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Electric current paths in a Si:P delta-doped device imaged by nitrogen-vacancy diamond magnetic microscopy

Nanotechnology

Basso, Luca B.; Kehayias, Pauli M.; Henshaw, Jacob D.; Ziabari, Maziar S.; Byeon, Heejun B.; Lilly, Michael L.; Bussmann, Ezra B.; Campbell, DeAnna M.; Misra, Shashank M.; Mounce, Andrew M.

The recently-developed ability to control phosphorous-doping of silicon at an atomic level using scanning tunneling microscopy, a technique known as atomic precision advanced manufacturing (APAM), has allowed us to tailor electronic devices with atomic precision, and thus has emerged as a way to explore new possibilities in Si electronics. In these applications, critical questions include where current flow is actually occurring in or near APAM structures as well as whether leakage currents are present. In general, detection and mapping of current flow in APAM structures are valuable diagnostic tools to obtain reliable devices in digital-enhanced applications. In this report, we used nitrogen-vacancy (NV) centers in diamond for wide-field magnetic imaging (with a few-mm field of view and micron-scale resolution) of magnetic fields from surface currents flowing in an APAM test device made of a P delta-doped layer on a Si substrate, a standard APAM witness material. We integrated a diamond having a surface NV ensemble with the device (patterned in two parallel mm-sized ribbons), then mapped the magnetic field from the DC current injected in the APAM device in a home-built NV wide-field microscope. The 2D magnetic field maps were used to reconstruct the surface current densities, allowing us to obtain information on current paths, device failures such as choke points where current flow is impeded, and current leakages outside the APAM-defined P-doped regions. Analysis on the current density reconstructed map showed a projected sensitivity of ~0.03 A m-1, corresponding to a smallest-detectable current in the 200 μm wide APAM ribbon of ~6 μA. These results demonstrate the failure analysis capability of NV wide-field magnetometry for APAM materials, opening the possibility to investigate other cutting-edge microelectronic devices.

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Hole in one: Pathways to deterministic single-acceptor incorporation in Si(100)-2 × 1

AVS Quantum Science

Campbell, Quinn C.; Baczewski, Andrew D.; Butera, R.E.; Misra, Shashank M.

Stochastic incorporation kinetics can be a limiting factor in the scalability of semiconductor fabrication technologies using atomic-precision techniques. While these technologies have recently been extended from donors to acceptors, the extent to which kinetics will impact single-acceptor incorporation has yet to be assessed. To identify the precursor molecule and dosing conditions that are promising for deterministic incorporation, we develop and apply an atomistic model for the single-acceptor incorporation rates of several recently demonstrated molecules: diborane (B2H6), boron trichloride (BCl3), and aluminum trichloride in both monomer (AlCl3) and dimer forms (Al2Cl6). While all three precursors can realize single-acceptor incorporation, we predict that diborane is unlikely to realize deterministic incorporation, boron trichloride can realize deterministic incorporation with modest heating (50 °C), and aluminum trichloride can realize deterministic incorporation at room temperature. We conclude that both boron and aluminum trichloride are promising precursors for atomic-precision single-acceptor applications, with the potential to enable the reliable production of large arrays of single-atom quantum devices.

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Revealing quantum effects in highly conductive δ-layer systems

Communications Physics

Mamaluy, Denis M.; Mendez Granado, Juan P.; Gao, Xujiao G.; Misra, Shashank M.

Thin, high-density layers of dopants in semiconductors, known as δ-layer systems, have recently attracted attention as a platform for exploration of the future quantum and classical computing when patterned in plane with atomic precision. However, there are many aspects of the conductive properties of these systems that are still unknown. Here we present an open-system quantum transport treatment to investigate the local density of electron states and the conductive properties of the δ-layer systems. A successful application of this treatment to phosphorous δ-layer in silicon both explains the origin of recently-observed shallow sub-bands and reproduces the sheet resistance values measured by different experimental groups. Further analysis reveals two main quantum-mechanical effects: 1) the existence of spatially distinct layers of free electrons with different average energies; 2) significant dependence of sheet resistance on the δ-layer thickness for a fixed sheet charge density.

