| 1. |
- Abdellah, Mohamed, et al.
(författare)
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Drastic difference between hole and electron injection through the gradient shell of CdxSeyZn1−xS1−y quantum dots
- 2017
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Ingår i: Nanoscale. - : Royal Society of Chemistry (RSC). - 2040-3364 .- 2040-3372. ; 9:34, s. 12503-12508
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Tidskriftsartikel (refereegranskat)abstract
- Ultrafast fluorescence spectroscopy was used to investigate the hole injection in CdxSeyZn1-xS1-y gradient core-shell quantum dot (CSQD) sensitized p-type NiO photocathodes. A series of CSQDs with a wide range of shell thicknesses was studied. Complementary photoelectrochemical cell measurements were carried out to confirm that the hole injection from the active core through the gradient shell to NiO takes place. The hole injection from the valence band of the QDs to NiO depends much less on the shell thickness when compared to the corresponding electron injection to n-type semiconductor (ZnO). We simulate the charge carrier tunneling through the potential barrier due to the gradient shell by numerically solving the Schrodinger equation. The details of the band alignment determining the potential barrier are obtained from X-ray spectroscopy measurements. The observed drastic differences between the hole and electron injection are consistent with a model where the hole effective mass decreases, while the gradient shell thickness increases.
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| 2. |
- Chen, Junsheng, et al.
(författare)
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Enhanced Size Selection in Two-Photon Excitation for CsPbBr3 Perovskite Nanocrystals
- 2017
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Ingår i: Journal of Physical Chemistry Letters. - : American Chemical Society (ACS). - 1948-7185. ; 8:20, s. 5119-5124
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Tidskriftsartikel (refereegranskat)abstract
- Cesium lead bromide (CsPbBr3) perovskite nanocrystals (NCs), with large two-photon absorption (TPA) cross-section and bright photoluminescence (PL), have been demonstrated as stable two-photon-pumped lasing medium. With two-photon excitation, red-shifted PL spectrum and increased PL lifetime is observed compared with one-photon excitation. We have investigated the origin of such difference using time-resolved laser spectroscopies. We ascribe the difference to the enhanced size selection of NCs by two-photon excitation. Because of inherent nonlinearity, the size dependence of absorption cross-section under TPA is stronger. Consequently, larger size NCs are preferably excited, leading to longer excited-state lifetime and red-shifted PL emission. In a broad view, the enhanced size selection in two-photon excitation of CsPbBr3 NCs is likely a general feature of the perovskite NCs and can be tuned via NC size distribution to influence their performance within NC-based nonlinear optical materials and devices.
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| 3. |
- Chen, Junsheng, et al.
(författare)
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Photostability of the Oleic Acid-Encapsulated Water-Soluble CdxSeyZn1-xS1-y Gradient Core-Shell Quantum Dots
- 2017
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Ingår i: ACS Omega. - : American Chemical Society (ACS). - 2470-1343. ; 2:5, s. 1922-1929
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Tidskriftsartikel (refereegranskat)abstract
- Composite systems where quantum dots (QDs) are combined with other nanomaterials (e.g., gold nanorods) in aqueous solutions have attracted broad attention - both for their potential in applications and for studies of fundamental processes. However, high-quality QDs are typically prepared in organic solvents, and the transfer of QDs to an aqueous phase is needed to create the desired QD composites. Photostability of the transferred QDs - both the steady-state and photo-induced dynamic properties - is essential for studying the processes in the composites and for their applications. We present a detailed study of the photostability of aqueous CdxSeyZn1-xS1-y gradient core-shell QDs obtained by various approaches using linker exchange and surfactant encapsulation. Beside the steady-state photoluminescence (PL) emission stability, we also study changes in the PL decay. From the variety of the studied samples, the water-soluble QDs encapsulated by a double layer of oleic acid show superior properties, that is, stable PL emission and PL decay under continuous light or pulsed-laser light irradiation. We demonstrate that the double-layer encapsulation of QDs can be used to create QDs-metal nanoparticle composites.
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| 4. |
- Chen, Junsheng, et al.
