Design and implementation of a device based on an off-axis parabolic mirror to perform luminescence experiments in a scanning tunneling microscope.

We present the design, implementation, and illustrative results of a light collection/injection strategy based on an off-axis parabolic mirror collector for a low-temperature Scanning Tunneling Microscope (STM). This device allows us to perform STM induced Light Emission (STM-LE) and Cathodoluminescence (STM-CL) experiments and in situ Photoluminescence (PL) and Raman spectroscopy as complementary techniques. Considering the Étendue conservation and using an off-axis parabolic mirror, it is possible to design a light collection and injection system that displays 72% of collection efficiency (considering the hemisphere above the sample surface) while maintaining high spectral resolution and minimizing signal loss. The performance of the STM is tested by atomically resolved images and scanning tunneling spectroscopy results on standard sample surfaces. The capabilities of our system are demonstrated by performing STM-LE on metallic surfaces and two-dimensional semiconducting samples, observing both plasmonic and excitonic emissions. In addition, we carried out in situ PL measurements on semiconducting monolayers and quantum dots and in situ Raman on graphite and hexagonal boron nitride (h-BN) samples. Additionally, STM-CL and PL were obtained on monolayer h-BN gathering luminescence spectra that are typically associated with intragap states related to carbon defects. The results show that the flexible and efficient light injection and collection device based on an off-axis parabolic mirror is a powerful tool to study several types of nanostructures with multiple spectroscopic techniques in correlation with their morphology at the atomic scale and electronic structure.

Tunneling-current-induced local excitonic luminescence in p-doped WSe2 monolayers.

We have studied the excitonic properties of exfoliated tungsten diselenide (WSe2) monolayers transferred to gold substrates using the tunneling current in a Scanning Tunneling Microscope (STM) operated in air to excite the light emission locally. In obtained spectra, emission energies are independent of the applied bias voltage and resemble photoluminescence (PL) results, indicating that, in both cases, the light emission is due to neutral and charged exciton recombination. Interestingly, the electron injection rate, that is, the tunneling current, can be used to control the ratio of charged to neutral exciton emission. The obtained quantum yield in the transition metal dichalcogenide (TMD) is ∼5 × 10-7 photons per electron. The proposed excitation mechanism is the direct injection of carriers into the conduction band. The monolayer WSe2 presents bright and dark defects spotted by STM images performed under UHV. STS confirms the sample as p-doped, possibly as a net result of the observed defects. The presence of an interfacial water layer decouples the monolayer from the gold support and allows excitonic emission from the WSe2 monolayer. The creation of a water layer is an inherent feature of the sample transferring process due to the ubiquitous air moisture. Consequently, vacuum thermal annealing, which removes the water layer, quenches excitonic luminescence from the TMD. The tunneling current can locally displace water molecules leading to excitonic emission quenching and to plasmonic emission due to the gold substrate. The present findings extend the use and the understanding of STM induced light emission (STM-LE) on semiconducting TMDs to probe exciton emission and dynamics with high spatial resolution.