Here we demonstrate a more effective use of III–V photoconversion material to achieve an ultrahigh power-per-weight ratio from a solar cell utilizing an axial p-i-n junction GaAs/AlGaAs nanowire (NW) array grown by molecular beam epitaxy on a Si substrate. By analyzing single NW multicontact devices, we first show that an n-GaAs shell is self-formed radially outside the axial p- and i-core of the GaAs NW during n-core growth, which significantly deteriorates the rectification property of the NWs in the axial direction. When employing a selective-area ex situ etching process for the n-GaAs shell, a clear rectification of the axial NW p-i-n junction with a high on/off ratio was revealed. Such a controlled etching process of the self-formed n-GaAs shell was further introduced to fabricate axial p-i-n junction GaAs NW array solar cells. Employing this method, a GaAs NW array solar cell with only ∼1.3% areal coverage of the NWs shows a photoconversion efficiency of ∼7.7% under 1 Sun intensity (AM 1.5G), which is the highest achieved efficiency from any single junction GaAs NW solar cell grown on a Si substrate so far. This corresponds to a power-per-weight ratio of the active III–V photoconversion material as high as 560 W/g, showing great promise for high-efficiency and low-cost III–V NW solar cells and III–V NW/Si tandem solar cells.
Catalysts are central to accelerating chemistry in biology and technology. In biochemistry, the relationship between the velocity of an enzymatic reaction and the concentration of chemical substrates is described via the Michaelis-Menten model. The modeling and benchmarking of synthetic molecular electrocatalysts are also well developed. However, such efforts have not been as rigorously extended to photoelectrosynthetic reactions, where, in addition to chemical substrates and charge carriers, light is a required reagent. In this perspective, we draw parallels between concepts involving enzyme catalytic efficiency, the benchmarking of molecular electrocatalysts, and the performance of photoelectrosynthetic assemblies, while highlighting key differences, assumptions, and limitations.
One of the recently established paradigms in condensed matter physics is examining a system’s behaviour in artificial potentials, giving insight into phenomena of quantum fluids in hard-to-reach settings. A prominent example is the matter-wave scatterer lattice, where high energy matter waves undergo transmission and reflection through narrow width barriers leading to stringent phase matching conditions with lattice band formation. In contrast to evanescently coupled lattice sites, the realisation of a scatterer lattice for macroscopic matter-wave fluids has remained elusive. Here, we implement a system of exciton-polariton condensates in a non-Hermitian Lieb lattice of scatterer potentials. By fine tuning the lattice parameters, we reveal a nonequilibrium phase transition between distinct regimes of polariton condensation: a scatterer lattice of gain guided polaritons condensing on the lattice potential maxima, and trapped polaritons condensing in the potential minima. Our results pave the way towards unexplored physics of non-Hermitian fluids in non-stationary mixtures of confined and freely expanding waves.
In contrast to light, matter-wave optics of quantum gases deals with interactions even in free space and for ensembles comprising millions of atoms. We exploit these interactions in a quantum degenerate gas as an adjustable lens for coherent atom optics. By combining an interaction-driven quadrupole-mode excitation of a Bose-Einstein condensate (BEC) with a magnetic lens, we form a time-domain matter-wave lens system. The focus is tuned by the strength of the lensing potential and the oscillatory phase of the quadrupole mode. By placing the focus at infinity, we lower the total internal kinetic energy of a BEC comprising 101(37) thousand atoms in three dimensions to 3/2 kB·38−7+6 pK. Our method paves the way for free-fall experiments lasting ten or more seconds as envisioned for tests of fundamental physics and high-precision BEC interferometry, as well as opens up a new kinetic energy regime.
Nature controls the assembly of complex architectures through self-limiting processes; however, few artificial strategies to mimic these processes have been reported to date. Here we demonstrate a system comprising two types of nanocrystal (NC), where the self-limiting assembly of one NC component controls the aggregation of the other. Our strategy uses semiconducting InP/ZnS core–shell NCs (3 nm) as effective assembly modulators and functional nanoparticle surfactants in cucurbit[n]uril-triggered aggregation of AuNCs (5–60 nm), allowing the rapid formation (within seconds) of colloidally stable hybrid aggregates. The resultant assemblies efficiently harvest light within the semiconductor substructures, inducing out-of-equilibrium electron transfer processes, which can now be simultaneously monitored through the incorporated surface-enhanced Raman spectroscopy–active plasmonic compartments. Spatial confinement of electron mediators (for example, methyl viologen (MV2+)) within the hybrids enables the direct observation of photogenerated radical species as well as molecular recognition in real time, providing experimental evidence for the formation of elusive σ–(MV+)2 dimeric species. This approach paves the way for widespread use of analogous hybrids for the long-term real-time tracking of interfacial charge transfer processes, such as the light-driven generation of radicals and catalysis with operando spectroscopies under irreversible conditions.
