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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. ispartof: NATURE COMMUNICATIONS vol:13 issue:1 ispartof: location:England status: published

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.

International audience; 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.

The influence of Mott physics on the doping–temperature phase diagram of copper oxides represents a major issue that is the subject of intense theoretical and experimental efforts. Here, we investigate the ultrafast electron dynamics in prototypical single-layer Bi-based cuprates at the energy scale of the O-2p → Cu-3d charge-transfer (CT) process. We demonstrate a clear evolution of the CT excitations from incoherent and localized, as in a Mott insulator, to coherent and delocalized, as in a conventional metal. This reorganization of the high-energy degrees of freedom occurs at the critical doping pcr ≈ 0.16 irrespective of the temperature, and it can be well described by dynamical mean-field theory calculations. We argue that the onset of low-temperature charge instabilities is the low-energy manifestation of the underlying Mottness that characterizes the p < pcr region of the phase diagram. This discovery sets a new framework for theories of charge order and low-temperature phases in underdoped copper oxides. The electron dynamics of single-layer Bi2Sr2−xLaxCuO6+δ is studied as a function of doping, revealing the evolution of charge-transfer excitations from incoherent and localized (as in a Mott insulator) to coherent and delocalized (as in a conventional metal).

A new paradigm for active nanophotonic structures and metadevices based on perovskites has recently emerged due to several unique features of these materials such as room-temperature exciton, tunable bandgap energy, and low-cost fabrication methods [1,2]. Progress towards future applications requiring dynamical control of the optical response will depend on our understanding of photoexcitations in these systems [3,4]. In this work, we report the first experimental observation of ultrafast all-optical modulation of Fano resonant halide perovskite nanoparticles (NP). Our measurements, corroborated by analytical and numerical models, show that the out-of-equilibrium dynamics of these systems can be thoroughly controlled by engineering the NP size.

Multiorbital correlated materials are often on the verge of multiple electronic phases (metallic, insulating, superconducting, charge and orbitally ordered), which can be explored and controlled by small changes of the external parameters. The use of ultrashort light pulses as a mean to transiently modify the band population is leading to fundamentally new results. In this paper we will review recent advances in the field and we will discuss the possibility of manipulating the orbital polarization in correlated multi-band solid state systems. This technique can provide new understanding of the ground state properties of many interesting classes of quantum materials and offers a new tool to induce transient emergent properties with no counterpart at equilibrium. We will address: the discovery of high-energy Mottness in superconducting copper oxides and its impact on our understanding of the cuprate phase diagram; the instability of the Mott insulating phase in photoexcited vanadium oxides; the manipulation of orbital-selective correlations in iron-based superconductors; the pumping of local electronic excitons and the consequent transient effective quasiparticle cooling in alkali-doped fullerides. Finally, we will discuss a novel route to manipulate the orbital polarization in a a k-resolved fashion. © 2018 COPYRIGHT SPIE. Downloading of the abstract is permitted for personal use only.

© 2017 American Chemical Society. Ultrathin metal nanoparticles coatings, synthesized by gas-phase deposition, are emerging as go-to materials in a variety of fields ranging from pathogens control and sensing to energy storage. Predicting their morphology and mechanical properties beyond a trial-and-error approach is a crucial issue limiting their exploitation in real-life applications. The morphology and mechanical properties of Ag nanoparticle ultrathin films, synthesized by supersonic cluster beam deposition, are here assessed adopting a bottom-up, multitechnique approach. A virtual film model is proposed merging high resolution scanning transmission electron microscopy, supersonic cluster beam dynamics, and molecular dynamics simulations. The model is validated against mechanical nanometrology measurements and is readily extendable to metals other than Ag. The virtual film is shown to be a flexible and reliable predictive tool to access morphology-dependent properties such as mesoscale gas-dynamics and elasticity of ultrathin films synthesized by gas-phase deposition. ispartof: Journal of Physical Chemistry C vol:121 issue:40 pages:22434-22441 status: published

