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Andrea Marini

Publications and source records attributed to Andrea Marini.

At least 55 records · Page 3Linked to original sources

Broadband optical parametric amplification by two-dimensional semiconductors

Optical parametric amplification is a second-order nonlinear process whereby an optical signal is amplified by a pump via the generation of an idler field. It is the key ingredient of tunable sources of radiation that play an important role in several photonic applications. This mechanism is inherently related to spontaneous parametric down-conversion that currently constitutes the building block for entangled photon pair generation, which has been exploited in modern quantum technologies ranging from computing to communications and cryptography. Here we demonstrate single-pass optical parametric amplification at the ultimate thickness limit; using semiconducting transition-metal dichalcogenides, we show that amplification can be attained over a propagation through a single atomic layer. Such a second-order nonlinear interaction at the 2D limit bypasses phase-matching requirements and achieves ultrabroad amplification bandwidths. The amplification process is independent on the in-plane polarization of the impinging signal and pump fields. First-principle calculations confirm the observed polarization invariance and linear relationship between idler and pump powers. Our results pave the way for the development of atom-sized tunable sources of radiation with applications in nanophotonics and quantum information technology.

physics.optics↗

Heat-induced soliton self-frequency redshift in the ultrafast nonlinear dynamics of active plasmonic waveguides

We investigate the ultrafast nonlinear dynamics of light emitted in an active plasmonic waveguide composed of a thin film of gold sandwiched by two silicon layers immersed in externally pumped Al$_2$O$_3$:Er$^{3+}$. We model optical propagation in such a dissipative system through a generalized cubic Ginzburg-Landau equation accounting for the amplification of the active medium and the effect of absorption and thermo-modulational nonlinearity of gold. We find that heating heavily affects the propagation of temporal dissipative solitons in such a plasmonic waveguide by producing a soliton self-frequency redshift accompanied by soliton deceleration in the time domain. By adopting a semi-analytical variational approach, we evaluate the dependence of the self-induced redshift by deriving a set of coupled differential equations for the pulse parameters. These equations provide physical insight into the complex nonlinear dynamics through simple approximate analytic expressions for temporal and frequency shifts. Such analytical predictions are found in excellent agreement with direct numerical simulations of the generalized cubic Ginzburg-Landau equation. Our results provide a general understanding of ultrafast nonlinear dynamics in gold-based active plasmonic waveguides, as in particular the spectral shaping properties of propagating optical pulses.

physics.optics↗

Reproducibility in $G_0W_0$ Calculations for Solids

Ab initio many-body perturbation theory within the $GW$ approximation is a Green's function formalism widely used in the calculation of quasiparticle excitation energies of solids. In what has become an increasingly standard approach, Kohn-Sham eigenenergies, generated from a DFT calculation with a strategically-chosen exchange correlation functional ``starting point'', are used to construct $G$ and $W$, and then perturbatively corrected by the resultant $GW$ self-energy. In practice, there are several ways to construct the $GW$ self-energy, and these can lead to variations in predicted quasiparticle energies. For example, for ZnO and TiO$_2$, reported $GW$ fundamental gaps can vary by more than 1 eV. In this work, we address the convergence and key approximations in contemporary $G_0W_0$ calculations, including frequency-integration schemes and the treatment of the Coulomb divergence in the exact-exchange term. We study several systems,and compare three different $GW$ codes: BerkeleyGW, Abinit and Yambo. We demonstrate, for the first time, that the same quasiparticle energies for systems in the condensed phase can be obtained with different codes, and we provide a comprehensive assessment of implementations of the $GW$ approximation.

cond-mat.mtrl-sci↗

AC conductivities of a holographic Dirac semimetal

We use the AdS/CFT correspondence to compute the AC conductivities for a (2+1)-dimensional system of massless fundamental fermions coupled to (3+1)-dimensional Super Yang-Mills theory at strong coupling. We consider the system at finite charge density, with a constant electric field along the defect and an orthogonal magnetic field. The holographic model we employ is the well studied D3/probe-D5-brane system. There are two competing phases in this model: a phase with broken chiral symmetry favored when the magnetic field dominates over the charge density and the electric field and a chirally symmetric phase in the opposite regime. The presence of the electric field induces Ohm and Hall currents, which can be straightforwardly computed by means of the Karch-O'Bannon technique.Studying the fluctuations around the stable configurations in linear response theory, we are able to derive the full frequency dependence of longitudinal and Hall conductivities in all the regions of the phase space.

hep-th↗

Optical harmonic generation in monolayer group-VI transition metal dichalcogenides

