Vibrational nonequilibrium effects in charge transport through single-molecule junctions are investigated. Focusing on molecular bridges with multiple electronic states, it is shown that electronic-vibrational coupling triggers a variety of vibronic emission and absorption processes, which influence the conductance properties and mechanical stability of single-molecule junctions profoundly. Employing a master equation and a nonequilibrium Green's function approach, these processes are analyzed in detail for a generic model of a molecular junction and for benzenedibutanethiolate bound to gold electrodes.
Within the hierarchical quantum master equation (HQME) framework, an approach is presented, which allows a numerically exact description of nonequilibrium charge transport in nanosystems with strong electronic-vibrational coupling. The method is applied to a generic model of vibrationally coupled transport considering a broad spectrum of parameters ranging from the nonadiabatic to the adiabatic regime and including both resonant and off-resonant transport. We show that nonequilibrium effects are important in all these regimes. In particular in the off-resonant transport regime, the inelastic c…
We present a novel hierarchical quantum master equation (HQME) approach which provides a numerically exact description of nonequilibrium charge transport in nanosystems with electronic-vibrational coupling. In contrast to previous work [Phys. Rev. B $\bf{94}$, 201407 (2016)], the active vibrational degrees of freedom are treated in the reservoir subspace and are integrated out. This facilitates applications to systems with very high excitation levels, for example due to current-induced heating, while properties of the vibrational degrees of freedom, such as the excitation level and other momen…
Nonequilibrium electron-vibration coupling and conductance fluctuations in a C60-junction
采用基于密度泛函理论和非平衡格林函数（DFT-NEGF）的第一性原理计算，研究了有限偏压下分子C60结中化学键的形成和电导.在接触形成的点，我们确定了一个非常强的耦合之间的C60运动和分子的电子结构。这仅在正样品偏压下可见，尽管电导本身不是强极性依赖性的。的非平衡效应追溯到一个突然的位移的电压降的位置与一个小的C60位移。结合振动加热机制，我们构建了一个模型，从我们的结果解释了最近的扫描隧道显微镜（STM）实验中观察到的极性相关的两能级电导波动[N. Néel等人，Nano Lett. 11，3593（2011）]。这些发现突出了非平衡效应在化学键形成/断裂和分子电子学中的电子振动耦合中的重要性。
We investigate the 1/f noise properties of epitaxial graphene devices at low temperatures as a function of temperature, current and magnetic flux density. At low currents, an exponential decay of the 1/f noise power spectral density with increasing temperature is observed that indicates mesoscopic conductance fluctuations as the origin of 1/f noise at temperatures below 50 K. At higher currents, deviations from the typical quadratic current dependence and the exponential temperature dependence occur as a result of nonequilibrium conditions due to current heating. By applying the theory of Kuba…
Thermal boundary conductance (TBC) is critical in many thermal and energy applications. A decades-old puzzle has been that many of the measured TBCs, such as those well characterized across Al/Si and ZnO/GaN interfaces, significantly exceed theoretical results or even the absolute upper limit called the ``radiation limit", suggesting the failure of the theory. Here, we identify that for high-transmission interfaces, the commonly assumed phonon local thermal equilibrium adjacent to the interface fails, and the measurable phonon temperatures are not their emission temperature. We hence develop a…
We calculate the nonequilibrium local density of states on a vibrational quantum dot coupled to two electrodes at T=0 using a numerically exact diagrammatic Monte Carlo method. Our focus is on the interplay between the electron-phonon interaction strength and the bias voltage. We find that the spectral density exhibits a significant voltage dependence if the voltage window includes one or more phonon sidebands. A comparison with well-established approximate approaches indicates that this effect could be attributed to the nonequilibrium distribution of the phonons. Moreover, we discuss the long…
We investigate the nonequilibrium quantum heat transfer in a triangle-coupled spin-boson system within a three-terminal setup. By including the nonequilibrium noninteracting blip approximation approach combined with the full counting statistics, we analytically obtain the steady state populations and heat currents. The negative differential thermal conductance and giant heat amplification factor are clearly observed at strong qubit-bath coupling. %and the heat amplification is dramatically suppressed in the moderate coupling regime. Moreover, the strong interaction between the gating qubit and…
The spin mixing conductance (SMC) is a key quantity determining efficiency of spin transport across interfaces. Thus, knowledge of its precise value is required for accurate measurement of parameters quantifying numerous effects in spintronics, such as spin-orbit torque, spin Hall magnetoresistance, spin Hall effect and spin pumping. However, the standard expression for SMC, provided by the scattering theory in terms of the reflection probability amplitudes, is inapplicable when strong spin-orbit coupling (SOC) is present directly at the interface. This is the precisely the case of topological…
We find the nonlinear conductance of a dissipative resonant level in the nonequilibrium steady state near its quantum critical point. The system consists of a spin-polarized quantum dot connected to two resistive leads that provide ohmic dissipation. We focus on the crossover from the strong-coupling, non-Fermi-liquid regime to the weak-coupling, Fermi-liquid ground state, a crossover driven by the instability of the quantum critical point to hybridization asymmetry or detuning of the level in the dot. We show that the crossover properties are given by tunneling through an effective single bar…
