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Since the first realization of borophene on Ag(111), two-dimensional (2D) boron nanomaterials have attracted significant interest due to their polymorphic diversity and potential for hosting solid-state quantum phenomena. Here, we use atomic-resolution scanning tunneling microscopy (STM) and field-emission resonance (FER) spectroscopy to elucidate the structure and properties of atomically thin boron phases grown on Cu(111). Specifically, FER spectroscopy reveals unique charge transfer and electronic states compared to the distinct borophene phases observed on silver, suggesting that the deposition of boron on copper can result in strong covalent bonding characteristic of a 2D copper boride. This conclusion is reinforced by detailed STM characterization of line defects that are consistent with density functional theory (DFT) calculations for atomically thin Cu8B14. This evidence for 2D copper boride is likely to motivate future synthetic efforts aimed at expanding the relatively unexplored family of atomically thin metal boride materials., Comment: 19 pages including supplementary information, 4 main figures

Understanding the mechanism of single photon emission (SPE) in two-dimensional (2D) materials is an unsolved problem important for quantum optical materials and the development of quantum information applications. In 2D transition metal dichalcogenides (TMDs) such as tungsten diselenide (WSe$_2$), quantum emission has been broadly attributed to exciton localization from atomic point defects, yet the precise microscopic picture is not fully understood. This work presents a new framework, supported by both computational and experimental evidence, to explain both the origins of facile SPE in WSe2 and the relative scarcity of SPE in the related 2D TMD, tungsten disulfide (WS$_2$). A vertical divacancy configuration of selenium creates a defect-centered, direct energy gap in the band structure of WSe2, giving rise to highly localized, radiative transitions. This configuration is shown to be energetically preferred in the monolayer lattice, which is reflected in the abundant experimental observation of SPE in WSe2 both from the literature and this work. In contrast, the same vertical divacancy configuration in WS2 does not create direct localized transitions, consistent with scarce observations of SPE in that material. By revealing a single mechanism in tungsten-based TMDs that addresses the prevalence of SPE and is consistent between theory and experiment, these results provide a framework for better understanding the rules governing the atomic origins of single photon emission in TMDs., Comment: 14 pages, 11 figures

As particle physics experiments evolve to achieve higher energies and resolutions, handling the massive data volumes produced by silicon pixel detectors, which are used for charged particle tracking, poses a significant challenge. To address the challenge of data transport from high resolution tracking systems, we investigate a support vector machine (SVM)-based data classification system designed to reject low-momentum particles in real-time. This SVM system achieves high accuracy through the use of a customized mixed kernel function, which is specifically adapted to the data recorded by a silicon tracker. Moreover, this custom kernel can be implemented using highly efficient, novel van der Waals heterojunction devices. This study demonstrates the co-design of circuits with applications that may be adapted to meet future device and processing needs in high-energy physics (HEP) collider experiments., Comment: 15 pages, 8 figures, 1 table

The performance of superconducting qubits is often limited by dissipation and two-level systems (TLS) losses. The dominant sources of these losses are believed to originate from amorphous materials and defects at interfaces and surfaces, likely as a result of fabrication processes or ambient exposure. Here, we explore a novel wet chemical surface treatment at the Josephson junction-substrate and the substrate-air interfaces by replacing a buffered oxide etch (BOE) cleaning process with one that uses hydrofluoric acid followed by aqueous ammonium fluoride. We show that the ammonium fluoride etch process results in a statistically significant improvement in median $\text{T}_1$ by $\sim22\%$ ($p=0.002$), and a reduction in the number of strongly-coupled TLS in the tunable frequency range. Microwave resonator measurements on samples treated with the ammonium fluoride etch prior to niobium deposition also show $\sim33\%$ lower TLS-induced loss tangent compared to the BOE treated samples. As the chemical treatment primarily modifies the Josephson junction-substrate interface and substrate-air interface, we perform targeted chemical and structural characterizations to examine materials' differences at these interfaces and identify multiple microscopic changes that could contribute to decreased TLS.

