Differential Conductance Spectra Research Articles

Topological Band Engineering of One-Dimensional π-d Conjugated Metal-Organic Frameworks.

One-dimensional (1D) π-d conjugated metal-organic frameworks (c-MOFs) have garnered widespread research interest in chemical energy storage and conversion. In this work, we introduce a universal principle to engineer the topological bands of 1D c-MOFs. Connected by d orbitals of transition metals, two equivalent hidden molecular π orbitals in 1D c-MOFs can generate a staggered hopping within and between the organic ligands, forming Su-Schrieffer-Heeger-shaped 1D topological bands. Guided by this discovery, we investigate the electronic structures of the typical 1D c-MOF assembled from Ni atoms and 2HQDI (QDI = 2,5-diamino-1,4-benzoquinonediimine) precursors (NiQDI) by first-principles calculations, revealing 1D topological bands around the Fermi level. Due to local bonding variations at the QDI terminations, these two hidden molecular π orbitals become atomically bonded but electronically separated at the edge QDI, creating spatially localized in-gap topological edge states at the end of the NiQDI chain. This definitive signature for 1D topological bands is identified through differential conductance spectra in scanning tunneling microscopy measurements. Our results provide conclusive experimental evidence for topological bands in 1D c-MOFs, paving the way for exploring the topological physics in organic materials through frontier molecular orbitals.

Electronic States of Single Perovskite Quantum Dots in Weak and Strong Interaction Regimes: Implications in Electrically Pumped Quantum Emitters.

We investigate the effect of Coulomb interactions on the electronic states of a single perovskite quantum dot (PQD), CsPbBr3, through scanning tunneling microscopy/spectroscopy (STM/S). Under a weak interaction regime, where the time-averaged occupation of electrons in a PQD remains zero, the peaks observed in the differential tunneling conductance (dI/dV) spectrum correspond to the single-particle density of states (DOS) without any electron-electron correlation. However, with a shorter tunnel distance between the STM tip and PQD, additional electrons are trapped in the QD, leading to a strong interaction regime with well-defined electronic fine structures due to the lifting of spin degeneracy in the conduction bands. Interestingly, we observe that the strong Coulomb interaction can modify the spin-orbit coupling (SOC) strength in the PQDs. We have concluded that the energy levels under a strong electron-electron interaction regime are of utmost importance since they will be applicable to electrically pumped PQD-based single photon quantum emitters.

Two-phase/two-gap scenario in heavily reduced superconducting ITO films revealed by point-contact spectroscopy

We present the first point-contact measurements of heavily reduced indium tin oxide (ITO) films in the superconducting state, which simultaneously demonstrate high transparency in the visible light spectrum. Analysis of the differential conductance spectrum indicates the presence of two superconducting phases, the main one with a critical temperature Tc of about 4.6 K and an additional phase with Tc ∼ 10 K, most likely localized near the surface. The phase separation is indirectly confirmed by resistance measurements of the layers and ab initio calculations of the doped ITO electronic structure. The results obtained give hope for the creation of transparent superconducting films with critical temperatures of about 10 K.

Proximity-induced superconductivity in type-II Weyl semimetal NbIrTe4

Heterostructures between conventional superconductors and materials with different electronic ground states have emerged as a powerful method for exploring the exotic superconducting properties induced by the proximity effect. Here, we investigate Andreev transport through the interface between an s-wave superconductor Nb and a type-II Wely semimetal NbIrTe4. The differential conductance measurement reveals an anomalous zero-bias conductance peak and prominent subgap structures at low temperatures. Furthermore, we found that these subgap structures are not only related to the interface coupling strength but also influenced by the thickness of the NbIrTe4 flake. For thin devices (≤100 nm), the differential conductance spectra only exhibit a single-gap structure. While in thicker devices (∼150 nm), we observed the distinct double-gap structure, which is likely to originate from the proximity-induced superconductivity gap on the bulk and surface of the NbIrTe4 flakes. These results can provide a good reference for understanding the superconducting phase in type-II Weyl semimetals and take a step toward its future application in the field of superconducting electronics.

Probing the Inelastic Electron Tunneling via the Photocurrent in a Vertical Graphene van der Waals Heterostructure.

