2D Perovskites with Giant Excitonic Optical Nonlinearities for High‐Performance Sub‐Bandgap Photodetection

Two‐dimensional (2D) perovskites have proved to be promising semiconductors for photovoltaics, photonics, and optoelectronics. Here, a strategy is presented toward the realization of highly efficient, sub‐bandgap photodetection by employing excitonic effects in 2D Ruddlesden–Popper‐type halide perovskites (RPPs). On near resonance with 2D excitons, layered RPPs exhibit degenerate two‐photon absorption (D‐2PA) coefficients as giant as 0.2–0.64 cm MW^?1. 2D RPP‐based sub‐bandgap photodetectors show excellent detection performance in the near‐infrared (NIR): a two‐photon‐generated current responsivity up to 1.2 × 10⁴ cm² W^?2 s^?1, two orders of magnitude greater than InAsSbP‐pin photodiodes; and a dark current as low as 2 pA at room temperature. More intriguingly, layered‐RPP detectors are highly sensitive to the light polarization of incoming photons, showing a considerable anisotropy in their D‐2PA coefficients (β_[001]/β_[011] = 2.4, 70% larger than the ratios reported for zinc‐blende semiconductors). By controlling the thickness of the inorganic quantum well, it is found that layered RPPs of (C₄H₉NH₃)₂(CH₃NH₃)Pb₂I₇ can be utilized for three‐photon photodetection in the NIR region.     

Near‐Infrared Excitation/Emission and Multiphoton‐Induced Fluorescence of Carbon Dots

Carbon dots (CDs) have significant potential for use in various fields including biomedicine, bioimaging, and optoelectronics. However, inefficient excitation and emission of CDs in both near‐infrared (NIR‐I and NIR‐II) windows remains an issue. Solving this problem would yield significant improvement in the tissue‐penetration depth for in vivo bioimaging with CDs. Here, an NIR absorption band and enhanced NIR fluorescence are both realized through the surface engineering of CDs, exploiting electron‐acceptor groups, namely molecules or polymers rich in sulfoxide/carbonyl groups. These groups, which are bound to the outer layers and the edges of the CDs, influence the optical bandgap and promote electron transitions under NIR excitation. NIR‐imaging information encryption and in vivo NIR fluorescence imaging of the stomach of a living mouse using CDs modified with poly(vinylpyrrolidone) in aqueous solution are demonstrated. In addition, excitation by a 1400 nm femtosecond laser yields simultaneous two‐photon‐induced NIR emission and three‐photon‐induced red emission of CDs in dimethyl sulfoxide. This study represents the realization of both NIR‐I excitation and emission as well as two‐photon‐ and three‐photon‐induced fluorescence of CDs excited in an NIR‐II window, and provides a rational design approach for construction and clinical applications of CD‐based NIR imaging agents.     

On the inverse of generalized λ‐matrices with singular leading term

An algorithm is introduced for the inverse of a λ‐matrix given as the truncated series A ₀?iλ A ₁?λ² A ₂+iλ³ A ₃+λ⁴ A ₄+···+O(λⁿ⁺¹) with square coefficient matrices and singular leading term A ₀. Moreover, A ₁ may be conditionally singular and no restrictions are made for the remaining terms. The result is a λ‐matrix given as a unique, truncated series of the same error order. Motivation for this problem is the evaluation of the frequency‐dependent stiffness matrix of general boundary or macro‐finite elements in the frame of a hybrid variational formulation that is based on a flexibility matrix F expressed as a truncated power series of the circular frequency ω. Copyright © 2005 John Wiley & Sons, Ltd.     

Semiconducting Polymer Nanoparticles for Centimeters‐Deep Photoacoustic Imaging in the Second Near‐Infrared Window

Thienoisoindigo‐based semiconducting polymer with a strong near‐infrared absorbance is synthesized and its water‐dispersed nanoparticles (TSPNs) are investigated as a contrast agent for photoacoustic (PA) imaging in the second near‐infrared (NIR‐II) window (1000–1350 nm). The TSPNs generate a strong PA signal in the NIR‐II optical window, where background signals from endogenous contrast agents, including blood and lipid, are at the local minima. By embedding a TSPN‐containing tube in chicken‐breast tissue, an imaging depth of more than 5 cm at 1064 nm excitation is achieved with a contrast‐agent concentration as low as 40 µg mL^?1. The TSPNs under the skin or in the tumor are clearly visualized at 1100 and 1300 nm, with negligible interference from the tissue background. TSPN as a PA contrast in the NIR‐II window opens new opportunities for biomedical imaging of deep tissues with improved contrast.     

