DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: On the mechanisms of stress relaxation and intensification at the lithium/solid-state electrolyte interface

Abstract

Under electrochemical cycling, stress intensification and relaxation within small volumes at the lithium/solid-state electrolyte (SSE) interface are thought to be critical factors contributing to mechanical failure of the SSE and subsequent short-circuiting of the device. Nanoindentation has been used to examine the diffusion-limited pressure lithium can support in the absence of active dislocation sources at high homologous temperatures. Based on the underlying physics of this deformation mechanism, a simple perturbation model coupling local current density, elastic stress, and diffusional creep relaxation is introduced. Combining this analysis with the indentation results, it is possible to describe a defect length scale which is too large for effective diffusional creep relaxation, but too small for efficient dislocation multiplication. In this instance, the properties of the SSE may become critical, and relevant indentation results of the SSE are described. Lastly, the final outcome of the proposed analysis is a newly developed deformation mechanism map.

Authors:
 [1]; ORCiD logo [2];  [1];  [1];  [1]
  1. Michigan Technological Univ., Houghton, MI (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1606763
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Research
Additional Journal Information:
Journal Volume: 34; Journal Issue: 21; Journal ID: ISSN 0884-2914
Publisher:
Materials Research Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; lithium metal; LLZO; critical current density; creep; nanoindentation

Citation Formats

Herbert, Erik G., Dudney, Nancy J., Rochow, Maria, Thole, Violet, and Hackney, Stephen A. On the mechanisms of stress relaxation and intensification at the lithium/solid-state electrolyte interface. United States: N. p., 2019. Web. doi:10.1557/jmr.2019.313.
Herbert, Erik G., Dudney, Nancy J., Rochow, Maria, Thole, Violet, & Hackney, Stephen A. On the mechanisms of stress relaxation and intensification at the lithium/solid-state electrolyte interface. United States. https://doi.org/10.1557/jmr.2019.313
Herbert, Erik G., Dudney, Nancy J., Rochow, Maria, Thole, Violet, and Hackney, Stephen A. Thu . "On the mechanisms of stress relaxation and intensification at the lithium/solid-state electrolyte interface". United States. https://doi.org/10.1557/jmr.2019.313. https://www.osti.gov/servlets/purl/1606763.
@article{osti_1606763,
title = {On the mechanisms of stress relaxation and intensification at the lithium/solid-state electrolyte interface},
author = {Herbert, Erik G. and Dudney, Nancy J. and Rochow, Maria and Thole, Violet and Hackney, Stephen A.},
abstractNote = {Under electrochemical cycling, stress intensification and relaxation within small volumes at the lithium/solid-state electrolyte (SSE) interface are thought to be critical factors contributing to mechanical failure of the SSE and subsequent short-circuiting of the device. Nanoindentation has been used to examine the diffusion-limited pressure lithium can support in the absence of active dislocation sources at high homologous temperatures. Based on the underlying physics of this deformation mechanism, a simple perturbation model coupling local current density, elastic stress, and diffusional creep relaxation is introduced. Combining this analysis with the indentation results, it is possible to describe a defect length scale which is too large for effective diffusional creep relaxation, but too small for efficient dislocation multiplication. In this instance, the properties of the SSE may become critical, and relevant indentation results of the SSE are described. Lastly, the final outcome of the proposed analysis is a newly developed deformation mechanism map.},
doi = {10.1557/jmr.2019.313},
journal = {Journal of Materials Research},
number = 21,
volume = 34,
place = {United States},
year = {Thu Nov 14 00:00:00 EST 2019},
month = {Thu Nov 14 00:00:00 EST 2019}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 27 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Elastic Properties of the Solid Electrolyte Li 7 La 3 Zr 2 O 12 (LLZO)
journal, December 2015


Lithium Mechanics: Roles of Strain Rate and Temperature and Implications for Lithium Metal Batteries
journal, January 2019

  • LePage, William S.; Chen, Yuxin; Kazyak, Eric
  • Journal of The Electrochemical Society, Vol. 166, Issue 2
  • DOI: 10.1149/2.0221902jes

Electromigration in stressed thin films
journal, January 1992


Indentation of a Power Law Creeping Solid
journal, April 1993

  • Bower, A. F.; Fleck, N. A.; Needleman, A.
  • Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 441, Issue 1911
  • DOI: 10.1098/rspa.1993.0050

Effect of Surface Microstructure on Electrochemical Performance of Garnet Solid Electrolytes
journal, January 2015

