4.8 Article

Unveiling defect -mediated carrier dynamics in monolayer semiconductors by spatiotemporal microwave

Publisher

NATL ACAD SCIENCES
DOI: 10.1073/pnas.2004106117

Keywords

transition-metal dichalcogenides; defects; charge carriers; spatiotemporal dynamics; laser-illuminated microwave impedance; microscopy

Funding

  1. NSF through the Center for Dynamics and Control of Materials, an NSF Materials Research Science and Engineering Center (MRSEC) [DMR-1720595]
  2. NSF MRSEC
  3. US Army Research Office [W911NF-16-1-0276, W911NF-17-1-0190]
  4. Welch Foundation [F-1662, F-1814]
  5. Department of Energy, Basic Energy Science [DE-SC0019398]
  6. King Abdullah University of Science and Technology, Office of Sponsored Research [CRF-2016-2996-CRG5]
  7. American Chemical Society (ACS) [ACS PRF 54717-DNI10]
  8. Office of Basic Energy Sciences, of the US Department of Energy [DE-AC02-05CH11231]
  9. UT-Austin
  10. NSF [EFMA-1542747]
  11. US Army Research Laboratory
  12. U.S. Department of Energy (DOE) [DE-SC0019398] Funding Source: U.S. Department of Energy (DOE)

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The optoelectronic properties of atomically thin transition -metal dichalcogenides are strongly correlated with the presence of de- fects in the materials, which are not necessarily detrimental for certain applications. For instance, defects can lead to an enhanced photoconduction, a complicated process involving charge genera- tion and recombination in the time domain and carrier transport in the spatial domain. Here, we report the simultaneous spatial and temporal photoconductivity imaging in two types of WS 2 mono - layers by laser -illuminated microwave impedance microscopy. The diffusion length and carrier lifetime were directly extracted from the spatial profile and temporal relaxation of microwave signals, respectively. Time -resolved experiments indicate that the critical process for photoexcited carriers is the escape of holes from trap states, which prolongs the apparent lifetime of mobile electrons in the conduction band. As a result, counterintuitively, the long-lived photoconductivity signal is higher in chemical -vapor deposited (CVD) samples than exfoliated monolayers due to the presence of traps that inhibits recombination. Our work reveals the intrinsic time and length scales of electrical response to photoexcitation in van der Waals materials, which is essential for their applications in optoelectronic devices.

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