Communication: The origin of many-particle signals in nonlinear optical spectroscopy of non-interacting particles

Journal Article · Fri Jul 29 00:00:00 EDT 2016 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4960049· OSTI ID:1467860

Mukamel, Shaul ^[1]

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1. Univ. of California, Irvine, CA (United States). Dept. of Chemistry and Dept. of Physics and Astronomy

Nonlinear spectroscopy signals detected by fluorescence from dilute samples of N non-interacting molecules are usually adequately described by simply multiplying the single molecule response by N. Here, we show that signals that scale with higher powers of N are generated by the joint detection of several particles. This can be accomplished by phase sensitive detection such as phase cycling, photo-acoustic modulation, or by Hanbury-Brown Twiss photon coincidence. Such measurements can dissect the ensemble according to the number of excited particles.

• Research Organization: Univ. of California, Irvine, CA (United States)
• Sponsoring Organization: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; National Science Foundation (NSF)
• Grant/Contract Number: FG02-04ER15571; CHE-1361516
• OSTI ID: 1467860
• Alternate ID(s): OSTI ID: 1275975
• Journal Information: Journal of Chemical Physics, Vol. 145, Issue 4; ISSN 0021-9606
• Publisher: American Institute of Physics (AIP)
• Country of Publication: United States
• Language: English

Related Subjects

71 CLASSICAL AND QUANTUM MECHANICS
GENERAL PHYSICS
74 ATOMIC AND MOLECULAR PHYSICS
nonlinear optics
fluorescence
excited states
photons
optical coherence
fourier transforms
signal coherence
single molecule techniques
nonlinear spectroscopy
quantum coherence