Stark deceleration has been utilized for slowing and trapping several species of neutral, ground-state polar molecules generated in a supersonic beam expansion. Due to the finite physical dimension of the electrode array and practical limitations of the applicable electric fields, only molecules within a specific range of velocities and positions can be efficiently slowed and trapped. These constraints result in a restricted phase space acceptance of the decelerator in directions both transverse and parallel to the molecular beam axis; hence, careful modeling is required for understanding and achieving efficient Stark decelerator operation. We present work on slowing of the hydroxyl radical (OH) elucidating the physics controlling the evolution of the molecular phase space packets both with experimental results and model calculations. From these results we deduce experimental conditions necessary for efficient operation of a Stark decelerator.
We report the Stark deceleration of CaF molecules in the strong-field seeking ground state and in a weak-field seeking component of a rotationally-excited state. We use two types of decelerator, a conventional Stark decelerator for the weak-field seekers, and an alternating gradient decelerator for the strong-field seekers, and we compare their relative merits. We also consider the application of laser cooling to increase the phase-space density of decelerated molecules.
We produce SO_2 molecules with a centre of mass velocity near zero using a Stark decelerator. Since the initial kinetic energy of the supersonic SO_2 molecular beam is high, and the removed kinetic energy per stage is small, 326 deceleration stages are necessary to bring SO_2 to a complete standstill, significantly more than in other experiments. We show that in such a decelerator possible loss due to coupling between the motional degrees of freedom must be considered. Experimental results are compared with 3D Monte-Carlo simulations and the quantum state selectivity of the Stark decelerator i…
We describe the production of cold, slow-moving LiH molecules. The molecules are produced in the ground state using laser ablation and supersonic expansion, and 68% of the population is transferred to the rotationally excited state using narrowband radiation at the rotational frequency of 444GHz. The molecules are then decelerated from 420m/s to 53m/s using a 100 stage Stark decelerator. We demonstrate and compare two different deceleration modes, one where every stage is used for deceleration, and another where every third stage decelerates and the intervening stages are used to focus the mol…
Controlling rovibrational state populations of polar molecules in inhomogeneous electric fields of the Stark deceleration: molecular dynamics and quantum chemistry simulations
We demonstrate the deceleration of heavy polar molecules in low-field seeking states by combining a cryogenic source and a travelling-wave Stark decelerator. The cryogenic source provides a high intensity beam with low speed and temperature, and the travelling-wave decelerator provides large deceleration forces and high phase-space acceptance. We prove these techniques using YbF molecules and find the experimental data to be in excellent agreement with numerical simulations. These methods extend the scope of Stark deceleration to a very wide range of molecules.
The large electric dipole moments associated with highly excited Rydberg states of atoms and molecules make gas-phase samples in these states very well suited to deceleration and trapping using inhomogeneous electric fields. The methods of Rydberg-Stark deceleration with which this can be achieved are reviewed here. Using these techniques, the longitudinal motion of beams of atoms and molecules moving at speeds as high as 2500~m/s have been manipulated, with changes in kinetic energy of up to $|ΔE_{\mathrm{kin}}|=1.3\times10^{-20}$~J ($|ΔE_{\mathrm{kin}}|/e=80$~meV or $|ΔE_{\mathrm{kin}}|/hc=6…
