Controlling Vibrational Excitation with Shaped Mid-IR Pulses

Strasfeld, David B.; Shim, Sang Hee; Zanni, Martin T.

doi:10.1103/physrevlett.99.038102

Cited by 104 publications

(99 citation statements)

References 19 publications

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“…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

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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.

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Section: Introductionmentioning

confidence: 99%

Searching for quantum optimal controls under severe constraints

Riviello¹,

Tibbetts²,

Brif³

et al. 2015

Phys. Rev. A

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“…[2][3][4]. So far the MIR pulse shaping was applied to the ladder climbing of a single vibrational mode [5].…”

Section: Motivation and Objectivesmentioning

confidence: 99%

“…[2][3][4]. So far the MIR pulse shaping was applied to the ladder climbing of a single vibrational mode [5].The broadband nature of the ultrashort MIR pulses, however, should also be able to excite multiple vibrational modes in a correlated manner to control nuclear motion in multi-dimensional coordinates and to create highly-excited vibrational states. The ability to handle multiple vibrational modes should increase the variety and efficiency of controllable reactions.…”

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confidence: 99%

Controlling Quantum Interferences in IR Vibrational Excitations in Metal Carbonyls

Ashihara

Enomoto

Tayama

2013

EPJ Web of Conferences

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Abstract.Coherent controls over vibrational excitations in metal di-carbonyls were demonstrated by using phase-shaped mid-infrared pulses. The phase of the inter-state coherence between two different normal-modes was controlled by changing the phase step of the stepwise spectral phase profile. The quantum interference between multiple vibrational excitation paths in resonant two-step excitations was manipulated by the similar spectral phase control. The results experimentally confirmed that coherent control over multiple vibrational degrees of freedom works properly in condensed phases. There remains the possibility for increasing excitation efficiency by introducing group-delays and by optimizing polarization state of the excitation pulse. Motivation and ObjectivesCoherent control is a technique that manipulates interference of wave functions by adjusting their amplitudes and phases. Recent developments in the pulse shaping technique in MIR [1] may open a way toward coherent control over molecular motions/reactions at the electronic ground states. Such control may serve for novel information processing and molecular reaction controls, including bond breakage, structural isomerization, hydrogen bond rearrangement, proton transfer, etc. [2][3][4]. So far the MIR pulse shaping was applied to the ladder climbing of a single vibrational mode [5].The broadband nature of the ultrashort MIR pulses, however, should also be able to excite multiple vibrational modes in a correlated manner to control nuclear motion in multi-dimensional coordinates and to create highly-excited vibrational states. The ability to handle multiple vibrational modes should increase the variety and efficiency of controllable reactions. For such coherent control applications, control over quantum interference as well as efficient ladder climbing is essential. In this paper, we show that the quantum interferences in IR vibrational excitations were successfully controlled for liquid-phase molecules by use of MIR phase-shaping. MIR Pulse Shaping and Transient Absorption SpectroscopyMIR pulses of 100-fs duration and 5-J energy were generated by the OPA/DFG system. Major portion of the pulse energy was delivered to the pulse shaper, consisting of diffraction gratings, concave mirrors and the germanium AOM, developed by Zanni-group [1]. The shaped pulse was characterized by the electric-field cross correlation in the spectral interferometry with a reference EPJ Web of Conferences

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“…15 Further experimental progress in vibrational ladder climbing has been reported in Ref. 16 where an evolutionary algorithm was used for pulse shaping such as to highly excite a CO mode in W(CO) 6 .…”

Section: Introductionmentioning

confidence: 99%

Carbonyl vibrational wave packet circulation in Mn2(CO)10 driven by ultrashort polarized laser pulses

Abdel-Latif

Kühn

2011

The Journal of Chemical Physics

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The excitation of the degenerate E 1 carbonyl stretching vibrations in dimanganese decacarbonyl is shown to trigger wave packet circulation in the subspace of these two modes. On the time scale of about 5 picoseconds intramolecular anharmonic couplings do not cause appreciable disturbance, even under conditions where the two E 1 modes are excited by up to about two vibrational quanta each. The compactness of the circulating wave packet is shown to depend strongly on the excitation conditions such as pulse duration and field strength. Numerical results for the solution of the seven-dimensional vibrational Schrödinger equation are obtained for a density functional theory based potential energy surface and using the multi-configuration time-dependent Hartree method.

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Controlling Vibrational Excitation with Shaped Mid-IR Pulses

Cited by 104 publications

References 19 publications

Searching for quantum optimal controls under severe constraints

Searching for quantum optimal controls under severe constraints

Controlling Quantum Interferences in IR Vibrational Excitations in Metal Carbonyls

Carbonyl vibrational wave packet circulation in Mn2(CO)10 driven by ultrashort polarized laser pulses

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