(författare)
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Size-And Wavelength-Dependent Two-Photon Absorption Cross-Section of CsPbBr3 Perovskite Quantum Dots
- 2017
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Ingår i: Journal of Physical Chemistry Letters. - : American Chemical Society (ACS). - 1948-7185. ; 8:10, s. 2316-2321
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Tidskriftsartikel (refereegranskat)abstract
- All-inorganic colloidal perovskite quantum dots (QDs) based on cesium, lead, and halide have recently emerged as promising light emitting materials. CsPbBr3 QDs have also been demonstrated as stable two-photon-pumped lasing medium. However, the reported two photon absorption (TPA) cross sections for these QDs differ by an order of magnitude. Here we present an in-depth study of the TPA properties of CsPbBr3 QDs with mean size ranging from 4.6 to 11.4 nm. By using femtosecond transient absorption (TA) spectroscopy we found that TPA cross section is proportional to the linear one photon absorption. The TPA cross section follows a power law dependence on QDs size with exponent 3.3 ± 0.2. The empirically obtained power-law dependence suggests that the TPA process through a virtual state populates exciton band states. The revealed power-law dependence and the understanding of TPA process are important for developing high performance nonlinear optical devices based on CsPbBr3 nanocrystals.
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| 5. |
- Chen, Yani, et al.
(författare)
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Tailoring Organic Cation of 2D Air-Stable Organometal Halide Perovskites for Highly Efficient Planar Solar Cells
- 2017
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Ingår i: Advanced Energy Materials. - : Wiley. - 1614-6832. ; 7:18
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Tidskriftsartikel (refereegranskat)abstract
- 2D perovskites have recently been shown to exhibit significantly improved environmental stability. Derived from their 3D analogues, 2D perovskites are formed by inserting bulky alkylammonium cations in-between the anionic layers. However, these insulating organic spacer cations also hinder charge transport. Herein, such a 2D perovskite, (iso-BA)2(MA)3Pb4I13, that contains short branched-chain spacer cations (iso-BA+) and shows a remarkable increase of optical absorption and crystallinity in comparison to the conventional linear one, n-BA+, is designed. After applying the hot-casting (HC) technique, all these properties are further improved. The HC (iso-BA)2(MA)3Pb4I13 sample exhibits the best ambient stability by maintaining its initial optical absorption after storage of 840 h in an environmental chamber at 20 °C with a relative humidity of 60% without encapsulation. More importantly, the out-of-plane crystal orientation of (iso-BA)2(MA)3Pb4I13 film is notably enhanced, which increases cross-plane charge mobility. As a result, the highest power conversion efficiencies (PCEs) measured from for current density versus voltage curves afford 8.82% and 10.63% for room-temperature and HC-processed 2D perovskites based planar solar cells, respectively. However, the corresponding steady-state PCEs are remarkably lower, which is presumably due to the significant hysteresis phenomena caused by low charge extraction efficiency at interfaces of C60/2D perovskites.
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| 6. |
- Damtie, Fikeraddis A., et al.
(författare)
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Two-dimensional action spectroscopy of excitonic systems : Explicit simulation using a phase-modulation technique
- 2017
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Ingår i: Physical Review A. - 2469-9926. ; 96:5
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Tidskriftsartikel (refereegranskat)abstract
- Two-dimensional (2D) spectroscopy has been intensively used to study electronic and vibronic coherences in biological systems and semiconductors. This technique studies coherent as well as incoherent signals that arise from the nonlinear interaction of a sequence of laser pulses. In this paper we present a direct evaluation of the 2D signal based on elementary quantum kinetics in order to compare with the common approximate diagrammatic approaches. Here we consider incoherent action signals such as fluorescence or photocurrent as the observable, which is easily accessible in a measurement. These observables are calculated by solving the time evolution of the density matrix in the Lindblad form, which can take into account all possible decoherence processes. The phase modulation technique is used to separate the relevant nonlinear signals from the other possible interaction pathways. The approach can be used to calculate 2D spectra of any quantum system. For our model system we find a good agreement for the quantum beating between the coupled states.
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| 7. |
- Osipov, Vladimir Al, et al.
(författare)
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Accumulation effects in modulation spectroscopy with high-repetition-rate pulses : Recursive solution of optical Bloch equations
- 2017
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Ingår i: Physical Review A. - 2469-9926. ; 96:4
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Tidskriftsartikel (refereegranskat)abstract
- 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, organized in analogy with the two-dimensional 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.
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| 8. |
- Peng, Jiajun, et al.
