LAUSR

Abstract Understanding the spatial radiation pattern in tip-enhanced spectroscopy (TES) is crucial for plasmon-enhanced spectroscopy, chemical analysis and biochemical sensing. Although the TES technique has many excellent advantages, there is still room for improvement in terms of detection sensitivity. In this paper, we theoretically demonstrate the tip-tilted TES configuration featuring high directivity by using side illumination-collection condition. Taking full advantage of the characteristic of high directional emission ascribed to the far-field interference between localized surface plasmon resonance (LSPR) and surface plasmon polariton (SPP) modes, the collection efficiency of TES signals can be largely improved, greatly boosting the detection sensitivity of TES technology. Our theoretical results not only provide a deep understanding of the underlying physical mechanism of the directional surface plasmon-coupled emission of TES, but also serves as a promising guide for the rational construction of a highly efficient TES platform at the single molecular level.