This content has been downloaded from IOPscience. Please scroll down to see the full text. Download details: IP Address: 18.51.1.63 This content was downloaded on 19/05/2017 at 13:22 Please note that terms and conditions apply. One-dimensional magneto-optical compression of a cold CaF molecular beam View the table of contents for this issue, or go to the journal homepage for more 2017 New J. Phys. 19 033035 (http://iopscience.iop.org/1367-2630/19/3/033035) Home Search Collections Journals About Contact us My IOPscience You may also be interested in: Laser slowing of CaF molecules to near the capture velocity of a molecular MOT Boerge Hemmerling, Eunmi Chae, Aakash Ravi et al. Improved magneto–optical trapping of a diatomic molecule D J McCarron, E B Norrgard, M H Steinecker et al. An intense, cold, velocity-controlled molecular beam by frequency-chirped laser slowing S Truppe, H J Williams, N J Fitch et al. 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Phys. 19 (2017) 033035 https://doi.org/10.1088/1367-2630/aa6470 PAPER One-dimensional magneto-optical compression of a cold CaF molecular beam EunmiChae1,2,5, Loic Anderegg1,2, Benjamin LAugenbraun1,2, AakashRavi1,2, BoergeHemmerling1,2,6, Nicholas RHutzler1,2, Alejandra LCollopy3, JunYe3,WolfgangKetterle2,4 and JohnMDoyle1,2 1 Department of Physics, HarvardUniversity, Cambridge,MA02138,United States of America 2 Harvard-MITCenter forUltracold Atoms, Cambridge,MA02138,United States of America 3 JILA,National Institute of Standards andTechnology andUniversity of Colorado, Boulder, CO80309,United States of America 4 Department of Physics,Massachusetts Institute of Technology, Cambridge,MA02139,United States of America 5 Present address: Photon ScienceCenter, School of Engineering, theUniversity of Tokyo, Japan 113-8656. 6 Present address: Department of Physics, University of California, Berkeley, CA 94720,United States of America. E-mail: eunmi@cua.harvard.edu Keywords: laser cooling ofmolecules,molecular RFmagneto-optical trap, cryogenicmolecular buffer-gas beam Abstract Wedemonstrate the one-dimensional, transversemagneto-optical compression of a cold beamof calciummonofluoride (CaF). By continually alternating themagnetic field direction and laser polarizations of themagneto-optical trap (RFMOT), a photon scattering rate of 2 0.4 MHzp ´ is achieved. A 3Dmodel for this RFMOT, validated by agreement with data, predicts a 3DRFMOT capture velocity for CaF of 5m s–1. 1. Introduction Molecules are intriguing candidates for the study of fundamental symmetry violation, quantum simulation of strongly correlatedHamiltonians, and the creation of new quantum information systems that take advantage of internalmolecular degrees of freedom [1–10]. In addition, active research is ongoing to create coldmolecules for new studies in order to understand the full role of quantummechanics in chemical reactions [11, 12]. Themain difficulty in pursuing these goals is to controllably preparemolecules in single quantum states, and to achieve long interaction times (typically achieved via trapping). Even the simplestmolecules, diatomicmolecules, have complex enough internal structure that, at room temperature, typically tens of thousands of states are thermally populated. Only very recently havemolecular quantum states been controlled in away to allow for quantum state-dependent chemical reactions [11, 12]. In that work, ultracold bi-alkalimolecules were produced in a single quantum state by combining two ultracold alkali atoms, taking advantage of themature, powerful tools for atom cooling [13–18]. However, this technique is so far limited to a specific subset ofmolecules, typically bialkalis in the 1S state. Extension of thesemethods tomore chemically diverse species is a formidable challenge. To fully utilize the powerful diversity ofmolecules, newmethods to produce cold and ultracoldmolecules (e.g. thosewith electron spin degree of freedom) are desirable. A crucial step towards achieving lower temperatures is trapping, which in itself allows for further coolingmethods to be applied.Major efforts are currently ongoing to trapmolecules using electric,magnetic, and optical forces [19–31]. One promising option is amagneto-optical trap (MOT), theworkhorse