Universal architecture and defect engineering dual strategy for hierarchical antimony phosphate composite toward fast and durable sodium storage

Antimony(Sb)-ba sed anode materials are feasible candidates for sodium-ion batteries(SIBs) due to their high theoretical specific capacity and excellent electrical conductivity.However,they still suffer from volume distortion,structural collapse,and ionic conduction interruption upon cycling.Herein,a hierarchical array-like nanofiber structure was designed to address these limitations by combining architecture engineering and anion tuning strategy,in which SbPO_(4-x) with oxygen vacancy nanosheet arrays are anchored on the surface of interwoven carbon nanofibers(SbPO_(4-x)@CNFs).In particular,bulky PO_(4)^(3-) anions mitigate the large volume distortion and generate Na_(3)PO_(4) with high ionic conductivity,collectively improving cyclic stability and ionic transport efficiency.The abundant oxygen vacancies substantially boost the intrinsic electronic conductivity of SbPO_4,further accelerating the reaction dynamics.In addition,hierarchical fibrous structures provide abundant active sites,construct efficient conducting networks,and enhance the electron/ion transport capacity.Benefiting from the advanced structural design,the SbPO_(4-x)@CNFs electrodes exhibit outstanding cycling stability(1000 cycles at 1.0 A g^(-1) with capacity decay of 0.05% per cycle) and rapid sodium storage performance(293.8 mA h g^(-1) at 5.0 A g^(-1)).Importantly,systematic in-/ex-situ techniques have revealed the "multi-step conversion-alloying" reaction process and the "battery-capacitor dual-mode" sodium-storage mechanism.This work provides valuable insights into the design of anode materials for advanced SIBs with elevated stability and superior rate performance.

Integrated adsorption and photocatalytic removal of methylene blue dye from aqueous solution by hierarchical Nb_(2)O_(5)@PAN/PVDF/ANO composite nanofibers

This work presents the development of hierarchical niobium pentoxide(Nb_(2)O_(5))-based composite nanofiber membranes for integrated adsorption and photocatalytic degradation of methylene blue(MB)pollutants from aqueous solutions.The Nb_(2)O_(5) nanorods were vertically grown using a hydrothermal process on a base electrospun nanofibrous membrane made of polyacrylonitrile/polyvinylidene fluoride/ammonium niobate(V)oxalate hydrate(Nb_(2)O_(5)@PAN/PVDF/ANO).They were characterized using field-emission scanning electron microscopy(FE-SEM),X-ray diffraction(XRD)analysis,and Fourier transform infrared(FTIR)spectroscopy.These composite nanofibers possessed a narrow optical bandgap energy of 3.31 eV and demonstrated an MB degradation efficiency of 96%after 480 min contact time.The pseudo-first-order kinetic study was also conducted,in which Nb_(2)O_(5)@PAN/PVDF/ANO nanofibers have kinetic constant values of 1.29×10^(-2) min^(-1) and 0.30×10^(-2) min^(-1) for adsorption and photocatalytic degradation of MB aqueous solutions,respectively.These values are 17.7 and 7.8 times greater than those of PAN/PVDF/ANO nanofibers without Nb_(2)O_(5) nanostructures.Besides their outstanding photocatalytic performance,the developed membrane materials exhibit advantageous characteristics in recycling,which subsequently widen their practical use in environmental remediation applications.

Macroscopic Regulation of Hierarchical Nanostructures in Liquid-crystalline Block Copolymers towards Functional Materials

The great potential of liquid-crystalline block copolymers(LCBCs)containing photoresponsive mesogens toward novel applications in photonics and nanotechnology has been attracting increasing attention,due to the combination of the inherent property of microphase separation of block copolymers and the hierarchically-assembled structures of liquid-crystalline polymers(LCPs).The periodically ordered nanostructures in bulk film of LCBCs can be acquired by supramolecular cooperative motion,derived from the interaction between liquid-crystalline elastic deformation and microphase separation,which are able to improve physical properties of polymer film toward advanced functional applications.Moreover,various micro/nano-patterned structures have been fabricated via light manipulation of photoresponsive LCBCs with good reproducibility and mass production.Thanks to recent developments in synthesis and polymerization techniques,diverse azobenzene-containing LCBCs have been designed,resulting in the creation of a wide variety of novel functions.This review illustrates recent progresses in macroscopic regulation of hierarchical nanostructures in LCBCs towards functional materials.The existing challenges are also discussed,showing perspectives for future studies.

