We report theoretical investigations on the role of interfacial bonding mechanism and its resulting structures to quantum transport in molecular wires. Two bonding mechanisms for the Au-S bond in an Au(111)/1,4-benzenedithiol(BDT)/Au(111) junction were identified by ab initio calculation, confirmed by a recent experiment, which, we showed, critically control charge conduction. It was found, for Au/ BDT/Au junctions, the hydrogen atom, bound by a dative bond to the Sulfur, is energetically non-dissociative after the interface formation. The calculated conductance and junction breakdown forces of H-non-dissociative Au/BDT/Au devices are consistent with the experimental values, while the H-dissociated devices, with the interface governed by typical covalent bonding, give conductance more than an order of magnitude larger. By examining the scattering states that traverse the junctions, we have revealed that mechanical and electric properties of a junction have strong correlation with the bonding configuration. This work clearly demonstrates that the interfacial details, rather than previously believed many-body effects, is of vital importance for correctly predicting equilibrium conductance of molecular junctions; and manifests that the interfacial contact must be carefully understood for investigating quantum transport properties of molecular nanoelectronics.
We have measured the effect of bonding of a CO molecule on the conductance of Au, Cu, Pt, and Ni atomic contacts at 4.2 K. When CO gas is admitted to the metal nano contacts, a conductance feature appears in the conductance histogram near 0.5 of the quantum unit of conductance, for all metals. For Au, the intensity of this fractional conductance feature can be tuned with the bias voltage, and it disappears at high bias voltage (above $\sim$ 200 mV). The bonding of CO to Au appears to be weakest, and associated with monotomic Au wire formation.
Spin-density-functional calculations of tip-suspended gold chains, with molecular oxygen, or dissociated oxygen atoms, incorporated in them, reveal structural transitions for varying lengths. The nanowires exhibit enhanced strength for both oxygen incorporation modes, and upon stretching tip atoms join the wire. With incorporated molecular oxygen the wire conductance is about 1(2e2/h), transforming to an insulating state beyond a critical length. The nanowire conductance with embedded oxygen atoms is low, 0.2 (2e2/h), and it develops magnetic moments localized on the oxygens and the neighborin…
We point out that the effective channel for the interfacial thermal conductance, the inverse of Kapitza resistance, of metal-insulator/semiconductor interfaces is governed by the electron-phonon interaction mediated by the surface states allowed in a thin region near the interface. Our detailed calculations demonstrate that the interfacial thermal conductance across Pb/Pt/Al/Au-diamond interfaces are only slightly different among these metals, and reproduce well the experimental results of the interfacial thermal conductance across metal-diamond interfaces observed by Stoner et al. [Phys. Rev.…
Thermal conductance across bonded SiOx-SiOx interfaces in hybrid bonding process
School of Integrated Circuits and Beijing Advanced Innovation Center for Integrated Circuits, Peking University（北京大学集成电路学院与北京集成电路先进创新中心）；School of Integrated Circuits, Southeast University（东南大学集成电路学院）
We report experimental and computational studies of thermal transport properties in hexagonal boron nitride (hBN) encapsulated molybdenum disulfide (MoS2) structure using refined optothermal Raman techniques, and reveal very high interfacial thermal conductance between hBN and MoS2. By studying the Raman shift of hBN and MoS2 in suspended and substrate-supported thin films under varying laser power and temperature, we calibrate lateral (in-plane) thermal conductivity of hBN and MoS2 and the vertical interfacial thermal conductance in the hBN/MoS2/hBN heterostructure as well as the interfaces b…
In this article, we report the influence of the interfacial roughness on the thermal boundary conductance between two crystals, using molecular dynamics. We show evidence of a transition between two regimes, depending on the interfacial roughness: when the roughness is small, the boundary conductance is constant taking values close to the conductance of the corresponding planar interface. When the roughness is larger, the conductance becomes larger than the planar interface conductance, and the relative increase is found to be close to the increase of the interfacial area. The cross-plane cond…
Exploring the mechanism of interfacial thermal transport and reducing the interfacial thermal resistance is of great importance for thermal management and modulation. Herein, the interfacial thermal resistance between overlapped graphene nanoribbons is largely reduced by adding bonded carbon chains by performing molecular dynamics simulations. And the analytical model (cross-interface model, CIM) is utilized to analyze and explain the two-dimensional thermal transport mechanism at cross-interface. An order of magnitude reduction in interfacial thermal resistance is found as the graphene nanori…
