Terahertz radiation has become an important diagnostic tool in the development of new technologies. However, the diffraction limit prevents terahertz radiation (λ ≈ 0.01–3 mm) from being focused to the nanometre length scale of modern devices. In response to this challenge, terahertz scanning probe microscopy techniques based on coupling terahertz radiation to subwavelength probes such as sharp tips have been developed. These probes enhance and confine the light, improving the spatial resolution of terahertz experiments by up to six orders of magnitude. In this Review, we survey terahertz scanning probe microscopy techniques that achieve spatial resolution on the scale of micrometres to ångströms, with particular emphasis on their overarching approaches and underlying probing mechanisms. Finally, we forecast the next steps in the field.
This is a preview of subscription content
Subscribe to Nature+
Get immediate online access to the entire Nature family of 50+ journals
Subscribe to Journal
Get full journal access for 1 year
only $8.25 per issue
All prices are NET prices.
VAT will be added later in the checkout.
Tax calculation will be finalised during checkout.
Get time limited or full article access on ReadCube.
All prices are NET prices.
Jepsen, P. U., Cooke, D. G. & Koch, M. Terahertz spectroscopy and imaging—modern techniques and applications. Laser Photon. Rev. 5, 124–166 (2011).
Ulbricht, R., Hendry, E., Shan, J., Heinz, T. F. & Bonn, M. Carrier dynamics in semiconductors studied with time-resolved terahertz spectroscopy. Rev. Mod. Phys. 83, 543–586 (2011).
Kampfrath, T., Tanaka, K. & Nelson, K. A. Resonant and nonresonant control over matter and light by intense terahertz transients. Nat. Photon. 7, 680–690 (2013).
Joyce, H. J., Boland, J. L., Davies, C. L., Baig, S. A. & Johnston, M. B. A review of the electrical properties of semiconductor nanowires: insights gained from terahertz conductivity spectroscopy. Semicond. Sci. Technol. 31, 103003 (2016).
Dhillon, S. S. et al. The 2017 terahertz science and technology roadmap. J. Phys. D 50, 043001 (2017).
Spies, J. A. et al. Terahertz spectroscopy of emerging materials. J. Phys. Chem. C 124, 22335 (2020).
Ponseca, C. S. Jr., Chábera, P., Uhlig, J., Persson, P. & Sundström, V. Ultrafast electron dynamics in solar energy conversion. Chem. Rev. 117, 10940–11024 (2017).
Lan, Y. et al. Ultrafast correlated charge and lattice motion in a hybrid metal halide perovskite. Sci. Adv. 5, eaaw5558 (2019).
Kužel, P. & Nĕmec, H. Terahertz conductivity in nanoscaled systems: effective medium theory aspects. J. Phys. D 47, 374005 (2014).
Cocker, T. L. et al. Microscopic origin of the Drude-Smith model. Phys. Rev. B 96, 205349 (2017).
Keilmann, F. & Hillenbrand, R. Near-field microscopy by elastic light scattering from a tip. Phil. Trans. R. Soc. Lond. A 362, 787–805 (2004).
Novotny, L. The history of near-field optics. Prog. Opt. 50, 137–180 (2007).
Chen, X. et al. Modern scattering-type scanning near-field optical microscopy for advanced material research. Adv. Mater. 31, 1804774 (2019).
Keiser, G. R. & Klarskov, P. Terahertz field confinement in nonlinear metamaterials and near-field imaging. Photonics 6, 22 (2019).
Kiwa, T., Tonouchi, M., Yamashita, M. & Kawase, K. Laser terahertz-emission microscope for inspecting electrical faults in integrated circuits. Opt. Lett. 28, 2058–2060 (2003).
van der Valk, N. C. J. & Planken, P. C. M. Electro-optic detection of subwavelength terahertz spot sizes in the near field of a metal tip. Appl. Phys. Lett. 81, 1558–1560 (2002).
Adam, A. J. L. et al. Advanced terahertz electric near-field measurements at sub-wavelength diameter metallic apertures. Opt. Express 16, 7407–7417 (2008).
Blanchard, F. & Tanaka, K. Improving time and space resolution in electro-optic sampling for near-field terahertz imaging. Opt. Lett. 41, 4645–4648 (2016).
