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Motional Control of Polyatomic Molecules for Precision Measurement

Alexander Frenett

Published Jan 1, 2024• 0 citations
OpenAlex

Abstract

Extending AMO techniques of motional control to heavy polyatomic molecules opens new possibilities for precision measurements of fundamental physics. Though various laser-cooling and deceleration techniques have been applied to diatomic molecules throughout the last decade, their application to more complex molecules has heretofore been focused on light species, leaving generalizability to heavy species an open question. To investigate the high-mass frontier, we here study how to extend motional control to heavy-atom-containing polyatomic molecules. First, we discuss Zeeman-Sisyphus deceleration of YbOH, which can be used to decelerate species capable of scattering only ~10s of photons. Then, we discuss radiative slowing and magneto-optical trapping of SrOH, techniques only extendable to species capable of scattering $\sim10^4$ photons. The last work focuses on spectroscopy of nonlinear molecules to assess the viability of extending techniques of motional control to more complex species. We find a dependence of both rotational and vibrational control on symmetry group, and identify a next-generation candidate for laser cooling. We end with a overview tying these projects together, and assessing the future of motional control along mass and complexity axes, including brief suggestions of how complementary methods to those studied here can further expand into the frontiers of molecular control.

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Molecules controlled at the single-quantum-state level offer wide-ranging applications spanning many of the frontiers of modern physics. Within the past decade, simple diatomic molecules have been brought under full quantum control both via assembly from pre-cooled atoms and by direct laser cooling. Polyatomic molecules\footnote{Molecules that contain three or more atoms.} have attracted focus as novel quantum resources providing distinct advantages (and challenges) compared to both atoms and diatomic molecules. For example, nearly all polyatomic molecules have long-lived states that can be fully polarized at low applied electric fields. These and other features generic to polyatomic molecules can be applied to quantum simulation, quantum chemistry, and tests of fundamental physics beyond the Standard Model. While these structural features of polyatomic molecules are highly promising for applications, they complicate the process of bringing molecules under full quantum control. In this thesis, we describe a series of experimental and theoretical advances toward the production of ultracold complex polyatomic molecules. We demonstrate the first laser cooling of the polyatomic radical ytterbium monohydroxide (YbOH), a promising candidate to search for particles and interactions beyond the Standard Model of particle physics. We develop a novel deceleration technique (``Zeeman-Sisyphus deceleration") capable of slowing molecular beams to trappable velocities while scattering fewer than 10 optical photons. This deceleration method is demonstrated using CaOH molecules, a lighter analog of YbOH. In order to determine a viable pathway to full three-dimensional cooling and trapping of YbOH, we develop a spectroscopic technique to measure vibrational branching ratios with relative intensity sensitivity around 1 part in $10^5$, approximately two orders of magnitude beyond the previous state of the art. We also perform the first spectroscopic observations and characterizations of the related molecule ytterbium monomethoxide, YbOCH$_3$, a promising species to probe beyond-the-Standard-Model physics. In addition, we show theoretically that an entire class of asymmetric top molecules can be laser cooled using essentially the same techniques used for much simpler species. Measurements of the vibrational branching ratios for a few prototypical asymmetric to molecules (CaSH and CaNH$_2$) are presented to confirm these predictions.

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Ultracold polyatomic molecules containing heavy nuclei, such as SrOH and YbOH, are sensitive to T- symmetry violating and P-symmetry violating physics beyond the Standard Model through the electron’s electric dipole moment. Furthermore, SrOH is sensitive to ultralight Dark Matter through measuring time variations of fundamental constants. However, in order to make full use of these molecules, they need to be cooled to ultracold temperatures and held in optical traps. We have realized a magneto-optical trap (MOT) of SrOH and used this as the essential element to achieve optical trap- ping in the microKelvin temperature regime. We observed MOT lifetimes approaching 200 ms with temperatures ∼ 1 mK and observed damped oscillations in the MOT. We further cooled the SrOH molecules to ∼ 40 μ K using Λ-enhanced gray molasses, and compressed the cloud to about 100 μm size using the conveyor belt MOT technique. Using this ultracold dense cloud of SrOH, we loaded an optical dipole trap (ODT), with a molecular lifetime of 1.2(1) seconds. In separate experiments with YbOH, which is heavier than SrOH, we demonstrated a novel deceleration method (Zeeman- Sisyphus deceleration) that can slow YbOH to under 20 m/s with only a few photons scattered utilizing high magnetic fields up to 2.5 T. By driving spin-flip transitions at the maxima and minima of the magnetic fields, slowing was achieved, which is a critical first step toward loading of a MOT for this species. We addressed the challenges associated with driving spin-flip transitions in molecules that have molecular perturbations among the electronic excited states and developed an understanding of the physics of such systems that is applicable to a wide range of molecules.

