Search

Helical molecules have been identified as potential candidates for investigating electronic transport, spin filtering, or even piezoelectricity. However, the description of the transport mechanism is not straightforward in single molecular junctions. In this work, we study the electronic transport in break junctions of a series of three helical molecules: dithia[$n$]helicenes, with $n=7, 9, 11$ molecular units, and detail the synthesis of two kinds of dithia[11]helicenes, varying the location of the sulfur atoms. Our experimental study demonstrates low conductance values that remain similar across different biases and molecules. Additionally, we assess the length dependence of the conductance for each helicene, revealing an exponential decay characteristic of off-resonant transport. This behaviour is primarily attributed to the misalignment between the energy levels of the molecule-electrodes system. The length dependence trend described above is supported by \textit{ab initio} calculations, further confirming the off-resonant transport mechanism.

Van der Waals (vdW) heterostructures composed of two-dimensional (2D) transition metal dichalcogenides (TMD) and vdW magnetic materials offer an intriguing platform to functionalize valley and excitonic properties in non-magnetic TMDs. Here, we report magneto-photoluminescence (PL) investigations of monolayer (ML) MoSe$_2$ on the layered A-type antiferromagnetic (AFM) semiconductor CrSBr under different magnetic field orientations. Our results reveal a clear influence of the CrSBr magnetic order on the optical properties of MoSe$_2$, such as an anomalous linear-polarization dependence, changes of the exciton/trion energies, a magnetic-field dependence of the PL intensities, and a valley $g$-factor with signatures of an asymmetric magnetic proximity interaction. Furthermore, first principles calculations suggest that MoSe$_2$/CrSBr forms a broken-gap (type-III) band alignment, facilitating charge transfer processes. The work establishes that antiferromagnetic-nonmagnetic interfaces can be used to control the valley and excitonic properties of TMDs, relevant for the development of opto-spintronics devices., Comment: 14 pages, 4 figures

Thermocurrent flowing through a single-molecule device contains valuable information about the quantum properties of the molecular structure and, in particular, on its electronic and phononic excitation spectra, and entropy. Furthermore, accessing the thermoelectric heat-to-charge conversion efficiency experimentally can help to select suitable molecules for future energy conversion devices, which - predicted by theoretical studies - could reach unprecedented efficiencies. However, one of the major challenges in quantifying thermocurrents in nanoscale devices is to determine the exact temperature bias applied to the junction. In this work, we have incorporated a superconductor-normal metal-superconductor (SNS) Josephson junction thermometer into a single-molecule device. The critical current of the Josephson junction depends accurately on minute changes of the electronic temperature in a wide temperature range from 100 mK to 1.6 K. Thus, we present a device architecture which can enable thermoelectric experiments on single molecules down to millikelvin temperatures with high precision.

Heat transport by acoustic phonons in 2D materials is fundamentally different from that in 3D crystals because the out-of-plane phonons propagate in a unique way that strongly depends on tension and bending rigidity. Since in-plane and out-of-plane phonon baths are decoupled, initial studies suggested they provide independent pathways for heat transport and storage in 2D materials. Here, we induce tension in freestanding graphene membranes by electrostatic force, and use optomechanical techniques to demonstrate that it can change the rate of heat transport by as much as 33%. Using a ballistic Debye model, we account for these observations and extract the average bending rigidity of the flexural acoustic phonons, which increases approximately linearly with the membrane's areal mass density, in contrast to the cubic dependence seen in bulk structures. Thus, we not only elucidate phononic heat transport mechanisms in suspended 2D materials, but also provide a promising route for controlling nanoscale heat transport by tension., Comment: 34 pages, 10 figures

Magnetic van der Waals materials provide an ideal playground for exploring the fundamentals of low-dimensional magnetism and open new opportunities for ultrathin spin processing devices. The Mermin-Wagner theorem dictates that as in reduced dimensions isotropic spin interactions cannot retain long-range correlations; the order is stabilized by magnetic anisotropy. Here, using ultrashort pulses of light, we demonstrate all-optical control of magnetic anisotropy in the two-dimensional van der Waals antiferromagnet NiPS$_3$. Tuning the photon energy in resonance with an orbital transition between crystal-field split levels of the nickel ions, we demonstrate the selective activation of a sub-THz two-dimensional magnon mode. The pump polarization control of the magnon amplitude confirms that the activation is governed by the instantaneous magnetic anisotropy axis emergent in response to photoexcitation of orbital states with a lowered symmetry. Our results establish pumping of orbital resonances as a universal route for manipulating magnetic order in low-dimensional (anti)ferromagnets.

