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Experimental evidence of new tetragonal polymorphs of silicon formed through ultrafast-laser-induced confined microexplosion...

Publication Type
Journal
Journal Name
Nature Communications
Publication Date
Page Number
7555
Volume
6

Ordinary materials can transform into novel phases with new crystal structures at extraordinary high pressure and temperature applied under both equilibrium and non-equilibrium conditions1-6. The recently developed method of ultra-short laser-induced confined microexplosions7-9 extends the range of possible new phases by initiating a highly non-equilibrium plasma state deep inside a bulk material7-12. Ultra-high quenching rates can help to overcome kinetic barriers to the formation of new metastable phases, while the surrounding pristine crystal confines the affected material and preserves it for further study10-12. Here we demonstrate that ultra-rapid pressure release from a completely disordered plasma state in silicon produces several new metastable end phases quenched to ambient conditions. Their structure is determined from comparison to an ab initio random structure search which revealed six new energetically competitive potential phases, four tetragonal and two monoclinic ones. We show the presence of bt8 and st12, which have been predicted theoretically previously13-15, but have not been observed in nature or in laboratory experiments. Additionally, the presence of the as yet unidentified silicon phase, Si-VIII and two of our other predicted tetragonal phases are highly likely within laser-affected zones. These findings pave the way for new materials with novel and exotic properties.