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1. Characterizing the fundamental bending vibration of a linear polyatomic molecule for symmetry violation searches

   https://doi.org/10.1088/1367-2630/ace471  

   Jadbabaie, Arian ; Takahashi, Yuiki ; Pilgram, Nickolas H ; Conn, Chandler J ; Zeng, Yi ; Zhang, Chi ; Hutzler, Nicholas R ( July 2023 , New Journal of Physics)

   Polyatomic molecules have been identified as sensitive probes of charge-parity violating and parity violating physics beyond the Standard Model (BSM). For example, many linear triatomic molecules are both laser-coolable and have parity doublets in the ground electronic$\tilde{X}{}^2{\mathrm{\Sigma }}^{+}(010)$state arising from the bending vibration, both features that can greatly aid BSM searches. Understanding the$\tilde{X}{}^2{\mathrm{\Sigma }}^{+}(010)$state is a crucial prerequisite to precision measurements with linear polyatomic molecules. Here, we characterize the fundamental bending vibration of${}^{174}$YbOH using high-resolution optical spectroscopy on the nominally forbidden$\tilde{X}{}^2{\mathrm{\Sigma }}^{+}(010)$$\to \tilde{A}{}^2{\mathrm{\Pi }}_{1/2}(000)$transition at 588 nm. We assign 39 transitions originating from the lowest rotational levels of the$\tilde{X}{}^2{\mathrm{\Sigma }}^{+}(010)$state, and accurately model the state’s structure with an effective Hamiltonian using best-fit parameters. Additionally, we perform Stark and Zeeman spectroscopy on the$\tilde{X}{}^2{\mathrm{\Sigma }}^{+}(010)$state and fit the molecule-frame dipole moment to$D_{\mathrm{m}\mathrm{o}\mathrm{l}}=2.16(1)$Dand the effective electrong-factor to$g_S=2.07(2)$. Further, we use an empirical model to explain observed anomalous line intensities in terms of interference from spin–orbit and vibronic perturbations in the excited$\tilde{A}{}^2{\mathrm{\Pi }}_{1/2}(000)$state. Our work is an essential step toward searches for BSM physics in YbOH and other linear polyatomic molecules.

    

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2. Electrostatic focusing of cold and heavy molecules for the ACME electron EDM search

   https://doi.org/10.1088/1367-2630/ac8014  

   Wu, X. ; Hu, P. ; Han, Z. ; Ang, D. G. ; Meisenhelder, C. ; Gabrielse, G. ; Doyle, J. M. ; DeMille, D. ( August 2022 , New Journal of Physics)

   The current best upper limit for electron electric dipole moment (EDM), |d_e| < 1.1 × 10⁻²⁹e cm (90% confidence), was set by the ACME Collaboration in 2018. The ACME experiment uses a spin-precession measurement in a cold beam of thorium monoxide (ThO) molecules to detectd_e. An improvement in statistical uncertainty would be possible with more efficient use of molecules from the cryogenic buffer gas beam source. Here, we demonstrate electrostatic focusing of the ThO beam with a hexapole lens. This results in a factor of 16 enhancement in the molecular flux detectable downstream, in a beamline similar to that built for the next generation of ACME. We also demonstrate an upgraded rotational cooling scheme that increases the ground state population by 3.5 times compared to no cooling, consistent with expectations and a factor of 1.4 larger than previously in ACME. When combined with other demonstrated improvements, we project over an order of magnitude improvement in statistical sensitivity for the next generation ACME electron EDM search.

    

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3. Tuning the H‐Atom Transfer Reactivity of Iron(IV)‐Oxo Complexes as Probed by Infrared Photodissociation Spectroscopy

   https://doi.org/10.1002/ange.202016695  

   Tripodi, Guilherme L. ; Dekker, Magda M. J. ; Roithová, Jana ; Que, Jr., Lawrence ( February 2021 , Angewandte Chemie)