We analyse the electrical response of narrow graphene nanogaps in search for transport signatures stemming from spin-polarized edge states. We find that the electrical transport across graphene nanogaps having perfectly defined zigzag edges does not carry any spin-related signature. We also analyse the magnetic and electrical properties of nanogaps whose electrodes have wedges that possibly occur in the currently fabricated nanogaps. These wedges can host spin polarized wedge low-energy states due to the bipartite nature of the graphene lattice. We find that these spin-polarized low-energy modes give rise to low-voltage signatures in the differential conductance and to distinctive features in the stability diagrams. These are caused by fully spin-polarized currents., Comment: This is a preprint version. An updated and corrected version that includes Supplemental Information has been published in Nanoscale

We explore the dynamics of a graphene nanomechanical oscillator coupled to a reference oscillator. Circular graphene drums are forced into self-oscillation, at a frequency fosc, by means of photothermal feedback induced by illuminating the drum with a continuous-wave red laser beam. Synchronization to a reference signal, at a frequency fsync, is achieved by shining a power-modulated blue laser onto the structure. We investigate two regimes of synchronization as a function of both detuning and signal strength for direct (fsync = fosc) and parametric locking (fsync = 2fosc). We detect a regime of phase resonance, where the phase of the oscillator behaves as an underdamped second-order system, with the natural frequency of the phase resonance showing a clear power-law dependence on the locking signal strength. The phase resonance is qualitatively reproduced using a forced van der Pol-Duffing-Mathieu equation., Comment: 11 pages, 4 figures, 25 references

Future multi-functional hybrid devices might combine switchable molecules and 2D material-based devices. Spin-crossover compounds are of particular interest in this context since they exhibit bistability and memory effects at room temperature while responding to numerous external stimuli. Atomically-thin 2D materials such as graphene attract a lot of attention for their fascinating electrical, optical, and mechanical properties, but also for their reliability for room-temperature operations. Here, we demonstrate that thermally-induced spin-state switching of spin-crossover nanoparticle thin films can be monitored through the electrical transport properties of graphene lying underneath the films. Model calculations indicate that the charge carrier scattering mechanism in graphene is sensitive to the spin-state dependence of the relative dielectric constants of the spin-crossover nanoparticles. This graphene sensor approach can be applied to a wide class of (molecular) systems with tunable electronic polarizabilities., Comment: main text: 13 pages, 5 figures ; SI: 14 pages, 12 figures

We review different electron transport methods to probe the magnetic properties, such as the magnetic anisotropy, of an individual Fe4 SMM. The different approaches comprise first and higher order transport through the molecule. Gate spectroscopy, focusing on the charge degeneracy-point, is presented as a robust technique to quantify the longitudinal magnetic anisotropy of the SMM in different redox states. We provide statistics showing the robustness and reproducibility of the different methods. In addition, conductance measurements typically show high-energy excited states well beyond the ground spin multiplet of SMM. Some of these excitations have their origin in excited spin multiplets, others in vibrational modes of the molecule. The interplay between vibrations, charge and spin may yield a new approach for spin control.

We investigate vibron-assisted electron transport in single-molecule transistors containing an individual Fe4 Single-Molecule Magnet. We observe a strong suppression of the tunneling current at low bias in combination with vibron-assisted excitations. The observed features are explained by a strong electron-vibron coupling in the framework of the Franck-Condon model supported by density-functional theory.