In the synthesis of nanostructures by pulsed laser deposition (PLD), a crucial role is played by the environmental deposition pressure and the substrate temperature. Due to the high temperature of nanoparticles (NPs) at landing, other factors may determine the structure of the resulting aggregates. Here, Au and TiO2 nanostructures are obtained by non-thermal fs-PLD in ambient conditions. On Si(100), only TiO2 NPs form fractals with areas up to ~ 1 × 106 nm2, while on quartz Au NPs also form fractals with areas up to ~ 5 × 103 nm2, a much smaller size with respect to the TiO2 case. The aggregation is described by a simple diffusive model, taking into account isotropic diffusion of the NPs, allowing quantitative simulations of the NPs and fractal area. The results highlight the key role of substrate thermal conductivity in determining the formation of fractals. [Figure not available: see fulltext.].

The Thermal Boundary Resistance at the interface between a nanosized Al film and an Al_{2}O_{3} substrate is investigated at an atomistic level. A room temperature value of 1.4 m^{2}K/GW is found. The thermal dynamics occurring in time-resolved thermo-reflectance experiments is then modelled via macro-physics equations upon insertion of the materials parameters obtained from atomistic simulations. Electrons and phonons non-equilibrium and spatio-temporal temperatures inhomo- geneities are found to persist up to the nanosecond time scale. These results question the validity of the commonly adopted lumped thermal capacitance model in interpreting transient nanocalorimetry experiments. The strategy adopted in the literature to extract the Thermal Boundary Resistance from transient reflectivity traces is revised at the light of the present findings. The results are of relevance beyond the specific system, the physical picture being general and readily extendable to other heterojunctions., 12 pages, 8 figures

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.

One-color transient reflectivity measurements are carried out on two different samples of vertically aligned single-wall carbon nanotube bundles and compared with the response recently published on unaligned bundles. The negative sign of the optical response for both samples indicates that the free electron character revealed on unaligned bundles is only due to the intertube interactions favored by the tube bending. Neither the presence of bundles nor the existence of structural defects in aligned bundles is able to induce a free-electron like behavior of the photoexcited carriers. This result is also confirmed by the presence of non-linear excitonic effects in the transient response of the aligned bundles. (C) 2013 Elsevier B.V. All rights reserved.

High-resolution time resolved transmittivity measurements on horizontally aligned free-standing multi-walled carbon nanotubes reveal a different electronic transient behavior from that of graphite. This difference is ascribed to the presence of discrete energy states in the multishell carbon nanotube electronic structure. Probe polarization dependence suggests that the optical transitions involve definite selection rules. The origin of these states is discussed and a rate equation model is proposed to rationalize our findings.

We use time- and energy-resolved optical spectroscopy to investigate the coupling of electron-hole excitations to the magnetic environment in the relativistic Mott insulator Na$_2$IrO$_3$. We show that, on the picosecond timescale, the photoinjected electron-hole pairs delocalize on the hexagons of the Ir lattice via the formation of quasi-molecular orbital (QMO) excitations and the exchange of energy with the short-range-ordered zig-zag magnetic background. The possibility of mapping the magnetic dynamics, which is characterized by typical frequencies in the THz range, onto high-energy (1-2 eV) charge excitations provides a new platform to investigate, and possibly control, the dynamics of magnetic interactions in correlated materials with strong spin-orbit coupling, even in the presence of complex magnetic phases., 5 pages, 4 figures, supplementary information

The possibility of investigating the dynamics of solids on timescales faster than the thermalization of the internal degrees of freedom has disclosed novel non-equilibrium phenomena that have no counterpart at equilibrium. Transition metal oxides (TMOs) provide an interesting playground in which the correlations among the charges in the metal $d$-orbitals give rise to a wealth of intriguing electronic and thermodynamic properties involving the spin, charge, lattice and orbital orders. Furthermore, the physical properties of TMOs can be engineered at the atomic level, thus providing the platform to investigate the transport phenomena on timescales of the order of the intrinsic decoherence time of the charge excitations. Here, we review and discuss three paradigmatic examples of transient emerging properties that are expected to open new fields of research: i) the creation of non-thermal magnetic states in spin-orbit Mott insulators; ii) the possible exploitation of quantum paths for the transport and collection of charge excitations in TMO-based few-monolayers devices; iii) the transient wave-like behavior of the temperature field in strongly anisotropic TMOs., Comment: 39 pages, 7 figures

