Abstract
Full-dimensionality quantum calculations of acetylene–vinylidene isomerization J. Full quantum mechanical calculations of vibrational energies of methane and fluoromethane are carried out using a polyspherical description combining Radau and Jacobi coordinates. The Hamiltonian is built in a potential-optimized discrete variable representation, and vibrational energies are solved using an iterative eigensolver. This new approach can be applied to a large variety of molecules. In particular, we show that it is able to accurately and efficiently compute eigenstates for four different molecules : CH4 , CHD3 , CH2D2 , and CH3F. Very good agreement is obtained with the results reported previously in the literature with different approaches and with experimental data.