Raman Strain-Shift Measurements and Prediction from First-Principles in Highly-Strained Silicon

TL;DR

This paper combines first-principles simulations with experimental Raman measurements to accurately predict strain-induced shifts in silicon's phonon modes, validated up to 2% strain.

Contribution

It introduces a validated first-principles approach for predicting Raman shifts in highly-strained silicon, improving accuracy over existing models.

Findings

Simulated strain-shift coefficients closely match experimental values.

Validated perturbation theory for high-strain conditions.

Quantified uncertainties in phonon deformation potentials.

Abstract

This work presents how first-principles simulations validated through experimental measurements lead to a new accurate prediction of the expected Raman shift as a function of strain in silicon. Structural relaxation of a strained primitive cell is first performed to tackle the relative displacement of the silicon atoms for each strain level. Density Functional Perturbation Theory (DFPT) is then used to compute the energy of the optical phonon modes in highly-strained silicon and retrieve the strain-shift trend. The simulations are validated by experimental characterization, using scanning electron microscopy (SEM) coupled with backscattering Raman spectroscopy, of silicon microbeams fabricated using a top-down approach. The beams are strained up to 2$\%$ thanks to the internal tensile stress of silicon nitride actuators, allowing a validation of the perturbation theory in high-strain conditions. The results are compared with the phonon deformation potentials (PDP) theory and the uncertainty caused by the various parameters found in the literature is discussed. The simulated strain-shift coefficients of -175.77 cm$^{-1}$ (resp. -400.85 cm$^{-1}$) and the experimental one of -160.99 cm$^{-1}$ (resp. -414.97 cm$^{-1}$) are found for the longitudinal optical LO (resp. transverse optical TO$_1$) mode, showing good agreement.