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Synthesis, nanocrystalline morphology, lattice dynamics and nonlinear optics of mesoporous SiO2&LiNbO3 nanocomposite
Citation Link: https://doi.org/10.15480/882.13609
Publikationstyp
Journal Article
Date Issued
2024-10-16
Sprache
English
TORE-DOI
Journal
Volume
14
Issue
1
Article Number
24237
Citation
Scientific Reports 14 (1): 24237 (2024)
Publisher DOI
Scopus ID
Publisher
Springer Nature
We demonstrate a hybrid nanocomposite combining mesoporous silica, pSiO2, as a host medium and guest lithium niobate LiNbO3 nanocrystals embedded into tubular silica nanochannels by calcination of the precursor mixed solution of lithium and niobium salts. High-resolution transmission electron microscopy, X-ray diffraction and Raman scattering techniques reveal trigonal LiNbO3 nanocrystals within the pSiO2 nanochannels, indicating their random texture morphology. Annealing at high temperatures (950∘C) during calcination also leads to partial crystallization of the pSiO2 matrix with the formation of trigonal α-SiO2 nanocrystals. The Raman microscopy analysis of the pSiO2:LiNbO3 nanocomposite reveals three structural crystalline phases, α-SiO2, LiNbO3 and a mixed phase which involves the α-SiO2 phase of host membrane and LiNbO3 nanocrystals embedded into the membrane. The finite size of the LiNbO3 nanocrystals results in specific features of the LO-TO phonon frequency splitting, which are investigated by Raman microscopy. In the transmission geometry, the second harmonic generation emission exhibits no Maker fringes and is characterized by a broad angular diagram of diffusely scattered light. The second harmonic generation response is independent of the polarization direction of the incident pump light, thus indicating a spatial isotropy of the nonlinear optical conversion in the pSiO2:LiNbO3 composite, consistent with the randomly oriented textural morphology of the deposited LiNbO3 nanocrystals. The contribution of the guest LiNbO3 nanocrystals to the second harmonic generation effect was found to be strongly dominant compared to the partially crystallized host pSiO2 matrix. The nanocomposite pSiO2:LiNbO3 membrane, set in the 90∘ nonlinear optical geometry, shows unusually high diffusely transmitted second harmonic generation light (back-reflected emission), apparently supported by internal light reflection from the tubular nanochannel network. Despite the fundamental interest, the revealed anomalous back-reflected second harmonic generation emission from pSiO2:LiNbO3 nanocomposite membranes expands the prospects for their photonic and nonlinear optical applications.
DDC Class
620.1: Engineering Mechanics and Materials Science
540: Chemistry
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