arXiv subjects

Federico Cilento

Publications and source records attributed to Federico Cilento.

At least 19 recordsLinked to original sources

arXiv2026

Spectroscopic signatures of persistent exciton condensation in a bulk magnetic topological insulator

Exciton condensates are long-sought correlated quantum states arising from macroscopic coherence of bound electron-hole pairs. Although equilibrium and transient excitonic states have been reported in several material platforms, direct evidence for a light-induced exciton condensate state has been challenging to achieve as an intrinsic property of a bulk quantum material. Here, we use time- and angle-resolved photoemission spectroscopy to investigate long-lived photoexcited carriers in the intrinsic magnetic topological insulator MnBi$_2$Te$_4$ with the chemical potential tuned to the topological surface state by Sb substitution. Following optical excitation, we observe the delayed emergence of a transient state whose formation coincides with depopulation of the bulk conduction band and whose lifetime extends to the microsecond timescale. The quasiparticle dispersion exhibits a pronounced flattening and develops a Mexican-hat-like profile. These spectral signatures are consistent with the formation of a metastable excitonic condensate state. Our results establish magnetic topological insulators as a promising platform for investigating long-lived photoinduced many-body states and their interplay with topology and magnetism.

cond-mat.mes-hall↗

arXiv2026

Robust spin splitting and fermiology in a layered altermagnet

Altermagnetism defies conventional classifications of collinear magnetic phases, standing apart from ferromagnetism and antiferromagnetism with its unique combination of spin-dependent symmetries, net-zero magnetization, and anomalous Hall transport. Although altermagnetic states have been realized experimentally, their integration into functional devices has been hindered by the structural rigidity and poor tunability of existing materials. First, through cobalt intercalation of the superconducting 2H-NbSe$_2$ polymorph, we induce and stabilize a robust altermagnetic phase and using both theory and experiment, we directly observe the lifting of Kramers degeneracy. Additionally, we present spectroscopic insight into a previously hinted low-temperature phase, and provide evidence of its electronic origin. While shedding light on overlooked aspects of altermagnetism, these findings open pathways to spin-based technologies and lay a foundation for advancing the emerging field of altertronics.

cond-mat.str-el↗

arXiv2026

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$_{8+δ}$ 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↗

arXiv2025

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↗

arXiv2025

Time-domain decoding of unconventional charge order mechanisms in nonmagnetic and magnetic kagome metals

In kagome lattice materials, quantum interplay between charge, spin, orbital, and lattice degrees of freedom gives rise to a remarkably rich set of emergent phenomena, ranging from unconventional charge order and superconductivity to topological magnetism. While the exact nature of these exotic orders is often challenging to comprehend in static experiments, time-resolved techniques can offer critical insights by disentangling coupled degrees of freedom on the time-axis. In this work, we demonstrate that the nature of charge orders in two representative kagome metals - nonmagnetic ScV6Sn6 and magnetic FeGe - which has been highly controversial in static studies, can be directly deciphered in the time-domain through their fundamentally distinct order parameter dynamics measured via time-resolved X-ray scattering at an X-ray free electron laser. In nonmagnetic ScV6Sn6, the dynamics are characterized by ultrafast melting and coherent amplitudon oscillations, typical of a phonon-coupled charge order. In stark contrast, magnetic FeGe exhibits resilient metastable charge order dynamics, hitherto unobserved in any other charge-ordered system - this unique time-domain behavior directly signifies an unconventional magnetism-interlocked charge order state realized in this kagome magnet. Our results not only provide a model case where unconventional nature of electronic order, hidden in equilibrium, is directly unraveled in the time-domain, but also pave the way for future out-of-equilibrium engineering of novel quantum orders in kagome lattice platforms.

cond-mat.str-el↗

arXiv2025

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↗

arXiv2025

Pump-driven opto-magnetic properties in semiconducting transition-metal dichalcogenides: an analytical model

Single-layer transition-metal dichalcogenides provide an unique intrinsic entanglement between the spin/valley/orbital degrees of freedom and the polarization of scattered photons. This scenario gives rise to the well-assessed optical dichroism observed by using both steady and time-resolved probes. In this paper we provide a compact analytical modelling of the onset of a finite Faraday/Kerr optical rotation upon shining with a circularly polarized light. We identify different optical features displaying optical rotation at different characteristic energies, and we describe in an analytical framework the time-dependence of their intensities as a consequence of the main spin-conserving and spin-flip processes.

