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

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

doi:10.1116/5.0075467

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

Journal Article · Thu Mar 03 00:00:00 EST 2022 · AVS Quantum Science

DOI:https://doi.org/10.1116/5.0075467· OSTI ID:1870448

^[1]; Baczewski, Andrew D. ^[1];

^[2]; Misra, Shashank ^[1]

Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Univ. of Maryland, College Park, MD (United States)

We report that 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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Research Organization:: Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: NA0003525; 213017

OSTI ID:: 1870448

Alternate ID(s):: OSTI ID: 1847198

Report Number(s):: SAND2022-3603J; 704496; TRN: US2306540

Journal Information:: AVS Quantum Science, Vol. 4, Issue 1; ISSN 2639-0213

Publisher:: American Institute of Physics (AIP) - American Vacuum SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (76)

Low thermal budget high-k/metal surface gate for buried donor-based devices Anderson, Evan M.; Campbell, DeAnna M.; Maurer, Leon N. Journal of Physics: Materials, Vol. 3, Issue 3 https://doi.org/10.1088/2515-7639/ab953b	journal	June 2020
Hole spin echo envelope modulations Philippopoulos, Pericles; Chesi, Stefano; Salfi, Joe Physical Review B, Vol. 100, Issue 12 https://doi.org/10.1103/PhysRevB.100.125402	journal	September 2019
Valley interference and spin exchange at the atomic scale in silicon Voisin, B.; Bocquel, J.; Tankasala, A. Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-19835-1	journal	November 2020
Strongly Nonlinear Superconducting Silicon Resonators Bonnet, P.; Chiodi, F.; Flanigan, D. Physical Review Applied, Vol. 17, Issue 3 https://doi.org/10.1103/PhysRevApplied.17.034057	journal	March 2022
Theory of two boron neutral pair defects in silicon Tarnow, E. Journal of Physics: Condensed Matter, Vol. 4, Issue 24 https://doi.org/10.1088/0953-8984/4/24/010	journal	June 1992
Quantum simulation of the Hubbard model with dopant atoms in silicon Salfi, J.; Mol, J. A.; Rahman, R. Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms11342	journal	April 2016
Linear combination of atomic orbitals model for deterministically placed acceptor arrays in silicon Zhu, Jianhua; Wu, Wei; Fisher, Andrew J. Physical Review B, Vol. 101, Issue 8 https://doi.org/10.1103/PhysRevB.101.085303	journal	February 2020
Reaction paths of phosphine dissociation on silicon (001) Warschkow, O.; Curson, N. J.; Schofield, S. R. The Journal of Chemical Physics, Vol. 144, Issue 1 https://doi.org/10.1063/1.4939124	journal	January 2016
Thermal dissociation and desorption of $P H_{3}$ on Si(001): A reinterpretation of spectroscopic data Wilson, H. F.; Warschkow, O.; Marks, N. A. Physical Review B, Vol. 74, Issue 19 https://doi.org/10.1103/PhysRevB.74.195310	journal	November 2006
Atomically Precise Placement of Single Dopants in Si Schofield, S. R.; Curson, N. J.; Simmons, M. Y. Physical Review Letters, Vol. 91, Issue 13 https://doi.org/10.1103/PhysRevLett.91.136104	journal	September 2003
Effect of local strain on single acceptors in Si Calvet, L. E.; Wheeler, R. G.; Reed, M. A. Physical Review B, Vol. 76, Issue 3 https://doi.org/10.1103/PhysRevB.76.035319	journal	July 2007
A single-atom transistor Fuechsle, Martin; Miwa, Jill A.; Mahapatra, Suddhasatta Nature Nanotechnology, Vol. 7, Issue 4 https://doi.org/10.1038/nnano.2012.21	journal	February 2012
