Ultrafast terahertz scattering scanning near-field optical microscope

WANG Youwei; MA Yihang; WANG Jiayi; WANG Ziquan; RAO Xinyu; DAI Mingcong; HUANG Ziyu; WU Xiaojun

doi:10.7498/aps.74.20250211

Abstract

Terahertz (THz) time-domain spectroscopy and imaging techniques on a nanoscale are crucial for material research, device detection, and others. However, traditional far-field THz time-domain spectroscopy faces inherent diffraction limitations, which limits the applications of carrier dynamics analysis that require femtosecond time resolution and nanoscale spatial precision. We present a scattering-type scanning near-field optical microscopy that overcomes these limitations by combining ultrafast THz time-domain spectroscopy with atomic force microscopy (AFM). The utilization of the near-field interaction between the needle tip and the sample surface is demonstrated to facilitate the study of semiconductor materials and devices by using static THz spectroscopy with a lateral spatial resolution of ~60 nm. This, in turn, enables the acquisition of static THz conductivity distributions of the semiconductor materials. Additionally, it facilitates the acquisition of transient conductivity distributions of semiconductor materials and laser THz emission ultrafast via photoexcited transient carrier kinetic processes, which provides substantial support for studying the performances of materials and devices in nanometer spatial resolution, ultrafast time resolution, and THz spectroscopic imaging. The experimental results show that the system has a signal-to-noise ratio as high as 56.34 dB in the static THz time-domain spectral mode, and can effectively extract the fifth-order harmonic signals covering the 0.2–2.2 THz frequency band with a spatial resolution of up to ~60 nm. Carrier excitation and complexation processes in topological insulators are successfully observed by optical pump-THz probe with a time resolution better than 100 fs. Imaging of SRAM samples by the system reveals differences in THz scattering intensity due to non-uniformity in doping concentration, thereby validating its potential application in nanoscale defect detection. This study not only provides an innovative means for studying the nanoscale electrical characterization of semiconductor materials and devices, but also opens a new way for applying the THz technology to interdisciplinary subjects such as nanophotonics and spintronics. In the future, by integrating the superlens technology, optimizing the probe design, and introducing deep learning algorithms, it is expected to further improve the temporal- and spatial-resolution and detection efficiency of the system.

Keywords:

terahertz electromagnetic wave /
scanning near-field optical microscope /
semiconductor materials /
devices

Authors and contacts

School of Electronic and Information Engineering, Beihang University, Beijing 100191, China

Corresponding author: WU Xiaojun, xiaojunwu@buaa.edu.cn

FullText HTML

References

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[51]	Dean P, Valavanis A, Keeley J, Bertling K, Lim Y L, Alhathlool R, Burnett A D, Li L H, Khanna S P, Indjin D, Taimre T, Rakić A D, Linfield E H, Davies A G 2014 J. Phys. D: Appl. Phys. 47 374008 Google Scholar
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Cited By

图 1 超快THz s-SNOM系统示意图, laser为光纤飞秒激光器, SHG为二次谐波转化器, HWP为半波片, OI为光隔离器, M1—M14为光学反射镜, BE为扩束器, S1为分束器, AT为发射光导天线, OAP为离轴抛物面镜, AR为接收光导天线, L1和L2为镜头

Figure 1. Schematic diagram of the ultrafast THz s-SNOM system. Laser represents the fiber femtosecond laser, SHG represents second harmonic trigger, HWP represents half-wave plate, OI represents optical isolator, M1–M14 represent mirror, BE represents beam spreader, S1 represents semi transparent and semi reflective mirror, AT represents transmitter antenna, OAP represents off-axis parabolic mirror, AR represents receiver antenna, L1 and L2 represent lenses.

DownLoad: Full-Size Img PowerPoint

图 2 SNOM针尖原理示意图

Figure 2. Schematic diagram operational principle of the SNOM tip.

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图 3 SRAM样品的高度信息　(a)表面光学照片; (b)样品的三维立体图像; (c) AFM高度形貌

Figure 3. Height information of SRAM sample: (a) Optical photographs of the surface taken with the cantilever; (b) three-dimensional images of the sample; (c) AFM height topography of the sample.

DownLoad: Full-Size Img PowerPoint

图 4 静态THz时域光谱扫描模式示意图　(a)时域波形; (b)频域波形; (c)不同阶数信号峰峰值

Figure 4. Static THz time-domain spectroscopy scanning pattern mapping: (a) Time-domain waveforms; (b) frequency-domain waveforms; (c) peak value of signals at different orders.

