Chip-scale, electrically-pumped terahertz (THz) quantum cascade lasers (QCLs) can be employed in scattering-type scanning near-field optical microscopy (s-SNOM) to image the response of organic and inorganic materials with nanometer spatial resolution and tomographic sensitivity, overcoming the diffraction limit. By exploiting the self-mixing mechanism, QCLs can work as both sources and detectors, being sensitive to the radiation that is re-injected in the laser cavity after interaction with the tip of the s-SNOM microscope. Interestingly, broadband THz QCL frequency combs (FCs) provide hyperspectral sensitivity to THz s-SNOM systems.
The developed technique can be used to perform fundamental investigations at the nanoscale, spanning from inspecting the carrier density distribution in two-dimensional materials, to monitoring the propagation of plasmon–polariton, and phonon–polariton modes with a ~10 nm spatial resolution and over a broad bandwidth. We applied this method to thin films of topological insulators grown by molecular beam epitaxy (MBE), revealing the presence of Dirac surface states by mapping the propagation of surface polaritons.
KEYWORDS: Imaging spectroscopy, Near field, Terahertz radiation, Quantum cascade lasers, Sensors, Near field optics, Hyperspectral imaging, Image sensors, Frequency combs, Super resolution microscopy
We demonstrate the first-ever hyperspectral s-SNOM imaging system, providing 160nm spatial resolution, coherent detection of multiple phase-locked modes and mapping of the THz optical response of nanoscale materials such as topological insulators in the 2.29-3.60 THz range with noise-equivalent-power ~400pW/√Hz, relying on a 6mW comb-emitting THz QCL. We provide near-field images of Bi2Se3 and Bi2Te3 and their spectroscopic characterization in a >1 THz optical bandwidth extracting their optical contrast response through the application of the synthetic optical holography technique.
We report the polarization, the interference far-filed pattern, the multimodal spectral emission and the power extraction of the emitted beam from a set of electrically-pumped random quantum cascade lasers in the terahertz range. By integrating, on chip, a non-linear multilayer graphene stack with the laser gain medium, we demonstrate self-induced phase-coherence between the naturally incoherent random modes. We then employ the devised random laser in a detectorless near-field imaging system, exploiting the intracavity reinjection of the laser field via self-mixing interferometry in a confocal microscope for speckle-free tomography with nm-size resolution
Nanoscale optical integration is nowadays a strategic technological challenge and the ability of generating and manipulating nonlinear optical processes in sub-wavelength volumes is pivotal to realize efficient sensing probes and photonic sources for the next-generation communication technologies. Yet, confining nonlinear processes below the diffraction limit remains a challenging task because phase-matching is not a viable approach at the nanoscale. The localized fields associated to the resonant modes of plasmonic and dielectric nanoantennas offer a route to enhance and control nonlinear processes in highly confined volumes. In my talk I will discuss two nonlinear platforms based on plasmonic and dielectric nanostructures. The first relies on a broken symmetry antenna design, which brings about an efficient second harmonic generation (SHG). We recently applied this concept to an extended array of non-centrosymmetric nanoantennas for sensing applications. I will also show the evidence of a cascaded second-order process in Third Harmonic Generation (THG) in these nanoantennas.
Recently, dielectric nanoantennas emerged as an alternative to plasmonic nanostructures for nanophotonics applications, thanks to their sharp magnetic and electric Mie resonances along with the low ohmic losses in the visible/near-infrared region of the spectrum. I will present our most recent studies on the nonlinear properties of AlGaAs dielectric nanopillars. The strong localized modes along with the broken symmetry in the crystal structure of AlGaAs allow obtaining more than two orders of magnitude higher SHG efficiency with respect to plasmonic nanoantennas with similar spatial footprint and using the same pump power. I will also discuss a few key strategies we recently adopted to optically switch the SHG in these antennas even on the ultrafast time scale. Finally, I will show how to effectively engineer the sum frequency generation via the Mie resonances in these nanoantennas. These results draw a viable blueprint towards room-temperature all optical logic operation at the nanoscale.
Daniele Vella, Victor Vega-Mayoral, Christoph Gadermaier, Natasa Vujicic, Tetiana Borzda, Peter Topolovsek, Matej Prijatelj, Iacopo Tempra, Eva Arianna Aurelia Pogna, Giulio Cerullo
Ionic surfactants, which are widely used to stabilize nanomaterials in dispersions, can drastically alter the nanomaterial’s photophysical properties. Here, we use femtosecond optical spectroscopy to study the dynamics of excitons and charges in few-layer flakes of the two-dimensional semiconductor MoS2. We compare samples obtained via exfoliation in water with different amounts of adsorbed sodium cholate, obtained by repeated washing of the dried flakes. We find that the femtosecond dynamics is remarkably stable against the surfactant adsorption, with a slight increase of the initial exciton quenching occurring during the first few picoseconds as the only appreciable effect.
Here we study the exciton valley relaxation dynamics in atomically thin MoS2 by non-equilibrium optical techniques. A spin polarized excitons population is selectively created in a single valley by circularly polarized ultrashort laser pulses resonant with the optical gap, while the subsequent decay of the valley polarization is measured as a rotation of a linearly polarized probe beam due to a transient Faraday effect. We show that the photoinduced valley polarization in monolayer MoS2 is quenched after few ps due to an efficient intervalley scattering channel and it displays a peculiar bi-exponential behavior. This rapid time scale is in a good agreement with an intervalley scattering mechanism mediated by an electron-hole exchange interaction. Moreover time resolved circular dichroism experiments performed in the same experimental condition confirms the fast valley relaxation dynamics observed with transient Faraday rotation technique.
Access to the requested content is limited to institutions that have purchased or subscribe to SPIE eBooks.
You are receiving this notice because your organization may not have SPIE eBooks access.*
*Shibboleth/Open Athens users─please
sign in
to access your institution's subscriptions.
To obtain this item, you may purchase the complete book in print or electronic format on
SPIE.org.
INSTITUTIONAL Select your institution to access the SPIE Digital Library.
PERSONAL Sign in with your SPIE account to access your personal subscriptions or to use specific features such as save to my library, sign up for alerts, save searches, etc.