000836896 001__ 836896 000836896 005__ 20210129231125.0 000836896 0247_ $$2doi$$a10.1063/1.4975767 000836896 0247_ $$2ISSN$$a0021-9606 000836896 0247_ $$2ISSN$$a1089-7690 000836896 0247_ $$2WOS$$aWOS:000397312800032 000836896 0247_ $$2Handle$$a2128/18948 000836896 0247_ $$2altmetric$$aaltmetric:13401149 000836896 037__ $$aFZJ-2017-05928 000836896 082__ $$a540 000836896 1001_ $$0P:(DE-HGF)0$$aGaudenzi, R.$$b0 000836896 245__ $$aTransport mirages in single-molecule devices 000836896 260__ $$aMelville, NY$$bAmerican Institute of Physics$$c2017 000836896 3367_ $$2DRIVER$$aarticle 000836896 3367_ $$2DataCite$$aOutput Types/Journal article 000836896 3367_ $$0PUB:(DE-HGF)16$$2PUB:(DE-HGF)$$aJournal Article$$bjournal$$mjournal$$s1502797621_5380 000836896 3367_ $$2BibTeX$$aARTICLE 000836896 3367_ $$2ORCID$$aJOURNAL_ARTICLE 000836896 3367_ $$00$$2EndNote$$aJournal Article 000836896 520__ $$aMolecular systems can exhibit a complex, chemically tailorable inner structure which allows for targeting of specific mechanical, electronic, and optical properties. At the single-molecule level, two major complementary ways to explore these properties are molecular quantum-dot structures and scanning probes. This article outlines comprehensive principles of electron-transport spectroscopy relevant to both these approaches and presents a new, high-resolution experiment on a high-spin single-molecule junction exemplifying these principles. Such spectroscopy plays a key role in further advancing our understanding of molecular and atomic systems, in particular, the relaxation of their spin. In this joint experimental and theoretical analysis, particular focus is put on the crossover between the resonant regime [single-electron tunneling] and the off-resonant regime [inelastic electron (co)tunneling spectroscopy (IETS)]. We show that the interplay of these two processes leads to unexpected mirages of resonances not captured by either of the two pictures alone. Although this turns out to be important in a large fraction of the possible regimes of level positions and bias voltages, it has been given little attention in molecular transport studies. Combined with nonequilibrium IETS—four-electron pump-probe excitations—these mirages provide crucial information on the relaxation of spin excitations. Our encompassing physical picture is supported by a master-equation approach that goes beyond weak coupling. The present work encourages the development of a broader connection between the fields of molecular quantum-dot and scanning probe spectroscopy 000836896 536__ $$0G:(DE-HGF)POF3-141$$a141 - Controlling Electron Charge-Based Phenomena (POF3-141)$$cPOF3-141$$fPOF III$$x0 000836896 588__ $$aDataset connected to CrossRef 000836896 7001_ $$0P:(DE-Juel1)145304$$aMisiorny, M.$$b1 000836896 7001_ $$0P:(DE-HGF)0$$aBurzurí, E.$$b2 000836896 7001_ $$0P:(DE-Juel1)131026$$aWegewijs, M. R.$$b3$$eCorresponding author 000836896 7001_ $$0P:(DE-HGF)0$$avan der Zant, H. S. 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