Local fields reveal atomic-scale nonadiabatic carrier-phonon dynamics

• 成果类型: Article
• 署名作者: Neb, Sergej; Shin, Dong-bin; Burri, Florence; Hollm, Marko; de Vos, Erik W.; Kuznetsov, Denis A.; Muller, Christoph R.; Fedorov, Alexey; Sato, Shunsuke A.; Rubio, Angel; Gallmann, Lukas; Keller, Ursula
• 署名单位: Swiss Federal Institutes of Technology Domain; ETH Zurich; Gwangju Institute of Science & Technology (GIST); Swiss Federal Institutes of Technology Domain; ETH Zurich; Max Planck Society; Tohoku University; Simons Foundation; Flatiron Institute
• 刊物名称: SCIENCE
• ISSN/ISSBN: 0036-8075; 1095-9203
• DOI: 10.1126/science.aea1523
• 发表日期: 2026-01-01
• 页码: 75-78
• 关键词: EXCITATION

摘要

Understanding nonadiabatic carrier-lattice interactions at the atomic scale remains a fundamental challenge, yet these processes govern energy transfer in materials and ultimately set limits in microelectronics. We combined attosecond core-level transient absorption spectroscopy with many-body theory to uncover how nonadiabatic electron-phonon coupling drives ultrafast relaxations in a titanium-carbide MXene. Phonon-driven changes in carrier localization modulated local field effects (LFEs), yielding carrier-, site-, and orbital-specific absorption signatures. LFEs served as sensitive fingerprints of electron-phonon coupling strength across the phonon spectrum and revealed a breakdown of the Born-Oppenheimer approximation: Electrons lagged lattice oscillations by 32 +/- 8 femtoseconds, whereas holes responded almost instantaneously (7 +/- 7 femtoseconds). Our results establish a framework for probing and controlling nonadiabatic carrier-phonon interactions with orbital and site specificity.