The decay rate $\gam$ of an excited dipole molecule inside a waveguide is evaluated for the strongly coupled matter-field case near a cutoff frequency $\ome_c$ without using perturbation analysis. Due to the singularity in the density of photon states at the cutoff frequency, we find that $\gam$ depends non-analytically on the coupling constant $\ggg$ as $\ggg^{4/3}$. In contrast to the ordinary evaluation of $\gam$ which relies on the Fermi golden rule (itself based on perturbation analysis), $\gam$ has an upper bound and does not diverge at $\ome_c$ even if we assume perfect conductance in the waveguide walls. As a result, again in contrast to the statement found in the literature, the speed of emitted light from the molecule does not vanish at $\ome_c$ and is proportional to $c\ggg^{2/3}$ which is on the order of $10^3 \sim 10^4$ m/s for typical dipole molecules.
Deactivation of broad quasi-one-dimensional dibosonic molecules is analyzed. Within integrable Lieb-Liniger-McGuire (LLMG) model an exact expression does not demonstrate suppression of the deactivation at low collision energies. Solution of Faddeev equations demonstrates that when a Feshbach resonance lifts the symmetry of the LLMG model the deactivation becomes suppressed. This effect shows a way for formation of a stable gas of dibosonic Feshbach molecules.
An integrated optical dipole trap uses two-color (red and blue-detuned) traveling evanescent wave fields for trapping cold neutral atoms. To achieve longitudinal confinement, we propose using an integrated optical waveguide coupler, which provides a potential gradient along the beam propagation direction sufficient to confine atoms. This integrated optical dipole trap can support an atomic ensemble with a large optical depth due to its small mode area. Its quasi-TE0 waveguide mode has an advantage over the HE11 mode of a nanofiber, with little inhomogeneous Zeeman broadening at the trapping re…
We propose an experiment to measure the electric dipole moment of the electron using ultracold YbF molecules. The molecules are produced as a thermal beam by a cryogenic buffer gas source, and brought to rest in an optical molasses that cools them to the Doppler limit or below. The molecular cloud is then thrown upward to form a fountain in which the electric dipole moment of the electron is measured.
We explore the quantum dynamics of heteronuclear atomic collisions in waveguides and demonstrate the existence of a novel mechanism for the resonant formation of polar molecules. The molecular formation probabilities can be tuned by changing the trap frequencies characterizing the transverse modes of the atomic species. The origin of this effect is the confinement-induced mixing of the relative and center of mass motions in the atomic collision process leading to a coupling of the diatomic continuum to center of mass excited molecular states in closed transverse channels.
We demonstrate one-dimensional sub-Doppler laser cooling of a beam of YbF molecules to 100 $μ$K. This is a key step towards a measurement of the electron's electric dipole moment using ultracold molecules. We compare the effectiveness of magnetically-assisted and polarization-gradient sub-Doppler cooling mechanisms. We model the experiment and find good agreement with our data.
Heavy polar diatomic molecules are the leading candidates in searches for the permanent electric dipole moment of the electron (eEDM). Next-generation eEDM search experiments ideally require extremely large coherence times, in large ensembles of trapped molecules that have a high sensitivity to the eEDM. We consider a family of molecules, mercury-alkali diatomics, that can be feasibly produced from ultracold atoms. We present calculations of the effective electric fields experienced by the electron in these molecules. The combination of reasonably large effective electric fields, and a straigh…
Because molecules can have their orientation locked when embedded into a solid rare-gas matrix, their hyperfine structure is strongly perturbed relative to the freely rotating molecule. The addition of an electric field further perturbs the structure, and fields parallel and antiparallel to the molecular orientation result in different shifts of the hyperfine structure. These shifts enable the selective detection of molecules with different orientations relative to the axes of a rare-gas crystal, which will be an important ingredient of an improved electron electric dipole moment measurement u…
We show the existence of ultra-long-range giant dipole molecules formed by a neutral alkali ground state atom that is bound to the decentered electronic wave function of a giant dipole atom. The adiabatic potential surfaces emerging from the interaction of the ground state atom with the giant dipole electron posses a rich topology depending on the degree of electronic excitation. Binding energies and the vibrational motion in the energetically lowest surfaces are analyzed by means of perturbation theory and exact diagonalization techniques. The resulting molecules are truly giant with internuc…
We calculate an effective electric field on the unpaired electron in the YbF molecule. This field determines sensitivity of the molecular experiment to the electric dipole moment of the electron. We use experimental value of the spin-doubling constant to estimate the admixture of the configuration with the hole in the 4f-shell of Ytterbium to the ground state of the molecule. This admixture reduces the field by 7%. Our value for the effictive field is 5.1 a.u. = 2.5 10^{10} V/cm.
