Over the past few decades, rapid development of laser cooling techniques and narrow-linewidth lasers have allowed atom-based quantum clocks to achieve unprecedented precision. Techniques originally developed for atomic clocks can be extended to ultracold molecules, with applications ranging from quantum-state-controlled ultracold chemistry to searches for new physics. Because of the richness of molecular structure, quantum metrology based on molecules provides possibilities for testing physics that is beyond the scope of traditional atomic clocks. This thesis presents the work performed to establish a state-of-the-art quantum clock based on ultracold molecules. The molecular clock is based on a frequency difference between two vibrational levels in the electronic ground state of 88Sr2 diatomic molecules. Such a clock allows us test molecular QED, improve constraints on nanometer-scale gravity, and potentially provide a model-independent test of temporal variations of the proton-electron mass ratio. Trap-insensitive spectroscopy is crucial for extending coherent molecule-light interactions and achieving a high quality factor Q. We have demonstrated a magic wavelength technique for molecules by manipulating the optical lattice frequency near narrow polarizability resonances. This general technique allows us to increase the coherence time to tens of ms, an improvement of a factor of several thousand, and to narrow the linewidth of a 25 THz vibrational transition initially to 30 Hz. This width corresponds to the quality factor Q=8x10^11. Besides the molecular quantum metrology, investigations of novel phenomena in state-selected photodissociation are also described in this thesis, including magnetic-field control of photodissociation and observation of the crossover from ultracold to quasiclassical chemistry.
Over the past few decades, rapid development of laser cooling techniques and narrow-linewidth lasers have allowed atom-based quantum clocks to achieve unprecedented precision. Techniques originally developed for atomic clocks can be extended to ultracold molecules, with applications ranging from quantum-state-controlled ultracold chemistry to searches for new physics. Because of the richness of molecular structure, quantum metrology based on molecules provides possibilities for testing physics that is beyond the scope of traditional atomic clocks. This thesis presents the work performed to establish a state-of-the-art quantum clock based on ultracold molecules. The molecular clock is based on a frequency difference between two vibrational levels in the electronic ground state of 88Sr2 diatomic molecules. Such a clock allows us test molecular QED, improve constraints on nanometer-scale gravity, and potentially provide a model-independent test of temporal variations of the proton-electron mass ratio. Trap-insensitive spectroscopy is crucial for extending coherent molecule-light interactions and achieving a high quality factor Q. We have demonstrated a magic wavelength technique for molecules by manipulating the optical lattice frequency near narrow polarizability resonances. This general technique allows us to increase the coherence time to tens of ms, an improvement of a factor of several thousand, and to narrow the linewidth of a 25 THz vibrational transition initially to 30 Hz. This width corresponds to the quality factor Q=8x10^11. Besides the molecular quantum metrology, investigations of novel phenomena in state-selected photodissociation are also described in this thesis, including magnetic-field control of photodissociation and observation of the crossover from ultracold to quasiclassical chemistry.
Clocks that are based on atomic and molecular transitions can serve as unparalleled sensors of fundamental phenomena. In particular, a clock based on vibrations in a diatomic molecule is a highly precise sensor of the interatomic force, including possible contributions from new physics. Such a clock is also of metrological interest, since vibrational states in homonuclear molecules have extremely long lifetimes. We present the technique of near-resonant magic-wavelength trapping for strontium dimers, which allows us to reach coherence times exceeding 100 ms for far-separated vibrational state superpositions. The development of the molecular clock is accelerated through state-of-the-art quantum chemistry work.
— Modern capabilities in quantum state engineering of ultracold matter and precise control of light fields now permit accurate control of interactions between matter and field to suit applications for precision tests of fundamental physics. We report on our recent development of a highly stable and accurate optical atomic clock based on ultracold neutral Sr atoms confined in an optical lattice. We discuss precision tools for the lattice clock, including stabilized lasers with sub-Hz linewidth, femtosecond-comb based technology allowing accurate clock comparison in both microwave and optical domains, and clock transfer over optical fibers. With microkelvin Sr atoms confined in an optical lattice that provide a zero differential a.c. Stark shift between two clock states, we achieve a resonance quality factor >2×10 on the S0 − P0 doubly forbidden Sr clock transition at 698 nm. High resolution spectroscopy of spin-polarized atoms is used for both high-performance clock operations and accurate atomic structure measurement. The overall systematic uncertainty of the clock has been evaluated at the 10−16 level, while the stability approaches low 10−15 at 1 s. These developments in precise engineering of lightatom interactions can be extended to the field of ultracold molecules, bringing new prospects for precision measurements, quantum control, and determinations of the constancy of the fundamental constants.
