Thermalization and breakdown of thermalization in photon condensates

The authors acknowledge financial support from EPSRC program “TOPNES” (Grant No. EP/I031014/1) and EPSRC (Grant No. EP/G004714/2). P.G.K. acknowledges support from EPSRC (Grant No. EP/M010910/1).We examine in detail the mechanisms behind thermalization and Bose-Einstein condensation (BEC) of a gas of photons in a dye-filled microcavity. We derive a microscopic quantum model, based on that of a standard laser, and show how this model can reproduce the behavior of recent experiments. Using the rate-equation approximation of this model, we show how a thermal distribution of photons arises. We go on to describe how the nonequilibrium effects in our model can cause thermalization to break down as one moves away from the experimental parameter values. In particular, we examine the effects of changing cavity length, and of altering the vibrational spectrum of the dye molecules. We are able to identify two measures which quantify whether the system is in thermal equilibrium. Using these, we plot “phase diagrams” distinguishing BEC and standard lasing regimes. Going beyond the rate-equation approximation, our quantum model allows us to investigate both the second-order coherence g(2) and the linewidth of the emission from the cavity. We show how the linewidth collapses as the system transitions to a Bose condensed state, and compare the results to the Schawlow-Townes linewidth.Publisher PDFPeer reviewe

Jacqueline Brunet, Grammaire critique de l\u27italien

We consider the orientational alignment of dipoles due to strong matter light coupling, for a non-vanishing density of excitations. We compare various approaches to this problem in the limit of large numbers of emitters, and show that direct Monte Carlo integration, mean-field theory, and large deviation methods match exactly in this limit. All three results show that orientational alignment develops in the presence of a macroscopically occupied polariton mode, and that the dipoles asymptotically approach perfect alignment in the limit of high density or low temperature.Comment: 7 pages, 4 figure

Superradiant and lasing states in driven-dissipative Dicke models

Funding: UK EPSRC (EP/M010910/1) (PK); EPSRC programs TOPNES (EP/I031014/1) and “Hybrid Polaritonics” (EP/M025330/1) (JK).We present the non-equilibrium phase diagram of a model which can demonstrate both Dicke-Hepp-Lieb superradiance and regular lasing by varying the coherent and incoherent driving terms. We find that the regions in the phase diagram corresponding to superradiance and standard lasing are always separated by a normal region. We analyse the behaviour of the system using a combination of exact numerics based on permutation symmetry of the density matrix for small to intermediate numbers of molecules, and second order cumulant equations for large numbers of molecules. We find that the nature of the photon distribution in the superradiant and lasing states are very similar, but the emission spectrum is very different. We also show that in the presence of both coherent and incoherent driving, a period-doubling route to a chaotic state occurs.Publisher PDFPeer reviewe

NHS-Functionalized THP Derivative for Efficient Synthesis of Kit-Based Precursors for 68Ga Labeled PET Probes

Hexadentate tris(3,4-hydroxypyridinone) ligands (THP) complex Fe3+ at very low iron concentrations and their high affinities for oxophilic trivalent metal ions have led to their development for new applications as bifunctional chelators for the radiometal gallium-68 (68Ga). THP-peptide bioconjugates rapidly and quantitatively complex 68Ga at room temperature, neutral pH, and micromolar ligand concentrations, making them amenable to kit-based radiosynthesis of 68Ga PET radiopharmaceuticals. With the aim to produce an N-hydroxysuccinimide-(NHS)-THP reagent for kit-based 68Ga-labeling and PET imaging, THP-derivatives were designed and synthesized to exploit the advantages of NHS chemistry for coupling with peptides, proteins, and antibodies. The more stable five-carbon atoms linker product was selected for a proof-of-concept conjugation and radiolabeling study with an anti-programmed death ligand 1 (PD-L1) camelid single domain antibody (sdAb) under mild conditions and further evaluated for site-specific amide bond formation with a synthesized glucagon-like peptide-1 (GLP-1) targeting peptide using solid-phase synthesis. The obtained THP-GLP-1 conjugate was tested for its 68Ga chelating ability, demonstrating to be a promising candidate for the detection and monitoring of GLP-1 aberrant malignancies. The obtained sdAb-THP conjugate was radiolabeled with 68Ga under mild conditions, providing sufficient labeling yields after 5 min, demonstrating that the novel NHS-THP bifunctional chelator can be widely used to easily conjugate the THP moiety to different targeting molecules (e.g., antibodies, anticalins, or peptides) under mild conditions, paving the way to the synthesis of different imaging probes with all the advantages of THP radiochemistry

⁶⁸Ga-Bisphosphonates for the Imaging of Extraosseous Calcification by Positron Emission Tomography

