Benjamin L. Augenbraun’s research while affiliated with MIT-Harvard Center for Ultracold Atoms and other places

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Publications (66)


Magneto-Optical Trapping of a Heavy Polyatomic Molecule for Precision Measurement
  • Article

February 2025

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22 Reads

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3 Citations

Physical Review Letters

Zack D. Lasner

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Hiromitsu Sawaoka

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[...]

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We report a magneto-optical trap of strontium monohydroxide (SrOH) containing 2000(600) molecules at a temperature of 1.2(3) mK. The lifetime is 91(9) ms, which is limited by decay to optically unaddressed vibrational states. This provides the foundation for future sub-Doppler cooling and optical trapping of SrOH, a polyatomic molecule suited for precision searches for physics beyond the standard model including new CP violating particles and ultralight dark matter. We also identify important features in this system that guide cooling and trapping of complex and heavy polyatomic molecules into the ultracold regime.



Magneto-optical trapping of a heavy polyatomic molecule for precision measurement

September 2024

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14 Reads

We report a magneto-optical trap of strontium monohydroxide (SrOH) containing 2000(600) molecules at a temperature of 1.2(3) mK. The lifetime is 91(9) ms, which is limited by decay to optically unaddressed vibrational states. This provides the foundation for future sub-Doppler cooling and optical trapping of SrOH, a polyatomic molecule suited for precision searches for physics beyond the Standard Model including new CP violating particles and ultralight dark matter. We also identify important features in this system that guide cooling and trapping of complex and heavy polyatomic molecules into the ultracold regime.


Optical Cycling and Sensitivity to the Electron's Electric Dipole Moment in Gold-Containing Molecules

July 2024

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8 Reads

We propose diatomic molecules built from gold and carbon-group atoms as promising candidates for optical cycling and precision measurements. We show that this class of molecules (AuX, X = C, Si, Ge, Sn, Pb) features laser-accessible electronic transitions with nearly diagonal Franck-Condon factors. The 2Π1/2^2\Pi_{1/2} ground states can be easily polarized in the laboratory frame and have near-zero magnetic moments, valuable features for quantum science and precision measurement applications. The sensitivities of AuX molecules to the electron electric dipole moment (EDM) are found to be favorable, with effective electric fields of 10-30 GV/cm. Together, these features imply that AuX molecules may enable significantly improved searches for time-reversal symmetry violation.



Figure 1: The polar orbitals in AcF and TlF (top) that make significant negative contributions to NSM sensitivity parameters and back-polarized Ac 7s orbital in AcF and Tl 6s orbital in TlF (bottom) that make positive contributions. Isosurfaces with an isovalue of 0.04 for the absolute value of the wave function are plotted. The red and blue colors represent opposite signs of the wave function values.
Figure 2: Back-polarized Th 7s orbital in the 1 Σ + states of ThO and ThF + . Isosurfaces with an isovalue of 0.04 for the absolute value of the wave function are plotted. The red and blue colors represent opposite signs of the wave function values.
Relativistic Exact Two-Component Coupled-Cluster Study of Molecular Sensitivity Factors for Nuclear Schiff Moments
  • Preprint
  • File available

July 2024

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98 Reads

Relativistic exact two-component coupled-cluster calculations of molecular sensitivity factors for nuclear Schiff moments (NSMs) are reported. We focus on molecules containing heavy nuclei, especially octupole-deformed nuclei. Analytic relativistic coupled-cluster gradient techniques are used and serve as useful tools for identifying candidate molecules that sensitively probe for physics beyond the Standard Model in the hadronic sector. Notably, these tools enable straightforward ``black-box'' calculations. Two competing chemical mechanisms that contribute to the NSM are analyzed, illuminating the physics of ligand effects on NSM sensitivity factors.

