Higher-Order Photon Statistics as a New Tool to Reveal Hidden Excited States in a Plasmonic Cavity

Among the best known quantities obtainable from photon correlation measurements are the $g^{(m)}$~correlation functions. Here, we introduce a new procedure to evaluate these correlation functions based on higher-order factorial cumulants $C_{\text{F},m}$ which integrate over the time dependence of the correlation functions, i.e., summarize the available information at different time spans. In a systematic manner, the information content of higher-order correlation functions as well as the distribution of photon waiting times is taken into account. Our procedure greatly enhances the sensitivity for probing correlations and, moreover, is robust against a limited counting efficiency and time resolution in experiment. It can be applied even in case $g^{(m)}$ is not accessible at short time spans. We use the new evaluation scheme to analyze the photon emission of a plasmonic cavity coupled to a single quantum dot. We derive criteria which must hold if the system can be described by a generic Jaynes-Cummings model. A violation of the criteria can be explained by the presence of an additional excited quantum dot state.Comment: 10 pages manuscript + 9 pages supporting informatio

Metallic monoclinic phase in VO2_2 induced by electrochemical gating: in-situ Raman study

We report in-situ Raman scattering studies of electrochemically top gated VO$_2$ thin film to address metal-insulator transition (MIT) under gating. The room temperature monoclinic insulating phase goes to metallic state at a gate voltage of 2.6 V. However, the number of Raman modes do not change with electrolyte gating showing that the metallic phase is still monoclinic. The high frequency Raman mode A$_g$(7) near 616 cm$^{-1}$ ascribed to V-O vibration of bond length 2.06 \AA~ in VO$_6$ octahedra hardens with increasing gate voltage and the B$_g$(3) mode near 654 cm$^{-1}$ softens. This shows that the distortion of the VO$_6$ octahedra in the monoclinic phase decreases with gating. The time dependent Raman data at fixed gate voltages of 1 V (for 50 minute, showing enhancement of conductivity by a factor of 50) and 2 V (for 130 minute, showing further increase in conductivity by a factor of 5) show similar changes in high frequency Raman modes A$_g$(7) and B$_g$(3) as observed in gating. This slow change in conductance together with Raman frequency changes show that the governing mechanism for metalization is more likely to the diffusion controlled oxygen vacancy formation due to the applied electric field.Comment: 5 pages, 6 figure

Raman anomalies as signatures of pressure induced electronic topological and structural transitions in black phosphorus: Experiments and Theory

We report high pressure Raman experiments of Black phosphorus up to 24 GPa. The line widths of first order Raman modes A$^1_g$, B$_{2g}$ and A$^2_g$ of the orthorhombic phase show a minimum at 1.1 GPa. Our first-principles density functional analysis reveals that this is associated with the anomalies in electron-phonon coupling at the semiconductor to topological insulator transition through inversion of valence and conduction bands marking a change from trivial to nontrivial electronic topology. The frequencies of B$_{2g}$ and A$^2_g$ modes become anomalous in the rhombohedral phase at 7.4 GPa, and new modes appearing in the rhombohedral phase show anomalous softening with pressure. This is shown to originate from unusual structural evolution of black phosphorous with pressure, based on first-principles theoretical analysis.Comment: 13pages, 12figure

Electron-Hole Asymmetry in the Electron-phonon Coupling in Top-gated Phosphorene Transistor

Using in-situ Raman scattering from phosphorene channel in an electrochemically top-gated field effect transistor, we show that its phonons with A$_g$ symmetry depend much more strongly on concentration of electrons than that of holes, while the phonons with B$_g$ symmetry are insensitive to doping. With first-principles theoretical analysis, we show that the observed electon-hole asymmetry arises from the radically different constitution of its conduction and valence bands involving $\pi$ and $\sigma$ bonding states respectively, whose symmetry permits coupling with only the phonons that preserve the lattice symmetry. Thus, Raman spectroscopy is a non-invasive tool for measuring electron concentration in phosphorene-based nanoelectronic devices

Complex plasmon-exciton dynamics revealed through quantum dot light emission in a nanocavity

