arXiv subjects

Roman Korol

Publications and source records attributed to Roman Korol.

9 recordsLinked to original sources

arXiv2026

How NOT to build control-target gates in semiconductor quantum dots and beyond

Universal quantum computation requires single-qubit control together with at least one entangling two-qubit gate. CNOT and CROT gates are two famous examples of such gates, wherein the state of one qubit (control) dictates the transformation applied to the other (target). By using a simple derivation motivated by symmetry, we show that current device architectures of semiconductor-based quantum dot devices prevent efficient implementation of a CNOT and other asymmetric control-target gates via Heisenberg exchange, Coulomb repulsion, or other interaction that is invariant under spin exchange. Guided by this general principle, we propose a heterogeneous blueprint of double quantum dot devices that enables efficient implementation of the CNOT by breaking the spin exchange symmetry. Crucially, our numerical simulations predict that this novel device blueprint can enable a single-pulse fault-tolerant 100-ns CNOT gate in isotopically purified silicon.

cond-mat.mes-hall↗

arXiv2026

Light-Matter Interactions Beyond the Dipole Approximation in Extended Systems Without Multipole Expansion

We present a general theoretical framework to capture light-matter interactions beyond the electric-dipole approximation (EDA), applicable to extended nano- and microscale materials interacting with spatially structured electric fields without truncation at finite multipolar order. The approach is based on the Power-Zienau-Woolley (PZW) Hamiltonian for light-matter interactions and a representation of the material's Hamiltonian in a basis of maximally localized Wannier functions (MLWFs), obtainable from first-principles calculations. We utilize this approach to clarify the limitations of the ubiquitous dipole approximation. We consider electric fields with both uniform and non-uniform intensities and a range of ratios of system size to the wavelength of light. Through this analysis, we identify the conditions under which the EDA breaks down, leading to significant errors in the light-induced dynamics. Contrary to conventional belief, we find that the EDA is remarkably robust for uniformly illuminated 1-D or 2-D materials when light propagates perpendicular to the material. For 3-D materials or non-perpendicular illumination of lower-dimensional materials, conventional wisdom holds and the EDA begins to break down when the wavelength becomes comparable to the system size. Furthermore, the EDA fails when the material is illuminated partially or non-uniformly. For slowly varying field intensities this failure can be corrected by finite-order multipolar corrections. However, for fields that vary substantially, correcting via multipolar terms becomes computationally impractical. In contrast, our approach captures beyond-dipole light-matter interactions at the computational cost of a standard dipole calculation. This efficiency enables accurate first-principles simulations of spatially structured light-matter dynamics in nanoscale devices, quantum materials, and interfaces.

quant-ph↗

arXiv2025

Robust purely optical signatures of Floquet states in laser-dressed crystals

Strong light-matter interactions can create non-equilibrium materials with on-demand novel functionalities. For periodically driven solids, the Floquet theorem provides the natural states to characterize the physical properties of these laser-dressed systems. However, signatures of the Floquet states are needed, as common experimental conditions, such as pulsed laser excitation and dissipative many-body dynamics, can disrupt their formation and survival. Here, we identify a tell-tale signature of Floquet states in the linear optical response of laser-dressed solids that remains prominent even in the presence of strong spectral congestion of bulk matter. To do so, we introduce a computationally efficient strategy based on the Floquet formalism to finally capture the full frequency-dependence in the optical response properties of realistic laser-dressed crystals, and use it investigate the Floquet engineering in a first-principle model for ZnO of full dimensionality. The computations reveal intense, spectrally isolated, laser-controllable, absorption/stimulated emission features at mid-infrared energies present for a wide range of laser-driving conditions that arise due to the hybridization of the Floquet states. As such, these spectral features open a purely optical pathway to investigate the birth and survival of Floquet states while avoiding the experimental challenges of fully reconstructing the band structure.

