Abstract

We have developed coherent two-dimensional (2D) fluorescence micro-spectroscopy which probes the nonlinear optical response at surfaces via fluorescence detection with sub-micron spatial resolution. This enables the investigation of microscopic variations in heterogeneous systems. An LCD-based pulse shaper in 4f geometry is used to create collinear trains of 12-fs visible/NIR laser pulses in the focus of an NA = 1.4 immersion-oil microscope objective. We demonstrate the capabilities of the new method by presenting 2D spectra, analyzed via phase cycling, as a function of position of selected sub-micron regions from a laterally nanostructured polycrystalline thin film of fluorinated zinc phthalocyanine (F16ZnPc).

© 2018 Optical Society of America under the terms of the OSA Open Access Publishing Agreement

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References

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    [Crossref] [PubMed]
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    [Crossref]
  46. S. Goetz, G. Razinskas, E. Krauss, C. Dreher, M. Wurdack, P. Geisler, M. Pawłowska, B. Hecht, and T. Brixner, “Investigation of the nonlinear refractive index of single-crystalline thin gold films and plasmonic nanostructures,” Appl. Phys. B 122, 1–10 (2016).
    [Crossref]
  47. T.-w. Wu, J. Tang, B. Hajj, and M. Cui, “Phase resolved interferometric spectral modulation (PRISM) for ultrafast pulse measurement and compression,” Opt. Express 19, 12961–12968 (2011).
    [Crossref] [PubMed]
  48. M. Brendel, S. Krause, A. Steindamm, A. K. Topczak, S. Sundarraj, P. Erk, S. Höhla, N. Fruehauf, N. Koch, and J. Pflaum, “The effect of gradual fluorination on the properties of FnZnPc thin films and FnZnPc/C60 bilayer photovoltaic cells,” Adv. Funct. Mater. 25, 1565–1573 (2015).
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    [Crossref] [PubMed]

2017 (5)

J. S. Ostrander, R. Knepper, A. S. Tappan, J. J. Kay, M. T. Zanni, and D. A. Farrow, “Energy transfer between coherently delocalized states in thin films of the explosive pentaerythritol tetranitrate (PETN) revealed by two-dimensional infrared spectroscopy,” J. Phys. Chem. B 121, 1352–1361 (2017).
[Crossref] [PubMed]

S. Draeger, S. Roeding, and T. Brixner, “Rapid-scan coherent 2D fluorescence spectroscopy,” Opt. Express 25, 3259–3267 (2017).
[Crossref] [PubMed]

Z. Guo, Y. Wan, M. Yang, J. Snaider, K. Zhu, and L. Huang, “Long-range hot-carrier transport in hybrid perovskites visualized by ultrafast microscopy,” Science 356, 59–62 (2017).
[Crossref] [PubMed]

G. Moody and S. T. Cundiff, “Advances in multi-dimensional coherent spectroscopy of semiconductor nanostructures,” Adv. Phys. X 2, 641–674 (2017).
[PubMed]

V. Kolb and J. Pflaum, “Hybrid metal-organic nanocavity arrays for efficient light out-coupling,” Opt. Express 25, 6678–6689 (2017).
[Crossref] [PubMed]

2016 (3)

S. Goetz, G. Razinskas, E. Krauss, C. Dreher, M. Wurdack, P. Geisler, M. Pawłowska, B. Hecht, and T. Brixner, “Investigation of the nonlinear refractive index of single-crystalline thin gold films and plasmonic nanostructures,” Appl. Phys. B 122, 1–10 (2016).
[Crossref]

E. Vella, H. Li, P. Grégoire, S. M. Tuladhar, M. S. Vezie, S. Few, C. M. Bazán, J. Nelson, C. Silva-Acuña, and E. R. Bittner, “Ultrafast decoherence dynamics govern photocarrier generation efficiencies in polymer solar cells,” Sci. Rep. 6, 29437 (2016).
[Crossref] [PubMed]

A. D. Sio, F. Troiani, M. Maiuri, J. Réhault, E. Sommer, J. Lim, S. F. Huelga, M. B. Plenio, C. A. Rozzi, G. Cerullo, E. Molinari, and C. Lienau, “Tracking the coherent generation of polaron pairs in conjugated polymers,” Nat. Commun. 7, 13742 (2016).
[Crossref] [PubMed]

2015 (8)

T. A. Oudenhoven, Y. Joo, J. E. Laaser, P. Gopalan, and M. T. Zanni, “Dye aggregation identified by vibrational coupling using 2D IR spectroscopy,” J. Chem. Phys. 142, 212449 (2015).
[Crossref] [PubMed]

G. Nardin, T. M. Autry, G. Moody, R. Singh, H. Li, and S. T. Cundiff, “Multi-dimensional coherent optical spectroscopy of semiconductor nanostructures: Collinear and non-collinear approaches,” J. Appl. Phys. 117, 112804 (2015).
[Crossref]

R. D. Mehlenbacher, T. J. McDonough, M. Grechko, M.-Y. Wu, M. S. Arnold, and M. T. Zanni, “Energy transfer pathways in semiconducting carbon nanotubes revealed using two-dimensional white-light spectroscopy,” Nat. Commun. 6, 6732 (2015).
[Crossref] [PubMed]

M. Aeschlimann, T. Brixner, D. Differt, U. Heinzmann, M. Hensen, C. Kramer, F. Lükermann, P. Melchior, W. Pfeiffer, M. Piecuch, C. Schneider, H. Stiebig, C. Strüber, and P. Thielen, “Perfect absorption in nanotextured thin films via Anderson-localized photon modes,” Nat. Photonics 9, 663–668 (2015).
[Crossref]

C. Y. Wong, B. L. Cotts, H. Wu, and N. S. Ginsberg, “Exciton dynamics reveal aggregates with intermolecular order at hidden interfaces in solution-cast organic semiconducting films,” Nat. Commun. 6, 6946 (2015).
[Crossref]

M. Brendel, S. Krause, A. Steindamm, A. K. Topczak, S. Sundarraj, P. Erk, S. Höhla, N. Fruehauf, N. Koch, and J. Pflaum, “The effect of gradual fluorination on the properties of FnZnPc thin films and FnZnPc/C60 bilayer photovoltaic cells,” Adv. Funct. Mater. 25, 1565–1573 (2015).
[Crossref]

R. Ciesielski, A. Comin, M. Handloser, K. Donkers, G. Piredda, A. Lombardo, A. C. Ferrari, and A. Hartschuh, “Graphene near-degenerate four-wave mixing for phase characterization of broadband pulses in ultrafast microscopy,” Nano Lett. 15, 4968–4972 (2015).
[Crossref] [PubMed]

F. D. Fuller and J. P. Ogilvie, “Experimental implementations of two-dimensional Fourier transform electronic spectroscopy,” Annu. Rev. Phys. Chem. 66, 667–690 (2015).
[Crossref] [PubMed]

2014 (7)

C. R. Baiz, D. Schach, and A. Tokmakoff, “Ultrafast 2D IR microscopy,” Opt. Express 22, 18724–18735 (2014).
[Crossref] [PubMed]

M. Pawłowska, S. Goetz, C. Dreher, M. Wurdack, E. Krauss, G. Razinskas, P. Geisler, B. Hecht, and T. Brixner, “Shaping and spatiotemporal characterization of sub-10-fs pulses focused by a high-NA objective,” Opt. Express 22, 31496–31510 (2014).
[Crossref]

C. Rewitz, G. Razinskas, P. Geisler, E. Krauss, S. Goetz, M. Pawłowska, B. Hecht, and T. Brixner, “Coherent control of plasmon propagation in a nanocircuit,” Phys. Rev. Applied 1, 014007 (2014).
[Crossref]

E. Wientjes, J. Renger, A. G. Curto, R. Cogdell, and N. F. v. Hulst, “Strong antenna-enhanced fluorescence of a single light-harvesting complex shows photon antibunching,” Nat. Commun. 5, 4236 (2014).
[Crossref] [PubMed]

M. M. Gabriel, E. M. Grumstrup, J. R. Kirschbrown, C. W. Pinion, J. D. Christesen, D. F. Zigler, E. E. M. Cating, J. F. Cahoon, and J. M. Papanikolas, “Imaging charge separation and carrier recombination in nanowire p-i-n junctions using ultrafast microscopy,” Nano Lett. 14, 3079–3087 (2014).
[Crossref] [PubMed]

A. K. De, D. Monahan, J. M. Dawlaty, and G. R. Fleming, “Two-dimensional fluorescence-detected coherent spectroscopy with absolute phasing by confocal imaging of a dynamic grating and 27-step phase-cycling,” J. Chem. Phys. 140, 194201 (2014).
[Crossref] [PubMed]

K. J. Karki, J. R. Widom, J. Seibt, I. Moody, M. C. Lonergan, T. Pullerits, and A. H. Marcus, “Coherent two-dimensional photocurrent spectroscopy in a PbS quantum dot photocell,” Nat. Commun. 5, 5869 (2014).
[Crossref] [PubMed]

2013 (4)

R. Hildner, D. Brinks, J. B. Nieder, R. J. Cogdell, and N. F. v. Hulst, “Quantum Coherent Energy Transfer over Varying Pathways in Single Light-Harvesting Complexes,” Science 340, 1448–1451 (2013).
[Crossref] [PubMed]

