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Article ; Online: Emissive brightening in molecular graphene nanoribbons by twilight states.

Sturdza, Bernd K / Kong, Fanmiao / Yao, Xuelin / Niu, Wenhui / Ma, Ji / Feng, Xinliang / Riede, Moritz K / Bogani, Lapo / Nicholas, Robin J

Nature communications

2024 Volume 15, Issue 1, Page(s) 2985

Abstract: Carbon nanomaterials are expected to be bright and efficient emitters, but structural disorder, intermolecular interactions and the intrinsic presence of dark states suppress their photoluminescence. Here, we study synthetically-made graphene nanoribbons ...

Abstract	Carbon nanomaterials are expected to be bright and efficient emitters, but structural disorder, intermolecular interactions and the intrinsic presence of dark states suppress their photoluminescence. Here, we study synthetically-made graphene nanoribbons with atomically precise edges and which are designed to suppress intermolecular interactions to demonstrate strong photoluminescence in both solutions and thin films. The resulting high spectral resolution reveals strong vibron-electron coupling from the radial-breathing-like mode of the ribbons. In addition, their cove-edge structure produces inter-valley mixing, which brightens conventionally-dark states to generate hitherto-unrecognised twilight states as predicted by theory. The coupling of these states to the nanoribbon phonon modes affects absorption and emission differently, suggesting a complex interaction with both Herzberg-Teller and Franck- Condon coupling present. Detailed understanding of the fundamental electronic processes governing the optical response will help the tailored chemical design of nanocarbon optical devices, via gap tuning and side-chain functionalisation.
Language	English
Publishing date	2024-04-06
Publishing country	England
Document type	Journal Article
ZDB-ID	2553671-0
ISSN	2041-1723 ; 2041-1723
ISSN (online)	2041-1723
ISSN	2041-1723
DOI	10.1038/s41467-024-47139-1
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Quantum interference enhances the performance of single-molecule transistors.

Chen, Zhixin / Grace, Iain M / Woltering, Steffen L / Chen, Lina / Gee, Alex / Baugh, Jonathan / Briggs, G Andrew D / Bogani, Lapo / Mol, Jan A / Lambert, Colin J / Anderson, Harry L / Thomas, James O

Nature nanotechnology

2024

Abstract: Quantum effects in nanoscale electronic devices promise to lead to new types of functionality not achievable using classical electronic components. However, quantum behaviour also presents an unresolved challenge facing electronics at the few-nanometre ... ...

Abstract	Quantum effects in nanoscale electronic devices promise to lead to new types of functionality not achievable using classical electronic components. However, quantum behaviour also presents an unresolved challenge facing electronics at the few-nanometre scale: resistive channels start leaking owing to quantum tunnelling. This affects the performance of nanoscale transistors, with direct source-drain tunnelling degrading switching ratios and subthreshold swings, and ultimately limiting operating frequency due to increased static power dissipation. The usual strategy to mitigate quantum effects has been to increase device complexity, but theory shows that if quantum effects can be exploited in molecular-scale electronics, this could provide a route to lower energy consumption and boost device performance. Here we demonstrate these effects experimentally, showing how the performance of molecular transistors is improved when the resistive channel contains two destructively interfering waves. We use a zinc-porphyrin coupled to graphene electrodes in a three-terminal transistor to demonstrate a >10
Language	English
Publishing date	2024-03-25
Publishing country	England
Document type	Journal Article
ZDB-ID	2254964-X
ISSN	1748-3395 ; 1748-3387
ISSN (online)	1748-3395
ISSN	1748-3387
DOI	10.1038/s41565-024-01633-1
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Article ; Online: Porphyrin-fused graphene nanoribbons.

Chen, Qiang / Lodi, Alessandro / Zhang, Heng / Gee, Alex / Wang, Hai I / Kong, Fanmiao / Clarke, Michael / Edmondson, Matthew / Hart, Jack / O'Shea, James N / Stawski, Wojciech / Baugh, Jonathan / Narita, Akimitsu / Saywell, Alex / Bonn, Mischa / Müllen, Klaus / Bogani, Lapo / Anderson, Harry L

Nature chemistry

2024

Abstract: Graphene nanoribbons (GNRs), nanometre-wide strips of graphene, are promising materials for fabricating electronic devices. Many GNRs have been reported, yet no scalable strategies are known for synthesizing GNRs with metal atoms and heteroaromatic units ...

