Quantum Control of Tightly Competitive Product Channels

Roth, Matthias; Guyon, Laurent; Roslund, Jonathan; Boutou, Véronique; Courvoisier, F.; Wolf, Jean‐Pierre; Rabitz, Herschel

doi:10.1103/physrevlett.102.253001

Cited by 109 publications

(98 citation statements)

References 11 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…21 This paper expands upon that groundwork and is organized as follows. Section II provides an underpinning of the ODD concept before introducing the flavin model systems in Sec.…”

Section: Introductionmentioning

confidence: 99%

Resolution of strongly competitive product channels with optimal dynamic discrimination: Application to flavins

Roslund

Roth

Guyon

et al. 2011

The Journal of Chemical Physics

Self Cite

View full text Add to dashboard Cite

Fundamental molecular selectivity limits are probed by exploiting laser-controlled quantum interferences for the creation of distinct spectral signatures in two flavin molecules, erstwhile nearly indistinguishable via steady-state methods. Optimal dynamic discrimination (ODD) uses optimally shaped laser fields to transiently amplify minute molecular variations that would otherwise go unnoticed with linear absorption and fluorescence techniques. ODD is experimentally demonstrated by combining an optimally shaped UV pump pulse with a time-delayed, fluorescence-depleting IR pulse for discrimination amongst riboflavin and flavin mononucleotide in aqueous solution, which are structurally and spectroscopically very similar. Closed-loop, adaptive pulse shaping discovers a set of UV pulses that induce disparate responses from the two flavins and allows for concomitant flavin discrimination of ∼16σ . Additionally, attainment of ODD permits quantitative, analytical detection of the individual constituents in a flavin mixture. The successful implementation of ODD on quantum systems of such high complexity bodes well for the future development of the field and the use of ODD techniques in a variety of demanding practical applications.

show abstract

“…21 This paper expands upon that groundwork and is organized as follows. Section II provides an underpinning of the ODD concept before introducing the flavin model systems in Sec.…”

Section: Introductionmentioning

confidence: 99%

Resolution of strongly competitive product channels with optimal dynamic discrimination: Application to flavins

Roslund

Roth

Guyon

et al. 2011

The Journal of Chemical Physics

Self Cite

View full text Add to dashboard Cite

show abstract

“…Successful optimal control experiments (OCEs) have included selective control of molecular vibrational [10][11][12][13][14][15][16][17] and electronic states [18][19][20][21][22][23][24][25][26][27], preservation of quantum coherence [28,29], control of photoisomerization reactions [30][31][32][33][34][35], selective manipulation of chemical bonds [36][37][38][39][40][41][42][43][44], high-harmonic generation and coherent manipulation of the resulting soft X-rays [45][46][47][48][49][50][51], and control of energy flow in biomolecular complexes [52][53][54][55]. Optimal control theory (OCT) [7,9,…”

Section: Introductionmentioning

confidence: 99%

Searching for quantum optimal controls under severe constraints

Riviello¹,

Tibbetts²,

Brif³

et al. 2015

Phys. Rev. A

Self Cite

View full text Add to dashboard Cite

The success of quantum optimal control for both experimental and theoretical objectives is connected to the topology of the corresponding control landscapes, which are free from local traps if three conditions are met: (1) the quantum system is controllable, (2) the Jacobian of the map from the control field to the evolution operator is of full rank, and (3) there are no constraints on the control field. This paper investigates how the violation of assumption (3) affects gradient searches for globally optimal control fields. The satisfaction of assumptions (1) and (2) ensures that the control landscape lacks fundamental traps, but certain control constraints can still introduce artificial traps. Proper management of these constraints is an issue of great practical importance for numerical simulations as well as optimization in the laboratory. Using optimal control simulations, we show that constraints on quantities such as the number of control variables, the control duration, and the field strength are potentially severe enough to prevent successful optimization of the objective. For each such constraint, we show that exceeding quantifiable limits can prevent gradient searches from reaching a globally optimal solution. These results demonstrate that careful choice of relevant control parameters helps to eliminate artificial traps and facilitate successful optimization.

