Halide Perovskite Artificial Solids as a New Platform to Simulate Collective Phenomena in Doped Mott Insulators.

The development of quantum simulators, artificial platforms where the predictions of many-body theories of correlated quantum materials can be tested in a controllable and tunable way, is one of the main challenges of condensed matter physics. Here we introduce artificial lattices made of lead halide perovskite nanocubes as a new platform to simulate and investigate the physics of correlated quantum materials. We demonstrate that optical injection of quantum confined excitons in this system realizes the two main features that ubiquitously pervade the phase diagram of many quantum materials: collective phenomena, in which long-range orders emerge from incoherent fluctuations, and the excitonic Mott transition, which has one-to-one correspondence with the insulator-to-metal transition described by the repulsive Hubbard model in a magnetic field. Our results demonstrate that time-resolved experiments provide a quantum simulator that is able to span a parameter range relevant for a broad class of phenomena, such as superconductivity and charge-density waves.

Nanoscale self-organization and metastable non-thermal metallicity in Mott insulators.

Mott transitions in real materials are first order and almost always associated with lattice distortions, both features promoting the emergence of nanotextured phases. This nanoscale self-organization creates spatially inhomogeneous regions, which can host and protect transient non-thermal electronic and lattice states triggered by light excitation. Here, we combine time-resolved X-ray microscopy with a Landau-Ginzburg functional approach for calculating the strain and electronic real-space configurations. We investigate V2O3, the archetypal Mott insulator in which nanoscale self-organization already exists in the low-temperature monoclinic phase and strongly affects the transition towards the high-temperature corundum metallic phase. Our joint experimental-theoretical approach uncovers a remarkable out-of-equilibrium phenomenon: the photo-induced stabilisation of the long sought monoclinic metal phase, which is absent at equilibrium and in homogeneous materials, but emerges as a metastable state solely when light excitation is combined with the underlying nanotexture of the monoclinic lattice.

Thermal dynamics and electronic temperature waves in layered correlated materials.

Understanding the mechanism of heat transfer in nanoscale devices remains one of the greatest intellectual challenges in the field of thermal dynamics, by far the most relevant under an applicative standpoint. When thermal dynamics is confined to the nanoscale, the characteristic timescales become ultrafast, engendering the failure of the common description of energy propagation and paving the way to unconventional phenomena such as wave-like temperature propagation. Here, we explore layered strongly correlated materials as a platform to identify and control unconventional electronic heat transfer phenomena. We demonstrate that these systems can be tailored to sustain a wide spectrum of electronic heat transport regimes, ranging from ballistic, to hydrodynamic all the way to diffusive. Within the hydrodynamic regime, wave-like temperature oscillations are predicted up to room temperature. The interaction strength can be exploited as a knob to control the dynamics of temperature waves as well as the onset of different thermal transport regimes.

Discrimination of nano-objects via cluster analysis techniques applied to time-resolved thermo-acoustic microscopy.

Time-effective, unsupervised clustering techniques are exploited to discriminate nanometric metal disks patterned on a dielectric substrate. The discrimination relies on cluster analysis applied to time-resolved optical traces obtained from thermo-acoustic microscopy based on asynchronous optical sampling. The analysis aims to recognize similarities among nanopatterned disks and to cluster them accordingly. Each cluster is characterized by a fingerprint time-resolved trace, synthesizing the common features of the thermo-acoustics response of the composing elements. The protocol is robust and widely applicable, not relying on any specific knowledge of the physical mechanisms involved. The present route constitutes an alternative diagnostic tool for on-chip non-destructive testing of individual nano-objects.

Optical and mechanical properties of streptavidin-conjugated gold nanospheres through data mining techniques.

The thermo-mechanical properties of streptavidin-conjugated gold nanospheres, adhered to a surface via complex molecular chains, are investigated by two-color infrared asynchronous optical sampling pump-probe spectroscopy. Nanospheres with different surface densities have been deposited and exposed to a plasma treatment to modify their polymer binding chains. The aim is to monitor their optical response in complex chemical environments that may be experienced in, e.g., photothermal therapy or drug delivery applications. By applying unsupervised learning techniques to the spectroscopic traces, we identify their thermo-mechanical response variation. This variation discriminates nanospheres in different chemical environments or different surface densities. Such discrimination is not evident based on a standard analysis of the spectroscopic traces. This kind of analysis is important, given the widespread application of conjugated gold nanospheres in medicine and biology.

Tuning the Ultrafast Response of Fano Resonances in Halide Perovskite Nanoparticles.

The full control of the fundamental photophysics of nanosystems at frequencies as high as few THz is key for tunable and ultrafast nanophotonic devices and metamaterials. Here we combine geometrical and ultrafast control of the optical properties of halide perovskite nanoparticles, which constitute a prominent platform for nanophotonics. The pulsed photoinjection of free carriers across the semiconducting gap leads to a subpicosecond modification of the far-field electromagnetic properties that is fully controlled by the geometry of the system. When the nanoparticle size is tuned so as to achieve the overlap between the narrowband excitons and the geometry-controlled Mie resonances, the ultrafast modulation of the transmittivity is completely reversed with respect to what is usually observed in nanoparticles with different sizes, in bulk systems, and in thin films. The interplay between chemical, geometrical, and ultrafast tuning offers an additional control parameter with impact on nanoantennas and ultrafast optical switches.

Temperonic Crystal: A Superlattice for Temperature Waves in Graphene.

