Nonadiabatic State Research Articles

A self-consistent unified solid-multiphase flow shock model under complex thermodynamic states: For the application of mass-loaded single-turn coils

Single-turn coil (STC) is a destructive pulsed magnet aiming at 100–300 T magnetic field. Mass-loading is the method to increase STC magnetic field. In this study, a unified solid-multiphase flow model is proposed to solve the shock contact problem between the conductor and mass-loading material. This model gives the approach to equate the solid to viscid fluid and equate the melted material to solid and derives the constitutive model for the conductor under non-adiabatic state. Especially, the method to calculate non-adiabatic modulus is investigated. The results show that the equivalent viscosity of solid decreases as the strain rate rises. Moreover, the equivalent shear modulus of the melted solid increases as the strain rate rises, and considering this equivalent shear modulus rather than setting it to zero improves the simulation convergence significantly. This model can provide not only theoretical support for the optimal design of destructive pulse magnets but also methods for theoretical modeling of other types of electromagnetic explosion and shock contact experiments under non-adiabatic condition.

Influence of donor or acceptor presence on excitation states in molecular chains: Nonadiabatic polaron approach.

In this paper, we considered a molecular structure that consists of a molecular chain and an additional molecule (donor or acceptor) that can inject (or remove) single excitation (vibron, electron, etc.) onto the molecular chain. We assumed that the excitation forms a self-trapped state due to the interaction with mechanical oscillations of the chain structure elements. We analyzed the energy spectra of the excitation and showed that its state (when it migrates to the molecular chain) has the properties of the nonadiabatic polaron state. The conditions under which the excitation can migrate from one subsystem to another one were considered. It was shown that the presence of a "donor" molecule cannot significantly change the properties of the excitation located on the molecular chain. At the same time, the molecular chain can affect the position of the energy level of the excitation localized on the donor subsystem. Indirectly, this can influence the process of excitation migration from one subsystem to another one. The influence of the basic energy parameters of the system and the environment temperature on this process are discussed. The entire system was assumed to be in thermal equilibrium with the environment.

Enhanced optical conductivity and many-body effects in strongly-driven photo-excited semi-metallic graphite

The excitation of quasi-particles near the extrema of the electronic band structure is a gateway to electronic phase transitions in condensed matter. In a many-body system, quasi-particle dynamics are strongly influenced by the electronic single-particle structure and have been extensively studied in the weak optical excitation regime. Yet, under strong optical excitation, where light fields coherently drive carriers, the dynamics of many-body interactions that can lead to new quantum phases remain largely unresolved. Here, we induce such a highly non-equilibrium many-body state through strong optical excitation of charge carriers near the van Hove singularity in graphite. We investigate the system’s evolution into a strongly-driven photo-excited state with attosecond soft X-ray core-level spectroscopy. We find an enhancement of the optical conductivity of nearly ten times the quantum conductivity and pinpoint it to carrier excitations in flat bands. This interaction regime is robust against carrier-carrier interaction with coherent optical phonons acting as an attractive force reminiscent of superconductivity. The strongly-driven non-equilibrium state is markedly different from the single-particle structure and macroscopic conductivity and is a consequence of the non-adiabatic many-body state.

Coronal Heating Rate in the Slow Solar Wind

This Letter reports the first observational estimate of the heating rate in the slowly expanding solar corona. The analysis exploits the simultaneous remote and local observations of the same coronal plasma volume, with the Solar Orbiter/Metis and the Parker Solar Probe instruments, respectively, and relies on the basic solar wind magnetohydrodynamic equations. As expected, energy losses are a minor fraction of the solar wind energy flux, since most of the energy dissipation that feeds the heating and acceleration of the coronal flow occurs much closer to the Sun than the heights probed in the present study, which range from 6.3 to 13.3 R ⊙. The energy deposited to the supersonic wind is then used to explain the observed slight residual wind acceleration and to maintain the plasma in a nonadiabatic state. As derived in the Wentzel–Kramers–Brillouin limit, the present energy transfer rate estimates provide a lower limit, which can be very useful in refining the turbulence-based modeling of coronal heating and subsequent solar wind acceleration.