G. Moody, R. Singh, H. Li, I. A. Akimov, M. Bayer, D. Reuter, A. D. Wieck, and S. T. Cundiff, “Fifth-order nonlinear optical response of excitonic states in an InAs quantum dot ensemble measured with two-dimensional spectroscopy,” Phys. Rev. B 87, 045313 (2013).
[Crossref]

V. M. Huxter, T. a. A. Oliver, D. Budker, and G. R. Fleming, “Vibrational and electronic dynamics of nitrogen-vacancy centres in diamond revealed by two-dimensional ultrafast spectroscopy,” Nat. Phys. 9, 744–749 (2013).
[Crossref]

P. Geisler, G. Razinskas, E. Krauss, X.-F. Wu, C. Rewitz, P. Tuchscherer, S. Goetz, C.-B. Huang, T. Brixner, and B. Hecht, “Multimode plasmon excitation and in situ analysis in top-down fabricated nanocircuits,” Phys. Rev. Lett. 111, 183901 (2013).
[Crossref] [PubMed]

2012 (2)

C. Rewitz, T. Keitzl, P. Tuchscherer, S. Goetz, P. Geisler, G. Razinskas, B. Hecht, and T. Brixner, “Spectral-interference microscopy for characterization of functional plasmonic elements,” Opt. Express 20, 14632–14647 (2012).
[Crossref] [PubMed]

J. Bylsma, P. Dey, J. Paul, S. Hoogland, E. H. Sargent, J. M. Luther, M. C. Beard, and D. Karaiskaj, “Quantum beats due to excitonic ground-state splitting in colloidal quantum dots,” Phys. Rev. B 86, 125322 (2012).
[Crossref]

2011 (7)

G. Moody, M. E. Siemens, A. D. Bristow, X. Dai, D. Karaiskaj, A. S. Bracker, D. Gammon, and S. T. Cundiff, “Exciton-exciton and exciton-phonon interactions in an interfacial GaAs quantum dot ensemble,” Phys. Rev. B 83, 115324 (2011).
[Crossref]

C. Y. Wong and G. D. Scholes, “Biexcitonic fine structure of CdSe nanocrystals probed by polarization-dependent two-dimensional photon echo spectroscopy,” J. Phys. Chem. A 115, 3797–3806 (2011).
[Crossref]

J. Kasprzak, B. Patton, V. Savona, and W. Langbein, “Coherent coupling between distant excitons revealed by two-dimensional nonlinear hyperspectral imaging,” Nat. Photonics 5, 57–63 (2011).
[Crossref]

R. Hildner, D. Brinks, and N. F. v. Hulst, “Femtosecond coherence and quantum control of single molecules at room temperature,” Nat. Phys. 7, 172–177 (2011).
[Crossref]

M. Aeschlimann, T. Brixner, A. Fischer, C. Kramer, P. Melchior, W. Pfeiffer, C. Schneider, C. Strüber, P. Tuchscherer, and D. V. Voronine, “Coherent two-dimensional nanoscopy,” Science 333, 1723–1726 (2011).
[Crossref] [PubMed]

J. Cabanillas-Gonzalez, G. Grancini, and G. Lanzani, “Pump-probe spectroscopy in organic semiconductors: monitoring fundamental processes of relevance in optoelectronics,” Adv. Mater. 23, 5468–5485 (2011).
[Crossref] [PubMed]

T.-w. Wu, J. Tang, B. Hajj, and M. Cui, “Phase resolved interferometric spectral modulation (PRISM) for ultrafast pulse measurement and compression,” Opt. Express 19, 12961–12968 (2011).
[Crossref] [PubMed]

2010 (1)

D. Brinks, F. D. Stefani, F. Kulzer, R. Hildner, T. H. Taminiau, Y. Avlasevich, K. Mullen, and N. F. van Hulst, “Visualizing and controlling vibrational wave packets of single molecules,” Nature 465, 905–908 (2010).
[Crossref] [PubMed]

2009 (2)

K. W. Stone, K. Gundogdu, D. B. Turner, X. Li, S. T. Cundiff, and K. A. Nelson, “Two-quantum 2D FT electronic spectroscopy of biexcitons in GaAs quantum wells,” Science 324, 1169–1173 (2009).
[Crossref] [PubMed]

S.-H. Shim and M. T. Zanni, “How to turn your pump–probe instrument into a multidimensional spectrometer: 2D IR and VIS spectroscopies via pulse shaping,” Phys. Chem. Chem. Phys. 11, 748–761 (2009).
[Crossref] [PubMed]

2008 (1)

H.-S. Tan, “Theory and phase-cycling scheme selection principles of collinear phase coherent multi-dimensional optical spectroscopy,” J. Chem. Phys. 129, 124501 (2008).
[Crossref] [PubMed]

2007 (3)

G. S. Engel, T. R. Calhoun, E. L. Read, T.-K. Ahn, T. Mančal, Y.-C. Cheng, R. E. Blankenship, and G. R. Fleming, “Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems,” Nature 446, 782–786 (2007).
[Crossref] [PubMed]

P. F. Tekavec, G. A. Lott, and A. H. Marcus, “Fluorescence-detected two-dimensional electronic coherence spectroscopy by acousto-optic phase modulation,” J. Chem. Phys. 127, 214307 (2007).
[Crossref] [PubMed]

W. Langbein and B. Patton, “Transient coherent nonlinear spectroscopy of single quantum dots,” J. Phys.: Condens. Matter 19, 295203 (2007).

2005 (2)

W. Wagner, C. Li, J. Semmlow, and W. S. Warren, “Rapid phase-cycled two-dimensional optical spectroscopy in fluorescence and transmission mode,” Opt. Express 13, 3697–3706 (2005).
[Crossref] [PubMed]

T. Brixner, J. Stenger, H. M. Vaswani, M. Cho, R. E. Blankenship, and G. R. Fleming, “Two-dimensional spectroscopy of electronic couplings in photosynthesis,” Nature 434, 625–628 (2005).
[Crossref] [PubMed]

2003 (1)

P. Tian, D. Keusters, Y. Suzaki, and W. S. Warren, “Femtosecond phase-coherent two-dimensional spectroscopy,” Science 300, 1553–1555 (2003).
[Crossref] [PubMed]

Aeschlimann, M.

M. Aeschlimann, T. Brixner, D. Differt, U. Heinzmann, M. Hensen, C. Kramer, F. Lükermann, P. Melchior, W. Pfeiffer, M. Piecuch, C. Schneider, H. Stiebig, C. Strüber, and P. Thielen, “Perfect absorption in nanotextured thin films via Anderson-localized photon modes,” Nat. Photonics 9, 663–668 (2015).
[Crossref]

M. Aeschlimann, T. Brixner, A. Fischer, C. Kramer, P. Melchior, W. Pfeiffer, C. Schneider, C. Strüber, P. Tuchscherer, and D. V. Voronine, “Coherent two-dimensional nanoscopy,” Science 333, 1723–1726 (2011).
[Crossref] [PubMed]

Ahn, T.-K.

G. S. Engel, T. R. Calhoun, E. L. Read, T.-K. Ahn, T. Mančal, Y.-C. Cheng, R. E. Blankenship, and G. R. Fleming, “Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems,” Nature 446, 782–786 (2007).
[Crossref] [PubMed]

Akimov, I. A.

G. Moody, R. Singh, H. Li, I. A. Akimov, M. Bayer, D. Reuter, A. D. Wieck, and S. T. Cundiff, “Fifth-order nonlinear optical response of excitonic states in an InAs quantum dot ensemble measured with two-dimensional spectroscopy,” Phys. Rev. B 87, 045313 (2013).
[Crossref]

Arnold, M. S.

R. D. Mehlenbacher, T. J. McDonough, M. Grechko, M.-Y. Wu, M. S. Arnold, and M. T. Zanni, “Energy transfer pathways in semiconducting carbon nanotubes revealed using two-dimensional white-light spectroscopy,” Nat. Commun. 6, 6732 (2015).
[Crossref] [PubMed]

Autry, T. M.

G. Nardin, T. M. Autry, G. Moody, R. Singh, H. Li, and S. T. Cundiff, “Multi-dimensional coherent optical spectroscopy of semiconductor nanostructures: Collinear and non-collinear approaches,” J. Appl. Phys. 117, 112804 (2015).
[Crossref]

Avlasevich, Y.

D. Brinks, F. D. Stefani, F. Kulzer, R. Hildner, T. H. Taminiau, Y. Avlasevich, K. Mullen, and N. F. van Hulst, “Visualizing and controlling vibrational wave packets of single molecules,” Nature 465, 905–908 (2010).
[Crossref] [PubMed]

Baiz, C. R.

Bayer, M.

G. Moody, R. Singh, H. Li, I. A. Akimov, M. Bayer, D. Reuter, A. D. Wieck, and S. T. Cundiff, “Fifth-order nonlinear optical response of excitonic states in an InAs quantum dot ensemble measured with two-dimensional spectroscopy,” Phys. Rev. B 87, 045313 (2013).
[Crossref]

Bazán, C. M.

E. Vella, H. Li, P. Grégoire, S. M. Tuladhar, M. S. Vezie, S. Few, C. M. Bazán, J. Nelson, C. Silva-Acuña, and E. R. Bittner, “Ultrafast decoherence dynamics govern photocarrier generation efficiencies in polymer solar cells,” Sci. Rep. 6, 29437 (2016).
[Crossref] [PubMed]

Beard, M. C.

