Abstract

We report on fluorescence and second-harmonic generation correlative microscopy of femtosecond direct laser-induced structures in a tailored silver-containing phosphate glass. We compare the spatial distributions of the related permanent electric field and silver clusters. The latter appear to be co-localized where the associated electric potential ensures favorable reduction-oxidation conditions for their formation and stabilization. Space charge separation is shown to occur prior the cluster formation. The associated electric field is a key parameter for silver clustering, thanks to electric field assisted silver ion motion. Future photonic structures combining 3D laser-structured fluorescence and nonlinear optical properties in such tailored glass will require an optimal control of the induced electric field distribution.

Highlights

  • Femtosecond direct laser writing (DLW) in homogeneous glasses gives three-dimensional access to local material modifications at the micro-nanoscale, at the root of chemical [1], mechanical [2] as well as optical [3] contrasts

  • We report on fluorescence and second-harmonic generation correlative microscopy of femtosecond direct laser-induced structures in a tailored silver-containing phosphate glass

  • We compare the spatial distributions of the related permanent electric field and silver clusters

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Summary

Introduction

Femtosecond direct laser writing (DLW) in homogeneous glasses gives three-dimensional access to local material modifications at the micro-nanoscale, at the root of chemical [1], mechanical [2] as well as optical [3] contrasts Such approach already demonstrated an extremely broadband range of fundamental mechanisms and original applications [4,5]. Nonlinear optical contrast has been reported, in a smaller proportion, with third-harmonic generation (THG) [8] and effective second-harmonic generation (SHG), even in an initially centro-symmetric material, thanks to local space charge separation Such buried static electric field induced second-harmonic generation (EFISHG) has largely been reported under thermal poling leading to intense electric fields up to 109 V.m−1 [9,10,11], with a typical thickness of the poled region ranging from 1 to few tens of microns. Such work provides a new interpretation of the sequence of mechanisms at play during fs DLW in our tailored glass

Experimental method
Correlative fluorescence and nonlinear SHG imaging setup
Topologies of laser-induced fluorescence and SHG patterns
Spatial correlation between fluorescence and SHG laser-induced patterns
Electric field Electric potential
Distinct EFISHG and fluorescence build-up processes versus DLW conditions
Conclusion & perspectives
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