Accordingly, the computed optical extinction cross sections of our model gels display distinct polarization-dependent responses to uniaxial strain, evidenced by qualitatively different shifts in their LSPR peak frequencies (Fig. ). For the 8-mer gel, the extinction maximum Colloid-colloid static structure factors S(q) for wavevectors parallel q ∥ and perpendicular q ⊥ to strain direction: (a,f) prior to strain and (b,g) in strain. Colloid-colloid one-dimensional radial distribution function parallel g ∥ (r) and perpendicular g ⊥ (r) to strain direction: (c,h) prior to strain and (d,i) in strain. Configuration snapshots in strain (e,j) showed blue-shifting for the polarization parallel to the extension direction, and moderate red-shifting for the perpendicular polarization. This is behavior anticipated with affine deformation such as that seen in Fig. for the 8-mer gel, with particles moving farther apart in the direction parallel to extension (weakening LSPR coupling), but closer together in the perpendicular direction (strengthening LSPR coupling). Though experimental systems have been prepared that show this intuitive behavior, the opposite trend -pronounced redshifting of the LSPR peak frequency for the parallel polarization and moderate blue-shifting in the perpendicular polarization -is more commonly observed for nanocomposites, where the plasmonic nanoparticles have a tendency to cluster. The simulated colloidal gel with a binary mixture of M 1 = 2 and M 2 = 12 linkers, which also formed nanoparticle clusters under uniaxial strain (Fig. ), displayed this more typical, though less intuitive, mechanooptical response (Fig. ). Unlike in the plasmonic nanocomposites, where the degree of nanoparticle clustering and structure-dependent optical response is extremely challenging to control, the present results suggest that such changes can be deliberately engineered in linked plasmonic nanoparticle networks via a macroscopic control parameter: the proportion of short linkers (i.e., the composition of the binary linker blend).