Collective Charge Excitations between Moiré Minibands in Twisted WSe_{2} Bilayers Probed with Resonant Inelastic Light Scattering.

We establish low-temperature resonant inelastic light scattering (RILS) spectroscopy as a tool to probe the formation of a series of moiré bands in twisted WSe_{2} bilayers by accessing collective inter-moiré-band excitations (IMBEs). We observe resonances in RILS spectra at energies in agreement with inter-moiré-band transitions obtained from an ab initio based continuum model. Transitions between the first and second moiré band for a twist angle of about 8° are reported and between the first and the third, and higher bands for a twist of about 3°.

Direct synthesis of controllable ultrathin heteroatoms-intercalated 2D layered materials.

Two-dimensional (2D) layered materials have been studied in depth during the past two decades due to their unique structure and properties. Transition metal (TM) intercalation of layered materials have been proven as an effective way to introduce new physical properties, such as tunable 2D magnetism, but the direct growth of atomically thin heteroatoms-intercalated layered materials remains untapped. Herein, we directly synthesize various ultrathin heteroatoms-intercalated 2D layered materials (UHI-2DMs) through flux-assisted growth (FAG) approach.

Giant chiral magnetoelectric oscillations in a van der Waals multiferroic.

Helical spin structures are expressions of magnetically induced chirality, entangling the dipolar and magnetic orders in materials. The recent discovery of helical van der Waals multiferroics down to the ultrathin limit raises prospects of large chiral magnetoelectric correlations in two dimensions. However, the exact nature and magnitude of these couplings have remained unknown so far.

Real-time dynamics of angular momentum transfer from spin to acoustic chiral phonon in oxide heterostructures.

Chiral phonons have recently been explored as a novel degree of freedom in quantum materials. The angular momentum carried by these quasiparticles is generated by the breaking of chiral degeneracy of phonons, owing to the chiral lattice structure or the rotational motion of ions of the material. In ferromagnets, a mechanism for generating non-equilibrium chiral phonons has been suggested, but their temporal evolution, which obeys Bose-Einstein statistics, remains unclear.

Magnetic field expulsion in optically driven YBaCuO.

Coherent optical driving in quantum solids is emerging as a research frontier, with many reports of interesting non-equilibrium quantum phases and transient photo-induced functional phenomena such as ferroelectricity, magnetism and superconductivity. In high-temperature cuprate superconductors, coherent driving of certain phonon modes has resulted in a transient state with superconducting-like optical properties, observed far above their transition temperature T and throughout the pseudogap phase. However, questions remain on the microscopic nature of this transient state and how to distinguish it from a non-superconducting state with enhanced carrier mobility.

Benchmarking Functionals for Strong-Field Light-Matter Interactions in Adiabatic Time-Dependent Density Functional Theory.

In recent years, time-dependent density functional theory (TDDFT) has been extensively employed for highly nonlinear optics in molecules and solids, including high harmonic generation (HHG), photoemission, and more. TDDFT exhibits a relatively low numerical cost while still describing both light-matter and electron-electron interactions ab initio, making it highly appealing. However, the majority of implementations of the theory utilize the simplest possible approximations for the exchange-correlation (XC) functional-either the local density or generalized gradient approximations, which are traditionally considered to have rather poor chemical accuracy.

A size-consistent multi-state mapping approach to surface hopping.

We develop a multi-state generalization of the recently proposed mapping approach to surface hopping (MASH) for the simulation of electronically nonadiabatic dynamics. This new approach extends the original MASH method to be able to treat systems with more than two electronic states. It differs from previous approaches in that it is size consistent and rigorously recovers the original two-state MASH in the appropriate limits.

Hidden Charge Order and Multiple Electronic Instabilities in EuTe.

The rare-earth telluride compound EuTe exhibits a charge density wave (CDW) and an unconventional thermal hysteresis transition. Herein, we report a comprehensive study of the CDW states in EuTe by using low-temperature scanning tunneling microscopy. Two types of charge orders are observed at 4 K, including a newly discovered spindle-shaped pattern and a typical stripe-like pattern.

An antiferromagnetic spin phase change memory.

