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/content/aip/journal/jcp/145/4/10.1063/1.4960049
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/content/aip/journal/jcp/145/4/10.1063/1.4960049
2016-07-29
2016-12-05

Abstract

Nonlinear spectroscopy signals detected by fluorescence from dilute samples of non-interacting molecules are usually adequately described by simply multiplying the single molecule response by . 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.

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