The mechanism of electron pairing in high-temperature superconductors is still the subject of intense debate. Here, we provide direct evidence of the role of structural dynamics, with selective atomic motions (buckling of copper-oxygen planes), in the anisotropic electron-lattice coupling. The transient structures were determined using time-resolved electron diffraction, following carrier excitation with polarized femtosecond heating pulses, and examined for different dopings and temperatures. The deformation amplitude reaches 0.5% of the c axis value of 30 Å when the light polarization is in the direction of the copper-oxygen bond, but its decay slows down at 45°. These findings suggest a selective dynamical lattice involvement with the anisotropic electronphonon coupling being on a time scale (1-3.5 ps depending on direction) of the same order of magnitude as that of the spin exchange of electron pairing in the high-temperature superconducting phase.electron diffraction ͉ electron-phonon coupling ͉ superconductivity ͉ ultrafast T he pairing of electrons is now accepted as being essential in the formation of the superconducting condensate in hightemperature superconductors. What is debatable is the nature of forces (''glue'') holding the pairs (1). The mechanism is different from that of conventional superconductors; for them, loss of the electric resistance is due to phonon-mediated electron pairing [Bardeen-Cooper-Schrieffer (BCS)] (2). Ceramic cuprates become superconductors when extra holes or electrons are doped into their magnetically ordered charge-transfer insulator (ground) state (3, 4); the highest transition temperature (T c ) occurs at a doping of 0.15 extra hole per copper ion and it increases with the number (n) of CuOO planes per unit cell, reaching a maximum at n ϭ 3 (5). Because of the d-wave symmetry of the superconducting gap (6), the relatively small isotope effect (7,8), and the magnitude of electron repulsion (U) and exchange (J) (appropriate for the antiferromagnetic phase), magnetic interactions have been considered as the source of binding (1, 9). The role of phonons in pairs formation has also been discussed, from both experimental and theoretical perspectives (10, 11).Angle-resolved photoemission spectroscopy (ARPES) experiments revealed the presence of kinks in the band dispersion at energies corresponding to specific (optical) phonon modes (7,(11)(12)(13). In some samples, inelastic neutron scattering data at similar energies supported a magnetic resonance mode below the transition temperature (14). The issue was raised over whether the low-energy features observed in the ARPES spectra are induced by magnetic or structural bosonic coupling. Based on energetics, the out-of-plane motion of the oxygen ions in the CuOO plane, referred to as the out-of-plane buckling mode, has been assigned as responsible for the kink in the band dispersion observed along the direction of CuOO bonds (11,12). However, the electron-phonon coupling strength obtained by means of angle-integrated probes is no...