Sukharev Maxim, Roslyak Oleksiy, Piryatinski Andrei
Department of Physics, Arizona State University, Tempe, Arizona 85287, USA.
Physics and Engineering Physics, Fordham University, Bronx, New York 10458, USA.
J Chem Phys. 2021 Feb 28;154(8):084703. doi: 10.1063/5.0037453.
We report on a theoretical study of second-harmonic generation (SHG) in plasmonic nanostructures interacting with two-level quantum emitters (QEs) under incoherent energy pump. We generalize the driven-dissipative Tavis-Cummings model by introducing the anharmonic surface plasmon-polariton (SPP) mode coupled to QEs and examine physical properties of corresponding SPP-QE polariton states. Our calculations of the SHG efficiency for strong QE-SPP coupling demonstrate orders of magnitude enhancement facilitated by the polariton gain. We further discuss time-domain numerical simulations of SHG in a square lattice comprising Ag nanopillars coupled to QEs utilizing a fully vectorial nonperturbative nonlinear hydrodynamic model for conduction electrons coupled to Maxwell-Bloch equations for QEs. The simulations support the idea of gain enhanced SHG and show orders of magnitude increase in the SHG efficiency as the QEs are tuned in resonance with the lattice plasmon mode and brought above the population inversion threshold by incoherent pumping. By varying pump frequency and tuning QEs to a localized plasmon mode, we demonstrate further enhancement of the SHG efficiency facilitated by strong local electric fields. The incident light polarization dependence of the SHG is examined and related to the symmetries of participating plasmon modes.
我们报告了在非相干能量泵浦下,与二能级量子发射器(QE)相互作用的等离子体纳米结构中二次谐波产生(SHG)的理论研究。我们通过引入与QE耦合的非谐表面等离激元极化激元(SPP)模式,推广了驱动耗散的塔维斯 - 卡明斯模型,并研究了相应的SPP - QE极化激元态的物理性质。我们对强QE - SPP耦合下的SHG效率的计算表明,极化激元增益促进了几个数量级的增强。我们进一步讨论了在由与QE耦合的银纳米柱组成的方形晶格中SHG的时域数值模拟,该模拟使用了与QE的麦克斯韦 - 布洛赫方程耦合的传导电子的全矢量非微扰非线性流体动力学模型。模拟结果支持增益增强SHG的观点,并表明随着QE与晶格等离激元模式调谐共振并通过非相干泵浦使其超过粒子数反转阈值,SHG效率会增加几个数量级。通过改变泵浦频率并将QE调谐到局域等离激元模式,我们证明了强局部电场促进了SHG效率的进一步增强。我们研究了SHG的入射光偏振依赖性,并将其与参与的等离激元模式的对称性相关联。