches.
Two-dimensional, atomically thin materials offer unique physical properties, such as a large second-order optical nonlinearity. Integrating these materials into a scalable and silicon-compatible platform could provide a pathway toward realizing low-power nonlinear optics. We have presented a formalism to calculate the effective nonlinear optical coefficient for a cavity integrated 2D material system as well as the cavity enhanced absorptive loss, which can be used to guide future experiments. We have also shown that the few-photon regime of cavity QED is within reach with a cavity quality factor of ∼10 5 –10 6, provided the loss at the second harmonic mode is minimized. As test applications, we have simulated the performances of (a) an optically bistable device and (b) a nanostructured device exhibiting single-photon blockade.
Achieving the regime of single-photon nonlinearities in photonic devices by just exploiting the intrinsic high-order susceptibilities of conventional materials would open the door to practical semiconductor-based quantum photonic technologies. Here we show that this regime can be achieved in a triply resonant integrated photonic device made of two coupled ring resonators, in a material platform displaying an intrinsic third-order nonlinearity. By strongly driving one of the three resonances of the system, a weak coherent probe at one of the others results in a strongly suppressed two-photon probability at the output, evidenced by an antibunched second-order correlation function at zero-time delay under continuous wave driving.