Support Vector Machine (SVM) is a state-of-the-art classification method widely used in science and engineering due to its high accuracy, its ability to deal with high dimensional data, and its flexibility in modeling diverse sources of data. In this paper, we propose an autotuning-based optimization framework to quantify the ranges of hyperparameters in SVMs to identify their optimal choices, and apply the framework to two SVMs with the mixed-kernel between Sigmoid and Gaussian kernels for smart pixel datasets in high energy physics (HEP) and mixed-kernel heterojunction transistors (MKH). Our experimental results show that the optimal selection of hyperparameters in the SVMs and the kernels greatly varies for different applications and datasets, and choosing their optimal choices is critical for a high classification accuracy of the mixed kernel SVMs. Uninformed choices of hyperparameters C and coef0 in the mixed-kernel SVMs result in severely low accuracy, and the proposed framework effectively quantifies the proper ranges for the hyperparameters in the SVMs to identify their optimal choices to achieve the highest accuracy 94.6\% for the HEP application and the highest average accuracy 97.2\% with far less tuning time for the MKH application., Comment: presented in SC24 Workshop on Extreme-Scale Experiment-in-the-Loop Computing (XLOOP2024)

Superconducting Nb thin films have recently attracted significant attention due to their utility for quantum information technologies. In the processing of Nb thin films, fluoride-based chemical etchants are commonly used to remove surface oxides that are known to affect superconducting quantum devices adversely. However, these same etchants can also introduce hydrogen to form Nb hydrides, potentially negatively impacting microwave loss performance. Here, we present comprehensive materials characterization of Nb hydrides formed in Nb thin films as a function of fluoride chemical treatments. In particular, secondary-ion mass spectrometry, X-ray scattering, and transmission electron microscopy reveal the spatial distribution and phase transformation of Nb hydrides. The rate of hydride formation is determined by the fluoride solution acidity and the etch rate of Nb2O5, which acts as a diffusion barrier for hydrogen into Nb. The resulting Nb hydrides are detrimental to Nb superconducting properties and lead to increased power-independent microwave loss in coplanar waveguide resonators. However, Nb hydrides do not correlate with two-level system loss or device aging mechanisms. Overall, this work provides insight into the formation of Nb hydrides and their role in microwave loss, thus guiding ongoing efforts to maximize coherence time in superconducting quantum devices.

Detecting electronic hot spots is important for understanding the heat dissipation and thermal management of electronic and semiconductor devices. Optical thermoreflective imaging is being used to perform precise temporal and spatial imaging of heat on wires and semiconductor materials. We apply quantum squeezed light to perform thermoreflective imaging on micro-wires, surpassing the shot-noise limit of classical approaches. We obtain a far-field temperature sensing accuracy of 42 mK after 50 ms of averaging and show that a $256\times256$ pixel image can be constructed with such sensitivity in 10 minutes. We can further obtain single-shot temperature sensing of 1.6 K after only 10 $\mathrm{\mu s}$ of averaging enabling dynamical study of heat dissipation. Not only do the quantum images provide accurate spatio-temporal information about heat distribution, but the measure of quantum correlation provides additional information, inaccessible by classical techniques, that can lead to a better understanding of the dynamics. We apply the technique to both Al and Nb microwires and discuss the applications of the technique in studying electron dynamics at low temperatures.

Antiferromagnetic (AFM) materials are a pathway to spintronic memory and computing devices with unprecedented speed, energy efficiency, and bit density. Realizing this potential requires AFM devices with simultaneous electrical writing and reading of information, which are also compatible with established silicon-based manufacturing. Recent experiments have shown tunneling magnetoresistance (TMR) readout in epitaxial AFM tunnel junctions. However, these TMR structures were not grown using a silicon-compatible deposition process, and controlling their AFM order required external magnetic fields. Here we show three-terminal AFM tunnel junctions based on the noncollinear antiferromagnet PtMn3, sputter-deposited on silicon. The devices simultaneously exhibit electrical switching using electric currents, and electrical readout by a large room-temperature TMR effect. First-principles calculations explain the TMR in terms of the momentum-resolved spin-dependent tunneling conduction in tunnel junctions with noncollinear AFM electrodes.

