Precision-Spectroscopic Determination of the Binding Energy of a Two-Body Quantum System: The Hydrogen Atom and the Proton-Size Puzzle.

Precision measurements in Rydberg states of H with principal quantum number n in the range between 20 and 30 are reported. In the presence of homogeneous electric fields with strengths below 2 V cm^{-1}, these Rydberg states are subject to a linear Stark effect with accurately calculable Stark shifts. From the spectral positions of field-independent and field-dependent Rydberg-Stark states, we derive the n=20 and 24 Bohr energies, and the ionization energy with respect to the 2 ^{2}S_{1/2}(f=0,1) [short 2S(0,1)] metastable states. Combining these results with the 2S(1)-1S(1) transition frequency [C. G. Parthey et al., Phys. Rev. Lett. 107, 203001 (2011)PRLTAO0031-900710.1103/PhysRevLett.107.203001; A. Matveev et al., Phys. Rev. Lett. 110, 230801 (2013)PRLTAO0031-900710.1103/PhysRevLett.110.230801] and the 1S hyperfine splitting [L. Essen et al., Nature (London) 229, 110 (1971)NATUAS0028-083610.1038/229110a0], we determine the ionization frequency of the 1S(0) ground state to be 3 288 087 922 407.2(3.7)_{stat}(1.8)_{syst} kHz, which is the most precise value ever determined for the binding energy of a two-body quantum system. Using the 2S(0)-2P_{1/2}(1) interval [N. Bezginov et al., Science 365, 1007 (2019)SCIEAS0036-807510.1126/science.aau7807], we determine the Rydberg frequency to be cR_{∞}=3 289 841 960 204(15)_{stat}(7)_{syst}(13)_{2S-2P} kHz in a procedure that is insensitive to the value of the proton charge radius. These new results are discussed in the context of the proton-size puzzle.

Imaging-Assisted Single-Photon Doppler-Free Laser Spectroscopy and the Ionization Energy of Metastable Triplet Helium.

Skimmed supersonic beams provide intense, cold, collision-free samples of atoms and molecules and are one of the most widely used tools in atomic and molecular laser spectroscopy. High-resolution optical spectra are typically recorded in a perpendicular arrangement of laser and supersonic beams to minimize Doppler broadening. Typical Doppler widths are nevertheless limited to tens of MHz by the residual transverse-velocity distribution in the gas-expansion cones. We present an imaging method to overcome this limitation that exploits the correlation between the positions of the atoms and molecules in the supersonic expansion and their transverse velocities, and thus their Doppler shifts. With the example of spectra of (1s)(np) ^{3}P_{0-2}←(1s)(2s) ^{3}S_{1} transitions to high Rydberg states of metastable triplet He, we demonstrate the suppression of the residual Doppler broadening and a reduction of the full linewidths at half maximum to only about 1 MHz in the UV. Using a retroreflection arrangement for the laser beam and a cross-correlation method, we determine Doppler-free spectra without any signal loss from the selection, by imaging, of atoms within ultranarrow transverse-velocity classes. As an illustration, we determine the ionization energy of triplet metastable He and confirm the significant discrepancy between recent experimental [G. Clausen et al., Phys. Rev. Lett. 127, 093001 (2021)PRLTAO0031-900710.1103/PhysRevLett.127.093001] and high-level theoretical [V. Patkós et al., Phys. Rev. A 103, 042809 (2021)PLRAAN2469-992610.1103/PhysRevA.103.042809] values of this quantity.

SI-traceable frequency dissemination at 1572.06 nm in a stabilized fiber network with ring topology.

