Abstract

Infrared vibrational nano-spectroscopy based on scattering scanning near-field optical microscopy (s-SNOM) provides intrinsic chemical specificity with nanometer spatial resolution. Here we use incoherent infrared radiation from a 1400 K thermal blackbody emitter for broadband infrared (IR) nano-spectroscopy. With optimized interferometric heterodyne signal amplification we achieve few-monolayer sensitivity in phonon polariton spectroscopy and attomolar molecular vibrational spectroscopy. Near-field localization and nanoscale spatial resolution is demonstrated in imaging flakes of hexagonal boron nitride (hBN) and determination of its phonon polariton dispersion relation. The signal-to-noise ratio calculations and analysis for different samples and illumination sources provide a reference for irradiance requirements and the attainable near-field signal levels in s-SNOM in general. The use of a thermal emitter as an IR source thus opens s-SNOM for routine chemical FTIR nano-spectroscopy.

© 2015 Optical Society of America

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2015 (5)

E. A. Muller, B. Pollard, and M. B. Raschke, “Infrared chemical nano-imaging: Accessing structure, coupling, and dynamics on molecular length scales,” J. Phys. Chem. Lett. 6, 1275–1284 (2015).
[Crossref] [PubMed]

Z. Shi, H. A. Bechtel, S. Berweger, Y. Sun, B. Zeng, C. Jin, H. Chang, M. C. Martin, M. B. Raschke, and F. Wang, “Amplitude- and phase-resolved nanospectral imaging of phonon polaritons in hexagonal boron nitride,” ACS Photonics 2, 790–796 (2015).
[Crossref]

S. Mastel, A. A. Govyadinov, T. V. A. G. de Oliveira, I. Amenabar, and R. Hillenbrand, “Nanoscale-resolved chemical identification of thin organic films using infrared near-field spectroscopy and standard fourier transform infrared references,” Appl. Phys. Lett. 106, 023113 (2015).
[Crossref]

S. Dai, Q. Ma, T. Andersen, A. S. Mcleod, Z. Fei, M. K. Liu, M. Wagner, K. Watanabe, T. Taniguchi, M. Thiemens, F. Keilmann, P. Jarillo-Herrero, M. M. Fogler, and D. N. Basov, “Subdiffractional focusing and guiding of polaritonic rays in a natural hyperbolic material,” Nat. Commun. 6, 6963 (2015).
[Crossref] [PubMed]

J. M. Atkin, P. M. Sass, P. E. Teichen, J. D. Eaves, and M. B. Raschke, “Nanoscale probing of dynamics in local molecular environments,” J. Phys. Chem. Lett. 6, 4616–4621 (2015).
[Crossref]

2014 (8)

A. A. Govyadinov, S. Mastel, F. Golmar, A. Chuvilin, P. S. Carney, and R. Hillenbrand, “Recovery of permittivity and depth from near-field data as a step toward infrared nanotomography,” ACS Nano 8, 6911–6921 (2014).
[Crossref] [PubMed]

S. Dai, Z. Fei, Q. Ma, A. S. Rodin, M. Wagner, A. S. McLeod, M. K. Liu, W. Gannett, W. Regan, K. Watanabe, T. Taniguchi, M. Thiemens, G. Dominguez, A. H. C. Neto, A. Zettl, F. Keilmann, P. Jarillo-Herrero, M. M. Fogler, and D. N. Basov, “Tunable phonon polaritons in atomically thin van der waals crystals of boron nitride,” Science 343, 1125–1129 (2014).
[Crossref] [PubMed]

J. D. Caldwell, A. V. Kretinin, Y. Chen, V. Giannini, M. M. Fogler, Y. Francescato, C. T. Ellis, J. G. Tischler, C. R. Woods, A. J. Giles, M. Hong, K. Watanabe, T. Taniguchi, S. A. Maier, and K. S. Novoselov, “Sub-diffractional volume-confined polaritons in the natural hyperbolic material hexagonal boron nitride,” Nat. Commun. 5, 6221 (2014).
[Crossref]

S. Bensmann, F. Gaußmann, M. Lewin, J. Wüppen, S. Nyga, C. Janzen, B. Jungbluth, and T. Taubner, “Near-field imaging and spectroscopy of locally strained GaN using an IR broadband laser,” Opt. Express 22, 22369–22381 (2014).
[Crossref] [PubMed]

H. A. Bechtel, E. A. Muller, R. L. Olmon, M. C. Martin, and M. B. Raschke, “Ultrabroadband infrared nanospectroscopic imaging,” Proc. Nat. Acad. Sci. USA 111, 7191–7196 (2014).
[Crossref] [PubMed]

P. Hermann, A. Hoehl, G. Ulrich, C. Fleischmann, A. Hermelink, B. Kästner, P. Patoka, A. Hornemann, B. Beckhoff, E. Rühl, and G. Ulm, “Characterization of semiconductor materials using synchrotron radiation-based near-field infrared microscopy and nano-FTIR spectroscopy,” Opt. Express 22, 17948–17958 (2014).
[Crossref] [PubMed]

C. Westermeier, A. Cernescu, S. Amarie, C. Liewald, F. Keilmann, and B. Nickel, “Sub-micron phase coexistence in small-molecule organic thin films revealed by infrared nano-imaging,” Nat. Commun. 5, 4101 (2014).
[Crossref] [PubMed]