DownLoad: Full-Size Img PowerPoint

图 5 样品SRAM的THz散射强度映射及拓扑绝缘体的光泵浦-THz探测响应　(a) THz散射时域波形; (b)同一区域的THz散射强度图; (c)拓扑绝缘体的光泵浦-THz探测时域波形; (d)拓扑绝缘体光激发前THz散射强度图; (e)拓扑绝缘体光激发后散射强度图

Figure 5. THz scattering intensity mapping of SRAM and optical pump-THz probe response of topological insulator: (a) THz scattering time-domain waveforms; (b) THz scattering intensity map of the same region; (c) optical pump-THz probe time-domain waveforms of topological insulator; (d) topological insulator morphology before photoexcitation; (e) topological insulator morphology after photoexcitation.

DownLoad: Full-Size Img PowerPoint

图 6 InAs样品THz发射信号　(a)二阶时域波形; (b)二阶频域波形; (c)高阶时域波形; (d)静态THz时域光谱散射扫描成像图; (e) AFM高度形貌

Figure 6. THz emission signals of the InAs sample: (a) Second-order time-domain waveform; (b) second-order frequency-domain waveform; (c) higher-order time-domain waveforms; (d) static THz time-domain spectral scattering scanning imaging; (e) AFM height topography of the sample.