Abstract	Graphene nanoribbons (GNRs), nanometre-wide strips of graphene, are promising materials for fabricating electronic devices. Many GNRs have been reported, yet no scalable strategies are known for synthesizing GNRs with metal atoms and heteroaromatic units at precisely defined positions in the conjugated backbone, which would be valuable for tuning their optical, electronic and magnetic properties. Here we report the solution-phase synthesis of a porphyrin-fused graphene nanoribbon (PGNR). This PGNR has metalloporphyrins fused into a twisted fjord-edged GNR backbone; it consists of long chains (>100 nm), with a narrow optical bandgap (~1.0 eV) and high local charge mobility (>400 cm
Language	English
Publishing date	2024-03-08
Publishing country	England
Document type	Journal Article
ZDB-ID	2464596-5
ISSN	1755-4349 ; 1755-4330
ISSN (online)	1755-4349
ISSN	1755-4330
DOI	10.1038/s41557-024-01477-1
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Article: Singly and Triply Linked Magnetic Porphyrin Lanthanide Arrays

Van Raden, Jeff M. / Alexandropoulos, Dimitris I. / Slota, Michael / Sopp, Simen / Matsuno, Taisuke / Thompson, Amber L. / Isobe, Hiroyuki / Anderson, Harry L. / Bogani, Lapo

Journal of the American Chemical Society. 2022 May 03, v. 144, no. 19

2022

Abstract: The introduction of paramagnetic metal centers into a conjugated π-system is a promising approach toward engineering spintronic materials. Here, we report an investigation of two types of spin-bearing dysprosium(III) and gadolinium(III) porphyrin dimers: ...

Abstract	The introduction of paramagnetic metal centers into a conjugated π-system is a promising approach toward engineering spintronic materials. Here, we report an investigation of two types of spin-bearing dysprosium(III) and gadolinium(III) porphyrin dimers: singly meso–meso-linked dimers with twisted conformations and planar edge-fused β,meso,β-linked tapes. The rare-earth spin centers sit out of the plane of the porphyrin, so that the singly linked dimers are chiral, and their enantiomers can be resolved, whereas the edge-fused tape complexes can be separated into syn and anti stereoisomers. We compare the crystal structures, UV–vis–NIR absorption spectra, electrochemistry, EPR spectroscopy, and magnetic behavior of these complexes. Low-temperature SQUID magnetometry measurements reveal intramolecular antiferromagnetic exchange coupling between the Gdᴵᴵᴵ centers in the edge-fused dimers (syn isomer: J = −51 ± 2 MHz; anti isomer: J = −19 ± 3 MHz), whereas no exchange coupling is detected in the singly linked twisted complex. The phase-memory times, Tₘ, are in the range of 8–10 μs at 3 K, which is long enough to test quantum computational schemes using microwave pulses. Both the syn and anti Dy₂ edge-fused tapes exhibit single-molecule magnetic hysteresis cycles at temperatures below 0.5 K with slow magnetization dynamics.
Keywords	absorption ; dysprosium ; electrochemistry ; electron paramagnetic resonance spectroscopy ; enantiomers ; ferrimagnetic materials ; gadolinium ; hysteresis ; magnetism ; porphyrins
Language	English
Dates of publication	2022-0503
Size	p. 8693-8706.
Publishing place	American Chemical Society
Document type	Article
ZDB-ID	3155-0
ISSN	1520-5126 ; 0002-7863
ISSN (online)	1520-5126
ISSN	0002-7863
DOI	10.1021/jacs.2c02084
Database	NAL-Catalogue (AGRICOLA)

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Article ; Online: Phase-Coherent Charge Transport through a Porphyrin Nanoribbon.

Chen, Zhixin / Deng, Jie-Ren / Hou, Songjun / Bian, Xinya / Swett, Jacob L / Wu, Qingqing / Baugh, Jonathan / Bogani, Lapo / Briggs, G Andrew D / Mol, Jan A / Lambert, Colin J / Anderson, Harry L / Thomas, James O

Journal of the American Chemical Society

2023 Volume 145, Issue 28, Page(s) 15265–15274

Abstract: Since the early days of quantum mechanics, it has been known that electrons behave simultaneously as particles and waves, and now quantum electronic devices can harness this duality. When devices are shrunk to the molecular scale, it is unclear under ... ...

