In-situ Surface-Enhanced Raman Spectroscopy Reveals a Mars-van Krevelen-Type Gas Sensing Mechanism in Au@SnO2 Nanoparticle-Based Chemiresistors.

Molecular-level understandings of gas sensing mechanisms of oxide-based chemiresistors are significant for designing high-performance gas sensors; however, the mechanisms are still controversial due to the lack of direct experimental evidence. This work demonstrates efficient in situ surface-enhanced Raman spectroscopy (SERS) tracing of the highly representative SnO2-ethanol gas sensing using Au@SnO2 nanoparticles (NPs), where the Au core and SnO2 shell provide SERS activity and a gas sensing response, respectively. The in situ SERS evidence suggests that the sensing follows a Mars-van Krevelen mechanism rather than the prevailing adsorbed oxygen (AO) model. This mechanism is also observed in sensing other gases based on the Au@SnO2 NPs, showing its universality. This work offers efficient in situ tracing for gas sensing and experimental elucidation of the specific gas sensing mechanism, potentially ending the long-term controversy over the gas sensing mechanisms. Therefore, it is highly significant to this field.

Engineered Au@CuO Nanoparticles for Wide-Range Quantitation of Sulfur Ions by Surface-Enhanced Raman Spectroscopy.

Efficient detection of sulfide ions (S2-), especially in a wide quantitative range, is of significance but faces challenges. This work strategizes and fabricates Au@CuO nanoparticles for quantitative surface-enhanced Raman spectroscopy (SERS) detection of the S2- ions based on the S2- concentration-dependent ion-solid interactions. We have achieved fast and quantitative S2- detection in a wide range from 5 ppb to 64,000 ppm (saturation concentration of the S2- source). We also demonstrated that the optimal CuO shell thickness for the detection is about 7 nm and that the detection can be further improved by prolonging the soaking duration. Moreover, this detection method has also shown the merits of reusable substrates (especially for low S2- concentrations) and good anti-interference ability to many common anions (Cl-, NO3-, OH-, HCOO-, CO32-, and SO42-). Finally, the high feasibility of this detection in actual water (tap water and pond water) has also been demonstrated. This work provides efficient S2- detection with great potential in practical use and also inspires the design of quantifiable SERS substrates for detecting more small inorganic molecules and ions.

Efficient SERS Response of Porous-ZnO-Covered Gold Nanoarray Chips to Trace Benzene-Volatile Organic Compounds.

Fast and sensitive detection of gaseous volatile organic compounds (VOCs), based on surface-enhanced Raman spectroscopy (SERS), is still a challenge due to their weak interaction with plasmonic metals and overly small Raman scattering cross sections. Herein, we propose a simple strategy to achieve the SERS-based highly efficient detection of trace benzene-VOCs (B-VOCs) based on a composite chip. The composite chip is designed and fabricated via covering the porous zinc oxide on gold nanoarrays by a one-step solution growth method. Such composite chip shows highly selective capture of gaseous B-VOCs (benzene, toluene, nitrobenzene, xylene, and chlorobenzene, etc.), which leads to the rapid and sensitive SERS responses to them. Typically, this chip can response to gaseous toluene within 30 s, and the lowest detectable concentration is below 10 ppb. Further experiments have revealed that there exists an optimal thickness of the ZnO covering layer for the highly efficient SERS response to the B-VOCs, which is about 150 nm. Also, such a composite chip is recoverable in SERS response and hence reusable. The highly efficient SERS response of the composite chip to the B-VOCs is attributed to the porous structure-enhanced molecular adsorption and the electromagnetic-chemical dual-enhancement mechanism. This work not only presents a practical SERS chip for the efficient detection of the typical B-VOCs but also provides a deep understand the interaction between the B-VOCs and the ZnO as well as the chemical enhancement mechanism.

High-Density-Nanotips-Composed 3D Hierarchical Au/CuS Hybrids for Sensitive, Signal-Reproducible, and Substrate-Recyclable SERS Detection.

