${\text{LiCu}}_3{\mathrm{O}}_3$ is an antiferromagnetic mixed valence cuprate where trilayers of edge-sharing Cu(II)O ($3d^9$) are sandwiched in between planes of Cu(I) ($3d^{10}$) ions, with Li stochastically substituting Cu(II). Angle-resolved photoemission spectroscopy (ARPES) and density functional theory reveal two insulating electronic subsystems that are segregated in spite of sharing common oxygen atoms: a Cu $d_{z^2}/\mathrm{O}$ $p_z$ derived valence band (VB) dispersing on the Cu(I) plane, and a Cu $3d_{x^2-y^2}/\mathrm{O}$ $2p_{x,y}$ derived Zhang-Rice singlet (ZRS) band dispersing on the Cu(II)O planes. First-principle analysis shows the Li substitution to stabilize the insulating ground state, but only if antiferromagnetic correlations are present. Li further induces substitutional disorder and a 2D electron glass behavior in charge transport, reflected in a large 530 meV Coulomb gap and a linear suppression of VB spectral weight at $E_F$ that is observed by ARPES. Surprisingly, the disorder leaves the Cu(II)-derived ZRS largely unaffected. This indicates a local segregation of Li and Cu atoms onto the two separate corner-sharing $\mathrm{Cu}(\mathrm{II}){\mathrm{O}}_2$ sub-lattices of the edge-sharing Cu(II)O planes, and highlights the ubiquitous resilience of the entangled two hole ZRS entity against impurity scattering.

Beyond 14 GPa of pressure, bilayered ${\mathrm{La}}_3{\mathrm{Ni}}_2{\mathrm{O}}_7$ was recently found to develop strong superconductivity above the liquid nitrogen boiling temperature. An immediate essential question is the pressure-induced qualitative change of electronic structure that enables the exciting high-temperature superconductivity. We investigate this timely question via a numerical multiscale derivation of effective many-body physics. At the atomic scale, we first clarify that the system has a strong charge transfer nature with itinerant carriers residing mainly in the in-plane oxygen between spin-1 ${\mathrm{Ni}}^{2+}$ ions. We then elucidate in electron-volt scale and sub-electron-volt scale the key physical effect of the applied pressure: it induces a cupratelike electronic structure via fractionalizing the Ni ionic spin from 1 to $1/2$. This suggests a high-temperature superconductivity in ${\mathrm{La}}_3{\mathrm{Ni}}_2{\mathrm{O}}_7$ with microscopic mechanism and ($d$-wave) symmetry similar to that in the cuprates.

Despite appealing high-symmetry properties that enable strong spatial confinement and ultrahigh-$Q$, optical whispering-gallery modes of spherical and circular resonators have been absent from the field of quantum-well exciton polaritons. Here we observe whispering-gallery exciton polaritons in a gallium arsenide microdisk cavity filled with indium gallium arsenide quantum wells, the test bed materials of polaritonics. Strong coupling is evidenced in photoluminescence and resonant spectroscopy accessed through concomitant confocal microscopy and near-field optical techniques. Excitonic and optical resonances are tuned by varying temperature and disk radius, revealing Rabi splittings between 5 and 10 meV. A dedicated analytical quantum model for such circular whispering-gallery polaritons is developed, which reproduces the measured values. At high power, lasing is observed and accompanied by a blueshift of the emission consistent with the regime of polariton lasing. With experimental methods and theory now established, whispering-gallery-mode polaritons in round dielectric resonators appear as a new viable platform toward low loss polaritonics.

Nonradiative exciton relaxation processes are critical for energy transduction and transport in optoelectronic materials, but how these processes are connected to the underlying crystal structure and the associated electron, exciton, and phonon band structures, as well as the interactions of all these particles, is challenging to understand. Here, we present a first-principles study of exciton-phonon relaxation pathways in pentacene, a paradigmatic molecular crystal and optoelectronic semiconductor. We compute the momentum- and band-resolved exciton-phonon interactions, and use them to analyze key scattering channels. We find that both exciton intraband scattering and interband scattering to parity-forbidden dark states occur on the same $\sim 100\mathrm{fs}$ timescale as a direct consequence of the longitudinal-transverse splitting of the bright exciton band. Consequently, exciton-phonon scattering exists as a dominant nonradiative relaxation channel in pentacene. We further show how the propagation of an exciton wave packet is connected with crystal anisotropy, which gives rise to the longitudinal-transverse exciton splitting and concomitant anisotropic exciton and phonon dispersions. Our results provide a framework for understanding the role of exciton-phonon interactions in exciton nonradiative lifetimes in molecular crystals and beyond.

