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Fulvio Parmigiani

Publications and source records attributed to Fulvio Parmigiani.

At least 19 recordsLinked to original sources

From the Light Quantum to the Photon: The Evolution of a Physical Concept

This work examines the physical and conceptual evolution of the light quantum from Planck's blackbody theory to the theoretical and experimental developments that led to the quantization of the electromagnetic field. The present study shows that the decisive transition occurred in Einstein's quantum theory of radiation (1916-1917). Absorption, stimulated emission, and spontaneous emission were formulated as elementary probabilistic mechanisms whose statistical balance alone reproduces the blackbody spectrum. In particular, spontaneous emission requires the emission of a light quantum, thereby implicitly proving its physical necessity before its theoretical status was clarified. At the same time, the already existing term photon began to acquire a stable usage following Lewis's 1926 proposal and became increasingly associated with Einstein's light quantum. By the mid-1920s, the central problem had shifted from whether light quanta were physically required to how radiation could be incorporated into the emerging quantum-mechanical formalism. This transition marks a key stage, illustrating how initial debates about the existence of light quanta gave way to their integration into a comprehensive theoretical structure. The resulting asymmetry between the novel quantum description of matter and the still-classical description of radiation, called into question by the phenomenon of spontaneous emission, identifies the physical problem that led to the quantization of the electromagnetic field.

physics.hist-ph

Ultrafast Two-Dimensional Spectroscopy Uncovers Ubiquitous Electron-Paramagnon Coupling in Cuprate Superconductors

The coupling between electronic excitations and collective bosonic modes is fundamental to the emergence of high-temperature superconductivity in cuprates. Despite extensive effort, conventional equilibrium and pump-probe optical spectroscopies still struggle to disentangle couplings to different bosonic modes when their energy scales overlap. Here we overcome this limitation using ultrafast two-dimensional electronic spectroscopy (2DES), which correlates coherent excitation and detection photon energies with femtosecond time resolution. Applied to optimally doped Bi$_2$Sr$_2$Ca$_{0.92}$Y$_{0.08}$Cu$_2$O$_{8+\delta}$, 2DES reveals a pronounced off-diagonal resonance arising from the ultrafast generation of non-thermal bosons with energy $\hbar\Omega_\mathbf{q}\simeq200$ meV. By comparing the measured spectra with a theoretical framework that explicitly includes the interaction between charge-transfer and magnetic excitations, we identify these bosons as paramagnons with momenta centered near $(\pi/2,\pi/2)$ and extending toward $(0,\pi)$ and $(\pi,0)$. The resonance persists across a large range of temperatures and doping concentrations, demonstrating that high-energy paramagnons are ubiquitously and strongly coupled to electronic excitations throughout the cuprate phase diagram. Time-domain analysis constrains the build-up of the paramagnon population to $\lesssim 10$ fs, placing a lower bound $\lambda \gtrsim 0.7$ on the coupling strength. More broadly, our results establish 2DES as a powerful approach for disentangling mode-selective electron-boson interactions and addressing decoherence dynamics, thereby establishing a new avenue for investigating strongly correlated quantum materials. These findings also provide a direct framework for future time-resolved resonant inelastic X-ray scattering experiments aimed at tracking the ultrafast dynamics of magnetic excitations.

cond-mat.supr-con

Photoinduced Electronic Band Dynamics and Defect-mediated Surface Potential Evolution in PdSe$_2$

We use time- and angle-resolved photoemission spectroscopy (TR-ARPES) combined with density functional theory to investigate ultrafast carrier dynamics in low-symmetry layered semiconducting PdSe$_2$. The indirect bandgap is determined to be 0.55~eV. Following photoexcitation above this gap, we resolve a valence band shift and broadening, both lasting less than a picosecond, consistent with bandgap renormalization and carrier scattering, indicative of strong many-body interactions. Subsequently, hot carriers populate the conduction band minimum and are captured by defect states. A surface photovoltage (SPV) of $\sim$ 67~meV emerges, persisting for over 50~ps, driven by defect-assisted charge separation. The formation of native vacancies, promoted by the low-symmetry lattice, likely gives rise to the mid-gap states responsible for this long-lived SPV response. Detailed analysis of TR-ARPES spectra disentangles the contributions of bandgap renormalization, carrier scattering, defect states, and SPV. These findings establish PdSe$_2$ as a prototypical layered quantum material exhibiting exotic photoresponses on ultrafast timescales.

