Investigation of plasmonic response of metal nanoparticles to ultrashort laser pulses

In this thesis the interaction of ultrashort laser pulses with metal nanostructures is investigated via two different phenomena: coherent acoustic oscillations of nanoparticles and generation of THz pulses on metal surfaces. Both of these effects rely on the collective oscillations of free conduction electrons in metal surfaces, plasmons. The field of plasmonics gained a great interest in the last twenty years due to the unique properties of these surface modes. It is the effects of the resonant response of plasmonic structures to incident electromagnetic wave, in particular, in visible and infrared bands and the concentration of the electromagnetic field in small subwavelength regions with significant enhancement of the incident field that make plasmonics so attractive for various applications, such as biochemical sensing, enhanced fluorescence, surface-enhanced Raman scattering, and second harmonic generation, amongst others. Investigation of the coherent particle vibrations is performed using the pump-probe technique which allows measurement of the transient transmission signals. The expansion and subsequent contraction of the nanoparticle following the ultrashort laser pulse excitation lead to a shift of the plasmon band which can be traced by transient spectroscopy. We have investigated the effect of the particle thickness on the frequency of the fundamental vibrational mode. In addition, we measured the vibrational particle response during the particle shape deformation, both symmetrical and asymmetrical. Exploration of the THz generation phenomena on plasmonic structures was performed using THz time-domain spectroscopy, the method which allows tracing of the generated THz field in the time-domain. We were able for the first time to measure the THz pulses generated from arrays of metal nanoparticles. Our observations verify the role of the particle plasmon mode in the generation of THz pulses. In addition, by exploring the dependence of the THz emission on the femtosecond pulse intensity we showed a high nonlinearity in the THz generation mechanism. The experimental results were assessed in the context of a recently proposed model where the THz radiation is generated via the acceleration of the ejected electrons by ponderomotive forces. To reveal another proposed mechanism of the THz generation from plasmonic structures, namely optical rectification, we investigated the THz generation and electron emission from the arrays of nanoparticles and nanoholes. Our results suggest that both mechanisms may contribute to generation of THz pulses from the same sample under different illumination conditions. In addition to periodic arrays of nanoparticles and nanoholes, THz generation from random metal-dielectric films was investigated. The microstructuring of such films allowed selective THz frequency generation which was explained by a model of dipole THz emitters. In addition, the effects of low temperature and pressure on the THz generation efficiency were investigated

Controlling the generation of THz radiation from metallic films using periodic microstructure

We report on THz frequency generation via irradiation of microstructured semicontinuous silver films by femtosecond laser pulses. By patterning the film so as to produce an array of microstrips, we show that one can use periodic microstructure to control the way nanostructured metal films produce THz radiation when illuminated by femtosecond infrared laser pulses. A simple analytical model based on the field distribution arising from an array of THz dipole emitters is used to assess the experimental data, allowing us to explain some of the main features of the generated THz radiation patterns, including the strongly resonant features of the emission spectrum

Optical imaging of strain in two-dimensional crystals

Strain engineering is widely used in material science to tune the (opto-)electronic properties of materials and enhance the performance of devices. Two-dimensional atomic crystals are a versatile playground to study the influence of strain, as they can sustain very large deformations without breaking. Various optical techniques have been employed to probe strain in two-dimensional materials, including micro-Raman and photoluminescence spectroscopy. Here we demonstrate that optical second harmonic generation constitutes an even more powerful technique, as it allows to extract the full strain tensor with a spatial resolution below the optical diffraction limit. Our method is based on the strain-induced modification of the nonlinear susceptibility tensor due to a photoelastic effect. Using a two-point bending technique, we determine the photoelastic tensor elements of molybdenum disulfide. Once identified, these parameters allow us to spatially image the two-dimensional strain field in an inhomogeneously strained sample.Comment: 13 pages, 4 figure

Novel highly conductive and transparent graphene based conductors

Future wearable electronics, displays and photovoltaic devices rely on highly conductive, transparent and yet mechanically flexible materials. Nowadays indium tin oxide (ITO) is the most wide spread transparent conductor in optoelectronic applications, however the mechanical rigidity of this material limits its use for future flexible devices. Here we report novel transparent conductors based on few layer graphene (FLG) intercalated with ferric chloride (FeCl3) with an outstandingly high electrical conductivity and optical transparency. We show that upon intercalation a record low sheet resistance of 8.8 Ohm/square is attained together with an optical transmittance higher than 84% in the visible range. These parameters outperform the best values of ITO and of other carbon-based materials, making these novel transparent conductors the best candidates for future flexible optoelectronics

Mechanisms of THz generation from silver nanoparticle and nanohole arrays illuminated by 100 fs pulses of infrared light

Copyright © 2014 American Physical SocietyWe study THz pulses generated from plasmonic metal nanostructures under femtosecond illumination of near-IR light. We find two regimes of excitation, according to the order of the dependence of the THz fluence on the incident near-IR intensity: less then second order at low intensities, changing to approximately fourth order for higher intensities. These regimes are most likely associated with two THz generation mechanisms: optical rectification, and the ponderomotive acceleration of ejected electrons. These data provide evidence that both mechanisms can be at work in the same experiment.Hungarian Scientific Research FundBolyai FellowshipPostdoctoral Fellowship of the Hungarian Academy of SciencesMarie Curie Fellowship of the EU (project acronym `UPNEX'

Mechanisms of THz generation from silver nanoparticle and nanohole arrays illuminated by 100 fs pulses of infrared light

Copyright © 2014 American Physical SocietyWe study THz pulses generated from plasmonic metal nanostructures under femtosecond illumination of near-IR light. We find two regimes of excitation, according to the order of the dependence of the THz fluence on the incident near-IR intensity: less then second order at low intensities, changing to approximately fourth order for higher intensities. These regimes are most likely associated with two THz generation mechanisms: optical rectification, and the ponderomotive acceleration of ejected electrons. These data provide evidence that both mechanisms can be at work in the same experiment.Hungarian Scientific Research FundBolyai FellowshipPostdoctoral Fellowship of the Hungarian Academy of SciencesMarie Curie Fellowship of the EU (project acronym `UPNEX'

In-sensor computing using a MoS2 photodetector with programmable spectral responsivity

Abstract Optical spectroscopy is an indispensable technique in almost all areas of scientific research and industrial applications. After its acquisition, an optical spectrum is usually further processed using a mathematical algorithm to classify or quantify the measurement results. Here we present the design and realization of a smart photodetector that provides such information directly without the need to explicitly record a spectrum. This is achieved by tailoring the spectral responsivity of the device to a specific purpose. In-sensor computation is performed at the lowest possible level of the sensor system hierarchy – the physical level of photon detection – and does not require any external processing of the measurement data. The device can be programmed to cover different types of spectral regression or classification tasks. We present the analysis of spectral mixtures as an example, but the scheme can also be applied to any other algorithm that can be represented by a linear operator. Our prototype physical implementation utilizes an ensemble of optical cavity-enhanced MoS2 photodetectors with different center wavelengths and individually adjustable peak responsivities. This spectroscopy method represents a significant advance in miniaturized and energy-efficient optical sensing