A simple analytical solution for the problem of multiphoton detachment from negative ions by a linearly polarized laser field is found. It is valid in the wide range of intensities and frequencies of the field, from the perturbation theory to the tunneling regime, and is applicable to the excess-photon as well as near-threshold detachment. Practically, the formulae are valid when the number of photons is greater than two. They produce the total detachment rates, relative intensities of the excess-photon peaks, and photoelectron angular distributions for the hydrogen and halogen negative ions, in agreement with those obtained in other, more numerically involved calculations in both perturbative and non-perturbative regimes. Our approach explains the extreme sensitivity of the multiphoton detachment probability to the asymptotic behaviour of the bound-state wave function. Rapid oscillations in the angular dependence of the $n$-photon detachment probability are shown to arise due to interference of the two classical trajectories which lead to the same final state after the electron emerges at the opposite sides of the atom when the field is close to maximal.
Two-photon detachment from the F-minus negative ion is investigated within the lowest order of perturbation theory. We show that in accordance with the adiabatic theory a proper asymptotic behaviour of the 2p bound state wave function is crucial for obtaining correct absolute values of the multiphoton detachment cross sections. We find that the latter are substantially higher than it was previously believed.
In this paper we compare the results of our adiabatic theory (Gribakin and Kuchiev, Phys. Rev. A, accepted for publication) with other theoretical and experimental results, mostly for halogen negative ions. The theory is based on the Keldysh approach. It shows that the multiphoton detachment rates and the corresponding n-photon detachment cross sections depend only on the asymptotic behaviour of the bound state radial wave function. The dependence on the exponent is very strong. This is the main reason for the disagreement with some previous calculations, which employed bound state wave functi…
A theory of electron detachment from atoms or negative ions by a superposition of a static and a laser (or, more generally, ac) fields, parallel to each other, is developed in the case when the photon energy and the field amplitude are much less than the detachment energy and intra-ion field, respectively. Simple analytical results together with their validity conditions are obtained. Several qualitatively different regimes of detachment have been identified. Applications of the present theory to electron emission from metal and semiconductor surfaces and from photosynthetic bio-complexes are …
Negative ion detachment in bichromatic laser field is considered within the adiabatic theory. The latter represents a recent modification of the famous Keldysh model for multiphoton ionization which makes it quantitatively reliable. We calculate angular differential detachment rates, partial rates for particular ATD (Above Threshold Detachment) channels and total detachment rates for the Hydrogen ion in a bichromatic field with 1:3 frequency ratio and various phase differences. Reliability of the present, extremely simple approach is testified by comparison with much more elaborate earlier cal…
Negative ion detachment in two-colour laser field is considered within the recent modification of Keldysh model which makes it quantitatively reliable. The general approach is illustrated by calculation of angular differential detachment rates, partial rates for particular ATD (Above Threshold Detachment) channels and total detachment rates for H$^-$ ion in bichromatic field with 1:2 frequency ratio. Both perturbative and strong field regimes are examined. Polar asymmetry and phase effects are quantitatively characterized with some new features revealed. Phase effects are found to result in a …
Absolute two-photon detachment cross sections and photoelectron angular distribution are calculated for halogen negative ions within lowest-order perturbation theory. The Dyson equation method is used to obtain the outer np ground-state wave functions with proper asymptotic behavior exp (-k r), corresponding to correct (experimental) binding energies E=k^2/2. The latter is crucial for obtaining correct absolute values of the multiphoton cross sections (Gribakin and Kuchiev 1997 Phys. Rev.A55 3760). Comparisons with previous calculations and experimental data are performed.
