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Cited by 20Terahertz technology and applicationsLaser-Matter Interactions and ApplicationsNear-Field Optical Microscopy

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Efficient and Continuous Carrier-Envelope Phase Control for Terahertz Lightwave-Driven Scanning Probe Microscopy

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Allerbeck, Jonas, Kuttruff, Joel, Bobzien, Laric, Huberich, Lysander, Tsarev, Maxim, Schuler, Bruno·2023·ACS Photonics
DOI 10.1021/acsphotonics.3c00555PMC PMC10655500
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Abstract

The fundamental understanding of quantum dynamics in advanced materials requires precise characterization at the limit of spatiotemporal resolution. Ultrafast scanning tunneling microscopy is a powerful tool combining the benefits of picosecond time resolution provided by single-cycle terahertz (THz) pulses and atomic spatial resolution of a scanning tunneling microscope (STM). For the selective excitation of localized electronic states, the transient field profile must be tailored to the energetic structure of the system. Here, we present an advanced THz-STM setup combining multi-MHz repetition rates, strong THz near fields, and continuous carrier-envelope phase (CEP) control of the transient waveform. In particular, we employ frustrated total internal reflection as an efficient and cost-effective method for precise CEP control of single-cycle THz pulses with >60% field transmissivity, high pointing stability, and continuous phase shifting of up to 0.75 π in the far and near field. Efficient THz generation and dispersion management enable peak THz voltages at the tip-sample junction exceeding 20 V at 1 MHz and 1 V at 41 MHz. The system comprises two distinct THz generation arms, which facilitate individual pulse shaping and amplitude modulation. This unique feature enables the flexible implementation of various THz pump-probe schemes, thereby facilitating the study of electronic and excitonic excited-state propagation in nanostructures and low-dimensional materials systems. Scalability of the repetition rate up to 41 MHz, combined with a state-of-the-art low-temperature STM, paves the way toward the investigation of dynamical processes in atomic quantum systems at their native length and time scales.

