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Title: Multimodal Broadband Vibrational Sum Frequency Generation (MM-BB-V-SFG) Spectrometer and Microscope

Abstract

A broadband sum frequency generation (BB-SFG) spectrometer with multimodal (MM) capabilities was constructed, which could be routinely reconfigured for tabletop experiments in reflection, transmission, and total internal reflection (TIR) geometries, as well as microscopic imaging. The system was constructed using a Ti:sapphire amplifier (800 nm, pulse width = 85 fs, repetition rate = 2 kHz), an optical parameter amplification (OPA) system for production of broadband IR pulses tunable between 1000 and 4000 cm–1, and two Fabry–Pérot etalons arranged in series for production of narrowband 800 nm pulses. The key feature allowing the MM operation was the nearly collinear alignment of the visible (fixed, 800 nm) and infrared (tunable, 1000–4000 cm–1) pulses which were spatially separated. Physical insights discussed in this paper include the comparison of spectral bandwidth produced with 40 and 85 fs pump beams, the improvement of spectral resolution using etalons, the SFG probe volume in bulk analysis, the normalization of SFG signals, the stitching of multiple spectral segments, and the operation in different modes for air/liquid and adsorbate/solid interfaces, bulk samples, as well as spectral imaging combined with principle component analysis (PCA). Finally, the SFG spectral features obtained with the MM-BB-SFG system were compared with those obtained withmore » picosecond-scanning-SFG system and high-resolution BB-SFG system (HR-BB-SFG) for dimethyl sulfoxide, α-pinene, and various samples containing cellulose (purified commercial products, Cladophora cell wall, cotton and flax fibers, and onion epidermis cell wall).« less

Authors:
 [1];  [1];  [1];  [1]
  1. Pennsylvania State Univ., University Park, PA (United States). Materials Research Inst.
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Lignocellulose Structure and Formation (CLSF); Pennsylvania State Univ., University Park, PA (United States
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1387342
Grant/Contract Number:  
SC0001090
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry
Additional Journal Information:
Journal Volume: 120; Journal Issue: 1; Related Information: CLSF partners with Pennsylvania State University (lead); North Carolina State University; University of Rhode Island; Virginia Tech University; Journal ID: ISSN 1520-6106
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
47 OTHER INSTRUMENTATION; biofuels (including algae and biomass); bio-inspired; membrane; carbon sequestration; materials and chemistry by design; synthesis (self-assembly)

Citation Formats

Lee, Christopher M., Kafle, Kabindra, Huang, Shixin, and Kim, Seong H. Multimodal Broadband Vibrational Sum Frequency Generation (MM-BB-V-SFG) Spectrometer and Microscope. United States: N. p., 2015. Web. doi:10.1021/acs.jpcb.5b10290.
Lee, Christopher M., Kafle, Kabindra, Huang, Shixin, & Kim, Seong H. Multimodal Broadband Vibrational Sum Frequency Generation (MM-BB-V-SFG) Spectrometer and Microscope. United States. https://doi.org/10.1021/acs.jpcb.5b10290
Lee, Christopher M., Kafle, Kabindra, Huang, Shixin, and Kim, Seong H. Thu . "Multimodal Broadband Vibrational Sum Frequency Generation (MM-BB-V-SFG) Spectrometer and Microscope". United States. https://doi.org/10.1021/acs.jpcb.5b10290. https://www.osti.gov/servlets/purl/1387342.
@article{osti_1387342,
title = {Multimodal Broadband Vibrational Sum Frequency Generation (MM-BB-V-SFG) Spectrometer and Microscope},
author = {Lee, Christopher M. and Kafle, Kabindra and Huang, Shixin and Kim, Seong H.},
abstractNote = {A broadband sum frequency generation (BB-SFG) spectrometer with multimodal (MM) capabilities was constructed, which could be routinely reconfigured for tabletop experiments in reflection, transmission, and total internal reflection (TIR) geometries, as well as microscopic imaging. The system was constructed using a Ti:sapphire amplifier (800 nm, pulse width = 85 fs, repetition rate = 2 kHz), an optical parameter amplification (OPA) system for production of broadband IR pulses tunable between 1000 and 4000 cm–1, and two Fabry–Pérot etalons arranged in series for production of narrowband 800 nm pulses. The key feature allowing the MM operation was the nearly collinear alignment of the visible (fixed, 800 nm) and infrared (tunable, 1000–4000 cm–1) pulses which were spatially separated. Physical insights discussed in this paper include the comparison of spectral bandwidth produced with 40 and 85 fs pump beams, the improvement of spectral resolution using etalons, the SFG probe volume in bulk analysis, the normalization of SFG signals, the stitching of multiple spectral segments, and the operation in different modes for air/liquid and adsorbate/solid interfaces, bulk samples, as well as spectral imaging combined with principle component analysis (PCA). Finally, the SFG spectral features obtained with the MM-BB-SFG system were compared with those obtained with picosecond-scanning-SFG system and high-resolution BB-SFG system (HR-BB-SFG) for dimethyl sulfoxide, α-pinene, and various samples containing cellulose (purified commercial products, Cladophora cell wall, cotton and flax fibers, and onion epidermis cell wall).},
doi = {10.1021/acs.jpcb.5b10290},
journal = {Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry},
number = 1,
volume = 120,
place = {United States},
year = {Thu Dec 31 00:00:00 EST 2015},
month = {Thu Dec 31 00:00:00 EST 2015}
}

