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Resonant transport occurs when there is a matching of frequencies across some spatial medium, increasing the efficiency of shuttling particles from one reservoir to another. We demonstrate that in a periodically driven, many--body titled lattice, there are sets of spatially fractured resonances. These ``emanate'' from two essential resonances due to scattering off internal surfaces created when the driving frequency and many--body interaction strength vary, a scattering reminiscent of lens flare. The confluence of these fractured resonances dramatically enhances transport. At one confluence, the interaction strength is finite and the essential resonance arises due to the interplay of interaction with the counter--rotating terms of the periodic drive. We discuss the origin and structure of the fractured resonances, as well as the scaling of the conductance with system parameters. These results furnish a new example of the richness of open, driven, many--body systems., Comment: significantly revised version! comments welcome

Extended reservoirs provide a framework for capturing macroscopic, continuum environments, such as metallic electrodes driving a current through a nanoscale contact, impurity, or material. We examine the application of this approach to periodically driven systems, specifically in the context of quantum transport. As with non--equilibrium steady states in time--independent scenarios, the current displays a Kramers' turnover including the formation of a plateau region that captures the physical, continuum limit response. We demonstrate that a simple stability criteria identifies an appropriate relaxation rate to target this physical plateau. Using this approach, we study quantum transport through a periodically driven tilted lattice coupled to two metallic reservoirs held at a finite bias and temperature. We use this model to benchmark the extended reservoir approach and assess the stability criteria. The approach recovers well--understood physical behavior in the limit of weak system--reservoir coupling. Extended reservoirs enable addressing strong coupling and non--linear response as well, where we analyze how transport responds to the dynamics inside the driven lattice. These results set the foundations for the use of extended reservoir approach for periodically driven, quantum systems, such as many--body Floquet states., Comment: 14 pages, 8 figures

The simulation of open many-body quantum systems is challenging, requiring methods to both handle exponentially large Hilbert spaces and represent the influence of (infinite) particle and energy reservoirs. These two requirements are at odds with each other: Larger collections of modes can increase the fidelity of the reservoir representation but come at a substantial computational cost when included in numerical many-body techniques. An increasingly utilized and natural approach to control the growth of the reservoir is to cast a finite set of reservoir modes themselves as an open quantum system. There are, though, many routes to do so. Here, we introduce an accumulative reservoir construction -- an ARC -- that employs a series of partial refreshes of the extended reservoirs. Through this series, the representation accumulates the character of an infinite reservoir. This provides a unified framework for both continuous (Lindblad) relaxation and a recently introduced periodically refresh approach (i.e., discrete resets of the reservoir modes to equilibrium). In the context of quantum transport, we show that the phase space for physical behavior separates into discrete and continuous relaxation regimes with the boundary between them set by natural, physical timescales. Both of these regimes "turnover" into regions of over- and under-damped coherence in a way reminiscent of Kramers' crossover. We examine how the range of behavior impacts errors and the computational cost, including within tensor networks. These results provide the first comparison of distinct extended reservoir approaches, showing that they have different scaling of error versus cost (with a bridging ARC regime decaying fastest). Exploiting the enhanced scaling, though, will be challenging, as it comes with a substantial increase in (operator space) entanglement entropy., Comment: 27 pages, 18 figures

Our everyday reality is characterized by objective information$\unicode{x2013}$information that is selected and amplified by the environment that interacts with quantum systems. Many observers can accurately infer that information indirectly by making measurements on fragments of the environment. The correlations between the system, $\mathcal{S}$, and a fragment, $\mathcal{F}$, of the environment, $\mathcal{E}$, is often quantified by the quantum mutual information or the Holevo quantity that bounds the classical information about $\mathcal{S}$ transmittable by a quantum channel $\mathcal{F}$. The latter is a quantum mutual information but of a classical-quantum state where measurement has selected outcomes on $\mathcal{S}$. The measurement generically reflects the influence of the remaining environment, $\mathcal{E}/\mathcal{F}$, but can also reflect hypothetical questions to deduce the structure of $\mathcal{S}\mathcal{F}$ correlations. Recently, Touil et al. examined a different Holevo quantity, one from a quantum-classical state (a quantum $\mathcal{S}$ to a measured $\mathcal{F}$). As shown here, this quantity upper bounds any accessible classical information about $\mathcal{S}$ in $\mathcal{F}$ and can yield a tighter bound than the typical Holevo quantity. When good decoherence is present$\unicode{x2013}$when the remaining environment, $\mathcal{E}/\mathcal{F}$, has effectively measured the pointer states of $\mathcal{S}$$\unicode{x2013}$this accessibility bound is the accessible information. For the specific model of Touil et al., the accessible information is related to the error probability for optimal detection and, thus, has the same behavior as the quantum Chernoff bound. The latter reflects amplification and provides a universal approach, as well as a single-shot framework, to quantify records of the missing, classical information about $\mathcal{S}$., Comment: 8 pages, 1 figure

Quantum transport simulations often use explicit, yet finite, electronic reservoirs. These should converge to the correct continuum limit, albeit with a trade-off between discretization and computational cost. Here, we study this interplay for extended reservoir simulations, where relaxation maintains a bias or temperature drop across the system. Our analysis begins in the non-interacting limit, where we parameterize different discretizations to compare them on an even footing. For many-body systems, we develop a method to estimate the relaxation that best approximates the continuum by controlling virtual transitions in Kramers' turnover for the current. While some discretizations are more efficient for calculating currents, there is little benefit with regard to the overall state of the system. Any gains become marginal for many-body, tensor network simulations, where the relative performance of discretizations varies when sweeping other numerical controls. These results indicate that a given reservoir discretization may have little impact on numerical efficiency for certain computational tools. The choice of a relaxation parameter, however, is crucial, and the method we develop provides a reliable estimate of the optimal relaxation for finite reservoirs., Comment: Manuscript + SI

