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We demonstrate nearly a microsecond of spin coherence in Er3+ ions doped in cerium dioxide nanocrystal hosts, despite a large gyromagnetic ratio and nanometric proximity of the spin defect to the nanocrystal surface. The long spin coherence is enabled by reducing the dopant density below the instantaneous diffusion limit in a nuclear spin-free host material, reaching the limit of a single erbium spin defect per nanocrystal. We observe a large Orbach energy in a highly symmetric cubic site, further protecting the coherence in a qubit that would otherwise rapidly decohere. Spatially correlated electron spectroscopy measurements reveal the presence of Ce3+ at the nanocrystal surface that likely acts as extraneous paramagnetic spin noise. Even with these factors, defect-embedded nanocrystal hosts show tremendous promise for quantum sensing and quantum communication applications, with multiple avenues, including core-shell fabrication, redox tuning of oxygen vacancies, and organic surfactant modification, available to further enhance their spin coherence and functionality in the future.

Since dissipative processes are ubiquitous in semiconductors, characterizing how electronic and thermal energy transduce and transport at the nanoscale is vital for understanding and leveraging their fundamental properties. For example, in low-dimensional transition metal dichalcogenides (TMDCs), excess heat generation upon photoexcitation is difficult to avoid since even with modest injected exciton densities, exciton-exciton annihilation still occurs. Both heat and photoexcited electronic species imprint transient changes in the optical response of a semiconductor, yet the unique signatures of each are difficult to disentangle in typical spectra due to overlapping resonances. In response, we employ stroboscopic optical scattering microscopy (stroboSCAT) to simultaneously map both heat and exciton populations in few-layer \chMoS2 on relevant nanometer and picosecond length- and time scales and with 100-mK temperature sensitivity. We discern excitonic contributions to the signal from heat by combining observations close to and far from exciton resonances, characterizing photoinduced dynamics for each. Our approach is general and can be applied to any electronic material, including thermoelectrics, where heat and electronic observables spatially interplay, and lays the groundwork for direct and quantitative discernment of different types of coexisting energy without recourse to complex models or underlying assumptions.

Monolayer transition metal dichalcogenide (TMDC) semiconductors exhibit strong excitonic optical resonances which serve as a microscopic, non-invasive probe into their fundamental properties. Like the hydrogen atom, such excitons can exhibit an entire Rydberg series of resonances. Excitons have been extensively studied in most TMDCs (MoS$_2$, MoSe$_2$, WS$_2$ and WSe$_2$), but detailed exploration of excitonic phenomena has been lacking in the important TMDC material molybdenum ditelluride (MoTe$_2$). Here, we report an experimental investigation of excitonic luminescence properties of monolayer MoTe$_2$ to understand the excitonic Rydberg series, up to 3s. We report significant modification of emission energies with temperature (4K to 300K), quantifying the exciton-phonon coupling. Furthermore, we observe a strongly gate-tunable exciton-trion interplay for all the Rydberg states governed mainly by free-carrier screening, Pauli blocking, and band-gap renormalization in agreement with the results of first-principles GW plus Bethe-Salpeter equation approach calculations. Our results help bring monolayer MoTe$_2$ closer to its potential applications in near-infrared optoelectronics and photonic devices.

Topological Hall effect (THE), an electrical transport signature of systems with chiral spin textures like skyrmions, has been observed recently in topological insulator (TI)-based magnetic heterostructures. However, the intriguing interplay between the topological surface state and THE is yet to be fully understood. In this work, we report a large THE of ~10 ohm (~4 micro-ohm*cm) at 2 K with an electrically reversible sign in a top-gated 4 nm TI (Bi0.3Sb0.7)2Te3 (BST) grown on a ferrimagnetic insulator (FI) europium iron garnet (EuIG). Temperature, external magnetic field angle, and top gate bias dependences of magnetotransport properties were investigated and consistent with a skyrmion-driven THE. Most importantly, a sign change in THE was discovered as the Fermi level was tuned from the upper to the lower parts of the gapped Dirac cone and vice versa. This discovery is anticipated to impact technological applications in ultralow power skyrmion-based spintronics.

