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Spectroscopic accuracy directly from quantum chemistry: application to ground and excited states of beryllium dimer

We combine explicit correlation via the canonical transcorrelation approach with the density matrix renormalization group and initiator full configuration interaction quantum Monte Carlo methods to compute a near-exact beryllium dimer curve, {\it without} the use of composite methods. In particular, our direct density matrix renormalization group calculations produce a well-depth of $D_e$=931.2 cm$^{-1}$ which agrees very well with recent experimentally derived estimates $D_e$=929.7$\pm 2$~cm$^{-1}$ [Science, 324, 1548 (2009)] and $D_e$=934.6~cm$^{-1}$ [Science, 326, 1382 (2009)]], as well the best composite theoretical estimates, $D_e$=938$\pm 15$~cm$^{-1}$ [J. Phys. Chem. A, 111, 12822 (2007)] and $D_e$=935.1$\pm 10$~cm$^{-1}$ [Phys. Chem. Chem. Phys., 13, 20311 (2011)]. Our results suggest possible inaccuracies in the functional form of the potential used at shorter bond lengths to fit the experimental data [Science, 324, 1548 (2009)]. With the density matrix renormalization group we also compute near-exact vertical excitation energies at the equilibrium geometry. These provide non-trivial benchmarks for quantum chemical methods for excited states, and illustrate the surprisingly large error that remains for 1$^1Σ^-_g$ state with approximate multi-reference configuration interaction and equation-of-motion coupled cluster methods. Overall, we demonstrate that explicitly correlated density matrix renormalization group and initiator full configuration interaction quantum Monte Carlo methods allow us to fully converge to the basis set and correlation limit of the non-relativistic Schrödinger equation in small molecules.

physics.chem-ph↗

A diabatic representation of the two lowest electronic states of Li3

Using the Multi-Reference Configuration Interaction method, the adiabatic potential energy surfaces of Li3 are computed. The two lowest electronic states are bound and exhibit a conical intersection. By fitting the calculated potential energy surfaces to the cubic Exe Jahn-Teller model we extract the effective Jahn-Teller parameters corresponding to Li3. These are used to set up the transformation matrix which transforms from the adiabatic to a diabatic representation. This diabatization method gives a Hamiltonian for Li3 which is free from singular adiabatic couplings and should be accurate for large internuclear distances, and it thereby allows for bound dynamics in the vicinity of the conical intersection to be explored.

physics.chem-ph↗

Magnetic-film atom chip with 10 $μ$m period lattices of microtraps for quantum information science with Rydberg atoms

We describe the fabrication and construction of a setup for creating lattices of magnetic microtraps for ultracold atoms on an atom chip. The lattice is defined by lithographic patterning of a permanent magnetic film. Patterned magnetic-film atom chips enable a large variety of trapping geometries over a wide range of length scales. We demonstrate an atom chip with a lattice constant of 10 $μ$m, suitable for experiments in quantum information science employing the interaction between atoms in highly-excited Rydberg energy levels. The active trapping region contains lattice regions with square and hexagonal symmetry, with the two regions joined at an interface. A structure of macroscopic wires, cut out of a silver foil, was mounted under the atom chip in order to load ultracold $^{87}$Rb atoms into the microtraps. We demonstrate loading of atoms into the square and hexagonal lattice sections simultaneously and show resolved imaging of individual lattice sites. Magnetic-film lattices on atom chips provide a versatile platform for experiments with ultracold atoms, in particular for quantum information science and quantum simulation.

physics.atom-ph↗

Compact two-electron wave function for bond dissociation and Van der Waals interactions: A natural amplitude assessment

Electron correlations in molecules can be divided in short range dynamical correlations, long range Van der Waals type interactions and near degeneracy static correlations. In this work we analyze for a one-dimensional model of a two-electron system how these three types of correlations can be incorporated in a simple wave function of restricted functional form consisting of an orbital product multiplied by a single correlation function $f(r_{12})$ depending on the interelectronic distance $r_{12}$. Since the three types of correlations mentioned lead to different signatures in terms of the natural orbital (NO) amplitudes in two-electron systems we make an analysis of the wave function in terms of the NO amplitudes for a model system of a diatomic molecule. In our numerical implementation we fully optimize the orbitals and the correlation function on a spatial grid without restrictions on their functional form. Due to this particular form of the wave function, we can prove that none of the amplitudes vanishes and moreover that it displays a distinct sign pattern and a series of avoided crossings as a function of the bond distance in agreement with the exact solution. This shows that the wave function Ansatz correctly incorporates the long range Van der Waals interactions. We further show that the approximate wave function gives an excellent binding curve and is able to describe static correlations. We show that in order to do this the correlation function $f(r_{12})$ needs to diverge for large $r_{12}$ at large internuclear distances while for shorter bond distances it increases as a function of $r_{12}$ to a maximum value after which it decays exponentially. We further give a physical interpretation of this behavior.

