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At least 55 records · Page 3

Resistivity of Surface Steps in Bulk-Insulating Topological Insulators

Electron transport in topological insulators usually involves both topologically protected surface states and trivial electronic states in the bulk material. The surface transport is particularly interesting; however, it is also susceptible to atomic defects on the surfaces, such as vacancies, impurities, and step edges. Experimental determination of scattering effects of these surface defects requires both nanoscale spatial resolution and the ability to decipher surface transport from bulk transport. Here we directly measure the resistivity of individual surface steps in the surface dominating transport process of topological insulator Bi 2 Te 2 Se. A variable probe-spacing transport spectroscopy with a multiprobe scanning tunneling microscope is used to differentiate the surface conductance from bulk conductance, allowing the identification of a surface dominant transport regime. The technique also reveals a deviation from ideal 2D transport at atomic steps. Then, a multi-probe scanning tunneling potentiometry is employed to visualize the electrochemical potentials across individual step edges. A quantitative analysis of the potential distributions enables us to acquire a resistivity of 0.530 mΩ · cm for the one quintuple-layer atomic step. The result indicates that atomic defects, despite preserving the time-reversal symmetry, can still significantly affect the transport in topological insulators.

36 MATERIALS SCIENCE↗

Quantifying the Variation in the Number of Donors in Quantum Dots Created Using Atomic Precision Advanced Manufacturing

Atomic-precision advanced manufacturing enables unique silicon quantum electronics built on quantum dots fabricated from small numbers of phosphorus dopants. The number of dopant atoms comprising a dot plays a central role in determining the behavior of charge and spin confined to the dots and thus overall device performance. Here in this work, we use both theoretical and experimental techniques to explore the combined impact of lithographic variation and stochastic kinetics on the number of P incorporations in quantum dots made using these techniques and how this variation changes as a function of the size of the dot. Using a kinetic model of PH3 dissociation augmented with novel reaction barriers, we demonstrate that for a 2 × 3 silicon dimer window the probability that no donor incorporates goes to zero, allowing for certainty in the placement of at least one donor. However, this still comes with some uncertainty in the precise number of incorporated donors (either one or two), and this variability may still impact certain applications. We also examine the impact of the size of the initial lithographic window, finding that the incorporation fraction saturates to δ-layer-like coverage as the circumference-to-area ratio decreases. We predict that this incorporation fraction depends strongly on the dosage of the precursor and that the standard deviation of the number of incorporations scales as ~√n, as would be expected for a sequence of largely independent incorporation events. Finally, we characterize an array of 36 experimentally prepared multidonor 3 × 3 nm lithographic windows with scanning tunneling microscopy, measuring the fidelity of the lithography to the desired array and the final location of PH x fragments within these lithographic windows. We use our kinetic model to examine the expected variability due to the observed lithographic error, predicting a negligible impact on incorporation statistics. We find good agreement between our model and the inferred incorporation locations in these windows from scanning tunneling microscope measurements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Observation of backscattering induced by magnetism in a topological edge state

Significance One of the predicted characteristics of helical topological boundary modes is the absence of backscattering when time-reversal symmetry (TRS) is preserved. While previous experiments have provided evidence for this topological protection, inducing backscattering by breaking TRS has yet to be demonstrated. We test this fundamental property by investigating quasiparticle scattering in the one-dimensional topological edge state of bismuth bilayers, coupled to ferromagnetic iron clusters, using a scanning tunneling microscope. Our experimental observations demonstrate that backscattering is induced by magnetism of iron clusters in these topological edge modes.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Topography and transport properties of oligo(phenylene ethynylene) molecular wires studied by scanning tunneling microscopy

Conjugated phenylene(ethynylene) molecular wires are of interest as potential candidates for molecular electronic devices. Scanning tunneling microscopic study of the topography and current-voltage (I-V) characteristics of self-assembled monolayers of two types of molecular wires are presented here. The study shows that the topography and I-Vs, for small scan voltages, of the two wires are quite similar and that the electronic and structural changes introduced by the substitution of an electronegative N atom in the central phenyl ring of these wires does not significantly alter the self-assembly or the transport properties.