  • Cheng, Lei; Chen, Wei; Kunz, Martin
  • ACS Applied Materials & Interfaces, Vol. 7, Issue 3
  • DOI: 10.1021/am508111r

Lithium dendrite growth mechanisms in polymer electrolytes and prevention strategies
journal, January 2017

  • Barai, Pallab; Higa, Kenneth; Srinivasan, Venkat
  • Physical Chemistry Chemical Physics, Vol. 19, Issue 31
  • DOI: 10.1039/C7CP03304D

The Interactions of Composition and Stress in Crystalline Solids
journal, November 1984

  • Larche, F. C.; Cahn, J. W.
  • Journal of Research of the National Bureau of Standards, Vol. 89, Issue 6
  • DOI: 10.6028/jres.089.026

A parameter study of intercalation of lithium into storage particles in a lithium-ion battery
journal, December 2013


Stress generation in silicon particles during lithium insertion
journal, July 2010

  • Golmon, Stephanie; Maute, Kurt; Lee, Se-Hee
  • Applied Physics Letters, Vol. 97, Issue 3
  • DOI: 10.1063/1.3458707

Analysis of local grain boundary strengthening utilizing the extrinsic indentation size effect
journal, May 2019

  • Soman, Prasad Pramod; Herbert, Erik G.; Aifantis, Katerina E.
  • Journal of Materials Research, Vol. 34, Issue 13
  • DOI: 10.1557/jmr.2019.102

Effects of Concentration-Dependent Elastic Modulus on Diffusion-Induced Stresses for Battery Applications
journal, January 2010

  • Deshpande, Rutooj; Qi, Yue; Cheng, Yang-Tse
  • Journal of The Electrochemical Society, Vol. 157, Issue 8
  • DOI: 10.1149/1.3454762

Mechanical behavior of electrochemically lithiated silicon
journal, January 2015


Characterizing the Li–Li7La3Zr2O12 interface stability and kinetics as a function of temperature and current density
journal, January 2016


The difference of phase distributions in silicon after indentation with Berkovich and spherical indenters
journal, October 2005


Stress and Electromigration in Thin Film Metallisation
journal, January 1991


Lattice continuum and diffusional creep
journal, April 2016

  • Mesarovic, Sinisa Dj.
  • Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 472, Issue 2188
  • DOI: 10.1098/rspa.2016.0039

Diffusion Induced Stresses in Cylindrical Lithium-Ion Batteries: Analytical Solutions and Design Insights
journal, January 2012

  • Song, Yicheng; Lu, Bo; Ji, Xiang
  • Journal of The Electrochemical Society, Vol. 159, Issue 12, p. A2060-A2068
  • DOI: 10.1149/2.079212jes

Intergranular Li metal propagation through polycrystalline Li6.25Al0.25La3Zr2O12 ceramic electrolyte
journal, January 2017


Interface migration and the kirkendall effect in diffusion-driven phase transformations
journal, September 1990


Electromigration in thin aluminum films on titanium nitride
journal, April 1976

  • Blech, I. A.
  • Journal of Applied Physics, Vol. 47, Issue 4, p. 1203-1208
  • DOI: 10.1063/1.322842

Elastic, plastic, and creep mechanical properties of lithium metal
journal, October 2018

  • Masias, Alvaro; Felten, Nando; Garcia-Mendez, Regina
  • Journal of Materials Science, Vol. 54, Issue 3
  • DOI: 10.1007/s10853-018-2971-3

Mechanical characterization of LiPON films using nanoindentation
journal, October 2011


A simple stochastic model for yielding in specimens with limited number of dislocations
journal, April 2013


Stress generation by electromigration
journal, August 1976

  • Blech, I. A.; Herring, Conyers
  • Applied Physics Letters, Vol. 29, Issue 3
  • DOI: 10.1063/1.89024

Solid-state thin-film rechargeable batteries
journal, February 2005


Enhanced strength and temperature dependence of mechanical properties of Li at small scales and its implications for Li metal anodes
journal, December 2016

  • Xu, Chen; Ahmad, Zeeshan; Aryanfar, Asghar
  • Proceedings of the National Academy of Sciences, Vol. 114, Issue 1
  • DOI: 10.1073/pnas.1615733114

Temperature dependent flux balance of the Li/Li7La3Zr2O12 interface
journal, February 2019


Nanoindentation of high-purity vapor deposited lithium films: A mechanistic rationalization of the transition from diffusion to dislocation-mediated flow
journal, May 2018

  • Herbert, Erik G.; Hackney, Stephen A.; Thole, Violet
  • Journal of Materials Research, Vol. 33, Issue 10
  • DOI: 10.1557/jmr.2018.85

