Fluorination or Not in Small Molecule Solar Cells: Achieving a Higher Efficiency with Halogen-free End Group.

Fluorination is an efficient strategy for improving organic solar cells (OSCs) efficiency, particularly by fluorinating the end group of emerging nonfullerene acceptors. Here, the fluorination effect was investigated by using small molecule donors with fluorine-free (SBz) and fluorinated (SBz-F) end groups, paired with the emerging nonfullerene acceptor Y6. Interestingly and unexpectedly, fluorination of the end group negatively affects OSCs efficiency, with fluorine-free SBz:Y6 OSCs achieving a higher power conversion efficiency (PCE) of 11.05% compared to the fluorine-containing SBz-F:Y6 blends (PCE = 9.61%). Analysis of space-charge limited currents reveals lower and unbalanced hole/electron mobility in SBz-F:Y6 compared to the SBz:Y6 blends. These findings are further supported by charge recombination dynamics and donor-acceptor miscibility analyses.

Ultrafast and Electrically Tunable Rabi Frequency in a Germanium Hut Wire Hole Spin Qubit.

Hole spin qubits based on germanium (Ge) have strong tunable spin-orbit interaction (SOI) and ultrafast qubit operation speed. Here we report that the Rabi frequency (fRabi) of a hole spin qubit in a Ge hut wire (HW) double quantum dot (DQD) is electrically tuned through the detuning energy (ϵ) and middle gate voltage (VM). fRabi gradually decreases with increasing ϵ; on the contrary, fRabi is positively correlated with VM. We attribute our results to the change of electric field on SOI and the contribution of the excited state in quantum dots to fRabi. We further demonstrate an ultrafast fRabi exceeding 1.2 GHz, which indicates the strong SOI in our device. The discovery of an ultrafast and electrically tunable fRabi in a hole spin qubit has potential applications in semiconductor quantum computing.

Theoretical Design of Tellurium-Based Two-Dimensional Perovskite Photovoltaic Materials.

In recent years, the photoelectric conversion efficiency of three-dimensional (3D) perovskites has seen significant improvements. However, the commercial application of 3D perovskites is hindered by stability issues and the toxicity of lead. Two-dimensional (2D) perovskites exhibit good stability but suffer from low efficiency. Designing efficient and stable lead-free 2D perovskite materials remains a crucial unsolved scientific challenge. This study, through structural prediction combined with first-principles calculations, successfully predicts a 2D perovskite, CsTeI5. Theoretical calculations indicate that this compound possesses excellent stability and a theoretical efficiency of up to 29.3%, showing promise for successful application in thin-film solar cells. This research provides a new perspective for the design of efficient and stable lead-free 2D perovskites.

Stability of H3O at extreme conditions and implications for the magnetic fields of Uranus and Neptune.

The anomalous nondipolar and nonaxisymmetric magnetic fields of Uranus and Neptune have long challenged conventional views of planetary dynamos. A thin-shell dynamo conjecture captures the observed phenomena but leaves unexplained the fundamental material basis and underlying mechanism. Here we report extensive quantum-mechanical calculations of polymorphism in the hydrogen-oxygen system at the pressures and temperatures of the deep interiors of these ice giant planets (to >600 GPa and 7,000 K). The results reveal the surprising stability of solid and fluid trihydrogen oxide (H3O) at these extreme conditions. Fluid H3O is metallic and calculated to be stable near the cores of Uranus and Neptune. As a convecting fluid, the material could give rise to the magnetic field consistent with the thin-shell dynamo model proposed for these planets. H3O could also be a major component in both solid and superionic forms in other (e.g., nonconvecting) layers. The results thus provide a materials basis for understanding the enigmatic magnetic-field anomalies and other aspects of the interiors of Uranus and Neptune. These findings have direct implications for the internal structure, composition, and dynamos of related exoplanets.

Intravenous insulin preparation administration for myocardial viability 18F-FDG imaging has the potential to reduce radiation exposure dose.

