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Optica

Polarization-entangled photon pairs from a single molecule

Mohammad Rezai, Jörg Wrachtrup, Ilja Gerhardt

Published Jan 3, 2019• 34 citations
Publisher

Abstract

Photonic entanglement is one of the key resources in modern quantum optics. It opens the door to schemes such as quantum communication, quantum teleportation, and quantum-enhanced precision sensing. Sources based on parametric down-conversion or cascaded decays in atomic and atom-like emitters are limited because of their weak interaction with stationary qubits. This is due to their commonly broadband emission. Furthermore, these sources are commonly in the near-infrared such that quantum emitters in the blue spectral region, such as ions or many defect centers, cannot be addressed. Here, we present a sodium-resonant (589.0 nm) and narrow-band (14 MHz) degenerate entanglement source based on a single molecule. A beam-splitter renders two independently emitted photons into a polarization-entangled state. The quality of the entangled photon pairs is verified by the violation of Bell’s inequality. We measure a Bell parameter of S=2.26±0.05. This attests that the detected photon pairs exceed the classical limit; it is reconfirmed by quantum-state tomography and an analysis of the raw detector counts, which result in a value of S=2.24±0.12. The tomography shows fidelity of 82% to a maximally entangled Bell state. This work opens the route to background-free solid-state entanglement sources which surpass the probabilistic nature of the commonly used sources and are free from unwanted multi-photon events. The source is ideal for combination with stationary qubits such as atoms, ions, quantum dots, or defect centers.

