Designing a mechanically driven spin-crossover molecular switch <i>via</i> organic embedding

Bhandary, Sumanta; Tomczak, Jan M.; Valli, Angelo

doi:10.1039/d1na00407g

Cited by 13 publications

(9 citation statements)

References 53 publications

(72 reference statements)

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“…An unpaired electron in the orbital predominantly contributes to the local moment in CuPc. The presence of the local spin in leads to a weakening of the Cu–N axial bonds, much like in the spin-crossover molecules. ,, The almost completely filled d R subshell and weakened hybridization in minimizes the screening effects, resulting in a sizable screened local moment in CuPc. Such a persisting local moment in CuPc, unlike in other TMPc molecules, is quite similar to the free molecule moment (see Supporting Information) and is hardly impacted by the presence of a surface underneath, as also observed in multiple experiments. ,, …”

Section: Resultsmentioning

confidence: 99%

“…An unpaired electron in the d x y weakening of the Cu−N axial bonds, much like in the spincrossover molecules. 34,52,56 The almost completely filled d R subshell and weakened hybridization in d…”

Section: Resultsmentioning

confidence: 99%

“… 33 A completely different approach for device development has emerged by means of organic embedding of metallo-organic molecules in two-dimensional (2D) systems. 34 Working in the opposite sense, organic molecules have been found to significantly affect the surface magnetization, in both the saturation magnetization and coercivity, of metallic substrates, 35 , 36 even turning conventional nonmagnets to weak ferromagnets, 37 , 38 leading to the field of emergent magnetism.…”

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confidence: 99%

“…Indeed, modification of a surface–molecule interaction has been used to change the magnetic properties of adsorbed molecules, which can give rise, for example, to spin state, − magnetic coupling, , magnetic anisotropy, or Kondo resonance. , Moreover, by coupling surface modification to external triggers, fundamental device functionalities have been demonstrated, such as spin-switches, − spin transistors, − and spin-valves . A completely different approach for device development has emerged by means of organic embedding of metallo-organic molecules in two-dimensional (2D) systems . Working in the opposite sense, organic molecules have been found to significantly affect the surface magnetization, in both the saturation magnetization and coercivity, of metallic substrates, , even turning conventional nonmagnets to weak ferromagnets, , leading to the field of emergent magnetism.…”

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confidence: 99%

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Dynamical Screening of Local Spin Moments at Metal–Molecule Interfaces

et al. 2023

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Transition-metal phthalocyanine molecules have attracted considerable interest in the context of spintronics device development due to their amenability to diverse bonding regimes and their intrinsic magnetism. The latter is highly influenced by the quantum fluctuations that arise at the inevitable metal–molecule interface in a device architecture. In this study, we have systematically investigated the dynamical screening effects in phthalocyanine molecules hosting a series of transition-metal ions (Ti, V, Cr, Mn, Fe, Co, and Ni) in contact with the Cu(111) surface. Using comprehensive density functional theory plus Anderson’s Impurity Model calculations, we show that the orbital-dependent hybridization and electron correlation together result in strong charge and spin fluctuations. While the instantaneous spin moments of the transition-metal ions are near atomic-like, we find that screening gives rise to considerable lowering or even quenching of these. Our results highlight the importance of quantum fluctuations in metal-contacted molecular devices, which may influence the results obtained from theoretical or experimental probes, depending on their possibly material-dependent characteristic sampling time-scales.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

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Dynamical Screening of Local Spin Moments at Metal–Molecule Interfaces

et al. 2023

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“…implying that charge carriers have a finite lifetime τ = ℏ/(2Γ). More sophisticated approximations further include dynamical renormalizations, either limited to low-energies via the quasi-particle weight [39], or account for the full frequency dependence, e.g., within GW [40][41][42] Anderson impurity calculations [43][44][45][46], dynamical mean-field theory [29,47] or its extensions [48][49][50][51].…”

Section: Electron Transport Theorymentioning

confidence: 99%

Resistivity saturation in semi-conducting polyacetylene molecular wires

Valli

Tomczak

2023

Preprint

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Realizing the promises of molecular electronic devices requires an understanding of transport on the nanoscale. Here, we consider a Su-Schrieffer-Heeger model for semi-conducting trans-polyacetylene molecular wires in which we endow charge carriers with a finite lifetime. The aim of this exercise is two-fold: (i) the simplicity of the model allows an insightful numerical and analytical comparison of the Landauer and Kubo linear response formalism; (ii) we distill the prototypical characteristics of charge transport through gapped mesoscopic systems and compare these to bulk semiconductors. We find that both techniques yield a residual differential conduction at low temperatures for contacted polyacetylene chains of arbitrary length—in line with the resistivity saturation in some correlated narrow-gap semiconductors. Quantitative agreement, however, is limited to not too long molecules. Indeed, while the Landauer transmission is suppressed exponentially with the system size, the Kubo response only decays hyperbolically. Our findings inform the choice of transport methodologies for the ab initio modelling of molecular devices.

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Smart bistable coordination complexes

Xiao,

Chen,

Varley

et al. 2024

Smart Molecules

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Smart molecules have attracted increasing attention due to their transformative role in creating the next generation of smart structures and devices. Smart bistable coordination complexes are a class of functional complexes which have two stable states that can be reversibly switched in response to external stimuli. Such bistable molecules play a vital role in various applications, such as sensors, data storage, spintronics, smart windows, optical switches, information encryption and decryption, displays, actuators, etc. Herein, the recent research studies into the development of these smart bistable metal coordination complexes are reviewed. According to the different external stimuli, these smart bistable coordination systems have been classified and summarized, including light‐responsive systems, thermally‐responsive systems, electrically‐responsive systems, mechanically‐responsive systems, and some other cases. These systems are further subdivided according to the changes in signals (e.g., color, fluorescence, spin state, crystalline phase) under external stimuli. The design principles of each type of smart bistable metal complexes as well as their broad and innovative applications are comprehensively described. Finally, the challenges and opportunities in this field are briefly analyzed and discussed.

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Designing a mechanically driven spin-crossover molecular switch via organic embedding

Abstract: Among spin-crossover complexes, Fe-porphyrin (FeP) stands out for molecular spintronic applications: An intricate, yet favourable balance between ligand fields, charge transfer, and the Coulomb interaction makes FeP highly manipulable, while...

Cited by 13 publications

References 53 publications

Dynamical Screening of Local Spin Moments at Metal–Molecule Interfaces

Dynamical Screening of Local Spin Moments at Metal–Molecule Interfaces

Resistivity saturation in semi-conducting polyacetylene molecular wires

Smart bistable coordination complexes

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