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We present developments in the technique of photo-induced near-field electron microscopy. (PINEM) We image the electron interaction with a far-field plane wave reflected from a mirror, and with the near-field resonance of a plasmonic nanowire.

The electronic, optical, and magnetic properties of quantum solids are determined by their low-energy (< 100 meV) many-body excitations. Dynamical characterization and manipulation of such excitations relies on tools that combine nm-spatial, fs-temporal, and meV-spectral resolution. Currently, phonons and collective plasmon resonances can be imaged in nanostructures with sub-nm and 10s meV space/energy resolution using state-of-the-art energy-filtered transmission electron microscopy (TEM), but only under static conditions, while fs-resolved measurements are common but lack spatial or energy resolution. Here, we demonstrate a new method of spectrally resolved photon-induced near-field electron microscopy (SRPINEM) that allows us to obtain nm-fs-resolved maps of nanoparticle plasmons with an energy resolution determined by the laser linewidth (20 meV in this work), and not limited by electron beam and spectrometer energy spreading. This technique can be extended to any optically-accessible low-energy mode, thus pushing TEM to a previously inaccessible spectral domain with an unprecedented combination of space, energy and temporal resolution., 19 pages, 7 figures

The authors became aware of a mistake in the original version of this Article. Specifically, an extra factor γ was incorrectly included in a number of mathematical equations and expressions. As a result of this, a number of changes have been made to both the PDF and the HTML versions of the Article. A full list of these changes is available online.

Magnetic skyrmions are promising candidates as information carriers in logic or storage devices thanks to their robustness, guaranteed by the topological protection, and their nanometric size. Currently, little is known about the influence of parameters such as disorder, defects or external stimuli, on the long-range spatial distribution and temporal evolution of the skyrmion lattice. Here, using a large (7.3x7.3{\mu}m$^{2}$) single crystal nano-slice of Cu$_{2}$OSeO$_{3}$, we image up to 70,000 skyrmions, by means of cryo-Lorentz Transmission Electron Microscopy as a function of the applied magnetic field. The emergence of the skyrmion lattice from the helimagnetic phase is monitored, revealing the existence of a glassy skyrmion phase at the phase transition field, where patches of an octagonally distorted skyrmion lattice are also discovered. In the skyrmion phase, dislocations are shown to cause the emergence and switching between domains with different lattice orientations and the temporal fluctuations of these domains is filmed. These results demonstrate the importance of direct-space and real-time imaging of skyrmion domains for addressing both their long-range topology and stability., Comment: 31 pages (16 + 15 supplementary material),17 figures (4 + 13 supplementary material)

Skyrmions are nanometric spin whirls that can be stabilized in magnets lacking inversion symmetry. The properties of isolated Skyrmions embedded in a ferromagnetic background have been intensively studied. We show that single Skyrmions and clusters of Skyrmions can also form in the helical phase and investigate theoretically their energetics and dynamics. The helical background provides natural one-dimensional channels along which a Skyrmion can move rapidly. In contrast to Skyrmions in ferromagnets, the Skyrmion-Skyrmion interaction has a strong attractive component and thus Skyrmions tend to form clusters with characteristic shapes. These clusters are directly observed in transmission electron microscopy measurements in thin films of Cu_{2}OSeO_{3}. Topological quantization, high mobility, and the confinement of Skyrmions in channels provided by the helical background may be useful for future spintronics devices.

In systems having an anisotropic electronic structure, such as the layered materials graphite, graphene, and cuprates, impulsive light excitation can coherently stimulate specific bosonic modes, with exotic consequences for the emergent electronic properties. Here we show that the population of E_{2g} phonons in the multiband superconductor MgB_{2} can be selectively enhanced by femtosecond laser pulses, leading to a transient control of the number of carriers in the σ-electronic subsystem. The nonequilibrium evolution of the material optical constants is followed in the spectral region sensitive to both the a- and c-axis plasma frequencies and modeled theoretically, revealing the details of the σ-π interband scattering mechanism in MgB_{2}.

Motion of ions and their interplay with bonded charge govern the functionality of materials. The scattering processes that undergo conduction carriers, such as electron-phonon or electron-electron interaction, influence their response to ultrafast stimuli such as time-varying electric fields or light pulses in terms of electrical mobility and bulk mechanics. Graphite and its derived materials, nanotubes, graphene, fullerenes, diamondoids, display a rich variety of electronic and mechanical properties which have found numerous exploitations in modern technology [1], and which are still stimulating intense research for future applications [2].

Extended abstract of a paper presented at Microscopy and Microanalysis 2012 in Phoenix, Arizona, USA, July 29 – August 2, 2012.