Quantum transport simulations are rapidly evolving and now encompass well-controlled tensor network techniques for many-body limits. One powerful approach combines matrix product states with extended reservoirs. In this method, continuous reservoirs are represented by explicit, discretized counterparts and a chemical potential or temperature drop is maintained by external relaxation. Currents are strongly influenced by relaxation when it is very weak or strong, resulting in a simulation analog of Kramers' turnover for solution-phase chemical reactions. At intermediate relaxation, the intrinsic conductance, that given by the Landauer or Meir-Wingreen expressions, moderates the current. We demonstrate that strong impurity scattering (i.e., a small steady-state current) reveals anomalous transport regimes within this methodology at weak-to-moderate and moderate-to-strong relaxation. The former is due to virtual transitions and the latter to unphysical broadening of the populated density of states. Thus, the turnover analog has $five$ standard transport regimes, further constraining the parameters that lead to recovery of the intrinsic conductance. In the worst case, the common strategy of choosing a relaxation strength proportional to the reservoir level spacing can prevent convergence to the continuum limit. This advocates a simulation strategy where one utilizes the current versus relaxation turnover profiles to identify simulation parameters that most efficiently reproduce the intrinsic physical behavior., Comment: 16 pages, 5 figures

Ionic transport in nano- to sub-nano-scale pores is highly dependent on translocation barriers and potential wells. These features in the free-energy landscape are primarily the result of ion dehydration and electrostatic interactions. For pores in atomically thin membranes, such as graphene, other factors come into play. Ion dynamics both inside and outside the geometric volume of the pore can be critical in determining the transport properties of the channel due to several commensurate length scales, such as the effective membrane thickness, radii of the first and the second hydration layers, pore radius, and Debye length. In particular, for biomimetic pores, such as the graphene crown ether we examine here, there are regimes where transport is highly sensitive to the pore size due to the interplay of dehydration and interaction with pore charge. Picometer changes in the size, e.g., due to a minute strain, can lead to a large change in conductance. Outside of these regimes, the small pore size itself gives a large resistance, even when electrostatic factors and dehydration compensate each other to give a relatively flat -- e.g., near barrierless -- free energy landscape. The permeability, though, can still be large and ions will translocate rapidly after they arrive within the capture radius of the pore. This, in turn, leads to diffusion and drift effects dominating the conductance. The current thus plateaus and becomes effectively independent of pore-free energy characteristics. Measurement of this effect will give an estimate of the magnitude of kinetically limiting features, and experimentally constrain the local electromechanical conditions.

Open system simulations of quantum transport provide a platform for the study of true steady states, Floquet states, and the role of temperature, time-dynamics, and fluctuations, among other physical processes. They are rapidly gaining traction, especially techniques that revolve around "extended reservoirs" - a collection of a finite number of degrees of freedom with relaxation that maintain a bias or temperature gradient - and have appeared under various guises (e.g., the extended or mesoscopic reservoir, auxiliary master equation, and driven Liouville-von Neumann approaches). Yet, there are still a number of open questions regarding the behavior and convergence of these techniques. Here, we derive general analytical solutions, and associated asymptotic analyses, for the steady-state current driven by finite reservoirs with proportional coupling to the system/junction. In doing so, we present a simplified and unified derivation of the non-interacting and many-body steady-state currents through arbitrary junctions, including outside of proportional coupling. We conjecture that the analytic solution for proportional coupling is the most general of its form for isomodal relaxation (i.e., relaxing proportional coupling will remove the ability to find compact, general analytical expressions for finite reservoirs). These results should be of broad utility in diagnosing the behavior and implementation of extended reservoir and related approaches, including the convergence to the Landauer limit (for non-interacting systems) and the Meir-Wingreen formula (for many-body systems)., Comment: 14 pages

In a recent article, Chiang and Hsu [The Journal of Chemical Physics 153, 044103 (2020)] examine one and two site electronic junctions identically connected to finite reservoirs. For these two examples, they derive analytical solutions, as well as provide asymptotic analyses, for the steady-state current from the driven Liouville-von Neumann (DLvN) equation - an open system approach to transport in non-interacting systems where relaxation maintains a bias. The two site junction they examine has destructive interference, which they show leads to slow convergence of the DLvN to the Landauer limit with respect to reservoir size and relaxation. We previously derived the general solution for the steady-state current in both the DLvN and its many-body analog [Gruss et al., Scientific Reports 6, 24514 (2016)]. The many-body analog is a Lindblad master equation, which, when restricted to non-interacting systems, is exactly the DLvN. Here, we demonstrate that applying the more general expression to identical left and right reservoirs (i.e., finite reservoirs with the same density of states and coupling to the system) and Markovian relaxation provides a simple analytic form that applies to arbitrary, but identically connected, junctions. Moreover, we briefly discuss the convergence of the current to the Landauer and Meir-Wingreen result for non-interacting and interacting systems, respectively. Convergence occurs as the reservoirs' lesser Green's functions begin conforming to the fluctuation-dissipation theorem. Our approach sheds light on the behavior Chiang and Hsu observe for destructive interference. Finally, we show that the analytical results yield the asymptotic formulas derived in Gruss et al., Comment: 4 pages

