86 research outputs found
Surface Doping Quantum Dots with Chemically Active Native Ligands: Controlling Valence without Ligand Exchange
One remaining challenge in the field of colloidal semiconductor nanocrystal quantum dots is learning to control the degree of functionalization or valence per nanocrystal. Current quantum dot surface modification strategies rely heavily on ligand exchange, which consists of replacing the nanocrystal\u27s native ligands with carboxylate- or amine-terminated thiols, usually added in excess. Removing the nanocrystal\u27s native ligands can cause etching and introduce surface defects, thus affecting the nanocrystal\u27s optical properties. More importantly, ligand exchange methods fail to control the extent of surface modification or number of functional groups introduced per nanocrystal. Here, we report a fundamentally new surface ligand modification or doping approach aimed at controlling the degree of functionalization or valence per nanocrystal while retaining the nanocrystal\u27s original colloidal and photostability. We show that surface-doped quantum dots capped with chemically active native ligands can be prepared directly from a mixture of ligands with similar chain lengths. Specifically, vinyl and azide-terminated carboxylic acid ligands survive the high temperatures needed for nanocrystal synthesis. The ratio between chemically active and inactive-terminated ligands is maintained on the nanocrystal surface, allowing to control the extent of surface modification by straightforward organic reactions. Using a combination of optical and structural characterization tools, including IR and 2D NMR, we show that carboxylates bind in a bidentate chelate fashion, forming a single monolayer of ligands that are perpendicular to the nanocrystal surface. Moreover, we show that mixtures of ligands with similar chain lengths homogeneously distribute themselves on the nanocrystal surface. We expect this new surface doping approach will be widely applicable to other nanocrystal compositions and morphologies, as well as to many specific applications in biology and materials science
Molecular Chemistry to the Fore: New Insights into the Fascinating World of Photoactive Colloidal Semiconductor Nanocrystals
Colloidal semiconductor nanocrystals possess unique properties that are unmatched by other chromophores such as organic dyes or transition-metal complexes. These versatile building blocks have generated much scientific interest and found applications in bioimaging, tracking, lighting, lasing, photovoltaics, photocatalysis, thermoelectrics, and spintronics. Despite these advances, important challenges remain, notably how to produce semiconductor nanostructures with predetermined architecture, how to produce metastable semiconductor nanostructures that are hard to isolate by conventional syntheses, and how to control the degree of surface loading or valence per nanocrystal. Molecular chemists are very familiar with these issues and can use their expertise to help solve these challenges. In this Perspective, we present our group\u27s recent work on bottom-up molecular control of nanoscale composition and morphology, low-temperature photochemical routes to semiconductor heterostructures and metastable phases, solar-to-chemical energy conversion with semiconductor-based photocatalysts, and controlled surface modification of colloidal semiconductors that bypasses ligand exchange
Multimessenger Gamma-Ray and Neutrino Coincidence Alerts using HAWC and IceCube sub-threshold Data
The High Altitude Water Cherenkov (HAWC) and IceCube observatories, through
the Astrophysical Multimessenger Observatory Network (AMON) framework, have
developed a multimessenger joint search for extragalactic astrophysical
sources. This analysis looks for sources that emit both cosmic neutrinos and
gamma rays that are produced in photo-hadronic or hadronic interactions. The
AMON system is running continuously, receiving sub-threshold data (i.e. data
that is not suited on its own to do astrophysical searches) from HAWC and
IceCube, and combining them in real-time. We present here the analysis
algorithm, as well as results from archival data collected between June 2015
and August 2018, with a total live-time of 3.0 years. During this period we
found two coincident events that have a false alarm rate (FAR) of
coincidence per year, consistent with the background expectations. The
real-time implementation of the analysis in the AMON system began on November
20th, 2019, and issues alerts to the community through the Gamma-ray
Coordinates Network with a FAR threshold of coincidences per year.Comment: 14 pages, 5 figures, 3 table
A muon-track reconstruction exploiting stochastic losses for large-scale Cherenkov detectors
IceCube is a cubic-kilometer Cherenkov telescope operating at the South Pole.
The main goal of IceCube is the detection of astrophysical neutrinos and the
identification of their sources. High-energy muon neutrinos are observed via
the secondary muons produced in charge current interactions with nuclei in the
ice. Currently, the best performing muon track directional reconstruction is
based on a maximum likelihood method using the arrival time distribution of
Cherenkov photons registered by the experiment's photomultipliers. A known
systematic shortcoming of the prevailing method is to assume a continuous
energy loss along the muon track. However at energies TeV the light yield
from muons is dominated by stochastic showers. This paper discusses a
generalized ansatz where the expected arrival time distribution is parametrized
by a stochastic muon energy loss pattern. This more realistic parametrization
of the loss profile leads to an improvement of the muon angular resolution of
up to for through-going tracks and up to a factor 2 for starting tracks
over existing algorithms. Additionally, the procedure to estimate the
directional reconstruction uncertainty has been improved to be more robust
against numerical errors
All-flavor constraints on nonstandard neutrino interactions and generalized matter potential with three years of IceCube DeepCore data
We report constraints on nonstandard neutrino interactions (NSI) from the observation of atmospheric neutrinos with IceCube, limiting all individual coupling strengths from a single dataset. Furthermore, IceCube is the first experiment to constrain flavor-violating and nonuniversal couplings simultaneously. Hypothetical NSI are generically expected to arise due to the exchange of a new heavy mediator particle. Neutrinos propagating in matter scatter off fermions in the forward direction with negligible momentum transfer. Hence the study of the matter effect on neutrinos propagating in the Earth is sensitive to NSI independently of the energy scale of new physics. We present constraints on NSI obtained with an all-flavor event sample of atmospheric neutrinos based on three years of IceCube DeepCore data. The analysis uses neutrinos arriving from all directions, with reconstructed energies between 5.6 GeV and 100 GeV. We report constraints on the individual NSI coupling strengths considered singly, allowing for complex phases in the case of flavor-violating couplings. This demonstrates that IceCube is sensitive to the full NSI flavor structure at a level competitive with limits from the global analysis of all other experiments. In addition, we investigate a generalized matter potential, whose overall scale and flavor structure are also constrained
Search for Quantum Gravity Using Astrophysical Neutrino Flavour with IceCube
Along their long propagation from production to detection, neutrino states
undergo quantum interference which converts their types, or flavours.