The olive fruit fly Bactrocera oleae (Diptera: Tephritidae) is the most devastating pest of cultivated olive (Olea europaea L.). Intraspecific variation in plant resistance to B. oleae has been described only at phenotypic level. In this work, we used a transcriptomic approach to study the molecular response to the olive fruit fly in two olive cultivars with contrasting level of susceptibility. Using next-generation pyrosequencing, we first generated a catalogue of more than 80,000 sequences expressed in drupes from approximately 700k reads. The assembled sequences were used to develop a microarray layout with over 60,000 olive-specific probes. The differential gene expression analysis between infested (i.e. with II or III instar larvae) and control drupes indicated a significant intraspecific variation between the more tolerant and susceptible cultivar. Around 2500 genes were differentially regulated in infested drupes of the tolerant variety. The GO annotation of the differentially expressed genes implies that the inducible resistance to the olive fruit fly involves a number of biological functions, cellular processes and metabolic pathways, including those with a known role in defence, oxidative stress responses, cellular structure, hormone signalling, and primary and secondary metabolism. The difference in the induced transcriptional changes between the cultivars suggests a strong genetic role in the olive inducible defence, which can ultimately lead to the discovery of factors associated with a higher level of tolerance to B. oleae. © 2017 Grasso et al. This is an open access article distributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.

Understanding the dynamics of atomic vibrations confined in quasi-zero dimensional systems is crucial from both a fundamental point-of-view and a technological perspective. Using ultrafast electron diffraction, we monitored the lattice dynamics of GaAs quantum dots—grown by Droplet Epitaxy on AlGaAs—with sub-picosecond and sub-picometer resolutions. An ultrafast laser pulse nearly resonantly excites a confined exciton, which efficiently couples to high-energy acoustic phonons through the deformation potential mechanism. The transient behavior of the measured diffraction pattern reveals the nonequilibrium phonon dynamics both within the dots and in the region surrounding them. The experimental results are interpreted within the theoretical framework of a non-Markovian decoherence, according to which the optical excitation creates a localized polaron within the dot and a travelling phonon wavepacket that leaves the dot at the speed of sound. These findings indicate that integration of a phononic emitter in opto-electronic devices based on quantum dots for controlled communication processes can be fundamentally feasible. © 2017 Author(s).

Background: Lettuce is a leafy vegetable that is extensively commercialized as a ready-to-eat product because of its widespread use in human nutrition as salad. It is well known that washing treatments can severely affect the quality and shelf-life of ready-to-eat vegetables. The study presented here evaluated the effect of two washing procedures on fresh-cut lettuce during storage.; Results: An omics approach was applied to reveal global changes at molecular level induced by peracetic acid washing in comparison with sodium hypochlorite treatment. Microbiological analyses were also performed to quantify total bacterial abundance and composition. The study revealed wide metabolic alterations induced by the two sanitizers. In particular, transcriptomic and proteomic analyses pointed out a number of transcripts and proteins differentially accumulated in response to peracetic acid washing, mainly occurring on the first day of storage. In parallel, different microbiota composition and significant reduction in total bacterial load following washing were also observed.; Conclusion: The results provide useful information for the fresh-cut industry to select an appropriate washing procedure preserving fresh-like attributes as much as possible during storage of the end product. Molecular evidence indicated peracetic acid to be a valid alternative to sodium hypochlorite as sanitizer solution. © 2017 Society of Chemical Industry.; © 2017 Society of Chemical Industry.

Skyrmions are nanometric spin whirls that can be stabilized in magnets lacking inversion symmetry. The properties of isolated Skyrmions embedded in a ferromagnetic background have been intensively studied. We show that single Skyrmions and clusters of Skyrmions can also form in the helical phase and investigate theoretically their energetics and dynamics. The helical background provides natural one-dimensional channels along which a Skyrmion can move rapidly. In contrast to Skyrmions in ferromagnets, the Skyrmion-Skyrmion interaction has a strong attractive component and thus Skyrmions tend to form clusters with characteristic shapes. These clusters are directly observed in transmission electron microscopy measurements in thin films of Cu_{2}OSeO_{3}. Topological quantization, high mobility, and the confinement of Skyrmions in channels provided by the helical background may be useful for future spintronics devices.

Ultrafast electron diffraction is a powerful technique to investigate out-of-equilibrium atomic dynamics in solids with high temporal resolution. When diffraction is performed in reflection geometry, the main limitation is the mismatch in group velocity between the overlapping pump light and the electron probe pulses, which affects the overall temporal resolution of the experiment. A solution already available in the literature involved pulse front tilt of the pump beam at the sample, providing a sub-picosecond time resolution. However, in the reported optical scheme, the tilted pulse is characterized by a temporal chirp of about 1 ps at 1mm away from the centre of the beam, which limits the investigation of surface dynamics in large crystals. In this paper, we propose an optimal tilting scheme designed for a radio-frequency-compressed ultrafast electron diffraction setup working in reflection geometry with 30 keV electron pulses containing up to 10(5) electrons/pulse. To characterize our scheme, we performed optical cross-correlation measurements, obtaining an average temporal width of the tilted pulse lower than 250 fs. The calibration of the electron-laser temporal overlap was obtained by monitoring the spatial profile of the electron beam when interacting with the plasma optically induced at the apex of a copper needle (plasma lensing effect). Finally, we report the first time-resolved results obtained on graphite, where the electron-phonon coupling dynamics is observed, showing an overall temporal resolution in the sub-500 fs regime. The successful implementation of this configuration opens the way to directly probe structural dynamics of low-dimensional systems in the sub-picosecond regime, with pulsed electrons. (C) 2017 Author(s).

