skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

This content will become publicly available on February 28, 2021

Title: In situ molecular imaging of adsorbed protein films in water indicating hydrophobicity and hydrophilicity

Abstract

In situ molecular imaging of protein films adsorbed on a solid surface in water was realized by using a vacuum compatible microfluidic interface and time-of-flight secondary ion mass spectrometry (ToF-SIMS). Amino acid fragments from such hydrated protein films are observed and identified in the positive ion mode and the results are in agreement with reported works on dry protein films. Moreover, water clusters from the hydrated protein films have been observed and identified in both the positive and negative ion mode for a series protein films. Thus the detailed composition of amino acids and water molecules in the hydrated protein films can be characterized, and the protein water microstructures can be revealed by the distinct three-dimensional spatial distribution reconstructed from in situ liquid ToF-SIMS molecular imaging. Furthermore, spectral principal component analysis of amino acid fragment peaks and water cluster peaks provides unique insights into the water cluster distribution, hydrophilicity, and hydrophobicity of hydrated adsorbed protein films in water.

Authors:
; ORCiD logo; ORCiD logo; ; ; ; ORCiD logo; ORCiD logo
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1604767
Alternate Identifier(s):
OSTI ID: 1605412
Report Number(s):
[PNNL-SA-152103]
[Journal ID: ISSN 2045-2322]
Grant/Contract Number:  
[DE-AC05-76RL01830; AC05-76RL01830]
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
[ Journal Volume: 10; Journal Issue: 1]; Journal ID: ISSN 2045-2322
Country of Publication:
United States
Language:
English
Subject:
SALVI, ToF-SIMS, protein, hydrophilicity, hydrophobicity

Citation Formats

Yu, Jiachao, Zhou, Yufan, Engelhard, Mark, Zhang, Yuchen, Son, Jiyoung, Liu, Songqin, Zhu, Zihua, and Yu, Xiao-Ying. In situ molecular imaging of adsorbed protein films in water indicating hydrophobicity and hydrophilicity. United States: N. p., 2020. Web. doi:10.1038/s41598-020-60428-1.
Yu, Jiachao, Zhou, Yufan, Engelhard, Mark, Zhang, Yuchen, Son, Jiyoung, Liu, Songqin, Zhu, Zihua, & Yu, Xiao-Ying. In situ molecular imaging of adsorbed protein films in water indicating hydrophobicity and hydrophilicity. United States. doi:10.1038/s41598-020-60428-1.
Yu, Jiachao, Zhou, Yufan, Engelhard, Mark, Zhang, Yuchen, Son, Jiyoung, Liu, Songqin, Zhu, Zihua, and Yu, Xiao-Ying. Fri . "In situ molecular imaging of adsorbed protein films in water indicating hydrophobicity and hydrophilicity". United States. doi:10.1038/s41598-020-60428-1.
@article{osti_1604767,
title = {In situ molecular imaging of adsorbed protein films in water indicating hydrophobicity and hydrophilicity},
author = {Yu, Jiachao and Zhou, Yufan and Engelhard, Mark and Zhang, Yuchen and Son, Jiyoung and Liu, Songqin and Zhu, Zihua and Yu, Xiao-Ying},
abstractNote = {In situ molecular imaging of protein films adsorbed on a solid surface in water was realized by using a vacuum compatible microfluidic interface and time-of-flight secondary ion mass spectrometry (ToF-SIMS). Amino acid fragments from such hydrated protein films are observed and identified in the positive ion mode and the results are in agreement with reported works on dry protein films. Moreover, water clusters from the hydrated protein films have been observed and identified in both the positive and negative ion mode for a series protein films. Thus the detailed composition of amino acids and water molecules in the hydrated protein films can be characterized, and the protein water microstructures can be revealed by the distinct three-dimensional spatial distribution reconstructed from in situ liquid ToF-SIMS molecular imaging. Furthermore, spectral principal component analysis of amino acid fragment peaks and water cluster peaks provides unique insights into the water cluster distribution, hydrophilicity, and hydrophobicity of hydrated adsorbed protein films in water.},
doi = {10.1038/s41598-020-60428-1},
journal = {Scientific Reports},
number = [1],
volume = [10],
place = {United States},
year = {2020},
month = {2}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on February 28, 2021
Publisher's Version of Record

Save / Share:

Works referenced in this record:

Biological Water or Rather Water in Biology?
journal, June 2015


Do we underestimate the importance of water in cell biology?
journal, September 2006

