4.7 Article

Tuning of molecular qubits: very long coherence and spin-lattice relaxation times

Journal

CHEMICAL COMMUNICATIONS
Volume 52, Issue 18, Pages 3623-3626

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/c6cc00300a

Keywords

-

Funding

  1. Fonds der Chemischen Industrie

Ask authors/readers for more resources

We report a pulsed EPR study on different transition metal phthalocyanines, elucidating the dependence of spin relaxation on solvent, ligand and metal ion. Coherence times of >40 mu s and spin-lattice relaxation times of up to 2 s were found. Minimization of SOMO-environment overlap leads to increased coherence times.

Authors

I am an author on this paper
Click your name to claim this paper and add it to your profile.

Reviews

Primary Rating

4.7
Not enough ratings

Secondary Ratings

Novelty
-
Significance
-
Scientific rigor
-
Rate this paper

Recommended

Article Chemistry, Physical

Dark Matter: Peculiarities within the Li1-xRE5+xW8O32 series (RE = Dy - Lu)

Katharina Dorn, Bjoern Blaschkowski, Heiko Bamberger, Joris van Slageren, Marc Widenmeyer, Anke Weidenkaff, Emmanuelle Suard, Ingo Hartenbach

Summary: The derivatives of the Li1-xRE5+xW8O32 series (RE = Dy-Lu) crystallize in the monoclinic system with C-center symmetry. These compounds exhibit a mixed occupation of Li+ and RE3+ cations in their crystal structures, with a deficiency of lithium leading to an excess of positive charges in the formula.

JOURNAL OF ALLOYS AND COMPOUNDS (2021)

Article Chemistry, Inorganic & Nuclear

A nonsymmetric Dy2 single-molecule magnet with two relaxation processes triggered by an external magnetic field: a theoretical and integrated EPR study of the rote of magnetic-site dilution

Nikolia Lalioti, Vassilis Nastopoulos, Nikos Panagiotou, Anastasios Tasiopoulos, Nikolaos Ioannidis, Joris van Slageren, Peng Zhang, Gopalan Rajaraman, Abinash Swain, Vassilis Tangoulis

Summary: The reaction between Dy(O2CMe)(3)•4H(2)O and 1-acetyl-2-napthol (LH) in MeOH yielded the complex [Dy2L6(MeOH)]•MeOH (1•MeOH) with good success. Characterization was done through single-crystal X-ray crystallography, elemental analyses, IR spectra, and powder X-ray patterns. The complex showed slow magnetic relaxation with a single relaxation mechanism under a 0 Oe dc field and two relaxation processes under a 1500 G external magnetic field.

DALTON TRANSACTIONS (2022)

Article Chemistry, Inorganic & Nuclear

(Spectro)Electrochemistry of 3-(Pyrid-2-yl)-s-Tetrazine- and 1,2-(Dihydro)pyridazine Tricarbonylrhenium(I)chloride

Marc Schnierle, Mario Winkler, Vasileios Filippou, Joris van Slageren, Mark R. Ringenberg

Summary: The electrochemistry and spectroelectrochemistry of three [ReCl(CO)(3)(N N)] complexes were investigated with N N=3-(pyrid-2-yl)-1,2,4,5-tetrazine [1], 3-(pyrid-2-yl)-4-ferrocenyl-4,5-dihydropyridazine [1H(2)Fc], and 3-(pyrid-2-yl)-4-ferrocenyl-pyridazine [1Fc]. The conjugation of the ligands was found to affect the reduction potentials and intramolecular charge transfers observed in the UV-vis-NIR spectrum, with support from DFT calculations.