Core–Satellite Polydopamine–Gadolinium‐Metallofullerene Nanotheranostics for Multimodal Imaging Guided Combination Cancer Therapy

Integration of magnetic resonance imaging (MRI) and other imaging modalities is promising to furnish complementary information for accurate cancer diagnosis and imaging‐guided therapy. However, most gadolinium (Gd)–chelator MR contrast agents are limited by their relatively low relaxivity and high risk of released‐Gd‐ions‐associated toxicity. Herein, a radionuclide‐⁶⁴Cu‐labeled doxorubicin‐loaded polydopamine (PDA)–gadolinium‐metallofullerene core–satellite nanotheranostic agent (denoted as CDPGM) is developed for MR/photoacoustic (PA)/positron emission tomography (PET) multimodal imaging‐guided combination cancer therapy. In this system, the near‐infrared (NIR)‐absorbing PDA acts as a platform for the assembly of different moieties; Gd₃N@C₈₀, a kind of gadolinium metallofullerene with three Gd ions in one carbon cage, acts as a satellite anchoring on the surface of PDA. The as‐prepared CDPGM NPs show good biocompatibility, strong NIR absorption, high relaxivity (r ₁ = 14.06 mM^?1 s^?1), low risk of release of Gd ions, and NIR‐triggered drug release. In vivo MR/PA/PET multimodal imaging confirms effective tumor accumulation of the CDPGM NPs. Moreover, upon NIR laser irradiation, the tumor is completely eliminated with combined chemo‐photothermal therapy. These results suggest that the CDPGM NPs hold great promise for cancer theranostics.     

N‐Type 2D Organic Single Crystals for High‐Performance Organic Field‐Effect Transistors and Near‐Infrared Phototransistors

Organic field‐effect transistors and near‐infrared (NIR) organic phototransistors (OPTs) have attracted world's attention in many fields in the past decades. In general, the sensitivity, distinguishing the signal from noise, is the key parameter to evaluate the performance of NIR OPTs, which is decided by responsivity and dark current. 2D single crystal films of organic semiconductors (2DCOS) are promising functional materials due to their long‐range order in spite of only few molecular layers. Herein, for the first time, air‐stable 2DCOS of n‐type organic semiconductors (a furan‐thiophene quinoidal compound, TFT‐CN) with strong absorbance around 830 nm, by the facile drop‐casting method on the surface of water are successfully prepared. Almost millimeter‐sized TFT‐CN 2DCOS are obtained and their thickness is below 5 nm. A competitive field‐effect electron mobility (1.36 cm² V^?1 s^?1) and high on/off ratio (up to 10⁸) are obtained in air. Impressively, the ultrasensitive NIR phototransistors operating at the off‐state exhibit a very low dark current of ≈0.3 pA and an ultrahigh detectivity (D*) exceeding 6 × 10¹⁴ Jones because the devices can operate in full depletion at the off‐state, superior to the majority of the reported organic‐based NIR phototransistors.     

Mixed Lead–Tin Halide Perovskites for Efficient and Wavelength‐Tunable Near‐Infrared Light‐Emitting Diodes

Near‐infrared (NIR) light‐emitting diodes (LEDs), with emission wavelengths between 800 and 950 nm, are useful for various applications, e.g., night‐vision devices, optical communication, and medical treatments. Yet, devices using thin film materials like organic semiconductors and lead based colloidal quantum dots face certain fundamental challenges that limit the improvement of external quantum efficiency (EQE), making the search of alternative NIR emitters important for the community. In this work, efficient NIR LEDs with tunable emission from 850 to 950 nm, using lead–tin (Pb‐Sn) halide perovskite as emitters are demonstrated. The best performing device exhibits an EQE of 5.0% with a peak emission wavelength of 917 nm, a turn‐on voltage of 1.65 V, and a radiance of 2.7 W Sr^?1 m^?2 when driven at 4.5 V. The emission spectra of mixed Pb‐Sn perovskites are tuned either by changing the Pb:Sn ratio or by incorporating bromide, and notably exhibit no phase separation during device operation. The work demonstrates that mixed Pb‐Sn perovskites are promising next generation NIR emitters.     

