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Laser-induced wavefront distortion is detectable by several techniques based on the photothermal effect. The effect is probed by monitoring the phase shift caused by the bulging of the heated area, the photoelastic effects, and the spatial distribution of the refractive index within the sample and in the fluid surrounding it. A simple analytical solution for the wavefront distortion was only possible for low absorbing materials, with the assumption that the stresses obey either the thin-disk or the long-rod type distributions. Recently, a unified theoretical description for the laser-induced optical path change was proposed to overcome part of this limitation for weakly absorbing materials, regardless of its thickness. In this work, we perform an experimental investigation taking the sample-fluid heat coupling effect into account using the thermal lens technique. The experimental investigation presented here validates the unified model. In addition, we show that the heat-coupling model provides an alternative method to obtain physical properties of non-absorbing fluid by using a reference solid sample.

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Recent improvements in the modeling of photo-induced thermo-optical-mechanical effects have broadened the application of photothermal techniques to a large class of solids and fluids. During laser excitation, changes in optical reflectivity due to temperature variation may affect the photothermal signal. In this study, the influence of the reflectivity change due to heating is analyzed for two pump-probe photothermal techniques, thermal lens and thermal mirror. A linear equation for the temperature dependence of the reflectivity is derived, and the solution is tested using optical properties of semi-transparent and opaque materials. For semi-transparent materials, the influence of the reflectivity change in photothermal signals is less than 0.01%, while for opaque materials it is lower than 3%.

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Emissions of gases from agricultural and animal feeding operations contribute to climate change, produce odors, degrade sensitive ecosystems, and pose a threat to public health. The complexity of processes and environmental variables affecting these emissions complicate accurate and reliable quantification of gas fluxes and production rates. Although a plethora of measurement technologies exist, each method has its limitations that exacerbate accurate quantification of gas fluxes. Despite a growing interest in gas emission measurements, only a few available technologies include real-time, continuous monitoring capabilities. Commonly applied state-of-the-art measurement frameworks and technologies were critically examined and discussed, and recommendations for future research to address real-time monitoring requirements for forthcoming regulation and management needs are provided.

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The effect of radiation forces at the interface between dielectric materials has been a long-standing debate for over a century. Yet there has been so far only limited experimental verification in complete accordance with the theory. Here we measure the surface deformation at the air-water interface induced by continuous and pulsed laser excitation and match this to rigorous theory of radiation forces. We demonstrate that the experimental results are quantitatively described by the numerical calculations of radiation forces. The Helmholtz force is used for the surface radiation pressure. The resulting surface pressure obtained is consistent with the momentum conservation using the Minkowski momentum density expression assuming that the averaged momentum per photon is given by the Minkowski momentum. Considering the total momentum as a sum of that propagating with the electromagnetic wave and that deposited locally in the material, the Abraham momentum interpretation also appears to be appropriate.

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We propose a combined thermal lens and thermal mirror method as concurrent photothermal techniques for the physical characterization of polymers. This combined method is used to investigate polymers as a function of temperature from room temperature up to 170 °C. The method permits a direct determination of thermal diffusivity and thermal conductivity. Additional measurements of specific heat, linear thermal expansion, and temperature-dependent optical path change are also performed. A complete set of thermal, optical, and mechanical properties of polycarbonate and poly (methyl methacrylate) samples are obtained. Methods presented here can be useful for in situ characterization of semitransparent materials, where fast and non-contacting measurements are required.

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A theoretical model for a time-resolved photothermal mirror technique using pulsed-laser excitation was developed for low absorption samples. Analytical solutions to the temperature and thermoelastic deformation equations are found for three characteristic pulse profiles and are compared to finite element analysis methods results for finite samples. An analytical expression for the intensity of the center of a continuous probe laser at the detector plane is derived using the Fresnel diffraction theory, which allows modeling of experimental results. Experiments are performed in optical glasses, and the models are fitted to the data. The parameters of the fit are in good agreement with previous literature data for absorption, thermal diffusion, and thermal expansion of the materials tested. The combined modeling and experimental techniques are shown to be useful for quantitative determination of the physical properties of low absorption homogeneous linear elastic material samples.

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A theoretical and experimental study taking sample-fluid heat coupling into account in time-resolved photothermal mirror experiments is presented. Thermoelastic equations were solved to obtain a semi-analytical solution to the phase shift induced by the sample and the surrounding fluid. The solution was used to model the thermal mirror effects and found to be in excellent agreement with the finite element method analysis and experiment. Heat transferred to the air-coupling fluid did not introduce important effects in the phase shift when compared with the solution obtained, without considering heat flux. However, when using water as the fluid, heat coupling led to a significant effect in fluid phase shift. Experimental results using stainless steel in air and water were used to demonstrate the potentiality of the thermal mirror technique to determine the thermal properties of both the sample and the fluid.

