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arXiv:2104.03041 · Physical Review A

Measuring time-dependent induced quantum coherences via two-dimensional coherence spectroscopy

William Barford, Allison Nicole Arber, Fynn McLennan, Max Marcus

Published Dec 27, 2021• 1 citation
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Abstract

We propose a two-dimensional spectroscopic protocol for measuring the time-dependent coherences between the stationary states of a system induced by a time-dependent system-bath interaction. We also investigate the role of temporally correlated noise on coherence dephasing. This protocol enables dynamical information about the system and its coupling to the environment to be determined. Our results are based on the quantum-trajectory method, and are obtained from both approximate, analytical and exact, numerical solutions of the time-dependent Schr\"odinger equation. As an example, we show how this protocol can be used to investigate exciton dynamics in conjugated polymers induced by the coupling of their torsional modes with the environment.

DOI
10.1103/physreva.104.063517

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We propose a two-dimensional spectroscopic protocol for measuring the time-dependent coherences between the stationary states of a system induced by a time-dependent system-bath interaction. We also investigate the role of temporally correlated noise on coherence dephasing. This protocol enables dynamical information about the system and its coupling to the environment to be determined. Our results are based on the quantum-trajectory method, and are obtained from both approximate, analytical and exact, numerical solutions of the time-dependent Schr"odinger equation. As an example, we show how this protocol can be used to investigate exciton dynamics in conjugated polymers induced by the coupling of their torsional modes with the environment.
We introduce multipulse quantum noise spectroscopy protocols for spectral estimation of the noise affecting multiple qubits coupled to Gaussian dephasing environments including both classical and quantum sources. Our protocols are capable of reconstructing all the noise auto- and cross-correlation spectra entering the multiqubit dynamics, providing access, in particular, to the asymmetric spectra associated with nonclassical environments. Our result relies on (i) an exact analytic solution for the reduced multiqubit dynamics that holds in the presence of an arbitrary Gaussian environment and dephasing-preserving control; (ii) the use of specific timing symmetries, which allow for a frequency comb to be engineered for all filter functions of interest, and for the spectra to be related to experimentally accessible observables. We show that quantum spectra have distinctive dynamical signatures, which we explore in two paradigmatic open-system models describing spin and charge qubits coupled to bosonic environments. Complete noise spectroscopy is demonstrated numerically in a realistic setting consisting of two-exciton qubits coupled to a phonon bath. The estimated spectra allow us to accurately predict the exciton dynamics as well as extract the temperature and spectral density of the quantum environment.
We study decoherence induced on a two-level system coupled to a one-dimensional quantum spin chain. We consider the cases where the dynamics of the chain is determined by the Ising, XYXYXY, or Heisenberg exchange Hamiltonian. This model of quantum baths can be of fundamental importance for the understanding of decoherence in open quantum systems, since it can be experimentally engineered by using atoms in optical lattices. As an example, here we show how to implement a pure dephasing model for a qubit system coupled to an interacting spin bath. We provide results that go beyond the case of a central spin coupled uniformly to all the spins of the bath, in particular showing what happens when the bath enters different phases, or becomes critical; we also study the dependence of the coherence loss on the number of bath spins to which the system is coupled and we describe a coupling-independent regime in which decoherence exhibits universal features, irrespective of the system-environment coupling strength. Finally, we establish a relation between decoherence and entanglement inside the bath. For the Ising and the XYXYXY models we are able to give an exact expression for the decay of coherences, while for the Heisenberg bath we resort to the numerical time-dependent density matrix renormalization group.
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.
