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Area of Science:

  • Quantum Dynamics
  • Materials Science
  • Spectroscopy

Background:

  • Understanding quantum dynamics in advanced materials necessitates characterization at ultimate spatiotemporal resolution.
  • Ultrafast scanning tunneling microscopy (U-STM) integrates picosecond time resolution with terahertz (THz) pulses and STM's atomic spatial resolution.

Purpose of the Study:

  • To present an advanced THz-STM setup for selective excitation of localized electronic states.
  • To enable tailored transient field profiles for specific energetic structures in quantum systems.

Main Methods:

  • Implementation of multi-MHz repetition rates, strong THz near fields, and continuous carrier-envelope phase (CEP) control.
  • Utilizing frustrated total internal reflection for efficient CEP control of single-cycle THz pulses (>60% transmissivity).
  • Employing two distinct THz generation arms for individual pulse shaping and amplitude modulation, enabling flexible THz pump-probe schemes.

Main Results:

  • Achieved peak THz voltages exceeding 20 V at 1 MHz and 1 V at 41 MHz at the tip-sample junction.
  • Demonstrated continuous phase shifting up to 0.75 π in both far and near fields.
  • Enabled scalable repetition rates up to 41 MHz for advanced U-STM investigations.

Conclusions:

  • The developed THz-STM system provides unprecedented spatiotemporal resolution for quantum dynamics studies.
  • Facilitates the investigation of excited-state propagation in nanostructures and low-dimensional materials.
  • Opens new avenues for studying dynamical processes in atomic quantum systems at their native scales.