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Sample records for bound exciton luminescence

  1. Luminescence of impurity-bound excitons in Li6GdB3O9:Ce3+ single crystals.

    PubMed

    Ogorodnikov, Igor N; Pustovarov, Vladimir A

    2012-10-10

    The anomalous (τ < 10 ns) luminescence of wide bandgap crystals of lithium-gadolinium orthoborate Li(6)GdB(3)O(9) doped with trivalent cerium ions, has been revealed for the first time and investigated through the low-temperature time-resolved vacuum ultraviolet synchrotron spectroscopy. It was shown that the optical transitions at 6.2 eV are due to electron transfer from the ground 4f(1) states of Ce(3+) ion onto the autoionized states near the conduction band bottom of a crystal. These transitions lead to the formation of impurity-bound excitons in the form of correlated electron-hole pair, in which the hole component is localized at 4f-level of the cerium ion and an electron component is located at the conduction band bottom in the attractive potential of this hole. It is established that the direct radiative recombination of the cerium impurity-bound exciton leads to a fast broadband emission at 4.25 eV. The energy threshold for creation of the impurity-bound excitons was determined on the basis of the obtained spectroscopic data. We calculated the H(k) functions of distribution of the elementary relaxations over the reaction rate constants and explained on this basis the decay kinetics and quenching processes, not only for the anomalous emission at 4.25 eV, but for the ordinary 5d-4f luminescence at 3.0 eV in Ce(3+) ions. The paper discusses the decay channels for the impurity-bound excitons and their influence on the decay kinetics and spectra of luminescence in Li(6)GdB(3)O(9) crystals.

  2. Luminescence dynamics of bound exciton of hydrogen doped ZnO nanowires

    DOE PAGES

    Yoo, Jinkyoung; Yi, Gyu -Chul; Chon, Bonghwan; ...

    2016-04-11

    In this study, all-optical camera, converting X-rays into visible photons, is a promising strategy for high-performance X-ray imaging detector requiring high detection efficiency and ultrafast detector response time. Zinc oxide is a suitable material for all-optical camera due to its fast radiative recombination lifetime in sub-nanosecond regime and its radiation hardness. ZnO nanostructures have been considered as proper building blocks for ultrafast detectors with spatial resolution in sub-micrometer scale. To achieve remarkable enhancement of luminescence efficiency n-type doping in ZnO has been employed. However, luminescence dynamics of doped ZnO nanostructures have not been thoroughly investigated whereas undoped ZnO nanostructures havemore » been employed to study their luminescence dynamics. Here we report a study of luminescence dynamics of hydrogen doped ZnO nanowires obtained by hydrogen plasma treatment. Hydrogen doping in ZnO nanowires gives rise to significant increase in the near-band-edge emission of ZnO and decrease in averaged photoluminescence lifetime from 300 to 140 ps at 10 K. The effects of hydrogen doping on the luminescent characteristics of ZnO nanowires were changed by hydrogen doping process variables.« less

  3. Luminescence dynamics of bound exciton of hydrogen doped ZnO nanowires

    SciTech Connect

    Yoo, Jinkyoung; Yi, Gyu -Chul; Chon, Bonghwan; Joo, Taiha; Wang, Zhehui

    2016-04-11

    In this study, all-optical camera, converting X-rays into visible photons, is a promising strategy for high-performance X-ray imaging detector requiring high detection efficiency and ultrafast detector response time. Zinc oxide is a suitable material for all-optical camera due to its fast radiative recombination lifetime in sub-nanosecond regime and its radiation hardness. ZnO nanostructures have been considered as proper building blocks for ultrafast detectors with spatial resolution in sub-micrometer scale. To achieve remarkable enhancement of luminescence efficiency n-type doping in ZnO has been employed. However, luminescence dynamics of doped ZnO nanostructures have not been thoroughly investigated whereas undoped ZnO nanostructures have been employed to study their luminescence dynamics. Here we report a study of luminescence dynamics of hydrogen doped ZnO nanowires obtained by hydrogen plasma treatment. Hydrogen doping in ZnO nanowires gives rise to significant increase in the near-band-edge emission of ZnO and decrease in averaged photoluminescence lifetime from 300 to 140 ps at 10 K. The effects of hydrogen doping on the luminescent characteristics of ZnO nanowires were changed by hydrogen doping process variables.

  4. Hyperfine structure and nuclear hyperpolarization observed in the bound exciton luminescence of Bi donors in natural Si.

    PubMed

    Sekiguchi, T; Steger, M; Saeedi, K; Thewalt, M L W; Riemann, H; Abrosimov, N V; Nötzel, N

    2010-04-02

    As the deepest group-V donor in Si, Bi has by far the largest hyperfine interaction and also a large I = 9/2 nuclear spin. At zero field this splits the donor ground state into states having total spin 5 and 4, which are fully resolved in the photoluminescence spectrum of Bi donor bound excitons. Under a magnetic field, the 60 expected allowed transitions cannot be individually resolved, but the effects of the nuclear spin distribution, -9/2 < or = I(z) < or = 9/2, are clearly observed. A strong hyperpolarization of the nuclear spin towards I(z) = -9/2 is observed to result from the nonresonant optical excitation. This is very similar to the recently reported optical hyperpolarization of P donors observed by EPR at higher magnetic fields. We introduce a new model to explain this effect, and predict that it may be very fast.

  5. Influence of lattice vibrations on luminescence and transfer of excitons in WS2 monolayer semiconductors

    NASA Astrophysics Data System (ADS)

    Wang, X. H.; Su, Z. C.; Ning, J. Q.; Wang, M. Z.; Xu, S. J.; Han, S.; Jia, F.; Zhu, D. L.; Lu, Y. M.

    2016-11-01

    Monolayers of transition metal dichalcogenides (TMDs) have been recently demonstrated to be a new family of direct bandgap semiconductors exhibiting extraordinary excitonic effects and high-efficiency luminescence. Here we present a micro-photoluminescence (PL) study on temperature dependent luminescence of excitons from an exfoliated WS2 monolayer. It is found that lattice vibrations (i.e. phonons) have a profound influence on the excitonic luminescence of the WS2 monolayer in several aspects including the spectral peak shift, lineshape broadening, transfer, and even formation entropy of excitons. Our study not only leads to the determination of the fundamental excitonic bandgap: {{E}\\text{g}}=2.061~ eV at T=0 \\text{K} , but also reveals that 120 K is a ‘turning’ temperature for the competition and formation entropy of free excitons and defect-bound excitons in the studied 2D WS2 crystals.

  6. The effect of magnetic field on free and bound exciton luminescence in GaAs/AlGaAs multiple quantum well structures: a quantitative study on the estimation of ultra-low disorder

    NASA Astrophysics Data System (ADS)

    Haldar, S.; Dixit, V. K.; Vashisht, Geetanjali; Porwal, S.; Sharma, T. K.

    2017-08-01

    The influence of ultra-low defects and atomic irregularities at the hetero-junction on the optical properties of free and bound excitons are investigated by the magneto photoluminescence (PL) spectroscopy. Magneto PL spectra of GaAs/AlGaAs multiple quantum wells (MQWs) are recorded in Faraday and Voigt configuration to understand the kinetics of excitons under the different extents of quantum confinement. Magnetic field induced suppression of the asymmetry in the PL line-shape is identified as the reduced effect of disorder due to the in-plane confinement of exciton. Such effects are distinctly observed in Faraday configuration compared to the Voigt configuration. It is due to the strong magnetic field dependent dimensionality confinement of the excitons, which is illustrated by comparing the diamagnetic/Landau energy for the two configurations via experimental and theoretical results. A simple model, based on the suppression of bound exciton PL with the magnetic field, is proposed to estimate the density of disorder in the GaAs/AlGaAs MQW system, which is found to be  ∼2×1015 cm-3 for the QWs. Additionally, the magnetic field driven re-distribution of charge carrier at the Landau levels and its effect on the free exciton luminescence is investigated. Thus, the magneto-PL spectroscopy in this study is found to be an excellent tool for the quantitative estimation of ultra-low disorder and QW parameters governing the optical properties of excitons, which shall be highly useful in the development of advanced optoelectronic devices.

  7. Influence of excitonic effects on luminescence quantum yield in silicon

    NASA Astrophysics Data System (ADS)

    Sachenko, A. V.; Kostylyov, V. P.; Vlasiuk, V. M.; Sokolovskyi, I. O.; Evstigneev, M.

    2017-03-01

    Nonradiative exciton lifetime in silicon is determined by comparison of the experimental and theoretical curves of bulk minority charge carriers lifetime on doping and excitation levels. This value is used to analyze the influence of excitonic effects on internal luminescence quantum yield at room temperature, taking into account both nonradiative and radiative exciton lifetimes. A range of Shockley-Hall-Reed lifetimes is found, where excitonic effects lead to an increase of internal luminescence quantum yield.

  8. Exciton luminescence from Cu2SnS3 bulk crystals

    NASA Astrophysics Data System (ADS)

    Aihara, Naoya; Matsumoto, Yusuke; Tanaka, Kunihiko

    2016-02-01

    The optical properties of Cu2SnS3 (CTS) bulk crystals grown by chemical vapor transport were studied by photoluminescence (PL) spectroscopy. The PL spectra from the CTS bulk crystals were analyzed as a function of excitation power and temperature. The main phase of the as-grown samples was determined to be monoclinic CTS by Raman spectroscopy. The observed PL spectra from the CTS bulk crystals were composed of peaks corresponding to free-exciton, two bound-excitons, and donor-acceptor pair recombination luminescence. The peak energies for the free-exciton and two bound-exciton emissions were 0.9317, 0.9291, and 0.9260 eV, respectively, at temperature of 4.2 K. The bound-exciton luminescence was not observed above 30 K. The thermal activation energies for the free-exciton and two bound-exciton emissions were 6.5, 4.8, and 5.2 meV, respectively. The fundamental band gap in the CTS bulk crystals was expected to be ca. 0.94 eV.

  9. Excitonic luminescence of SiGe/Si quantum wells δ-doped with boron

    SciTech Connect

    Bagaev, V. S.; Nikolaev, S. N.; Onishchenko, E. E.; Pruchkina, A. A.; Krivobok, V. S.; Novikov, A. V.

    2015-05-14

    Low-temperature photoluminescence of undoped and moderately δ-doped Si{sub 1−x}Ge{sub x}/Si (x < 0.1) quantum wells has been studied. The influence of boron δ-layer on the excitonic luminescence and the luminescence caused by a dense electron plasma was demonstrated. The conditions under which the luminescence spectra of quantum wells are dominated by impurity-bound excitons (BE) have been established. Some unusual properties of these BE are explained in terms of type II band-offset in Si{sub 1−x}Ge{sub x}/Si (x < 0.1) quantum wells, which favors a spatial separation of electrons and holes. It is shown that the temperature dependence of an excitonic emission in the quantum wells allows to calculate the BE-related density of states and, thus, can be used for contactless estimation of the impurity concentration in quantum wells.

  10. Bound exciton and free exciton states in GaSe thin slab

    PubMed Central

    Wei, Chengrong; Chen, Xi; Li, Dian; Su, Huimin; He, Hongtao; Dai, Jun-Feng

    2016-01-01

    The photoluminescence (PL) and absorption experiments have been performed in GaSe slab with incident light polarized perpendicular to c-axis of sample at 10 K. An obvious energy difference of about 34 meV between exciton absorption peak and PL peak (the highest energy peak) is observed. By studying the temperature dependence of PL and absorption spectra, we attribute it to energy difference between free exciton and bound exciton states, where main exciton absorption peak comes from free exciton absorption, and PL peak is attributed to recombination of bound exciton at 10 K. This strong bound exciton effect is stable up to 50 K. Moreover, the temperature dependence of integrated PL intensity and PL lifetime reveals that a non-radiative process, with activation energy extracted as 0.5 meV, dominates PL emission. PMID:27654064

  11. Bound exciton and free exciton states in GaSe thin slab

    NASA Astrophysics Data System (ADS)

    Wei, Chengrong; Chen, Xi; Li, Dian; Su, Huimin; He, Hongtao; Dai, Jun-Feng

    2016-09-01

    The photoluminescence (PL) and absorption experiments have been performed in GaSe slab with incident light polarized perpendicular to c-axis of sample at 10 K. An obvious energy difference of about 34 meV between exciton absorption peak and PL peak (the highest energy peak) is observed. By studying the temperature dependence of PL and absorption spectra, we attribute it to energy difference between free exciton and bound exciton states, where main exciton absorption peak comes from free exciton absorption, and PL peak is attributed to recombination of bound exciton at 10 K. This strong bound exciton effect is stable up to 50 K. Moreover, the temperature dependence of integrated PL intensity and PL lifetime reveals that a non-radiative process, with activation energy extracted as 0.5 meV, dominates PL emission.

  12. Excitonic luminescence upconversion in a two-dimensional semiconductor

    SciTech Connect

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

    2015-12-21

    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. Furthermore, this phenomenon lies at the heart of optical refrigeration in solids(1), where upconversion relies on anti-Stokes processes enabled either by rare-earth impurities(2) or exciton-phonon coupling(3). 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(4). Since the charged exciton binding energy(5) closely matches the 31 meV A(1)' optical phonon(6-9), 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. Additionally, 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.

  13. Excitonic luminescence upconversion in a two-dimensional semiconductor

    DOE PAGES

    Jones, Aaron M.; Yu, Hongyi; Schaibley, John R.; ...

    2015-12-21

    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. Furthermore, this phenomenon lies at the heart of optical refrigeration in solids(1), where upconversion relies on anti-Stokes processes enabled either by rare-earth impurities(2) or exciton-phonon coupling(3). 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(4). Since the charged exciton binding energy(5) closelymore » matches the 31 meV A(1)' optical phonon(6-9), 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. Additionally, 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.« less

  14. Exciton binding energies and luminescence of phosphorene under pressure

    NASA Astrophysics Data System (ADS)

    Seixas, L.; Rodin, A. S.; Carvalho, A.; Castro Neto, A. H.

    2015-03-01

    The optical response of phosphorene can be gradually changed by application of moderate uniaxial compression, as the material undergoes the transition into an indirect gap semiconductor and eventually into a semimetal. Strain tunes not only the gap between the valence band and conduction band local extrema but also the effective masses, and in consequence, the exciton anisotropy and binding strength. In this article, we consider from a theoretical point of view how the exciton stability and the resulting luminescence energy evolves under uniaxial strain. We find that the exciton binding energy can be as large as 0.87 eV in vacuum for 5% transverse strain, placing it amongst the highest for two-dimensional materials. Further, the large shift of the luminescence peak and its linear dependence on strain suggest that it can be used to probe directly the strain state of single layers.

  15. 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

  16. 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.

  17. Phonon-Induced Dephasing of Excitons in Semiconductor Quantum Dots: Multiple Exciton Generation, Fission, and Luminescence

    NASA Astrophysics Data System (ADS)

    Madrid, Angeline; Kim, Hyeon-Deuk; Habenicht, Bradley; Prezhdo, Oleg

    2010-03-01

    Phonon-induced dephasing processes that govern optical line widths, multiple exciton (ME) generation (MEG), and ME fission (MEF) in semiconductor quantum dots (QDs) are investigated by ab initio molecular dynamics simulation. Using Si QDs as an example, we propose that MEF occurs by phonon-induced dephasing and, for the first time, estimate its time scale to be 100 fs. In contrast, luminescence and MEG dephasing times are all sub-10 fs. Generally, dephasing is faster for higher-energy and higher-order excitons and increased temperatures. MEF is slow because it is facilitated only by low-frequency acoustic modes. Luminescence and MEG couple to both acoustic and optical modes of the QD, as well as ligand vibrations. The detailed atomistic simulation of the dephasing processes advances understanding of exciton dynamics in QDs and other nanoscale materials.

  18. Radiative properties of multicarrier bound excitons in GaAs

    NASA Astrophysics Data System (ADS)

    Karin, Todd; Barbour, Russell J.; Santori, Charles; Yamamoto, Yoshihisa; Hirayama, Yoshiro; Fu, Kai-Mei C.

    2015-04-01

    Excitons in semiconductors can have multiple lifetimes due to spin-dependent oscillator strengths and interference between different recombination pathways. In addition, strain and symmetry effects can further modify lifetimes via the removal of degeneracies. We present a convenient formalism for predicting the optical properties of k =0 excitons with an arbitrary number of charge carriers in different symmetry environments. Using this formalism, we predict three distinct lifetimes for the neutral acceptor bound exciton in GaAs, and confirm this prediction through polarization dependent and time-resolved photoluminescence experiments. We find the acceptor bound-exciton lifetimes to be To×(1 ,3 ,3/4 ) , where To=(0.61 ±0.12 ) ns . Furthermore, we provide an estimate of the intralevel and interlevel exciton spin-relaxation rates.

  19. Highly luminescent two dimensional excitons in atomically thin CdSe nanosheets

    NASA Astrophysics Data System (ADS)

    Halder, O.; Pradhani, A.; Sahoo, P. K.; Satpati, B.; Rath, S.

    2014-05-01

    Atomically thin Cadmium Selenide (CdSe) nanosheets have been synthesized using a surfactant mediated growth technique. The transmission electron microscopy studies confirm the presence of single layered nanosheets with thickness 1.31 nm and their stacking structures which are complemented by the small angle x-ray scattering measurements. The strongly bound and polarized character of two dimensional excitonic states with enhanced oscillator strength yielding distinct narrow blue luminescence has been observed from the CdSe nanosheets using room temperature based optical studies.

  20. Highly luminescent two dimensional excitons in atomically thin CdSe nanosheets

    SciTech Connect

    Halder, O.; Pradhani, A.; Rath, S.; Sahoo, P. K.; Satpati, B.

    2014-05-05

    Atomically thin Cadmium Selenide (CdSe) nanosheets have been synthesized using a surfactant mediated growth technique. The transmission electron microscopy studies confirm the presence of single layered nanosheets with thickness 1.31 nm and their stacking structures which are complemented by the small angle x-ray scattering measurements. The strongly bound and polarized character of two dimensional excitonic states with enhanced oscillator strength yielding distinct narrow blue luminescence has been observed from the CdSe nanosheets using room temperature based optical studies.

  1. Photoluminescence of isotopically purified silicon: how sharp are bound exciton transitions?

    PubMed

    Karaiskaj, D; Thewalt, M L; Ruf, T; Cardona, M; Pohl, H J; Deviatych, G G; Sennikov, P G; Riemann, H

    2001-06-25

    We report the first high resolution photoluminescence studies of isotopically pure Si (99.896% (28)Si). New information is obtained on isotopic effects on the indirect band gap energy, phonon energies, and phonon broadenings, which is in good agreement with calculations and previous results obtained in Ge and diamond. Remarkably, the linewidths of the no-phonon boron and phosphorus bound exciton transitions in the (28)Si sample are much narrower than in natural Si and are not well resolved at our maximum instrumental resolution of approximately 0.014 cm(-1). The removal of the dominant broadening resulting from isotopic randomness in natural Si reveals new fine structure in the boron bound exciton luminescence.

  2. Nature of excitons bound to inversion domain boundaries: Origin of the 3.45-eV luminescence lines in spontaneously formed GaN nanowires on Si(111)

    NASA Astrophysics Data System (ADS)

    Pfüller, Carsten; Corfdir, Pierre; Hauswald, Christian; Flissikowski, Timur; Kong, Xiang; Zettler, Johannes K.; Fernández-Garrido, Sergio; Doǧan, Pınar; Grahn, Holger T.; Trampert, Achim; Geelhaar, Lutz; Brandt, Oliver

    2016-10-01

    We investigate the 3.45-eV luminescence band of spontaneously formed GaN nanowires on Si(111) by photoluminescence and cathodoluminescence spectroscopy. This band is found to be particularly prominent for samples synthesized at comparatively low temperatures. At the same time, these samples exhibit a peculiar morphology, namely, isolated long nanowires are interspersed within a dense matrix of short ones. Cathodoluminescence intensity maps reveal the 3.45-eV band to originate primarily from the long nanowires. Transmission electron microscopy shows that these long nanowires are either Ga polar and are joined by an inversion domain boundary with their short N-polar neighbors, or exhibit a Ga-polar core surrounded by a N-polar shell with a tubular inversion domain boundary at the core/shell interface. For samples grown at high temperatures, which exhibit a uniform nanowire morphology, the 3.45-eV band is also found to originate from particular nanowires in the ensemble and thus presumably from inversion domain boundaries stemming from the coexistence of N- and Ga-polar nanowires. For several of the investigated samples, the 3.45-eV band splits into a doublet. We demonstrate that the higher-energy component of this doublet arises from the recombination of two-dimensional excitons free to move in the plane of the inversion domain boundary. In contrast, the lower-energy component of the doublet originates from excitons localized in the plane of the inversion domain boundary. We propose that this in-plane localization is due to shallow donors in the vicinity of the inversion domain boundaries.

  3. 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.

  4. Strongly Enhanced Free-Exciton Luminescence in Microcrystalline CsPbBr3 Films

    NASA Astrophysics Data System (ADS)

    Kondo, Shin-ichi; Kakuchi, Mitsugu; Masaki, Atsushi; Saito, Tadaaki

    2003-07-01

    The luminescence properties of CsPbBr3 films prepared via the amorphous phase by crystallization are dominated by free-exciton emission, and only a weak trace of emission due to trapped excitons was observed, in contrast to the case of bulk CsPbBr3 crystals. In particular, the films in the microcrystalline state show by more than an order of magnitude stronger free-exciton emission than in the polycrystalline state. The enhanced free-exciton emission is suggestive of excitonic superradiance.

  5. Spectroscopy of resonant excitation of exciton luminescence of GaSe-GaTe solid solutions

    NASA Astrophysics Data System (ADS)

    Starukhin, A. N.; Nelson, D. K.; Fedorov, D. L.; Syunyaev, D. K.

    2017-02-01

    The luminescence excitation spectra of localized excitons in GaSe0.85Te0.15 solid solutions have been investigated at the temperature T = 2 K. It has been shown that the excitation spectra of excitons with the localization energy ɛ > 10 mV exhibit an additional maximum M E located on the low-energy side of the maximum corresponding to the free exciton absorption band with n = 1. It has been found that the shift in the position of the maximum M E in the excitation spectrum with respect to the energy of detected photons increases as the energy of detected photons decreases, i.e., with an increase in the localization energy of excitons. Under the resonant excitation of localized excitons by a monochromatic light from the region of the exciton emission band, in the exciton luminescence spectrum on the low-energy side from the excitation line, there is also a maximum of the luminescence ( M L ). The energy distance between the position of the excitation line and the position of the maximum in the luminescence spectrum increases with a decrease in the frequency of the excitation light. The possible mechanisms of the formation of the described structure of the luminescence excitation and exciton luminescence spectra of GaSe0.85Te0.15 have been considered. It has been concluded that the maximum M E in the excitation spectrum and the maximum M L in the luminescence spectrum are attributed to electronic-vibrational transitions with the creation and annihilation of localized excitons, respectively.

  6. Temperature and composition dependent excitonic luminescence and exciton-phonon coupling in CdSeS nanocrystals

    PubMed Central

    2012-01-01

    The yellow- and red-emitting CdSeS nanocrystals (NCs) synthesized through one-step organometallic synthesis method are uniformly assembled in polymethyl methacrylate (PMMA). A higher-energy emission band originates from band-edge excitonic state appeared at low temperature. With the Se dopant concentration increasing, the luminescent spectra of CdSeS NCs have a red-shifted emission peak and a shorter luminescent lifetime, which is attributed to the existence of trapping state caused by surface defect and Se dopant. CdSeS NC shows a shorter luminescence lifetime and higher energy emission peak in PMMA matrix than that in toluene, indicating that the former is more favorable to transfer energy through exciton-phonon coupling. The upconversion luminescence (UCL) is observed using 800 nm femtosecond laser excitation. The pump power dependence demonstrated UCL spectra of yellow-emitting CdSeS NCs has a slope of 2.2, while that of red-emitting CdSeS NCs has a slope of 1.4. The results demonstrate that the two-photon absorption plays a dominating role when Se concentration of CdSeS NCs is lower, while phonon-assisted UCL by one-photon excitation gradually takes place with the amount of Se dopants increasing. PMID:22682098

  7. Optical identification of sulfur vacancies: Bound excitons at the edges of monolayer tungsten disulfide

    PubMed Central

    Carozo, Victor; Wang, Yuanxi; Fujisawa, Kazunori; Carvalho, Bruno R.; McCreary, Amber; Feng, Simin; Lin, Zhong; Zhou, Chanjing; Perea-López, Néstor; Elías, Ana Laura; Kabius, Bernd; Crespi, Vincent H.; Terrones, Mauricio

    2017-01-01

    Defects play a significant role in tailoring the optical properties of two-dimensional materials. Optical signatures of defect-bound excitons are important tools to probe defective regions and thus interrogate the optical quality of as-grown semiconducting monolayer materials. We have performed a systematic study of defect-bound excitons using photoluminescence (PL) spectroscopy combined with atomically resolved scanning electron microscopy and first-principles calculations. Spatially resolved PL spectroscopy at low temperatures revealed bound excitons that were present only on the edges of monolayer tungsten disulfide and not in the interior. Optical pumping of the bound excitons was sublinear, confirming their bound nature. Atomic-resolution images reveal that the areal density of monosulfur vacancies is much larger near the edges (0.92 ± 0.45 nm−2) than in the interior (0.33 ± 0.11 nm−2). Temperature-dependent PL measurements found a thermal activation energy of ~36 meV; surprisingly, this is much smaller than the bound-exciton binding energy of ~300 meV. We show that this apparent inconsistency is related to a thermal dissociation of the bound exciton that liberates the neutral excitons from negatively charged point defects. First-principles calculations confirm that sulfur monovacancies introduce midgap states that host optical transitions with finite matrix elements, with emission energies ranging from 200 to 400 meV below the neutral-exciton emission line. These results demonstrate that bound-exciton emission induced by monosulfur vacancies is concentrated near the edges of as-grown monolayer tungsten disulfide. PMID:28508048

  8. Phonon-induced pure-dephasing of luminescence, multiple exciton generation, and fission in silicon clusters

    NASA Astrophysics Data System (ADS)

    Liu, Jin; Neukirch, Amanda J.; Prezhdo, Oleg V.

    2013-10-01

    The size and temperature dependence of the pure-dephasing processes involved in luminescence, multiple exciton generation (MEG), and multiple exciton fission (MEF) are investigated for Sin clusters (n = 5-10, 15) using ab initio molecular dynamics and optical response function theory. The cluster bandgaps correlate with two types of binding energy, indicating that bandgaps can be used to characterize cluster stability. Ranging from 5 to 100 fs, the dephasing times are found to be longest for MEF and shortest for MEG, with luminescence falling in the middle range. Generally, the dephasing is fast, if the orbitals supporting the pair of states involved in the superpositions differ in energy, atomic localization, and number of nodes. The dephasing accelerates with temperature, because more phonon modes are activated, and lower frequency acoustic modes are able to explore the anhamonic part of the potential energy surface. The temperature dependence is stronger for larger clusters, since they possess a wider range of low-frequency anharmonic modes. Our research indicates that rapid dephasing in Si clusters favors generation of independent charge carriers from single and multiple excitons, making the clusters a promising material for photon energy conversion. The simulations of the dephasing processes reported in this work assist in understanding of the exciton evolution pathways in inorganic semiconductor clusters and other nanoscale materials.

  9. 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.

  10. Excitons Bound to Shallow Donors in Thin GaAs/AlAs Quantum Wells

    NASA Astrophysics Data System (ADS)

    da Cunha Lima, I. C.; Ghazali, A.; Emmel, P. D.

    1996-03-01

    The binding energy of excitons to ionized shallow donors in GaAs/AlAs quantum well in the vicinity of the type-I to type-II transition was obtained for impurities lying anywhere in the structure. We included the Γ -X hybridization in the Brillouin zone, which comes into play when the energies of the conduction subband minima in the two materials become close. The calculation is performed variationally using a three parameters trial function similar to the one describing a singly ionized molecule. We obtain a ratio between the binding energy of the bound exciton and that of the neutral donor equals to 0.95± 0.005, for all values of well widths explored, and independent on the impurity position inside the well. The joint density of states for the transition from free to bound exciton was obtained, and the role played by the doping and the compensation on the exciton dynamics was made clear.

  11. Reduced bound exciton and surface exciton emissions in Al-doped ZnO nanorods exposed to ambient air

    NASA Astrophysics Data System (ADS)

    Zhang, Y. Z.; He, H. P.; Jin, Y. Z.; Zhao, B. H.; Ye, Z. Z.; Tang, H. P.

    2008-11-01

    Temperature-dependent photoluminescence (PL) spectroscopy is employed to investigate the effects of exposure to ambient air on the optical property of Al-doped ZnO nanorods. Low temperature PL of the as-grown nanorods shows dominant D0X (excitons bound to neutral donors) emission at 3.363 eV and surface state-related emission at 3.310 eV. After exposure to ambient air, both of them vanish and the first LO phonon replica of free exciton is observed instead. It is proposed that surface adsorption and indiffusion of oxygen in ambient air result in surface modification and destruction of D0X complex.

  12. Enhanced room temperature excitonic luminescence in ZnO/polymethyl methacrylate nanocomposites prepared by bulk polymerization

    NASA Astrophysics Data System (ADS)

    Paramo, J. Antonio; Strzhemechny, Yuri M.; Anžlovar, Alojz; Žigon, Majda; Orel, Zorica Crnjak

    2010-07-01

    Homogeneous ZnO/polymethyl methacrylate (PMMA) nanocomposites were prepared by incorporating ZnO nanoparticles synthesized in various diols into a PMMA matrix by the free-radical bulk polymerization. Room temperature photoluminescence spectra of the as-grown and PMMA-embedded ZnO nanoparticles exhibit an excitonic band-gap emission at 3.3 eV, a near band-gap emission at ˜3.1 eV and a broad defect band centered at ˜2.4 eV. Relative intensity of the defect versus band-gap luminescence depends on the parameters of ZnO preparation as well as the average particle size. However, PMMA-embedded particles produce a much stronger excitonic luminescence, whereas the ratio of the 3.1 to 2.4 eV remains approximately constant. There is no indication of random lasing threshold pointing to the ZnO/PMMA interfacial origin of the enhanced band-gap emission.

  13. Self-Trapped Exciton Luminescence in Mixed K1-xRbxI Crystals

    NASA Astrophysics Data System (ADS)

    Itoh, Minoru; Ohno, Nobuhito; Hashimoto, Satoshi

    1990-12-01

    The self-trapped exciton (STE) luminescence of mixed K1-xRbxI crystals has been investigated by using D2 lamp and synchrotron radiation as light sources at 11 K. The results show that the σ emission band is kept well over the whole composition range, and its decay time changes continuously from 2.0 ns in KI to 4.1 ns in RbI. It is found that the virtual-crystal model is quite valid for the singlet STE state which is responsible for the σ luminescence. The π emission band of KI is closely connected to the Ex band, not the π band, of RbI with increasing x. The π band of RbI disappears in the region x<0.4. These facts are compatible with a recent theoretical model indicating that at equilibrium the lowest triplet STE is situated off-center. A brief discussion of the exciton relaxation into STE states in alkali halides is presented.

  14. A study of the red-shift of a neutral donor bound exciton in GaN nanorods by hydrogenation

    NASA Astrophysics Data System (ADS)

    Park, Byung-Guon; Lee, Sang-Tae; Reddeppa, Maddaka; Kim, Moon-Deock; Oh, Jae-Eung; Lee, Sang-Kwon

    2017-09-01

    In this paper we account for the physics behind the exciton peak shift in GaN nanorods (NRs) due to hydrogenation. GaN NRs were selectively grown on a patterned Ti/Si(111) substrate using plasma-assisted molecular beam epitaxy, and the effect of hydrogenation on their optical properties was investigated in detail using low-temperature photoluminescence measurements. Due to hydrogenation, the emissions corresponding to the donor-acceptor pair and yellow luminescence in GaN NRs were strongly suppressed, while the emission corresponding to the neutral to donor bound exciton (D0X) exhibited red-shift. Thermal annealing of hydrogenated GaN NRs demonstrated the recovery of the D0X and deep level emission. To determine the nature of the D0X peak shift due to hydrogenation, comparative studies were carried out on various diameters of GaN NRs, which can be controlled by different growth conditions and wet-etching times. Our experimental results reveal that the D0X shift depends on the diameter of the GaN NRs after hydrogenation. The results clearly demonstrate that the hydrogenation leads to band bending of GaN NRs as compensated by hydrogen ions, which causes a red-shift in the D0X emission.

  15. A study of the red-shift of a neutral donor bound exciton in GaN nanorods by hydrogenation.

    PubMed

    Park, Byung-Guon; Lee, Sang-Tae; Reddeppa, Maddaka; Kim, Moon-Deock; Oh, Jae-Eung; Lee, Sang-Kwon

    2017-09-08

    In this paper we account for the physics behind the exciton peak shift in GaN nanorods (NRs) due to hydrogenation. GaN NRs were selectively grown on a patterned Ti/Si(111) substrate using plasma-assisted molecular beam epitaxy, and the effect of hydrogenation on their optical properties was investigated in detail using low-temperature photoluminescence measurements. Due to hydrogenation, the emissions corresponding to the donor-acceptor pair and yellow luminescence in GaN NRs were strongly suppressed, while the emission corresponding to the neutral to donor bound exciton (D(0)X) exhibited red-shift. Thermal annealing of hydrogenated GaN NRs demonstrated the recovery of the D(0)X and deep level emission. To determine the nature of the D(0)X peak shift due to hydrogenation, comparative studies were carried out on various diameters of GaN NRs, which can be controlled by different growth conditions and wet-etching times. Our experimental results reveal that the D(0)X shift depends on the diameter of the GaN NRs after hydrogenation. The results clearly demonstrate that the hydrogenation leads to band bending of GaN NRs as compensated by hydrogen ions, which causes a red-shift in the D(0)X emission.

  16. Internal structure of acceptor-bound excitons in wide-band-gap wurtzite semiconductors

    NASA Astrophysics Data System (ADS)

    Gil, Bernard; Bigenwald, Pierre; Paskov, Plamen P.; Monemar, Bo

    2010-02-01

    We describe the internal structure of acceptor-bound excitons in wurtzite semiconductors. Our approach consists in first constructing, in the context of angular momentum algebra, the wave functions of the two-hole system that fulfill Pauli’s exclusion’s principle. Second, we construct the acceptor-bound exciton states by adding the electron states in a similar manner that two-hole states are constructed. We discuss the optical selection rules for the acceptor-bound exciton recombination. Finally, we compare our theory with experimental data for CdS and GaN. In the specific case of CdS for which much experimental information is available, we demonstrate that, compared with cubic semiconductors, the sign of the short-range hole-exchange interaction is reversed and more than one order of magnitude larger. The whole set of data is interpreted in the context of a large value of the short-range hole-exchange interaction Ξ0=3.4±0.2meV . This value dictates the splitting between the ground-state line I1 and the other transitions. The values we find for the electron-hole spin-exchange interaction and of the crystal-field splitting of the two-hole state are, respectively, -0.4±0.1 and 0.2±0.1meV . In the case of GaN, the experimental data for the acceptor-bound excitons in the case of Mg and Zn acceptors, show more than one bound-exciton line. We discuss a possible assignment of these states.

  17. Delayed luminescence of luminol initiated by a membrane-bound peroxidase.

    PubMed

    Ikariyama, Y; Suzuki, S; Aizawa, M

    1981-09-01

    The luminescense of the luminol-H2O2 system was initiated by either free or membrane-bound horseradish peroxideae (HRP). The instantaneous luminescene decayed rapidly and was followed by the delayed luminescence in the presence of excess luminol. The delayed luminescence was characterized by a chain reaction, in which luminescence intensity increased exponentially. Membrane-bound HRP demonstrated that the delayed luminescence took place even in the absence of HRP if the instantaneous luminescence was initiated by HRP. A mechanism for the nonenzymatic luminescence is proposed and discussed.

  18. Observation of Excitonic N-Body Bound States: Polyexcitons in Diamond

    NASA Astrophysics Data System (ADS)

    Omachi, J.; Suzuki, T.; Kato, K.; Naka, N.; Yoshioka, K.; Kuwata-Gonokami, M.

    2013-07-01

    We have found a series of resonances associated with the bound state (polyexcitons, PENs) of N excitons up to N=6 in the emission spectra of diamond under two-photon excitation at around 10 K. Time-resolved spectra show a stepwise formation of PENs with smaller to larger N, as well as a successive decay from larger to smaller N. At higher excitation levels, the transformation of PENs into a condensed phase of electron-hole droplets occurs. The binding energies of the PENs, normalized to the exciton Rydberg energy, agree well with those of silicon, suggesting the universality of the phenomena.

  19. Carbon related donor bound exciton transitions in ZnO nanowires

    SciTech Connect

    Mohammadbeigi, F.; Kumar, E. Senthil; Alagha, S.; Anderson, I.; Watkins, S. P.

    2014-08-07

    Several shallow donor bound exciton photoluminescence (PL) transitions are reported in ZnO nanowires doped with carbon. The emission energies are in the range of 3360.8–3361.9 meV, close to previously reported emission lines due to excitons bound to donor point defects, such as Ga, Al, In, and H. The addition of small amounts of hydrogen during growth results in a strong enhancement of the PL of these carbon related emission lines, yet PL and annealing measurements indicate no appreciable bulk hydrogen. The observation of two electron satellites for these emission lines enables the determination of the donor binding energies. The dependence of exciton localization energy on donor binding energy departs somewhat from the usual linear relationship observed for group III donors, indicating a qualitatively different central cell potential, as one would expect for a complex. Emission lines due to excitons bound to ionized donors associated with these defects are also observed. The dependence of the PL emission intensities on temperature and growth conditions demonstrates that the lines are due to distinct complexes and not merely excited states of each other.

  20. Ultrafast microscopy captures the dynamics of bound excitons in twisted bilayer van der Waals materials

    NASA Astrophysics Data System (ADS)

    Patel, Hiral; Vogt, Kyle T.; Huang, Lujie; Park, Jiwoong; Graham, Matt W.

    2017-05-01

    Stacking and twisting 2D van der Walls (vdW) materials can create unique electronic properties that are not accessible in a single sheet of material. When two sheets of van der Waals material such as graphene are stacked in an off-axis angle, in a twisted bilayer graphene (tBLG) configuration, electronic properties are modified from interlayer orbital hybridization effects. For instance, in tBLG we can access both massless and massive chiral quasiparticles characteristics of graphene and bilayer graphene, as well as angle tunable optical resonances that are not present in graphene or bilayer graphene. In addition, first principle simulation predicts that upon optical resonant excitation of tBLG, bound exciton formation is a possibility due to cancelation of exciton-continuum coupling from anti-symmetric superposition of degenerate resonant transitions. In order to study possible bound exciton formation, we map out the electronic structure of single grain tBLG using multi-photon transient absorption microscopy. Surprisingly, upon resonant optical excitations, tBLG shows enhanced transient response with longer carrier compared to AB stacked bilayer graphene. Further, we find that the origin of this unexpected optical response can be best explained by the presence of a lower lying bound exciton state predicted by recent theoretical simulations. This suggests that tBLG is a novel 2D hybrid material that enables the creation of both strongly-bound excitons along-side highly-conductive continuum states. Recently, the family of 2D vdW materials has grown appreciably. As such, there are countless possibilities for stacking and twisting 2D vDw materials to produce similar interlayer electronic states for next generation optoelectronics.

  1. 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.

  2. The identification and nature of bound exciton I-line PL systems in ZnO

    SciTech Connect

    Johnston, K.; Cullen, J.; Henry, M. O.; McGlynn, Enda; Khawaga, Rehab I.

    2013-12-04

    The chemical identification of donor bound excitons in ZnO has been studied using radioactive ions. Implantations of {sup 117}Ag - which decays to radioactive Cd and In - have enabled the identification of the I{sub 2} optical feature as being the ionized donor counterpart of I{sub 9}, one of the most prominent optical features in the photoluminescence spectrum of ZnO. Both of these lines are consistent with In occupying a Zn site.

  3. Light-emitting conjugated polymers with microporous network architecture: interweaving scaffold promotes electronic conjugation, facilitates exciton migration, and improves luminescence.

    PubMed

    Xu, Yanhong; Chen, Long; Guo, Zhaoqi; Nagai, Atsushi; Jiang, Donglin

    2011-11-09

    Herein we report a strategy for the design of highly luminescent conjugated polymers by restricting rotation of the polymer building blocks through a microporous network architecture. We demonstrate this concept using tetraphenylethene (TPE) as a building block to construct a light-emitting conjugated microporous polymer. The interlocked network successfully restricted the rotation of the phenyl units, which are the major cause of fluorescence deactivation in TPE, thus providing intrinsic luminescence activity for the polymers. We show positive "CMP effects" that the network promotes π-conjugation, facilitates exciton migration, and improves luminescence activity. Although the monomer and linear polymer analogue in solvents are nonemissive, the network polymers are highly luminescent in various solvents and the solid state. Because emission losses due to rotation are ubiquitous among small chromophores, this strategy can be generalized for the de novo design of light-emitting materials by integrating the chromophores into an interlocked network architecture.

  4. 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.

  5. Strongly bound excitons in anatase TiO2 single crystals and nanoparticles

    DOE PAGES

    Baldini, E.; Chiodo, L.; Dominguez, A.; ...

    2017-04-13

    Anatase TiO2 is among the most studied materials for light-energy conversion applications, but the nature of its fundamental charge excitations is still unknown. Yet it is crucial to establish whether light absorption creates uncorrelated electron-hole pairs or bound excitons and, in the latter case, to determine their character. Here, by combining steady-state angle-resolved photoemission spectroscopy and spectroscopic ellipsometry with state-of-the-art ab initio calculations, we demonstrate that the direct optical gap of single crystals is dominated by a strongly bound exciton rising over the continuum of indirect interband transitions. This exciton possesses an intermediate character between the Wannier-Mott and Frenkel regimesmore » and displays a peculiar two-dimensional wavefunction in the three-dimensional lattice. The nature of the higher-energy excitations is also identified. Furthermore, the universal validity of our results is confirmed up to room temperature by observing the same elementary excitations in defect-rich samples (doped single crystals and nanoparticles) via ultrafast two-dimensional deep-ultraviolet spectroscopy.« less

  6. On the correlations between the excitonic luminescence efficiency and the QW numbers in multiple InGaN/GaN QW structure

    NASA Astrophysics Data System (ADS)

    Hospodková, A.; Oswald, J.; Zíková, M.; Pangrác, J.; Kuldová, K.; Blažek, K.; Ledoux, G.; Dujardin, C.; Nikl, M.

    2017-06-01

    In this work, we compare the luminescence results obtained on InGaN/GaN multiple quantum well (QW) structures with different numbers of QWs. Structures are designed for scintillating applications, where large QW number covering particle penetration depth is necessary, and fast luminescence response is required. Special attention is devoted to increase the intensity of fast excitonic QW emission and to decrease the luminescence of the QW defect band, which has slower luminescence response and is undesired for fast scintillator applications. We found that increasing the In content in QWs suppresses the defect band luminescence and decreasing the QW growth rate increases the photoluminescence (PL) intensity of excitonic luminescence. We also show that increasing the number of InGaN further improves the PL properties of InGaN QWs. The photoluminescence and cathodoluminescence characteristics are compared and discussed.

  7. Lowest optical excitations in molecular crystals: bound excitons versus free electron-hole pairs in anthracene.

    PubMed

    Hummer, Kerstin; Puschnig, Peter; Ambrosch-Draxl, Claudia

    2004-04-09

    By solving the Bethe-Salpeter equation for the electron-hole Green function for crystalline anthracene we find the lowest absorption peak generated by strongly bound excitons or by a free electron-hole pair, depending on the polarization direction being parallel to the short or the long molecular axis, respectively. Both excitations are shifted to lower energies by pressure. The physical difference of these excitations is apparent from the electron-hole wave functions. Our findings are a major contribution to solve the long-standing puzzle about the nature of the lowest optical excitations in organic materials.

  8. Formation and condensation of excitonic bound states in the generalized Falicov-Kimball model

    NASA Astrophysics Data System (ADS)

    Farkašovský, Pavol

    2017-01-01

    The density-matrix-renormalization-group method and the Hartree-Fock approximation with the charge-density-wave instability are used to study a formation and condensation of excitonic bound states in the generalized Falicov-Kimball model. In particular, we examine effects of various factors, such as the f -electron hopping, the local and nonlocal hybridizations, as well as the increasing dimension of the system on the excitonic momentum distribution N (q ) and especially on the number of zero-momentum excitons N0=N (q =0 ) in the condensate. It is found that the negative values of the f -electron hopping integrals tf support the formation of a zero-momentum condensate, whereas the positive values of tf have the fully opposite effect. The opposite effects on the formation of the condensate exhibit also the local and nonlocal hybridizations. The first one strongly supports the formation of the condensate, whereas the second one destroys it completely. Moreover, it was shown that the zero-momentum condensate remains robust with increasing dimension of the system.

  9. Exciton Lines in Luminescence Spectra of NixZn1-xO under Inner Shell Excitation

    NASA Astrophysics Data System (ADS)

    Churmanov, V. N.; Sokolov, V. I.; Gruzdev, N. B.; Ivanov, V. Yu.; Pustovarov, V. A.

    The paper presents the results of the study of two narrow luminescence lines I1 and I2 at the energies of 3.339 and 3.393 eV respectively in NiO and solid state solution Ni0.6Zn0.4O. The luminescence spectroscopy with a sub-nanosecond time resolution upon selective photoexcitation in the energy range of absorption of the inner shells Zn M- and Ni L2,3- edges of Zn- and Ni- ions was used to promote proposed earlier mechanism of origin of luminescence lines I1 and I2. Photoluminescence decay kinetics of NiO and solid state solution Ni0.6Zn0.4O under soft x-ray excitation are discussed. The doublet of I1 and I2 lines is believed to arise due to the radiative annihilation of p-d excitons.

  10. Localized excitons and defects in PbWO4 single crystals: a luminescence and photo-thermally stimulated disintegration study

    NASA Astrophysics Data System (ADS)

    Krasnikov, A.; Nikl, M.; Zazubovich, S.

    The cover picture refers to the article by Aleksei Krasnikov et al., that was selected as Editor's Choice [1]. It depicts a fragment of a lead tungstate (PbWO4) crystal lattice structure and illustrates the complex anion (WO4)2- tetrahedra bonded to the Pb2+ cation. Perturbation of the (WO4)2- tetrahedra by defects nearby results in exciton localization near the defects and a slightly different emission spectrum, which is shown in the diagram. Localized excitons are evidenced for the first time in the PbWO4 structure. Under selective irradiation of PbWO4 crystals in the ultraviolet spectral region, the decay of various localized excitons into stable defects takes place, which can be detected by a sensitive thermally stimulated luminescence method. Aleksei Krasnikov is a PhD student at the University of Tartu, Estonia. Martin Nikl holds a position as a senior scientist and head of the Laboratory of Luminescence and Scintillation Materials at the Institute of Physics of the Czech Academy of Sciences. Svetlana Zazubovich is a senior scientist at the Institute of Physics, University of Tartu. The research groups of Martin Nikl and Svetlana Zazubovich have been collaborating closely for the last 15 years mainly in the field of optical spectroscopy of wide band-gap scintillation materials

  11. Time-resolved luminescence from Jahn-Teller split states of self-trapped excitons in PbWO4

    NASA Astrophysics Data System (ADS)

    Itoh, Minoru; Sakurai, Takaaki

    2006-06-01

    This paper reports the observation of time-resolved luminescence from a self-trapped exciton (STE) localized at tetrahedral (WO4)2- complex anion in PbWO4 . The results clearly reveal that the STE luminescence is composed of three emission bands peaking at 407, 425, and 450nm . Such a composite nature is explained well by assuming that the lowest triplet states of the STE split into three sublevels owing to the symmetry lowering from Td to C3v due to the Jahn-Teller effect. This assumption is in accordance with the theoretical prediction of Bacci [M. Bacci, S. Porcinai, E. Mihóková, M. Nikl, and K. Polák, Phys. Rev. B 64, 104302 (2001); M. Bacci, E. Mihóková, and L. S. Schulman, ibid. 66, 132301 (2002)]. The decay curve of each component and its temperature dependence are investigated in the range of 77to300K . These results are discussed on the basis of an adiabatic potential energy diagram of the triplet STE state. Time-resolved luminescence spectra are also measured for Mo-doped PbWO4 crystals. From a comparison with the spectra of undoped PbWO4 crystals, the Mo-related luminescence is clearly separated from the intrinsic luminescence due to STEs.

  12. Donor bound excitons in ZnSe nanoresonators - Applications in quantum information science

    SciTech Connect

    Pawlis, A.; Lischka, K.; Sanaka, K.; Yamamoto, Y.; Sleiter, D.

    2014-05-15

    Here we summarize the advantages of excitons bound to isolated fluorine donor in ZnSe/ZnMgSe quantum well nano-structures. Devices based on these semiconductors, are particularly suited to implement concepts of the optical manipulation of quantum states in solid-state material. The fluorine donor in ZnSe provides a physical qubit with potential advantages over previously researched qubits. In this context we show several initial demonstrations of devices, such as a low-threshold microdisk laser and an indistinguishable single photon source. Additionally we demonstrate the realization of a controllable three-level-system qubit consisting of a single Fluorine donor in a ZnSe nano-pillar, which provides an optical accessible single electon spin qubit.

  13. Dynamics of Charged Excitons and Biexcitons in CsPbBr3 Perovskite Nanocrystals Revealed by Femtosecond Transient-Absorption and Single-Dot Luminescence Spectroscopy.

    PubMed

    Yarita, Naoki; Tahara, Hirokazu; Ihara, Toshiyuki; Kawawaki, Tokuhisa; Sato, Ryota; Saruyama, Masaki; Teranishi, Toshiharu; Kanemitsu, Yoshihiko

    2017-03-16

    Metal-halide perovskite nanocrystals (NCs) are promising photonic materials for use in solar cells, light-emitting diodes, and lasers. The optoelectronic properties of these devices are determined by the excitons and exciton complexes confined in their NCs. In this study, we determined the relaxation dynamics of charged excitons and biexcitons in CsPbBr3 NCs using femtosecond transient-absorption (TA), time-resolved photoluminescence (PL), and single-dot second-order photon correlation spectroscopy. Decay times of ∼40 and ∼200 ps were obtained from the TA and PL decay curves for biexcitons and charged excitons, respectively, in NCs with an average edge length of 7.7 nm. The existence of charged excitons even under weak photoexcitation was confirmed by the second-order photon correlation measurements. We found that charged excitons play a dominant role in luminescence processes of CsPbBr3 NCs. Combining different spectroscopic techniques enabled us to clarify the dynamical behaviors of excitons, charged excitons, and biexcitons.

  14. Tightly bound indirect exciton in single-layer hybrid organic-inorganic perovskite semiconductor

    NASA Astrophysics Data System (ADS)

    Li, Jing; Liu, Tao; Liew, Timothy C. H.

    2017-10-01

    We theoretically study the direct and indirect excitons (IXs) in a single-layer hybrid organic-inorganic perovskite (HOIP) semiconductor. Due to the 2D nature, the single-layer HOIP supports the large binding energy of IXs and direct excitons over a wide range of applied electric fields, which exceed the thermal energy of room temperature. Moreover, the ground-state IX has a lower energy than that of direct exciton, which will extend the coherence and relaxation time of IXs. This is beneficial to optoelectronic applications and excitonic information processing devices of IXs.

  15. Study of the Linewidths of Excitonic Luminescence Transitions in AlGaN Alloys

    NASA Astrophysics Data System (ADS)

    Bajaj, K. K.; Coli, Giuliano; Li, J.; Lin, Jingyu; Jiang, H. X.

    2001-03-01

    We have investigated the linewidth of excitonic photoluminescence transitions at 10 K and as a function of Al concentration in AlGaN alloys grown by low-pressure metal organic chemical vapor deposition on (0001) oriented sapphire substrates, with low-temperature GaN buffer layers. Al composition ranged from 0 to 35 percent. By means of a lineshape analysis of the excitonic transition we identify the contribution of the compositional disorder in the alloy to the excitonic linewidth and find that the values of the excitonic linewidths in our samples are considerably smaller than those reported recently[1]. These values of the excitonic linewidths, as expected, increase as a function of Al concentration and agree very well with those calculated by a model presented by Lee and Bajaj[2]. [1] G. Steude, B.K. Meyer, A. Göldner, A. Hoffmann, F. Bertram, J.Christen, H. Amano and I. Akasaki, Appl. Phys. Lett 74, 2456 (1999) [2] S. M. Lee and K. K. Bajaj, J. Appl. Phys. 73, 1788 (1993)

  16. Effect of interlayer interactions on exciton luminescence in atomic-layered MoS2 crystals.

    PubMed

    Kim, Jung Gon; Yun, Won Seok; Jo, Sunghwan; Lee, JaeDong; Cho, Chang-Hee

    2016-07-15

    The atomic-layered semiconducting materials of transition metal dichalcogenides are considered effective light sources with both potential applications in thin and flexible optoelectronics and novel functionalities. In spite of the great interest in optoelectronic properties of two-dimensional transition metal dichalcogenides, the excitonic properties still need to be addressed, specifically in terms of the interlayer interactions. Here, we report the distinct behavior of the A and B excitons in the presence of interlayer interactions of layered MoS2 crystals. Micro-photoluminescence spectroscopic studies reveal that on the interlayer interactions in double layer MoS2 crystals, the emission quantum yield of the A exciton is drastically changed, whereas that of the B exciton remains nearly constant for both single and double layer MoS2 crystals. First-principles density functional theory calculations confirm that a significant charge redistribution occurs in the double layer MoS2 due to the interlayer interactions producing a local electric field at the interfacial region. Analogous to the quantum-confined Stark effect, we suggest that the distinct behavior of the A and B excitons can be explained by a simplified band-bending model.

  17. Effect of interlayer interactions on exciton luminescence in atomic-layered MoS2 crystals

    NASA Astrophysics Data System (ADS)

    Kim, Jung Gon; Yun, Won Seok; Jo, Sunghwan; Lee, Jaedong; Cho, Chang-Hee

    2016-07-01

    The atomic-layered semiconducting materials of transition metal dichalcogenides are considered effective light sources with both potential applications in thin and flexible optoelectronics and novel functionalities. In spite of the great interest in optoelectronic properties of two-dimensional transition metal dichalcogenides, the excitonic properties still need to be addressed, specifically in terms of the interlayer interactions. Here, we report the distinct behavior of the A and B excitons in the presence of interlayer interactions of layered MoS2 crystals. Micro-photoluminescence spectroscopic studies reveal that on the interlayer interactions in double layer MoS2 crystals, the emission quantum yield of the A exciton is drastically changed, whereas that of the B exciton remains nearly constant for both single and double layer MoS2 crystals. First-principles density functional theory calculations confirm that a significant charge redistribution occurs in the double layer MoS2 due to the interlayer interactions producing a local electric field at the interfacial region. Analogous to the quantum-confined Stark effect, we suggest that the distinct behavior of the A and B excitons can be explained by a simplified band-bending model.

  18. Excitons Bound to Nitrogen Pairs in GaAs as Seen by Photoluminescence of High Spectral and Spatial Resolution

    SciTech Connect

    Karaiskaj, D.; Mascarenhas, A.; Klem, J. F.; Volz, K.; Stolz, W.; Adamcyk, M.; Tiedje, T.

    2007-01-01

    High resolution photoluminescence (PL) spectroscopy was performed on high quality bulk GaAs, lightly doped with the nitrogen isoelectronic impurity. The shallowest nitrogen pair bound exciton center labeled as X{sub 1} revealed a total of six transitions. The photoluminescence lines from a small ensemble of nitrogen centers showed polarization dependent intensity. High spectral resolution PL spectroscopy was combined with confocal spectroscopy experiments performed on a GaAs:N/AlGaAs heterostructure. The high spatial resolution achieved by this technique enables us to localize and examine individual nitrogen bound excitons. Similar spectral structure and polarization dependence was observed for individual N-pair centers in GaAs. Both techniques support the C{sub 2v} symmetry of such isoelectronic impurity centers. The comparison between the PL spectra from an ensemble of nitrogen pairs and individual centers demonstrate the ability of the single impurity technique to lift the orientational degeneracy.

  19. Aharonov-Bohm Beats in Excitonic Luminescence from Quantum Rings and Type-II Quantum Dots

    NASA Astrophysics Data System (ADS)

    Dias da Silva, Luis; Shahbazyan, Tigran

    2005-03-01

    We study the absorption spectrum of neutral magnetoexcitons confined in ring-like structures. Despite their neutral character, excitons exhibit strong modulation effects on the energy and oscillator strength in the presence of magnetic fields [1] that have been recently observed [2]. We calculate the absorption coefficient α for neutral excitons confined in circular ring geometries with radii Re for electrons and Rh for holes. A particularly interesting situation comes about when Re!=Rh and a net radial charge polarization arises. In this case, we consider an attractive Coulomb interaction proportional to (Re- Rh)-1 and the excitonic absorption peak shows oscillatory behavior as function of the applied magnetic field both in position and amplitude. Such oscillations strongly depend on the dipole moment P=e(Rh-Re) of the exciton and on the dielectric constant of the system. Such intensity changes could in principle be experimentally observed with single dot spectroscopy in quantum rings [3]. Supported by the NSF-IMC and NSF-RUI [1] A.O. Govorov et al. Phys. Rev. B 66 081309 (2002); A.O. Govorov et al. Physica E 13, 297 (2002). [2] E. Ribeiro et al. Phys Rev. Lett. 92 126402 (2004). [3] R.J. Warburton et al. Nature 405 (6789) 926 (2000).

  20. Observation of bound and antibound states of two excitons in GaAs single quantum well by two-dimensional coherent spectroscopy

    NASA Astrophysics Data System (ADS)

    Ogawa, Y.

    2017-05-01

    We study the bound and antibound states of two excitons in a GaAs single quantum well by two-dimensional coherent spectroscopy. We also propose a method to directly observe the amplitude and phase (real and imaginary parts) of optical fields by using a heterodyne interference technique and through synchronized detection of the interference signals. In this scheme, the mechanical fluctuation of an unstabilized interferometer does not affect the measurement. In addition, the amplitude and phase of the optical fields, resulting from the coherent interactions between light and matter, are directly obtained by comparing a reference heterodyne beating signal by using a two-phase lock-in amplifier. By using this method, the bound and antibound states of two excitons are observed. It is expected that the excitons are localized to the quantum islands and the lateral confinement induces the large repulsive energy between the two excitons.

  1. Band-edge optical transitions in a nonpolar-plane GaN substrate: exciton-phonon coupling and temperature effects

    NASA Astrophysics Data System (ADS)

    Wang, M. Z.; Xu, S. J.

    2016-09-01

    We present a detailed investigation of the band-edge optical transitions involving the interacting exciton-phonon system, especially first-order longitudinal optical (LO) phonon-assisted luminescence of bound and free excitons in m- and c-plane GaN substrates in a low temperature range from 4 K to 40 K. The main luminescence features of all of the three kinds of excitons can be well described by the theoretical models that take exciton-LO-phonon coupling into account. The effective Bohr radii of the excitons play a key role in determining the Huang-Rhys factor characterizing the exciton-LO-phonon coupling strength in GaN. An interesting oscillatory structure is found to appear in the low-temperature luminescence spectra of the nonpolar-plane GaN substrate, which needs to be clarified by further investigations.

  2. Defects activated photoluminescence in two-dimensional semiconductors: interplay between bound, charged, and free excitons.

    PubMed

    Tongay, Sefaattin; Suh, Joonki; Ataca, Can; Fan, Wen; Luce, Alexander; Kang, Jeong Seuk; Liu, Jonathan; Ko, Changhyun; Raghunathanan, Rajamani; Zhou, Jian; Ogletree, Frank; Li, Jingbo; Grossman, Jeffrey C; Wu, Junqiao

    2013-01-01

    Point defects in semiconductors can trap free charge carriers and localize excitons. The interaction between these defects and charge carriers becomes stronger at reduced dimensionalities, and is expected to greatly influence physical properties of the hosting material. We investigated effects of anion vacancies in monolayer transition metal dichalcogenides as two-dimensional (2D) semiconductors where the vacancies density is controlled by α-particle irradiation or thermal-annealing. We found a new, sub-bandgap emission peak as well as increase in overall photoluminescence intensity as a result of the vacancy generation. Interestingly, these effects are absent when measured in vacuum. We conclude that in opposite to conventional wisdom, optical quality at room temperature cannot be used as criteria to assess crystal quality of the 2D semiconductors. Our results not only shed light on defect and exciton physics of 2D semiconductors, but also offer a new route toward tailoring optical properties of 2D semiconductors by defect engineering.

  3. Simultaneous observation of free and defect-bound excitons in CH3NH3PbI3 using four-wave mixing spectroscopy.

    PubMed

    March, Samuel A; Clegg, Charlotte; Riley, Drew B; Webber, Daniel; Hill, Ian G; Hall, Kimberley C

    2016-12-15

    Solar cells incorporating organic-inorganic perovskite, which may be fabricated using low-cost solution-based processing, have witnessed a dramatic rise in efficiencies yet their fundamental photophysical properties are not well understood. The exciton binding energy, central to the charge collection process, has been the subject of considerable controversy due to subtleties in extracting it from conventional linear spectroscopy techniques due to strong broadening tied to disorder. Here we report the simultaneous observation of free and defect-bound excitons in CH3NH3PbI3 films using four-wave mixing (FWM) spectroscopy. Due to the high sensitivity of FWM to excitons, tied to their longer coherence decay times than unbound electron- hole pairs, we show that the exciton resonance energies can be directly observed from the nonlinear optical spectra. Our results indicate low-temperature binding energies of 13 meV (29 meV) for the free (defect-bound) exciton, with the 16 meV localization energy for excitons attributed to binding to point defects. Our findings shed light on the wide range of binding energies (2-55 meV) reported in recent years.