Hierarchical AgAu alloy nanostructures for highly efficient electrocatalytic ethanol oxidation

The ethanol oxidation reaction is a significant anodic reaction for direct alcohol fuel cells.The most commonly used catalysts for this reaction are Pt‐based materials;however,Pt‐based electrocatalysts cause carbon monoxide poisoning with intermediates before the complete transformation of alcohol to CO_(2).Herein,we present hierarchical AgAu bimetallic nanoarchitectures for ethanol electrooxidation,which were fabricated via a partial galvanic reduction reaction between Ag and HAuCl_(4).The ethanol electrooxidation performance of the optimal AgAu nanohybrid was increased to 1834 mA mg^(‒1),which is almost 10 times higher than that of the pristine Au catalyst(190 mA mg^(‒1))in alkaline solutions.This was achieved by introducing Ag into the Au catalyst and controlling the time of the replacement reaction.The heterostructure also presents a higher current density than that of commercial Pt/C(1574 mA mg^(‒1)).Density functional theory calculations revealed that the enhanced activity and stability may stem from unavoidable defects on the surface of the integrated AgAu nanoarchitectures.Ethanol oxidation reactions over these defects are more energetically favorable,which facilitates the oxidative removal of carbonaceous poison and boosts the combination with radicals on adjacent Au active sites.

Strongly Anchoring Polysulfides by Hierarchical Fe3O4/C3N4 Nanostructures for Advanced Lithium-Sulfur Batteries

Li-S batteries have attracted considerable interest as nextgeneration energy storage devices owing to high energy density and the natural abundance of sulfur.However,the practical applications of Li-S batteries are hampered by the shuttle effect of soluble lithium polysulfides(LPS),which results in low cycle stability.Herein,a functional interlayer has been developed to efficiently regulate the LPS and enhance the sulfur utilization using hierarchical nanostructure of C3 N4(t-C3 N4)embedded with Fe304 nanospheres.t-C3 N4 exhibits high surface area and strong anchoring of LPS,and the Fe3 O4/t-C3 N4 accelerates the anchoring of LPS and improves the electronic pathways.The combination of these materials leads to remarkable battery performance with 400%improvement in a specific capacity and a low capacity decay per cycle of 0.02%at 2 C over 1000 cycles,and stable cycling at 6.4 mg cm-2 for high-sulfur-loading cathode.

Cu-alanine complex-derived CuO electrocatalysts with hierarchical nanostructures for efficient oxygen evolution

Nowadays,Cu-based materials have attracted extensive attention as electrocatalysts,while the inherent reason of the filling of high anti-bonding state of Cu d band(3 d^(10)4 s^(1))makes it difficult to hybridize with O2 p band of oxygen intermediates during the adsorption process of oxygen evolution reaction(OER).To increase the efficiency of Cu-based electrocatalysts,efforts have been made to optimize the electronic structures and to create surface defects and hierarchical nanostructures with more exposed accessible active sites.Herein,we report a facile method for preparing CuO electrocatalysts with hierarchical nanostructures using the Cu-alanine complex as a precursor through room-temperature chemical precipitation and subsequent calcination in air.Investigations of products obtained at different calcination temperatures reveal the relationship between OER activities and the material characteristics such as specific surface areas,crystal growth orientations,and element components.The product obtained at 500℃exhibits the smallest overpotential of 290 mV in 1.0 mol/L KOH for electrocatalyzing OER.Combining with various characterizations of CuO electrocatalysts after OER activities,the possible catalytic mechanism and the influence factors of their OER performance are also discussed.

Lanthanum-dopedα-Ni(OH)_(2)1D-2D-3D hierarchical nanostructures for robust bifunctional electro-oxidation

The development of advanced electrocatalysts for electro-oxidation reactions has attracted much attention because of the critical role of such electrocatalysts in improving the overall efficiency of coupled hydrogen production.We have developed an efficient lanthanum-dopedα-Ni(OH)_(2) bifunctional catalyst with a 1D-2D-3D hierarchical nanostructure.It shows superior activity and stability in the anodic oxygen evolution reaction(OER)and urea oxidation reaction(UOR).Enrichment of the edge sites and conducting La doping inα-Ni(OH)_(2) phase enable formation and stabilization of abundant local Ni^(3+)ions.This guarantees ultralow onset potentials in electro-oxidation reactions.The 1D-2D-3D hierarchical nanostructure significantly boosts the in situ generation of high-valence active species,which results in efficient and stable OER and UOR performances,and the synergistic merit of doping-induced facile reaction kinetics.Because of the structural benefits of a large surface area,charge-transfer promotion,good structural stability,and bifunctionality,a 1%La-dopedα-Ni(OH)_(2) hierarchical nanostructure gives superior OER and UOR performances with low overpotentials,large catalytic current densities,and excellent operational stability.It is therefore a promising catalyst for use in simultaneous alkaline wastewater treatment and hydrogen production.

