arXiv subjects

Carino Ferrante

Publications and source records attributed to Carino Ferrante.

15 recordsLinked to original sources

arXiv2026

Searching for Axions on a Higher Note: Third-Harmonic Generation from Colliding High-Intensity Laser Beams

We propose a new laboratory strategy to generate and detect axion-like particles via third-harmonic generation induced by two non-collinear, polarised high-intensity laser beams of peak intensity of the order of $10^{24}\,\mathrm{W/cm^2}$, where the third-harmonic signal is generated by the axion field. Starting from the axion-modified Maxwell equations, we analytically derive the axion-induced third-harmonic field, and show that by using state-of-the-art petawatt laser facilities, a detectable signal can be obtained over a broad range of axion masses and couplings. A key feature of the setup is that the axion-photon conversion rate can be resonantly enhanced by tuning the angle between the two beams through a mechanism that does not depend on the physical volume of the apparatus. The proposed configuration may therefore probe an unexplored region of axion parameter space and pave the way for next-generation high-power laser-based axion searches.

hep-ph↗

arXiv2026

Enantio-selective inverse Faraday effect in isotropic chiral molecular mixtures

Enantiomeric excess detection in a chiral molecular mixture is paramount because very often opposite enantiomers exhibit profound functional dissimilarities that play decisive roles in biochemical applications. Existing chiral sensing methods mostly rely on large operational sample volumes, hindering compatibility with integrated sensing schemes. Here, we propose a novel chiroptical sensing technique based on the inverse Faraday effect in a photonic micro-capillary filled with nl-volume chiral drug solution. We theoretically demonstrate that, upon excitation by intense laser light, an isotropic assembly of chiral drugs produces a static magnetisation, with amplitude and direction depending on the enantiomeric excess. In turn, by measuring the chirally-sensitive static magnetic field in the vicinity of the micro-tube one can retrieve the enantiomeric excess of the chiral drug solution. Our theoretical predictions unlock new opportunities for the development of innovative nanophotonic devices suitable for efficient chiroptical sensing with nl-volume sensitivity.

physics.optics↗

arXiv2026

Chirally-sensitive optical rectification by isotropic chiral media

Chiroptical sensing is central to gain fundamental insight into electronic, vibrational and rotational degrees of freedom of chiral molecules, and is a cornerstone for nanomedicine and drug discovery platforms. Current chiral sensing technologies to assess the enantiomeric imbalance of chiral pharmaceutical compounds are sensitive to ml volumes but are time-consuming and cannot be integrated on a chip, thus creating a major bottleneck for drug discovery and nanomedicine. Here, we propose a novel chiroptical sensing approach based on optical rectification in a photonic micro-cavity filled by a drug solution with nl volume. We theoretically demonstrate that, upon optical excitation by intense pulsed laser light, such a nonlinear effect produces a chirally-sensitive nV voltage burst at the electrically-gated micro-cavity boundaries, with sign depending solely on the drug enantiomeric imbalance. Our results shed light on the potential of optical rectification as a robust platform for innovative lab-on-a-chip devices enabling chiral sensing with nl sensitivity.

physics.optics↗

arXiv2025

Femtosecond self-diffraction as a measure of the nonlinear response spectrum

Self diffraction is a four-wave mixing process proportional to the square modulus of third-order nonlinearity susceptibility $\chi^{(3)}$, which is related to the material's electronic and thermal properties. In this study, we investigate the wavelength dependence of the self-diffracted signal generated by a femtosecond pulsed laser in a dye solution to directly evaluate the electronic third-order nonlinear susceptibility spectrum. By accounting for absorption effects and phase matching conditions, we determine the $\vert\chi^{(3)}\vert$ for different concentrations. Experimental results complemented with theoretical predictions, show that in the low absorption and thin sample limits, the signal reproduce the $\vert\chi^{(3)}\vert$ spectral profile. These findings demonstrate the feasibility of measuring nonlinear susceptibility spectra arising solely from the bound-electronic response across a wide spectral range and for various compounds.

