The solvent-provoked formation and evolution of thin film buckling-delamination on a compliant substrate have been studied. The film surface is observed by an optical microscope showing a remarkable dynamic buckling-delamination development and a subsequent stable branchedstraight state. It is revealed that the initiation, propagation, and the resulting patterns of film buckles are strongly dependent on the solvent type, film stress, interfacial adhesion, and film thickness. The buckling could be controlled further by a reasonable chemical solvent configuration and used to provide useful information for the pattern creation on polymer systems in diverse fields, such as micro/nanofabrication and optics. KEYWORDS buckle, film stress, polymer substrate, solvent diffusion, thin film 1 | INTRODUCTION Thin films and coatings are widely used in a substantial range of technological applications, ranging from protective layers to applications in optical, electric, engineering, biomedical, nuclear, and thermal fields. The high performance and reliability of film-substrate structures are strongly dependent on their mechanical integrity and the adhesion to the substrate. Failure of thin film coatings can occur in various forms, such as blistering, delamination, and dewetting.Surface instability is ubiquitous which can be frequently observed in many systems, involving metallic or soft polymeric thin films on elastomeric substrates, hydrogels on a rigid flat substrate, and biological tissues in response to external stimuli, such as mechanical pressure, 1,2 temperature, 3 pH level, 4 light, 5 humidity, 6 and solvent environment. 7 Although the phenomenon has been treated as a nuisance to be avoided, researchers have extensively exploited the surface instability in a wide range of applications ranging from microelectronics, 8,9 biotechnology, 10 fabrication of structures 11 to optical systems 12,13 and microfluidic devices. 14,15 Recently, buckling has attracted much attention as a useful approach for surface pattern controlment and material property characterization, 16,17 which arises when a relatively thick substrate-supported thin layer undergoes an excessive compression. The compression generally originates from the mechanical constants mismatch between different layers, which can be utilized to create interesting topographical patterns such as straight-sided wrinkles, 18 telephone cord structures, 19-23 and circular blisters. 24,25 A range of different strategies have been explored to produce patterns in thin films. Laser-induced well-ordered and controllable telephone cord patterns were constructed in as-deposited metallic thin films. 26 Pre-patterning the thin film under strain, in combination with a triggered release of the adhesion via electrochemistry, allowed for the design of well-controlled sub-micrometer. 27 Formation of mutually orthogonal multi-scale instability modes was triggered by electric-thermal loads. 28 A freely floating polymer film wrinkled under the capillary force exerted by a drop of water. 29 It is...