Inelastic electron tunneling (IET), accompanied by energy transfer between the tunneling charge carriers and other elementary excitations, is widely used to investigate the collective modes and quasiparticles in solid-state materials. In general, the inelastic contribution to the tunneling current is small compared to the elastic part and is therefore only prominent in the second derivative of the tunneling current with respect to the bias voltage. Here we demonstrate a direct observation of the IET by measuring the photoresponse in a graphene-based vertical tunnel junction device. Characteristic peaks/valleys are observed in the bias-voltage-dependent tunneling photocurrent at low temperatures, which barely shift with the gate voltage applied to graphene and diminish gradually as the temperature increases. By comparing with the second-order differential conductance spectra, we establish that these features are associated with the phonon-assisted IET. A simple model based on the photoexcited hot-carrier tunneling in graphene qualitatively explains the response. Our study points to a promising means of probing the low-energy elementary excitations utilizing the graphene-based van der Waals (vdW) heterostructures.

Realization of black phosphorus-like PbSe monolayer on Au(111) via epitaxial growth

Lead selenide (PbSe) has been attracted a lot attention in fundamental research and industrial applications due to its excellent infrared optical and thermoelectric properties, toward reaching the two-dimensional limit. Herein, we realize the black phosphorus-like PbSe (α-phase PbSe) monolayer on Au(111) via epitaxial growth, where a characteristic rectangular superlattice of 5 Å × 9 Å corresponding to 1 × 2 reconstruction with respect to the pristine of α-phase PbSe is observed by scanning tunneling microscopy. Corresponding density functional theory calculation confirmed the reconstruction and revealed the driven mechanism, the coupling between monolayer PbSe and Au(111) substrate. The metallic feature of differential conductance spectra as well as the transition of the density of states from semiconductor to metal further verified such coupling. As the unique anisotropic structure, our study provides a pathway towards the synthesis of BP-PbSe monolayer. In addition, it builds up an ideal platform for studying fundamental physics and also excellent prospects in PbSe-based device applications.

Fe-induced Kondo peak splitting in tip-functionalized scanning tunneling spectroscopy: A first-principles-based simulation

The spin-polarized scanning tunneling microscope (SP-STM) has been employed to enhance its capabilities of detecting the electronic and magnetic properties of organometallic molecules. Using a tip functionalized with a cobaltocene (Cc) molecule, recent SP-STM experiment performed on the Cu-tip/Cc/Fe/Cu(100) composite junction revealed an asymmetric Kondo resonance splitting in the differential conductance (dI/dV) spectrum. However, a systematic theoretical simulation of such system is lacking, and the important roles of the substrate spin-polarization and the Fe adatom still remain to be elucidated. In this work, by combining density functional theory and the hierarchical equations of motion methods, we achieve first-principles-based simulations of the tip control process of the Cu-tip/Cc/Fe/Cu(100) junction. We correctly reproduce the experimental results and demonstrate the influences of the Fe adatom on the spin-polarization of the substrate and on the Kondo resonance splitting in the dI/dV spectra.

Nonlinear transport properties of atomic copper point contacts

We report studies on the nonlinear electronic transport properties of copper point contacts. Utilizing the mechanically controllable break junction technique, various contact sizes can be realized to study ensemble-averaged differential conductance spectra at low temperatures. We investigate signatures of phonon excitations for contact sizes down to the atomic scale, where conductance fluctuations arise superimposing the phonon signatures. Applying high bias voltages to atomic-size copper contacts reveal additional features caused by atomic rearrangements.

Ultra-low-noise transimpedance amplifier in cryogenic STM for studying novel quantum states by measuring shot noise

An ultra-low-noise large-bandwidth transimpedance amplifier (TIA) for cryogenic scanning tunneling microscope (CryoSTM) is proposed. The TIA connected with the tip-sample component in CryoSTM is called as CryoSTM-TIA. Its transimpedance gain is as high as 1 GΩ, and its bandwidth is over 300 kHz, but its equivalent input noise current power spectral density is less than 4 (fA)2/Hz at 100 kHz. The low inherent noise for the CryoSTM-TIA is due to its special design: (1) its pre-amplifier is made of a pair of low-noise cryogenic high electron mobility transistors (HEMTs); (2) the noise generated by one HEMT is eliminated by a large capacitor; (3) the capacitance of the cable connected the gate of the other HEMT to the tip is minimized; (4) thermal noise sources, such as the feedback resistor, are placed in the cryogenic zone. The dc output voltage drift of the CryoSTM-TIA is very low, as 5 μV/°C. The apparatus can be used for measuring the scanning tunneling differential conductance spectra, especially the scanning tunneling shot noise spectra (STSNS) of quantum systems, even if the shot noise is very low. It provides a universal tool to study various novel quantum states by measuring STSNS, such as detecting the Majorana bound states.

