† Corresponding author. E-mail:
Project supported by the National Natural Science Foundation of China (Grant No. 11174218).
The branching ratios of ions and the angular distributions of electrons ejected from the Eu 4f76p1/2nd auto-ionizing states are investigated with the velocity-map-imaging technique. To populate the above auto-ionizing states, the relevant bound Rydberg states have to be detected first. Two new bound Rydberg states are identified in the region between 41150 cm−1 and 44580 cm−1, from which auto-ionization spectra of the Eu 4f76p1/2nd states are observed with isolated core excitation method. With all preparations above, the branching ratios from the above auto-ionizing states to different final ionic states and the angular distributions of electrons ejected from these processes are measured systematically. Energy dependence of branching ratios and anisotropy parameters within the auto-ionization spectra are carefully analyzed, followed by a qualitative interpretation.
For the last decade, spectra of highly excited states of rare-earth atoms[1–3] have attracted considerable attention. Although the position and width, as well as the line shape of an auto-ionizing resonance on both Eu and Sm atoms, have been reported,[4–6] they are only relevant to total cross section of auto-ionization, yielding no information on the dynamical process of auto-ionization, such as the final states of ions, and phases of the wave function of the ejected electrons. A more stringent test of future new theory on the rare-earth atoms is to measure the branching ratios (BR) of ions and the angular distributions (AD) of electrons ejected from auto-ionizing states, as the BR may provide the information of final ionic states, while the AD represents the differential cross section of auto-ionization, providing the information about phases of possible transition channels, which is important to the physical world.[7–9]
Systematic studies of the BR and the AD on the mp1/2nd auto-ionizing states of alkaline-earth atoms[10,11] have been carried out previously with the time-of-flight (TOF) method,[12,13] while similar investigations on the rare-earth atoms have been reported on the Eu 4f76p1/26d auto-ionizing state[14,15] until recently. Although the advanced velocity-map-imaging (VMI) method,[16–18] developed originally for the photo-dissociation of molecules, was employed there, to avoid rotating the axis of the polarizer, lack of systematic studies on the 4f76p1/2nd auto-ionizing states in terms of more n values is obvious. Additionally, there will be more final ionic states involved for the higher 4f76p1/2nd auto-ionizing states with n > 6, more challenge has to be faced than that for the 4f76p1/26d state. Based on the above facts, a systematic study of the spectra, the BR, and the AD of the 4f76p1/2nd auto-ionizing states, taking n = 7–9 for instance, with the VMI technique is a significant task.
In Section 2 the experimental setup and methods will be presented, while the results of the BR and the AD of auto-ionization process will be discussed in Section 3. In Section 4 some conclusions will be drawn.
Since the experimental apparatus used for measuring the auto-ionization BR and the AD of ejected electrons from Eu auto-ionizing states have been described in our previous work,[9] only a brief description will be given here. As shown in Fig.
A Eu atomic beam is produced by a resistively heated production system inside a vacuum chamber, whose pressure is kept at 10−5 Pa.
The three-step excitation in the experiment requires three pulsed dye lasers operated at 20 Hz, pumped by the 2nd or 3rd harmonic generation (at wavelength of 532 nm or 355 nm) of the same pulsed Nd:YAG laser. Each dye laser outputs laser pulses with a line width of 0.2 cm−1, pulse width of 5–8 ns, and pulse energy of 0.5 mJ. Having passed through three linear polarizers, the three dye laser beams are propagating collinearly, and crossed with the atomic beam perpendicularly in the interaction region to avoid the Doppler broadening effect. The laser pulses of the second and the third lasers are time-delayed properly, so that the three laser pulses are sequential in time. The laser polarization directions are set with three polarizers to be perpendicular to the electric field.
The signal collection system mainly includes an electron lens,[19] a position sensitive detector (PSD), a phosphor screen (PS), and a charge coupled device (CCD). Electrons produced in the interaction region are focused by a suitable electron lens and impacted onto the PSD. The fluorescence from the PS is captured by the CCD camera and transferred to a computer for the further data analysis.