  4. Simultaneous observation of free and defect-bound excitons in CH3NH3PbI3 using four-wave mixing spectroscopy

    PubMed Central

    March, Samuel A.; Clegg, Charlotte; Riley, Drew B.; Webber, Daniel; Hill, Ian G.; Hall, Kimberley C.

    2016-01-01

    Solar cells incorporating organic-inorganic perovskite, which may be fabricated using low-cost solution-based processing, have witnessed a dramatic rise in efficiencies yet their fundamental photophysical properties are not well understood. The exciton binding energy, central to the charge collection process, has been the subject of considerable controversy due to subtleties in extracting it from conventional linear spectroscopy techniques due to strong broadening tied to disorder. Here we report the simultaneous observation of free and defect-bound excitons in CH3NH3PbI3 films using four-wave mixing (FWM) spectroscopy. Due to the high sensitivity of FWM to excitons, tied to their longer coherence decay times than unbound electron- hole pairs, we show that the exciton resonance energies can be directly observed from the nonlinear optical spectra. Our results indicate low-temperature binding energies of 13 meV (29 meV) for the free (defect-bound) exciton, with the 16 meV localization energy for excitons attributed to binding to point defects. Our findings shed light on the wide range of binding energies (2–55 meV) reported in recent years. PMID:27974815

  5. Simultaneous observation of free and defect-bound excitons in CH3NH3PbI3 using four-wave mixing spectroscopy

    NASA Astrophysics Data System (ADS)

    March, Samuel A.; Clegg, Charlotte; Riley, Drew B.; Webber, Daniel; Hill, Ian G.; Hall, Kimberley C.

    2016-12-01

    Solar cells incorporating organic-inorganic perovskite, which may be fabricated using low-cost solution-based processing, have witnessed a dramatic rise in efficiencies yet their fundamental photophysical properties are not well understood. The exciton binding energy, central to the charge collection process, has been the subject of considerable controversy due to subtleties in extracting it from conventional linear spectroscopy techniques due to strong broadening tied to disorder. Here we report the simultaneous observation of free and defect-bound excitons in CH3NH3PbI3 films using four-wave mixing (FWM) spectroscopy. Due to the high sensitivity of FWM to excitons, tied to their longer coherence decay times than unbound electron- hole pairs, we show that the exciton resonance energies can be directly observed from the nonlinear optical spectra. Our results indicate low-temperature binding energies of 13 meV (29 meV) for the free (defect-bound) exciton, with the 16 meV localization energy for excitons attributed to binding to point defects. Our findings shed light on the wide range of binding energies (2–55 meV) reported in recent years.

  6. Defects activated photoluminescence in two-dimensional semiconductors: interplay between bound, charged, and free excitons

    PubMed Central

    Tongay, Sefaattin; Suh, Joonki; Ataca, Can; Fan, Wen; Luce, Alexander; Kang, Jeong Seuk; Liu, Jonathan; Ko, Changhyun; Raghunathanan, Rajamani; Zhou, Jian; Ogletree, Frank; Li, Jingbo; Grossman, Jeffrey C.; Wu, Junqiao

    2013-01-01

    Point defects in semiconductors can trap free charge carriers and localize excitons. The interaction between these defects and charge carriers becomes stronger at reduced dimensionalities, and is expected to greatly influence physical properties of the hosting material. We investigated effects of anion vacancies in monolayer transition metal dichalcogenides as two-dimensional (2D) semiconductors where the vacancies density is controlled by α-particle irradiation or thermal-annealing. We found a new, sub-bandgap emission peak as well as increase in overall photoluminescence intensity as a result of the vacancy generation. Interestingly, these effects are absent when measured in vacuum. We conclude that in opposite to conventional wisdom, optical quality at room temperature cannot be used as criteria to assess crystal quality of the 2D semiconductors. Our results not only shed light on defect and exciton physics of 2D semiconductors, but also offer a new route toward tailoring optical properties of 2D semiconductors by defect engineering. PMID:24029823

  7. Anisotropic optical properties of free and bound excitons in highly strained A-plane ZnO investigated with polarized photoreflectance and photoluminescence spectroscopy

    NASA Astrophysics Data System (ADS)

    Nam, Yoon Sung; Lee, Sang Wook; Baek, K. S.; Chang, S. K.; Song, Jae-Ho; Song, Jung-Hoon; Han, Seok Kyu; Hong, Soon-Ku; Yao, Takafumi

    2008-05-01

    We have investigated the polarization dependence of the near-band-edge photoluminescence and photoreflectance spectra in nonpolar (A-plane) ZnO films under strong biaxial compressive strain. We show that anisotropic strain and the orientation of the nonpolar plane play an important role in determining the polarization selectivity and properties of excitonic transitions. We identified four distinct band-edge transitions at 3.449, 3.420, 3.386, and 3.326eV. They were identified as E2 and E1 free excitons, E1 excitons bound to a donor, and free-electron-to-bound-hole transition, respectively. Unlike previously reported results on relatively thick nonpolar films, the E1 exciton (lowest energy) was mainly polarized to E ⊥c and weakly polarized to E ∥c under strong biaxial compressive strain in the 100nm thick film. The E2 exciton (next higher energy) was exclusively polarized to E ∥c. The localization energy of DX is 34meV, which is much larger than that in polar ZnO, and the DX was not thermally delocalized even at room temperature.

  8. Bound states and quantization of screening in the Wannier-Mott excitons

    SciTech Connect

    Makowski, Adam J.

    2011-02-15

    The problem of validity of the simple relation {lambda}=(n+2l)(n+2l+1) between the screening length {lambda} and the number of bound states in the Stern-Howard potential is discussed and the results are compared with those obtained for some potential with the same limiting behavior as the former one. The main conclusion of the present study is that the above relation does not hold for the Stern-Howard potential but most likely it is very close to an unknown relation to be discovered for the potential.

  9. Luminescence signature of free exciton dissociation and liberated electron transfer across the junction of graphene/GaN hybrid structure

    PubMed Central

    Wang, Jun; Zheng, Changcheng; Ning, Jiqiang; Zhang, Lixia; Li, Wei; Ni, Zhenhua; Chen, Yan; Wang, Jiannong; Xu, Shijie

    2015-01-01

    Large-area graphene grown on Cu foil with chemical vapor deposition was transferred onto intentionally undoped GaN epilayer to form a graphene/GaN Schottky junction. Optical spectroscopic techniques including steady-state and time-resolved photoluminescence (PL) were employed to investigate the electron transfer between graphene and n-type GaN at different temperatures. By comparing the near-band-edge excitonic emissions before and after the graphene covering, some structures in the excitonic PL spectra are found to show interesting changes. In particular, a distinct “dip” structure is found to develop at the center of the free exciton emission peak as the temperature goes up. A mechanism that the first dissociation of some freely moveable excitons at the interface was followed by transfer of liberated electrons over the junction barrier is proposed to interpret the appearance and development of the “dip” structure. The formation and evolution process of this “dip” structure can be well resolved from the measured time-resolved PL spectra. First-principles simulations provide clear evidence of finite electron transfer at the interface between graphene and GaN. PMID:25567005

  10. Minerals as Time-Integrating Luminescence Detectors for setting bounds on dark matter particle characteristics

    NASA Astrophysics Data System (ADS)

    Polymeris, G. S.; Kitis, G.; Liolios, A. K.; Tsirliganis, N. C.; Zioutas, K.

    2006-06-01

    Terrestrial material, since its formation, is supposed to receive additional radiation dose from its exposure to fluxes of dark matter particles. The present work investigates the possibility for bound estimation of interaction parameters of dark matter particles with ordinary matter, by measuring the accumulated doses of certain geological materials. It is proposed that Thermoluminescence (TL) and Optically Stimulated Luminescence (OSL) could enable the differentiation between the individual dose components, attributing a possible excessive dose, beyond the anticipated from cosmic rays and environmental radioactivity, to interactions with dark matter particles. Dosimetric properties of natural calcium fluoride, such as low detectable dose limit and low energy threshold (well below 1 keV), indicate it as a promising Thermoluminescent Dosimeter (TLD) for the proposed method. The limitations imposed by the "background" of cosmic rays and environmental radioactivity are discussed, and initial limits for the interaction strengths with ordinary matter, and/or the mass of WIMPs and axions are derived. The use of sedimentary quartz, sited in a free-from background-radiation environment, would yield a value of 4×10 -8 GeV -1 as an upper limit for the axion-to-photon interaction constant gaγγ and a value of 3×10 -8 GeV as a lower limit for the neutralino mass. The best limits, g=1.1×10-10 GeV for solar axions and m=3000 GeV for neutralinos, could be derived for natural calcium fluoride as a dosimeter.

  11. Quantum Interference between Energy Absorption Processes of Molecular Exciton and Interface Plasmons on Luminescence Induced by Scanning Tunneling Microscopy

    NASA Astrophysics Data System (ADS)

    Miwa, Kuniyuki; Imasa, Hiroshi; Sakaue, Mamoru; Kasai, Hideaki; Kim, Yousoo

    2015-03-01

    Luminescence induced by the tunneling current of a scanning tunneling microscope (STM) from molecule-covered metal surfaces is attributed to radiative decays of molecules and interface plasmons localized near the tip-substrate gap region. Since the dynamics of molecule and interface plasmons strongly influence each other, the interplay between these dynamics gives rise to peculiar phenomena originating from quantum many-body effects. In this study, we develop the effective model of the system and investigate the luminescence properties using the nonequilibrium Green's function method. The results show that, in addition to the dynamics of molecule, energy reabsorption by interface plasmons have a critical role in determining the luminescence spectral profile of interface plasmons. The additional peak structure arises owing to the interference between these energy absorption processes. Origin of prominent peak and dip structures observed in recent experiments are identified by the developed theory. The details of the interference effects on the luminescence properties will be discussed. This work was supported by JSPS KAKENHI Grant Number 26886013.

  12. Luminescence of [Ru(bpy)2(dppz)]2+ Bound to RNA Mismatches

    PubMed Central

    McConnell, Anna J.; Song, Hang; Barton, Jacqueline K.

    2013-01-01

    The luminescence of rac-[Ru(bpy)2(dppz)]2+ (bpy = 2,2′-bipyridine and dppz = dipyrido[3,2-a:2′,3′-c]phenazine) was explored in the presence of RNA oligonucleotides containing a single RNA mismatch (CA and GG) in order to develop a probe for RNA mismatches. While there is minimal luminescence of [Ru(bpy)2(dppz)]2+ in the presence of matched RNA due to weak binding, the luminescence is significantly enhanced in the presence of a single CA mismatch. The luminescence differential between CA mismatched and matched RNA is substantially higher compared to the DNA analogue, and therefore, [Ru(bpy)2(dppz)]2+ appears to be also a sensitive light switch probe for a CA mismatch in duplex RNA. Although the luminescence intensity is lower in the presence of RNA than DNA, Förster resonance energy transfer (FRET) between the donor ruthenium complex and FRET acceptor SYTO 61 is successfully exploited to amplify the luminescence in the presence of the mismatch. Luminescence and quenching studies with sodium iodide suggest that [Ru(bpy)2(dppz)]2+ binds to these mismatches via metalloinsertion from the minor groove. This work provides further evidence that metalloinsertion is a general binding mode of octahedral metal complexes to thermodynamically destabilized mismatches not only in DNA, but also in RNA. PMID:23968195

  13. Luminescence of [Ru(bpy)2(dppz)]2+ bound to RNA mismatches.

    PubMed

    McConnell, Anna J; Song, Hang; Barton, Jacqueline K

    2013-09-03

    The luminescence of rac-[Ru(bpy)2(dppz)](2+) (bpy = 2,2'-bipyridine and dppz = dipyrido[3,2-a:2',3'-c]phenazine) was explored in the presence of RNA oligonucleotides containing a single RNA mismatch (CA and GG) in order to develop a probe for RNA mismatches. While there is minimal luminescence of [Ru(bpy)2(dppz)](2+) in the presence of matched RNA due to weak binding, the luminescence is significantly enhanced in the presence of a single CA mismatch. The luminescence differential between CA mismatched and matched RNA is substantially higher compared to the DNA analogue, and therefore, [Ru(bpy)2(dppz)](2+) appears to be also a sensitive light switch probe for a CA mismatch in duplex RNA. Although the luminescence intensity is lower in the presence of RNA than DNA, Förster resonance energy transfer (FRET) between the donor ruthenium complex and FRET acceptor SYTO 61 is successfully exploited to amplify the luminescence in the presence of the mismatch. Luminescence and quenching studies with sodium iodide suggest that [Ru(bpy)2(dppz)](2+) binds to these mismatches via metalloinsertion from the minor groove. This work provides further evidence that metalloinsertion is a general binding mode of octahedral metal complexes to thermodynamically destabilized mismatches not only in DNA but also in RNA.

  14. Bound excitons and many-body effects in x-ray absorption spectra of azobenzene-functionalized self-assembled monolayers

    NASA Astrophysics Data System (ADS)

    Cocchi, Caterina; Draxl, Claudia

    2015-11-01

    We study x-ray absorption spectra of azobenzene-functionalized self-assembled monolayers (SAMs), investigating excitations from the nitrogen K edge. Azobenzene with H-termination and functionalized with CF3 groups is considered. The Bethe-Salpeter equation is employed to compute the spectra, including excitonic effects, and to determine the character of the near-edge resonances. Our results indicate that core-edge excitations are intense and strongly bound: their binding energies range from about 6 to 4 eV, going from isolated molecules to densely-packed SAMs. Electron-hole correlation rules these excitations, while the exchange interaction plays a negligible role.

  15. Fast reconstruction of a bounded ultrasonic beam using acoustically induced piezo-luminescence

    SciTech Connect

    Kersemans, Mathias Lammens, Nicolas; Degrieck, Joris; Van Paepegem, Wim; Smet, Philippe F.

    2015-12-07

    We report on the conversion of ultrasound into light by the process of piezo-luminescence in epoxy with embedded BaSi{sub 2}O{sub 2}N{sub 2}:Eu as active component. We exploit this acoustically induced piezo-luminescence to visualize several cross-sectional slices of the radiation field of an ultrasonic piston transducer (f = 3.3 MHz) in both the near-field and the far-field. Simply combining multiple slices then leads to a fast representation of the 3D spatial radiation field. We have confronted the luminescent results with both scanning hydrophone experiments and digital acoustic holography results, and obtained a good correlation between the different approaches.

  16. Fast reconstruction of a bounded ultrasonic beam using acoustically induced piezo-luminescence

    NASA Astrophysics Data System (ADS)

    Kersemans, Mathias; Smet, Philippe F.; Lammens, Nicolas; Degrieck, Joris; Van Paepegem, Wim

    2015-12-01

    We report on the conversion of ultrasound into light by the process of piezo-luminescence in epoxy with embedded BaSi2O2N2:Eu as active component. We exploit this acoustically induced piezo-luminescence to visualize several cross-sectional slices of the radiation field of an ultrasonic piston transducer (f = 3.3 MHz) in both the near-field and the far-field. Simply combining multiple slices then leads to a fast representation of the 3D spatial radiation field. We have confronted the luminescent results with both scanning hydrophone experiments and digital acoustic holography results, and obtained a good correlation between the different approaches.

  17. Triplet-triplet energy transfer between luminescent probes bound to albumins

    NASA Astrophysics Data System (ADS)

    Mel'Nikov, A. G.; Saletskii, A. M.; Kochubey, V. I.; Pravdin, A. B.; Kurchatov, I. S.; Mel'Nikov, G. V.

    2010-08-01

    The interaction of polar and nonpolar luminescent probes with human blood serum albumins is studied by absorption and luminescence spectroscopy. It is found that the probes (polar eosin and nonpolar anthracene) can efficiently bind to proteins. The radii of the quenching spheres of energy-donor (eosin) triplet states in the presence of an acceptor (anthracene) in the process of the triplet-triplet energy transfer in proteins are determined for homogeneous and inhomogeneous distributions of acceptor molecules over the solution volume. It is shown that a decrease in the radius of the quenching sphere observed upon the addition of sodium dodecylsulfate surfactant is caused by structural changes in the protein.

  18. Self-trapped excitons in pure and Na- and Tl-doped caesium halides and the recombination luminescence

    NASA Astrophysics Data System (ADS)

    Fu, Chun-Rong; Chen, Ling-Fu; Song, K. S.

    1999-07-01

    On the basis of a method used earlier to predict the off-centre relaxed triplet self-trapped excitons in alkali halides, similar systems in caesium halides are studied. This work confirms the expected off-centre relaxation along the [100] cubic axes with increasing magnitude in the order CsI, CsBr and CsCl. The calculated emission energies are in reasonable agreement with observed values. The well-known 2.95 eV emission band of CsI:Na has been studied as a tunnelling recombination between a close pair consisting of a VK centre and a Na atom. For a number of close-pair geometries the emission energies are close to 3 eV. The strong emission bands of CsI:Tl at 2.25 eV and 2.55 eV have been interpreted as arising from tunnelling recombination of close pairs each consisting of a Tl0 and a VK centre. The calculated emission energies and polarizations are discussed in conjunction with the experimental data.

  19. Excitonic luminescence of polycrystalline CuInS2 solar cell material under the influence of strain

    NASA Astrophysics Data System (ADS)

    Eberhardt, J.; Metzner, H.; Schulz, K.; Reislöhner, U.; Hahn, Th.; Cieslak, J.; Witthuhn, W.; Goldhahn, R.; Hudert, F.; Kräußlich, J.

    2007-08-01

    Using molecular beams, polycrystalline CuInS2 (CIS) films were deposited on Mo-covered Si substrates. In order to investigate the influence of growth-induced strain on the optical and structural properties, detailed photoluminescence, photoreflectance and x-ray diffraction (XRD) measurements were performed. The transition energy of the free A-exciton (FXA) transition decreases with (i) decreasing thickness of the CIS layer at a constant thickness of the Mo buffer layer and (ii) increasing thickness of the Mo buffer layer at a constant CIS layer thickness. This appreciable redshift of FXA is accompanied by an increase of the energetic splittings between FXA, FXB, and FXC. When we compare theoretically predicted valence band splittings as a function of the crystal field—obtained from the calculated relative valence band energies—to our experimental values, a completely coherent picture is obtained. We also derived the structure of the conduction band as a function of crystal field, based on the theoretically expected valence band structures combined with the measured transition energies of FXA, FXB, and FXC. The XRD data show the increasing strain to occur with decreasing lattice spacings in growth direction.

  20. Core and valence exciton formation in x-ray absorption, x-ray emission and x-ray excited optical luminescence from passivated Si nanocrystals at the Si L2,3 edge

    NASA Astrophysics Data System (ADS)

    Šiller, L.; Krishnamurthy, S.; Kjeldgaard, L.; Horrocks, B. R.; Chao, Y.; Houlton, A.; Chakraborty, A. K.; Hunt, M. R. C.

    2009-03-01

    Resonant inelastic x-ray scattering (RIXS), x-ray absorption spectroscopy and x-ray excited optical luminescence (XEOL) have been used to measure element specific filled and empty electronic states over the Si L2,3 edge of passivated Si nanocrystals of narrow size distribution (diameter 2.2 ± 0.4 nm). These techniques have been employed to directly measure absorption and luminescence specific to the local Si nanocrystal core. Profound changes occur in the absorption spectrum of the nanocrystals compared with bulk Si, and new features are observed in the nanocrystal RIXS. Clear signatures of core and valence band exciton formation, promoted by the spatial confinement of electrons and holes within the nanocrystals, are observed, together with band narrowing due to quantum confinement. XEOL at 12 K shows an extremely sharp feature at the threshold of orange luminescence (i.e., at ~1.56 eV (792 nm)) which we attribute to recombination of valence excitons, providing a lower limit to the nanocrystal band gap.

  1. Synthesis and Resonance Energy Transfer in Conjugates of Luminescent Cadmium Selenide Quantum Dots and Chlorin e6 Molecules

    NASA Astrophysics Data System (ADS)

    Fedosyuk, A. A.; Artemyev, M. V.

    2013-05-01

    We synthesized a new type of conjugates of highly luminescent water soluble CdSe/ZnS colloidal quantum dots covalently bound to Chlorin e6 dye molecules. We observed a resonance energy transfer from quantum dots emitting at 660 nm to Chlorine e6 molecules in our conjugates which can be utilized for phototherapy. Contrary to that quantum dots emitting at 588 nm show non-resonance quenching of excitonic luminescence without the energy transfer to dye molecules.

  2. The Change of Donor-bound Excitonic Photoluminescence to Free-to-Donor Photoluminescence in Chlorine-doped ZnBeSe

    NASA Astrophysics Data System (ADS)

    Gu, Yi; Kuskovsky, Igor; Neumark, Gertrude; Maksimov, Oleg; Tamargo, Maria

    2002-03-01

    ZnSe has been of great interest for light emitting devices in the green-yellow region (490nm-590nm). However, ZnSe-based devices have been suffering from limited lifetimes due to, among other reasons, relatively easy formation of defects under excitation. Therefore, Be has been introduced into ZnSe system to increase the lattice hardness and, thus, increase the device lifetime [1]. For fabrication of such light emitting devices, both n-type and p-type ZnBeSe are required. Here we used photoluminescence (PL) to study our Cl-doped ZnBeSe. We show that at high temperatures (T>200K), the dominant PL is due to the free-to-donor transition, while at low temperatures the PL spectrum is, as expected, predominantly due to the donor-bound excitonic transition. The dominant peaks of PL spectra at high temperatures are well fitted with the free-to-bound line-shape function. The analysis of the PL at intermediate temperatures also corroborates our conclusions. The activation energy of Cl as a function of Be concentration will be discussed. [1] A.Waag, Th.Litz, F.Fischer. H.-J,Lugauer, T.Baron, K.Schull, U.Zehnder, T.Gerhard, U.Lunz, M.Keim, G.Reuscher, and G.Landwehr, J.Crystal Growth, 184/185, 1 (1998)

  3. Effects of sp-d exchange on a bound polaron and the g-factor of the exciton in a GaMnAs quantum dot

    NASA Astrophysics Data System (ADS)

    Lalitha, D.; John Peter, A.; Yoo, Chang Kyoo

    2013-08-01

    Magneto bound polaron in a GaMnAs/Ga0.6Al0.4As quantum dot is investigated with the inclusion of exchange interaction effects due to Mn alloy content and the geometrical confinement. The exciton binding energy and the optical transition energy are computed as functions of dot radius and the magnetic field strength for a fixed Mn alloy content (x = 0.02) in a GaMnAs quantum dot. Numerical calculations are performed using variational method within a single band effective mass approximation. The spin polaronic energy of the heavy hole exciton is studied with the spatial confinement using a mean field theory in the presence of magnetic field strength. The magnetization as a function of dot radius is investigated in a GaMnAs/Ga0.6Al0.4As quantum dot. The magnetic field induced size dependence of g-factor is studied. The effective g-factor of conduction (valence) band electron (hole) is obtained in the GaMnAs quantum dot. The results bring out that (i) the geometrical dependence on sp-d exchange interaction in the GaMnAs/Ga0.6Al0.4As quantum dot has great influence with the magnetic field strength, (ii) the Landé factor is more sensitive if the geometrical confinement effect is included and (iii) the value of g-factor increases when the magnetic field strength is enhanced for all the dot radii. Our results are in good agreement with the other investigators.

  4. Excitonic devices

    NASA Astrophysics Data System (ADS)

    Butov, L. V.

    2017-08-01

    Indirect excitons can be controlled by voltage, can travel over large distances before recombination, and can cool down close to the temperature of semiconductor crystal lattice and below the temperature of quantum degeneracy. These properties form the basis for the development of excitonic devices with indirect excitons. In this contribution, we overview our studies of excitonic devices. We present traps, lattices, conveyers, and ramps for studying basic properties of cold indirect excitons - cold bosons in semiconductor materials. We also present proof-of-principle demonstration for excitonic signal processing devices.

  5. Exciton diffusion, end quenching, and exciton-exciton annihilation in individual air-suspended carbon nanotubes

    NASA Astrophysics Data System (ADS)

    Ishii, A.; Yoshida, M.; Kato, Y. K.

    2015-03-01

    Luminescence properties of carbon nanotubes are strongly affected by exciton diffusion, which plays an important role in various nonradiative decay processes. Here we perform photoluminescence microscopy on hundreds of individual air-suspended carbon nanotubes to elucidate the interplay between exciton diffusion, end quenching, and exciton-exciton annihilation processes. A model derived from random-walk theory as well as Monte Carlo simulations are utilized to analyze nanotube length dependence and excitation power dependence of emission intensity. We have obtained the values of exciton diffusion length and absorption cross section for different chiralities, and diameter-dependent photoluminescence quantum yields have been observed. The simulations have also revealed the nature of a one-dimensional coalescence process, and an analytical expression for the power dependence of emission intensity is given.

  6. Size dependence of the polarizability and Haynes rule for an exciton bound to an ionized donor in a single spherical quantum dot

    SciTech Connect

    Feddi, E. Zouitine, A.; Oukerroum, A.; Zazoui, M.; Dujardin, F.; Assaid, E.

    2015-02-14

    We study the effect of an external electric field on an exciton bound to an ionized donor (D{sup +}, X) confined in a spherical quantum dot using a perturbative-variational method where the wave function and energy are developed in series of powers of the electric field strength. After testing this new approach in the determination of the band gap for some semiconductor materials, we generalize it to the case of (D{sup +}, X) in the presence of the electric field and for several materials ZnO, PbSe, and InAs, with significant values of the mass ratio. Three interesting results can be deduced: First, we show that the present method allows to determine the ground state energy in the presence of a weak electric field in a simple way (E = E{sub 0} − αf{sup 2}) using the energy without electric field E{sub 0} and the polarizability α. The second point is that our theoretical predictions show that the polarizability of (D{sup +}, X) varies proportionally to R{sup 3.5} and follows an ordering α{sub D{sup 0}}<α{sub X}<α{sub (D{sup +},X)}. The last point to highlight is that the Haynes rule remains valid even in the presence of a weak electric field.

  7. Optical properties of ionized donor-bound excitons confined in strained wurtzite ZnO/MgxZn1-xO quantum dots

    NASA Astrophysics Data System (ADS)

    Dongmei, Zheng; Zongchi, Wang; Boqi, Xiao

    2015-03-01

    Within the framework of the effective-mass approximation and the dipole approximation, considering the three-dimensional confinement of the electron and hole and the strong built-in electric field (BEF) in strained wurtzite ZnO/Mg0.25Zn0.75O quantum dots (QDs), the optical properties of ionized donor-bound excitons (D+, X) are investigated theoretically using a variational method. The computations are performed in the case of finite band offset. Numerical results indicate that the optical properties of (D+, X) complexes sensitively depend on the donor position, the QD size and the BEF. The binding energy of (D+, X) complexes is larger when the donor is located in the vicinity of the left interface of the QDs, and it decreases with increasing QD size. The oscillator strength reduces with an increase in the dot height and increases with an increase in the dot radius. Furthermore, when the QD size decreases, the absorption peak intensity shows a marked increment, and the absorption coefficient peak has a blueshift. The strong BEF causes a redshift of the absorption coefficient peak and causes the absorption peak intensity to decrease remarkably. The physical reasons for these relationships have been analyzed in depth. Project supported by the National Natural Science Foundation for Young Scientists of China (No. 11102100), the Program for New Century Excellent Talents in Fujian Province University (No. JA14285) and the Program for Young Top-Notch Innovative Talents of Fujian Province of China.

  8. Excitons in Cuprous Oxide: Photoionization and Other Multiphoton Processes

    NASA Astrophysics Data System (ADS)

    Frazer, Nicholas Laszlo

    In cuprous oxide (Cu2O), momentum from the absorption of two infrared photons to make an orthoexciton is conserved and detected through the photon component of a resulting mixed exciton/photon (quadrupole exciton polariton) state. I demonstrated that this process, which actually makes the photon momentum more precisely defined, is disrupted by photoionization of excitons. Some processes are known to affect exciton propagation in both the pump and exciton stages, such as phonon emission, exciton-exciton (Auger) scattering, and third harmonic generation. These processes alone were not able to explain all observed losses of excitons or all detected scattering products, which lead me to design an optical pump-probe experiment to measure the exciton photoionization cross section, which is (3.9+/-0.2) x 10-22 m2. This dissertation describes the synthesis of cuprous oxide crystals using oxidation of copper, crystallization from melt with the optical floating zone method, and annealing. The cuprous oxide crystals were characterized using time and space resolved luminescence, leading to the discovery of new defect properties. Selection rules and overall efficiency of third harmonic generation in these crystals were characterized. Exciton photoionization was demonstrated through the depletion of polariton luminescence by an optical probe, the production of phonon linked luminescence as a scattering product, temporal delay of the probe, and time resolved luminescence. The results are integrated with the traditional dynamical model of exciton densities. An additional investigation of copper/cuprous oxide/gold photovoltaic devices is appended.

  9. Probing dark exciton diffusion using photovoltage

    PubMed Central

    Mullenbach, Tyler K.; Curtin, Ian J.; Zhang, Tao; Holmes, Russell J.

    2017-01-01

    The migration of weakly and non-luminescent (dark) excitons remains an understudied subset of exciton dynamics in molecular thin films. Inaccessible via photoluminescence, these states are often probed using photocurrent methods that require efficient charge collection. Here we probe exciton harvesting in both luminescent and dark materials using a photovoltage-based technique. Transient photovoltage permits a real-time measurement of the number of charges in an organic photovoltaic cell, while avoiding non-geminate recombination losses. The extracted exciton diffusion lengths are found to be similar to those determined using photocurrent. For the luminescent material boron subphthalocyanine chloride, the photovoltage determined diffusion length is less than that extracted from photoluminescence. This indicates that while photovoltage circumvents non-geminate losses, geminate recombination at the donor–acceptor interface remains the primary recombination pathway. Photovoltage thus offers a general approach for extracting a device-relevant diffusion length, while also providing insight in to the dominant carrier recombination pathways. PMID:28128206

  10. Probing dark exciton diffusion using photovoltage

    NASA Astrophysics Data System (ADS)

    Mullenbach, Tyler K.; Curtin, Ian J.; Zhang, Tao; Holmes, Russell J.

    2017-01-01

    The migration of weakly and non-luminescent (dark) excitons remains an understudied subset of exciton dynamics in molecular thin films. Inaccessible via photoluminescence, these states are often probed using photocurrent methods that require efficient charge collection. Here we probe exciton harvesting in both luminescent and dark materials using a photovoltage-based technique. Transient photovoltage permits a real-time measurement of the number of charges in an organic photovoltaic cell, while avoiding non-geminate recombination losses. The extracted exciton diffusion lengths are found to be similar to those determined using photocurrent. For the luminescent material boron subphthalocyanine chloride, the photovoltage determined diffusion length is less than that extracted from photoluminescence. This indicates that while photovoltage circumvents non-geminate losses, geminate recombination at the donor-acceptor interface remains the primary recombination pathway. Photovoltage thus offers a general approach for extracting a device-relevant diffusion length, while also providing insight in to the dominant carrier recombination pathways.

  11. Free and bound excitonic effects in Al0.5Ga0.5N/Al0.35Ga0.65N MQWs with different Si-doping levels in the well layers

    PubMed Central

    He, Chenguang; Qin, Zhixin; Xu, Fujun; Hou, Mengjun; Zhang, Shan; Zhang, Lisheng; Wang, Xinqiang; Ge, Weikun; Shen, Bo

    2015-01-01

    Free exciton (FX) and bound exciton (BX) in Al0.5Ga0.5N/Al0.35Ga0.65N multiple quantum wells (MQWs) with different Si-doping levels in the well layers are investigated by photoluminescence (PL) spectra. Low temperature (10 K) PL spectra identify a large binding energy of 87.4 meV for the BX in undoped sample, and 63.6 meV for the BX in Si-doped (2 × 1018 cm−3) sample. They are attributed to O-bound and Si-bound excitons, respectively. The large binding energies of BX are assumed to originate from the strong quantum confinement in the quantum wells, which also leads to a stronger FX PL peak intensity in comparison with BX at 10 K. Si-doping is found to suppress the FX quenching by reducing threading dislocation density (TDD) in the well layers, leading to a significant improvement of IQE from 33.7% to 45%. PMID:26267249

  12. Reduction of Inhomogeneous Broadening of Exciton Luminescence in CdxZn1-xSe Ternary Alloys and CdxZn1-xSe ZnSe Multiple Quantum Wells Grown by Molecular-Beam Epitaxy under Se-Excess Supply

    NASA Astrophysics Data System (ADS)

    Fujimoto, Masakatsu; Shigematsu, Hiroshi; Senda, Kazuhiko; Yoshikawa, Mitsutoshi; Kubo, Hachiya; Yamada, Yoichi; Taguchi, Tsunemasa

    1999-06-01

    Optical and structural properties of CdxZn1-xSe ternary alloy layers grown by molecular-beam epitaxy (MBE) have been studied as a function of the Se/(Cd, Zn) beam pressure ratio (BPR). With increasing Se/(Cd, Zn) BPR, the inhomogeneous broadening of exciton luminescence and the rms roughness of surfaces decreased drastically. This indicates that Se-excess supply during MBE growth suppresses alloy composition fluctuation and also enhances two-dimensional growth nucleation. Furthermore, CdxZn1-xSe ZnSe multiple quantum well (MQW) structures have been fabricated under Se-excess supply. Biexciton luminescence from MQW structures was observed, even under a cw weak excitation condition (less than 100 mW/cm2). This observation reflects the finding that exciton lifetime increase as a result of the improvement of crystalline quality, which results in the enhancement of carrier accumulation.

  13. Observation of long-lived interlayer excitons in monolayer MoSe2–WSe2 heterostructures

    DOE PAGES

    Rivera, Pasqual; Schaibley, John R.; Jones, Aaron M.; ...

    2015-02-24

    Van der Waals bound heterostructures constructed with two-dimensional materials, such as graphene, boron nitride and transition metal dichalcogenides, have sparked wide interest in both device physics and technologies at the two-dimensional limit. One highly coveted heterostructure is that of differing monolayer transition metal dichalcogenides with type-II band alignment, with bound electrons and holes localized in individual monolayers, that is, interlayer excitons. Here, we report the observation of interlayer excitons in monolayer MoSe2–WSe2 heterostructures by photoluminescence and photoluminescence excitation spectroscopy. The energy and luminescence intensity are highly tunable by an applied vertical gate voltage. Moreover, we measure an interlayer exciton lifetimemore » of ~1.8 ns, an order of magnitude longer than intralayer excitons in monolayers. Ultimately, our work demonstrates optical pumping of interlayer electric polarization, which may provoke further exploration of interlayer exciton condensation, as well as new applications in two-dimensional lasers, light-emitting diodes and photovoltaic devices.« less

  14. 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.

  15. Bose-Einstein condensation of dipolar excitons in quantum wells

    NASA Astrophysics Data System (ADS)

    Timofeev, V. B.; Gorbunov, A. V.

    2009-02-01

    The experiments on Bose-Einstein condensation (BEC) of dipolar (spatially-indirect) excitons in the lateral traps in GaAs/AlGaAs Schottky-diode heterostructures with double and single quantum wells are presented. The condensed part of dipolar excitons under detection in the far zone is placed in k-space in the range which is almost two orders of magnitude less than thermal exciton wave vector. BEC occurs spontaneously in a reservoir of thermalized excitons. Luminescence images of Bose-condensate of dipolar excitons exhibit along perimeter of circular trap axially symmetrical spatial structures of equidistant bright spots which strongly depend on excitation power and temperature. By means of two-beam interference experiments with the use of cw and pulsed photoexcitation it was found that the state of dipolar exciton Bose-condensate is spatially coherent and the whole patterned luminescence configuration in real space is described by a common wave function.

  16. 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.

  17. Quenching of the luminescence intensity of GaN nanowires under electron beam exposure: impact of C adsorption on the exciton lifetime.

    PubMed

    Lähnemann, Jonas; Flissikowski, Timur; Wölz, Martin; Geelhaar, Lutz; Grahn, Holger T; Brandt, Oliver; Jahn, Uwe

    2016-11-11

    Electron irradiation of GaN nanowires in a scanning electron microscope strongly reduces their luminous efficiency as shown by cathodoluminescence imaging and spectroscopy. We demonstrate that this luminescence quenching originates from a combination of charge trapping at already existing surface states and the formation of new surface states induced by the adsorption of C on the nanowire sidewalls. The interplay of these effects leads to a complex temporal evolution of the quenching, which strongly depends on the incident electron dose per area. Time-resolved photoluminescence measurements on electron-irradiated samples reveal that the carbonaceous adlayer affects both the nonradiative and the radiative recombination dynamics.

  18. Exciton strings in an organic charge-transfer crystal

    NASA Astrophysics Data System (ADS)

    Kuwata-Gonokami, M.; Peyghambarian, N.; Meissner, K.; Fluegel, B.; Sato, Y.; Ema, K.; Shimano, R.; Mazumdar, S.; Guo, F.; Tokihiro, T.; Ezaki, H.; Hanamura, E.

    1994-01-01

    COLLECTIVE excitations resulting from many-body Coulomb interactions have been studied extensively in the solid state1: for example, the exchange interaction between the electrons in two excitons (bound electron-hole pairs) can bind the excitons together, forming a biexciton. At the other extreme, if the number of excitons is sufficiently large (~106), they can condense into a degenerate 'liquid' phase known as an electron-hole drop. But in conventional semiconductors, intermediate bound states, consisting of more than two excitons, are not formed. We show here, both theoretically and experimentally, that bound states of multiple excitons can form in the organic charge-transfer solid anthracene-(pyromellitic acid dianhydride). Coulomb interactions along the one-dimensional stacks of this material can stabilize trains of several charge-transfer excitons, and we refer to the resulting collective excitations as exciton strings.

  19. Pulse Area Control of Exciton Rabi Oscillation in InAs/GaAs Single Quantum Dot

    NASA Astrophysics Data System (ADS)

    Goshima, Keishiro; Komori, Kazuhiro; Yamauchi, Shohgo; Morohashi, Isao; Shikanai, Amane; Sugaya, Takayoshi

    2006-04-01

    We investigated the optical properties of an exciton and a charged exciton in an InAs/GaAs single quantum dot (QD) with truncated pyramidal shape by microspectroscopy, and clarified the difference of sub-band structure between the exciton and the charged exciton in the same single QD. We observed the exciton population of the excited states by monitoring the luminescence of the ground state exciton and succeeded in the experimental demonstration of Rabi oscillation of the exciton and the charged exciton. The transition dipole moments estimated from experimental results in a pure InAs QD are 32 and 40 D for the charged exciton and exciton, respectively, which were comparable to those in InGaAs QD.

  20. Quantum confinement effect in 6H-SiC quantum dots observed via plasmon-exciton coupling-induced defect-luminescence quenching

    NASA Astrophysics Data System (ADS)

    Guo, Xiaoxiao; Zhang, Yumeng; Fan, Baolu; Fan, Jiyang

    2017-03-01

    The quantum confinement effect is one of the crucial physical effects that discriminate a quantum material from its bulk material. It remains a mystery why the 6H-SiC quantum dots (QDs) do not exhibit an obvious quantum confinement effect. We study the photoluminescence of the coupled colloidal system of SiC QDs and Ag nanoparticles. The experimental result in conjunction with the theoretical calculation reveals that there is strong coupling between the localized electron-hole pair in the SiC QD and the localized surface plasmon in the Ag nanoparticle. It results in resonance energy transfer between them and resultant quenching of the blue surface-defect luminescence of the SiC QDs, leading to uncovering of a hidden near-UV emission band. This study shows that this emission band originates from the interband transition of the 6H-SiC QDs and it exhibits a remarkable quantum confinement effect.

  1. 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.

  2. 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

  3. Observation of long-lived interlayer excitons in monolayer MoSe2–WSe2 heterostructures

    SciTech Connect

    Rivera, Pasqual; Schaibley, John R.; Jones, Aaron M.; Ross, Jason S.; Wu, Sanfeng; Aivazian, Grant; Klement, Philip; Seyler, Kyle; Clark, Genevieve; Ghimire, Nirmal J.; Yan, Jiaqiang; Mandrus, D. G.; Yao, Wang; Xu, Xiaodong

    2015-02-24

    Van der Waals bound heterostructures constructed with two-dimensional materials, such as graphene, boron nitride and transition metal dichalcogenides, have sparked wide interest in both device physics and technologies at the two-dimensional limit. One highly coveted heterostructure is that of differing monolayer transition metal dichalcogenides with type-II band alignment, with bound electrons and holes localized in individual monolayers, that is, interlayer excitons. Here, we report the observation of interlayer excitons in monolayer MoSe2–WSe2 heterostructures by photoluminescence and photoluminescence excitation spectroscopy. The energy and luminescence intensity are highly tunable by an applied vertical gate voltage. Moreover, we measure an interlayer exciton lifetime of ~1.8 ns, an order of magnitude longer than intralayer excitons in monolayers. Ultimately, our work demonstrates optical pumping of interlayer electric polarization, which may provoke further exploration of interlayer exciton condensation, as well as new applications in two-dimensional lasers, light-emitting diodes and photovoltaic devices.

  4. Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides

    DOE PAGES

    Selig, Malte; Berghäuser, Gunnar; Raja, Archana; ...

    2016-11-07

    Atomically thin transition metal dichalcogenides are direct-gap semiconductors with strong light–matter and Coulomb interactions. The latter accounts for tightly bound excitons, which dominate their optical properties. Besides the optically accessible bright excitons, these systems exhibit a variety of dark excitonic states. They are not visible in the optical spectra, but can strongly influence the coherence lifetime and the linewidth of the emission from bright exciton states. We investigate the microscopic origin of the excitonic coherence lifetime in two representative materials (WS2 and MoSe2) through a study combining microscopic theory with spectroscopic measurements. We also show that the excitonic coherence lifetimemore » is determined by phonon-induced intravalley scattering and intervalley scattering into dark excitonic states. Particularly, we identify exciton relaxation processes involving phonon emission into lower-lying dark states that are operative at all temperatures, in WS2.« less

  5. Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides

    PubMed Central

    Selig, Malte; Berghäuser, Gunnar; Raja, Archana; Nagler, Philipp; Schüller, Christian; Heinz, Tony F.; Korn, Tobias; Chernikov, Alexey; Malic, Ermin; Knorr, Andreas

    2016-01-01

    Atomically thin transition metal dichalcogenides are direct-gap semiconductors with strong light–matter and Coulomb interactions. The latter accounts for tightly bound excitons, which dominate their optical properties. Besides the optically accessible bright excitons, these systems exhibit a variety of dark excitonic states. They are not visible in the optical spectra, but can strongly influence the coherence lifetime and the linewidth of the emission from bright exciton states. Here, we investigate the microscopic origin of the excitonic coherence lifetime in two representative materials (WS2 and MoSe2) through a study combining microscopic theory with spectroscopic measurements. We show that the excitonic coherence lifetime is determined by phonon-induced intravalley scattering and intervalley scattering into dark excitonic states. In particular, in WS2, we identify exciton relaxation processes involving phonon emission into lower-lying dark states that are operative at all temperatures. PMID:27819288

  6. Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides

    NASA Astrophysics Data System (ADS)

    Selig, Malte; Berghäuser, Gunnar; Raja, Archana; Nagler, Philipp; Schüller, Christian; Heinz, Tony F.; Korn, Tobias; Chernikov, Alexey; Malic, Ermin; Knorr, Andreas

    2016-11-01

    Atomically thin transition metal dichalcogenides are direct-gap semiconductors with strong light-matter and Coulomb interactions. The latter accounts for tightly bound excitons, which dominate their optical properties. Besides the optically accessible bright excitons, these systems exhibit a variety of dark excitonic states. They are not visible in the optical spectra, but can strongly influence the coherence lifetime and the linewidth of the emission from bright exciton states. Here, we investigate the microscopic origin of the excitonic coherence lifetime in two representative materials (WS2 and MoSe2) through a study combining microscopic theory with spectroscopic measurements. We show that the excitonic coherence lifetime is determined by phonon-induced intravalley scattering and intervalley scattering into dark excitonic states. In particular, in WS2, we identify exciton relaxation processes involving phonon emission into lower-lying dark states that are operative at all temperatures.

  7. Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides

    SciTech Connect

    Selig, Malte; Berghäuser, Gunnar; Raja, Archana; Nagler, Philipp; Schüller, Christian; Heinz, Tony F.; Korn, Tobias; Chernikov, Alexey; Malic, Ermin; Knorr, Andreas

    2016-11-07

    Atomically thin transition metal dichalcogenides are direct-gap semiconductors with strong light–matter and Coulomb interactions. The latter accounts for tightly bound excitons, which dominate their optical properties. Besides the optically accessible bright excitons, these systems exhibit a variety of dark excitonic states. They are not visible in the optical spectra, but can strongly influence the coherence lifetime and the linewidth of the emission from bright exciton states. We investigate the microscopic origin of the excitonic coherence lifetime in two representative materials (WS2 and MoSe2) through a study combining microscopic theory with spectroscopic measurements. We also show that the excitonic coherence lifetime is determined by phonon-induced intravalley scattering and intervalley scattering into dark excitonic states. Particularly, we identify exciton relaxation processes involving phonon emission into lower-lying dark states that are operative at all temperatures, in WS2.

  8. 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

  9. Strong charge-transfer excitonic effects and the Bose-Einstein exciton condensate in graphane.

    PubMed

    Cudazzo, Pierluigi; Attaccalite, Claudio; Tokatly, Ilya V; Rubio, Angel

    2010-06-04

    Using first principles many-body theory methods (GW+Bethe-Salpeter equation) we demonstrate that the optical properties of graphane are dominated by localized charge-transfer excitations governed by enhanced electron correlations in a two-dimensional dielectric medium. Strong electron-hole interaction leads to the appearance of small radius bound excitons with spatially separated electron and hole, which are localized out of plane and in plane, respectively. The presence of such bound excitons opens the path towards an excitonic Bose-Einstein condensate in graphane that can be observed experimentally.

  10. 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)

  11. Physical theory of excitons in conducting polymers.

    PubMed

    Brazovskii, Serguei; Kirova, Natasha

    2010-07-01

    In this tutorial review, we cover the solid state physics approach to electronic and optical properties of conducting polymers. We attempt to bring together languages and advantages of the solid state theory for polymers and of the quantum chemistry for monomers. We consider polymers as generic one-dimensional semiconductors with features of strongly correlated electronic systems. Our model combines the long range electron-hole Coulomb attraction with a specific effect of strong intra-monomer electronic correlations, which results in effective intra-monomer electron-hole repulsion. Our approach allows to go beyond the single-chain picture and to compare excitons for polymers in solutions and in films. The approach helps connecting such different questions as shallow singlet and deep triplet excitons, stronger binding of interchain excitons in films, crossings of excitons' branches, 1/N energies shifts in oligomers. We describe a strong suppression of the luminescence from free charge carriers by long-range Coulomb interactions. Main attention is devoted to the most requested in applications phenyl based polymers. The specifics of the benzene ring monomer give rise to existence of three possible types of excitons: Wannier-Mott, Frenkel and intermediate ones. We discuss experimental manifestations of various excitons and of their transformations. We touch effects of the time-resolved self-trapping by libron modes leading to formation of torsion polarons.

  12. Exciton-Exciton Interaction in KMnF3

    NASA Astrophysics Data System (ADS)

    Strauss, E.; Maniscalco, W. J.; Yen, W. M.; Kellner, U. C.; Gerhardt, V.

    1980-03-01

    Exciton dynamics in KMnF3 at exciton densities up to 1016 cm-3 are examined with time-resolved emission spectroscopy. The exciton emission line shifts and broadens with increasing exciton density. A nonlinear exciton decay channel is observed. These effects are found to be consistent with an exciton-exciton process. The shift scales with the exciton density and suggests that the effect is dominated by pairwise interactions up to the densities reached in these experiments.

  13. Exciton formation in semiconductors and the influence of a photonic environment.

    PubMed

    Kira, M; Hoyer, W; Stroucken, T; Koch, S W

    2001-10-22

    A fully microscopic theory is presented for interacting electrons, holes, photons, and phonons in semiconductor heterostructures. The formation dynamics and statistics of incoherent excitons are analyzed for different densities, lattice temperatures, and photonic environments. Luminescence experiments are shown to depend strongly on the photonic environment in contrast to suggested terahertz absorption measurements. Whereas luminescence in free space is dominated by plasma contributions, terahertz absorption should be able to directly measure excitonic populations.

  14. Remote Plasma Driven Modifications in Luminescent Properties of ZnO Nanopowders

    NASA Astrophysics Data System (ADS)

    Vallejo, Henry; Paramo, Antonio; Peters, Raul; Kumar, Pankaj; Strzhemechny, Yuri

    2008-10-01

    Photoluminescence (PL) spectra of several commercially available ZnO nanopowders were investigated for as-received and remote-plasma treated samples. Sample-to-sample spectral discrepancies, even for materials from the same vendor, were observed at room temperatures as well as at 8 K. These differences, in both the near-band transitions and defect luminescence, are significant enough to obscure possible spectral dependence on the average nanocrystalline grain size and the grain size distribution (as measured by electron microscopy). Temperature-dependent PL spectra were analyzed in detail for the bound exciton range. Numerical fits of peak intensities and peak positions vs. temperature for a number of excitonic emissions using Arrhenius and Varshni approximations yielded activation energies and Debye temperatures. Significant spectral modifications were observed, at room and low temperatures, after the nanopowders were treated with remote O, N, and H plasmas. Different plasma species produced distinct signatures in the spectra.

  15. Compensation of dipolar-exciton spin splitting in magnetic field

    NASA Astrophysics Data System (ADS)

    Gorbunov, A. V.; Timofeev, V. B.

    2013-03-01

    Magnetoluminescence of spatially indirect dipolar excitons in 25 nm GaAs/AlGaAs single quantum well collected within a lateral potential trap has been studied in Faraday geometry. The paramagnetic spin splitting of the luminescence line of the heavy-hole excitons in the trap centre is completely compensated at magnetic field below critical value ≈2 Т. The effect of spin splitting compensation is caused by the exchange interaction in dense exciton Bose gas which is in qualitative agreement with the existing theoretical concepts.

  16. 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.

  17. A new class of collective excitations: Exciton strings

    NASA Astrophysics Data System (ADS)

    Mazumdar, S.; Guo, F.; Meissner, K.; Fluegel, B.; Peyghambarian, N.

    1996-06-01

    Optical excitation in a strongly neutral quasi-one-dimensional mixed-stack charge-transfer solid results in an exciton state, in which the electron and the hole are bound by electrostatic Coulomb interactions that are large compared to the one-electron hopping. We present a joint theoretical-experimental demonstration of a new class of collective excitations, multiexcitons or exciton strings, consisting of a string of several (more than two) bound excitons, in a prototype neutral charge-transfer solid. The stability of the multiexciton states arise from the combined effects of one dimensionality and strong Coulomb interactions. Theoretically, we show that in narrow band one-dimensional semiconductors with long range Coulomb interactions, the occurrence of stable 2-exciton string (biexciton) necessarily implies stable higher multiexcitons. Experimentally, evidence for the multiexciton strings is demonstrated by femtosecond pump-probe spectroscopy of anthracene pyromellitic acid dianhydride. Excellent qualitative agreement is found between the calculated and the measured differential transmission spectra. Photoinduced absorptions to the 2-exciton string at low pump intensity and to the 3-exciton string at high pump intensity are observed, in agreement with the theory of excited state absorption. The 2-exciton string is confirmed also by a direct two-photon absorption measurement. The binding energies of the 2-exciton and the 3-exciton strings are obtained from the experimental data. The larger binding energy of the 3-exciton is in agreement with theory.

  18. Exciton-exciton interactions in CdWO{sub 4} irradiated by intense femtosecond vacuum ultraviolet pulses

    SciTech Connect

    Kirm, M.; Nagirnyi, V.; Feldbach, E.; De Grazia, M.; Carre, B.; Merdji, H.; Guizard, S.; Geoffroy, G.; Gaudin, J.; Fedorov, N.; Martin, P.; Vasil'ev, A.; Belsky, A.

    2009-06-15

    Exciton-exciton interaction is experimentally revealed and quantitatively analyzed in a wide band-gap scintillator material CdWO{sub 4}. Under high-intensity femtosecond vacuum ultraviolet excitation, the CdWO{sub 4} luminescence is quenched, while its decay becomes essentially nonexponential. We propose an analytical model, which successfully reproduces the decay kinetics recorded in a wide range of excitation densities. The dipole-dipole interaction between excitons leading to their nonradiative decay is shown to be the main cause of a nonproportional response common for many scintillators.

  19. Excitons in nanoscale systems.

    PubMed

    Scholes, Gregory D; Rumbles, Garry

    2006-09-01

    Nanoscale systems are forecast to be a means of integrating desirable attributes of molecular and bulk regimes into easily processed materials. Notable examples include plastic light-emitting devices and organic solar cells, the operation of which hinge on the formation of electronic excited states, excitons, in complex nanostructured materials. The spectroscopy of nanoscale materials reveals details of their collective excited states, characterized by atoms or molecules working together to capture and redistribute excitation. What is special about excitons in nanometre-sized materials? Here we present a cross-disciplinary review of the essential characteristics of excitons in nanoscience. Topics covered include confinement effects, localization versus delocalization, exciton binding energy, exchange interactions and exciton fine structure, exciton-vibration coupling and dynamics of excitons. Important examples are presented in a commentary that overviews the present understanding of excitons in quantum dots, conjugated polymers, carbon nanotubes and photosynthetic light-harvesting antenna complexes.

  20. Singlet fission of hot excitons in π-conjugated polymers.

    PubMed

    Zhai, Yaxin; Sheng, Chuanxiang; Vardeny, Z Valy

    2015-06-28

    We used steady-state 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 two luminescent and non-luminescent π-conjugated polymers. From the high energy step in the triplet EXPA(ω) spectrum of the luminescent polymer poly(dioctyloxy)phenylenevinylene (DOO-PPV) films, we identified a hot-exciton SF (HE-SF) process having threshold energy at E≈2E(T) (=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 HE-SF process was confirmed by the triplet MPA(B) response for excitation at E>2E(T), which shows typical SF response. This process is missing in DOO-PPV solution, showing that it is predominantly interchain in nature. By contrast, the triplet EXPA(ω) spectrum in the non-luminescent polymer polydiacetylene (PDA) is flat with an onset at E=E(g) (≈2.25 eV). From this, we infer that intrachain SF that involves a triplet-triplet pair state, also known as the 'dark' 2A(g) exciton, dominates the triplet photogeneration in PDA polymer as E(g)>2E(T). The intrachain SF process was also identified from the MPA(B) response of the triplet PA band in PDA. Our work shows that the SF process in π-conjugated polymers is a much more general process than thought previously.

  1. Excitons in boron nitride single layer

    NASA Astrophysics Data System (ADS)

    Galvani, Thomas; Paleari, Fulvio; Miranda, Henrique P. C.; Molina-Sánchez, Alejandro; Wirtz, Ludger; Latil, Sylvain; Amara, Hakim; Ducastelle, François

    2016-09-01

    Boron nitride single layer belongs to the family of two-dimensional materials whose optical properties are currently receiving considerable attention. Strong excitonic effects have already been observed in the bulk and still stronger effects are predicted for single layers. We present here a detailed study of these properties by combining ab initio calculations and a tight-binding Wannier analysis in both real and reciprocal space. Due to the simplicity of the band structure with single valence (π ) and conduction (π*) bands the tight-binding analysis becomes quasiquantitative with only two adjustable parameters and provides tools for a detailed analysis of the exciton properties. Strong deviations from the usual hydrogenic model are evidenced. The ground-state exciton is not a genuine Frenkel exciton, but a very localized tightly bound one. The other ones are similar to those found in transition-metal dichalcogenides and, although more localized, can be described within a Wannier-Mott scheme.

  2. Large-scale coherence of the bose condensate of spatially indirect excitons

    NASA Astrophysics Data System (ADS)

    Gorbunov, A. V.; Timofeev, V. B.

    2006-11-01

    The Bose condensation of spatially indirect (dipolar) excitons in a wide single quantum well in an electric field transverse to the heterolayers is analyzed. Voltage is applied between a metallic film on the surface (Schottky gate) and a conducting electron layer inside a heterostructure (integrated electrode). The excitation of dipolar excitons and observation of their luminescence are performed through circle windows in a metallic mask 5 μm in diameter. Excitons are collected in a ring lateral trap, which is formed along the window perimeter owing to the strongly inhomogeneous electric field. When the critical condensation conditions in pump and temperature are reached, a narrow line of dipolar excitons corresponding to the exciton condensate appears stepwise in the luminescence spectrum. Under these conditions, a spatially periodic structure of equidistant luminescence spots appears in the luminescence pattern that is observed through a window with a resolution of about 1 μm and is selected by means of an interference filter. An in situ optical Fourier transform of spatially periodic structures from the real space to the k space is derived. The resulting Fourier transforms reproducing the pattern of the luminescence intensity distribution in the far field exhibit the result of the destructive and constructive interference, as well as the fact that the luminescence is directed along the normal to the heterolayers. These results are consequences of the large-scale coherence of the condensed exciton state in the ring lateral trap. Direct measurements of double-beam interference from pairs of luminescence spots in the ring show that the spatial coherence length is no less than 4 μm. Such a large scale means that the experimentally observed periodic luminescence structures are described by a common wavefunction under the condition of the Bose condensation of dipolar excitons.

  3. Indirect optical absorption and origin of the emission from β-FeSi2 nanoparticles: Bound exciton (0.809 eV) and band to acceptor impurity (0.795 eV) transitions

    NASA Astrophysics Data System (ADS)

    Lang, R.; Amaral, L.; Meneses, E. A.

    2010-05-01

    We investigated the optical absorption of the fundamental band edge and the origin of the emission from β-FeSi2 nanoparticles synthesized by ion-beam-induced epitaxial crystallization of Fe+ implanted SiO2/Si(100) followed by thermal annealing. From micro-Raman scattering and transmission electron microscopy measurements it was possible to attest the formation of strained β-FeSi2 nanoparticles and its structural quality. The optical absorption near the fundamental gap edge of β-FeSi2 nanoparticles evaluated by spectroscopic ellipsometry showed a step structure characteristic of an indirect fundamental gap material. Photoluminescence spectroscopy measurements at each synthesis stage revealed complex emissions in the 0.7-0.9 eV spectral region, with different intensities and morphologies strongly dependent on thermal treatment temperature. Spectral deconvolution into four transition lines at 0.795, 0.809, 0.851, and 0.873 eV was performed. We concluded that the emission at 0.795 eV may be related to a radiative direct transition from the direct conduction band to an acceptor level and that the emission at 0.809 eV derives from a recombination of an indirect bound exciton to this acceptor level of β-FeSi2. Emissions 0.851 and 0.873 eV were confirmed to be typical dislocation-related photoluminescence centers in Si. From the energy balance we determined the fundamental indirect and direct band gap energies to be 0.856 and 0.867 eV, respectively. An illustrative energy band diagram derived from a proposed model to explain the possible transition processes involved is presented.

  4. 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.

  5. Excitonic emission and N- and B-incorporation in homoepitaxial CVD-grown diamond investigated by cathodoluminescence

    NASA Astrophysics Data System (ADS)

    Araujo, D.; Kadri, M.; Wade, M.; Bustarret, E.; Deneuville, A.

    2005-03-01

    Diamond is a very large bandgap material arising high expectations either for optoelectronic applications or for active semiconducting layers in specific electronic devices to be used under extreme conditions of pressure, temperature, wear or radiation, as well as in chemically aggressive environments. Unintentionally boron-doped diamond layers were grown by microwave plasma-assisted chemical vapour deposition (CVD) on {001}-oriented undoped Ib substrates with the addition of oxygen gas during growth. The relative quantities of nitrogen and boron incorporated in the diamond lattice are evaluated by cathodoluminescence (CL) spectra recorded at 5 K. Two different effects are shown to limit nitrogen incorporation: the substrate crystalline quality and the addition of oxygen into the precursor during the growth. First, the CL spectra are shown to change strongly near the edges of the substrate in the regions corresponding to different bulk crystal growth modes. Some regions show a luminescence governed by UV emission while in other regions, where the H3 defect-related luminescence of the substrate is much stronger, the film UV emission is reduced. Second, the relative importance of the free exciton emission with respect to those from the nitrogen-related H3 centre and from the boron-bound exciton is shown to increase with the addition of oxygen during growth. Such observations are of first importance to improve the spectral emission and absorption threshold of the diamond material in the deep UV range.

  6. Exciton mobility edge in CdS 1-xSe x solid solutions

    NASA Astrophysics Data System (ADS)

    Permogorov, S.; Reznitsky, A.; Verbin, S.; Lysenko, V.

    1983-07-01

    Low temperature emission spectra of localized excitons in CdS 1-xSe x solid solutions under the monochromatic excitation with tunable laser have been studied. It has been found that the luminescence of localized excitons has a high degree of linear polarization with respect to the polarization direction of exciting light. This polarization reflects the "hidden" anisotropy of macroscopically isotropic localized exciton system and strongly depends on the frequency of exciting light. Study of this dependence has permitted for the first time a determination of position of the "mobility edge" for exciton migration in disordered semiconductor solid solution.

