2026
|
Sheng, Xiaoyu; Liu, Ningchao; Peng, Xinnan; Lawrence, James; Su, Jie; Wang, Lulu; Li, Zijie; Song, Shaotang; Zong, Zhaohui; Kino, Shota; Wu, Jishan; Shinokubo, Hiroshi; He, Yuanyuan; Ke, Xian-Sheng; Lu, Jiong Phenalenyl-Fused Nickel(II) Norcorroles with Precisely Oxygen-Edited
Skeletons: Tuning Aromaticity and Site-Selective Reactivity NANO LETTERS, 26 (30), pp. 9959-9967, 2026, DOI: 10.1021/acs.nanolett.6c02692. Abstract | BibTeX | Endnote @article{WOS:001827581300001,
title = {Phenalenyl-Fused Nickel(II) Norcorroles with Precisely Oxygen-Edited
Skeletons: Tuning Aromaticity and Site-Selective Reactivity},
author = {Xiaoyu Sheng and Ningchao Liu and Xinnan Peng and James Lawrence and Jie Su and Lulu Wang and Zijie Li and Shaotang Song and Zhaohui Zong and Shota Kino and Jishan Wu and Hiroshi Shinokubo and Yuanyuan He and Xian-Sheng Ke and Jiong Lu},
doi = {10.1021/acs.nanolett.6c02692},
times_cited = {0},
issn = {1530-6984},
year = {2026},
date = {2026-08-01},
journal = {NANO LETTERS},
volume = {26},
number = {30},
pages = {9959-9967},
publisher = {AMER CHEMICAL SOC},
address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA},
abstract = {Aromaticity governs molecular stability, electronic structure, and
reactivity, yet its atomically precise control on surfaces remains
challenging. Here, we synthesize phenalenyl-fused nickel(II) norcorrole
and oxygen-edited porphyrinoids on Au(111) via surface-assisted
cyclodehydrogenation of rationally designed precursors. Stepwise
insertion of one or two oxygen atoms at pyrrole-pyrrole linkages yields
PLY-Nor, PLY-OxCor, and PLY-2OxPor, enabling systematic modulation of
their electronic structures and aromatic character. Scanning probe
microscopy resolves their atomic backbones, while dI/dV spectroscopy
reveals a progressive widening of the frontier-orbital gap with oxygen
incorporation. Density functional theory calculations and complementary
aromaticity analyses confirm an evolution from a fragmented aromatic
framework toward a more delocalized aromatic character. Moreover, oxygen
skeletal editing redistributes frontier electron density at the
molecular edge, leading to distinct dimerization selectivity. Together,
these findings demonstrate atomic skeletal editing as a powerful
strategy for engineering of electronic structure, aromaticity, and
on-surface reactivity with atomic precision in organic molecules and
nanostructures.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Aromaticity governs molecular stability, electronic structure, and
reactivity, yet its atomically precise control on surfaces remains
challenging. Here, we synthesize phenalenyl-fused nickel(II) norcorrole
and oxygen-edited porphyrinoids on Au(111) via surface-assisted
cyclodehydrogenation of rationally designed precursors. Stepwise
insertion of one or two oxygen atoms at pyrrole-pyrrole linkages yields
PLY-Nor, PLY-OxCor, and PLY-2OxPor, enabling systematic modulation of
their electronic structures and aromatic character. Scanning probe
microscopy resolves their atomic backbones, while dI/dV spectroscopy
reveals a progressive widening of the frontier-orbital gap with oxygen
incorporation. Density functional theory calculations and complementary
aromaticity analyses confirm an evolution from a fragmented aromatic
framework toward a more delocalized aromatic character. Moreover, oxygen
skeletal editing redistributes frontier electron density at the
molecular edge, leading to distinct dimerization selectivity. Together,
these findings demonstrate atomic skeletal editing as a powerful
strategy for engineering of electronic structure, aromaticity, and
on-surface reactivity with atomic precision in organic molecules and
nanostructures. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AFXiaoyu Sheng
Ningchao Liu
Xinnan Peng
James Lawrence
Jie Su
Lulu Wang
Zijie Li
Shaotang Song
Zhaohui Zong
Shota Kino
Jishan Wu
Hiroshi Shinokubo
Yuanyuan He
Xian-Sheng Ke
Jiong Lu
- TIPhenalenyl-Fused Nickel(II) Norcorroles with Precisely Oxygen-Edited
Skeletons: Tuning Aromaticity and Site-Selective Reactivity - SONANO LETTERS
- DTArticle
- ABAromaticity governs molecular stability, electronic structure, and
reactivity, yet its atomically precise control on surfaces remains
challenging. Here, we synthesize phenalenyl-fused nickel(II) norcorrole
and oxygen-edited porphyrinoids on Au(111) via surface-assisted