In cuprates, a precursor state of superconductivity is speculated to exist above the critical temperature ${\mathrm{T}}_{\mathrm{C}}$. Here we show via a combination of far-infrared ellipsometry and ultrafast broadband optical spectroscopy that signatures of such a state can be obtained via three independent observables in an underdoped sample of ${\mathrm{NdBa}}_{2}{\mathrm{Cu}}_{3}{\mathrm{O}}_{6+\ensuremath{\delta}}$. The pseudogap correlations were disentangled from the response of laser-broken pairs by clocking their characteristic time scales. The onset of a superconducting precursor state was found at a temperature ${\mathrm{T}}_{\mathrm{ONS}}g{\mathrm{T}}_{\mathrm{C}}$, consistent with the temperature scale identified via static optical spectroscopy. Furthermore, the temperature evolution of the coherent vibration of the Ba ion, strongly renormalized by the onset of superconductivity, revealed a pronounced anomaly at the same temperature ${\mathrm{T}}_{\mathrm{ONS}}$. The microscopic nature of such a precursor state is discussed in terms of preformed pairs and enhanced bilayer coherence.

Magnetic skyrmions are localized nanometric spin textures with quantized winding numbers as the topological invariant. Rapidly increasing attention has been paid to the investigations of skyrmions since their experimental discovery in 2009, due both to the fundamental properties and the promising potential in spintronics based applications. However, controlled creation of skyrmions remains a pivotal challenge towards technological applications. Here, we report that skyrmions can be created locally by electric field in the magnetoelectric helimagnet Cu$\mathsf{_2}$OSeO$\mathsf{_3}$. Using Lorentz transmission electron microscopy, we successfully write skyrmions in situ from a helical spin background. Our discovery is highly coveted since it implies that skyrmionics can be integrated into contemporary field effect transistor based electronic technology, where very low energy dissipation can be achieved, and hence realizes a large step forward to its practical applications.

Symmetry breaking across phase transitions often causes changes in selection rules and emergence of optical modes which can be detected via spectroscopic techniques or generated coherently in pump-probe experiments. In second-order or weakly first-order transitions, fluctuations of the ordering field are present above the ordering temperature, giving rise to intriguing precursor phenomena, such as critical opalescence. Here, we demonstrate that in magnetite $({\mathrm{Fe}}_{3}{\mathrm{O}}_{4})$ light excitation couples to the critical fluctuations of the charge order and coherently generates structural modes of the ordered phase above the critical temperature of the Verwey transition. Our findings are obtained by detecting coherent oscillations of the optical constants through ultrafast broadband spectroscopy and analyzing their dependence on temperature. To unveil the coupling between the structural modes and the electronic excitations, at the origin of the Verwey transition, we combine our results from pump-probe experiments with spontaneous Raman scattering data and theoretical calculations of both the phonon dispersion curves and the optical constants. Our methodology represents an effective tool to study the real-time dynamics of critical fluctuations across phase transitions.

Recent advances in ultrafast technology enable both the study and the control of materials properties thanks to the ability to record high temporal resolution movies of their transformations, or the ability to generate new states of matter by selecting ad hoc an excitation to drive the system out of equilibrium. The holy grail of this type of experiments is to combine a high tuneability of the excitation with a wide observation window. For example, this is achieved in multidimensional optical spectroscopy where the response to several excitation energies is monitored in a broad energy range by a large bandwidth optical pulse. In this article, the possibility to combine the chemical sensitivity of intense tuneable X-rays pulses from a free electron laser, with the wide range of observables available in an ultrafast transmission electron microscope is discussed. The requirements for such experiments are quantified via estimates based on state of the art experiments and simulations, and it is proposed that ultrafast electron imaging, diffraction and spectroscopy experiments can be performed in combination with a chemically selective X-ray excitation of materials. (C) 2014 The Authors. Published by Elsevier Ltd. All rights reserved.