Lithium Metal Penetration Induced by Electrodeposition through Solid Electrolytes: Example in Single-Crystal Li 6 La 3 ZrTaO 12 Garnet
journal, January 2018

  • Swamy, Tushar; Park, Richard; Sheldon, Brian W.
  • Journal of The Electrochemical Society, Vol. 165, Issue 16
  • DOI: 10.1149/2.1391814jes

Grain Boundary Softening: A Potential Mechanism for Lithium Metal Penetration through Stiff Solid Electrolytes
journal, October 2018

  • Yu, Seungho; Siegel, Donald J.
  • ACS Applied Materials & Interfaces, Vol. 10, Issue 44
  • DOI: 10.1021/acsami.8b17223

Indentation size effects in crystalline materials: A law for strain gradient plasticity
journal, March 1998


The relation between load and penetration in the axisymmetric boussinesq problem for a punch of arbitrary profile
journal, May 1965


Stress and Strain-Energy Distributions within Diffusion-Controlled Insertion-Electrode Particles Subjected to Periodic Potential Excitations
journal, January 2009

  • Verbrugge, Mark W.; Cheng, Yang-Tse
  • Journal of The Electrochemical Society, Vol. 156, Issue 11
  • DOI: 10.1149/1.3205485

Plasticity in Confined Dimensions
journal, June 2010


Atomistic and computer modeling of metallization failure of integrated circuits by electromigration
journal, July 1991

  • Kirchheim, R.; Kaeber, U.
  • Journal of Applied Physics, Vol. 70, Issue 1
  • DOI: 10.1063/1.350305

A large deformation elastic–viscoplastic model for lithium
journal, October 2018


The Indentation Size Effect: A Critical Examination of Experimental Observations and Mechanistic Interpretations
journal, June 2010


Nanoindentation of high-purity vapor deposited lithium films: A mechanistic rationalization of diffusion-mediated flow
journal, May 2018

  • Herbert, Erik G.; Hackney, Stephen A.; Thole, Violet
  • Journal of Materials Research, Vol. 33, Issue 10
  • DOI: 10.1557/jmr.2018.84

Nanoindentation of high-purity vapor deposited lithium films: The elastic modulus
journal, May 2018

  • Herbert, Erik G.; Hackney, Stephen A.; Dudney, Nancy J.
  • Journal of Materials Research, Vol. 33, Issue 10
  • DOI: 10.1557/jmr.2018.83

The correlation of indentation experiments
journal, April 1970


Morphological Stability of a Particle Growing by Diffusion or Heat Flow
journal, February 1963

  • Mullins, W. W.; Sekerka, R. F.
  • Journal of Applied Physics, Vol. 34, Issue 2
  • DOI: 10.1063/1.1702607

Unravelling the physics of size-dependent dislocation-mediated plasticity
journal, January 2015


Li 7 La 3 Zr 2 O 12 Interface Modification for Li Dendrite Prevention
journal, April 2016

  • Tsai, Chih-Long; Roddatis, Vladimir; Chandran, C. Vinod
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 16
  • DOI: 10.1021/acsami.6b00831

Numerical Simulation of Intercalation-Induced Stress in Li-Ion Battery Electrode Particles
journal, January 2007

  • Zhang, Xiangchun; Shyy, Wei; Marie Sastry, Ann
  • Journal of The Electrochemical Society, Vol. 154, Issue 10
  • DOI: 10.1149/1.2759840

Theory of Growth of Spherical Precipitates from Solid Solution
journal, October 1949

  • Zener, Clarence
  • Journal of Applied Physics, Vol. 20, Issue 10
  • DOI: 10.1063/1.1698258

An improved technique for determining hardness and elastic modulus using load and displacement sensing indentation experiments
journal, June 1992

  • Oliver, W. C.; Pharr, G. M.
  • Journal of Materials Research, Vol. 7, Issue 06, p. 1564-1583
  • DOI: 10.1557/JMR.1992.1564

Controlling and correlating the effect of grain size with the mechanical and electrochemical properties of Li 7 La 3 Zr 2 O 12 solid-state electrolyte
journal, January 2017

  • Sharafi, Asma; Haslam, Catherine G.; Kerns, Robert D.
  • J. Mater. Chem. A, Vol. 5, Issue 40
  • DOI: 10.1039/C7TA06790A

Measurement of hardness and elastic modulus by instrumented indentation: Advances in understanding and refinements to methodology
journal, January 2004


Intercalation-Induced Stress and Heat Generation within Single Lithium-Ion Battery Cathode Particles
journal, January 2008

