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The structure of the light-induced metastable state SII ofNa2[Fe(CN)5NO]$\cdot$2H2O 14 was investigated by transmission M\"ossbauerspectroscopy (TMS) in the temperature range 15 between 85 and 135 K, nuclearinelastic scattering (NIS) at 98 K using synchrotron 16 radiation and densityfunctional theory (DFT) calculations. The DFT and TMS results 17 stronglysupport the view that the NO group in SII takes a side-on molecular orientation18 and, further, is dynamically displaced from one eclipsed, via a staggered,to a second 19 eclipsed orientation. The population conditions for generatingSII are optimal for 20 measurements by TMS, yet they are modest foraccumulating NIS spectra. Optimization 21 of population conditions for NISmeasurements is discussed and new NIS experiments on 22 SII are proposed.

M\"ossbauer, nuclear inelastic scattering and density functional studies on the second metastable state of Na2[Fe(CN)5NO]$\cdot$2H2O