  7. Cooling of radiative quantum dot excitons by THz-radiation

    NASA Astrophysics Data System (ADS)

    Boxberg, Fredrik; Tulkki, Jukka; Yusa, Go; Sakaki, Hiroyuki

    2007-04-01

    Yusa et al. reported an anomalous cooling of radiative quantum dot (QD) excitons by THz-radiation in [Proc. 24th ICPS, 1083 (1998)] We have analyzed this experiment using continuum elasticity, multi-band kṡp and spin-resolved Monte-Carlo methods. We show that the unexpected discovery is related to hole relaxation via piezo-electric potential minima, induced in the QD sample by InP stressor islands. The THz-radiation gives rise to a drift of dark excitons from the piezo-electric minima to radiative states in the deformation potential minimum. This increases the QD ground state luminescence at the expense of the luminescence from higher QD states. We reproduce also the delayed flash of QD ground state luminescences when a THz-radiation pulse hits the sample even ˜ 1 s after switching off the carrier generation.

  8. Ghost Fano Resonance of Excitons in Twisted Bilayer Graphene

    NASA Astrophysics Data System (ADS)

    Liang, Yufeng

    2014-03-01

    Metallic systems are generally considered to be unable to harbor tightly bound excitons because of the strong screening effect as well as the absence of a finite band gap. Previously, exception has only been found in one-dimensional metallic carbon nanotubes due to the depressed screening effects and the symmetry gap. We explore the exciton spectra of twisted bilayer graphene (tBLG) and predict the existence of even more strongly bound exciton (with binding energy as large as 0.5eV) in this system despite of its higher dimensionality. Based on our results from first-principles simulations and effective model calculations, a mechanism known as the ghost Fano resonance is proposed for the bound exciton formation in metallic systems beyond the dimensonality-related argument. Our results shed light on engineering the e-h excitations in the few-layer van der Waals heterojunction. NSF Grant No. DMR-1207141.

  9. Low-temperature luminescence and thermoluminescence from BeO:Zn single crystals

    NASA Astrophysics Data System (ADS)

    Ogorodnikov, I. N.; Petrenko, M. D.; Ivanov, V. Yu.

    2016-12-01

    Low-temperature luminescence and thermoluminescence (TL) of BeO:Zn single crystals have been studied in the temperature range of 6-380 K and energy ranges of 1.2-6.5 eV (emission spectra) and 3.7-20 eV (luminescence excitation and reflection spectra). The introduction of zinc impurity ions (0.05 at. %) into BeO host lattice leads to the creation of both the trapped electron and hole centers: Zn+ and Zn2+ O-. These two new centers are responsible for two TL glow peaks at 307 and 145 K with activation energies of 0.96 and 0.40 eV, and two emission bands at 6.0 and 1.9-2.6 eV. The first emission band is attributed to radiative annihilation of the Zn-impurity bound excitons, and the second one is associated with the intracenter electronic transitions in the defect complex comprising zinc impurity ion. The 6.0 eV luminescence center can be excited at 9.6 eV, the low-energy tail of the BeO host absorption, but below the first excitonic maximum (10.45 eV). The 1.9-2.6 eV luminescence center can be excited at the BeO optical transparency band. Both emission bands in BeO:Zn appear in the X-ray induced luminescence spectra at T = 6 K. This indicates that not only these luminescence centers are excited during band-to-band transitions, but they participate in recombination processes as well. The low-temperature (T0 = 6 K) TL study of BeO:Zn single crystals was made for the first time. Analysis of the low-temperature TL glow curves allowed us not only to experimentally determine the energy characteristics of the Zn impurity states in BeO:Zn, but reveal an extremely strong influence of the isovalent zinc impurity on fluctuation rearrangement of BeO host lattice. Note, the fluctuation rearrangement of BeO host lattice, which occurs in the temperature range of self-trapped exciton transformation (80-180 K), was previously known only for undoped BeO and BeO crystals with heterovalent impurities [I. N. Ogorodnikov and A. V. Kruzhalov, Proc. SPIE 2967 (1997) 42].

  10. Luminescence nanothermometry.

    PubMed

    Jaque, Daniel; Vetrone, Fiorenzo

    2012-08-07

    The current status of luminescence nanothermometry is reviewed in detail. Based on the main parameters of luminescence including intensity, bandwidth, bandshape, polarization, spectral shift and lifetime, we initially describe and compare the different classes of luminescence nanothermometry. Subsequently, the various luminescent materials used in each case are discussed and the mechanisms at the root of the luminescence thermal sensitivity are described. The most important results obtained in each case are summarized and the advantages and disadvantages of these approaches are discussed.

  11. Suppression of exciton-exciton annihilation in tungsten disulfide monolayers encapsulated by hexagonal boron nitrides

    NASA Astrophysics Data System (ADS)

    Hoshi, Yusuke; Kuroda, Takashi; Okada, Mitsuhiro; Moriya, Rai; Masubuchi, Satoru; Watanabe, Kenji; Taniguchi, Takashi; Kitaura, Ryo; Machida, Tomoki

    2017-06-01

    We investigates exciton-exciton annihilation (EEA) in tungsten disulfide (W S2) monolayers encapsulated by hexagonal boron nitride (hBN). It is revealed that decay signals observed by time-resolved photoluminescence (PL) are not strongly dependent on the exciton densities of hBN-encapsulated W S2 monolayers (W S2/hBN ) . In contrast, the sample without the bottom hBN layer (W S2/Si O2) exhibits a drastic decrease of decay time with increasing exciton density due to the appearance of a rapid PL decay component, signifying nonradiative EEA-mediated recombination. Furthermore, the EEA rate constant of W S2/hBN was determined as (6.3 ±1.7 ) ×10-3c m2s-1 , being about 2 orders of magnitude smaller than that of W S2/Si O2 . Thus, the observed EEA rate reduction played a key role in enhancing luminescence intensity at high exciton densities in the W S2 monolayer.

  12. Dirac cones and Dirac saddle points of bright excitons in monolayer transition metal dichalcogenides.

    PubMed

    Yu, Hongyi; Liu, Gui-Bin; Gong, Pu; Xu, Xiaodong; Yao, Wang

    2014-05-12

    In monolayer transition metal dichalcogenides, tightly bound excitons have been discovered with a valley pseudospin optically addressable through polarization selection rules. Here, we show that this valley pseudospin is strongly coupled to the exciton centre-of-mass motion through electron-hole exchange. This coupling realizes a massless Dirac cone with chirality index I = 2 for excitons inside the light cone, that is, bright excitons. Under moderate strain, the I = 2 Dirac cone splits into two degenerate I = 1 Dirac cones, and saddle points with a linear Dirac spectrum emerge. After binding an extra electron, the charged exciton becomes a massive Dirac particle associated with a large valley Hall effect protected from intervalley scattering. Our results point to unique opportunities to study Dirac physics, with exciton's optical addressability at specifiable momentum, energy and pseudospin. The strain-tunable valley-orbit coupling also implies new structures of exciton condensates, new functionalities of excitonic circuits and mechanical control of valley pseudospin.

  13. Identification of singlet and triplet states of negatively charged excitons in CdTe-based quantum wells

    NASA Astrophysics Data System (ADS)

    Astakhov, G. V.; Yakovlev, D. R.; Crooker, S. A.; Ossau, W.; Christianen, P. C. M.; Rudenkov, V. V.; Karczewski, G.; Wojtowicz, T.; Kossut, J.

    2004-02-01

    We present comprehensive study of negatively charged exciton in high magnetic fields for filling factors < 1. In magneto-optical spectra the fine structure was found to be contributed by neutral exciton and different a set of bound states of charged exciton. These states were identified due to their unique polarization properties charecteristics in emission and absorption spectra.

  14. Kinetic theory of exciton-exciton annihilation.

    PubMed

    May, Volkhard

    2014-02-07

    Weakly excited states of dye aggregates and supramolecular complexes can be characterized by single or two exciton states. Stronger excitation results in the presence of multiple excited molecules, and complex processes of internal energy transfer dynamics take place. The direct consideration of all excited states is limited to systems with a few molecules only. Therefore, an approach is used based on transition operators among the molecular states of interest and resulting in a dynamic theory for excitation energy transfer in strongly excited molecular systems. As a first application of this theory a detailed description of exciton-exciton annihilation is given. The obtained novel nonlinear theory is related to the standard description. Possible further approximation schemes in the offered theoretical framework are discussed.

  15. Upconversion luminescence from CdSe nanoparticles.

    PubMed

    Chen, Wei; Joly, Alan G; McCready, David E

    2005-06-08

    Efficient upconversion luminescence has been observed from CdSe nanoparticles ranging in size from 2.5 to 6 nm. The upconversion luminescence exhibits a near-quadratic laser power dependence. Emissions from both excitons and trap states are observed in the upconversion and photoluminescence spectra, and in the upconversion luminescence the emission from the trap states is enhanced relative to the trap-state emission in the photoluminescence. The upconversion decay lifetimes are slightly longer than the photoluminescence decay lifetimes. Time-resolved spectral measurements indicate that this is due to the involvement of long decay components from surface or trap states. Both the photoluminescence and upconversion luminescence decrease in intensity with increasing temperature due mainly to thermal quenching. All the observations indicate that trap states work as emitters rather than as intermediate states for upconversion luminescence and that two-photon absorption is the likely excitation mechanism.

  16. 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

  17. Exciton-phonon coupling efficiency in CdSe quantum dots embedded in ZnSe nanowires

    NASA Astrophysics Data System (ADS)

    Bounouar, S.; Morchutt, C.; Elouneg-Jamroz, M.; Besombes, L.; André, R.; Bellet-Amalric, E.; Bougerol, C.; den Hertog, M.; Kheng, K.; Tatarenko, S.; Poizat, J. Ph.

    2012-01-01

    Exciton luminescence of a CdSe quantum dot (QD) inserted in a ZnSe nanowire is strongly influenced by the dark exciton states. Because of the small size of these QDs (2-5 nm), exchange interaction between hole and electron is highly enhanced and we measured large energy splitting between bright and dark exciton states (ΔE∈[4,9.2] meV) and large spin-flip rates between these states. Statistics on many QDs showed that this splitting depends on the QD size. Moreover, we measured an increase of the spin-flip rate to the dark states with increasing energy splitting. We explain this observation with a model, taking into account the fact that the exciton-phonon interaction depends on the bright to dark exciton energy splitting, as well as on the size and shape of the exciton wave function. It also has consequences on the exciton line intensity at high temperature.

  18. Preparation of a DNA-bound [Ru(bpy)2(mbpibH2)]2+ film and its two-mode luminescence tuning by copper(II) ions and EDTA

    NASA Astrophysics Data System (ADS)

    Gan, Gui-Lian; Chao, Hui; Ji, Shi-Bo; Chen, Lin-Lin; Li, Hong

    2012-11-01

    An imidazophenanthroline-containing ruthenium(II) complex [Ru(bpy)2(mbpibH2)]2+ (bpy = 2,2'-bipyridine, mbpibH2 = 1,3-bis([1,10]phenanthroline[5,6-d]imidazol-2-yl)benzene) can bind DNA through groove-binding and/or non-classical intercalation modes, revealed by spectrophotometric methods, viscosity measurements and variable ionic strength experiments. On the basis of binding interactions between cationic [Ru(bpy)2(mbpibH2)]2+ and anionic DNA at a molar ratio of 1:1, a yellow transparent cast film has been assembled on an indium-tin oxide (ITO) surface using a solution-based self-standing method. The prepared DNA-[Ru(bpy)2(mbpibH2)]2+ film shows a bi-exponential luminescence decay with τ1 = 62.1 ns (8.0%) and τ2 = 594.5 ns (92.0%), whose lifetimes become much shorter than those of DNA-bound [Ru(bpy)2(mbpibH2)]2+ in buffer solutions. The Ru(II) complex with a free bi-dentate coordination site in the DNA cast film shows tunable luminescence, quenched dynamically by Cu2+ and restored by using EDTA to eliminate two modes of Cu2+-binding. The results from this study provide a significant foundation for better understanding the fabrication and modulation of a DNA-based solid luminescence device using the Ru(II) complexes as DNA-concentrating and signal-sensing agents.

  19. Photoluminescence and the exciton-phonon coupling in hydrothermally grown ZnO

    NASA Astrophysics Data System (ADS)

    Mendelsberg, R. J.; Allen, M. W.; Durbin, S. M.; Reeves, R. J.

    2011-05-01

    Near band-edge photoluminescence (PL) from hydrothermally grown bulk ZnO was studied as a function of temperature along with the effects of simultaneous excitation with below-gap photons, allowing for accurate assignment of the emission features not possible from low-temperature data alone. Free exciton emission was clearly observed at low temperatures and dominated the PL spectrum above 100 K. Emission from A excitons bound to three neutral donors dominated the low-temperature PL spectrum. Recombination of B excitons bound to these same neutral donors were also identified along with A excitons bound to the donors in their ionized state. A clear difference in the redshift of free and bound excitons with increasing temperature was observed and attributed to reduced exciton-phonon coupling for the bound excitons. Additionally, Fano resonance of the 1-LO replica of the dominant bound A exciton was observed to reduce its PL intensity which can lead to the misidentification of the 2-LO replica as a donor-acceptor-pair transition.

  20. Charge-transfer excitons at organic semiconductor surfaces and interfaces.

    PubMed

    Zhu, X-Y; Yang, Q; Muntwiler, M

    2009-11-17

    When a material of low dielectric constant is excited electronically from the absorption of a photon, the Coulomb attraction between the excited electron and the hole gives rise to an atomic H-like quasi-particle called an exciton. The bound electron-hole pair also forms across a material interface, such as the donor/acceptor interface in an organic heterojunction solar cell; the result is a charge-transfer (CT) exciton. On the basis of typical dielectric constants of organic semiconductors and the sizes of conjugated molecules, one can estimate that the binding energy of a CT exciton across a donor/acceptor interface is 1 order of magnitude greater than k(B)T at room temperature (k(B) is the Boltzmann constant and T is the temperature). How can the electron-hole pair escape this Coulomb trap in a successful photovoltaic device? To answer this question, we use a crystalline pentacene thin film as a model system and the ubiquitous image band on the surface as the electron acceptor. We observe, in time-resolved two-photon photoemission, a series of CT excitons with binding energies < or = 0.5 eV below the image band minimum. These CT excitons are essential solutions to the atomic H-like Schrodinger equation with cylindrical symmetry. They are characterized by principal and angular momentum quantum numbers. The binding energy of the lowest lying CT exciton with 1s character is more than 1 order of magnitude higher than k(B)T at room temperature. The CT(1s) exciton is essentially the so-called exciplex and has a very low probability of dissociation. We conclude that hot CT exciton states must be involved in charge separation in organic heterojunction solar cells because (1) in comparison to CT(1s), hot CT excitons are more weakly bound by the Coulomb potential and more easily dissociated, (2) density-of-states of these hot excitons increase with energy in the Coulomb potential, and (3) electronic coupling from a donor exciton to a hot CT exciton across the D

  1. Time-resolved photoluminescence study of excitonic relaxation in one-dimensional systems

    NASA Astrophysics Data System (ADS)

    Tanino, H.; Rühle, W. W.; Takahashi, K.

    1988-12-01

    Self-trapped exciton luminescence of quasi-one-dimensional (1D) halogen-bridged mixed-valence platinum complexes [Pt(II) (EA)4][Pt(IV)Cl2(EA)4] Cl4.4H2O (EA=ethylamine) and [Pt(II)(en)2] [Pt(IV)Cl2(en)2](ClO4)4 (en=1,2-diaminoethane) are studied by time-resolved photoluminescence experiments. The lifetimes of the luminescence of self-trapped exciton are exceptionally short, of the order of 100 psec. We interpret the short lifetime by a ``giant oscillator strength'' caused by a strong coupling between the electron and hole of the 1D charge transfer exciton and an extended polaronlike character of the 1D state. The lifetimes of the broad luminescence and of the resonant Raman lines during the barrier-free relaxation process are both faster than 7 psec.

  2. Effect of carrier confinement on effective mass of excitons and estimation of ultralow disorder in Al x Ga1-x As/GaAs quantum wells by magneto-photoluminescence.

    PubMed

    Haldar, S; Dixit, V K; Vashisht, Geetanjali; Khamari, Shailesh Kumar; Porwal, S; Sharma, T K; Oak, S M

    2017-07-07

    Effect of charge carrier confinement and ultra-low disorder acquainted in AlGaAs/GaAs multi-quantum well system is investigated via Magneto-photoluminescence spectroscopy. Significant increase of effective mass is observed for the confined exciton in narrow QWs. The foremost reason behind such an observation is due to the induced non-parabolicity in bands. Moreover, as the thickness of the QW are reduced, confined excitons in QW experience atomic irregularities at the hetero-junctions and their effects are prominent in the photoluminescence linewidth. Amount of photoluminescence line-broadening caused by the atomic irregularities at the hetero-junctions is correlated with average fluctuation (δ 1) in QW thickness. The estimated δ 1 for Al0.3Ga0.7As/GaAs QWs are found to be ±(0.14 - 1.6)× 'one monolayer thickness of GaAs layer'. Further, the strong perturbations due to magnetic field in a system helps in realizing optical properties of exciton in QWs, where magnetic field is used as a probe to detect ultralow defects in the QW. Additionally, the influence of magnetic field on the free and bound exciton luminescence is explained by a simple model. The proposed approach for measuring the interface and volume defects in an ultra-low disordered system by Magneto-PL spectroscopy technique will be highly beneficial in high mobility devices for advanced applications.

  3. Coherence of Bose-Einstein condensates of dipolar excitons in GaAs/AlGaAs heterostructures

    NASA Astrophysics Data System (ADS)

    Gorbunov, A. V.; Timofeev, V. B.

    2016-05-01

    Experiments relating to studies of the coherence of Bose condensates of dipolar excitons in GaAs/AlGaAs heterostructures with a wide, single quantum well and a Schottky gate are analyzed. Dipolar excitons were excited by light in an annular trap formed along the perimeter of a window in a metal gate with an applied electric voltage. A dual-beam interference technique involving interference combination of the amplitudes of the luminescence light field, together with subsequent analysis of first order correlators, is used to study the temporal (longitudinal) and spatial (transverse) coherence of the exciton condensates. It is found that the transverse coherence length of an exciton condensate is considerably longer than its thermal De Broglie wavelength. Experimental studies of the luminescence intensity correlator also confirm the coherence of the exciton Bose condensate.

  4. Gas–crystal phase transition in a 2D dipolar exciton system

    SciTech Connect

    Suris, R. A.

    2016-03-15

    A system of dipolar excitons at temperatures exceeding the expected Bose–Einstein condensation temperature is considered. It is shown that a first-order phase transition with the formation of a phase close to the crystal of such excitons is possible at such temperatures. The phase diagram in the range of low concentrations and temperatures is constructed. The effect of this transition on the luminescence spectrum of the system is analyzed.

  5. Control of exciton fluxes in an excitonic integrated circuit.

    PubMed

    High, Alex A; Novitskaya, Ekaterina E; Butov, Leonid V; Hanson, Micah; Gossard, Arthur C

    2008-07-11

    Efficient signal communication uses photons. Signal processing, however, uses an optically inactive medium, electrons. Therefore, an interconnection between electronic signal processing and optical communication is required at the integrated circuit level. We demonstrated control of exciton fluxes in an excitonic integrated circuit. The circuit consists of three exciton optoelectronic transistors and performs operations with exciton fluxes, such as directional switching and merging. Photons transform into excitons at the circuit input, and the excitons transform into photons at the circuit output. The exciton flux from the input to the output is controlled by a pattern of the electrode voltages. The direct coupling of photons, used in communication, to excitons, used as the device-operation medium, may lead to the development of efficient exciton-based optoelectronic devices.

  6. Exciton-exciton annihilation in organic polariton microcavities

    SciTech Connect

    Akselrod, G. M.; Tischler, Jonathan R.; Young, E. R.; Nocera, D.G.; Bulovic, Vladimir

    2010-09-27

    We investigate the incoherent diffusion of excitons in thin films (5.1±0.1 nm thick) of a highly absorbing J-aggregated cyanine dye material (106 cm-1 absorption constant) as the excitonic component of a polariton microcavity. Under high-intensity pulsed laser excitation, the J-aggregated molecular films exhibit significant exciton-exciton annihilation, indicating a large exciton diffusion radius of more than 100 nm. When the material is strongly coupled to a cavity, the polaritonic structure also shows exciton-exciton annihilation, which is a competing process against the establishment of a threshold population of polaritons needed for polariton lasing. This study suggests that exciton-exciton annihilation is a loss process which can significantly increase the lasing threshold in polariton microcavities.

  7. The convergence of longitudinal excitons onto the Γ5 transverse exciton in GaN and the thermal activation energy of longitudinal excitons

    NASA Astrophysics Data System (ADS)

    Elgawadi, Amal; Gainer, Gordon; Krasinski, Jerzy

    2013-08-01

    The crystal orientation dependence of GaN excitons was investigated via the photoluminescence (PL) technique. The PL emissions at a temperature of 10 K were obtained from two experimental configurations where the emission K vector (the propagation vector) was either parallel (K ∥ c) or perpendicular (K ∥ c) to the crystal c-axis. Longitudinal, transverse and donor-bound excitons were observed in the two configurations. However, the longitudinal excitons converged onto the transverse free exciton Γ5 in the K⊥c emission. This behavior was discussed in terms of electron screening due to the scattering of electrons moving perpendicular to charged dislocation lines. Additionally, the thermal activation energy of the longitudinal excitons was calculated from the temperature dependent PL measurements collected from the K ∥ c emission, and was found to be 5 to 6 times as high as the binding energy of the free excitons. This high energy was interpreted tentatively in view of the creation of polaritons in strong exciton-photon coupling regimes. These findings present fundamental concepts for applications such as vertical cavity surface-emitting lasers (VCSELs) and polariton lasers.

  8. Exciton localization in solution-processed organolead trihalide perovskites

    NASA Astrophysics Data System (ADS)

    He, Haiping; Yu, Qianqian; Li, Hui; Li, Jing; Si, Junjie; Jin, Yizheng; Wang, Nana; Wang, Jianpu; He, Jingwen; Wang, Xinke; Zhang, Yan; Ye, Zhizhen

    2016-03-01

    Organolead trihalide perovskites have attracted great attention due to the stunning advances in both photovoltaic and light-emitting devices. However, the photophysical properties, especially the recombination dynamics of photogenerated carriers, of this class of materials are controversial. Here we report that under an excitation level close to the working regime of solar cells, the recombination of photogenerated carriers in solution-processed methylammonium-lead-halide films is dominated by excitons weakly localized in band tail states. This scenario is evidenced by experiments of spectral-dependent luminescence decay, excitation density-dependent luminescence and frequency-dependent terahertz photoconductivity. The exciton localization effect is found to be general for several solution-processed hybrid perovskite films prepared by different methods. Our results provide insights into the charge transport and recombination mechanism in perovskite films and help to unravel their potential for high-performance optoelectronic devices.

  9. Exciton localization in solution-processed organolead trihalide perovskites

    PubMed Central

    He, Haiping; Yu, Qianqian; Li, Hui; Li, Jing; Si, Junjie; Jin, Yizheng; Wang, Nana; Wang, Jianpu; He, Jingwen; Wang, Xinke; Zhang, Yan; Ye, Zhizhen

    2016-01-01

    Organolead trihalide perovskites have attracted great attention due to the stunning advances in both photovoltaic and light-emitting devices. However, the photophysical properties, especially the recombination dynamics of photogenerated carriers, of this class of materials are controversial. Here we report that under an excitation level close to the working regime of solar cells, the recombination of photogenerated carriers in solution-processed methylammonium–lead–halide films is dominated by excitons weakly localized in band tail states. This scenario is evidenced by experiments of spectral-dependent luminescence decay, excitation density-dependent luminescence and frequency-dependent terahertz photoconductivity. The exciton localization effect is found to be general for several solution-processed hybrid perovskite films prepared by different methods. Our results provide insights into the charge transport and recombination mechanism in perovskite films and help to unravel their potential for high-performance optoelectronic devices. PMID:26996605

  10. 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.

  11. Quantum confinement-induced tunable exciton states in graphene oxide

    PubMed Central

    Lee, Dongwook; Seo, Jiwon; Zhu, Xi; Lee, Jiyoul; Shin, Hyeon-Jin; Cole, Jacqueline M.; Shin, Taeho; Lee, Jaichan; Lee, Hangil; Su, Haibin

    2013-01-01

    Graphene oxide has recently been considered to be a potential replacement for cadmium-based quantum dots due to its expected high fluorescence. Although previously reported, the origin of the luminescence in graphene oxide is still controversial. Here, we report the presence of core/valence excitons in graphene-based materials, a basic ingredient for optical devices, induced by quantum confinement. Electron confinement in the unreacted graphitic regions of graphene oxide was probed by high resolution X-ray absorption near edge structure spectroscopy and first-principles calculations. Using experiments and simulations, we were able to tune the core/valence exciton energy by manipulating the size of graphitic regions through the degree of oxidation. The binding energy of an exciton in highly oxidized graphene oxide is similar to that in organic electroluminescent materials. These results open the possibility of graphene oxide-based optoelectronic device technology. PMID:23872608

  12. Luminescence nanothermometry

    NASA Astrophysics Data System (ADS)

    Jaque, Daniel; Vetrone, Fiorenzo

    2012-07-01

    The current status of luminescence nanothermometry is reviewed in detail. Based on the main parameters of luminescence including intensity, bandwidth, bandshape, polarization, spectral shift and lifetime, we initially describe and compare the different classes of luminescence nanothermometry. Subsequently, the various luminescent materials used in each case are discussed and the mechanisms at the root of the luminescence thermal sensitivity are described. The most important results obtained in each case are summarized and the advantages and disadvantages of these approaches are discussed.The current status of luminescence nanothermometry is reviewed in detail. Based on the main parameters of luminescence including intensity, bandwidth, bandshape, polarization, spectral shift and lifetime, we initially describe and compare the different classes of luminescence nanothermometry. Subsequently, the various luminescent materials used in each case are discussed and the mechanisms at the root of the luminescence thermal sensitivity are described. The most important results obtained in each case are summarized and the advantages and disadvantages of these approaches are discussed. This work was supported by the Universidad Autónoma de Madrid and Comunidad Autónoma de Madrid (Project S2009/MAT-1756), by the Spanish Ministerio de Educacion y Ciencia (MAT2010-16161) and by Caja Madrid Foundation.

  13. Exciton-exciton interaction in transition-metal dichalcogenide monolayers

    NASA Astrophysics Data System (ADS)

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

    2017-09-01

    We study theoretically the Coulomb interaction between excitons in transition metal dichalcogenide (TMD) monolayers. We calculate direct and exchange interaction for both ground and excited states of excitons. The screening of the Coulomb interaction, specific to monolayer structures, leads to the unique behavior of the exciton-exciton scattering for excited states, characterized by the nonmonotonic dependence of the interaction as function of the transferred momentum. We find that the nontrivial screening enables the description of TMD exciton interaction strength by approximate formula which includes exciton binding parameters. The influence of screening and dielectric environment on the exciton-exciton interaction was studied, showing qualitatively different behavior for ground state and excited states of excitons. Furthermore, we consider exciton-electron interaction, which for the excited states is governed by the dominant attractive contribution of the exchange component, which increases with the excitation number. The results provide a quantitative description of the exciton-exciton and exciton-electron scattering in transition metal dichalcogenides, and are of interest for the design of perspective nonlinear optical devices based on TMD monolayers.

  14. The deformation stimulated luminescence in KCl, KBr and KI crystals

    NASA Astrophysics Data System (ADS)

    Shunkeyev, K.; Sergeyev, D.; Drozdowski, W.; Brylev, K.; Myasnikova, L.; Barmina, A.; Zhanturina, N.; Sagimbaeva, Sh; Aimaganbetova, Z.

    2017-05-01

    Currently, strengthening of the intensity of luminescence in alkali halide crystals (AHC) at lattice symmetry lowering is discussed as a promising direction for the development of scintillation detectors [1-3]. In this regard, for the study of anion excitons and radiation defects in the AHC anion sublattice at deformation, the crystals with the same sizes of cations and different sizes of anions were chosen. In the X-ray spectra of KCl at 10 K, the luminescence at 3.88 eV; 3.05 eV and 2.3 eV is clearly visible. The luminescence at 3.05 eV corresponds to the tunneling recharge [F*, H]. Luminescence at 3.88 eV is quenched in the region of thermal destruction of F‧-centers and characterizes tunneling recharge of F‧, VK-centers. In KCl at 90 K, the luminescence of self-trapped excitons (STE) is completely absent. In KBr at deformation not only STE luminescence, but also deformation stimulated luminescence at 3.58 eV were recorded, the last one corresponds to tunneling recharge of F‧, VK-centers. In KI crystal at 10 K and 90 K at deformation, only STE luminescence is enhanced. There are no deformation luminescence bands in KI compares with KBr and KCl crystals.

  15. The Aharonov-Bohm effect for an exciton

    NASA Astrophysics Data System (ADS)

    Römer, R. A.; Raikh, M. E.

    2000-03-01

    We study theoretically the exciton absorption (luminescence) of a ring-like quantum dot shreded by a magnetic flux. We consider the limit when the width of the ring is smaller than the excitonic Bohr radius a_B. We demonstrate that, despite the electrical neutrality of the exciton, both the spectral position of the exciton peak in the absorption (luminescence), and the corresponding oscillator strength oscillate with magnetic flux with a period Φ0 --- the universal flux quantum. Assuming that the attraction between electron and hole is short-ranged we find analytically the functional form of these oscillations for both quantities.^1 This enables us to trace the magnitude of the effect with changing the ratio 2 π R/aB where R is the radius of the ring. Physically, the origin of the oscillations is the finite probability for electron and hole, created by a photon at the same point, to tunnel in the opposite directions and meet each other on the opposite side of the ring. Possible candidates for the experimental observation of the effect are recently discovered self-assembled quantum ring-like structures of InAs embedded in GaAs.^2,3 ^1R.A. Römer and M.E. Raikh, preprint cond-mat/9906314. ^2A. Lorke et al., Microelectronic Engeneering 47, 95 (1999). ^3H. Petterson et al., Proceedings of EP2DS-13, to be published in Physica E, (1999).

  16. Transport of dipolar excitons in (Al,Ga)N/GaN quantum wells

    NASA Astrophysics Data System (ADS)

    Fedichkin, F.; Andreakou, P.; Jouault, B.; Vladimirova, M.; Guillet, T.; Brimont, C.; Valvin, P.; Bretagnon, T.; Dussaigne, A.; Grandjean, N.; Lefebvre, P.

    2015-05-01

    We investigate the transport of dipolar indirect excitons along the growth plane of polar (Al,Ga)N/GaN quantum well structures by means of spatially and time-resolved photoluminescence spectroscopy. The transport in these strongly disordered quantum wells is activated by dipole-dipole repulsion. The latter induces an emission blue shift that increases linearly with exciton density, whereas the radiative recombination rate increases exponentially. Under continuous, localized excitation, we observe continuously decreasing emission energy, as excitons propagate away from the excitation spot. This corresponds to a steady-state gradient of exciton density, measured over several tens of micrometers. Time-resolved microphotoluminescence experiments provide information on the dynamics of recombination and transport of dipolar excitons. We account for the ensemble of experimental results by solving the nonlinear drift-diffusion equation. Quantitative analysis suggests that in such structures, exciton propagation on the scale of 10 to 20 μ m is mainly driven by diffusion, rather than by drift, due to the strong disorder and the presence of nonradiative defects. Secondary exciton creation, most probably by the intense higher-energy luminescence, guided along the sample plane, is shown to contribute to the exciton emission pattern on the scale up to 100 μ m . The exciton propagation length is strongly temperature dependent, the emission being quenched beyond a critical distance governed by nonradiative recombination.

  17. Luminescence and photoconductivity of high-purity cadmium selenide

    SciTech Connect

    Martynov, V.N.

    1995-10-01

    Slightly off-stoichlometric high-purity cadmium and zinc chalcogenides are used as high-efficiency sensors in various optoelectronic devices. The procedure for preparing high-purity chalcogenides was described elsewhere. Such materials (wurtzite-type structure, sp. gr. C{sup 4}{sub 6v}) exhibit exciton luminescence and the photoconductivity associated with the A-, B-, and C-excitonic series over a wide temperature range. In this work, we studied the luminescence and photoconductivity (PC) of cadmium selenide prepared as described.

  18. Phase Separation of Bright and Dark Excitons in Coupled Quantum Wells

    NASA Astrophysics Data System (ADS)

    Sinclair, Nicholas; Voros, Zoltan; Wuenschell, Jeff; Snoke, David; West, Kenneth; Pfeiffer, Loren

    2009-03-01

    The diversity and complexity of solid-state environments suggests that Bose-Einstein Condensation (BEC) of excitations in a solid might manifest in a variety of interesting ways, in correspondence with the diversity of features among ground states of these systems. The pursuit of excitonic BEC is both enriched and obfuscated by this flexibility of condensate character. Previous research pursuing BEC of interwell excitons in GaAs coupled quantum wells (CQWs) has focused attention on observing unusual luminescence from `bright', dipole-coupled (J=1) excitons to detect a BEC. However, theorists have recently predicted a `dark' (J=2) ground state for interwell excitons in GaAs. Our recent work with interwell excitons confined in stress-induced, in-plane traps shows the critical onset of a dark spot in the exciton-recombination luminescence at trap center, suggestive of a dense population of dark excitons and a phase separation between the dark/bright species. The critical temperature vs. density in the low temperature regime matches well with ideal 2D harmonic trap BEC criteria, and preliminary theoretical work suggests that this degree of species separation cannot be explained by a model based on classical statistical level occupation using the bright/dark state energy separation.

  19. Indirect exciton luminescense and Raman scattering in CdI 2

    NASA Astrophysics Data System (ADS)

    Hayashi, T.; Ohata, T.; Koshino, S.

    1981-06-01

    Intrinsic luminescence and Raman scattering in 4HCdI 2 have been investigated at 2 K. Weak emission bands observed near the absorption edge are attributed to the phonon-assistes indirect exciton luminescence. Several new Raman lines are observed under resonant excitation in addition to known lines. The symmetry of the phonon modes associated with the indirect transitions as well as with Raman scattering is discussed.

  20. Large excitonic effects in group-IV sulfide monolayers

    NASA Astrophysics Data System (ADS)

    Tuttle, Blair R.; Alhassan, Saeed M.; Pantelides, Sokrates T.

    2015-12-01

    Large exciton binding energies are a distinguishing feature of two-dimensional semiconductors because of reduced screening, potentially leading to unique optoelectronic applications. Here we use electronic structure methods to calculate the properties of a two-dimensional material class: group-IV monosulfides including SiS, GeS, and SnS. Bulk SiS is predicted to be a metastable layered material. Quasiparticle excitations are calculated with the G0W0 method and the Bethe-Salpeter equation is are used to include electron-hole interactions. For monolayers, strongly bound excitons are found below the quasiparticle absorption edge. The predicted excitonic binding energies are as high as 0.7 eV. Due to large excitonic effects, these group-IV sulfide monolayers have great potential for nanoscale optoelectronic applications.

  1. Exact-diagonalization study of exciton condensation in electron bilayers

    NASA Astrophysics Data System (ADS)

    Kaneko, T.; Ejima, S.; Fehske, H.; Ohta, Y.

    2013-07-01

    We report on small-cluster exact-diagonalization calculations which prove the formation of electron-hole pairs (excitons) as a prerequisite for spontaneous interlayer phase coherence in double-layer systems described by the extended Falicov-Kimball model. Evaluating the anomalous Green's function and momentum distribution function of the pairs, and thereby analyzing the dependence of the exciton binding energy, condensation amplitude, and coherence length on the Coulomb interaction strength, we demonstrate a crossover between a BCS-like electron-hole pairing transition and a Bose-Einstein condensation of tightly bound preformed excitons. We furthermore show that a mass imbalance between electrons and holes tends to suppress the condensation of excitons.

  2. Quenching methods for background reduction in luminescence-based probe-target binding assays

    DOEpatents

    Cai, Hong; Goodwin, Peter M; Keller, Richard A.; Nolan, Rhiannon L.

    2007-04-10

    Background luminescence is reduced from a solution containing unbound luminescent probes, each having a first molecule that attaches to a target molecule and having an attached luminescent moiety, and luminescent probe/target adducts. Quenching capture reagent molecules are formed that are capable of forming an adduct with the unbound luminescent probes and having an attached quencher material effective to quench luminescence of the luminescent moiety. The quencher material of the capture reagent molecules is added to a solution of the luminescent probe/target adducts and binds in a proximity to the luminescent moiety of the unbound luminescent probes to quench luminescence from the luminescent moiety when the luminescent moiety is exposed to exciting illumination. The quencher capture reagent does not bind to probe molecules that are bound to target molecules and the probe/target adduct emission is not quenched.

  3. Red luminescence of CsI crystals

    SciTech Connect

    Smol`skaya, L.P.; Kolesnikova, T.A.

    1995-12-01

    Emission in the red spectral range with the maximum at 670 nm and two decay components <5 ns and 1 {mu}s is found in the cathodoluminescence of CsI crystals excited by a pulsed electron beam with the 5-ns duration. The short component is assigned to the ultrafast luminescence caused by the transitions within the valence band. It is assumed that the microsecond component of the red luminescence is caused by the radiative exciton annihilation at the unstable defects produced by ionizing radiation. 8 refs., 1 fig.

  4. Charge transfer state versus hot exciton dissociation in polymer-fullerene blended solar cells.

    PubMed

    Lee, Jiye; Vandewal, Koen; Yost, Shane R; Bahlke, Matthias E; Goris, Ludwig; Baldo, Marc A; Manca, Jean V; Van Voorhis, Troy

    2010-09-01

    We examine the significance of hot exciton dissociation in two archetypical polymer-fullerene blend solar cells. Rather than evolving through a bound charge transfer state, hot processes are proposed to convert excitons directly into free charges. But we find that the internal quantum yields of carrier photogeneration are similar for both excitons and direct excitation of charge transfer states. The internal quantum yield, together with the temperature dependence of the current-voltage characteristics, is consistent with negligible impact from hot exciton dissociation.

  5. Luminescence of GaN nanocolumns obtained by photon-assisted anodic etching

    NASA Astrophysics Data System (ADS)

    Tiginyanu, I. M.; Ursaki, V. V.; Zalamai, V. V.; Langa, S.; Hubbard, S.; Pavlidis, D.; Föll, H.

    2003-08-01

    GaN nanocolumns with transverse dimensions of about 50 nm were obtained by illumination-assisted anodic etching of epilayers grown by metalorganic chemical vapor deposition on sapphire substrates. The photoluminescence spectroscopy characterization shows that the as-grown bulk GaN layers suffer from compressive biaxial strain of 0.5 GPa. The majority of nanocolumns are fully relaxed from strain, and the room-temperature luminescence is free excitonic. The high quality of the columnar nanostructures evidenced by the enhanced intensity of the exciton luminescence and by the decrease of the yellow luminescence is explained by the peculiarities of the anodic etching processing.

  6. Energy and Information Transfer Via Coherent Exciton Wave Packets

    NASA Astrophysics Data System (ADS)

    Zang, Xiaoning

    Electronic excitons are bound electron-hole states that are generated when light interacts with matter. Such excitations typically entangle with phonons and rapidly decohere; the resulting electronic state dynamics become diffusive as a result. However, if the exciton-phonon coupling can be reduced, it may be possible to construct excitonic wave packets that offer a means of efficiently transmitting information and energy. This thesis is a combined theory/computation investigation to design condensed matter systems which support the requisite coherent transport. Under the idealizing assumption that exciton-phonon entanglement could be completely suppressed, the majority of this thesis focuses on the creation and manipulation of exciton wave packets in quasi-one-dimensional systems. While each site could be a silicon quantum dot, the actual implementation focused on organic molecular assemblies for the sake of computational simplicity, ease of experimental implementation, potential for coherent transport, and promise because of reduced structural uncertainty. A laser design was derived to create exciton wave packets with tunable shape and speed. Quantum interference was then exploited to manipulate these packets to block, pass, and even dissociate excitons based on their energies. These developments allow exciton packets to be considered within the arena of quantum information science. The concept of controllable excitonic wave packets was subsequently extended to consider molecular designs that allow photons with orbital angular momentum to be absorbed to create excitons with a quasi-angular momentum of their own. It was shown that a well-defined measure of topological charge is conserved in such light-matter interactions. Significantly, it was also discovered that such molecules allow photon angular momenta to be combined and later emitted. This amounts to a new way of up/down converting photonic angular momentum without relying on nonlinear optical materials. The

  7. Indirect excitons in hydrogen-doped ZnO

    NASA Astrophysics Data System (ADS)

    Zhu, Liangchen; Lem, Laurent L. C.; Nguyen, Thien-Phap; Fair, Kit; Ali, Sajid; Ford, Michael J.; Phillips, Matthew R.; Ton-That, Cuong

    2017-03-01

    We present a correlative experimental and theoretical study of bound excitons in hydrogen-doped ZnO, with a particular focus on the dynamics of their metastable state confined in the sub-surface region, using a combination of surface-sensitive characterisation techniques and density functional theory calculations. A metastable sub-surface emission at 3.31 eV found in H-doped ZnO is attributed to the radiative recombination of indirect excitons localised at basal plane stacking faults (BSFs) where the excitonic transition involves electrons bound to bond-centre hydrogen donors in the potential well of the BSF. Additionally, our work shows the electrical transport of ZnO Schottky junctions is dominated by electrons confined at BSFs in the near-surface region.

  8. 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

  9. Machine learning exciton dynamics

    SciTech Connect

    Häse, Florian; Valleau, Stéphanie; Pyzer-Knapp, Edward; Aspuru-Guzik, Alán

    2016-04-01

    Obtaining the exciton dynamics of large photosynthetic complexes by using mixed quantum mechanics/molecular mechanics (QM/MM) is computationally demanding. We propose a machine learning technique, multi-layer perceptrons, as a tool to reduce the time required to compute excited state energies. With this approach we predict time-dependent density functional theory (TDDFT) excited state energies of bacteriochlorophylls in the Fenna–Matthews–Olson (FMO) complex. Additionally we compute spectral densities and exciton populations from the predictions. Different methods to determine multi-layer perceptron training sets are introduced, leading to several initial data selections. In addition, we compute spectral densities and exciton populations. Once multi-layer perceptrons are trained, predicting excited state energies was found to be significantly faster than the corresponding QM/MM calculations. We showed that multi-layer perceptrons can successfully reproduce the energies of QM/MM calculations to a high degree of accuracy with prediction errors contained within 0.01 eV (0.5%). Spectral densities and exciton dynamics are also in agreement with the TDDFT results. The acceleration and accurate prediction of dynamics strongly encourage the combination of machine learning techniques with ab initio methods.

  10. Role of strain on the coherent properties of GaAs excitons and biexcitons

    NASA Astrophysics Data System (ADS)

    Wilmer, Brian L.; Webber, Daniel; Ashley, Joseph M.; Hall, Kimberley C.; Bristow, Alan D.

    2016-08-01

    Polarization-dependent two-dimensional Fourier-transform spectroscopy (2DFTS) is performed on excitons in strained bulk GaAs layers, probing the coherent response for differing amounts of strain. Uniaxial tensile strain lifts the degeneracy of heavy-hole (HH) and light-hole (LH) valence states, leading to an observed splitting of the associated excitons at low temperature. Increasing the strain increases the magnitude of the HH/LH exciton peak splitting, induces an asymmetry in the off-diagonal interaction coherences, increases the difference in the HH and LH exciton homogenous linewidths, and increases the inhomogeneous broadening of both exciton species. All results arise from strain-induced variations in the local electronic environment, which is not uniform along the growth direction of the thin layers. For cross-linear polarized excitation, wherein excitonic signals give way to biexcitonic signals, the high-strain sample shows evidence of bound LH, HH, and mixed biexcitons.

  11. Dielectric screening of excitons and trions in single-layer MoS2.

    PubMed

    Lin, Yuxuan; Ling, Xi; Yu, Lili; Huang, Shengxi; Hsu, Allen L; Lee, Yi-Hsien; Kong, Jing; Dresselhaus, Mildred S; Palacios, Tomás

    2014-10-08

    Photoluminescence (PL) properties of single-layer MoS2 are indicated to have strong correlations with the surrounding dielectric environment. Blue shifts of up to 40 meV of exciton or trion PL peaks were observed as a function of the dielectric constant of the environment. These results can be explained by the dielectric screening effect of the Coulomb potential; based on this, a scaling relationship was developed with the extracted electronic band gap and exciton and trion binding energies in good agreement with theoretical estimations. It was also observed that the trion/exciton intensity ratio can be tuned by at least 1 order of magnitude with different dielectric environments. Our findings are helpful to better understand the tightly bound exciton properties in strongly quantum-confined systems and provide a simple approach to the selective and separate generation of excitons or trions with potential applications in excitonic interconnects and valleytronics.

  12. Interlayer exciton optoelectronics in a 2D heterostructure p–n junction

    SciTech Connect

    Ross, Jason S.; Rivera, Pasqual; Schaibley, John; Lee-Wong, Eric; Yu, Hongyi; Taniguchi, Takashi; Watanabe, Kenji; Yan, Jiaqiang; Mandrus, David; Cobden, David; Yao, Wang; Xu, Xiaodong

    2016-12-22

    Semiconductor heterostructures are backbones for solid-state-based optoelectronic devices. Recent advances in assembly techniques for van der Waals heterostructures have enabled the band engineering of semiconductor heterojunctions for atomically thin optoelectronic devices. In two-dimensional heterostructures with type II band alignment, interlayer excitons, where Coulomb bound electrons and holes are confined to opposite layers, have shown promising properties for novel excitonic devices, including a large binding energy, micron-scale in-plane drift-diffusion, and a long population and valley polarization lifetime. Here, we demonstrate interlayer exciton optoelectronics based on electrostatically defined lateral p–n junctions in a MoSe2–WSe2 heterobilayer. Applying a forward bias enables the first observation of electroluminescence from interlayer excitons. At zero bias, the p–n junction functions as a highly sensitive photodetector, where the wavelength-dependent photocurrent measurement allows the direct observation of resonant optical excitation of the interlayer exciton. The resulting photocurrent amplitude from the interlayer exciton is about 200 times smaller than the resonant excitation of intralayer exciton. This implies that the interlayer exciton oscillator strength is 2 orders of magnitude smaller than that of the intralayer exciton due to the spatial separation of electron and hole to the opposite layers. Lastly, these results lay the foundation for exploiting the interlayer exciton in future 2D heterostructure optoelectronic devices.

  13. Enabling valley selective exciton scattering in monolayer WSe2 through upconversion

    PubMed Central

    Manca, M.; Glazov, M. M.; Robert, C.; Cadiz, F.; Taniguchi, T.; Watanabe, K.; Courtade, E.; Amand, T.; Renucci, P.; Marie, X.; Wang, G.; Urbaszek, B.

    2017-01-01

    Excitons, Coulomb bound electron–hole pairs, are composite bosons and their interactions in traditional semiconductors lead to condensation and light amplification. The much stronger Coulomb interaction in transition metal dichalcogenides such as WSe2 monolayers combined with the presence of the valley degree of freedom is expected to provide new opportunities for controlling excitonic effects. But so far the bosonic character of exciton scattering processes remains largely unexplored in these two-dimensional materials. Here we show that scattering between B-excitons and A-excitons preferably happens within the same valley in momentum space. This leads to power dependent, negative polarization of the hot B-exciton emission. We use a selective upconversion technique for efficient generation of B-excitons in the presence of resonantly excited A-excitons at lower energy; we also observe the excited A-excitons state 2s. Detuning of the continuous wave, low-power laser excitation outside the A-exciton resonance (with a full width at half maximum of 4 meV) results in vanishing upconversion signal. PMID:28367962

  14. Interlayer Exciton Optoelectronics in a 2D Heterostructure p–n Junction

    NASA Astrophysics Data System (ADS)

    Ross, Jason S.; Rivera, Pasqual; Schaibley, John; Lee-Wong, Eric; Yu, Hongyi; Taniguchi, Takashi; Watanabe, Kenji; Yan, Jiaqiang; Mandrus, David; Cobden, David; Yao, Wang; Xu, Xiaodong

    2017-02-01

    Semiconductor heterostructures are backbones for solid state based optoelectronic devices. Recent advances in assembly techniques for van der Waals heterostructures has enabled the band engineering of semiconductor heterojunctions for atomically thin optoelectronic devices. In two-dimensional heterostructures with type II band alignment, interlayer excitons, where Coulomb-bound electrons and holes are confined to opposite layers, have shown promising properties for novel excitonic devices, including a large binding energy, micron-scale in-plane drift-diffusion, and long population and valley polarization lifetime. Here, we demonstrate interlayer exciton optoelectronics based on electrostatically defined lateral p-n junctions in a MoSe2-WSe2 heterobilayer. Applying a forward bias enables the first observation of electroluminescence from interlayer excitons. At zero bias, the p-n junction functions as a highly sensitive photodetector, where the wavelength-dependent photocurrent measurement allows the direct observation of resonant optical excitation of the interlayer exciton. The resulting photocurrent amplitude from the interlayer exciton is about 200 times smaller compared to the resonant excitation of intralayer exciton. This implies that the interlayer exciton oscillator strength is two orders of magnitude smaller than that of the intralayer exciton due to the spatial separation of electron and hole to opposite layers. These results lay the foundation for exploiting the interlayer exciton in future 2D heterostructure optoelectronic devices.

  15. Enabling valley selective exciton scattering in monolayer WSe2 through upconversion

    NASA Astrophysics Data System (ADS)

    Manca, M.; Glazov, M. M.; Robert, C.; Cadiz, F.; Taniguchi, T.; Watanabe, K.; Courtade, E.; Amand, T.; Renucci, P.; Marie, X.; Wang, G.; Urbaszek, B.

    2017-04-01

    Excitons, Coulomb bound electron-hole pairs, are composite bosons and their interactions in traditional semiconductors lead to condensation and light amplification. The much stronger Coulomb interaction in transition metal dichalcogenides such as WSe2 monolayers combined with the presence of the valley degree of freedom is expected to provide new opportunities for controlling excitonic effects. But so far the bosonic character of exciton scattering processes remains largely unexplored in these two-dimensional materials. Here we show that scattering between B-excitons and A-excitons preferably happens within the same valley in momentum space. This leads to power dependent, negative polarization of the hot B-exciton emission. We use a selective upconversion technique for efficient generation of B-excitons in the presence of resonantly excited A-excitons at lower energy; we also observe the excited A-excitons state 2s. Detuning of the continuous wave, low-power laser excitation outside the A-exciton resonance (with a full width at half maximum of 4 meV) results in vanishing upconversion signal.

  16. Interlayer exciton optoelectronics in a 2D heterostructure p–n junction

    DOE PAGES

    Ross, Jason S.; Rivera, Pasqual; Schaibley, John; ...

    2016-12-22

    Semiconductor heterostructures are backbones for solid-state-based optoelectronic devices. Recent advances in assembly techniques for van der Waals heterostructures have enabled the band engineering of semiconductor heterojunctions for atomically thin optoelectronic devices. In two-dimensional heterostructures with type II band alignment, interlayer excitons, where Coulomb bound electrons and holes are confined to opposite layers, have shown promising properties for novel excitonic devices, including a large binding energy, micron-scale in-plane drift-diffusion, and a long population and valley polarization lifetime. Here, we demonstrate interlayer exciton optoelectronics based on electrostatically defined lateral p–n junctions in a MoSe2–WSe2 heterobilayer. Applying a forward bias enables the firstmore » observation of electroluminescence from interlayer excitons. At zero bias, the p–n junction functions as a highly sensitive photodetector, where the wavelength-dependent photocurrent measurement allows the direct observation of resonant optical excitation of the interlayer exciton. The resulting photocurrent amplitude from the interlayer exciton is about 200 times smaller than the resonant excitation of intralayer exciton. This implies that the interlayer exciton oscillator strength is 2 orders of magnitude smaller than that of the intralayer exciton due to the spatial separation of electron and hole to the opposite layers. Lastly, these results lay the foundation for exploiting the interlayer exciton in future 2D heterostructure optoelectronic devices.« less

  17. Interlayer Exciton Optoelectronics in a 2D Heterostructure p-n Junction.

    PubMed

    Ross, Jason S; Rivera, Pasqual; Schaibley, John; Lee-Wong, Eric; Yu, Hongyi; Taniguchi, Takashi; Watanabe, Kenji; Yan, Jiaqiang; Mandrus, David; Cobden, David; Yao, Wang; Xu, Xiaodong

    2017-02-08

    Semiconductor heterostructures are backbones for solid-state-based optoelectronic devices. Recent advances in assembly techniques for van der Waals heterostructures have enabled the band engineering of semiconductor heterojunctions for atomically thin optoelectronic devices. In two-dimensional heterostructures with type II band alignment, interlayer excitons, where Coulomb bound electrons and holes are confined to opposite layers, have shown promising properties for novel excitonic devices, including a large binding energy, micron-scale in-plane drift-diffusion, and a long population and valley polarization lifetime. Here, we demonstrate interlayer exciton optoelectronics based on electrostatically defined lateral p-n junctions in a MoSe2-WSe2 heterobilayer. Applying a forward bias enables the first observation of electroluminescence from interlayer excitons. At zero bias, the p-n junction functions as a highly sensitive photodetector, where the wavelength-dependent photocurrent measurement allows the direct observation of resonant optical excitation of the interlayer exciton. The resulting photocurrent amplitude from the interlayer exciton is about 200 times smaller than the resonant excitation of intralayer exciton. This implies that the interlayer exciton oscillator strength is 2 orders of magnitude smaller than that of the intralayer exciton due to the spatial separation of electron and hole to the opposite layers. These results lay the foundation for exploiting the interlayer exciton in future 2D heterostructure optoelectronic devices.

  18. Enabling valley selective exciton scattering in monolayer WSe2 through upconversion.

    PubMed

    Manca, M; Glazov, M M; Robert, C; Cadiz, F; Taniguchi, T; Watanabe, K; Courtade, E; Amand, T; Renucci, P; Marie, X; Wang, G; Urbaszek, B

    2017-04-03

    Excitons, Coulomb bound electron-hole pairs, are composite bosons and their interactions in traditional semiconductors lead to condensation and light amplification. The much stronger Coulomb interaction in transition metal dichalcogenides such as WSe2 monolayers combined with the presence of the valley degree of freedom is expected to provide new opportunities for controlling excitonic effects. But so far the bosonic character of exciton scattering processes remains largely unexplored in these two-dimensional materials. Here we show that scattering between B-excitons and A-excitons preferably happens within the same valley in momentum space. This leads to power dependent, negative polarization of the hot B-exciton emission. We use a selective upconversion technique for efficient generation of B-excitons in the presence of resonantly excited A-excitons at lower energy; we also observe the excited A-excitons state 2s. Detuning of the continuous wave, low-power laser excitation outside the A-exciton resonance (with a full width at half maximum of 4 meV) results in vanishing upconversion signal.

  19. 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

  20. Quantum Hall drag of exciton condensate in graphene

    NASA Astrophysics Data System (ADS)

    Liu, Xiaomeng; Watanabe, Kenji; Taniguchi, Takashi; Halperin, Bertrand I.; Kim, Philip

    2017-08-01

    An exciton condensate is a Bose-Einstein condensate of electron and hole pairs bound by the Coulomb interaction. In an electronic double layer (EDL) subject to strong magnetic fields, filled Landau states in one layer bind with empty states of the other layer to form an exciton condensate. Here we report exciton condensation in a bilayer graphene EDL separated by hexagonal boron nitride. Driving current in one graphene layer generates a near-quantized Hall voltage in the other layer, resulting in coherent exciton transport. Owing to the strong Coulomb coupling across the atomically thin dielectric, quantum Hall drag in graphene appears at a temperature ten times higher than previously observed in a GaAs EDL. The wide-range tunability of densities and displacement fields enables exploration of a rich phase diagram of Bose-Einstein condensates across Landau levels with different filling factors and internal quantum degrees of freedom. The observed robust exciton condensation opens up opportunities to investigate various many-body exciton phases.

  1. Probing the origin of excitonic states in monolayer WSe2

    PubMed Central

    Huang, Jiani; Hoang, Thang B.; Mikkelsen, Maiken H.

    2016-01-01

    Two-dimensional transition metal dichalcogenides (TMDCs) have spurred excitement for potential applications in optoelectronic and valleytronic devices; however, the origin of the dynamics of excitons, trions, and other localized states in these low dimensional materials is not well-understood. Here, we experimentally probed the dynamics of excitonic states in monolayer WSe2 by investigating the temperature and polarization dependent photoluminescence (PL) spectra. Four pronounced PL peaks were identified below a temperature of 60 K at near-resonant excitation and assigned to exciton, trion and localized states from excitation power dependence measurements. We find that the localized states vanish above 65 K, while exciton and trion emission peaks remain up to room temperature. This can be explained by a multi-level model developed for conventional semiconductors and applied to monolayer TMDCs for the first time here. From this model, we estimated a lower bound of the exciton binding energy of 198 meV for monolayer WSe2 and explained the vanishing of the localized states. Additionally, we observed a rapid decrease in the degree of circular polarization of the PL at increasing temperatures indicating a relatively strong electron-phonon coupling and impurity-related scattering. Our results reveal further insight into the excitonic states in monolayer WSe2 which is critical for future practical applications. PMID:26940069

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

    PubMed

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

    2014-09-11

    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

  3. Valley excitons in two-dimensional semiconductors

    DOE PAGES

    Yu, Hongyi; Cui, Xiaodong; Xu, Xiaodong; ...

    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

  4. 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.

  5. Study of Luminescence Characteristics of Trivalent Terbium in Silicate Glass

    NASA Technical Reports Server (NTRS)

    West, Mike S.; Armagan, Guzin; Winfree, William P.

    1995-01-01

    An important use of silicate glasses doped with terbium oxide (Tb2O3) is their use as fiber optic sensors for high-resolution imaging applications requiring the detection of x-rays (e.g. tomography and radiography). The x-ray radiation is absorbed by the glass, producing electron-hole pairs (excitons). The excitons migrate through the glass matrix and then recombine, emitting characteristic Tb(3+) luminescence in the optical wavelength region. This emission is due to forbidden transitions of 4f electrons and therefore has a long decay time. Long decay time is undesirable when imaging transient events since it results in blurring in time of the images. It has been reported elsewhere that in crystals Tb(3+) ions can act both as luminescence centers and as fluorescence traps. These traps can capture excitons and delay their recombination. This delayed fluorescence is seen as a long lived, secondary component to the luminescence decay curve, or afterglow. Such a secondary decay component to the luminescence decay of Tb(3+) has been observed before in soda glass following pulsed optical excitation. In order to determine the conditions under which afterglow occurs, an understanding of the material's luminescent properties is required.

  6. Study of Luminescence Characteristics of Trivalent Terbium in Silicate Glass

    NASA Technical Reports Server (NTRS)

    West, Mike S.; Armagan, Guzin; Winfree, William P.

    1995-01-01

    An important use of silicate glasses doped with terbium oxide (Tb2O3) is their use as fiber optic sensors for high-resolution imaging applications requiring the detection of x-rays (e.g. tomography and radiography). The x-ray radiation is absorbed by the glass, producing electron-hole pairs (excitons). The excitons migrate through the glass matrix and then recombine, emitting characteristic Tb(3+) luminescence in the optical wavelength region. This emission is due to forbidden transitions of 4f electrons and therefore has a long decay time. Long decay time is undesirable when imaging transient events since it results in blurring in time of the images. It has been reported elsewhere that in crystals Tb(3+) ions can act both as luminescence centers and as fluorescence traps. These traps can capture excitons and delay their recombination. This delayed fluorescence is seen as a long lived, secondary component to the luminescence decay curve, or afterglow. Such a secondary decay component to the luminescence decay of Tb(3+) has been observed before in soda glass following pulsed optical excitation. In order to determine the conditions under which afterglow occurs, an understanding of the material's luminescent properties is required.

  7. 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

  8. Ultrafast Mid-Infrared Intra-Excitonic Response of Individualized Single-Walled Carbon Nanotubes

    SciTech Connect

    Wang, Jigang; Graham, Matt W.; Ma, Yingzhong; Fleming, Graham R.; Kaindl, Robert A.

    2009-06-29

    The quasi-1D confinement and reduced screening of photoexcited charges in single-walled carbon nanotubes (SWNTs) entails strongly-enhanced Coulomb interactions and exciton binding energies. Such amplified electron-hole (e-h) correlations have important implications for both fundamental physics and optoelectronic applications of nanotubes. The availability of"individualized" SWNT ensembles with bright and structured luminescence has rendered specific tube chiralities experimentally accessible. In these samples, evidence for excitonic behavior was found in absorption-luminescence maps, two-photon excited luminescence, or ultrafast carrier dynamics. Here, we report ultrafast mid-infrared (mid-IR) studies of individualized SWNTs, evidencing strong photoinduced absorption around 200 meV in semiconducting tubes of (6,5) and (7,5) chiralities. This manifests the observation of quasi-1D intra-excitonic transitions between different relative-momentum states, in agreement with the binding energy and calculated oscillator strength. Our measurements further reveal a saturation of the photoinduced absorption with increasing phase-space filling of the correlated e-h pairs. The transient mid-IR response represents a new tool, unhindered by restrictions of momentum or interband dipole moment, to investigate the density and dynamics of SWNT excitons.

