Compared to individual nanoparticles, supracolloidal structures offer unique plasmonic properties with enhanced susceptibility to variations in the local refractive index. In this study, we report the template‐assisted fabrication of large‐scale ( ca . 1 cm ² ) linear periodic assemblies of AuNPs and demonstrate their polarization‐dependent biosensing performance at the proof‐of‐concept level. We explore two complementary approaches for template fabrication: i) laser interference lithography (LIL), offering high‐fidelity patterns over moderate areas, and ii) wrinkle‐assisted patterning, a more scalable and cost‐effective strategy. Despite structural differences, both approaches yield comparable sensing performances. This demonstrates the broad potential utility of the developed biosensing platform. First, sensors are characterized through varying concentrations of glycerol/water mixtures with known refractive indices. Next, as a proof‐of‐concept application, we perform biofunctionalization and detection of the antibody for Tumor Necrosis Factor‐Alpha (TNF‐α). TNF‐α is a pro‐inflammatory cytokine that plays a multifaceted role in cancer prognosis. The shifts in plasmonic resonance peaks of the AuNP assemblies are quantified using polarized‐light vis‐NIR spectrometry during various stages of the functionalization and detection process. The experimental results reveal a pronounced polarization‐dependent plasmonic resonance peak shift (Δλ). Overall, a signal enhancement of up to 5‐fold is observed in the longitudinal mode over the transversal case, a feature consistently achieved across both LIL and wrinkled templates. These findings present an innovative supracolloidal structuring approach for the development and scalable production of highly sensitive, plasmonic biochips.

Sensitivity of field‐effect transistor biosensors (BioFETs) for nucleic acid detection is often limited by weak electrostatic control and low probe density at the sensing interface. Here, we present a BioFET platform with improved sensitivity based on lightly p‐doped Schottky‐barrier silicon nanobelt transistors, exhibiting reproducible ambipolar behavior in a back‐gated configuration. These devices are encapsulated with an Al ₂ O ₃ /ZrO ₂ nanolaminate to prevent device performance degradation and facilitate stable biofunctionalization. Dry‐state measurements demonstrate selective detection of prostate cancer biomarker, miR‐141, after immobilization of complementary capture DNA, achieving detection down to the ≈100 pM range, and discrimination against the non‐complementary sequence, miR‐155. To enhance sensitivity, template‐assisted self‐assembly of gold nanoparticles (AuNPs) is used to form ordered linear structures directly on the sensing region. The supracolloidal assembly of AuNPs at the sensing interface tunes the receptor spacing and orientation and amplifies the influence of target hybridization on transistor response. Compared to planar devices, the hybrid AuNP‐BioFET exhibits improved signal modulation while preserving the label‐free detection mechanism. This approach bridges scalable top‐down semiconductor technology and bottom‐up self‐assembled nanostructures, providing an innovative pathway for developing biosensing platforms with high sensitivity and multiplexing capabilities for detecting nucleic acids.

Near-field interactions between individual gold nanoparticles (AuNPs) in clusters or arrays open a new avenue for highly sensitive plasmonic biosensors, owing to their significant impact on the localized surface plasmon resonance. Compared to individual nanoparticles, supracolloidal structures offer unique plasmonic properties with the enhanced susceptibilities to variations in the local refractive index. In this study, we report on the template-assisted fabrication of large-scale (ca. 1 cm²) linear periodic assemblies of AuNPs and demonstrate their polarization dependent biosensing performance at the proof-of concept level. We explored two complementary approaches for template fabrication: (i) laser interference lithography (LIL), offering high-fidelity patterns over moderate areas, and (ii) wrinkle-assisted patterning, a more scalable and costeffective strategy. Despite structural differences, both approaches yielded comparable high biosensing performances, demonstrating broad potential utility of the developed biosensing platform. As a proof-of-concept application, we performed biofunctionalization and detection of the antibody for Tumor Necrosis Factor-Alpha (TNF-α), a pro-inflammatory cytokine that plays a multifaceted role in cancer prognosis. The shifts in plasmonic resonance peaks of the AuNP assemblies were quantified using polarized-light vis-NIR spectrometry during various stages of the functionalization and detection process. The experimental results revealed a pronounced polarization-dependent plasmonic resonance peak shift (Δλ), with up to a 5-fold increase observed in the longitudinal mode over the transversal case, a feature consistently achieved across both LIL 3 and wrinkled templates. These findings present an innovative supracolloidal structuring approach for the development and scalable production of highly sensitive, plasmonic biochips.