physics.optics↗

arXiv2025

Enhanced vibrational optical activity by near-zero index chiral effective media

The enhancement of the inherently weak optical activity of solvated molecules by superchiral fields, crucial for detecting their chirality, is a research frontier of photonics and the basis of novel chiroptical detection schemes. Here, we show that an effective medium consisting of randomly dispersed metal-based nanoparticles embedded within an optically active solvated drug (aqueous reparixin) can enhance vibrational optical rotation and circular dichroism thanks to superchirality produced by slow light in near-zero index conditions. We evaluate from first principles the effective bianisotropic response of the bulk chiral effective medium, showing that, by adjusting the nanoparticles filling fraction, vibrational optical activity is greatly enhanced by a factor $\simeq 10^2-10^3$ at the near-zero index resonance. Our results are relevant for the development of innovative devices capable of detecting the chirality of low-volume samples, with applications in quantum chemistry and nanomedicine.

physics.optics↗

arXiv2023

Quasi-phase-matched up- and down-conversion in periodically poled layered semiconductors

Nonlinear optics lies at the heart of classical and quantum light generation. The invention of periodic poling revolutionized nonlinear optics and its commercial applications by enabling robust quasi-phase-matching in crystals such as lithium niobate. However, reaching useful frequency conversion efficiencies requires macroscopic dimensions, limiting further technology development and integration. Here we realize a periodically poled van der Waals semiconductor (3R-MoS$_2$). Due to its exceptional nonlinearity, we achieve macroscopic frequency conversion efficiency of 0.03% at the relevant telecom wavelength over a microscopic thickness of 3.4${\mu}$m (that is, 3 poling periods), $10-100\times$ thinner than current systems with similar performances. Due to unique intrinsic cavity effects, the thickness-dependent quasi-phase-matched second harmonic signal surpasses the usual quadratic enhancement by $50\%$. Further, we report the broadband generation of photon pairs at telecom wavelengths via quasi-phase-matched spontaneous parametric down-conversion, showing a maximum coincidence-to-accidental-ratio of $638 \pm 75$. This work opens the new and unexplored field of phase-matched nonlinear optics with microscopic van der Waals crystals, unlocking applications that require simple, ultra-compact technologies such as on-chip entangled photon-pair sources for integrated quantum circuitry and sensing.

physics.optics↗

arXiv2023

Retrieving genuine nonlinear Raman responses in ultrafast spectroscopy via deep learning

Noise manifests ubiquitously in nonlinear spectroscopy, where multiple sources contribute to experimental signals generating interrelated unwanted components, from random point-wise fluctuations to structured baseline signals. Mitigating strategies are usually heuristic, depending on subjective biases like the setting of parameters in data analysis algorithms and the removal order of the unwanted components. We propose a data-driven frequency-domain denoiser based on a convolutional neural network with kernels of different sizes acting in parallel to extract authentic vibrational features from nonlinear background in noisy spectroscopic raw data. We test our approach by retrieving asymmetric peaks in stimulated Raman spectroscopy (SRS), an ideal test-bed due to its intrinsic complex spectral features combined with a strong background signal. By using a theoretical perturbative toolbox, we efficiently train the network with simulated datasets resembling the statistical properties and lineshapes of the experimental spectra. The developed algorithm is successfully applied to experimental data to obtain noise- and background-free SRS spectra of organic molecules and prototypical heme proteins.

physics.optics↗

arXiv2023

Plasmon-enhanced circular dichroism spectroscopy of chiral drug solutions

We investigate the potential of surface plasmon polaritons at noble metal interfaces for surface-enhanced chiroptical sensing of dilute chiral drug solutions. The high quality factor of surface plasmon resonances in both Otto and Kretschmann configurations enables the enhancement of circular dichroism differenatial absorption thanks to the large near-field intensity of such plasmonic excitations. Furthermore, the subwavelength confinement of surface plasmon polaritons is key to attain chiroptical sensitivity to small amounts of drug volumes placed around $\simeq 100$ nm by the metal surface. Our calculations focus on reparixin, a pharmaceutical molecule currently used in clinical studies for patients with community-acquired pneumonia, including COVID-19 and acute respiratory distress syndrome. Considering realistic dilute solutions of reparixin dissolved in water with concentration $\leq 5$ mg$/$ml, we find a circular-dichroism differential absorption enhancement factor of the order $\simeq 20$ and chirality-induced polarization distortion upon surface plasmon polariton excitation.