Surface-enhanced Raman scattering (SERS) provides an unprecedented opportunity for fingerprinting identification and trace-level detection in chemistry, biomedicine, materials, and so on. Although great efforts have been devoted to fabricating sensitive plasmonic nanomaterials, it is still challenging to batch-produce a SERS substrate with high sensitivity, good reproducibility, and perfect recyclability. Here, we describe a facile fabrication of three-dimensional (3D) hierarchical Au/CuS nanocomposites, in which high-density Au nanotips enable highly SERS-active sensing, and the well-defined microflower (MF) geometry produces perfect signal reproducibility (RSD < 5%) for large laser spot excitations (>50 µm2), which is particularly suitable for practical on-site detection with a handheld Raman spectrometer. In addition, a self-cleaning ability of this Au/CuS Schottky junction photocatalyst under sunlight irradiation allows complete removal of the adsorbed analytes, realizing perfect regeneration of the SERS substrates over many cycles. The mass-production, ultra-sensitive, high-reproducibility, and fast-recyclability features of hierarchical Au/CuS MFs greatly facilitate cost-effective and field SERS detection of trace analytes in practice.

Abnormally Weak Surface-Enhanced Raman Scattering Activity of Tip-Rich Au Nanostars: The Role of Interfacial Defects.

Designing and regulating the geometry of a given plasmonic metal (Au, Ag, etc.) has become one of the most efficient approaches to achieve highly active surface-enhanced Raman spectroscopy (SERS) substrates, but this work demonstrates that plain efforts on this may not be enough. Here, we report that the often-neglected inner crystal defects also have huge impacts on the SERS activity, through a case of Au nanostars (NSs) with good SERS geometry but rich in defects. The results suggest that the interfacial defects (twin boundaries and superlattices) in the NSs aggravate the electronic oscillation damping via reducing the free path of electron scattering. This eventually results in weak local electromagnetic fields near the NS surfaces (or weak SERS activity of the NSs). This study has demonstrated the huge impact of interfacial defects on SERS activity and thus has a significant guideline for the design and fabrication of efficient SERS substrates.

Optimal Excitation Wavelength for Surface-Enhanced Raman Spectroscopy: The Role of Chemical Interface Damping.

The optimal excitation wavelength (OEW) for surface-enhanced Raman spectroscopy (SERS) is generally close to that of the local surface plasmon resonance (LSPR). In some cases, however, the OEW is significantly longer than that of the observed LSPR. Its origin is still unclear and controversial. Here, we propose a chemical interface damping (CID)-based mechanism and reveal the origin of the OEW's deviation from the LSPR by simulation and experiments using gold nanorods as the model material. Simulations show that the molecular adsorption induces CID, which causes a red-shift of the near-field peak relative to the far-field one, and that the chemical adsorption of target molecules on the plasmonic metals with enough strong CID would induce a significant red-shift of the OEW, even to the region far beyond the LSPR. Finally, we experimentally confirm the validity of the proposed CID theory and demonstrate the significant influence of the CID on the OEW during SERS measurements.

Quantitative Surface-Enhanced Raman Spectroscopy for Field Detections Based on Structurally Homogeneous Silver-Coated Silicon Nanocone Arrays.

Practical application of surface-enhanced Raman spectroscopy (SERS) is greatly limited by the inaccurate quantitative analyses due to the measuring parameter's fluctuations induced by different operators, different Raman spectrometers, and different test sites and moments, especially during the field tests. Herein, we develop a strategy of quantitative SERS for field detection via designing structurally homogeneous and ordered Ag-coated Si nanocone arrays. Such an array is fabricated as SERS chips by depositing Ag on the template etching-induced Si nanocone array. Taking 4-aminothiophenol as the typical analyte, the influences of fluctuations in measuring parameters (such as defocusing depth and laser powers) on Raman signals are systematically studied, which significantly change SERS measurements. It has been shown that the silicon underneath the Ag coating in the chip can respond to the measuring parameters' fluctuations synchronously with and similar to the analyte adsorbed on the chip surface, and the normalization with Si Raman signals can well eliminate the big fluctuations (up to 1 or 2 orders of magnitude) in measurements, achieving highly reproducible measurements (mostly, <5% in signal fluctuations) and accurate quantitative SERS analyses. Finally, the simulated field tests demonstrate that the developed strategy enables quantitatively analyzing the highly scattered SERS measurements well with 1 order of magnitude in signal fluctuation, exhibiting good practicability. This study provides a new practical chip and reliable quantitative SERS for the field detection of real samples.

Ultrasensitive surface-enhanced Raman spectroscopy detection of gaseous sulfur-mustard simulant based on thin oxide-coated gold nanocone arrays.