F. Peragut, J.-B. Brubach, P. Roy, and Y. De Wilde, “Infrared near-field imaging and spectroscopy based on thermal or synchrotron radiation,” Appl. Phys. Lett. 104, 251118 (2014).
[Crossref]

2013 (3)

X. G. Xu and M. B. Raschke, “Near-field infrared vibrational dynamics and tip-enhanced decoherence,” Nano Lett. 13, 1588–1595 (2013). .
[Crossref] [PubMed]

I. Amenabar, S. Poly, W. Nuansing, E. H. Hubrich, A. A. Govyadinov, F. Huth, R. Krutokhvostov, L. Zhang, M. Knez, J. Heberle, A. M. Bittner, and R. Hillenbrand, “Structural analysis and mapping of individual protein complexes by infrared nanospectroscopy,” Nat. Commun. 4, 2890 (2013).
[Crossref] [PubMed]

S. Berweger, D. M. Nguyen, E. A. Muller, H. A. Bechtel, T. T. Perkins, and M. B. Raschke, “Nano-chemical infrared imaging of membrane proteins in lipid bilayers,” J. Am. Chem. Soc. 135, 18292–18295 (2013).
[Crossref] [PubMed]

2012 (6)

J. M. Atkin, S. Berweger, A. C. Jones, and M. B. Raschke, “Nano-optical imaging and spectroscopy of order, phases, and domains in complex solids,” Adv. Phys. 61, 745–842 (2012).
[Crossref]

S. Amarie, P. Zaslansky, Y. Kajihara, E. Griesshaber, W. W. Schmahl, and F. Keilmann, “Nano-FTIR chemical mapping of minerals in biological materials,” Beilstein Journal of Nanotechnology 3, 312–323 (2012).
[Crossref] [PubMed]

F. Huth, A. Govyadinov, S. Amarie, W. Nuansing, F. Keilmann, and R. Hillenbrand, “Nano-FTIR absorption spectroscopy of molecular fingerprints at 20 nm spatial resolution,” Nano Lett. 12, 3973–3978 (2012). .
[Crossref] [PubMed]

A. Jones and M. B. Raschke, “Thermal infrared near-field spectroscopy,” Nano Letters 12, 1475–1481 (2012).
[Crossref] [PubMed]

M. Ishikawa, M. Katsura, S. Nakashima, Y. Ikemoto, and H. Okamura, “Broadband near-field mid-infrared spectroscopy and application to phonon resonances in quartz,” Opt. Express 20, 11064–11072 (2012).
[Crossref] [PubMed]

R. L. Olmon and M. B. Raschke, “Antenna-load interactions at optical frequencies: impedance matching to quantum systems,” Nanotechnology 23, 444001 (2012).
[Crossref] [PubMed]

2011 (3)

S. Amarie and F. Keilmann, “Broadband-infrared assessment of phonon resonance in scattering-type near-field microscopy,” Phys. Rev. B 83, 045404 (2011).
[Crossref]

Y. Kajihara, K. Kosaka, and S. Komiyama, “Thermally excited near-field radiation and far-field interference,” Opt. Express 19, 7695–7704 (2011).
[Crossref] [PubMed]

F. Huth, M. Schnell, J. Wittborn, N. Ocelic, and R. Hillenbrand, “Infrared-spectroscopic nanoimaging with a thermal source,” Nat. Mater. 10, 352–356 (2011).
[Crossref] [PubMed]

2006 (1)

Y. D. Wilde, F. Formanek, R. Carminati, B. Gralek, P. Lemoine, K. Joulain, J. Mulet, Y. Chen, and J. Greffet, “Thermal radiation scanning tunneling microscopy,” Nature 444, 740–743 (2006).
[Crossref] [PubMed]

2005 (1)

E. H. Korte and A. Röseler, “Infrared reststrahlen revisited: commonly disregarded optical details related to n<1,” Analytical and Bioanalytical Chemistry 382, 1987–1992 (2005).
[Crossref]

2004 (1)

F. Keilmann and R. Hillenbrand, “Near-field microscopy by elastic light scattering from a tip,” Philos. T. Roy. Soc. A 362, 787–805 (2004).
[Crossref]

2000 (2)

B. Knoll and F. Keilmann, “Enhanced dielectric contrast in scattering-type scanning near-field optical microscopy,” Opt. Commun. 182, 321–328 (2000).
[Crossref]

M. K. Gunde, “Vibrational modes in amorphous silicon dioxide,” Physica B: Condensed Matter 292, 286–295 (2000).
[Crossref]

1999 (1)

B. Knoll and F. Keilmann, “Near-field probing of vibrational absorption for chemical microscopy,” Nature 399, 134–137 (1999).
[Crossref]

1973 (1)

G. Masetti, F. Cabassi, G. Morelli, and G. Zerbi, “Conformational order and disorder in poly(tetrafluoroethylene) from the infrared spectrum,” Macromolecules 6, 700–707 (1973).
[Crossref]

1966 (1)

R. Geick, C. H. Perry, and G. Rupprecht, “Normal modes in hexagonal boron nitride,” Phys. Rev. 146, 543–547 (1966).
[Crossref]

1956 (1)

C. Y. Liang and S. Krimm, “Infrared spectra of high polymers. iii. polytetrafluoroethylene and polychlorotrifluoroethylene,” The Journal of Chemical Physics 25, 563–571 (1956).
[Crossref]

Amarie, S.

