Towards trapping of Rydberg Ps

Atoms and molecules in high Rydberg states can possess large electric dipole moments which can be exploited to control their motion using external electric fields. Ever since the demonstration of deflection of Rydberg Kr atoms using electric fields (, the field of atom optics has been widely investigated. Different techniques such as decelerators [EPJ Techniques and Instrumentation (2016) 3:2], mirrors [Phys. Rev. Lett. 97, 033002 (2006)], and traps [Phys. Rev. Lett. 100, 043001 (2008)] have been developed, however applications to positronium (Ps) are relatively recent. Only a handful of Ps atom optics experiments have been performed to date [Phys. Rev. Lett. 117, 073202 (2016) , Phys. Rev. A 95, 053409 (2017) , Phys. Rev. Lett. 119, 053201 (2017)]. Several Ps experiments can benefit from use of a cold Ps source but, due to the low mass of Ps, speeds are often on the order of 100 km/s when produced in targets like mesoporous silica. Also, using mesoporous silica, the Ps angular distribution during emission is broad and if a well collimated beam is required, significant loss in Ps number is unavoidable. The use of time-varying electric fields generated by a multi-ring structure can offer a solution to these limitations by capturing more emitted Ps and allowing manipulation via their electric dipole moments. Recently, we have developed a multi-ring structure which has been implemented to guide Rydberg Ps atoms using inhomogeneous electric fields, and, in principle, can also be used to decelerate and trap Ps.

The experimental set-up of the target and electrostatic guide including the excitation lasers and the gamma-ray detectors is shown in Figure 1. The Ps producing target is labelled T and the 11 electrodes of the guide are labelled 1, 2, 3,…, 11. Ground state Ps atoms, produced from the silica target, are excited to the n=13 Rydberg level in a two step process by the UV (1S –>2P) and IR (2P–>nD/nS) lasers in the region between T and electrode 1 (E1). Once excited to Rydberg states, Ps atoms have lifetimes on the order of μs, significantly longer than the triplet ground state lifetime of 142 ns. A 500 V/cm electric field, generated by biasing T and E1, Stark splits the Rydberg spectrum [Phys. Rev. Lett. 114, 173001 (2015)], enabling us to select specific states in the Stark manifold by tuning the IR laser wavelength. States selected with positive Stark shift(shorter wavelengths) are called low field seekers (LFS), because of their property to move toward regions of low field. States selected with negative Stark shift (longer wavelengths) are called high field seekers (HFS), because of their property to move toward regions of high field. Any atoms that are able to traverse the guide, LFS or HFS, can then be detected by detectors D2, D3, D4, and D5.

Figure 1: Schematic of the Ps production and excitation chamber. Inset shows the target electrode, T, and guide assembly comprising of 11 electrodes.
Figure 2: Simulated trajectories of atoms in HFS states (red solid lines) and LFS states (white solid lines) of the n=13 Stark manifold, with guide “off” (a) & (b) and “on” (c) & (d)

According to our simulations, see Figure 2, when the guide is not in operation (all electrodes grounded at 0V), the diverging cloud of Ps atoms from the target do not experience any external forces as expected, and therefore annihilate after colliding against the guide electrodes, with only a few forward collimated atoms reaching the end of the guide. If we apply a voltage to alternate electrodes (3,5,7 etc.), this turns the guide on. In this case the HFS states are deflected toward regions of high electric fields (i.e. away from the axis of the guide) while the LFS states are confined axially and transported along the length of the guide. These LFS atoms diverge after exiting the guide and some annihilate due to collisions with the surrounding vacuum chamber. Detectors D2, D3, D4, and D5, as shown in Figure 1, are able to record these annihilation events as time of flight (TOF) spectra, the results of which are shown in figure 3 below.

Figure 3: TOF spectra/annihilation events seen by detectors D2, D3, D4, and D5 for Ps atoms in (a) LFS and (b) HFS states with guide both on and off.

Neither the LFS states nor the HFS are detected at the end of the guide when the guide is off but an increased count rate is seen when both the guide is on and the IR laser is tuned to excite atoms to the LFS states.

To implement this device as a trap, we only have to reconfigure the voltages applied to the electrodes. For guiding, the odd numbered electrodes of the guide have a voltage applied (-4 kV) while the even numbered electrodes are kept at ground potential (0 V). If a positive voltage of order +1 kV is applied to E2 and E4 while E3 is at a potential of -4kV, then a region of electric field minimum is created in the centre of E3 (the voltages applied to the electrodes are based on the choice of n due to the field ionisation limit). Once the atoms have entered the trap, the LFS atoms should be confined in this region until the voltage applied to E4 is lowered,  opening the trap gate for the atoms to be guided towards the detectors. If atoms are trapped and guided out, then the TOF spectra, like in Figure 3(a), is expected to show a peak in events but occurring with a delay consistent with the length of trapping.

