Creating successful heterogeneous enantioselective catalysts remains an imp
ortant goal for the chemicals and pharmaceuticals industries, with consider
able attention being focused on chirally modified metals as promising candi
dates. Here, recent surface science results are reviewed, which throw, a ne
w and intriguing light on these modified metal surfaces, highlighting new p
henomena such as complex adsorption phases, two-dimensional organization, a
nd the surprising creation of extended chiral surfaces. This molecular leve
l information provides an important and fresh input into future design stra
tegies.