State Emission Research Articles

X-Ray Irradiation of the Giant Planet Orbiting the T Tauri Star TAP 26

We present new Chandra X-ray observations of TAP 26, a ≈17 Myr old magnetically active weak-lined T Tauri star that has been reported to host a massive planet in a ≈10.8 day orbit. At a separation of a = 0.097 au the planet will be exposed to intense X-ray and UV radiation from the star. The first observation caught the star in a state of elevated X-ray emission with variability on a timescale of a few hours and an X-ray temperature kT x ≈ 2–4 keV. Two subsequent observations 5–10 days later showed slow variability and a lower X-ray flux and temperature (kT x ≈ 1 keV). We characterize the X-ray emission and estimate the X-ray ionization and heating rates that will need to be incorporated into realistic models of the planet’s atmosphere.

Excited-State Engineering Enables Efficient Deep-Blue Light-Emitting Diodes Exhibiting BT.2020 Color Gamut.

Organic luminescent materials that exhibit thermally activated delayed fluorescence (TADF) can convert non-emissive triplet excitons into emissive singlet states through a reverse intersystem crossing (RISC) process. Therefore, they have tremendous potential for applications in organic light-emitting diodes (OLEDs). However, with the development of ultra-high definition 4K/8K display technologies, designing efficient deep-blue TADF materials to achieve the Commission Internationale de l'Éclairage (CIE) coordinates fulfilling BT.2020 remains a significant challenge. Here, an effective approach is proposed to design deep-blue TADF molecules based on hybrid long- and short-range charge-transfer by incorporation of multiple donor moieties into organoboron multiple resonance acceptors. The resulting TADF molecule exhibits deep-blue emission at 414nm with a full width at half maximum (FWHM) of 29nm, together with a thousand-fold increase in RISC rate. OLEDs based on the champion material achieve a record maximum external quantum efficiency (EQE) of 22.8% with CIE coordinates of (0.163, 0.046), approaching the coordinates of the BT.2020 blue standard. Moreover, TADF-assisted fluorescence devices employing the designed material as a sensitizer exhibit an exceptional EQE of 33.1%. This work thus provides a blueprint for future development of efficient deep-blue TADF emitters, representing an important milestone towards meeting the blue color gamut standard of BT.2020.

Numerical simulation of a spark ignition ammonia marine engine for future ship power applications

Given the current state of global carbon emissions, China has proposed the objectives of achieving carbon peaking by 2030 and carbon neutrality by 2060. To meet the requirement of zero-carbon and achieve the application of pure ammonia fuel in low-speed two-stroke marine engines, this paper proposes the Groove Diversion-Assist Ignition (GDAI) combustion system, which can effectively control the temperature, fuel distribution, and flow rate in the spark plug region near the top dead center and finally achieve the spark ignition of pure ammonia without any change in compression ratio and scavenging temperature. At the same time, the boundary conditions for the ignition of ammonia fuel have also been studied. The results show that enhancing the initial temperature can alleviate the requirement for spark ignition energy, and a minimum energy level of 75 mJ remains necessary for effective spark ignition of ammonia. Furthermore, the utilization of spark ignition of ammonia fuel can achieve a maximum thermal efficiency of 51.32%, representing a 2.8% increase in overall thermal efficiency compared to the diesel mode. Additionally, the application of ammonia fuel can relief the NOx emissions compare to diesel fuel, which provides a new and effective utilization way for the application of ammonia fuel on the marine engine.

