Sum Frequency Generation Imaging Microscopy of Self-Assembled Monolayers on Metal Surfaces: Factor Analysis of Mixed Monolayers

Pikalov, Aleksandr; Ngo, Dien; Lee, Han Ju; Lee, T Randall; Baldelli, Steven

doi:10.1021/acs.analchem.8b01840

Cited by 15 publications

(24 citation statements)

References 36 publications

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“…This group has also shown how factor analysis, which includes principal factor analysis and target factor analysis, can be applied to low-signal vSFG microscope images to reduce the total acquisition time without sacrificing image resolution. 96,97 Within the past few years, vSFG was also extended into three dimensions via holography as demonstrated by Ma et al 98 SFG microscopy that is resonant with electronic transitions, eSFG, is less developed than its vibrational counterpart. There have only been a few reports of eSFG microscopy that have explored chiral solutions 99 and 2D material systems.…”

Section: ■ Interrogating Interfacesmentioning

confidence: 99%

“…Baldelli and co-workers have taken a less conventional approach by implementing compressive-sensing, which they utilized for monitoring molecular adsorption and film formation on metallic surfaces. , An example of vSFG images of self-assembled monolayers depicting the chemicals adsorbed on a copper surface can be seen in Figure . This group has also shown how factor analysis, which includes principal factor analysis and target factor analysis, can be applied to low-signal vSFG microscope images to reduce the total acquisition time without sacrificing image resolution. , Within the past few years, vSFG was also extended into three dimensions via holography as demonstrated by Ma et al…”

Section: Interrogating Interfacesmentioning

confidence: 99%

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Leaving the Limits of Linearity for Light Microscopy

2020

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Nonlinear microscopy has enabled additional modalities for chemical contrast, deep penetration into biological tissues, and the ability to collect dynamics on ultrafast timescales across heterogeneous samples. The additional light fields introduced to a sample offer seemingly endless possibilities for variation to optimize and customize experimentation and the extraction of physical insight. This perspective highlights three areas of growth in this diverse field: the collection of information across multiple timescales, the selective imaging of interfacial chemistry, and the exploitation of quantum behavior for future imaging directions. Future innovations will leverage the work of the studies reviewed here as well as address the current challenges presented.

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Section: ■ Interrogating Interfacesmentioning

confidence: 99%

Section: Interrogating Interfacesmentioning

confidence: 99%

Leaving the Limits of Linearity for Light Microscopy

2020

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“…SAMs on gold substrate patterning were achieved by utilizing microcontact printing (μCP). The process of stamp manufacturing for μCP using PDMS has been described previously . The preparation procedure of the five components and the random pattern sample is shown in Figures a and b, respectively, and is only briefly outlined here.…”

Section: Experimental Sectionmentioning

confidence: 99%

“…Currently, this technique has been applied to a system consisting of five distinct molecules, but it can be extended to larger sample varieties and more complex chemical systems consisting of a larger numbers of species by using a wider spectral range. Isotope labels can also be successfully used due to the ability of FA to resolve spectra at the SFG spectra resolution limit of 5 cm –1 …”

Section: Introductionmentioning

confidence: 99%

Multicolor Chemical Imaging by Sum Frequency Generation Imaging Microscopy of Monolayers on Metal Surfaces

Pikalov

Rodriguez

et al. 2020

J. Phys. Chem. C

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Sum frequency generation imaging microscopy (SFG-IM) is a unique surface-specific technique that can detect the spatial distributions of differing monolayer species based on chemical contrast. Here SFG images of microcontact-patterned multicomponent self-assembled monolayers derived by the adsorption of alkanethiols on gold were analyzed by factor analysis (FA) utilizing a library consisting of SFG alkanethiol spectra to determine the chemical identity and spatial distribution of the patterned monolayers across the images. By utilizing the spectral library as a target test for factor analysis, we correctly identified the monolayer species, and their spatial distributions were mapped. The chemical identity and spatial distribution of a random-pattern multicomponent alkanethiol sample were determined and mapped. Furthermore, utilizing the alkanethiol library, factor analysis was able to identify an unknown monolayer region, the vibrational spectra of which were not present in the target library. The results demonstrate the capability of FA combined with the spectral library to determine the chemical composition and spatial distribution of organic molecules on the surface of multicomponent complex chemical systems acquired by SFG-IM.

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“…The quadratic susceptibility tensor, originating due to electric-dipolar transitions, is zero within the bulk of a centrosymmetric medium and hence the second order response manifests itself mainly at its surface where the inversion symmetry is locally lost. For this reason, the different second order processes have been extensively used as surface probes for these class of materials [19][20][21][22]. Besides providing remarkable non-invasive surface imaging techniques, they have demonstrated tremendous potential for numerous other applications, as in the development of coherent light sources at different frequencies.…”

Section: Introductionmentioning

confidence: 99%

Analytical theory for three wave-mixing processes in a slightly deformed cylinder

Singla,

Mochán

2021

Preprint

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The second order optical response of centrosymmetric materials manifests itself mostly at their surface, being strongly suppressed in their bulk. However, the overall surface response is also suppressed in nanoparticles with a centrosymmetric geometry subjected to homogeneous fields.Nevertheless, nanoparticles with a noncentrosymmetric geometry do exhibit second order optical properties. We develop an analytical theory to investigate the second order optical response of a noncentrosymmetric thin cylinder with a slightly deformed cross-section made up of a centrosymmetric material subjected to two monochromatic fields. We calculate the linear and nonlinear near fields perturbatively using the extent of the deformation away from a circular cross-section as the perturbation parameter. We obtain expressions for the quadratic hyperpolarizabilities in terms of the linear response evaluated at the three frequencies involved. We analyze the spectral features of the nonlinear response functions and explore their resonant structure for a model dielectric cylinder. Furthermore, we evaluate the second order radiated fields, the radiation patterns and efficiency of the different quadratic processes. We obtain a strong competition between electric dipolar, magnetic dipolar and electric quadrupolar contributions even for very small deformations.

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Sum Frequency Generation Imaging Microscopy of Self-Assembled Monolayers on Metal Surfaces: Factor Analysis of Mixed Monolayers

Cited by 15 publications

References 36 publications

Leaving the Limits of Linearity for Light Microscopy

Leaving the Limits of Linearity for Light Microscopy

Multicolor Chemical Imaging by Sum Frequency Generation Imaging Microscopy of Monolayers on Metal Surfaces

Analytical theory for three wave-mixing processes in a slightly deformed cylinder

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