Color centered-based single photon emitters in hexagonal boron nitride (h-BN) have shown promising photophysical properties as sources for quantum light emission. Despite significant advances towards such a goal, achieving lifetime-limited quantum light emission in h-BN has proven to be challenging, primarily due to various broadening mechanisms including spectral diffusion. Here, we propose and experimentally demonstrate suppression of spectral diffusion by applying an electrostatic field. We observe both Stark shift tuning of the resonant emission wavelength, and emission linewidth reduction nearly to the homogeneously broadened lifetime limit. Lastly, we find a cubic dependence of the linewidth with respect to temperature at the homogeneous broadening regime. Our results suggest that field tuning in electrostatically gated heterostructures is promising as an approach to control the emission characteristics of h-BN color centers, removing spectral diffusion and providing the energy tunability necessary for integrate of quantum light emission in nanophotonic architectures.

Strain is extensively used to controllably tailor the electronic properties of materials. In the context of indirect band-gap semiconductors such as silicon, strain lifts the valley degeneracy of the six conduction band minima, and by extension the valley states of electrons bound to phosphorus donors. Here, single phosphorus atoms are embedded in an engineered thin layer of silicon strained to 0.8% and their wave function imaged using spatially resolved spectroscopy. A prevalence of the out-of-plane valleys is confirmed from the real-space images, and a combination of theoretical modelling tools is used to assess how this valley repopulation effect can yield isotropic exchange and tunnel interactions in the $xy$-plane relevant for atomically precise donor qubit devices. Finally, the residual presence of in-plane valleys is evidenced by a Fourier analysis of both experimental and theoretical images, and atomistic calculations highlight the importance of higher orbital excited states to obtain a precise relationship between valley population and strain. Controlling the valley degree of freedom in engineered strained epilayers provides a new competitive asset for the development of donor-based quantum technologies in silicon.

Specialized applications of nanoparticles often call for particular, well-characterized particle size distributions in solution. But, this property can prove difficult to measure. High-throughput methods, such as dynamic light scattering, detect nanoparticles in solution with an efficiency that scales with diameter to the sixth power. This diminishes the accuracy of any determination that must span a range of particle sizes. The accurate classification of broadly distributed systems thus requires very large numbers of measurements. Mass-filtered particle-sensing techniques offer a better dynamic range, but are labor-intensive and so have low throughput. Progress in many areas of nanotechnology requires a faster, lower-cost, and more accurate measure of particle size distributions, particularly for diameters smaller than 20 nm. Here, we present a tailored interferometric microscope system, combined with a high-speed image-processing strategy, optimized for real-time particle tracking that determines accurate size distributions in nominal 5, 10, and 15 nm colloidal gold nanoparticle systems by automatically sensing and classifying thousands of single particles sampled from solution at rates as high as 4,000 particles per minute. We demonstrate this method by sensing the irreversible binding of gold nanoparticles to poly-D-lysine functionalized coverslips. Variations in the single-particle signal as a function of time and mass, calibrated by TEM, show clear evidence for the presence of diffusion-limited transport that most affects larger particles in solution.

To realize the quantum anomalous Hall effect (QAHE) at elevated temperatures, the approach of magnetic proximity effect (MPE) was adopted to break the time-reversal symmetry in the topological insulator (Bi0.3Sb0.7)2Te3 (BST) based heterostructures with a ferrimagnetic insulator europium iron garnet (EuIG) of perpendicular magnetic anisotropy. Here we demonstrate phenomenally large anomalous Hall resistance (RAHE) exceeding 8 \Omega (h̊oAHE of 3.2 \mu\Omega*cm) at 300 K and sustaining to 400 K in 35 BST/EuIG samples, surpassing the past record of 0.28 \Omega (h̊oAHE of 0.14 \mu\Omega*cm) at 300 K. The remarkably large RAHE as attributed to an atomically abrupt, Fe-rich interface between BST and EuIG. Importantly, the gate dependence of the AHE loops shows no sign change with varying chemical potential. This observation is supported by our first-principles calculations via applying a gradient Zeeman field plus a contact potential on BST. Our calculations further demonstrate that the AHE in this heterostructure is attributed to the intrinsic Berry curvature. Furthermore, for gate-biased 4 nm BST on EuIG, a pronounced topological Hall effect (THE) coexisting with AHE is observed at the negative top-gate voltage up to 15 K. Interface tuning with theoretical calculations has opened up new opportunities to realize topologically distinct phenomena in tailored magnetic TI-based heterostructures.

The theoretical maximum efficiency of a solar cell is typically characterized by a detailed balance of optical absorption and emission for a semiconductor in the limit of unity radiative efficiency and an ideal step-function response for the density of states and absorbance at the semiconductor band edges, known as the Shockley-Queisser limit. However, real materials have non-abrupt band edges, which are typically characterized by an exponential distribution of states, known as an Urbach tail. We develop here a modified detailed balance limit of solar cells with imperfect band edges, using optoelectronic reciprocity relations. We find that for semiconductors whose band edges are broader than the thermal energy, kT, there is an effective renormalized bandgap given by the quasi-Fermi level splitting within the solar cell. This renormalized bandgap creates a Stokes shift between the onset of the absorption and photoluminescence emission energies, which significantly reduces the maximum achievable efficiency. The abruptness of the band edge density of states therefore has important implications for the maximum achievable photovoltaic efficiency.

