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1. Quantum Metrology with a Molecular Lattice Clock and State-Selected Photodissociation of Ultracold Molecules

   Lee, C.-H. ( January 2020 , Columbia University thesis)

   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 = 8 × 10^11. 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. 

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2. Investigation of the fine structure of antihydrogen

   https://doi.org/10.1038/s41586-020-2006-5  

   Ahmadi, M. ; Alves, B. X. ; Baker, C. J. ; Bertsche, W. ; Capra, A. ; Carruth, C. ; Cesar, C. L. ; Charlton, M. ; Cohen, S. ; Collister, R. ; et al ( February 2020 , Nature)

   At the historic Shelter Island Conference on the Foundations of Quantum Mechanics in 1947, Willis Lamb reported an unexpected feature in the fine structure of atomic hydrogen: a separation of the 2S1/2 and 2P1/2 states1. The observation of this separation, now known as the Lamb shift, marked an important event in the evolution of modern physics, inspiring others to develop the theory of quantum electrodynamics2–5. Quantum electrodynamics also describes antimatter, but it has only recently become possible to synthesize and trap atomic antimatter to probe its structure. Mirroring the historical development of quantum atomic physics in the twentieth century, modern measurements on anti-atoms represent a unique approach for testing quantum electrodynamics and the foundational symmetries of the standard model. Here we report measurements of the fine structure in the n = 2 states of antihydrogen, the antimatter counterpart of the hydrogen atom. Using optical excitation of the 1S–2P Lyman-α transitions in antihydrogen6, we determine their frequencies in a magnetic field of 1 tesla to a precision of 16 parts per billion. Assuming the standard Zeeman and hyperfine interactions, we infer the zero-field fine-structure splitting (2P1/2–2P3/2) in antihydrogen. The resulting value is consistent with the predictions of quantum electrodynamics to a precision of 2 per cent. Using our previously measured value of the 1S–2S transition frequency6,7, we find that the classic Lamb shift in antihydrogen (2S1/2–2P1/2 splitting at zero field) is consistent with theory at a level of 11 per cent. Our observations represent an important step towards precision measurements of the fine structure and the Lamb shift in the antihydrogen spectrum as tests of the charge– parity–time symmetry8 and towards the determination of other fundamental quantities, such as the antiproton charge radius9,10, in this antimatter system. 

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3. Boosting the efficiency of high harmonic amplification by modulating a plasma-based X-ray laser with the second harmonic of the fundamental frequency laser field

   Khairulin, I.R. ; Antonov, I.R. ; Kocharovskaya, O. ( October 2021 , International conference on Ultrafast Optical Science)

   Attosecond pulses formed by high order harmonics (HHs) of an infrared (IR) laser field is a powerful tool for studying and controlling ultrafast dynamics of electrons in atoms, molecules and solids at its intrinsic time-scale. However, in the X-ray range the energy of attosecond pulses is rather limited. Their amplification is an important but very challenging problem since none of the existing amplifiers can support the corresponding PHz bandwidth. In our previous work [1] we proposed a method for the attosecond pulse amplification in hydrogen-like active medium of a recombination plasma-based X-ray laser dressed by a replica of the fundamental frequency IR field used for the HH generation. Due to the IRfield-induced sub-laser-cycle Stark shift and splitting of the lasing energy levels the gain of the active medium is redistributed over the combination frequencies, separated from the resonance by even multiples of the frequency of the IR field. If the incident HHs forming an attosecond pulse train are tuned in resonance with the induced gain lines and the active plasma medium is strongly dispersive for the modulating IR field, then during the amplification the relative phases of harmonics and (under the optimal choice of the IR field strength) the shape of the amplified pulses will be preserved. In the present work we show the possibility of boosting the efficiency of HH amplification by modulating the active medium of an X-ray laser with the second harmonic of the fundamental frequency IR field. We show that under the action of a laser field (with arbitrary frequency) the gain redistribution occurs not only over the even combination frequencies discussed in [1], but also over the odd frequencies separated from the resonance by odd multiples of the laser frequency. Besides, nearly half of the medium gain is contained in the even induced gain lines, and nearly half in the odd. If the modulating field is the second harmonic of the IR field, used for the generation the HHs and attosecond pulses, then the seeding HHs can be tuned in resonance with both even and odd gain lines simultaneously, which will make the overall gain much higher as compared to the previously considered case of the fundamental frequency modulating field (when only the even gain lines play the role). By the example of the C5+ X-ray laser with 3.38 nm wavelength of the inverted transition we show the possibility of increasing the efficiency of 430 as pulse amplification by 8.5 times when the active medium is modulated with the second harmonic of the fundamental frequency IR field with wavelength 2.1 µm. 

