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Semiconductor nanowires have shown great potential for enabling ultra-compact lasers for integrated photonics platforms. Despite the impressive progress in developing nanowire lasers, their integration into Si photonics platforms remains challenging largely due to the use of III-V and II-VI semiconductors as gain media. These materials not only have high material costs, but also require inherently complex integration with Si-based fabrication processing, increasing overall costs and thereby limiting their large-scale adoption. Furthermore, these material-based nanowire lasers rarely emit above 2 um, which is a technologically important wavelength regime for various applications in imaging and quantum sensing. Recently, group-IV nanowires, particularly direct bandgap GeSn nanowires capable of emitting above 2 um, have emerged as promising cost-effective gain media for Si-compatible nanowire lasers, but there has been no successful demonstration of lasing from this seemingly promising nanowire platform. Herein, we report the experimental observation of lasing above 2 um from a single bottom-up grown GeSn nanowire. By harnessing strain engineering and optimized cavity designs simultaneously, the single GeSn nanowire achieves an amplified material gain that can sufficiently overcome minimized optical losses, resulting in a single-mode lasing with an ultra-low threshold of ~5.3 kW cm-2. Our finding paves the way for all-group IV mid-infrared photonic-integrated circuits with compact Si-compatible lasers for on-chip classical and quantum sensing and free-space communication., Comment: 24 pages, 4 figures

The commercially available 4000-Watt continuous-wave Erbium-doped-fiber laser, emitting at the 1567-nanometer wavelength where the atmosphere has high transmission, provides an opportunity for harvesting electric power at remote off the grid locations using a multi-module photovoltaic receiver panel. This paper proposes a 32-element monocrystalline thick-layer Germanium photovoltaic panel for efficient harvesting of a collimated 1.13-meter-diameter beam.The 0.78-meter squared PV panel is constructed from commercial Ge wafers. For incident continuous-wave laser-beam power in the 4000 to 10000 Watt range, our thermal and electrical and infrared simulations predict 660 to 1510 Watts of electrical output at panel temperatures of 350 to 423 Kelvin., Comment: 11 pages, 6 figures

Transferring energy without transferring mass is a powerful paradigm to address the challenges faced when the access to, or the deployment of, the infrastructure for energy conversion is locally impossible or impractical. Laser beaming holds the promise of effectively implementing this paradigm. With this perspective, this work evaluates the optical-to-electrical power conversion that is created when a collimated laser beam illuminates a silicon photovoltaic solar cell that is located kilometers away from the laser. The laser is a CW high-energy Yb-doped fiber laser emitting at a center wavelength of 1075 nm with ~1 m2 of effective beam area. For 20 kW illumination of a solar panel having 0.6 m2 of area, optical simulations and thermal simulations indicate electrical output power of 3000 Watts at a panel temperature of 550 K. Our investigations show that thermo-radiative cells are rather inefficient. In contrast, an optimized approach to harvest laser energy is achieved by using a hybrid module consisting of a photovoltaic cell and a thermo-electric generator. Finally, practical considerations related to infrared power beaming are discussed and its potential applications are outlined., Comment: 14 pages, 11 Figures

The selective confinement of light holes (LHs) in a tensile-strained germanium (Ge) quantum well is studied by mapping the electronic structure of Ge$_{1-x}$Sn$_x$/Ge/Ge$_{1-x}$Sn$_x$ heterostructures as a function of Sn content, residual strain, and Ge well thickness. It is shown that above $12\,\text{at.}\%$ Sn and below $0.4\%$ residual compressive strain in the barriers, the tensile strain in Ge becomes sufficiently large to yield a valence band edge with LH-like character, thus forming a quasi two-dimensional LH gas in Ge. The LH ground state has a larger in-plane effective mass than that of heavy holes (HHs) in Si$_{1-y}$Ge$_y$/Ge/Si$_{1-y}$Ge$_y$ quantum wells. Moreover, LHs in optimal Ge$_{1-x}$Sn$_x$/Ge/Ge$_{1-x}$Sn$_x$ heterostructures are found to exhibit a strong $g$-tensor anisotropy, with the in-plane component one order of magnitude larger than that of HHs in typical planar systems. Two of three structure-inversion-asymmetry Rashba parameters, both of which are critical in electric-dipole-spin-resonance experiments, are effectively 10 times the size of the cubic Rashba parameter in HH quantum wells. In the regime of LH selective confinement, every layer of the heterostructure is of direct bandgap, which can be relevant for efficient optical photon-spin qubit interfaces. This work discusses the broad landscape of the characteristics of LH spin confined in Ge to guide the design and implementation of LH spin-based devices.

Due to their narrow band gap and compatibility with silicon processing, germanium-tin (Ge$_{1-x}$Sn$_x$) alloys are a versatile platform for scalable integrated mid-infrared photonics. These semiconductors are typically grown on silicon wafers using Ge as an interlayer. However, the large lattice mismatch in this heteroepitaxy protocol leads to the build-up of compressive strain in the grown layers. This compressive strain limits the material quality and its thermal stability besides expanding the band gap, thereby increasing the Sn content needed to cover a broader range in the mid-infrared. Released Ge$_{1-x}$Sn$_x$ membranes provide an effective way to mitigate these harmful effects of the epitaxial strain and control the band gap energy while enabling the hybrid integration onto different substrates. With this perspective, herein strain-relaxed Ge$_{0.89}$Sn$_{0.11}$ membranes are fabricated and subsequently transfer-printed with metal contacts to create multiple photodetectors in a single transfer step. The resulting photodetectors exhibit an extended photodetection cutoff reaching a wavelength of $3.1 \,\mu$m, coupled with a significant reduction in the dark current of two orders of magnitude as compared to as-grown photoconductive devices. The latter yields a reduced cutoff of $2.8 \,\mu$m due to the inherent compressive strain. Furthermore, the impact of chemical treatment and annealing on the device performance was also investigated showing a further reduction in the dark current. The demonstrated transfer printing, along with the use of an adhesive layer, would allow the transfer of multiple GeSn membranes onto virtually any substrate. This approach paves the way for scalable fabrication of hybrid optoelectronic devices leveraging the tunable band gap of Ge$_{1-x}$Sn$_x$ in the mid-wave infrared range.

