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Quantum Communications and Quantum Imaging

Orders of magnitude enhancement in two photon excitation efficiency using photonic molecules

Yao Zhou, Zihao Chen, Jung‐Tsung Shen

Published Sep 18, 2018• 2 citations
Publisher

Abstract

Photonic Molecule, also called Photonic Dimer, is a quantum bound state of two photons. A photonic bound state has a specific entanglement of a Lorentzian anti-correlation in frequency space and two photons are in proximity due to its binding nature.Such signatures of a photonic molecule illuminates a potential tool that increases the two-photon microscopy efficiency to orders of magnitude higher. Here we numerically and analytically demonstrate the two-photon excitation efficiency between photonic molecules, long uncorrelated light pulses and ultrashort light pulses. The high excitation efficiency of a photonic molecule enables a saturation of fluorophores, such that the linear dependence of two-photon excitation crosssection does not necessarily hold. Also, we exhibits two possible methods to obtain the photonic molecules, as a fundamental possibility for a continuous photonic molecule source.

DOI
10.1117/12.2323624

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Photonic Molecule, also called Photonic Dimer, is a quantum bound state of two photons. A photonic bound state has a specific entanglement of a Lorentzian anti-correlation in frequency space and two photons are in proximity due to its binding nature.Such signatures of a photonic molecule illuminates a potential tool that increases the two-photon microscopy efficiency to orders of magnitude higher. Here we numerically and analytically demonstrate the two-photon excitation efficiency between photonic molecules, long uncorrelated light pulses and ultrashort light pulses. The high excitation efficiency of a photonic molecule enables a saturation of fluorophores, such that the linear dependence of two-photon excitation crosssection does not necessarily hold. Also, we exhibits two possible methods to obtain the photonic molecules, as a fundamental possibility for a continuous photonic molecule source.
In this Letter, we show that photonic dimers, the quantum mechanical bound states of two photons, enable efficient nonlinear two-photon excitation, primarily due to the Lorentzian energy anti-correlation and to the temporal proximity between the constituent photons. We analytically and numerically demonstrate the order-of-magnitude improvement of the excitation efficiency per photon by the photonic dimers over the ultrashort pulses from a laser. We further show that, owing to the high excitation efficiency, the two-photon transition rate by photonic dimers deviates from the well-known linear intensity dependence at low intensities. Possible approaches for generating the photonic dimers in semiconductor platforms are also investigated.
In recent years, the study of quantum electrodynamics (QED) in light-matter interactions has discovered various interesting phenomenons that orient many applications. However, due to the ambient entanglement among photons and atoms, few-particle dynamics remains challenging to analyze precisely and limits the progress in several fields. In few-particle systems, different number of atoms interacting with the light field generates drastically different results, even when there is only a single photon involved in the system. The interference between individual atom’s spontaneous emission wavefunctions can cooperatively alter the effective atom-light coupling strength. Depending on the spatial distance between individual of atoms and the involved cavities in the interaction progresses, the collective spontaneous emission rate can alter drastically from superradiance, where the emission rate is enhanced to a high value proportional to the atom number, to subradiance, where the excited atom ensemble stays in a dark state with the light trapped forever. Superradiance provides a promising mechanism to create an ultra-strong light-matter coupling environment, which is an important ingredient for the design of ultra-fast optical devices, frequency comb generation and quantum mirrors. The dark state of subradiance, on the other hand, is essential for the quantum memory implementation. Also, nontrivial phenomenons also occur when multiple photons interacting with a single atom simultaneously. When a finite number of photons incidents on an atom, their scattering through an atom is highly nonlinear, and one special eigenstate component of such nonlinear process, namely photonic bound states, exhibits many interesting properties in nonlinear quantum optical systems. The photons in such state are strongly bunched with each other, as if a virtual attractive force is in effect. Also, the frequency of photons are anti-correlated so that their total frequency remains a constant value, no matter how arbitrary the frequency of any individual is. Thesefeatures benefit certain nonlinear quantum processes for quantum computing and quantum imaging. Specially for two-photon excitation imaging, the same-parity two-level fluorophore molecules suffers from extremely low excitation efficiencies due to the far off-resonant intermediate states. However, by replacing the current commonly used ultrashort laser pulse illuminations with two photon bound state photon pairs, namely photonic dimers, the efficiency can be enhanced to orders of magnitude higher. Such exceptionally high excitation efficiency can potentially bring the current in vivo deep brain imaging depth from millimeter level to several centimeters. To obtain a stable source of such photonic dimers, it is found that a laser structure with gain medium of two-photon emission materials is capable of generating the coherent state of photonic dimer and can serve as a promising light source for nonlinear quantum optical devices.
Quantum entanglement has been shown to imply correlations stronger than those allowed by classical models. The possibility of performing tasks that are classically impossible has made quantum entanglement a powerful resource for the development of novel methods and applications in various fields of research such as quantum computing, quantum cryptography, and quantum metrology. There is a great need for the development of next generation instrumentation and technologies utilizing entangled quantum light. Among the many applications of nonclassical states of light, nonlinear microscopy has the potential to make an impact in broad areas of science from physics to biology. Here, the microscopic image created by the fluorescence selectively excited by the process of the entangled two-photon absorption is reported. Entangled two-photon microscopy offers nonlinear imaging capabilities at an unprecedented low excitation intensity 10 7, which is 6 orders of magnitude lower than the excitation level for the classical two-photon image. The nonmonotonic dependence of the image on the femtosecond delay between the components of the entangled photon pair is demonstrated. This delay dependence is a result of specific quantum interference effects associated with the entanglement and this is not observable with classical excitation light. In combination with novel spectroscopic capabilities provided by a nonclassical light excitation, this is of critical importance for sensing and biological applications.
We theoretically investigate strongly enhanced vibrational-mode-selective two-step excitation by ultrabroadband frequency-entangled photons. A diatomic molecule having three sets of vibronic states is used to evaluate the excitation efficiency of the two-step excitation. We show that the photon entanglement has little influence on the populations of intermediate vibrational modes of intermediate states but selectively increases the population of a single vibrational mode of excited states, resonant with the total energy of the entangled photons. For an ultrashort pulse close to a monocycle with high degree of entanglement, the population of the vibrational mode is enhanced 2500 times more than by uncorrelated photons, and the selectivity nearly reaches unity. Our results indicate that the two-step excitation with ultrabroadband frequency-entangled photons can achieve highly selective and strongly enhanced excitation of a single vibrational mode.
We study in this paper the efficiency of different two-photon states of light to induce the simultaneous excitation of two atoms of different kinds when the sum of the energies of the two photons matches the sum of the energies of the two atomic transitions, while no photons are resonant with each individual transition. We find that entangled two-photon states produced by an atomic cascade are indeed capable of enhancing by a large factor the simultaneous excitation probability as compared to uncorrelated photons, as predicted some years ago by Muthukrishnan et al, but that several non-entangled, separable, correlated states, produced either by an atomic cascade or parametric down conversion, or even appropriate combinations of coher- ent states, have comparable efficiencies. We show that the key ingredient for the increase of simultaneous excitation probability is the presence of strong frequency anti-correlation and not time correlation nor time-frequency entanglement.