C. Westermeier, A. Cernescu, S. Amarie, C. Liewald, F. Keilmann, and B. Nickel, “Sub-micron phase coexistence in small-molecule organic thin films revealed by infrared nano-imaging,” Nat. Commun. 5, 4101 (2014).
[Crossref] [PubMed]

S. Amarie, P. Zaslansky, Y. Kajihara, E. Griesshaber, W. W. Schmahl, and F. Keilmann, “Nano-FTIR chemical mapping of minerals in biological materials,” Beilstein Journal of Nanotechnology 3, 312–323 (2012).
[Crossref] [PubMed]

F. Huth, A. Govyadinov, S. Amarie, W. Nuansing, F. Keilmann, and R. Hillenbrand, “Nano-FTIR absorption spectroscopy of molecular fingerprints at 20 nm spatial resolution,” Nano Lett. 12, 3973–3978 (2012). .
[Crossref] [PubMed]

S. Amarie and F. Keilmann, “Broadband-infrared assessment of phonon resonance in scattering-type near-field microscopy,” Phys. Rev. B 83, 045404 (2011).
[Crossref]

Amenabar, I.

S. Mastel, A. A. Govyadinov, T. V. A. G. de Oliveira, I. Amenabar, and R. Hillenbrand, “Nanoscale-resolved chemical identification of thin organic films using infrared near-field spectroscopy and standard fourier transform infrared references,” Appl. Phys. Lett. 106, 023113 (2015).
[Crossref]

I. Amenabar, S. Poly, W. Nuansing, E. H. Hubrich, A. A. Govyadinov, F. Huth, R. Krutokhvostov, L. Zhang, M. Knez, J. Heberle, A. M. Bittner, and R. Hillenbrand, “Structural analysis and mapping of individual protein complexes by infrared nanospectroscopy,” Nat. Commun. 4, 2890 (2013).
[Crossref] [PubMed]

Andersen, T.

S. Dai, Q. Ma, T. Andersen, A. S. Mcleod, Z. Fei, M. K. Liu, M. Wagner, K. Watanabe, T. Taniguchi, M. Thiemens, F. Keilmann, P. Jarillo-Herrero, M. M. Fogler, and D. N. Basov, “Subdiffractional focusing and guiding of polaritonic rays in a natural hyperbolic material,” Nat. Commun. 6, 6963 (2015).
[Crossref] [PubMed]

Atkin, J. M.

J. M. Atkin, P. M. Sass, P. E. Teichen, J. D. Eaves, and M. B. Raschke, “Nanoscale probing of dynamics in local molecular environments,” J. Phys. Chem. Lett. 6, 4616–4621 (2015).
[Crossref]

J. M. Atkin, S. Berweger, A. C. Jones, and M. B. Raschke, “Nano-optical imaging and spectroscopy of order, phases, and domains in complex solids,” Adv. Phys. 61, 745–842 (2012).
[Crossref]

Basov, D. N.

S. Dai, Q. Ma, T. Andersen, A. S. Mcleod, Z. Fei, M. K. Liu, M. Wagner, K. Watanabe, T. Taniguchi, M. Thiemens, F. Keilmann, P. Jarillo-Herrero, M. M. Fogler, and D. N. Basov, “Subdiffractional focusing and guiding of polaritonic rays in a natural hyperbolic material,” Nat. Commun. 6, 6963 (2015).
[Crossref] [PubMed]

S. Dai, Z. Fei, Q. Ma, A. S. Rodin, M. Wagner, A. S. McLeod, M. K. Liu, W. Gannett, W. Regan, K. Watanabe, T. Taniguchi, M. Thiemens, G. Dominguez, A. H. C. Neto, A. Zettl, F. Keilmann, P. Jarillo-Herrero, M. M. Fogler, and D. N. Basov, “Tunable phonon polaritons in atomically thin van der waals crystals of boron nitride,” Science 343, 1125–1129 (2014).
[Crossref] [PubMed]

Bechtel, H. A.

Z. Shi, H. A. Bechtel, S. Berweger, Y. Sun, B. Zeng, C. Jin, H. Chang, M. C. Martin, M. B. Raschke, and F. Wang, “Amplitude- and phase-resolved nanospectral imaging of phonon polaritons in hexagonal boron nitride,” ACS Photonics 2, 790–796 (2015).
[Crossref]

H. A. Bechtel, E. A. Muller, R. L. Olmon, M. C. Martin, and M. B. Raschke, “Ultrabroadband infrared nanospectroscopic imaging,” Proc. Nat. Acad. Sci. USA 111, 7191–7196 (2014).
[Crossref] [PubMed]

S. Berweger, D. M. Nguyen, E. A. Muller, H. A. Bechtel, T. T. Perkins, and M. B. Raschke, “Nano-chemical infrared imaging of membrane proteins in lipid bilayers,” J. Am. Chem. Soc. 135, 18292–18295 (2013).
[Crossref] [PubMed]

Beckhoff, B.

Bensmann, S.

Berweger, S.

