Nonlinear Optics Approaches Towards Subdiffraction Resolution in CARS Imaging

Klaus-Jochen Boller, Willem P. Beeker, Carsten Cleff, Kai Kruse, Chris J. Lee, Petra Gross, Herman L. Offerhaus, Carsten Fallnich, Jennifer Lynn Herek

Research output: Chapter in Book/Report/Conference proceedingChapterAcademicpeer-review

3 Citations (Scopus)

Abstract

In theoretical investigations, we review several nonlinear optical approaches towards subdiffraction-limited resolution in label-free imaging via coherent anti-Stokes Raman scattering (CARS). Using a density matrix model and numerical integration, we investigate various level schemes and combinations of the light fields that induce CARS along with additional control laser fields. As the key to techniques that gain far-field resolution below the diffraction limit, we identify the inhibition of the buildup of vibrational molecular coherence via saturation or depletion of population (Beeker et al. Opt Express 17:22632–22638, 2009) or the generation of Stark broadening and spatially dependent Rabi sideband generation (Beeker et al. Phys Rev A 81(1), 2010). Depending on the coherence and population decay rates offered by a particular molecular energy level scheme, we identify various different regimes. In the first case, where an additional state (called the control state) and a vibrational state are able to rapidly exchange population via incoherent processes, a prepopulation of the upper vibrational state inhibits the buildup of vibrational coherence. With increasing control laser intensity, this suppresses CARS emission via an incoherent, saturation type of nonlinear process. Using an intense, donut-shaped control laser beam, similar to stimulated emission depletion (STED) microscopy, this can suppress CARS emission from all sample locations except within a subdiffraction-sized range around the central node. Scanning the control beams across the sample provides subdiffraction-limited resolution imaging. An alternative, which does not require a rapid exchange of population with the control state, applies a control beam that only partially depletes the vibrational ground state. Thereby, a CARS point spread function containing a subdiffraction-limited component is generated. Subdiffraction images can then be retrieved through deconvolution. Further approaches are based on the coherent, nonlinear, resonant response of the sample. In this case, CARS signal depletion by Stark splitting of the weakly populated upper vibrational state or the observation of spatially dependent Rabi oscillation may increase the resolution beyond the diffraction limit.
Original languageEnglish
Title of host publicationSuper-Resolution Microscopy Techniques in the Neurosciences
EditorsEugenio F. Fornasiero, Silvio O. Rizzoli
Place of PublicationTotowa, NJ
PublisherHumana Press
Pages291-324
Number of pages391
ISBN (Electronic)978-1-62703-983-3
ISBN (Print)978-1-62703-982-6
DOIs
Publication statusPublished - 2014

Publication series

NameNeuromethod
PublisherHumana Press by Springer
Volume86

Fingerprint

nonlinear optics
Raman spectra
vibrational states
depletion
molecular energy levels
saturation
point spread functions
stimulated emission
numerical integration
sidebands
diffraction
decay rates
lasers
far fields
laser beams
microscopy
oscillations
scanning
ground state

Keywords

  • Nonlinear polarizability
  • Stimulated Raman
  • Multiphoton numerical modeling
  • Subdiffraction imaging
  • Coherent anti-Stokes Raman (CARS)

Cite this

Boller, K-J., Beeker, W. P., Cleff, C., Kruse, K., Lee, C. J., Gross, P., ... Herek, J. L. (2014). Nonlinear Optics Approaches Towards Subdiffraction Resolution in CARS Imaging. In E. F. Fornasiero, & S. O. Rizzoli (Eds.), Super-Resolution Microscopy Techniques in the Neurosciences (pp. 291-324). (Neuromethod; Vol. 86). Totowa, NJ: Humana Press. https://doi.org/10.1007/978-1-62703-983-3_12
Boller, Klaus-Jochen ; Beeker, Willem P. ; Cleff, Carsten ; Kruse, Kai ; Lee, Chris J. ; Gross, Petra ; Offerhaus, Herman L. ; Fallnich, Carsten ; Herek, Jennifer Lynn. / Nonlinear Optics Approaches Towards Subdiffraction Resolution in CARS Imaging. Super-Resolution Microscopy Techniques in the Neurosciences. editor / Eugenio F. Fornasiero ; Silvio O. Rizzoli. Totowa, NJ : Humana Press, 2014. pp. 291-324 (Neuromethod).
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keywords = "Nonlinear polarizability, Stimulated Raman, Multiphoton numerical modeling, Subdiffraction imaging, Coherent anti-Stokes Raman (CARS)",
author = "Klaus-Jochen Boller and Beeker, {Willem P.} and Carsten Cleff and Kai Kruse and Lee, {Chris J.} and Petra Gross and Offerhaus, {Herman L.} and Carsten Fallnich and Herek, {Jennifer Lynn}",
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Boller, K-J, Beeker, WP, Cleff, C, Kruse, K, Lee, CJ, Gross, P, Offerhaus, HL, Fallnich, C & Herek, JL 2014, Nonlinear Optics Approaches Towards Subdiffraction Resolution in CARS Imaging. in EF Fornasiero & SO Rizzoli (eds), Super-Resolution Microscopy Techniques in the Neurosciences. Neuromethod, vol. 86, Humana Press, Totowa, NJ, pp. 291-324. https://doi.org/10.1007/978-1-62703-983-3_12

