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Pulsed Laser Deposition of Thin Films

Pulsed Laser Deposition

Pulsed laser deposition (PLD) typically uses a pulsed nanosecond laser beam to vaporize pellets of target material in a low pressure, typically oxygen-containing, environment. Under these conditions, a nearly stoichiometric “plume” of that material is transported to a heated substrate where the material nucleates to create well-controlled thin films, or layered structures of multiple films, with nanometer-scale precision. This type of synthesis is performed to explore the effects of interfaces, confinement, and coupling between layers. The type of materials are typically complex metal-oxides that contain several atomic elements.

Science Overview

The CNMS pulsed laser deposition facilities are designed for thin film deposition in oxygen, argon, and a mixed ambient, if required. The incident excimer laser beam is delivered to one of four targets using a projection beamline, meaning spot size is easily adjusted and laser fluence at the target is fairly uniform. The benefits of this type of beam delivery are twofold: first, growth rates can be easily tuned to between low rates for superlattices or higher rates for more conventional films, and second, growth parameters are easily reproduced on future user visits as well as being easily translated to other PLD labs. For materials with sufficient structural perfection to also exhibit a layer-by-layer growth mode, film thickness evolution can be monitored using high pressure reflection high energy electron diffraction (RHEED).


The CNMS PLD facilities are used to synthesize a range of thin film materials to explore diverse phenomena ranging from as spin ices and proton conduction to magnetic ordering and morphologically-induced phase composition.


  • Laser source: 248 nm excimer laser, 1 J/pulse, 1 Hz to 20 Hz repetition rate
  • Number of targets: 4 with computer-controlled target sequencing
  • Spot size at target: adjustable from sub millimeter to a few millimeters
  • Fluence at target: adjustable from sub 1 J/cm2 up to 4 J/cm2
  • Deposition rate: adjustable from sub angstroms per laser shot to almost 1 angstrom per laser shot
  • In situ diagnostics: high pressure RHEED
  • Base pressure: 2x10-7 torr
  • Ambient: currently argon or oxygen, pressured controlled to multiple millitorrs up to 100s of millitorrs
  • Heating: radiant up to 800 °C
  • Substrate size: based on laser plume dimensions, typically 5 mm x 5 mm or 10 mm x 10 mm for uniformity.
  • Target-to-substrate: adjustable from 25 mm to 75 mm, but RHEED requires 40 mm.

Recent User Publications

L. Bovo, C.M. Rouleau, D. Prabhakaran, and S.T. Bramwell, Phase transitions in few-monolayer spin ice films, Nature Communications 10, 1219 (2019).

A. Herklotz, S.F. Rus, N. Balke-Wisinger, C.M. Rouleau, E.-J. Guo, A. Huon, K.C. Santosh, R. Roth, X. Yang, C. Vaswani, J. Wang, P. Orth, M.S. Scheurer, and T.Z. Ward, Designing Morphotropic Phase Composition in BiFeO3, Nano Letters 19, 1033 (2019).

K.A. Stoerzinger, X.R. Wang, J. Hwang, R.R. Rao, W.T. Hong, C.M. Rouleau, D. Lee, Y. Yu, E.J. Crumlin, and Y. Shao-Horn, Speciation and Electronic Structure of La1−xSrxCoO3−δ During Oxygen Electrolysis, Topics in Catalysis 61, 2161 (2018).

J. Ding, J. Balachandran, X. Sang, W. Guo, J.S. Anchell, G.M. Veith, C.A. Bridges, Y. Cheng, C.M. Rouleau, J.D. Poplawsky, N. Bassiri-Gharb, R.R. Unocic, and P. Ganesh, The Influence of Local Distortions on Proton Mobility in Acceptor Doped Perovskites, Chemistry of Materials 30, 4919 (2018).

J. Ding, J. Balachandran, X. Sang, W. Guo, G.M. Veith, C.A. Bridges, C.M. Rouleau, J.D. Poplawsky, N. Bassiri-Gharb, P. Ganesh, and R.R. Unocic, Influence of Nonstoichiometry on Proton Conductivity in Thin-Film Yttrium-Doped Barium Zirconate, ACS Applied Materials & Interfaces 10, 4816 (2018).

Y. Fujioka, J. Frantti, C. Rouleau, A. Puretzky, and H.M. Meyer, Vacancy filled nickel‐cobalt‐titanate thin films, Physica Status Solidi (B) 254, 1600799 (2017).

K.A. Stoerzinger, R.R. Rao, X.R. Wang, W.T. Hong, C.M. Rouleau, and Y. Shao-Horn, The role of Ru redox in pH-dependent oxygen evolution on rutile ruthenium dioxide surfaces, Chem 2, 668 (2017).

L. Bovo, C.M. Rouleau, D. Prabhakaran, and S.T. Bramwell, Layer-by-layer epitaxial thin films of the pyrochlore Tb2Ti2O7, Nanotechnology 28, 055708 (2016).

L. Fan, C.B. Jacobs, C.M. Rouleau, and G. Eres, Stabilizing Ir (001) epitaxy on yttria-stabilized zirconia using a thin Ir seed layer grown by pulsed laser deposition, Crystal Growth & Design 17, 89 (2016).