Size Confinement Effects on Electronic and Optical Properties of Silver Halide Nanocrystals as Probed by Cryo-EFTEM and EELS

Cryo-energy-filtering transmission electron microscopy and electron energy-loss spectroscopy have been applied to study size confinement effects on electronic, dielectric, and optical properties of Ag(Br, I) nanocrystals. The dielectric permittivity, optical joint density of states, refractive index, extinction, and absorption for nanocrystals derived via Kramers–Kronig relations have been compared with experimental data for Ag(Br, I) tabular microcystals and ab initio linear muffin-tin orbital method in its atomic spheres approximation calculations for AgBr. Contrast tuning with the selected energy window between 0 and 100 eV enabled visualizing valence electron excitations in silver halides because of plasmons superimposed with interband transitions and Mott–Wannier excitons. The nonuniform contrast of nanocrystals revealed by cryo-energy-filtering transmission electron microscopy was referred to a size-confined coupling of surface and volume losses that could lead to oscillations of the image intensity with the nanocrystal size. A size-dependent enhancement of interband transitions at 4 eV correlated with the enhancement of exciton luminescence from nanocrystals because of contributions to the energy-level structure from carrier confinement and surface states.     

Clustered magnetite nanocrystals cross-linked with PEI for efficient siRNA delivery

Magnetofection has been utilized as a powerful tool to enhance gene transfection efficiency via magnetic field-enforced cellular transport processes. The accelerated accumulation of nucleic acid molecules by applying an external magnetic force enables the rapid and improved transduction efficiency. In this study, we developed magnetite nanocrystal clusters (PMNCs) cross-linked with polyethylenimine (PEI) to magnetically trigger intracellular delivery of small interfering RNA (siRNA). PMNCs were produced by cross-linked assembly of catechol-functionalized branched polyethylenimine (bPEI) around magnetite nanocrystals through an oil-in-water (O/W) emulsion and solvent evaporation method. The physical properties of PMNC were characterized by TEM, DLS, TSA, and FT-IR. Finely tuned formulation of clustered magnetite nanocrystals with controlled size and shape exhibited superior saturation of magnetization value. Magnetite nanocrystal clusters could form nanosized polyelectrolyte complexes with negatively charged siRNA molecules, enabling efficient delivery of siRNA into cells upon exposure to an external magnetic field within a short time. This study introduces a new class of magnetic nanomaterials that can be utilized for magnetically driven intracellular siRNA delivery.     

Low Light Adaptation: Energy Transfer Processes in Different Types of Light Harvesting Complexes from Rhodopseudomonas palustris

Energy transfer processes in photosynthetic light harvesting 2 (LH2) complexes isolated from purple bacterium Rhodopseudomonas palustris grown at different light intensities were studied by ground state and transient absorption spectroscopy. The decomposition of ground state absorption spectra shows contributions from B800 and B850 bacteriochlorophyll (BChl) a rings, the latter component splitting into a low energy and a high energy band in samples grown under low light (LL) conditions. A spectral analysis reveals strong inhomogeneity of the B850 excitons in the LL samples that is well reproduced by an exponential-type distribution. Transient spectra show a bleach of both the low energy and high energy bands, together with the respective blue-shifted exciton-to-biexciton transitions. The different spectral evolutions were analyzed by a global fitting procedure. Energy transfer from B800 to B850 occurs in a mono-exponential process and the rate of this process is only slightly reduced in LL compared to high light samples. In LL samples, spectral relaxation of the B850 exciton follows strongly nonexponential kinetics that can be described by a reduction of the bleach of the high energy excitonic component and a red-shift of the low energetic one. We explain these spectral changes by picosecond exciton relaxation caused by a small coupling parameter of the excitonic splitting of the BChl a molecules to the surrounding bath. The splitting of exciton energy into two excitonic bands in LL complex is most probably caused by heterogenous composition of LH2 apoproteins that gives some of the BChls in the B850 ring B820-like site energies, and causes a disorder in LH2 structure.     

