The rapidly rotational motion of C$_{60}$ molecules provides us with an ingenious way to test Mashhoon's spin-rotation coupling. The spin-rotation coupling of electrons in the rotating C$_{60}$ molecule is considered in the present letter. It is shown that the intrinsic spin (gravitomagnetic moment) of the electron that can be coupled to the time-dependent rotating frequency of rotating frame of reference (C$_{60}$ molecule) results in a geometric phase, which may be measured through the electronic energy spectra of C$_{60}$ molecules.
We investigate the dynamics of a rotating Morse wave packet, appropriate for a ro-vibrating diatomic molecule. The coupling between vibrational and rotational degrees of freedom is explicated in real position space as well as in phase space Wigner distribution of a SU(2) coherent state at various dynamically evolved times. We choose the well studied $I_{2}$ molecule with the parameter values in good agrement with experiments. A quantitative measure of the angles of rotations for different angular momenta is also given.
The Tietz-Hua (TH) potential is one of the very best analytical model potentials for the vibrational energy of diatomic molecules. By using the Nikiforov-Uvarov (NU) method, we have obtained the exact analytical s-wave solutions of the radial Schrödinger equation (SE) for the TH potential. The energy eigenvalues and the corresponding eigenfunctions are calculated in closed forms. Some numerical results for diatomic molecules are also presented.
We study the classical and quantum rotation numbers of the free rotation of asymmetric top molecules. We show numerically that the quantum rotation number converges to its classical analog in the semi-classical limit. Different asymmetric molecules such as the water molecule are taken as illustrative example. A simple approximation of the classical rotation number is derived in a neighborhood of the separatrix connecting the two unstable fixed points of the system. Furthermore, a signature of the classical tennis racket effect in the spectrum of asymmetric molecules is identified.
The dynamics of non-polar diatomic molecules interacting with a far-detuned narrow-band laser field, that only may drive rotational transitions, is studied. The rotation of the molecule is considered both classically and quantum mechanically, providing links to features known from the heavy symmetric top. In particular, quantum decoherence in the molecular rotation, being induced by spontaneous Raman processes, is addressed. It is shown how this decoherence modifies the rotational dynamics in phase space.
We propose an implementation scheme for the continuous-time quantum walk using a diatomic molecule and an optical frequency comb. We show an analogy between the quantum walk and the cascade rotational transitions induced by the optical frequency comb whose frequency peaks are tuned to the pure rotational transitions in the molecule. The strategy to compensate for the centrifugal distortion of the real molecule is also demonstrated.
A general scheme for rotational cooling of diatomic heteronuclear molecules is proposed. It uses a superconducting microwave cavity to enhance the spontaneous decay via Purcell effect. Rotational cooling can be induced by sequentially tuning each rotational transition to cavity resonance, starting from the highest transition level to the lowest using an electric field. Electrostatic multipoles can be used to provide large confinement volume with essentially homogeneous background electric field.