Z. Shi, H. A. Bechtel, S. Berweger, Y. Sun, B. Zeng, C. Jin, H. Chang, M. C. Martin, M. B. Raschke, and F. Wang, “Amplitude- and phase-resolved nanospectral imaging of phonon polaritons in hexagonal boron nitride,” ACS Photonics 2, 790–796 (2015).
[Crossref]

S. Berweger, D. M. Nguyen, E. A. Muller, H. A. Bechtel, T. T. Perkins, and M. B. Raschke, “Nano-chemical infrared imaging of membrane proteins in lipid bilayers,” J. Am. Chem. Soc. 135, 18292–18295 (2013).
[Crossref] [PubMed]

J. M. Atkin, S. Berweger, A. C. Jones, and M. B. Raschke, “Nano-optical imaging and spectroscopy of order, phases, and domains in complex solids,” Adv. Phys. 61, 745–842 (2012).
[Crossref]

Bittner, A. M.

I. Amenabar, S. Poly, W. Nuansing, E. H. Hubrich, A. A. Govyadinov, F. Huth, R. Krutokhvostov, L. Zhang, M. Knez, J. Heberle, A. M. Bittner, and R. Hillenbrand, “Structural analysis and mapping of individual protein complexes by infrared nanospectroscopy,” Nat. Commun. 4, 2890 (2013).
[Crossref] [PubMed]

Brubach, J.-B.

F. Peragut, J.-B. Brubach, P. Roy, and Y. De Wilde, “Infrared near-field imaging and spectroscopy based on thermal or synchrotron radiation,” Appl. Phys. Lett. 104, 251118 (2014).
[Crossref]

Cabassi, F.

G. Masetti, F. Cabassi, G. Morelli, and G. Zerbi, “Conformational order and disorder in poly(tetrafluoroethylene) from the infrared spectrum,” Macromolecules 6, 700–707 (1973).
[Crossref]

Caldwell, J. D.

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Neto, A. H. C.

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Olmon, R. L.

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R. L. Olmon and M. B. Raschke, “Antenna-load interactions at optical frequencies: impedance matching to quantum systems,” Nanotechnology 23, 444001 (2012).
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E. A. Muller, B. Pollard, and M. B. Raschke, “Infrared chemical nano-imaging: Accessing structure, coupling, and dynamics on molecular length scales,” J. Phys. Chem. Lett. 6, 1275–1284 (2015).
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E. A. Muller, B. Pollard, and M. B. Raschke, “Infrared chemical nano-imaging: Accessing structure, coupling, and dynamics on molecular length scales,” J. Phys. Chem. Lett. 6, 1275–1284 (2015).
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J. M. Atkin, P. M. Sass, P. E. Teichen, J. D. Eaves, and M. B. Raschke, “Nanoscale probing of dynamics in local molecular environments,” J. Phys. Chem. Lett. 6, 4616–4621 (2015).
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S. Berweger, D. M. Nguyen, E. A. Muller, H. A. Bechtel, T. T. Perkins, and M. B. Raschke, “Nano-chemical infrared imaging of membrane proteins in lipid bilayers,” J. Am. Chem. Soc. 135, 18292–18295 (2013).
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X. G. Xu and M. B. Raschke, “Near-field infrared vibrational dynamics and tip-enhanced decoherence,” Nano Lett. 13, 1588–1595 (2013). .
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R. L. Olmon and M. B. Raschke, “Antenna-load interactions at optical frequencies: impedance matching to quantum systems,” Nanotechnology 23, 444001 (2012).
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B. Pollard, E. A. Muller, K. Hinrichs, and M. B. Raschke, “Vibrational nano-spectroscopic imaging correlating structure with intermolecular coupling and dynamics,” Nat. Commun.5 (2014).
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S. Dai, Z. Fei, Q. Ma, A. S. Rodin, M. Wagner, A. S. McLeod, M. K. Liu, W. Gannett, W. Regan, K. Watanabe, T. Taniguchi, M. Thiemens, G. Dominguez, A. H. C. Neto, A. Zettl, F. Keilmann, P. Jarillo-Herrero, M. M. Fogler, and D. N. Basov, “Tunable phonon polaritons in atomically thin van der waals crystals of boron nitride,” Science 343, 1125–1129 (2014).
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S. Dai, Z. Fei, Q. Ma, A. S. Rodin, M. Wagner, A. S. McLeod, M. K. Liu, W. Gannett, W. Regan, K. Watanabe, T. Taniguchi, M. Thiemens, G. Dominguez, A. H. C. Neto, A. Zettl, F. Keilmann, P. Jarillo-Herrero, M. M. Fogler, and D. N. Basov, “Tunable phonon polaritons in atomically thin van der waals crystals of boron nitride,” Science 343, 1125–1129 (2014).
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F. Peragut, J.-B. Brubach, P. Roy, and Y. De Wilde, “Infrared near-field imaging and spectroscopy based on thermal or synchrotron radiation,” Appl. Phys. Lett. 104, 251118 (2014).
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Rupprecht, G.

