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Register a new userTwo-photon spontaneous emission in atomically thin plasmonic nanostructures
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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.
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As a high-order quantum transition, two-photon emission has an extremely low occurrence rate compared to one-photon emission, thus having been considered a forbidden process. Here, we propose a scheme that allows ultrafast two-photon emission, leveraging highly confined surface plasmon polariton modes in a degenerately-doped, light-emitting semiconductor thin film. The surface plasmon polariton modes are tailored to have simultaneous spectral and spatial overlap with the two-photon emission in the semiconductor. Using degenerately-doped InSb as the prototype material, we show that the two-photon emission can be accelerated by 10 orders of magnitude: from tens of milliseconds to picoseconds, surpassing the one-photon emission rate. Our result provides a semiconductor platform for ultrafast single and entangled photon generation, with a tunable emission wavelength in the mid-infrared.
Deep subwavelength integration of high-definition plasmonic nanostructures is of key importance for the development of future optical nanocircuitry for high-speed communication, quantum computation and lab-on-a-chip applications. So far the experimental realization of proposed extended plasmonic networks consisting of multiple functional elements remains challenging, mainly due to the multi-crystallinity of commonly used thermally evaporated gold layers. Resulting structural imperfections in individual circuit elements will drastically reduce the yield of functional integrated nanocircuits. Here we demonstrate the use of very large (>100 micron^2) but thin (<80 nm) chemically grown single-crystalline gold flakes, which, after immobilization, serve as an ideal basis for focused-ion beam milling and other top-down nanofabrication techniques on any desired substrate. Using this methodology we obtain high-definition ultrasmooth gold nanostructures with superior optical properties and reproducible nano-sized features over micrometer length scales. Our approach provides a possible solution to overcome the current fabrication bottleneck and to realize high-definition plasmonic nanocircuitry.
Developments in quantum technologies lead to new applications that require radiation sources with specific photon statistics. A widely used Poissonian statistics are easily produced by lasers; however, some applications require super- or sub-Poissonian statistics. Statistical properties of a light source are characterized by the second-order coherence function g^(2)(0). This function distinguishes stimulated radiation of lasers with g^(2)(0)=1 from light of other sources. For example, g^(2)(0)=2 for black-body radiation, and g^(2)(0)=0 for single-photon emission. One of the applications requiring super-Poissonian statistics (g^(2)(0)>1) is ghost imaging with thermal light. Ghost imaging also requires light with a narrow linewidth and high intensity. Currently, rather expensive and inefficient light sources are used for this purpose. In the last year, a superluminescent diode based on amplified spontaneous emission (ASE) has been considered as a new light source for ghost imaging. Even though ASE has been widely studied, its photon statistics has not been settled - there are neither reliable theoretical estimates of the second-order coherence function nor unambiguous experimental data. Our computer simulation clearly establishes that coherence properties of light produced by ASE are similar to that of a thermal source with g^(2)(0)=2 independent of pump power. This result manifests the fundamental difference between ASE and laser radiation.
Nanofabrication of photonic components based on dielectric-loaded surface plasmon-polariton waveguides (DLSPPWs) excited by single nitrogen vacancy (NV) centers in nanodiamonds is demonstrated. DLSPPW circuits are built around NV containing nanodiamonds, which are certified to be single-photon emitters, using electron-beam lithography of hydrogen silsesquioxane (HSQ) resist on silver-coated silicon substrates. A propagation length of ~20 {mu}m for the NV single-photon emission is measured with DLSPPWs. A 5-fold enhancement in the total decay rate and up to 63% coupling efficiency to the DLSPPW mode is achieved, indicating significant mode confinement. Finally, we demonstrate routing of single plasmons with DLSPPW-based directional cou-plers, revealing the potential of our approach for on-chip realization of quantum-optical networks.
We demonstrate a fundamental breakdown of the photonic spontaneous emission (SE) formula derived from Fermis golden rule, in absorptive and amplifying media, where one assumes the SE rate scales with the local photon density of states, an approach often used in more complex, semiclassical nanophotonics simulations. Using a rigorous quantization of the macroscopic Maxwell equations in the presence of arbitrary linear media, we derive a corrected Fermis golden rule and master equation for a quantum two-level system (TLS) that yields a quantum pumping term and a modified decay rate that is net positive. We show rigorous numerical results of the temporal dynamics of the TLS for an example of two coupled microdisk resonators, forming a gain-loss medium, and demonstrate the clear failure of the commonly adopted formulas based solely on the local density of states.
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