OBJECTIVE: Fluorine-18-fluorodeoxyglucose (18F-FDG) injection activity is positively associated with radiation dose and positron emission tomography (PET) image count. Measurement error is greater with smaller counts; therefore, precise analysis is needed to avoid high doses of radiation exposure caused by high 18F-FDG injection. We aimed to identify and validate the optimal 18F-FDG injection activity and acquisition time for cardiac viability imaging with intravenous insulin preparation administration based on fixed 18F-FDG activity. MATERIALS AND METHODS: Cardiac PET images from 30 patients with coronary artery disease (CAD) were retrospectively reconstructed into different durations. An optimal product of the maximum standardized uptake value (SUV) of the myocardium, and segmental uptake (SU), and acquisition time (MSAT) was determined through a receiver operating characteristic curve. RESULTS: The optimal acquisition time (OAT) was equal to MSAT divided by mean SUV of the myocardium (MyoSUV) and was validated in another 26 patients with CAD. The optimal MSAT was 848.2s. In the validation group, the OAT was 129±76s (95% confidence interval, 99-160s), approximately one-third of the usual acquisition time. The MyoSUV and SU were equivalent between PET image duration of OAT and 600s (7.71±3.01 vs. 7.56±2.94; 67.1±15.4% vs. 67.7±15.6%). CONCLUSION: Intravenous insulin preparation administration has the potential to decrease the radiation exposure or acquisition time in cardiac viability 18F-FDG imaging to one-third, without losing the accurate measurement of MyoSUV or SU when reaching an OAT.

Valley Phase and Voltage Control of Coherent Manipulation in Si Quantum Dots.

With any roughness at the interface of an indirect-bandgap semiconducting dot, the phase of the valley-orbit coupling can take on a random value. This random value, in double quantum dots, causes a large change in the exchange splitting. We demonstrate a simple analytical method to calculate the phase, and thus the exchange splitting and singlet-triplet qubit frequency, for an arbitrary interface. We then show that, with lateral control of the position of a quantum dot using a gate voltage, the valley-orbit phase can be controlled over a wide range, so that variations in the exchange splitting can be controlled for individual devices. Finally, we suggest experiments to measure the valley phase and the concomitant gate voltage control.

Rational molecular and device design enables organic solar cells approaching 20% efficiency.

For organic solar cells to be competitive, the light-absorbing molecules should simultaneously satisfy multiple key requirements, including weak-absorption charge transfer state, high dielectric constant, suitable surface energy, proper crystallinity, etc. However, the systematic design rule in molecules to achieve the abovementioned goals is rarely studied. In this work, guided by theoretical calculation, we present a rational design of non-fullerene acceptor o-BTP-eC9, with distinct photoelectric properties compared to benchmark BTP-eC9. o-BTP-eC9 based device has uplifted charge transfer state, therefore significantly reducing the energy loss by 41 meV and showing excellent power conversion efficiency of 18.7%. Moreover, the new guest acceptor o-BTP-eC9 has excellent miscibility, crystallinity, and energy level compatibility with BTP-eC9, which enables an efficiency of 19.9% (19.5% certified) in PM6:BTP-C9:o-BTP-eC9 based ternary system with enhanced operational stability.

Insights Into Preaggregation Control of Y-Series Nonfullerene Acceptors in Liquid State for Highly Efficient Binary Organic Solar Cells.

Leveraging breakthroughs in Y-series nonfullerene acceptors (NFAs), organic solar cells (OSCs) have achieved impressive power conversion efficiencies (PCEs) exceeding 19%. However, progress in advancing OSCs has decelerated due to constraints in realizing the full potential of the Y-series NFAs. Herein, a simple yet effective solid additive-induced preaggregation control method employing 2-chloro-5-iodopyridine (PDCI) is reported to unlock the full potential of the Y-series NFAs. Specifically, PDCI interacts predominantly with Y-series NFAs enabling enhanced and ordered phase-aggregation in solution. This method leads to a notable improvement and a redshifted absorption of the acceptor phase during film formation, along with improved crystallinity. Moreover, the PDCI-induced preaggregation of NFAs in the solution enables ordered molecule packing during the film-formation process through delicate intermediate states transition. Consequently, the PDCI-induced preaggregated significantly improves the PCE of PM6:Y6 OSCs from 16.12% to 18.12%, among the best values reported for PM6:Y6 OSCs. Importantly, this approach is universally applicable to other Y-series NFA-based OSCs, achieving a champion PCE of 19.02% for the PM6:BTP-eC9 system. Thus, the preaggregation control strategy further unlocks the potential of Y-series NFAs, offering a promising avenue for enhancing the photovoltaic performance of Y-series NFA-based OSCs.

Balancing the Efficiency and Synthetic Accessibility of Organic Solar Cells with Isomeric Acceptor Engineering.

