Basic principles of ultrafast Raman loss spectroscopy

When a light beam passes through any medium, the effects of interaction of light with the material depend on the field intensity. At low light intensities the response of materials remain linear to the amplitude of the applied electromagnetic field. But for sufficiently high intensities, the optical properties of materials are no longer linear to the amplitude of applied electromagnetic field. In such cases, the interaction of light waves with matter can result in the generation of new frequencies due to nonlinear processes such as higher harmonic generation and mixing of incident fields. One such nonlinear process, namely, the third order nonlinear spectroscopy has become a popular tool to study molecular structure. Thus, the spectroscopy based on the third order optical nonlinearity called stimulated Raman spectroscopy (SRS) is a tool to extract the structural and dynamical information about a molecular system. Ultrafast Raman loss spectroscopy (URLS) is analogous to SRS but is more sensitive than SRS. In this paper, we present the theoretical basis of SRS (URLS) techniques which have been developed in our laboratory.

Experimental observations of watertable waves in an unconfined aquifer with a sloping boundary

Observations of horizontal and vertical variations in piezometric head in a homogeneous, laboratory aquifer are presented and discussed. The observed fluctuations are induced by a simple harmonic oscillation in the clear water reservoir acting across a sloping boundary. The data qualitatively supports existing theories in that higher harmonics are generated in the active forcing zone and that a significant increase in the inland, asymptotic watertable over height (relative to that found for the vertical boundary case) is observed. The observed overheight is shown to be accurately reproduced by existing small-amplitude perturbation theory. Detailed measurements in the vicinity of the sloping boundary reveal that the signal of generated higher harmonics is strongest near the sand surface and that vertical flows are significant in this region. The aquifer is of finite-depth and is influenced by capillary effects, the experimental data therefore exposes limitations of theories which are based on the assumption of a shallow aquifer free of capillary effects. The dispersive properties of the measured pressure wave in the aquifer are comparable to those found from field observations and likewise do not agree with those predicted by the capillary free, shallow aquifer theory. Although some improvement is obtained, discrepancies between the data and theory persist even when a finite-depth aquifer and capillary effects are considered in the theoretical model. Further sand column experiments eliminate a truncated capillary fringe as a possible contributor to these discrepancies. However, the neglect of horizontal flows in the fringe may have caused the discrepancies. (C) 2004 Elsevier Ltd. All rights reserved.

Phase control of higher spectral components in the presence of a static electric field

We investigate the higher spectral component generations driven by a few-cycle laser pulse in a dense medium when a static electric field is present. Our results show that, when assisted by a static electric field, the dependence of the transmitted laser spectrum on the carrier-envelope phase (CEP) is significantly increased. Continuum and distinct peaks can be achieved by controlling the CEP of the few-cycle ultrashort laser pulse. Such a strong variation is due to the fact that the presence of the static electric field modifies the waveform of the combined electric field, which further affects the spectral distribution of the generated higher spectral components.

Generation of attosecond pulses in a system with permanent dipole moment

The generation of attosecond pulses in a two-level system with permanent dipole moment is investigated. It is shown due to the presence of permanent dipole moments, that the plateau of the high-order harmonic generation spectrum can be extended to X-ray range. Moreover, attosecond pulses with higher intensity can be synthesized by using both even and odd harmonics because of their quantum interference. (c) 2006 Elsevier B.V. All rights reserved.

Isolated sub-30-as pulse generation of an He+ ion by an intense few-cycle chirped laser and its high-order harmonic pulses

We present an efficient method to generate a ultrashort attosecond (as) pulse when a model He+ ion is exposed to the combination of an intense few-cycle chirped laser pulse and its 27th harmonics. By solving the time-dependent Schroumldinger equation, we found that high-order harmonic generation (HHG) from He+ ion is enhanced by seven orders of magnitude due to the presence of the harmonic pulse. After optimizing the chirp of the fundamental pulse, we show that the cut-off energy of the generated harmonics is extended effectively to I-p+25.5U(p). As a result, an isolated 26-as pulse with a bandwidth of 170.5 eV can be obtained directly from the supercontinuum around the cut-off of HHG. To better understand the physical origin of HHG enhancement and attosecond pulse emission, we perform semiclassical simulations and analyze the time-frequency characteristics of attosecond pulse.

Generation of bright, extreme-ultraviolet harmonic radiation from a krypton fluoride laser

We present results of experiments studying the efficiency of high harmonic generation from a gas target using the TITANIA krypton fluoride laser at the Rutherford Appleton Laboratory. The variation of harmonic yield for the 7th to 13th harmonics (355-191 Angstrom) is studied as a function of the backing pressure of a solenoid valve gas jet and of the axial position of the laser focus relative to the centre of the gas jet nozzle. Harmonic energies up to 1 mu J were produced in helium and neon targets from laser energies of approximately 200 mJ. This corresponds to absolute conversion efficiencies of up to 5 x 10(-6).

Imaging of high harmonic radiation emitted during the interaction of a 20 TW laser with a solid target

We present images of the source of extreme ultraviolet (XUV) harmonic emission at a wavelength of 220 Angstrom from the interaction of a 20 TW, 1.053 mu m Nd:glass laser beam focused to intensities up to 4x10(18) W cm(-2) onto a solid target. From these measurements we determine an upper limit to the source size and brightness of the harmonic emission to show its efficacy as a novel source of short-pulse, coherent XUV radiation. We also demonstrate the empirical scaling of the harmonic generation efficiency with irradiance up to 10(19) W mu m(2) cm(-2), and extrapolate to estimate the possible source brightness at higher irradiances. These source brightnesses are compared to those available from an x-ray laser system. (C) 1997 American Institute of Physics.