Atomic-sized junctions of iron, created by controlled rupture, present unusually high values of conductance compared to other metals. This result is counter-intuitive since, at the nanoscale, body-centered cubic metals are expected to exhibit lower coordination than face-centered cubic metals. In this work, classical molecular dynamics simulations of contact rupture, using an interatomic potential that accounts for directional bonding, yield highly-coordinated stable structures before rupture, unlike an isotropic bonding potential, which results in the expected stable single-atom contacts. Den…
Due to its low intrinsic damping, Y$_3$Fe$_5$O$_{12}$ and its substituted variations are often used for ferromagnetic layer at spin pumping experiment. Spin pumping is an interfacial spin current generation in the interface of ferromagnet and non-magnetic metal, governed by spin mixing conductance parameter $G^{\uparrow\downarrow}$. $G^{\uparrow\downarrow}$ has been shown to enhance the damping of the ferromagnetic layer. The theory suggested that the effect of $G^{\uparrow\downarrow}$ on gyromagnetic ratio only come from its negligible imaginary part. In this article, we show that the differe…
Electron transport through a diatomic molecular tunnel junction shows wave like interference phenomenon. By using Keldysh non-equilibrium Green's function (NEGF) theory, we have explicitly presented current and differential conductance calculation for a diatomic molecular and two isolated atoms (two atoms having zero hybridization between their energy orbital) tunnel junctions. In case of a diatomic molecular tunnel junction, Green's function propagators entering into current and differential conductance formula interfere constructively for a molecular anti-bonding state and destructively for …
Accurate estimation of interfacial thermal conductance between silicon and diamond enabled by a machine learning interatomic potential
Imam Khomeini International University（伊玛目霍梅尼国际大学）；Institut Lumière Matière, Université Claude Bernard Lyon 1-CNRS, Université de Lyon（光物质研究所，里昂第一大学-CNRS，里昂大学）；Chair of Computational Science and Simulation Technology, Institute of Photonics, Department of Mathematics and Physics, Leibniz Universität Hannover（莱布尼茨汉诺威大学计算科学与仿真技术教席、光子学研究所、数学与物理系）；School of Energy Science and Engineering, Harbin Institute of Technology（哈尔滨工业大学能源学院）
The graphene morphology regulated by nanowires patterned in parallel on a substrate surface is quantitatively determined using energy minimization. The regulated graphene morphology is shown to be governed by the nanowire diameter, the nanowire spacing and the interfacial bonding energies between the graphene and the underlying nanowires and substrate. We demonstrate two representative regulated graphene morphologies and determine critical values of the nanowire spacing, nanowire diameter and interfacial bonding energies at which graphene switches between the two representative morphologies. I…
The defect induced interfacial states are created in an atomically thin two-dimensional molybdenum disulfide channel by underlying a narrow pattern of a graphene layer in a field effect transistor. Nondestructive method for the generation of charge-state allowed a highly sensitive molecular interaction with the sensitivity of nearly three-order of magnitude at room temperature. The presence of interfacial states in the channel lead to a conductance fluctuation and its magnitude is modulated using the nitrogen dioxide gas molecules in the subthreshold region. The study provides a systematic app…
We study the nonlinear interfacial thermal transport across atomic junctions by the quantum self-consistent mean field (QSCMF) theory based on nonequilibrium Green's function approach; the QSCMF theory we propose is very precise and matches well with the exact results from quantum master equations. The nonlinearity at the interface is studied by effective temperature dependent interfacial coupling calculated from the QSCMF theory. We find that nonlinearity can provide an extra channel for phonon transport in addition to the phonon scattering which usually blocks heat transfer. For weak linearl…
We proposed a new way, adding intertube atoms, to enhance interfacial thermal conductance (ITC) between SiC-carbon nanotube (CNT) array structure. Non-equilibrium molecular dynamics method was used to study the ITC. The results show that the intertube atoms can significantly enhance the ITC. The dependence of ITC on both the temperature and the number of intertube atoms are shown. The mechanism is analyzed by calculating probability distributions of atomic forces and vibrational density of states. Our study may provide some guidance on enhancing the ITC of CNT-based composites.