R. Geick, C. H. Perry, and G. Rupprecht, “Normal modes in hexagonal boron nitride,” Phys. Rev. 146, 543–547 (1966).
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J. M. Atkin, P. M. Sass, P. E. Teichen, J. D. Eaves, and M. B. Raschke, “Nanoscale probing of dynamics in local molecular environments,” J. Phys. Chem. Lett. 6, 4616–4621 (2015).
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S. Amarie, P. Zaslansky, Y. Kajihara, E. Griesshaber, W. W. Schmahl, and F. Keilmann, “Nano-FTIR chemical mapping of minerals in biological materials,” Beilstein Journal of Nanotechnology 3, 312–323 (2012).
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F. Huth, M. Schnell, J. Wittborn, N. Ocelic, and R. Hillenbrand, “Infrared-spectroscopic nanoimaging with a thermal source,” Nat. Mater. 10, 352–356 (2011).
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Z. Shi, H. A. Bechtel, S. Berweger, Y. Sun, B. Zeng, C. Jin, H. Chang, M. C. Martin, M. B. Raschke, and F. Wang, “Amplitude- and phase-resolved nanospectral imaging of phonon polaritons in hexagonal boron nitride,” ACS Photonics 2, 790–796 (2015).
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Z. Shi, H. A. Bechtel, S. Berweger, Y. Sun, B. Zeng, C. Jin, H. Chang, M. C. Martin, M. B. Raschke, and F. Wang, “Amplitude- and phase-resolved nanospectral imaging of phonon polaritons in hexagonal boron nitride,” ACS Photonics 2, 790–796 (2015).
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S. Dai, Z. Fei, Q. Ma, A. S. Rodin, M. Wagner, A. S. McLeod, M. K. Liu, W. Gannett, W. Regan, K. Watanabe, T. Taniguchi, M. Thiemens, G. Dominguez, A. H. C. Neto, A. Zettl, F. Keilmann, P. Jarillo-Herrero, M. M. Fogler, and D. N. Basov, “Tunable phonon polaritons in atomically thin van der waals crystals of boron nitride,” Science 343, 1125–1129 (2014).
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Teichen, P. E.

J. M. Atkin, P. M. Sass, P. E. Teichen, J. D. Eaves, and M. B. Raschke, “Nanoscale probing of dynamics in local molecular environments,” J. Phys. Chem. Lett. 6, 4616–4621 (2015).
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S. Dai, Q. Ma, T. Andersen, A. S. Mcleod, Z. Fei, M. K. Liu, M. Wagner, K. Watanabe, T. Taniguchi, M. Thiemens, F. Keilmann, P. Jarillo-Herrero, M. M. Fogler, and D. N. Basov, “Subdiffractional focusing and guiding of polaritonic rays in a natural hyperbolic material,” Nat. Commun. 6, 6963 (2015).
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S. Dai, Z. Fei, Q. Ma, A. S. Rodin, M. Wagner, A. S. McLeod, M. K. Liu, W. Gannett, W. Regan, K. Watanabe, T. Taniguchi, M. Thiemens, G. Dominguez, A. H. C. Neto, A. Zettl, F. Keilmann, P. Jarillo-Herrero, M. M. Fogler, and D. N. Basov, “Tunable phonon polaritons in atomically thin van der waals crystals of boron nitride,” Science 343, 1125–1129 (2014).
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J. D. Caldwell, A. V. Kretinin, Y. Chen, V. Giannini, M. M. Fogler, Y. Francescato, C. T. Ellis, J. G. Tischler, C. R. Woods, A. J. Giles, M. Hong, K. Watanabe, T. Taniguchi, S. A. Maier, and K. S. Novoselov, “Sub-diffractional volume-confined polaritons in the natural hyperbolic material hexagonal boron nitride,” Nat. Commun. 5, 6221 (2014).
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Ulrich, G.

Wagner, M.

S. Dai, Q. Ma, T. Andersen, A. S. Mcleod, Z. Fei, M. K. Liu, M. Wagner, K. Watanabe, T. Taniguchi, M. Thiemens, F. Keilmann, P. Jarillo-Herrero, M. M. Fogler, and D. N. Basov, “Subdiffractional focusing and guiding of polaritonic rays in a natural hyperbolic material,” Nat. Commun. 6, 6963 (2015).
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S. Dai, Z. Fei, Q. Ma, A. S. Rodin, M. Wagner, A. S. McLeod, M. K. Liu, W. Gannett, W. Regan, K. Watanabe, T. Taniguchi, M. Thiemens, G. Dominguez, A. H. C. Neto, A. Zettl, F. Keilmann, P. Jarillo-Herrero, M. M. Fogler, and D. N. Basov, “Tunable phonon polaritons in atomically thin van der waals crystals of boron nitride,” Science 343, 1125–1129 (2014).
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Wang, F.

