Spatially-resolved analysis of nanoparticle nucleation and growth in a microfluidic reactor.

Microfluidic systems provide a unique platform for investigation of fundamental reaction processes, which is critical to understanding how to control nanostructure synthesis on a production scale. We have examined the synthesis of cysteine-capped CdS quantum dot nanocrystals (CdS-Cys) between two interdiffusing reagent streams in a continuous-flow microfluidic reactor. Using spatially resolved photoluminescence imaging and spectroscopy of the microreactor, we have acquired kinetic and mechanistic data on the CdS-Cys nanoparticle nucleation and growth, and observed a binary shift in the particle emission spectrum from a higher (2.9 eV) to lower (2.5 eV) energy emission peak within the first second of residence time. Several reactor models have been tested against the spatially and spectrally resolved signals, which suggest that homogeneous reaction and particle nucleation are diffusion-limited and occur only at the boundary between the two laminar streams, while a slower activation process occurs on a longer (seconds) time scale. The results provide direct insight into the rapid processes that occur during crystallization in microfluidic mixing channels, and demonstrate the potential of using controlled microfluidic environments with spatially resolved monitoring to conduct fundamental studies of nanocrystal nucleation and growth.