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Shaul Mukamel

Publications and source records attributed to Shaul Mukamel.

At least 109 records · Page 6Linked to original sources
arXiv2007

Sum-over-states vs quasiparticle pictures of coherent correlation spectroscopy of excitons in semiconductors; femtosecond analogues of multidimensional NMR

Two-dimensional correlation spectroscopy (2DCS) based on the nonlinear optical response of excitons to sequences of ultrafast pulses, has the potential to provide some unique insights into carrier dynamics in semiconductors. The most prominent feature of 2DCS, cross peaks, can best be understood using a sum-over-states picture involving the many-body eigenstates. However, the optical response of semiconductors is usually calculated by solving truncated equations of motion for dynamical variables, which result in a quasiparticle picture. In this work we derive Green's function expressions for the four wave mixing signals generated in various phase-matching directions and use them to establish the connection between the two pictures. The formal connection with Frenkel excitons (hard-core bosons) and vibrational excitons (soft-core bosons) is pointed out.

cond-mat.mes-hall↗
arXiv2007

Fluctuation theorem for counting-statistics in electron transport through quantum junctions

We demonstrate that the probability distribution of the net number of electrons passing through a quantum system in a junction obeys a steady-state fluctuation theorem (FT) which can be tested experimentally by the full counting statistics (FCS) of electrons crossing the lead-system interface. The FCS is calculated using a many-body quantum master equation (QME) combined with a Liouville space generating function (GF) formalism. For a model of two coupled quantum dots, we show that the FT becomes valid for long binning times and provide an estimate for the finite-time deviations. We also demonstrate that the Mandel (or Fano) parameter associated with the incoming or outgoing electron transfers show subpoissonian (antibunching) statistics.

cond-mat.mes-hall↗
arXiv2007

Two-Dimensional Optical Spectroscopy of Excitons in Semiconductor Quantum Wells: Liouville-space pathway analysis

We demonstrate how dynamic correlations of heavy-hole and light-hole excitons in semiconductor quantum wells may be investigated by two dimensional correlation spectroscopy (2DCS). The coherent response to three femtosecond optical pulses is predicted to yield cross (off-diagonal) peaks that contain direct signatures of many-body two-exciton correlations. Signals generated at various phase-matching directions are compared.

cond-mat.mes-hall↗
arXiv2006

Quantum master equation for electron transport through quantum dots and single molecules

A quantum master equation (QME) is derived for the many-body density matrix of an open current-carrying system weakly coupled to two metal leads. The dynamics and the steady-state properties of the system for arbitrary bias are studied using projection operator techniques, which keep track of number of electrons in the system. We show that coherences between system states with different number of electrons, n, (Fock space coherences) do not contribute to the transport to second order in system-lead coupling. However, coherences between states with the same n may effect transport properties when the damping rate is of the order or faster then the system Bohr frequencies. For large bias, when all the system many-body states lie between the chemical potentials of the two leads, we recover previous results. In the rotating wave approximation (when the damping is slow compared to the Bohr frequencies of the system), the dynamics of populations and the coherences in the system eigenbasis are decoupled. The QME then reduces to a birth and death master equation for populations.

cond-mat.stat-mech↗
arXiv2006

Stochastic Simulation of Chemical Exchange in Two Dimensional Infrared Spectroscopy

The stochastic Liouville equations are employed to investigate the combined signatures of chemical exchange (two-state-jump) and spectral diffusion (coupling to an overdamped Brownian oscillator) in the coherent response of an anharmonic vibration to three femtosecond infrared pulses. Simulations reproduce the main features recently observed in the OD stretch of phenol in benzene.

physics.chem-ph↗
arXiv2006

Fluctuation theorems for quantum master equations

A quantum fluctuation theorem for a driven quantum subsystem interacting with its environment is derived based solely on the assumption that its reduced density matrix obeys a closed evolution equation i.e. a quantum master equation (QME). Quantum trajectories and their associated entropy, heat and work appear naturally by transforming the QME to a time dependent Liouville space basis that diagonalizes the instantaneous reduced density matrix of the subsystem. A quantum integral fluctuation theorem, a steady state fluctuation theorem and the Jarzynski relation are derived in a similar way as for classical stochastic dynamics.

