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Michał Tomza

Publications and source records attributed to Michał Tomza.

At least 37 records · Page 2Linked to original sources

Characterizing out-of-distribution generalization of neural networks: application to the disordered Su-Schrieffer-Heeger model

Machine learning (ML) is a promising tool for the detection of phases of matter. However, ML models are also known for their black-box construction, which hinders understanding of what they learn from the data and makes their application to novel data risky. Moreover, the central challenge of ML is to ensure its good generalization abilities, i.e., good performance on data outside the training set. Here, we show how the informed use of an interpretability method called class activation mapping (CAM), and the analysis of the latent representation of the data with the principal component analysis (PCA) can increase trust in predictions of a neural network (NN) trained to classify quantum phases. In particular, we show that we can ensure better out-of-distribution generalization in the complex classification problem by choosing such an NN that, in the simplified version of the problem, learns a known characteristic of the phase. We show this on an example of the topological Su-Schrieffer-Heeger (SSH) model with and without disorder, which turned out to be surprisingly challenging for NNs trained in a supervised way. This work is an example of how the systematic use of interpretability methods can improve the performance of NNs in scientific problems.

quant-ph↗

Spin--spin interaction and magnetic Feshbach resonances in collisions of high-spin atoms with closed-shell atoms

We investigate interactions and ultracold collisions of high-spin but spherical atoms with closed-shell atoms, focussing on the example of Cr with Yb. Such a combination has only one potential energy curve but gives rise to a substantial intra-atomic spin--spin interaction, which causes Feshbach resonances due to rotationally excited states. We find such resonances are guaranteed below 250 G and can reach widths of 10s of G in favorable circumstances. We study the effect of hyperfine structure, which can create additional wide resonances at low fields. Finally, we consider isotopic substitution and show that for any realistic potential it is very likely at least one combination of commonly used isotopes will have resonances with experimentally favorable properties. Thus, this is a promising system for both molecule formation and studying quantum mixtures including dipolar species.

physics.atom-ph↗

Photodissociation spectra of single trapped CaOH+ molecular ions

Molecular ions that are generated by chemical reactions with trapped atomic ions can serve as an accessible testbed for developing molecular quantum technologies. On the other hand, they are also a hindrance to scaling up quantum computers based on atomic ions as unavoidable reactions with background gas destroy the information carriers. Here, we investigate the single- and two-photon dissociation processes of single $\text{CaOH}^+$ molecular ions co-trapped in $\text{Ca}^+$ ion crystals using a femtosecond laser system. We report the photodissociation cross section spectra of $\text{CaOH}^+$ for single-photon processes at $λ=$245 - 275$\,$nm and for two-photon processes at $λ=$500 - 540$\,$nm. Measurements are interpreted with quantum-chemical calculations, which predict the photodissociation threshold for $\text{CaOH}^+\to \text{Ca}^++\text{OH}$ at 265$\,$nm. This result can serve as a basis for dissociation-based spectroscopy for studying the internal structure of $\text{CaOH}^+$. The result also gives a prescription for recycling $\text{Ca}^+$ ions in large-scale trapped $\text{Ca}^+$ quantum experiments from undesired $\text{CaOH}^+$ ions formed in the presence of background water vapor.

physics.atom-ph↗

Interactions and cold collisions of AlF in the ground and excited electronic states with He

Aluminium monofluoride (AlF) is a promising candidate for laser cooling and the production of dense ultracold molecular gases, thanks to its relatively high chemical stability and diagonal Frank-Condon factors. In this study, we examine the interactions and collisions of AlF in its $X^1Σ^+$, $a^3Π$, and $A^{1}Π$ electronic states with ground-state He using state-of-the-art \textit{ab initio} quantum chemistry techniques. We construct accurate potential energy surfaces (PESs) employing either the explicitly correlated coupled-cluster CCSD(T)-F12 method augmented by the CCSDT correction or the multireference configuration-interaction method for higher-excited electronic states. Subsequently, we employ these PESs in coupled-channel calculations to determine the scattering cross-sections for AlF+He collisions and bound states of the complex. We estimate the uncertainty of the calculated PESs and apply it to assess the uncertainty of the scattering results. We find a relatively low sensitivity of the cross-sections to the variation of the PESs, but the positions of shape resonances remain uncertain. The present results are relevant for further improvements and optimizations of buffer-gas cooling of AlF molecules.

physics.chem-ph↗

Diatomic molecules of alkali-metal and alkaline-earth-metal atoms: interaction potentials, dipole moments, and polarizabilities

