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Description:

Organic radicals have shown promise for tunable, low-cost spintronic function. However,
integrating the radicals with a Si metal‒oxide‒semiconductor (MOS) structure remains a
challenge. Here, we successfully incorporate stable (4-(((2,5-bis(2-
(phenyl)ethynyl)phenyl)carbonyl)(methyl)amino)-2,2,6,6-tetramethylpiperidin-1-yl)oxidanyl
(TEMPO-OPE) radicals in a Si-MOS-based double-tunnel junction and demonstrate a huge
positive magnetoresistance of up to 400 % at a magnetic field of 7 T and a temperature of 3 K.
This goes along with a significant splitting of the differential conductance peak corresponding
to the highest occupied molecular orbital of TEMPO-OPE under external magnetic fields. First-principles calculations suggest the radical’s singly occupied orbital to be close to the Fermi
level of the junction, and in close spatial proximity to one of the oxide layers and to the OPE
backbone. This could provide a possible origin of the large magnetoresistance. These findings
suggest a path towards incorporating magnetic molecular functionalities into conventional Si
devices, leading to large-scale integration of molecular spintronic devices.

Rights:

• Creative Commons BY Attribution 4.0 International
  

Keyword: organic radicals, magnetoresistance, unpaired electrons, resonant tunneling, molecular orbitals, Si-based double-tunnel junctions

Date published: 2026-07-01

Publisher: American Chemical Society (ACS)

Journal:

• Nano Letters (ISSN: 15306984) vol. 26 issue. 25 p. 8257-8264

Funding:

• Ministry of Education, Culture, Sports, Science and Technology 23K22802
• Ministry of Education, Culture, Sports, Science and Technology 24KF0270
• Advanced Research Infrastructure for Materials and Nanotechnology, Ministry of Education, Culture, Sports, Science and Technology JPMXP1223NM5170
• High-Performance Computing Center at University of Hamburg
• Research Center for Materials Nanoarchitectonics, National Institute for Materials Science
• German Research Foundation GRK 2536 NANOHYBRID
• German Research Foundation HE-5675/6-1

Manuscript type: Publisher's version (Version of record)

MDR DOI:

First published URL: https://doi.org/10.1021/acs.nanolett.6c01526

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Updated at: 2026-07-03 13:31:04 +0900

Published on MDR: 2026-07-03 16:29:20 +0900