Ultracold molecules are a powerful platform for metrology, precision measurements and searches for new, beyond-the-Standard-Model physics. Sr2, thanks to its simple structure, insensitivity to external fields and narrow optical transitions, provides an excellent testbed for the search for new interactions. Here, we present a detailed characterization of our 88Sr2 molecular clock for a vibrational transition spanning the entire depth of the ground state potential. We also discuss prospects to use strontium isotopologues to place improved constraints on new mass-dependent forces, including possible pathways toward the production of ultracold 86Sr2 and 84Sr2 dimers and spectroscopy of clock lines in these species for use in the search for new mass-dependent forces.
Abstract : We have established the strontium molecular clock as the leading ultracold-molecule precision measurement platform. We can fully control the molecules internal and external quantum states, as in state-of-the-art atomic lattice clocks. Using the quantized molecular spectra in an optical lattice, we devised a new lattice thermometry method that is advantageous for many lattice experiments, including clocks and manybody physics studies. The full quantum control allowed us to observe deeply subradiant molecular states, and coherently control them. We measured lifetimes enhanced by up to 300 times. Ultranarrow transitions to these states permitted a rigorous study of asymptotic physics at the atom-molecule threshold. We proved that subradiant states can decay to the ground state via higher-order electromagnetic transitions, with a rate that grows as the square of the bond length, and are quenched by predissociation at a rate proportional to the vibrational level spacing. We introduced a precise technique for measuring molecular binding energies via photofragmentation; controlled forbidden optical transition strengths with weak magnetic fields by five orders of magnitude; and explained anomalously large magnetic susceptibilities of the asymptotic molecules. The unprecedented precision, coupled with advanced ab initio theory, paves the way to exciting new directions for the molecular clock.
Abstract : Ultracold molecules provide an exciting testing ground for studies of fundamental interactions, new states of matter, and metrology. Diatomic molecules based on two-electron atoms are especially suitable for precise tests of interatomic interactions, molecular quantum electrodynamics, electron-proton mass ratio variations, and other measurements in molecular and fundamental physics. This thesis describes the construction of a new strontium apparatus, from initial vacuum system setup through characterization of ultracold atom samples, followed by a new method of efficient, all-optical production of ultracold 88Sr2 molecules in an optical lattice, with detection via optical fragmentation. High-Q spectra of the weakly bound molecules in magnetic fields are studied, yielding precise binding energies, anomalously large molecular g factors resulting from large nonadiabatic effects, and strongly enhanced magnetic susceptibility. The thesis then concludes with an outlook on future experiments in our lab, including studies of forbidden molecular transitions, and longer term studies of fundamental physics from deeply bound Sr2.
in a lattice. Sr2 has a range of electronically excited bound states which are readily accessible with optical wavelengths using the narrow 1S0->3P1 intercombination line. As in Nat. Phys. 11, 32, we measure the lifetimes of the narrow, deeply-bound subradiant states in the 1g (1S0+3P1 dissociative limit) potential, allowing for coherent control of molecules and a comparison with theoretical predictions of the lifetimes and transition strengths of these states. Next, we study ultracold photodissociation of Sr2 molecules through abortion of one and two photons near the atomic intercombination line. This allows us to observe the vector character of transition elements through the angular dissociation pattern and to directly measure barrier heights in the excited state potentials. Finally, as shown in PRL 114, 023001, we demonstrate that in a non-magic lattice, a narrow transition can be used to measure the trapped gas temperature through the linewidth of the spectral feature corresponding to the carrier transitions. We use this technique to measure the temperature of Sr2 molecules to 10x higher precision than with standard techniques. We discuss future prospects with this molecular lattice clock. 1 Funding from NIST, ARO, and NSF IGERT