Ultrafast lattice disordering can be accelerated by electronic collisional forces

In the prevalent picture of ultrafast structural phase transitions, atomic motion occurs in a slowly varying potential energy surface adiabatically determined by fast electrons. However, this ignores non-conservative forces caused by electron–lattice collisions, which can substantially influence atomic motion. Most ultrafast techniques only probe the average structure and are less sensitive to random displacements and therefore do not detect the role played by non-conservative forces in phase transitions. Here we show that the lattice dynamics of the prototypical insulator–metal transition of vanadium dioxide cannot be described by potential energy alone. We use the sample temperature to control the preexisting lattice disorder before ultrafast photoexcitation across the phase transition and our ultrafast diffuse scattering experiments show that the fluctuations characteristic of rutile metal develop equally fast (120 fs) at initial temperatures of 100 and 300 K. This indicates that additional non-conservative forces are responsible for the increased lattice disorder. These results highlight the need for more sophisticated descriptions of ultrafast phenomena beyond the Born–Oppenheimer approximation as well as ultrafast probes of spatial fluctuations beyond the average unit cell measured by diffraction.

Duke Scholars

Author Olivier Delaire Thomas Lord Department of Mechanical Engineering and Materia ...