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At least 19 records

Post-growth modulation doping by ion implantation

Modulation doping is a commonly adopted technique to create two-dimensional (2D) electrons or holes in semiconductor heterostructures. One constraint, however, is that the intentional dopants required for modulation doping are controlled and incorporated during the growth of heterostructures. Here, using undoped strained germanium quantum wells as the model material system, we show that modulation doping can be achieved post-growth of heterostructures by ion implantation and dopant-activation anneals. The carrier density is controlled ex situ by varying the ion fluence and implant energy, and an empirical calibration curve is obtained. While the mobility of the resulting 2D holes is lower than that in undoped heterostructure field-effect transistors built using the same material, the achievable carrier density is significantly higher. Potential applications of this modulation-doping technique are discussed.

42 ENGINEERING↗

Modulation-doping a correlated electron insulator

Abstract Correlated electron materials (CEMs) host a rich variety of condensed matter phases. Vanadium dioxide (VO 2 ) is a prototypical CEM with a temperature-dependent metal-to-insulator (MIT) transition with a concomitant crystal symmetry change. External control of MIT in VO 2 —especially without inducing structural changes—has been a long-standing challenge. In this work, we design and synthesize modulation-doped VO 2 -based thin film heterostructures that closely emulate a textbook example of filling control in a correlated electron insulator. Using a combination of charge transport, hard X-ray photoelectron spectroscopy, and structural characterization, we show that the insulating state can be doped to achieve carrier densities greater than 5 × 10 21 cm −3 without inducing any measurable structural changes. We find that the MIT temperature (T MIT ) continuously decreases with increasing carrier concentration. Remarkably, the insulating state is robust even at doping concentrations as high as ~0.2 e − /vanadium. Finally, our work reveals modulation-doping as a viable method for electronic control of phase transitions in correlated electron oxides with the potential for use in future devices based on electric-field controlled phase transitions.

36 MATERIALS SCIENCE↗

Modulation Doping via a Two-Dimensional Atomic Crystalline Acceptor

Two-dimensional nanoelectronics, plasmonics, and emergent phases require clean and local charge control, calling for layered, crystalline acceptors or donors. Our Raman, photovoltage, and electrical conductance measurements combined with ab initio calculations establish the large work function and narrow bands of α-RuCl 3 enable modulation doping of exfoliated single and bilayer graphene, chemical vapor deposition grown graphene and WSe 2 , and molecular beam epitaxy grown EuS. We further demonstrate proof of principle photovoltage devices, control via twist angle, and charge transfer through hexagonal boron nitride. Short-ranged lateral doping (≤65 nm) and high homogeneity are achieved in proximate materials with a single layer of α-RuCl 3 . Here, this leads to the best-reported monolayer graphene mobilities (4900 cm 2 /(V s)) at these high hole densities (3 × 10 13 cm -2 ) and yields larger charge transfer to bilayer graphene (6 × 10 13 cm -2 ).

2D atomic crystals↗

Doping-modulated strain control of bifunctional electrocatalysis for rechargeable zinc–air batteries

Changes in the local atomic arrangement in a crystal caused by lattice-mismatch-induced strain can efficiently regulate the performance of electrocatalysts for zinc–air batteries (ZABs) in many manners, mainly due to modulated electronic structure configurations that affect the adsorption energies for oxygen-intermediates formed during oxygen reduction and evolution reactions (ORR and OER). However, the application of strain engineering in electrocatalysis has been limited by the strain relaxation caused by structural instability such as dissolution and destruction, leading to insufficient durability towards the ORR/OER. In this work, we propose a doping strategy to modulate the phase transition and formation of self-supported cobalt fluoride–sulfide (CoFS) nanoporous films using a low amount of copper (Cu) as a dopant. This well-defined Cu–CoFS heterostructure overcomes the obstacle of structural instability. Our study of the proposed Cu–CoFS also helps establish the structure–property relationship of strained electrocatalysts by unraveling the role of local strain in regulating the electronic structure of the catalyst. As a proof-of-concept, the Cu–CoFS electrocatalyst with doping-modulated strain exhibited superior onset potentials of 0.91 V and 1.49 V for the ORR and OER, respectively, surpassing commercial Pt/C@RuO 2 and benchmarking non-platinum group metal (non-PGM) catalysts. ZABs with the Cu–CoFS catalyst delivered excellent charge/discharge cycling performance with an extremely low voltage gap of 0.5 V at a current density of 10 mA cm –2 and successively 0.93 V at a high current density of 100 mA cm –2 and afforded an outstanding peak power density of 255 mW cm –2 .

