A quantum yield map for synthetic eumelanin

The quantum yield of synthetic eumelanin is known to be extremely low and it has recently been reported to be dependent on excitation wavelength. In this paper, we present quantum yield as a function of excitation wavelength between 250 and 500 nm, showing it to be a factor of 4 higher at 250 nm than at 500 nm. In addition, we present a definitive map of the steady-state fluorescence as a function of excitation and emission wavelengths, and significantly, a three-dimensional map of the specific quantum yield: the fraction of photons absorbed at each wavelength that are subsequently radiated at each emission wavelength. This map contains clear features, which we attribute to certain structural models, and shows that radiative emission and specific quantum yield are negligible at emission wavelengths outside the range of 585 and 385 nm (2.2 and 3.2 eV), regardless of excitation wavelength. This information is important in the context of understanding melanin biofunctionality, and the quantum molecular biophysics therein. (c) 2005 American Institute of Physics.

Radiative relaxation in synthetic pheomelanin

We report a detailed photoluminescence study of cysteinyldopa-melanin ( CDM), the synthetic analogue of pheomelanin. Emission spectra are shown to be a far more sensitive probe of CDM's spectroscopic behavior than are absorption spectra. Although CDM and dopa-melanin ( DM, the synthetic analogue of eumelanin) have very similar absorption spectra, we find that they have very different excitation and emission characteristics; CDM has two distinct photoluminescence peaks that do not shift with excitation wavelength. Additionally, our data suggest that the radiative quantum yield of CDM is excitation energy dependent, an unusual property among biomolecules that is indicative of a chemically disordered system. Finally, we find that the radiative quantum yield for CDM is similar to 0.2%, twice that of DM, although still extremely low. This means that 99.8% of the energy absorbed by CDM is dissipated via nonradiative pathways, consistent with its role as a pigmentary photoprotectant.

Quantitative fluorescence excitation spectra of synthetic eumelanin

Previously reported excitation spectra for eumelanin are sparse and inconsistent. Moreover, these studies have failed to account for probe beam attenuation and emission reabsorption within the samples, making them qualitative at best. We report for the first time quantitative excitation spectra for synthetic eumelanin, acquired for a range of solution concentrations and emission wavelengths. Our data indicate that probe beam attenuation and emission reabsorption significantly affect the spectra even in low-concentration eumelanin solutions and that previously published data do not reflect the true excitation profile. We apply a correction procedure (previously applied to emission spectra) to account for these effects. Application of this procedure reconstructs the expected relationship of signal intensity with concentration, and the normalized spectra show a similarity in form to the absorption profiles. These spectra reveal valuable information regarding the photophysics and photochemistry of eumelanin. Most notably, an excitation peak at 365 urn (3.40 eV), whose position is independent of emission wavelength, is possibly attributable to a 5,6-dihydroxyindole-2-carboxylic acid (DHICA) component singly linked to a polymeric structure.

Anomalous fluorescence spectra in an extremely weak, broadband squeezed vacuum under monochromatic and bichromatic excitation

We show that a two-level atom interacting with an extremely weak squeezed vacuum can display resonance fluorescence spectra that are qualitatively different to those that can be obtained using fields with a classical analogue. We consider first the free space situation with monochromatic excitation, and then discuss a bichromatically driven two-level atom in a cavity as a practical scenario for experimentally detecting the anomalous features predicted. We show that in the bad cavity limit, the anomalous spectral features appear for a weak squeezed vacuum and large frequency differences of the bichromatic field, conditions which are easily accessible in laboratories. The advantage of bichromatic, as opposed to monochromatic, excitation is that there is no coherent scattering at line centre which could obscure the observations. A scaling law is derived, N similar to Omega(4) which relates the squeezed photon number to the Rabi frequency at which the anomalous features appear. (C) 1998 Elsevier Science B.V.

Response of a two-level atom to a narrow-bandwidth squeezed-vacuum excitation

Using the coupled-system approach we calculate the optical spectra of the fluorescence and transmitted fields of a two-level atom driven by a squeezed vacuum of bandwidths smaller than the natural atomic linewidth. We find that in this regime of squeezing bandwidths the spectra exhibit unique features, such as a hole burning and a three-peak structure, which do not appear for a broadband excitation. We show that the features are unique to the quantum nature of the driving squeezed vacuum field and donor appear when the atom is driven by a classically squeezed field. We find that a quantum squeezed-vacuum field produces squeezing in the emitted fluorescence field which appears only in the squeezing spectrum while there is no squeezing in the total field. We also discuss a nonresonant excitation and find that depending on the squeezing bandwidth there is a peak or a hole in the spectrum at a frequency corresponding to a three-wave-mixing process. The hole appears only for a broadband excitation and results from the strong correlations between squeezed-vacuum photons.

Supersonic velocimetry in a shock tube using laser enhanced ionisation and planar laser induced fluorescence

A novel flow-tagging technique is presented which was employed to measure gas velocities in the free stream of a shock tube. This method is based on the laser spectroscopic techniques of Laser-Enhanced Ionisation (LEI) and Laser-Induced Fluorescence (LIF). The flow in the shock tube is seeded with small amounts of sodium, and LEI is used to produce a substantial depletion of neutral sodium atom concentration in a well-defined region of the flow, by using two wavelength-resonance excitation and subsequent collisional ionisation. At a specific time delay, single-laser-pulse planar LIF is utilised to produce a two-dimensional (2-D) inverse image of the depleted tagged region downstream of the flow. By measuring the displacement of the tagged region, free stream velocities in a shock tube were determined. Large variations in the concentration of sodium seeded into the flow were observed and even in the presence of these large variations accurate free-stream velocity measurements were obtained. The experimentally determined value for velocity compares very well with the predicted velocity.