In the "Beyond Moore's Law" era, with increasing edge intelligence, domain-specific computing embracing unconventional approaches will become increasingly prevalent. At the same time, adopting a variety of nanotechnologies will offer benefits in energy cost, computational speed, reduced footprint, cyber resilience, and processing power. The time is ripe for a roadmap for unconventional computing with nanotechnologies to guide future research, and this collection aims to fill that need. The authors provide a comprehensive roadmap for neuromorphic computing using electron spins, memristive devices, two-dimensional nanomaterials, nanomagnets, and various dynamical systems. They also address other paradigms such as Ising machines, Bayesian inference engines, probabilistic computing with p-bits, processing in memory, quantum memories and algorithms, computing with skyrmions and spin waves, and brain-inspired computing for incremental learning and problem-solving in severely resource-constrained environments. These approaches have advantages over traditional Boolean computing based on von Neumann architecture. As the computational requirements for artificial intelligence grow 50 times faster than Moore's Law for electronics, more unconventional approaches to computing and signal processing will appear on the horizon, and this roadmap will help identify future needs and challenges. In a very fertile field, experts in the field aim to present some of the dominant and most promising technologies for unconventional computing that will be around for some time to come. Within a holistic approach, the goal is to provide pathways for solidifying the field and guiding future impactful discoveries., Comment: 80 pages accepted in Nano Futures

Optical control of spin in semiconductors has been pioneered using nanostructures of III-V and II-VI semiconductors, but the emergence of two-dimensional van der Waals materials offers an alternative low-dimensional platform for spintronic phenomena. Indium selenide (InSe), a group-III monochalcogenide van der Waals material, has shown promise for opto-electronics due to its high electron mobility, tunable direct bandgap, and quantum transport. There are predictions of spin-dependent optical selection rules suggesting potential for all-optical excitation and control of spin in a two-dimensional layered material. Despite these predictions, layer-dependent optical spin phenomena in InSe have yet to be explored. Here, we present measurements of layer-dependent optical spin dynamics in few-layer and bulk InSe. Polarized photoluminescence reveals layer-dependent optical orientation of spin, thereby demonstrating the optical selection rules in few-layer InSe. Spin dynamics are also studied in many-layer InSe using time-resolved Kerr rotation spectroscopy. By applying out-of-plane and in-plane static magnetic fields for polarized emission measurements and Kerr measurements, respectively, the $g$-factor for InSe was extracted. Further investigations are done by calculating precession values using a $\textbf{k} \cdot \textbf{p}$ model, which is supported by \textit{ab-initio} density functional theory. Comparison of predicted precession rates with experimental measurements highlights the importance of excitonic effects in InSe for understanding spin dynamics. Optical orientation of spin is an important prerequisite for opto-spintronic phenomena and devices, and these first demonstrations of layer-dependent optical excitation of spins in InSe lay the foundation for combining layer-dependent spin properties with advantageous electronic properties found in this material., Comment: 11 pages, 6 figures, supplemental material

Continued advances in superconducting qubit performance require more detailed understandings of the many sources of decoherence. Within these devices, two-level systems arise due to defects, interfaces, and grain boundaries, and are thought to be a major source of qubit decoherence at millikelvin temperatures. In addition to Al, Nb is a commonly used metalization layer for superconducting qubits. Consequently, a significant effort is required to develop and qualify processes that mitigate defects in Nb films. As the fabrication of complete superconducting qubits and their characterization at millikelvin temperatures is a time and resource intensive process, it is desirable to have measurement tools that can rapidly characterize the properties of films and evaluate different treatments. Here we show that measurements of the variation of the superconducting critical temperature $T_c$ with an applied external magnetic field $H$ (of the phase boundary $T_c - H$) performed with very high resolution show features that are directly correlated with the structure of the Nb films. In combination with x-ray diffraction measurements, we show that one can even distinguish variations quality and crystal orientation of the grains in a Nb film by small but reproducible changes in the measured superconducting phase boundary.

