2022
DOI: 10.1038/s41586-022-04401-0
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Orbital-resolved visualization of single-molecule photocurrent channels

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Cited by 40 publications
(29 citation statements)
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“…To explain such a bias-polarity dependence, for μ t,s > ε e > ε g > μ s,t , the current is then given by I normalt = true{ true 2 e Γ te Γ se / false( normalΓ te + 2 normalΓ se false) for Δ V < 0 2 e Γ te Γ se / false( 2 normalΓ te + normalΓ se false) for Δ V > 0 as discussed in previous studies and I s = − I t . The currents calculated with eq are consistent with the numerical results [Figure (a)], indicating that the electrical rectification occurs as a result of an interplay between Coulomb repulsion and asymmetric molecule–electrode coupling, and similar conditions have been realized in a recent experiment . Hence the bias-polarity-dependent squeezing is robust with respect to the external laser field.…”
supporting
confidence: 89%
See 1 more Smart Citation
“…To explain such a bias-polarity dependence, for μ t,s > ε e > ε g > μ s,t , the current is then given by I normalt = true{ true 2 e Γ te Γ se / false( normalΓ te + 2 normalΓ se false) for Δ V < 0 2 e Γ te Γ se / false( 2 normalΓ te + normalΓ se false) for Δ V > 0 as discussed in previous studies and I s = − I t . The currents calculated with eq are consistent with the numerical results [Figure (a)], indicating that the electrical rectification occurs as a result of an interplay between Coulomb repulsion and asymmetric molecule–electrode coupling, and similar conditions have been realized in a recent experiment . Hence the bias-polarity-dependent squeezing is robust with respect to the external laser field.…”
supporting
confidence: 89%
“…Moreover, the emitted light from the molecular excitonic mode can also be squeezed, along with the plasmon mode. Our results are of immediate relevance to STM single molecular junctions aiming to detect and control plasmon-enhanced light–matter interactions and take an important step toward the realization of quantum information processing using single molecules.…”
mentioning
confidence: 82%
“…These include: X-ray-based spectroscopies such as XAS, XES and XPS, Mössbauer, IR, Raman and surface enhanced Raman spectroscopies in addition to microscopies such as STEM and STM. [13][14][15][16][17][18][19][20][21][22] All of them enable the study of the structure and chemical nature of the catalysts. However, many of these techniques require expensive equipment preventing wider and regular use.…”
Section: Characterisation Of Electronic and Structural Propertiesmentioning
confidence: 99%
“…6−8 Also, the inverse process that is photoexcitation of nanoparticles and molecules and detecting local photocurrents with an STM tip has been demonstrated. 9,10 By using ultrashort laser pulses, optically driven processes can nowadays be studied at femtosecond time and nanometer length scales, opening powerful pathways to probe light−matter interactions at their natural dimensions. 11 Optical experiments based on scanning probe techniques often exploit the large field enhancement that emerges when placing plasmonic materials, e.g., silver and gold, into the cavity.…”
Section: Introductionmentioning
confidence: 99%
“…Luminescence spectroscopy with a scanning tunneling microscope (STM) has evolved to a powerful tool to probe the optical properties of surfaces with a nanometer spatial resolution. It has been successfully employed to investigate the emission response of individual metal particles and semiconductor quantum dots, of defects and impurity atoms in dielectric surfaces, , and of single molecules including their Raman fingerprint. Also, the inverse process that is photoexcitation of nanoparticles and molecules and detecting local photocurrents with an STM tip has been demonstrated. , By using ultrashort laser pulses, optically driven processes can nowadays be studied at femtosecond time and nanometer length scales, opening powerful pathways to probe light–matter interactions at their natural dimensions …”
Section: Introductionmentioning
confidence: 99%