Graphene electrodes are promising candidates to improve reproducibility and stability in molecular electronics through new electrode-molecule anchoring strategies. Here we report sequential electron transport in few-layer graphene transistors containing individual curcuminoid-based molecules anchored to the electrodes via pi-pi orbital bonding. We show the coexistence of inelastic co-tunneling excitations with single-electron transport physics owing to an intermediate molecule-electrode coupling; we argue that an intermediate electron-phonon coupling is the origin of these vibrational-assisted excitations. These experimental observations are complemented with density functional theory calculations to model electron transport and the interaction between electrons and vibrational modes of the curcuminoid molecule. We find that the calculated vibrational modes of the molecule are in agreement with the experimentally observed excitations.

We present a method for incorporating image-charge effects into the description of charge transport through molecular devices. A simple model allows us to calculate the adjustment of the transport levels, due to the polarization of the electrodes as charge is added to and removed from the molecule. For this, we use the charge distributions of the molecule between two metal electrodes in several charge states, rather than in gas phase, as obtained from a density-functional theory-based transport code. This enables us to efficiently model level shifts and gap renormalization caused by image-charge effects, which are essential for understanding molecular transport experiments. We apply the method to benzene di-amine molecules and compare our results with the standard approach based on gas phase charges. Finally, we give a detailed account of the application of our approach to porphyrin-derivative devices recently studied experimentally by Perrin et al. [Nat. Nanotechnol. 8, 282 (2013)], which demonstrates the importance of accounting for image-charge effects when modeling transport through molecular junctions.

Single-layer MoS2 is a direct-gap semiconductor whose electronic band structure strongly depends on the strain applied to its crystal lattice. While uniaxial strain can be easily applied in a controlled way, e.g., by bending of a flexible substrate with the atomically thin MoS2 layer on top, experimental realization of biaxial strain is more challenging. Here, we exploit the large mismatch between the thermal expansion coefficients of MoS2 and a silicone-based substrate to apply a controllable biaxial tensile strain by heating the substrate with a focused laser. The effect of this biaxial strain is directly observable in optical spectroscopy as a redshift of the MoS2 photoluminescence. We also demonstrate the potential of this method to engineer more complex strain patterns by employing highly absorptive features on the substrate to achieve non-uniform heat profiles. By comparison of the observed redshift to strain-dependent band structure calculations, we estimate the biaxial strain applied by the silicone-based substrate to be up to 0.2 percent, corresponding to a band gap modulation of 105 meV per percentage of biaxial tensile strain.

It is understood that molecular conjugation plays an important role in charge transport through single-molecule junctions. Here, we investigate electron transport through an anthraquinone based single-molecule three-terminal device. With the use of an electric-field induced by a gate electrode, the molecule is reduced resulting into a ten-fold increase in the off-resonant differential conductance. Theoretical calculations link the change in differential conductance to a reduction-induced change in conjugation, thereby lifting destructive interference of transport pathways., Comment: Nano Letters (2015)

We demonstrate that electronic transport through single molecules or molecular ensembles, commonly based on gold (Au) electrodes, can be extended to superconducting electrodes by combining gold with molybdenum-rhenium (MoRe). This combination induces proximity-effect superconductivity in the gold to temperatures of at least 4.6 Kelvin and magnetic fields of 6 Tesla, improving on previously reported aluminum based superconducting nanojunctions. As a proof of concept, we show three-terminal superconductive transport measurements through an individual Fe$_4$ single-molecule magnet., Comment: 4 pages, 3 figures

Nanocrystalline diamond (NCD) is a promising material for electronic and mechanical micro- and nanodevices. Here we introduce a versatile pick-up and drop technique that makes it possible to investigate the electrical, optical and mechanical properties of as-grown NCD films. Using this technique, NCD nanosheets, as thin as 55 nm, can be picked-up from a growth substrate and positioned on another substrate. As a proof of concept, electronic devices and mechanical resonators are fabricated and their properties are characterized. In addition, the versatility of the method is further explored by transferring NCD nanosheets onto an optical fibre, which allows measuring its optical absorption. Finally, we show that NCD nanosheets can also be transferred onto 2D crystals, such as MoS2, to fabricate heterostructures. Pick-up and drop transfer enables the fabrication of a variety of NCD-based devices without requiring lithography or wet processing., Comment: 15 pages, 6 figures

