arXiv subjects

Leonetta Baldassarre

Publications and source records attributed to Leonetta Baldassarre.

14 recordsLinked to original sources

arXiv2026

Resonantly-enhanced Raman response in graphene-capped bismuthene on SiC

Two-dimensional quantum spin Hall insulators based on atomic monolayers offer a promising route toward dissipationless electronics, yet their practical use is often limited by environmental instability. Encapsulating the system with a graphene capping layer has been shown to be a reliable method to prevent oxidation and degradation. However, the confirmation of a successful encapsulation still relies on ultra-high vacuum techniques, that considerably slow the process. Here, we present an ex situ, rapid, nondestructive and spatially resolved Raman characterization of graphene-capped bismuthene, a honeycomb monolayer of Bi on SiC. A pronounced Raman scattering peak at around 122 cm-1 is identified as the E2g phonon of bismuthene, via a comparison with density functional perturbation theory calculations. We use excitation-energy and polarization-dependent Raman measurements to enable an unambiguous assignment of the spectral features. Tuning the excitation energy close to the excitonic transition in pristine bismuthene, we observe a strong enhancement of the Raman response and the emergence of additional scattering peaks. In this regime, higher-order phonon features, as well as interfacial modes between bismuthene and the SiC substrate, become visible, suggesting the involvement of resonant scattering processes. Our results establish Raman micro-spectroscopy as a versatile tool for probing graphene-protected quantum materials, providing access to lattice dynamics and interlayer coupling.

cond-mat.mtrl-sci↗

arXiv2025

Probing enhanced electron-phonon coupling in graphene by infrared resonance Raman spectroscopy

We report on resonance Raman spectroscopy measurements with excitation photon energy down to 1.16 eV on graphene, to study how low-energy carriers interact with lattice vibrations. Thanks to the excitation energy close to the Dirac point at $\mathbf{K}$, we unveil a giant increase of the intensity ratio between the double-resonant 2D and 2D$^\prime$ peaks with respect to that measured in graphite. Comparing with fully \textit{ab initio} theoretical calculations, we conclude that the observation is explained by an enhanced, momentum-dependent coupling between electrons and Brillouin zone-boundary optical phonons. This finding applies to two dimensional Dirac systems and has important consequences for the modeling of transport in graphene devices operating at room temperature.

cond-mat.mes-hall↗

arXiv2024

Infrared resonance Raman of bilayer graphene: signatures of massive fermions and band structure on the 2D peak

Few-layer graphene possesses low-energy carriers which behave as massive fermions, exhibiting intriguing properties in both transport and light scattering experiments. Lowering the excitation energy of resonance Raman spectroscopy down to 1.17 eV we target these massive quasiparticles in the split bands close to the K point. The low excitation energy weakens some of the Raman processes which are resonant in the visible, and induces a clearer frequency-separation of the sub-structures of the resonance 2D peak in bi- and trilayer samples. We follow the excitation-energy dependence of the intensity of each sub-structure and, comparing experimental measurements on bilayer graphene with ab initio theoretical calculations, we trace back such modifications on the joint effects of probing the electronic dispersion close to the band splitting and enhancement of electron-phonon matrix elements.

cond-mat.mes-hall↗

arXiv2022

Detection of strong light-matter interaction in a single nano-cavity with a thermal transducer

Recently, the concept of strong light-matter coupling has been demonstrated in semiconductor structures, and it is poised to revolutionize the design and implementation of components, including solid state lasers and detectors. We demonstrate an original nanospectroscopy technique that permits to study the light-matter interaction in single subwavelength-sized nano-cavities where far-field spectroscopy is not possible using conventional techniques. We inserted a thin ($\approx$ 150 nm) polymer layer with negligible absorption in the mid-IR (5 $μ$m < $λ$ < 12 $μ$m) inside a metal-insulator-metal resonant cavity, where a photonic mode and the intersubband transition of a semiconductor quantum well are strongly coupled. The intersubband transition peaks at $λ$ = 8.3 $μ$m, and the nano-cavity is overall 270 nm thick. Acting as a non-perturbative transducer, the polymer layer introduces only a limited alteration of the optical response while allowing to reveal the optical power absorbed inside the concealed cavity. Spectroscopy of the cavity losses is enabled by the polymer thermal expansion due to heat dissipation in the active part of the cavity, and performed using an atomic force microscope (AFM). This innovative approach allows the typical anticrossing characteristic of the polaritonic dispersion to be identified in the cavity loss spectra at the single nano-resonator level. Results also suggest that near-field coupling of the external drive field to the top metal patch mediated by a metal-coated AFM probe tip is possible, and it enables the near-field mapping of the cavity mode symmetry including in the presence of strong light-matter interaction.

