Feasibility of nonlinear Raman lidar based on stimulated Raman gain spectroscopy without a tunable laser

A novel technique of lidar for atmospheric gas detection by use of stimulated Raman gain spectroscopy without any tunable laser is proposed. Detection sensitivity and detectable range are estimated on the basis of the lidar equation for CO2, CH4, and H2 in the atmosphere. The feasibility study clearly shows that the technique has a potential for application to lidar and that, in addition, the construction of the system is simpler than those of traditional differential absorption lidars.     

Raman spectroscopy of crystals for stimulated Raman scattering

Raman frequency shift, line width, integral and peak Raman scattering cross sections were measured in various crystals using spontaneous Raman spectroscopy. The highest Raman gain coefficient in steady state Stimulated Raman Scattering (SRS) regime was proved to be in barium nitrate crystal; for transient SRS it is expected to be in lithium niobate and tungstate crystals. Barium molybdate crystal is proposed as a new highly efficient Raman material.OCIS: 300.6450; 290.5910; 190.2640     

The imaginary components of dispersion parameters and the Stokes mode dynamics in stimulated Raman scattering

The Stokes pulse dynamics during stimulated Raman scattering has been studied in the constant pumping approximation. The nonlinear problem of interaction between a pumping wave and the Stokes component is reduced to a linear equation describing propagation of an optical pulse in the amplifying medium with imaginary components of the first-and second-order dispersion parameters, the presence of which leads to the possibility of the pulse envelope propagation at a supraluminal velocity.     

Dependence of the gain in stimulated rotational Raman scattering in H2 on the pump ellipticity

Abstract

The intensity of the radiation resulting from stimulated rotational Raman scattering of an elliptically polarized pump beam by gaseous H² was measured as a function of the pump ellipticity in an unseeded experiment. The results show excellent agreement with the predictions of a simple two-beam classical model of the process which incorporates only components at the pump and the Stokes frequencies but includes the effects of pump depletion.     

Squeezed states in spontaneous Raman and in stimulated Raman processes

The Hamiltonian and the equations of motion for various modes involving spontaneous and stimulated Raman processes are derived. The coupled differential equations involving these modes are solved analytically by using an intuitive approach (IA). The solution of the present paper does not require any short time approximation. As a matter of fact, the present solution for field operators and hence the squeezing for various modes are valid for all interaction time t. In this way, the present paper is more general compared to the earlier investigations where short-time approximations were found a must. By exploiting the solutions for the field operators, we obtain the squeezing effects of input coherent light for pure and for mixed field modes. The IA employs the perturbation theory and hence we came across the secular terms in the solution. Of course, for small coupling constants these secular terms could be summed for all orders. To establish our claim, we remove the secular terms at least for one occasion.     

Amplitude-squared and amplitude-cubed squeezing in stimulated Raman and in spontaneous Raman scattering

Coherent light coupled to a third-order nonlinear medium is responsible for spontaneous and for stimulated Raman processes. The analytical solutions up to second order in coupling constants of various field modes for spontaneous Raman and for stimulated Raman processes are utilized to obtain the amplitude-squared and amplitude-cubed squeezing of the input coherent light. The amplitude-squared and amplitude-cubed squeezing are completely ruled out for all modes for spontaneous Raman processes. For stimulated Raman processes, we observe that the squeezing for amplitude-squared and amplitude-cubed are possible for pump and for vibrational phonon modes. It is found that the percentage of higher ordered amplitude squeezing decreases with the increase of the orders. The squeezing in Stokes and in anti-Stokes modes are ruled out even for stimulated Raman processes.     