The specific mechanisms which leads to the formation of fractal nanostructures by pulsed laser deposition remain elusive despite intense research efforts, motivated mainly by the technological interest in obtaining tailored nanostructures with simple and scalable production methods. Here we focus on fractal nanostructures of titanium dioxide, $TiO_2$, a strategic material for many applications, obtained by femtosecond laser ablation at ambient conditions. We model the fractal formation through extensive Monte Carlo simulations based on a set of minimal assumptions: irreversible sticking and size independent diffusion. Our model is able to reproduce the fractal dimensions and the area distributions of the nanostructures obtained in the experiments for different densities of the ablated material. The comparison of theory and experiment show that such fractal aggregates are formed after landing of the ablated material on the substrate surface by a diffusive mechanism. Finally we discuss the role of the thermal conductivity of the substrate and the laser fluence on the properties of the fractal nanostructures. Our results represent an advancement towards controlling the production of fractal nanostructures by pulsed laser deposition., Comment: 21 pages

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.

Using time-resolved reflectivity measurements on unaligned and aligned bundled single-wall carbon nanotubes with a pump energy of 1.55 eV, quasi-resonant with the second Van Hoye singularity of semiconducting tubes, a positive sign of the transient reflectivity is detected in unaligned nanotubes. In contrast a negative sign is detected in aligned nanotubes. This discovery addresses a long-standing question showing that in unaligned nanotubes the stronger intertube interactions favor the formation of short-lived free charge carriers in semiconducting tubes. A detailed analysis of the transient reflectivity spectral response shows that the free carriers in the photo-excited state of semiconducting tubes move towards metallic tubes in about 400 fs. (C) 2011 Elsevier Ltd. All rights reserved.

The response of the torsional modes of a thermally excited cantilever across the jump-to-contact transition shows a modification of the oscillation amplitude, frequency, and damping. The measurement of these parameters is important because their analysis provides nanoscale information on the physical, chemical, and topographic properties of the sample. The tip-surface interaction potential is usually reconstructed by Fourier analysis of the cantilever oscillations around its equilibrium position. However, Fourier analysis can be correctly interpreted only in the case of stationary systems. The wavelet transform analysis overcomes these limitations, revealing the temporal evolution of the spectral content of a temporal trace. The one-dimensional time signal from the photodiode is converted into a two-dimensional time-frequency topography, which simultaneously exhibits the time and frequency behavior of the cantilever thermal fluctuations. In the present study, we show preliminary data obtained using wavelet transforms to analyze thermally excited torsional cantilever modes during jump-to-contact transition on a highly oriented pyrolitic graphite surface in air. [DOI: 10.1380/ejssnt.2011.228]

Transparent glasses having molar composition (23-x)K{sub 2}O.xNa{sub 2}O.27Nb{sub 2}O{sub 5}.50SiO{sub 2} (x=0, 5, 10, 15 and 23) have been synthesized by the melt-quenching technique and their devitrification behaviour has been investigated by DTA and XRD. Depending on the composition, the glasses showed a glass transition temperature in the range 660-680 deg. C and devitrified in several steps. XRD measurements showed that the replacement of K{sub 2}O by Na{sub 2}O strongly affects the crystallization behaviour. Particularly, in the glasses with only potassium or low sodium content the first devitrification step is related to the crystallization of an unidentified phase, while in the glass containing only sodium, NaNbO{sub 3} crystallizes. For an intermediate sodium content (x=10 and 15) a potassium sodium niobate crystalline phase, belonging to the tungsten-bronze family, is formed by bulk nucleation. This system looks promising to produce active nanostructured glasses as the tungsten-bronze type crystals have ferroelectric, electro-optical and non-linear optical properties. Preliminary measurements evidenced SHG activity in the crystallized glasses containing this phase. - Graphical abstract: Synthesis of glasses (23-x)K{sub 2}O.xNa{sub 2}O.27Nb{sub 2}O{sub 5}.50SiO{sub 2} (x=0, 5, 10, 15 and 23) from which SHG active phases crystallize by bulk nucleation for non-linear optical nanostructured glasses.

