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Sequence-defined polymers have been the object of many fascinating studies that focus on their implementation in both material and life science applications. In parallel, iterative synthetic methodologies have become more efficient, whereas the structure elucidation of these molecules is generally dependent on MS/MS analysis. Here, we report an alternative, simple strategy for the determination of the monomer order of uniform oligo(thioether ester)s. This approach, which relies on random cleavages of ester units within the macromolecular backbone via a basic treatment, enables the swift characterization of these macromolecules without the need for MS/MS. Consequently, this method can be used for decoding any information stored within the primary structure of oligoesters by means of ESI- or LC-MS. Finally, we speculate that a range of structurally diverse backbones could be susceptible towards this approach, which could promptly expand the library of chemically sequenceable macromolecules.

Analysis of crystal growth in thin films of phase-change materials can provide deeper insights in the extraordinary phase transformation kinetics of these materials excellently suited for data storage applications. In the present work crystal growth in GexSb100-x thin films with x = 6, 7, 8, 9, and 10 is studied in detail, demonstrating that the crystallization temperature increases from ∼80 °C for Ge6Sb94 to ∼200 °C for Ge10Sb90 and simultaneously the activation energy for crystal growth also significantly increases from 1.7 eV to 5.5 eV. The most interesting new finding is that in the thin films containing 8, 9, and 10 at% Ge two competing growth modes occur which can have several orders of magnitude difference in growth rate at a single external temperature: an initial mode with isotropic slow growth producing circular crystals with smooth surfaces and growth fronts and a fast growth mode producing crystals with triangular shape having rough surfaces and growth fronts indicative of dendritic-like growth. The slow-growth mode becomes increasingly dominant for crystallization at low temperatures when the Ge concentration is increased from 8 to 10 at% Ge. For a certain Ge concentration, the slow growth mode becomes increasingly dominant at lower temperatures and the fast growth mode at higher temperatures. Latent heat produced during crystallization is considered a principal factor explaining the observations. The fast growth mode is associated with (eutectic) decomposition generating more latent heat and instable growth fronts and the slow growth mode is associated with thermodynamically less stable homogeneously alloyed crystals generating less latent heat, but stable growth fronts.

The implementation of dense, one-selector one-resistor (1S1R), resistive switching memory arrays, can be achieved with an appropriate selector for correct information storage and retrieval. Ovonic threshold switches (OTS) based on chalcogenide materials are a strong candidate, but their low thermal stability is one of the key factors that prevents rapid adoption by emerging resistive switching memory technologies. A previously developed map for phase change materials is expanded and improved for OTS materials. Selected materials from different areas of the map, belonging to binary Ge-Te and Si-Te systems, are explored. Several routes, including Si doping and reduction of Te amount, are used to increase the crystallization temperature. Selector devices, with areas as small as 55 × 55 nm2, were electrically assessed. Sub-threshold conduction models, based on Poole-Frenkel conduction mechanism, are applied to fresh samples in order to extract as-processed material parameters, such as trap height and density of defects, tailoring of which could be an important element for designing a suitable OTS material. Finally, a glass transition temperature estimation model is applied to Te-based materials in order to predict materials that might have the required thermal stability. A lower average number of p-electrons is correlated with a good thermal stability.

A long-standing question for avant-garde data storage technology concerns the nature of the ultrafast photoinduced phase transformations in the wide class of chalcogenide phase-change materials (PCMs). Overall, a comprehensive understanding of the microstructural evolution and the relevant kinetics mechanisms accompanying the out-of-equilibrium phases is still missing. Here, after overheating a phase-change chalcogenide superlattice by an ultrafast laser pulse, we indirectly track the lattice relaxation by time resolved x-ray absorption spectroscopy (tr-XAS) with a sub-ns time resolution. The approach to the tr-XAS experimental results reported in this work provides an atomistic insight of the mechanism that takes place during the cooling process; meanwhile a first-principles model mimicking the microscopic distortions accounts for a straightforward representation of the observed dynamics. Finally, we envisage that our approach can be applied in future studies addressing the role of dynamical structural strain in PCMs.

Phase change materials (PCMs) can be rapidly and reversibly switched between the amorphous and crystalline state. The structural transformation is accompanied by a significant change of optical and electronic properties rendering PCMs suitable for rewritable optical data storage and non-volatile electronic memories. The phase transformation is also accompanied by an increase of the Casimir force of 20 to 25% between gold and AIST (Ag5In5Sb60Te30) upon crystallization. Here the focus is on reproducing and understanding the observed change in Casimir force, which is shown to be related to a change of the dielectric function upon crystallization. The dielectric function changes in two separate frequency ranges: the increase of absorption in the visible range is due to resonance bonding, which is unique for the crystalline phase, while free carrier absorption is responsible for changes in the infrared regime. It is shown that free carriers contribute 50% to the force contrast, while the other half comes from resonance bonding. This helps to identify PCMs that maximize force contrast. Finally it is shown that if this concept of force control is to be employed in microelectromechanical devices, then protective capping layers of PCMs must be only a few nanometers thick to minimize reduction of the force contrast.