cyclodehydrogenation of rationally designed precursors. Stepwise
insertion of one or two oxygen atoms at pyrrole-pyrrole linkages yields
PLY-Nor, PLY-OxCor, and PLY-2OxPor, enabling systematic modulation of
their electronic structures and aromatic character. Scanning probe
microscopy resolves their atomic backbones, while dI/dV spectroscopy
reveals a progressive widening of the frontier-orbital gap with oxygen
incorporation. Density functional theory calculations and complementary
aromaticity analyses confirm an evolution from a fragmented aromatic
framework toward a more delocalized aromatic character. Moreover, oxygen
skeletal editing redistributes frontier electron density at the
molecular edge, leading to distinct dimerization selectivity. Together,
these findings demonstrate atomic skeletal editing as a powerful
strategy for engineering of electronic structure, aromaticity, and
on-surface reactivity with atomic precision in organic molecules and
nanostructures. - Z90
- PUAMER CHEMICAL SOC
- PA1155 16TH ST, NW, WASHINGTON, DC 20036 USA
- SN1530-6984
- VL26
- BP9959
- EP9967
- DI10.1021/acs.nanolett.6c02692
- UTWOS:001827581300001
- ER
- EF
|
Chen, Jinxing; Liu, Jie; Sun, Jia-Lu; Li, Jun; Meng, Yang; Hu, Chengzhi; Li, Jiali; Lu, Jiong New Frontiersin Single-Atom Catalysis: Active-SiteDynamics and
AI-Enabled Design CHEMICAL REVIEWS, 126 (16), pp. 9357-9440, 2026, DOI: 10.1021/acs.chemrev.6c00200. Abstract | BibTeX | Endnote @article{WOS:001849322800001,
title = {New Frontiersin Single-Atom Catalysis: Active-SiteDynamics and
AI-Enabled Design},
author = {Jinxing Chen and Jie Liu and Jia-Lu Sun and Jun Li and Yang Meng and Chengzhi Hu and Jiali Li and Jiong Lu},
doi = {10.1021/acs.chemrev.6c00200},
times_cited = {0},
issn = {0009-2665},
year = {2026},
date = {2026-08-01},
journal = {CHEMICAL REVIEWS},
volume = {126},
number = {16},
pages = {9357-9440},
publisher = {AMER CHEMICAL SOC},
address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA},
abstract = {Single-atom catalysts (SACs) have emerged as a rapidly advancing
frontier in heterogeneous catalysis because of their unique electronic
structures, maximized atomic efficiency, and tunable catalytic
properties. Increasing evidence shows that SACs are inherently dynamic
under working conditions with their coordination environment, electronic
structure, and spatial configuration continuously adapting in response
to reactants, intermediates, or external stimuli. These dynamic
properties critically influence catalytic activity, selectivity, and
stability, challenging conventional design paradigms and opening new
opportunities for performance optimization. This review provides a
comprehensive overview of the active-site evolution in SACs under
reaction conditions. We discuss the fundamental mechanisms underlying
atomic migration, coordination changes, and reaction-induced
interconversion of desaturated single-atom states. We also highlight
strategies to harness and control these processes through support
engineering and coordination modulation, enabling the rational design of
desaturated active sites. Finally, we outline major challenges and
future directions, including the use of in situ/operando
characterization, multiscale modeling, and machine learning, to
accelerate the rational design of high-performance SACs. By elucidating
the fundamental aspects of SAC active site evolution, this Review
provides critical insights and design principles to advance the
development of high-performance SACs.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Single-atom catalysts (SACs) have emerged as a rapidly advancing
frontier in heterogeneous catalysis because of their unique electronic
structures, maximized atomic efficiency, and tunable catalytic
properties. Increasing evidence shows that SACs are inherently dynamic
under working conditions with their coordination environment, electronic
structure, and spatial configuration continuously adapting in response
to reactants, intermediates, or external stimuli. These dynamic
properties critically influence catalytic activity, selectivity, and
stability, challenging conventional design paradigms and opening new
opportunities for performance optimization. This review provides a
comprehensive overview of the active-site evolution in SACs under
reaction conditions. We discuss the fundamental mechanisms underlying
