The role of sulfur cycle in new particle formation: Cycloaddition reaction of SO3 to H2S.

The chemistry of sulfur cycle contributes significantly to the atmospheric nucleation process, which is the first step of new particle formation (NPF). In the present study, cycloaddition reaction mechanism of sulfur trioxide (SO3) to hydrogen sulfide (H2S) which is a typical air pollutant and toxic gas detrimental to the environment were comprehensively investigate through theoretical calculations and Atmospheric Cluster Dynamic Code simulations. Gas-phase stability and nucleation potential of the product thiosulfuric acid (H2S2O3, TSA) were further analyzed to evaluate its atmospheric impact. Without any catalysts, the H2S + SO3 reaction is infeasible with a barrier of 24.2 kcal/mol. Atmospheric nucleation precursors formic acid (FA), sulfuric acid (SA), and water (H2O) could effectively lower the reaction barriers as catalysts, even to a barrierless reaction with the efficiency of cis-SA > trans-FA > trans-SA > H2O. Subsequently, the gas-phase stability of TSA was investigated. A hydrolysis reaction barrier of up to 61.4 kcal/mol alone with an endothermic isomerization reaction barrier of 5.1 kcal/mol under the catalytic effect of SA demonstrates the sufficient stability of TSA. Furthermore, topological and kinetic analysis were conducted to determine the nucleation potential of TSA. Atmospheric clusters formed by TSA and atmospheric nucleation precursors (SA, ammonia NH3, and dimethylamine DMA) were thermodynamically stable. Moreover, the gradually decreasing evaporation coefficients for TSA-base clusters, particularly for TSA-DMA, suggests that TSA may participate in NPF where the concentration of base molecules are relatively higher. The present new reaction mechanism may contributes to a better understanding of atmospheric sulfur cycle and NPF.

Relevance of Bacteria in Causing Rain and Snow.

The Earth's climate is influenced by both natural phenomena (solar fluctuations, oceanic patterns, volcanic eruptions, and tectonic movements) and human activities (deforestation, CO and CO2 emissions, and desertification), all of which contribute to ongoing climate change and the resulting global warming. However, human actions are a major factor in exacerbating global warming and amplifying its adverse impacts worldwide. . With rising temperatures, water evaporation from water bodies and soils intensifies, leading to heightened water scarcity, particularly in drought-prone regions. This scarcity compounds rainfall deficits, posing significant challenges. Precipitation, essential for the biosphere's hydrological cycle, replenishes much of the world's freshwater. It occurs when condensed water vapor in the atmosphere falls back to Earth as rain, drizzle, sleet, graupel, hail, or snow due to gravity. Literature highlights the indispensable role of bacterial populations in this process, termed bio-precipitation. This phenomenon begins with bacterial colonization on plant surfaces, with colonies subsequently dispersed into the atmosphere by winds, triggering ice crystal formation. Through their ice nucleating property, these bacteria facilitate the growth of larger ice crystals, which eventually melt and precipitate as rain or snow. This mechanism aids in nutrient transfer from clouds to soil or vegetation. Pseudomonas syringae stands out as the most notable microorganism exhibiting this ice-nucleation property, serving as the primary source of ice nucleators driving bio-precipitation. Despite limited literature on "rain and snow-causing bacteria," this review comprehensively explores the conceptual background of bio-precipitation, the involved bioprocesses, and the critical role of bacteria like P. syringae, offering insights into future research directions.

Flow-Xl: a new facility for the analysis of crystallization in flow systems.

Characterization of crystallization processes in situ is of great importance to furthering knowledge of how nucleation and growth processes direct the assembly of organic and inorganic materials in solution and, critically, understanding the influence that these processes have on the final physico-chemical properties of the resulting solid form. With careful specification and design, as demonstrated here, it is now possible to bring combined X-ray diffraction and Raman spectroscopy, coupled to a range of fully integrated segmented and continuous flow platforms, to the laboratory environment for in situ data acquisition for timescales of the order of seconds. The facility used here (Flow-Xl) houses a diffractometer with a micro-focus Cu Kα rotating anode X-ray source and a 2D hybrid photon-counting detector, together with a Raman spectrometer with 532 and 785 nm lasers. An overview of the diffractometer and spectrometer setup is given, and current sample environments for flow crystallization are described. Commissioning experiments highlight the sensitivity of the two instruments for time-resolved in situ data collection of samples in flow. Finally, an example case study to monitor the batch crystallization of sodium sulfate from aqueous solution, by tracking both the solute and solution phase species as a function of time, highlights the applicability of such measurements in determining the kinetics associated with crystallization processes. This work illustrates that the Flow-Xl facility provides high-resolution time-resolved in situ structural phase information through diffraction data together with molecular-scale solution data through spectroscopy, which allows crystallization mechanisms and their associated kinetics to be analysed in a laboratory setting.