We have developed one electron detachment theory from a closed-shell atomic configuration in the relativistic Fock-space coupled-cluster ansatz. Using this method, we determine sensitivity coefficients to the variation of the fine structure constant in the first three important low-lying transitions of the astrophysically interesting highly charged Mn IX, Fe X, Co XI and Ni XII ions. The potential of this method has been assessed by evaluating the detachment energies of the removed electrons and determining lifetimes of the atomic states in the above ions. To account the sensitivity of the hig…
The description of threshold fragmentation under long range repulsive forces is presented. The dominant energy dependence near threshold is isolated by decomposing the cross section into a product of a back ground part and a barrier penetration probability resulting from the repulsive Coulomb interaction. This tunneling probability contains the dominant energy variation and it can be calculated analytically based on the same principles as Wannier's description for threshold ionization under attractive forces. Good agreement is found with the available experimental cross sections on detachment …
Absolute three-photon detachment cross sections are calculated for the fluorine negative ion within the lowest-order perturbation theory. The Dyson equation of the atomic many-body theory is used to obtain the ground-state 2p wavefunction with correct asymptotic behaviour, corresponding to the true (experimental) binding energy. We show that in accordance with the adiabatic theory (Gribakin and Kuchiev 1997 {Phys. Rev. A} {\bf 55} 3760) this is crucial for obtaining absolute values of the multiphoton cross sections. Comparisons with other calculations and experimental data are presented.
We report on the production of cold, state-selected H$_2^+$ molecular ions in a linear RF trap. The ions are produced by (3+1) resonance-enhanced multi-photon ionisation (REMPI) of H$_2$, and sympathetically cooled by laser-cooled Be$^+$ ions. After demonstrating and characterizing the REMPI process, we use photodissociation by a deep UV laser at 213~nm to verify the high vibrational purity of the produced H$_2^+$ ion samples. Moreover, the large difference between the photodissociation efficiencies of ions created in the $v=0$ and $v=1$ levels provides a way to detect a $v=0 \to 1$ transition…
Approximate scaling laws with respect to the nuclear charge are introduced for the time-dependent Dirac equation describing hydrogen-like ions subject to laser fields within the dipole approximation. In particular, scaling relations with respect to the laser wavelengths and peak intensities are discussed. The validity of the scaling relations is investigated for two-, three-, four-, and five-photon ionization of hydrogen-like ions with the nuclear charges ranging from $Z=1$ to $92$ by solving the corresponding time-dependent Dirac equations adopting the properly scaled laser parameters. Good a…
QED theory of multiphoton cascade transitions in atoms and ions is developed. In particular the $ 3s\rightarrow1s+2γ$, $ 4s\rightarrow1s+2γ$ and $ 3p\rightarrow1s+3γ$ processes are considered. Two different approaches (Quantum Electrodynamical and phenomenological Quantum Mechanical) are applied.
The multiphoton resonance transitions between ground hyperfine states are used for the time modulation of the electron capture decay of hydrogen like ions with the Gamow-Teller transition $1^+\to 0^+$. The proposed mechanism offers a time oscillating decay with the frequency up to 0.1 Hz. The experiment to observe the modulation is proposed for ions stored in a Penning trap. An attempt to understand the GSI anomaly with multiple photon transitions is made.
We investigate photodetachment from negative ions in a homogeneous 1.0-T magnetic field and a parallel electric field of approximately 10 V/cm. A theoretical model for detachment in combined fields is presented. Calculations show that a field of 10 V/cm or more should considerably diminish the Landau structure in the detachment cross section. The ions are produced and stored in a Penning ion trap and illuminated by a single-mode dye laser. We present preliminary results for detachment from S- showing qualitative agreement with the model. Future directions of the work are also discussed.
A theoretical study of the intense-field multiphoton ionization of hydrogenlike systems is performed by solving the time-dependent Dirac equation within the dipole approximation. It is shown that the velocity-gauge results agree to the ones in length gauge only if the negative-energy states are included in the time propagation. On the other hand, for the considered laser parameters, no significant difference is found in length gauge if the negative-energy states are included or not. Within the adopted dipole approximation the main relativistic effect is the shift of the ionization potential. A…
Double and triple detachment of the F-(1s2 2s2 2p6) negative ion by a single photon have been investigated in the photon energy range 660 to 1000 eV. The experimental data provide unambiguous evidence for the dominant role of direct photo-double-detachment with a subsequent single-Auger process in the reaction channel leading to F2+ product ions. Absolute cross sections were determined for the direct removal of a (1s+2p) pair of electrons from F- by the absorption of a single photon.