With the continuous development of organic semiconductor materials and on-going improvement of device technology, the power conversion efficiencies (PCEs) of organic solar cells (OSCs) have surpassed the threshold of 19%. Now, the low production cost of organic photovoltaic materials and devices have become an imperative demand for its practical application and future commercialization. Herein, the feasibility of simplified synthesis for cost-effective small-molecule acceptors via end-cap isomeric engineering is demonstrated, and two constitutional isomers, BTP-m-4Cl and BTP-o-4Cl, are synthesized and compared in parallel. These two non-fullerene acceptors (NFAs) have very similar optoelectronic properties but nonuniform morphological and crystallographic characteristics. Consequently, the OSCs composed of PM6:BTP-m-4Cl realize PCE of 17.2%, higher than that of the OSCs with PM6:BTP-o-4Cl (≈16%). When ternary OSCs are fabricated with PM6:BTP-m-4Cl:BTP-o-4Cl, the averaged PCE value reaches 17.95%, presenting outstanding photovoltaic performance. Most excitingly, the figure of merit (FOM) values of PM6:BTP-m-4Cl, PM6:BTP-o-4Cl, and PM6:BTP-m-4Cl:BTP-o-4Cl based devices are 0.190, 0.178, and 0.202 respectively. The FOM values of these systems are all among the top ones of the current high-efficiency OSC systems, revealing high cost-effectiveness of the two NFAs. This work provides a general but accessible strategy to minimize the efficiency-cost gap and promises the economic prospects of OSCs.

Printable high-efficiency organic ionic photovoltaic materials discovered by high-throughput first-principle calculations.

Printable solar cells are promising for low cost and large-scale production. As the two main classes of printable solar cells, organic and perovskite solar cells show distinct advantages and apparent drawbacks. The latter stand as major obstacle toward their commercialization. It is amazing if the advantages of organic and perovskite solar cells are integrated since some of them are complementary. Here, we report ionic-type high-efficiency photovoltaic materials which achieve this goal. We explore 46,388 organic materials from the Crystallography Open Database by extensive quantum mechanical calculations. Through photovoltaic-functionality-directed materials screening, we identify 5 organic ionic-type photovoltaic materials. They show the merits of nontoxic, high dielectric constant (27.03), high theoretical efficiency (28.7%), and superior thermal stability. Our findings propose ionic-type photovoltaic materials, which may surpass traditional organic and perovskite materials and open the door to next-generation printable solar cells.

Symmetrically Fluorinated Benzo[1,2-b:4,5-b']dithiophene-Cored Donor for High-Performance All-Small-Molecule Organic Solar Cells with Improved Active Layer Morphology and Crystallinity.

Side-chain engineering is an efficient molecular design strategy for morphology optimization and performance improvement of organic solar cells (OSCs). Herein, a novel small-molecule donor C-2F, which owns a benzo[1,2-b:4,5-b']dithiophene (BDT) central unit with a symmetrically difluorinated benzene ring as a conjugated side chain, has been synthesized. The conjugated side chain possesses both the symmetry and halogenation effect in novel small molecular donor material. The photovoltaic devices were fabricated with N3 as an acceptor. C-2F:N3 based devices achieved an outstanding power conversion efficiency of 14.64% with a Jsc of 24.87 mA/cm2, a Voc of 0.85 V, and an FF of 69.33%. Then, we investigated the basic material properties, photovoltaic mechanism, and active layer morphology, and the results show that this molecular design strategy of the symmetrically difluorinated moiety as the conjugated side chain provides an effective method for fine-tuning the molecular stacking pattern and active layer phase separation morphology, to improve the all-small-molecule (ASM) OSCs' performances.

Chemically Tuning Stability and Superconductivity of P-H Compounds.

Experimental evidence has revealed superconductivity with a critical temperature, Tc, around 100 K in compressed solid phosphine, but theoretical studies have hitherto found no stable structure in any binary P-H system, leaving the characterization of the new superconductor unsettled. Here we present the findings of an advanced structure search and first-principles calculations unveiling the effect of Li as an electron donor that stabilizes the crystal structure and produces robust phonon-mediated superconductivity in the resulting Li-P-H compounds in wide ranges of stoichiometry and pressure. We showcase a trigonal LiP2H14 phase that reaches Tc of 169 K at 230 GPa and then decreases with rising pressure, which can be remedied by substituting Li with Be or Na, which considerably enhances Tc. These findings highlight the intricate and effective chemical tuning of stabilizing the crystal structure and enhancing the superconductivity in a distinct class of ternary hydrides, opening new avenues for designing and optimizing new high-Tc hydride superconductors.

Possible Hundredfold Enhancement in the Direct Magnetic Coupling of a Single-Atom Electron Spin to a Circuit Resonator.

