arXiv subjects

Nicola Di Palo

Publications and source records attributed to Nicola Di Palo.

6 recordsLinked to original sources

arXiv2022

Field-driven attosecond photoinjection dynamics in semiconductors

The route towards manipulation of the optoelectronic properties of matter beyond the current limits of electronics starts from a comprehensive study of the ultrafast dynamics triggered by interaction with light. Among them, a fundamental role is played by charge photoinjection, a complex process that stems from the interplay of many different physical phenomena, which cannot be easily disentangled. Single- and multi-photon absorption, diabatic tunnelling, intra-band motion, and field-driven band dressing, all concur in determining the overall excited electron population, dictating the electro-optical properties of a material. Here we investigate ultrafast photoinjection in a prototypical semiconductor (monocrystalline germanium) by using attosecond transient reflection spectroscopy. The precise pump-field characterization ensured by a simultaneous attosecond streaking experiment, in tandem with a comprehensive theoretical approach, allowed us to disentangle the different physical phenomena unfolding at different positions in the reciprocal space and at different timing within the envelope of the pump pulse. Moreover, we found that intra-band phenomena hinder charge injection, in contrast to what was previously observed for resonant, direct band-gap semiconductors. Therefore, besides other known parameters as the central wavelength and peak intensity, our results indicate that the pulse temporal envelope and the local band structure probed by intra-band effects are of key importance to achieve an optimal control over the ultrafast carrier injection process and tailor the complex optical and electronic properties of a semiconductor on the few- to sub-femtosecond time scale.

physics.optics↗

arXiv2021

Reconstruction of ultrafast exciton dynamics with a phase-retrieval algorithm

The first step to gain optical control over the ultrafast processes initiated by light in solids is a correct identification of the physical mechanisms at play. Among them, exciton formation has been identified as a crucial phenomenon which deeply affects the electro-optical properties of most semiconductors and insulators of technological interest. While recent experiments based on attosecond spectroscopy techniques have demonstrated the possibility to observe the early-stage exciton dynamics, the description of the underlying exciton properties remains non-trivial. In this work we propose a new method called extended Ptychographic Iterative engine for eXcitons (ePIX), capable of reconstructing the main physical properties which determine the evolution of the quasi-particle with no prior knowledge of the exact relaxation dynamics or the pump temporal characteristics. By demonstrating its accuracy even when the exciton dynamics is comparable to the pump pulse duration, ePIX is established as a powerful approach to widen our knowledge of solid-state physics.

physics.optics↗

arXiv2021

Time-frequency mapping of two-colour photoemission driven by harmonic radiation

The use of few-femtosecond, extreme ultraviolet (XUV) pulses, produced by high-order harmonic generation, in combination with few-femtosecond infrared (IR) pulses in pump-probe experiments has great potential to disclose ultrafast dynamics in molecules, nanostructures and solids. A crucial prerequisite is a reliable characterization of the temporal properties of the XUV and IR pulses. Several techniques have been developed. The majority of them applies phase reconstruction algorithms to a photoelectron spectrogram obtained by ionizing an atomic target in a pump-probe fashion. If the ionizing radiation is a single harmonic, all the information is encoded in a two-color two-photon signal called sideband (SB). In this work, we present a simplified model to interpret the time-frequency mapping of the SB signal and we show that the temporal dispersion of the pulses directly maps onto the shape of its spectrogram. Finally, we derive an analytical solution, which allows us to propose a novel procedure to estimate the second-order dispersion of the XUV and IR pulses in real time and with no need for iterative algorithms.

physics.optics↗

arXiv2020

Attosecond state-resolved carrier motion in quantum materials probed by soft X-ray XANES

Recent developments in attosecond technology led to tabletop X-ray spectroscopy in the soft X-ray range, thus uniting the element- and state-specificity of core-level x-ray absorption spectroscopy with the time resolution to follow electronic dynamics in real time. We describe recent work in attosecond technology and investigations into materials such as Si, SiO2, GaN, Al2O3, Ti, TiO2, enabled by the convergence of these two capabilities. We showcase the state-of-the-art on isolated attosecond soft x-ray pulses for x-ray absorption near edge spectroscopy (XANES) to observe the 3d-state dynamics of the semi-metal TiS2 with attosecond resolution at the Ti L-edge (460 eV). We describe how the element- and state-specificity at the transition metal L-edge of the quantum material allows to unambiguously identify how and where the optical field influences charge carriers. This precision elucidates that the Ti:3d conduction band states are efficiently photo-doped to a density of 1.9 x 10^21 cm^-3 and that the light-field induces coherent motion of intra-band carriers across 38% of the first Brillouin zone. Lastly, we describe the prospects with such unambiguous real-time observation of carrier dynamics in specific bonding or anti-bonding states and speculate that such capability will bring unprecedented opportunities towards an engineered approach for designer materials with pre-defined properties and efficiency. Examples are composites of semiconductors and insulators like Si, Ge, SiO2, GaN, BN, quantum materials like graphene, TMDCs, or high-Tc superconductors like NbN or LaBaCuO. Exiting are prospects to scrutinize canonical questions in multi-body physics such as whether the electrons or lattice trigger phase transitions.

cond-mat.mtrl-sci↗

arXiv2018

Attosecond dispersive soft X-ray absorption fine structure spectroscopy in graphite

Phase transitions of solids and structural transformations of molecules are canonical examples of important photo-induced processes, whose underlying mechanisms largely elude our comprehension due to our inability to correlate electronic excitation with atomic position in real time. Here, we present a decisive step towards such new methodology based on water-window-covering (284 eV to 543 eV) attosecond soft X-ray pulses that can simultaneously access electronic and lattice parameters via dispersive X-ray absorption fine-structure (XAFS) spectroscopy. We validate attoXAFS with an identification of the σ* and π* orbital contributions to the density of states in graphite simultaneously with its lattice's four characteristic bonding distances. This work demonstrates the concept of attoXAFS as a powerful real-time investigative tool which is equally applicable to gas-, liquid- and condensed phase.

cond-mat.mtrl-sci↗

arXiv2017

Attosecond Streaking in the Water Window: A New Regime of Attosecond Pulse Characterization

We report on the first streaking measurement of water-window attosecond pulses generated via high harmonic generation, driven by sub-2-cycle, CEP-stable, 1850 nm laser pulses. Both the central photon energy and the energy bandwidth far exceed what has been demonstrated thus far, warranting the investigation of the attosecond streaking technique for the soft X-ray regime and the limits of the FROGCRAB retrieval algorithm under such conditions. We also discuss the problem of attochirp compensation and issues regarding much lower photo-ionization cross sections compared with the XUV in addition to the fact that several shells of target gases are accessed simultaneously. Based on our investigation, we caution that the vastly different conditions in the soft X-ray regime warrant a diligent examination of the fidelity of the measurement and the retrieval procedure.

physics.atom-ph↗