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Title: Far Infrared Synchrotron Near-Field Nanoimaging and Nanospectroscopy

Abstract

Scattering scanning near-field optical microscopy ($s$-SNOM) has emerged as a powerful imaging and spectroscopic tool for investigating nanoscale heterogeneities in biology, quantum matter, and electronic and photonic devices. However, many materials are defined by a wide range of fundamental molecular and quantum states at far-infrared (FIR) resonant frequencies currently not accessible by $s$-SNOM. Here we show ultrabroadband FIR $s$-SNOM nanoimaging and spectroscopy by combining synchrotron infrared radiation with a novel fast and low-noise copper-doped germanium (Ge:Cu) photoconductive detector. This approach of FIR synchrotron infrared nanospectroscopy (SINS) extends the wavelength range of $s$-SNOM to 31 μm (320 cm-1, 9.7 THz), exceeding conventional limits by an octave to lower energies. We demonstrate this new nanospectroscopic window by measuring elementary excitations of exemplary functional materials, including surface phonon polariton waves and optical phonons in oxides and layered ultrathin van der Waals materials, skeletal and conformational vibrations in molecular systems, and the highly tunable plasmonic response of graphene.

Authors:
ORCiD logo [1];  [2];  [2]; ORCiD logo [3];  [4]
  1. Univ. of Colorado, Boulder, CO (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  3. Univ. of Colorado, Boulder, CO (United States)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1439299
Alternate Identifier(s):
OSTI ID: 1526534
Report Number(s):
BNL-205714-2018-JAAM
Journal ID: ISSN 2330-4022
Grant/Contract Number:  
SC0012704; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
ACS Photonics
Additional Journal Information:
Journal Volume: 5; Journal Issue: 7; Journal ID: ISSN 2330-4022
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; far-infrared; graphene plasmonics; near-field microscopy; s-SNOM; spatiospectral nanoimaging; synchrotron infrared nanospectroscopy; 47 OTHER INSTRUMENTATION

Citation Formats

Khatib, Omar, Bechtel, Hans A., Martin, Michael C., Raschke, Markus B., and Carr, G. Lawrence. Far Infrared Synchrotron Near-Field Nanoimaging and Nanospectroscopy. United States: N. p., 2018. Web. https://doi.org/10.1021/acsphotonics.8b00565.
Khatib, Omar, Bechtel, Hans A., Martin, Michael C., Raschke, Markus B., & Carr, G. Lawrence. Far Infrared Synchrotron Near-Field Nanoimaging and Nanospectroscopy. United States. https://doi.org/10.1021/acsphotonics.8b00565
Khatib, Omar, Bechtel, Hans A., Martin, Michael C., Raschke, Markus B., and Carr, G. Lawrence. Fri . "Far Infrared Synchrotron Near-Field Nanoimaging and Nanospectroscopy". United States. https://doi.org/10.1021/acsphotonics.8b00565. https://www.osti.gov/servlets/purl/1439299.
@article{osti_1439299,
title = {Far Infrared Synchrotron Near-Field Nanoimaging and Nanospectroscopy},
author = {Khatib, Omar and Bechtel, Hans A. and Martin, Michael C. and Raschke, Markus B. and Carr, G. Lawrence},
abstractNote = {Scattering scanning near-field optical microscopy ($s$-SNOM) has emerged as a powerful imaging and spectroscopic tool for investigating nanoscale heterogeneities in biology, quantum matter, and electronic and photonic devices. However, many materials are defined by a wide range of fundamental molecular and quantum states at far-infrared (FIR) resonant frequencies currently not accessible by $s$-SNOM. Here we show ultrabroadband FIR $s$-SNOM nanoimaging and spectroscopy by combining synchrotron infrared radiation with a novel fast and low-noise copper-doped germanium (Ge:Cu) photoconductive detector. This approach of FIR synchrotron infrared nanospectroscopy (SINS) extends the wavelength range of $s$-SNOM to 31 μm (320 cm-1, 9.7 THz), exceeding conventional limits by an octave to lower energies. We demonstrate this new nanospectroscopic window by measuring elementary excitations of exemplary functional materials, including surface phonon polariton waves and optical phonons in oxides and layered ultrathin van der Waals materials, skeletal and conformational vibrations in molecular systems, and the highly tunable plasmonic response of graphene.},
doi = {10.1021/acsphotonics.8b00565},
journal = {ACS Photonics},
number = 7,
volume = 5,
place = {United States},
year = {2018},
month = {5}
}

Journal Article:
Free Publicly Available Full Text
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Cited by: 2 works
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Figures / Tables:

Figure 1 Figure 1: (a) Infrared energy scales and associated phenomena in molecular and quantum matter; (b) Top: ultrabroadband SINS experimental configuration with extension to far-infrared frequencies; bottom: SINS reference spectrum using MCT (black curve) and Ge:Cu (red curve) detectors, demonstrating extended near-field spectroscopic performance at frequencies down to 320 cm−1.

