Plasmonic nanofocused four-wave mixing for femtosecond near-field imaging


Femtosecond nonlinear optical imaging with nanoscale spatial resolution would provide access to coupled degrees of freedom and ultrafast response functions on the characteristic length scales of electronic and vibrational excitations. Although near-field microscopy provides the desired spatial resolution, the design of a broadband high-contrast nanoprobe for ultrafast temporal resolution is challenging due to the inherently weak nonlinear optical signals generated in subwavelength volumes. Here, we demonstrate broadband four-wave mixing with enhanced nonlinear frequency conversion efficiency at the apex of a nanometre conical tip. Far-field light is coupled through a grating at the shaft of the tip, generating plasmons that propagate to the apex while undergoing asymptotic compression and amplification, resulting in a nonlinear conversion efficiency of up to 1 × 10–5. We apply this nonlinear nanoprobe to image the few-femtosecond coherent dynamics of plasmonic hotspots on a nanostructured gold surface with spatial resolution of a few tens of nanometres. The approach can be generalized towards spatiotemporal imaging and control of coherent dynamics on the nanoscale, including the extension to multidimensional spectroscopy and imaging.

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Figure 1: FWM of nanofocused surface plasmon polaritons.
Figure 2: FWM dependence on spectral phase of the excitation pulse.
Figure 3: Dynamics of tip-generated FWM.
Figure 4: Femtosecond FWM nanoimaging of coherent plasmon dynamics in gold.
Figure 5: Localization of FWM response in adiabatic nanofocusing.


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The authors acknowledge funding from the National Science Foundation (NSF grant CHE 1306398), AFOSR (grant #FA9550-14-1-0376) and a partner proposal by the Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility from the DOE Office of Biological and Environmental Research at Pacific Northwest National Laboratory (PNNL). PNNL is operated by Battelle for the US DOE under contract DEAC06-76RL01830. R.U. acknowledges support by a Rubicon Grant of the Netherlands Organization for Scientific Research (NWO). The authors thank H. Petek and S. Cundiff for discussions.

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M.B.R., R.U. and V.K. conceived the experiment. R.U. and J.M.A. contributed to designing the experiment. V.K. performed the measurements and analysed the data. V.K. and M.B.R. wrote the manuscript with contributions from R.U. and J.M.A. All authors discussed the results and commented on the manuscript. M.B.R. supervised the project.

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Correspondence to Markus B. Raschke.

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The authors declare no competing financial interests.

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Kravtsov, V., Ulbricht, R., Atkin, J. et al. Plasmonic nanofocused four-wave mixing for femtosecond near-field imaging. Nature Nanotech 11, 459–464 (2016).

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