The interaction between a probing tip and an adsorbed molecule can significantly impact the molecular chemical structure and even induce its motion on the surface. In this study, the tip-induced bond weakening, tilting, and hopping processes of a single molecule were investigated by sub-nanometre resolved tip-enhanced Raman spectroscopy (TERS). We used single carbon monoxide (CO) molecules adsorbed on the Cu (100) surface as a model system for the investigation. The vibrational frequency of the C−O stretching mode is always redshifted as the tip approaches, revealing the weakening of the C−O bond owing to tip−molecule interactions. Further analyses of both the vibrational Stark effect and TERS imaging patterns suggest a delicate tilting phenomenon of the adsorbed CO molecule on Cu(100), which eventually leads to lateral hopping of the molecule. While a tilting orientation is found toward the hollow site along the [110] direction of the Cu(100) surface, the hopping event is more likely to proceed via the bridge site to the nearest Cu neighbour along the [100] or [010] direction. Our results provide deep insights into the microscopic mechanisms of tip−molecule interactions and tip-induced molecular motions on surfaces at the single-bond level.

We report all-optical mid-infrared phase and intensity modulators based on the photo-thermal effect in an acetylene-filled anti-resonant hollow-core fiber. Optical absorption of the control beam promotes the gas molecules to a higher energy level, which induces localized heating through non-radiative relaxation and modulates the refractive index of the gas material and hence the accumulated phase of the signal beam propagating through the hollow-core fiber. By modulating the intensity of the control beam, the phase of the signal beam is modulated accordingly. By use of a 1.53 µm near-infrared control beam, all-optical phase modulation up to 2.2π rad is experimentally demonstrated at the signal wavelength of 3.35 µm. With the phase modulator placed in one arm of a Mach-Zehnder interferometer, intensity modulation with on-off ratio of 25 dB is achieved. The gas-filled hollow-core-fiber modulators could operate over an ultra-broad wavelength band from near- to mid-infrared and have promising application in mid-infrared photonic systems.

Tilted Wave Interferometry (TWI) is a measurement technique for fast and flexible interferometric testing of aspheres and freeform surfaces. The first version of the tilted wave principle was implemented in a Twyman-Green type setup with separate reference arm, which is intrinsically susceptible to environmentally induced phase disturbances. In this contribution we present the TWI in a new robust common-path (Fizeau) configuration. The implementation of the Tilted Wave Fizeau Interferometer requires a new approach in illumination, calibration and evaluation. Measurements of two aspheres and a freeform surface show the flexibility and also the increased stability in both phase raw data and surface measurements, which leads to a reduced repeatability up to a factor of three. The novel configuration significantly relaxes the tolerances of the imaging optics used in the interferometer. We demonstrate this using simulations on calibration measurements, where we see an improvement of one order of magnitude compared to the classical Twyman-Green TWI approach and the capability to compensate higher order error contributions on the used optics.

To improve the lateral resolution in microscopic imaging, microspheres are placed close to the object’ s surface in order to support the imaging process by optical near-field information. Although microsphere-assisted measurements are part of various recent studies, no generally accepted explanation for the effect of microspheres exists. Photonic nanojets, enhancement of the numerical aperture, whispering-gallery modes and evanescent waves are usually named reasons in context with microspheres, though none of these effects is proven to be decisive for the resolution enhancement. We present a simulation model of the complete microscopic imaging process of microsphere-enhanced interference microscopy including a rigorous treatment of the light scattering process at the surface of the specimen. The model consideres objective lenses of high numerical aperture providing 3D conical illumination and imaging. The enhanced resolution and magnification by the microsphere is analyzed with respect to the numerical aperture of the objective lenses. Further, we give a criterion for the achievable resolution and demonstrate that a local enhancement of the numerical aperture is the most likely reason for the resolution enhancement.

Aspheric micro-lens array (AMLA), featured with low dispersion and diffraction-limited imaging quality, plays an important role in advanced optical imaging. Ideally, the fabrication of commercially applicable AMLAs should feature low cost, high precision, large area and high speed. However, these criteria have been achieved only partially with conventional fabrication process. Herein, we demonstrate the fabrication and characterization of AMLAs based on 12-bit direct laser writing lithography, which exhibits a high fabrication speed, large area, perfect lens shape control via a three-dimensional optical proximity correction and average surface roughness lower than 6 nm. In particular, the AMLAs can be flexibly designed with customized filling factor and arbitrary off-axis operation for each single micro-lens, and the proposed pattern transfer approach with polydimethylsiloxane (PDMS) suggests a low-cost way for mass manufacturing. An auto-stereoscopic-display flexible thin film with excellent display effect has been prepared by using above technology, which exhibits a new way to provide flexible auto-stereoscopic-display at low cost. In brief, the demonstrated fabrication of AMLAs based on direct laser writing lithography reduce the complexity of AMLA fabrication while significantly increasing their performance, suggesting a new route for high-quality three-dimentional optical manufacturing towards simplified fabrication process, high precision and large scale.

Surface plasmon devices mounted at the end-facets of optical fibers are appealing candidates for rapid and point-of-care sensing applications, by offering a special dip-and-read operation mode. At present, these devices’ noise-equivalent limits-of-detection lag far behind the free-space counterparts, leaving them incapable of most biosensing applications. Here we report a quasi-3D Fano resonance cavity and its fabrication method to fundamentally improve the quality factor and coupling efficiency for fiber-coupled surface plasmon resonance. In this device, the Fano resonance combines the high coupling efficiency of a Fabry-Pérot etalon and the high quality factor resonance of a plasmonic crystal cavity. The quasi-3D device was fabricated on a planar substrate and transferred to a single-mode fiber end-facet, which requires a low-adhesion yet surface-plasmon-tunneling interface between the device and the planar substrate. Such an interface was realized with a nanocap-slit unit structure, of which the plasmonic crystal was consisted. A noise-equivalent limit of detection of ~ 10^-7 RIU was experimentally obtained, allowing bovine serum albumin physical adsorption to be distinguished at ng mL^-1 level concentrations. Therefore, breaking through the long-standing signal-to-noise ratio bottleneck, this work makes fiber end-facet surface plasmon devices into one of high sensitivity label-free sensing technologies. At the same time, it provides an enabling top-down fabrication technology for making 3D plasmonic structures on fiber end-facets at the nanometer scale.