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Monitoring Spontaneous Charge-Density Fluctuations by Single-Molecule Diffraction of Quantum Light.

  • Author(s): Dorfman, Konstantin E;
  • Asban, Shahaf;
  • Ye, Lyuzhou;
  • Rouxel, Jérémy R;
  • Cho, Daeheum;
  • Mukamel, Shaul
  • et al.
Abstract

Homodyne X-ray diffraction signals produced by classical light and classical detectors are given by the modulus square of the charge density in momentum space |σ(q)|2, missing its phase, which is required in order to invert the signal to real space. We show that quantum detection of the radiation field yields a linear diffraction pattern that reveals σ(q) itself, including the phase. We further show that repeated diffraction measurements with variable delays constitute a novel multidimensional measure of spontaneous charge-density fluctuations. Classical diffraction, in contrast, only reveals a subclass of even-order correlation functions. Simulations of two-dimensional signals obtained by two diffraction events are presented for the amino acid cysteine.

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