arXiv subjects

G. Cerullo

Publications and source records attributed to G. Cerullo.

At least 19 recordsLinked to original sources

arXiv2025

Quantum Batteries: A Materials Science Perspective

In the context of quantum thermodynamics, quantum batteries have emerged as promising devices for energy storage and manipulation. Over the past decade, substantial progress has been made in understanding the fundamental properties of quantum batteries, with several experimental implementations showing great promise. This Perspective provides an overview of the solid-state materials platforms that could lead to fully operational quantum batteries. After briefly introducing the basic features of quantum batteries, we discuss organic microcavities, where superextensive charging has already been demonstrated experimentally. We then explore other materials, including inorganic nanostructures (such as quantum wells and dots), perovskite systems, and (normal and high-temperature) superconductors. Key achievements in these areas, relevant to the experimental realization of quantum batteries, are highlighted. We also address challenges and future research directions. Despite their enormous potential for energy storage devices, research into advanced materials for quantum batteries is still in its infancy. This paper aims to stimulate interdisciplinarity and convergence among different materials science research communities to accelerate the development of new materials and device architectures for quantum batteries.

cond-mat.mtrl-sci↗

arXiv2025

Selective electron-phonon coupling strength from nonequilibrium optical spectroscopy: The case of MgB$_2$

The coupling between quasiparticles and bosonic excitations rules the energy transfer pathways in condensed matter systems. The possibility of inferring the strength of specific coupling channels from their characteristic time scales measured in nonequilibrium experiments is still an open question. Here, we investigate MgB$_2$, in which conventional superconductivity at temperatures as high as 39 K is mediated by the strong coupling between the conduction electrons and the E$_{2g}$ phonon mode. By means of broadband time-resolved optical spectroscopy, we show that this selective electron-phonon coupling dictates the nonequilibrium optical response of MgB$_2$, at early times ($<$100 fs) after photoexcitation. Furthermore, based on an effective temperature model analysis, we estimate its contribution to the total electron-boson coupling function extracted from complementary equilibrium spectroscopy approaches, namely optical reflectivity and ARPES. The coupling strength with the E$_{2g}$ phonon modes is thus estimated to be $\lambda \simeq$ 0.56, which is approximately half of the total coupling constant, in agreement with ab-initio calculations from the literature. As a benchmark, broadband time-resolved optical spectroscopy is performed also on the isostructural and non-superconducting compound AlB$_2$, showing that the nonequilibrium optical response relaxes on a slower time scale due to the lack of strongly-coupled phonon modes. Our findings demonstrate the possibility to resolve and quantify selective electron-phonon coupling from nonequilibrium optical spectroscopy.

cond-mat.supr-con↗

arXiv2024

Identification of soft modes across the commensurate-to-incommensurate charge density wave transition in 1$T$-TaSe$_2$

1$T$-TaSe$_2$ is a prototypical charge density wave (CDW) material for which electron-phonon coupling and associated lattice distortion play an important role in driving and stabilizing the CDW phase. Here, we investigate the lattice dynamics of bulk 1$T$-TaSe$_2$ using angle-resolved ultralow wavenumber Raman spectroscopy down to 10 cm$^{-1}$. Our high-resolution spectra allow us to identify at least 27 Raman-active modes in the commensurate (CCDW) phase. Contrary to other layered materials, we do not find evidence of interlayer breathing or shear modes, suggestive of $AA$ stacking in the bulk, or sufficiently weak interlayer coupling. Polarization dependence of the mode intensities allows the assignment of their symmetry, which is supported by first-principles calculations of the phonons for the bulk structure using density functional theory. A detailed temperature dependence in the range $T$ = 80 - 500 K allows us to identify soft modes associated with the CDW superlattice. Upon entering the incommensurate (ICCDW) phase above 473 K, we observe a dramatic loss of resolution of all modes, and significant linewidth broadening associated with a reduced phonon lifetime as the charge-order becomes incommensurate with the lattice.

cond-mat.str-el↗

arXiv2023

Exploring the Charge Density Wave phase of 1$T$-TaSe$_2$: Mott or Charge-transfer Gap?

