Tuning the photophysical behavior of luminescent cyclam derivatives by cation binding and excited state redox potential

The emission from two photoactive 14-membered macrocyclic ligands, 6-((naphthalen-1-ylmethyl)-amino)trans-6,13-dimethyl- 13-amino- 1,4,8,11 -tetraaza-cyclotetradecane (L-1) and 6-((anthracen-9-ylmethyl)-amino)trans-6,13 -dimethyl - 13 -amino- 1,4,8, 1 1-tetraaza-cyclotetradecane (L-2) is strongly quenched by a photoinduced electron transfer (PET) mechanism involving amine lone pairs as electron donors. Time-correlated single photon counting (TCSPC), multiplex transient grating (TG), and fluorescence upconversion (FU) measurements were performed to characterize this quenching mechanism. Upon complexation with the redox inactive metal ion, Zn(II), the emission of the ligands is dramatically altered, with a significant increase in the fluorescence quantum yields due to coordination-induced deactivation of the macrocyclic amine lone pair electron donors. For [ZnL2](2+), the substituted exocyclic amine nitrogen, which is not coordinated to the metal ion, does not quench the fluorescence due to an inductive effect of the proximal divalent metal ion that raises the ionization potential. However, for [ZnL1](2+), the naphthalene chromophore is a sufficiently strong excited-state oxidant for PET quenching to occur.

Unified derivations of measurement-based schemes for quantum computation

We present unified, systematic derivations of schemes in the two known measurement-based models of quantum computation. The first model (introduced by Raussendorf and Briegel, [Phys. Rev. Lett. 86, 5188 (2001)]) uses a fixed entangled state, adaptive measurements on single qubits, and feedforward of the measurement results. The second model (proposed by Nielsen, [Phys. Lett. A 308, 96 (2003)] and further simplified by Leung, [Int. J. Quant. Inf. 2, 33 (2004)]) uses adaptive two-qubit measurements that can be applied to arbitrary pairs of qubits, and feedforward of the measurement results. The underlying principle of our derivations is a variant of teleportation introduced by Zhou, Leung, and Chuang, [Phys. Rev. A 62, 052316 (2000)]. Our derivations unify these two measurement-based models of quantum computation and provide significantly simpler schemes.

Optimal unravellings for feedback control in linear quantum systems

For quantum systems with linear dynamics in phase space much of classical feedback control theory applies. However, there are some questions that are sensible only for the quantum case: Given a fixed interaction between the system and the environment what is the optimal measurement on the environment for a particular control problem? We show that for a broad class of optimal (state- based) control problems ( the stationary linear-quadratic-Gaussian class), this question is a semidefinite program. Moreover, the answer also applies to Markovian (current-based) feedback.

Relativistically invariant quantum information

We show that quantum information can be encoded into entangled states of multiple indistinguishable particles in such a way that any inertial observer can prepare, manipulate, or measure the encoded state independent of their Lorentz reference frame. Such relativistically invariant quantum information is free of the difficulties associated with encoding into spin or other degrees of freedom in a relativistic context.

Quantum dynamics of a model for two Josephson-coupled Bose-Einstein condensates

In this work, we investigate the quantum dynamics of a model for two singlemode Bose-Einstein condensates which are coupled via Josephson tunnelling. Using direct numerical diagonalization of the Hamiltonian, we compute the time evolution of the expectation value for the relative particle number across a wide range of couplings. Our analysis shows that the system exhibits rich and complex behaviours varying between harmonic and non-harmonic oscillations, particularly around the threshold coupling between the delocalized and selftrapping phases. We show that these behaviours are dependent on both the initial state of the system and regime of the coupling. In addition, a study of the dynamics for the variance of the relative particle number expectation and the entanglement for different initial states is presented in detail.

A quantum yield map for synthetic eumelanin

The quantum yield of synthetic eumelanin is known to be extremely low and it has recently been reported to be dependent on excitation wavelength. In this paper, we present quantum yield as a function of excitation wavelength between 250 and 500 nm, showing it to be a factor of 4 higher at 250 nm than at 500 nm. In addition, we present a definitive map of the steady-state fluorescence as a function of excitation and emission wavelengths, and significantly, a three-dimensional map of the specific quantum yield: the fraction of photons absorbed at each wavelength that are subsequently radiated at each emission wavelength. This map contains clear features, which we attribute to certain structural models, and shows that radiative emission and specific quantum yield are negligible at emission wavelengths outside the range of 585 and 385 nm (2.2 and 3.2 eV), regardless of excitation wavelength. This information is important in the context of understanding melanin biofunctionality, and the quantum molecular biophysics therein. (c) 2005 American Institute of Physics.