Giant and Broadband Multiphoton Absorption Nonlinearities of a 2D Organometallic Perovskite Ferroelectric

Multiphoton absorption (MPA) has been utilized for important technological applications. High-order multiphoton harvesting (e.g., five-photon absorption, 5PA) exhibits unique properties that could benefit biophotonics. Within this field, perovskite oxide ferroelectrics (e.g., BaTiO₃) enable low-order optical nonlinearities of 2PA/3PA processes. However, it is challenging to obtain efficient, high-order 5PA effects. Herein, for the first time, giant and broadband MPA properties are presented in the 2D hybrid perovskite ferroelectric (IA)₂(MA)₂Pb₃Br₁₀ ( 1 ; IA = isoamylammonium and MA = methylammonium), where multiphoton-excited optical nonlinearities related to different MPA mechanisms over a broadband range of 550–2400 nm are observed. Strikingly, its 5PA absorption cross-section (σ₅) reaches up to 1.2 × 10⁻¹³² cm¹⁰ s⁴ photon⁻⁴ (at 2400 nm), almost 10 orders larger than some state-of-the-art organic molecules and a record-high value among all known ferroelectrics. This unprecedented 5PA effect results from the quantum-confined motif of inorganic trilayer sheets (wells) and organic cations (barriers) in 1 . Moreover, its large ferroelectric polarization of 5 µC cm⁻² could promote modulation of MPA effects under external electric fields. As far as it is known, this is the first report on giant, broadband high-order MPA properties in ferroelectrics, which provides potential, novel electric-ordered materials for next-generation biophotonic applications.     

π‐Conjugated Polymer–Fullerene Covalent Hybrids via Ambient Conditions Diels–Alder Ligation

The established ability of graphitic carbon‐nanomaterials to undergo ambient condition Diels–Alder reactions with cyclopentadienyl (Cp) groups is herein employed to prepare fullerene‐polythiophene covalent hybrids with improved electron transfer and film forming characteristics. A novel precisely designed polythiophene (M _n 9.8 kD, ? 1.4) with 17 mol% of Cp‐groups bearing repeat unit is prepared via Grignard metathesis polymerization. The UV/Vis absorption and fluorescence (λ_ex 450 nm) characteristics of polythiophene with pendant Cp‐groups (λ_max 447 nm, λ_e‐max 576 nm) are comparable to the reference poly(3‐hexylthiophene) (λ_max 450 nm, λ_e‐max 576 nm). The novel polythiophene with pendant Cp‐groups is capable of producing solvent‐stable free‐standing polythiophene films, and non‐solvent assisted self‐assemblies resulting in solvent‐stable nanoporous‐microstructures. ¹H‐NMR spectroscopy reveals an efficient reaction of the pendant Cp‐groups with C₆₀. The UV/Vis spectroscopic analyses of solution and thin films of the covalent and physical hybrids disclose closer donor‐acceptor packing in the case of covalent hybrids. AFM images evidence that the covalent hybrids form smooth films with finer lamellar‐organization. The effect is particularly remarkable in the case of poorly soluble C₆₀. A significant enhancement in photo‐voltage is observed for all devices constituted of covalent hybrids, highlighting novel avenues to developing efficient electron donor‐acceptor combinations for light harvesting systems.     

Novel Mn3[Co(CN)6]2@SiO2@Ag Core–Shell Nanocube: Enhanced Two‐Photon Fluorescence and Magnetic Resonance Dual‐Modal Imaging‐Guided Photothermal and Chemo‐therapy

The versatile Mn₃[Co(CN)₆]₂@SiO₂@Ag core–shell NCs are prepared by a simple coprecipitation method. Ag nanoparticles with an average diameter of 12 nm deposited on the surface of Mn₃[Co(CN)₆]₂@SiO₂ through S–Ag bonding are fabricated in ethanol solution by reducing silver nitrate (AgNO₃) with NaBH₄. The NCs possess T₁–T₂ dual‐modal magnetic resonance imaging ability. The inner Prussian blue analogs (PBAs) Mn₃[Co(CN)₆]₂ exhibit bright two‐photon fluorescence (TPF) imaging when excited at 730 nm. Moreover, the TPF imaging intensity displays 1.85‐fold enhancement after loading of Ag nanoparticles. Besides, the sample also has multicolor fluorescence imaging ability under 403, 488, and 543 nm single photon excitation. The as‐synthesized Mn₃[Co(CN)₆]₂@SiO₂@Ag NCs show a DOX loading capacity of 600 mg g⁻¹ and exhibit an excellent ability of near‐infrared (NIR)‐responsive drug release and photothermal therapy (PTT) which is induced from the relative high absorbance in NIR region. The combined chemotherapy and PTT against cancer cells in vitro test shows high therapeutic efficiency. The multimodal treatment and imaging could lead to this material a potential multifunctional system for biomedical diagnosis and therapy.     

