The optical nonlinearity of WS2 and MoS2 monolayer and few-layer films was investigated using the Z-scan technique with femtosecond pulses from the visible to the near-infrared range. The nonlinear absorption of few- and multilayer WS2 and MoS2 films and their dependences on excitation wavelength were studied. WS2 films with 1-3 layers exhibited a giant two-photon absorption (TPA) coefficient as high as (1.0 ± 0.8) × 10(4) cm/GW. TPA saturation was observed for the WS2 film with 1-3 layers and for the MoS2 film with 25-27 layers. The giant nonlinearity of WS2 and MoS2 films is attributed to a two-dimensional confinement, a giant exciton effect, and the band edge resonance of TPA.

Abstract-Compressed Sensing suggests that the required number of samples for reconstructing a signal can be greatly reduced if it is sparse in a known discrete basis, yet many real-world signals are sparse in a continuous dictionary. One example is the spectrally-sparse signal, which is composed of a small number of spectral atoms with arbitrary frequencies on the unit interval. In this paper we study the problem of line spectrum denoising and estimation with an ensemble of spectrally-sparse signals composed of the same set of continuous-valued frequencies from their partial and noisy observations. Two approaches are developed based on atomic norm minimization and structured covariance estimation, both of which can be solved efficiently via semidefinite programming. The first approach aims to estimate and denoise the set of signals from their partial and noisy observations via atomic norm minimization, and recover the frequencies via examining the dual polynomial of the convex program. We characterize the optimality condition of the proposed algorithm and derive the expected convergence rate for denoising, demonstrating the benefit of including multiple measurement vectors. The second approach aims to recover the population covariance matrix from the partially observed sample covariance matrix by motivating its low-rank Toeplitz structure without recovering the signal ensemble. Performance guarantee is derived with a finite number of measurement vectors. The frequencies can be recovered via conventional spectrum estimation methods such as MUSIC from the estimated covariance matrix. Finally, numerical examples are provided to validate the favorable performance of the proposed algorithms, with comparisons against several existing approaches.

Nonlinear optical property of transition metal dichalcogenide (TMDC) nanosheet dispersions, including MoS2, MoSe2, WS2, and WSe2, was performed by using Z-scan technique with ns pulsed laser at 1064 nm and 532 nm. The results demonstrate that the TMDC dispersions exhibit significant optical limiting response at 1064 nm due to nonlinear scattering, in contrast to the combined effect of both saturable absorption and nonlinear scattering at 532 nm. Selenium compounds show better optical limiting performance than that of the sulfides in the near infrared. A liquid dispersion system based theoretical modelling is proposed to estimate the number density of the nanosheet dispersions, the relationship between incident laser fluence and the size of the laser generated micro-bubbles, and hence the Mie scattering-induced broadband optical limiting behavior in the TMDC dispersions.

An in-depth knowledge of the interaction of water with amorphous silica is critical to fundamental studies of interfacial hydration water, as well as to industrial processes such as catalysis, nanofabrication, and chromatography. Silica has a tunable surface comprising hydrophilic silanol groups and moderately hydrophobic siloxane groups that can be interchanged through thermal and chemical treatments. Despite extensive studies of silica surfaces, the influence of surface hydrophilicity and chemical topology on the molecular properties of interfacial water is not well understood. In this work, we controllably altered the surface silanol density, and measured surface water diffusivity using Overhauser dynamic nuclear polarization (ODNP) and complementary silica-silica interaction forces across water using a surface forces apparatus (SFA). The results show that increased silanol density generally leads to slower water diffusivity and stronger silica-silica repulsion at short aqueous separations (less than ∼4 nm). Both techniques show sharp changes in hydration properties at intermediate silanol densities (2.0-2.9 nm). Molecular dynamics simulations of model silica-water interfaces corroborate the increase in water diffusivity with silanol density, and furthermore show that even on a smooth and crystalline surface at a fixed silanol density, adjusting the spatial distribution of silanols results in a range of surface water diffusivities spanning ∼10%. We speculate that a critical silanol cluster size or connectivity parameter could explain the sharp transition in our results, and can modulate wettability, colloidal interactions, and surface reactions, and thus is a phenomenon worth further investigation on silica and chemically heterogeneous surfaces.

cm/GW, larger than that of conventional semiconductors by a factor of 10 3 . As a result of TPA, two-photon pumped frequency up-converted luminescence is observed directly in the monolayer MoS2. For the multilayer MoS2, the SA response is demonstrated with the ratio of the excited-state absorption cross section to ground-state cross section of ∼0.18. In addition, the laser damage threshold of the monolayer MoS2 is ∼ 97 GW/cm 2 , larger than that of the multilayer MoS2 of ∼78 GW/cm 2 .2

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The saturation of two-photon absorption (TPA) in four types of layered transition metal dichalcogenides (TMDCs) (MoS 2 , WS 2 , MoSe 2 , WSe 2 ) was systemically studied both experimentally and theoretically. It was demonstrated that the TPA coefficient is decreased when either the incident pulse intensity or the thickness of the TMDC nanofilms increases, while TPA saturation intensity has the opposite behavior, under the excitation of 1.2 eV photons with a pulse width of 350 fs. A three-level excitonic dynamics simulation indicates that the fast relaxation of the excitonic dark states, the exciton−exciton annihilation, and the depletion of electrons in the ground state contribute significantly to TPA saturation in TMDC nanofilms. Large third-order nonlinear optical responses make these layered 2D semiconductors strong candidate materials for optical modulation and other photonic applications.

Composite Ni-YSZ fuel electrodes are able to operate only under strongly reducing conditions for the electrolysis of CO(2) in oxygen-ion conducting solid oxide electrolysers. In an atmosphere without a flow of reducing gas (i.e., carbon monoxide), a composite fuel electrode based on redox-reversible La(0.2)Sr(0.8)TiO(3+δ) (LSTO) provides a promising alternative. The Ti(3+) was approximately 0.3% in the oxidized LSTO (La(0.2)Sr(0.8)TiO(3.1)), whereas the Ti(3+) reached approximately 8.0% in the reduced sample (La(0.2)Sr(0.8)TiO(3.06)). The strong adsorption of atmospheric oxygen in the form of superoxide ions led to the absence of Ti(3+) either on the surface of oxidized LSTO or the reduced sample. Reduced LSTO showed typical metallic behaviour from 50 to 700 °C in wet H(2); and the electrical conductivity of LSTO reached approximately 30 S cm(-1) at 700 °C. The dependence of [Ti(3+)] concentration in LSTO on P(O(2)) was correlated to the applied potentials when the electrolysis of CO(2) was performed with the LSTO composite electrode. The electrochemical reduction of La(0.2)Sr(0.8)TiO(3+δ) was the main process but was still present up to 2 V at 700 °C during the electrolysis of CO(2); however, the electrolysis of CO(2) at the fuel electrode became dominant at high applied voltages. The current efficiency was approximately 36% for the electrolysis of CO(2) at 700 °C and a 2 V applied potential.