Isotope effect on electron paramagnetic resonance of boron acceptors in silicon Stegner, A. R.; Tezuka, H.; Andlauer, T. Physical Review B, Vol. 82, Issue 11 https://doi.org/10.1103/PhysRevB.82.115213	journal	September 2010
Phosphine Dissociation on the Si(001) Surface Wilson, H. F.; Warschkow, O.; Marks, N. A. Physical Review Letters, Vol. 93, Issue 22 https://doi.org/10.1103/PhysRevLett.93.226102	journal	November 2004
Readout and control of the spin-orbit states of two coupled acceptor atoms in a silicon transistor van der Heijden, Joost; Kobayashi, Takashi; House, Matthew G. Science Advances, Vol. 4, Issue 12 https://doi.org/10.1126/sciadv.aat9199	journal	December 2018
Quadrupolar interactions between acceptor pairs in $p$ -doped semiconductors Durst, Adam C.; Yang-Mejia, Genesis; Bhatt, R. N. Physical Review B, Vol. 101, Issue 3 https://doi.org/10.1103/PhysRevB.101.035202	journal	January 2020
Al-alkyls as acceptor dopant precursors for atomic-scale devices Owen, J. H. G.; Campbell, Q.; Santini, R. Journal of Physics: Condensed Matter, Vol. 33, Issue 46 https://doi.org/10.1088/1361-648X/ac1ddf	journal	September 2021
Observation of the Linear Stark Effect in a Single Acceptor in Si Calvet, L. E.; Wheeler, R. G.; Reed, M. A. Physical Review Letters, Vol. 98, Issue 9 https://doi.org/10.1103/PhysRevLett.98.096805	journal	March 2007
Engineering long spin coherence times of spin–orbit qubits in silicon Kobayashi, Takashi; Salfi, Joseph; Chua, Cassandra Nature Materials, Vol. 20, Issue 1 https://doi.org/10.1038/s41563-020-0743-3	journal	July 2020
Interface effects on acceptor qubits in silicon and germanium Abadillo-Uriel, J. C.; Calderón, M. J. Nanotechnology, Vol. 27, Issue 2 https://doi.org/10.1088/0957-4484/27/2/024003	journal	November 2015
Atomic-Scale Patterning of Arsenic in Silicon by Scanning Tunneling Microscopy Stock, Taylor J. Z.; Warschkow, Oliver; Constantinou, Procopios C. ACS Nano, Vol. 14, Issue 3 https://doi.org/10.1021/acsnano.9b08943	journal	March 2020
Spin read-out in atomic qubits in an all-epitaxial three-dimensional transistor Koch, Matthias; Keizer, Joris G.; Pakkiam, Prasanna Nature Nanotechnology, Vol. 14, Issue 2 https://doi.org/10.1038/s41565-018-0338-1	journal	January 2019
Toward Atomic-Scale Device Fabrication in Silicon Using Scanning Probe Microscopy Ruess, Frank J.; Oberbeck, Lars; Simmons, Michelle Y. Nano Letters, Vol. 4, Issue 10 https://doi.org/10.1021/nl048808v	journal	October 2004
KMCLib: A general framework for lattice kinetic Monte Carlo (KMC) simulations Leetmaa, Mikael; Skorodumova, Natalia V. Computer Physics Communications, Vol. 185, Issue 9 https://doi.org/10.1016/j.cpc.2014.04.017	journal	September 2014
Single-Shot Spin Readout in Semiconductors Near the Shot-Noise Sensitivity Limit Keith, D.; House, M. G.; Donnelly, M. B. Physical Review X, Vol. 9, Issue 4 https://doi.org/10.1103/PhysRevX.9.041003	journal	October 2019
Photothermal alternative to device fabrication using atomic precision advanced manufacturing techniques Katzenmeyer, Aaron M.; Dmitrovic, Sanja; Baczewski, Andrew D. Journal of Micro/Nanopatterning, Materials, and Metrology, Vol. 20, Issue 01 https://doi.org/10.1117/1.JMM.20.1.014901	journal	January 2021
Bipolar device fabrication using a scanning tunnelling microscope Škereň, Tomáš; Köster, Sigrun A.; Douhard, Bastien Nature Electronics, Vol. 3, Issue 9 https://doi.org/10.1038/s41928-020-0445-5	journal	July 2020
B-Doped δ-Layers and Nanowires from Area-Selective Deposition of BCl ₃ on Si(100) Dwyer, Kevin J.; Baek, Sungha; Farzaneh, Azadeh ACS Applied Materials & Interfaces, Vol. 13, Issue 34 https://doi.org/10.1021/acsami.1c10616	journal	August 2021
