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Physical Review A

Generation of metastable krypton using a 124-nm laser

Xi‐Ze Dong, Florian Ritterbusch, Dao-Fu Yuan, Jing-Wen Yan, W.-T. Chen, Wei Jiang, Zheng‐Tian Lu, Jie S. Wang, Xingan Wang, Guo‐Min Yang

Published Mar 9, 2022• 7 citations
Publisher

Abstract

We have realized the optical excitation of krypton to a metastable level with an efficiency as high as $23\phantom{\rule{0.16em}{0ex}}%$ using near-resonant 124-nm light produced by four-wave mixing in mercury vapor. Self-absorption in mercury is circumvented by adjusting the detuning and phase matching according to experimental and theoretical characterizations. Density-matrix calculations of the metastable krypton generation agree with the measured dependencies of the excitation efficiency, indicating pathways towards a further improvement. The obtained excitation efficiency, being one order of magnitude higher than that of previously demonstrated techniques, enables an extension of the metastable density regime for atomic physics applications, including magnetometry, atom lithography, and radioisotope dating.

DOI
10.1103/physreva.105.l031101

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We have realized the optical excitation of krypton to a metastable level with an efficiency as high as 2323\phantom{\rule{0.16em}{0ex}}%23 using near-resonant 124-nm light produced by four-wave mixing in mercury vapor. Self-absorption in mercury is circumvented by adjusting the detuning and phase matching according to experimental and theoretical characterizations. Density-matrix calculations of the metastable krypton generation agree with the measured dependencies of the excitation efficiency, indicating pathways towards a further improvement. The obtained excitation efficiency, being one order of magnitude higher than that of previously demonstrated techniques, enables an extension of the metastable density regime for atomic physics applications, including magnetometry, atom lithography, and radioisotope dating.
We demonstrate the generation of metastable krypton in the long-lived 1s^{5} state using laser excitation. The atoms are excited through a two-photon absorption process into the 2p^{6} state using a pulsed optical parametric oscillator laser operating near 215 nm, after which the atoms decay quickly into the metastable state with a branching ratio of 75%. The interaction dynamics are modeled using density matrix formalism and, by combining this with experimental observations, we are able to calculate photoionization and two-photon absorption cross sections. When compared to traditional approaches to metastable production, this approach shows great potential for high-density metastable krypton production with minimal heating of the sample. Here, we show metastable production efficiencies of up to 2% per pulse. The new experimental results gained here, when combined with the density matrix model we have developed, suggest that fractional efficiencies up to 30% are possible under optimal conditions.
Radioisotopes that break down at a constant rate over time through radioactive decay allow scientists to understand the development of geological and anthropological history by dating samples that contain such isotopes. While many techniques exist to measure the age of a sample, in this thesis we explore the possibility of enhancing the atom trap trace analysis (ATTA) method, which has made significant strides in the area of ultra-sensitive radioisotope detection, especially with the use of metastable noble gas radionuclides. A metastable atom is an atom in a stable, long-lived (>1 ms) excited state. Noble gases have the longest metastable lifetimes, which combined with their geochemical inertness, make them ideal candidates for geological and environmental radiometric techniques. The production of metastable noble gases for this purpose has traditionally relied on discharge sources, but this method suffers from important drawbacks such as high levels of crosscontamination and poor excitation efficiencies. In an effort to overcome these drawbacks, the method described in this work presents a new platform for implementing, characterising and comparing purely laser-based production of metastable noble gases. In the first part of this thesis, we present both state-of-the-art experimental results in the purely laser-based generation of metastable krypton atoms, and a physically realistic simulation with good agreement with our experimental results. Our calculation of the twophoton absorption cross section for krypton (to a metastable-generating excited state) using 215nm deep ultraviolet (DUV) laser radiation, obtained by fitting with theory, confirms that high metastable production