We demonstrate that highly ordered two-dimensional crystals of ligand-capped gold nanoparticles display a local photo-mechanical stiffness as high as that of solids such as graphite. In out-of-equilibrium electron diffraction experiments, a strong temperature jump is induced in a thin film with a femtosecond laser pulse. The initial electronic excitation transfers energy to the underlying structural degrees of freedom, with a rate generally proportional to the stiffness of the material. Using femtosecond small-angle electron diffraction, we observe the temporal evolution of the diffraction feature associated with the nearest-neighbor nanoparticle distance. The Debye-Waller decay for the octanethiol-capped nanoparticle supracrystal, in particular, is found to be unexpectedly fast, almost as fast as the stiffest solid known and observed by the same technique, i.e., graphite. Our observations unravel that local stiffness in a dense supramolecular assembly can be created by van der Waals interactions up to a level comparable to crystalline systems characterized by covalent bonding. (C) 2019 Author(s).

Polaron transport, in which electron motion is strongly coupled to the underlying lattice deformation or phonons, is crucial for understanding electrical and optical conductivities in many solids. However, little is known experimentally about the dynamics of individual phonon modes during polaron motion. It remains elusive whether polarons have a key role in materials with strong electronic correlations. Here we report the use of a new experimental technique, ultrafast MeV-electron diffraction, to quantify the dynamics of both electronic and atomic motions in the correlated LaSr2Mn2O7. Using photoexcitation to set the electronic system in motion, we find that Jahn-Teller-like O, Mn4+ and La/Sr displacements dominate the lattice response and exhibit a dichotomy in behaviour—overshoot-and-recovery for one sublattice versus normal behaviour for the other. This dichotomy, attributed to slow electronic relaxation, proves that polaron transport is a key process in doped manganites. Our technique promises to be applicable for specifying the nature of electron–phonon coupling in complex materials. Ultrafast interactions between electrons and the lattice of correlated materials can now be accessed with a new electron diffraction method. Knowing how electrons interact with the lattice as they travel through a material is crucial for understanding properties such as electrical conductivity. A team led by Yimei Zhu at Brookhaven National Laboratory showed that ultrahigh-energy electron diffraction can be used to quantitatively follow changes in the crystal structure and electronic system of a layered manganite on picosecond timescales, unveiling strong evidence for the formation of polarons — a quasiparticle that arises from strong electron-lattice interactions. This technique reveals the important role of electron-lattice interactions in doped magnanites, and could be used to study such interactions in a range of correlated materials.

Capturing and controlling plasmons at buried interfaces with nanometre and femtosecond resolution has yet to be achieved and is critical for next generation plasmonic devices. Here we use light to excite plasmonic interference patterns at a buried metal–dielectric interface in a nanostructured thin film. Plasmons are launched from a photoexcited array of nanocavities and their propagation is followed via photon-induced near-field electron microscopy (PINEM). The resulting movie directly captures the plasmon dynamics, allowing quantification of their group velocity at ∼0.3 times the speed of light, consistent with our theoretical predictions. Furthermore, we show that the light polarization and nanocavity design can be tailored to shape transient plasmonic gratings at the nanoscale. This work, demonstrating dynamical imaging with PINEM, paves the way for the femtosecond and nanometre visualization and control of plasmonic fields in advanced heterostructures based on novel two-dimensional materials such as graphene, MoS2, and ultrathin metal films., Visualizing surface plasmon polaritons at buried interfaces has remained elusive. Here, the authors develop a methodology to study the spatiotemporal evolution of buried near-fields within complex heterostructures, enabling the characterization of the next generation of plasmonic devices.

Recently, the switching between the different charge-ordered phases of $1T\ensuremath{-}{\mathrm{TaS}}_{2}$ has been probed by ultrafast techniques, revealing unexpected phenomena such as ``hidden'' metastable states and peculiar photoexcited charge patterns. Here, we apply broadband pump-probe spectroscopy with varying excitation energy to study the ultrafast optical properties of $1T\ensuremath{-}{\mathrm{TaS}}_{2}$ in the visible regime. By scanning the excitation energy in the near-IR region we unravel the coupling between different charge excitations and the low-lying charge-density wave state. We find that the amplitude mode of the charge-density wave exhibits strong coupling to a long-lived doublon state that is photoinduced in the center of the star-shaped charge-ordered Ta clusters by the near-IR optical excitation.

We use ultrafast small-angle electron diffraction combined with angular cross-correlation analysis to characterize the static local order and the dynamics of a glassy dodecanethiol-capped gold nanoparticles supracrystal with fs time-resolution and sensitivity to the light elements in the ligands.