EUROPEAN JOURNAL OF INORGANIC CHEMISTRY (2022)

Article Materials Science, Multidisciplinary

Composition and magnetic properties of thin films grown by interdiffusion of Mn and Sn-Rich, Ge lattice matched SixGe1-x-ySny layers

Hannes S. Funk, Michal Kern, David Weisshaupt, Christoph Suergers, Inga A. Fischer, Michael Oehme, Joris van Slageren, Joerg Schulze

Summary: This study investigates the structure and magnetic properties of Mn-based ferromagnetic layers on the semiconductor SixGe1-x-ySny with different Sn content compared to layers on Ge and Si0.75Ge0.25. The samples exhibit phase separation into Si-rich and Ge-rich Mn compounds, with all samples being ferromagnetic. Saturation magnetization decreases and coercive field increases with higher Si content x. The Curie temperature does not show a clear trend with increasing Si content. Based on composition, structure, and magnetic properties, a two-layer model is proposed to explain the observed magnetic behavior with Si content playing a key role.

JOURNAL OF MAGNETISM AND MAGNETIC MATERIALS (2022)

Letter Multidisciplinary Sciences

Reply to: [{Th(C8H8)Cl2}3]2- is stable but not aromatic

Josef T. Boronski, John A. Seed, David Hunger, Adam W. Woodward, Joris van Slageren, Ashley J. Wooles, Louise S. Natrajan, Nikolas Kaltsoyannis, Stephen T. Liddle

NATURE (2022)

Article Chemistry, Multidisciplinary

Remarkable Enhancement of Catalytic Activity of Cu-Complexes in the Electrochemical Hydrogen Evolution Reaction by Using Triply Fused Porphyrin

Shubhadeep Chandra, Arijit Singha Hazari, Qian Song, David Hunger, Nicolas. I. Neuman, Joris van Slageren, Elias Klemm, Biprajit Sarkar

Summary: A bimetallic triply fused copper(II) porphyrin complex shows remarkable catalytic activity for the electrochemical hydrogen evolution reaction, with lower overpotential and higher faradaic efficiency compared to the monomeric complex.

CHEMSUSCHEM (2022)

Article Chemistry, Inorganic & Nuclear

Facile Synthesis and Characterization of Pure Tochilinite-like Materials from Nanoparticulate FeS

Robert Bolney, Mario Grosch, Mario Winkler, Joris van Slageren, Wolfgang Weigand, Christian Robl

Summary: Three different tochilinite-like materials were synthesized using sophisticated methods that control the distribution of iron ions. Analyses confirmed their purity and allowed for determination of their detailed compositions. The obtained powders consist of thin sheets and nanotubes with varying thermal stability depending on the composition.

ZEITSCHRIFT FUR ANORGANISCHE UND ALLGEMEINE CHEMIE (2022)

Article Chemistry, Multidisciplinary

Modular Approach to Creating Functionalized Surface Arrays of Molecular Qubits

Lorenzo Tesi, Friedrich Stemmler, Mario Winkler, Sherri S. Y. Liu, Saunak Das, Xiuming Sun, Michael Zharnikov, Sabine Ludwigs, Joris van Slageren

Summary: The development of quantum technologies aims to achieve exponentially faster computations, ultrahigh performance sensing, and a comprehensive understanding of many-particle quantum systems. Molecular spins have emerged as excellent candidates for qubits due to their long coherence times, tunability through chemical synthesis, and compatibility with other quantum platforms. However, integrating molecular spin qubits into quantum devices and preserving their quantum properties on surfaces remains a challenge. This study presents a versatile bottom-up approach to arrange molecular qubits as self-assembled monolayers on surfaces, demonstrating the maintenance or even enhancement of qubit properties.

ADVANCED MATERIALS (2023)

Article Chemistry, Multidisciplinary

Towards Luminescent Vanadium(II) Complexes with Slow Magnetic Relaxation and Quantum Coherence

Matthias Dorn, David Hunger, Christoph Foerster, Robert Naumann, Joris van Slageren, Katja Heinze

Summary: Molecular entities with doublet or triplet ground states are being increasingly studied as potential qubits. Vanadium(II) ions in octahedral ligand fields with quartet ground states are considered as qubits with potential luminescent spin-flip states. Two V2+ complexes, [V(ddpd)(2)](2+), with the strong field ligand N,N'-dimethyl-N,N'-dipyridine-2-yl-pyridine-2,6-diamine (ddpd) in two isomeric forms (cis-fac and mer), were identified as suitable candidates. The energy gaps between the two lowest Kramers doublets allow pulsed EPR experiments at conventional Q-band frequencies. Both isomers have relatively long spin-lattice relaxation times and a phase memory time at low temperatures. Furthermore, the mer isomer shows slow magnetic relaxation in an applied field. The [V(ddpd)(2)](2+) complexes are non-luminescent due to charge transfer admixture to the spin-flip states.

