skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Ultrafast Exciton Dissociation and Long-Lived Charge Separation in a Photovoltaic Pentacene–MoS2 van der Waals Heterojunction

Journal Article · · Nano Letters

van der Waals heterojunctions between two-dimensional (2D) layered materials and nanomaterials of different dimensions present unique opportunities for gate-tunable optoelectronic devices. Mixed-dimensional p–n heterojunction diodes, such as p-type pentacene (0D) and n-type monolayer MoS2 (2D), are especially interesting for photovoltaic applications where the absorption cross-section and charge transfer processes can be tailored by rational selection from the vast library of organic molecules and 2D materials. In this work, we study the kinetics of excited carriers in pentacene–MoS2 p–n type-II heterojunctions by transient absorption spectroscopy. These measurements show that the dissociation of MoS2 excitons occurs by hole transfer to pentacene on the time scale of 6.7 ps. In addition, the charge-separated state lives for 5.1 ns, up to an order of magnitude longer than the recombination lifetimes from previously reported 2D material heterojunctions. By studying the fractional amplitudes of the MoS2 decay processes, the hole transfer yield from MoS2 to pentacene is found to be ~50%, with the remaining holes undergoing trapping due to surface defects. In general, the ultrafast charge transfer and long-lived charge-separated state in pentacene–MoS2 p–n heterojunctions suggest significant promise for mixed-dimensional van der Waals heterostructures in photovoltaics, photodetectors, and related optoelectronic technologies.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Argonne-Northwestern Solar Energy Research Center (ANSER)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0001059; DMR-1121262
OSTI ID:
1388150
Journal Information:
Nano Letters, Vol. 17, Issue 1; Related Information: ANSER partners with Northwestern University (lead); Argonne National Laboratory; University of Chicago; University of Illinois, Urbana-Champaign; Yale University; ISSN 1530-6984
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 143 works
Citation information provided by
Web of Science

References (40)

Mixed-dimensional van der Waals heterostructures journal August 2016
Emerging Device Applications for Semiconducting Two-Dimensional Transition Metal Dichalcogenides journal January 2014
Atomically thin resonant tunnel diodes built from synthetic van der Waals heterostructures journal June 2015
Field-Effect Tunneling Transistor Based on Vertical Graphene Heterostructures journal February 2012
Graphene Barristor, a Triode Device with a Gate-Controlled Schottky Barrier journal May 2012
Hybrid, Gate-Tunable, van der Waals p–n Heterojunctions from Pentacene and MoS 2 journal December 2015
Large-Area, Low-Voltage, Antiambipolar Heterojunctions from Solution-Processed Semiconductors journal December 2014
Gate-tunable carbon nanotube-MoS2 heterojunction p-n diode journal October 2013
Picosecond photoresponse in van der Waals heterostructures journal October 2015
Light-emitting diodes by band-structure engineering in van der Waals heterostructures journal February 2015
Photovoltaic Effect in an Electrically Tunable van der Waals Heterojunction journal July 2014
Ultrafast charge transfer in atomically thin MoS2/WS2 heterostructures journal August 2014
Ultrafast Charge Separation and Indirect Exciton Formation in a MoS 2 –MoSe 2 van der Waals Heterostructure journal November 2014
Probing charge transfer excitons in a MoSe 2 –WS 2 van der Waals heterostructure journal January 2015
Observation of long-lived interlayer excitons in monolayer MoSe2–WSe2 heterostructures journal February 2015
Electron transfer and coupling in graphene–tungsten disulfide van der Waals heterostructures journal November 2014
Interlayer Coupling in Twisted WSe 2 /WS 2 Bilayer Heterostructures Revealed by Optical Spectroscopy journal June 2016
Tuning Interlayer Coupling in Large-Area Heterostructures with CVD-Grown MoS 2 and WS 2 Monolayers journal May 2014
Influence of Stoichiometry on the Optical and Electrical Properties of Chemical Vapor Deposition Derived MoS 2 journal September 2014
Rotationally Commensurate Growth of MoS 2 on Epitaxial Graphene journal November 2015
Morphology and Current–Voltage Characteristics of Nanostructured Pentacene Thin Films Probed by Atomic Force Microscopy journal September 2001
Polarized Absorption in Crystalline Pentacene: Theory vs Experiment journal September 2015
Tightly bound trions in monolayer MoS2 journal December 2012
Bandgap, Mid-Gap States, and Gating Effects in MoS 2 journal July 2014
Evidence for Fast Interlayer Energy Transfer in MoSe 2 /WS 2 Heterostructures journal June 2016
Photoluminescence spectroscopy of pure pentacene, perfluoropentacene, and mixed thin films journal February 2012
Photo-Induced Bandgap Renormalization Governs the Ultrafast Response of Single-Layer MoS 2 journal December 2015
Exciton Dynamics in Suspended Monolayer and Few-Layer MoS 2 2D Crystals journal January 2013
Ultrafast studies of carrier relaxation in semiconductors and their microstructures journal January 1989
Singlet Exciton Fission in Polycrystalline Pentacene: From Photophysics toward Devices journal May 2013
Interpretation of the Ultrafast Photoinduced Processes in Pentacene Thin Films journal March 2010
Charge Trapping and Exciton Dynamics in Large-Area CVD Grown MoS 2 journal January 2016
Ultrafast Dynamics of Defect-Assisted Electron–Hole Recombination in Monolayer MoS 2 journal December 2014
Exciton Radiative Lifetimes in Two-Dimensional Transition Metal Dichalcogenides journal March 2015
Exciton Kinetics, Quantum Efficiency, and Efficiency Droop of Monolayer MoS 2 Light-Emitting Devices journal June 2014
Near-unity photoluminescence quantum yield in MoS2 journal November 2015
Atomically Thin MoS2 A New Direct-Gap Semiconductor journal September 2010
Transient optical studies of charge recombination dynamics in a polymer/fullerene composite at room temperature journal October 2002
Band alignment of two-dimensional transition metal dichalcogenides: Application in tunnel field effect transistors journal July 2013
Electron affinity of pentacene thin film studied by radiation-damage free inverse photoemission spectroscopy journal September 2013

