We have demonstrated the resonant control of the elastic scattering cross sections in the vicinity of Feshbach resonances between $^{23}$Na$^{40}$K molecules and $^{40}$K atoms by studying the thermalization between them. The elastic scattering cross sections vary by more than two orders of magnitude close to the resonance, and can be well described by an asymmetric Fano profile. The parameters that characterize the magnetically tunable s-wave scattering length are determined from the elastic scattering cross sections. The observation of resonantly controlled elastic scattering cross sections opens up the possibility to study strongly interacting atom-molecule mixtures and improve our understanding of the complex atom-molecule Feshbach resonances.
We report the observation of a dimer-dimer inelastic collision resonance for ultracold Feshbach molecules made of bosonic sodium and rubidium atoms. This resonance, which we attribute to the crossing of the dimer-dimer threshold with a heteronuclear tetramer state, manifests itself as a pronounced inelastic loss peak of dimers when the interspecies scattering length between the constituent atoms is tuned. Near this resonance, a strong modification of the temperature dependence of the dimer-dimer scattering is observed. Our result provides insight into the heteronuclear four-body system consist…
Stimulated Raman adiabatic passage (STIRAP) allows to efficiently transferring the populations between two discrete quantum states and has been used to prepare molecules in their rovibrational ground state. In realistic molecules, a well-resolved intermediate state is usually selected to implement the resonant STIRAP. Due to the complex molecular level structures, the detuned STIRAP always coexists with the resonant STIRAP and may cause unexpected interference phenomenon. However, it is generally accepted that the detuned STIRAP can be neglected if compared with the resonant STIRAP. Here we re…
We report on a novel method for photo-association of strongly polar trilobite Rydberg molecules. This exotic ultralong-range dimer, consisting of a ground-state atom bound to the Rydberg electron via electron-neutral scattering, inherits its polar character from the admixture of high angular momentum electronic orbitals. The absence of low-$L$ character hinders standard photo-association techniques. Here, we show that for suitable principal quantum numbers resonant coupling of the orbital motion with the nuclear spin of the perturber, mediated by electron-neutral scattering, hybridizes the tri…
General formulas describing the multiple scattering of electron by polyatomic molecules have been derived within the framework of the model of non-overlapping atomic potentials. These formulas are applied to different carbon molecules, both for fixed-in-space and randomly oriented molecules.
We demonstrate microwave dressing on ultracold, fermionic ${}^{23}$Na${}^{40}$K ground-state molecules and observe resonant dipolar collisions with cross sections exceeding three times the $s$-wave unitarity limit. The origin of these collisions is the resonant alignment of the approaching molecules' dipoles along the intermolecular axis, which leads to strong attraction. We explain our observations with a conceptually simple two-state picture based on the Condon approximation. Furthermore, we perform coupled-channels calculations that agree well with the experimentally observed collision rate…
We study the resonant control of two nonreactive polar molecules in an optical lattice site, focussing on the example of RbCs. Collisional control can be achieved by tuning bound states of the intermolecular dipolar potential, by varying the applied electric field or trap frequency. We consider a wide range of electric fields and trapping geometries, showing that a three-dimensional optical lattice allows for significantly wider avoided crossings than free space or quasi-two dimensional geometries. Furthermore, we find that dipolar confinement induced resonances can be created with reasonable …
We measure the resonant forward scattering of light by a highly saturated atomic medium through the flashes emitted immediately after an abrupt extinction of the probe beam. The experiment is done in a dilute regime where the phenomena are well captured using the independent scattering approximation. Comparing our measurements to a model based on Maxwell-Bloch equations, our experimental results are consistent with contributions from only the elastic component, whereas the attenuation of the coherent transmission power is linked to the elastic and inelastic scatterings. In the large saturation…
We show that dressing polar molecules with a far-off-resonant optical field leads to new types of intermolecular potentials, which undergo a crossover from the inverse-power to oscillating behavior depending on the intermolecular distance, and whose parameters can be tuned by varying the laser intensity and wavelength. We present analytic expressions for the potential energy surfaces, thereby providing direct access to the parameters of an optical field required to design intermolecular interactions experimentally.