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Direct Laser Cooling of Polyatomic Molecules

February 2023

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214 Reads

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1 Citation

Over the past decade, tremendous progress has been made to extend the tools of laser cooling and trapping to molecules. Those same tools have recently been applied to polyatomic molecules (molecules containing three or more atoms). In this review, we discuss the scientific drive to bring larger molecules to ultralow temperatures, the features of molecular structure that provide the most promising molecules for this pursuit, and some technical aspects of how lasers can be used to control the motion and quantum states of polyatomic molecules. We also present opportunities for and challenges to the use of polyatomic molecules for science and technology.


Zeeman-Sisyphus deceleration for heavy molecules with perturbed excited-state structure

February 2023

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48 Reads

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8 Citations

Physical Review A

We demonstrate and characterize Zeeman-Sisyphus (ZS) deceleration of a beam of ytterbium monohydroxide. Our method uses a combination of large magnetic fields (∼2.5 T) and optical spin-flip transitions to decelerate molecules while scattering only ∼10 photons per molecule. We study the challenges associated with the presence of internal molecular perturbations among the excited electronic states and discuss the methods used to overcome these challenges, including a modified ZS decelerator using microwave and optical transitions.



Citations (30)


... Recently, researchers have identified ultracold molecules as powerful tools for all of these areas, spurring rapid growth in molecular cooling methods. Ultracold molecules have been produced by assembling ultracold atoms via magneto-association [9,10], photo-association [11][12][13], optoelectrical Sisyphus cooling [14], and by buffer gas cooling followed by direct laser cooling [15][16][17][18][19][20]. Quantum computation, quantum simulation and precision searches for physics beyond the Standard Model have been demonstrated, utilizing optical traps [21] and optical tweezer arrays of ultracold molecules [22][23][24][25]. ...

Reference:

Conveyor-belt magneto-optical trapping of molecules
Magneto-Optical Trapping of a Heavy Polyatomic Molecule for Precision Measurement
  • Citing Article
  • February 2025

Physical Review Letters

... At present, the Bureau International des Poids et Mesures recommends only two frequency standards in the mid-infrared, one at 3.39 µm based on CH 4 with a relative uncertainty of 3 × 10 −12 , and the other at 10.3 µm based on OsO 4 with an uncertainty of 1.4 × 10 −13 [35]. Recent advances in cooling and controlling neutral molecules [36,37] and molecular ions [38] raise the prospect of a set of new frequency standards in the mid-infrared, based on the vibrational frequencies of trapped molecules, whose precision could match that available in the microwave and optical domains (10 −16 or better). These frequency standards could then be used to calibrate large sets of spectral lines in common gases such as N 2 O. Suitable molecular clocks are currently being developed, motivated in part by their potential to search for varying fundamental constants [18,[39][40][41][42]. ...

Direct laser cooling of polyatomic molecules
  • Citing Chapter
  • January 2023

Advances in Atomic, Molecular, and Optical Physics

... Moreover, cryogenic cooling has already made it possible to demonstrate quantum control over molecular chirality 85 . Further developments in this area, such as the possible laser cooling of chiral molecules 86 , promise to open a path to finally detecting the long-anticipated energy difference between different enantiomers of a chiral molecule due to the EWI 87 . As the field of ultracold molecules continues to advance, further ideas for harnessing the rich quantum resources associated with molecular degrees of freedom are likely to emerge, making this a most exciting time for the field. ...

High Sensitivity Chiral Detection in the Gas Phase via Microwave Spectroscopy and the Possible Frontier of Ultracold Chiral Molecules
  • Citing Conference Paper
  • February 2023

... However, both methods require specific molecular structures, which limit the choice of molecules. Furthermore, laser cooling needs 10 4 −10 5 photon scattering events and thus demands high precision spectroscopy, which is challenging and time-consuming for many heavy-atom containing [29,30] or large polyatomic molecules [31,32]. ...

