This chapter contributes to existing literature on psychological contracts by adopting a process-oriented lens to understand how psychological contract breach occurs. Drawing on neuroscientific insights, the authors extend and complement recently developed work on psychological contract dynamism by examining the intra-individual processes that precede the cognition of psychological contract breach. They argue that breach is affected by direct, indirect, and slow triggers that elicit conscious attention to the psychological contract terms and demand a shift from automatic processing to conscious attention. Moreover, stimuli matching with the (preconsciously buffered) memories of past triggers—connected triggers—will effortlessly activate the psychological contract. This results in an idiosyncratic chain of connected triggers processed in a cumulative manner, building up the pressure in the employment relationship and exacerbating the impact of breach. A better knowledge and understanding of these processes will offer employers alternative modes for handling and managing perceptions of psychological contract breach.