J. Bylsma, P. Dey, J. Paul, S. Hoogland, E. H. Sargent, J. M. Luther, M. C. Beard, and D. Karaiskaj, “Quantum beats due to excitonic ground-state splitting in colloidal quantum dots,” Phys. Rev. B 86, 125322 (2012).
[Crossref]

Bittner, E. R.

E. Vella, H. Li, P. Grégoire, S. M. Tuladhar, M. S. Vezie, S. Few, C. M. Bazán, J. Nelson, C. Silva-Acuña, and E. R. Bittner, “Ultrafast decoherence dynamics govern photocarrier generation efficiencies in polymer solar cells,” Sci. Rep. 6, 29437 (2016).
[Crossref] [PubMed]

Blankenship, R. E.

G. S. Engel, T. R. Calhoun, E. L. Read, T.-K. Ahn, T. Mančal, Y.-C. Cheng, R. E. Blankenship, and G. R. Fleming, “Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems,” Nature 446, 782–786 (2007).
[Crossref] [PubMed]

T. Brixner, J. Stenger, H. M. Vaswani, M. Cho, R. E. Blankenship, and G. R. Fleming, “Two-dimensional spectroscopy of electronic couplings in photosynthesis,” Nature 434, 625–628 (2005).
[Crossref] [PubMed]

Bracker, A. S.

G. Moody, M. E. Siemens, A. D. Bristow, X. Dai, D. Karaiskaj, A. S. Bracker, D. Gammon, and S. T. Cundiff, “Exciton-exciton and exciton-phonon interactions in an interfacial GaAs quantum dot ensemble,” Phys. Rev. B 83, 115324 (2011).
[Crossref]

Brendel, M.

M. Brendel, S. Krause, A. Steindamm, A. K. Topczak, S. Sundarraj, P. Erk, S. Höhla, N. Fruehauf, N. Koch, and J. Pflaum, “The effect of gradual fluorination on the properties of FnZnPc thin films and FnZnPc/C60 bilayer photovoltaic cells,” Adv. Funct. Mater. 25, 1565–1573 (2015).
[Crossref]

Brinks, D.

R. Hildner, D. Brinks, J. B. Nieder, R. J. Cogdell, and N. F. v. Hulst, “Quantum Coherent Energy Transfer over Varying Pathways in Single Light-Harvesting Complexes,” Science 340, 1448–1451 (2013).
[Crossref] [PubMed]

R. Hildner, D. Brinks, and N. F. v. Hulst, “Femtosecond coherence and quantum control of single molecules at room temperature,” Nat. Phys. 7, 172–177 (2011).
[Crossref]

D. Brinks, F. D. Stefani, F. Kulzer, R. Hildner, T. H. Taminiau, Y. Avlasevich, K. Mullen, and N. F. van Hulst, “Visualizing and controlling vibrational wave packets of single molecules,” Nature 465, 905–908 (2010).
[Crossref] [PubMed]

Bristow, A. D.

G. Moody, M. E. Siemens, A. D. Bristow, X. Dai, D. Karaiskaj, A. S. Bracker, D. Gammon, and S. T. Cundiff, “Exciton-exciton and exciton-phonon interactions in an interfacial GaAs quantum dot ensemble,” Phys. Rev. B 83, 115324 (2011).
[Crossref]

Brixner, T.

S. Draeger, S. Roeding, and T. Brixner, “Rapid-scan coherent 2D fluorescence spectroscopy,” Opt. Express 25, 3259–3267 (2017).
[Crossref] [PubMed]

S. Goetz, G. Razinskas, E. Krauss, C. Dreher, M. Wurdack, P. Geisler, M. Pawłowska, B. Hecht, and T. Brixner, “Investigation of the nonlinear refractive index of single-crystalline thin gold films and plasmonic nanostructures,” Appl. Phys. B 122, 1–10 (2016).
[Crossref]

M. Aeschlimann, T. Brixner, D. Differt, U. Heinzmann, M. Hensen, C. Kramer, F. Lükermann, P. Melchior, W. Pfeiffer, M. Piecuch, C. Schneider, H. Stiebig, C. Strüber, and P. Thielen, “Perfect absorption in nanotextured thin films via Anderson-localized photon modes,” Nat. Photonics 9, 663–668 (2015).
[Crossref]

M. Pawłowska, S. Goetz, C. Dreher, M. Wurdack, E. Krauss, G. Razinskas, P. Geisler, B. Hecht, and T. Brixner, “Shaping and spatiotemporal characterization of sub-10-fs pulses focused by a high-NA objective,” Opt. Express 22, 31496–31510 (2014).
[Crossref]

C. Rewitz, G. Razinskas, P. Geisler, E. Krauss, S. Goetz, M. Pawłowska, B. Hecht, and T. Brixner, “Coherent control of plasmon propagation in a nanocircuit,” Phys. Rev. Applied 1, 014007 (2014).
[Crossref]

P. Geisler, G. Razinskas, E. Krauss, X.-F. Wu, C. Rewitz, P. Tuchscherer, S. Goetz, C.-B. Huang, T. Brixner, and B. Hecht, “Multimode plasmon excitation and in situ analysis in top-down fabricated nanocircuits,” Phys. Rev. Lett. 111, 183901 (2013).
[Crossref] [PubMed]

C. Rewitz, T. Keitzl, P. Tuchscherer, S. Goetz, P. Geisler, G. Razinskas, B. Hecht, and T. Brixner, “Spectral-interference microscopy for characterization of functional plasmonic elements,” Opt. Express 20, 14632–14647 (2012).
[Crossref] [PubMed]

M. Aeschlimann, T. Brixner, A. Fischer, C. Kramer, P. Melchior, W. Pfeiffer, C. Schneider, C. Strüber, P. Tuchscherer, and D. V. Voronine, “Coherent two-dimensional nanoscopy,” Science 333, 1723–1726 (2011).
[Crossref] [PubMed]

T. Brixner, J. Stenger, H. M. Vaswani, M. Cho, R. E. Blankenship, and G. R. Fleming, “Two-dimensional spectroscopy of electronic couplings in photosynthesis,” Nature 434, 625–628 (2005).
[Crossref] [PubMed]

S. Roeding and T. Brixner, “Multidimensional electronic spectroscopy in molecular beams with mass-resolved ion detection,” in “International Conference on Ultrafast Phenomena XX,” (Optical Society of America, 2016), p. UM3A.2.

Budker, D.

V. M. Huxter, T. a. A. Oliver, D. Budker, and G. R. Fleming, “Vibrational and electronic dynamics of nitrogen-vacancy centres in diamond revealed by two-dimensional ultrafast spectroscopy,” Nat. Phys. 9, 744–749 (2013).
[Crossref]

Bylsma, J.

J. Bylsma, P. Dey, J. Paul, S. Hoogland, E. H. Sargent, J. M. Luther, M. C. Beard, and D. Karaiskaj, “Quantum beats due to excitonic ground-state splitting in colloidal quantum dots,” Phys. Rev. B 86, 125322 (2012).
[Crossref]

Cabanillas-Gonzalez, J.

J. Cabanillas-Gonzalez, G. Grancini, and G. Lanzani, “Pump-probe spectroscopy in organic semiconductors: monitoring fundamental processes of relevance in optoelectronics,” Adv. Mater. 23, 5468–5485 (2011).
[Crossref] [PubMed]

Cahoon, J. F.

M. M. Gabriel, E. M. Grumstrup, J. R. Kirschbrown, C. W. Pinion, J. D. Christesen, D. F. Zigler, E. E. M. Cating, J. F. Cahoon, and J. M. Papanikolas, “Imaging charge separation and carrier recombination in nanowire p-i-n junctions using ultrafast microscopy,” Nano Lett. 14, 3079–3087 (2014).
[Crossref] [PubMed]

Calhoun, T. R.

G. S. Engel, T. R. Calhoun, E. L. Read, T.-K. Ahn, T. Mančal, Y.-C. Cheng, R. E. Blankenship, and G. R. Fleming, “Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems,” Nature 446, 782–786 (2007).
[Crossref] [PubMed]

Cating, E. E. M.

M. M. Gabriel, E. M. Grumstrup, J. R. Kirschbrown, C. W. Pinion, J. D. Christesen, D. F. Zigler, E. E. M. Cating, J. F. Cahoon, and J. M. Papanikolas, “Imaging charge separation and carrier recombination in nanowire p-i-n junctions using ultrafast microscopy,” Nano Lett. 14, 3079–3087 (2014).
[Crossref] [PubMed]

Cerullo, G.

A. D. Sio, F. Troiani, M. Maiuri, J. Réhault, E. Sommer, J. Lim, S. F. Huelga, M. B. Plenio, C. A. Rozzi, G. Cerullo, E. Molinari, and C. Lienau, “Tracking the coherent generation of polaron pairs in conjugated polymers,” Nat. Commun. 7, 13742 (2016).
[Crossref] [PubMed]

Cheng, Y.-C.

G. S. Engel, T. R. Calhoun, E. L. Read, T.-K. Ahn, T. Mančal, Y.-C. Cheng, R. E. Blankenship, and G. R. Fleming, “Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems,” Nature 446, 782–786 (2007).
[Crossref] [PubMed]

Cho, M.

