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Eric Le Moal

Publications and source records attributed to Eric Le Moal.

6 recordsLinked to original sources

Sub-diffraction-resolved spatial distribution of emitting excitons in STM-induced luminescence of 2D semiconductors via Richardson-Lucy deconvolution

Using scanning tunneling microscopy-induced luminescence (STML), the optical properties of two-dimensional (2D) semiconductors may be investigated at the nanoscale. This is possible because the tunneling current under the tip is an extremely localized electrical excitation source. However, in most STML applications, the spatial distribution of the emission relative to the excitation point is unresolved. Yet this distribution contains key information about how the interaction of excitons with injected charge carriers affects the luminescence of these materials, and about exciton transport. Resolving this spatial distribution at the nanoscale is relevant both for a fundamental understanding of exciton physics and for device applications; yet it remains a significant challenge. In this work, we resolve the spatial distribution of the emission beyond the diffraction limit of light by deconvolving real-space optical microscopy images of the STML using an iterative algorithm, i.e., Richardson-Lucy (RL) deconvolution. To showcase this technique, we apply it to the STML of monolayer tungsten diselenide ($\mathrm{WSe_2}$) and tungsten disulfide ($\mathrm{WS_2}$). Thus, we highlight hitherto ignored or misunderstood aspects of STML on 2D semiconductors related to exciton and charge carrier transport, namely the dependence of the spatial distribution of emission on the tunnel current setpoint and the origin of the emission from hot spots located micrometers from the excitation source.

cond-mat.mes-hall

Fluorescent single-molecule STM probe

The plasmonic tip of a scanning tunnelling microscope (STM) is functionalized with a single fluorescent molecule and is scanned on a plasmonic substrate. The tunneling current flowing through the tip-molecule-substrate junction generates a narrow-line emission of light corresponding to the fluorescence of the negatively charged molecule suspended at the apex of the tip, i.e., the emission of the excited molecular anion (trion). The fluorescence of this molecular probe is recorded for tip-substrate nanocavities featuring different plasmonic resonances, for different tip-substrate distances and applied bias voltages, and on different substrates. We demonstrate that the width of the emission peak can be used as a probe of the trion-plasmon coupling strength and that the energy of the emitted photons is governed by the molecule interactions with its electrostatic environment. Additionally, we theoretically elucidate why the direct contact of the suspended molecule with the metallic tip does not totally quench the radiative emission of the molecule.

cond-mat.mes-hall

Many-body description of STM-induced fluorescence of charged molecules

A scanning tunneling microscope is used to study the fluorescence of a model charged molecule (quinacridone) adsorbed on a sodium chloride (NaCl)-covered metallic sample. Fluorescence from the neutral and positively charged species is reported and imaged using hyper-resolved fluorescence microscopy. A many-body excitation model is established based on a detailed analysis of voltage, current and spatial dependencies of the fluorescence and electron transport features. This model reveals that quinacridone adopts a large palette of charge states, transient or not, depending on the voltage used and the nature of the underlying substrate. This model has a universal character and explains the electronic and fluorescence properties of many other molecules adsorbed on thin insulators.

cond-mat.mes-hall

Electroluminescence of monolayer WS$_2$ in a scanning tunneling microscope: the effect of bias polarity on the spectral and angular distribution of the emitted light

Inelastic electron tunneling in a scanning tunneling microscope (STM) is used to generate excitons in monolayer tungsten disulfide (WS$_2$). Excitonic electroluminescence is measured both at positive and negative sample bias. Using optical spectroscopy and Fourier-space optical microscopy, we show that the bias polarity of the tunnel junction determines the spectral and angular distribution of the emitted light. At positive sample bias, only emission from excitonic species featuring an in-plane transition dipole moment is detected. Based on the spectral distribution of the emitted light, we infer that the dominant contribution is from charged excitons, i.e., trions. At negative sample bias, additional contributions from lower-energy excitonic species are evidenced in the emission spectra and the angular distribution of the emitted light reveals a mixed character of in-plane and out-of-plane transition dipole moments.

cond-mat.mes-hall

Plasmon scattering from holes: from single hole scattering to Young's experiment

In this article, the scattering of surface plasmon polaritons (SPPs) into photons at holes is investigated. A local, electrically excited source of SPPs using a scanning tunnelling microscope (STM) produces an outgoing circular plasmon wave on a thick (200 nm) gold film on glass containing holes of 250, 500 and 1000 nm diameter. Fourier plane images of the photons from hole-scattered plasmons show that the larger the hole diameter, the more directional the scattered radiation. These results are confirmed by a model where the hole is considered as a distribution of horizontal dipoles whose relative amplitudes, directions, and phases depend linearly on the local SPP electric field. An SPP-Young's experiment is also performed, where the STM-excited SPP-wave is incident on a pair of 1 $μ$m diameter holes in the thick gold film. The visibility of the resulting fringes in the Fourier plane is analyzed to show that the polarization of the electric field is maintained when SPPs scatter into photons. From this SPP-Young's experiment, an upper bound of $\approx$ 200 nm for the radius of this STM-excited source of surface plasmon polaritons is determined.

physics.optics

Nanoroughened plasmonic films for enhanced biosensing detection

Although fluorescence is the prevailing labeling technique in biosensing applications, sensitivity improvement is still a striving challenge. We show that coating standard microscope slides with nanoroughened silver films provides a high fluorescence signal enhancement due to plasmonic interactions. As a proof of concept, we applied these films with tailored plasmonic properties to DNA microarrays. Using common optical scanning devices, we achieved signal amplifications by more than 40-fold.

physics.ins-det