Photo-FETs: phototransistors enabled by 2D and 0D nanomaterials

The large diversity of applications in our daily lives that rely on photodetection technology requires photodetectors with distinct properties. The choice of an adequate photodetecting system depends on its application, where aspects such as spectral selectivity, speed, and sensitivity play a critical role. High-sensitivity photodetection covering a large spectral range from the UV to IR is dominated by photodiodes. To overcome existing limitations in sensitivity and cost of state-of-the-art systems, new device architectures and material systems are needed with low-cost fabrication and high performance. Low-dimensional nanomaterials (0D, 1D, 2D) are promising candidates with many unique electrical and optical properties and additional functionalities such as flexibility and transparency. In this Perspective, the physical mechanism of photo-FETs (field-effect transistors) is described and recent advances in the field of low-dimensional photo-FETs and hybrids thereof are discussed. Several requirements for the channel material are addressed in view of the photon absorption and carrier transport process, and a fundamental trade-off between them is pointed out for single-material-based devices. We further clarify how hybrid devices, consisting of an ultrathin channel sensitized with strongly absorbing semiconductors, can circumvent these limitations and lead to a new generation of highly sensitive photodetectors. Recent advances in the development of sensitized low-dimensional photo-FETs are discussed, and several promising future directions for their application in high-sensitivity photodetection are proposed.Peer ReviewedPostprint (author's final draft

Starry Messages: Searching for Signatures of Interstellar Archaeology

Searching for signatures of cosmic-scale archaeological artifacts such as Dyson spheres or Kardashev civilizations is an interesting alternative to conventional SETI. Uncovering such an artifact does not require the intentional transmission of a signal on the part of the original civilization. This type of search is called interstellar archaeology or sometimes cosmic archaeology. The detection of intelligence elsewhere in the Universe with interstellar archaeology or SETI would have broad implications for science. For example, the constraints of the anthropic principle would have to be loosened if a different type of intelligence was discovered elsewhere. A variety of interstellar archaeology signatures are discussed including non-natural planetary atmospheric constituents, stellar doping with isotopes of nuclear wastes, Dyson spheres, as well as signatures of stellar and galactic-scale engineering. The concept of a Fermi bubble due to interstellar migration is introduced in the discussion of galactic signatures. These potential interstellar archaeological signatures are classified using the Kardashev scale. A modified Drake equation is used to evaluate the relative challenges of finding various sources. With few exceptions interstellar archaeological signatures are clouded and beyond current technological capabilities. However SETI for so-called cultural transmissions and planetary atmosphere signatures are within reach.Comment: 29 pages including 4 figures and 1 tabl

Electron Sources for Future Lightsources, Summary and Conclusions for the Activities during FLS 2012

This paper summarizes the discussions, presentations, and activity of the Future Light Sources Workshop 2012 (FLS 2012) working group dedicated to Electron Sources. The focus of the working group was to discuss concepts and technologies that might enable much higher peak and average brightness from electron beam sources. Furthermore the working group was asked to consider methods to greatly improve the robustness of operation and lower the costs of providing electrons.Comment: 11 pages, 7 figures, summary paper from working group Future Light Sources 2012 Workshop at Newport News, Virginia, USA (http://www.jlab.org/conferences/FLS2012/

Beam-Material Interaction

Th is paper is motivated by the growing importance of better understanding of the phenomena and consequences of high- intensity energetic particle beam interactions with accelerator, generic target , and detector components. It reviews the principal physical processes of fast-particle interactions with matter, effects in materials under irradiation, materials response, related to component lifetime and performance, simulation techniques, and methods of mitigating the impact of radiation on the components and envir onment in challenging current and future applicationComment: 28 pages, contribution to the 2014 Joint International Accelerator School: Beam Loss and Accelerator Protection, Newport Beach, CA, USA , 5-14 Nov 201

Application of Two-Photon Absorbing Fluorene-Containing Compounds in Bioimaging and Photodyanimc Therapy