There is an increasing need for silicon-compatible high bandwidth extended-short wave infrared (e-SWIR) photodetectors (PDs) to implement cost-effective and scalable optoelectronic devices. These systems are quintessential to address several technological bottlenecks in detection and ranging, surveillance, ultrafast spectroscopy, and imaging. In fact, current e-SWIR high bandwidth PDs are predominantly made of III-V compound semiconductors and thus are costly and suffer a limited integration on silicon besides a low responsivity at wavelengths exceeding $2.3 \,\mu$m. To circumvent these challenges, Ge$_{1-x}$Sn$_{x}$ semiconductors have been proposed as building blocks for silicon-integrated high-speed e-SWIR devices. Herein, this study demonstrates a vertical all-GeSn PIN PDs consisting of p-Ge$_{0.92}$Sn$_{0.08}$/i-Ge$_{0.91}$Sn$_{0.09}$/n-Ge$_{0.89}$Sn$_{0.11}$ and p-Ge$_{0.91}$Sn$_{0.09}$/i-Ge$_{0.88}$Sn$_{0.12}$/n-Ge$_{0.87}$Sn$_{0.13}$ heterostructures grown on silicon following a step-graded temperature-controlled epitaxy protocol. The performance of these PDs was investigated as a function of the device diameter in the $10-30 \,\mu$m range. The developed PD devices yield a high bandwidth of 12.4 GHz at a bias of 5V for a device diameter of $10 \,\mu$m. Moreover, these devices show a high responsivity of 0.24 A/W, a low noise, and a $2.8 \,\mu$m cutoff wavelength thus covering the whole e-SWIR range.

Cost-effective mid-wave infrared (MWIR) optoelectronic devices are of utmost importance to a plethora of applications such as night vision, thermal sensing, autonomous vehicles, free-space communication, and spectroscopy. To this end, leveraging the ubiquitous silicon-based processing has emerged as a powerful strategy that can be accomplished through the use of group IV germanium-tin (GeSn) alloys. Indeed, due to their compatibility with silicon and their tunable bandgap energy covering the entire MWIR range, GeSn semiconductors are frontrunner platforms for compact and scalable MWIR technologies. However, the GeSn large lattice parameter has been a major hurdle limiting the quality of GeSn epitaxy on silicon wafers. Herein, it is shown that sub-20 nm Ge nanowires (NWs) provide effective compliant substrates to grow Ge$_{1-x}$Sn$_{x}$ alloys with a composition uniformity over several micrometers with a very limited build-up of the compressive strain. Ge/Ge$_{1-x}$Sn$_{x}$ core/shell NWs with Sn content spanning the 6 to 18 at.$\%$ range are demonstrated and integrated in photoconductive devices exhibiting a high signal-to-noise ratio at room temperature and a tunable cutoff wavelength covering the 2.0 $\mu$m to 3.9 $\mu$m range. Additionally, the processed NW-based detectors were used in uncooled imagers enabling the acquisition of high-quality images under both broadband and laser illuminations without a lock-in technique.

Silicon-compatible short- and mid-wave infrared emitters are highly sought-after for on-chip monolithic integration of electronic and photonic circuits to serve a myriad of applications in sensing and communication. To address this longstanding challenge, GeSn semiconductors have been proposed as versatile building blocks for silicon-integrated optoelectronic devices. In this regard, this work demonstrates light-emitting diodes (LEDs) consisting of a vertical PIN double heterostructure p-Ge$_{0.94}$Sn$_{0.06}$/i-Ge$_{0.91}$Sn$_{0.09}$/n-Ge$_{0.95}$Sn$_{0.05}$ grown epitaxially on a silicon wafer using germanium interlayer and multiple GeSn buffer layers. The emission from these GeSn LEDs at variable diameters in the 40-120 $\mu$m range is investigated under both DC and AC operation modes. The fabricated LEDs exhibit a room temperature emission in the extended short-wave range centered around 2.5 $\mu$m under an injected current density as low as 45 A/cm$^2$. By comparing the photoluminescence and electroluminescence signals, it is demonstrated that the LED emission wavelength is not affected by the device fabrication process or heating during the LED operation. Moreover, the measured optical power was found to increase monotonically as the duty cycle increases indicating that the DC operation yields the highest achievable optical power. The LED emission profile and bandwidth are also presented and discussed.

Compound semiconductors have been the predominant building blocks for the current mid-infrared thermophotovoltaic devices relevant to sub-2000 K heat conversion and power beaming. However, the prohibitively high cost associated with these technologies limits their broad adoption. Herein, to alleviate this challenge we introduce an all-group IV mid-infrared cell consisting of GeSn alloy directly on a silicon wafer. This emerging class of semiconductors provides strain and composition as degrees of freedom to control the bandgap energy thus covering the entire mid-infrared range. The proposed thermophotovoltaic device is composed of a fully relaxed Ge$_{0.83}$Sn$_{0.17}$ double heterostructure corresponding to a bandgap energy of 0.29 eV. A theoretical framework is derived to evaluate cell performance under high injection. The black-body radiation absorption is investigated using the generalized transfer matrix method thereby considering the mixed coherent/incoherent layer stacking. Moreover, the intrinsic recombination mechanisms and their importance in a narrow bandgap semiconductor were also taken into account. In this regard, the parabolic band approximation and Fermi's golden rule were combined for an accurate estimation of the radiative recombination rate. Based on these analyses, power conversion efficiencies of up to 9% are predicted for Ge$_{0.83}$Sn$_{0.17}$ thermophotovoltaic cells under black-body radiation at temperatures in the 500-1500 K range. A slight improvement in the efficiency is observed under the frontside illumination but vanishes below 800 K, while the use of a backside reflector improves the efficiency across the investigated black-body temperature range. The effects of the heterostructure thickness, surface recombination velocity, and carrier lifetime are also elucidated and discussed.

