Multidimensional spectroscopy with entangled light; loop vs ladder delay scanning protocols

Multidimensional optical signals are commonly recorded by varying the delays between time ordered pulses. These control the evolution of the density matrix and are described by ladder diagrams. We propose a new non-time-ordered protocol based on following the time evolution of the wavefunction and described by loop diagrams. The time variables in this protocol allow to observe different types of resonances and reveal information about intraband dephasing not readily available by time ordered techniques. The time variables involved in this protocol become coupled when using entangled light, which provides high selectivity and background free measurement of the various resonances. Entangled light can resolve certain states even when strong background due to fast dephasing suppresses the resonant features when probed by classical light

Nonlinear fluctuations and dissipation in matter revealed by quantum light

Quantum optical fields offer numerous control knobs which are not available with classical light and may be used for monitoring the properties of matter by novel types of spectroscopy. It has been recently argued that such quantum spectroscopy signals can be obtained by a simple averaging of their classical spectroscopy counterparts over the Glauber-Sudarshan quasiprobability distribution of the quantum field; the quantum light thus merely provides a novel gating window for the classical response functions. We show that this argument only applies to the linear response and breaks down in the nonlinear regime. The quantum response carries additional valuable information about response and spontaneous fluctuations of matter that may not be retrieved from the classical response by simple data processing. This is connected to the lack of a nonlinear fluctuation-dissipation relation

Efficiency at Maximum Power of Laser Quantum Heat Engine Enhanced by Noise-Induced Coherence

Quantum coherence has been demonstrated in various systems including organic solar cells and solid state devices. In this letter, we report the lower and upper bounds for the performance of quantum heat engines determined by the efficiency at maximum power. Our prediction based on the canonical 3-level Scovil and Schulz-Dubois maser model strongly depends on the ratio of system-bath couplings for the hot and cold baths and recovers the theoretical bounds established previously for the Carnot engine. Further, introducing a 4-th level to the maser model can enhance the maximal power and its efficiency, thus demonstrating the importance of quantum coherence in the thermodynamics and operation of the heat engines beyond the classical limit

Quantum phase-sensitive diffraction and imaging using entangled photons

We propose a novel quantum diffraction imaging technique whereby one photon of an entangled pair is diffracted off a sample and detected in coincidence with its twin. The image is obtained by scanning the photon that did not interact with matter. We show that when a dynamical quantum system interacts with an external field, the phase information is imprinted in the state of the field in a detectable way. The contribution to the signal from photons that interact with the sample scales as $\propto I_{p}^{1/2}$, where $I_{p}$ is the source intensity, compared to $\propto I_{p}$ of classical diffraction. This makes imaging with weak-field possible, avoiding damage to delicate samples. A Schmidt decomposition of the state of the field can be used for image enhancement by reweighting the Schmidt modes contributions.Comment: In pres

Detecting Electronic Coherence by Multidimensional Broadband Stimulated X-Ray Raman Signals

Nonstationary molecular states which contain electronic coherences can be impulsively created and manipulated by using recently-developed ultrashort optical and X-ray pulses via photoexcitation, photoionization and Auger processes. We propose several stimulated-Raman detection schemes that can monitor the phase-sensitive electronic and nuclear dynamics. Three detection protocols of an X-ray broadband probe are compared - frequency dispersed transmission, integrated photon number change, and total pulse energy change. In addition each can be either linear or quadratic in the X-ray probe intensity. These various signals offer different gating windows into the molecular response which is described by correlation functions of electronic polarizabilities. Off-resonant and resonant signals are compared

Nonlinear optical signals and spectroscopy with quantum light

Conventional nonlinear spectroscopy uses classical light to detect matter properties through the variation of its response with frequencies or time delays. Quantum light opens up new avenues for spectroscopy by utilizing parameters of the quantum state of light as novel control knobs and through the variation of photon statistics by coupling to matter. We present an intuitive diagrammatic approach for calculating ultrafast spectroscopy signals induced by quantum light, focusing on applications involving entangled photons with nonclassical bandwidth properties - known as "time-energy entanglement". Nonlinear optical signals induced by quantized light fields are expressed using time ordered multipoint correlation functions of superoperators. These are different from Glauber's g- functions for photon counting which use normally ordered products of ordinary operators. Entangled photon pairs are not subjected to the classical Fourier limitations on the joint temporal and spectral resolution. After a brief survey of properties of entangled photon pairs relevant to their spectroscopic applications, different optical signals, and photon counting setups are discussed and illustrated for simple multi-level model systems

MULTIPLE COMPARISONS WITH THE BEST: BAYESIAN PRECISION MEASURES OF EFFICIENCY RANKINGS

A large literature exists on measuring the allocative and technical efficiency of a set of firms. A segment of this literature uses data envelopment analysis (DEA), creating relative efficiency rankings that are nonstochastic and thus cannot be evaluated according to the precision of the rankings. A parallel literature uses econometric techniques to estimate stochastic production frontiers or distance functions, providing at least the possibility of computing the precision of the resulting efficiency rankings. Recently, Horrace and Schmidt (2000) have applied sampling theoretic statistical techniques known as multiple comparisons with control (MCC) and multiple comparisons with the best (MCB) to the issue of measuring the precision of efficiency rankings. This paper offers a Bayesian multiple comparison alternative that we argue is simpler to implement, gives the researcher increased exibility over the type of comparison made, and provides greater, and more in-tuitive, information content. We demonstrate this method on technical efficiency rankings of a set of U.S. electric generating firms derived within a distance function framework.Research Methods/ Statistical Methods,

Evaluation of optical probe signals from nonequilibrium systems

We predict several effects associated with the optical response of systems prepared in a nonequilibrium state by impulsive optical excitations. The linear response depends on the phase of the electric field even if the initial nonequilirbium state has only populations, no coherences. Initial quantum coherences induce additional phase dependence which also shows new resonances in nonlinear wave mixing. In systems strongly driven by an external optical field, the field frequency generates a phase dependent probe absorption. This gives further control to manipulate the relative contribution to the linear signal due to initial populations and coherences

Time-resolved broadband Raman spectroscopies; A unified six-wave-mixing representation

Excited-state vibrational dynamics in molecules can be studied by an electronically off-resonant Raman process induced by a probe pulse with variable delay with respect to an actinic pulse. We establish the connection between several variants of the technique that involve either spontaneous or stimulated Raman detection and different pulse configurations. By using loop diagrams in the frequency domain we show that all signals can be described as six wave mixing which depend on the same four point molecular correlation functions involving two transition dipoles and two polarizabilities and accompanied by a different gating. Simulations for the stochastic two-state-jump model illustrate the origin of the absorptive and dispersive features observed experimentally

Broadband infrared and Raman probes of excited-state vibrational molecular dynamics; Simulation protocols based on loop diagram

Vibrational motions in electronically excited states can be observed by either time and frequency resolved infrared absorption or by off resonant stimulated Raman techniques. Multipoint correlation function expressions are derived for both signals. Three representations for the signal which suggest different simulation protocols are developed. These are based on the forward and the backward propagation of the wavefunction, sum over state expansion using an effective vibration Hamiltonian and a semiclassical treatment of a bath. We show that the effective temporal ($\Delta t$) and spectral ($\Delta\omega$) resolution of the techniques is not controlled solely by experimental knobs but also depends on the system dynamics being probed. The Fourier uncertainty $\Delta\omega\Delta t>1$ is never violated