An electron beam traversing a structured plasmonic field is shown to undergo diffraction with characteristic angular patterns of both elastic and inelastic outgoing electron components. In particular, a plasmonic {\it grating} (e.g., a standing wave formed by two counter-propagating plasmons in a thin film) produces diffraction orders of the same parity as the net number of exchanged plasmons. Large diffracted beam fractions are predicted to occur for realistic plasmon intensities in attainable geometries due to a combination of phase and amplitude changes locally imprinted on the passing electron wave. Our study opens new vistas in the study of multiphoton exchanges between electron beams and evanescent optical fields with unexplored effects related to the transversal component of the electron wave function., Comment: 10 pages, 6 figures

In order to sense and respond to the fluctuating light conditions, higher plants possess several families of photoreceptors, such as phytochromes (PHYs), cryptochromes (CRYs) and phototropins. CRYs are responsible for photomorphogenesis and play a role in circadian, developmental and adaptive growth regulation of plants. In tomato (Solanum lycopersicum), CRY2 controls vegetative development, flowering time, fruit antioxidant content as well as the diurnal transcription of several other photoreceptor genes. We applied large-scale molecular approaches to identify altered transcripts and proteins in tomato wild-type (WT) versus a CRY2 overexpressing transgenic genotype, under a diurnal rhythm. Our results showed that tomato CRY2 profoundly affects both gene and protein expression in response to daily light cycle. Particularly altered molecular pathways are related to biotic/abiotic stress, photosynthesis, including components of the light and dark reactions and of starch and sucrose biosynthesis, as well as to secondary metabolism, such as phenylpropanoid, phenolic and flavonoid/anthocyanin biosynthesis pathways. One of the most interesting results is the coordinated up-regulation, in the transgenic genotype, of a consistent number of transcripts and proteins involved in photorespiration and photosynthesis. It is conceivable that light modulates the energetic metabolism of tomato through a fine CRY2-mediated transcriptional control.

Microscopic investigations were conducted into the interaction of Colletotrichum acutatum on white and red strawberry (Fragaria ×ananassa) fruit surfaces. The results showed that, whilst the early interaction events were similar in both white and red fruits, after 24 h fungal colonization dramatically varied: in white fruits C. acutatum became quiescent as melanized appressoria, but on red fruits it displayed subcuticular necrotrophic invasion. A microarray analysis of white and red strawberries after 24 h of interaction with C. acutatum was performed, in order to reveal differences in gene expression possibly related to the different susceptibility of unripe and ripe fruits. Epi/catechin-related genes and fatty acid metabolism genes, involved in the production of quiescence-related molecules such as flavan-3-ols, proanthocyanidins and antifungal dienes, were found to be regulated during strawberry ripening, supporting a role for these molecules as preformed defence mechanisms. Besides several genes commonly regulated upon pathogen interaction, different genes were specifically transcribed only in white or red challenged fruits; a number of these, such as those coding for lectin and polyphenol oxidase, possibly account for specific pathogen-induced responses. The putative biological role of these genes in the different susceptibility of fruits to C. acutatum is discussed.

Beyond their participation in fruit pigmentation and because of their high antioxidant activity, flavonoids are considered important constituents of fruits and vegetables. We have previously reported that in the ripe receptacles of Fragaria chiloensis only traces of flavonoids can be found, while cinnamic acid derivatives are highly accumulated. In order to characterize the molecular background of this uncommon phenotype we analyzed the transcriptional profile of different biosynthetic genes, with special regard to the gene encoding Cinnamate 4-Hydroxylase (C4H), the enzyme transforming cinnamic acid into the next intermediary of the phenylpropanoid pathway. Northern blot and quantitative RT-PCR showed low transcript abundance for the gene encoding C4H and also for a series of structural genes responsible for flavonoid biosynthesis. Together with this, high transcript levels were found for a repressive transcription factor, suggesting that the pathway would be inhibited at the transcriptional level, thus correlating to our previous findings on the chemical phenotype. Our results contribute to the comprehension of the pigmentation phenotype in strawberries, allowing the utilization of Fragaria chiloensis as a model system for the study of antioxidant pigment biosynthesis.

Electron energy loss spectroscopy (EELS) is a powerful tool in the study of valency, bonding and structure of solids. Previously, EEL spectra were either time-integrated or at best time-resolved on the millisecond to seconds scale, being limited by video rates and detector responses. Here, using our 4D electron microscope, we report ultrafast EELS, taking the time resolution in the energy–time space into the femtosecond regime, a 10 order of magnitude increase, and for a table-top apparatus. It is shown that the energy–time–amplitude space of graphite is selective to changes, especially in the electron density of the π + σ plasmon of the collective oscillation of the four electrons of carbon.

A comparative experimental study is presented of the electronic properties of MnSi films grown on Si(111) and of MnSi single crystals, using X-ray absorption spectroscopy (XAS), and core level and valence band photoemission spectroscopy (PES). No significant differences in the electronic structure of the two systems can be found. Absorption measurements on the Mn 2p threshold show a mixed valence ground state, where the multiplet structure is washed out by the hybridisation of the Mn 3d states with the Si sp states. These results are also confirmed by photoemission (PE) spectra from the valence band and the Mn 3s, 3p and 2p core levels. Strong attention has been paid to the effect of contamination. The occurrence of multiplet effects in the absorption spectra indicates unambiguously the localisation of the Mn 3d electrons in Mn-O bonds, which strongly influences the electronic properties of these systems. (C) 2007 Elsevier B.V. All rights reserved.

