arXiv subjects

H. S. J. van der Zant

Publications and source records attributed to H. S. J. van der Zant.

At least 19 recordsLinked to original sources

arXiv2026

Low-energy model for doped graphene nanoribbons

We analyse in this article the many-body behavior of free-standing doped graphene nanoribbons where the chemical potential lies inside the bulk single-particle bands. We perform an exact mapping from both an extended and an on-site Hubbard model of the ribbons to a Kanamori model, which includes ferromagnetic exchange and pair-hopping interactions. We determine the resulting Coulomb matrix elements analytically, and identify their scaling behavior as a function of ribbon width and length. We propose a low-energy version of the Kanamori Hamiltonian to address the response of the ribbons to external fields, with a view to their use as transport channels in nanoelectronics. We find that the model and the proposed ribbon parameters can produce open-shell, high-spin many-body states that can lead to shell- and spin-blockade responses.

cond-mat.mes-hall↗

arXiv2023

Evidence of an Off-resonant Electronic Transport Mechanism in Helicenes

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.

cond-mat.mes-hall↗

arXiv2023

Charge transfer and asymmetric coupling of MoSe$_2$ valleys to the magnetic order of CrSBr

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.

cond-mat.mes-hall↗

arXiv2023

Implementation of SNS thermometers into molecular devices for cryogenic thermoelectric experiments

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.

cond-mat.mes-hall↗

arXiv2022

Tension tuning of sound and heat transport in graphene

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.

cond-mat.mes-hall↗

arXiv2020

Controlling the anisotropy of a van der Waals antiferromagnet with light

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.

cond-mat.mtrl-sci↗

arXiv2018

Spin signatures in the electrical response of graphene nanogaps

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.

cond-mat.mes-hall↗

arXiv2017

Two-dimensional superconductivity at the (111)LaAlO$_3$/SrTiO$_3$ interface

We report on the discovery and transport study of the superconducting ground state present at the (111)LaAlO$_3$/SrTiO$_3$ interface. The superconducting transition is consistent with a Berezinskii-Kosterlitz-Thouless transition and its 2D nature is further corroborated by the anisotropy of the critical magnetic field, as calculated by Tinkham. The estimated superconducting layer thickness and coherence length are 10 nm and 60 nm, respectively. The results of this work provide a new platform to clarify the microscopic details of superconductivity at LaAlO$_3$/SrTiO$_3$ interfaces, in particular in what concerns the link with orbital symmetry.

cond-mat.supr-con↗

arXiv2017

Direct and parametric synchronization of a graphene self-oscillator

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.

cond-mat.mes-hall↗

arXiv2016

Franck-Condon Blockade in a Single-Molecule Transistor

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.

cond-mat.mes-hall↗

arXiv2016

Observing magnetic anisotropy in electronic transport through individual single-molecule magnets

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.

cond-mat.mes-hall↗

arXiv2016

Exchange coupling inversion in a high-spin organic triradical molecule

The magnetic properties of a nanoscale system are inextricably linked to its local environment. In ad-atoms on surfaces and inorganic layered structures the exchange interactions result from the relative lattice positions, layer thicknesses and other environmental parameters. Here, we report on a sample-dependent sign inversion of the magnetic exchange coupling between the three unpaired spins of an organic triradical molecule embedded in a three-terminal device. This ferro-to-antiferromagnetic transition is due to structural distortions and results in a high-to-low spin ground state change in a molecule traditionally considered to be a robust high-spin quartet. Moreover, the flexibility of the molecule yields an in-situ electric tunability of the exchange coupling via the gate electrode. These findings open a route to the controlled reversal of the magnetic states in organic molecule-based nanodevices by mechanical means, electrical gating or chemical tailoring.

cond-mat.mtrl-sci↗

arXiv2016

Sequential electron transport and vibrational excitations in an organic molecule coupled to few-kayer graphene electrodes

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.

cond-mat.mes-hall↗

arXiv2015

Image effects in transport at metal-molecule interfaces

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.

cond-mat.mes-hall↗

arXiv2015

Probing Transverse Magnetic Anisotropy by Electronic Transport through a Single-Molecule Magnet

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.

cond-mat.mes-hall↗

arXiv2015

Control of biaxial strain in single-layer Molybdenite using local thermal expansion of the substrate

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.

cond-mat.mes-hall↗

arXiv2015

Electric-field control of interfering transport pathways in a single-molecule anthraquinone transistor

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.

cond-mat.mes-hall↗

arXiv2015

Superconducting molybdenum-rhenium electrodes for single-molecule transport studies

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.

cond-mat.mes-hall↗