  • Zhang, Xiangchun; Sastry, Ann Marie; Shyy, Wei
  • Journal of The Electrochemical Society, Vol. 155, Issue 7
  • DOI: 10.1149/1.2926617

The interaction of lattice defects and grain boundaries
journal, August 1972


The morphological stability of lateral growth in solid-solid phase transformation during thin-film interdiffusion in Al/Cu bimetal films
journal, August 1994

  • McCarty, E. D.; Hackney, S. A.
  • Metallurgical and Materials Transactions A, Vol. 25, Issue 8
  • DOI: 10.1007/BF02668527

A Computational Model of the Mechanical Behavior within Reconstructed LixCoO2 Li-ion Battery Cathode Particles
journal, June 2014


A nanoindentation study of the viscoplastic behavior of pure lithium
journal, March 2017


Resolving the Amorphous Structure of Lithium Phosphorus Oxynitride (Lipon)
journal, July 2018

  • Lacivita, Valentina; Westover, Andrew S.; Kercher, Andrew
  • Journal of the American Chemical Society, Vol. 140, Issue 35
  • DOI: 10.1021/jacs.8b05192

Stability of a Planar Interface During Solidification of a Dilute Binary Alloy
journal, February 1964

  • Mullins, W. W.; Sekerka, R. F.
  • Journal of Applied Physics, Vol. 35, Issue 2
  • DOI: 10.1063/1.1713333

Annihilation and sources in continuum dislocation dynamics
journal, March 2018


Load–displacement behavior during sharp indentation of viscous–elastic–plastic materials
journal, January 2003

  • Oyen, Michelle L.; Cook, Robert F.
  • Journal of Materials Research, Vol. 18, Issue 1
  • DOI: 10.1557/JMR.2003.0020

Measurement of power-law creep parameters by instrumented indentation methods
journal, February 2013

  • Su, Caijun; Herbert, Erik G.; Sohn, Sangjoon
  • Journal of the Mechanics and Physics of Solids, Vol. 61, Issue 2
  • DOI: 10.1016/j.jmps.2012.09.009

Stress and electromigration in Al-lines of integrated circuits
journal, February 1992


A Mathematical Model of Stress Generation and Fracture in Lithium Manganese Oxide
journal, January 2006

  • Christensen, John; Newman, John
  • Journal of The Electrochemical Society, Vol. 153, Issue 6
  • DOI: 10.1149/1.2185287

Fast, vacancy-free climb of prismatic dislocation loops in bcc metals
journal, August 2016

  • Swinburne, Thomas D.; Arakawa, Kazuto; Mori, Hirotaro
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep30596

Stress evolution due to electromigration in confined metal lines
journal, April 1993

  • Korhonen, M. A.; Bo/rgesen, P.; Tu, K. N.
  • Journal of Applied Physics, Vol. 73, Issue 8
  • DOI: 10.1063/1.354073

A model for conductor failure considering diffusion concurrently with electromigration resulting in a current exponent of 2
journal, June 1986

  • Shatzkes, M.; Lloyd, J. R.
  • Journal of Applied Physics, Vol. 59, Issue 11
  • DOI: 10.1063/1.336731

Contact between Garnet-Type Solid Electrolyte and Lithium Metal Anode: Influence on Charge Transfer Resistance and Short Circuit Prevention
journal, January 2017

  • Basappa, Rajendra Hongahally; Ito, Tomoko; Yamada, Hirotoshi
  • Journal of The Electrochemical Society, Vol. 164, Issue 4
  • DOI: 10.1149/2.0841704jes

Role of material properties and mechanical constraint on stress-assisted diffusion in plate electrodes of lithium ion batteries
journal, February 2013


Stress generation and fracture in lithium insertion materials
journal, March 2006


Mechanical metallurgy.
book, January 1961


Vacancy Formation Energy at Metal-Silicon Interface Region
journal, April 2005

  • Suezawa, Masashi; Saitoh, Kesami; Kojima, Ken-ichi
  • Japanese Journal of Applied Physics, Vol. 44, Issue 4L
  • DOI: 10.1143/JJAP.44.L593

Mechanism of Lithium Metal Penetration through Inorganic Solid Electrolytes
journal, July 2017

  • Porz, Lukas; Swamy, Tushar; Sheldon, Brian W.
  • Advanced Energy Materials, Vol. 7, Issue 20
  • DOI: 10.1002/aenm.201701003

Approaches toward lithium metal stabilization
journal, October 2018


Thin-film lithium and lithium-ion batteries
journal, November 2000