We present a combined experimental and theoretical study on the radiative lifetime of CO in the $a^3Π_{1,2}, v=0$ state. CO molecules in a beam are prepared in selected rotational levels of this metastable state, Stark-decelerated and electrostatically trapped. From the phosphorescence decay in the trap, the radiative lifetime is measured to be $2.63\pm0.03$ ms for the $a^3Π_1, v=0, J=1$ level. From spin-orbit coupling between the $a^3Π$ and the $A^1Π$ state a 20% longer radiative lifetime of 3.16 ms is calculated for this level. It is concluded that coupling to other $^1Π$ states contributes to the observed phosphorescence rate of metastable CO.
We have measured the lifetime of the 5s5p ^3P_2 metastable state of strontium atoms by magneto-optically trapping the decayed atoms to the ground state, which allowed sensitive detection of the rare decay events. We found that the blackbody radiation-induced decay was the dominant decay channel for the state at T = 300 K. The lifetime was determined to be 500^{+280}_{-130} s in the limit of zero temperature.
Laser-induced fluorescence (LIF) performed on metastable ions is frequently used to probe the dynamics of ground-state ion motions in many laboratory plasmas. However, these measurements place restrictions on the metastable ion lifetime. Metastable states are produced from direct ionization of neutral atoms as well as ions in other electronic states, of which the former will only faithfully represent processes that act on the ion dynamics in a time shorter than the metastable lifetime. We present here the first experimental study of this type of systematic effect using wave-particle interactio…
The lifetime of the metastable 3P2 state of neon has been determined to 14.70(13) s (decay rate 0.06801(62) 1/s) by measuring the decay in fluorescence of an ensemble of Ne-20 atoms trapped in a magneto-optical trap (MOT). Due to low background gas pressure p < 5 10^-11 mbar and low relative excitation to the 3D3 state (0.5% excitation probability) operation only small corrections have to be included in the lifetime extrapolation. Together with a careful analysis of residual loss mechanisms in the MOT a lifetime determination to high precision is achieved.
The lifetime of the 3d^2D_5/2-level in singly-ionized calcium has been measured by the electron-shelving technique on different samples of rf trapped ions. The metastable state has been directly populated by exciting the dipole-forbidden 4S_1/2 - 3D_5/2 transition. In ion clouds, the natural lifetime of this metastable level has been measured to be (1095+-27) ms. For the single-ion case, we determined a lifetime of (1152+-20) ms. The 1sigma-error bars at the 2%-level have different origins for the two kinds of experiments: data fitting methods for lifetime measurements in an ion cloud and cont…
Externally applied electromagnetic fields in general have an influence on the width of atomic spectral lines. The decay rates of atomic states can also be affected by the geometry of an applied field configuration giving rise to an imaginary geometric phase. A specific chiral electromagnetic field configuration is presented which geometrically modifies the lifetimes of metastable states of hydrogen. We propose to extract the relevant observables in a realistic longitudinal atomic beam spin-echo apparatus which allows the initial and final fluxes of the metastable atoms to be compared with each…
We present a measurement of the lifetime of the metastable 3d 2D5/2 state in the 40Ca+ ion, using the so-called shelving technique on a string of five Doppler laser-cooled ions in a linear Paul trap. A detailed account of the data analysis is given, and systematic effects due to unwanted excitation processes and collisions with background gas atoms are discussed and estimated. From a total of 6805 shelving events, we obtain a lifetime tau=1149+/-14(stat.)+/-4(sys.)ms, a result which is in agreement with the most recent measurements.
