Adam Schwartzberg's research while affiliated with Lawrence Berkeley National Laboratory and other places

Publications (95)

Preprint
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Silicon is the most scalable optoelectronic material, and it has revolutionized our lives in many ways. The prospect of quantum optics in silicon is an exciting avenue because it has the potential to address the scaling and integration challenges, the most pressing questions facing quantum science and technology. We report the first all-silicon qua...
Preprint
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Tomonaga-Luttinger liquid (TLL) behavior in one-dimensional systems has been predicted and shown to occur at semiconductor-to-metal transitions within two-dimensional materials. Reports of mirror twin boundaries (MTBs) hosting a Fermi liquid or a TLL have suggested a dependence on the underlying substrate, however, unveiling the physical details of...
Article
The recent decade brought many advances to plasmonics, but high power density plasmonic antennas designed to behave as heaters or operate in high temperature environments are still facing material stability challenges preventing their ultimate use. Gold has been the optimal choice among plasmonic materials but experiences morphology changes at temp...
Preprint
Carrier and phonon dynamics in a multilayer WSe2 film are captured by extreme ultraviolet (XUV) transient absorption (TA) spectroscopy at the W N6,7, W O2,3, and Se M4,5 edges (30-60 eV). After the broadband optical pump pulse, the XUV probe directly reports on occupations of optically excited holes and phonon-induced band renormalizations. By comp...
Article
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Single-aperture cavities are a key component of lasers, instrumental for the amplification and emission of a single light mode. However, the appearance of high-order transverse modes as cavities size increases has frustrated efforts to scale up cavities whilst preserving single-mode operation since the invention of the laser six decades ago1-8. A s...
Article
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Despite the extraordinary advances in solar cell efficiency in laboratory settings, the deployment of solar cells continues to be limited to low efficiency (<25%) silicon cells because of cost. In this work, we take advantage of the extraordinary optical properties afforded by nanophotonic structures to create a photonic luminescent solar concentra...
Article
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Materials imperfections in planar superconducting quantum circuits—in particular, two-level-system (TLS) defects—contribute significantly to decoherence, ultimately limiting the performance of quantum computation and sensing. The identification of specific parasitic layers and their associated loss contributions has, however, proven elusive. Using...
Article
Ultrathin films suspended as freestanding membranes are critical to many microelectronic and materials science applications. However, fabrication methods are currently limited in either their flexibility, due to material selectivity issues during the final membrane release, or their scalability. Here, we demonstrate a novel fabrication process for...
Article
Metal-organic species can be designed to self-assemble in large-scale, atomically defined, supramolecular architectures. A particular example is hybrid quantum wells, where inorganic two-dimensional (2D) planes are separated by organic ligands. The ligands effectively form an intralayer confinement for charge carriers resulting in a 2D electronic s...
Conference Paper
We experimentally demonstrate Berkeley surface-emitting lasers (BerkSELs) from open-Dirac cavities. BerkSELs exploit symmetry-dependent scaling of losses in cavities with a linear dispersion and remain single-mode even as the cavity size increases.
Article
Qubits made from superconducting materials are a mature platform for quantum information science application, such as quantum computing. However, material-based losses are now a limiting factor in reaching the coherence times needed for applications. In particular, knowledge of the atomistic structure and properties of the circuit materials is need...
Preprint
Full-text available
Qubits made from superconducting materials are a mature platform for quantum information science application such as quantum computing. However, materials-based losses are now a limiting factor in reaching the coherence times needed for applications. In particular, knowledge of the atomistic structure and properties of the circuit materials is need...
Article
Few-femtosecond extreme ultraviolet (XUV) transient absorption spectroscopy, performed with optical 500–1000-nm supercontinuum and broadband XUV pulses (30–50 eV), simultaneously probes dynamics of photoexcited carriers in WS2 at the W O3 edge (37–45 eV) and carrier-induced modifications of core-exciton absorption at the WN6,7 edge (32–37 eV). Acce...
Article
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For two-dimensional (2D) layered semiconductors, control over atomic defects and understanding of their electronic and optical functionality represent major challenges towards developing a mature semiconductor technology using such materials. Here, we correlate generation, optical spectroscopy, atomic resolution imaging, and ab initio theory of cha...