T. Brixner, J. Stenger, H. M. Vaswani, M. Cho, R. E. Blankenship, and G. R. Fleming, “Two-dimensional spectroscopy of electronic couplings in photosynthesis,” Nature 434, 625–628 (2005).
[Crossref] [PubMed]

Christesen, J. D.

M. M. Gabriel, E. M. Grumstrup, J. R. Kirschbrown, C. W. Pinion, J. D. Christesen, D. F. Zigler, E. E. M. Cating, J. F. Cahoon, and J. M. Papanikolas, “Imaging charge separation and carrier recombination in nanowire p-i-n junctions using ultrafast microscopy,” Nano Lett. 14, 3079–3087 (2014).
[Crossref] [PubMed]

Ciesielski, R.

R. Ciesielski, A. Comin, M. Handloser, K. Donkers, G. Piredda, A. Lombardo, A. C. Ferrari, and A. Hartschuh, “Graphene near-degenerate four-wave mixing for phase characterization of broadband pulses in ultrafast microscopy,” Nano Lett. 15, 4968–4972 (2015).
[Crossref] [PubMed]

Cogdell, R.

E. Wientjes, J. Renger, A. G. Curto, R. Cogdell, and N. F. v. Hulst, “Strong antenna-enhanced fluorescence of a single light-harvesting complex shows photon antibunching,” Nat. Commun. 5, 4236 (2014).
[Crossref] [PubMed]

Cogdell, R. J.

R. Hildner, D. Brinks, J. B. Nieder, R. J. Cogdell, and N. F. v. Hulst, “Quantum Coherent Energy Transfer over Varying Pathways in Single Light-Harvesting Complexes,” Science 340, 1448–1451 (2013).
[Crossref] [PubMed]

Comin, A.

R. Ciesielski, A. Comin, M. Handloser, K. Donkers, G. Piredda, A. Lombardo, A. C. Ferrari, and A. Hartschuh, “Graphene near-degenerate four-wave mixing for phase characterization of broadband pulses in ultrafast microscopy,” Nano Lett. 15, 4968–4972 (2015).
[Crossref] [PubMed]

Cotts, B. L.

C. Y. Wong, B. L. Cotts, H. Wu, and N. S. Ginsberg, “Exciton dynamics reveal aggregates with intermolecular order at hidden interfaces in solution-cast organic semiconducting films,” Nat. Commun. 6, 6946 (2015).
[Crossref]

Cui, M.

Cundiff, S. T.

G. Moody and S. T. Cundiff, “Advances in multi-dimensional coherent spectroscopy of semiconductor nanostructures,” Adv. Phys. X 2, 641–674 (2017).
[PubMed]

G. Nardin, T. M. Autry, G. Moody, R. Singh, H. Li, and S. T. Cundiff, “Multi-dimensional coherent optical spectroscopy of semiconductor nanostructures: Collinear and non-collinear approaches,” J. Appl. Phys. 117, 112804 (2015).
[Crossref]

G. Moody, R. Singh, H. Li, I. A. Akimov, M. Bayer, D. Reuter, A. D. Wieck, and S. T. Cundiff, “Fifth-order nonlinear optical response of excitonic states in an InAs quantum dot ensemble measured with two-dimensional spectroscopy,” Phys. Rev. B 87, 045313 (2013).
[Crossref]

G. Moody, M. E. Siemens, A. D. Bristow, X. Dai, D. Karaiskaj, A. S. Bracker, D. Gammon, and S. T. Cundiff, “Exciton-exciton and exciton-phonon interactions in an interfacial GaAs quantum dot ensemble,” Phys. Rev. B 83, 115324 (2011).
[Crossref]

K. W. Stone, K. Gundogdu, D. B. Turner, X. Li, S. T. Cundiff, and K. A. Nelson, “Two-quantum 2D FT electronic spectroscopy of biexcitons in GaAs quantum wells,” Science 324, 1169–1173 (2009).
[Crossref] [PubMed]

Curto, A. G.

E. Wientjes, J. Renger, A. G. Curto, R. Cogdell, and N. F. v. Hulst, “Strong antenna-enhanced fluorescence of a single light-harvesting complex shows photon antibunching,” Nat. Commun. 5, 4236 (2014).
[Crossref] [PubMed]

Dai, X.

G. Moody, M. E. Siemens, A. D. Bristow, X. Dai, D. Karaiskaj, A. S. Bracker, D. Gammon, and S. T. Cundiff, “Exciton-exciton and exciton-phonon interactions in an interfacial GaAs quantum dot ensemble,” Phys. Rev. B 83, 115324 (2011).
[Crossref]

Dawlaty, J. M.

A. K. De, D. Monahan, J. M. Dawlaty, and G. R. Fleming, “Two-dimensional fluorescence-detected coherent spectroscopy with absolute phasing by confocal imaging of a dynamic grating and 27-step phase-cycling,” J. Chem. Phys. 140, 194201 (2014).
[Crossref] [PubMed]

De, A. K.

A. K. De, D. Monahan, J. M. Dawlaty, and G. R. Fleming, “Two-dimensional fluorescence-detected coherent spectroscopy with absolute phasing by confocal imaging of a dynamic grating and 27-step phase-cycling,” J. Chem. Phys. 140, 194201 (2014).
[Crossref] [PubMed]

Dey, P.

J. Bylsma, P. Dey, J. Paul, S. Hoogland, E. H. Sargent, J. M. Luther, M. C. Beard, and D. Karaiskaj, “Quantum beats due to excitonic ground-state splitting in colloidal quantum dots,” Phys. Rev. B 86, 125322 (2012).
[Crossref]

Differt, D.

M. Aeschlimann, T. Brixner, D. Differt, U. Heinzmann, M. Hensen, C. Kramer, F. Lükermann, P. Melchior, W. Pfeiffer, M. Piecuch, C. Schneider, H. Stiebig, C. Strüber, and P. Thielen, “Perfect absorption in nanotextured thin films via Anderson-localized photon modes,” Nat. Photonics 9, 663–668 (2015).
[Crossref]

Donkers, K.

R. Ciesielski, A. Comin, M. Handloser, K. Donkers, G. Piredda, A. Lombardo, A. C. Ferrari, and A. Hartschuh, “Graphene near-degenerate four-wave mixing for phase characterization of broadband pulses in ultrafast microscopy,” Nano Lett. 15, 4968–4972 (2015).
[Crossref] [PubMed]

Draeger, S.

Dreher, C.

S. Goetz, G. Razinskas, E. Krauss, C. Dreher, M. Wurdack, P. Geisler, M. Pawłowska, B. Hecht, and T. Brixner, “Investigation of the nonlinear refractive index of single-crystalline thin gold films and plasmonic nanostructures,” Appl. Phys. B 122, 1–10 (2016).
[Crossref]

M. Pawłowska, S. Goetz, C. Dreher, M. Wurdack, E. Krauss, G. Razinskas, P. Geisler, B. Hecht, and T. Brixner, “Shaping and spatiotemporal characterization of sub-10-fs pulses focused by a high-NA objective,” Opt. Express 22, 31496–31510 (2014).
[Crossref]

Engel, G. S.

G. S. Engel, T. R. Calhoun, E. L. Read, T.-K. Ahn, T. Mančal, Y.-C. Cheng, R. E. Blankenship, and G. R. Fleming, “Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems,” Nature 446, 782–786 (2007).
[Crossref] [PubMed]

Erk, P.

M. Brendel, S. Krause, A. Steindamm, A. K. Topczak, S. Sundarraj, P. Erk, S. Höhla, N. Fruehauf, N. Koch, and J. Pflaum, “The effect of gradual fluorination on the properties of FnZnPc thin films and FnZnPc/C60 bilayer photovoltaic cells,” Adv. Funct. Mater. 25, 1565–1573 (2015).
[Crossref]

Farrow, D. A.

J. S. Ostrander, R. Knepper, A. S. Tappan, J. J. Kay, M. T. Zanni, and D. A. Farrow, “Energy transfer between coherently delocalized states in thin films of the explosive pentaerythritol tetranitrate (PETN) revealed by two-dimensional infrared spectroscopy,” J. Phys. Chem. B 121, 1352–1361 (2017).
[Crossref] [PubMed]

Ferrari, A. C.

R. Ciesielski, A. Comin, M. Handloser, K. Donkers, G. Piredda, A. Lombardo, A. C. Ferrari, and A. Hartschuh, “Graphene near-degenerate four-wave mixing for phase characterization of broadband pulses in ultrafast microscopy,” Nano Lett. 15, 4968–4972 (2015).
[Crossref] [PubMed]

Few, S.

E. Vella, H. Li, P. Grégoire, S. M. Tuladhar, M. S. Vezie, S. Few, C. M. Bazán, J. Nelson, C. Silva-Acuña, and E. R. Bittner, “Ultrafast decoherence dynamics govern photocarrier generation efficiencies in polymer solar cells,” Sci. Rep. 6, 29437 (2016).
[Crossref] [PubMed]

Fischer, A.

M. Aeschlimann, T. Brixner, A. Fischer, C. Kramer, P. Melchior, W. Pfeiffer, C. Schneider, C. Strüber, P. Tuchscherer, and D. V. Voronine, “Coherent two-dimensional nanoscopy,” Science 333, 1723–1726 (2011).
[Crossref] [PubMed]

Fleming, G. R.

