arXiv subjects

G. Cerullo

Publications and source records attributed to G. Cerullo.

34 records · Page 2Linked to original sources

arXiv2019

Coherent anti-Stokes Raman Spectroscopy of single and multi-layer graphene

We report stimulated Raman spectroscopy of the G phonon in both single and multi-layer graphene, through Coherent anti-Stokes Raman Scattering (CARS). The signal generated by the third order nonlinearity is dominated by a vibrationally non-resonant background (NVRB), which obscures the Raman lineshape. We demonstrate that the vibrationally resonant CARS peak can be measured by reducing the temporal overlap of the laser excitation pulses, suppressing the NVRB. We model the observed spectra, taking into account the electronically resonant nature of both CARS and NVRB. We show that CARS can be used for graphene imaging with vibrational sensitivity.

cond-mat.mes-hall↗

arXiv2018

Role of matrix elements in the time-resolved photoemission signal

Time- and angle-resolved photoemission spectroscopy accesses the ultrafast evolution of quasiparticles and many-body interactions in solid-state systems. However, the momentum- and energy-resolved transient photoemission intensity may not be unambiguously related to the intrinsic relaxation dynamics of photoexcited electrons. In fact, interpretation of the time-dependent photoemission signal can be affected by the transient evolution of both the one-electron removal spectral function as well as the photoemission dipole matrix elements. Here we investigate the topological insulator Bi$_{1.1}$Sb$_{0.9}$Te$_2$S to demonstrate, by means of a careful probe-polarization study, the transient contribution of matrix elements to the time-resolved photoemission signal.

cond-mat.mtrl-sci↗

arXiv2018

Direct observation of intravalley spin relaxation in single-layer WS$_2$

In monolayer Transition Metal Dichalcogenides (TMDs) the valence and conduction bands are spin split because of the strong spin-orbit interaction. In tungsten-based TMDs the spin-ordering of the conduction band is such that the so-called dark exciton, consisting of an electron and a hole with opposite spin orientation, has lower energy than the A exciton. A possible mechanism leading to the transition from bright to dark excitons involves the scattering of the electrons from the upper to the lower conduction band state in K. Here we exploit the valley selective optical selection rules and use two-color helicity-resolved pump-probe spectroscopy to directly measure the intravalley spin-flip relaxation dynamics of electrons in the conduction band of single-layer WS$_2$. This process occurs on a sub-ps time scale and it is significantly dependent on the temperature, indicative of a phonon-assisted relaxation. These experimental results are supported by time-dependent ab-initio calculations which show that the intra-valley spin-flip scattering occurs on significantly longer time scales only exactly at the K point. In a realistic situation the occupation of states away from the minimum of the conduction band leads to a dramatic reduction of the scattering time.

cond-mat.mtrl-sci↗

arXiv2018

Raman spectroscopy of graphene under ultrafast laser excitation

The equilibrium optical phonons of graphene are well characterized in terms of anharmonicity and electron-phonon interactions, however their non-equilibrium properties in the presence of hot charge carriers are still not fully explored. Here we study the Raman spectrum of graphene under ultrafast laser excitation with 3ps pulses, which trade off between impulsive stimulation and spectral resolution. We localize energy into hot carriers, generating non-equilibrium temperatures in the ~1700-3100K range, far exceeding that of the phonon bath, while simultaneously detecting the Raman response. The linewidth of both G and 2D peaks show an increase as function of the electronic temperature. We explain this as a result of the Dirac cones' broadening and electron-phonon scattering in the highly excited transient regime, important for the emerging field of graphene-based photonics and optoelectronics.

cond-mat.mes-hall↗

arXiv2017

Out-of-plane heat transfer in van der Waals stacks: electron-hyperbolic phonon coupling