tool of optical cooling and confinement for atoms. Despite thorough study and understanding of atomicMOTs, the additional internal structure present inmolecules has made it difficult to produce amolecularMOT,mostly due to the lack of closed cycling transitions. It is possible to overcome this difficulty by usingmolecules with sufficiently diagonal Franck–Condon factors (FCFs), as was proposed in [32, 33]. Recently, 2D and 3DMOTs formolecules have been realizedwith YO and SrF [34–37]. This scheme, although limited tomolecules with strong optical transitions and highly diagonal FCFs, represents a powerful step toward broadening the scope ofmolecules that can be brought to the ultracold regime, including manywhich are of interest for new schemes in quantum simulation [6]. OPEN ACCESS RECEIVED 11 January 2017 REVISED 13 February 2017 ACCEPTED FOR PUBLICATION 3March 2017 PUBLISHED 27March 2017 Original content from this workmay be used under the terms of the Creative CommonsAttribution 3.0 licence. Any further distribution of this workmustmaintain attribution to the author(s) and the title of thework, journal citation andDOI. © 2017 IOPPublishing Ltd andDeutsche PhysikalischeGesellschaft CaF is a prototypicalmolecule for cold and ultracold applications and has been studied extensively, including its collisional properties [38–42]. It has an unpaired outer shell electron, strong laser cooling transitions, and reasonably diagonal FCFs. Furthermore, its lightmass leads to a larger velocity change per photon scatter, which, compared to largermass species with all other spectroscopic properties the same, shortens the slowing distance and increases the capture velocity of aMOT. It is therefore amolecule that is well suited for laser cooling. Using the X v A v0 0= - ¢ =( ) ( ) transition at 606 nmwith a linewidth of 2 8.29 MHzp ´ [38], about 105 photons can be scatteredwith 2 vibrational repump lasers, before falling into higher vibrational states [43]. Recent theoretical work indicates that CaF is a good candidate for sympathetic/ evaporative cooling to reach temperatures in themicrokelvin regime, a necessary step toward quantum degeneracy [41, 42]. Once an ensemble of ultracoldCaFmolecules is prepared, its large electric dipolemoment and spin degree of freedomwill expand theHamiltonians that can be simulated, including spin-lattice models [6]. Here we report a demonstration ofmagneto-optical compression of aCaFmolecular beam. This is a key milestone towards loadingCaF into a 3DMOT. This work verifies all of the processes and technology necessary formagneto-optical trapping of CaF, identifies an importantMOT-limiting feature of CaF due to level crossings, and provides crucial data for validating RFMOT loadingmodels. Our results also point towards the optimal parameters for achieving a RFMOTwith amaximumnumber of trappedCaFmolecules. 2.Methods Aschematic of the apparatus is depicted infigure1. Inour experiment, a cryogenic two-stage buffer-gas beamsource is used toproduce a coldCaFmolecular beam [44–47]. CaFmolecules are generatedby ablating ametallicCa target in anSF6 ice environmentwithin a copper cell, similar to thework in [48]. Themolecules are cooled through collisions withHegas in a cell held at a temperature of around2K.Coldmolecules and atomicHe exit the cell aperture, forming abeamwith amean forward velocity of 110±10m s–1, and velocity spreadof 40m s–1. To reduce the amountof buffer gas reaching the interaction region and to collimate themolecular beam, a 6mm×6mmaperture is placed 41 cm fromthe cell, 9 cmbefore themolecules interactwith theRFMOTmagneticfields and corresponding transverse laser beams.This aperture sets themolecular beamwidth in thedetection area. In these experiments only a singleMOTbeam—transverse to themolecular beam—is used toquantitatively study theRFmagneto-optical force in 1D [34]. Aftermolecules pass through the interaction region, they travel about 30 cm fartherwhere they are detectedon anEMCCD (Andor, LucaR)usingfluorescence. The relevant energy levels of CaF are shown infigure 2. The optical transitions in use are from the electronic ground stateX to thefirst electronic excited stateA. Themeasured FCF for X v A v0 0= - ¢ =( ) ( ) is 0.987 [38] and one vibrational