Compact Quantum Dots for Single-molecule Imaging

Single-molecule imaging is an important tool for understanding the mechanisms of biomolecular function and for visualizing the spatial and temporal heterogeneity of molecular behaviors that underlie cellular biology ^1-4. To image an individual molecule of interest, it is typically conjugated to a fluorescent tag (dye, protein, bead, or quantum dot) and observed with epifluorescence or total internal reflection fluorescence (TIRF) microscopy. While dyes and fluorescent proteins have been the mainstay of fluorescence imaging for decades, their fluorescence is unstable under high photon fluxes necessary to observe individual molecules, yielding only a few seconds of observation before complete loss of signal. Latex beads and dye-labeled beads provide improved signal stability but at the expense of drastically larger hydrodynamic size, which can deleteriously alter the diffusion and behavior of the molecule under study.Quantum dots (QDs) offer a balance between these two problematic regimes. These nanoparticles are composed of semiconductor materials and can be engineered with a hydrodynamically compact size with exceptional resistance to photodegradation ⁵. Thus in recent years QDs have been instrumental in enabling long-term observation of complex macromolecular behavior on the single molecule level. However these particles have still been found to exhibit impaired diffusion in crowded molecular environments such as the cellular cytoplasm and the neuronal synaptic cleft, where their sizes are still too large ^4,6,7.Recently we have engineered the cores and surface coatings of QDs for minimized hydrodynamic size, while balancing offsets to colloidal stability, photostability, brightness, and nonspecific binding that have hindered the utility of compact QDs in the past ^8,9. The goal of this article is to demonstrate the synthesis, modification, and characterization of these optimized nanocrystals, composed of an alloyed Hg_xCd_1-xSe core coated with an insulating Cd_yZn_1-yS shell, further coated with a multidentate polymer ligand modified with short polyethylene glycol (PEG) chains (Figure 1). Compared with conventional CdSe nanocrystals, Hg_xCd_1-xSe alloys offer greater quantum yields of fluorescence, fluorescence at red and near-infrared wavelengths for enhanced signal-to-noise in cells, and excitation at non-cytotoxic visible wavelengths. Multidentate polymer coatings bind to the nanocrystal surface in a closed and flat conformation to minimize hydrodynamic size, and PEG neutralizes the surface charge to minimize nonspecific binding to cells and biomolecules. The end result is a brightly fluorescent nanocrystal with emission between 550-800 nm and a total hydrodynamic size near 12 nm. This is in the same size range as many soluble globular proteins in cells, and substantially smaller than conventional PEGylated QDs (25-35 nm).     

The Shielding Effect of Microcrystalline Cellulose on Drug Nanocrystal Particles During Compaction

To elucidate the compaction behavior of drug nanocrystals based composite particles (NP) during tabletting, the compaction behavior of binary mixtures of microcrystalline cellulose (MCC) and nanocrystal particles was investigated. The force-displacement correlation of mixtures containing different ratios of MCC and micronized NP was studied in order to explain the nature on densification of NP during compaction, and the resultant compaction curves (pressure as function of in-die thickness) were systemically analyzed to elucidate the most important mechanisms of volume reduction for MCC and NP in different stages of compaction. The results showed that the close compaction of individual MCC was relatively quickly achieved, and the drug NP particles could slide into the intrinsic void spaces between MCC microparticles. This was the reason that the particles size of MCC used in this study was significantly larger compared to that of drug NP. This interstitial rearrangement phenomenon of NP occurred on a typical time scale and was strongly dependent on the speed of compaction. This migration behavior occurred on void spaces of MCC inter-particles might be identified as an elastic stress relaxation mechanism and be helpful to dissolution of NP. MCC can effectively shield the NP from significant aggregation during compaction process.     

Characterization of Nanocrystal Size Distribution using Raman Spectroscopy with a Multi-particle Phonon Confinement Model

Analysis of the size distribution of nanocrystals is a critical requirement for the processing and optimization of their size-dependent properties. The common techniques used for the size analysis are transmission electron microscopy (TEM), X-ray diffraction (XRD) and photoluminescence spectroscopy (PL). These techniques, however, are not suitable for analyzing the nanocrystal size distribution in a fast, non-destructive and a reliable manner at the same time. Our aim in this work is to demonstrate that size distribution of semiconductor nanocrystals that are subject to size-dependent phonon confinement effects, can be quantitatively estimated in a non-destructive, fast and reliable manner using Raman spectroscopy. Moreover, mixed size distributions can be separately probed, and their respective volumetric ratios can be estimated using this technique. In order to analyze the size distribution, we have formulized an analytical expression of one-particle PCM and projected it onto a generic distribution function that will represent the size distribution of analyzed nanocrystal. As a model experiment, we have analyzed the size distribution of free-standing silicon nanocrystals (Si-NCs) with multi-modal size distributions. The estimated size distributions are in excellent agreement with TEM and PL results, revealing the reliability of our model.     