efficiencies are possible with laser-based techniques. In addition to this parameter, the branching ratio and photoionisation rate from the excited state are calculated and agree with the literature. In the second part, we present the experimental progress to date for a brand new method of manipulating metastable noble gas atoms using a two-stage approach of metastable production then trapping via a magneto-optical trap (MOT). While the results are limited due to experimental difficulties, they are complemented by a physically realistic 3D simulation based on the Monte Carlo method. This simulation suggests that the production and trapping of metastable noble gases is feasible without the use of a discharge source, a Zeeman slower, and even a secondary excitation chamber. However, the loading rate for such a MOT is not sufficient for ATTA measurements without drastic changes in the experimental configuration. In the final part, we propose a next-generation ATTA system based on stimulated rapid adiabatic passage (STIRAP) to transfer noble gas atoms to their metastable state with near 100% efficiency. This technique for the generation of metastable noble gases would be purely laser-based and would compete with the loading rates of conventional production techniques, while avoiding their deleterious effects. We conclude by identifying limits of laser-based techniques and explore approaches to overcome them.
High-power tunable VUV light pulses with energies up to 0.7 μJ were generated in the 115.7–116.9-nm region by use of a two-photon resonant four-wave mixing scheme in a Xe–Ar gas mixture. This is the highest reported pulse energy that has been produced in this wavelength region using a four-wave mixing process. Efficient detection of krypton isotopes at densities as low as 10 atoms/cm3 was demonstrated by resonantly ionizing the atom through its one-photon allowed state at the vacuum wavelength of 116.49 nm.
A room-temperature beam of krypton atoms in the metastable 5s[3/2]2 level is demonstrated via an optical excitation method. A Kr-discharge lamp is used to produce vacuum ultraviolet photons at 124 nm for the first-step excitation from the ground level 4p6 1S0 to the 5s[3/2]1 level. An 819 nm Ti:sapphire laser is used for the second-step excitation from 5s[3/2]1 to 5s[3/2]2 followed by a spontaneous decay to the 5s[3/2]2 metastable level. A metastable atomic beam with an angular flux density of 3 x 10(14) s(-1) sr(-1) is achieved at the total gas flow rate of 0.01 cm3/s at STP (or 3 x 10(17) at./s). The dependences of the flux on the gas flow rate, laser power, and lamp parameters are investigated.
We report measurements of the absolute yield of 123.6-nm vacuum ultraviolet (VUV) radiation produced in a resonant four-wave-mixing scheme in krypton enhanced by electromagnetically induced transparency. One of the mixing fields, in the ultraviolet (UV) at 212.55 nm, was in two-photon resonance with the 4p61S0−−4p55p[0,12]{4p}^{6}{}^{1}{S}_{0}--{4p}^{5}5p[0,\frac{1}{2}]4p61S0​−−4p55p[0,21​] transition of krypton, while a second field (the coupling field) at 759 nm was resonant with the ${4p}^{5}5p[0,\frac{1}{2}]{\ensuremath{-}4p}^{5}5s[1,\frac{1}{2}]$ transition. Electromagnetically induced transparency has been predicted to be induced by this coupling field and to enhance the efficiency of the generation of the field at 123.6 nm, on the 4p55s[1,12]{4p}^{5}5s[1,\frac{1}{2}]4p55s[1,21​] to 4p61S0{4p}^{6}{}^{1}{S}_{0}4p61S0​ transition. This was confirmed by measurements of the absolute VUV radiation yield using a calibrated photodiode in the limit of a large density-length product. Energies of \ensuremath{\sim}30 nJ were produced, which gave a conversion efficiency, from the coupling field energy of \ensuremath{\sim}1%. Higher yields are thought to be achievable by increasing the coupling laser intensity, the path length of the medium, and by the use of a transform-limited UV pulse of the same duration as the coupling field.
Coherent radiation at several wavelengths in the vacuum ultraviolet (VUV) has been generated by four-wave parametric oscillation in mercury vapor. When a powerful ultraviolet pump laser of frequency omega(p) is tuned to a two-photon resonance, VUV signal photons at frequency omega(s), as well as idler photons at frequency omega(i), are generated such that omega(s) + omega(i) = 2omega(p). A frequency-doubled dye laser tuned to two-photon resonance with the 6s6d(1)D(2) level near 280.3 nm produced output at 184.9 and 143.5 nm. A tunable krypton fluoride excimer laser tuned to two-photon resonance with the 6s10s (1)S(0) level near 248.7 nm produced output at 140.1, 130.7, 130.1, 125.9, and 125.0 nm. Approximately 1-microJ, 200-W pulses were observed at 143.5 and 125.9 nm.