(författare)
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Insights into charge carrier dynamics in organo-metal halide perovskites : From neat films to solar cells
- 2017
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Ingår i: Chemical Society Reviews. - : Royal Society of Chemistry (RSC). - 0306-0012 .- 1460-4744. ; 46:19, s. 5714-5729
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Forskningsöversikt (refereegranskat)abstract
- Organo-metal halide perovskites have recently obtained world-wide attention as promising solar cell materials. They have broad and strong light absorption along with excellent carrier transport properties which partially explain their record power conversion efficiencies above 22%. However, the basic understanding of the underlying physical mechanisms is still limited and there remain large discrepancies among reported transport characteristics of perovskite materials. Notably, the carrier mobility of perovskite samples either in thin films or within solar cells obtained using different techniques can vary by up to 7-8 orders of magnitude. This tutorial review aims to offer insights into the scope, advantages, limitations and latest developments of the techniques that have been applied for studying charge carrier dynamics in perovskites. We summarize a comprehensive set of measurements including (1) time-resolved laser spectroscopies (transient absorption, time-resolved photoluminescence, terahertz spectroscopy and microwave conductivity); (2) electrical transient techniques (charge extraction by linearly increasing voltage and time-of-flight); and (3) steady-state methods (field-effect transistor, Hall effect and space charge limited current). Firstly, the basics of the above measurements are described. We then comparatively summarize the charge carrier characteristics of perovskite-based neat films, bilayer films and solar cells. Finally, we compare the different approaches in evaluating the key parameters of transport dynamics and unravel the reasons for the large discrepancies among these methods. We anticipate that this tutorial review will serve as the entry point for understanding the experimental results from the above techniques and provide insights into charge carrier dynamics in perovskite materials and devices.
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| 9. |
- Yang, B, et al.
(författare)
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Lead-Free, Air-Stable All-Inorganic Cesium Bismuth Halide Perovskite Nanocrystals
- 2017
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Ingår i: Angewandte Chemie - International Edition. - : Wiley. - 1433-7851 .- 1521-3773. ; 56:41, s. 12471-12475
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Tidskriftsartikel (refereegranskat)abstract
- Lead-based perovskite nanocrystals (NCs) have outstanding optical properties and cheap synthesis conferring them a tremendous potential in the field of optoelectronic devices. However, two critical problems are still unresolved and hindering their commercial applications: one is the fact of being lead-based and the other is the poor stability. Lead-free all-inorganic perovskite Cs3Bi2X9 (X=Cl, Br, I) NCs are synthesized with emission wavelength ranging from 400 to 560nm synthesized by a facile room temperature reaction. The ligand-free Cs3Bi2Br9 NCs exhibit blue emission with photoluminescence quantum efficiency (PLQE) about 0.2%. The PLQE can be increased to 4.5% when extra surfactant (oleic acid) is added during the synthesis processes. This improvement stems from passivation of the fast trapping process (2-20ps). Notably, the trap states can also be passivated under humid conditions, and the NCs exhibited high stability towards air exposure exceeding 30days.
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| 10. |
- Yang, B, et al.
(författare)
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Ultrasensitive and Fast All-Inorganic Perovskite-Based Photodetector via Fast Carrier Diffusion
- 2017
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Ingår i: Advanced Materials. - : Wiley. - 0935-9648. ; 29:40, s. 1703758-1703758
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Tidskriftsartikel (refereegranskat)abstract
- Low trap-state density, high carrier mobility, and efficient charge carrier collection are key parameters for photodetectors with high sensitivity and fast response time. This study demonstrates a simple solution growth method to prepare CsPbBr3 microcrystals (MCs) with low trap-state density. Time-dependent photoluminescence study with one-photon excitation (OPE) and two-photon excitation (TPE) indicates that CsPbBr3 MCs exhibit fast carrier diffusion with carrier mobility over 100 cm2 V-1 S-1. Furthermore, CsPbBr3 MC-based photodetectors with high charge carriers' collection efficiency are fabricated. Such photodetectors show ultrahigh responsivity (R) up to 6 × 104 A W-1 with OPE and high R up to 6 A W-1 with TPE. The R for OPE is over one order of magnitude higher (the R for TPE is three orders of magnitude higher) than that of previously reported all-inorganic perovskite-based photodetectors. Moreover, the photodetectors exhibit fast response time of ≈1 ms, which corresponds to a gain ≈105 and a gain- bandwidth product of 108 Hz for OPE (a gain ≈103 and a gain-bandwidth product of 106 Hz for TPE).
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