We report on the challenges and limitations of direct coupling of the magnetic field from a circuit resonator to an electron spin bound to a donor potential. We propose a device consisting of a trilayer lumped-element superconducting resonator and a single donor implanted in enriched 28Si. The resonator impedance is significantly smaller than the practically achievable limit obtained with prevalent coplanar resonators. Furthermore, the resonator includes a nanoscale spiral inductor to spatially focus the magnetic field from the photons at the location of the implanted donor. The design promises an increase of approximately 2 orders of magnitude in the local magnetic field, and thus the spin-to-photon coupling rate g , compared with the estimated rate of coupling to the magnetic field of coplanar transmission line resonators. We show that by use of niobium (aluminum) as the resonator's superconductor and a single phosphorous (bismuth) atom as the donor, a coupling rate of g / 2 π = 0.24 MHz ( 0.39 MHz ) can be achieved in the single-photon regime. For this hybrid cavity-quantum-electrodynamic system, such enhancement in g is sufficient to enter the strong-coupling regime.

Spin relaxation of a donor electron coupled to interface states.

An electron spin qubit in a silicon donor atom is a promising candidate for quantum information processing because of its long coherence time. To be sensed with a single-electron transistor, the donor atom is usually located near an interface, where the donor states can be coupled with interface states. Here we study the phonon-assisted spin-relaxation mechanisms when a donor is coupled to confined (quantum-dot-like) interface states. We find that both Zeeman interaction and spin-orbit interaction can hybridize spin and orbital states, each contributing to phonon-assisted spin relaxation in addition to the spin relaxation for a bulk donor or a quantum dot. When the applied magnetic field B is weak (compared to orbital spacing), the phonon assisted spin relaxation shows the B 5 dependence. We find that there are peaks (hot spots) in the B -dependent and detuning dependent spin relaxation due to strong hybridization of orbital states with opposite spin. We also find spin relaxation dips (cool spots) due to the interference of different relaxation channels. Qubit operations near spin relaxation hot spots can be useful for the fast spin initialization and near cool spots for the preservation of quantum information during the transfer of spin qubits.

Spin decoherence in a two-qubit CPHASE gate: the critical role of tunneling noise.

Rapid progress in semiconductor spin qubits has enabled experimental demonstrations of a two-qubit logic gate. Understanding spin decoherence in a two-qubit logic gate is necessary for optimal qubit operation. We study spin decoherence due to 1 / f charge noise for two electrons in a double quantum dot used for a two-qubit controlled-phase gate. In contrast to the usual belief, spin decoherence can be dominated by the tunneling noise from 1 / f charge noise instead of the detuning noise. Tunneling noise can dominate because the effect of tunneling noise on the spin qubit is first order in the charge admixture; while the effect of the detuning noise is only second order. The different orders of contributions result in different detuning dependence of the decoherence, which provides a way to identify the noise source. We find that decoherence in a recent two-qubit experiment was dominated by the tunneling noise from 1 / f charge noise. The results illustrate the importance of considering tunneling noise to design optimal operation of spin qubits.

Doppler effect induced spin relaxation boom.

We study an electron spin qubit confined in a moving quantum dot (QD), with our attention on both spin relaxation, and the product of spin relaxation, the emitted phonons. We find that Doppler effect leads to several interesting phenomena. In particular, spin relaxation rate peaks when the QD motion is in the transonic regime, which we term a spin relaxation boom in analogy to the classical sonic boom. This peak indicates that a moving spin qubit may have even lower relaxation rate than a static qubit, pointing at the possibility of coherence-preserving transport for a spin qubit. We also find that the emitted phonons become strongly directional and narrow in their frequency range as the qubit reaches the supersonic regime, similar to Cherenkov radiation. In other words, fast moving excited spin qubits can act as a source of non-classical phonons. Compared to classical Cherenkov radiation, we show that quantum dot confinement produces a small but important correction on the Cherenkov angle. Taking together, these results have important implications to both spin-based quantum information processing and coherent phonon dynamics in semiconductor nanostructures.

Non-markovian dynamics of a biased qubit coupled to a structured bath.

A new analytical approach, beyond the rotating wave approximation, based on unitary transformations and the non-markovian master equation for the density operator, is applied to treat the biased spin-boson model with a Lorentzian structured bath for arbitrary detunings at zero temperature. Compared to zero bias, we find that the non-equilibrium dynamics demonstrates two more damping oscillation frequencies and one additional relaxation frequency for non-zero bias. Analytical expressions for the non-markovian dynamics and the corresponding spectrum, the localized-delocalized transition point, the coherent-incoherent transition point, the analytical ground energy, the renormalized tunneling factor and the susceptibility are determined. The sum rule and the Shiba relation are checked in the coherent regime.