Low-Temperature ALD of SbOx /Sb2 Te3 Multilayers with Boosted Thermoelectric Performance.

Nanoscale superlattice (SL) structures have proven to be effective in enhancing the thermoelectric (TE) properties of thin films. Herein, the main phase of antimony telluride (Sb2 Te3 ) thin film with sub-nanometer layers of antimony oxide (SbOx ) is synthesized via atomic layer deposition (ALD) at a low temperature of 80 °C. The SL structure is tailored by varying the cycle numbers of Sb2 Te3 and SbOx . A remarkable power factor of 520.8 µW m-1 K-2 is attained at room temperature when the cycle ratio of SbOx and Sb2 Te3 is set at 1:1000 (i.e., SO:ST = 1:1000), corresponding to the highest electrical conductivity of 339.8 S cm-1 . The results indicate that at the largest thickness, corresponding to ten ALD cycles, the SbOx layers act as a potential barrier that filters out the low-energy charge carriers from contributing to the overall electrical conductivity. In addition to enhancing the scattering of the mid-to-long-wavelength at the SbOx /Sb2 Te3 interface, the presence of the SbOx sub-layer induces the confinement effect and strain forces in the Sb2 Te3 thin film, thereby effectively enhancing the Seebeck coefficient and reducing the thermal conductivity. These findings provide a new perspective on the design of SL-structured TE materials and devices.

Wafer-Scale Growth of Sb2Te3 Films via Low-Temperature Atomic Layer Deposition for Self-Powered Photodetectors.

In this work, we demonstrate the performance of a silicon-compatible, high-performance, and self-powered photodetector. A wide detection range from visible (405 nm) to near-infrared (1550 nm) light was enabled by the vertical p-n heterojunction between the p-type antimony telluride (Sb2Te3) thin film and the n-type silicon (Si) substrates. A Sb2Te3 film with a good crystal quality, low density of extended defects, proper stoichiometry, p-type nature, and excellent uniformity across a 4 in. wafer was achieved by atomic layer deposition at 80 °C using (Et3Si)2Te and SbCl3 as precursors. The processed photodetectors have a low dark current (∼20 pA), a high responsivity of (∼4.3 A/W at 405 nm and ∼150 mA/W at 1550 nm), a peak detectivity of ∼1.65 × 1014 Jones, and a quick rise time of ∼98 µs under zero bias voltage. Density functional theory calculations reveal a narrow, near-direct, type-II band gap at the heterointerface that supports a strong built-in electric field leading to efficient separation of the photogenerated carriers. The devices have long-term air stability and efficient switching behavior even at elevated temperatures. These high-performance and self-powered p-Sb2Te3/n-Si heterojunction photodetectors have immense potential to become reliable technological building blocks for a plethora of innovative applications in next-generation optoelectronics, silicon-photonics, chip-level sensing, and detection.

Electronic Signature of Subnanometer Interfacial Broadening in Heterostructures.

Interfaces are ubiquitous in semiconductor low-dimensional systems used in electronics, photonics, and quantum computing. Understanding their atomic-level properties has thus been crucial to controlling the basic behavior of heterostructures and optimizing the device performance. Herein, we demonstrate that subnanometer interfacial broadening in heterostructures induces localized energy states. This phenomenon is predicted within a theory incorporating atomic-level interfacial details obtained by atom probe tomography. The experimental validation is achieved using heteroepitaxial (Si1-xGex)m/(Si)m superlattices as a model system demonstrating the existence of additional paths for hole-electron recombination. These predicted interfacial electronic transitions and the associated absorptive effects are evaluated 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 is shown to provide an optical fingerprint for a straightforward and nondestructive probe of the subnanometer broadening in heterostructures.

A Light-Hole Germanium Quantum Well on Silicon.

The quiet quantum environment of holes in solid-state devices is at the core of increasingly reliable architectures for quantum processors and memories. 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 optical photon-spin interfaces needed for a direct mapping of the quantum information encoded in photon flying qubits to stationary spin processors. Herein, to alleviate this long-standing limitation, an all-group-IV low-dimensional system is demonstrated, consisting of a 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 sub-bands. 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.

Atomic Pathways of Solute Segregation in the Vicinity of Nanoscale Defects.

