Hello, I am trying to run a metal oxide (Mn3O4) which has a complicated spin state. There are Mn atoms with 2+, 3+ (all spin alpha), and 3+ (all spin beta). I am trying to specify the spins using the keywords under KIND. Mn atom has 4s2 3d5 configuration, with d electrons all spin alpha (high spin). Mn2+ has 3d5 configuration, and Mn3+ has either 3d4 (all alpha) or 3d4 (all beta). O becomes O2-, or 2s2 2p6. I am trying to follow the example discussed here: https://groups.google.com/forum/#!topic/cp2k/8fTVlCEjSME/discussion For Mn2+, I want to remove all beta electrons, remove 2 from alpha s states, and add 5 to alpha d states, which when divided by 2, should give 3d5 for alpha electrons. Unfortunately CP2K always give NaN for the energy of the alpha wavefunction when trying to calculate the initial guess wavefunction, which makes the whole calculation fail. Can anyone give some suggestions? Below is the input I have tried. &KIND Mn2 ELEMENT Mn BASIS_SET DZVP-MOLOPT-SR-GTH POTENTIAL GTH-PBE-q15 &BS &ALPHA NEL -2 5 L 0 2 N 4 3 &END &BETA NEL -2 -5 L 0 2 N 4 3 &END &END &END KIND &KIND Mn31 ELEMENT Mn BASIS_SET DZVP-MOLOPT-SR-GTH POTENTIAL GTH-PBE-q15 &BS &ALPHA NEL -2 3 L 0 2 N 4 3 &END &BETA NEL -2 -5 L 0 2 N 4 3 &END &END &END KIND &KIND Mn32 ELEMENT Mn BASIS_SET DZVP-MOLOPT-SR-GTH POTENTIAL GTH-PBE-q15 &BS &ALPHA NEL -2 -5 L 0 2 N 4 3 &END &BETA NEL -2 3 L 0 2 N 4 3 &END &END &END KIND &KIND O BASIS_SET DZVP-MOLOPT-GTH POTENTIAL GTH-PBE-q6 &BS &ALPHA NEL 2 L 1 N 2 &END &BETA NEL 2 L 1 N 2 &END &END &END KIND