In centrosymmetric molecules, like A(n+)[M-(CN)(6)](n-) (where A is alkali metal cation), normally all stretching vibrations of cyanide (CN-) Shift to high frequency in response to nonhydrostatic pressure, whereas, in non-centrosymmetric molecules in whiCh one axial CN ligand is replaced by NO ligand, one observes unusual softening of only equatorial CN stretching modes. This effect is pronounced when A(+) is replaced by Ag+ with,difference in coordination ability of latter, resulting in expression of characteristic sign-attire of back-bonding. One can correlate this uneven stretching of cyanide to Poisson-like effect, where the axial Fe-N, Fe-C, and C-N stretching modes harden but the equatorial C-N stretching modes soften due to expansion at the equatorial plane. Thus, the present study is focused on results of non-hydrostatic high-pressure Raman measurements on silver nitroprusside tip to 11.5 GPa, for not only observing Characteristic signature of "back-bonding" interaction, rarely featured in literature, but also for generating reversible flexible structures akin to noncovalent interaction.