Coherent Hopping Research Articles

Coherent Charge Hopping Suppresses Photoexcited Polarons in ErFeO3

We measure how coherent charge hopping competes with and slows small polaron formation. The coupling of photoexcited charge carriers with phonons in the crystal lattice that results in polaron formation causes carrier localization and limits transport to site-to-site hopping. ErFeO3, a rare-earth orthoferrite, is designed where the large rare earth atom frustrates the FeO6 octahedra, reducing the energetic favorability of polaron formation. We compare transient extreme ultraviolet (XUV) measurements with ab initio theory and transport measurements to quantify the polaron formation rate and mobility. Polaron formation occurs within several picoseconds following multiple coherent charge hopping events between neighboring Fe3+–Fe2+ sites. This timescale is more than an order of magnitude longer compared to previously studied materials. The delay in polaron formation is notable because the photoexcited carriers shed excess thermal energy before forming the polaron. To date, polarons have been measured to form instantaneously with the first electron-phonon scattering event. The measured interplay between optical phonons, electron coupling, and on-site lattice deformation emphasizes the importance of dynamic electron correlations for tuning polaron formation in photocatalysts.

Entanglement transition and heterogeneity in long-range quadratic Lindbladians

The generation of entanglement in mixed states is relevant to quantum systems coupled to an environment. The dissipative and mixing properties of the environment are unavoidable in physical platforms for quantum simulation and information processing, where entanglement can be a vital resource. In this work, we explore entanglement and heterogeneity in random Lindbladian dynamics describing open quantum systems. We propose a model of a one-dimensional chain of noninteracting, spinless fermions coupled to a local ensemble of baths. The jump operator mediating the interaction with the bath linked to each site has a power-law tail with an exponent p. We show that the system undergoes volume-to-area law entanglement phase transition in the mixed steady state by tuning p which remains stable in the presence of coherent hopping. Unlike the entanglement transition in the pure-state quantum trajectories of open systems, this transition is exhibited by the averaged steady-state density matrix of the Lindbladian. The steady state in the area-law phase is characterized by a spatial heterogeneity in local population imbalance, while the jump operators exhibit a constant participation ratio of the sites they affect. Our work provides a theoretical description of an entanglement transition realized in long-ranged open quantum systems and provides an avenue to stabilize quantum correlations in mixed states. Published by the American Physical Society 2024

Quantum reaction-limited reaction–diffusion dynamics of noninteracting Bose gases

We investigate quantum reaction–diffusion (RD) systems in one-dimension with bosonic particles that coherently hop in a lattice, and when brought in range react dissipatively. Such reactions involve binary annihilation ( A+A→∅ ) and coagulation ( A+A→A ) of particles at distance d. We consider the reaction-limited regime, where dissipative reactions take place at a rate that is small compared to that of coherent hopping. In classical RD systems, this regime is correctly captured by the mean-field approximation. In quantum RD systems, for noninteracting fermionic systems, the reaction-limited regime recently attracted considerable attention because it has been shown to give universal power law decay beyond mean field for the density of particles as a function of time. Here, we address the question whether such universal behavior is present also in the case of the noninteracting Bose gas. We show that beyond mean-field density decay for bosons is possible only for reactions that allow for destructive interference of different decay channels. Furthermore, we study an absorbing-state phase transition induced by the competition between branching A→A+A , decay A→∅ and coagulation A+A→A . We find a stationary phase-diagram, where a first and a second-order transition line meet at a bicritical point which is described by tricritical directed percolation. These results show that quantum statistics significantly impact on both the stationary and the dynamical universal behavior of quantum RD systems.

Coherent charge hopping suppresses photoexcited small polarons in ErFeO3 by antiadiabatic formation mechanism.

Polarons are prevalent in condensed matter systems with strong electron-phonon coupling. The adiabaticity of the polaron relates to its transport properties and spatial extent. To date, only adiabatic small polaron formation has been measured following photoexcitation. The lattice reorganization energy is large enough that the first electron-optical phonon scattering event creates a small polaron without requiring substantial carrier thermalization. We measure that frustrating the iron-centered octahedra in the rare-earth orthoferrite ErFeO3 leads to antiadiabatic polaron formation. Coherent charge hopping between neighboring Fe3+─Fe2+ sites is measured with transient extreme ultraviolet spectroscopy and lasts several picoseconds before the polaron forms. The resulting small polaron formation time is an order of magnitude longer than previous measurements and indicates a shallow potential well, even in the excited state. The results emphasize the importance of considering dynamic electron-electron correlations, not just electron-phonon-induced lattice changes, for small polarons for transport, catalysis, and photoexcited applications.

Quantum walk in stochastic environment.