By means of electronic transport, we study the transverse magnetic anisotropy of an individual Fe$_4$ single-molecule magnet (SMM) embedded in a three-terminal junction. In particular, we determine in situ the transverse anisotropy of the molecule from the pronounced intensity modulations of the linear conductance, which are observed as a function of applied magnetic field. The proposed technique works at temperatures exceeding the energy scale of the tunnel splittings of the SMM. We deduce that the transverse anisotropy for a single Fe$_4$ molecule captured in a junction is substantially larger than the bulk value., Comment: 18 pages with 16 figures; version as published

We measure the energy relaxation rate of single- and few-layer molybdenum disulphide ($\mathrm{MoS_2}$) nanomechanical resonators by detecting the resonator ring-down. Recent experiments on these devices show a remarkably low quality (Q)-factor when taking spectrum measurements at room temperature. The origin of the low spectral Q-factor is an open question, and it has been proposed that besides dissipative processes, frequency fluctuations contribute significantly to the resonance line-width. The spectral measurements performed thus far however, do not allow one to distinguish these two processes. Here, we use time-domain measurements to quantify the dissipation. We compare the Q-factor obtained from the ring-down measurements to those obtained from the thermal noise spectrum and from the frequency response of the driven device. In few-layer and single-layer $\mathrm{MoS_2}$ resonators the two are in close agreement, which demonstrates that the spectral line-width in $\mathrm{MoS_2}$ membranes at room temperature is limited by dissipation, and that excess spectral broadening plays a negligible role., Comment: 13 pages, 5 figures

The characteristics of molecular electronic devices are critically determined by metal-organic interfaces, which influence the arrangement of the orbital levels that participate in charge transport. Studies on self-assembled monolayers (SAMs) show (molecule-dependent) level shifts as well as transport-gap renormalization, suggesting that polarization effects in the metal substrate play a key role in the level alignment with respect to the metal's Fermi energy. Here, we provide direct evidence for an electrode-induced gap renormalization in single-molecule junctions. We study charge transport in single porphyrin-type molecules using electrically gateable break junctions. In this set-up, the position of the occupied and unoccupied levels can be followed in situ and with simultaneous mechanical control. When increasing the electrode separation, we observe a substantial increase in the transport gap with level shifts as high as several hundreds of meV for displacements of a few \aa ngstroms. Analysis of this large and tunable gap renormalization with image-charge calculations based on atomic charges obtained from density functional theory confirms and clarifies the dominant role of image-charge effects in single-molecule junctions.

We report fast readout of the motion of a carbon nanotube mechanical resonator. A close-proximity high electron mobility transistor amplifier is used to increase the bandwidth of the measurement of nanotube displacements from the kHz to the MHz regime. Using an electrical detection scheme with the nanotube acting as a mixer, we detect the amplitude of its mechanical motion at room temperature with an intermediate frequency of 6 MHz and a timeconstant of 780 ns, both up to five orders of magnitude faster than achieved before. The transient response of the mechanical motion indicates a ring-down time faster than our enhanced time resolution, placing an upper bound on the contribution of energy relaxation processes to the room temperature mechanical quality factor., Comment: 4 pages, 3 figures

Inspired by cotunneling spectroscopy of spin-states in a single OPE5-based molecule, we investigate the prospects for electric control of magnetism in purely organic molecules contacted in a three-terminal geometry. Using the gate electrode, the molecule is reversibly switched between three different redox states, with magnetic spectra revealing both ferromagnetic and antiferromagnetic exchange couplings on the molecule. These observations are shown to be captured by an effective low-energy Heisenberg model, which we substantiate microscopically by a simple valence bond description of the molecule. These preliminary findings suggest an interesting route towards functionalized all-organic molecular magnetism.