The way organic thin films properties are affected by molecular interactions at surfaces is an important research topic because thin molecular films constitute a model system for biological research and have applications ranging from light-emitting diodes and solar cells to chemical sensors. In this work, the formation of thin films of Methylene Blue in aqueous solution at a fused quartz surface was investigated with evanescent wave absorption spectroscopy, using a continuum spectrum generated in a non-linear fiber by short laser pulses.

The use of femtosecond laser pulses to impulsively excite thermal and mechanical transients in matter has led, in the last years, to the development of picosecond acoustics. Recently, the pump-probe approach has been applied to nano-engineered materials to optically generate and detect acoustic waves in the GHz-THz frequency range. In this paper, we review the latest advances on ultrafast generation and detection of thermal gradients and pseudo-surface acoustic waves in two-dimensional lattices of metallic nanostructures. Comparing the experimental findings to the numeric analysis of the full thermo-mechanical problem, these materials emerge as model systems to investigate both the mechanical and thermal energy transfer at the nanoscale. The sensitivity of the technique to the nanostructures mass and shape variations, coupled to the phononic crystal properties of the lattices opens the way to a variety of applications ranging from hypersonic waveguiding to mass sensors with femtosecond time-resolution.ens the way to a variety of applications ranging from hypersonic waveguiding to mass sensors with femtosecond time-resolution., Comment: 20 pages, 6 figures. Published on IEEE Photonics Journal

In this review we describe the development of ultrafast non-linear photoemission spectroscopy on metals from the first historic observations in the sixties to state-of-the-art experiments. We present an account that is focused on electron spectroscopy experiments that use short laser pulses to investigate the non-equilibrium response of electrons in metals. Several examples of the application of non-linear spectroscopy to the investigation of many-body effects and highly non-equilibrium processes will be illustrated. Furthermore, we give a brief overview of the wide spectrum of experimental methods based on non-linear photoemission spectroscopy.

Fractal TiO2 nanostructures in crystalline form are obtained at ambient pressure and temperature by pulsed laser deposition with femtosecond pulses. The synthesized structures have been studied by scanning electron microscopy, Raman spectroscopy, and X-ray photoemission spectroscopy. We show that the dendritic aggregations deposited on silicon wafers at room temperature are fractals. They are composed by nanoparticles with an average diameter in a range below 20 nm, with the presence of larger nanoparticles with a diameter above 50 nm. We demonstrate that the fractal dimension and area can be tuned by varying laser fluence and sample/target distance. X-ray photoemission spectroscopy shows that the as-deposited nanostructures are TiO2 while Raman spectroscopy reveals that the crystalline structure of fractals and nanoparticles are composed either by rutile or anatase phase, with a dominant relative concentration of anatase. We discuss possible mechanism of fractals and nanoparticles formation in comparison with the literature results.

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.

International audience; The impulsive acoustic dynamics of soft polymeric surface phononic crystals is investigated here in the hypersonic frequency range by near-IR time-resolved optical diffraction. The acoustic response is analysed by means of wavelet spectral methods and finite element modeling. An unprecedented class of acoustic modes propagating within the polymer surface phononic crystal and confined within 100 nm of the nano-patterned interface is revealed. The present finding opens the path to an alternative paradigm for characterizing the mechanical properties of soft polymers at interfaces and for sensing schemes exploiting polymers as embedding materials.

