Enhanced molecular yield from a cryogenic buffer gas beam source via excited state chemistry

We use narrow-band laser excitation of Yb atoms to substantially enhance the brightness of a cold beam of YbOH, a polyatomic molecule with high sensitivity to physics beyond the standard model (BSM). By exciting atomic Yb to the metastable ³P₁ state in a cryogenic environment, we significantly increase the chemical reaction cross-section for collisions of Yb with reactants. We characterize the dependence of the enhancement on the properties of the laser light, and study the final state distribution of the YbOH products. The resulting bright, cold YbOH beam can be used to increase the statistical sensitivity in searches for new physics utilizing YbOH, such as electron electric dipole moment and nuclear magnetic quadrupole moment experiments. We also perform new quantum chemical calculations that confirm the enhanced reactivity observed in our experiment and compare reaction pathways of Yb(³P) with the reactants H₂O and H₂O₂. More generally, our work presents a broad approach for improving experiments that use cryogenic molecular beams for laser cooling and precision measurement searches of BSM physics

Quantum-Enhanced Metrology for Molecular Symmetry Violation using Decoherence-Free Subspaces

We propose a method to measure time-reversal symmetry violation in molecules that overcomes the standard quantum limit while leveraging decoherence-free subspaces to mitigate sensitivity to classical noise. The protocol does not require an external electric field, and the entangled states have no first-order sensitivity to static electromagnetic fields as they involve superpositions with zero average lab-frame projection of spins and dipoles. This protocol can be applied with trapped neutral or ionic species, and can be implemented using methods which have been demonstrated experimentally.Comment: 7+11 pages, 3+3 figure

Direct measurement of high-lying vibrational repumping transitions for molecular laser cooling

Molecular laser cooling and trapping requires addressing all spontaneous decays to excited vibrational states that occur at the $\gtrsim 10^{-4} - 10^{-5}$ level, which is accomplished by driving repumping transitions out of these states. However, the transitions must first be identified spectroscopically at high-resolution. A typical approach is to prepare molecules in excited vibrational states via optical cycling and pumping, which requires multiple high-power lasers. Here, we demonstrate a general method to perform this spectroscopy without the need for optical cycling. We produce molecules in excited vibrational states by using optically-driven chemical reactions in a cryogenic buffer gas cell, and implement frequency-modulated absorption to perform direct, sensitive, high-resolution spectroscopy. We demonstrate this technique by measuring the spectrum of the $\tilde{A}^2\Pi_{1/2}(1,0,0)-\tilde{X}^2\Sigma^+(3,0,0)$ band in $^{174}$YbOH. We identify the specific vibrational repump transitions needed for photon cycling, and combine our data with previous measurements of the $\tilde{A}^2\Pi_{1/2}(1,0,0)-\tilde{X}^2\Sigma^+(0,0,0)$ band to determine all of the relevant spectral constants of the $\tilde{X}^2\Sigma^+(3,0,0)$ state. This technique achieves high signal-to-noise, can be further improved to measure increasingly high-lying vibrational states, and is applicable to other molecular species favorable for laser cooling.Comment: 14 pages, 5 figure

Enhanced molecular yield from a cryogenic buffer gas beam source via excited state chemistry

We use narrow-band laser excitation of Yb atoms to substantially enhance the brightness of a cold beam of YbOH, a polyatomic molecule with high sensitivity to physics beyond the standard model (BSM). By exciting atomic Yb to the metastable ³P₁ state in a cryogenic environment, we significantly increase the chemical reaction cross-section for collisions of Yb with reactants. We characterize the dependence of the enhancement on the properties of the laser light, and study the final state distribution of the YbOH products. The resulting bright, cold YbOH beam can be used to increase the statistical sensitivity in searches for new physics utilizing YbOH, such as electron electric dipole moment and nuclear magnetic quadrupole moment experiments. We also perform new quantum chemical calculations that confirm the enhanced reactivity observed in our experiment and compare reaction pathways of Yb(³P) with the reactants H₂O and H₂O₂. More generally, our work presents a broad approach for improving experiments that use cryogenic molecular beams for laser cooling and precision measurement searches of BSM physics