The biosynthesis of flavonoids and proanthocyanidins was studied in cultivated strawberry (Fragaria x ananassa) by combining biochemical and molecular approaches. Chemical analyses showed that ripe strawberries accumulate high amounts of pelargonidin-derived anthocyanins, and a larger pool of 3',4'-hydroxylated proanthocyanidins. Activities and properties of major recombinant enzymes were demonstrated by means of in vitro assays, with special emphasis on specificity for the biologically relevant 4'- and 3',4'-hydroxylated compounds. Only leucoanthocyanidin reductase showed a strict specificity for the 3',4'-hydroxylated leucocyanidin, while other enzymes accepted either hydroxylated substrate with different relative activity rates. The structure of late flavonoid pathway genes, leading to the synthesis of major compounds in ripe fruits, was elucidated. Complex developmental and spatial expression patterns were shown for phenylpropanoid and flavonoid genes in fruits throughout ripening as well as in leaves, petals and roots. Presented results elucidate key steps in the biosynthesis of strawberry flavonoid end products. (c) 2007 Elsevier Inc. All rights reserved.

Tailoring the properties of correlated oxides is accomplished by chemical doping, pressure, temperature, or magnetic field. Photoexcitation is a valid alternative to reach out-of-equilibrium states otherwise inaccessible. Here, we quantitatively estimate the coupling between a lattice distortion and the charge-transfer excitation in La2CuO4+delta. We photoinduce a coherent La ion vibration and monitor the response of the optical constants in a broad energy range, providing quantitative information on the electron-phonon matrix element that can be compared to theoretical models. We propose the same methodology to probe electron-phonon and electron-electron interactions in other materials.

The investigation of the static and dynamic structural properties of colloidal systems relies on techniques capable of atomic resolution in real space and femtosecond resolution in time. Recently, the cross-correlation function (CCF) analysis of both X-rays and electron diffraction patterns from dilute and dense aggregates has demonstrated the ability to retrieve information on the sample's local order and symmetry. Open questions remain regarding the role of the beam coherence in the formation of the diffraction pattern and the properties of the CCF, especially in dense systems. Here, we simulate the diffraction patterns of dense two-dimensional monodisperse systems of different symmetries, varying the transverse coherence of the probing wave, and analyze their CCF. We study samples with different symmetries at different size scale, as for example, pentamers arranged into a four-fold lattice where each pentamer is surrounded by triangular lattices, both ordered and disordered. In such systems, different symmetry modulations are arising in the CCF at specific scattering vectors. We demonstrate that the amplitude of the CCF is a fingerprint of the degree of the ordering in the sample and that at partial transverse coherence, the CCF of a dense sample corresponds to that of an individual scattering object., Comment: 22 pages, 7 figures

Molecular and biochemical studies were undertaken to elucidate gene/product relationships which influence key fruit quality traits in cultivated strawberry (Fragaria × ananassa Duch.). Comparative transcription profiling experiments in selected genotypes pointed out a number of differentially-expressed genes, possibly related to important fruit quality traits as aroma and fruit firmness. Some of the altered cDNAs encode putative cinnamyl alcohol dehydrogenase, cinnamoyl CoA reductase, cellulase and expansin genes, involved in the early steps of lignin biosynthesis and in cell wall structure, respectively. Parallel biochemical analyses studied the spectra of volatile compounds by Proton Transfer Reaction-Mass Spectrometry (PTR-MS) and alcohol acyl transferase (AAT) specific activity in red fruits. A correlation between the expression of an aat gene, total AAT activity and the presence of related esters in fruit headspace was found.

We present novel infrared optical conductivity data on the three layer high Tc superconductor Bi2Sr2Ca2Cu3O10 at optimal doping. We extend the analysis of an earlier publication, providing a universal scaling function sigma(omega,T)=g(omega/T)/T for the optical conductivity. In the present manuscript we obtain a good scaling collapse of the experimental curves on the g(omega/T) over a wide range of values of omega/T (at least in range 0 to 10), if we assume that g(omega/T) is superimposed on a non-universal background which is temperature independent. We obtain the same result, if in our analysis we allow this background to have a T-squared temperature dependent correction. The most striking property of g(omega/T) is, that it corresponds to a scattering rate which varies linearly as a function of temperature, but which is independent of the frequency., 17 pages, 10 figures, elsart

Recently, transcription profiling of ripening tomatoes has provided some information about genes involved in fruit maturation and ripening. Nevertheless, many fundamental molecular mechanisms need to be better investigated. Besides, despite their deep impact on fruit development, very little is known about the regulation of photosensory and light signalling genes during fruit ripening. Using the Tom1 microarray, we have compared the extent of transcriptional changes in three different stages of fruit development (immature green, breaker, and fully ripe) versus leaf in the cultivar Money Maker. The extent of transcriptional modulation was confirmed through quantitative real time RT-PCR on selected genes, showing significant levels of regulation during fruit development. Furthermore, real-time RT-PCR was used to study the regulation of transcripts encoding photosensory receptors, light signalling proteins, and carotenoid biosynthesis genes. Some of these transcripts are highly regulated during tomato fruit development, suggesting that light responsiveness of carotenoid biosynthesis tomato fruits could be at least partially regulated at the transcriptional level.