Spin-configuration of emission states in zero-dimensional metal halides

ABSTRACT Understanding the spin-configuration of excited states in a luminescent material is essential for tailoring its properties for many applications such as light-emitting diodes and spin-optoelectronic devices. Zero-dimensional organic-inorganic metal halide (0D-OIMH) materials have demonstrated remarkable potential in diverse applications owing to their captivating optoelectronic characteristics. However, the electronic structure and spin-configuration of the frequently observed dual-peak emission in these materials remains a subject of intensive debate. In this study, we employ low-temperature magneto-optical measurements to investigate the excited state structure of a representative 0D-OIMH, namely (Bmpip)2SnBr4. The spin-configurations of the dark and bright states are clearly elucidated by measuring the magneto-polarization of the emissions. Our results reveal that the high-energy peak arises from bright excited states within a higher energy band, whilst the low-energy peak originates from a combination of triplet-bright states and singlet-dark states. These findings provide an unambiguous understanding of the exciton structures of the distinctive 0D-OIMHs.

Spectrally Tunable Lead-Free Perovskite Rb2ZrCl6:Te for Information Encryption and X-ray Imaging.

A series of lead-free Rb2ZrCl6:xTe4+ (x = 0%, 0.1%, 0.5%, 1.0%, 2.0%, 3.0%, 5.0%, 10.0%) perovskite materials were synthesized through a hydrothermal method in this work. The substitution of Te4+ for Zr in Rb2ZrCl6 was investigated to examine the effect of Te4+ doping on the spectral properties of Rb2ZrCl6 and its potential applications. The incorporation of Te4+ induced yellow emission of triplet self-trapped emission (STE). Different luminescence wavelengths were regulated by Te4+ concentration and excitation wavelength, and under a low concentration of Te4+ doping (x ≤ 0.1%), different types of host STE emission and Te4+ triplet state emission could be achieved through various excitation energies. These luminescent properties made it suitable for applications in information encryption. When Te4+ was doped at high concentrations (x ≥ 1%), yellow triplet state emission of Te4+ predominated, resulting in intense yellow emission, which stemmed from strong exciton binding energy and intense electron-phonon coupling. In addition, a Rb2ZrCl6:2%Te4+@RTV scintillating film was fabricated and a spatial resolution of 3.7 lp/mm was achieved, demonstrating the potential applications of Rb2ZrCl6:xTe4+ in nondestructive detection and bioimaging.

Enhanced Intersystem Crossing in a Thiohelicene

AbstractThe photophysics of a helicene derivative in which two benzene units are replaced by thiophene units (thiohelicene, 6H) was studied by steady state and transient absorption and emission spectroscopies covering time ranges from femtoseconds to minutes. Efficient intersystem crossing (ISC) to the triplet state was observed, by far exceeding that of the parent helicene and the corresponding oxo‐helicene. Quantum chemical calculations indicate that the helical distortion and the heavy atom effect of sulfur cooperate in promoting spin‐orbit coupling, and that the most efficient decay channel involved the T2 or even the T3 state. These insights can help in the design of more efficient triplet sensitizers for many applications.

Investigation on Fluorescence Origin and Spectral Heterogeneity in Carbon Dots: A Dynamic Perspective

AbstractHeterogeneity in the fluorescence of carbon dots (CDs) has been hard to figure out so far. This could potentially be related to structural factors, size or intermediate fluorophores, especially when employing the bottom‐up synthesis. Herein, we unveil the origin of fluorescence and spectral heterogeneity of CDs using a simple dynamic method. This work reports the room light‐excited green fluorescence and dual‐emissive N‐doped CDs synthesized using a hydrothermal method. Studies were carried out considering the factors of fluorescence phenomena, such as excitation‐independent emission, fluorescent impurities, aggregation and solvation dynamics. The new steady‐state, Excitation‐resolved area‐normalized emission spectroscopy (ERANES) and ensemble measurements, including time‐resolved studies reveal that a heterogeneous environment exists in the ground state. Eventually, the results show the existence of core, edge and surface states in the CDs. Additionally, the fluorescence characteristics depend on the structural functionalization that occurs in both the intrinsic and extrinsic states of the CDs and it is proven that this does not violate the Kasha‐Vavilov rule. Although a highly purified material could still exhibit heterogeneity due to the ensemble emissive states and structural variations. Our results provide insights into the enduring debates about fluorescence and a deeper understanding of the structure‐ property relationship of CDs.