A. K. De, D. Monahan, J. M. Dawlaty, and G. R. Fleming, “Two-dimensional fluorescence-detected coherent spectroscopy with absolute phasing by confocal imaging of a dynamic grating and 27-step phase-cycling,” J. Chem. Phys. 140, 194201 (2014).
[Crossref] [PubMed]

V. M. Huxter, T. a. A. Oliver, D. Budker, and G. R. Fleming, “Vibrational and electronic dynamics of nitrogen-vacancy centres in diamond revealed by two-dimensional ultrafast spectroscopy,” Nat. Phys. 9, 744–749 (2013).
[Crossref]

G. S. Engel, T. R. Calhoun, E. L. Read, T.-K. Ahn, T. Mančal, Y.-C. Cheng, R. E. Blankenship, and G. R. Fleming, “Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems,” Nature 446, 782–786 (2007).
[Crossref] [PubMed]

T. Brixner, J. Stenger, H. M. Vaswani, M. Cho, R. E. Blankenship, and G. R. Fleming, “Two-dimensional spectroscopy of electronic couplings in photosynthesis,” Nature 434, 625–628 (2005).
[Crossref] [PubMed]

Fruehauf, N.

M. Brendel, S. Krause, A. Steindamm, A. K. Topczak, S. Sundarraj, P. Erk, S. Höhla, N. Fruehauf, N. Koch, and J. Pflaum, “The effect of gradual fluorination on the properties of FnZnPc thin films and FnZnPc/C60 bilayer photovoltaic cells,” Adv. Funct. Mater. 25, 1565–1573 (2015).
[Crossref]

Fuller, F. D.

F. D. Fuller and J. P. Ogilvie, “Experimental implementations of two-dimensional Fourier transform electronic spectroscopy,” Annu. Rev. Phys. Chem. 66, 667–690 (2015).
[Crossref] [PubMed]

Gabriel, M. M.

M. M. Gabriel, E. M. Grumstrup, J. R. Kirschbrown, C. W. Pinion, J. D. Christesen, D. F. Zigler, E. E. M. Cating, J. F. Cahoon, and J. M. Papanikolas, “Imaging charge separation and carrier recombination in nanowire p-i-n junctions using ultrafast microscopy,” Nano Lett. 14, 3079–3087 (2014).
[Crossref] [PubMed]

Gammon, D.

G. Moody, M. E. Siemens, A. D. Bristow, X. Dai, D. Karaiskaj, A. S. Bracker, D. Gammon, and S. T. Cundiff, “Exciton-exciton and exciton-phonon interactions in an interfacial GaAs quantum dot ensemble,” Phys. Rev. B 83, 115324 (2011).
[Crossref]

Geisler, P.

S. Goetz, G. Razinskas, E. Krauss, C. Dreher, M. Wurdack, P. Geisler, M. Pawłowska, B. Hecht, and T. Brixner, “Investigation of the nonlinear refractive index of single-crystalline thin gold films and plasmonic nanostructures,” Appl. Phys. B 122, 1–10 (2016).
[Crossref]

M. Pawłowska, S. Goetz, C. Dreher, M. Wurdack, E. Krauss, G. Razinskas, P. Geisler, B. Hecht, and T. Brixner, “Shaping and spatiotemporal characterization of sub-10-fs pulses focused by a high-NA objective,” Opt. Express 22, 31496–31510 (2014).
[Crossref]

C. Rewitz, G. Razinskas, P. Geisler, E. Krauss, S. Goetz, M. Pawłowska, B. Hecht, and T. Brixner, “Coherent control of plasmon propagation in a nanocircuit,” Phys. Rev. Applied 1, 014007 (2014).
[Crossref]

P. Geisler, G. Razinskas, E. Krauss, X.-F. Wu, C. Rewitz, P. Tuchscherer, S. Goetz, C.-B. Huang, T. Brixner, and B. Hecht, “Multimode plasmon excitation and in situ analysis in top-down fabricated nanocircuits,” Phys. Rev. Lett. 111, 183901 (2013).
[Crossref] [PubMed]

C. Rewitz, T. Keitzl, P. Tuchscherer, S. Goetz, P. Geisler, G. Razinskas, B. Hecht, and T. Brixner, “Spectral-interference microscopy for characterization of functional plasmonic elements,” Opt. Express 20, 14632–14647 (2012).
[Crossref] [PubMed]

Ginsberg, N. S.

C. Y. Wong, B. L. Cotts, H. Wu, and N. S. Ginsberg, “Exciton dynamics reveal aggregates with intermolecular order at hidden interfaces in solution-cast organic semiconducting films,” Nat. Commun. 6, 6946 (2015).
[Crossref]

Goetz, S.

S. Goetz, G. Razinskas, E. Krauss, C. Dreher, M. Wurdack, P. Geisler, M. Pawłowska, B. Hecht, and T. Brixner, “Investigation of the nonlinear refractive index of single-crystalline thin gold films and plasmonic nanostructures,” Appl. Phys. B 122, 1–10 (2016).
[Crossref]

C. Rewitz, G. Razinskas, P. Geisler, E. Krauss, S. Goetz, M. Pawłowska, B. Hecht, and T. Brixner, “Coherent control of plasmon propagation in a nanocircuit,” Phys. Rev. Applied 1, 014007 (2014).
[Crossref]

M. Pawłowska, S. Goetz, C. Dreher, M. Wurdack, E. Krauss, G. Razinskas, P. Geisler, B. Hecht, and T. Brixner, “Shaping and spatiotemporal characterization of sub-10-fs pulses focused by a high-NA objective,” Opt. Express 22, 31496–31510 (2014).
[Crossref]

P. Geisler, G. Razinskas, E. Krauss, X.-F. Wu, C. Rewitz, P. Tuchscherer, S. Goetz, C.-B. Huang, T. Brixner, and B. Hecht, “Multimode plasmon excitation and in situ analysis in top-down fabricated nanocircuits,” Phys. Rev. Lett. 111, 183901 (2013).
[Crossref] [PubMed]

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T. A. Oudenhoven, Y. Joo, J. E. Laaser, P. Gopalan, and M. T. Zanni, “Dye aggregation identified by vibrational coupling using 2D IR spectroscopy,” J. Chem. Phys. 142, 212449 (2015).
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J. Cabanillas-Gonzalez, G. Grancini, and G. Lanzani, “Pump-probe spectroscopy in organic semiconductors: monitoring fundamental processes of relevance in optoelectronics,” Adv. Mater. 23, 5468–5485 (2011).
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R. D. Mehlenbacher, T. J. McDonough, M. Grechko, M.-Y. Wu, M. S. Arnold, and M. T. Zanni, “Energy transfer pathways in semiconducting carbon nanotubes revealed using two-dimensional white-light spectroscopy,” Nat. Commun. 6, 6732 (2015).
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E. Vella, H. Li, P. Grégoire, S. M. Tuladhar, M. S. Vezie, S. Few, C. M. Bazán, J. Nelson, C. Silva-Acuña, and E. R. Bittner, “Ultrafast decoherence dynamics govern photocarrier generation efficiencies in polymer solar cells,” Sci. Rep. 6, 29437 (2016).
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C. Rewitz, G. Razinskas, P. Geisler, E. Krauss, S. Goetz, M. Pawłowska, B. Hecht, and T. Brixner, “Coherent control of plasmon propagation in a nanocircuit,” Phys. Rev. Applied 1, 014007 (2014).
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R. Hildner, D. Brinks, and N. F. v. Hulst, “Femtosecond coherence and quantum control of single molecules at room temperature,” Nat. Phys. 7, 172–177 (2011).
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T. A. Oudenhoven, Y. Joo, J. E. Laaser, P. Gopalan, and M. T. Zanni, “Dye aggregation identified by vibrational coupling using 2D IR spectroscopy,” J. Chem. Phys. 142, 212449 (2015).
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G. Moody, M. E. Siemens, A. D. Bristow, X. Dai, D. Karaiskaj, A. S. Bracker, D. Gammon, and S. T. Cundiff, “Exciton-exciton and exciton-phonon interactions in an interfacial GaAs quantum dot ensemble,” Phys. Rev. B 83, 115324 (2011).
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M. Brendel, S. Krause, A. Steindamm, A. K. Topczak, S. Sundarraj, P. Erk, S. Höhla, N. Fruehauf, N. Koch, and J. Pflaum, “The effect of gradual fluorination on the properties of FnZnPc thin films and FnZnPc/C60 bilayer photovoltaic cells,” Adv. Funct. Mater. 25, 1565–1573 (2015).
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M. Aeschlimann, T. Brixner, D. Differt, U. Heinzmann, M. Hensen, C. Kramer, F. Lükermann, P. Melchior, W. Pfeiffer, M. Piecuch, C. Schneider, H. Stiebig, C. Strüber, and P. Thielen, “Perfect absorption in nanotextured thin films via Anderson-localized photon modes,” Nat. Photonics 9, 663–668 (2015).
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[Crossref]

M. Pawłowska, S. Goetz, C. Dreher, M. Wurdack, E. Krauss, G. Razinskas, P. Geisler, B. Hecht, and T. Brixner, “Shaping and spatiotemporal characterization of sub-10-fs pulses focused by a high-NA objective,” Opt. Express 22, 31496–31510 (2014).
[Crossref]

