Transition Dipole Moment Measurements of Ultracold Photoassociated 85Rb133cs Molecules by Depletion Spectroscopy ∗

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Transition Dipole Moment Measurements of Ultracold Photoassociated 85Rb133cs Molecules by Depletion Spectroscopy ∗ CHIN. PHYS. LETT. Vol. 35, No. 10 (2018) 103301 Transition Dipole Moment Measurements of Ultracold Photoassociated 85Rb133Cs Molecules by Depletion Spectroscopy ∗ Juan-Juan Cao(曹娟娟)1;2, Ting Gong(宫廷)1;2, Zhong-Hao Li(李中豪)1;2, Zhong-Hua Ji(姬中华)1;2**, Yan-Ting Zhao(赵延霆)1;2, Lian-Tuan Xiao(肖连团)1;2, Suo-Tang Jia(贾锁堂)1;2 1State Key Laboratory of Quantum Optics and Quantum Optics Devices, Institute of Laser Spectroscopy, Shanxi University, Taiyuan 030006 2Collaborative Innovation Center of Extreme Optics, Shanxi University, Taiyuan 030006 (Received 6 July 2018) The transition dipole moments (TDMs) of ultracold 85Rb133Cs molecules between the lowest vibrational ground 1 + 3 0 0 1 0 level, X Σ (v = 0, J = 1), and the two excited rovibrational levels, 2 Π0+ (v = 10, J = 2) and 2 Π1 (v = 22, J 0 = 2), are measured using depletion spectroscopy. The ground-state 85Rb133Cs molecules are formed from 3 cold mixed component atoms via the 2 Π0− (v = 11, J = 0) short-range level, then detected by time-of-flight mass spectrum. A home-made external-cavity diode laser is used as the depletion laser to couple the ground level and the two excited levels. Based on the depletion spectroscopy, the corresponding TDMs are then derived −3 −2 to be 3.5(2)×10 ea0 and 1.6(1)×10 ea0, respectively, where ea0 represents the atomic unit of electric dipole 1 0 0 moment. The enhance of TDM with nearly a factor of 5 for the 2 Π1 (v = 22, J = 2) excited level means that it has stronger coupling with the ground level. It is meaningful to find more levels with much more strong coupling strength by the represented depletion spectroscopy to realize direct stimulated Raman adiabatic passage transfer from scattering atomic states to deeply molecular states. PACS: 33.80.−b, 32.70.Cs, 32.80.−t DOI: 10.1088/0256-307X/35/10/103301 Ultracold molecules have attracted widespread at- for other heteronuclear molecules. This is an obsta- tention in recent years. Compared with homonu- cle to transferring mixed cooled atoms directly to the clear molecules, heteronuclear (or polar) molecules deeply bound molecular state. Thus it is meaningful have unique properties: tunable, long-range and to search for more suitable excited PA states which anisotropic dipole-dipole interaction. These proper- have both singlet and triplet characters for efficiently ties mean ultracold polar molecules have many impor- producing and transfering molecules from atoms. Re- 1 tant applications, such as ultracold chemistry, quan- cently, Shimasaki et al. studied such mixed 2 Π1- 3 3 + [18] tum computer, quantum simulation and precision 2 Π1-3 Σ1 states. It is found that the product rate measurement.[1;2] is comparative with the previous value of two-photon Up to date, the methods to prepare ultra- cascade decay, and the direct spontaneous decay may cold molecules include photoassociation (PA) by play an important role due to the mixed characters. [3] [4] 1 continuous and shaped laser, magentoassocia- Especially for the 2 Π1 state, it has mainly a single tion (MA)[5] or spin-orbit coupling[6] from precooled character and may have stronger coupling with the atoms, and direct laser cooling[7] from preexisting ground state. Thus we need to measure the corre- molecules. Especially in recent years the short-range sponding transition dipole moments (TDMs), which PA, due to the merit of direct formation, continuous represent the strength of transition between the ini- accumulation and potential direct stimulated Raman tial and final states, and compare the values for the 3 adiabatic passage (STIRAP) transfer from scattering 2 Π0+ state. atomic states to deeply molecular states,[8;9] is veri- Many effective methods have been used to measure fied to be an interesting alternative pathway to pro- the TDM of atoms and molecules before, such as two- duce cold polar molecules in the lowest vibrational photon dark resonance spectroscopy,[19] electromag- ground state (v = 0).[10−17] Among these molecules, netically induced transparency,[20] and Autler–Townes 85Rb133Cs[13−16] (hereafter superscript will be omit- splitting.