arXiv subjects

Fabio Novelli

Publications and source records attributed to Fabio Novelli.

15 recordsLinked to original sources

arXiv2026

Hydrogen-Bond Donor-Acceptor Imbalance in Low-Frequency Terahertz Water Spectra

The low-frequency dielectric response of liquid water is commonly described by a dominant Debye relaxation together with additional faster contributions whose microscopic origin remains debated. Here we show that the dielectric function of water between 0.14 and 1.21 THz can be represented by a collective Debye relaxation plus a Drude-Smith term constrained to the zero-dc-conductivity limit. The Drude-Smith spectral weight increases upon heating pure H2O from 20 C to 50 C and decreases upon isotopic substitution (D2O at 20 C vs. H2O at 20 C). Molecular dynamics simulations including nuclear quantum effects show correlated changes in the population of water molecules with unequal numbers of donated and accepted hydrogen-bonds. Ab-initio-based spectra calculations further indicate that the ~0.1-1 THz response contains both nuclear-motion and explicit electronic-polarisation/charge-redistribution contributions. We therefore interpret the excess low-frequency THz response as a localised, mixed nuclear-electronic dielectric response correlated with transient donor-acceptor imbalance in the hydrogen-bond network.

physics.chem-ph↗

arXiv2026

Cavity-enhanced superconducting response in an underdoped cuprate

Superconductors carry electrical current without resistance when paired electrons condense into a coherent macroscopic quantum state. In underdoped cuprates, evidence suggests that pairing-related correlations and superconducting fluctuations can survive above the temperature at which global coherence is lost, pointing to phase fluctuations as a key limitation on superconductivity in this regime. Motivated by recent demonstrations of cavity-modified collective states in quantum materials, we investigate whether superconducting coherence can be stabilized by engineering the electromagnetic environment of the superconductor. We study an underdoped YBa$_2$Cu$_3$O$_{7-\delta}$ thin film in a tunable terahertz cavity formed with a semi-transparent gold mirror. From temperature-dependent terahertz transmission measurements, we find that the cavity enhances the superconducting response below the critical temperature, with an increase of the inferred superfluid weight. The effect becomes more pronounced at smaller cavity lengths and is accompanied by an upward shift of the superconducting onset temperature. Calculations based on a cavity-coupled model for phase-fluctuating superconductors capture these trends and support an interpretation in terms of cavity-enhanced phase stiffness. These results showcase the potential of cavity engineering for designing emergent functionalities in correlated systems.

cond-mat.supr-con↗

arXiv2022

Temperature-independent non-linear terahertz transmission by liquid water

Liquid water is one of the most studied substances, yet many of its properties are difficult to rationalize. The uniqueness of water is rooted in the dynamic network of hydrogen-bonded molecules with relaxation time constants of about one picosecond. Terahertz fields oscillate on a picosecond timescale and are inherently suited to study water. Recent advances in non-linear terahertz spectroscopy have revealed large signals from water, which have been interpreted with different, sometimes competing, theoretical models. Here we show that the non-linear transmission of liquid water at ~1 THz is equal at 21 °C and 4 °C, thus suggesting that the most appropriate microscopic models should depend weakly on temperature. Among the different mechanisms proposed to date, the resonant reorientation of hydrogen-bonded water molecules might be the most appropriate to describe all of the currently available experimental results.

physics.chem-ph↗

arXiv2021

Water Solvation of Charged and Neutral Gold Nanoparticles

Gold nanoparticles are unique electrocatalysts for oxygen reduction, carbon dioxide reduction, and alcohol oxidation. Electrocatalytic processes are influenced by the interaction with the solvent, yet the direct investigation of the solvation of nanoparticles is scarce. Here we select gold nanoparticles as 10 nm sized solutes of which we can control the charge. We perform mid-infrared and terahertz spectroscopy to compare the behavior of the water in solution with micelles loaded with neutral and positive gold nanoparticles. We find indications that the hydration water around the gold-loaded micelles is characterized by weaker hydrogen bonds than bulk water. A positive nanoparticle charge is observed to result in a larger blue shift of the OH stretch, quenches the intensity of the collective translational mode, and increases the absorption by librating water molecules. Water at the interface of a positive gold nanoparticle could experience a stiffer potential energy surface which, in turn, might unveil local thermodynamic properties.

physics.chem-ph↗

arXiv2020

Strong Anisotropy in Liquid Water upon Librational Excitation using Terahertz Laser Fields

