Collection of propagating electromagnetic fields by uncoated probe.

Understanding light-matter interaction at the nanoscale by observation of fine details of electromagnetic fields is achieved by bringing nanoscale probes into the nearfield of light sources, capturing information that is lost in the far field. Although metal coated probes are often used for nearfield microscopy, they strongly perturb the electromagnetic fields under study. Here, through experiment and simulation, we detail light collection by uncoated fiber probes, which minimize such perturbation. Second-harmonic light from intensely-irradiated sub-wavelength sub-surface features was imaged to avoid otherwise dominating fundamental light background, yielding clear nearfield details through a 50 nm aperture uncoated probe with ∼23 nm optical resolution. Simulations show how a metallic coating distorts optical nearfields and limits optical coupling into the probe in comparison to an uncoated probe.

Single-shot compressed optical field topography.

Femtosecond lasers are powerful in studying matter's ultrafast dynamics within femtosecond to attosecond time scales. Drawing a three-dimensional (3D) topological map of the optical field of a femtosecond laser pulse including its spatiotemporal amplitude and phase distributions, allows one to predict and understand the underlying physics of light interaction with matter, whose spatially resolved transient dielectric function experiences ultrafast evolution. However, such a task is technically challenging for two reasons: first, one has to capture in single-shot and squeeze the 3D information of an optical field profile into a two-dimensional (2D) detector; second, typical detectors are only sensitive to intensity or amplitude information rather than phase. Here we have demonstrated compressed optical field topography (COFT) drawing a 3D map for an ultrafast optical field in single-shot, by combining the coded aperture snapshot spectral imaging (CASSI) technique with a global 3D phase retrieval procedure. COFT can, in single-shot, fully characterize the spatiotemporal coupling of a femtosecond laser pulse, and live stream the light-speed propagation of an air plasma ionization front, unveiling its potential applications in ultrafast sciences.

Two-Photon Excitation Spectroscopy of Silicon Quantum Dots and Ramifications for Bio-Imaging.

Two-photon excitation in the near-infrared (NIR) of colloidal nanocrystalline silicon quantum dots (nc-SiQDs) with photoluminescence also in the NIR has potential opportunities in the field of deep biological imaging. Spectra of the degenerate two-photon absorption (2PA) cross section of colloidal nc-SiQDs are measured using two-photon excitation over a spectral range 1.46 < ℏω < 1.91 eV (wavelength 850 > λ > 650 nm) above the two-photon band gap Eg(QD)/2, and at a representative photon energy ℏω = 0.99 eV (λ = 1250 nm) below this gap. Two-photon excited photoluminescence (2PE-PL) spectra of nc-SiQDs with diameters d = 1.8 ± 0.2 nm and d = 2.3 ± 0.3 nm, each passivated with 1-dodecene and dispersed in toluene, are calibrated in strength against 2PE-PL from a known concentration of Rhodamine B dye in methanol. The 2PA cross section is observed to be smaller for the smaller diameter nanocrystals, and the onset of 2PA is observed to be blue shifted from the two-photon indirect band gap of bulk Si, as expected for quantum confinement of excitons. The efficiencies of nc-SiQDs for bioimaging using 2PE-PL are simulated in various biological tissues and compared to efficiencies of other quantum dots and molecular fluorophores and found to be comparable or superior at greater depths.

Brunel harmonics generated from ionizing clusters by few-cycle laser pulses.

We study theoretically harmonic generation from ionizing nano-clusters irradiated by intense few-cycle laser pulses and identify a Brunel-type harmonic generation mechanism that originates from subcycle ionization dynamics in clusters. Compared to Brunel harmonics in gases, the spectra are shifted toward odd-order harmonics of Mie frequency ωM due to efficient excitation of Mie oscillations. Considering the appreciable single-cluster harmonic yield and the relaxed phase-matching condition in overdense clustered plasmas, clusters driven by few-cycle laser pulses can be a promising source of vacuum-ultraviolet radiation.

New Mechanism for Ferroelectricity in the Perovskite Ca2-xMnxTi2O6 Synthesized by Spark Plasma Sintering.

Perovskite oxides hosting ferroelectricity are particularly important materials for modern technologies. The ferroelectric transition in the well-known oxides BaTiO3 and PbTiO3 is realized by softening of a vibration mode in the cubic perovskite structure. For most perovskite oxides, octahedral-site tilting systems are developed to accommodate the bonding mismatch due to a geometric tolerance factor t = (A-O)/[√2(B-O)] < 1. In the absence of cations having lone-pair electrons, e.g., Bi3+ and Pb2+, all simple and complex A-site and B-site ordered perovskite oxides with a t < 1 show a variety of tilting systems, and none of them become ferroelectric. The ferroelectric CaMnTi2O6 oxide is, up to now, the only one that breaks this rule. It exhibits a columnar A-site ordering with a pronounced octahedral-site tilting and yet becomes ferroelectric at Tc ≈ 650 K. Most importantly, the ferroelectricity at T < Tc is caused by an order-disorder transition instead of a displacive transition; this character may be useful to overcome the critical thickness problem experienced in all proper ferroelectrics. Application of this new ferroelectric material can greatly simplify the structure of microelectronic devices. However, CaMnTi2O6 is a high-pressure phase obtained at 7 GPa and 1200 °C, which limits its application. Here we report a new method to synthesize a gram-level sample of ferroelectric Ca2-xMnxTi2O6, having the same crystal structure as CaMnTi2O6 and a similarly high Curie temperature. The new finding paves the way for the mass production of this important ferroelectric oxide. We have used neutron powder diffraction to identify the origin of the peculiar ferroelectric transition in this double perovskite and to reveal the interplay between magnetic ordering and the ferroelectric displacement at low temperatures.

