We now turn to the last two reference systems. The employed examples are dimers formed by anisole with either methanol or 2-naphthol. Both dimers have already been extensively analysed experimentally and theoretically. We start our discussion with the anisole methanol dimer. The experimental analysis of this system is based on FTIR spectroscopy from a cold supersonic jet expansion in helium. They measured a 20 times lower abundance of the OH-⇡ isomer than the preferred OH-O isomer. As a result they estimate the OH-⇡ bound dimer to be at least 1 kJ mol 1 less stable than the OH-O dimer. The theoretical methods applied to this system give di↵erent results. In case of MP2 the OH-⇡ dimer is clearly favoured by 0.6 kJ mol 1 , B3LYP-D3(BJ) favours the OH-O dimer by 0.7 kJ mol 1 , the doublehybrid B2PLYP favours the OH-O dimer by 1.1 kJ mol 1 and CCSD(T) indicates an almost isoenergetic balance between the two. In general they found, that the balance could be further shifted towards the OH-O bound dimer by 0.2 kJ mol 1 , if the aug-cc-pVTZ basis set instead of the def2-TZVP basis set is employed for the geometry optimization and energy computation. However, the dependence of the initial geometry is dramatically reduced by employing multicomponent methods since the quantum particle will instantaneously adapt to its preferred position. This was already demonstrated in a thorough benchmark for the hydrogen bound methanol complexes with di↵erent furan derivatives. Therefore, we first compare the B3LYP-D3(BJ), NEO-B3LYP-D3(BJ) as well as NEO(MP2)-PNO-LCCSD(T)-F12 31 results on the basis of the B3LYP-D3(BJ)/def2-TZVP optimised structures. The obtained results are displayed in Fig. . The regular B3LYP-D3(BJ) method leads to a preference towards the OH-O structure with 0.7 kJ mol 1 compared to the OH-⇡ bound dimer. This is in agreement with the results obtained by Heger et al. Utilizing NEO-B3LYP-D3(BJ) and NEO(MP2)-PNO-LCCSD(T)-F12 instead of regular B3LYP-D3(BJ) carries several advantages as mentioned before. First of all the dependency of the initial geometry is reduced, allowing for computational e cient optimization with small basis sets. As a result, the NEO-B3LYP-D3(BJ) single point calculation utilizing the def2-TZVP basis set already leads to experimental comparable results by favoring the OH-O bound dimer by 2.99 kJ mol 1 . Compared to the NEO(MP2)-PNO-LCCSD(T)-F12 method, which includes explicit correlation in order to achieve almost complete basis set results, the NEO-B3LYP-D3(BJ) method performs very similarly. Given an absolute energy di↵erence of only 0.12 kJ mol 1 between both methods, the NEO-B3LYP-D3(BJ) seems to perform very well on this system. Moreover, the NEO-B3LYP-D3(BJ) exhibits favourable computational e↵ort to achieve the result compared to the higher level approach. The NEO(MP2)-PNO-LCCSD(T)-F12 was running with a total CPU time of 193 minutes to compute both systems, compared to 12 minutes for the NEO-B3LYP-D3(BJ) calculations.