Knab, J. R., Adam, A. J. L., Shaner, E., Starmans, H. J. A. J. & Planken, P. C. M. Terahertz near-field spectroscopy of filled subwavelength sized apertures in thin metal films. Opt. Express 21, 1101–1112 (2013).
Niessen, K. A. et al. Protein and RNA dynamical fingerprinting. Nat. Commun. 10, 1026 (2019).
Mitrofanov, O. et al. Terahertz pulse propagation through small apertures. Appl. Phys. Lett. 79, 907–909 (2001).
Macfaden, A. J., Reno, J. L., Brener, I. & Mitrofanov, O. 3 μm aperture probes for near-field terahertz transmission microscopy. Appl. Phys. Lett. 104, 011110 (2014).
Kawano, Y. & Ishibashi, K. An on-chip near-field terahertz probe and detector. Nat. Photon. 2, 618–621 (2008).
Mitrofanov, O. et al. Near-field terahertz probes with room-temperature nanodetectors for subwavelength resolution imaging. Sci. Rep. 7, 44240 (2017).
Wächter, M., Nagel, M. & Kurz, H. Tapered photoconductive terahertz field probe tip with subwavelength spatial resolution. Appl. Phys. Lett. 95, 041112 (2009).
Bhattacherya, A. & Gómez Rivas, J. Full vectorial mapping of the complex electric near-fields of THz resonators. APL Photon. 1, 086103 (2016).
Kawata, S. & Inouye, Y. Scanning probe optical microscopy using a metallic probe tip. Ultramicroscopy 57, 313–317 (1995).
Zenhausern, F., Martin, Y. & Wickramasinghe, H. K. Scanning interferometric apertureless microscopy: optical imaging at 10 angstrom resolution. Science 269, 1083–1085 (1995).
Lahrech, A., Bachelot, R., Gleyzes, P. & Boccara, A. C. Infrared-reflection-mode near-field microscopy using an apertureless probe with resolution of λ/600. Opt. Lett. 21, 1315–1317 (1996).
Knoll, B. & Keilmann, F. Near-field probing of vibrational absorption for chemical microscopy. Nature 399, 134–137 (1999).
Hillenbrand, R. & Keilmann, F. Complex optical constants on a subwavelength scale. Phys. Rev. Lett. 85, 3029–3032 (2000).
Knoll, B. & Keilmann, F. Infrared conductivity mapping for nanoelectronics. Appl. Phys. Lett. 77, 3980 (2000).
Hillenbrand, R., Taubner, T. & Keilmann, F. Phonon-enhanced light–matter interaction at the nanometre scale. Nature 418, 159–162 (2002).
Chen, H.-T., Kersting, R. & Cho, G. C. Terahertz imaging with nanometer resolution. Appl. Phys. Lett. 83, 3009–3011 (2003).
Wang, K., Mittleman, D. M., van der Valk, N. C. J. & Planken, P. C. M. Antenna effects in terahertz apertureless near-field optical microscopy. Appl. Phys. Lett. 85, 2715–2717 (2004).
Buersgens, F., Kersting, R. & Chen, H.-T. Terahertz microscopy of charge carriers in semiconductors. Appl. Phys. Lett. 88, 112115 (2006).
von Ribbeck, H.-G. et al. Spectroscopic THz near-field microscope. Opt. Express 16, 3430–3438 (2008).
Huber, A. J., Keilmann, F., Wittborn, J., Aizpurua, J. & Hillenbrand, R. Terahertz near-field nanoscopy of mobile carriers in single semiconductor nanodevices. Nano Lett. 8, 3766–3770 (2008).
Mastel, S. et al. Terahertz nanofocusing with cantilevered terahertz-resonant antenna tips. Nano Lett. 17, 6526–6533 (2017).
Maissen, C., Chen, S., Nikulina, E., Govyadinov, A. & Hillenbrand, R. Probes for ultrasensitive THz nanoscopy. ACS Photon. 6, 1279–1288 (2019).
Siday, T., Hale, L. L., Hermans, R. I. & Mitrofanov, O. Resonance-enhanced terahertz nanoscopy probes. ACS Photon. 7, 596–601 (2020).
Chen, C. et al. Terahertz nanoimaging and nanospectroscopy of chalcogenide phase-change materials. ACS Photon. 7, 3499–3506 (2020).
