Self-Assembled Au Nanoparticle Arrays for Precise Metabolic Assay of Cerebrospinal Fluid

Precise and rapid monitoring of metabolites in biofluids is a desirable but unmet goal for disease diagnosis and management. Matrix-assisted laser desorption/ionization mass spectrometry (MALDI-MS) exhibits advantages in metabolite analysis. However, the low accuracy in quantification of the technique limits its transformation to clinical usage. We report herein the use of Au nanoparticle arrays self-assembled at liquid–liquid interfaces for mass spectrometry (MS)-based quantitative biofluids metabolic profiling. The two-dimensional arrays feature uniformly and closely packed Au nanoparticles with 3 nm interparticle gaps. The experimental study and theoretical simulation show that the arrays exhibit high photothermal conversion and heat confinement effects, which enhance the laser desorption/ionization efficacy. With the nanoscale roughness, the AuNP arrays as laser desorption/ionization substrates can interrupt the coffee-ring effect during droplet evaporation. Therefore, high reproducibility (RSD