Search

The ionization potential (IP) of radium monofluoride (RaF) was measured to be 4.969(2)[10] eV, revealing a relativistic enhancement in the series of alkaline earth monofluorides. The results are in agreement with a relativistic coupled-cluster prediction of 4.969[7] eV, incorporating up to quantum electrodynamics corrections. Using the same computational methodology, an improved calculation for the dissociation energy ($D_{0}$) of 5.54[5] eV is presented. This confirms that radium monofluoride joins the small group of diatomic molecules for which $D_{0}>\mathrm{IP}$, paving the way for precision control and interrogation of its Rydberg states.

Rapid progress in the experimental control and interrogation of molecules, combined with developments in precise calculations of their structure, are enabling new opportunities in the investigation of nuclear and particle physics phenomena. Molecules containing heavy, octupole-deformed nuclei such as radium are of particular interest for such studies, offering an enhanced sensitivity to the properties of fundamental particles and interactions. Here, we report precision laser spectroscopy measurements and theoretical calculations of the structure of the radioactive radium monofluoride molecule, $^{225}$Ra$^{19}$F. Our results allow fine details of the short-range electron-nucleus interaction to be revealed, indicating the high sensitivity of this molecule to the distribution of magnetization, currently a poorly constrained nuclear property, within the radium nucleus. These results provide a direct and stringent test of the description of the electronic wavefunction inside the nuclear volume, highlighting the suitability of these molecules to investigate subatomic phenomena.

We report the spectroscopy of 11 electronic states in the radioactive molecule radium monofluoride (RaF). The observed excitation energies are compared with state-of-the-art relativistic Fock-space coupled cluster (FS-RCC) calculations, which achieve an agreement of >99.71% (within ~8 meV) for all states. High-order electron correlation and quantum electrodynamics corrections are found to be important at all energies. Establishing the accuracy of calculations is an important step towards high-precision studies of these molecules, which are proposed for sensitive searches of physics beyond the Standard Model., Comment: Submitted for publication

The use of radioactive molecules for fundamental physics research is a developing interdisciplinary field limited dominantly by their scarce availability. In this work, radioactive molecular ion beams containing actinide nuclei extracted from uranium carbide targets are produced via the Isotope Separation On-Line technique at the CERN-ISOLDE facility. Two methods of molecular beam production are studied: extraction of molecular ion beams from the ion source, and formation of molecular ions from the mass-separated ion beam in a gas-filled radio-frequency quadrupole ion trap. Ion currents of U$^+$, UO$_{1-3}^+$, UC$_{1-3}^+$, UF$_{1-4}^+$, UF$_{1,2}$O$_{1,2}^+$ are reported. Metastable tantalum and uranium fluoride molecular ions are identified. Formation of UO$_{1-3}^+$, U(OH)$_{1-3}^+$, UC$_{1-3}^+$, UF$_{1,2}$O$_{1,2}^+$ from mass-separated beams of U$^+$, UF$_{1,2}^+$ with residual gas is observed in the ion trap. The effect of trapping time on molecular formation is presented., Comment: 6 pages, 7 figures

We report on a joint experimental and theoretical study of photoelectron circular dichroism (PECD) in methyloxirane. By detecting O 1s-photoelectrons in coincidence with fragment ions, we deduce the molecule's orientation and photoelectron emission direction in the laboratory frame. Thereby, we retrieve a fourfold differential PECD clearly beyond 50%. This strong chiral asymmetry is reproduced by ab initio electronic structure calculations. Providing such a pronounced contrast makes PECD of fixed-in-space chiral molecules an even more sensitive tool for chiral recognition in the gas phase., Comment: 5 figures

Isotope shifts of $^{223-226,228}$Ra$^{19}$F were measured for different vibrational levels in the electronic transition $A^{2}{}{\Pi}_{1/2}\leftarrow X^{2}{}{\Sigma}^{+}$. The observed isotope shifts demonstrate the particularly high sensitivity of radium monofluoride to nuclear size effects, offering a stringent test of models describing the electronic density within the radium nucleus. Ab initio quantum chemical calculations are in excellent agreement with experimental observations. These results highlight some of the unique opportunities that short-lived molecules could offer in nuclear structure and in fundamental symmetry studies., Comment: The paper was accepted for publication as a Letter in Physical Review Letters