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4. Laser cooling of antihydrogen atoms

   https://doi.org/10.1038/s41586-021-03289-6  

   Baker, C. J. ; Bertsche, W. ; Capra, A. ; Carruth, C. ; Cesar, C. L. ; Charlton, M. ; Christensen, A. ; Collister, R. ; Mathad, A. Cridland ; Eriksson, S. ; et al ( April 2021 , Nature)

   null (Ed.)

   Abstract The photon—the quantum excitation of the electromagnetic field—is massless but carries momentum. A photon can therefore exert a force on an object upon collision 1 . Slowing the translational motion of atoms and ions by application of such a force 2,3 , known as laser cooling, was first demonstrated 40 years ago 4,5 . It revolutionized atomic physics over the following decades 6–8 , and it is now a workhorse in many fields, including studies on quantum degenerate gases, quantum information, atomic clocks and tests of fundamental physics. However, this technique has not yet been applied to antimatter. Here we demonstrate laser cooling of antihydrogen 9 , the antimatter atom consisting of an antiproton and a positron. By exciting the 1S–2P transition in antihydrogen with pulsed, narrow-linewidth, Lyman-α laser radiation 10,11 , we Doppler-cool a sample of magnetically trapped antihydrogen. Although we apply laser cooling in only one dimension, the trap couples the longitudinal and transverse motions of the anti-atoms, leading to cooling in all three dimensions. We observe a reduction in the median transverse energy by more than an order of magnitude—with a substantial fraction of the anti-atoms attaining submicroelectronvolt transverse kinetic energies. We also report the observation of the laser-driven 1S–2S transition in samples of laser-cooled antihydrogen atoms. The observed spectral line is approximately four times narrower than that obtained without laser cooling. The demonstration of laser cooling and its immediate application has far-reaching implications for antimatter studies. A more localized, denser and colder sample of antihydrogen will drastically improve spectroscopic 11–13 and gravitational 14 studies of antihydrogen in ongoing experiments. Furthermore, the demonstrated ability to manipulate the motion of antimatter atoms by laser light will potentially provide ground-breaking opportunities for future experiments, such as anti-atomic fountains, anti-atom interferometry and the creation of antimatter molecules. 

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5. Impacts of extending the π-conjugation of the 2,2′-biquinoline ligand on the photophysics and reverse saturable absorption of heteroleptic cationic iridium( iii ) complexes

   https://doi.org/10.1039/D1TC03601G  

   Lu, Taotao ; Lu, Cuifen ; Cui, Peng ; Kilina, Svetlana ; Sun, Wenfang ( November 2021 , Journal of Materials Chemistry C)

   Two heteroleptic monocationic Ir( iii ) complexes bearing 6,6′-bis(7-benzothiazolylfluoren-2-yl)-2,2′-biquinoline as the diimine ligand with different degrees of π-conjugation were synthesized and their photophysics was investigated by spectroscopic techniques and first principles calculations. These complexes possessed two intense absorption bands at 300–380 nm and 380–520 nm in toluene that are predominantly ascribed to the diimine ligand-localized 1 π,π* transition and intraligand charge transfer ( 1 ILCT)/ 1 π,π* transitions, respectively, with the latter being mixed with minor 1 MLCT (metal-to-ligand charge transfer)/ 1 LLCT (ligand-to-ligand charge transfer) configurations. Both complexes also exhibited a spin-forbidden, very weak 3 MLCT/ 3 LLCT/ 3 π,π* absorption band at 520–650 nm. The emission of these complexes appeared in the red spectral region ( λ em : 640 nm for Ir-1 and 648 nm for Ir-2 in toluene) with a quantum yield of <10% and a lifetime of hundreds of ns, which emanated from the 3 ILCT/ 3 π,π* state. The 3 ILCT/ 3 π,π* state also gave rise to broad and moderately strong transient absorption (TA) at ca. 480–800 nm. Extending the π-conjugation of the diimine ligand via inserting CC triplet bonds between the 7-benzothiazolylfluoren-2-yl substituents and 2,2′-biquinoline slightly red-shifted the absorption bands, the emission bands, and the TA bands in Ir-2 compared to those in Ir-1 that lacks the connecting CC triplet bonds in the diimine ligand. The stronger excited-state absorption with respect to the ground-state absorption at 532 nm led to strong reverse saturable absorption (RSA) for ns laser pulses at this wavelength, with the RSA of Ir-2 being slightly stronger than that of Ir-1, which correlated well with their ratios of the excited-state to ground-state absorption cross sections ( σ ex / σ 0 ). These results suggest that extending the π-conjugation of the 2,2′-biquinoline ligand via incorporating the 7-benzothiazolylfluoren-2-yl substituents retained the broad but weak ground-state absorption at 500–650 nm, meanwhile increased the triplet excited-state lifetimes, which resulted in the much stronger triplet excited-state absorption in this spectral region and strong RSA at 532 nm. Thus, these complexes are promising candidates as broadband reverse saturable absorbers. 

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