We report on the deceleration of a beam of SrF molecules from 290 to 120~m/s. Following supersonic expansion, the molecules in the $X^2Σ$ ($v=0$, $N=1$) low-field seeking states are trapped by the moving potential wells of a traveling-wave Stark decelerator. With a deceleration strength of 9.6 km/s$^2$ we have demonstrated the removal of 85 % of the initial kinetic energy in a 4 meter long modular decelerator. The absolute amount of kinetic energy removed is a factor 1.5 higher compared to previous Stark deceleration experiments. The demonstrated decelerator provides a novel tool for the creat…
We propose a promising scheme to decelerate a cw filtering out molecular beam using a red-detuned quasi-cw semi-Gaussian laser beam. By using Monte-Carlo simulation method, we demonstrate this optical Stark deceleration scheme, and study its decelerated dynamic process for a cw ND3 molecular beam as well as the dependence of the deceleration effect on the border width of the semi-Gaussian beam. Our study shows that the proposed scheme can be used to efficiently slow a cw ND3 molecular beam, and obtain a relative average kinetic-energy loss of 9.33% by using a single semi-Gaussian beam with a w…
The Stark deceleration of OH radicals in both low-field-seeking and high-field-seeking levels of the rovibronic ${}^2Π_{3/2},v=0,J=3/2$ ground state is demonstrated using a single experimental setup. Applying alternating-gradient focusing, OH radicals in their low-field-seeking ${}^2Π_{3/2},v=0,J=3/2,f$ state have been decelerated from 345 m/s to 239 m/s, removing 50 % of the kinetic energy using only 27 deceleration stages. The alternating-gradient decelerator allows to independently control longitudinal and transverse manipulation of the molecules. Optimized high-voltage switching sequences …
Cold, velocity-controlled molecular beams consisting of a single quantum state promise to be a powerful tool for exploring molecular scattering interactions. In recent years, Stark deceleration has emerged as one of the main methods for producing velocity-controlled molecular beams. However, Stark deceleration is shown not to be effective at producing a molecular beam consisting of a single quantum state in many circumstances. Therefore, quantum state purity must be carefully considered when using Stark decelerated beams, particularly in collision experiments where contributions from all quant…
We have designed and implemented a new Stark decelerator based on wire electrodes, which is suitable for ultrahigh vacuum applications. The 100 deceleration stages are fashioned out of 0.6 mm diameter tantalum and the array's total length is 110 mm, approximately 10 times smaller than a conventional Stark decelerator with the same number of electrode pairs. Using the wire decelerator, we have removed more than 90% of the kinetic energy from metastable CO molecules in a beam.
We demonstrate feedback control optimization for the Stark deceleration and trapping of neutral polar molecules using evolutionary strategies. In a Stark-decelerator beamline pulsed electric fields are used to decelerate OH radicals and subsequently store them in an electrostatic trap. The efficiency of the deceleration and trapping process is determined by the exact timings of the applied electric field pulses. Automated optimization of these timings yields an increase of 40 % of the number of trapped OH radicals.
We report on the electrostatic trapping of neutral SrF molecules. The molecules are captured from a cryogenic buffer-gas beam source into the moving traps of a 4.5 m long traveling-wave Stark decelerator. The SrF molecules in $X^2Σ^+(v=0, N=1)$ state are brought to rest as the velocity of the moving traps is gradually reduced from 190 m/s to zero. The molecules are held for up to 50 ms in multiple electric traps of the decelerator. The trapped packets have a volume (FWHM) of 1 mm$^{3}$ and a velocity spread of 5(1) m/s which corresponds to a temperature of $60(20)$ mK. Our result demonstrates …
We report on the production of a pulsed molecular beam of metastable NH ($a ^1Δ$) radicals and present first results on the Stark deceleration of the NH ($a ^1Δ, J=2, MΩ=-4$) radicals from 550 m/s to 330 m/s. The decelerated molecules are excited on the spin-forbidden $A ^3Π\leftarrow a ^1Δ$ transition, and detected via their subsequent spontaneous fluorescence to the $X ^3Σ^{-}, v"=0$ ground-state. These experiments demonstrate the feasibility of our recently proposed scheme [Phys. Rev. A 64 (2001) 041401] to accumulate ground-state NH radicals in a magnetic trap.