repump laser from the v=1 state is used, allowing up to 1000 photons to be scattered before pumping of themolecules to the v=2 state [43]. Loss to other rotational states is prevented by addressing a J to J J 1¢ = - transition [33]. In this transition, the rotationally excited X N 1=( ) state is excited to the N 0¢ = state of theA state so that a combination of parity and angularmomentum selection rules results in the A N 0¢ =( ) statemolecules decaying back to the X N 1=( ) state. Figure 1.Experimental setup (not to scale). The cell wheremolecules are generated is cooled by a pumped liquid 4He bath. An aperture of 6mm×6 mm is placed 41 cmdownstream from the cell to collimate themolecular beam and to reduce the remaining 4He buffer-gas. Themolecules interact with the lasers 50 cm from the cell where the in-vacuumRF coils are in place. After the interaction, themolecules travel 30 cm farther and are detected byfluorescencewith an electronmultiplying charge-coupled device (EMCCD) camera. All lasers include X v A v0, 1 0= - ¢ =( ) ( ) transitions and their hyperfine splittings. 2 New J. Phys. 19 (2017) 033035 EChae et al There are 4 hyperfine states that are spaced a few tens ofMHz in the X N 1=( ) statemanifold due to coupling of the electron’s spin S 1 2=( )with themolecular rotation N 1=( ) andfluorine’s nuclear spin I 1 2=( ). This hyperfine splitting weakens themagneto-optical force in twoways: reduction of the scattering rate and level-crossing inweakmagnetic fields at around 10Gauss (figure 2 inset). All states are individually addressed through frequency sidebands placed on the lasers. One of the hyperfine states (J F1 2, 1= = ) has an opposite sign of the g factor and the polarization of the lasers addressing this state has opposite handedness relative to the other states. The intensity of the X v A v0 0= - ¢ =( ) ( ) lasers for all hyperfine states is 150 mW cm−2 in total, and the intensity of the repump lasers for the X v A v1 0= - ¢ =( ) ( ) transition is 100 mW cm−2. The lasers areGaussian beamswith e1 2 diameter of 7 mm.The powers among the hyperfine states areweighted by the degeneracy of the state. This is due to the fact that scattering rate for theMOTdepends on the laser intensity for individual states as [37] R n n n I I2 1 4 , 1e g e j n j j j sc 1 2 2 sat, gå= G + + + D G=( ) ( ) ( ) whereΓ is a linewidth of the excited states (2 8.29 MHzp ´ [38]), ng(ne) is the number of involved states in the ground (excited) statemanifold, jD is a laser detuning for the j state, I jsat, is a two-level saturation intensity for the j state (4.87 mW cm−2 and 4.37 mW cm−2 for the v = 0 and v = 1 states respectively), and Ij is laser intensity for the j state. The experimental parameters result in the scattering rate R 2 0.43 MHzsc p~ ´ from equation (1). The hyperfine splitting of the excited stateA is unresolved [38]. One additional complication of amolecularMOT compared to an atomicMOT is that the number of involved groundmagnetic substates is greater than that of the excited states. Because of this, some of the states become dark states of the confining lasers. The onlywaymolecules could get out those states in a normalMOT would be scattering anti-confining photons, destroying theMOT effect. RFMOTs [34, 37] solve this problemby actively switching themagnetic field gradient and the polarization of the light synchronously at a rate comparable to the excited state’s lifetime.With this scheme,molecules in all states predominantly scatter photons that lead to confinement and can be trapped. Switching of the lasers’ polarizations is implemented using a Pockels cell. To switch the neededmagnetic fields at a rate on the order ofMHz, the coils aremade small and internal to the vacuumchamber (figure 3). The coils aremade out of a 0.85 mm thick copper sheet cut to a spiral coil shapewithwirewidth of 1 mmon a 1.5 mm thick alumina substrate. The inner diameter of the coils is about 15 mmand there are 6 turns for each coil. There are 4 coils total, 2 on the upper board and 2 on the lower board Figure 2. Level diagram forCaFmolecules. Only relevant levels are shown.Quantumnumbers for vibration, rotation, electronic angularmomentumplus rotation, and themolecule’s total angularmomentum are v,N, J, and F respectively. The parity of the state is denoted by±. The straight lines indicate lasers used in the experiment andwavy lines show the decay from the excited states. FCFs ( fij) are also shown. The inset shows the hyperfine states and their Zeeman shift in the ground state X v N0, 1= =( ). The red-detuned laser frequencies are shown in red broken lines in the inset. The hyperfine splitting and the Zeeman shift of the excited state A v J0, 1 2¢ = ¢ =( ) is negligible [39]. 