Magnetically tunable Feshbach resonances for polar paramagnetic ground-state diatomics are too narrow to allow for magnetoassociation starting from trapped, ultracold atoms. We show that non-resonant light can be used to engineer the Feshbach resonances in their position and width. For non-resonant field strengths of the order of $10^9\,$W/cm$^2$, we find the width to be increased by three orders of magnitude, reaching a few Gauss. This opens the way for producing ultracold molecules with sizeable electric and magnetic dipole moments and thus for many-body quantum simulations with such particl…
We report on a resonantly coupled 2(1) - 4 (1) photoassociation resonance in LiRb. This pair of states displays interesting decay physics that hint at interference-like effects caused by two different decay paths. We observe decay to predominantly $X \ ^1Σ^+ \ v=43$, with significant numbers of molecules produced in $X \ ^1Σ^+ \ v=2$ - 12. This photoassociation resonance also produces $\sim$300 $X \ ^1Σ^+ \ v=0 \ J=0$ molecules/second. Finally, we identify a stimulated Raman adiabatic passage transfer pathway from $v=43$ to $v=0$ that has the potential to produce up to $2 \times 10^5$ LiRb mol…
The polarization properties of the elastic electron scattering on H-like ions are investigated within the framework of the relativistic QED theory. The polarization properties are determined by a combination of relativistic effects and spin exchange between the incident and bound electrons. The scattering of a polarized electron on an initially unpolarized ion is fully described by five parameters. We study these parameters for non-resonant scattering, as well as in the vicinity of LL resonances, where scattering occurs through the formation and subsequent decay of intermediate autoionizing st…
Full control of molecular interactions, including reactive losses, would open new frontiers in quantum science. Here, we demonstrate extreme tunability of chemical reaction rates by using an external electric field to shift excited collision channels of ultracold molecules into degeneracy with the initial collision channel. In this situation, resonant dipolar interactions mix the channels at long range, dramatically altering the intermolecular potential. We prepare fermionic potassium-rubidium (KRb) molecules in their first excited rotational state and observe a three orders-of-magnitude modul…
This paper theoretically treats the spontaneous resonant inelastic scattering of Laguerre-Gauss (LG) beams from the totally symmetric vibrations of complex polyatomic molecules within the semi-classical framework. We develop an interaction Hamiltonian that accounts for the position of the molecule within the excitation beam to derive the effective differential scattering cross-section of a classical LG beam from a molecule using the frequency domain third order nonlinear optical response function. To gain physical insight into this scattering process, we utilize a model vibronic molecule to st…
We show that the probability of the collision-induced absorption of non-resonant microwave photons by a gas of ultracold molecules is dramatically enhanced near a Feshbach scattering resonance. This can be used for detecting Feshbach resonances of ultracold molecules by measuring the microwave field absorption and for tuning the elastic scattering cross sections of ultracold molecules by varying the frequency and intensity of the microwave field in a wide range of the field parameters.
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.
The 1:1:2 resonant elastic pendulum is a simple classical system that displays the phenomenon known as Hamiltonian monodromy. With suitable initial conditions, the system oscillates between nearly pure springing and nearly pure elliptical-swinging motions, with sequential major axes displaying a stepwise precession. The physical consequence of monodromy is that this stepwise precession is given by a smooth but multivalued function of the constants of motion. We experimentally explore this multivalued behavior. To our knowledge, this is the first experimental demonstration of classical monodrom…
The coherent radiation spectrum of two-level polar molecules with UV transition is studied at the multiphoton resonant excitation by a moderately strong laser field. The spectrum corresponding to harmonic generation and low-frequency radiation is investigated both analytically and numerically. Specifically, a mechanism for generation of intense smoothly tunable terahertz radiation by two-level molecular configurations (with dynamic Stark shifts) possessing permanent dipole moments, is considered.