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Works referenced in this record:

Surface properties probed by second-harmonic and sum-frequency generation
journal, February 1989


Quantitative spectral and orientational analysis in surface sum frequency generation vibrational spectroscopy (SFG-VS)
journal, April 2005

  • Wang *, Hong-Fei; Gan † ‡, Wei; Lu † ‡ §, Rong
  • International Reviews in Physical Chemistry, Vol. 24, Issue 2
  • DOI: 10.1080/01442350500225894

Quantitative Sum-Frequency Generation Vibrational Spectroscopy of Molecular Surfaces and Interfaces: Lineshape, Polarization, and Orientation
journal, April 2015


Effect of Nanoscale Geometry on Molecular Conformation:  Vibrational Sum-Frequency Generation of Alkanethiols on Gold Nanoparticles
journal, November 2006

  • Weeraman, Champika; Yatawara, Achani K.; Bordenyuk, Andrey N.
  • Journal of the American Chemical Society, Vol. 128, Issue 44
  • DOI: 10.1021/ja065756y

Absolute Orientation of Molecules at Interfaces
journal, February 2006

  • Rao, Yi; Comstock, Matthew; Eisenthal, Kenneth B.
  • The Journal of Physical Chemistry B, Vol. 110, Issue 4
  • DOI: 10.1021/jp055340r

Carboxylic Acid- and Ester-Functionalized Siloxane Scaffolds on Glass Studied by Broadband Sum Frequency Generation
journal, December 2004

  • Voges, Andrea B.; Al-Abadleh, Hind A.; Musorrafiti, Michael J.
  • The Journal of Physical Chemistry B, Vol. 108, Issue 48
  • DOI: 10.1021/jp046564x

Detection of Buried Microstructures by Nonlinear Light Scattering Spectroscopy
journal, March 2009


Selective Detection of Crystalline Cellulose in Plant Cell Walls with Sum-Frequency-Generation (SFG) Vibration Spectroscopy
journal, July 2011

  • Barnette, Anna L.; Bradley, Laura C.; Veres, Brandon D.
  • Biomacromolecules, Vol. 12, Issue 7
  • DOI: 10.1021/bm200518n

Biomolecular Imaging with Coherent Nonlinear Vibrational Microscopy
journal, April 2013


Vibrationally resolved sum-frequency generation with broad-bandwidth infrared pulses
journal, January 1998

  • Richter, Lee J.; Petralli-Mallow, Teresa P.; Stephenson, John C.
  • Optics Letters, Vol. 23, Issue 20
  • DOI: 10.1364/OL.23.001594

Combining Total Internal Reflection Sum Frequency Spectroscopy Spectral Imaging and Confocal Fluorescence Microscopy
journal, July 2014

  • Allgeyer, Edward S.; Sterling, Sarah M.; Gunewardene, Mudalige S.
  • Langmuir, Vol. 31, Issue 3
  • DOI: 10.1021/la5036932

Femtosecond time-resolved and two-dimensional vibrational sum frequency spectroscopic instrumentation to study structural dynamics at interfaces
journal, January 2008

  • Ghosh, Avishek; Smits, Marc; Bredenbeck, Jens
  • Review of Scientific Instruments, Vol. 79, Issue 9
  • DOI: 10.1063/1.2982058

Broadband Vibrational Sum Frequency Generation Spectroscopy of a Liquid Surface.
journal, January 2001

  • Hommel, Elizabeth L.; Ma, Gang; Alle, Heather C.
  • Analytical Sciences, Vol. 17, Issue 11
  • DOI: 10.2116/analsci.17.1325