Quantum systems are the foundation of quantum technology development. To harness these systems, one must extract information from them and be able to control their dynamics. This thesis presents a body of work, containing both published and unpublished papers, that focuses on two key research areas: quantum continuous measurement and quantum bath sensing. While these topics may seem distinct, they are fundamentally connected through the framework of open quantum systems. As such, this thesis is structured into two parts. The first part of this thesis is dedicated to diffusive continuous quantum measurement, where the system of interest is continuously monitored through a coupled Markovian bath or meter. A key challenge in this context is the numerical errors introduced in quantum trajectory simulations caused by the finite time resolution ( 𝑡) in real experiments. To address this, we propose a systematic framework to assess theoretical tools used in processing measurement records. Focusing on a single Lindblad channel, we analyze the errors of existing measurement (or Kraus) operators in literature, in orders of 𝑡 under conditions that ensure valid average evolution (complete positivity, convex linearity, and trace preservation). We also analyze a stronger condition: finding the order at which these existing measurement operators match the Lindblad equation. Based on these analyzes, we propose a Kraus operator that satisfies the conditions for valid quantum evolution and matches the Lindblad master equation to second order in 𝑡, surpassing all existing approaches. Moreover, to evaluate how well our operator reproduces exact quantum trajectories, we analyze two qubit measurement examples where exact maps can be derived: 𝑧-basis measurement and fluorescence (dissipative) measurement. We show analytically that our proposed operator achieves the smallest average trace distance to the exact quantum trajectories compared to existing methods. Finally, we extend this Kraus operator to multiple Lindblad channels with a driving Hamiltonian. We test our analytical findings numerically using the two qubit examples, considering both single and multiple Lindblad channels with a driving Hamiltonian. The numerical results confirm our theoretical predictions. The second part of this thesis focuses on quantum bath sensing, where we use a quantum system (qubit) to extract information about its surrounding baths. Specifically, we develop protocols to detect nonclassical pure-dephasing noise in a single-qubit system coupled to temporally correlated (non-Markovian) baths. Inspired by the Ramsey protocol, we introduce a coherent intervention (𝜋 2 -pulse) within the protocol, which can reveal the quantum noise - noise correlations affecting the probe qubit that originate from quantum degrees of freedom. Our protocols are simple, experimentally viable, and rigorously derived for general bath models. Using an exactly solvable bosonic bath model, we analyse how key noise parameters respond to fixed control schemes, identifying the optimal strategy for detecting the quantum noise. From the perspective of bath dynamics, we further decompose the qubit-bath state, demonstrating that only Gaussian components of the bath contribute to quantum noise, highlighting the bath's role in system dynamics. Finally, we extend the modified Ramsey protocol by incorporating multi-axis 𝜋 2 pulse and demonstrate that it can emulate the modified Ramsey protocol with any completely positive trace-preserving intervention. This applies to both Gaussian and non-Gaussian baths under the pure-dephasing assumption.
Multidimensional analysis of coherent signals is commonly used in nuclear magnetic resonance to study correlations among spins. These techniques were recently extended to the femtosecond regime and applied to chemical, biological and semiconductor systems. In this work, we apply a two-dimensional correlation spectroscopy technique which employs double-quantum-coherence to investigate many-body effects in a semiconductor quantum well. The signal is detected along the direction k(1)+ k(2)- k(3), where k(1), k(2) and k(3) are the pulse wave vectors in chronological order. We show that this signal is particularly sensitive to many-body correlations which are missed by time-dependent Hartree-Fock approximation. The correlation energy of two-exciton can be probed with a very high resolution arising from a two-dimensional correlation spectrum, where two-exciton couplings spread the cross peaks along both axes of the 2D spectrum to create 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 (-k(1)+ k(2)+ k(3)).
Interacting dipolar two-level systems form a special class of qubits that interact with a cavity in a particular way. We first prove that the Markovian dynamics of one 1/2-spin in interaction with a quantised magnetic field from a multi-mode cavity at thermal equilibrium is equivalent to a two-level atom interacting in the dipole approximation with the electric field of the cavity. We then use the Born-Markov approximation to study the dynamics of two spins interacting through the antiferromagnetic Heisenberg coupling in the same environment. By solving the GKSL equation, we find the exact expression of the density matrix of the system, with the off-diagonal coherence decay time and spin relaxation time. The concurrence for the stationary state is explicitly derived for any kind of initial state and the role of the singlet state is brought to light. The temporal evolution of the concurrence is numerically computed for different initial states, the phenomenon of sudden death and revival of the entanglement is observed for this dynamics. A detailed analysis of the sudden death and revival of the concurrence is conducted for Werner states, with new analytical results obtained thanks to the solution of the GKSL equation. We finally derive the equations and the stationary concurrence for the XXZ coupling.