Plasmonic cavities can confine electromagnetic radiation to deep sub-wavelength regimes. This facilitates strong coupling phenomena to be observed at the limit of individual quantum emitters. Here, we report an extensive set of measurements of plasmonic cavities hosting one to a few semiconductor quantum dots. Scattering spectra show Rabi splitting, demonstrating that these devices are close to the strong coupling regime. Using Hanbury Brown and Twiss interferometry, we observe non-classical emission, allowing us to directly determine the number of emitters in each device. Surprising features in photoluminescence spectra point to the contribution of multiple excited states. Using model simulations based on an extended Jaynes-Cummings Hamiltonian, we find that the involvement of a dark state of the quantum dots explains the experimental findings. The coupling of quantum emitters to plasmonic cavities thus exposes complex relaxation pathways and emerges as an unconventional means to control dynamics of quantum states.S.N.G. thanks the Government of Israel for a Planning and Budgeting Committee Fel-lowship. G.H. is the incumbent of the Hilda Pomeraniec Memorial Professorial Chair.R.E., T.N. and J.A. acknowledge funding from projects FIS2016-80174-P and PID2019-107432GB-I00 of the Spanish Ministry of Science, Innovation and Universities MICINN,as well as funding from grant IT1164-19 for consolidated groups of the Basque Uni-versity, through the Department of Universities of the Basque Government. This projectreceived partial support from the European Union’s Horizon 2020 research and inno-vation programme under grant agreement no. 861950, project POSEIDON, and grantagreement no. 810626, project SINNCE. We thank Garnett W. Bryant and PeterNordlander for stimulating discussion

Raman Signatures of Strong Kitaev Exchange Correlations in (Na1−x_{1-x}Lix_x)2_2IrO3_3 : Experiments and Theory

Inelastic light scattering studies on single crystals of (Na$_{1-x}$Li$_x$)$_2$IrO$_3$ ($x = 0, 0.05$ and $0.15$) show a polarization independent broad band at $\sim$~2750 cm$^{-1}$ with a large band-width $\sim 1800$~cm$^{-1}$. For Na$_2$IrO$_3$ the broad band is seen for temperatures $\leq 200$~K and persists inside the magnetically ordered state. For Li doped samples, the intensity of this mode increases, shifts to lower wave-numbers and persists to higher temperatures. Such a mode has recently been predicted (Knolle et.al.) as a signature of the Kitaev spin liquid. We assign the observation of the broad band to be a signature of strong Kitaev-exchange correlations. The fact that the broad band persists even inside the magnetically ordered state suggests that dynamically fluctuating moments survive even below $T_{N}$. This is further supported by our mean field calculations. The Raman response calculated in mean field theory shows that the broad band predicted for the spin liquid state survives in the magnetically ordered state near the zigzag-spin liquid phase boundary. A comparison with the theoretical model gives an estimate of the Kitaev exchange interaction parameter to be $J_K\approx 57$~meV.Comment: 14pages 4 figure

Complex plasmon-exciton dynamics revealed through quantum dot light emission in a nanocavity

Plasmonic cavities can confine electromagnetic radiation to deep sub-wavelength regimes. This facilitates strong coupling phenomena to be observed at the limit of individual quantum emitters. Here, we report an extensive set of measurements of plasmonic cavities hosting one to a few semiconductor quantum dots. Scattering spectra show Rabi splitting, demonstrating that these devices are close to the strong coupling regime. Using Hanbury Brown and Twiss interferometry, we observe non-classical emission, allowing us to directly determine the number of emitters in each device. Surprising features in photoluminescence spectra point to the contribution of multiple excited states. Using model simulations based on an extended Jaynes-Cummings Hamiltonian, we find that the involvement of a dark state of the quantum dots explains the experimental findings. The coupling of quantum emitters to plasmonic cavities thus exposes complex relaxation pathways and emerges as an unconventional means to control dynamics of quantum states.S.N.G. thanks the Government of Israel for a Planning and Budgeting Committee Fel-lowship. G.H. is the incumbent of the Hilda Pomeraniec Memorial Professorial Chair.R.E., T.N. and J.A. acknowledge funding from projects FIS2016-80174-P and PID2019-107432GB-I00 of the Spanish Ministry of Science, Innovation and Universities MICINN,as well as funding from grant IT1164-19 for consolidated groups of the Basque Uni-versity, through the Department of Universities of the Basque Government. This projectreceived partial support from the European Union’s Horizon 2020 research and inno-vation programme under grant agreement no. 861950, project POSEIDON, and grantagreement no. 810626, project SINNCE. We thank Garnett W. Bryant and PeterNordlander for stimulating discussion

