The photoisomerization mechanism of trans-azobenzene was investigated using the CTTSH approach 199 in comparison to the Tully surface-hopping (TSH) scheme, in order to assess the performance of the implementation of CTTSH in . This study represented the first application of CTTSH to a molecular system in full dimensionality, as previous applications of CTTSH have been limited to model systems of one or two dimensions, typically comprising only two electronic states. While the theoretical foundations of the CTTSH approach have been previously discussed for low-dimensional model systems, the algorithm required customization to address numerical and computational challenges encountered in simulations involving systems with a large number of nuclear degrees of freedom.