We report calculations of Born-Oppenheimer potential energy curves of the chromium-rubidium heteronuclear molecule 52Cr-87Rb, and the long-range dispersion coefficient for the interaction between ground state Cr and Rb atoms. Our calculated van der Waals coefficient (C6=1770 a.u.) has an expected error of 3%. The ground state 6Sigma+ molecule at its equilibrium separation has a permanent electric dipole moment of de (Re=3.34 A) = 2.90 D. We investigate the hyperfine and dipolar collisions between trapped Cr and Rb atoms, finding elastic to inelastic cross section ratio of 100-1000.
We observe that when an ultracold ground state cesium (Cs) atom becomes bound within the electronic cloud of an extended Cs electronic orbit, ultralong-range molecules with giant (kilo-Debye) permanent electric dipole moments form. Large molecular permanent electric dipole moments are challenging to experimentally realize. Meeting this challenge has garnered significant interest because permanent electric dipole moments are important for understanding symmetry breaking in molecular physics, control of chemical reactions and realization of strongly correlated many-body quantum systems. These ne…
Permanent electric dipole moments (EDMs) of fundamental particles such as the electron are signatures of parity and time-reversal violation due to physics beyond the standard model. EDM measurements probe new physics at energy scales well beyond the reach of present-day colliders. Recent advances in assembling molecules from ultracold atoms have opened up new opportunities for improving the reach of EDM experiments. But better measurement techniques, that are not limited by the magnetic field sensitivity of such molecules, are necessary before these opportunities can be fully exploited. We pre…
We predict the existence of a class of ultracold giant molecules formed from trapped ultracold Rydberg atoms and polar molecules. The interaction which leads to the formation of such molecules is the anisotropic charge-dipole interaction ($a/R^2$). We show that prominent candidate molecules such as KRb and deuterated hydroxyl (OD) should bind to Rydberg rubidium atoms, with energies $E_b\simeq 5-25$ GHz at distances $R\simeq 0.1-1 \ μ$m. These molecules form in double wells, mimicking chiral molecules, with each well containing a particular dipole orientation. We prepare a set of correlated dr…
We demonstrate loading of SrF molecules into an optical dipole trap (ODT) via in-trap $Λ$-cooling. We find that this cooling can be optimized by a proper choice of relative ODT and $Λ$ beam polarizations. In this optimized configuration, we observe molecules with temperatures as low as 14(1) $μ$K in traps with depths up to 570 $μ$K. With optimized parameters, we transfer $\!\sim\!5$% of molecules from our radio-frequency magneto-optical trap into the ODT, at a density of $\sim\!2\times 10^{9}$ cm$^{-3}$, a phase space density of $\sim\!2\times 10^{-7}$, and with a trap lifetime of $\!\sim\!1$ …
Recent improvements in experimental techniques for preparing ultracold molecules that contain alkali atoms (e.g., Li, Na, and K) have been reported. Based on these advances in ultracold molecules, new searches for the electric dipole moment of the electron and the scalar-pseudoscalar interaction can be proposed on such systems. We calculate the effective electric fields (Eeff) and the S-PS coefficients (Ws) of SrA and HgA (A = Li, Na, and K) molecules at the Dirac-Fock (DF) and the relativistic coupled cluster (RCC) levels. We elaborate on the following points: i) Basis set dependence of the m…
In this article we extend the theory of ultra-long-range giant dipole molecules, formed by an atom in a giant dipole state and a ground-state alkali atom, by angular-momentum couplings known from recent works on Rydberg molecules. In addition to $s$-wave scattering, the next higher order of $p$-wave scattering in the Fermi-pseudopotential describing the binding mechanism is considered. Furthermore, the singlet and triplet channels of the scattering interaction as well as angular-momentum couplings such as hyperfine interaction and Zeeman interactions are included. Within the framework of Born-…
Heavy polar diatomic molecules are the primary tools for searching for the T-violating permanent electric dipole moment of the electron (eEDM). Valence electrons in some molecules experience extremely large effective electric fields due to relativistic interactions. These large effective electric fields are crucial to the success of polar-molecule-based eEDM search experiments. Here we report on the results of relativistic ab initio calculations of the effective electric fields in a series of molecules that are highly sensitive to an eEDM, the mercury monohalides (HgF, HgCl, HgBr,and HgI). We …
Collisions of polar $^{1}Σ$ state molecules at ultralow energies are considered, within a model that accounts for long-range dipole-dipole interactions, plus rotation of the molecules. We predict a substantial suppression of dipole-driven inelastic collisions at high values of the applied electric field, namely, field values of several times $B_e/μ$. Here $B_e$ is the rotational constant, and $μ$ is the electric dipole moment of molecules. The sudden large drop in the inelastic cross section is attributed to the onset of degeneracy between molecular rotational levels, which dramatically alters…