Optical cycling in polyatomic molecules with complex hyperfine structure

We have developed and demonstrated a scheme to achieve rotationally-closed photon cycling in polyatomic molecules with complex hyperfine structure and sensitivity to hadronic symmetry violation, specifically $^{171}$YbOH and $^{173}$YbOH. We calculate rotational branching ratios for spontaneous decay and identify repumping schemes which use electro-optical modulators (EOMs) to address the hyperfine structure. We demonstrate our scheme by cycling photons in a molecular beam and verify that we have achieved rotationally-closed cycling by measuring optical pumping into unaddressed vibrational states. Our work makes progress along the path toward utilizing photon cycling for state preparation, readout, and laser cooling in precision measurements of polyatomic molecules with complex hyperfine structure.Comment: 10 pages, 7 figure

Quantum Control of Trapped Polyatomic Molecules for eEDM Searches

Ultracold polyatomic molecules are promising candidates for experiments in quantum science, quantum sensing, ultracold chemistry, and precision measurements of physics beyond the Standard Model. A key, yet unrealized, requirement of these experiments is the ability to achieve full quantum control over the complex internal structure of the molecules. Here, we establish coherent control of individual quantum states in a polyatomic molecule, calcium monohydroxide (CaOH), and use these techniques to demonstrate a method for searching for the electron electric dipole moment (eEDM). Optically trapped, ultracold CaOH molecules are prepared in a single quantum state, polarized in an electric field, and coherently transferred into an eEDM sensitive state where an electron spin precession measurement is performed. To extend the coherence time of the measurement, we utilize eEDM sensitive states with tunable, near-zero magnetic field sensitivity. The spin precession coherence time is limited by AC Stark shifts and uncontrolled magnetic fields. These results establish a path for eEDM searches with trapped polyatomic molecules, towards orders-of-magnitude improved experimental sensitivity to time-reversal-violating physics

Measuring Fundamental Symmetry Violation in Polyatomic Molecules

Open questions in fundamental physics, such as the cosmological origins of the observed imbalance of matter and antimatter, motivate the search for fundamental symmetry violating physics beyond the Standard Model (BSM). Recent measurements of heavy, polar, diatomic molecules constrain the existence of new, Parity (P) and Time-reversal (T) violating physics at 10-50 TeV energy scales, exceeding the reach of particle colliders. The power of existing molecular measurements motivates us to pursue the next-generation of searches for symmetry violation. By adopting polyatomic molecules as an experimental platform, we can generically combine laser-cooling and trapping, BSM sensitivity, and exquisite quantum control over P and/or T violating energy shifts. These improvements are projected to increase the sensitivity of measurements to the PeV energy scale. In this thesis, we develop the foundations for new physics searches using cold and ultracold, linear triatomic molecules. These molecules have long-lived vibrational bending modes with closely spaced, opposite parity doublets, a key structure that aids polarizability, molecule control, state engineering, and systematic suppression. We produce a cryogenic buffer gas beam of cold YbOH molecules, using laser-enhanced chemical reactions to increase molecular yield by an order of magnitude. As a prerequisite for precision measurements, we perform high-resolution spectroscopic characterization of both the ground and excited bending modes of YbOH. Next, we present detailed tests of quantum state preparation and readout protocols in a YbOH beam, successfully demonstrating Ramsey interferometry using two-photon transitions. Finally, as part of the PolyEDM collaboration, we illustrate the power of polyatomic molecules by combining laser cooling and optical trapping with quantum state engineering to perform proof-of-principle measurements of P,T violating physics in magnetically-insensitive states of ultracold CaOH molecules at Harvard University. Our results open the door to a wide range of quantum-enhanced symmetry violation searches benefiting from the unique structural features of polyatomic molecules.</p

Quantum Trajectory Dynamics of a Superconducting Qubit under Measurement and Unitary Evolution

From the Washington University Senior Honors Thesis Abstracts (WUSHTA), Spring 2015. Published by the Office of Undergraduate Research. Joy Zalis Kiefer, Director of Undergraduate Research and Associate Dean in the College of Arts & Sciences; Stacy Ross, Editor; Kristin G. Sobotka, Undergraduate Research Coordinator; Jennifer Kohl. Mentor: Kater Murc