cond-mat.mes-hall

Energy density driven ultrafast electronic excitations in a cuprate superconductor

Controlling nonequilibrium dynamics in quantum materials requires ultrafast probes with spectral selectivity. We report femtosecond reflectivity measurements on the cuprate superconductor Bi$_2$Sr$_2$CaCu$_2$O$_{8+\delta}$ using free-electron laser extreme-ultraviolet (23.5--177~eV) and near-infrared (1.5~eV) pump pulses. EUV pulses access deep electronic states, while NIR light excites valence-band transitions. Despite these distinct channels, both schemes produce nearly identical dynamics: above $T_c$, excitations relax through fast (100--300~fs) and slower (1--5~ps) channels; below $T_c$, a delayed component signals quasiparticle recombination and condensate recovery. We find that when electronic excitations are involved, the ultrafast response is governed mainly by absorbed energy rather than by the microscopic nature of the excitation. In contrast, bosonic driving in the THz or mid-infrared produces qualitatively different dynamics. By demonstrating that EUV excitation of a correlated superconductor yields macroscopic dynamics converging with those from optical pumping, this work defines a new experimental paradigm: FEL pulses at core-level energies provide a powerful means to probe and control nonequilibrium electronic states in quantum materials on their intrinsic femtosecond timescales. This establishes FEL-based EUV pumping as a new capability for ultrafast materials science, opening routes toward soft X-ray and attosecond studies of correlated dynamics.

cond-mat.supr-con

Ultrafast dynamics of vibronically dressed core-excitons in graphite: a femtosecond RIXS perspective

This study demonstrates one of the first implementations of time-resolved resonant inelastic X-ray scattering (tr-RIXS), marking a seminal extension of RIXS spectroscopy into the ultrafast time domain. By investigating the ultrafast dynamics of vibronically dressed core excitons in graphite using femtosecond X-ray pulses from a Free Electron Laser, we reveal previously inaccessible insights into the transient coupling between core excitons and specific optical phonon modes. Our approach establishes tr-RIXS as a powerful, transformative tool capable of elucidating the intricate interplay between electronic and lattice dynamics, opening new avenues in ultrafast materials research.

cond-mat.mtrl-sci

Quench of the electronic order in a strongly-coupled charge-density-wave system by enhanced lattice fluctuations

Charge-density-wave (CDW) materials having a strong electron-phonon coupling provide a powerful platform for investigating the intricate interplay between lattice fluctuations and a macroscopic quantum order. Using time- and angle-resolved photoemission spectroscopy (TR-ARPES), we reveal that the CDW gap closure in VTe2 is dominated by an incoherent process evolving on a sub-picosecond timescale, challenging the conventional view that the gap dynamics is primarily governed by the excitation of the CDW amplitude modes. Our findings, supported by a three-temperature model, show that the CDW gap evolution can be described by considering the population of a subset of strongly-coupled optical phonon modes, which leads to an increase in the lattice fluctuations. This microscopic framework extends beyond VTe2, offering a universal perspective for understanding the light-induced phase transition in strongly-coupled CDW systems.

cond-mat.str-el

Ultrafast Band Structure Dynamics in Bulk 1$T$-VSe$_2$

Complex materials encompassing different phases of matter can display new photoinduced metastable states differing from those attainable under equilibrium conditions. These states can be realized when energy is injected in the material following a non-equilibrium pathway, unbalancing the unperturbed energy landscape of the material. Guided by the fact that photoemission experiments allow for detailed insights in the electronic band structure of ordered systems, here we study bulk 1T-VSe$_2$ in its metallic and charge-density-wave phase by time- and angle-resolved photoelectron spectroscopy. After near-infrared optical excitation, the system shows a net increase of the density of states in the energy range of the valence bands, in the vicinity of the Fermi level, lasting for several picoseconds. We discuss possible origins as band shifts or correlation effects on the basis of a band structure analysis. Our results uncover the possibility of altering the electronic band structure of bulk 1T-VSe$_2$ for low excitation fluences, contributing to the understanding of light-induced electronic states.