The temperonic crystal, a periodic structure with a unit cell made of two slabs sustaining temperature wavelike oscillations on short timescales, is introduced. The complex-valued dispersion relation for the temperature scalar field is investigated for the case of a localized temperature pulse. The dispersion discloses frequency gaps, tunable upon varying the slabs' thermal properties. Results are shown for the paradigmatic case of a graphene-based temperonic crystal. The temperonic crystal extends the concept of superlattices to the realm of temperature waves, allowing for coherent control of ultrafast temperature pulses in the hydrodynamic regime at above liquid nitrogen temperatures.

Photoacoustic Sensing of Trapped Fluids in Nanoporous Thin Films: Device Engineering and Sensing Scheme.

Accessing fluid infiltration in nanogranular coatings is an outstanding challenge, of relevance for applications ranging from nanomedicine to catalysis. A sensing platform, allowing quantifying the amount of fluid infiltrated in a nanogranular ultrathin coating, with thickness in the 10-40 nm range, is here proposed and theoretically investigated by multiscale modeling. The scheme relies on impulsive photoacoustic excitation of hypersonic mechanical breathing modes in engineered gas-phase-synthesized nanogranular metallic ultrathin films and time-resolved acousto-optical read-out of the breathing modes frequency shift upon liquid infiltration. A superior sensitivity, exceeding 26 × 103 cm2/g, is predicted upon equivalent areal mass loading of a few ng/mm2. The capability of the present scheme to discriminate among different infiltration patterns is discussed. The platform is an ideal tool to investigate nanofluidics in granular materials and naturally serves as a distributed nanogetter coating, integrating fluid sensing capabilities. The proposed scheme is readily extendable to other nanoscale and mesoscale porous materials.

Dynamics of correlation-frozen antinodal quasiparticles in superconducting cuprates.

Many puzzling properties of high-critical temperature (Tc) superconducting (HTSC) copper oxides have deep roots in the nature of the antinodal quasiparticles, the elementary excitations with wave vector parallel to the Cu-O bonds. These electronic states are most affected by the onset of antiferromagnetic correlations and charge instabilities, and they host the maximum of the anisotropic superconducting gap and pseudogap. We use time-resolved extreme-ultraviolet photoemission with proper photon energy (18 eV) and time resolution (50 fs) to disclose the ultrafast dynamics of the antinodal states in a prototypical HTSC cuprate. After photoinducing a nonthermal charge redistribution within the Cu and O orbitals, we reveal a dramatic momentum-space differentiation of the transient electron dynamics. Whereas the nodal quasiparticle distribution is heated up as in a conventional metal, new quasiparticle states transiently emerge at the antinodes, similarly to what is expected for a photoexcited Mott insulator, where the frozen charges can be released by an impulsive excitation. This transient antinodal metallicity is mapped into the dynamics of the O-2p bands, thus directly demonstrating the intertwining between the low- and high-energy scales that is typical of correlated materials. Our results suggest that the correlation-driven freezing of the electrons moving along the Cu-O bonds, analogous to the Mott localization mechanism, constitutes the starting point for any model of high-Tc superconductivity and other exotic phases of HTSC cuprates.

Witnessing the formation and relaxation of dressed quasi-particles in a strongly correlated electron system.

The non-equilibrium approach to correlated electron systems is often based on the paradigm that different degrees of freedom interact on different timescales. In this context, photo-excitation is treated as an impulsive injection of electronic energy that is transferred to other degrees of freedom only at later times. Here, by studying the ultrafast dynamics of quasi-particles in an archetypal strongly correlated charge-transfer insulator (La2CuO(4+δ)), we show that the interaction between electrons and bosons manifests itself directly in the photo-excitation processes of a correlated material. With the aid of a general theoretical framework (Hubbard-Holstein Hamiltonian), we reveal that sub-gap excitation pilots the formation of itinerant quasi-particles, which are suddenly dressed by an ultrafast reaction of the bosonic field.

Revealing the high-energy electronic excitations underlying the onset of high-temperature superconductivity in cuprates.

In strongly correlated systems the electronic properties at the Fermi energy (E(F)) are intertwined with those at high-energy scales. One of the pivotal challenges in the field of high-temperature superconductivity (HTSC) is to understand whether and how the high-energy scale physics associated with Mott-like excitations (|E-E(F)|>1 eV) is involved in the condensate formation. Here, we report the interplay between the many-body high-energy CuO(2) excitations at 1.5 and 2 eV, and the onset of HTSC. This is revealed by a novel optical pump-supercontinuum-probe technique that provides access to the dynamics of the dielectric function in Bi(2)Sr(2)Ca(0.92)Y(0.08)Cu(2)O(8+δ) over an extended energy range, after the photoinduced suppression of the superconducting pairing. These results unveil an unconventional mechanism at the base of HTSC both below and above the optimal hole concentration required to attain the maximum critical temperature (T(c)).

Experimental evidence of above-threshold photoemission in solids.

Nonlinear photoemission from a silver single crystal is investigated by femtosecond laser pulses in a perturbative regime. A clear observation of above-threshold photoemission in solids is reported for the first time. The ratio between the three-photon above-threshold and the two-photon Fermi edges is found to be 10(-4). This value constitutes the only available benchmark for theories aimed at understanding the mechanism responsible for above-threshold photoemission in solids.

Violation of the electric-dipole selection rules in indirect multiphoton excitation of image-potential states on Ag(100).

Photoemission from image potential states on Ag(100) is investigated using angle resolved multiphoton photoemission induced by 150 fs laser pulses. For the first time we demonstrate that image potential states populated by indirect transitions can be observed with light polarized parallel to the plane of incidence and light polarized normal to the plane of incidence. The latter is a process normally forbidden by the dipole transition selection rules. These findings are related to the creation of a hot-electron population whose properties largely remains to be understood.