Breaking Interference‐Driven Reversal Currents to Boost Single‐Molecule Conductance

S Shun‐Da Wu (Department: State Key Laboratory of Natural Product Chemistry Key Laboratory of Special Function Materials and Structure Design (MOE) College of Chemistry and Chemical Engineering Institution: Lanzhou University Address: Lanzhou University Lanzhou China) S Shu‐Tong Liu (Department: State Key Laboratory of Natural Product Chemistry Key Laboratory of Special Function Materials and Structure Design (MOE) College of Chemistry and Chemical Engineering Institution: Lanzhou University Address: Lanzhou University Lanzhou China) Z Zi‐Ming Cai (State Key Laboratory of Natural Product Chemistry (SKLNPC) Key Laboratory of Special Function Materials and Structure Design (MOE) College of Chemistry and Chemical Engineering Lanzhou University 222 Tianshui South Road Lanzhou China) B Bing Sun X Xiao‐Di Liu (Department: State Key Laboratory of Natural Product Chemistry Key Laboratory of Special Function Materials and Structure Design (MOE) College of Chemistry and Chemical Engineering Institution: Lanzhou University Address: Lanzhou University Lanzhou China) L Li‐Yu‐Yang Shi (Department: State Key Laboratory of Natural Product Chemistry Key Laboratory of Special Function Materials and Structure Design (MOE) College of Chemistry and Chemical Engineering Institution: Lanzhou University Address: Lanzhou University Lanzhou China) C Colin J. Lambert (Department of Physics Lancaster University Lancaster LA1 4YB UK) H Hao‐Li Zhang (State Key Laboratory of Natural Product Chemistry Key Laboratory of Special Function Materials and Structure Design (MOE) College of Chemistry and Chemical Engineering Lanzhou University Lanzhou P.R. China)

Abstract

Abstract Controlling charge transport in single‐molecule junctions is essential for advancing molecular electronics. This study demonstrates a novel strategy to dramatically enhance conductance in cross‐conjugated systems by preventing reversal current formation in destructive quantum interference (DQI) regimes. We design four molecules with meta‐substituted phenyl rings replaced by hydrogen‐bonded diketone ( OHO ) or boron‐coordinated rings ( NBN , NBO , OBO ), all maintaining hexagonal cross‐conjugated topology. Experimental and theoretical analyses reveal a counterintuitive conductance enhancement arising from suppressed reversal currents. Replacing the prototype m‐phenyl ring ( mPh ) with diketone ( OHO ) elevates conductance by one order of magnitude. Further boron coordination synergistically modulates quantum interference and energy levels, achieving an unprecedented two orders of magnitude increase in conductance in OBO (from 10 −5.39 G 0 to 10 −3.41 G 0 ). This work establishes a paradigm for efficient conductance modulation via targeted reversal current suppression, enabling rationally designed quantum‐interference molecular devices.

Article Details

Volume / Issue Vol. 64, Issue 50
Published December 08, 2025
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (8)

S

Shun‐Da Wu

Department: State Key Laboratory of Natural Product Chemistry Key Laboratory of Special Function Materials and Structure Design (MOE) College of Chemistry and Chemical Engineering Institution: Lanzhou University Address: Lanzhou University Lanzhou China

S

Shu‐Tong Liu

Department: State Key Laboratory of Natural Product Chemistry Key Laboratory of Special Function Materials and Structure Design (MOE) College of Chemistry and Chemical Engineering Institution: Lanzhou University Address: Lanzhou University Lanzhou China

Z

Zi‐Ming Cai

State Key Laboratory of Natural Product Chemistry (SKLNPC) Key Laboratory of Special Function Materials and Structure Design (MOE) College of Chemistry and Chemical Engineering Lanzhou University 222 Tianshui South Road Lanzhou China

B

Bing Sun

X

Xiao‐Di Liu

Department: State Key Laboratory of Natural Product Chemistry Key Laboratory of Special Function Materials and Structure Design (MOE) College of Chemistry and Chemical Engineering Institution: Lanzhou University Address: Lanzhou University Lanzhou China

L

Li‐Yu‐Yang Shi

Department: State Key Laboratory of Natural Product Chemistry Key Laboratory of Special Function Materials and Structure Design (MOE) College of Chemistry and Chemical Engineering Institution: Lanzhou University Address: Lanzhou University Lanzhou China

C

Colin J. Lambert

Department of Physics Lancaster University Lancaster LA1 4YB UK

H

Hao‐Li Zhang

State Key Laboratory of Natural Product Chemistry Key Laboratory of Special Function Materials and Structure Design (MOE) College of Chemistry and Chemical Engineering Lanzhou University Lanzhou P.R. China