Polymers/chemistry↗

Atomic-scale manipulation of polar domain boundaries in monolayer ferroelectric In 2 Se 3

Domain boundaries have been intensively investigated in bulk ferroelectric materials and two-dimensional materials. Many methods such as electrical, mechanical and optical approaches have been utilized to probe and manipulate domain boundaries. So far most research focuses on the initial and final states of domain boundaries before and after manipulation, while the microscopic understanding of the evolution of domain boundaries remains elusive. In this paper, we report controllable manipulation of the domain boundaries in two-dimensional ferroelectric In 2 Se 3 with atomic precision using scanning tunneling microscopy. We show that the movements of the domain boundaries can be driven by the electric field from a scanning tunneling microscope tip and proceed by the collective shifting of atoms at the domain boundaries. Our density functional theory calculations reveal the energy path and evolution of the domain boundary movement. The results provide deep insight into domain boundaries in two-dimensional ferroelectric materials and will inspire inventive applications of these materials.

36 MATERIALS SCIENCE↗

Microscopic Manipulation of Ferroelectric Domains in SnSe Monolayers at Room Temperature

Two-dimensional (2D) van der Waals ferroelectrics provide an unprecedented architectural freedom for the creation of artificial multiferroics and nonvolatile electronic devices based on vertical and coplanar heterojunctions of 2D ferroic materials. Nevertheless, controlled microscopic manipulation of ferroelectric domains is still rare in monolayer-thick 2D ferroelectrics with in-plane polarization. Here we report the discovery of robust ferroelectricity with a critical temperature close to 400 K in SnSe monolayer plates grown on graphene and the demonstration of controlled room-temperature ferroelectric domain manipulation by applying appropriate bias voltage pulses to the tip of a scanning tunneling microscope (STM). This study shows that STM is a powerful tool for detecting and manipulating the microscopic domain structures in 2D ferroelectric monolayers, which are difficult for conventional approaches such as piezoresponse force microscopy, thus facilitating the hunt for other 2D ferroelectric monolayers with in-plane polarization with important technological applications.

2D ferroelectric↗

Atomically precise control of rotational dynamics in charged rare-earth complexes on a metal surface

Abstract Complexes containing rare-earth ions attract great attention for their technological applications ranging from spintronic devices to quantum information science. While charged rare-earth coordination complexes are ubiquitous in solution, they are challenging to form on materials surfaces that would allow investigations for potential solid-state applications. Here we report formation and atomically precise manipulation of rare-earth complexes on a gold surface. Although they are composed of multiple units held together by electrostatic interactions, the entire complex rotates as a single unit when electrical energy is supplied from a scanning tunneling microscope tip. Despite the hexagonal symmetry of the gold surface, a counterion at the side of the complex guides precise three-fold rotations and 100% control of their rotational directions is achieved using a negative electric field from the scanning probe tip. This work demonstrates that counterions can be used to control dynamics of rare-earth complexes on materials surfaces for quantum and nanomechanical applications.

36 MATERIALS SCIENCE↗

Accessing Atomic-scale Phosphorus Dopant Distribution in Precise Silicon Devices by Advanced STEM Imaging and Spectroscopy

The structural and chemical characterization at the atomic-scale plays a critical role in understanding the structure-property relationship in precise electrical devices such as those produced by atomic-precision advanced manufacturing (APAM). APAM, utilizing hydrogen lithography in a scanning tunneling microscope, offers a potential pathway to ultra-efficient transistors, and has been developed to produce phosphorus (P)-based donor devices integrated into bare Si substrates. Structural characterization of the buried, Si with P dopant (Si:P) delta-layer in the devices by scanning transmission electron microscopy (STEM), however, is a challenge due to similar atomic number and low concentration of the P dopants. In this paper, we describe several efforts of utilizing advanced STEM imagining and spectroscopic techniques to quantify the Si:P deltalayers. STEM imaging combining low-angle and high-angle annular dark-field (LAADF, HAADF) detectors as well as atomic-scale elemental mapping using energy-dispersive X-ray spectroscopy (EDS) are used to reveal the P and defect distribution across the delta-layer processed under various thermal conditions.