We consider a quantized version of the Sinai-Derrida model for "random walk in random environment." The model is defined in terms of a Lindblad master equation. For a ring geometry (a chain with periodic boundary condition) it features a delocalization-transition as the bias in increased beyond a critical value, indicating that the relaxation becomes underdamped. Counterintuitively, the effective disorder is enhanced due to coherent hopping. We analyze in detail this enhancement and its dependence on the model parameters. The nonmonotonic dependence of the Lindbladian spectrum on the rate of the coherent transitions is highlighted.

A fine synchronization method for coherent fast frequency hopping

A fine synchronization method for coherent fast frequency hopping

Reaction-Limited Quantum Reaction-Diffusion Dynamics.

We consider the quantum nonequilibrium dynamics of systems where fermionic particles coherently hop on a one-dimensional lattice and are subject to dissipative processes analogous to those of classical reaction-diffusion models. Particles can either annihilate in pairs, A+A→0, or coagulate upon contact, A+A→A, and possibly also branch, A→A+A. In classical settings, the interplay between these processes and particle diffusion leads to critical dynamics as well as to absorbing-state phase transitions. Here, we analyze the impact of coherent hopping and of quantum superposition, focusing on the so-called reaction-limited regime. Here, spatial density fluctuations are quickly smoothed out due to fast hopping, which for classical systems is described by a mean-field approach. By exploiting the time-dependent generalized Gibbs ensemble method, we demonstrate that quantum coherence and destructive interference play a crucial role in these systems and are responsible for the emergence of locally protected dark states and collective behavior beyond mean field. This can manifest both at stationarity and during the relaxation dynamics. Our analytical results highlight fundamental differences between classical nonequilibrium dynamics and their quantum counterpart and show that quantum effects indeed change collective universal behavior.

High-Efficiency PCSK-CFFH System Design for IoT Networks

Industrial Internet of Things (IIoT) brings opportunities for innovation and upgrading to industrial production, but meanwhile, it poses unprecedented challenges on the physical layer of wireless communications. In this article, we propose a novel frequency hopping transmission scheme for IIoT, which owns much high efficiency and strong anti-jamming ability. This new scheme is built based on the combination of coherent fast frequency hopping (CFFH) and cyclic code shift key (CCSK), named phase cyclic shift-keying-based CFFH (PCSK-CFFH). For the proposed PCSK-CFFH system, the shift of orthogonal base sequence is adopted to modulate the phases among interhop, instead of transmitting each hop with the same phase as conventional CFFH. This scheme is able to further exploit the extra dimensions of CFFH signals and enables the CFFH system to transmit additional information at no extra cost on either bandwidth or power. Moreover, the bit error rate performance of the proposed PCSK-CFFH system is analyzed theoretically. To improve its ability against severe narrow-band jamming, the selection combining is introduced in our scheme. Furthermore, the anti-jamming performance of the proposed PCSK-CFFH system is also demonstrated. Finally, the simulation results are shown to demonstrate that: by introducing the interhop dimension to CFFH, PCSK-CFFH improves the power efficiency and spectrum efficiency by multiple times and simultaneously inherits the excellent anti-jamming performance of the conventional CFFH system. It can be concluded that the proposed PCSK-CFFH scheme has a great potential to be applied to low-power and highly reliable IIoT communications.

Transport threshold in a quantum model for the KscA ion channel

The mechanism behind the high throughput rate in K+ channels is still an open problem. However, recent simulations have shown that the passage of potassium through the K+ channel core, the so-called selectivity filter (SF), is water-free against models where the strength of Coulomb repulsion freezes ions conduction. Thus, it has been suggested that coherent quantum hopping might be relevant in mediating ion conduction. Within the quantum approach and the hypothesis of desolvated ions along the pathway, we start with several particles in a source to see how they go across a SF, modeled by a linear chain of sites, to be collected in a drain. We show that the average SF occupancy is three ions, and the ion transfer rate is ∼108 ions s−1, results which agree with the recent findings in the literature.

Quantum versus classical transport of energy in coupled two-level systems

We consider the problem of energy transport in a chain of coupled quantum systems with the goal of shedding light on how nonclassical resources can affect transport. We study the cases for which either coherent or incoherent energy hopping takes place in the chain. Here, incoherent energy hopping is referred to as the "classical" scenario in allusion to its fully diagonal dynamics in the basis formed by the eigenstates of the decoupled sites. We focus on the case of a linear chain of two-level sites and find a hopping rate threshold above which the coherent quantum case is more efficient than the incoherent counterpart. We then link the quantum hopping rate to the coherence global maximum, which allows us to state that there is a coherence threshold above which the quantum scenario is more efficient. Next, we consider the integrated coherence generated by the dynamics and show how it is related to what is known as the invasiveness of a quantum operation. Our results strongly suggest the significant role played by quantum invasiveness as a resource for quantum transport.

