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arXiv:2505.05750 · Physical Review A

Selective ionization of Rydberg atoms to reduce the energy spread of a cold-atom focused ion beam

Kaih T. Mitchell, Allan Pennings, Rory W. Speirs, Christopher J. Billington, Andrew J. McCulloch, A. A. Wood, Robert E Scholten

Published Jul 17, 2025• 3 citations
arXivHTMLPDF

Abstract

The energy spread of a focused ion beam causes chromatic aberration that limits the focal spot size and resolution for imaging and fabrication. Ion beams based on photoionization of neutral atoms can have a much smaller energy spread and higher brightness than conventional liquid metal ion sources and are thus capable of higher resolution. We present a method for using selective ionization of Rydberg atoms to reduce the beam energy spread in a cold-atom focused ion beam. We produce experimental maps of the ionization rate of $^{85}\mathrm{Rb}$ near the classical ionization threshold, predict the energy spread of an ion beam produced from these states, and demonstrate energy spread reduction in situ in a focused ion beam. We use a novel method to measure the energy spread from images, using only components present in many commercial focused ion beam systems. We choose two states to illustrate the technique and show a 50% difference in energy spread, with opportunities to further reduce the energy spread by constructing a more favorable electric field gradient and finding atomic states with better ionization characteristics.

DOI
10.1103/r7g8-ws2t

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The energy spread of a focused ion beam causes chromatic aberration that limits the focal spot size and resolution for imaging and fabrication. Ion beams based on photoionization of neutral atoms can have a much smaller energy spread and higher brightness than conventional liquid metal ion sources and are thus capable of higher resolution. We present a method for using selective ionization of Rydberg atoms to reduce the beam energy spread in a cold-atom focused ion beam. We produce experimental maps of the ionization rate of 85Rb^{85}\mathrm{Rb}85Rb near the classical ionization threshold, predict the energy spread of an ion beam produced from these states, and demonstrate energy spread reduction in situ in a focused ion beam. We use a novel method to measure the energy spread from images, using only components present in many commercial focused ion beam systems. We choose two states to illustrate the technique and show a 50% difference in energy spread, with opportunities to further reduce the energy spread by constructing a more favorable electric field gradient and finding atomic states with better ionization characteristics.
The authors describe a new method for creating a high quality focused ion beam using laser-cooled neutral atoms in a magneto-optical trap as an ion source. They show that this new technique can provide spot resolutions and brightness values that are better than the state of the art in focused ion beams. The source can be used with a range of different ionic species and can be combined with laser cooling techniques to exert unprecedented control over the ion emission, for example, producing single ions “on demand.” The beam quality is a result of a high brightness and a narrow energy distribution, both of which stem from the cold temperature (≈100μK) of the atoms. The ions are produced by subjecting the cold neutral atoms to a photoionization laser, after which they become a compact source of nearly monoenergetic ions. With the application of a potential gradient, the ions form a beam that can be focused via standard ion optical techniques. They discuss estimations based on the initial size of the ion cloud and the energy distribution and show that the resulting beam has a low emittance.
We present an ionization mechanism for use in a cold atom electron source with the goal of producing highly monochromatic electron beams. We experimentally produce a map of the Stark states of 85Rb^{85}\mathrm{Rb}85Rb below the ionization threshold and identify states that undergo selective field ionization. The properties of an electron beam produced by field-assisted ionization of such states are quantified. A theoretical framework is established to predict the improvement to beam quality when ionization is conducted above the ionization threshold, where ionization conditions are typically more favorable than below the threshold. Calculations suggest that selective ionization of Rydberg states may offer a pathway to the production of high-brightness, highly monochromatic ion and electron beams.
At present, the smallest spot size which can be achieved with state-of-the-art focused ion beam (FIB) technology is mainly limited by the chromatic aberrations associated with the 4.5 eV energy spread of the liquid-metal ion source. Here we numerically investigate the performance of an ultracold ion source which has the potential for generating ion beams which combine high brightness with small energy spread. The source is based on creating very cold ion beams by near-threshold photoionization of a laser-cooled and trapped atomic gas. We present ab initio numerical calculations of the generation of ultracold beams in a realistic acceleration field and including all Coulomb interactions, i.e., both space charge effects and statistical Coulomb effects. These simulations demonstrate that with existing technology reduced brightness values exceeding 105 A m−2 sr−1 V−1 are feasible at an energy spread as low as 0.1 eV. The estimated spot size of the ultracold ion source in a FIB instrument ranges from 10 nm at a current of 100 pA to 0.8 nm at 1 pA.
The energy distribution of an ultracold rubidium ion beam, which is intended to be used as the source for a focused ion beam instrument, is measured with a retarding field analyzer. The ions are created from a laser-cooled and compressed atomic beam by two-step photoionization in which the ionization laser power is enhanced in a build-up cavity. Particle tracing simulations are performed to ensure the analyzer is able to resolve the distribution. The lowest achieved full width 50% energy spread is (0.205±0.006)\left(0.205\pm0.006\right)(0.205±0.006) eV. The energy spread originates from the variation in the ionization position of the ions which are created inside an extraction electric field. This extraction field is essential to limit disorder-induced heating which can decrease the ion beam brightness. The ionization position distribution is limited by a tightly focused excitation laser beam. Energy distributions are measured for various ionization and excitation laser intensities and compared with calculations based on numerical solutions of the optical Bloch equations including ionization. A good agreement is found between measurements and calculations.
