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Quasiparticles consisting of correlated electron(s) and hole(s), such as excitons and trions, play important roles in the optical phenomena of van der Waals semiconductors and serve as unique platforms for studies of many-body physics. Herein, we report a gate-tunable exciton-to-trion transition in pressurized monolayer MoSe2, in which the electronic band structures are modulated continuously within a diamond anvil cell. The emission energies of both the exciton and trion undergo large blueshifts over 90 meV with increasing pressure. Surprisingly, the trion binding energy remains constant at 30 meV, regardless of the applied pressure. Combining ab initiodensity functional theory calculations and quantum Monte Carlo simulations, we find that the remarkable robustness of the trion binding energy originates from the spatially diffused nature of the trion wave function and the weak correlation between its constituent electron–hole pairs. Our findings shed light on the optical properties of correlated excitonic quasiparticles in low-dimensional materials.

Laser-induced ultrafast demagnetization is a phenomenon of utmost interest and attracts significant attention because it enables potential applications in ultrafast optoelectronics and spintronics. As a spin–orbit coupling assisted magnetic insulator, α-RuCl3provides an attractive platform to explore the physics of electronic correlations and unconventional magnetism. Using time-dependent density functional theory, we explore the ultrafast laser-induced dynamics of the electronic and magnetic structures in α-RuCl3. Our study unveils that laser pulses can introduce ultrafast demagnetizations, accompanied by an out-of-equilibrium insulator-to-metal transition in a few tens of femtoseconds. The spin response significantly depends on the laser wavelength and polarization on account of the electron correlations, band renormalizations, and charge redistributions. These findings provide physical insights into the coupling between the electronic and magnetic degrees of freedom in α-RuCl3and shed light on suppressing the long-range magnetic orders and reaching a proximate spin liquid phase for two-dimensional magnets on an ultrafast time scale.

We investigate heterostructures composed of monolayer WSe2stacked on α-RuCl3using a combination of Terahertz (THz) and infrared (IR) nanospectroscopy and imaging, scanning tunneling spectroscopy (STS), and photoluminescence (PL). Our observations reveal itinerant carriers in the heterostructure prompted by charge transfer across the WSe2/α-RuCl3interface. Local STS measurements show the Fermi level is shifted to the valence band edge of WSe2which is consistent with p-type doping and verified by density functional theory (DFT) calculations. We observe prominent resonances in near-IR nano-optical and PL spectra, which are associated with the A-exciton of WSe2. We identify a concomitant, near total, quenching of the A-exciton resonance in the WSe2/α-RuCl3heterostructure. Our nano-optical measurements show that the charge-transfer doping vanishes while excitonic resonances exhibit near-total recovery in “nanobubbles”, where WSe2and α-RuCl3are separated by nanometer distances. Our broadband nanoinfrared inquiry elucidates local electrodynamics of excitons and an electron–hole plasma in the WSe2/α-RuCl3system.

Bioorthogonal metallocatalysis has opened up a xenobiotic route to perform nonenzymatic catalytic transformations in living settings. Despite their promising features, most metals are deactivated inside cells by a myriad of reactive biomolecules, including biogenic thiols, thereby limiting the catalytic functioning of these abiotic reagents. Here we report the development of cytocompatible alloyed AuPdnanoparticles with the capacity to elicit bioorthogonal depropargylations with high efficiency in biological media. We also show that the intracellular catalytic performance of these nanoalloys is significantly enhanced by protecting them following two different encapsulation methods. Encapsulation in mesoporous silica nanorods resulted in augmented catalyst reactivity, whereas the use of a biodegradable PLGA matrix increased nanoalloy delivery across the cell membrane. The functional potential of encapsulated AuPdwas demonstrated by releasing the potent chemotherapy drug paclitaxel inside cancer cells. Nanoalloy encapsulation provides a novel methodology to develop nanoreactors capable of mediating new-to-life reactions in cells.

Organic thermoelectric materials have potential for wearable heating, cooling, and energy generation devices at room temperature. For this to be technologically viable, high-conductance (G) and high-Seebeck-coefficient (S) materials are needed. For most semiconductors, the increase in Sis accompanied by a decrease in G. Here, using a combined experimental and theoretical investigation, we demonstrate that a simultaneous enhancement of Sand Gcan be achieved in single organic radical molecules, thanks to their intrinsic spin state. A counterintuitive quantum interference (QI) effect is also observed in stable Blatter radical molecules, where constructive QI occurs for a meta-connected radical, leading to further enhancement of thermoelectric properties. Compared to an analogous closed-shell molecule, the power factor is enhanced by more than 1 order of magnitude in radicals. These results open a new avenue for the development of organic thermoelectric materials operating at room temperature.

Twisting two adjacent layers of van der Waals materials with respect to each other can lead to flat two-dimensional electronic bands which enables a wealth of physical phenomena. Here, we generalize this concept of so-called moiré flat bands to engineer flat bands in all three spatial dimensions controlled by the twist angle. The basic concept is to stack the material such that the large spatial moiré interference patterns are spatially shifted from one twisted layer to the next. We exemplify the general concept by considering graphitic systems, boron nitride, and WSe2, but the approach is applicable to any two-dimensional van der Waals material. For hexagonal boron nitride, we develop an ab initiofitted tight binding model that captures the corresponding three-dimensional low-energy electronic structure. We outline that interesting three-dimensional correlated phases of matter can be induced and controlled following this route, including quantum magnets and unconventional superconducting states.