Time-dependent perturbations can drive a trivial two-dimensional band insulator into a quantum Hall-like phase, with protected nonequilibrium states bound to its edges. We propose an experiment to probe the existence of these topological edge states which consists of passing a tunneling current through a small two-dimensional sample out of equilibrium. The signature is a nonquantized metallic conductance near the edges of the sample and, in contrast, an excitation gap in the bulk. This proposal is demonstrated for the case of a two-dimensional lattice model of Dirac electrons with tunable mass…
The interaction between electronic and vibrational degrees of freedom in single-molecule junctions may result from the dependence of the electronic energies or the electronic states of the molecular bridge on the nuclear displacement. The latter mechanism leads to a direct coupling between different electronic states and is referred to as nonadiabatic electronic-vibrational coupling. Employing a perturbative nonequilibrium Green's function approach, we study the influence of nonadiabatic electronic-vibrational coupling in model molecular junctions. Thereby we distinguish between systems with w…
Self-assembled molecular structures have been intensively used in molecular electronics and spintronics. However, detailed nature of the interfaces between molecular layers and extended metallic contacts used to bias the real devices remains unclear. Buried interfaces greatly restrict application of standard techniques such as Raman or scanning electron microscopies. Here we introduce low frequency noise spectroscopy as a tool to characterize buried molecular-metal interfaces. We take advantage of vibrational heating of the molecules with incomplete contacts to the interface. Electrons, being …
Universal fractionalization of quantum transport characteristics in Majorana quantum dot devices is expected to emerge for well separated Majorana bound states. We show that the Majorana universality of the differential shot noise $\partial S^>/\partial V$ and conductance $\partial I/\partial V$ at low bias voltages $V$ arises only in ideal setups with only one Majorana mode entangled with the quantum dot. In realistic devices, where both Majorana modes are entangled with the quantum dot, $\partial S^>/\partial V$ and $\partial I/\partial V$ become very sensitive to tunneling phases and their …
We consider an open molecular junction in which electrons are coupled to multi-mode phonons. Using a master equation approach for equilibrated phonons, we show that nearly-degenerate phonon modes can be mapped into an effective single mode, which can result in a noticeable reduction of computational costs. As an illustration, we apply our theory to the OPV-5 molecule and show that we can obtain the consistent conductance spectra while reducing the computational time by orders of magnitude
We investigate the effects of alternating voltage on nonequilibrium quantum systems with localised phonon modes. Nonequilibrium Green's functions are utilised, with electron-phonon coupling being considered with the $GD$ approximation (self-consistent Born approximation). Using a Floquet approach, we assume periodicity of the dynamics. This approach allows us to investigate the influence of the driven electronic component on the nonequilibrium occupation of the vibrations. It was found that signatures of inelastic transport gained photon-assisted peaks. A simplistic model was proposed and foun…
In this work we analyze the nonequilibrium transport through a quantum impurity (quantum dot or molecule) attached to ferromagnetic leads by using a hybrid numerical renormalization group-time-dependent density matrix renormalization group thermofield quench approach.For this, we study the bias dependence of the differential conductance through the system, which shows a finite zero-bias peak, characteristic of the Kondo resonance and reminiscent of the equilibrium local density of states. In the non-equilibrium settings, the resonance in the differential conductance is also found to decrease w…
We extend a perturbative, nonequilibrium renormalization group approach to multi-orbital systems and apply it for studying transport through two parallel quantum dots coupled electrostatically. In general, the conductance shows pronounced Kondoesque peaks at three voltages. One of these peaks disappears if, as in some experiments, one of the dots is decoupled from one of the two leads. For an asymmetric coupling to the leads, also negative differential conductances are possible. This is a genuine nonequilibrium effect, accompanying the Kondoesque peaks. Moreover, a criterion to distinguish spi…
Inelastic effects in molecular junctions in the Coulomb and Kondo regimes: Nonequilibrium equation-of-motion approach
在一个简单的非平衡运动方程（EOM）的方法被认为是在库仑阻塞和近藤制度的电子输运通过分子结的非弹性效应。该方案是自洽的，并且可以定性地再现库仑阻塞中振动特征的主要实验观察[H.Park et al.，Nature 407，57（2000）]和Kondo [L. H. Yu等人，物理修订信函93，266802（2004）]制度。考虑类似于Meir等人的平衡EOM方法[Phys. Rev. Lett. 66，3048（1991）;同上，70，2601（1993）]用于Keldysh等值线以说明结的非平衡性质，并且通过适当的Franck-Condon（FC）因子进行修整以说明振动特征。Meir等人的平衡EOM方案的结果在适当的限度内重现。
We study vibrational statistics in current-carrying model molecular junctions using master equation approach. Especially, we concentrate on the validity of using an effective temperature $T_{\rm eff}$ to characterize the nonequilibrium steady state of a vibrational mode. We identify cases where a single $T_{\rm eff}$ can not fully describe one vibrational state. In such cases, the probability distribution among different vibrational states does not follow the Boltzmann type. Consequently, the actual entropy (free energy) of the vibrational mode is lower (higher) than the corresponding thermal …
The low conductance of nickel atomic junctions in the hydrogen environment is studied using the nonequilibrium Green's function theory combined with first-principles calculations. The Ni junction bridged by a $H_2$ molecule has a conductance of approximately 0.7 $G_0$. This conductance is contributed by the anti-bonding state of the $H_2$ molecule, which forms a bonding state with the $3d$ orbitals of the nearby Ni atoms. In contrast, the Ni junction bridged by the two single H atoms has a conductance of approximately 1 $G_0$, which is weakly spin-polarized. The spin-up channels were found to …
