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Bulletin of the American Physical Society

Single Photon Source Using Chiral Nematic Liquid Crystal

S. Ganesh, Anand K. Jha, Pavel Lougovski, Marian Florescu A, Robert W. Boyd, Jonathan P. Dowling

Published Mar 16, 2006• 0 citations
OpenAlex

Abstract

With the development of Linear Optics Quantum Computing, a demand for a good single photon source has increased. Here we describe how a cholesteric liquid crystal can be used as a photonic band-gap material to design a single-photon source.We have a dipole embedded in a liquid crystal for which we find the spontaneous emission rate. We calculate the band structureof the cholesteric liquid crystal using the eigenfuncton expansion method and ultimately compute the density of modes. We also determine the field of the dipole embedded inside the cholesteric liquid crystal using the Green's function method from which we determine the spontaneous emmission rate.

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With the development of Linear Optics Quantum Computing, a demand for a good single photon source has increased. Here we describe how a cholesteric liquid crystal can be used as a photonic band-gap material to design a single-photon source.We have a dipole embedded in a liquid crystal for which we find the spontaneous emission rate. We calculate the band structureof the cholesteric liquid crystal using the eigenfuncton expansion method and ultimately compute the density of modes. We also determine the field of the dipole embedded inside the cholesteric liquid crystal using the Green's function method from which we determine the spontaneous emmission rate.
We report on new approaches toward an implementation of an efficient, room temperature, deterministically polarized, single-photon source (SPS) on demand-a key hardware element for quantum information and quantum communication. Operation of a room temperature SPS is demonstrated via photon antibunching in the fluorescence from single terrylene-dye molecules embedded in a cholesteric liquid crystal host. Using oxygen-depleted liquid crystal hosts, dye-bleaching was avoided over the course of more than 1 h of continuous 532-nm excitation. Liquid crystal hosts (including liquid crystal oligomers/polymers) permit further increase of the efficiency of the source: 1) by aligning the dye molecules along a direction preferable for maximum excitation efficiency; 2) by tuning a one-dimensional (1-D) photonic-band-gap microcavity of planar-aligned cholesteric (chiral nematic) liquid crystal layer to the dye fluorescence band.
In this article, we investigate the spontaneous emission properties of radiating molecules embedded in a chiral nematic liquid crystal, under the assumption that the electronic transition frequency is close to the photonic edge mode of the structure, i.e., at resonance. We take into account the transition broadening and the decay of electromagnetic field modes supported by the so-called "mirrorless"cavity. We employ the Jaynes-Cummings Hamiltonian to describe the electron interaction with the electromagnetic field, focusing on the mode with the diffracting polarization in the chiral nematic layer. As known in these structures, the density of photon states, calculated via the Wigner method, has distinct peaks on either side of the photonic band gap, which manifests itself as a considerable modification of the emission spectrum. We demonstrate that, near resonance, there are notable differences between the behavior of the density of states and the spontaneous emission profile of these structures. In addition, we examine in some detail the case of the logarithmic peak exhibited in the density of states in two-dimensional photonic structures and obtain analytic relations for the Lamb shift and the broadening of the atomic transition in the emission spectrum. The dynamical behavior of the atom-field system is described by a system of two first-order differential equations, solved using the Green's-function method and the Fourier transform. The emission spectra are then calculated and compared with experimental data.
This paper describes a new application for liquid crystals: quantum information technology. A deterministically polarized single-photon source that efficiently produces photons exhibiting antibunching is a pivotal hardware element in absolutely secure quantum communication. Planar-aligned nematic liquid crystal hosts deterministically align the single dye molecules which produce deterministically polarized single (antibunched) photons. In addition, 1-D photonic bandgap cholesteric liquid crystals will increase single-photon source efficiency. The experiments and challenges in the observation of deterministically polarized fluorescence from single dye molecules in planar-aligned glassy nematic-liquid-crystal oligomer as well as photon antibunching in glassy cholesteric oligomer are described for the first time.
Abstract Liquid crystals, with their ability to self-assemble, strong response to an electric field and integrability into complex systems, are key materials in light-beam manipulation 1 . The recently discovered ferroelectric nematic liquid crystals 2,3 also have considerable second-order optical nonlinearity, making them a potential material for nonlinear optics 4,5 . Their use as sources of quantum light could considerably extend the boundaries of photonic quantum technologies 6 . However, spontaneous parametric down-conversion, the basic source of entangled photons 7 , heralded single photons 8 and squeezed light 9 , has so far not been observed in liquid crystals—or in any liquids or organic materials. Here we implement spontaneous parametric down-conversion in a ferroelectric nematic liquid crystal and demonstrate electric-field tunable broadband generation of entangled photons, with an efficiency comparable to that of the best nonlinear crystals. The emission rate and polarization state of photon pairs is markedly varied by applying a few volts or twisting the molecular orientation along the sample. A liquid-crystal source enables a special type of quasi-phase matching 10 , which is based on the molecular twist structure and is therefore reconfigurable for the desired spectral and polarization properties of photon pairs. Such sources promise to outperform standard nonlinear optical materials in terms of functionality, brightness and the tunability of the generated quantum state. The concepts developed here can be extended to complex topological structures, macroscopic devices and multi-pixel tunable quantum light sources.
Definite circular and linear polarizations of room-temperature single-photon sources, which can serve as polarization bases for quantum key distribution, are produced by doping planar-aligned liquid crystal hosts with single fluorescence emitters. Chiral 1-D photonic bandgap microcavities for a single handedness of circularly polarized light were prepared from both monomeric and oligomeric cholesteric liquid crystals. Fluorescent emitters, such as nanocrystal quantum dots, nitrogen vacancy color centers in nanodiamonds, and rare-earth ions in nanocrystals, were doped into these microcavity structures and used to produce circularly polarized fluorescence of definite handedness. Additionally, we observed circularly polarized resonances in the spectrum of nanocrystal quantum dot fluorescence at the edge of the cholesteric microcavity's photonic stopband. For this polarization we obtained a ~4.9 enhancement of intensity compared to the polarization of the opposite handedness that propagates without photonic bandgap microcavity effects. Such a resonance is indicative of coupling of quantum dot fluorescence to the cholesteric microcavity mode. We have also used planar-aligned nematic liquid crystal hosts to align DiI dye molecules doped into the host, thereby providing a single-photon source of linear polarization of definite direction. Antibunching is demonstrated for fluorescence of nanocrystal quantum dots, nitrogen vacancy color centers, and dye molecules in these liquid crystal structures.