Ultrashort pulses of X-rays from a free-electron laser capture the spatiotemporal evolution of spins in the different crystallographic directions of a complex magnetic material.

We present a fiber transmission system combining dispersion management with periodical hopping of channel frequencies by means of wavelength converters. We show that the signal distortion arising from chirp reversal may be substantially suppressed for optimized dispersion-managed links. We exemplify some potentialities of all-optical frequency conversion to limit the third-order dispersion impairments and timing jitter in long-haul fiber systems based on chirped RZ modulation format.

The propagation of ultrashort laser pulses into a microstructured fiber having a large nonlinear coefficient is found to give rise to various nonlinear phenomena. By using an input wavelength in the range 1300–1550 nm, the observed output spectrum presents, besides supercontinuum generation, sharp lines due to third-harmonic generation and four-wave mixing. When the input wavelength is around 800 nm, close to the zero-dispersion wavelength, the solitonic propagation is accompanied by a very intense and narrow-band emission in the blue spectral region.

We present a non-comprehensive review of some representative experimental studies in crystalline condensed matter systems where the effects of intense ultrashort light pulses are probed using x-ray diffraction and photoelectron spectroscopy. On an ultrafast (sub-picosecond) time scale, conventional concepts derived from the assumption of thermodynamic equilibrium must often be modified in order to adequately describe the time-dependent changes in material properties. There are several commonly adopted approaches to this modification, appropriate in different experimental circumstances. One approach is to treat the material as a collection of quasi-thermal subsystems in thermal contact with each other in the so-called “N-temperature” models. On the other extreme, one can also treat the time-dependent changes as fully coherent dynamics of a sometimes complex network of excitations. Here, we present examples of experiments that fall into each of these categories, as well as experiments that partake of both models. We conclude with a discussion of the limitations and future potential of these concepts. I. INTRODUCTION, Structural Dynamics, 4 (6), ISSN:2329-7778

Surface plasmon polaritons can confine electromagnetic fields in subwavelength spaces and are of interest for photonics, optical data storage devices and biosensing applications. In analogy to photons, they exhibit wave–particle duality, whose different aspects have recently been observed in separate tailored experiments. Here we demonstrate the ability of ultrafast transmission electron microscopy to simultaneously image both the spatial interference and the quantization of such confined plasmonic fields. Our experiments are accomplished by spatiotemporally overlapping electron and light pulses on a single nanowire suspended on a graphene film. The resulting energy exchange between single electrons and the quanta of the photoinduced near-field is imaged synchronously with its spatial interference pattern. This methodology enables the control and visualization of plasmonic fields at the nanoscale, providing a promising tool for understanding the fundamental properties of confined electromagnetic fields and the development of advanced photonic circuits., Mapping the field of surface plasmon polaritons is important to understand their fundamental properties and behaviour. Here, the authors show that ultrafast transmission electron microscopy can simultaneously obtain the spatial interference and quantization of nanowire-confined plasmonic fields.

Imaging of flux vortices in high quality MgB$_2$ single crystals has been successfully performed in a commercial Field Emission Gun-based Transmission Electron Microscope. In Cryo-Lorentz Microscopy, the sample quality and the vortex lattice can be monitored simultaneously, allowing one to relate microscopically the surface quality and the vortex dynamics. Such a vortex motion ultimately determines the flow resistivity, $\rho_{f}$, the knowledge of which is indispensable for practical applications such as superconducting magnets or wires for Magnetic Resonance Imaging. The observed patterns have been analyzed and compared with other studies by Cryo-Lorentz Microscopy or Bitter decoration. We find that the vortex lattice arrangement depends strongly on the surface quality obtained during the specimen preparation, and tends to form an hexagonal Abrikosov lattice at a relatively low magnetic field. Stripes or gossamer-like patterns, recently suggested as potential signatures of an unconventional behavior of MgB$_2$, were not observed.

