“…Herein, to guarantee the accurate homogeneous immunoassay, a self-validated immunoassay was proposed by simultaneously scrutinizing both the frequency and the intensity of the pulse signal from single gold nanoparticles (AuNPs). The metal isotopes inside nanoparticle tags were sensitively and selectively detected by inductively coupled plasma mass spectrometry (ICPMS), − which has been recently successfully demonstrated in the analysis of metals, , proteins, − nucleic acid, , enzymes, single cells, − etc. The frequency of the pulse signals represents the number concentration of AuNPs, while the recorded signal intensity represents the size of AuNPs. , Carcinoembryonic antigen (CEA), a 180 kDa glycoprotein which belongs to tumor-associated biomarkers in human serum, was selected as a model analyte.…”