We report on the lattice strain dependence of the nonlinear optical (NLO) parameters of strained Si nanoparticles (NPs), which are prepared in a controlled way by a mechanical ball milling process. X-ray diffraction analysis shows that the nature of strain is compressive and is primarily caused by milling-induced lattice dislocations, which is further supported by high-resolution transmission electron microscopy imaging. It is found that the nonlinear refractive index () and nonlinear absorption coefficient () are strongly influenced by the associated lattice strain present in Si NPs. With the increase of lattice strain, the gradually decreases while increases slowly. The strain-dependent observed changes in the NLO parameters of Si NPs are found to be advantageous for application purpose, and it is explained on the basis of strain-induced modification in the electronic structure of the highest occupied molecular orbital and lowest unoccupied molecular orbital states of Si NPs. These results demonstrate the potential of strain-dependent enhancement of nonlinearities for silicon photonics applications.
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