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Sample records for optically driven excitons

  1. Optically programmable excitonic traps

    PubMed Central

    Alloing, Mathieu; Lemaître, Aristide; Galopin, Elisabeth; Dubin, François

    2013-01-01

    With atomic systems, optically programmed trapping potentials have led to remarkable progress in quantum optics and quantum information science. Programmable trapping potentials could have a similar impact on studies of semiconductor quasi-particles, particularly excitons. However, engineering such potentials inside a semiconductor heterostructure remains an outstanding challenge and optical techniques have not yet achieved a high degree of control. Here, we synthesize optically programmable trapping potentials for indirect excitons of bilayer heterostructures. Our approach relies on the injection and spatial patterning of charges trapped in a field-effect device. We thereby imprint in-situ and on-demand electrostatic traps into which we optically inject cold and dense ensembles of excitons. This technique creates new opportunities to improve state-of-the-art technologies for the study of collective quantum behavior of excitons and also for the functionalisation of emerging exciton-based opto-electronic circuits. PMID:23546532

  2. Excitons and optical spectra of phosphorene nanoribbons

    NASA Astrophysics Data System (ADS)

    Nourbakhsh, Zahra; Asgari, Reza

    2016-07-01

    On the basis of many-body ab initio calculations, using the single-shot G0W0 method and Bethe-Salpeter equation, we study phosphorene nanoribbons (PNRs) in the two typical zigzag and armchair directions. The electronic structure, optical absorption, electron-hole (exciton) binding energy, exciton exchange splitting, and exciton wave functions are calculated for different sizes of PNRs. The typically strong splitting between singlet and triplet excitonic states make PNRs favorable systems for optoelectronic applications. Quantum confinement occurs in both kinds of PNRs, and it is stronger in the zPNRs, which behave like quasi-zero-dimensional systems. Scaling laws are investigated for the size-dependent behaviors of PNRs. The first bright excitonic state in PNRs is explored in detail.

  3. Temperature effects in excitonic condensation driven by the lattice distortion

    NASA Astrophysics Data System (ADS)

    Do, Thi-Hong-Hai; Nguyen, Huu-Nha; Nguyen, Thi-Giang; Phan, Van-Nham

    2016-06-01

    The stability of the excitonic condensation at low temperature driven by a coupling of electrons to vibrational degrees of freedom in semimetal two-dimensional electronic system is discussed. In the framework of the unrestricted Hartree-Fock approximation, we derive a set of equations to determine both the excitonic condensate order parameter and lattice displacement self-consistently. By lowering temperature we find out a semimetal-insulator transition in the system if the coupling is large enough. The insulating state typifies an excitonic condensation accompanied by a finite lattice distortion. Increasing temperature, both excitonic condensate order parameter and the lattice distortion decrease and then disappear in the same manner. Microscopic analysis in momentum space strongly specifies that the excitonic condensate driven by the lattice distortion favours the BCS type.

  4. Electro-optical properties of Rydberg excitons

    NASA Astrophysics Data System (ADS)

    Zielińska-Raczyńska, Sylwia; Ziemkiewicz, David; Czajkowski, Gerard

    2016-07-01

    We show how to compute the electro-optical functions (absorption, reflection, and transmission) when Rydberg exciton-polaritons appear, including the effect of the coherence between the electron-hole pair and the electromagnetic field. With the use of the real density matrix approach, numerical calculations applied for the Cu2O crystal are performed. We also examine in detail and explain the dependence of the resonance displacement on the state number and applied electric field strength. We report a fairly good agreement with recently published experimental data.

  5. Optical properties of Rydberg excitons and polaritons

    NASA Astrophysics Data System (ADS)

    Zielińska-Raczyńska, Sylwia; Czajkowski, Gerard; Ziemkiewicz, David

    2016-02-01

    We show how to compute the optical functions when Rydberg excitons appear, including the effect of the coherence between the electron-hole pair and the electromagnetic field. We use the real density matrix approach (RDMA), which, combined with the Green's function method, enables one to derive analytical expressions for the optical functions. Choosing the susceptibility, we performed numerical calculations appropriate to a Cu20 crystal, being a semiconductor with an indirect gap. The effect of the coherence is displayed in the line shape. We also examine in detail and explain the dependence of the oscillator strength and the resonance placement on the state number. We report good agreement with recently published experimental data. We also show that the presented method can be applied to semiconductors with a direct gap.

  6. Exciton states and optical properties of carbon nanotubes.

    PubMed

    Ajiki, Hiroshi

    2012-12-01

    Exciton states and related optical properties of a single-walled carbon nanotube are reviewed, primarily from a theoretical viewpoint. The energies and wavefunctions of excitons are discussed using a screened Hartree-Fock approximation with an effective-mass or k·p approximation. The close relationship between a long-range electron-hole exchange interaction and a depolarization effect is clarified. I discuss optical properties including the radiative lifetime of excitons, absorption spectra and radiation force. To describe these properties in a unified scheme, a self-consistent method is introduced for calculating the scattering light and induced current density due to excitons. I also briefly review experimental results on the Aharonov-Bohm effect in excitons and quasi-dark excitons excited by light polarized perpendicular to the tube axis. PMID:23139202

  7. Exciton Absorption in Semiconductor Quantum Wells Driven by a Strong Intersubband Pump Field

    NASA Technical Reports Server (NTRS)

    Liu, Ansheng; Ning, Cun-Zheng

    1999-01-01

    Optical interband excitonic absorption of semiconductor quantum wells (QW's) driven by a coherent pump field is investigated based on semiconductor Bloch equations. The pump field has a photon energy close to the intersubband spacing between the first two conduction subbands in the QW's. An external weak optical field probes the interband transition. The excitonic effects and pump-induced population redistribution within the conduction subbands in the QW system are included. When the density of the electron-hole pairs in the QW structure is low, the pump field induces an Autler-Townes splitting of the exciton absorption spectrum. The split size and the peak positions of the absorption doublet depend not only on the pump frequency and intensity but also on the carrier density. As the density of the electron-hole pairs is increased, the split contrast (the ratio between the maximum and minimum values) is decreased because the exciton effect is suppressed at higher densities due to the many-body screening.

  8. Terahertz driven intraband dynamics of excitons in nanorods

    NASA Astrophysics Data System (ADS)

    Sy, Fredrik

    Quantum dots and nanorods are becoming increasingly important structures due to their potential applications that range from photovoltaic devices to medicine. The majority of the research on carrier dynamics in these structures has been in the optical regime, with little work performed at Terahertz frequencies where excitonic dynamics can be more directly probed. In this work, we examine theoretically the interaction of Terahertz radiation with colloidal CdSe nanorods to determine the dynamics of excitons generated via a short optical pulse. We calculate the energies and wavefunctions for the excitons within the envelope function approximation in the low density limit where there is at most one exciton per nanorod. The linear Terahertz transmittance and absorbance is found for nanorods that are approximately 70 nm in length and 7 nm in diameter and are compared with experimental results that have shown the first observation of intra-excitonic transitions in nanorods. We find absorbance peaks at 8.5 THz and 11 THz that result from polarizations in the longitudinal (rod axis) and transverse directions respectively. Our theoretical results show that the 8.5 THz and 11 Thz peaks are due to 1s -- 2pz and 1s -- 2 px transitions respectively. The theoretical absorbance spectra is in good agreement with the experimental one and show that only the ground state is significantly populated 1 ps after optical excitation. This provides strong evidence of rapid trapping of excited holes into the ligand used to passivate the nanorods. A full set of dynamical equations were then constructed from Heisenberg's equation of motion, and were used to model the excitonic correlations as a function of time. Transmittance and absorbance were calculated for different nanorod orientations and electric field strengths in both the linear and nonlinear regime. These results were then averaged over nanorod orientation in order to more accurately reflect experimental conditions. Nonlinearity was

  9. A measurable force driven by an excitonic condensate

    SciTech Connect

    Hakioğlu, T.; Özgün, Ege; Günay, Mehmet

    2014-04-21

    Free energy signatures related to the measurement of an emergent force (≈10{sup −9}N) due to the exciton condensate (EC) in Double Quantum Wells are predicted and experiments are proposed to measure the effects. The EC-force is attractive and reminiscent of the Casimir force between two perfect metallic plates, but also distinctively different from it by its driving mechanism and dependence on the parameters of the condensate. The proposed experiments are based on a recent experimental work on a driven micromechanical oscillator. Conclusive observations of EC in recent experiments also provide a strong promise for the observation of the EC-force.

  10. Optical control of charged exciton states in tungsten disulfide

    NASA Astrophysics Data System (ADS)

    Currie, M.; Hanbicki, A. T.; Kioseoglou, G.; Jonker, B. T.

    2015-05-01

    A method is presented for optically preparing WS2 monolayers to luminescence from only the charged exciton (trion) state-completely suppressing the neutral exciton. When isolating the trion state, we observed changes in the Raman A1g intensity and an enhanced feature on the low energy side of the E12g peak. Photoluminescence and optical reflectivity measurements confirm the existence of the prepared trion state. This technique also prepares intermediate regimes with controlled luminescence amplitudes of the neutral and charged exciton. This effect is reversible by exposing the sample to air, indicating the change is mitigated by surface interactions with the ambient environment. This method provides a tool to modify optical emission energy and to isolate physical processes in this and other two-dimensional materials.

  11. Optical control of charged exciton states in tungsten disulfide

    SciTech Connect

    Currie, M.; Hanbicki, A. T.; Jonker, B. T.; Kioseoglou, G.

    2015-05-18

    A method is presented for optically preparing WS{sub 2} monolayers to luminescence from only the charged exciton (trion) state–completely suppressing the neutral exciton. When isolating the trion state, we observed changes in the Raman A{sub 1g} intensity and an enhanced feature on the low energy side of the E{sup 1}{sub 2g} peak. Photoluminescence and optical reflectivity measurements confirm the existence of the prepared trion state. This technique also prepares intermediate regimes with controlled luminescence amplitudes of the neutral and charged exciton. This effect is reversible by exposing the sample to air, indicating the change is mitigated by surface interactions with the ambient environment. This method provides a tool to modify optical emission energy and to isolate physical processes in this and other two-dimensional materials.

  12. Realization of an all optical exciton-polariton router

    NASA Astrophysics Data System (ADS)

    Marsault, Félix; Nguyen, Hai Son; Tanese, Dimitrii; Lemaître, Aristide; Galopin, Elisabeth; Sagnes, Isabelle; Amo, Alberto; Bloch, Jacqueline

    2015-11-01

    We report on the experimental realization of an all optical router for exciton-polaritons. This device is based on the design proposed by Flayac and Savenko [Appl. Phys. Lett. 103, 201105 (2013)], in which a zero-dimensional island is connected through tunnel barriers to two periodically modulated wires of different periods. Selective transmission of polaritons injected in the island, into either of the two wires, is achieved by tuning the energy of the island state across the band structure of the modulated wires. We demonstrate routing of ps polariton pulses using an optical control beam which controls the energy of the island quantum states, thanks to polariton-exciton interactions.

  13. Realization of an all optical exciton-polariton router

    SciTech Connect

    Marsault, Félix; Nguyen, Hai Son; Tanese, Dimitrii; Lemaître, Aristide; Galopin, Elisabeth; Sagnes, Isabelle; Amo, Alberto

    2015-11-16

    We report on the experimental realization of an all optical router for exciton-polaritons. This device is based on the design proposed by Flayac and Savenko [Appl. Phys. Lett. 103, 201105 (2013)], in which a zero-dimensional island is connected through tunnel barriers to two periodically modulated wires of different periods. Selective transmission of polaritons injected in the island, into either of the two wires, is achieved by tuning the energy of the island state across the band structure of the modulated wires. We demonstrate routing of ps polariton pulses using an optical control beam which controls the energy of the island quantum states, thanks to polariton-exciton interactions.

  14. Electrically driven optical antennas

    NASA Astrophysics Data System (ADS)

    Kern, Johannes; Kullock, René; Prangsma, Jord; Emmerling, Monika; Kamp, Martin; Hecht, Bert

    2015-09-01

    Unlike radiowave antennas, so far optical nanoantennas cannot be fed by electrical generators. Instead, they are driven by light or indirectly via excited discrete states in active materials in their vicinity. Here we demonstrate the direct electrical driving of an in-plane optical antenna by the broadband quantum-shot noise of electrons tunnelling across its feed gap. The spectrum of the emitted photons is determined by the antenna geometry and can be tuned via the applied voltage. Moreover, the direction and polarization of the light emission are controlled by the antenna resonance, which also improves the external quantum efficiency by up to two orders of magnitude. The one-material planar design offers facile integration of electrical and optical circuits and thus represents a new paradigm for interfacing electrons and photons at the nanometre scale, for example for on-chip wireless communication and highly configurable electrically driven subwavelength photon sources.

  15. Tunable optical delay via carrier induced exciton dephasing in semiconductor quantum wells.

    PubMed

    Sarkar, Susanta; Guo, Yan; Wang, Hailin

    2006-04-01

    We report the experimental realization of a tunable optical delay by exploiting unique incoherent nonlinear optical processes in semiconductors. The tunable optical delay takes advantage of the strong Coulomb interactions between excitons and free carriers and uses optical injection of free carriers to broaden and bleach an exciton absorption resonance. Fractional delay exceeding 200% has been obtained for an 8 ps optical pulse propagating near the heavy-hole excitonic transition in a GaAs quantum well structure. Tunable optical delay based on optical injection of free carriers avoids strong absorption of the pump beam and is also robust against variations in the frequency of the pump beam. PMID:19516421

  16. All-optical depletion of dark excitons from a semiconductor quantum dot

    SciTech Connect

    Schmidgall, E. R.; Schwartz, I.; Cogan, D.; Gershoni, D.; Gantz, L.; Heindel, T.; Reitzenstein, S.

    2015-05-11

    Semiconductor quantum dots are considered to be the leading venue for fabricating on-demand sources of single photons. However, the generation of long-lived dark excitons imposes significant limits on the efficiency of these sources. We demonstrate a technique that optically pumps the dark exciton population and converts it to a bright exciton population, using intermediate excited biexciton states. We show experimentally that our method considerably reduces the dark exciton population while doubling the triggered bright exciton emission, approaching thereby near-unit fidelity of quantum dot depletion.

  17. PREFACE: International Conference on Optics of Excitons in Confined Systems

    NASA Astrophysics Data System (ADS)

    Viña, Luis; Tejedor, Carlos; Calleja, José M.

    2010-01-01

    The OECS11 (International Conference on Optics of Excitons in Confined Systems) was the eleventh of a very successful series of conferences that started in 1987 in Rome (Italy). Afterwards the conference was held at Naxos (Sicily, Italy, 1991), Montpellier (France, 1993), Cortona (Italy, 1995), Göttingen (Germany, 1997), Ascona (Switzerland, 1999), Montpellier (France, 2001), Lecce (Italy, 2003), Southampton (UK, 2005) and Patti (Sicily, Italy, 2007). It is addressed to scientists who lead fundamental and applied research on the optical properties of excitons in novel condensed-matter nanostructures. The 2009 meeting (7-11 September 2009) has brought together a large representation of the world leading actors in this domain, with the aim of stimulating the exchange of ideas, promoting international collaborations, and coordinating research on the newest exciton-related issues such as quantum information science and exciton quantum-collective phenomena. The meeting has included invited lectures, contributed oral presentations and posters, covering the following general topics: low-dimensional heterostructures: quantum wells, quantum wires and quantum dots polaritons quantum optics with excitons and polaritons many-body effects under coherent and incoherent excitation coherent optical spectroscopy quantum coherence and quantum-phase manipulation Bose-Einstein condensation and other collective phenomena excitons in novel materials The OECS 11 was held at the campus of the Universidad Autónoma de Madrid in Cantoblanco. The scientific program was composed of more than 200 contributions divided into 16 invited talks, 44 oral contributions and 3 poster sessions with a total of 150 presentations. The scientific level of the presentations was guaranteed by a selection process where each contribution was rated by three members of the Program Committee. The Conference has gathered 238 participants from 21 different countries, with the following distribution: Germany (43

  18. CDW-Exciton Condensate Competition and a Condensate Driven Force

    NASA Astrophysics Data System (ADS)

    Özgün, Ege; Hakioğlu, Tuğrul

    2016-08-01

    We examine the competition between the charge-density wave (CDW) instability and the excitonic condensate (EC) in spatially separated layers of electrons and holes. The CDW and the EC order parameters (OPs), described by two different mechanisms and hence two different transition temperatures TcCDW and TcEC, are self-consistently coupled by a microscopic mean field theory. We discuss the results in our model specifically focusing on the transition-metal dichalcogenides which are considered as the most typical examples of strongly coupled CDW/EC systems with atomic layer separations where the electronic energy scales are large with the critical temperatures in the range TcEC ˜ TcCDW ˜ 100-200 K. An important consequence of this is that the excitonic energy gap, hence the condensed free energy, vary with the layer separation resulting in a new type of force FEC. We discuss the possibility of this force as the possible driver of the structural lattice deformation observed in some TMDCs with a particular attention on the 1T-TiSe2 below 200 K.

  19. Excitonic Effects and Optical Absorption Spectrum of Doped Graphene

    NASA Astrophysics Data System (ADS)

    Jornada, Felipe; Deslippe, Jack; Louie, Steven

    2012-02-01

    First-principles calculations based on the GW-Bethe-Salpeter Equation (GW-BSE) approach and subsequent experiments have shown large excitonic effects in the optical absorbance of graphene. Here we employ the GW-BSE formalism to probe the effects of charge carrier doping and of having an external electric field on the absorption spectrum of graphene. We show that the absorbance peak due to the resonant exciton exhibits systematic changes in both its position and profile when graphene is gate doped by carriers, in excellent agreement to very recent measurementsootnotetextTony F. Heinz, private communications.. We analyze the various contributions to these changes in the absorption spectrum, such as the effects of screening by carriers to the quasiparticle energies and electron-hole interactions. This work was supported by National Science Foundation Grant No. DMR10-1006184, the U.S. Department of Energy under Contract No. DE-AC02-05CH11231, and the U.S. DOD - Office of Naval Research under RTC Grant No. N00014-09-1-1066. Computer time was provided by NERSC.

  20. The excitonic insulator route through a dynamical phase transition induced by an optical pulse

    NASA Astrophysics Data System (ADS)

    Brazovskii, S.; Kirova, N.

    2016-03-01

    We consider a dynamical phase transition induced by a short optical pulse in a system prone to thermodynamical instability. We address the case of pumping to excitons whose density contributes directly to the order parameter. To describe both thermodynamic and dynamic effects on equal footing, we adopt a view of the excitonic insulator for the phase transition and suggest a formation of the Bose condensate for the pumped excitons. The work is motivated by experiments in donor-acceptor organic compounds with a neutral- ionic phase transition coupled to the spontaneous lattice dimerization and to charge transfer excitons. The double nature of the ensemble of excitons leads to an intricate time evolution, in particular, to macroscopic quantum oscillations from the interference between the Bose condensate of excitons and the ground state of the excitonic insulator. The coupling of excitons and the order parameter also leads to self-trapping of their wave function, akin to self-focusing in optics. The locally enhanced density of excitons can surpass a critical value to trigger the phase transformation, even if the mean density is below the required threshold. The system is stratified in domains that evolve through dynamical phase transitions and sequences of merging. The new circumstances in experiments and theory bring to life, once again, some remarkable inventions made by L.V. Keldysh.

  1. Optical lattices of excitons in InGaN/GaN quantum well systems

    SciTech Connect

    Chaldyshev, V. V. Bolshakov, A. S. Zavarin, E. E.; Sakharov, A. V.; Lundin, V. V.; Tsatsulnikov, A. F.; Yagovkina, M. A.

    2015-01-15

    Optical lattices of excitons in periodic systems of InGaN quantum wells with GaN barriers are designed, implemented, and investigated. Due to the collective interaction of quasi-two-dimensional excitons with light and a fairly high binding energy of excitons in GaN, optical Bragg reflection at room temperature is significantly enhanced. To increase the resonance optical response of the system, new structures with two quantum wells in a periodic supercell are designed and implemented. Resonance reflection of 40% at room temperatures for structures with 60 periods is demonstrated.

  2. Electronic and optical properties of exciton, trions and biexciton in II-VI parabolic quantum dot

    NASA Astrophysics Data System (ADS)

    Sujanah, P.; John Peter, A.; Woo Lee, Chang

    2015-08-01

    Binding energies of exciton, trions and biexciton and their interband optical transition energies are studied in a CdTe/ZnTe quantum dot nanostructure taking into consideration the geometrical confinement effect. The radial spread of the wavefunctions, binding energies, optical transition energies, oscillator strength, radiative life time and the absorption coefficients of exciton, positively and negatively charged excitons and biexciton are carried out. It is found that the ratio of the radiative life time of exciton with the trions and biexciton enhances with the reduction of geometrical confinement. The results show that (i) the binding energies of exciton, positive and negative trions and the biexciton have strong influence on the reduction of geometrical confinement effect, (ii) the binding energy is found to decrease from the binding energies of exciton to positive trion through biexciton and negative trion binding energies, (iii) the oscillator strength of trions is found to be lesser than exciton and the biexciton and (iv) the electronic and optical properties of exciton, trions and the biexciton are considerably dependent on the spatial confinement, incident photon energy and the radiative life time. The obtained results are in good agreement with the other existing literature.

  3. Hybrid optical-electrical detection of donor electron spins with bound excitons in silicon.

    PubMed

    Lo, C C; Urdampilleta, M; Ross, P; Gonzalez-Zalba, M F; Mansir, J; Lyon, S A; Thewalt, M L W; Morton, J J L

    2015-05-01

    Electrical detection of spins is an essential tool for understanding the dynamics of spins, with applications ranging from optoelectronics and spintronics, to quantum information processing. For electron spins bound to donors in silicon, bulk electrically detected magnetic resonance has relied on coupling to spin readout partners such as paramagnetic defects or conduction electrons, which fundamentally limits spin coherence times. Here we demonstrate electrical detection of donor electron spin resonance in an ensemble by transport through a silicon device, using optically driven donor-bound exciton transitions. We measure electron spin Rabi oscillations, and obtain long electron spin coherence times, limited only by the donor concentration. We also experimentally address critical issues such as non-resonant excitation, strain, and electric fields, laying the foundations for realizing a single-spin readout method with relaxed magnetic field and temperature requirements compared with spin-dependent tunnelling, enabling donor-based technologies such as quantum sensing. PMID:25799326

  4. Hybrid optical-electrical detection of donor electron spins with bound excitons in silicon

    NASA Astrophysics Data System (ADS)

    Lo, C. C.; Urdampilleta, M.; Ross, P.; Gonzalez-Zalba, M. F.; Mansir, J.; Lyon, S. A.; Thewalt, M. L. W.; Morton, J. J. L.

    2015-05-01

    Electrical detection of spins is an essential tool for understanding the dynamics of spins, with applications ranging from optoelectronics and spintronics, to quantum information processing. For electron spins bound to donors in silicon, bulk electrically detected magnetic resonance has relied on coupling to spin readout partners such as paramagnetic defects or conduction electrons, which fundamentally limits spin coherence times. Here we demonstrate electrical detection of donor electron spin resonance in an ensemble by transport through a silicon device, using optically driven donor-bound exciton transitions. We measure electron spin Rabi oscillations, and obtain long electron spin coherence times, limited only by the donor concentration. We also experimentally address critical issues such as non-resonant excitation, strain, and electric fields, laying the foundations for realizing a single-spin readout method with relaxed magnetic field and temperature requirements compared with spin-dependent tunnelling, enabling donor-based technologies such as quantum sensing.

  5. Optical properties of MgZnO alloys: Excitons and exciton-phonon complexes

    SciTech Connect

    Neumann, M. D.; Cobet, C.; Esser, N.; Laumer, B.; Wassner, T. A.; Eickhoff, M.; Feneberg, M.; Goldhahn, R.

    2011-07-01

    The characteristics of the excitonic absorption and emission around the fundamental bandgap of wurtzite Mg{sub x}Zn{sub 1-x}O grown on c-plane sapphire substrates by plasma assisted molecular beam epitaxy with Mg contents between x = 0 and x = 0.23 are studied using spectroscopic ellipsometry and photoluminescence (PL) measurements. The ellipsometric data were analyzed using a multilayer model yielding the dielectric function (DF). The imaginary part of the DF for the alloys exhibits a pronounced feature which is attributed to exciton-phonon coupling (EPC) similar to the previously reported results for ZnO. Thus, in order to determine reliable transition energies, the spectral dependence is analyzed by a model which includes free excitonic lines, the exciton continuum, and the enhanced absorption due to EPC. A line shape analysis of the temperature-dependent PL spectra yielded in particular the emission-related free excitonic transition energies, which are compared to the results from the DF line-shape analysis. The PL linewidth is discussed within the framework of an alloy disorder model.

  6. Exciton dynamics in pentacene and tetracene studied using optical pump-probe spectroscopy

    NASA Astrophysics Data System (ADS)

    Thorsmølle, V. K.; Averitt, R. D.; Demsar, J.; Chi, X.; Smith, D. L.; Ramirez, A. P.; Taylor, A. J.

    We present room temperature photoinduced reflection and transmission measurements in pentacene and tetracene single crystals using optical pump-probe spectroscopy. Singlet exciton recombination, singlet-triplet fission, excited singlet, and triplet state absorption is observed.

  7. Exciton dynamics in pentacene and tetracene studied using optical pump-probe spectroscopy

    SciTech Connect

    Thorsmølle, V. K.; Averitt, R. D.; Demsar, J.; Chi, X.; Smith, D. L.; Ramirez, A. P.; Taylor, Antoinette J.,

    2004-01-01

    We present room temperature photoinduced reflection and transmission measurements in pentacene and tetracene single crystals using optical pump-probe spectroscopy. Singlet exciton recombination, singlet-triplet fission, excited singlet, and triplet state absorption is observed.

  8. Electrically driven optical metamaterials

    PubMed Central

    Le-Van, Quynh; Le Roux, Xavier; Aassime, Abdelhanin; Degiron, Aloyse

    2016-01-01

    The advent of metamaterials more than 15 years ago has offered extraordinary new ways of manipulating electromagnetic waves. Yet, progress in this field has been unequal across the electromagnetic spectrum, especially when it comes to finding applications for such artificial media. Optical metamaterials, in particular, are less compatible with active functionalities than their counterparts developed at lower frequencies. One crucial roadblock in the path to devices is the fact that active optical metamaterials are so far controlled by light rather than electricity, preventing them from being integrated in larger electronic systems. Here we introduce electroluminescent metamaterials based on metal nano-inclusions hybridized with colloidal quantum dots. We show that each of these miniature blocks can be individually tuned to exhibit independent optoelectronic properties (both in terms of electrical characteristics, polarization, colour and brightness), illustrate their capabilities by weaving complex light-emitting surfaces and finally discuss their potential for displays and sensors. PMID:27328976

  9. Electrically driven optical metamaterials.

    PubMed

    Le-Van, Quynh; Le Roux, Xavier; Aassime, Abdelhanin; Degiron, Aloyse

    2016-01-01

    The advent of metamaterials more than 15 years ago has offered extraordinary new ways of manipulating electromagnetic waves. Yet, progress in this field has been unequal across the electromagnetic spectrum, especially when it comes to finding applications for such artificial media. Optical metamaterials, in particular, are less compatible with active functionalities than their counterparts developed at lower frequencies. One crucial roadblock in the path to devices is the fact that active optical metamaterials are so far controlled by light rather than electricity, preventing them from being integrated in larger electronic systems. Here we introduce electroluminescent metamaterials based on metal nano-inclusions hybridized with colloidal quantum dots. We show that each of these miniature blocks can be individually tuned to exhibit independent optoelectronic properties (both in terms of electrical characteristics, polarization, colour and brightness), illustrate their capabilities by weaving complex light-emitting surfaces and finally discuss their potential for displays and sensors. PMID:27328976

  10. Nano-optical imaging of WS e2 waveguide modes revealing light-exciton interactions

    NASA Astrophysics Data System (ADS)

    Fei, Z.; Scott, M. E.; Gosztola, D. J.; Foley, J. J.; Yan, J.; Mandrus, D. G.; Wen, H.; Zhou, P.; Zhang, D. W.; Sun, Y.; Guest, J. R.; Gray, S. K.; Bao, W.; Wiederrecht, G. P.; Xu, X.

    2016-08-01

    We report on a nano-optical imaging study of WS e2 thin flakes with scanning near-field optical microscopy (NSOM). The NSOM technique allows us to visualize in real space various waveguide photon modes inside WS e2 . By tuning the excitation laser energy, we are able to map the entire dispersion of these waveguide modes both above and below the A exciton energy of WS e2 . We found that all the modes interact strongly with WS e2 excitons. The outcome of the interaction is that the observed waveguide modes shift to higher momenta right below the A exciton energy. At higher energies, on the other hand, these modes are strongly damped due to adjacent B excitons or band-edge absorptions. The mode-shifting phenomena are consistent with polariton formation in WS e2 .

  11. Polarized excitons in nanorings and the optical Aharonov-Bohm effect

    NASA Astrophysics Data System (ADS)

    Govorov, A. O.; Ulloa, S. E.; Karrai, K.; Warburton, R. J.

    2002-08-01

    The quantum nature of matter lies in the wave function phases that accumulate while particles move along their trajectories. A prominent example is the Aharonov-Bohm phase, which has been studied in connection with the conductance of nanostructures. However, optical response in solids is determined by neutral excitations, for which no sensitivity to magnetic flux would be expected. We propose a mechanism for the topological phase of a neutral particle, a polarized exciton confined to a semiconductor quantum ring. We predict that this magnetic-field induced phase may strongly affect excitons in a system with cylindrical symmetry, resulting in switching between ``bright'' exciton ground states and novel ``dark'' states with nearly infinite lifetimes. Since excitons determine the optical response of semiconductors, the predicted phase can be used to tailor photon emission from quantum nanostructures.

  12. Toward room-temperature superfluidity of exciton polaritons in an optical microcavity with an embedded MoS_2 monolayer

    NASA Astrophysics Data System (ADS)

    Kolmakov, German V.; Pomirchi, Leonid M.; Kezerashvili, Roman Ya.

    2016-07-01

    By considering driven diffusive dynamics of exciton polaritons in an optical microcavity with an embedded molybdenum disulfide monolayer, we determine experimentally relevant range of parameters at which room-temperature superfuidity can be observed. It is shown that the superfluid transitions occurs in a trapped polariton gas at laser pumping power $P>600$ mW and and trapping potential strength $k > 50$ eV/cm$^2$. We also propose a simple analytic model that provides a useful estimate for the polariton gas density, which enables one to determine the conditions for observation of room temperature polariton superfluidity.

  13. Optical functionality of plasmon-exciton nanomaterials in the strong coupling regime

    NASA Astrophysics Data System (ADS)

    Sukharev, Maxim

    Understanding optical plasmon-exciton interaction in hybrid plasmonic nanostructures is important for tuning the optical response, e.g. for applications in nonlinear optics, organic solar cells, or organic light-emitting diodes. In developing such nanostructures, the strong coupling phenomena play crucial role allowing to efficiently transfer energy between plasmons and molecular excitons on a femtosecond time scale. In this talk I will discuss modeling aspects of various optical phenomena at plasmonic interfaces using Maxwell-Bloch equations in three dimensions. Various plasmonic systems including periodic V-grooves, bowtie antennas, nanowires, periodic hole arrays, and others will be considered. In particular, I will demonstrate that one can design hybrid nanomaterials with highly pronounced Fano resonances using femtosecond lasers. I will show that it is possible to use ultra-short laser pulses to materials with desired properties and functionality. Electromagnetic energy transport in systems composed of closely spaced nanowires in a presence of molecular excitons will also be discussed.

  14. Nonlinear optical spectra having characteristics of Fano interferences in coherently coupled lowest exciton biexciton states in semiconductor quantum dots

    SciTech Connect

    Gotoh, Hideki Sanada, Haruki; Yamaguchi, Hiroshi; Sogawa, Tetsuomi

    2014-10-15

    Optical nonlinear effects are examined using a two-color micro-photoluminescence (micro-PL) method in a coherently coupled exciton-biexciton system in a single quantum dot (QD). PL and photoluminescence excitation spectroscopy (PLE) are employed to measure the absorption spectra of the exciton and biexciton states. PLE for Stokes and anti-Stokes PL enables us to clarify the nonlinear optical absorption properties in the lowest exciton and biexciton states. The nonlinear absorption spectra for excitons exhibit asymmetric shapes with peak and dip structures, and provide a distinct contrast to the symmetric dip structures of conventional nonlinear spectra. Theoretical analyses with a density matrix method indicate that the nonlinear spectra are caused not by a simple coherent interaction between the exciton and biexciton states but by coupling effects among exciton, biexciton and continuum states. These results indicate that Fano quantum interference effects appear in exciton-biexciton systems at QDs and offer important insights into their physics.

  15. Chemically driven tunable light emission of charged and neutral excitons in monolayer WS₂.

    PubMed

    Peimyoo, Namphung; Yang, Weihuang; Shang, Jingzhi; Shen, Xiaonan; Wang, Yanlong; Yu, Ting

    2014-11-25

    Monolayer (1L) semiconducting transition metal dichacogenides (TMDs) possess remarkable physical and optical properties, promising for a wide range of applications from nanoelectronics to optoelectronics such as light-emitting and sensing devices. Here we report how the molecular adsorption can modulate the light emission and electrical properties of 1L WS2. The dependences of trion and exciton emission on chemical doping are investigated in 1L WS2 by microphotoluminescence (μPL) measurements, where different responses are observed and simulated theoretically. The total PL is strongly enhanced when electron-withdrawing molecules adsorb on 1L WS2, which is attributed to the increase of the exciton formation due to charge transfer. The electrical transport measurements of a 1L WS2 field effect transistor elucidate the effect of the adsorbates on the conductivity, which give evidence for charge transfer between molecules and 1L WS2. These findings open up many opportunities to manipulate the electrical and optical properties of two-dimensional TMDs, which are particularly important for developing optoelectronic devices for chemical and biochemical sensing applications. PMID:25317839

  16. Direct optical state preparation of the dark exciton in a quantum dot

    NASA Astrophysics Data System (ADS)

    Lüker, S.; Kuhn, T.; Reiter, D. E.

    2015-11-01

    Because of their weak coupling to the electromagnetic field, dark excitons in semiconductor quantum dots possess extremely long lifetimes, which makes them attractive candidates for quantum information processing. On the other hand, the preparation and manipulation of dark states is challenging, because commonly used optical excitation mechanisms are not applicable. We propose an efficient mechanism for the deterministic preparation of the dark exciton exploiting the application of a tilted magnetic field and the optical excitation with a chirped, i.e., frequency modulated, laser pulse.

  17. Excitonic structure of bulk AlN from optical reflectivity and cathodoluminescence measurements

    NASA Astrophysics Data System (ADS)

    Silveira, E.; Freitas, J. A., Jr.; Glembocki, O. J.; Slack, G. A.; Schowalter, L. J.

    2005-01-01

    Reflection measurements in the near-band-edge region of bulk AlN crystals have been performed as a function of temperature. The optical reflectance spectra of an a -face AlN sample show a feature at about 6.029 eV, which we assign to the free exciton A . The observation of the free exciton A first excited state yields the estimated values of the direct band gap and the limit of the electron effective mass. Optical reflectance measurements performed on AlN samples with two different crystallographic orientations allow the observation of transitions associated with the optical selection rules related to the so-called A,B , and C excitons. It was not possible to fully resolve the B - and C -excitonic transitions, which were observed at about 6.243 and 6.268 eV, respectively. Using the measured exciton energies and a quasicubic model developed for the wurzite crystal structure we estimate the spin-orbit splitting δ=36meV and the crystal-field splitting Δ=-225meV .

  18. In-situ optical transmission electron microscope study of exciton phonon replicas in ZnO nanowires by cathodoluminescence

    SciTech Connect

    Yang, Shize; Tian, Xuezeng; Wang, Lifen; Wei, Jiake; Qi, Kuo; Li, Xiaomin; Xu, Zhi E-mail: xdbai@iphy.ac.cn Wang, Wenlong; Zhao, Jimin; Bai, Xuedong E-mail: xdbai@iphy.ac.cn; Wang, Enge E-mail: xdbai@iphy.ac.cn

    2014-08-18

    The cathodoluminescence spectrum of single zinc oxide (ZnO) nanowires is measured by in-situ optical Transmission Electron Microscope. The coupling between exciton and longitudinal optical phonon is studied. The band edge emission varies for different excitation spots. This effect is attributed to the exciton propagation along the c axis of the nanowire. Contrary to free exciton emission, the phonon replicas are well confined in ZnO nanowire. They travel along the c axis and emit at the end surface. Bending strain increases the relative intensity of second order phonon replicas when excitons travel along the c-axis.

  19. Optically decomposed near-band-edge structure and excitonic transitions in Ga2S3

    PubMed Central

    Ho, Ching-Hwa; Chen, Hsin-Hung

    2014-01-01

    The band-edge structure and band gap are key parameters for a functional chalcogenide semiconductor to its applications in optoelectronics, nanoelectronics, and photonics devices. Here, we firstly demonstrate the complete study of experimental band-edge structure and excitonic transitions of monoclinic digallium trisulfide (Ga2S3) using photoluminescence (PL), thermoreflectance (TR), and optical absorption measurements at low and room temperatures. According to the experimental results of optical measurements, three band-edge transitions of EA = 3.052 eV, EB = 3.240 eV, and EC = 3.328 eV are respectively determined and they are proven to construct the main band-edge structure of Ga2S3. Distinctly optical-anisotropic behaviors by orientation- and polarization-dependent TR measurements are, respectively, relevant to distinguish the origins of the EA, EB, and EC transitions. The results indicated that the three band-edge transitions are coming from different origins. Low-temperature PL results show defect emissions, bound-exciton and free-exciton luminescences in the radiation spectra of Ga2S3. The below-band-edge transitions are respectively characterized. On the basis of experimental analyses, the optical property of near-band-edge structure and excitonic transitions in the monoclinic Ga2S3 crystal is revealed. PMID:25142550

  20. Nature of the narrow optical band in H*-aggregates: Dozy-chaos–exciton coupling

    SciTech Connect

    Egorov, Vladimir V.

    2014-07-15

    Dozy chaos emerges as a combined effect of the collective chaotic motion of electrons and nuclei, and their chaotic electromagnetic interactions in the transient state of molecules experiencing quantum transitions. Following earlier discussions of the well-known Brönsted relations for proton-transfer reactions; the temperature-dependent electron transfer in Langmuir–Blodgett films; the shape of the optical bands of polymethine dye monomers, their dimers, and J-aggregates, this paper reports one more application of the dozy-chaos theory of molecular quantum transitions. The qualitative and quantitative explanations for shape of a narrow and blue-shifted optical absorption band in H{sup *}-aggregates is given on the basis of the dozy-chaos theory by taking into account the dozy-chaos–exciton coupling effect. It is emphasized that in the H{sup *}-aggregate chromophore (dimer of cyclic bis-thiacarbocyanines) there is a competition between two Frenkel exciton transitions through the chaotic reorganization motion of nuclear environment. As a result, the highly organized quantum transition to the upper exciton state becomes an exciton-induced source of dozy chaos for the low organized transition to the lower exciton state. This manifests itself in appearing the narrow peak and broad wing in the optical spectrum pattern of H{sup *}-aggregates. A similar enhancement in the H{sup *}-effect caused by the strengthening of the exciton coupling in H{sup *}-dimers, which could be achieved by synthesizing tertiary and quarternary thiacarbocyanine monomers, is predicted.

  1. Photocurrent spectroscopy of exciton and free particle optical transitions in suspended carbon nanotube pn-junctions

    SciTech Connect

    Chang, Shun-Wen; Theiss, Jesse; Hazra, Jubin; Aykol, Mehmet; Kapadia, Rehan; Cronin, Stephen B.

    2015-08-03

    We study photocurrent generation in individual, suspended carbon nanotube pn-junction diodes formed by electrostatic doping using two gate electrodes. Photocurrent spectra collected under various electrostatic doping concentrations reveal distinctive behaviors for free particle optical transitions and excitonic transitions. In particular, the photocurrent generated by excitonic transitions exhibits a strong gate doping dependence, while that of the free particle transitions is gate independent. Here, the built-in potential of the pn-junction is required to separate the strongly bound electron-hole pairs of the excitons, while free particle excitations do not require this field-assisted charge separation. We observe a sharp, well defined E{sub 11} free particle interband transition in contrast with previous photocurrent studies. Several steps are taken to ensure that the active charge separating region of these pn-junctions is suspended off the substrate in a suspended region that is substantially longer than the exciton diffusion length and, therefore, the photocurrent does not originate from a Schottky junction. We present a detailed model of the built-in fields in these pn-junctions, which, together with phonon-assistant exciton dissociation, predicts photocurrents on the same order of those observed experimentally.

  2. New nonlinear optical effect: self-reflection phenomenon due to exciton-biexciton-light interaction in semiconductors

    NASA Astrophysics Data System (ADS)

    Khadzhi, P. I.; Lyakhomskaya, K. D.; Nadkin, L. Y.; Markov, D. A.

    2002-05-01

    The characteristic peculiarities of the self-reflection of a strong electromagnetic wave in a system of coherent excitons and biexcitons due to the exciton-photon interaction and optical exciton-biexciton conversion in semiconductors were investigated as one of the manifestations of nonlinear optical Stark-effect. It was found that a monotonously decreasing standing wave with an exponential decreasing spatial tail is formed in the semiconductor. Under the action of the field of a strong pulse, an optically homogeneous medium is converted, into the medium with distributed feedback. The appearance of the spatially separated narrow pears of the reflective index, extinction and reflection coefficients is predicted.

  3. Acoustically-Driven Trion and Exciton Modulation in Piezoelectric Two-Dimensional MoS2.

    PubMed

    Rezk, Amgad R; Carey, Benjamin; Chrimes, Adam F; Lau, Desmond W M; Gibson, Brant C; Zheng, Changxi; Fuhrer, Michael S; Yeo, Leslie Y; Kalantar-Zadeh, Kourosh

    2016-02-10

    By exploiting the very recent discovery of the piezoelectricity in odd-numbered layers of two-dimensional molybdenum disulfide (MoS2), we show the possibility of reversibly tuning the photoluminescence of single and odd-numbered multilayered MoS2 using high frequency sound wave coupling. We observe a strong quenching in the photoluminescence associated with the dissociation and spatial separation of electrons-holes quasi-particles at low applied acoustic powers. At the same applied powers, we note a relative preference for ionization of trions into excitons. This work also constitutes the first visual presentation of the surface displacement in one-layered MoS2 using laser Doppler vibrometry. Such observations are associated with the acoustically generated electric field arising from the piezoelectric nature of MoS2 for odd-numbered layers. At larger applied powers, the thermal effect dominates the behavior of the two-dimensional flakes. Altogether, the work reveals several key fundamentals governing acousto-optic properties of odd-layered MoS2 that can be implemented in future optical and electronic systems. PMID:26729449

  4. Coherent transfer of orbital angular momentum to excitons by optical four-wave mixing.

    PubMed

    Ueno, Y; Toda, Y; Adachi, S; Morita, R; Tawara, T

    2009-10-26

    We demonstrate the coherent transfer of optical orbital angular momentum (OAM) to the center of mass momentum of excitons in semiconductor GaN using a four-wave mixing (FWM) process. When we apply the optical vortex (OV) as an excitation pulse, the diffracted FWM signal exhibits phase singularities that satisfy the OAM conservation law, which remain clear within the exciton dephasing time (approximately 1ps). We also demonstrate the arbitrary control of the topological charge in the output signal by changing the OAM of the input pulse. The results provide a way of controlling the optical OAM through carriers in solids. Moreover, the time evolution of the FWM with OAM leads to the study of the closed-loop carrier coherence in materials. PMID:19997285

  5. Large polarization-dependent exciton optical Stark effect in lead iodide perovskites.

    PubMed

    Yang, Ye; Yang, Mengjin; Zhu, Kai; Johnson, Justin C; Berry, Joseph J; van de Lagemaat, Jao; Beard, Matthew C

    2016-01-01

    A strong interaction of a semiconductor with a below-bandgap laser pulse causes a blue-shift of the bandgap transition energy, known as the optical Stark effect. The energy shift persists only during the pulse duration with an instantaneous response time. The optical Stark effect has practical relevance for applications, including quantum information processing and communication, and passively mode-locked femtosecond lasers. Here we demonstrate that solution-processable lead-halide perovskites exhibit a large optical Stark effect that is easily resolved at room temperature resulting from the sharp excitonic feature near the bandedge. We also demonstrate that a polarized pump pulse selectively shifts one spin state producing a spin splitting of the degenerate excitonic states. Such selective spin manipulation is an important prerequisite for spintronic applications. Our result implies that such hybrid semiconductors may have great potential for optoelectronic applications beyond photovoltaics. PMID:27577007

  6. Phonon coupling in optical transitions for singlet-triplet pairs of bound excitons in semiconductors

    NASA Astrophysics Data System (ADS)

    Pistol, M. E.; Monemar, B.

    1986-05-01

    A model is presented for the observed strong difference in selection rules for coupling of phonons in the one-phonon sideband of optical spectra related to bound excitons in semiconductors. The present treatment is specialized to the case of a closely spaced pair of singlet-triplet character as the lowest electronic states, as is common for bound excitons associated with neutral complexes in materials like GaP and Si. The optical transition for the singlet bound-exciton state is found to couple strongly only to symmetric A1 modes. The triplet state has a similar coupling strength to A1 modes, but in addition strong contributions are found for replicas corresponding to high-density-of-states phonons TAX, LAX, and TOX. This can be explained by a treatment of particle-phonon coupling beyond the ordinary adiabatic approximation. A weak mixing between the singlet and triplet states is mediated by the phonon coupling, as described in first-order perturbation theory. The model derived in this work, for such phonon-induced mixing of closely spaced electronic states, is shown to explain the observed phonon coupling for several bound-exciton systems of singlet-triplet character in GaP. In addition, the observed oscillator strength of the forbidden triplet state may be explained as partly derived from phonon-induced mixing with the singlet state, which has a much larger oscillator strength.

  7. Excitons in a mirror: Formation of “optical bilayers” using MoS{sub 2} monolayers on gold substrates

    SciTech Connect

    Mertens, Jan; Baumberg, Jeremy J.; Shi, Yumeng; Yang, Hui Ying; Molina-Sánchez, Alejandro; Wirtz, Ludger

    2014-05-12

    We report coupling of excitons in monolayers of molybdenum disulphide to their mirror image in an underlying gold substrate. Excitons at the direct band gap are little affected by the substrate whereas strongly bound C-excitons associated with a van-Hove singularity change drastically. On quartz substrates only one C-exciton is visible (in the blue) but on gold substrates a strong red-shifted extra resonance in the green is seen. Exciton coupling to its image leads to formation of a “mirror biexciton” with enhanced binding energy. Estimates of this energy shift in an emitter-gold system match experiments well. The absorption spectrum of MoS{sub 2} on gold thus resembles a bilayer of MoS{sub 2} which has been created by optical coupling. Additional top-mirrors produce an “optical bulk.”.

  8. Optical orientation of bright excitons in InAs/GaAs quantum dots: Influence of a Faraday magnetic field and the dark exciton states

    NASA Astrophysics Data System (ADS)

    Sancho, S.; Chaouache, M.; Maaref, M. A.; Bernardot, F.; Eble, B.; Lemaître, A.; Testelin, C.

    2011-10-01

    We study the injection of polarized bright and dark excitons in quantum dots, under nonresonant or resonant excitation, by polarization-resolved photoluminescence experiments on an ensemble of self-assembled InAs/GaAs quantum dots. The importance of the polarized dark exciton creation on the optical emission under magnetic field is discussed. Under circular excitation, we observe the expected increase and saturation of the polarization rate with a magnetic field applied in Faraday geometry. Strikingly, the polarization rate slightly decreases for magnetic fields greater than ˜1.5 T; the feature is more pronounced for higher interband energies and is attributed to a more efficient initial polarization of the dark exciton states. This interpretation is confirmed by the lack of decrease of the polarization rate for quantum dots excited at exact resonance through a 1LO-phonon-assisted transition. Finally, we measure the bright exciton exchange energy as a function of interband emission energy, we measure a decrease from 65 to 30 μeV in the range 1.28-1.35 eV, and we obtain an estimate of the dark exciton splitting.

  9. Electric field effect on optical harmonic generation at the exciton resonances in GaAs

    NASA Astrophysics Data System (ADS)

    Brunne, D.; Lafrentz, M.; Pavlov, V. V.; Pisarev, R. V.; Rodina, A. V.; Yakovlev, D. R.; Bayer, M.

    2015-08-01

    An electric field applied to a semiconductor reduces its crystal symmetry and modifies its electronic structure which is expected to result in changes of the linear and nonlinear response to optical excitation. In GaAs, we observe experimentally strong electric field effects on the optical second (SHG) and third (THG) harmonic generation. The SHG signal for the laser-light k vector parallel to the [001] crystal axis is symmetry forbidden in the electric-dipole approximation, but can be induced by an applied electric field in the vicinity of the 1 s exciton energy. Surprisingly, the THG signal, which is allowed in this geometry, is considerably reduced by the electric field. We develop a theory which provides good agreement with the experimental data. In particular, it shows that the optical nonlinearities for the 1 s exciton resonance are modified in an electric field by the Stark effect, which mixes the 1 s and 2 p exciton states of opposite parity. This mixing acts in opposite way on the SHG and THG processes, as it leads to the appearance of forbidden SHG in (001)-oriented GaAs and decreases the crystallographic THG.

  10. Optical spectroscopy and imaging of the higher energy excitons and bandgap of monolayer MoS2

    NASA Astrophysics Data System (ADS)

    Borys, Nicholas; Bao, Wei; Barnard, Edward; Ko, Changhyun; Tongay, Sefaatin; Wu, Junqiao; Yang, Li; Schuck, P. James

    Monolayer MoS2 (ML-MoS2) exhibits a rich manifold of excitons that dictate optoelectronic performance and functionality. Disentangling these states, which include the quasi-particle bandgap, is critical for developing 2D optoelectronic devices that operate beyond the optical bandgap. Whereas photoluminescence (PL) spectroscopy only probes the lowest-energy radiative state and absorption spectroscopy fails to discriminate energetically degenerate states, photoluminescence excitation (PLE) spectroscopy selectively probes only the excited states that thermalize to the emissive ground state exciton. Using PLE spectroscopy of ML-MoS2, we identify the Rydberg series of the exciton A and exciton B states as well as signatures of the quasi-particle bandgap and coupling between the indirect C exciton and the lowest-energy A exciton, which have eluded previous PLE studies. The assignment of these states is confirmed with density functional theory. Mapping the PLE spectrum reveals spatial variations of the higher-energy exciton manifold and quasi-particle bandgap which mirror the heterogeneity in the PL but also indicate variations in local exciton thermalization processes and chemical potentials.

  11. NONLINEAR OPTICAL PHENOMENA: Self-reflection in a system of excitons and biexcitons in semiconductors

    NASA Astrophysics Data System (ADS)

    Khadzhi, P. I.; Lyakhomskaya, K. D.

    1999-10-01

    The characteristic features of the self-reflection of a powerful electromagnetic wave in a system of coherent excitons and biexcitons in semiconductors were investigated as one of the manifestations of the nonlinear optical skin effect. It was found that a monotonically decreasing standing wave with an exponentially falling spatial tail is formed in the surface region of a semiconductor. Under the influence of the field of a powerful pulse, an optically homogeneous medium is converted into one with distributed feedback. The appearance of spatially separated narrow peaks of the refractive index, extinction coefficient, and reflection coefficient is predicted.

  12. Excitonic optical properties of wurtzite ZnS quantum dots under pressure

    SciTech Connect

    Zeng, Zaiping; Garoufalis, Christos S.; Baskoutas, Sotirios; Bester, Gabriel

    2015-03-21

    By means of atomistic empirical pseudopotentials combined with a configuration interaction approach, we have studied the optical properties of wurtzite ZnS quantum dots in the presence of strong quantum confinement effects as a function of pressure. We find the pressure coefficients of quantum dots to be highly size-dependent and reduced by as much as 23% in comparison to the bulk value of 63 meV/GPa obtained from density functional theory calculations. The many-body excitonic effects on the quantum dot pressure coefficients are found to be marginal. The absolute gap deformation potential of quantum dots originates mainly from the energy change of the lowest unoccupied molecular orbital state. Finally, we find that the exciton spin-splitting increases nearly linearly as a function of applied pressure.

  13. Optical spectrum of bottom-up graphene nanoribbons: towards efficient atom-thick excitonic solar cells

    PubMed Central

    Villegas, Cesar E. P.; Mendonça, P. B.; Rocha, A. R.

    2014-01-01

    Recently, atomically well-defined cove-shaped graphene nanoribbons have been obtained using bottom-up synthesis. These nanoribbons have an optical gap in the visible range of the spectrum which make them candidates for donor materials in photovoltaic devices. From the atomistic point of view, their electronic and optical properties are not clearly understood. Therefore, in this work we carry out ab-initio density functional theory calculations combine with many-body perturbation formalism to study their electronic and optical properties. Through the comparison with experimental measurements, we show that an accurate description of the nanoribbon's optical properties requires the inclusion of electron-hole correlation effects. The energy, binding energy and the corresponding excitonic transitions involved are analyzed. We found that in contrast to zigzag graphene nanoribbons, the excitonic peaks in the absorption spectrum are a consequence of a group of transitions involving the first and second conduction and valence bands. Finally, we estimate some relevant optical properties that strengthen the potential of these nanoribbons for acting as a donor materials in photovoltaic. PMID:25301001

  14. Temperature-dependent excitonic effects in the optical properties of single-layer MoS2

    NASA Astrophysics Data System (ADS)

    Molina-Sánchez, Alejandro; Palummo, Maurizia; Marini, Andrea; Wirtz, Ludger

    2016-04-01

    Temperature influences the performance of two-dimensional (2D) materials in optoelectronic devices. Indeed, the optical characterization of these materials is usually realized at room temperature. Nevertheless, most ab initio studies are still performed without including any temperature effect. As a consequence, important features are thus overlooked, such as the relative height of the excitonic peaks and their broadening, directly related to the temperature and to the nonradiative exciton relaxation time. We present ab initio calculations of the optical response of single-layer MoS2, a prototype 2D material, as a function of temperature using density functional theory and many-body perturbation theory. We compute the electron-phonon interaction using the full spinorial wave functions, i.e., fully taking into account the effects of spin-orbit interaction. We find that bound excitons (A and B peaks) and resonant excitons (C peak) exhibit different behavior with temperature, displaying different nonradiative linewidths. We conclude that the inhomogeneous broadening of the absorption spectra is mainly due to electron-phonon scattering mechanisms. Our calculations explain the shortcomings of previous (zero-temperature) theoretical spectra and match well with the experimental spectra acquired at room temperature. Moreover, we disentangle the contributions of acoustic and optical phonon modes to the quasiparticles and exciton linewidths. Our model also allows us to identify which phonon modes couple to each exciton state, which is useful for the interpretation of resonant Raman-scattering experiments.

  15. Electro optical tuning of Tamm-plasmon exciton-polaritons

    SciTech Connect

    Gessler, J.; Baumann, V.; Emmerling, M.; Amthor, M.; Winkler, K.; Schneider, C.; Kamp, M.; Höfling, S.

    2014-11-03

    We report on electro optical tuning of the emission from GaAs quantum wells resonantly coupled to a Tamm-plasmon mode in a hybrid metal/dielectric structure. The structures were studied via momentum resolved photoluminescence and photoreflectance spectroscopy, and the surface metal layer was used as a top gate, which allowed for a precise tuning of the quantum well emission via the quantum confined Stark effect. By tuning the resonance, we were able to observe the characteristic anticrossing behavior of a polaritonic emission in the strong light-matter coupling regime, yielding a Rabi splitting of (9.2 ± 0.2) meV.

  16. Nanofabrication and applications of subwavelength optical probes: Chemical and biological sensors, light sources and exciton probes

    SciTech Connect

    Tan, W.

    1993-01-01

    The author has developed a new and controllable nanofabrication technique, photo-nanofabrication, based on near-field photo-chemical synthesis and nanometer optical sources. Photo-nanofabrication can produce subwavelength light and exciton probes with or without specific chemical or biological sensitivity. By applying near-field optics, the author has successfully demonstrated a new concept of near-field photochemical synthesis, in which the dimension of a product is solely determined by the size of the light source. The most successful application to date is the development of the smallest fiberoptic chemical sensors. Specifically, a thousandfold miniaturization of an immobilized fiberoptic pH sensor has been achieved, leading to at least a millionfold decrease in necessary sample volume and to at least a hundredfold shorter response time. The sensors have high fluorescence intensity and excellent detection limit. New internal calibration methods have also been developed for accurate pH quantification. The newly developed optical sensors have been used in real time measurements of pH on individual, viable, intact rat conceptuses during the period of organogenesis. The sensors can discriminate pH changes of less than 0.1 pH unit in the physiologic pH range. Static determinations of pH in rat conceptuses of varying gestational ages show decreasing pH with conceptal age. Chemical dynamic alterations in pH of intact rat conceptuses, in response to several variations in their environmental conditions, have been measured. Passive and active subwavelength light sources have been constructed with both micropipettes and fiberoptic tips. They have been used as exciton and light sources and in preliminary probe-to-sample distance regulated, Foerster energy transfer studies as well as in studies of the probe-to-sample interfacial Kasha effect. They were also used in supertip development for near-field scanning optical microscopy and for molecular exciton microscopy.

  17. Magneto-optical properties and recombination dynamics of isoelectronic bound excitons in ZnO

    SciTech Connect

    Chen, S. L.; Chen, W. M.; Buyanova, I. A.

    2014-02-21

    Magneto-optical and time-resolved photoluminescence (PL) spectroscopies are employed to evaluate electronic structure of a bound exciton (BX) responsible for the 3.364 eV line (labeled as I{sub 1}{sup *}) in bulk ZnO. From time-resolved PL spectroscopy, I{sub 1}{sup *} is concluded to originate from the exciton ground state. Based on performed magneto-PL studies, the g-factors of the involved electron and hole are determined as being g{sub e} = 1.98 and g{sub h}{sup ∥}(g{sub h}{sup ⊥}) = 1.2(1.62), respectively. These values are nearly identical to the reported g-factors for the I{sup *} line in ZnO (Phys. Rev. B 86, 235205 (2012)), which proves that I{sub 1}{sup *} should have a similar origin as I{sup *} and should arise from an exciton bound to an isoelectronic center with a hole-attractive potential.

  18. Decoherence processes during optical manipulation of excitonic qubits in semiconductor quantum dots

    NASA Astrophysics Data System (ADS)

    Wang, Q. Q.; Muller, A.; Bianucci, P.; Rossi, E.; Xue, Q. K.; Takagahara, T.; Piermarocchi, C.; MacDonald, A. H.; Shih, C. K.

    2005-07-01

    Using photoluminescence spectroscopy, we have investigated the nature of Rabi oscillation damping during optical manipulation of excitonic qubits in self-assembled quantum dots. Rabi oscillations were recorded by varying the pulse amplitude for fixed pulse durations between 4ps and 10ps . Up to five periods are visible, making it possible to quantify the excitation dependent damping. We find that this damping is more pronounced for shorter pulse widths and show that its origin is the nonresonant excitation of carriers in the wetting layer, most likely involving bound-to-continuum and continuum-to-bound transitions.

  19. Optical exciton Aharonov-Bohm effect, persistent current, and magnetization in semiconductor nanorings of type I and II

    NASA Astrophysics Data System (ADS)

    Grochol, M.; Grosse, F.; Zimmermann, R.

    2006-09-01

    The optical exciton Aharonov-Bohm effect—i.e., an oscillatory component in the energy of optically active (bright) states—is investigated in nanorings. It is shown that a small effective electron mass, strong confinement of the electron, and high barrier for the hole, achieved, e.g., by an InAs nanoring embedded in an AlGaSb quantum well, are favorable for observing the optical exciton Aharonov-Bohm effect. The second derivative of the exciton energy with respect to the magnetic field is utilized to extract Aharonov-Bohm oscillations even for the lowest bright state unambiguously. A connection between the theories for infinitesimal narrow and finite width rings is established. Furthermore, the magnetization is compared to the persistent current, which oscillates periodically with the magnetic field and confirms thus the nontrivial (connected) topology of the wave function in the nanoring.

  20. Dynamic quasi-energy-band modulation and exciton effects in biased superlattices driven by a two-color far-infrared field: Disappearance of dynamic localization

    NASA Astrophysics Data System (ADS)

    Yashima, Kenta; Hino, Ken-Ichi; Toshima, Nobuyuki

    2003-12-01

    A theoretical study of the optical and electronic properties of semiconductor superlattices in ac-dc fields, termed the dynamic Wannier-Stark ladder (DWSL), is done. The biased superlattices are driven by two far-infrared fields with different frequencies and relative phase of δ. Here, the frequency of the first laser is equal to the Bloch frequency ωB of the system under study, while that of the second laser is equal to 2ωB. Quasienergies of the DWSL are calculated based on the Floquet theorem, and the associated linear photoabsorption spectra are evaluated. For δ=0, a gourd-shaped quasi-energy structure characteristic of both dynamic localization (DL) and delocalization (DDL), similar to the usual DWSL driven by a single laser, appears. By changing the ratio of the two laser strengths, however, the width of the quasi-energy band and the locations of both DL and DDL vary noticeably. As for δ≠0, on the other hand, band collapse and the associated DL do not necessarily follow. In fact, DL vanishes and the quasi-energy degeneracy is lifted in a certain range of δ. Just DDL remains over the entire range of the laser strength, eventually resulting in a plateaulike band structure in the linear absorption spectra. The basic physics underlying this phenomenon, which can be readily interpreted in terms of a closed analytical expression, is that all quasi-energies for given crystal momenta are out of phase with each other as a function of laser strength without converging to a single point of energy. This is a feature of this DWSL which sharply distinguishes it from a conventional DWSL generated using a single laser to drive it. Furthermore, an exciton effect is incorporated with the above noninteracting problem, so that exciton dressed states are formed. It is found that this effect gives rise to more involved quasi-energy structures and a more pronounced release of the energy degeneracy of DL, leading again to the formation of a band structure in the absorption

  1. Electronic and optical properties of single excitons and biexcitons in type-II quantum dot nanocrystals

    SciTech Connect

    Koc, Fatih; Sahin, Mehmet E-mail: mehsahin@gmail.com

    2014-05-21

    In this study, a detailed investigation of the electronic and optical properties (i.e., binding energies, absorption wavelength, overlap of the electron-hole wave functions, recombination oscillator strength, etc.) of an exciton and a biexciton in CdTe/CdSe core/shell type-II quantum dot heterostructures has been carried out in the frame of the single band effective mass approximation. In order to determine the electronic properties, we have self-consistently solved the Poisson-Schrödinger equations in the Hartree approximation. We have considered all probable Coulomb interaction effects on both energy levels and also on the corresponding wave functions for both single exciton and biexciton. In addition, we have taken into account the quantum mechanical exchange-correlation effects in the local density approximation between same kinds of particles for biexciton. Also, we have examined the effect of the ligands and dielectric mismatch on the electronic and optical properties. We have used a different approximation proposed by Sahin and Koc [Appl. Phys. Lett. 102, 183103 (2013)] for the recombination oscillator strength of the biexciton for bound and unbound cases. The results obtained have been presented comparatively as a function of the shell thicknesses and probable physical reasons in behind of the results have been discussed in a detail.

  2. Statistical Transmutation in Floquet Driven Optical Lattices

    NASA Astrophysics Data System (ADS)

    Sedrakyan, Tigran A.; Galitski, Victor M.; Kamenev, Alex

    2015-11-01

    We show that interacting bosons in a periodically driven two dimensional (2D) optical lattice may effectively exhibit fermionic statistics. The phenomenon is similar to the celebrated Tonks-Girardeau regime in 1D. The Floquet band of a driven lattice develops the moat shape, i.e., a minimum along a closed contour in the Brillouin zone. Such degeneracy of the kinetic energy favors fermionic quasiparticles. The statistical transmutation is achieved by the Chern-Simons flux attachment similar to the fractional quantum Hall case. We show that the velocity distribution of the released bosons is a sensitive probe of the fermionic nature of their stationary Floquet state.

  3. Statistical Transmutation in Floquet Driven Optical Lattices.

    PubMed

    Sedrakyan, Tigran A; Galitski, Victor M; Kamenev, Alex

    2015-11-01

    We show that interacting bosons in a periodically driven two dimensional (2D) optical lattice may effectively exhibit fermionic statistics. The phenomenon is similar to the celebrated Tonks-Girardeau regime in 1D. The Floquet band of a driven lattice develops the moat shape, i.e., a minimum along a closed contour in the Brillouin zone. Such degeneracy of the kinetic energy favors fermionic quasiparticles. The statistical transmutation is achieved by the Chern-Simons flux attachment similar to the fractional quantum Hall case. We show that the velocity distribution of the released bosons is a sensitive probe of the fermionic nature of their stationary Floquet state. PMID:26588392

  4. Hydrodynamic synchronisation of optically driven rotors

    NASA Astrophysics Data System (ADS)

    Debono, Luke J.; Box, Stuart; Phillips, David B.; Simpson, Stephen H.; Hanna, Simon

    2015-08-01

    Hydrodynamic coupling is thought to play a role in the coordinated beating of cilia and flagella, and may inform the future design of artificial swimmers and pumps. In this study, optical tweezers are used to investigate the hydrodynamic coupling between a pair of driven oscillators. The theoretical model of Lenz and Ryskin [P. Lenz and A. Ryskin, Phys. Biol. 3, 285{294 (2006)] is experimentally recreated, in which each oscillator consists of a sphere driven in a circular trajectory. The optical trap position is maintained ahead of the sphere to provide a tangential driving force. The trap is also moved radially to harmonically constrain the sphere to the circular trajectory. Analytically, it has been shown that two oscillators of this type are able to synchronise or phase-lock under certain conditions. We explore the interplay between synchronisation mechanisms and find good agreement between experiment, theory and Brownian dynamics simulations.

  5. Fiber optic mounted laser driven flyer plates

    SciTech Connect

    Paisley, D.L.

    1990-12-31

    This invention is comprised of a laser driven flyer plate where the flyer plate is deposited directly onto the squared end of an optical fiber. The plasma generated by a laser pulse drives the flyer plate toward a target. In another embodiment, a first metal layer is deposited onto the squared end of an optical fiber, followed by a layer of a dielectric material and a second metal layer. The laser pulse generates a plasma in the first metal layer, but the plasma is kept away from the second metal layer by the dielectric layer until the pressure reaches the point where shearing occurs. 2 figs.

  6. Communication: Strong excitonic and vibronic effects determine the optical properties of Li2O2

    NASA Astrophysics Data System (ADS)

    Garcia-Lastra, J. M.; Bass, J. D.; Thygesen, K. S.

