J. R. Bochinski, Eric R. Hudson, H. J. Lewandowski, Jun Ye, Gerard Meijer
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.
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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 …
Ultracold CH radicals promise a fruitful testbed for probing quantum-state controllable organic chemistry. In this work, we calculate CH vibrational branching ratios (VBRs) and rotational branching ratios (RBRs) with ground state mixing. We subsequently use these values to inform optical cycling proposals and consider two possible radiative cooling schemes using the $X^{2}Π\leftarrow A^{2}Δ$ and $X^{2}Π\leftarrow B^{2}Σ^{-}$ transitions. As a first step towards laser cooled CH, we characterize the effective buffer gas cooling of this species and produce $\sim5\times10^{10}$ CH molecules per pu…
A special class of molecules that are important to many subfields in molecular dynamics and chemical physics, namely free radical molecules, now enjoy a significant degree of center-of-mass motion control in the laboratory frame. The example reported in this paper concerns hydroxyl radical (OH), which, after the internal degrees of freedom are cooled in a supersonic expansion, has been bunched, accelerated, and slowed using time-varying inhomogeneous electric fields. In situ observations of laser-induced fluorescence along the beam propagation path allows for detailed characterization of the l…
We demonstrate a cryogenic buffer gas-cooled molecular beam source capable of producing bright, continuous beams of cold and slow free radicals via laser ablation over durations of up to 60~seconds. The source design uses a closed liquid helium reservoir as a large thermal mass to minimize heating and ensure reproducible beam properties during operation. Under typical conditions, the source produces beams of our test species SrF, containing $5\times10^{12}~$molecules per steradian per second in the $X^{2}Σ(v=0, N=1)$ state with a rotational temperature of $1.0(2)~$K and a forward velocity of $…
We have produced a cryogenic buffer-gas cooled beam of the diatomic molecular radical CH (methylidyne). This molecule is of interest for studying cold chemical reactions and fundamental physics measurements. Its light mass and ground-state structure make it a promising candidate for electrostatic guiding and Stark deceleration, which allows for control over its kinetic energy. This control can facilitate studies of reactions with tuneable collision energies and trapping for precise spectroscopic studies. Here, we have demonstrated electrostatic guiding of CH with fluxes up to $10^9$ molecules …
An improved system for creating a pulsed, low-temperature molecular beam of OH radicals has been developed. We use a pulsed discharge to create OH from H$_2$O seeded in Xe during a supersonic expansion, where the high-voltage pulse duration is significantly shorter than the width of the gas pulse. The pulsed discharge allows for control of the mean speed of the molecular packet as well as maintains a low temperature supersonic expansion. A hot filament is placed in the source chamber to initiate the discharge for shorter durations and at lower voltages, resulting in a translationally and rotat…
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.
The spectroscopy of free radicals and radical containing entrance-channel complexes embedded in superfluid helium nano-droplets is reviewed. The collection of dopants inside individual droplets in the beam represents a micro-canonical ensemble, and as such each droplet may be considered an isolated cryo-reactor. The unique properties of the droplets, namely their low temperature (0.4 K) and fast cooling rates ($\sim10^{16}$ K s$^{-1}$) provides novel opportunities for the formation and high-resolution studies of molecular complexes containing one or more free radicals. The production methods o…
Coherent superpositions of the 49s and 48s Rydberg states of cold Rb atoms were studied near the surface of an atom chip. The superpositions were created and manipulated using microwaves resonant with the two-photon 49s-48s transition. Coherent behavior was observed using Rabi flopping, Ramsey sequences, spin-echo and spin-locking. These results are discussed in the context of Rydberg atoms as electric field noise sensors. We consider the coherence of systems quadratically coupled to noise fields with 1/f^k power spectral densities (k \approx 1).
