Adsorption and abstraction reactions of HCl on a single Si(100) dangling bond

Li, Hong-Dao; Chang, Chan-Yuen; Chien, Ling-Ying; Chang, Shang‐Hung; Chiang, T.‐C.; Lin, Deng−Sung

doi:10.1103/physrevb.83.075403

Cited by 11 publications

(11 citation statements)

References 28 publications

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“…18,19 These structured dangling bonds can be promising candidates for charge qubits 20 and can also be used for chemisorption of molecules such as I 2 21 and HCl. 22 Controllable manipulation of adatoms, molecules, nanoclusters, and dopants has already been achieved on/in surfaces of metals, semiconductors, and insulators. 5,23À29 However, while controlled lateral manipulation of individual vacancies across a surface lattice has been predicted theoretically to be possible using an atomic force microscope, 30 it has not been achieved experimentally.…”

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confidence: 99%

Lateral Manipulation of Atomic Vacancies in Ultrathin Insulating Films

Chen

Schouteden

et al. 2015

ACS Nano

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During the last 20 years, using scanning tunneling microscopy (STM) and atomic force microscopy, scientists have successfully achieved vertical and lateral repositioning of individual atoms on and in different types of surfaces. Such atom manipulation allows the bottom-up assembly of novel nanostructures that can otherwise not be fabricated. It is therefore surprising that controlled repositioning of virtual atoms, i.e., atomic vacancies, across atomic lattices has not yet been achieved experimentally. Here we use STM at liquid helium temperature (4.5 K) to create individual Cl vacancies and subsequently to laterally manipulate them across the surface of ultrathin sodium chloride films. This allows monitoring the interactions between two neighboring vacancies with different separations. Our findings are corroborated by density functional theory calculations and STM image simulations. The lateral manipulation of atomic vacancies opens up a new playground for the investigation of fundamental physical properties of vacancy nanostructures of any size and shape and their coupling with the supporting substrate, and of the interaction of various deposits with charged vacancies.

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confidence: 99%

Lateral Manipulation of Atomic Vacancies in Ultrathin Insulating Films

Chen

Schouteden

et al. 2015

ACS Nano

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“…H-passivated Si(100) has been the standard substrate for atomically precise device fabrication due in large part to its ease of lithographic patterning and the use of PH 3 and, more recently, B 2 H 6 and AsH 3 for doping reactions. , H-based dopant precursors experience no driving force to react with the H passivation layer. In contrast, the use of BCl 3 presents a possible pathway for reaction with the H passivation layer through abstraction , or nucleophilic attack of the Cl on the H, thereby compromising the selectivity required for device fabrication with good pattern fidelity.…”

Section: Results and Discussionmentioning

confidence: 99%

“…9,38 Hbased dopant precursors experience no driving force to react with the H passivation layer. In contrast, the use of BCl 3 presents a possible pathway for reaction with the H passivation layer through abstraction 37,39 or nucleophilic attack of the Cl on the H, thereby compromising the selectivity required for device fabrication with good pattern fidelity.…”

Section: ■ Experimental Methodsmentioning

confidence: 99%

B-Doped δ-Layers and Nanowires from Area-Selective Deposition of BCl₃ on Si(100)

