Laser-Driven Transient Phase Oscillations in Individual Spin Crossover Particles.

An unusual expansion dynamics of individual spin crossover nanoparticles is studied by ultrafast transmission electron microscopy. After exposure to nanosecond laser pulses, the particles exhibit considerable length oscillations during and after their expansion. The vibration period of 50-100 ns is of the same order of magnitude as the time that the particles need for a transition from the low-spin to the high-spin state. The observations are explained in Monte Carlo calculations using a model where elastic and thermal coupling between the molecules within a crystalline spin crossover particle govern the phase transition between the two spin states. The experimentally observed length oscillations are in agreement with the calculations, and it is shown that the system undergoes repeated transitions between the two spin states until relaxation in the high-spin state occurs due to energy dissipation. Spin crossover particles are therefore a unique system where a resonant transition between two phases occurs in a phase transformation of first order.

Probing Magnetic Defects in Ultra-Scaled Nanowires with Optically Detected Spin Resonance in Nitrogen-Vacancy Center in Diamond.

Magnetic nanowires (NWs) are essential building blocks of spintronics devices as they offer tunable magnetic properties and anisotropy through their geometry. While the synthesis and compositional control of NWs have seen major improvements, considerable challenges remain for the characterization of local magnetic features at the nanoscale. Here, we demonstrate nonperturbative field distribution mapping in ultrascaled magnetic nanowires with diameters down to 6 nm by scanning nitrogen-vacancy magnetometry. This enables localized, minimally invasive magnetic imaging with sensitivity down to 3 µT Hz-1/2. The imaging reveals the presence of weak magnetic inhomogeneities inside in-plane magnetized nanowires that are largely undetectable with standard metrology and can be related to local fluctuations of the NWs' saturation magnetization. In addition, the strong magnetic field confinement in the nanowires allows for the study of the interaction between the stray magnetic field and the nitrogen-vacancy sensor, thus clarifying the contrasting formation mechanisms for technologically relevant magnetic nanostructures.

Elastically driven cooperative response of a molecular material impacted by a laser pulse.

Photoinduced phase transformations occur when a laser pulse impacts a material, thereby transforming its electronic and/or structural orders, consequently affecting the functionalities. The transient nature of photoinduced states has thus far severely limited the scope of applications. It is of paramount importance to explore whether structural feedback during the solid deformation has the capacity to amplify and stabilize photoinduced transformations. Contrary to coherent optical phonons, which have long been under scrutiny, coherently propagating cell deformations over acoustic timescales have not been explored to a similar degree, particularly with respect to cooperative elastic interactions. Herein we demonstrate, experimentally and theoretically, a self-amplified responsiveness in a spin-crossover material during its delayed volume expansion. The cooperative response at the material scale prevails above a threshold excitation, significantly extending the lifetime of photoinduced states. Such elastically driven cooperativity triggered by a light pulse offers an efficient route towards the generation and stabilization of photoinduced phases in many volume-changing materials.

Photo-Thermal Switching of Individual Plasmonically Activated Spin Crossover Nanoparticle Imaged by Ultrafast Transmission Electron Microscopy.

Spin crossover (SCO) is a promising switching phenomenon when implemented in electronic devices as molecules, thin films or nanoparticles. Among the properties modulated along this phenomenon, optically induced mechanical changes are of tremendous importance as they can work as fast light-induced mechanical switches or allow to investigate and control microstructural strains and fatigability. The development of characterization techniques probing nanoscopic behavior with high spatio-temporal resolution allows to trigger and visualize such mechanical changes of individual nanoscopic objects. Here, ultrafast transmission electron microscopy (UTEM) is used to precisely probe the length changes of individual switchable nanoparticles induced thermally by nanosecond laser pulses. This allows revealing of the mechanisms of spin switching, leading to the macroscopic expansion of SCO materials. This study is conducted on individual pure SCO nanoparticles and SCO nanoparticles encapsulating gold nanorods that serve for plasmonic heating under laser pulses. Length changes are compared with time-resolved optical measurements performed on an assembly of these particles.

Model for elastic relaxation phenomena in finite 2D hexagonal molecular lattices.

The relaxation in a spin transition compound is modeled on the basis of molecules interacting by the way of connecting springs and situated in a bidimensional open boundary hexagonal lattice. The switch of individual molecules is randomly checked using a standard Monte Carlo procedure. The switching probability depends on the energy gap between the two states in the absence of interactions and on the elongations of the nearest springs. The main characteristics of the experimental relaxation curves are reproduced and clustering and nucleation phenomena are detected.