Two-photon absorbing (2PA) materials has been widely studied for their highly localized excitation and nonlinear excitation efficiency. Application of 2PA materials includes fluorescence imaging, microfabrication, 3D data storage, photodynamic therapy, etc. Many materials have good 2PA photophysical properties, among which, the fluorenyl structure and its derivatives have attracted attention with their high 2PA cross-section and high fluorescence quantum yield. Herein, several compounds with 2PA properties are discussed. All of these compounds contain one or two fluorenyl core units as part of the conjugated system. The aim of this dissertation is to discuss the application of these compounds according to their photophysical properties. In chapters 2 to 4, compounds were investigated for cell imaging and tissue imaging. In chapter 5, compounds were evaluated for photodynamic therapy effects on cancer cells. Chapters 2 and 3 detail compounds with quinolizinium and pyran as core structures, respectively. Fluorene was introduced into structures as substituents. Quinolizinium structures exhibited a large increase in fluorescence when binding with Bovine Serum Albumin (BSA). Further experiments in cell imaging demonstrated a fluorescence turn-on effect in cell membranes, indicating the possibility for these novel compounds to be promising membrane probes. Pyran structures were conjugated with arginylglycylaspartic acid peptide (RGD) to recognize integrin and introduced in cells and an animal model with tumors. Both probes showed specific targeting of tumor vasculature. Imaging reached penetration as deep as 350 µm in solid tumors and exhibited good resolution. These results suggest the RGD-conjugated pyran structure should be a good candidate probe for live tissue imaging. Chapter 4 applied a fluorene core structure conjugated with RGD as well. Application of this fluorenyl probe compound is in wound healing animal models. Fluorescence was collected from vasculature and fibroblasts up to ≈ 1600 µm within wound tissue in lesions made on the skin of mice. The resolution of images is also high enough to recognize cell types by immunohistochemical staining. This technology can be applied for reliable quantification and illustration of key biological processes taking place during tissue regeneration in the skin. Chapter 5 describes three fluorenyl core structures with photoacid generation properties. One of the structures showed excellent photo-induced toxicity. Cancer cells underwent necrotic cell death due to pH decrease in lysosomes and endosomes, suggesting a new mechanism for photodynamic therapy

On-a-chip microdischarge thruster arrays inspired by photonic device technology for plasma television

This study shows that the practical scaling of a hollow cathode thruster device to MEMS level should be possible albeit with significant divergence from traditional design. The main divergence is the need to operate at discharge pressures between 1-3bar to maintain emitter diameter pressure products of similar values to conventional hollow cathode devices. Without operating at these pressures emitter cavity dimensions become prohibitively large for maintenance of the hollow cathode effect and without which discharge voltage would be in the hundreds of volts as with conventional microdischarge devices. In addition this requires sufficiently constrictive orifice diameters in the 10µm – 50µm range for single cathodes or <5µm larger arrays. Operation at this pressure results in very small Debye lengths (4 -5.2pm) and leads to large reductions in effective work function (0.3 – 0.43eV) via the Schottky effect. Consequently, simple work function lowering compounds such as lanthanum hexaboride (LaB6) can be used to reduce operating temperature without the significant manufacturing complexity of producing porous impregnated thermionic emitters as with macro scale hollow cathodes, while still operating <1200°C at the emitter surface. The literature shows that LaB6 can be deposited using a variety of standard microfabrication techniques

Dynamics of frequency-swept nuclear spin optical pumping in powdered diamond at low magnetic fields

A broad effort is underway to improve the sensitivity of NMR through the use of dynamic nuclear polarization. Nitrogen vacancy (NV) centers in diamond offer an appealing platform because these paramagnetic defects can be optically polarized efficiently at room temperature. However, work thus far has been mainly limited to single crystals, because most polarization transfer protocols are sensitive to misalignment between the NV and magnetic field axes. Here we study the spin dynamics of NV− 13 C pairs in the simultaneous presence of optical excitation and microwave frequency sweeps at low magnetic fields. We show that a subtle interplay between illumination intensity, frequency sweep rate, and hyperfine coupling strength leads to efficient, sweep-direction-dependent 13 C spin polarization over a broad range of orientations of the magnetic field. In particular, our results strongly suggest that finely tuned, moderately coupled nuclear spins are key to the hyperpolarization process, which makes this mechanism distinct from other known dynamic polarization channels. These findings pave the route to applications where powders are intrinsically advantageous, including the hyperpolarization of target fluids in contact with the diamond surface or the use of hyperpolarized particles as contrast agents for in vivo imaging.Fil: Zangara, Pablo René. City University of New York; Estados Unidos. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Física Enrique Gaviola. Universidad Nacional de Córdoba. Instituto de Física Enrique Gaviola; ArgentinaFil: Dhomkar, Siddharth. City University of New York; Estados UnidosFil: Ajoy, Ashok. University of California at Berkeley; Estados Unidos. Lawrence Berkeley National Laboratory; Estados UnidosFil: Liu, Kristina. University of California at Berkeley; Estados Unidos. Lawrence Berkeley National Laboratory; Estados UnidosFil: Nazaryan, Raffi. Lawrence Berkeley National Laboratory; Estados Unidos. University of California at Berkeley; Estados UnidosFil: Pagliero, Daniela. City University of New York; Estados UnidosFil: Suter, Dieter. Universität Dortmund; AlemaniaFil: Reimer, Jeffrey A.. University of California at Berkeley; Estados Unidos. Lawrence Berkeley National Laboratory; Estados UnidosFil: Pines, Alexander. Lawrence Berkeley National Laboratory; Estados Unidos. University of California at Berkeley; Estados UnidosFil: Meriles, Carlos A.. City University of New York; Estados Unido