Extensive information, such as ion temperature and wave-particle interactions, can be obtained by direct measurement of ion distribution functions using laser-induced fluorescence (LIF). This nonintrusive plasma diagnostic provides an important window into the ion motions in phase-space. Previous simulation results suggest that LIF measurements, which are performed on metastable ions produced directly from neutral gas particles and also from ions in other electronic states, place restrictions on the metastable lifetime. In the case where metastable population is produced from direct ionization…
Magnetic quadrupole and electric octupole transitions from the configurations $4p^54d^{N+1}$ and $4p^64d^{N-1}4f$ were calculated along with magnetic dipole, electric dipole and electric quadrupole radiative transitions in quasirelativistic Hartree-Fock approximation. Their significance in determining the metastable level radiative lifetimes was investigated along several isoelectronic sequences for the ions from $Z=50$ to $Z=92$. Strontium-like ions, zirconium-like ions, molybdenum-like ions and rhodium-like ions were studied comprehensively. Remaining isoelectronic sequences with the ground …
Lifetimes of the first two metastable states in Sc^{2+} and Y^{2+} are determined using the relativistic coupled-cluster theory. There is a considerable interest in studying the electron correlation effects in these ions as though their electronic configurations are similar to the neutral alkali atoms, their structures are very different from the latter. We have made a comparative study of the correlation trends between the above doubly ionized systems with their corresponding neutral and singly ionized iso-electronic systems. The lifetimes of the excited states of these ions are very importan…
Metastable levels in rhodium-like ions with the ground configuration $4p^{6}4d^{9}$ and the excited configurations $4p^{6}4d^{8}4f$ and $4p^{5}4d^{10}$ are investigated. The {\sl ab initio} calculations of the level energies, radiative multipole transition probabilities are performed in a quasirelativistic Hartree-Fock approximation employing an extensive configuration interaction based on quasirelativistic transformed radial orbitals. A systematic trends in behavior of calculated radiative lifetimes of the metastable levels are studied for the ions from $Z=60$ to $Z=92$. The significance of t…
Medium resolution ($Δν$ ~ 3 GHz) laser-induced fluorescence (LIF) excitation spectra of a rotationally cold sample of YbOH in the 17300-17950 cm$^{-1}$ range have been recorded using two-dimensional (excitation and dispersed fluorescence) spectroscopy. High resolution ($Δλ$ ~ 0.65 nm) dispersed laser induced fluorescence (DLIF) spectra and radiative decay curves of numerous bands detected in the medium resolution LIF excitation spectra were recorded. The vibronic energy levels of the $\tilde{X} \, ^2Σ^+$ state were predicted using a discrete variable representation approach and compared with o…
The properties of the least-bound vibrational level (v=14) of the quintet sigma state formed during the ultracold collision of two spin-polarized metastable helium atoms are crucial to studies of photoassociation spectroscopy of metastable helium. We report a calculation of the autoionization lifetime of this state induced by spin-dipole coupling of the quintet sigma state to the singlet sigma state from which Penning and associative ionization processes are highly probable. We find a lifetime of about 150 microseconds, significantly larger than the recent experimental estimates of (4-5) micro…
Avoided crossings of level pairs with opposite slopes can form potential energy curves for the external degree of freedom of quantum particles. We investigate nonadiabatic decay of metastable states on such avoided crossings (MSACs) using diabatic and adiabatic representations. The system is described by a single scaled adiabaticity parameter, $V$. The time-independent two-component Schrödinger equation is solved in both representations, and the nonadiabatic lifetimes of MSACs are determined from a wave-function flux calculation and from the Breit-Wigner formula, leading to four lifetime value…
Spin-dipole mediated interactions between tightly confined metastable helium atoms couple the spin-polarized quintet ${}^{5}Σ^{+}_{g}$ state to the singlet ${}^{1}Σ^{+}_{g}$ state from which autoionization is highly probable, resulting in finite lifetimes for the trap eigenstates. We extend our earlier study on spherically symmetric harmonic traps to the interesting cases of axially symmetric anisotropic harmonic traps and report results for the lowest 10 states in "cigar-like" and "pancake-like" traps with average frequencies of 100 kHz and 1 MHz. We find that there is a significant suppressi…