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Figure 1 Concept and setup. (a) Metallic mirror (Ag) near the diagonal surface of a right-angle polymer prism changes the phase of a THz pulse undergoing total internal reflection. (b) Concept of field-driven tunneling and photoemission sampling of transient THz fields at the tip–sample junction. (c) THz pulses with different CEP enable state-selective tunneling in electronic states of molecules (HOMO and LUMO orbitals) or semiconductors with a conduction band (CB) and valence band (VB). (d) Optical setup as discussed in the main text. The infrared and THz beam paths are sketched in red and blue, respectively. LN: lithium niobate crystal, SH: second harmonic, EOS: electro-optic sampling, LT-STM: low-temperature scanning tunneling microscope, and UHV: ultrahigh vacuum.
Figure 1 Concept and setup. (a) Metallic mirror (Ag) near the diagonal surface of a right-angle polymer prism changes the phase of a THz pulse undergoing total internal reflection. (b) Concept of field-driven tunneling and photoemission sampling of transient THz fields at the tip–sample junction. (c) THz pulses with different CEP enable state-selective tunneling in electronic states of molecules (HOMO and LUMO orbitals) or semiconductors with a conduction band (CB) and valence band (VB). (d) Optical setup as discussed in the main text. The infrared and THz beam paths are sketched in red and blue, respectively. LN: lithium niobate crystal, SH: second harmonic, EOS: electro-optic sampling, LT-STM: low-temperature scanning tunneling microscope, and UHV: ultrahigh vacuum.CC BY · PubMed Central
Figure 2 Amplitude and phase control of the THz waveform measured in the far field. (a) Infrared pump to THz conversion efficiency. The THz peak field scales linearly with pump energies up to 10 μJ. The inset shows the corresponding THz pulse energies measured directly after THz generation and collimation. (b) Electro-optic sampling (EOS) of single-cycle THz pulses generated by optical rectification in lithium niobate (LN) at multi-MHz repetition rates. A slight red shift of the THz spectrum at high repetition rates relates to an increase of the fundamental laser pulse duration. (c) THz field amplitude control enabled by a pair of wiregrid polarizers and different repetition rates: 1, 5, 10, 20, and 41 MHz. A second axis shows an estimate for the peak far-field amplitude at the STM tip calibrated at 1 MHz. (d) Continuous CEP control between 0 and π/2 enabled by frustrated total internal reflection off the polymer prism. An additional π phase flip can be achieved by adding one additional mirror to the beam path.
Figure 2 Amplitude and phase control of the THz waveform measured in the far field. (a) Infrared pump to THz conversion efficiency. The THz peak field scales linearly with pump energies up to 10 μJ. The inset shows the corresponding THz pulse energies measured directly after THz generation and collimation. (b) Electro-optic sampling (EOS) of single-cycle THz pulses generated by optical rectification in lithium niobate (LN) at multi-MHz repetition rates. A slight red shift of the THz spectrum at high repetition rates relates to an increase of the fundamental laser pulse duration. (c) THz field amplitude control enabled by a pair of wiregrid polarizers and different repetition rates: 1, 5, 10, 20, and 41 MHz. A second axis shows an estimate for the peak far-field amplitude at the STM tip calibrated at 1 MHz. (d) Continuous CEP control between 0 and π/2 enabled by frustrated total internal reflection off the polymer prism. An additional π phase flip can be achieved by adding one additional mirror to the beam path.CC BY · PubMed Central
Figure 3 Modeling of the CEP shift. (a) Schematic of the multiple reflection model for the analytical calculation of the CEP phase shift. r and t denote Fresnel amplitude coefficients for reflection and transmission, respectively. k is the number of reflections at the mirror. (b) Analytical calculation of the phase delay as a function of mirror–prism distance for different refractive index materials assuming a monochromatic wave at 0.8 THz. (c) FDTD numerical simulation of the reflected THz pulse with a prism of refractive index of n = 1.43. The dotted line indicates the phase delay of the positive field cycle. (d) THz phase delay measured with PTFE and Zeonex prisms in the experiment and matching analytical calculations. (e) Relative phase change extracted from panel (c) using two methods: (i) tracking the peak field shift and (ii) fitting a single-cycle waveform to the data. (f) Experimental data and FDTD simulation using the CEP fit method. A 50 μm shift of the experimental data in panels (d) and (f) accounts for geometric roughness of the prism.
Figure 3 Modeling of the CEP shift. (a) Schematic of the multiple reflection model for the analytical calculation of the CEP phase shift. r and t denote Fresnel amplitude coefficients for reflection and transmission, respectively. k is the number of reflections at the mirror. (b) Analytical calculation of the phase delay as a function of mirror–prism distance for different refractive index materials assuming a monochromatic wave at 0.8 THz. (c) FDTD numerical simulation of the reflected THz pulse with a prism of refractive index of n = 1.43. The dotted line indicates the phase delay of the positive field cycle. (d) THz phase delay measured with PTFE and Zeonex prisms in the experiment and matching analytical calculations. (e) Relative phase change extracted from panel (c) using two methods: (i) tracking the peak field shift and (ii) fitting a single-cycle waveform to the data. (f) Experimental data and FDTD simulation using the CEP fit method. A 50 μm shift of the experimental data in panels (d) and (f) accounts for geometric roughness of the prism.CC BY · PubMed Central
Figure 4 THz CEP control at the STM tip. (a–d) THz waveform measured as a function of mirror-prism distance in the far field (EOS) and in the optical near field at the STM tip measured by photoemission sampling (PES). The dotted line in panels (a) and (c) indicates the phase shift of the electric field as a guide to the eye. (e) Current–voltage characteristic of photoemission sampling, providing a linear calibration estimate for the THz field indicated by the dashed line. The total THz field was attenuated to 30% so that peak voltages remain in this linear regime. For all PES measurements, the 517 nm gate pulse intensity at the tip was approximately 4.5 nJ (1 mJ/cm2 at a 25 μm spot size). (f) Amplitude spectra of the THz waveform in the far and near field and the amplitude transfer function (PES/EOS amplitude ratio) showing 1/f scaling (dotted line) shown as a guide to the eye. All curves in panel (f) are normalized to unity.
Figure 4 THz CEP control at the STM tip. (a–d) THz waveform measured as a function of mirror-prism distance in the far field (EOS) and in the optical near field at the STM tip measured by photoemission sampling (PES). The dotted line in panels (a) and (c) indicates the phase shift of the electric field as a guide to the eye. (e) Current–voltage characteristic of photoemission sampling, providing a linear calibration estimate for the THz field indicated by the dashed line. The total THz field was attenuated to 30% so that peak voltages remain in this linear regime. For all PES measurements, the 517 nm gate pulse intensity at the tip was approximately 4.5 nJ (1 mJ/cm2 at a 25 μm spot size). (f) Amplitude spectra of the THz waveform in the far and near field and the amplitude transfer function (PES/EOS amplitude ratio) showing 1/f scaling (dotted line) shown as a guide to the eye. All curves in panel (f) are normalized to unity.CC BY · PubMed Central

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Research works printed but not linked: 51

