Demonstration of the Effectiveness of the Cascaded Variational Quantum Eigensolver Using the Jastrow Ansatz for Molecular Calculations.

We demonstrate how the cascaded variational quantum eigensolver (CVQE) can be applied to study molecular systems for the family of Jastrow ansatzes. Specifically, we applied CVQE to the water molecule. We find that CVQE has a number of advantages. In particular, our results show that CVQE requires 2 to 3 orders of magnitude fewer quantum computing (QC) executions than VQE for the water molecule. Furthermore, our results indicate that CVQE might provide some robustness against two-qubit gate errors given that the number of CNOT gates used in our calculation was ∼300 and the errors in the QC calculations are still comparable to those obtained by VQE.

Emergent Moiré Phonons Due to Zone Folding in WSe2-WS2 Van der Waals Heterostructures.

Bilayers of 2D materials offer opportunities for creating devices with tunable electronic, optical, and mechanical properties. In van der Waals heterostructures (vdWHs) where the constituent monolayers have different lattice constants, a moiré superlattice forms with a length scale larger than the lattice constant of either constituent material regardless of twist angle. Here, we report the appearance of moiré Raman modes from nearly aligned WSe2-WS2 vdWHs in the range of 240-260 cm-1, which are absent in both monolayers and homobilayers of WSe2 and WS2 and in largely misaligned WSe2-WS2 vdWHs. Using first-principles calculations and geometric arguments, we show that these moiré Raman modes are a consequence of the large moiré length scale, which results in zone-folded phonon modes that are Raman active. These modes are sensitive to changes in twist angle, but notably, they occur at identical frequencies for a given small twist angle away from either the 0-degree or 60-degree aligned heterostructure. Our measurements also show a strong Raman intensity modulation in the frequency range of interest, with near 0 and near 60-degree vdWHs exhibiting a markedly different dependence on excitation energy. In near 0-degree aligned WSe2-WS2 vdWHs, a nearly complete suppression of both the moiré Raman modes and the WSe2 A1g Raman mode (∼250 cm-1) is observed when exciting with a 532 nm CW laser at room temperature. Temperature-dependent reflectance contrast measurements demonstrate the significant Raman intensity modulation arises from resonant Raman effects.

Stacking-dependent optical properties in bilayer WSe2.

The twist angle between the monolayers in van der Waals heterostructures provides a new degree of freedom in tuning material properties. We compare the optical properties of WSe2 homobilayers with 2H and 3R stacking using photoluminescence, Raman spectroscopy, and reflectance contrast measurements under ambient and cryogenic temperatures. Clear stacking-dependent differences are evident for all temperatures, with both photoluminescence and reflectance contrast spectra exhibiting a blue shift in spectral features in 2H compared to 3R bilayers. Density functional theory (DFT) calculations elucidate the source of the variations and the fundamental differences between 2H and 3R stackings. DFT finds larger energies for both A and B excitonic features in 2H than in 3R, consistent with experimental results. In both stacking geometries, the intensity of the dominant A1g Raman mode exhibits significant changes as a function of laser excitation wavelength. These variations in intensity are intimately linked to the stacking- and temperature-dependent optical absorption through resonant enhancement effects. The strongest enhancement is achieved when the laser excitation coincides with the C excitonic feature, leading to the largest Raman intensity under 514 nm excitation in 2H stacking and at 520 nm in 3R stacked WSe2 bilayers.

Twist Angle-Dependent Atomic Reconstruction and Moiré Patterns in Transition Metal Dichalcogenide Heterostructures.

Van der Waals layered materials, such as transition metal dichalcogenides (TMDs), are an exciting class of materials with weak interlayer bonding, which enables one to create so-called van der Waals heterostructures (vdWH). One promising attribute of vdWH is the ability to rotate the layers at arbitrary azimuthal angles relative to one another. Recent work has shown that control of the twist angle between layers can have a dramatic effect on TMD vdWH properties, but the twist angle has been treated solely through the use of rigid-lattice moiré patterns. No atomic reconstruction, that is, any rearrangement of atoms within the individual layers, has been reported experimentally to date. Here, we demonstrate that vdWH of MoSe2/WSe2 and MoS2/WS2 at twist angles ≤1° undergo significant atomic level reconstruction leading to discrete commensurate domains divided by narrow domain walls, rather than a smoothly varying rigid-lattice moiré pattern as has been assumed in prior experimental work. Using conductive atomic force microscopy (CAFM), we show that TMD vdWH at small twist angles exhibit large domains of constant conductivity. The domains in samples with R-type stacking are triangular, whereas the domains in samples with H-type stacking are hexagonal. Transmission electron microscopy provides additional evidence of atomic reconstruction in MoSe2/WSe2 structures and demonstrates the transition between a rigid-lattice moiré pattern for large angles and atomic reconstruction for small angles. We use density functional theory to calculate the band structures of the commensurate reconstructed domains and find that the modulation of the relative electronic band edges is consistent with the CAFM results and photoluminescence spectra. The presence of atomic reconstruction in TMD heterostructures and the observed impact on nanometer-scale electronic properties provide fundamental insight into the behavior of this important class of heterostructures.

