@article{d06e05c04be9460292e5ec61212dc649,
title = "Evidence for the Dominance of Carrier-Induced Band Gap Renormalization over Biexciton Formation in Cryogenic Ultrafast Experiments on MoS2 Monolayers",
abstract = "Transition-metal dichalcogenides (TMDs) such as MoS2 display promising electrical and optical properties in the monolayer limit. Due to strong quantum confinement, TMDs provide an ideal environment for exploring excitonic physics using ultrafast spectroscopy. However, the interplay between collective excitation effects on single excitons such as band gap renormalization/exciton binding energy (BGR/EBE) change and multiexciton effects such biexciton formation remains poorly understood. Using two-dimensional electronic spectroscopy, we observe the dominance of single-exciton BGR/EBE signals over optically induced biexciton formation. We make this determination based on a lack of strong PIA features at T = 0 fs in the cryogenic spectra. By means of nodal line slope analysis, we determine that spectral diffusion occurs faster than BGR/EBE change, indicative of distinct processes. These results indicate that at higher sub-Mott limit fluences, collective effects on single excitons dominate biexciton formation.",
author = "Wood, {Ryan E.} and Lloyd, {Lawson T.} and Fauzia Mujid and Lili Wang and Allodi, {Marco A.} and Hui Gao and Richard Mazuski and Ting, {Po Chieh} and Saien Xie and Jiwoong Park and Engel, {Gregory S.}",
note = "Funding Information: This work was supported by the Vannevar Bush Faculty Fellowship Program (Grant nos. N00014-16-1-2513 and N00014-15-1-0048), the Air Force Office of Scientific Research (AFOSR) (FA9550-18-1-0099 and FA9550-16-1-0347), and the NSF (under grant no. 1900359). This work was also supported by the NSF MRSEC grant programs at the University of Chicago (DMR-1420709) and the Cornell Center for Materials Research (DMR-1719875). R.E.W. acknowledges support from the National Defense Science & Engineering Graduate Fellowship (NDSEG) Program, 32 CFR 168a, funded through the AFOSR and the Department of Defense. F.M. and R.M. acknowledge support from the NSF-GRFP program under grant no. DGE-1746045. M.A.A. acknowledges support from a Yen Postdoctoral Fellowship from the Institute for Biophysical Dynamics at The University of Chicago and from an Arnold O. Beckman Postdoctoral Fellowship from the Arnold and Mabel Beckman Foundation. The authors acknowledge Prof. William Tisdale for useful discussions and thank Dr. Karen M. Watters for scientific editing. Funding Information: This work was supported by the Vannevar Bush Faculty Fellowship Program (Grant nos. N00014-16-1-2513 and N00014-15-1-0048) the Air Force Office of Scientific Research (AFOSR) (FA9550-18-1-0099 and FA9550-16-1-0347), and the NSF (under grant no. 1900359). This work was also supported by the NSF MRSEC grant programs at the University of Chicago (DMR-1420709) and the Cornell Center for Materials Research (DMR-1719875). R.E.W. acknowledges support from the National Defense Science & Engineering Graduate Fellowship (NDSEG) Program, 32 CFR 168a, funded through the AFOSR and the Department of Defense. F.M. and R.M. acknowledge support from the NSF-GRFP program under grant no. DGE-1746045. M.A.A. acknowledges support from a Yen Postdoctoral Fellowship from the Institute for Biophysical Dynamics at The University of Chicago and from an Arnold O. Beckman Postdoctoral Fellowship from the Arnold and Mabel Beckman Foundation. The authors acknowledge Prof. William Tisdale for useful discussions and thank Dr. Karen M. Watters for scientific editing. Publisher Copyright: Copyright {\textcopyright} 2020 American Chemical Society.",
year = "2020",
month = apr,
day = "2",
doi = "10.1021/acs.jpclett.0c00169",
language = "English (US)",
volume = "11",
pages = "2658--2666",
journal = "Journal of Physical Chemistry Letters",
issn = "1948-7185",
publisher = "American Chemical Society",
number = "7",
}