arXiv subjects

Mikhail Lemeshko

Publications and source records attributed to Mikhail Lemeshko.

At least 37 records · Page 2Linked to original sources

arXiv2025

Nonadiabatic laser-induced alignment dynamics of alkali dimers on the surface of a helium droplet

Alkali dimers, $\mathrm{Ak}_2$, located on the surface of a helium nanodroplet, are set into rotation through the polarizability interaction with a nonresonant 1-ps-long laser pulse. The time-dependent degree of alignment is recorded using femtosecond-probe-pulse-induced Coulomb explosion into a pair of $\mathrm{Ak}^+$ fragment ions. The results, obtained for $\mathrm{Na}_2$, $\mathrm{K}_2$, and $\mathrm{Rb}_2$ in both the ground state $1 ^1Σ_g^+$ and the lowest-lying triplet state $1 ^3Σ_u^+$, exhibit distinct, periodic revivals with a gradually decreasing amplitude. The dynamics differ from that expected for dimers had they behaved as free rotors. Numerically, we solve the time-dependent rotational Schrödinger equation, including an effective mean-field potential to describe the interaction between the dimer and the droplet. The experimental and simulated alignment dynamics agree well and their comparison enables us to determine the effective rotational constants of the alkali dimers with the exception of $\mathrm{Rb}_2$($1 ^3Σ_u^+$) that only exhibits a prompt alignment peak but no subsequent revivals. For $\mathrm{Na}_2$($1 ^3Σ_u^+$), $\mathrm{K}_2$($1 ^1Σ_g^+$), $\mathrm{K}_2$($1 ^3Σ_u^+$) and $\mathrm{Rb}_2$($1 ^1Σ_g^+$), the alignment dynamics are well-described by a 2D rotor model. We ascribe this to a significant confinement of the internuclear axis of these dimers, induced by the orientation-dependent droplet-dimer interaction, to the tangential plane of their residence point on the droplet.

physics.atm-clus↗

arXiv2025

Environment-limited transfer of angular momentum in Bose liquids

Impurity motion in a many-body environment has been a central issue in the field of low-temperature physics for decades. In bosonic quantum fluids, the onset of a drag force experienced by point-like objects is due to collective environment excitations, driven by the exchange of linear momentum between the impurity and the many-body bath. In this work we consider a rotating impurity, with the aim of exploring how angular momentum is exchanged with the surrounding bosonic environment. In order to elucidate this issues, we employ a quasiparticle approach based on the angulon theory, which allows us to effectively deal with the non-trivial algebra of quantized angular momentum in presence of a many-body environment. We uncover how impurity dressing by environmental excitations can establish an exchange channel, whose effectiveness crucially depends on the initial state of the impurity. Remarkably, we find that there is a critical value of initial angular momentum, above which this channel effectively freezes.

cond-mat.quant-gas↗

arXiv2025

Domain-Wall Ferroelectric Polarons in a two-dimensional Rotor Lattice Model

We demonstrate the formation of ferroelectric domain-wall polarons in a minimal two-dimensional lattice model of electrons interacting with rotating dipoles. Along the domain-wall, the rotors polarize in opposite directions, causing the electron to localize along a particular lattice direction. The rotor-electron coupling is identified as the origin of a structural instability in the crystal that leads to the domain-wall formation via a symmetry-breaking process. Our results provide the first theoretical description of ferroelectric polarons, as discussed in the context of soft semiconductors.

cond-mat.mes-hall↗

arXiv2024

Anomalous multi-gap topological phases in periodically driven quantum rotors

We demonstrate that periodically driven quantum rotors provide a promising and broadly applicable platform to implement multi-gap topological phases, where groups of bands can acquire topological invariants due to non-Abelian braiding of band degeneracies. By adiabatically varying the periodic kicks to the rotor we find nodal-line braiding, which causes sign flips of topological charges of band nodes and can prevent them from annihilating, indicated by non-zero values of the %non-Abelian patch Euler class. In particular, we report on the emergence of an anomalous Dirac string phase arising in the strongly driven regime, a truly out-of-equilibrium phase of the quantum rotor. This phase emanates from braiding processes involving all (quasienergy) gaps and manifests itself with edge states at zero angular momentum. Our results reveal direct applications in state-of-the-art experiments of quantum rotors, such as linear molecules driven by periodic far-off-resonant laser pulses or artificial quantum rotors in optical lattices, whose extensive versatility offers precise modification and observation of novel non-Abelian topological properties.

