arXiv subjects

Jacek Klos

Publications and source records attributed to Jacek Klos.

11 recordsLinked to original sources

arXiv2026

Quantum Scattering of Fullerene 12C60 with Rare Gas Atoms and its selection rules for rotational quenching

The discovery of the C60 fullerene opened new horizons to design carbon nanostructures with targeted electronic structure as well as transport and optical properties. For example, endohedral 12C60 molecules were proposed as candidates for functional quantum architectures to store and manipulate encased atomic and molecular qubits. Recent advances in cryogenic buffer-gas cooling and frequency-comb spectroscopy have enabled rovibrational quantum-state-resolved measurements of gas-phase 12C60, revealing rotational fine structure reflecting its high icosahedral symmetry. Here, we present a perturbative quantum description of the 12C60 molecule interacting with a buffer gas of 40Ar atoms at temperatures of order 100 K, including a detailed analysis of their electronic structure, their interaction anisotropies, and the collision-induced rotational quenching of 12C60 in its vibrational and electronic ground state. The role of the icosahedral symmetry on the collisional dynamics is emphasized leading to unusual selection rules. Finally, we compute the isotropic and anisotropic static and dynamic dipole polarizability of 12C60 in its absolute ground state in order to evaluate the long-range, van der Waals interaction between 12C60 and 40Ar.

physics.atom-ph↗

arXiv2025

Perturbation-assisted Observation of the Lowest Vibrational Level of the $\mathrm{b}^{3}\Pi_{0}$ State of Ultracold LiK Molecules

The narrow transition from the lowest rovibrational level of the $\mathrm{X}^{1}\Sigma^{+}$ electronic ground state to the lowest vibrational level of the $\mathrm{b}^{3}\Pi_{0}$ potential provides opportunities for achieving magic-wavelength trapping of ultracold bialkali molecules for enhancing their rotational coherence times. Guided by existing spectroscopic data of several perturbed and deeply-bound rovibrational states of the $\mathrm{A}^{1}\Sigma^{+}$ potential [Grochola et al., Chem. Phys. Lett., 2012, 535, 17-20], we conducted a targeted spectroscopic search and report the first observation of the lowest vibrational level of the $\mathrm{b}^{3}\Pi_{0}$ state in $^{6}\mathrm{Li}^{40}\mathrm{K}$. The transition frequency from $|\mathrm{X}^{1}\Sigma^{+},\,v=0,\,J=0>$ to $|\mathrm{b}^{3}\Pi_{0},\,v'=0,\,J'=1>$ is determined to be 314,230.5(5)GHz. Assisted by microwave spectroscopy, we resolved the rotational structure of $|\mathrm{b}^{3}\Pi_{0},\,v'=0>$ and extracted a rotational constant of $h\times8.576(44)$ GHz for the $\mathrm{b}^{3}\Pi_{0}$ state. From this, we deducted an energy separation between $|\mathrm{b}^{3}\Pi_{0},v'=0,J'=0>$ and $|\mathrm{X}^{1}\Sigma^{+},v=0,J=0>$ of $hc\times$10,481.03(2) $\mathrm{cm}^{-1}$. Our work provides timely and precise information on the deeply-bound region of the $\mathrm{b}^{3}\Pi_{0}$ triplet excited potential of LiK, and benefits future applications of ultracold LiK isotopologues in quantum simulation and quantum computation that demand long coherence times.

physics.atom-ph↗

arXiv2022

Collision-induced C_60 rovibrational relaxation probed by state-resolved nonlinear spectroscopy

Quantum state-resolved spectroscopy was recently achieved for C60 molecules when cooled by buffer gas collisions and probed with a midinfrared frequency comb. This rovibrational quantum state resolution for the largest molecule on record is facilitated by the remarkable symmetry and rigidity of C60, which also present new opportunities and challenges to explore energy transfer between quantum states in this many-atom system. Here we combine state-specific optical pumping, buffer gas collisions, and ultrasensitive intracavity nonlinear spectroscopy to initiate and probe the rotation-vibration energy transfer and relaxation. This approach provides the first detailed characterization of C60 collisional energy transfer for a variety of collision partners, and determines the rotational and vibrational inelastic collision cross sections. These results compare well with our theoretical modeling of the collisions, and establish a route towards quantum state control of a new class of unprecedentedly large molecules.

physics.atom-ph↗

arXiv2021

Prospects for assembling ultracold radioactive molecules from laser-cooled atoms

Molecules with unstable isotopes often contain heavy and deformed nuclei and thus possess a high sensitivity to parity-violating effects, such as Schiff moments. Currently the best limits on Schiff moments are set with diamagnetic atoms. Polar molecules with quantum-enhanced sensing capabilities, however, can offer better sensitivity. In this work, we consider the prototypical 223Fr107Ag molecule, as the octupole deformation of the unstable 223Fr francium nucleus amplifies the nuclear Schiff moment of the molecule by two orders of magnitude relative to that of spherical nuclei and as the silver atom has a large electronegativity. To develop a competitive experimental platform based on molecular quantum systems, 223Fr atoms and 107Ag atoms have to be brought together at ultracold temperatures. That is, we explore the prospects of forming 223Fr107Ag from laser-cooled Fr and Ag atoms. We have performed fully relativistic electronic-structure calculations of ground and excited states of FrAg that account for the strong spin-dependent relativistic effects of Fr and the strong ionic bond to Ag. In addition, we predict the nearest-neighbor densities of magnetic-field Feshbach resonances in ultracold 223Fr+107Ag collisions with coupled-channel calculations. These resonances can be used for magneto-association into ultracold, weakly-bound FrAg. We also determine the conditions for creating 223Fr107Ag molecules in their absolute ground state from these weakly-bound dimers via stimulated Raman adiabatic passage using our calculations of the relativistic transition electronic dipole moments.

