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Fulvio Parmigiani

Publications and source records attributed to Fulvio Parmigiani.

At least 55 records · Page 3Linked to original sources

Interband characterization and electronic transport control of nanoscaled GeTe/Sb$_2$Te$_3$ superlattices

The extraordinary electronic and optical properties of the crystal-to-amorphous transition in phase-change materials led to important developments in memory applications. A promising outlook is offered by nanoscaling such phase-change structures. Following this research line, we study the interband optical transmission spectra of nanoscaled GeTe/Sb$_2$Te$_3$ chalcogenide superlattice films. We determine, for films with varying stacking sequence and growth methods, the density and scattering time of the free electrons, and the characteristics of the valence-to-conduction transition. It is found that the free electron density decreases with increasing GeTe content, for sub-layer thickness below $\sim$3 nm. A simple band model analysis suggests that GeTe and Sb$_2$Te$_3$ layers mix, forming a standard GeSbTe alloy buffer layer. We show that it is possible to control the electronic transport properties of the films by properly choosing the deposition layer thickness and we derive a model for arbitrary film stacks.

cond-mat.mes-hall↗

Insights into ultrafast Ge-Te bond dynamics in a phase-change superlattice

A long-standing question for avant-grade data storage technology concerns the nature of the ultrafast photoinduced phase transformations in the wide class of chalcogenide phase-change materials (PCMs). Overall, a comprehensive understanding of the microstructural evolution and the relevant kinetics mechanisms accompanying the out-of-equilibrium phases is still missing. Here, after overheating a phase-change chalcogenide superlattice by an ultrafast laser pulse, we indirectly track the lattice relaxation by time resolved X-ray absorption spectroscopy (tr-XAS) with a sub-ns time resolution. The novel approach to the tr-XAS experimental results reported in this work provides an atomistic insight of the mechanism that takes place during the cooling process, meanwhile a first-principles model mimicking the microscopic distortions accounts for a straightforward representation of the observed dynamics. Finally, we envisage that our approach can be applied in future studies addressing the role of dynamical structural strain in phase-change materials.

cond-mat.mtrl-sci↗

Ultrafast optical spectroscopy of strongly correlated materials and high-temperature superconductors: a non-equilibrium approach

In the last two decades, non-equilibrium spectroscopies have evolved from avant-garde studies to crucial tools for expanding our understanding of the physics of strongly correlated materials. The possibility of obtaining simultaneously spectroscopic and temporal information has led to insights that are complementary to (and in several cases beyond) those attainable by studying the matter at equilibrium. Multiple phase transitions and new orders arising from competing interactions are benchmark examples where the interplay among electrons, lattice, and spin dynamics can be disentangled because of the different timescales that characterize the recovery of the initial ground state. The nature of the broken-symmetry phases and of the bosonic excitations that mediate the electronic interactions, eventually leading to superconductivity or other exotic states, can be revealed by observing the sub-picosecond dynamics of impulsively excited states. Recent experimental developments have made possible to monitor the time-evolution of both the single-particle and collective excitations under extreme conditions, such as those arising from strong and selective photo-stimulation. Here, we review the most recent achievements in the experimental and theoretical studies of the non-equilibrium electronic, optical, structural and magnetic properties of correlated materials. The focus will be mainly on the prototypical case of correlated oxides that exhibit unconventional superconductivity or other exotic phases, even though the discussion will extend also to other topical systems. The necessity of extending the actual experimental capabilities and the numerical and analytic tools to microscopically treat the non-equilibrium phenomena beyond the simple phenomenological approaches represents one of the most challenging new frontier in physics.

cond-mat.supr-con↗

Photon number statistics uncover the fluctuations in non-equilibrium lattice dynamics

Fluctuations of the atomic positions are at the core of a large class of unusual material properties ranging from quantum para-electricity to high temperature superconductivity. Their measurement in solids is the subject of an intense scientific debate focused on seeking a methodology capable of establishing a direct link between the variance of the atomic displacements and experimentally measurable observables. Here we address this issue by means of non-equilibrium optical experiments performed in shot-noise limited regime. The variance of the time dependent atomic positions and momenta is directly mapped into the quantum fluctuations of the photon number of the scattered probing light. A fully quantum description of the non-linear interaction between photonic and phononic fields is benchmarked by unveiling the squeezing of thermal phonons in $α$-quartz.