Surface Enhanced Raman Spectroscopy (SERS) could be a powerful technique for detecting trace gaseous sulfur-mustard, but it is still challenging due to the difficulty in efficiently capturing sulfur-mustard molecules by normal SERS substrates. Here, a chemically trapping strategy is presented for such detection via coating an ultrathin metal-oxide sensing layer on a SERS substrate. In the strategy, a SERS substrate Au-wrapped Si nanocone array is designed and fabricated by Si wafer-based organic template-etching and appropriate Au deposition, and coated with an ultrathin CuO for chemically capturing sulfur-mustard molecules. The validity of such strategy has been demonstrated via taking the gaseous 2-chloroethyl ethyl sulfide (a simulant of sulfur-mustard, or 2-CEES for short) as the target molecules. The response of the CuO-coated SERS substrate to the gaseous 2-CEES is detectable within 10 min, and the lowest detectable concentration is 10 ppb or less. Further experiments have shown that there exists an optimal CuO coating thickness which is about 6 nm. The CuO coating-based capture of 2-CEES molecules is attributed to the surface hydroxyl-induced specific adsorption, which is subject to the pseudo-second-order kinetics and Freundlich-typed model. This study presents the practical SERS chips and new route for the trace detection of gaseous sulfur-mustard.

Ultrathin Hexagonal PbO Nanosheets Induced by Laser Ablation in Water for Chemically Trapping Surface-Enhanced Raman Spectroscopy Chips and Detection of Trace Gaseous H2S.

Lead oxide (PbO) nanosheets are of significance in the design of functional devices. However, facile, green, and fast fabrication of ultrathin and homogenous PbO nanosheets with a chemically clean surface is still desirable. Herein, a simple and chemically clean route is developed for fabricating such nanosheets via laser ablation of a lead target in water for a short time and then ambient aging. The obtained PbO nanosheets are (002)-oriented with microsize in planar dimension and ∼15 nm in thickness. They are mostly hexagonal in shape. Experimental observations of the morphological evolution have revealed that the formation of such PbO nanosheets can be attributed to two processes: (i) laser ablation-induced formation of ultrafine Pb and PbO nanoparticles (NPs) and (ii) PbO NP aggregation and their oriented connection growth. Importantly, a composite surface-enhanced Raman spectroscopy (SERS) chip is designed and fabricated by covering a PbO nanosheet monolayer on a Au NP film. Such a composite SERS chip can be used for the fast and trace detection of gaseous H2S in which the PbO nanosheets can effectively chemically trap H2S molecules, demonstrating a new application of these PbO nanosheets. The response of this chip to H2S can be detected within 10 s, and the detection limit is below 1 ppb. Also, this PbO nanosheet-based chip is reusable by heating after use. This study not only deepens the understanding of the NP-based formation mechanism of nanosheets but also provides the renewable SERS chips for the highly efficient detection of trace gaseous H2S.

Conductometric Response-Triggered Surface-Enhanced Raman Spectroscopy for Accurate Gas Recognition and Monitoring Based on Oxide-wrapped Metal Nanoparticles.

Accurate and efficient gas monitoring is still a challenge because the existing sensing techniques mostly lack specific identification of gases or hardly meet the requirement of real-time readout. Herein, we present a strategy of conductometric response-triggered surface-enhanced Raman spectroscopy (SERS) for such gas monitoring, via designing and using ultrathin oxide-wrapped plasmonic metal nanoparticles (NPs). The oxide wrapping layer can interact with and capture target gaseous molecules and produce the conductometric response, while the plasmonic metal NPs possess strong SERS activity. In this strategy, the conductometric gas sensing is performed throughout the whole monitoring process, and once a conductometric response is generated, it will trigger SERS measurements, which can accurately recognize molecules and hence realize gas monitoring. The feasibility of this strategy has been demonstrated via using ultrathin SnO2 layer-wrapped Au NP films to monitor gaseous 2-phenylethanethiol molecules. It has been shown that the monitoring is rapid, accurate, and quantifiable. There exist optimal values of working temperature and SnO2 layer thickness, which are about 100 °C and 2.5 nm, respectively, for monitoring gaseous 2-phenylethanethiol. The monitoring signal intensity has a linear relation with the gas concentration in the range from 1 to 100 ppm on a logarithmic scale. Furthermore, the monitoring limits are at the ppm level for some typical gases, such as 2-phenylethanethiol, cyclohexanethiol, 1-dodecanethiol, and toluene. This study establishes the conductometric response-triggered SERS, which enables accurate gas recognition and real-time monitoring.

