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Kálmán Varga

Publications and source records attributed to Kálmán Varga.

10 recordsLinked to original sources

Strong-Field Coulomb Explosion of Ethane, Propane, and Butane in Circularly Polarized Laser Fields

We investigate the Coulomb explosion of ethane (C$_2$H$_6$), propane (C$_3$H$_8$), and \textit{n}-butane (C$_4$H$_{10}$) driven by intense circularly polarized laser pulses using real-time time-dependent density functional theory (RT-TDDFT). The ionization dynamics are benchmarked against those obtained with linearly polarized fields oriented along the $x$, $y$, and $z$ axes at the same peak intensity. Under the laser conditions considered here, circular polarization produces greater ionization than any of the linearly polarized configurations for all three molecules, indicating that the rotating electric field enhances the initial electron-removal stage that triggers Coulomb explosion. Using circularly polarized excitation, we systematically characterize fragmentation thresholds, product distributions, channel branching ratios, and bond-breaking dynamics across the alkane series. Atomic hydrogen is the most abundant fragment in all three systems, demonstrating that hydrogen loss is the dominant fragmentation pathway. Ethane primarily retains its two-carbon backbone through partial dehydrogenation, propane exhibits the broadest range of fragmentation channels and the strongest competition between C--H and C--C bond cleavage within the present ensemble, and butane favors backbone cleavage into relatively stable two-carbon fragments, most notably through the $2\mathrm{C_2H_4} + 2\mathrm{H}$ channel. Analysis of the earliest bond-breaking events further shows that C--H dissociation is the preferred initial fragmentation step throughout the series, although the degree of competition with C--C cleavage depends on molecular size.

physics.chem-ph↗

Light-induced nonadiabatic dissipative quantum dynamics of the Na2 molecule

Strong light-matter coupling between molecules and optical or plasmonic cavity modes has emerged as a promising platform for advancing photonics, materials science, and chemistry. However, optical cavities and plasmonic resonators in particular are inherently lossy systems characterized by finite photon lifetimes. Accurate theoretical descriptions of molecular dynamics under strong coupling therefore require a proper treatment of cavity losses. In this work, we compare three theoretical approaches for modeling dissipative molecule-cavity dynamics within a realistic parameter regime: the Lindblad master equation, the stochastic Schrödinger equation, and the non-Hermitian Schrödinger equation. As an example, we consider the two lowest energy state of Na2 molecule coupled to a cavity mode and analyze the time evolution of the excited-state population and the mean photon number. Our results demonstrate that the stochastic Schrödinger equation provides an accurate and computationally efficient alternative to the Lindblad master equation, while the non-Hermitian Schrödinger approach is found to be applicable only within a limited range of conditions. Furthermore, we show that inclusion of molecular rotation leads to rotational-vibrational-photonic coupling and gives rise to pronounced nonadiabatic dynamics through light-induced conical intersections. These findings highlight the importance of both dissipation and rotational degrees of freedom for a realistic description of molecular dynamics in strongly coupled molecule-cavity systems.

quant-ph↗

Ember: An Extensible Benchmark Suite for Quantum Annealing Embedding Algorithms

Minor embedding is a required compilation step for quantum annealing, mapping logical problem graphs onto sparse hardware topologies. Despite its central role in determining solution quality, no standardized benchmark exists for comparing embedding algorithms: prior studies use incompatible graph libraries, inconsistent metrics, and non-reproducible experimental setups, making cross-algorithm comparisons unreliable. We present Ember (Embedding Minor Benchmark for Evaluative Reproducibility), an open-source benchmarking framework addressing this gap. Ember provides a standardized algorithm interface with seeded, reproducible execution infrastructure; a diverse graph library of 24,016 instances spanning structured, random, and physics-motivated problem types not previously used in embedding benchmarks; and a unified analysis pipeline supporting all three current D-Wave hardware topologies (Chimera, Pegasus, Zephyr). We evaluate five algorithms across the full library on Chimera and find that no algorithm dominates universally: rankings vary systematically with graph structure, and the best algorithm depends on the family being embedded. We also examine the effects of hardware topology (including Pegasus and Zephyr), qubit error rates, and evaluate a reinforcement-learning approach (CHARME) within a narrower test set. Ember is available at https://github.com/zachmacsmith/ember and is installable via pip install ember-qc.

