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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Oriented semiconducting polymer nanostructures: photon statistics and far-field dipole interactions

Pradeep Kumar, Adosh Mehta, Predrag Krstić, Michael D. Barnes

Published Apr 4, 2005• 0 citations
Publisher

Abstract

We summarize recent experiments probing photon statistics and collective interactions amongst individual z-oriented semiconducting polymer nanostructures. We show that oriented nanostructures from single molecules of a conducting polymer act as highly robust room-temperature single-photon sources. These results suggest the feasibility of an inexpensive "push-button" technology for polymer-based single-photon sources in photonic-based quantum information processing applications. In addition, fluorescence lifetime measurements on pairs of uniformly z-oriented polymer nanostructures that reveal far-field coherent coupling persisting on a distance scale of several optical wavelengths. Farfield photonic coupling between pairs of oriented luminescent polymer nanostructures is manifested by an oscillatory modulation in the fluorescence decay rate as a function of interparticle distance (both enhancement and inhibition of spontaneous luminescence relative to isolated particles), that results from modification of the vacuum field at the position of the probe dipole by the presence of the second radiating dipole.

DOI
10.1117/12.597143

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We summarize recent experiments probing photon statistics and collective interactions amongst individual z-oriented semiconducting polymer nanostructures. We show that oriented nanostructures from single molecules of a conducting polymer act as highly robust room-temperature single-photon sources. These results suggest the feasibility of an inexpensive "push-button" technology for polymer-based single-photon sources in photonic-based quantum information processing applications. In addition, fluorescence lifetime measurements on pairs of uniformly z-oriented polymer nanostructures that reveal far-field coherent coupling persisting on a distance scale of several optical wavelengths. Farfield photonic coupling between pairs of oriented luminescent polymer nanostructures is manifested by an oscillatory modulation in the fluorescence decay rate as a function of interparticle distance (both enhancement and inhibition of spontaneous luminescence relative to isolated particles), that results from modification of the vacuum field at the position of the probe dipole by the presence of the second radiating dipole.
We have developed a theory for the one-photon and two-photon fluorescence of a nanohybrid composite comprised of an ensemble of quantum dots encased in a matrix of polymer. The quantum dots are comprised of four-level quantum emitters encased within a coating of dielectric material. The fluorescence of the quantum dot system is calculated using the master equation method where dipole–dipole interaction (DDI) coupling is present. The application of a probe field to the nanohybrid composite material in conjunction with the DDI between the quantum dots generates an enhancement of both the single-photon and double-photon fluorescence, and in certain conditions causes spectrum splitting. With a strong DDI field, the two-photon emission spectrum experiences slight quenching and shifts from one peak to two peaks. The dressed states are a result of strong coupling effects between the DDI field and the quantum dots. We generated an analytical expression for the fluorescence spectrum and intensity, and quantitatively compared it to experimental data in which ZnSe quantum dots were embedded within a P3HT polymer film, with our theory strongly correlating with the experiment. We also quantitatively compared our theory with experimental data that demonstrated the single-photon emission spectrum of colloidal quantum dots comprised of a CdZnS/ZnS gradient structure in varying probe field strengths. We found that our theory predicted the spectrum peak splitting that the experiment produced.
High Resolution Image Download MS PowerPoint Slide Single photon sources are fundamental for applications in quantum computing, secure communication, and sensing, as they enable the generation of individual photons and ensure strict control over photon number statistics. However, current single photon sources can be limited by a lack of robustness, difficulty of integration into existing optical or electronic devices, and high cost. In this study, we present the use of off-the-shelf C 60 fullerene molecules embedded in polystyrene as room-temperature reliable single-photon emitters. As our results demonstrate, these molecules exhibit on-demand single-photon emission, with short fluorescence lifetimes and, consequently, high emission rates. The wide availability and ease of preparation and manipulation of fullerenes as single photon sources can pave the way for the development of practical, economic and scalable quantum photonic technologies.
The resonance fluorescence of a two-level single molecular system interacting with a plasmonic nanostructure is investigated. Specific regions of space are identified, where a balance exists between the near-field enhancement and the modification of the decay rate, such that the fluorescence spectrum of the molecule exhibits the Mollow triplet and the emission photons are antibunched. The utilization of such quantum phenomena at the vicinity of custom-designed plasmonic nanostructures paves the way for applications in nanoscale quantum devices and quantum information processing.
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