Ultrafast negative thermal expansion driven by spin-disorder

We measure the transient strain profile in a nanoscale multilayer system composed of Yttrium, Holmium and Niobium after laser excitation using ultrafast X-ray diffraction. The strain propagation through each layer is determined by transient changes of the material-specific Bragg angles. We experimentally derive the exponentially decreasing stress profile driving the strain wave and show that it closely matches the optical penetration depth. Below the Neel temperature of Ho, the optical excitation triggers negative thermal expansion, which is induced by a quasi-instantaneous contractive stress, and a second contractive stress contribution rising on a 12 ps timescale. These two timescales have recently been measured for the spin-disordering in Ho [Rettig et al, PRL 116, 257202 (2016)]. As a consequence we observe an unconventional bipolar strain pulse with an inverted sign travelling through the heterostructure.