show abstract

“…Shaped pulses are also used in time-resolved coherent anti-Stokes Raman scattering (14-16) or 2D spectroscopy (17, 18). Adaptive shaping of the pulses via feedback control even allows the optimization of dynamical processes, e.g., the relative photodissociation yield of organometallic molecules (19), the relative twophoton fluorescence yield of dye molecules (20), and the energy transfer in light-harvesting molecules (21).However, the strong-field dynamics in complex systems, e.g., in the liquid phase, and its control have only recently moved into scientific focus (22)(23)(24)(25)(26)(27). The dynamics of complex systems was thus far studied mainly in perturbative experiments such as transient absorption spectroscopy, which measures the evolution of a system after absorbing a single or a few photons.…”

mentioning

confidence: 99%

Signatures and control of strong-field dynamics in a complex system

Meyer

Liu

Müller

et al. 2015

Proc. Natl. Acad. Sci. U.S.A.

View full text Add to dashboard Cite

Controlling chemical reactions by light, i.e., the selective making and breaking of chemical bonds in a desired way with strong-field lasers, is a long-held dream in science. An essential step toward achieving this goal is to understand the interactions of atomic and molecular systems with intense laser light. The main focus of experiments that were performed thus far was on quantum-state population changes. Phase-shaped laser pulses were used to control the population of final states, also, by making use of quantum interference of different pathways. However, the quantum-mechanical phase of these final states, governing the system's response and thus the subsequent temporal evolution and dynamics of the system, was not systematically analyzed. Here, we demonstrate a generalized phase-control concept for complex systems in the liquid phase. In this scheme, the intensity of a control laser pulse acts as a control knob to manipulate the quantum-mechanical phase evolution of excited states. This control manifests itself in the phase of the molecule's dipole response accessible via its absorption spectrum. As reported here, the shape of a broad molecular absorption band is significantly modified for laser pulse intensities ranging from the weak perturbative to the strongfield regime. This generalized phase-control concept provides a powerful tool to interpret and understand the strong-field dynamics and control of large molecules in external pulsed laser fields. C an we find universal concepts to understand and control the response of atoms and molecules in interactions with strong laser fields? This question is at the heart of a vast number of experiments in time-resolved spectroscopy (1-30). The wide range of light sources spanning the spectral range from the X-ray (e.g., free-electron laser sources, synchrotrons) over the visible (conventional laser systems) to the far-infrared regime and covering the temporal range from nanosecond down to attosecond time scales created a wealth of new physics insight into quantum mechanisms, however mostly of simple systems in the gas phase (1-4). In chemistry, the generation of femtosecond laser pulses enabled the investigation of wave packet dynamics in molecules, as the induced vibrations occur on these time scales. Experiments focusing on, for instance, dissociation reactions, atom transfer, isomerization, or solvation dynamics have led to a deeper understanding of chemical bonds and their breakage dynamics and have opened and established the field of femtochemistry (5, 6). The aim is not only to study the light−matter interaction, but to use the obtained understanding of the processes to control the dynamics in complex molecules and, in the future, even to be able to control chemical reactions (7-10). Shaping the amplitude and phase of femtosecond laser pulses has been used, for example, to control the shape of wavefunctions in atomic systems (11) or to control and optimize the single-photon and multiphoton fluorescence in atoms such as cesium (12) and complex systems, e.g....

show abstract

Quantum Control of Tightly Competitive Product Channels

Cited by 109 publications

References 11 publications

Resolution of strongly competitive product channels with optimal dynamic discrimination: Application to flavins

Resolution of strongly competitive product channels with optimal dynamic discrimination: Application to flavins

Searching for quantum optimal controls under severe constraints

Signatures and control of strong-field dynamics in a complex system

Contact Info

Product

Resources

About