Nonlinear plasmonics of metallic heptamers

Second-harmonic generation (SHG) from centrosymmetric nanostructures originating from the breaking of inversion symmetry at their surfaces is a well-known phenomenon and is extensively used as a surface probe in nonlinear optical microscopy. In recent years, SHG and its subsequent enhancement using plasmonics has been observed from nanostructures such as sharp metallic tips, nanoantennae and nanodimers. However, the process is still inefficient, its mechanism not well understood, and an improvement is required. In order to achieve a higher conversion efficiency, we investigate experimentally a way to minimize the radiative losses at the fundamental frequency. In the present investigation, we use silver heptamer nanostructures and tune the subradiant mode of the Fano resonance to the fundamental of the pump source, while tuning a higher order multipolar term to the second harmonic and in the process we obtain a significant enhancement of the second harmonic signal. A detailed explanation and analysis of this is provided by considering the contribution and effect of varying different parameters, such as gap size and radius, as well as the overall symmetry of the structure. In fact, recently gold heptamers have been studied and have indeed shown strong hybridization of their constituent resonant primitive plasmonic modes, leading to new hybridized superradiant 'bright' and subradiant 'dark' modes(1, 2). The ease of fabrication and possible tunability achievable, make these structures very versatile tools for studying surface SHG in nanostructures.

Génération de deuxième et troisième harmonique avec un laser Nd:YAG en régime pulsé libre

Sébastian Favre

Industrial laser precision machining is predominately based on pulsed Nd:YAG lasers operated at a wavelength of 1.06 µm in a free running pulse regime. The objective of this thesis work has been to investigate second and third harmonic generation for such "long pulse" Nd:YAG lasers. Visible and UV radiation can be better focused. The absorption coefficient at these wavelengths is higher in most materials. Processing at the doubled or tripled frequency increases machining precision and allows processing of new classes of materials such as, e.g., high reflective metals or ceramics. Frequency doubling and tripling of Q-switched, modelocked, or CW operated Nd:YAG lasers has been the subject of numerous publications. However, the particular problems associated with the free running pulse regime have not yet been addressed. The generation of harmonics requires a laser source that can deliver radiation with high brightness. A system based on a slab crystal with a beam quality factor of M2 ≈ 1.6 and a power of up to 1.5 kW has been used in the experiments. An external electro-optical switch has been implemented in order to precisely control the laser pulse shape and duration. The non-linear coefficient and the angular acceptance have been the main criteria for selecting LBO (LiB3O5), KTP (KTiOPO4), and MgO:LiNbO3 for the frequency conversion experiments. The conversion efficiency has been measured for these crystals as a function of the intensity at the fundamental wavelength. In contrast to simple model predictions, the efficiency does not increase linearly with intensity under long pulse conditions. An intensity dependant phase mismatch is at the origin of the deviations. A heuristic model for the efficiency prediction has been developed. It is based on a linear increase of phase mismatch with intensity and it allows describing the experimental findings with sufficient accuracy. The conversion efficiency for frequency doubling is limited to about 20% at pulse durations of 100 µsec. It decreases with increasing pulse duration. Catastrophic thermal damage is at the origin of the limitation in this pulse regime. Our experiments indicate that the damage is initiated by the frequency doubled light. Temporary color centers are created in the presence of the second harmonic light. The dynamic of the creation and annihilation of these centers has been investigated. It could be shown that finally the absorption of the fundamental harmonic (infrared) radiation at these centers results in irreversible thermal damages. A power of 140 W in the second harmonic (178 MW/cm2 on a waist of 5 µm) and 12 W in the third harmonic (61 MW/cm2 in a waist of 2.5 µm) was obtained with pulses of 200 µs. This allowed to demonstrate the feasibility of material processing with very high reproducibility and definition, which for instance allowed the design and the manufacturing of micro-grippers and several other prototypes in the field of robotics and micro-engineering.

