Halide Perovskite Quantum Dots Research Articles

Sensitive detection of bilirubin using highly luminescent benzylamine capped CH3NH3PbBr3 perovskite quantum dots

Luminescent organic–inorganic metal halide hybrid perovskite quantum dots (PQDs) as a new class of fluorophores are finding increasing attention towards chemical and biological sensing due to their exceptional photophysical properties. Herein, we synthesized highly fluorescent CH3NH3PbBr3 perovskite quantum dots (B-PQDs) through the ligand assisted reprecipitation method (LARP), using benzylamine as the surface capping ligand. Morphological and opto-structural properties of the as-synthesized B-PQDs were thoroughly investigated using high resolution transmission electron microscopy (HR-TEM), X-Ray diffraction (XRD), Fourier transform infra-red spectroscopy (FT-IR), UV–Vis absorption, and fluorescence spectroscopy. The as-synthesized electron-rich amine-capped B-PQDs were employed to study their sensing response towards bilirubin (BL). The aromatic amine capped B-PQDs enhance the sensory response towards BL due to the π-π interaction with BL’s conjugated system. The B-PQDs were found to be highly sensitive towards BL with a stern–volmer constant value ≈ 4.3 × 104 M−1 and limit of detection of 0.42 μM. A panel of characterizations were carried out to investigate the detailed sensing mechanism where resonance energy transfer was found to be the dominant quenching mechanism for BL detection. Our results demonstrated the potential for utilizing organic–inorganic halide perovskite quantum dots for sensing applications, through surface ligand modification tailored for detecting specific analytes.

Photoinduced Dehalogenation‐Based Direct In Situ Photolithography of CsPbBr3 Quantum Dots Micropatterns for Encryption and Anti‐Counterfeiting with High Capacity

Fluorescent lead halide perovskite quantum dots (LH PQDs) micropatterns hold great potential for photonic applications. However, current photolithography for LH PQDs micropatterning is hindered by their incompatibility with traditional photolithography methods, which involve development processes using numerous solvents and exhibit poor stability due to the ionic characteristics of LH PQDs. Herein, a direct in situ photolithography to fabricate CsPbBr3 PQDs micropatterns based on ultraviolet‐C light‐driven debromination is developed. Using this approach, fluorescent CsPbBr3 PQDs micropatterns with high theoretical information storage capacity (up to 10750205) can be achieved in a single step, without the need for tedious development processes. Furthermore, the fabricated CsPbBr3 PQDs micropatterns show high stability, remaining undamaged even after immersion in water for 6 months. The combination of excellent optical properties, development‐free process, high stability, and low cost makes the in situ photolithography strategy very promising for patterning LH PQDs toward photonic integrations.

3D‐cavity‐confined CsPbBr3 quantum dots for visible‐light‐driven photocatalytic C(sp3)–H bond activation

AbstractMetal halide perovskite (MHP) quantum dots (QDs) offer immense potential for several areas of photonics research due to their easy and low‐cost fabrication and excellent optoelectronic properties. However, practical applications of MHP QDs are limited by their poor stability and, in particular, their tendency to aggregate. Here, we develop a two‐step double‐solvent strategy to grow and confine CsPbBr3 QDs within the three‐dimensional (3D) cavities of a mesoporous SBA‐16 silica scaffold (CsPbBr3@SBA‐16). Strong confinement and separation of the MHP QDs lead to a relatively uniform size distribution, narrow luminescence, and good ambient stability over 2 months. In addition, the CsPbBr3@SBA‐16 presents a high activity and stability for visible‐light‐driven photocatalytic toluene C(sp3)–H bond activation to produce benzaldehyde with ∼730 µmol g−1 h−1 yield rate and near‐unity selectivity. Similarly, the structural stability of CsPbBr3@SBA‐16 QDs is superior to that of both pure CsPbBr3 QDs and those confined in MCM‐41 with 1D channels.