  • Chaplin, Martin
  • Nature Reviews Molecular Cell Biology, Vol. 7, Issue 11
  • DOI: 10.1038/nrm2021

Direct observation of hierarchical protein dynamics
journal, April 2015


Biological water at the protein surface: Dynamical solvation probed directly with femtosecond resolution
journal, February 2002

  • Pal, S. K.; Peon, J.; Zewail, A. H.
  • Proceedings of the National Academy of Sciences, Vol. 99, Issue 4
  • DOI: 10.1073/pnas.042697899

Strong reversible Fe3+-mediated bridging between dopa-containing protein films in water
journal, July 2010

  • Zeng, H.; Hwang, D. S.; Israelachvili, J. N.
  • Proceedings of the National Academy of Sciences, Vol. 107, Issue 29
  • DOI: 10.1073/pnas.1007416107

Location of the cell-attachment site in fibronectin with monoclonal antibodies and proteolytic fragments of the molecule
journal, October 1981


Surface Chemistry Influences Implant Biocompatibility
journal, March 2008

  • Tang, Liping; Thevenot, Paul; Hu, Wenjing
  • Current Topics in Medicinal Chemistry, Vol. 8, Issue 4
  • DOI: 10.2174/156802608783790901

Time-of-Flight Secondary Ion Mass Spectrometry Analysis of Conformational Changes in Adsorbed Protein Films
journal, May 2002

  • Xia, Nan; May, Collin J.; McArthur, Sally L.
  • Langmuir, Vol. 18, Issue 10
  • DOI: 10.1021/la020022u

Internal Water and Microsecond Dynamics in Myoglobin
journal, November 2013

  • Kaieda, Shuji; Halle, Bertil
  • The Journal of Physical Chemistry B, Vol. 117, Issue 47
  • DOI: 10.1021/jp409234g

New Insights into the Role of Water in Biological Function: Studying Solvated Biomolecules Using Terahertz Absorption Spectroscopy in Conjunction with Molecular Dynamics Simulations
journal, September 2014

  • Conti Nibali, Valeria; Havenith, Martina
  • Journal of the American Chemical Society, Vol. 136, Issue 37
  • DOI: 10.1021/ja504441h

Improving the Molecular Ion Signal Intensity for In Situ Liquid SIMS Analysis
journal, September 2016

  • Zhou, Yufan; Yao, Juan; Ding, Yuanzhao
  • Journal of The American Society for Mass Spectrometry, Vol. 27, Issue 12
  • DOI: 10.1007/s13361-016-1478-x

An investigation of the beam damage effect on in situ liquid secondary ion mass spectrometry analysis
journal, October 2017

  • Yu, Xiaofei; Yu, Jiachao; Zhou, Yufan
  • Rapid Communications in Mass Spectrometry, Vol. 31, Issue 23
  • DOI: 10.1002/rcm.7983

Mechanism of the SIMS matrix effect
journal, November 1978

  • Deline, V. R.; Katz, William; Evans, C. A.
  • Applied Physics Letters, Vol. 33, Issue 9
  • DOI: 10.1063/1.90546

SIMS quantification in Si, GaAs, and diamond - an update
journal, May 1995


Multivariate Analysis of ToF-SIMS Data from Multicomponent Systems: The Why, When, and How
journal, December 2012


Enhancing Ion Yields in Time-of-Flight-Secondary Ion Mass Spectrometry: A Comparative Study of Argon and Water Cluster Primary Beams
journal, January 2015

  • Sheraz née Rabbani, Sadia; Berrueta Razo, Irma; Kohn, Taylor
  • Analytical Chemistry, Vol. 87, Issue 4
  • DOI: 10.1021/ac504191m

In Situ Characterization of Hydrated Proteins in Water by SALVI and ToF-SIMS
journal, January 2016

  • Yu, Jiachao; Zhou, Yufan; Hua, Xin
  • Journal of Visualized Experiments, Issue 108
  • DOI: 10.3791/53708

Minimizing silicone transfer during micro-contact printing
journal, February 2007


Determination of organic contaminations on Si wafer surfaces by static ToF-SIMS: Improvement of the detection limit with C60+ primary ions
journal, July 2006


Affinity Transformation from Hydrophilicity to Hydrophobicity of Water Molecules on the Basis of Adsorption of Water in Graphitic Nanopores
journal, February 2004

  • Ohba, Tomonori; Kanoh, Hirofumi; Kaneko, Katsumi
  • Journal of the American Chemical Society, Vol. 126, Issue 5
  • DOI: 10.1021/ja038842w

