Nondestructively Visualizing and Understanding the Mechano‐Electro‐chemical Origins of “Soft Short” and “Creeping” in All‐Solid‐State Batteries

All‐solid‐state Li‐metal batteries (ASLMBs) represent a significant breakthrough in the quest to overcome limitations associated with traditional Li‐ion batteries, particularly in energy density and safety aspects. However, widespread implementation is stymied due to a lack of profound understanding of the complex mechano‐electro‐chemical behavior of Li metal in the ASLMBs. Herein, operando neutron imaging and X‐ray computed tomography (XCT) are leveraged to nondestructively visualize Li behaviors within ASLMBs. This approach offers real‐time observations of Li evolutions, both pre‐ and post‐ occurrence of a “soft short”. The coordination of 2D neutron radiography and 3D neutron tomography enables charting of the terrain of Li metal deformation operando. Concurrently, XCT offers a 3D insight into the internal structure of the battery following a “soft short”. Despite the manifestation of a “soft short”, the persistence of Faradaic processes is observed. To study the elusive “soft short” , phase field modeling is coupled with electrochemistry and solid mechanics theory. The research unravels how external pressure curbs dendrite growth, potentially leading to dendrite fractures and thus uncovering the origins of both “soft” and “hard” shorts in ASLMBs. Furthermore, by harnessing finite element modeling, it dive deeper into the mechanical deformation and the fluidity of Li metal. This work successfully visualizes the Li deformation and the “soft short” in all‐solid‐state Li metal batteries using operando neutron imaging. It unravels how external pressure curbs dendrite growth, but also leads to dendrite fractures, uncovering the origins of both “soft” and “hard” shorts in Li metal batteries. Furthermore, finite element modeling enables a deeper dive into the deformation and the fluidity of Li metal.