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arXiv:2111.03763 · Journal of Molecular Spectroscopy

Photon spin molasses for laser cooling molecular rotation

Wesley C. Campbell, Benjamin L. Augenbraun

Published Feb 26, 2022• 2 citations
arXivHTMLPDF

Abstract

Laser cooling of translational motion of small molecules is performed by addressing transitions that ensure spontaneous emission cannot cause net rotational excitation. This will not be possible once the rotational splitting becomes comparable to the operational excitation linewidth, as will occur for large molecules or wide bandwidth lasers. We show theoretically that in this regime, angular momentum transfer from red-detuned Doppler cooling light can also exert a damping torque on linear molecules, cooling rotation to the same Doppler limit (typically ≈500μK for molecules with ≈10ns excited-state lifetimes). This cooling process is derived from photon spin, and indicates that standard optical molasses can also cool molecular rotation with no additional experimental resources.

DOI
10.1016/j.jms.2022.111596

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Laser cooling of translational motion of small molecules is performed by addressing transitions that ensure spontaneous emission cannot cause net rotational excitation. This will not be possible once the rotational splitting becomes comparable to the operational excitation linewidth, as will occur for large molecules or wide bandwidth lasers. We show theoretically that in this regime, angular momentum transfer from red-detuned Doppler cooling light can also exert a damping torque on linear molecules, cooling rotation to the same Doppler limit (typically ≈500μK for molecules with ≈10ns excited-state lifetimes). This cooling process is derived from photon spin, and indicates that standard optical molasses can also cool molecular rotation with no additional experimental resources.
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We present a simple and general optical cooling method based on 3D degenerate Raman sideband cooling with adiabatic release that goes significantly beyond the density and temperature limitations of optical molasses. In 10 ms we cool a sample of 3×108 cesium atoms to a temperature of 330 nK at a density of 1.1×1011 cm−3, which corresponds to a phase-space density nλdB3=1/500.We further propose to cool atoms or molecules inside an optical cavity that enhances the scattering of blue-detuned photons and show that the dissipative mechanism can be viewed as a cavity-induced generalized Doppler cooling. Since the cooling depends on the atom’s internal level structure only through the photon scattering rate, cavity Doppler cooling is applicable to particles that do not possess a closed optical transition, which may allow one to extend laser cooling to a greater class of atoms or molecules. Large samples are cooled at the same rate as single atoms if the effect of one atom on the cavity resonance frequency is small. We also show how to achieve 3D cooling with a single optical cavity.
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Laser cooling to sub-Doppler temperatures by optical molasses is thought to be inhibited in atoms with unresolved, near-degenerate hyperfine structure in the excited state. We demonstrate that such cooling is possible in one to three dimensions, not only near the standard D2{D}_{2}D2​ line for laser cooling, but over a wide range extending to the D1{D}_{1}D1​ line. Via a combination of Sisyphus cooling followed by adiabatic expansion, we reach temperatures as low as 40 $\ensuremath{\mu}$K, which corresponds to atomic velocities a factor of 2.6 above the limit imposed by a single-photon recoil. Our method requires modest laser power at a frequency within reach of standard frequency-locking methods. It is largely insensitive to laser power, polarization and detuning, magnetic fields, and initial hyperfine populations. Our results suggest that optical molasses should be possible with all alkali-metal species.
Working with MgH+molecular ions in a linear Paul trap, we routinely cool their translational degrees of freedom by sympathetic cooling with Doppler laser cooled Mg+ions. Giving the time for the molecules to equilibrate internally to room temperature blackbody radiation, the vibrational degree of freedom is frozen out, leaving only the rotational degree of freedom to be cooled. We have implemented a new technique for laser-induced rotational ground-state cooling of vibrationally and translationally cold MgH+ions, using a scheme based on excitation of a single rovibrational transition. This technique is generalizable to any diatomic polar molecular ion, given an appropriate mid-infrared laser source such as a quantum cascade laser.