High-brightness ion sources are important for several applications such as focussed ion beam (FIB) systems, in which an ion beam is focussed on a sample to a spot size of a few nanometer. These systems have become an important tool in a wide array of material science and technological applications because they offer both high-resolution imaging as well as micromachining capabilities. The resolution in the most common FIB system, the Gallium-Liquid Metal Ion Source (Ga-LMIS) based FIB, is limited by chromatic aberrations in the lens column due to the energy spread of o2 eV. To reach a higher resolution, a high-brightness ion source is needed with a lower energy spread. In this thesis such a new source is presented, the ultra-cold ion source (UCIS) based on the photo-ionization of a laser-cooled atomic gas confined in a magneto-optical trap. The low temperature (_ 150 µK) of the source makes it possible to reach high-brightness with an extended source size. The charge density at the source is thereby reduced compared to sources with a sharp tip, such as the LMIS, and thus also the Coulombic interactions that deteriorate the beam and increase the longitudinal energy spread. Additionally many different atomic species can be laser-cooled, making the UCIS a versatile source for both heavy and light ion species. Light ion species such as Li are very suitable for imaging purposes without directly damaging the sample. Heavy ion species on the other hand, can be used for manipulation of a sample by sputtering away material at a small scale. A analytical model has been developed to estimate the initial source performance. The extractable current from the ionization volume is estimated based on the influx of atoms, which depends on temperature and atomic density. According to the model, the energy spread oU is proportional to the finite length of the ionization volume, limited by the size of the laser focus waist, and the acceleration field E0. To study the influence of the ionic interactions in the beam in more detail, particle tracking simulations have been performed which take all mutual Coulombic interaction into account under realistic experimental conditions. From these simulations we learned that when the current is increased, the brightness is lowered due to increased stochastic heating. Beam currents between 1 and 100 pA are feasible, with an energy spread much lower than that of the LMIS. At 1 pA the source has a peak brightness up to Br = 8 × 104 Am-2sr-1 with an energy spread _U = 0.08 eV. At 10 pA it has a brightness up to Br = 2 × 104 Am-2sr-1 with an energy spread oU = 0.14 eV. An experimental setup has been built, consisting of a rubidium magneto-optical trap inside a cylindrically symmetric accelerator structure. By using a two-step photo-ionization process, a small fraction of the cold atoms in the cross-section of two laser beams is ionized. A pulsed ionization laser was used to produce ion bunches. A short beam line with a multichannel plate detector was used to obtain both the temporal and the transverse spatial profileof the bunches. Time-of-flight measurements have been performed to characterize the longitudinal energy spread of the beam as function of the beam energy U. We have demonstrated, as predicted by the model, that the energy spread oU is indeed due to the length of the ionization volume in the acceleration field. By lowering the extraction field, well defined beams with an average energy of only 1 eV have been produced with an energy spread as low as 20 meV, more than two orders of magnitude lower than the LMIS. A transition from ballistic behavior at high beam energies, where oU / U, to a space-charge dominated regime at low beam energies, where oU / pU, has been observed. In the cross-over region an interesting new effect has been observed in which the space charge forces reduce the energy spread. The experimental results agree well with detailed particle tracking simulations. The combination of well-defined ion beams at low energy and time-dependent acceleration fields opens new possibilities. Precise manipulation of the bunch distribution in both longitudinal and transverse phase space has been demonstrated. Reduction of the longitudinal energy spread has been realized by switching the accelerator field off before the ions have had a chance to leave the accelerating structure. A reduction by a factor 3 is achieved, which is limited by the inhomogeneity of the field. Calculations show that much stronger reduction is achievable in a more homogenous acceleration field. This would make low-energy spread possible without the need to go to small _z0 and E0, enabling even lower energy spread. We also demonstrated that the accelerator structure, which normally acts as a fixed negative lens, can be transformed into a versatile lens by using time-dependent fields. Control over the focal length and sign, as well as the sign and strength of the spherical aberrations can be obtained by tailoring the applied time-dependent acceleration voltage. The possibility to create a negative spherical aberration may be used to correct for the spherical aberrations in the focal columns which are presently limiting the spatial resolution of FIBs. The dependence of the properties of this lens on the parameters of the applied tri-polar pulse has been studied in detail, both experimentally and with particle tracking simulations, which are in good agreement. Finally, based on lessons learned, the design of a next generation UCIS is briefly discussed, based on photo-ionization of a laser cooled and intensified atomic beam. The principle is similar as an UCIS based on a MOT, but with a higher current density. Calculations show that this source should be able to produce orders of magnitude brighter beams in a more compact configuration. With this new design it should be possible to beat the LMIS not only in energy spread but now also in brightness.