47 OTHER INSTRUMENTATION↗

Observation of Single-Electron Transport and Charging on Individual Point Defects in Atomically Thin WSe 2

Defects significantly impact the properties of 2D semiconductors, providing in-gap quantum states that can serve as a natural platform for single-electron operations, localization sites for excitons to serve as single-photon sources, and potentially quantum spin memories. To date, however, a microscopic observation of such a single-electron transport (SET) behavior has been rarely reported on single defects of 2D semiconductors. In this study, we report a SET and charge-state transition on individual point-defect states buried in the bilayer WSe 2 using scanning tunneling microscopy. SET characteristics of their states is evidenced by both the Coulomb staircase and the saturation behavior of the transport current, consistent with the SET model. Furthermore, we demonstrate that, through the local field of a scanning tunneling microscope tip, it is possible to successively charge the defects by single electrons, suggested by both the ring structures and charging peaks in dI/dV measurements. Our results provide new insights into the quantum nature of these defect-bound states, as well as the possibility of using their single-electron behavior and response for applications in quantum information and local-field sensing.

2D semiconductor↗

Ultrafast method for scanning tunneling spectroscopy

A scanning tunneling microscope (STM) combines unique capabilities in imaging and spectroscopy with atomic precision, and it can obtain energy-resolved spectroscopic data with atomic resolution. In this paper, we utilize a recently proposed modification to the STM feedback control loop to acquire high quality d 2 I/dV 2 images. We have developed a constant differential conductance imaging method by closing the STM feedback loop with a high precision dI/dV measurement. In this mode, the tip’s vertical position is adjusted so as to keep the differential conductance constant during raster scanning of the surface. Based on this imaging mode, we propose a new technique to acquire fast and reliable scanning tunneling spectroscopy (STS) data simultaneously with the imaging.

47 OTHER INSTRUMENTATION↗

Photothermal alternative to device fabrication using atomic precision advanced manufacturing techniques

The attachment of dopant precursor molecules to depassivated areas of hydrogen-terminated silicon templated with a scanning tunneling microscope (STM) has been used to create electronic devices with subnanometer precision, typically for quantum physics experiments. This process, which we call atomic precision advanced manufacturing (APAM), dopes silicon beyond the solid-solubility limit and produces electrical and optical characteristics that may also be useful for microelectronic and plasmonic applications. However, scanned probe lithography lacks the throughput required to develop more sophisticated applications. In this work, we demonstrate and characterize an APAM device workflow where scanned probe lithography of the atomic layer resist has been replaced by photolithography. An ultraviolet laser is shown to locally and controllably heat silicon above the temperature required for hydrogen depassivation on a nanosecond timescale, a process resistant to under- and overexposure. STM images indicate a narrow range of energy density where the surface is both depassivated and undamaged. Modeling that accounts for photothermal heating and the subsequent hydrogen desorption kinetics suggests that the silicon surface temperatures reached in our patterning process exceed those required for hydrogen removal in temperature-programmed desorption experiments. A phosphorus-doped van der Pauw structure made by sequentially photodepassivating a predefined area and then exposing it to phosphine is found to have a similar mobility and higher carrier density compared with devices patterned by STM. Lastly, it is also demonstrated that photodepassivation and precursor exposure steps may be performed concomitantly, a potential route to enabling APAM outside of ultrahigh vacuum.

nanoscale devices↗

Two-Dimensional Molecular Charge Density Waves in Single-Layer-Thick Islands of a Dirac Fermion System

