Energy of the 229Th nuclear clock transition.

Owing to its low excitation energy and long radiative lifetime, the first excited isomeric state of thorium-229, 229mTh, can be optically controlled by a laser1,2 and is an ideal candidate for the creation of a nuclear optical clock3, which is expected to complement and outperform current electronic-shell-based atomic clocks4. A nuclear clock will have various applications-such as in relativistic geodesy5, dark matter research6 and the observation of potential temporal variations of fundamental constants7-but its development has so far been impeded by the imprecise knowledge of the energy of 229mTh. Here we report a direct measurement of the transition energy of this isomeric state to the ground state with an uncertainty of 0.17 electronvolts (one standard deviation) using spectroscopy of the internal conversion electrons emitted in flight during the decay of neutral 229mTh atoms. The energy of the transition between the ground state and the first excited state corresponds to a wavelength of 149.7 ± 3.1 nanometres, which is accessible by laser spectroscopy through high-harmonic generation. Our method combines nuclear and atomic physics measurements to advance precision metrology, and our findings are expected to facilitate the application of high-resolution laser spectroscopy on nuclei and to enable the development of a nuclear optical clock of unprecedented accuracy.

X-ray pumping of the 229Th nuclear clock isomer.

The metastable first excited state of thorium-229, 229mTh, is just a few electronvolts above the nuclear ground state1-4 and is accessible by vacuum ultraviolet lasers. The ability to manipulate the 229Th nuclear states with the precision of atomic laser spectroscopy5 opens up several prospects6, from studies of fundamental interactions in physics7,8 to applications such as a compact and robust nuclear clock5,9,10. However, direct optical excitation of the isomer and its radiative decay to the ground state have not yet been observed, and several key nuclear structure parameters-such as the exact energies and half-lives of the low-lying nuclear levels of 229Th-remain unknown11. Here we present active optical pumping into 229mTh, achieved using narrow-band 29-kiloelectronvolt synchrotron radiation to resonantly excite the second excited state of 229Th, which then decays predominantly into the isomer. We determine the resonance energy with an accuracy of 0.07 electronvolts, measure a half-life of 82.2 picoseconds and an excitation linewidth of 1.70 nanoelectronvolts, and extract the branching ratio of the second excited state into the ground and isomeric state. These measurements allow us to constrain the 229mTh isomer energy by combining them with γ-spectroscopy data collected over the past 40 years.

Frequency conversion to the telecom O-band using pressurized hydrogen.

Large-scale quantum networks rely on optical fiber networks and photons as so-called flying qubits for information transport. While dispersion and absorption of optical fibers are minimum at the infrared telecom wavelengths, most atomic and solid state platforms operate at visible or near-infrared wavelengths. Quantum frequency conversion is required to bridge these two wavelength regimes, and nonlinear crystals are currently employed for this process. Here, we report a novel approach of frequency conversion to the telecom band. This interaction is based on coherent Stokes Raman scattering (CSRS), a four-wave mixing process resonantly enhanced in a dense molecular hydrogen gas. We show the conversion of photons from 863 nm to the telecom O-band and demonstrate that the input polarization state is preserved. This process is intrinsically broadband and can be adapted to any other wavelength.

Frequency conversion in pressurized hydrogen.

State-preserving frequency conversion in the optical domain is a necessary component in many configurations of quantum information processing and communication. Thus far, nonlinear crystals are used for this purpose. Here, we report on an approach based on coherent anti-Stokes Raman scattering (CARS) in a dense molecular hydrogen gas. This four-wave mixing process sidesteps the limitations imposed by crystal properties, it is intrinsically broadband and does not generate an undesired background. We demonstrate this method by converting photons from 434 nm to 370 nm and show that their polarization is preserved.

Converting single photons from an InAs/GaAs quantum dot into the ultraviolet: preservation of second-order correlations.

Wavelength conversion at the single-photon level is required to forge a quantum network from distinct quantum devices. Such devices include solid-state emitters of single or entangled photons, as well as network nodes based on atoms or ions. Here we demonstrate the conversion of single photons emitted from a III-V semiconductor quantum dot at 853 nm via sum frequency conversion to the wavelength of the strong transition of Yb+ ions at 370 nm. We measure the second-order correlation function of both the unconverted and the converted photon and show that the single-photon character of the quantum dot emission is preserved during the conversion process.

