Organic Hyperbolic Material Assisted Illumination Nanoscopy.

Resolution capability of the linear structured illumination microscopy (SIM) plays a key role in its applications in physics, medicine, biology, and life science. Many advanced methodologies have been developed to extend the resolution of structured illumination by using subdiffraction-limited optical excitation patterns. However, obtaining SIM images with a resolution beyond 40 nm at visible frequency remains as an insurmountable obstacle due to the intrinsic limitation of spatial frequency bandwidth of the involved materials and the complexity of the illumination system. Here, a low-loss natural organic hyperbolic material (OHM) that can support record high spatial-frequency modes beyond 50k0 , i.e., effective refractive index larger than 50, at visible frequencies is reported. OHM-based speckle structured illumination microscopy demonstrates imaging resolution at 30 nm scales with enhanced fluorophore photostability, biocompatibility, easy to use and low cost. This study will open up a new route in super-resolution microscopy by utilizing OHM films for various applications including bioimaging and sensing.

Unprecedented Fluorophore Photostability Enabled by Low-Loss Organic Hyperbolic Materials.

The dynamics of photons in fluorescent molecules plays a key role in fluorescence imaging, optical sensing, organic photovoltaics, and displays. Photobleaching is an irreversible photodegradation process of fluorophores, representing a fundamental limitation in relevant optical applications. Chemical reagents are used to suppress the photobleaching rate but with exceptionally high specificity for each type of fluorophore. Here, using organic hyperbolic materials (OHMs), an optical platform to achieve unprecedented fluorophore photostability without any chemical specificity is demonstrated. A more than 500-fold lengthening of the photobleaching lifetime and a 230-fold increase in the total emitted photon counts are observed simultaneously. These exceptional improvements solely come from the low-loss hyperbolic dispersion of OHM films and the large resultant Purcell effect in the visible spectral range. The demonstrated OHM platform may open up a new paradigm in nanophotonics and organic plasmonics for super-resolution imaging and the engineering of light-matter interactions at the nanoscale.

Low-Loss Organic Hyperbolic Materials in the Visible Spectral Range: A Joint Experimental and First-Principles Study.

Hyperbolic media strengthen numerous attractive applications in optics such as super-resolution imaging, enhanced spontaneous emission, and nanoscale waveguiding. Natural hyperbolic materials exist at visible frequencies; however, implementations of these materials suffer substantial compromises resulting from the high loss in the currently available candidates. Here, the first experimental and theoretical investigation of regioregular poly(3-alkylthiophenes) (rr-P3ATs), a naturally low-loss organic hyperbolic material (OHM) in the visible frequency range, is shown. These hyperbolic properties arise from a highly ordered structure of layered electron-rich conjugated thiophene ring backbones separated by insulating alkyl side chains. The optical and electronic properties of the rr-P3AT can be tuned by controlling the degree of crystallinity and alkyl side chain length. First-principles calculations support the experimental observations, which result from the rr-P3AT's structural and optical anisotropy. Conveniently, rr-P3AT-based OHMs are facile to fabricate, flexible, and biocompatible, which may lead to tremendous new opportunities in a wide range of applications.

Nanoscale optical pulse limiter enabled by refractory metallic quantum wells.

The past several decades have witnessed rapid development of high-intensity, ultrashort pulse lasers, enabling deeper laboratory investigation of nonlinear optics, plasma physics, and quantum science and technology than previously possible. Naturally, with their increasing use, the risk of accidental damage to optical detection systems rises commensurately. Thus, various optical limiting mechanisms and devices have been proposed. However, restricted by the weak optical nonlinearity of natural materials, state-of-the-art optical limiters rely on bulk liquid or solid media, operating in the transmission mode. Device miniaturization becomes complicated with these designs while maintaining superior integrability and controllability. Here, we demonstrate a reflection-mode pulse limiter (sub-100 nm) using nanoscale refractory films made of Al2O3/TiN/Al2O3 metallic quantum wells (MQWs), which provide large and ultrafast Kerr-type optical nonlinearities due to the quantum size effect of the MQW. Functional multilayers consisting of these MQWs could find important applications in nanophotonics, nonlinear optics, and meta-optics.

Large optical nonlinearity enabled by coupled metallic quantum wells.

New materials that exhibit strong second-order optical nonlinearities at a desired operational frequency are of paramount importance for nonlinear optics. Giant second-order susceptibility χ (2) has been obtained in semiconductor quantum wells (QWs). Unfortunately, the limited confining potential in semiconductor QWs causes formidable challenges in scaling such a scheme to the visible/near-infrared (NIR) frequencies for more vital nonlinear-optic applications. Here, we introduce a metal/dielectric heterostructured platform, i.e., TiN/Al2O3 epitaxial multilayers, to overcome that limitation. This platform has an extremely high χ (2) of approximately 1500 pm/V at NIR frequencies. By combining the aforementioned heterostructure with the large electric field enhancement afforded by a nanostructured metasurface, the power efficiency of second harmonic generation (SHG) achieved 10-4 at an incident pulse intensity of 10 GW/cm2, which is an improvement of several orders of magnitude compared to that of previous demonstrations from nonlinear surfaces at similar frequencies. The proposed quantum-engineered heterostructures enable efficient wave mixing at visible/NIR frequencies into ultracompact nonlinear optical devices.