Galaxy clusters are filled with hot, diffuse X-ray emitting plasma, with a stochastically tangled magnetic field whose energy is close to equipartition with the energy of the turbulent motions \cite{zweibel1997, Vacca}. In the cluster cores, the temperatures remain anomalously high compared to what might be expected considering that the radiative cooling time is short relative to the Hubble time \cite{cowie1977,fabian1994}. While feedback from the central active galactic nuclei (AGN) \cite{fabian2012,birzan2012,churazov2000} is believed to provide most of the heating, there has been a long debate as to whether conduction of heat from the bulk to the core can help the core to reach the observed temperatures \cite{narayan2001,ruszkowski2002,kunz2011}, given the presence of tangled magnetic fields. Interestingly, evidence of very sharp temperature gradients in structures like cold fronts implies a high degree of suppression of thermal conduction \cite{markevitch2007}. To address the problem of thermal conduction in a magnetized and turbulent plasma, we have created a replica of such a system in a laser laboratory experiment. Our data show a reduction of local heat transport by two orders of magnitude or more, leading to strong temperature variations on small spatial scales, as is seen in cluster plasmas \cite{markevitch2003}.

Many samples of current interest in molecular physics and physical chemistry exist in the liquid phase and are vaporized for the use in gas cells, diffuse gas targets or molecular gas jets. For some of these techniques the large sample consumption is a limiting factor. When rare, expensive molecules, such as chiral molecules or species with isotopic labels are used, wasting them in the exhaust line of the pumps is a quite expensive and inefficient approach. Therefore, we developed a closed-loop recycling system for molecules with vapor pressures below atmospheric pressure. Once filled, only a few valves have to be opened or closed and a cold trap must be moved. The recycling efficiency per turn exceeds 95 %., Comment: 5 pages, 4 figures

X-ray as well as electron diffraction are powerful tools for structure determination of molecules. Studies on randomly oriented molecules in the gas-phase address cases in which molecular crystals cannot be generated or the interaction-free molecular structure is to be addressed. Such studies usually yield partial geometrical information, such as interatomic distances. Here, we present a complementary approach, which allows obtaining insight to the structure, handedness and even detailed geometrical features of molecules in the gas phase. Our approach combines Coulomb explosion imaging, the information that is encoded in the molecular frame diffraction pattern of core-shell photoelectrons and ab initio computations. Using a loop-like analysis scheme we are able to deduce specific molecular coordinates with sensitivity even to the handedness of chiral molecules and the positions of individual atoms, as, e.g., protons., Comment: 13 pages, 3 figures

Radium compounds have attracted recently considerable attention due to both development of experimental techniques for high-precision laser spectroscopy of molecules with short-lived nuclei and amenability of certain radium compounds for direct cooling with lasers. Currently, radium monofluoride (RaF) is one of the most studied molecules among the radium compounds, both theoretically and recently also experimentally. Complementary studies of further diatomic radium derivatives are highly desired to assess the influence of chemical substitution on diverse molecular parameters, especially on those connected with laser cooling, such as vibronic transition probabilities, and those related to violations of fundamental symmetries. In this article high-precision \emph{ab initio} studies of electronic and vibronic levels of diatomic radium monochloride (RaCl) are presented. Recently developed approaches for treating electronic correlation with Fock-space coupled cluster methods are applied for this purpose. Theoretical results are compared to an early experimental investigation by Lagerqvist and used to partially reassign the experimentally observed transitions and molecular electronic levels of RaCl. Effective constants of $\mathcal{P}$-odd hyperfine interaction $W_{\rm{a}}$ and $\mathcal{P,T}$-odd scalar-pseudoscalar nucleus-electron interaction $W_{\rm{s}}$ in the ground electronic state of RaCl are estimated within the framework of a quasirelativistic Zeroth-Order Regular Approximation approach and compared to parameters in RaF and RaOH., Comment: 18 pages, 2 figures, 5 tables

The recent observation of non-classical electron transport regimes in two-dimensional materials has called for new high-resolution non-invasive techniques to locally probe electronic properties. We introduce a novel hybrid scanning probe technique to map the local resistance and electrochemical potential with nm- and $\mu$V resolution, and we apply it to study epigraphene nanoribbons grown on the sidewalls of SiC substrate steps. Remarkably, the potential drop is non uniform along the ribbons, and $\mu$m-long segments show no potential variation with distance. The potential maps are in excellent agreement with measurements of the local resistance. This reveals ballistic transport in ambient condition, compatible with micrometer-long room-temperature electronic mean free paths.

