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Konstantin E. Dorfman

Publications and source records attributed to Konstantin E. Dorfman.

28 records · Page 2Linked to original sources
arXiv2014

Stimulated Raman Spectroscopy with Entangled Light; Enhanced Resolution and Pathway Selection

We propose a novel femtosecond stimulated Raman spectroscopy (FSRS) technique that combines entangled photons with interference detection to select matter pathways and enhance the resolution. Following photo excitation by an actinic pump, the measurement uses a pair of broadband entangled photons, one (signal) interacts with the molecule together with a third narrowband pulse induces the Raman process. The other (idler) photon provides a reference for the coincidence measurement. This interferometric photon-coincidence counting detection allows to separately measure Raman gain and loss signals, which is not possible with conventional probe transmission detection. Entangled photons further provide a unique temporal and spectral detection window that can better resolve fast excited state dynamics compared to classical and correlated disentangled states of light.

quant-ph↗
arXiv2014

Time-, Frequency-, and Wavevector-Resolved X-Ray Diffraction from Single Molecules

Using a quantum electrodynamic framework, we calculate the off-resonant scattering of a broad-band X-ray pulse from a sample initially prepared in an arbitrary superposition of electronic states. The signal consists of single-particle (incoherent) and two-particle (coherent) contributions that carry different particle form factors that involve different material transitions. Single-molecule experiments involving incoherent scattering are more influenced by inelastic processes compared to bulk measurements. The conditions under which the technique directly measures charge densities (and can be considered as diffraction) as opposed to correlation functions of the charge-density are specified. The results are illustrated with time- and wavevector-resolved signals from a single amino acid molecule (cysteine) following an impulsive excitation by a stimulated X-ray Raman process resonant with the sulfur K-edge. Our theory and simulations can guide future experimental studies on the structures of nano-particles and proteins.

physics.chem-ph↗
arXiv2014

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.

quant-ph↗
arXiv2013

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.

physics.chem-ph↗
arXiv2013

Collective resonances in $χ^{(3)}$; a QED study

We calculate the third order susceptibility $χ^{(3)}$ of a pair of 2 level atoms which interact via the exchange of photons. QED corrections to second order in coupling to vacuum field modes yield collective two photon absorption resonances which can be observed in transmission spectroscopy of shaped broadband pulses. While some collective effects can be obtained by introducing an effective interatomic coupling using a quantum master equation, the predicted signals contain clear features that are missed by that level of theory and require a full diagrammatic QED treatment.

quant-ph↗
arXiv2013

Quantum-Coherence-Enhanced Surface Plasmon Amplification by Stimulated Emission of Radiation

We investigate surface plasmon amplification in a silver nanoparticle coupled to an externally driven three-level gain medium, and show that quantum coherence significantly enhances the generation of surface plasmons. Surface plasmon amplification by stimulated emission of radiation is achieved in the absence of population inversion on the spasing transition, which reduces the pump requirements. The coherent drive allows us to control the dynamics, and holds promise for quantum control of nanoplasmonic devices.

quant-ph↗
arXiv2013

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 ($Δt$) and spectral ($Δω$) resolution of the techniques is not controlled solely by experimental knobs but also depends on the system dynamics being probed. The Fourier uncertainty $ΔωΔt>1$ is never violated.

quant-ph↗
arXiv2013

Nonlinear light scattering in molecules triggered by an impulsive X-ray Raman process

The time-and-frequency resolved nonlinear light scattering (NLS) signals from a time evolving charge distribution of valence electrons prepared by impulsive X-ray pulses are calculated using a superoperator Green's function formalism. The signal consists of a coherent $\sim N^2$-scaling difference frequency generation and an incoherent fluorescence $\sim N$-scaling component where $N$ is the number of active molecules. The former is given by the classical Larmor formula based on the time-dependent charge density. The latter requires additional information about the electronic structure and may be recast in terms of transition amplitudes representing quantum matter pathways.

quant-ph↗
arXiv2011

Quantum interference controlled resonance profiles: From lasing without inversion to photo-detection

In this work we report a quantum interference mediated control of the resonance profiles in a generic three-level system and investigate its effect on key quantum interference (QI) phenomena. Namely in a three level configuration with doublets in the ground or excited states, we show control over enhancement and suppression of the emission (absorption) profiles. This is achieved by manipulation of the strength of QI and the energy spacing of the doublets. We analyze the application of such QI induced control of the resonance profile in the framework of two limiting cases of lasing without inversion and photo-detection.

physics.atom-ph↗