In pursuit of cold Ps

Experiments involving positronium (Ps), such as laser excitation for Rydberg state production, precision spectroscopy and positronium chemistry can benefit from a slow Ps source. The technical word for slow is cold. As the mass of positronium is twice the mass of an electron, even room temperature Ps have speeds on the order of 100 km/s. In comparison, atomic beams produced from supersonic jets have speeds of roughly 2 km/s. Atom optics techniques such a decelerating the Ps with electric fields to slow down the atoms may be possible, but at the cost of loss in intensity. An ideal alternative would be to fabricate a target that intrinsically produces slow positronium, and efficiently too.

In most of our experiments, Ps is produced from a mesoporous silica target grown on a silicon substrate. Ps, initially with energy of 1 eV, is emitted from the same side as the positrons enter the converter (“reflection geometry” production) and one can generally obtain Ps with final energy of approximately 50 meV.  Once produced inside granulated powders, such as silica or magnesium oxide (MgO), Ps will lose some of its energy by making collisions with the surrounding internal surfaces before being emitted into vacuum. Generally, more collisions means greater amounts of energy loss, therefore colder Ps. A silica target was fabricated so that the Ps traverses the whole thickness of the target to be emitted out of the opposite side after making the maximum amount of collisions with the internal surfaces (transmission geometry).  However, the internal spacing of this target was too large to efficiently cool Ps below 200 meV (~200 km/s), which is still hotter than Ps emitted from mesoporous silica. Ps can also be produced from MgO, albeit with a slightly higher initial energy of around 4 eV. Previous studies have indicated that this 4 eV energy is reduced down to energies of around 300 meV in a 6 μm thick MgO layer. So, that gave us an idea. If we make a thicker MgO layer to increase collisional cooling, Ps atoms could be produced with energies lower than 50 meV (Positronium emission from MgO smoke nanocrystals).

A scanning electron microscope (SEM) image of smoked MgO.

To make the MgO target, we set fire to a strip of magnesium ribbon and collected the smoke on a suitable substrate (tinted goggles and a fume cupboard are necessary as you might imagine). This procedure produces perfect cubic crystals, in a 30 μm MgO layer, that have a wide size distribution, as evident from the SEM image above. The substrate of our choice was a 50 nm silicon nitride film, as it allows us to implant the positrons into the SiN side, to make positronium in the SiN-MgO boundary, which is then emitted into vacuum from the opposite side in transmission geometry. In this configuration, Ps atoms will travel through the 30 μm thick MgO, making the maximum amount of collisions. For comparison, we can rotate the target by 180° so the positron hits the MgO side (“reflection geometry”) and Ps makes the least amount of collisions, for positrons which are implanted to a relatively shallow depth of only 100 nm. We expect colder Ps to be produced in the former case compared to the latter, due to the distance travelled by the Ps (30 μm vs 100 nm). These two orientations are shown below, including the positron pulse and the excitation lasers. VT and VG refer to voltages applied to the target and grid electrode to control the positron energy and electric field.

Experimental setup showing the target utilised in reflection and transmission geometry.

Once positronium atoms are emitted in either of the two set-ups, they are excited with UV and IR lasers to measure the Doppler profile, which gives an indication of their kinetic energy, KE. In the “reflection geometry” configuration, VT controls how deep into the MgO layer the positrons are implanted. Higher voltages results in deeper implantation, hence larger amount of collisions made by the Ps on their way out and colder Ps. However in the “transmission” set-up, around 2 keV voltage on VT is enough to make the positrons go through the SiN and form Ps in MgO. We found that for the 2 – 5 keV range we measured, positron penetration depths into the MgO layer in transmission set-up were essentially the same, meaning that Ps always travelled through 30 μm of MgO in this configuration. The resultant KE obtained from the Doppler profiles are shown below.

Left: An example of a Doppler profile. Right: Kinetic energies obtained from the Doppler profiles.

Surprisingly, Ps appears to be emitted with the same energy regardless of the amount of collisions it makes with the smoked MgO surfaces. This is inconsistent with the idea that Ps is formed in MgO with 4 eV of energy and reduction in energy takes place due to the collisions. If this is true then we expect KE in reflection set-up, when VT is 1 kV, to be very close to 4 eV. However, Ps kinetic energy is always around 400 meV. This is because Ps, in smoked MgO, is intrinsically produced with around 300 meV of energy with a wide distribution due to the grain sizes, and because of the large open volumes between the MgO crystals, cooling is rather inefficient.

