Positronium emission from mesoporous silica studied by laser-enhanced time-of-flight spectroscopy

The use of mesoporous silica films for the production and study of positronium (Ps) atoms has become increasingly important in recent years, providing a robust source of free Ps in vacuum that may be used for a wide variety of experiments, including precision spectroscopy and the production of antihydrogen. The ability of mesoporous materials to cool and confine Ps has also been utilized to conduct measurements of Ps–Ps scattering and Ps2 molecule formation, and this approach offers the possibility of making a sufficiently dense and cold Ps ensemble to realize a Ps Bose–Einstein condensate. As a result there is great interest in studying the dynamics of Ps atoms inside such mesoporous structures, and how their morphology affects Ps cooling, diffusion and emission into vacuum. It is now well established that Ps atoms are initially created in the bulk of such materials and are subsequently ejected into the internal voids with energies of the order of 1 eV, whereupon they rapidly cool via hundreds of thousands of wall collisions. This process can lead to thermalisation to the ambient sample temperature, but will be arrested when the Ps deBroglie wavelength approaches the size of the confining mesopores. At this point diffusion through the pore network can only proceed via tunneling, at a much slower rate. An important question then becomes, how long does it take for the Ps atoms to cool and escape into vacuum? In a direct measurement of this process, conducted using laser-enhanced positronium time-of-flight spectroscopy, we show that cooling to the quantum confinement regime in a film with approximately 5 nm diameter pores is nearly complete within 5 ns, and that emission into vacuum takes ~10 ns when the incident positron beam energy is 5 keV. The observed dependence of the Ps emission time on the positron implantation energy supports the idea that quantum confined Ps does not sample all of the available pore volume, but rather is limited to a subset of the mesoporous network

Selective Production of Rydberg-Stark States of Positronium

Rydberg positronium (Ps) atoms have been prepared in selected Stark states via two-step (1s→2p→nd/ns) optical excitation. Two methods have been used to achieve Stark-state selection: a field ionization filter that transmits the outermost states with positive Stark shifts, and state-selected photoexcitation in a strong electric field. The former is demonstrated for n=17 and 18 while the latter is performed for n=11 in a homogeneous electric field of 1.9  kV/cm. The observed spectral intensities and their dependence on the polarization of the laser radiation are in agreement with calculations that include the perturbations of the intermediate n=2 manifold. Our results pave the way for the generation of Rydberg Ps atoms with large electric dipole moments that are required for the realization of schemes to control their motion using inhomogeneous electric fields, an essential feature of some proposed Ps free-fall measurements requiring focused beams of long-lived atoms

Single-shot positron annihilation lifetime spectroscopy with LYSO scintillators

We have evaluated the application of a lutetium yttrium oxyorthosilicate (LYSO) based detector to single-shot positron annihilation lifetime spectroscopy. We compare this detector directly with a similarly configured PbWO4 scintillator, which is the usual choice for such measurements. We find that the signal to noise ratio obtained using LYSO is around three times higher than that obtained using PbWO4 for measurements of Ps excited to longer-lived (Rydberg) levels, or when they are ionized soon after production. This is due to the much higher light output for LYSO (75% and 1% of NaI for LYSO and PbWO4 respectively). We conclude that LYSO is an ideal scintillator for single-shot measurements of positronium production and excitation performed using a low-intensity pulsed positron beam

Positronium emission from mesoporous silica studied by laser-enhanced time-of-flight spectroscopy

The use of mesoporous silica films for the production and study of positronium (Ps) atoms has become increasingly important in recent years, providing a robust source of free Ps in vacuum that may be used for a wide variety of experiments, including precision spectroscopy and the production of antihydrogen. The ability of mesoporous materials to cool and confine Ps has also been utilized to conduct measurements of Ps–Ps scattering and Ps2 molecule formation, and this approach offers the possibility of making a sufficiently dense and cold Ps ensemble to realize a Ps Bose–Einstein condensate. As a result there is great interest in studying the dynamics of Ps atoms inside such mesoporous structures, and how their morphology affects Ps cooling, diffusion and emission into vacuum. It is now well established that Ps atoms are initially created in the bulk of such materials and are subsequently ejected into the internal voids with energies of the order of 1 eV, whereupon they rapidly cool via hundreds of thousands of wall collisions. This process can lead to thermalisation to the ambient sample temperature, but will be arrested when the Ps deBroglie wavelength approaches the size of the confining mesopores. At this point diffusion through the pore network can only proceed via tunneling, at a much slower rate. An important question then becomes, how long does it take for the Ps atoms to cool and escape into vacuum? In a direct measurement of this process, conducted using laser-enhanced positronium time-of-flight spectroscopy, we show that cooling to the quantum confinement regime in a film with approximately 5 nm diameter pores is nearly complete within 5 ns, and that emission into vacuum takes ~10 ns when the incident positron beam energy is 5 keV. The observed dependence of the Ps emission time on the positron implantation energy supports the idea that quantum confined Ps does not sample all of the available pore volume, but rather is limited to a subset of the mesoporous network

Formation of positron-atom bound states in collisions between Rydberg Ps and neutral atoms

Predicted 20 years ago, positron binding to neutral atoms has not yet been observed experimentally. A scheme is proposed to detect positron-atom bound states by colliding Rydberg positronium (Ps) with neutral atoms. Estimates of the charge-transfer reaction cross section are obtained using the first Born approximation for a selection of neutral atom targets and a wide range of incident Ps energies and principal quantum numbers. We also estimate the corresponding Ps ionization cross section. The accuracy of the calculations is tested by comparison with earlier predictions for charge transfer in Ps collisions with hydrogen and antihydrogen. We describe an existing Rydberg Ps beam suitable for producing positron-atom bound states and estimate signal rates based on the calculated cross sections and realistic experimental parameters. We conclude that the proposed methodology is capable of producing such states and of testing theoretical predictions of their binding energies

