arXiv subjects

Shaul Mukamel

Publications and source records attributed to Shaul Mukamel.

At least 91 records · Page 5Linked to original sources

arXiv2012

Two-Dimensional Stimulated Resonance Raman Spectroscopy of Molecules with Broadband X-ray Pulses

Expressions for the two-dimensional Stimulated x-ray Raman Spectroscopy (2D-SXRS) signal obtained using attosecond x-ray pulses are derived. The 1D- and 2D-SXRS signals are calculated for trans-N-methyl acetamide (NMA) with broad bandwidth (FWHM ~14.2eV, 181 as) pulses tuned to the oxygen and nitrogen K-edges. Crosspeaks in 2D signals reveal electronic Franck-Condon overlaps between valence orbitals and relaxed orbitals in the presence of the core hole.

physics.chem-ph↗

arXiv2011

Two-dimensional double-quantum spectra reveal collective resonances in an atomic vapor

We report the observation of double-quantum coherence signals in a gas of potassium atoms at twice the frequency of the one-quantum coherences. Since a single atom does not have a state at the corresponding energy, this observation must be attributed to a collective resonance involving multiple atoms. These resonances are induced by weak inter-atomic dipole-dipole interactions, which means that the atoms cannot be treated in isolation, even at a low density of $10^{12}$ cm$^{-3}$.

physics.atom-ph↗

arXiv2010

Multidimensional measures of impulsively driven stochastic systems based on the Kullback-Leibler distance

By subjecting a dynamical system to a series of short pulses and varying several time delays we can obtain multidimensional characteristic measures of the system. Multidimensional Kullback-Leibler response function (KLRF), which are based on the Kullback-Leibler distance between the initial and final states, are defined. We compare the KLRF, which are nonlinear in the probability density, with ordinary response functions (ORF) obtained from the expectation value of a dynamical variable, which are linear. We show that the KLRF encode different level of information regarding the system's dynamics. For overdamped stochastic dynamics two dimensional KLRF shows a qualitatively different variation with the time delays between pulses, depending on whether the system is initially in a steady state, or in thermal equilibrium.

cond-mat.stat-mech↗

arXiv2009

Many-body two-quantum coherences in semiconductor nanostructures

We present experimental coherent two-dimensional Fourier transform spectra of the exciton resonances in semiconductor quantum wells for a pulse sequence that isolates two-quantum coherences. By measuring the real part of the spectra, we can determine that the spectra are dominated by two quantum coherences due to many-body interactions, not bound biexcitons. Simulations performed using dynamics controlled truncation agree well with the experiments.

cond-mat.mes-hall↗

arXiv2009

Gaussian phase-space representation of Fermion dynamics; Beyond the time-dependent-Hartree-Fock approximation

A Gaussian operator representation for the many body density matrix of fermionic systems, developed by Corney and Drummond [Phys. Rev. Lett, v93, 260401 (2004)], is used to derive approximate decoupling schemes for their dynamics. In this approach the reduced single electron density matrix elements serve as stochastic variables which satisfy an exact Fokker-Planck equation. The number of variables scales as ~N^2 rather than ~exp(N) with the basis set size, and the time dependent Hartree Fock approximation (TDHF) is recovered in the "classical" limit. An approximate closed set of equations of motion for the one and two-particle reduced density matrices, provides a direct generalization of the TDHF.

cond-mat.other↗

arXiv2009

Nonequilibrium fluctuations, fluctuation theorems, and counting statistics in quantum systems

Fluctuation theorems (FTs), which describe some universal properties of nonequilibrium fluctuations, are examined from a quantum perspective and derived by introducing a two-point measurement on the system. FTs for closed and open systems driven out of equilibrium by an external time-dependent force, and for open systems maintained in a nonequilibrium steady-state by nonequilibrium boundary conditions, are derived from a unified approach. Applications to fermion and boson transport in quantum junctions are discussed. Quantum master equations and Green's functions techniques for computing the energy and particle statistics are presented.

cond-mat.stat-mech↗

arXiv2008

Double-quantum-coherence attosecond x-ray spectroscopy of spatially separated, spectrally overlapping core-electron transitions

