Stability, metallicity, and magnetism in niobium silicide nanofilms

Lu, Xuezeng; Goronzy, Dominic P.; Torres-Castanedo, Carlos G.; Masih Das, Paul; Kazemzadeh-Atoufi, Maryam; McFadden, Anthony; McRae, Corey H.; Voorhees, Peter W.; Dravid, Vinayak P.; Bedzyk, Michael J.; Hersam, Mark C.; Rondinelli, James M.

doi:10.1103/physrevmaterials.6.064402

Stability, metallicity, and magnetism in niobium silicide nanofilms

Journal Article · Fri Jun 03 00:00:00 EDT 2022 · Physical Review Materials

DOI:https://doi.org/10.1103/physrevmaterials.6.064402· OSTI ID:1871024

Lu, Xuezeng ^[1]; ^[2]; Torres-Castanedo, Carlos G. ^[2]; Masih Das, Paul ^[2]; ^[2]; ^[3]; ^[4]; Voorhees, Peter W. ^[2]; ^[2]; ^[2]; Hersam, Mark C. ^[2]; ^[2]

Northwestern Univ., Evanston, IL (United States); Northwestern University
Northwestern Univ., Evanston, IL (United States)
National Inst. of Standards and Technology (NIST), Boulder, CO (United States)
Univ. of Colorado, Boulder, CO (United States)

Modern superconducting qubits based on two-dimensional (2D) transmons typically involve the growth of Nb thin films on high-resistivity Si substrates. Since imperfections at the Nb-Si heterointerface have been implicated as a source of two-level systems that limit quantum coherence times, detailed characterization and understanding of niobium silicide interfacial layers are critical to improving superconducting qubit technology. While bulk binary intermetallic niobium silicide phases are well understood, the thermodynamic phase stability and properties of ultrathin niobium silicides, such as those found at the Nb-Si heterointerface in 2D transmons, have not yet been explored. Here, we report finite-sized effects for ultrathin niobium silicide films using density functional theory calculations and predict nanoscale stabilization of Nb₆Si₅ over the bulk α-Nb₅Si₃ phase. This result is consistent with our experimental observations of a niobium silicide interfacial layer between a sputtered Nb thin film and the underlying Si substrate. Furthermore, our calculations show that Nb₆Si₅ nanofilms are nonmagnetic, making them superior to nanofilms of α-Nb₅Si₃ that exhibit antiferromagnetic correlations detrimental to long coherence times in superconducting qubits. Furthermore, by providing atomic-scale insight into niobium silicide nanofilms, this paper can help guide ongoing efforts to optimize Nb-Si heterointerfaces for long coherence times in superconducting qubits.

View Accepted Manuscript (DOE)

Research Organization:: Northwestern Univ., Evanston, IL (United States); Fermi National Accelerator Laboratory (FNAL), Batavia, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), High Energy Physics (HEP)

Grant/Contract Number:: AC02-07CH11359; AC02-05CH11231

OSTI ID:: 1871024

Alternate ID(s):: OSTI ID: 1879474

Report Number(s):: FERMILAB-PUB-22-544-SQMS; ECCS-1542205; DMR-1720139

Journal Information:: Physical Review Materials, Journal Name: Physical Review Materials Journal Issue: 6 Vol. 6; ISSN 2475-9953

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

References (52)