quant-ph↗

Ultrafast Electron Dynamics in Epitaxial Graphene Investigated with Time- and Angle-Resolved Photoemission Spectroscopy

In order to exploit the intriguing optical properties of graphene it is essential to gain a better understanding of the light-matter interaction in the material on ultrashort timescales. Exciting the Dirac fermions with intense ultrafast laser pulses triggers a series of processes involving interactions between electrons, phonons and impurities. Here we study these interactions in epitaxial graphene supported on silicon carbide (semiconducting) and iridium (metallic) substrates using ultrafast time- and angle-resolved photoemission spectroscopy (TR-ARPES) based on high harmonic generation. For the semiconducting substrate we reveal a complex hot carrier dynamics that manifests itself in an elevated electronic temperature and an increase in linewidth of the $π$ band. By analyzing these effects we are able to disentangle electron relaxation channels in graphene. On the metal substrate this hot carrier dynamics is found to be severely perturbed by the presence of the metal, and we find that the electronic system is much harder to heat up than on the semiconductor due to screening of the laser field by the metal.

cond-mat.str-el↗

Tunable Carrier Multiplication and Cooling in Graphene

Time- and angle-resolved photoemission measurements on two doped graphene samples displaying different doping levels reveal remarkable differences in the ultrafast dynamics of the hot carriers in the Dirac cone. In the more strongly ($n$-)doped graphene, we observe larger carrier multiplication factors ($>$ 3) and a significantly faster phonon-mediated cooling of the carriers back to equilibrium compared to in the less ($p$-)doped graphene. These results suggest that a careful tuning of the doping level allows for an effective manipulation of graphene's dynamical response to a photoexcitation.

cond-mat.mtrl-sci↗

Phase separation in the non-equilibrium Verwey transition in magnetite

We present equilibrium and out-of-equilibrium studies of the Verwey transition in magnetite. In the equilibrium optical conductivity, we find a step-like change at the phase transition for photon energies below about 2 eV. The possibility of triggering a non-equilibrium transient metallic state in insulating magnetite by photo excitation was recently demonstrated by an x-ray study. Here we report a full characterization of the optical properties in the visible frequency range across the non-equilibrium phase transition. Our analysis of the spectral features is based on a detailed description of the equilibrium properties. The out-of-equilibrium optical data bear the initial electronic response associated to localized photo-excitation, the occurrence of phase separation, and the transition to a transient metallic phase for excitation density larger than a critical value. This allows us to identify the electronic nature of the transient state, to unveil the phase transition dynamics, and to study the consequences of phase separation on the reflectivity, suggesting a spectroscopic feature that may be generally linked to out-of-equilibrium phase separation.

cond-mat.str-el↗

Symmetry of the Fermi surface and evolution of the electronic structure across the paramagnetic-helimagnetic transition in MnSi/Si(111)

MnSi has been extensively studied for five decades, nonetheless detailed information on the Fermi surface (FS) symmetry is still lacking. This missed information prevented from a comprehensive understanding the nature of the magnetic interaction in this material. Here, by performing angle-resolved photoemission spectroscopy on high-quality MnSi films epitaxially grown on Si(111), we unveil the FS symmetry and the evolution of the electronic structure across the paramagnetic-helimagnetic transition at T$_C$ $\sim$ 40 K, along with the appearance of sharp quasiparticle emission below T$_C$. The shape of the resulting FS is found to fulfill robust nesting effects. These effects can be at the origin of strong magnetic fluctuations not accounted for by state-of-art quasiparticle self-consistent GW approximation. From this perspective, the unforeseen quasiparticle damping detected in the paramagnetic phase and relaxing only below T$_C$, along with the persistence of the d-bands splitting well above T$_C$, at odds with a simple Stoner model for itinerant magnetism, open the search for exotic magnetic interactions favored by FS nesting and affecting the quasiparticles lifetime.

cond-mat.str-el↗

Ramifications of Optical Pumping on the Interpretation of Time-Resolved Photoemission Experiments on Graphene

