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Selective amorphization of SiGe in Si/SiGe nanostructures via high energy Si+ implant

Journal of Applied Physics

Turner, Emily M.; Campbell, Quinn C.; Avci, Ibrahim A.; Weber, William J.; Lu, Ping L.; Wang, George T.; Jones, Kevin S.

The selective amorphization of SiGe in Si/SiGe nanostructures via a 1 MeV Si + implant was investigated, resulting in single-crystal Si nanowires (NWs) and quantum dots (QDs) encapsulated in amorphous SiGe fins and pillars, respectively. The Si NWs and QDs are formed during high-temperature dry oxidation of single-crystal Si/SiGe heterostructure fins and pillars, during which Ge diffuses along the nanostructure sidewalls and encapsulates the Si layers. The fins and pillars were then subjected to a 3 × 10 15  ions/cm 2 1 MeV Si + implant, resulting in the amorphization of SiGe, while leaving the encapsulated Si crystalline for larger, 65-nm wide NWs and QDs. Interestingly, the 26-nm diameter Si QDs amorphize, while the 28-nm wide NWs remain crystalline during the same high energy ion implant. This result suggests that the Si/SiGe pillars have a lower threshold for Si-induced amorphization compared to their Si/SiGe fin counterparts. However, Monte Carlo simulations of ion implantation into the Si/SiGe nanostructures reveal similar predicted levels of displacements per cm 3 . Molecular dynamics simulations suggest that the total stress magnitude in Si QDs encapsulated in crystalline SiGe is higher than the total stress magnitude in Si NWs, which may lead to greater crystalline instability in the QDs during ion implant. The potential lower amorphization threshold of QDs compared to NWs is of special importance to applications that require robust QD devices in a variety of radiation environments.

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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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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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Controlled Formation of Stacked Si Quantum Dots in Vertical SiGe Nanowires

Nano Letters

Turner, Emily M.; Campbell, Quinn C.; Pizarro, Joaquín; Yang, Hongbin; Sapkota, Keshab R.; Lu, Ping L.; Baczewski, Andrew D.; Wang, George T.; Jones, Kevin S.

We demonstrate the ability to fabricate vertically stacked Si quantum dots (QDs) within SiGe nanowires with QD diameters down to 2 nm. These QDs are formed during high-temperature dry oxidation of Si/SiGe heterostructure pillars, during which Ge diffuses along the pillars' sidewalls and encapsulates the Si layers. Continued oxidation results in QDs with sizes dependent on oxidation time. The formation of a Ge-rich shell that encapsulates the Si QDs is observed, a configuration which is confirmed to be thermodynamically favorable with molecular dynamics and density functional theory. The type-II band alignment of the Si dot/SiGe pillar suggests that charge trapping on the Si QDs is possible, and electron energy loss spectra show that a conduction band offset of at least 200 meV is maintained for even the smallest Si QDs. Our approach is compatible with current Si-based manufacturing processes, offering a new avenue for realizing Si QD devices.

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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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A New Route to Quantum-Scale Structures through a Novel Enhanced Germanium Diffusion Mechanism

Wang, George T.; Lu, Ping L.; Sapkota, Keshab R.; Baczewski, Andrew D.; Campbell, Quinn C.; Schultz, Peter A.; Jones, Kevin S.; Turner, Emily M.; Sharrock, Chappel J.; Law, Mark E.; Yang, Hongbin Y.

This project sought to develop a fundamental understanding of the mechanisms underlying a newly observed enhanced germanium (Ge) diffusion process in silicon germanium (SiGe) semiconductor nanostructures during thermal oxidation. Using a combination of oxidationdiffusion experiments, high resolution imaging, and theoretical modeling, a model for the enhanced Ge diffusion mechanism was proposed. Additionally, a nanofabrication approach utilizing this enhanced Ge diffusion mechanism was shown to be applicable to arbitrary 3D shapes, leading to the fabrication of stacked silicon quantum dots embedded in SiGe nanopillars. A new wet etch-based method for preparing 3D nanostructures for highresolution imaging free of obscuring material or damage was also developed. These results enable a new method for the controlled and scalable fabrication of on-chip silicon nanostructures with sub-10 nm dimensions needed for next generation microelectronics, including low energy electronics, quantum computing, sensors, and integrated photonics.

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FAIR DEAL Grand Challenge Overview

Allemang, Christopher R.; Anderson, Evan M.; Baczewski, Andrew D.; Bussmann, Ezra B.; Butera, Robert E.; Campbell, DeAnna M.; Campbell, Quinn C.; Carr, Stephen M.; Frederick, Esther F.; Gamache, Phillip G.; Gao, Xujiao G.; Grine, Albert D.; Gunter, Mathew M.; Halsey, Connor H.; Ivie, Jeffrey A.; Katzenmeyer, Aaron M.; Leenheer, Andrew J.; Lepkowski, William L.; Lu, Tzu-Ming L.; Mamaluy, Denis M.; Mendez Granado, Juan P.; Pena, Luis F.; Schmucker, Scott W.; Scrymgeour, David S.; Tracy, Lisa A.; Wang, George T.; Ward, Dan W.; Young, Steve M.

While it is likely practically a bad idea to shrink a transistor to the size of an atom, there is no arguing that it would be fantastic to have atomic-scale control over every aspect of a transistor – a kind of crystal ball to understand and evaluate new ideas. This project showed that it was possible to take a niche technique used to place dopants in silicon with atomic precision and apply it broadly to study opportunities and limitations in microelectronics. In addition, it laid the foundation to attaining atomic-scale control in semiconductor manufacturing more broadly.

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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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Results 1–25 of 26
Results 1–25 of 26