Measurement of Rydberg positronium fluorescence lifetimes

We report measurements of the fluorescence lifetimes of positronium (Ps) atoms with principal quantum numbers n=10–19. Ps atoms in Rydberg-Stark states were produced via a two-color two-step 1S3→2P3→nS3/nD3 excitation scheme and subsequently detected after traveling 1.2 m. The measured time-of-flight distributions were used to determine the mean lifetimes of the Rydberg levels, yielding values ranging from 3μs to 26μs. Our data are in accord with the expected radiative lifetimes of Rydberg-Stark states of Ps

Positronium decay from n=2 states in electric and magnetic fields

We report measurements and the results of calculations demonstrating that the annihilation dynamics of positronium (Ps) atoms can be controlled by Stark and Zeeman mixing of optically excited states. In the experiments a trap-based pulsed positron beam was employed to generate a dilute Ps gas with a density of ∼107 cm−3 using a porous silica target. These atoms were excited via 13S1→23PJ transitions in parallel electric and magnetic fields using a nanosecond pulsed dye laser, and Ps annihilation was measured using single-shot lifetime spectroscopy. The composition of the excited n=2 sublevels was controlled by varying the polarization of the excitation laser radiation and the strength of the electric and magnetic fields in the excitation region. The overall decay rates of the excited states can vary by a large amount, owing to the enormous differences between the annihilation and florescence lifetimes of the accessible field-free states. The energy-level structure, spectral intensities, and florescence and annihilation lifetimes in the presence of the fields were determined from the eigenvalues and eigenvectors of the complete n=2 Hamiltonian matrix in an |nSℓJMJ⟩ basis. Using these data as the input to a Monte Carlo model yielded calculated values which could be compared with experimentally measured quantities; qualitative agreement with the measurements was found. Varying the electric field in the presence of a weak parallel magnetic field provides control over the amount of level mixing that occurs, making it possible to increase or decrease the Ps lifetime. Field-controlled Ps decay can be used as an ionization-free detection method. Conversely, increasing the excited-state lifetime can potentially be exploited to optimize multistep excitation processes using mixed intermediate states. This will be useful either in minimizing losses through intermediate-state decay during excitation or by making it possible to separate excitation laser pulses in time. In addition, the adiabatic extraction of appropriate eigenstates from the electric field in which they are excited can, in principle, be used to prepare pure 23S1 atoms. The availability of atoms in these states produced via single-photon excitation will facilitate high-resolution microwave spectroscopy of the Ps n=2 fine structure

Electrostatically Guided Rydberg Positronium

We report experiments in which positronium (Ps) atoms were guided using inhomogeneous electric fields. Ps atoms in Rydberg-Stark states with principal quantum number n=10 and electric dipole moments up to 610 D were prepared via two-color two-photon optical excitation in the presence of a 670  V cm−1 electric field. The Ps atoms were created at the entrance of a 0.4 m long electrostatic quadrupole guide, and were detected at the end of the guide via annihilation gamma radiation. When the lasers were tuned to excite low-field-seeking Stark states, a fivefold increase in the number of atoms reaching the end of the guide was observed, whereas no signal was detected when high-field-seeking states were produced. The data are consistent with the calculated geometrical guide acceptance

Positronium production in cryogenic environments

We report measurements of positronium (Ps) formation following positron irradiation of mesoporous SiO2 films and Ge(100) single crystals at temperatures ranging from 12–700 K. As both of these materials generate Ps atoms via nonthermal processes, they are able to function as positron-positronium converters at cryogenic temperatures. Our data show that such Ps formation is possibly provided the targets are not compromised by adsorption of residual gas. In the case of SiO2 films, we observe a strong reduction in the Ps formation efficiency following irradiation with UV laser light (λ=243.01 nm) below 250 K, in accordance with previous observations of radiation-induced surface paramagnetic centers. Conversely, Ps emission from Ge is enhanced by irradiation with visible laser light (λ=532 nm) via a photoemission process that persists at cryogenic temperatures. Both mesoporous SiO2 films and Ge crystals were found to produce Ps efficiently in cryogenic environments. Accordingly, these materials are likely to prove useful in several areas of research, including Ps mediated antihydrogen formation conducted in the cold bore of a superconducting magnet, the production of Rydberg Ps for experiments in which the effects of black-body radiation must be minimized, and the utilization of mesoporous structures that have been modified to produce cold Ps atoms

Velocity selection of Rydberg positronium using a curved electrostatic guide

We report experiments in which a slow Rydberg positronium (Ps) beam was produced by velocity selection using a curved electrostatic quadrupole guide. Ps atoms in Rydberg-Stark states with principal quantum number n = 14 were prepared by a two-color optical excitation process in a uniform electric field. Low-field-seeking Stark states were produced at the entrance of a 0.6-m-long quadrupole guide that includes a 45◦ bend, and were detected at the end of the guide via their annihilation γ radiation. The mean speed (kinetic energy) of atoms entering the guide was estimated to be ≈180 km s−1 (185 meV), whereas the mean longitudinal speed of guided atoms was measured via time of flight and found to be ≈90 km s−1, equivalent to a kinetic energy of 45 meV. The measured transport data are in broad agreement with Monte Carlo simulations, which are also used to establish the efficacy with which the arrangement we describe could be used to perform Ps-atom scattering measurements