▎ 摘　　要

Graphene, a unique two-dimensional material comprising carbon in a honeycomb lattice(1), has brought breakthroughs across electronics, mechanics and thermal transport, driven by the quasiparticle Dirac fermions obeying a linear dispersion(2,3). Here, we demonstrate a counter-pumped all-optical difference frequency process to coherently generate and control terahertz plasmons in atomic-layer graphene with octave-level tunability and high efficiency. We leverage the inherent surface asymmetry of graphene for strong second-order non-linear polarizability(4,5), which, together with tight plasmon field confinement, enables a robust difference frequency signal at terahertz frequencies. The counter-pumped resonant process on graphene uniquely achieves both energy and momentum conservation. Consequently, we demonstrate a dual-layer graphene heterostructure with terahertz charge-and gate-tunability over an octave, from 4.7 THz to 9.4 THz, bounded only by the pump amplifier optical bandwidth. Theoretical modelling supports our single-volt-level gate tuning and optical-bandwidth-bounded 4.7 THz phase-matching measurements through the random phase approximation, with phonon coupling, saturable absorption and below the Landau damping, to predict and understand graphene plasmon physics.