cond-mat.stat-mech↗
arXiv2005

Multiple Core-Hole Coherence in X-Ray Four-Wave-Mixing Spectroscopies

Correlation-function expressions are derived for the coherent nonlinear response of molecules to three resonant ultrafast pulses in the x-ray regime. The ability to create two-core-hole states with controlled attosecond timing in four-wave-mixing and pump probe techniques should open up new windows into the response of valence electrons, which are not available from incoherent x-ray Raman and fluorescence techniques. Closed expressions for the necessary four-point correlation functions are derived for the electron-boson model by using the second order cumulant expansion to describe the fluctuating potentials. The information obtained from multidimensional nonlinear techniques could be used to test and refine this model, and establish an anharmonic oscillator picture for electronic excitations.

cond-mat.str-el↗
arXiv2005

Time-domain chirally-sensitive three-pulse coherent probes of vibrational excitons in proteins

The third order optical response of bosonic excitons is calculated using the Green's function solution of the Nonlinear Exciton Equations (NEE) which establish a quasiparticle-scattering mechanism for optical nonlinearities. Both time ordered and non ordered forms of the response function which represent time and frequency domain techniques, respectively, are derived. New components of the response tensor are predicted for isotropic ensembles of periodic chiral structures to first order in the optical wavevector. The nonlocal nonlinear response function is calculated in momentum space, where the finite exciton-exciton interaction length greatly reduces the computational effort. Applications are made to coupled anharmonic vibrations in the amide I infrared band of peptides. Chirally-sensitive and non sensitive signals for alpha helices and antiparallel beta sheets are compared.

cond-mat.mtrl-sci↗
arXiv2004

Current Profiles of Molecular Nanowires; DFT Green Function Representation

The Liouville-space Green function formalism is used to compute the current density profile across a single molecule attached to electrodes. Time ordering is maintained in real, physical, time, avoiding the use of artificial time loops and backward propagations. Closed expressions for molecular currents, which only require DFT calculations for the isolated molecule, are derived to fourth order in the molecule/electrode coupling.

cond-mat.mes-hall↗
arXiv2003

Time-Dependent Quasiparticle Current Density Functional Theory of X-Ray Nonlinear Response Functions

A real-space representation of the current response of many-electron systems with possible applications to x-ray nonlinear spectroscopy and magnetic susceptibilities is developed. Closed expressions for the linear, quadratic and third-order response functions are derived by solving the adiabatic Time Dependent Current Density Functional (TDCDFT) equations for the single-electron density matrix in Liouville space.

cond-mat.str-el↗
arXiv2003

Photon Statistics; Nonlinear Spectroscopy of Single Quantum Systems

A unified description of multitime correlation functions, nonlinear response functions, and quantum measurements is developed using a common generating function which allows a direct comparison of their information content. A general formal expression for photon counting statistics from single quantum objects is derived in terms of Liouville space correlation functions of the material system by making a single assumption that spontaneous emission is described by a master equation.

cond-mat.stat-mech↗
arXiv2003

Superoperator Representation of Nonlinear Response; Unifying Quantum Field and Mode Coupling Theories

Computing response functions by following the time evolution of superoperators in Liouville space (whose vectors are ordinary Hilbert space operators) offers an attractive alternative to the diagrammatic perturbative expansion of many-body equilibrium and nonequilibrium Green functions. The bookkeeping of time ordering is naturally maintained in real (physical) time, allowing the formulation of Wick's theorem for superoperators, giving a factorization of higher order response functions in terms of two fundamental Green's functions. Backward propagations and the analytic continuations using artificial times (Keldysh loops and Matsubara contours) are avoided. A generating functional for nonlinear response functions unifies quantum field theory and the classical mode coupling formalism of nonlinear hydrodynamics and may be used for semiclassical expansions. Classical response functions may be obtained without the explicit computation of stability matrices.

cond-mat.stat-mech↗
arXiv2003

Semiclassical Mode-Coupling Factorizations of Coherent Nonlinear Optical Response

