Two-step Photoionization Research Articles

Trapping Ba+ with seven-fold enhanced efficiency utilizing an autoionizing resonance

Trapped ions have emerged as a front runner in quantum information processing due to their identical nature, all-to-all connectivity, and high fidelity quantum operations. As current trapped ion technologies are scaled, it will be important to improve the efficiency of loading ions, especially when working with long chains of ions or rare isotopes. Here, we compare two different isotope-selective photoionization schemes for loading 138Ba+ ions. We show that a two-step photoionization scheme ending in an autoionizing transition increases the ion loading rate nearly an order of magnitude compared to an established technique which does not excite an autoionizing state. Our novel photoionization scheme can be extended to all isotopes of barium. Given that autoionizing resonances exist in every trapped ion species, exploitation of this process is a promising pathway to increase the loading rates for trapped ion computers.

The SPES Laser Ion Source: Time Structure and Laser Enhancement Measurements with Sm+ beam

A two-step resonance photo-ionization scheme has been used to ionize samarium atoms in the SPES tantalum hot-cavity ion source. The effect of the ion load on the ion beam time structure and the laser enhancement of the ion yield has been studied at different ion source temperatures. Generally, the introduction of more positive ions (ion load) affects negatively the overall confinement of the laser ions inside the volume of the ion source. Possible enhancement of the laser ion confinement through the introduction of neutrals is observed as well. The ion load is also observed to affect the confinement in the transfer line much more than in the hot cavity. Measurement of the time structure with inverted polarity of the cavity DC heating supply confirmed the significance of the longitudinal potential for ion extraction. The laser enhancements of the ion yield are found to be sensitive to the ion load at low operating temperature of the ion source i.e. 1800°C, whereas at 2050°C and 2200°C, they are relatively stable till an ion load value of 1.2 µA.

RF acceleration of ultracold electron bunches.

The ultrafast and ultracold electron source, based on laser cooling and trapping of atomic gas and its subsequent near-threshold two-step photoionization, is capable of generating electron bunches with a high transverse brightness at energies of roughly 10 keV. This paper investigates the possibility of increasing the range of applications of this source by accelerating the bunch using radio frequency electromagnetic fields. Bunch energies up to 35 keV are measured by analyzing the diffraction patterns generated from a mono-crystalline gold sample. It is found that the normalized transverse emittance is largely preserved during acceleration.

Laser isotope separation of 192Ir

The following two-step isotope selective photoionization process has been studied for the separation of 192Ir isotope from natural Iridium irradiated in a medium flux reactor for 28 days.5d76s2F9/240.0cm−1→247.5871nm5d76s6p40389.83cm−1J=9/2→307.9nmIr+Density matrix formalism has been used for the investigation of laser isotope separation process. Optimum system parameters such as peak power densities of the excitation and ionization lasers, bandwidth of the excitation laser, angular divergence limit to the atomic ensemble have been derived. Effects of number density and ion travel distance prior to collection on charge exchange probability have also been studied. It has been shown that it is possible produce ∼98% enriched 192Ir at rate of 82 μg/h (27.9 GBq/h or 0.76 Ci/h) which can provide activity of 334 TBq/g or 9027 Ci/g. The enriched 192Ir can be used in both high-dose brachytherapy and high speed radiography. This is the first ever study on the laser based enrichment of Iridium isotopes.

Analysis and simulation of time-of-flight spectrum in Rb<sup>+</sup>-Rb hybrid trap

The time-of-flight mass spectrum of charged particles, which are created through two-step cw-laser photoionization of laser-cooled <sup>87</sup>Rb atoms in an ion-neutral hybrid trap, is quantitatively investigated to further facilitate the study of Rb<sup>+</sup>-Rb reactive collisions. A microchannel plate (MCP) is used to detect charged particles, and two spectral peaks corresponding to the <sup>87</sup>Rb<sup>+</sup> ions and the product <inline-formula><tex-math id="Z-20230423060254-1">\begin{document}$ \rm {}^{87}Rb_2^+ $\end{document}</tex-math><alternatives><graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="9-20222273_Z-20230423060254-1.jpg"/><graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="9-20222273_Z-20230423060254-1.png"/></alternatives></inline-formula> of the Rb<sup>+</sup>-Rb reaction were observed in the time-of-flight spectrum, respectively. The two peaks overlapped with each other and both showed an asymmetric profile. The information about the intensity, position, and half-width of the peak for a specific ion species was derived by fitting the time-of-flight spectrum with the probability density function of the Gumbel distribution. Then the relative ion intensity was converted into absolute ion number through the following steps. The rate equation of the total number of ions, which includes the number of atoms, the calibration factor of MCP, and the effective decay rate of ions in the ion trap, was established by modeling the photoionization of atoms. Combined with the absolute number of atoms measured by absorption imaging, the calibration factor in converting the ion intensity into the ion number was derived and the relative ion intensity was converted into the absolute number of ions. This provides a method of calibrating the MCP. The reliability of our calibration method was proved by the fact that the calibration factor in converting the intensity measured by MCP into particle number is independent of the duration of photoionization, the intensity and wavelength of the ionizing laser. Moreover, in order to explain the relationship between the peak width and temperature of the corresponding ion species, the time-of-flight spectra of the ions trapped in the ion trap were simulated by using COMSOL Multiphysics. The simulation results demonstrated that the large ion kinetic energy results in a narrow spectral peak. In sum, we quantitatively analyze and simulate the time-of-flight spectrum of the photoionization of cold atoms in the Rb<sup>+</sup>-Rb hybrid trap. The absolute number of ions is obtained by the intensity of the spectral peak, and the width of the spectral peak is related to the temperature of the ions. These results lay a foundation for the in-depth analysis of the ion-atom reaction collision and charged particle temperature relaxation in the photoionization of cold atoms, and thus further elucidating the subsequent collisional dynamics of ultracold plasmas.

