Tuning the magnetic properties of a diamagnetic di-Blatter's zwitterion to antiferro- and ferromagnetically coupled diradicals

Khurana, Rishu; Bajaj, Ashima; Ali, Md. Ehesan

doi:10.1039/d1cp04807d

Cited by 14 publications

(19 citation statements)

References 102 publications

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“…To further validate the OSS character, the spin-squared value hS 2 i in the BS state and radicaloid character (y), which are used as the descriptors of diradical character of a molecule, 62,63 are presented in Fig. 1b and d.…”

Section: Electronic Structure Of Isolated Moleculesmentioning

confidence: 99%

Anti-ohmic nanoconductors: myth, reality and promise

Bajaj¹,

Ali²

2023

Phys. Chem. Chem. Phys.

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Section: Electronic Structure Of Isolated Moleculesmentioning

confidence: 99%

Anti-ohmic nanoconductors: myth, reality and promise

Bajaj¹,

Ali²

2023

Phys. Chem. Chem. Phys.

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“…To further validate the OSS character, spin-squared value <S 2 > in BS state and radicaloid character (y), which are used as the descriptors of diradical character of a molecule 61,62 are presented in Figure 1b acene and n=10 cumulene indicates CSS ground state. Afterwards, the <S 2 > value shows a regular increase with the increasing n for both the series.…”

Section: Electronic Structure Of Isolated Moleculesmentioning

confidence: 99%

Anti-ohmic Nanoconductors: Myth, Reality and Promise

Bajaj

Ali

2023

Preprint

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The recent accomplishments in the design of molecular nanowires characterised by an increasing conductance with length has embarked the origin of extraordinary new family of molecular junctions referred to as "anti-ohmic" wires. Herein, this highly desirable, non-classical behavior, has been examined for the longer enough molecules exhibiting pronounced diradical character in their ground state within the unrestricted DFT formalism with spin and spatial symmetry breaking. We demonstrate that highly conjugated acenes signals higher resistance in open-shell singlet (OSS) configuration as compared to their closed-shell counterparts. This anomaly has been further put to proof for experimentally certified cumulene wires, which reveals phenomenal modulation in the transport characteristics such that an increasing conductance is observed in closed-shell limit, while higher cumulenes in OSS ground state yields a regular decay of conductance.

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“…This overestimation of J, as predicted by Noodleman's and Yamaguchi's approaches, has been consistently reported in the literature, particularly for organic diradical systems. [65][66][67] Consequently, scaling factors of 0.3-0.5 have been employed to align with experimental J values. [68][69][70] As demonstrated in Figure S27, Tables S1 approach.…”

Section: Benchmark Of Broken-symmetry Dft Functionals For Triangulene...mentioning

confidence: 99%

Predicting Magnetic Coupling and Spin-Polarization Energy in Triangulene Analogues

Sun

Heine

2023

Preprint

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Triangulene and its analogue metal-free magnetic systems have garnered increasing attention since their discovery. Predicting the magnetic couplings and spin polarization energy with quantitative accuracy is beyond the predictive power of today’s density-functional theory (DFT) due to their intrinsic multi-reference character. Herein, we create a benchmark dataset of 25 magnetic systems with non-local spin densities, including the triangulene monomer, dimer, and their analogues. We calculate the magnetic coupling (J) and spin-polarization energy (ΔEspin) of these systems using complete active space self-consistent field (CASSCF) and coupled cluster methods as high-quality reference values. This reference data is then used to benchmark 22 DFT functionals commonly used in material science. Our results show that, while some functionals consistently correctly predict the qualitative character of the ground state, achieving quantitative accuracy with small relative errors is currently not feasible. PBE0, M06-2X, and MN15 are predicting the correct electronic ground state for all systems investigated here, and also have the lowest mean absolute error for predicting both ΔEspin (0.34 eV, 0.32 eV and 0.31 eV) and J (11.74 meV, 12.66 meV and 10.64 meV). They may therefore also serve as starting points for higher-level methods such as the GW or the random phase approximation. As other functionals fail for the prediction of the ground state, they cannot be recommended for metal-free magnetic systems.

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Tuning the magnetic properties of a diamagnetic di-Blatter's zwitterion to antiferro- and ferromagnetically coupled diradicals

Abstract: In the quest of obtaining organic molecular magnets based on stable diradicals, we have tuned the inherent zwitterionic ground state of tetraphenylhexaazaanthracene (TPHA), the molecule embraced with two Blatter’s moieties,...

Cited by 14 publications

References 102 publications

Anti-ohmic nanoconductors: myth, reality and promise

Anti-ohmic nanoconductors: myth, reality and promise

Anti-ohmic Nanoconductors: Myth, Reality and Promise

Predicting Magnetic Coupling and Spin-Polarization Energy in Triangulene Analogues

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