Ultrafast Charge Transfer and Hybrid Exciton Formation in 2D/0D Heterostructures

Boulesbaa, Abdelaziz; Wang, Kai; Mahjouri-Samani, Masoud; Tian, Mengkun; Puretzky, Alexander A.; Ivanov, Ilia; Rouleau, Christopher M.; Xiao, Kai; Sumpter, Bobby G.; Geohegan, David B.

doi:10.1021/jacs.6b08883

Ultrafast Charge Transfer and Hybrid Exciton Formation in 2D/0D Heterostructures

Journal Article · Tue Oct 18 00:00:00 EDT 2016 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.6b08883· OSTI ID:1334433

Boulesbaa, Abdelaziz ^[1]; Wang, Kai ^[1]; Mahjouri-Samani, Masoud ^[1]; Tian, Mengkun ^[1]; Puretzky, Alexander A. ^[1]; Ivanov, Ilia ^[1]; Rouleau, Christopher M. ^[1]; Xiao, Kai ^[1]; Sumpter, Bobby G. ^[1]; Geohegan, David B. ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)

We report that photoinduced interfacial charge transfer is at the heart of many applications, including photovoltaics, photocatalysis, and photodetection. With the emergence of a new class of semiconductors such as monolayer two-dimensional transition metal dichalcogenides (2D-TMDs), charge transfer at the 2D/2D heterojunctions attracted several efforts due to the remarkable optical and electrical properties of 2D-TMDs. Unfortunately, in 2D/2D heterojunctions, for a given combination of two materials, the relative energy band alignment and the charge transfer efficiency are locked. Due to their large variety and broad size tunability, semiconductor quantum dots (0D-QDs) interfaced with 2D-TMDs may become an attractive heterostructure for optoelectronic applications. Here, we incorporate femtosecond pump-probe spectroscopy to reveal the sub-45 fs charge transfer at a 2D/0D heterostructure composed of tungsten disulfide monolayers (2D-WS₂) and a single layer of cadmium selenide (CdSe)/zinc sulfide (ZnS) core/shell 0D-QDs. Furthermore, ultrafast dynamics and steady-state measurements suggested that following electron transfer from the 2D to the 0D, hybrid excitons (HXs), wherein the electron resides in the 0D and hole resides in the 2D-TMD monolayer, are formed with a binding energy on the order of ~140 meV, which is several times lower than that of tightly bound excitons in 2D-TMDs.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1334433

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 44 Vol. 138; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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