DownLoad: Full-Size Img PowerPoint

[1]	陈西良, 马明旺, 杨小敏, 杨康, 吉特, 吴胜伟, 朱智勇 2008 物理化学学报 24 1969 Google Scholar Chen X L, Ma M W, Yang X M, Yang K, Ji T, Wu S W, Zhu Z Y 2008 Acta Phys. -Chem. Sin. 24 1969 Google Scholar
[2]	Cocker T L, Jelic V, Hillenbrand R, Hegmann F 2021 Nat. Photon. 15 558 Google Scholar
[3]	Jepsen P U, Cooke D G, Koch M 2011 Laser Photon. Rev. 5 124 Google Scholar
[4]	Ulbricht R, Hendry E, Shan J, Heinz T F, Bonn M 2011 Rev. Mod. Phys. 83 543 Google Scholar
[5]	Kampfrath T, Tanaka K, Nelson, K A 2013 Nat. Photon. 7 680 Google Scholar
[6]	Lloyd-Hughes J 2005 Phys. Rev. B 71 195301 Google Scholar
[7]	Beard M C, Turner G M, Schmuttenmaer C A 2000 Phys. Rev. B 62 15764 Google Scholar
[8]	Xing X, Zhao L T, Zhang Z Y, Liu X K, Zhang K L, Yu Y, Lin X, Chen H Y, Chen J Q, Jin Z M, Xu J H, Ma G H 2017 J. Phys. Chem. C 121 20451 Google Scholar
[9]	Knoll B, Keilmann F, Kramer A, Guckenberger R 1997 Appl. Phys. Lett. 70 2667 Google Scholar
[10]	Lahrech A, Bachelot R, Gleyzes P, Boccara A C 1996 Opt. Lett. 21 1315 Google Scholar
[11]	Knoll B, Keilmann F 1999 Nature 399 134 Google Scholar
[12]	van der Valk N C J, Planken P C M 2002 Appl. Phys. Lett. 81 1558 Google Scholar
[13]	Chen H T, Kersting R, Cho G C 2003 Appl. Phys. Lett. 83 3009 Google Scholar
[14]	Buersgens F, Kersting R, Chen H T 2006 Appl. Phys. Lett. 88 112
[15]	Chen X Z, Liu X, Guo X D, Chen S, Hu H, Nikulina E, Ye X L, Yao Z H, Bechtel H A, Martin M C, Carr G L, Dai Q, Zhuang S L, Hu Q, Zhu Y M, Hillenbrand R, Liu M K, You G J 2020 ACS Photonics 7 687 Google Scholar
[16]	Plankl M, Faria P E Jr, Mooshammer F, Siday T, Zizlsperger M, Sandner F, Schiegl F, Maier S, Huber M A, Gmitra M, Fabian J, Boland J L, Cocker T L, Huber R 2021 Nat. Photon. 15 594 Google Scholar
[17]	Chen S, Leng P L, Konečná A, Modin E, Gutierrez-Amigo M, Vicentini E, Martín-García B, Barra-Burillo M, Niehues I, Maciel Escudero C, Xie X Y, Hueso L E, Artacho E, Aizpurua J, Errea I, Vergniory M G, Chuvilin A, Xiu F X, Hillenbrand R 2023 Nat. Mater. 22 860 Google Scholar
[18]	Cocker T L, Jelic V, Gupta M, Molesky S J, Burgess J A J, de los Reyes G, Titova L V, Tsui Y Y, Freeman M R, Hegmann F A 2013 Nat. Photon. 7 620 Google Scholar
[19]	Eisele M, Cocker T L, Huber M A, Plankl M, Viti L, Ercolani D, Sorba L, Vitiello M S, Huber R 2014 Nat. Photon. 8 841 Google Scholar
[20]	Wu X J, Kong D Y, Hao S B, Zeng Y S, Yu X Q, Zhang B L, Dai M C, Liu S J, Wang J Q, Ren Z J, Chen S, Sang J H, Wang K, Zhang D D, Liu Z K, Gui J Y, Yang X J, Xu Y, Leng Y X, Li Y T, Song L W, Tian Y, Li R X 2023 Adv. Mater. 35 2208947 Google Scholar
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[22]	Seifert T, Jaiswal S, Martens U, Hannegan J, Braun L, Maldonado P, Freimuth F, Kronenberg A, Henrizi J, Radu I, Beaurepaire E, Mokrousov Y, Oppeneer P M, Jourdan M, Jakob G, Turchinovich D, Hayden L M, Wolf M, Münzenberg M, Kläui M, Kampfrath T 2016 Nat. Photon. 10 483 Google Scholar
[23]	Kong D Y, Wu X J, Wang B, Nie T X, Xiao M, Pandey C, Gao Y, Wen L G, Zhao W S, Ruan C J, Miao J G, Li Y T, Wang L 2019 Adv. Opt. Mater. 7 1900487 Google Scholar
[24]	Wang B, Shan S Y, Wu X J, Wang C, Pandey C, Nie T X, Zhao W S, Li Y T, Miao J G, Wang L 2019 Appl. Phys. Lett. 115 121104 Google Scholar
[25]	Chen X H, Wang H T, Wang C, Ouyang C, Wei G S, Nie T X, Zhao W S, Miao J G, Li Y T, Wang L, Wu X J 2021 Adv. Photonics Res. 2 2000099 Google Scholar
[26]	Liu S J, Guo F W, Li P Y, Wei G S, Wang C, Chen X H, Wang B, Zhao W S, Miao J G, Wang L, Xu Y, Wu X J 2022 Adv. Mater. Interfaces 9 2101296 Google Scholar
[27]	Chen X H, Wang H T, Liu H J, Wang C, Wei G S, Fang C, Wang H C, Geng C Y, Liu S J, Li P Y, Yu H M, Zhao W S, Miao J G, Li Y T, Wang L, Nie T X, Zhao J M, Wu X J 2022 Adv. Mater. 34 2106172 Google Scholar