Time and Temperature Dependence of Drug Crystallization─The Role of Molecular Mobility.

Using the time-temperature-transformation diagrams, we demonstrated a correlation between molecular mobility and crystallization in amorphous solid dispersions of nifedipine (NIF) with each polyvinylpyrrolidone vinyl acetate (PVPVA64) and polyvinyl caprolactam polyvinyl acetate-polyethylene glycol graft copolymer (Soluplus). The behavior was compared with the NIF dispersions prepared with each polyvinylpyrrolidone (PVP) and hydroxypropyl methylcellulose acetate succinate (HPMCAS) [Lalge et al., Mol. Pharmaceutics 2023, 20(3), 1806-1817]. Each system was characterized by a unique temperature at which the crystallization onset time was the shortest. Below this temperature, a coupling was observed between the α-relaxation time determined by dielectric spectroscopy and crystallization onset time. Above this temperature, the activation barrier for crystallization had a more significant role than molecular mobility. In the solid state, PVP and PVPVA64 dispersion exhibited higher resistance to crystallization than HPMCAS and Soluplus. The role of polymers in inhibiting crystal growth in nucleated systems was discerned by monitoring crystallization following wetting of the amorphous dispersion with the dissolution medium. PVPVA64 and Soluplus dispersions exhibited higher resistance to crystal growth than PVP and HPMCAS.

From Ions to Crystals: A Comprehensive View of the Non-Classical Nucleation of Calcium Sulfate.

After years of intensive research and numerous important observations, our understanding of the early stages of crystallization is still limited due to the complexity of the underlying processes and their elusive character. In the present work, we provide a detailed view on the nucleation of calcium sulfate mineralization - an abundant mineral with broad use in construction industry - in aqueous systems at ambient conditions. As experimental basis, a co-titration procedure with potentiometric, turbidimetric and conductometric detection was developed, allowing solution speciation and the formation of crystallization precursors to be monitored quantitatively as the level of nominal (super)saturation gradually increases. The nature and spatiotemporal evolution of these precursors was further elucidated by time-resolved small-angle X-ray scattering (SAXS) and analytical ultracentrifugation (AUC) experiments, complemented by cryogenic transmission electron microscopy (cryo-TEM) as a direct imaging technique. The results reveal how ions associate into nanometric primary species, which subsequently aggregate and develop anisotropic order by intrinsic structural reorganization. Our observations challenge the common understanding of fundamental notions such as the nucleation barrier or the meaning of supersaturation, with broad implications for mineralization phenomena in general and the formation of calcium sulfate in geochemical settings and industrial applications in particular.

Exploring the use of ground-based remote sensing to identify new particle formation events: A case study in the Beijing area.

New Particle Formation (NPF) is an important process of secondary aerosol production in the atmosphere, which has significant impacts on the Earth's radiation balance, air quality, and climate change. In this study, we develop a method to identify NPF events based on ground-based remote sensing. We propose a proxy to characterize NPF events utilizing ground-based remote sensing of gaseous precursors and aerosol optical depth (AOD). This proxy is applied to identify the NPF events in Beijing in the winter of 2022 and tested by comparison with in-situ observations of aerosol particle number size distributions (PNSD) from SMPS. The comparison shows that the NPF events for regional nucleation can be identified effectively when the threshold for sulfur dioxide and organic gases (i.e. formaldehyde) are determined as 0.44 × 10-4 and 1.07 × 10-4. Based on these thresholds, the NPF events can be identified at a high percentage (84 %) compared with in-situ observations. The relationship between identification of NPF events and meteorological conditions shows that NPF events in Beijing winter occurred more frequently under weather conditions with north-west wind direction, high wind speed and low relative humidity.

Synthesis of metallic nanoparticles using biometabolites: mechanisms and applications.