    2011-09-01

    The band structure and optical absorption spectrum of lithium peroxide (Li2O2) is calculated from first-principles using the G0W0 approximation and the Bethe-Salpeter equation, respectively. A strongly localized (Frenkel type) exciton corresponding to the π*→σ* transition on the O2-2 peroxide ion gives rise to a narrow absorption peak around 1.2 eV below the calculated bandgap of 4.8 eV. In the excited state, the internal O2-2 bond is significantly weakened due to the population of the σ* orbital. As a consequence, the bond is elongated by almost 0.5 Å leading to an extreme Stokes shift of 2.6 eV. The strong vibronic coupling entails significant broadening of the excitonic absorption peak in good agreement with diffuse reflectance data on Li2O2 which shows a rather featureless spectrum with an absorption onset around 3.0 eV. These results should be important for understanding the origin of the high potential losses and low current densities, which are presently limiting the performance of Li-air batteries.

  7. Simultaneous monitoring of singlet and triplet exciton variations in solid organic semiconductors driven by an external static magnetic field

    SciTech Connect

    Ding, Baofu Alameh, Kamal

    2014-07-07

    The research field of organic spintronics has remarkably and rapidly become a promising research area for delivering a range of high-performance devices, such as magnetic-field sensors, spin valves, and magnetically modulated organic light emitting devices (OLEDs). Plenty of microscopic physical and chemical models based on exciton or charge interactions have been proposed to explain organic magneto-optoelectronic phenomena. However, the simultaneous observation of singlet- and triplet-exciton variations in an external magnetic field is still unfeasible, preventing a thorough theoretical description of the spin dynamics in organic semiconductors. Here, we show that we can simultaneously observe variations of singlet excitons and triplet excitons in an external magnetic field, by designing an OLED structure employing a singlet-exciton filtering and detection layer in conjunction with a separate triplet-exciton detection layer. This OLED structure enables the observation of a Lorentzian and a non-Lorentzian line-shape magnetoresponse for singlet excitons and triplet excitons, respectively.

  8. Linear and nonlinear optical properties of semiconductor nanorings with magnetic field and disorder - Influence on excitons and biexcitons

    NASA Astrophysics Data System (ADS)

    Meier, T.; Thomas, P.; Koch, S. W.

    2001-07-01

    Linear and nonlinear optical absorption spectra are studied theoretically for semiconductor nanorings penetrated by a magnetic field. Due to the Aharanov-Bohm effect the spectral position as well as the oscillator strength of the exciton change periodically as function of the magnetic flux enclosed by the ring. In the nonlinear differential absorption spectra it is found that the magnetic field strongly modifies Coulomb many-body correlations. In particular, the magnetic-field-induced increase of the exciton binding energy is accompanied by a decrease of the biexciton binding energy. The persistence of these effects in the presence of energetic disorder is analyzed.

  9. A detailed investigation of electronic and optical properties of the exciton, the biexciton and charged excitons in a multi-shell quantum dot nanocrystal

    NASA Astrophysics Data System (ADS)

    Aktürk, Abdurrahman; Sahin, Mehmet; Koc, Fatih; Erdinc, Ahmet

    2014-07-01

    In the present study, the electronic and optical properties of the exciton (X), the biexciton (XX) and charged excitons (X- and X+) in a multi-shell quantum dot nanocrystal have been systematically explored in detail. The electronic properties have been determined in the framework of the single-band effective mass approximation. For this purpose, the Poisson-Schrödinger equations have been solved self-consistently in the Hartree approximation. In the electronic structure calculations for XX, X- and X+, the quantum mechanical exchange-correlation potentials between particles of the same type have been taken into account in the local density approximation. Some optical parameters, such as the overlap integrals, recombination oscillator strengths, radiative lifetimes, etc, have been determined by using the single-particle energy levels and wavefunctions obtained. A different approximation, reported in Sahin and Koc 2013 Appl. Phys. Lett. 102 183103, has been used in the recombination oscillator strength calculations. The results have been presented comparatively as a function of the shell thicknesses, and the well widths and probable physical reasons underlying them have been discussed in detail.

  10. Optically engineered ultrafast pulses for controlled rotations of exciton qubits in semiconductor quantum dots

    NASA Astrophysics Data System (ADS)

    Gamouras, Angela; Mathew, Reuble; Hall, Kimberley C.

    2012-07-01

    Shaped ultrafast pulses designed for controlled-rotation (C-ROT) operations on exciton qubits in semiconductor quantum dots are demonstrated using a quantum control apparatus operating at ˜1 eV. Optimum pulse shapes employing amplitude and phase shaping protocols are implemented using the output of an optical parametric oscillator and a programmable pulse shaping system, and characterized using autocorrelation and multiphoton intrapulse interference phase scan techniques. We apply our pulse characterization results and density matrix simulations to assess the fundamental limits on the fidelity of the C-ROT operation, providing a benchmark for the evaluation of sources of noise in other quantum control experiments. Our results indicate the effectiveness of pulse shaping techniques for achieving high fidelity quantum operations in quantum dots with a gate time below 1 ps.

  11. Exciton Model Calculations up to 200 MeV: The Optical Model Points the Way

    SciTech Connect

    Duijvestijn, M.C.; Koning, A.J.

    2005-05-24

    We present a preequilibrium model for nucleons with incident energies from 7 to 200 MeV, for nuclides in the mass range A {>=} 24. This is accomplished by a new global approach for the two-component exciton model which, together with the complementary compound and direct reaction mechanisms, enables a description of continuum energy spectra over the whole outgoing energy range. We develop new forms for the internal transition rates with collision probabilities based on a recent optical-model potential. To connect with conventional semi-classical analyses, we derive from this approach a new energy-dependent form for the average square matrix element M2. We include surface effects and multiple preequilibrium emission up to any order. To assess the predictive power of our model, we have tested it against a complete experimental database of (n,xn) (n,xp) (p,xn), and (p,xp) spectra. In this paper we will show some examples.

  12. Interplay of Cu and oxygen vacancy in optical transitions and screening of excitons in ZnO:Cu films

    SciTech Connect

    Darma, Yudi; Rusydi, Andrivo; Seng Herng, Tun; Marlina, Resti; Fauziah, Resti; Ding, Jun

    2014-02-24

    We study room temperature optics and electronic structures of ZnO:Cu films as a function of Cu concentration using a combination of spectroscopic ellipsometry, photoluminescence, and ultraviolet-visible absorption spectroscopy. Mid-gap optical states, interband transitions, and excitons are observed and distinguishable. We argue that the mid-gap states are originated from interactions of Cu and oxygen vacancy (Vo). They are located below conduction band (Zn4s) and above valence band (O2p) promoting strong green emission and narrowing optical band gap. Excitonic states are screened and its intensities decrease upon Cu doping. Our results show the importance of Cu and Vo driving the electronic structures and optical transitions in ZnO:Cu films.

  13. Interaction Driven Subgap Spin Exciton in the Kondo Insulator SmB6

    SciTech Connect

    Fuhrman, W. T.; Leiner, Jonathan C.; Nikolić, P.; Granroth, Garrett E.; Stone, Matthew B.; Lumsden, Mark D.; DeBeer-Schmitt, Lisa M.; Alekseev, Pavel A.; Mignot, Jean-Michel; Koohpayeh, S. M.; Cottingham, P.; Phelan, William Adam; Schoop, L.; McQueen, T. M.; Broholm, C.

    2015-01-21

    In this paper, using inelastic neutron scattering, we map a 14 meV coherent resonant mode in the topological Kondo insulator SmB6 and describe its relation to the low energy insulating band structure. The resonant intensity is confined to the X and R high symmetry points, repeating outside the first Brillouin zone and dispersing less than 2 meV, with a 5d-like magnetic form factor. We present a slave-boson treatment of the Anderson Hamiltonian with a third neighbor dominated hybridized band structure. This approach produces a spin exciton below the charge gap with features that are consistent with the observed neutron scattering. Finally, we find that maxima in the wave vector dependence of the inelastic neutron scattering indicate band inversion.

  14. Interaction Driven Subgap Spin Exciton in the Kondo Insulator SmB6

    DOE PAGESBeta

    Fuhrman, W. T.; Leiner, Jonathan C.; Nikolić, P.; Granroth, Garrett E.; Stone, Matthew B.; Lumsden, Mark D.; DeBeer-Schmitt, Lisa M.; Alekseev, Pavel A.; Mignot, Jean-Michel; Koohpayeh, S. M.; et al

    2015-01-21

    In this paper, using inelastic neutron scattering, we map a 14 meV coherent resonant mode in the topological Kondo insulator SmB6 and describe its relation to the low energy insulating band structure. The resonant intensity is confined to the X and R high symmetry points, repeating outside the first Brillouin zone and dispersing less than 2 meV, with a 5d-like magnetic form factor. We present a slave-boson treatment of the Anderson Hamiltonian with a third neighbor dominated hybridized band structure. This approach produces a spin exciton below the charge gap with features that are consistent with the observed neutron scattering.more » Finally, we find that maxima in the wave vector dependence of the inelastic neutron scattering indicate band inversion.« less

  15. Optical Study of Exciton Localization Phenomena in Semimagnetic Semiconductors and Their Multiple Quantum Wells.

    NASA Astrophysics Data System (ADS)

    Zhang, Xi-Cheng

    1986-12-01

    The results of picosecond photomodulation and photoluminescence spectroscopies in novel II-VI semimagnetic semiconductors Cd(,1-x)Mn(,x)Te (x < 0.50) bulk and multiple quantum well (MQW) samples are presented. By studying excitonic emission near the bandgap of semiconductors, it is found that excitons can be confined or localized by alloy potential fluctuations, quantum well confinements, local strain of heterointerfaces and energy self-trapping. Steady-state photoluminescence in undoped CdTe/Cd(,1 -x)Mn(,x)Te MQW samples at low temperature shows intense excitonic emission where their radiative quantum efficiencies are two or three orders of magnitude larger than that of the high quality CdTe bulk samples. Time-resolved photoluminescence shows that the excitons have relatively short lifetime (500 picosecond). High quantum efficiency and short exciton lifetime suggest that the radiative recombination is a dominating factor in the excitonic-decay processes in the MQW samples. In general, excitonic emission energies in CdMnTe MQW samples are lower than the free exciton energies (typically 20-40 meV lower as noted from the reflectance spectra). The behavior of these emissions under an external magnetic field (up to 36 tesla) shows that excitons prefer to be localized at the heterointerfaces rather than at the center of the wells in MQW samples. The kinetics of the free and the heterointerface localized excitons in the Cd(,1-x)Mn(,x)Te/Cd(,1-y)Mn(,y)Te MQW samples have been studied by using a transient photoluminescence technique. Exciton lifetimes have been measured in several samples with various quantum well widths. The trapping time of the free exciton localized at the interface has been observed in the wide quantum well samples. The average energy loss rate of localized excitons has been calculated. The resonance excitation spectra of steady-state and transient luminescence show that the exciton spectra are spatially inhomogeneously broadened. An external magnetic

  16. Statistical Transmutation in Periodically Driven Optical Lattices

    NASA Astrophysics Data System (ADS)

    Sedrakyan, Tigran; Galitski, Victor; Kamenev, Alex

    We show that interacting bosons in a periodically driven two dimensional (2D) optical lattice may effectively exhibit fermionic statistics. The phenomenon is similar to the celebrated Tonks-Girardeau regime in 1D. The Floquet band of a driven lattice develops the moat shape, i.e., a minimum along a closed contour in the Brillouin zone. Such degeneracy of the kinetic energy favors fermionic quasiparticles. The statistical transmutation is achieved by the Chern-Simons flux attachment similar to the fractional quantum Hall case. We show that the velocity distribution of the released bosons is a sensitive probe of the fermionic nature of their stationary Floquet state. This work was supported by the PFC-JQI (T.S.), USARO and Simons Foundation (V.G.), and DOE Contract DE-FG02-08ER46482 (A.K.).

  17. Coherent dynamics of exciton orbital angular momentum transferred by optical vortex pulses

    NASA Astrophysics Data System (ADS)

    Shigematsu, K.; Yamane, K.; Morita, R.; Toda, Y.

    2016-01-01

    The coherent dynamics of the exciton center-of-mass motion in bulk GaN are studied using degenerate four-wave-mixing (FWM) spectroscopy with Laguerre-Gaussian (LG) mode pulses. We evaluate the exciton orbital angular momentum (OAM) dynamics from the degree of OAM, which is derived from the distributions of OAM (topological charge) of the FWM signals. When excitons are excited with two single-mode LG pulses, the exciton OAM decay time significantly exceeds the exciton dephasing time, which can be attributed to high uniformity of the exciton dephasing in our bulk sample because the decoherence of the exciton OAM is governed by the angular variation in the exciton dephasing. We also analyze the topological charge (ℓ ) dependence of the OAM decay using a multiple-mode LG pump pulse, which allows us to simultaneously observe the dynamics of the exciton OAM for different ℓ values under the same excitation conditions. The OAM decay times of the ℓ =1 component are usually longer than those of the ℓ =0 component. The ℓ -dependent OAM decay is supported by a phenomenological model which takes into account the local nonuniformity of the exciton dephasing.

  18. Excitons and the lifetime of organic semiconductor devices

    PubMed Central

    Forrest, Stephen R.

    2015-01-01

    While excitons are responsible for the many beneficial optical properties of organic semiconductors, their non-radiative recombination within the material can result in material degradation due to the dumping of energy onto localized molecular bonds. This presents a challenge in developing strategies to exploit the benefits of excitons without negatively impacting the device operational stability. Here, we will briefly review the fundamental mechanisms leading to excitonic energy-driven device ageing in two example devices: blue emitting electrophosphorescent organic light emitting devices (PHOLEDs) and organic photovoltaic (OPV) cells. We describe strategies used to minimize or even eliminate this fundamental device degradation pathway. PMID:25987572

  19. Optical Control of Semiconductor Quantum Dot Spin Qubits with Microcavity Exciton-Polaritons

    NASA Astrophysics Data System (ADS)

    Puri, Shruti; McMahon, Peter L.; Yamamoto, Yoshihisa

    2015-03-01

    Topological surface codes demand the least stringent threshold conditions and are most promising for implementing large quantum algorithms. Based on the resource requirements to reach fault tolerance, we develop a hardware platform for large scale quantum computation with semiconductor quantum dot (QD) electron spin qubits. The current proposals for implementation of two-qubit gates and quantum non demolition (QND) readout in a QuDOS (Quantum Dots with Optically Controlled Spins) architecture suffer from large error rates. In our scheme, the optical manipulation of the QD spin qubits is carried out using their Coulomb exchange interaction with optically excited, spin-polarized, laterally confined quantum well (LcQW) exciton-polaritons. The small mass of polaritons protects them from interaction with their solid-state environment (phonons) and enables strong coupling between spin qubits separated by a few microns. Furthermore, the excitation manifold of the QD is well separated from that of the LcQW polaritons, preventing a spin-flip event during readout. We will outline schemes for implementing fast, high-fidelity, single qubit gate, two-qubit geometric phase gate and single-shot QND measurement and analyze important decoherence mechanisms. The work being presented was carried out at Stanford University. Currently the author is at University of Sherbrooke, Canada.

  20. Optical absorption by Dirac excitons in single-layer transition-metal dichalcogenides

    NASA Astrophysics Data System (ADS)

    Trushin, Maxim; Goerbig, Mark Oliver; Belzig, Wolfgang

    2016-07-01

    We develop an analytically solvable model able to qualitatively explain nonhydrogenic exciton spectra observed recently in two-dimensional (2D) semiconducting transition-metal dichalcogenides. Our exciton Hamiltonian explicitly includes additional angular momentum associated with the pseudospin degree of freedom unavoidable in 2D semiconducting materials with honeycomb structure. We claim that this is the key ingredient for understanding the nonhydrogenic exciton spectra that was missing so far.

  1. Exciton-driven highly hyperthermal O-atom desorption from nanostructured CaO

    SciTech Connect

    Sushko, Petr V.; Shluger, Alexander L.; Joly, Alan G.; Beck, Kenneth M.; Hess, Wayne P.

    2011-01-27

    We report qualitatively new highly-hyperthermal (HHT) oxygen atom emission from nanostructured CaO excited by 6.4 eV nanosecond laser pulses. The kinetic energy distribution of emitted O-atoms peaks at 0.7 eV, which is over four times greater than previously observed. Excitation of MgO and CaO nanostructures with UV laser pulses is known to result in thermal and hyperthermal emission of oxygen atoms when photons with energies below and above the band gap, respectively, are used. The highly energetic atomic desorption we observe, following bulk excitation, challenges the conventional view that bulk excitation can only induce thermal desorption. Using density functional theory and an embedded cluster method, we propose a mechanism for this HHT feature based on the interaction of surface holes with bulk excitons. These experimental and theoretical results suggest that specific atomic desorption mechanisms in wide-bandgap materials can be controlled by selective electronic excitation of not only the surface but also the bulk of these materials

  2. Quantum confinement in semiconductor nanofilms: Optical spectra and multiple exciton generation

    NASA Astrophysics Data System (ADS)

    Khmelinskii, Igor; Makarov, Vladimir I.

    2016-04-01

    We report optical absorption and photoluminescence (PL) spectra of Si and SnO2 nanocrystalline films in the UV-vis-NIR range, featuring discrete bands resulting from transverse quantum confinement, observed in the optical spectra of nanofilms for the first time ever. The film thickness ranged from 3.9 to 12.2 nm, depending on the material. The results are interpreted within the particle-in-a-box model, with infinite walls. The calculated values of the effective electron mass are independent on the film thickness and equal to 0.17mo (Si) and 0.21mo (SnO2), with mo the mass of the free electron. The second calculated model parameter, the quantum number n of the HOMO (valence band), was also thickness-independent: 8.00 (Si) and 7.00 (SnO2). The transitions observed in absorption all start at the level n and correspond to Δn = 1, 2, 3, …. The photoluminescence bands exhibit large Stokes shifts, shifting to higher energies with increased excitation energy. In effect, nanolayers of Si, an indirect-gap semiconductor, behave as a direct-gap semiconductor, as regards the transverse-quantized level system. A prototype Si-SnO2 nanofilm photovoltaic cell demonstrated photoelectron quantum yields achieving 2.5, showing clear evidence of multiple exciton generation, for the first time ever in a working nanofilm device.

  3. Symmetry breaking and excitonic effects on optical properties of defective nanographenes

    NASA Astrophysics Data System (ADS)

    Noguchi, Yoshifumi; Sugino, Osamu

    2015-02-01

    We investigate optical properties of the nanographene family and predict a defect induced effect by utilizing the all-electron first-principles GW+Bethe-Salpeter equation (BSE) method based on the many-body perturbation theory. As an accuracy check of the GW+BSE, photoabsorption spectra are calculated for a grossly warped nanographene (C80H30), which was very recently synthesized [Kawasumi et al., Nat. Chem. 5, 739-744 (2013)]. The calculated spectra are found to faithfully reproduce the shape, height, and position of the measured peaks. Then the method is applied to the flat nanographene without defect (C24H12 and C38H16), the curved ones with single defect (C20H10, C28H14, and C32H16), and fragments of C80H30 with double defect (C36H16 and C42H20). The existence of the defects significantly changes the optical spectra. In particular, the interaction between the defects is found to break the symmetry of the atomic geometries and enhance the excitonic effect, thereby generating the extra peaks at the lower photon energy side of the main peak. The present results might help explain the origin of the first two peaks experimentally observed for C80H30.

  4. Broadband optical transparency in plasmonic nanocomposite polymer films via exciton-plasmon energy transfer.

    PubMed

    Dhama, R; Rashed, A R; Caligiuri, V; El Kabbash, M; Strangi, G; De Luca, A

    2016-06-27

    Inherent absorptive losses affect the performance of all plasmonic devices, limiting their fascinating applications in the visible range. Here, we report on the enhanced optical transparency obtained as a result of the broadband mitigation of optical losses in nanocomposite polymeric films, embedding core-shell quantum dots (CdSe@ZnS QDs) and gold nanoparticles (Au-NPs). Exciton-plasmon coupling enables non-radiative energy transfer processes from QDs to metal NPs, resulting in gain induced transparency of the hybrid flexible systems. Experimental evidences, such as fluorescence quenching and modifications of fluorescence lifetimes confirm the presence of this strong coupling between plexcitonic elements. Measures performed by means of an ultra-fast broadband pump-probe setup demonstrate loss compensation of gold NPs dispersed in plastic network in presence of gain. Furthermore, we compare two films containing different concentrations of gold NPs and same amount of QDs, to investigate the role of acceptor concentration (Au-NPs) in order to promote an effective and efficient energy transfer mechanism. Gain induced transparency in bulk systems represents a promising path towards the realization of loss compensated plasmonic devices. PMID:27410615

  5. Adaptive optics assisted reconfigurable liquid-driven optical switch

    NASA Astrophysics Data System (ADS)

    Fuh, Yiin-Kuen; Huang, Wei-Chi

    2013-07-01

    This study demonstrates a mechanical-based, liquid-driven optical switch integrated with adaptive optics and a reconfigurable black liquid (dye-doped liquid). The device aperture can be continuously tuned between 0.6 and 6.9 mm, precisely achieved by a syringe pump for volume control. Adaptive optics (AO) capability and possible enhancement of the lost power intensity of the ink-polluted glass plate have also been experimentally investigated. While measuring power intensity with/without AO indicates only a marginal difference of ˜1%, a significant difference of 3 s in the response characteristic of "switching on" time can be observed. An extremely high contrast ratio of ˜105 for a red-colored light is achieved.

  6. Steady-state propagation of ultrashort optical pulses in semiconductor excitonic medium

    NASA Astrophysics Data System (ADS)

    Talanina, Irina B.

    1996-06-01

    The form-invariant coherent pulse propagation in semiconductors excited at the 1 s -exciton resonance is studied analytically with the reduced semiconductor Maxwell-Bloch equations. The sech-shaped pulse solution for the electric field is presented. The effects of Coulomb interactions between excitons and spatial dispersion are discussed. Applications to CdS and CdSe crystals are made.

  7. Influence of the sign of the coupling on the temperature dependence of optical properties of one-dimensional exciton models

    NASA Astrophysics Data System (ADS)

    Cruzeiro, L.

    2008-10-01

    A new physical cause for a temperature-dependent double peak in exciton systems is put forward within a thermal equilibrium approach for the calculation of optical properties of exciton systems. Indeed, it is found that one-dimensional exciton systems with only one molecule per unit cell can have an absorption spectrum characterized by a double peak provided that the coupling between excitations in different molecules is positive. The two peaks, whose relative intensities vary with temperature, are located around the exciton band edges, being separated by an energy of approximately 4V, where V is the average coupling between nearest neighbours. For small amounts of diagonal and off-diagonal disorder, the contributions from the intermediate states in the band are also visible as intermediate structure between the two peaks, this being enhanced for systems with periodic boundary conditions. At a qualitative level, these results correlate well with experimental observations in the molecular aggregates of the thiacarbocyanine dye THIATS and in the organic crystals of acetanilide and N-methylacetamide.

  8. Excitons in ultrathin organic-inorganic perovskite crystals

    NASA Astrophysics Data System (ADS)

    Yaffe, Omer; Chernikov, Alexey; Norman, Zachariah M.; Zhong, Yu; Velauthapillai, Ajanthkrishna; van der Zande, Arend; Owen, Jonathan S.; Heinz, Tony F.

    2015-07-01

    We demonstrate the formation of large sheets of layered organic-inorganic perovskite (OIPC) crystals, as thin as a single unit cell, prepared by mechanical exfoliation. The resulting two-dimensional OIPC nanosheets of 2.4 nm thickness are direct semiconductors with an optical band gap of 2.4 eV. They exhibit unusually strong light-matter interaction with an optical absorption as high as 25% at the main excitonic resonance, as well as bright photoluminescence. We extract an exciton binding energy of 490 meV from measurement of the series of excited exciton states. The properties of the excitons are shown to be strongly influenced by the changes in the dielectric surroundings. The environmental sensitivity of these ultrathin OIPC sheets is further reflected in the strong suppression of a thermally driven phase transition present in the bulk crystals.

  9. Arnold diffusion in a driven optical lattice

    NASA Astrophysics Data System (ADS)

    Boretz, Yingyue; Reichl, L. E.

    2016-03-01

    The effect of time-periodic forces on matter has been a topic of growing interest since the advent of lasers. It is known that dynamical systems with 2.5 or more degrees of freedom are intrinsically unstable. As a consequence, time-periodic driven systems can experience large excursions in energy. We analyze the classical and quantum dynamics of rubidium atoms confined to a time-periodic optical lattice with 2.5 degrees of freedom. When the laser polarizations are orthogonal, the system consists of two 1.5 uncoupled dynamical systems. When laser polarizations are turned away from orthogonal, an Arnold web forms and the dynamics undergoes a fundamental change. For parallel polarizations, we find huge random excursions in the rubidium atom energies and significant entanglement of energies in the quantum dynamics.

  10. Arnold diffusion in a driven optical lattice.

    PubMed

    Boretz, Yingyue; Reichl, L E

    2016-03-01

    The effect of time-periodic forces on matter has been a topic of growing interest since the advent of lasers. It is known that dynamical systems with 2.5 or more degrees of freedom are intrinsically unstable. As a consequence, time-periodic driven systems can experience large excursions in energy. We analyze the classical and quantum dynamics of rubidium atoms confined to a time-periodic optical lattice with 2.5 degrees of freedom. When the laser polarizations are orthogonal, the system consists of two 1.5 uncoupled dynamical systems. When laser polarizations are turned away from orthogonal, an Arnold web forms and the dynamics undergoes a fundamental change. For parallel polarizations, we find huge random excursions in the rubidium atom energies and significant entanglement of energies in the quantum dynamics. PMID:27078351

  11. Optical Characterization of Strong UV Luminescence Emitted from the Excitonic Edge of Nickel Oxide Nanotowers

    PubMed Central

    Ho, Ching-Hwa; Kuo, Yi-Ming; Chan, Ching-Hsiang; Ma, Yuan-Ron

    2015-01-01

    NiO had been claimed to have the potential for application in transparent conducting oxide, electrochromic device for light control, and nonvolatile memory device. However, the detailed study of excitonic transition and light-emission property of NiO has rarely been explored to date. In this work, we demonstrate strong exciton-complex emission of high-quality NiO nanotowers grown by hot-filament metal-oxide vapor deposition with photoluminescence as an evaluation tool. Fine and clear emission features coming from the excitonic edge of the NiO are obviously observed in the photoluminescence spectra. A main excitonic emission of ~3.25 eV at 300 K can be decomposed into free exciton, bound excitons, and donor-acceptor-pair irradiations at lowered temperatures down to 10 K. The band-edge excitonic structure for the NiO nanocrystals has been evaluated and analyzed by transmission and thermoreflectacne measurements herein. All the experimental results demonstrate the cubic NiO thin-film nanotower is an applicable direct-band-gap material appropriate for UV luminescence and transparent-conducting-oxide applications. PMID:26506907

  12. Optical Characterization of Strong UV Luminescence Emitted from the Excitonic Edge of Nickel Oxide Nanotowers

    NASA Astrophysics Data System (ADS)

    Ho, Ching-Hwa; Kuo, Yi-Ming; Chan, Ching-Hsiang; Ma, Yuan-Ron

    2015-10-01

    NiO had been claimed to have the potential for application in transparent conducting oxide, electrochromic device for light control, and nonvolatile memory device. However, the detailed study of excitonic transition and light-emission property of NiO has rarely been explored to date. In this work, we demonstrate strong exciton-complex emission of high-quality NiO nanotowers grown by hot-filament metal-oxide vapor deposition with photoluminescence as an evaluation tool. Fine and clear emission features coming from the excitonic edge of the NiO are obviously observed in the photoluminescence spectra. A main excitonic emission of ~3.25 eV at 300 K can be decomposed into free exciton, bound excitons, and donor-acceptor-pair irradiations at lowered temperatures down to 10 K. The band-edge excitonic structure for the NiO nanocrystals has been evaluated and analyzed by transmission and thermoreflectacne measurements herein. All the experimental results demonstrate the cubic NiO thin-film nanotower is an applicable direct-band-gap material appropriate for UV luminescence and transparent-conducting-oxide applications.

  13. Bi donor hyperfine state populations studied by optical transitions of donor bound excitons in enriched {sup 28}Si

    SciTech Connect

    Ilkhchy, K. Saeedi; Steger, M.; Thewalt, M. L. W.; Abrosimov, N.; Riemann, H.; Becker, P.; Pohl, H.-J.

    2013-12-04

    We report on the first optical studies of Bi donor bound excitons in {sup 28}Si, using absorption rather than emission spectroscopy, and a new noncontact photoconductivity method which has much higher sensitivity and spectral resolution than photoluminescence spectroscopy. Individual hyperfine components of this potential semiconductor qubit can be resolved under an applied magnetic field, and we find that strong nonresonant optical hyperpolarization towards both the I{sub z} = +9/2 and −9/2 hyperfine states can be observed, depending on the intensity of the above-gap excitation.

  14. Resonant optical reflection by a periodic system of the quantum well excitons at the second quantum state

    SciTech Connect

    Chaldyshev, V. V.; Poddubny, A. N.; Vasil'ev, A. P.; Chen Yuechao; Liu Zhiheng

    2011-02-14

    A periodic multiple quantum well GaAs/AlGaAs structure was designed, grown, and characterized in order to reveal resonant features in optical spectra when the Bragg resonance was tuned to the second quantum state x(e2-hh2) of the heavy-hole exciton-polaritons in the multiple quantum wells. This double resonance was demonstrated by tuning the incident angle of the light as well as by comparison with a single quantum well structure. A significant enhancement of the light-matter interaction was observed, which manifests itself by strong resonant optical reflection and electroreflection.

  15. Stimulated emission and optical gain in PbSe quantum dot-doped liquid-core optical fiber based on multi-exciton state

    NASA Astrophysics Data System (ADS)

    Zhang, Lei; Zhang, Bing; Li, Shuai; Zhu, Qiang; Zheng, Youjin

    2016-06-01

    We studied the properties of stimulated emission and optical gain of 4.4 nm PbSe quantum dot (QD)-doped liquid-core optical fiber based on multi-exciton state under strong pumping condition as a function of QD solution concentration, fiber length and pump power in order to establish the conditions to maximize stimulated emission intensities and optical gain. Auger recombination lifetime and internal quantum efficiency (IQE) were introduced in the multi-exciton model for calculation. Shifts of the spectral peak position were observed and explained in detail. The narrowing spectral half band width and the super linear intensity dependence of the output power with the pump accounted for the generation of stimulated emission. The maximal optical gain of ~30 dB was obtained which was larger than that of the single-exciton model under the same fiber parameters. Our interesting results might be useful in the design of optical fiber-based amplifiers and lasers.

  16. Optical and spin properties of localized and free excitons in GaBi x As1‑x /GaAs multiple quantum wells

    NASA Astrophysics Data System (ADS)

    Balanta, M. A. G.; Kopaczek, J.; Orsi Gordo, V.; Santos, B. H. B.; Rodrigues, A. D.; Galeti, H. V. A.; Richards, R. D.; Bastiman, F.; David, J. P. R.; Kudrawiec, R.; Galvão Gobato, Y.

    2016-09-01

    Raman spectroscopy and magneto-photoluminescence measurements under high magnetic fields were used to investigate the optical and spin properties of GaBiAs/GaAs multiple quantum wells (MQWs). An anomalous negative diamagnetic energy shift was observed at higher temperatures and higher laser intensities, which was associated to a sign inversion of hole effective mass in these structures. In addition, an enhancement of the polarization degree with decreasing of laser intensity was observed (experimental condition where the emission is dominated by localized excitons). This effect was explained by changes of spin relaxation and exciton recombination times due to exciton localization by disorder.

  17. Optical spectroscopy of free excitons in a CuInS{sub 2} chalcopyrite semiconductor compound

    SciTech Connect

    Mudryi, A. V. Ivanyukovich, A. V.; Yakushev, M. V.; Martin, R.; Saad, A.

    2008-01-15

    The spectra of reflectance and luminescence of high-quality CuInS{sub 2} single crystals grown by oriented crystallization are studied at the temperature 4.2 K. In the region of the fundamental absorption edge, the two excitonic resonance reflectance peaks, nondegenerate peak A at the energy {approx}1.5356 eV and doubly degenerate peak BC at the energy {approx}1.5567 eV, and the luminescence signal produced by free and bound excitons are observed. The luminescence lines, A{sub UPB} at {approx}1.5361 eV and A{sub LPB} at {approx}1.5347 eV, with a half-width {approx}1 meV, are attributed to exciton-polariton recombination. From the experimentally observed energy position of the exciton ground state and excited states, the binding energy of free excitons is determined to be {approx}18.5 meV. In studying the photoluminescence in magnetic fields up to 10 T, a diamagnetic shift of the ground state of free excitons A is observed.

  18. Polaron master equation theory of pulse-driven phonon-assisted population inversion and single-photon emission from quantum-dot excitons

    NASA Astrophysics Data System (ADS)

    Manson, Ross; Roy-Choudhury, Kaushik; Hughes, Stephen

    2016-04-01

    We introduce an intuitive and semianalytical polaron master equation approach to model pulse-driven population inversion and emitted single photons from a quantum dot exciton. The master equation theory allows one to identify important phonon-induced scattering rates analytically and fully includes the role of the time-dependent pump field. As an application of the theory, we first study a quantum dot driven by a time-varying laser pulse on and off resonance, showing the population inversion caused by acoustic phonon emission in direct agreement with recent experiments of Quilter et al. [Phys. Rev. Lett. 114, 137401 (2015), 10.1103/PhysRevLett.114.137401]. We then model quantum dots in weakly coupled cavities and show the difference in population response between exciton-driven and cavity-driven systems. Finally, we assess the nonresonant phonon-assisted loading scheme with a quantum dot resonantly coupled to a cavity as a deterministic single-photon source. We also compare and contrast the important single photon figures of merit with direct Rabi oscillation of the population using a resonant π pulse, and show that the resonant scheme is much more efficient.

  19. Optical Absorption Spectra and Excitons of Dye-Substrate Interfaces: Catechol on TiO2(110).

    PubMed

    Mowbray, Duncan John; Migani, Annapaola

    2016-06-14

    Optimizing the photovoltaic efficiency of dye-sensitized solar cells (DSSC) based on staggered gap heterojunctions requires a detailed understanding of sub-band gap transitions in the visible from the dye directly to the substrate's conduction band (CB) (type-II DSSCs). Here, we calculate the optical absorption spectra and spatial distribution of bright excitons in the visible region for a prototypical DSSC, catechol on rutile TiO2(110), as a function of coverage and deprotonation of the OH anchoring groups. This is accomplished by solving the Bethe-Salpeter equation (BSE) based on hybrid range-separated exchange and correlation functional (HSE06) density functional theory (DFT) calculations. Such a treatment is necessary to accurately describe the interfacial level alignment and the weakly bound charge transfer transitions that are the dominant absorption mechanism in type-II DSSCs. Our HSE06 BSE spectra agree semiquantitatively with spectra measured for catechol on anatase TiO2 nanoparticles. Our results suggest deprotonation of catechol's OH anchoring groups, while being nearly isoenergetic at high coverages, shifts the onset of the absorption spectra to lower energies, with a concomitant increase in photovoltaic efficiency. Further, the most relevant bright excitons in the visible region are rather intense charge transfer transitions with the electron and hole spatially separated in both the [110] and [001] directions. Such detailed information on the absorption spectra and excitons is only accessible via periodic models of the combined dye-substrate interface. PMID:27183273

  20. Optical properties of one- and two-dimensional excitons in m-plane ZnO/MgZnO multiple quantum wells

    NASA Astrophysics Data System (ADS)

    Chen, H. R.; Tsai, C. Y.; Huang, Y. C.; Kuo, C. C.; Hsu, H. C.; Hsieh, W. F.

    2016-03-01

    Five pairs of ZnO/Zn0.9Mg0.1O multiple quantum wells (MQWs) with fixed barrier thickness of 55 nm and three well widths of 4, 8 and 16 nm have been grown on m-plane sapphires by pulsed laser deposition. Due to 2D quantum confinement with decreasing well width, the emission of excitons bound to the basal-plane stacking faults, which are one-dimensionally confined in MQWs, encounters larger blue shift than that of the near-band edge excitons. Furthermore, remarkably reducing coupling of free excitons with A 1 longitudinal optical phonons is closely correlated with increasing exciton binding energy but enhanced coupling of E 2-low phonons is a result of increasing interaction with the interface phonons with decreasing well width.

  1. Ultrafast optical spectroscopy of large-momentum excitons in GaAs.

    PubMed

    Göger, G; Betz, M; Leitenstorfer, A; Bichler, M; Wegscheider, W; Abstreiter, G

    2000-06-19

    Highly energetic excitons with wave vectors much larger than that of an absorbed photon are excited in thin GaAs films. We observe propagation beats between three polariton modes up to 300 meV above the absorption edge employing femtosecond transmission spectroscopy. The dispersion relations of the coherent excitations are measured. Ultrafast exciton damping via scattering with nonequilibrium carriers and with phonons is investigated. The dynamics is found to deviate strongly from the relaxation of free carriers. Theoretical simulations are in quantitative agreement with the data. PMID:10991061

  2. Exciton storage in type-II quantum dots using the optical Aharonov-Bohm effect

    SciTech Connect

    Climente, Juan I.; Planelles, Josep

    2014-05-12

    We investigate the bright-to-dark exciton conversion efficiency in type-II quantum dots subject to a perpendicular magnetic field. To this end, we take the exciton storage protocol recently proposed by Simonin and co-workers [Phys. Rev. B 89, 075304 (2014)] and simulate its coherent dynamics. We confirm the storage is efficient in perfectly circular structures subject to weak external electric fields, where adiabatic evolution is dominant. In practice, however, the efficiency rapidly degrades with symmetry lowering. Besides, the use of excited states is likely unfeasible owing to the fast decay rates. We then propose an adaptation of the protocol which does not suffer from these limitations.

  3. Optical microcavities enhance the exciton coherence length and eliminate vibronic coupling in J-aggregates

    SciTech Connect

    Spano, F. C.

    2015-05-14

    The properties of polaritons in J-aggregate microcavities are explored using a Hamiltonian which treats exciton-vibrational coupling and exciton-photon coupling on equal footing. When the cavity mode is resonant with the lowest-energy (0-0) transition in the J-aggregate, two polaritons are formed, the lowest-energy polariton (LP) and its higher-energy partner (P{sub 1}), separated by the Rabi splitting. Strong coupling between the material and cavity modes leads to a decoupling of the exciton and vibrational degrees of freedom and an overall reduction of disorder within the LP. Such effects lead to an expanded material coherence length in the LP which leads to enhanced radiative decay rates. Additional spectral signatures include an amplification of the 0-0 peak coincident with a reduction in the 0-1 peak in the photoluminescence spectrum. It is also shown that the same cavity photon responsible for the LP/P{sub 1} splitting causes comparable splittings in the higher vibronic bands due to additional resonances between vibrationally excited states in the electronic ground state manifold and higher energy vibronic excitons.

  4. Exciton-related nonlinear optical properties in cylindrical quantum dots with asymmetric axial potential: combined effects of hydrostatic pressure, intense laser field, and applied electric field.

    PubMed

    Zapata, Alejandro; Acosta, Ruben E; Mora-Ramos, Miguel E; Duque, Carlos A

    2012-01-01

    : The exciton binding energy of an asymmetrical GaAs-Ga1-xAlxAs cylindrical quantum dot is studied with the use of the effective mass approximation and a variational calculation procedure. The influence on this quantity of the application of a direct-current electric field along the growth direction of the cylinder, together with that of an intense laser field, is particularly considered. The resulting states are used to calculate the exciton-related nonlinear optical absorption and optical rectification, whose corresponding resonant peaks are reported as functions of the external probes, the quantum dot dimensions, and the aluminum molar fraction in the potential barrier regions. PMID:22971418

  5. Dissipation-Induced Symmetry Breaking in a Driven Optical Lattice

    SciTech Connect

    Gommers, R.; Bergamini, S.; Renzoni, F.

    2005-08-12

    We analyze the atomic dynamics in an ac driven periodic optical potential which is symmetric in both time and space. We experimentally demonstrate that in the presence of dissipation the symmetry is broken, and a current of atoms through the optical lattice is generated as a result.

  6. Using bound exciton transitions to optically resolve neutral donor hyperfine states of various donor species in Silicon-28

    NASA Astrophysics Data System (ADS)

    Salvail, Jeff; Dluhy, Phillip; Saeedi, Kamyar; Szech, Michael; Riemann, Helge; Abromisov, Nikolai; Becker, Peter; Pohl, Hans-Joachim; Thewalt, Michael

    2014-03-01

    Phosphorus in silicon is established as a promising resource for use in quantum information processing tasks. The neutral donor hyperfine states have been shown to have record long coherence times, high fidelity gates via RF pulses, and projective readout via optical bound exciton transitions. As Shannon's theory of information tells us, we can process more information in an alphabet of more symbols, so there is motivation to look at donors with higher nuclear spin than the I = 1 / 2 of 31P, which provide access to Hilbert spaces of dimension greater than two. In this talk I will describe optical studies of the donors 75As (I = 3 / 2), 121Sb (I = 5 / 2), and 209Bi (I = 9 / 2) in 28Si.

  7. Repulsively bound exciton-biexciton states in high-spin fermions in optical lattices

    SciTech Connect

    Argueelles, A.; Santos, L.

    2011-03-15

    We show that the interplay between spin-changing collisions and quadratic Zeeman coupling provides a mechanism for the formation of repulsively bound composites in high-spin fermions, which we illustrate by considering spin flips in an initially polarized hard-core one-dimensional Mott insulator of spin-3/2 fermions. We show that after the flips the dynamics is characterized by the creation of two types of exciton-biexciton composites. We analyze the conditions for the existence of these bound states and discuss their intriguing properties. In particular we show that the effective mass and stability of the composites depends nontrivially on spin-changing collisions, on the quadratic Zeeman effect, and on the initial exciton localization. Finally, we show that the composites may remain stable against inelastic collisions, opening the possibility of interesting quantum composite phases.

  8. Correlated structural-optical study of single nanocrystals in a gap-bar antenna: effects of plasmonics on excitonic recombination pathways

    NASA Astrophysics Data System (ADS)

    Wang, Feng; Karan, Niladri S.; Nguyen, Hue Minh; Ghosh, Yagnaseni; Sheehan, Chris J.; Hollingsworth, Jennifer A.; Htoon, Han

    2015-05-01

    We performed time-correlated single-photon counting experiments on individual silica coated CdSe/CdS core/thick-shell nanocrystal quantum dots (a.k.a., giant NQDs [g-NQDs]), placed on the plasmonic gap-bar antennas. Optical properties were directly correlated with the scanning electron microscopy (SEM) images of g-NQD-plasmonic antenna coupled structures. The structures, in which the g-NQDs are located in the gap of the antenna, afford a coupling with up to 9.6 fold enhancement of radiative recombination rates. These coupled g-NQDs are also characterized by a strong enhancement of bi-exciton emission efficiency that increases with their radiative enhancement factor. By analysing these findings with a simple model, we show that the plasmonic field of the antenna does not alter the Auger recombination processes of the bi-exciton states. As a result, enhancements of the single and bi-exciton radiative recombination rates lead directly to bi-exciton emission enhancement. These findings suggest that a plasmonic field can be utilized effectively in achieving a strong bi-exciton emission that is needed for photon pair generation and plasmon-assisted lasing.We performed time-correlated single-photon counting experiments on individual silica coated CdSe/CdS core/thick-shell nanocrystal quantum dots (a.k.a., giant NQDs [g-NQDs]), placed on the plasmonic gap-bar antennas. Optical properties were directly correlated with the scanning electron microscopy (SEM) images of g-NQD-plasmonic antenna coupled structures. The structures, in which the g-NQDs are located in the gap of the antenna, afford a coupling with up to 9.6 fold enhancement of radiative recombination rates. These coupled g-NQDs are also characterized by a strong enhancement of bi-exciton emission efficiency that increases with their radiative enhancement factor. By analysing these findings with a simple model, we show that the plasmonic field of the antenna does not alter the Auger recombination processes of the bi-exciton

  9. Excitons in nanorings. The signature of quantum phases in optical emission

    NASA Astrophysics Data System (ADS)

    Govorov, Alexander; Ulloa, Sergio

    2002-03-01

    When a quantum charged particle moves along a closed trajectory in an external magnetic field, the Aharonov-Bohm (AB) effect can occur, caused by quantum interference between paths with different phases. However, excitons in solids are neutral and hence a cursory analysis would not predict the AB effect. Nevertheless, we demonstrate here that a strong magnetic interference effect for neutral particles can exist, such as the polarizable excitons in quantum-ring structures. This phenomenon is akin to the Aharonov-Anandan quantum phases acquired under a cyclic evolution of the Hamiltonian. With increasing normal magnetic field, the ground state of the exciton acquires a nonzero angular momentum due to a net microscopic phase in the electron-hole pair. Under these conditions, the photoluminescence becomes suppressed in well-defined intervals of magnetic field, which depend on the degree of correlation of the two-particle motion. We demonstrate theoretically this novel magnetic interference effect using models of type-II quantum dots and InAs self-assembled quantum rings [1]. 1. A. Lorke et al., Phys. Rev. Lett. 84, 2223 (2000).

  10. Cell Signaling Experiments Driven by Optical Manipulation

    PubMed Central

    Difato, Francesco; Pinato, Giulietta; Cojoc, Dan

    2013-01-01

    Cell signaling involves complex transduction mechanisms in which information released by nearby cells or extracellular cues are transmitted to the cell, regulating fundamental cellular activities. Understanding such mechanisms requires cell stimulation with precise control of low numbers of active molecules at high spatial and temporal resolution under physiological conditions. Optical manipulation techniques, such as optical tweezing, mechanical stress probing or nano-ablation, allow handling of probes and sub-cellular elements with nanometric and millisecond resolution. PicoNewton forces, such as those involved in cell motility or intracellular activity, can be measured with femtoNewton sensitivity while controlling the biochemical environment. Recent technical achievements in optical manipulation have new potentials, such as exploring the actions of individual molecules within living cells. Here, we review the progress in optical manipulation techniques for single-cell experiments, with a focus on force probing, cell mechanical stimulation and the local delivery of active molecules using optically manipulated micro-vectors and laser dissection. PMID:23698758

  11. Laser-driven polyplanar optic display

    SciTech Connect

    Veligdan, J.T.; Biscardi, C.; Brewster, C.; DeSanto, L.; Beiser, L.

    1998-01-01

    The Polyplanar Optical Display (POD) is a unique display screen which can be used with any projection source. This display screen is 2 inches thick and has a matte-black face which allows for high contrast images. The prototype being developed is a form, fit and functional replacement display for the B-52 aircraft which uses a monochrome ten-inch display. The new display uses a 200 milliwatt green solid-state laser (532 nm) as its optical source. In order to produce real-time video, the laser light is being modulated by a Digital Light Processing (DLP) chip manufactured by Texas Instruments, Inc. A variable astigmatic focusing system is used to produce a stigmatic image on the viewing face of the POD. In addition to the optical design, the authors discuss the DLP chip, the optomechanical design and viewing angle characteristics.

  12. Optically Induced Nuclear Spin Polarization in the Quantum Hall Regime: The Effect of Electron Spin Polarization through Exciton and Trion Excitations

    NASA Astrophysics Data System (ADS)

    Akiba, K.; Kanasugi, S.; Yuge, T.; Nagase, K.; Hirayama, Y.

    2015-07-01

    We study nuclear spin polarization in the quantum Hall regime through the optically pumped electron spin polarization in the lowest Landau level. The nuclear spin polarization is measured as a nuclear magnetic field BN by means of the sensitive resistive detection. We find the dependence of BN on the filling factor nonmonotonic. The comprehensive measurements of BN with the help of the circularly polarized photoluminescence measurements indicate the participation of the photoexcited complexes, i.e., the exciton and trion (charged exciton), in nuclear spin polarization. On the basis of a novel estimation method of the equilibrium electron spin polarization, we analyze the experimental data and conclude that the filling factor dependence of BN is understood by the effect of electron spin polarization through excitons and trions.

  13. Optically Induced Nuclear Spin Polarization in the Quantum Hall Regime: The Effect of Electron Spin Polarization through Exciton and Trion Excitations.

    PubMed

    Akiba, K; Kanasugi, S; Yuge, T; Nagase, K; Hirayama, Y

    2015-07-10

    We study nuclear spin polarization in the quantum Hall regime through the optically pumped electron spin polarization in the lowest Landau level. The nuclear spin polarization is measured as a nuclear magnetic field B(N) by means of the sensitive resistive detection. We find the dependence of B(N) on the filling factor nonmonotonic. The comprehensive measurements of B(N) with the help of the circularly polarized photoluminescence measurements indicate the participation of the photoexcited complexes, i.e., the exciton and trion (charged exciton), in nuclear spin polarization. On the basis of a novel estimation method of the equilibrium electron spin polarization, we analyze the experimental data and conclude that the filling factor dependence of B(N) is understood by the effect of electron spin polarization through excitons and trions. PMID:26207494

  14. Correlated structural-optical study of single nanocrystals in a gap-bar antenna: effects of plasmonics on excitonic recombination pathways.

    PubMed

    Wang, Feng; Karan, Niladri S; Nguyen, Hue Minh; Ghosh, Yagnaseni; Sheehan, Chris J; Hollingsworth, Jennifer A; Htoon, Han

    2015-06-01

    We performed time-correlated single-photon counting experiments on individual silica coated CdSe/CdS core/thick-shell nanocrystal quantum dots (a.k.a., giant NQDs [g-NQDs]), placed on the plasmonic gap-bar antennas. Optical properties were directly correlated with the scanning electron microscopy (SEM) images of g-NQD-plasmonic antenna coupled structures. The structures, in which the g-NQDs are located in the gap of the antenna, afford a coupling with up to 9.6 fold enhancement of radiative recombination rates. These coupled g-NQDs are also characterized by a strong enhancement of bi-exciton emission efficiency that increases with their radiative enhancement factor. By analysing these findings with a simple model, we show that the plasmonic field of the antenna does not alter the Auger recombination processes of the bi-exciton states. As a result, enhancements of the single and bi-exciton radiative recombination rates lead directly to bi-exciton emission enhancement. These findings suggest that a plasmonic field can be utilized effectively in achieving a strong bi-exciton emission that is needed for photon pair generation and plasmon-assisted lasing. PMID:25947939

  15. Optically driven bacterial screw of Archimedes

    NASA Astrophysics Data System (ADS)

    Robbins, J. R.; Tierney, D. A.; Schmitzer, H.

    2006-01-01

    The linear momentum transfer from photons to asymmetrically shaped structures generates an optomechanical rotation, but these micron-sized structures require costly, high-precision fabrication. Nature, however, provides a great diversity of engineered forms and dead, but rigid, asymmetrically shaped bacteria can provide a low cost alternative. In this work, we show that helical bacteria rotate very quickly in optical tweezers. Their rotation is fast enough to create a strong whirl, such that they may act as micropumps in thin capillaries.

  16. Emulation of lossless exciton-polariton condensates by dual-core optical waveguides: stability, collective modes, and dark solitons.

    PubMed

    Salasnich, Luca; Malomed, Boris A; Toigo, Flavio

    2014-10-01

    We propose a possibility to simulate the exciton-polariton (EP) system in the lossless limit, which is not currently available in semiconductor microcavities, by means of a simple optical dual-core waveguide, with one core carrying the nonlinearity and operating close to the zero-group-velocity-dispersion point, and the other core being linear and dispersive. Both two-dimensional (2D) and one-dimensional (1D) EP systems may be emulated by means of this optical setting. In the framework of this system, we find that, while the uniform state corresponding to the lower branch of the nonlinear dispersion relation is stable against small perturbations, the upper branch is always subject to the modulational instability. The stability and instability are verified by direct simulations too. We analyze collective excitations on top of the stable lower-branch state, which include a Bogoliubov-like gapless mode and a gapped one. Analytical results are obtained for the corresponding sound velocity and energy gap. The effect of a uniform phase gradient (superflow) on the stability is considered too, with a conclusion that the lower-branch state becomes unstable above a critical wave number of the flux. Finally, we demonstrate that the stable 1D state may carry robust dark solitons. PMID:25375613

  17. Temperature-dependent exciton resonance energies and their correlation with IR-active optical phonon modes in β-Ga2O3 single crystals

    NASA Astrophysics Data System (ADS)

    Onuma, T.; Saito, S.; Sasaki, K.; Goto, K.; Masui, T.; Yamaguchi, T.; Honda, T.; Kuramata, A.; Higashiwaki, M.

    2016-03-01

    Temperature-dependent exciton resonance energies Eexciton in β-Ga2O3 single crystals are studied by using polarized reflectance measurement. The Eexciton values exhibit large energy changes in the range of 179-268 meV from 5 to 300 K. The IR-active Au and Bu optical phonon modes are selectively observed in the IR spectroscopic ellipsometry spectra by reflecting the polarization selection rules. The longitudinal optical (LO) phonon energies can be divided into three ranges: ℏωLO = 35-48, 70-73, and 88-99 meV. The broadening parameters, which are obtained from the reflectance measurements, correspond to the lower two ranges of ℏωLO at low temperature and 75 meV above 150 K. The large Eexciton changes with temperature in β-Ga2O3 are found to be originated from the exciton-LO-phonon interaction.

  18. Excitonic surface lattice resonances

    NASA Astrophysics Data System (ADS)

    Humphrey, A. D.; Gentile, M. J.; Barnes, W. L.

    2016-08-01

    Electromagnetic resonances are important in controlling light at the nanoscale. The most studied such resonance is the surface plasmon resonance that is associated with metallic nanostructures. Here we explore an alternative resonance, the surface exciton-polariton resonance, one based on excitonic molecular materials. Our study is based on analytical and numerical modelling. We show that periodic arrays of suitable molecular nanoparticles may support surface lattice resonances that arise as a result of coherent interactions between the particles. Our results demonstrate that excitonic molecular materials are an interesting alternative to metals for nanophotonics; they offer the prospect of both fabrication based on supramolecular chemistry and optical functionality arising from the way the properties of such materials may be controlled with light.

  19. Azimuthons and pattern formation in annularly confined exciton-polariton Bose-Einstein condensates

    NASA Astrophysics Data System (ADS)

    Li, Guangyao

    2016-01-01

    We present numerical analysis of steady states in a two-component (spinor) driven-dissipative quantum fluid formed by condensed exciton polaritons in an annular optically induced trap. We demonstrate that an incoherent ring-shaped optical pump creating the exciton-polariton confinement supports the existence of stationary and rotating azimuthon steady states with azimuthally modulated density associated with Josephson vortices. Such states can be imprinted by coherent light pulses with a defined orbital angular momentum, as well as generated spontaneously in the presence of thermal noise.

  20. Distributed fibre optic strain measurements on a driven pile

    NASA Astrophysics Data System (ADS)

    Woschitz, Helmut; Monsberger, Christoph; Hayden, Martin

    2016-05-01

    In civil engineering pile systems are used in unstable areas as a foundation of buildings or other structures. Among other parameters, the load capacity of the piles depends on their length. A better understanding of the mechanism of load-transfer to the soil would allow selective optimisation of the system. Thereby, the strain variations along the loaded pile are of major interest. In this paper, we report about a field trial using an optical backscatter reflectometer for distributed fibre-optic strain measurements along a driven pile. The most significant results gathered in a field trial with artificial pile loadings are presented. Calibration results show the performance of the fibre-optic system with variations in the strain-optic coefficient.

  1. Laser induced magneto-Raman optical gain of an exciton and a biexciton in a CdTe/ZnTe quantum dot

    NASA Astrophysics Data System (ADS)

    Sujanah, P.; John Peter, A.; Lee, Chang Woo

    2016-06-01

    Magnetic field and laser field amplitude dependent electronic and optical properties of exciton and biexciton in a CdTe/ZnTe quantum dot nanostructure are brought out taking into account the spatial confinement effect. Binding energies of exciton and biexciton as functions of laser field amplitude and magnetic field strength are computed in a CdTe/ZnTe quantum dot for the constant dot radius 30 Å. Oscillator strength, resonant absorption coefficients and resonant optical Raman intensity of the exciton and biexciton as a function of laser field amplitude are obtained in the presence of magnetic field strength in a CdTe/ZnTe quantum dot. The laser field induced magneto-Raman gain is studied for a constant dot radii. The Coulomb interaction energy which is involved in Hartree potential is obtained numerically. The result shows that the applications of magnetic field strength and the laser field amplitude alter the electronic and optical properties considerably in the CdTe/ZnTe quantum dot.

  2. Exciton Transport in Organic Semiconductors

    NASA Astrophysics Data System (ADS)

    Menke, Stephen Matthew

    Photovoltaic cells based on organic semiconductors are attractive for their use as a renewable energy source owing to their abundant feedstock and compatibility with low-cost coating techniques on flexible substrates. In contrast to photovoltaic cells based traditional inorganic semiconductors, photon absorption in an organic semiconductor results in the formation of a coulombically bound electron-hole pair, or exciton. The transport of excitons, consequently, is of critical importance as excitons mediate the interaction between charge and light in organic photovoltaic cells (OPVs). In this dissertation, a strong connection between the fundamental photophysical parameters that control nanoscopic exciton energy transfer and the mesoscopic exciton transport is established. With this connection in place, strategies for enhancing the typically short length scale for exciton diffusion (L D) can be developed. Dilution of the organic semiconductor boron subphthalocyanine chloride (SubPc) is found to increase the LD for SubPc by 50%. In turn, OPVs based on dilute layers of SubPc exhibit a 30% enhancement in power conversion efficiency. The enhancement in power conversion efficiency is realized via enhancements in LD, optimized optical spacing, and directed exciton transport at an exciton permeable interface. The role of spin, energetic disorder, and thermal activation on L D are also addressed. Organic semiconductors that exhibit thermally activated delayed fluorescence and efficient intersystem and reverse intersystem crossing highlight the balance between singlet and triplet exciton energy transfer and diffusion. Temperature dependent measurements for LD provide insight into the inhomogeneously broadened exciton density of states and the thermal nature of exciton energy transfer. Additional topics include energy-cascade OPV architectures and broadband, spectrally tunable photodetectors based on organic semiconductors.

  3. Optical and magnetic probes of hot singlet exciton fission in π-conjugated polymers for organic photovoltaic applications

    NASA Astrophysics Data System (ADS)

    Zhai, Yaxin; Olejnik, Ella; Vardeny, Z. Valy

    2015-09-01

    We used steady state and picosecond transient photoinduced absorption (PA), excitation dependence (EXPA(ω)) spectrum of the triplet exciton PA band, and its magneto-PA (MPA(B)) response to investigate singlet fission (SF) of hot-excitons into two separated triplet excitons in luminescent π-conjugated polymers. From the high energy step in the triplet EXPA(ω) spectrum of poly(dioctyloxy)-phenylenevinylene (DOO-PPV) films, we identified a hot-exciton SF (HE-SF) process having threshold energy at E≍2ET (=2.8 eV, where ET is the energy of the lowest lying triplet exciton), which is about 0.8 eV above the lowest singlet exciton energy. The picosecond transient PA with 3.1 eV pump excitation shows that in DOO-PPV film a triplet exciton is generated at time, t<500 ps. However the ultrafast triplet generation is missing in DOO-PPV solution, indicating that the HE-SF is predominantly interchain in nature. The HE-SF process was confirmed by the triplet MPA(B) response for excitation at E>2ET, which shows a typical SF response. Our work shows that the SF process in π-conjugated polymers is a much more general process than thought previously.

  4. Acoustically induced stark effect for excitons in intrinsic semiconductors.

    PubMed

    Ivanov, A L; Littlewood, P B

    2001-09-24

    A Stark effect for excitons parametrically driven by coherent acoustic phonons is proposed. Our scheme refers to a low-temperature intrinsic semiconductor or semiconductor nanostructure pumped by an acoustic wave (frequency band nu(ac) approximately equal to 1-40 GHz and intensity range I(ac) approximately equal to 10(-2)-10(2) W/cm(2)) and probed by low-intensity light. Tunable optical band gaps, which strongly change the spectral shape of the exciton line, are induced in the polariton spectrum by acoustic pumping. We develop an exactly solvable model of the acoustic Stark effect and apply our results to GaAs driven by bulk or surface acoustic waves. PMID:11580613

  5. Optical studies of magnons, excitons and polarons in CuO{sub 2}-layer compounds

    SciTech Connect

    Kastner, M.A.; Birgeneau, R.J.

    1996-12-31

    The optical properties of undoped and lightly doped lamellar copper oxides are reviewed. In the undoped materials the absorption below the charge-transfer gap is dominated by magnetic and crystal field excitations of the CuO{sub 2} layers. The temperature dependence of the charge-transfer absorption provides evidence that free charged excitations form large polarons. However, the optical ionization energy of holes bound to acceptors is much larger than the thermal ionization energy, indicating that the bound polarons are small. The parameters extracted from optical measurements predict the Hall mobility of holes in lightly doped La{sub 2}CuO{sub 4}, with no adjustable parameters, confirming that the carriers are polarons.

  6. Revealing the Exciton Fine Structure of PbSe Nanocrystal Quantum Dots Using Optical Spectroscopy in High Magnetic Fields

    SciTech Connect

    Schaller, Richard D.; Crooker, Scott A.; Bussian, David A.; Pietryga, Jeffrey M.; Joo, Jin; Klimov, Victor I.

    2010-08-04

    We measure the photoluminescence lifetime τ of excitons in colloidal PbSe nanocrystals (NCs) at low temperatures to 270 mK and in high magnetic fields to 15 T. For all NCs, τ increases sharply below 10 K but saturates by 500 mK. In contrast to the usual picture of well-separated “bright” and “dark” exciton states (found, e.g., in CdSe NCs), these dynamics fit remarkably well to a system having two exciton states with comparable—but small—oscillator strengths that are separated by only 300–900 μeV depending on NC size. Importantly, magnetic fields reduce τ below 10 K, consistent with field-induced mixing between the two states. Magnetic-circular dichroism studies reveal exciton g factors from 2–5, and magnetophotoluminescence shows >10% circularly polarized emission.

  7. Coherent Exciton Dynamics in Atomically Thin Semiconductors

    NASA Astrophysics Data System (ADS)

    Li, Xiaoqin (Elaine)

    The near band-edge optical response of an emerging class of semiconductors, known as the transitional metal dichalcogenides (TMDs), is dominated by tightly-bound excitons and charged excitons (i.e. trions). A fundamental property of these quasiparticles (excitons and trions) is quantum decoherence time, which reflects irreversible quantum dissipation arising from system (excitons and trions) and bath (vacuum and other quasiparticles) interactions and determines the timescale during which excitons can be coherently manipulated. Dephasing time is also equivalent to the intrinsic homogeneous linewidth of exciton resonance. In addition, excitons in TMDs are localized at the corners of the Brillouin zone and provide a convenient way to optical manipulate the valley degree of freedom, which may act as a useful information carrier analogous to electronic charge or spin. Direct measurement of valley coherence time is challenging because it corresponds to a non-radiative coherence between two degenerate states. Using ultrafast multi-dimensional optical spectroscopy, we investigate the intrinsic homogeneous linewidth of excitons, exciton valley coherence as well as coupling between excitons and trions. Our studies reveal coherent electronic dynamics on the order of ~100 fs in monolayer TMDs. We gratefully acknowledge financial support from NSF, AFOSR, and the Welch Foundation.

  8. Cross-polarized excitons in carbon nanotubes.

    PubMed

    Kilina, Svetlana; Tretiak, Sergei; Doorn, Stephen K; Luo, Zhengtang; Papadimitrakopoulos, Fotios; Piryatinski, Andrei; Saxena, Avadh; Bishop, Alan R

    2008-05-13

    Polarization of low-lying excitonic bands in finite-size semiconducting single-walled carbon nanotubes (SWNTs) is studied by using quantum-chemical methodologies. Our calculations elucidate properties of cross-polarized excitons, which lead to the transverse optical absorption of nanotubes and presumably couple to intermediate-frequency modes recently observed in resonance Raman excitation spectroscopy. We identify up to 12 distinct excitonic transitions below the second fundamental band associated with the E(22) van Hove singularity. Calculations for several chiral SWNTs distinguish the optically active "bright" excitonic band polarized parallel to the tube axis and several optically "weak" cross-polarized excitons. The rest are optically (near) forbidden "dark" transitions. An analysis of the transition density matrices related to excitonic bands provides detailed information about delocalization of excitonic wavefunction along the tube. Utilization of the natural helical coordinate system accounting for the tube chirality allows one to disentangle longitudinal and circumferential components. The distribution of the transition density matrix along a tube axis is similar for all excitons. However, four parallel-polarized excitons associated with the E(11) transition are more localized along the circumference of a tube, compared with others related to the E(12) and E(21) cross-polarized transitions. Calculated splitting between optically active parallel- and cross-polarized transitions increases with tube diameter, which compares well with experimental spectroscopic data. PMID:18463293

  9. Cross-polarized excitons in carbon nanotubes

    PubMed Central

    Kilina, Svetlana; Tretiak, Sergei; Doorn, Stephen K.; Luo, Zhengtang; Papadimitrakopoulos, Fotios; Piryatinski, Andrei; Saxena, Avadh; Bishop, Alan R.

    2008-01-01

    Polarization of low-lying excitonic bands in finite-size semiconducting single-walled carbon nanotubes (SWNTs) is studied by using quantum-chemical methodologies. Our calculations elucidate properties of cross-polarized excitons, which lead to the transverse optical absorption of nanotubes and presumably couple to intermediate-frequency modes recently observed in resonance Raman excitation spectroscopy. We identify up to 12 distinct excitonic transitions below the second fundamental band associated with the E22 van Hove singularity. Calculations for several chiral SWNTs distinguish the optically active “bright” excitonic band polarized parallel to the tube axis and several optically “weak” cross-polarized excitons. The rest are optically (near) forbidden “dark” transitions. An analysis of the transition density matrices related to excitonic bands provides detailed information about delocalization of excitonic wavefunction along the tube. Utilization of the natural helical coordinate system accounting for the tube chirality allows one to disentangle longitudinal and circumferential components. The distribution of the transition density matrix along a tube axis is similar for all excitons. However, four parallel-polarized excitons associated with the E11 transition are more localized along the circumference of a tube, compared with others related to the E12 and E21 cross-polarized transitions. Calculated splitting between optically active parallel- and cross-polarized transitions increases with tube diameter, which compares well with experimental spectroscopic data. PMID:18463293

  10. Optical Frequency Domain Visualization of Electron Beam Driven Plasma Wakefields

    NASA Astrophysics Data System (ADS)

    Zgadzaj, Rafal; Downer, M. C.; Muggli, Patric; Yakimenko, Vitaly; Babzien, Marcus; Kusche, Karl; Fedurin, Mikhail

    2010-11-01

    Beam-driven plasma wakefield accelerators (PWFA), such as the ``plasma afterburner,'' are a promising approach for significantly increasing the particle energies of conventional accelerators. The study and optimization of PWFA would benefit from an experimental correlation between the parameters of the drive bunch, the accelerated bunch and the corresponding, accelerating plasma wave structure. However, the plasma wave structure has not yet been observed directly in PWFA. We will report our current work on noninvasive optical Frequency Domain Interferometric (FDI) and Holographic (FDH) visualization of beam-driven plasma waves. Both techniques employ two laser pulses (probe and reference) co-propagating with the particle drive-beam and its plasma wake. The reference pulse precedes the drive bunch, while the probe overlaps the plasma wave and maps its longitudinal and transverse structure. The experiment is being developed at the BNL/ATF Linac to visualize wakes generated by two and multi-bunch drive beams.

