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arXiv:1911.07195 · Physical Chemistry Chemical Physics

Microwave-assisted coherent control of ultracold polar molecules in a ladder-type configuration of rotational states

Ting Gong, Zhonghua Ji, Jiaqi Du, Yanting Zhao, Liantuan Xiao, Suotang Jia

Published Jan 1, 2021• 1 citation
arXivHTMLPDF

Abstract

We demonstrate microwave-assisted coherent control of ultracold 85Rb133Cs molecules in a ladder-type configuration of rotational states. Specifically, we use a probe and a control MW field to address the transitions between the J = 1 → 2 and J = 2 → 3 rotational states of the X1Σ+(v = 0) vibrational level, respectively, and use the control field to modify the response of the probe MW transition by coherently reducing the population of the intermediate J = 2 state. We observe that an increased Rabi frequency of the control field leads to broadening of the probe spectrum splitting and a shift of the central frequency. We apply Akaike's information criterion (AIC) to conclude that the observed coherent spectral response appears across the crossover regime between electromagnetically induced transparency and Aulter-Townes splitting. Our work is a significant development in microwave-assisted quantum control of ultracold polar molecules with multilevel configuration.

DOI
10.1039/d1cp00202c

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•Jan 1, 2018•0 citations
We demonstrate microwave-assisted coherent control of ultracold 85Rb133Cs molecules in a ladder-type configuration of rotational states. Specifically, we use a probe and a control MW field to address the transitions between the J = 1 → 2 and J = 2 → 3 rotational states of the X1Σ+(v = 0) vibrational level, respectively, and use the control field to modify the response of the probe MW transition by coherently reducing the population of the intermediate J = 2 state. We observe that an increased Rabi frequency of the control field leads to broadening of the probe spectrum splitting and a shift of the central frequency. We apply Akaike's information criterion (AIC) to conclude that the observed coherent spectral response appears across the crossover regime between electromagnetically induced transparency and Aulter-Townes splitting. Our work is a significant development in microwave-assisted quantum control of ultracold polar molecules with multilevel configuration.
We report an experimental demonstration of microwave-assisted coherent control of ultracold 85^{85}85Rb133^{133}133Cs molecules in a ladder-type configuration of rotational-state double resonances, following an observation of Rabi oscillations of the related neighbouring rotational states. The population of middle rotational states, which is coupled with a probe microwave (MW) field, can be reduced by a control MW field. Broadening of spectral splitting and shift of central frequency are observed and both are attributed to the control MW field. Applying Akaike's information criterion, we conclude that our observed coherent spectra happen near the crossover range of electromagnetically induced transparency and Aulter-Townes splitting. Our work is a significant development in microwave-assisted quantum control of ultracold polar molecules with multilevel configuration, and also offers a great potential in quantum information based on ultracold molecules.
We explore coherent multi-photon processes in 87Rb133Cs 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 configuration, we show that we can generate and coherently populate microwave dressed states via the observation of an Autler-Townes doublet. We demonstrate that we can control the strength of this dressing by varying the intensity of the microwave coupling field. Finally, we perform spectroscopy of the rotational states of 87Rb133Cs up to N = 6, highlighting the potential of ultracold molecules for quantum simulation in synthetic dimensions. By fitting the measured transition frequencies we determine a new value of the centrifugal distortion coefficient Dv = h × 207.3(2) Hz.
Microwave (MW) fields with strong field strength, ultralow phase-noise, and tunable polarization are crucial for stabilizing and manipulating ultracold polar molecules, which have emerged as a promising platform for quantum science. In this article, we present the design, characterization, and performance of a robust MW setup tailored for precise control of molecular states. This setup achieves a high electric field intensity of 6.9 kV/m in the near-field from a dual-feed waveguide antenna, enabling a Rabi frequency as high as 71 MHz for the rotational transition of sodium-potassium molecules. In addition, the low noise signal source and controlled electronics provide ultralow phase-noise and dynamically tunable polarization. Narrowband filters within the MW circuitry further reduce phase noise by more than 20 dB at 20 MHz offset frequency, ensuring prolonged one-body molecular lifetimes up to 10 s. We also show practical methods to measure the MW field strength and polarization using a simple homemade dipole probe and to characterize phase-noise down to -170 dBc/Hz using a commercial spectrum analyzer and a notch filter. Those capabilities allowed us to evaporatively cool our molecular sample to deep quantum degeneracy. Furthermore, the polarization tunability enabled the observation of field-linked resonances and facilitated the creation of field-linked tetramers. These techniques advance the study of ultracold polar molecules and broaden the potential applications of MW tools in other platforms of quantum science.