Bio-metabolites have played a crucial role in the recent green synthesis of nanoparticles, resulting in more versatile, safer, and effective nanoparticles. Various primary and secondary metabolites, such as proteins, carbohydrates, lipids, nucleic acids, enzymes, vitamins, organic acids, alkaloids, flavonoids, and terpenes, have demonstrated strong metal reduction and stabilization properties that can be utilized to synthesize nanomaterials and influence their characters. While physical and chemical methods were previously used to synthesize these nanomaterials, their drawbacks, including high energy consumption, elevated cost, lower yield, and the use of toxic chemicals, have led to a shift towards eco-friendly, rapid, and efficient alternatives. Biomolecules act as reducing agents through deprotonation, nucleophilic reactions, transesterification reactions, ligand binding, and chelation mechanisms, which help sequester metal ions into stable metal nanoparticles (NPs). Engineered NPs have potential applications in various fields due to their optical, electronic, and magnetic properties, offering improved performance compared to bulkier counterparts. NPs can be used in medicine, food and agriculture, chemical catalysts, energy harvesting, electronics, etc. This review provides an overview of the role of primary and secondary metabolites in creating effective nanostructures and their potential applications.

Scalable Synthesis of Organic Core/Shell Architectures toward Dual-Wavelength Optical Waveguides.

Organic core/shell heterostructures have undergone rapid progress in materials chemistry owing to the integration of a wide array of unique properties. Nonetheless, the intricate challenge of regulating homogeneous nucleation and phase separation processes in excessively analogous cocrystal structures presents a formidable barrier to expanding the synthesis strategy for organic core/shell heterostructures. Herein, we successfully achieved a phase separation growth process facilitated by the organic alloy interface layer through a dynamic visualization to capture the intricate morphological evolution. By finely regulating the nucleation process, homogeneous self-assembly induced by high chemical and structural compatibility is circumvented, enabling the formation of organic core/shell heterostructures. Notably, this core/shell architecture boasts dual-wavelength emission at 496 and 696 nm, accompanied by an optical loss coefficient of 0.092 dB per micrometer. This methodology shows potential for extending to the scalable design of other conformational cocrystal heterostructure systems, thereby offering valuable insights into the realm of organic photonics.

TonEBP degradation is essential for microtubule nucleation and regrowth.

TonEBP is a transcription factor known for its involvement in diverse physiological processes, including cell cycle, mitosis, migration, and cytoskeletal remodeling. However, the role of TonEBP regarding microtubules, essential structural components of the cytoskeleton, remains unclear. Here, we introduce a novel function for TonEBP as a regulator of microtubule nucleation. Our initial findings reveal that Nocodazole, a well-known microtubule depolymerizing agent, significantly downregulates the protein level of TonEBP. Moreover, microtubule depolymerization induces rapid degradation of TonEBP through the ubiquitin-proteasome pathway. Knockdown of TonEBP results in enhanced microtubule polymerization and regrowth, whereas the presence of TonEBP impairs microtubule nucleation. Collectively, our data suggest that TonEBP negatively regulates microtubule nucleation.

Articular cartilage fatigue causes frequency-dependent softening and crack extension.

Soft biological polymers, such as articular cartilage, possess exceptional fracture and fatigue resistance, offering inspiration for the development of novel materials. However, we lack a detailed understanding of changes in cartilage material behavior and of crack propagation following cyclic compressive loading. We investigated the structure and mechanical behavior of cartilage as a function of loading frequency and number of cycles. Microcracks were initiated in cartilage samples using microindentation, then cracks were extended under cyclic compression. Thickness, apparent stiffness, energy dissipation, phase angle, and crack length were measured to determine the effects of cyclic loading at two frequencies (1 Hz and 5 Hz). To capture the fatigue-induced material response (thickness, stiffness, energy dissipation, and phase angle), material properties were compared between pre-and-post diagnostic tests. The findings indicate that irreversible structural damage (reduced thickness), cartilage softening (reduced apparent stiffness), and reduced energy dissipation (including phase angle) increased with an increase in the number of cycles. Higher frequency loading resulted in less reduction in energy dissipation, phase angle, and thickness change. Crack lengths, quantified through brightfield imaging, increased with number of cycles and frequency. This study sheds light on the complex response of cartilage under cyclic loading resulting in softening, structural damage, and altered dynamic behavior. The findings provide better understanding of failure mechanisms in cartilage and thus may help in diagnosis and treatment of osteoarthritis.

Anode-Free Li Metal Batteries: Feasibility Analysis and Practical Strategy.

