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Mechanisms Underlying a Quantum Superposition Microscope Based on THz-Driven Coherent Oscillations in a Two-Level

Yunpeng Xia1, Likun Wang1, W Ho1,2

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We used terahertz pulses to probe hydrogen molecules (H_{2}) in a scanning tunneling microscope. This revealed H_{2} acting as a two-level system (TLS) through oscillating currents, offering insights into its quantum states.

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Area of Science:

  • Quantum Mechanics
  • Molecular Spectroscopy
  • Surface Science

Background:

  • Scanning tunneling microscopy (STM) enables atomic-scale surface investigations.
  • Terahertz (THz) spectroscopy probes molecular vibrations and electronic transitions.
  • Understanding molecular behavior at surfaces is crucial for catalysis and materials science.

Purpose of the Study:

  • To investigate the quantum dynamics of hydrogen molecules (H_{2}) at a surface using pump-probe measurements.
  • To characterize H_{2} as a two-level system (TLS) under THz excitation.
  • To explore the influence of tip-sample interactions on molecular spectroscopy.

Main Methods:

  • Pump-probe measurements utilizing ultrashort terahertz (THz) pulses.
  • Coupling THz pulses with a scanning tunneling microscope (STM) tunnel junction.
  • Analysis of THz-induced dc tunneling current oscillations.

Main Results:

  • Observed coherent oscillations of the THz-induced dc tunneling current at ~0.5 THz, confirming H_{2} as a two-level system (TLS).
  • Identified two components in the oscillatory signal, reflecting both photon and field aspects of the THz pulses.
  • Evidence of loosely bound states for the upper TLS state through coherent revival of the oscillatory signal.

Conclusions:

  • The study demonstrates THz-driven pump-probe spectroscopy as a method to probe molecular quantum states in STM junctions.
  • Spectroscopic features of H_{2} were analyzed with different tips, providing insights into the TLS of H_{2} at the surface.
  • The findings contribute to understanding light-matter interactions at the nanoscale.