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Sample title 6observed in other publications under pulsed illumination ordepending on the material 23,36,37 . In the experiment, the darkregions are identical with the elevated areas, which, whencompared with the simulation, equates to a full movement ofthe material out of the illuminated regions. This is consistentwith the significantly longer illumination times of 20 h in theexperiment, compared to only a few picoseconds in the simulation.We conclude that very short cw or pulsed illuminationcan induce a double peak with maxima at the interfaces of illuminatedand dark regions, while a longer illumination leadsto a maximum in the dark region.In both the simulation and in the experiment, the polarizationof the incident light has no or only a minor impact onthe surface modulation. In the experiment, small bead-likestructures of 10 nm to 20 nm height emerge in the valleys.These are not predicted in the simulation. This differencecould again be due to the different time and length scales ofsimulation and experiment. The illumination times of only picosecondsand stripe sizes of a few nanometres investigatedin the simulation cannot be realized in these experiments andvice versa.The reason for this rare (virtual) independence of SRGformation on polarization could be the high fluence used inthese experiments. While in most SRG experiments, theazopolymer films are illuminated for a few seconds to severalminutes with intensities in the range of tens to hundredsof mWcm −2 , here the films are illuminated for 20 hourwith over 150 mWcm −2 and thus with a significantly higherfluence 4,7,16 . Also in our simulations, the fluence is veryhigh with ... photons per .. Our experiment and simulationare thus consistent with publications claiming polarizationindependentSRG formation under high-intensity cw andpulsed irradiation 7,20,21,23–26 .With regard to the cause of photomigration, the simulationsclearly show that the conversion of light-energy into local heatis a prerequisite for this phenomenon to occur. In the fluenceregime studied here, mass transport appears to take place inthe direction of the negative temperature gradient and can thusbe described my the theory of thermal diffusion 38 .IV.CONCLUSIONSWe have carried out a combined experimental and theoreticalstudy of the surface relief grating formation in the azopolymerpoly-disperse-orange3-methyl-methacrylate. On the experimentalside, azopolymer polymer films were illuminatedwith light patterns of bright and dark stripes created by a spatiallight modulator. The surface profile was subsequentlycharacterized using atom force microscopy. Thus is could beestablished that mass transport occurred away from the brightstripes into the dark stripes. Furthermore, the polarisation directionwas seen to have a minor effect. These experimentalfindings were corroborated by atomistic molecular dynamicssimulations that explicitly modelled the photoisomerisationdynamics and light polarisation. The simulations furthershowed that local heating due to light-absorption is necessaryfor mass transport to occur. In the high-fluence regime investigatedin this work, mass transport appears to be dominated bythe temperature gradient rather than any more subtle effectsrelated to the photoisomerisation dynamics.All AIP journals require that the initial citation of figures ortables be in numerical order. LATEX’s automatic numbering offloats is your friend here: just put each figure environmentimmediately following its first reference (\ref), as we havedone in this example file.ACKNOWLEDGMENTSWe wish to acknowledge the support of the author communityin using REVTEX, offering suggestions and encouragement,testing new versions, . . . .DATA AVAILABILITY STATEMENTThe data that support the findings of this study are availablefrom the corresponding author upon reasonable request.Appendix A: A little more on appendixes1. A subsection in an appendix1 H. Zhang, “Reprocessable photodeformable azobenzene polymers,”Molecules 26, 4455–4484 (2021).2 P. Weis, W. Tian, and S. Wu, “Reprocessable photodeformable azobenzenepolymers,” Chem. Eur. J. 24, 6494–6505 (2021).3 S. Lee, H. S. Kang, and J.-K. Park, “Directional photofluidization lithography:Micro/nanostructural evolution by photofluidic motions of azobenzenematerials,” Adv. Mater. 24, 2069–2103 (2012).4 C. J. Barrett, J. Mamiya, K. G. 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Netti, “Photonic applications of azobenzenemolecules embedded in amorphous polymer,” La Rivista del NuovoCimento 43, 599–629 (2020).11 M. Hendrikx, A. P. Schenning, M. G. Debije, and D. J. Broer, “Lighttriggeredformation of surface topographies in azo polymers,” Crystals 7,231 (2017).12 T. Fukuda, H. Matsuda, T. Shiraga, T. Kimura, M. Kato, N. K. Viswanathan,J. Kumar, and S. K. Tripathy, “Photofabrication of surface relief grating onfilms of azobenzene polymer with different dye functionalization,” Macromolecules33, 4220–4225 (2000).13 C. J. Barrett, A. L. Natansohn, and P. L. Rochon, “Mechanism of opticallyinscribed high-efficiency diffraction gratings in azo polymer films,” TheJournal of Physical Chemistry 100, 8836–8842 (1996).
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