Plasmonic Polarization Rotation in SERS Spectroscopy.

Surface-enhanced Raman optical activity (SEROA) has been extensively investigated due to its ability to directly probe stereochemistry and molecular structure. However, most works have focused on the Raman optical activity (ROA) effect arising from the chirality of the molecules on isotropic surfaces. Here, we propose a strategy for achieving a similar effect: i.e., a surface-enhanced Raman polarization rotation effect arising from the coupling of optically inactive molecules with the chiral plasmonic response of metasurfaces. This effect is due to the optically active response of metallic nanostructures and their interaction with molecules, which could extend the ROA potential to inactive molecules and be used to enhance the sensibility performances of surface-enhanced Raman spectroscopy. More importantly, this technique does not suffer from the heating issue present in traditional plasmonic-enhanced ROA techniques, as it does not rely on the chirality of the molecules.

A multi-resistance wide-range calibration sample for conductive probe atomic force microscopy measurements.

Measuring resistances at the nanoscale has attracted recent attention for developing microelectronic components, memory devices, molecular electronics, and two-dimensional materials. Despite the decisive contribution of scanning probe microscopy in imaging resistance and current variations, measurements have remained restricted to qualitative comparisons. Reference resistance calibration samples are key to advancing the research-to-manufacturing process of nanoscale devices and materials through calibrated, reliable, and comparable measurements. No such calibration reference samples have been proposed so far. In this work, we demonstrate the development of a multi-resistance reference sample for calibrating resistance measurements in conductive probe atomic force microscopy (C-AFM) covering the range from 100 Ω to 100 GΩ. We present a comprehensive protocol for in situ calibration of the whole measurement circuit encompassing the tip, the current sensing device, and the system controller. Furthermore, we show that our developed resistance reference enables the calibration of C-AFM with a combined relative uncertainty (given at one standard deviation) lower than 2.5% over an extended range from 10 kΩ to 100 GΩ and lower than 1% for a reduced range from 1 MΩ to 50 GΩ. Our findings break through the long-standing bottleneck in C-AFM measurements, providing a universal means for adopting calibrated resistance measurements at the nanoscale in the industrial and academic research and development sectors.

Evaluation of Self-Field Effects in Magnetometers Based on Meander-Shaped Arrays of Josephson Junctions or SQUIDs Connected in Series.

Arrays of superconducting quantum interference devices (SQUIDs) are highly sensitive magnetometers that can operate without a flux-locked loop, as opposed to single SQUID magnetometers. They have no source of ambiguity and benefit from a larger bandwidth. They can be used to measure absolute magnetic fields with a dynamic range scaling as the number of SQUIDs they contain. A very common arrangement for a series array of SQUIDs is with meanders as it uses the substrate area efficiently. As for most layouts with long arrays, this layout breaks the symmetry required for the elimination of adverse self-field effects. We investigate the scaling behavior of series arrays of SQUIDs, taking into account the self-field generated by the bias current flowing along the meander. We propose a design for the partial compensation of this self-field. In addition, we provide a comparison with the case of series arrays of long Josephson junctions, using the Fraunhofer pattern for applications in magnetometry. We find that compensation is required for arrays of the larger size and that, depending on the technology, arrays of long Josephson junctions may have better performance than arrays of SQUIDs.

Dynamic properties of high-Tc superconducting nano-junctions made with a focused helium ion beam.

The Josephson junction (JJ) is the corner stone of superconducting electronics and quantum information processing. While the technology for fabricating low Tc JJ is mature and delivers quantum circuits able to reach the "quantum supremacy", the fabrication of reproducible and low-noise high-Tc JJ is still a challenge to be taken up. Here we report on noise properties at RF frequencies of recently introduced high-Tc Josephson nano-junctions fabricated by mean of a Helium ion beam focused at sub-nanometer scale on a YBa2Cu3O7 thin film. We show that their current-voltage characteristics follow the standard Resistively-Shunted-Junction (RSJ) circuit model, and that their characteristic frequency fc = (2e/h)IcRn reaches ~300 GHz at low temperature. Using the "detector response" method, we evidence that the Josephson oscillation linewidth is only limited by the thermal noise in the RSJ model for temperature ranging from T ~ 20 K to 75 K. At lower temperature and for the highest He irradiation dose, the shot noise contribution must also be taken into account when approaching the tunneling regime. We conclude that these Josephson nano-junctions present the lowest noise level possible, which makes them very promising for future applications in the microwave and terahertz regimes.

Development of a new hybrid approach combining AFM and SEM for the nanoparticle dimensional metrology.