Frequency-quintupled laser at 308 nm for atomic physics applications.

We report on the development of a compact continuous-wave frequency-quintupled laser at 308 nm, which is based on a fiber laser operating in the telecom band. Three consecutive frequency conversion stages in nonlinear crystals are employed to achieve a 2ν+3ν=5ν frequency mixing. The performance of the laser system is demonstrated by linear absorption spectroscopy of a narrow intercombination line in zinc.

A Laser Excitation Scheme for

Direct laser excitation of the lowest known nuclear excited state in ^{229}Th has been a long-standing objective. It is generally assumed that reaching this goal would require a considerably reduced uncertainty of the isomer's excitation energy compared to the presently adopted value of (7.8±0.5) eV. Here we present a direct laser excitation scheme for ^{229m}Th, which circumvents this requirement. The proposed excitation scheme makes use of already existing laser technology and therefore paves the way for nuclear laser spectroscopy. In this concept, the recently experimentally observed internal-conversion decay channel of the isomeric state is used for probing the isomeric population. A signal-to-background ratio of better than 10^{4} and a total measurement time of less than three days for laser scanning appear to be achievable.

Laser cooling to quantum degeneracy.

We report on Bose-Einstein condensation in a gas of strontium atoms, using laser cooling as the only cooling mechanism. The condensate is formed within a sample that is continuously Doppler cooled to below 1 µK on a narrow-linewidth transition. The critical phase-space density for condensation is reached in a central region of the sample, in which atoms are rendered transparent for laser cooling photons. The density in this region is enhanced by an additional dipole trap potential. Thermal equilibrium between the gas in this central region and the surrounding laser cooled part of the cloud is established by elastic collisions. Condensates of up to 10(5) atoms can be repeatedly formed on a time scale of 100 ms, with prospects for the generation of a continuous atom laser.

Creation of ultracold Sr(2) molecules in the electronic ground state.

We report on the creation of ultracold (84)Sr(2) molecules in the electronic ground state. The molecules are formed from atom pairs on sites of an optical lattice using stimulated Raman adiabatic passage (STIRAP). We achieve a transfer efficiency of 30% and obtain 4×10(4) molecules with full control over the external and internal quantum state. STIRAP is performed near the narrow (1)S(0)-(3)P(1) intercombination transition, using a vibrational level of the 1(0(u)(+)) potential as an intermediate state. In preparation of our molecule association scheme, we have determined the binding energies of the last vibrational levels of the 1(0(u)(+)), 1(1(u)) excited-state and the X (1)Σ(g)(+) ground-state potentials. Our work overcomes the previous limitation of STIRAP schemes to systems with magnetic Feshbach resonances, thereby establishing a route that is applicable to many systems beyond alkali-metal dimers.

Bose-Einstein condensation of strontium.

We report on the attainment of Bose-Einstein condensation with ultracold strontium atoms. We use the (84)Sr isotope, which has a low natural abundance but offers excellent scattering properties for evaporative cooling. Accumulation in a metastable state using a magnetic-trap, narrowline cooling, and straightforward evaporative cooling in an optical trap lead to pure condensates containing 1.5 x 10(5) atoms. This puts (84)Sr in a prime position for future experiments on quantum-degenerate gases involving atomic two-electron systems.

Radioluminescence and photoluminescence of Th:CaF2 crystals.

We study thorium-doped CaF2 crystals as a possible platform for optical spectroscopy of the (229)Th nuclear isomer transition. We anticipate two major sources of background signal that might cover the nuclear spectroscopy signal: VUV-photoluminescence, caused by the probe light, and radioluminescence, caused by the radioactive decay of (229)Th and its daughters. We find a rich photoluminescence spectrum at wavelengths above 260 nm, and radioluminescence emission above 220 nm. This is very promising, as fluorescence originating from the isomer transition, predicted at a wavelength shorter than 200 nm, could be filtered spectrally from the crystal luminescence. Furthermore, we investigate the temperature-dependent decay time of the luminescence, as well as thermoluminescence properties. Our findings allow for an immediate optimization of spectroscopy protocols for both the initial search for the nuclear transition using synchrotron radiation, as well as future optical clock operation with narrow-linewidth lasers.