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Al-alkyls as acceptor dopant precursors for atomic-scale devices

Journal of Physics Condensed Matter

Owen, J.H.G.; Campbell, Quinn C.; Santini, R.; Ivie, J.A.; Baczewski, Andrew D.; Schmucker, S.W.; Bussmann, Ezra B.; Misra, Shashank M.; Randall, J.N.

Atomically precise ultradoping of silicon is possible with atomic resists, area-selective surface chemistry, and a limited set of hydride and halide precursor molecules, in a process known as atomic precision advanced manufacturing (APAM). It is desirable to expand this set of precursors to include dopants with organic functional groups and here we consider aluminium alkyls, to expand the applicability of APAM. We explore the impurity content and selectivity that results from using trimethyl aluminium and triethyl aluminium precursors on Si(001) to ultradope with aluminium through a hydrogen mask. Comparison of the methylated and ethylated precursors helps us understand the impact of hydrocarbon ligand selection on incorporation surface chemistry. Combining scanning tunneling microscopy and density functional theory calculations, we assess the limitations of both classes of precursor and extract general principles relevant to each.

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The stability of Cl-, Br-, and I-passivated Si(100)-(2 × 1) in ambient environments for atomically-precise pattern preservation

Journal of Physics Condensed Matter

Frederick, Esther F.; Dwyer, K.J.; Wang, George T.; Misra, Shashank M.; Butera, R.E.

Atomic precision advanced manufacturing (APAM) leverages the highly reactive nature of Si dangling bonds relative to H- or Cl-passivated Si to selectively adsorb precursor molecules into lithographically defined areas with sub-nanometer resolution. Due to the high reactivity of dangling bonds, this process is confined to ultra-high vacuum (UHV) environments, which currently limits its commercialization and broad-based appeal. In this work, we explore the use of halogen adatoms to preserve APAM-derived lithographic patterns outside of UHV to enable facile transfer into real-world commercial processes. Specifically, we examine the stability of H-, Cl-, Br-, and I-passivated Si(100) in inert N2 and ambient environments. Characterization with scanning tunneling microscopy and x-ray photoelectron spectroscopy (XPS) confirmed that each of the fully passivated surfaces were resistant to oxidation in 1 atm of N2 for up to 44 h. Varying levels of surface degradation and contamination were observed upon exposure to the laboratory ambient environment. Characterization by ex situ XPS after ambient exposures ranging from 15 min to 8 h indicated the Br– and I–passivated Si surfaces were highly resistant to degradation, while Cl–passivated Si showed signs of oxidation within minutes of ambient exposure. As a proof-of-principle demonstration of pattern preservation, a H–passivated Si sample patterned and passivated with independent Cl, Br, I, and bare Si regions was shown to maintain its integrity in all but the bare Si region post-exposure to an N2 environment. The successful demonstration of the preservation of APAM patterns outside of UHV environments opens new possibilities for transporting atomically-precise devices outside of UHV for integrating with non-UHV processes, such as other chemistries and commercial semiconductor device processes.

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Quantum Transport Simulations for Si:P δ-layer Tunnel Junctions

International Conference on Simulation of Semiconductor Processes and Devices, SISPAD

Mendez Granado, Juan P.; Mamaluy, Denis M.; Gao, Xujiao G.; Misra, Shashank M.

We present an efficient self-consistent implementation of the Non-Equilibrium Green Function formalism, based on the Contact Block Reduction method for fast numerical efficiency, and the predictor-corrector approach, together with the Anderson mixing scheme, for the self-consistent solution of the Poisson and Schrödinger equations. Then, we apply this quantum transport framework to investigate 2D horizontal Si:P δ-layer Tunnel Junctions. We find that the potential barrier height varies with the tunnel gap width and the applied bias and that the sign of a single charge impurity in the tunnel gap plays an important role in the electrical current.

