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Direct determination of multiphoton absorption cross-sections by transient absorption spectroscopy.

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Researchers developed a new method to measure light absorption in materials. This technique accurately quantifies single- to multi-photon absorption cross-sections, crucial for advanced imaging and photon-harvesting materials.

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Area of Science:

  • Materials Science
  • Optics
  • Photochemistry

Background:

  • Single- and multi-photon absorption cross-sections are key for light-matter interactions in spectroscopy, photochemistry, and advanced imaging.
  • Conventional measurement methods face limitations due to sample properties, concentration, and high excitation intensities, impacting reliability and sample integrity.

Purpose of the Study:

  • To present a direct, robust, and versatile method for quantifying absorption cross-sections across single- to multi-photon regimes.
  • To report novel three-photon and four-photon absorption cross-sections for CsPbI3 perovskite nanocrystals and CdSe/ZnS quantum dots.
  • To establish a generalizable tool for discovering and optimizing photon-harvesting materials.

Main Methods:

  • Developed a method based on the saturation behavior of transient absorption signals.
  • Applied the method to measure three- and four-photon absorption cross-sections using 1700 nm and 2100 nm excitation.
  • Validated the method's applicability to weakly or non-emissive materials.

Main Results:

  • Reported the first measurements of three- and four-photon absorption cross-sections for CsPbI3 perovskite nanocrystals and CdSe/ZnS quantum dots.
  • Demonstrated that these materials exhibit absorption cross-sections at least an order of magnitude higher than incumbent materials for mouse deep-brain imaging.
  • Showcased the method's independence from photoluminescence signals.

Conclusions:

  • The developed method offers a reliable and versatile approach to quantify absorption cross-sections.
  • CsPbI3 perovskite nanocrystals and CdSe/ZnS quantum dots show significant potential for advanced imaging and photon-harvesting applications.
  • This work provides a valuable tool for accelerating the development of next-generation optical materials.