Chiral structures, breaking spatial inversion symmetry, exhibit non-zero chiroptical activity (COA) due to the coupling between their electric and magnetic responses under external electromagnetic fields, an effect absent in achiral systems. Non-magnetic chiral structures also exhibit Chiral-Induced Spin Selectivity (CISS), primarily detected in two terminal measurements in the linear regime, where spin selection emerges without external magnetic influence. Despite the different origins of these physical phenomena, our model captures the relevant physics required to address CISS as an intrinsic molecular effect with the basic ingredients: (i) chirality/inversion asymmetry, (ii) meV atomic spin–orbit coupling, and (iii) decoherence as a source of reciprocity breaking. In this work, we derived how the electronic system couples with polarized electromagnetic radiation to yield a spin-dependent polarization rotation power, quantified through the Rosenfeld tensor, predicting characteristic spin signatures in the COA. The model also predicts that a net spin polarization manifests in the molecular terminations that have been surmised as an explanation for chiral species separation of racemic mixtures and interactions with surface magnetic domains. A recent sensitive spectroscopic measurement of electron transfer in donor–acceptor complexes is consistent with the standalone CISS effect.
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21 September 2024
Research Article|
September 16 2024
Chiral spin selectivity and chiroptical activity in helical molecules Available to Purchase
Solmar Varela
;
Solmar Varela
a)
(Formal analysis, Investigation, Methodology, Visualization, Writing – original draft, Writing – review & editing)
1
Institute for Materials Science and Max Bergmann Center of Biomaterials, TU Dresden
, 01062 Dresden, Germany
a)Authors to whom correspondence should be addressed: [email protected]; [email protected]; and [email protected]
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Rafael Gutierrez
;
Rafael Gutierrez
(Conceptualization, Formal analysis, Investigation, Methodology, Validation, Writing – original draft, Writing – review & editing)
1
Institute for Materials Science and Max Bergmann Center of Biomaterials, TU Dresden
, 01062 Dresden, Germany
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Gianaurelio Cuniberti
;
Gianaurelio Cuniberti
(Conceptualization, Funding acquisition, Writing – original draft, Writing – review & editing)
1
Institute for Materials Science and Max Bergmann Center of Biomaterials, TU Dresden
, 01062 Dresden, Germany
2
Dresden Center for Computational Materials Science (DCMS), TU Dresden
, 01062 Dresden, Germany
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Ernesto Medina
;
Ernesto Medina
a)
(Conceptualization, Formal analysis, Investigation, Methodology, Validation, Writing – original draft, Writing – review & editing)
3
Departamento de Física, Colegio de Ciencias e Ingeniería, Universidad San Francisco de Quito
, 170901 Quito, Ecuador
a)Authors to whom correspondence should be addressed: [email protected]; [email protected]; and [email protected]
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Vladimiro Mujica
Vladimiro Mujica
a)
(Conceptualization, Formal analysis, Investigation, Methodology, Supervision, Validation, Writing – original draft, Writing – review & editing)
4
School of Molecular Sciences, Arizona State University
, Tempe, Arizona 85287, USA
a)Authors to whom correspondence should be addressed: [email protected]; [email protected]; and [email protected]
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Solmar Varela
1,a)
Rafael Gutierrez
1
Gianaurelio Cuniberti
1,2
Ernesto Medina
3,a)
Vladimiro Mujica
4,a)
1
Institute for Materials Science and Max Bergmann Center of Biomaterials, TU Dresden
, 01062 Dresden, Germany
2
Dresden Center for Computational Materials Science (DCMS), TU Dresden
, 01062 Dresden, Germany
3
Departamento de Física, Colegio de Ciencias e Ingeniería, Universidad San Francisco de Quito
, 170901 Quito, Ecuador
4
School of Molecular Sciences, Arizona State University
, Tempe, Arizona 85287, USA
a)Authors to whom correspondence should be addressed: [email protected]; [email protected]; and [email protected]
J. Chem. Phys. 161, 114111 (2024)
Article history
Received:
July 08 2024
Accepted:
August 26 2024
Citation
Solmar Varela, Rafael Gutierrez, Gianaurelio Cuniberti, Ernesto Medina, Vladimiro Mujica; Chiral spin selectivity and chiroptical activity in helical molecules. J. Chem. Phys. 21 September 2024; 161 (11): 114111. https://doi.org/10.1063/5.0227365
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