cond-mat.str-el

Resonance-Induced Anomalies in Temperature-Dependent Raman Scattering of PdSe$_{2}$

We report a comprehensive Raman study of the phonon behaviour in PdSe$_2$ in the temperature range of 5 K to 300 K. A remarkable change in the Raman spectrum is observed at 120 K: a significant enhancement of the out-of-plane phonon A$^{1}_{g}$ mode, accompanied by a suppression of the in-plane A$^{2}_{g}$ and B$^{2}_{1g}$ modes. This intriguing behavior is attributed to a temperature-dependent resonant excitation effect. The results are supported by density functional theory (DFT) calculations, which demonstrate that the electron-phonon coupling for the phonon modes varies and is strongly associated with the relevant electronic states. Furthermore, nonlinear frequency shifts are identified in all modes, indicating the decay of an optical phonon into multiple acoustic phonons. The study of Raman emission reported here, complemented by linear optical spectroscopy, reveals an unexpected scenario for the vibrational properties of PdSe$_2$ that holds substantial promise for future applications in PdSe$_2$-based optoelectronics.

cond-mat.str-el

Impact of a $MoS_2$ monolayer on the nanoscale thermoelastic response of silicon heterostructures

Understanding the thermoelastic response of a nanostructure is crucial for the choice of materials and interfaces in electronic devices with improved and tailored transport properties, at the length scales of the present technology. Here we show how the deposition of a $MoS_2$ monolayer can strongly modify the nanoscale thermoelastic dynamics of silicon substrates close to their interface. We achieve this result by creating a transient grating with extreme ultraviolet light, using ultrashort free-electron laser pulses, whose $\approx$84 nm period is comparable to the size of elements typically used in nanodevices, such as electric contacts and nanowires. The thermoelastic response, featured by coherent acoustic waves and an incoherent relaxation, is tangibly modified by the presence of monolayer $MoS_2$. Namely, we observed a major reduction of the amplitude of the surface mode, which is almost suppressed, while the longitudinal mode is basically unperturbed, aside from a faster decay of the acoustic modulations. We interpret this behavior as a selective modification of the surface elasticity and we discuss the conditions to observe such effect, which might be of immediate relevance for the design of Si-based nanoscale devices.

cond-mat.mtrl-sci

Strain-induced enhancement of the charge-density-wave in the kagome metal ScV$_6$Sn$_6$

The kagome geometry is an example of frustrated configuration in which rich physics takes place, including the emergence of superconductivity and charge density wave (CDW). Among the kagome metals, ScV$_6$Sn$_6$ hosts an unconventional CDW, with its electronic order showing a different periodicity than that of the phonon which generates it. In this material, a CDW-softened flat phonon band has a second-order collapse at the same time that the first order transition occurs. This phonon band originates from the out-of-plane vibrations of the Sc and Sn atoms, and it is at the base of the electron-phonon-coupling driven CDW phase of ScV$_6$Sn$_6$. Here, we use uniaxial strain to tune the frequency of the flat phonon band, tracking the strain evolution via time-resolved optical spectroscopy and first-principles calculations. Our findings emphasize the capability to induce an enhancement of the unconventional CDW properties in ScV$_6$Sn$_6$ kagome metal through control of strain.

cond-mat.str-el

Unveiling the physics of the spin-orbit coupling at the surface of a model topological insulator: from theory to experiments