25 ENERGY STORAGE↗

P‐Doping Modulated RuIr Nanoparticles Anchored on Co/N/C Catalysts with Improved Alkaline Hydrogen Evolution Activity and Stability

Achieving efficient and stable hydrogen evolution reactions in alkaline conditions is crucial for hydrogen production. In this study, a RuIr/Co (SA) NC-P catalyst featuring RuIr alloys alongside P-doping and CoNx sites is developed. RuIr alloying optimizes the electronic structure between Ru and Ir, promoting electron transfer from Ru to Ir. P-doping further modulates the electronic properties of RuIr alloys, optimizing hydrogen binding energy and weakening Ru─OH binding energy, facilitating rapid H 2 generation and OH ad transfer. Meanwhile, CoNx promotes water dissociation, providing a fast proton delivery path for RuIr alloys. The catalyst exhibits enhanced HER activity with a low overpotential of 20 mV at 10 mA cm −2 , a Tafel slope of 20.4 mV dec −1 , and a turnover frequency of 19.5 H 2 s −1 at 150 mV overpotential. Moreover, catalyst stability is improved 8 times by mitigating RuIr alloy dissolution/agglomeration via P-doping. In conclusion, this work introduces a promising approach for developing efficient and stable HER electrocatalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

High-efficiency perovskite photovoltaic modules achieved via cesium doping

Perovskite solar modules have been attracting increasing attention due to their market potential, yet publications concerned with theintrinsic scale-up potential of different perovskite compositions remain relatively scarce. On the other hand, while great success is being made towards improving the power conversion efficiency (PCE) of perovskite solar cells (PSCs) by cesium cation (Cs + ) doping of the perovskite, more attention is being paid to the perovskite phase stabilization effect of Cs + doping, and less to other properties that are critical to understand and futher improve the PSC's. In this work, moderately-Cs-doped MAPbI 3 was employed as a model perovskite material in order to exclude the phase stabilization effect. Our systematic study revealed the influence of Cs + in organic-inorganic hybrid perovskites on the crystal structure, crystallization process, trap state density, band structure and charge (i.e., ions or photo-carriers) transport. Markedly, it has been observed that Cs + doping can greatly increase the carrier diffusion length in the perovskite films, thus improving the potential to scale-up PSC's.The PCE of small area devices (0.09 cm 2 ) was increased to 21.72% from 19.73%, with decreased hysteresis behavior and increased operational stability (T85 = 1000 h) after Cs + doped, where T85 refers to the retention of 85% of the initial PCE. Moreover, a PCE of 21.08% was obtained for a Cs + -containing perovskite module with an active area > 30 cm 2 , which demonstrates a better "reproducibility" than the reference sample (MAPbI3-based perovskite modules, PCE = 18.26%).

14 SOLAR ENERGY↗

Effect of p-doping on the intensity noise of epitaxial quantum dot lasers on silicon

This work experimentally investigates the impact of p-doping on the relative intensity noise (RIN) properties and subsequently on the modulation properties of semiconductor quantum dot (QD) lasers epitaxially grown on silicon. Owing to the low threading dislocation density and the p-modulation doped GaAs barrier layer in the active region, the RIN level is found very stable with temperature with a minimum value of − <#comment/> 150 d B / H z . The dynamical features extracted from the RIN spectra show that p-doping between zero and 20 holes/dot strongly modifies the modulation properties and gain nonlinearities through increased internal losses in the active region and thereby hinders the maximum achievable bandwidth. Overall, this Letter is important for designing future high-speed and low-noise QD devices integrated in future photonic integrated circuits.

