Ultrafast Singlet Energy Transfer before Fission in a Tetracene/WSe<sub>2</sub> Type II Hybrid Heterostructure

Ye, Lei; Liu, Yanping; Zhou, Qi; Tao, Weijian; Li, Yujie; Wang, Zukun; Zhu, Haiming

doi:10.1021/acs.jpclett.1c02540

Cited by 17 publications

(38 citation statements)

References 47 publications

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“…This result first seems contradictory with the PL lifetime (∼70.9 ns) of 380 nm. Note that the bleach signal in the TA spectrum can be contributed by the population of electrons in the excited states and holes in the ground states . Because of the Cd 2+ triplet emission with lifetime extending to milliseconds (Figures S3 and S5), the XB at 375 nm before t 0 is probably due to the long-lived Cd 2+ triplet states with the hole remaining in VB of Cd-PVK (or called 1 A 1g of Cd 2+ ).…”

Section: Results and Discussionmentioning

confidence: 99%

“…However, type II band alignment is found for Pb 2+ -doped Cd-PVK due to the strong hybridization of Pb and Br orbitals that raises the energy levels of the antibonding orbitals. Although type II band alignment usually promotes charge separation, the large energy offset (∼1 eV) will reduce the rate of hole transfer from the VBM to 1 S 0 of Pb 2+ . As a result, the XB of 375 nm before t 0 remains even for 15% Pb doping level.…”

Section: Results and Discussionmentioning

confidence: 99%

“…Note that the bleach signal in the TA spectrum can be contributed by the population of electrons in the excited states and holes in the ground states. 43 Because of the Cd 2+ triplet emission with lifetime extending to milliseconds (Figures S3 and S5), the XB at 375 nm before t 0 is probably due to the long-lived Cd 2+ triplet states with the hole remaining in VB of Cd-PVK (or called 1 A 1g of Cd 2+ ). However, due to the poor signal-to-noise of Cd-PVK and long-lived species with lifetime beyond the time window of our setup, it is hard to obtain the decay kinetics of excitons.…”

Section: Resultsmentioning

confidence: 99%

“…The fast decay component (∼2 ps) is attributed to the singlet exciton transfer (SET), agreeing well with previously reported work. 43 The slow decay (∼2.8−12.8 ns) is assigned to the triplet exciton transfer (TET) from Cd-PVK host to Sb 3+ dopant (the time constant of slow component is a rough estimate due to the lifetime being longer than the measurement window of our fs-TA setup). 28,47,48 This assignment is also consistent with the fact that both the fast and slow decays become faster with increasing Sb 3+ doping level.…”

Section: Resultsmentioning

confidence: 99%

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Ultrafast Study of Exciton Transfer in Sb(III)-Doped Two-Dimensional [NH₃(CH₂)₄NH₃]CdBr₄ Perovskite

Lian

et al. 2021

ACS Nano

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Antimony-based metal halide hybrids have attracted enormous attention due to the stereoactive 5s2 electron pair that drives intense triplet broadband emission. However, energy/charge transfer has been rarely achieved for Sb3+-doped materials. Herein, Sb3+ ions are homogeneously doped into 2D [NH3(CH2)4NH3]CdBr4 perovskite (Cd-PVK) using a wet-chemical method. Compared to the weak singlet exciton emission of Cd-PVK at 380 nm, 0.01% Sb3+-doped Cd-PVK exhibits intense triplet emission located at 640 nm with a near-unity quantum yield. Further increasing the doping concentration of Sb3+ completely quenches singlet exciton emission of Cd-PVK, concurrently with enhanced Sb3+ triplet emission. Delayed luminescence and femtosecond-transient absorption studies suggest that Sb3+ emission originates from exciton transfer (ET) from Cd-PVK host to Sb3+ dopant, while such ET cannot occur with Pb2+-doped Cd-PVK because of the mismatch of energy levels. In addition, density function theory calculations indicate that the introduced Sb3+ likely replace the Cd2+ ions along with the deprotonation of butanediammonium for charge balance, instead of generating Cd2+ vacancies. This work provides a deeper understanding of the ET of Sb3+-doped Cd-PVK and suggests an effective strategy to achieve efficient triplet Sb3+ emission beyond 0D Cl-based hybrids.