The electrical outputs of single-layer antiferromagnetic memory devices relying on the anisotropic magnetoresistance effect are typically rather small at room temperature. Here we report a new type of antiferromagnetic memory based on the spin phase change in a Mn-Ir binary intermetallic thin film at a composition within the phase boundary between its collinear and noncollinear phases. Via a small piezoelectric strain, the spin structure of this composition-boundary metal is reversibly interconverted, leading to a large nonvolatile room-temperature resistance modulation that is two orders of magnitude greater than the anisotropic magnetoresistance effect for a metal, mimicking the well-established phase change memory from a quantum spin degree of freedom.

Power Density Titration of Reversible Photoisomerization of a Fluorescent Protein Chromophore in the Presence of Thermally Driven Barrier Crossing Shown by Quantitative Millisecond Serial Synchrotron X-ray Crystallography.

We present millisecond quantitative serial X-ray crystallography at 1.7 Å resolution demonstrating precise optical control of reversible population transfer from Trans-Cis and Cis-Trans photoisomerization of a reversibly switchable fluorescent protein, rsKiiro. Quantitative results from the analysis of electron density differences, extrapolated structure factors, and occupancy refinements are shown to correspond to optical measurements of photoinduced population transfer and have sensitivity to a few percent in concentration differences.

Direct observation of photoinduced sequential spin transition in a halogen-bonded hybrid system by complementary ultrafast optical and electron probes.

A detailed understanding of the ultrafast dynamics of halogen-bonded materials is desired for designing supramolecular materials and tuning various electronic properties by external stimuli. Here, a prototypical halogen-bonded multifunctional material containing spin crossover (SCO) cations and paramagnetic radical anions is studied as a model system of photo-switchable SCO hybrid systems using ultrafast electron diffraction and two complementary optical spectroscopic techniques. Our results reveal a sequential dynamics from SCO to radical dimer softening, uncovering a key transient intermediate state.

Modeling the electroluminescence of atomic wires from quantum dynamics simulations.

Static and time-dependent quantum-mechanical approaches have been employed in the literature to characterize the physics of light-emitting molecules and nanostructures. However, the electromagnetic emission induced by an input current has remained beyond the realm of molecular simulations. This is the challenge addressed here with the help of an equation of motion for the density matrix coupled to a photon bath based on a Redfield formulation.

Chirality-Dependent Dynamic Evolution for Trions in Monolayer WS.

Monolayer transition metal dichalcogenides exhibit valley-dependent excitonic characters with a large binding energy, acting as the building block for future optoelectronic functionalities. Herein, combined with pump-probe ultrafast transient transmission spectroscopy and theoretical simulations, we reveal the chirality-dependent trion dynamics in h-BN encapsulated monolayer tungsten disulfide. By resonantly pumping trions in a single valley and monitoring their temporal evolution, we identify the temperature-dependent competition between two relaxation channels driven by chirality-dependent scattering processes.

Quantum Quality with Classical Cost: Nonadiabatic Dynamics Simulations Using the Mapping Approach to Surface Hopping.

Nonadiabatic dynamics methods are an essential tool for investigating photochemical processes. In the context of employing first-principles electronic structure techniques, such simulations can be carried out in a practical manner using semiclassical trajectory-based methods or wave packet approaches. While all approaches applicable to first-principles simulations are necessarily approximate, it is commonly thought that wave packet approaches offer inherent advantages over their semiclassical counterparts in terms of accuracy and that this trait simply comes at a higher computational cost.

Ultrafast Carrier Relaxation Dynamics in a Nodal-Line Semimetal PtSn.

Topological Dirac nodal-line semimetals host topologically nontrivial electronic structure with nodal-line crossings around the Fermi level, which could affect the photocarrier dynamics and lead to novel relaxation mechanisms. Herein, by using time- and angle-resolved photoemission spectroscopy, we reveal the previously inaccessible linear dispersions of the bulk conduction bands above the Fermi level in a Dirac nodal-line semimetal PtSn, as well as the momentum and temporal evolution of the gapless nodal lines. A surprisingly ultrafast relaxation dynamics within a few hundred femtoseconds is revealed for photoexcited carriers in the nodal line.

