25 research outputs found

    Accumulation effects in modulation spectroscopy with high repetition rate pulses: recursive solution of optical Bloch equations

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    Application of the phase modulated pulsed light for advance spectroscopic measurements is the area of growing interest. The phase modulation of the light causes modulation of the signal. Separation of the spectral components of the modulations allows to distinguish the contributions of various interaction pathways. The lasers with high repetition rate used in such experiments can lead to appearance of the accumulation effects, which become especially pronounced in systems with long-living excited states. Recently it was shown, that such accumulation effects can be used to evaluate parameters of the dynamical processes in the material. In this work we demonstrate that the accumulation effects are also important in the quantum characteristics measurements provided by modulation spectroscopy. In particular, we consider a model of quantum two-level system driven by a train of phase-modulated light pulses, organised in analogy with the 2D spectroscopy experiments. We evaluate the harmonics' amplitudes in the fluorescent signal and calculate corrections appearing from the accumulation effects. We show that the corrections can be significant and have to be taken into account at analysis of experimental data.Comment: 10 pages, 5 figure

    Digital Cavities and Their Potential Applications

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    The concept of a digital cavity is presented. The functionality of a tunable radio-frequency/microwave cavity with unrestricted Q-factor is implemented. The theoretical aspects of the cavity and its potential applications in high resolution spectroscopy and synchronization of clocks together with examples in signal processing and data acquisition are discussed

    Beating signals in CdSe quantum dots measured by low-temperature 2D spectroscopy

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    Advances in ultrafast spectroscopy can provide access to dynamics involving nontrivial quantum correlations and their evolutions. In coherent 2D spectroscopy, the oscillatory time dependence of a signal is a signature of such quantum dynamics. Here we study such beating signals in electronic coherent 2D spectroscopy of CdSe quantum dots (CdSe QDs) at 77 K. The beating signals are analyzed in terms of their positive and negative Fourier components. We conclude that the beatings originate from coherent LO-phonons of CdSe QDs. No evidence for the quantum dot size dependence of the LO-phonon frequency was identified.Comment: 18 page

    Sandwiched confinement of quantum dots in graphene matrix for efficient electron transfer and photocurrent production

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    Quantum dots (QDs) and graphene are both promising materials for the development of new-generation optoelectronic devices. Towards this end, synergic assembly of these two building blocks is a key step but remains a challenge. Here, we show a one-step strategy for organizing QDs in a graphene matrix via interfacial self-assembly, leading to the formation of sandwiched hybrid QD-graphene nanofilms. We have explored structural features, electron transfer kinetics and photocurrent generation capacity of such hybrid nanofilms using a wide variety of advanced techniques. Graphene nanosheets interlink QDs and significantly improve electronic coupling, resulting in fast electron transfer from photoexcited QDs to graphene with a rate constant of 1.3 √ó 10(9) s(-1). Efficient electron transfer dramatically enhances photocurrent generation in a liquid-junction QD-sensitized solar cell where the hybrid nanofilm acts as a photoanode. We thereby demonstrate a cost-effective method to construct large-area QD-graphene hybrid nanofilms with straightforward scale-up potential for optoelectronic applications

    Cation-Dependent Hot Carrier Cooling in Halide Perovskite Nanocrystals

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    Lead halide perovskites (LHPs) nanocrystals (NCs), owing to their outstanding photophysical properties, have recently emerged as a promising material not only for solar cells but also for lighting and display applications. The photophysical properties of these materials can be further improved by chemical engineering such as cation exchange. Hot carrier (HC) cooling, as one of the key photophysical processes in LHPs, can strongly influence performance of LHPs NCs based devices. Here, we study HC relaxation dynamics in LHP NCs with cesium (Cs), methylammonium (MA, CH 3 NH 3 + ), and formamidinium (FA, CH(NH 2 ) 2 + ) cations by using femtosecond transient absorption spectroscopy. The LHP NCs show excitation intensity and excitation energy-dependent HC cooling. We investigate the details of HC cooling in CsPbBr 3 , MAPbBr 3 , and FAPbBr 3 at three different excitation energies with low excitation intensity. It takes longer time for the HCs at high energy to relax (cool) to the band edge, compared to the HCs generated by low excitation energy. At the same excitation energy (350 nm, 3.54 eV), all the three LHP NCs show fast HC relaxation ( MAPbBr 3 (0.27 ps, 4.6 meV/fs) > FAPbBr 3 (0.21 ps, 5.8 meV/fs). The cation dependence can be explained by stronger interaction between the organic cations with the Pb-Br frameworks compared to the Cs. The revealed cation-dependent HC relaxation process is important for providing cation engineering strategies for developing high performance LHP devices