1$T$-TaSe$_2$ is widely believed to host a Mott metal-insulator transition in the charge density wave (CDW) phase according to the spectroscopic observation of a band gap that extends across all momentum space. Previous investigations inferred that the occurrence of the Mott phase is limited to the surface only of bulk specimens, but recent analysis on thin samples revealed that the Mott-like behavior, observed in the monolayer, is rapidly suppressed with increasing thickness. Here, we report combined time- and angle-resolved photoemission spectroscopy and theoretical investigations of the electronic structure of 1$T$-TaSe$_2$. Our experimental results confirm the existence of a state above $E_F$, previously ascribed to the upper Hubbard band, and an overall band gap of $\sim 0.7$ eV at $\overline{\Gamma}$. However, supported by density functional theory calculations, we demonstrate that the origin of this state and the gap rests on band structure modifications induced by the CDW phase alone, without the need for Mott correlation effects.

cond-mat.str-el↗

arXiv2023

A Stimulated Raman Loss spectrometer for metrological studies of quadrupole lines of hydrogen isotopologues

We discuss layout and performance of a high-resolution Stimulated Raman Loss spectrometer that has been newly developed for accurate studies of spectral lineshapes and line center frequencies of hydrogen isotopologues and in general of Raman active transitions. Thanks to the frequency comb calibration of the detuning between pump and Stokes lasers and to an active alignment of the two beams, the frequency accuracy is well below 100 kHz. Over the vertical axis the spectrometer benefits from shot-noise limited detection, signal enhancement via multipass cell, active flattening of the spectral baseline and measurement times of few seconds over spectral spans larger than 10 GHz. Under these conditions an efficient averaging of Raman spectra is possible over long measurement times with minimal distortion of spectral lineshapes. By changing the pump laser, transitions can be covered in a very broad frequency span, from 50 to 5000 $\mathrm{cm^{-1}}$, including both vibrational and rotational bands. The spectrometer has been developed for studies of fundamental and collisional physics of hydrogen isotopologues and has been recently applied to the metrology of the Q(1) 1-0 line of $\mathrm{H_2}$.

physics.optics↗

arXiv2022

Parametric Nonlinear Optics with Layered Materials and Related Heterostructures

Nonlinear optics is of crucial importance in several fields of science and technology with applications in frequency conversion, entangled-photon generation, self-referencing of frequency combs, crystal characterization, sensing, and ultra-short light pulse generation and characterization. In recent years, layered materials and related heterostructures have attracted huge attention in this field, due to their huge nonlinear optical susceptibilities, their ease of integration on photonic platforms, and their 2D nature which relaxes the phase-matching constraints and thus offers a practically unlimited bandwidth for parametric nonlinear processes. In this review the most recent advances in this field, highlighting their importance and impact both for fundamental and technological aspects, are reported and explained, and an outlook on future research directions for nonlinear optics with atomically thin materials is provided.

physics.optics↗

arXiv2022

Stimulated-Raman-Scattering Metrology

Frequency combs have revolutionized optical frequency metrology, allowing one to determine highly accurate transition frequencies of a wealth of molecular species. Despite a recognized scientific interest, these progresses have only marginally benefited infrared-inactive transitions, due to their inherently weak cross-sections. Here we overcome this limitation by introducing stimulated-Raman-scattering metrology, where a frequency comb is exploited to calibrate the frequency detuning between the pump and Stokes excitation lasers. We apply this approach to molecular hydrogen to test quantum electrodynamics. We measure the transition frequency of the Q(1) fundamental line of H$_2$ around 4155 cm$^{-1}$ with few parts-per-billion uncertainty, which is comparable to the theoretical benchmark of ab initio calculations and more than a decade better than the experimental state of the art. Our comb-calibrated stimulated Raman scattering spectrometer extends the toolkit of optical frequency metrology as it can be applied, with simple technical changes, to many other infrared-inactive transitions, over a 50-5000 cm$^{-1}$ range that covers also purely rotational bands.

physics.optics↗

arXiv2022

Superabsorption in an organic microcavity: towards a quantum battery

The rate at which matter emits or absorbs light can be modified by its environment, as dramatically exemplified by the widely-studied phenomenon of superradiance. The reverse process, superabsorption, is harder to demonstrate due to the challenges of probing ultrafast processes, and has only been seen for small numbers of atoms. Its central idea - superextensive scaling of absorption meaning larger systems absorb faster - is also the key idea underpinning quantum batteries. Here we implement experimentally a paradigmatic model of a quantum battery, constructed of a microcavity enclosing a molecular dye. Ultrafast optical spectroscopy allows us to observe charging dynamics at femtosecond resolution to demonstrate superextensive charging rates and storage capacity, in agreement with our theoretical modelling. We find that decoherence plays an important role in stabilising energy storage. Our work opens new opportunities for harnessing collective effects in light-matter coupling for nanoscale energy capture, storage, and transport technologies.

quant-ph↗

arXiv2021

Femtosecond phononic coupling to both spins and charges in a room temperature antiferromagnetic semiconductor