Hyperfine quenching rates of the lowest-energy metastable $^3P_0$ and $^3P_2$ states of Mg, Ca, Sr, and Yb atoms are computed. The calculations are carried out using ab initio relativistic many-body methods. The computed lifetimes may be useful for designing novel ultra-precise optical clocks and trapping experiments with the $3P_2$ fermionic isotopes. The resulting natural widths of the $^3P_0 -> ^1S_0$ clock transition are 0.44 mHz for $^{25}$Mg, 2.2 mHz for $^{43}$Ca, 7.6 mHz for $^{87}$Sr, 43.5 mHz for $^{171}$Yb, and 38.5 mHz for $^{173}$Yb. Compared to the bosonic isotopes, the lifetime …
The atomic states of the W IX (W8+) tungsten ion lying below the W9+ ionisation threshold have been studied theoretically, employing the multiconfiguration Dirac-Hartree-Fock method with configuration interaction. The level electronic structures and their energies are presented. The electric dipole (E1), magnetic dipole (M1), electric quadrupole (E2), and magnetic quadrupole (M2) radiative transitions have been computed in order to calculate the radiative lifetimes of given states. Transition wavelengths, energies, and decay rates are also presented for selected high-intensity E1 transitions. …
The photoionization cross-sections of two even-parity excited states, $5d6d ^3D_1$ and $6s7d ^3D_{2}$, of atomic Ba at the ionization-laser wavelength of 556.6 nm were measured. We found that the total cross-section depends on the relative polarization of the atoms and the ionization-laser light. With density-matrix algebra, we show that, in general, there are at most three parameters in the photoionization cross-section. Some of these parameters are determined in this work. We also present the measurement of the radiative lifetime of five even-parity excited states of barium.
When the atoms of a dimer remain most of the time very far apart, in so-called long-range molecular states, their mutual interaction is ruled by plain atomic properties. The high-resolution spectroscopic study of some molecular excited states populated by photoassociation of cold atoms (photoassociative spectroscopy) gives a good illustration of this property. It provides accurate determinations of atomic radiative lifetimes, which are known to be sensitive tests for atomic calculations. A number of such analyses has been performed up to now, for all stable alkali atoms and for some other atom…
Energy levels and radiative rates for transitions in five Br-like ions (Sr IV, Y V, Zr VI, Nb VII and Mo VIII) are calculated with the general-purpose relativistic atomic structure package ({\sc grasp}). Extensive configuration interaction has been included and results are presented among the lowest 31 levels of the 4s$^2$4p$^5$, 4s$^2$4p$^4$4d and 4s4p$^6$ configurations. Lifetimes for these levels have also been determined, although unfortunately no measurements are available with which to compare. However, recently theoretical results have been reported by Singh {\em et al} [Phys. Scr. {\bf…
The first metastable triplet state of HeH$^+$ was found to be present in ion beam experiments, with its lifetime estimated to be between hundreds of milliseconds and thousand of seconds. In this work, we use {\it ab initio} methods to evaluate the radiative lifetimes of the six vibrational levels of the $a\ ^3Σ^+$ of HeH$^+$. The transition $a\ ^3Σ^+ \rightarrow X \ ^1Σ^+$ is spin-forbidden, but acquires intensity through spin-orbit interaction with the singlet and triplet $Π$ states. Large scale CASSCF/MRCI calculations using an adapted basis set were performed to determine the potential ener…
The multiconfiguration Dirac-Hartree-Fock (MCDHF) model has been employed to calculate the transition rates between the nine lowest levels of radium. The dominant rates were then used to evaluate the radiative lifetimes. The decay of the metastable $ 7s7p ^3 P_0 $ state through 2-photon E1M1 and hyperfine induced channels is also studied.
A method is proposed to manipulate the annihilation dynamics of a dense gas of positronium atoms employing superradiance and subradiance regimes of the cooperative spontaneous emission of the system. The annihilation dynamics is controlled by the gas density and by the intensity of the driving strong resonant laser field. In particular, the method allows to increase the annihilation lifetime of an ensemble of positronium atoms more than hundred times by trapping the atoms in the excited state via collective radiative effects in the resonant laser and cavity fields.