Investigation of atomic surface potential on Si(111)-7×7 surface by high-frequency heterodyne-Kelvin probe force microscopy

The surface potential on n-type Si(111)-7 × 7 surface was measured at 78 K using high-frequency heterodyne-Kelvin probe force microscopy (HF-he-KPFM) method with atomic resolution. By comparing VCPD images obtained from conventional KPFM and HF-he-KPFM, we found that frequency dependence of carrier emission and capture of surface states on Si(111)-7 × 7 surface. Furthermore, donor- and accepter-like surface states on different atom position of Si(111)-7 × 7 surface are distinguished. In addition, the electric field effect of high-low Kelvin probe force spectroscopy (KPFS) was analyzed, and the dissipative force was revealed in the high-frequency KPFS. These findings underscore the potential of HF-he-KPFM as a promising method for studying semiconductor properties such as surface potential, band bending and capacitance.

Will digital trade provisions in regional trade agreements effectively reduce CO2 emissions in member states?

This paper constructs a depth index of the regional trade agreement (RTA) digital trade terms based on text data from 2000–2021 in the TAPED database and carbon dioxide (CO2) emission data from the Eora database since 2000. We construct a gravity model between the depth index of digital trade terms and carbon CO2 emissions to analyze the impact of digital trade terms in RTAs on the CO2 emissions of member countries. The results show that the depth of digital trade clauses in RTAs significantly reduces the CO2 emissions of member countries. Still, the impact of different clause depth indexes on CO2 emissions is different on the supply and consumption sides. The results of the heterogeneity analysis based on the types of trade agreements show that the depth of RTAs has the most significant impact on the CO2 emissions among members of South–North trade agreements. The analysis of results based on industry heterogeneity shows that digital trade terms significantly impact manufacturing CO2 emissions. The article proposes that more attention be paid to the negotiation of digital trade rules in RTAs, the construction of South–North trade agreements, and the impact of digital trade on the CO2 emissions of different industries.

Probing the carbon neutrality drive of environmental-related technologies and energy transition in France and Germany: a novel time–frequency technique

AbstractThis study presents a rare comparative analysis of the factors influencing environmental quality through greenhouse gas (GHG) emissions in the European Union member states’ largest economies, i.e., France and Germany. By considering the unique economic, energy, and environmental characteristics of both countries, the finding unveils a novel perspective in the literature. The research utilizes a recently developed wavelet local multiple correlation (WLMC) technique with quarterly dataset spanning from 1990/Q1 to 2020/Q4. The results demonstrate that environmental-related information and communication technologies innovations, energy transition, and financial development play significant roles in limiting the growth of GHGs emission, particularly in the medium and long term. The wavelet-based Granger causality analysis reveals evidence of feedback causality among the variables in both countries in the medium and long term. Moreover, there are slight differences in the short-term relationships given that the observations are generally similar in later period. Overall, the findings offer a deeper understanding and policy insights regarding the time and frequency dynamics of GHG drivers in France and Germany. Graphical abstract

The Study of Mode-switching Behavior of PSR J0614+2229 Using the Parkes Ultra–wide-bandwidth Receiver Observations

In this paper we present a detailed single-pulse and polarization study of PSR J0614+2229 based on the archived data observed on 2019 August 15 (MJD 58710) and 2019 September 12 (MJD 58738) using the ultra−wide-bandwidth low-frequency receiver on the Parkes radio telescope. The single-pulse sequences show that this pulsar switches between two emission states, in which the emission of state A occurs earlier than that of state B in pulse longitude. We found that the variation in relative brightness between the two states varies temporally and both states follow a simple power law very well. Based on the phase-aligned multifrequency profiles, we found that there is a significant difference in the distributions of spectral index across the emission regions of the two states. Furthermore, we obtained the emission height evolution for the two emission states and found that, at a fixed frequency, the emission height of state A is higher than that of state B. What is even more interesting is that the emission heights of both states A and B do not change with frequency. Our results suggest that the mode switching of this pulsar is possibly caused by changes in the emission heights that alter the distributions of spectral index across the emission regions of states A and B, resulting in frequency-dependent behaviors, i.e., intensity and pulse width.

