Journal
SMALL
Volume 17, Issue 45, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202103400
Keywords
excitons; layered two-dimensional materials; platinum diselenide; transient absorption microscopy; ultrafast exciton dynamics
Categories
Funding
- National Research Foundation of Korea (NRF) through the government of Korea (MSIP) [NRF-2019R1F1A1063457]
- Korea Basic Science Institute under the RD program [C140440]
- Abu Dhabi Department of Education and Knowledge (ADEK) [AARE19-126]
- US National Science Foundation (NSF) [CMMI-1825256]
- Korean Ministry of Trade, Industry and Energy (MOTIE) [P0002397]
- National Research Council of Science & Technology (NST), Republic of Korea [21A01073] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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Strongly bound excitons, characteristic of 2D semiconductors, are observed and theoretically confirmed in mono-, bi-, and tri-layer platinum diselenide (PtSe2) single crystals. The excitons in PtSe2 dominate the transient broadband response, with a redshift in the transient spectrum as the band-gap redshifts the exciton resonance. This study provides novel insights into exciton photophysics in platinum dichalcogenides.
Strongly bound excitons are a characteristic hallmark of 2D semiconductors, enabling unique light-matter interactions and novel optical applications. Platinum diselenide (PtSe2) is an emerging 2D material with outstanding optical and electrical properties and excellent air stability. Bulk PtSe2 is a semimetal, but its atomically thin form shows a semiconducting phase with the appearance of a band-gap, making one expect strongly bound 2D excitons. However, the excitons in PtSe2 have been barely studied, either experimentally or theoretically. Here, the authors directly observe and theoretically confirm excitons and their ultrafast dynamics in mono-, bi-, and tri-layer PtSe2 single crystals. Steady-state optical microscopy reveals exciton absorption resonances and their thickness dependence, confirmed by first-principles calculations. Ultrafast transient absorption microscopy finds that the exciton dominates the transient broadband response, resulting from strong exciton bleaching and renormalized band-gap-induced exciton shifting. The overall transient spectrum redshifts with increasing thickness as the shrinking band-gap redshifts the exciton resonance. This study provides novel insights into exciton photophysics in platinum dichalcogenides.
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