Artificial Macrophage with Hierarchical Nanostructure for Biomimetic Reconstruction of Antitumor Immunity

Artificial cells are constructed from synthetic materials to imitate the biological functions of natural cells.By virtue of nanoengineering techniques,artificial cells with designed biomimetic functions provide alternatives to natural cells,showing vast potential for biomedical applications.Especially in cancer treatment,the deficiency of immunoactive macrophages results in tumor progression and immune resistance.To overcome the limitation,a BaSO_(4)@ZIF-8/transferrin(TRF)nanomacrophage(NMΦ)is herein constructed as an alternative to immunoactive macrophages.Alike to natural immunoactive macrophages,NMΦis stably retained in tumors through the specific affinity of TRF to tumor cells.Zn^(2+)as an“artificial cytokine”is then released from the ZIF-8 layer of NMΦunder tumor microenvironment.Similar as proinflammatory cytokines,Zn^(2+)can trigger cell anoikis to expose tumor antigens,which are selectively captured by the BaSO_(4)cavities.Therefore,the hierarchical nanostructure of NMΦs allows them to mediate immunogenic death of tumor cells and subsequent antigen capture for T cell activation to fabricate long-term antitumor immunity.As a proof-of-concept,the NMΦmimics the biological functions of macrophage,including tumor residence,cytokine release,antigen capture and immune activation,which is hopeful to provide a paradigm for the design and biomedical applications of artificial cells.

Self-assembled Synthesis of 3D CuO Flocculus-like Nanosheet-based Hierarchical Nanostructures

A simple, surfactant-free, and environmentally benign method has been developed to synthesize a novel 3D flocculus-like CuO hierarchical nanostructure self-assembled with 2D nanosheet as building blocks. Detailed proofs demonstrate that the overall synthetic process underwent the dehydration and re-crystallization of precursor Cu（OH）2 nanowires, and the subsequent two-step oriented attachment. In addition, 3D butterfly-like and flower-like CuO nanostructures consisted of 2D nanosheets could be obtained by adjusting the concentration of NaOH（cNaoH） in the solution. CNaOH played a key role in tailoring the thickness of the nanosheets and changing the morphology of the product. This report may be helpful to constructing fine-tune hierarchical CuO nanostructures under basic conditions.

Simple Fabrication of Hierarchical Micro/Nanostructure Superhydrophobic Surface with Stable and Superior Anticorrosion Silicon Steel via Laser Marking Treatment

To improve the weak corrosion resistance of silicon steel to acid solution and alkaline solution with high temperature,a stable hierarchical micro/nanostructure superhydrophobic surface with myriad irregular micro-scale hump and sheet-like nanostructure was successfully prepared on silicon steel by a simple,efficient and facile operation in large-area laser marking treatment.The morphology,composition,wettability of the as-prepared surface were studied.The superhydrophobic performance of the surface was investigated as well.Additionally,the corrosion resistance of the superhydrophobic surface to acidic solutions at room temperature and alkaline solutions at high temperature (80 ℃) was carefully explored.The corrosion resistance mechanism was clarified.Moreover,considering the practical application of the surface in the future,the hardness of the hierarchical micro/nanostructure superhydrophobic surface was studied.The experimental results indicate that the hierarchical micro/nanostructure surface with texture spacing of 100 μm treated at laser scanning speed of 100 mms/ presents superior superhydrophobicity after decreasing surface energy.The contact angle can be as high as 156.6°.Additionally,the superhydrophobic surface provide superior and stable anticorrosive protection for silicon steel in various corrosive environments.More importantly,the prepared structure of the surface shows high hardness,which ensures that the surface of the superhydrophobic surface cannot be destroyed easily.The surface is able to maintain great superhydrophobic performance when it suffers from slight impacting and abrasion.

