Visualizing superexchange interactions: The resolution that can be achieved in scanning probe microscopy can be greatly enhanced by absorbing a molecule such as CO on the probe tip. Czap et al. now show that this approach can be used to scan spin and magnetic properties of molecules on a surface. They adsorbed a magnetic molecule, Ni(cyclopentadienyl) ₂ , on a silver surface and then transferred one of these molecules to a scanning tunnel microscope tip. They could then bring the tip toward the adsorbate-covered surface and map out the strength of superexchange interactions. Science , this issue p. 670

Spatially resolved vibrational mapping of nanostructures is indispensable to the development and understanding of thermal nanodevices¹, modulation of thermal transport² and novel nanostructured thermoelectric materials^3–5. Through the engineering of complex structures, such as alloys, nanostructures and superlattice interfaces, one can significantly alter the propagation of phonons and suppress material thermal conductivity while maintaining electrical conductivity². There have been no correlative experiments that spatially track the modulation of phonon properties in and around nanostructures due to spatial resolution limitations of conventional optical phonon detection techniques. Here we demonstrate two-dimensional spatial mapping of phonons in a single silicon–germanium (SiGe) quantum dot (QD) using monochromated electron energy loss spectroscopy in the transmission electron microscope. Tracking the variation of the Si optical mode in and around the QD, we observe the nanoscale modification of the composition-induced red shift. We observe non-equilibrium phonons that only exist near the interface and, furthermore, develop a novel technique to differentially map phonon momenta, providing direct evidence that the interplay between diffuse and specular reflection largely depends on the detailed atomistic structure: a major advancement in the field. Our work unveils the non-equilibrium phonon dynamics at nanoscale interfaces and can be used to study actual nanodevices and aid in the understanding of heat dissipation near nanoscale hotspots, which is crucial for future high-performance nanoelectronics.

Oxide solid electrolytes (OSEs) have the potential to achieve improved safety and energy density for lithium-ion batteries, but their high grain-boundary (GB) resistance generally is a bottleneck. In the well-studied perovskite oxide solid electrolyte, Li_3xLa_2/3-xTiO₃(LLTO), the ionic conductivity of grain boundaries is about three orders of magnitude lower than that of the bulk. In contrast, the related Li_0.375Sr_0.4375Ta_0.75Zr_0.25O₃(LSTZ0.75) perovskite exhibits low grain boundary resistance for reasons yet unknown. Here, we use aberration-corrected scanning transmission electron microscopy and spectroscopy, along with an active learning moment tensor potential, to reveal the atomic scale structure and composition of LSTZ0.75 grain boundaries. Vibrational electron energy loss spectroscopy is applied for the first time to reveal atomically resolved vibrations at grain boundaries of LSTZ0.75 and to characterize the otherwise unmeasurable Li distribution therein. We find that Li depletion, which is a major reason for the low grain boundary ionic conductivity of LLTO, is absent for the grain boundaries of LSTZ0.75. Instead, the low grain boundary resistivity of LSTZ0.75 is attributed to the formation of a nanoscale defective cubic perovskite interfacial structure that contained abundant vacancies. Our study provides new insights into the atomic scale mechanisms of low grain boundary resistivity.

We report single-molecule conformational transitions with joint angstrom-femtosecond resolution by irradiating the junction of a scanning tunneling microscope with femtosecond laser pulses. An isolated pyrrolidine molecule adsorbed on a Cu(001) surface undergoes reversible transitions between two conformational states. The transition rate decays in time and exhibits sinusoidal oscillations with periods of specific molecular vibrations. The dynamics of this transition depends sensitively on the molecular environment, as exemplified by the effects of another molecule in proximity.

Realization of the quantum spin Hall effect in graphene devices has remained an outstanding challenge dating back to the inception of the field of topological insulators. Graphene’s exceptionally weak spin-orbit coupling—stemming from carbon’s low mass—poses the primary obstacle. We experimentally and theoretically study artificially enhanced spin-orbit coupling in graphene via random decoration with dilute Bi₂Te₃ nanoparticles. Multiterminal resistance measurements suggest the presence of helical edge states characteristic of a quantum spin Hall phase; the magnetic field and temperature dependence of the resistance peaks, x-ray photoelectron spectra, scanning tunneling spectroscopy, and first-principles calculations further support this scenario. These observations highlight a pathway to spintronics and quantum information applications in graphene-based quantum spin Hall platforms.