Size‐Dependent Charge Transfer in Blends of PbS Quantum Dots with a Low‐Gap Silicon‐Bridged Copolymer

The photophysics of bulk heterojunctions of a high‐performance, low‐gap silicon‐bridged dithiophene polymer with oleic acid capped PbS quantum dots (QDs) are studied to assess the material potential for light harvesting in the visible‐ and IR‐light ranges. By employing a wide range of nanocrystal sizes, systematic dependences of electron and hole transfer on quantum‐dot size are established for the first time on a low‐gap polymer–dot system. The studied system exhibits type II band offsets for dot sizes up to ca. 4 nm, whch allow fast hole transfer from the quantum dots to the polymer that competes favorably with the intrinsic QD recombination. Electron transfer from the polymer is also observed although it is less competitive with the fast polymer exciton recombination for most QD sizes studied. The incorporation of a fullerene derivative provides efficient electron‐quenching sites that improve interfacial polymer‐exciton dissociation in ternary polymer–fullerene–QD blends. The study indicates that programmable band offsets that allow both electron and hole extraction can be produced for efficient light harvesting based on this low‐gap polymer‐PbS QD composite.     

Antipredatory behaviour in lizards: interactions between group size and predation risk

Group size effects on antipredatory behaviour are well documented in numerous animals, but little is known about how the level of predation risk influences this process. We tested the hypothesis that group size and level of risk interact to affect the levels of antipredatory behaviour in the group-living sun skink, Lampropholis delicata. We controlled the size of lizard groups (N=1, 2, 4, 8 or 12 females) and altered predation risk by providing either a basking tile covered with chemical cues from a predator (high risk) or one without scent (low risk). The time allocated to individual antipredatory behaviour decreased significantly with increasing group size. The relation between group size and time allocated to individual antipredatory behaviour was nonlinear and asymptotic, and did not change under low and high risks of predation. However, group size and predation risk interacted to affect significantly the time that lizards allocated to antipredatory behaviour. When the overall risk from predators was high, individual responsiveness decreased strongly as group size became larger. In contrast, when the overall risk from predators was low, individual responsiveness decreased weakly as group size became larger. Consequently, the time that lizards allocated to antipredatory behaviour under different risks of predation converged as group size increased.     

Light-dependent dynamics of gap junctions between horizontal cells in the retina of the crucian carp

Summary The dynamics of gap junctions between outer horizontal cells or their axon terminals in the retina of the crucian carp were investigated during light and dark adaptation by use of ultrathin-section and freeze-fracture electron microscopy. Light adaptation was induced by red light, while dark adaptation took place under ambient dark conditions. The two principal findings were: (1) The density of connexons within an observed gap junction is high in dark-adapted retina, and low in light-adapted retina. This, respectively, may reflect the coupled and uncoupled state of the gap junction. (2) The size of individual gap junctions is larger in light-than in dark-adapted retinae. Whereas the overall area occupied by gap junctions is reduced with dark adaptation, the percentage of small and very small gap junctions increases dramatically. A lateral shift of connexons in the gap junctional membrane is strongly suggested by these reversible processes of densification and dispersion. Two additional possibilities of gap junction modulation are discussed: (1) the de novo formation of very small gap junctions outside the large ones in the first few minutes of dark adaptation, and (2) the rearrangement of a portion of the very large gap junctions. The idea that the cytoskeleton is involved in such modulatory processes is corroborated by thin-section observations.Dedicated to Professor J. Peiffer on the occasion of his 65th birthday     

Effects of dynamic loading on solute transport through the human cartilage endplate

Nutrient and metabolite transport through the cartilage endplate (CEP) is important for maintaining proper disc nutrition, but the mechanisms of solute transport remain unclear. One unresolved issue is the role of dynamic loading. In comparison to static loading, dynamic loading is thought to enhance transport by increasing convection. However, the CEP has a high resistance to fluid flow, which could limit solute convection. Here we measure solute transport through site-matched cadaveric human lumbar CEP tissues under static vs. dynamic loading, and we determine how the degree of transport enhancement from dynamic loading depends on CEP porosity and solute size. We found that dynamic loading significantly increased small and large solute transport through the CEP: on average, dynamic loading increased the transport of sodium fluorescein (376 Da) by a factor of 1.85 ± 0.64 and the transport of a large dextran (4000 Da) by a factor of 4.97 ± 3.05. Importantly, CEP porosity (0.65 ± 0.07; range: 0.47–0.76) strongly influenced the degree of transport enhancement. Specifically, for both solutes, transport enhancement was greater for CEPs with low porosity than for CEPs with high porosity. This is because the CEPs with low porosity were susceptible to larger improvements in fluid flow under dynamic loading. The CEP becomes less porous and less hydrated with aging and as disc degeneration progresses. Together, these findings suggest that as those changes occur, dynamic loading has a greater effect on solute transport through the CEP compared to static loading, and thus may play a larger role in disc nutrition.     