Nonresonant Background Suppression in Broadband Vibrational Sum-Frequency Generation Spectroscopy
journal, August 2007

  • Lagutchev, Alexei; Hambir, Selezion A.; Dlott, Dana D.
  • The Journal of Physical Chemistry C, Vol. 111, Issue 37
  • DOI: 10.1021/jp075391j

Compact broadband vibrational sum-frequency generation spectrometer with nonresonant suppression
journal, April 2010

  • Lagutchev, Alexei; Lozano, Aaron; Mukherjee, Prabuddha
  • Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, Vol. 75, Issue 4
  • DOI: 10.1016/j.saa.2009.12.066

Sample cells for probing solid/liquid interfaces with broadband sum-frequency-generation spectroscopy
journal, June 2010

  • Verreault, Dominique; Kurz, Volker; Howell, Caitlin
  • Review of Scientific Instruments, Vol. 81, Issue 6
  • DOI: 10.1063/1.3443096

Generation and application of high power femtosecond pulses in the vibrational fingerprint region
journal, April 2008


Coherent Vibrational Dynamics and High‐resolution Nonlinear Spectroscopy: A Comparison with the Air/DMSO Liquid Interface
journal, December 2013


Ti:sapphire, broadband vibrational sum-frequency generation spectrometer with a counter-propagating geometry
journal, January 2009

  • Ding, Feng; Zhong, Qin; Brindza, Michael R.
  • Optics Express, Vol. 17, Issue 17
  • DOI: 10.1364/OE.17.014665

Accurate determination of complex χ (2) spectrum of the air/water interface
journal, September 2015

  • Adhikari, Aniruddha
  • The Journal of Chemical Physics, Vol. 143, Issue 12
  • DOI: 10.1063/1.4931485

Stabilized phase detection of heterodyne sum frequency generation for interfacial studies
journal, January 2015


Interfacial Processes of a Model Lithium Ion Battery Anode Observed, in Situ, with Vibrational Sum-Frequency Generation Spectroscopy
journal, May 2015

  • Nicolau, Bruno G.; Garcı́a-Rey, Natalia; Dryzhakov, Bogdan
  • The Journal of Physical Chemistry C, Vol. 119, Issue 19
  • DOI: 10.1021/acs.jpcc.5b01290

Real-Time Observation of Molecular Motion on a Surface
journal, December 2005


Frequency- and time-domain femtosecond vibrational sum frequency generation from CO adsorbed on Pt(111)
journal, November 2004

  • Roeterdink, W. G.; Berg, O.; Bonn, M.
  • The Journal of Chemical Physics, Vol. 121, Issue 20
  • DOI: 10.1063/1.1802291

Adding a dimension to the infrared spectra of interfaces using heterodyne detected 2D sum-frequency generation (HD 2D SFG) spectroscopy
journal, December 2011

  • Xiong, W.; Laaser, J. E.; Mehlenbacher, R. D.
  • Proceedings of the National Academy of Sciences, Vol. 108, Issue 52
  • DOI: 10.1073/pnas.1115055108

Vibrational Sum-Frequency Scattering for Detailed Studies of Collagen Fibers in Aqueous Environments
journal, September 2014

  • Johansson, Patrik K.; Koelsch, Patrick
  • Journal of the American Chemical Society, Vol. 136, Issue 39
  • DOI: 10.1021/ja508190d

Theory of optical second-harmonic and sum-frequency scattering from arbitrarily shaped particles
journal, January 2011

  • de Beer, Alex G. F.; Roke, Sylvie; Dadap, Jerry I.
  • Journal of the Optical Society of America B, Vol. 28, Issue 6
  • DOI: 10.1364/JOSAB.28.001374

Nonlinear optical scattering: The concept of effective susceptibility
journal, September 2004


Chiral Sum Frequency Generation for In Situ Probing Proton Exchange in Antiparallel β-Sheets at Interfaces
journal, February 2013

  • Fu, Li; Xiao, Dequan; Wang, Zhuguang
  • Journal of the American Chemical Society, Vol. 135, Issue 9
  • DOI: 10.1021/ja3119527

Biological Macromolecules at Interfaces Probed by Chiral Vibrational Sum Frequency Generation Spectroscopy
journal, January 2014

  • Yan, Elsa C. Y.; Fu, Li; Wang, Zhuguang
  • Chemical Reviews, Vol. 114, Issue 17
  • DOI: 10.1021/cr4006044

Femtosecond time-resolved electronic sum-frequency generation spectroscopy: A new method to investigate ultrafast dynamics at liquid interfaces
journal, March 2008