Van der Waals heterostructures have emerged as promising building blocks that offer access to new physics, novel device functionalities, and superior electrical and optoelectronic properties. Applications such as thermal management, photodetection, light emission, data communication, high-speed electronics and light harvesting require a thorough understanding of (nanoscale) heat flow. Here, using time-resolved photocurrent measurements we identify an efficient out-of-plane energy transfer channel, where charge carriers in graphene couple to hyperbolic phonon polaritons in the encapsulating layered material. This hyperbolic cooling is particularly efficient, giving picosecond cooling times, for hexagonal BN, where the high-momentum hyperbolic phonon polaritons enable efficient near-field energy transfer. We study this heat transfer mechanism through distinct control knobs to vary carrier density and lattice temperature, and find excellent agreement with theory without any adjustable parameters. These insights may lead to the ability to control heat flow in van der Waals heterostructures.

cond-mat.mes-hall↗

arXiv2017

Solution processable and optically switchable 1D photonic structures

In this work, we report the first demonstration of a solution processable, optically switchable 1D photonic crystal by implementing phototunable doped metal oxide nanocrystals. The resulting device structure shows bi-photonic response with the photonic bandgap covering the visible spectral range and the plasmon resonance of the doped metal oxide the near infrared. By means of a facile photodoping process, we tuned the plasmonic response and switched effectively the optical properties of the photonic crystal, translating the effect from the near infrared to the visible. The ultrafast bandgap pumping induces a signal change in the region of the photonic stopband, with recovery times of several picoseconds, providing a step toward the ultrafast optical switching. Optical modeling uncovers the importance to understand largely the variations of the dielectric function of the photodoped material, and variations in the high frequency region of the Drude response are responsible for the strong switching in the visible after photodoping. Our device configuration offers unprecedented tunablility due to flexibility in device design, cover wavelength ranges from the visible to the near infrared. Our findings indicate a new protocol to modify the optical response of photonic devices by optical triggers only.

cond-mat.mtrl-sci↗

arXiv2017

Broadband, electrically tuneable, third harmonic generation in graphene

Optical harmonic generation occurs when high intensity light ($>10^{10}$W/m$^{2}$) interacts with a nonlinear material. Electrical control of the nonlinear optical response enables applications such as gate-tunable switches and frequency converters. Graphene displays exceptionally strong-light matter interaction and electrically and broadband tunable third order nonlinear susceptibility. Here we show that the third harmonic generation efficiency in graphene can be tuned by over two orders of magnitude by controlling the Fermi energy and the incident photon energy. This is due to logarithmic resonances in the imaginary part of the nonlinear conductivity arising from multi-photon transitions. Thanks to the linear dispersion of the massless Dirac fermions, ultrabroadband electrical tunability can be achieved, paving the way to electrically-tuneable broadband frequency converters for applications in optical communications and signal processing.

cond-mat.mes-hall↗

arXiv2015

Probing equilibrium glass flow up to exapoise viscosities

Glasses are out-of-equilibrium systems aging under the crystallization threat. During ordinary glass formation, the atomic diffusion slows down rendering its experimental investigation impractically long, to the extent that a timescale divergence is taken for granted by many. We circumvent here these limitations, taking advantage of a wide family of glasses rapidly obtained by physical vapor deposition directly into the solid state, endowed with different "ages" rivaling those reached by standard cooling and waiting for millennia. Isothermally probing the mechanical response of each of these glasses, we infer a correspondence with viscosity along the equilibrium line, up to exapoise values. We find a dependence of the elastic modulus on the glass age, which, traced back to temperature steepness index of the viscosity, tears down one of the cornerstones of several glass transition theories: the dynamical divergence. Critically, our results suggest that the conventional wisdom picture of a glass ceasing to flow at finite temperature could be wrong.

cond-mat.dis-nn↗

arXiv2015

Quantum interference between charge excitation paths in a solid state Mott insulator