X-ray four-wave mixing signals generated in the $k_1 + k_2 - k_3$ phase-matching direction are simulated for N1s transitions in para-nitroanline and two-ring hydrocarbons disubstituted with an amine and a nitroso groups. The two-dimensional x-ray correlation spectra (2DXCS) provide background-free probes of couplings between core-electron transitions even for multiple core shells of the same type. Features attributed to couplings between spatially-separated core transitions connected by delocalized valence excitations provide information about molecular geometry and electronic structure unavailable from linear near-edge x-ray absorption (XANES).

physics.atom-ph↗

arXiv2008

Waiting time distributions of electron transfers through quantum dot Aharonov-Bohm interferometers

We present a statistical readout method for quantum interferences based on time series analysis of consecutive single electron transfers through a double quantum dot Aharonov-Bohm interferometer. Waiting time distributions qualitatively indicate the presence of interferences and provide information on orbital-detuning and coherent interdot-electron transfer. Interdot transfer induced oscillations are Aharonov-Bohm phase sensitive, while those due to level detuning are phase-independent. The signature of the quantum interference in the waiting time distribution is more apparent for weakly coupled electron transfer detectors.

cond-mat.mes-hall↗

arXiv2008

Single-electron counting spectroscopy: simulation study of porphyrin in a molecular junction

Electron counting of a single porphyrin molecule between two electrodes shows a crossover from sub- to super-Poissonian statistics as the bias voltage is scanned. This is attributed to the simultaneous activation of states with electron transfer rates spanning several orders of magnitude. Time-series analysis of consecutive single electron transfer events reveals fast and slow transport channels, which are not resolved by the average current alone.

cond-mat.mes-hall↗

arXiv2008

Interference effects in the counting statistics of electron transfers through a double quantum dot

We investigate the effect of quantum interferences and Coulomb interaction on the counting statistics of electrons crossing a double quantum dot in a parallel geometry using a generating function technique based on a quantum master equation approach. The skewness and the average residence time of electrons in the dots are shown to be the quantities most sensitive to interferences and Coulomb coupling. The joint probabilities of consecutive electron transfer processes show characteristic temporal oscillations due to interference. The steady-state fluctuation theorem which predicts a universal connection between the number of forward and backward transfer events is shown to hold even in the presence of Coulomb coupling and interference.

cond-mat.mes-hall↗

arXiv2007

Two-dimensional correlation spectroscopy of two-exciton resonances in semiconductor quantum wells

We propose a three-pulse coherent ultrafast optical technique that is particularly sensitive to two-exciton correlations. Two Liouville-space pathways for the density matrix contribute to this signal which reveals double quantum coherences when displayed as a two-dimensional correlation plot. Two-exciton couplings spread the cross peaks along both axes, creating a characteristic highly resolved pattern. This level of detail is not available from conventional one-dimensional four-wave mixing or other two-dimensional correlation spectroscopy signals such as the photo echo, in which two-exciton couplings show up along a single axis and are highly congested.

cond-mat.mes-hall↗

arXiv2007

Partially-Time-Ordered Schwinger-Keldysh Loop Expansion of Coherent Nonlinear Optical Susceptibilities

A compact correlation-function expansion is developed for nth order optical susceptibilities in the frequency domain using the Keldysh-Schwinger loop. By not keeping track of the relative time ordering of bra and ket interactions at the two branches of the loop, the resulting expressions contain only n+1 basic terms, compared to the 2n terms required for a fully time-ordered density matrix description. Superoperator Green's function expressions for the nth order suscpeptibility derived using both expansions reflect different types of interferences between pathways .These are demonstrated for correlation-induced resonances in four wave mixing signals.

quant-ph↗

arXiv2007

Nonlinear optical spectroscopy of single, few, and many molecules; nonequilibrium Green's function QED approach

