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Lindsay Davis

How to interpret orbital transition in TDDFT?

Anum Shahzadi Anum Shahzadi  Follow

Form this output you dont.

Find this in the output:

             EXCITATION  DE-EXCITATION OCC     VIR  AMPLITUDE      AMPLITUDE  I       A     X(I->A)        Y(A->I) ---     ---   --------       -------- 10      17   -0.039945       0.001926 16      17    0.996619      -0.032612 16      20   -0.070681       0.003443

it shows you the involved orbitals in the transitions. This a dominant transition from the 16ths orbital to the 17ths (HOMO to LUMO). You need to visualize the MOs and decide on the nature (sigma,pi,n) of the orbitals. Since they are MOs, it can be difficult with large molecules. You can look up natural transition orbitals that aim to simplify the visualization.

How you can look at orbitals with gamess? I have no clue.

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Giovanna Serenelli  Follow
jmol is useful for visualising orbitals. (@hokru So how do you tie your 16 -> 17 transition to the appropriate eV result in the OPs table?)More
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Ian Neuhaus  Follow
@user1945827 the section i gave is printed for every transition (1 to 9). OPs table is the summary at then end of the td-dft output. It becomes clear if you download the output file from OPs post.More
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Chas Alston  Follow

To visualise the orbitals of your calculation, use a program of your choice. For Gamess, there are a few options availabile. I use ChemCraft and Molden, and they work quite well. Here is a compilation of some with the former mentioned:

orbitals of acetone

You can further use the summary to identify the most interesting, strongest transitions:

                          SUMMARY OF TDDFT RESULTS   STATE             ENERGY     EXCITATION  TRANSITION DIPOLE, A.U.  OSCILLATOR                    HARTREE          EV         X       Y       Z     STRENGTH   0  A         -193.0290234748    0.000   1  A         -192.8724089055    4.262     0.0001  0.0000  0.0001    0.000   2  A         -192.7831335626    6.691     0.4051 -0.0004  0.0000    0.027   3  A         -192.7317175333    8.090     0.0018 -0.0976  0.0001    0.002   4  A         -192.7220472153    8.353    -0.4522 -0.0001  0.0000    0.042   5  A         -192.7210047911    8.382    -0.0121  0.0000 -0.0006    0.000   6  A         -192.7176816741    8.472    -0.0001 -0.0013  0.0724    0.001   7  A         -192.7167365427    8.498     0.0006 -0.0002  0.0075    0.000   8  A         -192.6964881601    9.049     0.0029 -0.3152  0.0008    0.022   9  A         -192.6862850361    9.326    -0.0022  1.1274 -0.0093    0.290

For the calculated 9 states that is the last one, with an oscillator strength of 0.290. Now skip back one section to where you find:

      -------------------      SINGLET EXCITATIONS      -------------------

Look for excited state number 9:

 STATE #   9  ENERGY =    9.326387 EV OSCILLATOR STRENGTH =    0.290423 LAMBDA DIAGNOSTIC   =    0.561 (RYDBERG/CHARGE TRANSFER CHARACTER) SYMMETRY OF STATE   =    A                    EXCITATION  DE-EXCITATION     OCC     VIR  AMPLITUDE      AMPLITUDE      I       A     X(I->A)        Y(A->I)     ---     ---   --------       --------      9      17    0.137515       0.018404     15      17    0.694034      -0.078753     13      18   -0.085768      -0.006093     14      19   -0.059549      -0.004510     16      19   -0.289828       0.018031     15      20    0.051487       0.010566     11      21    0.053380       0.009416     13      21   -0.060120      -0.009392     16      22   -0.607830       0.005676     11      24    0.052546       0.012226     13      25   -0.039117      -0.008987     16      26    0.112895       0.016712     16      30   -0.041659      -0.014274     16      33    0.052880       0.019973     16      36   -0.031783      -0.011699     13      40   -0.030352      -0.013004

There you find the orbital transitions. You can also have a look at the amplitudes to identify the most dominant one. In this case it is probably 15 to 17 and therefore corresponds to $\pi\to\pi^*$.

The more complicated the molecules get, the more confusing will this process be. Also the higher the level of theory, the more transitions you will need to consider. In this case Natural Transition Orbitals will certainly become very helpful, see Richard L. Martin, J. Chem. Phys., 2003, 118, 4775-4777.

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