Direct measurement of pulse distortion near the zero-dispersion wavelength in an optical fiber by frequency-resolved optical gating

The technique of frequency-resolved optical gating is used to characterize the intensity and the phase of picosecond pulses after propagation through 700 m of fiber at close to the zero-dispersion wavelength. Using the frequency-resolved optical gating technique, we directly measure the severe temporal distortion resulting from the interplay between self-phase modulation and higher-order dispersion in this regime. The measured intensity and phase of the pulses after propagation are found to be in good agreement with the predictions of numerical simulations with the nonlinear Schrodinger equation. (C) 1997 Optical Society of America.

Simultaneous two-wavelength holographic interferometry in a superorbital expansion tube facility

A new variation of holographic interferometry has been utilized to perform simultaneous two-wavelength measurements, allowing quantitative analysis of the heavy particle and electron densities in a superorbital facility. An air test gas accelerated to 12 km/s was passed over a cylindrical model, simulating reentry conditions encountered by a space vehicle on a superorbital mission. Laser beams with two different wavelengths have been overlapped, passed through the test section, and simultaneously recorded on a single holographic plate. Reconstruction of the hologram generated two separate interferograms at different. angles from which the quantitative measurements were made. With this technique, a peak electron concentration of (5.5 +/- 0.5) x 10(23) m(-3) was found behind a bow shock on a cylinder. (C) 1997 Optical Society of America.

Heat of desorption measured by means of electrical heat excitation

A new method of measuring heat of desorption is proposed in this Letter. The principle of the method is to measure the amount of mass released when a controlled amount of energy is supplied directly to a solid adsorbent. This is in contrast to conventional methods such as microcalorimetry, where heat released upon adsorption is measured. In this method, a quantified heat supply is generated by passing a de current through a carbon pellet, which is equilibrated with a gas phase confined in a closed vessel. As a consequence of the heating, the particle temperature is increased, resulting in partial desorption of adsorbed molecules. The variations of pellet temperature and the system pressure with respect to time are used to determine the heat of desorption as a function of loading.

The plausibility of long-wavelength stress correlation or stress magnitude as a mechanism for precursory seismicity: Results from two simple elastic models

Observations of accelerating seismic activity prior to large earthquakes in natural fault systems have raised hopes for intermediate-term eartquake forecasting. If this phenomena does exist, then what causes it to occur? Recent theoretical work suggests that the accelerating seismic release sequence is a symptom of increasing long-wavelength stress correlation in the fault region. A more traditional explanation, based on Reid's elastic rebound theory, argues that an accelerating sequence of seismic energy release could be a consequence of increasing stress in a fault system whose stress moment release is dominated by large events. Both of these theories are examined using two discrete models of seismicity: a Burridge-Knopoff block-slider model and an elastic continuum based model. Both models display an accelerating release of seismic energy prior to large simulated earthquakes. In both models there is a correlation between the rate of seismic energy release with the total root-mean-squared stress and the level of long-wavelength stress correlation. Furthermore, both models exhibit a systematic increase in the number of large events at high stress and high long-wavelength stress correlation levels. These results suggest that either explanation is plausible for the accelerating moment release in the models examined. A statistical model based on the Burridge-Knopoff block-slider is constructed which indicates that stress alone is sufficient to produce accelerating release of seismic energy with time prior to a large earthquake.

Organic microcavity light-emitting diodes with metal mirrors: dependence of the emission wavelength on the viewing angle

Organic microcavity light-emitting diodes typically exhibit a blueshift of the emitting wavelength with increasing viewing angle. We have modeled the shift of the resonance wavelength for several metal mirrors. Eight metals (Al, Ag, Cr, Ti, Au, Ni, Pt, and Cu) have been considered as top or bottom mirrors, depending on their work functions. The model fully takes into account the dependence of the phase change that occurs on reflection on angle and wavelength for both s and p polarization, as well as on dispersion in the organic layers. Different contributions to the emission wavelength shift are discussed. The influence of the thickness of the bottom mirror and of the choice and thickness of the organic materials inside the cavity has been investigated. Based on the results obtained, guidelines for a choice of materials to reduce blueshift; are given. (C) 2002 Optical Society of America.

Asymmetric Bragg mirrors for the reduction of emission wavelength dependence on the viewing angle in organic microcavity light emitting diodes

Organic microcavity light emitting diodes typically exhibit a blue shift of the emitting wavelength with increasing viewing angle. While the wavelength shift can be reduced with the appropriate choice of organic materials and metal mirrors, for further reduction of the emission wavelength shift it is necessary to consider a mirror whose phase shift can partly compensate the effect of the change of optical path within the cavity. In this work, we used a genetic algorithm (GA) to design an asymmetric Bragg mirror in order to minimize the emission wavelength shift with viewing angle. Based on simulation results, the use of asymmetric Bragg mirrors represents a promising way to reduce the emission wavelength shift. Detailed comparison between GA optimized and conventional Bragg mirrors in terms of resonant wavelength dependence on the viewing angle, spectral narrowing, and brightness enhancement is given. (C) 2004 Elsevier B.V. All rights reserved.