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Polyatomic molecules, while ubiquitous in nature, were generally perceived as too complicated and "unruly" for the majority of quantum physics experiments. However, recent theoretical analyses have pinpointed the multiple advantages of using complex molecules for diverse applications such as the creation of a universal quantum computer, quantum simulation of non-trivial many-body states, and tests of fundamental physical laws. Throughout my dissertation research I focused on extending experimental techniques from atomic physics to complex molecules. The goal of my work was to not only demonstrate new ways to control molecules, but also develop a novel experimental platform for quantum science - complex polyatomic molecules - and provide tools for physicists to conquer new frontiers in physics and chemistry.\nThe main theme of this thesis is the use of laser radiation to control internal and external degrees of freedom for the triatomic radical strontium monohydroxide (SrOH). The research achievements presented here can be primarily divided into the following areas:\ni) out-of-equilibrium studies of vibrationally inelastic collisions at cryogenic temperatures,\nii) demonstration of the radiation pressure force and the direct laser cooling of polyatomic molecules, and\niii) the development of concepts for laser cooling of molecules with six and more atoms.\nFor the collisional studies, off-diagonal optical pumping was used to populate excited Sr-O stretching state and the ratio of elastic to vibrational quenching collisions was determined to be ~700. In the laser cooling work, using only laser light, the transverse temperature of the cryogenic buffer-gas beam of SrOH was reduced from 50 mK to below 1 mK, leading to an order of magnitude increase in phase space density of the molecular beam. Additionally, the prospects of using a coherent bichromatic force for optical deceleration of polyatomics were analyzed and experimentally characterized with the transverse deflection of the SrOH beam. Our experimental results with SrOH and theoretical analysis of more complex strontium alkoxides not only open a wide range of future directions for laser manipulation and trapping of polyatomic molecules but also help overturn long held assumptions about the difficulties of performing "traditional" atomic physics experiments with complex molecules.

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Polyatomic molecules as quantum sensors for fundamental physics

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Abstract Precision measurements in molecules have advanced rapidly in recent years through developments in techniques to cool, trap, and control. The complexity of molecules makes them a challenge to study, but also offers opportunities for enhanced sensitivity to many interesting effects. Polyatomic molecules offer additional complexity compared to diatomic molecules, yet are still ‘simple’ enough to be laser-cooled and controlled. While laser cooling molecules is still a research frontier itself, there are many proposed and ongoing experiments seeking to combine the advanced control enabled by ultracold temperatures with the intrinsic sensitivity of molecules. In this perspective, we discuss some applications where laser-cooled polyatomic molecules may offer advantages for precision measurements of fundamental physics, both within and beyond the Standard Model.

