Interfering with interference

Solomon, Gemma C.

doi:10.1038/nchem.2314

Cited by 10 publications

(10 citation statements)

References 8 publications

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“…[18][19]45 Upon photoexcitation, an electron is transferred from the porphyrin to the C60, forming a charge-separated state, which will later recombine to generate the initial state. 46 It is obvious here that the CS is quite efficient because the electron received by C60…”

Section: Resultsmentioning

confidence: 99%

Controllable Charge-Transfer Mechanism at Push–Pull Porphyrin/Nanocarbon Interfaces

et al. 2019

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Ultrafast charge transfer at the interfaces between 5,15-donor-acceptor push-pull porphyrins (Por-tBu and Por-OC8) and nanocarbon materials in the form of fullerene (C60) and graphene carboxylate (GC) are investigated using femtosecond (fs) pump-probe spectroscopy with broadband capabilities. The strong photoluminescence (PL) quenching of the porphyrin indicates electron and/or energy transfer from the photoexcited porphyrin to the nanocarbon materials. More interestingly, the Stern-Volmer plots of PL quenching shows linear and nonlinear patterns upon increasing the concentration of GC or C60 in the porphyrin solution, respectively, clearly indicating static and a combination of static and dynamic quenching at the interfaces with these nanocarbon materials. Using femtosecond transient absorption (TA) spectroscopy, ultrafast electron transfer from a singlet-excited porphyrin to the nanocarbon materials is clearly identified by the fast ground state bleach recovery and the formation of cation radical species. Furthermore, a fs-TA study revealed that both porphyrins show very long-lived ground state bleach (GSB) and excited state absorption (ESA), which can be attributed to the triplet-state formation. This work provides new physical insights into the electron transfer process and its driving force in donor-accepter systems that include nanocarbon materials.

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Section: Resultsmentioning

confidence: 99%

Controllable Charge-Transfer Mechanism at Push–Pull Porphyrin/Nanocarbon Interfaces

et al. 2019

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“…For instance, the underlying sources governing the relative stability of polyynic and cumulenic structural forms of pure carbon networks may be probed, [237][238][239][240][241][242][243][244] and new light may potentially be shed on the many ways in which electronic structure influences the transmission of charges through molecules. [245][246][247][248] Hitherto, quantum transport and interference phenomena have typically been rationalized from symmetry arguments in the underlying MO basis, but it is our belief that the shapes and relative contributions of orb-and atom-RDM1s have the potential to further aid in the understanding of a variety of complex relationships between structure and property.…”

Section: Discussionmentioning

confidence: 99%

Mean-Field Density Matrix Decompositions

Eriksen

2020

Preprint

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We introduce new and robust decompositions of mean-field Hartree-Fock (HF) and Kohn-Sham density functional theory (KS-DFT) relying on the use of localized molecular orbitals and physically sound charge population protocols. The new lossless property decompositions, which allow for partitioning 1-electron reduced density matrices into either bond-wise or atomic contributions, are compared to alternatives from the literature with regards to both molecular energies and dipole moments. Besides commenting on possible applications as an interpretative tool in the rationalization of certain electronic phenomena, we demonstrate how decomposed mean-field theory makes it possible to expose and amplify compositional features in the context of machinelearned quantum chemistry. This is made possible by improving upon the granularity of the underlying data. On the basis of our preliminary proof-of-concept results, we conjecture that many of the structure-property inferences in existence today may be further refined by efficiently leveraging an increase in dataset complexity and richness.

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“…Further, the transmission cancellation proven in this paper can be used to also explain the DQI in molecular systems that contain a series of subsystems. If, for instance, the building block is a meta-benzene, we can obtain the zero conductance in biphenyl 7 , and if we use a T-shape as a building block we obtain the 2-3 hard zero in butadiene 34 . One may start also with multi-terminal lattices as pictured in Fig.1.…”

Section: The Arm-chair Zeroes In Graphenementioning

confidence: 99%

“…Finding systems where such property occurs is of both fundamental and practical interest, as in designing of on/off switches, for example. The existence of DQI phenomena has been investigated previously in various quantum dots or molecular systems [1][2][3][4][5][6][7][8][9] . More recently, this topic received renewed attention in connection with the transmission phase lapse of π at the conductance zeroes between the resonances of a quantum dot, arguably one of the longest standing puzzle in mesoscopic physics, whose elucidation spanned thirty years 10,11 .…”

Section: Introductionmentioning

confidence: 99%

Robust conductance zeros in graphene quantum dots and other bipartite systems

2020

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Within the Landauer transport formalism we demonstrate that conductance zeroes are possible in bipartite systems at half-filling when leads are contacted to different sublattice sites. In particular, we investigate the application of this theory to graphene quantum dots with leads in the armchair configuration. The obtained conductance cancellation is robust in the presence of any single-site impurity.

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Interfering with interference

Cited by 10 publications

References 8 publications

Controllable Charge-Transfer Mechanism at Push–Pull Porphyrin/Nanocarbon Interfaces

Controllable Charge-Transfer Mechanism at Push–Pull Porphyrin/Nanocarbon Interfaces

Mean-Field Density Matrix Decompositions

Robust conductance zeros in graphene quantum dots and other bipartite systems

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