Multidimensional pump-probe spectroscopy with entangled twin-photon states

Abstract

We show that entangled photons may be used in coherent multidimensional nonlinear spectroscopy to provide information on matter by scanning photon wave function parameters (entanglement time and delay of twin photons), rather than frequencies and time delays, as is commonly done with classical pulses. Signals are expressed and interpreted intuitively in terms of products of matter and field correlation functions using a diagrammatic close time path loop formalism which reveals the entangled quantum pathways of the fields and matter. The pumpprobe signal measured when the pump and the probe are in a twin entangled state shows twophoton resonant contributions which scale linearly rather than quadratically with the incident beam intensity and reveal frequencies of off-resonant transitions. Two-dimensional spectrograms obtained by double Fourier transform of the signal with respect to the entanglement time and delay of the twins could provide detailed information on correlations among states and dynamical processes with high temporal resolution. The analogy with multidimensional time-domain optical techniques which use sequences of short classical pulses and pulse shaping algorithms is pointed out.

Photon statistics of intense entangled photon pulses

“…Applications to spectroscopy received considerable attention in experiments [6][7][8][9] as well as in theoretical works [10][11][12][13][14][15][16]. These prospects necessitate the adaption of quantum information concepts to spectroscopic applications.…”

Multidimensional coherent optical spectroscopy of semiconductor nanostructures: a review

“…The use of entangled photons in MDCS has also been theoretically discussed, and promises to be a sensitive and selective way to probe coherences between transitions, beyond what is possible with classical light [113,114,115,116].…”

Two-photon spectroscopy of excitons with entangled photons

“…This favorable intensity scaling [15][16][17][18] has been demonstrated experimentally in various systems, and allows to perform measurements at low intensities, avoiding damage to the sample. Moreover, the non-classical time-bandwidth properties of entangled photon pairs [19][20][21] provide unconventional observation windows, and can be used to selectively excite specific two-exciton states 21 or specific vibrational states, 22,23 and control population transport. 24 New control parameters of quantum light can be varied to create novel twodimensional correlation plots.…”