An optical discrimination technique, tailored to nanometric-sized, low optical absorbance molecular complexes adhering to thin metal films, is proposed and demonstrated. It is based on a time-resolved evanescent-wave detection scheme in conjunction with hierarchical cluster analysis and principal value decomposition. The present approach aims to differentiate among molecular films based on statistical methods, without using previous detailed knowledge of the physical mechanisms responsible for the detected signal. The technique is open to integration in lab-on-a-chip architectures and nanoscopy platforms for applications ranging from medical screening to material diagnostics.

The application of all-optical time resolved techniques to nanostructured surface phononic crystals (SPCs) enables the generation and detection of hypersonic frequency surface acoustic waves up to 50 GHz, with great potential for innovations in nanometrology and sensing applications. In this paper, we review the advances in this field in both experiments and theory, focusing on the progress in nondestructive nanometrology of ultrathin films, on the potential for a dramatic increase in the sensitivity of mass sensors due to enhanced acoustic wave surface confinement, and on the evolution of this approach to include polymer-coated SPCs for soft material and gas sensing applications. A survey of the enabling innovative optical technologies involved is presented.

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., Comment: to appear in Nature Physics

Intrinsic linewidths of electronic image-potential states versus the momentum parallel to the surface on Ag(1 0 0) have been measured with angle resolved two-photon photoemission using the time of flight technique. The influence of the time of flight spectrometer angular acceptance on intrinsic linewidth measurements is taken into account and a proper data analysis is proposed. The inverse linewidth as a function of parallel momentum is compared with time-resolved measurements of image-state lifetimes on Ag(1 0 0) and Cu(1 0 0) reported in the literature. The data analysis shows that decay dynamics of image potential states in Ag and Cu may be determined by different physical mechanisms.

A major challenge in understanding the cuprate superconductors is to clarify the nature of the fundamental electronic correlations that lead to the pseudogap phenomenon. Here we use ultrashort light pulses to prepare a non-thermal distribution of excitations and capture novel properties that are hidden at equilibrium. Using a broadband (0.5-2 eV) probe we are able to track the dynamics of the dielectric function, unveiling an anomalous decrease of the scattering rate of the charge carriers in a pseudogap-like region of the temperature ($T$) and hole-doping ($p$) phase diagram. In this region, delimited by a well-defined $T^*_{neq}(p)$ line, the photo-excitation process triggers the evolution of antinodal excitations from gapped (localized) to delocalized quasi-particles characterized by a longer lifetime. The novel concept of photo-enhanced antinodal conductivity is naturally explained within the single-band Hubbard model, in which the short-range Coulomb repulsion leads to a k-space differentiation between "nodal" quasiparticles and antinodal excitations., accepted for publication on Nature Communications

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.

In strongly correlated materials the electronic and optical properties are significantly affected by the coupling of fermionic quasiparticles to different degrees of freedom, such as lattice vibrations and bosonic excitations of electronic origin. Broadband ultrafast spectroscopy is emerging as the premier technique to unravel the subtle interplay between quasiparticles and electronic or phononic collective excitations, by their different characteristic timescales and spectral responses. By investigating the femtosecond dynamics of the optical properties of Y-Bi2212 crystals over the 0.5-2 eV energy range, we disentangle the electronic and phononic contributions to the generalized electron-boson Eliashberg function, showing that the spectral distribution of the electronic excitations, such as spin fluctuations and current loops, and the strength of their interaction with quasiparticles can account for the high critical temperature of the superconducting phase transition. Finally, we discuss how the use of this technique can be extended to the underdoped region of the phase diagram of cuprates, in which a pseudogap in the quasiparticle density of states opens. The microscopic modeling of the interaction of ultrashort light pulses with unconventional superconductors will be one of the key challenges of the next-years materials science, eventually leading to the full understanding of the role of the electronic correlations in controlling the dynamics on the femtosecond timescale., Comment: 15 pages, 5 figures, Invited manuscript for the proceedings of "Materials & Mechanisms of Superconductivity" (M2S), Washington, 2012

Since their invention scanning tunneling microscopy (STM, (Binnig et al., 1982)) and atomic force microscopy (AFM, (Binnig et al., 1986)) have emerged as powerful and versatile techniques for atomic and nanometer-scale imaging. In this review we will focus on AFM, whose methods have found applications for imaging, metrology and manipulation at the nanometer level of a wide variety of surfaces, including biological ones (Braga & Ricci, 2004; Garcia, 2010; Jandt, 2001; Jena & Horber, 2002; Kopniczky, 2003; Morita et al., 2009; 2002; Yacoot & Koenders, 2008). Today AFM is regarded as an essential tool for nanotechnology and a basic tool for material science in general.