   Reactivities of non‐heme iron(IV)‐oxo complexes are mostly controlled by the ligands. Complexes with tetradentate ligands such as [(TPA)FeO]²⁺(TPA=tris(2‐pyridylmethyl)amine) belong to the most reactive ones. Here, we show a fine‐tuning of the reactivity of [(TPA)FeO]²⁺by an additional ligand X (X=CH₃CN, CF₃SO₃⁻, ArI, and ArIO; ArI=2‐(^tBuSO₂)C₆H₄I) attached in solution and reveal a thus far unknown role of the ArIO oxidant. The HAT reactivity of [(TPA)FeO(X)]^+/2+decreases in the order of X: ArIO > MeCN > ArI ≈ TfO⁻. Hence, ArIO is not just a mere oxidant of the iron(II) complex, but it can also increase the reactivity of the iron(IV)‐oxo complex as a labile ligand. The detected HAT reactivities of the [(TPA)FeO(X)]^+/2+complexes correlate with the Fe=O and FeO−H stretching vibrations of the reactants and the respective products as determined by infrared photodissociation spectroscopy. Hence, the most reactive [(TPA)FeO(ArIO)]²⁺adduct in the series has the weakest Fe=O bond and forms the strongest FeO−H bond in the HAT reaction.

    

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4. Tuning the H‐Atom Transfer Reactivity of Iron(IV)‐Oxo Complexes as Probed by Infrared Photodissociation Spectroscopy

   https://doi.org/10.1002/anie.202016695  

   Tripodi, Guilherme L. ; Dekker, Magda M. J. ; Roithová, Jana ; Que, Jr., Lawrence ( February 2021 , Angewandte Chemie International Edition)

   Reactivities of non‐heme iron(IV)‐oxo complexes are mostly controlled by the ligands. Complexes with tetradentate ligands such as [(TPA)FeO]²⁺(TPA=tris(2‐pyridylmethyl)amine) belong to the most reactive ones. Here, we show a fine‐tuning of the reactivity of [(TPA)FeO]²⁺by an additional ligand X (X=CH₃CN, CF₃SO₃⁻, ArI, and ArIO; ArI=2‐(^tBuSO₂)C₆H₄I) attached in solution and reveal a thus far unknown role of the ArIO oxidant. The HAT reactivity of [(TPA)FeO(X)]^+/2+decreases in the order of X: ArIO > MeCN > ArI ≈ TfO⁻. Hence, ArIO is not just a mere oxidant of the iron(II) complex, but it can also increase the reactivity of the iron(IV)‐oxo complex as a labile ligand. The detected HAT reactivities of the [(TPA)FeO(X)]^+/2+complexes correlate with the Fe=O and FeO−H stretching vibrations of the reactants and the respective products as determined by infrared photodissociation spectroscopy. Hence, the most reactive [(TPA)FeO(ArIO)]²⁺adduct in the series has the weakest Fe=O bond and forms the strongest FeO−H bond in the HAT reaction.

    

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5. Calibration of the Solid‐State Nuclear Magnetic Resonance Search for Axion‐Like Dark Matter

   https://doi.org/10.1002/andp.202300252  

   Winter, Andrew J. ; Marić, Tanja ; Balabanova, Viktoriya A. ; Ádám, János ; Randall, Glenn ; Wickenbrock, Arne ; Jackson Kimball, Derek F. ; Budker, Dmitry ; Sushkov, Alexander O. ( November 2023 , Annalen der Physik)

   Calibration of nuclear‐magnetic‐resonance‐based searches for axion‐like dark matter can be performed by free induction decay (FID) measurements. This manu‐ script describes FID experiments on several solid materials, motivated by the Cosmic Axion Spin Precession Experiment (CASPEr) program. Experiments with²⁰⁷Pb nuclear spins in ferroelectrics, lead magnesium niobate‐lead titanate (PbMg_1/3Nb_2/3O₃) (PbTiO₃)_1/3(PMN‐PT) and lead zirconium titante PbZr_0.52Ti_0.48O₃(PZT) are directly relevant to the CASPEr‐electric search for the electric dipole moment interaction of axion‐like dark matter. Experiments with³¹P nuclear spins in gadolinium‐doped hydroxypyromorphite Pb_4.95Gd_0.05(PO₄)₃OH (HPM:Gd) are used for apparatus calibration. The measurements characterized the nuclear spin ensemble coherence time and the magnetic resonance detection sensitivity for these samples. Calibration is performed using small tip‐angle pulses.

    

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