Typically, in real-time aerosol mass spectrometry (RTAMS), individual airbo
rne particles are ablated and ionized with a single focused laser pulse. Th
is technique yields information that permits bulk characterization of the p
article, but information about the particle's surface is often masked or di
luted by the particle bulk. Here we show that it is possible to probe the s
urface composition of individual airborne particles by separating the desor
ption and ionization steps using a two-laser real-time aerosol mass spectro
metry technique (L2RTAMS). First, a weak excimer laser pulse was used to de
sorb the semivolatile components of the particle surface when the particle
was in the center of the ion trap. After a short delay, another excimer las
er pulse was used to ionize the semivolatile surface components in the gas
phase and subsequently mass analyzed. The results from the one- and two-las
er techniques were compared and found to be complementary. The L2RTAMS tech
nique was found very sensitive to polycyclic aromatic hydrocarbons (PAHs).
PAHs, of the type emitted from diesel engines, were found on particle surfa
ces of National Institute of Standards and Technology (NIST) standard refer
ence materials (SRMs) from Indiana Harbor Canal (1645) and urban particulat
e matter (1648). PAH partitioning on the environmental particles is discuss
ed.