Demonstration of a simple entangling optical gate and its use in bell-state analysis

We demonstrate a new architecture for an optical entangling gate that is significantly simpler than previous realizations, using partially polarizing beam splitters so that only a single optical mode-matching condition is required. We demonstrate operation of a controlled-z gate in both continuous-wave and pulsed regimes of operation, fully characterizing it in each case using quantum process tomography. We also demonstrate a fully resolving, nondeterministic optical Bell-state analyzer based on this controlled-z gate. This new architecture is ideally suited to guided optics implementations of optical gates.

High-fidelity measurement and quantum feedback control in circuit QED

Circuit QED is a promising solid-state quantum computing architecture. It also has excellent potential as a platform for quantum control-especially quantum feedback control-experiments. However, the current scheme for measurement in circuit QED is low efficiency and has low signal-to-noise ratio for single-shot measurements. The low quality of this measurement makes the implementation of feedback difficult, and here we propose two schemes for measurement in circuit QED architectures that can significantly improve signal-to-noise ratio and potentially achieve quantum-limited measurement. Such measurements would enable the implementation of quantum feedback protocols and we illustrate this with a simple entanglement-stabilization scheme.

Entanglement under restricted operations: Analogy to mixed-state entanglement

We show that the classification of bipartite pure entangled states when local quantum operations are restricted yields a structure that is analogous in many respects to that of mixed-state entanglement. Specifically, we develop this analogy by restricting operations through local superselection rules, and show that such exotic phenomena as bound entanglement and activation arise using pure states in this setting. This analogy aids in resolving several conceptual puzzles in the study of entanglement under restricted operations. In particular, we demonstrate that several types of quantum optical states that possess confusing entanglement properties are analogous to bound entangled states. Also, the classification of pure-state entanglement under restricted operations can be much simpler than for mixed-state entanglement. For instance, in the case of local Abelian superselection rules all questions concerning distillability can be resolved.

Classical simulation of quantum many-body systems with a tree tensor network

We show how to efficiently simulate a quantum many-body system with tree structure when its entanglement (Schmidt number) is small for any bipartite split along an edge of the tree. As an application, we show that any one-way quantum computation on a tree graph can be efficiently simulated with a classical computer.

Complex numbers and symmetries in quantum mechanics, and a nonlinear superposition principle for Wigner functions

Complex numbers appear in the Hilbert space formulation of quantum mechanics, but not in the formulation in phase space. Quantum symmetries are described by complex, unitary or antiunitary operators defining ray representations in Hilbert space, whereas in phase space they are described by real, true representations. Equivalence of the formulations requires that the former representations can be obtained from the latter and vice versa. Examples are given. Equivalence of the two formulations also requires that complex superpositions of state vectors can be described in the phase space formulation, and it is shown that this leads to a nonlinear superposition principle for orthogonal, pure-state Wigner functions. It is concluded that the use of complex numbers in quantum mechanics can be regarded as a computational device to simplify calculations, as in all other applications of mathematics to physical phenomena.

Criteria for quantum coherent transfer of excitations between chromophores in a polar solvent

We show that the quantum decoherence of Forster resonant energy transfer between two optically active molecules can be described by a spin-boson model. This allows us to give quantitative criteria that are necessary for coherent quantum oscillations of excitations between the chromophores. Experimental tests of our results should be possible with flourescent resonant energy transfer (FRET) spectroscopy. Although we focus on the case of protein-pigment complexes our results are also relevant to quantum dots and organic molecules in a dielectric medium. (c) 2006 Elsevier B.V. All rights reserved.

Modelling photo-detectors in quantum optics

Photo-detection plays a fundamental role in experimental quantum optics and is of particular importance in the emerging field of linear optics quantum computing. Present theoretical treatment of photo-detectors is highly idealized and fails to consider many important physical effects. We present a physically motivated model for photo-detectors which accommodates for the effects of finite resolution, bandwidth and efficiency, as well as dark counts and dead-time. We apply our model to two simple well-known applications, which illustrates the significance of these characteristics.

Noise thresholds for optical quantum computers

In this Letter we numerically investigate the fault-tolerant threshold for optical cluster-state quantum computing. We allow both photon loss noise and depolarizing noise (as a general proxy for all local noise), and obtain a threshold region of allowed pairs of values for the two types of noise. Roughly speaking, our results show that scalable optical quantum computing is possible for photon loss probabilities < 3x10(-3), and for depolarization probabilities < 10(-4).

Quantum computation by communication

We present here a new approach to scalable quantum computing - a 'qubus computer' - which realizes qubit measurement and quantum gates through interacting qubits with a quantum communication bus mode. The qubits could be 'static' matter qubits or 'flying' optical qubits, but the scheme we focus on here is particularly suited to matter qubits. There is no requirement for direct interaction between the qubits. Universal two-qubit quantum gates may be effected by schemes which involve measurement of the bus mode, or by schemes where the bus disentangles automatically and no measurement is needed. In effect, the approach integrates together qubit degrees of freedom for computation with quantum continuous variables for communication and interaction.