  11. The dynamics of radiation-driven, optically thick winds

    NASA Astrophysics Data System (ADS)

    Shen, Rong-Feng; Nakar, Ehud; Piran, Tsvi

    2016-06-01

    Recent observation of some luminous transient sources with low colour temperatures suggests that the emission is dominated by optically thick winds driven by super-Eddington accretion. We present a general analytical theory of the dynamics of radiation pressure-driven, optically thick winds. Unlike the classical adiabatic stellar wind solution whose dynamics are solely determined by the sonic radius, here the loss of the radiation pressure due to photon diffusion also plays an important role. We identify two high mass-loss rate regimes (dot{M} > L_Edd/c^2). In the large total luminosity regime, the solution resembles an adiabatic wind solution. Both the radiative luminosity, L, and the kinetic luminosity, Lk, are super-Eddington with L < Lk and L ∝ L_k^{1/3}. In the lower total luminosity regime, most of the energy is carried out by the radiation with Lk < L ≈ LEdd. In a third, low mass-loss regime (dot{M} < L_Edd/c^2), the wind becomes optically thin early on and, unless gas pressure is important at this stage, the solution is very different from the adiabatic one. The results are independent from the energy generation mechanism at the foot of the wind; therefore, they are applicable to a wide range of mass ejection systems, from black hole accretion, to planetary nebulae, and to classical novae.

  12. Excitons at the (001) surface of anatase: Spatial behavior and optical signatures

    SciTech Connect

    Giorgi, Giacomo; Yamashita, Koichi; Palummo, Maurizia; Chiodo, Letizia

    2011-08-15

    Within an ab initio study, based on the application of Many-Body Perturbation Theory approaches on top of ground-state Density Functional Theory calculations, we study the optical behavior of the TiO{sub 2} anatase (001) surface. We focus on the (1 x 1) and the (1 x 4) reconstructions, both experimentally observed, which reveal a different optical response and an anisotropy, in the (001) plane, not present in the bulk phase. The determination of the spatial behavior of the electron-hole photoexcited couple provides a possible explanation of the observed enhanced photocatalytic activity of TiO{sub 2} anatase nanostructures with a high percentage of (001)-(1 x 1) exposed facets.

  13. Floquet engineering with quasienergy bands of periodically driven optical lattices

    NASA Astrophysics Data System (ADS)

    Holthaus, Martin

    2016-01-01

    A primer on the Floquet theory of periodically time-dependent quantum systems is provided, and it is shown how to apply this framework for computing the quasienergy band structure governing the dynamics of ultracold atoms in driven optical cosine lattices. Such systems are viewed here as spatially and temporally periodic structures living in an extended Hilbert space, giving rise to spatio-temporal Bloch waves whose dispersion relations can be manipulated at will by exploiting ac-Stark shifts and multiphoton resonances. The elements required for numerical calculations are introduced in a tutorial manner, and some example calculations are discussed in detail, thereby illustrating future prospects of Floquet engineering.

  14. Suppression of quantum decoherence via infrared-driven coherent exciton-plasmon coupling: Undamped field and Rabi oscillations

    SciTech Connect

    Sadeghi, S. M.; Patty, K. D.

    2014-02-24

    We show that when a semiconductor quantum dot is in the vicinity of a metallic nanoparticle and driven by a mid-infrared laser field, its coherent dynamics caused by interaction with a visible laser field can become free of quantum decoherence. We demonstrate that this process, which can offer undamped Rabi and field oscillations, is the result of coherent normalization of the “effective” polarization dephasing time of the quantum dot (T{sub 2}{sup *}). This process indicates formation of infrared-induced coherently forced oscillations, which allows us to control the value of T{sub 2}{sup *} using the infrared laser. The results offer decay-free ultrafast modulation of the effective field experienced by the quantum dot when neither the visible laser field nor the infrared laser changes with time.

  15. Exciton size and quantum transport in nanoplatelets

    SciTech Connect

    Pelzer, Kenley M. Gray, Stephen K.; Darling, Seth B.; Schaller, Richard D.

    2015-12-14

    Two-dimensional nanoplatelets (NPLs) are an exciting class of materials with promising optical and energy transport properties. The possibility of efficient energy transport between nanoplatelets raises questions regarding the nature of energy transfer in these thin, laterally extended systems. A challenge in understanding exciton transport is the uncertainty regarding the size of the exciton. Depending on the material and defects in the nanoplatelet, an exciton could plausibly extend over an entire plate or localize to a small region. The variation in possible exciton sizes raises the question how exciton size impacts the efficiency of transport between nanoplatelet structures. Here, we explore this issue using a quantum master equation approach. This method goes beyond the assumptions of Förster theory to allow for quantum mechanical effects that could increase energy transfer efficiency. The model is extremely flexible in describing different systems, allowing us to test the effect of varying the spatial extent of the exciton. We first discuss qualitative aspects of the relationship between exciton size and transport and then conduct simulations of exciton transport between NPLs for a range of exciton sizes and environmental conditions. Our results reveal that exciton size has a strong effect on energy transfer efficiency and suggest that manipulation of exciton size may be useful in designing NPLs for energy transport.

  16. Exciton size and quantum transport in nanoplatelets.

    PubMed

    Pelzer, Kenley M; Darling, Seth B; Gray, Stephen K; Schaller, Richard D

    2015-12-14

    Two-dimensional nanoplatelets (NPLs) are an exciting class of materials with promising optical and energy transport properties. The possibility of efficient energy transport between nanoplatelets raises questions regarding the nature of energy transfer in these thin, laterally extended systems. A challenge in understanding exciton transport is the uncertainty regarding the size of the exciton. Depending on the material and defects in the nanoplatelet, an exciton could plausibly extend over an entire plate or localize to a small region. The variation in possible exciton sizes raises the question how exciton size impacts the efficiency of transport between nanoplatelet structures. Here, we explore this issue using a quantum master equation approach. This method goes beyond the assumptions of Förster theory to allow for quantum mechanical effects that could increase energy transfer efficiency. The model is extremely flexible in describing different systems, allowing us to test the effect of varying the spatial extent of the exciton. We first discuss qualitative aspects of the relationship between exciton size and transport and then conduct simulations of exciton transport between NPLs for a range of exciton sizes and environmental conditions. Our results reveal that exciton size has a strong effect on energy transfer efficiency and suggest that manipulation of exciton size may be useful in designing NPLs for energy transport. PMID:26671357

  17. Exciton size and quantum transport in nanoplatelets

    NASA Astrophysics Data System (ADS)

    Pelzer, Kenley M.; Darling, Seth B.; Gray, Stephen K.; Schaller, Richard D.

    2015-12-01

    Two-dimensional nanoplatelets (NPLs) are an exciting class of materials with promising optical and energy transport properties. The possibility of efficient energy transport between nanoplatelets raises questions regarding the nature of energy transfer in these thin, laterally extended systems. A challenge in understanding exciton transport is the uncertainty regarding the size of the exciton. Depending on the material and defects in the nanoplatelet, an exciton could plausibly extend over an entire plate or localize to a small region. The variation in possible exciton sizes raises the question how exciton size impacts the efficiency of transport between nanoplatelet structures. Here, we explore this issue using a quantum master equation approach. This method goes beyond the assumptions of Förster theory to allow for quantum mechanical effects that could increase energy transfer efficiency. The model is extremely flexible in describing different systems, allowing us to test the effect of varying the spatial extent of the exciton. We first discuss qualitative aspects of the relationship between exciton size and transport and then conduct simulations of exciton transport between NPLs for a range of exciton sizes and environmental conditions. Our results reveal that exciton size has a strong effect on energy transfer efficiency and suggest that manipulation of exciton size may be useful in designing NPLs for energy transport.

  18. Theoretical Investigation Optical Properties of Si12C12 Clusters and Oligomers having Potential as Excitonic Materials

    NASA Astrophysics Data System (ADS)

    Duan, Xiaofeng; Burggraf, Larry

    2015-03-01

    SiC clusters may have potential in 2-D exciton circuits. We determined the most stable SinCn isomer structures (n <=12) out of hundreds to thousands isomers using a method combining Stochastic Potential Surface Search and Pseududopotential Plane-Wave Density Functional Theory Car-Parinello Molecular Dynamics simulated annealing (PSPW-CPMD-SA). Four low-energy Si12C12 isomer structures are discussed to illustrate the varying optical properties of clusters with structures: i) cage type with C- and Si- segregations, ii) symmetric type formed having π-stacked C aromatic rings and exterior Si regions, iii) nearly planar bowl with C fullerene fragment surrounded by Si atoms, and iv) symmetrical SiC cluster having alternate SiC bonding in the structure. We employed B3LYP and PBE0 functionals and both cc-pVTZ and aug-cc-pVTZ basis sets to perform TDDFT calculations of excitation energies and photo-absorption spectra to show how structure and bonding patterns affect photo excitations in different types of SiC clusters. The electron and the hole charge distribution patterns in excitation were calculated for major photoabsorption transitions, reported for the most stable isomer, closo Si12C12. To understand electric field effects we also calculated dynamical polarizabilities for all the four structures using Coupled Perturbed Hartree-Fock (CPHF) at B3LYP/aug-cc-pVTZ and PBE0/aug-cc-pVTZ level of theory. We gratefully acknowledge support from the Air Force Office of Scientific Research in a program managed by Dr Michael Berman.

  19. Properties of Type-II ZnTe/ZnSe Submonolayer Quantum Dots Studied via Excitonic Aharonov- Bohm Effect and Polarized Optical Spectroscopy

    NASA Astrophysics Data System (ADS)

    Ji, Haojie

    In this thesis I develop understanding of the fundamental physical and material properties of type-II ZnTe/ZnSe submonolayer quantum dots (QDs), grown via combination of molecular beam epitaxy (MBE) and migration enhanced epitaxy (MEE). I use magneto-photoluminescence, including excitonic Aharonov-Bohm (AB) effect and polarized optical spectroscopy as the primary tools in this work. I present previous studies as well as the background of optical and magneto-optical processes in semiconductor nanostructures and introduce the experimental methods in Chapters 1 - 3. In Chapter 4 I focus on the excitonic AB effect in the type-II QDs. I develop a lateral tightly-bound exciton model for ZnTe/ZnSe type-II QDs, using analytical methods and numerical calculations. This explained the magneto-PL observation and allowed for establishing the size and density of the QDs in each sample based on the results of PL and magneto-PL measurements. For samples with larger QDs, I observe behaviors that fall between properties of quantum-dot and quantum-well-like systems due to increased QD densities and their type-II nature. Finally, the decoherence mechanisms of the AB excitons are investigated via the temperature dependent studies of the magneto-PL. It is determined that the AB exciton decoherence is due to transport-like (acoustic phonon) scattering of the electrons moving in the ZnSe barriers, but with substantially smaller magnitude of electron-phonon coupling constant due to relatively strong electron-hole coupling within these type-II QDs. In Chapter 5 I discuss the results of circularly polarized magneto-PL measurements. A model with ultra-long spin-flip time of holes confined to submonolayer QDs is proposed. The g-factor of type-II excitons was extracted from the Zeeman splitting and the g-factor of electrons was obtained by fitting the temperature dependence of the degree of circular polarization (DCP), from which g-factor of holes confined within ZnTe QDs was found. It is shown

  20. Comparison of magneto-optical properties of various excitonic complexes in CdTe and CdSe self-assembled quantum dots.

    PubMed

    Kobak, J; Smoleński, T; Goryca, M; Rousset, J-G; Pacuski, W; Bogucki, A; Oreszczuk, K; Kossacki, P; Nawrocki, M; Golnik, A; Płachta, J; Wojnar, P; Kruse, C; Hommel, D; Potemski, M; Kazimierczuk, T

    2016-07-01

    We present a comparative study of two self-assembled quantum dot (QD) systems based on II-VI compounds: CdTe/ZnTe and CdSe/ZnSe. Using magneto-optical techniques we investigated a large population of individual QDs. The systematic photoluminescence studies of emission lines related to the recombination of neutral exciton X, biexciton XX, and singly charged excitons (X(+), X(-)) allowed us to determine average parameters describing CdTe QDs (CdSe QDs): X-XX transition energy difference 12 meV (24 meV); fine-structure splitting δ1=0.14 meV (δ1=0.47 meV); g-factor g  =  2.12 (g  =  1.71); diamagnetic shift γ=2.5 μeV T(-2) (γ =1.3 μeV T(-2)). We find also statistically significant correlations between various parameters describing internal structure of excitonic complexes. PMID:27173643

  1. Comparison of magneto-optical properties of various excitonic complexes in CdTe and CdSe self-assembled quantum dots

    NASA Astrophysics Data System (ADS)

    Kobak, J.; Smoleński, T.; Goryca, M.; Rousset, J.-G.; Pacuski, W.; Bogucki, A.; Oreszczuk, K.; Kossacki, P.; Nawrocki, M.; Golnik, A.; Płachta, J.; Wojnar, P.; Kruse, C.; Hommel, D.; Potemski, M.; Kazimierczuk, T.

    2016-07-01

    We present a comparative study of two self-assembled quantum dot (QD) systems based on II–VI compounds: CdTe/ZnTe and CdSe/ZnSe. Using magneto-optical techniques we investigated a large population of individual QDs. The systematic photoluminescence studies of emission lines related to the recombination of neutral exciton X, biexciton XX, and singly charged excitons (X+, X‑) allowed us to determine average parameters describing CdTe QDs (CdSe QDs): X–XX transition energy difference 12 meV (24 meV); fine-structure splitting δ1=0.14 meV (δ1=0.47 meV); g-factor g  =  2.12 (g  =  1.71) diamagnetic shift γ=2.5 μeV T‑2 (γ =1.3 μeV T‑2). We find also statistically significant correlations between various parameters describing internal structure of excitonic complexes.

  2. Monolayer excitonic laser

    NASA Astrophysics Data System (ADS)

    Ye, Yu; Wong, Zi Jing; Lu, Xiufang; Ni, Xingjie; Zhu, Hanyu; Chen, Xianhui; Wang, Yuan; Zhang, Xiang

    2015-11-01

    Two-dimensional van der Waals materials have opened a new paradigm for fundamental physics exploration and device applications because of their emerging physical properties. Unlike gapless graphene, monolayer transition-metal dichalcogenides (TMDCs) are two-dimensional semiconductors that undergo an indirect-to-direct bandgap transition, creating new optical functionalities for next-generation ultra-compact photonics and optoelectronics. Although the enhancement of spontaneous emission has been reported on TMDC monolayers integrated with photonic crystals and distributed Bragg reflector microcavities, coherent light emission from a TMDC monolayer has not been demonstrated. Here, we report the realization of a two-dimensional excitonic laser by embedding monolayer WS2 in a microdisk resonator. Using a whispering gallery mode with a high quality factor and optical confinement, we observe bright excitonic lasing at visible wavelengths. This demonstration of a two-dimensional excitonic laser marks a major step towards two-dimensional on-chip optoelectronics for high-performance optical communication and computing applications.

  3. All optical controlled-NOT gate based on an exciton-polariton circuit

    NASA Astrophysics Data System (ADS)

    Solnyshkov, D. D.; Bleu, O.; Malpuech, G.

    2015-07-01

    We propose an implementation of a CNOT gate for quantum computing based on a patterned microcavity polariton system, which can be manufactured using the modern technological facilities. The qubits are encoded in the spin-coherent polariton states. The structure consists of two wire cavities oriented at 45° with a micropillar between them. The polariton spin rotates due to the Longitudinal-Transverse splitting between polarization eigenstates in the wires. In the pillar, the optically generated circularly polarized polariton macrooccupied state plays the role of the control qubit. Because of the spin-anisotropic polariton interaction, it induces an effective magnetic field along the Z-direction with a sign depending on the qubit value.

  4. Exciton Binding Energy of Monolayer WS2

    PubMed Central

    Zhu, Bairen; Chen, Xi; Cui, Xiaodong

    2015-01-01

    The optical properties of monolayer transition metal dichalcogenides (TMDC) feature prominent excitonic natures. Here we report an experimental approach to measuring the exciton binding energy of monolayer WS2 with linear differential transmission spectroscopy and two-photon photoluminescence excitation spectroscopy (TP-PLE). TP-PLE measurements show the exciton binding energy of 0.71 ± 0.01 eV around K valley in the Brillouin zone. PMID:25783023

  5. Optical Frequency Domain Visualization of Electron Beam Driven Plasma Wakefields

    NASA Astrophysics Data System (ADS)

    Zgadzaj, Rafal; Downer, Michael C.; Muggli, Patric; Yakimenko, Vitaly; Kusche, Karl; Fedurin, Michhail; Babzien, Marcus

    2010-11-01

    Bunch driven plasma wakefield accelerators (PWFA), such as the "plasma afterburner," are a promising emerging method for significantly increasing the energy output of conventional particle accelerators [1]. The study and optimization of this method would benefit from an experimental correlation of the drive bunch parameters and the accelerated particle parameters with the corresponding plasma wave structure. However, the plasma wave structure has not been observed directly so far. We will report ongoing development of a noninvasive optical Frequency Domain Interferometric (FDI) [2] and Holographic (FDH) [3] diagnostics of bunch driven plasma wakes. Both FDI and FDH have been previously demonstrated in the case of laser driven wakes. These techniques employ two laser pulses co-propagating with the drive particle bunch and the trailing plasma wave. One pulse propagates ahead of the drive bunch and serves as a reference, while the second is overlapped with the plasma wave and probes its structure. The multi-shot FDI and single-shot FDH diagnostics permit direct noninvasive observation of longitudinal and transverse structure of the plasma wakes. The experiment is being developed at the 70 MeV Linac in the Accelerator Test Facility at Brookhaven National Laboratory to visualize wakes generated by two [4] and multi-bunch [5] drive beams.

  6. Optical Frequency Domain Visualization of Electron Beam Driven Plasma Wakefields

    SciTech Connect

    Zgadzaj, Rafal; Downer, Michael C.; Muggli, Patric; Yakimenko, Vitaly; Kusche, Karl; Fedurin, Michhail; Babzien, Marcus

    2010-11-04

    Bunch driven plasma wakefield accelerators (PWFA), such as the 'plasma afterburner', are a promising emerging method for significantly increasing the energy output of conventional particle accelerators. The study and optimization of this method would benefit from an experimental correlation of the drive bunch parameters and the accelerated particle parameters with the corresponding plasma wave structure. However, the plasma wave structure has not been observed directly so far. We will report ongoing development of a noninvasive optical Frequency Domain Interferometric (FDI) and Holographic (FDH) diagnostics of bunch driven plasma wakes. Both FDI and FDH have been previously demonstrated in the case of laser driven wakes. These techniques employ two laser pulses co-propagating with the drive particle bunch and the trailing plasma wave. One pulse propagates ahead of the drive bunch and serves as a reference, while the second is overlapped with the plasma wave and probes its structure. The multi-shot FDI and single-shot FDH diagnostics permit direct noninvasive observation of longitudinal and transverse structure of the plasma wakes. The experiment is being developed at the 70 MeV Linac in the Accelerator Test Facility at Brookhaven National Laboratory to visualize wakes generated by two and multi-bunch drive beams.

  7. Colloidal particles driven across periodic optical-potential-energy landscapes

    NASA Astrophysics Data System (ADS)

    Juniper, Michael P. N.; Straube, Arthur V.; Aarts, Dirk G. A. L.; Dullens, Roel P. A.

    2016-01-01

    We study the motion of colloidal particles driven by a constant force over a periodic optical potential energy landscape. First, the average particle velocity is found as a function of the driving velocity and the wavelength of the optical potential energy landscape. The relationship between average particle velocity and driving velocity is found to be well described by a theoretical model treating the landscape as sinusoidal, but only at small trap spacings. At larger trap spacings, a nonsinusoidal model for the landscape must be used. Subsequently, the critical velocity required for a particle to move across the landscape is determined as a function of the wavelength of the landscape. Finally, the velocity of a particle driven at a velocity far exceeding the critical driving velocity is examined. Both of these results are again well described by the two theoretical routes for small and large trap spacings, respectively. Brownian motion is found to have a significant effect on the critical driving velocity but a negligible effect when the driving velocity is high.

  8. Optical density of states in ultradilute GaAsN alloy: Coexistence of free excitons and impurity band of localized and delocalized states

    SciTech Connect

    Bhuyan, Sumi; Pal, Bipul; Bansal, Bhavtosh; Das, Sanat K.; Dhar, Sunanda

    2014-07-14

    Optically active states in liquid phase epitaxy-grown ultra-dilute GaAsN are studied. The feature-rich low temperature photoluminescence spectrum has contributions from excitonic band states of the GaAsN alloy, and two types of defect states—localized and extended. The degree of delocalization for extended states both within the conduction and defect bands, characterized by the electron temperature, is found to be similar. The degree of localization in the defect band is analyzed by the strength of the phonon replicas. Stronger emission from these localized states is attributed to their giant oscillator strength.

  9. Magneto-optical spectrum and the effective excitonic Zeeman splitting energies of Mn and Co-doped CdSe nanowires

    SciTech Connect

    Xiong, Wen; Chen, Wensuo

    2013-12-21

    The electronic structure of Mn and Co-doped CdSe nanowires are calculated based on the six-band k·p effective-mass theory. Through the calculation, it is found that the splitting energies of the degenerate hole states in Mn-doped CdSe nanowires are larger than that in Co-doped CdSe nanowires when the concentration of these two kinds of magnetic ions is the same. In order to analysis the magneto-optical spectrum of Mn and Co-doped CdSe nanowires, the four lowest electron states and the four highest hole states are sorted when the magnetic field is applied, and the 10 lowest optical transitions between the conduction subbands and the valence subbands at the Γ point in Mn and Co-doped CdSe nanowires are shown in the paper, it is found that the order of the optical transitions at the Γ point almost do not change although two different kinds of magnetic ions are doped in CdSe nanowires. Finally, the effective excitonic Zeeman splitting energies at the Γ point are found to increase almost linearly with the increase of the concentration of the magnetic ions and the magnetic field; meanwhile, the giant positive effective excitonic g factors in Mn and Co-doped CdSe nanowires are predicted based on our theoretical calculation.

  10. Spatially indirect excitons in coupled quantum wells

    SciTech Connect

    Lai, Chih-Wei Eddy

    2004-03-01

    observed. The spatial and energy distributions of optically active excitons were used as thermodynamic quantities to construct a phase diagram of the exciton system, demonstrating the existence of distinct phases. Optical and electrical properties of the CQW sample were examined thoroughly to provide deeper understanding of the formation mechanisms of these cold exciton systems. These insights offer new strategies for producing cold exciton systems, which may lead to opportunities for the realization of BEC in solid-state systems.

  11. Contrastive analysis of multiple exciton generation theories

    NASA Astrophysics Data System (ADS)

    Tan, Hengyu; Chang, Qing

    2015-10-01

    Multiple exciton generation (MEG) is an effect that semiconductor nanocrystals (NCs) quantum dots (QDs) generate multiple excitons (electron-hole pairs) through absorbing a single high energy photon. It can translate the excess photon energy of bandgap (Eg) into new excitons instead of heat loss and improve the photovoltaic performance of solar cells. However, the theories of MEG are not uniform. The main MEG theories can be divided into three types. The first is impact ionization. It explains MEG through a conventional way that a photogenerated exciton becomes multiple excitons by Coulomb interactions between carriers. The Second is coherent superposition of excitonic states. Multiple excitons are generated by the coherent superposition of single photogenerated exciton state with enough excess momentum and the two-exciton state with the same momentum. The third is excitation via virtual excitonic states. The nanocrystals vacuum generates a virtual biexciton by coulomb coupling between two valence band electrons. The virtual biexciton absorbing a photon with an intraband optical transition is converted into a real biexciton. This paper describes the MEG influence on solar photoelectric conversion efficiency, concludes and analyzes the fundamentals of different MEG theories, the MEG experimental measure, their merits and demerits, calculation methods of generation efficiency.

  12. Exciton spin dynamics in GaSe

    SciTech Connect

    Tang, Yanhao; Xie, Wei; McGuire, John A. Lai, Chih Wei; Mandal, Krishna C.

    2015-09-21

    We analyze exciton spin dynamics in GaSe under nonresonant circularly polarized optical pumping with an exciton spin-flip rate-equation model. The model reproduces polarized time-dependent photoluminescence measurements in which the initial circular polarization approaches unity even when pumping with 0.15 eV excess energy. At T = 10 K, the exciton spin relaxation exhibits a biexponential decay with sub-20 ps and >500 ps time constants, which are also reproduced by the rate-equation model assuming distinct spin-relaxation rates for hot (nonequilibrium) and cold band-edge excitons.

  13. Optically driven Archimedes micro-screws for micropump application.

    PubMed

    Lin, Chih-Lang; Vitrant, Guy; Bouriau, Michel; Casalegno, Roger; Baldeck, Patrice L

    2011-04-25

    Archimedes micro-screws have been fabricated by three-dimensional two-photon polymerization using a Nd:YAG Q-switched microchip laser at 532nm. Due to their small sizes they can be easily manipulated, and made to rotate using low power optical tweezers. Rotation rates up to 40 Hz are obtained with a laser power of 200 mW, i.e. 0.2 Hz/mW. A photo-driven micropump action in a microfluidic channel is demonstrated with a non-optimized flow rate of 6 pL/min. The optofluidic properties of such type of Archimedes micro-screws are quantitatively described by the conservation of momentum that occurs when the laser photons are reflected on the helical micro-screw surface. PMID:21643076

  14. Intrinsic optical bistability in a strongly driven Rydberg ensemble

    NASA Astrophysics Data System (ADS)

    de Melo, Natalia R.; Wade, Christopher G.; Šibalić, Nikola; Kondo, Jorge M.; Adams, Charles S.; Weatherill, Kevin J.

    2016-06-01

    We observe and characterize intrinsic optical bistability in a dilute Rydberg vapor. The bistability is characterized by sharp jumps between states of low and high Rydberg occupancy with jump-up and -down positions displaying hysteresis depending on the direction in which the control parameter is changed. We find that the shift in frequency of the jump point scales with the fourth power of the principal quantum number. Also, the width of the hysteresis window increases with increasing principal quantum number, before reaching a peak and then closing again. The experimental results are consistent with predictions from a simple theoretical model based on semiclassical Maxwell-Bloch equations including the effects of interaction-induced broadening and level shifts. These results provide insight into the dynamics of driven dissipative systems.

  15. Laser-driven Sisyphus cooling in an optical dipole trap

    SciTech Connect

    Ivanov, Vladyslav V.; Gupta, Subhadeep

    2011-12-15

    We propose a laser-driven Sisyphus-cooling scheme for atoms confined in a far-off resonance optical dipole trap. Utilizing the differential trap-induced ac Stark shift, two electronic levels of the atom are resonantly coupled by a cooling laser preferentially near the trap bottom. After absorption of a cooling photon, the atom loses energy by climbing the steeper potential, and then spontaneously decays preferentially away from the trap bottom. The proposed method is particularly suited to cooling alkaline-earth-metal-like atoms where two-level systems with narrow electronic transitions are present. Numerical simulations for the cases of {sup 88}Sr and {sup 174}Yb demonstrate the expected recoil and Doppler temperature limits. The method requires a relatively small number of scattered photons and can potentially lead to phase-space densities approaching quantum degeneracy in subsecond time scales.

  16. Laser-driven Sisyphus cooling in an optical dipole trap

    NASA Astrophysics Data System (ADS)

    Ivanov, Vladyslav V.; Gupta, Subhadeep

    2011-12-01

    We propose a laser-driven Sisyphus-cooling scheme for atoms confined in a far-off resonance optical dipole trap. Utilizing the differential trap-induced ac Stark shift, two electronic levels of the atom are resonantly coupled by a cooling laser preferentially near the trap bottom. After absorption of a cooling photon, the atom loses energy by climbing the steeper potential, and then spontaneously decays preferentially away from the trap bottom. The proposed method is particularly suited to cooling alkaline-earth-metal-like atoms where two-level systems with narrow electronic transitions are present. Numerical simulations for the cases of 88Sr and 174Yb demonstrate the expected recoil and Doppler temperature limits. The method requires a relatively small number of scattered photons and can potentially lead to phase-space densities approaching quantum degeneracy in subsecond time scales.

  17. Optically driven resonance of nanoscale flexural oscillators in liquid.

    PubMed

    Verbridge, Scott S; Bellan, Leon M; Parpia, Jeevak M; Craighead, H G

    2006-09-01

    We demonstrate the operation of radio frequency nanoscale flexural resonators in air and liquid. Doubly clamped string, as well as singly clamped cantilever resonators, with nanoscale cross-sectional dimensions and resonant frequencies as high as 145 MHz are driven in air as well as liquid with an amplitude modulated laser. We show that this laser drive technique can impart sufficient energy to a nanoscale resonator to overcome the strong viscous damping present in these media, resulting in a mechanical resonance that can be measured by optical interference techniques. Resonance in air, isopropyl alcohol, acetone, water, and phosphate-buffered saline is demonstrated for devices having cross-sectional dimensions close to 100 nm. For operation in air, quality factors as high as 400 at 145 MHz are demonstrated. In liquid, quality factors ranging from 3 to 10 and frequencies ranging from 20 to 100 MHz are observed. These devices, and an all-optical actuation and detection system, may provide insight into the physics of the interaction of nanoscale mechanical structures with their environments, greatly extending the viscosity range over which such small flexural resonant devices can be operated. PMID:16968035

  18. Plasmonic, excitonic and exciton-plasmonic photoinduced nanocomposites

    NASA Astrophysics Data System (ADS)

    Bityurin, N.; Ermolaev, N.; Smirnov, A. A.; Afanasiev, A.; Agareva, N.; Koryukina, T.; Bredikhin, V.; Kamensky, V.; Pikulin, A.; Sapogova, N.

    2016-03-01

    UV irradiation of materials consisting of a polymer matrix that possesses precursors of different kinds can result in creation of nanoparticles within the irradiated domains. Such photoinduced nanocomposites are promising for photonic applications due to the strong alteration of their optical properties compared to initial non-irradiated materials. We report our results on the synthesis and investigation of plasmonic, excitonic and exciton-plasmonic photoinduced nanocomposites. Plasmonic nanocomposites contain metal nanoparticles of noble metals with a pronounced plasmon resonance. Excitonic nanocomposites possess semiconductor nanoclusters (quantum dots). We consider the CdS-Au pair because the luminescent band of CdS nanoparticles enters the plasmon resonance band of gold nanoparticles. The obtaining of such particles within the same composite materials is promising for the creation of media with exciton-plasmon resonance. We demonstrate that it is possible to choose appropriate precursor species to obtain the initially transparent poly(methyl methacrylate) (PMMA) films containing both types of these molecules either separately or together. Proper irradiation of these materials by a light-emitting diode operating at the wavelength of 365 nm provides material alteration demonstrating light-induced optical absorption and photoluminescent properties typical for the corresponding nanoparticles. Thus, an exciton-plasmonic photoinduced nanocomposite is obtained. It is important that here we use the precursors that are different from those usually employed.

  19. Excitations, optical absorption spectra, and optical excitonic gaps of heterofullerenes: I. C60, C59N+ and C48N12

    SciTech Connect

    Xie, R; Bryant, G W; Sun, G; C.Nicklaus, M; Heringer, D; Frauenheim, T; Manaa, M R; Smith, Jr., V H; Araki, Y; Ito, O

    2003-10-02

    Low-energy excitations and optical absorption spectrum of C{sub 60} are computed by using time-dependent (TD) Hartree-Fock (HF), TD-density functional theory (TD-DFT), TD-DFT-based tight-binding (TD-DFT-TB) and a semiempirical ZINDO method. A detailed comparison of experiment and theory for the excitation energies, optical gap and absorption spectrum of C{sub 60} is presented. It is found that electron correlations and collective effects of exciton pairs play important roles in assigning accurately the spectral features of C{sub 60} and the TD-DFT method with non-hybrid functionals or a local spin density approximation leads to more accurate excitation energies than with hybrid functionals. The level of agreement between theory and experiment for C{sub 60} justifies similar calculations of the excitations and optical absorption spectrum of a monomeric azafullerene cation C{sub 59}N{sup +} exhibits distinguishing spectral features different from C{sub 60}: (1) the first singlet is dipole-allowed and the optical gap is redshifted by 1.44 eV; (2) several weaker absorption maxima occur in the visible region; (3) the transient triplet-triplet absorption at 1.60 eV (775 nm) is much broader and the decay of the triplet state is much faster. The calculated spectra of C{sub 59}N{sup +} characterize and explain well our measured ultraviolet-visible (UV-vis) and transient absorption spectra of the carborane anion salt [C{sub 59}N][Ag(CB{sub 11}H{sub 6}Cl{sub 6}){sub 2}]. For the most stable isomer of C{sub 48}N{sub 12}, we predict that the first singlet is dipole-allowed, the optical gap is redshifted by 1.22 eV relative to that of C{sub 60}, and optical absorption maxima occur at 585, 528, 443, 363, 340, 314 and 303 nm. We point out that the characterization of the UV-vis and transient absorption spectra of C{sub 48}N{sub 12} isomers is helpful in distinguishing the isomer structures required for applications in molecular electronics. For C{sub 59}N{sup +} and C{sub 48}N

  20. Plasmon and Exciton Coupling and Purcell Enhancement

    NASA Astrophysics Data System (ADS)

    Rice, Quinton; Rigo, Maria Veronica; Fudala, Rafal; Cho, Hyoyeong; Kim, Wan-Joong; Rich, Ryan; Tabibi, Bagher; Gryczynski, Zygmunt; Gryczynski, Ignacy; Yu, William; Seo, Jaetae

    2014-05-01

    The photoluminescence from plasmon-coupled exciton is of great interest for optoelectronic applications, because of the large quantum yield with localized field enhancement and reduced nonradiative transition. The Coulomb interaction through plasmon-exciton coupling results in the Purcell enhancement of quantum dots (QDs) in the vicinity of metal nanoparticles (MNPs). With plasmon-exciton coupling, the radiative and non-radiative decay rates and the coupling rates compete with each other. The coupling rate is closely related to the coupling distance between QDs and MNPs. The optimized coupling distance scales the re-excitation density of localized fields and the plasmon-exciton coupling rates. If the plasmon-exciton coupling rate is much faster than the radiative and non-radiative transitions of excitons, the re-excitations of excitons by the localized plasmonic field and the reduction of non-radiative transitions may occur. This presentation includes plasmon-exciton coupling dynamics, large enhancement and temporal properties of PL, and dipole-PL polarization fidelity of hybrid optical materials of plasmonic nanometals and excitonic semiconductor QDs. The work at Hampton University was supported by the National Science Foundation (NSF HRD-1137747), and Army Research Office (ARO W911NF-11-1-0177). The work at University of North Texas was supported by National Institutes of Health (NIH R01EB12003, and 5R21CA14897 (Z.G.)).

  1. Theory of core excitons

    SciTech Connect

    Dow, J. D.; Hjalmarson, H. P.; Sankey, O. F.; Allen, R. E.; Buettner, H.

    1980-01-01

    The observation of core excitons with binding energies much larger than those of the valence excitons in the same material has posed a long-standing theoretical problem. A proposed solution to this problem is presented, and Frenkel excitons and Wannier excitons are shown to coexist naturally in a single material. (GHT)

  2. Optical properties and exciton dynamics of alloyed core/shell/shell Cd(1-x)Zn(x)Se/ZnSe/ZnS quantum dots.

    PubMed

    Fitzmorris, Bob C; Pu, Ying-Chih; Cooper, Jason K; Lin, Yi-Fang; Hsu, Yung-Jung; Li, Yat; Zhang, Jin Z

    2013-04-24

    In this study we introduce a new method for the one-pot synthesis of core/shell/shell alloyed Cd1-xZnxSe/ZnSe/ZnS QDs and examine the effect of the shell coating on the optical properties and exciton dynamics of the alloy core. The photoluminescence (PL) quantum yield is greatly enhanced after shell growth, from 9.6% to 63%. The exciton dynamics were studied by time correlated single photon counting (TCSPC) and fit using integrated singular value decomposition global fitting (i-SVD-GF), which showed the biexponential observed lifetimes on the nanosecond time scale remain the same after shell growth. Using ultrafast transient absorption (TA) spectroscopy and SVD-GF, we have determined that surface passivation by ZnSe and ZnSe/ZnS shells reduces nonradiative recombination primarily on the picosecond time scale. These findings are helpful in directing the development of the next generation of QDs for biological labeling and other applications. PMID:23469824

  3. Attractive Coulomb interaction of two-dimensional Rydberg excitons

    NASA Astrophysics Data System (ADS)

    Shahnazaryan, V.; Shelykh, I. A.; Kyriienko, O.

    2016-06-01

    We analyze theoretically the Coulomb scattering processes of highly excited excitons in the direct-band-gap semiconductor quantum wells. We find that contrary to the interaction of ground-state excitons, the electron and hole exchange interaction between excited excitons has an attractive character both for s - and p -type two-dimensional (2D) excitons. Moreover, we show that similar to the three-dimensional highly excited excitons, the direct interaction of 2D Rydberg excitons exhibits van der Waals-type long-range interaction. The results predict the linear growth of the absolute value of exchange interaction strength with an exciton principal quantum number and point the way towards enhancement of optical nonlinearity in 2D excitonic systems.

  4. Entangled exciton states in quantum dot molecules

    NASA Astrophysics Data System (ADS)

    Bayer, Manfred

    2002-03-01

    Currently there is strong interest in quantum information processing(See, for example, The Physics of Quantum Information, eds. D. Bouwmeester, A. Ekert and A. Zeilinger (Springer, Berlin, 2000).) in a solid state environment. Many approaches mimic atomic physics concepts in which semiconductor quantum dots are implemented as artificial atoms. An essential building block of a quantum processor is a gate which entangles the states of two quantum bits. Recently a pair of vertically aligned quantum dots has been suggested as optically driven quantum gate(P. Hawrylak, S. Fafard, and Z. R. Wasilewski, Cond. Matter News 7, 16 (1999).)(M. Bayer, P. Hawrylak, K. Hinzer, S. Fafard, M. Korkusinski, Z.R. Wasilewski, O. Stern, and A. Forchel, Science 291, 451 (2001).): The quantum bits are individual carriers either on dot zero or dot one. The different dot indices play the same role as a "spin", therefore we call them "isospin". Quantum mechanical tunneling between the dots rotates the isospin and leads to superposition of these states. The quantum gate is built when two different particles, an electron and a hole, are created optically. The two particles form entangled isospin states. Here we present spectrocsopic studies of single self-assembled InAs/GaAs quantum dot molecules that support the feasibility of this proposal. The evolution of the excitonic recombination spectrum with varying separation between the dots allows us to demonstrate coherent tunneling of carriers across the separating barrier and the formation of entangled exciton states: Due to the coupling between the dots the exciton states show a splitting that increases with decreasing barrier width. For barrier widths below 5 nm it exceeds the thermal energy at room temperature. For a given barrier width, we find only small variations of the tunneling induced splitting demonstrating a good homogeneity within a molecule ensemble. The entanglement may be controlled by application of electromagnetic field. For

  5. Orientation of luminescent excitons in layered nanomaterials

    NASA Astrophysics Data System (ADS)

    Schuller, Jon A.; Karaveli, Sinan; Schiros, Theanne; He, Keliang; Yang, Shyuan; Kymissis, Ioannis; Shan, Jie; Zia, Rashid

    2013-04-01

    In nanomaterials, optical anisotropies reveal a fundamental relationship between structural and optical properties. Directional optical properties can be exploited to enhance the performance of optoelectronic devices, optomechanical actuators and metamaterials. In layered materials, optical anisotropies may result from in-plane and out-of-plane dipoles associated with intra- and interlayer excitations, respectively. Here, we resolve the orientation of luminescent excitons and isolate photoluminescence signatures arising from distinct intra- and interlayer optical transitions. Combining analytical calculations with energy- and momentum-resolved spectroscopy, we distinguish between in-plane and out-of-plane oriented excitons in materials with weak or strong interlayer coupling--MoS2 and 3,4,9,10-perylene tetracarboxylic dianhydride (PTCDA), respectively. We demonstrate that photoluminescence from MoS2 mono-, bi- and trilayers originates solely from in-plane excitons, whereas PTCDA supports distinct in-plane and out-of-plane exciton species with different spectra, dipole strengths and temporal dynamics. The insights provided by this work are important for understanding fundamental excitonic properties in nanomaterials and designing optical systems that efficiently excite and collect light from exciton species with different orientations.

  6. Orientation of luminescent excitons in layered nanomaterials.

    PubMed

    Schuller, Jon A; Karaveli, Sinan; Schiros, Theanne; He, Keliang; Yang, Shyuan; Kymissis, Ioannis; Shan, Jie; Zia, Rashid

    2013-04-01

    In nanomaterials, optical anisotropies reveal a fundamental relationship between structural and optical properties. Directional optical properties can be exploited to enhance the performance of optoelectronic devices, optomechanical actuators and metamaterials. In layered materials, optical anisotropies may result from in-plane and out-of-plane dipoles associated with intra- and interlayer excitations, respectively. Here, we resolve the orientation of luminescent excitons and isolate photoluminescence signatures arising from distinct intra- and interlayer optical transitions. Combining analytical calculations with energy- and momentum-resolved spectroscopy, we distinguish between in-plane and out-of-plane oriented excitons in materials with weak or strong interlayer coupling-MoS₂ and 3,4,9,10-perylene tetracarboxylic dianhydride (PTCDA), respectively. We demonstrate that photoluminescence from MoS₂ mono-, bi- and trilayers originates solely from in-plane excitons, whereas PTCDA supports distinct in-plane and out-of-plane exciton species with different spectra, dipole strengths and temporal dynamics. The insights provided by this work are important for understanding fundamental excitonic properties in nanomaterials and designing optical systems that efficiently excite and collect light from exciton species with different orientations. PMID:23455984

  7. A silicon-nanowire memory driven by optical gradient force induced bistability

    NASA Astrophysics Data System (ADS)

    Dong, B.; Cai, H.; Chin, L. K.; Huang, J. G.; Yang, Z. C.; Gu, Y. D.; Ng, G. I.; Ser, W.; Kwong, D. L.; Liu, A. Q.

    2015-12-01

    In this paper, a bistable optical-driven silicon-nanowire memory is demonstrated, which employs ring resonator to generate optical gradient force over a doubly clamped silicon-nanowire. Two stable deformation positions of a doubly clamped silicon-nanowire represent two memory states ("0" and "1") and can be set/reset by modulating the light intensity (<3 mW) based on the optical force induced bistability. The time response of the optical-driven memory is less than 250 ns. It has applications in the fields of all optical communication, quantum computing, and optomechanical circuits.

  8. A silicon-nanowire memory driven by optical gradient force induced bistability

    SciTech Connect

    Dong, B.; Cai, H. Gu, Y. D.; Kwong, D. L.; Chin, L. K.; Ng, G. I.; Ser, W.; Huang, J. G.; Yang, Z. C.; Liu, A. Q.

    2015-12-28

    In this paper, a bistable optical-driven silicon-nanowire memory is demonstrated, which employs ring resonator to generate optical gradient force over a doubly clamped silicon-nanowire. Two stable deformation positions of a doubly clamped silicon-nanowire represent two memory states (“0” and “1”) and can be set/reset by modulating the light intensity (<3 mW) based on the optical force induced bistability. The time response of the optical-driven memory is less than 250 ns. It has applications in the fields of all optical communication, quantum computing, and optomechanical circuits.

  9. Optical pump-terahertz probe analysis of long-lived d-electrons and relaxation to self-trapped exciton states in MnO

    NASA Astrophysics Data System (ADS)

    Nishitani, Junichi; Nagashima, Takeshi; Lippmaa, Mikk; Suemoto, Tohru

    2016-04-01

    The dynamics of photoexcited electrons in various excited d-states was investigated in a transition metal oxide MnO by tunable optical pump-terahertz probe measurements. Photoexcited electrons in the lowest excited d-state showed the longest relaxation time among the three excited d-states that are accessible in MnO at room temperature. The relaxation rate in the lowest excited d-state showed a drastic increase below the Neel temperature TN = 120 K in MnO. We conclude that this increase is caused by the appearance of a decay channel related to magnetic-excitation-assisted photoluminescence from self-trapped exciton (STE) states. The opening of relaxation channels to the STE states in an antiferromagnetic phase suggests that it may be possible to control photocarrier lifetime by magnetic order in transition metal oxides.

  10. Role of the Zhang-Rice-like exciton in optical absorption spectra of CuGeO3 and CuGe1-xSixO3 single crystals

    NASA Astrophysics Data System (ADS)

    Pagliara, S.; Parmigiani, F.; Galinetto, P.; Revcolevschi, A.; Samoggia, G.

    2002-07-01

    The optical excitations in pure and Si-substituted CuGeO3 are investigated in the 15-300 K temperature range. A structure, detected for the E field parallel to the c axis of the crystals at about 3.2 eV, is due to the formation of a Zhang-Rice-like (ZR) exciton. The weak oscillator strength is due to the low mobility of the ZR-like exciton between the edge-sharing CuO4 plaquettes of CuGeO3. The temperature dependence of the ZR-like energy is explained by a renormalization effect involving phonon-electron interactions or changes in spin ordering, while the increase of ZR-like exciton intensity with the Si content is argued to arise from a different hybridization of the Si-O bond with respect to Ge-O.

  11. Transmutation of skyrmions to half-solitons driven by the nonlinear optical spin Hall effect.

    PubMed

    Flayac, H; Solnyshkov, D D; Shelykh, I A; Malpuech, G

    2013-01-01

    We show that the spin domains, generated in the linear optical spin Hall effect by the analog of spin-orbit interaction for exciton polaritons, are associated with the formation of a Skyrmion lattice. In the nonlinear regime, the spin anisotropy of the polariton-polariton interactions results in a spatial compression of the domains and in a transmutation of the Skyrmions into oblique half-solitons. This phase transition is associated with both the focusing of the spin currents and the emergence of a strongly anisotropic emission pattern. PMID:23383815

  12. Bright and dark excitons in semiconductor carbon nanotubes

    SciTech Connect

    Tretiak, Sergei

    2008-01-01

    We report electronic structure calculations of finite-length semiconducting carbon nanotubes using the time dependent density functional theory (TD-DFT) and the time dependent Hartree Fock (TD-HF) approach coupled with semiempirical AM1 and ZINDO Hamiltonians. We specifically focus on the energy splitting, relative ordering, and localization properties of the optically active (bright) and optically forbidden (dark) states from the lowest excitonic band of the nanotubes. These excitonic states are very important in competing radiative and non-radiative processes in these systems. Our analysis of excitonic transition density matrices demonstrates that pure DFT functionals overdelocalize excitons making an electron-hole pair unbound; consequently, excitonic features are not presented in this method. In contrast, the pure HF and A111 calculations overbind excitons inaccurately predicting the lowest energy state as a bright exciton. Changing AM1 with ZINDO Hamiltonian in TD-HF calculations, predicts the bright exciton as the second state after the dark one. However, in contrast to AM1 calculations, the diameter dependence of the excitation energies obtained by ZINDO does not follow the experimental trends. Finally, the TD-DFT approach incorporating hybrid functions with a moderate portion of the long-range HF exchange, such as B3LYP, has the most generality and predictive capacity providing a sufficiently accurate description of excitonic structure in finite-size nanotubes. These methods characterize four important lower exciton bands. The lowest state is dark, the upper band is bright, and the two other dark and nearly degenerate excitons lie in-between. Although the calculated energy splittings between the lowest dark and the bright excitons are relatively large ({approx}0.1 eV), the dense excitonic manifold below the bright exciton allows for fast non-radiative relaxation leasing to the fast population of the lowest dark exciton. This rationalizes the low

  13. Simulation of Multi-Dimensional Signals in the Optical Domain: Quantum-Classical Feedback in Nonlinear Exciton Propagation.

    PubMed

    Richter, Martin; Fingerhut, Benjamin P

    2016-07-12

    We present an algorithm for the simulation of nonlinear 2D spectra of molecular systems in the UV-vis spectral region from atomistic molecular dynamics trajectories subject to nonadiabatic relaxation. We combine the nonlinear exciton propagation (NEP) protocol, that relies on a quasiparticle approach with the surface hopping methodology to account for quantum-classical feedback during the dynamics. Phenomena, such as dynamic Stokes shift due to nuclear relaxation, spectral diffusion, and population transfer among electronic states, are thus naturally included and benchmarked on a model of two electronic states coupled to a harmonic coordinate and a classical heatbath. The capabilities of the algorithm are further demonstrated for the bichromophore diphenylmethane that is described in a fully microscopic fashion including all 69 classical nuclear degrees of freedom. We demonstrate that simulated 2D signals are especially sensitive to the applied theoretical approximations (i.e., choice of active space in the CASSCF method) where population dynamics appears comparable. PMID:27248511

  14. Excitons in the Fractional Quantum Hall Effect

    DOE R&D Accomplishments Database

    Laughlin, R. B.

    1984-09-01

    Quasiparticles of charge 1/m in the Fractional Quantum Hall Effect form excitons, which are collective excitations physically similar to the transverse magnetoplasma oscillations of a Wigner crystal. A variational exciton wavefunction which shows explicitly that the magnetic length is effectively longer for quasiparticles than for electrons is proposed. This wavefunction is used to estimate the dispersion relation of these excitons and the matrix elements to generate them optically out of the ground state. These quantities are then used to describe a type of nonlinear conductivity which may occur in these systems when they are relatively clean.

  15. Nonlinear Exciton Dynamics in IndiumGalliumArsenic Quantum Wells

    NASA Astrophysics Data System (ADS)

    Zaks, Benjamin Rene

    Near infrared and optical light applied near the band edge of a semiconductor can lead to the formation of bound electron-hole pairs known as excitons. Using growth methods such as molecular beam epitaxy, semiconductor heterostructures can be engineered to have properties beneficial to particular experiments. The formation of thin layers of semiconductor can lead electrons and holes to be confined along a particular direction, and one structure that can be grown is called a quantum well. Confinement of charge in the quantum well increases the Coulomb interaction between the electron and hole, increasing exciton formation. When excitons are driven with an intense THz field, changes to the optical properties of the semiconductor are observed. These changes to the optical properties can not only provide interesting information about the exciton system, but also may provide insight on modulating optical beams at THz frequencies, information that may be necessary to further improve the speed of our cable and internet connections. By growing InGaAs quantum wells with AlGaAs barriers on a GaAs substrate, we have observed strong changes to the optical spectrum due to intense THz fields. We find that when the strong THz field is applied to an intersubband transition in the quantum well, the applied field can significantly shift the energy of that intersubband transition. This shift is unexpected within the approximations often used to describe this system, and we find that full numerical simulations of the system are necessary to interpret our results. When the strong THz field is polarized in the plane of the quantum well, we are able to observe optical light at up to 11 frequencies that were not present before application of the THz. The new frequencies are separated from the optical frequency by multiples of the THz frequency and are often referred to as sidebands. To understand the origin of the high-order sidebands observed, which are present up to 8 th order, a

  16. Exciton Resonances in Novel Silicon Carbide Polymers

    NASA Astrophysics Data System (ADS)

    Burggraf, Larry; Duan, Xiaofeng

    2015-05-01

    A revolutionary technology transformation from electronics to excitionics for faster signal processing and computing will be advantaged by coherent exciton transfer at room temperature. The key feature required of exciton components for this technology is efficient and coherent transfer of long-lived excitons. We report theoretical investigations of optical properties of SiC materials having potential for high-temperature excitonics. Using Car-Parinello simulated annealing and DFT we identified low-energy SiC molecular structures. The closo-Si12C12 isomer, the most stable 12-12 isomer below 1100 C, has potential to make self-assembled chains and 2-D nanostructures to construct exciton components. Using TDDFT, we calculated the optical properties of the isomer as well as oligomers and 2-D crystal formed from the isomer as the monomer unit. This molecule has large optical oscillator strength in the visible. Its high-energy and low-energy transitions (1.15 eV and 2.56 eV) are nearly pure one-electron silicon-to-carbon transitions, while an intermediate energy transition (1.28 eV) is a nearly pure carbon-to-silicon one-electron charge transfer. These results are useful to describe resonant, coherent transfer of dark excitons in the nanostructures. Research supported by the Air Force Office of Scientific Research.

  17. Nanotransformation and current fluctuations in exciton condensate junctions.

    PubMed

    Soller, H; Dolcini, F; Komnik, A

    2012-04-13

    We analyze the nonlinear transport properties of a bilayer exciton condensate that is contacted by four metallic leads by calculating the full counting statistics of electron transport for arbitrary system parameters. Despite its formal similarity to a superconductor the transport properties of the exciton condensate turn out to be completely different. We recover the generic features of exciton condensates such as counterpropagating currents driven by excitonic Andreev reflections and make predictions for nonlinear transconductance between the layers as well as for the current (cross)correlations and generalized Johnson-Nyquist relationships. Finally, we explore the possibility of connecting another mesoscopic system (in our case a quantum point contact) to the bottom layer of the exciton condensate and show how the excitonic Andreev reflections can be used for transforming voltage at the nanoscale. PMID:22587267

  18. Exciton radiative lifetime in transition metal dichalcogenide monolayers

    NASA Astrophysics Data System (ADS)

    Robert, C.; Lagarde, D.; Cadiz, F.; Wang, G.; Lassagne, B.; Amand, T.; Balocchi, A.; Renucci, P.; Tongay, S.; Urbaszek, B.; Marie, X.

    2016-05-01

    We have investigated the exciton dynamics in transition metal dichalcogenide monolayers using time-resolved photoluminescence experiments performed with optimized time resolution. For MoS e2 monolayer, we measure τrad0=1.8 ±0.2 ps at T =7 K that we interpret as the intrinsic radiative recombination time. Similar values are found for WS e2 monolayers. Our detailed analysis suggests the following scenario: at low temperature (T ≲50 K ), the exciton oscillator strength is so large that the entire light can be emitted before the time required for the establishment of a thermalized exciton distribution. For higher lattice temperatures, the photoluminescence dynamics is characterized by two regimes with very different characteristic times. First the photoluminescence intensity drops drastically with a decay time in the range of the picosecond driven by the escape of excitons from the radiative window due to exciton-phonon interactions. Following this first nonthermal regime, a thermalized exciton population is established gradually yielding longer photoluminescence decay times in the nanosecond range. Both the exciton effective radiative recombination and nonradiative recombination channels including exciton-exciton annihilation control the latter. Finally the temperature dependence of the measured exciton and trion dynamics indicates that the two populations are not in thermodynamical equilibrium.

  19. Micro-Ball-Lens Optical Switch Driven by SMA Actuator

    NASA Technical Reports Server (NTRS)

    Yang, Eui-Hyeok

    2003-01-01

    The figure is a simplified cross section of a microscopic optical switch that was partially developed at the time of reporting the information for this article. In a fully developed version, light would be coupled from an input optical fiber to one of two side-by-side output optical fibers. The optical connection between the input and the selected output fiber would be made via a microscopic ball lens. Switching of the optical connection from one output fiber to another would be effected by using a pair of thin-film shape-memory-alloy (SMA) actuators to toggle the lens between two resting switch positions. There are many optical switches some made of macroscopic parts by conventional fabrication techniques and some that are microfabricated and, hence, belong to the class of microelectromechanical systems (MEMS). Conventionally fabricated optical switches tend to be expensive. MEMS switches can be mass-produced at relatively low cost, but their attractiveness has been diminished by the fact that, heretofore, MEMS switches have usually been found to exhibit high insertion losses. The present switch is intended to serve as a prototype of low-loss MEMS switches. In addition, this is the first reported SMA-based optical switch. The optical fibers would be held in V grooves in a silicon frame. The lens would have a diameter of 1 m; it would be held by, and positioned between, the SMA actuators, which would be made of thin films of TiNi alloy. Although the SMA actuators are depicted here as having simple shapes for the sake of clarity of illustration, the real actuators would have complex, partly net-like shapes. With the exception of the lens and the optical fibers, the SMA actuators and other components of the switch would be made by microfabrication techniques. The components would be assembled into a sandwich structure to complete the fabrication of the switch. To effect switching, an electric current would be passed through one of the SMA actuators to heat it above

  20. Arbitrary GRIN component fabrication in optically driven diffusive photopolymers.

    PubMed

    Urness, Adam C; Anderson, Ken; Ye, Chungfang; Wilson, William L; McLeod, Robert R

    2015-01-12

    We introduce a maskless lithography tool and optically-initiated diffusive photopolymer that enable arbitrary two-dimensional gradient index (GRIN) polymer lens profiles. The lithography tool uses a pulse-width modulated deformable mirror device (DMD) to control the 8-bit gray-scale intensity pattern on the material. The custom polymer responds with a self-developing refractive index profile that is non-linear with optical dose. We show that this nonlinear material response can be corrected with pre-compensation of the intensity pattern to yield high fidelity, optically induced index profiles. The process is demonstrated with quadratic, millimeter aperture GRIN lenses, Zernike polynomials and GRIN Fresnel lenses. PMID:25835673

  1. Study of hybrid driven micromirrors for 3-D variable optical attenuator applications.

    PubMed

    Koh, Kah How; Soon, Bo Woon; Tsai, Julius Minglin; Danner, Aaron J; Lee, Chengkuo

    2012-09-10

    Aluminium-coated micromirrors driven by electrothermal and electromagnetic actuations have been demonstrated for 3-D variable optical attenuation applications. Three types of attenuation schemes based on electrothermal, electromagnetic and hybrid, i.e. combination of electrothermal and electromagnetic, actuations have been developed. In addition, two different designs have been fabricated and characterized to investigate the effects of the variations made to both the actuators on the optical attenuation performances of the micromirror. Our unique design of using both ET and EM actuators simultaneously to achieve attenuation is the first demonstration of such hybrid driven CMOS compatible MEMS VOA device. PMID:23037278

  2. Revealing and Characterizing Dark Excitons through Coherent Multidimensional Spectroscopy.

    PubMed

    Tollerud, Jonathan O; Cundiff, Steven T; Davis, Jeffrey A

    2016-08-26

    Dark excitons are of fundamental importance in a broad range of contexts but are difficult to study using conventional optical spectroscopy due to their weak interaction with light. We show how coherent multidimensional spectroscopy can reveal and characterize dark states. Using this approach, we identify parity-forbidden and spatially indirect excitons in InGaAs/GaAs quantum wells and determine details regarding lifetimes, homogeneous and inhomogeneous linewidths, broadening mechanisms, and coupling strengths. The observations of coherent coupling between these states and bright excitons hint at a role for a multistep process by which excitons in the barrier can relax into the quantum wells. PMID:27610881

  3. Binding energies of indirect excitons in double quantum well systems

    NASA Astrophysics Data System (ADS)

    Rossokhaty, Alex; Schmult, Stefan; Dietsche, Werner; von Klitzing, Klaus; Kukushkin, Igor

    2011-03-01

    A prerequisite towards Bose-Einstein condensation is a cold and dense system of bosons. Indirect excitons in double GaAs/AlGaAs quantum wells (DQWs) are believed to be suitable candidates. Indirect excitons are formed in asymmetric DQW structures by mass filtering, a method which does not require external electric fields. The exciton density and the electron-hole balance can be tuned optically. Binding energies are measured by a resonant microwave absorption technique. Our results show that screening of the indirect excitons becomes already relevant at densities as low as ~ 5 × 109 cm-2 and results in their destruction.

  4. TOPICAL REVIEW A review of the coherent optical control of the exciton and spin states of semiconductor quantum dots

    NASA Astrophysics Data System (ADS)

    Ramsay, A. J.

    2010-10-01

    The spin of a carrier trapped in a self-assembled quantum dot has the potential to be a robust optically active qubit that is compatible with existing III-V semiconductor device technology. A key requirement for building a quantum processor is the ability to dynamically prepare, control and detect single quantum states. Here, experimental progress in the coherent optical control of single semiconductor quantum dots over the past decade is reviewed, alongside an introductory discussion of the basic principles of coherent control.

  5. Optically induced excitonic electroabsorption in a periodically delta-doped InGaAs/GaAs multiple quantum well structure

    NASA Technical Reports Server (NTRS)

    Larsson, A.; Maserjian, J.

    1991-01-01

    Large optically induced Stark shifts have been observed in a periodically delta-doped InGaAs/GaAs multiple quantum well structure. With an excitation intensity of 10 mW/sq cm, an absolute quantum well absorption change of 7000/cm was measured with a corresponding differential absorption change as high as 80 percent. The associated maximum change in the quantum well refractive index is 0.04. This material is promising for device development for all-optical computing and signal processing.

  6. On the relation of protein dynamics and exciton relaxation in pigment-protein complexes: An estimation of the spectral density and a theory for the calculation of optical spectra

    NASA Astrophysics Data System (ADS)

    Renger, Thomas; Marcus, R. A.

    2002-06-01

    A theory for calculating time- and frequency-domain optical spectra of pigment-protein complexes is presented using a density matrix approach. Non-Markovian effects in the exciton-vibrational coupling are included. A correlation function is deduced from the simulation of 1.6 K fluorescence line narrowing spectra of a monomer pigment-protein complex (B777), and then used to calculate fluorescence line narrowing spectra of a dimer complex (B820). A vibrational sideband of an excitonic transition is obtained, a distinct non-Markovian feature, and agrees well with experiment on B820 complexes. The theory and the above correlation function are used elsewhere to make predictions and compare with data on time-domain pump-probe spectra and frequency-domain linear absorption, circular dichroism and fluorescence spectra of Photosystem II reaction centers.

  7. Excitonic gap formation and condensation in the bilayer graphene structure

    NASA Astrophysics Data System (ADS)

    Apinyan, V.; Kopeć, T. K.

    2016-09-01

    We have studied the excitonic gap formation in the Bernal Stacked, bilayer graphene (BLG) structures at half-filling. Considering the local Coulomb interaction between the layers, we calculate the excitonic gap parameter and we discuss the role of the interlayer and intralayer Coulomb interactions and the interlayer hopping on the excitonic pair formation in the BLG. Particularly, we predict the origin of excitonic gap formation and condensation, in relation to the furthermost interband optical transition spectrum. The general diagram of excitonic phase transition is given, explaining different interlayer correlation regimes. The temperature dependence of the excitonic gap parameter is shown and the role of the chemical potential, in the BLG, is discussed in details.

  8. Exciton mapping at subwavelength scales in two-dimensional materials.

    PubMed

    Tizei, Luiz H G; Lin, Yung-Chang; Mukai, Masaki; Sawada, Hidetaka; Lu, Ang-Yu; Li, Lain-Jong; Kimoto, Koji; Suenaga, Kazu

    2015-03-13

    Spatially resolved electron-energy-loss spectroscopy (EELS) is performed at diffuse interfaces between MoS2 and MoSe2 single layers. With a monochromated electron source (20 meV) we successfully probe excitons near the interface by obtaining the low loss spectra at the nanometer scale. The exciton maps clearly show variations even with a 10 nm separation between measurements; consequently, the optical band gap can be measured with nanometer-scale resolution, which is 50 times smaller than the wavelength of the emitted photons. By performing core-loss EELS at the same regions, we observe that variations in the excitonic signature follow the chemical composition. The exciton peaks are observed to be broader at interfaces and heterogeneous regions, possibly due to interface roughness and alloying effects. Moreover, we do not observe shifts of the exciton peak across the interface, possibly because the interface width is not much larger than the exciton Bohr radius. PMID:25815966

  9. Hot-exciton luminescence in ZnTe/MnTe quantum wells

    NASA Astrophysics Data System (ADS)

    Pelekanos, N.; Ding, J.; Fu, Q.; Nurmikko, A. V.; Durbin, S. M.; Kobayashi, M.; Gunshor, R. L.

    1991-04-01

    Hot-exciton luminescence phenomena are investigated in a ZnTe/MnTe single-quantum-well structure where tunneling through thin MnTe barriers suppresses the formation of thermalized luminescence. The longitudinal-optical-phonon-modulated recombination spectra are excitonic in nature and show strong resonance enhancement at energies that lie within localized states below the n=1 exciton.

  10. Optical field emission from resonant gold nanorods driven by femtosecond mid-infrared pulses

    SciTech Connect

    Kusa, F.; Echternkamp, K. E.; Herink, G.; Ropers, C.; Ashihara, S.

    2015-07-15

    We demonstrate strong-field photoelectron emission from gold nanorods driven by femtosecond mid-infrared optical pulses. The maximum photoelectron yield is reached at the localized surface plasmon resonance, indicating that the photoemission is governed by the resonantly-enhanced optical near-field. The wavelength- and field-dependent photoemission yield allows for a noninvasive determination of local field enhancements, and we obtain intensity enhancement factors close to 1300, in good agreement with finite-difference time domain computations.

  11. Optically driven oscillations of ellipsoidal particles. Part I: experimental observations.

    PubMed

    Mihiretie, B M; Snabre, P; Loudet, J-C; Pouligny, B

    2014-12-01

    We report experimental observations of the mechanical effects of light on ellipsoidal micrometre-sized dielectric particles, in water as the continuous medium. The particles, made of polystyrene, have shapes varying between near disk-like (aspect ratio k = 0.2) to very elongated needle-like (k = 8). Rather than the very tightly focused beam geometry of optical tweezers, we use a moderately focused laser beam to manipulate particles individually by optical levitation. The geometry allows us varying the longitudinal position of the particle, and to capture images perpendicular to the beam axis. Experiments show that moderate-k particles are radially trapped with their long axis lying parallel to the beam. Conversely, elongated (k > 3) or flattened (k < 0.3) ellipsoids never come to rest, and permanently "dance" around the beam, through coupled translation-rotation motions. The oscillations are shown to occur in general, be the particle in bulk water or close to a solid boundary, and may be periodic or irregular. We provide evidence for two bifurcations between static and oscillating states, at k ≈ 0.33 and k ≈ 3 for oblate and prolate ellipsoids, respectively. Based on a recently developed 2-dimensional ray-optics simulation (Mihiretie et al., EPL 100, 48005 (2012)), we propose a simple model that allows understanding the physical origin of the oscillations. PMID:25577402

  12. Dark solitons and vortices in the intrinsic bistability regime in exciton polariton condensates

    NASA Astrophysics Data System (ADS)

    Yulin, A. V.; Skryabin, D. V.; Gorbach, A. V.

    2015-08-01

    We report on a class of dark solitons and vortices existing in the exciton-polariton condensates and having discontinuity in their excitonic component. These solutions exist due to an intrinsic bistability of the exciton density in the given optical field and for nonzero detuning between the cavity and excitonic resonances. We specify a well defined energy boundary where they transform into previously known polaritonic dark solitons and vortices.

