arXiv subjects

Frank Matthes

Publications and source records attributed to Frank Matthes.

3 recordsLinked to original sources

arXiv2026

Chirality-induced spin selectivity without intrinsic spin-orbit coupling: Role of current-induced molecular orbital moment

The microscopic origin of the chirality-induced spin selectivity (CISS) in helical molecules remains an open question. Recent experiments suggest that a significant contribution to CISS arises from the molecule itself, which is disregarded in existing interfacial or scattering based theories. Here we present an alternative theory of CISS to address this molecular contribution. The mechanism is based on the circulation of charge current in molecular loops that generates a molecular orbital moment (MOM). The direction of the MOM is governed by the gauge field arising from the structural distortion of the molecule and is associated with the handedness of the molecule. Such a MOM can produce finite CISS magnetoresistance and magnetochiral conductance asymmetries that are even in bias voltage, without violating the Onsager-Casimir reciprocity relations. Depending on the Fermi level and bias voltage, the MOM can be controlled externally, which can result in additional crossings of the enantiomer $I-V$ curves. Finally we explain the origin of the electrical magnetochiral anisotropy within the same framework, which establishes its generic applicability.

cond-mat.mes-hall↗

arXiv2023

Enantioselective adsorption on magnetic surfaces

From the beginning of molecular theory, the interplay of chirality and magnetism has intrigued scientists. There is still the question if enantiospecific adsorption of chiral molecules occurs on magnetic surfaces. Enantiomer discrimination was conjectured to arise from chirality-induced spin separation within the molecules and exchange interaction with the substrate's magnetization. Here we show that single helical aromatic hydrocarbons undergo enantioselective adsorption on ferromagnetic cobalt surfaces. Spin and chirality sensitive scanning tunneling microscopy reveals that molecules of opposite handedness prefer adsorption onto cobalt islands with opposite out-of-plane magnetization. As mobility ceases in the final chemisorbed state, it is concluded that enantioselection must occur in a physisorbed transient precursor state. State-of-the-art spin-resolved ab initio simulations support this scenario by refuting enantio-dependent chemisorption energies. These findings demonstrate that van der Waals interaction should also include spin-fluctuations which are crucial for molecular magnetochiral processes.

cond-mat.mtrl-sci↗

arXiv2023

Spin-Selective Electron Transport Through Single Chiral Molecules

The interplay between chirality and magnetism has been a source of fascination among scientists for over a century. In recent years, chirality-induced spin selectivity (CISS) has attracted renewed interest. It has been observed that electron transport through layers of homochiral molecules leads to a significant spin polarization of several tens of percent. Despite the abundant experimental evidence gathered through mesoscopic transport measurements, the exact mechanism behind CISS remains elusive. In this study, we report spin-selective electron transport through single helical aromatic hydrocarbons that were sublimed in vacuo onto ferromagnetic cobalt surfaces and examined with spin-polarized scanning tunneling microscopy (SP-STM) at a temperature of 5 K. Direct comparison of two enantiomers under otherwise identical conditions revealed magnetochiral conductance asymmetries of up to 50% when either the molecular handedness was exchanged or the magnetization direction of the STM tip or Co substrate was reversed. Importantly, our results rule out electron-phonon coupling and ensemble effects as primary mechanisms responsible for CISS.

cond-mat.mes-hall↗