Tensor networks are a powerful tool for many-body ground states with limited entanglement. These methods can nonetheless fail for certain time-dependent processes - such as quantum transport or quenches - where entanglement growth is linear in time. Matrix-product-state decompositions of the resulting out-of-equilibrium states require a bond dimension that grows exponentially, imposing a hard limit on simulation timescales. However, in the case of transport, if the reservoir modes of a closed system are arranged according to their scattering structure, the entanglement growth can be made logarithmic. Here, we apply this ansatz to open systems via extended reservoirs that have explicit relaxation. This enables transport calculations that can access steady states, time dynamics and noise, and periodic driving (e.g., Floquet states). We demonstrate the approach by calculating the transport characteristics of an open, interacting system. These results open a path to scalable and numerically systematic many-body transport calculations with tensor networks., Comment: 7 pages, 4 figures

The adsorption of metal atoms on nanostructures, such as graphene and nanotubes, plays an important role in catalysis, electronic doping, and tuning material properties. Quantum chemical calculations permit the investigation of this process to discover desirable interactions and obtain mechanistic insights into adsorbate behavior, of which the binding strength is a central quantity. However, binding strengths vary widely in the literature, even when using almost identical computational methods. To address this issue, we investigate the adsorption of a variety of metals onto graphene, carbon nanotubes, and boron nitride nanotubes. As is well-known, calculations on periodic structures require a sufficiently large system size to remove interactions between periodic images. Our results indicate that there are both direct and indirect mechanisms for this interaction, where the latter can require even larger system sizes than typically employed. The magnitude and distance of the effect depend on the electronic state of the substrate and the open- or closed-shell nature of the adsorbate. For instance, insulating substrates (e.g., boron nitride nanotubes) show essentially no dependence on system size, whereas metallic or semi-metallic systems can have a substantial effect due to the delocalized nature of the electronic states interacting with the adsorbate. We derive a scaling relation for the length dependence with a representative tight-binding model. These results demonstrate how to extrapolate the binding energies to the isolated-impurity limit.

We investigate protocols for optimal molecular detection with electromechanical nanoscale sensors in ambient conditions. Our models are representative of suspended graphene nanoribbons, which due to their piezoelectric and electronic properties, provide responsive and versatile sensors. In particular, we analytically account for the corrections in the electronic transmission function and signal-to-noise ratio originating in environmental perturbations, such as thermal fluctuations and solvation effects. We also investigate the role of the sampling time in the current statistics. As a result, we formulate a protocol for optimal sensing based on the modulation of the Fermi level at fixed bias, and provide approximate forms for the current, linear susceptibility, and current fluctuations. We show how the algebraic tails in the thermally broadened transmission function affect the behavior of the signal-to-noise ratio and optimal sensing. These results provide further insights into the operation of graphene deflectometers and other techniques for electromechanical sensing.

Biological ion channels balance electrostatic and dehydration effects to yield large ion selectivities alongside high transport rates. These macromolecular systems are often interrogated through point mutations of their pore domain, limiting the scope of mechanistic studies. In contrast, we demonstrate that graphene crown ether pores afford a simple platform to directly investigate optimal ion transport conditions, i.e., maximum current densities and selectivity. Crown ethers are known for selective ion adsorption. When embedded in graphene, however, transport rates lie below the drift-diffusion limit. We show that small pore strains -- 1 % -- give rise to a colossal -- 100 % -- change in conductance. This process is electromechanically tunable, with optimal transport in a primarily diffusive regime, tending toward barrierless transport, as opposed to a knock-on mechanism. Measurements of mechanical current modulation will yield direct information on the local electrostatic conditions of the pore. These observations suggest a novel setup for nanofluidic devices while giving insight into the physical foundation of evolutionarily--optimized ion transport in biological pores.

The recognition that large classes of quantum many-body systems have limited entanglement in the ground and low-lying excited states led to dramatic advances in their numerical simulation via so-called tensor networks. However, global dynamics elevates many particles into excited states, and can lead to macroscopic entanglement and the failure of tensor networks. Here, we show that for quantum transport -- one of the most important cases of this failure -- the fundamental issue is the canonical basis in which the scenario is cast: When particles flow through an interface, they scatter, generating a "bit" of entanglement between spatial regions with each event. The frequency basis naturally captures that -- in the long-time limit and in the absence of inelastic scattering -- particles tend to flow from a state with one frequency to a state of identical frequency. Recognizing this natural structure yields a striking -- potentially exponential in some cases -- increase in simulation efficiency, greatly extending the attainable spatial- and time-scales, and broadening the scope of tensor network simulation to hitherto inaccessible classes of non-equilibrium many-body problems., Comment: Published version; 6+9 pages; 4+4 figures; Added: an example of interacting reservoirs, further evidence on performance scaling, and extended discussion of the numerical details

While ubiquitous, energy redistribution remains a poorly understood facet of the nonequilibrium thermodynamics of biomolecules. At the molecular level, finite-size effects, pronounced nonlinearities, and ballistic processes produce behavior that diverges from the macroscale. Here, we show that transient thermal transport reflects macromolecular energy landscape architecture through the topological characteristics of molecular contacts and the nonlinear processes that mediate dynamics. While the former determines transport pathways via pairwise interactions, the latter reflects frustration within the landscape for local conformational rearrangements. Unlike transport through small-molecule systems, such as alkanes, nonlinearity dominates over coherent processes at even quite short time- and length-scales. Our exhaustive all-atom simulations and novel local-in-time and space analysis, applicable to both theory and experiment, permit dissection of energy migration in biomolecules. The approach demonstrates that vibrational energy transport can probe otherwise inaccessible aspects of macromolecular dynamics and interactions that underly biological function., Comment: Final published version + supplementary info

Graphene and other 2D materials give a platform for electromechanical sensing of biomolecules in aqueous, room temperature environments. The electronic current changes in response to mechanical deflection, indicating the presence of forces due to interactions with, e.g., molecular species. We develop illustrative models of these sensors in order to give explicit, compact expressions for the current and signal-to-noise ratio. Electromechanical structures have an electron transmission function that follows a generalized Voigt profile, with thermal fluctuations giving a Gaussian smearing analogous to thermal Doppler broadening in solution/gas-phase spectroscopic applications. The Lorentzian component of the profile comes from the contact to the electrodes. After providing an accurate approximate form of this profile, we calculate the mechanical susceptibility for a representative two-level bridge and the current fluctuations for electromechanical detection. These results give the underlying mechanics of electromechanical sensing in more complex scenarios, such as graphene deflectometry.