  13. Self-organized optical device driven by motor proteins

    PubMed Central

    Aoyama, Susumu; Shimoike, Masahiko; Hiratsuka, Yuichi

    2013-01-01

    Protein molecules produce diverse functions according to their combination and arrangement as is evident in a living cell. Therefore, they have a great potential for application in future devices. However, it is currently very difficult to construct systems in which a large number of different protein molecules work cooperatively. As an approach to this challenge, we arranged protein molecules in artificial microstructures and assembled an optical device inspired by a molecular system of a fish melanophore. We prepared arrays of cell-like microchambers, each of which contained a scaffold of microtubule seeds at the center. By polymerizing tubulin from the fixed microtubule seeds, we obtained radially arranged microtubules in the chambers. We subsequently prepared pigment granules associated with dynein motors and attached them to the radial microtubule arrays, which made a melanophore-like system. When ATP was added to the system, the color patterns of the chamber successfully changed, due to active transportation of pigments. Furthermore, as an application of the system, image formation on the array of the optical units was performed. This study demonstrates that a properly designed microstructure facilitates arrangement and self-organization of molecules and enables assembly of functional molecular systems. PMID:24065817

  14. Self-organized optical device driven by motor proteins.

    PubMed

    Aoyama, Susumu; Shimoike, Masahiko; Hiratsuka, Yuichi

    2013-10-01

    Protein molecules produce diverse functions according to their combination and arrangement as is evident in a living cell. Therefore, they have a great potential for application in future devices. However, it is currently very difficult to construct systems in which a large number of different protein molecules work cooperatively. As an approach to this challenge, we arranged protein molecules in artificial microstructures and assembled an optical device inspired by a molecular system of a fish melanophore. We prepared arrays of cell-like microchambers, each of which contained a scaffold of microtubule seeds at the center. By polymerizing tubulin from the fixed microtubule seeds, we obtained radially arranged microtubules in the chambers. We subsequently prepared pigment granules associated with dynein motors and attached them to the radial microtubule arrays, which made a melanophore-like system. When ATP was added to the system, the color patterns of the chamber successfully changed, due to active transportation of pigments. Furthermore, as an application of the system, image formation on the array of the optical units was performed. This study demonstrates that a properly designed microstructure facilitates arrangement and self-organization of molecules and enables assembly of functional molecular systems. PMID:24065817

  15. Exciton-polariton laser

    NASA Astrophysics Data System (ADS)

    Moskalenko, S. A.; Tiginyanu, I. M.

    2016-05-01

    We present a review of the investigations realized in the last decades of the phenomenon of the Bose-Einstein condensation (BEC) in the system of two-dimensional cavity polaritons in semiconductor nanostructures. The conditions at which the excitons interacting with cavity photons form new type of quasiparticles named as polaritons are described. Since polaritons can form in a microcavity a weakly interacting Bose gas, similarly to the exciton gas in semiconductors, the microcavity exciton-polariton BEC emerged in the last decades as a new direction of the exciton BEC in solids, promising for practical applications. The high interest in BEC of exciton-polaritons in semiconductor microcavities is related to the ultra-low threshold lasing which has been demonstrated, in particular, for an electrically injected polariton laser based on bulk GaN microcavity diode working at room temperature.

  16. An opto-mechanical coupled-ring reflector driven by optical force for lasing wavelength control

    NASA Astrophysics Data System (ADS)

    Ren, M.; Cai, H.; Chin, L. K.; Huang, J. G.; Gu, Y. D.; Radhakrishnan, K.; Ser, W.; Liu, A. Q.

    2016-02-01

    In this paper, an opto-mechanical coupled-ring reflector driven by optical gradient force is applied in an external-cavity tunable laser. A pair of mutually coupled ring resonators with a free-standing arc serves as a movable reflector. It obtains a 13.3-nm wavelength tuning range based on an opto-mechanical lasing-wavelength tuning coefficient of 127 GHz/nm. The potential applications include optical network, on-chip optical trapping, sensing, and biology detection.

  17. Optical position feedback for electrostatically driven MOEMS scanners

    NASA Astrophysics Data System (ADS)

    Tortschanoff, A.; Baumgart, M.; Frank, A.; Wildenhain, M.; Sandner, T.; Schenk, H.; Kenda, A.

    2012-03-01

    For MOEMS devices which do not have intrinsic on-chip feedback, position information can be provided with optical methods, most simply by using a reflection from the backside of a MOEMS scanner. Measurement of timing signals using fast differential photodiodes can be used for resonant scanner mirrors performing sinusoidal motion with large amplitude. While this approach provides excellent accuracy it cannot be directly extended to arbitrary trajectories or static deflection angles. Another approach is based on the measurement of the position of the reflected laser beam with a quadrant diode. In this work, we present position sensing devices based on either principle and compare both approaches showing first experimental results from the implemented devices

  18. A Modular, IGBT Driven, Ignitron Switched, Optically Controlled Power Supply

    NASA Astrophysics Data System (ADS)

    Carroll, Evan; von der Linden, Jens; You, Setthivoine

    2013-10-01

    An experiment to investigate the dynamics of canonical flux tubes at the University of Washington uses two high energy pulsed power supplies to generate and sustain the plasma discharge. A modular 240 μF , 12 kV DC capacitor based power supply, discharged by ignitron, has been developed specifically for this application. Design considerations include minimizing inductance, rapid switching, fast rise times, and electrically isolated control. An optically coupled front panel and fast IGBT ignitron drive circuit, sequenced manually or by software, control the charge and discharge of the power supply. A complete, sequenced charge/discharge has been successfully tested with a dummy load, producing a peak current of 100 kA and a rise time of 25 μs . This work was sponsored in part by the US DOE Grant DE-SC0010340.

  19. Many-body Effects and the Role of Indirect Excitons in Asymmetric InGaAs/GaAs Double Quantum Wells

    NASA Astrophysics Data System (ADS)

    Smallwood, Christopher; Suzuki, Takeshi; Singh, Rohan; Autry, Travis; Day, Matthew; Jabeen, Fauzia; Cundiff, Steven

    In semiconductor research, a fundamental question is how excitons in nearby but distinct spatial locations interact and exchange energy. In quantum well heterostructures, these interactions can be conveniently probed via optical coherent multidimensional spectroscopy (CMDS). Recently, it has been shown using CMDS that reducing the GaAs barrier from 30 nm to 10 nm between two asymmetric InGaAs quantum wells results in interactions driven by many-body effects. Here, we use the technique to show that for narrower barrier thicknesses, the interactions are accompanied by an emergence of spatially indirect excitons. Quantitative measurements of the effects are presented, which will be useful in tailoring GaAs heterostructure devices, and may also inform the role that excitonic interactions play in more complicated systems like microcavity polariton structures and/or photosynthetic light harvesting complexes.

  20. Optical-parametric-oscillator solitons driven by the third harmonic.

    PubMed

    Lutsky, Vitaly; Malomed, Boris A

    2004-12-01

    We introduce a model of a lossy second-harmonic-generating (chi(2)) cavity externally pumped at the third harmonic, which gives rise to driving terms of a new type, corresponding to a cross-parametric gain. The equation for the fundamental-frequency (FF) wave may also contain a quadratic self-driving term, which is generated by the cubic nonlinearity of the medium. Unlike previously studied phase-matched models of chi(2) cavities driven at the second harmonic or at FF, the present one admits an exact analytical solution for the soliton, at a special value of the gain parameter. Two families of solitons are found in a numerical form, and their stability area is identified through numerical computation of the perturbation eigenvalues (stability of the zero solution, which is a necessary condition for the soliton's stability, is investigated in an analytical form). One family is a continuation of the special analytical solution. At given values of the parameters, one soliton is stable and the other one is not; they swap their stability at a critical value of the mismatch parameter. The stability of the solitons is also verified in direct simulations, which demonstrate that an unstable pulse rearranges itself into a stable one, or into a delocalized state, or decays to zero. A soliton which was given an initial boost C starts to move but quickly comes to a halt, if the boost is smaller than a critical value C(cr) . If C > C(cr) , the boost destroys the soliton (sometimes, through splitting into two secondary pulses). Interactions between initially separated solitons are investigated, too. It is concluded that stable solitons always merge into a single one. In the system with weak loss, it appears in a vibrating form, slowly relaxing to the static shape. With stronger loss, the final soliton emerges in the stationary form. PMID:15697523

  1. Optical-parametric-oscillator solitons driven by the third harmonic

    NASA Astrophysics Data System (ADS)

    Lutsky, Vitaly; Malomed, Boris A.

    2004-12-01

    We introduce a model of a lossy second-harmonic-generating (χ(2)) cavity externally pumped at the third harmonic, which gives rise to driving terms of a new type, corresponding to a cross-parametric gain. The equation for the fundamental-frequency (FF) wave may also contain a quadratic self-driving term, which is generated by the cubic nonlinearity of the medium. Unlike previously studied phase-matched models of χ(2) cavities driven at the second harmonic or at FF, the present one admits an exact analytical solution for the soliton, at a special value of the gain parameter. Two families of solitons are found in a numerical form, and their stability area is identified through numerical computation of the perturbation eigenvalues (stability of the zero solution, which is a necessary condition for the soliton’s stability, is investigated in an analytical form). One family is a continuation of the special analytical solution. At given values of the parameters, one soliton is stable and the other one is not; they swap their stability at a critical value of the mismatch parameter. The stability of the solitons is also verified in direct simulations, which demonstrate that an unstable pulse rearranges itself into a stable one, or into a delocalized state, or decays to zero. A soliton which was given an initial boost C starts to move but quickly comes to a halt, if the boost is smaller than a critical value Ccr . If C>Ccr , the boost destroys the soliton (sometimes, through splitting into two secondary pulses). Interactions between initially separated solitons are investigated, too. It is concluded that stable solitons always merge into a single one. In the system with weak loss, it appears in a vibrating form, slowly relaxing to the static shape. With stronger loss, the final soliton emerges in the stationary form.

  2. A photo-driven dual-frequency addressable optical device of banana-shaped molecules

    SciTech Connect

    Krishna Prasad, S. Lakshmi Madhuri, P.; Hiremath, Uma S.; Yelamaggad, C. V.

    2014-03-17

    We propose a photonic switch employing a blend of host banana-shaped liquid crystalline molecules and guest photoisomerizable calamitic molecules. The material exhibits a change in the sign of the dielectric anisotropy switching from positive to negative, at a certain crossover frequency of the probing field. The consequent change in electric torque can be used to alter the orientation of the molecules between surface-determined and field-driven optical states resulting in a large change in the optical transmission characteristics. Here, we demonstrate the realization of this feature by an unpolarized UV beam, the first of its kind for banana-shaped molecules. The underlying principle of photoisomerization eliminates the need for a second driving frequency. The device also acts as a reversible conductance switch with an order of magnitude increase of conductivity brought about by light. Possible usage of this for optically driven display devices and image storage applications is suggested.

  3. Preliminary study of lever-based optical driven micro-actuator

    NASA Astrophysics Data System (ADS)

    Lin, Chih-Lang; Li, Yi-Hsiung; Lin, Chin-Te; Chiang, Chia-Chin; Liu, Yi-Jui; Chung, Tien-Tung; Baldeck, Patrice L.

    2012-04-01

    This study presents a novel type of optically driven lever-based micro-actuator fabricated using two-photon polymerization 3D-microfabrication technique. The lever is composed of a beam, an arch, and a sphere. First, optical tweezers is applied on the spheres to demonstrate the actuation of the lever. A spring is jointed at the lever for verifying the induced forces. Under the dragging by laser focusing, the lever simultaneously turns and results a torque like a mechanical arm. Then, the demonstration of a photo-driven micro-transducer with a mechanical arm and a gear is preformed. The experimental result indicates that our design enables precise manipulation of the mirco-actuator by optical tweezers at micron scale. This study provides a possibility for driving micron-sized structured mechanisms, such as connecting rods, valves. It is expected to contribute on the investigation of "Lab-on-a-chip".

  4. Preliminary study of lever-based optical driven micro-actuator

    NASA Astrophysics Data System (ADS)

    Lin, Chih-Lang; Li, Yi-Hsiung; Lin, Chin-Te; Chiang, Chia-Chin; Liu, Yi-Jui; Chung, Tien-Tung; Baldeck, Patrice L.

    2011-11-01

    This study presents a novel type of optically driven lever-based micro-actuator fabricated using two-photon polymerization 3D-microfabrication technique. The lever is composed of a beam, an arch, and a sphere. First, optical tweezers is applied on the spheres to demonstrate the actuation of the lever. A spring is jointed at the lever for verifying the induced forces. Under the dragging by laser focusing, the lever simultaneously turns and results a torque like a mechanical arm. Then, the demonstration of a photo-driven micro-transducer with a mechanical arm and a gear is preformed. The experimental result indicates that our design enables precise manipulation of the mirco-actuator by optical tweezers at micron scale. This study provides a possibility for driving micron-sized structured mechanisms, such as connecting rods, valves. It is expected to contribute on the investigation of "Lab-on-a-chip".

  5. Bias activated dielectric response of excitons and excitonic Mott transition in quantum confined lasers structures.

    NASA Astrophysics Data System (ADS)

    Bhunia, Amit; Bansal, Kanika; Datta, Shouvik; Alshammari, Marzook S.; Henini, Mohamed

    In contrast to the widely reported optical techniques, there are hardly any investigations on corresponding electrical signatures of condensed matter physics of excitonic phenomena. We studied small signal steady state capacitance response in III-V materials based multi quantum well (AlGaInP) and MBE grown quantum dot (InGaAs) laser diodes to identify signatures of excitonic presence. Conductance activation by forward bias was probed using frequency dependent differential capacitance response (fdC/df), which changes characteristically with the onset of light emission indicating the occurrence of negative activation energy. Our analysis shows that it is connected with a steady state population of exciton like bound states. Calculated average energy of this bound state matches well with the binding energy of weakly confined excitons in this type of structures. Further increase in charge injection decreases the differential capacitive response in AlGaInP based diodes, indicating a gradual Mott transition of excitonic states into electron hole plasma. This electrical description of excitonic Mott transition is fully supplemented by standard optical spectroscopic signatures of band gap renormalization and phase space filling effects.

  6. Exciton fission and charge generation via triplet excitons in pentacene/C60 bilayers.

    PubMed

    Rao, Akshay; Wilson, Mark W B; Hodgkiss, Justin M; Albert-Seifried, Sebastian; Bässler, Heinz; Friend, Richard H

    2010-09-15

    Organic photovoltaic devices are currently studied due to their potential suitability for flexible and large-area applications, though efficiencies are presently low. Here we study pentacene/C(60) bilayers using transient optical absorption spectroscopy; such structures exhibit anomalously high quantum efficiencies. We show that charge generation primarily occurs 2-10 ns after photoexcitation. This supports a model where charge is generated following the slow diffusion of triplet excitons to the heterojunction. These triplets are shown to be present from early times (<200 fs) and result from the fission of a spin-singlet exciton to form two spin-triplet excitons. These results elucidate exciton and charge generation dynamics in the pentacene/C(60) system and demonstrate that the tuning of the energetic levels of organic molecules to take advantages of singlet fission could lead to greatly enhanced photocurrent in future OPVs. PMID:20735067

  7. Valley-Polarized Interlayer Excitons in 2D Semiconductor Heterostructures

    NASA Astrophysics Data System (ADS)

    Rivera, Pasqual; Seyler, Kyle; Yu, Hongyi; Schaibley, John; Yan, Jiaqiang; Mandrus, David; Xu, Xiaodong

    Vertically stacked monolayers of MoSe2 and WSe2 feature a type-II band alignment causing the formation of interlayer excitons, where the Coulomb bound hole and electron reside in different layers. This species of exciton has lifetime many orders of magnitude longer than intralayer valley excitons, providing a unique and advantageous system for investigating valley exciton physics. Here, we optically pump the MoSe2-WSe2 heterostructure with circularly polarized light, creating interlayer valley excitons with gate-tunable spin-valley polarization lifetime up to 40 ns. This long valley lifetime enables the diffusion of the interlayer valley exciton gas to be visualized. Under increasing excitation power we observe the formation of a ring in the spatial distribution of the valley polarization, a manifestation of significant valley-selective exchange interactions at high exciton densities. The combination of long valley polarization and spatial diffusion makes the interlayer exciton in semiconductor heterostructures an exciting platform for studies of valley exciton physics.

  8. Visible Light Driven Photocatalytic Reactor Based on Micro-structured Polymer Optical Fiber Preform

    NASA Astrophysics Data System (ADS)

    Li, Dong-Dong; She, Jiang-Bo; Wang, Chang-Shun; Peng, Bo

    2014-05-01

    A novel visible light driven photocatalytic reactor with 547 pieces of Ag/AgBr-film-modified capillaries is reported and it is derived from a microstructured polymer optical fiber (MPOF) preform. The MPOF preform not only plays the role of a light-transmitting media, but it is also a Ag/AgBr supporting and waste-water pipe to supply the photocatalytic degradation of dyes solute. The photocatalytic reactor has such a large surface area for Ag/AgBr loading, which is a visible light driven photocatalyst that photodegradation efficiency is enhanced.

  9. Micro optical diffusion sensor using a comb-driven micro Fresnel mirror.

    PubMed

    Matoba, Yoshiaki; Taguchi, Yoshihiro; Nagasaka, Yuji

    2015-01-12

    We have developed a novel micro optical diffusion sensor (MODS) with a newly proposed comb-driven-micro Fresnel mirror (CD-MFM) scanner to detect structural changes in biological samples. By controlling the fringe spacing of the excitation laser beam, we can tune the decay time to obtain quick and precise measurements. In this study, the pre-tilted mirror is rotated by vertical comb-driven actuators; the resulting change in the mirror angle alters the fringe spacing. The validity of the proposed mirror scanner is confirmed in simulations and in an experiment using a fabricated prototype device. PMID:25835693

  10. Exciton energy recycling from ZnO defect levels: towards electrically driven hybrid quantum-dot white light-emitting-diodes

    NASA Astrophysics Data System (ADS)

    Zhao, Xin; Liu, Weizhen; Chen, Rui; Gao, Yuan; Zhu, Binbin; Demir, Hilmi Volkan; Wang, Shijie; Sun, Handong

    2016-03-01

    An electrically driven quantum-dot hybrid white light-emitting diode is fabricated via spin coating CdSe quantum dots onto a GaN/ZnO nanorod matrix. For the first time, quantum dots are excited by fluorescence resonance energy transfer from the carriers trapped at surface defect levels. The prototype device exhibits achromatic emission, with a chromaticity coordinate of (0.327, 0.330), and correlated color temperature similar to sunlight.An electrically driven quantum-dot hybrid white light-emitting diode is fabricated via spin coating CdSe quantum dots onto a GaN/ZnO nanorod matrix. For the first time, quantum dots are excited by fluorescence resonance energy transfer from the carriers trapped at surface defect levels. The prototype device exhibits achromatic emission, with a chromaticity coordinate of (0.327, 0.330), and correlated color temperature similar to sunlight. Electronic supplementary information (ESI) available. See DOI: 10.1039/c5nr09261b

  11. Excitonic luminescence upconversion in a two-dimensional semiconductor

    NASA Astrophysics Data System (ADS)

    Jones, Aaron M.; Yu, Hongyi; Schaibley, John R.; Yan, Jiaqiang; Mandrus, David G.; Taniguchi, Takashi; Watanabe, Kenji; Dery, Hanan; Yao, Wang; Xu, Xiaodong

    2016-04-01

    Photon upconversion is an elementary light-matter interaction process in which an absorbed photon is re-emitted at higher frequency after extracting energy from the medium. This phenomenon lies at the heart of optical refrigeration in solids, where upconversion relies on anti-Stokes processes enabled either by rare-earth impurities or exciton-phonon coupling. Here, we demonstrate a luminescence upconversion process from a negatively charged exciton to a neutral exciton resonance in monolayer WSe2, producing spontaneous anti-Stokes emission with an energy gain of 30 meV. Polarization-resolved measurements find this process to be valley selective, unique to monolayer semiconductors. Since the charged exciton binding energy closely matches the 31 meV A1' optical phonon, we ascribe the spontaneous excitonic anti-Stokes to doubly resonant Raman scattering, where the incident and outgoing photons are in resonance with the charged and neutral excitons, respectively. In addition, we resolve a charged exciton doublet with a 7 meV splitting, probably induced by exchange interactions, and show that anti-Stokes scattering is efficient only when exciting the doublet peak resonant with the phonon, further confirming the excitonic doubly resonant picture.

  12. Josephson oscillations between exciton condensates in electrostatic traps

    SciTech Connect

    Rontani, Massimo

    2009-08-15

    Technological advances allow for tunable lateral confinement of cold dipolar excitons in coupled quantum wells. We consider theoretically the Josephson effect between exciton condensates in two traps separated by a weak link. The flow of the exciton supercurrent is driven by the dipole-energy difference between the traps. The Josephson oscillations may be observed after ensemble average of the time correlation of photons separately emitted from the two traps. The fringe visibility is controlled by the trap coupling and is robust against quantum and thermal fluctuations.

  13. Probing excitonic dark states in single-layer tungsten disulphide

    NASA Astrophysics Data System (ADS)

    Ye, Ziliang; Cao, Ting; O'Brien, Kevin; Zhu, Hanyu; Yin, Xiaobo; Wang, Yuan; Louie, Steven G.; Zhang, Xiang

    2014-09-01

    Transition metal dichalcogenide (TMDC) monolayers have recently emerged as an important class of two-dimensional semiconductors with potential for electronic and optoelectronic devices. Unlike semi-metallic graphene, layered TMDCs have a sizeable bandgap. More interestingly, when thinned down to a monolayer, TMDCs transform from indirect-bandgap to direct-bandgap semiconductors, exhibiting a number of intriguing optical phenomena such as valley-selective circular dichroism, doping-dependent charged excitons and strong photocurrent responses. However, the fundamental mechanism underlying such a strong light-matter interaction is still under intensive investigation. First-principles calculations have predicted a quasiparticle bandgap much larger than the measured optical gap, and an optical response dominated by excitonic effects. In particular, a recent study based on a GW plus Bethe-Salpeter equation (GW-BSE) approach, which employed many-body Green's-function methodology to address electron-electron and electron-hole interactions, theoretically predicted a diversity of strongly bound excitons. Here we report experimental evidence of a series of excitonic dark states in single-layer WS2 using two-photon excitation spectroscopy. In combination with GW-BSE theory, we prove that the excitons are of Wannier type, meaning that each exciton wavefunction extends over multiple unit cells, but with extraordinarily large binding energy (~0.7 electronvolts), leading to a quasiparticle bandgap of 2.7 electronvolts. These strongly bound exciton states are observed to be stable even at room temperature. We reveal an exciton series that deviates substantially from hydrogen models, with a novel energy dependence on the orbital angular momentum. These excitonic energy levels are experimentally found to be robust against environmental perturbations. The discovery of excitonic dark states and exceptionally large binding energy not only sheds light on the importance of many

  14. Deformation Measurement of a Driven Pile Using Distributed Fibre-optic Sensing

    NASA Astrophysics Data System (ADS)

    Monsberger, Christoph; Woschitz, Helmut; Hayden, Martin

    2016-03-01

    New developments in distributed fibre-optic sensing allow the measurement of strain with a very high precision of about 1 µm / m and a spatial resolution of 10 millimetres or even better. Thus, novel applications in several scientific fields may be realised, e. g. in structural monitoring or soil and rock mechanics. Especially due to the embedding capability of fibre-optic sensors, fibre-optic systems provide a valuable extension to classical geodetic measurement methods, which are limited to the surface in most cases. In this paper, we report about the application of an optical backscatter reflectometer for deformation measurements along a driven pile. In general, pile systems are used in civil engineering as an efficient and economic foundation of buildings and other structures. Especially the length of the piles is crucial for the final loading capacity. For optimization purposes, the interaction between the driven pile and the subsurface material is investigated using pile testing methods. In a field trial, we used a distributed fibre-optic sensing system for measuring the strain below the surface of an excavation pit in order to derive completely new information. Prior to the field trial, the fibre-optic sensor was investigated in the laboratory. In addition to the results of these lab studies, we briefly describe the critical process of field installation and show the most significant results from the field trial, where the pile was artificially loaded up to 800 kN. As far as we know, this is the first time that the strain is monitored along a driven pile with such a high spatial resolution.

  15. Atmospheric-pressure microplasma in dielectrophoresis-driven bubbles for optical emission spectroscopy.

    PubMed

    Fan, Shih-Kang; Shen, Yan-Ting; Tsai, Ling-Pin; Hsu, Cheng-Che; Ko, Fu-Hsiang; Cheng, Yu-Ting

    2012-10-01

    The manipulation of bubbles and the ignition of microplasma within a 200 nL bubble at atmospheric pressure and in an inert silicone oil environment were achieved. Driven by dielectrophoresis (DEP), bubble generation, transportation, mixing, splitting, and expelling were demonstrated. This process facilitated the preparation of various bubbles with tuneable gas compositions. Different gas bubbles, including air, argon (Ar), helium (He), and Ar/He mixtures, were manipulated and ignited to the plasma state by dielectric barrier discharge (DBD) within a 50 μm-high gap between parallel plates. Moving and splitting the atmospheric-pressure microplasma in different gas bubbles were achieved by DEP. The excited light of the microplasma was recorded by an optical spectrometer for the optical emission spectroscopy (OES) analyses. The characteristic peaks of air, Ar, and He were observed in the DEP-driven microplasma. With the capability to manipulate bubbles and microplasma, this platform could be used for gas analyses in the future. PMID:22878730

  16. Optical gain in 1.3-μm electrically driven dilute nitride VCSOAs.

    PubMed

    Lisesivdin, Sefer Bora; Khan, Nadir Ali; Mazzucato, Simone; Balkan, Naci; Adams, Michael John; Korpijärvi, Ville-Markus; Guina, Mircea; Mezosi, Gabor; Sorel, Marc

    2014-01-01

    We report the observation of room-temperature optical gain at 1.3 μm in electrically driven dilute nitride vertical cavity semiconductor optical amplifiers. The gain is calculated with respect to injected power for samples with and without a confinement aperture. At lower injected powers, a gain of almost 10 dB is observed in both samples. At injection powers over 5 nW, the gain is observed to decrease. For nearly all investigated power levels, the sample with confinement aperture gives slightly higher gain. PMID:24417791

  17. Optical gain in 1.3-μm electrically driven dilute nitride VCSOAs

    PubMed Central

    2014-01-01

    We report the observation of room-temperature optical gain at 1.3 μm in electrically driven dilute nitride vertical cavity semiconductor optical amplifiers. The gain is calculated with respect to injected power for samples with and without a confinement aperture. At lower injected powers, a gain of almost 10 dB is observed in both samples. At injection powers over 5 nW, the gain is observed to decrease. For nearly all investigated power levels, the sample with confinement aperture gives slightly higher gain. PMID:24417791

  18. Optical Spin-Transfer-Torque-Driven Domain-Wall Motion in a Ferromagnetic Semiconductor

    NASA Astrophysics Data System (ADS)

    Ramsay, A. J.; Roy, P. E.; Haigh, J. A.; Otxoa, R. M.; Irvine, A. C.; Janda, T.; Campion, R. P.; Gallagher, B. L.; Wunderlich, J.

    2015-02-01

    We demonstrate optical manipulation of the position of a domain wall in a dilute magnetic semiconductor, GaMnAsP. Two main contributions are identified. First, photocarrier spin exerts a spin-transfer torque on the magnetization via the exchange interaction. The direction of the domain-wall motion can be controlled using the helicity of the laser. Second, the domain wall is attracted to the hot spot generated by the focused laser. Unlike magnetic-field-driven domain-wall depinning, these mechanisms directly drive domain-wall motion, providing an optical tweezerlike ability to position and locally probe domain walls.

  19. Photophysics of pentacene thin films: The role of exciton fission and heating effects

    NASA Astrophysics Data System (ADS)

    Rao, Akshay; Wilson, Mark W. B.; Albert-Seifried, Sebastian; di Pietro, Riccardo; Friend, Richard H.

    2011-11-01

    There is evidence that the photo-generated singlet exciton in polycrystalline pentacene films undergoes rapid and efficient fission to form two triplet excitons. However, the role of exciton fission in pentacene has been controversial, with previous studies putting forward alternate relaxation pathways for the singlet exciton, such as excimer or charge formation, or internal conversion to a doubly excited exciton. We report temperature- and angular-dependent ultrafast transient optical absorption measurements in a wide spectral and temporal window. Angular-dependent transient spectra identify a common origin to photo-induced absorptions at 530 and 860 nm, which we associate with triplet excitons. These constitute the dominant relaxation channel for singlet excitons. Other features, particularly near 620 nm, previously assigned to excimers or electronic charges, are shown to be caused by thermal modulation from the optical pump.

  20. Time Dependent Study of Multiple Exciton Generation in Nanocrystal Quantum Dots

    NASA Astrophysics Data System (ADS)

    Damtie, Fikeraddis A.; Wacker, Andreas

    2016-03-01

    We study the exciton dynamics in an optically excited nanocrystal quantum dot. Multiple exciton formation is more efficient in nanocrystal quantum dots compared to bulk semiconductors due to enhanced Coulomb interactions and the absence of conservation of momentum. The formation of multiple excitons is dependent on different excitation parameters and the dissipation. We study this process within a Lindblad quantum rate equation using the full many-particle states. We optically excite the system by creating a single high energy exciton ESX in resonance to a double exciton EDX. With Coulomb electron-electron interaction, the population can be transferred from the single exciton to the double exciton state by impact ionisation (inverse Auger process). The ratio between the recombination processes and the absorbed photons provide the yield of the structure. We observe a quantum yield of comparable value to experiment assuming typical experimental conditions for a 4 nm PbS quantum dot.

  1. Measurement of an Explosively Driven Hemispherical Shell Using 96 Points of Optical Velocimetry

    SciTech Connect

    Danielson, J. R.; Daykin, E P; Diaz, A. B.; Doty, D. L.; Frogget, B. C.; Furlanetto, M. R.; Gallegos, C. H.; Gibo, M; Garza, A; Holtkamp, D B; Hutchins, M S; Perez, C; Perez, C; Pena, M; Romero, V T; Shinas, M A; Teel, M G; Tabaka, L J

    2014-04-01

    We report the measurement of the surface motion of a hemispherical copper shell driven by high explosives. This measurement was made using three 32-channel multiplexed photonic Doppler velocimetry (PDV) systems, in combination with a novel compound optical probe. Clearly visible are detailed features of the motion of the shell over time, enhanced by spatial correlation. Significant non-normal motion is apparent, and challenges in measuring such a geometry are discussed.

  2. Permanent Rabi oscillations in coupled exciton-photon systems with PT -symmetry

    PubMed Central

    Chestnov, Igor Yu.; Demirchyan, Sevak S.; Alodjants, Alexander P.; Rubo, Yuri G.; Kavokin, Alexey V.

    2016-01-01

    We propose a physical mechanism which enables permanent Rabi oscillations in driven-dissipative condensates of exciton-polaritons in semiconductor microcavities subjected to external magnetic fields. The method is based on stimulated scattering of excitons from the incoherent reservoir. We demonstrate that permanent non-decaying oscillations may appear due to the parity-time symmetry of the coupled exciton-photon system realized in a specific regime of pumping to the exciton state and depletion of the reservoir. At non-zero exciton-photon detuning, robust permanent Rabi oscillations occur with unequal amplitudes of exciton and photon components. Our predictions pave way to realization of integrated circuits based on exciton-polariton Rabi oscillators. PMID:26790534

  3. Permanent Rabi oscillations in coupled exciton-photon systems with PT-symmetry.

    PubMed

    Chestnov, Igor Yu; Demirchyan, Sevak S; Alodjants, Alexander P; Rubo, Yuri G; Kavokin, Alexey V

    2016-01-01

    We propose a physical mechanism which enables permanent Rabi oscillations in driven-dissipative condensates of exciton-polaritons in semiconductor microcavities subjected to external magnetic fields. The method is based on stimulated scattering of excitons from the incoherent reservoir. We demonstrate that permanent non-decaying oscillations may appear due to the parity-time symmetry of the coupled exciton-photon system realized in a specific regime of pumping to the exciton state and depletion of the reservoir. At non-zero exciton-photon detuning, robust permanent Rabi oscillations occur with unequal amplitudes of exciton and photon components. Our predictions pave way to realization of integrated circuits based on exciton-polariton Rabi oscillators. PMID:26790534

  4. Exciton complexes in low dimensional transition metal dichalcogenides

    NASA Astrophysics Data System (ADS)

    Thilagam, A.

    2014-08-01

    We examine the excitonic properties of layered configurations of low dimensional transition metal dichalcogenides (LTMDCs) using the fractional dimensional space approach. The binding energies of the exciton, trion, and biexciton in LTMDCs of varying layers are analyzed, and linked to the dimensionality parameter α, which provides insight into critical electro-optical properties (relative oscillator strength, absorption spectrum, exciton-exciton interaction) of the material systems. The usefulness of α is highlighted by its independence of the physical mechanisms underlying the confinement effects of geometrical structures. Our estimates of the binding energies of exciton complexes for the monolayer configuration of transition metal dichalcogenides suggest a non-collinear structure for the trion and a positronium-molecule-like square structure for the biexciton.

  5. Exciton complexes in low dimensional transition metal dichalcogenides

    SciTech Connect

    Thilagam, A.

    2014-08-07

    We examine the excitonic properties of layered configurations of low dimensional transition metal dichalcogenides (LTMDCs) using the fractional dimensional space approach. The binding energies of the exciton, trion, and biexciton in LTMDCs of varying layers are analyzed, and linked to the dimensionality parameter α, which provides insight into critical electro-optical properties (relative oscillator strength, absorption spectrum, exciton-exciton interaction) of the material systems. The usefulness of α is highlighted by its independence of the physical mechanisms underlying the confinement effects of geometrical structures. Our estimates of the binding energies of exciton complexes for the monolayer configuration of transition metal dichalcogenides suggest a non-collinear structure for the trion and a positronium-molecule-like square structure for the biexciton.

  6. Exciton Lifetime Paradoxically Enhanced by Dissipation and Decoherence: Toward Efficient Energy Conversion of a Solar Cell

    NASA Astrophysics Data System (ADS)

    Yamada, Yasuhiro; Yamaji, Youhei; Imada, Masatoshi

    2015-11-01

    Energy dissipation and decoherence are at first glance harmful to acquiring the long exciton lifetime desired for efficient photovoltaics. In the presence of both optically forbidden (namely, dark) and allowed (bright) excitons, however, they can be instrumental, as suggested in photosynthesis. By simulating the quantum dynamics of exciton relaxations, we show that the optimized decoherence that imposes a quantum-to-classical crossover with the dissipation realizes a dramatically longer lifetime. In an example of a carbon nanotube, the exciton lifetime increases by nearly 2 orders of magnitude when the crossover triggers a stable high population in the dark excitons.

  7. Exciton Lifetime Paradoxically Enhanced by Dissipation and Decoherence: Toward Efficient Energy Conversion of a Solar Cell.

    PubMed

    Yamada, Yasuhiro; Yamaji, Youhei; Imada, Masatoshi

    2015-11-01

    Energy dissipation and decoherence are at first glance harmful to acquiring the long exciton lifetime desired for efficient photovoltaics. In the presence of both optically forbidden (namely, dark) and allowed (bright) excitons, however, they can be instrumental, as suggested in photosynthesis. By simulating the quantum dynamics of exciton relaxations, we show that the optimized decoherence that imposes a quantum-to-classical crossover with the dissipation realizes a dramatically longer lifetime. In an example of a carbon nanotube, the exciton lifetime increases by nearly 2 orders of magnitude when the crossover triggers a stable high population in the dark excitons. PMID:26588415

  8. Exciton-exciton annihilation and biexciton stimulated emission in graphene nanoribbons.

    PubMed

    Soavi, Giancarlo; Dal Conte, Stefano; Manzoni, Cristian; Viola, Daniele; Narita, Akimitsu; Hu, Yunbin; Feng, Xinliang; Hohenester, Ulrich; Molinari, Elisa; Prezzi, Deborah; Müllen, Klaus; Cerullo, Giulio

    2016-01-01

    Graphene nanoribbons display extraordinary optical properties due to one-dimensional quantum-confinement, such as width-dependent bandgap and strong electron-hole interactions, responsible for the formation of excitons with extremely high binding energies. Here we use femtosecond transient absorption spectroscopy to explore the ultrafast optical properties of ultranarrow, structurally well-defined graphene nanoribbons as a function of the excitation fluence, and the impact of enhanced Coulomb interaction on their excited states dynamics. We show that in the high-excitation regime biexcitons are formed by nonlinear exciton-exciton annihilation, and that they radiatively recombine via stimulated emission. We obtain a biexciton binding energy of ≈ 250 meV, in very good agreement with theoretical results from quantum Monte Carlo simulations. These observations pave the way for the application of graphene nanoribbons in photonics and optoelectronics. PMID:26984281

  9. Exciton-exciton annihilation and biexciton stimulated emission in graphene nanoribbons

    NASA Astrophysics Data System (ADS)

    Soavi, Giancarlo; Dal Conte, Stefano; Manzoni, Cristian; Viola, Daniele; Narita, Akimitsu; Hu, Yunbin; Feng, Xinliang; Hohenester, Ulrich; Molinari, Elisa; Prezzi, Deborah; Müllen, Klaus; Cerullo, Giulio

    2016-03-01

    Graphene nanoribbons display extraordinary optical properties due to one-dimensional quantum-confinement, such as width-dependent bandgap and strong electron-hole interactions, responsible for the formation of excitons with extremely high binding energies. Here we use femtosecond transient absorption spectroscopy to explore the ultrafast optical properties of ultranarrow, structurally well-defined graphene nanoribbons as a function of the excitation fluence, and the impact of enhanced Coulomb interaction on their excited states dynamics. We show that in the high-excitation regime biexcitons are formed by nonlinear exciton-exciton annihilation, and that they radiatively recombine via stimulated emission. We obtain a biexciton binding energy of ~250 meV, in very good agreement with theoretical results from quantum Monte Carlo simulations. These observations pave the way for the application of graphene nanoribbons in photonics and optoelectronics.

  10. Nano-stepper-driven optical shutter for applications in free-space micro-optics

    NASA Astrophysics Data System (ADS)

    Zawadzka, Justyna; Li, Lijie; Unamuno, Anartz; Uttamchandani, Deepak G.

    2002-09-01

    In this paper we report a simple design of a micro-optical shutter/attenuator. The standard MUMPS process was used to fabricate the device. A vertically erected, gold-coated, 200x300 mm side length micro-mirror was precisely placed between the end faces of two closely spaced optical fibers. The position of the micro-mirror with respect to the optical fiber end face was controlled by a nano-stepping motor array. Optical and mechanical tests were performed on the device. A 1.55 mm laser beam was sent along the optical fiber. When the micro-mirror was removed from the front of the fiber, the coupling efficiency between two fibers was -10 dBm. Once the micro-mirror was placed in the optical path the coupling efficiency dropped to -51.5 dBm. The best attenuation was obtained when the micro-mirror blocked the whole cross-section of the laser beam diameter. It is evident that the device can operate as a high precision fiber optic attenuator or shutter.

  11. Storing excitons in transition-metal dichalcogenides using dark states

    NASA Astrophysics Data System (ADS)

    Gunlycke, Daniel; Tseng, Frank; Simsek, Ergun

    Monolayer transition-metal dichalcogenides exhibit strongly bound excitons confined to two dimensions. One challenge in exploiting these excitons is that they have a finite life time and collapse through electron-hole recombination. We propose that the exciton life time could be extended by transitioning the exciton population into dark states. The symmetry of these dark states require the electron and hole to be spatially separated, which not only causes these states to be optically inactive but also inhibits electron-hole recombination. Based on an atomistic model we call the Triangular Lattice Exciton (3ALE) model, we derive transition matrix elements and approximate selection rules showing that excitons could be transitioned into and out of dark states using a pulsed infrared laser. For illustration, we also present exciton population scenarios based on different recombination decay constants. Longer exciton lifetimes could make these materials candidates for applications in energy management and quantum information processing. This work was supported by the Office of Naval Research, directly and through the Naval Research Laboratory.

  12. Mapping the exciton diffusion in semiconductor nanocrystal solids.

    PubMed

    Kholmicheva, Natalia; Moroz, Pavel; Bastola, Ebin; Razgoniaeva, Natalia; Bocanegra, Jesus; Shaughnessy, Martin; Porach, Zack; Khon, Dmitriy; Zamkov, Mikhail

    2015-03-24

    Colloidal nanocrystal solids represent an emerging class of functional materials that hold strong promise for device applications. The macroscopic properties of these disordered assemblies are determined by complex trajectories of exciton diffusion processes, which are still poorly understood. Owing to the lack of theoretical insight, experimental strategies for probing the exciton dynamics in quantum dot solids are in great demand. Here, we develop an experimental technique for mapping the motion of excitons in semiconductor nanocrystal films with a subdiffraction spatial sensitivity and a picosecond temporal resolution. This was accomplished by doping PbS nanocrystal solids with metal nanoparticles that force the exciton dissociation at known distances from their birth. The optical signature of the exciton motion was then inferred from the changes in the emission lifetime, which was mapped to the location of exciton quenching sites. By correlating the metal-metal interparticle distance in the film with corresponding changes in the emission lifetime, we could obtain important transport characteristics, including the exciton diffusion length, the number of predissociation hops, the rate of interparticle energy transfer, and the exciton diffusivity. The benefits of this approach to device applications were demonstrated through the use of two representative film morphologies featuring weak and strong interparticle coupling. PMID:25682881

  13. Excitations, optical absorption spectra, and optical excitonic gaps of heterofullerenes. I. C60, C59N+, and C48N12: theory and experiment.

    PubMed

    Xie, Rui-Hua; Bryant, Garnett W; Sun, Guangyu; Nicklaus, Marc C; Heringer, David; Frauenheim, Th; Manaa, M Riad; Smith, Vedene H; Araki, Yasuyuki; Ito, Osamu

    2004-03-15

    Low-energy excitations and optical absorption spectrum of C(60) are computed by using time-dependent (TD) Hartree-Fock, TD-density functional theory (TD-DFT), TD DFT-based tight-binding (TD-DFT-TB), and a semiempirical Zerner intermediate neglect of diatomic differential overlap method. A detailed comparison of experiment and theory for the excitation energies, optical gap, and absorption spectrum of C(60) is presented. It is found that electron correlations and correlation of excitations play important roles in accurately assigning the spectral features of C(60), and that the TD-DFT method with nonhybrid functionals or a local spin density approximation leads to more accurate excitation energies than with hybrid functionals. The level of agreement between theory and experiment for C(60) justifies similar calculations of the excitations and optical absorption spectrum of a monomeric azafullerene cation C(59)N(+), to serve as a spectroscopy reference for the characterization of carborane anion salts. Although it is an isoelectronic analogue to C(60), C(59)N(+) exhibits distinguishing spectral features different from C(60): (1) the first singlet is dipole-allowed and the optical gap is redshifted by 1.44 eV; (2) several weaker absorption maxima occur in the visible region; (3) the transient triplet-triplet absorption at 1.60 eV (775 nm) is much broader and the decay of the triplet state is much faster. The calculated spectra of C(59)N(+) characterize and explain well the measured ultraviolet-visible (UV-vis) and transient absorption spectra of the carborane anion salt [C(59)N][Ag(CB(11)H(6)Cl(6))(2)] [Kim et al., J. Am. Chem. Soc. 125, 4024 (2003)]. For the most stable isomer of C(48)N(12), we predict that the first singlet is dipole-allowed, the optical gap is redshifted by 1.22 eV relative to that of C(60), and optical absorption maxima occur at 585, 528, 443, 363, 340, 314, and 303 nm. We point out that the characterization of the UV-vis and transient absorption

  14. Optically controlled dense current structures driven by relativistic plasma aperture-induced diffraction

    NASA Astrophysics Data System (ADS)

    Gonzalez-Izquierdo, Bruno; Gray, Ross J.; King, Martin; Dance, Rachel J.; Wilson, Robbie; McCreadie, John; Butler, Nicholas M. H.; Capdessus, Remi; Hawkes, Steve; Green, James S.; Borghesi, Marco; Neely, David; McKenna, Paul

    2016-05-01

    The collective response of charged particles to intense fields is intrinsic to plasma accelerators and radiation sources, relativistic optics and many astrophysical phenomena. Here we show that a relativistic plasma aperture is generated in thin foils by intense laser light, resulting in the fundamental optical process of diffraction. The plasma electrons collectively respond to the resulting laser near-field diffraction pattern, producing a beam of energetic electrons with a spatial structure that can be controlled by variation of the laser pulse parameters. It is shown that static electron-beam and induced-magnetic-field structures can be made to rotate at fixed or variable angular frequencies depending on the degree of ellipticity in the laser polarization. The concept is demonstrated numerically and verified experimentally, and is an important step towards optical control of charged particle dynamics in laser-driven dense plasma sources.

  15. Absorption of light by excitons and trions in monolayers of metal dichalcogenide MoS2: Experiments and theory

    NASA Astrophysics Data System (ADS)

    Zhang, Changjian; Wang, Haining; Chan, Weimin; Manolatou, Christina; Rana, Farhan

    2014-05-01

    We measure the optical-absorption spectra and optical conductivities of excitons and trions in monolayers of metal dichalcogenide MoS2 and compare the results with theoretical models. Our results show that the Wannier-Mott model for excitons with modifications to account for small exciton radii and large exciton relative wave function spread in momentum space, phase space blocking due to Pauli exclusion in doped materials, and wave-vector-dependent dielectric constant gives results that agree well with experiments. The measured exciton optical-absorption spectra are used to obtain experimental estimates for the exciton radii that fall in the 7-10Å range and agree well with theory. The measured trion optical-absorption spectra are used to obtain values for the trion radii that also agree well with theory. The measured values of the exciton and trion radii correspond to binding energies that are in good agreement with values obtained from first-principles calculations.

  16. Optical study of a doubly negatively charged exciton in a CdTe/ZnTe quantum dot containing a single Mn+2 ion

    NASA Astrophysics Data System (ADS)

    Smoleński, T.; Koperski, M.; Goryca, M.; Wojnar, P.; Kossacki, P.; Kazimierczuk, T.

    2015-08-01

    We present a magnetospectroscopic study of a doubly negatively charged exciton X2 - in a CdTe quantum dot doped with a single Mn+2 ion. The X2 - emission leading to the singlet final state of an excited electron pair is demonstrated to consist of six distinct lines corresponding to different projections of the Mn+2 spin, similarly as for the neutral exciton X . We show that the fine structure of X2 - energy levels, as well as the effects of the longitudinal magnetic field, are well reproduced by a simple spin Hamiltonian model featuring both carrier-ion and intershell electron-hole exchange interactions. We also point out two important effects distinguishing the X2 - from the X , which result from different symmetries of the electron wave function: the field-induced decrease of the anisotropic part of intershell electron-hole exchange, and the negligible value of the Mn+2 exchange integral with the p -shell electron.

  17. Dynamic Simulation of Trapping and Controlled Rotation of a Microscale Rod Driven by Line Optical Tweezers

    NASA Astrophysics Data System (ADS)

    Haghshenas-Jaryani, Mahdi; Bowling, Alan; Mohanty, Samarendra

    2013-03-01

    Since the invention of optical tweezers, several biological and engineering applications, especially in micro-nanofluid, have been developed. For example, development of optically driven micromotors, which has an important role in microfluidic applications, has vastly been considered. Despite extensive experimental studies in this field, there is a lack of theoretical work that can verify and analyze these observations. This work develops a dynamic model to simulate trapping and controlled rotation of a microscale rod under influence of the optical trapping forces. The laser beam, used in line optical tweezers with a varying trap's length, was modeled based on a ray-optics approach. Herein, the effects of viscosity of the surrounding fluid (water), gravity, and buoyancy were included in the proposed model. The predicted results are in overall agreement with the experimental observation, which make the theoretical model be a viable tool for investigating the dynamic behavior of small size objects manipulated by optical tweezers in fluid environments. This material is based upon work supported by the National Science Foundation under Grant No. MCB-1148541.

  18. Exciton Transfer in Carbon Nanotube Aggregates for Energy Harvesting Applications

    NASA Astrophysics Data System (ADS)

    Davoody, Amirhossein; Karimi, Farhad; Knezevic, Irena

    Carbon nanotubes (CNTs) are promising building blocks for organic photovoltaic devices, owing to their tunable band gap, mechanical and chemical stability. We study intertube excitonic energy transfer between pairs of CNTs with different orientations and band gaps. The optically bright and dark excitonic states in CNTs are calculated by solving the Bethe-Salpeter equation. We calculate the exciton transfer rates due to the direct and exchange Coulomb interactions, as well as the second-order phonon-assisted processes. We show the importance of phonons in calculating the transfer rates that match the measurements. In addition, we discuss the contribution of optically inactive excited states in the exciton transfer process, which is difficult to determine experimentally. Furthermore, we study the effects of sample inhomogeneity, impurities, and temperature on the exciton transfer rate. The inhomogeneity in the CNT sample dielectric function can increase the transfer rate by about a factor of two. We show that the exciton confinement by impurities has a detrimental effect on the transfer rate between pairs of similar CNTs. The exciton transfer rate increases monotonically with increasing temperature. Support by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under Award DE-SC0008712.

  19. Controlling the dark exciton spin eigenstates by external magnetic field

    NASA Astrophysics Data System (ADS)

    Gantz, L.; Schmidgall, E. R.; Schwartz, I.; Don, Y.; Waks, E.; Bahir, G.; Gershoni, D.

    2016-07-01

    We study the dark exciton's behavior as a coherent physical two-level spin system (qubit) using an external magnetic field in the Faraday configuration. Our studies are based on polarization-sensitive intensity autocorrelation measurements of the optical transition resulting from the recombination of a spin-blockaded biexciton state, which heralds the dark exciton and its spin state. We demonstrate control over the dark exciton eigenstates without degrading its decoherence time. Our observations agree well with computational predictions based on a master equation model.

  20. Confocal shift interferometry of coherent emission from trapped dipolar excitons

    SciTech Connect

    Repp, J.; Schinner, G. J.; Schubert, E.; Rai, A. K.; Wieck, A. D.; Reuter, D.; Wurstbauer, U.; Holleitner, A. W.; and others

    2014-12-15

    We introduce a confocal shift-interferometer based on optical fibers. The presented spectroscopy allows measuring coherence maps of luminescent samples with a high spatial resolution even at cryogenic temperatures. We apply the spectroscopy onto electrostatically trapped, dipolar excitons in a semiconductor double quantum well. We find that the measured spatial coherence length of the excitonic emission coincides with the point spread function of the confocal setup. The results are consistent with a temporal coherence of the excitonic emission down to temperatures of 250 mK.

  1. Electrical Activation of Dark Excitonic States in Carbon Nanotubes

    NASA Astrophysics Data System (ADS)

    Uda, Takushi; Yoshida, Masahiro; Ishii, Akihiro; Kato, Yuichiro K.

    Electrical activation of optical transitions to parity-forbidden dark excitonic states in individual carbon nanotubes is reported. We examine electric field effects on various excitonic states by simultaneously measuring both photocurrent and photoluminescence. As the applied field increases, we observe an emergence of new absorption peaks in the excitation spectra. From the diameter dependence of the energy separation between the new peaks and the ground state of E11 excitons, we attribute the peaks to the dark excited states which became optically active due to the applied field. A simple field-induced exciton dissociation model is introduced to explain the photocurrent threshold fields, and the edge of the E11 continuum states have been identified using this model. Work supported by JSPS (KAKENHI 24340066, 26610080), MEXT (Photon Frontier Network Program, Nanotechnology Platform), Canon Foundation, and Asahi Glass Foundation.

  2. Miniaturized magnetic-driven scanning probe for endoscopic optical coherence tomography.

    PubMed

    Pang, Ziwei; Wu, Jigang

    2015-06-01

    We designed and implemented a magnetic-driven scanning (MDS) probe for endoscopic optical coherence tomography (OCT). The probe uses an externally-driven tiny magnet in the distal end to achieve unobstructed 360-degree circumferential scanning at the side of the probe. The design simplifies the scanning part inside the probe and thus allows for easy miniaturization and cost reduction. We made a prototype probe with an outer diameter of 1.4 mm and demonstrated its capability by acquiring OCT images of ex vivo trachea and artery samples from a pigeon. We used a spectrometer-based Fourier-domain OCT system and the system sensitivity with our prototype probe was measured to be 91 dB with an illumination power of 850 μW and A-scan exposure time of 1 ms. The axial and lateral resolutions of the system are 6.5 μm and 8.1 μm, respectively. PMID:26114041

  3. Anomalous magnetization of a carbon nanotube as an excitonic insulator

    NASA Astrophysics Data System (ADS)

    Rontani, Massimo

    2014-11-01

    We show theoretically that an undoped carbon nanotube might be an excitonic insulator—the long-sought phase of matter proposed by Keldysh, Kohn, and others fifty years ago. We predict that the condensation of triplet excitons, driven by intervalley exchange interaction, spontaneously occurs at equilibrium if the tube radius is sufficiently small. The signatures of exciton condensation are its sizable contributions to both the energy gap and the magnetic moment per electron. The increase of the gap might have already been measured, albeit with a different explanation [V. V. Deshpande, B. Chandra, R. Caldwell, D. S. Novikov, J. Hone, and M. Bockrath, Science 323, 106 (2009), 10.1126/science.1165799]. The enhancement of the quasiparticle magnetic moment is a pair-breaking effect that counteracts the weak paramagnetism of the ground-state condensate of excitons. This property could rationalize the anomalous magnitude of magnetic moments recently observed in different devices close to charge neutrality.

  4. Using dark states for exciton storage in transition-metal dichalcogenides.

    PubMed

    Tseng, Frank; Simsek, Ergun; Gunlycke, Daniel

    2016-01-27

    We explore the possibility of storing excitons in excitonic dark states in monolayer semiconducting transition-metal dichalcogenides. In addition to being optically inactive, these dark states require the electron and hole to be spatially separated, thus inhibiting electron/hole recombination and allowing exciton lifetimes to be extended. Based on an atomistic exciton model, we derive transition matrix elements and an approximate selection rule showing that excitons could be transitioned into and out of dark states using a pulsed infrared laser. For illustration, we also present exciton population scenarios based on a population analysis for different recombination decay constants. Longer exciton lifetimes could make these materials candidates for applications in energy management and quantum information processing. PMID:26704568

  5. Radiative lifetimes of excitons and trions in monolayers of the metal dichalcogenide MoS2

    NASA Astrophysics Data System (ADS)

    Wang, Haining; Zhang, Changjian; Chan, Weimin; Manolatou, Christina; Tiwari, Sandip; Rana, Farhan

    2016-01-01

    We present results on the radiative lifetimes of excitons and trions in a monolayer of metal dichalcogenide MoS2. The small exciton radius and the large exciton optical oscillator strength result in radiative lifetimes in the 0.18-0.30 ps range for excitons that have small in-plane momenta and couple to radiation. Average lifetimes of thermally distributed excitons depend linearly on the exciton temperature and can be in the few picoseconds range at small temperatures and more than a nanosecond near room temperature. Localized excitons exhibit lifetimes in the same range and the lifetime increases as the localization length decreases. The radiative lifetimes of trions are in the hundreds of picosecond range and increase with the increase in the trion momentum. Average lifetimes of thermally distributed trions increase with the trion temperature as the trions acquire thermal energy and larger momenta. We expect our theoretical results to be applicable to most other 2D transition metal dichalcogenides.

  6. Optically driven Archimedes micro-screws for micropump applications: multiple blade design

    NASA Astrophysics Data System (ADS)

    Baldeck, Patrice L.; Lin, Chih-Lang; Lin, Yu-Sheng; Lin, Chin-Te; Chung, Tien-Tung; Bouriau, Michel; Vitrant, Guy

    2011-10-01

    We study the rotation of photo-driven Archimedes screw with multiple blades. The micron-sized Archimedes screws are readily made by the two-photon polymerization technique. Free-floating screws that are trapped by optical tweezers align in the laser irradiation direction, and rotate spontaneously. In this study we demonstrate that the rotation speeds of two-blade-screws is twice the rotation speed of one-blade-screw. However, more complex 3-blade-screws rotate slower than 2-blade-screws due to their limited geometry resolution at this micron scale.

  7. Non-adiabatic effects on the optical response of driven systems

    NASA Astrophysics Data System (ADS)

    Fregoso, Benjamin M.; Kolodrubetz, Michael; Moore, Joel

    Periodically driven systems have received renewed interest due to their capacity to engineer non-trivial effective Hamiltonians. A characteristic of such systems is how they respond to weak periodicity-breaking drive, as for example when a laser is pulsed instead of continuous wave. We develop semi-classical equations of motion of a wave packet in the presence of electric and magnetic fields which are turned on non-adiabatically. We then show the emergence of significant corrections to electronic collective excitations and optical responses of topological insulator surface states, Weyl metals and semiconductor mono-chalcogenides.

  8. Characterization of laser-driven shock waves in solids using a fiber optic pressure probe

    SciTech Connect

    Cranch, Geoffrey A.; Lunsford, Robert; Grun, Jacob; Weaver, James; Compton, Steve; May, Mark; Kostinski, Natalie

    2013-11-08

    Measurement of laser-driven shock wave pressure in solid blocks of polymethyl methacrylate is demonstrated using fiber optic pressure probes. Three probes based on a fiber Fabry–Perot, fiber Bragg grating, and interferometric fiber tip sensor are tested and compared. Shock waves are generated using a high-power laser focused onto a thin foil target placed in close proximity to the test blocks. The fiber Fabry–Perot sensor appears capable of resolving the shock front with a rise time of 91 ns. As a result, the peak pressure is estimated, using a separate shadowgraphy measurement, to be 3.4 GPa.

  9. Trapping and transport of indirect excitons in coupled quantum wells

    NASA Astrophysics Data System (ADS)

    Wuenschell, Jeffrey K.

    Spatially indirect excitons are optically generated composite bosons with a radiative lifetime sufficient to reach thermal equilibrium. This work explores the physics of indirect excitons in coupled quantum wells in the GaAs/AlGaAs system, specifically in the low-temperature, high-density regime. Particular attention is paid to a technique whereby a spatially inhomogeneous strain field is used as a trapping potential. In the process of modeling the trapping profile in wide quantum wells, dramatic effects due to intersubband coupling were observed at high strain. Experimentally, this regime coincides with the abrupt appearance of a dark population of indirect excitons at trap center, an effect originally suspected to be related to Bose-Einstein condensation. Here, the role of band mixing due to the strain-induced distortion of the crystal symmetry will be explored in detail in the context of this effect. Experimental studies presented here and in the literature suggest that Bose-Einstein condensation in indirect exciton systems may be difficult to detect with optical means (e.g., coherence measurements, momentum-space narrowing), possibly due to the strong dipole interaction between indirect excitons. Due to similarities between this system and liquid helium, it may be more fruitful to look for transport-related signatures of condensation, such as super fluidity. Here, a method for performing transport measurements on optically generated indirect excitons is also outlined and preliminary results are presented.

  10. High-Q silica zipper cavity for optical radiation pressure driven MOMS switch

    SciTech Connect

    Tetsumoto, Tomohiro; Tanabe, Takasumi

    2014-07-15

    We design a silica zipper cavity that has high optical and mechanical Q (quality factor) values and demonstrate numerically the feasibility of a radiation pressure driven micro opto-mechanical system (MOMS) directional switch. The silica zipper cavity has an optical Q of 4.0 × 10{sup 4} and an effective mode volume V{sub mode} of 0.67λ{sup 3} when the gap between two cavities is 34 nm. The mechanical Q (Q{sub m}) is determined by thermo-elastic damping and is 2.0 × 10{sup 6} in a vacuum at room temperature. The opto-mechanical coupling rate g{sub OM} is as high as 100 GHz/nm, which allows us to move the directional cavity-waveguide system and switch 1550-nm light with 770-nm light by controlling the radiation pressure.

  11. Development of dielectric elastomer driven micro-optical zoom lens system

    NASA Astrophysics Data System (ADS)

    Kim, Hyunseok; Park, Jongkil; Chuc, Nguyen Huu; Choi, H. R.; Nam, J. D.; Lee, Y.; Jung, H. S.; Koo, J. C.

    2007-04-01

    Normally, various micro-scale devices adopt electromechanical actuators for their basic mechanical functions. Those types of actuators require a complicated power transfer system even for generating a tiny scale motion. Since the mechanical power transfer system for the micro-scale motion may require many components, the system design to fit those components into a small space is always challenging. Micro-optical zoom lens systems are recently popularly used for many portable IT devices such as digital cameras, camcorder, and cell phones, Noting the advantages of EAP actuators over the conventional electromechanical counterparts in terms of simple actuator mechanisms, a micro-optic device that is driven with the EAP actuator is introduced in the present work. EAP material selection, device design and fabrication will be also delineated.

  12. Reflective optical probing of laser-driven plasmas at the rear surface of solid targets

    NASA Astrophysics Data System (ADS)

    Metzkes, J.; Zeil, K.; Kraft, S. D.; Rehwald, M.; Cowan, T. E.; Schramm, U.

    2016-03-01

    In this paper, a reflective optical pump-probe technique for laser-driven plasmas at solid density target surfaces is presented. The technique is termed high depth-of-field time-resolved microscopy and it exploits the angular redistribution of the probe beam intensity after the probe’s reflection from an expanded and hence non-planar iso-density surface in the plasma. The main application of the robust technique, which uses simple imaging of the probe beam, is the spatio-temporal resolution of the plasma formation and expansion at the target rear surface. Analytic and numerical modeling of the experimental setup are applied for the analysis of the experimental results. The relevance and potential of the optical plasma probing method is highlighted by the application to targets of different geometries, helping to understand the target shape-related differences in the ion acceleration performance.

  13. Optimization of torque on an optically driven micromotor by manipulation of the index of refraction

    NASA Astrophysics Data System (ADS)

    Wing, Frank M., III; Mahajan, Satish; Collett, Walter

    2004-12-01

    Since the 1970"s, the focused laser beam has become a familiar tool to manipulate neutral, dielectric micro-objects. A number of authors, including Higurashi and Gauthier, have described the effects of radiation pressure from laser light on microrotors. Collett, et al. developed a wave, rather than a ray optic, approach in the calculation of such forces on a microrotor for the first time. This paper describes a modification to the design of a laser driven, radiation pressure microrotor, intended to improve the optically generated torque. Employing the wave approach, the electric and magnetic fields in the vicinity of the rotor are calculated using the finite difference time domain (FDTD) method, which takes into account the wave nature of the incident light. Forces are calculated from the application of Maxwell"s stress tensor over the surfaces of the rotor. Results indicate a significant increase in torque when the index of refraction of the microrotor is changed from a single value to an inhomogeneous profile. The optical fiber industry has successfully employed a variation in the index of refraction across the cross section of a fiber for the purpose of increasing the efficiency of light transmission. Therefore, it is hoped that various fabrication methods can be utilized for causing desired changes in the index of refraction of an optically driven microrotor. Various profiles of the index of refraction inside a microrotor are considered for optimization of torque. Simulation methodology and results of torque on a microrotor for various profiles of the index of refraction are presented. Guidelines for improvised fabrication of efficient microrotors may then be obtained from these profiles.

  14. Coherent and Incoherent Coupling Dynamics between Neutral and Charged Excitons in Monolayer MoSe2.

    PubMed

    Hao, Kai; Xu, Lixiang; Nagler, Philipp; Singh, Akshay; Tran, Kha; Dass, Chandriker Kavir; Schüller, Christian; Korn, Tobias; Li, Xiaoqin; Moody, Galan

    2016-08-10

    The optical properties of semiconducting transition metal dichalcogenides are dominated by both neutral excitons (electron-hole pairs) and charged excitons (trions) that are stable even at room temperature. While trions directly influence charge transport properties in optoelectronic devices, excitons may be relevant through exciton-trion coupling and conversion phenomena. In this work, we reveal the coherent and incoherent nature of exciton-trion coupling and the relevant time scales in monolayer MoSe2 using optical two-dimensional coherent spectroscopy. Coherent interaction between excitons and trions is definitively identified as quantum beating of cross peaks in the spectra that persists for a few hundred femtoseconds. For longer times up to 10 ps, surprisingly, the relative intensity of the cross peaks increases, which is attributed to incoherent energy transfer likely due to phonon-assisted up-conversion and down-conversion processes that are efficient even at cryogenic temperature. PMID:27428509

  15. Coherent and Incoherent Coupling Dynamics between Neutral and Charged Excitons in Monolayer MoSe2

    NASA Astrophysics Data System (ADS)

    Hao, Kai; Xu, Lixiang; Nagler, Philipp; Singh, Akshay; Tran, Kha; Dass, Chandriker Kavir; Schüller, Christian; Korn, Tobias; Li, Xiaoqin; Moody, Galan

    2016-08-01

    The optical properties of semiconducting transition metal dichalcogenides are dominated by both neutral excitons (electron-hole pairs) and charged excitons (trions) that are stable even at room temperature. While trions directly influence charge transport properties in optoelectronic devices, excitons may be relevant through exciton-trion coupling and conversion phenomena. In this work, we reveal the coherent and incoherent nature of exciton-trion coupling and the relevant timescales in monolayer MoSe2 using optical two-dimensional coherent spectroscopy. Coherent interaction between excitons and trions is definitively identified as quantum beating of cross-coupling peaks that persists for a few hundred femtoseconds. For longer times up to 10 ps, surprisingly, the relative intensity of the cross-coupling peaks increases, which is attributed to incoherent energy transfer likely due to phonon-assisted up-conversion and down-conversion processes that are efficient even at cryogenic temperature.

  16. Bleaching in the region of exciton resonance of layered GaSe crystals

    NASA Astrophysics Data System (ADS)

    Kyazym-zade, A. G.; Salmanov, V. M.; Guseinov, A. G.; Salmanova, A. A.; Mamedov, R. M.; Dzhavadzade, A. A.

    2014-09-01

    Light absorption in the region of exciton resonance of GaSe crystal is studied experimentally at high levels of optical excitation. A picosecond YAG:Nd3+ laser emitting 30-ps light pulses and a dye laser with a pulse width of ˜3 ns tunable within the range 594-643 nm were used as light sources. It was found that, at high levels of optical excitation, the exciton absorption line of the GaSe crystal disappeared, which was attributed to increasing exciton density with arising mechanisms of their decay: exciton-exciton interactions and screening of excitons by the free charge-carrier plasma. It is shown that these mechanisms are also responsible for the arising new emission band in the long-wavelength region of the photoluminescence spectrum.

  17. Ab initio calculation of optical properties with excitonic effects in wurtzite InxGa1-xN and InxAl1-xN alloys

    NASA Astrophysics Data System (ADS)

    de Carvalho, Luiz Cláudio; Schleife, André; Furthmüller, Jürgen; Bechstedt, Friedhelm

    2013-05-01

    By combining modern many-body approaches with a cluster expansion scheme, frequency-dependent dielectric functions including excitonic and local-field effects are computed for wurtzitic group-III nitride alloys with varying composition x. The quasiparticle electronic structure required to construct the quasielectron-quasihole pair Hamiltonian for each cluster is approximated using a LDA+U+Δ approach. Two different cluster statistics are employed to perform configurational averages for the frequency-dependent complex dielectric functions. Comparing the resulting composition dependence of peak positions and intensities to experimental data allows conclusions regarding the distribution of the group-III cations in the alloys.

