Cracking mechanisms in lithiated silicon thin film electrodes

Huck Beng Chew, Binyue Hou, Xueju Wang, Shuman Xia

Research output: Contribution to journalArticlepeer-review


The massive cracking of silicon thin film electrodes in lithium ion batteries is associated with the colossal volume changes that occur during lithiation and delithiation cycles. However, the underlying cracking mechanism or even whether fracture initiates during lithiation or delithiation is still unknown. Here, we model the stress generation in amorphous silicon thin films during lithium insertion, fully accounting for the effects of finite strains, plastic flow, and pressure-gradients on the diffusion of lithium. Our finite element analyses demonstrate that the fracture of lithiated silicon films occurs by a sequential cracking mechanism which is distinct from fracture induced by residual tension in conventional thin films. During early-stage lithiation, the expansion of the lithium-silicon subsurface layer bends the film near the edges, and generates a high tensile stress zone at a critical distance away within the lithium-free silicon. Fracture initiates at this high tension zone and creates new film edges, which in turn bend and generate high tensile stresses a further critical distance away. Under repeated lithiation and delithiation cycles, this sequential cracking mechanism creates silicon islands of uniform diameter, which scales with the film thickness. The predicted island sizes, as well as the abrupt mitigation of fracture below a critical film thickness due to the diminishing tensile stress zone, is quantitatively in good agreement with experiments.

Original languageEnglish (US)
Pages (from-to)4176-4187
Number of pages12
JournalInternational Journal of Solids and Structures
Issue number23-24
StatePublished - Nov 1 2014


  • Finite element analysis
  • Lithiation-induced stress
  • Lithium ion battery
  • Sequential cracking
  • Silicon islands

ASJC Scopus subject areas

  • Modeling and Simulation
  • Materials Science(all)
  • Condensed Matter Physics
  • Mechanics of Materials
  • Mechanical Engineering
  • Applied Mathematics


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