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HighlightsA zero-reflection-induced phase singularity is achieved through precisely controlling the resonance characteristics using two-dimensional nanomaterials.    An atomically thin nano-layer having a high absorption coefficient is exploited to enhance the zero-reflection dip, which has led to the subsequent phase singularity and thus a giant lateral position shift.    We have improved the detection limit of low molecular weight molecules by more than three orders of magnitude compared to current state-of-art nanomaterial-enhanced plasmonic sensors.Abstract  Detection of small cancer biomarkers with low molecular weight and a low concentration range has always been challenging yet urgent in many clinical applications such as diagnosing early-stage cancer, monitoring treatment and detecting relapse. Here, a highly enhanced plasmonic biosensor that can overcome this challenge is developed using atomically thin two-dimensional phase change nanomaterial. By precisely engineering the configuration with atomically thin materials, the phase singularity has been successfully achieved with a significantly enhanced lateral position shift effect. Based on our knowledge, it is the first experimental demonstration of a lateral position signal change > 340 μm at a sensing interface from all optical techniques. With this enhanced plasmonic effect, the detection limit has been experimentally demonstrated to be 10 –15  mol L −1  for TNF-α cancer marker, which has been found in various human diseases including inflammatory diseases and different kinds of cancer. The as-reported novel integration of atomically thin Ge 2 Sb 2 Te 5  with plasmonic substrate, which results in a phase singularity and thus a giant lateral position shift, enables the detection of cancer markers with low molecular weight at femtomolar level. These results will definitely hold promising potential in biomedical application and clinical diagnostics.Supplementary Information  The online version contains supplementary material available at 10.1007/s40820-021-00613-7.

Targeted Sub-Attomole Cancer Biomarker Detection Based on Phase Singularity 2D Nanomaterial-Enhanced Plasmonic Biosensor