THz Generation by Two-Color Plasma: Time Shaping and Ultra-Broadband Polarimetry.

The generation of terahertz radiation via laser-induced plasma from two-color femtosecond pulses in air has been extensively studied due to its broad emission spectrum and significant pulse energy. However, precise control over the temporal properties of these ultra-broadband terahertz pulses, as well as the measurement of their polarization state, remain challenging. In this study, we review our latest findings on these topics and present additional results not previously reported in our earlier works. First, we investigate the impact of chirping on the fundamental wave and the effect of manipulating the phase difference between the fundamental wave and the second-harmonic wave on the properties of generated terahertz pulses. We demonstrate that we can tune the time shape of terahertz pulses, causing them to reverse polarity or become bipolar by carefully selecting the correct combination of chirp and phase. Additionally, we introduce a novel technique for polarization characterization, termed terahertz unipolar polarimetry, which utilizes a weak probe beam and avoids the systematic errors associated with traditional methods. This technique is effective for detecting polarization-structured terahertz beams and the longitudinal component of focused terahertz beams. Our findings contribute to the improved control and characterization of terahertz radiation, enhancing its application in fields such as nonlinear optics, spectroscopy, and microscopy.

High-resolution terahertz-driven atom probe tomography.

Ultrafast control of matter by a strong electromagnetic field on the atomic scale is essential for future investigations and manipulations of ionization dynamics and excitation in solids. Coupling picosecond duration terahertz pulses to metallic nanostructures allows the generation of extremely localized and intense electric fields. Here, using single-cycle terahertz pulses, we demonstrate control over field ion emission from metallic nanotips. The terahertz near field is shown to induce an athermal ultrafast evaporation of surface atoms as ions on the subpicosecond time scale, with the tip acting as a field amplifier. The ultrafast terahertz-ion interaction offers unprecedented control over ultrashort free-ion pulses for imaging, analyzing, and manipulating matter at atomic scales. Here, we demonstrate terahertz atom probe microscopy as a new platform for microscopy with atomic spatial resolution and ultimate chemical resolution.

Super-resolution Optical Spectroscopy of Nanoscale Emitters within a Photonic Atom Probe.

Atom Probe Tomography (APT) is a microscopy technique allowing for the 3D reconstruction of the chemical composition of a nanoscale needle-shaped sample with a precision close to the atomic scale. The photonic atom probe (PAP) is an evolution of APT featuring in situ and operando detection of the photoluminescence signal. The optical signatures of the light-emitting centers can be correlated with the structural and chemical information obtained by the analysis of the evaporated ions. It becomes thus possible to discriminate and interpret the spectral signatures of different light emitters as close as 20 nm, well beyond the resolution limit set by the exciting laser wavelength. This technique opens up new perspectives for the study of the physics of low dimensional systems, defects and optoelectronic devices.

Conduction mechanisms and voltage drop during field electron emission from diamond needles.

We report results of experimental investigation of field electron emission from diamond nanoemitters. The measurements were performed with single crystal diamond needles fixed at tungsten tips. The voltage drop along diamond needles during emission was revealed and measured using electron energy spectroscopy. The observed linear dependence of the voltage drop in diamond on voltage applied to the tungsten tip is explained in the frame of a simple macroscopic electrical model combining Poole-Frenkel conduction along the diamond tip and Fowler-Nordheim tunneling at the diamond-vacuum junction. Experimental evidences of electron emission sensitivity to laser illumination are discussed for possible modification of diamond emitter characteristics and voltage drop.

Dissociation Dynamics of Molecular Ions in High dc Electric Field.

In an atom probe, molecular ions can be field evaporated from the analyzed material and, then, can dissociate under the very intense electric field close to the field emitter. In this work, field evaporation of ZnO reveals the emission of Zn2O2(2+) ions and their dissociation into ZnO(+) ions. It is shown that the repulsion between the produced ZnO(+) ions is large enough to have a measurable effect on both the ion trajectories and times of flight. Comparison with numerical simulations of the ion trajectories gives information on the lifetime of the parent ions, the energy released by the dissociation and repulsion, and also the dissociation direction. This study not only opens the way to a new method to obtain information on the behavior of molecular ions in high electric fields by using an atom probe, but also opens up the interesting perspective to apply this technique to a wide class of materials and molecules.