We discuss the conductance of a molecular bridge between mesoscopic electrodes supporting low-dimensional transport and bearing an internal structure. As an example for such nanoelectrodes we assume semi-infinite (carbon) nanotubes. In the Landauer scattering matrix approach, we show that the conductance of this hybrid is very sensitive to the geometry of the contact unlike the usual behaviour in the presence of bulk electrodes.
Molecular dynamics simulations of thiolate-protected and solvated gold nanoparticles were carried out in the presence of a non-equilibrium heat flux between the solvent and the core of the particle. The interfacial thermal conductance ($G$) was computed for these interfaces, and the behavior of the thermal conductance was studied as a function of particle size, ligand flexibility, and ligand chain length. In all cases, thermal conductance of the ligand-protected particles was higher than the bare metal-solvent interface. A number of mechanisms for the enhanced conductance were investigated, in…
We theoretically explore the influence of end-group chemistry (bond stiffness and mass) on the interfacial thermal conductance at a gold-alkane interface. We accomplish this using the Non-Equilibrium Green's Function (NEGF) coupled with first principle parameters in Density Functional Theory (DFT) within the harmonic approximation. Our results indicate that the interfacial thermal conductance is not a monotonic function of either chemical parameters, but instead maximizes at an optimal set of mass and bonding strength. This maximum is a result of the interplay between the overlap in local dens…
We study the thermal conductance across solid-solid interfaces as the composition of an intermediate matching layer is varied. In absence of phonon-phonon interactions, an added layer can make the interfacial conductance increase or decrease depending on the interplay between (1) an increase in phonon transmission due to better bridging between the contacts, and (2) a decrease in the number of available conduction channels that must conserve their momenta transverse to the interface. When phonon-phonon interactions are included, the added layer is seen to aid conductance when the decrease in r…
We present experimental measurements of the thermal boundary conductance (TBC) from $77 - 500$ K across isolated heteroepitaxially grown ZnO films on GaN substrates. These data provide an assessment of the assumptions that drive the phonon gas model-based diffuse mismatch models (DMM) and atomistic Green's function (AGF) formalisms for predicting TBC. Our measurements, when compared to previous experimental data, suggest that the TBC can be influenced by long wavelength, zone center modes in a material on one side of the interface as opposed to the "vibrational mismatch" concept assumed in the…
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 …
Molecular materials enable a vast variety of functionalities for novel electronic and spintronic devices. The unique possibility to alter or substitute organic molecules or metallic substrates offers the opportunity to modify and optimize interfacial properties for almost any desired field of application. For this reason, we extend the successful approach to control molecular interfaces by surface alloying. We present a comprehensive characterization of the structural and electronic properties of the interface formed between the prototypical molecule PTCDA and a Sn-Ag surface alloy grown on an…
Thermal boundary conductance at a metal-dieletric interface is a quantity of prime importance for heat management at the nanoscale. While the boundary conductance is usually ascribed to the coupling between metal phonons and dielectric phonons, in this work we examine the influence of a direct coupling between the metal electrons and the dielectric phonons. The effect of electron- phonon processes is generally believed to be resistive, and tends to decrease the overall thermal boundary conductance as compared to the phonon-phonon conductance σp . Here, we find that the effect of a direct coupl…
We present results of electronic structure calculations for well-relaxed Au/benzene-1,4-dithiol/Au molecular contacts, based on density functional theory and the generalized gradient approximation. Electronic states in the vicinity of the Fermi energy are mainly of Au 5d and S 3p symmetry, whereas contributions of C 2p states are very small. Hybridization between C 2p orbitals within the benzene substructure is strongly suppressed due to S-C bonding. In agreement with experimental findings, this corresponds to a significantly reduced conductance of the molecular contact.
