2026
|
Yang, Tianhao; Huang, Pengru; Qiu, Zhizhan; Han, Yixuan; Guan, Dong; Lyu, Pin; Su, Jie; Novoselov, Kostya S; Fang, Hanyan; Lu, Jiong Atomic-Scale Engineering and Strain Modulation of Quantum Defects in
Hexagonal Boron Nitride ACS NANO, 20 (13), pp. 10594-10604, 2026, DOI: 10.1021/acsnano.5c22322. Abstract | BibTeX | Endnote @article{WOS:001724611900001,
title = {Atomic-Scale Engineering and Strain Modulation of Quantum Defects in
Hexagonal Boron Nitride},
author = {Tianhao Yang and Pengru Huang and Zhizhan Qiu and Yixuan Han and Dong Guan and Pin Lyu and Jie Su and Kostya S Novoselov and Hanyan Fang and Jiong Lu},
doi = {10.1021/acsnano.5c22322},
times_cited = {0},
issn = {1936-0851},
year = {2026},
date = {2026-04-01},
journal = {ACS NANO},
volume = {20},
number = {13},
pages = {10594-10604},
publisher = {AMER CHEMICAL SOC},
address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA},
abstract = {Understanding and engineering atomic defects in hexagonal boron nitride
(hBN) provides a powerful platform for realizing solid-state quantum
emitters and spin qubits, advancing the field of quantum information
science and technologies. However, the full potential of such quantum
defects remains locked by the critical lack of a deterministic
structure-property relationship at the atomic scale. Here, we
demonstrate a strategy to atomically engineer and decipher quantum
defects in hBN by integrating scanning tunneling microscopy/spectroscopy
(STM/STS) and noncontact atomic force-microscopy with a
CO-functionalized tip. We implemented controllable argon ion bombardment
to create both boron vacancies (VB) and nitrogen vacancies (VN) in
submonolayer hBN grown on Cu(111). Simultaneously, encapsulated Ar
species trapped between hBN and Cu(111) locally lift the hBN to form
nanobubbles, thereby decoupling atomic vacancies from the metal
substrate and enabling direct probing of their electronic states. For
the on-bubble VN, STS measurement reveals a prominent in-gap state with
a phonon replica. Furthermore, with aid of STM tip-assisted
manipulation, we demonstrate that the tuning of nanobubble sizes
modulates their strain profile, thereby modulating the energetic
positions of electronic states in on-bubble defects, corroborated by
density functional calculations. Our studies offer insight into the
intrinsic defect structures in hBN and quantum defect engineering via
local strain engineering.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Understanding and engineering atomic defects in hexagonal boron nitride
(hBN) provides a powerful platform for realizing solid-state quantum
emitters and spin qubits, advancing the field of quantum information
science and technologies. However, the full potential of such quantum
defects remains locked by the critical lack of a deterministic
structure-property relationship at the atomic scale. Here, we
demonstrate a strategy to atomically engineer and decipher quantum
defects in hBN by integrating scanning tunneling microscopy/spectroscopy
(STM/STS) and noncontact atomic force-microscopy with a
CO-functionalized tip. We implemented controllable argon ion bombardment
to create both boron vacancies (VB) and nitrogen vacancies (VN) in
submonolayer hBN grown on Cu(111). Simultaneously, encapsulated Ar
species trapped between hBN and Cu(111) locally lift the hBN to form
nanobubbles, thereby decoupling atomic vacancies from the metal
substrate and enabling direct probing of their electronic states. For
the on-bubble VN, STS measurement reveals a prominent in-gap state with
a phonon replica. Furthermore, with aid of STM tip-assisted
manipulation, we demonstrate that the tuning of nanobubble sizes
modulates their strain profile, thereby modulating the energetic