Growth and local electronic properties of Cobalt nanodots underneath graphene on SiC(0001)

The coupling of graphene with a ferromagnetic material opens opportunities for technological innovations in spintronics. To obtain this coupling it is necessary to control the elaboration of interfaces at the atomic scale. Here, we present results on cobalt intercalation between graphene and a buffer layer supported on a SiC(0001) substrate. As a result, we obtain cobalt islands covered by graphene whose local electronic properties are measured by scanning tunneling microscopy and spectroscopy. These islands reveal two very distinct shapes and properties. Small-islands with atomic height and very narrow size distribution and, more interestingly, flat cobalt nanodots lower than one nanometer high, that are encapsulated by graphene. Compared to a graphene monolayer on SiC, those nanodots exhibit very different spectroscopic signatures. Using dI/dV local differential conductance spectra together with an analysis of image potential surface states measured thanks to dz/dV spectra, we show that graphene on the nanodots is neutrally charged. Moreover, its 4.65 eV work function is surprisingly larger than the predicted value of 3.8 eV for graphene on Co. First principle calculations show that those Co nanodots can be seen as cobalt bilayer sandwiched between two carbon planes.

Efficient tunability of size and optical properties of reduced graphene oxide-ZnO composite nanocrystallites on solid substrates

Growth of ultra-thin luminescent reduced graphene oxide (rGO)-zinc oxide (ZnO) composite nanostructures was accomplished by Langmuir-Blodgett (LB) transfer of GO-Zn composite layers onto solid substrates and subsequent oxidation. Layer structure of LB transferred composites and oxidation procedure determine the size distribution, density, structural order, optical quality of grown ZnO and the extent of GO reduction. Prolonged oxidation (120 min) of composite monolayers produce ZnO nanocrystallites nearly deprived of defects and exhibiting substantially enhanced band edge emission. Prior anchoring of Zn2+ ions on GO layers and oxidation facilitate controlled growth of ZnO nanocrystallites and nanoclusters (20–100 nm), offer tunability of absorption edge (325–355 nm) and assists in amendment of surface defects/band edge emission (376–384 nm). Conductivity of precursor and oxidized composite layers was mapped by recording STM images as well as STS spectra and, the obtained differential conductivity spectra substantiate the changes in GO conductivity and provide range of bandgap values of grown ZnO nanocrystallites (3.1–3.4 eV). The multiple GO-Zn compositing procedures and optimum oxidation conditions introduced in present work facilitate development of rGO-ZnO composite nanostructures with high optical, crystalline quality and conductive characteristics, which pave path for fabrication of such nanostructures for optoelectronic device applications.

Molecular properties of PTCDA on graphene grown on a rectangular symmetry substrate

The chemical modulation associated with moiré patterns, arising at the interface of metal-supported 2D material systems, affects the interaction between molecules and 2D materials on surfaces. Since the crystallography of the support influences the interfacial chemistry of the moiré modulation, this parameter could also play a role in the graphene-molecule interaction, although studies using non-hexagonal metal supports are needed to investigate this effect. It is a key issue since graphene appears combined with organic films in most technological advances related to this material. Here, we have characterized the properties of PTCDA molecules on graphene grown on Rh(110) substrates, which exhibit a rectangular atomic packing, using scanning tunneling microscopy and spectroscopy. The results showed that PTCDA molecules are arranged on the surface into a herringbone structure exhibiting a long-range ordering, which grows continuously across substrate atomic steps edge and dislocations. The quasi-1D moiré patterns of the Gr/Rh(110) surfaces are found to provide an inert chemical landscape for the molecular arrangement. Bias voltage-dependent imaging of the orbital structure of PTCDA molecules and differential conductance spectra back up a weak molecule–substrate interaction scheme. Finally, the α-polymorph of bulk crystal PTCDA has been determined as the favored stacking configuration for bilayer molecules on Gr/Rh(110).