The origin of classical reality in our quantum world is a long-standing mystery. Here, we examine a nitrogen vacancy center evolving naturally in the presence of its environment to study quantum Darwinism - the proliferation of information about preferred quantum states throughout the world via the environment. This redundantly imprinted information accounts for the perception of objective reality, as it is independently accessible by many without perturbing the system of interest. To observe the emergence of redundant information, we implement a novel dynamical decoupling scheme that enables the measurement/control of several nuclear spins (the environment E) interacting with a nitrogen vacancy (the system S). In addition to showing how to create entangled SE states relevant to quantum metrology, we demonstrate that under the decoherence of S, redundant information is imprinted onto E, giving rise to classical objectivity - a consensus of the nuclear spins about the state of S. This provides the first laboratory verification of the objective classical world emerging from the underlying quantum substrate., Comment: accepted for publication in Physical Review Letters

Simulations are increasingly employing explicit reservoirs - internal, finite regions - to drive electronic or particle transport. This naturally occurs in simulations of transport via ultracold atomic gases. Whether the simulation is numerical or physical, these approaches rely on the rapid development of the steady state. We demonstrate that steady state formation is a manifestation of the Gibbs phenomenon well-known in signal processing and in truncated discrete Fourier expansions. Each particle separately develops into an individual steady state due to the spreading of its wave packet in energy. The rise to the steady state for an individual particle depends on the particle energy - and thus can be slow - and ringing oscillations appear due to filtering of the response through the electronic bandwidth. However, the rise to the total steady state - the one from all particles - is rapid, with timescale $\pi/W$, where $W$ is the bandwidth. Ringing oscillations are now also filtered through the bias window, and they decay with a higher power. The Gibbs constant - the overshoot of the first ring - can appear in the simulation error. These results shed light on the formation of the steady state and support the practical use of explicit reservoirs to simulate transport at the nanoscale or using ultracold atomic lattices., Comment: 6 pages, 4 figures

Ion transport through nanopores permeates through many areas of science and technology, from cell behavior to sensing and separation to catalysis and batteries. Two-dimensional materials, such as graphene, molybdenum disulfide (MoS$_2$), and hexagonal boron nitride (hBN), are recent additions to these fields. Low-dimensional materials present new opportunities to develop filtration, sensing, and power technologies, encompassing ion exclusion membranes, DNA sequencing, single molecule detection, osmotic power generation, and beyond. Moreover, the physics of ionic transport through pores and constrictions within these materials is a distinct realm of competing many-particle interactions (e.g., solvation/dehydration, electrostatic blockade, hydrogen bond dynamics) and confinement. This opens up alternative routes to creating biomimetic pores and may even give analogues of quantum phenomena, such as quantized conductance, in the classical domain. These prospects make membranes of 2D materials -- i.e., 2D membranes -- fascinating. We will discuss the physics and applications of ionic transport through nanopores in 2D membranes.opores in 2D membranes., Comment: New title, one new figure, some discussions removed, new discussions added, updated supplementary material

The interconversion between left- and right-handed helical folds of a polypeptide defines a dual-funneled free energy landscape. In this context, the funnel minima are connected through a continuum of unfolded conformations, evocative of the classical helix-coil transition. Physical intuition and recent conjectures suggest that this landscape can be mapped by assigning a left- or right-handed helical state to each residue. We explore this possibility using all-atom replica exchange molecular dynamics and an Ising-like model, demonstrating that the energy landscape architecture is at odds with a two-state picture. A three-state model - left, right, and unstructured - can account for most key intermediates during chiral interconversion. Competing folds and excited conformational states still impose limitations on the scope of this approach. However, the improvement is stark: Moving from a two-state to a three-state model decreases the fit error from 1.6 $k_B T$ to 0.3 $k_B T$ along the left-to-right interconversion pathway., Comment: Manuscript + SI

Single-molecule sensing is at the core of modern biophysics and nanoscale science, from revolutionizing healthcare through rapid, low-cost sequencing to understanding various physical, chemical, and biological processes at their most basic level. However, important processes at the molecular scale are often too fast for the detection bandwidth or otherwise outside the detection sensitivity. Moreover, most envisioned biophysical applications are at room temperature, which further limits detection due to significant thermal noise. Here, we theoretically demonstrate reliable transduction of forces into electronic currents via locally suspended graphene nanoribbons subject to ultra-low flexural deflection. The decay of electronic couplings with distance magnifies the effect of the deflection, giving rise to measurable electronic current changes even in aqueous solution. Due to thermal fluctuations, the characteristic charge carrier transmission peak follows a generalized Voigt profile, behavior which is reflected in the optimized sensor. The intrinsic sensitivity is less than 7 fN/$\sqrt{\mathbf{Hz}}$, allowing for the detection of ultra-weak and fast processes at room temperature. Graphene deflectometry thus presents new opportunities in the sensing and detection of molecular-scale processes, from ion dynamics to DNA sequencing and protein folding, in their native environment.

