Elsevier

Vacuum

Volume 157, November 2018, Pages 414-421
Vacuum

Thin films composed of Au nanoparticles embedded in AlN: Influence of metal concentration and thermal annealing on the LSPR band

https://doi.org/10.1016/j.vacuum.2018.09.013Get rights and content

Highlights

  • Nanocomposite films containing Au dispersed in AlN were deposited by sputtering.

  • Au nanoparticles growth was promoted by thermal annealing.

  • Au nanoparticles dispersed in the AlN matrix induced plasmonic responses.

  • LSPR bands appeared at 500 °C, positioned in the range 520–540 nm.

Abstract

Nanocomposite thin films, with noble nanoparticles dispersed in a dielectric matrix, are known to present unique optical properties. Based on the Localized Surface Plasmon Resonance (LSPR) phenomenon, these “nanoplasmonic” materials are the basis of a wide range of technological applications, namely (bio)molecular LSPR-sensors. They are regulated by the concentration, size, shape and distribution of the nanoparticles and dielectric environment properties. In this work, the possibility of using aluminium nitride (AlN) as a host dielectric matrix for LSPR films was evaluated. For this purpose, nanocomposite Au:AlN films were prepared by magnetron sputtering, followed by thermal annealing to promote the growth of the nanoparticles. Three sets of films were deposited with atomic Au concentrations of 2.2, 4.4 and 6.0 at.%. LSPR bands appeared from the temperature of 500 °C, with resonance positions of 520–540 nm. The films showed potential to be tested in LSPR-sensing applications due to their optical responses.

Introduction

Nanocomposite materials containing plasmonic metallic nanoparticles, such as Au or Ag, dispersed in a dielectric matrix have been receiving special attention in several areas of science and technology [[1], [2], [3], [4], [5], [6], [7], [8]]. Most of the applications are based on the Localized Surface Plasmon Resonance (LSPR) phenomenon, which arise from the interaction of the noble nanoparticles with an incident electromagnetic field [9], resulting in charge density oscillations confined in the metallic nanoparticles. This effect can give rise to strong absorption bands and the enhancement of the electromagnetic field near the nanoparticles [[10], [11], [12], [13], [14]]. Due to these unique optical properties, nanoplasmonic materials have been widely studied [[15], [16], [17], [18], [19], [20], [21], [22]]. Furthermore, their optical responses can be tailored by geometric characteristics (size, shape and distribution) of the nanoparticles and dielectric properties of the host matrix, presenting tuneable LSPR bands within the visible range. For that reason, this type of plasmonic thin films are being designed and produced to be used in a wide range of technological applications [[23], [24], [25], [26], [27], [28], [29]], particularly in plasmonic sensing such as the detection of gas molecules and biological agents [[30], [31], [32]].

In recent works, it was shown that the production of Au:TiO2 films by reactive magnetron sputtering (using a composite Ti-Au target) followed by post-deposition heat-treatment is a straightforward way to obtain nanoplasmonic thin films, where Au nanoparticles are embedded in the TiO2 matrix [5,22,33]. It was possible to obtain well defined Transmittance LSPR (T-LSPR) bands, associated to Au nanoparticles’ growth and coalescence, highly dependent of the deposition conditions and heat treatment temperatures [9,22,[33], [34], [35], [36], [37], [38]].

Envisaging the development of optical sensors based on LSPR effect, different sets of nanoplasmonic Au:AlN films, with variable Au concentrations, were prepared using a similar experimental procedure as the Au:TiO2 system The plasmonic metal concentration and annealing temperature were both changed in order to study their influence on the structural and morphological properties of the films. The chemical composition and structural changes (induced by thermal annealing at different temperatures) were then correlated with the optical response (transmittance and reflectance) and LSPR behaviour of the films.