Spin-orbit interaction affects the band structure of topological insulators beyond the opening of an inverted gap in the bulk bands, and the understanding of its effects on the surface states is of primary importance to access the underlying physics of these exotic states. Here, we propose an $\textit{ab initio}$ approach benchmarked by pump-probe angle-resolved photoelectron spectroscopy data to model the effect of spin-orbit coupling on the surface states of a topological insulator. The critical novelty of our approach lies in the possibility of accounting for a partial transfer of the spin-orbit coupling to the surface states, mediated by the hybridization with the surface resonance states. In topological insulators, the fraction of transferred spin-orbit coupling influences the strength of the hexagonal warping of the surface states, which we use as a telltale of the capability of our model to reproduce the experimental dispersion. The comparison between calculations and measurements, of both the unoccupied and part of the occupied Dirac cone, indicates that the fraction of spin-orbit coupling transferred to the surface states by hybridization with the resonance states is between 70% and 85% of its full atomic value. This offers a valuable insight to improve the modeling of surface state properties in topological insulators for both scientific purposes and technological applications.

cond-mat.mes-hall

Reply to Comment on "Doppler signature in electrodynamic retarded potentials"

Calin Galeriu(CG) has commented [1] about our manuscript, "Doppler signature in electrodynamic retarded potentials" [2], that must be properly addressed, amending at the same time of notation errors [3] to clarify some formal aspects which were discussed and criticized in C. Galeriu's comments. The same author (CG) has published three papers concerning the origin of the Doppler term, v/c, in the Liénard-Wiechert (L-W) potentials [4-6].

physics.class-ph

Sub-nanosecond free carrier recombination in an indirectly excited quantum-well heterostructure

Nanometer-thick quantum-well structures are quantum model systems offering a few discrete unoccupied energy states that can be impulsively filled and that relax back to equilibrium predominantly via spontaneous emission of light. Here we report on the response of an indirectly excited quantum-well heterostructure, probed by means of time and frequency resolved photoluminescence spectroscopy. This experiment provides access to the sub-nanosecond evolution of the free electron density, indirectly injected in the quantum-wells. In particular, the modelling of the time-dependent photoluminescence spectra unveils the time evolution of the temperature and of the chemical potentials for electrons and holes, from which the sub-nanosecond time-dependent electron density is determined. This information allows to prove that the recombination of excited carriers is mainly radiative and bimolecular at early delays after excitation, while, as the carrier density decreases, a monomolecular and non-radiative recombination channel becomes relevant. Access to the sub-nanosecond chronology of the mechanisms responsible for the relaxation of charge carriers provides a wealth of information for designing novel luminescent devices with engineered spectral and temporal behavior.

cond-mat.mtrl-sci

Out-of-equilibrium charge redistribution in a copper-oxide based superconductor by time-resolved X-ray photoelectron spectroscopy

Charge-transfer excitations are of paramount importance for understanding the electronic structure of copper-oxide based high-temperature superconductors. In this study, we investigate the response of a Bi$_2$Sr$_2$CaCu$_2$O$_{\mathrm{8}+ δ}$ crystal to the charge redistribution induced by an infrared ultrashort pulse. Element-selective time-resolved core-level photoelectron spectroscopy with a high energy resolution allows disentangling the dynamics of oxygen ions with different coordination and bonds thanks to their different chemical shifts. Our experiment shows that the O\,$1s$ component arising from the Cu-O planes is significantly perturbed by the infrared light pulse. Conversely, the apical oxygen, also coordinated with Sr ions in the Sr-O planes, remains unaffected. This result highlights the peculiar behavior of the electronic structure of the Cu-O planes. It also unlocks the way to study the out-of-equilibrium electronic structure of copper-oxide-based high-temperature superconductors by identifying the O\,$1s$ core-level emission originating from the oxygen ions in the Cu-O planes. This ability could be critical to gain information about the strongly-correlated electron ultrafast dynamical mechanisms in the Cu-O plane in the normal and superconducting phases.

cond-mat.str-el

Photoinduced dynamics of flat bands in the kagome metal CoSn

CoSn is a prototypical kagome compound showing lattice-born flat bands with suppressed bandwidth over large parts of the Brillouin zone. Here, by means of time- and angle-resolved photoelectron spectroscopy, we provide direct evidence of the response to photoexcitation of the flat bands, that underlie information about localization in real space. In particular, we detect a sudden shift and broadening of the flat bands, while after one picosecond only a broadening survives. We ascribe both these effects to an ultrafast disruption of electron localization, which renormalizes the effective electron-electron interaction and affects the flat band dispersion. Since both variations are in the order of a few meV, our measurements suggest that the flat bands are resilient to near-infrared photoexcitation.

