Mapping Local Charge Recombination Heterogeneity by Multidimensional Nanospectroscopic Imaging

Mind the Gap Near-field microscopy has benefited from subwavelength near-field plasmonic probes that make use of the field-concentrating properties of gaps. These probes achieve maximum enhancement only in the tip-substrate gap mode, which can yield large near-field signals, but only for a metallic substrate and for very small tip-substrate gap distances. Bao et al. (p. 1317) designed a probe that unites broadband field enhancement and confinement with bidirectional coupling between far-field and near-field electromagnetic energy. Their tips primarily rely on the internal gap modes of the tip itself, thereby enabling it to image nonmetallic samples. A near-field optical probe designed to maximize its own signal enhancement can be used to image nonmetallic samples. As materials functionality becomes more dependent on local physical and electronic properties, the importance of optically probing matter with true nanoscale spatial resolution has increased. In this work, we mapped the influence of local trap states within individual nanowires on carrier recombination with deeply subwavelength resolution. This is achieved using multidimensional nanospectroscopic imaging based on a nano-optical device. Placed at the end of a scan probe, the device delivers optimal near-field properties, including highly efficient far-field to near-field coupling, ultralarge field enhancement, nearly background-free imaging, independence from sample requirements, and broadband operation. We performed ~40-nanometer–resolution hyperspectral imaging of indium phosphide nanowires via excitation and collection through the probes, revealing optoelectronic structure along individual nanowires that is not accessible with other methods.