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Area of Science:

  • Materials Science
  • Quantum Mechanics
  • Solid-State Physics

Background:

  • Nonadiabatic carrier-lattice interactions are crucial for energy transfer in materials.
  • Understanding these interactions at the atomic scale is vital for advancing microelectronics.
  • Electron-phonon coupling significantly influences material properties and performance.

Purpose of the Study:

  • To investigate ultrafast carrier-lattice dynamics in titanium-carbide MXenes.
  • To elucidate the role of nonadiabatic electron-phonon coupling in material relaxation processes.
  • To establish a framework for probing and controlling these interactions with site and orbital specificity.

Main Methods:

  • Combined attosecond core-level transient absorption spectroscopy with many-body theory.
  • Utilized phonon-driven changes in carrier localization to modulate local field effects (LFEs).
  • Analyzed carrier-, site-, and orbital-specific absorption signatures.

Main Results:

  • Identified nonadiabatic electron-phonon coupling as the driver of ultrafast relaxations.
  • LFEs provided sensitive fingerprints of electron-phonon coupling strength across the phonon spectrum.
  • Observed a breakdown of the Born-Oppenheimer approximation: electrons lagged lattice oscillations by 32 ± 8 fs, while holes responded almost instantaneously (7 ± 7 fs).

Conclusions:

  • Established a novel framework for probing and controlling nonadiabatic carrier-phonon interactions.
  • Demonstrated the ability to achieve orbital and site specificity in analyzing these interactions.
  • Provided fundamental insights into energy transfer mechanisms limiting microelectronic performance.