A high-current annealing technique is used to fabricate nanogaps and hybrid diamond/graphite structures in boron-doped nanocrystalline diamond films. Nanometer-sized gaps down to 1 nm are produced using a feedback-controlled current annealing procedure. The nanogaps are characterized using scanning electron microscopy and electronic transport measurements. The structural changes produced by the elevated temperature, achieved by Joule heating during current annealing, are characterized using Raman spectroscopy. The formation of hybridized diamond/graphite structure is observed at the point of maximum heat accumulation., Comment: 14 pages 4 figures + 1 supplemental figure

The quantum behaviour of mechanical resonators is a new and emerging field driven by recent experiments reaching the quantum ground state. The high frequency, small mass, and large quality-factor of carbon nanotube resonators make them attractive for quantum nanomechanical applications. A common element in experiments achieving the resonator ground state is a second quantum system, such as coherent photons or superconducting device, coupled to the resonators motion. For nanotubes, however, this is a challenge due to their small size. Here, we couple a carbon nanoelectromechanical (NEMS) device to a superconducting circuit. Suspended carbon nanotubes act as both superconducting junctions and moving elements in a Superconducting Quantum Interference Device (SQUID). We observe a strong modulation of the flux through the SQUID from displacements of the nanotube. Incorporating this SQUID into superconducting resonators and qubits should enable the detection and manipulation of nanotube mechanical quantum states at the single-phonon level.

The nonlinear interactions between flexural and torsional modes of a microcantilever are experimentally studied. The coupling is demonstrated by measuring the frequency response of one mode, which is sensitive to the motion of another resonance mode. The flexural-flexural, torsional-torsional and flexural-torsional modes are coupled due to nonlinearities, which affect the dynamics at high vibration amplitudes and cause the resonance frequency of one mode to depend on the amplitude of the other modes. We also investigate the nonlinear dynamics of torsional modes, which cause a frequency stiffening of the response. By simultaneously driving another torsional mode in the nonlinear regime, the nonlinear response is tuned from stiffening to weakening. By balancing the positive and negative cubic nonlinearities a linear response is obtained for the strongly driven system. The nonlinear modal interactions play an important role in the dynamics of multi-mode scanning probe microscopes, Comment: 17 pages, 6 figures

We demonstrate strong coupling between the flexural vibration modes of a clamped-clamped micromechanical resonator vibrating at low amplitudes. This coupling enables the direct measurement of the frequency response via amplitude- and phase modulation schemes using the fundamental mode as a mechanical detector. In the linear regime, a frequency shift of $\mathrm{0.8\,Hz}$ is observed for a mode with a line width of $\mathrm{5.8\,Hz}$ in vacuum. The measured response is well-described by the analytical model based on the Euler-Bernoulli beam including tension. Calculations predict an upper limit for the room-temperature Q-factor of $\mathrm{4.5\times10^5}$ for our top-down fabricated micromechanical beam resonators., Comment: 9 pages, 2 figures

The interactions between parametrically and directly driven vibration modes of a clamped-clamped beam resonator are studied. An integrated piezoelectric transducer is used for direct and parametric excitation. First, the parametric amplification and oscillation of a single mode are analyzed by the power and phase dependence below and above the threshold for parametric oscillation. Then, the motion of a parametrically driven mode is detected by the induced change in resonance frequency in another mode of the same resonator. The resonance frequency shift is the result of the nonlinear coupling between the modes by the displacement-induced tension in the beam. These nonlinear modal interactions result in the quadratic relation between the resonance frequency of one mode and the amplitude of another mode. The amplitude of a parametrically oscillating mode depends on the square root of the pump frequency. Combining these dependencies yields a linear relation between the resonance frequency of the directly driven mode and the frequency of the parametrically oscillating mode., Comment: 5 pages, 4 figures

We demonstrate the coupling between the fundamental and second flexural mode of a microcantilever. A mechanical analogue of cavity-optomechanics is then employed, where the mechanical cavity is formed by the second vibrational mode of the same cantilever, coupled to the fundamental mode via the geometric nonlinearity. By exciting the cantilever at the sum and difference frequencies between fundamental and second flexural mode, the motion of the fundamental mode of the cantilever is amplified and damped. This concept makes it possible to enhance or suppress the Q-factor over a wide range., Comment: 9 pages, 3 figures

