Nonlinear optical properties of Bi2O3-GeO2 glass at 800 and 532 nm

The nonlinear (NL) optical properties of glassy xBi2O 3-(1-x) GeO2 with x = 0.72 and 0.82 were investigated. The experiments were performed with lasers at 800 nm (pulses of 150 fs) and 532 nm (pulses of 80 ps and 250 ns). Using the Kerr gate technique, we observed that the NL response of the samples at 800 nm is faster than 150 fs. NL refraction indices, | n 2 | ≈ 5 × 10-16 cm2/W, and two-photon absorption coefficients, α 2, smaller than 0.03 cm/GW, were measured at 800 nm. At 532 nm, we measured the NL transmittance of the samples. From the results obtained, we determined α 2 ≈1 cm/GW and excited-state absorption cross-sections of ≈10-22 cm2 due to free-carriers. © 2013 AIP Publishing LLC.

Seção de choque de absorção de buracos negros de Schwarzschild e de buracos acústicos canônicos

Na presente dissertação calculou-se a seção de choque de absorção de buracos negros de Schwarzschild para os campos escalar não massivo e eletromagnético. Também calculamos a seção de choque de absorção de buracos acústicos canônicos. Utilizamos um método numérico para obter os resultados em freqüências arbitrárias. Obtemos também expressões analíticas para as seções de choque de absorção nos limites de baixas e altas freqüências. Os resultados numéricos estão em excelente concordância com os valores das seções de choque de absorção em baixas e altas freqüências obtidos analiticamente. No limite em que a freqüência tende a zero, a seção de choque de absorção tende ao valor da área do horizonte de eventos tanto para o caso do campo escalar não massivo em Schwarzschild quanto para o buraco acústico canônico. Entretanto, a medida que a freqüência aumenta, estes resultados se tornam bastante distintos. Isto mostra que, apesar de a forma do espaço-tempo não exercer influência sobre a seção de choque escalar no limite em que a freqüência tende a zero, ela é determinante fora desse limite. Observamos também que os valores das seções de choque de absorção escalar e eletromagnética em Schwarzschild coincidem para freqüências e momentos angulares suficientemente grandes. O spin da partícula espalhada, neste caso, apesar de ter grande influência a baixas energias, é menos importante para o valor da seção de choque de absorção quanto maiores forem a freqüência e o momento angular da onda incidente.

IR-visible upconversion and thermal effects in Pr3+/Yb3+-codoped Ga2O3 : La2S3 chalcogenide glasses

IR-visible upconversion fluorescence spectroscopy and thermal effects in pr(3+)/Yb3+-codoped Ga2O3:La2S3 chalcogenide glasses excited at 1.064 mum is reported. Intense visible upconversion emission in the wavelength region of 480-680 nm peaked around 500, 550, 620 and 660 nm is observed. Upconversion excitation of the Pr3+ excited-state visible emitting levels is achieved by st combination of phonon-assisted absorption, energy-transfer and phonon-assisted excited-state absorption processes. A threefold upconversion emission enhancement induced by thermal effects when the codoped sample was heated in the temperature range of 20-200 degreesC is demonstrated. The thermal-induced enhancement is attributed to a multiphonon-assisted anti-Stokes process which takes place in the excitation of the ytterbium and excited-state absorption of the praseodymium. The thermal effect is modelled by conventional rate equations considering temperature-dependent effective absorption cross-sections for the F-2(7/2)-F-2(5/2) ytterbium transition and (1)G(4)-P-3(0) praseadymium excited-state absorption, and it is shown to agree very well with experimental results. Frequency upconversion in singly Pr3+-doped samples pumped at 836 nm and 1.064 mum in a two-beam configuration is also examined.

Effect of interaction with micelles on the excited-state optical properties of zinc porphyrins and J-aggregates formation

This work reports on the photophysical properties of zinc porphyrins meso-tetrakis methylpyridiniumyl (Zn2+TMPyP) and meso-tetrakis sulfonatophenyl (Zn2+TPPS) in homogeneous aqueous solutions and in the presence of sodium dodecyl sulfate (SDS) and cetyltrimethyl ammonium bromide (CTAB) micelles. The excited-state dynamic was investigated with the Z-scan technique, UV-Vis absorption, and fluorescence spectroscopy. Photophysical parameters were obtained by analyzing the experimental data with a conventional five-energy-level diagram. The interaction of the charged side porphyrin groups with oppositely charged surfactants can reduce the electrostatic repulsion between porphyrin molecules leading to aggregation, which affected the porphyrin characteristics such as absorption cross-sections, lifetimes and quantum yields. The interaction between anionic ZnTPPS with cationic CTAB micelles induced the formation of porphyrin J-aggregates, while this effect was not observed in the interaction of ZnTMPyP with SDS micelles. This difference is, probably, due to the difference in electrostatic repulsion between the porphyrin molecules. The insights obtained by these results are important for the understanding of the photophysical behavior of porphyrins, regarding potential applications in pharmacokinetics as encapsulation of photosensitizer for drug delivery systems and in its interaction with cellular membrane.