positions of electronic states in on-bubble defects, corroborated by
density functional calculations. Our studies offer insight into the
intrinsic defect structures in hBN and quantum defect engineering via
local strain engineering. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AFTianhao Yang
Pengru Huang
Zhizhan Qiu
Yixuan Han
Dong Guan
Pin Lyu
Jie Su
Kostya S Novoselov
Hanyan Fang
Jiong Lu
- TIAtomic-Scale Engineering and Strain Modulation of Quantum Defects in
Hexagonal Boron Nitride - SOACS NANO
- DTArticle
- ABUnderstanding and engineering atomic defects in hexagonal boron nitride
(hBN) provides a powerful platform for realizing solid-state quantum
emitters and spin qubits, advancing the field of quantum information
science and technologies. However, the full potential of such quantum
defects remains locked by the critical lack of a deterministic
structure-property relationship at the atomic scale. Here, we
demonstrate a strategy to atomically engineer and decipher quantum
defects in hBN by integrating scanning tunneling microscopy/spectroscopy
(STM/STS) and noncontact atomic force-microscopy with a
CO-functionalized tip. We implemented controllable argon ion bombardment
to create both boron vacancies (VB) and nitrogen vacancies (VN) in
submonolayer hBN grown on Cu(111). Simultaneously, encapsulated Ar
species trapped between hBN and Cu(111) locally lift the hBN to form
nanobubbles, thereby decoupling atomic vacancies from the metal
substrate and enabling direct probing of their electronic states. For
the on-bubble VN, STS measurement reveals a prominent in-gap state with
a phonon replica. Furthermore, with aid of STM tip-assisted
manipulation, we demonstrate that the tuning of nanobubble sizes
modulates their strain profile, thereby modulating the energetic
positions of electronic states in on-bubble defects, corroborated by
density functional calculations. Our studies offer insight into the
intrinsic defect structures in hBN and quantum defect engineering via
local strain engineering. - Z90
- PUAMER CHEMICAL SOC
- PA1155 16TH ST, NW, WASHINGTON, DC 20036 USA
- SN1936-0851
- VL20
- BP10594
- EP10604
- DI10.1021/acsnano.5c22322
- UTWOS:001724611900001
- ER
- EF
|
Wang, Qiang; Li, Tan; Huang, Pengru; Yu, Qi; Fu, Kun; Xi, Shibo; Han, Xiaocang; Hu, Jingcong; Zhao, Xiaoxu; Shao, Haipei; Lin, Ming; Meng, Yang; Chen, Jinxing; Li, Jiali; Diao, Caozheng; Hai, Xiao; Wang, Yulin; Fu, Xingjie; Sun, Jialu; Novoselov, Kostya S; Liu, Richard Y; Li, Jun; Lu, Jiong Geminal Atom Catalysts with Minimized d-Orbital Holes Enable
β-Elimination-Resistant C(sp2)-C(sp3)
Cross-Coupling JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 148 (15), pp. 16138-16150, 2026, DOI: 10.1021/jacs.6c00936. Abstract | BibTeX | Endnote @article{WOS:001736603300001,
title = {Geminal Atom Catalysts with Minimized d-Orbital Holes Enable
β-Elimination-Resistant C(sp2)-C(sp3)
Cross-Coupling},
author = {Qiang Wang and Tan Li and Pengru Huang and Qi Yu and Kun Fu and Shibo Xi and Xiaocang Han and Jingcong Hu and Xiaoxu Zhao and Haipei Shao and Ming Lin and Yang Meng and Jinxing Chen and Jiali Li and Caozheng Diao and Xiao Hai and Yulin Wang and Xingjie Fu and Jialu Sun and Kostya S Novoselov and Richard Y Liu and Jun Li and Jiong Lu},
doi = {10.1021/jacs.6c00936},
times_cited = {0},
issn = {0002-7863},
year = {2026},
date = {2026-04-01},
journal = {JOURNAL OF THE AMERICAN CHEMICAL SOCIETY},
volume = {148},
number = {15},
pages = {16138-16150},
publisher = {AMER CHEMICAL SOC},
address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA},
abstract = {Heterogeneous C(sp2)-C(sp3) Suzuki-Miyaura coupling offers an attractive
route for the large-scale and sustainable synthesis of structurally