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Works referenced in this record:

Scanning Interferometric Apertureless Microscopy: Optical Imaging at 10 Angstrom Resolution
journal, August 1995


Near-field probing of vibrational absorption for chemical microscopy
journal, May 1999

  • Knoll, B.; Keilmann, F.
  • Nature, Vol. 399, Issue 6732
  • DOI: 10.1038/20154

Performance of visible and mid-infrared scattering-type near-field optical microscopes
journal, June 2003


Nano-optical imaging and spectroscopy of order, phases, and domains in complex solids
journal, December 2012


Infrared vibrational nanocrystallography and nanoimaging
journal, October 2016

  • Muller, Eric A.; Pollard, Benjamin; Bechtel, Hans A.
  • Science Advances, Vol. 2, Issue 10
  • DOI: 10.1126/sciadv.1601006

Vibrational nano-spectroscopic imaging correlating structure with intermolecular coupling and dynamics
journal, April 2014

  • Pollard, Benjamin; Muller, Eric A.; Hinrichs, Karsten
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms4587

High-spatial-resolution mapping of catalytic reactions on single particles
journal, January 2017

  • Wu, Chung-Yeh; Wolf, William J.; Levartovsky, Yehonatan
  • Nature, Vol. 541, Issue 7638
  • DOI: 10.1038/nature20795

Mott Transition in VO2 Revealed by Infrared Spectroscopy and Nano-Imaging
journal, December 2007


Nanotextured phase coexistence in the correlated insulator V2O3
journal, September 2016

  • McLeod, A. S.; van Heumen, E.; Ramirez, J. G.
  • Nature Physics, Vol. 13, Issue 1
  • DOI: 10.1038/nphys3882

Gate-tuning of graphene plasmons revealed by infrared nano-imaging
journal, June 2012


Optical nano-imaging of gate-tunable graphene plasmons
journal, June 2012

  • Chen, Jianing; Badioli, Michela; Alonso-González, Pablo
  • Nature, Vol. 487, Issue 7405
  • DOI: 10.1038/nature11254

Tunable Phonon Polaritons in Atomically Thin van der Waals Crystals of Boron Nitride
journal, March 2014


Polaritons in van der Waals materials
journal, October 2016


A cryogenic scattering-type scanning near-field optical microscope
journal, February 2013

  • Yang, Honghua U.; Hebestreit, Erik; Josberger, Erik E.
  • Review of Scientific Instruments, Vol. 84, Issue 2
  • DOI: 10.1063/1.4789428

Ultrafast Dynamics of Surface Plasmons in InAs by Time-Resolved Infrared Nanospectroscopy
journal, July 2014

  • Wagner, Martin; McLeod, Alexander S.; Maddox, Scott J.
  • Nano Letters, Vol. 14, Issue 8
  • DOI: 10.1021/nl501558t

Ultrafast multi-terahertz nano-spectroscopy with sub-cycle temporal resolution
journal, October 2014


Nanoscale Probing of Dynamics in Local Molecular Environments
journal, October 2015

  • Atkin, Joanna M.; Sass, Paul M.; Teichen, Paul E.
  • The Journal of Physical Chemistry Letters, Vol. 6, Issue 22
  • DOI: 10.1021/acs.jpclett.5b02093

Ultrafast Nanoimaging of the Photoinduced Phase Transition Dynamics in VO 2
journal, April 2016


Atomic-force-microscope-compatible near-field scanning microwave microscope with separated excitation and sensing probes
journal, June 2007

  • Lai, K.; Ji, M. B.; Leindecker, N.
  • Review of Scientific Instruments, Vol. 78, Issue 6
  • DOI: 10.1063/1.2746768

Terahertz Near-Field Nanoscopy of Mobile Carriers in Single Semiconductor Nanodevices
journal, November 2008

  • Huber, A. J.; Keilmann, F.; Wittborn, J.
  • Nano Letters, Vol. 8, Issue 11
  • DOI: 10.1021/nl802086x

Nanoscale electrodynamics of strongly correlated quantum materials
journal, November 2016


Far-Infrared Spectroscopy of Protein Higher-Order Structures
journal, November 2010

  • Falconer, Robert J.; Zakaria, Hidayatul A.; Fan, Yuan Y.
  • Applied Spectroscopy, Vol. 64, Issue 11
  • DOI: 10.1366/000370210793335025

Nano-FTIR Absorption Spectroscopy of Molecular Fingerprints at 20 nm Spatial Resolution
journal, July 2012

  • Huth, Florian; Govyadinov, Alexander; Amarie, Sergiu
  • Nano Letters, Vol. 12, Issue 8
  • DOI: 10.1021/nl301159v

Terahertz Nanoscopy of Plasmonic Resonances with a Quantum Cascade Laser
journal, August 2017


Spectroscopic THz near-field microscope
journal, January 2008

  • von Ribbeck, H. -G.; Brehm, M.; van der Weide, D. W.
  • Optics Express, Vol. 16, Issue 5
  • DOI: 10.1364/OE.16.003430

Quantitative coherent scattering spectra in apertureless terahertz pulse near-field microscopes
journal, July 2012

  • Moon, Kiwon; Do, Youngwoong; Lim, Meehyun
  • Applied Physics Letters, Vol. 101, Issue 1
  • DOI: 10.1063/1.4733475