Magneto-optically trapped atoms enable the determination of lifetimes of metastable states and higher lying excited states like the $\rm{5d^{2}~^{3}F_{2}}$ state in barium. The state is efficiently populated by driving strong transitions from metastable states within the cooling cycle of the barium MOT. The lifetime is inferred from the increase of MOT fluorescence after the transfer of up to $30\,\%$ of the trapped atoms to this state. The radiative decay of the $\rm{5d^{2}~^{3}F_{2}}$ state cascades to the cooling cycle of the MOT with a probability of $96.0(7)\,\%$ corresponding to a trap l…
The fluorescence spectrum resulting from laser excitation of the A^{2}Π_{1/2} - X^{2}Σ^{+} (0,0) band of ytterbium monofluoride, YbF, has been recorded and analyzed to determine the Franck-Condon factors. The measured values are compared with those predicted from Rydberg-Klein-Rees (RKR) potential energy curves. From the fluorescence decay curve the radiative lifetime of the A^{2}Π_{1/2} state is measured to be 28\pm2 ns, and the corresponding transition dipole moment is 4.39\pm0.16 D. The implications for laser cooling YbF are discussed.
The intrinsic radiative lifetimes of the $5d^{10}6s$ $^{2}\text{S}_{1/2}$ and $5d^{9}6s^{2}$ $^{2}\text{D}_{3/2}$ bound excited states in the platinum anion $\text{Pt}^{-}$ have been studied at cryogenic temperatures at the Double ElectroStatic Ion Ring Experiment (DESIREE) facility at Stockholm University. The intrinsic lifetime of the higher-lying $5d^{10}6s$ $^{2}\text{S}_{1/2}$ state was measurement to be 2.54$\pm$0.10 s, while only a lifetime in the range of 50 - 200 ms could be estimated for the $5d^{9}6s^{2}$ $^{2}\text{D}_{3/2}$ fine-structure level. The storage lifetime of the $\text{…
This work reports new experimental radiative lifetimes and calculated oscillator strengths for transitions of astrophysical interest in singly ionized cobalt. More precisely, nineteen radiative lifetimes in Co+ have been measured with the time-resolved laser-induced fluorescence technique using one- and two-step excitations. Out of these, seven belonging to the high lying 3d$^7$($^4$F)4d configuration in the energy range 90697 - 93738 cm$^{-1}$ are new, and the other twelve from th3d$^7$($^4$F)F)4p configuration with energies between 45972 and 49328 cm$^{-1}$1 are compared with previous measur…
Photodetachment thermometry on a beam of OH$^-$ in a cryogenic storage ring cooled to below 10 K is carried out using two-dimensional, frequency and time dependent photodetachment spectroscopy over 20 minutes of ion storage. In equilibrium with the low-level blackbody field, we find an effective radiative temperature near 15 K with about 90% of all ions in the rotational ground state. We measure the J = 1 natural lifetime (about 193 s) and determine the OH$^-$ rotational transition dipole moment with 1.5% uncertainty. We also measure rotationally dependent relative near-threshold photodetachme…
The best limit on the electron electric dipole moment (eEDM) comes from the ACME II experiment [Nature \textbf{562} (2018), 355-360] which probes physics beyond the Standard Model at energy scales well above 1 TeV. ACME II measured the eEDM by monitoring electron spin precession in a cold beam of the metastable H$^3Δ_1$ state of thorium monoxide (ThO) molecules, with an observation time $τ\approx 1$ ms for each molecule. We report here a new measurement of the lifetime of the ThO (H$^3Δ_1$) state, $τ_H = 4.2\pm 0.5$ ms. Using an apparatus within which $τ\approx τ_H$ will enable a substantial r…
