Abstract

Since it allows to probe the fast vibrational dynamics of molecules during chemical or biological processes, ultra-fast two-dimensional infrared (2DIR) Fourier spectroscopy has now become a well-established technique [1]. In particular, methods such as 2DIR chemical exchange spectroscopy [2,3] allow to study the time dynamics of non-equilibrium systems. In this communication, we report on the application of 2DIR spectroscopy to a highly-excited vibrational system, namely the carbon monoxide stretching mode in carboxyhemoglobin. The system is brought to a highly-excited non-equilibrium state by coherent vibrational ladder climbing [4] using an intense mid-infrared chirped pulse (Fig. 1(a)), allowing to populate a large number of vibrational levels (Fig. 1(b)).

© 2015 IEEE