We obtained a simple theoretical unified parameter for the characterization of rotational population propagation of diatomic molecules in a periodic train of resonant optical pulses. The parameter comprises the peak intensity and interval between the pulses, and the level energies of the initial and final rotational states of the molecule. Using the unified parameter, we can predict the upper and lower boundaries of probability localization on the rotational level network, including the effect of centrifugal distortion. The unified parameter was tentatively derived from an analytical expressio…
We propose a quantum computer architecture which is robust against decoherence and scalable. As a qubit, we adopt rotational states of a nonpolar ionic molecule trapped in an ion-trap. It is revealed that the rotational-state qubits are much more immune to decoherence than the conventional electronic-state qubits of atomic ions. A complete method set for state preparation, single-qubit gate, controlled-NOT gate, and qubit-readout suitable for the rotational-state qubits is provided. Since the ionic molecules can be transported in an array of ion traps, the rotational-state qubits are expected …
We present arguments demonstrating that the application of the Nikiforov-Uvarov polynomial method to solve the Schrödinger equation with the Tietz-Hua potential is valid only when $e^{-b_{h}r_{e}}\leq c_{h}<1$ and $r_{0}<r<+\infty $. In particular, it is pointed out that the numerical results with $c_{h}\neq 0$ for the diatomic molecules $\mathrm{HF}$, $\mathrm{N}_{2}$, $\mathrm{I}_{2}$, $\mathrm{H}_{2}$, $\mathrm{O}_{2}$ and $\mathrm{O}_{2}^{+}$ given in Tables 3-5 by Hamzavi and co-workers are wrong. When $-1\leq c_{h}<0$ or $0<c_{h}<e^{-b_{h}r_{e}}$, this approach is not suitable. In both c…
The interaction of quantum light with matter like that inside a cavity is known to give rise to mixed light-matter states called polaritons. We discuss the impact of rotation of the cavity on the polaritons. It is shown that the number of polaritons increases due to this rotation. The structure of the original polaritons is modified and new ones are induced by the rotation that strongly depend on the angular velocity and the choice of axis of rotation. In molecules the rotation can change the number of light-induced conical intersections and their dimensionality and hence strongly impact their…
A beam of diatomic molecules scattered off a standing wave laser mode splits according to the rovibrational quantum state of the molecules. Our numerical calculation shows that single state resolution can be achieved by properly tuned, monochromatic light. The proposed scheme allows for selecting non-vibrating and non-rotating molecules from a thermal beam, implementing a laser Maxwell's demon to prepare a rovibrationally cold molecular ensemble.
The amplitude and probability of quantum transitions are represented as a path integrals in energy state space of the investigated multi-level quantum system. Using this approach we consider rotational dynamics of nitrogen molecules $^{14}N_{2}$ and $^{15}N_{2}$ which interact with a sequence of ultrashort laser pulses. Our computer simulations indicate the complex dependency of the high rotation states excitation probability upon ultrashort laser pulses sequence periods. We observe pronounced resonances, which correspond to the results of some experiments.
We provide a theory of the deflection of polar and non-polar rotating molecules by inhomogeneous static electric field. Rainbow-like features in the angular distribution of the scattered molecules are analyzed in detail. Furthermore, we demonstrate that one may efficiently control the deflection process with the help of short and strong femtosecond laser pulses. In particular the deflection process may by turned-off by a proper excitation, and the angular dispersion of the deflected molecules can be substantially reduced. We study the problem both classically and quantum mechanically, taking i…
We consider deflection of rotating symmetric molecules by inhomogeneous optical and static electric fields, compare results with the case of linear molecules, and find new singularities in the distribution of the scattering angle. Scattering of the prolate/oblate molecules is analyzed in detail, and it is shown that the process can be efficiently controlled by means of short and strong femtosecond laser pulses. In particular, the angular dispersion of the deflected molecules may be dramatically reduced by laser-induced molecular pre-alignment. We first study the problem by using a simple class…
An antiferromagnetically exchange-coupled dimer of single molecule magnets which possesses a large spin tunneling has been investigated. For this system the ground and first excited states are entangled states and the Hamiltonian is effectively similar to that of a two-state system at $2s^{\text{th}}$ order in perturbation theory, thus this system can be mapped to an entangled pseudospin 1/2 particles. We study the effects of interaction and rotation of this system about its staggered easy-axis direction . The corresponding Hamiltonian of a rotated two-state entangled spin system is derived wi…
A rigorous quantum description of molecular dynamics with a particular emphasis on internal observables is developed accounting explicitly for kinetic couplings between nuclei and electrons. Rotational modes are treated in a genuinely quantum framework by defining a molecular orientation operator. Canonical rotational commutation relations are established explicitly. Moreover, physical constraints are imposed on the observables in order to define the state of a molecular system located in the neighborhood of the ground state defined by the equilibrium condition.
In [14] Duca and Nersesyan proved a small-time controllability property of nonlinear Schrödinger equations on a d-dimensional torus $\mathbb{T}^d$. In this paper we study a similar property, in the linear setting, starting from a closed Riemannian manifold. We then focus on the 2-dimensional sphere $S^2$, which models the bilinear control of a rotating linear top: as a corollary, we obtain the approximate controllability in arbitrarily small times among particular eigenfunctions of the Laplacian of $S^2$.