Access resistance indicates how well current carriers from a bulk medium can converge to a pore or opening, and is an important concept in nanofluidic devices and in cell physiology. In simplified scenarios, when the bulk dimensions are infinite in all directions, it depends only on the resistivity and pore radius. These conditions are not valid in all-atom molecular dynamics (MD) simulations of transport, due to the computational cost of large simulation cells, and can even break down in micro- and nano-scale systems due to strong confinement. Here, we examine a scaling theory for the access resistance that predicts a special simulation cell aspect ratio -- the golden aspect ratio -- where finite size effects are eliminated. Using both continuum and all-atom simulations, we demonstrate that this golden aspect ratio exists and that it takes on a universal value in linear response and moderate concentrations. Outside of linear response, it gains an apparent dependence on characteristics of the transport scenario (concentration, voltages, etc.) for small simulation cells, but this dependence vanishes at larger length scales. These results will enable the use of all-atom molecular dynamics simulations to study contextual properties of access resistance -- its dependence on protein and molecular-scale fluctuations, the presence of charges, and other functional groups -- and yield the opportunity to quantitatively compare computed and measured resistances., Comment: a)A new expanded title, b) Previous Fig 1 and Fig 2 are merged into a new Fig 1, c) Improved figure legends

The resistance due to the convergence from bulk to a constriction, for example, a nanopore, is a mainstay of transport phenomena. In classical electrical conduction, Maxwell, and later Hall for ionic conduction, predicted this access or convergence resistance to be independent of the bulk dimensions and inversely dependent on the pore radius, $a$, for a perfectly circular pore. More generally, though, this resistance is contextual, it depends on the presence of functional groups/charges and fluctuations, as well as the (effective) constriction geometry/dimensions. Addressing the context generically requires all-atom simulations, but this demands enormous resources due to the algebraically decaying nature of convergence. We develop a finite-size scaling analysis, reminiscent of the treatment of critical phenomena, that makes the convergence resistance accessible in such simulations. This analysis suggests that there is a "golden aspect ratio" for the simulation cell that yields the infinite system result with a finite system. We employ this approach to resolve the experimental and theoretical discrepancies in the radius-dependence of graphene nanopore resistance., Comment: Minor grammatical fixes, simplification of equations, new Methods section, additional citations

The lack of an engaging pedagogy and the highly competitive atmosphere in introductory science courses tend to discourage students from pursuing science, technology, engineering, and mathematics (STEM) majors. Once in a STEM field, academic and social integration has been long thought to be important for students' persistence. Yet, it is rarely investigated. In particular, the relative impact of in-class and out-of-class interactions remains an open issue. Here, we demonstrate that, surprisingly, for students whose grades fall in the "middle of the pack," the out-of-class network is the most significant predictor of persistence. To do so, we use logistic regression combined with Akaike's information criterion to assess in- and out-of-class networks, grades, and other factors. For students with grades at the very top (and bottom), final grade, unsurprisingly, is the best predictor of persistence---these students are likely already committed (or simply restricted from continuing) so they persist (or drop out). For intermediate grades, though, only out-of-class closeness---a measure of one's immersion in the network---helps predict persistence. This does not negate the need for in-class ties. However, it suggests that, in this cohort, only students that get past the convenient in-class interactions and start forming strong bonds outside of class are or become committed to their studies. Since many students are lost through attrition, our results suggest practical routes for increasing students' persistence in STEM majors., Comment: 12 pages, 2 figures, 8 tables, 6 pages of Supplementary Materials

Topological effects typically discussed in the context of quantum physics are emerging as one of the central paradigms of physics. Here, we demonstrate the role of topology in energy transport through dimerized micro- and nano-mechanical lattices in the classical regime, i.e., essentially "masses and springs". We show that the thermal conductance factorizes into topological and non-topological components. The former takes on three discrete values and arises due to the appearance of edge modes that prevent good contact between the heat reservoirs and the bulk, giving a length-independent reduction of the conductance. In essence, energy input at the boundary mostly stays there, an effect robust against disorder and nonlinearity. These results bridge two seemingly disconnected disciplines of physics, namely topology and thermal transport, and suggest ways to engineer thermal contacts, opening a direction to explore the ramifications of topological properties on nanoscale technology., Comment: 6 pages, 3 figures; Supplemental information included as an ancillary file

Open-system approaches are gaining traction in the simulation of charge transport in nanoscale and molecular electronic devices. In particular, "extended reservoir" simulations, where explicit reservoir degrees of freedom are present, allow for the computation of both real-time and steady-state properties but require relaxation of the extended reservoirs. The strength of this relaxation, $\gamma$, influences the conductance, giving rise to a "turnover" behavior analogous to Kramers' turnover in chemical reaction rates. We derive explicit, general expressions for the weak and strong relaxation limits. For weak relaxation, the conductance increases linearly with $\gamma$ and every electronic state of the total explicit system contributes to the electronic current according to its "reduced" weight in the two extended reservoir regions. Essentially, this represents two conductors in series -- one at each interface with the implicit reservoirs that provide the relaxation. For strong relaxation, a "dual" expression -- one with the same functional form -- results, except now proportional to $1/\gamma$ and dependent on the system of interest's electronic states, reflecting that the strong relaxation is localizing electrons in the extended reservoirs. Higher order behavior (e.g., $\gamma^2$ or $1/\gamma^2$) can occur when there is a gap in the frequency spectrum. Moreover, inhomogeneity in the frequency spacing can give rise to a pseudo-plateau regime. These findings yield a physically motivated approach to diagnosing numerical simulations and understanding the influence of relaxation, and we examine their occurrence in both simple models and a realistic, fluctuating graphene nanoribbon., Comment: 6 pages, 3 figures