Vacuum Rabi splitting of a dark plasmonic cavity mode revealed by fast electrons

Recent years have seen a growing interest in strong coupling between plasmons and excitons, as a way to generate new quantum optical testbeds and influence chemical dynamics and reactivity. Strong coupling to bright plasmonic modes has been achieved even with single quantum emitters. Dark plasmonic modes fare better in some applications due to longer lifetimes, but are difficult to probe as they are subradiant. Here, we apply electron energy loss (EEL) spectroscopy to demonstrate that a dark mode of an individual plasmonic bowtie can interact with a small number of quantum emitters, as evidenced by Rabi-split spectra. Coupling strengths of up to 85meV place the bowtie-emitter devices at the onset of the strong coupling regime. Remarkably, the coupling occurs at the periphery of the bowtie gaps, even while the electron beam probes their center. Our findings pave the way for using EEL spectroscopy to study exciton-plasmon interactions involving non-emissive photonic modes

31st Annual Meeting and Associated Programs of the Society for Immunotherapy of Cancer (SITC 2016) : part two

Background The immunological escape of tumors represents one of the main ob- stacles to the treatment of malignancies. The blockade of PD-1 or CTLA-4 receptors represented a milestone in the history of immunotherapy. However, immune checkpoint inhibitors seem to be effective in specific cohorts of patients. It has been proposed that their efficacy relies on the presence of an immunological response. Thus, we hypothesized that disruption of the PD-L1/PD-1 axis would synergize with our oncolytic vaccine platform PeptiCRAd. Methods We used murine B16OVA in vivo tumor models and flow cytometry analysis to investigate the immunological background. Results First, we found that high-burden B16OVA tumors were refractory to combination immunotherapy. However, with a more aggressive schedule, tumors with a lower burden were more susceptible to the combination of PeptiCRAd and PD-L1 blockade. The therapy signifi- cantly increased the median survival of mice (Fig. 7). Interestingly, the reduced growth of contralaterally injected B16F10 cells sug- gested the presence of a long lasting immunological memory also against non-targeted antigens. Concerning the functional state of tumor infiltrating lymphocytes (TILs), we found that all the immune therapies would enhance the percentage of activated (PD-1pos TIM- 3neg) T lymphocytes and reduce the amount of exhausted (PD-1pos TIM-3pos) cells compared to placebo. As expected, we found that PeptiCRAd monotherapy could increase the number of antigen spe- cific CD8+ T cells compared to other treatments. However, only the combination with PD-L1 blockade could significantly increase the ra- tio between activated and exhausted pentamer positive cells (p= 0.0058), suggesting that by disrupting the PD-1/PD-L1 axis we could decrease the amount of dysfunctional antigen specific T cells. We ob- served that the anatomical location deeply influenced the state of CD4+ and CD8+ T lymphocytes. In fact, TIM-3 expression was in- creased by 2 fold on TILs compared to splenic and lymphoid T cells. In the CD8+ compartment, the expression of PD-1 on the surface seemed to be restricted to the tumor micro-environment, while CD4 + T cells had a high expression of PD-1 also in lymphoid organs. Interestingly, we found that the levels of PD-1 were significantly higher on CD8+ T cells than on CD4+ T cells into the tumor micro- environment (p < 0.0001). Conclusions In conclusion, we demonstrated that the efficacy of immune check- point inhibitors might be strongly enhanced by their combination with cancer vaccines. PeptiCRAd was able to increase the number of antigen-specific T cells and PD-L1 blockade prevented their exhaus- tion, resulting in long-lasting immunological memory and increased median survival