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arXiv:1603.00120 · Physical review. B./Physical review. B

Two-photon upconversion affected by intermolecule correlations near metallic nanostructures

Yoshiki Osaka, Nobuhiko Yokoshi, Hajime Ishihara

Published Apr 18, 2016• 1 citation
arXivHTMLPDF

Abstract

We investigate an efficient two-photon upconversion process in more than one molecule coupled to an optical antenna. In the previous paper [Y. Osaka et al., Phys. Rev. Lett. 112, 133601 (2014)], we considered the two-photon upconversion process in a single molecule within one-dimensional input-output theory and revealed that controlling the antenna-molecule coupling enables the efficient upconversion with radiative loss in the antenna suppressed. In this paper, aiming to propose a way to enhance the total probability of antenna-photon scattering, we extend the model to the case of multiple molecules. In general, the presence of more than one molecule decreases the upconversion probability because they equally share the energy of the two photons. However, it is shown that we can overcome the difficulty by controlling the intermolecule coupling. Our result implies that, without increasing the incident photon number (light power), we can enlarge the net probability of the two-photon upconversion.

DOI
10.1103/physrevb.93.155420

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We investigate an efficient two-photon upconversion process in more than one molecule coupled to an optical antenna. In the previous paper [Y. Osaka et al., Phys. Rev. Lett. 112, 133601 (2014)], we considered the two-photon upconversion process in a single molecule within one-dimensional input-output theory and revealed that controlling the antenna-molecule coupling enables the efficient upconversion with radiative loss in the antenna suppressed. In this paper, aiming to propose a way to enhance the total probability of antenna-photon scattering, we extend the model to the case of multiple molecules. In general, the presence of more than one molecule decreases the upconversion probability because they equally share the energy of the two photons. However, it is shown that we can overcome the difficulty by controlling the intermolecule coupling. Our result implies that, without increasing the incident photon number (light power), we can enlarge the net probability of the two-photon upconversion.
We theoretically investigate the up-conversion process of two entangled photons on a molecule, which is coupled by a cavity or nanoscale metallic structure. Within one-dimensional input-output theory, the propagators of the photons are derived analytically and the up-conversion probability is calculated numerically. It is shown that the coupling with the nanostructure clearly enhances the process. We also find that the enhancement becomes further pronounced for some balanced system parameters, such as the quantum correlation between photons, radiation decay, and coupling between the nanostructure and molecule. The nonmonotonic dependencies are reasonably explained in view of quantum interference between the coupled modes of the whole system. This result indicates that controlling quantum interference and correlation is crucial for few-photon nonlinearity, and provides a new guidance to wide variety of fields, e.g., quantum electronics and photochemistry.
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We analyze the dynamics of a quantum dipole emitter (QDE) illuminated by a resonant electromagnetic field and placed close to a metal nanostructure, whose response to the incident field is phase shifted by 3π/2 (-π/2). It is found that, due to the phase shift in a field scattered by the nanostructure (and acting on the QDE along with the incident field), QDE dynamics is characterized by a fast QDE transition to the excited state followed by relaxation to a stable superposition (of the excited and ground states) with a close to 1 probability of the QDE to be found in the excited state. We further argue that this effect can advantageously be used for luminescence upconversion enhancement when being realized for a lower excited state in the energy transfer upconversion process since, by largely eliminating the radiative relaxation channel, the probability of excitation transfer will be increased.
Optical nano-antennae have been integrated with semiconductor lasers to intensify light at the nanoscale and photodiodes to enhance photocurrent. In quantum optics, plasmonic metal structures have been used to enhance nonclassical light emission from single quantum dots. Absorption and detection of single photons from free space could also be enhanced by nanometallic antennae, but this has not previously been demonstrated. Here, we use nano-optical transmission effects in a one-dimensional gold structure, combined with optical cavity resonance, to form optical nano-antennae, which are further used to couple single photons from free space into a 80-nm-wide superconducting nanowire. This antenna-assisted coupling enables a superconducting nanowire single-photon detector with 47% device efficiency at the wavelength of 1550 nm and 9-μm-by-9-μm active area while maintaining a reset time of only 5 ns. We demonstrate nanoscale antenna-like structures to achieve exceptional efficiency and speed in single-photon detection.
Multiple photon absorption processes typically have a nonlinear dependence on the amplitude of the incident optical field. On the other hand, quantum technologies rely on single photon events. It has therefore been of great technical difficulty to achieve nonlinear devices using single photons. This is due to the small cross-section of absorption in room temperature devices, with multi-photon absorption events occurring with extremely low probability. The lack of access to nonlinear processes severely inhibits the use of optics for a large number of applications surrounding quantum technologies. We demonstrate experimentally that by exploiting a coherent absorption mechanism for N=2 N00N states, outlined theoretically by Jeffers in 2000 [1] and experimentally explored by Roger et. al. in 2016 [2], that it is possible to determine and enhance the number of two photon states that are absorbed. Here a 50% absorbing metasurface is placed inside a Sagnac interferometer into which we inject a N00N state. We show that by tuning the phase φ of the input state, |2,0〉 + exp(-ί2φ) |0,2〉, we can selectively tune the output state. For an input phase of φ = π/2 or 3π/2 we find that a single photon is absorbed with 100% probability. However, when we tune the input phase to φ = 0 or π we see that either 0 or 2 photons are absorbed with equal probability. We have developed a theoretical model that, with no free parameters, fits the experimentally measured two-photon contribution and finds the maximum contribution of |0,0) (0,0| to the output state to be 40.5%.