GeSn-on-GaAs with photoconductive carrier lifetime >400 ns: role of substrate orientation and atomistic simulation.

Group IV GeSn quantum material finds application in electronics and silicon-compatible photonics. Synthesizing these materials with low defect density and high carrier lifetime is a potential challenge due to lattice mismatch induced defects and tin segregation at higher growth temperature. Recent advancements in the growth of these GeSn materials on Si, Ge, GaAs, and with substrate orientations, demonstrated different properties using epitaxial and chemical deposition methods. This article addresses the effect of GaAs substrate orientation and misorientation on the materials' properties and carrier lifetimes in epitaxial Ge0.94Sn0.06 layers. With starting GaAs substrates of (100)/2°, (100)/6°, (110) and (111)A orientations, Ge0.94Sn0.06 epitaxial layers were grown with an intermediate Ge buffer layer by molecular beam epitaxy and analyzed by several analytical tools. X-ray analysis displayed good crystalline quality, and Raman spectroscopy measurements showed blue shifts in phonon wavenumber due to biaxial compressive strain in Ge0.94Sn0.06 epilayers. Cross-sectional transmission electron microscopy analysis confirmed the defect-free heterointerface of Ge0.94Sn0.06/Ge/GaAs heterostructure. Minority carrier lifetimes of the unintentionally doped n-type Ge0.94Sn0.06 epilayers displayed photoconductive carrier lifetimes of >400 ns on (100)/6°, 319 ns on (100)/2°, and 434 ns on (110) GaAs substrate at 1500 nm excitation wavelength. On the other hand, Ge0.94Sn0.06 layer showed poor carrier lifetime on (111)A GaAs substrate. The observed differences in carrier lifetimes were correlated with the formation energy of the Ge on (100)/6° and (100)/2° GaAs heterointerface using Stillinger-Weber interatomic potential model-based atomistic simulation with different heterointerfacial bonding by Synopsys QuantumATK tool. Total energy computation of 6280-atom Ge/GaAs supercell on (100)/6° leads to lower formation energy than (100)/2°, making it more thermodynamically stable. Hence, the growth of the GeSn/III-V material system using misoriented (100) substrates that are more thermodynamically stable will enhance the performances of optoelectronic devices.

A tight-binding study of single-atom transistors.

A detailed theoretical study of the electronic and transport properties of a single atom transistor, where a single phosphorus atom is embedded within a single crystal transistor architecture, is presented. Using a recently reported deterministic single-atom transistor as a reference, the electronic structure of the device is represented atomistically with a tight-binding model, and the channel modulation is simulated self-consistently with a Thomas-Fermi method. The multi-scale modeling approach used allows confirmation of the charging energy of the one-electron donor charge state and explains how the electrostatic environments of the device electrodes affects the donor confinement potential and hence extent in gate voltage of the two-electron charge state. Importantly, whilst devices are relatively insensitive to dopant ordering in the highly doped leads, a ∼1% variation of the charging energy is observed when a dopant is moved just one lattice spacing within the device. The multi-scale modeling method presented here lays a strong foundation for the understanding of single-atom device structures: essential for both classical and quantum information processing.

Spin blockade and exchange in Coulomb-confined silicon double quantum dots.

Electron spins confined to phosphorus donors in silicon are promising candidates as qubits because of their long coherence times, exceeding seconds in isotopically purified bulk silicon. With the recent demonstrations of initialization, readout and coherent manipulation of individual donor electron spins, the next challenge towards the realization of a Si:P donor-based quantum computer is the demonstration of exchange coupling in two tunnel-coupled phosphorus donors. Spin-to-charge conversion via Pauli spin blockade, an essential ingredient for reading out individual spin states, is challenging in donor-based systems due to the inherently large donor charging energies (∼45 meV), requiring large electric fields (>1 MV m(-1)) to transfer both electron spins onto the same donor. Here, in a carefully characterized double donor-dot device, we directly observe spin blockade of the first few electrons and measure the effective exchange interaction between electron spins in coupled Coulomb-confined systems.

Transport in asymmetrically coupled donor-based silicon triple quantum dots.

We demonstrate serial electron transport through a donor-based triple quantum dot in silicon fabricated with nanoscale precision by scanning tunnelling microscopy lithography. From an equivalent circuit model, we calculate the electrochemical potentials of the dots allowing us to identify ground and excited states in finite bias transport. Significantly, we show that using a scanning tunnelling microscope, we can directly demonstrate that a ∼1 nm difference in interdot distance dramatically affects transport pathways between the three dots.

Atomistic modeling of metallic nanowires in silicon.