We experimentally show that the N-H bond cleavage in pyrrole molecule following resonant electron attachment is allowed and controlled by the motion of the atoms which are not dissociating, namely of the carbon-attached hydrogen atoms. In order to interpret these findings, we have developed a method for locating all resonant and virtual states of an electron-molecule system in the complex plane, based on all-electron R-matrix scattering calculations. Mapping these as a function of molecular geometry allows us to separate two contributing dissociation mechanisms: a $π^*$ resonance formation ind…
We perform a comprehensive investigation of Förster resonant energy transfer in a room-temperature thermal mixture of ammonia molecules and rubidium Rydberg atoms. Fully state-resolved measurement of the Rydberg-atom populations is achieved by combining millimeter-wave state transfer with state-selective field ionization. This allows aspects of the energy transfer process such as state dependence, ammonia pressure dependence, and dependence on the energy resonance condition to be investigated in detail. Our results pave the way for future quantum experiments combining polar molecules and Rydbe…
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 calculate the cross sections for elastic scattering and Zeeman relaxation in binary collisions of molecules in the ro-vibrational ground state of a $^2Σ$ electronic state and the Zeeman state with the electron spin projection $M_S=1/2$ on the magnetic field axis. This is the lowest-energy state of $^2Σ$ molecules confined in a magnetic trap. The results are averaged over calculations with multiple molecule - molecule interaction potentials, which yields the expectation intervals for the cross sections and the elastic-to-inelastic cross section ratios. We find that the elastic-to-inelastic c…
We theoretically study collisions between ultracold polar molecules that are polarized by microwave or static electric fields. We systematically study the dependence on field strength, microwave polarization, and detuning from rotational transitions. We calculate the loss in two-body collisions that is observable experimentally and compare to the results expected for purely first-order dipolar interactions. For ground state molecules polarized by a static electric field, the dynamics are accurately described by first-order dipolar interactions. For microwave dressing, instead, resonant dipolar…
A magnetic field dependent Feshbach resonance has been observed in the elastic scattering collision rate between atoms in the F = 2, M = -2 state of 85 Rb. Changing the magnetic field by several Gauss caused the collision rate to vary by a factor of 10,000, and the sign of the scattering length could be reserved. The resonance peak is at 155.2(4) G and its width is 11.6(5) G. From these results we extract much improved values for the three quantities that characterize the interaction porential: the van der Waals coefficient C6, the singlet scattering length, and the triplet scattering length.
We present a theoretical study of the rotational dynamics of asymmetry top molecules in an electric field and a parallel non-resonant linearly polarized laser pulse. The time-dependent Schrödinger equation is solved within the rigid rotor approximation. Using the benzonitrile molecule as prototype, we investigate the field-dressed dynamics for experimentally accessible field configurations and compare these results to the adiabatic predictions. We show that for an asymmetric top molecule in parallel fields, the formation of the pendular doublets and the avoided crossings between neighboring le…
We propose an experimentally realizable scheme to produce triatomic ultralong-range Rydberg molecules (TURM), formed in ultracold KRb traps. A near resonant coupling of the non-zero quantum defect Rydberg levels with the KRb molecule in N=0 and N=2 rotational levels, is engineered which exploits the unique Rydberg electron-molecule anisotropic dipole interaction. This near resonant coupling enhances the TURM binding and produces favorable Franck-Condon factors. Schemes for both postassium and rubidium excitations are demonstrated.
We model the formation of stable heteronuclear molecules via pulsed Raman photoassociation of a two-component Bose-Einstein condensate near a strong Feshbach resonance, for both counterintuitive and intuitive pulse sequencing. Compared to lasers alone, weak Raman photoassociation is enhanced by as much as a factor of ten (five) for a counterintuitive (intuitive) pulse sequence, whereas strong Raman photoassociation is barely enhanced at all--regardless of pulse sequence. Stronger intra-atom, molecule, or atom-molecule collisions lead to an expected decrease in conversion efficiency, but strong…
We have studied the effect of resonant electronic state coupling on the formation of ultracold ground-state $^{85}$Rb$_2$. Ultracold Rb$_2$ molecules are formed by photoassociation (PA) to a coupled pair of $0_u^+$ states, $0_u^+(P_{1/2})$ and $0_u^+(P_{3/2})$, in the region below the $5S+5P_{1/2}$ limit. Subsequent radiative decay produces high vibrational levels of the ground state, $X ^1Σ_g^+$. The population distribution of these $X$ state vibrational levels is monitored by resonance-enhanced two-photon ionization through the $2 ^1Σ_u^+$ state. We find that the populations of vibrational l…
Using the ground potential energy surface[M. Ayouz \textit{et\, al}. J. Chem Phys \textbf{132} 194309 (2010)] of the H$_3^-$ molecule, we have determined the energies and widths of the complex resonant levels of H$_3^-$ located up to 4000 cm$^{-1}$ above the dissociation limit H$^-$+H$_2(v_d=0,j_d=0)$. Bound and resonant levels of the H$_2$D$^-$ and D$_2$H$^-$ isotopologues have been also characterized within the same energy range. The method combines the hyperspherical adiabatic approach, slow variable discretization method, and complex absorbing potential. These results represent the first s…