Static time-of-flight secondary ion mass spectrometry and x-ray photoelectron spectroscopy characterization of adsorbed albumin and fibronectin films
journal, January 2001

  • Tidwell, Caren D.; Castner, David G.; Golledge, Stephen L.
  • Surface and Interface Analysis, Vol. 31, Issue 8
  • DOI: 10.1002/sia.1101

Probing albumin adsorption onto calcium phosphates by x-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry
journal, July 2011

  • Baio, J. E.; Weidner, T.; Interlandi, G.
  • Journal of Vacuum Science & Technology B, Nanotechnology and Microelectronics: Materials, Processing, Measurement, and Phenomena, Vol. 29, Issue 4
  • DOI: 10.1116/1.3613919

Making a hybrid microfluidic platform compatible for in situ imaging by vacuum-based techniques
journal, November 2011

  • Yang, Li; Yu, Xiao-Ying; Zhu, Zihua
  • Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 29, Issue 6
  • DOI: 10.1116/1.3654147

Preserving the structure of adsorbed protein films for time-of-flight secondary ion mass spectrometry analysis
journal, September 2003

  • Xia, Nan; Castner, David G.
  • Journal of Biomedical Materials Research, Vol. 67A, Issue 1
  • DOI: 10.1002/jbm.a.10063

Stabilization of dry protein coatings with compatible solutes
journal, December 2018

  • Killian, Manuela S.; Taylor, Adam J.; Castner, David G.
  • Biointerphases, Vol. 13, Issue 6
  • DOI: 10.1116/1.5031189

Two-dimensional and three-dimensional dynamic imaging of live biofilms in a microchannel by time-of-flight secondary ion mass spectrometry
journal, May 2015

  • Hua, Xin; Marshall, Matthew J.; Xiong, Yijia
  • Biomicrofluidics, Vol. 9, Issue 3
  • DOI: 10.1063/1.4919807

The interaction of proteins with solid surfaces
journal, February 2004


ToF-SIMS investigations of adsorbed proteins on dental titanium: ToF-SIMS investigations of adsorbed proteins on dental titanium
journal, March 2010


Improving the interpretation of ToF-SIMS measurements on adsorbed proteins using PCA
journal, January 2006

  • Brüning, C.; Hellweg, S.; Dambach, S.
  • Surface and Interface Analysis, Vol. 38, Issue 4
  • DOI: 10.1002/sia.2233

Classification of adsorbed protein static ToF-SIMS spectra by principal component analysis and neural networks
journal, January 2002

  • Sanni, O. D.; Wagner, M. S.; Briggs, D.
  • Surface and Interface Analysis, Vol. 33, Issue 9
  • DOI: 10.1002/sia.1438

ToF-SIMS Analysis of Adsorbed Proteins: Principal Component Analysis of the Primary Ion Species Effect on the Protein Fragmentation Patterns
journal, November 2011

  • Muramoto, Shin; Graham, Daniel J.; Wagner, Matthew S.
  • The Journal of Physical Chemistry C, Vol. 115, Issue 49
  • DOI: 10.1021/jp208035x

In situ SEM and ToF-SIMS analysis of IgG conjugated gold nanoparticles at aqueous surfaces : In situ SEM and ToF-SIMS analysis of aqueous Au nanoparticles
journal, March 2013

  • Yang, Li; Zhu, Zihua; Yu, Xiao-Ying
  • Surface and Interface Analysis, Vol. 46, Issue 4
  • DOI: 10.1002/sia.5252

Probing the Orientation of Surface-Immobilized Protein G B1 Using ToF-SIMS, Sum Frequency Generation, and NEXAFS Spectroscopy
journal, November 2010

  • Baugh, Loren; Weidner, Tobias; Baio, J. E.
  • Langmuir, Vol. 26, Issue 21
  • DOI: 10.1021/la1007389

Probing the Orientation of Surface-Immobilized Immunoglobulin G by Time-of-Flight Secondary Ion Mass Spectrometry
journal, March 2004

  • Wang, Hua; Castner, David G.; Ratner, Buddy D.
  • Langmuir, Vol. 20, Issue 5
  • DOI: 10.1021/la035376f

Estimating confidence intervals for eigenvalues in exploratory factor analysis
journal, August 2010

  • Larsen, Ross; Warne, Russell T.
  • Behavior Research Methods, Vol. 42, Issue 3
  • DOI: 10.3758/brm.42.3.871