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106
result(s) for
"Brabec, Christoph J."
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Detection of X-ray photons by solution-processed lead halide perovskites
by
Stangl, Julian
,
Kriegner, Dominik
,
Azimi, Hamed
in
639/624/399
,
Applied and Technical Physics
,
Detectors
2015
The evolution of real-time medical diagnostic tools such as angiography and computer tomography from radiography based on photographic plates was enabled by the development of integrated solid-state X-ray photon detectors made from conventional solid-state semiconductors. Recently, for optoelectronic devices operating in the visible and near-infrared spectral regions, solution-processed organic and inorganic semiconductors have also attracted a great deal of attention. Here, we demonstrate a possibility to use such inexpensive semiconductors for the sensitive detection of X-ray photons by direct photon-to-current conversion. In particular, methylammonium lead iodide perovskite (CH
3
NH
3
PbI
3
) offers a compelling combination of fast photoresponse and a high absorption cross-section for X-rays, owing to the heavy Pb and I atoms. Solution-processed photodiodes as well as photoconductors are presented, exhibiting high values of X-ray sensitivity (up to 25 μC mGy
air
−1
cm
−3
) and responsivity (1.9 × 10
4
carriers/photon), which are commensurate with those obtained by the current solid-state technology.
Solid-state X-ray detectors have enabled real-time diagnostics as well as reduced patient dose. Now researchers have shown that potentially inexpensive perovskites can be used for efficient X-ray imaging.
Journal Article
High performance tandem organic solar cells via a strongly infrared-absorbing narrow bandgap acceptor
by
Li, Ning
,
Jia, Zhenrong
,
Zhang, Jinyuan
in
639/301/299/946
,
639/4077/909/4101/4096/946
,
639/638/298/398
2021
Tandem organic solar cells are based on the device structure monolithically connecting two solar cells to broaden overall absorption spectrum and utilize the photon energy more efficiently. Herein, we demonstrate a simple strategy of inserting a double bond between the central core and end groups of the small molecule acceptor Y6 to extend its conjugation length and absorption range. As a result, a new narrow bandgap acceptor BTPV-4F was synthesized with an optical bandgap of 1.21 eV. The single-junction devices based on BTPV-4F as acceptor achieved a power conversion efficiency of over 13.4% with a high short-circuit current density of 28.9 mA cm
−2
. With adopting BTPV-4F as the rear cell acceptor material, the resulting tandem devices reached a high power conversion efficiency of over 16.4% with good photostability. The results indicate that BTPV-4F is an efficient infrared-absorbing narrow bandgap acceptor and has great potential to be applied into tandem organic solar cells.
Development of tandem organic solar cells has been limited by the choice of near-infrared absorbing materials for the rear cell. Here, the authors report a simple strategy to extend the conjugation length of acceptor Y6 and broaden its absorption range to near-infrared region. A tandem organic solar cell with efficiency of 16.4% was achieved.
Journal Article
High-performance direct conversion X-ray detectors based on sintered hybrid lead triiodide perovskite wafers
2017
Lead halide perovskite semiconductors are in general known to have an inherently high X-ray absorption cross-section and a significantly higher carrier mobility than any other low-temperature solution-processed semiconductor. So far, the processing of several-hundred-micrometres-thick high-quality crystalline perovskite films over a large area has been unresolved for efficient X-ray detection. In this Article, we present a mechanical sintering process to fabricate polycrystalline methyl ammonium lead triiodide perovskite (MAPbI
3
) wafers with millimetre thickness and well-defined crystallinity. Benchmarking of the MAPbI
3
wafers against state-of-the-art CdTe detectors reveals competitive conversion efficiencies of 2,527 µC Gy
air
−1
cm
−2
under 70 kV
p
X-ray exposure. The high ambipolar mobility–lifetime product of 2 × 10
−4
cm
2
V
−1
is suggested to be responsible for this exceptionally high sensitivity. Our findings inform a new generation of highly efficient and low-cost X-ray detectors based on perovskite wafers.
Methyl ammonium lead triiodide perovskite wafers for application in direct conversion X-ray detectors are fabricated by a room-temperature sintering process. A conversion efficiency of 2,527 mC Gy
air
cm
–2
under 70 kVp X-ray exposure is obtained.
Journal Article
High-efficiency and air-stable P3HT-based polymer solar cells with a new non-fullerene acceptor
by
Durrant, James R.