The study of molecular systems provides exceptional opportunities for the exploration of the fundamental laws of nature and for the search for physics beyond the Standard Model of particle physics. Measurements of molecules composed of naturally occurring nuclei have provided the most stringent upper bounds to the electron electric dipole moment to date, and offer a route to investigate the violation of fundamental symmetries with unprecedented sensitivity. Radioactive molecules - where one or more of their atoms possesses a radioactive nucleus - can contain heavy and deformed nuclei, offering superior sensitivity for EDM measurements as well as for other symmetry-violating effects. Radium monofluoride, RaF, is of particular interest as it is predicted to have an appropriate electronic structure for direct laser cooling. Furthermore, some Ra isotopes are known to be octupole deformed, thereby resulting in a large enhancement of their symmetry-violating nuclear moments. Until now,however, no experimental measurements of RaF have been performed, and their study is impeded by major experimental challenges, as no stable isotopes of radium exist. Here, we present a novel experimental approach to study short-lived radioactive molecules using the highly sensitive collinear resonance ionisation method. With this technique we have measured, for the first time, the energetically low-lying electronic states for each of the isotopically pure RaF molecules at the ISOLDE-CERN. Our results provide strong evidence of the existence of a suitable laser-cooling scheme for these molecules and constitute a pivotal step towards high-precision studies in these systems. Our findings open up new opportunities in the synthesis, manipulation and study of short-lived radioactive molecules, which will have a direct impact in many-body physics, astrophysics, nuclear structure, and fundamental physics research., Comment: Submitted

An overview from the past and an outlook for the future of fundamental laser-plasma interactions research enabled by emerging laser systems.

Laser plasma amplification of sub-picosecond pulses above the Joule level is demonstrated, a major milestone for this scheme to become a solution for the next-generation of ultra-high intensity lasers. By exploring over 6 orders of magnitude the influence of the incident seed intensity on Brillouin laser amplification, we reveal the importance of a minimum intensity to ensure an early onset of the self-similar regime, and a large energy transfer with a very high efficiency, up to 20%. Evidence of energy losses of the seed by spontaneous backward Raman is found at high amplification. The first three-dimensional envelope simulations of the sub-picosecond amplification were performed, supplemented by one-dimensional PIC simulations. Comparisons with the experimental results demonstrate the capability of quantitative predictions on the transferred energy. The global behavior of the amplification process, is reproduced, including the evolution of the spatial profile of the amplified seed.

Modern momentum imaging techniques allow for the investigation of complex molecules in the gas phase by detection of several fragment ions in coincidence. For these studies, it is of great importance that the single-particle detection efficiency e is as high as possible, as the overall efficiency scales with e over n, i.e. the power of the number of detected particles. Here we present measured absolute detection efficiencies for protons of several micro-channel plates (MCPs), including efficiency enhanced "funnel MCPs". Furthermore, the relative detection efficiency for two-, three-, four-, and five-body fragmentation of CHBrClF has been examined. The "funnel" MCPs exhibit an efficiency of approx. 90 percent, gaining a factor of 24 (as compared to "normal" MCPs) in case of a five-fold ion coincidence detection., Comment: 8 pages, 7 figues, submitted to Review of Scientific Instruments

Carrier multiplication by singlet exciton fission enhances photovoltaic conversion efficiencies in organic solids. This decay of one singlet exciton into two triplet states promises to overcome the Shockley-Queisser limit as up to two electrons may be harvested per absorbed photon. Intermolecular coupling is deemed mandatory for both, singlet exciton fission and a band-like transport. Such a coupling is manifested, $e.g.$, by the Davydov-splitting of the lowest-energy exciton transition in crystalline organic solids. For the model system perfluoropentacene, the corresponding transitions in the experimental, polarisation-resolved absorption spectra are identified by theoretical calculations based on the concept of H- and J- aggregation. Optical injection into the first vibronic progression of the fundamental exciton transitions significantly perturbs the higher-energy transitions that are associated to H-type aggregates of the $S_0 \rightarrow S_3$ transition during and following efficient singlet exciton fission. These findings underline the necessity for efficient carrier extraction as triplet accumulation may be detrimental to both, singlet exciton fission and any potentially band like transport. More generally, our observations indicate that electronic excitations can perturb the electronic band structure in organic crystals and highlight their correlated nature by potentially distorting the lattice.

Photoelectron circular dichroism refers to the forward/backward asymmetry in the photoelectron angular distribution with respect to the propagation axis of circularly polarized light. It has recently been demonstrated in femtosecond multi-photon photoionization experiments with randomly oriented camphor and fenchone molecules [C. Lux et al., Angew. Chem. Int. Ed. 51, 5001 (2012);C. S. Lehmann et al., J. Chem. Phys. 139, 234307 (2013)]. A theoretical framework describing this process as (2+1) resonantly enhanced multi-photon ionization is constructed, which consists of two-photon photoselection from randomly oriented molecules and successive one-photon ionisation of the photoselected molecules. It combines perturbation theory for the light-matter interaction with ab initio calculations for the two-photon absorption and a single-center expansion of the photoelectron wavefunction in terms of hydrogenic continuum functions. It is verified that the model correctly reproduces the basic symmetry behavior expected under exchange of handedness and light helicity. When applied it to fenchone and camphor, semi-quantitative agreement with the experimental data is found, for which a sufficient d wave character of the electronically excited intermediate state is crucial.

