13 research outputs found
Ultrafast Tracking of Exciton and Charge Carrier Transport in Optoelectronic Materials on the Nanometer Scale.
We present a novel optical transient absorption and reflection microscope based on a diffraction-limited pump pulse in combination with a wide-field probe pulse, for the spatiotemporal investigation of ultrafast population transport in thin films. The microscope achieves a temporal resolution down to 12 fs and simultaneously provides sub-10 nm spatial accuracy. We demonstrate the capabilities of the microscope by revealing an ultrafast excited-state exciton population transport of up to 32 nm in a thin film of pentacene and by tracking the carrier motion in p-doped silicon. The use of few-cycle optical excitation pulses enables impulsive stimulated Raman microspectroscopy, which is used for in situ verification of the chemical identity in the 100-2000 cm-1 spectral window. Our methodology bridges the gap between optical microscopy and spectroscopy, allowing for the study of ultrafast transport properties down to the nanometer length scale.We acknowledge financial support from the EPSRC and the Winton Program for the Physics of Sustainability. This project has received funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (grant agreement No 758826). C.S. acknowledges financial support by the Royal Commission of the Exhibition of 1851
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Exciton-Phonon Interactions Govern Charge-Transfer-State Dynamics in CdSe/CdTe Two-Dimensional Colloidal Heterostructures.
CdSe/CdTe core-crown type-II nanoplatelet heterostructures are two-dimensional semiconductors that have attracted interest for use in light-emitting technologies due to their ease of fabrication, outstanding emission yields, and tunable properties. Despite this, the exciton dynamics of these complex materials, and in particular how they are influenced by phonons, is not yet well understood. Here, we use a combination of femtosecond vibrational spectroscopy, temperature-resolved photoluminescence (PL), and temperature-dependent structural measurements to investigate CdSe/CdTe nanoplatelets with a thickness of four monolayers. We show that charge-transfer (CT) excitons across the CdSe/CdTe interface are formed on two distinct time scales: initially from an ultrafast (∼70 fs) electron transfer and then on longer time scales (∼5 ps) from the diffusion of domain excitons to the interface. We find that the CT excitons are influenced by an interfacial phonon mode at ∼120 cm-1, which localizes them to the interface. Using low-temperature PL spectroscopy we reveal that this same phonon mode is the dominant mechanism in broadening the CT PL. On cooling to 4 K, the total PL quantum yield reaches close to unity, with an ∼85% contribution from CT emission and the remainder from an emissive sub-band-gap state. At room temperature, incomplete diffusion of domain excitons to the interface and scattering between CT excitons and phonons limit the PL quantum yield to ∼50%. Our results provide a detailed picture of the nature of exciton-phonon interactions at the interfaces of 2D heterostructures and explain both the broad shape of the CT PL spectrum and the origin of PL quantum yield losses. Furthermore, they suggest that to maximize the PL quantum yield both improved engineering of the interfacial crystal structure and diffusion of domain excitons to the interface, e.g., by altering the relative core/crown size, are required.We acknowledge financial support from the EPSRC [EP/M005143/1] and Winton Program for the Physics of Sustainability. The work of SI is supported by the program ANR JCJC NannoDoSe
Towards a tensionless string field theory for the N=(2,0) CFT in d=6
We describe progress in using the field theory of tensionless strings to
arrive at a Lagrangian for the six-dimensional conformal
theory. We construct the free part of the theory and propose an ansatz for the
cubic vertex in light-cone superspace. By requiring closure of the
supersymmetry algebra, we fix the cubic vertex up to two parameters.Comment: 46 pages, 2 figures. V2: references added; minor changes and
improvement
Microcavity-like exciton-polaritons can be the primary photoexcitation in bare organic semiconductors.
