Modulating nonequilibrium electron–phonon interactions and energy relaxation in MXenes by surface-anchored Mo3S7 nanoclusters

Abstract Electron–phonon (e–ph) interactions govern photoinduced nonequilibrium dynamics of MXenes, determining hot-carrier relaxation and parasitic heat accumulation. However, strategies to deliberately modulate these interactions through chemical control, together with mechanistic understanding, remain underexplored. Here, we demonstrate the effective modulation of nonequilibrium e–ph interactions in Ti 3 C 2 T x MXene via surface-anchored Mo 3 S 7 nanoclusters, which introduce a rapid energy harvesting pathway competing with intrinsic e–ph relaxation. Using mild ligand substitution, Mo 3 S 7 nanoclusters are densely and homogenously anchored onto Ti 3 C 2 T x via coordination bonding between Mo centers and O-terminations. Femtosecond transient absorption and optical-pump terahertz-probe spectroscopy reveal an ultrafast, sub-100 fs nonthermal electron and/or energy extraction, with efficiency increasing from ~28.6 % at 1.55 eV to ~38.2 % at 3.88 eV. This excitation-energy-dependent enhancement is enabled by improved energetic alignment between hot electrons in Ti 3 C 2 T x and the conduction-band manifold of Mo 3 S 7 . The competitive depletion of nonthermal electrons suppresses coherent A 1g phonon excitation, reducing effective e–ph interactions. Our study offers a viable strategy for modulating e–ph interactions in MXenes, advancing hot carrier relaxation and thermal management in next-generation optoelectronic devices.

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Publication Details

Journal
Nature Communications
Published
2026-07-16
DOI
https://doi.org/10.1038/s41467-026-75614-4
Primary Topic
MXene and MAX Phase Materials
Type
article
Field-Weighted Citation Impact
0.00

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article

Modulating nonequilibrium electron–phonon interactions and energy relaxation in MXenes by surface-anchored Mo3S7 nanoclusters

Kornelius Nielsch, Jingwei Du, Giuseppe Maria Paternò, Mischa Bonn et al.
Nature Communications
MXene and MAX Phase Materials
article

Modulating nonequilibrium electron–phonon interactions and energy relaxation in MXenes by surface-anchored Mo3S7 nanoclusters

Kornelius Nielsch, Jingwei Du, Giuseppe Maria Paternò, Mischa Bonn, Minghao Yu, Shuai Fu, Eva A. A. Pogna, Dongqi Li, Rafael Muñoz‐Mármol, Valentino Romano, Xingyuan Chu, Andrea Iudica, Xinliang Feng, Xiaodong Li, Jiaxu Zhang, Pengfei Cao, Juliane Scheiter, Zijie Xiao, Nicolás Pérez, Lei Gao, Francesco Scottognella
article en

Abstract

Abstract Electron–phonon (e–ph) interactions govern photoinduced nonequilibrium dynamics of MXenes, determining hot-carrier relaxation and parasitic heat accumulation. However, strategies to deliberately modulate these interactions through chemical control, together with mechanistic understanding, remain underexplored. Here, we demonstrate the effective modulation of nonequilibrium e–ph interactions in Ti 3 C 2 T x MXene via surface-anchored Mo 3 S 7 nanoclusters, which introduce a rapid energy harvesting pathway competing with intrinsic e–ph relaxation. Using mild ligand substitution, Mo 3 S 7 nanoclusters are densely and homogenously anchored onto Ti 3 C 2 T x via coordination bonding between Mo centers and O-terminations. Femtosecond transient absorption and optical-pump terahertz-probe spectroscopy reveal an ultrafast, sub-100 fs nonthermal electron and/or energy extraction, with efficiency increasing from ~28.6 % at 1.55 eV to ~38.2 % at 3.88 eV. This excitation-energy-dependent enhancement is enabled by improved energetic alignment between hot electrons in Ti 3 C 2 T x and the conduction-band manifold of Mo 3 S 7 . The competitive depletion of nonthermal electrons suppresses coherent A 1g phonon excitation, reducing effective e–ph interactions. Our study offers a viable strategy for modulating e–ph interactions in MXenes, advancing hot carrier relaxation and thermal management in next-generation optoelectronic devices.

Nature Communications
University of Alicante (ES), Forschungszentrum Jülich (DE), Politecnico di Torino (IT), Ernst Ruska Centre (DE), Leibniz Institute for Solid State and Materials Research (DE), Italian Institute of Technology (IT), Max Planck Institute of Microstructure Physics (DE), Max Planck Institute for Polymer Research (DE), Istituto di Fotonica e Nanotecnologie (IT), Center for Nano Science and Technology (IT), Center for Advancing Electronics Dresden (DE), Technische Universität Dresden (DE), Politecnico di Milano (IT)
Universidad de Alicante, European Commission, Deutsche Forschungsgemeinschaft, Technische Universität Dresden, China Scholarship Council, HORIZON EUROPE Framework Programme, Deutsches Elektronen-Synchrotron
Affordable and clean energy
Openalex Percentile: Top 19%
MXene and MAX Phase Materials
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