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.

Surface optical sensitivity enhanced by a single dielectric microsphere.

Single dielectric microspheres can manipulate light focusing and collection to enhance optical interaction with surfaces. To demonstrate this principle, we experimentally investigate the enhancement of the Raman signal collected by a single dielectric microsphere, with a radius much larger than the exciting laser spot size, residing on the sample surface. The absolute microsphere-assisted Raman signal from a single graphene layer measured in air is more than a factor of two higher than that obtained with a high numerical aperture objective. Results from Mie's theory are used to benchmark numerical simulations and an analytical model to describe the isolated microsphere focusing properties. The analytical model and the numerical simulations justify the Raman signal enhancement measured in the microsphere-assisted Raman spectroscopy experiments.

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.

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.

Side Effects of Insecticides on Leaf-Miners and Gall-Inducers Depend on Species Ecological Traits and Competition with Leaf-Chewers.

Internal feeding is considered to shield sessile herbivorous insects from exposure to nonsystemic insecticides aerially sprayed against forest defoliators, although this has not been tested. It is, however, established that leaf damage caused by defoliators affects the survivorship and oviposition behavior of sessile herbivores. Thus feeding ecology and competition may mediate nontarget effects of insecticides on these insects. We tested the ecological sensitivity of 3 guilds of sessile herbivores (upper-surface leaf-miners, lower-surface leaf-miners, and gall-inducers) to the lipophilic larvicides diflubenzuron and tebufenozide aerially applied either at operational rates (12 g active ingredient [a.i.]/ha and 69.6 g [a.i.]/ha, respectively) or at maximum legal rates (60 g [a.i.]/ha and 180 g [a.i.]/ha, respectively), in German oak forests. Diflubenzuron affected leaf-miners at different life stages depending on their position on the leaf but had no effect on gall-inducers. Tebufenozide showed a similar, but not significant, pattern in leaf-miners and did not affect gall-inducers. By reducing the incidence of chewing damage on leaves, both insecticides offset the negative effect of competition on leaf-miner and gall-inducers. The net outcome of insecticide treatment was positive for guilds avoiding exposure, but negative for upper-surface leaf-miners. Exposure to insecticides in situ can be mediated by subtle differences in species biology and species interactions, with potential implications for organisms usually considered safe in risk assessment studies. Environ Toxicol Chem 2021;00:1-17. © 2020 The Authors. Environmental Toxicology and Chemistry published by Wiley Periodicals LLC on behalf of SETAC.

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.

Few-cycle Regime Atomic Force Microscopy.

Traditionally, dynamic atomic force microscopy (AFM) techniques are based on the analysis of the quasi-steady state response of the cantilever deflection in terms of Fourier analysis. Here we describe a technique that instead exploits the often disregarded transient response of the cantilever through a relatively modern mathematical tool, which has caused important developments in several scientific fields but that is still quite unknown in the AFM context: the wavelet analysis. This tool allows us to localize the time-varying spectral composition of the initial oscillations of the cantilever deflection when an impulsive excitation is given (as in the band excitation method), a mode that we call the few-cycle regime. We show that this regime encodes very meaningful information about the tip-sample interaction in a unique and extremely sensitive manner. We exploit this high sensitivity to gain detailed insight into multiple physical parameters that perturb the dynamics of the AFM probe, such as the tip radius, Hamaker constant, sample's elastic modulus and height of an adsorbed water layer. We validate these findings with experimental evidence and computational simulations and show a feasible path towards the simultaneous retrieval of multiple physical parameters.

Theory of Single-Impact Atomic Force Spectroscopy in liquids with material contrast.

Scanning probe microscopy has enabled nanoscale mapping of mechanical properties in important technological materials, such as tissues, biomaterials, polymers, nanointerfaces of composite materials, to name only a few. To improve and widen the measurement of nanoscale mechanical properties, a number of methods have been proposed to overcome the widely used force-displacement mode, that is inherently slow and limited to a quasi-static regime, mainly using multiple sinusoidal excitations of the sample base or of the cantilever. Here, a different approach is put forward. It exploits the unique capabilities of the wavelet transform analysis to harness the information encoded in a short duration spectroscopy experiment. It is based on an impulsive excitation of the cantilever and a single impact of the tip with the sample. It performs well in highly damped environments, which are often seen as problematic in other standard dynamic methods. Our results are very promising in terms of viscoelastic property discrimination. Their potential is oriented (but not limited) to samples that demand imaging in liquid native environments and also to highly vulnerable samples whose compositional mapping cannot be obtained through standard tapping imaging techniques.

Transient eigenmodes analysis of single-impact cantilever dynamics combining Fourier and wavelet transforms.