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 demonstrate Doppler-free saturated absorption spectroscopy of cold molecular radicals formed by laser ablation inside a cryogenic buffer gas cell. By lowering the temperature, congested regions of the spectrum can be simplified, and by using different temperatures for different regions of the spectrum a wide range of rotational states can be studied optimally. We use the technique to study the optical spectrum of YbF radicals with a resolution of 30 MHz, measuring the magnetic hyperfine parameters of the electronic ground state. The method is suitable for high resolution spectroscopy of a g…
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…
A brief perspective on light scattering in dense and cold atomic rubidium is presented. We particularly focus on the influence of auxiliary applied fields on the system response to a weak and nearly resonant probe field. Auxiliary fields can strongly disturb light propagation; in addition to the steady state case, dynamically interesting effects appear clearly in both the time domain, and in the optical polarization dependence of the processes. Following a general introduction, two examples of features found in such studies are presented. These include nonlinear optical effects in (a) comparat…
A strongly confined light field necessarily exhibits a local polarization that varies on a subwavelength scale. We demonstrate that a single optical mode of such kind can be used to selectively and simultaneously manipulate atomic ensembles that are less than a micron away from each other and equally coupled to the light field. The technique is implemented with an optical nanofiber that provides an evanescent field interface between a strongly guided optical mode and two diametric linear arrays of cesium atoms. Using this single optical mode, the two atomic ensembles can simultaneously be opti…
Advanced techniques for manipulation of internal states, standard in atomic physics, are demonstrated for a charged molecular species for the first time. We address individual hyperfine states of ro-vibrational levels of a diatomic ion by optical excitation of individual hyperfine transitions, and achieve controlled transfer of population into a selected hyperfine state. We use molecular hydrogen ions (HD^{+}) as a model system and employ a novel frequency-comb-based, continuous-wave 5 \mum laser spectrometer. The achieved spectral resolution is the highest obtained so far in the optical domai…
We present a theory for manipulation of d-wave interaction of cold atoms with two lasers strongly driving two photoassociative transitions. The theory predicts the occurrence of a coherence between two excited ro-vibrational bound states due to the photoassociative dipole-couplings of ground-state d-wave scattering state to the bound states. We show that this excited-state coherence significantly influences atom-atom interaction. In particular, this leads to the enhancement of d-wave elastic scattering and to the suppression of inelastic scattering. In the presence of an s-wave magnetic Feshba…
Neutral atoms trapped by laser light are amongst the most promising candidates for storing and processing information in a quantum computer or simulator. The application certainly calls for a scalable and flexible scheme for addressing and manipulating the atoms. We have now made this a reality by implementing a fast and versatile method to dynamically control the position of neutral atoms trapped in optical tweezers. The tweezers result from a spatial light modulator (SLM) controlling and shaping a large number of optical dipole-force traps. Trapped atoms adapt to any change in the potential …
We present a rigorous theoretical study of low-temperature collisions of polyatomic molecular radicals with ^1S_0 atoms in the presence of an external magnetic field. Accurate quantum scattering calculations based on ab initio and scaled interaction potentials show that collision-induced spin relaxation of the prototypical organic molecule CH_2(X^3B_1) (methylene) and nine other triatomic radicals in cold 3He gas occurs at a slow rate, demonstrating that cryogenic buffer-gas cooling and magnetic trapping of these molecules is feasible with current technology. Our calculations further suggest t…
The coherence of quantum systems is crucial to quantum information processing. While it has been demonstrated that superconducting qubits can process quantum information at microelectronics rates, it remains a challenge to preserve the coherence and therefore the quantum character of the information in these systems. An alternative is to share the tasks between different quantum platforms, e.g. cold atoms storing the quantum information processed by superconducting circuits. In our experiment, we characterize the coherence of superposition states of 87Rb atoms magnetically trapped on a superco…
We report precise measurements of ground-state, $λ$-doublet microwave transitions in the hydroxyl radical molecule (OH). Utilizing slow, cold molecules produced by a Stark decelerator we have improved over the precision of the previous best measurement by twenty-five-fold for the F' = 2 $\to$ F = 2 transition, yielding (1 667 358 996 $\pm$ 4) Hz, and by ten-fold for the F' = 1 $\to$ F = 1 transition, yielding (1 665 401 803 $\pm$ 12) Hz. Comparing these laboratory frequencies to those from OH megamasers in interstellar space will allow a sensitivity of 1 ppm for $Δα/α$ over $\sim$$10^{10}$ yea…
We present the first experimental observation of cold collisions between two different species of neutral polar molecules, each prepared in a single internal quantum state. Combining for the first time the techniques of Stark deceleration, magnetic trapping, and cryogenic buffer gas cooling allows the enhancement of molecular interaction time by 10$^5$. This has enabled an absolute measurement of the total trap loss cross sections between OH and ND$_3$ at a mean collision energy of 3.6 cm$^{-1}$ (5 K). Due to the dipolar interaction, the total cross section increases upon application of an ext…
Trapping molecular ions that have been sympathetically cooled with laser-cooled atomic ions is a useful platform for exploring cold ion chemistry. We designed and characterized a new experimental apparatus for probing chemical reaction dynamics between molecular cations and neutral radicals at temperatures below 1 K. The ions are trapped in a linear quadrupole radio-frequency trap and sympathetically cooled by co-trapped, laser-cooled, atomic ions. The ion trap is coupled to a time-of-flight mass spectrometer to readily identify product ion species, as well as to accurately determine trapped i…
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 …
We demonstrate high resolution coherent control of cold atomic Rubidium utilizing spectral phase manipulation of a femtosecond optical frequency comb. Transient coherent accumulation is directly manifested by the enhancement of signal amplitude and spectral resolution via the pulse number. The combination of frequency comb technology and spectral phase manipulation enables coherent control techniques to enter a new regime with natural linewidth resolutions.
