Self-organized growth of metallic nanoparticles in a thin film under homogeneous and continuous-wave light excitation

Destouches, Nathalie; Crespo‐Monteiro, Nicolas; Vitrant, G.; Lefkir, Yaya; Reynaud, Stéphanie; Épicier, Thierry; Liu, Y.; Vocanson, Francis; Pigeon, Florent

doi:10.1039/c4tc00971a

Cited by 40 publications

(68 citation statements)

References 33 publications

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“…They correspond to a surface mode and a guided mode, respectively. Individually, either of them has already been shown to be capable of triggering self-organized patterns in any of the two directions, 15,[17][18][19] with periods (with respect to the laser wavelength) similar to the ones reported here, but never simultaneously in the same system before, leading only to 2D self-organized patterns. These modes are excited through scattering at heterogeneities and are initially no more than a perturbation signal generated by randomly distributed scatterers, preventing phase matching conditions and an efficient coupling of light in the guiding film.…”

Section: Acsmentioning

confidence: 88%

“…19,21 Self-organized 3D nanostructures can be generated in a certain range of laser fluence and scan speed (see methods) using a high repetition rate fs laser (500 kHz) exciting the localized surface plasmon resonance (LSPR) of Ag NPs. A localized surface plasmon is the result of the confinement of a surface plasmon in a nanoparticle that is smaller than the light wavelength used to excite the plasmon.…”

Section: Resultsmentioning

confidence: 99%

“…15,17 This fact implies the presence of different types of optical modes as the origin of the interference pattern, depending on the system. Quasi-guided modes 19 and surface waves 17 have been identified to be involved in such self-organization mechanisms. However, all NP gratings reported so far have been produced in single planes, buried below or lying at the material surface, as a result of interferences between the incident wave and a single optical mode.…”

mentioning

confidence: 99%

“…Addressing the challenge to modify NPs inside a dielectric matrix, Loeschner and co-workers have reported the generation of gold NP gratings embedded in polymer films using fs laser pulses, 18 while our group triggered the self-organized growth of silver NPs in high-index TiO 2 films with continuous wave (cw) laser light. 19 A common feature of all these self-organized metallic nanostructures is that their period results from the interference of the incident laser wave with optical modes excited in the structures. Interestingly, the dependence of the grating orientation on the laser polarization is not universal, but is found to be either parallel 18,19 or perpendicular.…”

mentioning

confidence: 99%

“…19 A common feature of all these self-organized metallic nanostructures is that their period results from the interference of the incident laser wave with optical modes excited in the structures. Interestingly, the dependence of the grating orientation on the laser polarization is not universal, but is found to be either parallel 18,19 or perpendicular. 15,17 This fact implies the presence of different types of optical modes as the origin of the interference pattern, depending on the system.…”

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confidence: 99%

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Three-Dimensional Self-Organization in Nanocomposite Layered Systems by Ultrafast Laser Pulses

et al. 2017

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Controlling plasmonic systems with nanometre resolution in transparent films and their colors over large non-planar areas is a key issue for spreading their use in various industrial fields. Using light to direct self-organization mechanisms provides high-speed and flexible processes to meet this challenge. Here, we describe a route for the laser-induced self-organization of metallic nanostructures in 3D. Going beyond the production of planar nanopatterns, we demonstrate that ultrafast laser-induced excitation combined with non-linear feedback mechanisms in a nanocomposite thin film can lead to 3D self-organized nanostructured films. The process, which can be extended to complex layered composite systems, produces highly uniform large-area nanopatterns. We show that 3D self-organization originates from the simultaneous excitation of independent optical modes at different depths in the film and is activated by the plasmon-induced charge separation and thermally-induced NP growth mechanisms. This laser color marking technique enables multiplexed optical image encoding and the generated nanostructured Ag NPs:TiO 2 films offer great promise for applications in solar energy harvesting, photocatalysis or photochromic devices. KeywordsUltrafast photonics; Laser-induced self-organization; Nanostructured thin film; plasmonic nanomaterials; plasmonic colors Controlling metallic nanostructures over large non-planar areas with high flexibility and speed is of strategic importance for developing industrial applications of plasmonic systems.

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Section: Acsmentioning

confidence: 88%

Section: Resultsmentioning

confidence: 99%

mentioning

confidence: 99%

mentioning

confidence: 99%

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confidence: 99%

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Three-Dimensional Self-Organization in Nanocomposite Layered Systems by Ultrafast Laser Pulses

et al. 2017

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Temperature rise during laser‐induced self‐organization of nanoparticle gratings revealed by R aman microspectroscopy and electron microscopy