Z. Shi, H. A. Bechtel, S. Berweger, Y. Sun, B. Zeng, C. Jin, H. Chang, M. C. Martin, M. B. Raschke, and F. Wang, “Amplitude- and phase-resolved nanospectral imaging of phonon polaritons in hexagonal boron nitride,” ACS Photonics 2, 790–796 (2015).
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S. Dai, Q. Ma, T. Andersen, A. S. Mcleod, Z. Fei, M. K. Liu, M. Wagner, K. Watanabe, T. Taniguchi, M. Thiemens, F. Keilmann, P. Jarillo-Herrero, M. M. Fogler, and D. N. Basov, “Subdiffractional focusing and guiding of polaritonic rays in a natural hyperbolic material,” Nat. Commun. 6, 6963 (2015).
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S. Dai, Z. Fei, Q. Ma, A. S. Rodin, M. Wagner, A. S. McLeod, M. K. Liu, W. Gannett, W. Regan, K. Watanabe, T. Taniguchi, M. Thiemens, G. Dominguez, A. H. C. Neto, A. Zettl, F. Keilmann, P. Jarillo-Herrero, M. M. Fogler, and D. N. Basov, “Tunable phonon polaritons in atomically thin van der waals crystals of boron nitride,” Science 343, 1125–1129 (2014).
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C. Westermeier, A. Cernescu, S. Amarie, C. Liewald, F. Keilmann, and B. Nickel, “Sub-micron phase coexistence in small-molecule organic thin films revealed by infrared nano-imaging,” Nat. Commun. 5, 4101 (2014).
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F. Huth, M. Schnell, J. Wittborn, N. Ocelic, and R. Hillenbrand, “Infrared-spectroscopic nanoimaging with a thermal source,” Nat. Mater. 10, 352–356 (2011).
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J. D. Caldwell, A. V. Kretinin, Y. Chen, V. Giannini, M. M. Fogler, Y. Francescato, C. T. Ellis, J. G. Tischler, C. R. Woods, A. J. Giles, M. Hong, K. Watanabe, T. Taniguchi, S. A. Maier, and K. S. Novoselov, “Sub-diffractional volume-confined polaritons in the natural hyperbolic material hexagonal boron nitride,” Nat. Commun. 5, 6221 (2014).
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Xu, X. G.

X. G. Xu and M. B. Raschke, “Near-field infrared vibrational dynamics and tip-enhanced decoherence,” Nano Lett. 13, 1588–1595 (2013). .
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S. Amarie, P. Zaslansky, Y. Kajihara, E. Griesshaber, W. W. Schmahl, and F. Keilmann, “Nano-FTIR chemical mapping of minerals in biological materials,” Beilstein Journal of Nanotechnology 3, 312–323 (2012).
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Z. Shi, H. A. Bechtel, S. Berweger, Y. Sun, B. Zeng, C. Jin, H. Chang, M. C. Martin, M. B. Raschke, and F. Wang, “Amplitude- and phase-resolved nanospectral imaging of phonon polaritons in hexagonal boron nitride,” ACS Photonics 2, 790–796 (2015).
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G. Masetti, F. Cabassi, G. Morelli, and G. Zerbi, “Conformational order and disorder in poly(tetrafluoroethylene) from the infrared spectrum,” Macromolecules 6, 700–707 (1973).
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S. Dai, Z. Fei, Q. Ma, A. S. Rodin, M. Wagner, A. S. McLeod, M. K. Liu, W. Gannett, W. Regan, K. Watanabe, T. Taniguchi, M. Thiemens, G. Dominguez, A. H. C. Neto, A. Zettl, F. Keilmann, P. Jarillo-Herrero, M. M. Fogler, and D. N. Basov, “Tunable phonon polaritons in atomically thin van der waals crystals of boron nitride,” Science 343, 1125–1129 (2014).
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Zhang, L.

I. Amenabar, S. Poly, W. Nuansing, E. H. Hubrich, A. A. Govyadinov, F. Huth, R. Krutokhvostov, L. Zhang, M. Knez, J. Heberle, A. M. Bittner, and R. Hillenbrand, “Structural analysis and mapping of individual protein complexes by infrared nanospectroscopy,” Nat. Commun. 4, 2890 (2013).
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ACS Nano (1)

A. A. Govyadinov, S. Mastel, F. Golmar, A. Chuvilin, P. S. Carney, and R. Hillenbrand, “Recovery of permittivity and depth from near-field data as a step toward infrared nanotomography,” ACS Nano 8, 6911–6921 (2014).
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ACS Photonics (1)

Z. Shi, H. A. Bechtel, S. Berweger, Y. Sun, B. Zeng, C. Jin, H. Chang, M. C. Martin, M. B. Raschke, and F. Wang, “Amplitude- and phase-resolved nanospectral imaging of phonon polaritons in hexagonal boron nitride,” ACS Photonics 2, 790–796 (2015).
[Crossref]

Adv. Phys. (1)

J. M. Atkin, S. Berweger, A. C. Jones, and M. B. Raschke, “Nano-optical imaging and spectroscopy of order, phases, and domains in complex solids,” Adv. Phys. 61, 745–842 (2012).
[Crossref]

Analytical and Bioanalytical Chemistry (1)

E. H. Korte and A. Röseler, “Infrared reststrahlen revisited: commonly disregarded optical details related to n<1,” Analytical and Bioanalytical Chemistry 382, 1987–1992 (2005).
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Appl. Phys. Lett. (2)

S. Mastel, A. A. Govyadinov, T. V. A. G. de Oliveira, I. Amenabar, and R. Hillenbrand, “Nanoscale-resolved chemical identification of thin organic films using infrared near-field spectroscopy and standard fourier transform infrared references,” Appl. Phys. Lett. 106, 023113 (2015).
[Crossref]

F. Peragut, J.-B. Brubach, P. Roy, and Y. De Wilde, “Infrared near-field imaging and spectroscopy based on thermal or synchrotron radiation,” Appl. Phys. Lett. 104, 251118 (2014).
[Crossref]

Beilstein Journal of Nanotechnology (1)