quant-ph↗

Ab initio study of highly charged ion-induced Coulomb explosion imaging

We present a theoretical investigation of ion-induced Coulomb explosion imaging (CEI) of pyridazine molecules driven by energetic C$^{5+}$ projectiles, using time-dependent density-functional theory (TDDFT) with Ehrenfest nuclear dynamics. By systematically varying the projectile's impact point and orientation relative to the molecular plane, we compare orthogonal and in-plane trajectories and quantify their effects on fragment momenta, electron-density response, and atom-resolved ionization. Newton plots and time-resolved density snapshots show that trajectories avoiding direct atomic collisions yield the most faithful structural reconstructions, whereas direct impacts impart large, highly localized momenta that distort the recovered geometry. Planar trajectories generate substantially greater ionization and broader momentum distributions than orthogonal ones due to deeper traversal through the molecular electron cloud. Quantitative analysis of electron removal at 10~fs confirms that projectile proximity and orientation strongly modulate both local and global ionization. These findings clarify how impact geometry governs the fidelity of ion-induced CEI structural recovery and help explain the variability and noise observed in experimental CEI measurements. More broadly, the results highlight both the strengths and the intrinsic limitations of ion-induced CEI and identify key considerations for interpreting experiments.

physics.chem-ph↗

Quantum effects of Coulomb explosion simulations revealed by time-dependent density-functional theory

This study investigates the influence of quantum effects on Coulomb explosion dynamics using time-dependent density functional theory (TDDFT) simulations, comparing classical, semi-classical, and quantum approaches. The goal is to elucidate how electron dynamics affect the kinetic energy, angular distribution, and final velocities of ejected ions. The results indicate that quantum effects result in lower kinetic energies all ions, deviating from classical predictions. Furthermore, quantum simulations exhibit broader angular distributions and more diverse ion trajectories, aligning closely with experimental observations. The research also highlights the role of laser intensity and the resultant ionization in enhancing quantum effects, particularly in modifying ion velocities and distributions. These findings provide a deeper understanding of the role of electron dynamics in Coulomb explosions, offering valuable insights for both experimental and theoretical studies of molecular fragmentation.

physics.chem-ph↗

Fragmentation in Coulomb explosion of hydrocarbon molecules

Fragmentation dynamics in the Coulomb explosion of hydrocarbons, specifically methane, ethane, propane, and butane, are investigated using time dependent density functional theory (TDDFT) simulations. The goal of this work is to elucidate the distribution of fragments generated under laser-driven Coulomb explosion conditions. Detailed analysis reveals the types of fragments formed, their respective charge states, and the optimal laser intensities required for achieving various fragmentations. Our results indicate distinct fragmentation patterns for each hydrocarbon, correlating with the molecular structure and ionization potential. Additionally, we identify the laser parameters that maximize fragmentation efficiency, providing valuable insights for experimental setups. This research advances our understanding of Coulomb explosion mechanisms and offers a foundation for further studies in controlled molecular fragmentation.

physics.chem-ph↗

Description of the hydrogen atom and the He+ ion in an optical cavity using the Pauli-Fierz Hamiltonian

A system of one electron in a Coulomb potential in an optical cavity is solved using a tensor-product light-matter basis. The problem was treated at the level of the Pauli-Fierz Hamiltonian describing both light and matter quantum mechanically. The effect of cavity size on the energy levels and high harmonics generation (HHG) spectrum is studied. We have shown that the energy levels, transition states, entanglement, and the HHG spectrum can be strongly influenced by changing the cavity size.

physics.chem-ph↗

Real-Space, Real-Time Approach to Quantum-Electrodynamical Time-Dependent Density Functional Theory

The Quantum-Electrodynamical Time-Dependent Density Functional Theory (QED-TDDFT) equations are solved by time propagating the wave function on a tensor product of a Fock-space and real-space grid. Applications for molecules in cavities show the accuracy of the approach. Examples include the coupling strength and light frequency dependence of the energies, wave functions, optical absorption spectra, and Rabi splitting magnitudes in cavities, as well as a description of high harmonic generation in cavities.

quant-ph↗

The biexciton puzzle

The Stochastic Variational Method (SVM) is used to show that the effective mass model correctly estimates the binding energies of excitons and trions, but fails to predict the experimental binding energy of the biexciton. Using high-accuracy variational calculations, it is demonstrated that the biexciton binding energy in transition metal dichalcogenides is smaller than the trion binding energy, contradicting experimental findings. It is also shown that an excited state of the biexciton is in very good agreement with experimental data. This excited state corresponds to an hole attached to a negative trion and may be a possible resolution of the discrepancy between theory and experiment.

cond-mat.mes-hall↗

Borromean Binding of Three or Four Bosons

We estimate the ratio $R=g_{3}/g_{2}$ of the critical coupling constants $g_{2}$ and $g_{3}$ which are required to achieve binding of 2 or 3 bosons, respectively, with a short-range interaction, and examine how this ratio depends on the shape of the potential. Simple monotonous potentials give $R\simeq 0.8$. A wide repulsive core pushes this ratio close to R=1. On the other hand, for an attractive well protected by an external repulsive barrier, the ratio approaches the rigorous lower bound $R=2/3$. We also present results for N=4 bosons, sketch the extension to $N>4$, and discuss various consequences.

nucl-th↗