We present an analysis of the deceleration and trapping of heavy diatomic molecules in low-field seeking states by a moving electric potential. This moving potential is created by a 'ring-decelerator', which consists of a series of ring-shaped electrodes to which oscillating high voltages are applied. Particle trajectory simulations have been used to analyze the deceleration and trapping efficiency for a group of molecules that is of special interest for precision measurements of fundamental discrete symmetries. For the typical case of the SrF molecule in the (N,M) = (2, 0) state, the ring-dec…
The transverse motion inside a Stark decelerator plays a large role in the total efficiency of deceleration. We differentiate between two separate regimes of molecule loss during the slowing process. The first mechanism involves distributed loss due to coupling of transverse and longitudinal motion, while the second is a result of the rapid decrease of the molecular velocity within the final few stages. In this work, we describe these effects and present means for overcoming them. Solutions based on modified switching time sequences with the existing decelerator geometry lead to a large gain o…
A microstructured array of 1254 electrodes on a substrate has been configured to generate an array of local minima of electric field strength with a periodicity of 120 $μ$m about 25 $μ$m above the substrate. By applying sinusoidally varying potentials to the electrodes, these minima can be made to move smoothly along the array. Polar molecules in low-field seeking quantum states can be trapped in these traveling potential wells. Recently, we experimentally demonstrated this by transporting metastable CO molecules at constant velocities above the substrate [Phys. Rev. Lett. 100 (2008) 153003]. …
Cryogenic buffer-gas beams are a promising method for producing bright sources of cold molecular radicals for cold collision and chemical reaction experiments. In order to use these beams in studies of reactions with controlled collision energies, or in trapping experiments, one needs a method of controlling the forward velocity of the beam. A Stark decelerator can be an effective tool for controlling the mean speed of molecules produced by supersonic jets, but efficient deceleration of buffer-gas beams presents new challenges due to longer pulse lengths. Traveling-wave decelerators are unique…
Beams of polar molecules can be focused using an array of electrostatic lenses in alternating gradient (AG) configuration. They can also be accelerated or decelerated by applying an appropriate high voltage switching sequence to the lenses. AG focusing is applicable to molecules in both low-field and high-field-seeking states and is particularly well suited to the problem of decelerating heavy molecules and those in their ground rotational state. We describe the principles of AG deceleration and set out criteria to be followed in decelerator design, construction and operation. We calculate the…
A pulsed beam of ground state OH radicals is slowed down using a Stark decelerator and is subsequently loaded into an electrostatic trap. Characterization of the molecular beam production, deceleration and trap loading process is performed via laser induced fluorescence detection inside the quadrupole trap. Depending on details of the trap loading sequence, typically $10^5$ OH ($X^2Π_{3/2}, J=3/2$) radicals are trapped at a density of around $10^7$ cm$^{-3}$ and at temperatures in the 50-500 mK range. The 1/e trap lifetime is around 1.0 second.
We study the dynamics of a supersonic molecular beam in a low-finesse optical cavity and demonstrate that most molecules in the beam can be decelerated to zero central velocity by the intracavity optical field in a process analogous to electrostatic Stark deceleration. We show that the rapid switching of the optical field for slowing the molecules is automatically generated by the cavity-induced dynamics. We further show that $\sim1\%$ of the molecules can be optically trapped at a few millikelvin in the same cavity.
