We present a microscopic explanation of the controversially discussed transient negative differential transmission observed in degenerate optical pump-probe measurements in graphene. Our approach is based on the density matrix formalism allowing a ti
me- and momentum-resolved study of carrier-light, carrier-carrier, and carrier-phonon interaction on microscopic footing. We show that phonon-assisted optical intraband transitions give rise to transient absorption in the optically excited hot carrier system counteracting pure absorption bleaching of interband transitions. While interband transition bleaching is relevant in the first hundreds of fs after the excitation, intraband absorption sets in at later times. In particular, in the low excitation regime, these intraband absorption processes prevail over the absorption bleaching resulting in a zero-crossing of the differential transmission. Our findings are in good agreement with recent experimental pump-probe studies.
We investigate the polarization dependence of the carrier excitation and relaxation in epitaxial multilayer graphene. Degenerate pump-probe experiments with a temporal resolution of 30 fs are performed for different rotation angles of the pump-pulse
polarization with respect to the polarization of the probe pulse. A pronounced dependence of the pump-induced transmission on this angle is found. It reflects a strong anisotropy of the pump-induced occupation of photogenerated carriers in momentum space even though the band structure is isotropic. Within 150 fs after excitation an isotropic carrier distribution is established. Our observations imply the predominant role of collinear scattering preserving the initially optically generated anisotropy in the carrier distribution. The experiments are well described by microscopic time-, momentum, and angle-resolved modelling, which allows us to unambiguously identify non-collinear carrier-phonon scattering to be the main relaxation mechanism giving rise to an isotropic distribution in the first hundred fs after optical excitation.
A transient femtosecond population inversion in graphene was recently reported by Li et al., Phys. Rev. Lett. 108, 167401 (2012). Based on a microscopic theory we clarify the underlying microscopic mechanism: Transient gain and population inversion i
n graphene occurs due to a complex interplay of strong optical pumping and carrier cooling that fills states close to the Dirac point giving rise to a relaxation bottleneck. The subsequent femtosecond decay of the optical gain is mainly driven by Coulomb-induced Auger recombination.
