Vibrational coherent control toward spectroscopic sensing and imaging applications

Abstract

Vibrational spectroscopy is widely used for a large variety of sensing and imaging applications. Nonlinear optical interactions using ultrashort laser pulses can facilitate selective coherent excitation of molecular vibrational modes, such as stretching and bending C-H and O-H vibrational modes. However, such spectroscopic probes are often based on the assumption that the energy distribution is static throughout the system, neglecting complex molecular dynamics and the effects of local nano- and microenvironments. To tackle this challenge, we developed a coherent control technique with a special focus on the temporal evolution of molecular vibrational modes. By utilizing a high-dynamic range detection, we demonstrate molecular vibrational dynamics and the environmental effects with multidimensional spectroscopic sensing. Such capability promises a broad range of sensing and imaging applications in biology, materials, and chemical sciences.