C. Rewitz, G. Razinskas, P. Geisler, E. Krauss, S. Goetz, M. Pawłowska, B. Hecht, and T. Brixner, “Coherent control of plasmon propagation in a nanocircuit,” Phys. Rev. Applied 1, 014007 (2014).
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P. Geisler, G. Razinskas, E. Krauss, X.-F. Wu, C. Rewitz, P. Tuchscherer, S. Goetz, C.-B. Huang, T. Brixner, and B. Hecht, “Multimode plasmon excitation and in situ analysis in top-down fabricated nanocircuits,” Phys. Rev. Lett. 111, 183901 (2013).
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D. Brinks, F. D. Stefani, F. Kulzer, R. Hildner, T. H. Taminiau, Y. Avlasevich, K. Mullen, and N. F. van Hulst, “Visualizing and controlling vibrational wave packets of single molecules,” Nature 465, 905–908 (2010).
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T. A. Oudenhoven, Y. Joo, J. E. Laaser, P. Gopalan, and M. T. Zanni, “Dye aggregation identified by vibrational coupling using 2D IR spectroscopy,” J. Chem. Phys. 142, 212449 (2015).
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J. Kasprzak, B. Patton, V. Savona, and W. Langbein, “Coherent coupling between distant excitons revealed by two-dimensional nonlinear hyperspectral imaging,” Nat. Photonics 5, 57–63 (2011).
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J. Cabanillas-Gonzalez, G. Grancini, and G. Lanzani, “Pump-probe spectroscopy in organic semiconductors: monitoring fundamental processes of relevance in optoelectronics,” Adv. Mater. 23, 5468–5485 (2011).
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G. Moody, R. Singh, H. Li, I. A. Akimov, M. Bayer, D. Reuter, A. D. Wieck, and S. T. Cundiff, “Fifth-order nonlinear optical response of excitonic states in an InAs quantum dot ensemble measured with two-dimensional spectroscopy,” Phys. Rev. B 87, 045313 (2013).
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K. W. Stone, K. Gundogdu, D. B. Turner, X. Li, S. T. Cundiff, and K. A. Nelson, “Two-quantum 2D FT electronic spectroscopy of biexcitons in GaAs quantum wells,” Science 324, 1169–1173 (2009).
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K. J. Karki, J. R. Widom, J. Seibt, I. Moody, M. C. Lonergan, T. Pullerits, and A. H. Marcus, “Coherent two-dimensional photocurrent spectroscopy in a PbS quantum dot photocell,” Nat. Commun. 5, 5869 (2014).
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P. F. Tekavec, G. A. Lott, and A. H. Marcus, “Fluorescence-detected two-dimensional electronic coherence spectroscopy by acousto-optic phase modulation,” J. Chem. Phys. 127, 214307 (2007).
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M. Aeschlimann, T. Brixner, D. Differt, U. Heinzmann, M. Hensen, C. Kramer, F. Lükermann, P. Melchior, W. Pfeiffer, M. Piecuch, C. Schneider, H. Stiebig, C. Strüber, and P. Thielen, “Perfect absorption in nanotextured thin films via Anderson-localized photon modes,” Nat. Photonics 9, 663–668 (2015).
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J. Bylsma, P. Dey, J. Paul, S. Hoogland, E. H. Sargent, J. M. Luther, M. C. Beard, and D. Karaiskaj, “Quantum beats due to excitonic ground-state splitting in colloidal quantum dots,” Phys. Rev. B 86, 125322 (2012).
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K. J. Karki, J. R. Widom, J. Seibt, I. Moody, M. C. Lonergan, T. Pullerits, and A. H. Marcus, “Coherent two-dimensional photocurrent spectroscopy in a PbS quantum dot photocell,” Nat. Commun. 5, 5869 (2014).
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P. F. Tekavec, G. A. Lott, and A. H. Marcus, “Fluorescence-detected two-dimensional electronic coherence spectroscopy by acousto-optic phase modulation,” J. Chem. Phys. 127, 214307 (2007).
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R. D. Mehlenbacher, T. J. McDonough, M. Grechko, M.-Y. Wu, M. S. Arnold, and M. T. Zanni, “Energy transfer pathways in semiconducting carbon nanotubes revealed using two-dimensional white-light spectroscopy,” Nat. Commun. 6, 6732 (2015).
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M. Aeschlimann, T. Brixner, D. Differt, U. Heinzmann, M. Hensen, C. Kramer, F. Lükermann, P. Melchior, W. Pfeiffer, M. Piecuch, C. Schneider, H. Stiebig, C. Strüber, and P. Thielen, “Perfect absorption in nanotextured thin films via Anderson-localized photon modes,” Nat. Photonics 9, 663–668 (2015).
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M. Aeschlimann, T. Brixner, A. Fischer, C. Kramer, P. Melchior, W. Pfeiffer, C. Schneider, C. Strüber, P. Tuchscherer, and D. V. Voronine, “Coherent two-dimensional nanoscopy,” Science 333, 1723–1726 (2011).
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A. D. Sio, F. Troiani, M. Maiuri, J. Réhault, E. Sommer, J. Lim, S. F. Huelga, M. B. Plenio, C. A. Rozzi, G. Cerullo, E. Molinari, and C. Lienau, “Tracking the coherent generation of polaron pairs in conjugated polymers,” Nat. Commun. 7, 13742 (2016).
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[Crossref]

G. Moody, R. Singh, H. Li, I. A. Akimov, M. Bayer, D. Reuter, A. D. Wieck, and S. T. Cundiff, “Fifth-order nonlinear optical response of excitonic states in an InAs quantum dot ensemble measured with two-dimensional spectroscopy,” Phys. Rev. B 87, 045313 (2013).
[Crossref]

G. Moody, M. E. Siemens, A. D. Bristow, X. Dai, D. Karaiskaj, A. S. Bracker, D. Gammon, and S. T. Cundiff, “Exciton-exciton and exciton-phonon interactions in an interfacial GaAs quantum dot ensemble,” Phys. Rev. B 83, 115324 (2011).
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K. J. Karki, J. R. Widom, J. Seibt, I. Moody, M. C. Lonergan, T. Pullerits, and A. H. Marcus, “Coherent two-dimensional photocurrent spectroscopy in a PbS quantum dot photocell,” Nat. Commun. 5, 5869 (2014).
[Crossref] [PubMed]

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D. Brinks, F. D. Stefani, F. Kulzer, R. Hildner, T. H. Taminiau, Y. Avlasevich, K. Mullen, and N. F. van Hulst, “Visualizing and controlling vibrational wave packets of single molecules,” Nature 465, 905–908 (2010).
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G. Nardin, T. M. Autry, G. Moody, R. Singh, H. Li, and S. T. Cundiff, “Multi-dimensional coherent optical spectroscopy of semiconductor nanostructures: Collinear and non-collinear approaches,” J. Appl. Phys. 117, 112804 (2015).
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E. Vella, H. Li, P. Grégoire, S. M. Tuladhar, M. S. Vezie, S. Few, C. M. Bazán, J. Nelson, C. Silva-Acuña, and E. R. Bittner, “Ultrafast decoherence dynamics govern photocarrier generation efficiencies in polymer solar cells,” Sci. Rep. 6, 29437 (2016).
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K. W. Stone, K. Gundogdu, D. B. Turner, X. Li, S. T. Cundiff, and K. A. Nelson, “Two-quantum 2D FT electronic spectroscopy of biexcitons in GaAs quantum wells,” Science 324, 1169–1173 (2009).
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Wong, C. Y.

C. Y. Wong, B. L. Cotts, H. Wu, and N. S. Ginsberg, “Exciton dynamics reveal aggregates with intermolecular order at hidden interfaces in solution-cast organic semiconducting films,” Nat. Commun. 6, 6946 (2015).
[Crossref]

C. Y. Wong and G. D. Scholes, “Biexcitonic fine structure of CdSe nanocrystals probed by polarization-dependent two-dimensional photon echo spectroscopy,” J. Phys. Chem. A 115, 3797–3806 (2011).
[Crossref]

Wu, H.

C. Y. Wong, B. L. Cotts, H. Wu, and N. S. Ginsberg, “Exciton dynamics reveal aggregates with intermolecular order at hidden interfaces in solution-cast organic semiconducting films,” Nat. Commun. 6, 6946 (2015).
[Crossref]

Wu, M.-Y.

R. D. Mehlenbacher, T. J. McDonough, M. Grechko, M.-Y. Wu, M. S. Arnold, and M. T. Zanni, “Energy transfer pathways in semiconducting carbon nanotubes revealed using two-dimensional white-light spectroscopy,” Nat. Commun. 6, 6732 (2015).
[Crossref] [PubMed]

Wu, T.-w.

Wu, X.-F.

P. Geisler, G. Razinskas, E. Krauss, X.-F. Wu, C. Rewitz, P. Tuchscherer, S. Goetz, C.-B. Huang, T. Brixner, and B. Hecht, “Multimode plasmon excitation and in situ analysis in top-down fabricated nanocircuits,” Phys. Rev. Lett. 111, 183901 (2013).
[Crossref] [PubMed]

Wurdack, M.

S. Goetz, G. Razinskas, E. Krauss, C. Dreher, M. Wurdack, P. Geisler, M. Pawłowska, B. Hecht, and T. Brixner, “Investigation of the nonlinear refractive index of single-crystalline thin gold films and plasmonic nanostructures,” Appl. Phys. B 122, 1–10 (2016).
[Crossref]

M. Pawłowska, S. Goetz, C. Dreher, M. Wurdack, E. Krauss, G. Razinskas, P. Geisler, B. Hecht, and T. Brixner, “Shaping and spatiotemporal characterization of sub-10-fs pulses focused by a high-NA objective,” Opt. Express 22, 31496–31510 (2014).
[Crossref]

Yang, M.

