This work has been funded by a public grant from the French National Research Agency (ANR) under the “France 2030” investment plan, which has the reference EUR MANUTECH SLEIGHT - ANR-17-EURE-0026. ; International audience ; The effect of femtosecond laser shock peening on a model Al-0.3Mn alloy was investigated experimentally and numerically by molecular dynamics. Micro-diffraction experiments performed at synchrotron source revealed the depth profiles of the residual stress and the stored energy of dislocations, a measure of local plasticity. The depth of the maximum compressive stress did not coincide with that of the maximum dislocation energy, which was found at the surface. The interaction between the laser and the metal was simulated with LAMMPS using a two-temperature molecular dynamics package. The model accurately described the equation of state of aluminum and showed nearly equal resolved shear stresses on all slip systems at the wavefront. The dislocation density at a depth of 1 μm, predicted by the Meyers' model [1], was higher than the experimental data, suggesting possible recovery due to the increased temperature of the sample after repeated shock loading.