A Statistical Route to Robust SERS Quantitation Beyond the Single-Molecule Level.
Hao ZhangLongkun YangMeng ZhangHong WeiLianming TongHongxing XuZhipeng LiPublished in: Nano letters (2024)
Single-molecule surface-enhanced Raman spectroscopy (SM-SERS) holds great potential to revolutionize ultratrace quantitative analysis. However, achieving quantitative SM-SERS is challenging because of strong intensity fluctuation and blinking characteristics. In this study, we reveal the relation P = 1 - e -α between the statistical SERS probability P and the microscopic average molecule number α in SERS spectra, which lays the physical foundation for a statistical route to implement SM-SERS quantitation. Utilizing SERS probability calibration, we achieve quantitative SERS analysis with batch-to-batch robustness, extremely wide detection range of concentration covering 9 orders of magnitude, and ultralow detection limit far below the single-molecule level. These results indicate the physical feasibility of robust SERS quantitation through statistical route and certainly open a new avenue for implementing SERS as a practical analysis tool in various application scenarios.
Keyphrases
- raman spectroscopy
- single molecule
- gold nanoparticles
- sensitive detection
- label free
- atomic force microscopy
- living cells
- ms ms
- mass spectrometry
- loop mediated isothermal amplification
- quantum dots
- liquid chromatography tandem mass spectrometry
- minimally invasive
- physical activity
- dna methylation
- gene expression
- risk assessment
- liquid chromatography
- tandem mass spectrometry
- simultaneous determination
- density functional theory