Ultracold diatomic molecules find application in quantum studies ranging from controlled chemistry and precision measurement physics to quantum many-body simulation and potentially quantum computing. Accurate knowledge of molecular properties is required to guide and explain ongoing experiments. Here, in an extensive and comparative study, we theoretically investigate the electronic properties of the ground-state diatomic molecules composed of alkali-metal (Li, Na, K, Rb, Cs, Fr) and alkaline-earth-metal (Be, Mg, Ca, Sr, Ba, Ra) atoms. We study 78 hetero- and homonuclear diatomic combinations, including 21 alkali-metal molecules in the $X^1Σ^+$ and $a^3Σ^+$ electronic states, 36 alkali-metal--alkaline-earth-metal molecules in the $X^2Σ^+$ electronic state, and 21 alkaline-earth-metal molecules in the $X^1Σ^+$ electronic state. We calculate potential energy curves, permanent electric dipole moments, and polarizabilities using the hierarchy of coupled cluster methods upto CCSDTQ with large Gaussian basis sets and small-core relativistic energy-consistent pseudopotentials. We collect and analyze corresponding spectroscopic constants. We estimate computational uncertainties and compare the present values with previous experimental and theoretical data to establish a new theoretical benchmark. The presented results should be useful for further application of the studied molecules in modern ultracold physics and chemistry experiments.

physics.atom-ph↗

Chemical reactions of ultracold alkaline-earth-metal diatomic molecules

We study the energetics of chemical reactions between ultracold ground-state alkaline-earth-metal diatomic molecules. We show that the atom-exchange reactions forming homonuclear dimers are energetically allowed for all heteronuclear alkaline-earth-metal combinations. We perform high-level electronic structure calculations on the potential energy surfaces of all possible homo- and heteronuclear alkaline-earth-metal trimers and show that trimer formation is also energetically possible in collisions of all considered dimers. Interactions between alkaline-earth-metal diatomic molecules lead to the formation of deeply bound reaction complexes stabilized by large non-additive interactions. We check that there are no barriers to the studied chemical reactions. This means that all alkaline-earth-metal diatomic molecules are chemically unstable at ultralow temperature, and optical lattice or shielding schemes may be necessary to segregate the molecules and suppress losses.

physics.atom-ph↗

Van der Waals coefficients for interactions of dysprosium and erbium atoms with alkali-metal and alkaline-earth-metal atoms

The long-range part of the interatomic interactions plays a substantial role in the collisional dynamics of ultracold gases. Here, we report on the calculation of the isotropic and anisotropic $C_6$ coefficients characterizing the van der Waals interaction between dysprosium or erbium atoms in the two lowest energy levels and the ground-state alkali-metal (Li, Na, K, Rb, Cs, Fr) or alkaline-earth-metal (Be, Mg, Ca, Sr, Ba) atoms. The calculations are done using the integral of dynamic dipole polarizabilities at so-called imaginary frequencies of the two interacting atoms. For all atom pairs, we find that the isotropic $C_6$ coefficients are two or three orders of magnitude larger than the anisotropic ones. Those coefficients are essential for modeling collisional properties of heteronuclear quantum mixtures containing highly magnetic dysprosium or erbium atoms and alkali-metal or alkaline-earth-metal atoms.

physics.atom-ph↗

Quantum simulation of the central spin model with a Rydberg atom and polar molecules in optical tweezers

Central spin models, where a single spinful particle interacts with a spin environment, find wide application in quantum information technology and can be used to describe, e.g., the decoherence of a qubit over time. We propose a method of realizing an ultracold quantum simulator of a central spin model with XX (spin-exchanging) interactions. The proposed system consists of a single Rydberg atom ("central spin") and surrounding polar molecules ("bath spins"), coupled to each other via dipole-dipole interactions. By mapping internal particle states to spin states, spin-exchanging interactions can be simulated. As an example system geometry, we consider a ring-shaped arrangement of bath spins, and show how it allows us to exact precise control over the interaction strengths. We numerically analyze two example dynamical scenarios which can be simulated in this setup: a decay of central spin polarization, which can represent qubit decoherence in a disordered environment, and a transfer of an input spin state to a specific output spin, which can represent the transmission of a single bit across a quantum network. We demonstrate that this setup allows us to realize a central spin model with highly tunable parameters and geometry, for applications in quantum science and technology.

quant-ph↗

Long-range interactions of aromatic molecules with alkali-metal and alkaline-earth-metal atoms