Critical temperature of the nonadiabatic superconducting state in mono- and bilayer systems

Critical temperature of the nonadiabatic superconducting state in mono- and bilayer systems

Crossover of energy deposition and semi-stable chemical bonding in the nonadiabatic dynamics of GaN under proton irradiation

Understanding the ion-solid interactions of charged particles in materials facilitates the development of ion beam irradiation techniques. Combining Ehrenfest dynamics and time-dependent density-functional theory, we investigated the electronic stopping power (ESP) of an energetic proton in GaN crystal and studied the ultrafast dynamic interaction between the proton and target atoms during the nonadiabatic process. We found a crossover phenomenon of ESP at 0.36 a.u. along the <100> and <110> channels, which is interpreted by the charge transfer between the host material and the projectile and the stopping force exerted on the proton. At velocities of 0.2 and 1.7 a.u., we demonstrated that the reversal of the average number of charge transfer and the average axial force resulted in the reversed energy deposition rate and ESP in the corresponding channel. Further analysis of the evolution of non-adiabatic electronic states revealed the existence of the transient and semi-stable N–H chemical bonding during irradiation process, which is introduced by the electron clouds overlap of N sp 3 hybridization and the s orbitals of the proton. These results provide meaningful information for the interactions between energetic ions and matter.

Optimally Controlled Non-Adiabatic Quantum State Transmission in the Presence of Quantum Noise

Pulse-controlled non-adiabatic quantum state transmission (QST) was proposed many years ago. However, in practice environmental noise inevitably damages communication quality in the proposal. In this paper, we study the optimally controlled non-adiabatic QST in the presence of quantum noise. By using the Adam algorithm, we find that the optimal pulse sequence can dramatically enhance the transmission fidelity of such an open system. In comparison with the idealized pulse sequence in a closed system, it is interesting to note that the improvement of the fidelity obtained by the Adam algorithm can even be better for a bath strongly coupled to the system. Furthermore, we find that the Adam algorithm remains powerful for different numbers of sites and different types of Lindblad operators, showing its universality in performing optimal control of quantum information processing tasks.

Surface crossing and energy flow in many-dimensional quantum systems

Energy flow in molecules, like the dynamics of other many-dimensional finite systems, involves quantum transport across a dense network of near-resonant states. For molecules in their electronic ground state, the network is ordinarily provided by anharmonic vibrational Fermi resonances. Surface crossing between different electronic states provides another route to chaotic motion and energy redistribution. We show that nonadiabatic coupling between electronic energy surfaces facilitates vibrational energy flow and, conversely, anharmonic vibrational couplings facilitate nonadiabatic electronic state mixing. A generalization of the Logan-Wolynes theory of quantum energy flow in many-dimensional Fermi resonance systems to the two-surface case gives a phase diagram describing the boundary between localized quantum dynamics and global energy flow. We explore these predictions and test them using a model inspired by the problem of electronic excitation energy transfer in the photosynthetic reaction center. Using an explicit numerical solution of the time-dependent Schrödinger equation for this ten-dimensional model, we find quite good agreement with the expectations from the approximate analytical theory.

Effects of Wall Temperature on Hypersonic Impinging Shock-Wave/Turbulent-Boundary-Layer Interactions

We carry out a parametric study of hypersonic impinging shock-wave/turbulent-boundary-layer interactions (SBLIs) at hypersonic conditions (Mach number 6.0) by means of numerical simulation of the Reynolds-averaged Navier–Stokes (RANS) equations, with the eventual goal of establishing wall temperature and Reynolds number effects. Comparison with available direct numerical simulation and experimental data shows that RANS is capable of predicting the main features of SBLI, namely, typical size and distribution of the wall properties. A large number of flow cases were computed to examine the scaling of the global flow parameters over a wide range of wall temperatures and Reynolds numbers. As expected, the interaction zone is reduced as the wall is cooled, and as the Reynolds number is increased. A modified form of the scaling originally introduced by Souverein et al. [Journal of Fluid Mechanics, Vol. 714, 2013, pp. 505–535] is here considered to account for nonadiabatic wall state, which is found to successfully collapse the data to the distributions obtained for adiabatic flow, with some remaining deviations associated with low-Reynolds-number effects.