Van der Waals materials exhibit naturally passivated surfaces and can form versatile heterostructures, enabling observation of carrier transport mechanisms not seen in three-dimensional materials. Here we report observation of a "band bending junction", a new type of semiconductor homojunction whose surface potential landscape depends solely on a difference in thickness between the two semiconductor regions atop a buried heterojunction interface. Using MoS2 on Au to form a buried heterojunction interface, we find that lateral surface potential differences can arise in MoS2 from the local extent of vertical band bending in thin and thick MoS2 regions. Using scanning ultrafast electron microscopy, we examine the spatiotemporal dynamics of photogenerated charge carriers and find that lateral carrier separation is enabled by a band bending junction, which is confirmed with semiconductor transport simulations. Band bending junctions may therefore enable new electronic and optoelectronic devices in Van der Waals materials that rely on thickness variations rather than doping to separate charge carriers.

Half of the energy is always lost when charging a capacitor. Even in the limit of vanishing resistance, half of the charging energy is still lost--to radiation instead of heat. While this fraction can technically be reduced by charging adiabatically, it otherwise places a fundamental limit on the charging efficiency of a capacitor. Here we show that this 1/2 limit can be broken by coupling a ferroelectric to the capacitor dielectric. Maxwell's equations are solved for the coupled system to analyze energy flow from the perspective of Poynting's theorem and show that (1) total energy dissipation is reduced below the fundamental limit during charging and discharging; (2) energy is saved by "recycling" the energy already stored in the ferroelectric phase transition; and (3) this phase transition energy is directly transferred between the ferroelectric and dielectric during charging and discharging. These results demystify recent works on low energy negative capacitance devices as well as lay the foundation for improving fundamental energy efficiency in all devices that rely on energy storage in electric fields.

Two-dimensional (2D) semiconductors provide a unique opportunity for optoelectronics due to their layered atomic structure, electronic and optical properties. To date, a majority of the application-oriented research in this field has been focused on field-effect electronics as well as photodetectors and light emitting diodes. Here we present a perspective on the use of 2D semiconductors for photovoltaic applications. We discuss photonic device designs that enable light trapping in nanometer-thickness absorber layers, and we also outline schemes for efficient carrier transport and collection. We further provide theoretical estimates of efficiency indicating that 2D semiconductors can indeed be competitive with and complementary to conventional photovoltaics, based on favorable energy bandgap, absorption, external radiative efficiency, along with recent experimental demonstrations. Photonic and electronic design of 2D semiconductor photovoltaics represents a new direction for realizing ultrathin, efficient solar cells with applications ranging from conventional power generation to portable and ultralight solar power.

The incorporation of electrically tunable materials into photonic structures such as waveguides and metasurfaces enables dynamic control of light propagation by an applied potential. While many materials have been shown to exhibit electrically tunable permittivity and dispersion, including transparent conducting oxides (TCOs) and III-V semiconductors and quantum wells, these materials are all optically isotropic in the propagation plane. In this work, we report the first known example of electrically tunable linear dichroism, observed here in few-layer black phosphorus (BP), which is a promising candidate for multi-functional, broadband, tunable photonic elements. We measure active modulation of the linear dichroism from the mid-infrared to visible frequency range, which is driven by anisotropic quantum-confined Stark and Burstein-Moss effects, and field-induced forbidden-to-allowed optical transitions. Moreover, we observe high BP absorption modulation strengths, approaching unity for certain thicknesses and photon energies.

We report experimental measurements for ultrathin (< 15 nm) van der Waals heterostructures exhibiting external quantum efficiencies exceeding 50%, and show that these structures can achieve experimental absorbance > 90%. By coupling electromagnetic simulations and experimental measurements, we show that pn WSe2/MoS2 heterojunctions with vertical carrier collection can have internal photocarrier collection efficiencies exceeding 70%.