Nonlinear Optics Approaches Towards Subdiffraction Resolution in CARS Imaging. / Boller, Klaus-Jochen; Beeker, Willem P.; Cleff, Carsten; Kruse, Kai; Lee, Chris J.; Gross, Petra; Offerhaus, Herman L.; Fallnich, Carsten; Herek, Jennifer Lynn.

Super-Resolution Microscopy Techniques in the Neurosciences. ed. / Eugenio F. Fornasiero; Silvio O. Rizzoli. Totowa, NJ : Humana Press, 2014. p. 291-324 (Neuromethod; Vol. 86).

Research output: Chapter in Book/Report/Conference proceedingChapterAcademicpeer-review

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T1 - Nonlinear Optics Approaches Towards Subdiffraction Resolution in CARS Imaging

AU - Boller, Klaus-Jochen

AU - Beeker, Willem P.

AU - Cleff, Carsten

AU - Kruse, Kai

AU - Lee, Chris J.

AU - Gross, Petra

AU - Offerhaus, Herman L.

AU - Fallnich, Carsten

AU - Herek, Jennifer Lynn

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AB - In theoretical investigations, we review several nonlinear optical approaches towards subdiffraction-limited resolution in label-free imaging via coherent anti-Stokes Raman scattering (CARS). Using a density matrix model and numerical integration, we investigate various level schemes and combinations of the light fields that induce CARS along with additional control laser fields. As the key to techniques that gain far-field resolution below the diffraction limit, we identify the inhibition of the buildup of vibrational molecular coherence via saturation or depletion of population (Beeker et al. Opt Express 17:22632–22638, 2009) or the generation of Stark broadening and spatially dependent Rabi sideband generation (Beeker et al. Phys Rev A 81(1), 2010). Depending on the coherence and population decay rates offered by a particular molecular energy level scheme, we identify various different regimes. In the first case, where an additional state (called the control state) and a vibrational state are able to rapidly exchange population via incoherent processes, a prepopulation of the upper vibrational state inhibits the buildup of vibrational coherence. With increasing control laser intensity, this suppresses CARS emission via an incoherent, saturation type of nonlinear process. Using an intense, donut-shaped control laser beam, similar to stimulated emission depletion (STED) microscopy, this can suppress CARS emission from all sample locations except within a subdiffraction-sized range around the central node. Scanning the control beams across the sample provides subdiffraction-limited resolution imaging. An alternative, which does not require a rapid exchange of population with the control state, applies a control beam that only partially depletes the vibrational ground state. Thereby, a CARS point spread function containing a subdiffraction-limited component is generated. Subdiffraction images can then be retrieved through deconvolution. Further approaches are based on the coherent, nonlinear, resonant response of the sample. In this case, CARS signal depletion by Stark splitting of the weakly populated upper vibrational state or the observation of spatially dependent Rabi oscillation may increase the resolution beyond the diffraction limit.

KW - Nonlinear polarizability

KW - Stimulated Raman

KW - Multiphoton numerical modeling

KW - Subdiffraction imaging

KW - Coherent anti-Stokes Raman (CARS)

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EP - 324

BT - Super-Resolution Microscopy Techniques in the Neurosciences

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PB - Humana Press

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Boller K-J, Beeker WP, Cleff C, Kruse K, Lee CJ, Gross P et al. Nonlinear Optics Approaches Towards Subdiffraction Resolution in CARS Imaging. In Fornasiero EF, Rizzoli SO, editors, Super-Resolution Microscopy Techniques in the Neurosciences. Totowa, NJ: Humana Press. 2014. p. 291-324. (Neuromethod). https://doi.org/10.1007/978-1-62703-983-3_12