We calculate the DC Stark effect for three molecular hydrogen ions in the non-relativistic approximation. The effect is calculated both in dependence on the rovibrational state and in dependence on the hyperfine state. We discuss special cases and approximations. We also calculate the AC polarisabilities for several rovibrational levels, and therefrom evaluate accurately the black-body radiation shift, including the effects of excited electronic states. The results enable the detailed evaluation of certain systematic shifts of the transitions frequencies for the purpose of ultra-high-precision…
In optical dipole traps, the excited rotational states of a molecule may experience a very different light shift than the ground state. For particles with two polarizability components (parallel and perpendicular), such as linear $^1Σ$ molecules, the differential shift can be nulled by choice of elliptical polarization. When one component of the polarization vector is $\pm i\sqrt{2}$ times the orthogonal component, the light shift for a sublevel of excited rotational states approaches that of the ground state at high optical intensity. In this case, fluctuating trap intensity need not limit co…
In a Stark decelerator, polar molecules are slowed down and focussed by an inhomogeneous electric field which switches between two configurations. For the decelerator to work, it is essential that the molecules follow the changing electric field adiabatically. When the decelerator switches from one configuration to the other, the electric field changes in magnitude and direction, and this can cause molecules to change state. In places where the field is weak, the rotation of the electric field vector during the switch may be too rapid for the molecules to maintain their orientation relative to…
We have focused and decelerated benzonitrile (C$_7$H$_5$N) molecules from a molecular beam, using an array of time-varying inhomogeneous electric fields in alternating gradient configuration. Benzonitrile is prototypical for large asymmetric top molecules that exhibit rich rotational structure and a high density of states. At the rotational temperature of 3.5 K in the pulsed molecular beam, many rotational states are populated. Benzonitrile molecules in their absolute ground state are decelerated from 320 m/s to 289 m/s, and similar changes in velocity are obtained for excited rotational state…
We present experiments on decelerating and trapping ammonia molecules using a combination of a Stark decelerator and a traveling wave decelerator. In the traveling wave decelerator a moving potential is created by a series of ring-shaped electrodes to which oscillating high voltages are applied. By lowering the frequency of the applied voltages, the molecules confined in the moving trap are decelerated and brought to a standstill. As the molecules are confined in a true 3D well, this new kind of deceleration has practically no losses, resulting in a great improvement on the usual Stark deceler…
In this paper we consider the feasibility of observing the gravitational quantum states of positronium. The proposed scheme employs the flow-throw technique used for the first observation of this effect with neutrons. Collimation and Stark deceleration of Rydberg positronium atoms allow to select the required velocity class. If this experiment could be realized with positronium it would lead to a determination of g for this matter-antimatter system at the few % level. As discussed in this contribution, most of the required techniques are currently available but important milestones have to be …
A new type of decelerator is presented where polar neutral molecules are guided and decelerated using the principle of traveling electric potential wells, such that molecules are confined in stable three-dimensional traps throughout. This new decelerator is superior to the best currently operational decelerator (Scharfenberg et al., Phys.Rev.A 79, 023410(2009)), providing a substantially larger acceptance even at higher accelerations. The mode of operation is described and experimentally demonstrated by guiding and decelerating CO molecules.
A Stark decelerator is an effective tool for controlling motional degrees of freedom of polar molecules. Due to technical limitations, many of the current Stark decelerators focus on molecules in low-field-seeking quantum states and are built based on a fixed electrode size and spacing (type-A architecture). Here, we present an alternative method based on a different architecture, so-called type-B, with microstructured electrodes and a simpler electric field pulse timing with the prospect of producing cold, quasi-CW molecular beams. We demonstrate with simulations the feasibility of this metho…
We investigate the effect of far-off-resonant trapping light on ultracold bosonic RbCs molecules. We use kHz-precision microwave spectroscopy to measure the differential AC Stark shifts between the ground and first excited rotational levels of the molecule with hyperfine-state resolution. We demonstrate through both experiment and theory that coupling between neighboring hyperfine states manifests in rich structure with many avoided crossings. This coupling may be tuned by rotating the polarization of the linearly polarized trapping light. A combination of spectroscopic and parametric heating …
Stark deceleration allows for precise control over the velocity of a pulsed molecular beam and, by the nature of its limited phase-space acceptance, reduces the energy width of the decelerated packet. We describe an alternate method of operating a Stark decelerator that further reduces the energy spread over the standard method of operation. In this alternate mode of operation, we aggressively decelerate the molecular packet using a high phase angle. This technique brings the molecular packet to the desired velocity before it reaches the end of the decelerator; the remaining stages are then us…