Atomic force microscopy (AFM) investigations of living cells provide new information in both biology and medicine. However, slow cell dynamics and the need for statistically significant sample sizes mean that data collection can be an extremely lengthy process. We address this problem by parallelizing AFM experiments using a two-dimensional cantilever array, instead of a single cantilever. We have developed an instrument able to operate a two-dimensional cantilever array, to perform topographical and mechanical investigations in both air and liquid. Deflection readout for all cantilevers of the probe array is performed in parallel and online by interferometry. Probe arrays were microfabricated in silicon nitride. Proof-of-concept has been demonstrated by analyzing the topography of hard surfaces and fixed cells in parallel, and by performing parallel force spectroscopy on living cells. These results open new research opportunities in cell biology by measuring the adhesion and elastic properties of a large number of cells. Both properties are essential parameters for research in metastatic cancer development. Copyright (C) 2011 John Wiley & Sons, Ltd.

Scientific reports 6, 22353 (2016). doi:10.1038/srep22353, Published by Nature Publishing Group, London

With the recent exponential growth of applications using artificial intelligence (AI), the development of efficient and ultrafast brain-like (neuromorphic) systems is crucial for future information and communication technologies. While the implementation of AI systems using computer algorithms of neural networks is emerging rapidly, scientists are just taking the very first steps in the development of the hardware elements of an artificial brain, specifically neuromorphic microchips. In this review article, we present the current state of neuromorphic photonic circuits based on solid-state optoelectronic oscillators formed by nanoscale double barrier quantum well resonant tunneling diodes. We address, both experimentally and theoretically, the key dynamic properties of recently developed artificial solid-state neuron microchips with delayed perturbations and describe their role in the study of neural activity and regenerative memory. This review covers our recent research work on excitable and delay dynamic characteristics of both single and autaptic (delayed) artificial neurons including all-or-none response, spike-based data encoding, storage, signal regeneration and signal healing. Furthermore, the neural responses of these neuromorphic microchips display all the signatures of extended spatio-temporal localized structures (LSs) of light, which are reviewed here in detail. By taking advantage of the dissipative nature of LSs, we demonstrate potential applications in optical data reconfiguration and clock and timing at high-speeds and with short transients. The results reviewed in this article are a key enabler for the development of high-performance optoelectronic devices in future high-speed brain-inspired optical memories and neuromorphic computing., 26 pages, 18 figures, Accepted in Chaos special issue on Time-delay Dynamics

It has been suggested that a single photon can interfere with itself even if the difference between the two paths in the interferometer is larger than the “length” of the photon [Kessel’ and Moiseev, JETP Lett. 58, 81 (1993)]. The interference is regained by detecting the photons using a photon-echo process, where the absorbing atoms will, effectively, act as narrow-band filters. Such an experiment has several unique features. For example, single photons are used to carry out what is generally regarded as a multiphoton process; the absorption of a single photon can be regarded as separated into two different moments in time; the fact that the single-photon interference is regained using atoms acting as narrow-band filters as the detector means that the control of the detection process is quite different from cases where electronic (or possibly photographic) detection is used to register the interference etc. In general, interference and absorption are combined and intertwined in the experiment, which is discussed in this paper, in a way that has not been done before. In the present paper the possibility to carry out such an experiment in practice is investigated in some detail. The signal strength is explicitly calculated and the results are compared with our experimental data for the case of many interfering photons. We imply that this result can readily be extrapolated to the single-photon situation. We analyze the material parameters that are important for carrying out the experiment and give specific examples of some suitable materials.

Colloidal magnetic nanoparticles (MNPs) based on a nearly monodisperse iron oxide core and capped by oleic acid have been used as model systems for investigating the superparamagnetic spin dynamics by means of magnetometry measurements and nuclear magnetic resonance (H-1 NMR) relaxometry. The key magnetic properties (saturation magnetization, coercive field, and frequency dependent "blocking" temperature) of MNPs with different core size (3.5 nm, 8.5 nm, and 17.5 nm), shape (spherical and cubic), and dispersant (hexane and water-based formulation) have been determined. H-1 NMR dispersion profiles obtained by measuring the r(1) (longitudinal) and r(2) (transverse) nuclear relaxivities in the frequency range 0.01-60 MHz confirmed that in all samples the physical mechanisms that drive the nuclear relaxation are the Neel reversal at low temperature and the Curie relaxation at high frequency. The magnetization reversal time at room temperature extracted from the fitting of NMR data falls in the typical range of superparamagnetic systems (10(-9)-10(-10) s). Furthermore, from the distance of minimum approach we could conclude that water molecules do not arrive in close vicinity of the magnetic core. Our findings contribute to elucidate the local spin dynamics mechanisms in colloidal superparamagnetic nanoparticles which are useful in biomedical application as, e.g., contrast agents for magnetic resonance imaging.

