Search

When live imaging is not feasible, sample fixation allows preserving the ultrastructure of biological samples for subsequent microscopy analysis. This process could be performed with various methods, each one affecting differently the biological structure of the sample. While these alterations were well-characterized using traditional microscopy, little information is available about the effects of the fixatives on the spatial molecular orientation of the biological tissue. We tackled this issue by employing Rotating-Polarization Coherent Anti-Stokes Raman Scattering (RP-CARS) microscopy to study the effects of different fixatives on the myelin sub-micrometric molecular order and micrometric morphology. RP-CARS is a novel technique derived from CARS microscopy that allows probing spatial orientation of molecular bonds while maintaining the intrinsic chemical selectivity of CARS microscopy. By characterizing the effects of the fixation procedures, the present work represents a useful guide for the choice of the best fixation technique(s), in particular for polarisation-resolved CARS microscopy. Finally, we show that the combination of paraformaldehyde and glutaraldehyde can be effectively employed as a fixative for RP-CARS microscopy, as long as the effects on the molecular spatial distribution, here characterized, are taken into account., Comment: 11 pages, 4 figures. This is the peer reviewed version of an article that has been published in final form by Applied Optics. Please note that the copyright statement on the front page of the article allows posting of this manuscript by authors on arXiv, as specified here: https://www.osapublishing.org/submit/review/copyright_permissions.cfm

Krabbe disease (KD) is a rare demyelinating sphingolipidosis, often fatal in the first years of life. It is caused by the inactivation of the galactocerebrosidase (GALC) enzyme that causes an increase in the cellular levels of psychosine considered to be at the origin of the tissue-level effects. GALC is inactivated also in the Twitcher (TWI) mouse: a genetic model of KD that is providing important insights into the understating of the pathogenetic process and the development of possible treatments. In this article an innovative optical technique, RP-CARS, is proposed as a tool to study the degree of order of the CH2 bonds inside the myelin sheaths of TWI-mice sciatic-nerve fibres. RP-CARS, a recently developed variation of CARS microscopy, is able to combine the intrinsic chemical selectivity of CARS microscopy with molecular-bond-spatial-orientation sensibility. This is the first time RP-CARS is applied to the study of a genetic model of a pathology, leading to the demonstration of a post-onset progressive spatial disorganization of the myelin CH2 bonds. The presented result could be of great interest for a deeper understanding of the pathogenic mechanisms underlying the human KD and, moreover, it is an additional proof of the experimental validity of this microscopy technique., Comment: 19 pages, 7 figures. This is the pre-peer reviewed version of an article that has been published in final form on Journal of Biophotonics

We investigate nanoscale local anodic oxidation (LAO) on hydrogen-intercalated graphene grown by controlled sublimation of silicon carbide (SiC). Scanning probe microscopy (SPM) was used as a lithographic and characterization tool in order to investigate the local properties of the nanofabricated structures. The anomalous thickness observed after the graphene oxidation process is linked to the impact of LAO on the substrate. Micro-Raman spectroscopy was employed to demonstrate the presence of two oxidation regimes depending on the applied bias. We show that partial and total etching of monolayer graphene can be achieved by tuning the bias voltage during LAO. Finally, a complete compositional characterization was achieved by scanning electron microscopy and energy dispersive spectroscopy (EDS)., Comment: 6 pages, 4 figures

We develop a computational framework to examine the factors responsible for scattering-induced distortions of coherent anti-Stokes Raman scattering (CARS) signals in turbid samples. We apply the Huygens-Fresnel Wave-based Electric Field Superposition (HF-WEFS) method combined with the radiating dipole approximation to compute the effects of scattering-induced distortions of focal excitation fields on the far-field CARS signal. We analyze the effect of spherical scatterers, placed in the vicinity of the focal volume, on the CARS signal emitted by different objects (2{\mu}m diameter solid sphere, 2{\mu}m diameter myelin cylinder and 2{\mu}m diameter myelin tube). We find that distortions in the CARS signals arise not only from attenuation of the focal field but also from scattering-induced changes in the spatial phase that modifies the angular distribution of the CARS emission. Our simulations further show that CARS signal attenuation can be minimized by using a high numerical aperture condenser. Moreover, unlike the CARS intensity image, CARS images formed by taking the ratio of CARS signals obtained using x- and y-polarized input fields is relatively insensitive to the effects of spherical scatterers. Our computational framework provide a mechanistic approach to characterizing scattering-induced distortions in coherent imaging of turbid media and may inspire bottom-up approaches for adaptive optical methods for image correction., Comment: 15 pages, 7 figures