cond-mat.str-el

Ultrafast all-optical manipulation of the charge-density-wave in VTe$_{2}$

The charge-density wave (CDW) phase in the layered transition-metal dichalcogenide VTe$_{2}$ is strongly coupled to the band inversion involving vanadium and tellurium orbitals. In particular, this coupling leads to a selective disappearance of the Dirac-type states that characterize the normal phase, when the CDW phase sets in. Here, by means of broadband time-resolved optical spectroscopy (TR-OS), we investigate the ultrafast reflectivity changes caused by collective and single particle excitations in the CDW ground state of VTe$_{2}$. Remarkably, our measurements show the presence of two collective (amplitude) modes of the CDW ground state. By applying a double-pulse excitation scheme, we show the possibility to manipulate these modes, demonstrating a more efficient way to control and perturb the CDW phase in VTe$_{2}$.

cond-mat.str-el

Dynamics and Resilience of the Charge Density Wave in a bilayer kagome metal

Long-range electronic order descending from a metallic parent state constitutes a rich playground to study the intricate interplay of structural and electronic degrees of freedom. With dispersive and correlation features as multifold as topological Dirac-like itinerant states, van-Hove singularities, correlated flat bands, and magnetic transitions at low temperature, kagome metals are located in the most interesting regime where both phonon and electronically mediated couplings are significant. Several of these systems undergo a charge density wave (CDW) transition, and the van-Hove singularities, which are intrinsic to the kagome tiling, have been conjectured to play a key role in mediating such an instability. However, to date, the origin and the main driving force behind this charge order is elusive. Here, we use the topological bilayer kagome metal ScV6Sn6 as a platform to investigate this puzzling problem, since it features both kagome-derived nested Fermi surface and van-Hove singularities near the Fermi level, and a CDW phase that affects the susceptibility, the neutron scattering, and the specific heat, similarly to the siblings AV3Sb5 (A = K, Rb, Cs) and FeGe. We report on our findings from high-resolution angle-resolved photoemission, density functional theory, and time-resolved optical spectroscopy to unveil the dynamics of its CDW phase. We identify the structural degrees of freedom to play a fundamental role in the stabilization of charge order. Along with a comprehensive analysis of the subdominant impact from electronic correlations, we find ScV6Sn6 to feature an instance of charge density wave order that predominantly originates from phonons. As we shed light on the emergent phonon profile in the low-temperature ordered regime, our findings pave the way for a deeper understanding of ordering phenomena in all CDW kagome metals.

cond-mat.str-el

External screening and lifetime of exciton population in single-layer ReSe$_2$ probed by time- and angle-resolved photoemission spectroscopy

The semiconductor ReSe$_2$ is characterized by a strongly anisotropic optical absorption and is therefore promising as an optically active component in two-dimensional heterostructures. However, the underlying femtosecond dynamics of photoinduced excitations in such materials has not been sufficiently explored. Here, we apply an infrared optical excitation to single-layer ReSe$_2$ grown on a bilayer graphene substrate and monitor the temporal evolution of the excited state signal using time- and angle-resolved photoemission spectroscopy. We measure an optical gap of $(1.53 \pm 0.02)$ eV, consistent with resonant excitation of the lowest exciton state. The exciton distribution is tunable via the linear polarization of the pump pulse and exhibits a biexponential decay with time constants given by $τ_1 = (110 \pm 10)$ fs and $τ_2 = (650 \pm 70)$ fs, facilitated by recombination via an in-gap state that is pinned at the Fermi level. By extracting the momentum-resolved exciton distribution we estimate its real-space radial extent to be greater than 17.1 Å, implying significant exciton delocalization due to screening from the bilayer graphene substrate.

cond-mat.mes-hall