At this time, there is no instrument capable of measuring a nano-object along the three spatial dimensions with a controlled uncertainty. The combination of several instruments is thus necessary to metrologically characterize the dimensional properties of a nano-object. This paper proposes a new approach of hybrid metrology taking advantage of the complementary nature of atomic force microscopy (AFM) and scanning electron microscopy (SEM) techniques for measuring the main characteristic parameters of nanoparticle (NP) dimensions in 3D. The NP area equivalent, the minimal and the maximal Feret diameters are determined by SEM and the NP height is measured by AFM. In this context, a kind of new NP repositioning system consisting of a lithographed silicon substrate has been specifically developed. This device makes it possible to combine AFM and SEM size measurements performed exactly on the same set of NPs. In order to establish the proof-of-concept of this approach and assess the performance of both instruments, measurements were carried out on several samples of spherical silica NP populations ranging from 5 to 110 nm. The spherical nature of silica NPs imposes naturally the equality between their height and their lateral diameters. However, discrepancies between AFM and SEM measurements have been observed, showing significant deviation from sphericity as a function of the nanoparticle size.

Transport in a Single Self-Doped Nanocrystal.

Addressing the optical properties of a single nanoparticle in the infrared is particularly challenging, thus alternative methods for characterizing the conductance spectrum of nanoparticles in this spectral range need to be developed. Here we describe an efficient method of fabricating single nanoparticle tunnel junctions on a chip circuit. We apply this method to narrow band gap nanoparticles of HgSe, which band structure combines the inverted character of the bulk semimetal with quantum confinement and self-doping. Upon tuning the gate bias, measurement reveals the presence of two energy gaps in the spectrum. The wider gap results from the interband gap, while the narrower gap results from intraband transitions. The observation of the latter near zero gate voltage confirms the doped character of the nanoparticle at the single particle level, which is in full agreement with the ensemble optical and transport measurements. Finally we probe the phototransport within a single quantum dot and demonstrate a large photogain mechanism resulting from photogating.

Ion-shaping of embedded gold hollow nanoshells into vertically aligned prolate morphologies.

Ion beam shaping is a novel technique with which one can shape nano-structures that are embedded in a matrix, while simultaneously imposing their orientation in space. In this work, we demonstrate that the ion-shaping technique can be implemented successfully to engineer the morphology of hollow metallic spherical particles embedded within a silica matrix. The outer diameter of these particles ranges between 20 and 60 nm and their shell thickness between 3 and 14 nm. Samples have been irradiated with 74 MeV Kr ions at room temperature and for increasing fluences up to 3.8 × 10(14) cm(-2). In parallel, the experimental results have been theoretically simulated by using a three-dimensional code based on the thermal-spike model. These calculations show that the particles undergo a partial melting during the ion impact, and that the amount of molten phase is maximal when the impact is off-center, hitting only one hemisphere of the hollow nano-particle. We suggest a deformation scenario which differs from the one that is generally proposed for solid nano-particles. Finally, these functional materials can be seen as building blocks for the fabrication of nanodevices with really three-dimensional architecture.

Fabrication of Ion-Shaped Anisotropic Nanoparticles and their Orientational Imaging by Second-Harmonic Generation Microscopy.

Ion beam shaping is a novel and powerful tool to engineer nanocomposites with effective three-dimensional (3D) architectures. In particular, this technique offers the possibility to precisely control the size, shape and 3D orientation of metallic nanoparticles at the nanometer scale while keeping the particle volume constant. Here, we use swift heavy ions of xenon for irradiation in order to successfully fabricate nanocomposites consisting of anisotropic gold nanoparticle that are oriented in 3D and embedded in silica matrix. Furthermore, we investigate individual nanorods using a nonlinear optical microscope based on second-harmonic generation (SHG). A tightly focused linearly or radially-polarized laser beam is used to excite nanorods with different orientations. We demonstrate high sensitivity of the SHG response for these polarizations to the orientation of the nanorods. The SHG measurements are in excellent agreement with the results of numerical modeling based on the boundary element method.

In-vacuum projection of nanoparticles for on-chip tunneling spectroscopy.

Starting with a discussion of the percolation problem applied to the trapping of conducting nanoparticles between nanometer-spaced electrodes, we show that a good strategy to trap a single nanoparticle between the electrodes is to prepare chips with low coverage of nanoparticles to avoid percolating current paths. To increase the probability of trapping a single nanoparticle, we developed a new method where nanoparticles are projected in-vacuum on the chip, followed by a measure of the tunnel current, in a cycle that is repeated up to a few thousand times until a preset threshold value is reached. A plot of the tunneling current as a function of time allows discriminating between the two possible current paths, i.e., a single nanoparticle trapped between the electrodes or a percolating path across many nanoparticles. We applied the method to prepare chip circuits with single gold nanoparticles, as demonstrated by the observation of Coulomb blockade. Furthermore, we applied the method to trap single magnetite nanoparticles for the study of electric-field-induced switching from insulator to metal in single nanoparticles.