Entangled photon assisted multidimensional nonlinear optics of exciton–polaritons

Abstract

We present a theoretical formulation of the frequency domain multidimensional pump-probe analog spectroscopy, which utilizes the spectral-temporal entanglement features of the biphoton sources. It has been shown, via a compact multi-time, convolutional Green's function expression and the accompanying numerical simulations, that utilizing the correlation properties of non-classical sources offers a viable scheme for the exploration of dissipative kinetics of the cavity confined quantum aggregates. The cooperative and competitive modifications brought in by the photonic cavity mode and the auxiliary vibrational modes into the scattering and dephasing properties of the excitonpolaritons have been explored via their signatures in the multidimensional correlation maps. The study offers a new parameter window for the investigation of the dynamical polariton characteristics and warrants the usage of multi-mode entanglement properties of the external photonic sources in future studies.

Generalization of the Tavis–Cummings model for multi-level anharmonic systems

“…The eigenfrequencies are tabulated in table II, while the matrix elements of transition operators between the eigenstates in the first excitation manifold and those in eqs. (44) to (46) are included in tables III to VI. The analytical expressions for the solutions with arbitrary N can be found in Appendix A.…”

“…Indeed, consideration of more realistic vibrational SC systems involving anharmonicities has been the subject of theoretical explorations, such as the use of single-molecule models to explain cavity-induced modifications to chemical reactivity, [33][34][35][36][37] as well as the use of many-molecule models a) Electronic mail: joelyuen@ucsd.edu; http://yuenzhougroup.ucsd.edu to explain non-linear response experiments. 28,[38][39][40][41][42][43] In particular, recent work [44][45][46][47][48][49] has elucidated novel multiphoton absorption phenomena where the TC description is insufficient, and a multilevel anharmonic spectrum of the material is essential. These effects go beyond vibrational SC and should have analogues in other electromagnetic ranges, such as those systems under electronic SC where more than two electronic states per quantum emitter must be considered.…”

Polarization-Entangled Two-Photon Absorption in Inhomogeneously Broadened Ensembles

“…Entangled photons have been identified as promising new tools for spectroscopic or imaging applications [1][2][3][4][5][6][7]. Their strong quantum correlations could circumvent certain classical Fourier uncertainties and thus enhance the sensing capabilities of optical measurements [8][9][10][11][12][13][14][15][16]. The detection of quantum correlations could also provide new spectroscopic information [17][18][19][20][21][22][23][24][25], and the use of quantum light in interferometric setups promises additional control knobs to analyze spectroscopic information [26][27][28][29] as well as access to out-of-time correlations [30].…”

Entangled biphoton enhanced double quantum coherence signal as a probe for cavity polariton correlations in presence of phonon induced dephasing

“…Hence, combining these two developments to the case of light-harvesting quantum aggregates offers an opportunity to investigate the role of the cavity in controlling a prototypical, extended yet aperiodic system that hosts collective excitons. Previous spectroscopic studies of the cavity-modulated dynamics [29][30][31][32][33][34][35] have increasingly focused their attention on the ultrafast, nonlinear techniques analogs e.g. pump-probe.…”

“…In comparison to the shaped laser pulses, the entangled biphotons have been shown to improve the spectral resolution while scaling favorably with the intensity of the sources. The nonclassical correlation properties can also be utilized to obtain favorable spectral-temporal resolution in the probing via selective state projections of the nonlinear polarization [29,33,[48][49][50][51][52][53][54][55]. The latter requires the selection of a few states whose correlation properties are of particular interest from a manifold.…”