complex and pharmaceutically relevant molecules that are otherwise
difficult to access. However, the low reactivity of unactivated alkyl
electrophiles and the intrinsic instability of alkyl metal
intermediates, particularly their propensity for beta-hydride
elimination, render selective C(sp2)-C(sp3) bond formation exceptionally
challenging. Here, we integrate high-throughput density functional
theory (DFT) screening with quantum-chemical calculations to identify
Cu-based geminal-atom catalysts as optimal candidates and uncover the
critical role of d-orbital holes that promote agostic interactions,
leading to undesired beta-hydride elimination. Guided by these insights,
we develope a d-orbital hole passivation strategy to fabricate a class
of high-fidelity Cu-based geminal-atom catalysts (HF-Cu/GACs),
simultaneously accelerating oxidative addition and suppressing
beta-hydride elimination, enabling broad-scope and highly selective
C(sp2)-C(sp3) cross-coupling between aryl boronic esters and alkyl
(pseudo)halides. These catalysts enable the synthesis of diverse
pharmaceutically relevant intermediates in fewer steps, with higher
yields and using safer, more sustainable conditions compared to
traditional routes. Mechanistic studies reveal that the HF-Cu/GACs
feature paired, low-valent Cu centers with minimal d-orbital holes, and
that C-Br bond activation proceeds through a surface-mediated
single-electron transfer between coadsorbed reactants, rather than
free-radical rebound pathways. The findings here establish a
generalizable strategy for electronic-state engineering of geminal metal
sites to overcome long-standing challenges in cross-coupling chemistry
and highlight the potential of heterogeneous Cu catalysts for the
sustainable synthesis of fine chemicals and pharmaceuticals.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Heterogeneous C(sp2)-C(sp3) Suzuki-Miyaura coupling offers an attractive
route for the large-scale and sustainable synthesis of structurally
complex and pharmaceutically relevant molecules that are otherwise
difficult to access. However, the low reactivity of unactivated alkyl
electrophiles and the intrinsic instability of alkyl metal
intermediates, particularly their propensity for beta-hydride
elimination, render selective C(sp2)-C(sp3) bond formation exceptionally
challenging. Here, we integrate high-throughput density functional
theory (DFT) screening with quantum-chemical calculations to identify
Cu-based geminal-atom catalysts as optimal candidates and uncover the
critical role of d-orbital holes that promote agostic interactions,
leading to undesired beta-hydride elimination. Guided by these insights,
we develope a d-orbital hole passivation strategy to fabricate a class
of high-fidelity Cu-based geminal-atom catalysts (HF-Cu/GACs),
simultaneously accelerating oxidative addition and suppressing
beta-hydride elimination, enabling broad-scope and highly selective
C(sp2)-C(sp3) cross-coupling between aryl boronic esters and alkyl
(pseudo)halides. These catalysts enable the synthesis of diverse
pharmaceutically relevant intermediates in fewer steps, with higher
yields and using safer, more sustainable conditions compared to
traditional routes. Mechanistic studies reveal that the HF-Cu/GACs
feature paired, low-valent Cu centers with minimal d-orbital holes, and
that C-Br bond activation proceeds through a surface-mediated
single-electron transfer between coadsorbed reactants, rather than
free-radical rebound pathways. The findings here establish a
generalizable strategy for electronic-state engineering of geminal metal
sites to overcome long-standing challenges in cross-coupling chemistry
and highlight the potential of heterogeneous Cu catalysts for the