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Modeling and Assessment of Atomic Precision Advanced Manufacturing (APAM) Enabled Vertical Tunneling Field Effect Transistor

International Conference on Simulation of Semiconductor Processes and Devices, SISPAD

Gao, Xujiao G.; Mendez Granado, Juan P.; Lu, Tzu-Ming L.; Anderson, Evan M.; Campbell, DeAnna M.; Ivie, Jeffrey A.; Schmucker, Scott W.; Grine, Albert D.; Lu, Ping L.; Tracy, Lisa A.; Arghavani, Reza A.; Misra, Shashank M.

The atomic precision advanced manufacturing (APAM) enabled vertical tunneling field effect transistor (TFET) presents a new opportunity in microelectronics thanks to the use of ultra-high doping and atomically abrupt doping profiles. We present modeling and assessment of the APAM TFET using TCAD Charon simulation. First, we show, through a combination of simulation and experiment, that we can achieve good control of the gated channel on top of a phosphorus layer made using APAM, an essential part of the APAM TFET. Then, we present simulation results of a preliminary APAM TFET that predict transistor-like current-voltage response despite low device performance caused by using large geometry dimensions. Future device simulations will be needed to optimize geometry and doping to guide device design for achieving superior device performance.

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Ultradoping Boron on Si(100) via Solvothermal Chemistry**

Chemistry - A European Journal

Frederick, Esther F.; Campbell, Quinn C.; Kolesnichenko, Igor K.; Pena, Luis F.; Benavidez, Angelica; Anderson, Evan M.; Wheeler, David R.; Misra, Shashank M.

Ultradoping introduces unprecedented dopant levels into Si, which transforms its electronic behavior and enables its use as a next-generation electronic material. Commercialization of ultradoping is currently limited by gas-phase ultra-high vacuum requirements. Solvothermal chemistry is amenable to scale-up. However, an integral part of ultradoping is a direct chemical bond between dopants and Si, and solvothermal dopant-Si surface reactions are not well-developed. This work provides the first quantified demonstration of achieving ultradoping concentrations of boron (∼1e14 cm2) by using a solvothermal process. Surface characterizations indicate the catalyst cross-reacted, which led to multiple surface products and caused ambiguity in experimental confirmation of direct surface attachment. Density functional theory computations elucidate that the reaction results in direct B−Si surface bonds. This proof-of-principle work lays groundwork for emerging solvothermal ultradoping processes.

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Atomic-precision advanced manufacturing for Si quantum computing

MRS Bulletin

Bussmann, Ezra B.; Butera, Robert E.; Owen, James H.G.; Randall, John N.; Rinaldi, Steven R.; Baczewski, Andrew D.; Misra, Shashank M.

A materials synthesis method that we call atomic-precision advanced manufacturing (APAM), which is the only known route to tailor silicon nanoelectronics with full 3D atomic precision, is making an impact as a powerful prototyping tool for quantum computing. Quantum computing schemes using atomic (31P) spin qubits are compelling for future scale-up owing to long dephasing times, one- and two-qubit gates nearing high-fidelity thresholds for fault-tolerant quantum error correction, and emerging routes to manufacturing via proven Si foundry techniques. Multiqubit devices are challenging to fabricate by conventional means owing to tight interqubit pitches forced by short-range spin interactions, and APAM offers the required (Å-scale) precision to systematically investigate solutions. However, applying APAM to fabricate circuitry with increasing numbers of qubits will require significant technique development. Here, we provide a tutorial on APAM techniques and materials and highlight its impacts in quantum computing research. Finally, we describe challenges on the path to multiqubit architectures and opportunities for APAM technique development. Graphic Abstract: [Figure not available: see fulltext.]

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AlCl3-Dosed Si(100)-2 × 1: Adsorbates, Chlorinated Al Chains, and Incorporated Al

Journal of Physical Chemistry C

Radue, Matthew S.; Baek, Sungha; Farzaneh, Azadeh; Dwyer, K.J.; Campbell, Quinn C.; Baczewski, Andrew D.; Bussmann, Ezra B.; Wang, George T.; Mo, Yifei; Misra, Shashank M.; Butera, R.E.