The electric dipole moment of the electron (eEDM) and the Scalar-PseudoScalar (S-PS) interaction are probes of new physics beyond the standard model of elementary particles, but experiments to observe them using atoms and molecules are still in progress. Molecules that have a large effective electric field (Eeff), S-PS coefficient (Ws), and permanent electric dipole moment (PDM) are in principle favorable candidates for such experiments, and hence, it is necessary to analyze these properties. In this work, we calculate Eeff, Ws, and PDM for Ra systems; RaF, RaX (X = Cl, Br, I, and At) and RaY …
Calculations of the BaF-Ar triatomic system are performed with a relativistic Hamiltonian and coupled cluster theory at the CCSD(T) level for 1386 positions of the Ar atom relative to the BaF molecule. Calculations are repeated with increasing basis sets (double-, triple-, quadruple- and quintuple-zeta), and these are extrapolated to estimate the complete-basis-set limit. The resulting energies provide a potential energy for the interaction of an Ar atom with a BaF molecule. A fit is presented that parametrizes this potential. This work is needed for an understanding of the position, modes of …
We explore one-dimensional (1-D) samples of ultracold polar molecules with attractive dipole-dipole interactions and show the existence of a repulsive barrier due to a strong quadrupole interaction between molecules. This barrier can stabilize a gas of ultracold KRb molecules and even lead to long-range wells supporting bound states between molecules. The properties of these wells can be controlled by external electric fields, allowing the formation of long polymer-like chains of KRb, and studies of quantum phase transitions by varying the effective interaction between molecules. We discuss th…
The rovibrational electric dipole transitions in the ground electronic state of the HD molecule are studied. A simple, yet rigorous formula is derived for the transition rates in terms of the electric dipole moment function $D(R)$, which is calculated in a wide range of $R$. Our numerical results for transition rates are in moderate agreement with experiments and previous calculations, but are at least an order of magnitude more accurate.
We analyze the electric dipole moments (PDMs) and static electric dipole polarizabilities of the alkali--alkaline-earth (Alk-AlkE) dimers by employing finite-field coupled-cluster methods, both in the frameworks of non-relativistic and four-component spinfree relativistic theory. In order to carry out comparative analyses rigorously, we consider those Alk-AlkE molecules made out of the lightest to the medium-heavy constituent atoms (Alk: Li to Rb and AlkE: Be through Sr). We present behaviour of electron correlation effects as well as relativistic effects with the size of the molecules. Uncert…
We show that the dipole-dipole interaction between two Rydberg atoms can give rise to long range molecules. The binding potential arises from two states that converge to different separated atom asymptotes. These states interact weakly at large distances, but start to repel each other strongly as the van der Waals interaction turns into a resonant dipole-dipole interaction with decreasing separation between the atoms. This mechanism leads to the formation of an attractive well for one of the potentials. If the two separated atom asymptotes come from the small Stark splitting of an atomic Rydbe…
The influence of evanescent waves on the nature of optical cooperative effects in atomic ensembles in a waveguide
Peter the Great St. Petersburg Polytechnic University（圣彼得堡彼得大帝理工大学）；Institute for Analytical Instrumentation of RAS（俄罗斯科学院分析仪器研究所）；Ioffe Institute（约费研究所）
A model for positron binding to polar molecules is considered by combining the dipole potential outside the molecule with a strongly repulsive core of a given radius. Using existing experimental data on binding energies leads to unphysically small core radii for all of the molecules studied. This suggests that electron-positron correlations neglected in the simple model play a large role in determining the binding energy. We account for these by including polarization potential via perturbation theory and non-perturbatively. The perturbative model makes reliable predictions of binding energies…
We review the current status of the study of parity and time invariance violation in atoms, nuclei and molecules. We focus on parity non-conservation in cesium and three of the most promising areas of research: (i) parity non-conservation in a chain of isotopes, (ii) search for nuclear anapole moments, and (iii) search for permanent electric dipole moments (EDMs) of atoms and molecules, which in turn are caused by either an electron EDM or nuclear $T,P$-odd moments such as a nuclear EDM or nuclear Schiff moment.