  9. Exciton absorption of entangled photons in semiconductor quantum wells

    NASA Astrophysics Data System (ADS)

    Rodriguez, Ferney; Guzman, David; Salazar, Luis; Quiroga, Luis; Condensed Matter Physics Group Team

    2013-03-01

    The dependence of the excitonic two-photon absorption on the quantum correlations (entanglement) of exciting biphotons by a semiconductor quantum well is studied. We show that entangled photon absorption can display very unusual features depending on space-time-polarization biphoton parameters and absorber density of states for both bound exciton states as well as for unbound electron-hole pairs. We report on the connection between biphoton entanglement, as quantified by the Schmidt number, and absorption by a semiconductor quantum well. Comparison between frequency-anti-correlated, unentangled and frequency-correlated biphoton absorption is addressed. We found that exciton oscillator strengths are highly increased when photons arrive almost simultaneously in an entangled state. Two-photon-absorption becomes a highly sensitive probe of photon quantum correlations when narrow semiconductor quantum wells are used as two-photon absorbers. Research funds from Facultad de Ciencias, Universidad de los Andes

  10. Magnetic Proximity Effects in Transition-Metal Dichalcogenides: Converting Excitons

    NASA Astrophysics Data System (ADS)

    Scharf, Benedikt; Xu, Gaofeng; Matos-Abiague, Alex; Žutić, Igor

    2017-09-01

    The two-dimensional character and reduced screening in monolayer transition-metal dichalcogenides (TMDs) lead to the ubiquitous formation of robust excitons with binding energies orders of magnitude larger than in bulk semiconductors. Focusing on neutral excitons, bound electron-hole pairs that dominate the optical response in TMDs, it is shown that they can provide fingerprints for magnetic proximity effects in magnetic heterostructures. These proximity effects cannot be described by the widely used single-particle description but instead reveal the possibility of a conversion between optically inactive and active excitons by rotating the magnetization of the magnetic substrate. With recent breakthroughs in fabricating Mo- and W-based magnetic TMD heterostructures, this emergent optical response can be directly tested experimentally.

  11. Long-range exciton dissociation in organic solar cells.

    PubMed

    Caruso, Domenico; Troisi, Alessandro

    2012-08-21

    It is normally assumed that electrons and holes in organic solar cells are generated by the dissociation of excitons at the interface between donor and acceptor materials in strongly bound hole-electron pairs. We show in this contribution that excitons can dissociate tens of angstroms away from the interface and generate partially separated electrons and holes, which can more easily overcome their coulombic attraction and form free charges. We first establish under what conditions long-range exciton dissociation is likely (using a kinetic model and a microscopic model for the calculation of the long-range electron transfer rate). Then, defining a rather general model Hamiltonian for the donor material, we show that the phenomenon is extremely common in the majority of polymer:fullerene bulk heterojunction solar cells.

  12. The luminescence of BaF{sub 2} nanoparticles upon high-energy excitation

    SciTech Connect

    Vistovskyy, V. V. Zhyshkovych, A. V.; Halyatkin, O. O.; Voloshinovskii, A. S.; Mitina, N. E.; Zaichenko, A. S.; Rodnyi, P. A.; Vasil'ev, A. N.; Gektin, A. V.

    2014-08-07

    The dependence of X-ray excited luminescence intensity on BaF{sub 2} nanoparticle size was studied. A sharp decrease of self-trapped exciton luminescence intensity was observed when the nanoparticle size is less than 80 nm. The main mechanism of the luminescence quenching is caused by the escape of electrons from the nanoparticles. Escape of electrons from nanoparticles is confirmed by the considerable increase of luminescence intensity of the polystyrene scintillator with embedded BaF{sub 2} nanoparticles comparing with pure polystyrene scintillator.

  13. Controlling exciton photophysics in single-walled carbon nanotubes

    NASA Astrophysics Data System (ADS)

    Sarpkaya, Ibrahim

    Single-walled carbon nanotubes (SWCNTs) have been studied extensively by scientists and engineers due to their unique mechanical, optical, electronic and thermal properties that make them attractive for both fundamental research and device applications. Specifically, important optical properties of SWCNTs such as formation of strongly bound excitons (electron-hole pairs), being stable at room temperature, and bandgap-tunable light emission from visible to telecom wavelengths make them a promising material for optoelectronic and nanophotonic devices. However, the photophysics of excitons in SWCNTs is not yet fully understood and is largely affected by detrimental extrinsic effects, which give rise to strongly reduced device performance. This dissertation demonstrates novel methods and techniques to better understand and to control the photophysics of excitons in SWCNTs. The first part presents novel ways to completely remove detrimental spectral diffusion and blinking in the optical emission of surfactant dispersed SWCNTs on millisecond time scales and also demonstrates 50-fold enhanced exciton emission. Furthermore, pronounced photon antibunching is observed for the first time under resonant excitation. The demonstrated single photon emission is promising for applications in quantum cryptography, while the achieved stable long term emission is important for optoelectronic devices. The second part demonstrates a new regime of intrinsic exciton photophysics in ultra-clean SWCNTs that is characterized by ultra-narrow exciton linewidth and prolonged emission times up to 18 ns. These lifetimes are two orders of magnitude better than prior measurements and in agreement with values predicted by theorists a decade ago. Moreover, I measure for the first time exciton decoherence times of individual nanotubes in the time-domain and demonstrate fourfold prolonged values up to 2 ps compared to previous ensemble studies. Finally, I demonstrate a novel method which controls

  14. Excitons versus free charges in organo-lead tri-halide perovskites

    NASA Astrophysics Data System (ADS)

    D'Innocenzo, Valerio; Grancini, Giulia; Alcocer, Marcelo J. P.; Kandada, Ajay Ram Srimath; Stranks, Samuel D.; Lee, Michael M.; Lanzani, Guglielmo; Snaith, Henry J.; Petrozza, Annamaria

    2014-04-01

    Excitonic solar cells, within which bound electron-hole pairs have a central role in energy harvesting, have represented a hot field of research over the last two decades due to the compelling prospect of low-cost solar energy. However, in such cells, exciton dissociation and charge collection occur with significant losses in energy, essentially due to poor charge screening. Organic-inorganic perovskites show promise for overcoming such limitations. Here, we use optical spectroscopy to estimate the exciton binding energy in the mixed-halide crystal to be in the range of 50 meV. We show that such a value is consistent with almost full ionization of the exciton population under photovoltaic cell operating conditions. However, increasing the total photoexcitation density, excitonic species become dominant, widening the perspective of this material for a host of optoelectronic applications.

  15. Excitons versus free charges in organo-lead tri-halide perovskites.

    PubMed

    D'Innocenzo, Valerio; Grancini, Giulia; Alcocer, Marcelo J P; Kandada, Ajay Ram Srimath; Stranks, Samuel D; Lee, Michael M; Lanzani, Guglielmo; Snaith, Henry J; Petrozza, Annamaria

    2014-04-08

    Excitonic solar cells, within which bound electron-hole pairs have a central role in energy harvesting, have represented a hot field of research over the last two decades due to the compelling prospect of low-cost solar energy. However, in such cells, exciton dissociation and charge collection occur with significant losses in energy, essentially due to poor charge screening. Organic-inorganic perovskites show promise for overcoming such limitations. Here, we use optical spectroscopy to estimate the exciton binding energy in the mixed-halide crystal to be in the range of 50 meV. We show that such a value is consistent with almost full ionization of the exciton population under photovoltaic cell operating conditions. However, increasing the total photoexcitation density, excitonic species become dominant, widening the perspective of this material for a host of optoelectronic applications.

  16. Evidence of harvesting electricity by exciton recombination in an n-n type solar cell.

    PubMed

    Song, Qun Liang; Yang, Hong Bin; Gan, Ye; Gong, Cheng; Ming Li, Chang

    2010-04-07

    Free electrons and holes bounded by weak interactions in organic molecules must be generated from excitons to produce photocurrent in organic solar cells. Free charge carriers, in either small molecule- or polymer-based solar cells, are generated so far by dissociation of excitons at the donor-acceptor interface through injecting electrons (holes) from a donor (acceptor) into an acceptor (donor) while leaving holes (electrons) in the donor (acceptor). Here we report a new way, intermolecular exciton recombination, to generate free carriers from organic semiconductors. Unlike the exciton dissociation between donor and acceptor, the recombination of electrons from perfluorinated hexadecafluorophthalo-cyaninatozinc (F16ZnPc) with holes from fullerene (C(60)) frees their counterpart carriers. A new organic solar cell based on this intermolecular exciton recombination at the interface is fabricated to clearly demonstrate this new way to produce free carriers and then harvest electricity from sunlight.

  17. Reconfigurable exciton-plasmon interconversion for nanophotonic circuits

    NASA Astrophysics Data System (ADS)

    Lee, Hyun Seok; Luong, Dinh Hoa; Kim, Min Su; Jin, Youngjo; Kim, Hyun; Yun, Seokjoon; Lee, Young Hee

    2016-11-01

    The recent challenges for improving the operation speed of nanoelectronics have motivated research on manipulating light in on-chip integrated circuits. Hybrid plasmonic waveguides with low-dimensional semiconductors, including quantum dots and quantum wells, are a promising platform for realizing sub-diffraction limited optical components. Meanwhile, two-dimensional transition metal dichalcogenides (TMDs) have received broad interest in optoelectronics owing to tightly bound excitons at room temperature, strong light-matter and exciton-plasmon interactions, available top-down wafer-scale integration, and band-gap tunability. Here, we demonstrate principal functionalities for on-chip optical communications via reconfigurable exciton-plasmon interconversions in ~200-nm-diameter Ag-nanowires overlapping onto TMD transistors. By varying device configurations for each operation purpose, three active components for optical communications are realized: field-effect exciton transistors with a channel length of ~32 μm, field-effect exciton multiplexers transmitting multiple signals through a single NW and electrical detectors of propagating plasmons with a high On/Off ratio of~190. Our results illustrate the unique merits of two-dimensional semiconductors for constructing reconfigurable device architectures in integrated nanophotonic circuits.

  18. Reconfigurable exciton-plasmon interconversion for nanophotonic circuits.

    PubMed

    Lee, Hyun Seok; Luong, Dinh Hoa; Kim, Min Su; Jin, Youngjo; Kim, Hyun; Yun, Seokjoon; Lee, Young Hee

    2016-11-28

    The recent challenges for improving the operation speed of nanoelectronics have motivated research on manipulating light in on-chip integrated circuits. Hybrid plasmonic waveguides with low-dimensional semiconductors, including quantum dots and quantum wells, are a promising platform for realizing sub-diffraction limited optical components. Meanwhile, two-dimensional transition metal dichalcogenides (TMDs) have received broad interest in optoelectronics owing to tightly bound excitons at room temperature, strong light-matter and exciton-plasmon interactions, available top-down wafer-scale integration, and band-gap tunability. Here, we demonstrate principal functionalities for on-chip optical communications via reconfigurable exciton-plasmon interconversions in ∼200-nm-diameter Ag-nanowires overlapping onto TMD transistors. By varying device configurations for each operation purpose, three active components for optical communications are realized: field-effect exciton transistors with a channel length of ∼32 μm, field-effect exciton multiplexers transmitting multiple signals through a single NW and electrical detectors of propagating plasmons with a high On/Off ratio of∼190. Our results illustrate the unique merits of two-dimensional semiconductors for constructing reconfigurable device architectures in integrated nanophotonic circuits.

  19. Reconfigurable exciton-plasmon interconversion for nanophotonic circuits

    PubMed Central

    Lee, Hyun Seok; Luong, Dinh Hoa; Kim, Min Su; Jin, Youngjo; Kim, Hyun; Yun, Seokjoon; Lee, Young Hee

    2016-01-01

    The recent challenges for improving the operation speed of nanoelectronics have motivated research on manipulating light in on-chip integrated circuits. Hybrid plasmonic waveguides with low-dimensional semiconductors, including quantum dots and quantum wells, are a promising platform for realizing sub-diffraction limited optical components. Meanwhile, two-dimensional transition metal dichalcogenides (TMDs) have received broad interest in optoelectronics owing to tightly bound excitons at room temperature, strong light-matter and exciton-plasmon interactions, available top-down wafer-scale integration, and band-gap tunability. Here, we demonstrate principal functionalities for on-chip optical communications via reconfigurable exciton-plasmon interconversions in ∼200-nm-diameter Ag-nanowires overlapping onto TMD transistors. By varying device configurations for each operation purpose, three active components for optical communications are realized: field-effect exciton transistors with a channel length of ∼32 μm, field-effect exciton multiplexers transmitting multiple signals through a single NW and electrical detectors of propagating plasmons with a high On/Off ratio of∼190. Our results illustrate the unique merits of two-dimensional semiconductors for constructing reconfigurable device architectures in integrated nanophotonic circuits. PMID:27892463

  20. Self-trapped exciton configurations in Beryllium Oxide

    NASA Astrophysics Data System (ADS)

    Botov, M. A.; Kuznetsov, A. Yu; Sobolev, A. B.

    2017-05-01

    The modern radiation technology, nuclear engineering, non-linear optics are associated with radiation-resistant optical material study. Evolution of electronic excitations in these materials is a complex multichannel process which currently has no integrated model. A special role belongs to the low-symmetry single crystals, such as beryllium oxide (BeO). We present theoretical results that advance our understanding of exciton-based channel of electronic excitations relaxation. The four possible self-trapped exciton (STE) configurations in beryllia single crystal have been investigated by using a quantum mechanical approach (Hartree-Fock and B3LYP HF-DFT hybrid functional, as implemented in the CRYSTAL09 code). B3LYP DFT functional with 30% of exact exchange was used (B3LYP30). All calculations were performed using periodic boundary conditions and full SC geometry relaxation. The lattice distortion and charge density distribution for considered defect configurations were obtained. STE-A1 luminescence energy was found to be 6.0 eV for HF and 6.5 eV for B3LYP30; STE-A2 luminescence energy was found to be 9.2 eV for HF and 7.8 eV for B3LYP30. STE-B1 luminescence energy was found to be 5.5 eV for HF, 6.2 eV for B3LYP30; STE-B2 luminescence energy was found to be 4.7 eV for HF.

  1. 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

    2015-07-08

    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.

  2. 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

  3. Transient terahertz spectroscopy of excitons and unbound carriers in quasi two-dimensional electron-hole gases

    SciTech Connect

    Kaindl, Robert A.; Hagele, D.; Carnahan, M. A.; Chemla, D. S.

    2008-09-11

    We report a comprehensive experimental study and detailed model analysis of the terahertz (THz) dielectric response and density kinetics of excitons and unbound electron-hole pairs in GaAs quantum wells. A compact expression is given, in absolute units, for the complex-valued THz dielectric function of intra-excitonic transitions between the 1s and higher-energy exciton and continuum levels. It closely describes the THz spectra of resonantly generated excitons. Exciton ionization and formation are further explored, where the THz response exhibits both intra-excitonic and Drude features. Utilizing a two-component dielectric function, we derive the underlying exciton and unbound pair densities. In the ionized state, excellent agreement is found with the Saha thermodynamic equilibrium, which provides experimental verification of the two-component analysis and density scaling. During exciton formation, in turn, the pair kinetics is quantitatively described by a Saha equilibrium that follows the carrier cooling dynamics. The THz-derived kinetics is, moreover, consistent with time-resolved luminescence measured for comparison. Our study establishes a basis for tracking pair densities via transient THz spectroscopy of photoexcited quasi-2D electron-hole gases.

  4. A study of polaritonic transparency in couplers made from excitonic materials

    SciTech Connect

    Singh, Mahi R.; Racknor, Chris

    2015-03-14

    We have studied light matter interaction in quantum dot and exciton-polaritonic coupler hybrid systems. The coupler is made by embedding two slabs of an excitonic material (CdS) into a host excitonic material (ZnO). An ensemble of non-interacting quantum dots is doped in the coupler. The bound exciton polariton states are calculated in the coupler using the transfer matrix method in the presence of the coupling between the external light (photons) and excitons. These bound exciton-polaritons interact with the excitons present in the quantum dots and the coupler is acting as a reservoir. The Schrödinger equation method has been used to calculate the absorption coefficient in quantum dots. It is found that when the distance between two slabs (CdS) is greater than decay length of evanescent waves the absorption spectrum has two peaks and one minimum. The minimum corresponds to a transparent state in the system. However, when the distance between the slabs is smaller than the decay length of evanescent waves, the absorption spectra has three peaks and two transparent states. In other words, one transparent state can be switched to two transparent states when the distance between the two layers is modified. This could be achieved by applying stress and strain fields. It is also found that transparent states can be switched on and off by applying an external control laser field.

  5. Slow light enhanced singlet exciton fission solar cells with a 126% yield of electrons per photon

    SciTech Connect

    Thompson, Nicholas J.; Congreve, Daniel N.; Baldo, Marc A. E-mail: baldo@mit.edu; Goldberg, David; Menon, Vinod M. E-mail: baldo@mit.edu

    2013-12-23

    Singlet exciton fission generates two triplet excitons per absorbed photon. It promises to increase the power extracted from sunlight without increasing the number of photovoltaic junctions in a solar cell. We demonstrate solar cells with an external quantum efficiency of 126% by enhancing absorption in thin films of the singlet exciton fission material pentacene. The device structure exploits the long photon dwell time at the band edge of a distributed Bragg reflector to achieve enhancement over a broad range of angles. Measuring the reflected light from the solar cell establishes a lower bound of 137% for the internal quantum efficiency.

  6. Editorial on indirect excitons: Physics and applications

    NASA Astrophysics Data System (ADS)

    2017-08-01

    This special issue contains 9 original review papers, research papers and discussion papers on indirect excitons. An exciton is a Coulomb-correlated electron-hole pair. Frenkel excitons dominate optical properties of organic semiconductors, while Wannier-Mott excitons are responsible for the hydrogen-like absorption spectra of inorganic semiconductors at low temperatures. The interest to the physics of excitons has strongly increased in the new century. This interest is motivated by unique bosonic properties of excitons that lead to the phenomena of exciton-polariton lasing and stimulated scattering, build-up of the spontaneous coherence and polarisation in cold exciton gases. In addition to the rich fundamental physics, excitons offer the perspective of applications in opto-electronic devices such as exciton transistors, switches, optical integrated circuits, etc.

  7. Final Report, DOE grant DE-FG02-99ER45780, "Indirect Excitons in Coupled Quantum Wells"

    SciTech Connect

    Snoke, david W.

    2014-07-21

    The is the final technical report for this project, which was funded by the DOE from 1999 to 2012. The project focused on experimental studies of spatially indirect excitons in coupled quantum wells, with the aim of understanding the quantum physics of these particles, including such effects as pattern formation due to electron-hole charge separation, the Mott plasma-insulator transition, luminescence up-conversion through field-assisted tunneling, luminescence line shifts due to many-body renormalization and magnetic field effects on tunneling, and proposed effects such as Bose-Einstein condensation of indirect excitons and phase separation of bright and dark indirect excitons. Significant results are summarized here and the relation to other work is discussed.

  8. 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.

  9. Energy Migration in Organic Thin Films--From Excitons to Polarons

    NASA Astrophysics Data System (ADS)

    Mullenbach, Tyler K.

    The rise of organic photovoltaic devices (OPVs) and organic light-emitting devices has generated interest in the physics governing exciton and polaron dynamics in thin films. Energy transfer has been well studied in dilute solutions, but there are emergent properties in thin films and greater complications due to complex morphologies which must be better understood. Despite the intense interest in energy transport in thin films, experimental limitations have slowed discoveries. Here, a new perspective of OPV operation is presented where photovoltage, instead of photocurrent, plays the fundamental role. By exploiting this new vantage point the first method of measuring the diffusion length (LD) of dark (non-luminescent) excitons is developed, a novel photodetector is invented, and the ability to watch exciton arrival, in real-time, at the donor-acceptor heterojunction is presented. Using an enhanced understanding of exciton migration in thin films, paradigms for enhancing LD by molecular modifications are discovered, and the first exciton gate is experimentally and theoretically demonstrated. Generation of polarons from exciton dissociation represents a second phase of energy migration in OPVs that remains understudied. Current approaches are capable of measuring the rate of charge carrier recombination only at open-circuit. To enable a better understanding of polaron dynamics in thin films, two new approaches are presented which are capable of measuring both the charge carrier recombination and transit rates at any OPV operating voltage. These techniques pave the way for a more complete understanding of charge carrier kinetics in molecular thin films.

  10. Luminescence Rings in Quantum Well Structures

    NASA Astrophysics Data System (ADS)

    Denev, S.; Liu, Y.; Snoke, D.; Rapaport, R.; Chen, Gang; Simon, S.; Pfeiffer, L.; West, K.

    2004-03-01

    An unique ring-shaped luminescence pattern with size of hundreds of microns to millimeters has been observed in GaAs-based quantum well structures excited by weak laser light [1]. The ring persists up to high temperatures, and its size can be manipulated by the laser power, electric field, external stress or magnetic field. We give a detailed description of the effect and discuss various proposed explanations including an optical effect, diffusion and excitonic superfluidity. A realistic explanation based on a simple, nonlinear model of charge separation is proposed, and numerical results from the model are compared to the experiment. This work has been supported by the National Science Foundation under grant No. DMR-0102457 and by the Department of Energy under grant No. DE-FG0299ER45780 [1] D. Snoke, S. Denev, Y. Liu, L. Pfeiffer, and K. West, "Long-range Transport in Excitonic Dark States in Coupled Quantum Wells," Nature 418, 754 (2002).

  11. Exciton transfer between localized states in CdS1- xSex alloys: Time-resolved photoluminescence and theoretical models

    NASA Astrophysics Data System (ADS)

    Gourdon, C.; Lavallard, P.

    1990-04-01

    Luminescence decay curves as well as time-resolved and time-integrated spectra obtained with selective excitation in the localized exciton band of CdS1- xSex are fitted using two theoretical models. In the first one, exciton transfer to lower energy states occurs through tunnel effect assisted by acoustical phonons. From the energy dependence of the lifetime measured with quasi-resonant excitation in the localized exciton band, we determine the characteristic energy of the tail density of states: E0 = 2.2 meV. The radiative lifetime is set equal to 1.5 ns. We show that both piezoelectric and deformation potential coupling have to be taken into account to describe exciton transfer. The second model is phenomenological and was used to describe exciton transfer in GaAs1- xPx alloys. We obtain a good agreement with experimental results using parameters close to the previous ones. We demonstrate that, for selective excitation in the low energy side of the luminescence band, not only the transfer process but also luminescence assisted by acoustical phonons must be taken into account in order to explain time-resolved luminescence results.

  12. 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.

  13. Recombination dynamics of type-II excitons in (Ga,In)As/GaAs/Ga(As,Sb) heterostructures

    NASA Astrophysics Data System (ADS)

    Gies, S.; Holz, B.; Fuchs, C.; Stolz, W.; Heimbrodt, W.

    2017-01-01

    (Ga,In)As/GaAs/Ga(As,Sb) multi-quantum well heterostructures have been investigated using continuous wave and time-resolved photoluminescence spectroscopy at various temperatures. A complex interplay was observed between the excitonic type-II transitions with electrons in the (Ga,In)As well and holes in the Ga(As,Sb) well and the type-I excitons in the (Ga,In)As and Ga(As,Sb) wells. The type-II luminescence exhibits a strongly non-exponential temporal behavior below a critical temperature of T c = 70 K. The transients were analyzed in the framework of a rate-equation model. It was found that the exciton relaxation and hopping in the localized states of the disordered ternary Ga(As,Sb) are the decisive processes to describe the dynamics of the type-II excitons correctly.

  14. Recombination dynamics of type-II excitons in (Ga,In)As/GaAs/Ga(As,Sb) heterostructures.

    PubMed

    Gies, S; Holz, B; Fuchs, C; Stolz, W; Heimbrodt, W

    2017-01-13

    (Ga,In)As/GaAs/Ga(As,Sb) multi-quantum well heterostructures have been investigated using continuous wave and time-resolved photoluminescence spectroscopy at various temperatures. A complex interplay was observed between the excitonic type-II transitions with electrons in the (Ga,In)As well and holes in the Ga(As,Sb) well and the type-I excitons in the (Ga,In)As and Ga(As,Sb) wells. The type-II luminescence exhibits a strongly non-exponential temporal behavior below a critical temperature of T c = 70 K. The transients were analyzed in the framework of a rate-equation model. It was found that the exciton relaxation and hopping in the localized states of the disordered ternary Ga(As,Sb) are the decisive processes to describe the dynamics of the type-II excitons correctly.

  15. X-ray excited luminescence of polystyrene composites loaded with SrF2 nanoparticles

    NASA Astrophysics Data System (ADS)

    Demkiv, T. M.; Halyatkin, O. O.; Vistovskyy, V. V.; Hevyk, V. B.; Yakibchuk, P. M.; Gektin, A. V.; Voloshinovskii, A. S.

    2017-03-01

    The polystyrene film nanocomposites of 0.3 mm thickness with embedded SrF2 nanoparticles up to 40 wt% have been synthesized. The luminescent and kinetic properties of the polystyrene composites with embedded SrF2 nanoparticles upon the pulse X-ray excitation have been investigated. The luminescence intensity of the pure polystyrene scintillator film significantly increases when it is loaded with the inorganic SrF2 nanoparticles. The film nanocomposites show fast (∼2.8 ns) and slow (∼700 ns) luminescence decay components typical for a luminescence of polystyrene activators (p-Terphenyl and POPOP) and SrF2 nanoparticles, respectively. It is revealed that the fast decay luminescence component of the polystyrene composites is caused by the excitation of polystyrene by the photoelectrons escaped from the nanoparticles due to photoeffect, and the slow component is caused by reabsorption of the self-trapped exciton luminescence of SrF2 nanoparticles by polystyrene.

  16. Scanning tunneling luminescence of individual CdSe nanowires.

    PubMed

    Lutz, Theresa; Kabakchiev, Alexander; Dufaux, Thomas; Wolpert, Christian; Wang, Zhe; Burghard, Marko; Kuhnke, Klaus; Kern, Klaus

    2011-08-22

    The local luminescence properties of individual CdSe nanowires composed of segments of zinc blende and wurtzite crystal structures are investigated by low-temperature scanning tunneling luminescence spectroscopy. Light emission from the wires is achieved by the direct injection of holes and electrons, without the need for coupling to tip-induced plasmons in the underlying metal substrate. The photon energy is found to increase with decreasing wire diameter due to exciton confinement. The bulk bandgap extrapolated from the energy versus diameter dependence is consistent with photon emission from the zinc blende-type CdSe sections.

  17. Direct Observation of Ultrafast Exciton Formation in a Monolayer of WSe2.

    PubMed

    Steinleitner, Philipp; Merkl, Philipp; Nagler, Philipp; Mornhinweg, Joshua; Schüller, Christian; Korn, Tobias; Chernikov, Alexey; Huber, Rupert

    2017-03-08

    Many of the fundamental optical and electronic properties of atomically thin transition metal dichalcogenides are dominated by strong Coulomb interactions between electrons and holes, forming tightly bound atom-like states called excitons. Here, we directly trace the ultrafast formation of excitons by monitoring the absolute densities of bound and unbound electron-hole pairs in single monolayers of WSe2 on a diamond substrate following femtosecond nonresonant optical excitation. To this end, phase-locked mid-infrared probe pulses and field-sensitive electro-optic sampling are used to map out the full complex-valued optical conductivity of the nonequilibrium system and to discern the hallmark low-energy responses of bound and unbound pairs. While the spectral shape of the infrared response immediately after above-bandgap injection is dominated by free charge carriers, up to 60% of the electron-hole pairs are bound into excitons already on a subpicosecond time scale, evidencing extremely fast and efficient exciton formation. During the subsequent recombination phase, we still find a large density of free carriers in addition to excitons, indicating a nonequilibrium state of the photoexcited electron-hole system.

  18. Scaling laws of Rydberg excitons

    NASA Astrophysics Data System (ADS)

    Heckötter, J.; Freitag, M.; Fröhlich, D.; Aßmann, M.; Bayer, M.; Semina, M. A.; Glazov, M. M.

    2017-09-01

    Rydberg atoms have attracted considerable interest due to their huge interaction among each other and with external fields. They demonstrate characteristic scaling laws in dependence on the principal quantum number n for features such as the magnetic field for level crossing or the electric field of dissociation. Recently, the observation of excitons in highly excited states has allowed studying Rydberg physics in cuprous oxide crystals. Fundamentally different insights may be expected for Rydberg excitons, as the crystal environment and associated symmetry reduction compared to vacuum give not only optical access to many more states within an exciton multiplet but also extend the Hamiltonian for describing the exciton beyond the hydrogen model. Here we study experimentally and theoretically the scaling of several parameters of Rydberg excitons with n , for some of which we indeed find laws different from those of atoms. For others we find identical scaling laws with n , even though their origin may be distinctly different from the atomic case. At zero field the energy splitting of a particular multiplet n scales as n-3 due to crystal-specific terms in the Hamiltonian, e.g., from the valence band structure. From absorption spectra in magnetic field we find for the first crossing of levels with adjacent principal quantum numbers a Br∝n-4 dependence of the resonance field strength, Br, due to the dominant paramagnetic term unlike for atoms for which the diamagnetic contribution is decisive, resulting in a Br∝n-6 dependence. By contrast, the resonance electric field strength shows a scaling as Er∝n-5 as for Rydberg atoms. Also similar to atoms with the exception of hydrogen we observe anticrossings between states belonging to multiplets with different principal quantum numbers at these resonances. The energy splittings at the avoided crossings scale roughly as n-4, again due to crystal specific features in the exciton Hamiltonian. The data also allow us to

  19. Collective phenomena in cold indirect excitons

    SciTech Connect

    Butov, L. V.

    2016-03-15

    Due to their long lifetimes, indirect excitons can cool to below the temperature of quantum degeneracy. This gives an opportunity to experimentally study cold composite bosons. Both theoretically predicted phenomena and phenomena that have not been anticipated were observed in a cold gas of indirect excitons. In this contribution, we overview our studies of cold indirect excitons over the past decade, presenting spontaneous coherence and condensation of excitons, spatially modulated exciton state, long-range spin currents and spin textures, and exciton localization–delocalization transitions.

  20. LASER APPLICATIONS AND OTHER TOPICS IN QUANTUM ELECTRONICS: Two-photon-excited luminescence of biologically active solid-state structures

    NASA Astrophysics Data System (ADS)

    Gorelik, V. S.; Kozulin, E. A.

    1994-05-01

    A study was made of the characteristics of two-photon-excited luminescence of a number of pharmaceutical and biologically active solid-state materials: aspirin, sulfadimethoxine, Streptocid (sulfanilamide), pig insulin, and lysozyme. This luminescence was excited by pulse-periodic laser radiation. The characteristics of the luminescence spectra were compared with the familiar spectra of two-photon-excited luminescence of L-tryptophan. The results were used to determine the characteristics of molecular excitons in the investigated organic crystals and to estimate the concentration of tryptophan in solid-state proteins.

  1. Optical and structural study of GaN nanowires grown by catalyst-free molecular beam epitaxy. II. Sub-band-gap luminescence and electron irradiation effects

    SciTech Connect

    Robins, Lawrence H.; Bertness, Kris A.; Barker, Joy M.; Sanford, Norman A.; Schlager, John B.

    2007-06-01

    GaN nanowires with diameters of 50-250 nm, grown by catalyst-free molecular beam epitaxy, were characterized by photoluminescence (PL) and cathodoluminescence (CL) spectroscopy at temperatures from 3 to 297 K. Both as-grown samples and dispersions of the nanowires onto other substrates were examined. The properties of the near-band-edge PL and CL spectra were discussed in Part I of this study by [Robins et al. [L. H. Robins, K. A. Bertness, J. M. Barker, N. A. Sanford, and J. B. Schlager, J. Appl. Phys. 101,113505 (2007)]. Spectral features below the band gap, and the effect of extended electron irradiation on the CL, are discussed in Part II. The observed sub-band-gap PL and CL peaks are identified as phonon replicas of the free-exciton transitions, or excitons bound to structural defects or surface states. The defect-related peaks in the nanowires are correlated with luminescence lines previously reported in GaN films, denoted the Y lines [M. A. Reshchikov and H. Morkoc, J. Appl. Phys. 97, 061301 (2005)]. The CL was partially quenched by electron beam irradiation for an extended time; the quenching was stronger for the free and shallow-donor-bound exciton peaks than for the defect-related peaks. The quenching appeared to saturate at high irradiation dose (with final intensity {approx_equal}30% of initial intensity) and was reversible on thermal cycling to room temperature. The electron irradiation-induced quenching of the CL is ascribed to charge injection and trapping phenomena.

  2. Optical and structural study of GaN nanowires grown by catalyst-free molecular beam epitaxy. II. Sub-band-gap luminescence and electron irradiation effects

    NASA Astrophysics Data System (ADS)

    Robins, Lawrence H.; Bertness, Kris A.; Barker, Joy M.; Sanford, Norman A.; Schlager, John B.

    2007-06-01

    GaN nanowires with diameters of 50-250 nm, grown by catalyst-free molecular beam epitaxy, were characterized by photoluminescence (PL) and cathodoluminescence (CL) spectroscopy at temperatures from 3 to 297 K. Both as-grown samples and dispersions of the nanowires onto other substrates were examined. The properties of the near-band-edge PL and CL spectra were discussed in Part I of this study by [Robins et al. [L. H. Robins, K. A. Bertness, J. M. Barker, N. A. Sanford, and J. B. Schlager, J. Appl. Phys. 101,113505 (2007)]. Spectral features below the band gap, and the effect of extended electron irradiation on the CL, are discussed in Part II. The observed sub-band-gap PL and CL peaks are identified as phonon replicas of the free-exciton transitions, or excitons bound to structural defects or surface states. The defect-related peaks in the nanowires are correlated with luminescence lines previously reported in GaN films, denoted the Y lines [M. A. Reshchikov and H. Morkoc, J. Appl. Phys. 97, 061301 (2005)]. The CL was partially quenched by electron beam irradiation for an extended time; the quenching was stronger for the free and shallow-donor-bound exciton peaks than for the defect-related peaks. The quenching appeared to saturate at high irradiation dose (with final intensity ≈30% of initial intensity) and was reversible on thermal cycling to room temperature. The electron irradiation-induced quenching of the CL is ascribed to charge injection and trapping phenomena.

  3. Ultrafast exciton dissociation at donor/acceptor interfaces

    NASA Astrophysics Data System (ADS)

    Grancini, G.; Fazzi, D.; Binda, M.; Maiuri, M.; Petrozza, A.; Criante, L.; Perissinotto, S.; Egelhaaf, H.-J.; Brida, D.; Cerullo, G.; Lanzani, G.

    2013-09-01

    Charge generation at donor/acceptor interface is a highly debated topic in the organic photovoltaics (OPV) community. The primary photoexcited state evolution happens in few femtosecond timescale, thus making very intriguing their full understanding. In particular charge generation is believed to occur in < 200 fs, but no clear picture emerged so far. In this work we reveal for the first time the actual charge generation mechanism following in real time the exciton dissociation mechanism by means of sub-22 fs pump-probe spectroscopy. We study a low-band-gap polymer: fullerene interface as an ideal system for OPV. We demonstrate that excitons dissociation leads, on a timescale of 20-50 fs, to two byproducts: bound interfacial charge transfer states (CTS) and free charges. The branching ratio of their formation depends on the excess photon energy provided. When high energy singlet polymer states are excited, well above the optical band gap, an ultrafast hot electron transfer happens between the polymer singlet state and the interfacial hot CTS* due to the high electronic coupling between them. Hot exciton dissociation prevails then on internal energy dissipation that occurs within few hundreds of fs. By measuring the internal quantum efficiency of a prototypical device a rising trend with energy is observed, thus indicating that hot exciton dissociation effectively leads to a higher fraction of free charges.

  4. Dynamical reconstruction of the exciton in LiF with inelastic x-ray scattering

    SciTech Connect

    Abbamonte, Peter; Graber, Tim; Reed, James P.; Smadici, Serban; Yeh, Chen-Lin; Shukla, Abhay; Rueff, Jean-Pascal; Ku, Wei

    2008-11-03

    The absorption of light by materials proceeds through the formation of excitons, which are states in which an excited electron is bound to the valence hole it vacated. Understanding the structure and dynamics of excitons is important, for example, for developing technologies for light-emitting diodes or solar energy conversion. However, there has never been an experimental means to study the time-dependent structure of excitons directly. Here, we use causality-inverted inelastic x-ray scattering (IXS) to image the charge-transfer exciton in the prototype insulator LiF, with resolutions {Delta}t = 20.67 as (2.067 x 10{sup -17} s) in time and {Delta}x = 0.533 {angstrom} (5.33 x 10{sup -11} m) in space. Our results show that the exciton has a modulated internal structure and is coherently delocalized over two unit cells of the LiF crystal ({approx}8 {angstrom}). This structure changes only modestly during the course of its life, which establishes it unambiguously as a Frenkel exciton and thus amenable to a simplified theoretical description. Our results resolve an old controversy about excitons in the alkali halides and demonstrate the utility of IXS for imaging attosecond electron dynamics in condensed matter.

  5. Dynamical reconstruction of the exciton in LiF with inelastic x-ray scattering.

    PubMed

    Abbamonte, Peter; Graber, Tim; Reed, James P; Smadici, Serban; Yeh, Chen-Lin; Shukla, Abhay; Rueff, Jean-Pascal; Ku, Wei

    2008-08-26

    The absorption of light by materials proceeds through the formation of excitons, which are states in which an excited electron is bound to the valence hole it vacated. Understanding the structure and dynamics of excitons is important, for example, for developing technologies for light-emitting diodes or solar energy conversion. However, there has never been an experimental means to study the time-dependent structure of excitons directly. Here, we use causality-inverted inelastic x-ray scattering (IXS) to image the charge-transfer exciton in the prototype insulator LiF, with resolutions Delta t = 20.67 as (2.067 x 10(-17) s) in time and Delta x = 0.533 A (5.33 x 10(-11) m) in space. Our results show that the exciton has a modulated internal structure and is coherently delocalized over two unit cells of the LiF crystal (approximately 8 A). This structure changes only modestly during the course of its life, which establishes it unambiguously as a Frenkel exciton and thus amenable to a simplified theoretical description. Our results resolve an old controversy about excitons in the alkali halides and demonstrate the utility of IXS for imaging attosecond electron dynamics in condensed matter.

  6. Dynamical reconstruction of the exciton in LiF with inelastic x-ray scattering

    PubMed Central

    Abbamonte, Peter; Graber, Tim; Reed, James P.; Smadici, Serban; Yeh, Chen-Lin; Shukla, Abhay; Rueff, Jean-Pascal; Ku, Wei

    2008-01-01

    The absorption of light by materials proceeds through the formation of excitons, which are states in which an excited electron is bound to the valence hole it vacated. Understanding the structure and dynamics of excitons is important, for example, for developing technologies for light-emitting diodes or solar energy conversion. However, there has never been an experimental means to study the time-dependent structure of excitons directly. Here, we use causality-inverted inelastic x-ray scattering (IXS) to image the charge-transfer exciton in the prototype insulator LiF, with resolutions Δt = 20.67 as (2.067 × 10−17 s) in time and Δx = 0.533 Å (5.33 × 10−11 m) in space. Our results show that the exciton has a modulated internal structure and is coherently delocalized over two unit cells of the LiF crystal (≈8 Å). This structure changes only modestly during the course of its life, which establishes it unambiguously as a Frenkel exciton and thus amenable to a simplified theoretical description. Our results resolve an old controversy about excitons in the alkali halides and demonstrate the utility of IXS for imaging attosecond electron dynamics in condensed matter. PMID:18711146

  7. 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.

  8. Giant exciton Fano resonance in quasi-one-dimensional Ta2NiSe5

    NASA Astrophysics Data System (ADS)

    Larkin, T. I.; Yaresko, A. N.; Pröpper, D.; Kikoin, K. A.; Lu, Y. F.; Takayama, T.; Mathis, Y.-L.; Rost, A. W.; Takagi, H.; Keimer, B.; Boris, A. V.

    2017-05-01

    We report the complex dielectric function of the quasi-one-dimensional chalcogenide Ta2NiSe5 , which undergoes a structural phase transition presumably associated with exciton condensation below Tc=326 K [Y. Wakisaka et al., Phys. Rev. Lett. 103, 026402 (2009), 10.1103/PhysRevLett.103.026402; Y. F. Lu et al., Nat. Commun. 8, 14408 (2017), 10.1038/ncomms14408], and of the isostructural Ta2NiS5 , which does not exhibit such a transition. Using spectroscopic ellipsometry, we have detected exciton doublets with pronounced Fano line shapes in both the compounds. The exciton Fano resonances in Ta2NiSe5 display an order-of-magnitude higher intensity than those in Ta2NiS5 . In conjunction with prior theoretical work [E. Rashba, Sov. Phys. Semicond. 8, 807 (1975)], we attribute this observation to the giant oscillator strength of spatially extended exciton-phonon bound states in Ta2NiSe5 . The formation of exciton-phonon complexes in Ta2NiS5 and Ta2NiSe5 is confirmed by the pronounced temperature dependence of sharp interband transitions in the optical spectra, the peak energies and widths of which scale with the thermal population of optical phonon modes. The description of the optically excited states in terms of strongly overlapping exciton complexes is in good agreement with the hypothesis of an exciton insulator ground state.

  9. Exciton dispersion in molecular solids.

    PubMed

    Cudazzo, Pierluigi; Sottile, Francesco; Rubio, Angel; Gatti, Matteo

    2015-03-25

    The investigation of the exciton dispersion (i.e. the exciton energy dependence as a function of the momentum carried by the electron-hole pair) is a powerful approach to identify the exciton character, ranging from the strongly localised Frenkel to the delocalised Wannier-Mott limiting cases. We illustrate this possibility at the example of four prototypical molecular solids (picene, pentacene, tetracene and coronene) on the basis of the parameter-free solution of the many-body Bethe-Salpeter equation. We discuss the mixing between Frenkel and charge-transfer excitons and the origin of their Davydov splitting in the framework of many-body perturbation theory and establish a link with model approaches based on molecular states. Finally, we show how the interplay between the electronic band dispersion and the exchange electron-hole interaction plays a fundamental role in setting the nature of the exciton. This analysis has a general validity holding also for other systems in which the electron wavefunctions are strongly localized, as in strongly correlated insulators.

  10. Exciton dispersion in molecular solids

    NASA Astrophysics Data System (ADS)

    Cudazzo, Pierluigi; Sottile, Francesco; Rubio, Angel; Gatti, Matteo

    2015-03-01

    The investigation of the exciton dispersion (i.e. the exciton energy dependence as a function of the momentum carried by the electron-hole pair) is a powerful approach to identify the exciton character, ranging from the strongly localised Frenkel to the delocalised Wannier-Mott limiting cases. We illustrate this possibility at the example of four prototypical molecular solids (picene, pentacene, tetracene and coronene) on the basis of the parameter-free solution of the many-body Bethe-Salpeter equation. We discuss the mixing between Frenkel and charge-transfer excitons and the origin of their Davydov splitting in the framework of many-body perturbation theory and establish a link with model approaches based on molecular states. Finally, we show how the interplay between the electronic band dispersion and the exchange electron-hole interaction plays a fundamental role in setting the nature of the exciton. This analysis has a general validity holding also for other systems in which the electron wavefunctions are strongly localized, as in strongly correlated insulators.

  11. Novel Exciton States in Monolayer MoS2: Unconventional Effective Hamiltonian

    NASA Astrophysics Data System (ADS)

    da Jornada, Felipe; Qiu, Diana; Louie, Steven

    2014-03-01

    Recent well-converged ab inito GW-BSE calculations show that monolayer MoS2 has a large number of strongly bound excitons with varying characters. We show that these excitonic states cannot be even qualitatively described by an effective mass hydrogenic model without a detailed understanding of the 2D screening. Additionally, we identify and analyze one exciton series having an unusually high binding energy, which originates around the Γ point of the Brillouin zone. We show that this excitonic series arises from a fundamentally different effective Hamiltonian with a kinetic energy term resembling a Mexican hat in momentum space, which is responsible for the unusual ordering of the energy levels and distribution of oscillator strength. This work was supported by NSF grant No. DMR10-1006184 and the U.S. DOE under Contract No. DE-AC02-05CH11231.

  12. Time-resolved study of luminescence in highly luminescent disubstituted polyacetylene and its blend with poorly luminescent monosubstituted polyacetylene

    NASA Astrophysics Data System (ADS)

    Hidayat, Rahmat; Tatsuhara, Satoshi; Kim, Dong Wook; Ozaki, Masanori; Yoshino, Katsumi; Teraguchi, Masahiro; Masuda, Toshio

    2000-04-01

    A highly luminescent disubstituted polyacetylene, poly(1-phenyl-2-p-n-butylphenylacetylene) (PDPA-nBu), and its blend with a poorly luminescent monosubstituted polyacetylene, poly(1-o-trimethylsilylphenylacetylene) (PPA-oSiMe3), are studied by time-resolved photoluminescence (PL) spectroscopy. In pure PDPA-nBu, PL intensity at short wavelength decays faster than that at long wavelength, whereas PL spectra exhibit a dynamic Stokes shift to longer wavelengths with time. In blends of PDPA-nBu/PPA-oSiMe3, only PL originating from PDPA-nBu is observed, without contribution from PPA-oSiMe3. The PL lifetime drastically decreases upon mixing a small amount of PPA-oSiMe3 in PDPA-nBu. The PL characteristics of pure PDPA-nBu and its blend with PPA-oSiMe3 are discussed in terms of lattice/vibrational relaxation of the excitonic state and exciton migration.

  13. Luminescence properties and electronic structure of Ce{sup 3+}-doped gadolinium aluminum garnet

    SciTech Connect

    Dotsenko, V.P.; Berezovskaya, I.V.; Voloshinovskii, A.S.; Zadneprovski, B.I.; Efryushina, N.P.

    2015-04-15

    Highlights: • The luminescence properties of Ce{sup 3+} ions in (Y, Gd){sub 3}Al{sub 5}O{sub 12} are analyzed. • The Gd{sup 3+} → Y{sup 3+} substitution leads to increasing of Ce{sup 3+} noncubic crystal field splitting parameter. • The excitation spectra for the Ce{sup 3+} emission in GdAG contain bands at 6.67, 7.75, and 9.76 eV. • These features are due to the Ce{sup 3+}-bound exciton formation and O 2p → Al 3s, 3p transitions. • Contributions from Al atoms to the conduction-band density of states are quite essential. - Abstract: Yttrium-gadolinium aluminum garnets (YGdAG) doped with Ce{sup 3+} ions have been prepared by co-precipitation method. The luminescent properties of Ce{sup 3+} ions in Gd{sub 3(1−x)}Ce{sub 3x}Al{sub 5}O{sub 12} (x = 0.01) have been studied upon excitation in the 2–20 eV region. The substitution of Gd{sup 3+} for Y{sup 3+} in the garnet structure results in broadening the emission band and shifting its maximum towards the longer wavelengths. It was found that in addition to the 4f → 5d excitation bands of Ce{sup 3+} ions, the excitation spectra for the Ce{sup 3+} emission contain bands at 6.67, 7.75, and 9.76 eV. These bands are attributed to the Ce{sup 3+}-bound exciton formation and O 2p → Al 3s, 3p transitions, respectively. Although gadolinium states dominate near the bottom of the conduction band of Gd{sub 3}Al{sub 5}O{sub 12}, contributions from Al{sub tetr} and Al{sub oct} atoms to the conduction-band density of states are evaluated as quite essential.

  14. Excitonic polaritons in Fibonacci quasicrystals.

    PubMed

    Hendrickson, J; Richards, B C; Sweet, J; Khitrova, G; Poddubny, A N; Ivchenko, E L; Wegener, M; Gibbs, H M

    2008-09-29

    The fabrication and characterization of light-emitting one-dimensional photonic quasicrystals based on excitonic resonances is reported. The structures consist of high-quality GaAs/AlGaAs quantum wells grown by molecular-beam epitaxy with wavelength-scale spacings satisfying a Fibonacci sequence. The polaritonic (resonant light-matter coupling) effects and light emission originate from the quantum well excitonic resonances. Measured reflectivity spectra as a function of detuning between emission and Bragg wavelength are in good agreement with excitonic polariton theory. Photoluminescence experiments show that active photonic quasicrystals, unlike photonic crystals, can be good light emitters: While their long-range order results in a stopband similar to that of photonic crystals, the lack of periodicity results in strong emission.

  15. Luminescence decay and the absorption cross section of individual single-walled carbon nanotubes.

    PubMed

    Berciaud, Stéphane; Cognet, Laurent; Lounis, Brahim

    2008-08-15

    The absorption cross section of highly luminescent individual single-walled carbon nanotubes is determined using time-resolved and cw luminescence spectroscopy. A mean value of approximately 1 x 10(-17) cm2 per carbon atom is obtained for (6,5) tubes excited at their second optical transition, and corroborated by single tube photothermal absorption measurements. Biexponential luminescence decays are systematically observed, with short and long lifetimes around 45 and 250 ps. This behavior is attributed to the band edge exciton fine structure with a dark level lying a few meV below a bright one.

  16. Environmental and synthesis-dependent luminescence properties of individual single-walled carbon nanotubes.

    PubMed

    Duque, Juan G; Pasquali, Matteo; Cognet, Laurent; Lounis, Brahim

    2009-08-25

    Luminescence properties of individual (6,5) single-walled carbon nanotubes (SWNTs) were studied using continuous wave and time-resolved spectroscopy. Nanotubes synthesized by different methods (HiPco and CoMoCat) and dispersed in two different ionic surfactants were examined either in aqueous environments or deposited on surfaces. SWNT preparations leading to the highest luminescence intensities and narrowest spectral widths exhibit the longest luminescence decay times. This highlights the role of the nanotube environment and synthesis methods in the nonradiative relaxation processes of the excitonic recombination. Samples of HiPco nanotubes dispersed in sodium deoxycholate contained the brightest nanotubes in aqueous environments.

  17. 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

  18. 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.”.

  19. Bosonic cascades of indirect excitons

    NASA Astrophysics Data System (ADS)

    Nalitov, A. V.; De Liberato, S.; Lagoudakis, P.; Savvidis, P. G.; Kavokin, A. V.

    2017-08-01

    Recently, the concept of the terahertz bosonic cascade laser (BCL) based on a parabolic quantum well (PQW) embedded in a microcavity was proposed. We refine this proposal by suggesting transitions between indirect exciton (IX) states as a source of terahertz emission. We explicitly propose a structure containing a narrow-square QW and a wide-parabolic QW for the realisation of a bosonic cascade. Advantages of this type of structures are in large dipole matrix elements for terahertz transitions and in long exciton radiative lifetimes which are crucial for realisation of threshold and quantum efficiency BCLs.

  20. Vibration-assisted upconversion of molecular luminescence induced by scanning tunneling microscopy.

    PubMed

    Miwa, Kuniyuki; Sakaue, Mamoru; Kasai, Hideaki

    2013-05-01

    : We investigate the effects of coupling between a molecular exciton, which consists of an electron and a hole in a molecule, and a surface plasmon (exciton-plasmon coupling) on the electron transitions of the molecule using nonequilibrium Green's function method. Due to the exciton-plasmon coupling, excitation channels of the molecule arise in the energy range lower than the electronic excitation energy of the molecule. It is found that the electron transitions via these excitation channels give rise to the molecular luminescence and the vibrational excitations at the bias voltage lower than the electronic excitation energy of the molecule. Our results also indicate that the vibrational excitations assist the emission of photons, whose energy exceeds the product of the elementary charge and the bias voltage, (upconverted luminescence).

  1. Excitonic transitions in highly efficient (GaIn)As/Ga(AsSb) type-II quantum-well structures

    SciTech Connect

    Gies, S.; Kruska, C.; Berger, C.; Hens, P.; Fuchs, C.; Rosemann, N. W.; Veletas, J.; Stolz, W.; Koch, S. W.; Heimbrodt, W.; Ruiz Perez, A.; Hader, J.; Moloney, J. V.

    2015-11-02

    The excitonic transitions of the type-II (GaIn)As/Ga(AsSb) gain medium of a “W”-laser structure are characterized experimentally by modulation spectroscopy and analyzed using microscopic quantum theory. On the basis of the very good agreement between the measured and calculated photoreflectivity, the type-I or type-II character of the observable excitonic transitions is identified. Whereas the energetically lowest three transitions exhibit type-II character, the subsequent energetically higher transitions possess type-I character with much stronger dipole moments. Despite the type-II character, the quantum-well structure exhibits a bright luminescence.

  2. Mechanisms of energy transport in BeO over the temperature region of self-trapped exciton transformation

    NASA Astrophysics Data System (ADS)

    Ogorodnikov, I. N.; Kruzhalov, A. V.

    1997-02-01

    The specificity of mechanism of energy transport in BeO over the temperature region of self-trapped exciton transformation is considered in the framework of the model of a field fluctuation process (FFP). The paper discusses the results of the computer simulation of a perturbing effect of FPP on kinetics and parameters of thermally stimulated luminescence in comparison with the appropriate experimental data gained for beryllium oxide crystals. It was shown that the observed peculiarities of recombination processes in BeO over the temperature region between 150 and 180 K are due to the self-trapped exciton transformation.

  3. Multiple exciton collection in a sensitized photovoltaic system.

    PubMed

    Sambur, Justin B; Novet, Thomas; Parkinson, B A

    2010-10-01

    Multiple exciton generation, the creation of two electron-hole pairs from one high-energy photon, is well established in bulk semiconductors, but assessments of the efficiency of this effect remain controversial in quantum-confined systems like semiconductor nanocrystals. We used a photoelectrochemical system composed of PbS nanocrystals chemically bound to TiO(2) single crystals to demonstrate the collection of photocurrents with quantum yields greater than one electron per photon. The strong electronic coupling and favorable energy level alignment between PbS nanocrystals and bulk TiO(2) facilitate extraction of multiple excitons more quickly than they recombine, as well as collection of hot electrons from higher quantum dot excited states. Our results have implications for increasing the efficiency of photovoltaic devices by avoiding losses resulting from the thermalization of photogenerated carriers.

  4. Exciton spectra in two-dimensional graphene derivatives

    NASA Astrophysics Data System (ADS)

    Huang, Shouting; Liang, Yufeng; Yang, Li

    2013-08-01

    The energy spectra and wave functions of bound excitons in important two-dimensional (2D) graphene derivatives, i.e., graphyne and graphane, are found to be strongly modified by quantum confinement, making them qualitatively different from the usual Rydberg series. However, their parity and optical selection rules are preserved. Thus a one-parameter modified hydrogenic model is applied to quantitatively explain the ab initio exciton spectra, and allows one to extrapolate the electron-hole binding energy from optical spectroscopies of 2D semiconductors without costly simulations. Meanwhile, our calculated optical absorption spectrum and enhanced spin singlet-triplet splitting project graphyne, an allotrope of graphene, as a candidate for intriguing energy and biomedical applications.

  5. Measurement of exciton correlations using electrostatic lattices

    NASA Astrophysics Data System (ADS)

    Remeika, M.; Leonard, J. R.; Dorow, C. J.; Fogler, M. M.; Butov, L. V.; Hanson, M.; Gossard, A. C.

    2015-09-01

    We present a method for determining correlations in a gas of indirect excitons in a semiconductor quantum well structure. The method involves subjecting the excitons to a periodic electrostatic potential that causes modulations of the exciton density and photoluminescence (PL). Experimentally measured amplitudes of energy and intensity modulations of exciton PL serve as an input to a theoretical estimate of the exciton correlation parameter and temperature. We also present a proof-of-principle demonstration of the method for determining the correlation parameter and discuss how its accuracy can be improved.

  6. Excitonic effects in two-dimensional semiconductors: Path integral Monte Carlo approach

    DOE PAGES

    Velizhanin, Kirill A.; Saxena, Avadh

    2015-11-01

    The most striking features of novel two-dimensional semiconductors (e.g., transition metal dichalcogenide monolayers or phosphorene) is a strong Coulomb interaction between charge carriers resulting in large excitonic effects. In particular, this leads to the formation of multicarrier bound states upon photoexcitation (e.g., excitons, trions, and biexcitons), which could remain stable at near-room temperatures and contribute significantly to the optical properties of such materials. In our work we have used the path integral Monte Carlo methodology to numerically study properties of multicarrier bound states in two-dimensional semiconductors. Specifically, we have accurately investigated and tabulated the dependence of single-exciton, trion, and biexcitonmore » binding energies on the strength of dielectric screening, including the limiting cases of very strong and very weak screening. Our results of this work are potentially useful in the analysis of experimental data and benchmarking of theoretical and computational models.« less

  7. Excitonic effects in two-dimensional semiconductors: Path integral Monte Carlo approach

    SciTech Connect

    Velizhanin, Kirill A.; Saxena, Avadh

    2015-11-01

    The most striking features of novel two-dimensional semiconductors (e.g., transition metal dichalcogenide monolayers or phosphorene) is a strong Coulomb interaction between charge carriers resulting in large excitonic effects. In particular, this leads to the formation of multicarrier bound states upon photoexcitation (e.g., excitons, trions, and biexcitons), which could remain stable at near-room temperatures and contribute significantly to the optical properties of such materials. In our work we have used the path integral Monte Carlo methodology to numerically study properties of multicarrier bound states in two-dimensional semiconductors. Specifically, we have accurately investigated and tabulated the dependence of single-exciton, trion, and biexciton binding energies on the strength of dielectric screening, including the limiting cases of very strong and very weak screening. Our results of this work are potentially useful in the analysis of experimental data and benchmarking of theoretical and computational models.

  8. 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.

  9. 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.

  10. 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.

  11. Luminescence from ZnS: Bulk vs nano

    NASA Astrophysics Data System (ADS)

    Mishra, R. K.; Kamal, Satya; Patel, D. K.; Rao, K. Ramachandra; Sudarsan, V.; Vatsa, R. K.

    2015-06-01

    Based on the detailed luminescence studies on bulk and nanoparticles of ZnS, it is inferred that the defect emission due to zinc (VZn) and sulfur (VS) vacancies in ZnS, significantly change in terms of line shape and peak position, when bulk form is converted to nanoparticles. From the XRD studies, this has been explained in terms of difference in the crystalline modifications of ZnS, namely the wurtzite and cubic forms. Copper doping in the sample quenches the luminescence and stabilize the cubic phase. Bright blue electro luminescence (efficiency of around 1.5 %) with CIE coordinates (0.18. 0.11) could be seen from bulk ZnS:Cu sample. Unlike this the nanoparticles did not give any emission due to the quenching of charge carriers/excitons. Lifetime values further supported these inferences.

  12. Improvement of luminescence properties of GaN buffer layer for fast nitride scintillator structures

    NASA Astrophysics Data System (ADS)

    Hubáček, T.; Hospodková, A.; Oswald, J.; Kuldová, K.; Pangrác, J.

    2017-04-01

    We have optimized technology of GaN buffer layer growth with respect to the application in fast scintillation structures. The deep defect luminescence so called yellow band (YB) with decay time up to tens of microseconds is undesired for these applications and should be suppressed or at least the ratio of intensities of excitonic to YB maximum has to be considerably increased. The required photoluminescence properties were achieved by optimization of growth parameters of nucleation and coalescence layer on sapphire substrate. We have shown that decrease of NH3 flow, decrease of coalescence temperature, increase of nucleation time and nucleation pressure lead to improvement of the structure and luminescence properties of the buffer layer. Results indicate a significant increased ratio of excitonic/YB luminescence intensity.

  13. Even exciton series in Cu2O

    NASA Astrophysics Data System (ADS)

    Schweiner, Frank; Main, Jörg; Wunner, Günter; Uihlein, Christoph

    2017-05-01

    Recent investigations of excitonic absorption spectra in cuprous oxide (Cu2O ) have shown that it is indispensable to account for the complex valence-band structure in the theory of excitons. In Cu2O , parity is a good quantum number and thus the exciton spectrum falls into two parts: the dipole-active exciton states of negative parity and odd angular momentum, which can be observed in one-photon absorption (Γ4- symmetry), and the exciton states of positive parity and even angular momentum, which can be observed in two-photon absorption (Γ5+ symmetry). The unexpected observation of D excitons in two-photon absorption has given first evidence that the dispersion properties of the Γ5+ orbital valence band are giving rise to a coupling of the yellow and green exciton series. However, a first theoretical treatment by Uihlein et al. [Phys. Rev. B 23, 2731 (1981), 10.1103/PhysRevB.23.2731] was based on a simplified spherical model. The observation of F excitons in one-photon absorption is a further proof of a coupling between yellow and green exciton states. Detailed investigations on the fine structure splitting of the F exciton by F. Schweiner et al. [Phys. Rev. B 93, 195203 (2016), 10.1103/PhysRevB.93.195203] have proved the importance of a more realistic theoretical treatment including terms with cubic symmetry. In this paper we show that the even and odd parity exciton system can be consistently described within the same theoretical approach. However, the Hamiltonian of the even parity system needs, in comparison to the odd exciton case, modifications to account for the very small radius of the yellow and green 1 S exciton. In the presented treatment, we take special care of the central-cell corrections, which comprise a reduced screening of the Coulomb potential at distances comparable to the polaron radius, the exchange interaction being responsible for the exciton splitting into ortho and para states, and the inclusion of terms in the fourth power of p in the

  14. Exciton-exciton scattering: Composite boson versus elementary boson

    NASA Astrophysics Data System (ADS)

    Combescot, M.; Betbeder-Matibet, O.; Combescot, R.

