A. A. Kolomenskii

Sensitivity and detection limit of concentration and adsorption measurements by laser-induced surface-plasmon resonance

The shot noise limitation as well as other factors that influence the sensitivity of measurements with a surface plasmon resonance (SPR) sensor are considered. It is demonstrated that minute changes in the refractive index of a medium close to the surface of a metal film can be detected owing to a shift in the resonance angle. In particular, changes in the adsorption layer of only a fraction of a biomolecular monolayer could be measured. Data for SPR are presented with adjacent media of air, water, as well as aqueous solutions of ethanol and sodium chloride at different concentrations. The immobilization of the protein bovine serum albumin to a specially prepared surface was monitored with the SPR technique. Specific responses to changes in the concentration and thickness of the adsorption layer were determined. The angular resolution of the present apparatus is approximately 1 millidegree, corresponding to a detection limit for an adsorbed protein layer of 15 pg/mm(2), which is still 2 to 3 orders of magnitude larger than the shot-noise limit, and therefore a further improvement in sensitivity is possible.

Propagation length of surface plasmons in a metal film with roughness.

The propagation of laser-excited surface plasmons along a gold film with surface roughness is directly observed via scattered light. The attenuation length of surface plasmons in a broad wavelength interval is calculated for smooth gold and silver films. The surface roughness, which was characterized with an AFM, introduces corrections to the attenuation length, angular dependence of the surface plasmon resonance, and the effective dielectric constant of the metal film. These corrections are also taken into account and discussed.

Surface-plasmon resonance spectrometry and characterization of absorbing liquids

The effect of absorption of the sample medium on the surface-plasmon resonance (SPR) characteristics is analyzed by approximate analytical and exact numerical models. We show that absorption leads to specific changes in the value of reflectivity near the SPR angle and that these can be used for absorbance detection. The strongest absorption-induced change in reflectivity occurs at two values of metal film thickness (28 and 55 nm for a gold film and lambda = 632.8 nm). Using a sample solution of Rhodamine 700 in ethanol, we measured the characteristic changes in the SPR angle and in reflectivity over the wavelength interval encompassing the strong absorption band at 610-680 nm. The possibility of the simultaneous determination of the refractive index and absorption from SPR measurements is demonstrated and has the potential for substance-specific detection.

Effect of varying electric potential on surface-plasmon resonance sensing.

The high sensitivity of surface-plasmon resonance (SPR) sensors allows measurements of small variations in surface potentials to be made. We studied the changes of the SPR angle when an oscillating electric potential was applied to a gold film on which surface plasmons were excited. The shifts of the SPR resonance angle were observed for various aqueous solutions as an adjacent medium. A model that takes into account the redistribution of charges at the double layer near the metal-liquid interface as well as the oxidation of the gold film was developed. It was found that a change in the electronic density at voltages below the oxidation potential and, in addition, the oxidation of the gold surface above this potential are the main mechanisms that account for the observed dependences. It was shown that relatively slow oxidation-reduction processes can explain the observed hysteresis effect. Application of these techniques to studies of dielectric properties and conformational changes of polar biomolecules, such as tubulin, are discussed.

High-power mid-infrared frequency comb source based on a femtosecond Er:fiber oscillator

We report on a high-power mid-infrared (MIR) frequency comb source based on a femtosecond (fs) Er:fiber oscillator with a stabilized repetition rate of 250 MHz. The MIR frequency comb is produced through difference frequency generation in a periodically poled MgO-doped lithium niobate crystal. The output power is about 120 mW, with a pulse duration of about 80 fs and spectrum coverage from 2.9 to 3.6 μm, and the single comb mode power is larger than 0.3 μW over the range of 700 nm. The coherence properties of the produced high-power broadband MIR frequency comb are maintained, which was verified by heterodyne measurements. As the first application, the spectrum of a ~200 ppm methane-air mixture in a short 20 cm glass cell at ambient atmospheric pressure and temperature was measured.

Coherent transfer of optical orbital angular momentum in multi-order Raman sideband generation

Experimental results from the generation of Raman sidebands using optical vortices are presented. By generating two sets of sidebands originating from different locations in a Raman-active crystal, one set containing optical orbital angular momentum and the other serving as a reference, Youngs double slit experiment was simultaneously realized for each sideband. The interference between the two sets of sidebands was used to determine the helicity and topological charge in each order. Topological charges in all orders were found to be discrete and follow selection rules predicted by a cascaded Raman process.

Mid-infrared dual frequency comb spectroscopy based on fiber lasers for the detection of methane in ambient air

We utilize mid-infrared dual frequency comb spectroscopy for the detection of methane in ambient air. Two mid-infrared frequency comb sources based on femtosecond Er:fiber oscillators are produced through difference frequency generation with periodically poled MgO-doped lithium niobate crystals and stabilized at slightly different repetition rates at about 250 MHz. We performed dual frequency comb spectroscopy in the spectral range between 2900 cm−1 and 3150 cm−1 with 0.07 cm−1 resolution using a multipass cell of ~580 m path length, and achieved the sensitivity about 7.6 × 10−7 cm−1 with 80 ms data acquisition time. We determined the methane concentration as ~1.5 ppmv in the ambient air of the laboratory, and the detection limit as ~60 ppbv for the current setup.

Real-time dual frequency comb spectroscopy in the near infrared

We use two femtosecond lasers with slightly different repetition rates to perform real-time dual frequency comb spectroscopy in the near infrared. The difference between the repetition rates is δ = 4403 Hz, yielding a minimal time interval between subsequently measured interferograms and spectra of 0.227 ms. It takes as short as 4 μs to record a single interferogram, opening the possibility of studying dynamical processes. We work with different spectral outputs from two Erbium-doped fiber lasers and employ a grating based spectral filter in a 2f-2f setup to select the common spectral region of interest, thereby increasing the signal-to-noise ratio.

White-light generation control with crossing beams of femtosecond laser pulses

We investigated the variations in generated white-light when crossing two femtosecond laser beams in a Kerr medium. By changing the relative delay of two interacting intense femtosecond laser pulses, we show that white-light generation can be enhanced or suppressed. With a decrease of the relative delay an enhancement of the white-light output was observed, which at even smaller delays was reverted to a suppression of white-light generation. Under choosen conditions, the level of suppression resulted in a white-light output lower than the initial level corresponding to large delays, when the pulses do not overlap in time. The enhancement of the white-light generation takes place in the pulse that is lagging. We found that the effect of the interaction of the beams depends on their relative orientation of polarization and increases when the polarizations are changed from perpendicular to parallel. The observed effects are explained by noting that at intermediate delays, the perturbations introduced in the path of the lagging beam lead to a shortening of the length of filament formation and enhancement of the white-light generation, whereas at small delays the stronger interaction and mutual rescattering reduces the intensity in the central part of the beams, suppressing filamentation and white-light generation.

Observation of coherent acoustic and optical phonons in bismuth nanowires by a femtosecond pump-probe technique

Coherent acoustic and optical phonon oscillations in Bi nanowire samples were studied with a femtosecond pump-probe technique. Laser pulses of 50 fs excited simultaneously acoustic oscillations at a frequency of about 9.5 GHz and optical phonons in the terahertz range. The transmission signal of nanowires on a glass substrate and the signal of light scattered from freestanding nanowires were measured. The acoustic velocity in nanowires was found to be close to that of bulk polycrystalline material. The changes in the optical phonon frequency at different laser fluences were simulated taking into account excitation inhomogeneity, lattice anharmonicity, diffusion, and recombination of the carriers and gave good agreement with experimental results.