Domain wall motion is detected for the first time during the transition to a ferroelastic and spin state ordered phase of a spin crossover complex. Single‐crystal X‐ray diffraction and resonant ultrasound spectroscopy (RUS) revealed two distinct symmetry‐breaking phase transitions in the mononuclear Mn 3+ compound [Mn(3,5‐diBr‐sal 2 (323))]BPh 4 , 1. The first at 250 K, involves the space group change Cc → Pc and is thermodynamically continuous, while the second, Pc → P 1 at 85 K, is discontinuous and related to spin crossover and spin state ordering. Stress‐induced domain wall mobility was interpreted on the basis of a steep increase in acoustic loss immediately below the the Pc ‐ P 1 transition
Pinned and mobile ferroelastic domain walls are detected in response to mechanical stress in a Mn 3+ complex with two-step thermal switching between the spin triplet and spin quintet forms. Single-crystal X-ray diffraction and resonant ultrasound spectroscopy on [Mn III (3,5-diCl-sal 2 (323))]BPh 4 reveal three distinct symmetry-breaking phase transitions in the polar space group series Cc → Pc → P 1 → P 1 (1/2) . The transition mechanisms involve coupling between structural and spin state order parameters, and the three transitions are Landau tricritical, first order, and first order, respectively. The two first-order phase transitions also show changes in magnetic properties and spin state ordering in the Jahn–Teller-active Mn 3+ complex. On the basis of the change in symmetry from that of the parent structure, Cc , the triclinic phases are also ferroelastic, which has been confirmed by resonant ultrasound spectroscopy. Measurements of magnetoelectric coupling revealed significant changes in electric polarization at both the Pc → P 1 and P 1 → P 1 (1/2) transitions, with opposite signs. All these phases are polar, while P 1 is also chiral. Remanent electric polarization was detected when applying a pulsed magnetic field of 60 T in the P 1→ P 1 (1/2) region of bistability at 90 K. Thus, we showcase here a rare example of multifunctionality in a spin crossover material where the strain and polarization tensors and structural and spin state order parameters are strongly coupled.
We investigate giant magnetoelectric coupling at a Mn 3+ spin crossover in [Mn III L]BPh4 (L = (3,5-diBr-sal)2323) with field-induced permanent switch of the structural, electric and magnetic properties. An applied magnetic field induces a 1 st order phase transition from a high spin/low spin (HS-LS) ordered phase to a HS-only phase at 87.5 K that remains after the field is removed. We observe this unusual effect for DC magnetic fields as low as 8.7 T. The spin-state switching driven by the magnetic field in the bistable molecular material is accompanied by a change in electric polarization amplitude and direction due to a symmetry-breaking phase transition between polar space groups. The magnetoelectric coupling occurs due to a γη 2 coupling between the order parameter γ related to the spin-state bistability, and the symmetry-breaking order parameter η, responsible for the change of symmetry between polar structural phases. We also observe conductivity occurring during the spin crossover, and evaluate the possibility that it results from conducting phase boundaries. We perform ab-initio calculations to understand the origin of the electric polarization change as well as the conductivity during the spin crossover. Thus we demonstrate a giant magnetoelectric effect with a field-induced electric polarization change that is 1/10 of the record for any material.
Domain wall motion is detected for the first time during the transition to af erroelastic and spin state ordered phase of as pin crossover complex. Single-crystal X-ray diffraction and resonant ultrasound spectroscopy(RUS) revealed two distinct symmetry-breaking phase transitions in the mononuclear Mn 3+ compound [Mn(3,5-diBr-sal 2-(323))]BPh 4 ,1 .T he first at 250 K, involves the space group change Cc!Pc and is thermodynamically continuous,w hile the second, Pc!P1 at 85 K, is discontinuous and related to spin crossover and spin state ordering. Stress-induced domain wall mobility was interpreted on the basis of asteep increase in acoustic loss immediately belowt he the Pc-P1 transition
A MnIII spin crossover complex with atypical two‐step hysteretic thermal switching at 74 K and 84 K shows rich structural–magnetic interplay and magnetic‐field‐induced spin state switching below 14 T with an onset below 5 T. The spin states, structures, and the nature of the phase transitions are elucidated via X‐ray and magnetization measurements. An unusual intermediate phase containing four individual sites, where 1/4 are in a pure low spin state, is observed. The splitting of equivalent sites in the high temperature phase into four inequivalent sites is due to a structural reorganization involving a primary and a secondary symmetry‐breaking order parameter that induces a crystal system change from orthorhombic→monoclinic and a cell doubling. Further cooling leads to a reconstructive phase transition and a monoclinic low‐temperature phase with two inequivalent low‐spin sites. The coupling between the order parameters is identified in the framework of Landau theory.
In an interview with Benjamin List, winner of the 2021 Nobel Prize in Chemistry, members of the Young Chemists’ Network (JCF) of the German Chemical Society (GDCh) asked him about his science, his career, and the academic system. Benjamin List, Director at the Max‐Planck‐Institut für Kohlenforschung in Germany, was awarded the Nobel Prize together with David W. C. MacMillan (Princeton University, USA) for the development of asymmetric organocatalysis. After studying chemistry at the Free University of Berlin, he received his doctorate from Goethe University in Frankfurt. He discovered the amino acid proline to be an efficient catalyst and thus co‐founded the field of organocatalysis. In 2016, he received the Gottfried Wilhelm Leibniz Prize, which is considered the most important research award in Germany.
Young chemists play an important role in the transformation of the chemical sector in the next couple of years. They will have to do the heavy lifting and find the solutions needed for a sustainable tomorrow. Therefore, it is important to give them a voice in what their expectations are, how they believe they should be educated and prepared, and what opportunities they see for implementation levels in different areas to promote sustainable development. To shed light on these often under-represented opinions, young chemists across the globe were asked to express their views on the role and responsibilities of the chemical sector anonymously. The result is a snapshot of how young chemists perceive the future of chemistry and the immediate actions that need to be taken to get there. Throughout all answers, their hopes are expressed that the chemical sector will realize its great role and responsibility in leading and promoting sustainable development, thus limiting global warming, through cooperation with authorities, other sectors, and civil society. In this regard, young chemists do have numerous specific ideas about appropriate measures and are eager to take part in shaping a sustainable future.
A MnIII spin crossover complex with atypical two‐step hysteretic thermal switching at 74 K and 84 K shows rich structural–magnetic interplay and magnetic‐field‐induced spin state switching below 14 T with an onset below 5 T. The spin states, structures, and the nature of the phase transitions are elucidated via X‐ray and magnetization measurements. An unusual intermediate phase containing four individual sites, where 1/4 are in a pure low spin state, is observed. The splitting of equivalent sites in the high temperature phase into four inequivalent sites is due to a structural reorganization involving a primary and a secondary symmetry‐breaking order parameter that induces a crystal system change from orthorhombic→monoclinic and a cell doubling. Further cooling leads to a reconstructive phase transition and a monoclinic low‐temperature phase with two inequivalent low‐spin sites. The coupling between the order parameters is identified in the framework of Landau theory.
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