[21] All of these systems involve three or four ted) is particularly interesting due to several distinc- energy levels. Also, a number of samples are usually tive merits, including chemical stability, considerable needed to obtain a good signal-to-noise ratio (SNR). permanent electric dipole moment, and low cost. In However, the number of experimentally formed cold addition, the molecule product rate is also consid- molecules is ordinarily on the order of thousands or erable. However, the formed mechanism for RbCs even fewer, which will limit the SNR based on these molecules decays through a two-photon cascade decay, methods. Usually a rapid, sensitive photoionization which is different from a one-step spontaneous decay (PI) spectroscopy is used to detect the formed cold ∗Supported by the National Key Research and Development Program of China under Grant No 2017YFA0304203, the National Natural Science Foundation of China under Grant Nos 61675120 and 11434007, the National Natural Science Foundation of China for Excellent Research Team under Grant No 61121064, the Shanxi Scholarship Council of China, the 1331KSC, the PCSIRT under Grant No IRT13076, and the Applied Basic Research Project of Shanxi Province under Grant No 201601D202008. **Corresponding author. Email: [email protected] © 2018 Chinese Physical Society and IOP Publishing Ltd 103301-1 CHIN. PHYS. LETT. Vol. 35, No. 10 (2018) 103301 molecules with vibrational resolution. To realize the in the X1Σ + (v = 0, J = 1) ground level. (i) First rotational resolution of ground state molecules, a de- of all, the loading procedure (the duration time of pletion spectroscopy is firstly introduced by Wang et 90 ms) of dark-SPOTs and PA procedure occur si- [22] 3 al. and has been widely used in recent years. As the multaneously to produce the molecules in the 2 Π0− depletion laser couples molecules between the ground (v = 11, J = 0) level. The PA laser (typical state and excited states, it is also suitable to measure linewidth of 100 kHz, output power of 1.5 W, Gaus- the corresponding TDM between them. sian radius of 150 µm) is locked by a subtle transfer In this work, we measure the transition dipole mo- cavity technique.[26] (ii) At the same time with (i), ments for 85Rb133Cs molecules from the lowest vibra- the molecules are distributing in different vibrational tional state, X1Σ + (v = 0) to different excited states, ground states after the two-photon-cascade sponta- 3 0 1 0 1 + 2 Π0+ (v = 10) and 2 Π1 (v = 22). The former of neous emission process, including the X Σ (v = 0, the excited states can produce ground-state RbCs mo- J = 1) level. (iii) Then all the dark-SPOT lasers and elecules via two-photon cascade decay while the lat- PA laser are turned off. Meanwhile, the depletion laser 3 3 + ter has strong spin-orbit mixing with 2 Π1 and 3 Σ1 is turned on for several ms to couple the transition 1 + 3 0 states, and thus may have more strong one-step spon- from the X Σ (v = 0) state to the 2 Π0+ (v = 10), 1 0 taneous decay due to strong coupling with the ground or 2 Π1 (v = 22) state. The depletion laser frequency state. The corresponding TDM is derived by fitting (linewidth of 2 MHz, actual power of up to 10 mW) the dependence of depletion ratio on both power and can be controlled based on the same transfer cavity irradiated time of depletion laser to the classical ab- technique. To locate the accurate depletion laser fre- sorption formula for a two-level system. The TDM for quency, the rotational levels of two upper states are 1 0 2 Π1 (v = 22) with a factor of 5 larger than the value measured with the PA spectrum in advance, as shown 3 0 for 2 Π0+ (v = 10) is observed, verifying the much in Figs.1(b) and1(c). The spectral widths are fitted to stronger mixing with the ground state. be 17(2) MHz and 200(10) MHz by single-peak Lorentz Most details of the apparatus have been described and multi-peaks Lorentz formulas, respectively. The [23] [15;16] 1 0 before, such as in our recent and previous large width for the 2 Π1 (v = 22) state arises works. The starting point for this work is a mix- from the hyperfine structure.[18] (iv) The PI laser ture of laser cooled 85Rb and Cs atoms in space- (pulse energy of around 1 mJ, pulse duration of 7 ns, adjustable dark spontaneous force optical traps (dark- linewidth of 6 GHz, diameter of about 3 mm) with res- SPOTs).[24] Under a vacuum background pressure of onant transition between X1Σ + (v = 0) and 21Π around 3×10−7 Pa and a magnetic gradient of around (v = 12)[15] is used to photoionize the formed ground- 15 G/cm, we trap mixed atomic clouds with about state molecules through one color resonance-enhanced 7 85 [27] 1 × 10 Rb atoms in the 5S1=2 (F = 2) state with a two-photon ionization (RETPI). The photoionized density of 8 × 1010 cm−3, and about 2 × 107 133Cs molecular ions are then accelerated by a pulsed ac- atoms in the 6S1=2 (F = 3) state with a density celerating electric field and detected by a pair of mi- of 1 × 1011 cm−3. The translational temperature of cro channel plates (MCPs). The repetition rate is the mixed atoms is measured by time-of-flight (TOF) 10 Hz in our experiment. To obtain depletion spec- imaging to be around 100 µK.
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