论文标题

宽带超快速金属的超快动力学:锡和ZRN

Broadband Ultrafast Dynamics of Refractory Metals: TiN and ZrN

论文作者

Diroll, Benjamin T., Saha, Soham, Shalaev, Vladimir M., Boltasseva, Alexandra, Schaller, Richard D.

论文摘要

过渡金属氮化物最近在等离子体,等离子体增强的光催化,光热应用和非线性光学元件上引起了人们的注意,因为它们具有合适的光学特性,难治性和较大的激光损伤阈值。这项工作报告了在飞秒激发下的氮化钛,氮化锆和Au膜的瞬时反应的比较研究。宽带瞬态光学表征有助于裁定基于单波长测量值的热电子寿命的早期,有些不一致的报告。这些泵探针实验仅在耐光化金属的epsilon-near-Zero窗口内显示了亚皮秒瞬态动力学。该动力学由超快电子重新分布引起的光诱导的带间跃迁主导。 Epsilon-near-Zero窗口中的增强反射调制使观察到低泵浦平均处这些薄膜的超快光学响应成为可能。这些结果表明,锡和ZRN中的电子偶联比AU大25-100倍。与AU相比,强的电子 - 音波耦合驱动了子秒的光学响应,并促进了更大的晶格加热,从而使锡和ZRN有望用于光热应用。锡和ZRN的光谱响应和动力学仅对泵的通量和泵激发能弱敏感。然而,在较高的泵光子能量和较高的平均值下,响应的大小要大得多,在epsilon-near-Zero窗口中,在锡tin中观察到的峰值为15%,ZRN的峰值为50%。

Transition metal nitrides have recently gained attention in the fields of plasmonics, plasmon-enhanced photocatalysis, photothermal applications, and nonlinear optics because of their suitable optical properties, refractory nature, and large laser damage thresholds. This work reports comparative studies of the transient response of films of titanium nitride, zirconium nitride, and Au under femtosecond excitation. Broadband transient optical characterization helps to adjudicate earlier, somewhat inconsistent reports regarding hot electron lifetimes based upon single wavelength measurements. These pump-probe experiments show sub-picosecond transient dynamics only within the epsilon-near-zero window of the refractory metals. The dynamics are dominated by photoinduced interband transitions resulting from ultrafast electron energy redistribution. The enhanced reflection modulation in the epsilon-near-zero window makes it possible to observe the ultrafast optical response of these films at low pump fluences. These results indicate that electron-phonon coupling in TiN and ZrN is 25-100 times greater than in Au. Strong electron-phonon coupling drives the sub-picosecond optical response and facilitates greater lattice heating compared to Au, making TiN and ZrN promising for photothermal applications. The spectral response and dynamics of TiN and ZrN are only weakly sensitive to pump fluence and pump excitation energy. However, the magnitude of the response is much greater at higher pump photon energies and higher fluences, reaching peak observed values of 15 % in TiN and 50 % in ZrN in the epsilon-near-zero window.

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