arXiv:2008.03398•Quantum Science and Technology•Sep 18, 2020•113 citations
Extending AMO techniques of motional control to heavy polyatomic molecules opens new possibilities for precision measurements of fundamental physics. Though various laser-cooling and deceleration techniques have been applied to diatomic molecules throughout the last decade, their application to more complex molecules has heretofore been focused on light species, leaving generalizability to heavy species an open question. To investigate the high-mass frontier, we here study how to extend motional control to heavy-atom-containing polyatomic molecules. First, we discuss Zeeman-Sisyphus deceleration of YbOH, which can be used to decelerate species capable of scattering only ~10s of photons. Then, we discuss radiative slowing and magneto-optical trapping of SrOH, techniques only extendable to species capable of scattering ∼104\sim10^4∼104 photons. The last work focuses on spectroscopy of nonlinear molecules to assess the viability of extending techniques of motional control to more complex species. We find a dependence of both rotational and vibrational control on symmetry group, and identify a next-generation candidate for laser cooling. We end with a overview tying these projects together, and assessing the future of motional control along mass and complexity axes, including brief suggestions of how complementary methods to those studied here can further expand into the frontiers of molecular control.
Molecules controlled at the single-quantum-state level offer wide-ranging applications spanning many of the frontiers of modern physics. Within the past decade, simple diatomic molecules have been brought under full quantum control both via assembly from pre-cooled atoms and by direct laser cooling. Polyatomic molecules\footnote{Molecules that contain three or more atoms.} have attracted focus as novel quantum resources providing distinct advantages (and challenges) compared to both atoms and diatomic molecules. For example, nearly all polyatomic molecules have long-lived states that can be fully polarized at low applied electric fields. These and other features generic to polyatomic molecules can be applied to quantum simulation, quantum chemistry, and tests of fundamental physics beyond the Standard Model. While these structural features of polyatomic molecules are highly promising for applications, they complicate the process of bringing molecules under full quantum control. In this thesis, we describe a series of experimental and theoretical advances toward the production of ultracold complex polyatomic molecules. We demonstrate the first laser cooling of the polyatomic radical ytterbium monohydroxide (YbOH), a promising candidate to search for particles and interactions beyond the Standard Model of particle physics. We develop a novel deceleration technique (``Zeeman-Sisyphus deceleration") capable of slowing molecular beams to trappable velocities while scattering fewer than 10 optical photons. This deceleration method is demonstrated using CaOH molecules, a lighter analog of YbOH. In order to determine a viable pathway to full three-dimensional cooling and trapping of YbOH, we develop a spectroscopic technique to measure vibrational branching ratios with relative intensity sensitivity around 1 part in 10510^5105, approximately two orders of magnitude beyond the previous state of the art. We also perform the first spectroscopic observations and characterizations of the related molecule ytterbium monomethoxide, YbOCH3_33​, a promising species to probe beyond-the-Standard-Model physics. In addition, we show theoretically that an entire class of asymmetric top molecules can be laser cooled using essentially the same techniques used for much simpler species. Measurements of the vibrational branching ratios for a few prototypical asymmetric to molecules (CaSH and CaNH2_22​) are presented to confirm these predictions.
Ultracold polyatomic molecules containing heavy nuclei, such as SrOH and YbOH, are sensitive to T- symmetry violating and P-symmetry violating physics beyond the Standard Model through the electron’s electric dipole moment. Furthermore, SrOH is sensitive to ultralight Dark Matter through measuring time variations of fundamental constants. However, in order to make full use of these molecules, they need to be cooled to ultracold temperatures and held in optical traps. We have realized a magneto-optical trap (MOT) of SrOH and used this as the essential element to achieve optical trap- ping in the microKelvin temperature regime. We observed MOT lifetimes approaching 200 ms with temperatures ∼ 1 mK and observed damped oscillations in the MOT. We further cooled the SrOH molecules to ∼ 40 μ K using Λ-enhanced gray molasses, and compressed the cloud to about 100 μm size using the conveyor belt MOT technique. Using this ultracold dense cloud of SrOH, we loaded an optical dipole trap (ODT), with a molecular lifetime of 1.2(1) seconds. In separate experiments with YbOH, which is heavier than SrOH, we demonstrated a novel deceleration method (Zeeman- Sisyphus deceleration) that can slow YbOH to under 20 m/s with only a few photons scattered utilizing high magnetic fields up to 2.5 T. By driving spin-flip transitions at the maxima and minima of the magnetic fields, slowing was achieved, which is a critical first step toward loading of a MOT for this species. We addressed the challenges associated with driving spin-flip transitions in molecules that have molecular perturbations among the electronic excited states and developed an understanding of the physics of such systems that is applicable to a wide range of molecules.