CMOS-compatible short- and mid-wave infrared emitters are highly coveted for the monolithic integration of silicon-based photonic and electronic integrated circuits to serve a myriad of applications in sensing and communications. In this regard, a group IV germanium-tin (GeSn) material epitaxially grown on silicon (Si) emerges as a promising platform to implement tunable infrared light emitters. Indeed, upon increasing the Sn content, the bandgap of GeSn narrows and becomes direct, making this material system suitable for developing an efficient silicon-compatible emitter. With this perspective, microbridge PIN GeSn LEDs with a small footprint of $1,520$ $\mu$m$^2$ are demonstrated and their operation performance is investigated. The spectral analysis of the electroluminescence emission exhibits a peak at $2.31$ $\mu$m and it red-shifts slightly as the driving current increases. It is found that the microbridge LED operates at a dissipated power as low as $10.8$ W at room temperature and just $3$ W at $80$ K. This demonstrated low operation power is comparable to that reported for LEDs having a significantly larger footprint reaching $10^6$ $\mu$m$^2$. The efficient thermal dissipation of the current design helped to reduce the heat-induced optical losses, thus enhancing light emission. Further performance improvements are envisioned through thermal and optical simulations of the microbridge design. The use of GeSnOI substrate for developing a similar device is expected to improve optical confinement for the realization of electrically driven GeSn lasers.

Ge$_{1-x}$Sn$_x$ semiconductors hold the premise for large-scale, monolithic mid-infrared photonics and optoelectronics. However, despite the successful demonstration of several Ge$_{1-x}$Sn$_x$-based photodetectors and emitters, key fundamental properties of this material system are yet to be fully explored and understood. In particular, little is known about the role of the material properties in controlling the recombination mechanisms and their consequences on the carrier lifetime. Evaluating the latter is in fact fraught with large uncertainties that are exacerbated by the difficulty to investigate narrow bandgap semiconductors. To alleviate these limitations, herein we demonstrate that the radiative carrier lifetime can be obtained from straightforward excitation power- and temperature- dependent photoluminescence measurements. To this end, a theoretical framework is introduced to simulate the measured spectra by combining the band structure calculations from the k.p theory and the envelope function approximation (EFA) to estimate the absorption and spontaneous emission. Based on this model, the temperature-dependent emission from Ge$_{0.83}$Sn$_{0.17}$ samples at a biaxial compressive strain of $-1.3\%$ was investigated. The simulated spectra reproduce accurately the measured data thereby enabling the evaluation of the steady-state radiative carrier lifetimes, which are found in the 3-22 ns range for temperatures between 10 and 300 K at an excitation power of 0.9 kW/cm$^2$. For a lower power of 0.07 kW/cm$^2$, the obtained lifetime has a value of 1.9 ns at 4 K. The demonstrated approach yielding the radiative lifetime from simple emission spectra will provide valuable inputs to improve the design and modeling of Ge$_{1-x}$Sn$_x$-based devices.

The optical injection of charge and spin currents are investigated in Ge$_{1-x}$Sn$_{x}$ semiconductors as a function of Sn content. These emerging silicon-compatible materials enable the modulation of these processes across the entire mid-infrared range. Under the independent particle approximation, the one- and two-photon interband absorption processes are elucidated, and the evolution of the coherent control is discussed for three different polarization configurations. To evaluate the contribution of high-energy transitions, a full-zone 30-band k$\cdot$p is employed in the calculations. It was found that, besides the anticipated narrowing of the direct gap and the associated shift of the absorption to longer wavelengths, incorporating Sn in Ge also increases the one-photon degree of spin polarization (DSP) at the $E_1$ resonance. Moreover, as the Sn content increases, the magnitude of the response tensors near the band edge exhibits an exponential enhancement. This behavior can be attributed to the Sn incorporation-induced decrease in the carrier effective masses. This trend appears to hold also at the $E_1$ resonance for pure spin current injection, at least at low Sn compositions. The two-photon DSP at the band edge exceeds the value in Ge to reach 60 % at a Sn content above 14 %. These results demonstrate that Ge$_{1-x}$Sn$_{x}$ semiconductors can be exploited to achieve the quantum coherent manipulation in the molecular fingerprint region relevant to quantum sensing., Comment: 8 pages, 9 figures, with a Supporting Material file

The short-wave infrared (SWIR) is an underexploited portion of the electromagnetic spectrum in metasurface-based nanophotonics despite its strategic importance in sensing and imaging applications. This is mainly attributed to the lack of material systems to tailor light-matter interactions in this range. Herein, we address this limitation and demonstrate an all-dielectric silicon-integrated metasurface enabling polarization-induced Fano resonance control at SWIR frequencies. The platform consists of a two-dimensional Si/GeSn core/shell nanowire array on a silicon wafer. By tuning the light polarization, we show that the metasurface reflectance can be efficiently engineered due to Fano resonances emerging from the electric and magnetic dipoles competition. The interference of optically induced dipoles in high-index nanowire arrays offers additional degrees of freedom to tailor the directional scattering and the flow of light while enabling sharp polarization-modulated resonances. This tunability is harnessed in nanosensors yielding an efficient detection of 10^{-2} changes in the refractive index of the surrounding medium.

The selective confinement of light-holes (LHs) is demonstrated by introducing a low-dimensional system consisting of highly tensile-strained Ge quantum well enabling the design of an ultrafast gate-defined spin qubit under the electric dipole spin resonance. The qubit size-dependent $g$-factor and dipole moment are mapped, and the parameters inducing their modulation are discussed. It is found that the LH qubit dipole moment is 2 to 3 orders of magnitude higher than that of the canonical heavy-hole qubit. This behavior originates from the significant spin splitting resulting from the combined action of large cubic and linear Rashba spin-orbit interactions that are peculiar to LHs. The qubit relaxation rate is also affected by the strong spin-orbit interaction and follows typically a $B^7$ behavior. The proposed all-group IV, direct bandgap LH qubit provides an effective platform for a scalable qubit-optical photon interface sought-after for long-range entanglement distribution and quantum networks.

Ge/SiGe multi-quantum well heterostructures are highly sought-after for silicon-integrated optoelectronic devices operating in the broad range of the electromagnetic spectrum covering infrared to terahertz wavelengths. However, the epitaxial growth of these heterostructures at a thickness of a few microns has been a challenging task due the lattice mismatch and its associated instabilities resulting from the formation of growth defects. To elucidates these limits, we outline herein a process for the strain-balanced growth on silicon of 11.1 nm/21.5 nm Ge/Si0.18Ge0.82 superlattices (SLs) with a total thickness of 16 {\mu}m corresponding to 500 periods. Composition, thickness, and interface width are preserved across the entire SL heterostructure, which is an indication of limited Si-Ge intermixing. High crystallinity and low defect density are obtained in the Ge/Si0.18Ge0.82 layers, however, the dislocation pile up at the interface with the growth substate induces micrometer-longs cracks on the surface. This eventually leads to significant layer tilt in the strain-balanced SL and in the formation of millimeter-long, free-standing flakes. These results confirm the local uniformity of structural properties and highlight the critical importance of threading dislocations in shaping the wafer-level stability of thick multi-quantum well heterostructures required to implement effective silicon-compatible Ge/SiGe photonic devices.