Monolayer transition metal dichalcogenides (TMDs) exhibit high nonlinear optical (NLO) susceptibilities. Experiments on MoS$_2$ have indeed revealed very large second-order ($χ^{(2)}$) and third-order ($χ^{(3)}$) optical susceptibilities. However, third harmonic generation results of other layered TMDs has not been reported. Furthermore, the reported $χ^{(2)}$ and $χ^{(3)}$ of MoS$_2$ vary by several orders of magnitude, and a reliable quantitative comparison of optical nonlinearities across different TMDs has remained elusive. Here, we investigate second- and third-harmonic generation, and three-photon photoluminescence in TMDs. Specifically, we present an experimental study of $χ^{(2)}$, and $χ^{(3)}$ of four common TMD materials (\ce{MoS2}, \ce{MoSe2}, \ce{WS2} and \ce{WSe2}) by placing different TMD flakes in close proximity to each other on a common substrate, allowing their NLO properties to be accurately obtained from a single measurement. $χ^{(2)}$ and $χ^{(3)}$ of the four monolayer TMDs have been compared, indicating that they exhibit distinct NLO responses. We further present theoretical simulations of these susceptibilities in qualitative agreement with the measurements. Our comparative studies of the NLO responses of different two-dimensional layered materials allow us to select the best candidates for atomic-scale nonlinear photonic applications, such as frequency conversion and all-optical signal processing.

physics.optics↗

Collision quenching in the ultrafast dynamics of plasmonic materials

We explore the nonlinear response of plasmonic materials driven by ultrashort pulses of electromagnetic radiation with temporal duration of few femtoseconds and high peak intensity. By developing the Fokker-Planck-Landau theory of electron collisions, we solve analytically the collisional integral and derive a novel set of hydrodynamical equations accounting for plasma dynamics at ultrashort time scales. While in the limit of small light intensities we recover the well established Drude model of plasmas, in the high intensity limit we observe nonlinear quenching of collision-induced damping leading to absorption saturation. Our results provide a general background to understand electron dynamics in plasmonic materials with promising photonic applications in the manipulation of plasma waves with reduced absorption at the femtosecond time scale.

physics.optics↗

A functional approach to the electronic and bosonic dynamics of many-body systems perturbed with an arbitrary strong electron-boson interaction

We present a formal derivation of the many-body perturbation theory for a system of electrons and bosons subject to a nonlinear electron-boson coupling. The interaction is treated at an arbitrary high order of bosons scattered. The considered Hamiltonian includes the well-known linear coupling as a special limit. This is the case, for example, of the Holstein and Fröhlich Hamiltonians. Indeed, whereas linear coupling have been extensively studied, the scattering processes of electrons with multiple bosonic quasiparticles are largely unexplored. We focus here on a self-consistent theory in terms of dressed propagators and generalize the Hedin's equations using the Schwinger technique of functional derivatives. The method leads to an exact derivation of the electronic and bosonic self-energies, expressed in terms of a new family of vertex functions, high order correlators and bosonic and electronic mean-field potentials. In the electronic case we prove that the mean-field potential is the $n$th-order extension of the well-known Debye-Waller potential. We also introduce a bosonic mean-field potential entirely dictated by nonlinear electron-boson effects. The present scheme, treating electrons and bosons on an equal footing, demonstrates the full symmetry of the problem. The vertex functions are shown to have purely electronic and bosonic character as well as a mixed electron-boson one. These four vertex functions are shown to satisfy a generalized Bethe-Salpeter equation. Multi bosons response functions are also studied and explicit expressions for the two and the three bosons case are given.

cond-mat.str-el↗

Lasing and Amplification from Two-Dimensional Atom Arrays

We explore the ability of two-dimensional periodic atom arrays to produce light amplification and generate laser emission when gain is introduced through external optical pumping. Specifically, we predict that lasing can take place for arbitrarily weak atomic scatterers assisted by cooperative interaction among atoms in a 2D lattice. We base this conclusion on analytical theory for three-level scatterers, which additionally reveals a rich interplay between lattice and atomic resonances. Our results provide a general background to understand light amplification and lasing in periodic atomic arrays, with promising applications in the generation, manipulation, and control of coherent photon states at the nanoscale.

cond-mat.mes-hall↗

Molecular Sensing with Tunable Graphene Plasmons

We study the potential of graphene plasmons for spectrometer-free sensing based on surface-enhanced infrared absorption and Raman scattering. The large electrical tunability of these excitations enables an accurate identification of infrared molecular resonances by recording broadband absorption or inelastic scattering, replacing wavelength-resolved light collection by a signal integrated over photon energy as a function of the graphene doping level. The high quality factor of graphene plasmons plays a central role in the proposed detection techniques, which we show to be capable of providing label-free identification of the molecular vibration fingerprints. We find an enhancement of the absorption and inelastic scattering cross-sections by 3-4 orders of magnitude for molecules in close proximity to doped graphene nanodisks under currently feasible conditions. Our results pave the way for the development of novel cost-effective sensors capable of identifying spectral signatures of molecules without using spectrometers and laser sources.

