Physics of optically driven nanojunctions

Recent years have seen spectacular developments in the domain of nano-optics. Alongside the well-known techniques of super-resolution microscopy progress in nanofabrication has enabled important improvements in the fields of optical imaging and spectroscopy. Nowadays enhancements of specific near-field interactions by nano-antennae/cavities allows the optical readout of single molecule properties in a number of different systems. The observation of normal modes of vibration for example carries essential information on the orientation, link to the interface and environment in which the molecule is embedded.

This thesis develops firstly a novel theoretical frame for these vibration-cavity interactions by following the optomechanical formalism, which has proven to be an accurate treatment of a wide variety of mechanical systems interacting with a laser field. By leveraging this framework, we investigate on the one hand several quantum limits. On the other hand, for the parameter space experimentally available and for well-designed cavities, novel regimes of interaction between the collective mode of vibration of an ensemble of molecules and an optical tone seem within reach.

In parallel, this thesis experimentally explores one specific realization of such a system. In collaboration with the group of Christophe Galland we constructed the optical setups necessary to interrogate our nanostructures. The class of structures constructed, known as self-assembled nanojunctions or nanoparticles on mirror, reaches confinement of electric fields via plasmonic modes close to its fundamental limit and enables the study of many different mechanical systems whose thickness consist in a single molecule. Along this research we have developed techniques to characterize mechanical, electronic and thermal observables of nanojunctions interacting with an optical field.

Our experimental study has enabled the discovery of a novel effect related to the electronic confinement of these quasi-0-dimensional structures. The characteristic photoluminescence of metallic nanostructures is found to consistently blink in nanojunctions akin to other quantum emitters. The mechanisms explaining in detail this blinking remain debatable but the numerous experimental data collected highlight the key role of the interface in the specificities of the blinking observed. This finding opens novel ways to characterize the important and to date ill-described question of the interfaces in nanojunctions. The observed modifications of the nanojunctions optical properties might constitute an interesting step towards the development of a novel class of functional materials ('gap-materials') with enhanced and tailored electro-optical properties.

The last part of this thesis considers one technological application for this class of material by conceptually developing a new kind of detector based on the upconversion of an infrared photon to the visible; exploiting thus in a unique way the optical properties of the molecular system. The study of the quantum noises of these detectors highlights two exciting and technologically relevant directions for such devices : at room temperature these systems operate with levels of noise below state of the art devices, at lower temperatures these systems open an unexplored path towards single photon detection in a spectral range where this technology remains unavailable to date.

Realization and study of InAs/GaAs quantum dot superluminescent diodes emitting at 1.3µm

