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Giacomo Jarc

Publications and source records attributed to Giacomo Jarc.

12 recordsLinked to original sources

Raman signatures of a non-reciprocal magnetic phase transition in Ca$_2$RuO$_4$

The magnetic behavior of Ca$_2$RuO$_4$ represents a unique puzzle due to the interplay of strong electronic correlations, magneto-elastic interactions, and large spin-orbit coupling. At low temperatures, an anomalous Mott insulating state emerges, characterized by a complex antiferromagnetic order with a collective amplitude excitation of the magnetic moment which has been discussed in analogy with the Higgs mode. We report here evidence of a magnetic first-order phase transition driven by an out-of-plane magnetic field along the crystallographic $c$-axis of Ca$_2$RuO$_4$. Raman measurements in magnetic field reveal the emergence of mode of magnetic origin and a concomitant modification of the coupling between a phonon and the Higgs amplitude mode. Both the Raman features are characterized by a non-reciprocal hysteresis in magnetic field. Surprisingly, the observed phase transition does not affect the Raman scattering from the in-plane magnons, indicating that the dipolar antiferromagnetic order is preserved. This is consistent with the onset of a new quadrupolar field-controlled state, whose fluctuations structure can trigger an hybridization between the lattice and the magnetic Higgs mode resulting in the observed Raman features.

cond-mat.str-el

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

Tracking the photoinduced dynamics of a dark excitonic state in single-layer WS$_2$ via resonant Autler-Townes splitting

Excitons in a monolayer transition metal dichalcogenide (1L-TMD) are highly bound states characterized by a Rydberg-like spectrum of discrete energy levels. Among these, states with odd-parity are known as dark excitons due to selection rules, which make their stationary and transient characterization challenging using linear optical techniques. Here, we demonstrate that the dynamics of a 2p dark excitonic state in 1L-WS$_2$ can be directly retrieved by measuring the Autler-Townes splitting of bright states in a three-pulse experiment. The splitting of the bright 1s excitonic state, observed by detuning a mid-infrared control field across the 1s-2p transition, provides an accurate characterization of the 2p state. Following carrier photoinjection, we observe a qualitatively different dynamics of the 1s and 2p levels, which is indicative of symmetry-dependent screening and exciton-exciton interactions. These findings provide new insights into many-body effects in TMDs, offering potential avenues for advancing the next generation optoelectronics.

cond-mat.mes-hall

Ultrafast pump-probe phase-randomized tomography

Measuring fluctuations in matter's low energy excitations is the key to unveil the nature of the nonequilibrium response of materials. A promising outlook in this respect is offered by spectroscopic methods that address matter fluctuations by exploiting the statistical nature of light-matter interactions with weak few-photon probes. Here we report the first implementation of ultrafast phase randomized tomography, combining pump-probe experiments with quantum optical state tomography, to measure the ultrafast non-equilibrium dynamics in complex materials. Our approach utilizes a time-resolved multimode heterodyne detection scheme with phase-randomized coherent ultrashort laser pulses, overcoming the limitations of phase-stable configurations and enabling a robust reconstruction of the statistical distribution of phase-averaged optical observables. This methodology is validated by measuring the coherent phonon response in $α$-quartz. By tracking the dynamics of the shot-noise limited photon number distribution of few-photon probes with ultrafast resolution, our results set an upper limit to the non-classical features of phononic state in $α$-quartz and provide a pathway to access nonequilibrium quantum fluctuations in more complex quantum materials.

quant-ph

Multimode vibrational coupling across the insulator-to-metal transition in 1T-TaS$_{2}$ in THz cavities

The use of optical cavities on resonance with material excitations allows controlling light-matter interaction in both the regimes of weak and strong coupling. We study here the multimode vibrational coupling of low energy phonons in the charge-density-wave material 1T-TaS$_{2}$ across its insulator-to-metal phase transition. For this purpose, we embed 1T-TaS$_{2}$ into THz Fabry-Pérot cryogenic cavities tunable in frequency within the spectral range of the vibrational modes of the insulating phase and track the linear response of the coupled phonons across the insulator-to-metal transition. In the low temperature dielectric state, we reveal the signatures of a multimode vibrational strong collective coupling. The observed polariton modes inherit character from all the vibrational resonances as a consequence of the cavity-mediated hybridization. We reveal that the vibrational strong collective coupling is suppressed across the insulator-to-metal transition as a consequence of the phonon-screening induced by the free charges. Our findings emphasize how the response of cavity-coupled vibrations can be modified by the presence of free charges, uncovering a new direction toward the tuning of coherent light-matter interaction in cavity-confined correlated materials.

cond-mat.mtrl-sci

Cavity-mediated thermal control of metal-to-insulator transition in 1T-TaS$_{2}$

Placing quantum materials into optical cavities provides a unique platform for controlling quantum cooperative properties of matter, via both weak and strong light-matter coupling. Here we report the experimental evidence of reversible cavity control of a metal-to-insulator phase transition in a correlated solid-state material. We embed the charge density wave material 1T-TaS$_{2}$ into cryogenic tunable terahertz cavities and show that a switch between conductive and insulating behaviors, associated with a large change in the sample temperature, is obtained by mechanically tuning the distance between the cavity mirrors and their alignment. The large thermal modification observed is indicative of a Purcell-like scenario in which the spectral profile of the cavity modifies the energy exchange between the material and the external electromagnetic field. Our findings provide opportunities for controlling the thermodynamics and macroscopic transport properties of quantum materials by engineering their electromagnetic environment.

cond-mat.mtrl-sci

Dynamics of non-thermal states in optimally-doped $Bi_2Sr_2Ca_{0.92}Y_{0.08}Cu_2O_{8+δ}$ revealed by mid-infrared three-pulse spectroscopy