cond-mat.mtrl-sci↗

arXiv2024

Unveiling exciton formation: exploring the early stages in time, energy and momentum domain

Resolving the early-stage dynamics of exciton formation following non-resonant photoexcitation in time, energy, and momentum is quite challenging due to their inherently fast timescales and the proximity of the excitonic state to the bottom of the conduction band. In this study, by combining time- and angle-resolved photoemission spectroscopy with \mathit{ab initio} numerical simulations, we capture the timing of the early-stage exciton dynamics in energy and momentum, starting from the photoexcited population in the conduction band, progressing through the formation of free excitons, and ultimately leading to their trapping in lattice deformations. The chosen material is bismuth tri-iodide ($BiI_3$), a layered semiconductor with a rich landscape of excitons in the electronic structure both in bulk and in monolayer form. The obtained results, providing a full characterization of the exciton formation, elucidate the early stages of the physical phenomena underlying the operation of the ultrafast semiconductor device.

cond-mat.mtrl-sci↗

arXiv2024

Van der Waals engineering of ultrafast carrier dynamics in magnetic heterostructures

Heterostructures composed of the intrinsic magnetic topological insulator MnBi$_2$Te$_4$ and its non-magnetic counterpart Bi$_2$Te$_3$ host distinct surface electronic band structures depending on the stacking order and exposed termination. Here, we probe the ultrafast dynamical response of MnBi$_2$Te$_4$ and MnBi$_4$Te$_7$ following near-infrared optical excitation using time- and angle-resolved photoemission spectroscopy, and disentangle surface from bulk dynamics based on density functional theory slab calculations of the surface-projected electronic structure. We gain access to the out-of-equilibrium charge carrier populations of both MnBi$_2$Te$_4$ and Bi$_2$Te$_3$ surface terminations of MnBi$_4$Te$_7$, revealing an instantaneous occupation of states associated with the Bi$_2$Te$_3$ surface layer followed by carrier extraction into the adjacent MnBi$_2$Te$_4$ layers with a laser fluence-tunable delay of up to 350 fs. The ensuing thermal relaxation processes are driven by phonon scattering with significantly slower relaxation times in the magnetic MnBi$_2$Te$_4$ septuple layers. The observed competition between interlayer charge transfer and intralayer phonon scattering demonstrates a method to control ultrafast charge transfer processes in MnBi$_2$Te$_4$-based van der Waals compounds.

cond-mat.mtrl-sci↗

arXiv2024

Ultrafast light-driven optical rotation and hidden orders in bulk WSe$_2$

Single-layer semiconducting transition-metal dichalcogenides, lacking point inversion symmetry, provide an efficient platform for valleytronics, where the electronic, magnetic, valley and lattice degrees of freedom can be selectively manipulated by using polarized light. This task is however thought to be limited in parent bulk compounds where the point inversion symmetry is restored. Exploiting the underlying quantum physics in bulk materials is thus one of the biggest paradigmatic challenges. Here we show that a sizable optical Kerr rotation can be efficiently generated in a wide energy range on ultrafast timescales in bulk WSe$_2$, by means of circularly-polarized light. We rationalize these findings as a result of the hidden spin/layer/valley quantum entanglement. The spectral analysis reveals clear features at the three characteristic frequencies corresponding to the A-, B- and C-exciton edges. The origin and the relative sign of all these features is shown to stem from the selective Pauli blocking of intralayer and interlayer optical transitions. The long lifetime of the broadband Kerr response ($τ\sim 500$ fs) provides a strong indication that coupled photo-induced electron and hole densities survive in bulk compounds longer than previously expected. The present report demonstrates that a hidden quantum entanglement is operative also in bulk centrosymmetric layered materials, opening the way for an effective exploitation of bulk WSe$_2$ in optoelectronic applications.

cond-mat.mes-hall↗

arXiv2024

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↗

arXiv2024

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↗

arXiv2024

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↗

arXiv2024

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↗

arXiv2023

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↗

arXiv2023

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↗

arXiv2023

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↗

arXiv2023

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↗