By exhibiting a measurable bandgap and exotic valley physics, atomically-thick tungsten disulfide (WS2) offers exciting prospects for optoelectronic applications. The synthesis of continuous WS2 films on other two-dimensional (2D) materials would greatly facilitate the implementation of novel all-2D photoactive devices. In this work we demonstrate the scalable growth of WS2 on graphene and hexagonal boron nitride (h-BN) via a chemical vapor deposition (CVD) approach. Spectroscopic and microscopic analysis reveal that the film is bilayer-thick, with local monolayer inclusions. Photoluminescence measurements show a remarkable conservation of polarization at room temperature peaking 74% for the entire WS2 film. Furthermore, we present a scalable bottom-up approach for the design of photoconductive and photoemitting patterns., Comment: 17 pages, 3 Figures in the main text, supplementary information included

Recently, hexagonal boron nitride (h-BN) has been shown to act as an ideal substrate to graphene by greatly improving the material transport properties thanks to its atomically flat surface, low interlayer electronic coupling and almost perfect reticular matching. Chemical vapour deposition (CVD) is presently considered the most scalable approach to grow graphene directly on h-BN. However, for the catalyst-free approach, poor control over the shape and crystallinity of the graphene grains and low growth rates are typically reported. In this work we investigate the crystallinity of differently shaped grains and identify a path towards a real van der Waals epitaxy of graphene on h-BN by adopting a catalyst-free CVD process. We demonstrate the polycrystalline nature of circular-shaped pads and attribute the stemming of different oriented grains to airborne contamination of the h-BN flakes. We show that single-crystal grains with six-fold symmetry can be obtained by adopting high hydrogen partial pressures during growth. Notably, growth rates as high as 100 nm/min are obtained by optimizing growth temperature and pressure. The possibility of synthesizing single-crystal graphene on h-BN with appreciable growth rates by adopting a simple CVD approach is a step towards an increased accessibility of this promising van der Waals heterostructure., Comment: 13 pages, 4 figures

We present a simple method and its experimental implementation to completely determine the characteristics of the pump-and-probe pulse and the Stokes pulse in a coherent anti-Stokes Raman scattering microscope at sample level without additional autocorrelators. Our approach exploits the delay line, ubiquitous in such microscopes, to perform a convolution of the pump-and-probe and Stokes pulses as a function of their relative delay and it is based on the detection of the photons emitted from an appropriate non-linear sample. The analysis of the non-resonant four-wave-mixing and sum-frequency-generation signals allows retrieving the pulse duration on the sample and the chirp of each pulse. This knowledge is crucial in maximizing the spectral-resolution and contrast in CARS imaging.

Water is believed to be harmful for the stability of phosphorene.On the contrary, the presence of small amount of water allows the synthesis of high-quality material in liquid exfoliation of black phosphorus using dimethylsulfoxide as solvent. A phosphorus/water molar ratio between 1.5 and 14 maximizes the quality of the phosphorene flakes and their stability.

In this work we present a simple pathway to obtain large single-crystal graphene on copper (Cu) foils with high growth rates using a commercially available cold-wall chemical vapour deposition (CVD) reactor. We show that graphene nucleation density is drastically reduced and crystal growth is accelerated when: i) using ex-situ oxidised foils; ii) performing annealing in an inert atmosphere prior to growth; iii) enclosing the foils to lower the precursor impingement flux during growth. Growth rates as high as 14.7 and 17.5 micrometers per minute are obtained on flat and folded foils, respectively. Thus, single-crystal grains with lateral size of about one millimetre can be obtained in just one hour. The samples are characterised by optical microscopy, scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), Raman spectroscopy as well as selected area electron diffraction (SAED) and low-energy electron diffraction (LEED), which confirm the high quality and homogeneity of the films. The development of a process for the quick production of large grain graphene in a commonly used commercial CVD reactor is a significant step towards an increased accessibility to millimetre-sized graphene crystals., Comment: Article: 7 pages, 6 figures. Supplementary Information: 5 pages, 7 figures

The transport properties of epitaxial graphene on SiC(0001) at quantizing magnetic fields are investigated. Devices patterned perpendicularly to SiC terraces clearly exhibit bilayer inclusions distributed along the substrate step edges. We show that the transport properties in the quantum Hall regime are heavily affected by the presence of bilayer inclusions, and observe a significant departure from the conventional quantum Hall characteristics. A quantitative model involving enhanced inter-channel scattering mediated by the presence of bilayer inclusions is presented that successfully explains the observed symmetry properties.