Direct Laser Cooling of Polyatomic Molecules

... As a result, there has been considerable experimental effort to bring molecules into the quantum toolbox. Diatomic molecules have been prepared in single quantum states and entangled [1][2][3][4][5][6][7][8]; polyatomic molecules are beginning to be explored with already some success in trapping and cooling [9][10][11][12][13][14][15][16][17][18]; and a number of laser-free quantum logic schemes have been proposed [19][20][21][22][23][24][25][26]. ...

Reference:

Æ codes
Zeeman-Sisyphus deceleration for heavy molecules with perturbed excited-state structure
  • Citing Article
  • February 2023

Physical Review A

... Polyatomic molecules, on the other hand, play crucial roles in the chemical and biological sciences and also exhibit numerous features advantageous for applications in physics. [18,19] For instance, they are of interest for improved searches for the electric dipole moment of the electron and other beyondstandard-model physics. [20] Chiral molecular ions offer possibilities for investigating parity violation, [21,22] while symmetric-top molecules with closely-spaced parity doublets present opportunities in the field of quantum simulation [23] and quantum information science. ...

Ultracold Polyatomic Molecules for Quantum Science and Precision Measurements
  • Citing Conference Paper
  • December 2022

... This suggests that even large molecules could potentially be laser-cooled if they possess optical cycling centers consisting of one metal atom and an attached entity. 79,[156][157][158] This means that the laser cooling technique for diatomic molecules can be extended to polyatomic molecules. However, polyatomic molecules have greater complexity and more degrees of freedom compared to diatomic molecules, which require a more complex control, and more repump lasers to form a quasicycling transition that is enough to capture the molecules. ...

Laser Spectroscopy of Aromatic Molecules with Optical Cycling Centers: Strontium(I) Phenoxides

The Journal of Physical Chemistry Letters

... Molecular optical cycling and direct laser cooling were first demonstrated for diatomic species, [29][30][31][32][33][34][35][36][37] and have now been extended to some triatomic [38][39][40] and a small polyatomic molecule CaOCH 3 [41]. Spectroscopic investigations of Ca-containing and Sr-containing phenoxides along with their derivatives via molecular functionalization, [42][43][44][45] have shown promise for optical cycling of much larger species with measured vibrational branching fractions of 0.84-0.99. Further, a variety of large polyatomic OCC systems have been proposed theoretically for these appli-cations, including alkaline-earth-metal-containing alkoxides [6][7][8]46], arenes [9,[47][48][49][50], fullerenes [51], diamondoids [46], and surfaces [27]. ...

High-Resolution Laser Spectroscopy of a Functionalized Aromatic Molecule
  • Citing Article
  • November 2022

The Journal of Physical Chemistry Letters

... Molecular optical cycling and direct laser cooling were first demonstrated for diatomic species, [29][30][31][32][33][34][35][36][37] and have now been extended to some triatomic [38][39][40] and a small polyatomic molecule CaOCH 3 [41]. Spectroscopic investigations of Ca-containing and Sr-containing phenoxides along with their derivatives via molecular functionalization, [42][43][44][45] have shown promise for optical cycling of much larger species with measured vibrational branching fractions of 0.84-0.99. Further, a variety of large polyatomic OCC systems have been proposed theoretically for these appli-cations, including alkaline-earth-metal-containing alkoxides [6][7][8]46], arenes [9,[47][48][49][50], fullerenes [51], diamondoids [46], and surfaces [27]. ...

Pathway toward Optical Cycling and Laser Cooling of Functionalized Arenes
  • Citing Article
  • July 2022

The Journal of Physical Chemistry Letters

... This is because molecular quantum coherence is particularly fragile to decoherence (or quantum noise) processes that arise due to the unavoidable and uncontrollable interactions of the molecules with their surrounding environment or bath. [7][8][9][10][11][12] In fact, electronic ( ∼10 fs) and vibrational (∼1000 fs) decoherence in molecules is typically remarkably fast. [12][13][14] To harness the potential of molecular qubits in QIS, it is important to identify robust molecular design principles to generate quantum subspaces with protected quantum coherence. ...

Functionalizing aromatic compounds with optical cycling centres

Nature Chemistry