The isotropic and anisotropic coefficients $C^{l,m}_n$ of the long-range spherical expansion $\sim 1/R^n$ ($R$ -- the intermolecular distance) of the dispersion and inductions intermolecular energies are calculated using the first principles for the complexes containing an aromatic molecule (benzene, pyridine, furan, and pyrrole) and alkali-metal (Li, Na, K, Rb, and Cs) or alkaline-earth-metal (Be, Mg, Ca, Sr, and Ba) atoms in their electronic ground states. The values of the first and second-order properties of the aromatic molecules are calculated using the response theory with the asymptotically corrected LPBE0 functional. The second-order properties of the closed-shell alkaline-earth-metal atoms are obtained using the expectation-value coupled cluster theory and of the open-shell alkali-metal atoms using analytical wavefunctions. These properties are used for the calculation of the dispersion $C^{l,m}_{n,\text{disp}}$ and induction $C^{l,m}_{n,\text{ind}}$ coefficients ($C^{l,m}_n=C^{l,m}_{n,\text{disp}}+C^{l,m}_{n,\text{ind}}$) with $n$ up to 12 using the available implemented analytical formulas. It is shown that the inclusion of the coefficients with $n>6$ is important for reproducing the interaction energy in the van der Waals region at $R\approx 6$ angstrom. The reported long-range potentials should be useful for constructing the analytical potentials, valid for the whole intermolecular interaction range, which are needed for spectroscopic and scattering studies.

physics.chem-ph↗

Excited electronic states of Sr$_2$: ab initio predictions and experimental observation of the $2^1Σ^{+}_{u}$ state

Despite its apparently simple nature with four valence electrons, the strontium dimer constitutes a challenge for modern electronic structure theory. Here we focus on excited electronic states of Sr$_2$, which we investigate theoretically up to 25000 cm$^{-1}$ above the ground state, to guide and explain new spectroscopic measurements. In particular, we focus on potential energy curves for the $1^1Σ^{+}_{u}$, $2^1Σ^{+}_{u}$, $1^1Π_{u}$, $2^1Π_{u}$, and $1^1Δ_{u}$ states computed using several variants of advanced \textit{ab initio} methods to benchmark them. In addition, a new experimental study of the excited $2^1Σ^{+}_{u}$ state using polarisation labelling spectroscopy is presented, which extends knowledge of this state to high vibrational levels, where perturbation by higher electronic states is observed. The available experimental observations are compared with the theoretical predictions and help to assess the accuracy and limitations of employed theoretical models. The present results pave the way for future more accurate theoretical and experimental spectroscopic studies.

physics.chem-ph↗

Spectrum of Feshbach resonances in NaLi $+$ Na collisions

Collisional resonances of molecules can offer a deeper understanding of interaction potentials and collision complexes, and allow control of chemical reactions. Here, we experimentally map out the spectrum of Feshbach resonances in collisions between ultracold triplet ro-vibrational ground-state NaLi molecules and Na atoms over a range of 1400 G. Preparation of the spin-stretched state puts the system initially into the non-reactive quartet potential. A total of 25 resonances are observed, in agreement with quantum-chemistry calculations using a coupled-channels approach. Although the theory cannot predict the positions of resonances, it can account for several experimental findings and provide unprecedented insight into the nature and couplings of ultracold, strongly interacting complexes. Previous work has addressed only weakly bound complexes. We show that the main coupling mechanism results from spin-rotation and spin-spin couplings in combination with the anisotropic atom-molecule interaction, and that the collisional complexes which support the resonances have a size of 30-40 $a_0$. This study illustrates the potential of a combined experimental and theoretical approach.

physics.atom-ph↗

Ab initio potential energy curves, scattering lengths, and rovibrational levels of the He$_2^+$ molecular ion in excited electronic states

We calculate accurate potential energy curves for a ground-state He$^+$ ion interacting with a He atom in the lowest-energy metastable $^3\!S$ electronic state. We employ the full configuration interaction method, equivalent to exact diagonalization, with results extrapolated to the complete basis set limit. The leading relativistic and adiabatic corrections are included using perturbation theory. We calculate rovibrational levels and spectroscopic constants of the He$_2^+$ molecular ion in excited electronic states for three stable isotopologues. We predict the scattering lengths for ultracold ion-atom collisions. The theoretical data are presented with their uncertainties and agree well with previous results for the ground state. The reported results may be useful for the spectroscopy of the He$_2^+$ molecular ion in the excited electronic state and collisional studies of He$^+$ ions immersed in ultracold gases of metastable He atoms.

physics.atom-ph↗

Two ultracold highly magnetic atoms in a one-dimensional harmonic trap

We theoretically investigate the properties of two interacting ultracold highly magnetic atoms trapped in a one-dimensional harmonic potential. The atoms interact via an anisotropic long-range dipole-dipole interaction, which in one dimension effectively can be modeled by the contact interaction. We investigate the interplay of the external magnetic field, the spin-spin interaction, and the trapping potential and how they affect the magnetization of the system. We show the role of indistinguishability and symmetries in the dynamics by studying the time evolution of the observables that could be measured experimentally. The presented model may depict the on-site interaction of the extended Hubbard models, therefore giving a better understanding of the fundamental building block of the respective many-body quantum simulators.