High‐Efficiency Single‐Photon Upconversion Photoluminescence of Perovskite Quantum Dots via Intragap State Regulation

AbstractLead halide perovskite quantum dots (PQDs) have shown remarkable single‐photon upconversion photoluminescence (SPUC‐PL) bringing them a brilliant perspective as the active media for biological imaging, optiag, and upconversion photovoltaics. However, the mechanism of SPUC in PQDs is still in dispute, and the specific strategy for optimizing PQDs toward a higher SPUC performance has yet to be established, which impedes the application of PQDs‐based SPUC‐PL in practice. In this work it is revealed that the PL quantum yield is declined by surface trap states, while the SPUC efficiency is promoted by Urbach tail states. These two types of intragap states can be chemically manipulated by engineering the surface ligand and the growth kinetics of perovskite nanocrystals, bringing on the improvement of light emission efficiency and the promotion of subgap low‐energy photon absorption, respectively. As a proof of concept, utilizing the synergistic effect of the proposed chemical manipulation method, the SPUC‐PL efficiency of PQDs is boosted by more than 40%, which gives rise to a spectral window of optical refrigeration gain as broad as ≈130 meV.

Defect Engineering Strategy for Superior Integration of Metal-Organic Framework and Halide Perovskite as a Fluorescence Sensing Material.

Combining halide perovskite quantum dots (QDs) and metal-organic frameworks (MOFs) material is challenging when the QDs' size is larger than the MOFs' nanopores. Here, we adopted a simple defect engineering approach to increase the size of zeolitic imidazolate framework 90 (ZIF-90)'s pores size to better load CH3NH3PbBr3 perovskite QDs. This defect structure effect can be easily achieved by adjusting the metal-to-ligand ratio throughout the ZIF-90 synthesis process. The QDs are then grown in the defective structure, resulting in a hybrid ZIF-90-perovskite (ZP) composite. The QDs in ZP composites occupied the gap of 10-18 nm defective ZIF-90 crystal and interestingly isolated the QDs with high stability in aqueous solution. We also investigated the relationship between defect engineering and fluorescence sensing, finding that the aqueous Cu2+ ion concentration was directly correlated to defective ZIF-90 and ZP composites. We also found that the role of the O-Cu coordination bonds and CH3NHCu+ species formation in the materials when they reacted with Cu2+ was responsible for this relationship. Finally, this strategy was successful in developing Cu2+ ion fluorescence sensing in water with better selectivity and sensitivity.

Weakly Confined Organic-Inorganic Halide Perovskite Quantum Dots as High-Purity Room-Temperature Single Photon Sources.

Colloidal perovskite quantum dots (PQDs) have emerged as highly promising single photon emitters for quantum information applications. Presently, most strategies have focused on leveraging quantum confinement to increase the nonradiative Auger recombination (AR) rate to enhance single-photon (SP) purity in all-inorganic CsPbBr3 QDs. However, this also increases the fluorescence intermittency. Achieving high SP purity and blinking mitigation simultaneously remains a significant challenge. Here, we transcend this limitation with room-temperature synthesized weakly confined hybrid organic-inorganic perovskite (HOIP) QDs. Superior single photon purity with a low g(2)(0) < 0.07 ± 0.03 and a nearly blinking-free behavior (ON-state fraction >95%) in 11 nm FAPbBr3 QDs are achieved at room temperature, attributed to their long exciton lifetimes (τX) and short biexciton lifetimes (τXX). The significance of the organic A-cation is further validated using the mixed-cation FAxCs1-xPbBr3. Theoretical calculations utilizing a combination of the Bethe-Salpeter (BSE) and k·p approaches point toward the modulation of the dielectric constants by the organic cations. Importantly, our findings provide valuable insights into an additional lever for engineering facile-synthesized room-temperature PQD single photon sources.

CsPbBr3 perovskite quantum dots-based Janus membrane with multifunction of luminescence, magnetism and aeolotropic electroconductivity