    2007-05-01

    This paper shows the necessity of introducing a quantum object, the “coboson,” to properly describe, through a fermion scheme, any composite particle, such as the exciton, which is made of two fermions. Although commonly dealt with as elementary bosons, these composite bosons—cobosons in short—differ from them due to their composite nature which makes the handling of their many-body effects quite different from the existing treatments valid for elementary bosons. As a direct consequence of this composite nature, there is no correct way to describe the interaction between cobosons as a potential V . This is rather dramatic because, with the Hamiltonian not written as H=H0+V , all the usual approaches to many-body effects fail. In particular, the standard form of the Fermi golden rule, written in terms of V , cannot be used to obtain the transition rates of two cobosons. To get them, we have had to construct an unconventional expression for this Fermi golden rule in which H only appears. Making use of this expression, we give here a detailed calculation of the time evolution of two excitons. We compare the results of this exact approach with the ones obtained by using an effective bosonic Hamiltonian in which the excitons are considered as elementary bosons with effective scatterings between them, these scatterings resulting from an elaborate mapping between the two-fermion space and the ideal boson space. We show that the relation between the inverse lifetime and the sum of the transition rates for elementary bosons differs from the one of the composite bosons by a factor of 1/2 , so that it is impossible to find effective scatterings between bosonic excitons giving these two physical quantities correctly, whatever the mapping from composite bosons to elementary bosons is. The present paper thus constitutes a strong mathematical proof that, in spite of a widely spread belief, we cannot forget the composite nature of these cobosons, even in the extremely low

  15. Photoluminescence characteristics of CdSe quantum dots: role of exciton-phonon coupling and defect/trap states

    NASA Astrophysics Data System (ADS)

    Kushavah, Dushyant; Mohapatra, P. K.; Ghosh, Pintu; Singh, Mamraj; Vasa, P.; Bahadur, D.; Singh, B. P.

    2017-07-01

    In this paper, we report temperature dependent photoluminescence (PL) characteristics of CdSe colloidal QDs with average diameter ~2.8 nm. Temperature dependence of strongly confined exciton PL peak position, linewidth and intensity were investigated in 30 K to 300 K temperature range. Our studies reveal nearly four times weaker exciton-LO phonon coupling than bulk CdSe crystal. Theoretically, it should be vanishingly small due to near identical electron and hole charge distributions in strongly confined QDs. On the other hand, exciton-acoustic phonon coupling is an order of magnitude larger than its bulk counterpart. Observed finite value of exciton-LO phonon coupling and enhanced exciton-acoustic phonon coupling are due to piezoelectric strain fields. PL intensity exhibits anomalous behavior in the temperature range 100-230 K. This has been explained by thermally activated detrapping of the charge carriers trapped in the potential wells formed at the interface adjoining dislocations/stacking faults developed during the synthesis process. Above 230 K, PL is partially quenched by thermal escape of charge carriers from luminescing exciton state to higher lying nonluminescing states.

  16. A Comparison Between Magnetic Field Effects in Excitonic and Exciplex Organic Light-Emitting Diodes

    NASA Astrophysics Data System (ADS)

    Sahin Tiras, Kevser; Wang, Yifei; Harmon, Nicholas J.; Wohlgenannt, Markus; Flatte, Michael E.

    In flat-panel displays and lighting applications, organic light emitting diodes (OLEDs) have been widely used because of their efficient light emission, low-cost manufacturing and flexibility. The electrons and holes injected from the anode and cathode, respectively, form a tightly bound exciton as they meet at a molecule in organic layer. Excitons occur as spin singlets or triplets and the ratio between singlet and triplet excitons formed is 1:3 based on spin degeneracy. The internal quantum efficiency (IQE) of fluorescent-based OLEDs is limited 25% because only singlet excitons contribute the light emission. To overcome this limitation, thermally activated delayed fluorescent (TADF) materials have been introduced in the field of OLEDs. The exchange splitting between the singlet and triplet states of two-component exciplex systems is comparable to the thermal energy in TADF materials, whereas it is usually much larger in excitons. Reverse intersystem crossing occurs from triplet to singlet exciplex state, and this improves the IQE. An applied small magnetic field can change the spin dynamics of recombination in TADF blends. In this study, magnetic field effects on both excitonic and exciplex OLEDs will be presented and comparison similarities and differences will be made.

  17. 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.

  18. Probing dark excitons in atomically thin semiconductors via near-field coupling to surface plasmon polaritons

    NASA Astrophysics Data System (ADS)

    Zhou, You; Scuri, Giovanni; Wild, Dominik S.; High, Alexander A.; Dibos, Alan; Jauregui, Luis A.; Shu, Chi; de Greve, Kristiaan; Pistunova, Kateryna; Joe, Andrew Y.; Taniguchi, Takashi; Watanabe, Kenji; Kim, Philip; Lukin, Mikhail D.; Park, Hongkun

    2017-09-01

    Transition metal dichalcogenide (TMD) monolayers with a direct bandgap feature tightly bound excitons, strong spin-orbit coupling and spin-valley degrees of freedom. Depending on the spin configuration of the electron-hole pairs, intra-valley excitons of TMD monolayers can be either optically bright or dark. Dark excitons involve nominally spin-forbidden optical transitions with a zero in-plane transition dipole moment, making their detection with conventional far-field optical techniques challenging. Here, we introduce a method for probing the optical properties of two-dimensional materials via near-field coupling to surface plasmon polaritons (SPPs). This coupling selectively enhances optical transitions with dipole moments normal to the two-dimensional plane, enabling direct detection of dark excitons in TMD monolayers. When a WSe2 monolayer is placed on top of a single-crystal silver film, its emission into near-field-coupled SPPs displays new spectral features whose energies and dipole orientations are consistent with dark neutral and charged excitons. The SPP-based near-field spectroscopy significantly improves experimental capabilities for probing and manipulating exciton dynamics of atomically thin materials, thus opening up new avenues for realizing active metasurfaces and robust optoelectronic systems, with potential applications in information processing and communication.

  19. Ultrafast formation of interlayer hot excitons in atomically thin MoS2/WS2 heterostructures

    NASA Astrophysics Data System (ADS)

    Chen, Hailong; Wen, Xiewen; Zhang, Jing; Wu, Tianmin; Gong, Yongji; Zhang, Xiang; Yuan, Jiangtan; Yi, Chongyue; Lou, Jun; Ajayan, Pulickel M.; Zhuang, Wei; Zhang, Guangyu; Zheng, Junrong

    2016-08-01

    Van der Waals heterostructures composed of two-dimensional transition-metal dichalcogenides layers have recently emerged as a new family of materials, with great potential for atomically thin opto-electronic and photovoltaic applications. It is puzzling, however, that the photocurrent is yielded so efficiently in these structures, despite the apparent momentum mismatch between the intralayer/interlayer excitons during the charge transfer, as well as the tightly bound nature of the excitons in 2D geometry. Using the energy-state-resolved ultrafast visible/infrared microspectroscopy, we herein obtain unambiguous experimental evidence of the charge transfer intermediate state with excess energy, during the transition from an intralayer exciton to an interlayer exciton at the interface of a WS2/MoS2 heterostructure, and free carriers moving across the interface much faster than recombining into the intralayer excitons. The observations therefore explain how the remarkable charge transfer rate and photocurrent generation are achieved even with the aforementioned momentum mismatch and excitonic localization in 2D heterostructures and devices.

  20. Probing dark excitons in atomically thin semiconductors via near-field coupling to surface plasmon polaritons.

    PubMed

    Zhou, You; Scuri, Giovanni; Wild, Dominik S; High, Alexander A; Dibos, Alan; Jauregui, Luis A; Shu, Chi; De Greve, Kristiaan; Pistunova, Kateryna; Joe, Andrew Y; Taniguchi, Takashi; Watanabe, Kenji; Kim, Philip; Lukin, Mikhail D; Park, Hongkun

    2017-09-01

    Transition metal dichalcogenide (TMD) monolayers with a direct bandgap feature tightly bound excitons, strong spin-orbit coupling and spin-valley degrees of freedom. Depending on the spin configuration of the electron-hole pairs, intra-valley excitons of TMD monolayers can be either optically bright or dark. Dark excitons involve nominally spin-forbidden optical transitions with a zero in-plane transition dipole moment, making their detection with conventional far-field optical techniques challenging. Here, we introduce a method for probing the optical properties of two-dimensional materials via near-field coupling to surface plasmon polaritons (SPPs). This coupling selectively enhances optical transitions with dipole moments normal to the two-dimensional plane, enabling direct detection of dark excitons in TMD monolayers. When a WSe2 monolayer is placed on top of a single-crystal silver film, its emission into near-field-coupled SPPs displays new spectral features whose energies and dipole orientations are consistent with dark neutral and charged excitons. The SPP-based near-field spectroscopy significantly improves experimental capabilities for probing and manipulating exciton dynamics of atomically thin materials, thus opening up new avenues for realizing active metasurfaces and robust optoelectronic systems, with potential applications in information processing and communication.

  1. Effective tight-binding models for excitons in branched conjugated molecules

    NASA Astrophysics Data System (ADS)

    Li, Hao; Malinin, Sergey V.; Tretiak, Sergei; Chernyak, Vladimir Y.

    2013-08-01

    Effective tight-binding models have been introduced to describe vertical electronic excitations in branched conjugated molecules. The excited-state electronic structure is characterized by quantum particles (excitons) that reside on an irregular lattice (graph) that reflects the molecular structure. The methodology allows for the exciton spectra and energy-dependent exciton scattering matrices to be described in terms of a small number of lattice parameters which can be obtained from quantum-chemical computations using the exciton scattering approach as a tool. We illustrate the tight-binding model approach using the time-dependent Hartree-Fock computations in phenylacetylene oligomers. The on-site energies and hopping constants have been identified from the exciton dispersion and scattering matrices. In particular, resonant, as well as bound states, are reproduced for a symmetric quadruple branching center. The capability of the tight-binding model approach to describe the exciton-phonon coupling and energetic disorder in large branched conjugated molecules is briefly discussed.

  2. Ultrafast formation of interlayer hot excitons in atomically thin MoS2/WS2 heterostructures

    PubMed Central

    Chen, Hailong; Wen, Xiewen; Zhang, Jing; Wu, Tianmin; Gong, Yongji; Zhang, Xiang; Yuan, Jiangtan; Yi, Chongyue; Lou, Jun; Ajayan, Pulickel M.; Zhuang, Wei; Zhang, Guangyu; Zheng, Junrong

    2016-01-01

    Van der Waals heterostructures composed of two-dimensional transition-metal dichalcogenides layers have recently emerged as a new family of materials, with great potential for atomically thin opto-electronic and photovoltaic applications. It is puzzling, however, that the photocurrent is yielded so efficiently in these structures, despite the apparent momentum mismatch between the intralayer/interlayer excitons during the charge transfer, as well as the tightly bound nature of the excitons in 2D geometry. Using the energy-state-resolved ultrafast visible/infrared microspectroscopy, we herein obtain unambiguous experimental evidence of the charge transfer intermediate state with excess energy, during the transition from an intralayer exciton to an interlayer exciton at the interface of a WS2/MoS2 heterostructure, and free carriers moving across the interface much faster than recombining into the intralayer excitons. The observations therefore explain how the remarkable charge transfer rate and photocurrent generation are achieved even with the aforementioned momentum mismatch and excitonic localization in 2D heterostructures and devices. PMID:27539942

  3. 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.

  4. Probing excitonic states in suspended two-dimensional semiconductors by photocurrent spectroscopy

    DOE PAGES

    Klots, A. R.; Newaz, A. K. M.; Wang, Bin; ...

    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

  5. Spatially indirect excitons in coupled quantum wells

    SciTech Connect

    Lai, Chih-Wei Eddy

    2004-03-01

    Microscopic quantum phenomena such as interference or phase coherence between different quantum states are rarely manifest in macroscopic systems due to a lack of significant correlation between different states. An exciton system is one candidate for observation of possible quantum collective effects. In the dilute limit, excitons in semiconductors behave as bosons and are expected to undergo Bose-Einstein condensation (BEC) at a temperature several orders of magnitude higher than for atomic BEC because of their light mass. Furthermore, well-developed modern semiconductor technologies offer flexible manipulations of an exciton system. Realization of BEC in solid-state systems can thus provide new opportunities for macroscopic quantum coherence research. In semiconductor coupled quantum wells (CQW) under across-well static electric field, excitons exist as separately confined electron-hole pairs. These spatially indirect excitons exhibit a radiative recombination time much longer than their thermal relaxation time a unique feature in direct band gap semiconductor based structures. Their mutual repulsive dipole interaction further stabilizes the exciton system at low temperature and screens in-plane disorder more effectively. All these features make indirect excitons in CQW a promising system to search for quantum collective effects. Properties of indirect excitons in CQW have been analyzed and investigated extensively. The experimental results based on time-integrated or time-resolved spatially-resolved photoluminescence (PL) spectroscopy and imaging are reported in two categories. (i) Generic indirect exciton systems: general properties of indirect excitons such as the dependence of exciton energy and lifetime on electric fields and densities were examined. (ii) Quasi-two-dimensional confined exciton systems: highly statistically degenerate exciton systems containing more than tens of thousands of excitons within areas as small as (10 micrometer)2 were

  6. 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.

  7. Exciton Rydberg series in mono- and few-layer WS2

    NASA Astrophysics Data System (ADS)

    Chernikov, Alexey; Berkelbach, Timothy C.; Hill, Heather M.; Rigosi, Albert; Li, Yilei; Aslan, Özgur B.; Hybertsen, Mark S.; Reichman, David R.; Heinz, Tony F.

    2014-03-01

    Considered a long-awaited semiconducting analogue to graphene, the family of atomically thin transition metal dichalcogenides (TMDs) attracted intense interest in the scientific community due to their remarkable physical properties resulting from the reduced dimensionality. A fundamental manifestation of the two-dimensional nature is a strong increase in the Coulomb interaction. The resulting formation of tightly bound excitons plays a crucial role for a majority of optical and transport phenomena. In our work, we investigate the excitons in atomically thin TMDs by optical micro-spectroscopy and apply a microscopic, ab-initio theoretical approach. We observe a full sequence of excited exciton states, i.e., the Rydberg series, in the monolayer WS2, identifying tightly bound excitons with energies exceeding 0.3 eV - almost an order of magnitude higher than in the corresponding, three-dimensional crystal. We also find significant deviations of the excitonic properties from the conventional hydrogenic physics - a direct evidence of a non-uniform dielectric environment. Finally, an excellent quantitative agreement is obtained between the experimental findings and the developed theoretical approach.

  8. Photoluminescence of localized excitons in ZnCdO thin films grown by molecular beam epitaxy

    NASA Astrophysics Data System (ADS)

    Wu, T. Y.; Huang, Y. S.; Hu, S. Y.; Lee, Y. C.; Tiong, K. K.; Chang, C. C.; Shen, J. L.; Chou, W. C.

    2016-07-01

    We have investigated the luminescence characteristics of Zn1-xCdxO thin films with different Cd contents grown by molecular beam epitaxy system. The temperature-dependent photoluminescence (PL) and excitation power-dependent PL spectra were measured to clarify the luminescence mechanisms of the Zn1-xCdxO thin films. The peak energy of the Zn1-xCdxO thin films with increasing the Cd concentration is observed as redshift and can be fitted by the quadratic function of alloy content. The broadened full-width at half-maximum (FWHM) estimated from the 15 K PL spectra as a function of Cd content shows a larger deviation between the experimental values and theoretical curve, which indicates that experimental FWHM values are affected not only by alloy compositional disorder but also by localized excitons occupying states in the tail of the density of states. The Urbach energy determined from an analysis of the lineshape of the low-energy side of the PL spectrum and the degree of localization effect estimated from the temperature-induced S-shaped PL peak position described an increasing mean exciton-localization effects in ZnCdO films with increasing the Cd content. In addition, the PL intensity and peak position as a function of excitation power are carried out to clarify the types of radiative recombination and the effects of localized exciton in the ZnCdO films with different Cd contents.

  9. Eu(2)(+) -induced enhancement of defect luminescence of ZnS.

    PubMed

    Xiao-Bo, Zhang; Fu-Xiang, Wei

    2016-12-01

    The Eu(2)(+) -induced enhancement of defect luminescence of ZnS was studied in this work. While photoluminescence (PL) spectra exhibited 460 nm and 520 nm emissions in both ZnS and ZnS:Eu nanophosphors, different excitation characteristics were shown in their photoluminescence excitation (PLE) spectra. In ZnS nanophosphors, there was no excitation signal in the PLE spectra at the excitation wavelength λex  > 337 nm (the bandgap energy 3.68 eV of ZnS); while in ZnS:Eu nanophosphors, two excitation bands appeared that were centered at 365 nm and 410 nm. Compared with ZnS nanophosphors, the 520 nm emission in the PL spectra was relatively enhanced in ZnS:Eu nanophosphors and, furthermore, in ZnS:Eu nanophosphors the 460 nm and 520 nm emissions increased more than 10 times in intensity. The reasons for these differences were analyzed. It is believed that the absorption of Eu(2)(+) intra-ion transition and subsequent energy transfer to sulfur vacancy, led to the relative enhancement of the 520 nm emission in ZnS:Eu nanophosphors. In addition, more importantly, Eu(2)(+) acceptor-bound excitons are formed in ZnS:Eu nanophosphors and their excited levels serve as the intermediate state of electronic relaxation, which decreases non-radiative electronic relaxation and thus increases the intensity of the 460 nm and 520 nm emission dramatically. In summary, the results in this work indicate a new mechanism for the enhancement of defect luminescence of ZnS in Eu(2)(+) -doped ZnS nanophosphors. Copyright © 2016 John Wiley & Sons, Ltd. Copyright © 2016 John Wiley & Sons, Ltd.

  10. Coherent exciton-polariton devices

    NASA Astrophysics Data System (ADS)

    Fraser, Michael D.

    2017-09-01

    The Bose-Einstein condensate of exciton-polaritons has emerged as a unique, coherent system for the study of non-equilibrium, macroscopically coherent Bose gases, while the full confinement of this coherent state to a semiconductor chip has also generated considerable interest in developing novel applications employing the polariton condensate, possibly even at room temperature. Such devices include low-threshold lasers, precision inertial sensors, and circuits based on superfluidity with ultra-fast non-linear elements. While the demonstration and development of such devices are at an early stage, rapid progress is being made. In this review, an overview of the exciton-polariton condensate system and the established and emerging material systems and fabrication techniques are presented, followed by a critical, in-depth assessment of the ability of the coherent polariton system to deliver on its promise of devices offering either new functionality and/or room-temperature operation.

  11. Electronic absorption of Frenkel excitons in topologically disordered systems

    NASA Astrophysics Data System (ADS)

    Schweizer, Kenneth S.

    1986-10-01

    A self-consistent effective medium theory of the electronic absorption spectra of tightly bound dipolar excitons in simple fluids is developed within the adiabatic picture. The theoretical approach is based on the isomorphism between the path-integral formulation of quantum theory and classical statistical mechanics and is an extension of previous work [D. Chandler, K. S. Schweizer, and P. G. Wolynes, Phys. Rev. Lett. 49, 1100 (1982)]. The consequences of fluid structural disorder on resonant excitation transfer and the statistical fluctuations of single molecule energy levels are simultaneously treated. Detailed numerical calculations are performed to establish the dependence of the absorption spectrum on fluid density, short range order, and the relative magnitude of the resonant transfer vs the single site disorder. The density dependence of the spectral features are found to be a sensitive function of fluid structure and the relative strength of the localizing vs the delocalizing interactions. By comparing the liquid state results with the corresponding crystalline solid behavior, the consequences of topological disorder on the exciton spectrum are identified. The relevance of the theoretical predictions to spectroscopic probes of exciton delocalization in molecular liquids and glasses is discussed.

  12. Exciton-polariton integrated circuits

    NASA Astrophysics Data System (ADS)

    Liew, T. C. H.; Kavokin, A. V.; Ostatnický, T.; Kaliteevski, M.; Shelykh, I. A.; Abram, R. A.

    2010-07-01

    We show that logical signals encoded in bistable states in semiconductor microcavities can be generated and controlled electronically by exploiting the electrical sensitivity of Tamm-plasmon-exciton-polariton modes. The signals can be transported along polariton neurons, created with a patterned metal surface. Using the Gross-Pitaevskii equations, we simulate an electrically controlled transistor and find that high repetition rates (10 GHz) are possible.

  13. Exciton Seebeck effect in molecular systems.

    PubMed

    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.

  14. 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.

  15. Excitonic-type polaron states: photoluminescence in SBN and in other ferroelectric oxides

    NASA Astrophysics Data System (ADS)

    Vikhnin, V. S.; Kislova, I.; Kutsenko, A. B.; Kapphan, S. E.

    2002-07-01

    A theoretical model for two characteristic photoluminescence (PL) bands in SBN, 'green luminescence' and 'red luminescence' is proposed on the basis of the extended photoluminescence experiments in SBN:Cr, and also in SBN:Ce and in nominally pure SBN systems under different conditions. While the RL-band is suggested to be connected with charge transfer vibronic exciton (CTVE) clusters induced by Cr3+ impurities in the Nb-sites, the GL- band is connected with Nb4+ electronic polarons in a new, charge transfer excited states. Here Nb4+ centers are the cores of the CTVE clusters induced by these charged scores. The PL mechanism is the in-cluster CTVE recombination for both bands under discussion. But the CTVE states are quasi-resonantly mixed here with 4T2 states of the Cr3+ core in the RL-band case, and with 5s-states of the Nb4+ core in the GL-band case. The role of excitonic polarons of CTVE nature is also discussed in connection with 'green' luminescence origin in KTaO3 and KNbO3 crystals.

  16. Metal-Semiconductor Nanoparticle Hybrids Formed by Self-Organization: A Platform to Address Exciton-Plasmon Coupling.

    PubMed

    Strelow, Christian; Theuerholz, T Sverre; Schmidtke, Christian; Richter, Marten; Merkl, Jan-Philip; Kloust, Hauke; Ye, Ziliang; Weller, Horst; Heinz, Tony F; Knorr, Andreas; Lange, Holger

    2016-08-10

    Hybrid nanosystems composed of excitonic and plasmonic constituents can have different properties than the sum of of the two constituents, due to the exciton-plasmon interaction. Here, we report on a flexible model system based on colloidal nanoparticles that can form hybrid combinations by self-organization. The system allows us to tune the interparticle distance and to combine nanoparticles of different sizes and thus enables a systematic investigation of the exciton-plasmon coupling by a combination of optical spectroscopy and quantum-optical theory. We experimentally observe a strong influence of the energy difference between exciton and plasmon, as well as an interplay of nanoparticle size and distance on the coupling. We develop a full quantum theory for the luminescence dynamics and discuss the experimental results in terms of the Purcell effect. As the theory describes excitation as well as coherent and incoherent emission, we also consider possible quantum optical effects. We find a good agreement of the observed and the calculated luminescence dynamics induced by the Purcell effect. This also suggests that the self-organized hybrid system can be used as platform to address quantum optical effects.

  17. Distinct exciton dissociation behavior of organolead trihalide perovskite and excitonic semiconductors studied in a same device

    DOE PAGES

    Hu, Miao; Bi, Cheng; Yuan, Yongbo; ...

    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.

  18. Distinct exciton dissociation behavior of organolead trihalide perovskite and excitonic semiconductors studied in the same system.

    PubMed

    Hu, Miao; Bi, Cheng; Yuan, Yongbo; Xiao, Zhengguo; Dong, Qingfeng; Shao, Yuchuan; Huang, Jinsong

    2015-05-13

    The nonexcitonic character for organometal trihalide perovskites is demonstrated by examining the field-dependent exciton dissociation behavior. 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.

  19. Distinct exciton dissociation behavior of organolead trihalide perovskite and excitonic semiconductors studied in a same device

    SciTech Connect

    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.

  20. Excitons in solids with non-empirical hybrid time-dependent density-functional theory

    NASA Astrophysics Data System (ADS)

    Ullrich, Carsten; Yang, Zeng-Hui; Sottile, Francesco

    2015-03-01

    The Bethe-Salpeter equation (BSE) accurately describes the optical properties of solids, but is computationally expensive. Time-dependent density-functional theory (TDDFT) is more efficient, but standard functionals do not produce excitons in extended systems. We present a new, non-empirical hybrid TDDFT approach whose computational cost is much less than BSE, while the accuracy for both bound excitons and the continuum spectra is comparable to that of the BSE. Good performance is observed for both small-gap semiconductors and large-gap insulators. Work supported by NSF Grant DMR-1408904.

  1. 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.

  2. Ballistic spin transport in exciton gases

    NASA Astrophysics Data System (ADS)

    Kavokin, A. V.; Vladimirova, M.; Jouault, B.; Liew, T. C. H.; Leonard, J. R.; Butov, L. V.

    2013-11-01

    Traditional spintronics relies on spin transport by charge carriers, such as electrons in semiconductor crystals. The challenges for the realization of long-range electron spin transport include rapid spin relaxation due to electron scattering. Scattering and, in turn, spin relaxation can be effectively suppressed in excitonic devices where the spin currents are carried by electrically neutral bosonic quasiparticles: excitons or exciton-polaritons. They can form coherent quantum liquids that carry spins over macroscopic distances. The price to pay is a finite lifetime of the bosonic spin carriers. We present the theory of exciton ballistic spin transport which may be applied to a range of systems supporting bosonic spin transport, in particular to indirect excitons in coupled quantum wells. We describe the effect of spin-orbit interaction for the electron and the hole on the exciton spin, account for the Zeeman effect induced by external magnetic fields and long-range and short-range exchange splittings of the exciton resonances. We also consider exciton transport in the nonlinear regime and discuss the definitions of the exciton spin current, polarization current, and spin conductivity.

  3. Scattering amplitudes for dark and bright excitons

    NASA Astrophysics Data System (ADS)

    Shiau, Shiue-Yuan; Combescot, Monique; Combescot, Roland; Dubin, François; Chang, Yia-Chung

    2017-05-01

    Using the composite boson many-body formalism that takes single-exciton states rather than free carrier states as a basis, we derive the integral equation fulfilled by the exciton-exciton effective scattering from which the role of fermion exchanges can be unraveled. For excitons made of (+/-1/2) -spin electrons and (+/-3/2) -spin holes, as in GaAs heterostructures, one major result is that most spin configurations lead to brightness-conserving scatterings with equal amplitude Δ, despite differences in the carrier exchanges involved. A brightness-changing channel also exists when two opposite-spin excitons scatter: dark excitons (2,-2) can end either in the same dark states with an amplitude Δe , or in opposite-spin bright states (1,-1) , with a different amplitude Δo , the number of carrier exchanges involved in these scatterings being even or odd, respectively. Another major result is that these amplitudes are linked by a striking relation, Δ_e+Δ_o=Δ , which has decisive consequence on exciton Bose-Einstein condensation. By using Born values, we show that the exciton condensate can be optically observed through a bright part when excitons have large dipole only, that is, when the electrons and holes are in two well-separated layers, as in current experiments.

  4. 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.

  5. Field-induced exciton dissociation in PTB7-based organic solar cells

    NASA Astrophysics Data System (ADS)

    Gerhard, Marina; Arndt, Andreas P.; Bilal, Mühenad; Lemmer, Uli; Koch, Martin; Howard, Ian A.

    2017-05-01

    The physics of charge separation in organic semiconductors is a topic of ongoing research of relevance to material and device engineering. Herein, we present experimental observations of the field and temperature dependence of charge separation from singlet excitons in PTB7 and PC71BM , and from charge-transfer states created across interfaces in PTB 7 /PC71BM bulk heterojunction solar cells. We obtain this experimental data by time-resolving the near infrared emission of the states from 10 K to room temperature and electric fields from 0 to 2.5 MVcm -1 . Examining how the luminescence is quenched by field and temperature gives direct insight into the underlying physics. We observe that singlet excitons can be split by high fields, and that disorder broadens the high threshold fields needed to split the excitons. Charge-transfer (CT) states, on the other hand, can be separated by both field and temperature. Also, the data imply a strong reduction of the activation barrier for charge splitting from the CT state relative to the exciton state. The observations provided herein of the field-dependent separation of CT states as a function of temperature offer a rich data set against which theoretical models of charge separation can be rigorously tested; it should be useful for developing the more advanced theoretical models of charge separation.

  6. Excitonic recombinations in h-BN: From bulk to exfoliated layers

    NASA Astrophysics Data System (ADS)

    Pierret, A.; Loayza, J.; Berini, B.; Betz, A.; Plaçais, B.; Ducastelle, F.; Barjon, J.; Loiseau, A.

    2014-01-01

    Hexagonal boron nitride (h-BN) and graphite are structurally similar but with very different properties. Their combination in graphene-based devices is now of intense research focus, and it becomes particularly important to evaluate the role played by crystalline defects on their properties. In this paper, the cathodoluminescence (CL) properties of hexagonal boron nitride crystallites are reported and compared to those of nanosheets mechanically exfoliated from them. First, the link between the presence of structural defects and the recombination intensity of trapped excitons, the so-called D series, is confirmed. Low defective h-BN regions are further evidenced by CL spectral mapping (hyperspectral imaging), allowing us to observe new features in the near-band-edge region, tentatively attributed to phonon replicas of exciton recombinations. Second, the h-BN thickness was reduced down to six atomic layers, using mechanical exfoliation, as evidenced by atomic force microscopy. Even at these low thicknesses, the luminescence remains intense and exciton recombination energies are not strongly modified with respect to the bulk, as expected from theoretical calculations, indicating extremely compact excitons in h-BN.

  7. Luminescence of CdSe quantum dots near a layer of silver nanoparticles ion-synthesized in sapphire

    NASA Astrophysics Data System (ADS)

    Galyametdinov, Yu. G.; Shamilov, R. R.; Nuzhdin, V. I.; Valeev, V. F.; Stepanov, A. L.

    2016-11-01

    We study the characteristics of the luminescence of composite films based on polymethyl methacrylate with CdSe quantum dots deposited from solution onto the surface of a sapphire substrate containing a preliminarily formed layer with ion-synthesized silver nanoparticles. The sapphire layer with silver nanoparticles exhibits selective plasmon absorption in the visible spectral range with a peak at 463 nm. Enhancement in the exciton luminescence intensity of quantum dots with a peak at 590 nm is observed upon excitation at wavelengths lying in the region of plasmon resonance of metal nanoparticles, as well as luminescence quenching for quantum dots located in the vicinity of silver nanoparticles.

  8. Temperature dependence of the fundamental excitonic resonance in lead-salt quantum dots

    SciTech Connect

    Yue, Fangyu; Tomm, Jens W.; Kruschke, Detlef; Chu, Junhao

    2015-07-13

    The temperature dependences of the fundamental excitonic resonance in PbS and PbSe quantum dots fabricated by various technologies are experimentally determined. Above ∼150 K, sub-linearities of the temperature shifts and halfwidths are observed. This behavior is analyzed within the existing standard models. Concordant modeling, however, becomes possible only within the frame of a three-level system that takes into account both bright and dark excitonic states as well as phonon-assisted carrier redistribution between these states. Our results show that luminescence characterization of lead-salt quantum dots necessarily requires both low temperatures and excitation densities in order to provide reliable ensemble parameters.

  9. Polymerization-enhanced intersystem crossing: new strategy to achieve long-lived excitons.

    PubMed

    Sun, Xingxing; Wang, Xijun; Li, Xinyang; Ge, Jing; Zhang, Qun; Jiang, Jun; Zhang, Guoqing

    2015-02-01

    For a singlet-triplet coupled molecular system, the efficiency of forward and reverse intersystem crossing processes can be enhanced by reducing the energy gap between the singlet and triplet excited states (ΔEST ), thus prolonging the exciton lifetimes. This has been proven beneficial for many emerging applications such as molecular luminescence, optoelectronics, and photonics. Here, a strategy is proposed to create small ΔEST by polymerizing fluorescent dye molecules, the efficacy of which is justified by density functional theory calculations and ultrafast spectroscopy. Thus, singlet-triplet exciton communication through polymerization-enhanced intersystem crossing is also proposed. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  10. The Effects of Aging on the Luminescence of PEG-Coated Water-Soluble ZnO Nanoparticles Solutions

    SciTech Connect

    Woo, Boon K.; Chen, Wei; Joly, Alan G.; Sammynaiken, Ramaswami

    2008-09-18

    Water-soluble ZnOnanoparticles coated with polyethylene glycol biscarboxymethyl (PEG(COOH)2)were prepared in ethanol/water solutions. The ZnOnanoparticles have a hexagonal structure with an average size of 10 nm. Three different luminescence bands are observed from the nanoparticle solutions: green emission at 530 nm from surface states or defects, UV emission at 380 nm from the ZnOexcitons, and an emission band at around 338 nm from the PEG(COOH)2. The fresh as-prepared samples have very strong green emission at 530 nm from surface states or defects but very weak excitonic emission at 380 nm. After dilution with ethanol, the green emission decreases in intensity and the excitonic emission increases. In the diluted samples, the excitonic luminescence intensity increases with storage time. This intensity increase is attributed to surface passivation by CH3COO-ligands resulting from precursor reactions in the ethanol solvent.

  11. 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.

  12. Observation of forbidden phonons, Fano resonance and dark excitons by resonance Raman scattering in few-layer WS2

    NASA Astrophysics Data System (ADS)

    Tan, Qing-Hai; Sun, Yu-Jia; Liu, Xue-Lu; Zhao, Yanyuan; Xiong, Qihua; Tan, Ping-Heng; Zhang, Jun

    2017-09-01

    The optical properties of the two-dimensional (2D) crystals are dominated by tightly bound electron-hole pairs (excitons) and lattice vibration modes (phonons). The exciton-phonon interaction is fundamentally important to understand the optical properties of 2D materials and thus helps to develop emerging 2D crystal based optoelectronic devices. Here, we presented the excitonic resonant Raman scattering (RRS) spectra of few-layer WS2 excited by 11 lasers lines covered all of A, B and C exciton transition energies at different sample temperatures from 4 to 300 K. As a result, we are not only able to probe the forbidden phonon modes unobserved in ordinary Raman scattering, but also can determine the bright and dark state fine structures of 1s A exciton. In particular, we also observed the quantum interference between low-energy discrete phonon and exciton continuum under resonant excitation. Our works pave a way to understand the exciton-phonon coupling and many-body effects in 2D materials.

  13. Generation of Multiple Excitons in Ag2S Quantum Dots: Single High-Energy versus Multiple-Photon Excitation.

    PubMed

    Sun, Jingya; Yu, Weili; Usman, Anwar; Isimjan, Tayirjan T; DGobbo, Silvano; Alarousu, Erkki; Takanabe, Kazuhiro; Mohammed, Omar F

    2014-02-20

    We explored biexciton generation via carrier multiplication (or multiple-exciton generation) by high-energy photons and by multiple-photon absorption in Ag2S quantum dots (QDs) using femtosecond broad-band transient absorption spectroscopy. Irrespective of the size of the QDs and how the multiple excitons are generated in the Ag2S QDs, two distinct characteristic time constants of 9.6-10.2 and 135-175 ps are obtained for the nonradiative Auger recombination of the multiple excitons, indicating the existence of two binding excitons, namely, tightly bound and weakly bound excitons. More importantly, the lifetimes of multiple excitons in Ag2S QDs were about 1 and 2 orders of magnitude longer than those of comparable size PbS QDs and single-walled carbon nanotubes, respectively. This result is significant because it suggests that by utilizing an appropriate electron acceptor, there is a higher possibility to extract multiple electron-hole pairs in Ag2S QDs, which should improve the performance of QD-based solar cell devices.

  14. Impurity trapped exciton states related to rare earth ions in crystals under high hydrostatic pressure

    SciTech Connect

    Grinberg, M. Mahlik, S.

    2013-01-15

    Emission related to rare earth ions in solids takes place usually due to 4f{sup n} {yields} 4f{sup n} and 4f{sup n-1}5d{sup 1} {yields} 4f{sup n} internal transitions. In the case of band to band excitation the effective energy transfer from the host to optically active impurity is required. Among other processes one of the possibilities is capturing of the electron at excited state and hole at the ground state of impurity. Localization of electron or hole at the dopand site creates a long range Coulomb potential that attracts the second carrier which then occupies the localized Rydberg-like states. Such a system can be considered as impurity trapped exciton. Usually impurity trapped exciton is a short living phenomenon which decays non-radiatively leaving the impurity ion in the excited state. However, in several compounds doped with Eu{sup 2+} the impurity trapped exciton states become stable and contribute to the radiative processes though anomalous luminescence that appears apart of the 4f{sup 7} {yields} 4f{sup 7} and 4f{sup 7}5d{sup 1} {yields} 5f{sup 7} emission. In this contribution pressure effect on energies of the 4f{sup n-1}5d{sup 1}{yields}5f{sup n} transitions in Ln doped oxides and fluorides as well as influence of pressure on the energy of impurity trapped exciton states is discussed. The latest results on high pressure investigations of luminescence related to Pr{sup 3+}, and Eu{sup 2+} in different lattices are reviewed.

  15. Exciton dynamics at a single dislocation in GaN probed by picosecond time-resolved cathodoluminescence

    SciTech Connect

    Liu, W. E-mail: gwenole.jacopin@epfl.ch; Carlin, J.-F.; Grandjean, N.; Deveaud, B.; Jacopin, G. E-mail: gwenole.jacopin@epfl.ch

    2016-07-25

    We investigate the dynamics of donor bound excitons (D°X{sub A}) at T = 10 K around an isolated single edge dislocation in homoepitaxial GaN, using a picosecond time-resolved cathodoluminescence (TR-CL) setup with high temporal and spatial resolutions. An ∼ 1.3 meV dipole-like energy shift of D°X{sub A} is observed around the dislocation, induced by the local strain fields. By simultaneously recording the variations of both the exciton lifetime and the CL intensity across the dislocation, we directly assess the dynamics of excitons around the defect. Our observations are well reproduced by a diffusion model. It allows us to deduce an exciton diffusion length of ∼24 nm as well as an effective area of the dislocation with a radius of ∼95 nm, where the recombination can be regarded as entirely non-radiative.

  16. Exciton photoluminescence and energy in a percolation cluster of ZnSe quantum dots as a fractal object

    SciTech Connect

    Bondar, N. V. Brodyn, M. S.

    2012-05-15

    The results of studies of samples containing ZnSe quantum dots with a density corresponding to or considerably higher than the exciton percolation threshold, at which quantum dots form conglomerates, are reported. Excitonic emission from a percolation cluster of bound quantum dots as a fractal object is observed for the first time. Analysis of the structure of the photoluminescence spectra shows that the spectra are determined by the contribution of exciton states that belong to different structural elements of the percolation cluster, specifically, to the skeleton (backbone), dangling (dead) ends, and internal hollow spaces. A qualitative model is proposed to interpret the dependence of the exciton energy in these structural elements on the concentration of quantum dots in the material.

  17. Cavity-less on-chip optomechanics using excitonic transitions in semiconductor heterostructures

    PubMed Central

    Okamoto, Hajime; Watanabe, Takayuki; Ohta, Ryuichi; Onomitsu, Koji; Gotoh, Hideki; Sogawa, Tetsuomi; Yamaguchi, Hiroshi

    2015-01-01

    The hybridization of semiconductor optoelectronic devices and nanomechanical resonators provides a new class of optomechanical systems in which mechanical motion can be coupled to light without any optical cavities. Such cavity-less optomechanical systems interconnect photons, phonons and electrons (holes) in a highly integrable platform, opening up the development of functional integrated nanomechanical devices. Here we report on a semiconductor modulation-doped heterostructure–cantilever hybrid system, which realizes efficient cavity-less optomechanical transduction through excitons. The opto-piezoelectric backaction from the bound electron–hole pairs enables us to probe excitonic transition simply with a sub-nanowatt power of light, realizing high-sensitivity optomechanical spectroscopy. Detuning the photon energy from the exciton resonance results in self-feedback cooling and amplification of the thermomechanical motion. This cavity-less on-chip coupling enables highly tunable and addressable control of nanomechanical resonators, allowing high-speed programmable manipulation of nanomechanical devices and sensor arrays. PMID:26477487

  18. Cavity-less on-chip optomechanics using excitonic transitions in semiconductor heterostructures.

    PubMed

    Okamoto, Hajime; Watanabe, Takayuki; Ohta, Ryuichi; Onomitsu, Koji; Gotoh, Hideki; Sogawa, Tetsuomi; Yamaguchi, Hiroshi

    2015-10-19

    The hybridization of semiconductor optoelectronic devices and nanomechanical resonators provides a new class of optomechanical systems in which mechanical motion can be coupled to light without any optical cavities. Such cavity-less optomechanical systems interconnect photons, phonons and electrons (holes) in a highly integrable platform, opening up the development of functional integrated nanomechanical devices. Here we report on a semiconductor modulation-doped heterostructure-cantilever hybrid system, which realizes efficient cavity-less optomechanical transduction through excitons. The opto-piezoelectric backaction from the bound electron-hole pairs enables us to probe excitonic transition simply with a sub-nanowatt power of light, realizing high-sensitivity optomechanical spectroscopy. Detuning the photon energy from the exciton resonance results in self-feedback cooling and amplification of the thermomechanical motion. This cavity-less on-chip coupling enables highly tunable and addressable control of nanomechanical resonators, allowing high-speed programmable manipulation of nanomechanical devices and sensor arrays.

  19. 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.

  20. Exciton spectrum in two-dimensional transition metal dichalcogenides: The role of Diracness

    NASA Astrophysics Data System (ADS)

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

    2017-06-01

    The physics of excitons, electron-hole pairs that are bound together by their mutual Coulomb attraction, can to great extent be understood in the framework of the quantum-mechanical hydrogen model. This model has recently been challenged by spectroscopic measurements on two-dimensional transition-metal dichalchogenides that unveil strong deviations from a hydrogenic spectrum. Here, we show that this deviation is due to the particular relativistic character of electrons in this class of materials. Indeed, their electrons are no longer described in terms of a Schrödinger but a massive Dirac equation that intimately links electrons to holes. Dirac excitons therefore inherit a relativistic quantum spin-1/2 that contributes to the angular momentum and thus the exciton spectrum. Most saliently, the level spacing is strongly reduced as compared to the hydrogen model, in agreement with spectroscopic measurements and ab-initio calculations.

  1. Luminescence quenching of a phosphorescent conjugated polyelectrolyte.

    PubMed

    Haskins-Glusac, Ksenija; Pinto, Mauricio R; Tan, Chunyan; Schanze, Kirk S

    2004-11-17

    The photophysical and luminescence quenching properties of a platinum(II) acetylide-based conjugated polyelectrolyte, Pt-p, which features carboxylic acid solubilizing groups are reported. The Pt-acetylide polymer is water soluble, and it exhibits phosphorescence from a triplet pi,pi exciton based on the conjugated backbone. The phosphorescence from Pt-p is quenched by viologens with different charges (MV(+), MV(2+), and MV(4+)), and in each case the quenching is dominated by a dynamic (diffusional) mechanism. Comparison of the Stern-Volmer quenching properties of Pt-p with those of a structurally analogous fluorescent organic polyelectrolyte leads to the conclusion that the amplified quenching effect, which is commonly observed for fluorescent conjugated polyelectrolytes, is not important for the platinum acetylide phosphorescent conjugated polyelectrolyte.

  2. 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.

  3. Exciton-polaritons condensate in a microwire

    NASA Astrophysics Data System (ADS)

    Kamoun, O.; Jaziri, S.

    2013-12-01

    Recently, polariton condensation has been claimed in microwires. Numerical solutions of the time-dependent Gross-Pitaevskii equation that describes the behavior of the condensate in a trap and exciton-polariton interaction, have been obtained. In this work we study theoretically exciton-polariton one dimensional condensation in several quantized states.

  4. Effects of excitons on solar cells

    NASA Astrophysics Data System (ADS)

    Zhang, Yong; Mascarenhas, Angelo; Deb, Satyen

    1998-10-01

    We have studied the effects of excitons on the two key parameters of a Si solar cell: the dark-saturation current and short-circuit current. We have found that the effect of excitons on the dark-saturation current is very sensitive to the boundary condition for excess excitons at the edge of the depletion region. With the assumption of near equilibrium between the electrons and excitons, we find that the exciton effect is rather small, which is contrary to the conclusion of significant reduction in the dark-saturation current made in previous work with the assumption of no excess excitons at the edge [J. Appl. Phys. 79, 195 (1996)]. The results for the short-circuit current are very similar to the previous work. However, the analytical results for the carrier concentrations and the corresponding currents are now presented in a simple way in which the physical meaning of each individual term is elucidated or revealed. Furthermore, we have found, for practical purposes, very accurate approximate solutions for the carrier concentrations and corresponding currents. Our conclusion is that the major effect of excitons on the Si solar cell performance relies on whether the effective diffusion length (L1) of the coupled electron-exciton system is significantly greater than that of the electron itself (Le).

  5. DNA-mediated excitonic upconversion FRET switching

    DOE PAGES

    Kellis, Donald L.; Rehn, Sarah M.; Cannon, Brittany L.; ...

    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

  6. The specifics of radiative annihilation of self-trapped excitons in a KI-Tl crystal under low-temperature deformation

    NASA Astrophysics Data System (ADS)

    Shunkeyev, K. Sh.; Zhanturina, N. N.; Aimaganbetova, Z. K.; Barmina, A. A.; Myasnikova, L. N.; Sagymbaeva, Sh. Zh.; Sergeyev, D. M.

    2016-07-01

    The effect of low-temperature uniaxial deformation on the self-trapping-limited mean free path of excitons in a KI-Tl crystal was revealed from x-ray luminescence spectra. The analysis of the dependence of the intensity ratio of the Tl-center emission (2.85 eV) and the luminescence of self-trapped excitons (π-component; 3.3 eV) on the extent of low-temperature deformation showed that in the KI-Tl crystal (3 × 10-3 mol. %) the self-trapping-limited mean free path of excitons is comparable with the distance between Tl atoms (20-27)a under a deformation ɛ = 2%. As the compression increases to ɛ ≥ 2%-5%, the mean free path drops to (27-5.35)a. The results of modeling based on the continuum approximation showed that with increasing temperature and the degree of low-temperature deformation the height of the potential barrier for the exciton self-trapping drops, which is consistent with the reduction of the mean free path of excitons in the KI-Tl crystal.

  7. Excitonic and electron-hole processes in NaCl and NaCl:Ag crystals under conditions of multiplication of electronic excitations

    NASA Astrophysics Data System (ADS)

    Feldbach, E.; Kirm, M.; Lushchik, A.; Lushchik, Ch; Martinson, I.

    2000-03-01

    The excitation spectra of icons/Journals/Common/pi" ALT="pi" ALIGN="TOP"/> and icons/Journals/Common/sigma" ALT="sigma" ALIGN="TOP"/> emissions of self-trapped excitons (3.4 eV and 5.4 eV, respectively) as well as the excitation spectra of 5.17 eV luminescence of Ag+ impurity centres were measured in NaCl and NaCl:Ag crystals using synchrotron radiation of 5 - 38 eV. Fast and slow components of these emissions were detected. An analysis of the differences in the excitation spectra measured at 8 and 295 K allowed us to separate the excitonic and electron-hole (e-h) mechanisms of the multiplication of electronic excitations. A photon of 17 - 19 eV forms an e-h pair and a secondary exciton, while the absorption of a 21 - 27 eV photon causes the creation of two e-h pairs. Using luminescent and photoelectric methods, it was shown that a 2p3s Na+ cation exciton, formed at the absorption of a 33.4 eV photon, decays with the creation of an anion exciton with a 3p hole component and two e-h pairs. Three e-h pairs are formed after the absorption of a 31 eV photon by a chlorine ion.

  8. Luminous butterflies: efficient exciton harvesting by benzophenone derivatives for full-color delayed fluorescence OLEDs.

    PubMed

    Lee, Sae Youn; Yasuda, Takuma; Yang, Yu Seok; Zhang, Qisheng; Adachi, Chihaya

    2014-06-16

    Butterfly-shaped luminescent benzophenone derivatives with small energy gaps between their singlet and triplet excited states are used to achieve efficient full-color delayed fluorescence. Organic light-emitting diodes (OLEDs) with these benzophenone derivatives doped in the emissive layer can generate electroluminescence ranging from blue to orange-red and white, with maximum external quantum efficiencies of up to 14.3%. Triplet excitons are efficiently harvested through delayed fluorescence channels. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  9. First-principles calculations of the self-trapped exciton in crystalline NaCl

    SciTech Connect

    Perebeinos, Vasili; Allen, Philip B.; Weinert, M.

    2000-11-15

    The atomic and electronic structure of the lowest triplet state of the off-center (C{sub 2v} symmetry) self-trapped exciton in crystalline NaCl is calculated using the local-spin-density (LSDA) approximation. In addition, the Franck-Condon broadening of the luminescence peak and the a{sub 1g}{yields}b{sub 3u} absorption peak are calculated and compared to experiment. LSDA accurately predicts transition energies if the initial and final states are both localized or delocalized, but 1 eV discrepancies with experiment occur if one state is localized and the other is delocalized.

  10. Single-Molecule Investigation of Energy Dynamics in a Coupled Plasmon-Exciton System

    NASA Astrophysics Data System (ADS)

    Imada, Hiroshi; Miwa, Kuniyuki; Imai-Imada, Miyabi; Kawahara, Shota; Kimura, Kensuke; Kim, Yousoo

    2017-07-01

    We investigate the near-field interaction between an isolated free-base phthalocyanine molecule and a plasmon localized in the gap between an NaCl-covered Ag(111) surface and the tip apex of a scanning tunneling microscope. When the tip is located in the close proximity of the molecule, asymmetric dips emerge in the broad luminescence spectrum of the plasmon generated by the tunneling current. The origin of the dips is explained by energy transfer between the plasmon and molecular excitons and a quantum mechanical interference effect, where molecular vibrations provide additional degrees of freedom in the dynamic process.

  11. Excitonic magnetism in d6 perovskites

    NASA Astrophysics Data System (ADS)

    Afonso, J. Fernández; Kuneš, J.

    2017-03-01

    We use the LDA+U method to study the possibility of exciton condensation in perovskites of transition metals with the d6 electronic configuration such as LaCoO3. For realistic interaction parameters we find several distinct solutions exhibiting a spin-triplet exciton condensate, which gives rise to a local spin density distribution while the ordered moments are vanishingly small. Rhombohedral distortion from the ideal cubic structure suppresses the ordered state, contrary to the spin-orbit coupling which enhances the excitonic condensation energy. We explain the trends observed in the numerical simulations with the help of a simplified strong-coupling model. Our results indicate that LaCoO3 is close to the excitonic instability and suggest ways how to achieve the exciton condensation.

  12. 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.

  13. Exciton binding energy in semiconductor quantum dots

    SciTech Connect

    Pokutnii, S. I.

    2010-04-15

    In the adiabatic approximation in the context of the modified effective mass approach, in which the reduced exciton effective mass {mu} = {mu}(a) is a function of the radius a of the semiconductor quantum dot, an expression for the exciton binding energy E{sub ex}(a) in the quantum dot is derived. It is found that, in the CdSe and CdS quantum dots with the radii a comparable to the Bohr exciton radii a{sub ex}, the exciton binding energy E{sub ex}(a) is substantially (respectively, 7.4 and 4.5 times) higher than the exciton binding energy in the CdSe and CdS single crystals.

  14. Calculating excitons, plasmons, and quasiparticles in 2D materials and van der Waals heterostructures

    NASA Astrophysics Data System (ADS)

    Sommer Thygesen, Kristian

    2017-06-01

    Atomically thin two-dimensional (2D) materials host a rich set of electronic states that differ substantially from those of their bulk counterparts due to quantum confinement and enhanced many-body effects. This Topical Review focuses on the theory and computation of excitons, plasmons and quasiparticle band structures in 2D materials and their heterostructures. The general theory is illustrated by applications to various types of 2D materials including transition metal dichalcogenides, graphene, phosphorene, and hexagonal boron nitride. The weak and highly non-local dielectric function of atomically thin crystals is shown to be responsible for many of the unique properties exhibited by the 2D materials such as the formation of strongly bound, non-Hydrogenic excitons, large band gap renormalization effects, and the different signatures of excitons and plasmons in electron energy loss spectroscopy (EELS). Among other topics covered are spin-orbit coupling, trions, interlayer excitons, exciton dissociation, and environmental screening. Technical issues associated with the application of the many-body GW method and the Bethe-Salpeter equation (BSE) to 2D materials are also discussed. A combined quantum/classical method is introduced and used throughout to account for dielectric screening and self-energy effects from substrates and van der Waals heterostructures including the difficult case of non-matching lattices.

  15. Dynamic Monte Carlo modeling of exciton dissociation in organic donor-acceptor solar cells.

    PubMed

    Heiber, Michael C; Dhinojwala, Ali

    2012-07-07

    A general dynamic Monte Carlo model for exciton dissociation at a donor-acceptor interface that includes exciton delocalization and hot charge separation is developed to model the experimental behavior observed for the poly(3-hexylthiophene):fullerene system and predict the theoretical performance of future materials systems. The presence of delocalized excitons and the direct formation of separated charge pairs has been recently measured by transient photo-induced absorption experiments and has been proposed to facilitate charge separation. The excess energy of the exciton dissociation process has also been observed to have a strong correlation with the charge separation yield for a series of thiophene based polymer:fullerene systems, suggesting that a hot charge separation process is also occurring. Hot charge separation has been previously theorized as a cause for highly efficient charge separation. However, a detailed model for this process has not been implemented and tested. Here, both conceptual models are implemented into a dynamic Monte Carlo simulation and tested using a simple bilayer donor-acceptor system. We find that exciton delocalization can account for a significant reduction in geminate recombination when compared to the traditional, bound polaron pair model. In addition, the hot charge separation process could further reduce the geminate recombination, but only if the hot charge mobility is several orders of magnitude larger than the standard charge mobility.

  16. 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.

  17. Spectrum of a lattice exciton in a transverse magnetic field: Emergence of full translational symmetry

    NASA Astrophysics Data System (ADS)

    Berciu, Mona

    2014-06-01

    We show that even in the presence of a transverse magnetic field, the eigenstates of an exciton remain invariant to the full lattice translation group. This is expected if the exciton is viewed as a neutral quasiparticle, but not if one views it as a bound electron-hole pair. Single electron and hole wave functions are invariant only to the magnetic translation group, and their momenta are restricted to the magnetic Brillouin zone; the associated folding is the origin of their Hofstadter butterfly spectra. We find that such folding is not necessary for exciton eigenstates, which are characterized by momenta in the full Brillouin zone and thus have higher symmetry than the Hamiltonian. The magnetic field can have a significant effect on the shape of the exciton dispersion, however. While similar effects have been noted in continuous models, we find qualitatively different behavior for Frenkel excitons, whose origin we clarify. We also derive an analytical solution for the Hofstadter butterfly on a square lattice and analyze its dispersion in the full Brillouin zone.

  18. Ultrafast exciton migration in an HJ-aggregate: Potential surfaces and quantum dynamics

    NASA Astrophysics Data System (ADS)

    Binder, Robert; Polkehn, Matthias; Ma, Tianji; Burghardt, Irene

    2017-01-01

    Quantum dynamical and electronic structure calculations are combined to investigate the mechanism of exciton migration in an oligothiophene HJ aggregate, i.e., a combination of oligomer chains (J-type aggregates) and stacked aggregates of such chains (H-type aggregates). To this end, a Frenkel exciton model is parametrized by a recently introduced procedure [Binder et al., J. Chem. Phys. 141, 014101 (2014)] which uses oligomer excited-state calculations to perform an exact, point-wise mapping of coupled potential energy surfaces to an effective Frenkel model. Based upon this parametrization, the Multi-Layer Multi-Configuration Time-Dependent Hartree (ML-MCTDH) method is employed to investigate ultrafast dynamics of exciton transfer in a small, asymmetric HJ aggregate model composed of 30 sites and 30 active modes. For a partially delocalized initial condition, it is shown that a torsional defect confines the trapped initial exciton, and planarization induces an ultrafast resonant transition between an HJ-aggregated segment and a covalently bound "dangling chain" end. This model is a minimal realization of experimentally investigated mixed systems exhibiting ultrafast exciton transfer between aggregated, highly planarized chains and neighboring disordered segments.

  19. Dimensionality effects on the luminescence properties of hBN.

    PubMed

    Schué, Léonard; Berini, Bruno; Betz, Andreas C; Plaçais, Bernard; Ducastelle, François; Barjon, Julien; Loiseau, Annick

    2016-04-07

    Cathodoluminescence (CL) experiments at low temperature have been undertaken on various bulk and exfoliated hexagonal boron nitride (hBN) samples. Different bulk crystals grown from different synthesis methods have been studied. All of them present the same so-called S series in the 5.6-6 eV range, proving its intrinsic character. Luminescence spectra of flakes containing 100 down to 6 layers have been recorded. Strong modifications in the same UV range are observed and discussed within the general framework of 2D exciton properties in lamellar crystals.

  20. Biexciton formation and exciton coherent coupling in layered GaSe

    SciTech Connect

    Dey, P.; Paul, J.; Stevens, C. E.; Glikin, N.; Karaiskaj, D.; Moody, G.; Kovalyuk, Z. D.; Kudrynskyi, Z. R.; Romero, A. H.; Cantarero, A.; Hilton, D. J.

    2015-06-07

    Nonlinear two-dimensional Fourier transform (2DFT) and linear absorption spectroscopy are used to study the electronic structure and optical properties of excitons in the layered semiconductor GaSe. At the 1s exciton resonance, two peaks are identified in the absorption spectra, which are assigned to splitting of the exciton ground state into the triplet and singlet states. 2DFT spectra acquired for co-linear polarization of the excitation pulses feature an additional peak originating from coherent energy transfer between the singlet and triplet. At cross-linear polarization of the excitation pulses, the 2DFT spectra expose a new peak likely originating from bound biexcitons. The polarization dependent 2DFT spectra are well reproduced by simulations using the optical Bloch equations for a four level system, where many-body effects are included phenomenologically. Although biexciton effects are thought to be strong in this material, only moderate contributions from bound biexciton creation can be observed. The biexciton binding energy of ∼2 meV was estimated from the separation of the peaks in the 2DFT spectra. Temperature dependent absorption and 2DFT measurements, combined with “ab initio” theoretical calculations of the phonon spectra, indicate strong interaction with the A{sub 1}{sup ′} phonon mode. Excitation density dependent 2DFT measurements reveal excitation induced dephasing and provide a lower limit for the homogeneous linewidth of the excitons in the present GaSe crystal.

  1. Supramolecular luminescence from oligofluorenol-based supramolecular polymer semiconductors.

    PubMed

    Zhang, Guang-Wei; Wang, Long; Xie, Ling-Hai; Lin, Jin-Yi; Huang, Wei

    2013-11-13

    Supramolecular luminescence stems from non-covalent exciton behaviors of active π-segments in supramolecular entities or aggregates via intermolecular forces. Herein, a π-conjugated oligofluorenol, containing self-complementary double hydrogen bonds, was synthesized using Suzuki coupling as a supramolecular semiconductor. Terfluorenol-based random supramolecular polymers were confirmed via concentration-dependent nuclear magnetic resonance (NMR) and dynamic light scattering (DLS). The photoluminescent spectra of the TFOH-1 solution exhibit a green emission band (g-band) at approximately ~520 nm with reversible features, as confirmed through titration experiments. Supramolecular luminescence of TFOH-1 thin films serves as robust evidence for the aggregates of g-band. Our results suggest that the presence of polyfluorene ketone defects is a sufficient condition, rather than a sufficient-necessary condition for the g-band. Supramolecular electroluminescence will push organic devices into the fields of supramolecular optoelectronics, spintronics, and mechatronics.

  2. Supramolecular Luminescence from Oligofluorenol-Based Supramolecular Polymer Semiconductors

    PubMed Central

    Zhang, Guang-Wei; Wang, Long; Xie, Ling-Hai; Lin, Jin-Yi; Huang, Wei

    2013-01-01

    Supramolecular luminescence stems from non-covalent exciton behaviors of active π-segments in supramolecular entities or aggregates via intermolecular forces. Herein, a π-conjugated oligofluorenol, containing self-complementary double hydrogen bonds, was synthesized using Suzuki coupling as a supramolecular semiconductor. Terfluorenol-based random supramolecular polymers were confirmed via concentration-dependent nuclear magnetic resonance (NMR) and dynamic light scattering (DLS). The photoluminescent spectra of the TFOH-1 solution exhibit a green emission band (g-band) at approximately ~520 nm with reversible features, as confirmed through titration experiments. Supramolecular luminescence of TFOH-1 thin films serves as robust evidence for the aggregates of g-band. Our results suggest that the presence of polyfluorene ketone defects is a sufficient condition, rather than a sufficient-necessary condition for the g-band. Supramolecular electroluminescence will push organic devices into the fields of supramolecular optoelectronics, spintronics, and mechatronics. PMID:24232455

  3. Excitonic polaritons of zinc diarsenide single crystals

    NASA Astrophysics Data System (ADS)

    Syrbu, N. N.; Stamov, I. G.; Zalamai, V. V.; Dorogan, A.