Scanning tunneling microscope (STM) lithography has recently demonstrated the ultimate in device scaling with buried, conducting nanowires just a few atoms wide and the realization of single atom transistors, where a single P atom has been placed inside a transistor architecture with atomic precision accuracy. Despite the dimensions of the critical parts of these devices being defined by a small number of P atoms, the device electronic properties are influenced by the surrounding 10(4) to 10(6) Si atoms. Such effects are hard to capture with most modeling approaches, and prior to this work no theory existed that could explore the realistic size of the complete device in which both dopant disorder and placement are important. This work presents a comprehensive study of the electronic and transport properties of ultra-thin (<10 nm wide) monolayer highly P δ-doped Si (Si:P) nanowires in a fully atomistic self-consistent tight-binding approach. This atomistic approach covering large device volumes allows for a systematic study of disorder on the physical properties of the nanowires. Excellent quantitative agreement is observed with recent resistance measurements of STM-patterned nanowires [Weber et al., Science, 2012, 335, 64], confirming the presence of metallic behavior at the scaling limit. At high doping densities the channel resistance is shown to be insensitive to the exact channel dopant placement highlighting their future use as metallic interconnects. This work presents the first theoretical study of Si:P nanowires that are realistically extended and disordered, providing a strong theoretical foundation for the design and understanding of atomic-scale electronics.

Engineering independent electrostatic control of atomic-scale (∼4 nm) silicon double quantum dots.

Scalable quantum computing architectures with electronic spin qubits hosted by arrays of single phosphorus donors in silicon require local electric and magnetic field control of individual qubits separated by ∼10 nm. This daunting task not only requires atomic-scale accuracy of single P donor positioning to control interqubit exchange interaction but also demands precision alignment of control electrodes with careful device design at these small length scales to minimize cross capacitive coupling. Here we demonstrate independent electrostatic control of two Si:P quantum dots, each consisting of ∼15 P donors, in an optimized device design fabricated by scanning tunneling microscope (STM)-based lithography. Despite the atomic-scale dimensions of the quantum dots and control electrodes reducing overall capacitive coupling, the electrostatic behavior of the device shows an excellent match to results of a priori capacitance calculations. These calculations highlight the importance of the interdot angle in achieving independent control at these length-scales. This combination of predictive electrostatic modeling and the atomic-scale fabrication accuracy of STM-lithography, provides a powerful tool for scaling multidonor dots to the single donor limit.

A single-atom transistor.

The ability to control matter at the atomic scale and build devices with atomic precision is central to nanotechnology. The scanning tunnelling microscope can manipulate individual atoms and molecules on surfaces, but the manipulation of silicon to make atomic-scale logic circuits has been hampered by the covalent nature of its bonds. Resist-based strategies have allowed the formation of atomic-scale structures on silicon surfaces, but the fabrication of working devices-such as transistors with extremely short gate lengths, spin-based quantum computers and solitary dopant optoelectronic devices-requires the ability to position individual atoms in a silicon crystal with atomic precision. Here, we use a combination of scanning tunnelling microscopy and hydrogen-resist lithography to demonstrate a single-atom transistor in which an individual phosphorus dopant atom has been deterministically placed within an epitaxial silicon device architecture with a spatial accuracy of one lattice site. The transistor operates at liquid helium temperatures, and millikelvin electron transport measurements confirm the presence of discrete quantum levels in the energy spectrum of the phosphorus atom. We find a charging energy that is close to the bulk value, previously only observed by optical spectroscopy.

Charge sensing of precisely positioned p donors in Si.

Real-time sensing of (spin-dependent) single-electron tunneling is fundamental to electrical readout of qubit states in spin quantum computing. Here, we demonstrate the feasibility of detecting such single-electron tunneling events using an atomically planar charge sensing layout, which can be readily integrated in scalable quantum computing architectures with phosphorus-donor-based spin qubits in silicon (Si:P). Using scanning tunneling microscopy (STM) lithography on a Si(001) surface, we patterned a single-electron transistor (SET), both tunnel and electrostatically coupled to a coplanar ultrasmall quantum dot, the latter consisting of approximately four P donors. Charge transitions of the quantum dot could be detected both in time-averaged and single-shot current response of the SET. Single electron tunneling between the quantum dot and the SET island on a time-scale (τ ∼ ms) two-orders-of-magnitude faster than the spin-lattice relaxation time of a P donor in Si makes this device geometry suitable for projective readout of Si:P spin qubits. Crucial to scalability is the ability to reproducibly achieve sufficient electron tunnel rates and charge sensitivity of the SET. The inherent atomic-scale control of STM lithography bodes extremely well to precisely optimize both of these parameters.