physics.optics↗

arXiv2024

High-frequency tails in spectral densities

Recent advances in numerically exact quantum dynamics methods have brought the dream of accurately modeling the dynamics of chemically complex open systems within reach. Path-integral-based methods, hierarchical equations of motion (HEOM) and quantum analog simulators all require the spectral density (SD) of the environment to describe its effect on the system. Here we focus on the decoherence dynamics of electronically excited species in solution in the common case where nonradiative electronic relaxation dominates and is much slower than electronic dephasing. We show that the computed relaxation rate is highly sensitive to the choice of SD representation $\unicode{x2013}$ such as the Drude-Lorentz or Brownian modes $\unicode{x2013}$ or strategy used to capture the main SD features, even when early-times dephasing dynamics remains robust. The key reason is that electronic relaxation is dominated by the resonant contribution from the high-frequency tails of the SD, which are orders of magnitude weaker than the main features of the SD and can vary significantly between strategies. This finding highlights an important, yet overlooked, numerical challenge: obtaining an accurate spectral density requires capturing its structure over several orders of magnitude to ensure correct decoherence dynamics at both early and late times. To address this, we provide a simple transformation that recovers the correct relaxation rates in quantum simulations constrained by algorithmic or physical limitations on the shape of the SD. Our findings enable comparison of different numerically exact simulation methods and expand the capabilities of analog simulations of open quantum dynamics.

physics.chem-ph↗

arXiv2020

Dimension-free path-integral molecular dynamics without preconditioning

Convergence with respect to imaginary-time discretization is an essential part of any path-integral-based calculation. However, an unfortunate property of existing non-preconditioned numerical integration schemes for path-integral molecular dynamics (PIMD) - including ring-polymer molecular dynamics (RPMD) and thermostatted RPMD (T-RPMD) - is that for a given MD timestep, the overlap between the exact ring-polymer Boltzmann-Gibbs distribution and that sampled using MD becomes zero in the infinite-bead limit. This has clear implications for hybrid Metropolis Monte-Carlo/MD sampling schemes. We show that these problems can be avoided through the introduction of "dimension-free" numerical integration schemes for which the sampled ring-polymer position distribution has non-zero overlap with the exact distribution in the infinite-bead limit for the case of a harmonic potential. We show that dimension freedom can be achieved via mollification of the forces from the physical potential and with the BCOCB integration scheme. The dimension-free numerical integration schemes yield finite error bounds for a given MD timestep as the number of beads is taken to infinity; these conclusions are proven for harmonic potential and borne out numerically for anharmonic systems, including water. The numerical results for BCOCB are particularly striking, allowing for three-fold increases in the stable timestep for liquid water with respect to the Bussi-Parrinello (OBABO) and Leimkuhler (BAOAB) integrators while introducing negligible errors in the statistical properties and absorption spectrum. Importantly, the dimension-free, non-preconditioned integration schemes introduced here preserve ergodicity and global second-order accuracy, and they remain simple, black-box methods that avoid additional computational costs, tunable parameters, or system-specific implementations.

physics.chem-ph↗

arXiv2019

Cayley modification for strongly stable path-integral and ring-polymer molecular dynamics

Path-integral-based molecular dynamics (MD) simulations are widely used for the calculation of numerically exact quantum Boltzmann properties and approximate dynamical quantities. A nearly universal feature of MD numerical integration schemes for equations of motion based on imaginary-time path integrals is the use of harmonic normal modes for the exact evolution of the free ring-polymer positions and momenta. In this work, we demonstrate that this standard practice creates numerical artifacts. In the context of conservative (i.e., microcanonical) equations of motion, it leads to numerical instability. In the context of thermostatted (i.e., canonical) equations of motion, it leads to non-ergodicity of the sampling. These pathologies are generally proven to arise at integration timesteps that depend only on the system temperature and the number of ring-polymer beads, and they are numerically demonstrated for the cases of conventional ring-polymer molecular dynamics (RPMD) and thermostatted RPMD (TRPMD). Furthermore, it is demonstrated that these numerical artifacts are removed via replacement of the exact free ring-polymer evolution with a second-order approximation based on the Cayley transform. The Cayley modification introduced here can immediately be employed with almost every existing integration scheme for path-integral-based molecular dynamics - including path-integral MD (PIMD), RPMD, TRPMD, and centroid MD - providing strong symplectic stability and ergodicity to the numerical integration, at no penalty in terms of computational cost, algorithmic complexity, or accuracy of the overall MD timestep. Furthermore, it is shown that the improved numerical stability of the Cayley modification allows for the use of larger MD timesteps. We suspect that the Cayley modification will therefore find useful application in many future path-integral-based MD simulations.