Dramatically sharp resonances manifesting stable negative-ion formation characterize Regge pole-calculated low-energy electron elastic total cross sections (TCSs) of heavy multi-electron systems. The novelty of the Regge pole analysis is in the extraction of rigorous and unambiguous negative-ion binding energies (BEs), corresponding to the measured electron affinities (EAs) of the investigated multi-electron systems. The measured EAs have engendered the crucial question: is the EA of multi-electron atoms and fullerene molecules identified with the BE of the attached electron in the ground, met…
We formulate the theory for a diatomic molecule in a spatially degenerate electronic state interacting with a non-resonant laser field and investigate its rovibrational structure in the presence of the field. We report on \textit{ab initio} calculations employing the double electron attachment intermediate Hamiltonian Fock space coupled cluster method restricted to single and double excitations for all electronic states of the Rb$_2$ molecule up to $5s+5d$ dissociation limit of about 26.000$\,$cm$^{-1}$. In order to correctly predict the spectroscopic behavior of Rb$_2$, we have also calculate…
Promising pathways for photoassociative formation of ultracold heteronuclear alkali metal dimers in their lowest rovibronic levels (denoted X(0,0)) are examined using high quality ab initio calculations of potential energy curves currently available. A promising pathway for KRb, involving the resonant coupling of the $2 ^1Π$ and $1 ^1Π$ states just below the lowest excited asymptote (K($4s$)+Rb($5p_{1/2}$)), is found to occur also for RbCs and less promisingly for KCs as well. The resonant coupling of the $3 ^1 Σ^+ $ and $1 ^1Π$ states, also just below the lowest excited asymptote, is found to…
The dominant mechanism of low-energy positron annihilation in polyatomic molecules is through positron capture in vibrational Feshbach resonances (VFR). In this paper we investigate theoretically the effect of anharmonic terms in the vibrational Hamiltonian on the positron annihilation rates. Such interactions enable positron capture in VFRs associated with multiquantum vibrational excitations, leading to enhanced annihilation. Mode coupling can also lead to faster depopulation of VFRs, thereby reducing their contribution to the annihlation rates. To analyze this complex picture, we use couple…
The elastic scattering of twisted electrons by diatomic molecules is studied within the framework of the non-relativistic first Born approximation. In this process, the coherent interaction of incident electrons with two molecular centers may cause interference patterns in the angular distributions of outgoing particles. We investigate how this Young-type interference is influenced by the complex internal structure of twisted beams. In particular, we show that the corkscrew-like phase front and the inhomogeneous intensity profile of the incident beam can strongly modify the angular distributio…
The non-resonant formation of $ddμ$ molecules in the loosely bound state in collisions of non-thermalized $dμ$ atoms with deuterium molecules D$_2$ has been considered. The process of such a type is possible only for collision energies exceeded the ionization potential of D$_2$. The calculated rates of $ddμ$ formation in the above-threshold energy region are about one order of magnitude higher than obtained earlier. The role of epithermal non-resonant $μ$-molecule formation for the kinetics of $μ$CF processes in D$_2$ gas was studied. It was shown that the non-resonant $ddμ$ formation by $dμ$ …
State-by-state cross sections for dissociative electron attachment and electron-impact dissociation for molecular oxygen are computed using ab initio resonance curves calculated with the R-matrix method. When O2 is in its vibrational ground state, the main contribution for both processes comes from the $^2Π_u$ resonance state of $O_2^-$ but with a significant contribution from the $^4Σ$ resonant state. Vibrational excitation leads to an increased contribution from the low-lying $^2Π_{g}$ resonance, greatly increased cross sections for both processes, and the threshold moving to lower energies.…
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…
This article presents an overview of current understanding of the interaction of low-energy positrons with molecules with emphasis on resonances, positron attachment and annihilation. Annihilation rates measured as a function of positron energy reveal the presence of vibrational Feshbach resonances (VFR) for many polyatomic molecules. These resonances lead to strong enhancement of the annihilation rates. They also provide evidence that positrons bind to many molecular species. A quantitative theory of VFR-mediated attachment to small molecules is presented. It is tested successfully for select…
The spin-exchange effect in spin-polarized electron collisions with unpolarized open-shell molecules, O$_2$, B$_2$, S$_2$ and Si$_2$, has been studied by the R-matrix method with the fixed-bond approximation. All of these molecules have ${}^3 Σ_{g}^{-}$ symmetry in their ground states. Usual integrated cross sections with unpolarized electrons has also been studied. We used the complete active space self consistent field orbitals and put more than 10 target electronic states in the R-matrix models. In electron O$_2$ elastic collisions, calculated polarization fractions agree well with the expe…
In collisions at ultralow temperatures, molecules will possess Feshbach resonances, foreign to ultracold atoms, whose virtual excited states consist of rotations of the molecules. We estimate the mean spacing and mean widths of these resonant states, exploiting the fact the molecular collisions at low energy display chaotic motion. As examples, we consider the experimentally relevant molecules O_2, OH, and PbO. The density of s-wave resonant states for these species is quite high, implying that a large number of narrow resonant states will exist.