Laboratory study on the optical properties of absorbing atmospheric aerosols and field applications

The interaction between aerosols and sun light plays an important role in the radiative balance of Earth’s atmosphere. This interaction is obtained by measuring the removal (extinction), redistribution (scattering), and transformation into heat (absorption) of light by the aerosols; i.e. their optical properties. Knowledge of these properties is crucial for our understanding of the atmospheric system. rn Light absorption by aerosols is a major contributor to the direct and indirect effects on our climate system, and an accurate and sensitive measurement method is crucial to further our understanding. A homebuilt photoacoustic sensor (PAS), measuring at a 532nm wavelength, was fully characterized and its functionality validated for measurements of absorbing aerosols. The optical absorption cross-sections of absorbing polystyrene latex spheres, to be used as a standard for aerosol absorption measurements, were measured and compared to literature values. Additionally, a calibration method using absorbing aerosol of known complex refractive index was presented.rn A new approach to retrieve the effective broadband refractive indices (mbroad,eff) of aerosol particles by a white light aerosol spectrometer (WELAS) optical particle counter (OPC) was achieved. Using a tandem differential mobility analyzer (DMA)-OPC system, the nbroad,eff are obtained for both laboratory and field applications. This method was tested in the laboratory using substances with a wide range of optical properties and it was used in ambient measurements to retrieve the nbroad,eff of biomass burning aerosols in a nationwide burning event in Israel. The retrieved effective broadband refractive indices for laboratory generated scattering aerosols were: ammonium sulfate (AS), glutaric acid (GA), and sodium chloride, all within 4% of literature values. For absorbing substances, nigrosine and various mixtures of nigrosine with AS and GA were measured, as well as a lightly absorbing substance, Suwannee river fulvic acid (SRFA). For the ambient measurements, the calibration curves generated from this method were to follow the optical evolution of biomass burning (BB) aerosols. A decrease in the overall aerosol absorption and scattering for aged aerosols during the day after the fires compared to the smoldering phase of the fires was found. rn The connection between light extinction of aerosols, their chemical composition and hygroscopicity for particles with different degrees of absorption was studied. The extinction cross-section (σext) at 532nm for different mobility diameters was measured at 80% and 90% relative humidity (RH), and at an RH<10%. The ratio of the humidified aerosols to the dry ones, fRHext(%RH,Dry), is presented. For purely scattering aerosols, fRHext(%RH,Dry) is inversely proportional with size; this dependence was suppressed for lightly absorbing ones. In addition, the validity of the mixing rules for water soluble absorbing aerosols is explored. The difference between the derived and calculated real parts of the complex RIs were less than 5.3% for all substances, wavelengths, and RHs. The obtained imaginary parts for the retrieved and calculated RIs were in good agreement with each other, and well within the measurement errors of retrieval from pulsed CRD spectroscopy measurements. Finally, a core-shell structure model is also used to explore the differences between the models, for substances with low growth factors, under these hydration conditions. It was found that at 80% RH and for size parameters less than 2.5, there is less than a 5 % difference between the extinction efficiencies calculated with both models. This difference is within measurement errors; hence, there is no significant difference between the models in this case. However, for greater size parameters the difference can be up to 10%. For 90% RH the differences below a size parameter of 2.5 were up to 7%.rn Finally, the fully characterized PAS together with a cavity ring down spectrometer (CRD), were used to study the optical properties of soot and secondary organic aerosol (SOA) during the SOOT-11 project in the AIDA chamber in Karlsruhe, Germany. The fresh fractal-like soot particles were allowed to coagulate for 28 hours before stepwise coating them with SOA. The single scattering albedo for fresh fractal-like soot was measured to be 0.2 (±0.03), and after allowing the soot to coagulate for 28 hours and coating it with SOA, it increased to 0.71(±0.01). An absorption enhancement of the coated soot of up to 1.71 (±0.03) times from the non-coated coagulated soot was directly measured with the PAS. Monodisperse measurements of SOA and soot coated with SOA were performed to derive the complex refractive index (m) of both aerosols. A complex refractive index of m = 1.471(±0.008) + i0.0(±0.002) for the SOA-αO3 was retrieved. For the compact coagulated soot a preliminary complex refractive index of m = 2.04(+0.21/-0.14) + i0.34(+0.18/-0.06) with 10nm(+4/-6) coating thickness was retrieved.rn These detail properties can be use by modelers to decrease uncertainties in assessing climatic impacts of the different species and to improve weather forecasting.rn