quant-ph↗

arXiv2021

Relativistic aspects of orbital and magnetic anisotropies in the chemical bonding and structure of lanthanide molecules

The electronic structure of magnetic lanthanide atoms is fascinating from a fundamental perspective. They have electrons in a submerged open 4f shell lying beneath a filled 6s shell with strong relativistic correlations leading to a large magnetic moment and large electronic orbital angular momentum. This large angular momentum leads to strong anisotropies, i. e. orientation dependencies, in their mutual interactions. The long-ranged molecular anisotropies are crucial for proposals to use ultracold lanthanide atoms in spin-based quantum computers, the realization of exotic states in correlated matter, and the simulation of orbitronics found in magnetic technologies. Short-ranged interactions and bond formation among these atomic species have thus far not been well characterized. Efficient relativistic computations are required. Here, for the first time we theoretically determine the electronic and ro-vibrational states of heavy homonuclear lanthanide Er2 and Tm2 molecules by applying state-of-the-art relativistic methods. In spite of the complexity of their internal structure, we were able to obtain reliable spin-orbit and correlation-induced splittings between the 91 Er2 and 36 Tm2 electronic potentials dissociating to two ground-state atoms. A tensor analysis allows us to expand the potentials between the atoms in terms of a sum of seven spin-spin tensor operators simplifying future research. The strengths of the tensor operators as functions of atom separation are presented and relationships among the strengths, derived from the dispersive long-range interactions, are explained. Finally, low-lying spectroscopically relevant ro-vibrational energy levels are computed with coupled-channels calculations and analyzed.

quant-ph↗

arXiv2021

Quantum spin state selectivity and magnetic tuning of ultracold chemical reactions of triplet alkali-metal dimers with alkali-metal atoms

We demonstrate that it is possible to efficiently control ultracold chemical reactions of alkali-metal atoms colliding with open-shell alkali-metal dimers in their metastable triplet states by choosing the internal hyperfine and rovibrational states of the reactants as well as by inducing magnetic Feshbach resonances with an external magnetic field. We base these conclusions on coupled-channel statistical calculations that include the effects of hyperfine contact and magnetic-field-induced Zeeman interactions on ultracold chemical reactions of hyperfine-resolved ground-state Na and the triplet NaLi(a$^3Σ^+$) producing singlet Na$_2$($^1Σ^+_g$) and a Li atom. We find that the reaction rates are sensitive to the initial hyperfine states of the reactants. The chemical reaction of fully spin-polarized, high-spin states of rotationless NaLi(a$^3Σ^+, v = 0, N = 0$) molecules with fully spin-polarized Na is suppressed by a factor of 10-100 compared to that of unpolarized reactants. We interpret these findings within the adiabatic state model, which treats the reaction as a sequence of nonadiabatic transitions between the initial non-reactive high-spin state and the final low-spin states of the reaction complex. In addition, we show that magnetic Feshbach resonances can similarly change reaction rate coefficients by several orders of magnitude. Some of these resonances are due to resonant trimer bound states dissociating to the $N=2$ rotational state of NaLi(a$^3Σ^+, v = 0$) and would thus exist in systems without hyperfine interactions.

physics.chem-ph↗

arXiv2020

Effects of Conical Intersections on Hyperfine Quenching of Hydroxyl OH in collision with an ultracold Sr atom

The effect of conical intersections (CIs) on electronic relaxation, transitions from excited states to ground states, is well studied, but their influence on hyperfine quenching in a reactant molecule is not known. Here, we report on ultracold collision dynamics of the hydroxyl free-radical OH with Sr atoms leading to quenching of OH hyperfine states. Our quantum-mechanical calculations of this process reveal that quenching is efficient due to anomalous molecular dynamics in the vicinity of the conical intersection at collinear geometry. We observe wide scattering resonance features in both elastic and inelastic rate coefficients at collision energies below k x 10 mK. They are identified as either p- or d-wave shape resonances. We also describe the electronic potentials relevant for these non-reactive collisions, their diabatization procedure, as well as the non-adiabatic coupling between the diabatic potentials near the CIs.

physics.chem-ph↗

arXiv2020

Photon-mediated charge-exchange reactions between 39K atoms and 40Ca+ ions in a hybrid trap

