Controlling 229Th isomeric state population in a VUV transparent crystal.

The radioisotope thorium-229 (229Th) is renowned for its extraordinarily low-energy, long-lived nuclear first-excited state. This isomeric state can be excited by vacuum ultraviolet (VUV) lasers and 229Th has been proposed as a reference transition for ultra-precise nuclear clocks. To assess the feasibility and performance of the nuclear clock concept, time-controlled excitation and depopulation of the 229Th isomer are imperative. Here we report the population of the 229Th isomeric state through resonant X-ray pumping and detection of the radiative decay in a VUV transparent 229Th-doped CaF2 crystal. The decay half-life is measured to 447(25) s, with a transition wavelength of 148.18(42) nm and a radiative decay fraction consistent with unity. Furthermore, we report a new "X-ray quenching" effect which allows to de-populate the isomer on demand and effectively reduce the half-life. Such controlled quenching can be used to significantly speed up the interrogation cycle in future nuclear clock schemes.

Growth and characterization of thorium-doped calcium fluoride single crystals.

We have grown [Formula: see text]Th:CaF[Formula: see text] and [Formula: see text]Th:CaF[Formula: see text] single crystals for investigations on the VUV laser-accessible first nuclear excited state of [Formula: see text]Th, with the aim of building a solid-state nuclear clock. To reach high doping concentrations despite the extreme scarcity (and radioactivity) of [Formula: see text]Th, we have scaled down the crystal volume by a factor 100 compared to established commercial or scientific growth processes. We use the vertical gradient freeze method on 3.2 mm diameter seed single crystals with a 2 mm drilled pocket, filled with a co-precipitated CaF[Formula: see text]:ThF[Formula: see text]:PbF[Formula: see text] powder in order to grow single crystals. Concentrations of [Formula: see text] cm[Formula: see text] have been realized with [Formula: see text]Th with good (> 10%) VUV transmission. However, the intrinsic radioactivity of [Formula: see text]Th drives radio-induced dissociation during growth and radiation damage after solidification. Both lead to a degradation of VUV transmission, currently limiting the [Formula: see text]Th concentration to [Formula: see text] cm[Formula: see text].

Measurement of the

We present a measurement of the low-energy (0-60 keV) γ-ray spectrum produced in the α decay of ^{233}U using a dedicated cryogenic magnetic microcalorimeter. The energy resolution of ∼10 eV, together with exceptional gain linearity, allows us to determine the energy of the low-lying isomeric state in ^{229}Th using four complementary evaluation schemes. The most precise scheme determines the ^{229}Th isomer energy to be 8.10(17) eV, corresponding to 153.1(32) nm, superseding in precision previous values based on γ spectroscopy, and agreeing with a recent measurement based on internal conversion electrons. We also measure branching ratios of the relevant excited states to be b_{29}=9.3(6)% and b_{42}<0.7%.

Nuclear Excitation of the

When Th nuclei are doped in CaF_{2} crystals, a set of electronic defect states appear in the crystal band gap which would otherwise provide complete transparency to vacuum-ultraviolet radiation. The coupling of these defect states to the 8 eV ^{229m}Th nuclear isomer in the CaF_{2} crystal is investigated theoretically. We show that although previously viewed as a nuisance, the defect states provide a starting point for nuclear excitation via electronic bridge mechanisms involving stimulated emission or absorption using an optical laser. The rates of these processes are at least 2 orders of magnitude larger than direct photoexcitation of the isomeric state using available light sources. The nuclear isomer population can also undergo quenching when triggered by the reverse mechanism, leading to a fast and controlled decay via the electronic shell. These findings are relevant for a possible solid-state nuclear clock based on the ^{229m}Th isomeric transition.

Phase Locking between Different Partial Waves in Atom-Ion Spin-Exchange Collisions.

