We show that the annihilation dynamics of excited positronium (Ps) atoms can be controlled using parallel electric and magnetic fields. To achieve this, Ps atoms were optically excited to n ¼ 2 sublevels in fields that were adjusted to control the amount of short-lived and long-lived character of the resulting mixed states. Inclusion of the former offers a practical approach to detection via annihilation radiation, whereas the increased lifetimes due to the latter can be exploited to optimize resonance-enhanced two-photon excitation processes (e.g., 1 3 S → 2 3 P → nS=nD), either by minimizing losses through intermediate state decay, or by making it possible to separate the excitation laser pulses in time. In addition, photoexcitation of mixed states with a 2 3 S 1 component represents an efficient route to producing long-lived pure 2 3 S 1 atoms via single-photon excitation. DOI: 10.1103/PhysRevLett.115.183401 PACS numbers: 36.10.Dr, 78.70.Bj Positronium (Ps) is an atomic system composed of an electron bound to a positron and has several unique properties, the most striking of which are its low mass (M Ps ¼ 2m e ) and the fact that it can decay through various annihilation pathways [1]. Electron-positron annihilation requires overlap of the particle wave functions [2] and in Ps is therefore dependent on the square of the radial wave function at the origin. This is zero for states with l > 0 [3]. Higher order annihilation processes can occur for states with l > 0 but are strongly suppressed [4] and in practice direct Ps annihilation occurs only from the ground 1 1 S 0 and 1 3 S 1 , and metastable 2 1 S 0 and 2 3 S 1 levels. The inhibition of Ps annihilation in states with l > 0 is the basis for several proposed schemes to manipulate annihilation rates using resonant and nonresonant laser fields [5][6][7][8][9][10][11]. More complex strategies have also been suggested [12,13], although these have also not yet been experimentally demonstrated.The radiative decay and annihilation time scales in the n ¼ 2 manifold in Ps span an enormous range: The 2 1 S 0 level is radiatively metastable, fluorescing on a time scale of ≃0.24 s [3], but annihilating in 1 ns; conversely the 2 3 P 0;1;2 levels decay by fluorescence to the 1 3 S 1 state in 3.19 ns, but their annihilation lifetimes exceed 100 μs [4]. The 2 3 S 1 level is also metastable and fluoresces in ≃0.24 s, but has an annihilation lifetime of ∼1.14 μs [1]. It is the disparate properties of these states that make the approach described here to manipulating decay rates particularly effective.We report the results of experiments in which Ps annihilation rates in a weak magnetic field are manipulated using parallel electric fields. This combination of fields permits control over the spin multiplicity and orbital angular momentum character of the n ¼ 2 sublevels accessible by single-photon excitation from the 1 3 S 1 ground state. By increasing the 2 1 P character of mixed states in the fields, radiative decay to the short-lived singlet ground state (1 1 S 0 ) can be...