Measurements of intense ultrafast laser-driven D<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:msub><mml:mrow /><mml:mn>3</mml:mn></mml:msub></mml:math><mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:msup><mml:mrow /><mml:mo>+</mml:mo></mml:msup></mml:math>fragmentation dynamics

Sayler, A. M.; Gaire, B.; Kling, Nora G.; Carnes, K. D.; Ben‐Itzhak, I.

doi:10.1103/physreva.86.033425

Cited by 31 publications

(37 citation statements)

References 55 publications

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“…As the arrival time of the probe pulse is further delayed from the pump pulse, the depletion becomes less prominent. The formed H 3 + are minimally disturbed by the probe pulse 32 . Therefore, the time scale for the H 3 + yield recovery is related to the lifetime of the precursor state, thus providing a time scale for the formation of H 3 + .…”

Section: Resultsmentioning

confidence: 99%

Mechanisms and time-resolved dynamics for trihydrogen cation (H3 +) formation from organic molecules in strong laser fields

Ekanayake

Nairat

Kaderiya

et al. 2017

Sci Rep

101

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Strong-field laser-matter interactions often lead to exotic chemical reactions. Trihydrogen cation formation from organic molecules is one such case that requires multiple bonds to break and form. We present evidence for the existence of two different reaction pathways for H3 + formation from organic molecules irradiated by a strong-field laser. Assignment of the two pathways was accomplished through analysis of femtosecond time-resolved strong-field ionization and photoion-photoion coincidence measurements carried out on methanol isotopomers, ethylene glycol, and acetone. Ab initio molecular dynamics simulations suggest the formation occurs via two steps: the initial formation of a neutral hydrogen molecule, followed by the abstraction of a proton from the remaining CHOH2+ fragment by the roaming H2 molecule. This reaction has similarities to the H2 + H2 + mechanism leading to formation of H3 + in the universe. These exotic chemical reaction mechanisms, involving roaming H2 molecules, are found to occur in the ~100 fs timescale. Roaming molecule reactions may help to explain unlikely chemical processes, involving dissociation and formation of multiple chemical bonds, occurring under strong laser fields.

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Section: Resultsmentioning

confidence: 99%

Mechanisms and time-resolved dynamics for trihydrogen cation (H3 +) formation from organic molecules in strong laser fields

Ekanayake

Nairat

Kaderiya

et al. 2017

Sci Rep

101

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“…Tellingly, the high-KER peaks in the D + + D 2 and D + D + 2 channels are absent for circular polarization, strongly supporting the supposition that they are from FTI. Since FTI is present for two-body dissociation, it can also be expected for the threebody channel D + + D + D. Despite the poorer statistics for this channel due to the low threebody dissociation rate (see [29,32]), the KER distribution in figure 8 for linearly polarized 7 fs pulses displays an unmistakable peak at large KER around 10 eV that resembles the D + + D + + D channel (note the peak at lower KER around 2 eV is likely to be from regular dissociation pathways by multiphoton excitation). As indicated by the inset, the high-KER peak for D + + D + D seems to be suppressed using circularly polarized pulses consistent with its origin arising from FTI.…”

Section: Further Signs Of Ftimentioning

confidence: 99%

“…Moreover, the probability of FTI is substantial, particularly for longer pulses. Indeed, the study of the intense field fragmentation of D + 3 (H + 3 ) is a substantial achievement in itself as this milestone has only recently been reached [29][30][31][32]. The large interest in H + 3 stems from the fact that it is the simplest stable polyatomic molecule, is of fundamental interest [33,34], and is viewed by many as a gateway to better understanding the dynamics of multi-centre systems in intense lasers (for some theoretical H + 3 and H 2+ 3 strong-field studies, see [35][36][37][38][39][40][41][42][43][44][45][46]).…”

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Frustrated tunnelling ionization during strong-field fragmentation of D₃⁺

et al. 2012

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We reveal surprisingly high kinetic energy release in the intense-field fragmentation of D + 3 to D + + D + + D with 10 16 W cm −2 , 790 nm, 40 fs (and 7 fs) laser pulses. This feature strongly mimics the behaviour of the D + + D + + D + channel. From the experimental evidence, we conclude that the origin of the feature is due to frustrated tunnelling ionization, the first observation of this mechanism in a polyatomic system. Furthermore, we unravel evidence of frustrated tunnelling ionization in dissociation, both two-body breakup to D + D + 2 and D + + D 2 , and three-body breakup to D + + D + D. Gesellschaft processes involving either elastic scattering [6][7][8], inelastic scattering [9, 10], or electron-ion recombination [11]. These phenomena have led to the birth of new areas of research such as high-harmonic generation and attosecond science [12][13][14][15], laser-driven electron diffraction imaging [5][6][7][8], molecular orbital tomography [16,17] and electron wavepacket probing of molecular dynamics [18-21]-naming only a few.Related to the electron recollision process, recently Nubbemeyer et al [22] reported a new phenomenon dubbed frustrated tunnelling ionization (FTI). Demonstrated originally in strong-field ionization of helium, Nubbemeyer et al showed that an electron wavepacket that starts to tunnel away from the core in an intense laser field, but fails to acquire sufficient drift momentum to escape the attractive potential of the remaining He + ion, can be captured into an excited Rydberg orbital of the He atom-in effect 'frustrating' the tunnel ionization process. This process must occur during the laser pulse to conserve energy and momentum, most likely during the trailing edge, as the electron is gently decelerated over many laser cycles before being pulled into orbit.The same mechanism has been observed in the dissociative ionization of a few diatomic molecules (H 2 [23], D 2 [24], O 2 [25] and Ar 2 [26][27][28]). For such molecules, following ionization, an electron that is excited to the continuum and driven by the laser field tends to be captured to a Rydberg orbital of one of the two 'Coulomb-exploding' fragment ions. The signature of frustrated tunnelling in molecules is that, counterintuitively, the final kinetic energy release (KER) is similar to that of a Coulomb explosion event even though only one product fragment is charged while the other fragment is neutral [23].This description of FTI uses language, such as electron capture, that is usually reserved for discussions involving ionization. Throughout the paper we use this language for convenience. However, it does pose an interesting question in relation to the actual mechanism for FTI, that is,

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“…15 in Ref. [54], a Dalitz plot showing the energy sharing of the (D 3+ 3 → D + + D + + D + ) fragments resulting from Coulomb explosion, taken at face value, could lead one to erroneous conclusions about the initial configuration as will be discussed below. Moreover, although the classical problem is unique and time-reversal invariant given a simultaneous determination of the exact time, position, and momentum upon impact at the detector, typical measurements only determine the position and time of the particle impacts and infer the momentum from this.…”

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confidence: 97%

“…assumed to not play a role, and the initial momenta of the protons are assumed to be zero. This system is ideal since (i) the ground state of the initial molecule, H + 3 , is an equilateral triangle [57], (ii) the force between the fragments is pure Coulomb repulsion, 1/R 2 ij , and (iii) the molecule is important as a benchmark for molecular interactions and calculations [53,54,[58][59][60][61][62] and plays a central role in interstellar chemistry [63][64][65].…”

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confidence: 99%