Impact of Incorporation Kinetics on Device Fabrication with Atomic Precision Ivie, Jeffrey A.; Campbell, Quinn; Koepke, Justin C. Physical Review Applied, Vol. 16, Issue 5 https://doi.org/10.1103/PhysRevApplied.16.054037	journal	November 2021
Spectroscopy of few-electron single-crystal silicon quantum dots Fuechsle, Martin; Mahapatra, S.; Zwanenburg, F. A. Nature Nanotechnology, Vol. 5, Issue 7 https://doi.org/10.1038/nnano.2010.95	journal	May 2010
Charge-Insensitive Single-Atom Spin-Orbit Qubit in Silicon Salfi, Joe; Mol, Jan A.; Culcer, Dimitrie Physical Review Letters, Vol. 116, Issue 24 https://doi.org/10.1103/PhysRevLett.116.246801	journal	June 2016
Silicon superconducting quantum interference device Duvauchelle, J. E.; Francheteau, A.; Marcenat, C. Applied Physics Letters, Vol. 107, Issue 7 https://doi.org/10.1063/1.4928660	journal	August 2015
Isotopic compositions of the elements 2013 (IUPAC Technical Report) Meija, Juris; Coplen, Tyler B.; Berglund, Michael Pure and Applied Chemistry, Vol. 88, Issue 3 https://doi.org/10.1515/pac-2015-0503	journal	March 2016
Quantum computing with acceptor spins in silicon Salfi, Joe; Tong, Mengyang; Rogge, Sven Nanotechnology, Vol. 27, Issue 24 https://doi.org/10.1088/0957-4484/27/24/244001	journal	May 2016
Ab initio pseudopotential calculations of B diffusion and pairing in Si Zhu, Jing; dela Rubia, Tomas Diaz; Yang, L. H. Physical Review B, Vol. 54, Issue 7 https://doi.org/10.1103/PhysRevB.54.4741	journal	August 1996
Exploiting a Single‐Crystal Environment to Minimize the Charge Noise on Qubits in Silicon Kranz, Ludwik; Gorman, Samuel Keith; Thorgrimsson, Brandur Advanced Materials, Vol. 32, Issue 40 https://doi.org/10.1002/adma.202003361	journal	August 2020
Atom‐by‐Atom Fabrication of Single and Few Dopant Quantum Devices Wyrick, Jonathan; Wang, Xiqiao; Kashid, Ranjit V. Advanced Functional Materials, Vol. 29, Issue 52 https://doi.org/10.1002/adfm.201903475	journal	August 2019
Topological phases of a dimerized Fermi–Hubbard model for semiconductor nano-lattices Le, Nguyen H.; Fisher, Andrew J.; Curson, Neil J. npj Quantum Information, Vol. 6, Issue 1 https://doi.org/10.1038/s41534-020-0253-9	journal	February 2020
AlCl ₃ -Dosed Si(100)-2 × 1: Adsorbates, Chlorinated Al Chains, and Incorporated Al Radue, Matthew S.; Baek, Sungha; Farzaneh, Azadeh The Journal of Physical Chemistry C, Vol. 125, Issue 21 https://doi.org/10.1021/acs.jpcc.1c00691	journal	May 2021
Roadmap on quantum nanotechnologies Laucht, Arne; Hohls, Frank; Ubbelohde, Niels Nanotechnology, Vol. 32, Issue 16 https://doi.org/10.1088/1361-6528/abb333	journal	February 2021
Nanoscale patterning and oxidation of H‐passivated Si(100)‐2×1 surfaces with an ultrahigh vacuum scanning tunneling microscope Lyding, J. W.; Shen, T. ‐C.; Hubacek, J. S. Applied Physics Letters, Vol. 64, Issue 15 https://doi.org/10.1063/1.111722	journal	April 1994
A two-qubit gate between phosphorus donor electrons in silicon He, Y.; Gorman, S. K.; Keith, D. Nature, Vol. 571, Issue 7765 https://doi.org/10.1038/s41586-019-1381-2	journal	July 2019
Atomic-Scale Desorption Through Electronic and Vibrational Excitation Mechanisms Shen, T. -C.; Wang, C.; Abeln, G. C. Science, Vol. 268, Issue 5217 https://doi.org/10.1126/science.268.5217.1590	journal	June 1995
A Model for Atomic Precision p-Type Doping with Diborane on Si(100)-2×1 Campbell, Quinn; Ivie, Jeffrey A.; Bussmann, Ezra The Journal of Physical Chemistry C, Vol. 125, Issue 1 https://doi.org/10.1021/acs.jpcc.0c08919	journal	January 2021
