Transient phonon vacuum squeezing due to femtosecond-laser-induced bond hardening

Ultrashort optical pulses can be used both to create fundamental quasiparticles in crystals and to change their properties. In noble metals, femtosecond lasers induce bond hardening, but little is known about its origin and consequences. Here we simulate ultrafast laser excitation of silver at high fluences. We compute laser-excited potential-energy surfaces by all-electron ab initio theory and analyze the resulting quantum lattice dynamics. We also consider incoherent lattice heating due to electron-phonon interactions using the generalized two-temperature model. We find phonon hardening, which we attribute to the excitation of s electrons. We demonstrate that this may result in phonon vacuum squeezed states with an optimal squeezing factor of ~ 0.001 at the L-point longitudinal mode. This finding implies that ultrafast laser-induced bond hardening may be used as a tool to manipulate the quantum state of opaque materials, where, so far, the squeezing of phonons below the zero-point motion has only been realized in transparent crystals by a different mechanism. On the basis of our finding, we further propose a method for directly measuring bond hardening.