We experimentally demonstrate single beam directional perfect absorption (to within experimental accuracy) of ppolarized light in the near-infrared using unpatterned, deep subwavelength films of indium tin oxide (ITO) on Ag. The experimental perfect absorption occurs slightly above the epsilon-near-zero (ENZ) frequency of ITO where the permittivity is less than one. Remarkably, we obtain perfect absorption for films whose thickness is as low as ~1/50 th of the operating free-space wavelength and whose single pass attenuation is only ~ 5%. We further derive simple analytical conditions for perfect absorption in the subwavelength-film regime that reveal the constraints that the ITO permittivity must satisfy if perfect absorption is to be achieved. Then, to get a physical insight on the perfect absorption properties, we analyze the eigenmodes of the layered structure by computing both the realfrequency/complex-wavenumber and the complex-frequency/real-wavenumber modal dispersion diagrams. These analyses allow us to attribute the experimental perfect absorption behavior to the crossover between bound and leaky behavior of one eigenmode of the layered structure. Both modal methods show that perfect absorption occurs at a frequency slightly larger than the ENZ frequency, in agreement with experimental results, and both methods predict a second perfect absorption condition at higher frequencies attributed to another crossover between bound and leaky behavior of the same eigenmode. Our results greatly expand the list of materials that can be considered for use as ultrathin perfect absorbers and also provide a methodology for the design of absorber systems at any desired frequency.
Silver metal nanoparticle (NP) enhanced fluorescence is investigated in thin films of cyanobacterial Photosystem I trimer complexes (PSI) by correlating confocal laser scanning microscopy, dark-field imaging, and fluorescence lifetime measurements. PSI represents an interesting light-harvesting complex with a 20 nm diameter that is not uniformly contained within the surface-localized plasmon field of the NPs. With weak far-field illumination, 5- to 20-fold fluorescence enhancement is observed for PSI complexes adjacent to NPs, arising from efficient nanoparticle light collection and subsequent localized, surface plasmon excitation of PSI. Enhanced PSI fluorescence is detected most prominently near "rafts" of aggregated NPs that more completely fill the confocal field of view. These results demonstrate opportunities to probe energy transfer within photosynthetic complexes using plasmonic excitation and to design nanostructures for optimizing artificial light-harvesting systems.
We investigate optical polariton modes supported by subwavelength-thick degenerately doped semiconductor nanolayers (e.g. indium tin oxide) on glass in the epsilon-near-zero (ENZ) regime. The dispersions of the radiative (R, on the left of the light line) and non-radiative (NR, on the right of the light line) ENZ polariton modes are experimentally measured and theoretically analyzed through the transfer matrix method and the complex-frequency/real-wavenumber analysis, which are in remarkable agreement. We observe directional near-perfect absorption using the Kretschmann geometry for incidence conditions close to the NR-ENZ polariton mode dispersion. Along with field enhancement, this provides us with an unexplored pathway to enhance nonlinear optical processes and to open up directions for ultrafast, tunable thermal emission.
The existence of hidden complex cavities formed inside a self-assembled nanocrystalline structure is discovered in real-time by using surface plasmon resonance near-field refractive index fingerprinting. Furthermore, computer analysis of the naturally occurring R-G-B interference fringes allowed us to reconstruct the 3D cavity formation and crystallization processes quantitatively. For the case of an aqueous droplet containing 10% by volume of 47 nm Al2O3 nanoparticles, the submicrometer-scale inner cavity peak grows up to 0.5% of the entire crystallized crust height of over 150 microm. The formation of the complex inner structure was found to be attributable to multiple cavity inceptions and their competing growth during the aquatic evaporation. This outcome provides a better understanding and feasible control of the formation of nanocrystalline inner structures.
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