Duan, Jianan (ORCID:0000000177104287)↗

Enhancing the Reaction Kinetics and Stability of Co‐Free Li‐Rich Cathode Materials via a Multifunctional Strategy

Co-free Li-rich layered oxides (CFLLOs) with anionic redox activity are among the most promising cathode materials for high-energy-density and low-cost lithium-ion batteries (LIBs). However, irreversible oxygen release often causes severe structural deterioration, electrolyte decomposition, and the formation of unstable cathode-electrolyte interface (CEI) film with high impedance. Additionally, the elimination of cobalt elements further deteriorates the reaction kinetics, leading to reduced capacity and poor rate performance. Here, in this study, a multifunctional strategy is proposed, incorporating Li 2 MnO 3 phase content regulation, micro-nano structure design, and heteroatom substitution. The increased content of Li 2 MnO 3 phase enhances the capacity through oxygen redox. The smaller nanoscale primary particles induce greater tensile strain and introduce more grain boundaries, thereby improving the reaction kinetics and reactivity, while the larger micron-sized secondary particles help to reduce interfacial side reactions. Furthermore, Na⁺ doping modulates the local coordination environment of oxygen, stabilizing both the anion framework and the crystal structure. As a result, the designed cathode exhibits enhanced rate performance, delivering a capacity of 158 mAh g⁻¹ at 5.0 C and improved cyclic stability, with a high capacity retention of 99% after 400 cycles at 1.0 C. This multifunctional strategy holds great promise for advancing the practical application of CFLLOs in next-generation LIBs.

Co-free Li-rich layered oxide↗

Upper critical magnetic field and multiband superconductivity in artificial high-𝑇 𝑐 superlattices of nano quantum wells

Artificial high-T c superlattices (AHTS) composed of quantum building blocks with tunable superconducting critical temperature have been synthesized by engineering their nanoscale geometry using the Bianconi-Perali Valletta (BPV) two-gap superconductivity theory. These quantum heterostructures consist of quantum wells made of superconducting, modulation-doped Mott insulators (S), confined by a metallic (N) potential barrier. The lattice geometry has been carefully engineered to induce the predicted Fano-Feshbach shape resonance between the gaps, near a topological Lifshitz transition. Here, we validate the BPV theory by providing compelling experimental evidence that AHTS samples, at the peak of the superconducting dome, exhibit resonant two-band, two-gap superconductivity. This is demonstrated by measuring the temperature dependence of the upper critical magnetic field, μ 0 H c2 , in samples with superlattice periods 3.3 < d < 5.28 nm and L/d ratios close to the magic value 2/3 (where L is the thickness of the superconducting La 2 CuO 4 layer and d is the superlattice period). Here, the data reveal the predicted upward concavity in H c2 (T) and a characteristic kink in the coherence length as a function of temperature, confirming the predicted two-band superconductivity with Fermi velocity ratio ≈ 0.25 and significant pair-exchange term among the two condensates.

Heterostructures↗

Thermal and Quantum Melting Phase Diagrams for a Magnetic-Field-Induced Wigner Solid

A sufficiently large perpendicular magnetic field quenches the kinetic (Fermi) energy of an interacting two-dimensional (2D) system of fermions, making them susceptible to the formation of a Wigner solid (WS) phase in which the charged carriers organize themselves in a periodic array in order to minimize their Coulomb repulsion energy. In low-disorder 2D electron systems confined to modulation-doped GaAs heterostructures, signatures of a magnetic-field-induced WS appear at low temperatures and very small Landau level filling factors ($\textit{ν}$ ≃ 1/5). In dilute GaAs 2D hole systems, on the other hand, thanks to the larger hole effective mass and the ensuing Landau level mixing, the WS forms at relatively higher fillings ($\textit{ν}$ ≃ 1/3). Here we report our measurements of the fundamental temperature vs filling phase diagram for the 2D holes’ WS-liquid thermal melting. Moreover, via changing the 2D hole density, we also probe their Landau level mixing vs filling WS-liquid quantum melting phase diagram. In this work, we find our data to be in good agreement with the results of very recent calculations, although intriguing subtleties remain.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Record-quality GaAs two-dimensional hole systems

