DNA at Aqueous/Solid Interfaces: Chirality-Based Detection via Second Harmonic Generation Activity

We present electronic spectra of single-strand and duplex DNA oligonucleotides covalently attached to fused quartz/aqueous interfaces and demonstrate that a strong nonlinear optical linear dichroism response is obtained when adenine and thymine bases undergo Watson-Crick base pairing to form a double helix. Complementary chi(3) charge screening studies indicate that the signal originates from 5 x 10(11) strands per square centimeter, or 6 attomoles of surface-bound oligonucleotides. The label-free, molecular-specific nature afforded by nonlinear optical studies of DNA at aqueous/solid interfaces allows for the real-time tracking of interfacial DNA hybridization for the first time.