Influence of Phonon Scattering on Exciton and Charge Diffusion in Polymer‐Fullerene Solar Cells

Thermally activated transport and phonon scattering in P3HT:PCBM (poly(3‐hexylthiophene‐2,5‐diyl):[6,6]‐phenylC61‐butyric acid methyl ester) bulk heterojunction (BHJ) organic solar cells is studied via temperature‐dependent external‐quantum‐efficiency (EQE) spectroscopy. The hopping barriers for combined exciton and charge transport are balanced for the individual blended materials in a sample, which possesses a blending ratio and a morphology that give rise to a maximal power‐conversion efficiency. Increasing the PCBM weight fraction leads to a reduction of exciton hopping barriers in PCBM, while for P3HT exciton hopping barriers remain constant. This reduction of PCBM exciton hopping barriers is attributed to a higher PCBM crystallinity in the PCBM‐rich solar cell as compared to the BHJ with the optimized blending ratio. The morphology‐dependent difference in exciton hopping activation energies between P3HT and PCBM is attributed to a higher impact of phonon scattering in P3HT than in PCBM, as concluded from the much stronger decrease of P3HT‐related temperature‐dependent external quantum efficiencies above room temperature in the PCBM‐rich BHJ solar cell. All EQE data of P3HT:PCBM‐based BHJ solar cells is modeled consistently over a broad temperature range by a simple analytical expression involving temperature activation and phonon scattering, without the need to distinguish two separate hopping regimes.     

Optical Properties of Organic Semiconductor Blends with Near‐Infrared Quantum‐Dot Sensitizers for Light Harvesting Applications

We report an optical investigation of conjugated polymer (P3HT)/fullerene (PCBM) semiconductor blends sensitized by near‐infrared absorbing quantum dots (PbS QDs). A systematic series of samples that include pristine, binary and ternary blends of the materials are studied using steady‐state absorption, photoluminescence (PL) and ultrafast transient absorption. Measurements show an enhancement of the absorption strength in the near‐infrared upon QD incorporation. PL quenching of the polymer and the QD exciton emission is observed and predominantly attributed to intermaterial photoinduced charge transfer processes. Pump‐probe experiments show photo‐excitations to relax via an initial ultrafast decay while longer‐lived photoinduced absorption is attributed to charge transfer exciton formation and found to depend on the relative ratio of QDs to P3HT:PCBM content. PL experiments and transient absorption measurements indicate that interfacial charge transfer processes occur more efficiently at the fullerene/polymer and fullerene/nanocrystal interfaces compared to polymer/nanocrystal interfaces. Thus the inclusion of the fullerene seems to facilitate exciton dissociation in such blends. The study discusses important and rather unexplored aspects of exciton recombination and charge transfer processes in ternary blend composites of organic semiconductors and near‐infrared quantum dots for applications in solution‐processed photodetectors and solar cells.     

High‐Voltage Photogeneration Exclusively via Aggregation‐Induced Triplet States in a Heavy‐Atom‐Free Nonplanar Organic Semiconductor

The electron–hole recombination kinetics of organic photovoltaics (OPVs) are known to be sensitive to the relative energies of triplet and charge‐transfer (CT) states. Yet, the role of exciton spin in systems having CT states above 1.7 eV—like those in near‐ultraviolet‐harvesting OPVs—has largely not been investigated. Here, aggregation‐induced room‐temperature intersystem crossing (ISC) to facilitate exciton harvesting in OPVs having CT states as high as 2.3 eV and open‐circuit voltages exceeding 1.6 V is reported. Triplet excimers from energy‐band splitting result in ultrafast CT and charge separation with nonradiative energy losses of <250 meV, suggesting that a 0.1 eV driving force is sufficient for charge separation, with entropic gain via CT state delocalization being the main driver for exciton dissociation and generation of free charges. This finding can inform engineering of next‐generation active materials and films for near‐ultraviolet OPVs with open‐circuit voltages exceeding 2 V. Contrary to general belief, this work reveals that exclusive and efficient ISC need not require heavy‐atom‐containing active materials. Molecular aggregation through thin‐film processing provides an alternative route to accessing 100% triplet states on photoexcitation.     