Z. Guo, Y. Wan, M. Yang, J. Snaider, K. Zhu, and L. Huang, “Long-range hot-carrier transport in hybrid perovskites visualized by ultrafast microscopy,” Science 356, 59–62 (2017).
[Crossref] [PubMed]

Zanni, M.

P. Hamm and M. Zanni, Concepts and Methods of 2D Infrared Spectroscopy (Cambridge University, 2011), 1st ed.
[Crossref]

Zanni, M. T.

J. S. Ostrander, R. Knepper, A. S. Tappan, J. J. Kay, M. T. Zanni, and D. A. Farrow, “Energy transfer between coherently delocalized states in thin films of the explosive pentaerythritol tetranitrate (PETN) revealed by two-dimensional infrared spectroscopy,” J. Phys. Chem. B 121, 1352–1361 (2017).
[Crossref] [PubMed]

T. A. Oudenhoven, Y. Joo, J. E. Laaser, P. Gopalan, and M. T. Zanni, “Dye aggregation identified by vibrational coupling using 2D IR spectroscopy,” J. Chem. Phys. 142, 212449 (2015).
[Crossref] [PubMed]

R. D. Mehlenbacher, T. J. McDonough, M. Grechko, M.-Y. Wu, M. S. Arnold, and M. T. Zanni, “Energy transfer pathways in semiconducting carbon nanotubes revealed using two-dimensional white-light spectroscopy,” Nat. Commun. 6, 6732 (2015).
[Crossref] [PubMed]

S.-H. Shim and M. T. Zanni, “How to turn your pump–probe instrument into a multidimensional spectrometer: 2D IR and VIS spectroscopies via pulse shaping,” Phys. Chem. Chem. Phys. 11, 748–761 (2009).
[Crossref] [PubMed]

Zhu, K.

Z. Guo, Y. Wan, M. Yang, J. Snaider, K. Zhu, and L. Huang, “Long-range hot-carrier transport in hybrid perovskites visualized by ultrafast microscopy,” Science 356, 59–62 (2017).
[Crossref] [PubMed]

Zigler, D. F.

M. M. Gabriel, E. M. Grumstrup, J. R. Kirschbrown, C. W. Pinion, J. D. Christesen, D. F. Zigler, E. E. M. Cating, J. F. Cahoon, and J. M. Papanikolas, “Imaging charge separation and carrier recombination in nanowire p-i-n junctions using ultrafast microscopy,” Nano Lett. 14, 3079–3087 (2014).
[Crossref] [PubMed]

Adv. Funct. Mater. (1)

M. Brendel, S. Krause, A. Steindamm, A. K. Topczak, S. Sundarraj, P. Erk, S. Höhla, N. Fruehauf, N. Koch, and J. Pflaum, “The effect of gradual fluorination on the properties of FnZnPc thin films and FnZnPc/C60 bilayer photovoltaic cells,” Adv. Funct. Mater. 25, 1565–1573 (2015).
[Crossref]

Adv. Mater. (1)

J. Cabanillas-Gonzalez, G. Grancini, and G. Lanzani, “Pump-probe spectroscopy in organic semiconductors: monitoring fundamental processes of relevance in optoelectronics,” Adv. Mater. 23, 5468–5485 (2011).
[Crossref] [PubMed]

Adv. Phys. X (1)

G. Moody and S. T. Cundiff, “Advances in multi-dimensional coherent spectroscopy of semiconductor nanostructures,” Adv. Phys. X 2, 641–674 (2017).
[PubMed]

Annu. Rev. Phys. Chem. (1)

F. D. Fuller and J. P. Ogilvie, “Experimental implementations of two-dimensional Fourier transform electronic spectroscopy,” Annu. Rev. Phys. Chem. 66, 667–690 (2015).
[Crossref] [PubMed]

Appl. Phys. B (1)

S. Goetz, G. Razinskas, E. Krauss, C. Dreher, M. Wurdack, P. Geisler, M. Pawłowska, B. Hecht, and T. Brixner, “Investigation of the nonlinear refractive index of single-crystalline thin gold films and plasmonic nanostructures,” Appl. Phys. B 122, 1–10 (2016).
[Crossref]

J. Appl. Phys. (1)

G. Nardin, T. M. Autry, G. Moody, R. Singh, H. Li, and S. T. Cundiff, “Multi-dimensional coherent optical spectroscopy of semiconductor nanostructures: Collinear and non-collinear approaches,” J. Appl. Phys. 117, 112804 (2015).
[Crossref]

J. Chem. Phys. (4)

T. A. Oudenhoven, Y. Joo, J. E. Laaser, P. Gopalan, and M. T. Zanni, “Dye aggregation identified by vibrational coupling using 2D IR spectroscopy,” J. Chem. Phys. 142, 212449 (2015).
[Crossref] [PubMed]

P. F. Tekavec, G. A. Lott, and A. H. Marcus, “Fluorescence-detected two-dimensional electronic coherence spectroscopy by acousto-optic phase modulation,” J. Chem. Phys. 127, 214307 (2007).
[Crossref] [PubMed]

A. K. De, D. Monahan, J. M. Dawlaty, and G. R. Fleming, “Two-dimensional fluorescence-detected coherent spectroscopy with absolute phasing by confocal imaging of a dynamic grating and 27-step phase-cycling,” J. Chem. Phys. 140, 194201 (2014).
[Crossref] [PubMed]

H.-S. Tan, “Theory and phase-cycling scheme selection principles of collinear phase coherent multi-dimensional optical spectroscopy,” J. Chem. Phys. 129, 124501 (2008).
[Crossref] [PubMed]

J. Phys. Chem. A (1)

C. Y. Wong and G. D. Scholes, “Biexcitonic fine structure of CdSe nanocrystals probed by polarization-dependent two-dimensional photon echo spectroscopy,” J. Phys. Chem. A 115, 3797–3806 (2011).
[Crossref]

J. Phys. Chem. B (1)

J. S. Ostrander, R. Knepper, A. S. Tappan, J. J. Kay, M. T. Zanni, and D. A. Farrow, “Energy transfer between coherently delocalized states in thin films of the explosive pentaerythritol tetranitrate (PETN) revealed by two-dimensional infrared spectroscopy,” J. Phys. Chem. B 121, 1352–1361 (2017).
[Crossref] [PubMed]

J. Phys.: Condens. Matter (1)

W. Langbein and B. Patton, “Transient coherent nonlinear spectroscopy of single quantum dots,” J. Phys.: Condens. Matter 19, 295203 (2007).

Nano Lett. (2)

M. M. Gabriel, E. M. Grumstrup, J. R. Kirschbrown, C. W. Pinion, J. D. Christesen, D. F. Zigler, E. E. M. Cating, J. F. Cahoon, and J. M. Papanikolas, “Imaging charge separation and carrier recombination in nanowire p-i-n junctions using ultrafast microscopy,” Nano Lett. 14, 3079–3087 (2014).
[Crossref] [PubMed]

R. Ciesielski, A. Comin, M. Handloser, K. Donkers, G. Piredda, A. Lombardo, A. C. Ferrari, and A. Hartschuh, “Graphene near-degenerate four-wave mixing for phase characterization of broadband pulses in ultrafast microscopy,” Nano Lett. 15, 4968–4972 (2015).
[Crossref] [PubMed]

Nat. Commun. (5)

E. Wientjes, J. Renger, A. G. Curto, R. Cogdell, and N. F. v. Hulst, “Strong antenna-enhanced fluorescence of a single light-harvesting complex shows photon antibunching,” Nat. Commun. 5, 4236 (2014).
[Crossref] [PubMed]

C. Y. Wong, B. L. Cotts, H. Wu, and N. S. Ginsberg, “Exciton dynamics reveal aggregates with intermolecular order at hidden interfaces in solution-cast organic semiconducting films,” Nat. Commun. 6, 6946 (2015).
[Crossref]

K. J. Karki, J. R. Widom, J. Seibt, I. Moody, M. C. Lonergan, T. Pullerits, and A. H. Marcus, “Coherent two-dimensional photocurrent spectroscopy in a PbS quantum dot photocell,” Nat. Commun. 5, 5869 (2014).
[Crossref] [PubMed]

A. D. Sio, F. Troiani, M. Maiuri, J. Réhault, E. Sommer, J. Lim, S. F. Huelga, M. B. Plenio, C. A. Rozzi, G. Cerullo, E. Molinari, and C. Lienau, “Tracking the coherent generation of polaron pairs in conjugated polymers,” Nat. Commun. 7, 13742 (2016).
[Crossref] [PubMed]

R. D. Mehlenbacher, T. J. McDonough, M. Grechko, M.-Y. Wu, M. S. Arnold, and M. T. Zanni, “Energy transfer pathways in semiconducting carbon nanotubes revealed using two-dimensional white-light spectroscopy,” Nat. Commun. 6, 6732 (2015).
[Crossref] [PubMed]

Nat. Photonics (2)

M. Aeschlimann, T. Brixner, D. Differt, U. Heinzmann, M. Hensen, C. Kramer, F. Lükermann, P. Melchior, W. Pfeiffer, M. Piecuch, C. Schneider, H. Stiebig, C. Strüber, and P. Thielen, “Perfect absorption in nanotextured thin films via Anderson-localized photon modes,” Nat. Photonics 9, 663–668 (2015).
[Crossref]

