Molecular isomerization induced by ultrashort infrared pulses. II. Pump–dump isomerization using pairs of time-delayed half-cycle pulses

Uiberacker, C.; Jakubetz, Werner

doi:10.1063/1.1753261

Cited by 15 publications

(16 citation statements)

References 16 publications

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“…109 the gas phase [279][280][281][282][283][284][285] and liquid environment 285,286 is the isomerization of the small molecule hydrogen cyanide. A very prominent example studied in both The open dots show the reference signal obtained with an unshaped laser pulse that is sent after each generation.…”

Section: Control Of Energy Flow and Isomerizationmentioning

confidence: 99%

Femtosecond quantum control of molecular dynamics in the condensed phase

Nuernberger

Vogt

Brixner

et al. 2007

Phys. Chem. Chem. Phys.

282

193

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We review the progress in controlling quantum dynamical processes in the condensed phase with femtosecond laser pulses. Due to its high particle density the condensed phase has both high relevance and appeal for chemical synthesis. Thus, in recent years different methods have been developed to manipulate the dynamics of condensed-phase systems by changing one or multiple laser pulse parameters. Single-parameter control is often achieved by variation of the excitation pulse's wavelength, its linear chirp or its temporal subpulse separation in case of pulse sequences. Multiparameter control schemes are more flexible and provide a much larger parameter space for an optimal solution. This is realized in adaptive femtosecond quantum control, in which the optimal solution is iteratively obtained through the combination of an experimental feedback signal and an automated learning algorithm. Several experiments are presented that illustrate the different control concepts and highlight their broad applicability. These fascinating achievements show the continuous progress on the way towards the control of complex quantum reactions in the condensed phase.

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Section: Control Of Energy Flow and Isomerizationmentioning

confidence: 99%

Femtosecond quantum control of molecular dynamics in the condensed phase

Nuernberger

Vogt

Brixner

et al. 2007

Phys. Chem. Chem. Phys.

282

193

View full text Add to dashboard Cite

show abstract

“…The ability to exert control over the migration could lead to advancement in topics such as the efficiency of catalytic reactions [11] and combustion reactions regarding fuel and energy research [12]. Furthermore, light-induced control of hydrogen migration may open new reaction pathways which cannot materialize by other means.Despite its direct relevance to applied chemistry, studies regarding the control of the hydrogen migration process have been scarce, and have been limited to theory [13,14] for a long time. However, recent progress has been made in coherently controlling isomerization reactions using fundamental parameters of ultrafast strongfield laser sources.…”

mentioning

confidence: 99%

Steering Proton Migration in Hydrocarbons Using Intense Few-Cycle Laser Fields

et al. 2016

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Proton migration is a ubiquitous process in chemical reactions related to biology, combustion, and catalysis. Thus, the ability to manipulate the movement of nuclei with tailored light within a hydrocarbon molecule holds promise for far-reaching applications. Here, we demonstrate the steering of hydrogen migration in simple hydrocarbons, namely, acetylene and allene, using waveform-controlled, few-cycle laser pulses. The rearrangement dynamics is monitored using coincident 3D momentum imaging spectroscopy and described with a widely applicable quantum-dynamical model. Our observations reveal that the underlying control mechanism is due to the manipulation of the phases in a vibrational wave packet by the intense off-resonant laser field. DOI: 10.1103/PhysRevLett.116.193001 The rearrangement of hydrocarbon bonds via the migration of a hydrogen atom can result in major deformations of molecular architecture and, thus, alter the molecule's chemical properties. Examples include keto-enol tautomerism where the migration of a proton changes an aldehyde into an alcohol. Isomerization reactions of that kind have been the subject of numerous studies [1,2]. Of particular interest was to determine the so-called isomerization time, which has been measured to be within several tens of fs in small hydrocarbons [3][4][5][6]. The phenomenon has also been observed in larger molecules, such as protonated triglycine [7]. Tracing of the hydrogen migration from different locations within the molecule has been made possible via isotope labeling; see, e.g., Refs. [8][9][10]. The ability to exert control over the migration could lead to advancement in topics such as the efficiency of catalytic reactions [11] and combustion reactions regarding fuel and energy research [12]. Furthermore, light-induced control of hydrogen migration may open new reaction pathways which cannot materialize by other means.Despite its direct relevance to applied chemistry, studies regarding the control of the hydrogen migration process have been scarce and have been limited to theory [13,14] for a long time. However, recent progress has been made in coherently controlling isomerization reactions using fundamental parameters of ultrafast strong-field laser sources. Xie et al. varied the pulse duration and intensity to explore the isomerization of ethylene [15] and reported control of the total fragmentation yields of various hydrocarbons [16].Here, we demonstrate steering of the direction of the hydrogen migration using the electric field waveform of intense few-cycle laser pulses. This approach goes beyond earlier work on toluene [17] and methanol [18] using twocolor pulses with a duration of tens of fs. In contrast, the duration of our few-cycle laser pulses is significantly shorter than the time scale of the isomerization dynamics, therefore, avoiding charge-resonance-enhanced ionization [19] occurring at large internuclear distances [20]. Moreover, an influence of electron localization-assisted enhanced ionization on the dissociation reactions, recently ...

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“…This is discussed in a companion article. 12 In addition, analytical results regarding such reactions in laser fields by using strong-field techniques are in preparation. 14 This mechanism is robust in several respects.…”

Section: Discussionmentioning

confidence: 99%

“…In a companion paper, 12 we give a comprehensive discussion of the dynamics in terms of wave packet propagation, and we extend the simulations to a pump-dump setup with pairs of time-delayed single-lobe half-cycle pulses.…”

Section: Introductionmentioning

confidence: 99%

Molecular isomerization induced by ultrashort infrared pulses. I. Few-cycle to sub-one-cycle Gaussian pulses and the role of the carrier-envelope phase

Uiberacker

Jakubetz

2004

The Journal of Chemical Physics

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Using 550 previously calculated vibrational energy levels and dipole moments we performed simulations of the HCN-->HNC isomerization dynamics induced by sub-one-cycle and few-cycle IR pulses, which we represent as Gaussian pulses with 0.25-2 optical cycles in the pulse width. Starting from vibrationally pre-excited states, isomerization probabilities of up to 50% are obtained for optimized pulses. With decreasing number of optical cycles a strong dependence on the carrier-envelope phase (CEP) emerges. Although the optimized pulse parameters change significantly with the number of optical cycles, the distortion by the Gaussian envelope produces nearly equal fields, with a positive lobe followed by a negative one. The positions and areas of the lobes are also almost unchanged, irrespective of the number of cycles in the half-width. Isomerization proceeds via a pump-dumplike mechanism induced by the sequential lobes. The first lobe prepares a wave packet incorporating many delocalized states above the barrier. It is the motion of this wave packet across the barrier, which determines the timing of the pump and dump lobes. The role of the pulse parameters, and in particular of the CEP, is to produce the correct lobe sequence, size and timing within a continuous pulse.

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Molecular isomerization induced by ultrashort infrared pulses. II. Pump–dump isomerization using pairs of time-delayed half-cycle pulses

Cited by 15 publications

References 16 publications

Femtosecond quantum control of molecular dynamics in the condensed phase

Femtosecond quantum control of molecular dynamics in the condensed phase

Steering Proton Migration in Hydrocarbons Using Intense Few-Cycle Laser Fields

Molecular isomerization induced by ultrashort infrared pulses. I. Few-cycle to sub-one-cycle Gaussian pulses and the role of the carrier-envelope phase

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