quant-ph↗

arXiv2024

Theory of angular momentum transfer from light to molecules

We present a theory describing interaction of structured light, such as light carrying orbital angular momentum, with molecules. The light-matter interaction Hamiltonian we derive is expressed through couplings between spherical gradients of the electric field and the (transition) multipole moments of a particle of any non-trivial rotation point group. Our model can therefore accommodate for an arbitrary complexity of the molecular and electric field structure, and can be straightforwardly extended to atoms or nanostructures. Applying this framework to ro-vibrational spectroscopy of molecules, we uncover the general mechanism of angular momentum exchange between the spin and orbital angular momenta of light, molecular rotation and its center-of-mass motion. We show that the non-zero vorticity of Laguerre-Gaussian beams can strongly enhance certain ro-vibrational transitions that are considered forbidden in the case of non-helical light. We discuss the experimental requirements for the observation of these forbidden transitions in state-of-the-art spatially-resolved spectroscopy measurements.

physics.atom-ph↗

arXiv2024

Linear rotor in an ideal Bose gas near the threshold for binding

We study a linear rotor in a bosonic bath within the angulon formalism. Our focus is on systems where isotropic or anisotropic impurity-boson interactions support a shallow bound state. To study the fate of the angulon in the vicinity of bound-state formation, we formulate a beyond-linear-coupling angulon Hamiltonian. First, we use it to study attractive, spherically symmetric impurity-boson interactions for which the linear rotor can be mapped onto a static impurity. The well-known polaron formalism provides an adequate description in this limit. Second, we consider anisotropic potentials, and show that the presence of a shallow bound state with pronounced anisotropic character leads to a many-body instability that washes out the angulon dynamics.

cond-mat.quant-gas↗

arXiv2023

Achiral dipoles on a ferromagnet can affect its magnetization direction

We demonstrate the possibility of a coupling between the magnetization direction of a ferromagnet and the tilting angle of adsorbed achiral molecules. To illustrate the mechanism of the coupling, we analyze a minimal Stoner model that includes Rashba spin-orbit coupling due to the electric field on the surface of the ferromagnet. The proposed mechanism allows us to study magnetic anisotropy of the system with an extended Stoner-Wohlfarth model, and argue that adsorbed achiral molecules can change magnetocrystalline anisotropy of the substrate. Our research's aim is to motivate further experimental studies of the current-free chirality induced spin selectivity effect involving both enantiomers.

cond-mat.mes-hall↗

arXiv2023

Bond polarizability as a probe of local crystal fields in hybrid lead-halide perovskites

A rotating organic cation and a dynamically disordered soft inorganic cage are the hallmark features of hybrid organic-inorganic lead-halide perovskites. Understanding the interplay between these two subsystems is a challenging problem but it is this coupling that is widely conjectured to be responsible for the unique behavior of photo-carriers in these materials. In this work, we use the fact that the polarizability of the organic cation strongly depends on the ambient electrostatic environment to put the molecule forward as a sensitive probe of local crystal fields inside the lattice cell. We measure the average polarizability of the C/N--H bond stretching mode by means of infrared spectroscopy, which allows us to deduce the character of the motion of the cation molecule, find the magnitude of the local crystal field and place an estimate on the strength of the hydrogen bond between the hydrogen and halide atoms. Our results pave the way for understanding electric fields in lead-halide perovskites using infrared bond spectroscopy.

cond-mat.mes-hall↗

arXiv2023

Nonadiabatic Laser-Induced Alignment Dynamics of Molecules on a Surface

We demonstrate that a sodium dimer, Na$_{2}$($1^3Σ_{u}^+$), residing on the surface of a helium nanodroplet, can be set into rotation by a nonresonant 1.0 ps infrared laser pulse. The time-dependent degree of alignment measured, exhibits a periodic, gradually decreasing structure that deviates qualitatively from that expected for gas phase dimers. Comparison to alignment dynamics calculated from the time-dependent rotational Schrödinger equation shows that the deviation is due to the alignment dependent interaction between the dimer and the droplet surface. This interaction confines the dimer to the tangential plane of the droplet surface at the point where it resides and is the reason that the observed alignment dynamics is also well-described by a 2D quantum rotor model.