CHEMISTRY-A EUROPEAN JOURNAL (2022)

Article Chemistry, Multidisciplinary

Molecular One- and Two-Qubit Systems with Very Long Coherence Times

Dennis Schaefter, Jonathan Wischnat, Lorenzo Tesi, J. Alejandro De Sousa, Edmund Little, Jake McGuire, Marta Mas-Torrent, Concepcio Rovira, Jaume Veciana, Floriana Tuna, Nuria Crivillers, Joris van Slageren

Summary: In this article, the spin dynamics of chlorinated triphenylmethyl organic radicals were investigated, revealing long ensemble coherence times and the achievement of two-qubit and individual qubit addressability in the biradical system. These results highlight the potential of molecular materials in the development of quantum architectures.

ADVANCED MATERIALS (2023)

Article Chemistry, Multidisciplinary

Enhancing SIM behaviour in a mononuclear tetrahedral [Co(N,N′-2-iminopyrrolyl)2] complex

Patricia S. Ferreira, Jose F. Malta, Nuno A. G. Bandeira, Alexander Allgaier, Joris van Slageren, Jose A. Paixao, Manuel Almeida, Laura C. J. Pereira, Pedro T. Gomes

Summary: A new homoleptic Co(ii) complex with two highly sterically congested 2-formiminopyrrolyl N,N'-chelating ligands is reported, showing slow relaxation of magnetization at zero static field. This compound has a large zero-field splitting parameter D of -42.6(4) cm(-1), resulting in a spin-reversal energy barrier U-eff of 85 cm(-1).

CHEMICAL COMMUNICATIONS (2022)

Article Chemistry, Inorganic & Nuclear

Single-ion magnet behaviour in homoleptic Co(II) complexes bearing 2-iminopyrrolyl ligands

Patricia S. Ferreira, Ana C. Cerdeira, Tiago F. C. Cruz, Nuno A. G. Bandeira, David Hunger, Alexander Allgaier, Joris van Slageren, Manuel Almeida, Laura C. J. Pereira, Pedro T. Gomes

Summary: In this study, the authors characterized the structure and magnetic properties of four distorted tetrahedral homoleptic Co(II) complexes. These complexes exhibit Single-Ion Magnet (SIM) behavior, with large and negative magnetic anisotropy. Theoretical calculations showed that the axial anisotropy is mainly caused by electronic transitions, and the structural distortion was also explained and reproduced by calculations.

INORGANIC CHEMISTRY FRONTIERS (2022)

Article Chemistry, Multidisciplinary

Mackinawite-Supported Reduction of C1 Substrates into Prebiotically Relevant Precursors

Mario Grosch, Martin T. Stiebritz, Robert Bolney, Mario Winkler, Eric Jueckstock, Hannah Busch, Sophia Peters, Alexander F. Siegle, Joris van Slageren, Markus Ribbe, Yilin Hu, Oliver Trapp, Christian Robl, Wolfgang Weigand

Summary: This study provides evidence for mackinawite-supported reduction of KCN and proposes a reaction mechanism. The findings open new avenues for investigating other substrates for mackinawite-supported reactions and shed light on the relevance of this type of reaction to the origin of life on Earth.