physics.chem-ph↗

In-Vacuum Active Electronics for Microfabricated Ion Traps

The advent of microfabricated ion traps for the quantum information community has allowed research groups to build traps that incorporate an unprecedented number of trapping zones. However, as device complexity has grown, the number of digital-to-analog converter (DAC) channels needed to control these devices has grown as well, with some of the largest trap assemblies now requiring nearly one hundred DAC channels. Providing electrical connections for these channels into a vacuum chamber can be bulky and difficult to scale beyond the current numbers of trap electrodes. This paper reports on the development and testing of an in-vacuum DAC system that uses only 9 vacuum feedthrough connections to control a 78-electrode microfabricated ion trap. The system is characterized by trapping single and multiple $^{40}$Ca$^+$ ions. The measured axial mode stability, ion heating rates, and transport fidelities for a trapped ion are comparable to systems with external(air-side) commercial DACs.

quant-ph↗

Dynamics of gas phase Ne$^*$ + NH$_3$ and Ne$^*$ + ND$_3$ Penning ionization at low temperatures

Two isotopic chemical reactions, $\mathrm{Ne}^*$ + NH$_3$, and $\mathrm{Ne}^*$ + ND$_3$, have been studied at low collision energies by means of a merged beams technique. Partial cross sections have been recorded for the two reactive channels, namely $\mathrm{Ne}^*$ + NH$_3$ $\rightarrow$ Ne + NH$_3^+$ + $e^-$, and $\mathrm{Ne}^*$ + NH$_3$ $\rightarrow$ Ne + NH$_2^+$ + H + $e^-$, by detecting the NH$_3^+$ and NH$_2^+$ product ions, respectively. The cross sections for both reactions were found to increase with decreasing collision energy, $E_{coll}$, in the range 8 $μ$eV$<E_{coll}<$ 20 meV. The measured rate constant exhibits a curvature in a log(k)-log($E_{coll}$) plot from which it is concluded that the Langevin capture model does not properly describe the $\mathrm{Ne}^*$ + NH$_3$ reaction in the entire range of collision energies covered here. Calculations based on multichannel quantum defect theory were performed to reproduce and interpret the experimental results. Good agreement was obtained by including long range van der Waals interactions combined with a 6-12 Lennard-Jones potential. The branching ratio between the two reactive channels, $Γ= \frac{[NH_2^+]}{[NH_2^+]+[NH_3^+]}$, is relatively constant, $Γ\approx 0.3$, in the entire collision energy range studied here. Possible reasons for this observation are discussed and rationalised in terms of relative time scales of the reactant approach and the molecular rotation. Isotopic differences between the $\mathrm{Ne}^*$ + NH$_3$ and $\mathrm{Ne}^*$ + ND$_3$ reactions are small, as suggested by nearly equal branching ratios and cross sections for the two reactions.

physics.chem-ph↗

High-intensity positron microprobe at the Thomas Jefferson National Accelerator Facility

We present a conceptual design for a novel continuous wave electron-linac based high-intensity high-brightness slow-positron production source with a projected intensity on the order of 10$^{10}$ e$^+$/s. Reaching this intensity in our design relies on the transport of positrons (T$_+$ below 600 keV) from the electron-positron pair production converter target to a low-radiation and low-temperature area for moderation in a high-efficiency cryogenic rare gas moderator, solid Ne. This design progressed through Monte Carlo optimizations of: electron/positron beam energies and converter target thickness, transport of the e$^+$ beam from the converter to the moderator, extraction of the e$^+$ beam from the magnetic channel, a synchronized raster system, and moderator efficiency calculations. For the extraction of e$^+$ from the magnetic channel, a magnetic field terminator plug prototype has been built and experimental results on the effectiveness of the prototype are presented. The dissipation of the heat away from the converter target and radiation protection measures are also discussed.

physics.acc-ph↗

Alkali vapor pressure modulation on the 100ms scale in a single-cell vacuum system for cold atom experiments

We describe and characterize a device for alkali vapor pressure modulation on the 100ms timescale in a single-cell cold atom experiment. Its mechanism is based on optimized heat conduction between a current-modulated alkali dispenser and a heat sink at room temperature. We have studied both the short-term behavior during individual pulses and the long-term pressure evolution in the cell. The device combines fast trap loading and relatively long trap lifetime, enabling high repetition rates in a very simple setup. These features make it particularly suitable for portable atomic sensors.