Lead halide perovskite quantum dots (QDs) are promising semiconductors for next-generation photoelectric devices. However, the development of perovskite QDs-based multifunctional materials still needs to be addressed in order to further advance the application of perovskite QDs. Herein, a successful synthesis of Janus microfibers array Janus membrane (JMAJM) with up-down structure and multifunction of luminescence, magnetism and electroconductivity is firstly achieved based on CsPbBr3 QDs through a parallel electrospinning. JMAJM comprises up-down two layers tightly bonded together. The up-layer of JMAJM is luminescence/magnetism Janus microfibers array (L/M-JMAJM) constructed by [CsPbBr3/polymethyl methacrylate (PMMA)]//[CoFe2O4/PMMA] Janus microfibers as building elements. The down-layer of JMAJM is luminescence/electroconductivity Janus microfibers array (L/E-JMAJM) fabricated by [CsPbBr3/PMMA]//[polyaniline (PANI)/PMMA] Janus microfibers as building elements. Two independent microcosmic regions are designed and realized in a Janus microfiber, confining luminescence with magnetic or conductive substances into their respective regions, thus minimizing adverse effects of other dark-colored functional substances on the fluorescence of CsPbBr3 QDs. This peculiar Janus microfiber enables the effective separation and high integration of CsPbBr3 QDs with other functional substances. The up-down structure of JMAJM ensures a high integration of luminescence, magnetism and conductivity. Meanwhile, JMAJM addresses the environmental instability of CsPbBr3 QDs while simultaneously endows perovskite QDs-based materials with additional functions to realize multifunction. Under ultraviolet excitation, fluorescence characteristics of the CsPbBr3 QDs in JMAJM are maintained, exhibiting a vibrant green emission at 517 nm. Meanwhile, JMAJM achieves a maximum saturation magnetization of 20.32 emu·g−1, high conductance of 10-2 S and aeolotropic electroconductivity degree of 107. The combination of micro-partition with macro-partition in JMAJM receives superior concurrent luminescence-magnetic-conductive multifunction. This work provides a novel idea and strategy for advancing perovskite QDs-based multifunctional materials.

Atomically Contacted Cs3Bi2Br9 QDs@UiO-66 Composite for Photocatalytic CO2 Reduction.

Metal halide perovskite quantum dots (QDs) are widely studied in the field of photocatalytic CO2 due to their strong light absorption and long carrier migration length. However, it can not exhibit high catalytic performance because of the radiative recombination and the lack of effective catalytic sites. Metal organic frameworks (MOFs) encapsulated QDs can not only solve the aforementioned problems, but also maintain their own unique characteristics with ultra-high specific surfaces area and abundant metal sites. In this work, lead-free bismuth-based halide perovskite QDs are encapsulated into Zr-based MOF (UiO-66), which combines the advantages with high power conversion efficiency of QDs and the high surface area and porosity of UiO-66. In addition, benefiting from the close contact between the Cs3Bi2Br9 QDs and the UiO-66 enables the photogenerated electrons in the QDs to be rapidly transferred to the MOF. As a result, the Cs3Bi2Br9@UiO-66 composite exhibits a higher yield for photocatalytic CO2 reduction than that of the prepared large-sized composite of Cs3Bi2Br9 and UiO-66.

Universal Surface Repairing Strategy Enabling Suppressed Auger Recombination in CsPbBr3 Perovskite Quantum Dots for Low Threshold Lasing in a Superlattice Microcavity

AbstractLead halide perovskite quantum dots (LHP QDs) emerge as versatile photonic sources in electroluminescence and laser devices. Their applications in optoelectronic devices are hindered by surface distortion and ligand stripping during the purification process. In addition, the device performance roll‐off suffers from the ultrafast non‐radiative Auger recombination (AR). To address these issues, herein, CsPbBr3 QDs are prepared with sizes ranging from 6.5 to 9.2 nm and the universal surface repairing strategy is proved to efficiently increase the biexciton lifetime and quantum yield up to 1.4 and 3 times, respectively. The strategy provides a PbBrx rich surface and strong binding didodecyldimethylammonium bromide (DDAB) ligands to achieve near‐unity photoluminescence efficiency, which significantly improves their stability against anti‐solvents and aging in ambient conditions. A single‐mode laser device is realized by self‐assembling the QDs into superlattice as optical microcavity, with low threshold of 9.45 µJ cm−2, quality factor of 2187 and ultrafast lifetime of 3.22 ps. The superlattice laser is demonstrated as an optical encoder with large coding bandwidth of 0.133 THz. This work proposes new insight into the non‐radiative AR process in these single‐component CsPbBr3 QDs, and will pave the way for optoelectronic devices working in intense conditions.

ZnS-coated Yb3+-doped perovskite quantum dots: A stable and efficient quantum cutting photon energy converter for silicon-based electronics