Discrimination of bacteria and bacteriophages by Raman spectroscopy and surface-enhanced Raman spectroscopy

Detection of pathogenic organisms in the environment presents several challenges due to the high cost and long times typically required for identification and quantification. Polymerase chain reaction (PCR) based methods are often hindered by the presence of polymerase inhibiting compounds and so direct methods of quantification that do not require enrichment or amplification are being sought. This work presents an analysis of pathogen detection using Raman spectroscopy to identify and quantify microorganisms without drying. Confocal Raman measurements of the bacterium Escherichia coli and of two bacteriophages, MS2 and PRD1, were analyzed for characteristic peaks and to estimate detection limits using traditional Raman and surface-enhanced Raman spectroscopy (SERS). MS2, PRD1, and E. coli produced differentiable Raman spectra with approximate detection limits for PRD1 and E. coli of 10(9) pfu/mL and 10(6) cells/mL, respectively. These high detection concentration limits are partly due to the small sampling volume of the confocal system but translate to quantification of as little as 100 bacteriophages to generate a reliable spectral signal. SERS increased signal intensity 10(3) fold and presented peaks that were visible using 2-second acquisitions; however, peak locations and intensities were variable, as typical with SERS. These results demonstrate that Raman spectroscopy and SERS have potential as a pathogen monitoring platform.     

Propagation of Helmholtz-Gauss beams in absorbing and gain media

The propagation of Helmholtz-Gauss beams in media exhibiting loss or gain is studied. The general expressions for the field propagation, the time-averaged power on propagation, the trajectory of the beam centroid, the beam spreading, the nondiffracting distance, and the far field are derived and discussed. Explicit expressions of these parameters for Bessel-Gauss and cosine-Gauss beams are included. The general expressions can be applied straightforwardly to describe the propagation of Mathieu-Gauss and parabolic-Gauss beams in complex media as well.     

Effect of interaction between deep impurity traps on thermally stimulated currents in semiconductors

We demonstrate that the problem of determining the concentrations of free and trapped charge carriers in wide-gap semiconductors from their thermally stimulated current (TSC) curves for m interacting levels in an implicit difference scheme for numerically solving differential rate equations of TSCs reduces to finding the roots of an algebraic equation of degree m + 1. For two interacting trap levels of the same nature (electron or hole traps), we present an algorithm for numerically solving differential rate equations of TSCs which allows the concentrations of free and trapped charge carriers to be determined. TSC curves can be divided into four types according to their shape (dependent on trap parameters and experimental conditions): “splitting” (two well-resolved peaks separated by a temperature range), “saddle” (a well-defined minimum between two peaks), shoulder (on the high- or low-energy side), and “coalescence-absorption” (one peak). The modeling results are used to interpret an experimental TSC curve for semiconducting InSe and to demonstrate that, to adequately interpret experimental TSC data, one should use a model for the interaction between levels.     

Detection of anions by normal Raman spectroscopy and surface-enhanced Raman spectroscopy of cationic-coated substrates

The use of normal Raman spectroscopy and surface-enhanced Raman spectroscopy (SERS) of cationic-coated silver and gold substrates to detect polyatomic anions in aqueous environments is examined. For normal Raman spectroscopy, using near-infrared excitation, linear concentration responses were observed. Detection limits varied from 84 ppm for perchlorate to 2600 ppm for phosphate. In general, detection limits in the ppb to ppm concentration range for the polyatomic anions were achieved using cationic-coated SERS substrates. Adsorption of the polyatomic anions on the cationic-coated SERS substrates was described by a Frumkin isotherm. The SERS technique could not be used to detect dichromate, as this anion reacted with the coatings to form thiol esters. A competitive complexation method was used to evaluate the interaction of chloride ion with the cationic coatings. Hydrogen bonding and pi-pi interactions play significant roles in the selectivity of the cationic coatings.     

Effect of conformation and drop properties on surface-enhanced Raman spectroscopy of dried biopolymer drops

Biofluids are complex solutions consisting of small ions and large biopolymers such as DNA, proteins, or proteoglycans. Biopolymers affect fluid properties but their effect on drop deposition has not been examined. Hyaluronic acid (HA), an important component in synovial fluid, was chosen as a model biopolymer, and examined using surface-enhanced Raman spectroscopy (SERS). Nanoliter volumes of HA solutions were dried onto a patterned SERS substrate and spectra were collected from the dried hyaluronic acid drops with a near-infrared Raman microscope. Characteristic hyaluronic acid bands were examined. Capillary viscometry measured properties of HA solutions, and entanglement behavior was also modeled using scaling theory principles. Viscosity measurements were incorporated into models of suspended particle droplets to account for the effect of inter-chain attraction on droplet formation. Microscope images were used to evaluate the shape of the dried drop. Relative drop thickness was estimated from concentric rings found at drop edges using established models of light interference by thin films. We found SERS spectra were sensitive not only to polymer conformation, but also to type of deposition (ring versus uniform), and the thickness of the resulting deposition. These data suggest an approach to elucidate the effects of biopolymers and dehydrated biofluids on SERS analysis.     