Marco Rossetti

A quantum dot is a semiconductor nanostructure that confines the motion of conduction band electrons and valence band holes in all three spatial directions, thus creating fully discrete energy levels. The confinement in the InAs/GaAs material system is generated by the bandgap difference for the two materials (∼ 0.4 eV for InAs, and ∼ 1.4 eV for GaAs) which provides a minimum of potential energy for both electrons and holes inside the InAs nanoparticle. The appearance of new nanoscale effects modifies the electro-optical properties of such a system which makes possible the improvement of existing device performance or even fascinating novel device applications. For the creation of coherent structures with very high purity and high density, as it is required for application in light emitting devices, self-assembling is a very important pathway. The quantum dot creation mostly relies on the relaxation of the strain accumulated during the growth of lattice mismatched materials, which happens in a non-equlibrium condition. This results in a statistical distribution of all the parameters characterizing the InAs nanocrystals as size, composition and strain, whose direct manifestation is the inhomogeneously broadened light emission deriving from quantum dot ensembles. At the dawning of the quantum dot development the broadening was considered as a limiting factor for application in semiconductor lasers. Today, it is considered favorably for all the applications where a broad gain spectrum is required as optical amplifiers, monolithic and external-cavity tunable lasers, and superluminescent diodes. The objective of this thesis is the application of InAs/GaAs self-assembled quantum dots to the active region of high power and broad-band superluminescent diodes emitting in the 1.3 μm wavelength region. Superluminescent diodes are edge-emitting semiconductor light sources based on the amplification of spontaneous emission along a waveguide where optical gain is achieved through current injection. They combine the high power and brightness of laser diodes with the low coherence of LEDs. The latter is a fundamental feature for the application in optical coherence tomography medical imaging, where the image resolution is related to the spectral bandwidth of the light source used. The achievement of bandwidths larger than 100 nm are demonstrated in this work through the optimization of molecular beam epitaxy growth conditions. This may be done optimizing the statistical size-dispersion of the dot ensemble, or through the use of different dot layers emitting at slightly different wavelengths. The large bandwidth emission is obtained also due to the peculiar energy structure of this material, for which a multi-state emission appears under particular injection conditions. As a term of comparison, best commercial single-chip superluminescent diodes for the imaging application at 1.3 μm show bandwidths around 60 nm. Moreover, the discrete nature of the energy levels in InAs quantum dots together with the implementation of a GaAs-based technology can be beneficial for the device temperature stability (the competing technology, based on InP, suffers from strong thermal degradation). The analysis and understanding of the device temperature characteristics will be detailed in the last chapter of the manuscript. Even though standard devices show an important temperature dependence, a better stability may be achieved through the use of p-doped active regions. In the last few years quantum dot devices have shown outstanding properties if compared to the competing quantum well technology. Low threshold currents, high temperature stability and low chirp in lasers, large bandwidths and low gain saturation in amplifiers have been demonstrated. However, in spite of the large interest among the scientific community, many of the microscopic processes at the origin of the electro-optical characteristics of this material are not completely understood yet. The physics of the quantum dot active material, will be modeled in this work through the use of systems of rate equations with different complexity depending on the system they are applied to. We will provide a mean-field rate equation model allowing to get insights about carrier dynamics in QD lasers. Also, we will develop two different traveling-wave rate equation models, one for the modeling of the L-I characteristics and the other for the modeling of the spectral characteristics of quantum dot superluminescent diodes. Considering the carrier and photon density distributions across the device cavity is essential in superluminescent diodes, where the high single pass gain results in large non-homogeneities of photon and carrier distributions. The work is motivated by an industrial cooperation with EXALOS AG, a leading company in the development, manufacturing, and sales of broadband superluminescent diodes.

EPFL2007

Investigation of photoinduced effects in plasmonic nanocavities

Aqeel Ahmed

Light matter interaction can be boosted by several orders of magnitude by tailoring the photonic environment, thus enabling a wide range of applications. One particular example are plasmonic nanostructures that support localized surface plasmon polariton (LSPP) leading to enhancement and confinement of incident electromagnetic fields. These novel properties provide access to a large number of optically driven effects within matter placed in the vicinity of such nanostructures. In this thesis, we investigate the effects of optical excitation on gold nanostructures in the presence of Raman active molecules. This is accomplished by fabricating nanoparticle on mirror (NPoM) plasmonic nanostructures where a gold nanoparticle is placed at a fixed distance from a smooth gold film using molecular monolayers. As the nanoparticle and mirror are placed only a few nanometers apart, optical excitation leads to formation of hybridized LSPP modes due to coupling between the plasmons within the nanoparticle and the mirror. This plasmonic coupling also results in confinement and subsequent enhancement of the incident light within the gap and is extremely sensitive to structural parameters of the NPoM. The creation of a homogeneous gap between the nanoparticle and mirror is quite challenging due the roughness of the mirror. Moreover, due to the large number of NPoM nanostructures present on the sample it is quite difficult to locate a specific NPoM. To bypass these difficulties atomically smooth and patterned substrates were developed using template stripping combined with conventional photolithography techniques. Next, in order to characterize the optical response of the NPoMs, a custom optical setup was built. The setup was primarily designed to investigate the plasmonic properties of the NPoM using elastic scattering spectroscopy along with surface enhanced Raman scattering (SERS) from the molecules within the gap. The combination of these two techniques was later used to investigate the effect of laser power on the NPoMs. It was discovered that the scattering spectra of the NPoMs changed irreversibly after laser exposure even with a few ÎŒW/ÎŒm2 incident intensities. Moreover, the plasmonic response of the NPoMs fabricated with well organized molecular monolayer changed much faster than the NPoMs prepared with disorganized ones. This phenomenon was also investigated in NPoMs prepared using a dielectric gap layer, by changing the gap conductivity, and by changing the nanoparticle shape. The experimental results combined with simulations suggest a decrease in gap height due to the reorientation of the molecular monolayer under optical excitation.