A theoretical framework incorporating atomic-level interfacial details is derived to include the electronic structure of buried interfaces and describe the behavior of charge carriers in heterostructures in the presence of finite interfacial broadening. Applying this model to ultrathin heteroepitaxial (SiGe)m/(Si)m superlattices predicts the existence of localized energy levels in the band structure induced by sub-nanometer broadening, which provides additional paths for hole-electron recombination. These predicted interfacial electronic transitions and the associated absorptive effects are confirmed experimentally at variable superlattice thickness and periodicity. By mapping the energy of the critical points, the optical transitions are identified between 2 and 2.5 eV thus extending the optical absorption to lower energies. This phenomenon enables a straightforward and non-destructive probe of the atomic-level broadening in heterostructures., Comment: 6 pages, 4 figures with a Supporting Material file

The monolithic integration of extended short-wave infrared (e-SWIR) photodetectors (PDs) on silicon is highly sought-after to implement manufacturable, cost-effective sensing and imaging technologies. With this perspective, GeSn PIN PDs have been the subject of extensive investigations because of their bandgap tunability and silicon compatibility. However, due to growth defects, these PDs suffer a relatively high dark current density as compared to commercial III-V PDs. Herein, we elucidate the mechanisms governing the dark current in $2.6 \, \mu$m GeSn PDs at a Sn content of $10$ at.%. It was found that in the temperature range of $293 \, $K -- $363 \,$K and at low bias, the diffusion and Shockley-Read-Hall (SRH) leakage mechanisms dominate the dark current in small diameter ($20 \, \mu$m) devices, while combined SRH and trap assisted tunneling (TAT) leakage mechanisms are prominent in larger diameter ($160 \, \mu$m) devices. However, at high reverse bias, TAT leakage mechanism becomes dominant regardless of the operating temperature and device size. The effective non-radiative carrier lifetime in these devices was found to reach $\sim 300$ -- $400$ ps at low bias. Owing to TAT leakage current, however, this lifetime reduces progressively as the bias increases.

Recent development on Ge$_{1-x}$Sn$_x$ nanowires with high Sn content, beyond its solid solubility limit, make them attractive for all group-IV Si-integrated infrared photonics at nanoscale. Herein, we report a chemical vapour deposition-grown high Sn-content Ge-Ge$_{0.92}$Sn$_{0.08}$ core-shell based single nanowire photodetector operating at the optical communication wavelength of 1.55 $\mu$m. The atomic concentration of Sn in nanowires has been studied using X-ray photoelectron and Raman spectroscopy data. A metal-semiconductor-metal based single nanowire photodetector, fabricated via electron beam lithography process, exhibits significant room-temperature photoresponse even at zero bias. In addition to the high-crystalline quality and identical shell composition of the nanowire, the efficient collection of photogenerated carriers under an external electric field result in the superior responsivity and photoconductive gain as high as ~70.8 A/W and ~57, respectively at an applied bias of -1.0 V. The extra-ordinary performance of the fabricated photodetector demonstrates the potential of GeSn nanowires for future Si CMOS compatible on-chip optical communication device applications., Comment: 16 pages, 4 figures, Supplementary material (2 Figures, 2 tables)

The quiet quantum environment of holes in solid-state devices has been at the core of increasingly reliable architectures for quantum processors and memories.1-6 However, due to the lack of scalable materials to properly tailor the valence band character and its energy offsets, the precise engineering of light-hole (LH) states remains a serious obstacle toward coherent photon-spin interfaces needed for a direct mapping of the quantum information encoded in photon flying qubits to stationary spin processor.4-9 Herein, to alleviate this long-standing limitation we demonstrate an all-group IV low-dimensional system consisting of highly tensile strained germanium quantum well grown on silicon allowing new degrees of freedom to control and manipulate the hole states. Wafer-level, high bi-isotropic in-plane tensile strain ($>1\%$) is achieved using strain-engineered, metastable germanium-tin alloyed buffer layers yielding quantum wells with LH ground state, high $g$-factor anisotropy, and a tunable splitting of the hole subbands. The epitaxial heterostructures display sharp interfaces with sub-nanometer broadening and show room-temperature excitonic transitions that are modulated and extended to the mid-wave infrared by controlling strain and thickness. This ability to engineer quantum structures with LH selective confinement and controllable optical response enables manufacturable silicon-compatible platforms relevant to integrated quantum communication and sensing technologies.

Electron spins in Si/SiGe quantum wells suffer from nearly degenerate conduction band valleys, which compete with the spin degree of freedom in the formation of qubits. Despite attempts to enhance the valley energy splitting deterministically, by engineering a sharp interface, valley splitting fluctuations remain a serious problem for qubit uniformity, needed to scale up to large quantum processors. Here, we elucidate and statistically predict the valley splitting by the holistic integration of 3D atomic-level properties, theory and transport. We find that the concentration fluctuations of Si and Ge atoms within the 3D landscape of Si/SiGe interfaces can explain the observed large spread of valley splitting from measurements on many quantum dot devices. Against the prevailing belief, we propose to boost these random alloy composition fluctuations by incorporating Ge atoms in the Si quantum well to statistically enhance valley splitting.

The prospect of GeSn semiconductors for silicon-integrated infrared optoelectronics brings new challenges related to the metastability of this class of materials. As a matter of fact, maintaining a reduced thermal budget throughout all processing steps of GeSn devices is essential to avoid possible material degradation. This constraint is exacerbated by the need for higher Sn contents along with an enhanced strain relaxation to achieve efficient mid-infrared devices. Herein, as a low thermal budget solution for post-epitaxy processing, we elucidate the effects of laser thermal annealing (LTA) on strain-relaxed Ge$_{0.89}$Sn0$_{.11}$ layers and Ni-Ge$_{0.89}$Sn0$_{.11}$ contacts. Key diffusion and recrystallization processes are proposed and discussed in the light of systematic microstructural studies. LTA treatment at a fluence of 0.40 J/cm2 results in a 200-300 nm-thick layer where Sn atoms segregate toward the surface and in the formation of Sn-rich columnar structures in the LTA-affected region. These structures are reminiscent to those observed in the dislocation-assisted pipe-diffusion mechanism, while the buried GeSn layers remain intact. Moreover, by tailoring the LTA fluence, the contact resistance can be reduced without triggering phase separation across the whole GeSn multi-layer stacking. Indeed, a one order of magnitude decrease in the Ni-based specific contact resistance was obtained at the highest LTA fluence, thus confirming the potential of this method for the functionalization of direct bandgap GeSn materials.

