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Daniele Fausti

Publications and source records attributed to Daniele Fausti.

At least 37 records · Page 2Linked to original sources

Signature of an Ultrafast Photo-Induced Lifshitz Transition in the Nodal-Line Semimetal ZrSiTe

Here we report an ultrafast optical spectroscopic study of the nodal-line semimetal ZrSiTe. Our measurements reveal that, converse to other compounds of the family, the sudden injection of electronic excitations results in a strongly coherent response of an $A_{1g}$ phonon mode which dynamically modifies the distance between Zr and Te atoms and Si layers. "Frozen phonon" DFT calculations, in which band structures are calculated as a function of nuclear position along the phonon mode coordinate, show that large displacements along this mode alter the material's electronic structure significantly, forcing bands to approach and even cross the Fermi energy. The incoherent part of the time domain response reveals that a delayed electronic response at low fluence discontinuously evolves into an instantaneous one for excitation densities larger than $3.43 \times 10^{17}$ cm$^{-3}$. This sudden change of the dissipative channels for electronic excitations is indicative of an ultrafast Lifshitz transition which we tentatively associate to a change in topology of the Fermi surface driven by a symmetry preserving $A_{1g}$ phonon mode.

cond-mat.mtrl-sci↗

Visible pump -- mid infrared pump -- broadband probe: development and characterization of a three-pulse setup for single-shot ultrafast spectroscopy at 50 kHz

We report here an experimental setup to perform three-pulse pump-probe measurements over a wide wavelength and temperature range. By combining two pump pulses in the visible (650-900 nm) and mid-IR (5-20 $μ$m) range, with a broadband supercontinuum white-light probe, our apparatus enables both the combined selective excitation of different material degrees of freedom and a full time-dependent reconstruction of the non-equilibrium dielectric function of the sample. We describe here the optical setup, the cryogenic sample environment and the custom-made acquisition electronics capable of referenced single-pulse detection of broadband spectra at the maximum repetition rate of 50 kHz, achieving a sensitivity of the order of 10$^{-4}$ over an integration time of 1 s. We demonstrate the performance of the setup by reporting data on mid-IR pump, optical push and broadband probe in a single-crystal of Bi$_2$Sr$_2$Y$_{0.08}$Ca$_{0.92}$Cu$_2$O$_{8+δ}$ across the superconducting and pseudogap phases.

physics.optics↗

Transient Drude Response Dominates Near-Infrared Pump-Probe Reflectivity in Nodal-Line Semimetals ZrSiS and ZrSiSe

The ultrafast optical response of two nodal-line semimetals, ZrSiS and ZrSiSe, was studied in the near-infrared using transient reflectivity. The two materials exhibit similar responses, characterized by two features, well resolved in time and energy. The first transient feature decays after a few hundred femtoseconds, while the second lasts for nanoseconds. Using Drude-Lorentz fits of the materials' equilibrium reflectance, we show that the fast response is well-represented by a decrease of the Drude plasma frequency, and the second feature by an increase of the Drude scattering rate. This directly connects the transient data to a physical picture in which carriers, after being excited away from the Fermi energy, return to that vicinity within a few hundred femtoseconds by sharing their excess energy with the phonon bath, resulting in a hot lattice that relaxes only through slow diffusion processes (ns). The emerging picture reveals that the sudden change of the density of carriers at the Fermi level instantaneously modifies the transport properties of the materials on a timescale not compatible with electron phonon thermalization and is largely driven by the reduced density of states at the nodal line.

cond-mat.mtrl-sci↗

Time-resolved multimode heterodyne detection for dissecting coherent states of matter

Unveiling and controlling the coherent evolution of low energy states is a key to attain light driven new functionalities of materials. Here we investigate the coherent evolution of non-equilibrium photon-phonon Raman interactions in the low photon number regime via femtosecond time-resolved multimode heterodyne detection. The time dependence of the weak probe spectral components is revealed by interferential amplification with shaped phase-locked reference fields that allow for a frequency selective amplification. We report measurements on $α$-quartz that show that both amplitude and phase of the probe spectral components are modulated at the phonon frequency, but encode qualitatively different responses which are representative respectively of the time dependent position and momentum of the atoms. We stress that the sensitivity achieved here (1-10 photons per pulse) may be of relevance for both quantum information technologies and time domain studies on photosensitive materials.

physics.app-ph↗

Vibrational coherent control of localized d-d electronic excitation

Addressing the role of quantum coherence in the interplay between the different matter constituents (electrons, phonons and spin) is a critical step towards understanding transition metal oxides and design complex materials with new functionalities. Here we use coherent vibrational control of onsite d-d electronic transitions in a model edge-sharing insulating transition metal oxide (CuGeO3) to single-out the effects of vibrational coherence in electron-phonon coupling. By comparing time domain experiments based on high and low frequency ultrashort pumps with a fully quantum description of phonon assisted absorption, we could distinguish the processes associated to incoherent thermal lattice fluctuations from those driven by the coherent motion of the atoms. In particular, while thermal fluctuation of the phonon bath uniformly increases the electronic absorption, the resonant excitation of phonon modes results also in light-induced transparency which is coherently controlled by the vibrational motion.