Modulation of cellulose nanocrystals amphiphilic properties to stabilize oil/water interface

Neutral cellulose nanocrystals dispersed in water were shown in a previous work to stabilize oil/water interfaces and produce Pickering emulsions with outstanding stability, whereas sulfated nanocrystals obtained from cotton did not show interfacial properties. To develop a better understanding of the stabilization mechanism, amphiphilic properties of the nanocrystals were modulated by tuning the surface charge density to investigate emulsifying capability on two sources of cellulose: cotton linters (CCN) and bacterial cellulose (BCN). This charge adjustment made it possible to determine the conditions where a low surface charge density, below 0.03 e/nm(2), remains compatible with emulsification, as well as when assisted by charge screening regardless of the source. This study discusses this ability to stabilize oil-in-water emulsions for cellulose nanocrystals varying in crystalline allomorph, morphology, and hydrolysis processes related to the amphiphilic character of nonhydrophobized cellulose nanocrystal.     

A Bottom‐Up Approach toward All‐Solution‐Processed High‐Efficiency Cu(In,Ga)S2 Photocathodes for Solar Water Splitting

The development of solution‐processable routes to prepare efficient photoelectrodes for water splitting is highly desirable to reduce manufacturing costs. Recently, sulfide chalcopyrites (Cu(In,Ga)S₂) have attracted attention as photocathodes for hydrogen evolution owing to their outstanding optoelectronic properties and their band gap—wider than their selenide counterparts—which can potentially increase the attainable photovoltage. A straightforward and all‐solution‐processable approach for the fabrication of highly efficient photocathodes based on Cu(In,Ga)S₂ is reported for the first time. It is demonstrated that semiconductor nanocrystals can be successfully employed as building blocks to prepare phase‐pure microcrystalline thin films by incorporating different additives (Sb, Bi, Mg) that promote the coalescence of the nanocrystals during annealing. Importantly, the grain size is directly correlated to improved charge transport for Sb and Bi additives, but it is shown that secondary effects can be detrimental to performance even with large grains (for Mg). For optimized electrodes, the sequential deposition of thin layers of n‐type CdS and TiO₂ by solution‐based methods, and platinum as an electrocatalyst, leads to stable photocurrents saturating at 8.0 mA cm^–2 and onsetting at ≈0.6 V versus RHE under AM 1.5G illumination for CuInS₂ films. Electrodes prepared by our method rival the state‐of‐the‐art performance for these materials.     

The Effect of Temperature on Photo-induced Carotenoid Biosynthesis in Neurospora crassa

The temperature dependence of carotenoid synthesis in Neurospora crassa was investigated. The primary light reaction is independent of temperature, but the amount of carotenoid pigment which subsequently accumulates in the dark is strongly dependent on the temperature during the dark incubation. Carotenoid synthesis shows a sensitivity to both high and low temperatures, and of the temperatures tested, 6 C is optimal. Exposure to temperatures above 6 C for various times immediately following irradiation brings about a temperature-dependent reduction in the amount of carotenoid pigment that is synthesized in a total dark incubation time of 24 hours. This sensitivity to incubations at temperatures above 6 C is reduced by either continuous irradiation during the entire time at the higher temperature or by a short irradiation at the end of this period, and the relative effectiveness of these two types of light treatments is presented. Carotenoid production is also sensitive to amino acid analogues and inhibitors of protein synthesis during a critical period after irradiation.     

Solution‐Processed TiO2 Nanoparticles as the Window Layer for CuIn(S,Se)2 Devices

