We present a new program implementation of the gaussian process regression
adaptive density-guided approach [J. Chem. Phys. 153 (2020) 064105] in the
MidasCpp program. A number of technical and methodological improvements made
allowed us to extend this approach towards calculations of larger molecular
systems than those accessible previously and maintain the very high accuracy of
constructed potential energy surfaces. We demonstrate the performance of this
method on a test set of molecules of growing size and show that up to 80 % of
single point calculations could be avoided introducing a root mean square
deviation in fundamental excitations of about 3 cmβ1. A much higher
accuracy with errors below 1 cmβ1 could be achieved with tighter
convergence thresholds still reducing the number of single point computations
by up to 68 %. We further support our findings with a detailed analysis of wall
times measured while employing different electronic structure methods. Our
results demonstrate that GPR-ADGA is an effective tool, which could be applied
for cost-efficient calculations of potential energy surfaces suitable for
highly-accurate vibrational spectra simulations