In a combined experimental and theoretical effort, we demonstrate a novel type of dipolar system made of ultracold bosonic dipolar molecules with large magnetic dipole moments. Our dipolar molecules are formed in weakly bound Feshbach molecular states from a sample of strongly magnetic bosonic erbium atoms. We show that the ultracold magnetic molecules can carry very large dipole moments and we demonstrate how to create and characterize them, and how to change their orientation. Finally, we confirm that the relaxation rates of molecules in a quasi-two dimensional geometry can be reduced by usi…
A new potential energy surface for the electronic ground state of the simplest triatomic anion H3- is determined for a large number of geometries. Its accuracy is improved at short and large distances compared to previous studies. The permanent dipole moment surface of the state is also computed for the first time. Nine vibrational levels of H3- and fourteen levels of D3- are obtained, bound by at most ~70 cm^{-1} and ~ 126 cm^{-1} respectively. These results should guide the spectroscopic search of the H3- ion in cold gases (below 100K) of molecular hydrogen in the presence of H3- ions.
Polyatomic polar molecules are promising systems for future experiments that search for violation of time-reversal and parity symmetries due to their advantageous electronic and vibrational structure, which allows laser cooling, full polarisation of the molecule, and reduction of systematic effects [I. Kozyryev and N.R. Hutzler, Phys, Rev. Lett. {\bf 119}, 133002 (2017)]. In this work we investigate the enhancement factor of the electric dipole moment of the electron ($E_\text{eff}$) in the triatomic monohydroxide molecules BaOH and YbOH within the high-accuracy relativistic coupled cluster me…
We propose a very sensitive method for measuring the electric dipole moment of the electron using polar molecules embedded in a cryogenic solid matrix of inert-gas atoms. The polar molecules can be oriented in the $\hat{\rm{z}}$ direction by an applied electric field, as has recently been demonstrated by Park, et al. [Angewandte Chemie {\bf 129}, 1066 (2017)]. The trapped molecules are prepared into a state which has its electron spin perpendicular to $\hat{\rm{z}}$, and a magnetic field along $\hat{\rm{z}}$ causes precession of this spin. An electron electric dipole moment $d_e$ would affect …
We predict that ultralong-range Rydberg bi-molecules form in collisions between polar molecules in cold and ultracold settings. The collision of $Λ$-doublet nitric oxide (NO) with long-lived Rydberg NO($nf$, $ng$) molecules forms ultralong-range Rydberg bi-molecules with GHz energies and kilo-Debye permanent electric dipole moments. The Hamiltonian includes both the anisotropic charge-molecular dipole interaction and the electron-NO scattering. The rotational constant for the Rydberg bi-molecules is in the MHz range, allowing for microwave spectroscopy of rotational transitions in Rydberg bi-m…
We review current status of the study of parity and time invariance phenomena in atoms, nuclei and molecules. We focus on three most promising areas of research: (i) parity non-conservation in a chain of isotopes, (ii) search for nuclear anapole moments, and (iii) search for permanent electric dipole moments (EDM) of atoms and molecules which are caused by either, electron EDM or nuclear $T,P$-odd moments such as nuclear EDM and nuclear Schiff moment.
We report results of ab initio calculation of the spin-rotational Hamiltonian parameters including P- and P,T-odd terms for the BaF molecule. The ground state wave function of BaF molecule is found with the help of the Relativistic Effective Core Potential method followed by the restoration of molecular four-component spinors in the core region of barium in the framework of a non-variational procedure. Core polarization effects are included with the help of the atomic Many Body Perturbation Theory for Barium atom. For the hyperfine constants the accuracy of this method is about 5-10%.
Understanding collisions between ultracold molecules is crucial for making stable molecular quantum gases and harnessing their rich internal degrees of freedom for quantum engineering. Transient complexes can strongly influence collisional physics, but in the ultracold regime, key aspects of their behavior have remained unknown. To explain experimentally observed loss of ground-state molecules from optical dipole traps, it was recently proposed that molecular complexes can be lost due to photo-excitation. By trapping molecules in a repulsive box potential using laser light near a narrow molecu…
We have calculated the atomic electric dipole moments (EDMs) induced in 229Pa and 225Ac by their respective nuclear Schiff moments S. The results are d(229Pa)= - 9.5 10^{-17} [S/(e fm)] e cm= - 1.1 10^{-20} ηe cm; d(225Ac})=- 8.6 10^{-17} [S/(e fm)] e cm=- 0.8 10^{-21} ηe cm. EDM of 229 Pa is 3 10^4 times larger than 199Hg EDM and 40 times larger than 225Ra EDM. Possible use of actinides in solid state experiments is also discussed. The T,P-odd spin-axis interaction in RaO molecule is 500 times larger than in TlF.