Charge density waves have been intensely studied in inorganic materials such as transition metal dichalcogenides however its counterpart in organic materials has yet to be explored in detail. Here we report the finding of a robust two dimensional charge density waves in molecular layers formed by α-(BEDT-TTF) 2 -I 3 on a Ag(111) surface. Low temperature scanning tunnelling microscopy images of a multi-layer thick α-(BEDT-TTF) 2 -I 3 on Ag(111) substrate reveal coexistence of 5a0 x 5a0 and √31 a0 x √31 a0 R9° charge density wave patterns commensurate with the underlying molecular lattice at 80 K. Both charge density wave patterns remain in nano-size molecular islands with just a single constituent molecular-layer thickness at 80 K and 5 K. Local tunneling spectroscopy measurements reveal the variation of the gap from 244 meV to 288 meV between the maximum and minimum charge density wave locations. Density functional theory calculations further confirm a vertical positioning of BEDT-TTF molecules in the molecular layer. While the observed charge density wave patterns are stable for the defect sites, they can be reversely switched for one molecular lattice site by means of inelastic tunnelling electron energy transfer with the electron energies exceeding 400 meV using a scanning tunneling microscope manipulation scheme.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Scanning tunneling microscopy studies of diamond films and optoelectronic materials

In this report, we report on progress achieved from 12/1/92 to 10/1/93 under the grant entitled 'Scanning Tunneling Microscopy Studies of Diamond Films and Optoelectronic Materials'. We have set-up a chemical vapor deposition (CVD) diamond film growth system and a Raman spectroscopy system to study the nucleation and growth of diamond films with atomic resolution using scanning tunneling microscopy (STM). A unique feature of the diamond film growth system is that diamond films can be transferred directly to the ultrahigh vacuum (UHV) chamber of a scanning tunneling microscope without contaminating the films by exposure to air. The University of North Texas (UNT) provided $20,000 this year as matching funds for the NASA grant to purchase the diamond growth system. In addition, UNT provided a Coherent Innova 90S Argon ion laser, a Spex 1404 double spectrometer, and a Newport optical table costing $90,000 to set-up the Raman spectroscopy system. The CVD diamond growth system and Raman spectroscopy system will be used to grow and characterize diamond films with atomic resolution using STM as described in our proposal. One full-time graduate student and one full-time undergraduate student are supported under this grant. In addition, several graduate and undergraduate students were supported during the summer to assist in setting-up the diamond growth and Raman spectroscopy systems. We have obtained research results concerning STM of the structural and electronic properties of CVD grown diamond films, and STM and scanning tunneling spectroscopy of carbon nanotubes. In collaboration with the transmission electron microscopy (TEM) group at UNT, we have also obtained results concerning the optoelectronic material siloxene. These results were published in refereed scientific journals, submitted for publication, and presented as invited and contributed talks at scientific conferences.

Perez, Jose M.↗

Polarized tip-enhanced Raman spectroscopy at liquid He temperature in ultrahigh vacuum using an off-axis parabolic mirror

Tip-enhanced Raman spectroscopy (TERS) combines inelastic light scattering well below the diffraction limit down to the nanometer range and scanning probe microscopy and, possibly, spectroscopy. In this way, topographic and spectroscopic as well as single- and two-particle information may simultaneously be collected. While single molecules can now be studied successfully, bulk solids are still not meaningfully accessible. It is the purpose of the work presented here to outline approaches toward this objective. We describe a home-built, liquid helium cooled, ultrahigh vacuum TERS. The setup is based on a scanning tunneling microscope and, as an innovation, an off-axis parabolic mirror having a high numerical aperture of ~0.85 and a large working distance. The system is equipped with a fast load-lock chamber, a chamber for the in situ preparation of tips, substrates, and samples, and a TERS chamber. Base pressure and temperature in the TERS chamber were ~3 × 10 –11 mbar and 15 K, respectively. Polarization dependent tip-enhanced Raman spectra of the vibration modes of carbon nanotubes were successfully acquired at cryogenic temperature. The new features described here including very low pressure and temperature and the external access to the light polarizations, thus the selection rules, may pave the way toward the investigation of bulk and surface materials.