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 present the integrated imaging of cold molecules in a microchip environment. The on-chip de- tection is based on REMPI, which is quantum-state-selective and generally applicable. We demon- strate and characterize time-resolved spatial imaging and subsequently use it to analyze the effect of a phase-space manipulation sequence aimed at compressing the velocity distribution of a molec- ular ensemble with a view to future high-resolution spectroscopic studies. The realization of such on-chip measurements adds the final fundamental component to the molecule chip, offering a new and promising ro…
Effective and unrestricted engineering of atom-photon interactions requires precise spatially-resolved control of light beams. The significant potential of such manipulations lies in a set of disciplines ranging from solid state to atomic physics. Here we use a Zeeman-like ac-Stark shift of a shaped laser beam to perform rotations of spins with spatial resolution in a large ensemble of cold rubidium atoms. We show that inhomogeneities of light intensity are the main source of dephasing and thus decoherence, yet with proper beam shaping this deleterious effect is strongly mitigated allowing rot…
We use accurate ab initio and quantum scattering calculations to explore the prospects for sympathetic cooling of the heavy molecular radical SrOH($^2Σ$) by ultracold Li atoms in a magnetic trap. A two-dimensional potential energy surface (PES) for the triplet electronic state of Li-SrOH is calculated ab initio using the partially spin-restricted coupled cluster method with single, double and perturbative triple excitations and a large correlation-consistent basis set. The highly anisotropic PES has a deep global minimum in the skewed Li-HOSr geometry with $D_e=4932$ cm$^{-1}$ and saddle point…
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, Ultr…
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…
Quantum state manipulation and cooling of ultracold molecules
本文综述了将超冷原子缔合为分子量子气体和直接激光冷却两种技术，它们使分子进入量子领域，实现了对分子内、外态的量子操控，为冷分子科学探索开辟了新空间。
The methods producing cold molecules from cold atoms tend to leave molecular ensembles with substantial residual internal energy. For instance, Cs2 molecules initially formed via photoassociation of cold Cs atoms are in several vibrational levels, v, of the electronic ground state. Here we apply a broadband femtosecond laser that redistributes the vibrational population in the ground state via a few electronic excitation - spontaneous emission cycles. The laser pulses are shaped to remove the excitation frequency band of the v = 0 level, preventing re-excitation from that state. We observe a f…
There has been a recent surge of interest and progress in creating subwavelength free-space optical potentials for ultra-cold atoms. A key open question is whether geometric potentials, which are repulsive and ubiquitous in the creation of subwavelength free-space potentials, forbid the creation of narrow traps with long lifetimes. Here, we show that it is possible to create such traps. We propose two schemes for realizing subwavelength traps and demonstrate their superiority over existing proposals. We analyze the lifetime of atoms in such traps and show that long-lived bound states are possi…
Chemistry in a Cryogenic Buffer Gas Cell
本研究在低温缓冲气体细胞中研究了钙与氢同位素的化学反应，发现H₂作为反应物和缓冲气体的性能优于D₂和HD，并揭示了反应物振动激发对分子产量的影响。
We report on the storage of orbital angu- lar momentum (OAM) of light of a Laguerre-Gaussian mode in an ensemble of cold cesium atoms and its re- trieval along an axis different from the incident light beam. We employed a time-delayed four-wave mixing configuration to demonstrate that at small angle (2o), after storage, the retrieved beam carries the same OAM as the one encoded in the input beam. A calculation based on mode decomposition of the retrieved beam over the Laguerre-Gaussian basis is in agreement with the experimental observations done at small angle values. However, the calculation…
Spatially structured light has opened a wide range of opportunities for enhanced imaging as well as optical manipulation and particle confinement. Here, we show that phase-coherent illumination with superpositions of radial Laguerre-Gauss (LG) beams provides improved localization for bright optical tweezer traps, with narrowed radial and axial intensity distributions. Further, the Gouy phase shifts for sums of tightly focused radial LG fields can be exploited for novel phase-contrast strategies at the wavelength scale. One example developed here is the suppression of interference fringes from …
Design and Performance of a Heated Gas Injector for Producing Cold Molecular Beams
本文设计并实现了一种加热气体注入器，将热气体直接送入低温环境，具有坚固、易安装、热隔离好等优点，并用于产生冷BaF自由基，未来将用于激光冷却含镭分子。
Dynamical low-noise microwave source for cold-atom experiments
针对冷原子实验对超低噪声动态可控微波场的需求，提出结合7 GHz超低噪声振荡器与射频直接数字合成器的双路低相位噪声微波源，实现亚微秒级参数更新与低积分相位噪声，支持整形脉冲与复合脉冲以抑制噪声。
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