We present a joint experimental and theoretical study of spin dynamics of a single ^{88}Sr^{+} ion colliding with an ultracold cloud of Rb atoms in various hyperfine states. While spin exchange between the two species occurs after 9.1(6) Langevin collisions on average, spin relaxation of the Sr^{+} ion Zeeman qubit occurs after 48(7) Langevin collisions, which is significantly slower than in previously studied systems due to a small second-order spin-orbit coupling. Furthermore, a reduction of the endothermic spin-exchange rate is observed as the magnetic field is increased. Interestingly, we find that while the phases acquired when colliding on the spin singlet and triplet potentials vary largely between different partial waves, the singlet-triplet phase difference, which determines the spin-exchange cross section, remains locked to a single value over a wide range of partial waves, which leads to quantum interference effects.

Direct Observation of Atom-Ion Nonequilibrium Sympathetic Cooling.

Sympathetic cooling is the process of energy exchange between a system and a colder bath. We investigate this fundamental process in an atom-ion experiment where the system is composed of a single ion trapped in a radio-frequency Paul trap and prepared in a classical oscillatory motion with total energy of ∼200 K, and the bath is an ultracold cloud of atoms at µK temperature. We directly observe the sympathetic cooling dynamics with single-shot energy measurements during one to several collisions in two distinct regimes. In one, collisions predominantly cool the system with very efficient momentum transfer leading to cooling in only a few collisions. In the other, collisions can both cool and heat the system due to nonequilibrium dynamics in the presence of the ion trap's oscillating electric fields. While the bulk of our observations agree well with a molecular-dynamics simulation of hard-sphere (Langevin) collisions, a measurement of the scattering angle distribution reveals forward-scattering (glancing) collisions which are beyond the Langevin model. This work paves the way for further nonequilibrium and collision dynamics studies using the well-controlled atom-ion system.

Publisher Correction: Spin-controlled atom-ion chemistry.

The original version of this Article contained an error in the third sentence of the first paragraph of the 'Spin polarizing the Sr+ ion with ultracold atoms' section of the Results, which incorrectly read 'The Langevin collision rate is 1.' The correct version adds 'kHz' after '1.' The fifth sentence of this same paragraph originally read as "Although 87Rb has a I = 3/2 nuclear spin and a hyperfine-split ground-state manifold, 88Sr has no nuclear spin and a Zeeman split two-fold ground state", which is incorrect. The correct version states "88Sr+" instead of "88Sr". The first sentence of the fourth paragraph of this same section originally read as "As the collisional energies are on the mK energy scale, spin exchange between Sr+ and Rb prepared in the F = 1 state is allowed only as long as it does not require Rb to change its hyperfine state and climb the 330 m hyperfine energy gap", which is incorrect. The correct version states "330 mK" instead of "330 m".In the Discussion section, the text was originally incorrectly repeated.This has been corrected in both the PDF and HTML versions of the Article.

Spin-controlled atom-ion chemistry.

Quantum control of chemical reactions is an important goal in chemistry and physics. Ultracold chemical reactions are often controlled by preparing the reactants in specific quantum states. Here we demonstrate spin-controlled atom-ion inelastic (spin-exchange) processes and chemical (charge-exchange) reactions in an ultracold Rb-Sr+ mixture. The ion's spin state is controlled by the atomic hyperfine spin state via spin-exchange collisions, which polarize the ion's spin parallel to the atomic spin. We achieve ~ 90% spin polarization due to the absence of strong spin-relaxation channel. Charge-exchange collisions involving electron transfer are only allowed for (RbSr)+ colliding in the singlet manifold. Initializing the atoms in various spin states affects the overlap of the collision wave function with the singlet molecular manifold and therefore also the reaction rate. Our observations agree with theoretical predictions.

Dynamics of a Ground-State Cooled Ion Colliding with Ultracold Atoms.

Ultracold atom-ion mixtures are gaining increasing interest due to their potential applications in ultracold and state-controlled chemistry, quantum computing, and many-body physics. Here, we studied the dynamics of a single ground-state cooled ion during few, to many, Langevin (spiraling) collisions with ultracold atoms. We measured the ion's energy distribution and observed a clear deviation from the Maxwell-Boltzmann distribution, characterized by an exponential tail, to a power-law distribution best described by a Tsallis function. Unlike previous experiments, the energy scale of atom-ion interactions is not determined by either the atomic cloud temperature or the ion's trap residual excess-micromotion energy. Instead, it is determined by the force the atom exerts on the ion during a collision which is then amplified by the trap dynamics. This effect is intrinsic to ion Paul traps and sets the lower bound of atom-ion steady-state interaction energy in these systems. Despite the fact that our system is eventually driven out of the ultracold regime, we are capable of studying quantum effects by limiting the interaction to the first collision when the ion is initialized in the ground state of the trap.