Giordano, M. C. et al. Phase-resolved terahertz self-detection near-field microscopy. Opt. Express 26, 18423–18435 (2018).
Jacob, R. et al. Intersublevel spectroscopy on single InAs-quantum dots by terahertz near-field microscopy. Nano Lett. 12, 4336–4340 (2012).
Kuschewski, F. et al. Narrow-band near-field nanoscopy in the spectral range from 1.3 to 8.5 THz. Appl. Phys. Lett. 108, 113102 (2016).
Liewald, C. et al. All-electronic terahertz nanoscopy. Optica 5, 159–162 (2018).
Chen, X. et al. THz near-field imaging of extreme subwavelength metal structures. ACS Photon. 7, 687–694 (2020).
Ocelic, N., Huber, A. & Hillenbrand, R. Pseudoheterodyne detection for background-free near-field spectroscopy. Appl. Phys. Lett. 89, 101124 (2006).
Huth, F., Schnell, M., Wittborn, J., Ocelic, N. & Hillenbrand, R. Infrared-spectroscopic nanoimaging with a thermal source. Nat. Mater. 10, 352–355 (2011).
Khatib, O., Bechtel, H. A., Martin, M. C., Raschke, M. B. & Carr, G. L. Far infrared synchrotron near-field nanoimaging and nanospectroscopy. ACS Photon. 5, 2773–2779 (2018).
Moon, K. et al. Subsurface nanoimaging by broadband terahertz pulse nearfield microscopy. Nano Lett. 15, 549–552 (2014).
Stinson, H. T. et al. Imaging the nanoscale phase separation in vanadium dioxide thin films at terahertz frequencies. Nat. Commun. 9, 3604 (2018).
Zhang, J. et al. Terahertz nanoimaging of graphene. ACS Photon. 5, 2645–2651 (2018).
Aghamiri, N. A. et al. Hyperspectral time-domain terahertz nanoimaging. Opt. Express 27, 24231–24242 (2019).
Moon, K. et al. Computed terahertz near-field mapping of molecular resonances of lactose stereo-isomer impurities with sub-attomole sensitivity. Sci. Adv. 9, 16915 (2019).
Eisele, M. et al. Ultrafast multi-terahertz nano-spectroscopy with sub-cycle temporal resolution. Nat. Photon. 8, 841–845 (2014).
Wagner, M. et al. Ultrafast dynamics of surface plasmons in InAs by time-resolved intrared nanospectroscopy. Nano Lett. 14, 4529–4534 (2014).
Yao, Z. et al. Photo-induced terahertz near-field dynamics of graphene/InAs heterostructures. Opt. Express 27, 13611–13623 (2019).
Yang, H. U., Hebestreit, E., Josberger, E. E. & Raschke, M. B. A cryogenic scattering-type scanning near-field optical microscope. Rev. Sci. Instrum. 84, 023701 (2013).
McLeod, A. S. et al. Nanotextured phase coexistence in the correlated insulator V2O3. Nat. Phys. 13, 80–86 (2016).
Lang, D. et al. Infrared nanoscopy down to liquid helium temperatures. Rev. Sci. Instrum. 89, 033702 (2018).
Weng, Q. et al. Imaging of nonlocal hot-electron energy dissipation via shot noise. Science 360, 775–778 (2018).
de Wilde, Y. et al. Thermal radiation scanning tunnelling microscopy. Nature 444, 740–743 (2006).
Komiyama, S. Perspective: nanoscopy of charge kinetics via terahertz fluctuation. J. Appl. Phys. 125, 010901 (2019).
Lin, K.-T., Komiyama, S., Kim, S., Kawamura, K. & Kajihara, Y. A high signal-to-noise ratio passive near-field microscope equipped with a helium-free cryostat. Rev. Sci. Instrum. 88, 013706 (2017).
Chen, J. et al. Optical nano-imaging of gate-tunable graphene plasmons. Nature 487, 77–81 (2012).
Fei, Z. et al. Gate-tuning of graphene plasmons revealed by infrared nano-imaging. Nature 487, 82–85 (2012).
de Oliveira, T. V. A. G. et al. Nanoscale-confined terahertz polaritons in a van der Waals crystal. Adv. Mater. 33, 2005777 (2021).