In the cuprates, the opening of a d-wave superconducting (SC) gap is accompanied by a redistribution of spectral weight at energies two orders of magnitude larger than this gap. This indicates the importance to the pairing mechanism of on-site electronic excitations, such as orbital transitions or charge transfer excitations. Here, we resort to a three-pulse pump-probe scheme to study the broadband non-equilibrium dielectric function in optimally-doped $Bi_2Sr_2Ca_{0.92}Y_{0.08}Cu_2O_{8+δ}$ and we identify two distinct dynamical responses: i) a blueshift of the central energy of an interband excitation peaked at 2 eV and ii) a change in spectral weight in the same energy range. Photoexcitation with near-IR and mid-IR pulses, with photon energies respectively above and below the SC gap, reveals that the transient changes in the central energy are not modified by the onset of superconductivity and do not depend on the pump photon energy. Conversely, the spectral weight dynamics strongly depends on the pump photon energy and has a discontinuity at the critical temperature. The picture that emerges is that, while high-energy pulses excite quasiparticles in both nodal and thermally inaccessible antinodal states, photoexcitation by low-energy pulses mostly accelerates the condensate and creates excitations predominantly at the nodes of the SC gap. These results, rationalized by kinetic equations for d-wave superconducting gaps, indicate that dynamical control of the momentum-dependent distribution of non-thermal quasiparticles may be achieved by the selective tuning of the photoexcitation.

cond-mat.supr-con

Tunable cryogenic THz cavity for strong light-matter coupling in complex materials

We report here the realization and commissioning of an experiment dedicated to the study of the optical properties of light matter hybrids constituted of crystalline samples embedded in an optical cavity. The experimental assembly developed offers the unique opportunity to study the weak and strong coupling regime between a tunable optical cavity in cryogenic environment and low energy degrees of freedom such as phonons, magnons or charge fluctuations. We describe here the setup developed which allows the positioning of crystalline samples in an optical cavity of different quality factor, the tuning of the cavity length at cryogenic temperatures and its optical characterization with a broadband time domain THz spectrometer (0.2-6 THz). We demonstrate the versatility of the setup by studying the vibrational strong coupling in CuGeO3 single crystal at cryogenic temperatures.

physics.ins-det

Non-adiabatic suppression of 3D excitonic screening in black phosphorus by mid-infrared pulses

The competition between the electron-hole Coulomb attraction and the three-dimensional dielectric screening dictates the optical properties of layered semiconductors. In low-dimensional materials, the equilibrium dielectric environment can be significantly altered by the ultrafast excitation of photo-carriers, leading to renormalized band gap and exciton binding energies. Recently, black phosphorus emerged as a 2D material with strongly layer-dependent electronic properties. Here, we resolve the coherent response of screening to sub-gap photo-excitation in bulk black phosphorus and find that mid-infrared pulses tuned across the band gap drive a transient non-thermal suppression of the dielectric screening, which is revealed by the emergence of the single-layer exciton resonance. Our work exposes the role of interlayer interactions in determining the electronic properties of 2D materials and discloses the possibility of optically manipulate them, which is of great relevance for the engineering of versatile van der Waals low-dimensional materials.

cond-mat.mtrl-sci

Anisotropic Time-Domain Electronic Response in Cuprates

Superconductivity in the cuprates is characterized by spatial inhomogeneity and an anisotropic electronic gap of d-wave symmetry. The aim of this work is to understand how this anisotropy affects the non-equilibrium electronic response of high-Tc superconductors. We compare the nodal and antinodal non-equilibrium response to photo-excitations with photon energy comparable to the superconducting gap and polarization along the Cu-Cu axis of the sample. The data are supported by an effective d-wave BCS model indicating that the observed enhancement of the superconducting transient signal mostly involves an increase of pair coherence in the antinodal region, which is not induced at the node.

cond-mat.supr-con

Visible pump -- mid infrared pump -- broadband probe: development and characterization of a three-pulse setup for single-shot ultrafast spectroscopy at 50 kHz

We report here an experimental setup to perform three-pulse pump-probe measurements over a wide wavelength and temperature range. By combining two pump pulses in the visible (650-900 nm) and mid-IR (5-20 $μ$m) range, with a broadband supercontinuum white-light probe, our apparatus enables both the combined selective excitation of different material degrees of freedom and a full time-dependent reconstruction of the non-equilibrium dielectric function of the sample. We describe here the optical setup, the cryogenic sample environment and the custom-made acquisition electronics capable of referenced single-pulse detection of broadband spectra at the maximum repetition rate of 50 kHz, achieving a sensitivity of the order of 10$^{-4}$ over an integration time of 1 s. We demonstrate the performance of the setup by reporting data on mid-IR pump, optical push and broadband probe in a single-crystal of Bi$_2$Sr$_2$Y$_{0.08}$Ca$_{0.92}$Cu$_2$O$_{8+δ}$ across the superconducting and pseudogap phases.

physics.optics

Time-resolved multimode heterodyne detection for dissecting coherent states of matter

Unveiling and controlling the coherent evolution of low energy states is a key to attain light driven new functionalities of materials. Here we investigate the coherent evolution of non-equilibrium photon-phonon Raman interactions in the low photon number regime via femtosecond time-resolved multimode heterodyne detection. The time dependence of the weak probe spectral components is revealed by interferential amplification with shaped phase-locked reference fields that allow for a frequency selective amplification. We report measurements on $α$-quartz that show that both amplitude and phase of the probe spectral components are modulated at the phonon frequency, but encode qualitatively different responses which are representative respectively of the time dependent position and momentum of the atoms. We stress that the sensitivity achieved here (1-10 photons per pulse) may be of relevance for both quantum information technologies and time domain studies on photosensitive materials.

physics.app-ph