Abstract	Since the early days of quantum mechanics, it has been known that electrons behave simultaneously as particles and waves, and now quantum electronic devices can harness this duality. When devices are shrunk to the molecular scale, it is unclear under what conditions does electron transmission remain phase-coherent, as molecules are usually treated as either scattering or redox centers, without considering the wave-particle duality of the charge carrier. Here, we demonstrate that electron transmission remains phase-coherent in molecular porphyrin nanoribbons connected to graphene electrodes. The devices act as graphene Fabry-Pérot interferometers and allow for direct probing of the transport mechanisms throughout several regimes. Through electrostatic gating, we observe electronic interference fringes in transmission that are strongly correlated to molecular conductance across multiple oxidation states. These results demonstrate a platform for the use of interferometric effects in single-molecule junctions, opening up new avenues for studying quantum coherence in molecular electronic and spintronic devices.
Language	English
Publishing date	2023-07-07
Publishing country	United States
Document type	Journal Article
ZDB-ID	3155-0
ISSN	1520-5126 ; 0002-7863
ISSN (online)	1520-5126
ISSN	0002-7863
DOI	10.1021/jacs.3c02451
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: N=8 Armchair Graphene Nanoribbons: Solution Synthesis and High Charge Carrier Mobility.

Yao, Xuelin / Zhang, Heng / Kong, Fanmiao / Hinaut, Antoine / Pawlak, Rémy / Okuno, Masanari / Graf, Robert / Horton, Peter N / Coles, Simon J / Meyer, Ernst / Bogani, Lapo / Bonn, Mischa / Wang, Hai I / Müllen, Klaus / Narita, Akimitsu

Angewandte Chemie (International ed. in English)

2023 Volume 62, Issue 46, Page(s) e202312610

Abstract: Structurally defined graphene nanoribbons (GNRs) have emerged as promising candidates for nanoelectronic devices. Low band gap (<1 eV) GNRs are particularly important when considering the Schottky barrier in device performance. Here, we demonstrate the ... ...

Abstract	Structurally defined graphene nanoribbons (GNRs) have emerged as promising candidates for nanoelectronic devices. Low band gap (<1 eV) GNRs are particularly important when considering the Schottky barrier in device performance. Here, we demonstrate the first solution synthesis of 8-AGNRs through a carefully designed arylated polynaphthalene precursor. The efficiency of the oxidative cyclodehydrogenation of the tailor-made polymer precursor into 8-AGNRs was validated by FT-IR, Raman, and UV/Vis-near-infrared (NIR) absorption spectroscopy, and further supported by the synthesis of naphtho[1,2,3,4-ghi]perylene derivatives (1 and 2) as subunits of 8-AGNR, with a width of 0.86 nm as suggested by the X-ray single crystal analysis. Low-temperature scanning tunneling microscopy (STM) and solid-state NMR analyses provided further structural support for 8-AGNR. The resulting 8-AGNR exhibited a remarkable NIR absorption extending up to ∼2400 nm, corresponding to an optical band gap as low as ∼0.52 eV. Moreover, optical-pump TeraHertz-probe spectroscopy revealed charge-carrier mobility in the dc limit of ∼270 cm
Language	English
Publishing date	2023-10-10
Publishing country	Germany
Document type	Journal Article
ZDB-ID	2011836-3
ISSN	1521-3773 ; 1433-7851
ISSN (online)	1521-3773
ISSN	1433-7851
DOI	10.1002/anie.202312610
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Article ; Online: Exceptionally clean single-electron transistors from solutions of molecular graphene nanoribbons.

Niu, Wenhui / Sopp, Simen / Lodi, Alessandro / Gee, Alex / Kong, Fanmiao / Pei, Tian / Gehring, Pascal / Nägele, Jonathan / Lau, Chit Siong / Ma, Ji / Liu, Junzhi / Narita, Akimitsu / Mol, Jan / Burghard, Marko / Müllen, Klaus / Mai, Yiyong / Feng, Xinliang / Bogani, Lapo

Nature materials

2023 Volume 22, Issue 2, Page(s) 180–185

Abstract: Only single-electron transistors with a certain level of cleanliness, where all states can be properly accessed, can be used for quantum experiments. To reveal their exceptional properties, carbon nanomaterials need to be stripped down to a single ... ...

Abstract	Only single-electron transistors with a certain level of cleanliness, where all states can be properly accessed, can be used for quantum experiments. To reveal their exceptional properties, carbon nanomaterials need to be stripped down to a single element: graphene has been exfoliated into a single sheet, and carbon nanotubes can reveal their vibrational, spin and quantum coherence properties only after being suspended across trenches
Language	English
Publishing date	2023-02-02
Publishing country	England
Document type	Journal Article
ZDB-ID	2088679-2
ISSN	1476-4660 ; 1476-1122
ISSN (online)	1476-4660
ISSN	1476-1122
DOI	10.1038/s41563-022-01460-6
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Article ; Online: Electronically Reconfigurable Photonic Switches Incorporating Plasmonic Structures and Phase Change Materials.

