Manipulation of Molecules with Electromagnetic Fields
Mikhail Lemeshko, Roman V. Krems, John M. Doyle, Sabre Kais
备注：
853 references, 39 pages. Review article for the special issue "Manipulation of Molecules with Electromagnetic Fields", edited by M. Lemeshko, R. Krems, J. Doyle, and S. Kais. A few minor corrections are made compared to the journal version
The goal of the present article is to review the major developments that have led to the current understanding of molecule-field interactions and experimental methods for manipulating molecules with electromagnetic fields. Molecule-field interactions are at the core of several, seemingly distinct, areas of molecular physics. This is reflected in the organization of this article, which includes sections on Field control of molecular beams, External field traps for cold molecules, Control of molecular orientation and molecular alignment, Manipulation of molecules by non-conservative forces, Ultracold molecules and ultracold chemistry, Controlled many-body phenomena, Entanglement of molecules and dipole arrays, and Stability of molecular systems in high-frequency super-intense laser fields. The article contains 853 references.
We experimentally observe the action of multiple light pulses on the transverse motion of a continuous beam of fullerenes. The light potential is generated by non-resonant ultra-short laser pulses in perpendicular spatial overlap with the molecule beam. We observe a small but clear enhancement of the number of molecules in the center fraction of the molecular beam. Relatively low light intensity and short laser pulse duration prevent the molecule from fragmentation and ionization. Experimental results are confirmed by Monte Carlo trajectory simulations.
This paper is a chapter from an upcoming book on cold molecule physics. In it we describe techniques for the preparation and manipulation of cold molecules. We further describe techniques for applying said cold molecules to tests of fundamental physics.
We report bunching, slowing, and acceleration of a supersonically cooled beam of diatomic hydroxyl radicals (OH). \textit{In situ} observation of laser-induced fluorescence along the beam propagation path allows for detailed characterization of longitudinal phase-space manipulation of OH molecules through the Stark effect by precisely sequenced inhomogeneous electric fields.
The use of tapered optical fibers, i.e., optical nanofibers, for spectroscopy and the detection of small numbers of particles, such as neutral atoms or molecules, has been gaining ground in recent years. In this review, we briefly introduce the optical nanofiber, its fabrication and optical mode propagation within. We discuss recent progress on the integration of optical nanofibers into laser-cooled atom and vapor systems, paying particular attention to spectroscopy, cold atom cloud characterization and optical trapping schemes. Next, a natural extension on this work to molecules will be intro…
The atom-to-molecule conversion by the technique of optical Feshbach resonance in a magnetic lattice is studied in the mean-field approximation. For the case of shallow lattice, we give the dependence of the atom-to-molecule conversion efficiency on the tunnelling strength and the atomic interaction by taking a double-well as an example. We find that one can obtain a high atom-to-molecule conversion by tuning the tunnelling and interaction strengths of the system. For the case of deep lattice, we show that the existence of lattice can improve the atom-to-molecule conversion for certain initial…
We propose a method for sensitive parallel detection of low-frequency electromagnetic fields based on the fine structure interactions in paramagnetic polar molecules. Compared to the recently implemented scheme employing ultracold $^{87}$Rb atoms [B{ö}hi \textit{et al.}, Appl. Phys. Lett. \textbf{97}, 051101 (2010)], the technique based on molecules offers a 100-fold higher sensitivity, the possibility to measure both the electric and magnetic field components, and a probe of a wide range of frequencies from the dc limit to the THz regime.
In this paper, we present an electrode geometry for the manipulation of ultracold rovibrational ground state NaK molecules. The electrode system allows to induce a dipole moment in trapped diatomic NaK molecules with a magnitude up to $68 \%$ of their internal dipole moment along any direction in a given two-dimensional plane. The strength, the sign and the direction of the induced dipole moment is therefore fully tunable. Furthermore, the possibility to create strong electric field gradients provides the opportunity to address molecules in single layers of an optical lattice. The maximal rela…
Ultracold molecules have experienced increasing attention in recent years. Compared to ultracold atoms, they possess several unique properties that make them perfect candidates for the implementation of new quantum-technological applications in several fields, from quantum simulation to quantum sensing and metrology. In particular, ultracold molecules of two-electron atoms (such as strontium or ytterbium) also inherit the peculiar properties of these atomic species, above all the possibility to access metastable electronic states via direct excitation on optical clock transitions with ultimate…
Doubly dipolar molecules exhibit complex internal spin-dynamics when electric and magnetic fields are both applied. Near magnetic trap minima, these spin-dynamics lead to enhancements in Majorana spin-flip transitions by many orders of magnitude relative to atoms, and are thus an important obstacle for progress in molecule trapping and cooling. We conclusively demonstrate and address this with OH molecules in a trap geometry where spin-flip losses can be tuned from over $200 \text{ s}^{-1} $ to below our $2\text{ s}^{-1}$ vacuum limited loss rate with only a simple external bias coil and with …
We explore the spatial enantioseparation of gaseous chiral molecules for the cyclic three-level systems coupled with three electromagnetic fields. Due to molecular rotations, the specific requirements of the polarization directions of the three electromagnetic fields lead to the space-dependent part of the overall phase of the coupling strengths. Thus, the overall phase of the coupling strengths, which differs with $π$ for the enantiomers in the cyclic three-level model of chiral molecules, varies intensely in the length scale of the typical wavelength of the applied electromagnetic fields. Un…
The extraordinary success in laser cooling, trapping, and coherent manipulation of atoms has energized the efforts in extending this exquisite control to molecules. Not only are molecules ubiquitous in nature, but the control of their quantum states offers unparalleled access to fundamental constants and possible physics beyond the Standard Model. Quantum state manipulation of molecules can enable high-precision measurements including tests of fundamental symmetries and searches for new particles and fields. At the same time, their complex internal structure presents experimental challenges to…
We calculate the rate of the spontaneous magnetic dipole radiation transitions from ortho- to para-states of the hydrogen molecule at the room temperature with the radiation wavelengths about 0.01 - 0.1 cm. Exponentially small differences between the rotational energies and heat capacities of parahydrogen and orthohydrogen molecules and also diatomic molecules consisting of different hydrogen atoms for high temperatures are derived.