One‐Step Synthesis of Monodispersed Mesoporous Carbon Nanospheres for High‐Performance Flexible Quasi‐Solid‐State Micro‐Supercapacitors

Cost‐effective synthesis of carbon nanospheres with a desirable mesoporous network for diversified energy storage applications remains a challenge. Herein, a direct templating strategy is developed to fabricate monodispersed N‐doped mesoporous carbon nanospheres (NMCSs) with an average particle size of 100 nm, a pore diameter of 4 nm, and a specific area of 1093 m² g^?1. Hexadecyl trimethyl ammonium bromide and tetraethyl orthosilicate not only play key roles in the evolution of mesopores but also guide the assembly of phenolic resins to generate carbon nanospheres. Benefiting from the high surface area and optimum mesopore structure, NMCSs deliver a large specific capacitance up to 433 F g^?1 in 1 m H₂SO₄. The NMCS electrodes–based symmetric sandwich supercapacitor has an output voltage of 1.4 V in polyvinyl alcohol/H₂SO₄ gel electrolyte and delivers an energy density of 10.9 Wh kg^?1 at a power density of 14014.5 W kg^?1. Notably, NMCSs can be directly applied through the mask‐assisted casting technique by a doctor blade to fabricate micro‐supercapacitors. The micro‐supercapacitors exhibit excellent mechanical flexibility, long‐term stability, and reliable power output.     

Bright Aggregation‐Induced‐Emission Dots for Targeted Synergetic NIR‐II Fluorescence and NIR‐I Photoacoustic Imaging of Orthotopic Brain Tumors

Precise diagnostics are of significant importance to the optimal treatment outcomes of patients bearing brain tumors. NIR‐II fluorescence imaging holds great promise for brain‐tumor diagnostics with deep penetration and high sensitivity. This requires the development of organic NIR‐II fluorescent agents with high quantum yield (QY), which is difficult to achieve. Herein, the design and synthesis of a new NIR‐II fluorescent molecule with aggregation‐induced‐emission (AIE) characteristics is reported for orthotopic brain‐tumor imaging. Encapsulation of the molecule in a polymer matrix yields AIE dots showing a very high QY of 6.2% with a large absorptivity of 10.2 L g^?1 cm^?1 at 740 nm and an emission maximum near 1000 nm. Further decoration of the AIE dots with c‐RGD yields targeted AIE dots, which afford specific and selective tumor uptake, with a high signal/background ratio of 4.4 and resolution up to 38 µm. The large NIR absorptivity of the AIE dots facilitates NIR‐I photoacoustic imaging with intrinsically deeper penetration than NIR‐II fluorescence imaging and, more importantly, precise tumor‐depth detection through intact scalp and skull. This research demonstrates the promise of NIR‐II AIE molecules and their dots in dual NIR‐II fluorescence and NIR‐I photoacoustic imaging for precise brain cancer diagnostics.     

Light Confinement Effect Induced Highly Sensitive,Self‐Driven Near‐Infrared Photodetector and Image Sensor Based on Multilayer PdSe2/Pyramid Si Heterojunction

In this study, a highly sensitive and self‐driven near‐infrared (NIR) light photodetector based on PdSe₂/pyramid Si heterojunction arrays, which are fabricated through simple selenization of predeposited Pd nanofilm on black Si, is demonstrated. The as‐fabricated hybrid device exhibits excellent photoresponse performance in terms of a large on/off ratio of 1.6 × 10⁵, a responsivity of 456 mA W^?1, and a high specific detectivity of up to 9.97 × 10¹³ Jones under 980 nm illumination at zero bias. Such a relatively high sensitivity can be ascribed to the light trapping effect of the pyramid microstructure, which is confirmed by numerical modeling based on finite‐difference time domain. On the other hand, thanks to the broad optical absorption properties of PdSe₂, the as‐fabricated device also exhibits obvious sensitivity to other NIR illuminations with wavelengths of 1300, 1550, and 1650 nm, which is beyond the photoresponse range of Si‐based devices. It is also found that the PdSe₂/pyramid Si heterojunction device can also function as an NIR light sensor, which can readily record both “tree” and “house” images produced by 980 and 1300 nm illumination, respectively.     