Two-step photoionization of barium atoms through excited levels in optical dense approximation

The kinetics of two-step photoionization of barium atoms through excited levels was studied by numerical simulation method in the optically dense approximation. The first laser at wavelength nm ( nm) pumps transition (). The second laser with nm ( nm) ionizes atoms from the level (). The third probe laser with wavelength nm causes resonant fluorescence of barium ions. It is shown that the metastable from the triplet in barium is strongly populated through levels. Therefore, the applying of the ionizing laser tuned to a continuum from this metastable can yield a significant increase in the ionization efficiency. The laser-induced fluorescence method makes it possible to estimate the photoionization yield of barium ions with an error of up to 8%. The loading rate of the barium ion beam into the ion trap, obtained numerically, is consistent with the experimental data [Opt. Exp. 19(17), 16438 (2011)]. The deceleration of ultracold plasma recombination due to the heating of electrons in superelastic collisions for the characteristic times of a two-stage process is predicted.

Three-body recombination of ultracold barium plasma created by two-step photoionization of atoms through an excited 6s6p P11 level

The kinetics of ionization and recombination of an ultracold barium plasma created in a two-step process, taking into account the transfer of resonant radiation in 3D cylindrical geometry, is studied by numerical simulation. At the first step, a pump laser excites the upper level of the resonant transition 6s2 S10↔6s6p P11 (λ1=553.5 nm). At the second step, the laser with quantum energy exceeding the ionization potential from the level 6s6p P11 (λ2=417.79 nm) ionizes the atoms. A scheme is proposed for increasing the efficiency of electron yield: at the second ionization step, the laser radiation with frequency corresponding to the continuum from the metastable D32 is used. The electron temperature from the initial value 0.1 K during the action of the pump and ionizing lasers increases by more than 200 times due to superelastic processes. As a result, the time of three-body recombination of plasma increases significantly. The results of numerical simulation indirectly confirm the fact of Killian et al. [Phys. Rev. Lett. 83(23), 4776 (1999)] that the deceleration of recombination of ultracold xenon plasma can be explained by the heating of electrons in superelastic quenching collisions.

Isotope-selective laser ablation ion-trap loading of Ba+137 using a BaCl2 target

The $^{133}\mathrm{Ba}^+$ ion is a promising candidate as a high-fidelity qubit, and the $^{137}\mathrm{Ba}^+$ isotope is promising as a high-fidelity qudit ($d>2$). Barium metal is very reactive, and $^{133}\mathrm{Ba}^+$ is radioactive and can only be sourced in small quantities, so the most commonly used loading method, oven heating, is less suited for barium, and is currently not possible for $^{133}\mathrm{Ba}^+$.Pulsed laser ablation solves both of these problems by utilizing compound barium sources, while also giving some distinct advantages, such as fast loading, less displaced material, and lower heat load near the ion trap. Because of the relatively low abundances of the isotopes of interest, a two-step photoionization technique is used, which gives us the ability to selectively load isotopes. Characterization of the ablation process for our $\mathrm{BaCl}_2$ targets are presented, including observation of neutral and ion ablation-fluence regimes, preparation/conditioning and lifetimes of ablation spots, and plume velocity distributions.We show that using laser ablation on $\mathrm{BaCl}_2$ salt targets with a two-step photoionization method, we can produce and trap barium ions reliably. Further, we demonstrate that with our photoionization method, we can trap $^{137}\mathrm{Ba}^+$ with an enhanced selectivity compared to its natural abundance.