sustainable synthesis of fine chemicals and pharmaceuticals. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AFQiang Wang
Tan Li
Pengru Huang
Qi Yu
Kun Fu
Shibo Xi
Xiaocang Han
Jingcong Hu
Xiaoxu Zhao
Haipei Shao
Ming Lin
Yang Meng
Jinxing Chen
Jiali Li
Caozheng Diao
Xiao Hai
Yulin Wang
Xingjie Fu
Jialu Sun
Kostya S Novoselov
Richard Y Liu
Jun Li
Jiong Lu
- TIGeminal Atom Catalysts with Minimized d-Orbital Holes Enable
β-Elimination-Resistant C(sp2)-C(sp3)
Cross-Coupling - SOJOURNAL OF THE AMERICAN CHEMICAL SOCIETY
- DTArticle
- ABHeterogeneous C(sp2)-C(sp3) Suzuki-Miyaura coupling offers an attractive
route for the large-scale and sustainable synthesis of structurally
complex and pharmaceutically relevant molecules that are otherwise
difficult to access. However, the low reactivity of unactivated alkyl
electrophiles and the intrinsic instability of alkyl metal
intermediates, particularly their propensity for beta-hydride
elimination, render selective C(sp2)-C(sp3) bond formation exceptionally
challenging. Here, we integrate high-throughput density functional
theory (DFT) screening with quantum-chemical calculations to identify
Cu-based geminal-atom catalysts as optimal candidates and uncover the
critical role of d-orbital holes that promote agostic interactions,
leading to undesired beta-hydride elimination. Guided by these insights,
we develope a d-orbital hole passivation strategy to fabricate a class
of high-fidelity Cu-based geminal-atom catalysts (HF-Cu/GACs),
simultaneously accelerating oxidative addition and suppressing
beta-hydride elimination, enabling broad-scope and highly selective
C(sp2)-C(sp3) cross-coupling between aryl boronic esters and alkyl
(pseudo)halides. These catalysts enable the synthesis of diverse
pharmaceutically relevant intermediates in fewer steps, with higher
yields and using safer, more sustainable conditions compared to
traditional routes. Mechanistic studies reveal that the HF-Cu/GACs
feature paired, low-valent Cu centers with minimal d-orbital holes, and
that C-Br bond activation proceeds through a surface-mediated
single-electron transfer between coadsorbed reactants, rather than
free-radical rebound pathways. The findings here establish a
generalizable strategy for electronic-state engineering of geminal metal
sites to overcome long-standing challenges in cross-coupling chemistry
and highlight the potential of heterogeneous Cu catalysts for the
sustainable synthesis of fine chemicals and pharmaceuticals. - Z90
- PUAMER CHEMICAL SOC
- PA1155 16TH ST, NW, WASHINGTON, DC 20036 USA
- SN0002-7863
- VL148
- BP16138
- EP16150
- DI10.1021/jacs.6c00936
- UTWOS:001736603300001
- ER
- EF
|
Peng, Xinnan; Wenlong, E; Teng, Yu; Zhang, Haoyu; Li, En; Wang, Yu; Wang, Lulu; Song, Shaotang; Lu, Jiong Designer π-magnetism in magnetic graphene nanostructures: advances and
future perspectives NATIONAL SCIENCE REVIEW, 13 (7), 2026, DOI: 10.1093/nsr/nwag157. Abstract | BibTeX | Endnote @article{WOS:001743856600001,
title = {Designer π-magnetism in magnetic graphene nanostructures: advances and
future perspectives},
author = {Xinnan Peng and E Wenlong and Yu Teng and Haoyu Zhang and En Li and Yu Wang and Lulu Wang and Shaotang Song and Jiong Lu},
doi = {10.1093/nsr/nwag157},
times_cited = {1},
issn = {2095-5138},
year = {2026},
date = {2026-04-01},
journal = {NATIONAL SCIENCE REVIEW},
volume = {13},
number = {7},
publisher = {OXFORD UNIV PRESS},
address = {GREAT CLARENDON ST, OXFORD OX2 6DP, ENGLAND},
abstract = {Magnetic graphene nanostructures (MGNs) represent a rapidly advancing
frontier in molecular quantum materials, distinguished by pi-magnetism
that arises from the topological design of their pi-electron networks.