Two-photon pumped upconversion and nonlinear optical properties of a new lasing dye: HMASPS

Abstract

Two-photon pumped frequency upconversion optical properties and two-photon absorption (TPA) induced nonlinear absorption of a new dye, trans-4-[p-(N-hydroxyethyl-N-methylamino)styryl]-N-methylpyridinium ptoluene sulfonate (abbreviated to HMASPS) have been experimentally investigated. This new dye exhibits strong superradiation properties when the pumping power is above its threshold. The superradiation upconversion efficiency from 900 to 1150 nm and the nonlinear absorption from 720 to 1100 nm have been measured. The largest effective molecular TPA cross-section was measured to be 44.3 × 10^?48 cm⁴·s·photon^?1at 920 nm. At 1064 nm, it was 2.77 × 10^?48 cm⁴·s·photon^?1, much smaller than that at 920 nm. The highest conversion efficiency is 7% at 990 nm, whereas 4.2% at 1064 nm.     

Scalable Design of Two‐Dimensional Oxide Nanosheets for Construction of Ultrathin Multilayer Nanocapacitor

Large size of capacitors is the main hurdle in miniaturization of current electronic devices. Herein, a scalable solution‐based layer‐by‐layer engineering of metallic and high‐κ dielectric nanosheets into multilayer nanosheet capacitors (MNCs) with overall thickness of ≈20 nm is presented. The MNCs are built through neat tiling of 2D metallic Ru_0.95O₂^0.2? and high‐κ dielectric Ca₂NaNb₄O₁₃^? nanosheets via the Langmuir–Blodgett (LB) approach at room temperature which is verified by cross‐sectional high‐resolution transmission electron microscopy (HRTEM). The resultant MNCs demonstrate a high capacitance of 40–52 µF cm^?2 and low leakage currents down to 10^?5–10^?6 A cm^?2. Such MNCs also possess complimentary in situ robust dielectric properties under high‐temperature measurements up to 250 °C. Based on capacitance normalized by the thickness, the developed MNC outperforms state‐of‐the‐art multilayer ceramic capacitors (MLCC, ≈22 µF cm^?2/5 × 10⁴ nm) present in the market. The strategy is effective due to the advantages of facile, economical, and ambient temperature solution assembly.     

Interlayer Hydrogen‐Bonded Metal Porphyrin Frameworks/MXene Hybrid Film with High Capacitance for Flexible All‐Solid‐State Supercapacitors

2D metal‐porphyrin frameworks (MPFs) are attractive for advanced energy storage devices. However, the inferior conductivity and low structural stability of MPFs seriously limit their application as flexible free‐standing electrodes with high performance. Here, for the first time, an interlayer hydrogen‐bonded MXene/MPFs film is proposed to overcome these disadvantages by intercalation of highly conductive MXene nanosheets into MPFs nanosheets via a vacuum‐assisted filtration technology. The alternant insertion of MXene and MPFs affords 3D interconnected “MPFs‐to‐MXene‐to‐MPFs” conductive networks to accelerate the ionic/electronic transport rates. Meanwhile, the interlayer hydrogen bonds (F···H? O and O···H? O) contribute a high chemical stability due to a favorable tolerance to volume change caused by phase separation and structural collapse during the charge/discharge process. The synergistic effect makes MXene/MPFs film deliver a capacitance of 326.1 F g^?1 at 0.1 A g^?1, 1.64 F cm^?2 at 1 mA cm^?2, 694.2 F cm^?3 at 1 mA cm^?3 and a durability of about 30 000 cycles. The flexible symmetric supercapacitor shows an areal capacitance of 408 mF cm^?2, areal energy density of 20.4 µW h cm^?2, and capacitance retention of 95.9% after 7000 cycles. This work paves an avenue for the further exploration of 2D MOFs in flexible energy storage devices.     

Graphitic Carbon Nitride (g‐C3N4)‐Derived N‐Rich Graphene with Tuneable Interlayer Distance as a High‐Rate Anode for Sodium‐Ion Batteries

Heteroatom‐doped carbon materials with expanded interlayer distance have been widely studied as anodes for sodium‐ion batteries (SIBs). However, it remains unexplored to further enlarge the interlayer spacing and reveal the influence of heteroatom doping on carbon nanostructures for developing more efficient SIB anode materials. Here, a series of N‐rich few‐layer graphene (N‐FLG) with tuneable interlayer distance ranging from 0.45 to 0.51 nm is successfully synthesized by annealing graphitic carbon nitride (g‐C₃N₄) under zinc catalysis and selected temperature (T = 700, 800, and 900 °C). More significantly, the correlation between N dopants and interlayer distance of resultant N‐FLG‐T highlights the effect of pyrrolic N on the enlargement of graphene interlayer spacing, due to its stronger electrostatic repulsion. As a consequence, N‐FLG‐800 achieves the optimal properties in terms of interlayer spacing, nitrogen configuration and electronic conductivity. When used as an anode for SIBs, N‐FLG‐800 shows remarkable Na⁺ storage performance with ultrahigh rate capability (56.6 mAh g^?1 at 40 A g^?1) and excellent long‐term stability (211.3 mAh g^?1 at 0.5 A g^?1 after 2000 cycles), demonstrating the effectiveness of material design.     