Collisional effects can play an essential role in the dynamics of plasma waves by setting a minimum damping rate and by interfering with wave-particle resonances. Kinetic simulations of the effects of electron-ion pitch angle scattering on Electron Plasma Waves (EPWs) are presented here. In particular, the effects of such collisions on the frequency and damping of small-amplitude EPWs for a range of collision rates and wave phase velocities are computed and compared with theory. Both the Vlasov simulations and linear kinetic theory find the direct contribution of electron-ion collisions to wave damping is about a factor of two smaller than is obtained from linearized fluid theory. To our knowledge, this simple result has not been published before. Simulations have been carried out using a grid-based (Vlasov) approach, based on a high-order conservative finite difference method for discretizing the Fokker-Planck equation describing the evolution of the electron distribution function. Details of the implementation of the collision operator within this framework are presented. Such a grid-based approach, which is not subject to numerical noise, is of particular interest for the accurate measurements of the wave damping rates., Comment: 44 pages, 11 figures

Relativistic ab initio calculations have been performed to assess the suitability of RaF for experimental search of P- and T,P-violating interactions. The parameters of P- and T,P-odd terms of the spin-rotational Hamiltonian have been calculated for the ${^2}\Sigma$ electronic ground state of RaF molecule. They include the parameter $W_a$, which is critical in experimental search for nuclear anapole moment and the parameters $W_d$ and $W_{\rm SP}$ required to obtain restrictions on the electric dipole moment of the electron and T,P-odd scalar-pseudoscalar interactions, respectively. The parameter $X$ corresponding to the "volume effect" in the T,P$-$odd interaction of the $^{223}$Ra nuclear Schiff moment with electronic shells of RaF has also been computed. Spectroscopic and hyperfine structure constants for $^{223}$RaF and $^{223}$Ra$^+$ have been computed as well, demonstrating the accuracy of the methods employed., Comment: 6 pages

We report high resolution neutron scattering measurements on the triangular lattice Mott insulator Na$_x$CrO$_2$ ($x$=1) which has recently been shown to exhibit an unusually broad fluctuating crossover regime extending far below the onset of spin freezing ($T_c\sim$41K). Our results show that below some crossover temperature ($T\sim0.75T_c$) a small incommensuration develops which helps resolve the spin frustration and drives three-dimensional magnetic order supporting coherent spin wave modes. This incommensuration assisted dimensional crossover suggests that inter-layer frustration is responsible for stabilizing the rare 2D correlated phase above 0.75$T_c$. In contrast to the host compound of 2D cobaltate superconductor such as Na$_x$CoO$_2$ ($\xi_c>50$\AA), no magnetic long-range order is observed down to 1.5K ($\xi_c<16$\AA)., Comment: 5 pages, 4 figures

The diatomic molecule radium monofluoride (RaF) has recently been proposed as a versatile probe for physics beyond the current standard model. Herein, a route towards production of a RaF molecular beam via radium ions is proposed. It takes advantage of the special electronic structure expected for group 2 halides and group 2 hydrides: The electronic ground state of neutral RaF and its monocation differ in occupation of a non-bonding orbital of $\sigma$ symmetry. This implies similar equilibrium distances and harmonic vibrational wavenumbers in the two charge states and thus favourable Franck--Condon factors for neutralisation without dissociation in neutralising collisions. According to the calculated ionisation energy of RaF, charge exchange collisions of RaF$^+$ with sodium atoms are almost iso-enthalpic, resulting in large cross-sections for the production of neutral radium monofluoride., Comment: 3 pages, 1 figure, 1 table, 1 ancillary file; references added in ancillary file

