Tõnu Pullerits

Bio: Tõnu Pullerits is an academic researcher from Lund University. The author has contributed to research in topics: Quantum dot & Exciton. The author has an hindex of 61, co-authored 268 publications receiving 14013 citations. Previous affiliations of Tõnu Pullerits include VU University Amsterdam & Estonian Academy of Sciences.

Organometal Halide Perovskite Solar Cell Materials Rationalized: Ultrafast Charge Generation, High and Microsecond-Long Balanced Mobilities, and Slow Recombination

Abstract: Organometal halide perovskite-based solar cells have recently been reported to be highly efficient, giving an overall power conversion efficiency of up to 15%. However, much of the fundamental photophysical properties underlying this performance has remained unknown. Here, we apply photoluminescence, transient absorption, time-resolved terahertz and microwave conductivity measurements to determine the time scales of generation and recombination of charge carriers as well as their transport properties in solution-processed CH3NH3PbI3 perovskite materials. We found that electron–hole pairs are generated almost instantaneously after photoexcitation and dissociate in 2 ps forming highly mobile charges (25 cm2 V–1 s–1) in the neat perovskite and in perovskite/alumina blends; almost balanced electron and hole mobilities remain very high up to the microsecond time scale. When the perovskite is introduced into a TiO2 mesoporous structure, electron injection from perovskite to the metal oxide is efficient in less ...

Photosynthetic light-harvesting: Reconciling dynamics and structure of purple bacterial LH2 reveals function of photosynthetic unit

Abstract: Great progress in the study of structure and dynamics of photosynthetic light-harvesting pigment−protein complexes has recently resulted in detailed understanding of the light-harvesting and light-...

Thermally Activated Exciton Dissociation and Recombination Control the Carrier Dynamics in Organometal Halide Perovskite

Abstract: Solar cells based on organometal halide perovskites have seen rapidly increasing efficiencies, now exceeding 15%. Despite this progress, there is still limited knowledge on the fundamental photophysics. Here we use microwave photoconductance and photoluminescence measurements to investigate the temperature dependence of the carrier generation, mobility, and recombination in (CH3NH3)PbI3. At temperatures maintaining the tetragonal crystal phase of the perovskite, we find an exciton binding energy of about 32 meV, leading to a temperature-dependent yield of highly mobile (6.2 cm(2)/(V s) at 300 K) charge carriers. At higher laser intensities, second-order recombination with a rate constant of γ = 13 × 10(-10) cm(3) s(-1) becomes apparent. Reducing the temperature results in increasing charge carrier mobilities following a T(-1.6) dependence, which we attribute to a reduction in phonon scattering (Σμ = 16 cm(2)/(V s) at 165 K). Despite the fact that Σμ increases, γ diminishes with a factor six, implying that charge recombination in (CH3NH3)PbI3 is temperature activated. The results underline the importance of the perovskite crystal structure, the exciton binding energy, and the activation energy for recombination as key factors in optimizing new perovskite materials.

Lead-Free, Air-Stable All-Inorganic Cesium Bismuth Halide Perovskite Nanocrystals

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 560 nm 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 (2–20 ps). Notably, the trap states can also be passivated under humid conditions, and the NCs exhibited high stability towards air exposure exceeding 30 days.

Origin of long-lived coherences in light-harvesting complexes.

Abstract: A vibronic exciton model is applied to explain the long-lived oscillatory features in the two-dimensional (2D) electronic spectra of the Fenna–Matthews–Olson (FMO) complex. Using experimentally determined parameters and uncorrelated site energy fluctuations, the model predicts oscillations with dephasing times of 1.3 ps at 77 K, which is in a good agreement with the experimental results. These long-lived oscillations originate from the coherent superposition of vibronic exciton states with dominant contributions from vibrational excitations on the same pigment. The oscillations obtain a large amplitude due to excitonic intensity borrowing, which gives transitions with strong vibronic character a significant intensity despite the small Huang–Rhys factor. Purely electronic coherences are found to decay on a 200 fs time scale.