  18. Optical design of the Fresnel lens for LED-driven flashlight.

    PubMed

    Chen, Yi-Cheng; Nian, Shih-Chih; Huang, Ming-Shyan

    2016-02-01

    The Fresnel lens is composed of micrometer-sized v-groove structures that determine the maximum illuminance and brightness uniformity of LED-driven flashlights, which are used in high-quality photography. The fabrication quality of the microstructures and the accuracy of the geometrical curvature of the Fresnel lens affect the optical characteristics of the emitted light traveling through the lens, which in turn determines the maximum illuminance and brightness uniformity. This paper presents a systematic design procedure for fabricating the Fresnel lens and investigates the influence of geometrical design and fabrication process on optical performance. The optical analysis was performed using the commercial software TracePro. The results revealed that a small tip radius of the v-groove microstructure facilitates brightness uniformity. Furthermore, both the simulation and the experimental results revealed that Fresnel lenses fabricated through injection molding or injection compression molding have either errors of microstructure height more than 3%-6% or curvature errors higher than 6%, which would affect the optical performance, especially the brightness uniformity. PMID:26836072

  19. Geminate and Nongeminate Recombination of Triplet Excitons Formed by Singlet Fission

    NASA Astrophysics Data System (ADS)

    Bayliss, Sam L.; Chepelianskii, Alexei D.; Sepe, Alessandro; Walker, Brian J.; Ehrler, Bruno; Bruzek, Matthew J.; Anthony, John E.; Greenham, Neil C.

    2014-06-01

    We report the simultaneous observation of geminate and nongeminate triplet-triplet annihilation in a solution-processable small molecule TIPS-tetracene undergoing singlet exciton fission. Using optically detected magnetic resonance, we identify recombination of triplet pairs directly following singlet fission, as well as recombination of triplet excitons undergoing bimolecular triplet-triplet annihilation. We show that the two processes give rise to distinct magnetic resonance spectra, and estimate the interaction between geminate triplet excitons to be 60 neV.

  20. Optically driven oscillations of ellipsoidal particles. Part II: ray-optics calculations.

    PubMed

    Loudet, J-C; Mihiretie, B M; Pouligny, B

    2014-12-01

    We report numerical calculations on the mechanical effects of light on micrometer-sized dielectric ellipsoids immersed in water. We used a simple two-dimensional ray-optics model to compute the radiation pressure forces and torques exerted on the object as a function of position and orientation within the laser beam. Integration of the equations of motion, written in the Stokes limit, yields the particle dynamics that we investigated for different aspect ratios k. Whether the beam is collimated or focused, the results show that above a critical aspect ratio k(C), the ellipsoids cannot be stably trapped on the beam axis; the particle never comes to rest and rather oscillates permanently in a back-and-forth motion involving both translation and rotation in the vicinity of the beam. Such oscillations are a direct evidence of the non-conservative character of optical forces. Conversely, stable trapping can be achieved for k < k(C) with the particle standing idle in a vertical position. These predictions are in very good qualitative agreement with experimental observations. The physical origin of the instability may be understood from the force and torque fields whose structures greatly depend on the ellipsoid aspect ratio and beam diameter. The oscillations arise from a non-linear coupling of the forces and torques and the torque amplitude was identified as the bifurcation control parameter. Interestingly, simulations predict that sustained oscillations can be suppressed through the use of two coaxial counterpropagating beams, which may be of interest whenever a static equilibrium is required as in basic force and torque measurements or technological applications. PMID:25577403

  1. Control of Exciton Photon Coupling in Nano-structures

    NASA Astrophysics Data System (ADS)

    Liu, Xiaoze

    In this thesis, we study the interaction of excitons with photons and plasmons and methods to control and enhance this interaction. This study is categorized in three parts: light-matter interaction in microcavity structures, direct dipole-dipole interactions, and plasmon-exciton interaction in metal-semiconductor systems. In the microcavity structures, the light-matter interactions become significant when the excitonic energy is in resonance with microcavity photons. New hybrid quantum states named polariton states will be formed if the strong coupling regime is achieved, where the interaction rate is faster than the average decay rate of the excitons and photons. Polaritons have been investigated in zinc oxide (ZnO) nanoparticles based microcavity at room temperature and stimulated emission of the polaritons has also been observed with a low optical pump threshold. Exictons in organic semiconductors (modeled as Frenkel excitons) are tightly bound to molecular sites, and differ considerably from loosely bound hydrogen atom-like inorganic excitons (modeled as Wannier-Mott excitons). This fundamental difference results in distinct optoelectronic properties. Not only strongly coupled to Wannier-Mott excitons in ZnO, the microcavity photons have also been observed to be simultaneously coupled to Frenkel excitons in 3,4,7,8-naphthalene tetracarboxylic dianhydride (NTCDA). The photons here act like a glue combining Wannier-Mott and Frenkel excitons into new hybrid polaritons taking the best from both constituents. Two-dimensional (2D) excitons in monolayer transition metal dichalcogenides (TMDs) have emerged as a new and fascinating type of Wannier-Mott-like excitons due to direct bandgap transition, huge oscillator strength and large binding energy. Monolayer molybdenum disulfide (MoS2) has been incorporated into the microcavity structure and 2D exciton-polaritons have been observed for the first time with directional emission in the strong coupling regime. Valley

  2. Singlet exciton fission photovoltaics.

    PubMed

    Lee, Jiye; Jadhav, Priya; Reusswig, Philip D; Yost, Shane R; Thompson, Nicholas J; Congreve, Daniel N; Hontz, Eric; Van Voorhis, Troy; Baldo, Marc A

    2013-06-18

    Singlet exciton fission, a process that generates two excitons from a single photon, is perhaps the most efficient of the various multiexciton-generation processes studied to date, offering the potential to increase the efficiency of solar devices. But its unique characteristic, splitting a photogenerated singlet exciton into two dark triplet states, means that the empty absorption region between the singlet and triplet excitons must be filled by adding another material that captures low-energy photons. This has required the development of specialized device architectures. In this Account, we review work to develop devices that harness the theoretical benefits of singlet exciton fission. First, we discuss singlet fission in the archetypal material, pentacene. Pentacene-based photovoltaic devices typically show high external and internal quantum efficiencies. They have enabled researchers to characterize fission, including yield and the impact of competing loss processes, within functional devices. We review in situ probes of singlet fission that modulate the photocurrent using a magnetic field. We also summarize studies of the dissociation of triplet excitons into charge at the pentacene-buckyball (C60) donor-acceptor interface. Multiple independent measurements confirm that pentacene triplet excitons can dissociate at the C60 interface despite their relatively low energy. Because triplet excitons produced by singlet fission each have no more than half the energy of the original photoexcitation, they limit the potential open circuit voltage within a solar cell. Thus, if singlet fission is to increase the overall efficiency of a solar cell and not just double the photocurrent at the cost of halving the voltage, it is necessary to also harvest photons in the absorption gap between the singlet and triplet energies of the singlet fission material. We review two device architectures that attempt this using long-wavelength materials: a three-layer structure that uses

  3. Strong Quantum Coherence between Fermi Liquid Mahan Excitons

    NASA Astrophysics Data System (ADS)

    Paul, J.; Stevens, C. E.; Liu, C.; Dey, P.; McIntyre, C.; Turkowski, V.; Reno, J. L.; Hilton, D. J.; Karaiskaj, D.

    2016-04-01

    In modulation doped quantum wells, the excitons are formed as a result of the interactions of the charged holes with the electrons at the Fermi edge in the conduction band, leading to the so-called "Mahan excitons." The binding energy of Mahan excitons is expected to be greatly reduced and any quantum coherence destroyed as a result of the screening and electron-electron interactions. Surprisingly, we observe strong quantum coherence between the heavy hole and light hole excitons. Such correlations are revealed by the dominating cross-diagonal peaks in both one-quantum and two-quantum two-dimensional Fourier transform spectra. Theoretical simulations based on the optical Bloch equations where many-body effects are included phenomenologically reproduce well the experimental spectra. Time-dependent density functional theory calculations provide insight into the underlying physics and attribute the observed strong quantum coherence to a significantly reduced screening length and collective excitations of the many-electron system.

  4. Analysis methodology for a piezoelectric-driven optical tracker for ground-based interferometry

    NASA Astrophysics Data System (ADS)

    Clark, James H.; Penado, F. Ernesto

    2014-09-01

    We present our analysis methodology for a 20.3 cm prototype optical tracker to determine why instabilities occur below 50 Hz and suggest improvements. The Navy Precision Optical Interferometer makes use of six small optical telescope stations spaced along a Y-array to synthesize an equivalent single larger telescope. Piezoelectric-driven optical trackers steer 12.5 cm output beams from each station to an optics laboratory up to 700 m distant. A percentage of this starlight is split off and used in a closed-loop feedback to update the pointing of the telescope and steering of the tracker. Steering stabilizes atmospheric induced beam trajectory deviations, required for fringe generation. Because of closedloop feedback, we require all fundamental frequencies to be at least 3 times the desired operational frequency, or 150 Hz. These trackers are modified commercial aluminum gimbal mounts with flex-pivot axles and very small damping ratio. Steering is tip/tilt mirror rotation by push-only actuators and a return spring. It is critical contact be maintained between actuator, mirror mount and return spring. From our dynamic analysis, the 122 N return spring is 2.9 times that required, and has a natural frequency equal to 238 Hz. The range of steering, 140 microradian, is double that required and the 0.077 microradian precision is 2.6 times that required. The natural frequency of the tracker is 66 Hz and the tuned closed-loop operational frequency is only 22 Hz. We conclude the low fundamental frequency of the mount limits its performance below 50 Hz and stiffening the structure is required.

  5. Data-driven approach to optimum wavelength selection for diffuse optical imaging

    NASA Astrophysics Data System (ADS)

    Dempsey, Laura A.; Cooper, Robert J.; Roque, Tania; Correia, Teresa; Magee, Elliott; Powell, Samuel; Gibson, Adam P.; Hebden, Jeremy C.

    2015-01-01

    The production of accurate and independent images of the changes in concentration of oxyhemoglobin and deoxyhemoglobin by diffuse optical imaging is heavily dependent on which wavelengths of near-infrared light are chosen to interrogate the target tissue. Although wavelengths can be selected by theoretical methods, in practice the accuracy of reconstructed images will be affected by wavelength-specific and system-specific factors such as laser source power and detector sensitivity. We describe the application of a data-driven approach to optimum wavelength selection for the second generation of University College London's multichannel, time-domain optical tomography system (MONSTIR II). By performing a functional activation experiment using 12 different wavelengths between 690 and 870 nm, we were able to identify the combinations of 2, 3, and 4 wavelengths which most accurately reproduced the results obtained using all 12 wavelengths via an imaging approach. Our results show that the set of 2, 3, and 4 wavelengths which produce the most accurate images of functional activation are [770, 810], [770, 790, 850], and [730, 770, 810, 850] respectively, but also that the system is relatively robust to wavelength selection within certain limits. Although these results are specific to MONSTIR II, the approach we developed can be applied to other multispectral near-infrared spectroscopy and optical imaging systems.

  6. Excitonic effects in oxyhalide scintillating host compounds

    SciTech Connect

    Shwetha, G.; Kanchana, V.; Valsakumar, M. C.

    2014-10-07

    Ab-initio calculations based on density functional theory have been performed to study the electronic, optical, mechanical, and vibrational properties of scintillator host compounds YOX (X = F, Cl, Br, and I). Semiempirical dispersion correction schemes are used to find the effect of van der Waals forces on these layered compounds and we found this effect to be negligible except for YOBr. Calculations of phonons and elastic constants showed that all the compounds studied here are both dynamically and mechanically stable. YOF and YOI are found to be indirect band gap insulators while YOCl and YOBr are direct band gap insulators. The band gap is found to decrease as we move from fluorine to iodine, while the calculated refractive index shows the opposite trend. As the band gap decreases on going down the periodic table from YOF to YOI, the luminescence increases. The excitonic binding energy calculated, within the effective mass approximation, is found to be more for YOF than the remaining compounds, suggesting that the excitonic effect to be more in YOF than the other compounds. The optical properties are calculated within the Time-Dependent Density Functional Theory (TDDFT) and compared with results obtained within the random phase approximation. The TDDFT calculations, using the newly developed bootstrap exchange-correlation kernel, showed significant excitonic effects in all the compounds studied here.

  7. Coherent coupling of excitons and trions in a photoexcited CdTe/CdMgTe quantum well.

    PubMed

    Moody, G; Akimov, I A; Li, H; Singh, R; Yakovlev, D R; Karczewski, G; Wiater, M; Wojtowicz, T; Bayer, M; Cundiff, S T

    2014-03-01

    We present zero-, one-, and two-quantum two-dimensional coherent spectra of excitons and trions in a CdTe/(Cd,Mg)Te quantum well. The set of spectra provides a unique and comprehensive picture of the coherent nonlinear optical response. Distinct peaks in the spectra are manifestations of exciton-exciton and exciton-trion coherent coupling. Excellent agreement using density matrix calculations highlights the essential role of many-body effects on the coupling. Strong exciton-trion coherent interactions open up the possibility for novel conditional control schemes in coherent optoelectronics. PMID:24655274

  8. Coherent Coupling of Excitons and Trions in a Photoexcited CdTe/CdMgTe Quantum Well

    NASA Astrophysics Data System (ADS)

    Moody, G.; Akimov, I. A.; Li, H.; Singh, R.; Yakovlev, D. R.; Karczewski, G.; Wiater, M.; Wojtowicz, T.; Bayer, M.; Cundiff, S. T.

    2014-03-01

    We present zero-, one-, and two-quantum two-dimensional coherent spectra of excitons and trions in a CdTe/(Cd,Mg)Te quantum well. The set of spectra provides a unique and comprehensive picture of the coherent nonlinear optical response. Distinct peaks in the spectra are manifestations of exciton-exciton and exciton-trion coherent coupling. Excellent agreement using density matrix calculations highlights the essential role of many-body effects on the coupling. Strong exciton-trion coherent interactions open up the possibility for novel conditional control schemes in coherent optoelectronics.

  9. Photocurrent, photoluminescence and exciton dynamics in rubrene molecular single crystals

    NASA Astrophysics Data System (ADS)

    Lyu, ByungGook

    This work discusses the photocurrent and photoluminescence that can be induced by short-pulse illumination in rubrene single crystals. The pulsed illumination excites a rubrene molecule from the ground state to its first optically accessible excited state, resulting in a singlet exciton state. In rubrene, a singlet exciton can transform into two triplet excitons - which together have a spin of zero - by an efficient spin-conserved fission process. On the other hand, two triplet excitons can interact to again form a singlet exciton by a fusion process. Quantitative modeling of the transformation of singlet excitons into triplet excitons and vice-versa shows that both photoconductivity dynamics and photocurrent dynamics after pulsed excitations can be understood within the same framework. The photoluminescence observed after pulsed excitation is only emitted upon radiative recombination of singlet excitons. A simple model of fission and fusion based on rate equations leads to a qualitatively different photoluminescence dynamics depending on the time scale. In particular, it predicts a fast exponential decay corresponding to the initial fission process, later a power-law (quadratic) decay corresponding to a regime when triplet-triplet interaction is dominant, and a final exponential decay with a time-constant which is half the triplet exciton lifetime. This last exponential decay corresponds to the case when only a lower density of triplet excitons is left. The same model can be used to predict the photocurrent dynamics after pulsed excitation. Experimental observations after pulsed illumination show that, for low excitation pulse energies, a large photocurrent grows exponentially with a time constant of the order of 100 microseconds. This photocurrent build-up time then becomes shorter at higher excitation energies, with the peak photocurrent also saturating. One finds that the observed photocurrent dynamics can be reproduced with the same model based on exciton

  10. High-Performance Genetically Targetable Optical Neural Silencing via Light-Driven Proton Pumps

    PubMed Central

    Chow, Brian Y.; Han, Xue; Dobry, Allison S.; Qian, Xiaofeng; Chuong, Amy S.; Li, Mingjie; Henninger, Michael A.; Belfort, Gabriel M.; Lin, Yingxi; Monahan, Patrick E.; Boyden, Edward S.

    2009-01-01

    The ability to silence the activity of genetically specified neurons in a temporally precise fashion would open up the ability to investigate the causal role of specific cell classes in neural computations, behaviors, and pathologies. Here we show that members of the class of light-driven outward proton pumps can mediate very powerful, safe, multiple-color silencing of neural activity. The gene archaerhodopsin-31 (Arch) from Halorubrum sodomense enables near-100% silencing of neurons in the awake brain when virally expressed in mouse cortex and illuminated with yellow light. Arch mediates currents of several hundred picoamps at low light powers, and supports neural silencing currents approaching 900 pA at light powers easily achievable in vivo. In addition, Arch spontaneously recovers from light-dependent inactivation, unlike light-driven chloride pumps that enter long-lasting inactive states in response to light. These properties of Arch are appropriate to mediate the optical silencing of significant brain volumes over behaviourally-relevant timescales. Arch function in neurons is well tolerated because pH excursions created by Arch illumination are minimized by self-limiting mechanisms to levels comparable to those mediated by channelrhodopsins2,3 or natural spike firing. To highlight how proton pump ecological and genomic diversity may support new innovation, we show that the blue-green light-drivable proton pump from the fungus Leptosphaeria maculans4 (Mac) can, when expressed in neurons, enable neural silencing by blue light, thus enabling alongside other developed reagents the potential for independent silencing of two neural populations by blue vs. red light. Light-driven proton pumps thus represent a high-performance and extremely versatile class of “optogenetic” voltage and ion modulator, which will broadly empower new neuroscientific, biological, neurological, and psychiatric investigations. PMID:20054397

  11. Effect of the Pauli exclusion principle on the singlet exciton yield in conjugated polymers

    NASA Astrophysics Data System (ADS)

    Thilagam, A.

    2016-03-01

    Optical devices fabricated using conjugated polymer systems give rise to singlet exciton yields which are high compared to the statistically predicted estimate of 25 % obtained using simple recombination schemes. In this study, we evaluate the singlet exciton yield in conjugated polymers systems by fitting to a model that incorporates the Pauli exclusion principle. The rate equations which describe the exciton dynamics include quantum dynamical components (both density and spin-dependent) which arise during the spin-allowed conversion of composite intra-molecular excitons into loosely bound charge-transfer (CT) electron-hole pairs. Accordingly, a crucial mechanism by which singlet excitons are increased at the expense of triplet excitons is incorporated in this work. Non-ideal triplet excitons which form at high densities, are rerouted via the Pauli exclusion mechanism to form loosely bound CT states which subsequently convert to singlet excitons. Our derived expression for the yield in singlet exciton incorporates the purity measure and provides a realistic description of the carrier dynamics at high exciton densities.

  12. Spatially Resolved Thermodynamics of the Partially Ionized Exciton Gas in GaAs.

    PubMed

    Bieker, S; Henn, T; Kiessling, T; Ossau, W; Molenkamp, L W

    2015-06-01

    We report on the observation of macroscopic free exciton photoluminescence (PL) rings that appear in spatially resolved PL images obtained on a high purity GaAs sample. We demonstrate that a spatial temperature gradient in the photocarrier system, which is due to nonresonant optical excitation, locally modifies the population balance between free excitons and the uncorrelated electron-hole plasma described by the Saha equation and accounts for the experimentally observed nontrivial PL profiles. The exciton ring formation is a particularly instructive manifestation of the spatially dependent thermodynamics of a partially ionized exciton gas in a bulk semiconductor. PMID:26196644

  13. Spatially Resolved Thermodynamics of the Partially Ionized Exciton Gas in GaAs

    NASA Astrophysics Data System (ADS)

    Bieker, S.; Henn, T.; Kiessling, T.; Ossau, W.; Molenkamp, L. W.

    2015-06-01

    We report on the observation of macroscopic free exciton photoluminescence (PL) rings that appear in spatially resolved PL images obtained on a high purity GaAs sample. We demonstrate that a spatial temperature gradient in the photocarrier system, which is due to nonresonant optical excitation, locally modifies the population balance between free excitons and the uncorrelated electron-hole plasma described by the Saha equation and accounts for the experimentally observed nontrivial PL profiles. The exciton ring formation is a particularly instructive manifestation of the spatially dependent thermodynamics of a partially ionized exciton gas in a bulk semiconductor.

  14. Excitons in asymmetric quantum wells

    NASA Astrophysics Data System (ADS)

    Grigoryev, P. S.; Kurdyubov, A. S.; Kuznetsova, M. S.; Ignatiev, I. V.; Efimov, Yu. P.; Eliseev, S. A.; Petrov, V. V.; Lovtcius, V. A.; Shapochkin, P. Yu.

    2016-09-01

    Resonance dielectric response of excitons is studied for the high-quality InGaAs/GaAs heterostructures with wide asymmetric quantum wells (QWs). To highlight effects of the QW asymmetry, we have grown and studied several heterostructures with nominally square QWs as well as with triangle-like QWs. Several quantum confined exciton states are experimentally observed as narrow exciton resonances. A standard approach for the phenomenological analysis of the profiles is generalized by introducing different phase shifts for the light waves reflected from the QWs at different exciton resonances. Good agreement of the phenomenological fit to the experimentally observed exciton spectra for high-quality structures allowed us to reliably obtain parameters of the exciton resonances: the exciton transition energies, the radiative broadenings, and the phase shifts. A direct numerical solution of the Schrödinger equation for the heavy-hole excitons in asymmetric QWs is used for microscopic modeling of the exciton resonances. Remarkable agreement with the experiment is achieved when the effect of indium segregation is taken into account. The segregation results in a modification of the potential profile, in particular, in an asymmetry of the nominally square QWs.

  15. Towards optical polarization control of laser-driven proton acceleration in foils undergoing relativistic transparency.

    PubMed

    Gonzalez-Izquierdo, Bruno; King, Martin; Gray, Ross J; Wilson, Robbie; Dance, Rachel J; Powell, Haydn; Maclellan, David A; McCreadie, John; Butler, Nicholas M H; Hawkes, Steve; Green, James S; Murphy, Chris D; Stockhausen, Luca C; Carroll, David C; Booth, Nicola; Scott, Graeme G; Borghesi, Marco; Neely, David; McKenna, Paul

    2016-01-01

    Control of the collective response of plasma particles to intense laser light is intrinsic to relativistic optics, the development of compact laser-driven particle and radiation sources, as well as investigations of some laboratory astrophysics phenomena. We recently demonstrated that a relativistic plasma aperture produced in an ultra-thin foil at the focus of intense laser radiation can induce diffraction, enabling polarization-based control of the collective motion of plasma electrons. Here we show that under these conditions the electron dynamics are mapped into the beam of protons accelerated via strong charge-separation-induced electrostatic fields. It is demonstrated experimentally and numerically via 3D particle-in-cell simulations that the degree of ellipticity of the laser polarization strongly influences the spatial-intensity distribution of the beam of multi-MeV protons. The influence on both sheath-accelerated and radiation pressure-accelerated protons is investigated. This approach opens up a potential new route to control laser-driven ion sources. PMID:27624920

  16. Giant optical enhancement of strain gradient in ferroelectric BiFeO3 thin films and its physical origin.

    PubMed

    Li, Yuelin; Adamo, Carolina; Chen, Pice; Evans, Paul G; Nakhmanson, Serge M; Parker, William; Rowland, Clare E; Schaller, Richard D; Schlom, Darrell G; Walko, Donald A; Wen, Haidan; Zhang, Qingteng

    2015-01-01

    Through mapping of the spatiotemporal strain profile in ferroelectric BiFeO3 epitaxial thin films, we report an optically initiated dynamic enhancement of the strain gradient of 10(5)-10(6) m(-1) that lasts up to a few ns depending on the film thickness. Correlating with transient optical absorption measurements, the enhancement of the strain gradient is attributed to a piezoelectric effect driven by a transient screening field mediated by excitons. These findings not only demonstrate a new possible way of controlling the flexoelectric effect, but also reveal the important role of exciton dynamics in photostriction and photovoltaic effects in ferroelectrics. PMID:26586421

  17. Giant optical enhancement of strain gradient in ferroelectric BiFeO3 thin films and its physical origin

    DOE PAGESBeta

    Li, Yuelin; Adamo, C.; Chen, Pice; Evans, Paul G.; Nakhmanson, Serge M.; Parker, William; Rowland, Clare E.; Schaller, Richard D.; Schlom, Darrell G.; Walko, Donald A.; et al

    2015-11-20

    Through mapping of the spatiotemporal strain profile in ferroelectric BiFeO3 epitaxial thin films, we report an optically initiated dynamic enhancement of the strain gradient of 105–106 m-1 that lasts up to a few ns depending on the film thickness. Correlating with transient optical absorption measurements, the enhancement of the strain gradient is attributed to a piezoelectric effect driven by a transient screening field mediated by excitons. In conclusion, these findings not only demonstrate a new possible way of controlling the flexoelectric effect, but also reveal the important role of exciton dynamics in photostriction and photovoltaic effects in ferroelectrics.

  18. Giant optical enhancement of strain gradient in ferroelectric BiFeO3 thin films and its physical origin

    PubMed Central

    Li, Yuelin; Adamo, Carolina; Chen, Pice; Evans, Paul G.; Nakhmanson, Serge M.; Parker, William; Rowland, Clare E.; Schaller, Richard D.; Schlom, Darrell G.; Walko, Donald A.; Wen, Haidan; Zhang, Qingteng

    2015-01-01

    Through mapping of the spatiotemporal strain profile in ferroelectric BiFeO3 epitaxial thin films, we report an optically initiated dynamic enhancement of the strain gradient of 105–106 m−1 that lasts up to a few ns depending on the film thickness. Correlating with transient optical absorption measurements, the enhancement of the strain gradient is attributed to a piezoelectric effect driven by a transient screening field mediated by excitons. These findings not only demonstrate a new possible way of controlling the flexoelectric effect, but also reveal the important role of exciton dynamics in photostriction and photovoltaic effects in ferroelectrics. PMID:26586421

  19. Control of excitons in multi-layer van der Waals heterostructures

    NASA Astrophysics Data System (ADS)

    Calman, E. V.; Dorow, C. J.; Fogler, M. M.; Butov, L. V.; Hu, S.; Mishchenko, A.; Geim, A. K.

    2016-03-01

    We report an experimental study of excitons in a double quantum well van der Waals heterostructure made of atomically thin layers of MoS2 and hexagonal boron nitride. The emission of neutral and charged excitons is controlled by gate voltage, temperature, and both the helicity and the power of optical excitation.

  20. Many-body effects and excitonic features in 2D biphenylene carbon.

    PubMed

    Lüder, Johann; Puglia, Carla; Ottosson, Henrik; Eriksson, Olle; Sanyal, Biplab; Brena, Barbara

    2016-01-14

    The remarkable excitonic effects in low dimensional materials in connection to large binding energies of excitons are of great importance for research and technological applications such as in solar energy and quantum information processing as well as for fundamental investigations. In this study, the unique electronic and excitonic properties of the two dimensional carbon network biphenylene carbon were investigated with GW approach and the Bethe-Salpeter equation accounting for electron correlation effects and electron-hole interactions, respectively. Biphenylene carbon exhibits characteristic features including bright and dark excitons populating the optical gap of 0.52 eV and exciton binding energies of 530 meV as well as a technologically relevant intrinsic band gap of 1.05 eV. Biphenylene carbon's excitonic features, possibly tuned, suggest possible applications in the field of solar energy and quantum information technology in the future. PMID:26772582

  1. Valley-polarized exciton dynamics in a 2D semiconductor heterostructure

    NASA Astrophysics Data System (ADS)

    Rivera, Pasqual; Seyler, Kyle L.; Yu, Hongyi; Schaibley, John R.; Yan, Jiaqiang; Mandrus, David G.; Yao, Wang; Xu, Xiaodong

    2016-02-01

    Heterostructures comprising different monolayer semiconductors provide an attractive setting for fundamental science and device technologies, such as in the emerging field of valleytronics. We realized valley-specific interlayer excitons in monolayer WSe2-MoSe2 vertical heterostructures. We created interlayer exciton spin-valley polarization by means of circularly polarized optical pumping and determined a valley lifetime of 40 nanoseconds. This long-lived polarization enables the visualization of the expansion of a valley-polarized exciton cloud over several micrometers. The spatial pattern of the polarization evolves into a ring with increasing exciton density, a manifestation of valley exciton exchange interactions. Our work introduces van der Waals heterostructures as a promising platform from which to study valley exciton physics.

  2. Many-body effects and excitonic features in 2D biphenylene carbon

    NASA Astrophysics Data System (ADS)

    Lüder, Johann; Puglia, Carla; Ottosson, Henrik; Eriksson, Olle; Sanyal, Biplab; Brena, Barbara

    2016-01-01

    The remarkable excitonic effects in low dimensional materials in connection to large binding energies of excitons are of great importance for research and technological applications such as in solar energy and quantum information processing as well as for fundamental investigations. In this study, the unique electronic and excitonic properties of the two dimensional carbon network biphenylene carbon were investigated with GW approach and the Bethe-Salpeter equation accounting for electron correlation effects and electron-hole interactions, respectively. Biphenylene carbon exhibits characteristic features including bright and dark excitons populating the optical gap of 0.52 eV and exciton binding energies of 530 meV as well as a technologically relevant intrinsic band gap of 1.05 eV. Biphenylene carbon's excitonic features, possibly tuned, suggest possible applications in the field of solar energy and quantum information technology in the future.

  3. Valley-polarized exciton dynamics in a 2D semiconductor heterostructure.

    PubMed

    Rivera, Pasqual; Seyler, Kyle L; Yu, Hongyi; Schaibley, John R; Yan, Jiaqiang; Mandrus, David G; Yao, Wang; Xu, Xiaodong

    2016-02-12

    Heterostructures comprising different monolayer semiconductors provide an attractive setting for fundamental science and device technologies, such as in the emerging field of valleytronics. We realized valley-specific interlayer excitons in monolayer WSe2-MoSe2 vertical heterostructures. We created interlayer exciton spin-valley polarization by means of circularly polarized optical pumping and determined a valley lifetime of 40 nanoseconds. This long-lived polarization enables the visualization of the expansion of a valley-polarized exciton cloud over several micrometers. The spatial pattern of the polarization evolves into a ring with increasing exciton density, a manifestation of valley exciton exchange interactions. Our work introduces van der Waals heterostructures as a promising platform from which to study valley exciton physics. PMID:26912854

  4. Evidence of Hybrid Excitons in Weakly Interacting Nanopeapods

    PubMed Central

    2013-01-01

    Nanopeapods, consisting of optically active π-conjugated molecules encapsulated inside of the cavity of carbon nanotubes, exhibit efficient photon emission in the visible spectral range. Combining optical experiments with ab initio theory, we show that the puzzling features observed in photoluminescence spectra are of excitonic nature. The subunits though being van der Waals bound are demonstrated to interact in the excited state, giving rise to the formation of hybrid excitons. We rationalize why this many-body effect makes such nanohybrids useful for optoelectronic devices. PMID:23991266

  5. Intrinsic homogeneous linewidth and broadening mechanisms of excitons in monolayer transition metal dichalcogenides.

    PubMed

    Moody, Galan; Kavir Dass, Chandriker; Hao, Kai; Chen, Chang-Hsiao; Li, Lain-Jong; Singh, Akshay; Tran, Kha; Clark, Genevieve; Xu, Xiaodong; Berghäuser, Gunnar; Malic, Ermin; Knorr, Andreas; Li, Xiaoqin

    2015-01-01

    The band-edge optical response of transition metal dichalcogenides, an emerging class of atomically thin semiconductors, is dominated by tightly bound excitons localized at the corners of the Brillouin zone (valley excitons). A fundamental yet unknown property of valley excitons in these materials is the intrinsic homogeneous linewidth, which reflects irreversible quantum dissipation arising from system (exciton) and bath (vacuum and other quasiparticles) interactions and determines the timescale during which excitons can be coherently manipulated. Here we use optical two-dimensional Fourier transform spectroscopy to measure the exciton homogeneous linewidth in monolayer tungsten diselenide (WSe2). The homogeneous linewidth is found to be nearly two orders of magnitude narrower than the inhomogeneous width at low temperatures. We evaluate quantitatively the role of exciton-exciton and exciton-phonon interactions and population relaxation as linewidth broadening mechanisms. The key insights reported here—strong many-body effects and intrinsically rapid radiative recombination—are expected to be ubiquitous in atomically thin semiconductors. PMID:26382305

  6. Resonant surface plasmon-exciton interaction in hybrid MoSe2@Au nanostructures.

    PubMed

    Abid, I; Bohloul, A; Najmaei, S; Avendano, C; Liu, H-L; Péchou, R; Mlayah, A; Lou, J

    2016-04-14

    In this work we investigate the interaction between plasmonic and excitonic resonances in hybrid MoSe2@Au nanostructures. The latter were fabricated by combining chemical vapor deposition of MoSe2 atomic layers, Au disk processing by nanosphere lithography and a soft lift-off/transfer technique. The samples were characterized by scanning electron and atomic force microscopy. Their optical properties were investigated experimentally using optical absorption, Raman scattering and photoluminescence spectroscopy. The work is focused on a resonant situation where the surface plasmon resonance is tuned to the excitonic transition. In that case, the near-field interaction between the surface plasmons and the confined excitons leads to interference between the plasmonic and excitonic resonances that manifests in the optical spectra as a transparency dip. The plasmonic-excitonic interaction regime is determined using quantitative analysis of the optical extinction spectra based on an analytical model supported by numerical simulations. We found that the plasmonic-excitonic resonances do interfere thus leading to a typical Fano lineshape of the optical extinction. The near-field nature of the plasmonic-excitonic interaction is pointed out experimentally from the dependence of the optical absorption on the number of monolayer stacks on the Au nanodisks. The results presented in this work contribute to the development of new concepts in the field of hybrid plasmonics. PMID:27029770

  7. Two-dminensional exciton states in monolayer semiconducting phosphorus alotropes

    NASA Astrophysics Data System (ADS)

    Rocha, Alexandre R.; Villegas, Cesar E. P.

    During the last decade, novel two-dimensional (2D) semiconducting materials have been synthesized and characterised. As a result, there have been several theoretical and experimental proposals to incorporate 2D materials for designing next generation electronic and optoelectronics devices. In particular, it has been demonstrated that light absorption in phosphorus-based monolayers can span the whole visible spectrum, suggesting they could be used for optolectronic applications. A key ingredient for optolectronic applications is the presence of excitons and their subsequent diffusion along a donor material. This is influenced by the character of the different excitations taking place, as well as, the exciton binding energy. Therefore, In this work we use accurate many-body corrected density functional theory by means of GW-BSE methodology to elucidate the most important optical transitions, exciton energy spectrum as well as exciton extension in different types of phosphorene materials. In addition, we solve the Schrodinger equation for different 2D screened potentials and estimate the 2D exciton energy levels and radius extension. Finally, in order to assess further studies based on these systems, we provide a simple analityc expression for estimating 2D exciton energy levels. Research funded by FAPESP-Brazil.

  8. Singlet fission in pentacene through multi-exciton quantum states.

    PubMed

    Zimmerman, Paul M; Zhang, Zhiyong; Musgrave, Charles B

    2010-08-01

    Multi-exciton generation-the creation of multiple charge carrier pairs from a single photon-has been reported for several materials and may dramatically increase solar cell efficiency. Singlet fission, its molecular analogue, may govern multi-exciton generation in a variety of materials, but a fundamental mechanism for singlet fission has yet to be described. Here, we use sophisticated ab initio calculations to show that singlet fission in pentacene proceeds through rapid internal conversion of the photoexcited state into a dark state of multi-exciton character that efficiently splits into two triplets. We show that singlet fission to produce a pair of triplet excitons must involve an intermediate state that (i) has a multi-exciton character, (ii) is energetically accessible from the optically allowed excited state, and (iii) efficiently dissociates into multiple electron-hole pairs. The rational design of photovoltaic materials that make use of singlet fission will require similar ab initio analysis of multi-exciton states such as the dark state studied here. PMID:20651727

  9. Femtosecond THz Studies of Intra-Excitonic Transitions

    SciTech Connect

    Huber, Rupert; Schmid, Ben A.; Kaindl, Robert A.; Chemla, Daniel S.

    2007-10-02

    Few-cycle THz pulses are employed to resonantly access the internal fine structure of photogenerated excitons in semiconductors, on the femtosecond time scale. This technique allows us to gain novel insight into many-body effects of excitons and reveal key quantum optical processes. We discuss experiments that monitor the density-dependent re?normalization of the binding energy of a high-density exciton gas in GaAs/AlGaAs quantum wells close to the Mott transition. In a dilute ensemble of 3p excitons in Cu2O, stimulated THz emission from internal transitions to the energetically lower 2s state is observed at a photon energy of 6.6 meV, with a cross section of 10-14 cm2. Simultaneous interband excitation of both exciton levels drives quantum beats, which cause efficient THz emission at the difference frequency. By extending this principle to various other exciton resonances, we develop a novel way of mapping the fine structure by two-dimensional THz emission spectroscopy.

  10. Parametric study and optimization of a micro-optical switch with a laterally driven electromagnetic microactuator

    NASA Astrophysics Data System (ADS)

    Han, Jeong Sam; Ko, Jong Soo; Kim, Youn Tae; Kwak, Byung Man

    2002-11-01

    In this paper we present an in-depth parametric study and structural optimization for a micro-optical switch based on the concept of a laterally driven electromagnetic microactuator (LaDEM). This utilizes the nonlinear behavior of a snap-through buckling occurring in two arch-shaped leaf springs of the switch, when actuated by a distributed Lorentz force induced along the leaf springs. A sudden jump in displacement can facilitate a large actuation stroke suitable for practical applications. The leaf springs are connected to the fixed frame with two meandering parts, which also enhance their flexibility. Thus, an important objective in the design of the micro-optical switch is to achieve a large displacement with low actuation force. For this purpose, the effect of important geometrical parameters, such as the initial height of the leaf spring and the dimensions of meandering part on the displacement response is first investigated and optimized to satisfy given design specifications. The nonlinear displacement-load response calculated by a modified Riks method in ABAQUS shows good agreement with the measurement result. Nonlinear finite element techniques and optimizations are found to be valuable tools for the analysis and design of microactuators, which utilize a complex nonlinear snap-through buckling behavior.

  11. Acoustical and Optical Characterization of Air Entrapment in Piezo-Driven Inkjet Printheads

    NASA Astrophysics Data System (ADS)

    de Jong, Jos; Reinten, Hans; Versluis, Michel

    2005-11-01

    Air entrapment leads to malfunctioning of jet formation in a piezo-driven inkjet printhead. The entrapped air bubbles disturb the acoustics and in many cases cause the droplet formation to stop. Here we will focus on piezo inkjet devices where a voltage pulse applied to a piezo-electric element causes an ink-filled channel to deform, thereby creating a pressure waveform in the ink. The nozzle diameter is typically 30 μm. Droplets are jetted every 50 μs and it is essential that the droplet formation remains stable for an extensive period. Here we detect air entrapment, reveal the air entrapment process, and the time evolution of the entrapped air bubble. The acoustical signal is monitored by using the piezo actuator as a sensor to measure the pressure in the channel after the pulse is applied. This signal is employed to detect air bubbles inside the ink channel and to trigger the optical setup. High speed imaging is employed to perfom optical measurements at microsecond timescales. Once entrapped, the air bubble has an initial radius of 10 μm and oscillates with a frequency near 200 kHz. The radial growth of the bubble is found to be 0.3 μm/ms.

  12. Coulomb Mediated Hybridization of Excitons in Coupled Quantum Dots

    NASA Astrophysics Data System (ADS)

    Ardelt, P.-L.; Gawarecki, K.; Müller, K.; Waeber, A. M.; Bechtold, A.; Oberhofer, K.; Daniels, J. M.; Klotz, F.; Bichler, M.; Kuhn, T.; Krenner, H. J.; Machnikowski, P.; Finley, J. J.

    2016-02-01

    We report Coulomb mediated hybridization of excitonic states in optically active InGaAs quantum dot molecules. By probing the optical response of an individual quantum dot molecule as a function of the static electric field applied along the molecular axis, we observe unexpected avoided level crossings that do not arise from the dominant single-particle tunnel coupling. We identify a new few-particle coupling mechanism stemming from Coulomb interactions between different neutral exciton states. Such Coulomb resonances hybridize the exciton wave function over four different electron and hole single-particle orbitals. Comparisons of experimental observations with microscopic eight-band k .p calculations taking into account a realistic quantum dot geometry show good agreement and reveal that the Coulomb resonances arise from broken symmetry in the artificial semiconductor molecule.

  13. Excitonic condensation in bilayer systems

    NASA Astrophysics Data System (ADS)

    Su, Jung-Jung

    Among the many examples of Bose condensation considered in physics, electron-hole-pair (exciton) condensation has maintained special interest because it has been difficult to realize experimentally, and because of controversy about condensate properties. In this thesis, we studied the various aspects of spontaneous symmetry broken state of exciton in bilayer using mean field theory. We calculated the photoluminescence of excitonic condensation created by laser. We developed a one-dimensional toy model of excitonic supercurrent using mean field theory plus non-equilibrium Green's function (NEGF) which give qualitatively consistent results with experiments. We proposed graphene bilayer as a novel system for excitonic condensation to occur and estimate it to exist even at temperature as high as room temperature.

  14. Valley excitons in two-dimensional semiconductors

    DOE PAGESBeta

    Yu, Hongyi; Cui, Xiaodong; Xu, Xiaodong; Yao, Wang

    2014-12-30

    Monolayer group-VIB transition metal dichalcogenides have recently emerged as a new class of semiconductors in the two-dimensional limit. The attractive properties include: the visible range direct band gap ideal for exploring optoelectronic applications; the intriguing physics associated with spin and valley pseudospin of carriers which implies potentials for novel electronics based on these internal degrees of freedom; the exceptionally strong Coulomb interaction due to the two-dimensional geometry and the large effective masses. The physics of excitons, the bound states of electrons and holes, has been one of the most actively studied topics on these two-dimensional semiconductors, where the excitons exhibitmore » remarkably new features due to the strong Coulomb binding, the valley degeneracy of the band edges, and the valley dependent optical selection rules for interband transitions. Here we give a brief overview of the experimental and theoretical findings on excitons in two-dimensional transition metal dichalcogenides, with focus on the novel properties associated with their valley degrees of freedom.« less

  15. Valley excitons in two-dimensional semiconductors

    SciTech Connect

    Yu, Hongyi; Cui, Xiaodong; Xu, Xiaodong; Yao, Wang

    2014-12-30

    Monolayer group-VIB transition metal dichalcogenides have recently emerged as a new class of semiconductors in the two-dimensional limit. The attractive properties include: the visible range direct band gap ideal for exploring optoelectronic applications; the intriguing physics associated with spin and valley pseudospin of carriers which implies potentials for novel electronics based on these internal degrees of freedom; the exceptionally strong Coulomb interaction due to the two-dimensional geometry and the large effective masses. The physics of excitons, the bound states of electrons and holes, has been one of the most actively studied topics on these two-dimensional semiconductors, where the excitons exhibit remarkably new features due to the strong Coulomb binding, the valley degeneracy of the band edges, and the valley dependent optical selection rules for interband transitions. Here we give a brief overview of the experimental and theoretical findings on excitons in two-dimensional transition metal dichalcogenides, with focus on the novel properties associated with their valley degrees of freedom.

  16. Recent developments in laser-driven and hollow-core fiber optic gyroscopes

    NASA Astrophysics Data System (ADS)

    Digonnet, M. J. F.; Chamoun, J. N.

    2016-05-01

    Although the fiber optic gyroscope (FOG) continues to be a commercial success, current research efforts are endeavoring to improve its precision and broaden its applicability to other markets, in particular the inertial navigation of aircraft. Significant steps in this direction are expected from the use of (1) laser light to interrogate the FOG instead of broadband light, and (2) a hollow-core fiber (HCF) in the sensing coil instead of a conventional solid-core fiber. The use of a laser greatly improves the FOG's scale-factor stability and eliminates the source excess noise, while an HCF virtually eliminates the Kerr-induced drift and significantly reduces the thermal and Faraday-induced drifts. In this paper we present theoretical evidence that in a FOG with a 1085-m coil interrogated with a laser, the two main sources of noise and drift resulting from the use of coherent light can be reduced below the aircraft-navigation requirement by using a laser with a very broad linewidth, in excess of 40 GHz. We validate this concept with a laser broadened with an external phase modulator driven with a pseudo-random bit sequence at 2.8 GHz. This FOG has a measured noise of 0.00073 deg/√h, which is 30% below the aircraft-navigation requirement. Its measured drift is 0.03 deg/h, the lowest reported for a laser-driven FOG and only a factor of 3 larger than the navigation-grade specification. To illustrate the potential benefits of a hollow-core fiber in the FOG, this review also summarizes the previously reported performance of an experimental FOG utilizing 235 m of HCF and interrogated with broadband light.

  17. Exciton-phonon system on a star graph: A perturbative approach

    NASA Astrophysics Data System (ADS)

    Yalouz, Saad; Pouthier, Vincent

    2016-05-01

    Based on the operatorial formulation of the perturbation theory, the properties of an exciton coupled with optical phonons on a star graph are investigated. Within this method, the dynamics is governed by an effective Hamiltonian, which accounts for exciton-phonon entanglement. The exciton is dressed by a virtual phonon cloud whereas the phonons are clothed by virtual excitonic transitions. In spite of the coupling with the phonons, it is shown that the energy spectrum of the dressed exciton resembles that of a bare exciton. The only differences originate in a polaronic mechanism that favors an energy shift and a decay of the exciton hopping constant. By contrast, the motion of the exciton allows the phonons to propagate over the graph so that the dressed normal modes drastically differ from the localized modes associated to bare phonons. They define extended vibrations whose properties depend on the state occupied by the exciton that accompanies the phonons. It is shown that the phonon frequencies, either red shifted or blue shifted, are very sensitive to the model parameter in general, and to the size of the graph in particular.

  18. Exciton-vibrational coupling in the dynamics and spectroscopy of Frenkel excitons in molecular aggregates

    NASA Astrophysics Data System (ADS)

    Schröter, M.; Ivanov, S. D.; Schulze, J.; Polyutov, S. P.; Yan, Y.; Pullerits, T.; Kühn, O.

    2015-03-01

    The influence of exciton-vibrational coupling on the optical and transport properties of molecular aggregates is an old problem that gained renewed interest in recent years. On the experimental side, various nonlinear spectroscopic techniques gave insight into the dynamics of systems as complex as photosynthetic antennae. Striking evidence was gathered that in these protein-pigment complexes quantum coherence is operative even at room temperature conditions. Investigations were triggered to understand the role of vibrational degrees of freedom, beyond that of a heat bath characterized by thermal fluctuations. This development was paralleled by theory, where efficient methods emerged, which could provide the proper frame to perform non-Markovian and non-perturbative simulations of exciton-vibrational dynamics and spectroscopy. This review summarizes the state of affairs of the theory of exciton-vibrational interaction in molecular aggregates and photosynthetic antenna complexes. The focus is put on the discussion of basic effects of exciton-vibrational interaction from the stationary and dynamics points of view. Here, the molecular dimer plays a prominent role as it permits a systematic investigation of absorption and emission spectra by numerical diagonalization of the exciton-vibrational Hamiltonian in a truncated Hilbert space. An extension to larger aggregates, having many coupled nuclear degrees of freedom, becomes possible with the Multi-Layer Multi-Configuration Time-Dependent Hartree (ML-MCTDH) method for wave packet propagation. In fact it will be shown that this method allows one to approach the limit of almost continuous spectral densities, which is usually the realm of density matrix theory. Real system-bath situations are introduced for two models, which differ in the way strongly coupled nuclear coordinates are treated, as a part of the relevant system or the bath. A rather detailed exposition of the Hierarchy Equations Of Motion (HEOM) method will be

  19. Radiative and nonradiative exciton energy transfer in monolayers of two-dimensional group-VI transition metal dichalcogenides

    NASA Astrophysics Data System (ADS)

    Manolatou, Christina; Wang, Haining; Chan, Weimin; Tiwari, Sandip; Rana, Farhan

    2016-04-01

    We present results on the rates of interlayer energy transfer between excitons in monolayers of two-dimensional group-VI transition metal dichalcogenides (TMDs). We consider both radiative (mediated by real photons) and nonradiative (mediated by virtual photons) mechanisms of energy transfer using a unified Green's function approach that takes into account modification of the exciton energy dispersions as a result of interactions. The large optical oscillator strengths associated with excitons in TMDs result in very fast energy transfer rates. The energy transfer times depend on the exciton momentum, exciton linewidth, and the interlayer separation and can range from values less than 100 femtoseconds to more than tens of picoseconds. Whereas inside the light cone the energy transfer rates of longitudinal and transverse excitons are comparable, outside the light cone the energy transfer rates of longitudinal excitons far exceed those of transverse excitons. Average energy transfer times for a thermal ensemble of longitudinal and transverse excitons is temperature dependent and can be smaller than a picosecond at room temperature for interlayer separations smaller than 10 nm. Energy transfer times of localized excitons range from values less than a picosecond to several tens of picoseconds. When the exciton scattering and dephasing rates are small, energy transfer dynamics exhibit coherent oscillations. Our results show that electromagnetic interlayer energy transfer can be an efficient mechanism for energy exchange between TMD monolayers.

  20. Nonlinear phenomena and multiphonon transitions in the exciton region of a spectrum

    NASA Astrophysics Data System (ADS)

    Lisitsa, M. P.; Taratuta, R. A.; Yaremko, A. M.

    1990-08-01

    Using the Keldysh diagram method, the nonlinear susceptibility for a Frenkel exciton with account for the multiquantum transitions is obtained. Propagation of the strong resonance electromagnetic wave through the crystal and the optical bistability phenomenon are considered.

  1. Exciton condensation in microcavities under three-dimensional quantization conditions

    SciTech Connect

    Kochereshko, V. P. Platonov, A. V.; Savvidis, P.; Kavokin, A. V.; Bleuse, J.; Mariette, H.

    2013-11-15

    The dependence of the spectra of the polarized photoluminescence of excitons in microcavities under conditions of three-dimensional quantization on the optical-excitation intensity is investigated. The cascade relaxation of polaritons between quantized states of a polariton Bose condensate is observed.

  2. Excitons in atomically thin black phosphorus

    NASA Astrophysics Data System (ADS)

    Surrente, A.; Mitioglu, A. A.; Galkowski, K.; Tabis, W.; Maude, D. K.; Plochocka, P.

    2016-03-01

    Raman scattering and photoluminescence spectroscopy are used to investigate the optical properties of single layer black phosphorus obtained by mechanical exfoliation of bulk crystals under an argon atmosphere. The Raman spectroscopy, performed in situ on the same flake as the photoluminescence measurements, demonstrates the single layer character of the investigated samples. The emission spectra, dominated by excitonic effects, display the expected in-plane anisotropy. The emission energy depends on the type of substrate on which the flake is placed due to the different dielectric screening. Finally, the blueshift of the emission with increasing temperature is well described using a two-oscillator model for the temperature dependence of the band gap.

  3. Feasibility study of a nuclear exciton laser

    NASA Astrophysics Data System (ADS)

    ten Brinke, Nicolai; Schützhold, Ralf; Habs, Dietrich

    2013-05-01

    Nuclear excitons known from Mössbauer spectroscopy describe coherent excitations of a large number of nuclei—analogous to Dicke states (or Dicke super-radiance) in quantum optics. In this paper, we study the possibility of constructing a laser based on these coherent excitations. In contrast to the free-electron laser (in its usual design), such a device would be based on stimulated emission and thus might offer certain advantages, e.g., regarding energy-momentum accuracy. Unfortunately, inserting realistic parameters, the window of operability is probably not open (yet) to present-day technology; but our design should be feasible in the UV regime, for example.

  4. Visualization and measurement of capillary-driven blood flow using spectral domain optical coherence tomography

    PubMed Central

    Cito, Salvatore; Ahn, Yeh-Chan; Pallares, Jordi; Duarte, Rodrigo Martinez; Chen, Zhongping; Madou, Marc; Katakis, Ioanis

    2013-01-01

    Capillary-driven flow (CD-flow) in microchannels plays an important role in many microfluidic devices. These devices, the most popular being those based in lateral flow, are becoming increasingly used in health care and diagnostic applications. CD-flow can passively pump biological fluids as blood, serum or plasma, in microchannels and it can enhance the wall mass transfer by exploiting the convective effects of the flow behind the meniscus. The flow behind the meniscus has not been experimentally identified up to now because of the lack of high-resolution, non-invasive, cross-sectional imaging means. In this study, spectral-domain Doppler optical coherence tomography is used to visualize and measure the flow behind the meniscus in CD-flows of water and blood. Microchannels of polydimethylsiloxane and glass with different cross-sections are considered. The predictions of the flow behind the meniscus of numerical simulations using the power-law model for non-Newtonian fluids are in reasonable agreement with the measurements using blood as working fluid. The extension of the Lucas–Washburn equation to non-Newtonian power-law fluids predicts well the velocity of the meniscus of the experiments using blood. PMID:23795150

  5. Exciton Scattering approach for conjugated macromolecules: from electronic spectra to electron-phonon coupling

    NASA Astrophysics Data System (ADS)

    Tretiak, Sergei

    2014-03-01

    The exciton scattering (ES) technique is a multiscale approach developed for efficient calculations of excited-state electronic structure and optical spectra in low-dimensional conjugated macromolecules. Within the ES method, the electronic excitations in the molecular structure are attributed to standing waves representing quantum quasi-particles (excitons), which reside on the graph. The exciton propagation on the linear segments is characterized by the exciton dispersion, whereas the exciton scattering on the branching centers is determined by the energy-dependent scattering matrices. Using these ES energetic parameters, the excitation energies are then found by solving a set of generalized ``particle in a box'' problems on the graph that represents the molecule. All parameters can be extracted from quantum-chemical computations of small molecular fragments and tabulated in the ES library for further applications. Subsequently, spectroscopic modeling for any macrostructure within considered molecular family could be performed with negligible numerical effort. The exciton scattering properties of molecular vertices can be further described by tight-binding or equivalently lattice models. The on-site energies and hopping constants are obtained from the exciton dispersion and scattering matrices. Such tight-binding model approach is particularly useful to describe the exciton-phonon coupling, energetic disorder and incoherent energy transfer in large branched conjugated molecules. Overall the ES applications accurately reproduce the optical spectra compared to the reference quantum chemistry results, and make possible to predict spectra of complex macromolecules, where conventional electronic structure calculations are unfeasible.

  6. Studies of low temperature photoluminescence spectra and excitonic valley polarization in monolayer MoTe2

    NASA Astrophysics Data System (ADS)

    Koirala, Sandhaya; Mouri, Shinichiro; Miyauchi, Yuhei; Matsuda, Kazunari; Kyoto University Team

    Recently, atomically thin layered transition-metal dichalcogenide (TMDs) in the form MX2 (M = Mo, W, X = S, Se, Te) have attracted much interest from the viewpoints of their fundamental physics and potential applications. The characteristic optical features of semiconducting TMDs arise from excitons confined in their atomically thin layers. Molybdenum ditelluride MoTe2 has attracted emerging research interest because of optical gap energy (lowest exciton transition) of 1.09 eV, and large spin-orbit coupling of 250 meV. Temperature-dependent photoluminescence (PL) and polarization-resolved PL measurement were performed for mechanically exfoliated monolayer MoTe2 from 4.4 to 300 K. At a low temperature, the PL spectra from MoTe2 show two sharp peaks for excitons and charged excitons (trions). The systematic temperature-dependent PL measurements revel that the homogeneous linewidth of the exciton peak broadens linearly as the temperature increased due to exciton-acoustic-phonon interactions. From polarization-resolved PL measurements, the valley polarization of above 40 % in the exciton state has been observed at low temperatures. In this meeting, we will discuss about exciton dephasing and valley polarization in monolayer MoTe2.

  7. Exciton interactions in reaction centers of the photosynthetic bacterium Rhodopseudomonas viridis probed by optical triplet-minus-singlet polarization spectroscopy at 1.2 K monitored through absorbance-detected magnetic resonance.

    PubMed

    Lous, E J; Hoff, A J

    1987-09-01

    Linear dichroic triplet-minus-singlet [LD-(T - S)] spectra of isolated reaction centers of the photosynthetic bacterium Rhodopseudomonas viridis have been measured at 1.2 K with the linear dichroic absorbance-detected magnetic resonance (LD-ADMR) technique for two mutually perpendicular directions of the preferred axis. The LD-(T - S) spectra have been calibrated with respect to the corresponding (T - S) spectra as a function of applied microwave power and quantitatively interpreted using the formalism of photoselection. The transition moment of the optical transition at 1007 nm makes angles of 72 degrees +/- 5 degrees and 15 degrees +/- 5 degrees with the triplet x and y spin axes, respectively. The experimental spectra have been simulated employing exciton theory and using the atomic coordinates of the resolved crystal structure of the reaction center. The spectral interpretation yields the angles between the transition moments of the various absorption bands of the (T - S) spectra and the triplet axes, and between the moments themselves, with the triplet state of the primary donor (3)P localized on the P-bacteriochlorophyll b in the "active" (L) chain. PMID:16578814

  8. Specific features of the hybridization of Frenkel and Wannier-Mott excitons in a microcavity

    NASA Astrophysics Data System (ADS)

    Dubovskii, O. A.; Agranovich, V. M.

    2016-07-01

    Polariton states have been investigated in a microcavity, where the energy of the Frenkel exciton in an organic quantum well and the energy of the semiconductor Wannier-Mott exciton in an inorganic quantum well are close to the microcavity optical mode. It has been shown that the interaction of each of these excitons with the microcavity optical mode leads to their interaction with each other and to the formation of mutually coupled hybrid excitations. The influence of the location of the quantum wells in a microcavity on the spectra of hybrid states with different polarizations has been analyzed.

  9. Momentum dependence of the excitons in pentacene

    SciTech Connect

    Roth, Friedrich; Schuster, Roman; Koenig, Andreas; Knupfer, Martin; Berger, Helmuth

    2012-05-28

    We have carried out electron energy-loss investigations of the lowest singlet excitons in pentacene at 20 K. Our studies allow to determine the full exciton band structure in the a*, b* reciprocal lattice plane. The lowest singlet exciton can move coherently within this plane, and the resulting exciton dispersion is highly anisotropic. The analysis of the energetically following (satellite) features indicates a strong admixture of charge transfer excitations to the exciton wave function.

  10. Excitonic complexes in single zinc-blende GaN/AlN quantum dots grown by droplet epitaxy

    SciTech Connect

    Sergent, S.; Kako, S.; Bürger, M.; Schupp, T.; As, D. J.; Arakawa, Y.

    2014-10-06

    We study by microphotoluminescence the optical properties of single zinc-blende GaN/AlN quantum dots grown by droplet epitaxy. We show evidences of both excitonic and multiexcitonic recombinations in individual quantum dots with radiative lifetimes shorter than 287 ± 8 ps. Owing to large band offsets and a large exciton binding energy, the excitonic recombinations of single zinc-blende GaN/AlN quantum dots can be observed up to 300 K.

  11. Crossed excitons in a semiconductor nanostructure of mixed dimensionality

    SciTech Connect

    Owschimikow, Nina Kolarczik, Mirco; Kaptan, Yücel I.; Grosse, Nicolai B.; Woggon, Ulrike

    2014-09-08

    Semiconductor systems of reduced dimensionality, e.g., quantum dots or quantum wells, display a characteristic spectrum of confined excitons. Combining several of these systems may lead to the formation of “crossed” excitons, and thus new equilibrium states and scattering channels. We derive gain excitation spectra from two-color pump-probe experiments on an In(Ga)As based quantum dot semiconductor optical amplifier by analyzing the amplitudes of the traces. This grants access to the quantum dot response, even in the presence of strong absorption by the surroundings at the excitation energy. The gain excitation spectra yield evidence of crossed quantum dot-bulk states.

  12. Exciton-plasmon interactions and energy transfer in nanoparticles

    NASA Astrophysics Data System (ADS)

    Govorov, Alexander

    2009-03-01

    Energy transfer between optically-excited nanocrystals coupled by the Coulomb interaction can be very efficient. The interaction of excitons and plasmons in nanocrystals leads to several effects: energy transfer between nanoparticles (NPs), electromagnetic enhancement, reduced exciton diffusion in nanowires (NWs), exciton energy shifts, and interference and non-linear phenomena [1-3]. Using kinetic equations for excitons, we model exciton transport in a NW and explain the origin of the blue shift of exciton emission observed in the recent experiments on hybrid NW-NP assemblies [2]. We also model artificial light-harvesting complexes composed of chlorophylls, bacterial reaction centers, and NPs [3]. Using superior optical properties of metal and semiconductor NPs, one can strongly enhance the efficiency of light harvesting [3]. An interaction between a discrete state of exciton and a continuum of plasmonic states can give rise to interference effects (Fano-like asymmetric resonances). These interference effects greatly enhance visibility of relatively weak exciton signals and can be used for spectroscopy of single nanoparticle and molecules. In the nonlinear regime, the Fano effect becomes strongly amplified [4]. In conclusion, our theory explains present experimental results and also provides motivation for future experiments and applications. Potential applications of dynamical exciton-plasmon systems include sensors and light-harvesting. The above theoretical studies were performed in collaboration with several groups [1-4]. [4pt] [1] A. O. Govorov, G. W. Bryant, W. Zhang, T. Skeini, J. Lee, N. A. Kotov, J. M. Slocik, and R. R. Naik, Nano Letters 6, 984 (2006).[0pt] [2] J. Lee, P. Hernandez, J. Lee, A. Govorov, and N. Kotov, Nature Materials 6, 291 (2007).[0pt] [3] A. O. Govorov and I. Carmeli, Nano Lett. 7, 620 (2007); S. Mackowski, S. W"ormke, A.J. Maier, T.H.P. Brotosudarmo, H. Harutyunyan, A. Hartschuh, A.O. Govorov, H. Scheer, C. Br"auchle, Nano Lett. 8, 558

  13. Optically driven quantum dots as source of coherent cavity phonons: a proposal for a phonon laser scheme.

    PubMed

    Kabuss, Julia; Carmele, Alexander; Brandes, Tobias; Knorr, Andreas

    2012-08-01

    We present a microscopically based scheme for the generation of coherent cavity phonons (phonon laser) by an optically driven semiconductor quantum dot coupled to a THz acoustic nanocavity. External laser pump light on an anti-Stokes resonance creates an effective Lambda system within a two-level dot that leads to coherent phonon statistics. We use an inductive equation of motion method to estimate a realistic parameter range for an experimental realization of such phonon lasers. This scheme for the creation of nonequilibrium phonons is robust with respect to radiative and phononic damping and only requires optical Rabi frequencies of the order of the electron-phonon coupling strength. PMID:23006175

  14. Significant Lowering Optical Loss of Electrodes via using Conjugated Polyelectrolytes Interlayer for Organic Laser in Electrically Driven Device Configuration

    PubMed Central

    Yi, Jianpeng; Niu, Qiaoli; Xu, Weidong; Hao, Lin; Yang, Lei; Chi, Lang; Fang, Yueting; Huang, Jinjin; Xia, Ruidong

    2016-01-01

    One of the challenges toward electrically driven organic lasers is the huge optical loss associated with the contact of electrodes and organic gain medium in device. We demonstrated a significant reduction of the optical loss by using our newly developed conjugated polyelectrolytes (CPE) PPFN+Br− as interlayer between gain medium and electrode. The optically pumped amplified spontaneous emission (ASE) was observed at very low threshold for PFO as optical gain medium and up to 37 nm thick CPE as interlayer in device configuration, c.f., a 5.7-fold ASE threshold reduction from pump energy 150 μJ/cm2 for ITO/PFO to 26.3 μJ/cm2 for ITO/PPFN+Br−/PFO. Furthermore, ASE narrowing displayed at pump energy up to 61.8 μJ/cm2 for device ITO/PEDOT:PSS/PFO/PPFN+Br−/Ag, while no ASE was observed for the reference devices without CPE interlayer at pump energy up to 240 μJ/cm2. The optically pumped lasing operation has also been achieved at threshold up to 45 μJ/cm2 for one-dimensional distributed feedback laser fabricated on ITO etched grating in devices with CPE interlayer, demonstrating a promising device configuration for addressing the challenge of electrically driven organic lasers. PMID:27165729

  15. Significant Lowering Optical Loss of Electrodes via using Conjugated Polyelectrolytes Interlayer for Organic Laser in Electrically Driven Device Configuration.

    PubMed

    Yi, Jianpeng; Niu, Qiaoli; Xu, Weidong; Hao, Lin; Yang, Lei; Chi, Lang; Fang, Yueting; Huang, Jinjin; Xia, Ruidong

    2016-01-01

    One of the challenges toward electrically driven organic lasers is the huge optical loss associated with the contact of electrodes and organic gain medium in device. We demonstrated a significant reduction of the optical loss by using our newly developed conjugated polyelectrolytes (CPE) PPFN(+)Br(-) as interlayer between gain medium and electrode. The optically pumped amplified spontaneous emission (ASE) was observed at very low threshold for PFO as optical gain medium and up to 37 nm thick CPE as interlayer in device configuration, c.f., a 5.7-fold ASE threshold reduction from pump energy 150 μJ/cm(2) for ITO/PFO to 26.3 μJ/cm(2) for ITO/PPFN(+)Br(-)/PFO. Furthermore, ASE narrowing displayed at pump energy up to 61.8 μJ/cm(2) for device ITO/PEDOT:PSS/PFO/PPFN(+)Br(-)/Ag, while no ASE was observed for the reference devices without CPE interlayer at pump energy up to 240 μJ/cm(2). The optically pumped lasing operation has also been achieved at threshold up to 45 μJ/cm(2) for one-dimensional distributed feedback laser fabricated on ITO etched grating in devices with CPE interlayer, demonstrating a promising device configuration for addressing the challenge of electrically driven organic lasers. PMID:27165729

  16. Significant Lowering Optical Loss of Electrodes via using Conjugated Polyelectrolytes Interlayer for Organic Laser in Electrically Driven Device Configuration

    NASA Astrophysics Data System (ADS)

    Yi, Jianpeng; Niu, Qiaoli; Xu, Weidong; Hao, Lin; Yang, Lei; Chi, Lang; Fang, Yueting; Huang, Jinjin; Xia, Ruidong

    2016-05-01

    One of the challenges toward electrically driven organic lasers is the huge optical loss associated with the contact of electrodes and organic gain medium in device. We demonstrated a significant reduction of the optical loss by using our newly developed conjugated polyelectrolytes (CPE) PPFN+Br‑ as interlayer between gain medium and electrode. The optically pumped amplified spontaneous emission (ASE) was observed at very low threshold for PFO as optical gain medium and up to 37 nm thick CPE as interlayer in device configuration, c.f., a 5.7-fold ASE threshold reduction from pump energy 150 μJ/cm2 for ITO/PFO to 26.3 μJ/cm2 for ITO/PPFN+Br‑/PFO. Furthermore, ASE narrowing displayed at pump energy up to 61.8 μJ/cm2 for device ITO/PEDOT:PSS/PFO/PPFN+Br‑/Ag, while no ASE was observed for the reference devices without CPE interlayer at pump energy up to 240 μJ/cm2. The optically pumped lasing operation has also been achieved at threshold up to 45 μJ/cm2 for one-dimensional distributed feedback laser fabricated on ITO etched grating in devices with CPE interlayer, demonstrating a promising device configuration for addressing the challenge of electrically driven organic lasers.