Using GeSn semiconductor as a model system, this work unravels the atomic-level details of the behavior of solutes in the vicinity of a dislocation prior to surface segregation in strained, metastable thin layers. The dislocations appear in the 3D atom probe tomography maps as columnar regions, 3.5-4.0 nm wide, with solute concentrations 3-4 times higher than the sounding matrix. During the initial stage of phase separation, the migration of solute atoms toward the dislocation is associated with a gradual increase in Sn concentration and in density of atomic clusters, which reach 175-190 per 103 nm3 with 12-15 atoms/cluster close to dislocations. The latter provide, at advanced stages, fast diffusive channels for Sn mass-transport to the surface, thus bringing the matrix around the dislocation to the equilibrium concentration. In parallel, an increase in solute concentration (∼0.05 at. %/nm) and in the number of atomic clusters (12-16 clusters/33 nm) is observed along the dislocation core.

3D Atomic Mapping of Interfacial Roughness and Its Spatial Correlation Length in Sub-10 nm Superlattices.

The interfacial abruptness and uniformity in heterostructures are critical to control their electronic and optical properties. With this perspective, this work demonstrates the three-dimensional (3D) atomic-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, 3D atom-by-atom maps were acquired and processed to generate isoconcentration 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 0.17 ± 0.02 to 0.26 ± 0.03 nm in the temperature range of 500-650 °C. The estimated horizontal correlation lengths were found to be 8.11 ± 0.5 nm at 650 °C and 10.09 ± 0.6 nm at 500 °C. Additionally, reducing the growth temperature was found to improve the interfacial abruptness, with a 30% smaller interfacial width is obtained at 500 °C. 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.

Highly tensile-strained Ge/InAlAs nanocomposites.

Self-assembled nanocomposites have been extensively investigated due to the novel properties that can emerge when multiple material phases are combined. Growth of epitaxial nanocomposites using lattice-mismatched constituents also enables strain-engineering, which can be used to further enhance material properties. Here, we report self-assembled growth of highly tensile-strained Ge/In0.52Al0.48As (InAlAs) nanocomposites by using spontaneous phase separation. Transmission electron microscopy shows a high density of single-crystalline germanium nanostructures coherently embedded in InAlAs without extended defects, and Raman spectroscopy reveals a 3.8% biaxial tensile strain in the germanium nanostructures. We also show that the strain in the germanium nanostructures can be tuned to 5.3% by altering the lattice constant of the matrix material, illustrating the versatility of epitaxial nanocomposites for strain engineering. Photoluminescence and electroluminescence results are then discussed to illustrate the potential for realizing devices based on this nanocomposite material.

Laser-Assisted Field Evaporation and Three-Dimensional Atom-by-Atom Mapping of Diamond Isotopic Homojunctions.

It addition to its high evaporation field, diamond is also known for its limited photoabsorption, strong covalent bonding, and wide bandgap. These characteristics have been thought for long to also complicate the field evaporation of diamond and make its control hardly achievable on the atomistic-level. Herein, we demonstrate that the unique behavior of nanoscale diamond and its interaction with pulsed laser lead to a controlled field evaporation thus enabling three-dimensional atom-by-atom mapping of diamond (12)C/(13)C homojunctions. We also show that one key element in this process is to operate the pulsed laser at high energy without letting the dc bias increase out of bounds for diamond nanotip to withstand. Herein, the role of the dc bias in evaporation of diamond is essentially to generate free charge carriers within the nanotip via impact ionization. The mobile free charges screen the internal electric field, eventually creating a hole rich surface where the pulsed laser is effectively absorbed leading to an increase in the nanotip surface temperature. The effect of this temperature on the uncertainty in the time-of-flight of an ion, the diffusion of atoms on the surface of the nanotip, is also discussed. In addition to paving the way toward a precise manipulation of isotopes in diamond-based nanoscale and quantum structures, this result also elucidates some of the basic properties of dielectric nanostructures under high electric field.

An electrically excited nanoscale light source with active angular control of the emitted light.

We report on the angular distribution, polarization, and spectrum of the light emitted from an electrically controlled nanoscale light source. This nanosource of light arises from the local, low-energy, electrical excitation of localized surface plasmons (LSP) on individual gold nanoparticles using a scanning tunneling microscope (STM). The gold nanoparticles (NP) are chemically synthesized truncated bitetrahedrons. The emitted light is collected through the transparent substrate and the emission characteristics (angular distribution, polarization, and spectrum) are analyzed. These three observables are found to strongly depend on the lateral position of the STM tip with respect to the triangular upper face of the gold NP. In particular, the resulting light emission changes orientation when the electrical excitation via the STM tip is moved from the base to the vertex of the triangular face. On the basis of the comparison of the experimental observations with an analytical dipole model and finite-difference time-domain (FDTD) calculations, we show that this behavior is linked to the selective excitation of the out-of-plane and in-plane dipolar LSP modes of the NP. This selective excitation is achieved through the lateral position of the tip with respect to the symmetry center of the NP.