疟原虫var基因转换速率变化导致抗原变异[英]／Paul H, Robert P, Christodoulou Z, et al//Proc Natl Acad Sci U S A

Abstract: 抗原变异可使得多种致病微生物易于逃避宿主免疫应答。表达在感染红细胞表面的恶性疟原虫红细胞表面蛋白1（PfPMP1）与感染红细胞、内皮细胞、树突状细胞以及胎盘的单个或多个受体作用，在黏附及免疫逃避中起关键的作用。每个单倍体基因组var基因家族编码约60种成员，通过启动转录不同的var基因变异体为抗原变异提供了分子基础。

Interface engineering of highly efficient perovskite solar cells

Abstract: Advancing perovskite solar cell technologies toward their theoretical power conversion efficiency (PCE) requires delicate control over the carrier dynamics throughout the entire device. By controlling the formation of the perovskite layer and careful choices of other materials, we suppressed carrier recombination in the absorber, facilitated carrier injection into the carrier transport layers, and maintained good carrier extraction at the electrodes. When measured via reverse bias scan, cell PCE is typically boosted to 16.6% on average, with the highest efficiency of ~19.3% in a planar geometry without antireflective coating. The fabrication of our perovskite solar cells was conducted in air and from solution at low temperatures, which should simplify manufacturing of large-area perovskite devices that are inexpensive and perform at high levels.

Stochastic Processes in Physics and Chemistry

Abstract: N G van Kampen 1981 Amsterdam: North-Holland xiv + 419 pp price Dfl 180 This is a book which, at a lower price, could be expected to become an essential part of the library of every physical scientist concerned with problems involving fluctuations and stochastic processes, as well as those who just enjoy a beautifully written book. It provides an extensive graduate-level introduction which is clear, cautious, interesting and readable.

Semiconducting π-conjugated systems in field-effect transistors: a material odyssey of organic electronics.

Abstract: Since the discovery of highly conducting polyacetylene by Shirakawa, MacDiarmid, and Heeger in 1977, π-conjugated systems have attracted much attention as futuristic materials for the development and production of the next generation of electronics, that is, organic electronics. Conceptually, organic electronics are quite different from conventional inorganic solid state electronics because the structural versatility of organic semiconductors allows for the incorporation of functionality by molecular design. This versatility leads to a new era in the design of electronic devices. To date, the great number of π-conjugated semiconducting materials that have either been discovered or synthesized generate an exciting library of π-conjugated systems for use in organic electronics. 11 However, some key challenges for further advancement remain: the low mobility and stability of organic semiconductors, the lack of knowledge regarding structure property relationships for understanding the fundamental chemical aspects behind the structural design, and realization of desired properties. Organic field-effect transistors (OFETs) are a kind of device consisting of an organic semiconducting layer, a gate insulator layer, and three terminals (drain, source, and gate electrodes). OFETs are not only essential building blocks for the next generation of cheap and flexible organic circuits, but they also provide an important insight into the charge transport of πconjugated systems. Therefore, they act as strong tools for the exploration of the structure property relationships of πconjugated systems, such as parameters of field-effect mobility (μ, the drift velocity of carriers under unit electric field), current on/off ratio (the ratio of the maximum on-state current to the minimum off-state current), and threshold voltage (the minimum gate voltage that is required to turn on the transistor). 17 Since the discovery of OFETs in the 1980s, they have attracted much attention. Research onOFETs includes the discovery, design, and synthesis of π-conjugated systems for OFETs, device optimization, development of applications in radio frequency identification (RFID) tags, flexible displays, electronic papers, sensors, and so forth. It is beyond the scope of this review to cover all aspects of π-conjugated systems; hence, our focus will be on the performance analysis of π-conjugated systems in OFETs. This should make it possible to extract information regarding the fundamental merit of semiconducting π-conjugated materials and capture what is needed for newmaterials and what is the synthesis orientation of newπ-conjugated systems. In fact, for a new science with many practical applications, the field of organic electronics is progressing extremely rapidly. For example, using “organic field effect transistor” or “organic field effect transistors” as the query keywords to search the Web of Science citation database, it is possible to show the distribution of papers over recent years as shown in Figure 1A. It is very clear

A hole-conductor-free, fully printable mesoscopic perovskite solar cell with high stability

Abstract: We fabricated a perovskite solar cell that uses a double layer of mesoporous TiO2 and ZrO2 as a scaffold infiltrated with perovskite and does not require a hole-conducting layer. The perovskite was produced by drop-casting a solution of PbI2, methylammonium (MA) iodide, and 5-ammoniumvaleric acid (5-AVA) iodide through a porous carbon film. The 5-AVA templating created mixed-cation perovskite (5-AVA)x(MA)1- xPbI3 crystals with lower defect concentration and better pore filling as well as more complete contact with the TiO2 scaffold, resulting in a longer exciton lifetime and a higher quantum yield for photoinduced charge separation as compared to MAPbI3. The cell achieved a certified power conversion efficiency of 12.8% and was stable for >1000 hours in ambient air under full sunlight.