As a wide‐bandgap semiconductor, titanium dioxide (TiO₂) with a porous structure has proven useful in dye‐sensitized solar cells, but its application in low‐cost, high‐efficiency inorganic photovoltaic devices based on materials such as Cu(InGa)Se₂ or Cu₂ZnSnS₄ is limited. Here, a thin film made from solution‐processed TiO₂ nanocrystals is demonstrated as an alternative to intrinsic zinc oxide (i‐ZnO) as the window layer of CuInS_xSe_1?x solar cells. The as‐synthesized, well‐dispersed, 6 nm TiO₂ nanocrystals are assembled into thin films with controllable thicknesses of 40, 80, and 160 nm. The TiO₂ nanocrystal films with thicknesses of 40 and 80 nm exhibit conversion efficiencies (6.2% and 6.33%, respectively) that are comparable to that of a layer of the typical sputtered i‐ZnO (6.42%). The conversion efficiency of the devices with a TiO₂ thickness of 160 nm decreases to 2.2%, owing to the large series resistance. A 9‐hour reaction time leads to aggregated nanoparticles with a much‐lower efficiency (2%) than that of the well‐dispersed TiO₂ nanoparticles prepared using a 15‐hour reaction time. Under optimized conditions, the champion TiO₂ nanocrystal‐film‐based device shows even higher efficiency (9.2%) than a control device employing a typical i‐ZnO film (8.6%).     

Size and growth relationships in juvenile steelhead: The advantage of large relative size diminishes with increasing water temperatures

In territorial stream salmonids, asymmetric competition can perpetuate individual size differences over time, but the extent to which this is manifested can be environmentally mediated. Here we study the variation in juvenile steelhead (Oncorhynchus mykiss) growth rates to identify the conditions (population density and water temperature) under which an individual’s size relative to its conspecifics conferred an advantage. Among steelhead rearing in the same stream section we found that relatively larger individuals on average grew faster than smaller conspecifics. However, comparing across stream sections there was a negative interaction between relative size and water temperature. The effect of an individual’s relative size on its growth rate decreased as temperatures were increasing, indicating that the advantages of being large diminished during periods of high temperatures or in locations with relatively higher temperatures. Compared to temperature, the effects of population density on the growth rate were less substantial. The results suggest that larger individuals on average acquire more resources than smaller individuals, and demonstrate that water temperature exerts an important, modulating control over growth performance in heterogeneous environments.     

Rational Core–Shell Design of Open Air Low Temperature In Situ Processable CsPbI3 Quasi‐Nanocrystals for Stabilized p‐i‐n Solar Cells

As a promising alternative, inorganic perovskite nanocrystals allow reinforced stability of photovoltaic device. Unfortunately, directly assembling these nanocrystals into film is uncontrollable. Instead, in situ assembling technology under low temperature in open air is attractive but limited due to the tendency of nonperovskite transition. The adverse shell ligands and unstable core lattices are known as the fundamental problems. In order to address this issue, here proposed is a rational core–shell design: 1) with respect to ligands, a new one, 4‐fluorophenethylammonium iodide, is used to enhance bonding force and charge coupling between ligands and nanocrystals; 2) with respect to lattices, a novel compound H₂PbI₄ is employed to assist divalent ion (Mn²⁺) doping into perovskite lattices. By low temperature in situ processing CsPbI₃ quasi‐nanocrystal film, the highest power conversion efficiency of 13.4% for p‐i‐n solar cells is achieved, which retains 92% after 500 h in ambient air. The current study underlines the significance of rational hierarchical design of inorganic perovskite nanocrystals, especially for low temperature in situ processable electronic devices.     

Laser‐Generated Nanocrystals in Perovskite: Universal Embedding of Ligand‐Free and Sub‐10 nm Nanocrystals in Solution‐Processed Metal Halide Perovskite Films for Effectively Modulated Optoelectronic Performance

Regulating the chemical/physical features of solution processed metal halide perovskite films by integrating sub‐10 nm nanocrystals is a highly promising strategy to advance their outstanding optoelectronic performance. However, significant challenges remain for the universal embedding of the well‐defined nanocrystals in the film matrix. By generating nanocrystals in desired solvents via pulsed laser irradiation in liquid, the authors demonstrate the effective decoration of sub‐10 nm nanocrystals in perovskite films for enhanced optoelectronic performance. It is believed that this improved performance is due to the modification of the widely adopted “antisolvent” to a novel “anti‐colloidal‐solution” (ACS). Exemplified by a typical ACS; carbon dots in chlorobenzene, its encouraging superiority in regulating, not only the films morphology, but also the electronic structure, is demonstrated. This results in perovskite solar cells with a champion efficiency of 21.41% as well as a pronounced stability over 5000 h in relative humidity of 40%. The capability of nanocrystal embedding for boosted photovoltaic performance is further exploited by employing other laser generated ACSs. Such a strategy may open up a route to regulating hybrid perovskite film performance via nanocrystal embedding for photovoltaics or even beyond optoelectronic applications.