No Arabic abstract
A theory of correlations between N photons of given frequencies and detected at given time delays is presented. These correlation functions are usually too cumbersome to be computed explicitly. We show that they are obtained exactly through intensity correlations between two-level sensors in the limit of their vanishing coupling to the system. This allows the computation of correlation functions hitherto unreachable. The uncertainties in time and frequency of the detection, which are necessary variables to describe the system, are intrinsic to the theory. We illustrate the formalism with the Jaynes--Cummings model, showing how correlations of various peaks at zero or finite time delays bring new insights into the dynamics of open quantum systems.
While two-photon absorption (TPA) and other forms of nonlinear interactions of molecules with isolated time-frequency-entangled photon pairs (EPP) have been predicted to display a variety of fascinating effects, their potential use in practical quantum-enhanced molecular spectroscopy requires close examination. This paper presents a detailed theoretical study of quantum-enhanced TPA by both photon-number correlations and spectral correlations, including an account of the deleterious effects of dispersion. While such correlations in EPP created by spontaneous parametric down conversion can increase the TPA rate significantly in the regime of extremely low optical flux, we find that for typical molecules in solution this regime corresponds to such low TPA event rates as to be unobservable in practice. Our results support the usefulness of EPP spectroscopy in atomic or other narrow-linewidth systems, while questioning the efficacy of such approaches for broadband systems including molecules in solution.
Pairs of photons entangled in their time-frequency degree of freedom are of great interest in quantum optics research and applications, due to their relative ease of generation and their high capacity for encoding information. Here we analyze, both theoretically and experimentally, the behavior of phase-insensitive spectrally-resolved interferences arising from two pairs of time-frequency entangled photons. At its core, this is a multimode entanglement swapping experiment, whereby a spectrally resolved joint measurement on the idler photons from both pairs results in projecting the signal photons onto a Bell state whose form depends on the measurement outcome. Our analysis is a thorough exploration of what can be achieved using time-frequency entanglement and spectrally-resolved Bell-state measurements.
We develop an ultrafast frequency-resolved Raman spectroscopy with entangled photons for polyatomic molecules in condensed phases, to probe the electronic and vibrational coherences. Using quantum correlation between the photons, the signal shows the capability of both temporal and spectral resolutions that are not accessible by either classical pulses or the fields without entanglement. We develop a microscopic theory for this Raman spectroscopy, revealing the electronic coherence dynamics which often shows a rapid decay within $sim$50fs. The heterodyne-detected Raman signal is further developed to capture the phases of electronic coherence and emission in real-time domain.
At the dawn of Quantum Physics, Wigner and Weisskopf obtained a full analytical description (a textit{photon portrait}) of the emission of a single photon by a two-level system, using the basis of frequency modes (Weisskopf and Wigner, Zeitschrift fur Physik, 63, 1930). A direct experimental reconstruction of this portrait demands an accurate measurement of a time resolved fluorescence spectrum, with high sensitivity to the off-resonant frequencies and ultrafast dynamics describing the photon creation. In this work we demonstrate such an experimental technique in a superconducting waveguide Quantum Electrodynamics (wQED) platform, using single transmon qubit and two coupled transmon qubits as quantum emitters. In both scenarios, the photon portraits agree quantitatively with the predictions of the input-output theory and qualitatively with Wigner-Weisskopf theory. We believe that our technique allows not only for interesting visualization of fundamental principles, but may serve as a tool, e.g. to realize multi-dimensional spectroscopy in waveguide Quantum Electrodynamics.
An accurate description of spatial variations in the energy levels of patterned semiconductor substrates on the micron and sub-micron scale as a function of local doping is an important technological challenge for the microelectronics industry. Spatially resolved surface analysis by photoelectron spectromicroscopy can provide an invaluable contribution thanks to the relatively non-destructive, quantitative analysis. We present results on highly doped n and p type patterns on, respectively, p and n type silicon substrates. Using synchrotron radiation and spherical aberration-corrected energy filtering, we have obtained a spectroscopic image series at the Si 2p core level and across the valence band. Local band alignments are extracted, accounting for doping, band bending and surface photovoltage.