Memory devices described herein are programmed and erased by physical segregation of an electrically insulating layer out of a memory material to establish a high resistance state, and by re-absorption of at least a portion of the electrically insulating layer into the memory material to establish a low resistance state. The physical mechanism of programming and erasing includes movement of structure vacancies to form voids, and/or segregation of doping material and bulk material, to create the electrically insulating layer consisting of voids and/or dielectric doping material along an inter-electrode current path between electrodes.