Optical gain and stimulated emission in periodic nanopatterned crystalline silicon

Persistent efforts have been made to achieve efficient light emission from silicon in the hope of extending the reach of silicon technology into fully integrated optoelectronic circuits, meeting the needs for high-bandwidth intrachip and interchip connects. Enhanced light emission from silicon is known to be theoretically possible, enabled mostly through quantum-confinement effects. Furthermore, Raman-laser conversion was demonstrated in silicon waveguides. Here we report on optical gain and stimulated emission in uniaxially nanopatterned silicon-on-insulator using a nanopore array as an etching mask. In edge-emission measurements, we observed threshold behaviour, optical gain, longitudinal cavity modes and linewidth narrowing, along with a collimated far-field pattern, all indicative of amplification and stimulated emission. The sub-bandgap 1,278 nm emission peak is attributed to A-centre mediated phononless direct recombination between trapped electrons and free holes. The controlled nanoscale silicon engineering, combined with the low material loss in this sub-bandgap spectral range and the long electron lifetime in such A-type trapping centres, gives rise to the measured optical gain and stimulated emission and provides a new pathway to enhance light emission from silicon.     

Raman spectroscopy and imaging of graphene

Graphene has many unique properties that make it an ideal material for fundamental studies as well as for potential applications. Here we review recent results on the Raman spectroscopy and imaging of graphene. We show that Raman spectroscopy and imaging can be used as a quick and unambiguous method to determine the number of graphene layers. The strong Raman signal of single layer graphene compared to graphite is explained by an interference enhancement model. We have also studied the effect of substrates, the top layer deposition, the annealing process, as well as folding (stacking order) on the physical and electronic properties of graphene. Finally, Raman spectroscopy of epitaxial graphene grown on a SiC substrate is presented and strong compressive strain on epitaxial graphene is observed. The results presented here are highly relevant to the application of graphene in nano-electronic devices and help in developing a better understanding of the physical and electronic properties of graphene. This article is published with open access at Springerlink.com     

Dependence of signal on depth in transmission Raman spectroscopy

Recently, transmission Raman spectroscopy has been shown to be a valuable tool in the volumetric quantification of pharmaceutical formulations. In this work a Monte Carlo simulation and experimental study are performed to elucidate the dependence of the Raman signal on depth from the viewpoint of probing pharmaceutical tablets and powders in this experimental configuration. The transmission Raman signal is shown to exhibit a moderate bias toward the center of the tablets and this can be considerably reduced by using a recently developed Raman signal-enhancing concept, the "photon diode." The enhancing element not only reduces the bias but also increases the overall Raman signal intensity and consequently improves the signal-to-noise ratio of the measured spectrum. Overall, its implementation with appropriately chosen reflectivity results in a more uniform volumetric sampling across the half of the tablet where the photon diode is used (or across the tablet's entire depth if two photon diodes are used on each side of tablet) and enhanced overall sensitivity. These findings are substantiated experimentally on a segmented tablet by inserting a poly(ethelyne terephthalate) (PET) film doped with TiO(2) at different depths and monitoring its contribution to the overall transmission Raman signal from the segmented tablet. The numerical simulations also indicate considerable sensitivity of the overall Raman signal to the absorption of the sample, which is in line with large migration distances traversed by photons in these measurements. The presence of sample absorption was shown numerically to reduce the signal enhancement effect while the overall depth-dependence profile remained broadly unchanged. The absorption was also shown to produce a depth profile with the photon diode similar to that without it, although with a reduced absolute intensity of Raman signals and diminished enhancement effect.     

Understanding excitation energy transfer in metalloporphyrin heterodimers with different linkers,bonding structures,and geometries through stimulated X-ray Raman spectroscopy

We present simulations of stimulated X-ray Raman (SXRS) signals from covalently bonded porphyrin heterodimers with different linkers, chemical bonding structures, and geometries. The signals are interpreted in terms of valence electron wavepacket motion. One- and two-color SXRS signals can both mark excitation energy transfer (EET) between the porphyrin monomers. It is shown that the SXRS signals provide a novel window into EET dynamics in multiporphyrin systems, and can be used as a powerful tool to monitor the subtle chemical environment which affects EET.     