3 New J. Phys. 19 (2017) 033035 EChae et al —with the boards spaced by 16 mm.Coils on the same board arewired in aHelmholtz configuration, while the two boards together provide an anti-Helmholtz field in the space between them.Aluminawas chosen due to its lowoutgassing rate (necessary for theUHVenvironment of theMOT) and good thermal conductivity (necessary to carry out the substantial heating producedwhen switching the coils at high frequencies). The alumina boards aremounted on an aluminumblock, which is itselfmounted to a copper block feedthrough.On the air-side of the feedthrough, we put a passive heatsink to further increase the cooling power.With this setup, we observe only a few degrees of temperature increase of the block feedthroughwhen running the coils in RFmode at 830 kHz. The coil assembly is connected to a resonant circuit outside of the chamber.With 1Ampof current run through the coils, a quadrupolemagnetic field of about 7.3 (3.7)Gauss cm–1 is produced in the axial (radial) direction. Themolecules are detected by collecting fluorescent photons using an EMCCDcamera. The excitation lasers (X v A v0, 1 0= - ¢ =( ) ( )) cross themolecular beam at 90 degrees in the detection region, 80 cm downstream from the source. Themeasuredwidth of themolecular beam is a convolution of the transverse velocity of the beam and the initial beam spread.We analyze thismolecular beamwidth to infer the compression and cooling effect from themagneto-optical force. 3. Results and discussion Figures 4 and 5 show the compression of themolecular beamby themagneto-optical force. Typicalmolecular beam signals with red-detuned X v A v0 0= - ¢ =( ) ( ) lasers when themagnetic field and the light polarization are in phase and out of phase are depicted infigure 4. Themagneto-optical compression narrows themolecular beamwhen the phase of themagnetic field and the light polarization arematched. In the opposite conditionwith the relative phase of 180°, themolecular beam experiences an anti-confining force and its width is increased. The measured beamprofiles arefit using super-Gaussian functions of order 4with their amplitudes, beamwidths as given by the e1 radius of a fit, and centers as free parameters. Thefitted beamwidths are plotted infigure 5. Each data point infigure 5 is the average of 350measurements (molecular pulses) for the red-detunedmagneto-optical compression andDoppler cooling (figure 5(a)), and 200 (800)measurements for the blue-detunedmagneto-optical compression (Doppler heating) (figure 5(b)). The relative phase between the polarization and themagnetic field is changed between each data point. Error bars indicate one-standard-deviation statistical uncertainties from fits to beamprofiles. In the absence of the magnetic field, Doppler cooling (heating) is observedwith red (blue)-detuning of lasers. The direction of the magneto-optical force is seen to reverse with blue-detuning of the lasers compared to the case with red-detuning as expected. We have createdMonte-Carlo simulations of the RFMOT similar to that described in [34]. The results of these simulations are shown infigure 5 as solid lineswith scattering of 150 photons, corresponding to a photon scattering rate of 2 0.4p ´ MHz. This agrees with the expected scattering rate based on themeasured laser powers and transition strengths. Due to the asymmetric hyperfine structure of CaF, aMonte-Carlo simulation with only one effective detuning gives good agreement for the red-detuning, while results are inworse agreement for the blue-detuned case. Thewidths of themolecular beam in the detection region for different conditions are summarized infigure 6. At a detuning of 7MHz, the optimal compression is achievedwith amagneticfield gradient of 7.3Gauss cm–1. Several otherfield gradients (3.7, 4.4, 5.8, 12.4, and 18.3Gauss cm–1)were tested but the compression effects are reduced compared to the optimal gradient. This is due to the small hyperfine splitting ofCaF. Specifically, in a Figure 3.RFMOTcoils inside the vacuum chamber. The picture was taken before the inside was blackenedwith a non conductive, low outgassing paint (MH2200 fromAlion) to reduce the background scattered light. 