EPFL2021

Development of Tunable Optical MEMS for Advanced Laser Beam Shaping, Homogenizing and Speckle Reduction

Jonathan Masson

In this thesis, the development, design, fabrication and characterization of three innovative laser beam shaping, homogenizing and speckle reduction devices are reported. Typical beam shaping devices are static and not easily adaptable to a large variety of optical setups. Furthermore, the main issues when shaping coherent light are diffraction effects, speckle patterns, interferences and wavelength dependency. The devices presented in this work solve these issues. The main subjects discussed are beam shaping of coherent light and speckle reduction. Beam shaping and speckle reduction are important in many applications like laser machining, illumination, laser displays and photolithography. The first device presented is a dynamic diffuser and homogenizer for line generation. The 1D linear diffuser consists of a large single crystal silicon membrane of 5x5, 10x10 or 15x15 mm2 areas and having a thickness of 5 μm to 10 μm. This optical surface has a 100 % fill factor. The goal is to deform the membrane in one dimension only so that the light is also diffused in one dimension. The free standing continuous silicon membrane has a bridge type configuration. The actuation of the device is made electromagnetically at resonance by the use of the Lorentz force. Stiffening beams are fabricated below the membrane to decouple the 1D and 2D modes and to prevents 2D dynamic deformations. The device is fabricated on SOI wafer using standard microfabrication technologies. The devices are characterized using a laser doppler vibrometer (LDV) and a goniometer. The LDV measurements have shown that 1D and 2D modes can be excited separately. The diffusion angle is tunable between 0 to 22 mrad. The device is used to smooth out the interference effects created by a static 1D beam shaping optical element. The relative optical power efficiency of is 99.8 %. The device is capable to sustain high optical load of at least 140 W/cm2. It is now being tested in an industrial environment with high power CO2 laser for sealing glass capillaries. The second device presented is a 2D dynamic diffuser. It has to fulfill several characteristics, namely to diffuse light with small and tunable angle with high efficiency, reduce the speckle contrast and interference patterns, have a simple driving and packaging scheme and handle high optical power. A device with a 5x5 mm2 optical surface is designed, fabricated and characterized. The mirror is made of a thin and large deformable a-Si membrane which is supported by an array of posts. The disposition of the posts determines how the membrane is deformed in smaller sub-reflecting elements. A periodic and a pseudo random arrangements of the post arrays are designed. Electrostatic actuation is used to deform the membrane. The whole v deformable mirror is fabricated over a scanning stage. Out of plane resonant comb drive actuators are used to actuate the scanning stage. The diffusion of the light is performed by the deformation of the membrane while the homogenization of the beam profile is accomplished by the simultaneous scanning of the whole deformed membrane. Optical simulations are successfully used to predict the optical properties of the diffuser and to set the requirements for the electro-mechanical part of the device design. The fabrication process is using parylene-C as a refilling material and as a sacrificial layer to enable the fabrication of a 100 % fill factor deformable mirror. The membrane is continuous and release hole free. It is aluminum coated and showed an absolute optical power efficiency of 81 % in the actuated state. The high optical power handling of the device could not be tested. Nevertheless , the material of the device is silicon and the stage is connected with large springs to the frame for high heat conductivity. The pseudo random devices showed ability to shape an incoming beam regardless of its intensity profile into a output beam having a Gaussian profile. Besides, the diffusion angle is small and tunable between 0 to 10 mrad FWHM. The periodic devices is able to transform an incoming Gaussian beam into a super Gaussian intensity profile. Finally, the dynamic diffuser is capable of reducing the speckle contrast of a laser beam projected on a diffusing screen. The speckle contrast is reduced from 0.7 to 0.21 using the device alone and it is reduced to 0.11 when the dynamic diffuser is used in combination with a static diffuser. Tunable diffusion angle, smoothing of interferences, tunable beam shaping and speckle re- duction is realized while keeping the degree of freedom of the device to a minimum. By taking advantage of the optical design of the pseudo random diffuser, only one control electrode is needed to deform the membrane and one signal is used to scan the diffuser. The result is a very compact device, simple actuation and a straightforward packaging schemes. The last device presented is a very small footprint speckle reduction device. A simple actuation scheme using comb drive actuators and four folded springs enable large in plane displacement of a random phase plate. 180 μm of in plane displacement is achieved with a driving voltage as low as 29 V. The speckle contrast is reduced to 0.21 when the device is translating at 314 Hz. A comprehensive study of the diffuser characteristics is made to understand the surface parameters of the diffuser that influence directly the performances on the speckle reduction. The surface profile of the binary height has to be well defined to insure a phase shift of π. This very small device is a good candidate for integration in any portable device where speckle reduction is needed.

EPFL2012