The pi-magnetism and correlated quantum phases in these systems can be
precisely engineered through deliberate control of the molecular
topology, sublattice symmetry and electron correlation, transforming
low-dimensional carbon-based architectures into versatile model
platforms for exploring exotic quantum phenomena. Recent advances in
on-surface synthesis have further propelled this field by enabling the
atomically precise fabrication of MGNs and fine control over their
electronic and magnetic properties. Complementing these synthetic
advances, progress in low-temperature scanning probe microscopy now
affords unprecedented capabilities to characterize individual pi-spins,
exchange coupling and correlated ground states at the single-molecule
level. Together, these developments have established a robust foundation
for exploring long-lived spin coherence, tunable quantum entanglement
and spin-based logic operations in carbon-based systems. This review
highlights recent conceptual and methodological advances, emphasizing
how rational molecular design, atomically precise synthesis and
state-of-the-art characterization techniques collectively advance the
understanding and realization of pi-magnetism in MGNs. Remaining
challenges, including stabilizing chemically reactive open-shell
structures, mitigating substrate-induced hybridization and integrating
molecular magnets into functional device architectures, are also
discussed. Continued progress in this field will reshape our perspective
on designing novel forms of magnetism in conjugated organic materials
and open up new pathways toward scalable molecular spintronics and
quantum technologies.
This review illustrates how designed graphene nanostructures can
function as tunable quantum magnets, highlighting their atomically
precise fabrication and characterization methods that open new
opportunities for future quantum devices.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Magnetic graphene nanostructures (MGNs) represent a rapidly advancing
frontier in molecular quantum materials, distinguished by pi-magnetism
that arises from the topological design of their pi-electron networks.
The pi-magnetism and correlated quantum phases in these systems can be
precisely engineered through deliberate control of the molecular
topology, sublattice symmetry and electron correlation, transforming
low-dimensional carbon-based architectures into versatile model
platforms for exploring exotic quantum phenomena. Recent advances in
on-surface synthesis have further propelled this field by enabling the
atomically precise fabrication of MGNs and fine control over their
electronic and magnetic properties. Complementing these synthetic
advances, progress in low-temperature scanning probe microscopy now
affords unprecedented capabilities to characterize individual pi-spins,
exchange coupling and correlated ground states at the single-molecule
level. Together, these developments have established a robust foundation
for exploring long-lived spin coherence, tunable quantum entanglement
and spin-based logic operations in carbon-based systems. This review
highlights recent conceptual and methodological advances, emphasizing
how rational molecular design, atomically precise synthesis and
state-of-the-art characterization techniques collectively advance the
understanding and realization of pi-magnetism in MGNs. Remaining
challenges, including stabilizing chemically reactive open-shell
structures, mitigating substrate-induced hybridization and integrating
molecular magnets into functional device architectures, are also
discussed. Continued progress in this field will reshape our perspective
on designing novel forms of magnetism in conjugated organic materials
and open up new pathways toward scalable molecular spintronics and
quantum technologies.
This review illustrates how designed graphene nanostructures can
function as tunable quantum magnets, highlighting their atomically
precise fabrication and characterization methods that open new
opportunities for future quantum devices. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AFXinnan Peng
E Wenlong
Yu Teng
Haoyu Zhang
En Li
Yu Wang
Lulu Wang
Shaotang Song
Jiong Lu
- TIDesigner π-magnetism in magnetic graphene nanostructures: advances and
future perspectives - SONATIONAL SCIENCE REVIEW
- DTArticle
- ABMagnetic graphene nanostructures (MGNs) represent a rapidly advancing
frontier in molecular quantum materials, distinguished by pi-magnetism
that arises from the topological design of their pi-electron networks.
