One of the great successes of quantum physics is the description of the long-lived Rydberg states of atoms and ions. The Bohr model is equally applicable to donor impurity atoms in semiconductor physics, where the conduction band corresponds to the vacuum, and the loosely bound electron orbiting a singly charged core has a hydrogen-like spectrum according to the usual Bohr-Sommerfeld formula, shifted to the far-infrared because of the small effective mass and high dielectric constant. Manipulation of Rydberg states in free atoms and ions by single and multiphoton processes has been tremendously productive since the development of pulsed visible laser spectroscopy. The analogous manipulations have not been conducted for donor impurities in silicon. Here, we use the FELIX pulsed free electron laser to perform time-domain measurements of the Rydberg state dynamics in phosphorus-and arsenicdoped silicon and we have obtained lifetimes consistent with frequency domain linewidths for isotopically purified silicon. This implies that the dominant decoherence mechanism for excited Rydberg states is lifetime broadening, just as for atoms in ion traps. The experiments are important because they represent a step toward coherent control and manipulation of atomic-like quantum levels in the most common semiconductor and complement magnetic resonance experiments in the literature, which show extraordinarily long spin lattice relaxation times-key to many well known schemes for quantum computing qubits-for the same impurities. Our results, taken together with the magnetic resonance data and progress in precise placement of single impurities, suggest that doped silicon, the basis for modern microelectronics, is also a model ion trap.coherence ͉ free electron laser ͉ quantum information ͉ picosecond population dynamics ͉ hydrogenic donor impurity H omogenous lifetime-broadened two-level atoms in ion traps (1) have become favorite objects of study for quantum optics with a view toward both fundamental physics and the eventual development of a quantum computer. Among the many schemes proposed (2), the states of ions in trap systems are attractive for the realization of quantum information ''qubits'' (quantum bits) because they are well isolated from the decohering effects of the environment and can be coherently controlled by lasers. The Bohr model is equally applicable to donor impurity atoms in semiconductor physics, where the conduction band corresponds to the vacuum, and the loosely bound electron orbiting a singly charged core has a hydrogen-like spectrum according to the usual Bohr-Sommerfeld formula, shifted to the far-infrared because of the small effective mass and high dielectric constant. As with atoms in traps the ground states are tightly confined and well isolated from the environment, giving rise to extraordinarily sharp transitions (3-5) and very long spin coherence times (6, 7), measured with magnetic resonance experiments. There are several proposals for quantum information processing based on the spin of silicon do...