In pump-probe time and angle-resolved photoemission spectroscopy (TR-ARPES) experiments the presence of the pump pulse adds a new level of complexity to the photoemission process in comparison to conventional ARPES. This is evidenced by pump-induced vacuum space-charge effects and surface photovoltages, as well as multiple pump excitations due to internal reflections in the sample-substrate system. These processes can severely affect a correct interpretation of the data by masking the out-of-equilibrium electron dynamics intrinsic to the sample. In this study, we show that such effects indeed influence TR-ARPES data of graphene on a silicon carbide (SiC) substrate. In particular, we find a time- and laser fluence-dependent spectral shift and broadening of the acquired spectra, and unambiguously show the presence of a double pump excitation. The dynamics of these effects is slower than the electron dynamics in the graphene sample, thereby permitting us to deconvolve the signals in the time domain. Our results demonstrate that complex pump-related processes should always be considered in the experimental setup and data analysis.

cond-mat.str-el↗

Photo-enhanced antinodal conductivity in the pseudogap state of high Tc cuprates

A major challenge in understanding the cuprate superconductors is to clarify the nature of the fundamental electronic correlations that lead to the pseudogap phenomenon. Here we use ultrashort light pulses to prepare a non-thermal distribution of excitations and capture novel properties that are hidden at equilibrium. Using a broadband (0.5-2 eV) probe we are able to track the dynamics of the dielectric function, unveiling an anomalous decrease of the scattering rate of the charge carriers in a pseudogap-like region of the temperature ($T$) and hole-doping ($p$) phase diagram. In this region, delimited by a well-defined $T^*_{neq}(p)$ line, the photo-excitation process triggers the evolution of antinodal excitations from gapped (localized) to delocalized quasi-particles characterized by a longer lifetime. The novel concept of photo-enhanced antinodal conductivity is naturally explained within the single-band Hubbard model, in which the short-range Coulomb repulsion leads to a k-space differentiation between "nodal" quasiparticles and antinodal excitations.

cond-mat.str-el↗

Witnessing the formation and relaxation of massive quasi-particles in a strongly correlated electron system

The non-equilibrium semiconductors physics is based on the paradigm that different degrees of freedom interact on different timescales. In this context the photo-excitation is often treated as an impulsive injection of electronic energy that is transferred to other degrees of freedom only at later times. Here, by studying the ultrafast particles dynamics in a archetypal strongly correlated charge-transfer insulator (La2CuO4), we show that the interaction between electrons and bosons manifest itself directly in the photo-excitation processes of a correlated material. With the aid of a general theoretical framework (Hubbard Holstein Hamiltonian), we reveal that sub-gap excitation pilots the formation of itinerant quasi-particles which are suddently dressed (<100 fs) by an ultrafast reaction of the bosonic field.

cond-mat.str-el↗

Ultrafast Dynamics of Massive Dirac Fermions in Bilayer Graphene

Bilayer graphene is a highly promising material for electronic and optoelectronic applications since it is supporting massive Dirac fermions with a tuneable band gap. However, no consistent picture of the gap's effect on the optical and transport behavior has emerged so far, and it has been proposed that the insulating nature of the gap could be compromised by unavoidable structural defects, by topological in-gap states, or that the electronic structure could be altogether changed by many-body effects. Here we directly follow the excited carriers in bilayer graphene on a femtosecond time scale, using ultrafast time- and angle-resolved photoemission. We find a behavior consistent with a single-particle band gap. Compared to monolayer graphene, the existence of this band gap leads to an increased carrier lifetime in the minimum of the lowest conduction band. This is in sharp contrast to the second sub-state of the conduction band, in which the excited electrons decay through fast, phonon-assisted inter-band transitions.

cond-mat.mes-hall↗

Pulsed homodyne Gaussian quantum tomography with low detection efficiency

Pulsed homodyne quantum tomography usually requires a high detection efficiency limiting its applicability in quantum optics. Here, it is shown that the presence of low detection efficiency ($<50\%$) does not prevent the tomographic reconstruction of quantum states of light, specifically, of Gaussian type. This result is obtained by applying the so-called "minimax" adaptive reconstruction of the Wigner function to pulsed homodyne detection. In particular, we prove, by both numerical and real experiments, that an effective discrimination of different Gaussian quantum states can be achieved. Our finding paves the way to a more extensive use of quantum tomographic methods, even in physical situations in which high detection efficiency is unattainable.