Yb3+ doped lead halide perovskite quantum dots (PeQDs) with efficient quantum cutting emission are thought to be the most promising photon energy converter for improving the performance of silicon-based electronics. Nevertheless, the low external quantum efficiency (EQE) and instability make it unfeasible for industrial use. Here, we present a unique PeQDs@ ZnS core–shell device that achieves outstanding stability and up to 39 % EQE by effectively controlling energy transfer from the PeQDs to the Yb3+ through ZnS coating. These advances are attributed to the large UV absorption and the strong localized effect of the ZnS shells on the conduction band electrons of the PeQDs. Density functional theory (DFT) first-principles simulations indicate that ZnS coating can facilitate the energy transfer of PeQDs to Yb3+. Power conversion efficiency (PCE) of silicon solar cells was significantly enhanced by ZnS-coated Yb3+ doped PeQDs, yielding a noteworthy 13.5 % relative PCE improvement over 30 measurement sets. Significantly, the stability of SSCs with ZnS-coated PeQDs films is considerably improved, resulting in a capped device T80 lifespan of up to 11,224 h. Moreover, ZnS-coated PeQDs films can significantly boost the EQE of silicon photodiodes (Si-PDs) and extend their response to deep ultraviolet light. This paper presents an efficient and consistently stable photon energy converter with great commercialization potential.

Highly Luminescent and Stable Perovskite Quantum Dots Films for Light‐Emitting Devices and Information Encryption

AbstractThe inherent flexibility and excellent mechanical strength of lead halide perovskite quantum dots (LHP‐QDs) films have attracted much attention in the fields of flexible lighting, displays, non‐planar x‐ray imaging, and wearable optoelectronics. Unfortunately, the complicated synthesis process and poor stability limit its practical applications, hence there is an urgent need to develop a feasible fabrication process for films to attain high device performance. Herein, a molecular level hybridization of bridged polysilsesquioxane (BPSQ) is designed as matrix to harvest both flexibility of organics and stability of inorganics, resulting in improved interfacial compatibility between the CsPbBr3 QDs and the matrix through chemical bond anchoring. The CsPbBr3@3‐aminopropyl‐triethoxysilane (APTES)@BPSQ films showcase bright narrow‐band photoluminescence, with a photoluminescence quantum yield of 61% and a half‐peak full width at half maximum of &lt;17 nm. Notably, these films demonstrate excellent environmental stability, UV resistance, water stability (experiencing only an 18% decrease in luminescence intensity after 168 h of water immersion), and high‐temperature stability (withstanding temperatures up to 500 K). Furthermore, white light‐emitting diodes (WLEDs) and anti‐counterfeiting patterns have been fabricated using CsPbBr3@APTES@BPSQ, highlighting their wide application potential in flexible light‐emitting devices and information encryption.

Cognitively Driven Autonomous Flow Chemistry for Producing On-Demand Perovskite Quantum Dots Via Advanced Closed-Loop Feedback Control.

Recent developments in the synthesis of hybrid organic-inorganic halide perovskite quantum dots (HP-QDs) through compositional adjustments have highlighted their potential applications in the fields of photovoltaics and light sources due to their unique optoelectronic properties. However, traditional methods to fine-tune their composition involve repetitive, labor-intensive, and costly processes. Herein, the utilization of a continuous flow chemistry approach is developed, in combination with a Proportional-Integral (PI) feedback control system as an effective method for producing on-demand methylammonium lead bromoiodide (MAPbBrx I3-x ) HP-QDs. The PI feedback control allows for real-time optimization of the flow rates of halide precursor solutions (halide PSs), enabling the precise tuning of the emission wavelength of HP-QDs. HP-QDs having an emission wavelength of 550 and 650nm are synthesized through a blue-shifted and red-shifted algorithm, respectively, from any arbitrary reaction condition within 400 s. The iterative process through the PI feedback control produces the target HP-QDs with short rise time and low overshoot. The proposed automatic flow chemistry system integrated with a universal and accessible control algorithm of PI can generate the target HP-QDs with high accuracy, stability, and robustness, demonstrating a significant advancement in constructing an autonomous flow chemistry synthetic system.

Remarkable emission enhancement of CsPbBr3 quantum dots based on an Ag nanoparticle-Ag film plasmonic coupling structure.

All-inorganic halide perovskite quantum dots (QDs) have recently received much attention due to their excellent optoelectronic properties. And their emission properties still need to be improved for further applications. Here, we demonstrated a remarkable emission enhancement of the CsPbBr3 QDs based on an Ag nanoparticle-Ag film plasmonic coupling structure. Through precise control of the gap distance between Ag nanoparticle and Ag film, the localized surface plasmon resonance (LSPR) peak was tuned to match the emission wavelength of the CsPbBr3 QDs. We achieved a 30-fold fluorescence intensity enhancement and a lower lasing threshold, which is 25% of that of the CsPbBr3 QDs without plasmonic coupling structure. It is attributed to that the plasmonic coupling structure exhibits an extremely strong local electric field owing to the coupling between LSPR of Ag nanoparticle and surface plasmon polariton of Ag film. This work provides an effective way to enhance the optical emission of perovskite QDs and promotes the further exploration of on-chip light source.