Cited By (28)

Modulated interlayer charge transfer dynamics in a monolayer TMD/metal junction journal January 2019
Environmental engineering of transition metal dichalcogenide optoelectronics journal June 2018
Recent Progress and Future Prospects of 2D-Based Photodetectors journal July 2018
The organic–2D transition metal dichalcogenide heterointerface journal January 2018
Ultrafast Dynamics of Charge Transfer and Photochemical Reactions in Solar Energy Conversion journal October 2018
Efficient and Layer-Dependent Exciton Pumping across Atomically Thin Organic-Inorganic Type-I Heterostructures journal August 2018
Interface Characterization and Control of 2D Materials and Heterostructures journal July 2018
Highly mobile charge-transfer excitons in two-dimensional WS 2 /tetracene heterostructures journal January 2018
Mixed-Dimensional 1D ZnO-2D WSe 2 van der Waals Heterojunction Device for Photosensors journal November 2017
High-efficiency energy transfer in perovskite heterostructures journal January 2018
MoS 2 and Perylene Derivative Based Type‐II Heterostructure: Bandgap Engineering and Giant Photoluminescence Enhancement journal December 2019
2D Layered Material-Based van der Waals Heterostructures for Optoelectronics journal January 2018
Nanosculpting of Atomically Thin 2D Materials for Site-Specific Photoluminescence Modulation journal February 2018
Robust type-II band alignment in Janus-MoSSe bilayer with extremely long carrier lifetime induced by the intrinsic electric field journal March 2019
Tailoring the growth and electronic structures of organic molecular thin films journal September 2019
Microsecond charge separation at heterojunctions between transition metal dichalcogenide monolayers and single-walled carbon nanotubes journal January 2019
Identifying the acceptor state in NiO hole collection layers: direct observation of exciton dissociation and interfacial hole transfer across a Fe 2 O 3 /NiO heterojunction journal January 2018
Merits and Challenges of Ruddlesden-Popper Soft Halide Perovskites in Electro-Optics and Optoelectronics journal October 2018
Phase engineering of seamless heterophase homojunctions with co-existing 3R and 2H phases in WS 2 monolayers journal January 2018
Long-lived charge separation in two-dimensional ligand-perovskite heterostructures journal January 2020
Inhomogeneous photocarrier dynamics and transport in monolayer MoS 2 by ultrafast microscopy journal September 2019
Graphene wrinkle effects on molecular resonance states journal March 2018
Engineering graphene and TMDs based van der Waals heterostructures for photovoltaic and photoelectrochemical solar energy conversion journal January 2018
Enhanced two-photon absorption and two-photon luminescence in monolayer MoS 2 and WS 2 by defect repairing journal January 2019
2D–Organic Hybrid Heterostructures for Optoelectronic Applications journal February 2019
Controllable Interlayer Charge and Energy Transfer in Perovskite Quantum Dots/ Transition Metal Dichalcogenide Heterostructures journal September 2019
Chemical vapor deposition growth of two-dimensional heterojunctions journal November 2017
In-situ visualization of hydrogen evolution sites on helium ion treated molybdenum dichalcogenides under reaction conditions journal July 2019