Very recently, a fundamental observable has been introduced and analyzed to quantify the exploration of random walks: the time ${\tau }_k$ required for a random walk to find a site that it never visited previously, when the walk has already visited $k$ distinct sites. Here, we tackle the natural issue of the statistics of $M_n$, the longest duration out of ${\tau }_0,\dots ,{\tau }_{n-1}$. This problem belongs to the active field of extreme value statistics, with the difficulty that the random variables ${\tau }_k$ are both correlated and nonidentically distributed. Beyond this fundamental aspect, we show that the asymptotic determination of the statistics of $M_n$ finds explicit applications in foraging theory and allows us to solve the open $d$-dimensional starving random walk problem, in which each site of a lattice initially contains one food unit, consumed upon visit by the random walker, which can travel $\mathcal{S}$ steps without food before starving. Processes of diverse nature, including regular diffusion, anomalous diffusion, and diffusion in disordered media and fractals, share common properties within the same universality classes.

We report the measurement of the helicity asymmetry $E$ for the $p{\pi }^0$ and $n{\pi }^{+}$ final states using, for the first time, an elliptically polarized photon beam in combination with a longitudinally polarized target at the Crystal Ball experiment at MAMI. The results agree very well with data that were taken with a circularly polarized photon beam, showing that it is possible to simultaneously measure polarization observables that require linearly (e.g., $G$) and circularly polarized photons (e.g., $E$) and a longitudinally polarized target. The new data cover a photon energy range 270–1400 MeV for the $p{\pi }^0$ final state (230–842 MeV for the $n{\pi }^{+}$ final state) and the full range of pion polar angles, $\theta$, providing the most precise measurement of the observable $E$. A moment analysis gives a clear observation of the $p\eta$ cusp in the $p{\pi }^0$ final state.

Coulomb explosion imaging (CEI) with x-ray free electron lasers has recently been shown to be a powerful method for obtaining detailed structural information of gas-phase planar ring molecules [R. Boll et al., X-ray multiphoton-induced Coulomb explosion images complex single molecules, Nat. Phys. 18, 423 (2022).]. In this Letter, we investigate the potential of CEI driven by a tabletop laser and extend this approach to differentiating three-dimensional structures. We study the static CEI patterns of planar and nonplanar organic molecules that resemble the structures of typical products formed in ring-opening reactions. Our results reveal that each molecule exhibits a well-localized and distinctive pattern in three-dimensional fragment-ion momentum space. We find that these patterns yield direct information about the molecular structures and can be qualitatively reproduced using a classical Coulomb explosion simulation. Our findings suggest that laser-induced CEI can serve as a robust method for differentiating molecular structures of organic ring and chain molecules. As such, it holds great promise as a method for following ultrafast structural changes, e.g., during ring-opening reactions, by tracking the motion of individual atoms in pump-probe experiments.

Although topological phenomena attract growing interest not only in linear systems but also in nonlinear systems, the bulk-edge correspondence under the nonlinearity of eigenvalues has not been established so far. We address this issue by introducing auxiliary eigenvalues. We reveal that the topological edge states of auxiliary eigenstates are topologically inherited as physical edge states when the nonlinearity is weak but finite (i.e., auxiliary eigenvalues are monotonic as for the physical one). This result leads to the bulk-edge correspondence with the nonlinearity of eigenvalues.

The competition between on-site electronic correlation and local crystal field stands out as a captivating topic in research. However, its physical ramifications often get overshadowed by influences of strong periodic potential and orbital hybridization. The present study reveals this competition may become more pronounced or even dominant in two-dimensional systems, driven by the combined effects of dimensional confinement and orbital anisotropy. This leads to electronic orbital reconstruction in certain perovskite superlattices or thin films. To explore the emerging physics, we investigate the interfacial orbital disorder-order transition with an effective Hamiltonian and how to modulate this transition through strains.