Quantum stochastic transport along chains

The spreading of a particle along a chain, and its relaxation, are central themes in statistical and quantum mechanics. One wonders what are the consequences of the interplay between coherent and stochastic transitions. This fundamental puzzle has not been addressed in the literature, though closely related themes were in the focus of the Physics literature throughout the last century, highlighting quantum versions of Brownian motion. Most recently this question has surfaced again in the context of photo-synthesis. Here we consider both an infinite tight-binding chain and a finite ring within the framework of an Ohmic master equation. With added disorder it becomes the quantum version of the Sinai-Derrida-Hatano-Nelson model, which features sliding and delocalization transitions. We highlight non-monotonic dependence of the current on the bias, and a counter-intuitive enhancement of the effective disorder due to coherent hopping.

Phase Coherent Frequency Hopping in Direct Digital Synthesizers and Phase Locked Loops

Phase coherent, frequency hopping direct digital synthesizer (DDS) and Type-II phase locked loop (PLL) circuits are presented in this paper. The proposed approach eliminates the memory effects of prior frequency states in the phase (DDS) and fractional (PLL) accumulators by employing a master accumulator with a fixed increment and multiplying its output to generate the appropriate phase and fractional outputs. This approach allows for an arbitrary sequence of frequency hops, since it is not based on multiple simultaneous accumulators to store phase. We present phase coherent topologies for standard and parallelized DDS circuits, a fractional-N PLL and a multistage sigma-delta modulator (MASH)-111 fractional-N PLL, along with mathematical analysis showing phase coherency. We also present measured results of parallelized DDS and MASH-111 fractional-N PLL hardware.

Optical Activity from the Exciton Aharonov–Bohm Effect: A Floquet Engineering Approach

Floquet engineering is a convenient strategy to induce nonequilibrium phenomena in molecular and solid-state systems, or to dramatically alter the physicochemical properties of matter, bypassing costly and time-consuming synthetic modifications. In this article, we investigate theoretically some interesting consequences of the fact that an originally achiral molecular system can exhibit nonzero circular dichroism (CD) when it is driven with elliptically polarized light. More specifically, we consider an isotropic ensemble of small cyclic molecular aggregates in solution whose local low-frequency vibrational modes are driven by an elliptically polarized continuous-wave infrared pump. We attribute the origin of a nonzero CD signal to time-reversal symmetry breaking due to an excitonic Aharonov-Bohm (AB) phase arising from a time-varying laser electric field, together with coherent interchromophoric exciton hopping. The obtained Floquet engineered excitonic AB phases are far more tunable than analogous magnetically-induced electronic AB phases in nanoscale rings, highlighting a virtually unexplored potential that Floquet engineered AB phases have in the coherent control of molecular processes and simultaneously introducing new analogues of magneto-optical effects in molecular systems which bypass the use of strong magnetic fields.

125Te-NMR Study in Novel Superconductor Pb1−xTlxTe with Valence Skipping Dopants

Pb1−xTlxTe is an anomalous low carrier density superconductor for which the origin of the superconductivity is not understood. Thallium is the only dopant to cause superconductivity in PbTe, suggesting that these specific impurities have a unique effect on the electronic states. Systematic 125Te-NMR studies on single-crystallines Pb1−xTlxTe (x = 0, 0.35, 1.0 at%) reveal that the Tl dopants induce spatially inhomogeneous electronic states around the Tl dopants. In the superconducting sample at x = 1.0 at%, 125Te nuclear spin relaxation rate (1/T1T) in the vicinity of the Tl dopants is unexpectedly enhanced below $\sim $ 10 K. This coincides with the temperature below which the resistivity exhibits an upturn. By contrast, such anomalies were not detected in the non-superconducting sample at x = 0.35 at%. These observations can be consistently explained by charge Kondo effect, in which two nearly degenerate valence states of the Tl dopant form a resonating valence state upon cooling below 10 K. Based on these observations, we suggest that the coherent hopping of 6s-electron pair may provide the pairing interaction (i.e., a negative-U scenario), leading to the anomalously high Tc found for Pb1−xTlxTe.