physics.chem-ph↗

arXiv2018

Machine Learning Prediction of DNA Charge Transport

First principle calculations of charge transfer in DNA molecules are computationally expensive given that charge carriers migrate in interaction with intra- and inter-molecular atomic motion. Screening sequences, e.g. to identify excellent electrical conductors is challenging even when adopting coarse-grained models and effective computational schemes that do not explicitly describe atomic dynamics. In this work, we present a machine learning (ML) model that allows the inexpensive prediction of the electrical conductance of millions of {\it long} double-stranded DNA (dsDNA) sequences, reducing computational costs by orders of magnitude. The algorithm is trained on {\it short} DNA nanojunctions with $n=3-7$ base pairs. The electrical conductance of the training set is computed with a quantum scattering method, which captures charge-nuclei scattering processes. We demonstrate that the ML method accurately predicts the electrical conductance of varied dsDNA junctions tracing different transport mechanisms: coherent (short-range) quantum tunneling, on-resonance (ballistic) transport, and incoherent site-to-site hopping. Furthermore, the ML approach supports physical observations that clusters of nucleotides regulate DNA transport behavior. The input features tested in this work could be used in other ML studies of charge transport in complex polymers, in the search for promising electronic and thermoelectric materials.

cond-mat.mes-hall↗

arXiv2017

From exhaustive simulations to key principles in DNA nanoelectronics

Charge transfer can take place along double helical DNA over distances as long as 30 nanometers. However, given the active role of the thermal environment surrounding charge carriers in DNA, physical mechanisms driving the transfer process are highly debated. Moreover, the overall potential of DNA to act as a conducting material in nanoelectronic circuits is questionable. Here, we identify key principles in DNA nanoelectronics by performing an exhaustive computational study. The electronic structure of double-stranded DNA is described with a coarse-grained model. The dynamics of the molecular system and its environment is taken into account using a quantum scattering method, mimicking incoherent, elastic and inelastic effects. By analyzing all possible sequences with 3 to 7 base pairs, we identify fundamental principles in DNA nanoelectronics: The environment crucially influences the electrical conductance of DNA, and the majority of sequences conduct via a mixed, coherent-incoherent mechanism. Likewise, the metal-molecule coupling and the gateway states play significant roles in the transport behavior. While most sequences analyzed here are exposed to be rather poor electrical conductors, we identify exceptional DNA molecules, which we predict to be excellent and robust conductors of electric current over a wide range of physical conditions.

cond-mat.mes-hall↗

arXiv2016

Thermopower of molecular junctions: Tunneling to hopping crossover in DNA

We study the electrical conductance $G$ and the thermopower $S$ of single-molecule junctions, and reveal signatures of different transport mechanisms: off-resonant tunneling, on-resonant coherent (ballistic) motion, and multi-step hopping. These mechanisms are identified by studying the behavior of $G$ and $S$ while varying molecular length and temperature. Based on a simple one-dimensional model for molecular junctions, we derive approximate expressions for the thermopower in these different regimes. Analytical results are compared to numerical simulations, performed using a variant of Büttiker's probe technique, the so-called voltage-temperature probe, which allows us to phenomenologically introduce environmentally-induced elastic and inelastic electron scattering effects, while applying both voltage and temperature biases across the junction. We further simulate the thermopower of GC-rich DNA molecules with mediating A:T blocks, and manifest the tunneling-to-hopping crossover in both the electrical conductance and the thermopower, in accord with measurements by Y. Li et al., Nature Comm. 7, 11294 (2016).

cond-mat.mes-hall↗