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 experimentally study the optical- and terahertz- induced rotational dynamics of asymmetric molecules in the gas phase. Terahertz and optical fields are identified as two distinct control handles over asymmetric molecules, as they couple to the rotational degrees of freedom via the molecular- dipole and polarizability selectively. The distinction between those two rotational handles is highlighted by different types of quantum revivals observed in long duration (>100ps) field-free rotational evolution. The experimental results are in excellent agreement with Random Phase Wave Function simula…
We analyze in detail the possibility to use charge-dipole interaction between a single polar molecule or a 1D molecular array and a single Rydberg atom to read out rotational populations. The change in the Rydberg electron energy is conditioned on the rotational state of the polar molecules, allowing for realization of a CNOT quantum gate between the molecules and the atom. Subsequent readout of the atomic fluorescence results in a non-destructive measurement of the rotational state. We study the interaction between a 1D array of polar molecules and an array or a cloud of atoms in a Rydberg su…
We study the influence of the rotations and vibrations of the symmetric top RaOCH$_3$ molecule on its effectiveness as a probe for the $\mathcal{P}$ and $\mathcal{T}$-violating effects, such as the electron electric dipole moment (eEDM) and the scalar-pseudoscalar electron-nucleon interaction (Ne-SPS). The corresponding enhancement parameters $E_{\rm eff}$ and $E_{\rm s}$ are computed for the ground and first excited rovibrational states with different values of the angular momentum component $K$. For the lowest $K$-doublet with $v_\perp=0$ and $K=1$ the values are $E_{\rm eff}=47.647\,\mathrm…
We discuss the rotational cooling of diatomic molecules in a Bose-Einstein condensate (BEC) of ultra-cold atoms by emission of phonons with orbital angular momentum. Despite the superfluidity of the BEC there is no frictionless rotation for typical molecules since the dominant cooling occurs via emission of particle-like phonons. Only for macro-dimers, whose size becomes comparable or larger than the condensate healing length, a Landau-like, critical angular momentum exists below which phonon emission is suppressed. We find that the rotational relaxation of typical molecules is in general fast…
We argue that certain materials exhibit asymmetry of their mechanical and conducting properties with respect to clockwise/counterclockwise rotation. We show that a cylinder made of a suitably chosen semiconductor coated in a metallic film and placed in the magnetic-field background can serve as a "rotational diode" which conducts electricity only at a specific range of angular frequencies. The critical angular frequency and the direction of rotation can be tuned with the magnetic field's strength. Mechanically, the rotational diode possesses different moments of inertia when rotated in clockwi…
In this paper we study the controllability problem for a symmetric-top molecule, both for its classical and quantum rotational dynamics. The molecule is controlled through three orthogonal electric fields interacting with its electric dipole. We characterize the controllability in terms of the dipole position: when it lies along the symmetry axis of the molecule neither the classical nor the quantum dynamics are controllable, due to the presence of a conserved quantity, the third component of the total angular momentum; when it lies in the orthogonal plane to the symmetry axis, a quantum symme…
By making use of the quantization rule of Raab and Friedrich [P. Raab and H. Friedrich, Phys. Rev. A 78, 022707 (2008)], we derive simple and accurate formulae for the number of rotational states supported by a weakly-bound vibrational level of a diatomic molecule and the rotational constants of any such levels up to the threshold, and provide a criterion for determining whether a given weakly-bound vibrational level is rotationless. The results depend solely on the long-range part of the molecular potential and are applicable to halo molecules.
We analyze theoretically the interplay between the torsional and the rotational motion of an aligned biphenyl-like molecule. To do so, we consider a transition between two electronic states with different internal torsional potentials, induced by means of a resonant laser pulse. The change in the internal torsional potential provokes the motion of the torsional wavepacket in the excited electronic state, modifying the structure of the molecule, and hence, its inertia tensor. We find that this process has a strong impact on the rotational wave function, displaying different behavior depending o…
This article covers few selected aspects of quantum theory of molecular rotations and vibrations. Triatomic molecules are the simplest systems, which show qualitative characteristics of larger polyatomic molecules. On the minimal example of triatomic molecules we demonstrate several theoretical methods used to calculate highly accurate rotational-vibrational-electronic energies, wavefunctions and transition intensities. The reader can view this article as a tutorial, by no means comprehensive, which still touches some of the unsolved problems in modern theoretical molecular spectroscopy.