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This work presents a theoretical study of a heat transfer effect, taking into account the heat transfer within the heated sample and out to the surrounding medium. The analytical solution is used to model the thermal lens and thermal mirror effects and the results are compared with the finite element analysis (FEA) software solution. The FEA modeling results were found to be in excellent agreement with the analytical solutions. Our results also show that the heat transfer between the sample surface and the air coupling fluid does not introduce an important effect over the induced phase shift in the sample when compared to the solution obtained without considering axial heat flux. On the other hand, the thermal lens created in the air coupling fluid has a significant effect on the predicted time-dependent photothermal signals. When water is used as fluid, the heat coupling leads to a more significant effect in both sample and fluid phase shift. Our results could be used to obtain physical properties of low optical absorption fluids by using a reference solid sample in both thermal lens and thermal mirror experiments.

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Experimental results for photothermal lens measurements are compared to finite elemental analysis models for commercial colored glass filters. Finite elemental analysis software is used to model the photothermal effect by simulating the coupling of heat both within the sample and out to the surroundings. Modeling shows that heat transfer between the glass surface and the air coupling fluid has a significant effect on the predicted time-dependent photothermal lens signals. For comparison with experimental signals, a simple equation based on the finite element analysis result is proposed for accounting for the variance of experimental data where this type of heat coupling situation occurs. The colored glass filters are found to have positive thermo-optical coefficients. The net positive dn/dT of CdSxSe(1-x) doped glass filters is considered to be the consequence of counteracting factors: optical nonlinearity, stress-induced birefringence, and the structural network of glass. Finite element analysis modeling results are also used to correlate experimental measurements of different sample geometries. In particular, the glass samples are compared to ethanol solutions of iron (II) dicylopentadiene in a sample cuvette even though heat transfer is different for these two samples.

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A finite element analysis method for numerical modeling of the photothermal deflection spectroscopy of aerosols is presented. The models simulate pulse-laser excited photothermal deflection from aerosols collected on a plane surface substrate in air medium. The influence of the aerosol and substrate properties on the transient photothermal deflection signal is examined. We have previously obtained experimental results for photothermal deflection spectrometry of aerosols deposited onto a plate from an impactor system (O. O. Dada and S. E. Bialkowski, Appl. Spectrosc. 62, 1336 (2008)). This paper supports the validity of the experimental results presented in that paper and helps in answering some of the questions raised. The modeling results presented here demonstrate that the (peak) normalized transient temperature change profile and (peak) normalized transient photothermal deflection profile are a good approximation and invariant with number of particles, inter-particle distance, and particulate shape, which suggests that the photothermal deflection signal amplitude may be calibrated linearly with total mass of aerosols and the method could be applied to analysis of complex aerosols.

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The potential of mid-infrared photothermal deflection spectrometry for aerosol analysis is demonstrated. Ammonium nitrate aerosols are deposited on a flat substrate using a micro-orifice uniform deposit impactor (MOUDI). Photothermal spectroscopy with optical beam deflection (mirage effect) is used to detect deposited aerosols. Photothermal deflection from aerosols is measured by using pulsed infrared laser light to heat up aerosols collected on the substrate. The deflection signal is obtained by measuring the position of a spot from a beam of light as it passes near the heated surface. The results indicate non-rotating impaction as the preferred MOUDI impaction method. Energy-dependent photothermal measurement shows a linear relationship between signal and laser intensity, and no loss of signal with time is observed. The detection limit from the signal-mass curve is 7.31 ng. For 30 minutes collection time and 30 L/min flow rate of the impactor, the limit of detection in terms of aerosol mass concentration is 0.65 microg m(-3).

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Photothermal lens measurements and finite element modeling are used to examine the physical changes taking place in optical filter glasses. Colored glass and neutral density filters are found to have a strong positive temperature-dependent refractive index change. The overall positive refractive index change is thought to be a consequence of complex counteracting factors: stress-induced birefringence, polarizability, structural network, and temperature-dependent carrier density changes in the CdSxSe1-x microcrystals that produce optical properties of these glasses. Finite element analysis (FEA) modeling is used to examine the temperature profiles and the goodness of the semi-infinite thermal diffusion solution normally used for thermal lens experiments. The results of FEA were used to optimize experimental parameters and calculate values of dn/dT for the glass by comparison with standard liquid samples.

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This paper examines the solutions of kinetic rate equations for prediction of the photothermal lens signals under irradiance conditions that can lead to optical saturation or bleaching. The relaxation kinetics resulting from forcing excited state populations in multiple levels by high excitation irradiance continuous lasers is examined and irradiance-dependent photothermal lens signals are predicted. The analyses described in this paper are based on simple kinetic models for optical excitation and subsequent excited state relaxation. Dark-state relaxation is assumed to be extremely fast compared to limiting kinetics resulting in simplified excited state models. Kinetic models are derived for two, four and five active level molecular systems. Gaussian laser beam profiles are assumed and time dependent photothermal lens signals are calculated. Models account for excitation laser profile, thermal relaxation of the spatially and temporally distorted heating rate distribution resulting from nonlinear absorption, and metastable state relaxation. This heating rate is used to calculate the temperature change distribution and subsequently the optical elements needed to model the experimental photothermal signals.