Strong Coupling of Molecular and Mid-Infrared Perfect Absorber Resonances

Mason, J. A.; Allen, G.; Podolskiy, Viktor A.; Wasserman, D.

doi:10.1109/lpt.2011.2171942

Cited by 68 publications

(47 citation statements)

References 14 publications

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“…15,16,17,18 While strong normal mode coupling has been widely investigated for electronic-state transitions, it is only very recently that cavity coupling to vibrational transitions were proposed and experimentally realized. 19,20,21 Work in this field has compared measured Rabi splittings to classical 19 and quantum mechanical descriptions 21 and the work by George et al 22 greatly extended the experimental landscape by utilizing molecular liquids and higher order cavity modes. Vibrational modes are particularly interesting because they involve nuclear motion along coordinates related to bond 3 formation and cleavage.…”

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confidence: 99%

Spanning Strong to Weak Normal Mode Coupling between Vibrational and Fabry–Pérot Cavity Modes through Tuning of Vibrational Absorption Strength

et al. 2015

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Designing coupled vibrational-cavity polariton systems modify chemical reaction rates and paths requires an understanding of how this coupling depends on system parameters (i.e. absorber strength, modal distribution, and vibrational absorber and cavity linewidths). Here, we evaluate the impact of absorption coefficient and cavity design on normal mode coupling between a FabryPérot cavity and a molecular vibration. For a vibrational band of urethane in a polymer matrix, the coupling strength increases with its concentration so that the system spans the weak and strong coupling regimes. The experimentally-determined Rabi splitting values are in excellent agreement with an analytical expression derived for classical coupled oscillators that includes no fitting parameters. Also, the cavity mode profile is altered through choice of mirror type with metal mirrors resulting in stronger confinement, and thus coupling, while dielectric stack mirrors provide higher transmission for a given cavity quality factor, and decreased coupling due to greater mode penetration into the dielectric mirror. In addition to polymers, the cavities can couple to molecular vibrational bands of dissolved species in solution, which greatly expands the range of systems that can be explored. Finally, longer pathlength cavities are used to demonstrate the pathlength-independence of the coupling strength. The ability to adjust the cavity linewidth, through the use of higher order modes, represents a route to match the cavity dephasing time to that of the molecular vibration and may be applied to a range of molecular systems. Understanding the roles of cavity design and validating empirical and analytical descriptions of absorber properties on coupling strength will facilitate application of these strong coupling effects to enable currently unreachable chemistries.Coupling between an optically-driven material excitation (e.g., a semiconductor quantum dot excitonic absorption) and a confined optical-mode (e.g., an optical microcavity) can drastically alter the behavior of both modes. Strong coupling, which occurs when the two modes are in resonance and the interaction between the two exceeds the damping rate, produces two hybridized states whose fundamental character is a quantum-mechanical superposition of the two original modes. Each of these mixed-character eigenstates is shifted from the original resonant frequency by half the Rabi splitting, Ω. 1 Such coupled systems are variously referred to as cavity polaritons, 2 coupled normal modes, 1 plexcitons 3 , or simply coupled normal modes. If the system consists of a single quantum oscillator (twolevel atom, single quantum dot, etc.) interacting with a single cavity photon, nonlinear effects such as photon blocking and climbing of the Jaynes-Cummings ladder may occur. The splitting in such a system is referred to as vacuum Rabi splitting 1,4,5 as opposed to simply Rabi or polariton splitting associated with ensembles of individual oscillators, as described herein. Relaxation lifetimes, 6,7 linewidt...

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Spanning Strong to Weak Normal Mode Coupling between Vibrational and Fabry–Pérot Cavity Modes through Tuning of Vibrational Absorption Strength

et al. 2015

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“…Solar thermionics is being developed that uses lithiated diamond to create a very efficient electron emitter [9] and if it was possible to integrate the diamond material within a solar absorbing surface this may lead to very low cost technology. Absorbing layers in MDM structures have been studied previously, in [15] a Spin-On-Glass with an absorption resonance in the mid infrared is used to show strong coupling between the metasurface resonance and the absorber. In [16] an MDM structure is incorporated into an organic photovoltaic cell in order to increase solar absorption.…”

Section: Introductionmentioning

confidence: 99%

Broadband metasurface absorber for solar thermal applications

Wan

Chen

Cryan

2015

J. Opt.

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In this paper we propose a broadband polarization independent selective absorber for solar thermal applications. It is based on a metal-dielectric-metal metasurface structure, but with an inter-layer of absorbing amorphous carbon rather than a low loss dielectric. Optical absorbance results derived from Finite Difference Time Domain modelling are shown for ultra-thin carbon layers in air and on 200nm of gold for a range of carbon thicknesses. A gold-amorphous carbon-gold trilayer with a top layer consisting of a 1D grating is then optimised in 2D to give a sharp transition from strong absorption up to 2m to strong reflection above 2m resulting in good solar selective performance. The gold was replaced by the high melting point metal tungsten and is shown to have very similar performance to the gold case. 3D simulations then show that the gold based structure performs well as a square periodic array of squares, however there is low absorption around 400nm. A cross based structure is found to increase this absorption without significantly reducing the performance at longer wavelengths.

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“…Since they were first demonstrated by experiment [2], the design and fabrication of metamaterial absorbers have been investigated intensively, finding a vast range of potential applications including biochemical sensors [3], bolometers [4] and tunable photon detectors [5]. However, the conventional metamaterial absorber with a single absorption band can hardly meet the requirement in some fields such as spectroscopic detection or energy harvesting.…”

Section: Introductionmentioning

confidence: 99%

Theoretical and Experimental Demonstrations of a Dual-Band Metamaterial Absorber at Mid-Infrared

Wen

2014

IEEE Photon. Technol. Lett.

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We present the design, fabrication, and physical interpretation of an infrared dual-band metamaterial absorber. The unit cell of the metamaterial absorber consists of a cross resonator ringed by four split-ring resonators spaced a distance above a gold ground plane with a dielectric layer of SiO 2 . The absorber shows two absorption peaks of 90.3% and 88.4% at 4.17 µm and 4.86 µm, respectively. The multireflection interference theory is applied to explain the absorption mechanism with the gold ground plane described by Drude model, and the theoretical calculation agrees well with the simulations and experiments. In addition, the designed absorber is insensitive to incident angle and polarization direction in a broad range, which are highly favorable features in practical applications.

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Strong Coupling of Molecular and Mid-Infrared Perfect Absorber Resonances

Cited by 68 publications

References 14 publications

Spanning Strong to Weak Normal Mode Coupling between Vibrational and Fabry–Pérot Cavity Modes through Tuning of Vibrational Absorption Strength

Spanning Strong to Weak Normal Mode Coupling between Vibrational and Fabry–Pérot Cavity Modes through Tuning of Vibrational Absorption Strength

Broadband metasurface absorber for solar thermal applications

Theoretical and Experimental Demonstrations of a Dual-Band Metamaterial Absorber at Mid-Infrared

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