Frequency dissemination in phase-stabilized optical fiber networks for metrological frequency comparisons and precision measurements are promising candidates to overcome the limitations imposed by satellite techniques. However, in an architecture shared with telecommunication data traffic, network constraints restrict the availability of dedicated channels in the commonly-used C-band. Here, we demonstrate the dissemination of an SI-traceable ultrastable optical frequency in the L-band over a 456 km fiber network with ring topology, in which data traffic occupies the full C-band. We characterize the optical phase noise and evaluate a link instability of 4.7 × 10-16 at 1 s and 3.8 × 10-19 at 2000 s integration time, and a link accuracy of 2 × 10-18. We demonstrate the application of the disseminated frequency by establishing the SI-traceability of a laser in a remote laboratory. Finally, we show that our metrological frequency does not interfere with data traffic in the telecommunication channels. Our approach combines an unconventional spectral choice in the telecommunication L-band with established frequency-stabilization techniques, providing a novel, cost-effective solution for ultrastable frequency-comparison and dissemination, and may contribute to a foundation of a world-wide metrological network.

Ionization Energy of the Metastable 2

In a recent breakthrough in first-principles calculations of two-electron systems, Patkós, Yerokhin, and Pachucki [Phys. Rev. A 103, 042809 (2021)PLRAAN2469-992610.1103/PhysRevA.103.042809] have performed the first complete calculation of the Lamb shift of the helium 2 ^{3}S_{1} and 2 ^{3}P_{J} triplet states up to the term in α^{7}m. Whereas their theoretical result of the frequency of the 2 ^{3}P←2 ^{3}S transition perfectly agrees with the experimental value, a more than 10σ discrepancy was identified for the 3 ^{3}D←2 ^{3}S and 3 ^{3}D←2 ^{3}P transitions, which hinders the determination of the He^{2+} charge radius from atomic spectroscopy. We present here a new measurement of the ionization energy of the 2 ^{1}S_{0} state of He [960 332 040.491(32) MHz] which we use in combination with the 2 ^{3}S_{1}←2 ^{1}S_{0} interval measured by Rengelink et al. [Nat. Phys. 14, 1132 (2018).NPAHAX1745-247310.1038/s41567-018-0242-5] and the 2 ^{3}P←2 ^{3}S_{1} interval measured by Zheng et al. [Phys. Rev. Lett. 119, 263002 (2017)PRLTAO0031-900710.1103/PhysRevLett.119.263002] and Cancio Pastor et al. [Phys. Rev. Lett. 92, 023001 (2004)PRLTAO0031-900710.1103/PhysRevLett.92.023001] to derive experimental ionization energies of the 2 ^{3}S_{1} state [1152 842 742.640(32) MHz] and the 2 ^{3}P centroid energy [876 106 247.025(39) MHz]. These values reveal disagreements with the α^{7}m Lamb shift prediction by 6.5σ and 10σ, respectively, and support the suggestion by Patkós et al. of an unknown theoretical contribution to the Lamb shifts of the 2 ^{3}S and 2 ^{3}P states of He.

Spectroscopy of Highly Excited States of the Hydrogen Atom.

In this contribution, we describe the status of the development of a precision-spectroscopic experiment aimed at measuring transitions to states of high principal quantum number n of the hydrogen atom (H). These states form series (called Rydberg series) which converge for n → ∞ to the ionization threshold of H. The ionization energy of H can thus be determined directly by measuring the frequencies of transitions to high-n states and extrapolating the Rydberg series to n → ∞.

3CAPS - a structural AP-site analogue as a tool to investigate DNA base excision repair.