Correlation of microphotoluminescence spectroscopy, scanning transmission electron microscopy, and atom probe tomography on a single nano-object containing an InGaN/GaN multiquantum well system.

A single nanoscale object containing a set of InGaN/GaN nonpolar multiple-quantum wells has been analyzed by microphotoluminescence spectroscopy (µPL), high-resolution scanning transmission electron microscopy (HR-STEM) and atom probe tomography (APT). The correlated measurements constitute a rich and coherent set of data supporting the interpretation that the observed µPL narrow emission lines, polarized perpendicularly to the crystal c-axis and with energies in the interval 2.9-3.3 eV, are related to exciton states localized in potential minima induced by the irregular 3D In distribution within the quantum well (QW) planes. This novel method opens up interesting perspectives, as it will be possible to apply it on a wide class of quantum confining emitters and nano-objects.

Coupling atom probe tomography and photoluminescence spectroscopy: exploratory results and perspectives.

The development of laser-assisted atom probes makes it possible, in principle, to exploit the femtosecond laser pulse not only for triggering ion evaporation from a nanometric field emission tip, but also for generating photons via the radiative recombination of electron-hole pairs in tips made of dielectric materials. In this article we demonstrate a first step towards a correlation of micro-photoluminescence (µ-PL) and laser-assisted tomographic atom probe (LA-TAP) analysis applied separately on the same objects, namely on ZnO microwires. In particular, we assess that the use of the focused ion beam (FIB) tip preparation method significantly degrades the radiative recombination yield of the analyzed microwires. We discuss the strategies to avoid the FIB-induced damage on the optical properties of the sample and how to get beyond the correlated µ-PL and LA-TAP analysis with a coupled approach allowing to perform the two analyses within the same instrument.

Electric-field-induced deformation dynamics of a single nematic disclination.

Disclinations in nematic liquid crystals usually adopt a straight shape in order to minimize their elastic energy. Once created in the course of a nonequilibrium process such as a temperature quench from the isotropic to the nematic phase, the topologically stable disclinations of half-integer strength either annihilate each other in pairs of opposite strength or form topologically unstable disclinations of integer strength. In this article, we demonstrate that the annihilation process can be inhibited and the defects can be deformed by an applied electric field. We study the disclination lines in the deep uniaxial nematic phase, located at the boundary between two different types of walls, the so-called pi wall (a planar soliton stabilized by the surface anchoring) and the Brochard-Léger (BL) wall stabilized by the applied electric field. By changing the electric voltage, one can control the energy of director deformations associated with the two walls and thus control the deformation and dynamics of the disclination line. At small voltages, the disclinations are straight lines connecting the opposite plates of the cell, located at the two ends of the pi walls. The pi walls tend to shrink. When the voltage increases above E(F), the Fréedericksz threshold, the BL walls appear and connect pairs of disclinations along a path complementary to the pi wall. At E>2 E(F), the BL walls store sufficient energy to prevent shrinking of the pi walls. Reconstruction of the three-dimensional director configuration using a fluorescent confocal polarizing microscopy demonstrates that the disclinations are strongly bent in the region between the pi and the BL walls. The distortions and the related dynamics are associated with the transformation of the BL wall into two surface disclination lines; we characterize it experimentally as a function of the applied electric field, the cell thickness, and the sample temperature. A simple model captures the essential details of the experimental data.

Optical Fréedericksz transition in liquid crystals and transfer of the orbital angular momentum of light.

Multistability, out-of-polarization-plane reorientation, and persistent oscillations have been observed in the optical Fréedericks transition in a homeotropically aligned nematic film using a normally incident linearly polarized laser beam with elliptical rather than circular cross section. These features could be ascribed to the presence of an additional optical torque connected with a transfer of the orbital angular momentum of light to the liquid crystal film. A model based on Ritz's variational method confirms this picture.

Optical angular momentum transfer to transparent isotropic particles using laser beam carrying zero average angular momentum.

The torque exerted by an astigmatic optical beam on small transparent isotropic particles was dynamically measured observing the angular motion of the particles under a microscope. The data confirmed that torque was originated by the transfer of orbital angular momentum associated with the spatial changes in the phase of the optical field induced by the moving particle. This mechanism for angular momentum transfer works also with incident light beams with no net angular momentum.