An exterior complex scaling technique is applied to compute Stark resonance parameters for two molecular orbitals ($1b_{1}$ and $1b_{2}$) represented in the field-free limit in a single-center expansion. For electric DC field configurations that guarantee azimuthal symmetry of the solution the calculation is carried out by solving a two-dimensional partial differential equation in spherical polar coordinates using a finite-element method. The resonance positions and widths as a function of electric field strengths are shown for field strengths starting in the tunnelling ionization regime, and …
We extend a model of two-center interference to include the superposition of opposite orientations in aligned polar molecules. We show that the position of the minimum in the harmonic spectrum from both aligned and oriented CO depends strongly on the relative recombination strength at different atoms, not just the relative phase. We reinterpret the minimum in aligned CO as an interference between opposite orientations, and obtain good agreement with numerical calculations. Inclusion of the first-order Stark effect shifts the position of the interference minimum in aligned CO even though aligne…
Beams of neutral polar molecules in a low-field seeking quantum state can be slowed down using a Stark decelerator, and can subsequently be loaded and confined in electrostatic quadrupole traps. The efficiency of the trap loading process is determined by the ability to couple the decelerated packet of molecules into the trap without loss of molecules and without heating. We discuss the inherent difficulties to obtain ideal trap loading, and describe and compare different trap loading strategies. A new "split-endcap" quadrupole trap design is presented that enables improved trap loading efficie…
A method for decelerating a continuous beam of neutral polar molecules is theoretically demonstrated. This method utilizes non-uniform, static electric fields and regions of adiabatic population transfer to generate a mechanical force that opposes the molecular beam's velocity. By coupling this technique with dissipative trap-loading, molecular densities $\geq10^{11}$ cm$^{-3}$ are possible. When used in combination with forced evaporative cooling the proposed method may represent a viable route to quantum degeneracy for a wide-class of molecular species.
Carbon monoxide molecules in their electronic, vibrational, and rotational ground state are highly attractive for trapping experiments. The optical or ac electric traps that can be envisioned for these molecules will be very shallow, however, with depths in the sub-milliKelvin range. Here we outline that the required samples of translationally cold CO (X$^1Σ^+$, $v"$=0, $N"$=0) molecules can be produced after Stark deceleration of a beam of laser-prepared metastable CO (a$^3Π_1$) molecules followed by optical transfer of the metastable species to the ground state \emph{via} perturbed levels in…
Polar heavy-atom molecules have been well recognized as promising candidates for precision measurements and tests of fundamental physics. A much slower molecular beam to increase the interaction time should lead to a more sensitive measurement. Here we theoretically demonstrate the possibility of the stimulated longitudinal slowing of heavy-atom molecules by the coherent optical bichromatic force with a constant beat phase. Taking the YbF meolecule as an example, we show that a rapid and short-distance deceleration of heavy molecules by a phase-compensation method is feasible with moderate con…
In this paper we study the ionization rate and the Stark shift of a one-dimensional model of the H$_{2}^{+}$ ion. The finding of these two quantities is reduced to the solutions of a complex eigenvalue problem. We solve this problem both numerically and analytically. In the latter case we consider the regime of small external electrostatic fields and small internuclear distances. We find an excellent agreement between the ionization rate computed with the two approaches, even when the approximate result is pushed beyond its expected validity. The ionization rate is very sensitive to small chan…
Patterson, Schnell, \& Doyle, {\it Nature} {\bf 497}, 475 (2013) introduced a microwave experiment that produces a perpendicularly polarized molecular emission when chiral molecules are resonantly excited in the presence of a Stark Field that is then adiabatically switched off before observation of the emission. The sign of the signal is opposite for two stereo-enantiomers and thus the magnitude of the signal gives the enantiomeric excess of the sample. This paper presents a detailed presentation of the theory behind this and provides expressions for the absolute calculation of the expected si…
Recently, a decelerator for neutral polar molecules has been presented that operates on the basis of macroscopic, three-dimensional, traveling electrostatic traps (Osterwalder et al., Phys. Rev. A 81, 051401 (2010)). In the present paper, a complete description of this decelerator is given, with emphasis on the electronics and the mechanical design. Experimental results showing the transverse velocity distributions of guided molecules are shown and compared to trajectory simulations. An assessment of non-adiabatic losses is made by comparing the deceleration signals from 13-CO with those from …