RBM7 subunit of the NEXT complex binds U-rich sequences and targets 3'-end extended forms of snRNAs.

The Nuclear Exosome Targeting (NEXT) complex is a key cofactor of the mammalian nuclear exosome in the removal of Promoter Upstream Transcripts (PROMPTs) and potentially aberrant forms of other noncoding RNAs, such as snRNAs. NEXT is composed of three subunits SKIV2L2, ZCCHC8 and RBM7. We have recently identified the NEXT complex in our screen for oligo(U) RNA-binding factors. Here, we demonstrate that NEXT displays preference for U-rich pyrimidine sequences and this RNA binding is mediated by the RNA recognition motif (RRM) of the RBM7 subunit. We solved the structure of RBM7 RRM and identified two phenylalanine residues that are critical for interaction with RNA. Furthermore, we showed that these residues are required for the NEXT interaction with snRNAs in vivo. Finally, we show that depletion of components of the NEXT complex alone or together with exosome nucleases resulted in the accumulation of mature as well as extended forms of snRNAs. Thus, our data suggest a new scenario in which the NEXT complex is involved in the surveillance of snRNAs and/or biogenesis of snRNPs.

NMR spectroscopic detection of chirality and enantiopurity in referenced systems without formation of diastereomers.

Enantiomeric excess of chiral compounds is a key parameter that determines their activity or therapeutic action. The current paradigm for rapid measurement of enantiomeric excess using NMR is based on the formation of diastereomeric complexes between the chiral analyte and a chiral resolving agent, leading to (at least) two species with no symmetry relationship. Here we report an effective method of enantiomeric excess determination using a symmetrical achiral molecule as the resolving agent, which is based on the complexation with analyte (in the fast exchange regime) without the formation of diastereomers. The use of N,N'-disubstituted oxoporphyrinogen as the resolving agent makes this novel method extremely versatile, and appropriate for various chiral analytes including carboxylic acids, esters, alcohols and protected amino acids using the same achiral molecule. The model of sensing mechanism exhibits a fundamental linear response between enantiomeric excess and the observed magnitude of induced chemical shift non-equivalence in the (1)H NMR spectra.

Recognition of asymmetrically dimethylated arginine by TDRD3.

Asymmetric dimethylarginine (aDMA) marks are placed on histones and the C-terminal domain (CTD) of RNA Polymerase II (RNAP II) and serve as a signal for recruitment of appropriate transcription and processing factors in coordination with transcription cycle. In contrast to other Tudor domain-containing proteins, Tudor domain-containing protein 3 (TDRD3) associates selectively with the aDMA marks but not with other methylarginine motifs. Here, we report the solution structure of the Tudor domain of TDRD3 bound to the asymmetrically dimethylated CTD. The structure and mutational analysis provide a molecular basis for how TDRD3 recognizes the aDMA mark. The unique aromatic cavity of the TDRD3 Tudor domain with a tyrosine in position 566 creates a selectivity filter for the aDMA residue. Our work contributes to the understanding of substrate selectivity rules of the Tudor aromatic cavity, which is an important structural motif for reading of methylation marks.

Colorimetric detection of trace water in tetrahydrofuran using N,N'-substituted oxoporphyrinogens.

Oxoporphyrinogens (OxPs) bind water molecules at pyrrolic NH and quinonoid carbonyl groups leading to visible colour changes due to variation in the π-electronic structure of OxPs. Introduction of hydrophilic substituents at two pyrrole NH groups improves sensitivity to H(2)O, and one OxP derivative is a colorimetric indicator of trace H(2)O (~50 ppm) in THF.