Exploring electron donor and acceptor effects: DFT analysis of ESIPT/GSIPT in 2-(oxazolinyl)-phenols for photophysical and luminophore enhancement.

Understanding excited-state intramolecular proton transfer (ESIPT) is essential for designing organic molecules to enhance photophysical and luminophore properties in the development of optoelectronic devices. In this context, an attempt has been made to understand the impact of substituents on the ESIPT process of 2-(oxazolinyl)-phenol. Electron donating (EDG: -NH2, -OCH3, and -CH3) and electron withdrawing (EWG: -Cl, -Br, -COOH, -CF3, -CN, and -NO2) substitutions have been computationally designed and screened through density functional theory (DFT) and time-dependent density-functional theory (TDDFT) calculations. Furthermore, the ground state intramolecular proton transfer and ESIPT mechanisms of these designed luminophores are explored using the transition state theory. The results reveal that molecules with EDG show higher absorption and emission peaks than molecules with EWG and also indicate that the mobility of charge carriers in 2-(oxazolinyl)-phenol derivatives is significantly influenced by substituents. We found that the EWGs decrease the reorganization energy and increase the vertical ionization potential and electron affinity values, as well as the highest occupied molecular orbital-lowest unoccupied molecular orbital gap, compared to the EDG substituted molecules. Significantly, the excited state (S1) of the keto emission (K) form shows notably larger values for the EDG substitutions. The intersystem crossing pathway efficiency weakens with reduced spin-orbit coupling matrix element in the enol form with electron-donating substituents and vice versa in the keto form during S1-T3 transitions. Our research links intramolecular proton transfers and triplet generation, making these substituted molecules appealing for optoelectronic devices. Introducing EDGs, such as -NH2, boosts the ESIPT reaction in 2-(oxazolinyl)-phenol. This study guides designing ESIPT emitters with unique photophysical properties.

Effect of Mixture Composition on the Photophysics of Indoline Dyes in Imidazolium Ionic Liquid-Molecular Solvent Mixtures: A Femtosecond Transient Absorption Study.

We conducted a study on the photophysics of three indoline dyes, D102, D149, and D205, in binary mixtures of ionic liquids (IL) and polar aprotic molecular solvents (MS). Specifically, we examined the behavior of these dyes in IL-MS mixtures containing four different imidazolium-based ILs and three different polar aprotic MSs. Our investigation involved several techniques, including stationary absorption and emission measurements, as well as femtosecond transient absorption (TA) spectroscopy. Through our analysis, we discovered a peculiar behavior of several photophysical properties at low IL mole fractions (0 < XIL < 0.2). Indeed, in this range of mixture composition, the absorption maximum wavelength decreases noticeably, while the emission maximum wavelength and the Stokes shift, expressed in wavenumbers, reach a maximum. while a minimum occurs in the relative quantum yield and the excited state lifetime. These results indicate that the solvation of dye undergoes a large change in this range of mixture composition. We found that, at high ionic liquid content, the excited relaxation times are correlated with the high viscosity, while at low content, it is the polarity of the solvent that influences the behavior of the excited relaxation times. At a mixture composition of around 0.10, the behavior of the photophysical properties of the studied IL-MS mixtures indicates a crossover between situations where the solvation is dominated by that of ions and that dominated by the solvent.

Quantum Defect Sensitization via Phase-Changing Supercharged Antibody Fragments.