Selection of "magic" trapping conditions with ultracold atoms or molecules, where pairs of internal states experience identical trapping potentials, brings substantial benefits to precision measurements and quantum computing schemes. Working at such conditions could ensure that detrimental effects of inevitable inhomogeneities across an ultracold sample are significantly reduced. However, this aspect of confinement remains unexplored for ultracold polar molecules. Here, we present means to control the AC Stark shift of rotational states of ultracold polar molecules, when subjected to both trap…
We show that combined permanent and induced electric dipole interactions of polar and polarizable molecules with collinear electric fields lead to a sui generis topology of the corresponding Stark energy surfaces and of other observables - such as alignment and orientation cosines - in the plane spanned by the permanent and induced dipole interaction parameters. We find that the loci of the intersections of the surfaces can be traced analytically and that the eigenstates as well as the number of their intersections can be characterized by a single integer index. The value of the index, distinc…
We present ultrahigh-resolution measurements of state-to-state inelastic differential cross sections for NO-Ne and NO-Ar collisions, obtained by combining the Stark deceleration and velocity map imaging techniques. We show that for counterpropagating crossed beam geometries, the effect of the velocity spreads of the reagent beams on the angular resolution of the images is minimized. Futhermore, the counterpropagating geometry results in images that are symmetric with respect to the relative velocity vector. This allows for the use of inverse Abel transformation methods that enhance the resolut…
By invoking supersymmetry, we found a condition under which the Stark effect problem for a polar and polarizable molecule subject to nonresonant electric fields becomes exactly solvable. The exact solvability condition for the interaction parameters involved yields exact wavefunction for the "stretched" states, $|J=m,m>$, and for the $|1,1>$ state in the case of a purely induced-dipole interaction. The analytic expressions for the eigenenergy, the space-fixed dipole moment, the alignment cosine, and the expectation value of the angular momentum allow to readily reverse-engineer the problem of …
We perform precision microwave spectroscopy--aided by Stark deceleration--to reveal the low magnetic field behavior of OH in its ^2Π_{3/2} ro-vibronic ground state, identifying two field-insensitive hyperfine transitions suitable as qubits and determining a differential Lande g-factor of 1.267(5)\times10^{-3} between opposite parity components of the Λ-doublet. The data are successfully modeled with an effective hyperfine Zeeman Hamiltonian, which we use to make a tenfold improvement of the magnetically sensitive, astrophysically important ΔF=\pm1 satellite-line frequencies, yielding 172052988…
The Stark resonance parameters for the $3a_{1}$ molecular orbital of H$_{2}$O are computed by solving a system of partial differential equations in spherical polar coordinates. The starting point of the calculation is the quantum potential derived for this orbital from a single-center expanded Hartree-Fock orbital. The resonance positions and widths are obtained after applying an exterior complex scaling technique to describe the ionization regime for external fields applied along the two distinct $\hat{z}$ directions associated with the symmetry axis. The procedure thus avoids the computation…
We study the chirality of ground-state alkali atoms in E and B fields, dressed with a circularly-polarized laser beam close-detuned from an E-field-assisted forbidden transition, such as 7S-8S in Fr. We predict a parity violating energy shift of their sublevels, linear in E, and the weak nuclear charge Q_W$. A dressing beam of 10 kW/cm$^2$ at 506 nm produces a shift of $\sim100 μ$Hz at E=100 V/cm, B $\gtrsim$30 mG. It should be observable with $\sim 10^4$ Fr atoms confined in an optical dipole trap. We discuss optimal conditions, parameter reversals and a calibration procedure to measure $Q_W$…
We demonstrate theoretically the existence of a linear dc Stark shift of the individual substates of an alkali atom in its ground state, dressed by a circularly polarized laser field. It arises from the electroweak nuclear anapole moment violating P but not T. It is characterized by the pseudoscalar equal to the mixed product formed with the photon angular momentum and static electric and magnetic fields. We derive the relevant left-right asymmetry with its complete signature in a field configuration selected for a precision measurement with cold atom beams. The 3,3 to 4,3 Cs hyperfine-transit…
Arrays of trapped ultracold molecules represent a promising platform for implementing a universal quantum computer. DeMille has detailed a prototype design based on Stark states of polar $^1Σ$ molecules as qubits. Herein, we consider an array of polar $^2Σ$ molecules which are, in addition, inherently paramagnetic and whose Hund's case (b) free-rotor states are Bell states. We show that by subjecting the array to combinations of concurrent homogeneous and inhomogeneous electric and magnetic fields, the entanglement of the array's Stark and Zeeman states can be tuned and the qubit sites address…
We present single-molecule and macroscopic calculations showing that laser-induced Stark shifts contribute significantly to the phase of high-order harmonics from polar molecules. This is important for orbital tomography, where phases of field-free dipole matrix elements are needed in order to reconstruct molecular orbitals. We derive an analytical expression that allows the first-order Stark phase to be subtracted from experimental measurements.