4 New J. Phys. 19 (2017) 033035 EChae et al magneticfield greater than 5Gauss, the energy difference betweenmagnetic sublevels of different hyperfine states approaches the natural linewidth. This increases theprobability of scattering anti-confining photons, and thus weakens the compression effect. The 1Dmagneto-optical compression demonstrated here provides uswith an improved understanding of the 3DMOT forCaF.Using the number of scattered photons in 1Dmagneto-optical compression, simple calculations estimate amaximum (on-axis, perfect conditions) capture velocity of about 13 m s–1 for the 3D MOT in this experimental setupwith our current geometry and a fairly generic laser configuration for theX–A transition.We have also performed a full 3DMOTMonte-Carlo simulation of trap loading for both on-axis and themore realistic set ofmolecular trajectories that include off-axismolecules. Considering the limiting case of molecules entering theMOT region only directly on-axis with the zeromagnetic field point of theMOT, the capture velocity is seen in the simulation to be 10 m s–1, which agrees with the simple calculation.However, since the capture velocity decreases as themolecules travel off axis, wefind that the averaged capture velocity is about half of the ideal on-axis estimation, resulting in an effective capture velocity (simulating themolecular beam as a whole, including off-axis trajectories) of about 5 m s–1 for themolecular beam as awhole.White-light slowing of Figure 4. (a)Typical beamdatawith red-detuned lasers. The transverse beam shape after (anti)magneto-optical compression is depicted as a (red) blue line. The two configurations are achieved by changing the phase of themagnetic fields by 180°. The integrated area of the beam is conserved for the both cases. (b)The residuals of thefits to super-Gaussian functions are shown. The vertical unit is same as in (a). Due to the original beam shape that is skewed to the leftside, the residuals differ from zero on the edges of the beams , as expected. However, the residuals of theMOT and the anti-MOTdata are equal to a level smaller than the average shift where the profile ismost sensitive, thewings and peak. This assures that thefitting is a valuable quantitative evaluation of themagneto-optical compression. Figure 5.Molecular beamwidths are plotted as a function of the relative phase between themagnetic field and the polarization of the lasers: red dots in (a) for the X v A v0 0= - =( ) ( ) laser detuning of−7 MHz, and blue dots in (b) for the X v A v0 0= - =( ) ( ) laser detuning of+7 MHz. The black dot in eachfigure indicates the beamwidthwhen theMOT coils were switched off and reflects the effect of Doppler cooling or heating. Gray area is a guide to eyes, indicating the 1s confidence region of theDopplerwidth. Error bars are one-standard-deviation statistical uncertainties fromfits to beamprofiles. Lines show theMonte-Carlo simulation results for each case. 5 New J. Phys. 19 (2017) 033035 EChae et al aCaFmolecular beamdemonstrated previously in our group [47] resulted in about 5×104molecules at 5±4 m s–1 detected in the capture volume of theMOT.We expect a good fraction of thesemolecules would be captured in a RFMOTwith current techniques. 4. Conclusion Magneto-optical compression of a buffer-gas cooledCaF beamhas been achieved. By scattering 150 photons during the timemolecules spend in the RFMOT region (about 60μs), themolecular beam is compressed, in good agreement with ourfirst principlesmodel. From the demonstratedmolecular beam compression, we estimate a RFMOT capture velocity of 5 m s–1 for CaF. This work provides a deeper understanding of themagneto-optical forces onCaFmolecules and guides the necessary experimental conditions for effective loading ofmolecularMOTs. 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