Imaging the motion of electrons across semiconductor heterojunctions

• Published in: Nature nanotechnology Vol. 12; no. 1; pp. 36 - 40
• Main Authors: Man, Michael K. L., Margiolakis, Athanasios, Deckoff-Jones, Skylar, Harada, Takaaki, Wong, E Laine, Krishna, M. Bala Murali, Madéo, Julien, Winchester, Andrew, Lei, Sidong, Vajtai, Robert, Ajayan, Pulickel M., Dani, Keshav M.
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 01.01.2017; Nature Publishing Group
• Subjects: 147/28; 639/301/357/1018; 639/4077/4072/4062; 639/766/119/544; 639/925/927/1007; 639/925/930/2735; Electric fields; Electrons; Energy; Equilibrium; Imaging; letter; Materials Science; Microscopy; Nanotechnology; Nanotechnology and Microengineering; Photovoltaic cells; Probes; Semiconductor devices; Semiconductors; Solar cells; Temporal resolution; Transistors; Japan; Okinawa
• ISSN: 1748-3387; 1748-3395
• DOI: 10.1038/nnano.2016.183

The flow of photoexcited electrons in a type-II heterostructure can be imaged with energy, spatial and temporal resolution. Technological progress since the late twentieth century has centred on semiconductor devices, such as transistors, diodes and solar cells 1 , 2 , 3 , 4 , 5 , 6 , 7 , 8 . At the heart of these devices is the internal motion of electrons through semiconductor materials due to applied electric fields 3 , 9 or by the excitation of photocarriers 2 , 4 , 5 , 8 . Imaging the motion of these electrons would provide unprecedented insight into this important phenomenon, but requires high spatial and temporal resolution. Current studies of electron dynamics in semiconductors are generally limited by the spatial resolution of optical probes, or by the temporal resolution of electronic probes. Here, by combining femtosecond pump–probe techniques with spectroscopic photoemission electron microscopy 10 , 11 , 12 , 13 , we imaged the motion of photoexcited electrons from high-energy to low-energy states in a type-II 2D InSe/GaAs heterostructure. At the instant of photoexcitation, energy-resolved photoelectron images revealed a highly non-equilibrium distribution of photocarriers in space and energy. Thereafter, in response to the out-of-equilibrium photocarriers, we observed the spatial redistribution of charges, thus forming internal electric fields, bending the semiconductor bands, and finally impeding further charge transfer. By assembling images taken at different time-delays, we produced a movie lasting a few trillionths of a second of the electron-transfer process in the photoexcited type-II heterostructure—a fundamental phenomenon in semiconductor devices such as solar cells. Quantitative analysis and theoretical modelling of spatial variations in the movie provide insight into future solar cells, 2D materials and other semiconductor devices.