Towards Rational Modulation of In‐Plane Molecular Arrangements in Metal–Organic Framework Nanosheets

Makiura, Rie; Usui, Ryo; Sakai, Yuta; Nomoto, Akihiro; Ogawa, Akiya; Sakata, Osami; Fujiwara, Akihiko

doi:10.1002/cplu.201402150

Cited by 53 publications

(35 citation statements)

References 52 publications

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“…Adequate compression of the preassembled domains is key to yield the obtained dense full substrate coverage. Indeed, transfer conducted at 0.5 mN m −1 only provides an uneven partial coverage (Figure S26, Supporting Information), while higher surface pressures (above 30 mN m −1 for metalloporphyrin analogs) result in increased surface roughness due to deformation or stacking of neighboring sheets.…”

Section: Resultsmentioning

confidence: 99%

“…The advantages of this method for our objectives are the robustness of the metalloporphyrin core, the coherence of bulk deposits in terms of structural phase and 2D layer domains, and their demonstrated stability. [17b] Interestingly, the method has also been successfully extended to [Pd(H 4 TCPP)], as well as to ditopic and extended analogs of H 6 TCPP . Nonetheless, this research has mainly been aimed at crystal engineering goals, and so far only paramagnetic Cu(II) ions have been used for the paddle‐wheel node connecting the metalloporphyrin units.…”

Section: Introductionmentioning

confidence: 99%

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A Porphyrin Spin Qubit and Its 2D Framework Nanosheets

Urtizberea

Natividad

Alonso

et al. 2018

Adv Funct Materials

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Molecular spin qubits have been shown to reach sufficiently long quantum coherence times to envision their use as hardware in quantum processors. These will however require their implementation in hybrid solid-state devices for which the controlled localization and homogeneous orientation of the molecular qubits will be necessary. An alternative to isolated molecules that can ensure these key aspects is 2D framework in which the qubit would act as node. In this work, it is demonstrated that the isolated metalloporphyrin [Cu(H 4 TCPP)] molecule is a potential spin qubit, and maintains similar quantum coherence as node in a 2D [{CuTCPP}Zn 2 (H 2 O) 2 ] metal-organic framework. Mono-and multilayer deposits of nanosheets of a similar 2D framework are then successfully formed following a modular method based on Langmuir-Schaefer conditions. The orientation of the {CuTCPP} qubit nodes in these nanosheets is homogeneous parallel to the substrate. These nanosheets are also formed with a control over the qubit concentration, i.e., by dilution with the unmetallated porphyrin. Eventually, 2D nanosheets are formed in situ directly on a substrate, through a simple protocol devised to reproduce the Langmuir-Schaefer conditions locally. Altogether these studies show that 2D spin qubit frameworks are ideal components to develop a hybrid quantum computing architecture. and gates first arose in the form of purely organic systems, using either the multiple nuclear spins of rationally selected molecules or the electronic spin(s) of open shell organic molecules bearing one or multiple radicals. The careful design and selection of such organic molecules coupled to sophisticated experiments have allowed implementing realistic quantum operations using ensembles of these. [2] Paramagnetic coordination complexes were later proposed as alternative molecular spin qubits, after it was argued and shown that the molecule electronic spin orientation and quantum superpositions allow to encode quantum bit (qubit) states. [3] Recent improvements in the coherence times of these molecular spin qubits [4] and the unique ability to design molecules with multiple qubits as prototypes of quantum gates [5] have brought this scheme to a point where it becomes reasonable to envision the design of a magnetic quantum processor. A magnetic molecule has even recently been used to implement Grover's quantum algorithm, albeit using its metal ion nuclear spin. [6] One of the advantages of the molecular scheme is that macroscopic numbers of identical qubits are obtained in one sole reaction. While this is appealing for the daunting challenge of scaling to a usable size, common to all proposed schemes, [7] the technology to build a scalable quantum architecture based on molecular qubits is

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

A Porphyrin Spin Qubit and Its 2D Framework Nanosheets

Urtizberea

Natividad

Alonso

et al. 2018

Adv Funct Materials

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“…[179][180][181][182][183][184] In the following paragraphs, we will briefly introduce the synthesis of MOF nanosheets at various interfaces, including air-liquid, liquid-liquid, and solid-liquid interfaces. [179][180][181][182][183][184] In the following paragraphs, we will briefly introduce the synthesis of MOF nanosheets at various interfaces, including air-liquid, liquid-liquid, and solid-liquid interfaces.…”

