Proposed molecular quantum gate takes advantage of internal coherence and resonant electric dipolar interaction with high fidelity and optical scalability.

Femtochemistry techniques have been instrumental in accessing the short time scales necessary to probe transient intermediates in chemical reactions. In this study, we took the contrasting approach of prolonging the lifetime of an intermediate by preparing reactant molecules in their lowest rovibronic quantum state at ultralow temperatures, thereby markedly reducing the number of exit channels accessible upon their mutual collision. Using ionization spectroscopy and velocity-map imaging of a trapped gas of potassium-rubidium (KRb) molecules at a temperature of 500 nanokelvin, we directly observed reactants, intermediates, and products of the reaction 40K87Rb + 40K87Rb → K2Rb2* → K2 + Rb2. Beyond observation of a long-lived, energy-rich intermediate complex, this technique opens the door to further studies of quantum-state–resolved reaction dynamics in the ultracold regime.

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STIRAP (Stimulated Raman Adiabatic Passage) is a powerful laser-based method, usually involving two photons, for efficient and selective transfer of population between quantum states. A particularly interesting feature is the fact that the coupling between the initial and the final quantum states is via an intermediate state even though the lifetime of the latter can be much shorter than the interaction time with the laser radiation. Nevertheless, spontaneous emission from the intermediate state is prevented by quantum interference. Maintaining the coherence between the initial and final state throughout the transfer process is crucial.STIRAP was initially developed with applications in chemical dynamics in mind. That is why the original paper of 1990 was published in The Journal of Chemical Physics. However, as of about the year 2000, the unique capabilities of STIRAP and its robustness with respect to small variations of some experimental parameters stimulated many researchers to apply the scheme in a variety of other fields of physics. The successes of these efforts are documented in this collection of articles. In Part A the experimental success of STIRAP in manipulating or controlling molecules, photons, ions or even quantum systems in a solid-state environment is documented. After a brief introduction to the basic physics of STIRAP, the central role of the method in the formation of ultra-cold molecules is discussed, followed by a presentation of how precision experiments (measurement of the upper limit of the electric dipole moment of the electron or detecting the consequences of parity violation in chiral molecules) or chemical dynamics studies at ultra-low temperatures benefit from STIRAP. Next comes the STIRAP-based control of photons in cavities followed by a group of three contributions which highlight the potential of the STIRAP concept in classical physics by presenting data on the transfer of waves (photonic, magnonic and phononic) between respective wave guides. The works on ions or ion-strings discuss options for applications e.g. in quantum information. Finally, the success of STIRAP in the controlled manipulation of quantum states in solid-state systems, which are usually hostile towards coherent processes, is presented, dealing with data storage in rare-earth ion doped crystals and in NV-centers or even in superconducting quantum circuits. The works on ions and those involving solid-state systems emphasize the relevance of the results for quantum information protocols.Part B deals with theoretical work including further concepts relevant for quantum information or invoking STIRAP for the manipulation of matter waves. The subsequent articles discuss experiments underway to demonstrate the potential of STIRAP for populating otherwise inaccessible high-lying Rydberg states of molecules, or controlling and cooling the translational motion of particles in a molecular beam or the polarization of angular momentum states. The series of articles concludes with a more speculative application of STIRAP i...

Guided by ab initio calculations, Fourier transform microwave spectra in the 6-21 GHz region are obtained for seven isotopomers of the complex formed between 1-chloro-1-fluoroethylene and acetylene. These include the four possible combinations of (35)Cl- and (37)Cl-containing CH(2)CClF with the most abundant acetylene isotopic modification, HCCH, and its H(13)C(13)CH analogue, as well as three singly substituted deuterated isotopomers. Analysis of the spectra determines the rotational constants and additionally, the complete chlorine quadrupole hyperfine coupling tensors in both the inertial and principal electric field gradient axis systems, and where appropriate, the diagonal components of the deuterium quadrupole coupling tensors. The inertial information contained in the rotational constants provides the structure for CH(2)CClF-HCCH: a primary, hydrogen bonding interaction existing between the HCCH donor and the F atom acceptor on the 1-chloro-1-fluoroethylene moiety, while a secondary interaction occurs between the acetylenic bond on the HCCH molecule and the H atom cis to the hydrogen-bonded F atom on the substituted ethylene, which causes the hydrogen bond to deviate from linearity. This is similar to the structure obtained for 1,1-difluoroethylene-HCCH [H. O. Leung and M. D. Marshall, J. Chem. Phys. 126, 154301 (2006)], and indeed, to within experimental uncertainty, the intermolecular interactions in CH(2)CClF-HCCH and its 1,1-difluoroethylene counterpart are practically indistinguishable, even though ab initio calculations at the MP2∕6-311G++(2d, 2p) level suggest that the former complex is more strongly bound.