Hierarchically Micro/Nanostructured Current Collectors Induced by Ultrafast Femtosecond Laser Strategy for High-Performance Lithium-ion Batteries

Commercial Cu and Al current collectors for lithium-ion batteries(LIBs)possess high electrical conductivity,suitable chemical and electrochemical stability.However,the relatively flat surface of traditional current collectors causes weak bonding strength and poor electrochemical contact between current collectors and electrode materials,resulting in potential detachment of active materials and rapid capacity degradation during extended cycling.Here,we report an ultrafast femtosecond laser strategy to manufacture hierarchical micro/nanostructures on commercial Al and Cu foils as current collectors for high-performance LIBs.The hierarchically micro/nanostructured current collectors(HMNCCs)with high surface area and roughness offer strong adhesion to active materials,fast electronic delivery of entire electrodes,significantly improving reversible capacities and cyclic stability of HMNCCs based LIBs.Consequently,LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2)(NCM523)cathode with Al HMNCC generated a high reversible capacity after 200 cycles(25%higher than that of cathode with Al CC).Besides,graphite anode with Cu HMNCC also maintained prominent reversible capacity even after 600 cycles.Moreover,the full cell assembled by graphite anode with Cu HMNCC and NCM523 cathode with Al HMNCC achieved high reversible capacity and remarkable cycling stability under industrial-grade mass loading.This study provides promising candidate for achieving high-performance LIBs current collectors.

Underwater persistent bubble-assisted femtosecond laser ablation for hierarchical micro/nanostructuring

In this study,we demonstrate a technique termed underwater persistent bubble assisted femtosecond laser ablation in liquids(UPB-fs-LAL)that can greatly expand the boundaries of surface micro/nanostructuring through laser ablation because of its capability to create concentric circular macrostructures with millimeter-scale tails on silicon substrates.Long-tailed macrostructures are composed of layered fan-shaped(central angles of 45°–141°)hierarchical micro/nanostructures,which are produced by fan-shaped beams refracted at the mobile bubble interface(.50°light tilt,referred to as the vertical incident direction)during UPB-fs-LAL line-by-line scanning.Marangoni flow generated during UPB-fs-LAL induces bubble movements.Fast scanning(e.g.1mms−1)allows a long bubble movement(as long as 2mm),while slow scanning(e.g.0.1mms−1)prevents bubble movements.When persistent bubbles grow considerably(e.g.hundreds of microns in diameter)due to incubation effects,they become sticky and can cause both gas-phase and liquidphase laser ablation in the central and peripheral regions of the persistent bubbles.This generates low/high/ultrahigh spatial frequency laser-induced periodic surface structures(LSFLs/HSFLs/UHSFLs)with periods of 550–900,100–200,40–100 nm,which produce complex hierarchical surface structures.A period of 40 nm,less than 1/25th of the laser wavelength(1030 nm),is the finest laser-induced periodic surface structures(LIPSS)ever created on silicon.The NIR-MIR reflectance/transmittance of fan-shaped hierarchical structures obtained by UPB-fs-LAL at a small line interval(5μm versus 10μm)is extremely low,due to both their extremely high light trapping capacity and absorbance characteristics,which are results of the structures’additional layers and much finer HSFLs.In the absence of persistent bubbles,only grooves covered with HSFLs with periods larger than 100 nm are produced,illustrating the unique attenuation abilities of laser properties(e.g.repetition rate,energy,incident angle,etc)by persistent bubbles with different curvatures.This research represents a straightforward and cost-effective approach to diversifying the achievable hierarchical micro/nanostructures for a multitude of applications.

Engineering hierarchical metal-organic@metal-DNA heterostructures for combinational tumor treatment

Development of simple methods for controlled integration of DNA molecules with metal-organic frameworks(MOFs)is important for various biomedical applications,yet remains a challenge.Herein,a simple and general approach to load DNA on the surface of MOFs is developed via one-pot self-assembly of DNA and FeII ions on nanoscale MOFs,resulting in hierarchical core-shell nanostructures of metal-organic@metal-DNA coordination polymers.The strategy enables assembly of DNA molecules on MOFs with ultra-high contents and precise controllability.By incorporation of a chemotherapeutic drug into the Fe-DNA shell,the systems allow to integrate chemotherapy and gene therapy with photodynamic therapy for combinational tumor treatment.Moreover,the hybrid nanostructures enable light-triggered production of cytotoxic singlet oxygen,which further boosts the endosomal escape of the system for an enhanced gene silencing efficacy and thus improved therapeutic outcome.This work highlights a robust approach for the construction of coordination-based drug delivery systems to combat tumor.