Open Ocean and coastal phytoplankton communities of of Western Antarctic Peninsula and Drake Passage waters

Photophysiological processes as well as uptake characteristics of iron and inorganic carbon were studied in inshore phytoplankton assemblages of the Western Antarctic Peninsula (WAP) and offshore assemblages of the Drake Passage. Chlorophyll a concentrations and primary productivity decreased from in- to offshore waters. The inverse relationship between low maximum quantum yields of photochemistry in PSII (Fv/Fm) and large sizes of functional absorption cross sections (sigma PSII) in offshore communities indicated iron-limitation. Congruently, the negative correlation between Fv/Fm values and iron uptake rates across our sampling locations suggest an overall better iron uptake capacity in iron-limited pelagic phytoplankton communities. Highest iron uptake capacities could be related to relative abundances of the haptophyte Phaeocystis antarctica. As chlorophyll a-specific concentrations of humic-like substances were similarly high in offshore and inshore stations, we suggest humic-like substances may play an important role in iron chemistry in both coastal and pelagic phytoplankton assemblages. Regarding inorganic carbon uptake kinetics, the measured maximum short-term uptake rates (Vmax(CO2)) and apparent half-saturation constants (K1/2(CO2)) did not differ between offshore and inshore phytoplankton. Moreover, Vmax(CO2) and K1/2(CO2) did not exhibit any CO2-dependent trend over the natural pCO2 range from 237 to 507 µatm. K1/2(CO2) strongly varied among the sampled phytoplankton communities, ranging between 3.5 and 35.3 µmol/L CO2. While in many of the sampled phytoplankton communities, the operation of carbon-concentrating mechanisms (CCMs) was indicated by low K1/2(CO2) values relative to ambient CO2 concentrations, some coastal sites exhibited higher values, suggesting down-regulated CCMs. Overall, our results demonstrate a complex interplay between photophysiological processes, iron and carbon uptake of phytoplankton communities of the WAP and the Drake Passage.

Photophysiological responses of Southern Ocean phytoplankton to changes in CO2 concentrations: Short-term versus acclimation effects

The present study examines how different pCO2 acclimations affect the CO2- and light-dependence of photophysiological processes and O2 fluxes in four Southern Ocean (SO) key phytoplankton species. We grew Chaetoceros debilis (Cleve), Pseudo-nitzschia subcurvata (Hasle), Fragilariopsis kerguelensis (O'Meara) and Phaeocystis antarctica (Karsten) under low (160 µatm) and high (1000 ?atm) pCO2. The CO2- and light-dependence of fluorescence parameters of photosystem II (PSII) were determined by means of a fluorescence induction relaxation system (FIRe). In all tested species, nonphotochemical quenching (NPQ) is the primary photoprotection strategy in response to short-term exposure to high light or low CO2 concentrations. In C. debilis and P. subcurvata, PSII connectivity (p) and functional absorption cross-sections of PSII in ambient light (sigma PSII') also contributed to photoprotection while changes in re-oxidation times of Qa acceptor (tQa) were more significant in F. kerguelensis. The latter was also the only species being responsive to high acclimation pCO2, as these cells had enhanced relative electron transport rates (rETRs) and sigma PSII' while tQa and p were reduced under short-term exposure to high irradiance. Low CO2-acclimated cells of F. kerguelensis and all pCO2 acclimations of C. debilis and P. subcurvata showed dynamic photoinhibition with increasing irradiance. To test for the role and presence of the Mehler reaction in C. debilis and P. subcurvata, the light-dependence of O2 fluxes was estimated using membrane inlet mass spectrometry (MIMS). Our results show that the Mehler reaction is absent in both species under the tested conditions. We also observed that dark respiration was strongly reduced under high pCO2 in C. debilis while it remained unaltered in P. subcurvata. Our study revealed species-specific differences in the photophysiological responses to pCO2, both on the acclimation as well as the short-term level.

