Direct measurement of quantum phases in graphene via photoemission spectroscopy

Quantum phases provide us with important information for understanding the fundamental properties of a system. However, the observation of quantum phases, such as Berry's phase and the sign of the matrix element of the Hamiltonian between two non-equivalent localized orbitals in a tight-binding formalism, has been challenged by the presence of other factors, e.g., dynamic phases and spin/valley degeneracy, and the absence of methodology. Here, we report a new way to directly access these quantum phases, through polarization-dependent angle-resolved photoemission spectroscopy (ARPES), using graphene as a prototypical two-dimensional material. We show that the momentum- and polarization-dependent spectral intensity provides direct measurements of (i) the phase of the band wavefunction and (ii) the sign of matrix elements for non-equivalent orbitals. Upon rotating light polarization by \pi/2, we found that graphene with a Berry's phase of n\pi (n=1 for single- and n=2 for double-layer graphene for Bloch wavefunction in the commonly used form) exhibits the rotation of ARPES intensity by \pi/n, and that ARPES signals reveal the signs of the matrix elements in both single- and double-layer graphene. The method provides a new technique to directly extract fundamental quantum electronic information on a variety of materials.