Section: Interfacial Growthmentioning

confidence: 99%

Structural Engineering of Low‐Dimensional Metal–Organic Frameworks: Synthesis, Properties, and Applications

et al. 2019

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Low‐dimensional metal–organic frameworks (LD MOFs) have attracted increasing attention in recent years, which successfully combine the unique properties of MOFs, e.g., large surface area, tailorable structure, and uniform cavity, with the distinctive physical and chemical properties of LD nanomaterials, e.g., high aspect ratio, abundant accessible active sites, and flexibility. Significant progress has been made in the morphological and structural regulation of LD MOFs in recent years. It is still of great significance to further explore the synthetic principles and dimensional‐dependent properties of LD MOFs. In this review, recent progress in the synthesis of LD MOF‐based materials and their applications are summarized, with an emphasis on the distinctive advantages of LD MOFs over their bulk counterparties. First, the unique physical and chemical properties of LD MOF‐based materials are briefly introduced. Synthetic strategies of various LD MOFs, including 1D MOFs, 2D MOFs, and LD MOF‐based composites, as well as their derivatives, are then summarized. Furthermore, the potential applications of LD MOF‐based materials in catalysis, energy storage, gas adsorption and separation, and sensing are introduced. Finally, challenges and opportunities of this fascinating research field are proposed.

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“…In Zukunft sollten vermehrt Neutronen-und Synchrotronrçntgenstrahlung unter streifendem Einfallswinkel verwendet werden, die einzigartige Beiträge zur Aufklärung der Grçße und Orientierung von Kristalldomänen in Monomer-und 2D-Polymerfilmen liefern kçnnen. [177] Auch der Anteil der in den Angewandte Chemie Aufsätze…”

Section: Angewandte Chemieunclassified

Makroskopische kristalline 2D‐Polymere

Feng

Schlüter²

2018

Angewandte Chemie

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Monolagen mit interner Periodizität können als 2D‐Polymere oder “molekulare Fischernetze” beschrieben werden. Solche Strukturen sind in der Vergangenheit durch photochemische Reaktionen in Einkristallen hergestellt worden, die aus Monomeren mit spezifisch entworfenen Strukturen bestehen. Einzelne Schichten wurden später durch Exfolierung isoliert. Diese milden Bedingungen ermöglichen zwar exzellente Kontrolle über die gebildete Struktur, allerdings ist die Ausdehnung der erhaltenen 2D‐Polymere durch die Kristallausdehnung limitiert. Dieser Aufsatz befasst sich mit Ansätzen zur Herstellung von 2D‐Polymeren mit makroskopischen lateralen Abmessungen. Solche Abmessungen sind zugänglich, wenn Polymerisationsreaktionen an Grenzflächen zwischen zwei Flüssigkeiten bzw. zwischen einer Flüssigkeit und einem Gas (besonders der Wasser/Luft‐Grenzfläche) durchgeführt werden. Damit lassen sich zwar prinzipiell 2D‐Polymere makroskopischer Größe erzeugen, allerdings eröffnen sich neue analytische Probleme. Einige dieser Herausforderungen werden besprochen und die vielversprechendsten Lösungsansätze hervorgehoben. Anhand dreier repräsentativer Strukturen demonstriert dieser Aufsatz den gegenwärtigen Stand der Technik im noch jungen Feld der 2D‐Polymeranalytik. Zuletzt werden mögliche Anwendungen für neue organische 2D‐Materialien beschrieben, z. B. als Nanomembranen, organische (opto)elektronische Komponenten oder Katalysatoren für die Wasserspaltung.

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Towards Rational Modulation of In‐Plane Molecular Arrangements in Metal–Organic Framework Nanosheets

Cited by 53 publications

References 52 publications

A Porphyrin Spin Qubit and Its 2D Framework Nanosheets

A Porphyrin Spin Qubit and Its 2D Framework Nanosheets

Structural Engineering of Low‐Dimensional Metal–Organic Frameworks: Synthesis, Properties, and Applications

Makroskopische kristalline 2D‐Polymere

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