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Renske M. van der Veen

Publications and source records attributed to Renske M. van der Veen.

5 recordsLinked to original sources

Light-Stabilized Metastable Electronic State in NiO with Enhanced Orbital Hybridization

Light-driven control of electronic structure in correlated metal oxides offers new opportunities for optimizing materials used in photovoltaic and photoelectrochemical technologies. We show that photoexcitation of NiO, a prototypical transparent semiconductor and hole-transport material, across its charge-transfer gap produces a long-lived metastable state with enhanced Ni 3d-O 2p orbital hybridization. We characterize this state using Ni K-edge X-ray absorption spectroscopy, which probes how structural and electronic changes affect the unoccupied p density of states during continuous and pulsed ultraviolet excitation. Under pulsed excitation, high carrier densities of approximately 10^20 per cubic centimeter generate a state with a lifetime of approximately 600 picoseconds, in which enhanced hybridization coexists with lattice heating. By contrast, continuous ultraviolet irradiation at much lower carrier densities of approximately 10^13 per cubic centimeter stabilizes a similar electronic state with negligible lattice heating, demonstrating that its formation is not solely thermally driven. First-principles DFT+U+V calculations attribute the spectral changes to stronger Ni 3d-O 2p hybridization, which alters the unoccupied Ni 4p states probed by dipole-allowed K-edge transitions. We attribute this change to the dynamic screening of on-site electronic correlations following photoexcitation, which redistributes the charge density. Because orbital hybridization governs carrier transport and charge-transfer energetics, our results identify photoinduced screening as a mechanism for dynamically tuning correlated oxides and suggest new design principles for optoelectronic materials.

cond-mat.mtrl-sci↗

Ultrafast dynamic Coulomb screening of X-ray core excitons in photoexcited semiconductors

Ultrafast X-ray spectroscopy has been revolutionized in recent years due to the advent of fourth-generation X-ray facilities. In solid-state materials, core excitons determine the energy and line shape of absorption features in core-level spectroscopies such as X-ray absorption spectroscopy. The screening of core excitons is an inherent many-body process that can reveal insight into charge-transfer excitations and electronic correlations. Under non-equilibrium conditions such as after photoexcitation, however, core-exciton screening is still not fully understood. Here we demonstrate the dynamic Coulomb screening of core excitons induced by photoexcited carriers by employing X-ray transient absorption (XTA) spectroscopy with picosecond time resolution. Our interpretation is supported by state-of-the-art ab initio theory, combining constrained and real-time time-dependent density functional theory with many-body perturbation theory. Using ZnO as an archetypal wide band-gap semiconductor, we show that the Coulomb screening by photoexcited carriers at the Zn K-edge leads to a decrease in the core-exciton binding energy, which depends nonlinearly on both the excitation density and the distribution of photoexcited carriers in reciprocal space. The effect of Coulomb screening dominates over Pauli blocking in the XTA spectra. We show that dynamic core-exciton screening is also observed at other X-ray absorption edges and theoretically predict the effect of core-exciton screening on the femtosecond time scale for the case of ZnO, a major step towards hard X-ray excitonics. The results have implications for the interpretation of ultrafast X-ray spectra in general and their use in tracking charge carrier dynamics in complex materials on atomic length scales.

cond-mat.mtrl-sci↗

Diamagnetic/Paramagnetic Phase Transitions in Non-equilibrium Confined Single-Component Plasmas

In this letter, a phase transition of a non-equilibrated single component plasma evolving within a uniform constant magnetic field is demonstrated for the first time. We present classical fluid models that capture this phenomenon, confirm with N -particle simulations, derive constraints on parameters necessary to induce this phase transition, and suggest an experiment to test the novel predictions of the theory.

physics.plasm-ph↗

General Formulation of Coulomb Explosion Dynamics of Highly Symmetric Charge Distributions

We present a theoretical approach to study the dynamics of spherical, cylindrical and ellipsoidal charge distributions under their self-Coulomb field and a stochastic force due to collisions and random motions of charged particles. The approach is based on finding the current density of the charge distribution from the charge-current continuity equation and determining the drift velocities of the particles. The latter can be used either to derive the Lagrangian of the system, or to write Newtons equation of motion with the Lorentz force. We develop a kinetic theory to include the stochastic force due to random motions of electrons into our model. To demonstrate the efficacy of our method, we apply it to various charge distributions and compare our results to N-body simulations. We show that our method reproduces the well-known emittance term in the envelope equation of uniform spherical and cylindrical charge distributions with correct coefficients. We use our model for the gravitational collapse of an ideal gas as well as the cyclotron dynamics of a cylindrical charge distribution in a uniform magnetic field and propose a method to measure the emittance of electron beams.

physics.plasm-ph↗

Ultrafast electron energy-loss spectroscopy in transmission electron microscopy

In the quest for dynamic multimodal probing of a material's structure and functionality, it is critical to be able to quantify the chemical state on the atomic and nanoscale using element specific electronic and structurally sensitive tools such as electron energy loss spectroscopy (EELS). Ultrafast EELF, with combined energy, time, and spatial resolution in a transmission electron microscope, has recently enabled transformative studies of photo excited nanostructure evolution and mapping of evanescent electromagnetic fields. This article aims to describe the state of the art experimental techniques in this emerging field and its major uses and future applications.

physics.app-ph↗