Abstract Radiolabelled bisphosphonates (BPs) and [18F]NaF (18F-fluoride) are the two types of radiotracers available to image calcium mineral (e.g. bone), yet only [18F]NaF has been widely explored for the non-invasive molecular imaging of extraosseous calcification (EC) using positron emission tomography (PET) imaging. These two radiotracers bind calcium mineral deposits via different mechanisms, with BPs chelating to calcium ions and thus being non-selective, and [18F]NaF being selective for hydroxyapatite (HAp) which is the main component of bone mineral. Considering that the composition of EC has been reported to include a diverse range of non-HAp calcium minerals, we hypothesised that BPs may be more sensitive for imaging EC due to their ability to bind to both HAp and non-HAp deposits. We report a comparison between the 68Ga-labelled BP tracer [68Ga]Ga-THP-Pam and [18F]NaF for PET imaging in a rat model of EC that develops macro- and microcalcifications in several organs. Macrocalcifications were identified using preclinical computed tomography (CT) and microcalcifications were identified using µCT-based 3D X-ray histology (XRH) on isolated organs ex vivo. The morphological and mineral analysis of individual calcified deposits was performed using scanning electron microscopy (SEM) and energy-dispersive X-ray spectroscopy (EDX). PET imaging and ex vivo analysis results demonstrated that while both radiotracers behave similarly for bone imaging, the BP-based radiotracer [68Ga]Ga-THP-Pam was able to detect EC more sensitively in several organs in which the mineral composition departs from that of HAp. Our results strongly suggest that BP-based PET radiotracers such as [68Ga]Ga-THP-Pam may have a particular advantage for the sensitive imaging and early detection of EC by being able to detect a wider array of relevant calcium minerals in vivo than [18F]NaF, and should be evaluated clinically for this purpose

68Ga-bisphosphonates for the imaging of extraosseous calcification by positron emission tomography

Radiolabelled bisphosphonates (BPs) and [18F]NaF (18F-fluoride) are the two types of radiotracers available to image calcium mineral (e.g. bone), yet only [18F]NaF has been widely explored for the non-invasive molecular imaging of extraosseous calcification (EC) using positron emission tomography (PET) imaging. These two radiotracers bind calcium mineral deposits via different mechanisms, with BPs chelating to calcium ions and thus being non-selective, and [18F]NaF being selective for hydroxyapatite (HAp) which is the main component of bone mineral. Considering that the composition of EC has been reported to include a diverse range of non-HAp calcium minerals, we hypothesised that BPs may be more sensitive for imaging EC due to their ability to bind to both HAp and non-HAp deposits. We report a comparison between the 68Ga-labelled BP tracer [68Ga]Ga-THP-Pam and [18F]NaF for PET imaging in a rat model of EC that develops macro- and microcalcifications in several organs. Macrocalcifications were identified using preclinical computed tomography (CT) and microcalcifications were identified using µCT-based 3D X-ray histology (XRH) on isolated organs ex vivo. The morphological and mineral analysis of individual calcified deposits was performed using scanning electron microscopy (SEM) and energy-dispersive X-ray spectroscopy (EDX). PET imaging and ex vivo analysis results demonstrated that while both radiotracers behave similarly for bone imaging, the BP-based radiotracer [68Ga]Ga-THP-Pam was able to detect EC more sensitively in several organs in which the mineral composition departs from that of HAp. Our results strongly suggest that BP-based PET radiotracers such as [68Ga]Ga-THP-Pam may have a particular advantage for the sensitive imaging and early detection of EC by being able to detect a wider array of relevant calcium minerals in vivo than [18F]NaF, and should be evaluated clinically for this purpose

Vaccination against Foot-and-mouth disease : do initial conditions affect its benefit?

When facing incursion of a major livestock infectious disease, the decision to implement a vaccination programme is made at the national level. To make this decision, governments must consider whether the benefits of vaccination are sufficient to outweigh potential additional costs, including further trade restrictions that may be imposed due to the implementation of vaccination. However, little consensus exists on the factors triggering its implementation on the field. This work explores the effect of several triggers in the implementation of a reactive vaccination-to-live policy when facing epidemics of foot-and-mouth disease. In particular, we tested whether changes in the location of the incursion and the delay of implementation would affect the epidemiological benefit of such a policy in the context of Scotland. To reach this goal, we used a spatial, premises-based model that has been extensively used to investigate the effectiveness of mitigation procedures in Great Britain. The results show that the decision to vaccinate, or not, is not straightforward and strongly depends on the underlying local structure of the population-at-risk. With regards to disease incursion preparedness, simply identifying areas of highest population density may not capture all complexities that may influence the spread of disease as well as the benefit of implementing vaccination. However, if a decision to vaccinate is made, we show that delaying its implementation in the field may markedly reduce its benefit. This work provides guidelines to support policy makers in their decision to implement, or not, a vaccination-to-live policy when facing epidemics of infectious livestock disease