We estimate the range of the radiative lifetime and energy of the anomalous, low-energy $3/2^+(7.8 \pm 0.5$ eV) state in the $^{229}$Th nucleus. Our phenomenological calculations are based on the available experimental data for the intensities of $M1$ and $E2$ transitions between excited levels of the $^{229}$Th nucleus in the $K^π[Nn_ZΛ]=5/2^+[633]$ and $3/2^+[631]$ rotational bands. We also discuss the influence of certain branching coefficients, which affect the currently accepted measured energy of the isomeric state. From this work, we establish a favored region where the transition lifet…
We tabulate spontaneous emission rates for all possible 811 electric-dipole-allowed transitions between the 75 lowest-energy states of Ca I. These involve the $4sns$ ($n=4-8$), $4snp$ ($n=4-7$), $4snd$ ($n=3-6$), $4snf$ ($n=4-6$), $4p^2$, and $3d4p$ electronic configurations. We compile the transition rates by carrying out ab initio relativistic calculations using the combined method of configuration interaction and many-body perturbation theory. The results are compared to the available literature values. The tabulated rates can be useful in various applications, such as optimizing laser cool…
A different technique is used to study the radiative decay of a metastable state in multiply ionized atoms. With use of a unitary Penning trap to selectively capture Kr$^{17+}$ ions from an ion source at NIST, the decay of the 3d $^2D_{5/2}$ metastable state is measured in isolation at low energy, without any active cooling. The highly ionized atoms are trapped in the fine structure of the electronic ground configuration with an energy spread of 4(1) eV, which is narrower than within the ion source by a factor of about 100. By observing the visible 637 nm photon emission of the forbidden trans…
Energy levels and radiative rates are reported for transitions in Br-like W XL, calculated with the general-purpose relativistic atomic structure package ({\sc grasp}). Configuration interaction (CI) has been included among 46 configurations (generating 4215 levels) over a wide energy range up to 213 Ryd. However, for conciseness results are only listed for the lowest 360 levels (with energies up to $\sim$ 43 Ryd), which mainly belong to the 4s$^2$4p$^5$, 4s$^2$4p$^4$4d, 4s$^2$4p$^4$4f, 4s4p$^6$, 4p$^6$4d, 4s4p$^5$4d, 4s$^2$4p$^3$4d$^2$, and 4s$^2$4p$^3$4d4f configurations, and provided for fo…
Using the multiconfiguration Dirac-Hartree-Fock (MCDHF) and the relativistic configuration interaction (RCI) methods, a consistent set of transition energies and radiative transition data for the lowest 150 states of the $3s^2 3p^3$, $3s 3p^4$, $3s^2 3p^2 3d$, $3s 3p^3 3d$, $3p^5$, and $3s^2 3p 3d^2$ configurations in P-like Ge XVIII is provided. To assess the accuracy of the MCDHF transition energies, we have also performed calculations using the many-body perturbation theory (MBPT). Comparisons are made between the present MCDHF and MBPT data sets, as well as with other available experimenta…
We report calculations of energy levels, radiative decay rates, and lifetimes for transitions among the 3s$^2$3p$^5$, 3s3p$^6$, and 3s$^2$3p$^4$3d configurations of Cl-like W LVIII. The general-purpose relativistic atomic structure package (GRASP) has been adopted for our calculations. Comparisons are made with the most recent results of Mohan et al. [Can. J. Phys. {\bf 92} (2014) xxx] and discrepancies in lifetimes are noted, up to four orders of magnitude in some instances. Our energy levels are estimated to be accurate to better than 0.5\%, whereas results for radiative rates and lifetimes …
Energy levels and radiative rates are reported for transitions in Cl-like W LVIII. Configuration interaction (CI) has been included among 44 configurations (generating 4978 levels) over a wide energy range up to 363 Ryd, and the general-purpose relativistic atomic structure package ({\sc grasp}) adopted for the calculations. Since no other results of comparable complexity are available, calculations have also been performed with the flexible atomic code ({\sc fac}), which help in assessing the accuracy of our results. Energies are listed for the lowest 400 levels (with energies up to $\sim$ 98…
