We introduce a new scheme for controlling the sense of molecular rotation. By varying the polarization and the delay between two ultrashort laser pulses, we induce unidirectional molecular rotation, thereby forcing the molecules to rotate clockwise/counterclockwise under field-free conditions. We show that unidirectionally rotating molecules are confined to the plane defined by the two polarization vectors of the pulses, which leads to a permanent anisotropy in the molecular angular distribution. The latter may be useful for controlling collisional cross-sections and optical and kinetic processes in molecular gases. We discuss the application of this control scheme to individual components within a molecular mixture in a selective manner.
An isotropic medium, having magnetic sublevels, when subjected to a magnetic field or an electromagnetic field can induce anisotropy in the medium; and as a result the plane of polarization of the probe field can rotate. Therefore the rotation due to the magnetic field alone, can be {\em controlled efficiently} with use of a coherent field. We show, using a control field, significant enhancement of the magneto-optical rotation and demonstrate the possibility of realizing {\em magneto-optical switch}.
Semiclassical catastrophes in the dynamics of a quantum rotor (molecule) driven by a strong time-varying field are considered. We show that for strong enough fields, a sharp peak in the rotor angular distribution can be achieved via time-domain focusing phenomenon, followed by the formation of angular rainbows and glory-like angular structures. Several scenarios leading to the enhanced angular squeezing are proposed that use specially designed and optimized sequences of pulses. The predicted effects can be observed in many processes, ranging from molecular alignment (orientation) by laser fiel…
We report on the possibility of controlling quantum random walks with a step-dependent coin. The coin is characterized by a (single) rotation angle. Considering different rotation angles, one can find diverse probability distributions for this walk including: complete localization, Gaussian and asymmetric likes. In addition, we explore the entropy of walk in two contexts; for probability density distributions over position space and walker's internal degrees of freedom space (coin space). We show that entropy of position space can decrease for a step-dependent coin with the step-number, quite …
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…
Photonic topological insulator plates violate Lorentz reciprocity which leads to a directionality of surface-guided modes. This in-plane directionality can be imprinted via an applied magnetic field. On the basis of macroscopic quantum electrodynamics in nonreciprocal media, we show that two photonic topological insulator surfaces are subject to a tuneable, magnetic-field dependent Casimir torque. Due to the directionality, this torque exhibits a unique $2π$ periodicity, in contradistinction to the Casimir torques encountered for reciprocal uniaxial birefringent media or corrugated surfaces wh…
We demonstrate coherent control of both the rotational and hyperfine state of ultracold, chemically stable $^{87}$Rb$^{133}$Cs molecules with external microwave fields. We create a sample of ~2000 molecules in the lowest hyperfine level of the rovibronic ground state N = 0. We measure the transition frequencies to 8 different hyperfine levels of the N = 1 state at two magnetic fields ~23 G apart. We determine accurate values of rotational and hyperfine coupling constants that agree well with previous calculations. We observe Rabi oscillations on each transition, allowing complete population tr…
Recently, it was predicted theoretically and verified experimentally that a pair of delayed and cross-polarized short laser pulses can create molecular ensembles with a well defined sense of rotation (clockwise or counterclockwise). Here we provide a comparative study of the classical and quantum aspects of the underlying mechanism for linear molecules and for symmetric tops, like benzene molecules, that were used for the first experimental demonstration of the effect. Very good quantitative agreement is found between the classical description of the process and the rigorous quantum mechanical…
Sagnac interferometers with massive particles promise unique advantages in achieving high precision measurements of rotation rates over their optical counterparts. Recent proposals and experiments are exploring non-ballistic Sagnac interferometers where trapped atoms are transported along a closed path. This is achieved by using superpositions of internal quantum states and their control with state-dependent potentials. We address emergent questions regarding the dynamical behavior of Bose-Einstein condensates in such an interferometer and its impact on rotation sensitivity. We investigate com…