Farmakidis, Nikolaos / Youngblood, Nathan / Lee, June Sang / Feldmann, Johannes / Lodi, Alessandro / Li, Xuan / Aggarwal, Samarth / Zhou, Wen / Bogani, Lapo / Pernice, Wolfram Hp / Wright, C David / Bhaskaran, Harish

Advanced science (Weinheim, Baden-Wurttemberg, Germany)

2022 Volume 9, Issue 20, Page(s) e2200383

Abstract: The ever-increasing demands for data processing and storage will require seamless monolithic co-integration of electronics and photonics. Phase-change materials are uniquely suited to fulfill this function due to their dual electro-optical sensitivity, ... ...

Abstract	The ever-increasing demands for data processing and storage will require seamless monolithic co-integration of electronics and photonics. Phase-change materials are uniquely suited to fulfill this function due to their dual electro-optical sensitivity, nonvolatile retention properties, and fast switching dynamics. The extreme size disparity however between CMOS electronics and dielectric photonics inhibits the realization of efficient and compact electrically driven photonic switches, logic and routing elements. Here, the authors achieve an important milestone in harmonizing the two domains by demonstrating an electrically reconfigurable, ultra-compact and nonvolatile memory that is optically accessible. The platform relies on localized heat, generated within a plasmonic structure; this uniquely allows for both optical and electrical readout signals to be interlocked with the material state of the PCM while still ensuring that the writing operation is electrically decoupled. Importantly, by miniaturization and effective thermal engineering, the authors achieve unprecedented energy efficiency, opening up a path towards low-energy optoelectronic hardware for neuromorphic and in-memory computing.
Language	English
Publishing date	2022-04-17
Publishing country	Germany
Document type	Journal Article
ZDB-ID	2808093-2
ISSN	2198-3844 ; 2198-3844
ISSN (online)	2198-3844
ISSN	2198-3844
DOI	10.1002/advs.202200383
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Exchange-induced spin polarization in a single magnetic molecule junction.

Pei, Tian / Thomas, James O / Sopp, Simen / Tsang, Ming-Yee / Dotti, Nicola / Baugh, Jonathan / Chilton, Nicholas F / Cardona-Serra, Salvador / Gaita-Ariño, Alejandro / Anderson, Harry L / Bogani, Lapo

Nature communications

2022 Volume 13, Issue 1, Page(s) 4506

Abstract: Many spintronic devices rely on the presence of spin-polarized currents at zero magnetic field. This is often obtained by spin exchange-bias, where an element with long-range magnetic order creates magnetized states and displaces the hysteresis loop. ... ...

Abstract	Many spintronic devices rely on the presence of spin-polarized currents at zero magnetic field. This is often obtained by spin exchange-bias, where an element with long-range magnetic order creates magnetized states and displaces the hysteresis loop. Here we demonstrate that exchange-split spin states are observable and usable in the smallest conceivable unit: a single magnetic molecule. We use a redox-active porphyrin as a transport channel, coordinating a dysprosium-based single-molecule-magnet inside a graphene nano-gap. Single-molecule transport in magnetic field reveals the existence of exchange-split channels with different spin-polarizations that depend strongly on the field orientation, and comparison with the diamagnetic isostructural compound and milikelvin torque magnetometry unravels the role of the single-molecule anisotropy and the molecular orientation. These results open a path to using spin-exchange in molecular electronics, and offer a method to quantify the internal spin structure of single molecules in multiple oxidation states.
Language	English
Publishing date	2022-08-03
Publishing country	England
Document type	Journal Article
ZDB-ID	2553671-0
ISSN	2041-1723 ; 2041-1723
ISSN (online)	2041-1723
ISSN	2041-1723
DOI	10.1038/s41467-022-31909-w
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Article ; Online: Singly and Triply Linked Magnetic Porphyrin Lanthanide Arrays.

Van Raden, Jeff M / Alexandropoulos, Dimitris I / Slota, Michael / Sopp, Simen / Matsuno, Taisuke / Thompson, Amber L / Isobe, Hiroyuki / Anderson, Harry L / Bogani, Lapo

Journal of the American Chemical Society

2022 Volume 144, Issue 19, Page(s) 8693–8706

Abstract	The introduction of paramagnetic metal centers into a conjugated π-system is a promising approach toward engineering spintronic materials. Here, we report an investigation of two types of spin-bearing dysprosium(III) and gadolinium(III) porphyrin dimers: singly
Language	English
Publishing date	2022-05-03
Publishing country	United States
Document type	Journal Article
ZDB-ID	3155-0
ISSN	1520-5126 ; 0002-7863
ISSN (online)	1520-5126
ISSN	0002-7863
DOI	10.1021/jacs.2c02084
Database	MEDical Literature Analysis and Retrieval System OnLINE

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