Directional sliding of water:biomimetic snake scale surfaces

Bioinspired superhydrophobic surfaces have attracted many industrial and academic interests in recent years.Inspired by unique superhydrophobicity and anisotropic friction properties of snake scale surfaces,this study explores the feasibility to produce a bionic superhydrophobic stainless steel surface via laser precision engineering,which allows the realization of directional superhydrophobicity and dynamic control of its water transportation.Dynamic mechanism of water sliding on hierarchical snake scale structures is studied,which is the key to reproduce artificially bioinspired multifunctional materials with great potentials to be used for water harvesting,droplet manipulation,pipeline transportation,and vehicle acceleration.

Three-dimensional noble-metal nanostructure: A new kind of substrate for sensitive, uniform, and reproducible surface-enhanced Raman scattering

Surface-enhanced Raman spectroscopy （SERS） is a powerful vibrational spectroscopy technique for highly sensitive structural detection of low concentration analyte. The SERS activities largely depend on the topography of the substrate. In this review, we summarize the recent progress in SERS substrate, especially focusing on the three-dimensional （3D） noble-metal substrate with hierarchical nanostructure. Firstly, we introduce the background and general mechanism of 3D hierarchical SERS nanostructures. Then, a systematic overview on the fabrication, growth mechanism, and SERS property of various noble-metal substrates with 3D hierarchical nanostructures is presented. Finally, the applications of 3D hierarchical nanostructures as SERS substrates in many fields are discussed.

Self-Organizing Evolution of Anodized Oxide Films on Ti-25Nb-3Mo-2Sn-3Zr Alloy and Hydrophilicity

In the present work,hierarchical nanostructured titanium dioxide(TiO2) films were fabricated on Ti-25Nb-3Mo-2Sn-3Zr(TLM) alloy for biomedical applications via one-step anodization process in ethylene glycolbased electrolyte containing 0.5wt% NH4F.The nanostructured TiO2 films exhibited three distinct types depending on the anodization time:top irregular nanopores(INP)/beneath regular nanopores(RNP),top INP/middle regular nanotubes(RNT)/bottom RNP and top RNT with underlying RNP.The evolution of the nanostructured TiO2 films with anodization time demonstrated that self-organizing nanopores formed at the very beginning and individual nanotubes originated from underlying nanopore dissolution.Furthermore,a modified two-stage self-organizing mechanism was introduced to illustrate the growth of the nanostructured TiO2 films.Compared with TLM titanium alloy matrix,the TiO2 films with special nano-structure hold better hydrophilicity and higher specific surface area,which lays the foundation for their biomedical applications.

Hierarchically nanostructured nitrogen-doped porous carbon multilayer confining Fe particles for high performance hydrogen evolution

Precise assembly of active component with sophisticated confinement in electrocatalyst are promising to increase the active site exposure for enhanced hydrogen evolution reaction(HER).Here,PCN-333 films with mesopores are firstly assembled on titanium carbide MXene with the assistance of atomic layer deposited oxide nanomembrane.With the whereafter pyrolysis process,the composite is converted to Ndoped porous carbon multi-layer containing Fe nanoparticles.The strong confinement of Fe active particle in carbon as well as great contact between metal and carbon effectively enhance active site exposure.Furthermore,this multi-layer porous structure provides high specific surface area and plentiful mesopores for electrolyte penetration.Due to the structural advantage,the composite can be well functioned in both acid and alkaline electrolytes with excellent HER performance,e.g.,low overpotential/Tafel slope.The present work may have great potential in developing high efficiency transition-metal based electrocatalysts.

Polar solvent induced in-situ self-assembly and oxygen vacancies on Bi_(2)MoO_(6)for enhanced photocatalytic degradation of tetracycline

