We analyze the alignment of molecules generated by a pair of crossed ultra-short pump pulses of different polarizations by a technique based on the induced time-dependent gratings. Parallel polarizations yield an intensity grating, while perpendicular polarizations induce a polarization grating. We show that both configurations can be interpreted at moderate intensity as an alignment induced by a single polarized pump pulse. The advantage of the perpendicular polarizations is to give a signal of alignment that is free from the plasma contribution. Experiments on femtosecond transient gratings with aligned molecules were performed in CO2 at room temperature in a static cell and at 30 K in a molecular expansion jet.
Quantum reflection is a universal property of atoms and molecules when scattered from surfaces in ultracold collisions. Recent experimental work has documented the quantum reflection and diffraction of He atoms, dimers, trimers and Neon atoms when reflected from a grating. Conditions for the observation of emerging beam resonances have been discussed and measured. In this paper, we provide a theoretical simulation of the quantum reflection in these cases from a grating. We confirm, as expected the universal dependence on the incident de Broglie wavelength only of the threshold angles for the o…
We extend the theory of matter-wave interferometry of point-like particles to non-spherical objects by taking the orientational degrees of freedom into account. In particular, we derive the grating transformation operator, that maps the impinging state onto the outgoing state, for a general, orientation-dependent interaction potential between the grating and the molecule. The grating operator is then worked out for the diffraction of symmetric top molecules from standing light waves, and the resulting interference pattern is calculated in the near-field. This allows us to identify a signature …
We present a theory for the diffraction of large molecules or nanoparticles at a standing light wave. Such particles can act as a genuine photon absorbers due to their numerous internal degrees of freedom effecting fast internal energy conversion. Our theory incorporates the interplay of three light-induced properties: the coherent phase modulation due to the dipole interaction, a non-unitary absorption-induced amplitude modulation described as a generalized measurement, and a coherent recoil splitting that resembles a quantum random walk in steps of the photon momentum. We discuss how these e…
By modulating transmission function of a weak probe field via a strong control standing wave, an electromagnetically induced grating can be created in the probe channel. Such a nonmaterial grating may lead to self-imaging of ultra-cold atoms or molecules in the Fresnel near-field regime. This work may offer a nondestructive and lensless way to image ultra-cold atoms or molecules.
Matter-wave interferometry with atoms and molecules has attracted a rapidly growing interest over the past two decades, both in demonstrations of fundamental quantum phenomena and in quantum-enhanced precision measurements. Such experiments exploit the non-classical superposition of two or more position and momentum states which are coherently split and rejoined to interfere. Here, we present the experimental realization of a universal near-field interferometer built from three short-pulse single-photon ionization gratings. We observe quantum interference of fast molecular clusters, with a com…
We demonstrate a 2-grating free electron Mach-Zehnder interferometer constructed in a transmission electron microscope. A symmetric binary phase grating and condenser lens system forms two spatially separated, focused probes at the sample which can be scanned while maintaining alignment. The two paths interfere at a second grating, creating in constructive or destructive interference in output beams. This interferometer has many notable features: positionable probe beams, large path separations relative to beam width, continuously tunable relative phase between paths, and real-time phase infor…
We present a theoretical study of the time-dependent laser alignment of molecules taking into account the hyperfine coupling due to nuclear-quadrupole interactions. The coupling of nuclear spins to the overall angular momentum of molecules significantly influences their rotational dynamics. Here, we systematically analyze the impact of the nuclear-quadrupole coupling on the rotational dynamics of the linear $\text{I}_2$ and the asymmetric-top diiodobenzene molecule induced by external laser fields. We explore different regimes of pulse shapes and laser-pulse intensities and detail under which …
Path integrals give a possibility to compute in details routes of particles from particle sources through slit gratings and further to detectors. The path integral for a particle passing through the Gaussian slit results in the Gaussian wavepacket. The wavepackets prepared on N slits and superposed together give rise to interference pattern in the near-field zone. It transforms to diffraction in the far-field zone represented by divergent principal rays, at that all rays are partitioned from each other by (N-2) subsidiary rays. The Bohmian trajectories in the near-field zone of N-slit gratings…
We explore the electronic structure and rovibrational properties of an ultralong-range triatomic Rydberg molecule formed by a Rydberg atom and a ground state heteronuclear diatomic molecule. We focus here on interaction of Rb($27s$) Rydberg atom with KRb($N=0$) diatomic polar molecule. There's significant electronic hybridization of Rb($n=24$, $l\ge 3$) degenerate manifold. The polar diatomic molecule is allowed to rotate in the electric fields generated by the Rydberg electron and core as well as an external field. We investigate the metamorphosis of the Born-Oppenheimer potential curves, ess…
We present a novel design of optical micro-cavity where the optical energy resides primarily in free space, therefore is readily accessible to foreign objects such as atoms, molecules, mechanical resonators, etc. We describe the physics of these resonators, and propose a design method based on stochastic optimization. Cavity designs with diffraction-limited mode volumes and quality factors in the range of $10^4$--$10^6$ are presented. With a purely planar geometry, the cavity can be easily integrated on-chip using conventional micro- and nano- fabrication processes.