Nanoscale stacking fault-assisted room temperature plasticity in flash-sintered TiO2.

Ceramic materials have been widely used for structural applications. However, most ceramics have rather limited plasticity at low temperatures and fracture well before the onset of plastic yielding. The brittle nature of ceramics arises from the lack of dislocation activity and the need for high stress to nucleate dislocations. Here, we have investigated the deformability of TiO2 prepared by a flash-sintering technique. Our in situ studies show that the flash-sintered TiO2 can be compressed to ~10% strain under room temperature without noticeable crack formation. The room temperature plasticity in flash-sintered TiO2 is attributed to the formation of nanoscale stacking faults and nanotwins, which may be assisted by the high-density preexisting defects and oxygen vacancies introduced by the flash-sintering process. Distinct deformation behaviors have been observed in flash-sintered TiO2 deformed at different testing temperatures, ranging from room temperature to 600°C. Potential mechanisms that may render ductile ceramic materials are discussed.

Double Indirect Interlayer Exciton in a MoSe2/WSe2 van der Waals Heterostructure.

An emerging class of semiconductor heterostructures involves stacking discrete monolayers such as transition metal dichalcogenides (TMDs) to form van der Waals heterostructures. In these structures, it is possible to create interlayer excitons (ILEs), spatially indirect, bound electron-hole pairs with the electron in one TMD layer and the hole in an adjacent layer. We are able to clearly resolve two distinct emission peaks separated by 24 meV from an ILE in a MoSe2/WSe2 heterostructure fabricated using state-of-the-art preparation techniques. These peaks have nearly equal intensity, indicating they are of common character, and have opposite circular polarizations when excited with circularly polarized light. Ab initio calculations successfully account for these observations: they show that both emission features originate from excitonic transitions that are indirect in momentum space and are split by spin-orbit coupling. Also, the electron is strongly hybridized between both the MoSe2 and WSe2 layers, with significant weight in both layers, contrary to the commonly assumed model. Thus, the transitions are not purely interlayer in character. This work represents a significant advance in our understanding of the static and dynamic properties of TMD heterostructures.

Optical polarization of excitons and trions under continuous and pulsed excitation in single layers of WSe2.

The potential for valleytronic operation has stimulated much interest in studying polarized emission from transition metal dichalcogenides. In most studies, however, little regard is given to the character of laser excitation. We measure the circularly polarized photoluminescence of WSe2 monolayers as a function of excitation energy for both continuous-wave (cw) and pulsed laser excitation sources. Using cw excitation, the temperature dependence of the depolarization of the trion follows the same trend as that of the neutral exciton and involves collisional broadening. However, the polarization of the trion is nearly twice the polarization of the neutral exciton at low temperatures. When a pulsed laser with the same average fluence is used as the excitation source, the degrees of polarization become very similar, in stark contrast to the cw results. The difference in polarization behaviors is linked to the different amounts of energy deposited in the system during these measurements for similar average fluences. At a moderate fluence, pulsed excitation also has the potential to fundamentally alter the emission characteristics of WSe2.

Anomalous temperature-dependent spin-valley polarization in monolayer WS2.

Single layers of transition metal dichalcogenides (TMDs) are direct gap semiconductors with nondegenerate valley indices. An intriguing possibility for these materials is the use of their valley index as an alternate state variable. Several limitations to such a utility include strong intervalley scattering, as well as multiparticle interactions leading to multiple emission channels. We prepare single-layer WS2 films such that the photoluminescence is from either the neutral or charged exciton (trion). After excitation with circularly polarized light, the neutral exciton emission has zero polarization. However, the trion emission has a large polarization (28%) at room temperature. The trion emission also has a unique, non-monotonic temperature dependence that is a consequence of the multiparticle nature of the trion. This temperature dependence enables us to determine that intervalley scattering, electron-hole radiative recombination, and Auger processes are the dominant mechanisms at work in this system. Because this dependence involves trion systems, one can use gate voltages to modulate the polarization (or intensity) emitted from TMD structures.