The transient eigenmode structure of an interacting cantilever during a single impact on different surfaces evidences the excitation of higher flexural modes and low frequency oscillations. The frequency shift of the fundamental mode after the tip comes into contact with the sample surface allows calculating the tip-sample interaction stiffness and evidences the role of capillary condensation and surface wettability on the cantilever dynamics. Wavelet transforms are used to trace the origin of spectral features in the cantilever spectra and calculate force gradients of the tip-sample interaction.

Energy dissipation in multifrequency atomic force microscopy.

The instantaneous displacement, velocity and acceleration of a cantilever tip impacting onto a graphite surface are reconstructed. The total dissipated energy and the dissipated energy per cycle of each excited flexural mode during the tip interaction is retrieved. The tip dynamics evolution is studied by wavelet analysis techniques that have general relevance for multi-mode atomic force microscopy, in a regime where few cantilever oscillation cycles characterize the tip-sample interaction.

Complex force dynamics in atomic force microscopy resolved by wavelet transforms.

The amplitude and phase evolution of the oscillations of a cantilever after a single tip-sample impact are investigated using a cross-correlation wavelet analysis. The excitation of multiple flexural modes is evidenced and the instantaneous amplitude and phase evolution is extracted from the experimental data at all frequencies simultaneously. The instantaneous total force acting on the tip during a single impact is reconstructed. This method has general relevance for the development of an atomic force spectroscopy of single tip-sample interactions, that develop in a few oscillation cycles of the interacting cantilever eigenmodes and their harmonics.

Wavelet cross-correlation and phase analysis of a free cantilever subjected to band excitation.

This work introduces the concept of time-frequency map of the phase difference between the cantilever response signal and the driving signal, calculated with a wavelet cross-correlation technique. The wavelet cross-correlation quantifies the common power and the relative phase between the response of the cantilever and the exciting driver, yielding "instantaneous" information on the driver-response phase delay as a function of frequency. These concepts are introduced through the calculation of the response of a free cantilever subjected to continuous and impulsive excitation over a frequency band.

High pressure effect on the color of minced cured restructured ham at different levels of drying, pH, and NaCl.

Color changes of minced cured restructured ham was studied considering the effects of high pressure (HP) treatment (600MPa, 13°C, 5min), raw meat pH(24) (low, normal, high), salt content (15, 30g/kg), and drying (20%, 50% weight loss). Raw hams were selected based on pH(24) in Semimembranosus, mixed with additives, frozen, sliced, and dried using the Quick-Dry-Slice® process. Meat color (CIE 1976 L*a*b*) and reflectance spectra were measured before and after HP treatment. HP significantly increased L*, decreased a*, and decreased b* for restructured ham dried to 20% weight loss, regardless of salt content and pH(24). L* and a* were best preserved in high pH/high salt restructured ham. HP had no effect on the color of restructured ham dried to 50% weight loss. HP had no effect on the shape of reflectance curves, indicating that the pigment responsible for minced cured restructured ham color did not change due to HP.

Probing thermomechanics at the nanoscale: impulsively excited pseudosurface acoustic waves in hypersonic phononic crystals.

High-frequency surface acoustic waves can be generated by ultrafast laser excitation of nanoscale patterned surfaces. Here we study this phenomenon in the hypersonic frequency limit. By modeling the thermomechanics from first-principles, we calculate the system's initial heat-driven impulsive response and follow its time evolution. A scheme is introduced to quantitatively access frequencies and lifetimes of the composite system's excited eigenmodes. A spectral decomposition of the calculated response on the eigemodes of the system reveals asymmetric resonances that result from the coupling between surface and bulk acoustic modes. This finding allows evaluation of impulsively excited pseudosurface acoustic wave frequencies and lifetimes and expands our understanding of the scattering of surface waves in mesoscale metamaterials. The model is successfully benchmarked against time-resolved optical diffraction measurements performed on one-dimensional and two-dimensional surface phononic crystals, probed using light at extreme ultraviolet and near-infrared wavelengths.

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)).

Wavelet transforms to probe long- and short-range forces by thermally excited dynamic force spectroscopy.

The use of wavelet transforms in thermally excited dynamic force spectroscopy allows us to gain insight into the fundamental thermodynamical properties of a cantilever's Brownian motion as well as giving a meaningful and intuitive representation of the cantilever dynamics in time and frequency caused by the interaction with long- and short-range forces. The possibility of carrying out measurements across the jump-to-contact transition without interruption, providing information on both van der Waals forces and short-range adhesion surface forces, is remarkable.

Tip-sample interactions on graphite studied using the wavelet transform.

Wavelet transform analysis is applied to a thermally excited cantilever to get insights into fundamental thermodynamical properties of its motion. The shortcomings of the widely used Fourier analysis are briefly discussed to put into perspective the wavelet transform analysis, used to describe the temporal evolution of the spectral content of the thermal oscillations of a cantilever with an interacting tip. This analysis allows to retrieve the force gradients, the forces and the Hamaker constant in a measurement time of less than 40 ms.

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.