cond-mat.mes-hall↗

An ab-initio approach to describe coherent and non-coherent exciton dynamics

The use of ultra-short laser pulses to pump and probe materials activates a wealth of processes which involve the coherent and non coherent dynamics of interacting electrons out of equilibrium. Non equilibrium (NEQ) many body perturbation theory (MBPT) offers an equation of motion for the density-matrix of the system which well describes both coherent and non coherent processes. In the non correlated case there is a clear relation between these two regimes and the matrix elements of the density-matrix. The same is not true for the correlated case, where the potential binding of electrons and holes in excitonic states need to be considered. In the present work we discuss how NEQ-MBPT can be used to describe the dynamics of both coherent and non-coherent excitons in the low density regime. The approach presented is well suited for an ab initio implementation.

cond-mat.mes-hall↗

Diode-like asymmetric transmission in ultrathin hyperbolic epsilon-near-zero slabs: extreme anisotropy mimicking chirality

We demonstrate that a strong asymmetric transmission for forward and backward propagation of tilted circular polarized optical waves is supported by ultrathin epsilon-near-zero hyperbolic slabs. We find that, remarkably, this effect is solely triggered by anisotropy without resorting to any breaking of reciprocity and chiral symmetries or spatial nonlocal effects. In addition, we show that the asymmetric transmission undergoes a dramatic enhancement if the slab is hyperbolic in the epsilon-near-zero regime. This happens since, close to epsilon-near-zero point, the hyperbolic dispersion activates etalon resonances where extraordinary waves accumulate propagation phase even though the slab is ultrathin. The proposed strategy holds promise for realizing ultra-compact and efficient polarization devices at different frequency bands.

physics.optics↗

The Flowing BIon

In this paper we use the effective blackfold description of branes to extend the study of the thermal BIon, a D-brane and parallel anti-D-brane connected by a wormhole with F-string charge in hot flat space, by introducing a radial boost along the brane. The boosted system behaves qualitatively differently from both the extremal and the thermal BIon considered previously. Interestingly, we are able to formulate a first law of thermodynamics for the system as a whole, despite the fact that it is not a stationary blackfold. In particular, the global temperature is given by the rest frame temperature times the gamma factor of special relativity which is the inverse transformation compared to the case of stationary blackfolds. In addition we define two new kinds of thermodynamic conjugate variables, the energy flux $W$ and the integrated velocity on the brane. We find that a phase transition occurs by varying the energy flux $W$. Below a critical value of $W$ the brane separation $Δ$ changes only slightly with $W$. Instead above the critical value $Δ$ grows exponentially.

hep-th↗

The Nonlinear Optical Effects of Opening a Gap in Graphene

Graphene possesses remarkable electronic, optical and mechanical properties that have taken the research of two-dimensional relativistic condensed matter systems to prolific levels. However, the understanding of how its nonlinear optical properties are affected by relativistic-like effects has been broadly uncharted. It has been recently shown that highly-nontrivial currents can be generated in free-standing samples, notably leading to the generation of even harmonics. Since graphene monolayers are centrosymmetric media, for which such harmonic generation is deemed inaccessible, this light-driven phenomenon is both startling and promising. More realistically, graphene samples are often deposited on a dielectric substrate, leading to additional intricate interactions. Here, we present a treatment to study this instance by gapping the spectrum and we show this leads to the appearance of a Berry phase in the carrier dynamics. We analyse the role of such a phase in the generated nonlinear current and conclude that it suppresses odd-harmonic generation. The pump energy can be tuned to the energy gap to yield interference among odd harmonics mediated by interband transitions, allowing even harmonics to be generated. Our results and general methodology pave the way for understanding the role of gap-opening physical factors in the nonlinear optics of hexagonal two-dimensional lattices.

cond-mat.mes-hall↗

Ab initio calculations of ultra-short carrier dynamics in 2D materials: valley depolarization in single-layer WSe$_2$

In single-layer WSe$_2$, a paradigmatic semiconducting transition metal dichalcogenide, a circularly polarized laser field can selectively excite electronic transitions in one of the inequivalent $K^{\pm}$ valleys. Such selective valley population corresponds to a pseudospin polarization. This can be used as a degree of freedom in a valleytronic device provided that the time scale for its depolarization is sufficiently large. Yet, the mechanism behind the valley depolarization still remains heavily debated. Recent time-dependent Kerr experiments have provided an accurate way to visualize the valley dynamics by measuring the rotation of a linearly polarized probe pulse applied after a circularly polarized pump pulse. We present here a clear, accurate and parameter-free description of the valley dynamics. By using an atomistic, ab initio, approach we fully disclose the elemental mechanisms that dictate the depolarization effects. Our results are in excellent agreement with recent time-dependent Kerr experiments. We explain the Kerr dynamics and its temperature dependence in terms of electron-phonon mediated processes that induce spin-flip inter-valley transitions.