We have measured the radiative lifetimes of ns, np and nd Rydberg states of rubidium in the range 28 < n < 45. To enable long-lived states to be measured, our experiment uses slow-moving Rb atoms in a magneto-optical trap (MOT). Two experimental techniques have been adopted to reduce random and systematic errors. First, a narrow-bandwidth pulsed laser is used to excite the target Rydberg state, resulting in minimal shot-to-shot variation in the initial state population. Second, we monitor the target state population as a function of time delay from the laser pulse using a short-duration, milli…
Employing two state-of-the-art methods, second-order many-body perturbation theory and multiconfiguration Dirac-Fock, highly accurate calculations are performed for the lowest 318 fine-structure levels arising from the $2s^{2} 2p^{4}$, $2s 2p^{5}$, $2p^{6}$, $2s^{2} 2p^{3} 3l$, $2s 2p^{4} 3l$, $2p^{5} 3l$, and $2s^{2} 2p^{3} 4l$ configurations in O-like \mbox{Mo XXXV}. Complete and consistent atomic data, including excitation energies, lifetimes, wavelengths, and E1, E2, M1 line strengths, oscillator strengths, and transition rates among these 318 levels are provided. Comparisons are made betw…
The lifetime of the metastable 5d$^2$D$_{5/2}$ state has been measured for a single trapped Ba$^+$ ion in a Paul trap in Ultra High Vacuum (UHV) in the 10$^{-10}$ mbar pressure range. A total of 5046 individual periods when the ion was shelved in this state have been recorded. A preliminary value $τ_{D_{5/2}} = 26.4(1.7)$~s is obtained through extrapolation to zero residual gas pressure.
We report a precise determination of the lifetime of the (4p)$^2$P$_{3/2}$ state of $^{40}$Ca$^+$, $τ_{\textrm{P}_{3/2}}=6.639(42)$ ns, using a combination of measurements of the induced light shift and scattering rate on a single trapped ion. Good agreement with the result of a recent high-level theoretical calculation, $6.69(6)$ ns [Safronova et al., PRA 83, 012503 (2011)], but a 6-$σ$ discrepancy with the most precise previous experimental value, $6.924(19)$ ns [Jin et al., PRL 70, 3213 (1993)] is found. To corroborate the consistency and accuracy of the new measurements, relativistically c…
New experiments were proposed recently to investigate the regime of cold atomic and molecular ion-atom collision processes in a special hybrid neutral-atom--ion trap under high vacuum conditions. The collisional cooling of laser pre-cooled Ca$^+$ ions by ultracold Na atoms is being studied. Modeling this process requires knowledge of the radiative lifetime of the excited singlet A$^1Σ^+$ state of the (NaCa)$^+$ molecular system. We calculate the rate coefficient for radiative charge transfer using a semiclassical approach. The dipole radial matrix elements between the ground and the excited st…
This work reports new experimental radiative lifetimes and calculated oscillator strengths for transitions from 3d8 4d levels of astrophysical interest in singly ionized nickel. Radiative lifetimes of seven high-lying levels of even parity in Ni II (98400 -100600 cm-1) have been measured using the time-resolved laser-induced fluorescence method. Two-step photon excitation of ions produced by laser ablation has been utilized to populate the levels. Theoretical calculations of the radiative lifetimes of the measured levels and transition probabilities from these levels are reported. The calculat…
Lifetime of the $^2F_{7/2}$ level in Yb$^+$ for spontaneous emission of electric octupole radiation
Physikalisch-Technische Bundesanstalt（德国联邦物理技术研究院）；Institut für Mathematische Physik, Technische Universität Braunschweig（布伦瑞克工业大学数学物理研究所）；Laboratory for Emerging Nanometrology（新兴纳米计量学实验室）