  17. Charged two-exciton emission from a single semiconductor nanocrystal

    SciTech Connect

    Hu, Fengrui; Zhang, Qiang; Zhang, Chunfeng; Wang, Xiaoyong; Xiao, Min

    2015-03-30

    Here, we study the photoluminescence (PL) time trajectories of single CdSe/ZnS nanocrystals (NCs) as a function of the laser excitation power. At the low laser power, the PL intensity of a single NC switches between the “on” and “off” levels arising from the neutral and positively charged single excitons, respectively. With the increasing laser power, an intermediate “grey” level is formed due to the optical emission from a charged multiexciton state composed of two excitons and an extra electron. Both the inter-photon correlation and the PL decay measurements demonstrate that lifetime-indistinguishable photon pairs are emitted from this negatively charged two-exciton state.

  18. High-gain optical Cherenkov oscillator driven by low-voltage electron beam

    SciTech Connect

    Smetanin, I.V.; Oraevsky, A.N.

    1995-12-31

    A novel scheme of high-gain optical (from IR up to UV) Cherenkov-type oscillator driven by low-voltage high-current electron beam is proposed in the present report. In the scheme discussed the magnetized electron beam propagates above the surface of absorbing medium of complex dielectric susceptibility {epsilon}{omega} = {epsilon}{sub 1}({omega}) + i{epsilon}{sub 2}({omega}), {epsilon}{sub 2}>0. We have found that at frequencies {omega} that {beta}{sup 2}> 2{epsilon}{sub 1}/{vert_bar}{epsilon}{vert_bar}{sup 2} ({beta} = v/c, v is the electron velocity), an amplification of co-propagating slow surface electromagnetic wave is possible. In contrast to the conventional Cherenkov oscillators, the absorption condition {epsilon}2>0 is crucial for the gain, which is absent for transparent medium. The physics of this amplification effect is analogous to that of electron beam dissipative instability. The wavelength generated is determined here by dielectric properties of the surface, and does not depend strongly on electron energy. Thus it is possible to use rather compact low voltage ({le} 1MeV) high-current accelerators as drivers. Optimum oscillation conditions are found to be at frequencies near the resonance absorption lines of surface material (i.e. from IR up to UV). The gain up to {approximately}0.5cm{sup -1} in the near IR ({approximately}10THz, SrF{sub 2} absorption line) is possible for 250keV high current (density {approximately}10{sup 12}cm{sup -3}) electron beam.

  19. Self-trapped exciton and core-valence luminescence in BaF{sub 2} nanoparticles

    SciTech Connect

    Vistovskyy, V. V. Zhyshkovych, A. V.; Chornodolskyy, Ya. M.; Voloshinovskii, A. S.; Myagkota, O. S.; Gloskovskii, A.; Gektin, A. V.; Vasil'ev, A. N.; Rodnyi, P. A.

    2013-11-21

    The influence of the BaF{sub 2} nanoparticle size on the intensity of the self-trapped exciton luminescence and the radiative core-valence transitions is studied by the luminescence spectroscopy methods using synchrotron radiation. The decrease of the self-trapped exciton emission intensity at energies of exciting photons in the range of optical exciton creation (hν ≤ E{sub g}) is less sensitive to the reduction of the nanoparticle sizes than in the case of band-to-band excitation, where excitons are formed by the recombination way. The intensity of the core-valence luminescence shows considerably weaker dependence on the nanoparticle sizes in comparison with the intensity of self-trapped exciton luminescence. The revealed regularities are explained by considering the relationship between nanoparticle size and photoelectron or photohole thermalization length as well as the size of electronic excitations.

  20. Giant permanent dipole moment of two-dimensional excitons bound to a single stacking fault

    NASA Astrophysics Data System (ADS)

    Karin, Todd; Linpeng, Xiayu; Glazov, M. M.; Durnev, M. V.; Ivchenko, E. L.; Harvey, Sarah; Rai, Ashish K.; Ludwig, Arne; Wieck, Andreas D.; Fu, Kai-Mei C.

    2016-07-01

    We investigate the magneto-optical properties of excitons bound to single stacking faults in high-purity GaAs. We find that the two-dimensional stacking fault potential binds an exciton composed of an electron and a heavy hole, and we confirm a vanishing in-plane hole g -factor, consistent with the atomic-scale symmetry of the system. The unprecedented homogeneity of the stacking-fault potential leads to ultranarrow photoluminescence emission lines (with a full width at half-maximum ≲80 μ eV ) and reveals a large magnetic nonreciprocity effect that originates from the magneto-Stark effect for mobile excitons. These measurements unambiguously determine the direction and magnitude of the giant electric dipole moment (≳e ×10 nm ) of the stacking-fault exciton, making stacking faults a promising new platform to study interacting excitonic gases.

  1. Revealing the dark side of a bright exciton-polariton condensate.

    PubMed

    Ménard, J-M; Poellmann, C; Porer, M; Leierseder, U; Galopin, E; Lemaître, A; Amo, A; Bloch, J; Huber, R

    2014-01-01

    Condensation of bosons causes spectacular phenomena such as superfluidity or superconductivity. Understanding the nature of the condensed particles is crucial for active control of such quantum phases. Fascinating possibilities emerge from condensates of light-matter-coupled excitations, such as exciton-polaritons, photons hybridized with hydrogen-like bound electron-hole pairs. So far, only the photon component has been resolved, while even the mere existence of excitons in the condensed regime has been challenged. Here we trace the matter component of polariton condensates by monitoring intra-excitonic terahertz transitions. We study how a reservoir of optically dark excitons forms and feeds the degenerate state. Unlike atomic gases, the atom-like transition in excitons is dramatically renormalized on macroscopic ground state population. Our results establish fundamental differences between polariton condensation and photon lasing and open possibilities for coherent control of condensates. PMID:25115964

  2. Radiative recombination from dark excitons in nanocrystals: Activation mechanisms and polarization properties

    NASA Astrophysics Data System (ADS)

    Rodina, Anna V.; Efros, Alexander L.

    2016-04-01

    We analyze theoretically physical mechanisms responsible for the radiative recombination of the ground optically passive ("dark") exciton (DE), which dominates in photoluminescence (PL) of colloidal nanocrystals (NCs) at low temperatures. The DE becomes optically active due to its mixing with the bright excitons caused by an external magnetic field, dangling-bond spins or by acoustic and optical phonons. These activation mechanisms mix the DE with different bright excitons and, consequently, lead to different PL polarization properties, because they are determined by dipole orientations of the bright excitons, which the DE is coupled with. We show that the PL polarization properties of prolate and oblate shape NCs are different due to different activation mechanisms responsible for the DE recombination.

  3. Exciton annihilation and dephasing dynamics in semiconducting single-walled carbon nanotubes

    SciTech Connect

    Graham, Matt; Ma, Yingzhong; Green, Alexander A.; Hersam, Mark C.; Fleming, Graham

    2010-01-01

    Semiconducting single-walled carbon nanotubes (SWNTs) are one of the most intriguing nanomaterials due to their large aspect ratios, size tunable properties, and dominant many body interactions. While the dynamics of exciton population relaxation have been well characterized, optical dephasing processes have only been exam- ined indirectly through steady-state measurements such as single-molecule spectroscopy that can yield highly variable estimates of the homogeneous linewidth. To bring clarity to these conflicting estimates, a time-domain measurement of exciton dephasing at an ensemble level is necessary. Using two-pulse photon echo (2PE) spec- troscopy, comparatively long dephasing times approaching 200 fs are extracted for the (6,5) tube species at room temperature. In this contribution, we extend our previous study of 2PE and pump-probe spectroscopy to low temperatures to investigate inelastic exciton-exciton scattering. In contrast to the population kinetics observed upon excitation of the second transition-allowed excitonic state (E22 ), our one-color pump-probe data instead shows faster relaxation upon cooling to 60 K when the lowest transition-allowed state (E11 ) is directly excited for the (6,5) tube species. Analysis of the kinetics obtained suggests that the observed acceleration of kinetic decay at low temperature originates from an increasing rate of exciton-exciton annihilation. In order to directly probe exciton-exciton scattering processes, femtosecond 2PE signal is measured as a function of excitation fluence and temperature. Consistent with the observed enhancement of exciton-exciton scattering and annihilation at low temperatures, the dephasing rates show a correlated trend with the temperature dependence of the population lifetimes extracted from one-color pump-probe measurements.

  4. Exciton Transport and Perfect Coulomb Drag

    NASA Astrophysics Data System (ADS)

    Nandi, Debaleena

    2013-03-01

    Exciton condensation is realized in closely-spaced bilayer quantum Hall systems at νT = 1 when the total density in the two 2D electron layers matches the Landau level degeneracy. In this state, electrons in one layer become tightly bound to holes in the other layer, forming a condensate similar to the Cooper pairs in a superconductor. Being charge neutral, these excitons ought to be free to move throughout the bulk of the quantum Hall fluid. One therefore expects that electron current driven in one layer would spontaneously generate a ``hole'' current in the other layer, even in the otherwise insulating bulk of the 2D system. We demonstrate precisely this effect, using a Corbino geometry to defeat edge state transport. Our sample contains two essentially identical two-dimensional electron systems (2DES) in GaAs quantum wells separated by a thin AlGaAs barrier. It is patterned into an annulus with arms protruding from each rim that provide contact to each 2DES separately. A current drag geometry is realized by applying a drive voltage between the outer and inner rim on one 2DES layer while the two rims on the opposite layer are connected together in a closed loop. There is no direct electrical connection between the two layers. At νT = 1 the bulk of the Corbino annulus becomes insulating owing to the quantum Hall gap and net charge transport across the bulk is suppressed. Nevertheless, we find that in the drag geometry appreciable currents do flow in each layer. These currents are almost exactly equal magnitude but, crucially, flow in opposite directions. This phenomenon reflects exciton transport within the νT = 1 condensate, rather than its quasiparticle excitations. We find that quasiparticle transport competes with exciton transport at elevated temperatures, drive levels, and layer separations. This work represents a collaboration with A.D.K. Finck, J.P. Eisenstein, L.N. Pfeiffer and K.W. West. This work is supported by the NSF under grant DMR-1003080.

  5. Trion and exciton dephasing measurements in modulation-doped quantum wells: A probe for trion and carrier localization

    NASA Astrophysics Data System (ADS)

    Brinkmann, D.; Kudrna, J.; Gilliot, P.; Hönerlage, B.; Arnoult, A.; Cibert, J.; Tatarenko, S.

    1999-08-01

    To investigate the properties of a two-dimensional carrier gas at intermediate densities, we perform picosecond transient four-wave mixing experiments on trions (charged excitons) and neutral excitons in modulation p-doped CdTe/Cd1-x-yMgxZnyTe quantum wells. The determination of trion and exciton dephasing rates reveals a localization of both trions and holes in potential fluctuations induced by the ionized remote acceptors. We demonstrate that trions can be efficiently used as a charged optical probe sensitive to electrostatic potential fluctuations which are imperceptible for neutral excitons.

  6. Exciton size and binding energy limitations in one-dimensional organic materials

    SciTech Connect

    Kraner, S. Koerner, C.; Leo, K.; Scholz, R.; Plasser, F.

    2015-12-28

    In current organic photovoltaic devices, the loss in energy caused by the charge transfer step necessary for exciton dissociation leads to a low open circuit voltage, being one of the main reasons for rather low power conversion efficiencies. A possible approach to avoid these losses is to tune the exciton binding energy to a value of the order of thermal energy, which would lead to free charges upon absorption of a photon, and therefore increase the power conversion efficiency towards the Shockley-Queisser limit. We determine the size of the excitons for different organic molecules and polymers by time dependent density functional theory calculations. For optically relevant transitions, the exciton size saturates around 0.7 nm for one-dimensional molecules with a size longer than about 4 nm. For the ladder-type polymer poly(benzimidazobenzophenanthroline), we obtain an exciton binding energy of about 0.3 eV, serving as a lower limit of the exciton binding energy for the organic materials investigated. Furthermore, we show that charge transfer transitions increase the exciton size and thus identify possible routes towards a further decrease of the exciton binding energy.

  7. Identification of a triplet pair intermediate in singlet exciton fission in solution.

    PubMed

    Stern, Hannah L; Musser, Andrew J; Gelinas, Simon; Parkinson, Patrick; Herz, Laura M; Bruzek, Matthew J; Anthony, John; Friend, Richard H; Walker, Brian J

    2015-06-23

    Singlet exciton fission is the spin-conserving transformation of one spin-singlet exciton into two spin-triplet excitons. This exciton multiplication mechanism offers an attractive route to solar cells that circumvent the single-junction Shockley-Queisser limit. Most theoretical descriptions of singlet fission invoke an intermediate state of a pair of spin-triplet excitons coupled into an overall spin-singlet configuration, but such a state has never been optically observed. In solution, we show that the dynamics of fission are diffusion limited and enable the isolation of an intermediate species. In concentrated solutions of bis(triisopropylsilylethynyl)[TIPS]--tetracene we find rapid (<100 ps) formation of excimers and a slower (∼ 10 ns) break up of the excimer to two triplet exciton-bearing free molecules. These excimers are spectroscopically distinct from singlet and triplet excitons, yet possess both singlet and triplet characteristics, enabling identification as a triplet pair state. We find that this triplet pair state is significantly stabilized relative to free triplet excitons, and that it plays a critical role in the efficient endothermic singlet fission process. PMID:26060309

  8. Identification of a triplet pair intermediate in singlet exciton fission in solution

    PubMed Central

    Stern, Hannah L.; Musser, Andrew J.; Gelinas, Simon; Parkinson, Patrick; Herz, Laura M.; Bruzek, Matthew J.; Anthony, John; Friend, Richard H.; Walker, Brian J.

    2015-01-01

    Singlet exciton fission is the spin-conserving transformation of one spin-singlet exciton into two spin-triplet excitons. This exciton multiplication mechanism offers an attractive route to solar cells that circumvent the single-junction Shockley–Queisser limit. Most theoretical descriptions of singlet fission invoke an intermediate state of a pair of spin-triplet excitons coupled into an overall spin-singlet configuration, but such a state has never been optically observed. In solution, we show that the dynamics of fission are diffusion limited and enable the isolation of an intermediate species. In concentrated solutions of bis(triisopropylsilylethynyl)[TIPS]—tetracene we find rapid (<100 ps) formation of excimers and a slower (∼10 ns) break up of the excimer to two triplet exciton-bearing free molecules. These excimers are spectroscopically distinct from singlet and triplet excitons, yet possess both singlet and triplet characteristics, enabling identification as a triplet pair state. We find that this triplet pair state is significantly stabilized relative to free triplet excitons, and that it plays a critical role in the efficient endothermic singlet fission process. PMID:26060309

  9. Exciton size and binding energy limitations in one-dimensional organic materials

    NASA Astrophysics Data System (ADS)

    Kraner, S.; Scholz, R.; Plasser, F.; Koerner, C.; Leo, K.

    2015-12-01

    In current organic photovoltaic devices, the loss in energy caused by the charge transfer step necessary for exciton dissociation leads to a low open circuit voltage, being one of the main reasons for rather low power conversion efficiencies. A possible approach to avoid these losses is to tune the exciton binding energy to a value of the order of thermal energy, which would lead to free charges upon absorption of a photon, and therefore increase the power conversion efficiency towards the Shockley-Queisser limit. We determine the size of the excitons for different organic molecules and polymers by time dependent density functional theory calculations. For optically relevant transitions, the exciton size saturates around 0.7 nm for one-dimensional molecules with a size longer than about 4 nm. For the ladder-type polymer poly(benzimidazobenzophenanthroline), we obtain an exciton binding energy of about 0.3 eV, serving as a lower limit of the exciton binding energy for the organic materials investigated. Furthermore, we show that charge transfer transitions increase the exciton size and thus identify possible routes towards a further decrease of the exciton binding energy.

  10. An FBG sensor interrogation technique based on a precise optical recirculating frequency shifter driven by RF signals

    NASA Astrophysics Data System (ADS)

    Wang, Zifei; Yang, Tianxin; Jia, Dongfang; Wang, Zhaoying; Sang, Mei

    2013-03-01

    Fiber Bragg grating (FBG) sensors have numerous advantages to sense multi-physical quantities such as the temperature and strain simultaneously by monitoring the shift of the returned "Bragg" wavelength resulting from changes in these quantities. Several FBG interrogation systems have been set up using photo detectors instead of an optical spectrum analyzer (OSA) to convert wavelength to time measurements. However, in those systems, it is necessary to use mechanical tuning components to generate fast-speed wavelength-swept light sources for high-precision FBG interrogation. In this paper, a low-cost and delicate wavelength-shift detection system, without any mechanical scanning parts, is proposed and demonstrated. The wavelength scanning system is a recirculating frequency shifter (RFS) which consists of an optical amplifier, an under test FBG sensor and an optical single-sideband (SSB) modulator driven by RF signals at 10 GHz. The measurement accuracy of this system is 0.08nm.

  11. Excitons and exciton-phonon interactions in 2D MoS2 , WS2 and WSe2 studied by resonance Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Pimenta, Marcos; Del Corro, Elena; Carvalho, Bruno; Malard, Leandro; Alves, Juliana; Fantini, Cristiano; Terrones, Humberto; Elias, Ana Laura; Terrones, Mauricio

    The 2D materials exhibit a very strong exciton binding energy, and the exciton-phonon coupling plays an important role in their optical properties. Resonance Raman spectroscopy (RRS) is a very useful tool to provide information about excitons and their couplings with phonons. We will present in this work a RRS study of different samples of 2D transition metal dichalcogenides (MoS2, WS2 and WSe2) with one, two and three layers (1L, 2L, 3L) and bulk samples, using more than 30 different laser excitation lines covering the visible range. We have observed that all Raman features are enhanced by resonances with excitonic transitions. From the laser energy dependence of the Raman excitation profile (REP) we obtained the energies of the excitonic states and their dependence with the number of atomic layers.. In the case of MoS2, we observed that the electron-phonon coupling is symmetry dependent, and our results provide experimental evidence of the C exciton recently predicted theoretically. The RRS results WSe2 show that the Raman modes are enhanced by the excited excitonic states and we will present the dependence of the excited states energies on the number of layers.

  12. Coherence-mediated laser control of exciton and trion spins in CdTe/CdMgTe quantum wells studied by the magneto-optical Kerr effect.

    PubMed

    Versluis, J H; Kimel, A V; Gridnev, V N; Yakovlev, D R; Karczewski, G; Wojtowicz, T; Kossut, J; Kirilyuk, A; Rasing, Th

    2010-03-24

    Two temporally non-overlapping linearly cross-polarized 140 fs laser pulses are shown to control the spin polarization in a three-level system. Simultaneous excitation of the two excited states triggers quantum beatings originating from the interference of the wavefunctions corresponding to different spin sublevels of the states. Although the beatings are not seen in the spin densities of the excited states they are clearly observed in the magneto-optical Kerr effect. An analytical expression for the description of the beatings is obtained. Experimental results are in good agreement with theoretical predictions and demonstrate the control of beatings with attosecond resolution. PMID:21389474

  13. Aharonov-Bohm effect of excitons in nanorings

    NASA Astrophysics Data System (ADS)

    Hu, Hui; Zhu, Jia-Lin; Li, Dai-Jun; Xiong, Jia-Jiong

    2001-05-01

    The magnetic field effects on excitons in an InAs nanoring are studied theoretically. By numerically diagonalizing the effective-mass Hamiltonian of the problem that can be separated into terms in center-of-mass and relative coordinates, we calculate the low-lying excitonic energy levels and oscillator strengths as a function of the ring width and the strength of an external magnetic field. It is shown that in the presence of Coulomb correlation, the so-called Aharonov-Bohm effect of excitons exists in a finite (but small) width nanoring. However, when the ring width becomes large, the non-simply-connected geometry of nanorings is destroyed, causing the suppression of the Aharonov-Bohm effect. The analytical results are obtained for a narrow-width nanoring in which the radial motion is the fastest one and adiabatically decoupled from the azimuthal motions. The conditional probability distribution calculated for the low-lying excitonic states allows identification of the presence of the Aharonov-Bohm effect. The linear optical susceptibility is also calculated as a function of the magnetic field, to be compared with the future measurements of optical emission experiments on InAs nanorings.

  14. Excitons and charged excitons in semiconductor quantum wells

    SciTech Connect

    Riva, C.; Peeters, F. M.; Varga, K.

    2000-05-15

    A variational calculation of the ground-state energy of neutral excitons and of positively and negatively charged excitons (trions) confined in a single-quantum well is presented. We study the dependence of the correlation energy and of the binding energy on the well width and on the hole mass. The conditional probability distribution for positively and negatively charged excitons is obtained, providing information on the correlation and the charge distribution in the system. A comparison is made with available experimental data on trion binding energies in GaAs-, ZnSe-, and CdTe-based quantum well structures, which indicates that trions become localized with decreasing quantum well width. (c) 2000 The American Physical Society.

  15. Exciton transport, charge extraction, and loss mechanisms in organic photovoltaics

    NASA Astrophysics Data System (ADS)

    Scully, Shawn Ryan

    Organic photovoltaics have attracted significant interest over the last decade due to their promise as clean low-cost alternatives to large-scale electric power generation such as coal-fired power, natural gas, and nuclear power. Many believe power conversion efficiency targets of 10-15% must be reached before commercialization is possible. Consequently, understanding the loss mechanisms which currently limit efficiencies to 4-5% is crucial to identify paths to reach higher efficiencies. In this work, we investigate the dominant loss mechanisms in some of the leading organic photovoltaic architectures. In the first class of architectures, which include planar heterojunctions and bulk heterojunctions with large domains, efficiencies are primarily limited by the distance photogenerated excitations (excitons) can be transported (termed the exciton diffusion length) to a heterojunction where the excitons may dissociate. We will discuss how to properly measure the exciton diffusion length focusing on the effects of optical interference and of energy transfer when using fullerenes as quenching layers and show how this explains the variety of diffusion lengths reported for the same material. After understanding that disorder and defects limit exciton diffusion lengths, we suggest some approaches to overcome this. We then extensively investigate the use of long-range resonant energy transfer to increase exciton harvesting. Using simulations and experiments as support, we discuss how energy transfer can be engineered into architectures to increase the distance excitons can be harvested. In an experimental model system, DOW Red/PTPTB, we will show how the distance excitons are harvested can be increased by almost an order of magnitude up to 27 nm from a heterojunction and give design rules and extensions of this concept for future architectures. After understanding exciton harvesting limitations we will look at other losses that are present in planar heterojunctions. One of

  16. Ultrahigh resolution endoscopic spectral domain optical coherence tomography with a tiny rotary probe driven by a hollow ultrasonic motor

    NASA Astrophysics Data System (ADS)

    Zhang, Ning; Chen, Tianyuan; Huo, Tiancheng; Wang, Chengming; Zheng, Jing-gao; Zhou, Tieying; Xue, Ping

    2013-03-01

    This paper proposes a novel rotary endoscopic probe for spectral-domain optical coherence tomography (SD-OCT). The probe with a large N.A. objective lens is driven by an ultra-small hollow rectangular ultrasonic motor for circular scanning. Compared to the conventional driven techniques, the hollow ultrasonic motor enables the fiber to pass through its inside. Therefore the fiber, the objective lens and the motor are all at the same side. This enables 360 degree unobstructed imaging without any shadow resulted from power wire as in the conventional motor-driven endoscopic OCT. Moreover, it shortens the length of the rigid tip and enhances the flexibility of the probe. Meanwhile, the ultrasonic motor is robust, simple, quiet and of high torque, very suitable for OCT endoscopic probe. The side length of the motor is 0.7 mm with 5mm in length. The outer diameter of the probe is 1.5mm. A significant improvement in the lateral resolution is demonstrated due to the novel design of the objective lens. A right-angle lens is utilized instead of the traditional right-angle prism as the last optics close to the sample, leading to a reduction of the working distance and an enlargement of the N.A. of the objective lens. It is demonstrated that the endoscopic SD-OCT system achieves an axial resolution of ~7μm, a lateral resolution of ~6μm and a SNR of ~96dB.

  17. Intrinsic homogeneous linewidth and broadening mechanisms of excitons in monolayer transition metal dichalcogenides

    PubMed Central

    Moody, Galan; Kavir Dass, Chandriker; Hao, Kai; Chen, Chang-Hsiao; Li, Lain-Jong; Singh, Akshay; Tran, Kha; Clark, Genevieve; Xu, Xiaodong; Berghäuser, Gunnar; Malic, Ermin; Knorr, Andreas; Li, Xiaoqin

    2015-01-01

    The band-edge optical response of transition metal dichalcogenides, an emerging class of atomically thin semiconductors, is dominated by tightly bound excitons localized at the corners of the Brillouin zone (valley excitons). A fundamental yet unknown property of valley excitons in these materials is the intrinsic homogeneous linewidth, which reflects irreversible quantum dissipation arising from system (exciton) and bath (vacuum and other quasiparticles) interactions and determines the timescale during which excitons can be coherently manipulated. Here we use optical two-dimensional Fourier transform spectroscopy to measure the exciton homogeneous linewidth in monolayer tungsten diselenide (WSe2). The homogeneous linewidth is found to be nearly two orders of magnitude narrower than the inhomogeneous width at low temperatures. We evaluate quantitatively the role of exciton–exciton and exciton–phonon interactions and population relaxation as linewidth broadening mechanisms. The key insights reported here—strong many-body effects and intrinsically rapid radiative recombination—are expected to be ubiquitous in atomically thin semiconductors. PMID:26382305

  18. Tuning excitons in monolayer and few-layer MoS2

    NASA Astrophysics Data System (ADS)

    Qiu, Diana Y.; da Jornada, Felipe H.; Louie, Steven G.

    2014-03-01

    Our recent ab initio GW-BSE calculations showed that monolayer MoS2 is a computationally challenging system, requiring a large number of empty bands and very fine k-point sampling to converge its quasiparticle band structure and optical properties. Careful convergence of a GW-BSE calculation reveals that MoS2 has a large number of bound excitons with varying k-space characteristics. Specifically, there are two series of excitons: a low-energy series with k-space wavefunctions localized at the K/K' valleys in the Brillouin zone and a higher energy series localized in a ring around the Γ point. There is very little hybridization between these two exciton series in monolayer MoS2, but changes in electronic structure and screening due to additional layers, strain, or doping can lead to changes in exciton binding energies, character, and hybridization. Thus, we have carried out ab initio GW-BSE calculations to study the excitonic properties of few-layer MoS2. We find that layering and straining MoS2 systematically changes the exciton binding energies, the peak positions and amount of absorbance in the optical spectrum, and the character and hybridization of the excitons near Γ. This work was supported by NSF grant No. DMR10-1006184 and U.S. DOE under Contract No. DE-AC02-05CH11231.

  19. Entropy-based measures of in vivo cilia-driven microfluidic mixing derived from quantitative optical imaging

    NASA Astrophysics Data System (ADS)

    Chandrasekera, Kenny; Jonas, Stephan; Bhattacharya, Dipankan; Khokha, Mustafa; Choma, Michael A.

    2012-02-01

    Motile cilia are cellular organelles that project from different epithelial surfaces including respiratory epithelium. They generate directional fluid flow that removes harmful pathogens and particulate matter from the respiratory system. While it has been known that primary ciliary dyskinesia increases the risk of recurrent pulmonary infections, there is now heightened interest in understanding the role that cilia play in a wide-variety of respiratory diseases. Different optical imaging technologies are being investigated to visualize cilia-driven fluid flow, and quantitative image analysis is used to generate measures of ciliary performance. Here, we demonstrate the quantification of in vivo cilia-driven microfluidic mixing using spatial and temporal measures of Shannon information entropy. Using videomicroscopy, we imaged in vivo cilia-driven fluid flow generated by the epidermis of the Xenopus tropicalis embryo. Flow was seeded with either dyes or microparticles. Both spatial and temporal measures of entropy show significant levels of mixing, with maximum entropy measures of ~6.5 (out of a possible range of 0 to 8). Spatial entropy measures showed localization of mixing "hot-spots" and "cold-spots" and temporal measures showed mixing throughout.In sum, entropy-based measures of microfluidic mixing can characterize in vivo cilia-driven fluid flow and hold the potential for better characterization of ciliary dysfunction.

  20. Determination of the Exciton Binding Energy in CdSe Quantum Dots

    SciTech Connect

    Meulenberg, R; Lee, J; Wolcott, A; Zhang, J; Terminello, L; van Buuren, T

    2009-10-27

    The exciton binding energy (EBE) in CdSe quantum dots (QDs) has been determined using x-ray spectroscopy. Using x-ray absorption and photoemission spectroscopy, the conduction band (CB) and valence band (VB) edge shifts as a function of particle size have been determined and combined to obtain the true band gap of the QDs (i.e. without and exciton). These values can be compared to the excitonic gap obtained using optical spectroscopy to determine the EBE. The experimental EBE results are compared with theoretical calculations on the EBE and show excellent agreement.

  1. Geminate and nongeminate recombination of triplet excitons formed by singlet fission.

    PubMed

    Bayliss, Sam L; Chepelianskii, Alexei D; Sepe, Alessandro; Walker, Brian J; Ehrler, Bruno; Bruzek, Matthew J; Anthony, John E; Greenham, Neil C

    2014-06-13

    We report the simultaneous observation of geminate and nongeminate triplet-triplet annihilation in a solution-processable small molecule TIPS-tetracene undergoing singlet exciton fission. Using optically detected magnetic resonance, we identify recombination of triplet pairs directly following singlet fission, as well as recombination of triplet excitons undergoing bimolecular triplet-triplet annihilation. We show that the two processes give rise to distinct magnetic resonance spectra, and estimate the interaction between geminate triplet excitons to be 60 neV. PMID:24972236

  2. Electric-Field Induced Activation of Dark Excitonic States in Carbon Nanotubes.

    PubMed

    Uda, T; Yoshida, M; Ishii, A; Kato, Y K

    2016-04-13

    Electrical activation of optical transitions to parity-forbidden dark excitonic states in individual carbon nanotubes is reported. We examine electric-field effects on various excitonic states by simultaneously measuring photocurrent and photoluminescence. As the applied field increases, we observe an emergence of new absorption peaks in the excitation spectra. From the diameter dependence of the energy separation between the new peaks and the ground state of E11 excitons, we attribute the peaks to the dark excited states which became optically active due to the applied field. Field-induced exciton dissociation can explain the photocurrent threshold field, and the edge of the E11 continuum states has been identified by extrapolating to zero threshold. PMID:26999284

  3. Ab-initio calculation of excitons in conventional and anorganic semiconductors

    NASA Astrophysics Data System (ADS)

    Ambrosch-Draxl, Claudia; Laskowsky, Robert

    2005-03-01

    The excitonic effects on the optical absorption properties of organic as well as inorganic semiconductors are studied from first-principles. The Coulomb interaction between the electron and the hole is accounted for by solving the two-particle Bethe-Salpeter equation. In the organic semiconductors the exciton binding energies strongly depend on the molecular size, the crystalline packing, as well as the polarization direction of the incoming light. We show that the electron-hole interaction can lead to strongly bound excitons with binding energies of the order of 1eV or to a mere redistribution of oscillator strength. In several cases, the screening is efficient enough such that free charge carriers govern the optical absorption process. In the inorganic counterparts the sensitivity of the exciton binding energy is tested against the structural parameters and the screening of the electron-hole Coulomb interaction.

  4. Talbot Effect for Exciton Polaritons.

    PubMed

    Gao, T; Estrecho, E; Li, G; Egorov, O A; Ma, X; Winkler, K; Kamp, M; Schneider, C; Höfling, S; Truscott, A G; Ostrovskaya, E A

    2016-08-26

    We demonstrate, experimentally and theoretically, a Talbot effect for hybrid light-matter waves-an exciton-polariton condensate formed in a semiconductor microcavity with embedded quantum wells. The characteristic "Talbot carpet" is produced by loading the exciton-polariton condensate into a microstructured one-dimensional periodic array of mesa traps, which creates an array of phase-locked sources for coherent polariton flow in the plane of the quantum wells. The spatial distribution of the Talbot fringes outside the mesas mimics the near-field diffraction of a monochromatic wave on a periodic amplitude and phase grating with the grating period comparable to the wavelength. Despite the lossy nature of the polariton system, the Talbot pattern persists for distances exceeding the size of the mesas by an order of magnitude. Thus, our experiment demonstrates efficient shaping of the two-dimensional flow of coherent exciton polaritons by a one-dimensional "flat lens." PMID:27610883

  5. Exciton coupling in molecular crystals

    NASA Technical Reports Server (NTRS)

    Ake, R. L.

    1976-01-01

    The implications of perfect exciton coupling and molecular vibrations were investigated, as well as the effect they have on the lifetime of singlet and triplet excitons coupled in a limiting geometry. Crystalline bibenzyl, Cl4Hl4, provided a situation in which these mechanisms involving exciton coupling can be studied in the limit of perfect coupling between units due to the crystal's geometry. This geometry leads to a coupling between the two halves of the molecule resulting in a splitting of the molecular excited states. The study reported involves an experimental spectroscopic approach and begins with the purification of the bibenzyl. The principal experimental apparatus was an emission spectrometer. A closed cycle cryogenic system was used to vary the temperature of the sample between 20 K and 300 K. The desired results are the temperature-dependent emission spectra of the bibenzyl; in addition, the lifetimes and quantum yields measured at each temperature reveal the effect of competing radiationless processes.

  6. Electrical Control of Exciton-Enhanced Second-Harmonic Generation in Monolayer WSe2

    NASA Astrophysics Data System (ADS)

    Seyler, Kyle; Schaibley, John; Gong, Pu; Rivera, Pasqual; Jones, Aaron; Wu, Sanfeng; Yan, Jiaqiang; Mandrus, David; Yao, Wang; Xu, Xiaodong

    2015-03-01

    Nonlinear optical frequency conversion, in which optical fields interact with a nonlinear medium to produce new field frequencies, is ubiquitous in modern photonic systems. However, the nonlinear electric susceptibilities that give rise to such phenomena are often challenging to tune in a given material, and so far, dynamical control of optical nonlinearities remains confined to research labs. In this talk, we report a new mechanism to electrically control second-order optical nonlinearities in monolayer WSe2. We show that the intensity of second-harmonic generation (SHG) at its lowest exciton resonance is widely tunable through electrostatic doping in a field-effect transistor device. Such remarkable tunability arises from the strong exciton charging effects in monolayer semiconductors, which allow for exceptional control over the exciton and trion oscillator strengths. Our study paves the way for a new platform of chip-scale, electrically tunable nonlinear optical devices based on two-dimensional semiconductors.

  7. Excitons and charges at organic semiconductor heterojunctions.

    PubMed

    Friend, Richard H; Phillips, Matthew; Rao, Akshay; Wilson, Mark W B; Li, Zhe; McNeill, Christopher R

    2012-01-01

    All-organic heterojunction solar cells now provide very high quantum efficiencies for charge generation and rapidly-improving power conversion efficiencies. Charge generation and separation however, must overcome the strong Coulomb interactions between electrons and holes in these materials that is manifest also through the large exchange energies usually observed. We show for a polymer-polymer system with low charge generation efficiency that this arises through intersystem crossing from the photogenerated charge-transfer state to a lower lying triplet state, mediated by the proton hyperfine interaction, and that the activation barrier for full separation of electrons and holes is of the order of 250 meV. We observe, using transient optical spectroscopy, the processes of charge separation, recombination and sweep-out in efficient polymer-fullerene devices. We report also on the process of singlet exciton fission to form a pair of triplet excitons in pentacene that can later be dissociated against a heterojunction formed with C60. PMID:22470984

  8. Exciton-photon correlations in bosonic condensates of exciton-polaritons

    PubMed Central

    Kavokin, Alexey V.; Sheremet, Alexandra S.; Shelykh, Ivan A.; Lagoudakis, Pavlos G.; Rubo, Yuri G.

    2015-01-01

    Exciton-polaritons are mixed light-matter quasiparticles. We have developed a statistical model describing stochastic exciton-photon transitions within a condensate of exciton polaritons. We show that the exciton-photon correlator depends on the rate of incoherent exciton-photon transformations in the condensate. We discuss implications of this effect for the quantum statistics of photons emitted by polariton lasers. PMID:26153979

  9. Exciton-photon correlations in bosonic condensates of exciton-polaritons.

    PubMed

    Kavokin, Alexey V; Sheremet, Alexandra S; Shelykh, Ivan A; Lagoudakis, Pavlos G; Rubo, Yuri G

    2015-01-01

    Exciton-polaritons are mixed light-matter quasiparticles. We have developed a statistical model describing stochastic exciton-photon transitions within a condensate of exciton polaritons. We show that the exciton-photon correlator depends on the rate of incoherent exciton-photon transformations in the condensate. We discuss implications of this effect for the quantum statistics of photons emitted by polariton lasers. PMID:26153979

  10. Electronic structure and absorption spectrum of biexciton obtained by using exciton basis

    SciTech Connect

    Shiau, Shiue-Yuan; Combescot, Monique; Chang, Yia-Chung

    2013-09-15

    We approach the biexciton Schrödinger equation not through the free-carrier basis as usually done, but through the free-exciton basis, exciton–exciton interactions being treated according to the recently developed composite boson many-body formalism which allows an exact handling of carrier exchange between excitons, as induced by the Pauli exclusion principle. We numerically solve the resulting biexciton Schrödinger equation with the exciton levels restricted to the ground state and we derive the biexciton ground state as well as the bound and unbound excited states as a function of hole-to-electron mass ratio. The biexciton ground-state energy we find, agrees reasonably well with variational results. Next, we use the obtained biexciton wave functions to calculate optical absorption in the presence of a dilute exciton gas in quantum well. We find an asymmetric peak with a characteristic low-energy tail, identified with the biexciton ground state, and a set of Lorentzian-like peaks associated with biexciton unbound states, i.e., exciton–exciton scattering states. Last, we propose a pump–probe experiment to probe the momentum distribution of the exciton condensate. -- Highlights: •New composite boson many-body theory is used to derive exactly the biexciton Schrödinger equation using the exciton basis. •We solved the 2D and 3D biexciton ground- and excited-state binding energies for various electron-to-hole mass ratios. •The absorption spectrum shows an asymmetric low-energy peak identified with the biexciton ground state. •High-energy Lorentzian-like peaks in the absorption spectrum are associated with the exciton–exciton scattering states. •The exciton gas momentum distribution can be determined by the absorption spectrum via the biexciton wave functions.

  11. Charge-transfer excitations steer the Davydov splitting and mediate singlet exciton fission in pentacene.

    PubMed

    Beljonne, D; Yamagata, H; Brédas, J L; Spano, F C; Olivier, Y

    2013-05-31

    Quantum-chemical calculations are combined to a model Frenkel-Holstein Hamiltonian to assess the nature of the lowest electronic excitations in the pentacene crystal. We show that an admixture of charge-transfer excitations into the lowest singlet excited states form the origin of the Davydov splitting and mediate instantaneous singlet exciton fission by direct optical excitation of coherently coupled single and double exciton states, in agreement with recent experiments. PMID:23767738

  12. Charge-Transfer Excitations Steer the Davydov Splitting and Mediate Singlet Exciton Fission in Pentacene

    NASA Astrophysics Data System (ADS)

    Beljonne, D.; Yamagata, H.; Brédas, J. L.; Spano, F. C.; Olivier, Y.

    2013-05-01

    Quantum-chemical calculations are combined to a model Frenkel-Holstein Hamiltonian to assess the nature of the lowest electronic excitations in the pentacene crystal. We show that an admixture of charge-transfer excitations into the lowest singlet excited states form the origin of the Davydov splitting and mediate instantaneous singlet exciton fission by direct optical excitation of coherently coupled single and double exciton states, in agreement with recent experiments.

  13. Resonant surface plasmon-exciton interaction in hybrid MoSe2@Au nanostructures

    NASA Astrophysics Data System (ADS)

    Abid, I.; Bohloul, A.; Najmaei, S.; Avendano, C.; Liu, H.-L.; Péchou, R.; Mlayah, A.; Lou, J.

    2016-04-01

    In this work we investigate the interaction between plasmonic and excitonic resonances in hybrid MoSe2@Au nanostructures. The latter were fabricated by combining chemical vapor deposition of MoSe2 atomic layers, Au disk processing by nanosphere lithography and a soft lift-off/transfer technique. The samples were characterized by scanning electron and atomic force microscopy. Their optical properties were investigated experimentally using optical absorption, Raman scattering and photoluminescence spectroscopy. The work is focused on a resonant situation where the surface plasmon resonance is tuned to the excitonic transition. In that case, the near-field interaction between the surface plasmons and the confined excitons leads to interference between the plasmonic and excitonic resonances that manifests in the optical spectra as a transparency dip. The plasmonic-excitonic interaction regime is determined using quantitative analysis of the optical extinction spectra based on an analytical model supported by numerical simulations. We found that the plasmonic-excitonic resonances do interfere thus leading to a typical Fano lineshape of the optical extinction. The near-field nature of the plasmonic-excitonic interaction is pointed out experimentally from the dependence of the optical absorption on the number of monolayer stacks on the Au nanodisks. The results presented in this work contribute to the development of new concepts in the field of hybrid plasmonics.In this work we investigate the interaction between plasmonic and excitonic resonances in hybrid MoSe2@Au nanostructures. The latter were fabricated by combining chemical vapor deposition of MoSe2 atomic layers, Au disk processing by nanosphere lithography and a soft lift-off/transfer technique. The samples were characterized by scanning electron and atomic force microscopy. Their optical properties were investigated experimentally using optical absorption, Raman scattering and photoluminescence spectroscopy. The

  14. Laser-optical path to nuclear energy without radioactivity: Fusion of hydrogen-boron by nonlinear force driven plasma blocks

    NASA Astrophysics Data System (ADS)

    Hora, H.; Miley, G. H.; Ghoranneviss, M.; Malekynia, B.; Azizi, N.

    2009-10-01

    Anomalous interaction of terawatt-picosecond laser pulses allows side-on ignition of solid state density fusion fuel with the unexpected possibility of igniting uncompressed hydrogen-boron p- 11B. Suppression of relativistic self-focusing by using very clean laser pulses with an extremely high contrast ratio is essential to achieve ignition thresholds only ten times more difficult than fusion of deuterium-tritium (DT). This opens the possibility for laser driven fusion energy without neutrons and less radioactivity than from burning coal. The complex nonlinear optical properties involved are elaborated.

  15. Low noise and low drift in a laser-driven fiber optic gyroscope with a 1-km coil

    NASA Astrophysics Data System (ADS)

    Chamoun, J. N.; Evans, A.; Mosca, F. A.; Digonnet, M. J. F.

    2014-05-01

    We report an experimental fiber optic gyroscope (FOG) utilizing a 1085-m coil of 8-cm diameter driven with a laser of 10- MHz linewidth, with a record rotation-rate noise as low as 0.2 deg/h/√Hz and a drift below 0.038 deg/h. Simulations and comparison to the measured performance of a similar 150-m FOG show that the noise is limited approximately equally by coherent backscattering and polarization coupling in the sensing coil, and unaffected by the Kerr effect.

  16. Ab Initio study of multiple exciton generation in layered structure quantum dots

    NASA Astrophysics Data System (ADS)

    Zhang, Zhiyong; Zimmerman, Paul; Cui, Yi; Musgrave, Charles

    2011-03-01

    Multiple Exciton Generation (MEG) can potentially increase the photovoltaic conversion efficiency significantly and has been reported in a large number of systems and has been extensively studies theoretically and experimentally. Here we report our study of the MEG process in inorganic layered structure quantum dots using high level Ab Initio methods that are capable of electronic states of multi-exciton in character. Our results show that multiple states that are of multi-exciton character exist in quantum dots and different mechanisms govern the MEG process in quantum dots: (1) MEG through an internal crossing mechanism from a optically active state to an optically dark multi-exciton state, as in the singlet fission process of pentacene; and (2) direct multi-exciton generation through an optically active excited state. We also discuss detailed structure evolution of quantum dots, from stable molecular like structures of various shapes and sizes, to larger quantum dots of bulk like bonding motifs with distinctive surface structures and illustrate the correlation between structure and the multi-exciton states.

  17. Singlet Fission and Multi-Exciton Generation in Organic Systems

    NASA Astrophysics Data System (ADS)

    Musgrave, Charles

    2012-02-01

    Multi-exciton generation (MEG) has been observed in a variety of materials and might be exploited in solar-cells to dramatically increase efficiency. In tetracene and pentacene MEG has been attributed to singlet fission (SF), however a fundamental mechanism for SF has not been previously described. Here, we use sophisticated ab initio calculations to show that MEG in pentacene proceeds by transition of the lowest optically allowed excited state S1 to a dark state (D) of multi-exciton character, which subsequently undergoes SF to generate two triplets (2xT0). D satisfies the energy requirement for SF (ED>2ET0) and lies just below S1 in pentacene, but above S1 in tetracene, consistent with the observed thermally activated SF process in tetracene, but no thermal activation in pentacene. While S1 exhibits single exciton character, D shows multi-exciton character comprising two separated electron-hole pairs. Dimer simulations predict S1 excimer formation and that fission of D into triplets proceeds through the excimer. The predicted energetics, wavefunctions and excimer interaction support the proposed mechanism, which accounts for the observed rapid, unactivated SF in pentacene. Results for SF in polyacenes, grapheme nanoribbons, rubrene and carbon nanotubes will be presented.

  18. Highly anisotropic and robust excitons in monolayer black phosphorus.

    PubMed

    Wang, Xiaomu; Jones, Aaron M; Seyler, Kyle L; Tran, Vy; Jia, Yichen; Zhao, Huan; Wang, Han; Yang, Li; Xu, Xiaodong; Xia, Fengnian

    2015-06-01

    Semi-metallic graphene and semiconducting monolayer transition-metal dichalcogenides are the most intensively studied two-dimensional materials of recent years. Lately, black phosphorus has emerged as a promising new two-dimensional material due to its widely tunable and direct bandgap, high carrier mobility and remarkable in-plane anisotropic electrical, optical and phonon properties. However, current progress is primarily limited to its thin-film form. Here, we reveal highly anisotropic and strongly bound excitons in monolayer black phosphorus using polarization-resolved photoluminescence measurements at room temperature. We show that, regardless of the excitation laser polarization, the emitted light from the monolayer is linearly polarized along the light effective mass direction and centres around 1.3 eV, a clear signature of emission from highly anisotropic bright excitons. Moreover, photoluminescence excitation spectroscopy suggests a quasiparticle bandgap of 2.2 eV, from which we estimate an exciton binding energy of ∼0.9 eV, consistent with theoretical results based on first principles. The experimental observation of highly anisotropic, bright excitons with large binding energy not only opens avenues for the future explorations of many-electron physics in this unusual two-dimensional material, but also suggests its promising future in optoelectronic devices. PMID:25915195

  19. Exciton-polariton condensation in transition metal dichalcogenide bilayer heterostructure

    NASA Astrophysics Data System (ADS)

    Lee, Ki Hoon; Jeong, Jae-Seung; Min, Hongki; Chung, Suk Bum

    For the bilayer heterostructure system in an optical microcavity, the interplay of the Coulomb interaction and the electron-photon coupling can lead to the emergence of quasiparticles consisting of the spatially indirect exciton and cavity photons known as dipolariton, which can form the Bose-Einstein condensate above a threshold density. Additional physics comes into play when each layer of the bilayer system consists of the transition metal dichalcogenide (TMD) monolayer. The TMD monolayer band structure in the low energy spectrum has two valley components with nontrivial Berry phase, which gives rise to a selection rule in the exciton-polariton coupling, e.g. the exciton from one (the other) valley can couple only to the clockwise (counter-clockwise) polarized photon. We investigate possible condensate phases of exciton-polariton in the bilayer TMD microcavity changing relevant parameters such as detuning, excitation density and interlayer distance. This work was supported in part by the Institute for Basic Science of Korea (IBS) under Grant IBS-R009-Y1 and by the National Research Foundation of Korea (NRF) under the Basic Science Research Program Grant No. 2015R1D1A1A01058071.

  20. Strong Quantum Coherence between Fermi Liquid Mahan Excitons.

    PubMed

    Paul, J; Stevens, C E; Liu, C; Dey, P; McIntyre, C; Turkowski, V; Reno, J L; Hilton, D J; Karaiskaj, D

    2016-04-15

    In modulation doped quantum wells, the excitons are formed as a result of the interactions of the charged holes with the electrons at the Fermi edge in the conduction band, leading to the so-called "Mahan excitons." The binding energy of Mahan excitons is expected to be greatly reduced and any quantum coherence destroyed as a result of the screening and electron-electron interactions. Surprisingly, we observe strong quantum coherence between the heavy hole and light hole excitons. Such correlations are revealed by the dominating cross-diagonal peaks in both one-quantum and two-quantum two-dimensional Fourier transform spectra. Theoretical simulations based on the optical Bloch equations where many-body effects are included phenomenologically reproduce well the experimental spectra. Time-dependent density functional theory calculations provide insight into the underlying physics and attribute the observed strong quantum coherence to a significantly reduced screening length and collective excitations of the many-electron system. PMID:27127985

  1. Highly anisotropic and robust excitons in monolayer black phosphorus

    NASA Astrophysics Data System (ADS)

    Wang, Xiaomu; Jones, Aaron M.; Seyler, Kyle L.; Tran, Vy; Jia, Yichen; Zhao, Huan; Wang, Han; Yang, Li; Xu, Xiaodong; Xia, Fengnian

    2015-06-01

    Semi-metallic graphene and semiconducting monolayer transition-metal dichalcogenides are the most intensively studied two-dimensional materials of recent years. Lately, black phosphorus has emerged as a promising new two-dimensional material due to its widely tunable and direct bandgap, high carrier mobility and remarkable in-plane anisotropic electrical, optical and phonon properties. However, current progress is primarily limited to its thin-film form. Here, we reveal highly anisotropic and strongly bound excitons in monolayer black phosphorus using polarization-resolved photoluminescence measurements at room temperature. We show that, regardless of the excitation laser polarization, the emitted light from the monolayer is linearly polarized along the light effective mass direction and centres around 1.3 eV, a clear signature of emission from highly anisotropic bright excitons. Moreover, photoluminescence excitation spectroscopy suggests a quasiparticle bandgap of 2.2 eV, from which we estimate an exciton binding energy of ∼0.9 eV, consistent with theoretical results based on first principles. The experimental observation of highly anisotropic, bright excitons with large binding energy not only opens avenues for the future explorations of many-electron physics in this unusual two-dimensional material, but also suggests its promising future in optoelectronic devices.

  2. Exciton radiative lifetimes in two-dimensional transition metal dichalcogenides.

    PubMed

    Palummo, Maurizia; Bernardi, Marco; Grossman, Jeffrey C

    2015-05-13

    Light emission in two-dimensional (2D) transition metal dichalcogenides (TMDs) changes significantly with the number of layers and stacking sequence. While the electronic structure and optical absorption are well understood in 2D-TMDs, much less is known about exciton dynamics and radiative recombination. Here, we show first-principles calculations of intrinsic exciton radiative lifetimes at low temperature (4 K) and room temperature (300 K) in TMD monolayers with the chemical formula MX2 (X = Mo, W, and X = S, Se), as well as in bilayer and bulk MoS2 and in two MX2 heterobilayers. Our results elucidate the time scale and microscopic origin of light emission in TMDs. We find radiative lifetimes of a few picoseconds at low temperature and a few nanoseconds at room temperature in the monolayers and slower radiative recombination in bulk and bilayer than in monolayer MoS2. The MoS2/WS2 and MoSe2/WSe2 heterobilayers exhibit very long-lived (∼20-30 ns at room temperature) interlayer excitons constituted by electrons localized on the Mo-based and holes on the W-based monolayer. The wide radiative lifetime tunability, together with the ability shown here to predict radiative lifetimes from computations, hold unique potential to manipulate excitons in TMDs and their heterostructures for application in optoelectronics and solar energy conversion. PMID:25798735

  3. Excitons and Davydov splitting in sexithiophene from first-principles many-body Green's function theory

    NASA Astrophysics Data System (ADS)

    Leng, Xia; Yin, Huabing; Liang, Dongmei; Ma, Yuchen

    2015-09-01

    Organic semiconductors have promising and broad applications in optoelectronics. Understanding their electronic excited states is important to help us control their spectroscopic properties and performance of devices. There have been a large amount of experimental investigations on spectroscopies of organic semiconductors, but theoretical calculation from first principles on this respect is still limited. Here, we use density functional theory (DFT) and many-body Green's function theory, which includes the GW method and Bethe-Salpeter equation, to study the electronic excited-state properties and spectroscopies of one prototypical organic semiconductor, sexithiophene. The exciton energies of sexithiophene in both the gas and bulk crystalline phases are very sensitive to the exchange-correlation functionals used in DFT for ground-state structure relaxation. We investigated the influence of dynamical screening in the electron-hole interaction on exciton energies, which is found to be very pronounced for triplet excitons and has to be taken into account in first principles calculations. In the sexithiophene single crystal, the energy of the lowest triplet exciton is close to half the energy of the lowest singlet one. While lower-energy singlet and triplet excitons are intramolecular Frenkel excitons, higher-energy excitons are of intermolecular charge-transfer type. The calculated optical absorption spectra and Davydov splitting are in good agreement with experiments.

  4. Low-temperature exciton absorption in InSe under pressure

    NASA Astrophysics Data System (ADS)

    Goi, A. R.; Cantarero, A.; Schwarz, U.; Syassen, K.; Chevy, A.

    1992-02-01

    We have investigated the effect of pressure on the lowest direct band-edge exciton of the layered semiconductor InSe by optical-absorption measurements at 10 K and for pressures up to 4 GPa. The Elliott-Toyozawa formalism is used to analyze the line shape of the exciton absorption spectra. In this way we determine the pressure dependence of the lowest direct band gap, the exciton binding energy, and the exciton linewidth. The band gap exhibits a pronounced nonlinear shift with pressure, which is a consequence of the strong anisotropy of intralayer and interlayer bonding. The exciton binding energy decreases with pressure, mainly due to the large increase of the low-frequency dielectric constant parallel to the c axis. The reversible broadening of the exciton line with pressure is related to phonon-assisted scattering of electrons into lower-lying indirect-gap states. From the pressure dependence of the exciton linewidth, we determine the magnitude of the related intervalley-deformation-potential constant.

  5. Effect of pressure on the low-temperature exciton absorption in GaAs

    NASA Astrophysics Data System (ADS)

    Goi, A. R.; Cantarero, A.; Syassen, K.; Cardona, M.

    1990-05-01

    We have measured low-temperature exciton optical-absorption spectra at the lowest direct band edge (E0) of GaAs as a function of pressure up to 9 GPa. Spectra are analyzed in terms of the Elliott model by taking into account the broadening of the exciton line. In this way, we determine the dependence on pressure of the E0 gap, the exciton binding energy scrR, and exciton linewidth at different temperatures. The pressure coefficient of the E0 fundamental gap [107(4) meV/GPa] is found to be independent of temperature. The exciton binding energy increases with pressure at a rate of d lnscrR/dP=0.083(3) GPa-1. The exciton lifetime becomes smaller for pressures above the crossover between Γ- and X-point conduction-band minima (P>4.2 GPa), a fact which is attributed to phonon-assisted intervalley scattering. From the pressure dependence of the exciton linewidth we determine an accurate value for the intervalley deformation-potential constant DΓX=4.8(3) eV/Å.

  6. Polycrystalline magnetic garnet films comprising weakly coupled crystallites for piezoelectrically-driven magneto-optic spatial light modulators

    SciTech Connect

    Mito, S.; Sakurai, H.; Takagi, H.; Inoue, M.; Baryshev, A. V.

    2012-04-01

    We have investigated the magnetization process of the polycrystalline magnetic garnet films in order to determine the most suitable composition of garnet films for piezoelectrically-driven magneto-optic spatial light modulators (MOSLMs). For experiment, the bismuth-dysprosium-aluminum-substituted yttrium iron (Bi{sub 1.3}Dy{sub 0.7}Y{sub 1.0}Fe{sub 3.1}Al{sub 1.9}O{sub 12}) garnet films were deposited by an RF magnetron sputter and annealed at 700 deg. C in air. The annealing time was varied in a range of several minutes to control the grain size. The saturation magnetization, the remanent magnetization and the composition of the fabricated garnet films slightly changed versus the annealing time. Experiments showed that the coercivity and the grain size increased at longer annealing; the coercivity was larger for films with bigger grains. This work shows that garnet films with smaller coercivity are most suitable for controlling the magnetization of garnet and, correspondingly, the magneto-optical rotation of MOSLM pixels driven by piezoelectrics.

  7. Exciton-polariton state in nanocrystalline SiC films

    NASA Astrophysics Data System (ADS)

    Semenov, А. V.; Lopin, А. V.

    2016-05-01

    We studied the features of optical absorption in the films of nanocrystalline SiC (nc-SiC) obtained on the sapphire substrates by the method of direct ion deposition. The optical absorption spectra of the films with a thickness less than ~500 nm contain a maximum which position and intensity depend on the structure and thickness of the nc-SiC films. The most intense peak at 2.36 eV is observed in the nc-SiC film with predominant 3C-SiC polytype structure and a thickness of 392 nm. Proposed is a resonance absorption model based on excitation of exciton polaritons in a microcavity. In the latter, under the conditions of resonance, there occurs strong interaction between photon modes of light with λph=521 nm and exciton of the 3С polytype with an excitation energy of 2.36 eV that results in the formation of polariton. A mismatch of the frequencies of photon modes of the cavity and exciton explains the dependence of the maximum of the optical absorption on the film thickness.

  8. Exciton dynamics of C60-based single-photon emitters explored by Hanbury Brown–Twiss scanning tunnelling microscopy

    PubMed Central

    Merino, P.; Große, C.; Rosławska, A.; Kuhnke, K.; Kern, K.

    2015-01-01

    Exciton creation and annihilation by charges are crucial processes for technologies relying on charge-exciton-photon conversion. Improvement of organic light sources or dye-sensitized solar cells requires methods to address exciton dynamics at the molecular scale. Near-field techniques have been instrumental for this purpose; however, characterizing exciton recombination with molecular resolution remained a challenge. Here, we study exciton dynamics by using scanning tunnelling microscopy to inject current with sub-molecular precision and Hanbury Brown–Twiss interferometry to measure photon correlations in the far-field electroluminescence. Controlled injection allows us to generate excitons in solid C60 and let them interact with charges during their lifetime. We demonstrate electrically driven single-photon emission from localized structural defects and determine exciton lifetimes in the picosecond range. Monitoring lifetime shortening and luminescence saturation for increasing carrier injection rates provides access to charge-exciton annihilation dynamics. Our approach introduces a unique way to study single quasi-particle dynamics on the ultimate molecular scale. PMID:26416705

  9. Exciton dynamics of C60-based single-photon emitters explored by Hanbury Brown-Twiss scanning tunnelling microscopy

    NASA Astrophysics Data System (ADS)

    Merino, P.; Große, C.; Rosławska, A.; Kuhnke, K.; Kern, K.

    2015-09-01

    Exciton creation and annihilation by charges are crucial processes for technologies relying on charge-exciton-photon conversion. Improvement of organic light sources or dye-sensitized solar cells requires methods to address exciton dynamics at the molecular scale. Near-field techniques have been instrumental for this purpose; however, characterizing exciton recombination with molecular resolution remained a challenge. Here, we study exciton dynamics by using scanning tunnelling microscopy to inject current with sub-molecular precision and Hanbury Brown-Twiss interferometry to measure photon correlations in the far-field electroluminescence. Controlled injection allows us to generate excitons in solid C60 and let them interact with charges during their lifetime. We demonstrate electrically driven single-photon emission from localized structural defects and determine exciton lifetimes in the picosecond range. Monitoring lifetime shortening and luminescence saturation for increasing carrier injection rates provides access to charge-exciton annihilation dynamics. Our approach introduces a unique way to study single quasi-particle dynamics on the ultimate molecular scale.

  10. Steering, splitting, and cloning of an optical beam in a coherently driven Raman gain system

    NASA Astrophysics Data System (ADS)

    Verma, Onkar N.; Dey, Tarak N.

    2015-01-01

    We propose an all-optical antiwaveguide mechanism for steering, splitting, and cloning of an optical beam without diffraction. We use a spatially inhomogeneous pump beam to create an antiwaveguide structure in a Doppler broadened N -type four-level Raman gain medium for a copropagating weak probe beam. We show that a transverse modulated index of refraction and gain due to the spatially dependent pump beam hold the keys to steering, splitting, and cloning of an optical beam. We have also shown that an additional control field permits the propagation of an optical beam through an otherwise gain medium without diffraction and instability. We further discuss how finesse of the cloned images can be increased by changing the detuning of the control field. We arrive at similar results by using homogeneously broadened gain media at higher density.

  11. Fast optical frequency sweeping using voltage controlled oscillator driven single sideband modulation combined with injection locking.

    PubMed

    Wang, Jian; Chen, Dijun; Cai, Haiwen; Wei, Fang; Qu, Ronghui

    2015-03-23

    An ultrafast optical frequency sweeping technique for narrow linewidth lasers is reported. This technique exploits the large frequency modulation bandwidth of a wideband voltage controlled oscillator (VCO) and a high speed electro-optic dual parallel Mach-Zehnder modulator (DPMZM) which works on the state of carrier suppressed single sideband modulation(CS-SSB). Optical frequency sweeping of a narrow linewidth fiber laser with 3.85 GHz sweeping range and 80 GHz/μs tuning speed is demonstrated, which is an extremely high tuning speed for frequency sweeping of narrow linewidth lasers. In addition, injection locking technique is adopted to improve the sweeper's low optical power output and small side-mode suppression ratio (SMSR). PMID:25837048

  12. External quantum efficiency exceeding 100% in a singlet-exciton-fission-based solar cell

    NASA Astrophysics Data System (ADS)

    Baldo, Marc

    2013-03-01

    Singlet exciton fission can be used to split a molecular excited state in two. In solar cells, it promises to double the photocurrent from high energy photons, thereby breaking the single junction efficiency limit. We demonstrate organic solar cells that exploit singlet exciton fission in pentacene to generate more than one electron per incident photon in the visible spectrum. Using a fullerene acceptor, a poly(3-hexylthiophene) exciton confinement layer, and a conventional optical trapping scheme, the peak external quantum efficiency is (109 +/-1)% at λ = 670 nm for a 15-nm-thick pentacene film. The corresponding internal quantum efficiency is (160 +/-10)%. Independent confirmation of the high internal efficiency is obtained by analysis of the magnetic field effect on photocurrent, which determines that the triplet yield approaches 200% for pentacene films thicker than 5 nm. To our knowledge, this is the first solar cell to generate quantum efficiencies above 100% in the visible spectrum. Alternative multiple exciton generation approaches have been demonstrated previously in the ultraviolet, where there is relatively little sunlight. Singlet exciton fission differs from these other mechanisms because spin conservation disallows the usual dominant loss process: a thermal relaxation of the high-energy exciton into a single low-energy exciton. Consequently, pentacene is efficient in the visible spectrum at λ = 670 nm because only the collapse of the singlet exciton into twotriplets is spin-allowed. Supported as part of the Center for Excitonics, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number DE-SC0001088.

  13. Photonic Crystal Architecture for Room-Temperature Equilibrium Bose-Einstein Condensation of Exciton Polaritons

    NASA Astrophysics Data System (ADS)

    Jiang, Jian-Hua; John, Sajeev

    2014-07-01

    We describe photonic crystal microcavities with very strong light-matter interaction to realize room-temperature, equilibrium, exciton-polariton Bose-Einstein condensation (BEC). This goal is achieved through a careful balance between strong light trapping in a photonic band gap (PBG) and large exciton density enabled by a multiple quantum-well (QW) structure with a moderate dielectric constant. This approach enables the formation of a long-lived, dense 10-μm-1-cm- scale cloud of exciton polaritons with vacuum Rabi splitting that is roughly 7% of the bare exciton-recombination energy. We introduce a woodpile photonic crystal made of Cd0.6 Mg0.4Te with a 3D PBG of 9.2% (gap-to-central-frequency ratio) that strongly focuses a planar guided optical field on CdTe QWs in the cavity. For 3-nm QWs with 5-nm barrier width, the exciton-photon coupling can be as large as ℏΩ=55 meV (i.e., a vacuum Rabi splitting of 2ℏΩ=110 meV). The exciton-recombination energy of 1.65 eV corresponds to an optical wavelength of 750 nm. For N =106 QWs embedded in the cavity, the collective exciton-photon coupling per QW (ℏΩ/√N =5.4 meV) is much larger than the state-of-the-art value of 3.3 meV, for the CdTe Fabry-Pérot microcavity. The maximum BEC temperature is limited by the depth of the dispersion minimum for the lower polariton branch, over which the polariton has a small effective mass of approximately 10-5m0, where m0 is the electron mass in vacuum. By detuning the bare exciton-recombination energy above the planar guided optical mode, a larger dispersion depth is achieved, enabling room-temperature BEC. The BEC transition temperature ranges as high as 500 K when the polariton density per QW is increased to (11aB)-2, where aB≃3.5 nm is the exciton Bohr radius and the exciton-cavity detuning is increased to 30 meV. A high-quality PBG can suppress exciton radiative decay and enhance the polariton lifetime to beyond 150 ps at room temperature, sufficient for thermal

  14. Light matter interactions in 2D transitional metal dichalcogenides: excitonic emission and valley splitting

    NASA Astrophysics Data System (ADS)

    Yu, Ting

    2015-03-01

    Two-dimensional (2D) semiconductors, such as transitional-metal-dichalcogenide monolayers (TMD 1Ls), have aroused great interest because of the underlying fundamental physics (e.g. many body effects and wealth excitonic states) and the promising optoelectronic applications such as light-emitting diodes and solar cells. Here, we report excitonic emission and valley splitting of monolayer WS2 and MoS2 under electrical, optical and magnetic manipulation. Through electrical and optical injection of charge carriers, tunable excitonic emission has been realized due to interplay of various excitonic states, and basic binding energies of trions have been extracted. At low temperature, the Zeeman shifts of excitons and trions have been determined by polarization-dependent photoluminescence measurements under perpendicular magnetic fields, which reveal the breaking of valley degeneracy. Our studies provide the fundamental understanding on large excitonic and unique valleytronic effects in TMD 1Ls. Moreover, we also develop multiple strategies for managing the light emission, which opens up many possibilities for improving the performance and creating the multifunction of 2D TMD-based light emitting applications. Also at Department of Physics, Faculty of Science, National University of Singapore 117542, Singapore; Centre for Advanced 2D Materials and Graphene Research Centre, National University of Singapore 117546, Singapore.