Mars-van-Krevelen mechanism-based blackening of nano-sized white semiconducting oxides for synergetic solar photo-thermocatalytic degradation of dye pollutants.

Blackening (or enhancing the optical absorption in the visible region) of nano-sized white semiconducting oxides (N-WSOs) is of significant importance for solar utilization. Here, we present a novel Mars-van-Krevelen mechanism-based method for blackening the N-WSOs via facile one-step heating of the N-WSOs with alcohols. Taking n-butanol-induced blackening of TiO2 (anatase) as an example, the pristine TiO2 NP powders can be successfully blackened to form black TiO2 (B-TiO2) via heating with n-butanol at 300 °C for 20 min. Technical analyses demonstrate that the B-TiO2 nanocrystals are wrapped with a 2 nm thick disordered layer, which is rich in oxygen vacancies, Ti3+ and hydroxyl groups. Both theoretical and experimental results show that B-TiO2 has much stronger optical absorption in the visible region than pristine TiO2. Furthermore, the influence factors (including heating temperatures and alcohol types) and good universality of this blackening method are also demonstrated. A blackening principle based on Mars-van-Krevelen mechanism-induced oxygen vacancy generation and hydroxylation-anchoring of oxygen vacancies has been proposed, and the mechanism can well explain all the phenomena observed in experiments. Importantly, such B-TiO2 shows hugely enhanced activity in solar photodegradation of dye pollutants. Under simulated solar irradiation, the degradation rate constant achieved by the B-TiO2 catalyst is 2.3 times that of the pristine TiO2, showing an obvious enhancement. Further experiments reveal that the improved degradation activity is mainly attributed to the enhanced optical absorption in the visible region and the synergistic photothermal and photocatalytic effect. This study demonstrates a new and facile approach to blacken the N-WSOs for enhanced solar utilization.

Ultrathin layer solid transformation-enabled-surface enhanced Raman spectroscopy for trace harmful small gaseous molecule detection.

Detection of trace harmful small gaseous molecules (h-SGMs), based on surface enhanced Raman spectroscopy (SERS), has been expected to be a useful strategy but is challenging due to the extremely small Raman cross section (RCS) and weak metal affinity of the h-SGMs. Here, a new strategy, ultrathin layer solid transformation-enabled (ULSTE)-SERS, is proposed. It uses the chemical reaction between the target h-SGM and an ultrathin layer of solid sensing matter coated on a plasmonic metal SERS substrate. This reaction in situ produces a new solid matter with large RCS, which ensures the detection of trace h-SGMs via SERS. The validity of this strategy has been demonstrated by detecting trace H2S gas with an ultrathin CuO layer wrapped around Au nanoparticles. Furthermore, this strategy allows fast and ultrasensitive detection. The detection limit can be down to ppb (even ppt) levels with 10 min preprocessing. Importantly, this strategy has good universality for various other h-SGMs, such as SO2, CS2, CH3SH, and HCl, etc., using appropriate sensing matter. Additionally, the ULSTE-SERS is also suitable for unstable molecules and fast portable detection due to the stable solid layer. This work provides highly efficient SERS-based detection of trace h-SGMs, which is easily applied in practical situations.

Rapid and ultrasensitive surface-enhanced Raman spectroscopy detection of mercury ions with gold film supported organometallic nanobelts.

Rapid, ultrasensitive and reliable detection of mercury ions (Hg2+) by surface enhanced Raman spectroscopy (SERS) is of importance, but is restricted by the extremely low Raman cross section of the Hg2+. Here, we report a facile methodology that can realize such detection based on the organometallic Cu(CH4N2S)Cl · 0.5H2O nanobelts and SERS. In the assay, Hg2+ react with the nanobelts coated on a SERS active gold nanoparticle (NP) film to form ultrafine HgS NPs in situ. Subsequently, solid HgS is SERS determined to mirror the presence of Hg2+. Importantly, such detection is rapid and ultrasensitive. Within 10 min, limit of detection (LoD) of ppt level can be realized. The high detection efficiency is attributed to the superhydrophilicity, rich micropores and ultrathin nature of the organometallic nanobelts besides the strong SERS effect of Au NP film. In addition, this detection is highly resistant to various metal ions (Cu2+, Fe3+, Bi3+, Cr3+, Na+, Ni2+, Cd2+, etc) and is highly reliable in actual water (lake and tap water). Finally, influences of some substrate parameters and detection conditions on the test results are revealed. The optimal thickness of the gold NP film is about 80 nm, and the optimal wavelength of excitation light is about 633 nm. A small amount of Cu(CH4N2S)Cl · 0.5H2O nanobelts or a large volume of Hg2+ contaminated solution contributes to low LoDs. We believe that this work provides a rapid and sensitive detection for Hg2+.