We propose a method for controlling a class of low temperature chemical reactions. Specifically, we show the hydrogen abstraction channel in the reaction of formaldehyde (H$_{2}$CO) and the hydroxyl radical (OH) can be controlled through either the molecular state or an external electric field. We also outline experiments for investigating and demonstrating control over this important reaction. To this end, we report the first Stark deceleration of the H$_{2}$CO molecule. We have decelerated a molecular beam of H$_{2}$CO essentially to rest, producing cold molecule packets at a temperature of …
We propose and analyze an electrostatic-optical nano-scale trap for cold diatomic polar molecules. The main ingredient of our proposal is an square-array of ferroelectric nano-rods {with alternating polarization}. We show that, in contrast to electrostatic traps using the linear Stark effect, a quadratic Stark potential supports long-lived trapped states. The molecules are kept at a fixed height from the nano-rods by a standing-wave optical dipole trap. For the molecules and materials considered, we find that nano-traps with trap frequency up to 1MHz, ground-state width $\sim20$nm with lattice…
We made use of supersymmetric (SUSY) quantum mechanics to find a condition under which the Stark effect problem for a polar and polarizable closed-shell diatomic molecule subject to collinear electrostatic and nonresonant radiative fields becomes exactly solvable. The condition, $Δω= \frac{ω^2}{4 (m+1)^2}$, connects values of the dimensionless parameters $ω$ and $Δω$ that characterize the strengths of the permanent and induced dipole interactions of the molecule with the respective fields. The exact solutions are obtained for the $|\tilde{J}=m,m;ω,Δω>$ family of "stretched" states. The field-f…
We report on the Stark deceleration and electrostatic trapping of $^{14}$NH ($a ^1Δ$) radicals. In the trap, the molecules are excited on the spin-forbidden $A ^3Π\leftarrow a ^1Δ$ transition and detected via their subsequent fluorescence to the $X ^3Σ^-$ ground state. The 1/e trapping time is 1.4 $\pm$ 0.1 s, from which a lower limit of 2.7 s for the radiative lifetime of the $a ^1Δ, v=0,J=2$ state is deduced. The spectral profile of the molecules in the trapping field is measured to probe their spatial distribution. Electrostatic trapping of metastable NH followed by optical pumping of the t…
We make use of an inhomogeneous electrostatic dipole field to impart a quantum-state-dependent deflection to a pulsed beam of OCS molecules, and show that those molecules residing in the absolute ground state, $X ^1Σ^+$, $\ket{00^00}$, J=0, can be separated out by selecting the most deflected part of the molecular beam. Past the deflector, we irradiate the molecular beam by a linearly polarized pulsed nonresonant laser beam that impulsively aligns the OCS molecules. Their alignment, monitored via velocity-map imaging, is measured as a function of time, and the time dependence of the alignment …
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.