  1. 10.1038/nature19816 · DOI
  2. 10.1038/s41567-019-0745-8 · DOI
  3. 10.1021/acsphotonics.2c00995 · DOI
  4. 10.1021/acsphotonics.3c00584 · DOI
  5. 10.1038/nphoton.2013.151 · DOI
  6. 10.1021/acsphotonics.9b00266 · DOI
  7. 10.1021/acsphotonics.0c01652 · DOI
  8. 10.1021/acsphotonics.0c01572 · DOI
  9. 10.1126/sciadv.abq5682 · DOI
  10. 10.1038/s41566-021-00813-y · DOI
  11. 10.1021/acsphotonics.0c01755 · DOI
  12. 10.1088/1361-648X/abfe21 · DOI
  13. 10.1126/science.abn9220 · DOI
  14. 10.1364/OE.18.012311 · DOI
  15. 10.1007/s00340-015-6315-6 · DOI
  16. 10.1002/adom.201900681 · DOI
  17. 10.1364/OL.386305 · DOI
  18. 10.1364/PRJ.428418 · DOI
  19. 10.1364/OE.457773 · DOI
  20. 10.1038/s41467-021-26656-3 · DOI
  21. 10.1364/OE.26.013876 · DOI
  22. 10.1038/s41467-022-35517-6 · DOI
  23. 10.1364/OL.41.000986 · DOI · Paper page
  24. 10.1021/acs.nanolett.8b02161 · DOI
  25. 10.1103/PhysRevLett.83.3410 · DOI
  26. 10.1364/OL.26.000485 · DOI
  27. 10.1103/PhysRevLett.92.113001 · DOI
  28. 10.1038/nphoton.2016.205 · DOI
  29. 10.1002/adom.202200541 · DOI
  30. 10.1134/S0021364007190046 · DOI
  31. 10.1103/PhysRevB.105.115427 · DOI
  32. 10.1063/5.0144218 · DOI
  33. 10.1038/s41566-020-00720-8 · DOI
  34. 10.1021/acsphotonics.0c00386 · DOI
  35. 10.1364/OE.426228 · DOI
  36. 10.1088/1612-202X/ab4d56 · DOI
  37. 10.1126/science.aat1603 · DOI
  38. Bichon, J.; Pillet, A.; Sklia, A.; Petitprez, D.; Peretti, R.; Eliet, S. In Complex Refractive Index Determination of PTFE, TPX and Polypropylene Windows for TeraHertz Broadband Spectroscopy , 022 47th International Conference on Infrared, Millimeter and Terahertz Waves (IRMMW-THz); IEEE: Delft, Netherlands, 2022. · DOI
  39. 10.1109/ACCESS.2020.2996278 · DOI
  40. 10.12693/APhysPolA.116.585 · DOI
  41. 10.1038/nphys2974 · DOI
  42. 10.1038/nphys4047 · DOI
  43. 10.1038/s41586-020-2620-2 · DOI
  44. 10.1038/s41566-021-00835-6 · DOI
  45. 10.1021/acsami.2c04736 · DOI
  46. 10.1126/science.aae0003 · DOI
  47. 10.1103/PhysRevApplied.11.024034 · DOI
  48. 10.1103/PhysRevLett.124.054801 · DOI
  49. 10.1063/5.0065185 · DOI
  50. 10.1063/1.1656779 · DOI
  51. 10.1063/1.118691 · DOI

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Metadata

Authors
Allerbeck, J., Kuttruff, J., Bobzien, L., Huberich, L., Tsarev, M., & Schuler, B.
Affiliations
  • Empa (CH)
  • University of Konstanz (DE)
Corresponding author
  • Allerbeck, Jonas
  • Schuler, Bruno
ORCID
Venue
ACS Photonics
Publisher
American Chemical Society (ACS)
Published
2023-10-11
Volume
10
Issue
11
Pages
3888-3895
ISSN
2330-4022 (ISSN-L)
DOI
10.1021/acsphotonics.3c00555
PMC
PMC10655500
OpenAlex
W4387540611
Cited by
20
References
1
Citations by year
2026: 6 · 2025: 6 · 2024: 8
FWCI
1.49
Type
journal article
Language
en
Open access
Licence
Locations
  • ACS Photonics (publishedVersion, cc-by)
  • PubMed Central (publishedVersion, cc-by)
  • PubMed (publishedVersion)
  • DORA Empa (Swiss Federal Laboratories for Materials Science and Technology (Empa)) (submittedVersion, cc-by)
  • KOPS (University of Konstanz) (submittedVersion, cc-by)
Funders
  • Deutsche Forschungsgemeinschaft (SFB 1432)
  • H2020 European Research Council (948243)
Topics
  • Physical Sciences › Engineering › Electrical and Electronic Engineering › Terahertz technology and applications
  • Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Laser-Matter Interactions and Applications
  • Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Near-Field Optical Microscopy
Keywords
carrier-envelope phase control, frustrated total internal reflection, single-cycle terahertz pulses, pulse shaping, excitonic dynamics, low-dimensional materials, electronic dynamics

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