2ND-HARMONIC LIGHT GENERATION IN THE INTERACTION OF LASER-BEAMS WITH UNDERCRITICAL PLASMAS

The process of second harmonic generation (SHG) in undercritical plasmas is studied. It is shown that filamentation and self-focusing of the laser beam in the plasma can break the plasma density symmetry and lead to SHG by free electrons. In turn, second harmonic emission may be used to investigate the plasma parameters and to diagnose the process of laser beam filamentation itself.

Optical autocorrelator that uses a surface-emitting second-harmonic generator on (211)B GaAs

An optical autocorrelator grown on a (211)B GaAs substrate that uses visible surface-emitted second-harmonic generation is demonstrated. The (211)B orientation needs TE mode excitation only, thus eliminating the problem of the beating between the TE and TM modes that is required for (100)-grown devices; it also has the advantage of giving higher upconversion efficiency than (111) growth. Values of waveguide loss and the difference in the effective refractive index between the TE(0) and TE(1) modes were also obtained from the autocorrelation experiment.

Optical autocorrelator that uses a surface-emitting second-harmonic generator on (211)B GaAs

An optical autocorrelator grown on a (211)B GaAs substrate that uses visible surface-emitted second-harmonic generation is demonstrated. The (211)B orientation needs TE mode excitation only, thus eliminating the problem of the beating between the TE and TM modes that is required for (100)-grown devices; it also has the advantage of giving higher upconversion efficiency than (111) growth. Values of waveguide loss and the difference in the effective refractive index between the TE(0) and TE(1) modes were also obtained from the autocorrelation experiment.

Theoretical and numerical investigation of plasmon nanofocusing in metallic tapered rods and grooves

Effective focusing of electromagnetic (EM) energy to nanoscale regions is one of the major challenges in nano-photonics and plasmonics. The strong localization of the optical energy into regions much smaller than allowed by the diffraction limit, also called nanofocusing, offers promising applications in nano-sensor technology, nanofabrication, near-field optics or spectroscopy. One of the most promising solutions to the problem of efficient nanofocusing is related to surface plasmon propagation in metallic structures. Metallic tapered rods, commonly used as probes in near field microscopy and spectroscopy, are of a particular interest. They can provide very strong EM field enhancement at the tip due to surface plasmons (SP’s) propagating towards the tip of the tapered metal rod. A large number of studies have been devoted to the manufacturing process of tapered rods or tapered fibers coated by a metal film. On the other hand, structures such as metallic V-grooves or metal wedges can also provide strong electric field enhancements but manufacturing of these structures is still a challenge. It has been shown, however, that the attainable electric field enhancement at the apex in the V-groove is higher than at the tip of a metal tapered rod when the dissipation level in the metal is strong. Metallic V-grooves also have very promising characteristics as plasmonic waveguides. This thesis will present a thorough theoretical and numerical investigation of nanofocusing during plasmon propagation along a metal tapered rod and into a metallic V-groove. Optimal structural parameters including optimal taper angle, taper length and shape of the taper are determined in order to achieve maximum field enhancement factors at the tip of the nanofocusing structure. An analytical investigation of plasmon nanofocusing by metal tapered rods is carried out by means of the geometric optics approximation (GOA), which is also called adiabatic nanofocusing. However, GOA is applicable only for analysing tapered structures with small taper angles and without considering a terminating tip structure in order to neglect reflections. Rigorous numerical methods are employed for analysing non-adiabatic nanofocusing, by tapered rod and V-grooves with larger taper angles and with a rounded tip. These structures cannot be studied by analytical methods due to the presence of reflected waves from the taper section, the tip and also from (artificial) computational boundaries. A new method is introduced to combine the advantages of GOA and rigorous numerical methods in order to reduce significantly the use of computational resources and yet achieve accurate results for the analysis of large tapered structures, within reasonable calculation time. Detailed comparison between GOA and rigorous numerical methods will be carried out in order to find the critical taper angle of the tapered structures at which GOA is still applicable. It will be demonstrated that optimal taper angles, at which maximum field enhancements occur, coincide with the critical angles, at which GOA is still applicable. It will be shown that the applicability of GOA can be substantially expanded to include structures which could be analysed previously by numerical methods only. The influence of the rounded tip, the taper angle and the role of dissipation onto the plasmon field distribution along the tapered rod and near the tip will be analysed analytically and numerically in detail. It will be demonstrated that electric field enhancement factors of up to ~ 2500 within nanoscale regions are predicted. These are sufficient, for instance, to detect single molecules using surface enhanced Raman spectroscopy (SERS) with the tip of a tapered rod, an approach also known as tip enhanced Raman spectroscopy or TERS. The results obtained in this project will be important for applications for which strong local field enhancement factors are crucial for the performance of devices such as near field microscopes or spectroscopy. The optimal design of nanofocusing structures, at which the delivery of electromagnetic energy to the nanometer region is most efficient, will lead to new applications in near field sensors, near field measuring technology, or generation of nanometer sized energy sources. This includes: applications in tip enhanced Raman spectroscopy (TERS); manipulation of nanoparticles and molecules; efficient coupling of optical energy into and out of plasmonic circuits; second harmonic generation in non-linear optics; or delivery of energy to quantum dots, for instance, for quantum computations.