Ultrafast Electron Diffraction (UED) has been widely used to investigate the structural dynamics of molecules and materials. Femtosecond (fs) electron bunches are used to obtain diffraction images of a specimen upon photo-excitation by a temporally delayed light pulse. The high cross-section of electrons makes it a very flexible tool for the study of light elements, monolayers and surfaces; at the same time, electrons can travel down to few nanometers (nm) and structural information from the bulk can also be retrieved. In this article, we discuss the design and implementation of a flexible beamline for fs electron diffraction experiments in transmission or reflection geometry. By the use of a radiofrequency (RF) compression cavity synchronized to our laser system, in combination with a set of electron optics, we demonstrate that we can control the beam properties in terms of charge per pulse, transverse spot-size on the sample and temporal duration of the bunches. The characterization of the beam is performed via a light-electrons cross-correlation experiment and we demonstrate an overall temporal resolution around 300 fs for bunches containing up to 10(5) electrons at a repetition rate of 20 kHz. (c) 2012 Elsevier B.V. All rights reserved.

The strength of the electron-phonon coupling parameter and its evolution throughout a solid's phase diagram often determines phenomena such as superconductivity, charge- and spin-density waves. Its experimental determination relies on the ability to distinguish thermally activated phonons from those emitted by conduction band electrons, which can be achieved in an elegant way by ultrafast techniques. Separating the electronic from the out-of-equilibrium lattice subsystems, we probed their reequilibration by monitoring the transient lattice temperature through femtosecond x-ray diffraction in La2-xSrxCuO4 single crystals with x = 0.1 and 0.21. The temperature dependence of the electron-phonon coupling is obtained experimentally and shows similar trends to what is expected from the ab initio calculated shape of the electronic density of states near the Fermi energy. This study evidences the important role of band effects in the electron-lattice interaction in solids, in particular, in superconductors.

In this paper, the design and implementation of a femtosecond-resolved ultrafast transmission electron microscope is presented, based on a thermionic gun geometry. Utilizing an additional magnetic lens between the electron acceleration and the nominal condenser lens system, a larger percentage of the electrons created at the cathode are delivered to the specimen without degrading temporal, spatial and energy resolution significantly, while at the same time maintaining the femtosecond temporal resolution. Using the photon-induced near field electron microscopy effect (PINEM) on silver nanowires the cross-correlation between the light and electron pulses was measured, showing the impact of the gun settings and initiating laser pulse duration on the electron bunch properties. Tuneable electron pulses between 300 fs and several ps can be obtained, and an overall energy resolution around 1 eV was achieved. (C) 2013 Elsevier B.V. All rights reserved.

A femtosecond pump-probe setup is described that is optimised for broadband transient reflectivity experiments on solid samples over a wide range of temperatures. By combining a temporal resolution of 45 fs and a broad detection range between 1.75 and 2.85 eV, this apparatus can provide insightful information on the interplay between coherent collective modes and high-energy electronic excitations, which is one of the distinctive characteristics of strongly interacting and correlated quantum systems. The use of a single-shot readout CMOS array detector at frame rates up to 10 kHz allows to resolve coherent oscillations with amplitudes below 10$^{-4}$ in $\Delta$R/R. We demonstrate the operation of this setup on the prototypical charge-transfer insulator La$_2$CuO$_4$, revealing the presence of coherent optical phonons with frequencies as high as 13 THz., Comment: 16 pages, 4 figures

We examine planar double split-ring resonators (SRRs) consisting of two concentric rings with either opposite, similar, or asymmetric gap orientation. Depending on the geometry we observe resonance hybridization, metamaterial induced transparency, or the excitation of dark resonances. These properties can be used for SRR based sensing applications, to realize strongly dispersive behavior, or for determining the optical properties of metals. We further find that THz SRRs featuring very narrow gaps on the micro- or nanoscale can provide in-gap enhancement factors of several 10,000, a property particularly useful for the realization of nonlinear THz experiments.

In order to sense and respond to the fluctuating light conditions, higher plants possess several families of photoreceptors, such as phytochromes (PHYs), cryptochromes (CRYs) and phototropins. CRYs are responsible for photomorphogenesis and play a role in circadian, developmental and adaptive growth regulation of plants. In tomato (Solanum lycopersicum), CRY2 controls vegetative development, flowering time, fruit antioxidant content as well as the diurnal transcription of several other photoreceptor genes. We applied large-scale molecular approaches to identify altered transcripts and proteins in tomato wild-type (WT) versus a CRY2 overexpressing transgenic genotype, under a diurnal rhythm. Our results showed that tomato CRY2 profoundly affects both gene and protein expression in response to daily light cycle. Particularly altered molecular pathways are related to biotic/abiotic stress, photosynthesis, including components of the light and dark reactions and of starch and sucrose biosynthesis, as well as to secondary metabolism, such as phenylpropanoid, phenolic and flavonoid/anthocyanin biosynthesis pathways. One of the most interesting results is the coordinated up-regulation, in the transgenic genotype, of a consistent number of transcripts and proteins involved in photorespiration and photosynthesis. It is conceivable that light modulates the energetic metabolism of tomato through a fine CRY2-mediated transcriptional control.