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arXiv:2009.01944 · Physical Chemistry Chemical Physics

Coherent manipulation of the internal state of ultracold 87 Rb 133 Cs molecules with multiple microwave fields

Jacob A. Blackmore, Philip D. Gregory, Sarah Bromley, Simon L. Cornish

Published Jan 1, 2020• 19 citations
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Abstract

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.

DOI
10.1039/d0cp04651e

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arXiv:1911.07195•Physical Chemistry Chemical Physics•Jan 1, 2021•1 citation
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.
Coherence and Collisions in Ultracold 87^{87}87Rb133^{133}133Cs Molecules
This thesis presents work towards the development of a quantum simulator based on 87^{87}87Rb133^{133}133Cs molecules using a bulk sample of up to ~4000 molecules at temperatures of ~1 µK. We demonstrate coherent control over the molecules' internal state using resonant microwave fields. We test this coherence by performing high resolution Ramsey spectroscopy of the first rotational transition and observing how the contrast of the spectroscopic fringes decay. We are able to affect the coherence of the superposition using an external laser field, as the two component states have a significant differential AC Stark shift. We extend this microwave control by including an additional microwave field, demonstrating the Autler-Townes effect with hyperfine state resolution and transfer between two hyperfine states in N=0N=0N=0. We study the internal structure of the molecule in the presence of external fields focussing on controlling the differential AC Stark shift between the rotational ground state and the first excited state. We investigate the effect of the off-resonant light on the internal structure in static magnetic and electric fields. In the DC electric field we use two models to describe the molecular structure, demonstrating that at modest values of the electric field the nuclear spin angular momentum is decoupled from the rotational angular momentum of the molecule, this enables us to construct a set of optimum trapping parameters for states with MN=0M_N=0MN​=0. Through careful measurements of the molecular lifetime we are able to determine that molecular losses are limited by two-body collisions. By introducing a time dependent intensity modulation to our optical trap we are further able to determine that the dominant loss process in bulk samples of ultracold 87^{87}87Rb133^{133}133Cs molecules is the laser excitation of collision complexes. Finally, we investigate the collisional properties of 87^{87}87Rb133^{133}133Cs with 87^{87}87Rb and 133^{133}133Cs atoms. We find that the loss is caused by single molecule-single atom collisions and sub-universal over a wide range of magnetic fields.
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.
Polar molecules offer a new platform for quantum simulation of systems with long-range interactions, based on the electrostatic interaction between their electric dipole moments. Here, we report the development of coherent quantum state control using microwave fields in 40 Ca 19 F and 87 Rb 133 Cs molecules, a crucial ingredient for many quantum simulation applications. We perform Ramsey interferometry measurements with fringe spacings of ∼1 kHz and investigate the dephasing time of a superposition of N = 0 and N = 1 rotational states when the molecules are confined. For both molecules, we show that a judicious choice of molecular hyperfine states minimises the impact of spatially varying transition-frequency shifts across the trap. For magnetically trapped 40 Ca 19 F we use a magnetically insensitive transition and observe a coherence time of 0.61(3) ms. For optically trapped 87 Rb 133 Cs we exploit an avoided crossing in the AC Stark shifts and observe a maximum coherence time of 0.75(6) ms.
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 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.