表面之下：通过束缚电子揭示铝的非线性光学特性的复杂性
Below the Surface: Unraveling the Intricacies of the Nonlinear Optical Properties of Aluminum through Bound Electrons
AI总结：
通过实验发现铝中束缚电子在二次谐波产生中导致光谱空洞，揭示共振吸收下束缚电子的关键作用，挑战现有表面物理理论。
摘要：
通过揭示铝中二次谐波产生的新颖方面，我们展示了共振吸收所带来的不寻常且显著的结果，即束缚电子在跨光学光谱的光与物质相互作用中扮演着出乎意料的关键角色，这表明需要一种不同的基本方法来充分解释表面物理。我们解决了一个在共振吸收下光传播普遍恶劣条件下从未被考虑的问题。与大多数贵金属不同，铝表现出洛伦兹型行为以及中心位于810纳米附近的带间跃迁，从而以非典型方式划分了等离激元范围，并使其线性和非线性光学特性与众不同。关于具有复杂拓扑结构的铝纳米结构的研究比比皆是，关于表面等离激元的线性光谱响应和谐波产生的报道不一致也是如此。我们对铝纳米层二次谐波产生的实验观察表明，束缚电子导致了一种既未被预测也未被观察到的独特特征：二次谐波光谱中的一个空洞。流体动力学-麦克斯韦理论极好地解释了这些发现，并成为重新研究表面物理的基础。
英文摘要：
By uncovering novel aspects of second harmonic generation in aluminum we show that there are unusual and remarkable consequences of resonant absorption, namely an unexpectedly critical role that bound electrons play for light-matter interactions across the optical spectrum, suggesting that a different basic approach is required to fully explain the physics of surfaces. We tackle an issue that is never under consideration given the generic hostile conditions to the propagation of light under resonant absorption. Unlike most noble metals, aluminum displays Lorentz-like behavior and interband transitions centered near 810 nm, thus splitting the plasmonic range in an atypical manner and setting its linear and nonlinear optical properties apart. Studies of aluminum nanostructures having complex topologies abound, as do reported inconsistencies in the linear spectral response of surface plasmons and harmonic generation. Our experimental observations of second harmonic generation from aluminum nanolayers show that bound electrons are responsible for a unique signature neither predicted nor observed previously: a hole in the second harmonic spectrum. A hydrodynamic-Maxwell theory explains these findings exceptionally well and becomes the basis for renewed studies of surface physics.
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