Control of Optical Transitions with Magnetic Fields in Weakly Bound Molecules

McGuyer, B. H.; McDonald, Mickey; Iwata, Geoffrey Z.; Skomorowski, Wojciech; Moszyński, Robert; Zelevinsky, Tanya

doi:10.1103/physrevlett.115.053001

Cited by 26 publications

(26 citation statements)

References 23 publications

(76 reference statements)

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“…The photodissociation laser light has strictly controlled frequency and polarization, yielding photofragments in fully defined quantum states. The ab initio theory is aided by a state-of-the-art molecular model [11,12] that captures the effects of nonadiabatic mixing and yields excellent agreement with spectroscopic measurements [13][14][15][16].…”

Section: Introductionmentioning

confidence: 99%

Experimental and theoretical investigation of the crossover from the ultracold to the quasiclassical regime of photodissociation

et al. 2018

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At ultralow energies, atoms and molecules undergo collisions and reactions that are best described in terms of quantum mechanical wave functions. In contrast, at higher energies these processes can be understood quasiclassically. Here, we investigate the crossover from the quantum mechanical to the quasiclassical regime both experimentally and theoretically for photodissociation of ultracold diatomic strontium molecules. This basic reaction is carried out with a full control of quantum states for the molecules and their photofragments. The photofragment angular distributions are imaged, and calculated using a quantum mechanical model as well as the WKB and a semiclassical approximation that are explicitly compared across a range of photofragment energies. The reaction process is shown to converge to its high-energy (axial recoil) limit when the energy exceeds the height of any reaction barriers. This phenomenon is quantitatively investigated for two-channel photodissociation using intuitive parameters for the channel amplitude and phase. While the axial recoil limit is generally found to be well described by a commonly used quasiclassical model, we find that when the photofragments are identical particles, their bosonic or fermionic quantum statistics can cause this model to fail, requiring a quantum mechanical treatment even at high energies.

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Section: Introductionmentioning

confidence: 99%

Experimental and theoretical investigation of the crossover from the ultracold to the quasiclassical regime of photodissociation

et al. 2018

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“…Considering I CPP(1) baa , the major difference as compared with the derivation given in III B is that two spherical harmonics placed on the centre a need to be coupled first. Next, translation of the STO from the centre b to the centre a enables to integrate over the angles and the Jacobian cancels the apparent 1/r 2 singularity introduced by the potential (59). This allows to expand the Gaussian damping function with help of the binomial theorem and the final result is written as a linear combination of the W lmn integrals defined by Eq.…”

Section: Core Polarisation Matrix Elementsmentioning

confidence: 99%

“…See, for instance, Refs. [56][57][58][59][60][61] for joint experimental and theoretical studies of new spectroscopic features of the strontium molecule. Electronic structure calculations can also be used to predict new schemes for the formation of ultracold diatomic molecules [62][63][64][65][66][67].…”

Section: Introductionmentioning

confidence: 99%

Combining Slater-type orbitals and effective core potentials

2017

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We present a general methodology to evaluate matrix elements of the effective core potentials (ECPs) within one-electron basis set of Slater-type orbitals (STOs). The scheme is based on translation of individual STO distributions in the framework of Barnett-Coulson method. We discuss different types of integrals which naturally appear and reduce them to few basic quantities which can be calculated recursively or purely numerically. Additionally, we consider evaluation of the STOs matrix elements involving the core polarisation potentials (CPP) and effective spin-orbit potentials. Construction of the STOs basis sets designed specifically for use with ECPs is discussed and differences in comparison with all-electron basis sets are briefly summarised. We verify the validity of the present approach by calculating excitation energies, static dipole polarisabilities and valence orbital energies for the alkaline earth metals (Ca, Sr, Ba). Finally, we evaluate interaction energies, permanent dipole moments and ionisation energies for barium and strontium hydrides, and compare them with the best available experimental and theoretical data.

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“…When a reaction proceeds at such low temperatures, it becomes possible to control its outcome by applying modest electric or magnetic fields. This occurs because the size of Stark or Zeeman shifts can be much greater than the kinetic energy [1], and the density of molecular states is high near the threshold, facilitating mixing by external fields [2]. Field control of diatomicmolecule collisions and reactions has been investigated recently for polar molecules, largely focusing on rate constants [3][4][5].Photodissociation of a diatomic molecule is a basic chemical reaction where a bond breaks under the influence of light.…”

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confidence: 99%

Control of Ultracold Photodissociation with Magnetic Fields

McDonald¹,

Majewska²,

Lee³

et al. 2018

Phys. Rev. Lett.

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Photodissociation of a molecule produces a spatial distribution of photofragments determined by the molecular structure and the characteristics of the dissociating light. Performing this basic reaction at ultracold temperatures allows its quantum mechanical features to dominate. In this regime, weak applied fields can be used to control the reaction. Here, we photodissociate ultracold diatomic strontium in magnetic fields below 10 G and observe striking changes in photofragment angular distributions. The observations are in excellent agreement with a multichannel quantum chemistry model that includes nonadiabatic effects and predicts strong mixing of partial waves in the photofragment energy continuum. The experiment is enabled by precise quantum-state control of the molecules.

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Control of Optical Transitions with Magnetic Fields in Weakly Bound Molecules

Cited by 26 publications

References 23 publications

Experimental and theoretical investigation of the crossover from the ultracold to the quasiclassical regime of photodissociation

Experimental and theoretical investigation of the crossover from the ultracold to the quasiclassical regime of photodissociation

Combining Slater-type orbitals and effective core potentials

Control of Ultracold Photodissociation with Magnetic Fields

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