Ultrathin and Isotropic Metal Sulfide Wrapping on Plasmonic Metal Nanoparticles for Surface Enhanced Ram Scattering-Based Detection of Trace Heavy-Metal Ions.

A facile and general strategy is presented for homogenous and ultrathin metal sulfide wrapping on plasmonic metal (PM) nanoparticles (NPs) based on a thiourea-induced isotropic shell growth. This strategy is typically implemented just via adding the thiourea into pre-formed PM colloidal solutions containing target metal ions. The validity of this strategy is demonstrated by taking the wrapped NPs with Au core and CuS shell or Au@CuS NPs as an example. They are successfully fabricated via adding the thiourea and Cu2+ solutions into pre-formed Au NP colloidal solution. The CuS shell layer is highly homogenous (<10% in relative standard deviation of shell thickness), regardless of the NPs' shape or curvature. The shell thickness can be controlled from tens down to 0.5 nm just by the addition of different amounts of shell precursors. The formation of the shell layer on the Au NPs can be attributed to the alternative deposition of Cu2+ and S2- ions on the thiourea-modified surface of Au NPs in the solution, which induces the isotropic shell growth. Further, this strategy is of good universality. Many other sulfide-wrapped PM NPs, such as Ag@CuS, Au@PtS2, Au@HgS, Ag@Ag2S NPs, and Ag@CuS nanorods, have been successfully obtained with homogeneous and ultrathin shells. Importantly, such ultrathin sulfide-wrapped PM NPs can be used for surface enhanced Raman scattering (SERS)-based detection of trace heavy-metal ions with strong anti-interference via the ion exchange process between the metal sulfide shell and heavy-metal ions. This study provides a simple and controllable route for wrapping the homogenous and ultrathin sulfide layers on the PM NPs, and such wrapped NPs have good practical applications in the SERS-based detection of trace heavy-metal ions.

Large Area α-Cu2S Particle-Stacked Nanorod Arrays by Laser Ablation in Liquid and Their Strong Structurally Enhanced and Stable Visible Photoelectric Performances.

A flexible route is developed for fabrication of large area α-Cu2S nanorod arrays (NRAs) on the basis of one-step laser ablation of a copper foil in CS2 liquid. It has been demonstrated that the obtained products are the high-temperature phase α-Cu2S and consist of the nanorods vertically standing on the Cu foil, exhibiting the array. The nanorods were about 1 µm in length and around 100 nm in thickness and built by stacking the nearly spherical and ⟨110⟩-oriented nanoparticles (NPs) up. Such array can be peeled off from the foil and remain freestanding. Further, it has been found that the ablation duration, the laser power, and the foil surface state are crucial to the formation of the Cu2S NRA. The formation of such oriented NP-stacked Cu2S NRAs is attributed to the laser-induced generation of α-Cu2S NPs and the NPs' deposition/oriented connection growth on the surface-vulcanized copper foil. Importantly, the visible photocurrent response of the α-Cu2S NRAs is 8 times higher than that of the Cu2S NPs' film with the equivalent thickness and also larger than that of previously reported Cu2S, showing significantly enhanced photoelectric performances. As an application, such NRAs have exhibited markedly enhanced visible photocatalytic activity and highly stable recycling performances, compared with the α-Cu2S NPs. Further studies have revealed that the enhanced performances are attributed to the structurally enhanced light trapping effect of the NRAs as well as short and smooth carrier diffusion path in the oriented NP-stacked nanorods. This work provides a new and simple method for fabrication of the large area Cu2S NRAs with high and stable photoelectric performances.

Ultrathin Oxide Layer-Wrapped Noble Metal Nanoparticles via Colloidal Electrostatic Self-Assembly for Efficient and Reusable Surface Enhanced Raman Scattering Substrates.