It has been proved to be an effective route to efficiently ameliorate photocatalytic performance of catalysts via designing three-dimensional(3D)hierarchical nanostructures and constructing oxygen vacancies(VOs).However,controlling the self-assembly of organization into 3D hierarchical nanostructures while introducing VOs in photocatalysts remains a challenge.Herein,we reported an ethylene glycol(EG)mediated approach to craft 3D hydrangea-structure Bi_(2)MoO_(6)with VOs for efficient photocatalytic degradation of tetracycline.Through manipulating the EG concentration during the fabrication process,the influence of EG concentration on the Bi_(2)MoO_(6)structure was systematically investigated.EG could promote the self-assembly of Bi_(2)MoO_(6)nanosheets to form a 3D hierarchical structure.Compared with 2D nanoplates,3D hierarchical architecture enhanced the surface area and the amount of active sites of Bi_(2)MoO_(6).In addition,the reduction effect of EG on metallic oxide enabled the generation of VOs in Bi_(2)MoO_(6).The VOs adjusted the electronic structure of Bi_(2)MoO_(6),which not only enhanced the light harvesting,but also facilitated the simultaneous utilization of photo-induced electrons and holes to form reactive oxygen species(·O2−and·OH)for the efficient tetracycline decomposition.3D Bi_(2)MoO_(6)hydrangea with VOs achieved a 79.4%removal efficiency of tetracycline after 75 min.This work provides a simple yet robust EG-mediated strategy,which not only promotes the self-assembly of nano-catalysts into 3D hierarchical architectures,but also crafts tunable VOs for highly efficient photocatalysis.

Construction of hierarchical three-dimensional interspersed flower-like nickel hydroxide for asymmetric supercapacitors

Low-cost and easily obtainable electrode materials are crucial for the application of supercapacitors.Nickel hydroxides have recently attracted intensive attention owning to their high theoretical specific capacitance,high redox activity,low cost,and eco-friendliness.In this study,novel three-dimensional （3D） interspersed flower-like nickel hydroxide was assembled under mild conditions.When ammonia was used as the precipitant and inhibitor and CTAB was used as an exfoliation agent,the obtained exfoliated ultrathin Ni（OH）2 nanosheets were assembled into 3D interspersed flower-like nickel hydroxide.In this novel 3D structure,the ultrathin Ni（OH）2 nanosheets not only provided a large contact area with the electrolyte,reducing the polarization of the electrochemical reaction and providing more active sites,but also reduced the concentration polarization in the electrode solution interface.Consequently,the utilization efficiency of the active material was improved,yielding a high capacitance.The electrochemical performance was improved via promoting the electrical conductivity by mixing the as-synthesized Ni（OH）2 with carbon tubes （N-4-CNT electrode）,yielding excellent specific capacitances of 2,225.1 F＆#183;g-1 at 0.5 A＆#183;g-1 in a three-electrode system and 722.0 F＆#183;g-1 at 0.2 A＆#183;g-1 in a two-electrode system.The N-4-CNT//active carbon （AC） device exhibited long-term cycling performance （capacitance-retention ratio of 111.4% after 10,000 cycles at 5 A＆#183;g-1） and a high specific capacitance of 180.5 F＆#183;g-1 with a high energy density of 33.5 W＆#183;h＆#183;kg-1 and a power density of 2,251.6 W＆#183;kg-1.

Femtosecond laser induced simultaneous functional nanomaterial synthesis,in situ deposition and hierarchical LIPSS nanostructuring for tunable antireflectance and iridescence applications

Femtosecond laser induced periodic surface structures(LIPSSs)are excellent biomimetic iridescent antireflective interfaces.In this work,we demonstrate the feasibility to develop tunable iridescent antireflective surfaces via simultaneous synthesis of functional metal-oxide nanomaterials,in situ deposition and hierarchical LIPSSs nanostructuring by means of femtosecond laser ablation(fs-LA)of tungsten(W)and molybdenum(Mo)in air.Adjusting the scanning interval from 1μm to 20μm allows the modulation of particle deposition rates on LIPSSs.Diminishing the scan interval enables a higher particle deposition rate,which facilitates the development of better UV-to-MIR ultrabroadband antireflective surfaces with a less pronounced iridescence.Through comparing the reflectance of hierarchical LIPSSs with different densities of loosely/tightly deposited particles,it is found that the deposited WO_(x)and MoO_(x)particle aggregates have high UV-to-MIR ultrabroadband absorbance,especially extraordinary in the MIR range.Loosely deposited particles which self-assembly into macroporous structures outperform tightly deposited particles for ultrabroadband antireflective applications.The presence of loosely deposited MoO_(x)and WO_(x)particle absorbers can cause up to 80%and 60%enhancement of antireflectance performances as compared to the tightly particle deposited LIPSSs samples.One stone of"fs-LA technique"with three birds of(particle generation,in situ deposition and LIPSS hierarchical nanostructuring)presented in this work opens up new opportunities to tune the reflectance and iridescence of metallic surfaces.