Odd-parity autoionizing levels of uranium observed by two-color two-step photoionization optogalvanic spectroscopy

Two-color two-step photoionization optogalvanic spectroscopy was performed using high-repetition-rate titanium sapphire lasers and a uranium hollow cathode lamp to find the two-step resonance ionization schemes of uranium. Many ionization transitions were observed by exciting uranium atoms in a ground state into five, even parity, excited levels with the first-step laser and by scanning the second-step laser wavelengths. By blocking the first-step laser, single-color, two-photon ionization transitions were also identified. From these results, we have found more than 50 odd-parity autoionizing levels of uranium in the energy, ranging from the ionization potential (49958.4 cm−1) to 51 150 cm−1. The determined energy levels are within ∼±1 cm−1 of previously reported values.

The longer timescale excited state dynamics of isolated benzene.

The excited state photodynamics of isolated benzene have been studied in the nanosecond range by two-step photoionization through various vibrations of the lowest singlet state, with imaging photoelectron spectroscopy detection. Photoelectron spectra are measured as a function of pump-probe delay time, and their time evolution is successfully compared to a biexponential decay function without regard to a particular kinetic model. The only reasonable kinetic model with only two exponentials is the one that involves an intersystem crossing from S1 to T1, although that model has previously been called into question by high-resolution studies that failed to find any singlet-triplet perturbations in Zeeman studies of the S1 spectrum. That contradiction remains unresolved.

Angular interferences of sequentially ionized double-continuum wave packets

Following the recent report of energy and angle interferences in below-threshold photoexcitation Auger processes due to postcollision interactions [Wang and Robicheaux, Phys. Rev. A 98, 013421 (2018)], similar interferences are also found in double-continuum wave packets from a two-step time-delayed photoionization of a two-electron atom. Properties of the interferences are studied in detail with respect to laser pulse time widths, laser frequency chirping, and ionization time delay. The effects of these physical quantities on the resulting interferences are discussed.

Laser assisted isotope separation of lithium by two-step photoionization using time of flight mass-spectrometer

Laser assisted isotope separation of lithium is carried out by isotope-selective two-step photoionization method using time of flight mass-spectrometer. The isotopes of lithium are important for nuclear industry. A narrowband tunable dye laser in combination with mass-spectrometer on tuning with 6Li (2S1/2 → 2P1/2) and 7Li (2S1/2 → 2P3/2) resonance levels confirms high degree of isotope selectivity (∼32). Both the dye laser (∼0.2 cm−1, 6 ns, 640–680 nm) and the mass-spectrometer are developed in-house and optimized. Measured relative isotopic abundance (6Li/7Li ≈ 0.080) is found in close agreement with literature. It is also found that concentration of naturally less abundant (6Li) isotope get enhanced remarkably from 7.5% up to over 72% upon precise tuning of the dye laser to 6Li (2S1/2 → 2P1/2) resonance level. Photoionization cross-sections of both the isotopes are measured as 6Li (15.53 ± 2.1 Mb) and 7Li (18.62 ± 2.4 Mb) for 2p excited state using more popular and accurate saturation technique, whereas number density are determined as N0 ≈ 5.9 × 109 and 5.62 × 1010 atoms/cm3 respectively. It is inferred that selected energy pathway [2S1/2 → ∼671 nm → 2P1/2, 3/2 → ∼337 nm → 1S0 (Li+)] gives high photoionization yield and the large (∼10 folds) isotope enrichment.

Laser ablation and two-step photo-ionization for the generation of 40Ca+

In this paper, we present a detailed method for rapidly and effectively loading a single 40Ca+ ion into a miniature linear Paul trap. Calcium atoms are generated by laser ablation, and the single ion is loaded and specific isotopes are selected by a two-step photo-ionization method. Compared to the traditional photo-ionization method in which atoms are typically emitted from a resistively heated oven, the advantages of laser ablation are that it can be precisely controlled, it can effectively avoid the problem of fluxed calcium deposition on the trap electrodes, and it restricts the generation of dark ions, which can influence atomic-precision spectroscopy measurements. With its short loading time, it is possible to load an ion in few seconds with the appropriate parameters. The technique of laser ablation has been applied to generate several species of atoms and ions at present, it will potentially benefit in the studies of optical frequency standards, quantum simulation and quantum information processing in an ultra-high vacuum condition and cryogenic system.

Measurements of the energy distribution of a high brightness rubidium ion beam

The energy distribution of a high brightness 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) eV, which is measured at a beam current of 9 pA. 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.

