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Magnetic phenomena are ubiquitous in our surroundings and indispensable for modern science and technology, but it is notoriously difficult to change the magnetic order of a material in a rapid way. However, if a thin nickel film is subjected to ultrashort laser pulses, it can lose its magnetic order almost completely within merely femtosecond times. This phenomenon, in the meantime also observed in many other materials, has connected magnetism with femtosecond optics in an efficient, ultrafast and complex way, offering opportunities for rapid information processing or ultrafast spintronics at frequencies approaching those of light. Consequently, the physics of ultrafast demagnetization is central to modern material research, but a crucial question has remained elusive: If a material loses its magnetization within only femtoseconds, where is the missing angular momentum in such short time? Here we use ultrafast electron diffraction to reveal in nickel an almost instantaneous, long-lasting, non-equilibrium population of anisotropic high-frequency phonons that appear as quickly as the magnetic order is lost. The anisotropy plane is perpendicular to the direction of the initial magnetization and the atomic oscillation amplitude is 2 pm. We explain these observations by means of circularly polarized phonons that quickly absorb the missing angular momentum of the spin system before the slower onset of a macroscopic sample rotation. The time that is needed for demagnetization is related to the time it takes to accelerate the atoms. These results provide an atomistic picture of ultrafast demagnetization under adherence to all conservation laws but also demonstrate the general importance of polarized phonons for non-equilibrium dynamics and provide innovative ways for controlling materials on atomic dimensions.
Chiral phonons are the ones with nonzero polarization and can be observed only via a selective coupling with valley electrons and circularly polarized photons. In such process, a new physical quantity, i.e., pseudo-angular momentum (PAM), is required
We have studied ultrafast photoinduced demagnetization in GaMnAs via two-color time-resolved magneto-optical Kerr spectroscopy. Below-bandgap midinfrared pump pulses strongly excite the valence band, while near-infrared probe pulses reveal sub-picose
Spin and orbital angular momenta are two intrinsic properties of an electron and are responsible for the physics of a solid. How the spin and orbital evolve with respect to each other on several hundred femtoseconds is largely unknown, but it is at t
We use femtosecond time-resolved hard x-ray scattering to detect coherent acoustic phonons excited during ultrafast laser demagnetization of bcc Fe films. We determine the lattice strain propagating through the film through analysis of the oscillatio
We group materials into five symmetry classes and determine in which of these classes phonons carry angular momentum in the Brillouin zone, away from a high-symmetry point, line, or plane. In some materials phonons acquire angular momentum via the fo