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Niccolò Sellati

Publications and source records attributed to Niccolò Sellati.

9 recordsLinked to original sources

Measuring momentum-resolved dissipation of phonon-polaritons in LiNbO$_3$ with terahertz driving

Mapping the dispersion of polaritons, hybrid quasiparticles arising from light-matter coupling, can provide key insights into the material dielectric response, coupling strength, and energy transfer pathways with other excitations. In this work, we present THz pump-Raman probe (TP-RP) as a versatile method for mapping the polariton dispersion in polar non-centrosymmetric materials, demonstrated here for the case of phonon-polaritons in LiNbO$_3$. By resonantly driving polaritonic modes with a broadband THz pump and probing them with a tunable NIR Raman pulse, TP-RP allows for the extraction of the momentum-dependence of both their frequency and damping rate with high accuracy. The spectral features observed in the pump-probe signal, including the polaritonic response as well as pulse artifacts, are reproduced within a many-body theoretical approach. Applying the technique to study the E(TO$_1$) phonon of LiNbO$_3$ enables the combined analysis of theory and experiments to uncover a nontrivial frequency dependence of the phonon intrinsic damping rate, revealing possible anharmonic couplings to other modes.

cond-mat.mtrl-sci

Two-dimensional THz spectroscopy in electronic systems: a many-body diagrammatic approach

The term two-dimensional coherent spectroscopy (2DCS) usually refers to experimental setups where a coherently generated electric field in a sample is recorded over many runs as a function of two time variables: the delay $τ$ between two consequent excitation pulses and the time $t$ over which the signal is emitted. While its implementation in the femtosecond time domain for studying vibrational molecular states has been developed for over two decades, its experimental application in the THz domain to interacting electronic systems remains in its infancy. This work provides a general theoretical framework for describing and interpreting 2DCS using a many-body language based on a perturbative diagrammatic expansion, as widely applied in linear spectroscopy. Focusing on centrosymmetric systems, we show that interpreting the 2D maps can be recast into two complementary problems. The first is the evaluation of a third-order response function to the gauge field. In the velocity gauge, this leads to semi-analytical expressions that both reduce computational complexity and assist in assigning spectral features to microscopic processes, as shown using a toy model of electrons undergoing a charge-density wave transition. The second is a careful treatment of multi-wave propagation effects, which, in bulk systems, can obscure the intrinsic nonlinear response, demonstrated here for soft superconducting Josephson plasmons. Our results provide a solid foundation for extending 2DCS to complex interacting systems and offer a flexible method to realistically model nonlinear responses across arbitrary spectral widths.

cond-mat.supr-con

Light-induced Faraday effect from dynamical breakdown of Kleinman symmetry

The observation of anomalously large polarization rotations in pump-probe experiments with circularly polarized light has recently challenged the conventional understanding of the inverse Faraday effect. The striking magnitude of these responses implies the generation of effective magnetic fields orders of magnitude larger than theoretical expectations, raising fundamental questions about the nature of light-induced time-reversal symmetry breaking. In this work we demonstrate that a static polarization rotation can originate entirely from the antisymmetric component of the third-order optical susceptibility, without generating a macroscopic magnetization of the material. We show that this light-induced Faraday effect is inherently dynamical, emerging when Kleinman symmetry breaks down. Using a minimal sp tight-binding model on a square lattice, we demonstrate that the light-induced Faraday response can be sizable even far from dissipative resonances. While the effect emerges at a purely electronic level, we show that resonant coupling with phonons can significantly enhance the pump-probe response.

cond-mat.mtrl-sci

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$_{8+δ}$, 2DES reveals a pronounced off-diagonal resonance arising from the ultrafast generation of non-thermal bosons with energy $\hbarΩ_\mathbf{q}\simeq200$ 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 $(π/2,π/2)$ and extending toward $(0,π)$ and $(π,0)$. 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 $λ\gtrsim 0.7$ 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

Investigating Josephson plasmons in layered cuprates via nonlinear terahertz spectroscopy

