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Hot carrier-enhanced interlayer electron–hole pair multiplication in 2D semiconductor heterostructure photocells

Abstract

Strong electronic interactions can result in novel particle–antiparticle (electron–hole, e–h) pair generation effects1, which may be exploited to enhance the photoresponse of nanoscale optoelectronic devices. Highly efficient e–h pair multiplication has been demonstrated in several important nanoscale systems, including nanocrystal quantum dots2,3,4,5,6, carbon nanotubes7,8,9 and graphene10,11,12,13. The small Fermi velocity and nonlocal nature of the effective dielectric screening in ultrathin layers of transition-metal dichalcogenides (TMDs) indicates that e–h interactions are very strong14,15,16, so high-efficiency generation of e–h pairs from hot electrons is expected. However, such e–h pair multiplication has not been observed in 2D TMD devices. Here, we report the highly efficient multiplication of interlayer e–h pairs in 2D semiconductor heterostructure photocells. Electronic transport measurements of the interlayer I–VSD characteristics indicate that layer-indirect e–h pairs are generated by hot-electron impact excitation at temperatures near T = 300 K. By exploiting this highly efficient interlayer e–h pair multiplication process, we demonstrate near-infrared optoelectronic devices that exhibit 350% enhancement of the optoelectronic responsivity at microwatt power levels. Our findings, which demonstrate efficient carrier multiplication in TMD-based optoelectronic devices, make 2D semiconductor heterostructures viable for a new class of ultra-efficient photodetectors based on layer-indirect e–h excitations.

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Figure 1: Device geometry, band-structure, photoluminescence and current–voltage characteristics of the 2D semiconductor heterostructure device.
Figure 2: Gate voltage dependence of the interlayer current characteristics in the 2D TMD heterostructure device.
Figure 3: Temperature dependence of the interlayer I–VSD characteristics.
Figure 4: Gate voltage, source–drain voltage and temperature dependence of the interlayer current in the 2D semiconductor heterostructure device.
Figure 5: Interlayer photocurrent characteristics and multiplication enhancement in the 2D heterojunction photocell.

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Acknowledgements

This work was made possible by support from SHINES, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Basic Energy Sciences under award no. SC0012670. N.M.G. and F.B. acknowledge support from the Air Force Office of Scientific Research, Biosystems Directorate award no. FA9550-16-1-0216. N.M.G. acknowledges a Cottrell Scholar Award and support from the National Science Foundation Division of Materials Research CAREER award no. 1651247. M.G., S.S. and R.K.L. acknowledge support from SHINES. Nanofabrication and Raman characterization was performed at the Center for Nanoscale Science and Engineering (CNSE) at the University of California Riverside. DFT calculations were supported by the SHINES centre. This work used the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by National Science Foundation grant no. ACI-1053575. V.A. acknowledges support from the National Science Foundation Division of Materials Research under award no. 1506707.

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N.M.G., F.B. and M.G. conceived and designed the experiment. F.B. fabricated the heterostructure devices, and conducted Raman, photoluminescence and photocurrent characterization. M.G. and F.B. performed transport and photocurrent measurements and, in cooperation with V.A., conducted data analysis. N.M.G., V.A. and F.B. developed the interlayer transport model. S.S. and R.K.L. conducted DFT band-structure calculations. All authors discussed the results, analysed data and wrote the manuscript.

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Correspondence to Nathaniel M. Gabor.

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Barati, F., Grossnickle, M., Su, S. et al. Hot carrier-enhanced interlayer electron–hole pair multiplication in 2D semiconductor heterostructure photocells. Nature Nanotech 12, 1134–1139 (2017). https://doi.org/10.1038/nnano.2017.203

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