The identification of relevant collective coordinates is crucial for the interpretation of coherent nonlinear spectroscopies of complex molecules and liquids. Using an $\hbar$ expansion of Liouville space generating functions, we show how to factorize multitime nonlinear response functions into products of lower-order correlation functions of collective coordinates, and derive closed expressions for linear, second and third order response functions. In addition to providing systematic quantum corrections, $\hbar$ offers a convenient bookkeeping device even for the purely classical response, since including quantum fluctuations allows to circumvent the expensive computation of stability matrices which is a major bottleneck in Molecular Dynamics (MD) simulations. The existing classical simulation strategies, including Mode-Coupling in $\mathbf{k}$ space and in real-space, Langevin equations, and Instantaneous Normal Modes are compared from a unified viewpoint.

cond-mat.mtrl-sci↗
arXiv2003

Generalized Coherent State Derivation of TDDFT Equations for Superconductors

Equations of motion are derived for the normal and the anomalous single-electron density matrices of a Fermi liquid using a time dependent finite temperature generalized coherent state (GCS) variational ansatz for the many-body density matrix. Self-consistent equations for the order parameter $Δ$ allow to investigate the interplay of Coulomb repulsion and pairing attraction in homogeneous and inhomogeneous Fermi-liquids with spontaneously broken symmetry such as high temperature superconductors. The temperature of the Kosterlitz-Thouless transition to the two-dimensional superfluidity is calculated.

cond-mat.supr-con↗
arXiv2003

Quantum Extension of the Jarzynski Relation

The relation between the distribution of work performed on a classical system by an external force switched on an arbitrary timescale, and the corresponding equilibrium free energy difference, is generalized to quantum systems. Using the adiabatic representation we show that this relation holds for isolated systems as well as for systems coupled to a bath described by a master equation. A close formal analogy is established between the present classical trajectory picture over populations of adiabatic states and phase fluctuations (dephasing) of a quantum coherence in spectral lineshapes, described by the stochastic Liouville equation.

cond-mat.stat-mech↗
arXiv2003

Quasiparticle Density-Matrix Representation of Nonlinear TDDFT Response Functions

The time-dependent density functional (TDDFT) equations may be written either for the Kohn-Sham orbitals in Hilbert space or for the single electron density matrix in Liouville space. A collective-oscillator, quasiparticle, representation of the density response of many-electron systems which explicitly reveals the relevant electronic coherence sizes is developed using the Liouville space representation of adiabatic TDDFT. Closed expressions for the nonlinear density-density response are derived, eliminating the need to solve nonlinear integral equations, as required in the Hilbert space formulation of the response.

cond-mat.str-el↗
arXiv2001

Disorder and Funneling Effects on Exciton Migration in Tree-Like Dendrimers

The center-bound excitonic diffusion on dendrimers subjected to several types of non-homogeneous funneling potentials, is considered. We first study the mean-first passage time (MFPT) for diffusion in a linear potential with different types of correlated and uncorrelated random perturbations. Increasing the funneling force, there is a transition from a phase in which the MFPT grows exponentially with the number of generations $g$, to one in which it does so linearly. Overall the disorder slows down the diffusion, but the effect is much more pronounced in the exponential compared to the linear phase. When the disorder gives rise to uncorrelated random forces there is, in addition, a transition as the temperature $T$ is lowered. This is a transition from a high-$T$ regime in which all paths contribute to the MFPT to a low-$T$ regime in which only a few of them do. We further explore the funneling within a realistic non-linear potential for extended dendrimers in which the dependence of the lowest excitonic energy level on the segment length was derived using the Time-Dependent Hatree-Fock approximation. Under this potential the MFPT grows initially linearly with $g$ but crosses-over, beyond a molecular-specific and $T$-dependent optimal size, to an exponential increase. Finally we consider geometrical disorder in the form of a small concentration of long connections as in the {\it small world} model. Beyond a critical concentration of connections the MFPT decreases significantly and it changes to a power-law or to a logarithmic scaling with $g$, depending on the strength of the funneling force.

cond-mat.stat-mech↗