Chemically Tuning between Ferromagnetism and Antiferromagnetism by Combining Theory and Synthesis in Iron/Manganese Rhodium Borides Dronskowski, Richard; Korczak, Karol; Lueken, Heiko Angewandte Chemie International Edition, Vol. 41, Issue 14 https://doi.org/10.1002/1521-3773(20020715)41:14%3C2528::AID-ANIE2528%3E3.0.CO;2-6	journal	July 2002
The Nb-Si (Niobium-Silicon) system Schlesinger, M. E.; Okamoto, H.; Gokhale, A. B. Journal of Phase Equilibria, Vol. 14, Issue 4 https://doi.org/10.1007/BF02671971	journal	August 1993
Correlation between electronic structure, mechanical properties and phase stability in intermetallic compounds Ravindran, P.; Asokamani, R. Bulletin of Materials Science, Vol. 20, Issue 4 https://doi.org/10.1007/BF02744780	journal	July 1997
Investigation of ultrashort laser excitation of aluminum and tungsten by reflectivity measurements Genieys, T.; Sentis, M.; Utéza, O. Applied Physics A, Vol. 126, Issue 4 https://doi.org/10.1007/s00339-020-3440-9	journal	March 2020
Atomistic Modeling of Metal-Nanotube Contacts Kienle, Diego; Ghosh, Avik W. Journal of Computational Electronics, Vol. 4, Issue 1-2 https://doi.org/10.1007/s10825-005-7116-7	journal	April 2005
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
Influence of vibrational entropy on structural stability of Nb–Si and Mo–Si systems at elevated temperatures Chen, Yue; Hammerschmidt, T.; Pettifor, D. G. Acta Materialia, Vol. 57, Issue 9 https://doi.org/10.1016/j.actamat.2009.02.014	journal	May 2009
Growth mechanism of phases by interdiffusion and diffusion of species in the niobium–silicon system Prasad, S.; Paul, A. Acta Materialia, Vol. 59, Issue 4 https://doi.org/10.1016/j.actamat.2010.11.022	journal	February 2011
An efficient ab-initio quasiharmonic approach for the thermodynamics of solids Huang, Liang-Feng; Lu, Xue-Zeng; Tennessen, Emrys Computational Materials Science, Vol. 120 https://doi.org/10.1016/j.commatsci.2016.04.012	journal	July 2016
Theoretical study of structural characteristics, mechanical properties and electronic structure of metal (TM = V, Nb and Ta) silicides Wan, Biao; Xiao, Furen; Zhang, Yunkun Journal of Alloys and Compounds, Vol. 681 https://doi.org/10.1016/j.jallcom.2016.04.253	journal	October 2016
RuAl ₆ —An Endohedral Aluminide Superconductor Ryżyńska, Zuzanna; Chamorro, Juan R.; McQueen, Tyrel M. Chemistry of Materials, Vol. 32, Issue 9 https://doi.org/10.1021/acs.chemmater.9b05277	journal	April 2020
Crystal orbital Hamilton populations (COHP): energy-resolved visualization of chemical bonding in solids based on density-functional calculations Dronskowski, Richard; Bloechl, Peter E. The Journal of Physical Chemistry, Vol. 97, Issue 33 https://doi.org/10.1021/j100135a014	journal	August 1993
Unusual Electronic and Bonding Properties of the Zintl Phase Ca ₅ Ge ₃ and Related Compounds. A Theoretical Analysis ¹ Mudring, Anja-Verena; Corbett, John D. Journal of the American Chemical Society, Vol. 126, Issue 16 https://doi.org/10.1021/ja030216b	journal	March 2004
Atomic Layer Deposition and Superconducting Properties of NbSi Films Proslier, Thomas; Klug, Jeffrey A.; Elam, Jeffrey W. The Journal of Physical Chemistry C, Vol. 115, Issue 19 https://doi.org/10.1021/jp201873b	journal	April 2011
Crystal Orbital Hamilton Population (COHP) Analysis As Projected from Plane-Wave Basis Sets Deringer, Volker L.; Tchougréeff, Andrei L.; Dronskowski, Richard The Journal of Physical Chemistry A, Vol. 115, Issue 21 https://doi.org/10.1021/jp202489s	journal	June 2011
Surface Structure and Coverage of an Oligonucleotide Probe Tethered onto a Gold Substrate and Its Hybridization Efficiency for a Polynucleotide Target Huang, Eva; Satjapipat, Munlika; Han, Shubo Langmuir, Vol. 17, Issue 4 https://doi.org/10.1021/la001019i	journal	January 2001
Accurate first-principles structures and energies of diversely bonded systems from an efficient density functional Sun, Jianwei; Remsing, Richard C.; Zhang, Yubo Nature Chemistry, Vol. 8, Issue 9 https://doi.org/10.1038/nchem.2535	journal	June 2016
