arXiv subjects

Franco V. A. Camargo

Publications and source records attributed to Franco V. A. Camargo.

6 recordsLinked to original sources

arXiv2026

Many-body Interactions in Ultrafast Spectroscopy

Nonlinear spectroscopy is widely used to probe ultrafast dynamics in matter. Signals of higher nonlinear orders encode valuable many-body dynamics but only recently have become individually retrievable. However, their physical interpretation in terms of double-sided Feynman diagrams is cumbersome and non-intuitive. Here, we establish an alternative framework that connects them to the underlying excitation conditions and many-body interactions. This approach predicts two classes of dynamic nonlinearities, due either to direct many-body interactions or to saturable kinetic channels. The method provides a direct physical interpretation of the retrieved signals, explaining their sign, magnitude, and dynamics. It also enables model-free reconstruction of the dynamics of a sub-ensemble of particles starting with a given number of excitons, which we demonstrate to be especially insightful. We validate the framework using colloidal CdSe/CdS core/shell quantum dots, which enable us to model nonlinearities of both classes in isolation and also combined.

physics.chem-ph↗

arXiv2024

Ultrafast valleytronic logic operations

Information processing currently reaches speeds as high as 800 GHz. However, the underlying transistor technology is quickly approaching its fundamental limits and further progress requires a disruptive approach. One such path is to manipulate quantum properties of solids, such as the valley degree of freedom, with ultrashort controlled lightwaves. Here we employ a sequence of few-optical-cycle visible pulses controlled with attosecond precision to excite and switch the valley pseudospin in a 2D semiconductor. We show that a pair of pulses separated in time with linear orthogonal polarizations can induce a valley-selective population. Additionally, exploiting a four-pump excitation protocol, we perform logic operations such as valley de-excitation and re-excitation at room temperature at rates as high as ~10 THz.

cond-mat.mes-hall↗

arXiv2024

The fate of optical excitons in FAPbI3 nanocube superlattices

Understanding the nature of the photoexcitation and ultrafast charge dynamics pathways in organic halide perovskite nanocubes and their aggregation into superlattices is key for the potential applications as tunable light emitters, photon harvesting materials and light-amplification systems. In this work, we apply two-dimensional coherent electronic spectroscopy (2DES) to track in real time the formation of near-infrared optical excitons and their ultrafast relaxation in CH(NH2)2PbI3 nanocube superlattices. Our results unveil that the coherent ultrafast dynamics is limited by the combination of the inherent short exciton decay time ~40 fs and the dephasing due to the coupling with selective optical phonon modes at higher temperatures. On the picosecond timescale, we observe the progressive formation of long-lived localized trap states. The analysis of the temperature dependence of the excitonic intrinsic linewidth, as extracted by the anti-diagonal components of the 2D spectra, unveils a dramatic change of the excitonic coherence time across the cubic to tetragonal structural transition. Our results offer a new way to control and enhance the ultrafast coherent dynamics of photocarrier generation in hybrid halide perovskite synthetic solids.

cond-mat.mes-hall↗

arXiv2024

Ultra-broadband Optical Diffraction Tomography

Optical diffraction tomography (ODT) is a powerful non-invasive 3D imaging technique, but its combination with broadband light sources is difficult. In this study, we introduce ultrabroadband ODT, covering over 150 nm of visible spectral bandwidth with a lateral spatial resolution of 150 nm. Our work addresses a critical experimental gap by enabling the measurement of broadband refractive index changes in 3D samples, a crucial information that is difficult to assess with existing methodologies. We present broadband, spectrally resolved ODT images of HeLa cells, obtained via pulse-shaping based Fourier transform spectroscopy. The spectral observations enabled by ultrabroadband ODT, combined with material-dependent refractive index responses, allow for precise three-dimensional identification of the nanoparticles within cellular structures. Our work represents a crucial step towards time and spectrally-resolved tomography of complex 3D structures with implications for life and materials science applications.

physics.optics↗

arXiv2022

Rapid-scan nonlinear time-resolved spectroscopy over arbitrary delay intervals

Femtosecond dual-comb lasers have revolutionized linear Fourier-domain spectroscopy by offering a rapid motion-free, precise and accurate measurement mode with easy registration of the combs beat note in the RF domain. Extensions of this technique found already application for nonlinear time-resolved spectroscopy within the energy limit available from sources operating at the full oscillator repetition rate. Here, we present a technique based on time filtering of femtosecond frequency combs by pulse gating in a laser amplifier. This gives the required boost to the pulse energy and provides the flexibility to engineer pairs of arbitrarily delayed wavelength-tunable pulses for pump-probe techniques. Using a dual-channel millijoule amplifier, we demonstrate programmable generation of both extremely short, fs, and extremely long (>ns) interpulse delays. A predetermined arbitrarily chosen interpulse delay can be directly realized in each successive amplifier shot, eliminating the massive waiting time required to alter the delay setting by means of an optomechanical line or an asynchronous scan of two free-running oscillators. We confirm the versatility of this delay generation method by measuring chi^(2) cross-correlation and chi^(3) multicomponent population recovery kinetics.

physics.optics↗

arXiv2021

Widefield phototransient imaging for visualizing 3D motion of resonant particles in scattering environments

Identifying, visualising and ultimately tracking dynamically moving non-fluorescent nanoparticles in the presence of non-specific scattering is a long-standing challenge across the nano- and life-sciences. In this work we demonstrate that our recently developed ultrafast holographic transient (UHT) microscope is ideally suited for meeting this challenge. We show that UHT microscopy allows reliably distinguishing off-resonant, dielectric, from resonant, metallic, nanoparticles, based on the phototransient signal: a pre-requisite for single-particle tracking in scattering environments. We then demonstrate the capability of UHT microscopy to holographically localize in 3D single particles over large volumes of view. Ultimately, we combine the two concepts to simultaneously track several tens of freely diffusing gold nanoparticles, within a 110x110x110 $μ$m volume of view at an integration time of 10 ms per frame, while simultaneously recording their phototransient signals. The combined experimental concepts outlined and validated in this work lay the foundation for background-free 3D single-particle tracking applications or spectroscopy in scattering environments and are immediately applicable to systems as diverse as live cells and tissues or supported heterogeneous catalysts.

physics.optics↗