Energy storage devices are striving to achieve high energy density, long lifespan, and enhanced safety. In view of the current popular lithiated cathode, anode-free lithium metal batteries (AFLMBs) will deliver the theoretical maximum energy density among all the battery chemistries. However, AFLMBs face challenges such as low plating-stripping efficiency, significant volume change, and severe Li-dendrite growth, which negatively impact their lifespan and safety. This study provides an overview and analysis of recent progress in electrode structure, characterization, performance, and practical challenges of AFLMBs. The deposition behavior of lithium is categorized into two stages: heterogeneous and homogeneous interface deposition. The feasibility and practical application value of AFLMBs are critically evaluated. Additionally, key test models, evaluation parameters, and advanced characterization techniques are discussed. Importantly, practical strategies of different battery components in AFLMBs, including current collector, interface layer, solid-state electrolyte, liquid-state electrolyte, cathode, and cycling protocol, are presented to address the challenges posed by the two types of deposition processes, lithium loss, crosstalk effect and volume change. Finally, the application prospects of AFLMBs are envisioned, with a focus on overcoming the current limitations and unlocking their full potential as high-performance energy storage solutions.

Induced Extracellular Ice Nucleation Protects Cocultured Spheroid Interior and Exterior during Cryopreservation.

Spheroids and other 3D cellular models more accurately recapitulate physiological responses when compared to 2D models and represent potential alternatives to animal testing. The cryopreservation of spheroids remains challenging, limiting their wider use. Standard DMSO-only cryopreservation results in supercooling to low subzero temperatures, reducing viability, shedding surface cells, and perforating spheroid interiors. Here, cocultured spheroids with differentially labeled outer cell layers allow spatial evaluation of the protective effect of macromolecular ice nucleators by microscopy and histology. Extracellular nucleation is shown to reduce damage to both interior and exterior regions of the spheroids, which will support the development of "off-the-shelf" 3D models.

Impact of controlled ice nucleation on intracellular dehydration, ice formation and their implications on T cell freeze-thaw viability.

Cryopreservation is important in manufacturing of cell therapy products, influencing their safety and effectiveness. During freezing and thawing, intracellular events such as dehydration and ice formation can impact cell viability. In this study, the impact of controlling the ice nucleation temperature on intracellular events and viability were investigated. A model T cell line, Jurkat cells, were evaluated in commercially relevant cryoformulations (2.5 and 5 % v/v DMSO in Plasma-Lyte A) using a cryomicroscopic setup to monitor the dynamic changes cells go through during freeze-thaw as well as a controlled rate freezer to study bulk freeze-thaw. The equilibrium freezing temperatures of the studied formulations and a DMSO/Plasma-Lyte A liquidus curve were determined using DSC. The cryomicroscopic studies revealed that an ice nucleation temperature of -6°C, close to the equilibrium freezing temperatures of cryoformulations, led to more intracellular dehydration and less intracellular ice formation during freezing compared to either a lower ice nucleation temperature (-10 °C) or uncontrolled ice nucleation. The cell membrane integrity and post thaw viability in bulk cryopreservation consistently demonstrated the advantage of the higher ice nucleation temperature, and the correlation between the cellular events and cell viability.

Atmospheric Bases-Enhanced Iodic Acid Nucleation: Altitude-Dependent Characteristics and Molecular Mechanisms.

Iodic acid (IA), the key driver of marine aerosols, is widely detected within the gas and particle phases in the marine boundary layer (MBL) and even the free troposphere (FT). Although atmospheric bases like dimethylamine (DMA) and ammonia (NH3) can enhance IA particles formation, their different efficiencies and spatial distributions make the dominant base-stabilization mechanisms of forming IA particles unclear. Herein, we investigated the IA-DMA-NH3 nucleation system through quantum chemical calculations at the DLPNO-CCSD(T)/aug-cc-pVTZ(-PP)//ωB97X-D/6-311++G(3df,3pd) + aug-cc-pVTZ-PP level of theory and cluster dynamics simulations. We provide molecular-level evidence that DMA and NH3 can jointly stabilize the IA clusters. The formation rates of IA clusters initially decline before rising from the MBL to the FT, owing to variations in mechanism. In the MBL, IA-DMA nucleation predominates, while the contribution of IA-DMA-NH3 synergistic nucleation cannot be overlooked in polar and NH3-polluted regions. In the lower FT, IA-DMA-NH3 nucleation prevails, whereas in the upper FT, IA-NH3 nucleation dominates. The efficiency of IA-DMA-NH3 nucleation is comparable to that of IA-iodous acid nucleation in the MBL and sulfuric acid-NH3 nucleation in the FT. Hence, the IA-DMA-NH3 mechanism holds promise for revealing the missing sources of tropospheric IA particles.