CHEMSYSTEMSCHEM (2022)

Article Chemistry, Multidisciplinary

Three individually addressable spin qubits in a single molecule

Ivana Borilovic, Olivier Roubeau, Boris Le Guennic, Joris van Slageren, Samuel Lenz, Simon J. Teat, Guillem Aromi

Summary: An asymmetric bis-phenol-beta-diketone (H4L) has been designed as a ligand that promotes the assembly of three magnetically exchanged [NiCu] pairs, each exhibiting an S = 1/2 spin. EPR and magnetometry measurements show that these pairs are good qubit realizations and non-equivalent within the molecule in the solid state, meeting the requirements for conditional quantum gates.

CHEMICAL COMMUNICATIONS (2022)

Article Chemistry, Multidisciplinary

A mesoionic carbene complex of manganese in five oxidation states

Benjamin Wittwer, Nicole Dickmann, Stephan Berg, Daniel Leitner, Lorenzo Tesi, David Hunger, Raphael Gratzl, Joris van Slageren, Nicolas Neuman, Dominik Munz, Stephan Hohloch

Summary: This study elucidates the electronic structure of a rare manganese complex formed by the reaction between a carbazole-based mesoionic carbene ligand and manganese(ii) iodide using a combination of chemical, spectroscopic, magnetic, and computational techniques.

CHEMICAL COMMUNICATIONS (2022)

Review Chemistry, Multidisciplinary

Trap suppression in ordered organic photovoltaic heterojunctions

Dan He, Yawen Li, Fuwen Zhao, Yuze Lin

Summary: High trap density in organic solar cells leads to localized charge carriers and reduced carrier lifetime, limiting device efficiency. This feature article summarizes the recent advances of trap suppression by material design and device engineering.

CHEMICAL COMMUNICATIONS (2024)

Review Chemistry, Multidisciplinary

Controversial mechanism of simultaneous photocatalysis and Fenton-based processes: additional effect or synergy?

Olivier Monfort, Arshitha Madhusudhan, Martin Motola

Summary: This article presents the advantages of coupling photocatalysis and Fenton-based processes for environmental remediation and discusses their synergy. It critically examines the simultaneous triggering of these two processes and provides insights into research approaches. The study aims to enhance understanding of this complex process and highlight the potential integration of new catalysts in current wastewater treatment technology.

CHEMICAL COMMUNICATIONS (2024)

Article Chemistry, Multidisciplinary

Polymerization of monomer aggregates for tailoring and patterning water wettability

Manideepa Dhar, Chittaranjan Mishra, Avijit Das, Uttam Manna

Summary: An approach of 'polymerization of monomers in its aggregated form' has been introduced to tailor the water wettability of fibrous and porous substrates, achieving hydrophobicity to superhydrophobicity transition, as well as patterned wettability. This facile chemical method provides a durable coating with adjustable and patterned wettability for various potential applications.

CHEMICAL COMMUNICATIONS (2024)

Article Chemistry, Multidisciplinary

Pd/Brønsted acid catalysed intramolecular N-allylation of indoles and pyrroles with alkynes for the synthesis of N-fused heterocycles

Saswat Ranjan Bhoi, Chhanda Debnath, Shikha Gandhi

Summary: In this article, a novel catalytic reaction using Pd(0) and Bronsted acid is reported for the synthesis of biologically important imidazolidinone-fused N-heterocycles through redox-neutral intramolecular N-allylation of indoles and pyrroles with alkynes. This atom-economical method is applicable to a wide range of substrates and eliminates the need for leaving groups or oxidizing agents commonly used in traditional allylation reactions.

CHEMICAL COMMUNICATIONS (2024)

Article Chemistry, Multidisciplinary

Rh(III)-catalyzed selective mono- and dual-functionalization/cyclization of 1-aryl-5-aminopyrazoles with iodonium ylides

Longkun Chen, Mingshuai Zhang, Meichen Liu, Zhuoyuan Liu, Yuetong Qiu, Zhilai Zhang, Fuchao Yu, Jiuzhong Huang

Summary: In this study, an efficient Rh(III)-catalyzed selective mono- and dual-C-H bond functionalization/cyclization with iodonium ylide as the sole coupling partner was demonstrated. Fused benzodiazepine skeletons were obtained in excellent yields, providing an improved approach to dual C-H unsymmetrical functionalization.