[28]	Liu S J, Lu C H, Fan Z Q, Wang S X, Li P Y, Chen X H, Pan J, Xu Y, Liu Y, Wu X J 2022 Appl. Phys. Lett. 120 172404 Google Scholar
[29]	Li P Y, Liu S J, Liu Z, Li M, Xu H, Xu Y, Zeng H P, Wu X J 2022 Appl. Phys. Lett. 120 201102 Google Scholar
[30]	Klarskov P, Kim H, Colvin V L, Mittleman D M 2017 ACS Photonics 4 2676 Google Scholar
[31]	Pizzuto A, Ma P C, Mittleman D M 2023 Light Sci. Appl. 12 96 Google Scholar
[32]	Hillenbrand R, Abate Y, Liu M, Chen X, Basov D N 2025 Nat. Rev. Mater. 10 285 Google Scholar
[33]	von Ribbeck H G, Brehm M, van der Weide D W, Winnerl S, Drachenko O, Helm M, Keilmann F 2008 Opt. Express 16 3430 Google Scholar
[34]	Siday T, Hale L L, Hermans R I, Mitrofanov O 2020 ACS Photonics 7 596 Google Scholar
[35]	Mastel S, Lundeberg M B, Alonso-González P, Gao Y, Watanabe K, Taniguchi T, Hone J, Koppens F H L, Nikitin A Y, Hillenbrand R 2017 Nano Lett. 17 6526 Google Scholar
[36]	Maissen C, Chen S, Nikulina E, Govyadinov A, Hillenbrand R 2019 ACS Photonics 6 1279 Google Scholar
[37]	Moon Y, Lee H, Lim J, Lee G, Kim J, Han H 2023 AIP Adv. 13 065211 Google Scholar
[38]	Pistore V, Schiattarella C, Viti L, Siday T, Johnston M B, Mitrofanov O, Vitiello M S 2024 Appl. Phys. Lett. 124 221105 Google Scholar
[39]	Cai J H, Dai M C, Chen S, Chen P, Wang J Q, Xiong H T, Ren Z J, Liu S J, Liu Z K, Wan C H, Bai M, Wu X J 2023 Appl. Phys. Rev. 10 041414 Google Scholar
[40]	Huang Z Y, Li J, Li P Y, Du L, Dai M C, Cai J H, Ren Z J, Nie T X, Wu X J 2025 iScience 28 111840 Google Scholar
[41]	Tanaka S, More S D, Murakami J, Itoh M, Fujii Y, Kamada M 2001 Phys. Rev. B 64 155308 Google Scholar
[42]	Maeda N, Hata H, Osada N, Shen Q, Toyoda T, Kuwahara S, Katayama K 2013 Phys. Chem. Chem. Phys. 15 11006 Google Scholar
[43]	Shingai D, Ide Y, Sohn W Y, Katayama K 2018 Phys. Chem. Chem. Phys. 20 3484 Google Scholar
[44]	Huang S Y, Wang C, Xie Y G, Yu B Y, Yan H G 2023 Photonics Insights 2 R03 Google Scholar
[45]	Astratov V N, Sahel Y B, Eldar Y C, Huang L, Ozcan A, Zheludev N, Zhao J, Burns Z, Liu Z, Narimanov E, Goswami N, Popescu G, Pfitzner E, Kukura P, Hsiao Y-T, Hsieh C-L, Abbey B, Diaspro A, LeGratiet A, Bianchini P, Shaked N T, Simon B, Verrier N, Debailleul M, Haeberlé O, Wang S, Liu M, Bai Y, Cheng J-X, Kariman B S, Fujita K, Sinvani M, Zalevsky Z, Li X, Huang G-J, Chu S-W, Tzang O, Hershkovitz D, Cheshnovsky O, Huttunen M J, Stanciu S G, Smolyaninova V N, Smolyaninov I I, Leonhardt U, Sahebdivan S, Wang Z, Luk'yanchuk B, Wu L, Maslov A V, Jin B, Simovski C R, Perrin S, Montgomery P, Lecler S 2023 Laser & Photonics Rev. 17 2200029
[46]	陶伟灏, 赵书浩, 董涵瑾, 张国锋, 杨树明 2024 计量科学与技术 68 76 Google Scholar Tao W H, Zhao S H, Dong H J, Zhang G F, Yang S M 2024 Metro. Sci. Technol. 68 76 Google Scholar
[47]	Park Y, Depeursinge C, Popescu G 2018 Nat. Photon. 12 578 Google Scholar
[48]	Paturzo M, Merola F, Grilli S, Nicola S D, Finizio A, Ferraro P 2008 Opt. Express 16 17107 Google Scholar
[49]	Jiaji L, Alex C M, Yunzhe L, Qian C, Chao Z, Lei T 2019 Adv. Photon. 1 066004
[50]	Lü X, Röben B, Biermann K, Wubs J R, Macherius U, Weltmann K D, van Helden J H, Schrottke L, Grahn H T 2023 Semicond. Sci. Technol. 38 035003 Google Scholar
[51]	Dean P, Valavanis A, Keeley J, Bertling K, Lim Y L, Alhathlool R, Burnett A D, Li L H, Khanna S P, Indjin D, Taimre T, Rakić A D, Linfield E H, Davies A G 2014 J. Phys. D: Appl. Phys. 47 374008 Google Scholar
[52]	Hübers H W, Eichholz R, Pavlov S G, Richter H 2013 J. Infrared Milli. Terahz. Waves 34 325 Google Scholar

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Vol. 74, Issue 14 - 2025-07-20

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