ABSTRACT
Phase-pure, highly crystalline sub-50 nm LiNbO3 nanocrystals were prepared from a non-aqueous solvothermal process for 72 h at 230 °C and a commercial precursor solution of mixed lithium niobium ethoxide in its parent alcohol. A systematic variation of the reaction medium composition with the addition of different amounts of co-solvent including butanol, 1,3-propanediol, 1,4-butanediol, and 1,5-pentanediol resulted in the formation of nanocrystals of adjustable mean size and shape anisotropy, as demonstrated from XRD measurements and TEM imaging. Colloidal stability of ethanol- and water-based suspensions was evaluated from dynamic light scattering (DLS)/zeta potential studies and correlated with FTIR data. Thanks to the evolution in the nanocrystal size and shape distribution we observed, as well as to the available literature on the alkoxide chemistry, the reaction pathways and growth mechanisms were finally discussed with a special attention on the monomer formation rate, leading to the nucleation step. The polar, non-perovskite crystalline structure of LiNbO3 was also evidenced to play a major role in the nanocrystal shape anisotropy.
ABSTRACT
Hyper Rayleigh scattering (HRS) was used to measure the second-order nonlinear susceptibility, χ(2), for liquid exfoliated WS2 monolayers. To the best of our knowledge, it is the first reported application of the HRS technique to assess the bulk-like χ(2) of a two-dimensional (2D) material. The concentration-dependent HRS signal indicated a 4.90±0.30×10-25 esu first hyperpolarizability for 42 nm WS2 monolayers under 1064 nm laser irradiation using para-nitroaniline as an external reference. The corresponding value of χxxx(2) was calculated to be 460±28 pm V-1. This was within 46% of independent density functional theory predictions. Agreement with theory was improved over related microscopy-based approaches. These results support the use of HRS to evaluate 2D materials for nonlinear frequency mixing applications.
ABSTRACT
We use Hyper Rayleigh Scattering and polarization resolved multiphoton microscopy to investigate simultaneously the second and third-order nonlinear response of Potassium Niobate and Bismuth Ferrite harmonic nanoparticles. We first derive the second-to-third harmonic intensity ratio for colloidal ensembles and estimate the average third-order efficiency of these two materials. Successively, we explore the orientation dependent tensorial response of individual nanoparticles fixed on a substrate. The multi-order polarization resolved emission curves are globally fitted with an analytical model to retrieve individual elements of susceptibility tensors.
