Abstract
The coupling of HgTe quantum dots to a gold nanobump plasmonic array can enhance the spontaneous infrared emission by a factor of five and reduce the influence of nonradiative decay channels.
The demand for efficient, room-temperature shortwavelength infrared (SWIR) emitters is increasing since they can find important applications in night vision, healthcare, spectroscopy, and light detection and ranging (LIDAR) systems1. Despite their tremendous technical importance, there are still challenges associated with the material synthesis and light emission efficiency. First, there are very limited material choices for the fabrication of SWIR light emitters. Although narrow-bandgap III–V compounds can cover this wavelength range2, these materials are usually grown epitaxially on lattice-matched substrates, which is an expensive process2. Second, the narrow bandgap makes the spontaneous light emission process inefficient—the excited electrons are susceptible to nonradiative transitions such as defect and infrared phonon scattering, thus compromising the spontaneous light emission efficiency2,3.
Quantum dots (QDs) provide an alternative avenue for the realization of tunable narrow-bandgap materials. Due to strong quantum confinement, QDs can exhibit a larger bandgap than their bulk counterparts4 (see Fig. 1a). By controlling their physical sizes, tunable emission at infrared wavelengths can be realized in mercury telluride (HgTe) QDs, which is a semimetal in its bulk form5. In addition, the spontaneous emission rate is not necessarily a fixed material property but can also be controlled by its local electromagnetic environment6,7. The modification of the spontaneous emission of emitters by engineering the electromagnetic environment was originally proposed by Purcell in 19468 and was first experimentally demonstrated by Drexhage in 19709. In a recent publication, A. A. Sergeev and coworkers leveraged nanobump plasmonic resonator arrays and significantly enhanced the spontaneous emission of HgTe QDs10. Specifically, a HgTe QD and organic dodecanethiol (DDT) ligand layer was coated on a glass-supported gold plasmonic nanobump-array film, which was fabricated through melt and resolidification induced by a femtosecond laser.
Let us assume that the spontaneous emission rate of an emitter in free space is Γr (Fig. 1a) without surrounding photonic structures. When the emitter is coupled to resonant structures, such as nanobump resonators (Fig. 1b), the emitter can excite resonant modes of the structure at a rate of Γcp. In a judiciously designed resonant structure, Γcp can be much larger than the original Γr due to the greatly enhanced local density of states11. The resonant structure then radiates into free space at a rate of Γr,pl, or the energy can dissipate as heat at a rate of Γh (Fig. 1b). Along with coupling to the resonant structure, the emitter is also directly emitted into free space at a modified rate of \(\varGamma_{\it{r}}^\prime\). Considering all of the factors above, \(\varGamma_{far} = \varGamma_r^\prime + \varGamma_{cp}\varGamma_{r,pl}/\left(\varGamma_{r,pl} + \varGamma_h \right)\) is the overall far-field emission rate6. Therefore, an enhancement in the spontaneous emission (Γfar > Γr) can be observed when the energy is efficiently transferred from the emitter to the resonant structure (high Γcp) and then effectively radiated into free space (high Γr,pl/(Γr,pl + Γh)).
In the work by A. A. Sergeev and coworkers, two types of pyramid-shaped QDs were synthesized with average sizes of 3.9 and 5.0 nm, exhibiting spontaneous emission peaks at 1.6 and 2.2 µm, respectively10. By tuning the periodicity of the nanobumps, the spontaneous emission of QDs matches the first-order resonance wavelength of the plasmonic arrays, giving rise to an emission enhancement factor of five10. The observed photoluminescence (PL) decay rate was also faster than the decay rate of QDs on a smooth silicon substrate without cavities, which confirmed the enhanced radiative rate enabled by the plasmonic nanobump arrays10. Moreover, an average four-fold enhancement of absorption was also achieved because of the strong local field in these plasmonic nanobump arrays10. The integration of HgTe QDs with designed nanophotonic structures offers a new route to on-chip, compact and tunable SWIR light emission devices, which may find various applications in spectroscopy and sensing. As a result, this demonstration represents an important step towards the realization of future on-chip infrared photonic systems.
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Yuan, S., Chen, C., Guo, Q. et al. Enhancing infrared emission of mercury telluride (HgTe) quantum dots by plasmonic structures. Light Sci Appl 9, 37 (2020). https://doi.org/10.1038/s41377-020-0276-1
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DOI: https://doi.org/10.1038/s41377-020-0276-1