Strong field ionization of molecules on the surface of nanosystems

Besides the diverse investigations on the interactions between intense laser fields and molecular systems,extensive research has been recently dedicated to exploring the response of nanosystems excited by well-tailored femtosecond laser fields.Due to the fact that nanostructures hold peculiar effects when illuminated by laser pulses,the underlying mechanisms and the corresponding potential applications can make significant improvements in both fundamental research and development of novel techniques.In this review,we provide a summarization of the strong field ionization occurring on the surface of nanosystems.The molecules attached to the nanoparticle surface perform as the precursor in the ionization and excitation of the whole nanosystem,the fundamental processes of which are yet to be discovered.We discuss the influence on nanoparticle constituents,geometric shapes and sizes,as well as the specific waveforms of the excitation laser fields.The intriguing characteristics observed in surface ion emission reflect how enhanced near field affects the localized ionizations and nanoplasma expansions,thereby paving the way for further precision controls on the light-and-matter interactions in the extreme spatial temporal levels.

Simultaneous low extinction and high local field enhancement in Ag nanocubes

We theoretically investigate surface plasmon resonance properties in Au and Ag cubic nanoparticles and find a novel plasmonic mode that exhibits simultaneous low extinction and high local field enhancement properties. We analyse this mode from different aspects by looking at the distribution patterns of local field intensity, energy flux, absorption and charge density. We find that in the mode the polarized charge is highly densified in a very limited volume around the corner of the nanocube and results in very strong local field enhancement. Perturbations of the incident energy flux and light absorption are also strongly localized in this small volume of the corner region, leading to both low absorption and low scattering cross section. As a result, the extinction is low for the mode. Metal nanoparticles involving such peculiar modes may be useful for constructing nonlinear compound materials with low linear absorption and high nonlinearity.

Coherent control of negative refraction based on local-field enhancement and dynamically induced chirality

This paper studies the electromagnetic response of a coherently driven dense atomic ensemble to a weak probe. It finds that negative refraction with little absorption may be achieved in the presence of local-field enhanced interaction and dynamically induced chirality. The complex refractive index governing the probe refraction and absorption depends critically on the atomic density, the steady population distribution, the coherence dephasings, and the frequency de- tunings, and is also sensitive to the phase of the driving field because the photonic transition paths form a close loop. Thus, it can periodically tune the refractive index at a fixed frequency from negative to positive values and vice versa just by modulating the driving phase. Moreover, the optimal negative refraction is found to be near the probe magnetic resonance, which then requires the electric fields of the probe and the drive being on two-photon resonance due to the dipole synchronisation.

Ultrafast dynamics of femtosecond laser-induced high spatial frequency periodic structures on silicon surfaces

Femtosecond laser-induced periodic surface structures(LIPSS)have been extensively studied over the past few decades.In particular,the period and groove width of high-spatial-frequency LIPSS(HSFL)is much smaller than the diffraction limit,making it a useful method for efficient nanomanufacturing.However,compared with the low-spatial-frequency LIPSS(LSFL),the structure size of the HSFL is smaller,and it is more easily submerged.Therefore,the formation mechanism of HSFL is complex and has always been a research hotspot in this field.In this study,regular LSFL with a period of 760 nm was fabricated in advance on a silicon surface with two-beam interference using an 800 nm,50 fs femtosecond laser.The ultrafast dynamics of HSFL formation on the silicon surface of prefabricated LSFL under single femtosecond laser pulse irradiation were observed and analyzed for the first time using collinear pump-probe imaging method.In general,the evolution of the surface structure undergoes five sequential stages:the LSFL begins to split,becomes uniform HSFL,degenerates into an irregular LSFL,undergoes secondary splitting into a weakly uniform HSFL,and evolves into an irregular LSFL or is submerged.The results indicate that the local enhancement of the submerged nanocavity,or the nanoplasma,in the prefabricated LSFL ridge led to the splitting of the LSFL,and the thermodynamic effect drove the homogenization of the splitting LSFL,which evolved into HSFL.

Numerical analysis of surface plasmon nanocavities formed in thickness-modulated metal-insulator-metal waveguides

The enhancement characteristics of the local field in the surface plasmon nanocavities are investigated numerically. The cavity is constructed by placing a defect structure in the thickness-modulated metal-insulator-metal waveguide Bragg gratings. The characteristic impedance based transfer matrix method is used to calculate the transmission spectra and the resonant wavelength of the cavities with various geometric parameters. The finite-difference time- domain method is used to obtain the field pattern of the resonant mode and validate the results of the transfer matrix method. The calculation and simulation results reveal the existence of resonant wavelength shift and intensity variation with structural parameters, such as the modulation period of the gratings, the length and the width of the defect structure. Both numerical analysis and theoretical interpretation on these phenomena are given in details.

