Nano-Enabled Single-Photon Sources for Quantum Applications
Jennifer Hollingsworth a
a Center for Integrated Nanotechnologies, Los Alamos National Laboratory, United States
Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe Spring Meeting 2022 (NSM22)
#NANOQ22. Colloidal Semiconductor nanocrystals for Quantum Technologies
Online, Spain, 2022 March 7th - 11th
Organizers: Francesco Di Stasio, Iwan Moreels and Riccardo Sapienza
Invited Speaker, Jennifer Hollingsworth, presentation 130
DOI: https://doi.org/10.29363/nanoge.nsm.2022.130
Publication date: 7th February 2022

Recent and nearly simultaneous developments in the fields of nanocrystal semiconductors, nanoplasmonics and nanophotonics may conspire to address deficiencies of available single-photon sources (SPSs). Namely, SPSs may now be accessible that operate in the telecommunications bands at room temperature, that are bright, and that can be easily integrated into quantum-advantaged communications, networking and sensing technologies. I will discuss our efforts to understand, design and synthesize heterostructured colloidal semiconductor quantum dots (QDs) that can meet the rigorous requirements for single-photons-on-demand in the infrared (IR) and at room-temperature.1-4 In general, QD emitters, especially those that emit in the infrared, are slow to cycle photons. In order to dramatically enhance the rate of spontaneous emission, such emitters can be combined with nanoscale plasmonic materials or antennas. Traditionally, nanoscale noble metals such as gold and silver have been used to achieve the targeted enhancements in light-matter interactions that result from the presence of localized surface plasmons (LSPs). However, interest has recently shifted to intrinsically doped semiconductor nanocrystals (NCs) for their ability to display LSP resonances (LSPRs) over a much broader spectral range, including the IR. Among semiconducting plasmonic NCs, spinel metal oxides (sp-MOs) are an emerging material with distinct advantages in accessing the telecommunications bands in the IR and affording useful environmental stability. Here, I will discuss the plasmonic properties of several sp-MO NCs, known previously only for their magnetic functionality, and demonstrate their ability to modify the light-emission properties of telecom-emitting QDs, achieving Purcell enhancement factors up to ~50-fold for telecom-emitting QDs in simple plasmonic-spacer-emitter sandwich structures or significantly higher radiative rate enhancement aided by more sophisticated plasmonic nanoantenna architectures. Finally, in collaborative work,5 we have demonstrated prospects for on-chip integration and addressing losses in brightness associated with the omnidirectionality of free-standing emitters. In particular, using a scanning-probe method we directly place QDs into hybrid metal-dielectric antenna that cause their photons to emit in a highly focused, directional stream, dramatically enhancing collection efficiency and utility as a SPS. Taken together, these advances in nanomaterial chemistry, nanointegration and hybrid-material design are showing the way to practical utilization of nano-enabled SPSs for quantum applications.

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