Quantum defects in single-walled carbon nanotubes promote exciton localization, which enables potential applications in biodevices and quantum light sources. However, the effects of local electric fields on the emissive energy states of quantum defects and how they can be controlled are unexplored. Here, we investigate quantum defect sensitization by engineering an intrinsically disordered protein to undergo a phase change at a quantum defect site. We designed a supercharged single-chain antibody fragment (scFv) to enable a full ligand-induced folding transition from an intrinsically disordered state to a compact folded state in the presence of a cytokine. The supercharged scFv was conjugated to a quantum defect to induce a substantial local electric change upon ligand binding. Employing the detection of a proinflammatory biomarker, interleukin-6, as a representative model system, supercharged scFv-coupled quantum defects exhibited robust fluorescence wavelength shifts concomitant with the protein folding transition. Quantum chemical simulations suggest that the quantum defects amplify the optical response to the localization of charges produced upon the antigen-induced folding of the proteins, which is difficult to achieve in unmodified nanotubes. These findings portend new approaches to modulate quantum defect emission for biomarker sensing and protein biophysics and to engineer proteins to modulate binding signal transduction.

Molecular Design Using Selected Concentration Effects in Optically Activated Fluorescent Matrices.

Molecular physics plays a pivotal role in various fields, including medicine, pharmaceuticals, and broader industrial applications. This study aims to enhance the methods for producing specific optically active materials with distinct spectroscopic properties at the molecular level, which are crucial for these sectors, while prioritizing human safety in both production and application. Forensic science, a significant socio-economic field, often employs hazardous substances in analyzing friction ridges on porous surfaces, posing safety concerns. In response, we formulated novel, non-toxic procedures for examining paper evidence, particularly thermal papers. Our laboratory model utilizes a polyvinyl alcohol polymer as a rigid matrix to emulate the thermal paper's environment, enabling precise control over the spectroscopic characteristics of 1,8-diazafluoro-9-one (DFO). We identified and analyzed the cyclodimer 1,8-diazafluoren-9-one (DAK DFO), which is a non-toxic and biocompatible alternative for revealing forensic marks. The reagents used to preserve fingerprints were optimized for their effectiveness and stability. Using stationary absorption and emission spectroscopy, along with time-resolved emission studies, we verified the spectroscopic attributes of the new structures under deliberate aggregation conditions. Raman spectroscopy and quantum mechanical computations substantiated the cyclodimer's configuration. The investigation provides robust scientific endorsement for the novel compound and its structural diversity, influenced by the solvatochromic sensitivity of the DFO precursor. Our approach to monitoring aggregation processes signifies a substantial shift in synthetic research paradigms, leveraging simple chemistry to yield an innovative contribution to forensic science methodologies.

The Relationships between Emission Geometry and Jitter Noise in Millisecond Pulsars

The relationships between several parameters of an emission geometry and jitter noise in 17 millisecond pulsars (MSPs) are investigated. By assuming the jitter noise is due only to a pulse variation in phase, the former can be modeled as changes in the plasma flow rate leading to variation in the measured pulse arrival time relative to the predicted time. In the model for pulsar magnetospheres with multiple emission states, the plasma flow is associated with the emission states, and a change in the emission state corresponds to a change in the plasma flow causing variation in the pulse arrival time. These can be specified in an emission geometry defined by the obliquity and viewing angles, measured from the rotation axis to the magnetic axis and to the line of sight, respectively. We calculate the maximum change in the emission state based on the reported jitter noise for each of the MSPs. Using the results, we show that the MSPs possess relatively large obliquity angles, which is consistent with observation, and the jitter noise exhibits dependency on frequency. We find that the jitter noise in our sample displays an exponential decay as a function that combines the obliquity angle and the rotation period, revealing the correlation among the three parameters. This suggests that the magnitude of the jitter noise is likely specific to an MSP. We discuss how jitter noise may be related to the evolution of an MSP.

Synthesis and Photophysical Properties of Silver(I) Coordination Polymers Bridged by Dimethylpyrazine: Comparison of Emissive Excited States between Silver(I) and Copper(I) Congeners.

