Abstract

We develop a coherent control theory for multimode quantum light. It allows us to examine a fundamental problem in quantum optics: what is the optimal pulse form to drive a two-photon-transition? In formulating the question as a coherent control problem, we show that—and quantify how much—the strong frequency quantum correlations of entangled photons enhance the transition compared to shaped classical pulses. In ensembles of collectively driven two-level systems, such enhancement requires nonvanishing interactions.

Highlights

  • The nonlinear interaction between faint light and matter on a single atom/molecule and few-photon level is of great fundamental and practical interest: while Gedanken experiments involving single photons and single quantum emitters have recently come within reach of experimental verification [1,2,3], similar applications in single molecule spectroscopy may unravel the quantum dynamics of photo-sensitive materials beyond the ensemble average [4], and promise to elucidate, for instance, the role of fluctuations in energy transport [5, 6]

  • Since the above discussion establishes that entangled photons can enhance the two-photon transition probability when either D 1 0 or d 1 0, we investigate the optimal pulse forms in detail

  • We investigated optimal pulse forms to efficiently drive a resonant two-photon transition with weak fields

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Summary

Introduction

The nonlinear interaction between faint light and matter on a single atom/molecule and few-photon level is of great fundamental and practical interest: while Gedanken experiments involving single photons and single quantum emitters have recently come within reach of experimental verification [1,2,3], similar applications in single molecule spectroscopy may unravel the quantum dynamics of photo-sensitive materials beyond the ensemble average [4], and promise to elucidate, for instance, the role of fluctuations in energy transport [5, 6]. The feeble probe and signal fields in such experiments pose a formidable challenge: in order to detect the typically very weak nonlinear effects at small photon numbers (on the order of one), one seeks to, either, optimize the nonlinearity of the optical medium, or to manipulate the light fields: the former route includes the cavity-enhanced coupling of light to the medium [13,14,15], or the enhancement of the medium’s nonlinearity by additional strong driving fields [7, 8], large dipoles in highly excited Rydberg states [16, 17], or molecular design of target molecules [18, 19] In the latter route, strong focussing of the light beams, i.e. the choice of a suitable geometry, was exploited to detect the nonlinear response on a single molecule level [1,2,3].

F Schlawin and A Buchleitner
Two-photon absorption
Classical versus quantum light
Summary and outlook
Full Text
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