    2017-02-01

    Excitonic polaritons of ZnAs2 single crystals had been investigated. Parameters of singlet excitons with D2bar(z) symmetry and orthoexcitons 2D1bar(y)+D2bar(x) had been determined. Spectral dependencies of ordinary and extraordinary dispersion of refractive index had been calculated using interferential reflection and transmittance spectra. It was shown, that A excitonic series were due to hole (V1) and electron (C1) bands. The values of effective masses of electrons (mc*=0.10 m0) and holes (mv1*=0.89 m0) had been estimated. It was revealed that the hole mass mv1* changes from 1.03 m0 to 0.55 m0 at temperature increasing from 10 K up to 230 K and that the electron mass mc* does not depend on temperature. The integral absorption A (eV cm-1) of the states n=1, 2 and 3 of D2bar(z) excitons depends on the An≈n-3 equality, which it is characteristic for S-type excitonic functions. Temperature dependences of the integral absorption of ground states for D2bar(z) and D2bar(D) excitons differ. The ground states of B and C excitons formed by V3 - C1 and V4 - C1 bands and its parameters had been determined.

  4. Time-resolved spectroscopy of intrinsic luminescence of Y 3Ga 5O 12 and (LaLu) 3Lu 2Ga 3O 12 single crystals

    NASA Astrophysics Data System (ADS)

    Zorenko, Yu.; Zorenko, T.; Vistovskyy, V.; Grinberg, M.; Łukasiewicz, T.

    2009-10-01

    The nature of intrinsic luminescence of Y 3Ga 5O 12 (YGG) and (LaLu) 3Lu 2Ga 3O 12 (LLGG) single crystals grown from a melt was determined. In the case of a YGG single crystal containing Y Ga antisite defects with a concentration of 0.25-0.275 at.% the intrinsic luminescence was considered as a superposition of luminescence of self-trapped excitons (STE), luminescence of excitons localized near antisite defects (LE(AD) centers) and luminescence caused by a recombination of an electron with a hole captured at Y Ga antisite defects. Due to a large (2-3%) concentration of Lu La antisite defects in LLGG single crystals the intrinsic luminescence was a superposition mainly of the LE(AD) center emission and the recombination luminescence of Lu La antisite defects. The energy structure of the mentioned centers in YGG and LGGG hosts was determined from the excitation spectra of their luminescence under excitation by synchrotron radiation in the range of the fundamental absorption edge of these garnets.

  5. Topological Exciton Bands in Moire Heterojunctions.

    DOE PAGES

    Wu, Fengcheng; Lovorn, Timothy; MacDonald, A. H.

    2017-04-05

    Moire patterns are common in Van der Waals heterostructures and can be used to apply periodic potentials to elementary excitations. Here, we show that the optical absorption spectrum of transition metal dichalcogenide bilayers is profoundly altered by long period moire patterns that introduce twist-angle dependent satellite excitonic peaks. Topological exciton bands with non-zero Chern numbers that support chiral excitonic edge states can be engineered by combining three ingredients: i) the valley Berry phase induced by electron-hole exchange interactions, ii) the moire potential, and iii) the valley Zeeman field.

  6. 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.

  7. Ultracold Gas of Excitons in Traps

    DTIC Science & Technology

    2012-06-08

    Excitons in a GaAs Quantum-Well Structurewith a Diamond-Shaped Electrostatic Trap, Physical Review Letters, (08 2009): 87403. doi: 2012/06/08 14:38:06 19...Kinetics of the inner ring in the exciton emission pattern in coupled GaAs quantum wells, Physical Review B, (10 2009): 155331. doi: 2012/06/08 14:28:30...17 Sen Yang, , L. V. Butov, , L. S. Levitov, , B. D. Simons,, A. C. Gossard. Exciton front propagation in photoexcited GaAs quantum wells, Physical

  8. Spin currents in a coherent exciton gas.

    PubMed

    High, A A; Hammack, A T; Leonard, J R; Yang, Sen; Butov, L V; Ostatnický, T; Vladimirova, M; Kavokin, A V; Liew, T C H; Campman, K L; Gossard, A C

    2013-06-14

    We report the observation of spin currents in a coherent gas of indirect excitons. The realized long-range spin currents originate from the formation of a coherent gas of bosonic pairs--a new mechanism to suppress the spin relaxation. The spin currents result in the appearance of a variety of polarization patterns, including helical patterns, four-leaf patterns, spiral patterns, bell patterns, and periodic patterns. We demonstrate control of the spin currents by a magnetic field. We also present a theory of coherent exciton spin transport that describes the observed exciton polarization patterns and indicates the trajectories of the spin currents.

  9. Free exciton emission and vibrations in pentacene monolayers

    NASA Astrophysics Data System (ADS)

    He, Rui

    2011-03-01

    Pentacene is a benchmark organic semiconductor material because of its potential applications in electronic and optoelectronic devices. Recently we demonstrated that optical and vibrational characterizations of pentacene films can be carried out down to the sub-monolayer limit. These milestones were achieved in highly uniform pentacene films that were grown on a compliant polymeric substrate. Films with thickness ranging from sub- monolayer to tens of monolayers were studied at low temperatures. The intensity of the free exciton (FE) luminescence band increases quadratically with the number of layers N when N is small. This quadratic dependence is explained as arising from the linear dependence of the intensity of absorption and the probability of emission on the number of layers N. Large enhancements of Raman scattering intensities at the FE resonance enable the first observations of low-lying lattice modes in the monolayers. The measured low- lying modes (in the 20 to 100 cm-1 range) display characteristic changes when going from a single monolayer to two layers. The Raman intensities by high frequency intra-molecular vibrations display resonance enhancement double-peaks when incident or scattered photon energies overlap the FE optical emission. The double resonances are about the same strength which suggests that Franck-Condon overlap integrals for the respective vibronic transitions have the same magnitude. The interference between scattering amplitudes in the Raman resonance reveals quantum coherence of the symmetry-split states (Davydov doublet) of the lowest intrinsic singlet exciton. These results demonstrate novel venues for ultra-thin film characterization and studies of fundamental physics in organic semiconductor structures. In collaboration with Nancy G. Tassi (Dupont), Graciela B. Blanchet (Nanoterra, Cambridge, MA), and Aron Pinczuk (Columbia University).

  10. Diamagnetic excitons in semiconductors (Review)

    NASA Astrophysics Data System (ADS)

    Seisyan, R. P.

    2016-05-01

    Optical properties of semiconductor crystals in the presence of a high magnetic field have been considered. The field turn-on gives rise to oscillations of the optical-absorption edge or, more specifically, the formation of a complex absorption spectrum with a periodic structure, referred to as the spectrum of "diamagnetic excitons." Such spectra appear a source of the most accurate knowledge about the band structure of semiconductors. Moreover, these spectra can be used for simulating the low-dimensional state in semiconductors and possible interpretation of the emission spectra of neutron stars. The proposed analytical review is based on extensive experimental and theoretical data contained mostly in cited original works of the author with colleagues.

  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. Optical nutation in the exciton range of spectrum

    SciTech Connect

    Khadzhi, P. I.; Vasiliev, V. V.

    2013-08-15

    Optical nutation in the exciton range of spectrum is studied in the mean field approximation taking into account exciton-photon and elastic exciton-exciton interactions. It is shown that the features of nutation development are determined by the initial exciton and photon densities, the resonance detuning, the nonlinearity parameter, and the initial phase difference. For nonzero initial exciton and photon concentrations, three regimes of temporal evolution of excitons and photons exist: periodic conversion of excitons to photons and vice versa, aperiodic conversion of photons to excitons, and the rest regime. In the rest regime, the initial exciton and photon densities are nonzero and do not change with time. The oscillation amplitudes and periods of particle densities determined by the system parameters are found. The exciton self-trapping and photon trapping appearing in the system at threshold values of the nonlinearity parameter were predicted. As this parameter increases, the oscillation amplitudes of the exciton and photon densities sharply change at the critical value of the nonlinearity parameter. These two phenomena are shown to be caused by the elastic exciton-exciton interaction, resulting in the dynamic concentration shift of the exciton level.

  13. Acoustic-excitonic effects in a two-dimensional gas of dipolar excitons

    NASA Astrophysics Data System (ADS)

    Boev, M. V.; Kovalev, V. M.; Chaplik, A. V.

    2016-08-01

    The theory of the interaction of a two-dimensional gas of indirect dipolar excitons with Rayleigh surface elastic waves has been developed. The absorption and renormalization of the phase velocity of a surface wave, as well as the drag of excitons by the surface acoustic wave and the generation of bulk acoustic waves by a twodimensional gas of dipolar excitons irradiated by external electromagnetic radiation, have been considered. These effects have been studied both in a normal phase at high temperatures and in a condensed phase of the exciton gas. The calculations have been performed in the ballistic and diffusion limits for both phases.

  14. Direct observation of giant binding energy modulation of exciton complexes in monolayer MoS e2

    NASA Astrophysics Data System (ADS)

    Gupta, Garima; Kallatt, Sangeeth; Majumdar, Kausik

    2017-08-01

    Screening due to the surrounding dielectric medium reshapes the electron-hole interaction potential and plays a pivotal role in deciding the binding energies of strongly bound exciton complexes in quantum confined monolayers of transition metal dichalcogenides (TMDs). However, owing to strong quasiparticle band-gap renormalization in such systems, a direct quantification of estimated shifts in binding energy in different dielectric media remains elusive using optical studies. In this work, by changing the dielectric environment, we show a conspicuous photoluminescence peak shift at low temperature for higher energy excitons (2 s ,3 s ,4 s ,5 s ) in monolayer MoS e2 , while the 1 s exciton peak position remains unaltered - a direct evidence of varying compensation between screening induced exciton binding energy modulation and quasiparticle band-gap renormalization. The estimated modulation of binding energy for the 1 s exciton is found to be 58.6 % (72.8 % for 2 s ,75.85 % for 3 s , and 85.6 % for 4 s ) by coating an A l2O3 layer on top, while the corresponding reduction in quasiparticle band-gap is estimated to be 246 meV. Such direct evidence of large tunability of the binding energy of exciton complexes as well as the band-gap in monolayer TMDs holds promise of novel device applications.

  15. Luminescence of SiO2 and GeO2 crystals with rutile structure. Comparison with α-quartz crystals and relevant glasses (Review Article)

    NASA Astrophysics Data System (ADS)

    Trukhin, A. N.

    2016-07-01

    Luminescence properties of SiO2 in different structural states are compared. Similar comparison is made for GeO2. Rutile and α-quartz structures as well as glassy state of these materials are considered. Main results are that for α-quartz crystals the luminescence of self-trapped exciton is the general phenomenon that is absent in the crystal with rutile structure. In rutile structured SiO2 (stishovite) and GeO2 (argutite) the main luminescence is due to a host material defect existing in as-received (as-grown) samples. The defect luminescence possesses specific two bands, one of which has a slow decay (for SiO2 in the blue and for GeO2, in green range) and another, a fast ultraviolet (UV) band (4.75 eV in SiO2 and at 3 eV in GeO2). In silica and germania glasses, the luminescence of self-trapped exciton coexists with defect luminescence. The latter also contains two bands: one in the visible range and another in the UV range. The defect luminescence of glasses was studied in details during last 60-70 years and is ascribed to oxygen deficient defects. Analogous defect luminescence in the corresponding pure nonirradiated crystals with α-quartz structure is absent. Only irradiation of a α-quartz crystal by energetic electron beam, γ-rays and neutrons provides defect luminescence analogous to glasses and crystals with rutile structure. Therefore, in glassy state the structure containing tetrahedron motifs is responsible for existence of self-trapped excitons and defects in octahedral motifs are responsible for oxygen deficient defects.

  16. Outward Bound.

    ERIC Educational Resources Information Center

    Outward Bound, Inc., Andover, MA.

    The Outward Bound concept was developed in Germany and Great Britain with the saving of human life as the ultimate goal. Courses are designed to help students discover their true physical and mental limits through development of skills including emergency medical aid, firefighting, search and rescue, mountaineering, and sailing. Five Outward Bound…

  17. Excitonic susceptibility in near triangular quantum wells

    NASA Astrophysics Data System (ADS)

    Anitha, A.; Arulmozhi, M.

    2017-03-01

    Diamagnetic susceptibility and binding energy of an exciton in a near triangular quantum well, with potential profile proportional to |z|2/3 composed of GaAs/Ga1- x Al x As and ZnO/Zn1- x Mg x O are calculated as a function of the wellwidth and concentration of Al and Mg respectively varying the magnetic field applied along growth direction (i.e. z-axis). Diamagnetic susceptibility of light hole exciton and heavy hole exciton, shows inverse behaviors in the two materials below 20 nm wellwidth and the binding energy of both excitons increases, as the magnetic field increases. The results obtained, are compared with those of quantum wells with varied potential profiles and the experimental results reported in the literature.

  18. Exciton absorption in narrow armchair graphene nanoribbons

    NASA Astrophysics Data System (ADS)

    Monozon, B. S.; Schmelcher, P.

    2016-11-01

    We develop an analytical approach to the exciton optical absorption for narrow gap armchair graphene nanoribbons (AGNR). We focus on the regime of dominant size quantization in combination with the attractive electron-hole interaction. An adiabatic separation of slow and fast motions leads via the two-body Dirac equation to the isolated and coupled subband approximations. Discrete and continuous exciton states are in general coupled and form quasi-Rydberg series of purely discrete and resonance type character. The corresponding oscillator strengths and widths are derived. We show that the exciton peaks are blue-shifted, become broader and increase in magnitude upon narrowing the ribbon. At the edge of a subband the singularity related to the 1D density of states is transformed into finite absorption via the presence of the exciton. Our analytical results are in good agreement with those obtained by other methods including numerical approaches. Estimates of the expected experimental values are provided for realistic AGNR.

  19. Radiative lifetime of excitons in carbon nanotubes.

    PubMed

    Perebeinos, Vasili; Tersoff, J; Avouris, Phaedon

    2005-12-01

    We calculate the radiative lifetime and energy bandstructure of excitons in semiconducting carbon nanotubes within a tight-binding approach including the electron-hole correlations via the Bethe-Salpeter equation. In the limit of rapid interband thermalization, the radiative decay rate is maximized at intermediate temperatures and decreases at low temperature because the lowest-energy excitons are optically forbidden. The intrinsic phonons cannot scatter excitons between optically active and forbidden bands, so sample-dependent extrinsic effects that break the symmetries can play a central role. We calculate the diameter-dependent energy splittings between singlet and triplet excitons of different symmetries and the resulting dependence of radiative lifetime on temperature and tube diameter.

  20. Signatures of Quantum Coherences in Rydberg Excitons

    NASA Astrophysics Data System (ADS)

    Grünwald, P.; Aßmann, M.; Heckötter, J.; Fröhlich, D.; Bayer, M.; Stolz, H.; Scheel, S.

    2016-09-01

    Coherent optical control of individual particles has been demonstrated both for atoms and semiconductor quantum dots. Here we demonstrate the emergence of quantum coherent effects in semiconductor Rydberg excitons in bulk Cu2O . Because of the spectral proximity between two adjacent Rydberg exciton states, a single-frequency laser may pump both resonances with little dissipation from the detuning. As a consequence, additional resonances appear in the absorption spectrum that correspond to dressed states consisting of two Rydberg exciton levels coupled to the excitonic vacuum, forming a V -type three-level system, but driven only by one laser light source. We show that the level of pure dephasing in this system is extremely low. These observations are a crucial step towards coherently controlled quantum technologies in a bulk semiconductor.

  1. Quantum and classical solutions for statically screened two-dimensional Wannier-Mott excitons

    SciTech Connect

    Makowski, Adam J.

    2011-08-15

    Quantum solutions and classical orbits are discussed for statically screened Wannier-Mott excitons for two closely related potentials: the Stern-Howard potential and a suggested simple focusing one. Bound states and exact ''quantized'' values of screening are obtained as well. For the suggested potential, the scattering matrix, the Regge poles, and the transmission coefficient are calculated exactly. We argue that the simple potential can be utilized in applications instead of the Stern-Howard potential, which is difficult to handle.

  2. Exciton properties of selected aromatic hydrocarbon systems

    NASA Astrophysics Data System (ADS)

    Roth, Friedrich; Mahns, Benjamin; Hampel, Silke; Nohr, Markus; Berger, Helmuth; Büchner, Bernd; Knupfer, Martin

    2013-02-01

    We have examined the singlet excitons in two representatives of acene-type (tetracene and pentacene) and phenacene-type (chrysene and picene) molecular crystals, respectively, using electron energy-loss spectroscopy at low temperatures. We show that the excitation spectra of the two hydrocarbon families significantly differ. Moreover, close inspection of the data indicates that there is an increasing importance of charge-transfer excitons at lowest excitation energy with increasing length of the molecules.

  3. Exciton-polariton wakefields in semiconductor microcavities

    NASA Astrophysics Data System (ADS)

    Terças, H.; Mendonça, J. T.

    2016-02-01

    We consider the excitation of polariton wakefields due to a propagating light pulse in a semiconductor microcavity. We show that two kinds of wakes are possible, depending on the constituents fraction (either exciton or photon) of the polariton wavefunction. The nature of the wakefields (pure excitonic or polaritonic) can be controlled by changing the speed of propagation of the external pump. This process could be used as a diagnostic for the internal parameters of the microcavity.

  4. Ultrafast exciton dynamics at molecular surfaces

    NASA Astrophysics Data System (ADS)

    Monahan, Nicholas R.

    Further improvements to device performance are necessary to make solar energy conversion a compelling alternative to fossil fuels. Singlet exciton fission and charge separation are two processes that can heavily influence the power conversion efficiency of a solar cell. During exciton fission one singlet excitation converts into two triplet excitons, potentially doubling the photocurrent generated by higher energy photons. There is significant discord over the singlet fission mechanism and of particular interest is whether the process involves a multiexciton intermediate state. I used time-resolved two-photon photoemission to investigate singlet fission in hexacene thin films, a model system with strong electronic coupling. My results indicate that a multiexciton state forms within 40 fs of photoexcitation and loses singlet character on a 280 fs timescale, creating two triplet excitons. This is concordant with the transient absorption spectra of hexacene single crystals and definitively proves that exciton fission in hexacene proceeds through a multiexciton state. This state is likely common to all strongly-coupled systems and my results suggest that a reassessment of the generally-accepted singlet fission mechanism is required. Charge separation is the process of splitting neutral excitons into carriers that occurs at donor-acceptor heterojunctions in organic solar cells. Although this process is essential for device functionality, there are few compelling explanations for why it is highly efficient in certain organic photovoltaic systems. To investigate the charge separation process, I used the model system of charge transfer excitons at hexacene surfaces and time-resolved two-photon photoemission. Charge transfer excitons with sufficient energy spontaneously delocalize, growing from about 14 nm to over 50 nm within 200 fs. Entropy drives this delocalization, as the density of states within the Coulomb potential increases significantly with energy. This charge

  5. Plasmonic pumping of excitonic photoluminescence in hybrid MoS2-Au nanostructures.

    PubMed

    Najmaei, Sina; Mlayah, Adnen; Arbouet, Arnaud; Girard, Christian; Léotin, Jean; Lou, Jun

    2014-12-23

    We report on the fabrication of monolayer MoS2-coated gold nanoantennas combining chemical vapor deposition, e-beam lithography surface patterning, and a soft lift-off/transfer technique. The optical properties of these hybrid plasmonic-excitonic nanostructures are investigated using spatially resolved photoluminescence spectroscopy. Off- and in-resonance plasmonic pumping of the MoS2 excitonic luminescence showed distinct behaviors. For plasmonically mediated pumping, we found a significant enhancement (∼65%) of the photoluminescence intensity, clear evidence that the optical properties of the MoS2 monolayer are strongly influenced by the nanoantenna surface plasmons. In addition, a systematic photoluminescence broadening and red-shift in nanoantenna locations is observed which is interpreted in terms of plasmonic enhanced optical absorption and subsequent heating of the MoS2 monolayers. Using a temperature calibration procedure based on photoluminescence spectral characteristics, we were able to estimate the local temperature changes. We found that the plasmonically induced MoS2 temperature increase is nearly four times larger than in the MoS2 reference temperatures. This study shines light on the plasmonic-excitonic interaction in these hybrid metal/semiconductor nanostructures and provides a unique approach for the engineering of optoelectronic devices based on the light-to-current conversion.

  6. Fluorescence dynamics and fine structure of dark excitons in semiconducting single-wall carbon nanotubes.

    PubMed

    Alfonsi, Jessica; Meneghetti, Moreno

    2012-06-27

    Exact diagonalization results are reported for the bright and dark exciton structure of semiconducting single-wall carbon nanotubes in the framework of the Hubbard model combined with a small crystal approach for several values of the correlation coupling strength U/t. Our findings, in the low-intermediate correlation regime (1.5 < U/t < 2.1), show the presence of dark states above and below the first bright exciton |B> and can account for reported experimental values of deep triplet states below |B> and of a K-momentum singlet dark exciton above this state. In order to fit the temporal profile of the photoluminescence (PL) decay, a bottleneck mechanism is considered involving a few dark states, with the respective energy gaps correspondingly obtained in the above-mentioned correlation range. We find that a kinetic model with one dark state above and two below |B> is able to recover the observed biexponential features of the PL behaviour with a reasonable set of parameters. Within this model we attribute the long tail of the PL to a delayed luminescence process of the bright state caused by the nearby calculated dark states.

  7. Enhancement of photoluminescence from excitons in silicon nanocrystals via coupling to surface plasmon polaritons

    NASA Astrophysics Data System (ADS)

    Takeda, Eiji; Fujii, Minoru; Nakamura, Toshihiro; Mochizuki, Yugo; Hayashi, Shinji

    2007-07-01

    The enhancement of photoluminescence (PL) is demonstrated from silicon nanocrystals (Si-ncs) by strong coupling of excitons to surface plasmon polaritons (SPPs) supported by a Au thin film. SPPs excited via excitons in Si-ncs were Bragg scattered to photons by one- or two-dimensional gratings, and strong and directional PL was obtained. From the angular dependence of PL spectra, dispersion relations of electromagnetic modes involved in the light emission process were obtained. The overall agreement between experimentally obtained and theoretically calculated dispersion relations confirmed that the strong and directional PL is mediated by SPPs. The PL decay rate of Si-ncs increased by placing a Au thin film on top and the wavelength dependence of the rate enhancement agreed well with that of the calculated SPP excitation rate. This suggests that the observed PL enhancement is due to efficient energy transfer from excitons to SPPs followed by efficient scattering of SPPs to photons, resulting in the enhancement of luminescence quantum efficiency.

  8. 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.

  9. Exciton Dynamics in Monolayer Transition Metal Dichalcogenides

    PubMed Central

    Moody, Galan; Schaibley, John; Xu, Xiaodong

    2017-01-01

    Since the discovery of semiconducting monolayer transition metal dichalcogenides, a variety of experimental and theoretical studies have been carried out seeking to understand the intrinsic exciton population recombination and valley relaxation dynamics. Reports of the exciton decay time range from hundreds of femtoseconds to ten nanoseconds, while the valley depolarization time can exceed one nanosecond. At present, however, a consensus on the microscopic mechanisms governing exciton radiative and non-radiative recombination is lacking. The strong exciton oscillator strength resulting in up to ~ 20% absorption for a single monolayer points to ultrafast radiative recombination. However, the low quantum yield and large variance in the reported lifetimes suggest that non-radiative Auger-type processes obscure the intrinsic exciton radiative lifetime. In either case, the electron-hole exchange interaction plays an important role in the exciton spin and valley dynamics. In this article, we review the experiments and theory that have led to these conclusions and comment on future experiments that could complement our current understanding. PMID:28890600

  10. Advanced synchronous luminescence system

    DOEpatents

    Vo-Dinh, Tuan

    1997-01-01

    A method and apparatus for determining the condition of tissue or otherwise making chemical identifications includes exposing the sample to a light source, and using a synchronous luminescence system to produce a spectrum that can be analyzed for tissue condition.

  11. Universal Length Dependence of Rod-to-Seed Exciton Localization Efficiency in Type I and Quasi-Type II CdSe@CdS Nanorods.

    PubMed

    Wu, Kaifeng; Hill, Lawrence J; Chen, Jinquan; McBride, James R; Pavlopolous, Nicholas G; Richey, Nathaniel E; Pyun, Jeffrey; Lian, Tianquan

    2015-04-28

    A critical step involved in many applications of one-dimensional seeded CdSe@CdS nanorods, such as luminescent solar concentrators, optical gains, and photocatalysis, is the localization of excitons from the light-harvesting CdS nanorod antenna into the light-emitting CdSe quantum dot seed. We report that the rod-to-seed exciton localization efficiency decreases with the rod length but is independent of band alignment between the CdSe seed and CdS rod. This universal dependence can be well modeled by the competition between exciton one-dimensional diffusion to the CdSe seed and trapping on the CdS rod. This finding provides a rational approach for optimizing these materials for their various device applications.

  12. Multidimensional Luminescence Measurements

    DTIC Science & Technology

    1985-04-30

    reflector in the dye laser cavity; BS, beam splitter ; PD, photodiode; M, beam steering mirrors; P, HPLC solvent 20 • ’ ’ ’ ’ , ’ , i i i . ..... i...the excitation beam , the -’ luminescence till also have an associated modulation depending on the time delay. This property is used in phase resolved...luminescence measurements. The phase resolved method uses a continuous sinusoidally modulated L ex-itation beam . Knowing the modulation frequency (f

  13. Structured luminescence conversion layer

    DOEpatents

    Berben, Dirk; Antoniadis, Homer; Jermann, Frank; Krummacher, Benjamin Claus; Von Malm, Norwin; Zachau, Martin

    2012-12-11

    An apparatus device such as a light source is disclosed which has an OLED device and a structured luminescence conversion layer deposited on the substrate or transparent electrode of said OLED device and on the exterior of said OLED device. The structured luminescence conversion layer contains regions such as color-changing and non-color-changing regions with particular shapes arranged in a particular pattern.

  14. "Cloud" assemblies: quantum dots form electrostatically bound dynamic nebulae around large gold nanoparticles.

    PubMed

    Lilly, G Daniel; Lee, Jaebeom; Kotov, Nicholas A

    2010-10-14

    Dynamic self-assembled structures of nanoparticles can be produced using predominantly electrostatic interactions. Such assemblies were made from large, positively charged Au metal nanoparticles surrounded by an electrostatically bound cloud of smaller, negatively charged CdSe/ZnS or CdTe quantum dots. At low concentrations they are topologically similar to double electric layers of ions and corona-like assemblies linked by polymer chains. They can also be compared to the topological arrangement of some planetary systems in space. The great advantages of the cloud assemblies are (1) their highly dynamic nature compared to more rigid covalently bound assemblies, (2) simplicity of preparation, and (3) exceptional versatility in components and resulting optical properties. Photoluminescence intensity enhancement originating from quantum resonance between excitons and plasmons was observed for CdSe/ZnS quantum dots, although CdTe dots displayed emission quenching. To evaluate more attentively their dynamic behavior, emission data were collected for the cloud-assemblies with different ratios of the components and ionic strengths of the media. The emission of the system passes through a maximum for 80 QDs ∶ 1 Au NP as determined by the structure of the assemblies and light absorption conditions. Ionic strength dependence of luminescence intensity contradicts the predictions based on the Gouy-Chapman theory and osmotic pressure at high ionic strengths due to formation of larger chaotic colloidally stable assemblies. "Cloud" assemblies made from different nanoscale components can be used both for elucidation of most fundamental aspects of nanoparticle interactions, as well as for practical purposes in sensing and biology.

  15. “Cloud” assemblies: quantum dots form electrostatically bound dynamic nebulae around large gold nanoparticle

    SciTech Connect

    Lilly, G. Daniel; Lee, Jaebeom; Kotov, Nicholas A.

    2010-07-29

    Dynamic self-assembled structures of nanoparticles can be produced using predominantly electrostatic interactions. Such assemblies were made from large, positively charged Au metal nanoparticles surrounded by an electrostatically bound cloud of smaller, negatively charged CdSe/ZnS or CdTe quantum dots. At low concentrations they are topologically similar to double electric layers of ions and corona-like assemblies linked by polymer chains. They can also be compared to the topological arrangement of some planetary systems in space. The great advantages of the cloud assemblies are (1) their highly dynamic nature compared to more rigid covalently bound assemblies, (2) simplicity of preparation, and (3) exceptional versatility in components and resulting optical properties. Photoluminescence intensity enhancement originating from quantum resonance between excitons and plasmons was observed for CdSe/ZnS quantum dots, although CdTe dots displayed emission quenching. To evaluate more attentively their dynamic behavior, emission data were collected for the cloud-assemblies with different ratios of the components and ionic strengths of the media. The emission of the system passes through a maximum for 80 QDs:1 Au NP as determined by the structure of the assemblies and light absorption conditions. Ionic strength dependence of luminescence intensity contradicts the predictions based on the Gouy–Chapman theory and osmotic pressure at high ionic strengths due to formation of larger chaotic colloidally stable assemblies. “Cloud” assemblies made from different nanoscale components can be used both for elucidation of most fundamental aspects of nanoparticle interactions, as well as for practical purposes in sensing and biology.

  16. Interaction of Dirac Fermion excitons and biexciton-exciton cascade in graphene quantum dots

    NASA Astrophysics Data System (ADS)

    Ozfidan, Isil; Korkusinski, Marek; Hawrylak, Pawel

    2015-03-01

    We present a microscopic theory of interacting Dirac quasi-electrons and quasi-holes confined in graphene quantum dots. The single particle states of quantum dots are described using a tight binding model and screened direct, exchange, and scattering Coulomb matrix elements are computed using Slater pz orbitals. The many-body ground and excited states are expanded in a finite number of electron-hole pair excitations from the Hartree-Fock ground state and computed using exact diagonalization techniques. The resulting exciton and bi-exciton spectrum reflects the degeneracy of the top of the valence and bottom of the conduction band characteristic of graphene quantum dots with C3 symmetry. We study the interaction of multi-electron and hole complexes as a function of quantum dot size, shape and strength of Coulomb interactions. We identify two degenerate bright exciton (X) states and a corresponding biexciton (XX) state as XX-X cascade candidates, a source of entangled photon pairs. We next calculate the exciton to bi-exciton transitions detected in transient absorption experiments to extract the strength of exciton-exciton interactions and biexciton binding energies. We further explore the possibility of excitonic instability.

  17. Microscopic theories of excitons and their dynamics

    NASA Astrophysics Data System (ADS)

    Berkelbach, Timothy C.

    This thesis describes the development and application of microscopically-defined theories of excitons in a wide range of semiconducting materials. In Part I, I consider the topic of singlet exciton fission, an organic photophysical process which generates two spin-triplet excitons from one photoexcited spin-singlet exciton. I construct a theoretical framework that couples a realistic treatment of the static electronic structure with finite-temperature quantum relaxation techniques. This framework is applied separately, but consistently, to the problems of singlet fission in pentacene dimers, crystalline pentacene, and crystalline hexacene. Through this program, I am able to rationalize observed behaviors and make non-trivial predictions, some of which have been confirmed by experiment. In Part II, I present theoretical developments on the properties of neutral excitons and charged excitons (trions) in atomically thin transition metal dichalcogenides. This work includes an examination of material trends in exciton binding energies via an effective mass approach. I also present an experimental and theoretical collaboration, which links the unconventional disposition of excitons in the Rydberg series to the peculiar screening properties of atomically thin materials. The light-matter coupling in these materials is examined within low-energy models and is shown to give rise to bright and dark exciton states, which can be qualitatively labeled in analogy with the hydrogen series. In Part III, I explore theories of relaxation dynamics in condensed phase environments, with a focus on methodology development. This work is aimed towards biological processes, including resonant energy transfer in chromophore complexes and electron transfer in donor-bridge-acceptor systems. Specifically, I present a collaborative development of a numerically efficient but highly accurate hybrid approach to reduced dynamics, which exploits a partitioning of environmental degrees of freedom into

  18. Light-hole exciton in a nanowire quantum dot

    NASA Astrophysics Data System (ADS)

    Jeannin, Mathieu; Artioli, Alberto; Rueda-Fonseca, Pamela; Bellet-Amalric, Edith; Kheng, Kuntheak; André, Régis; Tatarenko, Serge; Cibert, Joël; Ferrand, David; Nogues, Gilles

    2017-01-01

    Quantum dots inserted inside semiconductor nanowires are extremely promising candidates as building blocks for solid-state-based quantum computation and communication. They provide very high crystalline and optical properties and offer a convenient geometry for electrical contacting. Having a complete determination and full control of their emission properties is one of the key goals of nanoscience researchers. Here we use strain as a tool to create in a single magnetic nanowire quantum dot a light-hole exciton, an optically active quasiparticle formed from a single electron bound to a single light hole. In this frame, we provide a general description of the mixing within the hole quadruplet induced by strain or confinement. A multi-instrumental combination of cathodoluminescence, polarization-resolved Fourier imaging, and magneto-optical spectroscopy, allows us to fully characterize the hole ground state, including its valence band mixing with heavy-hole states.

  19. Exciton interference revealed by energy dependent exciton transfer rate for ring-structured molecular systems

    SciTech Connect

    Yan, Yun-An

    2016-01-14

    The quantum interference is an intrinsic phenomenon in quantum physics for photon and massive quantum particles. In principle, the quantum interference may also occur with quasi-particles, such as the exciton. In this study, we show how the exciton quantum interference can be significant in aggregates through theoretical simulations with hierarchical equations of motion. The systems under investigation are generalized donor-bridge-acceptor model aggregates with the donor consisting of six homogeneous sites assuming the nearest neighbor coupling. For the models with single-path bridge, the exciton transfer time only shows a weak excitation energy dependence. But models with double-path bridge have a new short transfer time scale and the excitation energy dependence of the exciton transfer time assumes clear peak structure which is detectable with today’s nonlinear spectroscopy. This abnormality is attributed to the exciton quantum interference and the condition for a clear observation in experiment is also explored.

  20. High pressure luminescence spectra of CaMoO4:Ln3+ (Ln = Pr, Tb).

    PubMed

    Mahlik, S; Behrendt, M; Grinberg, M; Cavalli, E; Bettinelli, M

    2013-03-13

    Photoluminescence spectra and luminescence kinetics of pure CaMoO(4) and CaMoO(4) doped with Ln(3+) (Ln = Pr or Tb) are presented. The spectra were obtained at high hydrostatic pressure up to 240 kbar applied in a diamond anvil cell. At ambient pressure undoped and doped samples exhibit a broad band emission extending between 380 and 700 nm with a maximum at 520 nm attributed to the MoO(4)(2-) luminescence. CaMoO(4) doped with Pr(3+) or Tb(3+) additionally yields narrow emission lines related to f-f transitions. The undoped CaMoO(4) crystal was characterized by a strong MoO(4)(2-) emission up to 240 kbar. In the cases of CaMoO(4):Pr(3+) and CaMoO(4):Tb(3+), high hydrostatic pressure caused quenching of Pr(3+) and Tb(3+) emission, and this effect was accompanied by a strong shortening of the luminescence lifetime. In doped samples, CaMoO(4):Pr(3+) and CaMoO(4):Tb(3+), quenching of the emission band attributed to MoO(4)(2-) was also observed, and at pressure above 130 kbar this luminescence was totally quenched. The effects mentioned above were related to the influence of the praseodymium (terbium) trapped exciton PTE (ITE-impurity trapped exciton) on the efficiency of the Pr(3+) (Tb(3+)) and MoO(4)(2-) emissions.

  1. High pressure luminescence spectra of CaMoO4:Ln3+ (Ln = Pr, Tb)

    NASA Astrophysics Data System (ADS)

    Mahlik, S.; Behrendt, M.; Grinberg, M.; Cavalli, E.; Bettinelli, M.

    2013-03-01

    Photoluminescence spectra and luminescence kinetics of pure CaMoO4 and CaMoO4 doped with Ln3+ (Ln = Pr or Tb) are presented. The spectra were obtained at high hydrostatic pressure up to 240 kbar applied in a diamond anvil cell. At ambient pressure undoped and doped samples exhibit a broad band emission extending between 380 and 700 nm with a maximum at 520 nm attributed to the {{MoO}}_{4}^{2-} luminescence. CaMoO4 doped with Pr3+ or Tb3+ additionally yields narrow emission lines related to f-f transitions. The undoped CaMoO4 crystal was characterized by a strong MoO{}_{4}^{2-} emission up to 240 kbar. In the cases of CaMoO4:Pr3+ and CaMoO4:Tb3+, high hydrostatic pressure caused quenching of Pr3+ and Tb3+ emission, and this effect was accompanied by a strong shortening of the luminescence lifetime. In doped samples, CaMoO4:Pr3+ and CaMoO4:Tb3+, quenching of the emission band attributed to {{MoO}}_{4}^{2-} was also observed, and at pressure above 130 kbar this luminescence was totally quenched. The effects mentioned above were related to the influence of the praseodymium (terbium) trapped exciton PTE (ITE—impurity trapped exciton) on the efficiency of the Pr3+ (Tb3+) and {{MoO}}_{4}^{2-} emissions.

  2. Exciton polarizability in semiconductor nanocrystals.

    PubMed

    Wang, Feng; Shan, Jie; Islam, Mohammad A; Herman, Irving P; Bonn, Mischa; Heinz, Tony F

    2006-11-01

    The response of charge to externally applied electric fields is an important basic property of any material system, as well as one critical for many applications. Here, we examine the behaviour and dynamics of charges fully confined on the nanometre length scale. This is accomplished using CdSe nanocrystals of controlled radius (1-2.5 nm) as prototype quantum systems. Individual electron-hole pairs are created at room temperature within these structures by photoexcitation and are probed by terahertz (THz) electromagnetic pulses. The electronic response is found to be instantaneous even for THz frequencies, in contrast to the behaviour reported in related measurements for larger nanocrystals and nanocrystal assemblies. The measured polarizability of an electron-hole pair (exciton) amounts to approximately 10(4) A(3) and scales approximately as the fourth power of the nanocrystal radius. This size dependence and the instantaneous response reflect the presence of well-separated electronic energy levels induced in the system by strong quantum-confinement effects.

  3. Exciton transport and dissociation at organic interfaces

    NASA Astrophysics Data System (ADS)

    Beljonne, David

    2011-03-01

    This paper focuses on modeling studies of exciton transport and dissociation at organic interfaces and includes three parts: 1) Experiments have shown that the values of exciton diffusion length LD in conjugated polymers (CPs) are rather low, in the range of 5-10 nm, apparently regardless of their chemical structure and solid-state packing. In contrast, larger LD values have been reported in molecular materials that are chemically more well-defined than CPs. Here we demonstrate that energetic disorder alone reduces the exciton diffusion length more than one order of magnitude, from values typically encountered in molecules (> 50nm) to values actually measured in CPs (<10nm). 2) A number of organic crystals show anisotropic excitonic couplings, with weak interlayer interactions between molecules that are more strongly coupled within the layers. The resulting energy carriers are intra-layer 2D excitons that diffuse along the interlayer direction. We model this analytically for infinite layers and using quantum-chemical calculations of the electronic couplings for anthracene clusters. We show that the exciton hopping rates and diffusion lengths depend in a subtle manner on the size and shape of the interacting aggregates, temperature and the presence of energetic disorder. 3) The electronic structure at organic/organic interfaces plays a key role, among others, in defining the quantum efficiency of organic-based photovoltaic cells. Here, we perform quantum-chemical and microelectrostatic calculations on molecular aggregates of various sizes and shapes to characterize the interfacial dipole moment at pentacene/C60 heterojunctions. The results show that the interfacial dipole mostly originates in polarization effects due to the asymmetry in the multipolar expansion of the electronic density distribution between the interacting molecules. We will discuss how the quadrupoles on the pentacene molecules produce direct electrostatic interactions with charge carriers and how

  4. Efficient exciton funneling in cascaded PbS quantum dot superstructures.

    PubMed

    Xu, Fan; Ma, Xin; Haughn, Chelsea R; Benavides, Jamie; Doty, Matthew F; Cloutier, Sylvain G

    2011-12-27

    Benzenedithiol (BDT) and ethanedithiol (EDT) ligand-exchange treatments can be used to cross-link colloidal PbS quantum dots into nanocrystalline film structures with distinct optoelectronic properties. Such structures can provide a unique platform to study the energy transfer between layers of quantum dots with different sizes. In this report, efficient exciton funneling and recycling of surface state-bound excitons is observed in cascaded PbS quantum dot-based multilayered superstructures, where the excitons transfer from the larger band gap or donor layers to the smallest band gap or acceptor layers. In this system, both the BDT- and EDT-treated cascaded structures exhibit dramatically enhanced photoluminescence from the acceptor layers. As we show, the energy transfer mechanisms involved and their efficiencies are significantly different depending on the ligand-exchange treatment. In the future, we believe these efficient exciton recycling and funneling mechanisms could be used to improve significantly the photocurrent, charge-transport, and conversion efficiencies in low-cost nanocrystalline and hybrid solar cells and the emission efficiencies in hybrid light-emitting devices.

  5. Ultrafast terahertz snapshots of excitonic Rydberg states and electronic coherence in an organometal halide perovskite

    DOE PAGES

    Luo, Liang; Men, Long; Liu, Zhaoyu; ...

    2017-06-01

    How photoexcitations evolve into Coulomb-bound electron and hole pairs, called excitons, and unbound charge carriers is a key cross-cutting issue in photovoltaics and optoelectronics. Until now, the initial quantum dynamics following photoexcitation remains elusive in the hybrid perovskite system. Furthermore we reveal excitonic Rydberg states with distinct formation pathways by observing the multiple resonant, internal quantum transitions using ultrafast terahertz quasi-particle transport. Nonequilibrium emergent states evolve with a complex co-existence of excitons, carriers and phonons, where a delayed buildup of excitons under on- and off-resonant pumping conditions allows us to distinguish between the loss of electronic coherence and hot statemore » cooling processes. The nearly ~1 ps dephasing time, efficient electron scattering with discrete terahertz phonons and intermediate binding energy of ~13.5 meV in perovskites are distinct from conventional photovoltaic semiconductors. In addition to providing implications for coherent energy conversion, these are potentially relevant to the development of light-harvesting and electron-transport devices.« less

  6. Dissociating excitons photogenerated in semiconducting carbon nanotubes at polymeric photovoltaic heterojunction interfaces.

    PubMed

    Bindl, Dominick J; Safron, Nathaniel S; Arnold, Michael S

    2010-10-26

    Semiconducting single-walled carbon nanotubes (s-SWCNTs) have strong near-infrared and visible absorptivity and exceptional charge transport characteristics, rendering them highly attractive semiconductor absorbers for photovoltaic and photodetector technologies. However, these applications are limited by a poor understanding of how photogenerated charges, which are bound as excitons in s-SWCNTs, can be dissociated in large-area solid-state devices. Here, we measure the dissociation of excitons in s-SWCNT thin films that form planar heterojunction interfaces with polymeric photovoltaic materials using an exciton dissociation-sensitive photocapacitor measurement technique that is advantageously insensitive to optically induced thermal photoconductive effects. We find that fullerene and polythiophene derivatives induce exciton dissociation, resulting in electron and hole transfer, respectively, away from optically excited s-SWCNTs. Significantly weaker or no charge transfer is observed using wider gap polymers due to insufficient energy offsets. These results are expected to critically guide the development of thin film s-SWCNT-based photosensitive devices.

  7. Excitonic effects in third-harmonic generation: The case of carbon nanotubes and nanoribbons

    NASA Astrophysics Data System (ADS)

    Attaccalite, C.; Cannuccia, E.; Grüning, M.

    2017-03-01

    Linear and nonlinear optical properties of low-dimensional nanostructures have attracted great interest from the scientific community as tools to probe the strong confinement of electrons and for possible applications in optoelectronic devices. In particular it has been shown that the linear optical response of carbon nanotubes [F. Wang et al., Science 308, 838 (2005), 10.1126/science.1110265] and graphene nanoribbons [Nat. Commun. 5 4253 (2014), 10.1038/ncomms5253] is dominated by bounded electron-hole pairs, excitons. The role of excitons in linear response has been widely studied, but still, little is known about their effect on nonlinear susceptibilities. Using a recently developed methodology [Phys. Rev. B 88, 235113 (2013), 10.1103/PhysRevB.88.235113] based on well-established ab initio many-body perturbation theory approaches, we find that quasiparticle shifts and excitonic effects significantly modify the third-harmonic generation in carbon nanotubes and graphene nanoribbons. For both systems the net effect of many-body effects is to reduce the intensity of the main peak in the independent-particle spectrum and redistribute the spectral weight among several excitonic resonances.

  8. Ultrafast terahertz snapshots of excitonic Rydberg states and electronic coherence in an organometal halide perovskite

    NASA Astrophysics Data System (ADS)

    Luo, Liang; Men, Long; Liu, Zhaoyu; Mudryk, Yaroslav; Zhao, Xin; Yao, Yongxin; Park, Joong M.; Shinar, Ruth; Shinar, Joseph; Ho, Kai-Ming; Perakis, Ilias E.; Vela, Javier; Wang, Jigang

    2017-06-01

    How photoexcitations evolve into Coulomb-bound electron and hole pairs, called excitons, and unbound charge carriers is a key cross-cutting issue in photovoltaics and optoelectronics. Until now, the initial quantum dynamics following photoexcitation remains elusive in the hybrid perovskite system. Here we reveal excitonic Rydberg states with distinct formation pathways by observing the multiple resonant, internal quantum transitions using ultrafast terahertz quasi-particle transport. Nonequilibrium emergent states evolve with a complex co-existence of excitons, carriers and phonons, where a delayed buildup of excitons under on- and off-resonant pumping conditions allows us to distinguish between the loss of electronic coherence and hot state cooling processes. The nearly ~1 ps dephasing time, efficient electron scattering with discrete terahertz phonons and intermediate binding energy of ~13.5 meV in perovskites are distinct from conventional photovoltaic semiconductors. In addition to providing implications for coherent energy conversion, these are potentially relevant to the development of light-harvesting and electron-transport devices.

  9. Polarization analysis of excitons in monolayer and bilayer transition-metal dichalcogenides

    NASA Astrophysics Data System (ADS)

    Dery, Hanan; Song, Yang

    2015-09-01

    The polarization analysis of optical transitions in monolayer and bilayer transition-metal dichalcogenides provides invaluable information on the spin and valley (pseudospin) degrees of freedom. To explain optical properties of a given monolayer transition-metal dichalcogenide, one should consider (i) the order of its spin-split conduction bands, (ii) whether intervalley scattering is prone to phonon bottleneck, (iii) and whether valley mixing by electron-hole exchange can take place. Using these principles, we present a consistent physical picture that elucidates a variety of features in the optical spectra of these materials. We explain the differences between optical transitions in monolayer MoSe2 and monolayer WSe2, finding that indirect excitons in the latter correspond to several low-energy optical transitions that so far were attributed to excitons bound to impurities. A possible mechanism that can explain the vanishing polarization in MoSe2 is discussed. Finally, we consider the effect of an out-of-plane electric field, showing that it can reduce the initial polarization of bright excitons due to a Rashba-type coupling with dark excitons.

  10. Localised and delocalised excitons in star-like squaraine homo- and heterotrimers.

    PubMed

    Ceymann, Harald; Balkenhohl, Moritz; Schmiedel, Alexander; Holzapfel, Marco; Lambert, Christoph

    2016-01-28

    Exciton coupling of localised chromophore states within covalently bound superchromophores is a viable strategy to modify optical properties such as spectral broadening and red-shifting of absorption bands. These are desirable properties for e.g. organic photovoltaic applications. Attaching three squaraine dyes to a central nitrogen core in a star-shaped manner leads to the formation of superchromophores that may form localised and delocalised excitons upon photoexcitation. In this work we investigated two homotrimers, two heterotrimers and a heterodimer formed by the combination of two different squaraines SQA and SQB. Due to exciton coupling the two homotrimers display a red shift of the main absorption band by about 1000 cm(-1) compared to their monomeric reference compounds. On the other hand, the heterotrimers show a broadening of the absorption spectra with three peak maxima at the exciton manifold band. In fluorescence experiments the homotrimers display signals similar to the emission of the monomeric compounds but red shifted. However, the heterotrimers and the heterodimer show, beside emission from the delocalised lowest energy state, an additional signal that overlaps strongly with the absorption. Excitation and time-dependent emission spectra of the hetero compounds indicate that this emission stems from a localised higher energy state. This interpretation is corroborated by transient absorption measurements with fs-time resolution.

  11. Excitons in a quasi-one-dimensional quantum nanorod under a strong electric field

    SciTech Connect

    Lyo, S. K.

    2014-03-21

    The response of an exciton in the ground and first excited states to a strong DC electric field is studied in a quasi-one-dimensional nano quantum well (i.e., nanorod) bounded by high symmetric barriers by studying the energy, the oscillator strength, the root-mean-square (RMS) average of the electron-hole (e-h) separation, and the average positions of the electron and the hole. The interplaying effect between the barrier confinement, e-h attraction, and the field-induced e-h separation for exciton binding is examined. We find that, for a long nanorod, the exciton energy, as well as, the oscillator strength drops abruptly as a function of the field near the exciton-dissociation field while the RMS average of the e-h separation rises rapidly. For shorter rods, the transition is more gradual due to the combined effect of the confinement and the long-range e-h interaction. A strong field is shown to transform the optically-inactive first excited state into an optically-active state in the field range between the dissociation field of the ground state and that of the first excited level. We also find that, in the ground state, the (lighter) electron is dragged by the (heavier) hole below the dissociation field. The dependence of the above mentioned properties on the rod length is also investigated for varying fields. The results are compared with those obtained for the rods with parabolic confinement.

  12. Highly efficient excitonic emission of CBD grown ZnO micropods (Presentation Recording)

    NASA Astrophysics Data System (ADS)

    Aad, Roy; Gokarna, Anisha; Nomenyo, Komla; Miska, Patrice; Geng, Wei; Couteau, Christophe; Lérondel, Gilles

    2015-10-01

    Due to its wide direct band gap and large exciton binding energy allowing for efficient excitonic emission at room temperature, ZnO has attracted attention as a luminescent material in various applications such as UV-light emitting diodes, chemical sensors and solar cells. While low-cost growth techniques, such as chemical bath deposition (CBD), of ZnO thin films and nanostructures have been already reported; nevertheless, ZnO thin films and nanostructures grown by costly techniques, such as metalorganic vapour phase epitaxy, still present the most interesting properties in terms of crystallinity and internal quantum efficiency. In this work, we report on highly efficient and highly crystalline ZnO micropods grown by CBD at a low temperature (< 90°C). XRD and low-temperature photoluminescence (PL) investigations on as-grown ZnO micropods revealed a highly crystalline ZnO structure and a strong UV excitonic emission with internal quantum efficiency (IQE) of 10% at room temperature. Thermal annealing at 900°C of the as-grown ZnO micropods leads to further enhancement in their structural and optical properties. Low-temperature PL measurements on annealed ZnO micropods showed the presence of phonon replicas, which was not the case for as-grown samples. The appearance of phonon replicas provides a strong proof of the improved crystal quality of annealed ZnO micropods. Most importantly, low-temperature PL reveals an improved IQE of 15% in the excitonic emission of ZnO micropods. The ZnO micropods IQE reported here are comparable to IQEs reported on ZnO structures obtained by costly and more complex growth techniques. These results are of great interest demonstrating that high quality ZnO microstructures can be obtained at low temperatures using a low-cost CBD growth technique.

  13. Photophysics of the cationic 5,10,15,20-tetrakis (4-N-methylpyridyl) porphyrin bound to DNA, [poly (dA-dT)]2 and [poly (dG-dC)]2: interaction with molecular oxygen studied by porphyrin triplet-triplet absorption and singlet oxygen luminescence.

    PubMed

    Kruk, N N; Dzhagarov, B M; Galievsky, V A; Chirvony, V S; Turpin, P Y

    1998-03-01

    Interaction between molecular oxygen and the cationic free-base 5,10,15,20-tetrakis (4-N-methylpyridyl) porphyrin (H2TMpyP4+) complexed with [poly (dA-dT)]2, [poly (dG-dC)]2 and calf thymus DNA, has been monitored in air-saturated heavy water solutions through porphyrin triplet-triplet absorption and singlet oxygen luminescence. Three different rate constants of porphyrin triplet state quenching have been found which correspond to different accessibilities of molecular oxygen to porphyrins embedded in the duplexes. The longest triplet state lifetime (30 microseconds), found for porphyrin bound to [poly (dG-dC)]2, corresponds to molecules well protected from oxygen. This supports the hypothesis of an intercalative binding mode of the porphyrin between GC base-pairs ('type A' sites). The fraction fT delta of the porphyrin triplet states quenched by molecular oxygen with singlet oxygen generation, is unity. In [poly (dA-dT)]2-porphyrin complexes, two sites ('type B' and 'C' sites of interaction) are involved, yielding very different triplet state lifetimes (5.5 microseconds and 20.5 microseconds) and efficiencies of singlet oxygen generation (fT delta = 0.50 and 0.82). The fT delta decreases can likely be explained in terms of competition between energy and electron transfer from the porphyrin excited triplet state to molecular oxygen. All three types (A, B and C) of interaction sites can be expected in porphyrin-DNA complexes.

  14. Recombination luminescence of LaPO4-Eu and LaPO4-Pr nanoparticles

    NASA Astrophysics Data System (ADS)

    Malyy, T. S.; Vistovskyy, V. V.; Khapko, Z. A.; Pushak, A. S.; Mitina, N. E.; Zaichenko, A. S.; Gektin, A. V.; Voloshinovskii, A. S.

    2013-06-01

    The study of the spectral-luminescence parameters of LaPO4-Eu and LaPO4-Pr nanoparticles upon excitation by the synchrotron radiation with photon energies 4-40 eV was performed. The differences of the luminescence intensity dependence on the size for LaPO4-Eu and LaPO4-Pr nanoparticles excited at the range of matrix transparency, the range of band-to-band transitions, and the range of electronic excitation multiplication were revealed. The observed regularities are explained in terms of the electron-phonon and electron-electron scattering, surface losses, and exciton diffusion. The ratio between the length of thermalization and electron mean free path and the size of nanoparticle is determinative for the luminescence intensity upon excitation in the range of fundamental absorption of matrix and X-ray excitation.

  15. Defect luminescence in films containing Ge and GeO{sub 2} nanocrystals

    SciTech Connect

    Zacharias, M.; Atherton, S.J.; Fauchet, P.M.

    1997-07-01

    Amorphous SiO{sub x} alloys containing Ge or GeO{sub 2} nanocrystals are produced by dc-magnetron sputtering and controlled crystallization. The samples are investigated by Raman scattering, transmission electron microscopy, photoluminescence and excitation spectroscopy. Under UV excitation, both types of films luminesce around 3.1 eV, with identical PL line shapes and subnanosecond PL dynamics. The strongest PL intensity is found for the films containing FeO{sub 2} crystals and for the largest nanocrystals. These results are a clear indication that although the blue luminescence is without a doubt correlated with the formation of Ge (or GeO{sub 2}) nanocrystals, it is not produced by the radiative recombination of excitons confined in the nanocrystals. Possible mechanisms for the luminescence are discussed, including defects at the nanocrystal/matric interface or in the matrix itself.

  16. Stark effect of intrinsic and extrinsic charge-transfer excitons in a linear donor-acceptor stack: anthracene-pyromellitic dianhydride.

    PubMed

    Weiser, Gerhard; Elschner, Andreas

    2009-06-25

    Anthracene-PMDA single crystals display at 2K about 70 meV below a well-known intrinsic charge-transfer exciton three narrow absorption lines, which are attributed to CT excitons bound to defects of a few 10(-5) concentration. All excitons respond very sensitively to electric fields along the molecular stack because of the large dipole moment, about 2 eA, of an ionized donor-acceptor pair, but only intrinsic excitons observe an optical selection rule. Although the triclinic unit cell contains only one pair of molecules, excitons appear in field-modulated spectra as near-degenerate doublets of different parity with very small splitting. The line shape of the EA spectra and selection rules with respect to the polarization of light and orientation of the field are consistent with the inversion symmetry of the lattice and the molecules. The simple crystal structure enables identification of the defects that are responsible for extrinsic excitons. Symmetry consideration based on translation invariance lead to a new interpretation of intrinsic excitons as true crystal states with charge transfer from the donor to the acceptor sublattice.

  17. Plasmon-excitonic polaritons in superlattices

    NASA Astrophysics Data System (ADS)

    Kosobukin, V. A.

    2017-05-01

    A theory for propagation of polaritons in superlattices with resonant plasmon-exciton coupling is presented. A periodical superlattice consists of a finite number of cells with closely located a quantum well and a monolayer of metal nanoparticles. Under study is the spectrum of hybrid modes formed of the quasitwo- dimensional excitons of quantum wells and the dipole plasmons of metal particles. The problem of electrodynamics is solved by the method of Green's functions with taking account of the resonant polarization of quantum wells and nanoparticles in a self-consistent approximation. The effective polarizability of spheroidal particles occupying a square lattice is calculated with taking into consideration the local-field effect of dipole plasmons of the layer and their images caused by the excitonic polarization of nearest quantum well. Optical reflection spectra of superlattices with GaAs/AlGaAs quantum wells and silver particles are numerically analyzed. Special attention is paid to the superradiant regime originated in the Bragg diffraction of polaritons in superlattice. Superradiance is investigated separately for plasmons and excitons, and then for hybrid plasmonexcitonic polaritons. It is demonstrated that the broad spectrum of reflectance associated with plasmons depends on the number of cells in superlattice, and it has a narrow spectral dip in the range of plasmon-excitonic Rabi splitting.

  18. Excitonic Coupling Modulated by Mechanical Stimuli.

    PubMed

    Pirrotta, Alessandro; Solomon, Gemma C; Franco, Ignacio; Troisi, Alessandro

    2017-09-21

    Understanding energy transfer is of vital importance in a diverse range of applications from biological systems to photovoltaics. The ability to tune excitonic coupling in any of these systems, however, is generally limited. In this work, we have simulated a new class of single-molecule spectroscopy in which force microscopy is used to control the excitonic coupling between chromophores. Here we demonstrate that the excitonic coupling can be controlled by mechanical manipulation of the molecule (perylenediimide dimers and terrylenediimide-perylenediimide heterodimers) and can be tuned over a broad range of values (0.02-0.15 eV) that correspond to different regimes of exciton dynamics going from the folded to the elongated structure of the dimer. In all of the systems considered here, the switching from high to low coupling takes place simultaneously with the mechanical deformation detected by a strong increase and subsequent decay of the force. These simulations suggest that single-molecule force spectroscopy can be used to understand and eventually aid the design of excitonic devices.

  19. Lanthanide luminescence enhancements in porous silicon resonant microcavities.

    PubMed

    Jenie, S N Aisyiyah; Pace, Stephanie; Sciacca, Beniamino; Brooks, Robert D; Plush, Sally E; Voelcker, Nicolas H

    2014-08-13

    In this paper, the covalent immobilization and luminescence enhancement of a europium (Eu(III)) complex in a porous silicon (pSi) layer with a microcavity (pSiMC) structure are demonstrated. The alkyne-pendant arm of the Eu(III) complex was covalently immobilized on the azide-modified surface via ligand-assisted "click" chemistry. The design parameters of the microcavity were optimized to obtain an efficient luminescence-enhancing device. Luminescence enhancements by a factor of 9.5 and 3.0 were observed for Eu(III) complex bound inside the pSiMC as compared to a single layer and Bragg reflector of identical thickness, respectively, confirming the increased interaction between the immobilized molecules and the electric field in the spacer of the microcavity. When comparing pSiMCs with different resonance wavelength position, luminescence was enhanced when the resonance wavelength overlapped with the maximum emission wavelength of the Eu(III) complex at 614 nm, allowing for effective coupling between the confined light and the emitting molecules. The pSiMC also improved the spectral color purity of the Eu(III) complex luminescence. The ability of a pSiMC to act as an efficient Eu(III) luminescence enhancer, combined with the resulting sharp linelike emission, can be exploited for the development of ultrasensitive optical biosensors.

  20. Theoretical study on the cooperative exciton dissociation process based on dimensional and hot charge-transfer state effects in an organic photocell

    NASA Astrophysics Data System (ADS)

    Shimazaki, Tomomi; Nakajima, Takahito

    2016-06-01

    This paper discusses the exciton dissociation process at the donor-acceptor interface in organic photocells. In our previous study, we introduced a local temperature to handle the hot charge-transfer (CT) state and calculated the exciton dissociation probability based on the 1D organic semiconductor model [T. Shimazaki and T. Nakajima, Phys. Chem. Chem. Phys. 17, 12538 (2015)]. Although the hot CT state plays an essential role in exciton dissociations, the probabilities calculated are not high enough to efficiently separate bound electron-hole pairs. This paper focuses on the dimensional (entropy) effect together with the hot CT state effect and shows that cooperative behavior between both effects can improve the exciton dissociation process. In addition, we discuss cooperative effects with site-disorders and external-electric-fields.