Cell membranes regulate the distribution of biological machinery between phase-separated lipid domains to facilitate key processes including signaling and transport, which are among the life-like functionalities that bottom-up synthetic biology aims to replicate in artificial-cellular systems. Here, we introduce a modular approach to program partitioning of amphiphilic DNA nanostructures in coexisting lipid domains. Exploiting the tendency of different hydrophobic “anchors” to enrich different phases, we modulate the lateral distribution of our devices by rationally combining hydrophobes and by changing nanostructure size and topology. We demonstrate the functionality of our strategy with a bioinspired DNA architecture, which dynamically undergoes ligand-induced reconfiguration to mediate cargo transport between domains via lateral redistribution. Our findings pave the way to next-generation biomimetic platforms for sensing, transduction, and communication in synthetic cellular systems.

Two-dimensional materials, obtained by van der Waals stacking of layers, are fascinating objects of contemporary condensed matter research, exhibiting a variety of new physics. Inspired by the breakthroughs of twisted bilayer graphene (TBG), we demonstrate that twisted bilayer boron nitride (TBBN) is an even more exciting novel system that turns out to be an excellent platform to realize new correlated phases and phenomena; exploration of its electronic properties shows that in contrast to TBG in TBBN multiple families of 2,4, and 6-fold degenerate flat bands emerge without the need to fine tune close to a “magic angle”, resulting in dramatic and tunable changes in optical properties and exciton physics, and providing an additional platform to study strong correlations. Upon doping, unforeseen new correlated phases of matter (insulating and superconducting) emerge. TBBN could thus provide a promising experimental platform, insensitive to small deviations in the twist angle, to study novel exciton condensate and spatial confinement physics, and correlations in two dimensions.

Bulk and single-layer 2H-NbSe2exhibit identical charge density wave order (CDW) with a quasi-commensurate 3 × 3 superlattice periodicity. Here we combine scanning tunnelling microscopy (STM) imaging at T= 1 K of 2H-NbSe2with first-principles density functional theory (DFT) calculations to investigate the structural atomic rearrangement of this CDW phase. Our calculations for single-layers reveal that six different atomic structures are compatible with the 3 × 3 CDW distortion, although all of them lie on a very narrow energy range of at most 3 meV per formula unit, suggesting the coexistence of such structures. Our atomically resolved STM images of bulk 2H-NbSe2unambiguously confirm this by identifying two of these structures. Remarkably, these structures differ from the X-ray crystal structure reported for the bulk 3 × 3 CDW which in fact is also one of the six DFT structures located for the single-layer. Our calculations also show that due to the minute energy difference between the different phases, the ground state of the 3 × 3 CDW could be extremely sensitive to doping, external strain or internal pressure within the crystal. The presence of multiphase CDW order in 2H-NbSe2may provide further understanding of its low temperature state and the competition between different instabilities.

The way nuclear motion affects electronic responses has become a very hot topic in materials science. Coherent acoustic phonons can dynamically modify optical, magnetic, and mechanical properties at ultrasonic frequencies, with promising applications as sensors and transducers. Here, by means of ultrafast broadband deep-ultraviolet spectroscopy, we demonstrate that coherent acoustic phonons confined in anatase TiO2nanoparticles can selectively modulate the oscillator strength of the two-dimensional bound excitons supported by the material. We use many-body perturbation-theory calculations to reveal that the deformation potential is the mechanism behind the generation of the observed coherent acoustic wavepackets. Our results offer a route to manipulate and dynamically tune the properties of excitons in the deep-ultraviolet at room temperature.

The ability to create nanometer-scale lateral p–n junctions is essential for the next generation of two-dimensional (2D) devices. Using the charge-transfer heterostructure graphene/α-RuCl3, we realize nanoscale lateral p–n junctions in the vicinity of graphene nanobubbles. Our multipronged experimental approach incorporates scanning tunneling microscopy (STM) and spectroscopy (STS) and scattering-type scanning near-field optical microscopy (s-SNOM) to simultaneously probe the electronic and optical responses of nanobubble p–n junctions. Our STM/STS results reveal that p–n junctions with a band offset of ∼0.6 eV can be achieved with widths of ∼3 nm, giving rise to electric fields of order 108V/m. Concurrent s-SNOM measurements validate a point-scatterer formalism for modeling the interaction of surface plasmon polaritons (SPPs) with nanobubbles. Ab initiodensity functional theory (DFT) calculations corroborate our experimental data and reveal the dependence of charge transfer on layer separation. Our study provides experimental and conceptual foundations for generating p–n nanojunctions in 2D materials.

The rate of electron transfer at carbon electrodes depends on various factors such as the structure and morphology of the carbon material used in the electrodes. With the advent of new carbon structures, such as fullerenes and carbon nanotubes, well-defined carbon surfaces have become available to probe electron-transfer kinetics on these surfaces. We show here that micron-size electrodes made of multiwalled carbon nanotubes show Nernstien behavior and fast electron-transfer kinetics for electrochemical reactions of Fe(CN)6^3-/4-. This is achieved without any pretreatments for the electrodes, suggesting the possibility of developing superior carbon electrodes based on carbon nanotubes, for electrochemical applications.

Floquet theory has spawned many exciting possibilities for electronic structure control with light, with enormous potential for future applications. The experimental demonstration in solids, however, remains largely unrealized. In particular, the influence of scattering on the formation of Floquet–Bloch states remains poorly understood. Here we combine time- and angle-resolved photoemission spectroscopy with time-dependent density functional theory and a two-level model with relaxation to investigate the survival of Floquet–Bloch states in the presence of scattering. We find that Floquet–Bloch states will be destroyed if scattering—activated by electronic excitations—prevents the Bloch electrons from following the driving field coherently. The two-level model also shows that Floquet–Bloch states reappear at high field intensities where energy exchange with the driving field dominates over energy dissipation to the bath. Our results clearly indicate the importance of long scattering times combined with strong driving fields for the successful realization of various Floquet phenomena.