In order to simulate the residual chemical shift anisotropy, we follow a slightly altered version of the calculation procedure published in ref . The theoretical background is presented in more detail in Section 1.2.1 of the Supporting Information, as it is thus far only completely available in German. It can shortly be described by the following procedure: For an anisotropic, linear molecule like CO2, the shielding tensor σ contains two contributions, one for parallel (𝛿 || ) and one for perpendicular (𝛿 ⊥ ) orientation to the external magnetic field 𝐵 0 ⃗⃗⃗⃗ .