Section snippets

Experimental details

The different sets of Au:AlN films were prepared by reactive DC magnetron sputtering using an aluminium target (200 × 100 × 6 mm3) with 99.8% purity. Small Au disks (pellets) with 99.99% purity, each one with surface area of 16 mm2 and 0.5 mm thick, were symmetrically placed on the preferential erosion zone of the Al target. In order to increment the atomic concentration of the noble metal in the matrix, the films were deposited with three different fluxes of sputtered Au atoms, by simply

Deposition rate

The deposition process depends on several factors (applied current, working and reactive gas partial pressures, etc.) that can influence the deposition kinetics and, consequently, the characteristics and properties of the thin films produced [39,[42], [43], [44], [45]]. In this particular case it is of primordial importance to understand the influence of the area of the Au pellets in the evolution of the deposition (growth) rate of the films. The results are plotted in Fig. 2.

The deposition

Conclusions

In order to study the influence of Au concentration and annealing temperature on the structure, morphology and optical behaviour of Au:AlN nanoplasmonic thin films, three different sets of films were prepared. The films were deposited by reactive DC magnetron sputtering using an aluminium target with small Au pellets on its preferential erosion zone and posteriorly submitted to in-air thermal treatments at different temperatures.

Regarding the characteristics of the deposition process, the

Conflicts of interest

The authors certify that there is no conflict of interest regarding this study.

Acknowledgements

This work is financed by National Funds through FCT - Portuguese National Funding Agency for Science, Research and Technology, in the framework of the project PTDC/FIS-NAN/1154/2014 (FCT Projet 9471-RIDTI Reforçar a Investigação, o Desenvolvimento Tecnológico e a Inovação), co-financed by FEDER (POCI-01-0145-FEDER-016902). This research was also sponsored by FCT in the framework of the Strategic Funding UID/FIS/04650/2013. The authors also acknowledge project CICECO-Aveiro Institute of

References (52)

  • S. Berg et al.

    Fundamental understanding and modeling of reactive sputtering processes

    Thin Solid Films

    (2005)
  • N.P. Barradas et al.

    Advanced physics and algorithms in the IBA DataFurnace

    Nucl. Instrum. Methods Phys. Res. Sect. B Beam Interact. Mater. Atoms

    (2008)
  • R.C. Adochite et al.

    The influence of annealing treatments on the properties of Ag:TiO2 nanocomposite films prepared by magnetron sputtering

    Appl. Surf. Sci.

    (2012)
  • S. Berg et al.

    Resputtering effects during ion beam assisted deposition and the sputter yield amplification effect

    Surf. Coating. Technol.

    (1996)
  • A. Politano et al.

    Electronic properties of gold thin films studied by electron energy loss spectroscopy

    Gold Bull.

    (2009)
  • J.H. Hodak et al.

    Electron-phonon coupling dynamics in very small (between 2 and 8 nm diameter) Au nanoparticles

    J. Chem. Phys.

    (2000)
  • G. Walters et al.

    The incorporation of noble metal nanoparticles into host matrix thin films: synthesis characterisation and applications

    J. Mater. Chem.

    (2009)
  • N.M. Figueiredo et al.

    Optical properties and refractive index sensitivity of reactive sputtered oxide coatings with embedded Au clusters

    J. Appl. Phys.

    (2014)
  • J. Borges et al.

    Broadband optical absorption caused by the plasmonic response of coalesced Au nanoparticles embedded in a TiO2 matrix

    J. Phys. Chem. C

    (2016)
  • S.K. Ghosh et al.

    Interparticle coupling effect on the surface plasmon resonance of gold nanoparticles: from theory to applications

    Chem. Rev.

    (2007)
  • E. Hutter et al.

    Exploitation of localized surface plasmon resonance

    Adv. Mater.

    (2004)
  • J. Toudert et al.

    Advanced optical effective medium modeling for a single layer of polydisperse ellipsoidal nanoparticles embedded in a homogeneous dielectric medium: surface plasmon resonances

    Phys. Rev. B Condens. Matter

    (2012)
  • A. Politano et al.

