Understanding the transfer of spin angular momentum is essential in modern magnetism research. A model case is the generation of magnons in magnetic insulators by heating an adjacent metal film. Here, we reveal the initial steps of this spin Seebeck effect with <27 fs time resolution using terahertz spectroscopy on bilayers of ferrimagnetic yttrium iron garnet and platinum. Upon exciting the metal with an infrared laser pulse, a spin Seebeck current js arises on the same ~100 fs time scale on which the metal electrons thermalize. This observation highlights that efficient spin transfer critically relies on carrier multiplication and is driven by conduction electrons scattering off the metal–insulator interface. Analytical modeling shows that the electrons’ dynamics are almost instantaneously imprinted onto js because their spins have a correlation time of only ~4 fs and deflect the ferrimagnetic moments without inertia. Applications in material characterization, interface probing, spin-noise spectroscopy and terahertz spin pumping emerge.

The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adma.201803054.Among the exceptional properties of lead halide perovskites (LHPs) is the ultraslow cooling of hot carriers. Carrier densities below the Mott density for large polarons (≤ ≈10 18 cm −3 ) are focused on here. As in other semiconductors, a nascent hot electron distribution initially cools down via emission of longitudinal optical (LO) phonons on the 10 −14 -10 −13 s timescale. What distinguishes LHPs from conventional semiconductors is the exceptionally efficient screening in the former. The dielectric screening in LHPs on the 10 −13 s timescale results in an order-of-magnitude reduction in the Coulomb potential upon the formation of a large polaron, likely with ferroelectric-like local ordering. Further LO-phonon emission is inhibited, and this leads to partial retention of hot electron energy on the 10 −12 s timescale, more so in hybrid LHPs than in their all-inorganic counterparts. Further cooling of hot polarons occurs on the 10 −10 s timescale, and this can be attributed to the slow diffusion of heat out of the large polaron volume due to the low thermal conductivity of LHPs. Like other carrier properties, slow hot carrier cooling in LHPs can be intimately related to efficient screening in a soft, anharmonic, and dynamically disordered lattice.

Lead halide perovskites (LHPs) are solution processable semiconductors characterized by long carrier lifetimes. Recent studies have suggested that electrons and holes in LHPs interact with phonons to form large polarons on subpicosecond time-scales and polaron formation may also slow down hot carrier cooling. Using femtosecond time-resolved two-photon photoemission (TR-2PPE) and transient reflectance (TR) spectroscopies, we follow the initial electron cooling and polaron formation dynamics in single-crystal CsPbBr 3 perovskite. We find that the hot electrons cool down initially (≤0.2 ps) with rates of −0.64 ± 0.06 eV/ps and −0.82 ± 0.08 eV/ps at 300 and 80 K, respectively. This weakly temperature-dependent rate is attributed to the initial relaxation of unscreened hot electrons by the emission of longitudinal optical (LO) phonons. On longer time scales, we observe dynamic changes in the photoemission cross-section and in the red-shift of the optical bandgap. We attribute these dynamic changes to large polaron formation from electron−LO phonon interaction, with temperature-dependent polaron formation time constants of τ p = 0.7 ± 0.1 and 2.1 ± 0.2 ps at 300 and 80 K, respectively. The increase in polaron formation rate with temperature is correlated with the broadening in phonon resonances, suggesting that phonon disorder and dephasing facilitate large-polaron formation. The large polaron formation rate is not competitive with the cooling rate of unscreened hot electrons in CsPbBr 3 , in contrast to hybrid CH 3 NH 3 PbBr 3 (or CH 3 NH 3 PbI 3 ) where the two rates are similar. This contrast explains the observation of long-lived hot carriers in the latter but not the former.

Ultrafast heating of a ferrimagnet’s crystal lattice leads to a new state of matter with hot spins yet unchanged magnetization.