  15. Exciton formation in monolayer transition metal dichalcogenides.

    PubMed

    Ceballos, Frank; Cui, Qiannan; Bellus, Matthew Z; Zhao, Hui

    2016-06-01

    Two-dimensional transition metal dichalcogenides provide a unique platform to study excitons in confined structures. Recently, several important aspects of excitons in these materials have been investigated in detail. However, the formation process of excitons from free carriers has yet to be understood. Here we report time-resolved measurements on the exciton formation process in monolayer samples of MoS2, MoSe2, WS2, and WSe2. The free electron-hole pairs, injected by an ultrashort laser pulse, immediately induce a transient absorption signal of a probe pulse tuned to the exciton resonance. The signal quickly drops by about a factor of two within 1 ps and is followed by a slower decay process. In contrast, when excitons are resonantly injected, the fast decay component is absent. Based both on its excitation excess energy and intensity dependence, this fast decay process is attributed to the formation of excitons from the electron-hole pairs. This interpretation is also consistent with a model that shows how free electron-hole pairs can be about twice more effective than excitons in altering the exciton absorption strength. From our measurements and analysis of our results, we determined that the exciton formation times in these monolayers to be shorter than 1 ps. PMID:27219022

  16. Exciton formation in monolayer transition metal dichalcogenides

    NASA Astrophysics Data System (ADS)

    Ceballos, Frank; Cui, Qiannan; Bellus, Matthew Z.; Zhao, Hui

    2016-06-01

    Two-dimensional transition metal dichalcogenides provide a unique platform to study excitons in confined structures. Recently, several important aspects of excitons in these materials have been investigated in detail. However, the formation process of excitons from free carriers has yet to be understood. Here we report time-resolved measurements on the exciton formation process in monolayer samples of MoS2, MoSe2, WS2, and WSe2. The free electron-hole pairs, injected by an ultrashort laser pulse, immediately induce a transient absorption signal of a probe pulse tuned to the exciton resonance. The signal quickly drops by about a factor of two within 1 ps and is followed by a slower decay process. In contrast, when excitons are resonantly injected, the fast decay component is absent. Based both on its excitation excess energy and intensity dependence, this fast decay process is attributed to the formation of excitons from the electron-hole pairs. This interpretation is also consistent with a model that shows how free electron-hole pairs can be about twice more effective than excitons in altering the exciton absorption strength. From our measurements and analysis of our results, we determined that the exciton formation times in these monolayers to be shorter than 1 ps.

  17. Multiple-exciton generation in lead selenide nanorod solar cells with external quantum efficiencies exceeding 120%

    PubMed Central

    Davis, Nathaniel J. L. K.; Böhm, Marcus L.; Tabachnyk, Maxim; Wisnivesky-Rocca-Rivarola, Florencia; Jellicoe, Tom C.; Ducati, Caterina; Ehrler, Bruno; Greenham, Neil C.

    2015-01-01

    Multiple-exciton generation—a process in which multiple charge-carrier pairs are generated from a single optical excitation—is a promising way to improve the photocurrent in photovoltaic devices and offers the potential to break the Shockley–Queisser limit. One-dimensional nanostructures, for example nanorods, have been shown spectroscopically to display increased multiple exciton generation efficiencies compared with their zero-dimensional analogues. Here we present solar cells fabricated from PbSe nanorods of three different bandgaps. All three devices showed external quantum efficiencies exceeding 100% and we report a maximum external quantum efficiency of 122% for cells consisting of the smallest bandgap nanorods. We estimate internal quantum efficiencies to exceed 150% at relatively low energies compared with other multiple exciton generation systems, and this demonstrates the potential for substantial improvements in device performance due to multiple exciton generation. PMID:26411283

  18. Phonon induced pure dephasing process of excitonic state in colloidal semiconductor quantum dots

    NASA Astrophysics Data System (ADS)

    Huang, Tongyun; Han, Peng; Wang, Xinke; Feng, Shengfei; Sun, Wenfeng; Ye, Jiasheng; Zhang, Yan

    2016-04-01

    We present a theoretical study on the pure dephasing process of colloidal semiconductor quantum dots induced by lattice vibrations using continuum model calculations. By solving the time dependent Liouville-von Neumann equation, we present the ultrafast Rabi oscillations between excitonic state and virtual state via exciton-phonon interaction and obtain the pure dephasing time from the fast decayed envelope of the Rabi oscillations. The interaction between exciton and longitudinal optical phonon vibration is found to dominate the pure dephasing process and the dephasing time increases nonlinearly with the reduction of exciton-phonon coupling strength. We further find that the pure dephasing time of large quantum dots is more sensitive to temperature than small quantum dots.

  19. Resonant energy transfer of triplet excitons from pentacene to PbSe nanocrystals

    NASA Astrophysics Data System (ADS)

    Tabachnyk, Maxim; Ehrler, Bruno; Gélinas, Simon; Böhm, Marcus L.; Walker, Brian J.; Musselman, Kevin P.; Greenham, Neil C.; Friend, Richard H.; Rao, Akshay

    2014-11-01

    The efficient transfer of energy between organic and inorganic semiconductors is a widely sought after property, but has so far been limited to the transfer of spin-singlet excitons. Here we report efficient resonant-energy transfer of molecular spin-triplet excitons from organic semiconductors to inorganic semiconductors. We use ultrafast optical absorption spectroscopy to track the dynamics of triplets, generated in pentacene through singlet exciton fission, at the interface with lead selenide (PbSe) nanocrystals. We show that triplets transfer to PbSe rapidly (<1 ps) and efficiently, with 1.9 triplets transferred for every photon absorbed in pentacene, but only when the bandgap of the nanocrystals is close to resonance (±0.2 eV) with the triplet energy. Following triplet transfer, the excitation can undergo either charge separation, allowing photovoltaic operation, or radiative recombination in the nanocrystal, enabling luminescent harvesting of triplet exciton energy in light-emitting structures.

  20. Resonant energy transfer of triplet excitons from pentacene to PbSe nanocrystals.

    PubMed

    Tabachnyk, Maxim; Ehrler, Bruno; Gélinas, Simon; Böhm, Marcus L; Walker, Brian J; Musselman, Kevin P; Greenham, Neil C; Friend, Richard H; Rao, Akshay

    2014-11-01

    The efficient transfer of energy between organic and inorganic semiconductors is a widely sought after property, but has so far been limited to the transfer of spin-singlet excitons. Here we report efficient resonant-energy transfer of molecular spin-triplet excitons from organic semiconductors to inorganic semiconductors. We use ultrafast optical absorption spectroscopy to track the dynamics of triplets, generated in pentacene through singlet exciton fission, at the interface with lead selenide (PbSe) nanocrystals. We show that triplets transfer to PbSe rapidly (<1 ps) and efficiently, with 1.9 triplets transferred for every photon absorbed in pentacene, but only when the bandgap of the nanocrystals is close to resonance (±0.2 eV) with the triplet energy. Following triplet transfer, the excitation can undergo either charge separation, allowing photovoltaic operation, or radiative recombination in the nanocrystal, enabling luminescent harvesting of triplet exciton energy in light-emitting structures. PMID:25282509

  1. Geometry strategy for engineering the recombination possibility of excitons in nanowires.

    PubMed

    Wang, Youwei; Zhang, Yubo; Zhu, Haiming; Liu, Jianjun; Lian, Tianquan; Zhang, Wenqing

    2016-04-01

    We proposed a geometry strategy to engineer the radiative recombination possibility and thus the lifetime of excitons in nanowires of some photovoltaic semiconductors by using theoretical analysis and first-principles calculations. We demonstrated that the shape can engineer the symmetry of the wave-functions of band-edge states and influence the radiative recombination possibility. The nanowires need to satisfy the following requirements to forbid the radiative recombination possibility of band-edge excitons: (i) wurtzite structure; (ii) pxy-characterized wave-function of VBM state and (iii) C3v-symmetry shape. The geometrical symmetry results in the pxy-characterized C3v-symmetry wave-function of VBM state and leads to forbidden radiative recombination of band-edge excitons. The geometry strategy offers a flexible proposal to prolong the exciton lifetime, leaving optical absorption impregnable. PMID:26980541

  2. Multiple-exciton generation in lead selenide nanorod solar cells with external quantum efficiencies exceeding 120.

    PubMed

    Davis, Nathaniel J L K; Böhm, Marcus L; Tabachnyk, Maxim; Wisnivesky-Rocca-Rivarola, Florencia; Jellicoe, Tom C; Ducati, Caterina; Ehrler, Bruno; Greenham, Neil C

    2015-01-01

    Multiple-exciton generation-a process in which multiple charge-carrier pairs are generated from a single optical excitation-is a promising way to improve the photocurrent in photovoltaic devices and offers the potential to break the Shockley-Queisser limit. One-dimensional nanostructures, for example nanorods, have been shown spectroscopically to display increased multiple exciton generation efficiencies compared with their zero-dimensional analogues. Here we present solar cells fabricated from PbSe nanorods of three different bandgaps. All three devices showed external quantum efficiencies exceeding 100% and we report a maximum external quantum efficiency of 122% for cells consisting of the smallest bandgap nanorods. We estimate internal quantum efficiencies to exceed 150% at relatively low energies compared with other multiple exciton generation systems, and this demonstrates the potential for substantial improvements in device performance due to multiple exciton generation. PMID:26411283

  3. External pumping of hybrid nanostructures in microcavity with Frenkel and Wannier-Mott excitons

    NASA Astrophysics Data System (ADS)

    Dubovskiy, O. A.; Agranovich, V. M.

    2016-09-01

    The exciton-exciton interaction in hybrid nanostructures with resonating Frenkel and Wannier-Mott excitons was investigated in many publications. In microcavity the hybrid nanostructures can be exposed to different types of optical pumping, the most common one being pumping through one of the microcavity side. However, not investigated and thus never been discussed the hybrid excitons generation by pumping of confined quantum wells from the side of empty microcavity without nanostructures in a wave guided configuration. Here, we consider the hybrid excitations in cavity with organic and inorganic quantum wells and with different types of pumping from external source. The frequency dependence for intensity of excitations in hybrid structure is also investigated. The results may be used for search of most effective fluorescence and relaxation processes. The same approach may be used when both quantum wells are organic or inorganic.

  4. Effect of periodic potential on exciton states in semiconductor carbon nanotubes

    DOE PAGESBeta

    Roslyak, Oleksiy; Piryatinski, Andrei

    2016-05-28

    Here we develop a theoretical background to treat exciton states in semiconductor single-walled carbon nanotubes (SWCNTs) in the presence of a periodic potential induced by a surface acoustic wave (SAW) propagating along SWCNT. The formalism accounts for the electronic band splitting into the Floquet subbands induced by the Bragg scattering on the SAW potential. Optical transitions between the Floquet states and correlated electron–hole pairs (excitons) are numerically examined. Formation of new van Hove singularities within the edges of Floquet sub-bands and associated transfer of the exciton oscillator strengths resulting in the photoluminescence quenching are predicted. The simulations demonstrate the excitonmore » energy red Stark shift and reduction in the exciton binding energy. We provide comparison of our results with reported theoretical and experimental studies.« less

  5. Geometry strategy for engineering the recombination possibility of excitons in nanowires

    NASA Astrophysics Data System (ADS)

    Wang, Youwei; Zhang, Yubo; Zhu, Haiming; Liu, Jianjun; Lian, Tianquan; Zhang, Wenqing

    2016-03-01

    We proposed a geometry strategy to engineer the radiative recombination possibility and thus the lifetime of excitons in nanowires of some photovoltaic semiconductors by using theoretical analysis and first-principles calculations. We demonstrated that the shape can engineer the symmetry of the wave-functions of band-edge states and influence the radiative recombination possibility. The nanowires need to satisfy the following requirements to forbid the radiative recombination possibility of band-edge excitons: (i) wurtzite structure; (ii) pxy-characterized wave-function of VBM state and (iii) C3v-symmetry shape. The geometrical symmetry results in the pxy-characterized C3v-symmetry wave-function of VBM state and leads to forbidden radiative recombination of band-edge excitons. The geometry strategy offers a flexible proposal to prolong the exciton lifetime, leaving optical absorption impregnable.

  6. Two-exciton excited states of J-aggregates in the presence of exciton-exciton annihilation

    NASA Astrophysics Data System (ADS)

    Levinsky, B.; Fainberg, B. D.; Nesterov, L. A.; Rosanov, N. N.

    2016-07-01

    We study decay of two-exciton states of a J-aggregate that is collective in nature. We use mathematical formalism based on effective non-Hermitian Hamiltonian suggested in nuclear theory. We show that decay of two-exciton states is strongly affected by the interference processes in the exciton-exciton annihilation. Our evaluations of the imaginary part of the effective Hamiltonian show that it exceeds the spacing between real energies of the two-exciton states that gives rise to the transition to the regime of overlapping resonances supplying the system by the new collectivity - the possibility of coherent decay in the annihilation channel. The decay of two-exciton states varies from twice bimolecular decay rate to the much smaller values that is associated with population trapping. We have also considered the corresponding experiment in the framework of our approach, the picture of which appears to be more complex and richer than it was reasoned before.

  7. Uncovering location-specific ultrafast exciton dynamics in organic semiconducting thin films

    NASA Astrophysics Data System (ADS)

    Ginsberg, Naomi

    2014-03-01

    In solid state semiconducting molecular materials used in electro-optical applications, relatively long exciton diffusion lengths hold the promise to boost device performance by relaxing proximity constraints on the locations for light absorption and interfacial charge separation. The architecture of such materials determines their optical and electronic properties as a result of spacing- and orientation-dependent Coulomb couplings between adjacent molecules. Exciton character and dynamics are generally inferred from bulk optical measurements, which can present a severe limitation on our understanding of these films because their constituent molecules are neither perfectly ordered nor perfectly disordered. Nevertheless, such microstructure can have profound impacts on transport properties. The ultrafast spectroscopy of single domains of polycrystalline films of TIPS-pentacene, a small-molecule organic semiconductor of interest in electronic and photovoltaic applications, is investigated using transient absorption microscopy. Individual domains are distinguished by their different polarization-dependent linear and nonlinear optical responses. As compared to bulk measurements, we show that the nonlinear response within a given domain can be tied more concretely to specific physical processes that transfer exciton populations between specified electronic states. By use of this approach and a simple kinetic model, the signatures of singlet fission as well as vibrational relaxation of the initially excited singlet state are identified. As such, observing exciton dynamics within and comparing exciton dynamics between different TIPS-pentacene domains reveal the relationship between photophysics and film morphology and the potential to resolve unique signatures at interfaces between different regions of the film.

  8. Excitability and optical pulse generation in semiconductor lasers driven by resonant tunneling diode photo-detectors.

    PubMed

    Romeira, Bruno; Javaloyes, Julien; Ironside, Charles N; Figueiredo, José M L; Balle, Salvador; Piro, Oreste

    2013-09-01

    We demonstrate, experimentally and theoretically, excitable nanosecond optical pulses in optoelectronic integrated circuits operating at telecommunication wavelengths (1550 nm) comprising a nanoscale double barrier quantum well resonant tunneling diode (RTD) photo-detector driving a laser diode (LD). When perturbed either electrically or optically by an input signal above a certain threshold, the optoelectronic circuit generates short electrical and optical excitable pulses mimicking the spiking behavior of biological neurons. Interestingly, the asymmetric nonlinear characteristic of the RTD-LD allows for two different regimes where one obtain either single pulses or a burst of multiple pulses. The high-speed excitable response capabilities are promising for neurally inspired information applications in photonics. PMID:24103966

  9. Testing of optical diagnostics for ion-beam-driven WDM experiments at NDCX-1

    NASA Astrophysics Data System (ADS)

    Ni, P. A.; Bieniosek, F. M.; Leitner, M.; Weber, C.; Waldron, W. L.

    2009-07-01

    We report on the testing of optical diagnostics developed for warm-dense-matter (WDM) experiments on the neutralized drift compression experiments (NDCX-1) at Lawrence Berkeley National Laboratory (LBNL). The diagnostics consists of a fast optical pyrometer, a streak camera spectrometer, and a Doppler-shift laser interferometer (VISAR). While the NDCX is in the last stage of commissioning for the target experiments, the diagnostics were tested elsewhere in an experiment where an intense laser pulse was used to generate the WDM state in metallic and carbon samples.

  10. Magnetically driven microconvective instability of optically induced concentration grating in ferrofluids.

    PubMed

    Zablotsky, Dmitry; Blums, Elmars

    2011-08-01

    In this paper, we consider a concentration grating of magnetic nanoparticles optically induced by thermodiffusion in a layer of ferrofluid in the presence of the external homogeneous magnetic field. The applied field is directed along the concentration gradient and leads to the appearance of the internal nonhomogeneous demagnetizing fields. When the system reaches equilibrium, the optical pumping is switched off, and the grating is allowed to relax. We carry out a stability analysis using the Galerkin approach and numerical simulations of the full system of equations to determine the growth rates and the mode amplitudes of the hydrodynamic and concentration perturbations during the relaxation stage. PMID:21929102

  11. Plexciton Dynamics: Exciton-Plasmon Coupling in a J-Aggregate-Au Nanoshell Complex Provides a Mechanism for Nonlinearity

    SciTech Connect

    Fofang, Nche T.; Grady, Nathaniel K.; Fan, Zhiyuan; Govorov, Alexander; Halas, Naomi J.

    2011-03-18

    Coherently coupled plasmons and excitons give rise to new optical excitations- plexcitons - due to the strong coupling of these two oscillator systems. Time-resolved studies of J-aggregate-Au nanoshell complexes when the nanoshell plasmon and J-aggregate exciton energies are degenerate probe the dynamical behavior of this coupled system. Transient absorption of the interacting plasmon-exciton system is observed, in dramatic contrast to the photoinduced transmission of the pristine J-aggregate. An additional, transient Fano-shaped modulation within the Fano dip is also observable. The behavior of the J-aggregate-Au nanoshell complex is described by a combined one-exciton and two-exciton state model coupled to the nanoshell plasmon.

  12. Heterogeneous integration of electrically driven microdisk based laser sources for optical interconnects and photonic ICs.

    PubMed

    Rojo Romeo, P; Van Campenhout, J; Regreny, P; Kazmierczak, A; Seassal, C; Letartre, X; Hollinger, G; Van Thourhout, D; Baets, R; Fedeli, J M; Di Cioccio, L

    2006-05-01

    A new approach for an electrically driven microlaser based on a microdisk transferred onto Silicon is proposed. The structure is based on a quaternary InGaAsP p-i-n junction including three InAsP quantum wells, on a thin membrane transferred onto silicon by molecular bonding. A p++/n++ tunnel junction is used as the p-type contact. The technological procedure is described and first experimental results show a laser emission in pulsed regime at room temperature, with a threshold current near 1.5 mA. PMID:19516533

  13. Second harmonic generation by charge-transfer excitons interacting with phonons

    SciTech Connect

    Reineker, P.; Yudson, V. I.

    2001-06-15

    Effects of exciton-phonon interaction on the nonlinear optical response of charge-transfer excitons (CTE) are studied in the framework of an exactly solvable model. It is found that the second order excitonic optical polarizability {beta} is modified due to the CTE-phonon interaction. For a nonresonant frequency range, where {beta} is relatively small, the change is not significant. On the contrary, in the vicinity of resonances (when the light frequency {omega}{approximately}{omega}{sub 0} or {omega}{approximately}{omega}{sub 0}/2, {omega}{sub 0} is the CTE transition frequency), the CTE-phonon interaction may remarkably diminish the value of {beta}. This should be taken into account when considering CTE systems in nonlinear optics.

  14. Splitting between bright and dark excitons in transition metal dichalcogenide monolayers

    NASA Astrophysics Data System (ADS)

    Echeverry, J. P.; Urbaszek, B.; Amand, T.; Marie, X.; Gerber, I. C.

    2016-03-01

    The optical properties of transition metal dichalcogenide monolayers such as the two-dimensional semiconductors MoS2 and WSe2 are dominated by excitons, Coulomb bound electron-hole pairs. The light emission yield depends on whether the electron-hole transitions are optically allowed (bright) or forbidden (dark). By solving the Bethe-Salpeter equation on top of G W wave functions in density functional theory calculations, we determine the sign and amplitude of the splitting between bright and dark exciton states. We evaluate the influence of the spin-orbit coupling on the optical spectra and clearly demonstrate the strong impact of the intra-valley Coulomb exchange term on the dark-bright exciton fine structure splitting.

  15. Excitonic transport in ZnO

    NASA Astrophysics Data System (ADS)

    Noltemeyer, Martin; Bertram, Frank; Hempel, Thomas; Bastek, Barbara; Christen, Juergen; Brandt, Matthias; Lorenz, Michael; Grundmann, Marius

    2012-02-01

    The temperature dependence of diffusion length and lifetime or diffusivity of the free exciton is measured in a commercial ZnO-substrate and in an epitaxial ZnO quantum well using nm-spatially and ps-time resolved cathodoluminescence (CL) spectroscopy. The characteristic temperature dependence of the exciton mobility is a fingerprint of the underlying excitonic scattering processes. Since excitons are neutral particles scattering at ionized impurities should be not effective. With decreasing temperature diffusion lengths and lifetimes give rise to a monotonous increase of the excitonic mobility. Two different methods for determining the excitonic transport parameters will be presented. On the one hand we are able to perform completely pulsed excitation experiments and on the other hand a combination of cw- and pulsed excitation in two independent measurements are needed.

  16. Exciton Seebeck effect in molecular systems

    SciTech Connect

    Yan, Yun-An; Cai, Shaohong

    2014-08-07

    We investigate the exciton dynamics under temperature difference with the hierarchical equations of motion. Through a nonperturbative simulation of the transient absorption of a heterogeneous trimer model, we show that the temperature difference causes exciton population redistribution and affects the exciton transfer time. It is found that one can reproduce not only the exciton population redistribution but also the change of the exciton transfer time induced by the temperature difference with a proper tuning of the site energies of the aggregate. In this sense, there exists a site energy shift equivalence for any temperature difference in a broad range. This phenomenon is similar to the Seebeck effect as well as spin Seebeck effect and can be named as exciton Seebeck effect.

  17. Cloud-Driven Changes in Aerosol Optical Properties - Final Technical Report

    SciTech Connect

    Ogren, John A.; Sheridan, Patrick S.; Andrews, Elisabeth

    2007-09-30

    The optical properties of aerosol particles are the controlling factors in determining direct aerosol radiative forcing. These optical properties depend on the chemical composition and size distribution of the aerosol particles, which can change due to various processes during the particles’ lifetime in the atmosphere. Over the course of this project we have studied how cloud processing of atmospheric aerosol changes the aerosol optical properties. A counterflow virtual impactor was used to separate cloud drops from interstitial aerosol and parallel aerosol systems were used to measure the optical properties of the interstitial and cloud-scavenged aerosol. Specifically, aerosol light scattering, back-scattering and absorption were measured and used to derive radiatively significant parameters such as aerosol single scattering albedo and backscatter fraction for cloud-scavenged and interstitial aerosol. This data allows us to demonstrate that the radiative properties of cloud-processed aerosol can be quite different than pre-cloud aerosol. These differences can be used to improve the parameterization of aerosol forcing in climate models.

  18. Localized Excitons in Carbon Nanotubes.

    NASA Astrophysics Data System (ADS)

    Adamska, Lyudmyla; Doorn, Stephen K.; Tretiak, Sergei

    2015-03-01

    It has been historically known that unintentional defects in carbon nanotubes (CNTs) may fully quench the fluorescence. However, some dopants may enhance the fluorescence by one order of magnitude thus turning the CNTs, which are excellent light absorbers, in good emitters. We have correlated the experimentally observed photoluminescence spectra to the electronic structure simulations. Our experiment reveals multiple sharp asymmetric emission peaks at energies 50-300 meV red-shifted from that of the lowest bright exciton peak. Our simulations suggest an association of these peaks with deep trap states tied to different specific chemical adducts. While the wave functions of excitons in undoped CNTs are delocalized, those of the deep-trap states are strongly localized and pinned to the dopants. These findings are consistent with the experimental observation of asymmetric broadening of the deep trap emission peaks, which can result from scattering of acoustic phonons on localized excitons. Our work lays the foundation to utilize doping as a generalized route for wave function engineering and direct control of carrier dynamics in SWCNTs toward enhanced light emission properties for photonic applications.

  19. Analytical approach to excitonic properties of MoS2

    NASA Astrophysics Data System (ADS)

    Berghäuser, Gunnar; Malic, Ermin

    2014-03-01

    We present an analytical investigation of the optical absorption spectrum of monolayer molybdenum-disulfide. Based on the density matrix formalism, our approach gives insights into the microscopic origin of excitonic transitions, their relative oscillator strength, and binding energy. We show analytical expressions for the carrier-light coupling element, which contains the optical selection rules and describes well the valley-selective polarization in MoS2. In agreement with experimental results, we find the formation of strongly bound electron-hole pairs due to the efficient Coulomb interaction. The absorption spectrum of MoS2 features two pronounced peaks corresponding to the A and B exciton. For MoS2 on a SiO2 substrate, these are characterized by binding energies of 455 meV and 465 meV, respectively. Our calculations reveal their relative oscillator strength and predict the appearance of further low-intensity excitonic transitions at higher energies. The presented approach is applicable to other transition metal dichalcogenides and can be extended to investigations of trion and biexcitonic effects.

  20. Bright solitons and self-trapping with a Bose-Einstein condensate of atoms in driven tilted optical lattices

    SciTech Connect

    Kolovsky, Andrey R.

    2010-07-15

    We discuss a method for creating bright matter solitons by loading a Bose-Einstein condensate of atoms in a driven tilted optical lattice. It is shown that one can realize the self-focusing regime for the wave-packet dynamics by properly adjusting the phase of the driving field with respect to the phase of Bloch oscillations. If atom-atom interactions are larger than some critical value g{sub min}, this self-focusing regime is followed by the formation of bright solitons. Increasing the interactions above another critical value g{sub max} makes this process unstable. Instead of soliton formation one now meets the phenomenon of incoherent self-trapping. In this regime a fraction of atoms is trapped in incoherent localized wave packets, while the remaining atoms spread ballistically.

  1. Steady-state bistability and long-range order in optically driven Rydberg gases in the anti-blockade regime

    NASA Astrophysics Data System (ADS)

    Letscher, Fabian; Linzner, Dominik; Fleischhauer, Michael

    2016-05-01

    Motivated by recent experiments, we study spatial and temporal correlations of Rydberg excitations of optically driven ultra-cold atoms in the anti-blockade regime. In particular, we discuss the influence of dissipation on the excitation dynamics of a linear chain of atoms, described by the dissipative, transverse-field Ising model. Using t-DMRG simulations of the density matrix we identify parameter regimes with diverging correlation lengths in the coherent regime of weak dissipation. Correlation lengths remain short-ranged in the incoherent regime of strong dissipation, where classical rate equations can be employed. We discuss the different physical mechanisms determining the many-body dynamics in the two regimes and compare theoretical predictions with recent experimental results. In particular we discuss the formation of excitation cluster in the incoherent regime and explain the observed slow-down of the relaxation process due to cluster formation.

  2. A compact, widely tunable intracavity PPLN optical parameter oscillator driven by an Nd:YAG/Cr:YAG composite crystal laser

    NASA Astrophysics Data System (ADS)

    Yang, X.-Q.; Yang, J.-F.; Zhang, B.-T.; Liu, S.-D.

    2012-03-01

    Based on periodically poled lithium niobate (PPLN), a mini intracavity optical parameter oscillator (IOPO) driven by an diode-end-pumped composite Nd3+:YAG/Cr4+:YAG laser was demonstrated. The PPLN wafer has 20 domain reversal periods from 27.8 to 31.6 μm with a step of 0.2 μm between the neighbor periods. The output signal laser of OPO can be widely tunable in the range of 1402-1676 nm by changing the period at a certain temperature of 50°C. Under the diode pump power of 14 W, the maximum average output power of 600 mW at 1534 nm with pulse width of 2.0 ns and repetition rate of 16 kHz was obtained, corresponding to a peak power of 18.7 kW and a single pulse energy of 37.5 μJ, respectively.

  3. Magnetic Brightening of Dark Excitons in Carbon Nanotubes

    NASA Astrophysics Data System (ADS)

    Kono, Junichiro

    2007-03-01

    To gain insight into the internal energy structure and radiative properties of excitons in single-walled carbon nanotubes (SWNTs), we have studied photoluminescence (PL) from individualized HiPco and CoMoCAT samples as a function of magnetic field (B) and temperature (T). The PL intensity increased, or ``brightened,'' with B applied along the tube axis and the amount of brightening increased with decreasing T. These results are consistent with the existence of a dark state below the first bright state [1]. In the presence of time reversal symmetry, exchange-interaction-induced mixing between excitons in two equivalent valleys (the K and K' valleys) is expected to result in a set of exciton states, only one of which is optically active. This predicted bright state, however, is not the lowest in energy. Excitons would be trapped in the dark, lowest-energy state without a radiative recombination path. When a tube-threading B is applied, addition of an Aharonov-Bohm phase modifies the circumferential boundary conditions on the wave functions and lifts time reversal symmetry [2,3]. This symmetry breaking splits the K and K' valley transitions, lessening the intervalley mixing and causing the recovery of the unmixed direct K and K' excitons, which are both optically active. We have calculated PL spectra through B-dependent effective masses, populations of finite-k states, and acoustic phonon scattering, which quantitatively agree with the observations. These results demonstrate the existence of dark excitons, their influence on the PL quantum yield, and their elimination through symmetry manipulation by a B. This work was performed in collaboration with J. Shaver, S. Zaric, O. Portugall, V. Krstic, G. L. J. A. Rikken, X. Wei, S. A. Crooker, Y. Miyauchi, S. Maruyama, and V. Perebeinos and supported by the Robert A. Welch Foundation, the NSF, and EuroMagNET. [1] V. Perebeinos et al., Phys. Rev. Lett. 92, 257402 (2004); H. Zhao and S. Mazumdar, Phys. Rev. Lett. 93, 157402

  4. Charge-transfer excitons in DNA.

    PubMed

    Conwell, E M; McLaughlin, P M; Bloch, S M

    2008-02-21

    There have been a number of theoretical treatments of excitons in DNA, most neglecting both the intrachain and interchain wavefunction overlaps of the electron and hole, treating them as Frenkel excitons. Recently, the importance of the intrachain and interchain coupling has been highlighted. Experiments have shown that in (dA)n oligomers and in duplex (dA)n.(dT)n, to be abbreviated (A/T), where A is adenine and T is thymine, the exciton wavefunction is delocalized over several bases. In duplexes it is possible to have charge-transfer (CT) excitons. Theoretical calculations have suggested that CT excitons in DNA may have lower energy than single chain excitons. In all the calculations of excitons in DNA, the polarization of the surrounding water has been neglected. Calculations have shown, however, that polarization of the water by an excess electron or a hole in DNA lowers its energy by approximately 1/2 eV, causing it to become a polaron. It is therefore to be expected that polarization charge induced in the surrounding water has a significant effect on the properties of the exciton. In what follows, we present calculations of some properties CT excitons would have in an A/T duplex taking into account the wavefunction overlaps, the effect of the surrounding water, which results in the electron and hole becoming polarons, and the ions in the water. As expected, the CT exciton has lowest energy when the electron and hole polarons are directly opposite each other. By appropriate choice of the dielectric constant, we can obtain a CT exciton delocalized over the number of sites found in photoinduced absorption experiments. The absorption threshold that we then calculate for CT exciton creation in A/T is in reasonable agreement with the lowest singlet absorption deduced from available data. PMID:18232682

  5. Observation of Dressed Excitonic States in a Single Quantum Dot

    NASA Astrophysics Data System (ADS)

    Jundt, Gregor; Robledo, Lucio; Högele, Alexander; Fält, Stefan; Imamoǧlu, Atac

    2008-05-01

    We report the observation of dressed states of a quantum dot. The optically excited exciton and biexciton states of the quantum dot are coupled by a strong laser field and the resulting spectral signatures are measured using differential transmission of a probe field. We demonstrate that the anisotropic electron-hole exchange interaction induced splitting between the x- and y-polarized excitonic states can be completely erased by using the ac-Stark effect induced by the coupling field, without causing any appreciable broadening of the spectral lines. We also show that by varying the polarization and strength of a resonant coupling field, we can effectively change the polarization axis of the quantum dot.

  6. Direct measurement of exciton valley coherence in monolayer WSe2

    NASA Astrophysics Data System (ADS)

    Hao, Kai; Moody, Galan; Wu, Fengcheng; Dass, Chandriker Kavir; Xu, Lixiang; Chen, Chang-Hsiao; Sun, Liuyang; Li, Ming-Yang; Li, Lain-Jong; MacDonald, Allan H.; Li, Xiaoqin

    2016-07-01

    In crystals, energy band extrema in momentum space can be identified by a valley index. The internal quantum degree of freedom associated with valley pseudospin indices can act as a useful information carrier, analogous to electronic charge or spin. Interest in valleytronics has been revived in recent years following the discovery of atomically thin materials such as graphene and transition metal dichalcogenides. However, the valley coherence time--a crucial quantity for valley pseudospin manipulation--is difficult to directly probe. In this work, we use two-dimensional coherent spectroscopy to resonantly generate and detect valley coherence of excitons (Coulomb-bound electron-hole pairs) in monolayer WSe2 (refs ,). The imposed valley coherence persists for approximately one hundred femtoseconds. We propose that the electron-hole exchange interaction provides an important decoherence mechanism in addition to exciton population recombination. This work provides critical insight into the requirements and strategies for optical manipulation of the valley pseudospin for future valleytronics applications.

  7. Probing semiconductor confined excitons decay into surface plasmon polaritons

    NASA Astrophysics Data System (ADS)

    Sobreira, F. W. A.; de Oliveira, E. R. Cardozo; Teodoro, M. D.; Marques, G. E.; Marega, E.

    2016-04-01

    The study of the interaction of surface plasmon polaritons (SPPs) with quantum emitters has become very important in the last few years. The ability to design optical devices as well as investigate the physics of strongly interacting systems is some of its useful applications. In this paper, we will show some results on the decay of excitons confined in a InAs/GaAs quantum dot into SPP modes confined in a metallic thin film made of Au, an important step toward the investigation of the basic features of the SPP-exciton interaction. The lifetime of the ground state level was investigated and shown to decrease with the presence of the metallic film.

  8. Quasiparticle and excitonic gaps of one-dimensional carbon chains.

    PubMed

    Mostaani, E; Monserrat, B; Drummond, N D; Lambert, C J

    2016-06-01

    We report diffusion quantum Monte Carlo (DMC) calculations of the quasiparticle and excitonic gaps of hydrogen-terminated oligoynes and extended polyyne. The electronic gaps are found to be very sensitive to the atomic structure in these systems. We have therefore optimised the geometry of polyyne by directly minimising the DMC energy with respect to the lattice constant and the Peierls-induced carbon-carbon bond-length alternation. We find the bond-length alternation of polyyne to be 0.136(2) Å and the excitonic and quasiparticle gaps to be 3.30(7) and 3.4(1) eV, respectively. The DMC zone-centre longitudinal optical phonon frequency of polyyne is 2084(5) cm(-1), which is consistent with Raman spectroscopic measurements for large oligoynes. PMID:27104222

  9. Exciton Fine Structure in Single CdSe Nanorods

    NASA Astrophysics Data System (ADS)

    Le Thomas, N.; Herz, E.; Schöps, O.; Woggon, U.; Artemyev, M. V.

    2005-01-01

    We study the optical properties of excitons in one-dimensional (1D) nanostructures at low temperatures. In single CdSe/ZnS core-shell nanorods we observe a fine structure splitting and explain it by exchange interaction. Two peaks are observed with different degrees of linear polarization of DLP<0.85 and DLP>0.95. For small nanorod radii R≤aB/2, an increase in the photoluminescence decay time is found when the temperature increases from 10 to 80K. The observations are explained by a radius-dependent change in the symmetry of the 1D-exciton ground state which transforms from a dark state into bright states below a critical radius of Rcrit≈3.7 nm.

  10. Linewidths in excitonic absorption spectra of cuprous oxide

    NASA Astrophysics Data System (ADS)

    Schweiner, Frank; Main, Jörg; Wunner, Günter

    2016-02-01

    We present a theoretical calculation of the absorption spectrum of cuprous oxide (Cu2O ) based on the general theory developed by Y. Toyozawa. An inclusion not only of acoustic phonons but also of optical phonons and of specific properties of the excitons in Cu2O like the central-cell corrections for the 1 S exciton allows us to calculate the experimentally observed linewidths in experiments by T. Kazimierczuk et al. [T. Kazimierczuk, D. Fröhlich, S. Scheel, H. Stolz, and M. Bayer, Nature (London) 514, 343 (2014), 10.1038/nature13832] within the same order of magnitude, which demonstrates a clear improvement in comparison to earlier work on this topic. We also discuss a variety of further effects, which explain the still observable discrepancy between theory and experiment but can hardly be included in theoretical calculations.

  11. Multiple exciton generation and ultrafast exciton dynamics in HgTe colloidal quantum dots.

    PubMed

    Al-Otaify, Ali; Kershaw, Stephen V; Gupta, Shuchi; Rogach, Andrey L; Allan, Guy; Delerue, Christophe; Binks, David J

    2013-10-21

    The investigation of sub-nanosecond exciton dynamics in HgTe colloidal quantum dots using ultrafast transient absorption spectroscopy is reported. The transmittance change spectrum acquired immediately after pumping is dominated by a bleach blue-shifted by ~200-300 nm from the photoluminescent emission band. Comparison with a tight-binding model of the electronic structure allows this feature to be attributed to the filling of band edge states. The form of the pump-induced transmittance transients is dependent on the excitation rate and the rate of sample stirring. For moderate pumping of stirred samples, the transmittance transients are well-described by a mono-exponential decay associated with biexciton recombination, with a lifetime of 49 ± 2 ps. For samples that are strongly-pumped or unstirred, the decay becomes bi-exponential in form, indicating that trap-related recombination has become significant. We also present a new analysis that enables fractional transmittance changes to be related to band edge occupation for samples with arbitrary optical density at the pump wavelength. This allows us to identify the occurrence of multiple exciton generation, which results in a quantum yield of 1.36 ± 0.04 for a photon energy equivalent to 3.1 times the band gap, in good agreement with the results of the model. PMID:23999734

  12. Distinct exciton dissociation behavior of organolead trihalide perovskite and excitonic semiconductors studied in a same device

    DOE PAGESBeta

    Hu, Miao; Bi, Cheng; Yuan, Yongbo; Xiao, Zhengguo; Dong, Qingfeng; Shao, Yuchuan; Huang, Jinsong

    2015-01-15

    The nonexcitonic character for organometal trihalide perovskites is demonstrated by examining the field-dependent exciton dissociation behavior. Moreover, it is found that photogenerated excitons can be effectively dissociated into free charges inside perovskite without the assistance of charge extraction layer or external field, which is a stark contrast to the charge-separation behavior in excitonic materials in the same photovoltaic operation system.

  13. Ground state energy of N Frenkel excitons

    NASA Astrophysics Data System (ADS)

    Pogosov, W.; Combescot, M.

    2009-03-01

    By using the composite many-body theory for Frenkel excitons we have recently developed, we here derive the ground state energy of N Frenkel excitons in the Born approximation through the Hamiltonian mean value in a state made of N identical Q = 0 excitons. While this quantity reads as a density expansion in the case of Wannier excitons, due to many-body effects induced by fermion exchanges between N composite particles, we show that the Hamiltonian mean value for N Frenkel excitons only contains a first order term in density, just as for elementary bosons. Such a simple result comes from a subtle balance, difficult to guess a priori, between fermion exchanges for two or more Frenkel excitons appearing in Coulomb term and the ones appearing in the N exciton normalization factor - the cancellation being exact within terms in 1/Ns where Ns is the number of atomic sites in the sample. This result could make us naively believe that, due to the tight binding approximation on which Frenkel excitons are based, these excitons are just bare elementary bosons while their composite nature definitely appears at various stages in the precise calculation of the Hamiltonian mean value.

  14. Terahertz spectroscopy of two-dimensional electron-hole pairs: probing Mott physics of magneto-excitons

    NASA Astrophysics Data System (ADS)

    Zhang, Qi; Gao, Weilu; Watson, John; Manfra, Michael; Kono, Junichiro

    2015-03-01

    Density-dependent Coulomb interactions can drive electron-hole (e - h) pairs in semiconductors through an excitonic Mott transition from an excitonic gas into an e - h plasma. Theoretical studies suggest that these interactions can be strongly modified by an external magnetic field, including the absence of inter-exciton interactions in the high magnetic field limit in two dimensions, due to an e - h charge symmetry, which results in ultrastable magneto-excitons. Here, we present a systematic experimental study of e - h pairs in photo-excited undoped GaAs quantum wells in magnetic fields with ultrafast terahertz spectroscopy. We simultaneously monitored the dynamics of the intraexcitonic 1 s-2 p transition (which splits into 1 s-2p+ and 1 s-2p- transitions in a magnetic field) and the cyclotron resonance of unbound electrons and holes up to 10 Tesla. We found that the 1 s-2p- absorption feature is robust at high magnetic fields even under high excitation fluences, indicating magnetically enhanced stability of excitons. We will discuss the Mott physics of magneto-excitons as a function of temperature, e - h pair density, optical pump delay time, as well as magnetic field, and also compare two-dimensional excitons in GaAs quantum wells with three-dimensional excitons in bulk GaAs.

  15. Fulde-Ferrell Superfluids without Spin Imbalance in Driven Optical Lattices.

    PubMed

    Zheng, Zhen; Qu, Chunlei; Zou, Xubo; Zhang, Chuanwei

    2016-03-25

    Spin-imbalanced ultracold Fermi gases have been widely studied recently as a platform for exploring the long-sought Fulde-Ferrell-Larkin-Ovchinnikov superfluid phases, but so far conclusive evidence has not been found. Here we propose to realize an Fulde-Ferrell (FF) superfluid without spin imbalance in a three-dimensional fermionic cold atom optical lattice, where s- and p-orbital bands of the lattice are coupled by another weak moving optical lattice. Such coupling leads to a spin-independent asymmetric Fermi surface, which, together with the s-wave scattering interaction between two spins, yields an FF type of superfluid pairing. Unlike traditional schemes, our proposal does not rely on the spin imbalance (or an equivalent Zeeman field) to induce the Fermi surface mismatch and provides a completely new route for realizing FF superfluids. PMID:27058062

  16. Holographic optical manipulation of motor-driven membranous structures in living NG-108 cells

    NASA Astrophysics Data System (ADS)

    Farré, Arnau; López-Quesada, Carol; Andilla, Jordi; Martín-Badosa, Estela; Montes-Usategui, Mario

    2010-08-01

    Optical tweezer experiments have partially unveiled the mechanical properties of processive motor proteins while driving polystyrene or silica microbeads in vitro. However, the set of forces underlying the more complex transport mechanisms in living samples remains poorly understood. Several studies have shown that optical tweezers are capable of trapping vesicles and organelles in the cytoplasm of living cells, which can be used as handles to mechanically interact with engaged (active) motors, or other components regulating transport. This may ultimately enable the exploration of the mechanics of this trafficking mechanism in vivo. These cell manipulation experiments have been carried out using different strategies to achieve dynamic beam steering capable of trapping these subcellular structures. We report here the first trapping and manipulation, to our knowledge, of such small motor-propelled cargos in living cells using holographic technology.

  17. Nematicon-driven injection of amplified spontaneous emission into an optical fiber.

    PubMed

    Bolis, Serena; Virgili, Tersilla; Rajendran, Sai Kiran; Beeckman, Jeroen; Kockaert, Pascal

    2016-05-15

    We investigate experimentally the interaction between amplified spontaneous emission (ASE) and a soliton, which are both generated in a dye-doped nematic liquid crystal (LC) cell. A light beam is injected through an optical fiber slid into the cell to form a soliton beam. ASE is then automatically collected by this self-induced waveguide and efficiently coupled into the same optical fiber, in the backward direction. We demonstrate that the presence of the soliton improves the ASE collection by one order of magnitude. We also show that the ASE is highly polarized in the plane of the LC cell and that the ASE spectrum depends on the pump stripe orientation with respect to the LC director. The origin of the spectral anisotropy of the gain curves is determined with the help of femtosecond pump-probe spectroscopy. PMID:27176973

  18. Directly driven source of multi-gigahertz, sub-picosecond optical pulses

    SciTech Connect

    Messerly, Michael J.; Dawson, Jay W.; Barty, Christopher P.J.; Gibson, David J.; Prantil, Matthew A.; Cormier, Eric

    2015-10-20

    A robust, compact optical pulse train source is described, with the capability of generating sub-picosecond micro-pulse sequences, which can be periodic as well as non-periodic, and at repetition rates tunable over decades of baseline frequencies, from MHz to multi-GHz regimes. The micro-pulses can be precisely controlled and formatted to be in the range of many ps in duration to as short as several fs in duration. The system output can be comprised of a continuous wave train of optical micro-pulses or can be programmed to provide gated bursts of macro-pulses, with each macro-pulse consisting of a specific number of micro-pulses or a single pulse picked from the higher frequency train at a repetition rate lower than the baseline frequency. These pulses could then be amplified in energy anywhere from the nJ to MJ range.

  19. Dynamics of a mesoscopic nuclear spin ensemble interacting with an optically driven electron spin

    NASA Astrophysics Data System (ADS)

    Stanley, M. J.; Matthiesen, C.; Hansom, J.; Le Gall, C.; Schulte, C. H. H.; Clarke, E.; Atatüre, M.

    2014-11-01

    The ability to discriminate between simultaneously occurring noise sources in the local environment of semiconductor InGaAs quantum dots, such as electric and magnetic field fluctuations, is key to understanding their respective dynamics and their effect on quantum dot coherence properties. We present a discriminatory approach to all-optical sensing based on two-color resonance fluorescence of a quantum dot charged with a single electron. Our measurements show that local magnetic field fluctuations due to nuclear spins in the absence of an external magnetic field are described by two correlation times, both in the microsecond regime. The nuclear spin bath dynamics show a strong dependence on the strength of resonant probing, with correlation times increasing by a factor of 4 as the optical transition is saturated. We interpret the behavior as motional averaging of both the Knight field of the resident electron spin and the hyperfine-mediated nuclear spin-spin interaction due to optically induced electron spin flips.

  20. Noise-driven optical absorption coefficients of impurity doped quantum dots

    NASA Astrophysics Data System (ADS)

    Ganguly, Jayanta; Saha, Surajit; Pal, Suvajit; Ghosh, Manas

    2016-01-01

    We make an extensive investigation of linear, third-order nonlinear, and total optical absorption coefficients (ACs) of impurity doped quantum dots (QDs) in presence and absence of noise. The noise invoked in the present study is a Gaussian white noise. The quantum dot is doped with repulsive Gaussian impurity. Noise has been introduced to the system additively and multiplicatively. A perpendicular magnetic field acts as a source of confinement and a static external electric field has been applied. The AC profiles have been studied as a function of incident photon energy when several important parameters such as optical intensity, electric field strength, magnetic field strength, confinement energy, dopant location, relaxation time, Al concentration, dopant potential, and noise strength take on different values. In addition, the role of mode of application of noise (additive/multiplicative) on the AC profiles has also been analyzed meticulously. The AC profiles often consist of a number of interesting observations such as one photon resonance enhancement, shift of AC peak position, variation of AC peak intensity, and bleaching of AC peak. However, presence of noise alters the features of AC profiles and leads to some interesting manifestations. Multiplicative noise brings about more complexity in the AC profiles than its additive counterpart. The observations indeed illuminate several useful aspects in the study of linear and nonlinear optical properties of doped QD systems, specially in presence of noise. The findings are expected to be quite relevant from a technological perspective.

  1. Magnetospherically driven optical and radio aurorae at the end of the stellar main sequence.

    PubMed

    Hallinan, G; Littlefair, S P; Cotter, G; Bourke, S; Harding, L K; Pineda, J S; Butler, R P; Golden, A; Basri, G; Doyle, J G; Kao, M M; Berdyugina, S V; Kuznetsov, A; Rupen, M P; Antonova, A

    2015-07-30

    Aurorae are detected from all the magnetized planets in our Solar System, including Earth. They are powered by magnetospheric current systems that lead to the precipitation of energetic electrons into the high-latitude regions of the upper atmosphere. In the case of the gas-giant planets, these aurorae include highly polarized radio emission at kilohertz and megahertz frequencies produced by the precipitating electrons, as well as continuum and line emission in the infrared, optical, ultraviolet and X-ray parts of the spectrum, associated with the collisional excitation and heating of the hydrogen-dominated atmosphere. Here we report simultaneous radio and optical spectroscopic observations of an object at the end of the stellar main sequence, located right at the boundary between stars and brown dwarfs, from which we have detected radio and optical auroral emissions both powered by magnetospheric currents. Whereas the magnetic activity of stars like our Sun is powered by processes that occur in their lower atmospheres, these aurorae are powered by processes originating much further out in the magnetosphere of the dwarf star that couple energy into the lower atmosphere. The dissipated power is at least four orders of magnitude larger than what is produced in the Jovian magnetosphere, revealing aurorae to be a potentially ubiquitous signature of large-scale magnetospheres that can scale to luminosities far greater than those observed in our Solar System. These magnetospheric current systems may also play a part in powering some of the weather phenomena reported on brown dwarfs. PMID:26223623

  2. Optically driven translational and rotational motions of microrod particles in a nematic liquid crystal

    PubMed Central

    Eremin, Alexey; Hirankittiwong, Pemika; Chattham, Nattaporn; Nádasi, Hajnalka; Stannarius, Ralf; Limtrakul, Jumras; Haba, Osamu; Yonetake, Koichiro; Takezoe, Hideo

    2015-01-01

    A small amount of azo-dendrimer molecules dissolved in a liquid crystal enables translational and rotational motions of microrods in a liquid crystal matrix under unpolarized UV light irradiation. This motion is initiated by a light-induced trans-to-cis conformational change of the dendrimer adsorbed at the rod surface and the associated director reorientation. The bending direction of the cis conformers is not random but is selectively chosen due to the curved local director field in the vicinity of the dendrimer-coated surface. Different types of director distortions occur around the rods, depending on their orientations with respect to the nematic director field. This leads to different types of motions driven by the torques exerted on the particles by the director reorientations. PMID:25624507

  3. Controlling the polarization eigenstate of a quantum dot exciton with light.

    PubMed

    Belhadj, Thomas; Simon, Claire-Marie; Amand, Thierry; Renucci, Pierre; Chatel, Beatrice; Krebs, Olivier; Lemaître, Aristide; Voisin, Paul; Marie, Xavier; Urbaszek, Bernhard

    2009-08-21

    We demonstrate optical control of the polarization eigenstates of a neutral quantum dot exciton without any external fields. By varying the excitation power of a circularly polarized laser in microphotoluminescence experiments on individual InGaAs quantum dots we control the magnitude and direction of an effective internal magnetic field created via optical pumping of nuclear spins. The adjustable nuclear magnetic field allows us to tune the linear and circular polarization degree of the neutral exciton emission. The quantum dot can thus act as a tunable light polarization converter. PMID:19792745

  4. Controlled exciton transfer between quantum dots with acoustic phonons taken into account

    SciTech Connect

    Golovinski, P. A.

    2015-09-15

    A system of excitons in two quantum dots coupled by the dipole–dipole interaction is investigated. The excitation transfer process controlled by the optical Stark effect at nonresonant frequencies is considered and the effect of the interaction between excitons and acoustic phonons in a medium on this process is taken into account. The system evolution is described using quantum Heisenberg equations. A truncated set of equations is obtained and the transfer dynamics is numerically simulated. High-efficiency picosecond switching of the excitation transfer by a laser pulse with a rectangular envelope is demonstrated. The dependence of picosecond switching on the quantum-dot parameters and optical-pulse length is presented.

  5. Resonant internal quantum transitions and femtosecond radiative decay of excitons in monolayer WSe2

    NASA Astrophysics Data System (ADS)

    Poellmann, C.; Steinleitner, P.; Leierseder, U.; Nagler, P.; Plechinger, G.; Porer, M.; Bratschitsch, R.; Schüller, C.; Korn, T.; Huber, R.

    2015-09-01

    Atomically thin two-dimensional crystals have revolutionized materials science. In particular, monolayer transition metal dichalcogenides promise novel optoelectronic applications, owing to their direct energy gaps in the optical range. Their electronic and optical properties are dominated by Coulomb-bound electron-hole pairs called excitons, whose unusual internal structure, symmetry, many-body effects and dynamics have been vividly discussed. Here we report the first direct experimental access to all 1s A excitons, regardless of momentum--inside and outside the radiative cone--in single-layer WSe2. Phase-locked mid-infrared pulses reveal the internal orbital 1s-2p resonance, which is highly sensitive to the shape of the excitonic envelope functions and provides accurate transition energies, oscillator strengths, densities and linewidths. Remarkably, the observed decay dynamics indicates an ultrafast radiative annihilation of small-momentum excitons within 150 fs, whereas Auger recombination prevails for optically dark states. The results provide a comprehensive view of excitons and introduce a new degree of freedom for quantum control, optoelectronics and valleytronics of dichalcogenide monolayers.

  6. Features of exciton dynamics in molecular nanoclusters (J-aggregates): Exciton self-trapping (Review Article)

    NASA Astrophysics Data System (ADS)

    Malyukin, Yu. V.; Sorokin, A. V.; Semynozhenko, V. P.

    2016-06-01

    We present thoroughly analyzed experimental results that demonstrate the anomalous manifestation of the exciton self-trapping effect, which is already well-known in bulk crystals, in ordered molecular nanoclusters called J-aggregates. Weakly-coupled one-dimensional (1D) molecular chains are the main structural feature of J-aggregates, wherein the electron excitations are manifested as 1D Frenkel excitons. According to the continuum theory of Rashba-Toyozawa, J-aggregates can have only self-trapped excitons, because 1D excitons must adhere to barrier-free self-trapping at any exciton-phonon coupling constant g = ɛLR/2β, wherein ɛLR is the lattice relaxation energy, and 2β is the half-width of the exciton band. In contrast, very often only the luminescence of free, mobile excitons would manifest in experiments involving J-aggregates. Using the Urbach rule in order to analyze the low-frequency region of the low-temperature exciton absorption spectra has shown that J-aggregates can have both a weak (g < 1) and a strong (g > 1) exciton-phonon coupling. Moreover, it is experimentally demonstrated that under certain conditions, the J-aggregate excited state can have both free and self-trapped excitons, i.e., we establish the existence of a self-trapping barrier for 1D Frenkel excitons. We demonstrate and analyze the reasons behind the anomalous existence of both free and self-trapped excitons in J-aggregates, and demonstrate how exciton-self trapping efficiency can be managed in J-aggregates by varying the values of g, which is fundamentally impossible in bulk crystals. We discuss how the exciton-self trapping phenomenon can be used as an alternate interpretation of the wide band emission of some J-aggregates, which has thus far been explained by the strongly localized exciton model.

  7. Temperature-driven band inversion in Pb0.77Sn0.23Se: Optical and Hall effect studies

    DOE PAGESBeta

    Anand, Naween; Buvaev, Sanal; Hebard, A. F.; Tanner, D. B.; Chen, Zhiguo; Li, Zhiqiang; Choudhary, Kamal; Sinnott, S. B.; Gu, Genda; Martin, C.

    2014-12-23

    Optical and Hall-effect measurements have been performed on single crystals of Pb₀.₇₇Sn₀.₂₃Se, a IV-VI mixed chalcogenide. The temperature dependent (10–300 K) reflectance was measured over 40–7000 cm⁻¹ (5–870 meV) with an extension to 15,500 cm⁻¹ (1.92 eV) at room temperature. The reflectance was fit to the Drude-Lorentz model using a single Drude component and several Lorentz oscillators. The optical properties at the measured temperatures were estimated via Kramers-Kronig analysis as well as by the Drude-Lorentz fit. The carriers were p-type with the carrier density determined by Hall measurements. A signature of valence intraband transition is found in the low-energy opticalmore » spectra. It is found that the valence-conduction band transition energy as well as the free carrier effective mass reach minimum values at 100 K, suggesting temperature-driven band inversion in the material. Thus, density function theory calculation for the electronic band structure also make similar predictions.« less

  8. Josephson effects in condensates of excitons and exciton polaritons

    SciTech Connect

    Shelykh, I. A.; Solnyshkov, D. D.; Pavlovic, G.; Malpuech, G.

    2008-07-15

    We analyze theoretically the phenomena related to the Josephson effect for exciton and polariton condensates, taking into account their specific spin degrees of freedom. We distinguish between two types of Josephson effects: the extrinsic effect, related to the coherent tunneling of particles with the same spin between two spatially separated potential traps, and the intrinsic effect, related to the 'tunneling' between different spinor components of the condensate within the same trap. We show that the Josephson effect in the nonlinear regime can lead to nontrivial polarization dynamics and produce spontaneous separation of the condensates with opposite polarization in real space.

  9. Probing excitonic states in suspended two-dimensional semiconductors by photocurrent spectroscopy

    SciTech Connect

    Klots, A. R.; Newaz, A. K. M.; Wang, Bin; Prasai, D.; Krzyzanowska, H.; Lin, Junhao; Caudel, D.; Ghimire, N. J.; Yan, J.; Ivanov, B. L.; Velizhanin, K. A.; Burger, A.; Mandrus, D. G.; Tolk, N. H.; Pantelides, S. T.; Bolotin, K. I.

    2014-10-16

    The optical response of semiconducting monolayer transition-metal dichalcogenides (TMDCs) is dominated by strongly bound excitons that are stable even at room temperature. However, substrate-related effects such as screening and disorder in currently available specimens mask many anticipated physical phenomena and limit device applications of TMDCs. Here, we demonstrate that that these undesirable effects are strongly suppressed in suspended devices. Extremely robust (photogain > 1,000) and fast (response time < 1 ms) photoresponse allow us to study, for the first time, the formation, binding energies, and dissociation mechanisms of excitons in TMDCs through photocurrent spectroscopy. By analyzing the spectral positions of peaks in the photocurrent and by comparing them with first-principles calculations, we obtain binding energies, band gaps and spin-orbit splitting in monolayer TMDCs. For monolayer MoS2, in particular, we obtain an extremely large binding energy for band-edge excitons, Ebind ≥ 570 meV. Along with band-edge excitons, we observe excitons associated with a van Hove singularity of rather unique nature. In conclusion, the analysis of the source-drain voltage dependence of photocurrent spectra reveals exciton dissociation and photoconversion mechanisms in TMDCs.

  10. Probing excitonic states in suspended two-dimensional semiconductors by photocurrent spectroscopy

    DOE PAGESBeta

    Klots, A. R.; Newaz, A. K. M.; Wang, Bin; Prasai, D.; Krzyzanowska, H.; Lin, Junhao; Caudel, D.; Ghimire, N. J.; Yan, J.; Ivanov, B. L.; et al

    2014-10-16

    The optical response of semiconducting monolayer transition-metal dichalcogenides (TMDCs) is dominated by strongly bound excitons that are stable even at room temperature. However, substrate-related effects such as screening and disorder in currently available specimens mask many anticipated physical phenomena and limit device applications of TMDCs. Here, we demonstrate that that these undesirable effects are strongly suppressed in suspended devices. Extremely robust (photogain > 1,000) and fast (response time < 1 ms) photoresponse allow us to study, for the first time, the formation, binding energies, and dissociation mechanisms of excitons in TMDCs through photocurrent spectroscopy. By analyzing the spectral positions ofmore » peaks in the photocurrent and by comparing them with first-principles calculations, we obtain binding energies, band gaps and spin-orbit splitting in monolayer TMDCs. For monolayer MoS2, in particular, we obtain an extremely large binding energy for band-edge excitons, Ebind ≥ 570 meV. Along with band-edge excitons, we observe excitons associated with a van Hove singularity of rather unique nature. In conclusion, the analysis of the source-drain voltage dependence of photocurrent spectra reveals exciton dissociation and photoconversion mechanisms in TMDCs.« less

  11. Probing excitonic states in suspended two-dimensional semiconductors by photocurrent spectroscopy

    PubMed Central

    Klots, A. R.; Newaz, A. K. M.; Wang, Bin; Prasai, D.; Krzyzanowska, H.; Lin, Junhao; Caudel, D.; Ghimire, N. J.; Yan, J.; Ivanov, B. L.; Velizhanin, K. A.; Burger, A.; Mandrus, D. G.; Tolk, N. H.; Pantelides, S. T.; Bolotin, K. I.

    2014-01-01

    The optical response of semiconducting monolayer transition-metal dichalcogenides (TMDCs) is dominated by strongly bound excitons that are stable even at room temperature. However, substrate-related effects such as screening and disorder in currently available specimens mask many anticipated physical phenomena and limit device applications of TMDCs. Here, we demonstrate that that these undesirable effects are strongly suppressed in suspended devices. Extremely robust (photogain > 1,000) and fast (response time < 1 ms) photoresponse allow us to study, for the first time, the formation, binding energies, and dissociation mechanisms of excitons in TMDCs through photocurrent spectroscopy. By analyzing the spectral positions of peaks in the photocurrent and by comparing them with first-principles calculations, we obtain binding energies, band gaps and spin-orbit splitting in monolayer TMDCs. For monolayer MoS2, in particular, we obtain an extremely large binding energy for band-edge excitons, Ebind ≥ 570 meV. Along with band-edge excitons, we observe excitons associated with a van Hove singularity of rather unique nature. The analysis of the source-drain voltage dependence of photocurrent spectra reveals exciton dissociation and photoconversion mechanisms in TMDCs. PMID:25318849

  12. Probing excitonic states in suspended two-dimensional semiconductors by photocurrent spectroscopy

    NASA Astrophysics Data System (ADS)

    Klots, A. R.; Newaz, A. K. M.; Wang, Bin; Prasai, D.; Krzyzanowska, H.; Lin, Junhao; Caudel, D.; Ghimire, N. J.; Yan, J.; Ivanov, B. L.; Velizhanin, K. A.; Burger, A.; Mandrus, D. G.; Tolk, N. H.; Pantelides, S. T.; Bolotin, K. I.

    2014-10-01

    The optical response of semiconducting monolayer transition-metal dichalcogenides (TMDCs) is dominated by strongly bound excitons that are stable even at room temperature. However, substrate-related effects such as screening and disorder in currently available specimens mask many anticipated physical phenomena and limit device applications of TMDCs. Here, we demonstrate that that these undesirable effects are strongly suppressed in suspended devices. Extremely robust (photogain > 1,000) and fast (response time < 1 ms) photoresponse allow us to study, for the first time, the formation, binding energies, and dissociation mechanisms of excitons in TMDCs through photocurrent spectroscopy. By analyzing the spectral positions of peaks in the photocurrent and by comparing them with first-principles calculations, we obtain binding energies, band gaps and spin-orbit splitting in monolayer TMDCs. For monolayer MoS2, in particular, we obtain an extremely large binding energy for band-edge excitons, Ebind >= 570 meV. Along with band-edge excitons, we observe excitons associated with a van Hove singularity of rather unique nature. The analysis of the source-drain voltage dependence of photocurrent spectra reveals exciton dissociation and photoconversion mechanisms in TMDCs.

  13. Ultrafast transient absorption studies of hematite nanoparticles: the effect of particle shape on exciton dynamics.

    PubMed

    Fitzmorris, Bob C; Patete, Jonathan M; Smith, Jacqueline; Mascorro, Xiomara; Adams, Staci; Wong, Stanislaus S; Zhang, Jin Z

    2013-10-01

    Much progress has been made in using hematite (α-Fe2 O3 ) as a potentially practical and sustainable material for applications such as solar-energy conversion and photoelectrochemical (PEC) water splitting; however, recent studies have shown that the performance can be limited by a very short charge-carrier diffusion length or exciton lifetime. In this study, we performed ultrafast studies on hematite nanoparticles of different shapes to determine the possible influence of particle shape on the exciton dynamics. Nanorice, multifaceted spheroidal nanoparticles, faceted nanocubes, and faceted nanorhombohedra were synthesized and characterized by using SEM and XRD techniques. Their exciton dynamics were investigated by using femtosecond transient absorption (TA) spectroscopy. Although the TA spectral features differ for the four samples studied, their decay profiles are similar, which can be fitted with time constants of 1-3 ps, approximately 25 ps, and a slow nanosecond component extending beyond the experimental time window that was measured (2 ns). The results indicate that the overall exciton lifetime is weakly dependent on the shape of the hematite nanoparticles, even though the overall optical absorption and scattering are influenced by the particle shape. This study suggests that other strategies need to be developed to increase the exciton lifetime or to lengthen the exciton diffusion length in hematite nanostructures. PMID:24058060

  14. Phase conjugation and adiabatic mode conversion in a driven optical parametric oscillator with orbital angular momentum

    SciTech Connect

    Coutinho dos Santos, B.; Souza, C. E. R.; Dechoum, K.; Khoury, A. Z.

    2007-11-15

    We developed a theoretical model for the spatial mode dynamics of an optical parametric oscillator under injection of orbital angular momentum. This process is interpreted in terms of a Poincare representation of first order spatial modes. The spatial properties of the down-converted fields can be easily understood from their symmetries in this geometric representation. By considering an adiabatic mode conversion of the injected signal, we calculate the evolution of the down-converted beams. A phase conjugation effect is predicted which is a consequence of the symmetry in the Poincare sphere. We also propose an experiment to measure this effect.

  15. Collective atomic motion and spin dynamics in a driven optical cavity

    NASA Astrophysics Data System (ADS)

    Stamper-Kurn, Dan

    2016-05-01

    Cavity quantum electrodynamics generally highlights the interchange of quantum noise and information between light and matter. I will discuss experiments in which the collective motion and spin of a trapped gas of ultracold atoms interact with and are detected by light in a single mode of a high-finesse optical cavity. I will present recent results on quantum-limited force detection, on the damping and amplification of Larmor precession through dynamical backaction, and on cavity-induced coupling between mechanical oscillators and between spin and motional degrees of freedom.

  16. Injected-charge-driven increase in electro-optic effect of KTN crystals

    SciTech Connect

    Toyoda, Seiji; Imai, Tadayuki; Miyazu, Jun; Okabe, Yuichi; Ueno, Masahiro; Kobayashi, Junya

    2014-05-15

    We report a significant increase in the electro-optic (EO) effect of KTa{sub x}Nb{sub 1-x}O{sub 3} (KTN) crystals that we achieved by injecting carriers into them. The dielectric constant of KTN was increased approximately twofold by carrier injection. The EO beam scanning performance was effectively improved by the increase in the EO effect resulting from the increased dielectric constant. The estimated densities of the trapped electrons were as small as 5.8 × 10{sup 20}m{sup -3}. The very small quantity of injected electrons greatly affected the dielectric constant and EO effect of the KTN crystals.

  17. Lightwave-driven quasiparticle collisions on a subcycle timescale.

    PubMed

    Langer, F; Hohenleutner, M; Schmid, C P; Poellmann, C; Nagler, P; Korn, T; Schüller, C; Sherwin, M S; Huttner, U; Steiner, J T; Koch, S W; Kira, M; Huber, R

    2016-05-12

    Ever since Ernest Rutherford scattered α-particles from gold foils, collision experiments have revealed insights into atoms, nuclei and elementary particles. In solids, many-body correlations lead to characteristic resonances--called quasiparticles--such as excitons, dropletons, polarons and Cooper pairs. The structure and dynamics of quasiparticles are important because they define macroscopic phenomena such as Mott insulating states, spontaneous spin- and charge-order, and high-temperature superconductivity. However, the extremely short lifetimes of these entities make practical implementations of a suitable collider challenging. Here we exploit lightwave-driven charge transport, the foundation of attosecond science, to explore ultrafast quasiparticle collisions directly in the time domain: a femtosecond optical pulse creates excitonic electron-hole pairs in the layered dichalcogenide tungsten diselenide while a strong terahertz field accelerates and collides the electrons with the holes. The underlying dynamics of the wave packets, including collision, pair annihilation, quantum interference and dephasing, are detected as light emission in high-order spectral sidebands of the optical excitation. A full quantum theory explains our observations microscopically. This approach enables collision experiments with various complex quasiparticles and suggests a promising new way of generating sub-femtosecond pulses. PMID:27172045

  18. Lightwave-driven quasiparticle collisions on a subcycle timescale

    NASA Astrophysics Data System (ADS)

    Langer, F.; Hohenleutner, M.; Schmid, C. P.; Poellmann, C.; Nagler, P.; Korn, T.; Schüller, C.; Sherwin, M. S.; Huttner, U.; Steiner, J. T.; Koch, S. W.; Kira, M.; Huber, R.