physics.optics↗

Direct view on the ultrafast carrier dynamics in graphene

The ultrafast dynamics of excited carriers in graphene is closely linked to the Dirac spectrum and plays a central role for many electronic and optoelectronic applications. Harvesting energy from excited electron-hole pairs, for instance, is only possible if these pairs can be separated before they lose energy to vibrations, merely heating the lattice. While the hot carrier dynamics in graphene could so far only be accessed indirectly, we here present a direct time-resolved view on the Dirac cone by angle-resolved photoemission (ARPES). This allows us to show the quasi-instant thermalisation of the electron gas to a temperature of more than 2000 K; to determine the time-resolved carrier density; to disentangle the subsequent decay into excitations of optical phonons and acoustic phonons (directly and via supercollisions); and to show how the presence of the hot carrier distribution affects the lifetime of the states far below the Fermi energy.

cond-mat.mes-hall↗

In search for the pairing glue in cuprates by non-equilibrium optical spectroscopy

In strongly correlated materials the electronic and optical properties are significantly affected by the coupling of fermionic quasiparticles to different degrees of freedom, such as lattice vibrations and bosonic excitations of electronic origin. Broadband ultrafast spectroscopy is emerging as the premier technique to unravel the subtle interplay between quasiparticles and electronic or phononic collective excitations, by their different characteristic timescales and spectral responses. By investigating the femtosecond dynamics of the optical properties of Y-Bi2212 crystals over the 0.5-2 eV energy range, we disentangle the electronic and phononic contributions to the generalized electron-boson Eliashberg function, showing that the spectral distribution of the electronic excitations, such as spin fluctuations and current loops, and the strength of their interaction with quasiparticles can account for the high critical temperature of the superconducting phase transition. Finally, we discuss how the use of this technique can be extended to the underdoped region of the phase diagram of cuprates, in which a pseudogap in the quasiparticle density of states opens. The microscopic modeling of the interaction of ultrashort light pulses with unconventional superconductors will be one of the key challenges of the next-years materials science, eventually leading to the full understanding of the role of the electronic correlations in controlling the dynamics on the femtosecond timescale.

cond-mat.supr-con↗

Mixed regime of light-matter interaction revealed by phase sensitive measurements of the dynamical Franz-Keldysh effect

The speed of ultra-fast optical switches is generally limited by the intrinsic electronic response time of the material. Here we show that the phase content of selected electromagnetic pulses can be used to measure the timescales characteristic for the different regimes of matter-light interactions. By means of combined single cycle THz pumps and broadband optical probes, we explore the field-induced opacity in GaAs (the Franz-Keldysh effect). Our phase-resolved measurements allow to identify a novel quasi-static regime of saturation where memory effects are of relevance.

physics.optics↗

Evidence of vectorial photoelectric effect on Copper

Quantum Efficiency (QE) measurements of single photon photoemission from a Cu(111) single crystal and a Cu polycrystal photocathodes, irradiated by 150 fs-6.28 eV laser pulses, are reported over a broad range of incidence angle, both in s and p polarizations. The maximum QE (\simeq 4\times10^{-4}) for polycrystalline Cu is obtained in p polarization at an angle of incidence θ = 65deg. We observe a QE enhancement in p polarization which can not be explained in terms of optical absorption, a phenomenon known as vectorial photoelectric effect. Issues concerning surface roughness and symmetry considerations are addressed. An explanation in terms of non local conductivity tensor is proposed.

cond-mat.mtrl-sci↗

Experimental evidence of above-threshold photoemission in solids

Nonlinear photoemission from a silver single crystal is investigated by femtosecond laser pulses in a perturbative regime. A clear observation of above-threshold photoemission in solids is reported for the first time. The ratio between the three-photon above-threshold and the two-photon Fermi edges is found to be 10^{-4}. This value constitutes the only available benchmark for theories aimed at understanding the mechanism responsible for above-threshold photoemission in solids.

cond-mat.mtrl-sci↗