We investigate experimentally the effect of quantum resonance in the rotational excitation of the simplest quantum rotor - a diatomic molecule. By using the techniques of high-resolution femtosecond pulse shaping and rotational state-resolved detection, we measure directly the amount of energy absorbed by molecules interacting with a periodic train of laser pulses, and study its dependence on the train period. We show that the energy transfer is significantly enhanced at quantum resonance, and use this effect for demonstrating selective rotational excitation of two nitrogen isotopologues, $ ^{…
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 …
Detecting the internal state of polar molecules is a substantial challenge when standard techniques such as resonance-enhanced multi photon ionization (REMPI) or laser-induced fluorescense (LIF) do not work. As this is the case for most polyatomic molecule species, we here investigate an alternative based on state selective removal of molecules from an electrically trapped ensemble. Specifically, we deplete molecules by driving rotational and/or vibrational transitions to untrapped states. Fully resolving the rotational state with this method can be a considerable challenge as the frequency di…
We study theoretically the collective dynamics of rotational excitations of polar molecules loaded into an optical lattice in two dimensions. These excitations behave as hard-core bosons with a relativistic energy dispersion arising from the dipolar coupling between molecules. This has interesting consequences for the collective many-body phases. The rotational excitations can form a Bose-Einstein condensate at non-zero temperature, manifesting itself as a divergent $T_2$ coherence time of the rotational transition even in the presence of inhomogeneous broadening. The dynamical evolution of a …
We discuss the friction experienced by the body rotating in superfluid liquid at T=0. The effect is analogous to the amplification of electromagnetic radiation and spontaneous emission by the body or black hole rotating in quantum vacuum, first discussed by Zel'dovich and Starobinsky. The friction is caused by the interaction of the part of the liquid, which is rigidly connected with the rotating body and thus represents the comoving detector, with the "Minkowski" vacuum outside the body. The emission process is the quantum tunneling of quasiparticles from the detector to the ergoregion, where…
Ultracold polar molecules trapped on an optical lattice is a many-body system that, under appropriate conditions, may support collective excitations reminiscent of excitons in solid state crystals. Here, we discuss the rotational excitations of molecules on an optical lattice leading to rotational Frenkel excitons. Apart from solid hydrogen, there is no other natural system that exhibits rotational excitons. The rotational excitons have unique properties that can be exploited for tuning non-linear exciton interactions and exciton-impurity scattering by applying an external electric field. We s…
We propose a set of devices of simple geometrical design which may exhibit a permanent rotation due to quantum (vacuum) fluctuations. These objects - which have no moving parts - impose certain boundary conditions on quantum fluctuations thus affecting their vacuum energy similarly to the standard Casimir effect. The boundary conditions are chosen in such a way that the vacuum energy for a static device is larger compared to the energy of the vacuum fluctuations in a state when the device rotates about a certain axis. The optimal frequency of rotation is determined by geometry and moment of in…
The rotational dynamics of particles subject to external illumination is found to produce light amplification and inelastic scattering at high rotation velocities. Light emission at frequencies shifted with respect to the incident light by twice the rotation frequency dominates over elastic scattering within a wide range of light and rotation frequencies. Remarkably, net amplification of the incident light is produced in this classical linear system via stimulated emission. Large optically-induced acceleration rates are predicted in vacuum accompanied by moderate heating of the particle, thus …
We combine experimental and theoretical approaches to explore excited rotational states of molecules embedded in helium nanodroplets using CS$_2$ and I$_2$ as examples. Laser-induced nonadiabatic molecular alignment is employed to measure spectral lines for rotational states extending beyond those initially populated at the 0.37 K droplet temperature. We construct a simple quantum mechanical model, based on a linear rotor coupled to a single-mode bosonic bath, to determine the rotational energy structure in its entirety. The calculated and measured spectral lines are in good agreement. We show…