physics.atom-ph↗

Dynamic stabilization of the magnetic field surrounding the neutron electric dipole moment spectrometer at the Paul Scherrer Institute

The Surrounding Field Compensation (SFC) system described in this work is installed around the four-layer Mu-metal magnetic shield of the neutron electric dipole moment spectrometer located at the Paul Scherrer Institute. The SFC system reduces the DC component of the external magnetic field by a factor of about 20. Within a control volume of approximately 2.5m x 2.5m x 3m disturbances of the magnetic field are attenuated by factors of 5 to 50 at a bandwidth from $10^{-3}$ Hz up to 0.5 Hz, which corresponds to integration times longer than several hundreds of seconds and represent the important timescale for the nEDM measurement. These shielding factors apply to random environmental noise from arbitrary sources. This is achieved via a proportional-integral feedback stabilization system that includes a regularized pseudoinverse matrix of proportionality factors which correlates magnetic field changes at all sensor positions to current changes in the SFC coils.

physics.ins-det↗

Hybridizing matter-wave and classical accelerometers

We demonstrate a hybrid accelerometer that benefits from the advantages of both conventional and atomic sensors in terms of bandwidth (DC to 430 Hz) and long term stability. First, the use of a real time correction of the atom interferometer phase by the signal from the classical accelerometer enables to run it at best performances without any isolation platform. Second, a servo-lock of the DC component of the conventional sensor output signal by the atomic one realizes a hybrid sensor. This method paves the way for applications in geophysics and in inertial navigation as it overcomes the main limitation of atomic accelerometers, namely the dead times between consecutive measurements.

physics.atom-ph↗

Shot-noise-limited magnetometer with sub-pT sensitivity at room temperature

We report a photon shot-noise-limited (SNL) optical magnetometer based on amplitude modulated optical rotation using a room-temperature $^{85}$Rb vapor in a cell with anti-relaxation coating. The instrument achieves a room-temperature sensitivity of $70$ fT/$\sqrt{\mathrm{Hz}}$ at $7.6$ $μ$T. Experimental scaling of noise with optical power, in agreement with theoretical predictions, confirms the SNL behaviour from $5$ $μ$T to $75$ $μ$T. The combination of best-in-class sensitivity and SNL operation makes the system a promising candidate for application of squeezed light to a state-of-the-art atomic sensor.

quant-ph↗

High-resolution collision energy control through ion position modulation in atom-ion hybrid systems

We demonstrate an ion shuttling technique for high-resolution control of atom-ion collision energy by translating an ion held within a radio-frequency trap through a magneto-optical atom trap. The technique is demonstrated both experimentally and through numerical simulations, with the experimental results indicating control of ion kinetic energies from $0.05-1$ K with a fractional resolution of $\sim10$ and the simulations demonstrating that kinetic energy control up to $120$ K with a maximum predicted resolution of $\sim100$ is possible, offering order-of-magnitude improvements over most alternative techniques. Lastly, we perform a proof-of-principle chemistry experiment using this technique and outline how the method may be refined in the future and applied to the study of molecular ion chemistry.

physics.atom-ph↗

A low-steering piezo-driven mirror

We present a piezo-driven translatable mirror with excellent pointing stability, capable of driving at frequencies up to tens of kilohertz. Our system uses a tripod of piezo actuators with independently controllable drive voltages, where the ratios of the individual drive voltages are tuned to minimize residual tilting. Attached to a standard {\varnothing}= 12.7mm mirror, the system has a resonance-free mechanical bandwidth up to 51kHz, with displacements up to 2μm at 8kHz. The maximum static steering error is 5.5rad per micrometer displaced and the dynamic steering error is lower than 0.6rad/μm. This simple design should be useful for a large set of optical applications where tilt-free displacements are required, and we demonstrate its application in an ensemble of cold atoms trapped in periodically driven optical lattices.

physics.atom-ph↗

Non-destructive structural imaging of steelwork with atomic magnetometers

We demonstrate the imaging of ferromagnetic carbon steel samples and we detect the thinning of their profile with a sensitivity of 0.1 mm using a Cs radio-frequency atomic magnetometer. Images are obtained at room temperature, in magnetically unscreened environments. By using a dedicated arrangement of the setup and active compensation of background fields, the magnetic disturbance created by the samples' magnetization is compensated. Proof-of-concept demonstrations of non-destructive structural evaluation in the presence of concealing conductive barriers are also provided. The relevant impact for steelwork inspection and health and usage monitoring without disruption of operation is envisaged, with direct benefit for industry, from welding in construction to pipeline inspection and corrosion under insulation in the energy sector.