A surface code quantum computer in silicon Hill, Charles D.; Peretz, Eldad; Hile, Samuel J. Science Advances, Vol. 1, Issue 9 https://doi.org/10.1126/sciadv.1500707	journal	October 2015
A new algorithm for Monte Carlo simulation of Ising spin systems Bortz, A. B.; Kalos, M. H.; Lebowitz, J. L. Journal of Computational Physics, Vol. 17, Issue 1 https://doi.org/10.1016/0021-9991(75)90060-1	journal	January 1975
Exchange in Silicon-Based Quantum Computer Architecture Koiller, Belita; Hu, Xuedong; Das Sarma, S. Physical Review Letters, Vol. 88, Issue 2 https://doi.org/10.1103/PhysRevLett.88.027903	journal	December 2001
Interplay between quantum confinement and dielectric mismatch for ultrashallow dopants Mol, J. A.; Salfi, J.; Miwa, J. A. Physical Review B, Vol. 87, Issue 24 https://doi.org/10.1103/PhysRevB.87.245417	journal	June 2013
Spin readout and addressability of phosphorus-donor clusters in silicon Büch, H.; Mahapatra, S.; Rahman, R. Nature Communications, Vol. 4, Issue 1 https://doi.org/10.1038/ncomms3017	journal	June 2013
Atomic-scale control of tunneling in donor-based devices Wang, Xiqiao; Wyrick, Jonathan; Kashid, Ranjit V. Communications Physics, Vol. 3, Issue 1 https://doi.org/10.1038/s42005-020-0343-1	journal	May 2020
Atomically engineered electron spin lifetimes of 30 s in silicon Watson, Thomas F.; Weber, Bent; Hsueh, Yu-Ling Science Advances, Vol. 3, Issue 3 https://doi.org/10.1126/sciadv.1602811	journal	March 2017
STM-Induced Desorption and Lithographic Patterning of Cl–Si(100)-(2 × 1) Dwyer, K. J.; Dreyer, Michael; Butera, R. E. The Journal of Physical Chemistry A, Vol. 123, Issue 50 https://doi.org/10.1021/acs.jpca.9b07127	journal	November 2019
Spatially resolving valley quantum interference of a donor in silicon Salfi, J.; Mol, J. A.; Rahman, R. Nature Materials, Vol. 13, Issue 6 https://doi.org/10.1038/nmat3941	journal	April 2014
Addressable electron spin resonance using donors and donor molecules in silicon Hile, Samuel J.; Fricke, Lukas; House, Matthew G. Science Advances, Vol. 4, Issue 7 https://doi.org/10.1126/sciadv.aaq1459	journal	July 2018
Atomic-precision advanced manufacturing for Si quantum computing Bussmann, Ezra; Butera, Robert E.; Owen, James H. G. MRS Bulletin, Vol. 46, Issue 7 https://doi.org/10.1557/s43577-021-00139-8	journal	July 2021
Probing the Spin States of a Single Acceptor Atom van der Heijden, Joost; Salfi, Joe; Mol, Jan A. Nano Letters, Vol. 14, Issue 3 https://doi.org/10.1021/nl4047015	journal	February 2014
First-Principle Study of Phosphine Adsorption on Si(001)-2 × 1–Cl Pavlova, Tatiana V.; Zhidomirov, Georgy M.; Eltsov, Konstantin N. The Journal of Physical Chemistry C, Vol. 122, Issue 3 https://doi.org/10.1021/acs.jpcc.7b11519	journal	January 2018
Implantation and transient boron diffusion: the role of the silicon self-interstitial Stolk, P. A.; Gossmann, H. -J.; Eaglesham, D. J. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 96, Issue 1-2 https://doi.org/10.1016/0168-583X(94)00481-1	journal	March 1995
Multihole models for deterministically placed acceptor arrays in silicon Zhu, Jianhua; Wu, Wei; Fisher, Andrew J. Physical Review B, Vol. 104, Issue 12 https://doi.org/10.1103/PhysRevB.104.125415	journal	September 2021
Adequacy of Si:P chains as Fermi–Hubbard simulators Dusko, Amintor; Delgado, Alain; Saraiva, André npj Quantum Information, Vol. 4, Issue 1 https://doi.org/10.1038/s41534-017-0051-1	journal	January 2018