Surface states passivation in GaN single crystal by ruthenium solution

GaN single crystal samples were cleaned and passivated with ruthenium solution. Photoluminescence (PL) and scanning tunneling spectroscopy (STS) were used to characterize the passivated surface. PL study showed an effective increase in band edge emission after passivation. I–V (current–voltage) and dI/dV (differential conductance) spectra measurements of GaN single crystal samples using ambient STS revealed the variation in the density of states (local), shifting of Fermi-level position, and onset/offset of valence and conduction bands. We found a significant change in I–V and dI/dV measurements after surface treatment, which means modification in surface electronic properties. The ruthenium solvent passivates the surface states, converting the surface into a highly ordered and air oxidation-resistant state. Finally, Ni/GaN Schottky diodes were fabricated to demonstrate improved device characteristics after passivation, which was a direct indication of improved GaN interface due to ruthenium passivation.

Mo-Re alloy: A new benchmark two-band superconductor

Multigap superconductivity, emerging in metals with several bands crossing the Fermi level, favors exotic superconducting orders that have no equivalent in a single-band counterpart. In this context, it is important to search for new materials with well-established two (or more) gaps having distinctly different sizes. In this work, we confirm previous statements and present new evidence to support the claim that Mo-Re alloy with a comparable concentration of the components is a two-band/two-gap superconductor. The differential conductance spectra obtained in point-contact experiments demonstrate the presence of a bosonic, undamped collective mode and its harmonics associated with the superconducting state. Following previous works on MgB2, we have identified these features as manifestations of the so-called Leggett mode arising due to relative phase fluctuations between two superconducting order parameters.

Anomalous temperature dependence of multiple Andreev reflections in a topological insulator Josephson junction

As a promising platform for unconventional superconductivity, Josephson junctions (JJs) of tetradymite topological insulators (TIs) and s-wave superconductors have been investigated in recent years. This family of TI materials, however, often suffers from spurious bulk transport, which hampers the observation of the exotic physics of their topological surface states. Thus, disentangling the transport mechanism of bulk and surface contributions in TI JJs is of high importance when investigating proximity induced superconductivity in those crystals. In this work, we add to the insights regarding these contributions by studying the temperature-dependent behaviour of a Bi2Te3-based JJ with transparent interfaces. In electrical transport measurements, we investigate differential conductance spectra of multiple Andreev reflections (MARs) and find a qualitative temperature-dependent change from peak features at low temperatures to dip features at higher ones. The observation of both kind of MAR patterns in a single JJ suggests contributions of diffusive bulk and ballistic surface states and links to a similar finding in the temperature dependence of the critical current. Our work advances the research of induced superconductivity in TIs and offers new avenues to study the induced superconductivity in the topological surface states of these materials.

STM/STS Study of the Density of States and Contrast Behavior at the Boundary between (7 × 7)N and (8 × 8) Structures in the SiN/Si(111) System

The origin of the contrast appearing in STM images at the boundary between diverse ordered structures is studied using the example of two structures, (7 × 7)N and (8 × 8), formed in the system of a two-dimensional silicon nitride layer on the Si(111) surface during ammonia nitridation. A significant dependence of the contrast between these structures on the voltage applied to the tunnel gap was found and studied both experimentally and theoretically. Variations in the contrast were quantitatively studied in the range from −3 V to +3 V, and they were studied in more detail for the positive biases on the sample from +1 V to +2.5 V, where the contrast was changed more than 2 times. Within the one-dimensional Wentzel–Kramers–Brillouin (WKB) model for the tunnel current, a comparatively simple procedure is proposed for the correction of the experimental STS-spectra of differential conductivity to identify the adequate (feasible) density of electron states (DOS). It is shown that the (8 × 8) structure DOS corresponds to a graphene-like layer of silicon nitride structure. The proposed correction procedure of the empirical differential conductivity spectra measured by STS will be useful for the quantitative determination of the DOS of new two-dimensional materials and surface structures.