Superconducting thin films of niobium have been extensively employed in transmon qubit architectures. Although these architectures have demonstrated remarkable improvements in recent years, further improvements in performance through materials engineering will aid in large-scale deployment. Here, we use information retrieved from secondary ion mass spectrometry and electron microscopy to conduct a detailed assessment of the surface oxide that forms in ambient conditions for transmon test qubit devices patterned from a niobium film. We observe that this oxide exhibits a varying stoichiometry with NbO and NbO$_2$ found closer to the niobium film and Nb$_2$O$_5$ found closer to the surface. In terms of structural analysis, we find that the Nb$_2$O$_5$ region is semicrystalline in nature and exhibits randomly oriented grains on the order of 1-2 nm corresponding to monoclinic N-Nb$_2$O$_5$ that are dispersed throughout an amorphous matrix. Using fluctuation electron microscopy, we are able to map the relative crystallinity in the Nb$_2$O$_5$ region with nanometer spatial resolution. Through this correlative method, we observe that amorphous regions are more likely to contain oxygen vacancies and exhibit weaker bonds between the niobium and oxygen atoms. Based on these findings, we expect that oxygen vacancies likely serve as a decoherence mechanism in quantum systems., Comment: 13 pages, 4 figures

Mixtures containing different weight ratios of single wall carbon nanotubes (SWCNT) and double wall carbon nanotubes (DWCNT) were prepared and studied by in-situ Raman spectroelectrochemistry. Two components of the G-prime mode in the Raman spectra, which can be resolved at high electrode potentials, were assigned to the signals from inner tubes of DWCNT and outer tubes of DWCNT together with SWCNT. The dependence of the ratios of these two components of the G-prime mode on the nominal amount of SWCNT and DWCNT in the samples was simulated so that the residual amount of SWCNT in the original DWCNT could be determined. Additionally, the individual contributions of all components of carbon nanotubes into the total area of the G-prime mode at high electrode potentials were estimated from the simulation.

To fully leverage the power of image simulation to corroborate and explain patterns and structures in atomic resolution microscopy (e.g., electron and scanning probe), an initial correspondence between the simulation and experimental image must be established at the outset of further high accuracy simulations or calculations. Furthermore, if simulation is to be used in context of highly automated processes or high-throughput optimization, the process of finding this correspondence itself must be automated. In this work, we introduce ingrained, an open-source automation framework which solves for this correspondence and fuses atomic resolution image simulations into the experimental images to which they correspond. We describe herein the overall ingrained workflow, focusing on its application to interface structure approximations, and the development of an experimentally rationalized forward model for scanning tunneling microscopy simulation.

There is accelerating interest in developing memory devices using antiferromagnetic (AFM) materials, motivated by the possibility for electrically controlling AFM order via spin-orbit torques, and its read-out via magnetoresistive effects. Recent studies have shown, however, that high current densities create non-magnetic contributions to resistive switching signals in AFM/heavy metal (AFM/HM) bilayers, complicating their interpretation. Here we introduce an experimental protocol to unambiguously distinguish current-induced magnetic and nonmagnetic switching signals in AFM/HM structures, and demonstrate it in IrMn$_3$/Pt devices. A six-terminal double-cross device is constructed, with an IrMn$_3$ pillar placed on one cross. The differential voltage is measured between the two crosses with and without IrMn$_3$ after each switching attempt. For a wide range of current densities, reversible switching is observed only when write currents pass through the cross with the IrMn$_3$ pillar, eliminating any possibility of non-magnetic switching artifacts. Micromagnetic simulations support our findings, indicating a complex domain-mediated switching process.

Using field-emission resonance spectroscopy with an ultrahigh vacuum scanning tunneling microscope, we reveal Stark-shifted image-potential states of the v_1/6 and v_1/5 borophene polymorphs on Ag(111) with long lifetimes, suggesting high borophene lattice and interface quality. These image-potential states allow the local work function and interfacial charge transfer of borophene to be probed at the nanoscale and test the widely employed self-doping model of borophene. Supported by apparent barrier height measurements and density functional theory calculations, electron transfer doping occurs for both borophene phases from the Ag(111) substrate. In contradiction with the self-doping model, a higher electron transfer doping level occurs for denser v_1/6 borophene compared to v_1/5 borophene, thus revealing the importance of substrate effects on borophene electron transfer.

