In nanomaterials, optical anisotropies reveal a fundamental relationship between structural and optical properties. Directional optical properties can be exploited to enhance the performance of optoelectronic devices, optomechanical actuators and metamaterials. In layered materials, optical anisotropies may result from in-plane and out-of-plane dipoles associated with intra- and interlayer excitations, respectively. Here, we resolve the orientation of luminescent excitons and isolate photoluminescence signatures arising from distinct intra- and interlayer optical transitions. Combining analytical calculations with energy- and momentum-resolved spectroscopy, we distinguish between in-plane and out-of-plane oriented excitons in materials with weak or strong interlayer coupling-MoS₂ and 3,4,9,10-perylene tetracarboxylic dianhydride (PTCDA), respectively. We demonstrate that photoluminescence from MoS₂ mono-, bi- and trilayers originates solely from in-plane excitons, whereas PTCDA supports distinct in-plane and out-of-plane exciton species with different spectra, dipole strengths and temporal dynamics. The insights provided by this work are important for understanding fundamental excitonic properties in nanomaterials and designing optical systems that efficiently excite and collect light from exciton species with different orientations.
Tremendous advances in the study of magnetic light-matter interactions have recently been achieved using man-made nanostructures that exhibit and exploit an optical magnetic response. However, naturally occurring emitters can also exhibit magnetic resonances in the form of optical-frequency magnetic-dipole transitions. Here we quantify the magnetic nature of light emission using energy-and momentum-resolved spectroscopy, and leverage a pair of spectrally close electric-and magnetic-dipole transitions in trivalent europium to probe vacuum fluctuations in the electric and magnetic fields at the nanometre scale. These results reveal a new tool for nano-optics: an atomic-size quantum emitter that interacts with the magnetic component of light.
We demonstrate that magnetic dipole transitions provide an additional degree of freedom for engineering emission spectra. Without the need for a high-quality optical cavity, we show how a simple gold mirror can strongly tune the emission of trivalent europium. We exploit the differing field symmetries of electric and magnetic dipoles to selectively direct the majority of emission through each of three major transitions (centered at 590, 620, and 700 nm), and present a model that accurately predicts this tuning from the local electric and magnetic density of optical states.
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