Guillaume Bachelier

Optical Second Harmonic Generation of Single Metallic Nanoparticles Embedded in a Homogeneous Medium

We report the optical second harmonic generation from individual 150 nm diameter gold nanoparticles dispersed in gelatin. The quadratic hyperpolarizability of the particles is determined and the input polarization dependence of the second harmonic intensity obtained. These results are found in excellent agreement with ensemble measurements and finite element simulations. These results open up new perspectives for the investigation of the nonlinear optical properties of noble metal nanoparticles.

Origin of optical second-harmonic generation in spherical gold nanoparticles: Local surface and nonlocal bulk contributions

The second-harmonic generation of 150 nm spherical gold nanoparticles is investigated both experimentally and theoretically. We demonstrate that the interference effects between dipolar and octupolar plasmons can be used as a fingerprint to discriminate the local surface and non-local bulk contributions to the second-harmonic generation. By fitting the experimental data with the electric fields computed with finite-element method (FEM) simulations, the Rudnick and Stern parameters weighting the relative nonlinear sources efficiencies are evaluated and the validity of the hydrodynamic model and the local density approximation approaches are discussed.

Multipolar second-harmonic generation in noble metal nanoparticles

Second-harmonic generation from noble metal nanoparticles with a noncentrosymmetrical shape is theoretically investigated by using finite element method simulations. The relative weight of the dipolar and quadrupolar responses is investigated in terms of both light polarization and size dependence of the harmonic scattered intensity. It is shown that, even for small deformations as compared with purely spherical particles, the dipolar response dominates and scales as the nanoparticle surface area squared. The difference between gold and silver metal nanoparticles is also addressed.

Silencing and enhancement of second-harmonic generation in optical gap antennas

Amplifying local electromagnetic fields by engineering optical interactions between individual constituents of an optical antenna is considered fundamental for efficient nonlinear wavelength conversion in nanometer-scale devices. In contrast to this general statement we show that high field enhancement does not necessarily lead to an optimized nonlinear activity. In particular, we demonstrate that second-harmonic responses generated at strongly interacting optical gap antennas can be significantly suppressed. Numerical simulations are confirming silencing of second-harmonic in these coupled systems despite the existence of local field amplification. We then propose a simple approach to restore and amplify the second-harmonic signal by changing the manner in which electrically-connected optical antennas are interacting in the charge-transfer plasmon regime. Our observations provide critical design rules for realizing optimal structures that are essential for a broad variety of nonlinear surface-enhanced characterizations and for realizing the next generation of electrically-driven optical antennas.

Plasma formation and structural modification below the visible ablation threshold in fused silica upon femtosecond laser irradiation

We have investigated the temporal and spatial evolution of the ablation process induced in fused silica upon irradiation with single 120fs laser pulses at 800nm. Time-resolved microscopy images of the surface reflectivity at 400nm reveal the existence of a transient plasma distribution with annular shape surrounding the visible ablation crater. The material in this annular zone shows an increased reflectivity after irradiation, consistent with a local refractive index increase of approximately 0.01. White light interferometry measurements indicate a shallow surface depression in this outer region, most likely due to material densification.

Time- and space-resolved dynamics of ablation and optical breakdown induced by femtosecond laser pulses in indium phosphide

Femtosecond time-resolved microscopy has been used to analyze the structural transformation dynamics (melting, ablation, and solidification phenomena) induced by single intense 130 fs laser pulses in single-crystalline (100)-indium phosphide wafers in air on a time scale from ∼100 fs up to 8 ns. In the ablative regime close to the ablation threshold, transient surface reflectivity patterns are observed by fs microscopy on a ps to ns time scale as a consequence of the complex spatial density structure of the ablating material (dynamic Newton fringes). At higher fluences, exceeding six times the ablation threshold, optical breakdown causes another, more violent ablation regime, which reduces the energy deposition depth along with the time of significant material removal. As a consequence, ablation lasts longer in a ring-shaped region around the region of optical breakdown. This leads to the formation of a crater profile with a central protrusion. In the melting regime below the ablation threshold, the melti...

First Hyperpolarizability of the Natural Aromatic Amino Acids Tryptophan, Tyrosine, and Phenylalanine and the Tripeptide Lysine−Tryptophan−Lysine Determined by Hyper-Rayleigh Scattering

We report the first hyperpolarizability of tryptophan (Trp) and tyrosine (Tyr) and an upper limit for that of phenylalanine (Phe), three natural aromatic amino acids. The measurements were performed with hyper-Rayleigh scattering in an aqueous Tris buffer solution at a pH of 8.5 and 150 mM salt concentration with a fundamental wavelength of 780 nm. A value of (4.7 ± 0.7) × 10(-30) esu is found for Trp and (4.1 ± 0.7) × 10(-30) esu for Tyr whereas the upper limit of 1.4 × 10(-30) esu is found for that of Phe due to its limited solubility. The influence of the presence of lysine (Lys) in close vicinity of Trp is investigated with a measurement of the first hyperpolarizabilty of Trp in an excess of Lys and compared to the first hyperpolarizability obtained for the tripeptide Lys-Trp-Lys. The clear decrease of the values measured in these two cases indicates that the first hyperpolarizabilty of Trp is very sensitive to its local environment.

Far-field background suppression in tip-modulated apertureless near-field optical microscopy

In apertureless near-field optical microscopy the vertical dithering of the tip, associated with demodulation at higher harmonics (n>1), allows us to suppress the far-field background, providing artifact free elastic scattering images. This paper analyzes, both theoretically and experimentally, the physical origin of the background signal at the different harmonics and the mechanisms underlying its rejection for the general case of propagative-field illumination. We show that Fourier components of the background must be expected at every harmonic, evidencing why demodulation at higher harmonics is not an inherently background-free technique, and assessing the experimental conditions in which it becomes like that. In particular, we put forward the fundamental roles of both the harmonic order and the tip oscillation amplitude in the background suppression mechanisms. Furthermore, we outline how the lock-in detection of the signals amplitude can enhance the nonlinear dependence of the background on the tip-s...

Three-dimensional mapping of single gold nanoparticles embedded in a homogeneous transparent matrix using optical second-harmonic generation

We report the three-dimensional mapping of 150 nm gold metallic nanoparticles dispersed in a homogeneous transparent polyacrylamide matrix using second-harmonic generation. We demonstrate that the position of single nanoparticles can be well defined using only one incident fundamental beam and the harmonic photon detection performed at right angle. The fundamental laser beam properties are determined using its spatial autocorrelation function and used to prove that single nanoparticles are observed. Polarization resolved measurements are also performed allowing for a clear separation of the second-harmonic response of the single gold metallic nanoparticles from that of aggregates of such nanoparticles.

Wigner and Kondo physics in quantum point contacts revealed by scanning gate microscopy.

Quantum point contacts exhibit mysterious conductance anomalies in addition to well-known conductance plateaus at multiples of 2e(2)/h. These 0.7 and zero-bias anomalies have been intensively studied, but their microscopic origin in terms of many-body effects is still highly debated. Here we use the charged tip of a scanning gate microscope to tune in situ the electrostatic potential of the point contact. While sweeping the tip distance, we observe repetitive splittings of the zero-bias anomaly, correlated with simultaneous appearances of the 0.7 anomaly. We interpret this behaviour in terms of alternating equilibrium and non-equilibrium Kondo screenings of different spin states localized in the channel. These alternating Kondo effects point towards the presence of a Wigner crystal containing several charges with different parities. Indeed, simulations show that the electron density in the channel is low enough to reach one-dimensional Wigner crystallization over a size controlled by the tip position.