FROG: Exploiting all-atom molecular dynamics trajectories to calculate linear and non-linear optical responses of molecular liquids within Dalton's QM/MM polarizable embedding scheme.

Quantum mechanical/molecular mechanics (QM/MM) methods are interesting to model the impact of a complex environment on the spectroscopic properties of a molecule. In this context, a FROm molecular dynamics to second harmonic Generation (FROG) code is a tool to exploit molecular dynamics trajectories to perform QM/MM calculations of molecular optical properties. FROG stands for "FROm molecular dynamics to second harmonic Generation" since it was developed for the calculations of hyperpolarizabilities.

Liquid Water: When Hyperpolarizability Fluctuations Boost and Reshape the Second Harmonic Scattering Intensities.

Second harmonic scattering (SHS) is a method of choice to investigate the molecular structure of liquids. While a clear interpretation of SHS intensity exists for diluted solutions of dyes, the scattering due to solvents remains difficult to interpret quantitatively. Here, we report a quantum mechanics/molecular mechanics (QM/MM) approach to model the polarization-resolved SHS intensity of liquid water, quantifying different contributions to the signal.

First hyperpolarizability of water in bulk liquid phase: long-range electrostatic effects included the second hyperpolarizability.

The molecular first hyperpolarizability contributes to second-order optical non-linear signals collected from molecular liquids. For the Second Harmonic Generation (SHG) response, the first hyperpolarizability (2, , ) often depends on the molecular electrostatic environment. This is especially true for water, due to its large second hyperpolarizability (2, , ,0).

First hyperpolarizability of water at the air-vapor interface: a QM/MM study questions standard experimental approximations.

Surface Second-Harmonic Generation (S-SHG) experiments provide a unique approach to probe interfaces. One important issue for S-SHG is how to interpret the S-SHG intensities at the molecular level. Established frameworks commonly assume that each molecule emits light according to an average molecular hyperpolarizability tensor (-2,,).

Electrokinetic sweeping of colloids at a reactive magnesium oxide interface.

Investigating the electrokinetic (EK) response in the vicinity of interfaces has regained interest due to the development of new membrane based processes for energy harvesting or soil depollution. However, the case of reactive interfaces, ubiquitous in these processes, remains scarcely explored. Here we experimentally investigate the EK response of a model interface between an aqueous electrolyte and a bulk MgO crystal surface (100), for different pH.

Longitudinal position dependence of the second-harmonic generation of optically trapped silica microspheres.

We report the design of a setup combining the simultaneous and independent optical trapping and second-harmonic generation (SHG) of 1 µm diameter silica microspheres with two independent laser beams. Optical trapping is achieved with a tightly focused continuous wave infrared laser beam whereas the SHG intensity from the trapped microparticles is obtained with a 810 nm femtosecond pulsed laser. The silica microparticles are dispersed in an aqueous solution, and a microfluidic channel flow is used to remove untrapped microparticles.

Electroosmosis near surfactant laden liquid-air interfaces.

Generation of an electroosmostic (EO) flow near a liquid-gas interface covered with ionic surfactants is experimentally investigated. A combination of microscopic flow measurements with a molecular characterization of the interface by second harmonic generation (SHG) shows that under an electrical forcing, although a liquid flow is generated below the free surface, the surfactants remain immobile. The zeta potential was then determined and compared to the surfactant surface coverage.

Electrokinetic transport in liquid foams.

Investigating electrokinetic transport in a liquid foam is at the confluence of two well developed research areas. On one hand, the study of electrokinetic flows (i.e.

Surface conductivity measurements in nanometric to micrometric foam films.

Foam films (a liquid lamella in air covered by surfactants) are tools of choice for nanofluidic characterization as they are intrinsically nanometric. Their size is indeed fixed by a balance between external pressure and particular molecular interactions in the vicinity of interfaces. To probe the exact nature of these interfaces, different characterizations can be performed.

Osteoid Osteoma with a Multicentric Nidus: Interstitial Laser Ablation under MRI Guidance.

Osteoid osteoma (OO) is a common benign tumor of the bone and is typically treated by thermal ablation with computed tomography (CT) guidance. Only a few cases of multicentric OO have been described. We here report the case of an 11-year-old boy with multicentric OO of the right femur treated with laser ablation under open high-field MRI guidance.

Soft nanofluidic transport in a soap film.

We investigate experimentally the electrokinetic properties of soft nanofluidic channels that consist in soap films with nanometric thickness, covered with charged surfactants. Both the electric and fluidic responses of the system are measured under an applied voltage drop along the film. The electric field is shown to induce an electro-osmotic hydrodynamic flow in the film.

Elastic instability in stratified core annular flow.

We study experimentally the interfacial instability between a layer of dilute polymer solution and water flowing in a thin capillary. The use of microfluidic devices allows us to observe and quantify in great detail the features of the flow. At low velocities, the flow takes the form of a straight jet, while at high velocities, steady or advected wavy jets are produced.