High-temperature and pressure Raman spectroscopy of diamond

This study presents the results of the first use of the moissanite anvil cell (MAC) for the in-situ high-temperature and pressure Raman spectroscopy measurement of diamond. It is observed that the T_2g vibrational mode of diamond shifts toward low frequency with increasing temperature; on the other hand, the vibration band shifts toward high frequency with increasing pressure. In the high-temperature and pressure process, the slope (∂υ/∂T) becomes zero which indicates the thermal expansion. It resulted from the temperature effect, and the pressure caused by MAC will reach a balanced state about 1.6 GPa and 175 °C. The behavior of diamonds at high temperature and high pressure is mainly dominated by temperature effects for the temperature below 320 °C and the pressure less than 5 GPa.     

Surface-enhanced Raman spectroscopy of bacteria and pollen

A technique for distinguishing biological material based on surface-enhanced Raman scattering (SERS) is reported in this work. Of particular interest is biological material that can be airborne. Silver colloidal particles with diameters in the range 10 to 20 nm and with a characteristic ultraviolet-visible (UV-VIS) absorption band at 400 nm were used to obtain SERS spectra of Escherichia coli, Pseudomonas aeruginosa, and Salmonella typhimurium bacteria and a number of tree and grass pollens (Cupressus arizonica (cypress), Sequoia sempervirens (redwood), Populus deltoides (cottonwood), Poa pratensis (Kentucky bluegrass), and Anthoxanthum odoratum (sweet vernal grass)). While differences in the SERS spectra among the bacteria were small, we found that the pollen spectra we analyzed could readily be distinguished from the bacteria spectra, and there were significant differences between pollen from different families. In order to obtain reproducible results, we studied the parameters controlling the interaction between the analyte and the nanoscale metallic surface. Our results show that the volume ratio of analyte to colloidal particles must be within a narrow range of values to optimize the signal-to-noise ratio of the SERS spectra and minimize the fluorescence from the analyte. Also, we found that the time-dependent behavior of colloidal/bacterial suspensions (or adsorption rate of the silver colloid particles on the bacteria) is strongly dependent on pH, density of bacteria in solution, and even, to some extent, the type of bacteria.     

Raman spectroscopy of diamond and doped diamond

The optimization of diamond films as valuable engineering materials for a wide variety of applications has required the development of robust methods for their characterization. Of the many methods used, Raman microscopy is perhaps the most valuable because it provides readily distinguishable signatures of each of the different forms of carbon (e.g. diamond, graphite, buckyballs). In addition it is non-destructive, requires little or no specimen preparation, is performed in air and can produce spatially resolved maps of the different forms of carbon within a specimen. This article begins by reviewing the strengths (and some of the pitfalls) of the Raman technique for the analysis of diamond and diamond films and surveys some of the latest developments (for example, surface-enhanced Raman and ultraviolet Raman spectroscopy) which hold the promise of providing a more profound understanding of the outstanding properties of these materials. The remainder of the article is devoted to the uses of Raman spectroscopy in diamond science and technology. Topics covered include using Raman spectroscopy to assess stress, crystalline perfection, phase purity, crystallite size, point defects and doping in diamond and diamond films.     

Raman spectroscopy of fullerenes and fullerene-nanotube composites

The discovery of fullerenes in 1985 opened a completely new field of materials research. Together with the single-wall carbon nanotubes (SWCNTs) discovered later, these curved carbon networks are a playground for pure as well as applied science. We present a review of Raman spectroscopy of fullerenes, SWCNTs and composite materials. Beginning with pristine C(60), we discuss intercalated C(60) compounds and polymerized C(60), as well as higher and endohedral fullerenes. Concerning SWCNTs, we show how the diameter distribution can be obtained from the Raman spectra and how doping modifies the spectra. Finally, the Raman response of C(60) encapsulated into SWCNTs (C(60) peapods) is discussed.