Influence of the temperature-dependent dielectric constant on the photoacoustic effect of gold nanospheres.

Photoacoustic imaging techniques with gold nanoparticles as contrast agents have received a great deal of attention. The photoacoustic response of gold nanoparticles strongly depends on the far-field optical properties, which essentially depend on the dielectric constant of the material. The dielectric constant of gold not only varies with wavelength but is also affected by temperature. However, the effect of the temperature dependence of the dielectric constant on gold nanoparticles' photoacoustic response has not been fully investigated. In this work, the Drude-Lorentz model and Mie theory are used to calculate the dielectric constant and absorption efficiency of gold nanospheres in aqueous solution, respectively. Then, the finite element method is used to simulate the heat transfer process of gold nanospheres and surrounding water. Finally, the one-dimensional velocity-stress equation is solved by the finite-difference time-domain method to obtain the photoacoustic response of gold nanospheres. The results show that under the irradiation of a high-fluence nanosecond pulse laser, ignoring the temperature dependence of the dielectric constant will lead to large errors in the photothermal response and the nonlinear photoacoustic signals (it can even exceed 20% and 30%). The relative error of the photothermal and photoacoustic response caused by ignoring the temperature-dependent dielectric constant is determined from both the temperature dependence of absorption efficiency and the maximum temperature increase of gold nanospheres. This work provides a new perspective for the photothermal and photoacoustic effects of gold nanospheres, which is meaningful for the development of high-resolution photoacoustic detectors and nano/microscale temperature measurement techniques.

Simultaneous determination of primary particle size distribution and thermal accommodation coefficient of soot aggregates using low-fluence LII.

For the ill-posed inverse problem of LII-based nanoparticle size measurement, recovered primary particle size distribution (PPSD) is sensitive to the uncertainty of LII model parameters. In the absence of reliable prior knowledge, the thermal accommodation coefficient (TAC) and fractal-dependent shielding factor are often required to be inferred simultaneously with the PPSD. In the simplified LII model for low fluence regime, TAC and fractal-dependent shielding factor are combined to define a new fractal-dependent TAC. The present study theoretically verified the feasibility of inferring PPSD and fractal-dependent TAC from the normalized LII signals. Moreover, the inversion is independent of prior knowledge of most full LII model parameters, which is attributed to low laser fluence, normalized signal, and fractal-dependent TAC.

Retrieval of fractal dimension and size distribution of non-compact soot aggregates from relative intensities of multi-wavelength angular-resolved light scattering.

A new technique is developed to retrieve the fractal dimension and size distribution of soot aggregates simultaneously from the relative intensities of multi-wavelength angular-resolved light scattering. Compared with other techniques, the main advantage of this method is its independence of knowing complex refractive index, number density of aggregate, fractal prefactor and primary particle diameter. The forward light scattering procedure of soot aggregate is described by Rayleigh-Debye-Gans polydisperse fractal aggregate (RDG-PFA) scattering theory, and the retrieval process is performed by using the covariance matrix adaption-evolution strategy algorithm (CMA-ES). Three different measurement models, i.e. absolute scattering and transmittance, absolute scattering, relative scattering (RS), are investigated in present research. Numerical experiments have been performed to test the feasibility of the CMA-ES algorithm. Combined with the multi-wavelength RDG-PFA strategy, the retrieval accuracy of soot aggregate size distribution is proved to be more effectively by using the RS model. Satisfactory results under 10% Gaussian measurement noise have demonstrated the feasibility of the proposed method.

Dependence of the Nonlinear Photoacoustic Response of Gold Nanoparticles on the Heat-Transfer Process.

Photoacoustic (PA) imaging using the nonlinear PA response of gold nanoparticles (GNPs) can effectively attenuate the interference from background noise caused by biomolecules (e.g., hemoglobin), thus offering a highly potential noninvasive biomedical imaging method. However, the mechanism of the nonlinear PA response of GNPs based on the thermal expansion mechanism, especially the effect of heat-transfer ability, still lacks quantitative investigation. Therefore, this work investigated the effect of heat-transfer ability on the nonlinear PA response of GNPs using the critical energy and fluence concept, taking into account the Au@SiO2 core-shell nanoparticles (weakened heat transfer) and gold nanochains (enhanced heat transfer). The results showed that the stronger the heat transferability, the smaller the critical energy, indicating that the nonlinear PA response of different nanoparticles cannot be contrasted directly through the critical energy. Moreover, the critical fluence can directly contrast the proportion of nonlinear components in the PA response of different GNPs as governed by the combined effect of heat transferability and photothermal conversion ability.