Nanotechnology for catalysis and solar energy conversion

This roadmap on Nanotechnology for Catalysis and Solar Energy Conversion focuses on the application of nanotechnology in addressing the current challenges of energy conversion: 'high efficiency, stability, safety, and the potential for low-cost/scalable manufacturing' to quote from the contributed article by Nathan Lewis. This roadmap focuses on solar-to-fuel conversion, solar water splitting, solar photovoltaics and bio-catalysis. It includes dye-sensitized solar cells (DSSCs), perovskite solar cells, and organic photovoltaics. Smart engineering of colloidal quantum materials and nanostructured electrodes will improve solar-to-fuel conversion efficiency, as described in the articles by Waiskopf and Banin and Meyer. Semiconductor nanoparticles will also improve solar energy conversion efficiency, as discussed by Boschloo et al in their article on DSSCs. Perovskite solar cells have advanced rapidly in recent years, including new ideas on 2D and 3D hybrid halide perovskites, as described by Spanopoulos et al 'Next generation' solar cells using multiple exciton generation (MEG) from hot carriers, described in the article by Nozik and Beard, could lead to remarkable improvement in photovoltaic efficiency by using quantization effects in semiconductor nanostructures (quantum dots, wires or wells). These challenges will not be met without simultaneous improvement in nanoscale characterization methods. Terahertz spectroscopy, discussed in the article by Milot et al is one example of a method that is overcoming the difficulties associated with nanoscale materials characterization by avoiding electrical contacts to nanoparticles, allowing characterization during device operation, and enabling characterization of a single nanoparticle. Besides experimental advances, computational science is also meeting the challenges of nanomaterials synthesis. The article by Kohlstedt and Schatz discusses the computational frameworks being used to predict structure–property relationships in materials and devices, including machine learning methods, with an emphasis on organic photovoltaics. The contribution by Megarity and Armstrong presents the 'electrochemical leaf' for improvements in electrochemistry and beyond. In addition, biohybrid approaches can take advantage of efficient and specific enzyme catalysts. These articles present the nanoscience and technology at the forefront of renewable energy development that will have significant benefits to society

Transient Photophysics of Bismuth Halide Semiconductors for Optoelectronic Applications

This thesis describes a series of spectroscopic studies of three different semiconductors based on bismuth halides in order to discover their fundamental photophysical properties. The materials investigated — the double perovskite Cs2AgBiBr6, bismuth iodide, and bismuth oxyiodide — have all been demonstrated in thin film photovoltaic devices fabricated at low temperatures. Propelled by the success of lead halide perovskites, this work forms part of the search for defect tolerant, non-toxic and stable materials for next-generation solar cells. I use transient absorption spectroscopy to show that the charge carrier lifetime in Cs2AgBiBr6 thin films is 1.4 μs. This is significantly longer than previous estimates based on time-resolved photoluminescence measurements, which measure the radiatively decaying carriers, but is a less sensitive probe of the high proportion of carriers which recombine non-radiatively. I propose a radiative recombination mechanism via defects, based on the detection of mid-gap electronic states in the transient absorption spectra. Coherent phonon transients are also measured on ultrafast timescales showing strong electron-phonon coupling in the material, which may contribute to the slow recombination in this material. The recombination dynamics of excitons in the layered material bismuth iodide, BiI3, are investigated using temperature dependent photoluminescence and transient absorption. I show that coupling to interlayer and intralayer phonon modes strongly affects the direct exciton decay pathway through scattering and modulation of the band gap energy. In a single crystal of BiI3, the room temperature exciton lifetime is 72 ns, which indicates this material’s potential for photovoltaics if the defects in thin films can be passivated. I show that the excited states of thin films of layered bismuth oxyiodide, BiOI, have a great degree of energetic disorder, most likely due to the presence of self-trapped excitons and defect states. Transient absorption measurements give an excited state lifetime of 47 ps, which would make efficient photovoltaic performance of BiOI thin film absorbers very unlikely. On the basis of my findings, all three materials show strong coupling between phonons and electronic states, but have excited state lifetimes varying over many orders of magnitude. This should guide the direction of future research towards different applications: the most promising candidate for photovoltaic applications is therefore Cs2AgBiBr6, whereas BiI3 and BiOI have more potential for use in nanostructured devices, such as ultrathin photodetectors, which can exploit their anisotropic nature