High Performance of N‐Doped Graphene with Bubble‐like Textures for Supercapacitors

Nitrogen‐doped graphene (NG) with wrinkled and bubble‐like texture is fabricated by a thermal treatment. Especially, a novel sonication‐assisted pretreatment with nitric acid is used to further oxidize graphene oxide and its binding with melamine molecules. There are many bubble‐like nanoflakes with a dimension of about 10 nm appeared on the undulated graphene nanosheets. The bubble‐like texture provides more active sites for effective ion transport and reversible capacitive behavior. The specific surface area of NG (5.03 at% N) can reach up to 438.7 m² g^?1, and the NG electrode demonstrates high specific capacitance (481 F g^?1 at 1 A g^?1, four times higher than reduced graphene oxide electrode (127.5 F g^?1)), superior cycle stability (the capacitance retention of 98.9% in 2 m KOH and 99.2% in 1 m H₂SO₄ after 8000 cycles), and excellent energy density (42.8 Wh kg^?1 at power density of 500 W kg^?1 in 2 m KOH aqueous electrolyte). The results indicate the potential use of NG as graphene‐based electrode material for energy storage devices.     

Near‐Infrared Photodetectors Based on MoTe2/Graphene Heterostructure with High Responsivity and Flexibility

2D transition metal dichalcogenides (TMDCs) have attracted considerable attention due to their impressively high performance in optoelectronic devices. However, efficient infrared (IR) photodetection has been significantly hampered because the absorption wavelength range of most TMDCs lies in the visible spectrum. In this regard, semiconducting 2D MoTe₂ can be an alternative choice owing to its smaller band gap ≈1 eV from bulk to monolayer and high carrier mobility. Here, a MoTe₂/graphene heterostructure photodetector is demonstrated for efficient near‐infrared (NIR) light detection. The devices achieve a high responsivity of ≈970.82 A W^?1 (at 1064 nm) and broadband photodetection (visible‐1064 nm). Because of the effective photogating effect induced by electrons trapped in the localized states of MoTe₂, the devices demonstrate an extremely high photoconductive gain of 4.69 × 10⁸ and detectivity of 1.55 × 10¹¹ cm Hz^1/2 W^?1. Moreover, flexible devices based on the MoTe₂/graphene heterostructure on flexible substrate also retains a good photodetection ability after thousands of times bending test (1.2% tensile strain), with a high responsivity of ≈60 A W^?1 at 1064 nm at V _DS = 1 V, which provides a promising platform for highly efficient, flexible, and low cost broadband NIR photodetectors.     

DNA‐Driven Two‐Layer Core–Satellite Gold Nanostructures for Ultrasensitive MicroRNA Detection in Living Cells

It is a significant challenge to achieve controllable self‐assembly of superstructures for biological applications in living cells. Here, a two‐layer core–satellite assembly is driven by a Y‐DNA, which is designed with three nucleotide chains that hybridized through complementary sequences. The two‐layer core–satellite nanostructure (C₃₀S₅S₁₀ NS) is constructed using 30 nm gold nanoparticles (Au NPs) as the core, 5 nm Au NPs as the first satellite layer, and 10 nm Au NPs as the second satellite layer, resulting in a very strong circular dichroism (CD) and surface‐enhanced Raman scattering. After optimization, the yield is up to 85%, and produces a g‐factor of 0.16 × 10^?2. The hybridization of the target microRNA (miRNA) with the molecular probe causes a significant drop in the CD and Raman signals, and this phenomenon is used to detect the miRNA in living cells. The CD signal has a good linear range of 0.011–20.94 amol ng_RNA^?1 and a limit of detection (LOD) of 0.0051 amol ng_RNA^?1, while Raman signal with the range of 0.052–34.98 amol ng_RNA^?1 and an LOD of 2.81 × 10^?2 amol ng_RNA^?1. This innovative dual‐signal method can be used to quantify biomolecules in living cells, opening the way for ultrasensitive, highly accurate, and reliable diagnoses of clinical diseases.