physics.atm-clus↗

arXiv2023

Modeling laser pulses as $δ$-kicks: reevaluating the impulsive limit in molecular rotational dynamics

The impulsive limit (the "sudden approximation") has been widely employed to describe the interaction between molecules and short, far-off-resonant laser pulses. This approximation assumes that the timescale of the laser--molecule interaction is significantly shorter than the internal rotational period of the molecule, resulting in the rotational motion being instantaneously "frozen" during the interaction. This simplified description of laser-molecule interaction is incorporated in various theoretical models predicting rotational dynamics of molecules driven by short laser pulses. In this theoretical work, we develop an effective theory for ultrashort laser pulses by examining the full time-evolution operator and solving the time-dependent Schrödinger equation at the operator level. Our findings reveal a critical angular momentum, $l_\mathrm{crit}$, at which the impulsive limit breaks down. In other words, the validity of the sudden approximation depends not only on the pulse duration, but also on its intensity, since the latter determines how many angular momentum states are populated. We explore both ultrashort multi-cycle (Gaussian) pulses and the somewhat less studied half-cycle pulses, which produce distinct effective potentials. We discuss the limitations of the impulsive limit and propose a new method that rescales the effective matrix elements, enabling an improved and more accurate description of laser-molecule interactions.

physics.chem-ph↗

arXiv2023

Finite-range bias in fitting three-body loss to the zero-range model

We study the impact of finite-range physics on the zero-range-model analysis of three-body recombination in ultracold atoms. We find that temperature dependence of the zero-range parameters can vary from one set of measurements to another as it may be driven by the distribution of error bars in the experiment, and not by the underlying three-body physics. To study finite-temperature effects in three-body recombination beyond the zero-range physics, we introduce and examine a finite-range model based upon a hyperspherical formalism. The systematic error discussed in the paper may provide a significant contribution to the error bars of measured three-body parameters.

cond-mat.quant-gas↗

arXiv2023

Effective model for studying optical properties of lead-halide perovskites

We use general symmetry-based arguments to construct an effective model suitable for studying optical properties of lead-halide perovskites. To build the model, we identify an atomic-level interaction between electromagnetic fields and the spin degree of freedom that should be added to a minimally-coupled $\mathbf{k\cdot p}$ Hamiltonian. As a first application, we study two basic optical characteristics of the material: the Verdet constant and the refractive index. Beyond these linear characteristics of the material the model is suitable for calculating non-linear effects such as the third-order optical susceptibility. Analysis of this quantity shows that the geometrical properties of the spin-electric term imply isotropic optical response of the system, and that optical anisotropy of lead-halide perovskites is a manifestation of hopping of charge carriers. To illustrate this, we discuss third-harmonic generation.

cond-mat.mes-hall↗

arXiv2023

Spin-Electric Coupling in Lead Halide Perovskites

Lead-halide perovskites enjoy a number of remarkable optoelectronic properties. To explain their origin, it is necessary to study how electromagnetic fields interact with these systems. We address this problem here by studying two classical quantities: Faraday rotation and the complex refractive index in a paradigmatic perovskite CH$_3$NH$_3$PbBr$_3$ in a broad wavelength range. We find that the minimal coupling of electromagnetic fields to the k$\cdot$p Hamiltonian is insufficient to describe the observed data even on the qualitative level. To amend this, we demonstrate that there exists a relevant atomic-level coupling between electromagnetic fields and the spin degree of freedom. This spin-electric coupling allows for quantitative description of a number of previous as well as present experimental data. In particular, we use it here to show that the Faraday effect in lead-halide perovskites is dominated by the Zeeman splitting of the energy levels, and has a substantial beyond-Becquerel contribution. Finally, we present general symmetry-based phenomenological arguments that in the low-energy limit our effective model includes all basis coupling terms to the electromagnetic field in the linear order.

cond-mat.other↗

arXiv2023

Rotor Lattice Model of Ferroelectric Large Polarons

We present a minimal model of charge transport in hybrid perovskites, which provides an intuitive explanation for the recently proposed formation of ferroelectric large polarons. We demonstrate that short-ranged charge--rotor interactions lead to long-range ferroelectic ordering of rotors, which strongly affects the carrier mobility. In the nonperturbative regime, where our theory cannot be reduced to any of the earlier models, we predict polaron properties in good agreement with experiment. This shows the potential of simple models to reveal electronic properties of molecular materials.