Electron pairing without superconductivity.

Strontium titanate (SrTiO3) is the first and best known superconducting semiconductor. It exhibits an extremely low carrier density threshold for superconductivity, and possesses a phase diagram similar to that of high-temperature superconductors--two factors that suggest an unconventional pairing mechanism. Despite sustained interest for 50 years, direct experimental insight into the nature of electron pairing in SrTiO3 has remained elusive. Here we perform transport experiments with nanowire-based single-electron transistors at the interface between SrTiO3 and a thin layer of lanthanum aluminate, LaAlO3. Electrostatic gating reveals a series of two-electron conductance resonances-paired electron states--that bifurcate above a critical pairing field Bp of about 1-4 tesla, an order of magnitude larger than the superconducting critical magnetic field. For magnetic fields below Bp, these resonances are insensitive to the applied magnetic field; for fields in excess of Bp, the resonances exhibit a linear Zeeman-like energy splitting. Electron pairing is stable at temperatures as high as 900 millikelvin, well above the superconducting transition temperature (about 300 millikelvin). These experiments demonstrate the existence of a robust electronic phase in which electrons pair without forming a superconducting state. Key experimental signatures are captured by a model involving an attractive Hubbard interaction that describes real-space electron pairing as a precursor to superconductivity.

LaAlO3 stoichiometry is key to electron liquid formation at LaAlO3/SrTiO3 interfaces.

Emergent phenomena, including superconductivity and magnetism, found in the two-dimensional electron liquid (2-DEL) at the interface between the insulators lanthanum aluminate (LaAlO3) and strontium titanate (SrTiO3) distinguish this rich system from conventional 2D electron gases at compound semiconductor interfaces. The origin of this 2-DEL, however, is highly debated, with focus on the role of defects in the SrTiO3, while the LaAlO3 has been assumed perfect. Here we demonstrate, through experiments and first-principle calculations, that the cation stoichiometry of the nominal LaAlO3 layer is key to 2-DEL formation: only Al-rich LaAlO3 results in a 2-DEL. Although extrinsic defects, including oxygen deficiency, are known to render LaAlO3/SrTiO3 samples conducting, our results show that in the absence of such extrinsic defects an interface 2-DEL can form. Its origin is consistent with an intrinsic electronic reconstruction occurring to counteract a polarization catastrophe. This work provides insight for identifying other interfaces where emergent behaviours await discovery.

Efficiency of multiexciton generation in colloidal nanostructures.

Solar energy production, one of the world's most important unsolved problems, has the potential to be a source of clean, renewable energy if scientists can find a way of generating cheap and efficient solar cells. Generation of multiple excitons from single photons is one way to increase the efficiency of solar energy collection, but the process suffers from low efficiency in bulk materials. An increase of multiexciton generation efficiency in nanocrystals was proposed by Nozik in 2002 and demonstrated by Schaller and Klimov in 2004 in PbSe nanocrystals. Since then, scientists have observed efficient multiexciton generation in nanostructures made of many semiconductors using various measurement techniques. Although the experimental evidence of efficient carrier multiplication is overwhelming, there is no complete theory of this phenomenon. Researchers cannot develop such a theory without a self-consistent description of the Coulomb interaction and a knowledge of mechanisms of electron and hole thermalization in nanostructures. The full theoretical description requires the strength of the Coulomb interaction between exciton and multiexciton states and the thermalization rates, which both vary with the dimensionality of the confining potential. As a result, the efficiency of multiexciton generation depends strongly on the material and the shape of the nanostructure. In this Account, we discuss the theoretical aspects of efficient carrier multiplication in nanostructures. The Coulomb interaction couples single excitons with multiexciton states. Phenomenological many-electron calculations of the evolution of single-photon excitations have shown that efficient multiexciton generation can exist only if the rate of the Coulomb mixing between photo-created exciton and biexciton states is significantly faster than the rate of exciton relaxation. Therefore, to increase multiexciton generation efficiency, we need to either increase the exciton-biexciton mixing rate or suppress the exciton relaxation rate. Following this simple recipe, we show that multiexciton generation efficiency should be higher in semiconductor nanorods and nanoplatelets, which have stronger exciton-biexciton coupling due to the enhancement of the Coulomb interaction through the surrounding medium.

