Institute for Research in Electronics and Applied Physics, University of Maryland , College Park, Maryland 20742, United States.
Helmholtz-Zentrum Dresden-Rossendorf , P.O. Box 510119, 01314 Dresden, Germany.
Nano Lett. 2016 Apr 13;16(4):2734-8. doi: 10.1021/acs.nanolett.6b00405. Epub 2016 Mar 18.
Subwavelength graphene structures support localized plasmonic resonances in the terahertz and mid-infrared spectral regimes. The strong field confinement at the resonant frequency is predicted to significantly enhance the light-graphene interaction, which could enable nonlinear optics at low intensity in atomically thin, subwavelength devices. To date, the nonlinear response of graphene plasmons and their energy loss dynamics have not been experimentally studied. We measure and theoretically model the terahertz nonlinear response and energy relaxation dynamics of plasmons in graphene nanoribbons. We employ a terahertz pump-terahertz probe technique at the plasmon frequency and observe a strong saturation of plasmon absorption followed by a 10 ps relaxation time. The observed nonlinearity is enhanced by 2 orders of magnitude compared to unpatterned graphene with no plasmon resonance. We further present a thermal model for the nonlinear plasmonic absorption that supports the experimental results. The model shows that the observed strong linearity is caused by an unexpected red shift of plasmon resonance together with a broadening and weakening of the resonance caused by the transient increase in electron temperature. The model further predicts that even greater resonant enhancement of the nonlinear response can be expected in high-mobility graphene, suggesting that nonlinear graphene plasmonic devices could be promising candidates for nonlinear optical processing.
亚波长石墨烯结构在太赫兹和中红外光谱范围内支持局域等离子体共振。在共振频率处的强场限制预计将显著增强光与石墨烯的相互作用,从而能够在原子薄的亚波长器件中实现低强度下的非线性光学。迄今为止,石墨烯等离子体的非线性响应及其能量损失动力学尚未得到实验研究。我们测量并理论模拟了石墨烯纳米带中等离子体的太赫兹非线性响应和能量弛豫动力学。我们在等离子体频率处采用太赫兹泵浦-太赫兹探针技术,并观察到等离子体吸收的强烈饱和,随后是 10 ps 的弛豫时间。与没有等离子体共振的非图案化石墨烯相比,观察到的非线性增强了 2 个数量级。我们进一步提出了一个用于非线性等离子体吸收的热模型,该模型支持实验结果。该模型表明,观察到的强线性是由于等离子体共振的意外红移以及电子温度瞬态增加引起的共振的展宽和减弱所致。该模型进一步预测,在高迁移率的石墨烯中,非线性响应的共振增强甚至更大,这表明非线性石墨烯等离子体器件可能是非线性光学处理的有前途的候选者。