A new approach for the calculation of eigenstates with the state-averaged (multi-layer) multi-configurational time-dependent Hartree (MCTDH) approach is presented. The approach is inspired by the recent work of Larsson [J. Chem. Phys. 151, 204102 (2019)]. It employs local optimization of the basis sets at each node of the multi-layer MCTDH tree and successive downward and upward sweeps to obtain a globally converged result. At the top node, the Hamiltonian represented in the basis of the single-particle functions (SPFs) of the first layer is diagonalized. Here p wavefunctions corresponding to the p lowest eigenvalues are computed by a block Lanczos approach. At all other nodes, a non-linear operator consisting of the respective mean-field Hamiltonian matrix and a projector onto the space spanned by the respective SPFs is considered. Here, the eigenstate corresponding to the lowest eigenvalue is computed using a short iterative Lanczos scheme. Two different examples are studied to illustrate the new approach: the calculation of the vibrational states of methyl and acetonitrile. The calculations for methyl employ the single-layer MCTDH approach, a general potential energy surface, and the correlation discrete variable representation. A five-layer MCTDH representation and a sum of product-type Hamiltonian are used in the acetonitrile calculations. Very fast convergence and order of magnitude reductions in the numerical effort compared to the previously used block relaxation scheme are found. Furthermore, a detailed comparison with the results of Avila and Carrington [J. Chem. Phys. 134, 054126 (2011)] for acetonitrile highlights the potential problems of convergence tests for high-dimensional systems.
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