CHEMICAL COMMUNICATIONS (2024)

Article Chemistry, Multidisciplinary

Modified minimal-size fragments of heparan sulfate as inhibitors of endosulfatase-2 (Sulf-2)

Alice Kennett, Sven Epple, Gabriella van der Valk, Irene Georgiou, Evelyne Gout, Romain R. Vives, Angela J. Russell

Summary: This study presents the design and synthesis of sulfated disaccharide inhibitors based on IdoA(2S)-GlcNS(6S), which showed potent inhibition of Sulf-2. The results suggest that IdoA(2S)-GlcNS(6S) is the shortest fragment size required for effective inhibition of Sulfs, and a trisulfated disaccharide is identified as the minimal fragment size of heparan sulfate for effective endosulfatase inhibition.

CHEMICAL COMMUNICATIONS (2024)

Article Chemistry, Multidisciplinary

Reductive cyclodimerization of chalcones: exploring the self-adaptability of galvanostatic electrosynthesis

Mauro Garbini, Andrea Brunetti, Riccardo Pedrazzani, Magda Monari, Massimo Marcaccio, Giulio Bertuzzi, Marco Bandini

Summary: The self-adaptability of galvanostatic electrolysis was found to be helpful in a multistage chemo- and diastereoselective electrochemically promoted cyclodimerization of chalcones. Through a series of reductive events, densely functionalized cyclopentanes with five contiguous stereocenters were obtained (25 examples, yields up to 95%, dr values up to >20:1). Further experimental and electrochemical investigations indicated the crucial role of dynamic kinetic resolution of the aldol intermediate in the reaction mechanism.

CHEMICAL COMMUNICATIONS (2024)

Article Chemistry, Multidisciplinary

Rh(III)-catalyzed oxidative [4+2] annulation of 2-arylquinoxalines and 2-aryl-2H-indazoles with allyl alcohols

Dhananjay S. Nipate, Neha Meena, Prakash N. Swami, Krishnan Rangan, Anil Kumar

Summary: In this study, the synthesis of functionalized benzo[a]phenazines and indazolo[2,3-a]quinolines was achieved through Rh(III)-catalyzed oxidative annulation of 2-arylquinoxalines and 2-aryl-2H-indazoles with allyl alcohols. The method showed a wide substrate scope, excellent functional group tolerance, good to high yields of annulated products, and the capability for scaled-up synthesis. A tentative mechanism of the annulation reaction was proposed based on a preliminary mechanistic investigation.

CHEMICAL COMMUNICATIONS (2024)

Article Chemistry, Multidisciplinary

PbTeB4O9: a lead tellurium borate with unprecedented fundamental building block [B4O10] and large birefringence

Ruonan Zhang, Abudukadi Tudi, Xia Yang, Xuping Wang, Zhihua Yang, Shujuan Han, Shilie Pan

Summary: A new lead tellurium borate material with a unique fundamental building block [B4O10] was synthesized and found to exhibit high birefringence. The structure-property relationship was discussed using first-principles calculations.

CHEMICAL COMMUNICATIONS (2024)

Article Chemistry, Multidisciplinary

Wafer-scale synthesis of two-dimensional ultrathin films

Amresh Kumar Singh, Baishali Thakurta, Anupam Giri, Monalisa Pal

Summary: This study introduces three key concepts for the quick synthesis of large-scale high-quality 2D materials films and their utilization in device fabrication.

CHEMICAL COMMUNICATIONS (2024)

Article Chemistry, Multidisciplinary

Precise design of copolymer-conjugated nanocatalysts for active electron transfer

Reina Hagiwara, Shun Nishimura, Kosuke Okeyoshi

Summary: A copolymer-conjugated nanocatalytic system has been developed to improve electron transfer and enhance photoinduced H2 generation.

CHEMICAL COMMUNICATIONS (2024)