arXiv subjects

Roman V. Krems

Publications and source records attributed to Roman V. Krems.

At least 55 records · Page 3Linked to original sources

arXiv2015

Gaussian Process Model for Collision Dynamics of Complex Molecules

We show that a Gaussian Process model can be combined with a small number (of order 100) of scattering calculations to provide a multi-dimensional dependence of scattering observables on the experimentally controllable parameters such as the collision energy or temperature) as well as the potential energy surface (PES) parameters. For the case of Ar - C$_6$H$_6$ collisions, we show that 200 classical trajectory calculations are sufficient to provide a 10-dimensional hypersurface, giving the dependence of the collision lifetimes on the collision energy, internal temperature and 8 PES parameters. This can be used for solving the inverse scattering problem, the efficient calculation of thermally averaged observables, for reducing the error of the molecular dynamics calculations by averaging over the PES variations, and the analysis of the sensitivity of the observables to individual parameters determining the PES.Trained by a combination of classical and quantum calculations, the model provides an accurate description of the quantum scattering cross sections, even near scattering resonances.

physics.chem-ph↗

arXiv2015

Quantum walk and Anderson localization of rotational excitations in disordered ensembles of polar molecules

We consider the dynamics of rotational excitations placed on a single molecule in spatially disordered 1D, 2D and 3D ensembles of ultracold molecules trapped in optical lattices. The disorder arises from incomplete populations of optical lattices with molecules. This leads to a model corresponding to a quantum particle with long-range tunnelling amplitudes moving on a lattice with the same on-site energy but with forbidden access to random sites (vacancies). We examine the time and length scales of Anderson localization for this type of disorder with realistic experimental parameters in the Hamiltonian. We show that for an experimentally realized system of KRb molecules on an optical lattice this type of disorder leads to disorder-induced localization in 1D and 2D systems on a time scale $t \sim 1$ sec. For 3D lattices with $55$ sites in each dimension and vacancy concentration $ 90~\%$, the rotational excitations diffuse to the edges of the lattice and show no signature of Anderson localization. We examine the role of the long-range tunnelling amplitudes allowing for transfer of rotational excitations between distant lattice sites. Our results show that the long-range tunnelling has little impact on the dynamics in the diffusive regime but affects significantly the localization dynamics in lattices with large concentrations of vacancies, enhancing the width of the localized distributions in 2D lattices by more than a factor of 2. Our results raise a general question whether quantum particles with long-range tunnelling can undergo quantum localization in 3D lattices with substitutional disorder.

cond-mat.quant-gas↗

arXiv2014

Magnetic Feshbach resonances in collisions of non-magnetic closed-shell $^1Σ$ molecules

Magnetic Feshbach resonances play a central role in experimental research of atomic gases at ultracold temperatures, as they allow one to control the microscopic interactions between ultracold atoms by tuning an applied magnetic field. These resonances arise due to strong hyperfine interactions between the unpaired electron and the nuclear magnetic moment of the alkali metal atoms. A major thrust of current research is to create an ultracold gas of diatomic alkali-metal molecules in the ground rovibrational state of the ground electronic $^1Σ$ state. Unlike alkali metal atoms, $^1Σ$ diatomic molecules have no unpaired electrons. However, the hyperfine interactions of molecules may give rise to magnetic Feshbach resonances. We use quantum scattering calculations to study the possible width of these resonances. Our results show that the widths of magnetic Feshbach resonances in ultracold molecule-molecule collisions for $^1Σ$ molecules may exceed 1 milliGauss, rendering such resonances experimentally detectable. We hope that this work will stimulate the experimental search of these resonances.

physics.atom-ph↗

arXiv2013

Chemical reactions of ultracold alkali-metal dimers in the lowest-energy $^3Σ$ state

We show that the interaction of polar alkali dimers in the quintet spin state leads to the formation of a deeply bound reaction complex. The reaction complex can decompose adiabatically into homonuclear alkali dimers (for all molecules except KRb) and into alkali trimers (for all molecules). We show that there are no barriers for these chemical reactions. This means that all alkali dimers in the $a^3Σ^+$ state are chemically unstable at ultracold temperature, and the use of an optical lattice to segregate the molecules and suppress losses may be necessary. In addition, we calculate the minimum energy path for the chemical reactions of alkali hydrides. We find that the reaction of two molecules is accelerated by a strong attraction between the alkali atoms, leading to a barrierless process that produces hydrogen atoms with large kinetic energy. We discuss the unique features of the chemical reactions of ultracold alkali dimers in the $a^3Σ^+$ electronic state.