Nonadiabatic quantum state engineering by time-dependent decoherence-free subspaces in open quantum systems

We extend the theory of quantum state engineering (QSE) to the open quantum systems which simultaneously suffer time-dependent decoherence and time-independent decoherence. A hybrid approach is proposed to effectively realize QSE by combination of time-dependent decoherence-free subspaces and shortcuts to adiabaticity theories. As an application, a concrete single-qubit QSE example with an open five-level system is presented. Numerical simulations confirm that the approach is reliable and robust against both of time-dependent decoherence and time-independent decoherence. Certain dissipation effects are no longer harmful but play a positive role in the QSE. In addition, the approach can be generalized to realize QSE in high-dimensional quantum systems. Therefore, this proposal is quite useful for quantum computation and quantum information processing in open systems.

First-Principles Demonstration of Nonadiabatic Thouless Pumping of Electrons in a Molecular System.

We demonstrate nonadiabatic Thouless pumping of electrons in trans-polyacetylene in the framework of Floquet engineering using first-principles theory. We identify the regimes in which the quantized pump is operative with respect to the driving electric field for a time-dependent Hamiltonian. By employing the time-dependent maximally localized Wannier functions in real-time time-dependent density functional theory simulation, we connect the winding number, a topological invariant, to a molecular-level understanding of the quantized pumping. While the pumping dynamics constitutes the opposing movement of the Wannier functions that represent both double and single bonds, the resulting current is unidirectional due to the greater number of double-bond electrons. Using a gauge-invariant formulation called dynamical transition orbitals, an alternative viewpoint on the nonequilibrium dynamics is obtained in terms of the particle-hole excitation. A single time-dependent transition orbital is found to be largely responsible for the observed quantized pumping. In this representation, the pumping dynamics manifests itself in the dynamics of this single orbital as it undergoes changes from its π bonding orbital character at equilibrium to acquiring resonance and antibonding character in the driving cycle. The work demonstrates the Floquet engineering of the nonadiabatic topological state in an extended molecular system, paving the way for experimental realization of the new quantum material phase.

The shape of the electric dipole function determines the sub-picosecond dynamics of anharmonic vibrational polaritons

Vibrational strong coupling has emerged as a promising route for manipulating the reactivity of molecules inside infrared cavities. We develop a full-quantum methodology to study the unitary dynamics of a single anharmonic vibrational mode interacting with a quantized infrared cavity field. By comparing multi-configurational time-dependent Hartree simulations for an intracavity Morse oscillator with an equivalent formulation of the problem in Hilbert space, we describe for the first time the essential role of permanent dipole moments in the femtosecond dynamics of vibrational polariton wavepackets. We classify molecules into three general families according to the shape of their electric dipole function de(q) along the vibrational mode coordinate q. For polar species with a positive slope of the dipole function at equilibrium, an initial diabatic light-matter product state without vibrational or cavity excitations evolves into a polariton wavepacket with a large number of intracavity photons for interaction strengths at the conventional onset of ultrastrong coupling. This buildup of the cavity photon amplitude is accompanied by an effective lengthening of the vibrational mode that is comparable with a laser-induced vibrational excitation in free space. In contrast, polar molecules with a negative slope of the dipole function experience an effective mode shortening, under equivalent coupling conditions. We validate our predictions using realistic ab initio ground state potentials and dipole functions for HF and CO2 molecules. We also propose a non-adiabatic state preparation scheme to generate vibrational polaritons with molecules near infrared nanoantennas for the spontaneous radiation of infrared quantum light.