New material platform for superconducting transmon qubits with coherence times exceeding 0.3 milliseconds Place, Alexander P. M.; Rodgers, Lila V. H.; Mundada, Pranav Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-22030-5	journal	March 2021
Introducing DDEC6 atomic population analysis: part 1. Charge partitioning theory and methodology Manz, Thomas A.; Limas, Nidia Gabaldon RSC Advances, Vol. 6, Issue 53 https://doi.org/10.1039/C6RA04656H	journal	January 2016
Introducing DDEC6 atomic population analysis: part 2. Computed results for a wide range of periodic and nonperiodic materials Limas, Nidia Gabaldon; Manz, Thomas A. RSC Advances, Vol. 6, Issue 51 https://doi.org/10.1039/C6RA05507A	journal	January 2016
Prediction of superconducting iron–bismuth intermetallic compounds at high pressure Amsler, Maximilian; Naghavi, S. Shahab; Wolverton, Chris Chemical Science, Vol. 8, Issue 3 https://doi.org/10.1039/C6SC04683E	journal	January 2017
Schottky barrier and contact resistance at a niobium/silicon interface Heslinga, D. R.; Klapwijk, T. M. Applied Physics Letters, Vol. 54, Issue 11 https://doi.org/10.1063/1.100793	journal	March 1989
Effect of metal/substrate interfaces on radio-frequency loss in superconducting coplanar waveguides Wisbey, David S.; Gao, Jiansong; Vissers, Michael R. Journal of Applied Physics, Vol. 108, Issue 9 https://doi.org/10.1063/1.3499608	journal	November 2010
Formation of metal‐rich silicides in the initial stage of interfacial reactions in Nb/Si systems Nakanishi, Taichi; Takeyama, Mayumi; Noya, Atsushi Journal of Applied Physics, Vol. 77, Issue 2 https://doi.org/10.1063/1.359584	journal	January 1995
Electron density fluctuations at interfaces in Nb/Si bilayer, trilayer, and multilayer films: An x-ray reflectivity study Suresh, N.; Phase, D. M.; Gupta, Ajay Journal of Applied Physics, Vol. 87, Issue 11 https://doi.org/10.1063/1.373479	journal	June 2000
Oxidation of the two-phase Nb/Nb ₅ Si ₃ composite: The role of energetics, thermodynamics, segregation, and interfaces Liu, Shi-Yu; Shang, Jia-Xiang; Wang, Fu-He The Journal of Chemical Physics, Vol. 138, Issue 1 https://doi.org/10.1063/1.4773447	journal	January 2013
TOF-SIMS analysis of decoherence sources in superconducting qubits Murthy, A. A.; Lee, J.; Kopas, C. Applied Physics Letters, Vol. 120, Issue 4 https://doi.org/10.1063/5.0079321	journal	January 2022
Characterization of silicide precipitates in Nb–Si and Nb–Ti–Si alloys Grylls, R. J.; Bewlay, B. P.; Lipsitt, H. A. Philosophical Magazine A, Vol. 81, Issue 8 https://doi.org/10.1080/01418610108216647	journal	August 2001
The impact of Ti and temperature on the stability of Nb ₅ Si ₃ phases: a first-principles study Papadimitriou, Ioannis; Utton, Claire; Tsakiropoulos, Panos Science and Technology of Advanced Materials, Vol. 18, Issue 1 https://doi.org/10.1080/14686996.2017.1341802	journal	July 2017
The electronic structure of 4d and 5d silicides Speier, W.; Kumar, L.; Sarma, D. D. Journal of Physics: Condensed Matter, Vol. 1, Issue 46 https://doi.org/10.1088/0953-8984/1/46/006	journal	November 1989
Effects of alloying element Ti on α-Nb ₅ Si ₃ and Nb ₃ Al from first principles Chen, Yue; Shang, Jia-Xiang; Zhang, Yue Journal of Physics: Condensed Matter, Vol. 19, Issue 1 https://doi.org/10.1088/0953-8984/19/1/016215	journal	December 2006
Three-Dimensional Superconducting Resonators at T < 20 mK with Photon Lifetimes up to τ = 2 s Romanenko, A.; Pilipenko, R.; Zorzetti, S. Physical Review Applied, Vol. 13, Issue 3 https://doi.org/10.1103/PhysRevApplied.13.034032	journal	March 2020
Stability in ordered and amorphous transition-metal compounds Moruzzi, V. L.; Oelhafen, P.; Williams, A. R. Physical Review B, Vol. 27, Issue 12 https://doi.org/10.1103/PhysRevB.27.7194	journal	June 1983
Crystal structure, phase stability, and electronic structure of Ti-Al intermetallics: Ti 3 Al Hong, T.; Watson-Yang, T. J.; Guo, X. -Q. Physical Review B, Vol. 43, Issue 3 https://doi.org/10.1103/PhysRevB.43.1940	journal	January 1991
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
