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Deterministicall y polarized fluorescence from single dyemolecules aligned inliquid crystal host

Russell P. Knox, Patrick Freivald

Published Jan 1, 2005• 0 citations
OpenAlex

Abstract

We demonstrated forthefirst timetoourknowledge deterministically polarized fluorescence fromsingle dyemolecules. Planar aligned nematic liquid crystal hosts provide deterministic alignment of single dyemolecules inapreferred direction. ©2003 Optical Society ofAmerica OCIScodes: (180.1790) Confocal microscopy; (180.2520) Fluorescence microscopy. Determninistically polarized fluorescence ofsingle emitters isimportant forapplications inphotonic quantum information. Forinstance, deterministically

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We demonstrated forthefirst timetoourknowledge deterministically polarized fluorescence fromsingle dyemolecules. Planar aligned nematic liquid crystal hosts provide deterministic alignment of single dyemolecules inapreferred direction. ©2003 Optical Society ofAmerica OCIScodes: (180.1790) Confocal microscopy; (180.2520) Fluorescence microscopy. Determninistically polarized fluorescence ofsingle emitters isimportant forapplications inphotonic quantum information. Forinstance, deterministically
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.
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.
An efficient technique for producing deterministically polarized single photons uses liquid-crystal hosts of either monomeric or oligomeric/polymeric form to preferentially align the single emitters for maximum excitation efficiency. Deterministic molecular alignment also provides deterministically polarized output photons; using planar-aligned cholesteric liquid crystal hosts as 1-D photonic-band-gap microcavities tunable to the emitter fluorescence band to increase source efficiency, using liquid crystal technology to prevent emitter bleaching. Emitters comprise soluble dyes, inorganic nanocrystals or trivalent rare-earth chelates.
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.