atomic migration, coordination changes, and reaction-induced
interconversion of desaturated single-atom states. We also highlight
strategies to harness and control these processes through support
engineering and coordination modulation, enabling the rational design of
desaturated active sites. Finally, we outline major challenges and
future directions, including the use of in situ/operando
characterization, multiscale modeling, and machine learning, to
accelerate the rational design of high-performance SACs. By elucidating
the fundamental aspects of SAC active site evolution, this Review
provides critical insights and design principles to advance the
development of high-performance SACs. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AFJinxing Chen
Jie Liu
Jia-Lu Sun
Jun Li
Yang Meng
Chengzhi Hu
Jiali Li
Jiong Lu
- TINew Frontiersin Single-Atom Catalysis: Active-SiteDynamics and
AI-Enabled Design - SOCHEMICAL REVIEWS
- DTArticle
- ABSingle-atom catalysts (SACs) have emerged as a rapidly advancing
frontier in heterogeneous catalysis because of their unique electronic
structures, maximized atomic efficiency, and tunable catalytic
properties. Increasing evidence shows that SACs are inherently dynamic
under working conditions with their coordination environment, electronic
structure, and spatial configuration continuously adapting in response
to reactants, intermediates, or external stimuli. These dynamic
properties critically influence catalytic activity, selectivity, and
stability, challenging conventional design paradigms and opening new
opportunities for performance optimization. This review provides a
comprehensive overview of the active-site evolution in SACs under
reaction conditions. We discuss the fundamental mechanisms underlying
atomic migration, coordination changes, and reaction-induced
interconversion of desaturated single-atom states. We also highlight
strategies to harness and control these processes through support
engineering and coordination modulation, enabling the rational design of
desaturated active sites. Finally, we outline major challenges and
future directions, including the use of in situ/operando
characterization, multiscale modeling, and machine learning, to
accelerate the rational design of high-performance SACs. By elucidating
the fundamental aspects of SAC active site evolution, this Review
provides critical insights and design principles to advance the
development of high-performance SACs. - Z90
- PUAMER CHEMICAL SOC
- PA1155 16TH ST, NW, WASHINGTON, DC 20036 USA
- SN0009-2665
- VL126
- BP9357
- EP9440
- DI10.1021/acs.chemrev.6c00200
- UTWOS:001849322800001
- 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, 5 (7), pp. 989-998, 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 = {5},
year = {2026},
date = {2026-07-01},
journal = {NATURE SYNTHESIS},
volume = {5},
number = {7},
pages = {989-998},
publisher = {SPRINGERNATURE},
address = {THE 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. - Z95
- PUSPRINGERNATURE
- PATHE CAMPUS, 4 CRINAN ST, LONDON, N1 9XW, ENGLAND
- VL5
- BP989
- EP998
- DI10.1038/s44160-026-01052-1
- UTWOS:001745079300001
- ER
- EF
|
Telychko, Mykola; Huda, Md. Nurul; Huang, Jingsong; Lu, Wenchang; Zarkadoula, Eva; Park, Jewook; Wang, Xinzhe; Chen, Zhaolong; Bernholc, Jerzy; Rodin, Aleksandr; Lu, Jiong; Li, An-Ping Controllable Formation of Threefold-Coordinated Oxygen in Graphene by
Low-Energy Ion Implantation NANO LETTERS, 26 (20), pp. 6576-6584, 2026, DOI: 10.1021/acs.nanolett.6c00728. Abstract | BibTeX | Endnote @article{WOS:001768529300001,
title = {Controllable Formation of Threefold-Coordinated Oxygen in Graphene by
Low-Energy Ion Implantation},
author = {Mykola Telychko and Md. Nurul Huda and Jingsong Huang and Wenchang Lu and Eva Zarkadoula and Jewook Park and Xinzhe Wang and Zhaolong Chen and Jerzy Bernholc and Aleksandr Rodin and Jiong Lu and An-Ping Li},
doi = {10.1021/acs.nanolett.6c00728},
times_cited = {0},
issn = {1530-6984},
year = {2026},
date = {2026-05-01},
journal = {NANO LETTERS},
volume = {26},
number = {20},
pages = {6576-6584},
publisher = {AMER CHEMICAL SOC},
address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA},
abstract = {The atomically precise engineering of impurities in graphene and the
understanding of their structural and carrier-dependent electronic
properties at the nanoscale are crucial for advancing graphene-based
