Strongly inhibited spontaneous emission of PbS quantum dots covalently bound to 3D silicon photonic band gap crystals

Andreas Stefan Schulz, Marek Kozon, Julius Vancso, J. Huskens, Willem L. Vos*

*Corresponding author for this work

Research output: Working paperPreprintAcademic

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Abstract

We present an optical study of the spontaneous emission of lead sulfide (PbS) nanocrystal quantum dots in three-dimensional (3D) photonic band gap crystals made from silicon. The nanocrystals emit in the near-infrared (NIR) range to be compatible with the 3D silicon nanophotonics. The nanocrystals are covalently bonded to polymer brush layers that are grafted from the Si-air interfaces inside the nanostructure using surface-initiated atom transfer radical polymerization (SI-ATRP), and their presence and position of the quantum dots was previously characterized by synchrotron X-ray fluorescence tomography. We report both continuous wave (cw) emission spectra and time-resolved time-correlated single photon counting. In time-resolved measurements, we observe that the total emission rate greatly increases when the quantum dots are transferred from suspension to the silicon nanostructures, likely due to quenching (or increased non-radiative decay) that is tentatively attributed to the presence of Cu-catalyst during the synthesis. In this regime, continuous wave emission spectra are known to be proportional to the radiative rate and thus to the local density of states. In spectra normalized to those taken on flat silicon outside the crystals, we observe a broad and deep stop band that we attribute to a 3D photonic band gap with a relative bandwidth up to 26%. The shapes of the relative emission spectra match well with the theoretical density of states spectra calculated with the plane wave expansion. The observed inhibition is 5 to 30 times, similar to previously reported record inhibitions, yet for completely coincidental reasons. Our results are relevant to applications in photochemistry, sensing, photovoltaics, and to efficient miniature light sources.
Original languageEnglish
PublisherChemRxiv
DOIs
Publication statusPublished - 20 Oct 2023

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