Second-harmonic and sum-frequency imaging of organic nanocrystals with photon scanning tunneling microscope

Shen, Yuzhen; Swiatkiewicz, Jacek; Winiarz, Jeffrey G.; Markowicz, Przemyslaw P.; Prasad, Paras N.

doi:10.1063/1.1322629

Cited by 42 publications

(29 citation statements)

References 24 publications

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“…Molecular specific imaging on non-centrosymmetric molecular interfaces and domains [1][2][3][4][5][6][7][8][9][10][11][12] is crucial for understanding structures and dynamics on many inhomogeneous systems, such as chemical reactions on heterogeneous catalysts, 13 protein interactions with lipid bilayers, 14 structure of optical metamatials, 15 and formation of structure color materials. 16 By spatially resolving interfaces and domains, microscopy could obtain domain specific knowledge and mitigate ensemble averaging.…”

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confidence: 99%

“…Using this code, we can differentiate domains with various molecular conformations, which would otherwise be difficult to distinguish using optical imaging techniques 41 or homodyne VSFG microscopes. [4][5][6][7][8][9][10][11][12] We implemented this phase-stable collinear HD VSFG microscope to study a guest-host molecular self-assembly 42 spin-coated on gold. We found that the self-assembly contains non-centrosymmetric domains at sizes from about 20 to 100 μm 2 , and there are mainly two types of domains, which have opposite molecular alignment relative to each other.…”

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confidence: 99%

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Self-Phase-Stabilized Heterodyne Vibrational Sum Frequency Generation Microscopy

2017

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Vibrational sum frequency generation (VSFG) spectroscopy has been a powerful technique to probe molecular structures at non-centrosymmetric media. Recent developed heterodyne (HD) detection can further reveal spectral phase and molecular orientations. Adding imaging capability to an HD VSFG signal can bring spatial visualization capability into this non-linear optical technique. However, it has been a challenge to build an HD VSFG microscope that is both easy to align and has good spectral phase stability -two necessary criterions for the broad application of this technique into various areas of science. Here, we report a fully-collinear HD VSFG microscope, which meets both phase stability and optical alignment requirements that can spatially resolve images of molecular interfaces and domains, with chemical and structural sensitivities. The phase stability is more than nine times better than a Michelson Interferometric HD VSFG microscope. Using this HD VSFG microscope, we study the structures of molecular selfassembly films. Because of the superior phase sensitivity, we successfully identify two molecular domains with different molecular orientations, which we show is not possible to extract from an ensemble-averaged VSFG spectrum or homodyne-detected VSFG image.

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confidence: 99%

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confidence: 99%

Self-Phase-Stabilized Heterodyne Vibrational Sum Frequency Generation Microscopy

2017

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“…Surface SHG Enhancement Induced by Specific Surface Morphology. Surface plasmon-assisted SHG enhancement from metal clusters has been reported for several systems, [32][33][34] including Au nanocluster-deposited Si(111) surfaces. Suni and co-workers [35][36][37][38] studied deposition kinetics of Au nanoclusters grown on p-Si(111) by means of surface plasmon-enhanced SHG and noncontact AFM.…”

Section: Modification Of the Sh-ra Pattern By Cu Depositionmentioning

confidence: 99%

Electrodeposition of Flattened Cu Nanoclusters on a p-GaAs(001) Electrode Monitored by in situ Optical Second Harmonic Generation

et al. 2005

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In situ optical second harmonic generation (SHG) technique was employed to investigate the shape and density of Cu nanoclusters, which were electrochemically formed on p-GaAs(001) electrode surfaces. Since GaAs is not a centrosymmetric medium, a significant portion of SHG signal arises from the bulk dipole susceptibility, but it was possible to separate a surface-induced signal from a bulk-induced signal by choosing an appropriate experimental geometry and appropriate data processing. The rotational anisotropy (RA) pattern of the SHG signal from a p-GaAs(001) electrode changed in both shape and magnitude during potential cycling in an electrolyte solution containing Cu 2+ . The surface plasmon-induced SHG signal from Cu nanoclusters deposited on GaAs was attributed to the modulation source for the RA-SHG pattern. More detailed study was carried out with both in situ SHG and ex situ AFM measurements for Cu nanoclusters deposited by potential step. The results showed that the SHG signal at the present optical geometry was sensitive to the number of oblate or flattened Cu nanoclusters with lateral diameter larger than 30 nm and that the SHG enhancement occurred because of resonant coupling between the surface plasmon induced in the flattened Cu nanoclusters and the near-infrared fundamental light.

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“…In a similar context, it should be highlighted the experiment realized by the Prasad group on nonlinear excitation of organic nanocrystals with a photon scanning tunneling microscope. [14] Our results are discussed in terms of efficiency and polarization properties. Further information about individual nanoparticles' orientation and coherent emission are derived within the defined image defocusing framework first …”

Section: Introductionmentioning

confidence: 99%

Evanescent-Field-Induced Second Harmonic Generation by Noncentrosymmetric Nanoparticles

Bäumner¹,

Bonacina²,

Enderlein³

et al. 2010

Opt. Express

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Abstract:We demonstrate the excitation of second harmonic radiation of noncentrosymmetric nanoparticles dispersed on a planar optical waveguide by the evanescent field of the guided mode. Polarization imaging reveals information on the orientation of the crystal axis of individual nanoparticles. Interference patterns generated from adjacent particles at the second harmonic frequency are -to the authors knowledge -observed for the first time. The actual form of the interference pattern is explained on the basis of a dipole radiation model, taking into account the nanoparticles' orientation, surface effects, and the characteristics of the imaging optics.

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Second-harmonic and sum-frequency imaging of organic nanocrystals with photon scanning tunneling microscope

Cited by 42 publications

References 24 publications

Self-Phase-Stabilized Heterodyne Vibrational Sum Frequency Generation Microscopy

Self-Phase-Stabilized Heterodyne Vibrational Sum Frequency Generation Microscopy

Electrodeposition of Flattened Cu Nanoclusters on a p-GaAs(001) Electrode Monitored by in situ Optical Second Harmonic Generation

Evanescent-Field-Induced Second Harmonic Generation by Noncentrosymmetric Nanoparticles

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