Optofluidic sensors have accelerated the growth of smart
sensor
platforms with improved sensitivity, reliability, and innovation.
In this article, we report the integration of a surface-enhanced Raman
scattering (SERS) material consisting of silver nanoparticle-decorated
diatomaceous earth (AgNPs–DE) with a flow-through microfluidic
device, building up a hierarchical structured micro-total analysis
system (μ-TAS) capable of achieving part-per-quadrillion (ppq)-level
sensitivity. By the synergic integration of millimeter-scale microfluidic
devices and porous laboratory filter paper with a micrometer-sized
crosslinked cellulosic network that carries SERS-active AgNPs–DE,
which possesses submicron to nanometer regimes of photonic crystals
and plasmonic nanostructures, we achieved enhanced mass-transfer efficiency
and unprecedented detection sensitivity. In our experiment, fentanyl
as the testing analyte at different concentrations was measured using
a portable Raman spectrometer. The limit of detection (LOD) was estimated
to be 10 ppq from a small detection volume of 10 mL with an ultrafast
time of sensing (TOS) of 3 min. To attain comparable signals, the
traditional soaking method took more than 90 min to detect 10 part-per-trillion
fentanyl from a 10 mL sample. Compared with existing SERS sensing
results of fentanyl, the limit-defying μ-TAS reduced the LOD-TOS
product by almost 4 orders of magnitude, which represents a new stage
of ultrafast sensing of extremely low concentration analytes.