physics.optics↗

arXiv2022

Raman Scattering with infrared excitation resonant with MoSe$_2$ indirect band gap

Resonance Raman scattering, which probes electrons, phonons and their interplay in crystals, is extensively used in two-dimensional materials. Here we investigate Raman modes in MoSe$_2$ at different laser excitation energies from 2.33 eV down to the near infrared 1.16 eV. The Raman spectrum at 1.16 eV excitation energy shows that the intensity of high-order modes is strongly enhanced if compared to the first-order phonon modes intensity due to resonance effects with the MoSe$_2$ indirect band gap. By comparing the experimental results with the two-phonon density of states calculated with density functional theory, we show that the high-order modes originate mostly from two-phonon modes with opposite momenta. In particular, we identify the momenta of the phonon modes that couple strongly with the electrons to produce the resonance process at 1.16 eV, while we verify that at 2.33 eV the two-phonon modes lineshape compares well with the two-phonon density of state calculated over the entire Brillouin Zone. We also show that, by lowering the crystal temperature, we actively suppress the intensity of the resonant two-phonon modes and we interpret this as the result of the increase of the indirect band gap at low temperature that moves our excitation energy out of the resonance condition.

cond-mat.mtrl-sci↗

arXiv2022

Terahertz control of photoluminescence emission in few-layer InSe

A promising route for the development of opto-elelctronic technology is to use terahertz radiation to modulate the optical properties of semiconductors. Here we demonstrate the dynamical control of photoluminescence (PL) emission in few-layer InSe using picosecond terahertz pulses. We observe a strong PL quenching (up to 50%) after the arrival of the terahertz pulse followed by a reversible recovery of the emission on the time scale of 50ps at T =10K. Microscopic calculations reveal that the origin of the photoluminescence quenching is the terahertz absorption by photo-excited carriers: this leads to a heating of the carriers and a broadening of their distribution, which reduces the probability of bimolecular electron-hole recombination and, therefore, the luminescence. By numerically evaluating the Boltzmann equation, we are able to clarify the individual roles of optical and acoustic phonons in the subsequent cooling process. The same PL quenchingmechanismis expected in other van derWaals semiconductors and the effectwill be particularly strong for materials with low carrier masses and long carrier relaxation time, which is the case for InSe. This work gives a solid background for the development of opto-electronic applications based on InSe, such as THz detectors and optical modulators.

cond-mat.mtrl-sci↗

arXiv2021

Modelling photothermal induced resonance microscopy: the role of interface thermal resistances

Infrared (IR) nanospectroscopy by photothermal induced resonance (PTIR) is a novel experimental technique that combines the nanoscale resolution granted by atomic force microscopy (AFM) and the chemical labelling made possible by IR absorption spectroscopy. While the technique has developed enormously over the last decade from an experimental point of view, the theoretical modelling of the signal still varies significantly throughout the literature and misses a solid benchmark. Here, we report an analysis focused on the electromagnetic and thermal simulations of a PTIR experiment. Thanks to a control experiment where the signal is acquired as a function of the thickness of a polymer film and for different tip geometries, we find clear evidence that the interface thermal resistances play a key role in the determination of the measured signal and should therefore always be accounted for by any quantitative modelling.

cond-mat.mtrl-sci↗

arXiv2021

Second harmonic generation in germanium quantum wells for nonlinear silicon photonics