EPFL2001

Light Confinement and Nonlinear Light-Matter Interaction in Semiconductor Photonic Crystal Cavities

Mohamed Sabry Abdel-Aliem Mohamed

The ability to control and manipulate light is a fundamental aspect that is at the very core of the development of integrated photonic circuits. It is desirable to achieve such control down to a scale that is comparable to or smaller than the wavelength of light, to enable highly efficient interaction with matter, which can eventually go down to single photon levels. Photonic crystals are particularly appealing in that respect, by providing optical bandgaps and facilitating dispersion shaping, through the precise patterning of layers. This is to be accomplished ideally in compact designs that are well-suited for fabrication with current technology and by utilizing material that has the capacity for integration. By exploiting existing light-matter interaction mechanisms, the available toolset for component design can be expanded, allowing to build optical chips with a wide range of functionality. In the current work, a platform for integrated III-nitride photonic components on silicon is designed and implemented. A refined fabrication process for III-nitride micro- and nanostructures is developed, leading to the realization of suspended optical devices with both high performance and structural stability. Thorough optical and material characterization of the semiconductor layers is conducted to identify potential limitations, particularly with epitaxial GaN on Si technology, with respect to current crystal growth techniques. AlN layers based on a sputter-deposition process are proposed as an alternative for passive optical devices. Two-dimensional photonic crystals are designed in gallium nitride and aluminum nitride, targeting operational wavelengths in the near-infrared telecom range. Optimized photonic crystal cavities are considered for maximizing light confinement in the semiconductor layers. By utilizing resonance enhancement, second and third harmonic generation are demonstrated in gallium nitride photonic crystal cavities featuring record-high quality factor values. This is achieved through a far-field coupling approach under low-power continuous-wave operation. High conversion efficiencies are attained in gallium nitride, exceeding previous demonstrations in the material. Propagation of the harmonic signals in the semiconductor layer is analyzed using finite-element time-domain modeling for the feasibility of an extraction mechanism. Moreover, slow light coupled cavity waveguides are developed in a silicon platform, relying on optimized cavity designs that feature wideband operation in the near-infrared telecom range. A record-high value for group-index bandwidth product is achieved in the devices through improved design implementation. An end-fire based Fourier-space imaging technique is applied for the characterization of the optical structures, through which spatially-selective reconstruction of dispersion maps enabled accurate extraction of slow light properties. The influence of finite-size effects on slow light behavior is elucidated by implementing extended cavity chains. Furthermore, light transport regimes across the dispersion band are identified including the transition towards diffusive light transport and subsequent localization. The performance of coupled-cavity waveguides in the presence of disorder is quantified, revealing constraints on slow light transport, considering state-of-the-art fabrication.

EPFL2018

Novel Concepts for Functional High Resolution Microscopy

Matthias Geissbühler

Functional imaging of biological cells and organs is one of the key techniques that drives new discoveries in life science research and medicine. In this thesis novel concepts for functional imaging at high spatial and temporal resolution are presented. In the first part, an imaging modality named Triplet Lifetime Imaging is developed. The technique allows oxygen consumption within single cells to be monitored at sub-cellular resolution. Measurement of tissue and cell oxygenation is important in order to understand cell metabolism. The method exploits oxygen induced triplet lifetime changes. The technique is applied to a biological cell system, employing as reporter a cytosolic fusion protein of -galactosidase SNAP-tag labeled with TMR. Oxygen consumption in single smooth muscle cells A7r5 during an [Arg8]-vasopressin (AVP) induced contraction is measured. The results indicate a consumption leading to an intracellular oxygen concentration that decays mono-exponentially with time. The proposed method has the potential to become a new tool for investigating oxygen metabolism at the single cell and sub-cellular level. The method is further applied to various other biological systems, demonstrating its versatility and the usefulness of this novel imaging modality. In the second part of this thesis, a concept for optical spectroscopy named nonlinear correlation spectroscopy (NLCS) is developed. The method allows monitoring of diffusing and flowing nanoparticles made of nonlinear optical material. NLCS is a method related to fluorescence correlation spectroscopy (FCS), but instead of fluorescence intensity fluctuations, NLCS analyses coherent field fluctuations of the second and third harmonic light. In bulk material, the third harmonic contribution vanishes due to the destructive interference of the third harmonic light generated in front of and behind of the focal field (Guoy phase shift). On the other hand, nanoparticles with dimensions comparable or smaller than the focal volume can generate strong higher harmonic signals. Particles based on non-centrosymmetric non-linear materials such as KNbO3 have been found to show a strong second and third harmonic signal. The method and the theory are introduced and NLCS results for diffusing polystyrene spheres (PS) as well as KNbO3 particles are presented. These spectroscopic results open the door for future extension into imaging concepts.

EPFL2011