Spin Polarization Spectroscopy of Alkali-Noble Gas Interatomic Potentials My pleasure to share our recent experimental results A. E. Mironov, W. Goldshlag, and J. G. Eden University of Illinois at Urbana Champaign June 22, 2017

Overview of Accomplishments Selective population of Rb and Cs 2P3/2 hyperfine states has been demonstrated Circularly-polarized (σ -) ASE emission on the alkali D2 line is generated when Rb-Xe and Cs-Xe collision pairs are photoexcited by a σ+-polarized optical field through the D2 blue satellite continuum The degree of spin polarization of Cs (6p 2P3/2) is found to be dependent on the interatomic distance (R) at which the excited complex is born Based on paper submitted to PRL \\ we’ve demonstrated a new technique. Populate specific hyperfine excited states \\ generate ASE on D2 \\ degree of spin pol depends on the excitation wavelength which in its turn is a single value function of interatomic distance (R) -we believe that this is a new powerful spectroscopic technique allowing to identify weak interactions between molecular states. -We also believe that this new method of producing spin polarized atoms may draw attention of people doing research on hyperpolarized noble gases, magnetometry and spintronics A. E. Mironov, J. D. Hewitt, and J. G. Eden “Spin Polarization of Rb and Cs np 2P3/2 (n=5,6) Atoms by Circularly-Polarized Photoexcitation of a Transient Diatomic Molecule”, Phys. Rev. Lett., 118(11), 2017 2

Alkali Atoms 2P3/2 2P1/2 2S1/2 3 + 3/2 + 1/2 - 1/2 - 3/2 + 1/2 - 1/2 Main fields – magnetometry and bio imaging (NMR) 2S1/2 + 1/2 - 1/2 3

Ground State Spin Polarization of Alkali Atoms Main fields – magnetometry and bio imaging (NMR) Hyperpolarized 129Xe Magnetometry Atomic Clocks Quantum Memory Hyperpolarized Xenon-129 Magnetic Resonance: Concepts, Production, Techniques and Applications (New Developments in NMR), 504 pages, Royal Society of Chemistry (April 14, 2015) 3

Photoassociation of Ground State Cs-Xe Collision Pairs Hyperfine splitting is not to scale. - 4

Experimental Arrangement 5

Cs-Xe Photoexcitation Spectra 6

Cs D2 Line ASE Threshold 7

Relative Contribution of σ--Polarized ASE with λ For different gas mixteres and pressures the optimal pump wavelength varies significantly. So the gas composition should be carefully picked in order to achieve higher efficiencies 8

Theoretical Prediction of the 6pσ - 5dσ MO interaction “…the hump in the 6pΣ state occurs through the interaction with the neighboring states of the same symmetry corresponding to 5D3/2 and 5D5/2 levels in their dissociation limits. We also observe a configuration mixing with the 6s→5dσ component in the 6pΣ state, which may cause the shoulder in the potential curve….” The calculated harmonic vibrational frequency for the bound states of the CsXe 5d∆ state is 33.2 cm-1 M. Ehara and H. Nakatsuji “Collision induced absorption spectra and line broadening of CsRg system (Rg=Xe, Kr, Ar, Ne) studied by the symmetry adapted cluster‐configuration interaction (SAC‐Cl) method”, J. Chem. Phys. 102, 6822 (1995) 9

A new laser spectroscopy has been demonstrated. Summary Electronic spin polarization of Cs 6p 2P3/2 atoms has been demonstrated in the absence of an external magnetic field by photoexciting a transient diatomic molecule with a circularly-polarized optical field. A new laser spectroscopy has been demonstrated. Interaction of the 6pσ antibonding MO with the 5dσ MO [Cs(5d)+Xe] has been observed. 10

Acknowledgements J. Luginsland and J. Marshall

Andrey: amirono2@illinois.edu