    Optimizing ZnO nanoparticle surface for bulk heterojunction hybrid solar cells

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    The performance of hybrid solar cells composed of polymer and ZnO is mainly hindered by the defects of ZnO. Here, we investigate the effects of ZnO nanoparticle surface modification with poly(ethylene oxide) (PEO) on the performance of bulk heterojunction hybrid solar cells based on poly[2-methoxy-5-(2′-ethyl-hexyloxy)-1,4-phenylene vinylene] (MEH-PPV) and ZnO nanoparticles. The reference device using ZnO nanoparticles as electron acceptor shows an open-circuit voltage (VOC) of 0.83 V, a short-circuit current (JSC) of 3.00 mA/cm2, a fill factor (FF) of 0.46 and a power conversion efficiency (PCE) of 1.15%. After modification with very small amount of PEO, the PCE will be enhanced, which is attributed to less surface traps of ZnO nanoparticles with PEO modification. With optimized PEO (0.05%) modified ZnO nanoparticles as electron acceptors, the device typically shows a VOC of 0.86 V, a JSC of 3.84 mA/cm2, a FF of 0.51 and a PCE of 1.68% due to less recombination loss of carriers, smaller series resistance, and improved electrical coupling between ZnO nanoparticle and MEH-PPV. However, further increase of PEO content to 0.3% will deteriorate device performance.Funding Agencies|Swedish energy agency (Energimyndigheten)||Swedish Research Council (VR)||Knut, Alice Wallenberg Foundation||Crafoord foundation||VINNOVA||</p

    High carrier mobility in low band gap polymer-based field-effect transistors

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    A conjugated polymer with a low band gap of 1.21 eV, i.e., absorbing IR light, is demonstrated as active material in field-effect transistors (FETs). The material consists of alternating fluorene units and low band gap segments with electron donor-acceptor-donor units composed of two electron-donating thiophene rings attached on both sides of a thiadiazolo-quinoxaline electron-acceptor group. The polymer is soln.-processable and air-stable; the resulting FETs exhibit typical p-channel characteristics and field-effect mobility of 0.03 cm2 V-1 s-1. [on SciFinder (R)

    Plasmon-exciton coupling of monolayer MoS2-Ag nanoparticles hybrids for surface catalytic reaction

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    The optical properties of monolayer molybdenum disulfide (MoS2)/Ag nanoparticle (NP) hybrids and their application to surface catalytic reactions were studied by transmission, photoluminescence (PL) and Raman spectroscopies. The local surface plasmon resonance (LSPR) of Ag nanoparticles was tuned to better match the exciton energy of monolayer MoS2. The PL of the hybrids was enhanced by more than 50 times when the local surface plasmon resonance (LSPR) peak was tuned systematically from 438 nm to 532 nm, indicating a stronger coupling and higher energy transfer rate between the plasmon of the Ag NPs and the excitons of the MoS2. Additionally, photocatalytic reactions of 4-nitrobenzenethiol (4NBT) were performed on the MoS2, the Ag nanoparticles, and the hybrid MoS2 with Ag nanoparticles. On the MoS2 substrate alone, there is no photocatalytic reaction. With a low laser intensity, the probability of a chemical reaction occurring for molecules directly adsorbed onto the Ag NPs is much lower than the probability of a reaction involving those molecules adsorbed onto the MoS2/Ag substrate. At a higher power, although the electric field was reduced by approximately 30% by the MoS2 layer, there is better efficiency for the plasmon-exciton co-driven surface catalytic reactions on the MoS2/Ag substrate compared to the Ag substrate alone. Our findings illustrate the potential to control hot carriers for better surface catalytic reactions by tuning the exciton-plasmon coupling between the 2D transition metal dichalcogenides (TMDCs) and Ag NPs

    Light-Induced Defect Healing and Strong Many-Body Interactions in Formamidinium Lead Bromide Perovskite Nanocrystals

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    Organic lead halide perovskite (OLHP) nanocrystals (NCs) have paved the way to advanced optoelectronic devices through their extraordinary electrical and optical properties. However, understanding of the light-induced complex dynamic phenomena in OLHP NCs remains a subject of debate. Here we used wide field microscopy and time-resolved spectroscopy to correlate the local changes in photophysics and the dynamical behavior of photocarriers. We demonstrate that light-induced brightening of the photoluminescence from the formamidinium lead bromide NC films is related to the film preparation condition and reduction of trap density. The density of trap states is reduced via halide ion migration from interstitial position. Our femtosecond transient absorption study identifies transient Stark effect due to the generation of hot carriers. Because of slow carrier trapping, Auger recombination through many-body carrier-carrier interactions dominates over trion recombination. This work presents unprecedented insights into the light-driven processes enabling better device design in the future.status: publishe