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The uncertainties in metastable state populations indicated here and throughout the paper are estimated. The values output directly from the least-squares analysis are known to be too small, since they do not take into account off-diagonal terms in the covariance matrix, which will be significant due to the high correlation between, for example, the atomic displacement parameters and the occupancy fractions. Further comment on the reliability of refining occupancy fractions can be found in Ref.. We note that despite the hazards of simultaneously refining atomic displacement parameters and occupancy, the excited-state atomic positions do not substantially overlap with the ground state, thus making this system easier to model than, for instance, NO complexes.
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