Article
Significance Halide perovskites, especially layered perovskites, offer a number of advantages to creating bright and efficient light-emitting devices and other optoelectronic applications. The organic–inorganic hybrid layered perovskite features complex lattice dynamics due to the ionic character of the crystal and the softness arising from noncova...
Article
Full-text available
Surface plasmons have found a wide range of applications in plasmonic and nanophotonic devices. The combination of plasmonics with three-dimensional photonic crystals has enormous potential for the efficient localization of light in high surface area photoelectrodes. However, the metals traditionally used for plasmonics are difficult to form into t...
Preprint
Attosecond transient absorption spectroscopy, performed with optical 500-1000 nm supercontinuum and broadband extreme ultraviolet (XUV) pulses (30-50 eV), simultaneously probes dynamics of photoexcited carriers in WS$_{2}$ at the W O$_3$ edge (37-45 eV) and carrier-induced modifications of core-exciton absorption at the W N$_{6,7}$ edge (32-37 eV)....
Preprint
Full-text available
Metal-organic species can be designed to self-assemble in large-scale, atomically defined, supramolecular architectures. Hybrid quantum wells, where inorganic two-dimensional (2D) planes are separated by organic ligands, are a particular example. The ligands effectively provide an intralayer confinement for charge carriers resulting in a 2D electro...
Preprint
Organic-inorganic layered perovskites are two-dimensional quantum wells with layers of lead-halide octahedra stacked between organic ligand barriers. The combination of their dielectric confinement and ionic sublattice results in excitonic excitations with substantial binding energies that are strongly coupled to the surrounding soft, polar lattice...
Article
Understanding electronic dynamics in multiexcitonic quantum dots (QDs) is important for designing efficient systems useful in high power scenarios, such as solar concentrators and multielectron charge transfer. The multiple charge carriers within a QD can undergo undesired Auger recombination events, which rapidly annihilate carriers on picosecond...
Preprint
Full-text available
Quantum sensing and computation can be realized with superconducting microwave circuits. Qubits are engineered quantum systems of capacitors and inductors with non-linear Josephson junctions. They operate in the single-excitation quantum regime, photons of $27 \mu$eV at 6.5 GHz. Quantum coherence is fundamentally limited by materials defects, in pa...
Article
Attosecond transient absorption spectroscopy (ATAS) is used to observe photoexcited dynamics with outstanding time resolution. The main experimental challenge of this technique is that high-harmonic generation sources show significant instabilities, resulting in sub-par sensitivity when compared to other techniques. This paper proposes edge-pixel r...
Article
Pentacene's extraordinary photophysical and electronic properties are highly dependent on intermolecular through-space interactions. Macrocyclic arrangements of chromophores have been shown to provide a high level of control over these interactions, but few examples exist for pentacene due to inherent synthetic challenges. In this work, zirconocene...
Preprint
Full-text available
For two-dimensional (2D) layered semiconductors, control over atomic defects and understanding of their electronic and optical functionality represent major challenges towards developing a mature semiconductor technology using such materials. Here, we correlate generation, optical spectroscopy, atomic resolution imaging, and ab-initio theory of cha...
Preprint
Full-text available
Attosecond transient absorption spectroscopy (ATAS) is used to observe photoexcited dynamics with outstanding time resolution. The main experimental challenge of this technique is that high-harmonic generation sources show significant instabilities, resulting in sub-par sensitivity when compared to other techniques. This paper proposes edge-pixel r...
Preprint
p>Pentacene’s extraordinary photophysical and electronic properties are highly dependent on intermolecular, through-space interactions. Macrocyclic arrangements of chromophores have been shown to provide a high level of control over these interactions, but few examples exist for pentacene due to inherent synthetic challenges. In this work, zirconoc...
Article
Plasmonic nanostructures serve as optical antennas for concentrating the energy of incoming light in localized hotspots close to their surface. By positioning nanoemitters in the antenna hotspots, energy transfer is enabled, leading to novel hybrid antenna-emitter-systems, where the antenna can be used to manipulate the optical properties of the na...