Dwyer

Baek

Farzaneh

et al. 2021

ACS Appl. Mater. Interfaces

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Atomically precise, δ-doped structures forming electronic devices in Si have been routinely fabricated in recent years by using depassivation lithography in a scanning tunneling microscope (STM). While H-based precursor/monatomic resist chemistries for incorporation of donor atoms have dominated these efforts, the use of halogen-based chemistries offers a promising path toward atomic-scale manufacturing of acceptor-based devices. Here, B-doped δ-layers were fabricated in Si(100) by using BCl 3 as an acceptor dopant precursor in ultrahigh vacuum. Additionally, we demonstrate compatibility of BCl 3 with both H and Cl monatomic resists to achieve area-selective deposition on Si. In comparison to bare Si, BCl 3 adsorption selectivity ratios for H-and Cl-passivated Si were determined by secondary ion mass spectrometry depth profiling (SIMS) to be 310(10):1 and 1529(5):1, respectively. STM imaging revealed that BCl 3 adsorbed readily on bare Si at room temperature, with SIMS measurements indicating a peak B concentration greater than 1.2(1) × 10 21 cm −3 with a total areal dose of 1.85(1) × 10 14 cm −2 resulting from a 30 langmuir BCl 3 dose at 150 °C. In addition, SIMS showed a δ-layer thickness of ∼0.5 nm. Hall bar measurements of a similar sample were performed at 3.0 K, revealing a sheet resistance of ρ □ = 1.9099(4) kΩ □ −1 , a hole carrier concentration of p = 1.90(2) × 10 14 cm −2 , and a hole mobility of μ = 38.0(4) cm 2 V −1 s −1 without performing an incorporation anneal. Finally, 15 nm wide B δ-doped nanowires were fabricated from BCl 3 and were found to exhibit ohmic conduction. This validates the use of BCl 3 as a dopant precursor for atomicprecision fabrication of acceptor-doped devices in Si and enables development of simultaneous n-and p-type doped bipolar devices.

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“…Earlier experiments of HCl and HBr on Si(100) were performedin contrast to the present workat saturation coverage 21−24 or on a hydrogenated surface. 25 While dissociative attachment was found to be a major pathway, previous authors found evidence of the abstraction of single atoms, H or Cl, by the surface. Adsorbate−adsorbate interactions were investigated to explain the pattern of longrange ordering of Cl at high coverage.…”

Section: Introductionmentioning

confidence: 98%

Charge-Transfer in Silicon Governs the Pattern of Dissociative Attachment of Hydrogen Halides: HCl, HBr, and HI

et al. 2016

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The dissociative attachment of hydrogen halides, HCl, HBr, and HI, on Si(100) was studied by scanning tunneling microscopy, and modeled by molecular dynamics computations based on density functional theory. The relative yields of on-dimer (OD), inter-dimer (ID), and inter-row (IR) products, reported here for the first time, were unaltered by temperature change, indicative of barrier-free reaction. Interdimer reaction was found experimentally to be overwhelmingly the favored reaction path at all temperatures, 175−300 K. This is a preference that theory accounts for by a combination of kinematics favoring the initial approach of H, and subsequent charge-displacement directing the halogen atom to an inter-dimer site. Molecular dynamics, with statistical sampling of the initial collision-geometry at the surface, showed that the light H-atom invariably was the first to engage with the surface, forming H−Si. This bond-formation resulted in directional charge-transfer to a neighboring Si dimer-pair of the same dimer-row. As a consequence this neighboring Si became attractive to the incoming electrophilic halogen-atom, accounting for the observed strong preference for the inter-dimer outcome.

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Adsorption and abstraction reactions of HCl on a single Si(100) dangling bond

Cited by 11 publications

References 28 publications

Lateral Manipulation of Atomic Vacancies in Ultrathin Insulating Films

Lateral Manipulation of Atomic Vacancies in Ultrathin Insulating Films

B-Doped δ-Layers and Nanowires from Area-Selective Deposition of BCl₃ on Si(100)

Charge-Transfer in Silicon Governs the Pattern of Dissociative Attachment of Hydrogen Halides: HCl, HBr, and HI

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Adsorption and abstraction reactions of HCl on a single Si(100) dangling bond

Cited by 11 publications

References 28 publications

Lateral Manipulation of Atomic Vacancies in Ultrathin Insulating Films

Lateral Manipulation of Atomic Vacancies in Ultrathin Insulating Films

B-Doped δ-Layers and Nanowires from Area-Selective Deposition of BCl3 on Si(100)

Charge-Transfer in Silicon Governs the Pattern of Dissociative Attachment of Hydrogen Halides: HCl, HBr, and HI

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B-Doped δ-Layers and Nanowires from Area-Selective Deposition of BCl₃ on Si(100)