We  use  high-level  computational  theory  to  demonstrate  how  a novel  class  of  crystalline  semiconductor  materials,  so-called  layered hybrid organic-inorganic perovskites (HOIPs), can be designed at the atomic  scale  to  provide  targeted  semiconductor  properties.  The  tun-ability of the materials arises from the atomic-scale combination of an inorganic   semi-conductor   integrated   with   functionalized   organic molecules that offer a wide range of properties.

With input from predictive theory, the resulting hybrid materials can be  deliberately  designed  to  fulfill  a  set  of  target  criteria,  for  instance specific   optical   emission,   absorption   and/or   electrical   carrier properties  in  different  quantum-well  arrangements.  The  approach  is here  applied  to  HOIPs  with  oligothiophene  molecules  as  the  organic component. The same  principle  opens a vast space  of  possible  new materials for discovery and design in the spirit of the MGI.