We have employed a feedback cooling scheme, which combines high-frequency mixing with digital signal processing. The frequency and damping rate of a 2 MHz micromechanical resonator embedded in a dc SQUID are adjusted with the feedback, and active cooling to a temperature of 14.3 mK is demonstrated. This technique can be applied to GHz resonators and allows for flexible control strategies., Comment: To appear in Appl. Phys. Lett

We have measured the backaction of a dc superconducting quantum interference device (SQUID) position detector on an integrated 1 MHz flexural resonator. The frequency and quality factor of the micromechanical resonator can be tuned with bias current and applied magnetic flux. The backaction is caused by the Lorentz force due to the change in circulating current when the resonator displaces. The experimental features are reproduced by numerical calculations using the resistively and capacitively shunted junction (RCSJ) model., Comment: Submitted to Phys. Rev. Lett

A theoretical and experimental investigation is presented on the intermodal coupling between the flexural vibration modes of a single clamped-clamped beam. Nonlinear coupling allows an arbitrary flexural mode to be used as a self-detector for the amplitude of another mode, presenting a method to measure the energy stored in a specific resonance mode. Experimentally observed complex nonlinear dynamics of the coupled modes are quantitatively captured by a model which couples the modes via the beam extension; the same mechanism is responsible for the well-known Duffing nonlinearity in clamped-clamped beams., Comment: 5 pages, 3 figures

By first lithographically fabricating contact electrodes and then as last step growing carbon nanotubes with chemical vapour deposition across the ready-made chip, many potential contamination mechanisms for nanotube devices can be avoided. Combining this with pre-defined trenches on the chip, such that the nanotubes are freely suspended above the substrate, enables the formation of highly regular electronic systems. We show that, in addition, such suspended ultra-clean nanotubes provide excellent high-frequency and low-dissipation mechanical resonators. The motion detection mechanism of our experiment is discussed, and we measure the effect of Coulomb blockade and the back-action of single electron tunneling on the mechanical motion. In addition data on the mechanical higher modes is presented., Comment: 7 pages, 6 figures

We report on the observation of Kondo and split Kondo peaks in single-molecule transistors containing a single spin transition molecule with a Fe2+ ion. Coulomb blockade characteristics reveal a double quantum dot behavior in a parallel configuration, making our system a molecular equivalent to a semiconducting double-quantum-dot system. As the gate voltage is increased the charging of the second dot by an additional electron induces a splitting of the Kondo peak. We discuss possible origins of this effect including a spin transition into a high-spin state.

Nanoscale resonators that oscillate at high frequencies are useful in many measurement applications. We studied a high-quality mechanical resonator made from a suspended carbon nanotube driven into motion by applying a periodic radio frequency potential using a nearby antenna. Single-electron charge fluctuations created periodic modulations of the mechanical resonance frequency. A quality factor exceeding 10^5 allows the detection of a shift in resonance frequency caused by the addition of a single-electron charge on the nanotube. Additional evidence for the strong coupling of mechanical motion and electron tunneling is provided by an energy transfer to the electrons causing mechanical damping and unusual nonlinear behavior. We also discovered that a direct current through the nanotube spontaneously drives the mechanical resonator, exerting a force that is coherent with the high-frequency resonant mechanical motion., Comment: Main text 12 pages, 4 Figures, Supplement 13 pages, 6 Figures

We have observed the transversal vibration mode of suspended carbon nanotubes at millikelvin temperatures by measuring the single-electron tunneling current. The suspended nanotubes are actuated contact-free by the radio frequency electric field of a nearby antenna; the mechanical resonance is detected in the time-averaged current through the nanotube. Sharp, gate-tuneable resonances due to the bending mode of the nanotube are observed, combining resonance frequencies of up to \nu_0 = 350 MHz with quality factors above Q = 10^5, much higher than previously reported results on suspended carbon nanotube resonators. The measured magnitude and temperature dependence of the Q-factor shows a remarkable agreement with the intrinsic damping predicted for a suspended carbon nanotube. By adjusting the RF power on the antenna, we find that the nanotube resonator can easily be driven into the non-linear regime., Comment: 18 pages including supplementary information, fixed minor LaTeX figure reference labelling problem