Alonso-González, P. et al. Acoustic terahertz graphene plasmons revealed by photocurrent nanoscopy. Nat. Nanotechnol. 12, 31–35 (2017).
Lundeberg, M. B. et al. Tuning quantum nonlocal effects in graphene plasmonics. Science 357, 187–191 (2017).
Klarskov, P., Kim, H., Colvin, V. L. & Mittleman, D. M. Nanoscale laser terahertz emission microscopy. ACS Photonics 4, 2676–2680 (2017).
Pizzuto, A., Mittleman, D. M. & Klarskov, P. Laser THz emission nanoscopy and THz nanoscopy. Opt. Express 28, 18778–18789 (2020).
Schumacher, Z. et al. Nanoscale force sensing of an ultrafast nonlinear optical response. Proc. Natl Acad. Sci. USA 117, 19773–19779 (2020).
Cocker, T. L. et al. An ultrafast terahertz scanning tunnelling microscope. Nat. Photon. 7, 620–625 (2013).
Keldysh, L. V. Ionization in the field of a strong electromagnetic wave. Sov. Phys. JETP 20, 1307–1314 (1965).
Yoshioka, K. et al. Real-space coherent manipulation of electrons in a single tunnel junction by single-cycle terahertz electric fields. Nat. Photon. 10, 762–765 (2016).
Cocker, T. L., Peller, D., Yu, P., Repp, J. & Huber, R. Tracking the ultrafast motion of a single molecule by femtosecond orbital imaging. Nature 539, 263–267 (2016).
Yoshida, S. et al. Subcycle transient scanning tunneling spectroscopy with visualization of enhanced terahertz near field. ACS Photon. 6, 1356–1364 (2019).
Peller, D. et al. Sub-cycle atomic-scale forces coherently control a single-molecule switch. Nature 585, 58–62 (2020).
Tian, Y., Yang, F., Guo, C. & Jiang, Y. Recent advances in ultrafast time-resolved scanning tunneling microscopy. Surf. Rev. Lett. 25, 1841003 (2018).
Chen, C. J. Introduction to Scanning Tunneling Microscopy 2nd edn (Oxford Univ. Press, 2008).
Jelic, V. et al. Ultrafast terahertz control of extreme tunnel currents through single atoms on a silicon surface. Nat. Phys. 13, 591–598 (2017).
Luo, Y. et al. Nanoscale terahertz STM imaging of a metal surface. Phys. Rev. B 102, 205417 (2020).
Nguyen, P. H. et al. Coupling terahertz pulses to a scanning tunneling microscope. Phys. Can. 71, 157–160 (2015).
Yoshioka, K. et al. Tailoring single-cycle near field in a tunnel junction with carrier-envelope phase-controlled terahertz electric fields. Nano Lett. 18, 5198–5204 (2018).
Müller, M., Sabanés, N. M., Kampfrath, T. & Wolf, M. Phase-resolved detection of ultrabroadband THz pulses inside a scanning tunneling microscope junction. ACS Photon. 7, 2046–2055 (2020).
Peller, D. et al. Quantitative sampling of atomic-scale electromagnetic waveforms. Nat. Photon. 15, 143–147 (2021).
Wimmer, L. et al. Terahertz control of nanotip photoemission. Nat. Phys. 10, 432–436 (2014).
Du, S., Yoshida, K., Zhang, Y., Hamada, I. & Hirakawa, K. Terahertz dynamics of electron-vibron coupling in single molecules with tunable electrostatic potential. Nat. Photon. 12, 608–612 (2018).
Kang, T., Bahk, Y.-M. & Kim, D.-S. Terahertz quantum plasmonics at nanoscales and angstrom scales. Nanophotonics 9, 435–451 (2020).
Lange, S. L., Noori, N. K., Kristensen, T. M. B., Steenberg, K. & Jepsen, P. U. Ultrafast THz-driven electron emission from metal metasurfaces. J. Appl. Phys. 128, 070901 (2020).
Yarotski, D. A. et al. Ultrafast carrier-relaxation dynamics in self-assembled InAs/GaAs quantum dots. J. Opt. Soc. Am. B 19, 1480–1484 (2002).
Shi, T., Cirac, J. I. & Demler, E. Ultrafast molecular dynamics in terahertz-STM experiments: theoretical analysis using Anderson-Holstein model. Phys. Rev. Res. 2, 033379 (2020).