J. Kasprzak, B. Patton, V. Savona, and W. Langbein, “Coherent coupling between distant excitons revealed by two-dimensional nonlinear hyperspectral imaging,” Nat. Photonics 5, 57–63 (2011).
[Crossref]

Nat. Phys. (2)

R. Hildner, D. Brinks, and N. F. v. Hulst, “Femtosecond coherence and quantum control of single molecules at room temperature,” Nat. Phys. 7, 172–177 (2011).
[Crossref]

V. M. Huxter, T. a. A. Oliver, D. Budker, and G. R. Fleming, “Vibrational and electronic dynamics of nitrogen-vacancy centres in diamond revealed by two-dimensional ultrafast spectroscopy,” Nat. Phys. 9, 744–749 (2013).
[Crossref]

Nature (3)

T. Brixner, J. Stenger, H. M. Vaswani, M. Cho, R. E. Blankenship, and G. R. Fleming, “Two-dimensional spectroscopy of electronic couplings in photosynthesis,” Nature 434, 625–628 (2005).
[Crossref] [PubMed]

G. S. Engel, T. R. Calhoun, E. L. Read, T.-K. Ahn, T. Mančal, Y.-C. Cheng, R. E. Blankenship, and G. R. Fleming, “Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems,” Nature 446, 782–786 (2007).
[Crossref] [PubMed]

D. Brinks, F. D. Stefani, F. Kulzer, R. Hildner, T. H. Taminiau, Y. Avlasevich, K. Mullen, and N. F. van Hulst, “Visualizing and controlling vibrational wave packets of single molecules,” Nature 465, 905–908 (2010).
[Crossref] [PubMed]

Opt. Express (7)

Phys. Chem. Chem. Phys. (1)

S.-H. Shim and M. T. Zanni, “How to turn your pump–probe instrument into a multidimensional spectrometer: 2D IR and VIS spectroscopies via pulse shaping,” Phys. Chem. Chem. Phys. 11, 748–761 (2009).
[Crossref] [PubMed]

Phys. Rev. Applied (1)

C. Rewitz, G. Razinskas, P. Geisler, E. Krauss, S. Goetz, M. Pawłowska, B. Hecht, and T. Brixner, “Coherent control of plasmon propagation in a nanocircuit,” Phys. Rev. Applied 1, 014007 (2014).
[Crossref]

Phys. Rev. B (3)

G. Moody, M. E. Siemens, A. D. Bristow, X. Dai, D. Karaiskaj, A. S. Bracker, D. Gammon, and S. T. Cundiff, “Exciton-exciton and exciton-phonon interactions in an interfacial GaAs quantum dot ensemble,” Phys. Rev. B 83, 115324 (2011).
[Crossref]

J. Bylsma, P. Dey, J. Paul, S. Hoogland, E. H. Sargent, J. M. Luther, M. C. Beard, and D. Karaiskaj, “Quantum beats due to excitonic ground-state splitting in colloidal quantum dots,” Phys. Rev. B 86, 125322 (2012).
[Crossref]

G. Moody, R. Singh, H. Li, I. A. Akimov, M. Bayer, D. Reuter, A. D. Wieck, and S. T. Cundiff, “Fifth-order nonlinear optical response of excitonic states in an InAs quantum dot ensemble measured with two-dimensional spectroscopy,” Phys. Rev. B 87, 045313 (2013).
[Crossref]

Phys. Rev. Lett. (1)

P. Geisler, G. Razinskas, E. Krauss, X.-F. Wu, C. Rewitz, P. Tuchscherer, S. Goetz, C.-B. Huang, T. Brixner, and B. Hecht, “Multimode plasmon excitation and in situ analysis in top-down fabricated nanocircuits,” Phys. Rev. Lett. 111, 183901 (2013).
[Crossref] [PubMed]

Sci. Rep. (1)

E. Vella, H. Li, P. Grégoire, S. M. Tuladhar, M. S. Vezie, S. Few, C. M. Bazán, J. Nelson, C. Silva-Acuña, and E. R. Bittner, “Ultrafast decoherence dynamics govern photocarrier generation efficiencies in polymer solar cells,” Sci. Rep. 6, 29437 (2016).
[Crossref] [PubMed]

Science (5)

Z. Guo, Y. Wan, M. Yang, J. Snaider, K. Zhu, and L. Huang, “Long-range hot-carrier transport in hybrid perovskites visualized by ultrafast microscopy,” Science 356, 59–62 (2017).
[Crossref] [PubMed]

R. Hildner, D. Brinks, J. B. Nieder, R. J. Cogdell, and N. F. v. Hulst, “Quantum Coherent Energy Transfer over Varying Pathways in Single Light-Harvesting Complexes,” Science 340, 1448–1451 (2013).
[Crossref] [PubMed]

M. Aeschlimann, T. Brixner, A. Fischer, C. Kramer, P. Melchior, W. Pfeiffer, C. Schneider, C. Strüber, P. Tuchscherer, and D. V. Voronine, “Coherent two-dimensional nanoscopy,” Science 333, 1723–1726 (2011).
[Crossref] [PubMed]

P. Tian, D. Keusters, Y. Suzaki, and W. S. Warren, “Femtosecond phase-coherent two-dimensional spectroscopy,” Science 300, 1553–1555 (2003).
[Crossref] [PubMed]

K. W. Stone, K. Gundogdu, D. B. Turner, X. Li, S. T. Cundiff, and K. A. Nelson, “Two-quantum 2D FT electronic spectroscopy of biexcitons in GaAs quantum wells,” Science 324, 1169–1173 (2009).
[Crossref] [PubMed]

Other (3)

S. Roeding and T. Brixner, “Multidimensional electronic spectroscopy in molecular beams with mass-resolved ion detection,” in “International Conference on Ultrafast Phenomena XX,” (Optical Society of America, 2016), p. UM3A.2.

P. Hamm and M. Zanni, Concepts and Methods of 2D Infrared Spectroscopy (Cambridge University, 2011), 1st ed.
[Crossref]

L. Novotny and B. Hecht, Principles of Nano-Optics (Cambridge University Press, Cambridge, 2006).
[Crossref]

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Figures (5)

Fig. 1
Fig. 1 Experimental basics. (a) Overview of setup for 2D fluorescence micro-spectroscopy. Chirped mirrors and a spatial light modulator are used for temporal pulse compression, the latter additionally for generation of pulse sequences. The laser spectrum is confined by longpass (LP) and shortpass (SP) apertures in front of the liquid-crystal display (LCD) and by a Schott KG5 color filter in front of the dichroic beam splitter (DBS). Excitation of the sample and collection of the fluorescence is conducted by a high-numerical-aperture (NA) microscope objective. Separated from scattered light by an additional LP filter, the fluorescence is detected either by an avalanche photodiode (APD) or a spectrometer. (b) Laser spectrum measured after reflection from the DBS. (c) Collinear interferometric autocorrelation (blue) recorded by placing a two-photon photodiode at the sample position. From the Fourier-filtered curve (red), the duration of a single pulse is determined to be 12.1 fs (FWHM). (d) Four-pulse sequence. The inter-pulse delays are defined by τ, T and t. Each pulse has an adjustable phase Φi (i = 1, . . ., 4).
Fig. 2
Fig. 2 Microscopic characterization of the in-plane structured F16ZnPc pillar array. (a) Reflection intensity map, showing low reflectivity in regions where the regular hexagonal pattern is perturbed. (b) Fluorescence map of the same area as in (a). The regions of low reflectivity show the highest fluorescence yield due to the thick chromophore layer coverage. (c) AFM map from a homogeneously structured region of the same sample (but not necessarily the same area), indicating the defects in the lateral pattern of chromophore pillars. Scalebar 1000 nm.
Fig. 3
Fig. 3 (a) Absorption of a nanostructured (red) and a homogeneous (black) F16ZnPc thin film in comparison to the laser spectrum (blue). (b) Excitation-power-dependent fluorescence of the F16ZnPc nanopillar array, showing an onset of the non-linear response above approximately 1 GW/cm2 peak excitation intensity, deviating from the linear trend (black line). Each color corresponds to an individual measurement with a different set of neutral density filters where a half-waveplate is rotated in front of a linear polarizer to scan the attenuation.
Fig. 4
Fig. 4 Zero-padded rephasing (upper row) and non-rephasing (lower row) 2D spectra before the final processing step. The high-power measurements (a,b) contain the expected nonlinear signals in the lower right (a) and lower left (b) quadrants. Additional artifacts occur in other positions. For low-power measurements (c,d), only the linear artifacts remain, allowing for an artifact correction. The correction is done by subtracting the measured low-power from the high-power maps in the time domain (not shown). The corrected 2D maps are then retrieved by Fourier transformation, from which the absolute values are shown (e,f).
Fig. 5
Fig. 5 Final 2D spectrum of a hotspot in the nanostructured F16ZnPc pillar array. The complex-valued maps are shown for the rephasing (a) real and (b) imaginary part as well as the non-rephasing (d) real and (e) imaginary part. The real-valued maps are added to obtain (e) the absorptive spectrum. (f) Projection of the 2D absorptive spectrum onto the ωt axis (black) compared to a separately measured Fourier-transformed linear two-pulse scan (red).

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