Article
Full-text available
Quantum dot-like single-photon sources in transition metal dichalcogenides (TMDs) exhibit appealing quantum optical properties but lack a well-defined atomic structure and are subject to large spectral variability. Here, we demonstrate electrically stimulated photon emission from individual atomic defects in monolayer WS2 and directly correlate the...
Article
Free-standing ultra-thin (~2 nm) films of several oxides (Al2O3, TiO2, and others) have been developed, which are mechanically robust and transparent to electrons with Ekin ≥ 200 eV, and to photons. We demonstrate their applicability in environmental X-ray photoelectron and infrared spectroscopy for molecular level studies of solid-gas (≥1 bar) and...
Article
Full-text available
Atomically thin polycrystalline transition-metal dichalcogenides (TMDs) are relevant to both fundamental science investigation and applications. TMD thin-films present uniquely difficult challenges to effective nanoscale crystalline characterization. Here we present a method to quickly characterize the nanocrystalline grain structure and texture of...
Article
Two-dimensional (2D) excitons arise from electron-hole confinement along one spatial dimension. Such excitations are often described in terms of Frenkel or Wannier limits according to the degree of exciton spatial localization and the surrounding dielectric environment. In hybrid material systems, such as the 2D perovskites, the complex underlying...
Article
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Colloidal inorganic perovskite nanocrystals (PNCs) are solution‐processable optoelectronic materials whose emission can be easily tuned via both size and composition while maintaining high photoluminescence quantum yield. Despite their relative defect tolerance, they suffer from photoinduced damage and degradation under ambient conditions. The lack...
Article
Förster Resonant Energy Transfer (FRET)-mediated exciton diffusion through artificial nanoscale building block assemblies could be used as an optoelectronic design element to transport energy. However, so far nanocrystal (NC) systems supported only diffusion lengths of 30 nm, which are too small to be useful in devices. Here, we demonstrate a FRET-...
Preprint
Full-text available
Control of impurity concentrations in semiconducting materials is essential to device technology. Because of their intrinsic confinement, the properties of two-dimensional semiconductors such as transition metal dichalcogenides (TMDs) are more sensitive to defects than traditional bulk materials. The technological adoption of TMDs is dependent on t...
Preprint
F\"orster Resonant Energy Transfer (FRET)-mediated exciton diffusion through artificial nanoscale building block assemblies could be used as a new optoelectronic design element to transport energy. However, so far nanocrystal (NC) systems supported only diffusion length of 30 nm, which are too small to be useful in devices. Here, we demonstrate a F...
Article
Full-text available
Zinc oxide (ZnO) is a stable, direct bandgap semiconductor emitting in the UV with a multitude of technical applications. It is well known that ZnO emission can be shifted into the green for visible light applications through the introduction of defects. However, generating consistent and efficient green emission through this process is challenging...
Preprint
Atomically thin polycrystalline transition-metal dichalcogenides (TMDs) are relevant to both fundamental science investigation and applications. TMD thin-films present uniquely difficult challenges to effective nanoscale crystalline characterization. Here we present a method to quickly characterize the nanocrystalline grain structure and texture of...
Preprint
Optical quantum emitters are a key component of quantum devices for metrology and information processing. In particular, atomic defects in 2D materials can operate as optical quantum emitters that overcome current limitations of conventional bulk emitters, such as yielding a high single-photon generation rate and offering surface accessibility for...
Article
In manufacturing, etch profiles play a significant role in device patterning. Here, the authors present a study of the evolution of etch profiles of nanopatterned silicon oxide using a chromium hard mask and a CHF3/Ar atomic layer etching in a conventional inductively coupled plasma tool. The authors show the effect of substrate electrode temperatu...
Article
Full-text available
Transition metal dichalcogenides (TMDs) promise to revolutionize optoelectronic applications. While monolayer exfoliation and vapor phase growth produce extremely high quality 2D materials, direct fabrication at wafer scale remains a significant challenge. Here, we present a method that we call ‘lateral conversion’, which enables the synthesis of p...