S. Amarie, P. Zaslansky, Y. Kajihara, E. Griesshaber, W. W. Schmahl, and F. Keilmann, “Nano-FTIR chemical mapping of minerals in biological materials,” Beilstein Journal of Nanotechnology 3, 312–323 (2012).
[Crossref] [PubMed]

J. Am. Chem. Soc. (1)

S. Berweger, D. M. Nguyen, E. A. Muller, H. A. Bechtel, T. T. Perkins, and M. B. Raschke, “Nano-chemical infrared imaging of membrane proteins in lipid bilayers,” J. Am. Chem. Soc. 135, 18292–18295 (2013).
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J. Phys. Chem. Lett. (2)

E. A. Muller, B. Pollard, and M. B. Raschke, “Infrared chemical nano-imaging: Accessing structure, coupling, and dynamics on molecular length scales,” J. Phys. Chem. Lett. 6, 1275–1284 (2015).
[Crossref] [PubMed]

J. M. Atkin, P. M. Sass, P. E. Teichen, J. D. Eaves, and M. B. Raschke, “Nanoscale probing of dynamics in local molecular environments,” J. Phys. Chem. Lett. 6, 4616–4621 (2015).
[Crossref]

Macromolecules (1)

G. Masetti, F. Cabassi, G. Morelli, and G. Zerbi, “Conformational order and disorder in poly(tetrafluoroethylene) from the infrared spectrum,” Macromolecules 6, 700–707 (1973).
[Crossref]

Nano Lett. (2)

F. Huth, A. Govyadinov, S. Amarie, W. Nuansing, F. Keilmann, and R. Hillenbrand, “Nano-FTIR absorption spectroscopy of molecular fingerprints at 20 nm spatial resolution,” Nano Lett. 12, 3973–3978 (2012). .
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X. G. Xu and M. B. Raschke, “Near-field infrared vibrational dynamics and tip-enhanced decoherence,” Nano Lett. 13, 1588–1595 (2013). .
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Nano Letters (1)

A. Jones and M. B. Raschke, “Thermal infrared near-field spectroscopy,” Nano Letters 12, 1475–1481 (2012).
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Nanotechnology (1)

R. L. Olmon and M. B. Raschke, “Antenna-load interactions at optical frequencies: impedance matching to quantum systems,” Nanotechnology 23, 444001 (2012).
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Nat. Commun. (4)

J. D. Caldwell, A. V. Kretinin, Y. Chen, V. Giannini, M. M. Fogler, Y. Francescato, C. T. Ellis, J. G. Tischler, C. R. Woods, A. J. Giles, M. Hong, K. Watanabe, T. Taniguchi, S. A. Maier, and K. S. Novoselov, “Sub-diffractional volume-confined polaritons in the natural hyperbolic material hexagonal boron nitride,” Nat. Commun. 5, 6221 (2014).
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I. Amenabar, S. Poly, W. Nuansing, E. H. Hubrich, A. A. Govyadinov, F. Huth, R. Krutokhvostov, L. Zhang, M. Knez, J. Heberle, A. M. Bittner, and R. Hillenbrand, “Structural analysis and mapping of individual protein complexes by infrared nanospectroscopy,” Nat. Commun. 4, 2890 (2013).
[Crossref] [PubMed]

C. Westermeier, A. Cernescu, S. Amarie, C. Liewald, F. Keilmann, and B. Nickel, “Sub-micron phase coexistence in small-molecule organic thin films revealed by infrared nano-imaging,” Nat. Commun. 5, 4101 (2014).
[Crossref] [PubMed]

S. Dai, Q. Ma, T. Andersen, A. S. Mcleod, Z. Fei, M. K. Liu, M. Wagner, K. Watanabe, T. Taniguchi, M. Thiemens, F. Keilmann, P. Jarillo-Herrero, M. M. Fogler, and D. N. Basov, “Subdiffractional focusing and guiding of polaritonic rays in a natural hyperbolic material,” Nat. Commun. 6, 6963 (2015).
[Crossref] [PubMed]

Nat. Mater. (1)

F. Huth, M. Schnell, J. Wittborn, N. Ocelic, and R. Hillenbrand, “Infrared-spectroscopic nanoimaging with a thermal source,” Nat. Mater. 10, 352–356 (2011).
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Nature (2)

B. Knoll and F. Keilmann, “Near-field probing of vibrational absorption for chemical microscopy,” Nature 399, 134–137 (1999).
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Y. D. Wilde, F. Formanek, R. Carminati, B. Gralek, P. Lemoine, K. Joulain, J. Mulet, Y. Chen, and J. Greffet, “Thermal radiation scanning tunneling microscopy,” Nature 444, 740–743 (2006).
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Opt. Commun. (1)

B. Knoll and F. Keilmann, “Enhanced dielectric contrast in scattering-type scanning near-field optical microscopy,” Opt. Commun. 182, 321–328 (2000).
[Crossref]

Opt. Express (4)

Philos. T. Roy. Soc. A (1)

F. Keilmann and R. Hillenbrand, “Near-field microscopy by elastic light scattering from a tip,” Philos. T. Roy. Soc. A 362, 787–805 (2004).
[Crossref]

Phys. Rev. (1)

R. Geick, C. H. Perry, and G. Rupprecht, “Normal modes in hexagonal boron nitride,” Phys. Rev. 146, 543–547 (1966).
[Crossref]

Phys. Rev. B (1)

