Mikhail Lemeshko

Manipulation of molecules with electromagnetic fields

The goal of the present article is to review the major developments that have led to the current understanding of molecule–field interactions and experimental methods for manipulating molecules with electromagnetic fields. Molecule–field interactions are at the core of several, seemingly distinct areas of molecular physics. This is reflected in the organisation of this article, which includes sections on field control of molecular beams, external field traps for cold molecules, control of molecular orientation and molecular alignment, manipulation of molecules by non-conservative forces, ultracold molecules and ultracold chemistry, controlled many-body phenomena, entanglement of molecules and dipole arrays, and stability of molecular systems in high-frequency super-intense laser fields. The article contains 852 references.

In situ X-ray absorption spectroscopy measurement of vapour-brine fractionation of antimony at hydrothermal conditions

Abstract Despite the growing geological evidence that fluid boiling and vapour-liquid separation affect the distribution of metals in magmatic-hydrothermal systems significantly, there are few experimental data on the chemical status and partitioning of metals in the vapour and liquid phases. Here we report on an in situ measurement, using X-ray absorption fine structure (XAFS) spectroscopy, of antimony speciation and partitioning in the system Sb2O3-H2O-NaCl-HCl at 400°C and pressures 270-300 bar corresponding to the vapour-liquid equilibrium. Experiments were performed using a spectroscopic cell which allows simultaneous determination of the total concentration and atomic environment of the absorbing element (Sb) in each phase. Results show that quantitative vapour-brine separation of a supercritical aqueous salt fluid can be achieved by a controlled decompression and monitoring the X-ray absorbance of the fluid phase. Antimony concentrations in equilibrium with Sb2O3 (cubic, senarmontite) in the coexisting vapour and liquid phases and corresponding SbIII vapour-liquid partitioning coefficients are in agreement with recent data obtained using batch-reactor solubility techniques. The XAFS spectra analysis shows that hydroxy-chloride complexes, probably Sb(OH)2Cl0, are dominant both in the vapour and liquid phase in a salt-water system at acidic conditions. This first in situ XAFS study of element fractionation between coexisting volatile and dense phases opens new possibilities for systematic investigations of vapour-brine and fluid-melt immiscibility phenomena, avoiding many experimental artifacts common in less direct techniques.

Nonadiabatic Preparation of Spin Crystals with Ultracold Polar Molecules

We study the growth dynamics of ordered structures of strongly interacting polar molecules in optical lattices. Using a dipole blockade of microwave excitations, we map the system onto an interacting spin-1/2 model possessing ground states with crystalline order, and describe a way to prepare these states by nonadiabatically driving the transitions between molecular rotational levels. The proposed technique bypasses the need to cross a phase transition and allows for the creation of ordered domains of considerably larger size compared to approaches relying on adiabatic preparation.

Laser-Induced Rotation of Iodine Molecules in Helium Nanodroplets: Revivals and Breaking Free

Rotation of molecules embedded in helium nanodroplets is explored by a combination of fs laser-induced alignment experiments and angulon quasiparticle theory. We demonstrate that at low fluence of the fs alignment pulse, the molecule and its solvation shell can be set into coherent collective rotation lasting long enough to form revivals. With increasing fluence, however, the revivals disappear-instead, rotational dynamics as rapid as for an isolated molecule is observed during the first few picoseconds. Classical calculations trace this phenomenon to transient decoupling of the molecule from its helium shell. Our results open novel opportunities for studying nonequilibrium solute-solvent dynamics and quantum thermalization.

Deformation of a Quantum Many-Particle System by a Rotating Impurity

During the last 70 years, the quantum theory of angular momentum has been successfully applied to describing the properties of nuclei, atoms, and molecules, their interactions with each other as well as with external fields. Due to the properties of quantum rotations, the angular momentum algebra can be of tremendous complexity even for a few interacting particles, such as valence electrons of an atom, not to mention larger many-particle systems. In this work, we study an example of the latter: a rotating quantum impurity coupled to a many-body bosonic bath. In the regime of strong impurity-bath couplings the problem involves addition of an infinite number of angular momenta which renders it intractable using currently available techniques. Here, we introduce a novel canonical transformation which allows to eliminate the complex angular momentum algebra from such a class of many-body problems. In addition, the transformation exposes the problems constants of motion, and renders it solvable exactly in the limit of a slowly-rotating impurity. We exemplify the technique by showing that there exists a critical rotational speed at which the impurity suddenly acquires one quantum of angular momentum from the many-particle bath. Such an instability is accompanied by the deformation of the phonon density in the frame rotating along with the impurity.

Strongly aligned molecules inside helium droplets in the near-adiabatic regime

Iodine (I2) molecules embedded in He nanodroplets are aligned by a 160 ps long laser pulse. The highest degree of alignment, occurring at the peak of the pulse and quantified by ⟨cos2𝜃2D⟩, is measured as a function of the laser intensity. The results are well described by ⟨cos2𝜃2D⟩ calculated for a gas of isolated molecules each with an effective rotational constant of 0.6 times the gas-phase value and at a temperature of 0.4 K. Theoretical analysis using the angulon quasiparticle to describe rotating molecules in superfluid helium rationalizes why the alignment mechanism is similar to that of isolated molecules with an effective rotational constant. A major advantage of molecules in He droplets is that their 0.4 K temperature leads to stronger alignment than what can generally be achieved for gas phase molecules-here demonstrated by a direct comparison of the droplet results to measurements on a ∼1 K supersonic beam of isolated molecules. This point is further illustrated for a more complex system by measurements on 1,4-diiodobenzene and 1,4-dibromobenzene. For all three molecular species studied, the highest values of ⟨cos2𝜃2D⟩ achieved in He droplets exceed 0.96.

Dissipative binding of atoms by non-conservative forces

The formation of molecules and supramolecular structures results from bonding by conservative forces acting among electrons and nuclei and giving rise to equilibrium configurations defined by minima of the interaction potential. Here we show that bonding can also occur by the non-conservative forces responsible for interaction-induced coherent population trapping. The bound state arises in a dissipative process and manifests itself as a stationary state at a preordained interatomic distance. Remarkably, such a dissipative bonding is present even when the interactions among the atoms are purely repulsive. The dissipative bound states can be created and studied spectroscopically in present-day experiments with ultracold atoms or molecules and can potentially serve for cooling strongly interacting quantum gases.

Shaping interactions between polar molecules with far-off-resonant light

We show that dressing polar molecules with a far-off-resonant optical field leads to new types of intermolecular potentials, which undergo a crossover from the inverse power to oscillating behavior depending on the intermolecular distance, and whose parameters can be tuned by varying the laser intensity and wavelength. We present analytic expressions for the potential energy surfaces, thereby providing direct access to the parameters of an optical field required to design intermolecular interactions experimentally.

Rotation of cold molecular ions inside a Bose-Einstein condensate

We use recently developed angulon theory [Phys. Rev. Lett. 114, 203001 (2015)] to study the rotational spectrum of a cyanide molecular anion immersed into Bose-Einstein condensates of rubidium and strontium. Based on

Fine-tuning molecular energy levels by nonresonant laser pulses

\textit {ab initio}