Article
Structural defects in 2D materials offer an effective way to engineer new material functionalities beyond conventional doping. We report on the direct experimental correlation of the atomic and electronic structure of a sulfur vacancy in monolayer WS2 by a combination of CO-tip noncontact atomic force microscopy and scanning tunneling microscopy. S...
Article
Control of impurity concentrations in semiconducting materials is essential to device technology. Because of their intrinsic confinement, the properties of two-dimensional semiconductors such as transition metal dichalcogenides (TMDs) are more sensitive to defects than traditional bulk materials. The technological adoption of TMDs is dependent on t...
Article
Full-text available
Chalcogen vacancies are generally considered to be the most common point defects in transition metal dichalcogenide (TMD) semiconductors because of their low formation energy in vacuum and their frequent observation in transmission electron microscopy studies. Consequently, unexpected optical, transport, and catalytic properties in 2D-TMDs have bee...
Article
Full-text available
Plasmonic nanoantennas are ideal for single molecule detection since they nano-focus the light beyond diffraction and enhance the optical fields by several orders of magnitude. But delivering the molecules into these nanometric hot-spots is a real challenge. Here, we present a dynamic sensor, with label-free real-time detection capabilities, which...
Article
With ever increasing demands on device patterning to achieve smaller critical dimensions, the need for precise, controllable atomic layer etching (ALE) is steadily increasing. In this work, a cyclical fluorocarbon/argon plasma is successfully used for patterning silicon oxide by ALE in a conventional inductively coupled plasma tool. The impact of p...
Article
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One-dimensional (1D) nanomaterials with highly anisotropic optoelectronic properties are key components in energy harvesting, flexible electronics, and biomedical imaging devices. 3D patterning methods that precisely assemble nanowires with locally controlled composition and orientation would enable new optoelectronic device designs. As an exemplar...
Article
Superefficient light emission A challenge to improving synthesis methods for superefficient light-emitting semiconductor nanoparticles is that current analytical methods cannot measure efficiencies above 99%. Hanifi et al. used photothermal deflection spectroscopy to measure very small nonradiative decay components in quantum dot photoluminescence....
Article
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Materials for nanophotonic devices ideally combine ease of deposition, very high refractive index, and facile pattern formation through lithographic templating and/or etching. In this work, we present a scalable method for producing high refractive index WS2 layers by chemical conversion of WO3 synthesized via atomic layer deposition (ALD). These c...
Article
Two-dimensional materials with engineered composition and structure will provide designer materials beyond conventional semiconductors. However, the potentials of defect engineering remain largely untapped, because it hinges on a precise understanding of electronic structure and excitonic properties, which are not yet predictable by theory alone. H...
Preprint
Full-text available
Chalcogen vacancies are considered to be the most abundant point defects in two-dimensional (2D) transition-metal dichalcogenide (TMD) semiconductors, and predicted to result in deep in-gap states (IGS). As a result, important features in the optical response of 2D-TMDs have typically been attributed to chalcogen vacancies, with indirect support fr...
Preprint
Full-text available
Structural defects in 2D materials offer an effective way to engineer new material functionalities beyond conventional doping in semiconductors. Specifically, deep in-gap defect states of chalcogen vacancies have been associated with intriguing phenomena in monolayer transition metal dichalcogenides (TMDs). Here, we report the direct experimental c...
Conference Paper
Controlling Angstrom-thick film etching is essential to further develop sub-10 nanometer semiconductor manufacturing. Single digit nanofabrication requires the ability to achieve atomic scale etching control and material selectivity during pattern transfer. Atomic Layer Etching (ALE) satisfies these needs as critical dimensions continue to shrink....
Article
Chemical transformations that occur on photoactive materials, such as photoelectrochemical water splitting, are strongly influenced by the surface properties as well as by the surrounding environment. Herein, we elucidate the effects of oxygen and water surface adsorption on band alignment, interfacial charge transfer, and charge carrier transport...
Article
Ternary structure is an important design strategy to obtain high-efficiency non-fullerene organic photovoltaics (OPVs). However, the role of the third component to the standard binary system is still unclear. Here, a wide-bandgap small-molecule acceptor, denoted IDT-T, is synthesized and used together with a wide-bandgap donor polymer, PBDB-T, and...