Nonreciprocal signal routing in an active quantum network

As superconductor quantum technologies are moving towards large-scale integrated circuits, a robust and flexible approach to routing photons at the quantum level becomes a critical problem. Active circuits, which contain parametrically driven elements selectively embedded in the circuit offer a viable solution. Here, we present a general strategy for routing nonreciprocally quantum signals between two sites of a given lattice of oscillators, implementable with existing superconducting circuit components. Our approach makes use of a dual lattice of overdamped oscillators linking the nodes of the main lattice. Solutions for spatially selective driving of the lattice elements can be found, which optimally balance coherent and dissipative hopping of microwave photons to nonreciprocally route signals between two given nodes. In certain lattices these optimal solutions are obtained at the exceptional point of the dynamical matrix of the network. We also demonstrate that signal and noise transmission characteristics can be separately optimized.

Optimal dephasing for ballistic energy transfer in disordered linear chains.

We study the interplay between dephasing, disorder, and coupling to a sink on transport efficiency in a one-dimensional chain of finite length N, and in particular the beneficial or detrimental effect of dephasing on transport. The excitation moves along the chain by coherent nearest-neighbor hopping Ω, under the action of static disorder W and dephasing γ. The last site is coupled to an external acceptor system (sink), where the excitation can be trapped with a rate Γ_{trap}. While it is known that dephasing can help transport in the localized regime, here we show that dephasing can enhance energy transfer even in the ballistic regime. Specifically, in the localized regime we recover previous results, where the optimal dephasing is independent of the chain length and proportional to W or W^{2}/Ω. In the ballistic regime, the optimal dephasing decreases as 1/N or 1/sqrt[N], respectively, for weak and moderate static disorder. When focusing on the excitation starting at the beginning of the chain, dephasing can help excitation transfer only above a critical value of disorder W^{cr}, which strongly depends on the sink coupling strength Γ_{trap}. Analytic solutions are obtained for short chains.

Generalization of fewest-switches surface hopping for coherences.

Fewest-switches surface hopping (FSSH) is perhaps the most widely used mixed quantum-classical approach for the modeling of non-adiabatic processes, but its original formulation is restricted to (adiabatic) population terms of the quantum density matrix, leaving its implementations with an inconsistency in the treatment of populations and coherences. In this article, we propose a generalization of FSSH that treats both coherence and population terms on equal footing and which formally reduces to the conventional FSSH algorithm for the case of populations. This approach, coherent fewest-switches surface hopping (C-FSSH), employs a decoupling of population relaxation and pure dephasing and involves two replicas of the classical trajectories interacting with two active surfaces. Through extensive benchmark calculations of a spin-boson model involving a Debye spectral density, we demonstrate the potential of C-FSSH to deliver highly accurate results for a large region of parameter space. Its uniform description of populations and coherences is found to resolve incorrect behavior observed for conventional FSSH in various cases, in particular at low temperature, while the parameter space regions where it breaks down are shown to be quite limited. Its computational expenses are virtually identical to conventional FSSH.

Bias-induced conductance switching in single molecule junctions containing a redox-active transition metal complex.

The paper provides a comprehensive theoretical description of electron transport through transition metal complexes in single molecule junctions, where the main focus is on an analysis of the structural parameters responsible for bias-induced conductance switching as found in recent experiments, where an interpretation was provided by our simulations. The switching could be theoretically explained by a two-channel model combining coherent electron transport and electron hopping, where the underlying mechanism could be identified as a charging of the molecule in the junction made possible by the presence of a localized electronic state on the transition metal center. In this article, we present a framework for the description of an electron hopping-based switching process within the semi-classical Marcus–Hush theory, where all relevant quantities are calculated on the basis of density functional theory (DFT). Additionally, structural aspects of the junction and their respective importance for the occurrence of irreversible switching are discussed.Graphical abstract

Tailoring Rydberg interactions via Förster resonances: state combinations, hopping and angular dependence

Förster resonances provide a highly flexible tool to tune both the strength and the angular shape of interactions between two Rydberg atoms. We give a detailed explanation about how Förster resonances can be found by searching through a large range of possible quantum number combinations. We apply our search method to SS, SD and DD pair states of 87Rb with principal quantum numbers from 30 to 100, taking into account the fine structure splitting of the Rydberg states. We find various strong resonances between atoms with a large difference in principal quantum numbers. We quantify the strength of these resonances by introducing a figure of merit which is independent of the magnetic quantum numbers and geometry to classify the resonances by interaction strength. We further predict to what extent excitation exchange is possible on different resonances and point out limitations of the coherent hopping process. Finally, we discuss the angular dependence of the dipole–dipole interaction and its tunability near resonances.

Long-Range Tunneling Processes across Ferritin-Based Junctions.

The mechanism of long-range charge transport across tunneling junctions with monolayers of ferritin is investigated. It is shown that the mechanism can be switched between coherent tunneling, sequential tunneling, and hopping by changing the iron content inside the ferritin. This study shows that ferritins are an interesting class of biomolecules to control charge transport.