Measuring Photoexcited Free Charge Carriers in Mono- to Few-Layer Transition-Metal Dichalcogenides with Steady-State Microwave Conductivity

Blackburn, Jeffrey L.; Zhang, Hanyu; Myers, Alexis R.; Dunklin, Jeremy R.; Coffey, David C.; Hirsch, Rebecca N.; Vigil-Fowler, Derek W.; Yun, Seok Joon; Cho, Byeong Wook; Lee, Young Hee; Miller, Elisa M.; Rumbles, Garry; Reid, Obadiah G.

doi:10.1021/acs.jpclett.9b03117

Title: Measuring Photoexcited Free Charge Carriers in Mono- to Few-Layer Transition-Metal Dichalcogenides with Steady-State Microwave Conductivity

Journal Article · 01 December 2019 · Journal of Physical Chemistry Letters

DOI: https://doi.org/10.1021/acs.jpclett.9b03117 · OSTI ID:1580328

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^[1]; Myers, Alexis R. ^[2];

^[1]; Coffey, David C. ^[3]; Hirsch, Rebecca N. ^[4]; Vigil-Fowler, Derek W. ^[1];

^[5]; Cho, Byeong Wook ^[6];

^[6];

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National Renewable Energy Lab. (NREL), Golden, CO (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)
Warren Wilson College, Swannanoa, NC (United States)
Univ. of Colorado, Boulder, CO (United States)
Institute for Basic Science (IBS), Suwon (Korea)
Institute for Basic Science (IBS), Suwon (Korea); Sungkyunkwan Univ., Suwon (Korea)

We present that photoinduced generation of mobile charge carriers is the fundamental process underlying many applications, such as solar energy harvesting, solar fuel production, and efficient photodetectors. Monolayer transition-metal dichalcogenides (TMDCs) are an attractive model system for studying photoinduced carrier generation mechanisms in low-dimensional materials because they possess strong direct band gap absorption, large exciton binding energies, and are only a few atoms thick. While a number of studies have observed charge generation in neat TMDCs for photoexcitation at, above, or even below the optical band gap, the role of nonlinear processes (resulting from high photon fluences), defect states, excess charges, and layer interactions remains unclear. In this study, we introduce steady-state microwave conductivity (SSMC) spectroscopy for measuring charge generation action spectra in a model WS₂ mono- to few-layer TMDC system at fluences that coincide with the terrestrial solar flux. Despite utilizing photon fluences well below those used in previous pump-probe measurements, the SSMC technique is sensitive enough to easily resolve the photoconductivity spectrum arising in mono- to few-layer WS₂. By correlating SSMC with other spectroscopy and microscopy experiments, we find that photoconductivity is observed predominantly for excitation wavelengths resonant with the excitonic transition of the multilayer portions of the sample, the density of which can be controlled by the synthesis conditions. Lastly, these results highlight the potential of layer engineering as a route toward achieving high yields of photoinduced charge carriers in neat TMDCs, with implications for a broad range of optoelectronic applications.

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Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1580328

Report Number(s):: NREL/JA-5K00-75256

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 1 Vol. 11; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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