The competition between electron localization and de-localization in Mott insulators underpins the physics of strongly-correlated electron systems. Photo-excitation, which re-distributes charge between sites, can control this many-body process on the ultrafast timescale. To date, time-resolved studies have been performed in solids in which other degrees of freedom, such as lattice, spin, or orbital excitations come into play. However, the underlying quantum dynamics of bare electronic excitations has remained out of reach. Quantum many-body dynamics have only been detected in the controlled environment of optical lattices where the dynamics are slower and lattice excitations are absent. By using nearly-single-cycle near-IR pulses, we have measured coherent electronic excitations in the organic salt ET-F2TCNQ, a prototypical one-dimensional Mott Insulator. After photo-excitation, a new resonance appears on the low-energy side of the Mott gap, which oscillates at 25 THz. Time-dependent simulations of the Mott-Hubbard Hamiltonian reproduce the oscillations, showing that electronic delocalization occurs through quantum interference between bound and ionized holon-doublon pairs.

cond-mat.str-el↗

arXiv2015

Macrospin Dynamics in Antiferromagnets Triggered by Sub-20 femtosecond Injection of Nanomagnons

The understanding of how the sub-nanoscale exchange interaction evolves in macroscale correlations and ordered phases of matter, such as magnetism and superconductivity, requires to bridge the quantum and classical worlds. This monumental challenge has so far only been achieved for systems close to their thermodynamical equilibrium. Here we follow in real time the ultrafast dynamics of the macroscale magnetic order parameter triggered by the impulsive optical generation of spin excitations with the shortest possible nanometer-wavelength and femtosecond-period. Our experiments also disclose a possibility for the coherent control of these femtosecond nanomagnons, which are defined by the exchange energy. These findings open up novel opportunities for fundamental research on the role of short-wavelength spin excitations in magnetism and high-temperature superconductivity, since they provide a macroscopic probe of the femtosecond dynamics of sub-nanometer spin-spin correlations and, ultimately, of the exchange energy. With this approach it becomes possible to trace the dynamics of such short-range magnetic correlations for instance during phase transitions. Moreover, our work suggests that nanospintronics and nanomagnonics can employ phase-controllable spin waves with frequencies in the 20 THz domain.

cond-mat.mes-hall↗

arXiv2015

Valley and spin dynamics in monolayer MoS$_{2}$

Valleytronics targets the exploitation of the additional degrees of freedom in materials where the energy of the carriers may assume several equal minimum values (valleys) at non-equivalent points of the reciprocal space. In single layers of transition metal dichalcogenides (TMDs) the lack of inversion symmetry, combined with a large spin-orbit interaction, leads to a conduction (valence) band with different spin-polarized minima (maxima) having equal energies. This offers the opportunity to manipulate information at the level of the charge (electrons or holes), spin (up or down) and crystal momentum (valley). Any implementation of these concepts, however, needs to consider the robustness of such degrees of freedom, which are deeply intertwined. Here we address the spin and valley relaxation dynamics of both electrons and holes with a combination of ultrafast optical spectroscopy techniques, and determine the individual characteristic relaxation times of charge, spin and valley in a MoS$_{2}$ monolayer. These results lay the foundations for understanding the mechanisms of spin and valley polarization loss in two-dimensional TMDs: spin/valley polarizations survive almost two-orders of magnitude longer for holes, where spin and valley dynamics are interlocked, than for electrons, where these degrees of freedom are decoupled. This may lead to novel approaches for the integration of materials with large spin-orbit in robust spintronic/valleytronic platforms.

cond-mat.mtrl-sci↗

arXiv2015

Snapshots of the retarded interaction of charge carriers with ultrafast fluctuations in cuprates

One of the pivotal questions in the physics of high-temperature superconductors is whether the low-energy dynamics of the charge carriers is mediated by bosons with a characteristic timescale. This issue has remained elusive since electronic correlations are expected to dramatically speed up the electron-boson scattering processes, confining them to the very femtosecond timescale that is hard to access even with state-of-the-art ultrafast techniques. Here we simultaneously push the time resolution and the frequency range of transient reflectivity measurements up to an unprecedented level that enables us to directly observe the 16 fs build-up of the effective electron-boson interaction in hole-doped copper oxides. This extremely fast timescale is in agreement with numerical calculations based on the t-J model and the repulsive Hubbard model, in which the relaxation of the photo-excited charges is achieved via inelastic scattering with short-range antiferromagnetic excitations.