A MASH simulation of the photoexcited dynamics of cyclobutanone.

In response to a community prediction challenge, we simulate the nonadiabatic dynamics of cyclobutanone using the mapping approach to surface hopping (MASH). We consider the first 500 fs of relaxation following photoexcitation to the S2 state and predict the corresponding time-resolved electron-diffraction signal that will be measured by the planned experiment. 397 ab initio trajectories were obtained on the fly with state-averaged complete active space self-consistent field using a (12,11) active space.

Unraveling a Cavity-Induced Molecular Polarization Mechanism from Collective Vibrational Strong Coupling.

We demonstrate that collective vibrational strong coupling of molecules in thermal equilibrium can give rise to significant local electronic polarizations in the thermodynamic limit. We do so by first showing that the full nonrelativistic Pauli-Fierz problem of an ensemble of strongly coupled molecules in the dilute-gas limit reduces in the cavity Born-Oppenheimer approximation to a cavity-Hartree equation for the electronic structure. Consequently, each individual molecule experiences a self-consistent coupling to the dipoles of all other molecules, which amount to non-negligible values in the thermodynamic limit (large ensembles).

Chemical passivation of 2D transition metal dichalcogenides: strategies, mechanisms, and prospects for optoelectronic applications.

The interest in obtaining high-quality monolayer transition metal dichalcogenides (TMDs) for optoelectronic device applications has been growing dramatically. However, the prevalence of defects and unwanted doping in these materials remain challenges, as they both limit optical properties and device performance. Surface chemical treatments of monolayer TMDs have been effective in improving their photoluminescence yield and charge transport properties.

Photonic time-crystalline behaviour mediated by phonon squeezing in TaNiSe.

Photonic time crystals refer to materials whose dielectric properties are periodic in time, analogous to a photonic crystal whose dielectric properties is periodic in space. Here, we theoretically investigate photonic time-crystalline behaviour initiated by optical excitation above the electronic gap of the excitonic insulator candidate TaNiSe. We show that after electron photoexcitation, electron-phonon coupling leads to an unconventional squeezed phonon state, characterised by periodic oscillations of phonon fluctuations.

Correlated order at the tipping point in the kagome metal CsVSb.

Spontaneously broken symmetries are at the heart of many phenomena of quantum matter and physics more generally. However, determining the exact symmetries that are broken can be challenging due to imperfections such as strain, in particular when multiple electronic orders are competing. This is exemplified by charge order in some kagome systems, where evidence of nematicity and flux order from orbital currents remains inconclusive due to contradictory measurements.

Exploring the Mechanisms behind Non-aromatic Fluorescence with the Density Functional Tight Binding Method.

Recent experimental findings reveal nonconventional fluorescence emission in biological systems devoid of conjugated bonds or aromatic compounds, termed (NAF). This phenomenon is exclusive to aggregated or solid states and remains absent in monomeric solutions. Previous studies focused on small model systems in vacuum show that the carbonyl stretching mode along with strong interaction of short hydrogen bonds (SHBs) remains the primary vibrational mode explaining NAF in these systems.

Two-photon absorption cross sections of pulsed entangled beams.

Entangled two-photon absorption (ETPA) could form the basis of nonlinear quantum spectroscopy at very low photon fluxes, since, at sufficiently low photon fluxes, ETPA scales linearly with the photon flux. When different pairs start to overlap temporally, accidental coincidences are thought to give rise to a "classical" quadratic scaling that dominates the signal at large photon fluxes and, thus, recovers a supposedly classical regime, where any quantum advantage is thought to be lost. Here, we scrutinize this assumption and demonstrate that quantum-enhanced absorption cross sections can persist even for very large photon numbers.

Terminable Transitions in a Topological Fermionic Ladder.

Interacting fermionic ladders are versatile platforms to study quantum phases of matter, such as different types of Mott insulators. In particular, there are D-Mott and S-Mott states that hold preformed fermion pairs and become paired-fermion liquids upon doping (d wave and s wave, respectively). We show that the D-Mott and S-Mott phases are in fact two facets of the same topological phase and that the transition between them is terminable.