Nonlinear optical signals from an assembly of N noninteracting particles consist of an incoherent and a coherent component, whose magnitudes scale \sim N and \sim N(N-1), respectively. A unified microscopic description of both types of signals is developed using a quantum electrodynamical (QED) treatment of the optical fields. Closed nonequilibrium Green's function expressions are derived that incorporate both stimulated and spontaneous processes. General (n+1)-wave mixing experiments are discussed as an example of spontaneously generated signals. When performed on a single particle, such signals cannot be expressed in terms of the nth order polarization, as predicted by the semiclassical theory. Stimulated processes are shown to be purely incoherent in nature. Within the QED framework, heterodyne-detected wave mixing signals are simply viewed as incoherent stimulated emission, whereas homodyne signals are generated by coherent spontaneous emission.

quant-ph↗

arXiv2007

A Coherent Nonlinear Optical Signal Induced by Electron Correlations

The correlated behavior of electrons determines the structure and optical properties of molecules, semiconductor and other systems. Valuable information on these correlations is provided by measuring the response to femtosecond laser pulses, which probe the very short time period during which the excited particles remain correlated. The interpretation of four-wave-mixing techniques, commonly used to study the energy levels and dynamics of many-electron systems, is complicated by many competing effects and overlapping resonances. Here we propose a coherent optical technique, specifically designed to provide a background-free probe for electronic correlations in many-electron systems. The proposed signal pulse is generated only when the electrons are correlated, which gives rise to an extraordinary sensitivity. The peak pattern in two-dimensional plots, obtained by displaying the signal vs. two frequencies conjugated to two pulse delays, provides a direct visualization and specific signatures of the many-electron wavefunctions.

cond-mat.mes-hall↗

arXiv2007

Entropy fluctuation theorems in driven open systems: application to electron counting statistics

The total entropy production generated by the dynamics of an externally driven systems exchanging energy and matter with multiple reservoirs and described by a master equation is expressed as the sum of three contributions, each corresponding to a distinct mechanism for bringing the system out of equilibrium: nonequilibrium initial conditions, external driving, and breaking of detailed balance. We derive three integral fluctuation theorems (FTs) for these contributions and show that they lead to the following universal inequality: an arbitrary nonequilibrium transformation always produces a change in the total entropy production greater or equal than the one produced if the transformation is done very slowly (adiabatically). Previously derived fluctuation theorems can be recovered as special cases. We show how these FTs can be experimentally tested by performing the counting statistics of the electrons crossing a single level quantum dot coupled to two reservoirs with externally varying chemical potentials. The entropy probability distributions are simulated for driving protocols ranging from the adiabatic to the sudden switching limit.

cond-mat.stat-mech↗

arXiv2007

Anomalous Lineshapes and Aging Effects in Two-Dimensional Correlation Spectroscopy

Multitime correlation functions provide useful probes for the ensembles of trajectories underlying the stochastic dynamics of complex systems. These can be obtained by measuring their optical response to sequences of ultrashort optical pulse. Using the continuous time random walk model for spectral diffusion, we analyze the signatures of anomalous relaxation in two-dimensional four wave mixing signals. Different models which share the same two point joint probability distribution show markedly different lineshapes and may be distinguished. Aging random walks corresponding to waiting time distributions with diverging first moment show dependence of 2D lineshapes on initial observation time, which persist for long times.

cond-mat.soft↗

arXiv2007

Coherent ultrafast core-hole correlation spectroscopy: x-ray analogues of multidimensional NMR

We propose two dimensional x-ray coherent correlation spectroscopy (2DXCS) for the study of interactions between core-electron and valence transitions. This technique might find experimental applications in the future when very high intensity x-ray sources become available. Spectra obtained by varying two delay periods between pulses show off-diagonal cross-peaks induced by coupling of core transitions of two different types. Calculations of the N1s and O1s signals of aminophenol isomers illustrate how novel information about many-body effects in electronic structure and excitations of molecules can be extracted from these spectra.

quant-ph↗

arXiv2007

Causal vs. Noncausal Description of Nonlinear Wave Mixing; Resolving the Damping-Sign Controversy

Frequency-domain nonlinear wave mixing processes may be described either using response functions whereby the signal is generated after all interactions with the incoming fields, or in terms of scattering amplitudes where all fields are treated symetrically with no specific time ordering. Closed Green's function expressions derived for the two types of signals have different analytical properties. The recent controversy regarding the sign of radiative damping in the linear (Kramers Heisenberg) formula is put in a broader context.

quant-ph↗