We have investigated multiphoton multiple ionization dynamics of argon and xenon atoms using a new x-ray free electron laser (XFEL) facility, SPring-8 Angstrom Compact free electron LAser (SACLA) in Japan, and identified that highly charged Xe ions with the charge state up to +26 are produced predominantly via four-photon absorption as well as highly charged Ar ions with the charge state up to +10 are produced via two-photon absorption at a photon energy of 5.5 keV. The absolute fluence of the XFEL pulse, needed for comparison between theory and experiment, has been determined using two-photon…
In a recent experiment at the VUV free-electron laser facility at DESY in Hamburg, the generation of multiply charged ions in a gas of atomic xenon was observed. This paper develops a theoretical description of multiphoton ionization of xenon and its ions. The numerical results lend support to the view that the experimental observation may be interpreted in terms of the nonlinear absorption of several VUV photons. The method rests on the Hartree-Fock-Slater independent-particle model. The multiphoton physics is treated within a Floquet scheme. The continuum problem of the photoelectron is solv…
Multiphoton detachment of F$^-$ by strong few-cycle laser pulses was studied by Shearer and Monteith using a Keldysh-type approach [Phys. Rev. A 88, 033415 (2013)]. We believe that this work contained errors in the calculation of the detachment amplitude and photoelectron spectra. We describe the necessary corrections to the theory and show that the results, in particular, the interference features of the photoelectron spectra, appear noticeably different.
QED theory of multiphoton cascade transitions in atoms and ions is developed. This theory allows for the accurate description of the process important for astrophysical studies of the cosmological hydrogen recombination. In particular the $ 3s\rightarrow1s+2γ$, $ 4s\rightarrow1s+2γ$ and $ 3p\rightarrow1s+3γ$ processes are considered and some controversies existing in the literature are resolved.
The quantum electrodynamical theory of the three-photon transitions in hydrogen-like ions is presented. Emission probabilities of various three-photon decay channels for $ 2p_{3/2} $, $ 2p_{1/2} $ and $ 2s_{1/2} $ states are calculated for the nuclear charge $Z$ values $1\leqslant Z \leqslant 95$. The results are given in two different gauges. The fully relativistic three-photon decay rates of hydrogen-like ions with half-integer nuclear spin are given for transitions between fine structure components. The results can be applied to the tests of the Bose-Einstein statistics for the multiphoton …
We review the recent experimental and theoretical progress in $K$-shell detachment studies of atomic anions. On the experimental side, this field has largely benefitted from technical advances at 3rd generation synchrotron radiation sources. For multiple detachment of C$^-$, O$^-$, and F$^-$ ions, recent results were obtained at the photon-ion merged-beams setup PIPE which is a permanent end station at beamline P04 of the PETRA III synchrotron light source in Hamburg. In addition to a much increased photon flux as compared to what was available previously, the PIPE setup has an extraordinary d…
Time projection chambers drifting negative ions (NITPC) instead of electrons have several advantages. A NITPC can operate at very high reduced drift fields without diffusion runaway, and the readout digitization sampling rate requirement is considerably relaxed due to the low drift speed of negative ions. The initiation of Townsend avalanches to allow gas gain in these devices has not been understood until now. It is shown here that the avalanche in low pressure CS$_2$ vapor is most likely initiated by collisional detachment of the electron from the negative molecular ion. In mixtures of Nitro…
We study the feasibility of nearly-degenerate two-photon rovibrational spectroscopy in ensembles of trapped, sympathetically cooled hydrogen molecular ions using a resonance-enhanced multiphoton dissociation (REMPD) scheme. Taking advantage of quasi-coincidences in the rovibrational spectrum, the excitation lasers are tuned close to an intermediate level to resonantly enhance two-photon absorption. Realistic simulations of the REMPD signal are obtained using a four-level model that takes into account saturation effects, ion trajectories, laser frequency noise and redistribution of population b…