This rules out smoked MgO as a candidate for cold Ps production but there are many experiments where the Ps production and interaction region needs to be separated from the positron beam line. In such experiments, a simple and easily producible MgO target as discussed here, in “transmission geometry” configuration, can be employed where, for example, a scattering gas cell can be installed without interfering with the incoming positrons.

We have also noticed some interesting observations when the lasers are fired into the MgO rather than travelling just in front of the MgO surface. More on that in the next blog post.

Rydberg Positronium-electron scattering

In our last experiment, we showed how a curved quadrupole guide can be used to transport Rydberg Positronium (Ps*) around a 45 degree bend (blue path in picture below) into a region away from the positron beam line (yellow path below), which can then be implemented into a scattering region (PRA 95 053409). In addition, this new off-axis setup eliminated detection difficulties that were encountered in our previous straight guide experiments.

The scattering chamber setup is shown in the right hand side picture below. Guided Ps* atoms emerging from the end of the quadrupole are introduced into a scattering region where they collide with electrons that are thermoinically ejected (orange path) from a Molybdenum filament . This region is surrounded by gamma-ray detectors coupled to photomultiplier tubes (PMT) which record annihilation events inside the chamber. However, these PMTs in themselves are not sufficient to conclude what kind of interaction has taken place, we can only conclude that a Ps atom annihilated if an event is detected, but not if there were intermediate steps (such as charge exchange between the free electrons and the valence electron) before annihilation. To overcome this, we used a micro-channel plate (MCP) which has the benefit of being able to detect only certain charged particles (i.e. differentiating between electrons and positrons) depending on the electric fields applied in the detection region.

When the Ps*collides with free electrons a few different things can happen; the electron could break up the Ps* into electron and positron (ionisation: e^{-} + Ps^{*} \rightarrow e^{-} + e^{+} + e^{-} ) or, the positron from the Ps* will be stolen away by the incoming free electron, resulting in a new short lived Ps which annihilates before hitting the MCP, thus giving a diminished signal (charge exchange: e^{-} + Ps^{*} \rightarrow Ps + e^{-}). Additionally, Positronium and an electron can form a negative Ps ion (Ps¯ ), which is the bound state of a Ps atom and an orbiting electron, this ions have been shown to be quite unstable, having a lifetime of <1ns.

Above you can see some experimental Time of Flight (TOF) data showing the possibility of having detected a charge exchange process. The blue curve on the left panel is a TOF signal of guided Positronium atoms after hitting the MCP detector. The Ps* atoms have a mean flight time of around 10\mus. When we let the electron beam into the scattering region  we observe a suppression of the TOF spectra (green curve), this is due to the electric fields in front of the MCP detector, which should only allow positrons to be detected. The PMT signal for both cases (shown in the right panel) are the same indicating that this drop in MCP signal is in fact electron related, not as a result of less Positronium being guided. All that remains to do now is to determine the nature of this signal but nonetheless, it’s intriguing how readily Ps* interacts with electrons (maybe other particles too), especially when considering that a direct method of producing anti-Hydrogen is via charge exchange collisions between Ps* and antiproton ( Ps^{*} + \overline{p} \rightarrow \overline{H}+ e^{-} ).

Optimizing Positronium Rydberg manipulation

In recent experiments we showed how we successfully manipulated the trajectories of Rydberg Positronium atoms using electric field inside a curved quadrupole guide, which allows us to perform velocity selection on the Positronium atoms that enter the quadrupole field.

These curved guide experiments were performed by exciting Positronium to n = 14, which is a state that has a relatively low mean lifetime of ~8 \mus, which is comparable to the flight time of our experiment, meaning that many of the n = 14 atoms undergo radiative decay before they can be detected. However, when judging what the most efficient n for guiding is, we need to have into consideration a few other factors. The lifetime of different n states goes up as n^3, but the field-ionisation rate goes up as ~n^{-4}, and the dipole moment as n^2. Combining all of these factors and implementing them into trajectory-simulations based on the electric fields generated by the curved guide, we were able to determine that the most efficient n for curved guiding is n = 14, as it can be seen from the graph below.

These simulations agree with our data and were instrumental in determining the optimum parameters of the experiment.

We are currently working on implementing this off-axis curved guide into a scattering experiment using helium ions, below you can see at the bottom of the image the new scattering chamber that has been coupled to the Positronium Rydberg beam.