Laser control of molecular rotation is an area of active research. A number of recent studies has aimed at expanding the reach of rotational control to extreme, previously inaccessible rotational states, as well as controlling the directionality of molecular rotation. Dense ensembles of molecules undergoing ultrafast uni-directional rotation, known as molecular superrotors, are anticipated to exhibit unique properties, from spatially anisotropic diffusion and vortex formation to the creation of powerful acoustic waves and tuneable THz radiation. Here we describe our recent progress in controll…
We treat control of several two-level atoms interacting with one mode of the electromagnetic field in a cavity. This provides a useful model to study pertinent aspects of quantum control in infinite dimensions via the emergence of infinite-dimensional system algebras. Hence we address problems arising with infinite-dimensional Lie algebras and those of unbounded operators. For the models considered, these problems can be solved by splitting the set of control Hamiltonians into two subsets: The first obeys an abelian symmetry and can be treated in terms of infinite-dimensional Lie algebras and …
We investigate theoretically the interaction of polar molecules with optical lattices and microwave fields. We demonstrate the existence of frequency windows in the optical domain where the complex internal structure of the molecule does not influence the trapping potential of the lattice. In such frequency windows the Franck-Condon factors are so small that near-resonant interaction of vibrational levels of the molecule with the lattice fields have a negligible contribution to the polarizability and light-induced decoherences are kept to a minimum. In addition, we show that microwave fields c…
In the framework of optical quantum computing and communications, a major objective consists in building receiving nodes that implement conditional operations on incoming photons, using the interaction with a single stationary qubit. In particular, the quest for scalable nodes motivated the development of cavity-enhanced spin-photon interfaces with solid-state emitters. An important challenge remains, however, to produce a stable, controllable, spin-dependant photon state, in a deterministic way. Here we use a pillar-based high-Q cavity, embedding a singly-charged semiconductor quantum dot, to…
We show that detuned optical pulse trains with a modest spectral width can polarize nuclear spins in InAs quantum dots. The pulse bandwidth is large enough to excite a coherent superposition of both electron spin eigenstates in these negatively charged dots but narrow enough to give partial spectral selectivity between the eigenstates. The coherent precession of electron spin states and periodic excitation focuses the nuclear spin distribution, producing a discrete set of precession modes. The spectral selectivity generates a net nuclear polarization, through a mechanism that relies on optical…
By applying a circularly polarized and slightly blue-detuned microwave field with respect to the first excited rotational state of a dipolar molecule, one can engineer a long-range, shallow potential well in the entrance channel of the two colliding partners. As the applied microwave ac-field is increased, the long-range well becomes deeper and can support a certain numbers of bound states, which in turn bring the value of the molecule-molecule scattering length from a large negative value to a large positive one. We adopt an adimensional approach where the molecules are described by a rescale…
Ultracold molecules trapped in optical tweezers show great promise for the implementation of quantum technologies and precision measurements. We study a prototypical scenario where two interacting polar molecules placed in separate traps are controlled using an external electric field. This, for instance, enables a quantum computing scheme in which the rotational structure is used to encode the qubit states. We estimate the typical operation timescales needed for state engineering to be in the range of few microseconds. We further underline the important role of the spatial structure of the tw…
Controlling the internal degrees of freedom is a key challenge for applications of cold and ultracold molecules. Here, we demonstrate rotational-state cooling of trapped methyl fluoride molecules (CH3F) by optically pumping the population of 16 M-sublevels in the rotational states J=3,4,5, and 6 into a single level. By combining rotational-state cooling with motional cooling, we increase the relative number of molecules in the state J=4, K=3, M=4 from a few percent to over 70%, thereby generating a translationally cold (~30mK) and nearly pure state ensemble of about 10^6 molecules. Our scheme …
We present an analysis of two experimental approaches to controlling the directionality of molecular rotation with ultrashort laser pulses. The two methods are based on the molecular interaction with either a pair of pulses (a "double kick" scheme) or a longer pulse sequence (a "chiral pulse train" scheme). In both cases, rotational control is achieved by varying the polarization of and the time delay between the consecutive laser pulses. Using the technique of polarization sensitive resonance-enhanced multi-photon ionization, we show that both methods produce significant rotational directiona…