High diffraction efficiencies have been achieved with polarization gratings recorded in thin films of an azobenzene side-chain liquid crystalline polyester by means of biphotonic processes. Efficiency values up to 30% have been reached after an induction period of 300 s and subsequent evolution with the sample in darkness. These values are at least two orders of magnitude higher than those previously reported for biphotonic recording. The gratings can be erased with unpolarized blue light and partial recovery of the diffraction efficiency has been observed after the erasure process when the sample is kept in darkness. Red light illumination of the erased film increases the recovered efficiency value and the recovery rate.

In recent years, many nanophotonic devices have been developed. Much attention has been given to the waveguides carrying surface plasmon polariton modes with subwavelength confinement and long propagation length. However, coupling far field light into a nano structure is a significant challenge. In this work, we present an architecture that enables high efficiency excitation of nanoscale waveguides in the direction normal to the waveguide. Our approach employs a bowtie aperture to provide both field confinement and high transmission efficiency. More than six times the power incident on the open area of the bowtie aperture can be coupled into the waveguide. The intensity in the waveguide can be more than twenty times higher than that of the incident light, with mode localization better than lambda(2)/250. The vertical excitation of waveguide allows easy integration. The bowtie aperture/waveguide architecture presented in this work will open up numerous possibilities for the development of nanoscale optical systems for applications ranging from localized chemical sensing to compact communication devices.

Nanoscale ridge aperture antennas have been shown to have high transmission efficiency and confined nanoscale radiation in the near field region compared with regularly-shaped apertures. The radiation enhancement is attributed to the fundamental electric-magnetic field propagating in the TE(10) mode concentrated in the gap between the ridges. This paper reports experimental demonstration of field enhancement using such ridge antenna apertures in a bowtie shape for the manufacture of nanometer size structures using an NSOM (near field scanning optical microscopy) probe integrated with nanoscale bowtie aperture. Consistent lines with width of 59 nm and as small as 24 nm have be written on photoresist using such probes.

We derive the response of a volume grating to arbitrary small deformations, using a perturbative approach. This result is of interest for two applications: (a) when a deformation is undesirable and one seeks to minimize the diffracted field's sensitivity to it and (b) when the deformation itself is the quantity of interest and the diffracted field is used as a probe into the deformed volume where the hologram was originally recorded. We show that our result is consistent with previous derivations motivated by the phenomenon of shrinkage in photopolymer holographic materials. We also present the analysis of the grating's response to deformation due to a point indenter and present experimental results consistent with theory. (c) 2005 Optical Society of America.

The reversible amorphous-crystalline phase change in a chalcogenide material, specifically the Se1-xTex alloy, has been investigated for the first time using ultrafast differential scanning calorimetry. Heating rates and cooling rates up to 5000 K/s were used. Repeated reversible amorphous-crystalline phase switching was achieved by consecutively melting, melt-quenching, and recrystallizing upon heating. Using a well-conditioned method, the composition of a single sample was allowed to shift slowly from 15 at. % Te to 60 at. % Te, eliminating sample-to-sample variability from the measurements. Using Energy Dispersive X-ray Spectroscopy composition analysis, the onset of melting for different Te-concentrations was confirmed to coincide with the literature solidus line, validating the use of the onset of melting T-m as a composition indicator. The glass transition T-g and crystallization temperature T-c could be determined accurately, allowing the construction of extended phase diagrams. It was found that T-m and T-g increase (but T-g/T-m decrease slightly) with increasing Te-concentration. Contrarily, the T-c decreases substantially, indicating that the amorphous phase becomes progressively unfavorable. This coincides well with the observation that the critical quench rate to prevent crystallization increases about three orders of magnitude with increasing Te concentration. Due to the employment of a large range of heating rates, non-Arrhenius behavior was detected, indicating that the undercooled liquid SeTe is a fragile liquid. The activation energy of crystallization was found to increase 0.5-0.6 eV when the Te concentration increases from 15 to 30 at. % Te, but it ceases to increase when approaching 50 at. % Te. (C) 2014 AIP Publishing LLC.