Spintronics is postulated on the possibility to employ the magnetic degree of freedom of electrons for computation and couple it to charges. In this view, the combination of the high-frequency of spin manipulations offered by antiferromagnets, with the wide tunability of the electronic properties peculiar of semiconductors provides a promising and intriguing platform. Here we explore this scenario in $α$-MnTe, which is a semiconductor antiferromagnetically ordered at room temperature. Relying on a Raman mechanism and femtosecond laser pulses, we drive degenerate modes of coherent optical phonons, which modulate the chemical bonds involved in the super-exchange interaction. The spectrally-resolved measurements of the transient reflectivity reveal a coherent modulation of the band-gap at the frequency of 5.3 THz. The detection of the rotation of the polarisation, typically associated with magneto-optical effects, shows coherent and incoherent contributions. Modelling how the ionic motion induced by the phonons affects the exchange interaction in the material, we calculate the photoinduced THz spin dynamics: the results predict both a coherent and incoherent response, the latter of which is consistent with the experimental observation. Our work demonstrates that the same phonon modes modulate both the charge and magnetic degree of freedom, suggesting the resonant pumping of phonons as a viable way to link spin and charge dynamics even in nonlinear regimes.

physics.optics↗

arXiv2021

Cryogenic Penning-Trap Apparatus for Precision Experiments with Sympathetically Cooled (anti)protons

Current precision experiments with single (anti)protons to test CPT symmetry progress at a rapid pace, but are complicated by the need to cool particles to sub-thermal energies. We describe a cryogenic Penning-trap setup for $^9$Be$^+$ ions designed to allow coupling of single (anti)protons to laser-cooled atomic ions for sympathetic cooling and quantum logic spectroscopy. We report on trapping and laser cooling of clouds and single $^9$Be$^+$ ions. We discuss prospects for a microfabricated trap to allow coupling of single (anti)protons to laser-cooled $^9$Be$^+$ ions for sympathetic laser cooling to sub-mK temperatures on ms time scales.

physics.atom-ph↗

arXiv2020

Coherent phonons and the interplay between charge density wave and Mott phases in 1$T$-TaSe$_{2}$

1$T$-TaSe$_{2}$ is host to coexisting strongly-correlated phases including charge density waves (CDWs) and an unusual Mott transition at low temperature. Here, we investigate coherent phonon oscillations in 1$T$-TaSe$_{2}$ using a combination of time- and angle-resolved photoemission spectroscopy (TR-ARPES) and time-resolved reflectivity (TRR). Perturbation by a femtosecond laser pulse triggers a modulation of the valence band binding energy at the $\Gamma$-point, related to the Mott gap, that is consistent with the in-plane CDW amplitude mode frequency. By contrast, TRR measurements show a modulation of the differential reflectivity comprised of multiple frequencies belonging to the distorted CDW lattice modes. Comparison of the temperature dependence of coherent and spontaneous phonons across the CDW transition shows that the amplitude mode intensity is more easily suppressed during perturbation of the CDW state by the optical excitation compared to other modes. Our results clearly identify the relationship of the in-plane CDW amplitude mode with the Mott phase in 1$T$-TaSe$_{2}$ and highlight the importance of lattice degrees of freedom.

cond-mat.str-el↗

arXiv2020

Non-equilibrium Band Broadening, Gap Renormalization and Band Inversion in Black Phosphorus

Black phosphorous (BP) is a layered semiconductor with high carrier mobility, anisotropic optical response and wide bandgap tunability. In view of its application in optoelectronic devices, understanding transient photo-induced effects is crucial. Here, we investigate by time- and angle-resolved photoemission spectroscopy BP in its pristine state and in the presence of Stark splitting, chemically induced by Cs ad-sorption. We show that photo-injected carriers trigger bandgap renormalization and a concurrent valence band attening caused by Pauli blocking. In the biased sample, photoexcitation leads to a long-lived (ns) surface photovoltage of few hundreds mV that counterbalances the Cs-induced surface band bending. This allows us to disentangle bulk from surface electronic states and to clarify the mechanism underlying the band inversion observed in bulk samples.

cond-mat.mes-hall↗

arXiv2019

Strongly coupled coherent phonons in single-layer MoS$_2$

We present a transient absorption setup combining broadband detection over the visible-UV range with high temporal resolution ($\sim$20fs) which is ideally suited to trigger and detect vibrational coherences in different classes of materials. We generate and detect coherent phonons (CPs) in single layer (1L) MoS$_2$, as a representative semiconducting 1L-transition metal dichalcogenide (TMD), where the confined dynamical interaction between excitons and phonons is unexplored. The coherent oscillatory motion of the out-of-plane $A'_{1}$ phonons, triggered by the ultrashort laser pulses, dynamically modulates the excitonic resonances on a timescale of few tens fs. We observe an enhancement by almost two orders of magnitude of the CP amplitude when detected in resonance with the C exciton peak, combined with a resonant enhancement of CP generation efficiency. Ab initio calculations of the change in 1L-MoS$_2$ band structure induced by the $A'_{1}$ phonon displacement confirm a strong coupling with the C exciton. The resonant behavior of the CP amplitude follows the same spectral profile of the calculated Raman susceptibility tensor. This demonstrates that CP excitation in 1L-MoS$_2$ can be described as a Raman-like scattering process. These results explain the CP generation process in 1L-TMDs, paving the way for coherent all-optical control of excitons in layered materials in the THz frequency range.