Tracking the excitation of water molecules in the homogeneous liquid is challenging due to the ultrafast dissipation of rotational excitation energy through the hydrogen-bonded network. Here we demonstrate strong transient anisotropy of liquid water through librational excitation using single-color pump-probe experiments at 12.3 THz. We deduce a third order response of chi^3 exceeding previously reported values in the optical range by three orders of magnitude. Using a theory that replaces the nonlinear response with a material response property amenable to molecular dynamics simulation, we show that the rotationally damped motion of water molecules in the librational band is resonantly driven at this frequency, which could explain the enhancement of the anisotropy in the liquid by the external Terahertz field. By addition of salt (MgSO4), the hydration water is instead dominated by the local electric field of the ions, resulting in reduction of water molecules that can be dynamically perturbed by THz pulses.

physics.chem-ph↗

arXiv2019

Persistent coherence of quantum superpositions in an optimally doped cuprate revealed by 2D spectroscopy

Understanding of the precise mechanisms of high-temperature superconductivity is elusive. In particular, in order to solve the puzzle of the pairing mechanism, it is important to understand the detailed nature of the excitations at energies around the superconducting gap. While measurements of the dynamics of excited electronic populations have been able to give some insight, they have largely neglected the intricate dynamics of quantum coherence. Here, we apply multidimensional coherent spectroscopy for the first time to a prototypical cuprate and report unprecedented coherent dynamics persisting for ~500 fs, originating directly from the quantum superposition of optically excited states separated by 20 - 60 meV. These results reveal the correlation between high and low energy excitations, and indicate that the interplay between many-body states on different energy scales conserves phase coherence. In revealing these dynamics we demonstrate that multidimensional coherent spectroscopy can address electronic correlations and interrogate many-body quantum systems in unprecedented ways.

cond-mat.supr-con↗

arXiv2017

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↗

arXiv2017

Time-domain THz spectroscopy reveals coupled protein-hydration dielectric response in solutions of native and fibrils of human lyso-zyme

Here we reveal details of the interaction between human lysozyme proteins, both native and fibrils, and their water environment by intense terahertz time domain spectroscopy. With the aid of a rigorous dielectric model, we determine the amplitude and phase of the oscillating dipole induced by the THz field in the volume containing the protein and its hydration water. At low concentrations, the amplitude of this induced dipolar response decreases with increasing concentration. Beyond a certain threshold, marking the onset of the interactions between the extended hydration shells, the amplitude remains fixed but the phase of the induced dipolar response, which is initially in phase with the applied THz field, begins to change. The changes observed in the THz response reveal protein-protein interactions me-diated by extended hydration layers, which may control fibril formation and may have an important role in chemical recognition phenomena.

physics.bio-ph↗

arXiv2017

Transient THz conductivity of silicon with optical pumping above and below the second indirect transition

Here we perform a series of time-resolved experiments where a 100 fs pump pulse is tuned between 528 nm and 555 nm, across the second indirect gap of intrinsic silicon at ~540 nm which involves electrons in a higher-lying conduction band with minimum at the L point. The photo-injected carriers, after inter- and intra-band relaxations are complete, are subsequently probed with high-field single-cycle terahertz radiation. When the energy of the pump pulses exceeds the second indirect gap, the probed terahertz absorption decreases by a factor 2.7$\pm$0.2. We suggest that this dramatic change could be due to the different phonon populations obtained when the carriers undergo the L to X inter-band scattering, instead of just cooling within the X-valley.

physics.optics↗

arXiv2015

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↗

arXiv2015

Vibronic resonances facilitate excited state coherence in light harvesting proteins at room temperature

Until recently it was believed that photosynthesis, a fundamental process for life on earth, could be fully understood with semi-classical models. However, puzzling quantum phenomena have been observed in several photosynthetic pigment-protein complexes, prompting questions regarding the nature and role of these effects. Recent attention has focused on discrete vibrational modes that are resonant or quasi-resonant with excitonic energy splittings and strongly coupled to these excitonic states. Here we unambiguously identify excited state coherent superpositions in photosynthetic light-harvesting complexes using a new experimental approach. Decoherence on the timescale of the excited state lifetime allows low energy (56 cm-1) oscillations on the signal intensity to be observed. In conjunction with an appropriate model, these oscillations provide clear and direct experimental evidence that the persistent coherences observed require strong vibronic mixing among excited states.

physics.bio-ph↗

arXiv2014

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↗

arXiv2014

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↗

arXiv2013

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↗

arXiv2012

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↗