,
Holliday, Sarah
,
Wadsworth, Andrew
in
140/125
,
639/301/299/946
,
639/624/1075/524
2016
Solution-processed organic photovoltaics (OPV) offer the attractive prospect of low-cost, light-weight and environmentally benign solar energy production. The highest efficiency OPV at present use low-bandgap donor polymers, many of which suffer from problems with stability and synthetic scalability. They also rely on fullerene-based acceptors, which themselves have issues with cost, stability and limited spectral absorption. Here we present a new non-fullerene acceptor that has been specifically designed to give improved performance alongside the wide bandgap donor poly(3-hexylthiophene), a polymer with significantly better prospects for commercial OPV due to its relative scalability and stability. Thanks to the well-matched optoelectronic and morphological properties of these materials, efficiencies of 6.4% are achieved which is the highest reported for fullerene-free P3HT devices. In addition, dramatically improved air stability is demonstrated relative to other high-efficiency OPV, showing the excellent potential of this new material combination for future technological applications.
In organic photovoltaics, the best performing devices usually involve low-bandgap polymers whose limited solubility and stability constrain the scalability of organic solar cells. Here, Holliday
et al
. develop a new acceptor and pair it with canonical P3HT to obtain 6.4% efficient and stable devices.
Journal Article
Abnormal strong burn-in degradation of highly efficient polymer solar cells caused by spinodal donor-acceptor demixing
2017
The performance of organic solar cells is determined by the delicate, meticulously optimized bulk-heterojunction microstructure, which consists of finely mixed and relatively separated donor/acceptor regions. Here we demonstrate an abnormal strong burn-in degradation in highly efficient polymer solar cells caused by spinodal demixing of the donor and acceptor phases, which dramatically reduces charge generation and can be attributed to the inherently low miscibility of both materials. Even though the microstructure can be kinetically tuned for achieving high-performance, the inherently low miscibility of donor and acceptor leads to spontaneous phase separation in the solid state, even at room temperature and in the dark. A theoretical calculation of the molecular parameters and construction of the spinodal phase diagrams highlight molecular incompatibilities between the donor and acceptor as a dominant mechanism for burn-in degradation, which is to date the major short-time loss reducing the performance and stability of organic solar cells.
Li
et al
. study degradation in organic photovoltaics from a morphological perspective. They find that donor and acceptor phases undergo excessive demixing via spinodal decomposition resulting in a reduction of charge generation. Demixing is due to the inherently low miscibility of both materials.
Journal Article
A generic interface to reduce the efficiency-stability-cost gap of perovskite solar cells
by
Li, Ning
,
Levchuk, Ievgen
,
Wang, Zhiping
in
Commercialization
,
Contact resistance
,
Current carriers
2017
A major bottleneck delaying the further commercialization of thin-film solar cells based on hybrid organohalide lead perovskites is interface loss in state-of-the-art devices. We present a generic interface architecture that combines solution-processed, reliable, and cost-efficient hole-transporting materials without compromising efficiency, stability, or scalability of perovskite solar cells. Tantalum-doped tungsten oxide (Ta-WOₓ)/conjugated polymer multilayers offer a surprisingly small interface barrier and form quasi-ohmic contacts universally with various scalable conjugated polymers. In a simple device with regular planar architecture and a self-assembled monolayer, Ta-WOₓ–doped interface–based perovskite solar cells achieve maximum efficiencies of 21.2% and offer more than 1000 hours of light stability. By eliminating additional ionic dopants, these findings open up the entire class of organics as scalable hole-transporting materials for perovskite solar cells.
Journal Article
Delocalization of exciton and electron wavefunction in non-fullerene acceptor molecules enables efficient organic solar cells
2020
A major challenge for organic solar cell (OSC) research is how to minimize the tradeoff between voltage loss and charge generation. In early 2019, we reported a non-fullerene acceptor (named Y6) that can simultaneously achieve high external quantum efficiency and low voltage loss for OSC. Here, we use a combination of experimental and theoretical modeling to reveal the structure-property-performance relationships of this state-of-the-art OSC system. We find that the distinctive π–π molecular packing of Y6 not only exists in molecular single crystals but also in thin films. Importantly, such molecular packing leads to (i) the formation of delocalized and emissive excitons that enable small non-radiative voltage loss, and (ii) delocalization of electron wavefunctions at donor/acceptor interfaces that significantly reduces the Coulomb attraction between interfacial electron-hole pairs. These properties are critical in enabling highly efficient charge generation in OSC systems with negligible donor-acceptor energy offset.