Density-functional theory and strong interactions: Orbital ordering in Mott-Hubbard insulators Liechtenstein, A. I.; Anisimov, V. I.; Zaanen, J. Physical Review B, Vol. 52, Issue 8 https://doi.org/10.1103/PhysRevB.52.R5467	journal	August 1995
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Bonding characteristics and site occupancies of alloying elements in different Nb 5 Si 3 phases from first principles Chen, Yue; Shang, Jia-Xiang; Zhang, Yue Physical Review B, Vol. 76, Issue 18 https://doi.org/10.1103/PhysRevB.76.184204	journal	November 2007
High-throughput computational screening of thermal conductivity, Debye temperature, and Grüneisen parameter using a quasiharmonic Debye model Toher, Cormac; Plata, Jose J.; Levy, Ohad Physical Review B, Vol. 90, Issue 17 https://doi.org/10.1103/PhysRevB.90.174107	journal	November 2014
Electrochemical phase diagrams for Ti oxides from density functional calculations Huang, Liang-Feng; Rondinelli, James M. Physical Review B, Vol. 92, Issue 24 https://doi.org/10.1103/PhysRevB.92.245126	journal	December 2015
Competing magnetic instabilities in the weak itinerant antiferromagnetic TiAu Goh, Wen Fong; Pickett, Warren E. Physical Review B, Vol. 95, Issue 20 https://doi.org/10.1103/PhysRevB.95.205124	journal	May 2017
First-principles study of localized and delocalized electronic states in crystallographic shear phases of niobium oxide Koçer, Can P.; Griffith, Kent J.; Grey, Clare P. Physical Review B, Vol. 99, Issue 7 https://doi.org/10.1103/PhysRevB.99.075151	journal	February 2019
Strongly Constrained and Appropriately Normed Semilocal Density Functional Sun, Jianwei; Ruzsinszky, Adrienn; Perdew, John P. Physical Review Letters, Vol. 115, Issue 3 https://doi.org/10.1103/PhysRevLett.115.036402	journal	July 2015
Stable MoSi 2 nanofilms with controllable and high metallicity Huang, Liang-Feng; Rondinelli, James M. Physical Review Materials, Vol. 1, Issue 6 https://doi.org/10.1103/PhysRevMaterials.1.063001	journal	November 2017
Antiferromagnetic ground state in the MnGa 4 intermetallic compound Verchenko, V. Yu.; Tsirlin, A. A.; Kasinathan, D. Physical Review Materials, Vol. 2, Issue 4 https://doi.org/10.1103/PhysRevMaterials.2.044408	journal	April 2018
Co-refinement of multiple-contrast neutron/X-ray reflectivity data using MOTOFIT Nelson, Andrew Journal of Applied Crystallography, Vol. 39, Issue 2 https://doi.org/10.1107/S0021889806005073	journal	March 2006
Insight into the structures, melting points, and mechanical properties of NbSi ₂ from first‐principles calculations Wang, Shuang‐Lun; Pan, Yong Journal of the American Ceramic Society, Vol. 102, Issue 8 https://doi.org/10.1111/jace.16345	journal	February 2019
A mechanism for weak itinerant antiferromagnetism: Mirrored van Hove singularities Goh, Wen Fong; Pickett, Warren E. EPL (Europhysics Letters), Vol. 116, Issue 2 https://doi.org/10.1209/0295-5075/116/27004	journal	October 2016
Electrical and structural characterization of Nb-Si thin alloy film Nava, F.; Psaras, P. A.; Takai, H. Journal of Materials Research, Vol. 1, Issue 2 https://doi.org/10.1557/JMR.1986.0327	journal	April 1986
Materials in superconducting quantum bits Oliver, William D.; Welander, Paul B. MRS Bulletin, Vol. 38, Issue 10 https://doi.org/10.1557/mrs.2013.229	journal	October 2013
The Crystal Orbital Hamilton Population (COHP) Method as a Tool to Visualize and Analyze Chemical Bonding in Intermetallic Compounds Steinberg, Simon; Dronskowski, Richard Crystals, Vol. 8, Issue 5 https://doi.org/10.3390/cryst8050225	journal	May 2018

Similar Records

TOF-SIMS analysis of decoherence sources in superconducting qubits

Journal Article · Sun Jan 23 19:00:00 EST 2022 · Appl.Phys.Lett. · OSTI ID:1834168

Related Subjects

36 MATERIALS SCIENCE
X-ray reflectivity
density functional calculations
niobium silicide nanofilm
phase stability
silicides
thin films
transmission electron microscopy
transmons
superconducting qubits

Stability, metallicity, and magnetism in niobium silicide nanofilms

Citation Formats

References (52)

Similar Records

Related Subjects