  1. Two-Exciton and Exciton-Magnon Bands in DIMANGANESE(+) Magnets.

    NASA Astrophysics Data System (ADS)

    Darwish, Saqer Mohammed

    The temperature dependence of several exciton -magnon and two-exciton bands in the optical absorption spectra of three antiferromagnets have been studied using a Cary 14 spectrophotometer in conjunction with an Air Product Displex, closed-cycle helium refrigerator. The three antiferromagnets with their T_{ rm N} are: KMnF_3, T_{rm N} = 88.3 K; RbMnF_3, T_{ rm N} = 82.6 K; and MnF_2 , T_{rm N} = 67.3 K. In this work the temperature dependence (10 ^circK to 300^ circK) of the line position E, the oscillator strength f, and the half-width of half maximum delta, for several of these bands were measured. For the two-exciton bands f increases where as for the exciton-magnon and exciton-magnon-phonon bands f decreases as the temperature is lowered through T _{rm N}. The temperature dependence of f for the two-exciton bands in the three antiferromagnets agrees well with the theoretical predictions of Fujiwara et al. For the exciton-magnon bands, f increases with increasing T up to T_{rm N} and then remains essentially constant above T_{rm N}, in reasonable agreement with the theory of Shinagawa and Tanabe. For the exciton-magnon-phonon bands, a slight increase in f above T_{rm N} is believed to be due to the role of a phonon. The temperature dependence of the line positions E(T) is also different for the exciton-magnon and two-exciton bands. The exciton-magnon or exciton-magnon-phonon bands undergo a blue shift in E(T) as the temperature is lowered through T_{rm N}. This is semiquantitatively understood in terms of the exchange field using the molecular field theory of Yen et al. On the other hand, most of the two-exciton bands do not show any anomaly in E(T) below T_{rm N}. Instead their line positions are described well by the Einstein-type relation E(T) = E(O) + A ^{*}/ (exp(T^ {*}/T) - 1), where T^{*} represents an odd symmetry phonon with frequency upsilon * = kT^{*} /h. Above T_{rm N} , the exciton-magnon-phonon bands also follow the same equation. From these fits

  2. Exciton-to-Dopant Energy Transfer in Mn-Doped Cesium Lead Halide Perovskite Nanocrystals.

    PubMed

    Parobek, David; Roman, Benjamin J; Dong, Yitong; Jin, Ho; Lee, Elbert; Sheldon, Matthew; Son, Dong Hee

    2016-12-14

    We report the one-pot synthesis of colloidal Mn-doped cesium lead halide (CsPbX3) perovskite nanocrystals and efficient intraparticle energy transfer between the exciton and dopant ions resulting in intense sensitized Mn luminescence. Mn-doped CsPbCl3 and CsPb(Cl/Br)3 nanocrystals maintained the same lattice structure and crystallinity as their undoped counterparts with nearly identical lattice parameters at ∼0.2% doping concentrations and no signature of phase separation. The strong sensitized luminescence from d-d transition of Mn(2+) ions upon band-edge excitation of the CsPbX3 host is indicative of sufficiently strong exchange coupling between the charge carriers of the host and dopant d electrons mediating the energy transfer, essential for obtaining unique properties of magnetically doped quantum dots. Highly homogeneous spectral characteristics of Mn luminescence from an ensemble of Mn-doped CsPbX3 nanocrystals and well-defined electron paramagnetic resonance spectra of Mn(2+) in host CsPbX3 nanocrystal lattices suggest relatively uniform doping sites, likely from substitutional doping at Pb(2+). These observations indicate that CsPbX3 nanocrystals, possessing many superior optical and electronic characteristics, can be utilized as a new platform for magnetically doped quantum dots expanding the range of optical, electronic, and magnetic functionality.

  3. Exciton-Exciton Annihilation in Copper-Phthalocyanine Single-Crystal Nanowires

    SciTech Connect

    Ma, Yingzhong; Xiao, Kai; Shaw, Robert W

    2012-01-01

    Femtosecond one-color pump-probe spectroscopy was applied to study exciton dynamics in single-crystal copper-phthalocyanine (CuPc) nanowires grown on an opaque silicon substrate. The transient reflectance kinetics measured at different pump fluences exhibit a remarkable intensity-dependent decay behavior which accelerates significantly with increasing pump pulse intensity. All the kinetic decays can be satisfactorily described using a bi-exponential decay function with lifetimes of 22 and 204 ps, and corresponding relative amplitudes depending on the pump intensity. The accelerated decay behavior observed at high pump intensities arises from a nonlinear exciton-exciton annihilation process. While this phenomenon has been found previously in crystalline metallophthalocyanine (MPc) polymorphs such as colloidal particles and thin films, the results obtained using the CuPc nanowires are markedly distinct, namely, much longer decay times and a linear intensity dependence of the initial peak amplitudes. Despite these differences, detailed data analysis further shows that, as found for other metal-phthalocyanine polymorphs, exciton-exciton annihilation in the CuPc nanowires is one-dimensional (1D) diffusion-limited, which possibly involves intra-chain exciton diffusion along 1D molecular stacks. The significantly long-lived excitons of CuPc nanowires in comparison to those of other crystalline polymorphs make them particularly suitable for photovoltaic applications.

  4. Microscopic theory of two-dimensional spatially-indirect-exciton condensates and exciton-polariton condensates

    NASA Astrophysics Data System (ADS)

    Xue, Fei; Wu, Feng Cheng; MacDonald, Allan

    BEC of excitons and polaritons have drawn attention in recent years because of the demonstration of their ability to host macroscopic quantum phenomena and because of their promise for applications. We study the case of a system containing two TMD monolayers that are separated and surrounded by h-BN. Under appropriate conditions this system is expected to support a spatially indirect thermal equilibrium exciton condensate. We combine a microscopic mean-field calculation and a weakly interacting boson model to explore the bilayer exciton condensates phase diagram. By varying the layer separation and exciton density, we find a phase transition occurs between states containing one and two condensate flavors. We also use a microscopic time-dependent mean-field theory to address condensate collective mode spectra and quantum fluctuations. Next we study the case of exciton-polariton formed by strong coupling between quantum well excitons and confined photon modes when the system is placed in a vertical microcavity. We build a microscopic mean-field theory starting from electrons and holes, and account for their coupling to coherent light field. We compare our model with the normal weakly interacting boson model that starts from weakly interacting excitons that are coupled to photons. This work was supported by the SRC and NIST under the Nanoelectronic Research Initiative (NRI) and SWAN, by the Welch Foundation under Grant No. F1473, and by the ARO Grant No. 26-3508-81.

  5. Optically Discriminating Carrier-Induced Quasiparticle Band Gap and Exciton Energy Renormalization in Monolayer MoS2

    NASA Astrophysics Data System (ADS)

    Yao, Kaiyuan; Yan, Aiming; Kahn, Salman; Suslu, Aslihan; Liang, Yufeng; Barnard, Edward S.; Tongay, Sefaattin; Zettl, Alex; Borys, Nicholas J.; Schuck, P. James

    2017-08-01

    Optoelectronic excitations in monolayer MoS2 manifest from a hierarchy of electrically tunable, Coulombic free-carrier and excitonic many-body phenomena. Investigating the fundamental interactions underpinning these phenomena—critical to both many-body physics exploration and device applications—presents challenges, however, due to a complex balance of competing optoelectronic effects and interdependent properties. Here, optical detection of bound- and free-carrier photoexcitations is used to directly quantify carrier-induced changes of the quasiparticle band gap and exciton binding energies. The results explicitly disentangle the competing effects and highlight longstanding theoretical predictions of large carrier-induced band gap and exciton renormalization in two-dimensional semiconductors.

  6. Estimating Excitonic Effects in the Absorption Spectra of Solids: Problems and Insight from a Guided Iteration Scheme

    NASA Astrophysics Data System (ADS)

    Rigamonti, Santiago; Botti, Silvana; Veniard, Valérie; Draxl, Claudia; Reining, Lucia; Sottile, Francesco

    2015-04-01

    A major obstacle for computing optical spectra of solids is the lack of reliable approximations for capturing excitonic effects within time-dependent density functional theory. We show that the accurate prediction of strongly bound electron-hole pairs within this framework using simple approximations is still a challenge and that available promising results have to be revisited. Deriving a set of analytical formulas we analyze and explain the difficulties. We deduce an alternative approximation from an iterative scheme guided by previously available knowledge, significantly improving the description of exciton binding energies. Finally, we show how one can "read" exciton binding energies from spectra determined in the random phase approximation, without any further calculation.

  7. Disorder-enhanced exciton delocalization in an extended dendrimer

    NASA Astrophysics Data System (ADS)

    Pouthier, Vincent

    2014-08-01

    The exciton dynamics in a disordered extended dendrimer is investigated numerically. Because a homogeneous dendrimer exhibits few highly degenerate energy levels, a dynamical localization arises when the exciton is initially located on the periphery. However, it is shown that the disorder lifts the degeneracy and favors a delocalization-relocalization transition. Weak disorder enhances the delocalized nature of the exciton and improves any quantum communication, whereas strong disorder prevents the exciton from propagating in accordance with the well-known Anderson theory.

  8. Probing Bose-Einstein condensation of excitons with electromagnetic radiation.

    PubMed

    Johnsen, K; Kavoulakis, G M

    2001-01-29

    We examine the absorption spectrum of electromagnetic radiation from excitons, where an exciton in the 1s state absorbs a photon and makes a transition to the 2p state. We demonstrate that the absorption spectrum depends strongly on the quantum degeneracy of the exciton gas, and that it will generally manifest many-body effects. Based on our results we propose that absorption of infrared radiation could resolve recent contradictory experimental results on excitons in Cu(2)O.

  9. Bose-Einstein condensation and indirect excitons: a review

    NASA Astrophysics Data System (ADS)

    Combescot, Monique; Combescot, Roland; Dubin, François

    2017-06-01

    We review recent progress on Bose-Einstein condensation (BEC) of semiconductor excitons. The first part deals with theory, the second part with experiments. This Review is written at a time where the problem of exciton Bose-Einstein condensation has just been revived by the understanding that the exciton condensate must be dark because the exciton ground state is not coupled to light. Here, we theoretically discuss this missed understanding before providing its experimental support through experiments that scrutinize indirect excitons made of spatially separated electrons and holes. The theoretical part first discusses condensation of elementary bosons. In particular, the necessary inhibition of condensate fragmentation by exchange interaction is stressed, before extending the discussion to interacting bosons with spin degrees of freedom. The theoretical part then considers composite bosons made of two fermions like semiconductor excitons. The spin structure of the excitons is detailed, with emphasis on the crucial fact that ground-state excitons are dark: indeed, this imposes the exciton Bose-Einstein condensate to be not coupled to light in the dilute regime. Condensate fragmentations are then reconsidered. In particular, it is shown that while at low density, the exciton condensate is fully dark, it acquires a bright component, coherent with the dark one, beyond a density threshold: in this regime, the exciton condensate is ‘gray’. The experimental part first discusses optical creation of indirect excitons in quantum wells, and the detection of their photoluminescence. Exciton thermalisation is also addressed, as well as available approaches to estimate the exciton density. We then switch to specific experiments where indirect excitons form a macroscopic fragmented ring. We show that such ring provides efficient electrostatic trapping in the region of the fragments where an essentially-dark exciton Bose-Einstein condensate is formed at sub-Kelvin bath

  10. Excitons in Time-Dependent Density-Functional Theory.

    PubMed

    Ullrich, Carsten A; Yang, Zeng-hui

    2016-01-01

    This chapter gives an overview of the description of the optical and dielectric properties of bulk insulators and semiconductors in time-dependent density-functional theory (TDDFT), with an emphasis on excitons. We review the linear-response formalism for periodic solids, discuss excitonic exchange-correlation kernels, calculate exciton binding energies for various materials, and compare the treatment of excitons with TDDFT and with the Bethe-Salpeter equation.

  11. Bose-Einstein condensation and indirect excitons: a review.

    PubMed

    Combescot, Monique; Combescot, Roland; Dubin, François

    2017-06-01

    We review recent progress on Bose-Einstein condensation (BEC) of semiconductor excitons. The first part deals with theory, the second part with experiments. This Review is written at a time where the problem of exciton Bose-Einstein condensation has just been revived by the understanding that the exciton condensate must be dark because the exciton ground state is not coupled to light. Here, we theoretically discuss this missed understanding before providing its experimental support through experiments that scrutinize indirect excitons made of spatially separated electrons and holes. The theoretical part first discusses condensation of elementary bosons. In particular, the necessary inhibition of condensate fragmentation by exchange interaction is stressed, before extending the discussion to interacting bosons with spin degrees of freedom. The theoretical part then considers composite bosons made of two fermions like semiconductor excitons. The spin structure of the excitons is detailed, with emphasis on the crucial fact that ground-state excitons are dark: indeed, this imposes the exciton Bose-Einstein condensate to be not coupled to light in the dilute regime. Condensate fragmentations are then reconsidered. In particular, it is shown that while at low density, the exciton condensate is fully dark, it acquires a bright component, coherent with the dark one, beyond a density threshold: in this regime, the exciton condensate is 'gray'. The experimental part first discusses optical creation of indirect excitons in quantum wells, and the detection of their photoluminescence. Exciton thermalisation is also addressed, as well as available approaches to estimate the exciton density. We then switch to specific experiments where indirect excitons form a macroscopic fragmented ring. We show that such ring provides efficient electrostatic trapping in the region of the fragments where an essentially-dark exciton Bose-Einstein condensate is formed at sub-Kelvin bath

  12. Excitonic superfluid phase in double bilayer graphene

    NASA Astrophysics Data System (ADS)

    Li, J. I. A.; Taniguchi, T.; Watanabe, K.; Hone, J.; Dean, C. R.

    2017-08-01

    A spatially indirect exciton is created when an electron and a hole, confined to separate layers of a double quantum well system, bind to form a composite boson. Such excitons are long-lived, and in the limit of strong interactions are predicted to undergo a Bose-Einstein condensate-like phase transition into a superfluid ground state. Here, we report evidence of an exciton condensate in the quantum Hall effect regime of double-layer structures of bilayer graphene. Interlayer correlation is identified by quantized Hall drag at matched layer densities, and the dissipationless nature of the phase is confirmed in the counterflow geometry. A selection rule for the condensate phase is observed involving both the orbital and valley indices of bilayer graphene. Our results establish double bilayer graphene as an ideal system for studying the rich phase diagram of strongly interacting bosonic particles in the solid state.

  13. Triplet excitons in 4,4'-dichlorobenzophenone

    SciTech Connect

    Singham, S.B.; Pratt, D.W.

    1982-02-18

    Low-temperature optical and magnetic resonance experiments, both continuous-wave (CW) and time-resolved, have been performed on photoexcited single crystals of 4,4'-dichlorobenzophenone (DCBP). The CW results show the presence of both triplet excitons and several intrinsic traps in this system. A kinetic model is developed to describe excitation transport between exciton and trap states in the presence of resonant microwaves. By comparing the results of the time-resolved experiments with the predictions of the model, we conclude that the triplet exciton lifetime in DCBP is of the order of microseconds or less. This lifetime, which is much shorter than those in pseudo-one-dimensional systems, appears to be a consequence of the two-dimensional nature of the exchange interaction in the DCBP crystal.

  14. Excitonic interaction in the fluorene dimer

    NASA Astrophysics Data System (ADS)

    Wessel, John; Beck, Steven; Highstrete, Clark

    1994-12-01

    The fluorene van der Waals dimer exhibits a complex origin spectrum. This region has been studied by resonance two-photon ionization and by fluorescence excitation spectroscopies. The spectra can be interpreted on the basis of intermediate strength exciton coupling, in which the electronic interaction is comparable to the van der Waals vibrational energies. The spectra are reasonably well described by two distorted adiabatic potential surfaces, which correspond to the two excitonic components of the origin system. A single Franck-Condon active intermolecular mode provides a reasonable description of the system, however the potentials have significant cubic and quartic contributions. Non-Born-Oppenheimer nuclear momentum coupling is present and intermodal (IVR) interactions are observed, even for intermolecular modes as low as v=1. The results are remarkably different from prior observations of excitonic structure in other systems, providing a detailed picture of coupling between electronic and intermolecular motion in a van der Waals dimer.

  15. Lunar luminescence measurements

    NASA Technical Reports Server (NTRS)

    Morgan, T. H.

    1983-01-01

    Spectra of lunar sites obtained in June 1983 have been analyzed for residual luminescence using the spectral line depth technique. The results or three sites each at three wavelengths are presented. The sites observed were Mare Crisium, Kepler, and Aristarchus. In each case, the value quoted was based not only on the strong Fraunhofer line in the spectral range covered but also on from 11 to 21 weaker lines within 80 A of the strongest feature. These data do not support previous observations. The values given do not indicate a greatly reddened spectrum, and the luminescence spectrum of the mare site is not significantly different from the two young crater sites. These observations cannot be adequately explained by thermal luminescence, theories of direct excitation are also unable to explain the strength of the flux.

  16. Observation of charged excitons in V-groove quantum wires

    NASA Astrophysics Data System (ADS)

    Otterburg, T.; Oberli, D. Y.; Dupertuis, M.-A.; Dwir, B.; Pelucchi, E.; Kapon, E.

    2004-02-01

    We report on the observation of negatively and positively charged excitons in the photoluminescence spectra of V-groove quantum wires. The charged exciton binding energy increases with the strength of the quantum confinement. We demonstrate that the charged excitons are localized by the fluctuations of the confinement potential and estimate a minimal value of the localization length.

  17. Exciton Level Structure and Dynamics in Tubular Porphyrin Aggregates

    SciTech Connect

    Wan, Yan; Stradomska, Anna; Fong, Sarah; Guo, Zhi; Schaller, Richard D.; Wiederrecht, Gary P; Knoester, Jasper; Huang, Libai

    2014-10-30

    We present an account of the optical properties of the Frenkel excitons in self-assembled porphyrin tubular aggregates that represent an analog to natural photosynthetic antennae. Using a combination of ultrafast optical spectroscopy and stochastic exciton modeling, we address both linear and nonlinear exciton absorption, relaxation pathways, and the role of disorder. The static disorder-dominated absorption and fluorescence line widths show little temperature dependence for the lowest excitons (Q band), which we successfully simulate using a model of exciton scattering on acoustic phonons in the host matrix. Temperature-dependent transient absorption of and fluorescence from the excitons in the tubular aggregates are marked by nonexponential decays with time scales ranging from a few picoseconds to a few nanoseconds, reflecting complex relaxation mechanisms. Combined experimental and theoretical investigations indicate that nonradiative pathways induced by traps and defects dominate the relaxation of excitons in the tubular aggregates. We model the pumpprobe spectra and ascribe the excited-state absorption to transitions from one-exciton states to a manifold of mixed one- and two-exciton states. Our results demonstrate that while the delocalized Frenkel excitons (over 208 (1036) molecules for the optically dominant excitons in the Q (B) band) resulting from strong intermolecular coupling in these aggregates could potentially facilitate efficient energy transfer, fast relaxation due to defects and disorder probably present a major limitation for exciton transport over large distances.

  18. Positive Root Bounds and Root Separation Bounds

    NASA Astrophysics Data System (ADS)

    Herman, Aaron Paul

    In this thesis, we study two classes of bounds on the roots of a polynomial (or polynomial system). A positive root bound of a polynomial is an upper bound on the largest positive root. A root separation bound of a polynomial is a lower bound on the distance between the roots. Both classes of bounds are fundamental tools in computer algebra and computational real algebraic geometry, with numerous applications. In the first part of the thesis, we study the quality of positive root bounds. Higher quality means that the relative over-estimation (the ratio of the bound and the largest positive root) is smaller. We find that all known positive root bounds can be arbitrarily bad. We then show that a particular positive root bound is tight for certain important classes of polynomials. In the remainder of the thesis, we turn to root separation bounds. We observe that known root separation bounds are usually very pessimistic. To our surprise, we also find that known root separation bounds are not compatible with the geometry of the roots (unlike positive root bounds). This motivates us to derive new root separation bounds. In the second part of this thesis, we derive a new root separation for univariate polynomials by transforming a known bound into a new improved bound. In the third part of this thesis, we use a similar strategy to derive a new improved root separation bound for polynomial systems.

  19. Exciton dynamics in perturbed vibronic molecular aggregates

    PubMed Central

    Brüning, C.; Wehner, J.; Hausner, J.; Wenzel, M.; Engel, V.

    2015-01-01

    A site specific perturbation of a photo-excited molecular aggregate can lead to a localization of excitonic energy. We investigate this localization dynamics for laser-prepared excited states. Changing the parameters of the electric field significantly influences the exciton localization which offers the possibility for a selective control of this process. This is demonstrated for aggregates possessing a single vibrational degree of freedom per monomer unit. It is shown that the effects identified for the molecular dimer can be generalized to larger aggregates with a high density of vibronic states. PMID:26798840

  20. Excitons and energy transport in crystals KPb 2Cl 5 and RbPb 2Br 5

    NASA Astrophysics Data System (ADS)

    Pustovarov, V. A.; Ogorodnikov, I. N.; Omelkov, S. I.; Smirnov, A. A.; Yelisseyev, A. P.

    2005-05-01

    A complex investigation of the dynamics of electronic excitations and energy transport in the KPb 2Cl 5 (KPC) and RbPb 2Br 5 (RPB) crystals was performed by means of low-temperature time-resolved vacuum ultraviolet optical luminescence spectroscopy with time resolution under selective excitation with synchrotron radiation. Data on the kinetics of the photoluminescence (PL) decay, time-resolved PL spectra (2-6.2 eV), and time-resolved PL excitation spectra (4-24 eV) at 7-300 K were obtained for the first time. The intrinsic PL bands at 2.4 (KPC) and 2.05 eV (RPB) were attributed to the radiative annihilation of the triplet excitons. This rare-earth (Pr, Er, Nd, Ho) doped crystals exhibit the characteristic luminescence of the appropriate activators. This paper discusses the electronic excitation dynamics and energy transport in these crystals.

  1. Nanostructured luminescently labeled nucleic acids.

    PubMed

    Kricka, Larry J; Fortina, Paolo; Park, Jason Y

    2017-03-01

    Important and emerging trends at the interface of luminescence, nucleic acids and nanotechnology are: (i) the conventional luminescence labeling of nucleic acid nanostructures (e.g. DNA tetrahedron); (ii) the labeling of bulk nucleic acids (e.g. single-stranded DNA, double-stranded DNA) with nanostructured luminescent labels (e.g. copper nanoclusters); and (iii) the labeling of nucleic acid nanostructures (e.g. origami DNA) with nanostructured luminescent labels (e.g. silver nanoclusters). This review surveys recent advances in these three different approaches to the generation of nanostructured luminescently labeled nucleic acids, and includes both direct and indirect labeling methods. Copyright © 2016 John Wiley & Sons, Ltd.

  2. Excitons in van der Waals heterostructures: The important role of dielectric screening

    NASA Astrophysics Data System (ADS)

    Latini, S.; Olsen, T.; Thygesen, K. S.

    2015-12-01

    The existence of strongly bound excitons is one of the hallmarks of the newly discovered atomically thin semiconductors. While it is understood that the large binding energy is mainly due to the weak dielectric screening in two dimensions, a systematic investigation of the role of screening on two-dimensional (2D) excitons is still lacking. Here we provide a critical assessment of a widely used 2D hydrogenic exciton model, which assumes a dielectric function of the form ɛ (q )=1 +2 π α q , and we develop a quasi-2D model with a much broader applicability. Within the quasi-2D picture, electrons and holes are described as in-plane point charges with a finite extension in the perpendicular direction, and their interaction is screened by a dielectric function with a nonlinear q dependence which is computed ab initio. The screened interaction is used in a generalized Mott-Wannier model to calculate exciton binding energies in both isolated and supported 2D materials. For isolated 2D materials, the quasi-2D treatment yields results almost identical to those of the strict 2D model, and both are in good agreement with ab initio many-body calculations. On the other hand, for more complex structures such as supported layers or layers embedded in a van der Waals heterostructure, the size of the exciton in reciprocal space extends well beyond the linear regime of the dielectric function, and a quasi-2D description has to replace the 2D one. Our methodology has the merit of providing a seamless connection between the strict 2D limit of isolated monolayer materials and the more bulk-like screening characteristics of supported 2D materials or van der Waals heterostructures.

  3. Exciton effects in the index of refraction of multiple quantum wells and superlattices

    NASA Technical Reports Server (NTRS)

    Kahen, K. B.; Leburton, J. P.

    1986-01-01

    Theoretical calculations of the index of refraction of multiple quantum wells and superlattices are presented. The model incorporates both the bound and continuum exciton contributions for the gamma region transitions. In addition, the electronic band structure model has both superlattice and bulk alloy properties. The results indicate that large light-hole masses, i.e., of about 0.23, produced by band mixing effects, are required to account for the experimental data. Furthermore, it is shown that superlattice effects rapidly decrease for energies greater than the confining potential barriers. Overall, the theoretical results are in very good agreement with the experimental data and show the importance of including exciton effects in the index of refraction.

  4. Extremely efficient internal exciton dissociation through edge states in layered 2D perovskites

    NASA Astrophysics Data System (ADS)

    Blancon, J.-C.; Tsai, H.; Nie, W.; Stoumpos, C. C.; Pedesseau, L.; Katan, C.; Kepenekian, M.; Soe, C. M. M.; Appavoo, K.; Sfeir, M. Y.; Tretiak, S.; Ajayan, P. M.; Kanatzidis, M. G.; Even, J.; Crochet, J. J.; Mohite, A. D.

    2017-03-01

    Understanding and controlling charge and energy flow in state-of-the-art semiconductor quantum wells has enabled high-efficiency optoelectronic devices. Two-dimensional (2D) Ruddlesden-Popper perovskites are solution-processed quantum wells wherein the band gap can be tuned by varying the perovskite-layer thickness, which modulates the effective electron-hole confinement. We report that, counterintuitive to classical quantum-confined systems where photogenerated electrons and holes are strongly bound by Coulomb interactions or excitons, the photophysics of thin films made of Ruddlesden-Popper perovskites with a thickness exceeding two perovskite-crystal units (>1.3 nanometers) is dominated by lower-energy states associated with the local intrinsic electronic structure of the edges of the perovskite layers. These states provide a direct pathway for dissociating excitons into longer-lived free carriers that substantially improve the performance of optoelectronic devices.

  5. Extremely efficient internal exciton dissociation through edge states in layered 2D perovskites.

    PubMed

    Blancon, J-C; Tsai, H; Nie, W; Stoumpos, C C; Pedesseau, L; Katan, C; Kepenekian, M; Soe, C M M; Appavoo, K; Sfeir, M Y; Tretiak, S; Ajayan, P M; Kanatzidis, M G; Even, J; Crochet, J J; Mohite, A D

    2017-03-24

    Understanding and controlling charge and energy flow in state-of-the-art semiconductor quantum wells has enabled high-efficiency optoelectronic devices. Two-dimensional (2D) Ruddlesden-Popper perovskites are solution-processed quantum wells wherein the band gap can be tuned by varying the perovskite-layer thickness, which modulates the effective electron-hole confinement. We report that, counterintuitive to classical quantum-confined systems where photogenerated electrons and holes are strongly bound by Coulomb interactions or excitons, the photophysics of thin films made of Ruddlesden-Popper perovskites with a thickness exceeding two perovskite-crystal units (>1.3 nanometers) is dominated by lower-energy states associated with the local intrinsic electronic structure of the edges of the perovskite layers. These states provide a direct pathway for dissociating excitons into longer-lived free carriers that substantially improve the performance of optoelectronic devices. Copyright © 2017, American Association for the Advancement of Science.

  6. Exciton effects in the index of refraction of multiple quantum wells and superlattices

    NASA Technical Reports Server (NTRS)

    Kahen, K. B.; Leburton, J. P.

    1986-01-01

    Theoretical calculations of the index of refraction of multiple quantum wells and superlattices are presented. The model incorporates both the bound and continuum exciton contributions for the gamma region transitions. In addition, the electronic band structure model has both superlattice and bulk alloy properties. The results indicate that large light-hole masses, i.e., of about 0.23, produced by band mixing effects, are required to account for the experimental data. Furthermore, it is shown that superlattice effects rapidly decrease for energies greater than the confining potential barriers. Overall, the theoretical results are in very good agreement with the experimental data and show the importance of including exciton effects in the index of refraction.

  7. High-temperature superfluidity with indirect excitons in van der Waals heterostructures.

    PubMed

    Fogler, M M; Butov, L V; Novoselov, K S

    2014-07-28

    All known superfluid and superconducting states of condensed matter are enabled by composite bosons (atoms, molecules and Cooper pairs) made of an even number of fermions. Temperatures where such macroscopic quantum phenomena occur are limited by the lesser of the binding energy and the degeneracy temperature of the bosons. High-critical temperature cuprate superconductors set the present record of ~100 K. Here we propose a design for artificially structured materials to rival this record. The main elements of the structure are two monolayers of a transition metal dichalcogenide separated by an atomically thin spacer. Electrons and holes generated in the system would accumulate in the opposite monolayers and form bosonic bound states--the indirect excitons. The resultant degenerate Bose gas of indirect excitons would exhibit macroscopic occupation of a quantum state and vanishing viscosity at high temperatures.

  8. High-temperature superfluidity with indirect excitons in van der Waals heterostructures

    NASA Astrophysics Data System (ADS)

    Fogler, M. M.; Butov, L. V.; Novoselov, K. S.

    2014-07-01

    All known superfluid and superconducting states of condensed matter are enabled by composite bosons (atoms, molecules and Cooper pairs) made of an even number of fermions. Temperatures where such macroscopic quantum phenomena occur are limited by the lesser of the binding energy and the degeneracy temperature of the bosons. High-critical temperature cuprate superconductors set the present record of ~100 K. Here we propose a design for artificially structured materials to rival this record. The main elements of the structure are two monolayers of a transition metal dichalcogenide separated by an atomically thin spacer. Electrons and holes generated in the system would accumulate in the opposite monolayers and form bosonic bound states—the indirect excitons. The resultant degenerate Bose gas of indirect excitons would exhibit macroscopic occupation of a quantum state and vanishing viscosity at high temperatures.

  9. Temperature Evolution of Excitonic Absorptions in Cd(1-x)Zn(x)Te Materials

    NASA Technical Reports Server (NTRS)

    Quijada, Manuel A.; Henry, Ross

    2007-01-01

    The studies consist of measuring the frequency dependent transmittance (T) and reflectance (R) above and below the optical band-gap in the UV/Visible and infrared frequency ranges for Cd(l-x),Zn(x),Te materials for x=0 and x=0.04. Measurements were also done in the temperature range from 5 to 300 K. The results show that the optical gap near 1.49 eV at 300 K increases to 1.62 eV at 5 K. Finally, we observe sharp absorption peaks near this gap energy at low temperatures. The close proximity of these peaks to the optical transition threshold suggests that they originate from the creation of bound electron-hole pairs or excitons. The decay of these excitonic absorptions may contribute to a photoluminescence and transient background response of these back-illuminated HgCdTe CCD detectors.

  10. Free-exciton states in crystalline GaTe

    NASA Astrophysics Data System (ADS)

    Wan, J. Z.; Brebner, J. L.; Leonelli, R.

    1995-12-01

    Polarized properties of both the singlet and triplet ground exciton states in the photoluminescence and transmission spectra of crystalline GaTe are explained based on the possible symmetry properties of the energy band edge of GaTe. Some experimental results about excited exciton states in GaTe are presented and discussed. The energy positions of exciton series in GaTe follow the three-dimensional direct allowed Wannier exciton formula just as in the the other III-VI layered compounds of GaSe and InSe. The nonthermalized, ``hot'' nature of excitons inside GaTe under higher optical excitation intensities is also discussed.

  11. Exciton dynamics in a single layer MoS2

    NASA Astrophysics Data System (ADS)

    Kim, Jonghwan; Hong, Xiaoping; Shi, Sufei; Jin, Chenhao; Sun, Yinghui; Wang, Feng

    2014-03-01

    In a low dimensional semiconductor, exciton plays a crucial role in the optical property. Recently, a single layer of MoS2 has attracted significant attention due to its unique excitonic features. For example, exciton in MoS2 is predicted to have order of magnitude larger binding energy than conventional direct band gap material. For deeper understanding on such properties, however, it is important to understand how exciton is formed and decays in time domain. Our work on exciton dynamics in MoS2 by pump probe spectroscopy will be presented with control of both power and wavelength.

  12. Exciton-plasmaritons in graphene/semiconductor structures

    NASA Astrophysics Data System (ADS)

    Velizhanin, Kirill A.; Shahbazyan, Tigran V.

    2014-08-01

    We study strong coupling between plasmons in monolayer charge-doped graphene and excitons in a narrow gap semiconductor quantum well separated from graphene by a potential barrier. We show that the Coulomb interaction between excitons and plasmons results in mixed states described by a Hamiltonian similar to that for exciton-polaritons and derive the exciton-plasmon coupling constant that depends on system parameters. We calculate numerically the Rabi splitting of exciton-plasmariton dispersion branches for several semiconductor materials and find that it can reach values of up to 50-100 meV.

  13. Strong exciton-plasmon coupling in graphene-semiconductor structures

    NASA Astrophysics Data System (ADS)

    Velizhanin, Kirill A.; Shahbazyan, Tigran V.

    2014-09-01

    We study strong coupling between plasmons in monolayer charge-doped graphene and excitons in a narrow gap semiconductor quantum well separated from graphene by a potential barrier. We show that the Coulomb interaction between excitons and plasmons result in mixed states described by a Hamiltonian similar to that for exciton-polaritons and derive the exciton-plasmon coupling constant that depends on system parameters. We calculate numerically the Rabi splitting of exciton-plasmariton dispersion branches for several semiconductor materials and find that it can reach values of up to 50 - 100 meV.

  14. Strong exciton-plasmon coupling in graphene-semiconductor structures

    NASA Astrophysics Data System (ADS)

    Shahbazyan, Tigran V.; Velizhanin, Kirill A.

    2015-03-01

    We study strong coupling between plasmons in monolayer doped graphene and excitons in narrow gap semiconductor quantum well separated from graphene by a potential barrier. We show that Coulomb interactions between excitons and plasmons result in mixed states described by Hamiltonian similar to one describing exciton-polaritons and derive the exciton-plasmon coupling parameter that depends on system geometry and material properties. We calculate numerically the Rabi splitting of exciton-plasmariton dispersion branches for several semiconductor materials and find that it can reach 100 meV for small graphene and quantum well separations.

  15. Engineering excitonic dynamics and environmental stability of post-transition metal chalcogenides by pyridine functionalization technique

    NASA Astrophysics Data System (ADS)

    Meng, Xiuqing; Pant, Anupum; Cai, Hui; Kang, Jun; Sahin, Hasan; Chen, Bin; Wu, Kedi; Yang, Sijie; Suslu, Aslihan; Peeters, F. M.; Tongay, Sefaattin

    2015-10-01

    Owing to their strong photon emission, low excitonic binding energies, and nearly-ideal band offset values for water splitting reactions, direct gap quasi-2D gallium chalcogenides are potential candidates for applications in energy harvesting, optoelectronics, and photonics. Unlike other 2D materials systems, chemical functionalization of gallium chalcogenides is still at its seminal stages. Here, we propose vapor phase pyridine intercalation technique to manipulate optical properties of gallium chalcogenides. After functionalization, the excitonic dynamics of quasi-2D GaSe change significantly as evidenced by an increase in integrated PL intensity and emergence of a new emission feature that is below the band edge. Based on our DFT calculations, we attribute these to formation of bound exciton complexes at the trap sites introduced by chemical reaction between pyridine and GaSe. On the contrary, pyridine functionalization does not impact the optical properties of GaTe, instead treats GaTe surface to prevent oxidization of tellurium atoms. Overall, results suggest novel ways to control properties of gallium chalcogenides on demand and unleash their full potential for a range of applications in photonics and optoelectronics.Owing to their strong photon emission, low excitonic binding energies, and nearly-ideal band offset values for water splitting reactions, direct gap quasi-2D gallium chalcogenides are potential candidates for applications in energy harvesting, optoelectronics, and photonics. Unlike other 2D materials systems, chemical functionalization of gallium chalcogenides is still at its seminal stages. Here, we propose vapor phase pyridine intercalation technique to manipulate optical properties of gallium chalcogenides. After functionalization, the excitonic dynamics of quasi-2D GaSe change significantly as evidenced by an increase in integrated PL intensity and emergence of a new emission feature that is below the band edge. Based on our DFT calculations

  16. CCD Luminescence Camera

    NASA Technical Reports Server (NTRS)

    Janesick, James R.; Elliott, Tom

    1987-01-01

    New diagnostic tool used to understand performance and failures of microelectronic devices. Microscope integrated to low-noise charge-coupled-device (CCD) camera to produce new instrument for analyzing performance and failures of microelectronics devices that emit infrared light during operation. CCD camera also used to indentify very clearly parts that have failed where luminescence typically found.

  17. Advanced synchronous luminescence system

    DOEpatents

    Vo-Dinh, T.

    1997-02-04

    A method and apparatus are disclosed for determining the condition of tissue or otherwise making chemical identifications includes exposing the sample to a light source, and using a synchronous luminescence system to produce a spectrum that can be analyzed for tissue condition. 14 figs.

  18. Free and trapped hybrid charge transfer excitons at a ZnO/small-molecule heterojunction

    NASA Astrophysics Data System (ADS)

    Panda, Anurag; Ding, Kan; Liu, Xiao; Forrest, Stephen R.

    2016-09-01

    We study the temperature-dependent electrical and optical properties of hybrid charge transfer excitons (HCTEs) at a ZnO/4,4'-bis(N-carbazolyl)-1,1'-biphenyl (CBP) organic/inorganic semiconductor heterojunction (OI-HJ). The electroluminescence spectrum of the HCTE formed by recombination of injected charge undergoes a hypsochromic shift from 1.65 ± 0.01 eV to 2.05 ± 0.01 eV with decreasing temperature from T =300 K to 30 K at a current density of J =100 mA c m-2 , and with increasing voltage from V =1.5 V to 4.5 V. We observe an external quantum efficiency of 6.0 ± 0.2% at a wavelength of 332 nm for excitons generated in CBP, indicating exciton to charge conversion via HCTEs. However, no HCTE photoluminescence is observed at temperatures as low as T =25 K . A quantum mechanical model based on the coexistence of both free and trapped singlet HCTE states at the OI-HJ describes these observations. The free HCTE consists of a hole in CPB Coulombically bound with an energy of 9 meV to a delocalized electron in ZnO, and it is the precursor to photocurrent generation via CBP Frenkel excitons. The observed electroluminescence is due to electron injection into localized defect states at the ZnO surface that are bound to holes in CBP forming a trapped HCTE with binding energies of 60-430 meV and oscillator strength that is four orders of magnitude higher compared to the free HCTE.

  19. Multiple exciton generation in colloidal silicon nanocrystals.

    PubMed

    Beard, Matthew C; Knutsen, Kelly P; Yu, Pingrong; Luther, Joseph M; Song, Qing; Metzger, Wyatt K; Ellingson, Randy J; Nozik, Arthur J

    2007-08-01

    Multiple exciton generation (MEG) is a process whereby multiple electron-hole pairs, or excitons, are produced upon absorption of a single photon in semiconductor nanocrystals (NCs) and represents a promising route to increased solar conversion efficiencies in single-junction photovoltaic cells. We report for the first time MEG yields in colloidal Si NCs using ultrafast transient absorption spectroscopy. We find the threshold photon energy for MEG in 9.5 nm diameter Si NCs (effective band gap identical with Eg = 1.20 eV) to be 2.4 +/- 0.1Eg and find an exciton-production quantum yield of 2.6 +/- 0.2 excitons per absorbed photon at 3.4Eg. While MEG has been previously reported in direct-gap semiconductor NCs of PbSe, PbS, PbTe, CdSe, and InAs, this represents the first report of MEG within indirect-gap semiconductor NCs. Furthermore, MEG is found in relatively large Si NCs (diameter equal to about twice the Bohr radius) such that the confinement energy is not large enough to produce a large blue-shift of the band gap (only 80 meV), but the Coulomb interaction is sufficiently enhanced to produce efficient MEG. Our findings are of particular importance because Si dominates the photovoltaic solar cell industry, presents no problems regarding abundance and accessibility within the Earth's crust, and poses no significant environmental problems regarding toxicity.

  20. electric dipole superconductor in bilayer exciton system

    NASA Astrophysics Data System (ADS)

    Sun, Qing-Feng; Jiang, Qing-Dong; Bao, Zhi-Qiang; Xie, X. C.

    Recently, it was reported that the bilayer exciton systems could exhibit many new phenomena, including the large bilayer counterflow conductivity, the Coulomb drag, etc. These phenomena imply the formation of exciton condensate superfluid state. On the other hand, it is now well known that the superconductor is the condensate superfluid state of the Cooper pairs, which can be viewed as electric monopoles. In other words, the superconductor state is the electric monopole condensate superfluid state. Thus, one may wonder whether there exists electric dipole superfluid state. In this talk, we point out that the exciton in a bilayer system can be considered as a charge neutral electric dipole. And we derive the London-type and Ginzburg-Landau-type equations of electric dipole superconductivity. From these equations, we discover the Meissner-type effect (against spatial variation of magnetic fields), and the dipole current Josephson effect. The frequency in the AC Josephson effect of the dipole current is equal to that in the normal (monopole) superconductor. These results can provide direct evidence for the formation of exciton superfluid state in the bilayer systems and pave new ways to obtain the electric dipole current. We gratefully acknowledge the financial support by NBRP of China (2012CB921303 and 2015CB921102) and NSF-China under Grants Nos. 11274364 and 11574007.

  1. (Gene sequencing by scanning molecular exciton microscopy)

    SciTech Connect

    Not Available

    1991-01-01

    This report details progress made in setting up a laboratory for optical microscopy of genes. The apparatus including a fluorescence microscope, a scanning optical microscope, various spectrometers, and supporting computers is described. Results in developing photon and exciton tips, and in preparing samples are presented. (GHH)

  2. Conjugated “Molecular Wire” for Excitons

    SciTech Connect

    Shibano, Y.; Miller, J.; Imahori, H.; Sreearunothai, P.; Cook, A.R.

    2010-05-06

    We have synthesized new conjugated, rigid rod oligomers of fluorene, F{sub n}(C{sub 60}){sub 2}, n = 4, 8, 12, and 16. These pure compounds have F{sub n} chains up to 140 {angstrom} long. The C{sub 60} groups covalently attached at both ends serve as traps for excitons created in the F{sub n} chains. Excitons created in the chains by photoexcitation reacted rapidly with the C{sub 60} groups with decays described well by the sum of two exponentials. Mean reaction times were 2.3, 5.5, and 10.4 ps for n = 8, 12, and 16. In F{sub 16}(C{sub 60}){sub 2}, the 10.4 ps reaction time was 40 times faster than that found in earlier reports on molecules of slightly longer length. The simplest possible model, that of one-dimensional diffusion of excitonic polarons that react whenever they encounter the end of a chain, fits the results to obtain diffusion coefficients. Deviations of those fits from the data may point to the need for alternative pictures or may just indicate that diffusion is not ideal. The definite lengths of these molecules enable a stringent test for theories. These results reveal that exciton transport can be much faster than previously believed, a finding that could, along with appropriate nanoassembly, enable new kinds of high-efficiency organic photovoltaics.

  3. Coupled exciton-photon Bose condensate in path integral formalism

    NASA Astrophysics Data System (ADS)

    Elistratov, A. A.; Lozovik, Yu. E.

    2016-03-01

    We study the behavior of exciton polaritons in an optical microcavity with an embedded semiconductor quantum well. We use a two-component exciton-photon approach formulated in terms of path integral formalism. In order to describe spatial distributions of the exciton and photon condensate densities, the two coupled equations of the Gross-Pitaevskii type are derived. For a homogeneous system, we find the noncondensate photon and exciton spectra, calculate the coefficients of transformation from the exciton-photon basis to the lower-upper polariton basis, and obtain the exciton and photon occupation numbers of the lower and upper polariton branches for nonzero temperatures. For an inhomogeneous system, the set of coupled equations of the Bogoliubov-de Gennes type is derived. The equations govern the spectra and spatial distributions of noncondensate photons and excitons.

  4. Luminescence sensitization of Tb(3+)-DNA complexes by Ag().

    PubMed

    Xu, Lijun; Zhou, Lu; Chen, Xing; Shen, Xiaoqiang; Wang, Jine; Zhang, Jianye; Pei, Renjun

    2017-03-03

    Terbium ions (Tb(3+)) with unique photophysical properties have been utilized to develop biosensors with low background and high sensitivity. In this study, the Ag(+)-sensitized luminescence of Tb(3+)-DNA complexes was uncovered. The luminescence of Tb(3+)-DNA complexes could be enhanced by more than 30 times in the presence of Ag(+), when Tb(3+) was bound with poly(G) and poly(T) whereas not with other homopolymers. This research confirmed that the sensitization resulted from the interaction of Ag(+) with certain bases involved in DNA, not just with the reported certain G-quadruplex sequence. The coordination of Ag(+) to guanine and thymine bases was expected to increase their rigidities, form Tb(3+)-DNA-Ag(+) ternary structures, and thus enhance energy transfer from guanine and thymine to Tb(3+). These findings benefit the development of sensitive luminescence probes for various nucleic acids-related targets.

  5. Luminescence sensitization of Tb3 +-DNA complexes by Ag+

    NASA Astrophysics Data System (ADS)

    Xu, Lijun; Zhou, Lu; Chen, Xing; Shen, Xiaoqiang; Wang, Jine; Zhang, Jianye; Pei, Renjun

    2017-06-01

    Terbium ions (Tb3 +) with unique photophysical properties have been utilized to develop biosensors with low background and high sensitivity. In this study, the Ag+-sensitized luminescence of Tb3 +-DNA complexes was uncovered. The luminescence of Tb3 +-DNA complexes could be enhanced by more than 30 times in the presence of Ag+, when Tb3 + was bound with poly(G) and poly(T) whereas not with other homopolymers. This research confirmed that the sensitization resulted from the interaction of Ag+ with certain bases involved in DNA, not just with the reported certain G-quadruplex sequence. The coordination of Ag+ to guanine and thymine bases was expected to increase their rigidities, form Tb3 +-DNA-Ag+ ternary structures, and thus enhance energy transfer from guanine and thymine to Tb3 +. These findings benefit the development of sensitive luminescence probes for various nucleic acids-related targets.

  6. Characterization of Macroscopic Ordering in Exciton Rings

    NASA Astrophysics Data System (ADS)

    Yang, Sen; Levitov, L. S.; Simons, B. D.; Gossard, A. C.

    2005-03-01

    Recently observed complex PL patterns in 2D QW structures exhibit the inner [1,3] and the outer [1-4] exciton rings, localized bright spots [1,3], and the macroscopically ordered exciton state (MOES) [1,3]. The latter appears at the outer ring via its fragmentation into a periodic array of aggregates. While the gross features have been explained within classical framework, attributing the inner rings to nonradiative exciton transport and cooling [1], and the outermost rings and the bright spots to macroscopic charge separation [3,4], the origin of the MOES remains unidentified [5]. Here, for the first time, we report experiments demonstrating the exciton energy modulation over the MOES as well as the phase diagram of MOES in exciton density and temperature coordinates. The experiments shed new light on the dynamical origin of MOES. Besides, we present the studies of dynamical processes within MOES including the observation of aggregate instabilities and bifurcations that point to the spontaneous character of the instability.[1] L.V. Butov, A.C. Gossard, D.S. Chemla, Nature 418, 751 (2002). [2] D. Snoke, S. Denev, Y. Liu, L. Pfeiffer, K. West, Nature 418, 754 (2002). [3] L.V. Butov, L.S. Levitov, A.V. Mintsev, B.D. Simons, A.C. Gossard, D.S. Chemla PRL 92, 117404 (2004). [4] R. Rapaport, G. Chen, D. Snoke, S.H. Simon, L. Pfeiffer, K. West, Y. Liu, S. Denev PRL 92, 117405 (2004). [5] L.S. Levitov, B.D. Simons, L.V. Butov, cond-mat/0403377.

  7. Dynamics of exciton transfer in coupled polymer chains

    NASA Astrophysics Data System (ADS)

    Zhang, Y. L.; Liu, X. J.; Sun, Z.; An, Z.

    2013-05-01

    The dynamics of singlet and triplet exciton transfer in coupled polymer chains are investigated within the Su-Schrieffer-Heeger+Pariser-Parr-Pople model including both electron-phonon (e-p) coupling and electron-electron (e-e) interactions, using a multi-configurational time-dependent Hartree-Fock dynamic method. In order to explain the processes involved, the effects of on-site and long-range e-e interactions on the locality of the singlet and triplet excitons are first investigated on an isolated chain. It is found that the locality of the singlet exciton decreases, while the locality of the triplet exciton increases with an increase in the on-site e-e interactions. On the other hand, an increase in the long-range e-e interaction results in a more localized singlet exciton and triplet exciton. In coupled polymer chains, we then quantitatively show the yields of singlet and triplet exciton transfer products under the same interchain coupling. It is found that the yield of singlet interchain excitons is much higher than that of triplet interchain excitons, that is to say, singlet exciton transfer is significantly easier than that for triplet excitons. This results from the fact that the singlet exciton is more delocalized than the triplet exciton. In addition, hopping of electrons with opposite spins between the coupled chains can facilitate the transfer of singlet excitons. The results are of great significance for understanding the photoelectric conversion process and developing high-power organic optoelectronic applications.

  8. LETTER TO THE EDITOR: Quantum chemical modelling of electron polarons and excitons in ABO3 perovskites

    NASA Astrophysics Data System (ADS)

    Kotomin, E. A.; Eglitis, R. I.; Borstel, G.

    2000-09-01

    Quantum chemical calculations using the intermediate neglect of the differential overlap (INDO) method, combined with the large unit cell periodic model argue for an existence of the self-trapped electrons in KNbO3 and KTaO3 perovskite crystals. An electron in the ground state occupies predominantly t2g orbital of a Nb4+ ion. Its orbital degeneracy is lifted by a combination of the breathing and Jahn-Teller modes where four nearest equatorial O atoms are displaced outwards and two oxygens shift inwards along the z axis. Triplet exciton is shown to be in a good approximation of a pair of nearest Jahn-Teller electron and hole polarons (a bipolaron) which is very likely responsible for the `green' luminescence observed in these crystals.

  9. Highly sensitive nonlinear luminescent ceramics for volumetric and multilayer data carriers

    SciTech Connect

    Martynovich, E F; Dresvyanskiy, V P; Voitovich, A P; Bagayev, S N

    2015-10-31

    The interaction of optical ceramics based on wide-bandgap crystals with near-IR femtosecond laser radiation is studied experimentally. The formation of luminescent centres in LiF and MgF{sub 2} ceramics under the action of single laser pulses is considered. Two interaction regimes are used. In the regime of low-aperture focusing of laser radiation (800 nm, 30 fs, 0.3 mJ), multiple selffocusing and filamentation in the samples are observed. The luminescent centres are formed in thin channels induced by light filaments. The average effective self-focusing length is ∼100 μm; the formation of luminescent centres begins at this length and ceases at a wavelength of about 380 mm. The luminescent trace (spur) induced by a single laser filament was ∼30 μm long and 1.3 μm in diameter. The second regime of light interaction with the sample was based on high-aperture focusing with a simultaneous decrease in the laser pulse energy. This led to the formation of single pits with a diameter smaller than the optical diffraction limit. The luminescent centres induced by the laser radiation were aggregated colour centres. The mechanism of their creation included the highly-nonlinear generation of electron – hole pairs in the filamentation region, their recombination with the formation of anion excitons and the decay of excitons into Fresnel defects by the Lushchik – Vitol – Hersh – Pooley mechanism, as well as their recharging, migration and aggregation. (laser applications and other topics in quantum electronics)

  10. Luminescence of La0.2Y1.8O3 nanostructured scintillators.

    PubMed

    Chen, Wei; Tu, Haiqing; Sahi, Sunil; Mao, Defeng; Kenarangui, Rasool; Luo, Junming; Jin, Peng; Liu, Shuman; Ma, Lun; Brandt, Andrew; Weiss, Alex

    2014-10-01

    For the first time, transparent La0.2Y1.8O3 nanostructured polycrystalline scintillators were fabricated by sintering nanoparticle powders at high temperatures and their scintillation properties are reported. La0.2Y1.8O3 is a host material that has never been investigated as scintillators for radiation detection. Our observations found that La0.2Y1.8O3 has an intense scintillation luminescence, a detection efficiency higher than that of YAG:Ce and a comparable energy resolution to NaI and CsI scintillators. In addition, La0.2Y1.8O3 is stable and has luminescence decay lifetime in the picosecond range which is favorable for radiation detection. The luminescence of La0.2Y1.8O3 has a large Stokes-shift and a large emission bandwidth, and the luminescence is highly temperature dependent. Different from most doped scintillators, the luminescence of La0.2Y1.8O3 is most likely from the self-trapped excitons. The discovery of La0.2Y1.8O3 scintillators opens a new door for the research of new materials for radiation detection.

  11. Synthesis and luminescence of silicon remnants formed by truncated glassmelt-particle reaction

    NASA Astrophysics Data System (ADS)

    Risbud, Subhash H.; Liu, Li-Chi; Shackelford, James F.

    1993-09-01

    We have obtained nanometer sized silicon remnants sequestered in glass matrices by terminating the reaction of pure silicon powders dispersed in the viscous melt at a temperature of 1400 °C. Repeated use of this truncated melt-particle reaction process dilutes the amount and size of silicon remnants, and bulk samples containing nanosize silicon crystallites embedded in a glass matrix were eventually obtained. These quantum dot sized silicon-in-glass materials emit greenish luminescence with peak wavelengths from ≊480 to 530 nm, considerably shorter than the reddish luminescence (at about 700-850 nm) observed in porous silicon structures prepared by electrochemical etching techniques; upon complete digestion of Si particles by the melt, the luminescence peaks disappear. Since our silicon-in-glass preparation method does not involve etching, the origin of the luminescence is not likely to be due to Si-O-H compounds (e.g., siloxene) postulated recently. The location of the luminescence peaks and the observed silicon crystallite size suggest quantum confinement leading to a widened silicon band gap arising from remnants in the glass matrix smaller than the exciton diameter of bulk silicon (10 nm).

  12. Phonon induced luminescence decay in monolayer MoS2 on SiO2/Si substrates

    NASA Astrophysics Data System (ADS)

    Saigal, Nihit; Ghosh, Sandip

    2015-12-01

    Exfoliated monolayer MoS2 films on SiO2/Si substrates have been studied using photoluminescence (PL), Raman and reflectance contrast (RC) spectroscopies. With increase in temperature, the intensity of the two dominant PL spectral features A and D, attributed to A exciton/trion and to defects, seemingly decay in an activated fashion with an energy ˜ 50 meV , which is close to the energies of E2 g 1 and A1g phonons. Comparison of absorption spectrum derived from RC with circular polarization resolved PL spectrum suggests that both D and A emissions are associated with bound excitons, the A emission involving relatively weakly localized ones. The PL decay behaviour is explained using a phenomenological model where non-radiative loss of excitons is determined by the number of excited phonon modes. This corroborates the recent finding of strong A exciton and A1g phonon coupling in monolayer MoS2.

  13. Exciton polaritons in two-dimensional dichalcogenide layers placed in a planar microcavity: Tunable interaction between two Bose-Einstein condensates

    NASA Astrophysics Data System (ADS)

    Vasilevskiy, Mikhail I.; Santiago-Pérez, Darío G.; Trallero-Giner, Carlos; Peres, Nuno M. R.; Kavokin, Alexey

    2015-12-01

    Exciton-polariton modes arising from interaction between bound excitons in monolayer thin semiconductor sheets and photons in a Fabry-Perot microcavity are considered theoretically. We calculate the dispersion curves, mode lifetimes, Rabi splitting, and Hopfield coefficients of these structures for two nearly 2D semiconductor materials, MoS2 and WS2, and suggest that they are interesting for studying the rich physics associated with the Bose-Einstein condensation of exciton polaritons. The large exciton binding energy and dipole allowed exciton transitions, in addition to the relatively easily controllable distance between the semiconductor sheets, are the advantages of this system in comparison with traditional GaAs or CdTe based semiconductor microcavities. In particular, in order to mimic the rich physical properties of the quantum degenerate mixture of two bosonic species of dilute atomic gases with tunable interspecies interaction, we put forward a structure containing two semiconductor sheets separated by some atomic-scale distance (l ) using a nearly 2D dielectric (e.g., h-BN), which offers the possibility of tuning the interaction between two exciton-polariton Bose-Enstein condensates. We show that the dynamics of this structure are ruled by two coupled Gross-Pitaevskii equations with the coupling parameter ˜l-1 .

  14. Observation of hybrid Tamm-plasmon exciton- polaritons with GaAs quantum wells and a MoSe2 monolayer.

    PubMed

    Wurdack, Matthias; Lundt, Nils; Klaas, Martin; Baumann, Vasilij; Kavokin, Alexey V; Höfling, Sven; Schneider, Christian

    2017-08-15

    Strong light matter coupling between excitons and microcavity photons, as described in the framework of cavity quantum electrodynamics, leads to the hybridization of light and matter excitations. The regime of collective strong coupling arises, when various excitations from different host media are strongly coupled to the same optical resonance. This leads to a well-controllable admixture of various matter components in three hybrid polariton modes. Here, we study a cavity device with four embedded GaAs quantum wells hosting excitons that are spectrally matched to the A-valley exciton resonance of a MoSe2 monolayer. The formation of hybrid polariton modes is evidenced in momentum resolved photoluminescence and reflectivity studies. We describe the energy and k-vector distribution of exciton-polaritons along the hybrid modes by a thermodynamic model, which yields a very good agreement with the experiment.Light and matter excitations from host media can hybridize in the strong coupling regime, resulting in the formation of hybrid polariton modes. Here, the authors demonstrate hybridization between tightly bound excitons in a MoSe2 monolayer and excitons in GaAs quantum wells via coupling to a cavity resonance.

  15. Anomalous excitons and screenings unveiling strong electronic correlations in SrTi1 -xNbxO3 (0 ≤x ≤0.005 )

    NASA Astrophysics Data System (ADS)

    Gogoi, Pranjal Kumar; Sponza, Lorenzo; Schmidt, Daniel; Asmara, Teguh Citra; Diao, Caozheng; Lim, Jason C. W.; Poh, Sock Mui; Kimura, Shin-ichi; Trevisanutto, Paolo E.; Olevano, Valerio; Rusydi, Andrivo

    2015-07-01

    Electron-electron (e-e) and electron-hole (e-h) interactions are often associated with many exotic phenomena in correlated electron systems. Here, we report an observation of anomalous excitons at 3.75, 4.67, and 6.11 eV at 4.2 K in bulk SrTiO3. Fully supported by ab initio G W Bethe-Salpeter equation calculations, these excitons are due to strong e-h and e-e interactions with different characters: 4.67 and 6.11 eV are resonant excitons and 3.75 eV is a bound Wannier-like exciton with an unexpectedly higher level of delocalization. Measurements and calculations on SrTi1 -xNbxO3 for 0.0001 ≤x ≤0.005 further show that the energy and spectral-weight of the excitonic peaks vary as a function of electron doping (x ) and temperature, which are attributed to screening effects. Our results show the importance of e-h and e-e interactions yielding to anomalous excitons and thus bring out a new fundamental perspective in SrTiO3.

  16. Zero-reabsorption doped-nanocrystal luminescent solar concentrators.

    PubMed

    Erickson, Christian S; Bradshaw, Liam R; McDowall, Stephen; Gilbertson, John D; Gamelin, Daniel R; Patrick, David L

    2014-04-22

    Optical concentration can lower the cost of solar energy conversion by reducing photovoltaic cell area and increasing photovoltaic efficiency. Luminescent solar concentrators offer an attractive approach to combined spectral and spatial concentration of both specular and diffuse light without tracking, but they have been plagued by luminophore self-absorption losses when employed on practical size scales. Here, we introduce doped semiconductor nanocrystals as a new class of phosphors for use in luminescent solar concentrators. In proof-of-concept experiments, visibly transparent, ultraviolet-selective luminescent solar concentrators have been prepared using colloidal Mn(2+)-doped ZnSe nanocrystals that show no luminescence reabsorption. Optical quantum efficiencies of 37% are measured, yielding a maximum projected energy concentration of ∼6× and flux gain for a-Si photovoltaics of 15.6 in the large-area limit, for the first time bounded not by luminophore self-absorption but by the transparency of the waveguide itself. Future directions in the use of colloidal doped nanocrystals as robust, processable spectrum-shifting phosphors for luminescent solar concentration on the large scales required for practical application of this technology are discussed.

  17. Plasmonic control of near-interface exciton dynamics in defect-rich ZnO thin films

    SciTech Connect

    Lawrie, Benjamin J; Mu, Richard; HaglundJr., Richard F

    2012-01-01

    ZnO is an attractive material for many electro-optical applications, but the control of impurities remains an issue in device fabrication. For this paper, the dynamics of defect states produced by annealing ZnO thin-films at temperatures of 400-800C were probed by band-edge pump probe spectroscopy in differential reflection and transmission. The distinction between the differential reflection and transmission spectra allowed for the analysis of ultrafast near-interface dynamics, which cannot be separated from the bulk thin film dynamics by traditional ultrafast spectroscopies. In particular, simulataneous differential reflection and transmission spectroscopy provided clear evidence that the band-edge recombination dynamics in samples annealed at 400C were absent near the ZnO/substrate interface. However, the Purcell enhancement observed in Ag/ZnO heterostructures resulted in the dramatic emergence of the band-edge recombination signal where none was previously observable due to the dominant defect luminescence. Plasmon-exciton coupling enhances band-edge exciton recombination by nearly two orders of magnitude over the defect luminescence. This indicates that the spatial range of the Purcell effect is at least twice as large as inferred from photoluminescence studies.

  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. Fine structure of the exciton electroabsorption in semiconductor superlattices

    NASA Astrophysics Data System (ADS)

    Monozon, B. S.; Schmelcher, P.

