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Jacopo Fiore

Publications and source records attributed to Jacopo Fiore.

10 recordsLinked to original sources

Coherent driving of displacive Higgs fluctuations in superconductors

Intense phase-stable terahertz (THz) laser pulses can drive collective modes coherently via multi-photon excitation pathways in a manner different than the standard resonant mechanism operative in linear response. Here we show that in superconductors the nonlinear optical response can be enhanced when excited quasiparticles activate a (non-resonant) static displacement of the superconducting order parameter, in full analogy with the displacive excitation of coherent phonons in opaque materials. By combining numerical simulations with analytical results we demonstrate that the displacive mechanism to excite the Higgs mode is operative in both $s$-wave and $d$-wave superconductors. We validate this prediction experimentally by the temperature dependence of the phase of the nonlinear first harmonic in superconducting $s$-wave NbN. We also discuss how the order-parameter relaxation at large times, which can be experimentally accessed via pump-probe protocols is connected to energy-dissipative processes. Our results offer a novel perspective on the ability of intense THz fields to measure, and eventually control, the parametric dependence of the optical response on collective degrees of freedom.

cond-mat.supr-con

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

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

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 $\tau$ 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

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

Revealing novel aspects of light-matter coupling in terahertz two-dimensional coherent spectroscopy: the case of the amplitude mode in superconductors

Recently developed terahertz (THz) two-dimensional coherent spectroscopy (2DCS) is a powerful technique to obtain materials information in a fashion qualitatively different from other spectroscopies. Here, we utilized THz 2DCS to investigate the THz nonlinear response of conventional superconductor NbN. Using broad-band THz pulses as light sources, we observed a third-order nonlinear signal whose spectral components are peaked at twice the superconducting gap energy $2\Delta$. With narrow-band THz pulses, a THz nonlinear signal was identified at the driving frequency $\Omega$ and exhibited a resonant enhancement at temperature when $\Omega = 2\Delta$. General theoretical considerations show that such a resonance can only arise from a disorder-activated paramagnetic coupling between the light and the electronic current. This proves that the nonlinear THz response can access processes distinct from the diamagnetic Raman-like density fluctuations, which are believed to dominate the nonlinear response at optical frequencies in metals. Our numerical simulations reveal that even for a small amount of disorder, the $\Omega=2\Delta$ resonance is dominated by the superconducting amplitude mode over the entire investigated disorder range. This is in contrast to other resonances, whose amplitude-mode contribution depends on disorder. Our findings demonstrate the unique ability of THz 2DCS to explore collective excitations inaccessible in other spectroscopies.

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

Contribution of Collective Excitations to Third Harmonic Generation in Multiband Superconductors: the case of MgB$_2$

Multiband superconductors can host collective excitations with marked differences with respect to their single-band counterpart. We first study the spectrum of collective amplitude fluctuations in a clean two-bands superconductor, showing that the spectral weight of the Higgs mode rapidly deviates from the naive extension of the single band case as the interband coupling is turned on. These results are then used to critically analyze the non-linear optical response in MgB$_2$, providing an explanation for the apparently contradictory results of recent experiments, pointing towards a selective relevance either of the Leggett mode or of the amplitude fluctuations at twice the lower gap. By using exact numerical simulations and realistic estimate of disorder we compute the relative contribution of the quasiparticle, amplitude and phase fluctuations to the non-linear optical response. We show that at low pumping frequency only the resonance at twice the smaller gap emerges, as due to the BCS response, while the Leggett mode dominates only in a narrow range of higher pumping frequencies matching its low-temperature value. Our findings provide a fresh perspective on the potential of non-linear THz spectroscopy to detect collective modes in other multiband systems, as e.g. iron-based superconductors.

cond-mat.supr-con

THz non-linear optical response in cuprates: predominance of the BCS response over the Higgs mode

Recent experiments with strong THz fields in unconventional cuprates superconductors have clearly evidenced an increase of the non-linear optical response below the superconducting critical temperature Tc. As in the case of conventional superconductors, a theoretical estimate of the various effects contributing to the non-linear response is needed in order to interpret the experimental findings. Here we report a detailed quantitative analysis of the non-linear THz optical kernel in cuprates within a realistic model, accounting for the band structure and disorder level appropriate for these systems. We show that the BCS quasiparticle response is the dominant contribution for cuprates, and its polarization dependence accounts very well for the third-harmonic generation measurements. On the other hand, the polarization dependence of the THz Kerr effect is only partly captured by our calculations, suggesting the presence of additional effects when the system is probed using light pulses with different central frequencies.

cond-mat.supr-con