Spectroscopy of Triatomic Hydrogen Molecules in a Beam

Figger, H.; Dixit, M. N.; Maier, Robert R. J.; Schrepp, W.; Walther, H.; Peterkin, I. R.; Watson, J. K. G.

doi:10.1103/physrevlett.52.906

Cited by 30 publications

(14 citation statements)

References 11 publications

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“…Recently considerable progress in the spectroscopy of H3 has been achieved with the use of neutralized massselected ion beams [9][10][11][12][13][14][15][16][17][18][19][20][21]. Emission spectra from n= 3 and n = 4 Rydberg states of H3, H2D, DHz and D 3 have been obtained by Figger et al.…”

Section: Introductionmentioning

confidence: 97%

Analysis of the Jahn-Teller effect in then p 2 E′ Rydberg series of H3 and D3

Staib

Domcke

1990

Z Phys D - Atoms, Molecules and Clusters

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Spectroscopic signatures of Jahn-Teller (JT) coupling in the np~,.y2E ' Rydberg series of H3 and D3 are analyzed within a simple multi-channel-quantum-defect-type model. The JT coupling constant has been inferred from existing ab initio calculations of the potential-energy surfaces of low Rydberg states of H3. The model predicts pronounced resonant perturbations in Rydberg members with intermediate n (n = 5-7) as well as strong JT-induced autoionization in absorption and ion-yield spectra from vibrationally excited initial levels. The JTinduced effects are shown to exhibit a characteristic dependence on the vibrational angular momentum of the bending mode in the initial state.

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Section: Introductionmentioning

confidence: 97%

Analysis of the Jahn-Teller effect in then p 2 E′ Rydberg series of H3 and D3

Staib

Domcke

1990

Z Phys D - Atoms, Molecules and Clusters

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“…2, Black Line). The triatomic hydrogen molecule is unstable in the electronic ground state, but excited and ionized states are longlived and play an important role in molecular spectroscopy (36)(37)(38)(39)(40).…”

Section: Resultsmentioning

confidence: 99%

Femtosecond quantum control of molecular bond formation

Nuernberger

Wolpert

Weiß

et al. 2010

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

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Ultrafast lasers are versatile tools used in many scientific areas, from welding to eye surgery. They are also used to coherently manipulate light-matter interactions such as chemical reactions, but so far control experiments have concentrated on cleavage or rearrangement of existing molecular bonds. Here we demonstrate the synthesis of several molecular species starting from small reactant molecules in laser-induced catalytic surface reactions, and even the increase of the relative reaction efficiency by feedbackoptimized laser pulses. We show that the control mechanism is nontrivial and sensitive to the relative proportion of the reactants.The control experiments open up a pathway towards photocatalysis and are relevant for research in physics, chemistry, and biology where light-induced bond formation is important.femtochemistry | surface science E ver since their invention, lasers were considered the ideal tool for microscopic control over chemical bonds, and several seminal coherent control approaches have been developed (1-3). A very successful method to this task is femtosecond quantum control, where selectivity over photoinduced reactions is achieved by exploiting the coherence properties and ultrashort time scales of femtosecond laser radiation (4-6). Combined with learning algorithms processing experimental feedback to adaptively find optimized pulses best suited for solving the control task (7), chemical reactions can even be controlled without a priori knowledge about the reaction mechanisms. This scheme has been successfully applied to dissociative reactions in the gas phase, first on organometallic compounds (8) and later on many other systems. The method is not limited to gas phase experiments, as fluorescence optimizations of molecules in the liquid phase have shown (9-12). Recently, also more complex control tasks have been realized, like the energy flow in large biomolecules (13) or the quantum yield in a photoisomerization reaction (14-16). Femtosecond lasers have also been introduced to the field of photoassociation from atoms in cold traps, in both theory (17,18) and first experiments (19,20). However, the selective laser manipulation of bond-forming reactions starting from small reactant molecules that may furthermore exhibit competing bond-forming reaction channels has not been shown yet.In this contribution, we present the realization of femtosecond laser-assisted catalytic reactions of carbon monoxide and hydrogen or deuterium at a metal surface and further demonstrate that the relative reaction efficiency can be increased by the benefits of femtosecond laser pulses tailored especially for a desired reaction outcome. These experiments represent a first step and a reaction path toward laser-induced catalysis of molecular systems.Femtosecond laser sources have been employed by laser scientists to explore processes on metal surfaces as soon as they were available. Other types of lasers have been used earlier for this purpose, but starting from the first demonstration of intact desorption of ...

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“…In the present contribution, the bands at 5600Å of D 2 H and H 2 D which we measured some time ago by our ion beam neutralization method [4][5][6][7] are computer-simulated and rotational constants were determined.…”

Section: Introductionmentioning

confidence: 99%

“…The breakthrough in studying the complete series of the isotopomers (not containing tritium), in particular D 2 H and H 2 D, was achieved when spectra were observed emitted by a mass-selected and then neutralized ion beam of H + 3 , D + 3 , D 2 H + and H 2 D + [4][5][6][7]. Also lifetimes of the n = 3 states (of the isotopomers mentioned above) could be measured from the exponential decay of the light intensity emitted along the neutralized beam.…”

Section: Introductionmentioning

confidence: 99%

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Analysis of the molecular bands of D2H and H2D at 5600 Å

Azinović

Figger

1997

Z Phys D - Atoms, Molecules and Clusters

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Spectral simulation was used to analyze the molecular rovibrational bands of D 2 H and H 2 D at 5600Å.These bands were previously measured by the ion beam neutralization method. They were assigned to the electronic 3p 2 B 1 -2s 2 A 1 and vibrational (v − v ) = (0, 0, 0, −0, 0, 0) transitions. Least squares fits to the experimental line-positions were made to determine the asymmetric rotator constants A, B and C for the 2s 2 A 1 and 3p 2 B 1 v = 0 states of D 2 H and H 2 D, hitherto unknown. Lorentz line-profiles were assumed for the D 2 H and H 2 D rotational lines, whose widths are mainly governed by the lifetimes of the lower states. The bands at 5600Å were simulated and the 2s 2 A 1 state lifetimes were estimated to be σ ≥ 0.5 ± 0.2 ps for D 2 H and σ ≥ 0.4 ± 0.2 ps for H 2 D. Vibrational constants of D 3 and D 2 H in the 2s 2 A 1 states are determined from the positions of the 0-0 and 0-1 vibrational bands given in respective experimental spectra previously measured. For the first time the vibrational constants ω 1 and ω 2 of the 2s 2 A 1 state of H 2 D were estimated from the positions of the 0-0 and 0-1 band maxima. These vibrational constants are compared with the corresponding vibrational constants of their ions.

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Spectroscopy of Triatomic Hydrogen Molecules in a Beam

Cited by 30 publications

References 11 publications

Analysis of the Jahn-Teller effect in then p 2 E′ Rydberg series of H3 and D3

Analysis of the Jahn-Teller effect in then p 2 E′ Rydberg series of H3 and D3

Femtosecond quantum control of molecular bond formation

Analysis of the molecular bands of D2H and H2D at 5600 Å

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