The complex band structure, large spin-orbit induced band splitting, and heavy effective mass of two-dimensional (2D) hole systems hosted in GaAs quantum wells render them rich platforms to study many-body physics and ballistic transport phenomena. Here we report ultra-high-quality (001) GaAs 2D hole systems, fabricated using molecular beam epitaxy and modulation doping, with mobility values as high as 5.8 × 10 6 cm 2 /(V s) at a hole density of p = 1.3 × 10 11 /cm 2 , implying a mean free path of ≃ 27 μm. In the low-temperature magnetoresistance trace of this sample, we observe high-order fractional quantum Hall states up to the Landau level filling ν = 12/25 near ν = 1/2. Furthermore, we see a deep minimum develop at ν = 1/5 in the magnetoresistance of a sample with a much lower hole density of p = 4.0 × 10 10 /cm 2 where we measure a mobility of 3.6 × 10 6 cm2/(V s). Finally, these improvements in sample quality were achieved by the reduction of residual impurities both in the GaAs channel and in the AlGaAs barrier material, as well as optimization in the design of the sample structure.

2-dimensional systems↗

Transient Studies of Nonequilibrium Transport in Two-Dimensional Semiconductors

The overarching objective of research under DOE support has been to investigate emergent carrier phenomena in different two-dimensional (2D) systems, under conditions where they are driven far from equilibrium. The description of nonequilibrium transport has long represented one of the most enduring challenges in condensed-matter physics, in large part due to the need to invoke the role of complex many-body phenomena (electron-phonon and electron-electron coupling) in this regime. In this project, we have explored aspects of this problem in a variety of different two-dimensional systems. These include the modulation-doped two-dimensional electrons gas, or 2DEG, in GaAs/AlGaAs heterostructures; the electron and hole systems in graphene and its related hetero-structures, and; the strongly-confined electron layers in transition-metal dichalcogenide (MoS 2 and WS 2 ) and trichalcogenide (TiS 3 ) materials. Significant understanding has been achieved in a number of different areas, as we elaborate upon in subsequent sections of this proposal: Nanoscale spectroscopy of defect-related barriers in MoS2 Negative differential conductance due to inter-valley scattering in WS 2 under high fields Incipient localization due to scattering from frozen-phonon disorder in quantum point contacts High-field transient transport in graphene/hexagonal BN heterostructures Universal voltage scaling of quantum corrections in graphene under nonequilibrium A defining feature of much of this research has been an approach to problem solving in which novel experimental techniques (such as transient electrical pulsing and scanning-probe microscopy) are combined with the development (in collaboration with colleagues from condensed-matter theory) of sophisticated models, a strategy that we propose to continue in our future research. In recent years, we have developed an increasing capacity for handling atomically-thin materials, and their van der Waals systems, a capacity that is reflected in the balance of topics listed above.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Correlated States of Two-dimensional Electron Systems in AlAs Quantum Wells

Two-dimensional (2D) carrier systems confined to modulation-doped semiconductor hetero-structures provide a nearly ideal testing ground for exploring new physical phenomena. At low temperatures and in the presence of a strong magnetic field, these systems exhibit fascinating, often unexpected, many-body states, arising from the strong electron-electron interaction. In our work, we studied various many-body states of different 2D systems. These included 2D electron and hole systems confined to GaAs and also to AlAs quantum wells, including wide quantum wells where the charge distribution is bilayer like. We observed and reported new phenomena in these systems, including new (even-denominator) fractional quantum Hall states, Wigner crystal solid phases, and composite fermion compressible states.

36 MATERIALS SCIENCE↗