Second-harmonic generation (SHG) is a direct measure of the strength of second-order nonlinear optical effects, which also include frequency mixing and parametric oscillations. Natural and artificial materials with broken center-of-inversion symmetry in their unit cell display high SHG efficiency, however the silicon-foundry compatible group-IV semiconductors (Si, Ge) are centrosymmetric, thereby preventing full integration of second-order nonlinearity in silicon photonics platforms. Here we demonstrate strong SHG in Ge-rich quantum wells grown on Si wafers. The symmetry breaking is artificially realized with a pair of asymmetric coupled quantum wells (ACQW), in which three of the quantum-confined states are equidistant in energy, resulting in a double resonance for SHG. Laser spectroscopy experiments demonstrate a giant second-order nonlinearity at mid-infrared pump wavelengths between 9 and 12 microns. Leveraging on the strong intersubband dipoles, the nonlinear susceptibility almost reaches 10^5 pm/V

physics.optics↗

arXiv2020

Intersubband transition engineering in the conduction band of asymmetric coupled Ge/SiGe quantum wells

: n-type Ge/SiGe asymmetric-coupled quantum wells represent the building block of a variety of nanoscale quantum devices, including recently proposed designs for a silicon-based THz quantum cascade laser. In this paper, we combine structural and spectroscopic experiments on 20-module superstructures, each featuring two Ge wells coupled through a Ge-rich tunnel barrier, as a function of the geometry parameters of the design and the P dopant concentration. Through the comparison of THz spectroscopic data with numerical calculations of intersubband optical absorption resonances, we demonstrated that it is possible to tune by design the energy and the spatial overlap of quantum confined subbands in the conduction band of the heterostructures. The high structural/interface quality of the samples and the control achieved on subband hybridization are the promising starting point towards a working electrically pumped light-emitting device.

cond-mat.mes-hall↗

arXiv2019

Tip-Enhanced Infrared Difference-Nanospectroscopy of the Proton Pump Activity of Bacteriorhodopsin in Single Purple Membrane Patches

Photosensitive proteins embedded in the cell membrane (about 5 nm thickness) act as photoactivated proton pumps, ion gates, enzymes, or more generally, as initiators of stimuli for the cell activity. They are composed of a protein backbone and a covalently bound cofactor (e.g. the retinal chromophore in bacteriorhodopsin (BR), channel rhodopsin, and other opsins). The light-induced conformational changes of both the cofactor and the protein are at the basis of the physiological functions of photosensitive proteins. Despite the dramatic development of microscopy techniques, investigating conformational changes of proteins at the membrane monolayer level is still a big challenge. Techniques based on atomic force microscopy (AFM) can detect electric currents through protein monolayers and even molecular binding forces in single-protein molecules but not the conformational changes. For the latter, Fourier-transform infrared spectroscopy (FTIR) using difference-spectroscopy mode is typically employed, but it is performed on macroscopic liquid suspensions or thick films containing large amounts of purified photosensitive proteins. In this work, we develop AFM-assisted, tip-enhanced infrared difference-nanospectroscopy to investigate light-induced conformational changes of the bacteriorhodopsin mutant D96N in single submicrometric native purple membrane patches. We obtain a significant improvement compared with the signal-to-noise ratio of standard IR nanospectroscopy techniques by exploiting the field enhancement in the plasmonic nanogap that forms between a gold-coated AFM probe tip and an ultraflat gold surface, as further supported by electromagnetic and thermal simulations. IR difference-spectra in the 1450-1800 cm^{-1} range are recorded from individual patches as thin as 10 nm, with a diameter of less than 500 nm, well beyond the diffraction limit for FTIR microspectroscopy...

