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The coupling of excitons with atomic vibrations plays a pivotal role on the nonequilibrium optical properties of layered semiconductors. However, how exciton-phonon coupling manifests in the time and energy domains is still an open debate between experiment and theory. By means of time-resolved broadband optical reflectivity combined with ab initio calculations of a bismuth tri-iodide single crystal, we set the spectral fingerprints for the optical detection of exciton-phonon coupling in layered semiconductors. Our joint experimental and theoretical effort allows us to unravel the impact of exciton-phonon coupling by microscopically relating the photoinduced coherent energy modulation of the excitonic resonance to coherent optical phonons. This enables us to track the extent of the photoinduced atomic displacement in real space. Our findings represent a step forward on the road to coherent manipulation of the excitonic properties on ultrafast timescales.

Avalanche resistive switching is the fundamental process that triggers the sudden change of the electrical properties in solid-state devices under the action of intense electric fields. Despite its relevance for information processing, ultrafast electronics, neuromorphic devices, resistive memories and brain-inspired computation, the nature of the local stochastic fluctuations that drive the formation of metallic regions within the insulating state has remained hidden. Here, using operando X-ray nano-imaging, we have captured the origin of resistive switching in a V 2 O 3 -based device under working conditions. V 2 O 3 is a paradigmatic Mott material, which undergoes a first-order metal-to-insulator phase transition together with a lattice transformation that breaks the threefold rotational symmetry of the rhombohedral metallic phase. We reveal a new class of volatile electronic switching triggered by nanoscale topological defects appearing in the shear-strain based order parameter that describes the insulating phase. Our results pave the way to the use of strain engineering approaches to manipulate such topological defects and achieve the full dynamical control of the electronic Mott switching. Topology-driven, reversible electronic transitions are relevant across a broad range of quantum materials, comprising transition metal oxides, chalcogenides and kagome metals., (© 2024. The Author(s).)

Understanding the nature of the photoexcitation and ultrafast charge dynamics pathways in organic halide perovskite nanocubes and their aggregation into superlattices is key for potential applications as tunable light emitters, photon-harvesting materials, and light-amplification systems. In this work, we apply two-dimensional coherent electronic spectroscopy (2DES) to track in real time the formation of near-infrared optical excitons and their ultrafast relaxation in CH(NH 2 ) 2 PbI 3 nanocube superlattices. Our results unveil that the coherent ultrafast dynamics is limited by the combination of the inherent short exciton decay time (≃40 fs) and the dephasing due to the coupling with selective optical phonon modes at higher temperatures. On the picosecond time scale, we observe the progressive formation of long-lived localized trap states. The analysis of the temperature dependence of the excitonic intrinsic line width, as extracted by the antidiagonal components of the 2D spectra, unveils a dramatic change of the excitonic coherence time across the cubic to tetragonal structural transition. Our results offer a new way to control and enhance the ultrafast coherent dynamics of photocarrier generation in hybrid halide perovskite synthetic solids., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Published by American Chemical Society.)

Understanding the thermoelastic response of a nanostructure is crucial for the choice of materials and interfaces in electronic devices with improved and tailored transport properties at the nanoscale. Here, we show how the deposition of a MoS 2 monolayer can strongly modify the nanoscale thermoelastic dynamics of silicon substrates close to their interface. We demonstrate this by creating a transient grating with extreme ultraviolet light, using ultrashort free-electron laser pulses, whose ≈84 nm period is comparable to the size of elements typically used in nanodevices, such as electric contacts and nanowires. The thermoelastic response, featuring coherent acoustic waves and incoherent relaxation, is tangibly modified by the presence of monolayer MoS 2 . Namely, we observed a major reduction of the amplitude of the surface mode, which is almost suppressed, while the longitudinal mode is basically unperturbed, aside from a faster decay of the acoustic modulations. We interpret this behavior as a selective modification of the surface elasticity, and we discuss the conditions to observe such effect, which may be of immediate relevance for the design of Si-based nanoscale devices., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Published by American Chemical Society.)

The development of quantum simulators, artificial platforms where the predictions of many-body theories of correlated quantum materials can be tested in a controllable and tunable way, is one of the main challenges of condensed matter physics. Here we introduce artificial lattices made of lead halide perovskite nanocubes as a new platform to simulate and investigate the physics of correlated quantum materials. We demonstrate that optical injection of quantum confined excitons in this system realizes the two main features that ubiquitously pervade the phase diagram of many quantum materials: collective phenomena, in which long-range orders emerge from incoherent fluctuations, and the excitonic Mott transition, which has one-to-one correspondence with the insulator-to-metal transition described by the repulsive Hubbard model in a magnetic field. Our results demonstrate that time-resolved experiments provide a quantum simulator that is able to span a parameter range relevant for a broad class of phenomena, such as superconductivity and charge-density waves.

In solids, the response of the lattice to photoexcitation is often described by the inertial evolution on an impulsively modified potential energy surface which leads to coherent motion. However, it remains unknown if vibrational coherence is sustained through a phase transition, during which coupling between modes can be strong and may lead to rapid loss of coherence. Here we use coherent phonon spectroscopy to track lattice coherence in the structural phase transition of V_{2}O_{3}. In both the low and high symmetry phases unique coherent phonon modes are generated at low fluence. However, coherence is lost when driving between the low and high symmetry phases. Our results suggest strongly damped noninertial dynamics dominate during the phase transition due to disorder and multimode coupling.

Mott transitions in real materials are first order and almost always associated with lattice distortions, both features promoting the emergence of nanotextured phases. This nanoscale self-organization creates spatially inhomogeneous regions, which can host and protect transient non-thermal electronic and lattice states triggered by light excitation. Here, we combine time-resolved X-ray microscopy with a Landau-Ginzburg functional approach for calculating the strain and electronic real-space configurations. We investigate V 2 O 3 , the archetypal Mott insulator in which nanoscale self-organization already exists in the low-temperature monoclinic phase and strongly affects the transition towards the high-temperature corundum metallic phase. Our joint experimental-theoretical approach uncovers a remarkable out-of-equilibrium phenomenon: the photo-induced stabilisation of the long sought monoclinic metal phase, which is absent at equilibrium and in homogeneous materials, but emerges as a metastable state solely when light excitation is combined with the underlying nanotexture of the monoclinic lattice., (© 2022. The Author(s).)

Superconductivity and charge density waves (CDWs) are competitive, yet coexisting, orders in cuprate superconductors. To understand their microscopic interdependence, a probe capable of discerning their interaction on its natural length and time scale is necessary. We use ultrafast resonant soft x-ray scattering to track the transient evolution of CDW correlations in YBa 2 Cu 3 O 6+ x after the quench of superconductivity by an infrared laser pulse. We observe a nonthermal response of the CDW order characterized by a near doubling of the correlation length within ≈1 picosecond of the superconducting quench. Our results are consistent with a model in which the interaction between superconductivity and CDWs manifests inhomogeneously through disruption of spatial coherence, with superconductivity playing the dominant role in stabilizing CDW topological defects, such as discommensurations.