Y6, as a non-fullerene acceptor for organic solar cells, has attracted intensive attention because of the low voltage loss and high charge generation efficiency. Here, Zhang et al. find that the delocalization of exciton and electron wavefunction due to strong π-π packing of Y6 is the key for the high performance.
Journal Article
Robust nonfullerene solar cells approaching unity external quantum efficiency enabled by suppression of geminate recombination
by
Hamid, Zeinab
,
Durrant, James R.
,
Wadsworth, Andrew
in
140/125
,
639/301/1005/1007
,
639/4077/909/4101/4096/946
2018
Nonfullerene solar cells have increased their efficiencies up to 13%, yet quantum efficiencies are still limited to 80%. Here we report efficient nonfullerene solar cells with quantum efficiencies approaching unity. This is achieved with overlapping absorption bands of donor and acceptor that increases the photon absorption strength in the range from about 570 to 700 nm, thus, almost all incident photons are absorbed in the active layer. The charges generated are found to dissociate with negligible geminate recombination losses resulting in a short-circuit current density of 20 mA cm
−2
along with open-circuit voltages >1 V, which is remarkable for a 1.6 eV bandgap system. Most importantly, the unique nano-morphology of the donor:acceptor blend results in a substantially improved stability under illumination. Understanding the efficient charge separation in nonfullerene acceptors can pave the way to robust and recombination-free organic solar cells.
The nonfullerene-based small molecules start to attract more attention for solar cell research than the fullerene acceptors due to their wider tunability. Here Baran et al. demonstrate nonfullerene-based solar cells with high power conversion efficiency of 12% and quantum efficiencies approaching 100%.
Journal Article
Unraveling the influence of non-fullerene acceptor molecular packing on photovoltaic performance of organic solar cells
by
Chandrabose, Sreelakshmi
,
Zhou, Jiadong
,
Li, Ning
in
639/301/299/946
,
639/4077/4072/4062
,
Assembly
2020
In non-fullerene organic solar cells, the long-range structure ordering induced by end-group π–π stacking of fused-ring non-fullerene acceptors is considered as the critical factor in realizing efficient charge transport and high power conversion efficiency. Here, we demonstrate that side-chain engineering of non-fullerene acceptors could drive the fused-ring backbone assembly from a π–π stacking mode to an intermixed packing mode, and to a non-stacking mode to refine its solid-state properties. Different from the above-mentioned understanding, we find that close atom contacts in a non-stacking mode can form efficient charge transport pathway through close side atom interactions. The intermixed solid-state packing motif in active layers could enable organic solar cells with superior efficiency and reduced non-radiative recombination loss compared with devices based on molecules with the classic end-group π–π stacking mode. Our observations open a new avenue in material design that endows better photovoltaic performance.
Non-fullerene acceptors are crucial for realising efficient charge transport and high power conversion in organic solar cells, yet the relationship of molecular packing and carrier transport is not well-understood. Here, the authors study the effect of side-chain engineering on the backbone assembly and the corresponding charge transport pathway.
Journal Article
Discovery of temperature-induced stability reversal in perovskites using high-throughput robotic learning
by
Sun, Shijing
,
Li, Ning
,
Feng, Yexin
in
639/301/1005/1007
,
639/301/299/946
,
Accelerated aging tests
2021
Stability of perovskite-based photovoltaics remains a topic requiring further attention. Cation engineering influences perovskite stability, with the present-day understanding of the impact of cations based on accelerated ageing tests at higher-than-operating temperatures (e.g. 140°C). By coupling high-throughput experimentation with machine learning, we discover a weak correlation between high/low-temperature stability with a stability-reversal behavior. At high ageing temperatures, increasing organic cation (e.g. methylammonium) or decreasing inorganic cation (e.g. cesium) in multi-cation perovskites has detrimental impact on photo/thermal-stability; but below 100°C, the impact is reversed. The underlying mechanism is revealed by calculating the kinetic activation energy in perovskite decomposition. We further identify that incorporating at least 10 mol.% MA and up to 5 mol.% Cs/Rb to maximize the device stability at device-operating temperature (<100°C). We close by demonstrating the methylammonium-containing perovskite solar cells showing negligible efficiency loss compared to its initial efficiency after 1800 hours of working under illumination at 30°C.
Current view of the impact of A-site cation on the stability of perovskite materials and devices is derived from accelerated ageing tests at high temperature, which is beyond normal operation range. Here, the authors reveal the great impact of ageing condition on assessing the photothermal stability of mixed-cation perovskites using high-throughput robot system coupled with machine learning.
Journal Article