We demonstrate an electrically induced, non-volatile, metal-insulator phase transition in a MoS$_2$ transistor. A single crystalline, epitaxially grown, PbZr$_{0.2}$Ti$_{0.8}$O$_3$ (PZT) was placed in the gate of a field effect transistor made of thin film MoS$_2$. When a gate voltage is applied to this ferroelectric gated transistor, a clear transition from insulator to metal and vice versa is observed. Importantly, when the gate voltage is turned off, the remnant polarization in the ferroelectric can keep the MoS$_2$ in its original phase, thereby providing a non-volatile state. Thus a metallic or insulating phase can be written, erased or retained simply by applying a gate voltage to the transistor.

We demonstrate non-volatile, n-type, back-gated, MoS$_{2}$ transistors, placed directly on an epitaxial grown, single crystalline, PbZr$_{0.2}$Ti$_{0.8}$O$_{3}$ (PZT) ferroelectric. The transistors show decent ON current (19 ${\mu}A/{\mu}$m), high on-off ratio (10$^{7}$), and a subthreshold swing of (SS ~ 92 mV/dec) with a 100 nm thick PZT layer as the back gate oxide. Importantly, the ferroelectric polarization can directly control the channel charge, showing a clear anti-clockwise hysteresis. We have selfconsistently confirmed the switching of the ferroelectric and corresponding change in channel current from a direct time-dependent measurement. Our results demonstrate that it is possible to obtain transistor operation directly on polar surfaces and therefore it should be possible to integrate 2D electronics with single crystalline functional oxides.

Nanoscale CoFeB amorphous films have been synthesized on GaAs(100) and studied with X-ray magnetic circular dichroism (XMCD) and transmission electron microscopy (TEM). We have found that the ratios of the orbital to spin magnetic moments of both the Co and Fe in the ultrathin amorphous film have been enhanced by more than 300% compared with those of the bulk crystalline Co and Fe, and in specifically, a large orbital moment of 0.56*10^-6 B from the Co atoms has been observed and at the same time the spin moment of the Co atoms remains comparable to that of the bulk hcp Co. The results indicate that the large uniaxial magnetic anisotropy (UMA) observed in the ultrathin CoFeB film on GaAs(100) is related to the enhanced spin-orbital coupling of the Co atoms in the CoFeB. This work offers experimental evidences of the correlation between the UMA and the elementary specific spin and orbital moments in the CoFeB amorphous film on the GaAs(100) substrate, which is significant for spintronics applications.

We demonstrate near unity, broadband absorbing optoelectronic devices using sub-15 nm thick transition metal dichalcogenides (TMDCs) of molybdenum and tungsten as van der Waals semiconductor active layers. Specifically, we report that near-unity light absorption is possible in extremely thin (< 15 nm) Van der Waals semiconductor structures by coupling to strongly damped optical modes of semiconductor/metal heterostructures. We further fabricate Schottky junction devices using these highly absorbing heterostructures and characterize their optoelectronic performance. Our work addresses one of the key criteria to enable TMDCs as potential candidates to achieve high optoelectronic efficiency.

Magnetism in graphene is an emerging field that has received much theoretical attention. In particular, there have been exciting predictions for induced magnetism through proximity to a ferromagnetic insulator as well as through localized dopants and defects. Here, we discuss our experimental work using molecular beam epitaxy (MBE) to modify the surface of graphene and induce novel spin-dependent phenomena. First, we investigate the epitaxial growth the ferromagnetic insulator EuO on graphene and discuss possible scenarios for realizing exchange splitting and exchange fields by ferromagnetic insulators. Second, we investigate the properties of magnetic moments in graphene originating from localized p_z-orbital defects (i.e. adsorbed hydrogen atoms). The behavior of these magnetic moments is studied using non-local spin transport to directly probe the spin-degree of freedom of the defect-induced states. We also report the presence of enhanced electron g-factors caused by the exchange fields present in the system. Importantly, the exchange field is found to be highly gate dependent, with decreasing g-factors with increasing carrier densities.

We investigate the initial growth modes and the role of interfacial electrostatic interactions of EuO epitaxy on MgO(001) by reactive molecular beam epitaxy. A TiO2 interfacial layer is employed to produce high quality epitaxial growth of EuO on MgO(001) with a 45\deg in plane rotation. For comparison, direct deposition of EuO on MgO, without the TiO2 layer shows a much slower time evolution in producing a single crystal film. Conceptual arguments of electrostatic repulsion of like-ions are introduced to explain the increased EuO quality at the interface with the TiO2 layer. It is shown that ultrathin EuO films in the monolayer regime can be produced on the TiO2 surface by substrate-supplied oxidation and that such films have bulk-like magnetic properties.