Wannier States of FCC Symmetry Qualifying Paramagnetic NiO to Be a Mott Insulator

This letter extends my recent paper on antiferromagnetic NiO [Structural Distortion Stabilizing the Antiferromagnetic and Insulating Ground State of NiO, Symmetry 2020, 12(1), 56] by including also the paramagnetic phase of this compound. I report evidence that paramagnetic NiO possesses a narrow, roughly half-filled energy band that produces a nonadiabatic atomic-like motion providing the basis for a Mott insulator in the paramagnetic phase. While the atomic-like motion operating in the antiferromagnetic phase is adapted to the symmetry of the antiferromagnetic state, in the paramagnetic phase, the related localized states are represented by optimally localized Wannier functions possessing the full fcc symmetry of paramagnetic NiO. The nonadiabatic Wannier states are twofold degenerate, have d-like symmetry, and are situated at the Ni atoms.

Nonadiabatic simulation of singlet fission dynamics in tetracene clusters: The topology of quantum coherence in a global view

The delocalization of excitonic states and the interstate quantum coherence are of great importance in understanding fundamental mechanisms in exciton dynamics such as singlet fission. The accurate theoretical description on this key component requires dynamic simulations to be performed at the molecular level in a nonadiabatic framework. Here, we apply the recently developed nonadiabatic active state trajectory method to simulate fission dynamics in tetracene clusters of up to 10 monomers. It is shown that a global view of the topology of quantum coherence in terms of molecular details such as packing configurations, spatial delocalization of states, and the topology of coherent regime plays an important role in modulating fission dynamics, which suggests a new focus for nonadiabatic control of exciton dynamics and provides valuable dynamical information and physical insights for artificial design.

Elucidation of near-resonance vibronic coherence lifetimes by nonadiabatic electronic-vibrational state character mixing

Recent work suggests that the long-lived coherences observed in both natural and artificial light-harvesting systems (such as the Fenna-Matthews-Olson complex) could be attributed to the mixing of the pigments' electronic and vibrational degrees of freedom. To investigate the underlying mechanism of these long coherence lifetimes, a sophisticated description of interactions between the molecular aggregates and the nonequilibrium fluctuations in the surrounding environment is necessary. This is done by implementing the hierarchical equations of motion approach on model homodimers, a method used in the intermediate coupling regime for many molecular aggregates wherein the nonequilibrium environment phonons play nontrivial roles in exciton dynamics. Here we report a character change in the vibronic states-reflective of property mixing between the electronic and vibrational states-induced by an interplay between system coupling parameters within the exciton-vibrational near-resonance regime. This mixing dictates vital aspects of coherence lifetime; by tracking the degree of mixing, we are able to elucidate the relationship between coherence lifetime and both the electronic energy fluctuation and the vibrational relaxation dephasing pathways.

Nonadiabatic rotational states of the hydrogen molecule.

We present a new computational method for the determination of energy levels in four-particle systems like H2, HD, and HeH+ using explicitly correlated exponential basis functions and analytic integration formulas. In solving the Schrödinger equation, no adiabatic separation of the nuclear and electronic degrees of freedom is introduced. We provide formulas for the coupling between the rotational and electronic angular momenta, which enable calculations of arbitrary rotationally excited energy levels. To illustrate the high numerical efficiency of the method, we present the results for various states of the hydrogen molecule. The relative accuracy to which we determined the nonrelativistic energy reached the level of 10-12-10-13, which corresponds to an uncertainty of 10-7-10-8 cm-1.

Non-adiabatic quantum state preparation and quantum state transport in chains of Rydberg atoms

Motivated by recent progress in the experimental manipulation of cold atoms in optical lattices, we study three different protocols for non-adiabatic quantum state preparation and state transport in chains of Rydberg atoms. The protocols we discuss are based on the blockade mechanism between atoms which, when excited to a Rydberg state, interact through a van der Waals potential, and rely on single-site addressing. Specifically, we discuss protocols for efficient creation of an antiferromagnetic GHZ state, a class of matrix product states including a so-called Rydberg crystal and for the state transport of a single-qubit quantum state between two ends of a chain of atoms. We identify system parameters allowing for the operation of the protocols on timescales shorter than the lifetime of the Rydberg states while yielding high fidelity output states. We discuss the effect of positional disorder on the resulting states and comment on limitations due to other sources of noise such as radiative decay of the Rydberg states. The proposed protocols provide a testbed for benchmarking the performance of quantum information processing platforms based on Rydberg atoms.