47 OTHER INSTRUMENTATION↗

Transmission measurement based on STM observation to detect the penetration depth of low-energy heavy ions in botanic samples

The penetration depth of low-energy heavy ions in botanic samples was detected with a new transmission measurement. In the measurement, highly oriented pyrolytic graphite (HOPG) pieces were placed behind the botanic samples with certain thickness. During the irradiation of heavy ions with energy of tens of keV, the energetic particles transmitted from those samples were received by the HOPG pieces. After irradiation, scanning tunneling microscope (STM) was applied to observe protrusion-like damage induced by these transmitted ions on the surface of the HOPG. The statistical average number density of protrusions and the minimum transmission rate of the low-energy heavy ions can be obtained. The detection efficiency of the new method for low-energy heavy ions was about 0.1-1 and the background in the measurement can be reduced to as low as 1.0 x 10(8) protrusions/cm2. With this method, the penetration depth of the energetic particles was detected to be no less than 60 micrometers in kidney bean slices when the slices were irradiated by 100 keVAr+ ion at the fluence of 5 x 10(16) ions/cm2. c2002 Elsevier Science Ltd. All rights reserved.

DNA Damage↗

Defect‐Free Nanowelding of Bilayer SnSe Nanoplates

Nanowelding is a bottom‐up technique to create custom‐designed nanostructures and devices beyond the precision of lithographic methods. Here, a new technique is reported based on anisotropic lubricity at the van der Waals interface between monolayer and bilayer SnSe nanoplates and a graphene substrate to achieve precise control of the crystal orientation and the interface during the welding process. As‐grown SnSe monolayer and bilayer nanoplates are commensurate with graphene's armchair direction but lack commensuration along graphene's zigzag direction, resulting in a reduced friction along that direction and a rail‐like, 1D movement that permits joining nanoplates with high precision. This way, molecular beam epitaxially grown SnSe nanoplates of lateral sizes 30–100 nm are manipulated by the tip of a scanning tunneling microscope at room temperature. In situ annealing is applied afterward to weld contacting nanoplates without atomic defects at the interface. This technique can be generalized to any van der Waals interfaces with anisotropic lubricity and is highly promising for the construction of complex quantum devices, such as field effect transistors, quantum interference devices, lateral tunneling junctions, and solid‐state qubits.

2D ferroelectrics↗

Imaging the Breakdown and Restoration of Topological Protection in Magnetic Topological Insulator MnBi 2 Te 4

Quantum anomalous Hall (QAH) insulators transport charge without resistance along topologically protected chiral 1D edge states. Yet, in magnetic topological insulators to date, topological protection is far from robust, with zero-magnetic field QAH effect only realized at temperatures an order of magnitude below the Néel temperature T N , though small magnetic fields can stabilize QAH effect. Understanding why topological protection breaks down is therefore essential to realizing QAH effect at higher temperatures. Here a scanning tunneling microscope is used to directly map the size of exchange gap (E g,ex ) and its spatial fluctuation in the QAH insulator 5-layer MnBi 2 Te 4 . Long-range fluctuations of E g,ex are observed, with values ranging between 0 (gapless) and 70 meV, appearing to be uncorrelated to individual surface point defects. The breakdown of topological protection is directly imaged, showing that the gapless edge state, the hallmark signature of a QAH insulator, hybridizes with extended gapless regions in the bulk. Finally, it is unambiguously demonstrated that the gapless regions originate from magnetic disorder, by demonstrating that a small magnetic field restores E g,ex in these regions, explaining the recovery of topological protection in magnetic fields. The results indicate that overcoming magnetic disorder is the key to exploiting the unique properties of QAH insulators.

36 MATERIALS SCIENCE↗

Atomically precise engineering of spin–orbit polarons in a kagome magnetic Weyl semimetal

Atomically precise defect engineering is essential to manipulate the properties of emerging topological quantum materials for practical quantum applications. However, this remains challenging due to the obstacles in modifying the typically complex crystal lattice with atomic precision. Here, we report the atomically precise engineering of the vacancy-localized spin–orbit polarons in a kagome magnetic Weyl semimetal Co 3 Sn 2 S 2 , using scanning tunneling microscope. We achieve the step-by-step repair of the selected vacancies, leading to the formation of artificial sulfur vacancies with elaborate geometry. We find that that the bound states localized around these vacancies undergo a symmetry dependent energy shift towards Fermi level with increasing vacancy size. As the vacancy size increases, the localized magnetic moments of spin–orbit polarons become tunable and eventually become itinerantly negative due to spin–orbit coupling in the kagome flat band. These findings provide a platform for engineering atomic quantum states in topological quantum materials at the atomic scale.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