The pi-magnetism and correlated quantum phases in these systems can be
precisely engineered through deliberate control of the molecular
topology, sublattice symmetry and electron correlation, transforming
low-dimensional carbon-based architectures into versatile model
platforms for exploring exotic quantum phenomena. Recent advances in
on-surface synthesis have further propelled this field by enabling the
atomically precise fabrication of MGNs and fine control over their
electronic and magnetic properties. Complementing these synthetic
advances, progress in low-temperature scanning probe microscopy now
affords unprecedented capabilities to characterize individual pi-spins,
exchange coupling and correlated ground states at the single-molecule
level. Together, these developments have established a robust foundation
for exploring long-lived spin coherence, tunable quantum entanglement
and spin-based logic operations in carbon-based systems. This review
highlights recent conceptual and methodological advances, emphasizing
how rational molecular design, atomically precise synthesis and
state-of-the-art characterization techniques collectively advance the
understanding and realization of pi-magnetism in MGNs. Remaining
challenges, including stabilizing chemically reactive open-shell
structures, mitigating substrate-induced hybridization and integrating
molecular magnets into functional device architectures, are also
discussed. Continued progress in this field will reshape our perspective
on designing novel forms of magnetism in conjugated organic materials
and open up new pathways toward scalable molecular spintronics and
quantum technologies.
This review illustrates how designed graphene nanostructures can
function as tunable quantum magnets, highlighting their atomically
precise fabrication and characterization methods that open new
opportunities for future quantum devices. - Z91
- PUOXFORD UNIV PRESS
- PAGREAT CLARENDON ST, OXFORD OX2 6DP, ENGLAND
- SN2095-5138
- VL13
- DI10.1093/nsr/nwag157
- UTWOS:001743856600001
- ER
- EF
|
Li, En; Kumar, Manish; Peng, Xinnan; Shen, Tong; Soler-Polo, Diego; Wang, Yu; Teng, Yu; Zhang, Haoyu; Su, Jie; Song, Shaotang; Wu, Jishan; Jelinek, Pavel; Lu, Jiong Rationally designed polyradical nanographenes with strong spin
entanglement and perturbation resilience via Clar's goblet extension NATURE SYNTHESIS, 2026, DOI: 10.1038/s44160-026-01052-1. Abstract | BibTeX | Endnote @article{WOS:001745079300001,
title = {Rationally designed polyradical nanographenes with strong spin
entanglement and perturbation resilience via Clar's goblet extension},
author = {En Li and Manish Kumar and Xinnan Peng and Tong Shen and Diego Soler-Polo and Yu Wang and Yu Teng and Haoyu Zhang and Jie Su and Shaotang Song and Jishan Wu and Pavel Jelinek and Jiong Lu},
doi = {10.1038/s44160-026-01052-1},
times_cited = {1},
year = {2026},
date = {2026-04-01},
journal = {NATURE SYNTHESIS},
publisher = {SPRINGERNATURE},
address = {CAMPUS, 4 CRINAN ST, LONDON, N1 9XW, ENGLAND},
abstract = {Polyradical nanographenes featuring strong spin entanglement and robust
many-body spin states against external magnetic perturbations not only
enable the exploration of correlated quantum magnetism at the molecular
scale, but also constitute promising candidates for developing molecular
qubits with chemical tunability and building scalable quantum networks.
Here we use a predictive design strategy to realize the on-surface
synthesis of two homologues of Clar's goblet, C62H22 and C76H26, via
lateral and vertical extensions of the parent structure, respectively.
Vertical extension increases the number of topologically frustrated
zero-energy modes, which scales linearly with the total number of
benzene-ring rows. By contrast, lateral extension enhances
electron-electron interactions, leading to the emergence of additional
radical states beyond those predicted by the topological zero-energy
modes. Consequently, both structures exhibit correlated tetraradical
character and a many-body singlet ground state, as confirmed by
multireference theoretical calculations. These magnetic states arise
from unique magnetic origins and also display distinct resilience to
external perturbations, as experimentally validated using
nickelocene-functionalized scanning probe techniques. Our work presents
a general strategy for the rational design of highly entangled
polyradical nanographenes with tunable spin numbers and resilience of
many-body spin states to perturbations, opening up exciting
possibilities for exploring correlated spin phases in molecular systems
and advancing quantum information technologies.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Polyradical nanographenes featuring strong spin entanglement and robust
many-body spin states against external magnetic perturbations not only
enable the exploration of correlated quantum magnetism at the molecular
scale, but also constitute promising candidates for developing molecular
qubits with chemical tunability and building scalable quantum networks.