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Section: Results and Discussionmentioning

confidence: 99%

Section: Results and Discussionmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

See 2 more Smart Citations

Ultrafast Study of Exciton Transfer in Sb(III)-Doped Two-Dimensional [NH₃(CH₂)₄NH₃]CdBr₄ Perovskite

Lian

et al. 2021

ACS Nano

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“…[1][2][3][4][5][6][7][8][9] Depending on their density on the substrate and on their physico-chemical characteristics, physisorbed moieties can introduce localized electronic states, [10][11][12] dispersive bands, 7 or a combination thereof. [13][14][15] The electronic structure of the interface results from the level alignment between the organic and inorganic components [16][17][18][19][20] and the hybridization between their electronic wave-functions. 15,[21][22][23][24] As both these effects depend on the intrinsic nature of the building blocks, the need for systematic analyses on the electronic structure of hybrid systems are in high demand.…”

Section: Introductionmentioning

confidence: 99%

Donors, Acceptors, and a Bit of Aromatics: Electronic Interactions of Molecular Adsorbates on hBN and MoS$_2$ Monolayers

Melani,

Guerrero-Felipe,

Valencia

et al. 2022

Preprint

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The design of low-dimensional organic-inorganic interfaces for the next generation of opto-electronic applications requires an in-depth understanding of the microscopic mechanisms ruling electronic interactions in these systems. In this work, we present a first-principles study based on density-functional theory inspecting the structural, energetic, and electronic properties of five molecular donors and acceptors adsorbed on freestanding hexagonal boron nitride (hBN) and molybdenum disulfide (MoS 2 ) monolayers. All considered heterostructures are stable, due to the crucial contribution of dispersion interactions, which are maximized by the overall flat arrangement of the physisorbed molecules on both substrates. The level alignment of the hybrid systems depends on the characteristics of the constituents. On hBN, both type-I and type-II heterostructures may form, depending on the relative energies of the frontier orbitals with respect to the vacuum level. On the other hand, all MoS 2 -based hybrid systems exhibit a type-II level alignment, with the molecular frontier orbitals positioned across the energy gap of the semiconductor. The electronic structure of the hybrid materials is further determined by the formation of interfacial dipole moments and by the wavefunction hybridization between the organic and inorganic constituents. These results provide important indications for the design of novel low-dimensional hybrid materials with suitable characteristics for opto-electronics.

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Two‐dimensional Transition metal Dichalcogenides as an Emerging Platform for Singlet Fission Solar Cells

Jang

Kim

2022

Chemistry An Asian Journal

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Singlet fission, a rapid exciton doubling process via inverse Auger recombination, is recognized as one of the most practical and feasible means for overcoming the Shockley–Queisser limit. Singlet fission solar cells are generally developed by integrating photon downconversion organic semiconductors into conventional photovoltaic devices to break the maximum photovoltaic response of the host semiconductors by virtue of extra triplet excitons. In this regard, proper matching of two different semiconductors and heterointerface engineering are both crucial for highly efficient singlet fission solar cells. Therefore, the aim of this study is to review the prerequisite conditions for efficient triplet transfer at the heterointerfaces and thus highlight the robust spin and valley degrees of freedom of transition metal dichalcogenides with the ultimate goal of stimulating research into next‐generation singlet fission solar cells.

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Ultrafast Singlet Energy Transfer before Fission in a Tetracene/WSe₂ Type II Hybrid Heterostructure

Cited by 17 publications

References 47 publications

Ultrafast Study of Exciton Transfer in Sb(III)-Doped Two-Dimensional [NH₃(CH₂)₄NH₃]CdBr₄ Perovskite

Ultrafast Study of Exciton Transfer in Sb(III)-Doped Two-Dimensional [NH₃(CH₂)₄NH₃]CdBr₄ Perovskite

Donors, Acceptors, and a Bit of Aromatics: Electronic Interactions of Molecular Adsorbates on hBN and MoS$_2$ Monolayers

Two‐dimensional Transition metal Dichalcogenides as an Emerging Platform for Singlet Fission Solar Cells

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Ultrafast Singlet Energy Transfer before Fission in a Tetracene/WSe2 Type II Hybrid Heterostructure

Cited by 17 publications

References 47 publications

Ultrafast Study of Exciton Transfer in Sb(III)-Doped Two-Dimensional [NH3(CH2)4NH3]CdBr4 Perovskite

Ultrafast Study of Exciton Transfer in Sb(III)-Doped Two-Dimensional [NH3(CH2)4NH3]CdBr4 Perovskite

Donors, Acceptors, and a Bit of Aromatics: Electronic Interactions of Molecular Adsorbates on hBN and MoS$_2$ Monolayers

Two‐dimensional Transition metal Dichalcogenides as an Emerging Platform for Singlet Fission Solar Cells

Contact Info

Product

Resources

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Ultrafast Singlet Energy Transfer before Fission in a Tetracene/WSe₂ Type II Hybrid Heterostructure

Ultrafast Study of Exciton Transfer in Sb(III)-Doped Two-Dimensional [NH₃(CH₂)₄NH₃]CdBr₄ Perovskite

Ultrafast Study of Exciton Transfer in Sb(III)-Doped Two-Dimensional [NH₃(CH₂)₄NH₃]CdBr₄ Perovskite