The fringe pattern that allows geometrical and orbital structure information to be extracted from LIED spectra of symmetric molecules is shown to reflect a symmetry conservation principle. We show that under a field polarization which preserves certain symmetry elements of the molecule, the symmetry character of the initial wave function is conserved during its time-evolution. We present a symmetry analysis of a deviation from a perfect alignment by decomposing the field into a major, symmetry-determining part, and a minor, symmetry breaking, part. This decomposition leads to a corresponding f…
We introduce a new optical tool - a "two-dimensional optical centrifuge", capable of aligning molecules in extreme rotational states. Unlike the conventional centrifuge, which confines the molecules in the plane of their rotation, its two-dimensional version aligns the molecules along a well-defined axis, similarly to the effect of a single linearly polarized laser pulse, but at a much higher level of rotational excitation. The increased robustness of ultra-high rotational states with respect to collisions results in a longer life time of the created alignment in dense media, offering new poss…
We develop two novel models of the H$_2^+$ molecule and its isotopes from which we assess quantum-mechanically and semi-classically whether the molecule anti-aligns with the field in the first excited electronic state. The results from both models allow us to predict anti-alignment dynamics even for the HD$^+$ isotope, which possesses a permanent dipole moment. The molecule dissociates at angles perpendicular to the field polarization in both the excited and the ground electronic state, as the population is exchanged through a conical intersection. The quantum mechanical dispersion of the init…
We consider deflection of polarizable molecules by inhomogeneous optical fields, and analyze the role of molecular orientation and rotation in the scattering process. It is shown that molecular rotation induces spectacular rainbow-like features in the distribution of the scattering angle. Moreover, by preshaping molecular angular distribution with the help of short and strong femtosecond laser pulses, one may efficiently control the scattering process, manipulate the average deflection angle and its distribution, and reduce substantially the angular dispersion of the deflected molecules. We pr…
We investigate the structure and features of an ultralong-range triatomic Rydberg molecule formed by a Rb Rydberg atom and a KRb diatomic molecule. In our numerical description, we perform a realistic treatment of the internal rotational motion of the diatomic molecule, and take into account the Rb($n, l\ge 3$) Rydberg degenerate manifold and the energetically closest neighboring levels with principal quantum numbers $n'>n$ and orbital quantum number $l\le2$. We focus here on the adiabatic electronic potentials evolving from the Rb($n, l\ge 3$) and Rb($n=26, l=2$) manifolds. The directional pr…
Machine learning for predicting control landscape maps of quantum molecular dynamics: Laser-induced three-dimensional alignment of asymmetric top molecules
Photoassociation of ultracold atoms is shown to lead to alignment of the product molecules along the excitation laser polarization axis. We theoretically investigate pulsed photoassociation of $^{87}Rb$ atoms into a specific weakly-bound level of the a $^3Σ_u^+$ metastable electronic state and find both stationary and time-dependent field-free alignment. Although a transform-limited pulse yields significant alignment, a frequency-chirped pulse dramatically enhances the molecular formation rate at the cost of a slight decrease in the alignment. Employing multiple pulses synchronized with the vi…
We report on the formation of ultralong-range Rydberg D-state molecules via photoassociation in an ultracold cloud of rubidium atoms. By applying a magnetic offset field on the order of 10 G and high resolution spectroscopy, we are able to resolve individual rovibrational molecular states. A full theory, using the Born-Oppenheimer approximation including s- and p-wave scattering, reproduces the measured binding energies. The calculated molecular wavefunctions show that in the experiment we can selectively excite stationary molecular states with an extraordinary degree of alignment or anti-alig…
We review recent progress and future prospects of matter wave interferometry with complex organic molecules and inorganic clusters. Three variants of a near-field interference effect, based on diffraction by material nanostructures, at optical phase gratings, and at ionizing laser fields are considered. We discuss the theoretical concepts underlying these experiments and the experimental challenges. This includes optimizing interferometer designs as well as understanding the role of decoherence. The high sensitivity of matter wave interference experiments to external perturbations is demonstra…
Coherent control of chaotic molecular systems, using laser-assisted alignment of sulphur dioxide (SO$_2$) molecules in the presence of a static electric field as an example, is considered. Conditions for which the classical version of this system is chaotic are established, and the quantum and classical analogs are shown to be in very good correspondence. It is found that the chaos present in the classical system does not impede the alignment, neither in the classical nor the quantum system. Using the results of numerical calculations, we suggest that laser-assisted alignment is stable against…
We examine the rotational states of a pair of polar $^2Σ$ molecules subject to a uniform magnetic field. The electric dipole-dipole interaction between the molecules creates entangled pair-eigenstates of two types. In one type, the Zeeman interaction between the inherently paramagnetic molecules and the magnetic field destroys the entanglement of the pair-eigenstates, whereas in the other type it does not. The pair-eigenstates exhibit numerous intersections, which become avoided for pair-eigenstates comprised of individual states that meet the selection rules $ΔJ_{i}=0,\pm 1$, $ΔN_{i}=0,\pm 2$…
A theoretical study of the rotational dynamics of a linear polar molecule in a two-color non-resonant cw laser field is presented. By systematically considering the interactions of this field with the electric dipole moment, polarizability and hyperpolarizability of the molecule, the effect of the symmetries of the Hamiltonian on the orientation and alignment is explored in a regime where the time-average approximation does not hold. It is shown that the alignment and orientation satisfy certain symmetries as a function of the phases and field strengths. On average a one-color cw laser field d…