Understanding microbial biomineralization at the molecular level: recent advances.

Microbial biomineralization is a phenomenon involving deposition of inorganic minerals inside or around microbial cells as a direct consequence of biogeochemical cycling. The microbial metabolic processes often create environmental conditions conducive for the precipitation of silicate, carbonate or phosphate, ferrate forms of ubiquitous inorganic ions. Till date the fundamental mechanisms underpinning two of the major types of microbial biomineralization such as, microbially controlled and microbially induced remains poorly understood. While microbially-controlled mineralization (MCM) depends entirely on the genetic makeup of the cell, microbially-induced mineralization (MIM) is dependent on factors such as cell morphology, cell surface structures and extracellular polymeric substances (EPS). In recent years, the organic template-mediated nucleation of inorganic minerals has been considered as an underlying mechanism based on the principles of solid-state bioinorganic chemistry. The present review thus attempts to provide a comprehensive and critical overview on the recent progress in holistic understanding of both MCM and MIM, which involves, organic-inorganic biomolecular interactions that lead to template formation, biomineral nucleation and crystallization. Also, the operation of specific metabolic pathways and molecular operons in directing microbial biomineralization have been discussed. Unravelling these molecular mechanisms of biomineralization can help in the biomimetic synthesis of minerals for potential therapeutic applications, and facilitating the engineering of microorganisms for commercial production of biominerals.

Transcrystalline Mechanism of Banded Spherulites Development in Melt-Crystallized Semicrystalline Polymers.

The decades-long paradigm of continuous and perpetual lamellar twisting constituting banded spherulites has been found to be inconsistent with several recent studies showing discontinuity regions between consecutive bands, for which, however, no explanation has been found. The present research demonstrates, in three different semicrystalline polymers (HDPE, PEG10000 and Pluronic F-127), that sequential transcrystallinity is the predominant mechanism of banded spherulite formation, heterogeneously nucleated on intermittent self-shear-oriented amorphous layers excluded during the crystals' growth. It is hereby demonstrated that a transcrystalline layer can be nucleated on amorphous self-shear-oriented polymer chains in the melt, by a local melt flow in the bulk or in contact with any interface-even in contact with the interface with air, e.g., in contact with an entrapped air bubble or at the edges of the sample-or nucleated following the multiple directions and orientations induced by a turbulent flow. The bilateral excessive local exclusion of amorphous non-crystallizable material, following a short period of initial non-banded growth, is found to be the source of dislocations leading to spirally banded spherulites, through the transcrystalline layers' nucleation thereon. The present research reveals and demonstrates the sequential transcrystalline morphology of banded spherulites and the mechanism of its formation, which may lead to new insights in the understanding and design of polymer processing for specific applications.

Dual Grain Refinement Effect for Pure Aluminum with the Addition of Micrometer-Sized TiB2 Particles.

The inefficiency of grain refinement processes has traditionally been attributed to the limited utilization of heterogeneous nucleation particles within master alloy systems, resulting in the formation of abundant inactive particles. This study aims to investigate the alternative influences of particles by incorporating external micrometer-sized TiB2 particles into the grain refinement process. Through a series of experiments, the refinement efficiency, grain refinement mechanism, and resultant microstructure of TiB2 particle-induced grain refinement specimens are comprehensively examined using various microscopy and analytical techniques, including polarization microscopy (OM), scanning electron microscopy (SEM), differential scanning calorimetry (DSC), and transmission electron microscopy (TEM). Our findings demonstrate a direct correlation between increased levels of TiB2 particles and enhanced grain refinement efficiency. Moreover, the microstructure analysis reveals the distribution of TiB2 particles along grain boundaries, forming a coating due to self-assembly phenomena, while regions with a lower particle content may exhibit irregular grain structures. DSC analysis further confirms reduced undercooling, indicating the occurrence of heterogeneous nucleation events. However, TEM observations suggest that heterogeneous nucleation is not significantly influenced by the growth restriction factor attributed to TiAl3 2DC compounds. The grain refinement mechanism involving TiB2 particles is elucidated to entail both heterogeneous nucleation and physical growth restriction effects. Specifically, a reduction in average grain size is attributed not only to heterogeneous nucleation but also to the physical growth restriction effect facilitated by the TiB2 particle coating. This study offers insights into leveraging particles that do not participate in heterogeneous nucleation within master alloy-based grain refinement systems.