Hybrid organic-inorganic halide perovskite solar cells have emerged as leading candidates for third-generation photovoltaic technology. Despite the rapid improvement in power conversion efficiency (PCE) for perovskite solar cells in recent years, the low-frequency carrier kinetics that underlie practical roadblocks such as hysteresis and degradation remain relatively poorly understood. In an effort to bridge this knowledge gap, we perform here correlated low-frequency noise (LFN) and impedance spectroscopy (IS) characterization that elucidates carrier kinetics in operating perovskite solar cells. Specifically, we focus on planar cell geometries with a SnO2 electron transport layer and two different hole transport layers, namely, poly(triarylamine) (PTAA) and Spiro-OMeTAD. PTAA and Sprio-OMeTAD cells with moderate PCEs of 5 to 12 percent possess a Lorentzian feature at 200 Hz in LFN measurements that corresponds to a crossover from electrode to dielectric polarization. In comparison, Spiro-OMeTAD cells with high PCEs (15 percent) show four orders of magnitude lower LFN amplitude and are accompanied by a cyclostationary process. Through a systematic study of more than a dozen solar cells, we establish a correlation with noise amplitude, power conversion efficiency, and fill factor. Overall, this work establishes correlated LFN and IS as an effective methodology for quantifying low frequency carrier kinetics in perovskite solar cells, thereby providing new physical insights that can rationally guide ongoing efforts to improve device performance, reproducibility, and stability.

Layered indium selenide (InSe) is a van der Waals solid that has emerged as a promising material for high-performance ultrathin solar cells. The optoelectronic parameters that are critical to photoconversion efficiencies, such as hot carrier lifetime and surface recombination velocity, are however largely unexplored in InSe. Here, these key photophysical properties of layered InSe are measured with femtosecond transient reflection spectroscopy. The hot carrier cooling process is found to occur through phonon scattering. The surface recombination velocity and ambipolar diffusion coefficient are extracted from fits to the pump energy-dependent transient reflection kinetics using a free carrier diffusion model. The extracted surface recombination velocity is approximately an order of magnitude larger than that for methylammonium lead-iodide perovskites, suggesting that surface recombination is a principal source of photocarrier loss in InSe. The extracted ambipolar diffusion coefficient is consistent with previously reported values of InSe carrier mobility.

The development of high-performance multifunctional polymer-based electronic circuits is a major step towards future flexible electronics. Here, we demonstrate a tunable approach to fabricate such devices based on rationally designed dielectric super-lattice structures with photochromic azo-benzene molecules. These nanodielectrics possessing ionic, molecular, and atomic polarization are utilized in polymer thin-film transistors (TFTs) to realize high performance electronics with p-type field-effect mobility exceeding 2 cm^2/(V.s). A crossover in the transport mechanism from electrostatic dipolar disorder to ionic-induced disorder is observed in the transistor characteristics over a range of temperatures. The facile supramolecular design allows the possibility to optically control the extent of molecular and ionic polarization in the ultra-thin nanodielectric. Thus, we demonstrate a three-fold increase in the capacitance from 0.1 uF/cm^2 to 0.34 uF/cm^2, which results in a 200% increase in TFT channel current.

Mixed-dimensional van der Waals heterojunctions comprising polymer and twodimensional (2D) semiconductors have many characteristics of an ideal charge separation interface for optoelectronic and photonic applications. However, the photoelectron dynamics at polymer- 2D semiconductor heterojunction interfaces are currently not sufficiently understood to guide the optimization of devices for these applications. This manuscript is a report of a systematic exploration of the time-dependent photophysical processes that occur upon photoexcitation of a type-II heterojunction between the polymer PTB7 and monolayer MoS2. In particular, photoinduced electron transfer from PTB7 to electronically hot states of MoS2 occurs in less than 250 fs. This process is followed by a slower (1-5 ps) exciton diffusion-limited electron transfer from PTB7 to MoS2 with a yield of 58%, and a sub-3-ps photoinduced hole transfer from MoS2 to PTB7. The equilibrium between excitons and polaron pairs in PTB7 determines the charge separation yield, whereas the 3-4 ns lifetime of photogenerated carriers is limited by MoS2 defects. Overall, this work elucidates the mechanisms of ultrafast charge carrier dynamics at PTB7-MoS2 interfaces, which will inform ongoing efforts to exploit polymer-2D semiconductor heterojunctions for photovoltaic and photodetector applications.