Recent studies showed that the in-plane and inter-plane thermal conductivities of two-dimensional (2D) MoS2 are low, posing a significant challenge in heat management in MoS2-based electronic devices. To address this challenge, we design the interfaces between MoS2 and graphene by fully utilizing graphene, a 2D material with an ultra-high thermal conduction. We first perform ab initio atomistic simulations to understand the bonding nature and structure stability of the interfaces. Our results show that the designed interfaces, which are found to be connected together by strong covalent bonds b…
In this article, we compare the results of non-equilibrium (NEMD) and equilibrium (EMD) molecular dynamics methods to compute the thermal conductance at the interface between solids. We propose to probe the thermal conductance using equilibrium simulations measuring the decay of the thermally induced energy fluctuations of each solid. We also show that NEMD and EMD give generally speaking inconsistent results for the thermal conductance: Green Kubo simulations probe the Landauer conductance between two solids which assumes phonons on both sides of the interface to be at equilibrium. On the oth…
A unified understanding of interfacial thermal transport is missing due to the complicated nature of interfaces which involves complex factors such as interfacial bonding, interfacial mixing, surface chemistry, crystal orientation, roughness, contamination, and interfacial disorder. This is especially true for metal nonmetal interfaces which incorporate multiple fundamental heat transport mechanisms such as elastic and inelastic phonon scattering as well as electron phonon coupling in the metal and across the interface. All these factors jointly affect thermal boundary conductance (TBC). As a …
Detailed understanding of vibrational heat transfer mechanisms between solids is essential for the efficient thermal engineering and control of nanomaterials. We investigate the frequency dependence of anharmonic scattering and interfacial thermal conduction between two acoustically mismatched solids in planar contact by calculating the spectral decomposition of the heat current flowing through an interface between two materials. The calculations are based on analyzing the correlations of atomic vibrations using the data extracted from non-equilibrium molecular dynamics simulations. Inelastic …
Interfaces dominate heat conduction in nanostructured systems, and much work has focused on methods to enhance interfacial conduction. These approaches generally address planar interfaces, where the heat flux vector is everywhere normal to the interface. Here, we explore a nanostructured interface geometry that uses nonplanar features to enhance the effective interfacial conductance beyond what is possible with planar interfaces. This interface consists of interdigitating Al pillars embedded within SiO2 with characteristic feature size ranging from 100 nm to 800 nm. The total sidewall surface …
We argue that the relative thermal conductance between interfaces with different morphologies is controlled by crystal structure through $M_{min}/M_c > 1$, the ratio between the {\it minimum mode} count on either side $M_{min}$, and the {\it conserving modes} $M_c$ that preserve phonon momentum transverse to the interface. Junctions with an added homogenous layer, "uniform", and "abrupt" junctions are limited to $M_c$ while junctions with interfacial disorder, "mixed", exploit the expansion of mode spectrum to $M_{min}$. In our studies with cubic crystals, the largest enhancement of conductanc…
We present a theoretical study of the transport characteristics of molecular junctions, where first-row diatomic molecules are attached to (001) gold and platinum electrodes. We find that the conductance of all of these junctions is of the order of the conductance quantum unit $G_0$, spelling out that they belong to the transparent regime. We further find that the transmission coefficients show wide plateaus as a function of the energy, instead of the usual sharp resonances that signal the molecular levels in the tunneling regime. We use Caroli's model to show that this is a rather generic pro…
We present a mechanism to improve the conductivity of carbon nanotube (CNT) networks by improving the conductance between CNTs of different chirality. We argue generally that a weak perturbation can greatly improve the inter-tube conductance by allowing momentum-conserving tunnelling. The mechanism is verified with a tight-binding model, allowing an investigation of its impact for a network containing a range of chiralities. We discuss practical implementations, and conclude that it may be effected by weak physical interactions, and therefore does not require chemical bonding to the CNTs.
