Spin-Selective Electron Transport Through Single Chiral Molecules

Small 20 (2024) 2308233

Mohammad Reza Safari, Frank Matthes, Claus M. Schneider, Karl-Heinz Ernst and Daniel E. Bürgler

The interplay between chirality and magnetism is a source of fascination among scientists for over a century. In recent years, chirality-induced spin selectivity (CISS) has attracted renewed interest. It is 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. This study reports spin-selective electron transport through single helical aromatic hydrocarbons that are 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 is exchanged or the magnetization direction of the STM tip or Co substrate is reversed. Importantly, the results rule out electron–phonon coupling and ensemble effects as primary mechanisms responsible for CISS.

Evaluation of magnetochiral electron tunneling asymmetries with SP-STM

Spin-Selective Electron Transport Through Single Chiral Molecules
Figure: Adsorption configurations of heptahelicene ([7]H) on Co nanoislands. Both enantiomers, (P)-[7]H and (M)-[7]H, can adsorb on Co nanoislands with both (a) magnetization up (M =↑) or (b) magnetization down (M =↓). The pitch vectors of the molecular helices h =↑ (green) and h =↓ (red) represent (P)-[7]H and (M)-[7]H enantiomers, respectively.

CISS for a single pair of [7]H enantiomers

Spin-Selective Electron Transport Through Single Chiral Molecules
Figure: Enantio-resolved STM and chirality counting. (a) Ball-and-stick model of [7]H enantiomers (top) and assignment of their absolute handedness from topographic STM contrast (bottom). Counterclockwise increase of brightness denotes a (P)-enantiomer, while clockwise increase of brightness denotes an (M)-enantiomer. (b) Example for “chirality counting” of [7]H molecules on a single Co nanoisland. Indicated by circular arrows, 4 (P)- and 7 (M)-enantiomers are identified.

Letzte Änderung: 05.11.2024