Direct imaging of the near field and dynamics of surface plasmon resonance on gold nanostructures using photoemission electron microscopy

Localized surface plasmon resonance(LSPR)can be supported by metallic nanoparticles and engineered nanostructures.An understanding of the spatially resolved near-field properties and dynamics of LSPR is important,but remains experimentally challenging.We report experimental studies toward this aim using photoemission electron microscopy(PEEM)with high spatial resolution of sub-10 nm.Various engineered gold nanostructure arrays(such as rods,nanodisk-like particles and dimers)are investigated via PEEM using near-infrared(NIR)femtosecond laser pulses as the excitation source.When the LSPR wavelengths overlap the spectrum of the femtosecond pulses,the LSPR is efficiently excited and promotes multiphoton photoemission,which is correlated with the local intensity of the metallic nanoparticles in the near field.Thus,the local field distribution of the LSPR on different Au nanostructures can be directly explored and discussed using the PEEM images.In addition,the dynamics of the LSPR is studied by combining interferometric time-resolved pump-probe technique and PEEM.Detailed information on the oscillation and dephasing of the LSPR field can be obtained.The results identify PEEM as a powerful tool for accessing the near-field mapping and dynamic properties of plasmonic nanostructures.

Fluorescence enhancement of acridine orange in a water solution by Au nanoparticles

The surface enhanced fluorescence effect of acridine orange fluorophore in the proximity of Au nanoparticles has been investigated experimentally in the system of aqueous solution.Significant enhancement of the fluorescence intensity was observed when the system was excited with 532 nm or 442 nm CW lasers.The influence of the distances between neighboring Au particles as well as that between the fluorophore molecules and the Au surface were explored experimentally.The results demonstrated that a compact distribution of metallic particles was able to produce stronger fluorescence enhancement.Proper separation between the fluorophore molecules and the metal surface was favorable for a better enhancement.

High resolution and high signal-to-noise ratio imaging with nearfield high-order optical signals

The properties of near-field optics have always been the focus of nano-measurement technology.The 11th order effective nearfield optical signal with an incident laser wavelength of 1,550 nm is obtained using a platinum-coated optical probe(Pt–Si probe).The experimental results show that the local electric field intensity of the Pt–Si probe is nearly 30 times higher than that of silicon probe(Si probe).Therefore,the highest 7th order near-field optical imaging results are obtained with the Pt–Si probe.Further,near-field optical imaging is performed on samples such as gold grids and carbon nanotubes using the Pt–Si probe.The measurement results show that the high-order signal has the characteristics of less background,higher signal-to-noise ratio,and resolution up to 5.7 nm.

Synthesis and Photoluminescence Enhancement of Silver Nanoparticles Decorated Porous Anodic Alumina

Silver nanoparticles（Ag NPs） were successfully assembled in porous anodic alumina（AAO） templates via a green silver mirror reaction.The Ag NPs/AAO composite templates then were characterized by field emission scanning electron microscopy（FESEM）,energy-dispersive X-ray microanalysis（EDX）,and X-ray diffraction（XRD）.Furthermore,the photoluminescence（PL） properties were also investigated.Compared with the blank AAO,the PL intensity of Ag NPs/AAO templates are enhanced and the maximum enhancement is 2.58 times.Based on the local electric field enhancement effect,the theoretical values were also deduced,which are basically coincident with the experimental.

A flat-based plasmonic fiber probe for nanoimaging

The difficulty of obtaining high-intensity localized light spots for optical probes leads to their lack of good applications in nanoimaging.Here we demonstrate a Fabry–Pérot resonance flat-based plasmonic fiber probe(FPFP).The simulation results show that the probe can obtain a nanofocusing spot at the tip with the radially polarized mode.The Fabry–Pérot interference structure is used to control the plasmon propagation on the surface of the probe,it effectively improves the local spot intensity at the tip.Furthermore,the experimental results verify that the FPFP(tip curvature radius is 20 nm)prepared by chemical etching method can obtain a nanofocusing spot at the tip.The nanoimaging of the gold slit structure demonstrates the nanoimaging capability of the FPFP,the 36.9 nm slit width is clearly identified by the FPFP.

Design of a sector bowtie nano-rectenna for optical power and infrared detection

We designed a sector bowtie nanoantenna integrated with a rectifier （Au-TiOx-Ti diode） for collect- ing infrared energy. The optical performance of the metallic bowtie nanoantenna was numerically investigated at infrared frequencies （5-30 μm） using three-dimensional frequency-domain electro- magnetic field calculation software based on the finite element method. The simulation results indi- cate that the resonance wavelength and local field enhancement are greatly affected by the shape and size of the bowtie nanoantenna, as well as the relative permittivity and conductivity of the dielectric layer. The output current of the rectified nano-rectenna is substantially at nanoampere magnitude with an electric field intensity of 1 V/m. Moreover, the power conversion efficiency for devices with three different substrates illustrates that a substrate with a larger refractive index yields a higher efficiency and longer infrared response wavelength. Consequently, the optimized structure can pro- vide theoretical support for the design of novel optical rectennas and fabrication of optoelectronic devices.