Group IV Ge1-xSnx semiconductors hold the premise of enabling broadband silicon-integrated infrared optoelectronics due to their tunable bandgap energy and directness. Herein, we exploit these attributes along with the enhanced lattice strain relaxation in Ge/Ge0.92Sn0.08 core-shell nanowire heterostructures to implement highly responsive, room-temperature short-wave infrared nanoscale photodetectors. Atomic-level studies confirm the uniform shell composition and its higher crystallinity with respect to thin films counterparts. The demonstrated Ge/Ge0.92Sn0.08 p-type field-effect nanowire transistors exhibit superior optoelectronic properties achieving simultaneously a relatively high mobility, a high ON/OFF ratio, and a high responsivity, in addition to a broadband absorption in the short-wave infrared range. Indeed, the reduced bandgap of the Ge0.92Sn0.08 shell yields an extended cutoff wavelength of 2.1 um, with a room-temperature responsivity reaching 2.7 A/W at 1550 nm. These results highlight the potential of Ge/Ge1-xSnx core/shell nanowires as silicon-compatible building blocks for nanoscale integrated infrared photonics., Comment: 22 pages, 4 figures, 1 Tables, 5 Supplementary information Figures

Indium antimonide (InSb) nanowires are used as building blocks for quantum devices because of their unique properties, i.e., strong spin-orbit interaction and large Land\'e g-factor. Integrating InSb nanowires with other materials could potentially unfold novel devices with distinctive functionality. A prominent example is the combination of InSb nanowires with superconductors for the emerging topological particles research. Here, we combine the II-VI cadmium telluride (CdTe) with the III-V InSb in the form of core-shell (InSb-CdTe) nanowires and explore potential applications based on the electronic structure of the InSb-CdTe interface and the epitaxy of CdTe on the InSb nanowires. We determine the electronic structure of the InSb-CdTe interface using density functional theory and extract a type-I band alignment with a small conduction band offset ($\leq$ 0.3 eV). These results indicate the potential application of these shells for surface passivation or as tunnel barriers in combination with superconductors. In terms of the structural quality of these shells, we demonstrate that the lattice-matched CdTe can be grown epitaxially on the InSb nanowires without interfacial strain or defects. These epitaxial shells do not introduce disorder to the InSb nanowires as indicated by the comparable field-effect mobility we measure for both uncapped and CdTe-capped nanowires.

Advances in quantum technology may come from the discovery of new materials systems that improve the performance or allow for new functionality in electronic devices. Lead telluride (PbTe) is a member of the group IV-VI materials family that has significant untapped potential for exploration. Due to its high electron mobility, strong spin-orbit coupling and ultrahigh dielectric constant it can host few-electron quantum dots and ballistic quantum wires with opportunities for control of electron spins and other quantum degrees of freedom. Here, we report the fabrication of PbTe nanowires by molecular beam epitaxy. We achieve defect-free single crystalline PbTe with large aspect ratios up to 50 suitable for quantum devices. Furthermore, by fabricating a single nanowire field effect transistor, we attain bipolar transport, extract the bandgap and observe Fabry-Perot oscillations of conductance, a signature of quasiballistic transmission.

Semiconductor nanowires have emerged as versatile components in superconducting hybrid devices for Majorana physics and quantum computing. The transport properties of nanowires can be tuned either by field-effect or doping. We investigated a series of InAs nanowires which conductivity has been modified by n-type doping using tellurium. In addition to electron microscopy studies, the wires were also examined with atomic probe tomography to obtain information about the local incorporation of Te atoms. It was found that the Te atoms mainly accumulate in the core of the nanowire and at the corners of the {110} side facets. The efficiency of n-type doping was also confirmed by transport measurements. As a demonstrator hybrid device, a Josephson junction was fabricated using a nanowire as a weak link. The corresponding measurements showed a clear increase of the critical current with increase of the dopant concentration., Comment: 9 pages, 9 figures

GeSn alloys have been regarded as a potential lasing material for a complementary metal-oxide-semiconductor (CMOS)-compatible light source. Despite their remarkable progress, all GeSn lasers reported to date have large device footprints and active areas, which prevent the realization of densely integrated on-chip lasers operating at low power consumption. Here, we present a 1D photonic crystal (PC) nanobeam with a very small device footprint of 7 ${\mu}m^2$ and a compact active area of ~1.2 ${\mu}m^2$ on a high-quality GeSn-on-insulator (GeSnOI) substrate. We also report that the improved directness in our strain-free nanobeam lasers leads to a lower threshold density and a higher operating temperature compared to the compressive strained counterparts. The threshold density of the strain-free nanobeam laser is ~18.2 kW cm$^{ -2}$ at 4 K, which is significantly lower than that of the unreleased nanobeam laser (~38.4 kW cm$^{ -2}$ at 4 K). Lasing in the strain-free nanobeam device persists up to 90 K, whereas the unreleased nanobeam shows a quenching of the lasing at a temperature of 70 K. Our demonstration offers a new avenue towards developing practical group-IV light sources with high-density integration and low power consumption., Comment: 14 pages, 6 figures

This work unravels the atomic details of the interaction of solute atoms with nanoscale crystalline defects. The complexity of this phenomenon is elucidated through detailed atom probe tomographic investigations on epitaxially-strained, compositionally metastable, semiconductor alloys. Subtle variations are uncovered in the concentration and distribution of solute atoms surrounding dislocations, and their dynamic evolution is highlighted. The results demonstrate that crystal defects, such as dislocations, are instrumental in initiating the process of phase separation in strained metastable layers. Matrix regions, close to the dislocations, show clear signs of compositional degradation only after a relatively short time from disrupting the local equilibrium. The solute concentration as well as the density of non-random atomic clusters increases while approaching a dislocation from the surrounding matrix region. In parallel, far from a dislocation the lattice remains intact preserving the metastable structure and composition uniformity. At advanced stages of phase separation, the matrix outside the dislocation reaches the equilibrium concentration, while dislocations act as vehicles of mass-transport, providing fast diffusive channels for solute atoms to reach the surface. Besides, the number of atomic clusters almost doubles and the number of atoms per cluster increases steadily, moving along a dislocation towards the surface. In addition to understanding the atomic features involved in the phase separation of strained metastable alloys, the work also illustrates the thermodynamic and kinetic behavior of solute atoms in the vicinity of a nanoscale defect and describe quantitatively the key processes, thus providing the empirical input to improve the atomic models and simulations.