Nodeless vibrational amplitudes and quantum nonadiabatic dynamics in the nested funnel for a pseudo Jahn-Teller molecule or homodimer.

The nonadiabatic states and dynamics are investigated for a linear vibronic coupling Hamiltonian with a static electronic splitting and weak off-diagonal Jahn-Teller coupling through a single vibration with a vibrational-electronic resonance. With a transformation of the electronic basis, this Hamiltonian is also applicable to the anti-correlated vibration in a symmetric homodimer with marginally strong constant off-diagonal coupling, where the non-adiabatic states and dynamics model electronic excitation energy transfer or self-exchange electron transfer. For parameters modeling a free-base naphthalocyanine, the nonadiabatic couplings are deeply quantum mechanical and depend on wavepacket width; scalar couplings are as important as the derivative couplings that are usually interpreted to depend on vibrational velocity in semiclassical curve crossing or surface hopping theories. A colored visualization scheme that fully characterizes the non-adiabatic states using the exact factorization is developed. The nonadiabatic states in this nested funnel have nodeless vibrational factors with strongly avoided zeroes in their vibrational probability densities. Vibronic dynamics are visualized through the vibrational coordinate dependent density of the time-dependent dipole moment in free induction decay. Vibrational motion is amplified by the nonadiabatic couplings, with asymmetric and anisotropic motions that depend upon the excitation polarization in the molecular frame and can be reversed by a change in polarization. This generates a vibrational quantum beat anisotropy in excess of 2/5. The amplitude of vibrational motion can be larger than that on the uncoupled potentials, and the electronic population transfer is maximized within one vibrational period. Most of these dynamics are missed by the adiabatic approximation, and some electronic and vibrational motions are completely suppressed by the Condon approximation of a coordinate-independent transition dipole between adiabatic states. For all initial conditions investigated, the initial nonadiabatic electronic motion is driven towards the lower adiabatic state, and criteria for this directed motion are discussed.

Properties of suprathermal electrons associated with discrete auroral arcs

AbstractWe report on the properties of suprathermal electrons observed over three discrete auroral arcs from a sounding rocket. By applying shifted kappa distributions and analyzing kappa parameters (density, temperature, and kappa), we found three novel characteristics to provide clues to understand the auroral acceleration mechanisms and magnetosphere‐ionosphere coupling processes. First, the auroral potential drop was proportional to the inverse square of kappa, consistent with previous theoretical investigations by Dors and Kletzing (). The observed dependency was slightly stronger than their calculations, suggesting additional contributions from nonlinear plasma processes. Second, the polytropic relation showed nonadiabatic (near isothermal) state of the source electrons. This can provide a restriction on the pressure balance issues in the plasma sheet convection. Third, there was a clear difference in the polytropic and kappa indices for the first arc as opposed to the second and the third arcs, suggesting different source locations in the plasma sheet for the precipitating electrons that cause these nearby arcs.

Reversibility and energy dissipation in adiabatic superconductor logic

Reversible computing is considered to be a key technology to achieve an extremely high energy efficiency in future computers. In this study, we investigated the relationship between reversibility and energy dissipation in adiabatic superconductor logic. We analyzed the evolution of phase differences of Josephson junctions in the reversible quantum-flux-parametron (RQFP) gate and confirmed that the phase differences can change time reversibly, which indicates that the RQFP gate is physically, as well as logically, reversible. We calculated energy dissipation required for the RQFP gate to perform a logic operation and numerically demonstrated that the energy dissipation can fall below the thermal limit, or the Landauer bound, by lowering operation frequencies. We also investigated the 1-bit-erasure gate as a logically irreversible gate and the quasi-RQFP gate as a physically irreversible gate. We calculated the energy dissipation of these irreversible gates and showed that the energy dissipation of these gate is dominated by non-adiabatic state changes, which are induced by unwanted interactions between gates due to logical or physical irreversibility. Our results show that, in reversible computing using adiabatic superconductor logic, logical and physical reversibility are required to achieve energy dissipation smaller than the Landauer bound without non-adiabatic processes caused by gate interactions.