The adsorption of AlCl3 on Si(100) and the effect of annealing the AlCl3-dosed substrate were studied to reveal key surface processes for the development of atomic-precision, acceptor-doping techniques. This investigation was performed via scanning tunneling microscopy (STM), X-ray photoelectron spectroscopy (XPS), and density functional theory (DFT) calculations. At room temperature, AlCl3 readily adsorbed to the Si substrate dimers and dissociated to form a variety of species. Annealing the AlCl3-dosed substrate at temperatures below 450 °C produced unique chlorinated aluminum chains (CACs) elongated along the Si(100) dimer row direction. An atomic model for the chains is proposed with supporting DFT calculations. Al was incorporated into the Si substrate upon annealing at 450 °C and above, and Cl desorption was observed for temperatures beyond 450 °C. Al-incorporated samples were encapsulated in Si and characterized by secondary ion mass spectrometry (SIMS) depth profiling to quantify the Al atom concentration, which was found to be in excess of 1020 cm-3 across a ∼2.7 nm-thick δ-doped region. The Al concentration achieved here and the processing parameters utilized promote AlCl3 as a viable gaseous precursor for novel acceptor-doped Si materials and devices for quantum computing.

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A Model for Atomic Precision p-Type Doping with Diborane on Si(100)-2×1

Journal of Physical Chemistry C

Campbell, Quinn C.; Ivie, Jeffrey A.; Bussmann, Ezra B.; Schmucker, Scott W.; Baczewski, Andrew D.; Misra, Shashank M.

Diborane (B2H6) is a promising molecular precursor for atomic precision p-type doping of silicon that has recently been experimentally demonstrated [ Škereň et al. Nat. Electron. 2020 ]. We use density functional theory (DFT) calculations to determine the reaction pathway for diborane dissociating into a species that will incorporate as electrically active substitutional boron after adsorbing onto the Si(100)-2×1 surface. Our calculations indicate that diborane must overcome an energy barrier to adsorb, explaining the experimentally observed low sticking coefficient (<1 × 10-4 at room temperature) and suggesting that heating can be used to increase the adsorption rate. Upon sticking, diborane has an ≈50% chance of splitting into two BH3 fragments versus merely losing hydrogen to form a dimer such as B2H4. As boron dimers are likely electrically inactive, whether this latter reaction occurs is shown to be predictive of the incorporation rate. The dissociation process proceeds with significant energy barriers, necessitating the use of high temperatures for incorporation. Using the barriers calculated from DFT, we parameterize a Kinetic Monte Carlo model that predicts the incorporation statistics of boron as a function of the initial depassivation geometry, dose, and anneal temperature. Our results suggest that the dimer nature of diborane inherently limits its doping density as an acceptor precursor and furthermore that heating the boron dimers to split before exposure to silicon can lead to poor selectivity on hydrogen and halogen resists. This suggests that, while diborane works as an atomic precision acceptor precursor, other non-dimerized acceptor precursors may lead to higher incorporation rates at lower temperatures.

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Photothermal alternative to device fabrication using atomic precision advanced manufacturing techniques

Journal of Micro/Nanopatterning, Materials and Metrology

Katzenmeyer, Aaron M.; Dmitrovic, Sanja; Baczewski, Andrew D.; Campbell, Quinn C.; Bussmann, Ezra B.; Lu, Tzu-Ming L.; Anderson, Evan M.; Schmucker, Scott W.; Ivie, Jeffrey A.; Campbell, DeAnna M.; Ward, Daniel R.; Scrymgeour, David S.; Wang, George T.; Misra, Shashank M.

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. Here, 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.

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Modeling assisted room temperature operation of atomic precision advanced manufacturing devices

International Conference on Simulation of Semiconductor Processes and Devices, SISPAD

Gao, Xujiao G.; Tracy, Lisa A.; Anderson, Evan M.; Campbell, DeAnna M.; Ivie, Jeffrey A.; Lu, Tzu-Ming L.; Mamaluy, Denis M.; Schmucker, Scott W.; Misra, Shashank M.

