Excitons dominate the light absorption and re-emission spectra of monolayer transition-metal dichalcogenides (TMD). Microscopic investigations of the excitonic response in TMD almost invariably extract information from the radiative recombination step, which only constitutes one part of the picture. Here, by exploiting imaging spectroscopic ellipsometry (ISE), we investigate the spatial dependence of the dielectric function of chemical vapor deposition (CVD)-grown WS2 flakes with a microscopic lateral resolution, thus providing information about the spatially varying, exciton-induced light absorption in the monolayer WS2. Comparing the ISE results with imaging photoluminescence spectroscopy data, the presence of several correlated features was observed, along with the unexpected existence of a few uncorrelated characteristics. The latter demonstrates that the exciton-induced absorption and emission features are not always proportional at the microscopic scale. Microstructural modulations across the flakes, having a different influence on the absorption and re-emission of light, are deemed responsible for the effect.
The interaction of ultrashort pulsed laser radiation with intensities of 1013 W cm−2 and above with materials often results in an unexpected high X-ray photon flux. It has been shown so far, on the one hand, that X-ray photon emissions increase proportionally with higher laser power and the accumulated X-ray dose rates can cause serious health risks for the laser operators. On the other hand, there is clear evidence that little variations of the operational conditions can considerably affect the spectral X-ray photon flux and X-ray emissions dose. In order to enhance the knowledge in this field, four ultrashort pulse laser systems for providing different complementary beam characteristics were employed in this study on laser-induced X-ray emissions, including peak intensities between 8 × 1012 W∙cm−2 < I0 < 5.2 × 1016 W∙cm−2, up to 72.2 W average laser power as well as burst/bi-burst processing mode. By the example of AISI 304 stainless steel, it was verified that X-ray emission dose rates as high as > 45 mSv h−1 can be produced when low-intensity ultrashort pulses irradiate at a small 1 µm intra-line pulse distance during laser beam scanning and megahertz pulse repetition frequencies. For burst and bi-burst pulses, the second intra-burst pulse was found to significantly enhance the X-ray emission potentially induced by laser pulse and plasma interaction.
3 August 2021 in The Journal of Physical Chemistry C
We demonstrate micrometer-resolved imaging of the transient dielectric function of a c-ZnO thin film with femtosecond resolution in the visible to near-IR spectral range measured by pump-probe ellipsometry at five different probe photon-energies. The spatial profile of the real part of the dielectric function broadens drastically with increasing time delay, which we associate with the combined effect of carrier cooling and fast carrier transport with an effective diffusion coefficient of cm2/s. A ring structure is detected in the image after a few picoseconds, which can be explained by a random-walk model including ballistic transport due to the thermal gradient induced by the hot-phonon effect.
Laser ablation of dielectrics by ultrashort pulsed laser radiation is induced by nonlinear photoexcitation, such as multiphoton and tunneling processes, and the subsequent impact excitation, due to electron-electron collisions. Previous theoretical and experimental studies demonstrate that these two phenomena strongly depend on the transient optical properties of the dielectric and the electron-electron collision times. To estimate these transient optical properties and the collision time, the excited electrons are usually considered as a nearly free-electron gas, being described by the Drude theory. All previous experimental studies support using the Drude theory by time-resolved measurements of the transient reflectance during and after irradiation. However, a comprehensive characterization of the transient complex refractive index, and, thus, a more complex view of the optical properties upon irradiation above the ablation threshold fluence was still missing. Therefore, this paper presents the time-, spectral-, and fluence-resolved complex refractive index of fused silica during the interaction with ultrashort pulsed laser radiation (800 nm, 40 fs, and 4.4 J/) measured by spectroscopic imaging pump-probe ellipsometry. Comparing the state-of-the-art Drude model to the experimental data reveals that, although the Drude model replicates the transient reflectance of the material, it deviates significantly from the transient refractive index in the considered temporal range up to 200 fs after irradiation. Thus, the Drude model cannot correctly describe the transient optical properties, which leads to the assumption that the electrons cannot be considered as a nearly free-electron gas at this time. Alternatively, a Lorentz model, considering the excited electrons as bound, can replicate the measured data much better, which indicates that the electrons might be excited into localized states.