Efficient and robust photo-ionization loading of beryllium ions

We demonstrate the efficient generation of Be$^+$ ions with a 60 ns and 150 nJ laser pulse near 235 nm for two-step photo-ionization, proven by subsequent counting the number of ions loaded into a linear Paul trap. The bandwidth and power of the laser pulse are chosen in such a way that a first, resonant step fully saturates the entire velocity distribution of beryllium atoms effusing from a thermal oven. The second excitation step is driven by the same light field causing efficient non-resonant ionization. Our ion-loading scheme is more than 15 times more efficient as compared to former pathways using two-photon continuous wave laser excitation.

Cavity-enhanced photoionization of an ultracold rubidium beam for application in focused ion beams

A two-step photoionization strategy of an ultracold rubidium beam for application in a focused ion beam instrument is analyzed and implemented. In this strategy the atomic beam is partly selected with an aperture after which the transmitted atoms are ionized in the overlap of a tightly cylindrically focused excitation laser beam and an ionization laser beam whose power is enhanced in a build-up cavity. The advantage of this strategy, as compared to without the use of a build-up cavity, is that higher ionization degrees can be reached at higher currents. Optical Bloch equations including the photoionization process are used to calculate what ionization degree and ionization position distribution can be reached. Furthermore, the ionization strategy is tested on an ultracold beam of $^{85}$Rb atoms. The beam current is measured as a function of the excitation and ionization laser beam intensity and the selection aperture size. Although details are different, the global trends of the measurements agree well with the calculation. With a selection aperture diameter of 52 $\mu$m, a current of $\left(170\pm4\right)$ pA is measured, which according to calculations is 63% of the current equivalent of the transmitted atomic flux. Taking into account the ionization degree the ion beam peak reduced brightness is estimated at $1\times10^7$ A/(m$^2\,$sr$\,$eV).

The role of two-step excitation processes in laser cooling experiments: CaF2:Eu2+

The fluorescence of CaF2 single-crystals containing Eu2+ ions was studied under the excitation in the long-wavelength tail of the absorption spectrum which is due to electric dipole allowed transitions (“laser cooling regime”). Though no actual cooling was detected, spectra with a dominant anti-Stokes component were observed which demonstrate the possibility to employ electron-phonon bands of Eu2+ f-d transitions for optical refrigeration. The absence of observable optical refrigeration is ascribed to Eu2+ two-step photoionization processes that are responsible for the excited state absorption. The role of two-step excitation of impurity centers (excited state absorption) in laser cooling experiments is discussed.

Photosensitized Reactions of Psoralen and Herbicides Revealed by the Pump-Probe Method

Formation of triplet states in aqueous herbicide solutions excited by nanosecond radiation of 4th harmonic of Nd:YAG laser (wavelength 266 nm) is revealed by the pump-probe method. During photosensitized 8-MOP oxidation of herbicides, formation of triplet states of the photosensitizer and of the hydrated electron is observed in the process of two-step photoionization of 8-MOP.

Temperature of the Remaining Cold Atoms after Two-Step Photoionization in an 87Rb Vapor Cell Magneto-Optical Trap

The temperature of the remaining cold 87Rb atoms confined in a vapor cell magneto-optical trap after two-step photoionization has been measured. In the two-step photoionization process, the first excitation laser is served by the cooling laser and the second excitation laser is served by a continuous semiconductor laser with a wavelength of 450 nm. The results show that the temperature of the remaining cold atoms decreases as the intensity of the second excitation laser increases. Moreover, the relationship between the temperature T and number N of the remaining cold atoms generally follows a power law, while it deviates from the well-known T ∝ N1/3 and the power factor is smaller than 1/3. We propose that ion-atom collisions occurring during a photoionization process strongly influence the temperature scaling law in an optically dense magneto-optical trap in the presence of an ionization laser. In addition, the forced evaporative cooling due to the combined effect of the detuning of the first excitation laser and the two-step photoionization plays a role in cooling the remaining cold atoms and results in the dependence of the power factor on the detuning of the first excitation laser.

High Sensitive and Spatial-Resolution Atom Sensor Using Two-Step Photoionization with Two-Color Near-Field Lights Generated at a Nano-Slit

We develop a nanoslit to detect a small number of neutral atoms in the ground state. The detection scheme of using two-step photoionization is very sensitive and the use of nanometric near-field lights leads to an ultrahigh spatial resolution. An edge-sharpened nanoslit is fabricated with FIB milling. Considering the case of detecting Rb atoms, the polarization-dependent spatial distribution of near-field light generated at the nanoslit by total-internal reflection of a 476.5-nm Ar-ion laser beam is obtained with a scanning near-field optical microscope. Based on the experimental results, the ionization efficiency is estimated for both s-polarization and p-polarization. We also discuss the discrepancy between the experimental value and the numerical one obtained from the finite difference time domain simulations in the p-polarization case.