Initiation and control of catalytic surface reactions with shaped femtosecond laser pulses

Nuernberger, Patrick; Wolpert, Daniel; Weiß, Horst; Gerber, G.

doi:10.1039/c1cp21827a

Cited by 14 publications

(9 citation statements)

References 107 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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“…35 Recently, Gerber and co-workers have demonstrated that CO and hydrogen coadsorbed on Pd(100) produce various molecules including formaldehyde, water, etc., upon the irradiation of fs laser pulses. 36,37 In addition, they showed that the product yield ratio can be optimized by changing the time profile of excitation pulses. Definitely, we need more examples of photoinduced chemistry among adsorbates.…”

Section: B Surface Photochemistrymentioning

confidence: 99%

Toward photochemistry of integrated heterogeneous systems

Matsumoto

2012

The Journal of Chemical Physics

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This paper begins with describing the excitation mechanisms in surface photochemistry and nuclear dynamics of adsorbate induced by electronic excitation. An illustrative example is Cs adsorbate on a Cu(111) surface. This adsorption system shows drastic changes in the electronic structure with coverage; this allows us to examine different types of electronic excitations that stimulate nuclear motions of Cs. Remarks are made on challenges in photoinduced processes at well-defined surfaces: direct observations of adsorbate-substrate vibrational modes and photoinduced reactions between adsorbates. Then, the paper addresses some issues in more complex systems: metal-liquid interfaces and powdered photocatalysts of metal oxides. Photochemistry and photoinduced nuclear dynamics at metal-liquid interfaces have not been well explored. Studies on this subject may make it possible to bridge the gap between surface photochemistry and electrochemistry. Photocatalysis with powdered catalysts has been extensively studied and is still an active area, but our understanding of the mechanism of photocatalysis is far from satisfactory. Although complicated, the highly integrated systems provide an opportunity to extend our knowledge of surface photochemistry.

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“…Since the advent of powerful femtosecond lasers, the field of material response to irradiation has been developing fast [1]. It is driven by a wide range of applications in materials surface and bulk processing and nanostructuring for photonics [2], catalysis [3] and biomedicine [4]. Elemental metals and alloys are a class of materials that is widely used in the ultrafast community for its relative simplicity and versatile functionality [5][6][7].…”

Section: Introductionmentioning

confidence: 99%

Contribution of inter- and intraband transitions into electron–phonon coupling in metals

Medvedev

Milov

2021

Eur. Phys. J. D

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We recently developed an approach for calculation of the electron–phonon (electron–ion in a more general case) coupling in materials based on tight-binding molecular dynamics simulations. In the present work, we utilize this approach to study partial contributions of inter- and intraband electron scattering events into total electron–phonon coupling in Al, Au, and Cu elemental metals and in AlCu alloy. We demonstrate that the interband scattering plays an important role in the electron–ion energy exchange process in Al and AlCu, whereas intraband d–d transitions are dominant in Au and Cu. Moreover, inter- and intraband transitions exhibit qualitatively different dependencies on the electron temperature. Our findings should be taken into account for the interpretation of experimental results on the electron–phonon coupling parameter. Graphic abstract

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Initiation and control of catalytic surface reactions with shaped femtosecond laser pulses

Cited by 14 publications

References 107 publications

Searching for quantum optimal controls under severe constraints

Searching for quantum optimal controls under severe constraints

Toward photochemistry of integrated heterogeneous systems

Contribution of inter- and intraband transitions into electron–phonon coupling in metals

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