No Arabic abstract
The development of spectroscopic techniques able to detect and verify quantum coherence is a goal of increasing importance given the rapid progress of new quantum technologies, the advances in the field of quantum thermodynamics, and the emergence of new questions in chemistry and biology regarding the possible relevance of quantum coherence in biochemical processes. Ideally, these tools should be able to detect and verify the presence of quantum coherence in both the transient dynamics and the steady state of driven-dissipative systems, such as light-harvesting complexes driven by thermal photons in natural conditions. This requirement poses a challenge for standard laser spectroscopy methods. Here, we propose photon correlation measurements as a new tool to analyse quantum dynamics in molecular aggregates in driven-dissipative situations. We show that the photon correlation statistics on the light emitted by a molecular dimer model can signal the presence of coherent dynamics. Deviations from the counting statistics of independent emitters constitute a direct fingerprint of quantum coherence in the steady state. Furthermore, the analysis of frequency resolved photon correlations can signal the presence of coherent dynamics even in the absence of steady state coherence, providing direct spectroscopic access to the much sought-after site energies in molecular aggregates.
The measured multi-dimensional spectral response of different light harvesting complexes exhibits oscillatory features which suggest an underlying coherent energy transfer. However, making this inference rigorous is challenging due to the difficulty of isolating excited state coherences in highly congested spectra. In this work, we provide a coherent control scheme that suppresses ground state coherences, thus making rephasing spectra dominated by excited state coherences. We provide a benchmark for the scheme using a model dimeric system and numerically exact methods to analyze the spectral response. We argue that combining temporal and spectral control methods can facilitate a second generation of experiments that are tailored to extract desired information and thus significantly advance our understanding of complex open many-body structure and dynamics.
Quantum tunneling events occurring through biochemical bonds are capable to generate quantum correlations between bonded systems, which in turn makes the conventional second law of thermodynamics approach insufficient to investigate these systems. This means that the utilization of these correlations in their biological functions could give an evolutionary advantage to biomolecules to an extent beyond the predictions of molecular biology that are generally based on the second law in its standard form. To explore this possibility, we first compare the tunneling assisted quantum entanglement shared in the ground states of covalent and hydrogen bonds. Only the latter appears to be useful from a quantum information point of view. Also, significant amounts of quantum entanglement can be found in the thermal state of hydrogen bond. Then, we focus on an illustrative example of ligand binding in which a receptor protein or an enzyme is restricted to recognize its ligands using the same set of proton-acceptors and donors residing on its binding site. In particular, we show that such a biomolecule can discriminate between $3^n - 1$ agonist ligands if it uses the entanglement shared in $n$ intermolecular hydrogen bonds as a resource in molecular recognition. Finally, we consider the molecular recognition events encountered in both the contemporary genetic machinery and its hypothetical primordial ancestor in pre-DNA world, and discuss whether there may have been a place for the utilization of quantum entanglement in the evolutionary history of this system.
We report photon correlation measurements that allow us to observe unique signatures of biexcitons in a single self-assembled InAs quantum dot. Photon correlation measurements of biexciton emission exhibit both bunching and antibunching under continuous-wave excitation while only antibunching is observed under pulsed excitation. Cross-correlation between biexciton and single-exciton peaks reveal highly asymmetric features, demonstrating that biexciton and exciton emissions have strong correlations due to cascaded emission. The anticipated correlation between the polarization of exciton and biexciton emissions however, is absent under our excitation conditions. Photon correlation measurements also provide evidence for the identification of the charged exciton emission.
Recent practical approaches for the use of current generation noisy quantum devices in the simulation of quantum many-body problems have been dominated by the use of a variational quantum eigensolver (VQE). These coupled quantum-classical algorithms leverage the ability to perform many repeated measurements to avoid the currently prohibitive gate depths often required for exact quantum algorithms, with the restriction of a parameterized circuit to describe the states of interest. In this work, we show how the calculation of zero-temperature dynamic correlation functions defining the linear response characteristics of quantum systems can also be recast into a modified VQE algorithm, which can be incorporated into the current variational quantum infrastructure. This allows for these important physical expectation values describing the dynamics of the system to be directly converged on the frequency axis, and they approach exactness over all frequencies as the flexibility of the parameterization increases. The frequency resolution hence does not explicitly scale with gate depth, which is approximately twice as deep as a ground state VQE. We apply the method to compute the single-particle Greens function of ab initio dihydrogen and lithium hydride molecules, and demonstrate the use of a practical active space embedding approach to extend to larger systems. While currently limited by the fidelity of two-qubit gates, whose number is increased compared to the ground state algorithm on current devices, we believe the approach shows potential for the extraction of frequency dynamics of correlated systems on near-term quantum processors.
Understanding gravity in the framework of quantum mechanics is one of the great challenges in modern physics. Along this line, a prime question is to find whether gravity is a quantum entity subject to the rules of quantum mechanics. It is fair to say that there are no feasible ideas yet to test the quantum coherent behaviour of gravity directly in a laboratory experiment. Here, we introduce an idea for such a test based on the principle that two objects cannot be entangled without a quantum mediator. We show that despite the weakness of gravity, the phase evolution induced by the gravitational interaction of two micron size test masses in adjacent matter-wave interferometers can detectably entangle them even when they are placed far apart enough to keep Casimir-Polder forces at bay. We provide a prescription for witnessing this entanglement, which certifies gravity as a quantum coherent mediator, through simple correlation measurements between two spins: one embedded in each test mass. Fundamentally, the above entanglement is shown to certify the presence of non-zero off-diagonal terms in the coherent state basis of the gravitational field modes.