Amenabar, I. et al. Structural analysis and mapping of individual protein complexes by infrared nanospectroscopy. Nat. Commun. 4, 2890 (2013).
Kravtsov, V., Ulbricht, R., Atkin, J. M. & Raschke, M. B. Plasmonc nanofocused four-wave mixing for femtosecond near-field imaging. Nat. Nanotechnol. 11, 459–464 (2016).
Lang, D. et al. Nonlinear plasmonic response of doped nanowires observed by infrared nanospectroscopy. Nanotechnology 30, 084003 (2019).
Kwok, Y., Chen, G. & Mukamel, S. STM imaging of electron migration in real space and time: a simulation study. Nano Lett. 19, 7006–7012 (2019).
Frankerl, M. & Donarini, A. Spin-orbit interaction induces charge beatings in a lightwave-STM–single molecule junction. Phys. Rev. B 103, 085420 (2021).
Yoshida, S. et al. Terahertz scanning tunneling microscopy for visualizing ultrafast electron motion in nanoscale potential variations. ACS Photon. 8, 315–323 (2021).
Kimura, K. et al. Terahertz-field-driven scanning tunneling luminescence spectroscopy. ACS Photon. 8, 982–987 (2021).
Abdo, M. et al. Variable repetition rate THz source for ultrafast scanning tunneling microscopy. ACS Photon. 8, 702–708 (2021).
Peplow, M. The next big hit in molecule Hollywood. Nature 544, 408–410 (2017).
Geaney, S. et al. Near-field scanning microwave microscopy in the single photon regime. Sci. Rep. 9, 12539 (2019).
Li, S. & Jones, R. R. High-energy electron emission from metallic nanotips driven by intense single-cycle terahertz pulses. Nat. Commun. 7, 13405 (2016).
Matte, D. et al. Extreme lightwave electron field emission from a nanotip. Phys. Rev. Res. 3, 013137 (2021).
Völcker, M., Krieger, W. & Walther, H. Laser-driven scanning tunneling microscope. Phys. Rev. Lett. 66, 1717–1720 (1991).
Rybka, T. et al. Sub-cycle optical phase control of nanotunnelling in the single-electron regime. Nat. Photon. 10, 667–670 (2016).
Garg, M. & Kern, K. Attosecond coherent manipulation of electrons in tunnelling microscopy. Science 367, 411–415 (2020).
Qazilbash, M. M. et al. Mott transition in VO2 revealed by infrared spectroscopy and nano-imaging. Science 318, 1750–1753 (2007).
Fei, Z. et al. Infrared nanoscopy of dirac plasmons at the graphene–SiO2 interface. Nano Lett. 11, 4701–4705 (2011).
Taubner, T., Hillenbrand, R. & Keilmann, F. Nanoscale polymer recognition by spectral signature in scattering infrared near-field microscopy. Appl. Phys. Lett. 85, 5064–5066 (2004).
We thank L. Mester (CIC nanoGUNE BRTA) for the preparation of panel e of the figure in Box 1. T.L.C. acknowledges financial support from the Department of the Navy, Office of Naval Research (ONR award number N00014−19-1-2051) and the Cowen Family Endowment. R.H. acknowledges financial support from the Spanish Ministry of Science, Innovation and Universities (national project number RTI2018-094830-B-100 and project number MDM-2016-0618 of the Marie de Maeztu Units of Excellence Program) and the Basque Government (grant number IT1164-19). F.A.H. acknowledges support from the Natural Sciences and Engineering Research Council of Canada (NSERC), the Canada Foundation for Innovation (CFI) and the Alberta Innovates Technology Futures (AITF) Strategic Chairs Program.
R.H. is a co-founder of Neaspec GmbH, a company producing scattering-type scanning near-field optical microscope systems, such as the ones described in this Review. The remaining authors declare no competing interests.
Peer review information Nature Photonics thanks Mengkun Liu and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
About this article
Cite this article
Cocker, T.L., Jelic, V., Hillenbrand, R. et al. Nanoscale terahertz scanning probe microscopy. Nat. Photon. 15, 558–569 (2021). https://doi.org/10.1038/s41566-021-00835-6
Light: Science & Applications (2022)
Applied Physics B (2022)
Frontiers of Optoelectronics (2022)