Understanding the nature of the photoexcitation and ultrafast charge dynamics pathways in organic halide perovskite nanocubes and their aggregation into superlattices is key for potential applications as tunable light emitters, photon-harvesting materials, and light-amplification systems. In this work, we apply two-dimensional coherent electronic spectroscopy (2DES) to track in real time the formation of near-infrared optical excitons and their ultrafast relaxation in CH(NH)PbI nanocube superlattices. Our results unveil that the coherent ultrafast dynamics is limited by the combination of the inherent short exciton decay time (≃40 fs) and the dephasing due to the coupling with selective optical phonon modes at higher temperatures.
View Article and Find Full Text PDFThe 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.
View Article and Find Full Text PDFSingle 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.
View Article and Find Full Text PDFMott 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.
View Article and Find Full Text PDFTime-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.
View Article and Find Full Text PDFInternal 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.
View Article and Find Full Text PDFThe 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.
View Article and Find Full Text PDFThe 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.
View Article and Find Full Text PDFTraditionally, 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.
View Article and Find Full Text PDFScanning 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.
View Article and Find Full Text PDFThe 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.
View Article and Find Full Text PDFThe 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.
View Article and Find Full Text PDFThe 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.
View Article and Find Full Text PDFBeilstein J Nanotechnol
August 2012
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.
View Article and Find Full Text PDFColor 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.
View Article and Find Full Text PDFHigh-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.
View Article and Find Full Text PDFIn 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.
View Article and Find Full Text PDFThe 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.
View Article and Find Full Text PDFBeilstein J Nanotechnol
November 2011
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.
View Article and Find Full Text PDFNonlinear 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).
View Article and Find Full Text PDFPhotoemission 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.
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