We study the two-body bound states of a model Hamiltonian that describes the interaction between two field-oriented dipole moments. This model has been used extensively in many-body physics of ultracold polar molecules and magnetic atoms, but its few-body physics has been explored less fully. With a hard-wall short-range boundary condition, the dipole-dipole bound states are universal and exhibit a complicated pattern of avoided crossings between states of different character. For more realistic Lennard-Jones short-range interactions, we consider parameters representative of magnetic atoms and…
Observation of resonant monopole-dipole energy transfer between Rydberg atoms and polar molecules
University College London（伦敦大学学院）；Department of Physics, Harvard University（哈佛大学物理系）；Instituto Carlos I de Física Teórica y Computacional, and Departamento de Física Atómica, Molecular y Nuclear, Universidad de Granada（格拉纳达大学理论计算物理卡洛斯一世研究所及原子、分子和核物理系）；Department of Physics and Astronomy, University College London（伦敦大学学院物理与天文系）
We create fermionic dipolar $^{23}$Na$^6$Li molecules in their triplet ground state from an ultracold mixture of $^{23}$Na and $^6$Li. Using magneto-association across a narrow Feshbach resonance followed by a two-photon STIRAP transfer to the triplet ground state, we produce $3\,{\times}\,10^4$ ground state molecules in a spin-polarized state. We observe a lifetime of $4.6\,\text{s}$ in an isolated molecular sample, approaching the $p$-wave universal rate limit. Electron spin resonance spectroscopy of the triplet state was used to determine the hyperfine structure of this previously unobserve…
We show that the electric dipole-dipole interaction between a pair of polar molecules undergoes an all-out transformation when superimposed by a far-off resonant optical field. The combined interaction potential becomes tunable by variation of wavelength, polarization and intensity of the optical field and its dependence on the intermolecular separation exhibits a crossover from an inverse-power to an oscillating behavior. The ability thereby offered to control molecular interactions opens up avenues toward the creation and manipulation of novel phases of ultracold polar gases among whose char…
We study a simple model consisting of an atomic ion and a polar molecule trapped in a single setup, taking into consideration their electrostatic interaction. We determine analytically their collective modes of excitation as a function of their masses, trapping frequencies, distance, and the molecule's electric dipole moment. We then discuss the application of these collective excitations to cool molecules, to entangle molecules and ions, and to realize two-qubit gates between them. We finally present a numerical analysis of the possibility of applying these tools to study magnetically ordered…
Nucleon Electric Dipole Moments in Paramagnetic Molecules through Effective Field Theory
Institute for Nuclear Theory, University of Washington（华盛顿大学核理论研究所）；Nikhef, Theory Group（尼赫夫理论组）；Departament de Física Quàntica i Astrofísica, Universitat de Barcelona（巴塞罗那大学量子物理与天体物理学系）；Institut de Ciències del Cosmos, Universitat de Barcelona（巴塞罗那宇宙科学研究所）；Van Swinderen Institute for Particle Physics and Gravity, University of Groningen（格罗宁根大学范斯温德恩粒子物理与引力研究所）；Department of Physics and Astronomy, University of North Carolina（北卡罗来纳大学物理与天文系）
Half-cycle laser pulse is applied on an absorbed molecule to investigate its alignment and orientation behavior. Crossover from field-free to hindered rotation motion is observed by varying the angel of hindrance of potential well. At small hindered angle, both alignment and orientation show sinusoidal-like behavior because of the suppression of higher excited states. However, mean alignment decreases monotonically as the hindered angle is increased, while mean orientation displays a minimum point at certain hindered angle. The reason is attributed to the symmetry of wavefunction and can be ex…
We first give a short review of the ``local-current approximation'' (LCA), derived from a general variation principle, which serves as a semiclassical description of strongly collective excitations in finite fermion systems starting from their quantum-mechanical mean-field ground state. We illustrate it for the example of coupled translational and compressional dipole excitations in metal clusters. We then discuss collective electronic dipole excitations in C$_{60}$ molecules (Buckminster fullerenes). We show that the coupling of the pure translational mode (``surface plasmon'') with compressi…
Heteronuclear dimers are of significant interest to experiments seeking to exploit ultracold polar molecules in a number of novel ways including precision measurement, quantum computing, and quantum simulation. We calculate highly accurate Born-Oppenheimer total energies and electric dipole moments as a function of internuclear separation for two such dimers, LiSr and KRb. We apply fully-correlated, high-accuracy quantum Monte Carlo methods for evaluating these molecular properties in a many-body framework. We use small-core effective potentials combined with multi-reference Slater-Jastrow tri…