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.

This communication presents and discusses an experimental proof of the correlation among local structure and second harmonic generation (SHG) in bulk nanostructured potassium niobiosilicate (KNS) glasses. In particular, SHG shows a maximum in correspondence of the early stages of nanostructuring, that are characterized by the segregation within the amorphous matrix of nanosized inhomogeneities. EXAFS experiments indicate that these inhomogeneities are determined by the maximum size reached by the niobium second coordination shell combined with the sudden inclusion of potassium atoms in it. Such rearrangement at the local level determines the maximum fluctuation of the bulk glass refractive index and in turn its maximum SHG activity.

In strongly-correlated systems the electronic properties at the Fermi energy (EF) 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 show the interplay between the many-body high-energy CuO2 excitations at 1.5 and 2 eV and the onset of HTSC. This is revealed by a novel optical pump supercontinuum-probe technique, which provides access to the dynamics of the dielectric function in Bi$_2$Sr$_2$Ca$_{0.92}$Y$_{0.08}$Cu$_2$O$_{8+{\delta}}$ 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$_c$)., Comment: Text and Supplementary Information

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.

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.

In this letter we demonstrate the possibility to determine the temporal and spectral structure (spectrogram) of a complex light pulse exploiting the ultrafast switching character of a non-thermal photo-induced phase transition. As a proof, we use a VO2 multi-film, undergoing an ultrafast insulator-to-metal phase transition when excited by femtosecond near-infrared laser pulses. The abrupt variation of the multi-film optical properties, over a broad infrared/visible frequency range, is exploited to determine, in-situ and in a simple way, the spectrogram of a supercontinuum pulse produced by a photonic crystal fiber. The determination of the structure of the pulse is mandatory to develop new pump-probe experiments with frequency resolution over a broad spectral range (700-1100 nm)., Comment: 4 pages, 3 figures, letter

In this work an optical pump‐probe set‐up is used to study the photo‐induced non‐equilibrium dynamics of a superconducting underdoped Bi2212 single crystal in a strong excitation regime (10

Time-and-frequency resolved pump-probe optical spectroscopy is used to investigate the effect of the impulsive injection of delocalized excitations through a charge-transfer process in insulating CuGeO3. A large broadening of the charge-transfer edge is observed on the sub-ps timescale. The modification of this spectral feature can not be attributed to the local increase of the effective temperature, as a consequence of the energy absorbed by the pump pulse. The measured modifications of the optical properties of the system are consistent with the creation of a non-thermal state, metastable on the ps timescale, after the pump-induced impulsive modification of the electron interactions., Comment: 8 pages, 5 figures. Published on Physical Review B.

The thermal dynamics induced by ultrashort laser pulses in nanoscale systems, i.e. all-optical time-resolved nanocalorimetry is theoretically investigated from 300 to 1.5 K. We report ab-initio calculations describing the temperature dependence of the electron-phonon interactions for Cu nanodisks supported on Si. The electrons and phonons temperatures are found to decouple on the ns time scale at 10 K, which is two orders of magnitude in excess with respect to that found for standard low-temperature transport experiments. By accounting for the physics behind our results we suggest an alternative route for overhauling the present knowledge of the electron-phonon decoupling mechanism in nanoscale systems by replacing the mK temperature requirements of conventional experiments with experiments in the time-domain., Comment: 5 pages, 3 figures. Accepted on Physical Review B.