nanoelectronics, catalysis, and energy technologies. Here, we
demonstrate controllable incorporation of the elusive 3-fold-coordinated
O substitutions into graphene using low-energy O+ ion implantation under
ultrahigh-vacuum conditions. By combining high-resolution scanning
tunneling microscopy and spectroscopy (STM/S), bond-resolved noncontact
atomic force microscopy techniques, and density functional theory (DFT)
calculations, we resolve both the structural and electronic properties
of the O-related defects. The STM/S measurements, corroborated by DFT
calculations, uncover a characteristic impurity state that is
energetically pinned to the Dirac point across different charge-carrier
doping regimes. Molecular dynamics simulations further reveal the
distribution of implantation-induced configurations and identify the
formation of 3-fold-coordinated O dopants. This work provides a viable
route to incorporate 3-fold-coordinated O dopants and opens new
opportunities for controlled defect engineering in graphene.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
The atomically precise engineering of impurities in graphene and the
understanding of their structural and carrier-dependent electronic
properties at the nanoscale are crucial for advancing graphene-based
nanoelectronics, catalysis, and energy technologies. Here, we
demonstrate controllable incorporation of the elusive 3-fold-coordinated
O substitutions into graphene using low-energy O+ ion implantation under
ultrahigh-vacuum conditions. By combining high-resolution scanning
tunneling microscopy and spectroscopy (STM/S), bond-resolved noncontact
atomic force microscopy techniques, and density functional theory (DFT)
calculations, we resolve both the structural and electronic properties
of the O-related defects. The STM/S measurements, corroborated by DFT
calculations, uncover a characteristic impurity state that is
energetically pinned to the Dirac point across different charge-carrier
doping regimes. Molecular dynamics simulations further reveal the
distribution of implantation-induced configurations and identify the
formation of 3-fold-coordinated O dopants. This work provides a viable
route to incorporate 3-fold-coordinated O dopants and opens new
opportunities for controlled defect engineering in graphene. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AFMykola Telychko
Md. Nurul Huda
Jingsong Huang
Wenchang Lu
Eva Zarkadoula
Jewook Park
Xinzhe Wang
Zhaolong Chen
Jerzy Bernholc
Aleksandr Rodin
Jiong Lu
An-Ping Li
- TIControllable Formation of Threefold-Coordinated Oxygen in Graphene by
Low-Energy Ion Implantation - SONANO LETTERS
- DTArticle
- ABThe atomically precise engineering of impurities in graphene and the
understanding of their structural and carrier-dependent electronic
properties at the nanoscale are crucial for advancing graphene-based
nanoelectronics, catalysis, and energy technologies. Here, we
demonstrate controllable incorporation of the elusive 3-fold-coordinated
O substitutions into graphene using low-energy O+ ion implantation under
ultrahigh-vacuum conditions. By combining high-resolution scanning
tunneling microscopy and spectroscopy (STM/S), bond-resolved noncontact
atomic force microscopy techniques, and density functional theory (DFT)
calculations, we resolve both the structural and electronic properties
of the O-related defects. The STM/S measurements, corroborated by DFT
calculations, uncover a characteristic impurity state that is
energetically pinned to the Dirac point across different charge-carrier
doping regimes. Molecular dynamics simulations further reveal the
distribution of implantation-induced configurations and identify the
formation of 3-fold-coordinated O dopants. This work provides a viable
route to incorporate 3-fold-coordinated O dopants and opens new
opportunities for controlled defect engineering in graphene. - Z90
- PUAMER CHEMICAL SOC
- PA1155 16TH ST, NW, WASHINGTON, DC 20036 USA
- SN1530-6984
- VL26
- BP6576
- EP6584
- DI10.1021/acs.nanolett.6c00728
- UTWOS:001768529300001
- ER
- EF
|
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 = {2},
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. - Z92
- PUAMER CHEMICAL SOC
- PA1155 16TH ST, NW, WASHINGTON, DC 20036 USA
- SN1936-0851
- VL20
- BP10594
- EP10604
- DI10.1021/acsnano.5c22322
- UTWOS:001724611900001
- ER
- EF
|
