Tip-enhanced Raman spectroscopy (TERS), tip-enhanced photoluminescence (TEPL), and scanning tunneling microscope-induced luminescence (STML) combine the high spatial resolution of probe microscopies with the spectroscopic capabilities of optical techniques. Here, we describe the upgrade of an ultrahigh vacuum (UHV) variable-temperature scanning probe microscope (VT-SPM) to perform tip-enhanced spectromicroscopy experiments at cryogenic temperatures. The home-made design includes a portable focusing lens (NA=0.45) that allows the simultaneous collection and injection of light from the tip-sample junction while assuring easy tip and sample transfers. We demonstrate the capabilities of our upgrade to resolve electroluminescence (EL), Raman, and TERS spectra using plasmonically active probes (Ag and Au tips) on various surfaces. We are able to observe the vibrational levels of C60 deposited on Ag(111) with a lateral resolution of ∼2 nanometers. Moreover, we use the tunability of the gap plasmon distribution to observe intense anti-Stokes signals of C60, highlighting the spectral sensitivity of the system. This upgrade opens new possibilities for studying surface chemistry, catalysis, and molecular electronics at state-of-the-art spatial and spectral resolutions using accessible SPM systems.•Portable lens holder•In-situ adjustable position•Nanometer-scale vibrational spectroscopy.

Faculty of Mathematics and Physics Charles University; Ke Karlovu 3 CZ12116 Praha 2 Czech Republic

Institute of Organic Chemistry and Biochemistry Czech Academy of Sciences; Flemingovo náměstí 542 2 Praha 6 CZ160 00 Czech Republic

Institute of Physics Czech Academy of Sciences; Cukrovarnická 10 112 Praha 6 CZ16200 Czech Republic

Material Science Institute of Madrid c Sor Juana Inés de la Cruz 3 28049 Spain

Zobrazit více v PubMed

Lee J., Crampton K.T., Tallarida N., Apkarian V.A. Nature. 2019;568:78–82. PubMed

Xu J., Zhu X., Tan S., Zhang Y., Li B., Tian Y., Shan H., Cui X., Zhao A., Dong Z., Yang J., Luo Y., Wang B., Hou J.G. Science. 2021;371:818–822. PubMed

Gutzler R., Garg M., Ast C.R., Kuhnke K., Kern K. Nat. Rev. Phys. 2021;3:441–453.

Kuhnke K., Große C., Merino P., Kern K. Chem. Rev. 2017;117:5174–5222. PubMed

Cahlík A., Müller C.C., Natterer F.D. MethodsX. 2024;13:102828. PubMed PMC

https://scientaomicron.com/en/products-solutions/SPM/VT-SPM-Lab

Xing Y., Bae S., Ritz E., Yang F., Birol T., Capa Salinas A.N., Ortiz B.R., Wilson S.D., Wang Z., Fernandes R.M., Madhavan V. Nature. 2024;631:60–66. PubMed

Liu S., Cirera B., Sun Y., Hamada I., Müller M., Hammud A., Wolf M., Kumagai T. Nano Lett. 2020;20:5879–5884. PubMed PMC

An H., Li J., Liu Y., Xu P., Han S., Liu Y., Chen S., Li S.-Y., Lin C., Pan A. J. Phys. Chem. C. 2024;128:7583–7590.

Liu S., Müller M., Sun Y., Hamada I., Hammud A., Wolf M., Kumagai T. Nano Lett. 2019;19:5725–7731. PubMed PMC

Garg M., Martín-Jiménez A., Pisarra M., Luo Y., Martín F., Kern K. Nat. Photonics. 2022;16:196–202.

Gieseking R.L.M, Lee J., Tallarida N., Ara Apkarian V., Schatz G.C. J. Phys. Chem. Lett. 2018;9:3074–3080. PubMed

de Campos Ferreira R.C., Sagwal A., Doležal J., Canola S., Merino P., Neuman T., Švec M. ACS. Nano. 2024;18:13164–13170. PubMed PMC

Zhang C., Gao B., Chen L.G., Meng Q.S., Yang H., Zhang R., Tao X., Gao H.Y., Liao Y., Dong Z.C. Review of Scientific Instruments. 2011;82 PubMed

Cirera B., Liu S., Park Y., Hamada I., Wolf M., Shiotari A., Kumagai T. Phys. Chem. Chem. Phys. 2024;26:21325–21331. PubMed

Menéndez J., Page J.B. Light Scattering in Solids VIII. Springer Nature; 2006. pp. 27–95.

Cirera B., Litman Y., Lin C., Akkoush A., Hammud A., Wolf M., Rossi M., Kumagai T. Nano Lett. 2022;22:2170–2176. PubMed PMC

Cirera B., Wolf M., Kumagai T. ACS. Nano. 2022;16:16443–16451. PubMed

Meng Q., Zhang J., Zhang Y., Chu W., Mao W., Zhang Y., Yang J., Luo Y., Dong Z., Hou J.G. Sci. Adv. 2024;10:eadl1015. PubMed PMC

Böckmann H., Liu S., Müller M., Hammud A., Wolf M., Kumagai T. Nano Lett. 2019;19:3597–3602. PubMed PMC

Liu S., Wolf M., Kumagai T. Phys. Rev. Lett. 2018;121 PubMed

Kaiser K., Jiang S., Romeo M., Scheurer F., Schull G., Rosławska A. Phys. Rev. Lett. 2024;133 PubMed

Doležal J., Sagwal A., de Campos Ferreira R.C., Švec M. Nano Lett. 2024;24:1629–1634. PubMed PMC