In an anharmonic crystal, large-amplitude vibrational fluctuations on the scale of the lattice spacing can develop frequencies that do not resonate with the normal modes, causing energy to become trapped in intrinsically localized modes (ILMs)--also called 'discrete breathers' or 'lattice solitons'. This mechanism has been observed in analogous systems on a larger scale, but unambiguous sightings in atomic lattice vibrations, where quantum mechanics may play a role, have proved difficult. Two challenges have hampered progress: (1) the need to separate ILMs from defect modes, and (2) complications that arise at high temperatures, including feature broadening and multiphonon processes. Here we solve these problems by using x-ray and neutron scattering to induce ILM-forming amplitude fluctuations in uranium at low temperatures, thereby creating nonequilibrium ILMs. Creation of ILMs occurs at a discrete energy, indicating an unexpected quantum character to ILM formation and greatly simplifying detection