We report results of parallel optical nanolithography using nanoscale bowtie aperture array. These nanoscale bowtie aperture arrays are used to focus a laser beam into multiple nanoscale light spots for parallel nano-lithography. Our work employed a frequency-tripled diode-pumped solid state (DPSS) laser (lambda = 355 nm) and Shipley S1805 photoresist. An interference-based optical alignment system was employed to position the bowtie aperture arrays with the photoresist surface. Nanoscale direct-writing of sub-100nm features in photoresist in parallel is demonstrated.

Ridge nanoscale aperture antennas have been shown to be a high transmission nanoscale light source. They provide a small, polarization-dependent near-field optical spot with much higher transmission efficiency than circularly-shaped apertures with similar field confinement. This provides significant motivations to understand the electromagnetic fields in the immediate proximity to the apertures. This paper describes an experimental three-dimensional optical near-field mapping of a bowtie nano-aperture. The measurements are performed using a home-built near-field scanning optical microscopy (NSOM) system. An aluminum coated Si(3)N(4) probe with a 150 nm hole at the tip is used to collect optical signals. Both contact and constant-height scan (CHS) modes are used to measure the optical intensity at different longitudinal distances. A force-displacement curve is used to determine the tip-sample separation distance allowing the optical intensities to be mapped at distances as small as 50 nm and up to micrometer level. The experimental results also demonstrate the polarization dependence of the transmission through the bowtie aperture. Numerical simulations are also performed to compute the aperture's electromagnetic near-field distribution and are shown to agree with the experimental results.

Fundamental aspects and state-of-the-art results of thermal scanning probe lithography (t-SPL) are reviewed here. t-SPL is an emerging direct-write nanolithography method with many unique properties which enable original or improved nano-patterning in application fields ranging from quantum technologies to material science. In particular, ultrafast and highly localized thermal processing of surfaces can be achieved through the sharp heated tip in t-SPL to generate high-resolution patterns. We investigate t-SPL as a means of generating three types of material interaction: removal, conversion, and addition. Each of these categories is illustrated with process parameters and application examples, as well as their respective opportunities and challenges. Our intention is to provide a knowledge base of t-SPL capabilities and current limitations and to guide nanoengineers to the best-fitting approach of t-SPL for their challenges in nanofabrication or material science. Many potential applications of nanoscale modifications with thermal probes still wait to be explored, in particular when one can utilize the inherently ultrahigh heating and cooling rates. Review: Thermal scanning probe lithographyThermal scanning probe lithography is reviewed in the context of material removal, conversion and deposition. Scanning probe lithography has long been a promising technique for direct-write nanoscale patterning on surfaces. However, while the technique is widely used in research labs, the slow write speed has limited its use in industrial settings. Instead, thermal scanning probe lithography has emerged, in which a heated tip is used to induce localized changes in the material, enabling write speeds limited by the speed of movement of the tip itself. A team from Ecole Polytechnique Federale de Lausanne led by Juergen Brugger now reviews the current state of play for thermal scanning probe lithography, focusing on whether material is removed, changed or deposited by the heated tip, and the types of materials that have been studied.

The prospect of massive parallelism of optics enabling fast and low energy cost operations is attracting interest for novel photonic circuits where 3-dimensional (3D) implementations have a high potential for scalability. Since the technology for data input-output channels is 2-dimensional (2D), there is an unavoidable need to take 2D-nD transformations into account. Similarly, the 3D-2D and its reverse transformations are also tackled in a variety of fields such as optical tomography, additive manufacturing, and 3D optical memories. Here, we review how these 3D-2D transformations are tackled using iterative techniques and neural networks. This high-level comparison across different, yet related fields could yield a useful perspective for 3D optical design.

WE examine the present state of holographic random access memory (HRAM) systems and address the primary challenges that face this technology, specifically size, speed, and cost. We show that a fast HRAM system can be implemented with a compact architecture by incorporating conjugate readout, a smart-pixel array, and a linear array of laser diodes. Preliminary experimental results support the feasibility of this architecture. Our analysis shows that in order for the HRAM to become competitive, the principal tasks will be to reduce spatial light modulator (SLM) and detector pixel sizes to I mu m, increase the output power of compact visible-wavelength lasers to several hundred milliwatts, and develop ways to raise the sensitivity of holographic media to the order of 1 cm/J.

We describe a two-center holographic recording method for the storage of persistent holograms in doubly doped lithium niobate crystals. We use a two-center model, and we show that our experimental observations can be explained by the model. We describe experimental methods for finding the unknown material parameters of LiNbO3:Fe:Mn crystals for the two-center model, and we discuss the optimization of two-center recording. (C) 2001 Optical Society of America.