GeSn alloys are promising candidates for complementary metal-oxide-semiconductor (CMOS)-compatible, tunable lasers. Relaxation of residual compressive strain in epitaxial GeSn has recently shown promise in improving the lasing performance. However, the suspended device configuration that has thus far been introduced to relax the strain is destined to limit heat dissipation, thus hindering the device performance. Herein, we demonstrate that strain-free GeSn microdisk laser devices fully released on Si outperform the canonical suspended devices. This approach allows to simultaneously relax the limiting compressive strain while offering excellent thermal conduction. Optical simulations confirm that, despite a relatively small refractive index contrast between GeSn and Si, optical confinement in strain-free GeSn optical cavities on Si is superior to that in conventional strain-free GeSn cavities suspended in the air. Moreover, thermal simulations indicate a negligible temperature increase in our device. Conversely, the temperature in the suspended devices increases substantially reaching, for instance, 120 K at a base temperature of 75 K under the employed optical pumping conditions. Such improvements enable increasing the operation temperature by ~40 K and reducing the lasing threshold by 30%. This approach lays the groundwork to implement new designs in the quest for room temperature GeSn lasers on Si., Comment: 16 pages, 7 figures

A true monolithic infrared photonics platform is within reach if strain and bandgap energy can be independently engineered in SiGeSn semiconductors. Herein, we investigate the structural and optoelectronic properties of a 1.5 {\mu}m-thick Si0.06Ge0.90Sn0.04 layer that is nearly lattice-matched to a Ge on Si substrate. Atomic-level studies demonstrate high crystalline quality and uniform composition and show no sign of short-range ordering and clusters. Room temperature spectroscopic ellipsometry and transmission measurements show direct bandgap absorption at 0.83 eV and a reduced indirect bandgap absorption at lower energies. Si0.06Ge0.90Sn0.04 photoconductive devices operating at room temperature exhibit dark current and spectral responsivity (1 A/W below 1.5 {\mu}m wavelengths) similar to Ge on Si devices, with the advantage of a near-infrared band gap tunable by alloy composition. These results underline the relevance of SiGeSn semiconductors in implementing a group IV material platform for silicon-integrated infrared optoelectronics.

GeSn alloys are metastable semiconductors that have been proposed as building blocks for silicon-integrated short-wave and mid-wave infrared photonic and sensing platforms. Exploiting these semiconductors requires, however, the control of their epitaxy and their surface chemistry to reduce non-radiative recombination that hinders the efficiency of optoelectronic devices. Herein, we demonstrate that a combined sulfur- and iodine-based treatments yields effective passivation of Ge and Ge0.9Sn0.1 surfaces. X-ray photoemission spectroscopy and in situ spectroscopic ellipsometry measurements were used to investigate the dynamics of surface stability and track the reoxidation mechanisms. Our analysis shows that the largest reduction in oxide after HI treatment, while HF+(NH4)2S results in a lower re-oxidation rate. A combined HI+(NH4)2S treatment preserves the lowest oxide ratio <10 % up to 1 hour of air exposure, while less than half of the initial oxide coverage is reached after 4 hours. These results highlight the potential of S- and I-based treatments in stabilizing the GeSn surface chemistry thus enabling a passivation method that is compatible with materials and device processing.

(Si)GeSn semiconductors are finally coming of age after a long gestation period. The demonstration of device quality epi-layers and quantum-engineered heterostructures has meant that tunable all-group IV Si-integrated infrared photonics is now a real possibility. Notwithstanding the recent exciting developments in (Si)GeSn materials and devices, this family of semiconductors is still facing serious limitations that need to be addressed to enable reliable and scalable applications. The main outstanding challenges include the difficulty to grow high crystalline quality layers and heterostructures at the desired Sn content and lattice strain, preserve the material integrity during growth and throughout device processing steps, and control doping and defect density. Other challenges are related to the lack of optimized device designs and predictive theoretical models to evaluate and simulate the fundamental properties and performance of (Si)GeSn layers and heterostructures. This Perspective highlights key strategies to circumvent these hurdles and bring this material system to maturity to create far-reaching new opportunities for Si-compatible infrared photodetectors, sensors, and emitters for applications in free-space communication, infrared harvesting, biological and chemical sensing, and thermal imaging.

Strain engineering has been a ubiquitous paradigm to tailor the electronic band structure and harness the associated new or enhanced fundamental properties in semiconductors. In this regard, semiconductor membranes emerged as a versatile class of nanoscale materials to control lattice strain and engineer complex heterostructures leading to the development of a variety of innovative applications. Herein we exploit this quasi-two-dimensional platform to tune simultaneously the lattice parameter and bandgap energy in group IV GeSn semiconductor alloys. As Sn content is increased to reach a direct band gap, these semiconductors become metastable and typically compressively strained. We show that the release and transfer of GeSn membranes lead to a significant relaxation thus extending the absorption wavelength range deeper in the mid-infrared. Fully released Ge$_{0.83}$Sn$_{0.17}$ membranes were integrated on silicon and used in the fabrication of broadband photodetectors operating at room temperature with a record wavelength cutoff of 4.6 $\mu$m, without compromising the performance at shorter wavelengths down to 2.3 $\mu$m. These membrane devices are characterized by two orders of magnitude reduction in dark current as compared to devices processed from as-grown strained epitaxial layers. The latter exhibit a content-dependent, shorter wavelength cutoff in the 2.6-3.5 $\mu$m range, thus highlighting the role of lattice strain relaxation in shaping the spectral response of membrane photodetectors. This ability to engineer all-group IV transferable mid-infrared photodetectors lays the groundwork to implement scalable and flexible sensing and imaging technologies exploiting these integrative, silicon-compatible strained-relaxed GeSn membranes.