Controllable and flexible fabrication of ultrathin and uniform oxide layer-wrapped noble metal nanoparticles (NPs) has been expected. Here a new strategy is presented for them based on colloidal electrostatic attraction and self-assembly on the metal NPs via one-step laser ablation of noble metal targets in the hydrolysis-induced hydroxide sol solutions at room temperature. The Au NPs, with several tens of nanometers in size, are taken as core part and TiO2 as shell-layer to demonstrate the validity of the presented strategy. It has been shown that the TiO2 shell-wrapped Au NPs are obtained after laser ablation of Au target in the hydrolysis-induced Ti(OH)4 sol solution. The Au NPs are about 35 nm in mean size, and the TiO2 shell layers are amorphous in structure and about 2.5 nm in thickness. The shell thickness is nearly independent of the Au NPs' size. Further experiments have shown that the thickness and crystallinity of the shell-layer can be tuned and controlled via changing the temperature or pH value of the Ti(OH)4 sol solution or prolonging the laser ablation duration. The formation of the TiO2 shell-wrapped Au NPs is attributed to attachment and self-assembly of Ti(OH)4 colloids on the laser-induced Au NPs due to the electrostatic attraction between them. Importantly, the presented strategy is universal and suitable for fabrication of many other ultrathin oxide-wrapped noble metal NPs. A series of oxide shell-wrapped noble metal NPs have been successfully fabricated, such as Au@oxides (Fe2O3, Al2O3, CuO, and ZnO) as well as Pt@TiO2 and Pd@TiO2, etc. Further, compared with the pure gold NPs-built film, the TiO2-wrapped Au NPs-built film has exhibited much stronger surface enhanced Raman scattering (SERS) performance to the anions NO3-, which weakly interact with noble metals, and the good reusability for the SERS-based detection of 4-nitrophenol, which could be photodegraded by xenon lamp irradiation. This work provides a flexible and universal route to the ultrathin and uniform oxide layer-wrapped noble metal NPs.

Nanoscaled Amorphous TiO2 Hollow Spheres: TiCl4 Liquid Droplet-Based Hydrolysis Fabrication and Strong Hollow Structure-Enhanced Surface-Enhanced Raman Scattering Effects.

A very simple route is developed for fast fabrication of nanosized amorphous titanium dioxide (TiO2) hollow spheres (THPs) just via dropping the pure four titanium chloride (TiCl4) liquid droplets into deionized water at around room temperature. The THPs, at around 80 nm in mean diameter, can be formed within a few seconds after dropping TiCl4 droplets into water. The shell layers of the obtained THPs are amorphous and porous in structure with a porosity of 58-80% and show a linear increase in thickness with the size of THPs. Further experiments have revealed that the reaction temperature, initial pH value, and size of the TiCl4 droplet are crucial to the formation, size, productivity, and microstructure of the THPs. A model is proposed on the basis of the fragmentation of liquid droplets, hydrolysis-induced formation, and inward growth of TiO2 shell layers, which can well describe the formation of the THPs. Importantly, such amorphous nanoscaled THPs have exhibited some strong hollow structure-enhanced performances. Typically, the THP-built film shows the highest reflectivity in the visible region compared to the other structured TiO2 films. Especially, if it supports the film of the Au nanoparticle, the surface-enhanced Raman scattering effect is significantly enhanced by more than 1 order of magnitude. This work provides not only a simple and quick fabrication method for the THPs but also a new member for their family.

Ultrathin tin oxide layer-wrapped gold nanoparticles induced by laser ablation in solutions and their enhanced performances.

A simple and flexible method of preparing an ultrathin semiconducting oxide layer-wrapped gold nanoparticles (NPs) is presented. The method is a single-step procedure based on laser ablation in a precursor solution. The spherical Au NPs (<20nm in mean size) wrapped with a SnO2 layer of approximately 2nm in thickness are formed after the laser ablation of a gold target in SnCl4 solutions with concentrations of 0.01-0.1M. The thickness of such SnO2 shell is nearly independent of Au particle sizes. Results reveal that the formation of Au@SnO2 NPs involves a two-step process: the laser ablation-induced formation of Au NPs and subsequent Coulomb effect-based colloidal attachment and self-assembly on the Au NPs. Au@SnO2 NPs-built film exhibits significantly stronger surface-enhanced Raman scattering effect to organic phosphor molecules (phenylphosphonic acid) and much better gas sensing performance to H2S at room temperature compared with the bare Au NPs and pure SnO2 NPs films, respectively. This work presents a simple route to fabricating noble-metal NPs wrapped with symmetrical and ultrathin semiconducting oxide shells.