GPAW: An open Python package for electronic structure calculations.

We review the GPAW open-source Python package for electronic structure calculations. GPAW is based on the projector-augmented wave method and can solve the self-consistent density functional theory (DFT) equations using three different wave-function representations, namely real-space grids, plane waves, and numerical atomic orbitals. The three representations are complementary and mutually independent and can be connected by transformations via the real-space grid. This multi-basis feature renders GPAW highly versatile and unique among similar codes. By virtue of its modular structure, the GPAW code constitutes an ideal platform for the implementation of new features and methodologies. Moreover, it is well integrated with the Atomic Simulation Environment (ASE), providing a flexible and dynamic user interface. In addition to ground-state DFT calculations, GPAW supports many-body GW band structures, optical excitations from the Bethe-Salpeter Equation, variational calculations of excited states in molecules and solids via direct optimization, and real-time propagation of the Kohn-Sham equations within time-dependent DFT. A range of more advanced methods to describe magnetic excitations and non-collinear magnetism in solids are also now available. In addition, GPAW can calculate non-linear optical tensors of solids, charged crystal point defects, and much more. Recently, support for graphics processing unit (GPU) acceleration has been achieved with minor modifications to the GPAW code thanks to the CuPy library. We end the review with an outlook, describing some future plans for GPAW.

High-throughput computational stacking reveals emergent properties in natural van der Waals bilayers.

Stacking of two-dimensional (2D) materials has emerged as a facile strategy for realising exotic quantum states of matter and engineering electronic properties. Yet, developments beyond the proof-of-principle level are impeded by the vast size of the configuration space defined by layer combinations and stacking orders. Here we employ a density functional theory (DFT) workflow to calculate interlayer binding energies of 8451 homobilayers created by stacking 1052 different monolayers in various configurations. Analysis of the stacking orders in 247 experimentally known van der Waals crystals is used to validate the workflow and determine the criteria for realisable bilayers. For the 2586 most stable bilayer systems, we calculate a range of electronic, magnetic, and vibrational properties, and explore general trends and anomalies. We identify an abundance of bistable bilayers with stacking order-dependent magnetic or electrical polarisation states making them candidates for slidetronics applications.

Indirect Band Gap Semiconductors for Thin-Film Photovoltaics: High-Throughput Calculation of Phonon-Assisted Absorption.

Discovery of high-performance materials remains one of the most active areas in photovoltaics (PV) research. Indirect band gap materials form the largest part of the semiconductor chemical space, but predicting their suitability for PV applications from first-principles calculations remains challenging. Here, we propose a computationally efficient method to account for phonon-assisted absorption across the indirect band gap and use it to screen 127 experimentally known binary semiconductors for their potential as thin-film PV absorbers. Using screening descriptors for absorption, carrier transport, and nonradiative recombination, we identify 28 potential candidate materials. The list, which contains 20 indirect band gap semiconductors, comprises well-established (3), emerging (16), and previously unexplored (9) absorber materials. Most of the new compounds are anion-rich chalcogenides (TiS3 and Ga2Te5) and phosphides (PdP2, CdP4, MgP4, and BaP3) containing homoelemental bonds and represent a new frontier in PV materials research. Our work highlights the previously underexplored potential of indirect band gap materials for optoelectronic thin-film technologies.

Electrical tuning of optically active interlayer excitons in bilayer MoS2.

Interlayer (IL) excitons, comprising electrons and holes residing in different layers of van der Waals bonded two-dimensional semiconductors, have opened new opportunities for room-temperature excitonic devices. So far, two-dimensional IL excitons have been realized in heterobilayers with type-II band alignment. However, the small oscillator strength of the resulting IL excitons and difficulties with producing heterostructures with definite crystal orientation over large areas have challenged the practical applicability of this design. Here, following the theoretical prediction and recent experimental confirmation of the existence of IL excitons in bilayer MoS2, we demonstrate the electrical control of such excitons up to room temperature. We find that the IL excitonic states preserve their large oscillator strength as their energies are manipulated by the electric field. We attribute this effect to the mixing of the pure IL excitons with intralayer excitons localized in a single layer. By applying an electric field perpendicular to the bilayer MoS2 crystal plane, excitons with IL character split into two peaks with an X-shaped field dependence as a clear fingerprint of the shift of the monolayer bands with respect to each other. Finally, we demonstrate the full control of the energies of IL excitons distributed homogeneously over a large area of our device.

Two-Dimensional Materials with Giant Optical Nonlinearities near the Theoretical Upper Limit.

Nonlinear optical (NLO) phenomena such as harmonic generation and Kerr and Pockels effects are of great technological importance for lasers, frequency converters, modulators, switches, etc. Recently, two-dimensional (2D) materials have drawn significant attention due to their strong and peculiar NLO properties. Here, we describe an efficient first-principles workflow for calculating the quadratic optical response and apply it to 375 non-centrosymmetric semiconductor monolayers from the Computational 2D Materials Database (C2DB). Sorting the nonresonant nonlinearities with respect to bandgap Eg reveals an upper limit proportional to Eg-4, which is neatly explained by two distinct generic models. We identify multiple promising candidates with giant nonlinearities and bandgaps ranging from 0.4 to 5 eV, some of which approach the theoretical upper limit and greatly outperform known materials. Our comprehensive library of ab initio NLO spectra for all 375 monolayers is freely available via the C2DB Web site.

A library of ab initio Raman spectra for automated identification of 2D materials.