We incorporate single crystal Fe$_3$O$_4$ thin films into a gated device structure and demonstrate the ability to control the Verwey transition with static electric fields. The Verwey transition temperature ($T_V$) increases for both polarities of the electric field, indicating the effect is not driven by changes in carrier concentration. Energetics of induced electric polarization and/or strain within the Fe$_3$O$_4$ film provide a possible explanation for this behavior. Electric field control of the Verwey transition leads directly to a large magnetoelectric effect with coefficient of 585 pT m/V.

The spin dependent properties of epitaxial Fe3O4 thin films on GaAs(001) are studied by the ferromagnetic proximity polarization (FPP) effect and magneto-optic Kerr effect (MOKE). Both FPP and MOKE show oscillations with respect to Fe3O4 film thickness, and the oscillations are large enough to induce repeated sign reversals. We attribute the oscillatory behavior to spin-polarized quantum well states forming in the Fe3O4 film. Quantum confinement of the t2g states near the Fermi level provides an explanation for the similar thickness dependences of the FPP and MOKE oscillations.

We achieve tunneling spin injection from Co into single layer graphene (SLG) using TiO2 seeded MgO barriers. A non-local magnetoresistance (∆RNL) of 130 \Omega is observed at room temperature, which is the largest value observed in any material. Investigating ∆RNL vs. SLG conductivity from the transparent to the tunneling contact regimes demonstrates the contrasting behaviors predicted by the drift-diffusion theory of spin transport. Furthermore, tunnel barriers reduce the contact-induced spin relaxation and are therefore important for future investigations of spin relaxation in graphene.

We demonstrate the epitaxial growth of EuO on GaAs by reactive molecular beam epitaxy. Thin films are grown in an adsorption-controlled regime with the aid of an MgO diffusion barrier. Despite the large lattice mismatch, it is shown that EuO grows well on MgO(001) with excellent magnetic properties. Epitaxy on GaAs is cube-on-cube and longitudinal magneto-optic Kerr effect measurements demonstrate a large Kerr rotation of 0.57\deg, a significant remanent magnetization, and a Curie temperature of 69 K.

We achieve tunneling spin injection from Co into single layer graphene (SLG) using TiO2 seeded MgO barriers. A non-local magnetoresistance (∆RNL) of 130 \Omega is observed at room temperature, which is the largest value observed in any material. Investigating ∆RNL vs. SLG conductivity from the transparent to the tunneling contact regimes demonstrates the contrasting behaviors predicted by the drift-diffusion theory of spin transport. Furthermore, tunnel barriers reduce the contact-induced spin relaxation and are therefore important for future investigations of spin relaxation in graphene.

We investigate the interlayer exchange coupling in Fe/MgO/Fe and Fe/MgO/Co systems with magnetic Fe nanoclusters embedded in the MgO spacer. Samples are grown by molecular beam epitaxy (MBE) and utilize wedged MgO films to independently vary the film thickness and the position of the Fe nanoclusters. Depending on the position of the Fe nanoclusters, the bilinear coupling (J1) exhibits strong variations in magnitude and can even switch between antiferromagnetic and ferromagnetic. This effect is explained by the magnetic coupling between the ferromagnetic films and the magnetic nanoclusters. Interestingly, the coupling of Fe nanoclusters to a Co film is 160% stronger than their coupling to a Fe film (at MgO spacing of 0.56 nm). This is much greater than the coupling difference of 20% observed in the analogous thin film systems (i.e. Fe/MgO/Co vs. Fe/MgO/Fe), identifying an interesting nano-scaling effect related to the coupling between films and nanoclusters.

Magnetic configurations in heterostructures are often difficult to probe when the magnetic entities are buried inside. In this study we have captured magnetic and magnetoresistance "fingerprints" of Co nanodiscs embedded in Co/Cu multilayered nanowires using a first-order reversal curve method. In 200nm diameter nanowires, the magnetic configurations can be tuned by adjusting the Co nanodisc aspect ratio. Nanowires with the thinnest Co nanodiscs exhibit single domain behavior, while those with thicker Co reverse via vortex states. A superposition of giant and anisotropic magnetoresistance is observed, which corresponds to the different magnetic configurations of the Co nanodiscs.

B and N K-edge x-ray absorption spectroscopy measurements have been performed on three BN thin films grown on Si substrates using ion-assisted pulsed laser deposition. Comparison of the films' spectra to those of several single-phase BN powder standards shows that the films consist primarily of $sp^2$ bonds. Other features in the films' spectra suggest the presence of secondary phases, possibly cubic or rhombohedral BN. Films grown at higher deposition rates and higher ion-beam voltages are found to be more disordered, in agreement with previous work.