We consider harmonics generation and wave-mixing by two-color multi photon resonant excitation of three-level atoms/molecules in strong laser fields. The coherent part of the spectra corresponding to multicolor harmonics generation is investigated. The obtained analytical results on the basis of generalized rotating wave approximation are in a good agreement with numerical calculations. The results applied to the hydrogen atom and homonuclear diatomic molecular ion show that one can achieve efficient generation of moderately high multicolor harmonics via multiphoton resonant excitation by appr…
We propose a novel way to image dynamical properties of nonstationary electron systems using ultrafast resonant x-ray scattering. Employing a rigorous theoretical analysis within the framework of quantum electrodynamics, we demonstrate that a single scattering pattern from a nonstationary electron system encodes the instantaneous interatomic electron current in addition to the structural information usually obtained by resonant x-ray scattering from stationary systems. Thus, inelastic contributions that are indistinguishable from elastic processes induced by a broadband probe pulse, instead of…
We discuss laser dressed dipolar and Van der Waals interactions between atoms and polar molecules, so that a cold atomic gas with laser admixed Rydberg levels acts as a designed reservoir for both elastic and inelastic collisional processes. The elastic scattering channel is characterized by large elastic scattering cross sections and repulsive shields to protect from close encounter collisions. In addition, we discuss a dissipative (inelastic) collision where a spontaneously emitted photon carries away (kinetic) energy of the collision partners, thus providing a significant energy loss in a s…
Molecular ions can be held in a chain of laser-cooled atomic ions by sympathetic cooling. This system is ideal for performing high-precision molecular spectroscopy with applications in astrochemistry and fundamental physics. Here we show that this same system can be coupled with a broadband laser to discover new molecular transitions. We use three-ion chains of Ca$^{+}$ and CaH$^{+}$ to observe vibrational transitions via resonance enhanced multiphoton dissociation detected by Ca$^{+}$ fluorescence. Based on theoretical calculations, we assign the observed peaks to the transition from the grou…
Multichannel quantum defect theory (MQDT) has been widely applied to resonant and non-resonant scattering in a variety of atomic collision processes. In recent years, the method has been applied to cold collisions with considerable success, and it has proven to be a computationally viable alternative to full-close coupling (CC) calculations when spin, hyperfine and external field effects are included. In this paper, we describe a hybrid approach for molecule-molecule scattering that includes the simplicity of MQDT while treating the short-range interaction explicitly using CC calculations. Thi…
Resonant formation of $dμt$ molecules in collisions of muonic tritium ($μt$) on D$_2$ was investigated using a beam of $μt$ atoms, demonstrating a new direct approach in muon catalyzed fusion studies. Strong epithermal resonances in $dμt$ formation were directly revealed for the first time. From the time-of-flight analysis of $2036\pm 116$ $dt$ fusion events, a formation rate consistent with $0.73\pm (0.16)_{meas} \pm (0.09)_{model}$ times the theoretical prediction was obtained. For the largest peak at a resonance energy of $0.423 \pm 0.037$ eV, this corresponds to a rate of $(7.1 \pm 1.8) \t…
Photoassociation, assembling molecules from atoms using laser light, is limited by the low density of atom pairs at sufficiently short interatomic separations. Here, we show that non-resonant light with intensities of the order of 10^10 W/cm^2 modifies the thermal cloud of atoms, enhancing the Boltzmann weight of shape resonances and pushing scattering states below the dissociation limit. This leads to an enhancement of photoassociation rates by several orders of magnitude and opens the way to significantly larger numbers of ground state molecules in a thermal ensemble than achieved so far.
We propose a new class of bosonic dark matter (DM) detectors based on resonant absorption onto a gas of small polyatomic molecules. Bosonic DM acts on the molecules as a narrow-band perturbation, like an intense but weakly coupled laser. The excited molecules emit the absorbed energy into fluorescence photons that are picked up by sensitive photodetectors with low dark count rates. This setup is sensitive to any DM candidate that couples to electrons, photons, and nuclei, and may improve on current searches by several orders of magnitude in coupling for DM masses between 0.2 eV and 20 eV. This…
Bound states and collisions of atoms with two-channel two-body interactions in harmonic waveguides are analyzed. The closed-channel contributions to two-atom bound states become dominant in the case of a weak resonance. At low energies and values of the non-resonant scattering length the problem can be approximated by a one-dimensional resonant model. Three-body problem becomes nonintegrable and the properties of triatomic molecules become different from those predicted by the integrable Lieb-Liniger-McGuire model.