cond-mat.mes-hall↗

Photo-Induced Bandgap Renormalization Governs the Ultrafast Response of Single-Layer MoS2

Transition metal dichalcogenides (TMDs) are emerging as promising two-dimensional (2d) semiconductors for optoelectronic and flexible devices. However, a microscopic explanation of their photophysics -- of pivotal importance for the understanding and optimization of device operation -- is still lacking. Here we use femtosecond transient absorption spectroscopy, with pump pulse tunability and broadband probing, to monitor the relaxation dynamics of single-layer MoS2 over the entire visible range, upon photoexcitation of different excitonic transitions. We find that, irrespective of excitation photon energy, the transient absorption spectrum shows the simultaneous bleaching of all excitonic transitions and corresponding red-shifted photoinduced absorption bands. First-principle modeling of the ultrafast optical response reveals that a transient bandgap renormalization, caused by the presence of photo-excited carriers, is primarily responsible for the observed features. Our results demonstrate the strong impact of many-body effects in the transient optical response of TMDs even in the low-excitation-density regime.

cond-mat.mtrl-sci↗

Anomalous temperature dependence of the band-gap in Black Phosphorus

Black Phosphorus (BP) has gained renewed attention due to its singular anisotropic electronic and optical properties that might be exploited for a wide range of technological applications. In this respect, the thermal properties are particularly important both to predict its room temperature operation and to determine its thermoelectric potential. From this point of view, one of the most spectacular and poorly understood phenomena is, indeed, the BP temperature-induced band-gap opening: when temperature is increased the fundamental band-gap increases instead of decreasing. This anomalous thermal dependence has also been observed, recently, in its monolayer counterpart. In this work, based on \textit{ab-initio} calculations, we present an explanation for this long known, and yet not fully explained, effect. We show that it arises from a combination of harmonic and lattice thermal expansion contributions, which are, in fact, highly interwined. We clearly narrow down the mechanisms that cause this gap opening by identifying the peculiar atomic vibrations that drive the anomaly. The final picture we give explains both the BP anomalous band-gap opening and the frequency increase with increasing volume (tension effect).

cond-mat.mtrl-sci↗

Non equilibrium optical properties in semiconductors from first--principles: a combined theoretical and experimental study of bulk silicon

The calculation of the equilibrium optical properties of bulk silicon by using the Bethe--Salpeter equation solved in the Kohn--Sham basis represents a cornerstone in the development of an ab--initio approach to the optical and electronic properties of materials. Nevertheless calculations of the {\em transient} optical spectrum using the same efficient and successful scheme are scarce. We report, here, a joint theoretical and experimental study of the transient reflectivity spectrum of bulk silicon. Femtosecond transient reflectivity is compared to a parameter--free calculation based on the non--equilibrium Bethe--Salpeter equation. By providing an accurate description of the experimental results we disclose the different phenomena that determine the transient optical response of a semiconductor. We give a parameter--free interpretation of concepts like bleaching, photo--induced absorption and stimulated emission, beyond the Fermi golden rule. We also introduce the concept of optical gap renormalization, as a generalization of the known mechanism of band gap renormalization. The present scheme successfully describes the case of bulk silicon, showing its universality and accuracy.

physics.optics↗

Petahertz optical response in graphene

The temporal dynamics of charge carriers determines the speed with which electronics can be realized in condensed matter, and their direct manipulation with optical fields promises electronic processing at unprecedented petahertz frequencies, consisting in a million-fold increase from state of the art technology. Graphene is of particular interest for the implementation of petahertz optoelectronics due to its unique transport properties, such as high carrier mobility with near-ballistic transport and exceptionally strong coupling to optical fields. The back action of carriers in response to an optical field is therefore of key importance towards applications. Here we investigate the instantaneous response of graphene to petahertz optical fields and elucidate the role of hot carriers on a sub-100 fs timescale. Measurements of the nonlinear response and its dependence on interaction time and field polarization allow us to identify the back action of hot carriers over timescales that are commensurate with the optical field. An intuitive picture is given for the carrier trajectories in response to the optical-field polarization state. We note that the peculiar interplay between optical fields and charge carriers in graphene may also apply to surface states in topological insulators with similar Dirac cone dispersion relations.

cond-mat.mes-hall↗