On the Al + HCN reaction in helium nanodroplets

► The Al + HCN reaction is carried out at low temperature in a helium nanodroplet. ► Barrierless association leads to a bent HCNAl species with a 130° HCN bond angle. ► A Rotationally resolved CH stretch band for bent HCNAl is found red shifted 619 cm−1 from free HCN. ► Natural Bond Orbital analysis reveals substantial Al p-electron delocalization within HCNAl.