Low-temperature transport spectroscopy measurements on a suspended few-hole carbon nanotube quantum dot are presented, showing a gate-dependent harmonic excitation spectrum which, strikingly, occurs in the Coulomb blockade regime. The quantized excitation energy corresponds to the scale expected for longitudinal vibrations of the nanotube. The electronic transport processes are identified as cotunnel-assisted sequential tunneling, resulting from non-equilibrium occupation of the mechanical mode. They appear only above a high-bias threshold at the scale of electronic nanotube excitations. We discuss models for the pumping process that explain the enhancement of the non-equilibrium occupation and show that it is connected to a subtle interplay between electronic and vibrational degrees of freedom.

We have fabricated suspended metal paddle resonators with carbon nanotubes functioning as self-detecting torsional springs. We observe gate-tunable resonances, that either tune to higher or to lower frequencies when increasing the dc voltage on the back-gate. We attribute the former modes to flexural vibrations of the paddle resonator, while the latter ones are identified as torsional vibrations. Compared to top-down silicon fabricated paddle resonators, nanotube springs have smaller torsional spring constants and provide a larger frequency tunability., Comment: 7 pages, 3 figures, 1 supplementary information. This article has been accepted by Appl. Phys. Lett. After it is published, it will be found at this http://apl.aip.org/

We have investigated electrical transport through the molecular model systems benzenedithiol, benzenediamine, hexanedithiol and hexanediamine. Conductance histograms under different experimental conditions indicate that measurements using mechanically controllable break junctions in vacuum are limited by the surface density of molecules at the contact. Hexanedithiol histograms typically exhibit a broad peak around 7 * 10^{-4} G_0. In contrast to recent results on STM-based break junctions in solution we find that the spread in single-molecule conductance is not reduced by amino anchoring groups. Histograms of hexanediamine exhibit a very wide peak around 4 * 10^{-4} G_0. For both benzenedithiol and benzenediamine we observe a large variability in low-bias conductance. We attribute these features to the slow breaking of the lithographic mechanically controllable break junctions and the absence of a solvent that may enable molecular readsorption after bond breaking. Nevertheless, we have been able to acquire reproducible current-voltage characteristics of benzenediamine and benzenedithiol using a statistical measurement approach. Benzenedithiol measurements yield a conductance gap of about 0.9 V at room temperature and 0.6 V at 77 K. In contrast, the current-voltage characteristics of benzenediamine-junctions typically display conductance gaps of about 0.9 V at both temperatures., Comment: 19 pages, 6 figures; v2: changed wrongly given HDA peak position in abstract to correct value, removed typing mistakes; v3: added three plots, improved discussion, removed typos

We present results on electromigrated Au nanojunctions broken near the conductance quantum $77.5 \mu$S. At room temperature we find that wires, initially narrowed by an actively-controlled electromigration technique down to a few conductance quanta, continue to narrow after removing the applied voltage. Separate electrodes form as mobile gold atoms continuously reconfigure the constriction. We find, from results obtained on over 300 samples, no evidence for gold cluster formation in junctions broken without an applied voltage, implying that gold clusters may be avoided by using this self-breaking technique., Comment: accepted in Applied physics letters

We report transport measurements through a single-molecule magnet, the Mn12 derivative [Mn12O12(O2C-C6H4-SAc)16(H2O)4], in a single-molecule transistor geometry. Thiol groups connect the molecule to gold electrodes that are fabricated by electromigration. Striking observations are regions of complete current suppression and excitations of negative differential conductance on the energy scale of the anisotropy barrier of the molecule. Transport calculations, taking into account the high-spin ground state and magnetic excitations of the molecule, reveal a blocking mechanism of the current involving non-degenerate spin multiplets., Comment: Accepted for Phys. Rev. Lett., 5 pages, 4 figures

We measure transport through gold grain quantum dots fabricated using electromigration, with magnetic impurities in the leads. A Kondo interaction is observed between dot and leads, but the presence of magnetic impurities results in a gate-dependent zero-bias conductance peak that is split due to an RKKY interaction between the spin of the dot and the static spins of the impurities. A magnetic field restores the single Kondo peak in the case of an antiferromagnetic RKKY interaction. This system provides a new platform to study Kondo and RKKY interactions in metals at the level of a single spin., Comment: 5 pages, 4 figures