Strong-coupling between excitons and confined photonic modes can lead to the formation of new quasi-particles termed exciton-polaritons which can display a range of interesting properties such as super-fluidity, ultrafast transport and Bose-Einstein condensation. Strong-coupling typically occurs when an excitonic material is confided in a dielectric or plasmonic microcavity. Here, we show polaritons can form at room temperature in a range of chemically diverse, organic semiconductor thin films, despite the absence of an external cavity. We find evidence of strong light-matter coupling via angle-dependent peak splittings in the reflectivity spectra of the materials and emission from collective polariton states. We additionally show exciton-polaritons are the primary photoexcitation in these organic materials by directly imaging their ultrafast (5 × 106 m s-1), ultralong (~270 nm) transport. These results open-up new fundamental physics and could enable a new generation of organic optoelectronic and light harvesting devices based on cavity-free exciton-polaritons.EPSRC (EP/R025517/1),
EPSRC (EP/M025330/1),
ERC Horizon 2020 (grant agreements No 670405 and No 758826),
ERC (ERC-2014-STG H2020 639088),
Netherlands Organisation for Scientific Research,
Swedish Research Council (VR, 2014-06948),
Knut and Alice Wallenberg Foundation 3DEM-NATUR (no. 2012.0112),
Royal Commission for the Exhibition of 1851,
CNRS (France),
US Department of Energy, Office of Science, Basic Energy Sciences, CPIMS Program, Early Career Research Program (DE-SC0019188)
Genome-wide association analysis identifies six new loci associated with forced vital capacity
Forced vital capacity (FVC), a spirometric measure of pulmonary function, reflects lung volume and is used to diagnose and monitor lung diseases. We performed genome-wide association study meta-analysis of FVC in 52,253 individuals from 26 studies and followed up the top associations in 32,917 additional individuals of European ancestry. We found six new regions associated at genome-wide significance (P < 5 × 10−8) with FVC in or near EFEMP1, BMP6, MIR129-2–HSD17B12, PRDM11, WWOX and KCNJ2. Two loci previously associated with spirometric measures (GSTCD and PTCH1) were related to FVC. Newly implicated regions were followed up in samples from African-American, Korean, Chinese and Hispanic individuals. We detected transcripts for all six newly implicated genes in human lung tissue. The new loci may inform mechanisms involved in lung development and the pathogenesis of restrictive lung disease
CyPhyS plus : A Reliable and Managed Cyber-Physical System for Old-age Home Healthcare over a 6LoWPAN using Wearable Motes
We present design and implementation of CyPhyS+, a comprehensive, low-cost and standards compliant Cyber-Physical System (CPS) using 6LoWPAN based Internet of Things for remote health monitoring of elderly staying in old-age homes. It is a closed-loop system that incorporates an end-to-end reliable message transfer scheme for the resource constrained environment, data security, real-time medical signal processing and data analytics, and FHIR/HL7 compliant web services. The low power operation of CyPhyS+ allows the CPS an extended uptime, ensuring connectivity to the medical sensors, via the Internet, anytime/anywhere. The end-to-end reliable and secure messaging mechanism of CyPhyS+ does not necessitate intermediate application end-points at the old-age homes. This enables easy deployment with low operational overheads, scalability as well as easy introduction of newer applications or application upgrades. The paper describes system architecture, design and implementation details of software and hardware sub-systems. HealthMote, a power efficient Bluetooth-6LoWPAN mote was designed and deployed as a sub-system. We describe the novel low power end-to-end multi-stage message reliability scheme for UDP based sensor applications that does not require intermediate application-aware devices within the network. The experimental results presented show the efficacy of the approach. CyPhyS+ employs an application performance aware SNMP based network monitoring for robust operations of the 6LoWPAN multihop network. It incorporates a 128-bit AES, CBC-MAC based encryption and authentication mechanism for security and privacy. CyPhyS+ is compliant with FHIR/HL7 standards framework, with support for RESTful FHIR, and medical data analytics of ECG. We report on the extensive field trials carried out across a city
Singlet exciton fission via an intermolecular charge transfer state in coevaporated pentacene-perfluoropentacene thin films.
Singlet exciton fission is a spin-allowed process in organic semiconductors by which one absorbed photon generates two triplet excitons. Theory predicts that singlet fission is mediated by intermolecular charge-transfer states in solid-state materials with appropriate singlet-triplet energy spacing, but direct evidence for the involvement of such states in the process has not been provided yet. Here, we report on the observation of subpicosecond singlet fission in mixed films of pentacene and perfluoropentacene. By combining transient spectroscopy measurements to nonadiabatic quantum-dynamics simulations, we show that direct excitation in the charge-transfer absorption band of the mixed films leads to the formation of triplet excitons, unambiguously proving that they act as intermediate states in the fission process.I.S. acknowledges support from the Natural Sciences and Engineering Research Council of Canada (NSERC) (Funding Ref. No. RGPIN-2018-05092) and Concordia University. The authors thank the Winton Programme for the Physics of Sustainability and the Engineering and Physical Sciences Research Council for funding. The work in Mons was supported by Fonds de la Recherche Scientifique de Belgique (FNRS-F.R.S). Computational resources have been provided by the Consortium des Equipements de Calcul Intensif (CECI), funded by the F.R.S.-FNRS under Grant No. 2.5020.1 and by the Walloon Region. D.B. is FNRS research director