A method of forming a microelectronic structure, said method comprising: providing a stack comprising: a substrate having a surface; and one or more optional intermediate layers on said substrate surface; forming a patternable layer having first and second surfaces, said first surface being on said intermediate layers, if present, or on said substrate surface, if no intermediate layers are present, and said second surface being remote from said first surface, said patternable layer having an initial surface property at said second surface and comprising a polymer dispersed or dissolved in a solvent system, said polymer comprising recurring monomers comprising -OH groups; exposing said patternable layer to radiation so as to selectively alter said initial surface property to yield an altered surface property at the areas of exposure, forming a patterned layer having first and second surfaces, said first surface of said patterned layer being on said intermediate layers, if present, or on said substrate surface, if no intermediate layers are present, and said second surface of said patterned layer being remote from said first surface of said patterned layer; without altering said patterned layer, applying a self-assembling composition to the second surface of said patterned layer, said composition comprising a block copolymer comprising a first block and a second block; and causing said composition to self-assemble into a self-assembled layer in response to the initial surface property, the altered surface property, or both, wherein said self-assembled layer comprises a first self-assembled region and a second self-assembled region different from said first self-assembled region, wherein: said initial surface property is an affinity towards one of said first and second blocks over the other of said first and second blocks; and during said exposing, said affinity disappears so that said altered surface property is neutral towards said first and second blocks. providing a stack comprising: a substrate having a surface; and one or more optional intermediate layers on said substrate surface; a substrate having a surface; and one or more optional intermediate layers on said substrate surface; forming a patternable layer having first and second surfaces, said first surface being on said intermediate layers, if present, or on said substrate surface, if no intermediate layers are present, and said second surface being remote from said first surface, said patternable layer having an initial surface property at said second surface and comprising a polymer dispersed or dissolved in a solvent system, said polymer comprising recurring monomers comprising -OH groups; exposing said patternable layer to radiation so as to selectively alter said initial surface property to yield an altered surface property at the areas of exposure, forming a patterned layer having first and second surfaces, said first surface of said patterned layer being on said intermediate layers, if present, or on said substrate surface, if no intermediate layers are present, and said second surface of said patterned layer being remote from said first surface of said patterned layer; without altering said patterned layer, applying a self-assembling composition to the second surface of said patterned layer, said composition comprising a block copolymer comprising a first block and a second block; and causing said composition to self-assemble into a self-assembled layer in response to the initial surface property, the altered surface property, or both, wherein said self-assembled layer comprises a first self-assembled region and a second self-assembled region different from said first self-assembled region, wherein: said initial surface property is an affinity towards one of said first and second blocks over the other of said first and second blocks; and during said exposing, said affinity disappears so that said altered surface property is neutral towards said first and second blocks. said initial surface property is an affinity towards one of said first and second blocks over the other of said first and second blocks; and during said exposing, said affinity disappears so that said altered surface property is neutral towards said first and second blocks.