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Optics Express

Modeling and correction of distorted two-dimensional Fourier transform spectra from pixelated pulse shaping devices

Erik M. Grumstrup, Niels H. Damrauer

Published Aug 28, 2012• 0 citations
Publisher

Abstract

Two-dimensional Fourier transform spectra of a three level model system are simulated using a non-perturbative density matrix formalism. The electric field distortions resultant from using pixelated pulse shaping devices to produce phase-locked pulse pairs are modeled and the effects on the recovered spectra are examined. To minimize spectral distortions, a temporal filtering scheme is employed which eliminates contributions from spurious sample polarizations.

DOI
10.1364/oe.20.020908

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Two-dimensional Fourier transform spectra of a three level model system are simulated using a non-perturbative density matrix formalism. The electric field distortions resultant from using pixelated pulse shaping devices to produce phase-locked pulse pairs are modeled and the effects on the recovered spectra are examined. To minimize spectral distortions, a temporal filtering scheme is employed which eliminates contributions from spurious sample polarizations.
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Two-dimensional (2D) spectroscopy is a powerful pump-pump-probe technique for revealing couplings between quantum states and disentangling the different contributions to the optical response of a system. We present an efficient method for 2D spectroscopy simulations in the Markovian limit for the environment, capable of handling arbitrary pulse shapes and reproducing time-ordering and overlapping pulse effects, while maintaining a computational cost that scales linearly with the number of sampling points. We leverage this framework to investigate how 2D spectra are affected by spectral phase distortions and highly non-Gaussian pulse shapes, such as those produced experimentally by hollow-core fibers or non-collinear optical amplifiers. We show that realistic pulses can induce the appearance of additional spectral features, lineshape distortions and oscillating contributions in the system's dynamics. Notably, even weak temporal pulse tails arising from uncorrected high-order spectral phase terms cause visible changes in the 2D spectra. We also find that homodyne detection schemes employed in experiments can mitigate the presence of such pulse effects. These results emphasize the importance of including realistic pulses in 2D spectroscopy simulations to identify pulse-induced effects and minimize ambiguities in the interpretation of experimental data.
In a series of experiments we explore various aspects of femtosecond pulse shaping by coherent filters engraved in a persistent spectral hole burning (PSHB) material. We have in mind the coherent control of quantum systems, with high resolution and large number of addressable spectral points. We examine the phase correction efficiency of this approach, relying on Fourier transform spectral interferometry techniques to characterize the coherent filter. Two different PSHB materials are considered, with two different setups, involving different values of repetition rate, fluence, wavelength, spectral width and pulse duration.
In time-dependent optical spectra, fast dynamics of narrow transitions give rise to artifacts consisting of spectral oscillations. In contrast with spectrally-integrated experiments, the interpretation of spectrally-resolved pump-probe experiments is thus far from straightforward in regimes where such coherent effects dominate, i.e., when the timescales of pump-induced processes are shorter than the medium dephasing times. Analyzing the two-dimensional Fourier transform of the time-dependent spectrum, we identify the components responsible for these artifacts and we introduce a simple Fourier-filtering procedure for their systematic removal. This technique is theoretically demonstrated on the time-dependent spectrum of a transition undergoing a frequency shift. The technique is also shown to have the additional benefit of efficient noise filtering of time-dependent spectra.
Gate-defined semiconductor quantum dots utilize fast electrical control to manipulate spin and charge states of individual electrons. Electrical pulse distortions can limit control fidelities but are difficult to measure at the device level. Here, we use detuning-axis pulsed spectroscopy to characterize baseband pulse distortions in a silicon double quantum-dot. We extract the gate-voltage impulse response and apply a digital pre-distortion filter to eliminate pulse distortions on timescales longer than 1~ns. With the pre-distortion, we reduce the frequency chirp of coherent exchange oscillations in a singlet-triplet qubit. Our results suggest a scalable and tuning-efficient method for characterizing pulse distortions in quantum-dot spin qubits.
A systematic theoretical and computational investigation of the microscopic factors which determine the phase of the signal field in time-resolved quasidegenerate three-pulse scattering experiments is presented. The third-order phase-matched response is obtained by density-matrix perturbation theory using a Green-function formalism for a system composed of two well-separated sets of closely spaced energy levels. Equations for calculating the electric field of four-wave-mixing signals generated by path-length delayed pulses are given. It is found that the phase of the signal field is determined by the excitation pulse phases, the dynamics of the nonlinear polarization decay, the product of four transition dipole matrix elements, and by a pulse-delay-dependent phase modulation at the frequency of the first dipole oscillation in the four-wave-mixing process. Analytic results for a two-level Bloch model show the phase shift from rapid nonlinear polarization decay. The product of dipole matrix elements is real and positive for three-level processes (bleached ground-state absorption and excited-state emission), but can be real and negative for some four-level Raman processes. The pulse-delay-dependent phase modulation treated here is closely related to the interferometric pulse-delay-dependent amplitude modulation observed in some collinear experiments, and plays a role in producing photon echos in inhomogeneously broadened samples. Numerical calculations of phase-resolved electric fields for finite duration pulses using a Brownian oscillator model appropriate for condensed-phase dynamics are presented. The ability of pulse-delay-dependent phase modulation to encode the frequency of the initially excited dipole onto the phase of the signal field can be exploited to examine energy-level connectivity, reveal correlations hidden under the inhomogeneous lineshape, and probe relaxation pathways in multilevel systems.