High‐resolution Photoelectron Spectroscopy

Merkt, Frédéric; Willitsch, Stefan; Hollenstein, U.

doi:10.1002/9780470749593.hrs071

Cited by 41 publications

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“…Ionization energies represent important thermochemical quantities and serve as reference data to test abinitio quantum chemical calculations of atomic and molecular structure. Numerous methods can be employed to measure ionization energies, including photoelectron spectroscopy in various variants [1,2], photoionization spectroscopy [3][4][5], photodetachment microscopy [6], and Rydberg-state spectroscopy in combination with Rydberg-series extrapolation [7].…”

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confidence: 99%

“…28 in Ref. [2]), approaching the accuracy of 100 MHz in the case of neutral polyatomic molecules [8] and singly negatively charged atoms and small molecules [6,9], and even surpassing this accuracy in special cases such as atoms [10,11] or molecular hydrogen [12]. With the rapid development of methods to generate cold samples of molecules [13][14][15][16] and the extension of frequency combs to shorter wavelengths [17,18], measurements of molecular ionization energies with sub-MHz precision are becoming possible by Rydberg-state spectroscopy.…”

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Precision measurement of the ionization energy of Cs i

et al. 2016

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We present absolute-frequency measurements for the transitions from the 6s 1/2 ground state of 133 Cs to np 1/2 and np 3/2 Rydberg states. The transition frequencies are determined by one-photon UV spectroscopy in ultracold samples of Cs atoms using a narrowband laser system referenced to a frequency comb. From a global fit of the ionization energy EI and the quantum defects of the two series we determine an improved value of EI = hc · 31 406.467 732 5(14) cm −1 for the ionization energy of Cs with a relative uncertainty of 5 × 10 −11 . We also report improved values for the quantum defects of the np 1/2 , np 3/2 , ns 1/2 , and nd 5/2 series.

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Precision measurement of the ionization energy of Cs i

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“…Schemes using these twophoton resonances for two-photon resonant sum-frequency (Hilber et al 1987, Marangos et al 1990) as well as difference-frequency mixing (Hilbig and Wallenstein 1982) were amply explored. Merkt and coworkers developed a multipurpose XUV spectrometer based on these schemes of narrow bandwidth and wide tunability up to 20 eV (Hollenstein et al 2000, Rupper andMerkt 2004), which was used in a wide variety of high-resolution spectroscopic applications (see Merkt et al 2011: High-resolution Photoelectron Spectroscopy, this handbook).…”

Section: Resonance Enhancement Effectsmentioning

confidence: 99%

Precision Laser Spectroscopy in the Extreme Ultraviolet

Eikema

Ubachs

2011

Handbook of High‐resolution Spectroscopy

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Techniques for the production of short wavelengths in the extreme ultraviolet wavelength range are described, spanning low‐order harmonic generation in the perturbative regime for narrow bandwidth XUV production to the plateau‐regime with the three‐step collisional model for the generation of high harmonics with broadband ultrafast pulses. In addition, the intermediate regime is discussed for pulses of 300 ps duration, as well as the regime of harmonic conversion based on continuous wave lasers aiming at the production of coherent Lyman‐α radiation. Applications of XUV sources in the frequency domain typically rely on the production of XUV‐light from narrowband Fourier‐transform‐limited pulses for recording high‐resolution spectra. Alternatively, harmonically upconverted pulses of ultrashort duration (with inter‐pulse coherence) can be used for spectroscopic studies in the time and frequency domain (such as direct frequency comb spectroscopy techniques). Examples of both approaches for atomic and molecular spectroscopy are discussed at some length. For precision metrology on atomic systems, a focus is put on the Lamb shift determination in the He ground state. In the realm of molecular spectroscopy, predissociation phenomena in the nitrogen molecule are highlighted, with relevance for dissociation processes occurring in the upper layers of the Earth atmosphere. Similar predissociation phenomena in carbon monoxide are also treated in some detail, in this case with relevance for the chemistry in interstellar clouds. Precision XUV spectroscopy of molecular hydrogen is discussed as well, as it relates to the possibility of detecting a variation of the proton–electron mass ratio on a cosmological time scale. In the last section, applications of direct frequency comb spectroscopic techniques at short wavelengths are explained and prospects are given for using these techniques at extreme ultraviolet wavelengths.

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“…[1][2][3][4] Since the first photoelectron spectroscopic studies of molecules in the 1960s, the resolution of the technique has steadily been improved, such that vibrational and thereon rotational structures were resolved during the following decades. [4][5][6] Along with the experimental progress, the theoretical understanding of molecular photoionization has been successively refined. Vibrational structure in the spectra can often be modeled in terms of the Franck-Condon principle (see, e.g., Ref.…”

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Fine- and hyperfine-structure effects in molecular photoionization. I. General theory and direct photoionization

Germann

Willitsch

2016

The Journal of Chemical Physics

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We develop a model for predicting fine-and hyperfine intensities in the direct photoionization of molecules based on the separability of electron and nuclear spin states from vibrational-electronic states. Using spherical tensor algebra, we derive highly symmetrized forms of the squared photoionization dipole matrix elements from which we derive the salient selection and propensity rules for fineand hyperfine resolved photoionizing transitions. Our theoretical results are validated by the analysis of the fine-structure resolved photoelectron spectrum of O 2 reported by Palm and Merkt [Phys. Rev. Lett. 81, 1385 (1998)] and are used for predicting hyperfine populations of molecular ions produced by photoionization. Published by AIP Publishing. [http://dx

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High‐resolution Photoelectron Spectroscopy

Cited by 41 publications

References 138 publications

Precision measurement of the ionization energy of Cs i

Precision measurement of the ionization energy of Cs i

Precision Laser Spectroscopy in the Extreme Ultraviolet

Fine- and hyperfine-structure effects in molecular photoionization. I. General theory and direct photoionization

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