Frozen non-equilibrium dynamics of exciton Mott insulators in moiré superlattices
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Controlling Coulomb correlations and fine structure of quasi-one-dimensional excitons by magnetic order
Many surprising properties of quantum materials result from Coulomb correlations defining electronic quasiparticles and their interaction chains. In van der Waals layered crystals, enhanced correlations have been tailored in reduced dimensions, enabling excitons with giant binding energies and emergent phases including ferroelectric, ferromagnetic and multiferroic orders. Yet, correlation design has primarily relied on structural engineering. Here we present quantitative experiment–theory proof that excitonic correlations can be switched through magnetic order. By probing internal Rydberg-like transitions of excitons in the magnetic semiconductor CrSBr, we reveal their binding energy and a dramatic anisotropy of their quasi-one-dimensional orbitals manifesting in strong fine-structure splitting. We switch the internal structure from strongly bound, monolayer-localized states to weakly bound, interlayer-delocalized states by pushing the system from antiferromagnetic to paramagnetic phases. Our analysis connects this transition to the exciton’s spin-controlled effective quantum confinement, supported by the exciton’s dynamics. In future applications, excitons or even condensates may be interfaced with spintronics; extrinsically switchable Coulomb correlations could shape phase transitions on demand.
Shaping exciton polarization dynamics in 2D semiconductors by tailored ultrafast pulses
The ultrafast formation of strongly bound excitons in two-dimensional semiconductors provides a rich platform for studying fundamental physics as well as developing novel optoelectronic technologies. While extensive research has explored the excitonic coherence, many-body interactions, and nonlinear optical properties, the potential to study these phenomena by directly controlling their coherent polarization dynamics has not been fully realized. In this work, we use a sub-10 fs pulse shaper to study how temporal control of coherent exciton polarization affects the generation of four-wave mixing in monolayer ({rm{WS}}{{rm{e}}}_{2}) under ambient conditions. By tailoring multiphoton pathway interference, we tune the nonlinear response from destructive to constructive interference, resulting in a 2.6-fold enhancement over the four-wave mixing generated by a transform-limited pulse. This demonstrates a general method for nonlinear enhancement by shaping the pulse to counteract the temporal dispersion experienced during resonant light–matter interactions. Our method allows us to excite both 1s and 2s states, showcasing a selective control over the resonant state that produces nonlinearity. By comparing our results with theory, we find that exciton-exciton interactions dominate the nonlinear response, rather than Pauli blocking. This capability to manipulate exciton polarization dynamics in atomically thin crystals lays the groundwork for exploring a wide range of resonant phenomena in condensed matter systems and opens up new possibilities for precise optical control in advanced optoelectronic devices.
Ultrafast exciton-phonon coupling and energy transfer dynamics in quasi-2D layered Ruddlesden-Popper perovskites
Understanding the performance of perovskite solar cells is critical for advancing sustainable energy solutions. Hot-drop casted quasi-2D Ruddlesden-Popper perovskites (RPPs) exhibit remarkable efficiency and stability, making them promising for commercial applications. However, the ultrafast energy transfer and exciton-phonon interactions in these materials remain unclear. Here, we show that using advanced techniques like two-dimensional electronic spectroscopy (2DES) and transient grating (TG), we can unravel energy dynamics in hot-drop casted RPP films. Our study reveals rapid energy transfer between perovskite layers occurring within 100–220 femtoseconds and highlights how exciton-phonon coupling drives structural changes in the material. Coherent vibrational signals identify key lattice and organic cation modes, providing insights into their role in energy dissipation. These findings deepen our understanding of how 2D perovskites work and pave the way for improving the efficiency and stability of next-generation optoelectronic devices.
Non-replicative herpes simplex virus genomic and amplicon vectors for gene therapy – an update
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