Phonon surface scattering has been at the core of heat transport engineering in nanoscale structures and devices. Herein, we demonstrate that this phonon pathway can be the sole mechanism only below a characteristic, size-dependent temperature. Above this temperature, the lattice phonon scattering co-exist along with surface effects. By artificially controlling mass disorder and lattice dynamics at the atomic-level in nanowires without affecting morphology, crystallinity, chemical composition, and electronic properties, the temperature-thermal conductivity-diameter triple parameter space is mapped, and the main phonon scattering mechanisms are disentangled. This led to the identification of the critical temperature at which the effect of lattice mass-disorder on thermal conductivity is suppressed to an extent that phonon transport becomes governed entirely by the surface. This behavior is discussed based on Landauer-Dutta-Lundstrom near-equilibrium transport model. The established framework provides the necessary input to further advance the design and modelling of phonon and heat transport in semiconductor nanoscale systems., Comment: 12 pages text, 4 Figures, 13 pages Supplementary Information

A clear signature of Zeeman split states crossing is observed in Landau fan diagram of strained germanium two-dimensional hole gas. The underlying mechanisms are discussed based on a perturbative model yielding a closed formula for the critical magnetic fields. These fields depend strongly on the energy difference between the top-most and the neighboring valence bands and are sensitive to the quantum well thickness, strain, and spin-orbit-interaction. The latter is a necessary feature for the crossing to occur. This framework enables a straightforward quantification of the hole-state parameters from simple measurements, thus paving the way for its use in design and modelling of hole-based quantum devices., Comment: Corrected typos in expressions for F_l. Minor changes to sections layout

Pnictogens have multiple allotropic forms resulting from their ns2 np3 valence electronic configuration, making them the only elemental materials to crystallize in layered van der Waals (vdW) and quasi-vdW structures throughout the group. Light group VA elements are found in the layered orthorhombic A17 phase such as black phosphorus, and can transition to the layered rhombohedral A7 phase at high pressure. On the other hand, bulk heavier elements are only stable in the A7 phase. Herein, we demonstrate that these two phases not only co-exist during the vdW growth of antimony on weakly interacting surfaces, but also undertake a spontaneous transformation from the A17 phase to the thermodynamically stable A7 phase. This metastability of the A17 phase is revealed by real-time studies unraveling its thickness-driven transition to the A7 phase and the concomitant evolution of its electronic properties. At a critical thickness of ~4 nm, A17 antimony undergoes a diffusionless shuffle transition from AB to AA stacked alpha-antimonene followed by a gradual relaxation to the A7 bulk-like phase. Furthermore, the electronic structure of this intermediate phase is found to be determined by surface self-passivation and the associated competition between A7- and A17-like bonding in the bulk. These results highlight the critical role of the atomic structure and interfacial interactions in shaping the stability and electronic characteristics of vdW layered materials, thus enabling a new degree of freedom to engineer their properties using scalable processes.

By independently engineering strain and composition, this work demonstrates and investigates direct band gap emission in the mid-infrared range from GeSn layers grown on silicon. We extend the room-temperature emission wavelength above ~4.0 {\mu}m upon post-growth strain relaxation in layers with uniform Sn content of 17 at.%. The fundamental mechanisms governing the optical emission are discussed based on temperature-dependent photoluminescence, absorption measurements, and theoretical simulations. Regardless of strain and composition, these analyses confirm that single-peak emission is always observed in the probed temperature range of 4-300 K, ruling out defect- and impurity-related emission. Moreover, carrier losses into thermally-activated non-radiative recombination channels are found to be greatly minimized as a result of strain relaxation. Absorption measurements validate the direct band gap absorption in strained and relaxed samples at energies closely matching photoluminescence data. These results highlight the strong potential of GeSn semiconductors as versatile building blocks for scalable, compact, and silicon-compatible mid-infrared photonics and quantum opto-electronics.

Controlling the growth kinetics from the vapor phase has been a powerful paradigm enabling a variety of metastable epitaxial semiconductors such as Sn-containing group IV semiconductors (Si)GeSn. In addition to its importance for emerging photonic and optoelectronic applications, this class of materials is also a rich platform to highlight the interplay between kinetics and thermodynamic driving forces during growth of strained, nonequilibrium alloys. Indeed, these alloys are inherently strained and supersaturated in Sn and thus can suffer instabilities that are still to be fully elucidated. In this vein, in this work the atomic-scale microstructure of Ge0.82Sn0.18 is investigated at the onset of phase separation as the epitaxial growth aborts. In addition to the expected accumulation of Sn on the surface leading to Sn-rich droplets and sub-surface regions with the anticipated equilibrium Sn composition of 1.0at.%, the diffusion of Sn atoms also yields conspicuous Sn-decorated filaments with nonuniform Sn content in the range of ~1 to 11at.% . The latter are attributed to the formation and propagation of dislocations, facilitating the Sn transport toward the surface through pipe diffusion. Furthermore, the interface between the Sn droplet and GeSn shows a distinct, defective layer with Sn content of ~22at.%. This layer is likely formed by the expelled excess equilibrium Ge as the Sn solidifies, and its content seems to be a consequence of strain minimization between tetragonal Sn-rich and cubic Ge-rich equilibrium phases. The elucidation of these phenomena is crucial to understand the stability of GeSn semiconductors and control their epitaxial growth at a uniform composition., Comment: Submitted to Crystal Growth & Design. 20 pages. 5 figures

: n-type Ge/SiGe asymmetric-coupled quantum wells represent the building block of a variety of nanoscale quantum devices, including recently proposed designs for a silicon-based THz quantum cascade laser. In this paper, we combine structural and spectroscopic experiments on 20-module superstructures, each featuring two Ge wells coupled through a Ge-rich tunnel barrier, as a function of the geometry parameters of the design and the P dopant concentration. Through the comparison of THz spectroscopic data with numerical calculations of intersubband optical absorption resonances, we demonstrated that it is possible to tune by design the energy and the spatial overlap of quantum confined subbands in the conduction band of the heterostructures. The high structural/interface quality of the samples and the control achieved on subband hybridization are the promising starting point towards a working electrically pumped light-emitting device.