    2016-05-01

    Ever since Ernest Rutherford scattered α-particles from gold foils, collision experiments have revealed insights into atoms, nuclei and elementary particles. In solids, many-body correlations lead to characteristic resonances—called quasiparticles—such as excitons, dropletons, polarons and Cooper pairs. The structure and dynamics of quasiparticles are important because they define macroscopic phenomena such as Mott insulating states, spontaneous spin- and charge-order, and high-temperature superconductivity. However, the extremely short lifetimes of these entities make practical implementations of a suitable collider challenging. Here we exploit lightwave-driven charge transport, the foundation of attosecond science, to explore ultrafast quasiparticle collisions directly in the time domain: a femtosecond optical pulse creates excitonic electron–hole pairs in the layered dichalcogenide tungsten diselenide while a strong terahertz field accelerates and collides the electrons with the holes. The underlying dynamics of the wave packets, including collision, pair annihilation, quantum interference and dephasing, are detected as light emission in high-order spectral sidebands of the optical excitation. A full quantum theory explains our observations microscopically. This approach enables collision experiments with various complex quasiparticles and suggests a promising new way of generating sub-femtosecond pulses.

  19. Driven-dissipative many-body pairing states for cold fermionic atoms in an optical lattice

    NASA Astrophysics Data System (ADS)

    Yi, W.; Diehl, S.; Daley, A. J.; Zoller, P.

    2012-05-01

    We discuss the preparation of many-body states of cold fermionic atoms in an optical lattice via controlled dissipative processes induced by coupling the system to a reservoir. Based on a mechanism combining Pauli blocking and phase locking between adjacent sites, we construct complete sets of jump operators describing coupling to a reservoir that leads to dissipative preparation of pairing states for fermions with various symmetries in the absence of direct inter-particle interactions. We discuss the uniqueness of these states, and demonstrate it with small-scale numerical simulations. In the late-time dissipative dynamics, we identify a ‘dissipative gap’ that persists in the thermodynamic limit. This gap implies exponential convergence of all many-body observables to their steady-state values. We then investigate how these pairing states can be used as a starting point for the preparation of the ground state of the Fermi-Hubbard Hamiltonian via an adiabatic state preparation process also involving the parent Hamiltonian of the pairing state. We also provide a proof-of-principle example for implementing these dissipative processes and the parent Hamiltonians of the pairing states, based on 171Yb atoms in optical lattice potentials.

  20. Observation of non-Hermitian degeneracies in a chaotic exciton-polariton billiard

    NASA Astrophysics Data System (ADS)

    Gao, T.; Estrecho, E.; Bliokh, K. Y.; Liew, T. C. H.; Fraser, M. D.; Brodbeck, S.; Kamp, M.; Schneider, C.; Höfling, S.; Yamamoto, Y.; Nori, F.; Kivshar, Y. S.; Truscott, A. G.; Dall, R. G.; Ostrovskaya, E. A.

    2015-10-01

    Exciton-polaritons are hybrid light-matter quasiparticles formed by strongly interacting photons and excitons (electron-hole pairs) in semiconductor microcavities. They have emerged as a robust solid-state platform for next-generation optoelectronic applications as well as for fundamental studies of quantum many-body physics. Importantly, exciton-polaritons are a profoundly open (that is, non-Hermitian) quantum system, which requires constant pumping of energy and continuously decays, releasing coherent radiation. Thus, the exciton-polaritons always exist in a balanced potential landscape of gain and loss. However, the inherent non-Hermitian nature of this potential has so far been largely ignored in exciton-polariton physics. Here we demonstrate that non-Hermiticity dramatically modifies the structure of modes and spectral degeneracies in exciton-polariton systems, and, therefore, will affect their quantum transport, localization and dynamical properties. Using a spatially structured optical pump, we create a chaotic exciton-polariton billiard--a two-dimensional area enclosed by a curved potential barrier. Eigenmodes of this billiard exhibit multiple non-Hermitian spectral degeneracies, known as exceptional points. Such points can cause remarkable wave phenomena, such as unidirectional transport, anomalous lasing/absorption and chiral modes. By varying parameters of the billiard, we observe crossing and anti-crossing of energy levels and reveal the non-trivial topological modal structure exclusive to non-Hermitian systems. We also observe mode switching and a topological Berry phase for a parameter loop encircling the exceptional point. Our findings pave the way to studies of non-Hermitian quantum dynamics of exciton-polaritons, which may uncover novel operating principles for polariton-based devices.

  1. Observation of non-Hermitian degeneracies in a chaotic exciton-polariton billiard.

    PubMed

    Gao, T; Estrecho, E; Bliokh, K Y; Liew, T C H; Fraser, M D; Brodbeck, S; Kamp, M; Schneider, C; Höfling, S; Yamamoto, Y; Nori, F; Kivshar, Y S; Truscott, A G; Dall, R G; Ostrovskaya, E A

    2015-10-22

    Exciton-polaritons are hybrid light-matter quasiparticles formed by strongly interacting photons and excitons (electron-hole pairs) in semiconductor microcavities. They have emerged as a robust solid-state platform for next-generation optoelectronic applications as well as for fundamental studies of quantum many-body physics. Importantly, exciton-polaritons are a profoundly open (that is, non-Hermitian) quantum system, which requires constant pumping of energy and continuously decays, releasing coherent radiation. Thus, the exciton-polaritons always exist in a balanced potential landscape of gain and loss. However, the inherent non-Hermitian nature of this potential has so far been largely ignored in exciton-polariton physics. Here we demonstrate that non-Hermiticity dramatically modifies the structure of modes and spectral degeneracies in exciton-polariton systems, and, therefore, will affect their quantum transport, localization and dynamical properties. Using a spatially structured optical pump, we create a chaotic exciton-polariton billiard--a two-dimensional area enclosed by a curved potential barrier. Eigenmodes of this billiard exhibit multiple non-Hermitian spectral degeneracies, known as exceptional points. Such points can cause remarkable wave phenomena, such as unidirectional transport, anomalous lasing/absorption and chiral modes. By varying parameters of the billiard, we observe crossing and anti-crossing of energy levels and reveal the non-trivial topological modal structure exclusive to non-Hermitian systems. We also observe mode switching and a topological Berry phase for a parameter loop encircling the exceptional point. Our findings pave the way to studies of non-Hermitian quantum dynamics of exciton-polaritons, which may uncover novel operating principles for polariton-based devices. PMID:26458102

  2. Role of many-body effects in the coherent dynamics of excitons in low-temperature-grown GaAs

    SciTech Connect

    Webber, D.; Hacquebard, L.; Hall, K. C.; Liu, X.; Dobrowolska, M.; Furdyna, J. K.

    2015-10-05

    Femtosecond four-wave mixing experiments on low-temperature-grown (LT-) GaAs indicate a polarization-dependent nonlinear optical response at the exciton, which we attribute to Coulomb-mediated coupling between excitons and electron-hole pairs simultaneously excited by the broad-bandwidth laser pulses. Strong suppression of the exciton response through screening by carriers injected by a third pump pulse was observed, an effect that is transient due to rapid carrier trapping. Our findings highlight the need to account for the complex interplay of disorder and many-body effects in the design of ultrafast optoelectronic devices using this material.

  3. Observation of excitonic super-radiance in quantum well structures and its application for laser cooling of solids

    NASA Astrophysics Data System (ADS)

    Hassani Nia, Iman; Weinberg, David; Wheaton, Skylar; Weiss, Emily A.; Mohseni, Hooman

    2016-03-01

    Excitons, bound electron-hole pairs, possess distinct physical properties from free electrons and holes that can be employed to improve the performance of optoelectronic devices. In particular, the signatures of excitons are enhanced optical absorption and radiative emission. These characteristics could be of major benefit for the laser cooling of semiconductors, a process which has stringent requirements on the parasitic absorption of incident radiation and the internal quantum efficiency. Here we experimentally demonstrate the dominant ultrafast excitonic super-radiance of our quantum well structure from 78 K up to room temperature. The experimental results are followed by our detailed discussions about the advantages and limitations of this method.

  4. Noncircular semiconductor nanorings of types I and II: Emission kinetics in the excitonic Aharonov-Bohm effect

    NASA Astrophysics Data System (ADS)

    Grochol, Michal; Zimmermann, Roland

    2007-11-01

    Transition energies and oscillator strengths of excitons in dependence on magnetic field are investigated in types I and II semiconductor nanorings. A slight deviation from circular (concentric) shape of the type II nanoring gives a better observability of the Aharonov-Bohm oscillations since the ground state is always optically active. Kinetic equations for the exciton occupation are solved with acoustic phonon scattering as the major relaxation process, and absorption and luminescence spectra are calculated, showing deviations from equilibrium. The presence of a nonradiative exciton decay leads to a quenching of the integrated photoluminescence with magnetic field.

  5. Population Pulsation Resonances of Excitons in Monolayer MoSe 2 with Sub- 1 μ eV Linewidths

    DOE PAGESBeta

    Schaibley, John R.; Karin, Todd; Yu, Hongyi; Ross, Jason S.; Rivera, Pasqual; Jones, Aaron M.; Scott, Marie E.; Yan, Jiaqiang; Mandrus, D. G.; Yao, Wang; et al

    2015-04-01

    Monolayer transition metal dichalcogenides, a new class of atomically thin semiconductors, possess optically coupled 2D valley excitons. The nature of exciton relaxation in these systems is currently poorly understood. Here, we investigate exciton relaxation in monolayer MoSe₂ using polarization-resolved coherent nonlinear optical spectroscopy with high spectral resolution. We report strikingly narrow population pulsation resonances with two different characteristic linewidths of 1 and <0.2 μeV at low temperature. These linewidths are more than 3 orders of magnitude narrower than the photoluminescence and absorption linewidth, and indicate that a component of the exciton relaxation dynamics occurs on time scales longer than 1more » ns. The ultranarrow resonance (<0.2 μeV) emerges with increasing excitation intensity, and implies the existence of a long-lived state whose lifetime exceeds 6 ns.« less

  6. Single-pulse driven, large-aperture 2×1 array plasma-electrodes optical switch for SG-II upgrading facility

    NASA Astrophysics Data System (ADS)

    Zhang, Jun; Wu, Dengsheng; Zheng, Jiangang; Zheng, Kuixing; Zhu, Qihua; Zhang, Xiongjun

    2014-12-01

    We demonstrate the design and performance of an optical switch that has been constructed for the SG-II upgrading facility. The device is a longitudinal, potassium di-hydrogen phosphate (KDP), 360 mm×360 mm aperture, and 2×1 array electro-optical switch driven by a 20 kV output switching-voltage pulse generator through two plasma electrodes produced at the rise edge of the switching-voltage pulse. The results show that the temporal responses and the spatial performance of the optical switch fulfill the operation requirements of the SG-II upgrading facility.

  7. DNA-mediated excitonic upconversion FRET switching

    NASA Astrophysics Data System (ADS)

    Kellis, Donald L.; Rehn, Sarah M.; Cannon, Brittany L.; Davis, Paul H.; Graugnard, Elton; Lee, Jeunghoon; Yurke, Bernard; Knowlton, William B.

    2015-11-01

    Excitonics is a rapidly expanding field of nanophotonics in which the harvesting of photons, ensuing creation and transport of excitons via Förster resonant energy transfer (FRET), and subsequent charge separation or photon emission has led to the demonstration of excitonic wires, switches, Boolean logic and light harvesting antennas for many applications. FRET funnels excitons down an energy gradient resulting in energy loss with each step along the pathway. Conversely, excitonic energy upconversion via upconversion nanoparticles (UCNPs), although currently inefficient, serves as an energy ratchet to boost the exciton energy. Although FRET-based upconversion has been demonstrated, it suffers from low FRET efficiency and lacks the ability to modulate the FRET. We have engineered an upconversion FRET-based switch by combining lanthanide-doped UCNPs and fluorophores that demonstrates excitonic energy upconversion by nearly a factor of 2, an excited state donor to acceptor FRET efficiency of nearly 25%, and an acceptor fluorophore quantum efficiency that is close to unity. These findings offer a promising path for energy upconversion in nanophotonic applications including artificial light harvesting, excitonic circuits, photovoltaics, nanomedicine, and optoelectronics.

  8. DNA-mediated excitonic upconversion FRET switching

    SciTech Connect

    Kellis, Donald L.; Rehn, Sarah M.; Cannon, Brittany L.; Davis, Paul H.; Graugnard, Elton; Lee, Jeunghoon; Yurke, Bernard; Knowlton, William B.

    2015-11-17

    Excitonics is a rapidly expanding field of nanophotonics in which the harvesting of photons, ensuing creation and transport of excitons via Förster resonant energy transfer (FRET), and subsequent charge separation or photon emission has led to the demonstration of excitonic wires, switches, Boolean logic and light harvesting antennas for many applications. FRET funnels excitons down an energy gradient resulting in energy loss with each step along the pathway. Conversely, excitonic energy up conversion via up conversion nanoparticles (UCNPs), although currently inefficient, serves as an energy ratchet to boost the exciton energy. Although FRET-based up conversion has been demonstrated, it suffers from low FRET efficiency and lacks the ability to modulate the FRET. We have engineered an up conversion FRET-based switch by combining lanthanide-doped UCNPs and fluorophores that demonstrates excitonic energy up conversion by nearly a factor of 2, an excited state donor to acceptor FRET efficiency of nearly 25%, and an acceptor fluorophore quantum efficiency that is close to unity. These findings offer a promising path for energy up conversion in nanophotonic applications including artificial light harvesting, excitonic circuits, photovoltaics, nanomedicine, and optoelectronics.

  9. DNA-mediated excitonic upconversion FRET switching

    DOE PAGESBeta

    Kellis, Donald L.; Rehn, Sarah M.; Cannon, Brittany L.; Davis, Paul H.; Graugnard, Elton; Lee, Jeunghoon; Yurke, Bernard; Knowlton, William B.

    2015-11-17

    Excitonics is a rapidly expanding field of nanophotonics in which the harvesting of photons, ensuing creation and transport of excitons via Förster resonant energy transfer (FRET), and subsequent charge separation or photon emission has led to the demonstration of excitonic wires, switches, Boolean logic and light harvesting antennas for many applications. FRET funnels excitons down an energy gradient resulting in energy loss with each step along the pathway. Conversely, excitonic energy up conversion via up conversion nanoparticles (UCNPs), although currently inefficient, serves as an energy ratchet to boost the exciton energy. Although FRET-based up conversion has been demonstrated, it suffersmore » from low FRET efficiency and lacks the ability to modulate the FRET. We have engineered an up conversion FRET-based switch by combining lanthanide-doped UCNPs and fluorophores that demonstrates excitonic energy up conversion by nearly a factor of 2, an excited state donor to acceptor FRET efficiency of nearly 25%, and an acceptor fluorophore quantum efficiency that is close to unity. These findings offer a promising path for energy up conversion in nanophotonic applications including artificial light harvesting, excitonic circuits, photovoltaics, nanomedicine, and optoelectronics.« less

  10. Valley dynamics probed through charged and neutral exciton emission in monolayer WSe2

    NASA Astrophysics Data System (ADS)

    Wang, G.; Bouet, L.; Lagarde, D.; Vidal, M.; Balocchi, A.; Amand, T.; Marie, X.; Urbaszek, B.

    2014-08-01

    Optical interband transitions in monolayer transition metal dichalcogenides such as WSe2 and MoS2 are governed by chiral selection rules. This allows efficient optical initialization of an electron in a specific K valley in momentum space. Here we probe the valley dynamics in monolayer WSe2 by monitoring the emission and polarization dynamics of the well-separated neutral excitons (bound electron-hole pairs) and charged excitons (trions) in photoluminescence. The neutral exciton photoluminescence intensity decay time is about 4 ps, whereas the trion emission occurs over several tens of ps. The trion polarization dynamics shows a partial, fast initial decay within tens of ps before reaching a stable polarization of ≈20%, for which a typical valley polarization decay time of the order of 1 ns can be inferred.

  11. Geminate and non-geminate recombination of triplet excitons formed by singlet fission

    NASA Astrophysics Data System (ADS)

    Bayliss, Sam L.; Chepelianskii, Alexei; Sepe, Alessandro; Ehrler, Bruno; Walker, Brian J.; Bruzek, Matt J.; Anthony, John E.; Greenham, Neil C.

    2014-03-01

    Singlet fission is a promising route to enhance solar cells by harvesting two electron-hole pairs from high-energy photons. Through singlet fission, an optically generated singlet exciton is transformed into two spin-correlated triplet excitons, which serve as a unique signature of the process. We use optically detected magnetic resonance to identify and study triplet excitons created through singlet fission in the solution-processable small molecule TIPS-tetracene (bis(triisopropylsilylethynyl)tetracene). Through changes in photoluminescence under spin resonance, we identify geminate recombination of triplet pairs directly following singlet fission, as well as recombination from bimolecular triplet-triplet annihilation. We show that both processes can be present in spin-coated films, and correlate the two distinct annihilation pathways to film morphology.

  12. Tailoring double Fano profiles with plasmon-assisted quantum interference in hybrid exciton-plasmon system

    SciTech Connect

    Zhao, Dongxing; Wu, Jiarui; Gu, Ying Gong, Qihuang

    2014-09-15

    We propose tailoring of the double Fano profiles via plasmon-assisted quantum interference in a hybrid exciton-plasmon system. Tailoring is performed by the interference between two exciton channels interacting with a common localized surface plasmon. Using an applied field of low intensity, the absorption spectrum of the hybrid system reveals a double Fano lineshape with four peaks. For relatively large field intensity, a broad flat window in the absorption spectrum appears which results from the destructive interference between excitons. Because of strong constructive interference, this window vanishes as intensity is further increased. We have designed a nanometer bandpass optical filter for visible light based on tailoring of the optical spectrum. This study provides a platform for quantum interference that may have potential applications in ultracompact tunable quantum devices.

  13. Delicate and robust dynamical recurrences of matter waves in driven optical crystals

    NASA Astrophysics Data System (ADS)

    Ayub, Muhammad; Saif, Farhan

    2012-02-01

    We study dynamical recurrences of a Bose-Einstein condensate in an optical crystal subject to a periodic external driving force. The recurrence behavior of the condensate is analyzed as a function of time close to nonlinear resonances occurring in the classical counterpart. Our mathematical formalism for the recurrence time scales is presented as delicate recurrences, which take place, for instance, when the lattice is perturbed weakly and robust recurrences, which may manifest themselves for a sufficiently strong external driving force. The analysis not only is valid for a dilute condensate, but also is applicable for the strongly interacting homogeneous condensate provided; the external modulation causes no significant change in the density profile of the condensate. We explain the parametric dependence of the dynamical recurrence times, which can easily be realized in laboratory experiments. In addition, we find good agreement between the obtained analytical results and the numerical calculations.

  14. Optically driven nanostructures as the basis for large-scale quantum computing

    NASA Astrophysics Data System (ADS)

    Tsukanov, Alexander V.

    2008-03-01

    We propose a large-scale quantum computer architecture based upon the regular arrays of dopant atoms implanted into the semiconductor host matrix. The singly-ionized pairs of donors represent charge qubits on which arbitrary quantum operations can be achieved by application of two strongly detuned laser pulses. The implementation of two-qubit operations as well as the qubit read-out utilize the intermediate circuit containing a probe electron that is able to shuttle along the array of ionized ancilla donors providing the indirect conditional coupling between the qubits. The quantum bus strategy enables us to handle the qubits connected in parallel and enhances the efficiency of the quantum information processing. We demonstrate that non-trivial multi-qubit operations in the quantum register (e.g., an entanglement generation) can be accomplished by the sequence of the optical pulses combined with an appropriate voltage gate pattern.

  15. Electro-optical properties of low viscosity driven holographic polymer dispersed liquid crystals

    NASA Astrophysics Data System (ADS)

    Moon, K. R.; Bae, S. Y.; Kim, B. K.

    2015-04-01

    Relative diffraction efficiency (RDE), operating voltage, and response times are most important performance characteristics of holographic polymer dispersed liquid crystals (HPDLC). Two types of triallyl isocyanurate (TI) having different structures were incorporated into the conventional transmission grating of HPDLC. Premix viscosity decreased by 13-18% with up to 3% TI, beyond which it increased. TI eliminated induction period and augmented initial grating formation rate at all contents. Saturation RDE increased over 200% while threshold voltage and rise time decreased to about half and 2/3, respectively up to 3% TI, beyond which the tendencies were reversed. Among the two TIs, low viscosity monomer (TA) showed high RDE, while high miscibility monomer (TE) low characteristic voltages and short response times. It is concluded that grating formation is largely favored by low viscosity, while interface tensions and electro-optical performances by miscibility at similar viscosities.

  16. Excitonic superconductivity in copper oxides

    SciTech Connect

    Tesanovic, Z.; Bishop, A.R.; Martin, R.L.; Harris, C.

    1988-01-01

    We discuss the possibility of excitonic superconductivity in high T/sub c/ copper oxides. The Hamiltonians describing CuO/sub 2/ planes supports both antiferromagnetism and low-lying Cu /longleftrightarrow/ O intra- and interband charge fluctuations. One crosses from one regime to another as the number of holes per unit cell increases. The high T/sub c/ superconductivity takes place at hole concentrations most favorable for intraband charge transfer excitations. The dynamic polarizability of the environment surrounding CuO/sub 2/ planes plays an important role in enhancing T/sub c/. 15 refs., 4 figs.

  17. The Structure and Dynamics of Molecular Excitons

    NASA Astrophysics Data System (ADS)

    Bardeen, Christopher J.

    2014-04-01

    The photophysical behavior of organic semiconductors is governed by their excitonic states. In this review, I classify the three different exciton types (Frenkel singlet, Frenkel triplet, and charge transfer) typically encountered in organic semiconductors. Experimental challenges that arise in the study of solid-state organic systems are discussed. The steady-state spectroscopy of intermolecular delocalized Frenkel excitons is described, using crystalline tetracene as an example. I consider the problem of a localized exciton diffusing in a disordered matrix in detail, and experimental results on conjugated polymers and model systems suggest that energetic disorder leads to subdiffusive motion. Multiexciton processes such as singlet fission and triplet fusion are described, emphasizing the role of spin state coherence and magnetic fields in studying singlet -- triplet pair interconversion. Singlet fission provides an example of how all three types of excitons (triplet, singlet, and charge transfer) may interact to produce useful phenomena for applications such as solar energy conversion.

  18. Thermodynamic efficiency limit of excitonic solar cells

    SciTech Connect

    Giebink, Noel C.; Wiederrecht, Gary P.; Wasielewski, Michael R.; Forrest, Stephen R.

    2011-01-01

    Excitonic solar cells, comprised of materials such as organic semiconductors, inorganic colloidal quantum dots, and carbon nanotubes, are fundamentally different than crystalline, inorganic solar cells in that photogeneration of free charge occurs through intermediate, bound exciton states. Here, we show that the Second Law of Thermodynamics limits the maximum efficiency of excitonic solar cells below the maximum of 31% established by Shockley and Queisser [J. Appl. Phys. 32, 510 (1961)] for inorganic solar cells (whose exciton-binding energy is small). In the case of ideal heterojunction excitonic cells, the free energy for charge transfer at the interface, ΔG, places an additional constraint on the limiting efficiency due to a fundamental increase in the recombination rate, with typical -ΔG in the range 0.3 to 0.5 eV decreasing the maximum efficiency to 27% and 22%, respectively.

  19. Broadband Absorbing Exciton-Plasmon Metafluids with Narrow Transparency Windows.

    PubMed

    Yang, Jihua; Kramer, Nicolaas J; Schramke, Katelyn S; Wheeler, Lance M; Besteiro, Lucas V; Hogan, Christopher J; Govorov, Alexander O; Kortshagen, Uwe R

    2016-02-10

    Optical metafluids that consist of colloidal solutions of plasmonic and/or excitonic nanomaterials may play important roles as functional working fluids or as means for producing solid metamaterial coatings. The concept of a metafluid employed here is based on the picture that a single ballistic photon, propagating through the metafluid, interacts with a large collection of specifically designed optically active nanocrystals. We demonstrate water-based metafluids that act as broadband electromagnetic absorbers in a spectral range of 200-3300 nm and feature a tunable narrow (∼100 nm) transparency window in the visible-to-near-infrared region. To define this transparency window, we employ plasmonic gold nanorods. We utilize excitonic boron-doped silicon nanocrystals as opaque optical absorbers ("optical wall") in the UV and blue-green range of the spectrum. Water itself acts as an opaque "wall" in the near-infrared to infrared. We explore the limits of the concept of a "simple" metafluid by computationally testing and validating the effective medium approach based on the Beer-Lambert law. According to our simulations and experiments, particle aggregation and the associated decay of the window effect are one example of the failure of the simple metafluid concept due to strong interparticle interactions. PMID:26808215

  20. Excitonic transitions in spherical inhomogeneous QD, new monocolor nanosource

    NASA Astrophysics Data System (ADS)

    Benhaddou, F.; Zorkani, I.; Jorio, A.; Feddi, E.

    2015-11-01

    We study in this investigation the excitonic transitions in new spherical nanosystems also called inhomogeneous quantum dots IQD. They are promising in many technological applications: photovoltaic, LED, QD Laser and quantum computing. The excitonic binding energy significantly increases; which gives them greater stability at room temperature. The well-semiconductors in these nanostructures become luminescent under dual control core-well, in a wide spectral range from near UV to near and medium infrared IR. These optical properties enriched the field of IQD which generally have a high quantum efficiency and high photostability. The IQD presented are made out off ZnSe/HgS/ZnSe; CdS/GaSb/CdS; ZnS/HgS/ZnS and CdS/InSb/CdS modeled by a spherical well with infinite potential. Our theoretical investigation shows that the high degree of confinement in the well retains the 1 se - 1 pe - 2 se (1 sh - 1 ph - 2 sh) order, guarantees excitonic transitions and isolates the ground state 1 se - 1 sh (E2se,h - E1pe,h can be exceed 6 eV). The strong confinement provided by the infinite barrier, reduces the population relaxation and limit the coupling between the well and the electrostatic environment. These results qualify the nanostructure as a monocolor source and a system of two levels.

  1. Enhancement of the Aharonov-Bohm effect of neutral excitons in semiconductor nanorings with an electric field

    NASA Astrophysics Data System (ADS)

    Maslov, A. V.; Citrin, D. S.

    2003-03-01

    This work demonstrates that the Aharonov-Bohm effect for excitons, practically indistinguishable from the numerical noise without an applied electric field, becomes clearly evident in the optical absorption once the electric field is applied in the plane containing the nanoring. The enhancement arises as a result of the field-induced delocalization of the relative electron-hole motion around the entire ring. The excitonic effects are essential to describe even qualitatively the absorption spectra.

  2. Line-driven ablation of circumstellar discs – I. Optically thin decretion discs of classical Oe/Be stars

    PubMed Central

    Kee, Nathaniel Dylan; Owocki, Stanley; Sundqvist, J. O.

    2016-01-01

    discussion of future extensions to study line-driven ablation of denser, optically thick, accretion discs of pre-main-sequence massive stars. PMID:27346978

  3. Line-driven ablation of circumstellar discs - I. Optically thin decretion discs of classical Oe/Be stars

    NASA Astrophysics Data System (ADS)

    Kee, Nathaniel Dylan; Owocki, Stanley; Sundqvist, J. O.

    2016-05-01

    discussion of future extensions to study line-driven ablation of denser, optically thick, accretion discs of pre-main-sequence massive stars.

  4. A self-stabilized coherent phonon source driven by optical forces

    PubMed Central

    Navarro-Urrios, D.; Capuj, N. E.; Gomis-Bresco, J.; Alzina, F.; Pitanti, A.; Griol, A.; Martínez, A.; Sotomayor Torres, C. M.

    2015-01-01

    We report a novel injection scheme that allows for “phonon lasing” in a one-dimensional opto-mechanical photonic crystal, in a sideband unresolved regime and with cooperativity values as low as 10−2. It extracts energy from a cw infrared laser source and is based on the triggering of a thermo-optical/free-carrier-dispersion self-pulsing limit-cycle, which anharmonically modulates the radiation pressure force. The large amplitude of the coherent mechanical motion acts as a feedback that stabilizes and entrains the self-pulsing oscillations to simple fractions of the mechanical frequency. A manifold of frequency-entrained regions with two different mechanical modes (at 54 and 122 MHz) are observed as a result of the wide tuneability of the natural frequency of the self-pulsing. The system operates at ambient conditions of pressure and temperature in a silicon platform, which enables its exploitation in sensing, intra-chip metrology or time-keeping applications. PMID:26503448

  5. Optical signatures of electric-field-driven magnetic phase transitions in graphene quantum dots

    NASA Astrophysics Data System (ADS)

    Basak, Tista; Shukla, Alok

    2016-06-01

    Experimental challenges in identifying various types of magnetic ordering in graphene quantum dots (QDs) pose a major hurdle in the application of these nanostructures for spintronic devices. Based upon phase diagrams obtained by employing the π -electron Pariser-Parr-Pople (PPP) model Hamiltonian, we demonstrate that the magnetic states undergo phase transition under the influence of an external electric field. Our calculations of the electroabsorption spectra of these QDs indicate that the spectrum in question carries strong signatures of their magnetic state (FM vs AFM), thus suggesting the possibility of an all-optical characterization of their magnetic nature. Further, the gaps for the up and the down spins are the same in the absence of an external electric field, both for the antiferromagnetic (AFM) and the ferromagnetic (FM) states of QDs. But, once the QDs are exposed to a suitably directed external electric field, gaps for different spins split and exhibit distinct variations with respect to the strength of the field. The nature of variation exhibited by the energy gaps corresponding to the up and down spins is different for the AFM and FM configurations of QDs. This selective manipulation of the spin-polarized gap splitting by an electric field in finite graphene nanostructures can open up new frontiers in the design of graphene-based spintronic devices.

  6. Thermal radiation from optically driven Kerr (χ{sup (3)}) photonic cavities

    SciTech Connect

    Khandekar, Chinmay; Rodriguez, Alejandro W.; Lin, Zin

    2015-04-13

    We describe thermal radiation from nonlinear (χ{sup (3)}) photonic cavities coupled to external channels and subject to incident monochromatic light. Our work extends related work on nonlinear mechanical oscillators to the problem of thermal radiation, demonstrating that bistability can enhance thermal radiation by orders of magnitude and result in strong lineshape alternations, including “super-narrow spectral peaks” occurring at the onset of kinetic phase transitions. We show that when the cavities are designed to exhibit perfect linear emissivity (rate matching), such thermally activated transitions can be exploited to dramatically tune the output power and radiative properties of the cavity, leading to a kind of Kerr-mediated thermo-optic effect. Finally, we demonstrate that in certain parameter regimes, the output radiation exhibits Stokes and anti-Stokes side peaks whose relative magnitudes can be altered by tuning the internal temperature of the cavity relative to its surroundings, a consequence of strong correlations and interference between the emitted and reflected radiation.

  7. A Geometry-Driven Optical Flow Warping for Spatial Normalization of Cortical Surfaces

    PubMed Central

    Tosun, Duygu; Prince, Jerry L.

    2008-01-01

    Spatial normalization is frequently used to map data to a standard coordinate system by removing inter-subject morphological differences, thereby allowing for group analysis to be carried out. The work presented in this paper is motivated by the need for an automated cortical surface normalization technique that will automatically identify homologous cortical landmarks and map them to the same coordinates on a standard manifold. The geometry of a cortical surface is analyzed using two shape measures that distinguish the sulcal and gyral regions in a multi-scale framework. A multichannel optical flow warping procedure aligns these shape measures between a reference brain and a subject brain, creating the desired normalization. The partial differential equation that carries out the warping is implemented in a Euclidean framework in order to facilitate a multi-resolution strategy, thereby permitting large deformations between the two surfaces. The technique is demonstrated by aligning 33 normal cortical surfaces and showing both improved structural alignment in manually labeled sulci and improved functional alignment in positron emission tomography data mapped to the surfaces. A quantitative comparison between our proposed surface-based spatial normalization method and a leading volumetric spatial normalization method is included to show that the surface-based spatial normalization performs better in matching homologous cortical anatomies. PMID:19033090

  8. Emission energy, exciton dynamics and lasing properties of buckled CdS nanoribbons.

    PubMed

    Wang, Qi; Sun, Liaoxin; Lu, Jian; Ren, Ming-Liang; Zhang, Tianning; Huang, Yan; Zhou, Xiaohao; Sun, Yan; Zhang, Bo; Chen, Changqing; Shen, Xuechu; Agarwal, Ritesh; Lu, Wei

    2016-01-01

    We report the modulation of emission energy, exciton dynamics and lasing properties in a single buckled CdS nanoribbon (NR) by strain-engineering. Inspired by ordered structure fabrication on elastomeric polymer, we develop a new method to fabricate uniform buckled NRs supported on polydimethylsiloxane (PDMS). Wavy structure, of which compressive and tensile strain periodically varied along the CdS NR, leads to a position-dependent emission energy shift as large as 14 nm in photoluminescence (PL) mapping. Both micro-PL and micro-reflectance reveal the spectral characteristics of broad emission of buckled NR, which can be understood by the discrepancy of strain-induced energy shift of A- and B-exciton of CdS. Furthermore, the dynamics of excitons under tensile strain are also investigated; we find that the B-exciton have much shorter lifetime than that of redshifted A-exciton. In addition, we also present the lasing of buckled CdS NRs, in which the strain-dominated mode selection in multi-mode laser and negligible mode shifts in single-mode laser are clearly observed. Our results show that the strained NRs may serve as new functional optical elements for flexible light emitter or on-chip all-optical devices. PMID:27210303

  9. Well separated trion and neutral excitons on superacid treated MoS2 monolayers

    NASA Astrophysics Data System (ADS)

    Cadiz, Fabian; Tricard, Simon; Gay, Maxime; Lagarde, Delphine; Wang, Gang; Robert, Cedric; Renucci, Pierre; Urbaszek, Bernhard; Marie, Xavier

    2016-06-01

    Developments in optoelectronics and spin-optronics based on transition metal dichalcogenide monolayers (MLs) need materials with efficient optical emission and well-defined transition energies. In as-exfoliated MoS2 MLs, the photoluminescence (PL) spectra even at low temperature consist typically of broad, overlapping contributions from neutral, charged excitons (trions) and localized states. Here, we show that in superacid treated MoS2 MLs, the PL intensity increases by up to 60 times at room temperature. The neutral and charged exciton transitions are spectrally well separated in PL and reflectivity at T = 4 K, with linewidth for the neutral exciton of 15 meV, but both transitions have similar intensities compared to the ones in as-exfoliated MLs at the same temperature. Time resolved experiments uncover picoseconds recombination dynamics analyzed separately for charged and neutral exciton emissions. Using the chiral interband selection rules, we demonstrate optically induced valley polarization for both complexes and valley coherence for only the neutral exciton.

  10. Emission energy, exciton dynamics and lasing properties of buckled CdS nanoribbons

    NASA Astrophysics Data System (ADS)

    Wang, Qi; Sun, Liaoxin; Lu, Jian; Ren, Ming-Liang; Zhang, Tianning; Huang, Yan; Zhou, Xiaohao; Sun, Yan; Zhang, Bo; Chen, Changqing; Shen, Xuechu; Agarwal, Ritesh; Lu, Wei

    2016-05-01

    We report the modulation of emission energy, exciton dynamics and lasing properties in a single buckled CdS nanoribbon (NR) by strain-engineering. Inspired by ordered structure fabrication on elastomeric polymer, we develop a new method to fabricate uniform buckled NRs supported on polydimethylsiloxane (PDMS). Wavy structure, of which compressive and tensile strain periodically varied along the CdS NR, leads to a position-dependent emission energy shift as large as 14 nm in photoluminescence (PL) mapping. Both micro-PL and micro-reflectance reveal the spectral characteristics of broad emission of buckled NR, which can be understood by the discrepancy of strain-induced energy shift of A- and B-exciton of CdS. Furthermore, the dynamics of excitons under tensile strain are also investigated; we find that the B-exciton have much shorter lifetime than that of redshifted A-exciton. In addition, we also present the lasing of buckled CdS NRs, in which the strain-dominated mode selection in multi-mode laser and negligible mode shifts in single-mode laser are clearly observed. Our results show that the strained NRs may serve as new functional optical elements for flexible light emitter or on-chip all-optical devices.

  11. Emission energy, exciton dynamics and lasing properties of buckled CdS nanoribbons

    PubMed Central

    Wang, Qi; Sun, Liaoxin; Lu, Jian; Ren, Ming-Liang; Zhang, Tianning; Huang, Yan; Zhou, Xiaohao; Sun, Yan; Zhang, Bo; Chen, Changqing; Shen, Xuechu; Agarwal, Ritesh; Lu, Wei

    2016-01-01

    We report the modulation of emission energy, exciton dynamics and lasing properties in a single buckled CdS nanoribbon (NR) by strain-engineering. Inspired by ordered structure fabrication on elastomeric polymer, we develop a new method to fabricate uniform buckled NRs supported on polydimethylsiloxane (PDMS). Wavy structure, of which compressive and tensile strain periodically varied along the CdS NR, leads to a position-dependent emission energy shift as large as 14 nm in photoluminescence (PL) mapping. Both micro-PL and micro-reflectance reveal the spectral characteristics of broad emission of buckled NR, which can be understood by the discrepancy of strain-induced energy shift of A- and B-exciton of CdS. Furthermore, the dynamics of excitons under tensile strain are also investigated; we find that the B-exciton have much shorter lifetime than that of redshifted A-exciton. In addition, we also present the lasing of buckled CdS NRs, in which the strain-dominated mode selection in multi-mode laser and negligible mode shifts in single-mode laser are clearly observed. Our results show that the strained NRs may serve as new functional optical elements for flexible light emitter or on-chip all-optical devices. PMID:27210303

  12. Atomistic model for excitons: Capturing Strongly Bound Excitons in Monolayer Transition-Metal Dichalcogenides

    NASA Astrophysics Data System (ADS)

    Tseng, Frank; Simsek, Ergun; Gunlycke, Daniel

    2015-03-01

    Monolayer transition-metal dichalcogenides form a direct bandgap predicted in the visible regime making them attractive host materials for various electronic and optoelectronic applications. Due to a weak dielectric screening in these materials, strongly bound electron-hole pairs or excitons have binding energies up to at least several hundred meV's. While the conventional wisdom is to think of excitons as hydrogen-like quasi-particles, we show that the hydrogen model breaks down for these experimentally observed strongly bound, room-temperature excitons. To capture these non-hydrogen-like photo-excitations, we introduce an atomistic model for excitons that predicts both bright excitons and dark excitons, and their broken degeneracy in these two-dimensional materials. For strongly bound exciton states, the lattice potential significantly distorts the envelope wave functions, which affects predicted exciton peak energies. The combination of large binding energies and non-degeneracy of exciton states in monolayer transition metal dichalogendies may furthermore be exploited in room temperature applications where prolonged exciton lifetimes are necessary. This work has been funded by the Office of Naval Research (ONR), directly and through the Naval Research Laboratory (NRL). F.T and E.S acknowledge support from NRL through the NRC Research Associateship Program and ONR Summer Faculty Program, respectively.

  13. Optically pumped ultraviolet and infrared lasers driven by exploding metal films and wires

    SciTech Connect

    Jones, C.R.; Ware, K.D.

    1983-01-01

    The 342-nm molecular iodine and 1315-nm atomic iodine lasers have been optically pumped by intense light from exploding-metal-film and exploding-wire discharges. Brightness temperatures for the exploding-film discharges were approx. 25,000 K and for the wire discharges were approx. 30,000 K. For the I/sub 2/ laser the 3.5-cm-diameter by 40-cm-long pumped volume lies adjacent to the wire or film of the same length. Pressures of 1 to 6 torr I/sub 2/ and 1 to 3 atm SF, CF/sub 4/, or Ar were used in the stainless-steel cell. Using 20-..mu..F capacitance charged to 40 kV, a 0.25-mm tungsten wire, 3-torr I/sub 2/, and a 2-atm SF/sub 6/, an energy of 2 J was obtained from the laser in a pulse of 8-..mu..s duration. The specific output energy was 7 J/l. Substitution of a cylindrical Al film for the wire, under otherwise similar conditions, led to a X10 output energies and efficiencies were obtained with similar input energy. An output pulse of 12 J and 12-..mu..s duration was measured for a specific output energy of 18 J/l. A laser energy of 110 J in a 20-us-long pulse has been measured from atomic iodine using a wire discharge along the axis of a larger cell. The active volume available was 20 cm in diameter and 80 cm in length. Input energy was 32 kJ. In similar measurements using a cylindrical Al film for discharge initiation, the measured output energy was 40 J.

  14. Observations of exciton-surface plasmon polariton coupling and exciton-phonon coupling in InGaN/GaN quantum wells covered with Au, Ag, and Al films

    NASA Astrophysics Data System (ADS)

    Estrin, Y.; Rich, D. H.; Keller, S.; DenBaars, S. P.

    2015-07-01

    The coupling of excitons to surface plasmon polaritons (SPPs) and longitudinal optical (LO) phonons in Au-, Ag-, and Al-coated InxGa1-xN/GaN multiple and single quantum wells (SQWs) was studied with time-resolved cathodoluminescence (CL) and CL wavelength imaging techniques. Excitons were generated in the metal-coated SQWs by injecting a pulsed high-energy electron beam through the thin metal films, which is found to be an ideal method of excitation for plasmonic quantum heterostructures and nanostructures which are opaque to laser/light excitation. The Purcell enhancement factor (Fp) at low temperatures was obtained by the direct measurement of changes in the carrier lifetime caused by the SQW excitonSPP coupling. The deposition of thin films of Al, Ag, and Au on an InGaN/GaN QW enabled a comparison of excitonSPP coupling for energy ranges in which the surface plasmon energy is greater than, approximately equal to, and less than the QW excitonic transition energy. We investigated the temperature dependence of the Huang-Rhys factors for exciton-to-LO phonon coupling for the metal-covered and bare samples. CL imaging and spectroscopy with variable excitation densities are used to examine the spatial correlations between CL emission intensity, carrier lifetime, QW excitonic emission energy, and the Huang-Rhys factor, all of which are strongly influenced by local fluctuations in the In composition and formation of InN-rich centers.

  15. Observations of exciton-surface plasmon polariton coupling and exciton-phonon coupling in InGaN/GaN quantum wells covered with Au, Ag, and Al films.

    PubMed

    Estrin, Y; Rich, D H; Keller, S; DenBaars, S P

    2015-07-01

    The coupling of excitons to surface plasmon polaritons (SPPs) and longitudinal optical (LO) phonons in Au-, Ag-, and Al-coated InxGa1-xN/GaN multiple and single quantum wells (SQWs) was studied with time-resolved cathodoluminescence (CL) and CL wavelength imaging techniques. Excitons were generated in the metal-coated SQWs by injecting a pulsed high-energy electron beam through the thin metal films, which is found to be an ideal method of excitation for plasmonic quantum heterostructures and nanostructures which are opaque to laser/light excitation. The Purcell enhancement factor (Fp) at low temperatures was obtained by the direct measurement of changes in the carrier lifetime caused by the SQW exciton-SPP coupling. The deposition of thin films of Al, Ag, and Au on an InGaN/GaN QW enabled a comparison of exciton-SPP coupling for energy ranges in which the surface plasmon energy is greater than, approximately equal to, and less than the QW excitonic transition energy. We investigated the temperature dependence of the Huang-Rhys factors for exciton-to-LO phonon coupling for the metal-covered and bare samples. CL imaging and spectroscopy with variable excitation densities are used to examine the spatial correlations between CL emission intensity, carrier lifetime, QW excitonic emission energy, and the Huang-Rhys factor, all of which are strongly influenced by local fluctuations in the In composition and formation of InN-rich centers. PMID:26076324

  16. A Survey on Next-Generation Mixed Line Rate (MLR) and Energy-Driven Wavelength-Division Multiplexed (WDM) Optical Networks

    NASA Astrophysics Data System (ADS)

    Iyer, Sridhar

    2015-06-01

    With the ever-increasing traffic demands, infrastructure of the current 10 Gbps optical network needs to be enhanced. Further, since the energy crisis is gaining increasing concerns, new research topics need to be devised and technological solutions for energy conservation need to be investigated. In all-optical mixed line rate (MLR) network, feasibility of a lightpath is determined by the physical layer impairment (PLI) accumulation. Contrary to PLI-aware routing and wavelength assignment (PLIA-RWA) algorithm applicable for a 10 Gbps wavelength-division multiplexed (WDM) network, a new Routing, Wavelength, Modulation format assignment (RWMFA) algorithm is required for the MLR optical network. With the rapid growth of energy consumption in Information and Communication Technologies (ICT), recently, lot of attention is being devoted toward "green" ICT solutions. This article presents a review of different RWMFA (PLIA-RWA) algorithms for MLR networks, and surveys the most relevant research activities aimed at minimizing energy consumption in optical networks. In essence, this article presents a comprehensive and timely survey on a growing field of research, as it covers most aspects of MLR and energy-driven optical networks. Hence, the author aims at providing a comprehensive reference for the growing base of researchers who will work on MLR and energy-driven optical networks in the upcoming years. Finally, the article also identifies several open problems for future research.

  17. Optical emission spectroscopy at the large RF driven negative ion test facility ELISE: Instrumental setup and first results

    SciTech Connect

    Wünderlich, D.; Fantz, U.; Franzen, P.; Riedl, R.; Bonomo, F.

    2013-09-15

    One of the main topics to be investigated at the recently launched large (A{sub source}= 1.0 × 0.9 m{sup 2}) ITER relevant RF driven negative ion test facility ELISE (Extraction from a Large Ion Source Experiment) is the connection between the homogeneity of the plasma parameters close to the extraction system and the homogeneity of the extracted negative hydrogen ion beam. While several diagnostics techniques are available for measuring the beam homogeneity, the plasma parameters are determined by optical emission spectroscopy (OES) solely. First OES measurements close to the extraction system show that without magnetic filter field the vertical profile of the plasma emission is more or less symmetric, with maxima of the emission representing the projection of the plasma generation volumes, and a distinct minimum in between. The profile changes with the strength of the magnetic filter field but under all circumstances the plasma emission in ELISE is much more homogeneous compared to the smaller IPP prototype sources. Planned after this successful demonstration of the ELISE OES system is to combine OES with tomography in order to determine locally resolved values for the plasma parameters.

  18. Optical emission spectroscopy at the large RF driven negative ion test facility ELISE: Instrumental setup and first results

    NASA Astrophysics Data System (ADS)

    Wünderlich, D.; Fantz, U.; Franzen, P.; Riedl, R.; Bonomo, F.

    2013-09-01

    One of the main topics to be investigated at the recently launched large (Asource = 1.0 × 0.9 m2) ITER relevant RF driven negative ion test facility ELISE (Extraction from a Large Ion Source Experiment) is the connection between the homogeneity of the plasma parameters close to the extraction system and the homogeneity of the extracted negative hydrogen ion beam. While several diagnostics techniques are available for measuring the beam homogeneity, the plasma parameters are determined by optical emission spectroscopy (OES) solely. First OES measurements close to the extraction system show that without magnetic filter field the vertical profile of the plasma emission is more or less symmetric, with maxima of the emission representing the projection of the plasma generation volumes, and a distinct minimum in between. The profile changes with the strength of the magnetic filter field but under all circumstances the plasma emission in ELISE is much more homogeneous compared to the smaller IPP prototype sources. Planned after this successful demonstration of the ELISE OES system is to combine OES with tomography in order to determine locally resolved values for the plasma parameters.

  19. Oblique half-solitons and their generation in exciton-polariton condensates

    SciTech Connect

    Flayac, H.; Solnyshkov, D. D.; Malpuech, G.

    2011-05-15

    We describe oblique half-solitons, a new type of topological defects in a two-dimensional spinor Bose-Einstein condensate. A realistic protocol based on the optical spin Hall effect is proposed toward their generation within an exciton-polariton system.

  20. Exciton dynamics in chromophore aggregates with correlated environment fluctuations

    PubMed Central

    Abramavicius, Darius; Mukamel, Shaul

    2011-01-01

    We study the effects of correlated molecular transition energy fluctuations in molecular aggregates on the density matrix dynamics, and their signatures in the optical response. Correlated fluctuations do not affect single-exciton dynamics and can be described as a nonlocal contribution to the spectral broadening, which appears as a multiplicative factor in the time-domain response function. Intraband coherences are damped only by uncorrelated transition energy fluctuations. The signal can then be expressed as a spectral convolution of a local contribution of the uncorrelated fluctuations and the nonlocal contribution of the correlated fluctuations. PMID:21548696

  1. Exciton recombination dynamics in single ZnO tetrapods

    SciTech Connect

    Fernandes-Silva, Lígia C.; Martín, Maria D.; Meulen, Herko P. van der; Calleja, José M.; Viña, Luis; Klopotowski, Lukasz

    2013-12-04

    We present the optical properties of individual ZnO tetrapods as a function of excitation power and temperature by time-integrated and time-resolved spectroscopy. At 10K, we identify the different excitonic transitions by both their characteristic energy and their excitation power dependence. When we increase the tetrapod temperature we observe that the emission intensity decrease and occur a red shift of the emission energies. Our time-resolved studies confirm the predominance of the radiative recombination at low temperatures (< 45 K). Increasing the temperature opens up the non-radiative channels, which are evidenced by a much faster decay time.

  2. Correlated fluctuations in the exciton dynamics and spectroscopy of DNA

    NASA Astrophysics Data System (ADS)

    Dijkstra, Arend G.; Tanimura, Yoshitaka

    2010-05-01

    The absorption of ultraviolet light creates excitations in DNA, which subsequently start moving in the helix. Their fate is important for an understanding of photodamage, and is determined by the interplay of electronic couplings between bases and the structure of the DNA environment. We model the effect of dynamical fluctuations in the environment and study correlation, which is present when multiple base pairs interact with the same mode in the environment. We find that the correlations strongly affect the exciton dynamics, and show how they are observed in the decay of the anisotropy as a function of coherence and population time in a nonlinear optical experiment.

  3. Nonradiative exciton energy transfer in hybrid organic-inorganic heterostructures

    NASA Astrophysics Data System (ADS)

    Chanyawadee, S.; Lagoudakis, P. G.; Harley, R. T.; Lidzey, D. G.; Henini, M.

    2008-05-01

    Nonradiative energy transfer from a GaAs quantum well to a thin overlayer of an infrared organic semiconductor dye is unambiguously demonstrated. The dynamics of exciton transfer are studied in the time domain by using pump-probe spectroscopy at the donor site and fluorescence spectroscopy at the acceptor site. The effect is observed as simultaneous increase in the population decay rate at the donor and of the rise time of optical emission at the acceptor sites. The hybrid configuration under investigation provides an alternative nonradiative, noncontact pumping route to electrical carrier injection that overcomes the losses imposed by the associated low carrier mobility of organic emitters.

  4. Tunable Magnetic Alignment between Trapped Exciton-Polariton Condensates.

    PubMed

    Ohadi, H; Del Valle-Inclan Redondo, Y; Dreismann, A; Rubo, Y G; Pinsker, F; Tsintzos, S I; Hatzopoulos, Z; Savvidis, P G; Baumberg, J J

    2016-03-11

    Tunable spin correlations are found to arise between two neighboring trapped exciton-polariton condensates which spin polarize spontaneously. We observe a crossover from an antiferromagnetic to a ferromagnetic pair state by reducing the coupling barrier in real time using control of the imprinted pattern of pump light. Fast optical switching of both condensates is then achieved by resonantly but weakly triggering only a single condensate. These effects can be explained as the competition between spin bifurcations and spin-preserving Josephson coupling between the two condensates, and open the way to polariton Bose-Hubbard ladders. PMID:27015497

  5. Excitons and Davydov splitting in sexithiophene from first-principles many-body Green’s function theory

    SciTech Connect

    Leng, Xia; Yin, Huabing; Liang, Dongmei; Ma, Yuchen

    2015-09-21

    Organic semiconductors have promising and broad applications in optoelectronics. Understanding their electronic excited states is important to help us control their spectroscopic properties and performance of devices. There have been a large amount of experimental investigations on spectroscopies of organic semiconductors, but theoretical calculation from first principles on this respect is still limited. Here, we use density functional theory (DFT) and many-body Green’s function theory, which includes the GW method and Bethe-Salpeter equation, to study the electronic excited-state properties and spectroscopies of one prototypical organic semiconductor, sexithiophene. The exciton energies of sexithiophene in both the gas and bulk crystalline phases are very sensitive to the exchange-correlation functionals used in DFT for ground-state structure relaxation. We investigated the influence of dynamical screening in the electron-hole interaction on exciton energies, which is found to be very pronounced for triplet excitons and has to be taken into account in first principles calculations. In the sexithiophene single crystal, the energy of the lowest triplet exciton is close to half the energy of the lowest singlet one. While lower-energy singlet and triplet excitons are intramolecular Frenkel excitons, higher-energy excitons are of intermolecular charge-transfer type. The calculated optical absorption spectra and Davydov splitting are in good agreement with experiments.

  6. Effect of heteroboundary spreading on the properties of exciton states in Zn(Cd)Se/ZnMgSSe quantum wells

    SciTech Connect

    Adiyatullin, A. F. Belykh, V. V.; Kozlovsky, V. I.; Krivobok, V. S. Martovitsky, V. P.; Nikolaev, S. N.

    2012-11-15

    Exciton states in Zn(Cd)Se/ZnMgSSe quantum wells with different diffusion spreading of interfaces are studied by optical spectroscopy methods. It is shown that the emission spectrum of quantum wells at low temperatures is determined by free excitons and bound excitons on neutral donors. The nonlinear dependence of the stationary photoluminescence intensity on the excitation power density and the biexponential luminescence decay are explained by the neutralization of charged defects upon photoexcitation of heterostructures. With the stationary illumination on, durable (about 40 min) reversible changes in the reflection coefficient near the exciton resonances of quantum wells are observed. It is shown that, along with the shift of exciton levels, the spreading of heteroboundaries leads to three effects: an increase in the excitonphonon interaction, an increase in the energy shift between the emission lines of free and bound excitons, and a decrease in the decay time of exciton luminescence in a broad temperature range. The main reasons for these effects are discussed.

  7. Real-time verification of multileaf collimator-driven radiotherapy using a novel optical attenuation-based fluence monitor

    SciTech Connect

    Goulet, Mathieu; Gingras, Luc; Beaulieu, Luc

    2011-03-15

    Purpose: Multileaf collimator (MLC)-driven conformal radiotherapy modalities [e.g., such as intensity-modulated radiotherapy (IMRT), intensity-modulated arc therapy, and stereotactic body radiotherapy] are more subject to delivery errors and dose calculation inaccuracies than standard modalities. Fluence monitoring during treatment delivery could reduce such errors by allowing an independent interface to quantify and assess measured difference between the delivered and planned treatment administration. We developed an optical attenuation-based detector to monitor fluence for the on-line quality control of radiotherapy delivery. The purpose of the current study was to develop the theoretical background of the invention and to evaluate the detector's performance both statistically and in clinical situations. Methods: We aligned 60 27-cm scintillating fibers coupled to a photodetector via clear optical fibers in the direction of motion of each of the 60 leaf pairs of a 120 leaves Millenium MLC on a Varian Clinac iX. We developed a theoretical model to predict the intensity of light collected on each side of the scintillating fibers when placed under radiation fields of varying sizes, intensities, and positions. The model showed that both the central position of the radiation field on the fiber (x{sub c}) and the integral fluence passing through the fiber ({Phi}{sub int}) could be assessed independently in a single measurement. We evaluated the performance of the prototype by (1) measuring the intrinsic variation of the measured values of x{sub c} and {Phi}{sub int}, (2) measuring the impact on the measured values of x{sub c} and {Phi}{sub int} of random leaf positioning errors introduced into IMRT fields, and (3) comparing the predicted values of x{sub c} and {Phi}{sub int} calculated with the treatment planning software to the measured values of x{sub c} and {Phi}{sub int} in order to assess the predictive effectiveness of the developed theoretical model. Results: We

  8. Orbital diamagnetic susceptibility in excitonic condensation phase

    NASA Astrophysics Data System (ADS)

    Sugimoto, Koudai; Ohta, Yukinori

    2016-08-01

    We study the orbital diamagnetic susceptibility in excitonic condensation phase using the mean-field approximation for a two-band model defined on a square lattice. We find that, in semiconductors, the excitonic condensation acquires a finite diamagnetic susceptibility due to spontaneous hybridization between the valence and the conduction bands, whereas in semimetals, the diamagnetic susceptibility in the normal phase is suppressed by the excitonic condensation. We also study the orbital diamagnetic and Pauli paramagnetic susceptibilities of Ta2NiSe5 using a two-dimensional three-band model and find that the calculated temperature dependence of the magnetic susceptibility is in qualitative agreement with experiment.

  9. Exciton effects in strained armchair graphene nanoribbons

    NASA Astrophysics Data System (ADS)

    Jia, Yonglei; Liu, Junlin

    2016-01-01

    The exciton effects in 1-nm-wide armchair graphene nanoribbons (AGNRs) under the uniaxial strain were studied within the nonorthogonal tight-binding (TB) model, supplemented by the long-range Coulomb interactions. The obtained results show that both the excitation energy and exciton binding energy are modulated by the uniaxial strain. The variation of these energies depends on the ribbon family. In addition, the results show that the variation of the exciton binding energy is much weaker than the variation of excitation energy. Our results provide new guidance for the design of optomechanical systems based on graphene nanoribbons.

  10. Exciton Regeneration at Polymeric Semiconductor Heterojunctions

    NASA Astrophysics Data System (ADS)

    Morteani, Arne C.; Sreearunothai, Paiboon; Herz, Laura M.; Friend, Richard H.; Silva, Carlos

    2004-06-01

    Control of the band-edge offsets at heterojunctions between organic semiconductors allows efficient operation of either photovoltaic or light-emitting diodes. We investigate systems where the exciton is marginally stable against charge separation and show via E-field-dependent time-resolved photoluminescence spectroscopy that excitons that have undergone charge separation at a heterojunction can be efficiently regenerated. This is because the charge transfer produces a geminate electron-hole pair (separation 2.2 3.1nm) which may collapse into an exciplex and then endothermically (EA=100 200 meV) back transfer towards the exciton.

  11. Multiple Exciton Generation Solar Cells

    SciTech Connect

    Luther, J. M.; Semonin, O. E.; Beard, M. C.; Gao, J.; Nozik, A. J.

    2012-01-01

    Heat loss is the major factor limiting traditional single junction solar cells to a theoretical efficiency of 32%. Multiple Exciton Generation (MEG) enables efficient use of the solar spectrum yielding a theoretical power conversion efficiency of 44% in solar cells under 1-sun conditions. Quantum-confined semiconductors have demonstrated the ability to generate multiple carriers but present-day materials deliver efficiencies far below the SQ limit of 32%. Semiconductor quantum dots of PbSe and PbS provide an active testbed for developing high-efficiency, inexpensive solar cells benefitting from quantum confinement effects. Here, we will present recent work of solar cells employing MEG to yield external quantum efficiencies exceeding 100%.

  12. Singlet exciton fission in solution

    NASA Astrophysics Data System (ADS)

    Walker, Brian J.; Musser, Andrew J.; Beljonne, David; Friend, Richard H.

    2013-12-01

    Singlet exciton fission, the spin-conserving process that produces two triplet excited states from one photoexcited singlet state, is a means to circumvent the Shockley-Queisser limit in single-junction solar cells. Although the process through which singlet fission occurs is not well characterized, some local order is thought to be necessary for intermolecular coupling. Here, we report a triplet yield of 200% and triplet formation rates approaching the diffusion limit in solutions of bis(triisopropylsilylethynyl (TIPS)) pentacene. We observe a transient bound excimer intermediate, formed by the collision of one photoexcited and one ground-state TIPS-pentacene molecule. The intermediate breaks up when the two triplets separate to each TIPS-pentacene molecule. This efficient system is a model for future singlet-fission materials and for disordered device components that produce cascades of excited states from sunlight.

  13. Singlet exciton fission in solution.

    PubMed

    Walker, Brian J; Musser, Andrew J; Beljonne, David; Friend, Richard H

    2013-12-01

    Singlet exciton fission, the spin-conserving process that produces two triplet excited states from one photoexcited singlet state, is a means to circumvent the Shockley-Queisser limit in single-junction solar cells. Although the process through which singlet fission occurs is not well characterized, some local order is thought to be necessary for intermolecular coupling. Here, we report a triplet yield of 200% and triplet formation rates approaching the diffusion limit in solutions of bis(triisopropylsilylethynyl (TIPS)) pentacene. We observe a transient bound excimer intermediate, formed by the collision of one photoexcited and one ground-state TIPS-pentacene molecule. The intermediate breaks up when the two triplets separate to each TIPS-pentacene molecule. This efficient system is a model for future singlet-fission materials and for disordered device components that produce cascades of excited states from sunlight. PMID:24256865

  14. Emission spectrum of a dressed exciton-biexciton complex in a semiconductor quantum dot.

    PubMed

    Muller, Andreas; Fang, Wei; Lawall, John; Solomon, Glenn S

    2008-07-11

    The photoluminescence spectrum of a single quantum dot was recorded as a secondary resonant laser optically dressed either the vacuum-to-exciton or the exciton-to-biexciton transitions. High-resolution polarization-resolved measurements using a scanning Fabry-Pérot interferometer reveal splittings of the linearly polarized fine-structure states that are nondegenerate in an asymmetric quantum dot. These splittings manifest as either triplets or doublets and depend sensitively on laser intensity and detuning. Our approach realizes complete resonant control of a multiexcitonic system in emission, which can be either pulsed or continuous wave, and offers direct access to the emitted photons. PMID:18764226

  15. Excitons in solids with time-dependent density-functional theory: the bootstrap kernel and beyond

    NASA Astrophysics Data System (ADS)

    Byun, Young-Moo; Yang, Zeng-Hui; Ullrich, Carsten

    Time-dependent density-functional theory (TDDFT) is an efficient method to describe the optical properties of solids. Lately, a series of bootstrap-type exchange-correlation (xc) kernels have been reported to produce accurate excitons in solids, but different bootstrap-type kernels exist in the literature, with mixed results. In this presentation, we reveal the origin of the confusion and show a new empirical TDDFT xc kernel to compute excitonic properties of semiconductors and insulators efficiently and accurately. Our method can be used for high-throughput screening calculations and large unit cell calculations. Work supported by NSF Grant DMR-1408904.

  16. Observation of an Excitonic Quantum Coherence in CdSe Nanocrystals.

    PubMed

    Dong, Shuo; Trivedi, Dhara; Chakrabortty, Sabyasachi; Kobayashi, Takayoshi; Chan, Yinthai; Prezhdo, Oleg V; Loh, Zhi-Heng

    2015-10-14

    Recent observations of excitonic coherences within photosynthetic complexes suggest that quantum coherences could enhance biological light harvesting efficiencies. Here, we employ optical pump-probe spectroscopy with few-femtosecond pulses to observe an excitonic quantum coherence in CdSe nanocrystals, a prototypical artificial light harvesting system. This coherence, which encodes the high-speed migration of charge over nanometer length scales, is also found to markedly alter the displacement amplitudes of phonons, signaling dynamics in the non-Born-Oppenheimer regime. PMID:26359970

  17. Center-of-mass and internal motion of excitons in quantum wires

    NASA Astrophysics Data System (ADS)

    Glutsch, S.; Bechstedt, F.

    The properties of excitons, which are optically excited in single or coupled quantum wires, are studied within the effective-mass approximation. The two-particle wave functions and energies obey a Schrödinger equation with screened Coulomb interaction of electron and hole and their corresponding wire confinement potentials. This equation is approximately separated into an equation for the center-of-mass motion and another one more or less for the internal motion of the electron hole pairs. This allows a representation of absorption and luminescence spectra near a quantum-well exciton transition by a generalized Elliott formula.

  18. Type II InAs/GaAsSb quantum dots: Highly tunable exciton geometry and topology

    SciTech Connect

    Llorens, J. M.; Wewior, L.; Cardozo de Oliveira, E. R.; Alén, B.; Ulloa, J. M.; Utrilla, A. D.; Guzmán, A.; Hierro, A.

    2015-11-02

    External control over the electron and hole wavefunctions geometry and topology is investigated in a p-i-n diode embedding a dot-in-a-well InAs/GaAsSb quantum structure with type II band alignment. We find highly tunable exciton dipole moments and largely decoupled exciton recombination and ionization dynamics. We also predicted a bias regime where the hole wavefunction topology changes continuously from quantum dot-like to quantum ring-like as a function of the external bias. All these properties have great potential in advanced electro-optical applications and in the investigation of fundamental spin-orbit phenomena.

  19. Plasmonic-exciton coupling in synthesized metal/semiconductor hybrid nanocomposites

    SciTech Connect

    Gadalla, A.; Hamad, D. A.; Mohamed, M. B.

    2015-12-31

    A new method has been developed to grow plasmonic semiconductor nanocomposites of Au/CdSe and Ag/CdSe. Their chemical composition and crystal structure are determined by X-ray diffraction. The collective optical properties of the prepared semiconductor nanohybrid have been measured using spectrophotometer techniques and compared to those of the individual components. The electron transfer processes from CdSe to the gold are faster than that of the silver. Au/CdSe has a strong plasmonic-excitonic coupling, but Ag/CdSe has a weak plasmonic-excitonic coupling.

  20. Femtosecond spectroscopy on MoS2 flakes from liquid exfoliation: surfactant independent exciton dynamics

    NASA Astrophysics Data System (ADS)

    Vella, Daniele; Vega-Mayoral, Victor; Gadermaier, Christoph; Vujicic, Natasa; Borzda, Tetiana; Topolovsek, Peter; Prijatelj, Matej; Tempra, Iacopo; Pogna, Eva A. A.; Cerullo, Giulio

    2016-03-01

    Ionic surfactants, which are widely used to stabilize nanomaterials in dispersions, can drastically alter the nanomaterial's photophysical properties. Here, we use femtosecond optical spectroscopy to study the dynamics of excitons and charges in few-layer flakes of the two-dimensional semiconductor MoS2. We compare samples obtained via exfoliation in water with different amounts of adsorbed sodium cholate, obtained by repeated washing of the dried flakes. We find that the femtosecond dynamics is remarkably stable against the surfactant adsorption, with a slight increase of the initial exciton quenching occurring during the first few picoseconds as the only appreciable effect.