Non-equilibrium molecular dynamics (NEMD) simulations were performed on Au-SAM (self-assembly monolayer)-Au junctions to study the thermal energy transport across the junctions. Thermal conductance of the Au-SAM interfaces was calculated. Temperature effects, simulated external pressure effects, SAM molecule coverage effects and Au-SAM bond strength effects on the interfacial thermal conductance were studied. It was found that the interfacial thermal conductance increased with temperature increase at temperatures lower than 250K, but it did not have large changes at temperatures from 250K to 4…
Low-loss cavities are important in building high-coherence superconducting quantum computers. Generating high quality joints between parts is crucial to the realization of a scalable quantum computer using the circuit quantum electrodynamics (cQED) framework. In this paper, we adapt the technique of indium bump bonding to the cQED architecture to realize high quality superconducting microwave joints between chips. We use this technique to fabricate compact superconducting cavities in the multilayer microwave integrated quantum circuits (MMIQC) architecture and achieve single photon quality fac…
Spin-dependent transport at heavy metal/magnetic insulator interfaces is at the origin of many phenomena at the forefront of spintronics research. A proper quantification of the different interfacial spin conductances is crucial for many applications. Here, we report the first measurement of the spin Hall magnetoresistance (SMR) of Pt on a purely ferromagnetic insulator (EuS). We perform SMR measurements in a wide range of temperatures and fit the results by using a microscopic model. From this fitting procedure we obtain the temperature dependence of the spin conductances ($G_s$, $G_r$ and $G…
We present a comprehensive study of the properties of the off-resonant conductance spectrum in oligomer nanojunctions between graphitic electrodes. By employing first-principle-based methods and the Landauer approach of quantum transport, we identify how the electronic structure of the molecular junction components is reflected in electron transport across such systems. For virtually all energies within the conduction gap of the corresponding idealised polymer chain, we show that: a) the inverse decay length of the tunnelling conductance is intrinsically defined by the complex-band structure o…
We present first principles calculations for the conductance of a hydrogen molecule bridging a pair of Pt electrodes. The transmission function has a wide plateau with T~1 which extends across the Fermi level and indicates the existence of a single, robust conductance channel with nearly perfect transmission. Through a detailed Wannier function analysis we show that the H2 bonding state is not involved in the transport and that the plateau forms due to strong hybridization between the H2 anti-bonding state and states on the adjacent Pt atoms. The Wannier functions furthermore allow us to deriv…
We investigate resonant tunneling through molecular states of coupled double quantum dots embedded in an Aharonov-Bohm (AB) interferometer. The conductance through the system consists of two resonances associated with the bonding and the antibonding quantum states. We predict that the two resonances are composed of a Breit-Wigner resonance and a Fano resonance, those widths and Fano factor depending on the AB phase very sensitively. Further, we point out that the bonding properties, such as the covalent and the ionic bonding, can be identified by the AB oscillations.
We study electrical and thermoelectrical properties for a double quantum dot system. We consider the cases of both single-level and multilevel quantum dots whatever the way they are coupled, either in a series or in a parallel arrangement. The calculations are performed by using the nonequilibrium Green function theory. In the case of a single-level double quantum dot, the problem is exactly solvable whereas for a multilevel double quantum dot, an analytical solution is obtained in the limit of energy-independent hopping integrals. { We present a detailed discussion about} the dependences of e…
We propose phonon spectroscopy by electric measurements of the low-temperature conductance of coupled-quantum dots, specifically employing dephasing of the quantum electronic transport by the phonons. The setup we consider consists of a T-shaped double-quantum-dot (DQD) system in which only one of the dots (dot 1) is connected to external leads and the other (dot 2) is coupled solely to the first one. For noninteracting electrons, the differential conductance of such a system vanishes at a voltage located in-between the energies of the bonding and the anti-bonding states, due to destructive in…
Thermopower measurements of molecular junctions have recently gained interest as a characterization technique that supplements the more traditional conductance measurements. Here we investigate the electronic conductance and thermopower of benzenediamine (BDA) and benzenedicarbonitrile (BDCN) connected to gold electrodes using first-principles calculations. We find excellent agreement with experiments for both molecules when exchange-correlation effects are described by the many-body GW approximation. In contrast, results from standard density functional theory (DFT) deviate from experiments b…
We study the conductance and current noise of a superconductor/ferromagnet (S/F) single channel Quantum Point Contact (QPC) as a function of the QPC bias voltage, using a scattering approach. We show that the Spin-Dependence of Interfacial Phase Shifts (SDIPS) acquired by electrons upon scattering by the QPC can strongly modify these signals. For a weakly transparent contact, the SDIPS induces sub-gap resonances in the conductance and differential Fano factor curves of the QPC. For high transparencies, these resonances are smoothed, but the shape of the signals remain extremely sensitive to th…
