Precise study of asymptotic physics with subradiant ultracold molecules

Weakly bound molecules have physical properties without atomic analogues, even as the bond length approaches dissociation. In particular, the internal symmetries of homonuclear diatomic molecules result in formation of two-body superradiant and subradiant excited states. While superradiance has been demonstrated in a variety of systems, subradiance is more elusive due to the inherently weak interaction with the environment. Here we characterize the properties of deeply subradiant molecular states with intrinsic quality factors exceeding $10^{13}$ via precise optical spectroscopy with the longest molecule-light coherent interaction times to date. We find that two competing effects limit the lifetimes of the subradiant molecules, with different asymptotic behaviors. The first is radiative decay via weak magnetic-dipole and electric-quadrupole interactions. We prove that its rate increases quadratically with the bond length, confirming quantum mechanical predictions. The second is nonradiative decay through weak gyroscopic predissociation, with a rate proportional to the vibrational mode spacing and sensitive to short-range physics. This work bridges the gap between atomic and molecular metrology based on lattice-clock techniques, yielding new understanding of long-range interatomic interactions and placing ultracold molecules at the forefront of precision measurements.Comment: 12 pages, 6 figure

Accurate determination of blackbody radiation shifts in a strontium molecular lattice clock

Molecular lattice clocks enable the search for new physics, such as fifth forces or temporal variations of fundamental constants, in a manner complementary to atomic clocks. Blackbody radiation (BBR) is a major contributor to the systematic error budget of conventional atomic clocks and is notoriously difficult to characterize and control. Here, we combine infrared Stark-shift spectroscopy in a molecular lattice clock and modern quantum chemistry methods to characterize the polarizabilities of the Sr2 molecule from dc to infrared. Using this description, we determine the static and dynamic blackbody radiation shifts for all possible vibrational clock transitions to the 10−16 level. This constitutes an important step toward millihertz-level molecular spectroscopy in Sr2 and provides a framework for evaluating BBR shifts in other homonuclear molecules

Precise Determination of Blackbody Radiation Shifts in a Strontium Molecular Lattice Clock

Molecular lattice clocks enable the search for new physics, such as fifth forces or temporal variations of fundamental constants, in a manner complementary to atomic clocks. Blackbody radiation (BBR) is a major contributor to the systematic error budget of conventional atomic clocks and is notoriously difficult to characterize and control. Here, we combine infrared Stark-shift spectroscopy in a molecular lattice clock and modern quantum chemistry methods to characterize the polarizabilities of the Sr$_2$ molecule from dc to infrared. Using this description, we determine the static and dynamic blackbody radiation shifts for all possible vibrational clock transitions to the $10^{-16}$ level. This constitutes an important step towards mHz-level molecular spectroscopy in Sr$_2$, and provides a framework for evaluating BBR shifts in other homonuclear molecules.Comment: 6 pages, 4 figures, updated reference

Prospects for sympathetic cooling of molecules in electrostatic, ac and microwave traps

We consider how trapped molecules can be sympathetically cooled by ultracold atoms. As a prototypical system, we study LiH molecules co-trapped with ultracold Li atoms. We calculate the elastic and inelastic collision cross sections of 7LiH + 7Li with the molecules initially in the ground state and in the first rotationally excited state. We then use these cross sections to simulate sympathetic cooling in a static electric trap, an ac electric trap, and a microwave trap. In the static trap we find that inelastic losses are too great for cooling to be feasible for this system. The ac and microwave traps confine ground-state molecules, and so inelastic losses are suppressed. However, collisions in the ac trap can take molecules from stable trajectories to unstable ones and so sympathetic cooling is accompanied by trap loss. In the microwave trap there are no such losses and sympathetic cooling should be possible

Phase protection of Fano-Feshbach resonances

Decay of bound states due to coupling with free particle states is a general phenomenon occurring at energy scales from MeV in nuclear physics to peV in ultracold atomic gases. Such a coupling gives rise to Fano-Feshbach resonances (FFR) that have become key to understanding and controlling interactions—in ultracold atomic gases, but also between quasiparticles, such as microcavity polaritons. Their energy positions were shown to follow quantum chaotic statistics. In contrast, their lifetimes have so far escaped a similarly comprehensive understanding. Here, we show that bound states, despite being resonantly coupled to a scattering state, become protected from decay whenever the relative phase is a multiple of π. We observe this phenomenon by measuring lifetimes spanning four orders of magnitude for FFR of spin–orbit excited molecular ions with merged beam and electrostatic trap experiments. Our results provide a blueprint for identifying naturally long-lived states in a decaying quantum system

Software for the frontiers of quantum chemistry:An overview of developments in the Q-Chem 5 package

This article summarizes technical advances contained in the fifth major release of the Q-Chem quantum chemistry program package, covering developments since 2015. A comprehensive library of exchange–correlation functionals, along with a suite of correlated many-body methods, continues to be a hallmark of the Q-Chem software. The many-body methods include novel variants of both coupled-cluster and configuration-interaction approaches along with methods based on the algebraic diagrammatic construction and variational reduced density-matrix methods. Methods highlighted in Q-Chem 5 include a suite of tools for modeling core-level spectroscopy, methods for describing metastable resonances, methods for computing vibronic spectra, the nuclear–electronic orbital method, and several different energy decomposition analysis techniques. High-performance capabilities including multithreaded parallelism and support for calculations on graphics processing units are described. Q-Chem boasts a community of well over 100 active academic developers, and the continuing evolution of the software is supported by an “open teamware” model and an increasingly modular design

Directly probing anisotropy in atom-molecule collisions through quantum scattering resonances

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