Layered two-dimensional (2-D) semiconductors can be combined with other low-dimensional semiconductors to form non-planar mixed-dimensional van der Waals (vdW) heterojunctions whose charge transport behavior is influenced by the heterojunction geometry, providing a new degree of freedom to engineer device functions. Towards that end, we investigated the photoresponse of Si nanowire/MoS2 heterojunction diodes with scanning photocurrent microscopy and time-resolved photocurrent measurements. Comparison of n-Si/MoS2 isotype heterojunctions with p-Si/MoS2 heterojunction diodes under varying biases shows that the depletion region in the p-n heterojunction promotes exciton dissociation and carrier collection. We measure an instrument limited response time of 1 us, which is 10 times faster than previously reported response times for planar Si/MoS2 devices, highlighting the advantages of the 1-D/2-D heterojunction. Finite element simulations of device models provide a detailed understanding of how the electrostatics affect charge transport in nanowire/vdW heterojunctions and inform the design of future vdW heterojunction photodetectors and transistors., Comment: 30 pages, 4 figures

In the last decade, a 2-terminal passive circuit element called a memristor has been developed for non-volatile resistive random access memory and has more recently shown promise for neuromorphic computing. Compared to flash memory, memristors have higher endurance, multi-bit data storage, and faster read/write times. However, although 2-terminal memristors have demonstrated basic neural functions, synapses in the human brain outnumber neurons by more than a factor of 1000, which implies that multiterminal memristors are needed to perform complex functions such as heterosynaptic plasticity. Previous attempts to move beyond 2-terminal memristors include the 3-terminal Widrow-Hoff memistor and field-effect transistors with nanoionic gates or floating gates, albeit without memristive switching in the transistor. Here, we report the scalable experimental realization of a multi-terminal hybrid memristor and transistor (i.e., memtransistor) using polycrystalline monolayer MoS2. Two-dimensional (2D) MoS2 memtransistors show gate tunability in individual states by 4 orders of magnitude in addition to large switching ratios with high cycling endurance and long-term retention of states. In addition to conventional neural learning behavior of long-term potentiation/depression, 6-terminal MoS2 memtransistors possess gate-tunable heterosynaptic functionality that is not achievable using 2-terminal memristors. For example, the conductance between a pair of two floating electrodes (pre-synaptic and post-synaptic neurons) is varied by 10X by applying voltage pulses to modulatory terminals. In situ scanning probe microscopy, cryogenic charge transport measurements, and device modeling reveal that bias-induced MoS2 defect motion drives resistive switching by dynamically varying Schottky barrier heights., Comment: 22 pages, 4 figures

Controlled placement of nanomaterials at predefined locations with nanoscale precision remains among the most challenging problems that inhibit their large-scale integration in the field of semiconductor process technology. Methods based on surface functionalization have a drawback where undesired chemical modifications can occur and deteriorate the deposited material. The application of electric-field assisted placement techniques eliminates the element of chemical treatment; however, it requires an incorporation of conductive placement electrodes that limit the performance, scaling, and density of integrated electronic devices. Here, we report a method for electric-field assisted placement of solution-processed nanomaterials by using large-scale graphene layers featuring nanoscale deposition sites. The structured graphene layers are prepared via either transfer or synthesis on standard substrates, then are removed without residue once nanomaterial deposition is completed, yielding material assemblies with nanoscale resolution that cover surface areas larger than 1mm2. In order to demonstrate the broad applicability, we have assembled representative zero-, one-, and two-dimensional semiconductors at predefined substrate locations and integrated them into nanoelectronic devices. This graphene-based placement technique affords nanoscale resolution at wafer scale, and could enable mass manufacturing of nanoelectronics and optoelectronics involving a wide range of nanomaterials prepared via solution-based approaches., Comment: 17 pages, 5 figures