Raman spectroscopy is frequently used to identify composition, structure and layer thickness of 2D materials. Here, we describe an efficient first-principles workflow for calculating resonant first-order Raman spectra of solids within third-order perturbation theory employing a localized atomic orbital basis set. The method is used to obtain the Raman spectra of 733 different monolayers selected from the Computational 2D Materials Database (C2DB). We benchmark the computational scheme against available experimental data for 15 known monolayers. Furthermore, we propose an automatic procedure for identifying a material based on an input experimental Raman spectrum and apply it to the cases of MoS2 (H-phase) and WTe2 (T[Formula: see text]-phase). The Raman spectra of all materials at different excitation frequencies and polarization configurations are freely available from the C2DB. Our comprehensive and easily accessible library of ab initio Raman spectra should be valuable for both theoreticians and experimentalists in the field of 2D materials.

Plasmons in ultra-thin gold slabs with quantum spill-out: Fourier modal method, perturbative approach, and analytical model.

We numerically study the effect of the quantum spill-out (QSO) on the plasmon mode indices of an ultra-thin metallic slab, using the Fourier modal method (FMM). To improve the convergence of the FMM results, a novel nonlinear coordinate transformation is suggested and employed. Furthermore, we present a perturbative approach for incorporating the effects of QSO on the plasmon mode indices, which agrees very well with the full numerical results. The perturbative approach also provides additional physical insight, and is used to derive analytical expressions for the mode indices using a simple model for the dielectric function. The analytical expressions reproduce the results obtained from the numerically-challenging spill-out problem with much less effort and may be used for understanding the effects of QSO on other plasmonic structures.

Control of exceptional points in photonic crystal slabs.

Various ways of controlling the extent of the ring of exceptional points in photonic crystal slabs are investigated. The extent of the ring in photonic crystal slabs is found to vary with the thickness of the slab. This enables recovery of Dirac cones in open, non-Hermitian systems, such as a photonic crystal slab. In this case, all three bands exhibit a bound state in the continuum in close proximity of the Γ point. These results may lead to new designs of small photonic-crystal-based lasers exhibiting high-quality factors.

Dynamical dispersion engineering in coupled vertical cavities employing a high-contrast grating.

Photon's effective mass is an important parameter of an optical cavity mode, which determines the strength of light-matter interaction. Here, we propose a novel method for controlling the photon's effective mass by using coupled photonic cavities and designing the angular dependence of the coupling strength. This can be implemented by employing a high-contrast grating (HCG) as the coupling reflector in a system of two coupled vertical cavities, and engineering both the HCG reflection phase and amplitude response. Several examples of HCG-based coupled cavities with novel features are discussed, including a case capable of dynamically controlling the photon's effective mass to a large extent while keeping the resonance frequency same. We believe that full-control and dynamical-tuning of the photon's effective mass may enable new possibilities for cavity quantum electrodynamics studies or conventional/polariton laser applications. For instance, one can dynamically control the condensate formation in polariton lasers by modifying the polariton mass.

Hybrid III-V/SOI resonant cavity enhanced photodetector.

A hybrid III-V/SOI resonant-cavity-enhanced photodetector (RCE-PD) structure comprising a high-contrast grating (HCG) reflector, a hybrid grating (HG) reflector, and an air cavity between them, has been proposed and investigated. In the proposed structure, a light absorbing material is integrated as part of the HG reflector, enabling a very compact vertical cavity. Numerical investigations show that a quantum efficiency close to 100 % and a detection linewidth of about 1 nm can be achieved, which are desirable for wavelength division multiplexing applications. Based on these results, a hybrid RCE-PD sample has been fabricated by heterogeneously integrating an InP-based material onto a silicon-on-insulator wafer and has been characterized, which shows a clear enhancement in photo-current at the designed wavelength. This indicates that the HG reflector provides a field enhancement sufficient for RCE-PD operation. In addition, a capability of feasibly selecting the detection wavelength during fabrication as well as a possibility of realizing silicon-integrated bidirectional transceivers are discussed.

Ultracompact resonator with high quality-factor based on a hybrid grating structure.

We numerically investigate the properties of a hybrid grating structure acting as a resonator with ultrahigh quality factor. This reveals that the physical mechanism responsible for the resonance is quite different from the conventional guided mode resonance (GMR). The hybrid grating consists of a subwavelength grating layer and an un-patterned high-refractive-index cap layer, being surrounded by low index materials. Since the cap layer may include a gain region, an ultracompact laser can be realized based on the hybrid grating resonator, featuring many advantages over high-contrast-grating resonator lasers. The effect of fabrication errors and finite size of the structure is investigated to understand the feasibility of fabricating the proposed resonator.

Hybrid grating reflector with high reflectivity and broad bandwidth.

We suggest a new type of grating reflector denoted hybrid grating (HG) which shows large reflectivity in a broad wavelength range and has a structure suitable for realizing a vertical cavity laser with ultra-small modal volume. The properties of the grating reflector are investigated numerically and explained. The HG consists of an un-patterned III-V layer and a Si grating. The III-V layer has a thickness comparable to the grating layer, introduces more guided mode resonances and significantly increases the bandwidth of the reflector compared to the well-known high-index-contrast grating (HCG). By using an active III-V layer, a laser can be realized where the gain region is integrated into the mirror itself.

Becker's nevus with ipsilateral breast hypoplasia: a case report and review of literature.

Specific cutaneous associations in patients with Becker's nevus have been reported. We present a patient with typical clinical and histopathological features clearly consistent with Becker's nevus associated with ipsilateral breast hypoplasia. The changes were distinct and could be separated from smooth muscle hamartoma. We include clinical and histological illustrations of our case.