An Approach To “Quantumness” In Coherent Control

Scholak, Torsten; Brumer, Paul

doi:10.1002/9781119324560.ch2

Cited by 6 publications

(3 citation statements)

References 143 publications

(288 reference statements)

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“…The interaction of light with matter is ubiquitous in nature and central to the function of many natural processes . Sample issues, of longstanding physical chemistry interest, are bacterial or plant photosynthesis, and isomerization in the first steps in vision. , Challenging questions that have emerged , from pulsed laser experiments − have motivated vigorous discussions as to the role of quantum mechanics and “nontrivial” quantum effects (such as interference, entanglement, nonlocality, etc. − ) in natural nanoscale biological systems. In addition, information gleaned from these systems are stimulating new directions in light-based technologies such as photocells, , and recent results have provided new insights into the way in which these systems should be considered computationally and conceptually …”

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confidence: 99%

Shedding (Incoherent) Light on Quantum Effects in Light-Induced Biological Processes

Brumer

2018

J. Phys. Chem. Lett.

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Light-induced processes that occur in nature, such as photosynthesis and photoisomerization in the first steps in vision, are often studied in the laboratory using coherent pulsed laser sources, which induce time-dependent coherent wavepacket molecule dynamics. Nature, however, uses stationary incoherent thermal radiation, such as sunlight, leading to a totally different molecular response, the time-independent steady state. It is vital to appreciate this difference in order to assess the role of quantum coherence effects in biological systems. Developments in this area are discussed in detail.

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Shedding (Incoherent) Light on Quantum Effects in Light-Induced Biological Processes

Brumer

2018

J. Phys. Chem. Lett.

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“…Hence, for open systems, deviation from an equilibrium population distribution can also serve as a signature of the quantum behavior. Scholak and Brumer demonstrated the nontrivial aspect of quantumness in coherent control …”

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Quantum Coherence and Its Signatures in Extended Quantum Systems

Dutta

Bagchi

2020

J. Phys. Chem. B

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Quantum coherence controls almost every aspect of static and dynamic response of a strongly correlated quantum system, although details of this control have not been elucidated in many cases. We find that, in the presence of a significant static off-diagonal coupling, quantum coherence can survive much longer than the bath correlation time in a noisy environment. In the presence of time correlated noise (non-Markovian limit), coherence could propagate through the excited bath states, and this plays a nontrivial role in giving rise to a noncanonical temperature dependence of population distribution in an extended conjugated polymer-like system. The quantum coherence through the excited bath states vanishes in the high temperature limit, giving rise to the equilibrium Boltzmann distribution. Second, we discuss a role of quantum coherence in exciton localization that bears resemblance to Anderson localization. Calculations have been carried out not only with a chain of conjugated polymer but also with dimer and trimer subunits of the Fenna−Matthews−Olson (FMO) complex. We derive an analytical expression of the relation between steady state coherence and excitionic population distribution. We analytically showed that steady state coherence in equilibrium bath states is governed by interchromophoric coupling (J) whereas coherence in excited bath states is dictated by fluctuation strength (V d ) for the spatially correlated bath model. For the spatially uncorrelated bath model, we observe that at the low temperature limit coherence in the excited bath states dominates over coherence in equilibrium bath states and vice versa. In the study of the localization problem, we analytically show that, in the limit of a negligibly small fluctuation rate (b d ), the diffusion coefficient is exactly proportional to the fluctuation rate, leading to complete breakdown of the Haken−Strobl−Silbey Markovian prediction.

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“…Quantum coherent control is a well-established approach free of these limitations, whereby quantum interference of transition pathways from an initially pre-pared coherent superposition of molecular states is used to maximize or minimize the transition amplitudes, as in the classic Young double-slit experiment [40,41]. While coherent control has enjoyed great success when applied to unimolecular processes (such as photodissociation), its application to bimolecular collision dynamics has been limited by the need to entangle the internal and external degrees of freedom of collision partners, a significant experimental challenge [40,42,43] that can be circumvented by using superpositions of degenerate magnetic sublevels (m-superpositions) as initial scattering states [44][45][46].…”

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Complete quantum coherent control of ultracold molecular collisions

Devolder,

Brumer,

Tscherbul

2020

Preprint

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We show that quantum interference-based coherent control is a highly efficient tool for tuning ultracold molecular collision dynamics, and is free from the limitations of commonly used methods that rely on external electromagnetic fields. By varying the relative populations and phases of an initial coherent superpositions of degenerate molecular states, we demonstrate complete coherent control over integral scattering cross sections in the ultracold s-wave regime of both the initial and final collision channels. The proposed control methodology is applied to ultracold O2 + O2 collisions, showing extensive control over s-wave spin-exchange cross sections and product branching ratios over many orders of magnitude.

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An Approach To “Quantumness” In Coherent Control

Cited by 6 publications

References 143 publications

Shedding (Incoherent) Light on Quantum Effects in Light-Induced Biological Processes

Shedding (Incoherent) Light on Quantum Effects in Light-Induced Biological Processes

Quantum Coherence and Its Signatures in Extended Quantum Systems

Complete quantum coherent control of ultracold molecular collisions

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