Phytoplankton pigment concentrations during POLARSTERN cruise ANT-XXVII/2

Photophysiological processes as well as uptake characteristics of iron and inorganic carbon were studied in inshore phytoplankton assemblages of the Western Antarctic Peninsula (WAP) and offshore assemblages of the Drake Passage. Chlorophyll a concentrations and primary productivity decreased from in- to offshore waters. The inverse relationship between low maximum quantum yields of photochemistry in PSII (Fv/Fm) and large sizes of functional absorption cross sections (sigma PSII) in offshore communities indicated iron-limitation. Congruently, the negative correlation between Fv/Fm values and iron uptake rates across our sampling locations suggest an overall better iron uptake capacity in iron-limited pelagic phytoplankton communities. Highest iron uptake capacities could be related to relative abundances of the haptophyte Phaeocystis antarctica. As chlorophyll a-specific concentrations of humic-like substances were similarly high in offshore and inshore stations, we suggest humic-like substances may play an important role in iron chemistry in both coastal and pelagic phytoplankton assemblages. Regarding inorganic carbon uptake kinetics, the measured maximum short-term uptake rates (Vmax(CO2)) and apparent half-saturation constants (K1/2(CO2)) did not differ between offshore and inshore phytoplankton. Moreover, Vmax(CO2) and K1/2(CO2) did not exhibit any CO2-dependent trend over the natural pCO2 range from 237 to 507 µatm. K1/2(CO2) strongly varied among the sampled phytoplankton communities, ranging between 3.5 and 35.3 µmol/L CO2. While in many of the sampled phytoplankton communities, the operation of carbon-concentrating mechanisms (CCMs) was indicated by low K1/2(CO2) values relative to ambient CO2 concentrations, some coastal sites exhibited higher values, suggesting down-regulated CCMs. Overall, our results demonstrate a complex interplay between photophysiological processes, iron and carbon uptake of phytoplankton communities of the WAP and the Drake Passage.

Absorption of planar waves in a draining bathtub

We present an analysis of the absorption of acoustic waves by a black hole analogue in (2 + 1) dimensions generated by a fluid flow in a draining bathtub. We show that the low-frequency absorption length is equal to the acoustic hole circumference and that the high-frequency absorption length is 4 times the ergoregion radius. For intermediate values of the wave frequency, we compute the absorption length numerically and show that our results are in excellent agreement with the low-and high-frequency limits. We analyze the occurrence of superradiance, manifested as negative partial absorption lengths for corotating modes at low frequencies.

Experimental and theoretical study of two-photon absorption in nitrofuran derivatives: Promising compounds for photochemotherapy

We report experimental and theoretical studies of the two-photon absorption spectrum of two nitrofuran derivatives: nitrofurantoine, (1-(5-nitro-2-furfurilideneamine)-hidantoine) and quinifuryl, 2-(5`-nitro-2`-furanyl) ethenyl-4-{N-[4`-(N,N-diethylamino)-1`-methylbutyl]carbamoyl} quinoline. Both molecules are representative of a family of 5-nitrofuran-ethenyl-quinoline drugs that have been demonstrated to display high toxicity to various species of transformed cells in the dark. We determine the two-photon absorption cross-section for both compounds, from 560 to 880 nm, which present peak values of 64 GM for quinifuryl and 20 GM for nitrofurantoine (1 GM = 1 x 10(-50) cm(4).s.photon(-1)). Besides, theoretical calculations employing the linear and quadratic response functions were carried out at the density functional theory level to aid the interpretations of the experimental results. The theoretical results yielded oscillator strengths, two-photon transition probabilities, and transition energies, which are in good agreement with the experimental data. A higher number of allowed electronic transitions was identified for quinifuryl in comparison to nitrofurantoine by the theoretical calculations. Due to the planar structure of both compounds, the differences in the two-photon absorption cross-section values are a consequence of their distinct conjugation lengths. (c) 2011 American Institute of Physics. [doi:10.1063/1.3514911]

Theoretical study of one- and two-photon absorption spectra of azoaromatic compounds