Abasic sites (AP-sites) are frequent DNA lesions, arising by spontaneous base hydrolysis or as intermediates of base excision repair (BER). The hemiacetal at the anomeric centre renders them chemically reactive, which presents a challenge to biochemical and structural investigation. Chemically more stable AP-site analogues have been used to avoid spontaneous decay, but these do not fully recapitulate the features of natural AP-sites. With its 3'-phosphate replaced by methylene, the abasic site analogue 3CAPS was suggested to circumvent some of these limitations. Here, we evaluated the properties of 3CAPS in biochemical BER assays with mammalian proteins. 3CAPS-containing DNA substrates were processed by APE1, albeit with comparably poor efficiency. APE1-cleaved 3CAPS can be extended by DNA polymerase ß but repaired only by strand displacement as the 5'-deoxyribophosphate (dRP) cannot be removed. DNA glycosylases physically and functionally interact with 3CAPS substrates, underlining its structural integrity and biochemical reactivity. The AP lyase activity of bifunctional DNA glycosylases (NTH1, NEIL1, FPG), however, was fully inhibited. Notably, 3CAPS-containing DNA also effectively inhibited the activity of bifunctional glycosylases on authentic substrates. Hence, the chemically stable 3CAPS with its preserved hemiacetal functionality is a potent tool for BER research and a potential inhibitor of bifunctional DNA glycosylases.

Precision Spectroscopy in Cold Molecules: The Lowest Rotational Interval of He_{2}

Multistage Zeeman deceleration was used to generate a slow, dense beam of translationally cold He_{2} molecules in the metastable a ^{3}Σ_{u}^{+} state. Precision measurements of the Rydberg spectrum of these molecules at high values of the principal quantum number n have been carried out. The spin-rotational state selectivity of the Zeeman-deceleration process was exploited to reduce the spectral congestion, minimize residual Doppler shifts, resolve the Rydberg series around n=200 and assign their fine structure. The ionization energy of metastable He_{2} and the lowest rotational interval of the X^{+} ^{2}Σ_{u}^{+} (ν^{+}=0) ground state of ^{4}He_{2}^{+} have been determined with unprecedented precision and accuracy by Rydberg-series extrapolation. Comparison with ab initio predictions of the rotational energy level structure of ^{4}He_{2}^{+} [W.-C. Tung, M. Pavanello, and L. Adamowicz, J. Chem. Phys. 136, 104309 (2012)] enabled us to quantify the magnitude of relativistic and quantum-electrodynamics contributions to the fundamental rotational interval of He_{2}^{+}.

Strand invasion properties and serum stability of alpha-tricyclo-DNA.

beta-tricyclo DNA (tcDNA) is a third generation antisense oligonucleotide developed and studied extensively in our laboratory. We recently became interested in the pairing properties of its alpha-anomeric form and observed parallel duplex formation with natural DNA and RNA. These duplexes were of the same level of thermal stability as their natural counterparts. In addition alpha-tcDNA exhibited poor thermal stability of antiparallel duplexes within its own backbone series which makes it a candidate for double strand invasion applications. Here we report on the strand invasion properties of alpha-tc-DNA and its stability in human serum.

Synthesis and pairing properties of alpha-tricyclo-DNA.

We describe the synthesis of the phosphoramidite building blocks of alpha-tricyclo-DNA (alpha-tc-DNA) covering all four natural bases, starting from the already known corresponding alpha-tc-nucleosides. These building blocks were used for the preparation of three alpha-tc-oligonucleotide 10-mers representing a homopurine, a homopyrimidine, and a mixed purine/pyrimidine base sequence. The base-pairing properties with complementary parallel and antiparallel oriented DNA and RNA were studied by UV-melting analysis and CD spectroscopy. We found that alpha-tc-DNA binds preferentially to parallel nucleic acid complements through Watson-Crick duplex formation, with a preference for RNA over DNA. In comparison with natural DNA, alpha-tc-DNA shows equal to enhanced affinity to RNA and also pairs to antiparallel DNA or RNA complements, although with much lower affinity. In the mixed-base sequence these antiparallel duplexes are of the reversed Watson-Crick type, while in the homopurine/homopyrimidine sequences Hoogsteen and/or reversed Hoogsteen pairing is observed. Antiparallel duplex formation of two alpha-tc-oligonucleotides was also observed, although the thermal stability of this duplex was surprisingly low. The base-pairing properties of alpha-tc-DNA are discussed in the context of alpha-DNA, alpha-RNA, and alpha-LNA.