During the catalytic synthesis of graphene, nanotubes, fibers, and other nanostructures, many intriguing phenomena occur, such as phase separation, precipitation, and analogs of capillary action. We demonstrate that catalytic nanoparticles display metastable states that influence growth, reminiscent of some protein ensembles in vivo. As a carbon nanostructure grows, the nanoparticle elongates due to an energetically favorable metal-carbon interaction that overrides the surface energy increase of the metal. The formation of subsequent nested tubes, however, drives up the particle's free energy, but the particle remains trapped until an accessible free energy surface allows it to exit the tube. During this time, the nanoparticle continues to catalyze tube growth internally within the nested structure. This nonequilibrium thermodynamic cycle of elongation and retraction is heavily influenced by tapering of the structure, which, ultimately, determines the final product and catalyst lifetime. Our results provide a unifying framework to interpret similar phenomena for other catalytic reactions, such as during CO oxidation, and suggest routes to the practical optimization of such processes., Comment: 5 pages, 4 figures; Supplemental Information 16 pages, 8 figures

Selective ion transport is a hallmark of biological ion channel behavior but is a major challenge to engineer into artificial membranes. Here, we demonstrate, with all-atom molecular dynamics simulations, that bare graphene nanopores yield measurable ion selectivity that varies over one to two orders of magnitude simply by changing the pore radius and number of graphene layers. Monolayer graphene does not display dehydration-induced selectivity until the pore radius is small enough to exclude the first hydration layer from inside the pore. Bi- and tri-layer graphene, though, display such selectivity already for a pore size that barely encroaches on the first hydration layer, which is due to the more significant water loss from the second hydration layer. Measurement of selectivity and activation barriers from both first and second hydration layer barriers will help elucidate the behavior of biological ion channels. Moreover, the energy barriers responsible for selectivity -- while small on the scale of hydration energies -- are already relatively large, i.e., many $k_B$. For separation of ions from water, therefore, one can exchange longer, larger radius pores for shorter, smaller radius pores, giving a practical method for maintaining exclusion efficiency while enhancing other properties (e.g., water throughput)., Comment: Minor fixes, updated references

Master equations are increasingly popular for the simulation of time-dependent electronic transport in nanoscale devices. Several recent Markovian approaches use "extended reservoirs" - explicit degrees of freedom associated with the electrodes - distinguishing them from many previous classes of master equations. Starting from a Lindblad equation, we develop a common foundation for these approaches. Due to the incorporation of explicit electrode states, these methods do not require a large bias or even "true Markovianity" of the reservoirs. Nonetheless, their predictions are only physically relevant when the Markovian relaxation is weaker than the thermal broadening and when the extended reservoirs are "sufficiently large," in a sense that we quantify. These considerations hold despite complete positivity and respect for Pauli exclusion at any relaxation strength., Comment: Accepted version. To appear in The Journal of Chemical Physics

The objective, classical world emerges from the underlying quantum substrate via the proliferation of redundant copies of selected information into the environment, which acts as a communication channel, transmitting that information to observers. These copies are independently accessible, allowing many observers to reach consensus about the state of a quantum system via its imprints in the environment. Quantum Darwinism recognizes that the redundancy of information is thus central to the emergence of objective reality in the quantum world. However, in addition to the "quantum system of interest," there are many other systems "of no interest" in the Universe that can imprint information on the common environment. There is therefore a danger that the information of interest will be diluted with irrelevant bits, suppressing the redundancy responsible for objectivity. We show that mixing of the relevant (the "wheat") and irrelevant (the "chaff") bits of information makes little quantitative difference to the redundancy of the information of interest. Thus, we demonstrate that it does not matter whether one separates the relevant information) from the (irrelevant) chaff: The large redundancy of the relevant information survives dilution, providing evidence of the objective, effectively classical world., Comment: 5 pages, 0 figures

Photoelectron emission microscopy PEEM is a powerful tool to spectroscopically image dynamic surface processes at the nanoscale but is traditionally limited to ultra high or moderate vacuum conditions. Here, we develop a novel grapheme capped multichannel array sample platform that extends the capabilities of photoelectron spectromicroscopy to routine liquid and atmospheric pressure studies with standard PEEM setups. Using this platform, we show that graphene has only a minor influence on the electronic structure of water in the first few layers and thus will allow for the examination of minimally perturbed aqueous phase interfacial dynamics. Analogous to microarray screening technology in biomedical research, our platform is highly suitable for applications in tandem with large-scale data mining, pattern recognition, and combinatorial methods for spectro temporal and spatiotemporal analyses at solid liquid interfaces. Using Bayesian linear unmixing algorithm, we were able to discriminate between different X-ray induced water radiolysis scenarios and observe a metastable wetting intermediate water layer during the late stages of bubble formationformation, Comment: 20 pages, 4 figures

We propose a method to probe the local density of states (LDOS) of atomic systems that provides both spatial and energy resolution. The method combines atomic and tunneling techniques to supply a simple, yet quantitative and operational, definition of the LDOS for both interacting and non-interacting systems: It is the rate at which particles can be siphoned from the system of interest by a narrow energy band of non-interacting states contacted locally to the many-body system of interest. Ultracold atoms in optical lattices are a natural platform for implementing this broad concept to visualize the energy and spatial dependence of the atom density in interacting, inhomogeneous lattices. This includes models of strongly correlated condensed matter systems, as well as ones with non-trivial topologies., Comment: 9 pages, 7 figures; Appeared in the Focus on Quantum Transport in Ultracold Atoms in the New Journal of Physics

The double slit experiment provides a classic example of both interference and the effect of observation in quantum physics. When particles are sent individually through a pair of slits, a wave-like interference pattern develops, but no such interference is found when one observes which "path" the particles take. We present a model of interference, dephasing, and measurement-induced decoherence in a one-dimensional version of the double-slit experiment. Using this model, we demonstrate how the loss of interference in the system is correlated with the information gain by the measuring apparatus/observer. In doing so, we give a modern account of measurement in this paradigmatic example of quantum physics that is accessible to students taking quantum mechanics at the graduate or senior undergraduate levels., Comment: 11 pages, 5 figures

