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The ab initio electronic structure calculations of the Ni$_{2}$MnGa The alloyindicate that the orthorhombic 4O structure exhibits the lowest energy comparedto all known martensitic structures. The 4O structure is formed by nanotwindouble layers, i.e., oppositely oriented nanotwins consisting of two (101)lattice planes of nonmodulated martensitic structure. It exhibits the lowestoccupation of density of states at the Fermi level. The total energy 1.98meV/atom below the energy of nonmodulated martensite is achieved withinstructural relaxation by shifting Mn and Ga atoms at the nanotwin boundaries.The same atomic shift can also be found in other martensitic nanotwinned ormodulated structures such as 10M and 14M, which indicates the importance of thenanotwin double layer for the stability of these structures. Our discoveryshows that the nanotwinning or modulation is a natural property oflow-temperature martensitic phases in Ni-Mn-Ga alloys.

Ab initio prediction of stable nanotwin double layers and 4O structure in Ni$_{2}$MnGa