Dielectric probe for scattering-type terahertz scanning near-field optical microscopy
journal, October 2013

  • Kurihara, T.; Yamaguchi, K.; Watanabe, H.
  • Applied Physics Letters, Vol. 103, Issue 15
  • DOI: 10.1063/1.4824496

Narrow-band near-field nanoscopy in the spectral range from 1.3 to 8.5 THz
journal, March 2016

  • Kuschewski, F.; von Ribbeck, H. -G.; Döring, J.
  • Applied Physics Letters, Vol. 108, Issue 11
  • DOI: 10.1063/1.4943793

Infrared nanoscopy down to liquid helium temperatures
journal, March 2018

  • Lang, Denny; Döring, Jonathan; Nörenberg, Tobias
  • Review of Scientific Instruments, Vol. 89, Issue 3
  • DOI: 10.1063/1.5016281

Ultrabroadband infrared nanospectroscopic imaging
journal, May 2014

  • Bechtel, H. A.; Muller, E. A.; Olmon, R. L.
  • Proceedings of the National Academy of Sciences, Vol. 111, Issue 20
  • DOI: 10.1073/pnas.1400502111

Broadband-infrared assessment of phonon resonance in scattering-type near-field microscopy
journal, January 2011


Optical constants of silica glass from extreme ultraviolet to far infrared at near room temperature
journal, January 2007

  • Kitamura, Rei; Pilon, Laurent; Jonasz, Miroslaw
  • Applied Optics, Vol. 46, Issue 33
  • DOI: 10.1364/AO.46.008118

Infrared dielectric anisotropy and phonon modes of sapphire
journal, March 2000


Phonon and Raman scattering of two-dimensional transition metal dichalcogenides from monolayer, multilayer to bulk material
journal, January 2015

  • Zhang, Xin; Qiao, Xiao-Fen; Shi, Wei
  • Chemical Society Reviews, Vol. 44, Issue 9
  • DOI: 10.1039/C4CS00282B

Theoretical studies of the vibrational properties of the 3,4,9,10,-perylene tetracarboxylic dianhydride (PTCDA) molecule
journal, May 2003


Phase-Resolved Surface Plasmon Interferometry of Graphene
journal, July 2014


Highly confined low-loss plasmons in graphene–boron nitride heterostructures
journal, December 2014

  • Woessner, Achim; Lundeberg, Mark B.; Gao, Yuanda
  • Nature Materials, Vol. 14, Issue 4
  • DOI: 10.1038/nmat4169

Ultrafast optical switching of infrared plasmon polaritons in high-mobility graphene
journal, March 2016


Electrodynamics of correlated electron materials
journal, June 2011

  • Basov, D. N.; Averitt, Richard D.; van der Marel, Dirk
  • Reviews of Modern Physics, Vol. 83, Issue 2
  • DOI: 10.1103/RevModPhys.83.471

Band-like temperature dependence of mobility in a solution-processed organic semiconductor
journal, August 2010

  • Sakanoue, Tomo; Sirringhaus, Henning
  • Nature Materials, Vol. 9, Issue 9
  • DOI: 10.1038/nmat2825

Graphene Plasmonics: Challenges and Opportunities
journal, February 2014


Graphene Plasmonics for Terahertz to Mid-Infrared Applications
journal, January 2014


Naturally hyperbolic
journal, March 2015


A far-infrared Fourier transform spectrometer with an antenna-coupled niobium bolometer
journal, October 2007

  • Santavicca, D. F.; Annunziata, A. J.; Reese, M. O.
  • Superconductor Science and Technology, Vol. 20, Issue 11
  • DOI: 10.1088/0953-2048/20/11/S19

Measuring optical frequencies in the 0–40 THz range with non-synchronized electro–optic sampling
journal, October 2007


    Works referencing / citing this record:

    Near-field infrared spectroscopy of monolayer MnPS 3
    journal, August 2019


    Ultrabroadband infrared near-field spectroscopy and imaging of local resonators in percolative gold films
    journal, January 2019

    • Chen, Xinzhong; Zhang, Jiawei; Yao, Ziheng
    • Journal of the Optical Society of America B, Vol. 36, Issue 12
    • DOI: 10.1364/josab.36.003315

    Comparison of active and passive methods for the infrared scanning near-field microscopy
    journal, April 2019

    • Weng, Qianchun; Panchal, Vishal; Lin, Kuan-Ting
    • Applied Physics Letters, Vol. 114, Issue 15
    • DOI: 10.1063/1.5088056

    Infrared nanospectroscopic imaging in the rotating frame
    journal, January 2019


    Probing Polaritons in 2D Materials with Synchrotron Infrared Nanospectroscopy
    journal, December 2019

    • Barcelos, Ingrid D.; Bechtel, Hans A.; de Matos, Christiano J. S.
    • Advanced Optical Materials, Vol. 8, Issue 5
    • DOI: 10.1002/adom.201901091

    Modern Scattering‐Type Scanning Near‐Field Optical Microscopy for Advanced Material Research
    journal, April 2019


    Nanoimaging and Nanospectroscopy of Polaritons with Time Resolved s ‐SNOM
    journal, September 2019


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