cond-mat.mtrl-sci↗

arXiv2019

A Hyperspectral Microscope based on an Ultrastable Common-Path Interferometer

We introduce a wide field hyperspectral microscope using the Fourier-transform approach. The interferometer is based on the Translating-Wedge-Based Identical Pulses eNcoding System (TWINS) [Opt. Lett. 37, 3027 (2012)], a common-path birefringent interferometer which combines compactness, intrinsic interferometric delay precision, long-term stability and insensitivity to vibrations. We describe three different implementations of our system: two prototypes designed to test different optical schemes and an add-on for a commercial microscope. We show high-quality spectral microscopy of the fluorescence from stained cells and powders of inorganic pigments, demonstrating that the device is suited to biology and materials science. We demonstrate the acquisition of a 1Mpixel hyperspectral image in 75 seconds in the spectral range from 400 to 1100 nm. We also introduce an acquisition method which synthesizes a tunable spectral filter, providing band-passed images by the measurement of only two maps.

physics.ins-det↗

arXiv2019

Laser-driven quantum magnonics and THz dynamics of the order parameter in antiferromagnets

The impulsive generation of two-magnon modes in antiferromagnets by femtosecond optical pulses, so-called femto-nanomagnons, leads to coherent longitudinal oscillations of the antiferromagnetic order parameter that cannot be described by a thermodynamic Landau-Lifshitz approach. We argue that this dynamics is triggered as a result of a laser-induced modification of the exchange interaction. In order to describe the oscillations we have formulated a quantum mechanical description in terms of magnon pair operators and coherent states. Such an approach allowed us to} derive an effective macroscopic equation of motion for the temporal evolution of the antiferromagnetic order parameter. An implication of the latter is that the photo-induced spin dynamics represents a macroscopic entanglement of pairs of magnons with femtosecond period and nanometer wavelength. By performing magneto-optical pump-probe experiments with 10 femtosecond resolution in the cubic KNiF$_3$ and the uniaxial K$_2$NiF$_4$ collinear Heisenberg antiferromagnets, we observed coherent oscillations at the frequency of 22 THz and 16 THz, respectively. The detected frequencies as a function of the temperature ideally fit the two-magnon excitation up to the Néel point. The experimental signals are described as dynamics of magnetic linear dichroism due to longitudinal oscillations of the antiferromagnetic vector.

cond-mat.mes-hall↗

arXiv2019

Multi-channel lock-in based differential front-end for broadband Raman spectroscopy

In Broadband Stimulated Raman Spectroscopy, the intrinsic limit given by the laser shot noise is seldom reached due to the electronic noise of the front-end amplifier and the intensity fluctuations of the laser source. In this paper we present a low-noise multi-channel acquisition system, with an integration-oriented design, able to compensate the common-mode fluctuations of the laser output power with the pseudo-differential structure and reach a sensitivity better than 10 ppm thanks to the lock-in technique.

eess.SP↗

arXiv2019

Versatile control of $^9$Be$^+$ ions using a spectrally tailored UV frequency comb

We demonstrate quantum control of $^9$Be$^+$ ions directly implemented by an optical frequency comb. Based on numerical simulations of the relevant processes in $^9$Be$^+$ for different magnetic field regimes, we demonstrate a wide applicability when controlling the comb's spectral properties. We introduce a novel technique for the selective and efficient generation of a spectrally tailored narrow-bandwidth optical frequency comb near 313 nm. We experimentally demonstrate internal state control and internal-motional state coupling of $^9$Be$^+$ ions implemented by stimulated-Raman manipulation using a spectrally optimized optical frequency comb. Our pulsed laser approach is a key enabling step for the implementation of quantum logic and quantum information experiments in Penning traps.

physics.atom-ph↗

arXiv2019

Hot electrons modulation of third harmonic generation in graphene

Hot electrons dominate the ultrafast ($\sim$fs-ps) optical and electronic properties of metals and semiconductors and they are exploited in a variety of applications including photovoltaics and photodetection. We perform power-dependent third harmonic generation measurements on gated single-layer graphene and detect a significant deviation from the cubic power-law expected for a third harmonic generation process. We assign this to the presence of hot electrons. Our results indicate that the performance of nonlinear photonics devices based on graphene, such as optical modulators and frequency converters, can be affected by changes in the electronic temperature, which might occur due to increase of absorbed optical power or Joule heating.

cond-mat.mes-hall↗