    Dispersion and damping of gold surface plasmon

    Plasmonics

    (2008)
  • J.M. Pitarke et al.

    Theory of surface plasmons and surface-plasmon polaritons

    (2006)
  • M. Torrell et al.

    Tuning of the surface plasmon resonance in TiO2/Au thin films grown by magnetron sputtering: the effect of thermal annealing

    J. Appl. Phys.

    (2011)
  • Y. Sun et al.

    Shape-controlled synthesis of gold and silver nanoparticles

    Science

    (2002)
  • Cited by (24)

    • Observation of negative photoresponse in joule-heated Au/Cu<inf>2</inf>SnS<inf>3</inf> ternary chalcogenide thin film deposited by low energy pulsed laser deposition

      2022, Optical Materials
      Citation Excerpt :

      The same tetragonal (I-42m) structure was observed also in CTS2 and CTS3 thin films. In the CTS2 XRD pattern, two more peaks were observed at 2θ = 38.40° and 44.61° that can be attributed to the planes (111) and (002) the cubic structure of Au matrix (ICCD#98-016-3723) indicating the formation of well crystalized Au clusters caused by the agglomeration of Au atoms at 500 °C annealing temperature process [45,46]. The diffraction peaks also appeared at the CTS3 diffraction pattern with higher intensity due to the increase of pulse number that induced more Au nanoparticles depositions.

    • Nanostructured Cr(N,O) based thin films for relative humidity sensing

      2021, Vacuum
      Citation Excerpt :

      The presence of O in the samples can be attributed to the PVD system itself (although a base pressure of 5.0 × 10−4 Pa was set), where studies have demonstrated a low concentration of oxygen, between 10 and 13 at. %, in metallic films of AlN [32]. This means that the water vapor in the system influence the low percentage of O in the production of the metallic films.

    • Nanocomposite Au-ZnO thin films: Influence of gold concentration and thermal annealing on the microstructure and plasmonic response

      2020, Surface and Coatings Technology
      Citation Excerpt :

      The power supply was set to work in the current regulating mode, and the (negative) target potential measured for each deposition was 500 V, 560 V, 570 V and 590 V, respectively for gold pellets area of 0, 32, 64 and 112 mm2. After the depositions, the samples were subjected to an in-air annealing treatment to promote the growth and coalescence of Au nanoparticles, since the heat treatment increases the diffusion of Au atoms throughout the matrix as reported in other works [9,20,39]. The thermal treatments were performed in a programmable furnace (Termolab FP21) at several temperatures, ranging from 200 °C to 600 °C.

    • Thin films of Au-Al<inf>2</inf>O<inf>3</inf> for plasmonic sensing

      2020, Applied Surface Science
      Citation Excerpt :

      In addition, it also allows to tune the position of the LSPR band, shifting it to higher wavelengths as the refractive index of the surrounding medium increases [42]. In recent works, it has been demonstrated that reactive magnetron sputtering, followed by a post-deposition heat-treatment, is a straightforward way to obtain nanoplasmonic thin films exhibiting Transmittance LSPR bands [11,41,49,50]. The LSPR effect of plasmonic thin film can occur after the growth and coalescence of nanoparticles embedded in the matrix, which is highly dependent of the deposition conditions and heat-treatment temperature [11,35,41,50–55].

    • High performance piezoresistive response of nanostructured ZnO/Ag thin films for pressure sensing applications

      2019, Thin Solid Films
      Citation Excerpt :

      % purity), using a custom-made vacuum chamber. The Zn target was customized with different amounts of Ag pellets (with individual area of ~0.2 cm2), symmetrically distributed along the preferential erosion area (~50 cm2) [23], Fig. 1a), in order to tune the silver content in the coatings. The Zn target was located at 70 mm from the substrate holder (Fig. 1b).

    View all citing articles on Scopus
    View full text