We analyze the temporal evolution of the population of ultracold polar molecules in a microwave (mw) field with a circular polarization. The molecules are in their ground state and treated as rigid rotors with a permanent dipole moment which interact with each other via the dipole–dipole (DD) interaction V dd . The mw field mixes states with different quantum and photon numbers and the collisional dynamics in the mw field is mostly controlled by the ratios of the mw field frequency versus the rotational constant, and mw field Rabi frequency versus the rotational constant. There exists a special scattering process which is elastic by nature and due to a rotational energy exchange between the ground and the first excited rotational states. To analyze dynamics of polar molecules system in the mw field the equation of motion for the bare and dressed states is solved under different mw field parameters and molecular gas characteristics. Depending on the ratio of the Rabi frequency of a mw field and the magnitude of the DD interaction, beatings and oscillations occur in the bare and dressed states time-development. At a certain relation between the magnitudes of the mw detuning δ and the DD interaction , peak structures appear in the population of the excited bare state. Each peak is associated with an avoided crossing between the dressed states adiabatic curves at the same position of mw detuning.
We demonstrate coherent control of the rotational and hyperfine state of ultracold, chemically stable 87Rb133Cs^{87}\mathrm{Rb}^{133}\mathrm{Cs}87Rb133Cs molecules with external microwave fields. We create a sample of $\ensuremath{\sim}2000$ molecules in the lowest hyperfine level of the rovibronic ground state N=0N=0N=0. We measure the transition frequencies to eight different hyperfine levels of the N=1N=1N=1 state at two magnetic fields $\ensuremath{\sim}23$ G apart. We determine accurate values of rotational and hyperfine coupling constants that agree well with previous calculations. We observe Rabi oscillations on each transition, allowing complete population transfer to a selected hyperfine level of N=1N=1N=1. Subsequent application of a second microwave pulse allows the transfer of molecules back to a different hyperfine level of N=0N=0N=0.
This thesis presents the development of a toolbox for the coherent control of ultracold polar molecules. Such systems of molecules promise the creation of long-lived, highly dipolar quantum gases with applications spanning the fields of quantum state controlled chemistry, quantum information, quantum simulation, and precision measurement. However, the addition of vibrational and rotational degrees of freedom leads to molecular systems being significantly more complex than their widely used atomic counterparts. In this work we demonstrate full control of the quantum state down to the hyperfine level of an optically trapped sample of ultracold bosonic 87Rb133 Cs molecules, and exploit that control to begin an investigation into the collision processes which take place in an ultracold molecular gas. We create a sample of up to ∼ 4000 optically trapped molecules in their rovibronic and hyperfine ground state. We characterise the molecules by measuring their temperature, binding energy, and molecule-frame electric dipole moment. We perform spectroscopy of the first rotationally excited state with hyperfine state resolution using microwaves to determine accurate values of rotational and hyperfine coupling constants. We use coherent π pulses to perform complete transfer population between selected hyperfine levels of the ground, first-excited, and second-excited rotational states. We investigate the effect of the off-resonant light of our optical dipole trap on the rotational and hyperfine structure of the molecules. Through a combination of high-resolution microwave spectroscopy and parametric heating measurements, we characterise the polarisability of the 87Rb133Cs molecule. We demonstrate that coupling between neighbouring hyperfine states manifests in rich structure with many avoided crossings in any rotational state other than the ground state. This coupling may be tuned by rotating the polarisation of the linearly polarised trapping light. Finally, we study the lifetime of polar bosonic 87Rb133Cs molecules in our 3D optical dipole trap. We examine the lifetime of the molecules as a function of dipole trap intensity, magnetic field, and hyperfine and rotational state. Despite the chemical stability of the 87Rb133 Cs molecule, we observe lifetimes of ∼1 s corresponding to 2-body decay rates close to the universal limit.