Electrochemical Modulation of Strong Vibration–Cavity Coupling,ACS Photonics

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Electrochemical Modulation of Strong Vibration–Cavity Coupling
ACS Photonics ( IF 6.5 ) Pub Date : 2019-12-31 , DOI: 10.1021/acsphotonics.9b01339
J. J. Pietron ₁ , K. P. Fears ₁ , J. C. Owrutsky ₁ , B. S. Simpkins ₁

Affiliation

Modulation of strong coupling has implications for on-demand reactivity, optical modulation devices, and greater understanding of molecule–cavity coupling effects. Here, we electrochemically switch the redox couple benzoquinone/dihydroquinone (BQ/dHQ) within an optical cavity. We find that the BQ carbonyl species can be reduced, under appropriate biases, resulting in the complete elimination of the Rabi splitting, which is the signature of strong coupling. We achieve optical signal modulation of ∼100% at frequencies near the fundamental BQ carbonyl absorption as well as the polariton bands, and we experimentally evaluate the switching rate of such systems, finding that repeated cycling degrades performance, likely due to compositional changes in the electrochemical medium during the electrochemical reactions. Cavity resonances shift in correlation with the change of the solvent dielectric constant during electrochemical cycling. Although this consequent detuning influences the magnitude of optical modulation at the fundamental BQ resonance frequency, it makes optical modulation possible at many frequencies simultaneously since cavity fringe position scales with the refractive index. These results expand the understanding and utility of strong vibrational–cavity coupling and may lead to demonstrations of modified electrochemical response for technologically relevant material systems.

中文翻译：

强振动-腔耦合的电化学调制

强耦合的调制对按需反应性，光学调制装置以及对分子-腔耦合效应的更多理解具有影响。在这里，我们在光学腔内电化学切换氧化还原对苯醌/二氢醌（BQ / dHQ）。我们发现可以在适当的偏压下还原BQ羰基物质，从而完全消除Rabi分裂，这是强耦合的标志。我们在接近基本BQ羰基吸收以及极化带的频率上实现了约100％的光信号调制，并通过实验评估了此类系统的开关速率，发现重复循环会降低性能，这可能是由于电化学中的成分变化所致介质在电化学反应过程中。在电化学循环过程中，腔共振随溶剂介电常数的变化而变化。尽管这种失谐会影响基本BQ共振频率下的光调制幅度，但由于腔条纹位置随折射率而变，因此它使得在许多频率上同时进行光调制成为可能。这些结果扩大了对强振动腔耦合的理解和实用性，并可能导致对技术上相关的材料系统进行改进的电化学响应的演示。由于空腔条纹的位置随折射率而定，因此它使得在许多频率上同时进行光调制成为可能。这些结果扩大了对强振动腔耦合的理解和实用性，并可能导致对技术上相关的材料系统进行改进的电化学响应的演示。由于空腔条纹的位置随折射率而定，因此它使得在许多频率上同时进行光调制成为可能。这些结果扩大了对强振动腔耦合的理解和实用性，并可能导致对技术上相关的材料系统进行改进的电化学响应的演示。

更新日期：2019-12-31

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