We present experimental evidence of charge exchange between laser-cooled potassium $^{39}$K atoms and calcium $^{40}$Ca$^+$ ions in a hybrid atom-ion trap and give quantitative theoretical explanations for the observations. The $^{39}$K atoms and $^{40}$Ca$^+$ ions are held in a magneto-optical (MOT) and a linear Paul trap, respectively. Fluorescence detection and high resolution time of flight mass spectra for both species are used to determine the remaining number of $^{40}$Ca$^+$ ions, the increasing number of $^{39}$K$^+$ ions, and $^{39}$K number density as functions of time. Simultaneous trap operation is guaranteed by alternating periods of MOT and $^{40}$Ca$^+$ cooling lights, thus avoiding direct ionization of $^{39}$K by the $^{40}$Ca$^+$ cooling light. We show that the K-Ca$^+$ charge-exchange rate coefficient increases linearly from zero with $^{39}$K number density and, surprisingly, the fraction of $^{40}$Ca$^+$ ions in the 4p\,$^2$P$_{1/2}$ electronically-excited state. Combined with our theoretical analysis, we conclude that these data can only be explained by a process that starts with a potassium atom in its electronic ground state and a calcium ion in its excited 4p\,$^2$P$_{1/2}$ state producing ground-state $^{39}$K$^+$ ions and metastable, neutral Ca\,(3d4p$^3$P$_1$) atoms, releasing only 150 cm$^{-1}$ equivalent relative kinetic energy. Charge-exchange between either ground- or excited-state $^{39}$K and ground-state $^{40}$Ca$^+$ is negligibly small as no energetically-favorable product states are available. Our experimental and theoretical rate coefficients of $9\times10^{-10}$ cm$^3$/s are in agreement given the uncertainty budgets.

physics.atom-ph↗

arXiv2019

Enhanced Yield from a Cryogenic Buffer Gas Beam Source via Excited State Chemistry

We use narrow-band laser excitation of Yb to substantially enhance the brightness of a cold beam of YbOH, a polyatomic molecule with high sensitivity to physics beyond the Standard Model (BSM). By exciting atomic Yb to the metastable $^3$P$_1$ state in a cryogenic environment, we significantly increase the chemical reaction cross-section for collisions of Yb with reactants. We characterize the dependence of the enhancement on the properties of the laser light, and study the final state distribution of the YbOH products. The resulting bright, cold YbOH beam can be used to increase the statistical sensitivity in searches for new physics utilizing YbOH, such as electron electric dipole moment (eEDM) and nuclear magnetic quadrupole moment (NMQM) experiments. We also perform new quantum chemical calculations that confirm the enhanced reactivity observed in our experiment. Additionally, our calculations compare reaction pathways of Yb($^3$P) with the reactants H$_2$O and H$_2$O$_2$. More generally, our work presents a broad approach for improving experiments that use cryogenic molecular beams for laser cooling and precision measurement searches of BSM physics.

physics.atom-ph↗

arXiv2012

Cold collisions of polyatomic molecular radicals with S-state atoms in a magnetic field: An ab initio study of He + CH2(X) collisions

We develop a rigorous quantum mechanical theory for collisions of polyatomic molecular radicals with S-state atoms in the presence of an external magnetic field. The theory is based on a fully uncoupled space-fixed basis set representation of the multichannel scattering wavefunction. Explicit expressions are presented for the matrix elements of the scattering Hamiltonian for spin-1/2 and spin-1 polyatomic molecular radicals interacting with structureless targets. The theory is applied to calculate the cross sections and thermal rate constants for spin relaxation in low-temperature collisions of the prototypical organic molecule methylene [CH2(X)] with He atoms. To this end, two highly accurate three-dimensional potential energy surfaces (PESs) of the He-CH2(X) complex are developed using the state-of-the-art CCSD(T) method and large basis sets. Both PESs exhibit shallow minima and are weakly anisotropic. Our calculations show that spin relaxation in collisions of CH2, CHD, and CD2 molecules with He atoms occurs at a much slower rate than elastic scattering over a large range of temperatures (1 uK -- 1 K) and magnetic fields (0.01 - 1 T), suggesting excellent prospects for cryogenic helium buffer-gas cooling of ground-state ortho-CH2(X) molecules in a magnetic trap. Furthermore, we find that ortho-CH2 undergoes collision-induced spin relaxation much more slowly than para-CH2, which indicates that magnetic trapping can be used to separate nuclear spin isomers of open-shell polyatomic molecules.

physics.chem-ph↗

arXiv2010

Cold heteromolecular dipolar collisions

We present the first experimental observation of cold collisions between two different species of neutral polar molecules, each prepared in a single internal quantum state. Combining for the first time the techniques of Stark deceleration, magnetic trapping, and cryogenic buffer gas cooling allows the enhancement of molecular interaction time by 10$^5$. This has enabled an absolute measurement of the total trap loss cross sections between OH and ND$_3$ at a mean collision energy of 3.6 cm$^{-1}$ (5 K). Due to the dipolar interaction, the total cross section increases upon application of an external polarizing electric field. Cross sections computed from \emph{ab initio} potential energy surfaces are in excellent agreement with the measured value at zero external electric field. The theory presented here represents the first such analysis of collisions between a $^2Π$ radical and a closed-shell polyatomic molecule.

physics.chem-ph↗