physics.atom-ph↗

arXiv2013

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 organization 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 853 references.

physics.atom-ph↗

arXiv2013

Elastic and inelastic collisions of $^2Σ$ molecules in a magnetic field

We calculate the cross sections for elastic scattering and Zeeman relaxation in binary collisions of molecules in the ro-vibrational ground state of a $^2Σ$ electronic state and the Zeeman state with the electron spin projection $M_S=1/2$ on the magnetic field axis. This is the lowest-energy state of $^2Σ$ molecules confined in a magnetic trap. The results are averaged over calculations with multiple molecule - molecule interaction potentials, which yields the expectation intervals for the cross sections and the elastic-to-inelastic cross section ratios. We find that the elastic-to-inelastic cross section ratios under conditions corresponding to trapped molecular ensembles at $T \sim 10^{-3}$ K exceed 100 for the majority of $^2Σ$ molecules. The range of $^2Σ$ molecules expected to be collisionally unstable in magnetic traps at $T < 10^{-3}$ K is limited to molecules with the spin-rotation interaction constant $γ_{\rm SR} > 0.5$ cm$^{-1}$ and the rotational constant $B_e < 4$ cm$^{-1}$.

physics.chem-ph↗

arXiv2013

Non-adiabatic control of quantum energy transfer in ordered and disordered arrays

An elementary excitation in an aggregate of coupled particles generates a collective excited state. We show that the dynamics of these excitations can be controlled by applying a transient external potential which modifies the phase of the quantum states of the individual particles. The method is based on an interplay of adiabatic and sudden time scales in the quantum evolution of the many-body states. We show that specific phase transformations can be used to accelerate or decelerate quantum energy transfer and spatially focus delocalized excitations onto different parts of arrays of quantum particles. We consider possible experimental implementations of the proposed technique and study the effect of disorder due to the presence of impurities on its fidelity. We further show that the proposed technique can allow control of energy transfer in completely disordered systems.

quant-ph↗

arXiv2013

Investigating polaron transitions with polar molecules

We determine the phase diagram of a polaron model with mixed breathing-mode and Su-Schrieffer-Heeger couplings and show that it has two sharp transitions, in contrast to pure models which exhibit one (for Su-Schrieffer-Heeger coupling) or no (for breathing-mode coupling) transition. Our results indicate that the physics of realistic mixed polaron models is much richer than that of simplified models. We then show that ultracold molecules trapped in optical lattices can be used to study precisely this mixed Hamiltonian, and that the relative contributions of the two couplings can be tuned with external electric fields. The parameters of current experimental set-ups place them in the region where one of the transitions occurs. We propose a scheme to measure the polaron dispersion using stimulated Raman spectroscopy.

cond-mat.quant-gas↗

arXiv2012

Rotational excitations of polar molecules on an optical lattice: from novel exciton physics to quantum simulation of new lattice models

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 show that this can be used to explore the competing role of the dynamical and kinematic exciton-exciton interactions in excitonic energy transfer and to study quantum localization in a dynamically tunable disordered potential. The rotational excitons can also be used as a basis for quantum simulation of condensed matter models that cannot be realized with ultracold atoms. As an example, we discuss the possibility of engineering the Holstein model with polar molecules on an optical lattice.

physics.atom-ph↗

arXiv2012

Controlling collisional decoherence of ultracold molecules in superposition states by an external magnetic field

We present expressions demonstrating that collisional decoherence of ultracold atoms or molecules in a coherent superposition of non-degenerate quantum states is suppressed when both the real and imaginary parts of the scattering lengths for the states in the coherent superposition are equal. We show that the rate of collisional decoherence can be enhanced or suppressed by varying an external magnetic field near a Feshbach resonance. For some resonances, the suppression is very dramatic. We propose a method for measuring the scattering length of ultracold particles in excited quantum states exhibiting Feshbach resonances.

quant-ph↗

arXiv2012

Sensitive imaging of electromagnetic fields with paramagnetic polar molecules

We propose a method for sensitive parallel detection of low-frequency electromagnetic fields based on the fine structure interactions in paramagnetic polar molecules. Compared to the recently implemented scheme employing ultracold $^{87}$Rb atoms [B{ö}hi \textit{et al.}, Appl. Phys. Lett. \textbf{97}, 051101 (2010)], the technique based on molecules offers a 100-fold higher sensitivity, the possibility to measure both the electric and magnetic field components, and a probe of a wide range of frequencies from the dc limit to the THz regime.