Ion channels play a key role in regulating cell behavior and in electrical signaling. In these settings, polar and charged functional groups -- as well as protein response -- compensate for dehydration in an ion-dependent way, giving rise to the ion selective transport critical to the operation of cells. Dehydration, though, yields ion-dependent free-energy barriers and thus is predicted to give rise to selectivity by itself. However, these barriers are typically so large that they will suppress the ion currents to undetectable levels. Here, we establish that graphene displays a measurable dehydration-only mechanism for selectivity of $\mathrm{K}^+$ over $\mathrm{Cl}^-$. This fundamental mechanism -- one that depends only on the geometry and hydration -- is the starting point for selectivity for all channels and pores. Moreover, while we study selectivity of $\mathrm{K}^+$ over $\mathrm{Cl}^-$, we find that dehydration-based selectivity functions for all ions, i.e., cation over cation selectivity (e.g., $\mathrm{K}^+$ over $\mathrm{Na}^+$). Its likely detection in graphene pores resolves conflicting experimental results, as well as presents a new paradigm for characterizing the operation of ion channels and engineering molecular/ionic selectivity in filtration and other applications., Comment: 27 pages

Landauer's formula is the standard theoretical tool to examine ballistic transport in nano- and meso-scale junctions, but it necessitates that any variation of the junction with time must be slow compared to characteristic times of the system, e.g., the relaxation time of local excitations. Transport through structurally dynamic junctions is, however, increasingly of interest for sensing, harnessing fluctuations, and real-time control. Here, we calculate the steady-state current when relaxation of electrons in the reservoirs is present and demonstrate that it gives rise to three regimes of behavior: weak relaxation gives a contact-limited current; strong relaxation localizes electrons, distorting their natural dynamics and reducing the current; and in an intermediate regime the Landauer view of the system only is recovered. We also demonstrate that a simple equation of motion emerges, which is suitable for efficiently simulating time-dependent transport., Comment: 16 pages, 5 figures

Quantum Darwinism recognizes the role of the environment as a communication channel: Decoherence can selectively amplify information about the pointer states of a system of interest (preventing access to complementary information about their superpositions) and can make records of this information accessible to many observers. This redundancy explains the emergence of objective, classical reality in our quantum Universe. Here, we demonstrate that the amplification of information in realistic spin environments can be quantified by the quantum Chernoff information, which characterizes the distinguishability of partial records in individual environment subsystems. We show that, except for a set of initial states of measure zero, the environment always acquires redundant information. Moreover, the Chernoff information captures the rich behavior of amplification in both finite and infinite spin environments, from quadratic growth of the redundancy to oscillatory behavior. These results will considerably simplify experimental testing of quantum Darwinism, e.g., using nitrogen vacancies in diamond., Comment: 10 pages, 5 figures

We compare the Landauer, Kubo, and microcanonical [J. Phys. Cond. Matter {\bf 16}, 8025 (2004)] approaches to quantum transport for the average current, the entanglement entropy and the semiclassical full-counting statistics (FCS). Our focus is on the applicability of these approaches to isolated quantum systems such as ultra-cold atoms in engineered optical potentials. For two lattices connected by a junction, we find that the current and particle number fluctuations from the microcanonical approach compare well with the values predicted by the Landauer formalism and FCS assuming a binomial distribution. However, we demonstrate that well-defined reservoirs (i.e., particles in Fermi-Dirac distributions) are not present for a substantial duration of the quasi-steady state. Thus, the Landauer assumption of reservoirs and/or inelastic effects is not necessary for establishing a quasi-steady state. Maintaining such a state indefinitely requires an infinite system, and in this limit well-defined Fermi-Dirac distributions can occur. A Kubo approach -- in the spirit of the microcanonical picture -- bridges the gap between the two formalisms, giving explicit analytical expressions for the formation of the steady state. The microcanonical formalism is designed for closed, finite-size quantum systems and is thus more suitable for studying particle dynamics in ultra-cold atoms. Our results highlight both the connection and differences with more traditional approaches to calculating transport properties in condensed matter systems, and will help guide the way to their simulations in cold-atom systems., Comment: 16 pages, 15 figures

Kramers' theory frames chemical reaction rates in solution as reactants overcoming a barrier in the presence of friction and noise. For weak coupling to the solution, the reaction rate is limited by the rate at which the solution can restore equilibrium after a subset of reactants have surmounted the barrier to become products. For strong coupling, there are always sufficiently energetic reactants. However, the solution returns many of the intermediate states back to the reactants before the product fully forms. Here, we demonstrate that the thermal conductance displays an analogous physical response to the friction and noise that drive the heat current through a material or structure. A crossover behavior emerges where the thermal reservoirs dominate the conductance at the extremes and only in the intermediate region are the intrinsic properties of the lattice manifest. Not only does this shed new light on Kramers' classic turnover problem, this result is significant for the design of devices for thermal management and other applications, as well as the proper simulation of transport at the nanoscale., Comment: 8 pages, 5 figures. Supplementary Information available at the journal publication or by request from the authors

Amplification was regarded, since the early days of quantum theory, as a mysterious ingredient that endows quantum microstates with macroscopic consequences, key to the "collapse of the wavepacket", and a way to avoid embarrassing problems exemplified by Schr\"odinger's cat. Such a bridge between the quantum microworld and the classical world of our experience was postulated ad hoc in the Copenhagen Interpretation. Quantum Darwinism views amplification as replication, in many copies, of the information about quantum states. We show that such amplification is a natural consequence of a broad class of models of decoherence, including the photon environment we use to obtain most of our information. This leads to objective reality via the presence of robust and widely accessible records of selected quantum states. The resulting redundancy (the number of copies deposited in the environment) follows from the Quantum Chernoff Information that quantifies the information transmitted by a typical elementary subsystem of the environment., Comment: 5 pages, 1 figure

