Interface-Tailored Secondary Excitation and Ultrafast Charge/Energy Transfer in Ti 3 C 2 T x -MoS 2 Heterostructure Films
Year: 2025
Type: article
Abstract: High Resolution Image Download MS PowerPoint Slide Charge/energy separation across interfaces of plasmonic materials is vital for minimizing plasmonic losses and enhancing their performance in photochemical and optoelectronic applications. While heterostructures combining plasmonic two-dimensional transition metal carbides/nitrides (MXenes) and semiconducting transition metal dichalcogenides (TMDs) hold significant potential, the mechanisms governing plasmon-induced carrier dynamics at these interfaces remain elusive. Here, we uncover a distinctive secondary excitation phenomenon and an ultrafast charge/energy transfer process in heterostructure films composed of macro-scale Ti 3 C 2 T x and MoS 2 films. Using Rayleigh–Bénard convection and Marangoni effect-induced self-assembly, we fabricate large-scale (square centimeters) Ti 3 C 2 T x and MoS 2 films composed of edge-connected monolayer nanoflakes. These films are flexibly stacked in a controlled sequence to form macroscopic heterostructures, enabling the investigation and manipulation of excited-state dynamics using transient absorption and optical pump-terahertz probe spectroscopy. In the Ti 3 C 2 T x -MoS 2 heterostructure, we observe a secondary excitation in MoS 2 driven by the surface plasmon resonance of Ti 3 C 2 T x . This phenomenon, with a characteristic rise time constant of ∼70 ps, is likely facilitated by acoustic phonon recycling across the interface. Further interfacial thermal transport engineering─achieved by tailoring the sequence and combination of interfaces in trilayer heterostructures─allows extending the characteristic time to ∼175 ps. Furthermore, we identify a sub-150 fs ultrafast charge/energy transfer process from Ti 3 C 2 T x to MoS 2 . The transfer efficiency is strongly dependent on the excitation photon energy, resulting in amplified photoconductivity in MoS 2 by up to ∼180% under 3.10 eV excitation. These insights are crucial for developing plasmonic MXene-based heterostructures, paving the way for advancements in photochemical and optoelectronic applications.
DOI: 10.1021/jacs.5c01826
Institutions: Center for Advancing Electronics Dresden, Technische Universität Dresden, University of Alicante, Instituto de Ciencia de Materiales de Madrid, Politecnico di Milano, Max Planck Institute of Microstructure Physics, Max Planck Institute for Polymer Research, Italian Institute of Technology, Center for Nano Science and Technology, Dresden Center for Nanoanalysis, Utrecht University, Politecnico di Torino
Language: English
Subfield: Materials Chemistry
Field: Materials Science
Domain: Physical Sciences
Open Access status: hybrid
Estimated APC paid: $4,500
Funders: Universidad de Alicante, Politecnico di Torino, Ministerio de Ciencia, Innovación y Universidades, European Commission, Deutsche Forschungsgemeinschaft, Technische Universität Dresden, China Scholarship Council, HORIZON EUROPE Framework Programme, H2020 Future and Emerging Technologies, HORIZON EUROPE Digital, Industry and Space, HORIZON EUROPE European Innovation Council, HORIZON EUROPE European Research Council, Ministerio de Universidades, NextGenerationEU
Awards: G145958901, MULTI-ELECTRON PROCESSES FOR LIGHT DRIVEN ELECTRODES AND ELECTROLYTES IN CONVERSION AND STORAGE OF SOLAR ENERGY, Graphene, MXene and ionic liquid-based sustainable supercapacitor, G2036493699, G2210096415, G2333345521, SFB 1415: Chemie der synthetischen zweidimensionalen Materialien, G2460755258, G3391785330, G3461059926, Engineering of bacteria to see light, Developing New 2D Materials and Heterostructures for Printed Digital Devices, G3803364461, G423459364, G4262022988, G42699959, G4344090363, G505403199, SeLf-powered self-rEshaping Autarkic skin For wireless motes - LEAF, G5378338472, G575692854, G6131097486, MULTI-ELECTRON PROCESSES FOR LIGHT DRIVEN ELECTRODES AND ELECTROLYTES IN CONVERSION AND STORAGE OF SOLAR ENERGY, Graphene, MXene and ionic liquid-based sustainable supercapacitor, G7621391830, G7687122804, G7806810045, Developing New 2D Materials and Heterostructures for Printed Digital Devices, G892739404, G909203908
OpenAlex ID: W4408234841