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A mode-locked ultrafast laser focused on the tunneling junction of a scanning tunneling microscope (STM) superimposes harmonics of the laser pulse repetition frequency on the DC tunneling current. The power measured at each of the first 200 harmonics (up to 15 GHz) varies inversely as the square of the frequency due to stray capacitance shunting the tunneling junction. Fourier analysis suggests that in the tunneling junction the harmonics have no significant decay up to a frequency of 1/2τ ≈ 33 THz where τ = 15 fs, the laser pulse width. Two different analyses will be presented to model the generation of the frequency comb within the tunneling junction. The first is based on the observed current-voltage characteristics for the nanoscale tunneling junction. The second is a solution of the time-dependent Schrodinger equation for a modulated barrier. Both analyses indicate that optical rectification of the pulsed laser radiation in the tunneling junction causes harmonics of the pulse repetition frequency of the laser and that these harmonics may extend to terahertz frequencies. It appears that the tunneling junction may be used as a sub-nm sized source of terahertz radiation. Transmission and back scattering could not be used but loading of this source by the finite conductivity of the semiconductor would cause a loss varying inversely with the carrier density. Carrier dynamics could be measured by time-domain measurements, and time-averaged carrier profiling, but presumably with finer resolution due to the sub-nm size of the terahertz source.
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Ultrafast state-selective tunneling in two-dimensional semiconductors with a phase- and amplitude-controlled THz-scanning tunneling microscope
THz-pulse driven scanning tunneling microscopy (THz-STM) enables access to the ultrafast quantum dynamics of low-dimensional material systems at simultaneous ultrafast temporal and atomic spatial resolution. State-selective tunneling requires precise amplitude and phase control of the THz pulses combined with quantitative near-field waveform characterization. Here, we employ our state-of-the-art THz-STM with multi-MHz repetition rates, efficient THz generation, and precisely tunable THz waveforms to investigate a single sulfur vacancy in monolayer MoS2. We demonstrate that 2D transition metal dichalcogenides (TMDs) are an ideal platform for near-field waveform sampling by THz cross-correlation. Furthermore, we determine the THz voltage via QEV scans, which measure the THz rectified charge Q as a function of THz field amplitude E and dc bias Vdc. Mapping the complex energy landscape of localized states with a resolution down to 0.01 electrons per pulse facilitates state-selective tunneling to the HOMO and LUMO orbitals of a charged sulfur vacancy.
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- PAR ID:
- 10595151
- Publisher / Repository:
- American Institute of Physics
- Date Published:
- Journal Name:
- APL Materials
- Volume:
- 12
- Issue:
- 5
- ISSN:
- 2166-532X
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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