physics.optics↗

arXiv2023

XUV plasmonic waveguides by near-zero index heterostructures

The lack of transmissive photonic components in the extreme ultra-violet (XUV) constitutes a challenge for micro/nano-metric confinement. Here, we theoretically design a novel approach to attain XUV radiation guidance based on the electromagnetic properties of Titanium-Aluminum-Titanium heterostructures in such a spectral domain. We show that, thanks to the near-zero-index properties of aluminum and titanium, XUV radiation can couple efficiently with plasma oscillations in such heterostructures, enabling the excitation of several distinct plasmon polariton modes. Our predictions, based on the semi-analytical solution of fully vectorial Maxwell's equations, indicate that the dispersion profile of plasmon polariton modes can get efficiently modulated by the aluminum thickness, enabling nanometre confinement and micrometre propagation length. Moreover, we quantify the third-order nonlinearity enhancement factor, finding that it is resonant at the zero-index wavelength. Our results are promising for the development of future devices enabling advanced control and manipulation of XUV radiation.

physics.optics↗

arXiv2022

Picosecond energy transfer in a transition metal dichalcogenide-graphene heterostructure revealed by transient Raman spectroscopy

Intense light-matter interactions and unique structural and electrical properties make Van der Waals heterostructures composed by Graphene (Gr) and monolayer transition metal dichalcogenides (TMD) promising building blocks for tunnelling transistors, flexible electronics, as well as optoelectronic devices, including photodetectors, photovoltaics and quantum light emitting devices (QLEDs), bright and narrow-line emitters using minimal amounts of active absorber material. The performance of such devices is critically ruled by interlayer interactions which are still poorly understood in many respects. Specifically, two classes of coupling mechanisms have been proposed: charge transfer (CT) and energy transfer (ET), but their relative efficiency and the underlying physics is an open question. Here, building on a time resolved Raman scattering experiment, we determine the electronic temperature profile of Gr in response to TMD photo-excitation, tracking the picosecond dynamics of the G and 2D bands. Compelling evidence for a dominant role ET process accomplished within a characteristic time of ~ 4 ps is provided. Our results suggest the existence of an intermediate process between the observed picosecond ET and the generation of a net charge underlying the slower electric signals detected in optoelectronic applications.

cond-mat.mes-hall↗

arXiv2021

Excited-state energy surfaces in molecules revealed by impulsive stimulated Raman excitation profiles

Photophysical and photochemical processes are ruled by the interplay between transient vibrational and electronic degrees of freedom, which are ultimately determined by the multidimensional potential energy surfaces (PESs). Differences between ground and excited PESs are encoded in the relative intensities of resonant Raman bands, but they are experimentally challenging to access requiring measurements at multiple wavelengths under identical conditions. Here we perform a two-color impulsive vibrational scattering experiment to launch nuclear wavepacket motions by an impulsive pump and record their coupling with a targeted excited-state potential by resonant Raman processes with a delayed probe, generating in a single-measurement background-free vibrational spectra across the entire sample absorption. Building on the interference between the multiple pathways resonant with the excited-state manifold that generate the Raman signal, we show how to experimentally tune their relative phase by varying the probe chirp, decoding nuclear displacements along different normal modes and revealing the multidimensional PESs. Our results are validated against time-dependent density functional theory.

physics.chem-ph↗

arXiv2021

Non-linear self-driven spectral tuning of Extreme Ultraviolet Femtosecond Pulses in monoatomic materials