Magnetic field constraint for Majorana zero modes in a hybrid nanowire

The hybrid semiconductor-superconductor nanowire is expected to serve as an experimental platform to support Majorana zero modes. By rederiving its effective Kitaev model with spins, we discover a topological phase diagram, which assigns a more precise constraint on the magnetic field strength for the emergence of Majorana zero modes. We find that the effective pairing strength dressed by the proximity effect exhibits a significant dependence on the magnetic field, and thus the topological phase region is refined into a closed triangle in the phase diagram with chemical potential vs Zeeman energy (which is obviously different from the open hyperbolic region known before). This prediction is confirmed again by an exact calculation of quantum transport, where the zero bias peak of $2{e}^{2}/h$ in the differential conductance spectrum, as the necessary evidence for the Majorana zero modes, disappears when the magnetic field grows too strong. Therefore, the hybrid nanowire system does not support Majorana zero modes under a too strong magnetic field. For illustrations with practical hybrid systems, in the InSb nanowire coupled to NbTiN, the accessible magnetic field range is around 0.1--1.5 T; when coupled to an aluminum shell, the accessible magnetic field range should be smaller than 0.12 T. Our predictions are essential to significantly narrow down the range of magnetic fields for further searching Majorana zero modes in experiments.

Spin-related electronic pathway through single molecule on Au(111)

Spin properties of organic molecules have attracted great interest for their potential applications in spintronic devices and quantum computing. Fe-tetraphenyl porphyrin (FeTPP) is of particular interest for its robust magnetic properties on metallic substrates. FeTPP is prepared in vacuum via on-surface synthesis. Molecular structure and spin-related transport properties are characterized by low-temperature scanning tunneling microscope and spectroscopy at 0.5 K. Density functional theory calculations are performed to understand molecular adsorption and spin distribution on Au(111). The molecular structure of FeTPP is distorted upon adsorption on the substrate. Spin excitations of FeTPP are observed on the Fe atom and high pyrrole groups in differential conductance spectra. The calculated spin density distribution indicates that the electron spin of FeTPP is mainly distributed on the Fe atom. The atomic transmission calculation indicates that electrons transport to substrate is mediated through Fe atom, when the tip is above the high pyrrole group.

Disentangling the electronic structure of an adsorbed graphene nanoring by scanning tunneling microscopy

Graphene nanorings are promising model structures to realize persistent ring currents and Aharonov–Bohm effect at the single molecular level. To investigate such intriguing effects, precise molecular characterization is crucial. Here, we combine low-temperature scanning tunneling imaging and spectroscopy with CO functionalized tips and algorithmic data analysis to investigate the electronic structure of the molecular cycloarene C108 (graphene nanoring) adsorbed on a Au(111) surface. We demonstrate that CO functionalized tips enhance the visibility of molecular resonances, both in differential conductance spectra and in real-space topographic images. Comparing our experimental data with ab-initio density functional theory reveals a remarkably precise agreement of the molecular orbitals and enables us to disentangle close-lying molecular states only separated by 50 meV at an energy of 2 eV below the Fermi level. We propose this combination of techniques as a promising new route for a precise electronic characterization of complex molecules and other physical properties which have electronic resonances in the tip-sample junction.

Spin-polarized supercurrent through the van der Waals Kondo-lattice ferromagnet Fe3GeTe2

In the new van der Waals Kondo-lattice Fe$_3$GeTe$_2$, itinerant ferromagnetism and heavy fermionic behaviour coexist. Both the key properties of such a system namely a spin-polarized Fermi surface and a low Fermi momentum are expected to significantly alter Andreev reflection dominated transport at a contact with a superconducting electrode, and display unconventional proximity-induced superconductivity. We observed interplay between Andreev reflection and Kondo resonance at mesoscopic interfaces between superconducting Nb and Fe$_3$GeTe$_2$. Above the critical temperature ($T_c$) of Nb, the recorded differential conductance ($dI/dV$) spectra display a robust zero-bias anomaly which is described well by a characteristic Fano line shape arising from Kondo resonance. Below $T_c$, the Fano line mixes with Andreev reflection dominated $dI/dV$ leading to a dramatic, unconventional suppression of conductance at zero bias. As a consequence, an analysis of the Andreev reflection spectra within a spin-polarized model yields an anomalously large spin-polarization which is not explained by the density of states of the spin-split bands at the Fermi surface alone. The results open up the possibilities of fascinating interplay between various quantum phenomena that may potentially emerge at the mesoscopic superconducting interfaces involving Kondo lattice systems hosting spin-polarized conduction electrons.