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Molecular Crystals and Liquid Crystals

Single-Photon Source for Quantum Information Based on Single Dye Molecule Fluorescence in Liquid Crystal Host

Svetlana G. Lukishova, Russell P. Knox, Patrick Freivald, Andrew J. McNamara, Robert W. Boyd, Carlos R. Stroud, Ansgar W. Schmid, Kenneth Lee Marshall

Published Jun 27, 2006• 17 citations
Publisher

Abstract

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.

DOI
10.1080/15421400600653977

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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.
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.
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.
A definite polarization in fluorescence from single emitters (dye molecules) at room temperature is demonstrated. A planar-aligned, nematic liquid-crystal host provides definite alignment of single dye molecules in a preferred direction. Well-defined polarized fluorescence from single emitters (single photon source) is important for applications in photonic quantum information. Polarized single-photon sources based on single emitters, for example, are key hardware elements both for absolutely secure quantum communication and quantum computation systems.
We present here our results on using liquid crystals (LCs) in experiments with nonclassical light sources: (1) single-photon sources exhibiting antibunching (separation of all photons in time), which are key components for secure quantum communication systems and (2) entangled photon source with photons exhibiting quantum interference in a Hong–Ou–Mandel interferometer. In the first part, both nematic and cholesteric liquid crystal (CLC) hosts were used to create definite linear or circular polarization of antibunched photons emitted by different types of single emitters (dye molecules, nanocrystal quantum dots (NQDs), nanodiamonds with color centers, etc.). If the photon has unknown polarization, filtering it through a polarizer to produce the desired polarization for quantum key distribution with bits based on polarization states of photons will reduce by half the efficiency of a quantum cryptography system. In the first part, we also provide our results on observation of a circular polarized microcavity resonance in NQD fluorescence in a 1-D chiral photonic bandgap CLC microcavity. In the second part of this paper with indistinguishable, time-entangled photons, we demonstrate our experimental results on simulating quantum mechanical barrier tunneling phenomena. A Hong–Ou–Mandel dip (quantum interference effect) is shifted when a phase change was introduced on the way of one of entangled photons in pair (one arm of the interferometer) by inserting in this arm an electrically controlled planar-aligned nematic LC layer between two prisms in the conditions close to a frustrated total internal reflection. By applying different AC-voltages to the planar-aligned nematic layer and changing its refractive index, we can obtain various conditions for incident photon propagation – from total reflection to total transmission. Measuring changes of tunneling times of photon through this structure with femtosecond resolution permitted us to answer some unresolved questions in quantum mechanical barrier tunneling phenomena.