We report here gate-tunable memristors based on monolayer MoS2 grown by chemical vapor deposition (CVD). These memristors are fabricated in a field-effect geometry with the channel consisting of polycrystalline MoS2 films with grain sizes of 3-5 um. The device characteristics show switching ratios up to 500, with the resistance in individual states being continuously gate-tunable by over three orders of magnitude. The resistive switching results from dynamically varying threshold voltage and Schottky barrier heights, whose underlying physical mechanism appears to be vacancy migration and/or charge trapping. Top-gated devices achieve reversible tuning of the threshold voltage, with potential utility in non-volatile memory or neuromorphic architectures.

Two-dimensional (2D) materials have captured the attention of the scientific community due to the wide range of unique properties at nanometer-scale thicknesses. While significant exploratory research in 2D materials has been achieved, the understanding of 2D electronic transport and carrier dynamics remains in a nascent stage. Furthermore, since prior review articles have provided general overviews of 2D materials or specifically focused on charge transport in graphene, here we instead highlight charge transport mechanisms in post-graphene 2D materials with particular emphasis on transition metal dichalcogenides and black phosphorus. For these systems, we delineate the intricacies of electronic transport including bandstructure control with thickness and external fields, valley polarization, scattering mechanisms, electrical contacts, and doping. In addition, electronic interactions between 2D materials are considered in the form of van der Waals heterojunctions and composite films. This review concludes with a perspective on the most promising future directions in this fast-evolving field., Comment: 48 pages, 8 figures, Annual Reviews of Physical Chemistry

A general self-aligned fabrication scheme is reported here for a diverse class of electronic devices based on van der Waals materials and heterojunctions. In particular, self-alignment enables the fabrication of source-gated transistors in monolayer MoS2 with near-ideal current saturation characteristics and channel lengths down to 135 nm. Furthermore, self-alignment of van der Waals p-n heterojunction diodes achieves complete electrostatic control of both the p-type and n-type constituent semiconductors in a dual-gated geometry, resulting in gate-tunable mean and variance of anti-ambipolar Gaussian characteristics. Through finite-element device simulations, the operating principles of source-gated transistors and dual-gated anti-ambipolar devices are elucidated, thus providing design rules for additional devices that employ self-aligned geometries. For example, the versatility of this scheme is demonstrated via contact-doped MoS2 homojunction diodes and mixed-dimensional heterojunctions based on organic semiconductors. The scalability of this approach is also shown by fabricating self-aligned short-channel transistors with sub-diffraction channel lengths in the range of 150 nm to 800 nm using photolithography on large-area MoS2 films grown by chemical vapor deposition. Overall, this self-aligned fabrication method represents an important step towards the scalable integration of van der Waals heterojunction devices into more sophisticated circuits and systems.

The ability to monitor and control distinct states is at the heart of emerging quantum technologies. The valley pseudospin in transition metal dichalcogenide (TMDC) monolayers is a promising degree of freedom for such control, with the optical Stark effect allowing for valley-selective manipulation of energy levels in WS$_2$ and WSe$_2$ using ultrafast optical pulses. Despite these advances, understanding of valley-sensitive optical Stark shifts in TMDCs has been limited by reflectance-based detection methods where the signal is small and prone to background effects. More sensitive polarization-based spectroscopy is required to better probe ultrafast Stark shifts for all-optical manipulation of valley energy levels. Here, we show time-resolved Kerr rotation to be a more sensitive probe of the valley-selective optical Stark effect in monolayer TMDCs. Compared to the established time-resolved reflectance methods, Kerr rotation is less sensitive to background effects. Kerr rotation provides a five-fold improvement in the signal-to-noise ratio of the Stark effect optical signal and a more precise estimate of the energy shift. This increased sensitivity allows for observation of an optical Stark shift in monolayer MoS$_2$ that exhibits both valley- and energy-selectivity, demonstrating the promise of this method for investigating this effect in other layered materials and heterostructures., Comment: 9 pages, 4 figures, supplementary information