Out-of-Plane Piezoelectricity and Ferroelectricity in Layered α-In2Se3 Nanoflakes.

Piezoelectric and ferroelectric properties in the two-dimensional (2D) limit are highly desired for nanoelectronic, electromechanical, and optoelectronic applications. Here we report the first experimental evidence of out-of-plane piezoelectricity and ferroelectricity in van der Waals layered α-In2Se3 nanoflakes. The noncentrosymmetric R3m symmetry of the α-In2Se3 samples is confirmed by scanning transmission electron microscopy, second-harmonic generation, and Raman spectroscopy measurements. Domains with opposite polarizations are visualized by piezo-response force microscopy. Single-point poling experiments suggest that the polarization is potentially switchable for α-In2Se3 nanoflakes with thicknesses down to ∼10 nm. The piezotronic effect is demonstrated in two-terminal devices, where the Schottky barrier can be modulated by the strain-induced piezopotential. Our work on polar α-In2Se3, one of the model 2D piezoelectrics and ferroelectrics with simple crystal structures, shows its great potential in electronic and photonic applications.

Single-shot tomographic movies of evolving light-velocity objects.

Tomography--cross-sectional imaging based on measuring radiation transmitted through an object along different directions--enables non-invasive imaging of hidden stationary objects, such as internal bodily organs, from their sequentially measured projections. Here we adapt tomographic methods to visualize--in one laser shot--the instantaneous structure and evolution of a laser-induced object propagating through a transparent Kerr medium. We reconstruct 'movies' of a laser pulse's diffraction, self-focusing and filamentation from phase 'streaks' imprinted onto probe pulses that cross the main pulse's path simultaneously at different angles. Multiple probes are generated and detected compactly and simply, making the system robust, easy to align and adaptable to many problems. Our technique could potentially visualize, for example, plasma wakefield accelerators, optical rogue waves or fast ignitor pulses, light-velocity objects, whose detailed space-time dynamics are known only through intensive computer simulations.

Raman Spectroscopy of Oxide-Embedded and Ligand-Stabilized Silicon Nanocrystals.

Oxide-embedded and oxide-free alkyl-terminated silicon (Si) nanocrystals with diameters ranging from 3 nm to greater than 10 nm were studied by Raman spectroscopy. For ligand-passivated nanocrystals, the zone center Raman-active mode of diamond cubic Si shifted to lower frequency with decreasing size, accompanied by asymmetric peak broadening, as extensively reported in the literature. The size dependence of the Raman peak shifts, however, was significantly more pronounced than previously reported or predicted by the RWL (Richter, Wang, and Ley) and bond polarizability models. In contrast, Raman peak shifts for oxide-embedded nanocrystals were significantly less pronounced as a result of the stress induced by the matrix.

Laser electron accelerators for radiation medicine: a feasibility study.

Table-top laser wakefield accelerators (LWFAs), proposed theoretically in 1979, have now generated individual electron bunches in the laboratory with a significant number of electrons having energies up to 10 MeV and beyond with the maximum energy reaching tens of MeV and charge per laser pulse of > 1 nC. The attained electron beam properties have stimulated a discussion about the possible applications of LWFAs to medical radiation treatment, either directly or via conversion to x-rays. Our purpose in this paper is to analyze whether or not such applications are feasible, or can be made feasible with existing laser technology. Clinical electron beam applications require the selection of specific electron energies in the range of 6-25 MeV with a narrow energy bin (deltaE <5 MeV) for depth control, and a beam expansion to as much as 25 cm x 25 cm for various tumor radiation treatments. As a result, we show that present LWFA sources provide a dose rate that falls short of the requirements for clinical application by at least an order of magnitude. We then use particle simulations to evaluate the feasibility of developing an improved LWFA-based medical accelerator. Current LWFA sources require such high peak intensity that laser repetition rate is restricted to < or = 10 Hz. A scheme to lower the threshold and increase the repetition rate of efficient LWFA thus appears essential. We analyze one such scheme. We show that by "seeding" the primary laser pulse with a second, hundred-fold less intense pulse that is shifted downward in frequency by approximately the plasma frequency omegap, LWFA produces a yield of clinically useful electrons per pulse comparable to that provided by an unseeded source, except that the primary pulse energy is now more than one order of magnitude lower than that in current LWFAs. This enables a repetition rate of approximately 100 Hz or more using existing laser technology, and thus dose rates (several Gy/min) in the range required for medical radiation applications.