A droplet depositing on a solid substrate leads to the wetting phenomenon, such as dew on plant leaves. On an ideally smooth substrate, the classic Young’s law has been employed to describe the wetting effect. However, no real substrate is ideally smooth at the microscale. Given this fact, we introduce a surface composition concept to scrutinize the wetting mechanism via considering the liquid-gas density asymmetry and the fluid-solid van der Waals interaction. The current concept enables one to comprehend counterintuitive phenomenon of contact-angle hysteresis on a smooth substrate and increase of contact angle with temperature as well as gas bubble wetting.

The computer simulation of many molecular processes is complicated by long timescales caused by rare transitions between long-lived states. Here, we propose a new approach to simulate such rare events, which combines transition path sampling with enhanced exploration of configuration space. The method relies on exchange moves between configuration and trajectory space, carried out based on a generalized ensemble. This scheme substantially enhances the efficiency of the transition path sampling simulations, particularly for systems with multiple transition channels, and yields information on thermodynamics, kinetics and reaction coordinates of molecular processes without distorting their dynamics. The method is illustrated using the isomerization of proline in the KPTP tetrapeptide.

Single molecule junctions are important examples of complex out-of-equilibrium many-body quantum systems. We identify a nontrivial clustering of steady state populations into distinctive subspaces with Boltzmann-like statistics, which persist far from equilibrium. Such Boltzmann subspaces significantly reduce the information needed to describe the steady state, enabling modeling of high-dimensional systems that are otherwise beyond the reach of current computations. The emergence of Boltzmann subspaces is demonstrated analytically and numerically for fermionic transport systems of increasing complexity.

Certain non-Hermitian systems exhibit the skin effect, whereby the wave functions become exponentially localized at one edge of the system. Such exponential amplification of wavefunction has received significant attention due to its potential applications in, e.g., classical and quantum sensing. However, the opposite edge of the system, featured by exponentially suppressed wave functions, remains largely unexplored. Leveraging this phenomenon, we introduce a non-Hermitian cooling mechanism, which is fundamentally distinct from traditional refrigeration or laser cooling techniques. Notably, non-Hermiticity will not amplify thermal excitations, but rather redistribute them. Hence, thermal excitations can be cooled down at one edge of the system, and the cooling effect can be exponentially enhanced by the number of auxiliary modes, albeit with a lower bound that depends on the dissipative interaction with the environment. Non-Hermitian cooling does not rely on intricate properties such as exceptional points or nontrivial topology, and it can apply to a wide range of excitations.

A theory of the measurement-induced entanglement phase transition for free-fermion models in $d>1$ dimensions is developed. The critical point separates a gapless phase with ${\ell }^{d-1}\ln \ell$ scaling of the second cumulant of the particle number and of the entanglement entropy and an area-law phase with ${\ell }^{d-1}$ scaling, where $\ell$ is a size of the subsystem. The problem is mapped onto an $\mathrm{SU}(R)$ replica nonlinear sigma model in $d+1$ dimensions, with $R\to 1$. Using renormalization-group analysis, we calculate critical indices in one-loop approximation justified for $d=1+\epsilon$ with $\epsilon \ll 1$. Further, we carry out a numerical study of the transition for a $d=2$ model on a square lattice, determine numerically the critical point, and estimate the critical index of the correlation length, $\nu \approx 1.4$.

Saturated absorption measurements of transitions in the (2-0) band of radioactive tritium hydride are performed with the ultrasensitive noise-immune cavity-enhanced optical-heterodyne molecular spectroscopy intracavity absorption technique in the range 1460–1510 nm. The hyperfine structure of rovibrational transitions of tritium hydride, in contrast to that of hydrogen deuteride, exhibits a single isolated hyperfine component, allowing for the accurate determination of hyperfineless rovibrational transition frequencies, resulting in $\mathrm{R}(0)=203396426692(22)\mathrm{kHz}$ and $\mathrm{R}(1)=205380033644(21)\mathrm{kHz}$. This corresponds to an accuracy 3 orders of magnitude better than previous measurements in tritiated hydrogen molecules. Observation of an isolated component in P(1) with reversed signal amplitude contradicts models for line shapes in hydrogen deuteride based on crossover resonances.