Computational Framework for the Identification of Bioprivileged Molecules

Bioprivileged molecules are biology-derived chemical intermediates that can be efficiently converted to a diversity of chemical products including both novel molecules and drop-in replacements. Bridging chemical and biological catalysis by bioprivileged molecules provides a useful and flexible new paradigm for producing biobased chemicals. However, the discovery of bioprivileged molecules has been demonstrated to require extensive experimental effort over a long period of time. In this work, we developed a computational framework for identification of all possible C6HxOy molecules (29252) that can be honed down to a manageable number of candidate bioprivileged molecules based on analysis of structural features, reactive moieties, and reactivity of species, and the evaluation of the reaction network and resulting products based on automated network generation. Required input is the structure data file (SDF) of the starting molecules and the reaction rules. On-the-fly estimation of thermodynamics by a group contribution method is introduced as a screening criterion to identify the feasibility of reactions and pathways. Generated species are dynamically linked to the PubChem database for identification of novel products and evaluation of the known products as attractive candidates. Application of the proposed computational framework in screening 29252 C6 species and identifying a list of 100 C6HxOy bioprivileged molecule candidates is presented. Each of the 100 candidate molecules falls into one of nine broad compound classes and is typically composed of carbon atoms with a different chemical environment and, as a result, distinct reactivity patterns. Sensitivity analysis of the parameters used in the filtering steps leading to the candidate molecules that were identified is discussed, and analysis of favorable structural features, reactive moieties, and functionalities of C6HxOy candidate bioprivileged molecules is performed

The effects of changing climate on faunal depth distributions determine winners and losers

Changing climate is predicted to impact all depths of the global oceans, yet projections of range shifts in marine faunal distributions in response to changing climate seldom evaluate potential shifts in depth distribution. Marine ectotherms’ thermal tolerance is limited by their ability to maintain aerobic metabolism (oxygen- and capacity-limited tolerance), and is functionally associated with their hypoxia tolerance. Shallow-water (<200 m depth) marine invertebrates and fishes demonstrate limited tolerance of increasing hydrostatic pressure (pressure exerted by the overlying mass of water), and hyperbaric (increased pressure) tolerance is proposed to depend on the ability to maintain aerobic metabolism, too. Here, we report significant correlation between the hypoxia thresholds and the hyperbaric thresholds of taxonomic groups of shallow-water fauna, suggesting that pressure tolerance is indeed oxygen-limited. Consequently, it appears that the combined effects of temperature, pressure, and oxygen concentration constrain the fundamental ecological niches (FENs) of marine invertebrates and fishes. Including depth in a conceptual model of oxygen- and capacity-limited FENs’ responses to ocean warming and deoxygenation confirms previous predictions made based solely on consideration of the latitudinal effects of ocean warming (e.g. Cheung et al., 2009), that polar taxa are most vulnerable to the effects of climate change, with Arctic fauna experiencing the greatest FEN contraction. In contrast, the inclusion of depth in the conceptual model reveals for the first time that temperate fauna as well as tropical fauna may experience substantial FEN expansion with ocean warming and deoxygenation, rather than FEN maintenance or contraction suggested by solely considering latitudinal range shifts

Efficient non-Markovian quantum dynamics using time-evolving matrix product operators

AS acknowledges a studentship from EPSRC (EP/L505079/1). PK acknowledges support from EPSRC (EP/M010910/1). DK acknowledges support from the EPSRC CM-CDT (EP/L015110/1). JK acknowledges support from EPSRC programs "TOPNES" (EP/I031014/1) and "Hybrid Polaritonics" (EP/M025330/1). BWL acknowledges support from EPSRC (EP/K025562/1).In order to model realistic quantum devices it is necessary to simulate quantum systems strongly coupled to their environment. To date, most understanding of open quantum systems is restricted either to weak system-bath couplings or to special cases where specific numerical techniques become effective. Here we present a general and yet exact numerical approach that efficiently describes the time evolution of a quantum system coupled to a non-Markovian harmonic environment. Our method relies on expressing the system state and its propagator as a matrix product state and operator, respectively, and using a singular value decomposition to compress the description of the state as time evolves. We demonstrate the power and flexibility of our approach by numerically identifying the localisation transition of the Ohmic spin-boson model, and considering a model with widely separated environmental timescales arising for a pair of spins embedded in a common environment.Publisher PDFPeer reviewe