604 research outputs found

    Theory for Nonlinear Spectroscopy of Vibrational Polaritons

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    Molecular polaritons have gained considerable attention due to their potential to control nanoscale molecular processes by harnessing electromagnetic coherence. Although recent experiments with liquid-phase vibrational polaritons have shown great promise for exploiting these effects, significant challenges remain in interpreting their spectroscopic signatures. In this letter, we develop a quantum-mechanical theory of pump-probe spectroscopy for this class of polaritons based on the quantum Langevin equations and the input-output theory. Comparison with recent experimental data shows good agreement upon consideration of the various vibrational anharmonicities that modulate the signals. Finally, a simple and intuitive interpretation of the data based on an effective mode-coupling theory is provided. Our work provides a solid theoretical framework to elucidate nonlinear optical properties of molecular polaritons as well as to analyze further multidimensional spectroscopy experiments on these systems

    Revealing Hidden Vibration Polariton Interactions by 2D IR Spectroscopy

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    We report the first experimental two-dimensional infrared (2D IR) spectra of novel molecular photonic excitations - vibrational-polaritons. The application of advanced 2D IR spectroscopy onto novel vibrational-polariton challenges and advances our understanding in both fields. From spectroscopy aspect, 2D IR spectra of polaritons differ drastically from free uncoupled molecules; from vibrational-polariton aspects, 2D IR uniquely resolves hybrid light-matter polariton excitations and unexpected dark states in a state-selective manner and revealed hidden interactions between them. Moreover, 2D IR signals highlight the role of vibrational anharmonicities in generating non-linear signals. To further advance our knowledge on 2D IR of vibrational polaritons, we develop a new quantum-mechanical model incorporating the effects of both nuclear and electrical anharmonicities on vibrational-polaritons and their 2D IR signals. This work reveals polariton physics that is difficult or impossible to probe with traditional linear spectroscopy and lays the foundation for investigating new non-linear optics and chemistry of molecular vibrational-polaritons

    Highly enantioselective access to diketopiperazines via cinchona alkaloid catalyzed Michael additions

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    Alkaloid catalysed additions to triketopiperazines gives products in high yield and er (88 : 12 to 99 : 1), including bridged hydroxy-DKPs via Michael-addition–ring closure.</p

    Two-dimensional Navier--Stokes simulation of deformation and break up of liquid patches

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    The large deformations and break up of circular 2D liquid patches in a high Reynolds number (Re=1000) gas flow are investigated numerically. The 2D, plane flow Navier--Stokes equations are directly solved with explicit tracking of the interface between the two phases and a new algorithm for surface tension. The numerical method is able to pursue the simulation beyond the breaking or coalescence of droplets. The simulations are able to unveil the intriguing details of the non-linear interplay between the deforming droplets and the vortical structures in the droplet's wake.Comment: 13 pages including 4 postscript figures; Revised version as resubmitted to PRL. Title has change

    Air entrainment through free-surface cusps

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    In many industrial processes, such as pouring a liquid or coating a rotating cylinder, air bubbles are entrapped inside the liquid. We propose a novel mechanism for this phenomenon, based on the instability of cusp singularities that generically form on free surfaces. The air being drawn into the narrow space inside the cusp destroys its stationary shape when the walls of the cusp come too close. Instead, a sheet emanates from the cusp's tip, through which air is entrained. Our analytical theory of this instability is confirmed by experimental observation and quantitative comparison with numerical simulations of the flow equations

    The prognostic significance of tumour-stroma ratio in oestrogen receptor-positive breast cancer

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    We are grateful to Breast Cancer Campaign for funding our collection of male breast carcinomas and for supporting DLH and SP. SAS was funded by the Wolfson Foundation and a Wellcome Trust Vacation Scholarship. HHT was funded by Cancer Research UK. We convey special thanks to members of the Leeds Breast Team for input and support at various stages of this project.Peer reviewedPublisher PD

    BET Bromodomain Inhibition Synergizes with PARP Inhibitor in Epithelial Ovarian Cancer

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    © 2017 The Author(s) PARP inhibition is known to be an effective clinical strategy in BRCA mutant cancers, but PARP inhibition has not been applied to BRCA-proficient tumors. Here, we show the synergy of BET bromodomain inhibition with PARP inhibition in BRCA-proficient ovarian cancers due to mitotic catastrophe. Treatment of BRCA-proficient ovarian cancer cells with the BET inhibitor JQ1 downregulated the G2-M cell-cycle checkpoint regulator WEE1 and the DNA-damage response factor TOPBP1. Combining PARP inhibitor Olaparib with the BET inhibitor, we observed a synergistic increase in DNA damage and checkpoint defects, which allowed cells to enter mitosis despite the accumulation of DNA damage, ultimately causing mitotic catastrophe. Moreover, JQ1 and Olaparib showed synergistic suppression of growth of BRCA-proficient cancer in vivo in a xenograft ovarian cancer mouse model. Our findings indicate that a combination of BET inhibitor and PARP inhibitor represents a potential therapeutic strategy for BRCA-proficient cancers. Karakashev et al. show synergy of BET bromodomain inhibition with PARP inhibition in BRCA-proficient ovarian cancers. This combination of inhibitors can synergistically increase DNA damage and cell-cycle checkpoint defects, which allows cells to enter mitosis despite the accumulation of DNA damage, ultimately causing mitotic catastrophe
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