S. Amarie and F. Keilmann, “Broadband-infrared assessment of phonon resonance in scattering-type near-field microscopy,” Phys. Rev. B 83, 045404 (2011).
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Physica B: Condensed Matter (1)

M. K. Gunde, “Vibrational modes in amorphous silicon dioxide,” Physica B: Condensed Matter 292, 286–295 (2000).
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Proc. Nat. Acad. Sci. USA (1)

H. A. Bechtel, E. A. Muller, R. L. Olmon, M. C. Martin, and M. B. Raschke, “Ultrabroadband infrared nanospectroscopic imaging,” Proc. Nat. Acad. Sci. USA 111, 7191–7196 (2014).
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Science (1)

S. Dai, Z. Fei, Q. Ma, A. S. Rodin, M. Wagner, A. S. McLeod, M. K. Liu, W. Gannett, W. Regan, K. Watanabe, T. Taniguchi, M. Thiemens, G. Dominguez, A. H. C. Neto, A. Zettl, F. Keilmann, P. Jarillo-Herrero, M. M. Fogler, and D. N. Basov, “Tunable phonon polaritons in atomically thin van der waals crystals of boron nitride,” Science 343, 1125–1129 (2014).
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L. Mandel and E. Wolf, Optical Coherence and Quantum Optics (Cambridge University, 1995) (Chap. 13).
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B. Pollard, E. A. Muller, K. Hinrichs, and M. B. Raschke, “Vibrational nano-spectroscopic imaging correlating structure with intermolecular coupling and dynamics,” Nat. Commun.5 (2014).
[Crossref]

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Figures (8)

Fig. 1
Fig. 1 (a) Schematic of infrared nano-spectroscopy using broadband infrared thermal radiation from a ceramic globar, utilizing heterodyne detection by asymmetric Michelson interferometry with beamsplitter (BS), compensation plate (CP) and mercury-cadmium-telluride (MCT) detector. (b) Reference interferogram of blackbody source. (c) Corresponding broadband Fourier transform of (b).
Fig. 2
Fig. 2 Thermal source asymmetric s-SNOM interferograms of hexagonal boron nitride flake on SiO2 (hBN, blue) and Au reference sample (red, offset for clarity) obtained at first harmonic demodulation (a). Normalized near-field amplitude and phase spectra acquired on a 60 nm ((b), integration time t = 15 minutes and spectral resolution δ v ¯ = 26 cm 1) and a 8 nm thick flake ((c), t = 56 minutes, δ v ¯ = 31 cm 1). AFM topography (d), and spectrally integrated optical image (e) across an hBN/Au step edge. Line traces shown in panel (f) correspond to the dashed line in panel (e) and show ~ 25 nm spatial resolution (5-95% signal level).
Fig. 3
Fig. 3 (a) Spatially resolved spectra near an hBN edge with emergence of blue-shifted resonance near the in-plane TO phonon peak at 1370 cm−1 due to the constructive interference of phonon polaritons excited by the tip and reflected by the edge. (b) Topography of the ~ 60 nm thick flake with the colored points representing the acquisition positions of the spectra in (a). Distance d from the edge is indicated. (c) Dispersion relation of the phonon polaritons with red points extracted from the spectra in (a). Grayscale plot is Im(rp) calculated using results from [21]. Blue line is the dispersion relation based on the model presented in [22].
Fig. 4
Fig. 4 Near-field magnitude (blue) and phase (red) spectra for (a) a 300 nm thick amorphous SiO2 layer and (b) PTFE. Spectra were obtained with integration times of 30 min and 5 min, and spectral resolution of 26 cm−1 and 21 cm−1 for SiO2 and PTFE, respectively. The SiO2 spectrum matches the predictions from the point dipole model (PDM) over a broad spectral range. The PTFE near-field spectrum is plotted in comparison with the complex index of refraction n ( v ¯ ) and k ( v ¯ ) [29].
Fig. 5
Fig. 5 Signal-to-noise ratio analysis for s-SNOM spectra of different samples using the thermal blackbody source (red, first harmonic), synchrotron infrared near-field spectroscopy (SINS) (blue, second harmonic) and different laser sources (black, third harmonic). NSNR analysis for published work are referenced [X] with corresponding citation number.
Fig. 6
Fig. 6 NSNRs of the in-plane (red) and out-of-plane (blue) TO phonon response of hBN as a function of spectral irradiance I incident on the tip. The results were obtained by decreasing the temperature of the thermal source primarily resulting in a decrease in IR intensity. Dashed blue and red lines are fits to a theoretical NSNR ( I ) = A I / ( I + B ) irradiance dependence.
Fig. 7
Fig. 7 Measurement of the focal spot at the tip using a knife edge technique. Data (black) is approximately described by a Gaussian intensity profile with FHWM of 70 μm (red).
Fig. 8
Fig. 8 Approach curves of the s-SNOM signal taken above a gold surface with reference arm at zero path difference. Demodulation at both the first (Ω) and second harmonic (2Ω) show strong near-field content with an order-of-magnitude increase within the last 50 nm.

Equations (2)

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I = | E nf + E bkg + E ref | 2
= | E nf | 2 + | E bkg | 2 + | E ref | 2 + 2 Re ( E bkg E ref ) + 2 Re ( E nf E bkg ) + 2 Re ( E nf E ref ) .

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