Ultrafast 2D spectroscopy reveals a wealth of information regarding the structure and dynamics of chemical systems. The modulation of peaks identifies the formation of coherent superpositions within the system, whilst spectral lineshape is a result of dephasing and relaxation processes caused by the solvent environment. Studies of such coherences formed within systems with coupled vibrational and electronic, or vibronic, states have provided insight into the efficient energy transfer observed within molecular aggregates and biological complexes. Here we present a model for the 2D spectroscopy of vibronic systems which employs the latest formulation of the non-Markovian Hierarchical Equations of Motion. The long-term memory of the environment is incorporated through the simultaneous propagation of a set of auxiliary density matrices, introducing inhomogeneous spectral broadening implicitly within the dynamical evolution.
|Publication status||Unpublished - 10 Sep 2018|
|Event||National Training School in Theoretical Chemistry - University of Oxford, Oxford, United Kingdom|
Duration: 2 Sep 2018 → 14 Sep 2018
|External training||National Training School in Theoretical Chemistry|
|Period||2/09/18 → 14/09/18|