physics.bio-ph↗

arXiv2019

Plasmonic superchiral lattice resonances in the mid-infrared

Recent efforts in the field of surface-enhanced spectroscopies have focused on the paradigm of superchirality, entailing the engineering of the local electromagnetic fields to boost the enantiospecific interaction between light and chiral molecules. In this framework, approaches based on both metallic and dielectric nanostructures have been proposed and have also recently been extended to vibrational circular dichroism in the mid-infrared. In this work, we design, fabricate and characterize arrays of chiral plasmonic slits featuring enhanced chiral fields in the mid-infrared. We exploit collective lattice resonances to further enhance the local intensity and to generate sharp features in the circular dichroism spectra of the platform. Such features are ideally suited to test the superchiral coupling with the vibrational resonances of chiral molecules.

cond-mat.mes-hall↗

arXiv2016

Tunability and Losses of Mid-infrared Plasmonics in Heavily Doped Germanium Thin Films

Heavily-doped semiconductor films are very promising for application in mid-infrared plasmonic devices because the real part of their dielectric function is negative and broadly tunable in this wavelength range. In this work we investigate heavily n-type doped germanium epilayers grown on different substrates, in-situ doped in the $10^{17}$ to $10^{19}$ cm$^{-3}$ range, by infrared spectroscopy, first principle calculations, pump-probe spectroscopy and dc transport measurements to determine the relation between plasma edge and carrier density and to quantify mid-infrared plasmon losses. We demonstrate that the unscreened plasma frequency can be tuned in the 400 - 4800 cm$^{-1}$ range and that the average electron scattering rate, dominated by scattering with optical phonons and charged impurities, increases almost linearly with frequency. We also found weak dependence of losses and tunability on the crystal defect density, on the inactivated dopant density and on the temperature down to 10 K. In films where the plasma was optically activated by pumping in the near-infrared, we found weak but significant dependence of relaxation times on the static doping level of the film. Our results suggest that plasmon decay times in the several-picosecond range can be obtained in n-type germanium thin films grown on silicon substrates hence allowing for underdamped mid-infrared plasma oscillations at room temperature.

cond-mat.mtrl-sci↗

arXiv2015

Mid-Infrared Plasmonic Platform based on Heavily Doped Epitaxial Ge-on-Si: Retrieving the Optical Constants of Thin Ge Epilayers

The n-type Ge-on-Si epitaxial material platform enables a novel paradigm for plasmonics in the mid-infrared, prompting the future development of lab-on-a-chip and subwavelength vibrational spectroscopic sensors. In order to exploit this material, through proper electrodynamic design, it is mandatory to retrieve the dielectric constants of the thin Ge epilayers with high precision due to the difference from bulk Ge crystals. Here we discuss the procedure we have employed to extract the real and imaginary part of the dielectric constants from normal incidence reflectance measurements, by combining the standard multilayer fitting procedure based on the Drude model with Kramers-Kronig transformations of absolute reflectance data in the zero-transmission range of the thin film.

cond-mat.mes-hall↗

arXiv2013

Transmittance and reflectance measurements at terahertz frequencies on a superconducting BaFe_{1.84}Co_{0.16}As_2 ultrathin film: an analysis of the optical gaps in the Co-doped BaFe_2As_2 pnictide

Here we report an optical investigation in the terahertz region of a 40 nm ultrathin BaFe$_{1.84}$Co$_{0.16}$As$_2$ superconducting film with superconducting transition temperature T$_c$ = 17.5 K. A detailed analysis of the combined reflectance and transmittance measurements showed that the optical properties of the superconducting system can be described in terms of a two-band, two-gap model. The zero temperature value of the large gap $Δ_B$, which seems to follow a BCS-like behavior, results to be $Δ_B$(0) = 17 cm$^{-1}$. For the small gap, for which $Δ_A$(0) = 8 cm$^{-1}$, the temperature dependence cannot be clearly established. These gap values and those reported in the literature for the BaFe$_{2-x}$Co$_{x}$As$_2$ system by using infrared spectroscopy, when put together as a function of T$_c$, show a tendency to cluster along two main curves, providing a unified perspective of the measured optical gaps. Below a temperature around 20 K, the gap-sizes as a function of T$_c$ seem to have a BCS-like linear behavior, but with different slopes. Above this temperature, both gaps show different supra-linear behaviors.

cond-mat.supr-con↗