One big challenge of the emerging atomic precision advanced manufacturing (APAM) technology for microelectronics application is to realize APAM devices that operate at room temperature (RT). We demonstrate that semiclassical technology computer aided design (TCAD) device simulation tool can be employed to understand current leakage and improve APAM device design for RT operation. To establish the applicability of semiclassical simulation, we first show that a semiclassical impurity scattering model with the Fermi-Dirac statistics can explain the very low mobility in APAM devices quite well; we also show semiclassical TCAD reproduces measured sheet resistances when proper mobility values are used. We then apply semiclassical TCAD to simulate current leakage in realistic APAM wires. With insights from modeling, we were able to improve device design, fabricate Hall bars, and demonstrate RT operation for the very first time.

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Assessing atomically thin delta-doping of silicon using mid-infrared ellipsometry

Journal of Materials Research

Katzenmeyer, Aaron M.; Luk, Ting S.; Bussmann, Ezra B.; Young, Steve M.; Anderson, Evan M.; Marshall, Michael T.; Ohlhausen, J.A.; Kotula, Paul G.; Lu, Ping L.; Campbell, DeAnna M.; Lu, Tzu-Ming L.; Liu, Peter Q.; Ward, Daniel R.; Misra, Shashank M.

Hydrogen lithography has been used to template phosphine-based surface chemistry to fabricate atomic-scale devices, a process we abbreviate as atomic precision advanced manufacturing (APAM). Here, we use mid-infrared variable angle spectroscopic ellipsometry (IR-VASE) to characterize single-nanometer thickness phosphorus dopant layers (δ-layers) in silicon made using APAM compatible processes. A large Drude response is directly attributable to the δ-layer and can be used for nondestructive monitoring of the condition of the APAM layer when integrating additional processing steps. The carrier density and mobility extracted from our room temperature IR-VASE measurements are consistent with cryogenic magneto-transport measurements, showing that APAM δ-layers function at room temperature. Finally, the permittivity extracted from these measurements shows that the doping in the APAM δ-layers is so large that their low-frequency in-plane response is reminiscent of a silicide. However, there is no indication of a plasma resonance, likely due to reduced dimensionality and/or low scattering lifetime.

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Low thermal budget high-k/metal surface gate for buried donor-based devices

JPhys Materials

Anderson, Evan M.; Campbell, De A.; Maurer, Leon N.; Baczewski, Andrew D.; Marshall, Michael T.; Lu, Tzu-Ming L.; Lu, Ping L.; Tracy, Lisa A.; Schmucker, Scott W.; Ward, Daniel R.; Misra, Shashank M.

Atomic precision advanced manufacturing (APAM) offers creation of donor devices in an atomically thin layer doped beyond the solid solubility limit, enabling unique device physics. This presents an opportunity to use APAM as a pathfinding platform to investigate digital electronics at the atomic limit. Scaling to smaller transistors is increasingly difficult and expensive, necessitating the investigation of alternative fabrication paths that extend to the atomic scale. APAM donor devices can be created using a scanning tunneling microscope (STM). However, these devices are not currently compatible with industry standard fabrication processes. There exists a tradeoff between low thermal budget (LT) processes to limit dopant diffusion and high thermal budget (HT) processes to grow defect-free layers of epitaxial Si and gate oxide. To this end, we have developed an LT epitaxial Si cap and LT deposited Al2O3 gate oxide integrated with an atomically precise single-electron transistor (SET) that we use as an electrometer to characterize the quality of the gate stack. The surface-gated SET exhibits the expected Coulomb blockade behavior. However, the gate’s leverage over the SET is limited by defects in the layers above the SET, including interfaces between the Si and oxide, and structural and chemical defects in the Si cap. We propose a more sophisticated gate stack and process flow that is predicted to improve performance in future atomic precision devices.

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Photothermal alternative to device fabrication using atomic precision advanced manufacturing techniques

Proceedings of SPIE - The International Society for Optical Engineering

Katzenmeyer, Aaron M.; Dmitrovic, S.; Baczewski, Andrew D.; Bussmann, Ezra B.; Lu, Tzu-Ming L.; Anderson, Evan M.; Schmucker, S.W.; Ivie, J.A.; Campbell, DeAnna M.; Ward, D.R.; Wang, George T.; Misra, Shashank M.