Einstein's theory of general relativity states that clocks at different
gravitational potentials tick at different rates - an effect known as the
gravitational redshift. As fundamental probes of space and time, atomic clocks
have long served to test this prediction at distance scales from 30 centimeters
to thousands of kilometers. Ultimately, clocks will study the union of general
relativity and quantum mechanics once they become sensitive to the finite
wavefunction of quantum objects oscillating in curved spacetime. Towards this
regime, we measure a linear frequency gradient consistent with the
gravitational redshift within a single millimeter scale sample of ultracold
strontium. Our result is enabled by improving the fractional frequency
measurement uncertainty by more than a factor of 10, now reaching 7.6×10−21. This heralds a new regime of clock operation necessitating
intra-sample corrections for gravitational perturbations.
The interplay between strong electron–electron interactions and band topology can produce electronic states that spontaneously break symmetries. The discovery of flat bands in magic-angle twisted bilayer graphene (MATBG)1–3 with non-trivial topology4–7 has provided a compelling platform in which to search for new symmetry-broken phases. Recent scanning tunnelling microscopy8,9 and transport experiments10–13 have revealed a sequence of topological insulating phases in MATBG near integer filling of the electronic bands produced by the moiré pattern. These correspond to a simple pattern of flavour-symmetry-breaking Chern insulators that fill bands of different flavours one after the other. Here we report the high-resolution local compressibility measurements of MATBG with a scanning single-electron transistor, which reveal an additional sequence of incompressible states with unexpected Chern numbers observed down to zero magnetic field. We find that the Chern numbers for eight of the observed incompressible states are incompatible with the simple picture in which the bands are sequentially filled. We show that the emergence of these unusual incompressible phases can be understood as a consequence of broken translation symmetry that doubles the moiré unit cell and splits each flavour band in two. Our findings expand the known phase diagram of MATBG, and shed light on the origin of the close competition between different correlated phases in the system.
Strong light–matter coupling provides a promising path for the control of quantum matter where the latter is routinely described from first principles. However, combining the quantized nature of light with this ab initio tool set is challenging and merely developing as the coupled light–matter Hilbert space is conceptually different and computational cost quickly becomes overwhelming. In this work, we provide a nonperturbative photon-free formulation of quantum electrodynamics (QED) in the long-wavelength limit, which is formulated solely on the matter Hilbert space and can serve as an accurate starting point for such ab initio methods. The present formulation is an extension of quantum mechanics that recovers the exact results of QED for the zero- and infinite-coupling limit and the infinite-frequency as well as the homogeneous limit, and we can constructively increase its accuracy. We show how this formulation can be used to devise approximations for quantum-electrodynamical density-functional theory (QEDFT), which in turn also allows us to extend the ansatz to the full minimal-coupling problem and to nonadiabatic situations. Finally, we provide a simple local density–type functional that takes the strong coupling to the transverse photon degrees of freedom into account and includes the correct frequency and polarization dependence. This QEDFT functional accounts for the quantized nature of light while remaining computationally simple enough to allow its application to a large range of systems. All approximations allow the seamless application to periodic systems.
Voltage control of magnetic order is desirable for spintronic device applications, but 180° magnetization switching is not straightforward because electric fields do not break time-reversal symmetry. Ferrimagnets are promising candidates for 180° switching owing to a multi-sublattice configuration with opposing magnetic moments of different magnitudes. In this study we used solid-state hydrogen gating to control the ferrimagnetic order in rare earth–transition metal thin films dynamically. Electric field-induced hydrogen loading/unloading in GdCo can shift the magnetic compensation temperature by more than 100 K, which enables control of the dominant magnetic sublattice. X-ray magnetic circular dichroism measurements and ab initio calculations indicate that the magnetization control originates from the weakening of antiferromagnetic exchange coupling that reduces the magnetization of Gd more than that of Co upon hydrogenation. We observed reversible, gate voltage-induced net magnetization switching and full 180° Néel vector reversal in the absence of external magnetic fields. Furthermore, we generated ferrimagnetic spin textures, such as chiral domain walls and skyrmions, in racetrack devices through hydrogen gating. With gating times as short as 50 μs and endurance of more than 10,000 cycles, our method provides a powerful means to tune ferrimagnetic spin textures and dynamics, with broad applicability in the rapidly emerging field of ferrimagnetic spintronics.
Subwavelength electromagnetic field localization has been central to photonic research in the last decade, allowing us to enhance sensing capabilities as well as increase the coupling between photons and material excitations. The strong and ultrastrong light–matter coupling regime in the terahertz range using split-ring resonators coupled to magnetoplasmons has been widely investigated, achieving successive world records for the largest light–matter coupling ever achieved. Ever shrinking resonators have allowed us to approach the regime of few-electron strong coupling, in which single-dipole properties can be modified by the vacuum field. Here, we demonstrate, theoretically and experimentally, the existence of a limit to the possibility of arbitrarily increasing electromagnetic confinement in polaritonic systems. Strongly subwavelength fields can excite a continuum of high-momenta propagative magnetoplasmons. This leads to peculiar nonlocal polaritonic effects, as certain polaritonic features disappear and the system enters the regime of discrete-to-continuum strong coupling.