Characterization of Parallel β-Sheets at Interfaces by Chiral Sum Frequency Generation Spectroscopy

Fu, Li; Wang, Zhuguang; Psciuk, Brian T.; Xiao, Dequan; Batista, Víctor S.; Yan, Elsa C. Y.

doi:10.1021/acs.jpclett.5b00326

Cited by 33 publications

(48 citation statements)

References 42 publications

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“…18 SFG-VS study of surface chirality was subsequently developed for simple liquid surfaces and biomolecular surfaces using the chiral intensity measurements. 15,[19][20][21][22][23][24][25] Amongst these studies, we find that the observations of the chiral SFG-VS spectra for the N-H group in the 3000-3500cm -1 range in the folded peptides and proteins are most striking. 15,24,[26][27] Since the unfolded N-H does not give any chiral SFG-VS signal, this characteristic N-H chiral signature can be used to reveal the hydrogen-boning structure of the folded peptides and proteins, as well as to study the folding and unfolding processes of peptides and proteins.…”

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confidence: 87%

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N–H Chirality in Folded Peptide LK₇β Is Governed by the C_α–H Chirality

Hou

et al. 2020

J. Phys. Chem. Lett.

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Recent chiral sum-frequency generation vibrational spectroscopy (cSFG-VS) measurements revealed that the two N-H stretching modes in the 3000-3500 cm-1 range in folded protein and peptide exhibit chiral characteristics. Here we report the first phase-resolved sub-wavenumber high-resolution broadband SFG-VS (HR-BB-SFG-VS) measurement of the LK 7 β peptide. The results show that this chiral N-H band consists of four, instead of two, distinctive peaks, and they are with two groups of opposite spectral phases. Moreover, the phases of these N-H peaks completely flip from the L-LK 7 β to the D-LK 7 β peptide, suggesting that the chirality of the N-H in the folded LK 7 β peptide is completely governed by the chirality of the C α-H of the amino acids. This discovery provides clue on why proteins in nature are composed of α-amino acids rather than βor γ-amino acids, and may help us understand the question on the origin of life.

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confidence: 87%

“…27 Similar N-H spectra were also observed for several proteins, but detailed analysis of these spectra is yet to be reported. [24][25] Further studies on these chiral N-H or O-H bands need to be explored.…”

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confidence: 99%

N–H Chirality in Folded Peptide LK₇β Is Governed by the C_α–H Chirality

Hou

et al. 2020

J. Phys. Chem. Lett.

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“…In addition to the conventional techniques, several spectroscopic characterizations have been improved for the specific requirements of sample analysis. For example, the analysis of peptide assemblies at the interface is quite challenging using conventional methods, but thesum frequency generation (SFG) spectroscopy technique provides a new opportunity foranalysing thesecondary structure and the molecular organization of the peptide assemblies at the lipidwater and solid-air interfaces [294,295]. The structural dynamics of surface-bonded peptide monolayers hasbeen studied using a 2D SFG approach, and IR spectra were used to demonstrate that the helical structure of the soluble peptide is retained following its incorporation onto a gold surface [296].…”

Section: Spectroscopic Analysismentioning

confidence: 99%

Self-assembled peptide nanostructures for functional materials

et al. 2016

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Nature is an important inspirational source for scientists, and presents complex and elegant examples of adaptive and intelligent systems created by self-assembly. Significant effort has been devoted to understanding these sophisticated systems. The self-assembly process enables us to create supramolecular nanostructures with high order and complexity, and peptide-based self-assembling building blocks can serve as suitable platforms to construct nanostructures showing diverse features and applications. In this review, peptide-based supramolecular assemblies will be discussed in terms of their synthesis, design, characterization and application. Peptide nanostructures are categorized based on their chemical and physical properties and will be examined by rationalizing the influence of peptide design on the resulting morphology and the methods employed to characterize these high order complex systems. Moreover, the application of self-assembled peptide nanomaterials as functional materials in information technologies and environmental sciences will be reviewed by providing examples from recently published high-impact studies.

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“…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. This microscope development should pave the way for implementing HD VSFG imaging in a broad range of applications in biophysics, 43 materials 44 and surface sciences. 45,46 The core experimental setup of HD VSFG microscope is illustrated in Figure 1.…”

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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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Characterization of Parallel β-Sheets at Interfaces by Chiral Sum Frequency Generation Spectroscopy

Cited by 33 publications

References 42 publications

N–H Chirality in Folded Peptide LK₇β Is Governed by the C_α–H Chirality

N–H Chirality in Folded Peptide LK₇β Is Governed by the C_α–H Chirality

Self-assembled peptide nanostructures for functional materials

Self-Phase-Stabilized Heterodyne Vibrational Sum Frequency Generation Microscopy

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Characterization of Parallel β-Sheets at Interfaces by Chiral Sum Frequency Generation Spectroscopy

Cited by 33 publications

References 42 publications

N–H Chirality in Folded Peptide LK7β Is Governed by the Cα–H Chirality

N–H Chirality in Folded Peptide LK7β Is Governed by the Cα–H Chirality

Self-assembled peptide nanostructures for functional materials

Self-Phase-Stabilized Heterodyne Vibrational Sum Frequency Generation Microscopy

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Product

Resources

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N–H Chirality in Folded Peptide LK₇β Is Governed by the C_α–H Chirality

N–H Chirality in Folded Peptide LK₇β Is Governed by the C_α–H Chirality