The rich internal structure of polyatomic molecules has inspired a number of theoretical proposals exploring a myriad of unique scientific and engineering frontiers, including quantum simulation and next-generation searches for physics beyond the standard model. Establishing full control over these complex quantum objects is likely necessary to harness their full potential; however, the same rich internal structure that gives rise to the immense scientific potential of polyatomic molecules also makes manipulating them a daunting task. In the past decade there has been considerable progress in the production, cooling, and control of diatomic species using direct laser cooling and magneto-optical trapping. This dissertation focuses on extending direct laser cooling and trapping to polyatomic molecules. Direct laser cooling of triatomic radical calcium monohydroxide (CaOH) is demonstrated. This molecules is a prototypical example of a broad class of polyatomic molecules that includes symmetric and asymmetric tops. Transverse magneto-optical trapping is demonstrated, establishing the ability to scatter an unprecedented number of photons in a polyatomic species. An understanding of previously unappreciated intricacies of molecular structure is developed, that explains observations of novel vibrational decay pathways. High resolution spectroscopy of hybrid vibrational modes is performed. A laser cooling scheme is constructed that will support future efforts to use the full range of laser cooling and high-fidelity detection techniques required to implement an optical tweezer array of polyatomic molecules. Our experimental efforts demonstrate the feasibility of direct laser cooling applied to CaOH, up ending long-standing assumptions of the inextricable complexity of polyatomic molecules.
Abstract Recently, a few diatomic and polyatomic molecules have been identified as prospective systems for Doppler/Sisyphus cooling. Doppler/Sisyphus cooling allows us to decrease the kinetic energy of molecules down to μ K temperatures with high efficiency and allows their capture in molecular traps, including magneto-optical traps. Trapped molecules can be used for creating molecular fountains and/or performing controlled chemical reactions, high-precision spectra measurements, and a wealth of other applications. Polyatomic molecules with heavy nuclei are of considerable interest for the ‘new physics’ search outside of the Standard Model and other applications including cold chemistry and photochemistry, quantum informatics, etc. Here, we focus on the radium monohydroxide molecule (RaOH), which is on the one hand amenable to laser cooling and on the other hand opens excellent possibilities for  -odd and  ,  -odd effects research. At present, RaOH is the heaviest polyatomic molecule proposed for direct cooling with lasers.
Polyatomic molecules, while ubiquitous in nature, were generally perceived as too complicated and "unruly" for the majority of quantum physics experiments. However, recent theoretical analyses have pinpointed the multiple advantages of using complex molecules for diverse applications such as the creation of a universal quantum computer, quantum simulation of non-trivial many-body states, and tests of fundamental physical laws. Throughout my dissertation research I focused on extending experimental techniques from atomic physics to complex molecules. The goal of my work was to not only demonstrate new ways to control molecules, but also develop a novel experimental platform for quantum science - complex polyatomic molecules - and provide tools for physicists to conquer new frontiers in physics and chemistry.\nThe main theme of this thesis is the use of laser radiation to control internal and external degrees of freedom for the triatomic radical strontium monohydroxide (SrOH). The research achievements presented here can be primarily divided into the following areas:\ni) out-of-equilibrium studies of vibrationally inelastic collisions at cryogenic temperatures,\nii) demonstration of the radiation pressure force and the direct laser cooling of polyatomic molecules, and\niii) the development of concepts for laser cooling of molecules with six and more atoms.\nFor the collisional studies, off-diagonal optical pumping was used to populate excited Sr-O stretching state and the ratio of elastic to vibrational quenching collisions was determined to be ~700. In the laser cooling work, using only laser light, the transverse temperature of the cryogenic buffer-gas beam of SrOH was reduced from 50 mK to below 1 mK, leading to an order of magnitude increase in phase space density of the molecular beam. Additionally, the prospects of using a coherent bichromatic force for optical deceleration of polyatomics were analyzed and experimentally characterized with the transverse deflection of the SrOH beam. Our experimental results with SrOH and theoretical analysis of more complex strontium alkoxides not only open a wide range of future directions for laser manipulation and trapping of polyatomic molecules but also help overturn long held assumptions about the difficulties of performing "traditional" atomic physics experiments with complex molecules.
Abstract Precision measurements in molecules have advanced rapidly in recent years through developments in techniques to cool, trap, and control. The complexity of molecules makes them a challenge to study, but also offers opportunities for enhanced sensitivity to many interesting effects. Polyatomic molecules offer additional complexity compared to diatomic molecules, yet are still ‘simple’ enough to be laser-cooled and controlled. While laser cooling molecules is still a research frontier itself, there are many proposed and ongoing experiments seeking to combine the advanced control enabled by ultracold temperatures with the intrinsic sensitivity of molecules. In this perspective, we discuss some applications where laser-cooled polyatomic molecules may offer advantages for precision measurements of fundamental physics, both within and beyond the Standard Model.