Highly luminescent silver(I) coordination polymers [Ag2X2(PPh3)2(Me2pyz)]n (X = I, Br, Cl; Me2pyz: 2,5-dimethylpyrazine) were prepared together with copper congeners [Cu2X2(PPh3)2(Me2pyz)]n (X = I, Br). All the complexes showed thermally activated delayed fluorescence from the charge-transfer states in the visible region, from blue to red. The isomorphous relationship among the complexes allowed a detailed discussion of the effect of halogenido ligands and crystal packing on their luminescence energy. The relaxation in the emissive excited states (ESs) was determined to be more remarkable in silver complexes than in copper complexes despite their isomorphous structures, and the electronic effect of halogenido ligands was comparable to the effect of relaxation in emissive ESs.

Electrochemically controlled blinking of fluorophores for quantitative STORM imaging

Stochastic optical reconstruction microscopy (STORM) allows wide-field imaging with single-molecule resolution by calculating the coordinates of individual fluorophores from the separation of fluorophore emission in both time and space. Such separation is achieved by photoswitching the fluorophores between a long-lived OFF state and an emissive ON state. Although STORM can image single molecules, molecular counting remains challenging due to undercounting errors from photobleached or overlapping dyes and overcounting artefacts from the repetitive random blinking of dyes. Here we show that fluorophores can be electrochemically switched for STORM imaging (EC-STORM), with excellent control over the switching kinetics, duty cycle and recovery yield. Using EC-STORM, we demonstrate molecular counting by using electrochemical potential to control the photophysics of dyes. The random blinking of dyes is suppressed by a negative potential but the switching-ON event can be activated by a short positive-potential pulse, such that the frequency of ON events scales linearly with the number of underlying dyes. We also demonstrate EC-STORM of tubulin in fixed cells with a spatial resolution as low as ~28 nm and counting of single Alexa 647 fluorophores on various DNA nanoruler structures. This control over fluorophore switching will enable EC-STORM to be broadly applicable in super-resolution imaging and molecular counting.

The potential of carbon markets to accelerate green infrastructure based water quality trading

Green infrastructure solutions can improve in-stream water quality in lieu of building electricity-consuming gray infrastructure. Permitted under the United States Clean Water Act, these programs allow regulated utilities to trade point-source water quality obligations with non-point source mitigation efforts in the watershed. Carbon financing can provide an incentive for water quality trading. Here we combine data on impaired waters, treatment technologies, and life cycle greenhouse gas emissions in the Contiguous United States, and compare traditional treatment technologies to alternative green infrastructure. We find green infrastructure could save $15.6 billion dollars, 21.2 terawatt-hours of electricity, and 29.8 million tonnes of carbon dioxide equivalent emissions per year while sequestering over 4.2 million tonnes CO2e per year over a 40 year time horizon. Green infrastructure solutions may have the potential to generate $679 million annually in carbon credit revenue (at $20 per credit), which represents a unique opportunity to help accelerate water quality trading.

Smart Agriculture and Greenhouse Gas Emission Mitigation: A 6G-IoT Perspective

Smart farming has emerged as a promising approach to address the agriculture industry’s significant contribution to greenhouse gas (GHG) emissions. However, the effectiveness of current smart farming practices in mitigating GHG emissions remains a matter of ongoing debate. This review paper provides an in-depth examination of the current state of GHG emissions in smart farming, highlighting the limitations of existing practices in reducing GHG emissions and introducing innovative strategies that leverage the advanced capabilities of 6G-enabled IoT (6G-IoT). By enabling precise resource management, facilitating emission source identification and mitigation, and enhancing advanced emission reduction techniques, 6G-IoT integration offers a transformative solution for managing GHG emissions in agriculture. However, while smart agriculture focuses on technological applications for immediate efficiency gains, it also serves as a crucial component of sustainable agriculture by providing the tools necessary for long-term environmental supervision and resource sustainability. As a result, this study also contributes to sustainable agriculture by providing insights and guiding future advancements in smart farming, particularly in the context of 6G-IoT, to develop more effective GHG mitigation strategies for smart farming applications, promoting a more sustainable agricultural future.