Help with mcscf convergence

Always always always double-check your active space and your geometry. Always. I ran this computation myself, and it looks like the ordering of orbital energies in vanilla SCF is:

    Doubly Occupied:                                                      

       1Ag    -2.661020     1B1u   -2.548529     2Ag    -0.209733  

    Virtual:                                                              

       1B3u    0.005156     1B2u    0.005156     2B1u    0.011595  
       3Ag     0.049491     1B2g    0.059896     1B3g    0.059896  
       3B1u    0.063416     2B3u    0.078978     2B2u    0.078978  
       4Ag     0.123702     5Ag     0.160921     4B1u    0.180307  
       2B2g    0.182642     2B3g    0.182642     1B1g    0.326548  
       6Ag     0.326548     5B1u    0.348420     3B3u    0.402386  
       3B2u    0.402386     7Ag     0.434997     3B2g    0.441744  
       3B3g    0.441744     1Au     0.490063     6B1u    0.490063  
       7B1u    0.547246     4B3u    0.626574     4B2u    0.626574  
       8Ag     0.658857     4B2g    1.041967     4B3g    1.041967  
       8B1u    1.157239     9Ag     1.775201     9B1u    2.239306  
      10B1u    6.233364     5B3u    6.241537     5B2u    6.241537  
       5B2g    6.422021     5B3g    6.422021    10Ag     6.605620  
      11Ag    15.192822    11B1u   15.320472  

Psi itself reports your active space of choice as:

   ------------------------------------------------------------------------------
               Space    Total    Ag   B1g   B2g   B3g    Au   B1u   B2u   B3u
   ------------------------------------------------------------------------------
         Frozen DOCC        0     0     0     0     0     0     0     0     0
     Restricted DOCC        0     0     0     0     0     0     0     0     0
              Active       16     5     0     0     0     0     5     3     3
     Restricted UOCC       28     6     1     5     5     1     6     2     2
         Frozen UOCC        0     0     0     0     0     0     0     0     0
   ------------------------------------------------------------------------------

With no core orbitals, the key information is in the active section. Cross-referencing that against the Hartree-Fock orbitals, you’re skipping over two B2g/B3g pairs, a B1g/Ag pair, and another Ag to get a high-lying B1u, B3u, and B2u. I would need to work through the correlation tables to be sure, but I have a very strong suspicion that this does not make good chemical sense.

When I tried a CAS(6, 15) with the active space [5, 0, 1, 1, 0, 4, 2, 2], it still didn’t converge, but I got a lower energy (-14.78393), which tells me I’m on the right track. I tried removing the highest-energy orbital, the 4th B1u, and the computation still failed to converge, but with a much higher energy.

However, this is a strange geometry. A 1.25 separation for the lithium dimer is tiny. NIST tells me 2.7 angstroms is more realistic for the ground state. Did you mean to have the atoms that close together? This is causing problems even in a conventional SCF - there’s a UHF solution about 0.2 hartrees lower. It’s horrifically spin contaminated, of course, but that shouldn’t be there. My hunch is that it’s making your CASSCF harder than it should be.