  • Sekiguchi, Kentaro; Yamaguchi, Shoichi; Tahara, Tahei
  • The Journal of Chemical Physics, Vol. 128, Issue 11
  • DOI: 10.1063/1.2841023

Precise Electronic χ (2) Spectra of Molecules Adsorbed at an Interface Measured by Multiplex Sum Frequency Generation
journal, December 2004

  • Yamaguchi, Shoichi; Tahara, Tahei
  • The Journal of Physical Chemistry B, Vol. 108, Issue 50
  • DOI: 10.1021/jp045306x

Effect of Surface Charge on the Vibrational Dynamics of Interfacial Water
journal, September 2009

  • Eftekhari-Bafrooei, Ali; Borguet, Eric
  • Journal of the American Chemical Society, Vol. 131, Issue 34
  • DOI: 10.1021/ja903340e

Background-Free Fourth-Order Sum Frequency Generation Spectroscopy
journal, May 2015

  • Schleeger, Michael; Grechko, Maksim; Bonn, Mischa
  • The Journal of Physical Chemistry Letters, Vol. 6, Issue 11
  • DOI: 10.1021/acs.jpclett.5b00768

Polarization of water molecules at a charged interface: second harmonic studies of the silica/water interface
journal, April 1992


Vibrational Spectroscopy at Electrified Interfaces
book, July 2013


Random quasi-phase-matching in bulk polycrystalline isotropic nonlinear materials
journal, November 2004

  • Baudrier-Raybaut, M.; Haïdar, R.; Kupecek, Ph.
  • Nature, Vol. 432, Issue 7015
  • DOI: 10.1038/nature03027

Consistency in the Sum Frequency Generation Intensity and Phase Vibrational Spectra of the Air/Neat Water Interface
journal, June 2011

  • Feng, Ran-ran; Guo, Yuan; Lü, Rong
  • The Journal of Physical Chemistry A, Vol. 115, Issue 23
  • DOI: 10.1021/jp110404h

Accurate Line Shapes from Sub-1 cm –1 Resolution Sum Frequency Generation Vibrational Spectroscopy of α-Pinene at Room Temperature
journal, February 2015

  • Mifflin, Amanda L.; Velarde, Luis; Ho, Junming
  • The Journal of Physical Chemistry A, Vol. 119, Issue 8
  • DOI: 10.1021/jp510700z

Angle-tuned etalon filters for optical channel selection in high density wavelength division multiplexed systems
journal, April 1989

  • Frenkel, A.; Lin, C.
  • Journal of Lightwave Technology, Vol. 7, Issue 4
  • DOI: 10.1109/50.19087

Vibrationally resonant sum-frequency generation microscopy with a solid immersion lens
journal, January 2014

  • Lee, Eun Seong; Lee, Sang-Won; Hsu, Julie
  • Biomedical Optics Express, Vol. 5, Issue 7
  • DOI: 10.1364/BOE.5.002125

Sum-Frequency-Generation Vibration Spectroscopy and Density Functional Theory Calculations with Dispersion Corrections (DFT-D2) for Cellulose Iα and Iβ
journal, May 2013

  • Lee, Christopher M.; Mohamed, Naseer M. A.; Watts, Heath D.
  • The Journal of Physical Chemistry B, Vol. 117, Issue 22
  • DOI: 10.1021/jp402998s

Characterization of Starch Polymorphic Structures Using Vibrational Sum Frequency Generation Spectroscopy
journal, February 2014

  • Kong, Lingyan; Lee, Christopher; Kim, Seong H.
  • The Journal of Physical Chemistry B, Vol. 118, Issue 7
  • DOI: 10.1021/jp411130n

Monitoring Meso-Scale Ordering of Cellulose in Intact Plant Cell Walls Using Sum Frequency Generation Spectroscopy
journal, August 2013


Time-Domain SFG Spectroscopy Using Mid-IR Pulse Shaping: Practical and Intrinsic Advantages
journal, March 2011

  • Laaser, Jennifer E.; Xiong, Wei; Zanni, Martin T.
  • The Journal of Physical Chemistry B, Vol. 115, Issue 11
  • DOI: 10.1021/jp200757x

Phase matching considerations in second harmonic generation from tissues: Effects on emission directionality, conversion efficiency and observed morphology
journal, April 2008


Hydrogen-Bonding Network and OH Stretch Vibration of Cellulose: Comparison of Computational Modeling with Polarized IR and SFG Spectra
journal, November 2015