We explore coherent multi-photon processes in $^{87}$Rb$^{133}$Cs molecules using 3-level lambda and ladder configurations of rotational and hyperfine states, and discuss their relevance to future applications in quantum computation and quantum simulation. In the lambda configuration, we demonstrate the driving of population between two hyperfine levels of the rotational ground state via a two-photon Raman transition. Such pairs of states may be used in the future as a quantum memory, and we measure a Ramsey coherence time for a superposition of these states of 58(9) ms. In the ladder configur…
Laser cooling and trapping of atoms and atomic ions has led to numerous advances including the observation of exotic phases of matter, development of exquisite sensors and state-of-the-art atomic clocks. The same level of control in molecules could also lead to profound developments such as controlled chemical reactions and sensitive probes of fundamental theories, but the vibrational and rotational degrees of freedom in molecules pose a formidable challenge for controlling their quantum mechanical states. Here, we use quantum-logic spectroscopy (QLS) for preparation and nondestructive detecti…
We theoretically study non-destructive detection of ultracold molecules, using a Fabry-Perot cavity. Specifically, we consider vacuum Rabi splitting where we demonstrate the use of collective strong coupling for detection of molecules with many participating energy levels. We also consider electromagnetically induced transparency and transient response of light for the molecules interacting with a Fabry-Perot cavity mode, as a mean for non-destructive detection. We identify the parameters that are required for the detection of molecules in the cavity electromagnetically induced transparency co…
The coherent control of light with matter, enabling storage and manipulation of optical signals, was revolutionized by electromagnetically induced transparency (EIT), which is a quantum interference effect. For strong electromagnetic fields that induce a wide transparency band, this quantum interference vanishes, giving rise to the well-known phenomenon of Autler-Townes splitting (ATS). To date, it is an open question whether ATS can be directly leveraged for coherent control as more than just a case of "bad" EIT. Here, we establish a protocol showing that dynamically controlled absorption of …
Exploration of a new ultrafast-ultrasmall frontier in atomic and molecular physics has begun. Not only is is possible to control outer-shell electron dynamics with intense ultrafast optical lasers, but now control of inner-shell processes has become possible by combining intense infrared/optical lasers with tunable sources of x-ray radiation. This marriage of strong-field laser and x-ray physics has led to the discovery of methods to control reversibly resonant x-ray absorption in atoms and molecules on ultrafast timescales. Using a strong optical dressing field, resonant x-ray absorption in a…
Ultracold polar molecules are an ideal platform for studying many-body physics with long-range dipolar interactions. Experiments in this field have progressed enormously, and several groups are pursuing advanced apparatus for manipulation of molecules with electric fields as well as single-atom-resolved in situ detection. Such detection has become ubiquitous for atoms in optical lattices and tweezer arrays, but has yet to be demonstrated for ultracold polar molecules. Here we present a proposal for the implementation of quantum gas microscopy for polar molecules, and specifically discuss a tec…
We present a theory for rigorous quantum scattering calculations of probabilities for chemical reactions of atoms with diatomic molecules in the presence of an external electric field. The approach is based on the fully uncoupled basis set representation of the total wave function in the space-fixed coordinate frame, the Fock-Delves hyperspherical coordinates and adiabatic partitioning of the total Hamiltonian of the reactive system. The adiabatic channel wave functions are expanded in basis sets of hyperangular functions corresponding to different reaction arrangements and the interactions wi…
Photoassociation (PA) is a powerful technique to synthesize molecules directly and continuously from cold and ultracold atoms into deeply bound molecular states. In freespace, however, PA efficiency is constrained by the number of spontaneous decay channels linking the initial excited molecular state to a sea of final (meta)stable rovibronic levels. Here, we propose a novel scheme based on molecules strongly coupled to a guided photonic mode in a photonic crystal waveguide that turns PA into a powerful tool for near deterministic formation of ultracold molecules in their ground rovibrational l…
Ultracold collisions of cold atoms or molecules make the bound states of the collision complex formed from the two colliding species accessible for control and manipulation of the cold species or the complex. Such resonances are best treated by a resonant scattering theory, which in the ultracold domain can take advantage of the properties of the long-range potential and the methods of multichannel quantum defect theory. Coupled channels calculations on the threshold scattering states and bound states of the 40K87Rb molecule illustrate the ideas and methodology of quantum defect theory using t…
We demonstrate the measurement and manipulation of the temperature of cold CO molecules in a microchip environment. Through the use of time-resolved spatial imaging, we are able to observe the phase-space distribution of the molecules, and hence deduce the corresponding temperature. We do this both by observing the expansion of the molecular ensemble in time and through the use of numerical trajectory simulations. Furthermore, we demonstrate the adiabatic cooling of the trapped molecular sample and discuss this process.
We show that the excitation of long-range Rydberg molecules in a three-dimensional optical lattice can be used as a position- and time-sensitive probe of the site occupancy in the system. To this end, we detect the ions which are continuously generated by the decay of the formed Rydberg molecules. While a superfluid gas shows molecule formation for all parameters, a Mott insulator with $n=1$ filling reveals a strong suppression of the number of formed molecules. In the limit of weak probing, the technique can be used to probe the superfluid to Mott-insulator transition in real-time. Our method…