The future of quantum technologies: superfluorescence from solution-processed, tunable materials

Abstract One of the most significant and surprising recent developments in nanocrystal studies was the observation of superfluorescence from a system of self-assembled, colloidal perovskite nanocrystals [G. Rainò, M. A. Becker, M. I. Bodnarchuk, R. F. Mahrt, M. V. Kovalenko, and T. Stöferle, “Superfluorescence from lead halide perovskite quantum dot superlattices,” Nature, vol. 563, no. 7733, pp. 671–675, 2018]. Superfluorescence is a quantum-light property in which many dipoles spontaneously synchronize in phase to create a collective, synergistic photon emission with a much faster lifetime. Thus, it is surprising to observe this in more inhomogenous systems as solution-processed and colloidal structures typically suffer from high optical decoherence and non-homogeneous size distributions. Here we outline recent developments in the demonstration of superfluorescence in colloidal and solution-processed systems and explore the chemical and materials science opportunities allowed by such systems. The ability to create bright and tunable superfluorescent sources could enable transformative developments in quantum information applications and advance our understanding of quantum phenomena.

APTES and CTAB Synergistic Induce a Heterozygous CsPbBr3/Cs4PbBr6 Perovskite Composite and its Application on the Sensitive Fluorescent Detection of Iodide ions.

Recently, all-inorganic halide perovskite quantum dots (IPQD) as a new fluorescent material with excellent fluorescence properties have attracted wide attention. However, their instability in polar solvents is the main factor hindering their application in analysis. Herein, a heterozygous perovskite (CsPbBr3/Cs4PbBr6) was simultaneously prepared and stabilized by a silylanization strategy using (3-aminopropyl)-triethoxysilane (APTES) and cetyltrimethyl ammonium bromide (CTAB) assisted precipitation encapsulation method. The synthesized CsPbBr3/Cs4PbBr6 emitted an independent fluorescence at 520nm. The obtained CsPbBr3/Cs4PbBr6 exhibited good stability in ethanol/water mixtures. It was used as a fluorescent probe for sensitively detecting iodide ions (I-) by fluorescence quenching mechanism in the concentration range of 1 ~ 70.0 µM with the detection limit (LOD) of 0.83 µM (relative standard deviation (RSD) = 1.33%, n = 20). The simplicity and high selectivity of the proposed fluorescent analysis method were the prominent features. This work could be extended to the other target ion detection by a perovskite fluorescent quenching.

A smartphone-assisted fluorescent sensing platform for ochratoxin A using Mn-doped CsPbBr3 perovskite quantum dots embedded in the mesoporous silica as a ratiometric probe

Food sources are susceptible to contamination with ochratoxin A (OTA), which is a serious threat to human health. Thus, the construction of novel, simple sensing platforms for OTA monitoring is of utmost need. Manganese-doped lead halide perovskite quantum dots encapsulated with mesoporous SiO2 (Mn-CsPbBr3 QDs@SiO2) were prepared here and used as a ratiometric fluorescent probe for OTA. Mn-CsPbBr3 QDs, synthesized at room temperature, exhibit dual emission with maximum wavelengths of 440 and 570 nm and, when embedded in the SiO2 layer, produce a stable and robust photoluminescence signal. By adding OTA to the probe, emission at 440 nm increases while emission at 570 nm decreases, so a ratiometric response is obtained. Experimental variables affecting the probe signal were studied and optimized and the mechanism of sensing was discussed. This ratiometric sensor demonstrated excellent selectivity and low detection limit (4.1 ng/ml) as well as a wide linear range from 5.0 to 250 ng/ml for OTA. A simple portable smartphone-based device was also constructed and applied for the fluorescence assay. With different OTA concentrations, the multicolor transition from pink to blue under a UV lamp led to simple visual and smartphone-assisted sensing of OTA by using a color analyzing application. Satisfactory recoveries in black tea, coffee, moldy fig and flour samples confirmed the reliability of the assay. The accuracy of the probe was proved by comparison of the results with high-performance liquid chromatography (HPLC).