Self-action nonlinearity is a key aspect -- either as a foundational element or a detrimental factor -- of several optical spectroscopies and photonic devices. Supercontinuum generation, wavelength converters and chirped pulse amplification are just a few examples. The recent advent of Free Electron Lasers (FEL) fostered building on nonlinearity to propose new concepts and extend optical wavelengths paradigms for extreme ultraviolet (EUV) and X-ray regimes. No evidence for intrapulse dynamics, however, has been reported at such short wavelengths, where the light-matter interactions are ruled by the sharp absorption edges of core-electrons. Here, we provide experimental evidence for self-phase modulation of femtosecond FEL pulses, which we exploit for fine self-driven spectral tunability by interaction with sub-micrometric foils of selected monoatomic materials. Moving the pulse wavelength across the absorption edge, the spectral profile changes from a non-linear spectral blue-shift to a red-shifted broadening. These findings are rationalized accounting for ultrafast ionization and delayed thermal response of highly excited electrons above and below threshold, respectively.

physics.optics↗

arXiv2020

Accessing Excited State Molecular Vibrations by Femtosecond Stimulated Raman Spectroscopy

Excited-state vibrations are crucial for determining photophysical and photochemical properties of molecular compounds. Stimulated Raman scattering can coherently stimulate and probe molecular vibrations with optical pulses, but it is generally restricted to ground state properties. Working in resonance conditions, indeed, enables cross-section enhancement and selective excitation to a targeted electronic level, but is hampered by an increased signal complexity due to the presence of overlapping spectral contributions. Here, we show how detailed information on ground and excited state vibrations can be disentangled, by exploiting the relative time delay between Raman and probe pulses to control the excited state population, combined with a diagrammatic formalism to dissect the pathways concurring to the signal generation. The proposed method is then exploited to elucidate the vibrational properties of ground and excited electronic states in the paradigmatic case of Cresyl Violet. We anticipate that the presented approach holds the potential for selective mapping the reaction coordinates pertaining to transient electronic stages implied in photo-active compounds.

physics.optics↗

arXiv2019

Broadband Impulsive Stimulated Raman Scattering based on a Chirped Detection

In Impulsive Stimulated Raman Scattering vibrational oscillations, coherently stimulated by a femtosecond Raman pulse, are real time monitored and read out as intensity modulations in the transmission of a temporally delayed probe pulse. Critically, in order to retrieve broadband Raman spectra, a fine sampling of the time delays between the Raman and probe pulses is required, making conventional ISRS ineffective for probing irreversible phenomena and/or weak scatterers typically demanding long acquisition times, with signal to noise ratios that crucially depend on the pulse fluences and overlap stabilities. To overcome such limitations, here we introduce Chirped based Impulsive Stimulated Raman Scattering (CISRS) technique. Specifically, we show how introducing a chirp in the probe pulse can be exploited for recording the Raman information without scanning the Raman-probe pulse delay. Then we experimentally demonstrate with a few examples how to use the introduced scheme to measure Raman spectra.

physics.chem-ph↗

arXiv2017

Probing Femtosecond Lattice Displacement upon Photo-carrier generation in Lead Halide Perovskite

Electronic properties and lattice vibrations are supposed to be strongly correlated in metal-halide perovskites, due to the "soft" fluctuating nature of their crystal lattice. Thus, unveiling electron-phonon coupling dynamics upon ultra-fast photoexcitation is necessary for understanding the optoelectronic behaviour of the semiconductor. Here, we use impulsive vibrational spectroscopy to reveal ground and excited state vibrational modes of methylammonium lead-bromide perovskite. We observe a coherent phonon at 106 cm-1 (13 meV), pertaining to the inorganic octahedral, which is peculiar of the electronic excited state and generated via displacive excitation mechanism. This indicates the formation of a new geometry, reached after a quarter of the phonon period T/4=80 fs, and fully equilibrated within the phonon lifetime of about 1 ps. Our observations unambiguously prove that this mode drives the crystalline distortion occurring upon carrier generation, implying the presence of polaronic effects.

cond-mat.mtrl-sci↗