cond-mat.mes-hall↗

arXiv2023

Topological charges of periodically kicked molecules

We show that the simplest of existing molecules -- closed-shell diatomics not interacting with one another -- host topological charges when driven by periodic far-off-resonant laser pulses. A periodically kicked molecular rotor can be mapped onto a ''crystalline'' lattice in angular momentum space. This allows to define quasimomenta and the band structure in the Floquet representation, by analogy with the Bloch waves of solid-state physics. Applying laser pulses spaced by $1/3$ of the molecular rotational period creates a lattice with three atoms per unit cell with staggered hopping. Within the synthetic dimension of the laser strength, we discover Dirac cones with topological charges. These Dirac cones, topologically protected by reflection and time-reversal symmetry, are reminiscent of (although not equivalent to) that seen in graphene. They -- and the corresponding edge states -- are broadly tunable by adjusting the laser strength and can be observed in present-day experiments by measuring molecular alignment and populations of rotational levels. This paves the way to study controllable topological physics in gas-phase experiments with small molecules as well as to classify dynamical molecular states by their topological invariants.

cond-mat.mes-hall↗

arXiv2022

Variational theory of angulons and their rotational spectroscopy

The angulon, a quasiparticle formed by a quantum rotor dressed by the excitations of a many-body bath, can be used to describe an impurity rotating in a fluid or solid environment. Here we propose a coherent state ansatz in the co-rotating frame which provides a comprehensive theoretical description of angulons. We reveal the quasiparticle properties, such as energies, quasiparticle weights and spectral functions, and show that our ansatz yields a persistent decrease in the impurity's rotational constant due to many-body dressing, consistent with experimental observations. From our study, a picture of the angulon emerges as an effective spin interacting with a magnetic field that is self-consistently generated by the molecule's rotation. Moreover, we discuss rotational spectroscopy, which focuses on the response of rotating molecules to a laser perturbation in the linear response regime. Importantly, we take into account initial-state interactions that have been neglected in prior studies and reveal their impact on the excitation spectrum. To examine the angulon instability regime, we use a single-excitation ansatz and obtain results consistent with experiments, in which a broadening of spectral lines is observed while phonon wings remain highly suppressed due to initial-state interactions.

cond-mat.quant-gas↗

arXiv2022

Dissipative dynamics of an impurity with spin-orbit coupling

Brownian motion of a mobile impurity in a bath is affected by spin-orbit coupling (SOC). Here, we discuss a Caldeira-Leggett-type model that can be used to propose and interpret quantum simulators of this problem in cold Bose gases. First, we derive a master equation that describes the model and explore it in a one-dimensional (1D) setting. To validate the standard assumptions needed for our derivation, we analyze available experimental data without SOC; as a byproduct, this analysis suggests that the quench dynamics of the impurity is beyond the 1D Bose-polaron approach at temperatures currently accessible in a cold-atom laboratory -- motion of the impurity is mainly driven by dissipation. For systems with SOC, we demonstrate that 1D spin-orbit coupling can be 'gauged out' even in the presence of dissipation -- the information about SOC is incorporated in the initial conditions. Observables sensitive to this information (such as spin densities) can be used to study formation of steady spin polarization domains during quench dynamics.

cond-mat.quant-gas↗

arXiv2022

Artificial atoms from cold bosons in one dimension

We investigate the ground-state properties of weakly repulsive one-dimensional bosons in the presence of an attractive zero-range impurity potential. First, we derive mean-field solutions to the problem on a finite ring for the two asymptotic cases: (i) all bosons are bound to the impurity and (ii) all bosons are in a scattering state. Moreover, we derive the critical line that separates these regimes in the parameter space. In the thermodynamic limit, this critical line determines the maximum number of bosons that can be bound by the impurity potential, forming an artificial atom. Second, we validate the mean-field results using the flow equation approach and the multi-layer multi-configuration time-dependent Hartree method for atomic mixtures. While beyond-mean-field effects destroy long-range order in the Bose gas, the critical boson number is unaffected. Our findings are important for understanding such artificial atoms in low-density Bose gases with static and mobile impurities.

cond-mat.quant-gas↗