We demonstrate a novel nanoheating scheme that yields very large and uniform temperature gradients up to about 1K every 100nm, in an architecture which is compatible with the field-effect control of the nanostructure under test. The temperature gradients demonstrated largely exceed those typically obtainable with standard resistive heaters fabricated on top of the oxide layer. The nanoheating platform is demonstrated in the specific case of a short-nanowire device., Comment: 6 pages, 6 figures

The ability of atomic hydrogen to chemisorb on graphene makes the latter a promising material for hydrogen storage. Based on scanning tunneling microscopy techniques, we report on site-selective adsorption of atomic hydrogen on convexly curved regions of monolayer graphene grown on SiC(0001). This system exhibits an intrinsic curvature owing to the interaction with the substrate. We show that at low coverage hydrogen is found on convex areas of the graphene lattice. No hydrogen is detected on concave regions. These findings are in agreement with theoretical models which suggest that both binding energy and adsorption barrier can be tuned by controlling the local curvature of the graphene lattice. This curvature-dependence combined with the known graphene flexibility may be exploited for storage and controlled release of hydrogen at room temperature making it a valuable candidate for the implementation of hydrogen-storage devices.

On the SiC(0001) surface (the silicon face of SiC), epitaxial graphene is obtained by sublimation of Si from the substrate. The graphene film is separated from the bulk by a carbon-rich interface layer (hereafter called the buffer layer) which in part covalently binds to the substrate. Its structural and electronic properties are currently under debate. In the present work we report scanning tunneling microscopy (STM) studies of the buffer layer and of quasi-free-standing monolayer graphene (QFMLG) that is obtained by decoupling the buffer layer from the SiC(0001) substrate by means of hydrogen intercalation. Atomic resolution STM images of the buffer layer reveal that, within the periodic structural corrugation of this interfacial layer, the arrangement of atoms is topologically identical to that of graphene. After hydrogen intercalation, we show that the resulting QFMLG is relieved from the periodic corrugation and presents no detectable defect sites.

We present a planar laser diode based on a simple fabrication scheme compatible with virtually any geometry accessible by standard semiconductor lithography technique. We show that our lasers exhibit ~1 GHz -3dB-modulation-bandwidth already in this prototypical implementation. Directions for a significant speed increase are discussed.

We demonstrate anti-bunched emission from a lateral-light emitting diode. Sub-Poissonian emission statistic, with a g$^{(2)}$(0)=0.7, is achieved at cryogenic temperature in the pulsed low-current regime, by exploiting electron injection through shallow impurities located in the diode depletion region. Thanks to its simple fabrication scheme and to its modulation bandwidth in the GHz range, we believe our devices are an appealing substitute for highly-attenuated lasers in existing quantum-key-distribution systems. Our devices outperform strongly-attenuated lasers in terms of multi-photon emission events and can therefore lead to a significant security improvement in existing quantum key distribution systems.

We report on suspended single-layer graphene deposition by a transfer-printing approach based on polydimethylsiloxane stamps. The transfer printing method allows the exfoliation of graphite flakes from a bulk graphite sample and their residue-free deposition on a silicon dioxide substrate. This deposition system creates a blistered graphene surface due to strain induced by the transfer process itself. Single-layer-graphene deposition and its "blistering" on the substrate are demonstrated by a combination of Raman spectroscopy, scanning electron microscopy and atomic-force microscopy measurements. Finally, we demonstrate that blister-like suspended graphene are self-supporting single-layer structures and can be flattened by employing a spatially-resolved direct-lithography technique based on electron-beam induced etching., Comment: 17 pages, 5 figures

A surface-acoustic-wave (SAW) driven light-emitting-diode structure that can implement a single-photon-source for quantum-cryptography applications is demonstrated. Our lateral n-i-p junction is realized starting from an undoped GaAs/AlGaAs quantum well by gating. It incorporates interdigitated transducers for SAW generation and lateral gates for current control. We demonstrate acoustoelectric transport and SAW-driven electroluminescence. The acoustoelectric current can be controlled down to complete pinch-off by means of the lateral gates.