  • Lee, Christopher M.; Kubicki, James D.; Fan, Bingxin
  • The Journal of Physical Chemistry B, Vol. 119, Issue 49
  • DOI: 10.1021/acs.jpcb.5b08015

Mechanism for vibrational relaxation in water investigated by femtosecond infrared spectroscopy
journal, July 1999

  • Nienhuys, Han-Kwang; Woutersen, Sander; van Santen, Rutger A.
  • The Journal of Chemical Physics, Vol. 111, Issue 4
  • DOI: 10.1063/1.479408

Multireflection Sum Frequency Generation Vibrational Spectroscopy
journal, July 2015


Sum Frequency Generation Microscopy Study of Cellulose Fibers
journal, November 2011

  • Hieu, Hoang Chi; Tuan, Nguyen Anh; Li, Hongyan
  • Applied Spectroscopy, Vol. 65, Issue 11
  • DOI: 10.1366/11-06388

Rapid vibrational imaging with sum frequency generation microscopy
journal, January 2011

  • Raghunathan, Varun; Han, Yang; Korth, Olaf
  • Optics Letters, Vol. 36, Issue 19
  • DOI: 10.1364/OL.36.003891

Demonstration of confocal sum frequency microscopy
journal, January 2009

  • Locharoenrat, Kitsakorn; Sano, Haruyuki; Mizutani, Goro
  • physica status solidi (c), Vol. 6, Issue 1
  • DOI: 10.1002/pssc.200879865

Sum Frequency Generation Microscopy of Microcontact-Printed Mixed Self-Assembled Monolayers
journal, February 2006

  • Cimatu, Katherine; Baldelli, Steven
  • The Journal of Physical Chemistry B, Vol. 110, Issue 4
  • DOI: 10.1021/jp0562779

Sum Frequency Generation Imaging Microscopy of CO on Platinum
journal, December 2006

  • Cimatu, Katherine; Baldelli, Steven
  • Journal of the American Chemical Society, Vol. 128, Issue 50
  • DOI: 10.1021/ja067063n

Polarization-Sensitive Sum-Frequency Generation Microscopy of Collagen Fibers
journal, February 2015

  • Han, Yang; Hsu, Julie; Ge, Nien-Hui
  • The Journal of Physical Chemistry B, Vol. 119, Issue 8
  • DOI: 10.1021/jp511058b

Mapping Molecular Orientation with Phase Sensitive Vibrationally Resonant Sum-Frequency Generation Microscopy
journal, May 2013

  • Han, Yang; Raghunathan, Varun; Feng, Ran-ran
  • The Journal of Physical Chemistry B, Vol. 117, Issue 20
  • DOI: 10.1021/jp4022147

Cellulose polymorphs and physical properties of cotton fabrics processed with commercial textile mills for mercerization and liquid ammonia treatments
journal, March 2014

  • Kafle, Kabindra; Greeson, Kenneth; Lee, Christopher
  • Textile Research Journal, Vol. 84, Issue 16
  • DOI: 10.1177/0040517514527379

Works referencing / citing this record:

The Shape of Native Plant Cellulose Microfibrils
journal, September 2018


Flexible pulse shaping for sum frequency microspectroscopies
journal, December 2019

  • Müller, Niklas; Buckup, Tiago; Motzkus, Marcus
  • Journal of the Optical Society of America B, Vol. 37, Issue 1
  • DOI: 10.1364/josab.37.000117

Probing cellulose structures with vibrational spectroscopy
journal, January 2019


Toward an understanding of the increase in enzymatic hydrolysis by mechanical refining
journal, October 2018

  • de Assis, Tiago; Huang, Shixin; Driemeier, Carlos Eduardo
  • Biotechnology for Biofuels, Vol. 11, Issue 1
  • DOI: 10.1186/s13068-018-1289-3

Effects of ball milling on the structure of cotton cellulose
journal, January 2019


Cellulose synthase complexes act in a concerted fashion to synthesize highly aggregated cellulose in secondary cell walls of plants
journal, September 2016

  • Li, Shundai; Bashline, Logan; Zheng, Yunzhen
  • Proceedings of the National Academy of Sciences, Vol. 113, Issue 40
  • DOI: 10.1073/pnas.1613273113

Toward an understanding of the increase in enzymatic hydrolysis by mechanical refining
journal, October 2018

  • de Assis, Tiago; Huang, Shixin; Driemeier, Carlos Eduardo
  • Biotechnology for Biofuels, Vol. 11, Issue 1
  • DOI: 10.1186/s13068-018-1289-3