The interaction between the field emission resonance states and the photodetached electron in an electric field is studied by semiclassical theory. An analytical expression of the photodetachment cross section is derived in the framework. It is found that the Stark shifted image state modulates the photodetachment cross section by adding irregular staircase or smooth oscillation in the spectrum. When the photodetached electron is trapped in Stark shifted image potential well, the detachment spectrum displays an irregular staircase structure which corresponds to the modified Rydberg series. Whi…
The photon-ion merged-beams technique was used at a synchrotron light source for measuring absolute cross sections of double and triple photodetachment of O$^{-}$ ions. The experimental photon energy range of 524-543 eV comprised the threshold for K-shell ionization. Using resolving powers of up to 13,000, the position, strength and width of the below-threshold 1s 2s2 2p6 2S resonance as well as the positions of the 1s 2s2 2p5 3P and 1s 2s2 2p5 1P thresholds for K-shell ionization were determined with high precision. In addition, systematically enlarged multi-configuration Dirac-Fock calculati…
We report on a kinematically complete experiment on strong field double ionization of helium using laser pulses with a wavelength of 394\,nm and intensities of $3.5-5.7\times10^{14}\,W/cm^2$. Our experiment reaches the most complete level of detail which previously has only been reached for single photon double ionization. We give an overview over the observables on many levels of integration, starting from the ratio of double to single ionization, the individual electron and ion momentum distributions over joint momentum and energy distributions to fully differential cross sections showing th…
We investigate ground state properties of singly charged chlorine (Cl$^-$) and gold (Au$^-$) negative ions by employing four-component relativistic many-body methods. In our approach, we attach an electron to the respective outer orbitals of chlorine (Cl) and gold (Au) atoms to determine the Dirac-Fock (DF) wave functions of the ground state configurations of Cl$^-$ and Au$^-$, respectively. As a result, all the single-particle orbitals see the correlation effects due to the appended electron of the negative ion. After obtaining the DF wave functions, lower-order many-body perturbation methods…
We investigate the interwoven dynamic evolutions of neutral nitrogen molecules together with nitrogen ions created through transient tunnel ionization in an intense laser field. By treating the molecules as open quantum systems, it is found that considering real-time injection of ions and strong couplings among their electronic states, nitrogen molecular ions are primarily populated in the electronically excited states, rather than staying in the ground state as predicted by the well-known tunneling theory. The unexpected result is attributed to sub-cycle switch-on of time-dependent polarizati…
The spin polarization of electrons from multiphoton ionization of Xe by 395 nm circularly polarized laser pulses at $6\cdot10^{13}$ W/cm$^2$ has been measured. At this photon energy of 3.14 eV the above threshold ionization peaks connected to Xe$^+$ ions in the ground state ($J=3/2$, ionization potential $I_p=12.1$ eV) and the first exicted state ($J=1/2$, $I_p=13.4$ eV) are clearly separated in the electron energy distribution. These two combs of ATI peaks show opposite spin polarizations. The magnitude of the spin polarization is a factor of two higher for the $J=1/2$ than for the $J=3/2$ fi…
We use (1+1$'$) resonance-enhanced multiphoton photodissociation (REMPD) to detect the population in individual rovibronic states of trapped HfF$^+$ with a single-shot absolute efficiency of 18%, which is over 200 times better than that obtained with fluorescence detection. The first photon excites a specific rotational level to an intermediate vibronic band at 35,000-36,500 cm$^{-1}$, and the second photon, at 37,594 cm$^{-1}$ (266 nm), dissociates HfF$^+$ into Hf$^+$ and F. Mass-resolved time-of-flight ion detection then yields the number of state-selectively dissociated ions. Using this met…
The level structure of negative-ions near the electron detachment limit dictates the low-energy scattering of an electron with the parent neutral atom. We demonstrate that a single ultracold atom bound inside a Rydberg orbit forming an ultralong-range Rydberg molecule provides an atomic-scale system which is highly sensitive to electron-neutral scattering and thus allows for detailed insights into the underlying near-threshold anion states. Our measurements reveal the so far unobserved fine structure of the $^3P_J$ triplet of Rb$^-$ and allow us to extract parameters of the associated $p$-wave…
