Uniaxial strain in graphene by Raman spectroscopy: G peak splitting, Grüneisen parameters, and sample orientation

Graphene is the two-dimensional building block for carbon allotropes of every other dimensionality. Since its experimental discovery, graphene continues to attract enormous interest, in particular as a new kind of matter, in which electron transport is governed by a Dirac-like wave equation, and as a model system for studying electronic and phonon properties of other, more complex, graphitic materials[1-4]. Here, we uncover the constitutive relation of graphene and probe new physics of its optical phonons, by studying its Raman spectrum as a function of uniaxial strain. We find that the doubly degenerate E2g optical mode splits in two components, one polarized along the strain and the other perpendicular to it. This leads to the splitting of the G peak into two bands, which we call G+ and G-, by analogy with the effect of curvature on the nanotube G peak[5-7]. Both peaks red shift with increasing strain, and their splitting increases, in excellent agreement with first-principles calculations. Their relative intensities are found to depend on light polarization, which provides a useful tool to probe the graphene crystallographic orientation with respect to the strain. The singly degenerate 2D and 2D' bands also red shift, but do not split for small strains. We study the Gruneisen parameters for the phonons responsible for the G, D and D' peaks. These can be used to measure the amount of uniaxial or biaxial strain, providing a fundamental tool for nanoelectronics, where strain monitoring is of paramount importance[8, 9]