We present a theoretical framework allowing to properly address the nature of surface-like eigenmodes in a hypersonic surface phononic crystal, a composite structure made of periodic metal stripes of nanometer size and periodicity of 1 micron, deposited over a semi-infinite silicon substrate. In surface-based phononic crystals there is no distinction between the eigenmodes of the periodically nanostructured overlayer and the surface acoustic modes of the semi-infinite substrate, the solution of the elastic equation being a pseudo-surface acoustic wave partially localized on the nanostructures and radiating energy into the bulk. This problem is particularly severe in the hypersonic frequency range, where semi-infinite substrate's surface acoustic modes strongly couple to the periodic overlayer, thus preventing any perturbative approach. We solve the problem introducing a surface-likeness coefficient as a tool allowing to find pseudo-surface acoustic waves and to calculate their line shapes. Having accessed the pseudo-surface modes of the composite structure, the same theoretical frame allows reporting on the gap opening in the now well-defined pseudo-SAW frequency spectrum. We show how the filling fraction, mass loading and geometric factors affect both the frequency gap, and how the mechanical energy is scattered out of the surface waveguiding modes., 8 pages, 7 figures, 2 tables. Published on Phys. Rev. B

We present the experimental evidence of the interplay between the variation of the linewidth and effective mass of electrons in image potential states on a Cu(1 1 1) surface induced by a selective alteration of the hot-electron gas density generated by ultra-short laser pulse excitations. (C) 2008 Elsevier B.V. All rights reserved.

The ultrafast thermal and mechanical dynamics of a two-dimensional lattice of metallic nano-disks has been studied by near infrared pump-probe diffraction measurements, over a temporal range spanning from 100 fs to several nanoseconds. The experiments demonstrate that, in these systems, a two-dimensional surface acoustic wave (2DSAW), with a wavevector given by the reciprocal periodicity of the array, can be excited by ~120 fs Ti:sapphire laser pulses. In order to clarify the interaction between the nanodisks and the substrate, numerical calculations of the elastic eigenmodes and simulations of the thermodynamics of the system are developed through finite-element analysis. At this light, we unambiguously show that the observed 2DSAW velocity shift originates from the mechanical interaction between the 2DSAWs and the nano-disks, while the correlated 2DSAW damping is due to the energy radiation into the substrate., 13 pages, 10 figures

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., Comment: 5 pages, 4 figures

The intrinsic linewidth of Ag(100) electronic image-potential states versus the momentum parallel to the surface has been obtained from line-shape analysis of high-resolution angle-resolved two-photon photoemission spectra. For the n = 1 state, the measured intrinsic linewidths have been observed to increase from 14 meV at normal emission (k∥=0) to 70 meV at k∥=0.18 A - 1 . This finding, when compared to the significantly lower inverse lifetime broadening measured on Cu(100), opens the question of the interplay between collective particle effects and nonlocal mechanisms associated with the image-potential electrons decay dynamics. In addition, the effective electron masses for the n = 1 and n=2 states, observed in our experiments along the ΓM and rX directions of the surface Brillouin zone, improve the agreement between the measured values and the theoretical predictions.

A design for photoacoustic mass sensors operating above 100 GHz is proposed. The design is based on impulsive optical excitation of a pseudosurface acoustic wave in a surface phononic crystal with nanometric periodic grating, and on time-resolved extreme ultraviolet detection of the pseudosurface acoustic wave frequency shift upon mass loading the device. The present design opens the path to sensors operating in a frequency range currently unaccessible to electro-acoustical transducers, providing enhanced sensitivity, miniaturization and incorporating time-resolving capability while forgoing the piezoelectric substrate requirement., Comment: 4 pages, 2 figures

The temperature dependence of the thermal boundary resistivity is investigated in glass-embedded Ag particles of radius 4.5 nm, in the temperature range from 300 to 70 K, using all-optical time-resolved nanocalorimetry. The present results provide a benchmark for theories aiming at explaining the thermal boundary resistivity at the interface between metal nanoparticles and their environment, a topic of great relevance when tailoring thermal energy delivery from nanoparticles as for applications in nanomedicine and thermal management at the nanoscale, Comment: 4 pages, 3 figures