Article
The next generation of hard disk drive technology for data storage densities beyond 5 Tb/in<sup>2</sup> will require single-bit patterning of features with sub-10 nm dimensions by nanoimprint lithography. To address this challenge master templates are fabricated using pattern multiplication with atomic layer deposition. Sub-10 nm lithography requir...
Article
Full-text available
The performance of energy materials hinges on the presence of structural defects and heterogeneity over different length scales. Here we map the correlation between morphological and functional heterogeneity in bismuth vanadate, a promising metal oxide photoanode for photoelectrochemical water splitting, by photoconductive atomic force microscopy....
Article
Full-text available
Van der Waals epitaxy enables the integration of 2D transition metal dichalcogenides with other layered materials to form heterostructures with atomically sharp interfaces. However, the ability to fully utilize and understand these materials using surface science techniques such as angle resolved photoemission spectroscopy (ARPES) and scanning tunn...
Conference Paper
Strong enhancement of exciton binding has been observed in valence-excitons in the optical regime of 2D materials. We report direct observation of long-lived core-exciton states in transition metal dichalcogenides by attosecond transient absorption spectroscopy in the XUV.
Article
Full-text available
While electrochemical supercapacitors often show high power density and long operation lifetimes, they are plagued by limited energy density. Pseudocapacitive materials, in contrast, operate by fast surface redox reactions and are shown to enhance energy storage of supercapacitors. Furthermore, several reported systems exhibit high capacitance but...
Article
Gap plasmonic nanostructures are of great interest due to their ability to concentrate light into small volumes. Theoretical studies, considering quantum mechanical effects, have predicted the optimal spatial gap between adjacent nanoparticles to be in the sub-nanometer regime in order to achieve the strongest possible field enhancement. Here, we p...
Article
Iron is the most abundant transition metal in the Earth's crust, and naturally occurring iron oxide minerals play a commanding role in environmental redox reactions. Although iron oxide redox reactions are well studied, their precise mechanisms are not fully understood. Recent work has shown that these involve electron transfer pathways within the...
Article
2D transition metal dichalcogenides (TMDs) are commonly grown by chemical vapor deposition using transition metal oxides as solid precursors. Despite the widespread use of this technique, challenges in reproducibility, coverage, and material quality are pervasive, suggestive of unknown and uncontrolled process parameters. In this communication, we...
Chapter
This chapter discusses metal-oxide resists by focusing on two materials—hydrogen silsesquioxane (HSQ) and hafnium peroxide sulfate (HafSOx). Small HSQ and HafSOx nanocluster building blocks enable single-digit-nm patterning via electron beam and extreme UV exposures. Nanocluster components, metals and organic ligands, affect resist shelf stability,...
Article
Artificial photosystems are advanced by the development of conformal catalytic materials that promote desired chemical transformations, while also maintaining stability and minimizing parasitic light absorption for integration on surfaces of semiconductor light absorbers. Here, we demonstrate that multifunctional, nanoscale catalysts that enable hi...
Article
Significance Solar-powered chemical production from CO 2 promises to alleviate petrochemical consumption. Hybrid systems of an inorganic semiconductor light harvester and a microbial catalyst offer a viable way forward. Whereas a number of such systems have been described, the semiconductor-to-bacterium electron transfer mechanism remains largely u...
Article
Ultrafast pump-probe measurements of plasmonic nanostructures probe the non-equilibrium behavior of excited carriers, which involves several competing effects obscured in typical empirical analyses. Here we present pump-probe measurements of plasmonic nanoparticles along with a complete theoretical description based on first-principles calculations...
Article
Peptoid nanosheets can be broadly functionalized for a variety of applications. However, they are susceptible to degradation when exposed to chemical or mechanical stress. To improve their strength, photolabile monomers were introduced in order to crosslink the nanosheet interior. Photo-crosslinking produced a more robust material that could surviv...
Article
Using Surface Enhanced Raman Scattering (SERS), we report on intensity-dependent broadening in graphene-deposited broad-band antennas. The antenna gain curve includes both the incident frequency and some of the scattered mode frequencies. By comparing antennas with various gaps and types (bow-tie vs. diamond-shape antennas) we make the case that th...