Surface-enhanced photoluminescence and Raman spectroscopy of single molecule confined in coupled Au bowtie nanoantenna.

Optical nanoantennas possess broad applications in the fields of photodetection, environmental science, biosensing and nonlinear optics, owing to their remarkable ability to enhance and confine the optical field at the nanoscale. In this article, we present a theoretical investigation of surface-enhanced photoluminescence spectroscopy for single molecules confined within novel Au bowtie nanoantenna, covering a wavelength range from the visible to near-infrared spectral regions. We employ the finite element method to quantitatively study the optical enhancement properties of the plasmonic field, quantum yield, Raman scattering and fluorescence. Additionally, we systematically examine the contribution of nonlocal dielectric response in the gap mode to the quantum yield, aiming to gain a better understanding of the fluorescence enhancement mechanism. Our results demonstrate that altering the configuration of the nanoantenna has a significant impact on plasmonic sensitivity. The nonlocal dielectric response plays a crucial role in reducing the quantum yield and corresponding fluorescence intensity when the gap distance is less than 3 nm. However, a substantial excitation field can effectively overcome fluorescence quenching and enhance the fluorescence intensity. By optimizing nanoantenna configuration, the maximum enhancement of surface-enhanced Raman can be turned to 9 and 10 magnitude orders in the visible and near-infrared regions, and 3 and 4 magnitude orders for fluorescence enhancement, respectively. The maximum spatial resolutions of 0.8 nm and 1.5 nm for Raman and fluorescence are also achieved, respectively. Our calculated results not only provide theoretical guidance for the design and application of new nanoantennas, but also contribute to expanding the range of surface-enhanced Raman and fluorescence technology from the visible to the near-infrared region.

Biobased Composites with High Lignin Content and Excellent Mechanical Properties toward the Ingenious Photoresponsive Actuator.

The fabrication of biobased smart materials from renewable biomasses is of great importance for sustainable development. Although lignin possesses photothermal conversion potential, the development of lignin-based actuators with large contraction and fast photoresponse has various hurdles. Herein, simply by blending with castor oil-derived polyamide elastomers, a lignin-based photoresponsive actuator can be obtained, which accomplishes up to 18% light-driven contraction under loading within 3 s. The crystals in polymer matrix serve as switch segments, firmly locking the stress-induced strain energy, which is swiftly released due to photothermal processes and induced a huge contraction. The composite, LP4-50, can contract and induce dynamic bending in multiple directions when irradiated locally with a near-infrared 808 nm laser. Furthermore, at standard 1 sun irradiation (100 mW/cm2), LP4-50 was successfully employed to power a thermoelectric generator. This strategy establishes the groundwork for further research into the photothermal characteristics of lignin and encourages new applications in stimulus-responsive actuators.