    2017-02-01

    Wannier-Mott excitons in a semiconductor layered superlattice (SL) are investigated analytically for the case that the period of the superlattice is much smaller than the 2D exciton Bohr radius. Additionally we assume the presence of a longitudinal external static electric field directed parallel to the SL axis. The exciton states and the optical absorption coefficient are derived in the tight-binding and adiabatic approximations. Strong and weak electric fields providing spatially localized and extended electron and hole states, respectively, are studied. The dependencies of the exciton states and the exciton absorption spectrum on the SL parameters and the electric field strength are presented in an explicit form. We focus on the fine structure of the ground quasi-2D exciton level formed by the series of closely spaced energy levels adjacent from the high frequencies. These levels are related to the adiabatically slow relative exciton longitudinal motion governed by the potential formed by the in-plane exciton state. It is shown that the external electric fields compress the fine structure energy levels, decrease the intensities of the corresponding optical peaks and increase the exciton binding energy. A possible experimental study of the fine structure of the exciton electroabsorption is discussed.

  20. Taming excitons in II-VI semiconductor nanowires and nanobelts

    NASA Astrophysics Data System (ADS)

    Xu, Xinlong; Zhang, Qing; Zhang, Jun; Zhou, Yixuan; Xiong, Qihua

    2014-10-01

    Excitons are one of the most important fundamental quasi-particles, and are involved in a variety of processes forming the basis of a wide range of opto-electronic and photonic devices based on II-VI semiconductor nanowires and nanobelts, such as light-emitting diodes, photovoltaic cells, photodetectors and nanolasers. A clear understanding of their properties and unveiling the potential engineering for excitons is of particular importance for the design and optimization of nanoscale opto-electronic and photonic devices. Herein, we present a comprehensive review on discussing the fundamental behaviours of the excitons in one-dimensional (1D) II-VI semiconductor nanomaterials (nanowires and nanobelts). We will start with a focus on the unique properties (origin, generation, etc) and dynamics of excitons and exciton complexes in the II-VI semiconductor nanowires and nanobelts. Then we move to the recent progress on the excitonic response in 1D nanomaterials and focus on the tailoring and engineering of excitonic properties through rational controlling of the physical parameters and conditions, intrinsically and extrinsically. These include (1) exciton-exciton interaction, which is important for 1D nanomaterial nanolasing; (2) exciton-phonon interaction, which has interesting applications for laser cooling; and (3) exciton-plasmon interaction, which is the cornerstone towards the realization of plasmonic lasers. The potential of electric field, morphology and size control for excitonic properties is also discussed. Unveiling and controlling excitonic properties in II-VI semiconductor nanowires and nanobelts would promote the development of 1D nanoscience and nanotechnology.

  1. Time-resolved spectroscopy of exciton states in single crystals and single crystalline films of YAlO3 and YAlO3 : Ce

    NASA Astrophysics Data System (ADS)

    Babin, V.; Gorbenko, V.; Kondakova, I.; Kärner, T.; Laguta, V. V.; Nikl, M.; Zazubovich, S.; Zorenko, Yu

    2011-08-01

    Luminescence characteristics of single crystals (SC) and single crystalline films (SCF) of YAlO3 and YAlO3 : Ce are studied at 4.2-300 K under photoexcitation in the 4-20 eV energy range. The origin and structure of the intrinsic and impurity defects responsible for various exciton-related emission and excitation bands are identified. The ≈5.6 eV emission of YAlO3 SCF is ascribed to the self-trapped excitons. In YAlO3 SC, the dominating 5.63 eV and 4.12 eV emissions are ascribed to the excitons localized at the isolated antisite defect Y_{Al}^{3+} and at the Y_{Al}^{3+} defect associated with the nearest-neighbouring oxygen vacancy, respectively. The thermally stimulated release of the electrons, trapped at these defects, takes place around 200 K and 280 K, respectively. The presence of Y_{Al}^{3+} -related defects and isolated oxygen vacancies (AlO5 units) in YAlO3 SC is confirmed by NMR measurements. The formation energies of various Y_{Al}^{3+} -related defects are calculated within the density functional theory. The influence of various intrinsic and impurity defects on the luminescence characteristics of Ce3+ centres is clarified.

  2. Dynamics induced by electronic transitions: Finite-temperature relaxation of self-trapped excitons to defects in NaCl

    NASA Astrophysics Data System (ADS)

    Williams, R. T.; Song, K. S.

    2005-11-01

    Molecular dynamics simulations of self-trapped exciton relaxation and associated defect formation in 621-atom NaCl clusters provide a useful framework for discussing hypotheses suggested by the recent experimental results of Tanimura and Hess. Their experiments on subpicosecond absorption spectroscopy of NaCl versus temperature showed that a major part of the temperature-dependent F-H defect formation yield in NaCl occurs within a few picoseconds, a time much shorter than the lifetime of equilibrated self-trapped excitons at the corresponding temperatures. This forces a re-examination of mechanisms for temperature-dependent conversion from self-trapped excitons to defect pairs. Molecular dynamics simulations are able to test some suppositions and display dynamic population of characteristic vibrational modes during the relaxation. The results suggest a hypothesis that a particular low-frequency, odd-parity mode of the halogen molecular ion, which is strongly excited and has a long lifetime in the simulation, is important in the dynamics of fast, temperature-dependent defect formation, in the observed slow cooling of STE luminescence in KI, and in anomalous mobility of the "dynamic H-center" observed by Saidoh, Hoshi, and Itoh. A periodic, coherent attempt on the main barrier to defect formation is assisted by thermal noise, and yields a result in phase with the periodic attempt. This concept is describable in the framework of stochastic resonance.

  3. Quantitative luminescence imaging system

    DOEpatents

    Erwin, D.N.; Kiel, J.L.; Batishko, C.R.; Stahl, K.A.

    1990-08-14

    The QLIS images and quantifies low-level chemiluminescent reactions in an electromagnetic field. It is capable of real time nonperturbing measurement and simultaneous recording of many biochemical and chemical reactions such as luminescent immunoassays or enzyme assays. The system comprises image transfer optics, a low-light level digitizing camera with image intensifying microchannel plates, an image process or, and a control computer. The image transfer optics may be a fiber image guide with a bend, or a microscope, to take the light outside of the RF field. Output of the camera is transformed into a localized rate of cumulative digitalized data or enhanced video display or hard-copy images. The system may be used as a luminescent microdosimetry device for radiofrequency or microwave radiation, as a thermal dosimeter, or in the dosimetry of ultra-sound (sonoluminescence) or ionizing radiation. It provides a near-real-time system capable of measuring the extremely low light levels from luminescent reactions in electromagnetic fields in the areas of chemiluminescence assays and thermal microdosimetry, and is capable of near-real-time imaging of the sample to allow spatial distribution analysis of the reaction. It can be used to instrument three distinctly different irradiation configurations, comprising (1) RF waveguide irradiation of a small Petri-dish-shaped sample cell, (2) RF irradiation of samples in a microscope for the microscopic imaging and measurement, and (3) RF irradiation of small to human body-sized samples in an anechoic chamber. 22 figs.

  4. Microstructural lines involving luminescence

    NASA Astrophysics Data System (ADS)

    Shimada, Kazuhiko

    2004-06-01

    Japanese National Printing Bureau has been focused upon the development of anti-copy lines for many years. The basic concept with regard to security measure lies in the merge of art and technology. On this basis, our originally developed anti-copy lines show flexibility to various security designs. Our newest anti-copy lines comprising from the Tri-Branched and Divided Lines shows clearer latent image effect compared to that of our other developed anti-copy lines. However, the anti-copy effect of security printing lines with microstructure is deteriorating due to the emergence of digital image techniques with higher resolution. In this situation, this paper introduces a new security measure comprising from luminescence and security printing lines with microstructure. It gives rise to a latent image effect under UV light due to the characteristic microstructure while visually same density. The principle advantage is that the combination of the anti-copy and luminescent feature strongly enhances its secure effect in documents. There is no necessity of two kinds of inks and any specially designed equipment to produce security documents with microstructural lines involving luminescence.

  5. Quantitative luminescence imaging system

    DOEpatents

    Erwin, David N.; Kiel, Johnathan L.; Batishko, Charles R.; Stahl, Kurt A.

    1990-01-01

    The QLIS images and quantifies low-level chemiluminescent reactions in an electromagnetic field. It is capable of real time nonperturbing measurement and simultaneous recording of many biochemical and chemical reactions such as luminescent immunoassays or enzyme assays. The system comprises image transfer optics, a low-light level digitizing camera with image intensifying microchannel plates, an image process or, and a control computer. The image transfer optics may be a fiber image guide with a bend, or a microscope, to take the light outside of the RF field. Output of the camera is transformed into a localized rate of cumulative digitalized data or enhanced video display or hard-copy images. The system may be used as a luminescent microdosimetry device for radiofrequency or microwave radiation, as a thermal dosimeter, or in the dosimetry of ultra-sound (sonoluminescence) or ionizing radiation. It provides a near-real-time system capable of measuring the extremely low light levels from luminescent reactions in electromagnetic fields in the areas of chemiluminescence assays and thermal microdosimetry, and is capable of near-real-time imaging of the sample to allow spatial distribution analysis of the reaction. It can be used to instrument three distinctly different irradiation configurations, comprising (1) RF waveguide irradiation of a small Petri-dish-shaped sample cell, (2) RF irradiation of samples in a microscope for the microscopie imaging and measurement, and (3) RF irradiation of small to human body-sized samples in an anechoic chamber.

  6. 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.

  7. Two-dimensional coherent spectroscopy of excitons, biexcitons, and exciton-polaritons

    NASA Astrophysics Data System (ADS)

    Bristow, Alan D.

    2016-10-01

    Semiconductors systems exhibiting excitonic properties are discussed in terms of their coherent response, which is extracted using two-dimensional coherent spectroscopy. This control method allows for separation of quantum pathways that comprise the optical response, such as interactions between excitons, their dephasing rates, the effects of many-body interactions and the role of structure on the microscopic electronic environment. Additional controls, such as polarization can be used to further distinguish biexcitons and suppress many-body interactions. These result are compared and contrasted with those from a semiconductor microcavity where the excitons form polaritonic modes due to normal-mode splitting. Rephrasing spectra map the detuning dependence of the exciton-polariton branches. Increasing the detuning shifts all features to higher energy and the expected anti-crossing is observed. An isolated biexciton is seen only at negative detuning, separated by a binding energy. For positive detuning, the spectral weight of the off-diagonal features swap, as the lower polariton branch and biexciton come into resonance. This indicates that the off-diagonal features are sensitive to the interactions of the exciton-polaritons and other resonances in the system.

  8. An Introduction to Luminescence in Inorganic Solids.

    ERIC Educational Resources Information Center

    DeLuca, John A.

    1980-01-01

    Introduces luminescence by characterizing phosphors, describing phosphor phenomena, presenting a configurational coordinate model of characteristic luminescence, and describing some commercial applications of phosphors. (CS)

  9. An Introduction to Luminescence in Inorganic Solids.

    ERIC Educational Resources Information Center

    DeLuca, John A.

    1980-01-01

    Introduces luminescence by characterizing phosphors, describing phosphor phenomena, presenting a configurational coordinate model of characteristic luminescence, and describing some commercial applications of phosphors. (CS)

  10. Intrachain exciton dynamics in conjugated polymer chains in solution.

    PubMed

    Tozer, Oliver Robert; Barford, William

    2015-08-28

    We investigate exciton dynamics on a polymer chain in solution induced by the Brownian rotational motion of the monomers. Poly(para-phenylene) is chosen as the model system and excitons are modeled via the Frenkel exciton Hamiltonian. The Brownian fluctuations of the torsional modes were modeled via the Langevin equation. The rotation of monomers in polymer chains in solution has a number of important consequences for the excited state properties. First, the dihedral angles assume a thermal equilibrium which causes off-diagonal disorder in the Frenkel Hamiltonian. This disorder Anderson localizes the Frenkel exciton center-of-mass wavefunctions into super-localized local exciton ground states (LEGSs) and higher-energy more delocalized quasi-extended exciton states (QEESs). LEGSs correspond to chromophores on polymer chains. The second consequence of rotations-that are low-frequency-is that their coupling to the exciton wavefunction causes local planarization and the formation of an exciton-polaron. This torsional relaxation causes additional self-localization. Finally, and crucially, the torsional dynamics cause the Frenkel Hamiltonian to be time-dependent, leading to exciton dynamics. We identify two distinct types of dynamics. At low temperatures, the torsional fluctuations act as a perturbation on the polaronic nature of the exciton state. Thus, the exciton dynamics at low temperatures is a small-displacement diffusive adiabatic motion of the exciton-polaron as a whole. The temperature dependence of the diffusion constant has a linear dependence, indicating an activationless process. As the temperature increases, however, the diffusion constant increases at a faster than linear rate, indicating a second non-adiabatic dynamics mechanism begins to dominate. Excitons are thermally activated into higher energy more delocalized exciton states (i.e., LEGSs and QEESs). These states are not self-localized by local torsional planarization. During the exciton's temporary

  11. Multiple Exciton Generation in Colloidal Nanocrystals

    PubMed Central

    Smith, Charles; Binks, David

    2013-01-01

    In a conventional solar cell, the energy of an absorbed photon in excess of the band gap is rapidly lost as heat, and this is one of the main reasons that the theoretical efficiency is limited to ~33%. However, an alternative process, multiple exciton generation (MEG), can occur in colloidal quantum dots. Here, some or all of the excess energy is instead used to promote one or more additional electrons to the conduction band, potentially increasing the photocurrent of a solar cell and thereby its output efficiency. This review will describe the development of this field over the decade since the first experimental demonstration of multiple exciton generation, including the controversies over experimental artefacts, comparison with similar effects in bulk materials, and the underlying mechanisms. We will also describe the current state-of-the-art and outline promising directions for further development.

  12. Proposal for dark exciton based chemical sensors

    PubMed Central

    Feierabend, Maja; Berghäuser, Gunnar; Knorr, Andreas; Malic, Ermin

    2017-01-01

    The rapidly increasing use of sensors throughout different research disciplines and the demand for more efficient devices with less power consumption depends critically on the emergence of new sensor materials and novel sensor concepts. Atomically thin transition metal dichalcogenides have a huge potential for sensor development within a wide range of applications. Their optimal surface-to-volume ratio combined with strong light–matter interaction results in a high sensitivity to changes in their surroundings. Here, we present a highly efficient sensing mechanism to detect molecules based on dark excitons in these materials. We show that the presence of molecules with a dipole moment transforms dark states into bright excitons, resulting in an additional pronounced peak in easy accessible optical spectra. This effect exhibits a huge potential for sensor applications, since it offers an unambiguous optical fingerprint for the detection of molecules—in contrast to common sensing schemes relying on small peak shifts and intensity changes. PMID:28294110

  13. Emission of Tamm plasmon/exciton polaritons

    NASA Astrophysics Data System (ADS)

    Symonds, C.; Lemaître, A.; Homeyer, E.; Plenet, J. C.; Bellessa, J.

    2009-10-01

    We report on the observation of the strong coupling regime occurring between a Tamm plasmon (TP) mode and an exciton from inorganic quantum wells (QWs). The sample is formed by a silver thin film deposited onto an AlAs/GaAlAs Bragg reflector containing InGaAs QWs located in the high refractive index layers. Angular resolved reflectometry experiments evidence a clear anticrossing in the dispersion relations, a signature of the strong coupling regime. The Rabi splitting energy is 11.5 meV. The experimental data are in very good agreement with simple transfer matrix calculations. The emission from low and high energy TP/exciton polaritons is also demonstrated.

  14. Proposal for dark exciton based chemical sensors.

    PubMed

    Feierabend, Maja; Berghäuser, Gunnar; Knorr, Andreas; Malic, Ermin

    2017-03-15

    The rapidly increasing use of sensors throughout different research disciplines and the demand for more efficient devices with less power consumption depends critically on the emergence of new sensor materials and novel sensor concepts. Atomically thin transition metal dichalcogenides have a huge potential for sensor development within a wide range of applications. Their optimal surface-to-volume ratio combined with strong light-matter interaction results in a high sensitivity to changes in their surroundings. Here, we present a highly efficient sensing mechanism to detect molecules based on dark excitons in these materials. We show that the presence of molecules with a dipole moment transforms dark states into bright excitons, resulting in an additional pronounced peak in easy accessible optical spectra. This effect exhibits a huge potential for sensor applications, since it offers an unambiguous optical fingerprint for the detection of molecules-in contrast to common sensing schemes relying on small peak shifts and intensity changes.

  15. Proposal for dark exciton based chemical sensors

    NASA Astrophysics Data System (ADS)

    Feierabend, Maja; Berghäuser, Gunnar; Knorr, Andreas; Malic, Ermin

    2017-03-01

    The rapidly increasing use of sensors throughout different research disciplines and the demand for more efficient devices with less power consumption depends critically on the emergence of new sensor materials and novel sensor concepts. Atomically thin transition metal dichalcogenides have a huge potential for sensor development within a wide range of applications. Their optimal surface-to-volume ratio combined with strong light-matter interaction results in a high sensitivity to changes in their surroundings. Here, we present a highly efficient sensing mechanism to detect molecules based on dark excitons in these materials. We show that the presence of molecules with a dipole moment transforms dark states into bright excitons, resulting in an additional pronounced peak in easy accessible optical spectra. This effect exhibits a huge potential for sensor applications, since it offers an unambiguous optical fingerprint for the detection of molecules--in contrast to common sensing schemes relying on small peak shifts and intensity changes.

  16. Investigation of the collective properties of excitons in polar semiconductors (ZnO)

    SciTech Connect

    Litovchenko, V.G.; Korbutyak, D.V.; Kryuchenko, Y.V.

    1981-12-01

    Systematic investigations were made of the exciton--plasma collective effects in a semiconductor with polar binding. Two types of a bulk electron--hole liquid formed at high excitation intensities and relatively high temperatures (above that of liquid nitrogen). A quasi-two-dimensional liquid was observed on the surface of ZnO subjected to a low-dose argon ion treatment. The properties of a layer liquid, distinguishing it from the bulk form, were investigated. An analyisis was made of the phase diagrams for bound bulk and surface liquids.

  17. Imaging exciton-polariton transport in MoSe2 waveguides

    NASA Astrophysics Data System (ADS)

    Hu, F.; Luan, Y.; Scott, M. E.; Yan, J.; Mandrus, D. G.; Xu, X.; Fei, Z.

    2017-06-01

    The exciton-polariton (EP), a half-light and half-matter quasiparticle, is potentially an important element for future photonic and quantum technologies. It provides both strong light-matter interactions and long-distance propagation that is necessary for applications associated with energy or information transfer. Recently, strongly coupled cavity EPs at room temperature have been demonstrated in van der Waals (vdW) materials due to their strongly bound excitons. Here, we report a nano-optical imaging study of waveguide EPs in MoSe2, a prototypical vdW semiconductor. The measured propagation length of the EPs is sensitive to the excitation photon energy and reaches over 12 µm. The polariton wavelength can be conveniently altered from 600 nm down to 300 nm by controlling the waveguide thickness. Furthermore, we found an intriguing back-bending polariton dispersion close to the exciton resonance. The observed EPs in vdW semiconductors could be useful in future nanophotonic circuits operating in the near-infrared to visible spectral regions.

  18. Hole-Burning Spectroscopy on Excitonically Coupled Pigments in Proteins: Theory Meets Experiment.

    PubMed

    Adolphs, Julian; Berrer, Manuel; Renger, Thomas

    2016-03-09

    A theory for the calculation of resonant and nonresonant hole-burning (HB) spectra of pigment-protein complexes is presented and applied to the water-soluble chlorophyll-binding protein (WSCP) from cauliflower. The theory is based on a non-Markovian line shape theory ( Renger and Marcus J. Chem. Phys. 2002 , 116 , 9997 ) and includes exciton delocalization, vibrational sidebands, and lifetime broadening. An earlier approach by Reppert ( J. Phys. Chem. Lett. 2011 , 2 , 2716 ) is found to describe nonresonant HB spectra only. Here we present a theory that can be used for a quantitative description of HB data for both nonresonant and resonant burning conditions. We find that it is important to take into account the excess energy of the excitation in the HB process. Whereas excitation of the zero-phonon transition of the lowest exciton state, that is, resonant burning allows the protein to access only its conformational substates in the neighborhood of the preburn state, any higher excitation gives the protein full access to all conformations present in the original inhomogeneous ensemble. Application of the theory to recombinant WSCP from cauliflower, reconstituted with chlorophyll a or chlorophyll b, gives excellent agreement with experimental data by Pieper et al. ( J. Phys. Chem. B 2011 , 115 , 4053 ) and allows us to obtain an upper bound of the lifetime of the upper exciton state directly from the HB experiments in agreement with lifetimes measured recently in time domain 2D experiments by Alster et al. ( J. Phys. Chem. B 2014 , 118 , 3524 ).

  19. Resonant pairing of excitons in semiconductor heterostructures

    NASA Astrophysics Data System (ADS)

    Andreev, S. V.

    2016-10-01

    We suggest indirect excitons in two-dimensional semiconductor heterostructures as a platform for the realization of a bosonic analog of the Bardeen-Cooper-Schrieffer superconductor. The quantum phase transition to a biexcitonic gapped state can be controlled in situ by tuning the electric field applied to the structure in the growth direction. The proposed playground should allow one to go to strongly correlated and high-temperature regimes, unattainable with Feshbach resonant atomic gases.

  20. Miniband-related 1.4-1.8 μm luminescence of Ge/Si quantum dot superlattices

    NASA Astrophysics Data System (ADS)

    Talalaev, V. G.; Cirlin, G. E.; Tonkikh, A. A.; Zakharov, N. D.; Werner, P.; Gösele, U.; Tomm, J. W.; Elsaesser, T.

    2006-12-01

    The luminescence properties of highly strained, Sb-doped Ge/Si multi-layer heterostructures with incorporated Ge quantum dots (QDs) are studied. Calculations of the electronic band structure and luminescence measurements prove the existence of an electron miniband within the columns of the QDs. Miniband formation results in a conversion of the indirect to a quasi-direct excitons takes place. The optical transitions between electron states within the miniband and hole states within QDs are responsible for an intense luminescence in the 1.4-1.8 µm range, which is maintained up to room temperature. At 300 K, a light emitting diode based on such Ge/Si QD superlattices demonstrates an external quantum efficiency of 0.04% at a wavelength of 1.55 µm.

  1. Interlayer exciton dynamics in a dichalcogenide monolayer heterostructure

    NASA Astrophysics Data System (ADS)

    Nagler, Philipp; Plechinger, Gerd; Ballottin, Mariana V.; Mitioglu, Anatolie; Meier, Sebastian; Paradiso, Nicola; Strunk, Christoph; Chernikov, Alexey; Christianen, Peter C. M.; Schüller, Christian; Korn, Tobias

    2017-06-01

    In heterostructures consisting of different transition-metal dichalcogenide monolayers, a staggered band alignment can occur, leading to rapid charge separation of optically generated electron-hole pairs into opposite monolayers. These spatially separated electron-hole pairs are Coulomb-coupled and form interlayer excitons. Here, we study these interlayer excitons in a heterostructure consisting of MoSe2 and WSe2 monolayers using photoluminescence spectroscopy. We observe a non-trivial temperature dependence of the linewidth and the peak energy of the interlayer exciton, including an unusually strong initial redshift of the transition with temperature, as well as a pronounced blueshift of the emission energy with increasing excitation power. By combining these observations with time-resolved photoluminescence measurements, we are able to explain the observed behavior as a combination of interlayer exciton diffusion and dipolar, repulsive exciton-exciton interaction.

  2. Excitonic Stark effect in MoS2 monolayers

    NASA Astrophysics Data System (ADS)

    Scharf, Benedikt; Frank, Tobias; Gmitra, Martin; Fabian, Jaroslav; Žutić, Igor; Perebeinos, Vasili

    2016-12-01

    We theoretically investigate excitons in MoS2 monolayers in an applied in-plane electric field. Tight-binding and Bethe-Salpeter equation calculations predict a quadratic Stark shift, of the order of a few meV for fields of 10 V/μ m , in the linear absorption spectra. The spectral weight of the main exciton peaks decreases by a few percent with an increasing electric field due to the exciton field ionization into free carriers as reflected in the exciton wave functions. Subpicosecond exciton decay lifetimes at fields of a few tens of V/μ m could be utilized in solar energy harvesting and photodetection. We find simple scaling relations of the exciton binding, radius, and oscillator strength with the dielectric environment and an electric field, which provides a path to engineering the MoS2 electro-optical response.

  3. Hybrid states of Tamm plasmons and exciton-polaritons

    NASA Astrophysics Data System (ADS)

    Kaliteevski, M.; Brand, S.; Abram, R. A.; Iorsh, I.; Kavokin, A. V.; Liew, T. C. H.; Shelykh, I. A.

    2011-03-01

    We have demonstrated theoretically that it is possible to use the resonant coupling of exciton-polaritons in a planar microcavity and Tamm plasmons at a metal film on the surface of the structure to provide lateral spatial control of the exciton-polaritons within the cavity. The resonant coupling of the Tamm plasmons to cavity exciton-polaritons results in a triplet of hybrid plasmon-exciton-polariton modes with the lowest at a significantly lower energy than that of the unperturbed exciton-polaritons. Further, a patterned metal film on the structure surface can provide a sufficiently large lateral modulation of the excitation energy that localization of the exciton-polaritons within chosen regions of the cavity is possible. We show how the approach opens the way to a practical demonstration of polariton channels, traps, and devices, including logic gates.

  4. Singlet exciton fission in nanostructured organic solar cells.

    PubMed

    Jadhav, Priya J; Mohanty, Aseema; Sussman, Jason; Lee, Jiye; Baldo, Marc A

    2011-04-13

    Singlet exciton fission is an efficient multiexciton generation process in organic molecules. But two concerns must be satisfied before it can be exploited in low-cost solution-processed organic solar cells. Fission must be combined with longer wavelength absorption in a structure that can potentially surpass the single junction limit, and its efficiency must be demonstrated in nanoscale domains within blended devices. Here, we report organic solar cells comprised of tetracene, copper phthalocyanine, and the buckyball C(60). Short wavelength light generates singlet excitons in tetracene. These are subsequently split into two triplet excitons and transported through the phthalocyanine. In addition, the phthalocyanine absorbs photons below the singlet exciton energy of tetracene. To test tetracene in nanostructured blends, we fabricate coevaporated bulk heterojunctions and multilayer heterojunctions of tetracene and C(60). We measure a singlet fission efficiency of (71 ± 18)%, demonstrating that exciton fission can efficiently compete with exciton dissociation on the nanoscale.

  5. Geometric decoherence of valley excitons in monolayer transition metal dichalcogenides

    NASA Astrophysics Data System (ADS)

    Gong, Z. R.; Jiang, Z. F.; Xu, Fuming; Wang, B.; Fu, H. C.

    2017-07-01

    We study the effects of the Berry phases of the valley excitons in the monolayer transition metal dichalcogenides (TMDs) when the valley excitons are manipulated by an external terahertz field. We find that the decoherence of the valley degree of freedom of the valley excitons is spontaneously induced because of the different Berry phases of valley excitons accumulated along the opposite trajectories under the manipulation of the external field. It is called the geometric decoherence because it completely results from the geometric phases. The obvious phenomenon related to such spontaneous decoherence is the gradual decrement of the dipole moment matrix element of the valley exciton and consequently the decrement of the emitted signals after the valley excitons are recombined. Moreover, another effect due to the Berry phases is the giant Faraday rotation of the polarization of the emitted photons. Such imperfection of the valley degree of freedom is supposed to provide the potential limits of the valleytronics based on the TMDs optoelecronic devices.

  6. Exciton/plasmon mixing in metal-semiconductor heterostructures

    NASA Astrophysics Data System (ADS)

    Symonds, Clémentine; Bellessa, Joel; Plenet, Jean-Claude; Cambril, Edmond; Miard, Audrey; Ferlazzo, Laurence; Lemaître, Aristide

    2010-01-01

    We report on the strong coupling between surface plasmons and inorganic quantum well excitons. The sample is formed by a corrugated silver film deposited on the top of a heterostructure consisting of five GaAs/GaAlAs quantum wells grown by molecular beam epitaxy. Reflectometry experiments at low temperature (77 K) evidence the formation of plasmon/heavy-hole exciton/light-hole exciton mixed states. The interaction energies, deduced by fitting the experimental data with a coupled oscillator model, amount to 22 meV for the plasmon/light-hole exciton and 21 meV for the plasmon/heavy-hole exciton. Some particularities of the plasmon-exciton coupling are also discussed and qualitatively related to the plasmon polarization.

  7. Chiral topological excitons in the monolayer transition metal dichalcogenides

    PubMed Central

    Gong, Z. R.; Luo, W. Z.; Jiang, Z. F.; Fu, H. C.

    2017-01-01

    We theoretically investigate the chiral topological excitons emerging in the monolayer transition metal dichalcogenides, where a bulk energy gap of valley excitons is opened up by a position dependent external magnetic field. We find two emerging chiral topological nontrivial excitons states, which exactly connects to the bulk topological properties, i.e., Chern number = 2. The dependence of the spectrum of the chiral topological excitons on the width of the magnetic field domain wall as well as the magnetic filed strength is numerically revealed. The chiral topological valley excitons are not only important to the excitonic transport due to prevention of the backscattering, but also give rise to the quantum coherent control in the optoelectronic applications. PMID:28186154

  8. Chiral topological excitons in the monolayer transition metal dichalcogenides.

    PubMed

    Gong, Z R; Luo, W Z; Jiang, Z F; Fu, H C

    2017-02-10

    We theoretically investigate the chiral topological excitons emerging in the monolayer transition metal dichalcogenides, where a bulk energy gap of valley excitons is opened up by a position dependent external magnetic field. We find two emerging chiral topological nontrivial excitons states, which exactly connects to the bulk topological properties, i.e., Chern number = 2. The dependence of the spectrum of the chiral topological excitons on the width of the magnetic field domain wall as well as the magnetic filed strength is numerically revealed. The chiral topological valley excitons are not only important to the excitonic transport due to prevention of the backscattering, but also give rise to the quantum coherent control in the optoelectronic applications.

  9. Chiral topological excitons in the monolayer transition metal dichalcogenides

    NASA Astrophysics Data System (ADS)

    Gong, Z. R.; Luo, W. Z.; Jiang, Z. F.; Fu, H. C.

    2017-02-01

    We theoretically investigate the chiral topological excitons emerging in the monolayer transition metal dichalcogenides, where a bulk energy gap of valley excitons is opened up by a position dependent external magnetic field. We find two emerging chiral topological nontrivial excitons states, which exactly connects to the bulk topological properties, i.e., Chern number = 2. The dependence of the spectrum of the chiral topological excitons on the width of the magnetic field domain wall as well as the magnetic filed strength is numerically revealed. The chiral topological valley excitons are not only important to the excitonic transport due to prevention of the backscattering, but also give rise to the quantum coherent control in the optoelectronic applications.

  10. 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.

  11. Wannier-Mott excitons in semiconductors with a superlattice

    SciTech Connect

    Suris, R. A.

    2015-06-15

    The effect of the motion of a Wannier-Mott exciton in semiconductors with a superlattice formed by heterojunctions on the exciton binding energy and wave function is analyzed. This effect arises as a result of the fact that the dispersion laws of the electron and hole that form an exciton in a superlattice differ from the quadratic law. The investigated one-dimensional superlattice consists of alternating semiconductor layers with different energy positions of the conduction and valence bands, i.e., with one-dimensional wells and barriers. The exciton state in a superlattice consisting of quantum dots is analyzed. It is demonstrated that the closer the electron and hole effective masses, the greater the dependence of the binding energy on the exciton quasi-momentum. The possibility of replacing the tunneling excitation transfer between superlattice cells with the dipole-dipole one at certain exciton quasi-wave vector values is investigated.

  12. Engineering and manipulating exciton wave packets

    NASA Astrophysics Data System (ADS)

    Zang, Xiaoning; Montangero, Simone; Carr, Lincoln D.; Lusk, Mark T.

    2017-05-01

    When a semiconductor absorbs light, the resulting electron-hole superposition amounts to a uncontrolled quantum ripple that eventually degenerates into diffusion. If the conformation of these excitonic superpositions could be engineered, though, they would constitute a new means of transporting information and energy. We show that properly designed laser pulses can be used to create such excitonic wave packets. They can be formed with a prescribed speed, direction, and spectral make-up that allows them to be selectively passed, rejected, or even dissociated using superlattices. Their coherence also provides a handle for manipulation using active, external controls. Energy and information can be conveniently processed and subsequently removed at a distant site by reversing the original procedure to produce a stimulated emission. The ability to create, manage, and remove structured excitons comprises the foundation for optoexcitonic circuits with application to a wide range of quantum information, energy, and light-flow technologies. The paradigm is demonstrated using both tight-binding and time-domain density functional theory simulations.

  13. Fractional Solitons in Excitonic Josephson Junctions

    PubMed Central

    Hsu, Ya-Fen; Su, Jung-Jung

    2015-01-01

    The Josephson effect is especially appealing to physicists because it reveals macroscopically the quantum order and phase. In excitonic bilayers the effect is even subtler due to the counterflow of supercurrent as well as the tunneling between layers (interlayer tunneling). Here we study, in a quantum Hall bilayer, the excitonic Josephson junction: a conjunct of two exciton condensates with a relative phase ϕ0 applied. The system is mapped into a pseudospin ferromagnet then described numerically by the Landau-Lifshitz-Gilbert equation. In the presence of interlayer tunneling, we identify a family of fractional sine-Gordon solitons which resemble the static fractional Josephson vortices in the extended superconducting Josephson junctions. Each fractional soliton carries a topological charge Q that is not necessarily a half/full integer but can vary continuously. The calculated current-phase relation (CPR) shows that solitons with Q = ϕ0/2π is the lowest energy state starting from zero ϕ0 – until ϕ0 > π – then the alternative group of solitons with Q = ϕ0/2π − 1 takes place and switches the polarity of CPR. PMID:26511770

  14. Multiple Exciton Generation in Semiconductor Quantum Dots.

    PubMed

    Beard, Matthew C

    2011-06-02

    Multiple exciton generation in quantum dots (QDs) has been intensively studied as a way to enhance solar energy conversion by utilizing the excess energy in the absorbed photons. Among other useful properties, quantum confinement can both increase Coulomb interactions that drive the MEG process and decrease the electron-phonon coupling that cools hot excitons in bulk semiconductors. However, variations in the reported enhanced quantum yields (QYs) have led to disagreements over the role that quantum confinement plays. The enhanced yield of excitons per absorbed photon is deduced from a dynamical signature in the transient absorption or transient photoluminescence and is ascribed to the creation of biexcitons. Extraneous effects such as photocharging are partially responsible for the observed variations. When these extraneous effects are reduced, the MEG efficiency, defined in terms of the number of additional electron-hole pairs produced per additional band gap of photon excitation, is about two times better in PbSe QDs than that in bulk PbSe. Thin films of electronically coupled QDs have shown promise in simple photon-to-electron conversion architectures. If the MEG efficiency can be further enhanced and charge separation and transport can be optimized within QD films, then QD solar cells can lead to third-generation solar energy conversion technologies.

  15. Fractional Solitons in Excitonic Josephson Junctions

    NASA Astrophysics Data System (ADS)

    Hsu, Ya-Fen; Su, Jung-Jung

    2015-10-01

    The Josephson effect is especially appealing to physicists because it reveals macroscopically the quantum order and phase. In excitonic bilayers the effect is even subtler due to the counterflow of supercurrent as well as the tunneling between layers (interlayer tunneling). Here we study, in a quantum Hall bilayer, the excitonic Josephson junction: a conjunct of two exciton condensates with a relative phase ϕ0 applied. The system is mapped into a pseudospin ferromagnet then described numerically by the Landau-Lifshitz-Gilbert equation. In the presence of interlayer tunneling, we identify a family of fractional sine-Gordon solitons which resemble the static fractional Josephson vortices in the extended superconducting Josephson junctions. Each fractional soliton carries a topological charge Q that is not necessarily a half/full integer but can vary continuously. The calculated current-phase relation (CPR) shows that solitons with Q = ϕ0/2π is the lowest energy state starting from zero ϕ0 - until ϕ0 > π - then the alternative group of solitons with Q = ϕ0/2π - 1 takes place and switches the polarity of CPR.

  16. Topological Excitonic Superfluids in Three Dimensions

    NASA Astrophysics Data System (ADS)

    Gilbert, Matthew; Hankiewicz, Ewelina; Kim, Youngseok

    2013-03-01

    We study the equilibrium and non-equilibrium properties of topological dipolar intersurface exciton condensates within time-reversal invariant topological insulators in three spatial dimensions without a magnetic field. We elucidate that, in order to correctly identify the proper pairing symmetry within the condensate order parameter, the full three-dimensional Hamiltonian must be considered. As a corollary, we demonstrate that only particles with similar chirality play a significant role in condensate formation. Furthermore, we find that the intersurface exciton condensation is not suppressed by the interconnection of surfaces in three-dimensional topological insulators as the intersurface polarizability vanishes in the condensed phase. This eliminates the surface current flow leaving only intersurface current flow through the bulk. We conclude by illustrating how the excitonic superfluidity may be identified through an examination of the terminal currents above and below the condensate critical current. Army Research Office (ARO) under contract number W911NF-09-1-0347, the Office of Naval Research (ONR) under contract number N0014-11-1-0728, and the Air Force Office of Scientific Research (AFOSR) under contract number FA9550-10-1-0459, DFG Grant HA 5893

  17. Microcavity controlled coupling of excitonic qubits.

    PubMed

    Albert, F; Sivalertporn, K; Kasprzak, J; Strauß, M; Schneider, C; Höfling, S; Kamp, M; Forchel, A; Reitzenstein, S; Muljarov, E A; Langbein, W

    2013-01-01

    Controlled non-local energy and coherence transfer enables light harvesting in photosynthesis and non-local logical operations in quantum computing. This process is intuitively pictured by a pair of mechanical oscillators, coupled by a spring, allowing for a reversible exchange of excitation. On a microscopic level, the most relevant mechanism of coherent coupling of distant quantum bits--like trapped ions, superconducting qubits or excitons confined in semiconductor quantum dots--is coupling via the electromagnetic field. Here we demonstrate the controlled coherent coupling of spatially separated quantum dots via the photon mode of a solid state microresonator using the strong exciton-photon coupling regime. This is enabled by two-dimensional spectroscopy of the sample's coherent response, a sensitive probe of the coherent coupling. The results are quantitatively understood in a rigorous description of the cavity-mediated coupling of the quantum dot excitons. This mechanism can be used, for instance in photonic crystal cavity networks, to enable a long-range, non-local coherent coupling.

  18. 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

    2016-03-17

    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.

  19. Plasmon-Frenkel-exciton in a clustered solid

    NASA Astrophysics Data System (ADS)

    Rotkin, Slava V.; Suris, Robert A.

    1998-08-01

    The standard theory of the Frenkel exciton (a small radius exciton) is applied to a fullerene 2D solid. It is the dipole collective electron excitation of a single cluster which forms the delocalized plasmon-Frenkel-exciton (PFE) in a crystal. The PFE retarded interaction is taken into account. We present transverse PFE-polariton dispersion curves along with the Coulomb problem solution for longitudinal excitation in the 2D plane.

  20. Spatially indirect exciton condensate phases in double bilayer graphene

    NASA Astrophysics Data System (ADS)

    Su, Jung-Jung; MacDonald, Allan H.

    2017-01-01

    We present a theory of spatially indirect exciton condensate states in systems composed of a pair of electrically isolated Bernal graphene bilayers. The ground-state phase diagram in a two-dimensional displacement-field/inter-bilayer-bias space includes layer-polarized semiconductors, spin-density-wave states, exciton condensates, and states with mixed excitonic and spin order. We find that two different condensate states, distinguished by a chirality index, are stable under different electrical control conditions.

  1. Photogenerated exciton dissociation in highly coupled lead salt nanocrystal assemblies.

    PubMed

    Choi, Joshua J; Luria, Justin; Hyun, Byung-Ryool; Bartnik, Adam C; Sun, Liangfeng; Lim, Yee-Fun; Marohn, John A; Wise, Frank W; Hanrath, Tobias

    2010-05-12

    Internanocrystal coupling induced excitons dissociation in lead salt nanocrystal assemblies is investigated. By combining transient photoluminescence spectroscopy, grazing incidence small-angle X-ray scattering, and time-resolved electric force microscopy, we show that excitons can dissociate, without the aid of an external bias or chemical potential gradient, via tunneling through a potential barrier when the coupling energy is comparable to the exciton binding energy. Our results have important implications for the design of nanocrystal-based optoelectronic devices.

  2. Evidence That the Anomalous Emission from CaF2:Yb(2+) Is Not Described by the Impurity Trapped Exciton Model.

    PubMed

    MacKeen, C; Bridges, F; Kozina, M; Mehta, A; Reid, M F; Wells, J-P R; Barandiarán, Z

    2017-07-20

    Yb-substituted CaF2 exhibits an anomalous red-shifted luminescence after UV excitation, attributed to the relaxation of impurity trapped excitons (ITE). CaF2:Yb is the archetype system for this model, in which the Yb(2+) ions can be excited into a long-lived (ms) exciton state. Upon de-excitation, the emission intensity should be proportional to the Yb(2+) concentration, but that could not be checked when this model was first proposed. Using the X-ray absorption near edge structure (XANES) technique, we determine the fractions of Yb(2+) and Yb(3+) for low Yb concentrations, 0.01% to 0.1%, and thus determine the net concentration of Yb(2+). A comparison with luminescence data shows that the intensity is not proportional to the Yb(2+) concentration, and only a fraction of Yb(2+) ions contributes to the anomalous luminescence. This is inconsistent with the ITE model and illustrates the importance of checking the dependence of the emission intensity on the Yb(2+) concentration.

  3. A spectroscopic study of the wavelength-dependent photoisomerizations of bilirubins bound to human serum albumin

    NASA Astrophysics Data System (ADS)

    Mazzoni, Marina; Agati, Giovanni; Pratesi, Riccardo; Persico, Maurizio

    2005-12-01

    The wavelength-dependent photoisomerizations of the asymmetric bilirubin BR-IXα and of the symmetric bilirubin-IIIα (BR-III) and mesobilirubin-XIIIα (MBR-XIII) bound to human serum albumin (HSA) in aqueous solution were analysed with the help of an exciton coupling model. The modelling was based on the absorption and circular dichroism (CD) spectra (bisignate Cotton effect). Time-dependent density functional theory (TD-DFT) of the free BR-IX molecule suggested the presence of two main bands of exciton coupling character in the blue region of the spectrum, and other weaker bands of charge transfer character at longer wavelengths. These peculiarities were taken into account to fit the photoisomerization quantum yields in the blue-green region as functions of the wavelength, obtaining the bandshape of the exciton coupling bands from the experimental CD spectra. The other excitons were extracted from the decomposition of the band resulting from the difference between the absorption spectrum and the sum (normalized-to-absorption) of the two CD excitons. We expressed photoisomerization quantum yields in terms of the sum of the contributions to photon absorption deriving from all the exciton states normalized to total absorption. For all the reversible photoprocesses of bilirubins and for the irreversible one of BR-IXα in HSA (i.e. lumirubin formation), we give reliable mean values of the individual state excitation probabilities and photoisomerization efficiencies in the pigment protein complex.

  4. Simulations of singlet exciton diffusion in organic semiconductors: a review

    SciTech Connect

    Bjorgaard, Josiah A.; Kose, Muhammet Erkan

    2014-12-22

    Our review describes the various aspects of simulation strategies for exciton diffusion in condensed phase thin films of organic semiconductors. Several methods for calculating energy transfer rate constants are discussed along with procedures for how to account for energetic disorder. Exciton diffusion can be modelled by using kinetic Monte-Carlo methods or master equations. Recent literature on simulation efforts for estimating exciton diffusion lengths of various conjugated polymers and small molecules are introduced. Moreover, these studies are discussed in the context of the effects of morphology on exciton diffusion and the necessity of accurate treatment of disorder for comparison of simulation results with those of experiment.

  5. Multiple exciton generation and recombination in carbon nanotubes and nanocrystals.

    PubMed

    Kanemitsu, Yoshihiko

    2013-06-18

    Semiconducting nanomaterials such as single-walled carbon nanotubes (SWCNTs) and nanocrystals (NCs) exhibit unique size-dependent quantum properties. They have therefore attracted considerable attention from the viewpoints of fundamental physics and functional device applications. SWCNTs and NCs also provide an excellent new stage for experimental studies of many-body effects of electrons and excitons on optical processes in nanomaterials. In this Account, we discuss multiple exciton generation and recombination in SWCNTs and NCs for next-generation photovoltaics. Strongly correlated ensembles of conduction-band electrons and valence-band holes in semiconductors are complex quantum systems that exhibit unique optical phenomena. In bulk crystals, the carrier recombination dynamics can be described by a simple model, which includes the nonradiative single-carrier trapping rate, the radiative two-carrier recombination rate, and the nonradiative three-carrier Auger recombination rate. The nonradiative Auger recombination rate determines the carrier recombination dynamics at high carrier density and depends on the spatial localization of carriers in two-dimensional quantum wells. The Auger recombination and multiple exciton generation rates can be advantageously manipulated by nanomaterials with designated energy structures. In addition, SWCNTs and NCs show quantized recombination dynamics of multiple excitons and carriers. In one-dimensional SWCNTs, excitons have large binding energies and are very stable at room temperature. The extremely rapid Auger recombination between excitons determines the photoluminescence (PL) intensity, the PL linewidth, and the PL lifetime. SWCNTs can undergo multiple exciton generation, while strong exciton-exciton interactions and complicated exciton structures affect the quantized Auger rate and the multiple exciton generation efficiency. Interestingly, in zero-dimensional NC quantum dots, quantized Auger recombination causes unique

  6. Exciton transport in π-conjugated polymers with conjugation defects.

    PubMed

    Meng, Ruixuan; Li, Yuan; Li, Chong; Gao, Kun; Yin, Sun; Wang, Luxia

    2017-09-06

    In π-conjugated polymers for photovoltaic applications, intrinsic conjugation defects are known to play crucial roles in impacting exciton transport after photoexcitation. However, the understanding of the associated microscopic processes still remains limited. Here, we present a theoretical investigation of the effects of different conjugation defects on the dynamics of exciton transport in two linearly coupled poly(p-phenylene vinylene) (PPV) molecules. The model system is constructed by employing an extended version of the Su-Schrieffer-Heeger model and the exciton behaviors are simulated by means of a quantum nonadiabatic dynamics. We identify two types of conjugation defects, i.e., weakening conjugation and strengthening conjugation, which are demonstrated to play different roles in impacting the dynamics of exciton transport in the system. The weakening conjugation acts as an energy well inclined to trap a moving exciton, while the strengthening conjugation acts as an energy barrier inclined to block the exciton. We also systematically simulate both intrachain and interchain dynamics of exciton transport, and find that an exciton could experience a "short-time delaying", "trapping", "blocking", or "hopping" process, which is determined by the defect type, strength, and position. These findings provide a microscopic understanding of how the exciton transport dynamics can be impacted by conjugation defects in an actual polymer system.

  7. Exciton management in organic photovoltaic multidonor energy cascades.

    PubMed

    Griffith, Olga L; Forrest, Stephen R

    2014-05-14

    Multilayer donor regions in organic photovoltaics show improved power conversion efficiency when arranged in decreasing exciton energy order from the anode to the acceptor interface. These so-called "energy cascades" drive exciton transfer from the anode to the dissociating interface while reducing exciton quenching and allowing improved overlap with the solar spectrum. Here we investigate the relative importance of exciton transfer and blocking in a donor cascade employing diphenyltetracene (D1), rubrene (D2), and tetraphenyldibenzoperiflanthene (D3) whose optical gaps monotonically decrease from D1 to D3. In this structure, D1 blocks excitons from quenching at the anode, D2 accepts transfer of excitons from D1 and blocks excitons at the interface between D2 and D3, and D3 contributes the most to the photocurrent due to its strong absorption at visible wavelengths, while also determining the open circuit voltage. We observe singlet exciton Förster transfer from D1 to D2 to D3 consistent with cascade operation. The power conversion efficiency of the optimized cascade OPV with a C60 acceptor layer is 7.1 ± 0.4%, which is significantly higher than bilayer devices made with only the individual donors. We develop a quantitative model to identify the dominant exciton processes that govern the photocurrent generation in multilayer organic structures.

  8. Surface photovoltage in exciton absorption range in CdS

    NASA Technical Reports Server (NTRS)

    Morawski, A.; Banisch, R.; Lagowski, J.

    1977-01-01

    The high resolution, intrinsic spectra of surface photovoltage are reported for semiconducting n-type CdS single crystals. At reduced temperatures (120-160 K) the spectra exhibit three sharp maxima due to A, B and C free exciton transitions. Energy positions of these lines and valence band parameters (spin-orbit and crystal field splittings) estimated from surface photovoltage are in good agreement with values obtained by other methods. The excitonic transitions are very sensitive to surface treatment, i.e. polishing, etching, background illumination and surface doping. The mechanism of direct interaction of free excitons with surface states is proposed to explain exciton lines in surface photovoltage.

  9. Charged excitons in modulation-doped quantum wires

    NASA Astrophysics Data System (ADS)

    Otterburg, T.; Oberli, D. Y.; Dupertuis, M.-A.; Moret, N.; Malko, A.; Pelucchi, E.; Dwir, B.; Kapon, E.

    2005-06-01

    We report on the observation of negatively- and positively-charged excitons in the photoluminescence spectra of V-groove quantum wires. The charged exciton binding energy increases with the strength of the quantum confinement. We demonstrate that fluctuations of the confinement potential cause the localization of the exciton and of the charged exitons on the same location. We discover that a large fraction of the enhancement of the charged exciton "binding energies" has a kinetic origin associated with the recoil energy transferred to the remaining carrier during the emission process.

  10. Phase diagram of microcavity exciton-polariton condensates

    NASA Astrophysics Data System (ADS)

    Bui, Dinh-Hoi; Phan, Van-Nham

    2016-12-01

    In this work, we study the exciton-polariton condensate phase transition in a microcavity matter-light system in which electron-hole Coulomb interaction and matter-light coupling effects are treated on an equal footing. In the framework of the unrestricted Hartree-Fock approximation applying the two-dimensional exciton-polariton model, we derive the self-consistent equations determining simultaneously the excitonic and the photonic condenstate order parameters. In the thermal-equilibrium limit, we find a condensed state of the exciton-polariton systems and phase diagrams are then constructed. At a given low temperature, the condensate by its nature shows a crossover from an excitonic to a polaritonic and finally photonic condensed state as the excitation density increases at large detuning. Without the detuning, the excitonic condensed state disappears whereas the polaritonic or photonic phases dominate. The crossover is also found by lowering the Coulomb interaction at a finite matter-light coupling. Lowering the Coulomb interaction or increasing the temperature, the excitonic Mott transition occurs, at which the exciton-polariton condensates dissociate to free electron-hole/photon. Depending on temperature and excitation density, the phase transition of the exciton-polariton condensates is also addressed in signatures of photoluminescence mapping to the photonic momentum distribution.

  11. Minimal model for charge transfer excitons at the dielectric interface

    NASA Astrophysics Data System (ADS)

    Ono, Shota; Ohno, Kaoru

    2016-03-01

    A theoretical description of the charge transfer (CT) exciton across the donor-acceptor interface without the use of a completely localized hole (or electron) is a challenge in the field of organic solar cells. We calculate the total wave function of the CT exciton by solving an effective two-particle Schrödinger equation for the inhomogeneous dielectric interface. We formulate the magnitude of the CT and construct a minimal model of the CT exciton under the breakdown of inversion symmetry. We demonstrate that both a light hole mass and a hole localization along the normal to the dielectric interface are crucial to yield the CT exciton.

  12. Localization length scales of triplet excitons in singlet fission materials

    NASA Astrophysics Data System (ADS)

    Bayliss, Sam L.; Thorley, Karl J.; Anthony, John E.; Bouchiat, Hélène; Greenham, Neil C.; Chepelianskii, Alexei D.

    2015-09-01

    We measure the dielectric confinement length scales of triplet excitons in organic semiconductors by jointly measuring their microwave-domain electric and magnetic susceptibilities. We apply this technique to characterize triplet excitons in two singlet fission materials with distinct solid-state packing and correlate the extracted localization length scales with the role of the excitonic environment. By using the magnetic susceptibility simultaneously determined through our experiments, we compare the independently extracted dielectric and spin-spin localization length scales, highlighting the role of local anisotropy on the properties of excitonic triplet states.

  13. Phase diagram for the trapping kinetics of partially coherent excitons

    NASA Astrophysics Data System (ADS)

    Pearlstein, Robert M.

    1998-06-01

    The kinetics of exciton trapping within molecular assemblies similar to those of recently reported structural models of photosynthetic light-harvesting antennas have been described theoretically for any degree of exciton coherence. It is shown here that in the space of two of the kinetic parameters - the local exciton scattering rate constant and the nearest-neighbor separation distance of the exciton-generating transition dipoles - the trapping kinetics segregate into coherent and incoherent phases delineated by universal curves. Consequences of these findings are discussed, particularly as they may apply to purple photosynthetic bacteria.

  14. Plasmon-induced enhancement of yellow-red luminescence in InGaN/Au nanocomposites

    SciTech Connect

    Belyaev, K. G. Usikova, A. A.; Jmerik, V. N.; Kop’ev, P. S.; Ivanov, S. V.; Toropov, A. A.; Brunkov, P. N.

    2015-02-15

    A significant (by up to a factor of 7) increase in the internal quantum efficiency of luminescence is achieved at room temperature in semiconductor-metal-insulator hybrid structures fabricated by the successive deposition of gold and Si{sub 3}N{sub 4} over an array of InGaN nanoblocks, grown by molecular-beam epitaxy. The observed effect can be accounted for by the resonant interaction of excitons localized in InGaN nanoblocks with localized surface-plasmon modes in gold intrusions embedded into InGaN and Si{sub 3}N{sub 4}.

  15. Luminescence excitation of InAs/GaAs coupled quantum dots

    NASA Astrophysics Data System (ADS)

    Garrido, Mauricio; Wijesundara, Kushal C.; Ramanathan, Swati; Stinaff, Eric A.; Scheibner, Michael; Bracker, Allan S.; Gammon, Dan

    2008-03-01

    An understanding of the excited states in coupled quantum dots is a necessary step in the road towards a coherent control of this system. Photoluminescence excitation studies were performed on an InAs/GaAs coupled quantum dot system embedded in a Schottky diode structure. The ground states of the positive trion, negative trion and neutral exciton are first clearly identified by their photoluminescence spectra in bias maps. Preliminary results are reported on the luminescence excitation spectra of these charge configurations; both near and far away from the region where molecule-like behavior is observed.

  16. X-ray-excited optical luminescence and X-ray absorption fine-structures studies of CdWO4 scintillator.

    PubMed

    Novais, S M V; Valerio, M E G; Macedo, Z S

    2012-07-01

    X-ray-excited optical luminescence (XEOL) emission and excitation spectra as well as the EXAFS signal of CdWO(4) were measured in the energy region of the Cd and W absorption edges. From EXAFS refinement, structural parameters such as number of atoms, distance from the absorbing atom and width of coordination shells in the W neighborhood were determined. The role of W-O interactions on the intrinsic luminescence of CdWO(4) is discussed. The efficiencies of conversion, transfer and emission processes involved in the scintillation mechanism showed to be high when self-trapped excitons are formed locally by direct excitation of W ions. Annihilation of these excitons provides the characteristic scintillation of CdWO(4), a broad band emission with maximum at 500 nm. The presence of two energetically different O positions in the lattice gives rise to the composite structure of the luminescence band, and no influence of extrinsic defects was noticed. A mismatch between the X-ray absorption coefficient and the zero-order luminescence curves corroborates that the direct excitation of Cd ions induces secondary electronic excitations not very effective in transferring energy to the luminescent group, WO(6).

  17. Analysis of wavelength-dependent photoisomerization quantum yields in bilirubins by fitting two exciton absorption bands

    NASA Astrophysics Data System (ADS)

    Mazzoni, M.; Agati, G.; Troup, G. J.; Pratesi, R.

    2003-09-01

    The absorption spectra of bilirubins were deconvoluted by two Gaussian curves of equal width representing the exciton bands of the non-degenerate molecular system. The two bands were used to study the wavelength dependence of the (4Z, 15Z) rightarrow (4Z, 15E) configurational photoisomerization quantum yield of the bichromophoric bilirubin-IXalpha (BR-IX), the intrinsically asymmetric bile pigment associated with jaundice and the symmetrically substituted bilirubins (bilirubin-IIIalpha and mesobilirubin-XIIIalpha), when they are irradiated in aqueous solution bound to human serum albumin (HSA). The same study was performed for BR-IX in ammoniacal methanol solution (NH4OH/MeOH). The quantum yields of the configurational photoprocesses were fitted with a combination function of the two Gaussian bands normalized to the total absorption, using the proportionality coefficients and a scaling factor as parameters. The decrease of the (4Z, 15Z) rightarrow (4Z, 15E) quantum yield with increasing wavelength, which occurs for wavelengths longer than the most probable Franck-Condon transition of the molecule, did not result in a unique function of the exciton absorptions. In particular we found two ranges corresponding to different exciton interactions with different proportionality coefficients and scaling factors. The wavelength-dependent photoisomerization of bilirubins was described as an abrupt change in quantum yield as soon as the resulting excitation was strongly localized in each chromophore. The change was correlated to a variation of the interaction between the two chromophores when the short-wavelength exciton absorption became vanishingly small. With the help of the circular dichroism (CD) spectrum of BR-IX in HSA, a small band was resolved in the bilirubin absorption spectrum, delivering part of the energy required for the (4Z, 15Z) rightarrow (4Z, 15E) photoisomerization of the molecule.

  18. Excitons and multi-excitons in single CdTe quantum dots probed by near-field spectroscopy

    NASA Astrophysics Data System (ADS)

    Brun, M.; Huant, S.; Woehl, J. C.; Motte, J.-F.; Marsal, L.; Mariette, H.

    2002-03-01

    A near-field optical spectroscopy study of a single CdTe/ZnTe quantum dot at low temperatures is presented. While the photoluminescence spectrum at low excitation power reveals only one single sharp peak due to the radiative recombination of excitons (X) in the single dot, several additional sharp peaks appear with increasing excitation density. The dominant features are ascribed to exciton complexes and charged exciton complexes such as negatively charged excitons (X -), neutral (2X and 3X) and negative (2X - and 3X -) biexcitons and triexcitons. Exciton charging arises due to efficient hole trapping by residual acceptors in the barrier material. This partly inhibits the formation of biexcitons and triexcitons. A spectral feature appearing close to the X - peak is tentatively assigned to X 2- negative excitons. This feature is found to shift to the red with increasing power: two possible explanations for this unexpected behaviour are proposed.

  19. Comparison of transient state and steady state exciton-exciton annihilation rates based on Förster-type energy transfer

    NASA Astrophysics Data System (ADS)

    Yonehara, Toshiya; Goushi, Kenichi; Sawabe, Tomoaki; Takasu, Isao; Adachi, Chihaya

    2015-07-01

    We investigated differences between the transient state and steady state exciton-exciton annihilation rates based on Förster-type energy transfer. The exciton-exciton annihilation rate of an organic semiconductor is usually determined by transient state photoluminescence measurements using a pulsed laser or steady state photoluminescence measurements using a continuous wave laser. However, it is unclear that the respective annihilation rates determined by their rate equations are the same. In calculations with platinum-octaethylporphyrin (PtOEP) parameters, Monte Carlo simulations gave two different annihilation rates for the transient state and the steady state. The analytical models based on Förster-type energy transfer also showed the same result. These results indicate that the exciton-exciton annihilation rates in transient state and steady state are distinguished.

  20. Picosecond Dynamics of Excitonic Magnetic Polarons in Colloidal Diffusion-Doped Cd(1-x)Mn(x)Se Quantum Dots.

    PubMed

    Nelson, Heidi D; Bradshaw, Liam R; Barrows, Charles J; Vlaskin, Vladimir A; Gamelin, Daniel R

    2015-11-24

    Spontaneous magnetization is observed at zero magnetic field in photoexcited colloidal Cd(1-x)Mn(x)Se (x = 0.13) quantum dots (QDs) prepared by diffusion doping, reflecting strong Mn(2+)-exciton exchange coupling. The picosecond dynamics of this phenomenon, known as an excitonic magnetic polaron (EMP), are examined using a combination of time-resolved photoluminescence, magneto-photoluminescence, and Faraday rotation (TRFR) spectroscopies, in conjunction with continuous-wave absorption, magnetic circular dichroism (MCD), and magnetic circularly polarized photoluminescence (MCPL) spectroscopies. The data indicate that EMPs form with random magnetization orientations at zero external field, but their formation can be directed by an external magnetic field. After formation, however, external magnetic fields are unable to reorient the EMPs within the luminescence lifetime, implicating anisotropy in the EMP potential-energy surfaces. TRFR measurements in a transverse magnetic field reveal rapid (<5 ps) spin transfer from excitons to Mn(2+) followed by coherent EMP precession at the Mn(2+) Larmor frequency for over a nanosecond. A dynamical TRFR phase inversion is observed during EMP formation attributed to the large shifts in excitonic absorption energies during spontaneous magnetization. Partial optical orientation of the EMPs by resonant circularly polarized photoexcitation is also demonstrated. Collectively, these results highlight the extraordinary physical properties of colloidal diffusion-doped Cd(1-x)Mn(x)Se QDs that result from their unique combination of strong quantum confinement, large Mn(2+) concentrations, and relatively narrow size distributions. The insights gained from these measurements advance our understanding of spin dynamics and magnetic exchange in colloidal doped semiconductor nanostructures, with potential ramifications for future spin-based information technologies.