Highly luminescent CsPbX3/PMMA (X=Br, I) composites with improved stability for full-color Micro-LED displays

Inorganic metal halide perovskite quantum dots (PQDs) have recently emerged as promising candidates for color conversion materials in Micro-LED displays, due to their outstanding color purity, high absorption coefficient, tunable emission wavelength. However the inferior stability and undesirable photoluminescence quantum yield (PLQY) restrict their particle applications. Herein, CsPbX3/PMMA (X = Br, I) composites with improved stability and optical performance were successfully prepared by a general and mild in-situ polymerization strategy. The ester carbonyl (CO) group in MMA formed complexes with Pb2+, leading to the in-situ thermal polymerization of polymethyl methacrylate (PMMA) under the action of the initiator. The multifunctional PMMA can efficiently passivate halogen vacancies while acting as a barrier against the degradation caused by heat, water, and oxygen. As a result, the PLQYs and stability of PMMA-coated CsPbX3 PQDs have been significantly improved. When implementing CsPbX3/PMMA/PDMS composites as color conversion layers in Micro-LEDs, they achieve an impressive color gamut of 127.23% with excellent stability. We believe our work will stimulate the exploration of perovskite/polymer composites for industrial Micro-LED applications.

Strong Light-Matter Coupling in Lead Halide Perovskite Quantum Dot Solids.

Strong coupling between lead halide perovskite materials and optical resonators enables both polaritonic control of the photophysical properties of these emerging semiconductors and the observation of fundamental physical phenomena. However, the difficulty in achieving optical-quality perovskite quantum dot (PQD) films showing well-defined excitonic transitions has prevented the study of strong light-matter coupling in these materials, central to the field of optoelectronics. Herein we demonstrate the formation at room temperature of multiple cavity exciton-polaritons in metallic resonators embedding highly transparent Cesium Lead Bromide quantum dot (CsPbBr3-QD) solids, revealed by a significant reconfiguration of the absorption and emission properties of the system. Our results indicate that the effects of biexciton interaction or large polaron formation, frequently invoked to explain the properties of PQDs, are seemingly absent or compensated by other more conspicuous effects in the CsPbBr3-QD optical cavity. We observe that strong coupling enables a significant reduction of the photoemission line width, as well as the ultrafast modulation of the optical absorption, controllable by means of the excitation fluence. We find that the interplay of the polariton states with the large dark state reservoir plays a decisive role in determining the dynamics of the emission and transient absorption properties of the hybridized light-quantum dot solid system. Our results should serve as the basis for future investigations of PQD solids as polaritonic materials.

"Whole-Body" Fluorination for Highly Efficient and Ultra-Stable All-Inorganic Halide Perovskite Quantum Dots.

Inherent "soft" ionic lattice nature of halide perovskite quantum dots (QDs), triggered by the weak Pb-X (X=Cl, Br, I) bond, is recognized as the primary culprit for their serious instability. A promising way is to construct exceedingly strong ionic interaction inside the QDs and increase their crystal cohesive energy by substituting the interior X- with highly electronegative F- , however, which is challenging and hitherto remains unreported. Here, a "whole-body" fluorination strategy is proposed for strengthening the interior bonding architecture of QDs, wherein the F- are uniformly distributed throughout the whole nanocrystal encompassing both the interior lattice and surface, successfully stabilizing their "soft" crystal lattice and passivating surface defects. This approach effectively mitigates their intrinsic instability issues including light-induced phase segregation. As a result, light-emitting devices based on these QDs exhibit exceptional efficiency and remarkable stability.

“Whole‐Body” Fluorination for Highly Efficient and Ultra‐Stable All‐Inorganic Halide Perovskite Quantum Dots

AbstractInherent “soft” ionic lattice nature of halide perovskite quantum dots (QDs), triggered by the weak Pb−X (X=Cl, Br, I) bond, is recognized as the primary culprit for their serious instability. A promising way is to construct exceedingly strong ionic interaction inside the QDs and increase their crystal cohesive energy by substituting the interior X− with highly electronegative F−, however, which is challenging and hitherto remains unreported. Here, a “whole‐body” fluorination strategy is proposed for strengthening the interior bonding architecture of QDs, wherein the F− are uniformly distributed throughout the whole nanocrystal encompassing both the interior lattice and surface, successfully stabilizing their “soft” crystal lattice and passivating surface defects. This approach effectively mitigates their intrinsic instability issues including light‐induced phase segregation. As a result, light‐emitting devices based on these QDs exhibit exceptional efficiency and remarkable stability.