Lineshape characterization of excitons in monolayer WS2 by two-dimensional electronic spectroscopy

Guo, Liang; Chen, Chun-An; Zhang, Zhuquan; Monahan, Daniele M.; Lee, Yi-Hsien; Fleming, Graham R.

doi:10.1039/d0na00240b

Lineshape characterization of excitons in monolayer WS₂ by two-dimensional electronic spectroscopy

Journal Article · Tue Apr 21 00:00:00 EDT 2020 · Nanoscale Advances

DOI:https://doi.org/10.1039/d0na00240b· OSTI ID:2470943

Guo, Liang ^[1]; Chen, Chun-An ^[2]; Zhang, Zhuquan ^[3]; Monahan, Daniele M. ^[4]; Lee, Yi-Hsien ^[2]; ^[5]

University of California, Berkeley, CA (United States); Kavli Energy NanoScience Institute, Berkeley, CA (United States); Southern University of Science and Technology (SUSTech), Shenzhen (China)
National Tsing-Hua University, Hsinchu (Taiwan)
Wuhan University (China)
University of California, Berkeley, CA (United States); Kavli Energy NanoScience Institute, Berkeley, CA (United States)
University of California, Berkeley, CA (United States); Kavli Energy NanoScience Institute, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

The optical properties of monolayer transition metal dichalcogenides (TMDCs), an important family of two-dimensional (2D) semiconductors for optoelectronic applications, are dominated by two excitons A (XA) and B (XB) located at K/K's valleys. The lineshape of the excitons is an indicator of the interaction of the excitons with other particles and also largely determines the performance of TMDC-based optoelectronic devices. In this work, we apply 2D electronic spectroscopy (2DES), which enables separation of the intrinsic homogeneous linewidth and the extrinsic inhomogeneous linewidth, to dissect the lineshape of XA in monolayer WS₂. With a home-built broadband optical parametric amplifier, the 2D spectra give the exciton linewidth values for extensive ranges of excitation densities and temperatures, reflecting inter-exciton and exciton–phonon interactions. Meanwhile, the time-domain evolution of the lineshape reveals a similar rate of spectral diffusion to that in quantum wells (QWs) based on III–V semiconductors.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: Ministry of Science and Technology (MOST); National Science Foundation (NSF); USDOE

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 2470943

Journal Information:: Nanoscale Advances, Journal Name: Nanoscale Advances Journal Issue: 6 Vol. 2; ISSN 2516-0230

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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