High-energy astrophysical neutrinos, first observed by the IceCube Neutrino
Observatory, are known to propagate unperturbed over a billion light years in
vacuum. These neutrinos act as the largest quantum interferometer and are
sensitive to the smallest effects in vacuum due to new physics. Quantum gravity
(QG) aims to describe gravity in a quantum mechanical framework, unifying
matter, forces and space-time. QG effects are expected to appear at the
ultra-high-energy scale known as the Planck energy, ~giga-electronvolts (GeV). Such a high-energy universe would have
existed only right after the Big Bang and it is inaccessible by human
technologies. On the other hand, it is speculated that the effects of QG may
exist in our low-energy vacuum, but are suppressed by the Planck energy as
(~GeV), (~GeV), or its higher powers. The coupling of particles to these
effects is too small to measure in kinematic observables, but the phase shift
of neutrino waves could cause observable flavour conversions. Here, we report
the first result of neutrino interferometry~\cite{Aartsen:2017ibm} using
astrophysical neutrino flavours to search for new space-time structure. We did
not find any evidence of anomalous flavour conversion in IceCube astrophysical
neutrino flavour data. We place the most stringent limits of any known
technologies, down to ~GeV, on the dimension-six operators
that parameterize the space-time defects for preferred astrophysical production
scenarios. For the first time, we unambiguously reach the signal region of
quantum-gravity-motivated physics.Comment: The main text is 7 pages with 3 figures and 1 table. The Appendix
includes 5 pages with 3 figure
Strong Constraints on Neutrino Nonstandard Interactions from TeV-Scale ν Disappearance at IceCube
We report a search for nonstandard neutrino interactions (NSI) using eight years of TeV-scale atmospheric muon neutrino data from the IceCube Neutrino Observatory. By reconstructing incident energies and zenith angles for atmospheric neutrino events, this analysis presents unified confidence intervals for the NSI parameter εμτ. The best-fit value is consistent with no NSI at a p value of 25.2%. With a 90% confidence interval of −0.0041≤εμτ≤0.0031 along the real axis and similar strength in the complex plane, this result is the strongest constraint on any NSI parameter from any oscillation channel to date
Anisotropic nanomaterials: structure, growth, assembly, and functions
Comprehensive knowledge over the shape of nanomaterials is a critical factor in designing devices with desired functions. Due to this reason, systematic efforts have been made to synthesize materials of diverse shape in the nanoscale regime. Anisotropic nanomaterials are a class of materials in which their properties are direction-dependent and more than one structural parameter is needed to describe them. Their unique and fine-tuned physical and chemical properties make them ideal candidates for devising new applications. In addition, the assembly of ordered one-dimensional (1D), two-dimensional (2D), and three-dimensional (3D) arrays of anisotropic nanoparticles brings novel properties into the resulting system, which would be entirely different from the properties of individual nanoparticles. This review presents an overview of current research in the area of anisotropic nanomaterials in general and noble metal nanoparticles in particular. We begin with an introduction to the advancements in this area followed by general aspects of the growth of anisotropic nanoparticles. Then we describe several important synthetic protocols for making anisotropic nanomaterials, followed by a summary of their assemblies, and conclude with major applications
Globally invariant metabolism but density-diversity mismatch in springtails.
Soil life supports the functioning and biodiversity of terrestrial ecosystems. Springtails (Collembola) are among the most abundant soil arthropods regulating soil fertility and flow of energy through above- and belowground food webs. However, the global distribution of springtail diversity and density, and how these relate to energy fluxes remains unknown. Here, using a global dataset representing 2470 sites, we estimate the total soil springtail biomass at 27.5 megatons carbon, which is threefold higher than wild terrestrial vertebrates, and record peak densities up to 2 million individuals per square meter in the tundra. Despite a 20-fold biomass difference between the tundra and the tropics, springtail energy use (community metabolism) remains similar across the latitudinal gradient, owing to the changes in temperature with latitude. Neither springtail density nor community metabolism is predicted by local species richness, which is high in the tropics, but comparably high in some temperate forests and even tundra. Changes in springtail activity may emerge from latitudinal gradients in temperature, predation and resource limitation in soil communities. Contrasting relationships of biomass, diversity and activity of springtail communities with temperature suggest that climate warming will alter fundamental soil biodiversity metrics in different directions, potentially restructuring terrestrial food webs and affecting soil functioning
Pesticide seed dressings can affect the activity of various soil organisms and reduce decomposition of plant material
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