Structure of SrTiO3 films on Si.

The epitaxial deposition of oxides on silicon opens the possibility of incorporating their diverse properties into silicon-device technology. Deposition of SrTiO(3) on silicon was first reported over a decade ago, but growing the coherent, lattice-matched films that are critical for many applications has been difficult for thicknesses beyond 5 unit cells. Using a combination of density functional calculations and x-ray diffraction measurements, we determine the atomic structure of coherent SrTiO(3) films on silicon, finding that the Sr concentration at the interface varies with the film thickness. The structures with the lowest computed energies best match the x-ray diffraction. During growth, Sr diffuses from the interface to the surface of the film; the increasing difficulty of Sr diffusion with film thickness may cause the disorder seen in thicker films. The identification of this unique thickness-dependent interfacial structure opens the possibility of modifying the interface to improve the thickness and quality of metal oxide films on silicon.

Quantum simulation of multiple-exciton generation in a nanocrystal by a single photon.

We have shown theoretically that efficient multiple-exciton generation (MEG) by a single photon can be observed in small nanocrystals. Our quantum simulations that include hundreds of thousands of exciton and multiexciton states demonstrate that the complex time-dependent dynamics of these states in a closed electronic system yields a saturated MEG effect on a picosecond time scale. Including phonon relaxation confirms that efficient MEG requires the exciton-biexciton coupling time to be faster than exciton relaxation time.

Imaging the phase separation in atomically thin buried SrTiO(3) layers by electron channeling.

A phase-separation instability, resulting in the dewetting of thin SrTiO(3) films grown on Si(100) is shown by scanning transmission electron microscopy. Plan-view imaging of 1-nm thick, buried SrTiO(3) films was achieved by exploiting electron channeling through the substrate to focus the incident 0.2 nm beam down to a 0.04 nm diameter, revealing a nonuniform coverage by epitaxial SrTiO(3) islands and 2 x 1 Sr-covered regions. Density-functional calculations predict the ground state is a coexistence of 2 x 1 Sr-reconstructed Si and Sr-deficient SrTiO(3), in correspondence with the observed islanding.

Scalable architecture for coherence-preserving qubits.

We propose scalable architectures for the coherence-preserving qubits introduced by Bacon, Brown, and Whaley [Phys. Rev. Lett. 87, 247902 (2001)]. These architectures employ extra qubits providing additional degrees of freedom to the system. These extra degrees of freedom can be used to counter coupling strength errors within the coherence-preserving qubit and combat interactions with environmental qubits. Importantly, these architectures provide flexibility in qubit arrangement, allowing all physical qubits to be arranged in two spatial dimensions.

Entanglement generation of nearly random operators.

We study the entanglement generation of operators whose statistical properties approach those of random matrices but are restricted in some way. These include interpolating ensemble matrices, where the interval of the independent random parameters are restricted, pseudorandom operators, where there are far fewer random parameters than required for random matrices, and quantum chaotic evolution. Restricting randomness in different ways allows us to probe connections between entanglement and randomness. We comment on which properties affect entanglement generation and discuss ways of efficiently producing random states on a quantum computer.

Effects of symmetries on quantum fidelity decay.

We explore the effect of a system's symmetries on fidelity decay behavior. Chaoslike exponential fidelity decay behavior occurs in nonchaotic systems when the system possesses symmetries and the applied perturbation is not tied to a classical parameter. Similar systems without symmetries exhibit faster-than-exponential decay under the same type of perturbation. This counterintuitive result, that extra symmetries cause the system to behave in a chaotic fashion, may have important ramifications for quantum-error correction.

Quantum fidelity decay in quasi-integrable systems.

We show, via numerical simulations, that the fidelity decay behavior of quasi-integrable systems is strongly dependent on the location of the initial coherent state with respect to the underlying classical phase space. In parallel to classical fidelity, the quantum fidelity generally exhibits Gaussian decay when the perturbation affects the frequency of periodic phase space orbits and power-law decay when the perturbation changes the shape of the orbits. For both behaviors the decay rate also depends on initial state location. The spectrum of the initial states in the eigenbasis of the system reflects the different fidelity decay behaviors. In addition, states with initial Gaussian decay exhibit a stage of exponential decay for strong perturbations. This elicits a surprising phenomenon: a strong perturbation can induce a higher fidelity than a weak perturbation of the same type.