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arXiv:1502.02363 · The Journal of Chemical Physics

Quantum process tomography by 2D fluorescence spectroscopy

Leonardo A. Pachón, Andrew H. Marcus, Alán Aspuru‐Guzik

Published May 18, 2015• 23 citations
arXivHTMLPDF

Abstract

Reconstruction of the dynamics (quantum process tomography) of the single-exciton manifold in energy transfer systems is proposed here on the basis of two-dimensional fluorescence spectroscopy (2D-FS) with phase-modulation. The quantum-process-tomography protocol introduced here benefits from, e.g., the sensitivity enhancement ascribed to 2D-FS. Although the isotropically averaged spectroscopic signals depend on the quantum yield parameter Γ of the doubly excited-exciton manifold, it is shown that the reconstruction of the dynamics is insensitive to this parameter. Applications to foundational and applied problems, as well as further extensions, are discussed.

DOI
10.1063/1.4919954

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Reconstruction of the dynamics (quantum process tomography) of the single-exciton manifold in energy transfer systems is proposed here on the basis of two-dimensional fluorescence spectroscopy (2D-FS) with phase-modulation. The quantum-process-tomography protocol introduced here benefits from, e.g., the sensitivity enhancement ascribed to 2D-FS. Although the isotropically averaged spectroscopic signals depend on the quantum yield parameter Γ of the doubly excited-exciton manifold, it is shown that the reconstruction of the dynamics is insensitive to this parameter. Applications to foundational and applied problems, as well as further extensions, are discussed.
The description of excited state dynamics in energy transfer systems constitutes a theoretical and experimental challenge in modern chemical physics. A spectroscopic protocol that systematically characterizes both coherent and dissipative processes of the probed chromophores is desired. Here, we show that a set of two-color photon-echo experiments performs quantum state tomography (QST) of the one-exciton manifold of a dimer by reconstructing its density matrix in real time. This possibility in turn allows for a complete description of excited state dynamics via quantum process tomography (QPT). Simulations of a noisy QPT experiment for an inhomogeneously broadened ensemble of model excitonic dimers show that the protocol distills rich information about dissipative excitonic dynamics, which appears nontrivially hidden in the signal monitored in single realizations of four-wave mixing experiments.
The description of excited state dynamics in multichromophoric systems constitutes both a theoretical and experimental challenge in modern physical chemistry. An experimental protocol which can systematically characterize both coherent and dissipative processes at the level of the evolving quantum state of the chromophores is desired. In this article, we show that a carefully chosen set of polarization controlled two-color heterodyned photon-echo experiments can be used to reconstruct the time-evolving density matrix of the one-exciton manifold of a heterodimer. This possibility in turn allows for a complete description of the excited state dynamics via quantum process tomography (QPT). Calculations on the dimer show that QPT can reveal rich information about system-bath interactions, which otherwise appear nontrivially hidden in the polarization monitored in standard four-wave mixing experiments. Our study presents a novel method for analyzing condensed phase experiments with a quantum information processing perspective.
Two-dimensional (2D) spectroscopy has been intensively used to study electronic and vibronic coherences in biological systems and semiconductors. This technique studies coherent as well as incoherent signals that arise from the nonlinear interaction of a sequence of laser pulses. In this paper we present a direct evaluation of the 2D signal based on elementary quantum kinetics in order to compare with the common approximate diagrammatic approaches. Here we consider incoherent action signals such as fluorescence or photocurrent as the observable, which is easily accessible in a measurement. These observables are calculated by solving the time evolution of the density matrix in the Lindblad form, which can take into account all possible decoherence processes. The phase modulation technique is used to separate the relevant nonlinear signals from the other possible interaction pathways. The approach can be used to calculate 2D spectra of any quantum system. For our model system we find a good agreement for the quantum beating between the coupled states.
For an initially well designed but imperfect quantum information system, the process matrix is almost sparse in an appropriate basis. Existing theory and associated computational methods (L1-norm minimization) for reconstructing sparse signals establish conditions under which the sparse signal can be perfectly reconstructed from a very limited number of measurements (resources). Although a direct extension to quantum process tomography of the L1-norm minimization theory has not yet emerged, the numerical examples presented here, which apply L1-norm minimization to quantum process tomography, show a significant reduction in resources to achieve a desired estimation accuracy over existing methods.
Abstract To harness the power of controllable quantum systems for information processing or quantum simulation, it is essential to be able to accurately characterise the system's Hamiltonian. Although in principle this requires determining less parameters than full quantum process tomography, a general and extendable method for reconstructing a general Hamiltonian has been elusive. In their recent paper, Wang et al (2015 New J. Phys. 17 093017 ) apply dynamical decoupling to the problem of Hamiltonian tomography and show how to reconstruct a general many-body Hamiltonian comprised of arbitrary interactions between qubits.
Coherent multidimensional spectroscopy allows us to inspect the energies and the coupling of quantum systems. Coupled quantum systems—such as a coupled semiconductor quantum dot or pigments in photosynthesis—form delocalized exciton and two-exciton states. A technique is presented to decompose these delocalized wave functions into the basis of individual quantum emitters. This quantum state tomography protocol is illustrated for three coupled InAs quantum dots. To achieve the decomposition of the wavefunction, we combine the double-quantum-coherence spectroscopy with spatiotemporal control, which allows us to localize optical excitations at a specific quantum dot. Recently, a protocol was proposed for single exciton states (Richter et al 2012 Phys. Rev. B 86 085308). In this paper, we extend the method presented by Richter et al with respect to: the reconstruction of two-exciton states, a detailed analysis process of reconstruction and the effect of filtering to enhance the quality of the reconstructed wave function.