cond-mat.mtrl-sci↗

Quantum model for Impulsive Stimulated Raman Scattering

The interaction between ultrashort light pulses and non-absorbing materials is dominated by Impulsive Stimulated Raman Scattering (ISRS). The description of ISRS in the context of pump\&probe experiments is based on effective classical models describing the interaction between the phonon and pulsed electromagnetic fields. Here we report a theoretical description of ISRS where we do not make any semi-classical approximation and we treat both photonic and phononic degrees of freedom at the quantum level. The results of the quantum model are compared with semiclassical results and validated by means of spectrally resolved pump\&probe measurements on $α$-quartz.

quant-ph↗

Signatures of enhanced superconducting phase coherence through MID-IR excitation in optimally doped Y-Bi2212

Optimally doped cuprate superconductors are characterized by the presence of superconducting fluctuations in a relatively large temperature region above the critical transition temperature. We reveal here that the effect of thermal disorder, which decreases the condensate phase coherence at equilibrium, can be dynamically contrasted by photoexcitation with ultrashort mid-infrared pulses. In particular, our findings reveal that light pulses with photon energy comparable to the amplitude of the superconducting gap and polarized in plane along the copper-copper direction [110] can dynamically enhance the optical response which is associated to the onset of superconductivity. We propose that this effect could be rationalized by an effective d-wave BCS model, which reveals that mid-infrared pulses result in a transient increase of the phase coherence.

cond-mat.str-el↗

Localised vibrations in superconducting YBCO revealed by ultra-fast optical coherent spectroscopy

The interaction between phonons and high-energy excitations of electronic origin in cuprates and their role in the superconducting mechanisms is still controversial. Here we use coherent vibrational time-domain spectroscopy together with density functional and dynamical mean-field theory calculations to establish a direct link between the c-axis phonon modes and the in-plane electronic charge excitations in optimally doped YBCO. The non-equilibrium Raman tensor is measured by means of the broadband 'coherent-phonon' response in pump-probe experiments and is qualitatively described by our model using DFT in frozen phonon approximation plus single band DMFT to account for the electronic correlations. The major outcome of our experimental and theoretical study is to establish the link between out-of-plane copper ions displacements and the in-plane electronic correlations, and to estimate at few unit cells the correlation length of the associated phonon mode. The approach introduced here could help revealing the complex interplay between fluctuations of different nature and spatial correlation in several strongly-correlated materials.

cond-mat.str-el↗

Probing the fluctuations of the optical properties in time-resolved spectroscopy

We show that, in optical pump-probe experiments on bulk samples, the statistical distribution of the intensity of ultrashort light pulses after the interaction with a nonequilibrium complex material can be used to measure the time-dependent noise of the current in the system. We illustrate the general arguments for a photo-excited Peierls material. The transient noise spectroscopy allows to measure to what extent electronic degrees of freedom dynamically obey the fluctuation-dissipation theorem, and how well they thermalize during the coherent lattice vibrations. The proposed statistical measurement developed here provides a new general framework to retrieve dynamical information on the excited distributions in nonequilibrium experiments which could be extended to other degrees of freedom of magnetic or vibrational origin.

cond-mat.str-el↗

Bypassing the energy-time uncertainty in time-resolved photoemission

The energy-time uncertainty is an intrinsic limit for time-resolved experiments imposing a tradeoff between the duration of the light pulses used in experiments and their frequency content. In standard time-resolved photoemission, this limitation maps directly onto a tradeoff between the time resolution of the experiment and the energy resolution that can be achieved on the electronic spectral function. Here we propose a protocol to disentangle the energy and time resolutions in photoemission. We demonstrate that dynamical information on all time scales can be retrieved from time-resolved photoemission experiments using suitably shaped light pulses of quantum or classical nature. As a paradigmatic example, we study the dynamical buildup of the Kondo peak, a narrow feature in the electronic response function arising from the screening of a magnetic impurity by the conduction electrons. After a quench, the electronic screening builds up on timescales shorter than the inverse width of the Kondo peak and we demonstrate that the proposed experimental scheme could be used to measure the intrinsic time scales of such electronic screening. The proposed approach provides an experimental framework to access the nonequilibrium response of collective electronic properties beyond the spectral uncertainty limit and will enable the direct measurement of phenomena such as excited Higgs modes and, possibly, the retarded interactions in superconducting systems.

cond-mat.str-el↗

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↗

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↗

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↗

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↗

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↗

Hubbard exciton revealed by time-domain optical spectroscopy

We use broadband ultra-fast pump-probe spectroscopy in the visible range to study the lowest excitations across the Mott-Hubbard gap in the orbitally ordered insulator YVO3. Separating thermal and non-thermal contributions to the optical transients, we show that the total spectral weight of the two lowest peaks is conserved, demonstrating that both excitations correspond to the same multiplet. The pump-induced transfer of spectral weight between the two peaks reveals that the low-energy one is a Hubbard exciton, i.e. a resonance or bound state between a doublon and a holon. Finally, we speculate that the pump-driven spin-disorder can be used to quantify the kinetic energy gain of the excitons in the ferromagnetic phase.

cond-mat.str-el↗