Here we use a predictive design strategy to realize the on-surface
synthesis of two homologues of Clar's goblet, C62H22 and C76H26, via
lateral and vertical extensions of the parent structure, respectively.
Vertical extension increases the number of topologically frustrated
zero-energy modes, which scales linearly with the total number of
benzene-ring rows. By contrast, lateral extension enhances
electron-electron interactions, leading to the emergence of additional
radical states beyond those predicted by the topological zero-energy
modes. Consequently, both structures exhibit correlated tetraradical
character and a many-body singlet ground state, as confirmed by
multireference theoretical calculations. These magnetic states arise
from unique magnetic origins and also display distinct resilience to
external perturbations, as experimentally validated using
nickelocene-functionalized scanning probe techniques. Our work presents
a general strategy for the rational design of highly entangled
polyradical nanographenes with tunable spin numbers and resilience of
many-body spin states to perturbations, opening up exciting
possibilities for exploring correlated spin phases in molecular systems
and advancing quantum information technologies. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AFEn Li
Manish Kumar
Xinnan Peng
Tong Shen
Diego Soler-Polo
Yu Wang
Yu Teng
Haoyu Zhang
Jie Su
Shaotang Song
Jishan Wu
Pavel Jelinek
Jiong Lu
- TIRationally designed polyradical nanographenes with strong spin
entanglement and perturbation resilience via Clar's goblet extension - SONATURE SYNTHESIS
- DTArticle
- ABPolyradical nanographenes featuring strong spin entanglement and robust
many-body spin states against external magnetic perturbations not only
enable the exploration of correlated quantum magnetism at the molecular
scale, but also constitute promising candidates for developing molecular
qubits with chemical tunability and building scalable quantum networks.
Here we use a predictive design strategy to realize the on-surface
synthesis of two homologues of Clar's goblet, C62H22 and C76H26, via
lateral and vertical extensions of the parent structure, respectively.
Vertical extension increases the number of topologically frustrated
zero-energy modes, which scales linearly with the total number of
benzene-ring rows. By contrast, lateral extension enhances
electron-electron interactions, leading to the emergence of additional
radical states beyond those predicted by the topological zero-energy
modes. Consequently, both structures exhibit correlated tetraradical
character and a many-body singlet ground state, as confirmed by
multireference theoretical calculations. These magnetic states arise
from unique magnetic origins and also display distinct resilience to
external perturbations, as experimentally validated using
nickelocene-functionalized scanning probe techniques. Our work presents
a general strategy for the rational design of highly entangled
polyradical nanographenes with tunable spin numbers and resilience of
many-body spin states to perturbations, opening up exciting
possibilities for exploring correlated spin phases in molecular systems
and advancing quantum information technologies. - Z91
- PUSPRINGERNATURE
- PACAMPUS, 4 CRINAN ST, LONDON, N1 9XW, ENGLAND
- DI10.1038/s44160-026-01052-1
- UTWOS:001745079300001
- ER
- EF
|
Lawrence, James; Dordevic, Luka; Bachtiger, Fabienne; Pinfold, Harry; Walker, Marc; Lu, Jiong; Sosso, Gabriele C; Bonifazi, Davide; Costantini, Giovanni Ultra-narrow donor-acceptor nanoribbons NATURE COMMUNICATIONS, 17 (1), 2026, DOI: 10.1038/s41467-026-71660-0. Abstract | BibTeX | Endnote @article{WOS:001748164500007,
title = {Ultra-narrow donor-acceptor nanoribbons},
author = {James Lawrence and Luka Dordevic and Fabienne Bachtiger and Harry Pinfold and Marc Walker and Jiong Lu and Gabriele C Sosso and Davide Bonifazi and Giovanni Costantini},
doi = {10.1038/s41467-026-71660-0},
times_cited = {0},
year = {2026},
date = {2026-04-01},
journal = {NATURE COMMUNICATIONS},
volume = {17},
number = {1},
publisher = {NATURE PORTFOLIO},
address = {HEIDELBERGER PLATZ 3, BERLIN, 14197, GERMANY},
abstract = {Donor-acceptor (D-A) architectures underpin many high-performance
conjugated polymers but remain largely unexplored in atomically precise
nanoribbons. Here, we report the on-surface synthesis of ultra-narrow
D-A nanoribbons using two complementary brominated precursors based on
the electron donor peri-xanthenoxanthene and the acceptor anthanthrone.