Current-voltage characteristics of suspended single-wall carbon nanotube quantum dots show a series of steps equally spaced in voltage. The energy scale of this harmonic, low-energy excitation spectrum is consistent with that of the longitudinal low-k phonon mode (stretching mode) in the nanotube. Agreement is found with a Franck-Condon-based model in which the phonon-assisted tunneling process is modeled as a coupling of electronic levels to underdamped quantum harmonic oscillators. Comparison with this model indicates a rather strong electron-phonon coupling factor of order unity., Comment: 4 pages

We have studied the discrete electronic spectrum of closed metallic nanotube quantum dots. At low temperatures, the stability diagrams show a very regular four-fold pattern that allows for the determination of the electron addition and excitation energies. The measured nanotube spectra are in excellent agreement with theoretical predictions based on the nanotube band structure. Our results permit the complete identification of the electron quantum states in nanotube quantum dots., Comment: 4 pages, 3 figures

We report magnetic field spectroscopy measurements in carbon nanotube quantum dots exhibiting four-fold shell structure in the energy level spectrum. The magnetic field induces a large splitting between the two orbital states of each shell, demonstrating their opposite magnetic moment and determining transitions in the spin and orbital configuration of the quantum dot ground state. We use inelastic cotunneling spectroscopy to accurately resolve the spin and orbital contributions to the magnetic moment. A small coupling is found between orbitals with opposite magnetic moment leading to anticrossing behavior at zero field., Comment: 7 pages, 4 figures

We report a systematic study of the transport properties of coupled one-dimensional metallic chains as a function of the number of parallel chains. When the number of parallel chains is less than 2000, the transport properties show power-law behavior on temperature and voltage, characteristic for one-dimensional systems., Comment: 4 pages, 5 figures, submitted to Phys. Rev. Lett

We theoretically study the interplay between electrical and mechanical properties of suspended, doubly clamped carbon nanotubes in which charging effects dominate. In this geometry, the capacitance between the nanotube and the gate(s) depends on the distance between them. This dependence modifies the usual Coulomb models and we show that it needs to be incorporated to capture the physics of the problem correctly. We find that the tube position changes in discrete steps every time an electron tunnels onto it. Edges of Coulomb diamonds acquire a (small) curvature. We also show that bistability in the tube position occurs and that tunneling of an electron onto the tube drastically modifies the quantized eigenmodes of the tube. Experimental verification of these predictions is possible in suspended tubes of sub-micron length., Comment: 8 pages, 5 eps figures included. Major changes; new material added

CDW/Normal metal/CDW junctions and nanoconstrictions in crystals of the quasi-one-dimensional conductor NbSe$_3$ are manufactured using a focused-ion-beam. It is found that the low-temperature conduction of these structures changes dramatically and loses the features of the charge-density-wave transition. Instead, a dielectric phase is developed. Up to 6-order power-law variations of the conduction as a function of both temperature and electric field can be observed for this new phase. The transition from quasi-one-dimensional behavior to one-dimensional behavior is associated with destruction of the three-dimensional order of the charge-density waves by fluctuations. It results in a recovery of the Luttinger-liquid properties of metallic chains, like it takes place in sliding Luttinger liquid phase., Comment: 5 pages, 5 figures, RevTeX 4, Presented at PLDS-3 (9-14 October, Chernogolovka, Russia), to be published in proceedings of PLDS-3, Physics of Low-Dimensional Strucutires

Charge-density-wave dynamics is studied on a submicron length scale in NbSe_3 and o-TaS_3. Regions of negative absolute resistance are observed in the CDW sliding regime at sufficiently low temperatures. The origin of the negative resistance is attributed to the different forces that the deformed CDW and quasi-particles feel: the force on the CDW is merely caused by a difference of the electric potentials, while the quasi-particle current is governed by a difference of the electrochemical potentials., Comment: RevTeX, 4 pages with 3 figures, Submitted to PRL