Josephson plasmons in layered superconductors represent a natural source of optical non-linearity, thanks to their intrinsically anharmonic nature. Here we derive the selection rules behind non-linear plasmonics showing its dependence on plasmonic branches hidden to other spectroscopies, like RIXS. We benchmark our results for the case of layered cuprates, showing how in a layered system the combined effect of plasmon dispersion and light polarization can move the resonance of the bilayer system away from the plasma edge measured in linear spectroscopy. Our results demonstrate the dependence of the non-linear THz response on the convoluted plasmon dispersion in a momentum region complementary to RIXS, and offer a possible perspective for the generation of THz pulses by artificially designed Josephson heterostructures.

cond-mat.supr-con

Ghost Josephson plasmon in bilayer superconductors

The experimental measurement of collective charge fluctuations in metals and superconductors is a preferential tool to benchmark fundamental interactions in solids. Recent experiments in multicomponent systems, from superconducting layered cuprates to multiband metals, highlighted striking effects due to the interplay between different degrees of freedom. In this paper we provide a physical explanation for the existence of a "ghost" Josephson plasmon in bilayer superconductors, layered systems with two layers per unit cells that interact with two different Josephson couplings. We show that one of the two plasmons that emerge after the breaking of the translational symmetry along the out-of-plane direction is connected to counterflowing current fluctuations polarized perpendicularly to the planes. This effect makes it a staggered mode that is virtually transverse at small out-of-plane momenta qc, explaining why it is hidden in the density response at small qc. Our work offers an additional perspective on the understanding of collective excitations in systems with multiple intertwined degrees of freedom.

cond-mat.supr-con

Phonon-Polaritons in Non-Centrosymmetric Systems: Theory of Terahertz Pump-Optical Probe Spectroscopy

Hybrid lattice-light modes, known as phonon-polaritons, represent the backbone of advanced protocols based on THz pumping of infrared modes. Here we provide a theoretical framework able to capture the different roles played by phonon-polaritons in experimental protocols based either on Raman-like pump and probe schemes, typical of four-wave-mixing processes, or on THz pump-visible probe three-wave mixing protocols. By using a many-body description of the nonlinear optical kernel, along with a perturbative solution of nonlinear Maxwell's equations, we highlight the advantages of exploiting broadband THz pumps to enlarge the phase space of the phonon-polariton dispersion accessible in a single experiment. Besides providing a quantitative description of existing and future experiments, our results offer a general framework for the theoretical modeling of the hybridization between light and lattice degrees of freedom in time-resolved experiments.

cond-mat.mtrl-sci

Optical absorption in tilted geometries as an indirect measurement of longitudinal plasma waves in layered cuprates

Electromagnetic waves propagating in a layered superconductor with arbitrary momentum with respect to the main crystallographic directions display an unavoidable mixing between longitudinal and transverse degrees of freedom. Here we show that this basic physical mechanism explains the emergence of a well-defined absorption peak in the in-plane optical conductivity for light propagating at small tilting angles with respect to the stacking direction in layered cuprates. More specifically, we show that this peak, often interpreted as a spurious leakage of the $c$-axis Josephson plasmon, is instead a signature of the true longitudinal plasma mode occurring at larger momenta. By combining a classical approach based on Maxwell's equations with a full quantum derivation of the plasma modes based on the modelling of the superconducting phase degrees of freedom, we provide an analytical expression for the absorption peak as a function of the tilting angle and light polarization. We suggest that an all-optical measurement in tilted geometry can be used as an alternative way to access plasma-wave dispersion, usually measured by means of large-momenta scattering techniques like resonant inelastic X-ray scattering (RIXS) or electron energy loss spectroscopy (EELS).

cond-mat.supr-con

Generalized Josephson plasmons in bilayer superconductors

Layered superconductors like High-Tc cuprates display out-of-plane plasma oscillations between layers sustained by the weak Josephson coupling among the superconducting sheets, the so-called Josephson plasmons. Bilayer cuprates hosts two of such modes, but due to the anisotropy of the electronic response their description at generic wavevector cannot be separated from that of the in-plane oscillations. In this paper we provide an analytical theoretical framework able to describe the dispersions and the polarizations of the generalized plasma modes of such systems, that has been only partly addressed by previous work in the literature. We then employ it to explain the peculiar characteristics of their linear optical response, by providing a fully microscopic explanation for the appearance of a finite-frequency peak in the real part of the optical conductivity. On a wider perspective, the complete characterization of the Josephson plasma modes provided by our approach represents a groundwork to address open issues raised by recent experiments with strong THz pulses, able to drive them beyond the linear-response regime.

cond-mat.supr-con