Unraveling the Deposition and Dissolution Behavior of the Ag-Modified Li Surface Based on Electrochemical Atomic Force Microscopy.

Lithium is a promising anode material for advanced batteries because of its high capacity and low redox potential. However, its practical use is hindered by nonuniform Li deposition and dendrite formation, leading to safety concerns in Li metal batteries. Our study shows that Ag-based materials enhance the uniformity of Li deposition on Ag-modified Li (AgLi) surfaces, thereby addressing these key challenges. This improvement is due to the strong affinity of Ag for Li, which promotes uniform deposition and dissolution. Additionally, the AgLi surface demonstrated an improved cycling stability, which is crucial for long-term battery reliability. Emphasizing our analytical approach, we utilized comprehensive techniques such as Kelvin probe force microscopy (KPFM) and electrochemical atomic force microscopy (EC-AFM) to locally analyze the electrical properties and unravel the Li deposition/dissolution mechanisms. KPFM analysis provided crucial insights into surface potential variations, while EC-AFM highlighted topographical changes during the Li deposition and dissolution processes, contributing significantly to the development of safer and more efficient Li metal batteries.

Quantitative label-free digital holographic imaging of cardiomyocyte optical volume, nucleation, and cell division.

Cardiac regeneration in newborn rodents depends on the ability of pre-existing cardiomyocytes to proliferate and divide. This capacity is lost within the first week of postnatal development when these cells rapidly switch from hyperplasia to hypertrophy, withdraw from the cell cycle, become binucleated, and increase in size. How these dynamic changes in cell size and nucleation impact cardiomyocyte proliferative potential is not well understood. In this study, we innovate the application of a commercially available digital holographic imaging microscope, the Holomonitor M4, to evaluate the proliferative responses of mononucleated and binucleated cardiomyocytes after CHIR99021 treatment, a model proliferative stimulus. This system enables long-term label-free quantitative tracking of primary cardiomyocyte dynamics in real-time with single-cell resolution. Our results confirm that chemical inhibition of glycogen synthase kinase 3 with CHIR99021 promotes complete cell division of both mononucleated and binucleated cardiomyocytes with high frequency. Quantitative tracking of cardiomyocyte volume dynamics during these proliferative events revealed that both mononucleated and binucleated cardiomyocytes reach a similar size-increase threshold prior to attempted cell division. Binucleated cardiomyocytes attempt to divide with lower frequency than mononucleated cardiomyocytes, which may be associated with inadequate increases in cell size. By defining the interrelationship between cardiomyocyte size, nucleation, and cell cycle control, we may better understand the cellular mechanisms that drive the loss of mammalian cardiac regenerative capacity after birth.

Heterogeneous Nucleation Regulation Amends Unfavorable Crystallization Orientation and Defect Features of Antimony Selenosulfide Film for High-Efficient Planar Solar Cells.

Antimony selenosulfide (Sb2(S,Se)3) has obtained widespread concern for photovoltaic applications as a light absorber due to superior photoelectric features. Accordingly, various deposition technologies have been developed in recent years, especially hydrothermal deposition method, which has achieved a great success. However, device performances are limited with severe carrier recombination, relating to the quality of absorber and interfaces. Herein, bulk and interface defects are simultaneously suppressed by regulating heterogeneous nucleation kinetics with barium dibromide (BaBr2) introduction. In details, the Br adsorbs and dopes on the polar planes of cadmium sulfide (CdS) buffer layer, promoting the exposure of nonpolar planes of CdS, which facilitates the favorable growth of [hk1]-Sb2(S,Se)3 films possessing superior crystallinity and small interface defects. Additionally, the Se/S ratio is increased due to the replacement of S/Se by Br, causing a downshift of the Fermi levels with a benign band alignment and a shallow-level defect. Moreover, Ba2+ is located at grain boundaries by coordination with S and Se ions, passivating grain boundary defects. Consequently, the efficiency is increased from 7.70% to 10.12%. This work opens an avenue towards regulating the heterogeneous nucleation kinetics of Sb2(S,Se)3 film deposited via hydrothermal deposition approach to optimize its crystalline orientation and defect features.