physics.atom-ph↗

Collisional losses of ultracold molecules due to intermediate complex formation

Understanding the sources of losses and chemical reactions of ultracold alkali-metal molecules is among the critical elements needed for their application in precision measurements and quantum technologies. Recent experiments with nonreactive systems have reported unexpectedly large loss rates, posing a challenge for theoretical explanation. Here, we examine the dynamics of intermediate four-atom complexes formed in bimolecular collisions. We calculate the nuclear spin--rotation, spin--spin, and quadrupole coupling constants for bialkali tetramers using ab intio quantum-chemical methods. We show that the nuclear spin--spin and quadrupole couplings are strong enough to couple different rotational manifolds to increase the density of states and lifetimes of the collision complexes, which is consistent with experimental results. We propose further experiments to confirm our predictions.

cond-mat.quant-gas↗

Controlling the dynamics of ultracold polar molecules in optical tweezers

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 two-body states, with the potential for significant gate speedup employing trap-induced resonances.

quant-ph↗

Van der Waals molecules consisting of a zinc or cadmium atom interacting with an alkali-metal or alkaline-earth-metal atom

Alkaline-earth-like transition-metal atoms such as Zn and Cd are promising candidates for precision measurements and quantum many-body physics experiments. Here, we theoretically investigate the properties of diatomic molecules containing these closed-shell atoms. We calculate potential energy curves, permanent electric dipole moments, and spectroscopic constants for molecules consisting of either a Zn or Cd atom interacting with an alkali-metal (Li, Na, K, Rb, Cs, Fr) or alkaline-earth-metal (Be, Mg, Ca, Sr, Ba, Ra) atom. We use the ab initio electronic structure coupled cluster method with single, double, and triple excitations combined with large Gaussian basis sets and small-core relativistic energy-consistent pseudopotentials for heavier atoms. We predict that the studied molecules in the ground electronic state are chemically reactive weakly bound van der Waals complexes with small permanent electric dipole moments. The present results may be useful for spectroscopy and application of the studied molecules in modern ultracold physics and chemistry experiments.

physics.atom-ph↗

Hessian-based toolbox for reliable and interpretable machine learning in physics

Machine learning (ML) techniques applied to quantum many-body physics have emerged as a new research field. While the numerical power of this approach is undeniable, the most expressive ML algorithms, such as neural networks, are black boxes: The user does neither know the logic behind the model predictions nor the uncertainty of the model predictions. In this work, we present a toolbox for interpretability and reliability, agnostic of the model architecture. In particular, it provides a notion of the influence of the input data on the prediction at a given test point, an estimation of the uncertainty of the model predictions, and an extrapolation score for the model predictions. Such a toolbox only requires a single computation of the Hessian of the training loss function. Our work opens the road to the systematic use of interpretability and reliability methods in ML applied to physics and, more generally, science.

quant-ph↗

Interaction potentials, electric moments, polarizabilities, and chemical reactions of YbCu, YbAg, and YbAu molecules

Ultracold YbAg molecules have been recently proposed as promising candidates for electron electric dipole moment searches [Verma, Jayich, and Vutha, Phys. Rev. Lett. 125, 153201 (2020)]. Here, we calculate potential energy curves, permanent electric dipole and quadrupole moments, and static electric dipole polarizabilities for the YbCu, YbAg, and YbAu molecules in their ground electronic states. We use the coupled cluster method restricted to single, double, and noniterative triple excitations with large Gaussian basis sets, while the scalar relativistic effects are included within the small-core energy-consistent pseudopotentials. We find that the studied molecules are relatively strongly bound with the well depths of 5708$\,$cm$^{-1}$, 5253$\,$cm$^{-1}$, 13349$\,$cm$^{-1}$ and equilibrium distances of 5.50$\,$bohr, 5.79$\,$bohr, 5.55$\,$bohr for the YbCu, YbAg, and YbAu, respectively. They have large permanent electric dipole moments of 3.2$\,$D, 3.3$\,$D, and 5.3$\,$D at equilibrium distances, respectively. We also calculate equilibrium geometries and energies of corresponding trimers. The studied molecules are chemically reactive unless they are segregated in an optical lattice or shielded with external fields. The investigated molecules may find application in ultracold controlled chemistry, dipolar many-body physics, or precision measurement experiments.

physics.atom-ph↗