High-resolution scanning tunnelling microscopy, non-contact atomic force
microscopy and scanning tunnelling spectroscopy reveal submolecular
structural and electronic features of the resulting nanoribbons.
Homopolymerisation of each precursor yields structurally well-defined
donor-only and acceptor-only nanoribbons, whose electronic character
strengthens with length. Co-deposition of both precursors produces mixed
D-A nanoribbons with tuneable electronic structures governed by monomer
sequence. The spatial character and energetic alignment of their
frontier orbitals match gas-phase density functional theory
calculations, while a simplified linear combination of molecular
orbitals model captures dominant trends. This bottom-up synthetic
strategy enables precise control over nanoribbon composition and
functionality, offering a versatile platform for engineering
pi-conjugated nanostructures with tailored optoelectronic properties.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Donor-acceptor (D-A) architectures underpin many high-performance
conjugated polymers but remain largely unexplored in atomically precise
nanoribbons. Here, we report the on-surface synthesis of ultra-narrow
D-A nanoribbons using two complementary brominated precursors based on
the electron donor peri-xanthenoxanthene and the acceptor anthanthrone.
High-resolution scanning tunnelling microscopy, non-contact atomic force
microscopy and scanning tunnelling spectroscopy reveal submolecular
structural and electronic features of the resulting nanoribbons.
Homopolymerisation of each precursor yields structurally well-defined
donor-only and acceptor-only nanoribbons, whose electronic character
strengthens with length. Co-deposition of both precursors produces mixed
D-A nanoribbons with tuneable electronic structures governed by monomer
sequence. The spatial character and energetic alignment of their
frontier orbitals match gas-phase density functional theory
calculations, while a simplified linear combination of molecular
orbitals model captures dominant trends. This bottom-up synthetic
strategy enables precise control over nanoribbon composition and
functionality, offering a versatile platform for engineering
pi-conjugated nanostructures with tailored optoelectronic properties. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AFJames Lawrence
Luka Dordevic
Fabienne Bachtiger
Harry Pinfold
Marc Walker
Jiong Lu
Gabriele C Sosso
Davide Bonifazi
Giovanni Costantini
- TIUltra-narrow donor-acceptor nanoribbons
- SONATURE COMMUNICATIONS
- DTArticle
- ABDonor-acceptor (D-A) architectures underpin many high-performance
conjugated polymers but remain largely unexplored in atomically precise
nanoribbons. Here, we report the on-surface synthesis of ultra-narrow
D-A nanoribbons using two complementary brominated precursors based on
the electron donor peri-xanthenoxanthene and the acceptor anthanthrone.
High-resolution scanning tunnelling microscopy, non-contact atomic force
microscopy and scanning tunnelling spectroscopy reveal submolecular
structural and electronic features of the resulting nanoribbons.
Homopolymerisation of each precursor yields structurally well-defined
donor-only and acceptor-only nanoribbons, whose electronic character
strengthens with length. Co-deposition of both precursors produces mixed
D-A nanoribbons with tuneable electronic structures governed by monomer
sequence. The spatial character and energetic alignment of their
frontier orbitals match gas-phase density functional theory
calculations, while a simplified linear combination of molecular
orbitals model captures dominant trends. This bottom-up synthetic
strategy enables precise control over nanoribbon composition and
functionality, offering a versatile platform for engineering
pi-conjugated nanostructures with tailored optoelectronic properties. - Z90
- PUNATURE PORTFOLIO
- PAHEIDELBERGER PLATZ 3, BERLIN, 14197, GERMANY
- VL17
- DI10.1038/s41467-026-71660-0
- UTWOS:001748164500007
- ER
- EF
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