The particular advantages of using the diatomic molecule radium monofluoride (RaF) as a versatile molecular probe for physics beyond the Standard Model are highlighted. i) RaF was previously suggested as being potentially amenable to direct cooling with lasers. As shown in the present work, RaF's energetically lowest electronically excited state is of ${}^{2}\Pi$ symmetry (in contrast to BaF), such that no low-lying ${}^{2}\Delta$ state prevents efficient optical cooling cycles. ii) The effective electric field acting on the unpaired electron in the electronic ground state of RaF is estimated larger than in YbF, from which the best restrictions on the electron electric dipole moment (eEDM) were obtained experimentally. iii) Favourable crossings of spin-rotational levels of opposite parity in external magnetic fields exist, which are important for the measurement of the nuclear anapole moment of nuclei with a valence neutron. Thus, RaF appears currently as one of the most attractive candidates for investigation of parity-odd as well as simultaneously parity- and time-reversal-odd interactions in the realms of molecular physics., Comment: Minor correction of the 2013 manuscript version: Notes regarding theoretical estimate of omega_e added to caption and footnote of table 1 (conversion factors, uncertainty of fit, exchange of two entries), reference included and corrected, parity information in ancillary file corrected. 5 pages, 2 tables, ancillary file with 3 figures and additional details

The scaling of nuclear spin-dependent parity violating effects with increasing nuclear charge $Z$ is discussed in two series of isovalent open-shell diatomic molecules. The parameter $W_\mathrm{a}$ characterising the strength of parity violation in diatomic molecules is calculated in the framework of the zeroth-order regular approximation (ZORA) and found to be in good agreement with the $R(Z) Z^k$ scaling law derived for atoms in which $R(Z)$ represents a relativistic enhancement factor. The influence of electron correlation is studied on the molecular level, with spin-polarisation effects being conveniently accounted for by a previously established approximate relation between the hyperfine coupling tensor and $W_\mathrm{a}$. For high accuracy predictions of parity violating effects in radium fluoride the necessity for systematically improvable correlation calculations is emphasised., Comment: 17 pages, 2 figures, 4 tables; Results for copernicium hydride (CnH) added and included in figure 2, additional reference included, details concerning basis sets added and corrected, minor changes in text, tables and figures, typos corrected

The parameter $W_\mathrm{a}$, which characterizes nuclear spin-dependent parity violation effects within the effective molecular spin-rotational Hamiltonian, was computed for the electronic ground state of radium fluoride (RaF) and found to be one of the largest absolute values predicted so far. These calculations were performed with the complex generalised Hartree-Fock method within a two-component (quasi-relativistic) zeroth-order regular approximation framework. Peculiarities of the molecular electronic structure of RaF lead to highly diagonal Franck-Condon matrices between vibrational states of the electronic ground and first excited states, which renders the molecule in principle suitable for direct laser cooling. As a trapped gas of cold molecules offers a superior coherence time, RaF can be considered a promising candidate for high-precision spectroscopic experiments aimed at the search of molecular parity-violation effects., Comment: 4.5 pages, 1 figure, 2 tables. Supplementary material can be requested from the authors. Minor changes to version 1

The effect on parametric instability growth of pump wave incoherence is treated by deriving a set of equations governing the space-time evolution of the ensemble-average coupled-mode amplitudes and intensities. Particular attention is paid to establishing the regions of validity of the statistical description. Thresholds, growth rates, and amplification rates are given for both spatially and temporally incoherent pump waves. Both absolutely and convectively unstable modes are considered. The statistical results are verified where appropriate by numerical integration of the coupled-mode equations with different models of pump incoherence., Comment: 39 pages, 8 figures

The magnetic properties of $\alpha$-NaFeO$_2$ are studied by neutron diffraction and magnetization measurements. An ordered phase with spins aligned along the b$_hex$ axis exists at low temperatures (T < 4 K). At intermediate temperatures (4 K < T < 11 K), the system passes through an incommensurate ordered phase before transforming into a short range ordered state at higher temperatures that persists up to at least 50 K. Although the short range ordering does not persist to room temperature according to neutron diffraction, the magnetic susceptibility does not follow Curie-Weiss behavior, even up to 320 K. This rich magnetic behavior can be understood qualitatively as a competition between different magnetic exchange interactions that are similar in magnitude. The delicate balance between these interactions makes $\alpha$-NaFeO$_2$ a candidate for more detailed theoretical work to understand magnetic behavior in frustrated magnetic systems., Comment: Submitted to Phys Rev B, 7 pages, 8 figures

We report magnetization, specific heat, muon spin rotation and Na NMR measurements on the S=3/2 rhombohedrally stacked Heisenberg antiferromagnet NaCrO2. This compound appears to be an ideal candidate for the study of triangular Heisenberg antiferromagnets with very weak interlayer coupling. While specific heat and magnetization measurements indicate the occurrence of a transition in the range 40-46 K, both muon spin rotation and NMR reveal a fluctuating regime extending well below T_c, with a peak of relaxation rate 1/T1 around 30 K. This novel finding is discussed within the context of excitations in the triangular Heisenberg antiferromagnets., Comment: revised version