1s-intraexcitonic dynamics in monolayer MoS2 probed by ultrafast mid-infrared spectroscopy

Soonyoung Cha, Ji Ho Sung, Sangwan Sim, Jun Park, Hoseok Heo, Moon-Ho Jo () and Hyunyong Choi ()
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Soonyoung Cha: School of Electrical and Electronic Engineering, Yonsei University
Ji Ho Sung: Center for Artificial Low Dimensional Electronic Systems, Institute for Basic Science (IBS), Pohang University of Science and Technology (POSTECH)
Sangwan Sim: School of Electrical and Electronic Engineering, Yonsei University
Jun Park: School of Electrical and Electronic Engineering, Yonsei University
Hoseok Heo: Center for Artificial Low Dimensional Electronic Systems, Institute for Basic Science (IBS), Pohang University of Science and Technology (POSTECH)
Moon-Ho Jo: Center for Artificial Low Dimensional Electronic Systems, Institute for Basic Science (IBS), Pohang University of Science and Technology (POSTECH)
Hyunyong Choi: School of Electrical and Electronic Engineering, Yonsei University

Nature Communications, 2016, vol. 7, issue 1, 1-7

Abstract: Abstract The 1s exciton—the ground state of a bound electron-hole pair—is central to understanding the photoresponse of monolayer transition metal dichalcogenides. Above the 1s exciton, recent visible and near-infrared investigations have revealed that the excited excitons are much richer, exhibiting a series of Rydberg-like states. A natural question is then how the internal excitonic transitions are interrelated on photoexcitation. Accessing these intraexcitonic transitions, however, demands a fundamentally different experimental tool capable of probing optical transitions from 1s ‘bright’ to np ‘dark’ states. Here we employ ultrafast mid-infrared spectroscopy to explore the 1s intraexcitonic transitions in monolayer MoS2. We observed twofold 1s→3p intraexcitonic transitions within the A and B excitons and 1s→2p transition between the A and B excitons. Our results revealed that it takes about 0.7 ps for the 1s A exciton to reach quasi-equilibrium; a characteristic time that is associated with a rapid population transfer from the 1s B exciton, providing rich characteristics of many-body exciton dynamics in two-dimensional materials.

Date: 2016
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DOI: 10.1038/ncomms10768

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