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 sub-nanometer precision, typically for quantum physics demonstrations, and to dope silicon past the solid-solubility limit, with potential applications in microelectronics and plasmonics. However, this process, which we call atomic precision advanced manufacturing (APAM), currently lacks the throughput required to develop sophisticated applications because there is no proven scalable hydrogen lithography pathway. Here, we demonstrate and characterize an APAM device workflow where STM lithography has been replaced with photolithography. An ultraviolet laser is shown to locally heat silicon controllably above the temperature required for hydrogen depassivation. STM images indicate a narrow range of laser energy density where hydrogen has been depassivated, and the surface remains well-ordered. A model for photothermal heating of silicon predicts a local temperature which is consistent with atomic-scale STM images of the photo-patterned regions. Finally, a simple device made by exposing photo-depassivated silicon to phosphine is found to have a carrier density and mobility similar to that produced by similar devices patterned by STM.

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Designer quantum materials

Misra, Shashank M.; Ward, Daniel R.; Baczewski, Andrew D.; Campbell, Quinn C.; Schmucker, Scott W.; Mounce, Andrew M.; Tracy, Lisa A.; Lu, Tzu-Ming L.; Marshall, Michael T.; Campbell, DeAnna M.

Quantum materials have long promised to revolutionize everything from energy transmission (high temperature superconductors) to both quantum and classical information systems (topological materials). However, their discovery and application has proceeded in an Edisonian fashion due to both an incomplete theoretical understanding and the difficulty of growing and purifying new materials. This project leverages Sandia's unique atomic precision advanced manufacturing (APAM) capability to design small-scale tunable arrays (designer materials) made of donors in silicon. Their low-energy electronic behavior can mimic quantum materials, and can be tuned by changing the fabrication parameters for the array, thereby enabling the discovery of materials systems which can't yet be synthesized. In this report, we detail three key advances we have made towards development of designer quantum materials. First are advances both in APAM technique and underlying mechanisms required to realize high-yielding donor arrays. Second is the first-ever observation of distinct phases in this material system, manifest in disordered 2D sheets of donors. Finally are advances in modeling the electronic structure of donor clusters and regular structures incorporating them, critical to understanding whether an array is expected to show interesting physics. Combined, these establish the baseline knowledge required to manifest the strongly-correlated phases of the Mott-Hubbard model in donor arrays, the first step to deploying APAM donor arrays as analogues of quantum materials.

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Scanning microwave impedance microscopy (sMIM) in electronic and quantum materials

NanoScience and Technology

Rubin, Kurt A.; Yang, Yongliang; Amster, Oskar; Scrymgeour, David S.; Misra, Shashank M.

Scanning Microwave Impedance Microscopy (sMIM) is a sensitive electrical measurement technique which can characterize local static and temporal variations of electrical permittivity, and conductivity of materials and devices as well as for failure analysis. It is being used to characterize dielectrics, semiconductors and their doping response, and metals. Measurements can be made at room temperature down to cryogenic temperatures where quantum effects become important. Leveraging near-field electrical interactions between a probe and the sample, sMIM can measure and image electrical properties and operation at the nanoscale to micron scale by incorporation into an atomic force microscope. sMIM is being applied to a wide range of industrial and scientific applications to improve fundamental and functional understanding and operational performance of advanced, exploratory and quantum electronic devices and materials and their fabrication.

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DEAL annual report

Misra, Shashank M.

The digital electronics at the atomic limit (DEAL) project seeks to leverage Sandia's atomic-precision fabrication capability to realize the theorized orders-of-magnitude improvement in operating voltage for tunnel field effect transistors (TFETs) compared to CMOS. Not only are low-power digital circuits a critical element of many national security systems (e.g. satellites), TFETs can perform circuit functions inaccessible to CMOS (e.g. polymorphism).

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117 Results
117 Results