Rapid progress in atomic, molecular, and optical (AMO) physics techniques enabled the creation of ultracold samples of molecular species and opened opportunities to explore chemistry in the ultralow temperature regime. In particular, both the external and internal quantum degrees of freedom of the reactant atoms and molecules are controlled, allowing studies that explored the role of the longrange potential in ultracold reactions. The kinetics of these reactions have typically been determined using the loss of reactants as proxies. To extend such studies into the short-range, we developed an experimental apparatus that combines the production of quantum-state-selected ultracold KRb molecules with ion mass and kinetic energy spectrometry, and directly observed KRb + KRb reaction intermediates and products [Science, 2019[Science, , 366, 1111. Here, we present the apparatus in detail. For future studies that aim for detecting the quantum states of the reaction products, we demonstrate a photodissociation based scheme to calibrate the ion kinetic energy spectrometer at low energies.

We have directly detected millimeter wave (mm-wave) free space superradiant emission from Rydberg states (n ∼ 30) of barium atoms in a single shot. We trigger the cooperative effects with a weak initial pulse and detect with single-shot sensitivity and 20 ps time resolution, which allows measurement and shot-by-shot analysis of the distribution of decay rates, time delays, and timedependent frequency shifts. Cooperative line shifts and decay rates are observed that exceed values that would correspond to the Doppler width of 250 kHz by a factor of 20 and the spontaneous emission rate of 50 Hz by a factor of 10 5 . The initial superradiant output pulse is followed by evolution of the radiation-coupled many-body system toward complex long-lasting emission modes. A comparison to a mean-field theory is presented which reproduces the quantitative time-domain results, but fails to account for either the frequency-domain observations or the long-lived features.Superradiance is an effect in which emitters radiate collectively and coherently due to constructive interference between electric dipoles that communicate with each other via a shared radiation field [1]. Subradiance is exactly the opposite -a collective inhibition of radiation due to destructive interference between the radiation from an array of dipoles [2,3]. These cooperative phenomena provide insights into fundamental many-body physics [4][5][6] and suggest applications ranging from quantum information storage [7][8][9] to narrow linewidth lasers [10][11][12][13].The large electric dipole transition moments and long wavelengths associated with Rydberg-Rydberg transitions make these transitions natural candidates for observing collective effects at relatively low atom number densities (ρ ∼ 10 6 cm −3 ). Hydrogenic scaling rules show that, for ∆n = 1 (where n is the principal quantum number), the transition dipole moment between Rydberg states scales as µ ∝ n 2 and the wavelength scales as λ ∝ n 3 . The transition dipole moment controls only the individual atom spontaneous decay rate, which is independent of density. Collective effects, however, scale in multiples of the spontaneous decay rate. The multiplicative factors scale as the optical depth (OD = ρλ 2 L, where ρ is the density and L is the length of the sample) [6] or the relative density (RD = ρλ 3 ) [14]. Thus, these two scaling rules result in strong collective effects at several orders of magnitude lower densities than between valence states of atoms or molecules. Superradiant emission is also focused primarily on the transition with the smallest ∆n allowed by the ∆ = ±1 angular momentum selection rule [15]. For Rydberg states with n ∼ 30, ∆n = 1 transitions lie at ∼300 GHz (λ ∼ 1mm) and have transition moments on the order of 500 debye [16].Typically, the total number of Rydberg state atoms in a single experiment has been too small to permit direct detection of the emitted electric field. Previous studies of collective effects in ensembles of Rydberg states have relied on state-selective field ioni...

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