89 research outputs found

    Model-independent determination of the carrier multiplication time constant in CdSe nanocrystals

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    The experimental determination of the carrier multiplication (CM) time constant is complicated by the fact that this process occurs within the initial few hundreds of femtoseconds after excitation and, in transient-absorption experiments, cannot be separated from the buildup time of the 1p-state population. This work provides an accurate theoretical determination of the electron relaxation lifetime during the last stage of the p-state buildup, in CdSe nanocrystals, in the presence of a single photogenerated hole (no CM) and of a hole plus an additional electron–hole pair (following CM). From the invariance of the 1p buildup time observed experimentally for excitations above and below the CM threshold producing hot carriers with the same average per-exciton excess energy, and the calculated corresponding variations in the electron decay time in the two cases, an estimate is obtained for the carrier multiplication time constant. Unlike previous estimates reported in the literature so far, this result is model-independent, i.e., is obtained without making any assumption on the nature of the mechanism governing carrier multiplication. It is then compared with the time constant calculated, as a function of the excitation energy, assuming an impact-ionization-like process for carrier multiplication (DCM). The two results are in good agreement and show that carrier multiplication can occur on timescales of the order of tens of femtoseconds at energies close to the observed onset. These findings, which are compatible with the fastest lifetime estimated experimentally, confirm the suitability of the impact-ionization model to explain carrier multiplication in CdSe nanocrystals

    The XMM Cluster Survey: Active Galactic Nuclei and Starburst Galaxies in XMMXCS J2215.9-1738 at z=1.46

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    We use Chandra X-ray and Spitzer infrared observations to explore the AGN and starburst populations of XMMXCS J2215.9-1738 at z=1.46, one of the most distant spectroscopically confirmed galaxy clusters known. The high resolution X-ray imaging reveals that the cluster emission is contaminated by point sources that were not resolved in XMM observations of the system, and have the effect of hardening the spectrum, leading to the previously reported temperature for this system being overestimated. From a joint spectroscopic analysis of the Chandra and XMM data, the cluster is found to have temperature T=4.1_-0.9^+0.6 keV and luminosity L_X=(2.92_-0.35^+0.24)x10^44 erg/s extrapolated to a radius of 2 Mpc. As a result of this revised analysis, the cluster is found to lie on the sigma_v-T relation, but the cluster remains less luminous than would be expected from self-similar evolution of the local L_X-T relation. Two of the newly discovered X-ray AGN are cluster members, while a third object, which is also a prominent 24 micron source, is found to have properties consistent with it being a high redshift, highly obscured object in the background. We find a total of eight >5 sigma 24 micron sources associated with cluster members (four spectroscopically confirmed, and four selected using photometric redshifts), and one additional 24 micron source with two possible optical/near-IR counterparts that may be associated with the cluster. Examining the IRAC colors of these sources, we find one object is likely to be an AGN. Assuming that the other 24 micron sources are powered by star formation, their infrared luminosities imply star formation rates ~100 M_sun/yr. We find that three of these sources are located at projected distances of <250 kpc from the cluster center, suggesting that a large amount of star formation may be taking place in the cluster core, in contrast to clusters at low redshift.Comment: Accepted for publication in ApJ, 16 pages, 10 figure

    Theory of multiexciton generation in semiconductor nanocrystals

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    We develop a generalized framework based on a Green's function formalism to calculate the efficiency of multiexciton gen-eration in nanocrystal quantum dots. The direct/indirect absorption and coherent/incoherent impact ionization mechanisms, often used to describe multiexciton generation in nanocrystals, are reviewed and rederived from the unified theory as certain approximations. In addition, two new limits are described systematically - the weak Coulomb coupling limit and the semi-wide band limit. We show that the description of multiexciton generation in nanocrystals can be described as incoherent process and we discuss the scaling of multiexciton generation with respect to the photon energy and nanocrystal size. Illustrations are given for three prototype systems: CdSe, InAs and silicon quantum dots.Comment: 9 pages, 5 figure

    Distribution of carrier multiplication rates in CdSe and InAs nanocrystals

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    The distribution of rates of carrier multiplication (CM) following photon absorption is calculated for semiconductor nanocrystals (NCs). The NC electronic structure is described using a screened pseudopotential method known to give reliable description of NC excitons. The rates of biexciton generation are calculated using the Fermi golden rule with all relevant Coulomb matrix elements, taking into account proper selection rules. In CdSe and InAs NCs we find a broad distribution biexciton generation rates depending strongly on the exciton energy and size of the NC. The process becomes inefficient for NC exceeding 3 nm in diameter in the photon energy range of 2-3 times the band gap.Comment: 4 pages 3 fi

    Can impact excitation explain efficient carrier multiplication in carbon nanotube photodiodes?

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    We address recent experiments (Science 325, 1367 (2009)) reporting on highly efficient multiplication of electron-hole pairs in carbon nanotube photodiodes at photon energies near the carrier multiplication threshold (twice the quasi-particle band gap). This result is surprising in light of recent experimental and theoretical work on multiexciton generation in other confined materials, such as semiconducting nanocrystals. We propose a detailed mechanism based on carrier dynamics and impact excitation resulting in highly efficient multiplication of electron-hole pairs. We discuss the important time and energy scales of the problem and provide analysis of the role of temperature and the length of the diode

    Federated learning enables big data for rare cancer boundary detection.

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    Although machine learning (ML) has shown promise across disciplines, out-of-sample generalizability is concerning. This is currently addressed by sharing multi-site data, but such centralization is challenging/infeasible to scale due to various limitations. Federated ML (FL) provides an alternative paradigm for accurate and generalizable ML, by only sharing numerical model updates. Here we present the largest FL study to-date, involving data from 71 sites across 6 continents, to generate an automatic tumor boundary detector for the rare disease of glioblastoma, reporting the largest such dataset in the literature (n = 6, 314). We demonstrate a 33% delineation improvement for the surgically targetable tumor, and 23% for the complete tumor extent, over a publicly trained model. We anticipate our study to: 1) enable more healthcare studies informed by large diverse data, ensuring meaningful results for rare diseases and underrepresented populations, 2) facilitate further analyses for glioblastoma by releasing our consensus model, and 3) demonstrate the FL effectiveness at such scale and task-complexity as a paradigm shift for multi-site collaborations, alleviating the need for data-sharing

    Author Correction: Federated learning enables big data for rare cancer boundary detection.

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    10.1038/s41467-023-36188-7NATURE COMMUNICATIONS14

    Excited-State Dynamics in Colloidal Semiconductor Nanocrystals

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