physics.ins-det↗

A New Quantum-Based Power Standard: Using Rydberg Atoms for a SI-Traceable Radio-Frequency Power Measurement Technique in Rectangular Waveguides

In this work we demonstrate an approach for the measurement of radio-frequency (RF) power using electromagnetically induced transparency (EIT) in a Rydberg atomic vapor. This is accomplished by placing alkali atomic vapor in a rectangular waveguide and measuring the electric (E) field strength (utilizing EIT and Autler-Townes splitting) for a wave propagating down the waveguide. The RF power carried by the wave is then related to this measured E-field, which leads to a new direct International System of Units (SI) measurement of RF power. To demonstrate this approach, we first measure the field distribution of the fundamental mode in the waveguide and then measure the power carried by the wave at both 19.629 GHz and 26.526 GHz. We obtain good agreement between the power measurements obtained with this new technique and those obtained with a conventional power meter.

physics.atom-ph↗

Method for Determination of Technical Noise Contributions to Ion Motional Heating

Microfabricated Paul ion traps show tremendous promise for large-scale quantum information processing. However, motional heating of ions can have a detrimental effect on the fidelity of quantum logic operations in miniaturized, scalable designs. In many experiments, contributions to ion heating due to technical voltage noise present on the static (DC) and radio frequency (RF) electrodes can be overlooked. We present a reliable method for determining the extent to which motional heating is dominated by residual voltage noise on the DC or RF electrodes. Also, we demonstrate that stray DC electric fields can shift the ion position such that technical noise on the RF electrode can significantly contribute to the motional heating rate. After minimizing the pseudopotential gradient experienced by the ion induced by stray DC electric fields, the motional heating due to RF technical noise can be significantly reduced.

quant-ph↗

Ultrafast extreme ultraviolet photoemission without space charge

Time- and Angle-resolved photoelectron spectroscopy from surfaces can be used to record the dynamics of electrons and holes in condensed matter on ultrafast time scales. However, ultrafast photoemission experiments using extreme-ultraviolet (XUV) light have previously been limited by either space-charge effects, low photon flux, or limited tuning range. In this article, we describe space-charge-free XUV photoelectron spectroscopy experiments with up to 5 nA of average sample current using a tunable cavity-enhanced high-harmonic source operating at 88 MHz repetition rate. The source delivers $ > 10^{11}$ photons/s in isolated harmonics to the sample over a broad photon energy range from 18 to 37 eV with a spot size of $58 \times 100 \; μ$m$^2$. From photoelectron spectroscopy data, we place conservative upper limits on the XUV pulse duration and photon energy bandwidth of 93 fs and 65 meV, respectively. The high photocurrent, lack of space charge distortions of the photoelectron spectra, and excellent isolation of individual harmonic orders allow us to observe the laser-assisted photoelectric effect with sideband amplitudes as low as $6 \times 10^{-4}$, enabling time-resolved XUV photoemission experiments in a qualitatively new regime.

physics.optics↗

A scalable hardware and software control apparatus for experiments with hybrid quantum systems

Modern experiments with fundamental quantum systems - like ultracold atoms, trapped ions, single photons - are managed by a control system formed by a number of input/output electronic channels governed by a computer. In hybrid quantum systems, where two or more quantum systems are combined and made to interact, establishing an efficient control system is particularly challenging due to the higher complexity, especially when each single quantum system is characterized by a different timescale. Here we present a new control apparatus specifically designed to efficiently manage hybrid quantum systems. The apparatus is formed by a network of fast communicating Field Programmable Gate Arrays (FPGAs), the action of which is administrated by a software. Both hardware and software share the same tree-like structure, which ensures a full scalability of the control apparatus. In the hardware, a master board acts on a number of slave boards, each of which is equipped with an FPGA that locally drives analog and digital input/output channels and radiofrequency (RF) outputs up to 400 MHz. The software is designed to be a general platform for managing both commercial and home-made instruments in a user-friendly and intuitive Graphical User Interface (GUI). The architecture ensures that complex control protocols can be carried out, such as performing of concurrent commands loops by acting on different channels, the generation of multi-variable error functions and the implementation of self-optimization procedures. Although designed for managing experiments with hybrid quantum systems, in particular with atom-ion mixtures, this control apparatus can in principle be used in any experiment in atomic, molecular, and optical physics.

physics.ins-det↗