To investigate the 4f76p1/2nd auto-ionizing states, it is preferable to use the three-step isolated core excitation (ICE) method,[20] which has been utilized extensively in studies of alkaline-earth and rare-earth atoms, and has several advantages: i) only low power is required for each excitation laser; ii) the spectrum obtained by ICE is simple, where interference effects can be reduced significantly for lower-n states; iii) the n values of the 4f76p1/2nd auto-ionizing states are determined by the 4f76snd states, which is the initial states of the third-step excitation, 4f76snd→4f76p1/2nd. However, since the 4f76snd states have been known for n = 6 and 7 only,[21] one has to begin with detecting the 4f76snd states (n > 6) for studying the 4f76p1/2nd (n > 6) auto-ionizing series.
To detect the 4f76snd states in the region of 41150–44580 cm−1, a two-color three-photon resonant ionization method[22] is employed. Furthermore, the three different paths, named Scheme I, II, and III, are designed, to uniquely determine the total angular momentum of 4f76snd states. According to the selection rule ΔJ = 0, ±1, the possible values of angular momentum J0 for the detected Rydberg states with Scheme I are 3/2, 5/2, or 7/2, with Scheme II are 5/2, 7/2, or 9/2, and the possible values of J0 are 7/2, 9/2, or 11/2 with Scheme III. For example, J=9/2 can be assigned to the states that can only be detected with Scheme III.
Scheme I:
Scheme II:
Scheme III:
As illustrated above, the wavelength of the first lasers, λ1, are fixed at 466.32 nm, 462.85 nm, and 459.53 nm to excite the Eu atom to three different 4f76s6p states, respectively. The wavelength of the second laser, λ2, is tuned over a certain range, to excite the Eu atom to many highly excited states, including some 4f76snd states, which can be detected by absorbing another λ2 photon, as shown in Fig.
As shown in Fig.
As shown in Table
In order to obtain the total cross section of Eu 4f76p1/2nd series states, this work uses three different intermediate states in the ICE excitation scheme, namely,
Scheme IV:
Scheme V:
Scheme VI:
Electrons ejected from the process of auto-ionizing are probed by the VMI method.[16–18] Figure
As shown in Fig.
In the present study, several parameters of VMI will be adjusted in order to obtain the most accurate data. To ensure that the electrons ejected from the auto-ionization are located accurately, it is necessary for the spatial location of the image with VMI to be calibrated. Namely, the ejected electrons with zero kinetic energy should be in the center of the image. In addition, the brightness calibration of the VMI image leads to the uncertainty in boundaries within which angular integral is undertaken. In general, the uncertainty of this experiment is estimated to be 5%.
Before describing the BR of ions and the AD of ejected electrons from 4f76p1/2nd states, the auto-ionization spectra of 4f76p1/2nd states will be discussed briefly. Eu atoms can be excited from the ground state to 4f76p1/2nd auto-ionizing states by absorbing three photons, while auto-ionization spectra of 4f76p1/2nd states are obtained by collecting the ions due to the instability of auto-ionization states.
For example, the auto-ionization spectrum (solid line) of 4f76p1/27d state together with the Lorentzian fitting result (dashed line) is shown in Fig.
According to the above discussion, it is curious to know whether there is difference between 4f76p1/27d and 4f76p1/2nd (n = 8, 9) auto-ionizing states in terms of their spectra. As expected, the auto-ionization spectra of 4f76p1/28d and 9d states with the Lorentzian fitting results (dashed line) shown in Fig.
Since λ3 is scanned across the
With the combination of Figs.
The energies of the three 4f76p1/2nd auto-ionizing states are different, leading to 4f76p1/2nd auto-ionizing states interacting with different 4f75dnl states. Therefore, the three auto-ionization spectra have different complexity. Obviously, the spectrum of 4f76p1/28d state is the simplest one, while 4f76p1/29d state is the most complex.
Furthermore, the comparison between Figs.
Because the energy of 4f76p1/29d state approaches the
Since the spectra of 4f76p1/2nd states provide no information about the dynamical process of auto-ionization and energy conservation results in one-to-one correspondence between the energy of the ejected electrons and the final ionic states, the energy of the ejected electrons is analyzed instead to determine the final states.