cond-mat.supr-con↗

arXiv2014

Strain-induced enhancement of the electron energy relaxation in strongly correlated superconductors

We use femtosecond optical spectroscopy to systematically measure the primary energy relaxation rate k1 of photoexcited carriers in cuprate and pnictide superconductors. We find that k1 increases monotonically with increased negative strain in the crystallographic a-axis. Generally, the Bardeen-Shockley deformation potential theorem and, specifically, pressure-induced Raman shifts reported in the literature suggest that increased negative strain enhances electron-phonon coupling, which implies that the observed direct correspondence between a and k1 is consistent with the canonical assignment of k1 to the electron-phonon interaction. The well-known non-monotonic dependence of the superconducting critical temperature Tc on the a-axis strain is also reflected in a systematic dependence Tc on k1, with a distinct maximum at intermediate values (~16 ps-1 at room temperature). The empirical non-monotonic systematic variation of Tc with the strength of the electron-phonon interaction provides us with unique insight into the role of electron-phonon interaction in relation to the mechanism of high-Tc superconductivity as a crossover phenomenon.

cond-mat.supr-con↗

arXiv2012

Ultrafast collinear scattering and carrier multiplication in graphene

Graphene is emerging as a viable alternative to conventional optoelectronic, plasmonic, and nanophotonic materials. The interaction of light with carriers creates an out-of-equilibrium distribution, which relaxes on an ultrafast timescale to a hot Fermi-Dirac distribution, that subsequently cools via phonon emission. Here we combine pump-probe spectroscopy, featuring extreme temporal resolution and broad spectral coverage, with a microscopic theory based on the quantum Boltzmann equation, to investigate electron-electron collisions in graphene during the very early stages of relaxation. We identify the fundamental physical mechanisms controlling the ultrafast dynamics in graphene, in particular the significant role of ultrafast collinear scattering, enabling Auger processes, including charge multiplication, key to improving photovoltage generation and photodetectors.

cond-mat.mes-hall↗

arXiv2012

Dynamics of four-photon photoluminescence in gold nanoantennas

Two-pulse correlation is employed to investigate the temporal dynamics of both two-photon photoluminescence (2PPL) and four-photon photoluminescence (4PPL) in resonant and nonresonant nanoantennas excited at a wavelength of 800 nm. Our data are consistent with the same two-step model being the cause of both 4PPL and 2PPL, implying that the first excitation step in 4PPL is a three-photon sp->sp direct interband transition. Considering energy and parity conservation, we also explain why 4PPL behavior is favored over three-and five-photon photoluminescence in the power range below the damage threshold of our antennas. Since sizeable 4PPL requires larger peak intensities of the local field, we are able to select either 2PPL or 4PPL in the same gold nanoantennas by choosing a suitable laser pulse duration. We thus provide a first consistent model for the understanding of multiphoton photoluminescence generation in gold nanoantennas, opening new perspectives for applications ranging from the characterization of plasmonic resonances to biomedical imaging.

physics.optics↗

arXiv2010

Electron-Phonon Coupling in High-Temperature Cuprate Superconductors Determined from Electron Relaxation Rates

We determined electronic relaxation times via pump-probe optical spectroscopy using sub-15 fs pulses for the normal state of two different cuprate superconductors.We show that the primary relaxation process is the electron-phonon interaction and extract a measure of its strength, the second moment of the Eliashberg functionλ<ω^{2}>=800\pm200 meV^{2} for La_{1.85}Sr_{0.15}CuO_{4} and λ<ω^{2}>=400\pm100 meV^{2} for YBa_{2}Cu_{3}O_{6.5}. These values suggest a possible fundamental role of the electron-phonon interaction in the superconducting pairing mechanism.

cond-mat.supr-con↗