Deep-Ultraviolet Frequency Metrology of H_{2} for Tests of Molecular Quantum Theory.

Molecular hydrogen and its isotopic and ionic species are benchmark systems for testing quantum chemical theory. Advances in molecular energy structure calculations enable the experimental verification of quantum electrodynamics and potentially a determination of the proton charge radius from H_{2} spectroscopy. We measure the ground state energy in ortho-H_{2} relative to the first electronically excited state by Ramsey-comb laser spectroscopy on the EF^{1}Σ_{g}^{+}-X^{1}Σ_{g}^{+}(0,0) Q1 transition. The resulting transition frequency of 2 971 234 992 965(73) kHz is 2 orders of magnitude more accurate than previous measurements. This paves the way for a considerably improved determination of the dissociation energy (D_{0}) for fundamental tests with molecular hydrogen.

High-Precision Ramsey-Comb Spectroscopy at Deep Ultraviolet Wavelengths.

High-precision spectroscopy in systems such as molecular hydrogen and helium ions is very interesting in view of tests of quantum electrodynamics and the proton radius puzzle. However, the required deep ultraviolet and shorter wavelengths pose serious experimental challenges. Here we show Ramsey-comb spectroscopy in the deep ultraviolet for the first time, thereby demonstrating its enabling capabilities for precision spectroscopy at short wavelengths. We excite ^{84}Kr in an atomic beam on the two-photon 4p^{6}→4p^{5}5p[1/2]_{0} transition at 212.55 nm. It is shown that the ac-Stark shift is effectively eliminated, and combined with a counterpropagating excitation geometry to suppress Doppler effects, a transition frequency of 2 820 833 101 679(103) kHz is found. The uncertainty of our measurement is 34 times smaller than the best previous measurement, and only limited by the 27 ns lifetime of the excited state.