physics.atom-ph↗

arXiv2012

Non-adiabatic 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 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 non-adiabatically 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.

cond-mat.quant-gas↗

arXiv2012

Tunable exciton interactions in optical lattices with polar molecules

Rotational excitation of polar molecules trapped in an optical lattice gives rise to rotational excitons. Here we show that non-linear interactions of such excitons can be controlled by an electric field. The exciton--exciton interactions can be tuned to induce exciton pairing, leading to the formation of biexcitons. Tunable non-linear interactions between excitons can be used for many applications ranging from the controlled preparation of entangled quasiparticles to the study of polaron interactions and the effects of non-linear interactions on quantum energy transport in molecular aggregates.

cond-mat.mes-hall↗

arXiv2011

Tunable Holstein model with cold polar molecules

We show that an ensemble of polar molecules trapped in an optical lattice can be considered as a controllable open quantum system. The coupling between collective rotational excitations and the motion of the molecules in the lattice potential can be controlled by varying the strength and orientation of an external DC electric field as well as the intensity of the trapping laser. The system can be described by a generalized Holstein Hamiltonian with tunable parameters and can be used as a quantum simulator of excitation energy transfer and polaron phenomena. We show that the character of excitation energy transfer can be modified by tuning experimental parameters.

physics.atom-ph↗

arXiv2011

Rotational predissociation of extremely weakly bound atom-molecule complexes produced by Feshbach resonance association

We study the rotational predissociation of atom - molecule complexes with very small binding energy. Such complexes can be produced by Feshbach resonance association of ultracold molecules with ultracold atoms. Numerical calculations of the predissociation lifetimes based on the computation of the energy dependence of the scattering matrix elements become inaccurate when the binding energy is smaller than the energy width of the predissociating state. We derive expressions that represent accurately the predissociation lifetimes in terms of the real and imaginary parts of the scattering length and effective range for molecules in an excited rotational state. Our results show that the predissociation lifetimes are the longest when the binding energy is positive, i.e. when the predissociating state is just above the excited state threshold.

physics.chem-ph↗

arXiv2010

Greatly enhanced absorption of non-resonant microwave fields by ultracold molecules near a Feshbach resonance

We show that the probability of the collision-induced absorption of non-resonant microwave photons by a gas of ultracold molecules is dramatically enhanced near a Feshbach scattering resonance. This can be used for detecting Feshbach resonances of ultracold molecules by measuring the microwave field absorption and for tuning the elastic scattering cross sections of ultracold molecules by varying the frequency and intensity of the microwave field in a wide range of the field parameters.

physics.atom-ph↗

arXiv2010

External field control of collective spin excitations in an optical lattice of $^2Σ$ molecules

We show that an ensemble of $^2Σ$ molecules in the rotationally ground state trapped on an optical lattice exhibits collective spin excitations that can be controlled by applying superimposed electric and magnetic fields. In particular, we show that the lowest energy excitation of the molecular ensemble at certain combinations of electric and magnetic fields leads to the formation of a magnetic Frenkel exciton. The exciton bandwidth can be tuned by varying the electric or magnetic fields. We show that the exciton states can be localized by creating vacancies in the optical lattice. The localization patterns of the magnetic exciton states are sensitive to the number and distribution of vacancies, which can be exploited for engineering many-body entangled spin states. We consider the dynamics of magnetic exciton wavepackets and show that the spin excitation transfer between molecules in an optical lattice can be accelerated or slowed down by tuning an external magnetic or electric field.

physics.chem-ph↗

arXiv2010

Tunable disorder in a crystal of cold polar molecules

In the present work, we demonstrate the possibility of controlling by an external field the dynamics of collective excitations (excitons) of molecules on an optical lattice. We show that a suitably chosen two-species mixture of ultracold polar molecules loaded on an optical lattice forms a phononless crystal, where exciton-impurity interactions can be controlled by applying an external electric field. This can be used for the controlled creation of many-body entangled states of ultracold molecules and the time-domain quantum simulation of disorder-induced localization and delocalization of quantum particles.

physics.atom-ph↗