Reaction of BCl3 with H- and Cl-terminated Si(1 0 0) as a pathway for selective, monolayer doping through wet chemistry Silva-Quinones, Dhamelyz; He, Chuan; Butera, Robert E. Applied Surface Science, Vol. 533 https://doi.org/10.1016/j.apsusc.2020.146907	journal	December 2020
Entanglement control and magic angles for acceptor qubits in Si Abadillo-Uriel, J. C.; Salfi, Joe; Hu, Xuedong Applied Physics Letters, Vol. 113, Issue 1 https://doi.org/10.1063/1.5036521	journal	July 2018
High-temperature infrared and Raman spectra of aluminium chloride dimer and monomer in the vapour phase Tomita, T.; Sjøgren, C. E.; Klaeboe, P. Journal of Raman Spectroscopy, Vol. 14, Issue 6 https://doi.org/10.1002/jrs.1250140611	journal	December 1983
Atomic precision lithography on Si Randall, J. N.; Lyding, J. W.; Schmucker, S. Journal of Vacuum Science & Technology B: Microelectronics and Nanometer Structures, Vol. 27, Issue 6 https://doi.org/10.1116/1.3237096	journal	January 2009
A general method for numerically simulating the stochastic time evolution of coupled chemical reactions Gillespie, Daniel T. Journal of Computational Physics, Vol. 22, Issue 4 https://doi.org/10.1016/0021-9991(76)90041-3	journal	December 1976
Bottom-up superconducting and Josephson junction devices inside a group-IV semiconductor Shim, Yun-Pil; Tahan, Charles Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms5225	journal	July 2014
Phosphine adsorption and dissociation on the Si(001) surface: An ab initio survey of structures Warschkow, O.; Wilson, H. F.; Marks, N. A. Physical Review B, Vol. 72, Issue 12 https://doi.org/10.1103/PhysRevB.72.125328	journal	September 2005
Extended Hubbard model for mesoscopic transport in donor arrays in silicon Le, Nguyen H.; Fisher, Andrew J.; Ginossar, Eran Physical Review B, Vol. 96, Issue 24 https://doi.org/10.1103/PhysRevB.96.245406	journal	December 2017
Barriers for hydrogen atom diffusion on the Si(100)‐2×1 surface Nachtigall, P.; Jordan, K. D. The Journal of Chemical Physics, Vol. 102, Issue 20 https://doi.org/10.1063/1.468954	journal	May 1995
Valley Filtering in Spatial Maps of Coupling between Silicon Donors and Quantum Dots Salfi, J.; Voisin, B.; Tankasala, A. Physical Review X, Vol. 8, Issue 3 https://doi.org/10.1103/PhysRevX.8.031049	journal	August 2018
Über die Reaktionsgeschwindigkeit bei der Inversion von Rohrzucker durch Säuren Arrhenius, Svante Zeitschrift für Physikalische Chemie, Vol. 4U, Issue 1 https://doi.org/10.1515/zpch-1889-0416	journal	January 1889
Quantum Simulators: Architectures and Opportunities Altman, Ehud; Brown, Kenneth R.; Carleo, Giuseppe PRX Quantum, Vol. 2, Issue 1 https://doi.org/10.1103/PRXQuantum.2.017003	journal	February 2021
Superconductivity in doped cubic silicon Bustarret, E.; Marcenat, C.; Achatz, P. Nature, Vol. 444, Issue 7118 https://doi.org/10.1038/nature05340	journal	November 2006
Coherent electrical control of a single high-spin nucleus in silicon Asaad, Serwan; Mourik, Vincent; Joecker, Benjamin Nature, Vol. 579, Issue 7798 https://doi.org/10.1038/s41586-020-2057-7	journal	March 2020
Reactivity of the Si(100)-2 × 1-Cl surface with respect to PH ₃ , PCl ₃ , and BCl ₃ : comparison with PH ₃ on Si(100)-2 × 1-H Pavlova, T. V.; Eltsov, K. N. Journal of Physics: Condensed Matter, Vol. 33, Issue 38 https://doi.org/10.1088/1361-648X/ac1092	journal	July 2021
Towards the fabrication of phosphorus qubits for a silicon quantum computer O’Brien, J. L.; Schofield, S. R.; Simmons, M. Y. Physical Review B, Vol. 64, Issue 16 https://doi.org/10.1103/PhysRevB.64.161401	journal	September 2001

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