Germanium-Tin (GeSn) alloys have emerged as a promising material for future optoelectronics, energy harvesting and nanoelectronics owing to their direct bandgap and compatibility with existing Si-based electronics. Yet, their metastability poses significant challenges calling for in-depth investigations of their thermal behavior. With this perspective, this work addresses the interdiffusion processes throughout thermal annealing of pseudomorphic GeSn binary and SiGeSn ternary alloys. In both systems, the initially pseudomorphic layers are relaxed upon annealing exclusively via thermally induced diffusional mass transfer of Sn. Systematic post-growth annealing experiments reveal enhanced Sn and Si diffusion regimes that manifest at temperatures below 600{\deg}C. The amplified low-temperature diffusion and the observation of only subtle differences between binary and ternary hint at the unique metastability of the Si-Ge-Sn material system as the most important driving force for phase separation., Comment: 15 pages, 3 figures

The interfacial abruptness and uniformity in heterostructures are critical to control their electronic and optical properties. With this perspective, this work demonstrates the 3-D atomistic-level mapping of the roughness and uniformity of buried epitaxial interfaces in Si/SiGe superlattices with a layer thickness in the 1.5-7.5 nm range. Herein, 3-D atom-by-atom maps were acquired and processed to generate iso-concentration surfaces highlighting local fluctuations in content at each interface. These generated surfaces were subsequently utilized to map the interfacial roughness and its spatial correlation length. The analysis revealed that the root mean squared roughness of the buried interfaces in the investigated superlattices is sensitive to the growth temperature with a value varying from about 0.2 nm (+/- 13%) to about 0.3 nm (+/- 11.5%) in the temperature range of 500-650 Celsius. The estimated horizontal correlation lengths were found to be 8.1 nm (+/- 5.8%) at 650 Celsius and 10.1 nm (+/- 6.2%) at 500 Celsius. Additionally, reducing the growth temperature was found to improve the interfacial abruptness, with 30 % smaller interfacial width is obtained at 500 Celsius. This behavior is attributed to the thermally activated atomic exchange at the surface during the heteroepitaxy. Finally, by testing different optical models with increasing levels of interfacial complexity, it is demonstrated that the observed atomic-level roughening at the interface must be accounted for to accurately describe the optical response of Si/SiGe heterostructures., Comment: 17 A4 pages of main manuscript, 2 table, 5 figures, 20 A4 pages of supplementary information

Understanding the nature and behavior of vacancy-like defects in epitaxial GeSn metastable alloys is crucial to elucidate the structural and optoelectronic properties of these emerging semiconductors. The formation of vacancies and their complexes is expected to be promoted by the relatively low substrate temperature required for the epitaxial growth of GeSn layers with Sn contents significantly above the equilibrium solubility of 1 at.%. These defects can impact both the microstructure and charge carrier lifetime. Herein, to identify the vacancy-related complexes and probe their evolution as a function of Sn content, depth-profiled pulsed low-energy positron annihilation lifetime spectroscopy and Doppler broadening spectroscopy were combined to investigate GeSn epitaxial layers with Sn content in the 6.5-13.0 at.% range. The samples were grown by chemical vapor deposition method at temperatures between 300 and 330 {\deg}C. Regardless of the Sn content, all GeSn samples showed the same depth-dependent increase in the positron annihilation line broadening parameters, which confirmed the presence of open volume defects. The measured average positron lifetimes were the highest (380-395 ps) in the region near the surface and monotonically decrease across the analyzed thickness, but remain above 350 ps. All GeSn layers exhibit lifetimes that are 85 to 110 ps higher than the Ge reference layers. Surprisingly, these lifetimes were found to decrease as Sn content increases in GeSn layers. These measurements indicate that divacancies are the dominant defect in the as-grown GeSn layers. However, their corresponding lifetime was found to be shorter than in epitaxial Ge thus suggesting that the presence of Sn may alter the structure of divacancies. Additionally, GeSn layers were found to also contain a small fraction of vacancy clusters, which become less important as Sn content increases.

We report on the behavior of Ge-Ge, Ge-Sn, Sn-Sn like and disorder-activated vibrational modes in GeSn semiconductors investigated using Raman scattering spectroscopy. By using an excitation wavelength close to E1 gap, all modes are clearly resolved and their evolution as a function of strain and Sn content is established. In order to decouple the individual contribution of content and strain, the analysis was conducted on series of pseudomorphic and relaxed epitaxial layers with a Sn content in the 5-17at.% range. All vibrational modes were found to display the same qualitative behavior as a function of content and strain, viz. a linear downshift as the Sn content increases or the compressive strain relaxes. Simultaneously, Ge-Sn and Ge-Ge peaks broaden, and the latter becomes increasingly asymmetric. This asymmetry, coupled with the peak position, is exploited in an empirical method to accurately quantify the Sn composition and lattice strain from Raman spectra.

Sn-containing Si and Ge alloys belong to an emerging family of semiconductors with the potential to impact group IV semiconductor devices. Indeed, the ability to independently engineer both lattice parameter and band gap holds the premise to develop enhanced or novel photonic, optoelectronic, and electronic devices. With this perspective, we present detailed investigations of the influence of Ge1-y-xSixSny layers on the optical properties of Si- and Ge-based heterostructures and nanowires. We found that adding a thin Ge1-x-ySixSny capping layer on Si or Ge greatly enhances light absorption especially in the near IR range leading to an increase in short-circuit current density. For the Ge1-y-xSixSny structure at thicknesses below 30 nm, a 14-fold increase in the short-circuit current is predicted with respect to bare Si. This enhancement decreases by reducing the capping layer thickness. Conversely, decreasing the shell thickness was found to improve the short-circuit current in Si/Ge1-y-xSixSny and Ge/Ge1-y-xSixSny core/shell nanowires. The optical absorption becomes very important when increasing the Sn content. Moreover, by exploiting optical antenna effect, these nanowires show an extreme light absorption reaching an enhancement factor, with respect to Si or Ge nanowires, on the order of ~104 in Si/Ge0.84Si0.04Sn0.12 and ~12 in Ge/Ge0.84Si0.04Sn0.12 core/shell nanowires. Furthermore, we analyzed the optical response of the addition of a dielectric capping layer consisting of Si3N4 to the Si/Ge1-y-xSixSny core-shell nanowire and found about 50% increase in short-circuit current density for a dielectric layer thickness of 45 nm and a core radius and shell thickness superior to 40 nm. The core/shell optical antenna benefits from a multiplication of enhancements contributed by leaky mode resonances in the semiconductor part and antireflection effects in the dielectric part., Comment: 47 pages, 11 figures