DOI
10.1364/optica.6.000034

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Photonic entanglement is one of the key resources in modern quantum optics. It opens the door to schemes such as quantum communication, quantum teleportation, and quantum-enhanced precision sensing. Sources based on parametric down-conversion or cascaded decays in atomic and atom-like emitters are limited because of their weak interaction with stationary qubits. This is due to their commonly broadband emission. Furthermore, these sources are commonly in the near-infrared such that quantum emitters in the blue spectral region, such as ions or many defect centers, cannot be addressed. Here, we present a sodium-resonant (589.0 nm) and narrow-band (14 MHz) degenerate entanglement source based on a single molecule. A beam-splitter renders two independently emitted photons into a polarization-entangled state. The quality of the entangled photon pairs is verified by the violation of Bell’s inequality. We measure a Bell parameter of S=2.26±0.05. This attests that the detected photon pairs exceed the classical limit; it is reconfirmed by quantum-state tomography and an analysis of the raw detector counts, which result in a value of S=2.24±0.12. The tomography shows fidelity of 82% to a maximally entangled Bell state. This work opens the route to background-free solid-state entanglement sources which surpass the probabilistic nature of the commonly used sources and are free from unwanted multi-photon events. The source is ideal for combination with stationary qubits such as atoms, ions, quantum dots, or defect centers.
Single organic dye molecules have been studied for almost three decades. A majority of experiments are now conducted under ambient conditions and aim towards material science and micro-biology. The experiments under cryogenic conditions are often based on highly rigid polycyclic hydrocarbons, which have excellent fluorescing properties when they are operated at temperatures below 2 K. Their photonic advantages integrate their high flux, their narrow-band nature and their tunability over the entire visible spectrum. Therefore the use of organic molecules as efficient and narrow-band single photon sources facilitated a number of quantum optical advances in the past years. The results mostly cover quantum sensing, the formation of quantum hybrid systems and the optical combination of multiple photons in all-optical experiments. Here we present all three fields and outline our own experiments in the combination of single molecule studies, atomic spectroscopy and entanglement generation. The brightness and the narrow-band nature of the molecules are outlined and a delayed-choice quantum eraser is presented. The mode-mixing of two photons on a beam-splitter allows for the generation of a degenerate photon pair, which is resonant to the sodium D2-line. Furthermore, its spectral width matches roughly to the natural linewidth of an isolated sodium atom, such that further experiments are feasible. The entanglement of the post-selected photon pair is testified by a violation of Bell's inequality. Even the raw collected clicks violate Bell's inequality by more than two standard deviations.
The hybrid quantum network, a universal form of quantum network which is aimed for quantum communication and distributed quantum computation, is that the quantum nodes in it are realized with different physical systems. This universal form of quantum network can combine the advantages and avoid the inherent defects of the different physical system. However, one obstacle standing in the way is the compatible photonic quantum interface. One possible solution is using non-degenerate, narrow-band, entangled photon pairs as the photonic interface. Here, for the first time, we generate nondegenrate narrow-band polarization-entangled photon pairs in cavity-enhanced spontaneous parametric down-conversion process. The bandwidths and central wavelengths of the signal and idler photons are 9 MHz at 935 nm and 9.5 MHz at 880 nm, which are compatible with trapped ion system and solid-state quantum memory system. The entanglement of the photon source is certified by quantum state tomography, showing a fidelity of 89.6% between the generated quantum state with a Bell state. Besides, a strong violation against Bell inequality with 2.36+/-0.03 further confirms the entanglement property of the photon pairs. Our method is suitable for the hybrid quantum network and will take a big step in this field.
Using the process of cavity-enhanced spontaneous parametric down-conversion (SPDC), we generate a narrow-band polarization-entangled photon pair resonant on the rubidium (Rb) D1 line (795 nm). The degenerate single-mode photon pair is selected by multiple temperature controlled etalons. The linewidth of generated polarization-entangled photon pairs is 15 MHz which matches the typical atomic memory bandwidth. The measured Bell parameter for the polarization-entangled photons S=2.73+-0.04 which violates the Bell-CHSH inequality by ~18 standard deviations. The presented entangled photon pair source could be utilized in quantum communication and quantum computing based on quantum memories in atomic ensemble.
Bell states are fundamental resources in quantum optics, underpinning a range of applications in quantum computation and communication. However, many experimental sources focus on generating a single Bell state, limiting their utility for protocols that require the full set of maximally entangled states. In this work, we present a polarization-entangled photon-pair source based on spontaneous parametric down-conversion in a periodically poled potassium titanyl phosphate crystal integrated into a Sagnac loop interferometer. Our source initially generates one Bell state, which is then transformed into the complete set of Bell states through the application of phase and bit flips using phase plates. We characterize the entanglement quality of all generated states via two-photon interference measurements, quantum state tomography, and evaluation of the Bell parameter. Our results show spectral brightness of 0.15 kHz/mW/nm with interference visibilities of ∼98% (H/V basis) and ∼96% (A/D basis) and state fidelity of ∼0.97 across all Bell states, with all states demonstrating a clear violation of the Clauser–Horne–Shimony–Holt inequality (S≥2.6). This approach offers a practical solution for obtaining all four Bell states with high efficiency from a single source, which could facilitate more versatile implementations in quantum information processing.
The first two-photon entanglement experiment performed 50 years ago by Kocher and Commins (KC) provided isolated pairs of entangled photons from an atomic three-state fluorescence cascade. In view of questioning of Bell’s theorem, data from these experiments are re-analyzed and shown sufficiently precise to confirm quantum mechanical and dismiss semi-classical theory without need for Bell’s inequalities. Polarization photon correlation anisotropy (A) is useful: A is near unity as predicted quantum mechanically and well above the semi-classic range, 0⩽A⩽1/2. Although yet to be found, one may envisage a three-state molecule emitting entangled photon pairs, in analogy with the KC atomic system. Antibunching in fluorescence from single molecules in matrix and entangled photons from quantum dots promise it be possible. Molecules can have advantages to parametric down-conversion as the latter photon distribution is Poissonian and unsuitable for producing isolated pairs of entangled photons. Analytical molecular applications of entangled light are also envisaged.
We report the generation of polarization-entangled photons, using a quantum dot single photon source, linear optics, and photodetectors. Two photons created independently are observed to violate Bell's inequality. The density matrix describing the polarization state of the postselected photon pairs is reconstructed and agrees well with a simple model predicting the quality of entanglement from the known parameters of the single photon source. Our scheme provides a method to create no more than one entangled photon pair per cycle after postselection, a feature useful to enhance quantum cryptography protocols based on shared entanglement.