Fuel up with a single-brew cortado and freshly made almond croissant from Pastelería Hofmann, a two-year-old pastry shop owned by Mey Hofmann of Barcelona’s top cooking school, before heading out of the city to Costa Brava, a picturesque region that has inspired the likes of Salvador Dalí and Pablo Picasso. The Catalunya Express ($31) leaves Estacio-Sants for Dalí’s hometown of Figueres every hour and takes 90 minutes. Once there, the surrealist’s namesake Theatre-Museum ($15) is a fifteen-minute walk from the station. Allot a couple of hours to browse the permanent collection, which houses thousands of Dalí’s works, including 39 jewels designed by the artist—the centerpiece is a ruby-encrusted beating heart—and their respective sketches. After that, walk over to the Museu del Joguet de Catalunya ($7) and marvel at the 4,000 toys on display, including some owned by Dalí, Joan Miró, and Federico García Lorca. Catch the 1 p.m. train to the medieval city of Girona (30 minutes away) to claim your 2 p.m. lunch reservation (Friday and Saturday bookings require six months' notice) at El Celler de Can Roca, a three-Michelin-starred restaurant run by molecular gastronomist Joan Roca and his brothers. Ask for a table overlooking the central arboretum and spring for the artfully plated thirteen-course “feast menu” ($200), a nearly three-hour flavor progression showcasing spherification, deconstruction, and sous vide techniques. After dessert, walk along the Roman wall in the city’s well-preserved old quarter to explore El Call, a medieval Jewish neighborhood made up of labyrinthine alleyways, winding streets, and narrow staircases. Catch the last train ($21, about 80 minutes) from Girona to Barcelona by 8 p.m.