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High-resolution laser spectroscopy between 0.9 and 14.3 THz in a supersonic beam: Rydberg-Rydberg transitions of atomic Xe at intermediate n values
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FIG. 1.

Excitation scheme used to measure spectra of 33 Rydberg-Rydberg transitions of Xe. The transitions were detected by selective field ionization of the final 33 level. The figure illustrates the range of initial states corresponding to the frequency range from 0.9 THz ( = 31) to 14.3 THz ( = 16).

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FIG. 2.

Schematic optical layout of the spectrometer used to record VUV-THz double-resonance spectra. AOM: acousto-optical modulator; FR: Fresnel rhomb; PBS: polarization beamsplitter; OF: optical fiber; OI: optical isolator; DAST: -4-(dimethylamino)--methyl-4-stilbazolium tosylate crystal; OAPM: off-axis parabolic mirror; and PE: polyethylene window.

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FIG. 3.

Spectrometer used to record VUV-THz double-resonance spectra of Xe in a supersonic expansion. A: entrance window for NIR radiation; B: screw for lateral displacement of the DAST crystal; C and D: screws for adjusting the orientation of the DAST crystal; and E and F: screws to adjust the tilt angles of the off-axis parabolic mirror (see text for details). TOF: time-of flight.

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FIG. 4.

Spectrum of the 33[5/2] ← 17[3/2] transition of Xe plotted as a function of the wave number of the tunable NIR laser (a) and as a function of the difference of the wave numbers of the tunable and fixed-frequency NIR lasers (b). The top and middle traces in (a) represent the Doppler-free absorption spectrum of I and the transmission spectrum through an etalon, respectively. The asterisks designate transitions of Xe and Xe.

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FIG. 5.

Spectra of the 33 ← 31 transition of Xe recorded using pulse lengths of (a) 400 ns, (b) 200 ns, (c) 60 ns, (d) 20 ns, and (e) 10 ns. The assignments of the lines labeled 1–8 are given in Table I . The spectra have been shifted along the vertical axis for clarity.

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FIG. 6.

Effect of the NIR pulse length on the spectral resolution with the example of the 33[3/2] ← 31[3/2] transition of the = 0 isotopes of Xe. (a) and (b) display two measured NIR pulse shapes and (c) and (d) the corresponding spectral lineshapes.

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FIG. 7.

Fine and hyperfine structure of the 33 transitions of Xe for = 31 (a), 21 (b), 18 (c), 17 (d), and 16 (e). The assignments of the lines labeled 1–8 are given in Table I . Lines 9 and 10 correspond to the 33[3/2](5/2) ← 21[3/2](5/2) transitions of Xe and 33[3/2](3/2) ← 21[3/2](1/2) of Xe, respectively.

Image of FIG. 8.

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FIG. 8.

(a) Time-of-flight (TOF) spectrum of Xe ions formed following photoionization above the SP ionization threshold. Spectra of the 33 ← 31 transitions of Xe (b), Xe (c), and Xe (d) recorded following selective field ionization of the 33 level and measuring the ion signal at the relevant TOF position.


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Table I.

Assignments and relative positions (in cm) of the fine and hyperfine-structure components of the 33 ← 31 transitions observed in Fig. 5 .

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Table II.

Comparison of the NIR laser pulses with the measured (expt.) full widths at half-maximum (FWHM) of the Rydberg-Rydberg transitions. The calculated (calc.) widths were determined by convolution and Fourier-transformation assuming a Gaussian temporal profile of the NIR pulses.

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Table III.

Observed and calculated frequencies of the 33[3/2][3/2] and 33[5/2][3/2] transitions for n = 16, 17, 18, 21, 29, 30, and 31. The calculated frequencies were obtained using the set of MQDT parameters reported in Ref. .


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A laser-based, pulsed, narrow-band source of submillimeter-wave radiation has been developed that is continuously tunable from 0.1 THz to 14.3 THz. The source is based on difference-frequency mixing in the nonlinear crystal -4-(dimethylamino)--methyl-4-stilbazolium tosylate. By varying the pulse length, the bandwidth of the submillimeter-wave radiation can be adjusted between 85 MHz and 2.8 MHz. This new radiation source has been integrated in a vacuum-ultraviolet–submillimeter-ware double-resonance spectrometer, with which low-frequency transitions of atoms and molecules in supersonic beams can be detected mass-selectively by photoionization and time-of-flight mass spectrometry. The properties of the radiation source and spectrometer are demonstrated in a study of 33 Rydberg-Rydberg transitions in Xe with in the range 16–31. The frequency calibration of the submillimeter-wave radiation was performed with an accuracy of 2.8 MHz. The narrowest lines observed experimentally have a full-width at half-maximum of ∼3 MHz, which is sufficient to fully resolve the hyperfine structure of the Rydberg-Rydberg transitions of Xe and Xe. A total of 72 transitions were measured in the range between 0.937 THz and 14.245 THz and their frequencies are compared with frequencies calculated by multichannel quantum defect theory.


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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: High-resolution laser spectroscopy between 0.9 and 14.3 THz in a supersonic beam: Rydberg-Rydberg transitions of atomic Xe at intermediate n values