2023
DOI: 10.1021/acs.nanolett.3c00271
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Single-Molecule Continuous-Wave Terahertz Rectification Spectroscopy and Microscopy

Abstract: We report rectification spectroscopy (RS) for single molecules performed with continuous-wave terahertz (CW THz) radiation at the tunneling junction of a scanning tunneling microscope (STM) at 8 K. CW THz-RS serves as a new technique in single-molecule vibrational and magnetic excitation spectroscopy besides inelastic electron tunneling spectroscopy (IETS). By quantitatively studying IETS and THz RS, we show that CW THz induces a sinusoidal bias modulation with amplitude linearly dependent on the THz far-field… Show more

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Cited by 6 publications
(3 citation statements)
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“…Considering: (i) the area per molecule on the surface (as estimated from the calculated geometry optimization), and (ii) the estimated C-AFM tip contact surface (see below), we estimate N, the number of molecules contacted under the C-AFM tip, as follows. As usually reported in literature [13][14][15][16] the contact radius, a, between the C-AFM tip and the SAM surface, and the SAM elastic deformation, δ, are estimated from a Hertzian model: These parameters for the present SAM are not known and, in general, they are not easily determined in such a monolayer material. Thus, we consider the value of an effective Young modulus of the SAM E*SAM ≈ 38 GPa as determined for the "model system" alkylthiol SAMs from a combined mechanic and electron transport study.…”
Section: Loading Force and C-afm Tip Contact Areamentioning
confidence: 99%
See 1 more Smart Citation
“…Considering: (i) the area per molecule on the surface (as estimated from the calculated geometry optimization), and (ii) the estimated C-AFM tip contact surface (see below), we estimate N, the number of molecules contacted under the C-AFM tip, as follows. As usually reported in literature [13][14][15][16] the contact radius, a, between the C-AFM tip and the SAM surface, and the SAM elastic deformation, δ, are estimated from a Hertzian model: These parameters for the present SAM are not known and, in general, they are not easily determined in such a monolayer material. Thus, we consider the value of an effective Young modulus of the SAM E*SAM ≈ 38 GPa as determined for the "model system" alkylthiol SAMs from a combined mechanic and electron transport study.…”
Section: Loading Force and C-afm Tip Contact Areamentioning
confidence: 99%
“…ultrafast electron transfer), from simple H2 to pentacene, nickelocene, for example. [11][12][13] These works have demonstrated their benefit to overcome the diffraction limits allowing to reach simultaneously high spatial and ultrafast temporal resolution affording new insights for nanoscale devices (see a review in Ref. 9).…”
mentioning
confidence: 99%
“…At the nanoscale, the interactions between molecular-based devices and microwave-to-terahertz electromagnetic waves are a fascinating and relatively recent field of research since the beginning of molecular-scale electronics 50 years ago. , As examples, the polarizability of alkyl chains and π-conjugated oligomers in self-assembled monolayers (SAMs) were first measured by combining a dc bias and a microwave signal (around a few to a few tens of GHz) in a rf-STM (radio frequency scanning tunneling microscope) experiment. , The spin resonance of single molecules deposited on surfaces can be probed and manipulated (in UHV and at low temperatures) with a rf-STM, combined with a magnetic field (ESR-STM: electron spin resonance STM). THz waves coupled with a STM (lightwave-driven THz-STM) , was proven to be a powerful approach to study ultrafast dynamics of single molecules (e.g., ultrafast electron transfer), from simple H 2 , pentacene to nickelocene, for example. These works have demonstrated their benefit to overcome the diffraction limits allowing to reach simultaneously high spatial and ultrafast temporal resolution, affording new insights for nanoscale devices (see a review in ref ). However, to the best of our knowledge, none of these works concern the direct measurement of the dynamic conductance of molecular devices in this microwave frequency regime and at room temperature.…”
mentioning
confidence: 99%