May 20, 2010
In this paper, we develop a quantum-jump approach for describing the photon-emission process of single fluorophore systems coupled to complex classically fluctuating reservoirs. The formalism relies on an open quantum system approach where the dynamic of the system and the reservoir fluctuations are described through a density matrix whose evolution is defined by a Lindblad rate equation. For each realization of the photon measurement processes it is possible to define a conditional system state (stochastic density matrix) whose evolution depends on both the photon detection events and the fluctuations between the configurational states of the reservoir. In contrast to standard fluorescent systems the photon-to-photon emission process is not a renewal one, being defined by a (stochastic) waiting time distribution that in each recording event parametrically depends on the conditional state. The formalism allows calculating experimental observables such as the full hierarchy of joint probabilities associated to the time intervals between consecutive photon recording events. These results provide a powerful basis for characterizing different situations arising in single-molecule spectroscopy, such as spectral fluctuations, lifetime fluctuations, and light assisted processes.
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February 23, 2009
In this paper, single-molecule spectroscopy experiments based on continuous laser excitation are characterized through an open quantum system approach. The evolution of the fluorophore system follows from an effective Hamiltonian microscopic dynamic where its characteristic parameters, i.e., its electric dipole, transition frequency, and Rabi frequency, as well as the quantization of the background electromagnetic field and their mutual interaction, are defined in an extended...
December 3, 2010
The large-deviation method can be used to study the measurement trajectories of open quantum systems. For optical arrangements this formalism allows to describe the long time properties of the (non-equilibrium) photon counting statistics in the context of a (equilibrium) thermodynamic approach defined in terms of dynamical phases and transitions between them in the trajectory space [J.P. Garrahan and I. Lesanovsky, Phys. Rev. Lett. 104, 160601 (2010)]. In this paper, we study...
February 1, 1997
Dissipation, the irreversible loss of energy and coherence, from a microsystem, is the result of coupling to a much larger macrosystem (or reservoir) which is so large that one has no chance of keeping track of all of its degrees of freedom. The microsystem evolution is then described by tracing over the reservoir states, resulting in an irreversible decay as excitation leaks out of the initially excited microsystems into the outer reservoir environment. Earlier treatments of...
January 21, 2022
We first use the quantum method to replicate the well-known results of a single atom relaxing, whilst demonstrating the intuitive picture it provides for dissipative dynamics. By use of individual "quantum trajectories", the method allows for simulation of systems inaccessible to ensemble treatments. This is shown by replicating resonance fluorescence, allowing us to concurrently demonstrate the method's facilitation of calculating photon statistics by the creation of discret...
April 29, 2006
We extend the generating function technique for calculation of single molecule photon emission statistics [Y. Zheng and F. L. H. Brown, Phys. Rev. Lett., 90,238305 (2003)] to systems governed by multi-level quantum dynamics. This opens up the possibility to study phenomena that are outside the realm of purely stochastic and mixed quantum-stochastic models. In particular, the present methodology allows for calculation of photon statistics that are spectrally resolved and subje...
April 16, 2024
Using the principles of the ETH - Approach to Quantum Mechanics we study fluorescence and the phenomenon of ``quantum jumps'' in idealized models of atoms coupled to the quantized electromagnetic field. In a limiting regime where the orbital motion of the atoms is neglected and the velocity of light tends to infinity we derive explicit non-linear stochastic differential equations describing the effective time evolution of states of individual atoms. These equations give rise ...
November 25, 2005
Non-Markovian quantum state diffusion (NMQSD) is an exact method for calculating the reduced density matrix of an arbitrary subsystem interacting linearly with the radiation field. Applications of the theory have however been few due to the intractable nature of the variational-differential NMQSD evolution equation. Recently, we argued that the variational-differential equation can be rewritten as an integrodifferential equation which can be readily solved numerically. This m...
June 29, 2007
Open quantum systems that interact with structured reservoirs exhibit non-Markovian dynamics. We present a quantum jump method for treating the dynamics of such systems. This approach is a generalization of the standard Monte Carlo Wave Function (MCWF) method for Markovian dynamics. The MCWF method identifies decay rates with jump probabilities and fails for non-Markovian systems where the time-dependent rates become temporarily negative. Our non-Markovian quantum jump (NMQJ)...
May 17, 2019
In quantum transport through nanoscale devices, fluctuations arise from various sources: the discreteness of charge carriers, the statistical non-equilibrium that is required for device operation, and unavoidable quantum uncertainty. As experimental techniques have improved over the last decade, measurements of these fluctuations have become available.} They have been accompanied by a plethora of theoretical literature using many different fluctuation statistics to describe t...
October 31, 2013
Single-shot read-out of individual qubits is typically the slowest process among the elementary single- and two-qubit operations required for quantum information processing. Here, we use resonance fluorescence from a single-electron charged quantum dot to read-out the spin-qubit state in 800 nanoseconds with a fidelity exceeding 80%. Observation of the spin evolution on longer timescales reveals quantum jumps of the spin state: we use the experimentally determined waiting-tim...