We present an unconventional approach to realize acoustic charge transport devices that takes advantage from an original input region geometry in place of standard Ohmic input contacts. Our scheme is based on a n-i-n lateral junction as electron injector, an etched intrinsic channel, a standard Ohmic output contact and a pair of in-plane gates. We show that surface acoustic waves are able to pick up electrons from a current flowing through the n-i-n junction and steer them toward the output contact. Acoustic charge transport was studied as a function of the injector current and bias, the SAW power and at various temperatures. The possibility to modulate the acoustoelectric current by means of lateral in-plane gates is also discussed. The main advantage of our approach relies on the possibility to drive the n-i-n injector by means of both voltage or current sources, thus allowing to sample and process voltage and current signals as well., Comment: 9 pages, 3 figures. Submitted to Applied Physics Letters

Electroluminescence emission from surface acoustic wave-driven light-emitting diodes (SAWLEDs) is studied by means of time-resolved techniques. We show that the intensity of the SAW-induced electroluminescence is modulated at the SAW frequency (~1 GHz), demonstrating electron injection into the p-type region synchronous with the SAW wavefronts., Comment: 4 pages, 3 figures

Electroluminescence emission controlled by means of surface acoustic waves (SAWs) in planar light-emitting diodes (pLEDs) is demonstrated. Interdigital transducers for SAW generation were integrated onto pLEDs fabricated following the scheme which we have recently developed. Current-voltage, light-voltage and photoluminescence characteristics are presented at cryogenic temperatures. We argue that this scheme represents a valuable building block for advanced optoelectronic architectures.

Planar light-emitting diodes (LEDs) fabricated within a single high-mobility quantum well are demonstrated. Our approach leads to a dramatic reduction of radiative lifetime and junction area with respect to conventional vertical LEDs, promising very high-frequency device operation. Devices were fabricated by UV lithography and wet chemical etching starting from p-type modulation-doped AlGaAs/GaAs heterostructures grown by molecular beam epitaxy. Electrical and optical measurements from room temperature down to 1.8 K show high spectral purity and high external efficiency. Time-resolved measurements yielded extremely short recombination times of the order of 50 ps, demonstrating the relevance of the present scheme for high-frequency device applications in the GHz range., Comment: 5 pages, 3 figures

Time-dependent capacitance measurements reveal an unstable phase of electrons in gallium arsenide quantum well that occurs when two Landau levels with opposite spin are brought close to degeneracy by applying a gate voltage. This phase emerges below a critical temperature and displays a peculiar non-equilibrium dynamical evolution. The relaxation dynamics is found to follow a stretched exponential behavior and correlates with hysteresis loops observed by sweeping the magnetic field. These experiments indicate that metastable randomly-distributed magnetic domains are involved in the relaxation process in a way that is equivalently tunable by a change in gate voltage or temperature., Comment: 7 pages, including 4 figures Changes made to introduction Added figure Submitted to SSC

Aharonov-Bohm (AB) interference is reported for the first time in the conductance of a vertical nanostructure based on a single GaAs/AlGaAs quantum well (QW). The two lowest subbands of the well are spatially separated by the Hartree barrier originating from electronic repulsion in the modulation-doped QW and provide AB two-path geometry. Split-gates control the in-plane electronic momentum dispersion. In our system, we have clearly demonstrated AB interference in both electrostatic and magnetic modes. In the latter case the magnetic field was applied parallel to the QW plane, and perpendicular to the 0.02 um^2 AB loop. In the electrostatic mode of operation the single-QW scheme adopted led to large transconductance oscillations with relative amplitudes exceeding 30 %. The relevance of the present design strategy for the implementation of coherent nanoelectronic devices is underlined., Comment: Accepted for publication on Physical Review B Rapid Communications

The single-particle energy spectrum of a two-dimensional electron gas in a perpendicular magnetic field consists of equally-spaced spin-split Landau levels, whose degeneracy is proportional to the magnetic field strength. At integer and particular fractional ratios between the number of electrons and the degeneracy of a Landau level (filling factors n) quantum Hall effects occur, characterised by a vanishingly small longitudinal resistance and quantised Hall voltage. The quantum Hall regime offers unique possibilities for the study of cooperative phenomena in many-particle systems under well-controlled conditions. Among the fields that benefit from quantum-Hall studies is magnetism, which remains poorly understood in conventional material. Both isotropic and anisotropic ferromagnetic ground states have been predicted and few of them have been experimentally studied in quantum Hall samples with different geometries and filling factors. Here we present evidence of first-order phase transitions in n = 2 and 4 quantum Hall states confined to a wide gallium arsenide quantum well. The observed hysteretic behaviour and anomalous temperature dependence in the longitudinal resistivity indicate the occurrence of a transition between the two distinct ground states of an Ising quantum-Hall ferromagnet. Detailed many-body calculations allowed the identification of the microscopic origin of the anisotropy field.