  Quantum molecular dynamics simulations with MCTDH or ML-MCTDH perform best if
the potential energy surface (PES) has a sum-of-products (SOP) or multi-layer
operator (MLOp) structure. Here we investigate four different POTFIT-based
methods for representing a general PES as such a structure, among them the
novel random-sampling multi-layer Potfit (RS-MLPF). We study how the format and
accuracy of the PES representation influences the runtime of a benchmark
(ML-)MCTDH calculation, namely the computation of the ground state of the
${\text{H}_3\text{O}_2}^-$ ion. Our results show that compared to the SOP
format, the MLOp format leads to a much more favorable scaling of the
(ML-)MCTDH runtime with the PES accuracy. At reasonably high PES accuracy,
ML-MCTDH calculations thus become up to 20 times faster, and taken to the
extreme, the RS-MLPF method yields extremely accurate PES representations
(global root-mean-square error of $\sim 0.1\,\text{cm}^{-1}$) which still lead
to only moderate computational demands for ML-MCTDH.