Motivated by the advances of quantum Darwinism and recognizing the role played by redundancy in identifying the small subset of quantum states with resilience characteristic of objective classical reality, we explore the implications of redundant records for consistent histories. The consistent histories formalism is a tool for describing sequences of events taking place in an evolving closed quantum system. A set of histories is consistent when one can reason about them using Boolean logic, i.e., when probabilities of sequences of events that define histories are additive. However, the vast majority of the sets of histories that are merely consistent are flagrantly non-classical in other respects. This embarras de richesses (known as the set selection problem) suggests that one must go beyond consistency to identify how the classical past arises in our quantum Universe. The key intuition we follow is that the records of events that define the familiar objective past are inscribed in many distinct systems, e.g., subsystems of the environment, and are accessible locally in space and time to observers. We identify histories that are not just consistent but redundantly consistent using the partial-trace condition introduced by Finkelstein as a bridge between histories and decoherence. The existence of redundant records is a sufficient condition for redundant consistency. It selects, from the multitude of the alternative sets of consistent histories, a small subset endowed with redundant records characteristic of the objective classical past. The information about an objective history of the past is then simultaneously within reach of many, who can independently reconstruct it and arrive at compatible conclusions in the present., Comment: Further elaboration on the mathematical definition of a record was added. Final published version. 18 pages

The sum of the Holevo quantity (that bounds the capacity of quantum channels to transmit classical information about an observable) and the quantum discord (a measure of the quantumness of correlations of that observable) yields an observable-independent total given by the quantum mutual information. This split naturally delineates information about quantum systems accessible to observers -- information that is redundantly transmitted by the environment -- while showing that it is maximized for the quasi-classical pointer observable. Other observables are accessible only via correlations with the pointer observable. Further, we prove an anti-symmetry property relating accessible information and discord. It shows that information becomes objective -- accessible to many observers -- only as quantum information is relegated to correlations with the global environment, and, therefore, locally inaccessible. The resulting complementarity explains why, in a quantum Universe, we perceive objective classical reality while flagrantly quantum superpositions are out of reach., Comment: 12 pages, 4 figures

Novel approaches to DNA sequencing and detection require the measurement of electrical currents between metal probes immersed in ionic solution. Here, we experimentally demonstrate that these systems maintain large background currents with a transient response that decays very slowly in time and noise that increases with ionic concentration. Using a non-equilibrium stochastic model, we obtain an analytical expression for the ionic current that shows these results are due to a fast electrochemical reaction at the electrode surface followed by the slow formation of a diffusion layer. During the latter, ions translocate in the weak electric field generated after the initial rapid screening of the strong fields near the electrode surfaces. Our theoretical results are in very good agreement with experimental findings.

DNA has a well-defined structural transition -- the denaturation of its double-stranded form into two single strands -- that strongly affects its thermal transport properties. We show that, according to a widely implemented model for DNA denaturation, one can engineer DNA "heattronic" devices that have a rapidly increasing thermal conductance over a narrow temperature range across the denaturation transition (~350 K). The origin of this rapid increase of conductance, or "switching", is the softening of the lattice and suppression of nonlinear effects as the temperature crosses the transition temperature and DNA denatures. Most importantly, we demonstrate that DNA nanojunctions have a broad range of thermal tunability due to varying the sequence and length, and exploiting the underlying nonlinear behavior. We discuss the role of disorder in the base sequence, as well as the relation to genomic DNA. These results set the basis for developing thermal devices out of materials with nonlinear structural dynamics, as well as understanding the underlying mechanisms of DNA denaturation., Comment: 11+5 pages, 4 figures + 1 table

A state selected at random from the Hilbert space of a many-body system is overwhelmingly likely to exhibit highly non-classical correlations. For these typical states, half of the environment must be measured by an observer to determine the state of a given subsystem. The objectivity of classical reality-the fact that multiple observers can agree on the state of a subsystem after measuring just a small fraction of its environment-implies that the correlations found in nature between macroscopic systems and their environments are very exceptional. Building on previous studies of quantum Darwinism showing that highly redundant branching states are produced ubiquitously during pure decoherence, we examine conditions needed for the creation of branching states and study their demise through many-body interactions. We show that even constrained dynamics can suppress redundancy to the values typical of random states on relaxation timescales, and prove that these results hold exactly in the thermodynamic limit., Comment: 20 pages, 5 figures. Typos fixed

The study of time-dependent, many-body transport phenomena is increasingly within reach of ultra-cold atom experiments. We show that the introduction of spatially inhomogeneous interactions, e.g., generated by optically-controlled collisions, induce negative differential conductance in the transport of atoms in 1D optical lattices. Specifically, we simulate the dynamics of interacting fermionic atoms via a micro-canonical transport formalism within both mean-field and a higher-order approximation, as well as with time-dependent DMRG. For weakly repulsive interactions, a quasi steady-state atomic current develops that is similar to the situation occurring for electronic systems subject to an external voltage bias. At the mean-field level, we find that this atomic current is robust against the details of how the interaction is switched on. Further, a conducting-to-nonconducting transition exists when the interaction imbalance exceeds some threshold from both our approximate and time-dependent DMRG simulations. This transition is preceded by the atomic equivalent of negative differential conductivity observed in transport across solid-state structures., Comment: 10 pages, 8 figures