Liu

Vitrant

Saviot

et al. 2016

European Microscopy Congress 2016: Proceedings

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Self‐organization of metallic nanoparticles (NPs) has recently been reported upon visible continuous‐wave (cw) laser exposure [1]. The self‐organized structures are Ag NP gratings embedded in a thin TiO 2 film deposited on glass. Such composite structures exhibit singular visual effects that can find applications in secured traceability. The related optical properties directly depend on the NP size distribution, the average grating period, the organization rate and the TiO 2 thickness and refractive index. These sample features appear to be largely controlled by the temperature rise that occurs during the laser‐induced self‐organization process. The aim of the present contribution is to estimate the plasmon‐induced temperature rise which appears to be strongly influenced by the laser scanning speed. To do so, Raman microspectroscopy and various modes of transmission electron microscopy (TEM) are used. The latter allow accurate information to be acquired on the NP size distributions resulting from different temperature rises, on their localization in the film and on the phase and chemical changes that occur in the film and the substrate surrounding NPs. Finally, we show how such thermal effects can be considerably decreased when using femtosecond (fs) laser pulses to initiate the NP self‐organization. The TiO 2 thin layer used in this work is initially mesoporous and amorphous and contains small silver NP of 1‐3 nm as described in a previously published article [1]. The self‐organized growth of silver NPs is implemented by scanning a laser beam focused on the sample surface at a constant speed. Post mortem Raman microspectroscopy shows that TiO 2 remains amorphous or adopt successively anatase, both anatase and rutile or only rutile crystalline forms for increasing laser scanning speeds, which was confirmed by high resolution TEM micrographs. Further in situ Raman microspectrocopy characterizations also attest an increase in temperature from 200°C to 750°C from low speed to higher speed in a range where anatase is formed; This increase of the temperature when the scanning speed increases was totally unexpected. In addition to TEM crystallographic characterization, scanning electron microscopy (SEM) appeared to be useful to identify different morphologies for anatase and rutile nanocrystals and to study changes in the nanocrystal density as a function of speed. Scanning TEM (STEM) micrographs and electron energy loss spectroscopy (EELS) analysis of sample cross‐sections prepared by focused ion beam (FIB) give further interesting information about the in‐depth structure of samples. Ag nanoparticles are located below the TiO 2 film (Fig. 1a) made of TiO 2 nanocrystals immersed in a Si‐based amorphous phase, in a new interfacial thin amorphous layer mixing both Ti from the initial film and Si from the glass substrate (Fig. 1b). A three‐dimensional reconstruction of the film sample from a series of FIB‐SEM experiments confirms that all Ag NPs are rather spherical and located in a single plane just below the nanocrystalized TiO 2 layer. High angle annular dark field scanning TEM (HAADF STEM) imaging was used to study systematically non‐monotonous changes in the NP size distribution with the temperature rise for many samples. All studies that we have performed so far point out that the temperature rise can be considered as a drawback since it affects the integrity of the supporting material; we present here few results obtained with fs laser pulses in order to investigate a way to self‐organize metallic NPs without high temperature rise in order to preserve the substrate and give the ability to work on softer substrates like plastic ones. Self‐organization can successfully be obtained without altering the substrate top surface (Fig. 1 c‐d). Ag NPs remain localized in the TiO 2 films, which is only locally crystallized around the grown NPs, as attested by STEM‐diffraction maps recorded in TEM. To conclude, this paper demonstrates the interest of a multimodal application of TEM techniques in order to provide a thorough study of the 3D nanostructure and chemical composition of complex samples made of Ag NP gratings embedded in a nanocrystallized TiO 2 film, which result from laser‐induced self‐organization processes. It provides crucial information on thermal effects that drive the laser‐induced self‐organization process.

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Laser‐Empowered Random Metasurfaces for White Light Printed Image Multiplexing

Destouches

Sharma

Vangheluwe

et al. 2021

Adv Funct Materials

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Printed image multiplexing based on the design of metasurfaces has attracted much interest in the past decade. Optical switching between different images displayed directly on the metasurface is performed by altering parameters of the incident light such as polarization, wavelength or incidence angle. When using white light, only two-image multiplexing is implemented with polarization switching. Such metasurfaces are made of nanostructures perfectly controlled individually, which provide high-resolution pixels but small images and involve long fabrication processes. Here, we demonstrate that laser processing of nanocomposites offers a versatile low-cost, high-speed method with large area processing capabilities for controlling the statistical properties of random metasurfaces, allowing up to three-image multiplexing under white light illumination. By controlling independently absorption and interference effects, colors in reflection and transmission can be varied independently yielding two-image multiplexing under white light. Using anisotropy of plasmonic nanoparticles a third image can be multiplexed and revealed through polarization changes. The design strategy, the fundamental properties and the versatility of implementation of these laser-empowered random metasurfaces are discussed. The technique, applied on flexible substrate, can find applications in information encryption or functional switchable optical devices, and offers many advantages for visual security and anticounterfeiting.

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Self-organized growth of metallic nanoparticles in a thin film under homogeneous and continuous-wave light excitation

Abstract: International audienc

Cited by 40 publications

References 33 publications

Three-Dimensional Self-Organization in Nanocomposite Layered Systems by Ultrafast Laser Pulses

Three-Dimensional Self-Organization in Nanocomposite Layered Systems by Ultrafast Laser Pulses

Temperature rise during laser‐induced self‐organization of nanoparticle gratings revealed by R aman microspectroscopy and electron microscopy

Laser‐Empowered Random Metasurfaces for White Light Printed Image Multiplexing

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