Energy distribution of ejected electrons, which can be extracted from fitting the Abel-inverted image, is a key factor in the experiment. An example is shown in Fig.
As shown in Fig.
One of the primary objectives of the present work is to discuss the BR of the 4f76p1/2nd states, which can be extracted from the energy distributions of elected electrons based on the areas under different profiles. Let BR1, BR2, BR3, and BR4 be the BRs to the four different ionic states 4f76s+(9So), 4f76s+(7So), 4f75d+(9Do), and 4f75d+(7Do) in Figs.
As shown in Fig.
Similar measurements and analysis are performed for 4f76p1/28d state, and the final results are presented in Fig.
The population inversion between 4f75d+(9Do) and two 4f76s+ionic states is still kept in the whole energy region. However, several differences between Figs.
The last example is shown in Fig.
More interestingly, BR3 is much larger than BR12 in the energy region of 66552.4–66917.4 cm−1, and also BR4 is much larger than BR12 in the energy region of 66445.1–66532.8 cm−1. This means that population inversion is not only between 4f75d+(9Do) and 4f76s+, but also between 4f75d+(7Do) and 4f76s+ionic state. This phenomenon can be partially attributed to the fact that the J value of 4f76p1/29d is bigger than those of the other two auto-ionizing states. Furthermore, the BRs of the 4f76p1/29d auto-ionizing state to the 4f76s+, 4f75d+(9Do), and 4f75d+(7Do) ionic states fluctuate from 24% to 50%, 28% to 46%, and 16% to 44%, respectively.
After the partial cross section of 4f76p1/2nd auto-ionizing states, it is time to discuss the differential cross section. In addition, the AD of ejected electrons allows one to obtain more detailed information.
Both symmetry considerations and angular momentum selection rules constrain AD from the 4f76p1/2nd states to be of the form
From Table
As can be seen from Fig.
As seen from Fig.
Meanwhile, the AD diagrams should be of much interest, because they reveal more intuitive space distribution of ejected electrons. AD patterns may be generated in every energy point, but only some examples will be discussed below. For example, AD patterns of electrons ejected from 4f76p1/27d auto-ionizing state together with auto-ionization spectrum and one β spectrum are shown in Fig.
As the three excitation lasers apply an additional force on the electron cloud in the direction of the polarization axis, the expected propensity of the AD is the electrons that are mainly ejected along the direction of the polarization axis, such as the AD patterns marked with 2 and 4. However, the unexpected patterns of the ADs marked with 1 and 5 are also discovered in Fig.
In order to make a comparison, another example for the AD patterns of 4f76p1/29d state is shown in Fig.
What can be seen from Fig.
As seen from Figs.
The last example is shown in Fig.
The relation between the AD patterns and the spectrum of β parameter can also be seen from Fig.
A comparison of Figs.
A detailed study of the auto-ionization dynamics of Eu atom, which consists of the auto-ionization spectra, the BRs of ions, and the ADs of ejected electrons, is undertaken. From the systematical study of the auto-ionization spectra of multiple d states, it is found that the ICE method is valid for the higher-n 6pnl auto-ionizing state of the Eu. Both the auto-ionization spectra and the BRs of the 4f76p1/2nd auto-ionizing states reveal the complex configuration interaction between 4f76p1/2nd auto-ionizing states and the 4f75dnl auto-ionizing series. The link between AD patterns and the β spectrum is a significant finding from the systematic study, indicating that the AD patterns are not only influenced by the Rydberg–continuum coupling but also by the complex channel interactions.
On the whole, 4f76p1/29d auto-ionizing state is a particular state that belongs to 4f76p1/2nd, but it is the different 4f76p1/27d state and 4f76p1/28d state in case of the auto-ionizing spectrum, the auto-ionization BRs and the ADs of ejected electrons. Furthermore, in view of the specificity of 4f76p1/29d state, 4f76p3/2nl auto-ionizing series states need to be investigated further.
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