In this study, the one- and two-photon absorption spectra of seven azoaromatic compounds (five pseudostilbenes-type and two aminoazobenzenes) were theoretically investigated using the density functional theory combined with the response functions formalism. The equilibrium molecular structure of each compound was obtained at three different levels of theory: Hartree-Fock, density functional theory (DFT), and Moller-Plesset 2. The effect of solvent on the equilibrium structure and the electronic transitions of the compounds were investigated using the polarizable continuum model. For the one-photon absorption, the allowed pi ->pi(*) transition energy showed to be dependent on the molecular structures and the effect of solvent, while the n ->pi(*) and pi ->pi(*)(n) transition energies exhibited only a slight dependence. An inversion between the bands corresponding to the pi ->pi(*) and n ->pi(*) states due to the effect of solvent was observed for the pseudostilbene-type compounds. To characterize the allowed two-photon absorption transitions for azoaromatic compounds, the response functions formalism combined with DFT using the hybrid B3LYP and PBE0 functionals and the long-range corrected CAM-B3LYP functional was employed. The theoretical results support the previous findings based on the three-state model. The model takes into account the ground and two electronic excited states and has already been used to describe and interpret the two-photon absorption spectrum of azoaromatic compounds. The highest energy two-photon allowed transition for the pseudostilbene-type compounds shows to be more effectively affected (similar to 20%) by the torsion of the molecular structure than the lowest allowed transition (similar to 10%). In order to elucidate the effect of the solvent on the two-photon absorption spectra, the lowest allowed two-photon transition (dipolar transition) for each compound was analyzed using a two-state approximation and the polarizable continuum model. The results obtained reveal that the effect of solvent increases drastically the two-photon cross-section of the dipolar transition of the pseudostilbene-type compounds. In general, the features of both one- and two-photon absorption spectra of the azoaromatic compounds are well reproduced by the theoretical calculations.

Cross section of a resonant-mass detector for scalar gravitational waves

Gravitationally coupled scalar fields, originally introduced by Jordan, Brans and Dicke to account for a non-constant gravitational coupling, are a prediction of many non-Einsteinian theories of gravity not excluding perturbative formulations of string theory. In this paper, we compute the cross sections for scattering and absorption of scalar and tensor gravitational waves by a resonant-mass detector in the framework of the Jordan-Brans-Dicke theory. The results are then specialized to the case of a detector of spherical shape and shown to reproduce those obtained in general relativity in a certain limit. Eventually we discuss the potential detectability of scalar waves emitted in a spherically symmetric gravitational collapse.

Molecular effects on the cross section for pair production and their importance in the evaluation of the total photonuclear cross section of {^16}O in the {\delta-resonance} region

The screening correction to the coherent pair-production cross section on the oxygen molecule has been calculated using self-consistent relativistic wave functions for the one-center and two-center Coulomb potentials. It is shown that the modification of the wave function due to molecular binding and the interference between contributions from the two atoms have both sizeable effects on the screening correction. The so-obtained coherent pair-production cross section which makes up the largest part of the total atomic cross section was used to evaluate the total nuclear absorption cross section from photon attenuation measurements on liquid oxygen. The result agrees with cross sections for other nuclei if A-scaling is assumed. The molecular effect on the pair cross section amounts to 15 % of the nuclear cross section in the {\delta-resonance} region.

Degenerate Two-Photon Absorption in All-Trans Retinal: Nonlinear Spectrum and Theoretical Calculations

In this work we investigate the degenerate two-photon absorption spectrum of all-trans retinal ill ethanol employing the Z-scan technique with femtosecond pulses, The two-photon absorption (2PA) spectrum presents a monotonous increase as the excitation wavelength approaches the one-photon absorption band and it peak at 790 nm. We attribute the 2PA hand to the mixing of states (1)B(u)+-like and vertical bar S(1)>, which are strongly allowed by one- and two-photon, respectively. We modeled the 2PA spectrum by using the sum-over-states approach and obtained spectroscopic parameters of the electronic transitions to vertical bar S >, vertical bar S(2)> (""(1)Bu(+)""), vertical bar S(3)>, and vertical bar S(4)> singlet-excited states. The results were compared with theoretical predictions of one- and two-photon transition calculations using the response Functions formalism within the density functional theory framework with the aid of the CAM-B3LYP functional.

Two-photon absorption of perylene derivatives: Interpreting the spectral structure

This work investigates the two-photon absorption spectrum of perylene tetracarboxylic derivatives using the white-light continuum Z-scan technique. Perylene derivatives present relatively high two-photon absorption cross-section, which makes them attractive for applications in photonics. Because of the spectral resolution of the white-light continuum Z-scan, we were able to observe a well defined structure in the two-photon absorption spectrum, composed by two distinct peaks. These peaks, as well as the resonant enhancement of the nonlinearity, were modeled using the sum-over-states approach considering a four-level energy diagram with two final two-photon states. The existence of such states was confirmed using the response function formalism within the DFT framework. (C) 2009 Elsevier B.V. All rights reserved.