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Esry, B. D.

Publications and source records attributed to Esry, B. D..

12 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Native frames: An approach for separating sequential and concerted three-body fragmentation

Disentangling sequential and concerted three-body fragmentation has been a longstanding endeavor in studies of molecular dynamics. To accomplish this goal, we recently introduced a novel method to separate sequential from concerted breakup, where the sequential events are analyzed in their native frames [J. Rajput et al., Phys. Rev. Lett. 120, 103001 (2018)]. The essence of this method is the use of the Jacobi coordinates' conjugate momenta to reduce the dimensionality of the multibody fragmentation in combination with a clear signature for sequential breakup. To demonstrate this method, we employ coincidence momentum imaging to study the strong-field dissociative ionization of OCS into O + +C + + S + , which typically undergoes concerted fragmentation or sequential breakup involving either a metastable CO 2+ or CS 2+ molecule. We identify sequential breakup using a uniform distribution as a function of the angle between the conjugate momenta, associated with the first and second fragmentation steps, which is due to the rotation of the intermediate molecule in the fragmentation plane. Furthermore, by exploiting this uniform distribution, we separate the sequential and concerted distributions in any plot created from the measured momenta.

Atomic & molecular processes in external fields↗
DOE OSTI2022

Direct evidence of the dominant role of multiphoton permanent-dipole transitions in strong-field dissociation of NO 2 +

We study laser-induced dissociation of a metastable NO 2+ ion-beam target into N + +O + , focusing on the prominent contribution by molecules breaking parallel to the polarization at high peak laser intensity (~10 15 W/cm 2 ). Our experimental results and time-dependent Schrödinger equation calculations show that, contrary to commonly held intuition that electronic transitions always prevail, the dominant process underlying this highly aligned dissociation is a multiphoton permanent-dipole transition involving only the electronic ground state and leading to its vibrational continuum. Strong-field permanent-dipole transitions should thus be considered generally, as they may play a significant role in other heteronuclear molecules. Moreover, their role should only grow in importance for longer wavelengths, a trending direction in ultrafast laser studies.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Importance of one- and two-photon transitions in the strong-field dissociation of NO 2+

Employing a coincidence three-dimensional momentum imaging technique, we investigate the ultrafast, intense laser-induced dissociation of a metastable NO 2+ ion beam into N + + O + . Based on the kinetic energy release and angular distributions, measured using both 774-nm and second-order-harmonic 387-nm pulses, we show that the main processes driving dissociation in pulses of about 10 14 W/cm 2 peak intensity are one- and two-photon transitions from the X 2 Σ + ground state to the A 2 Π first-excited state. First-order perturbation theory calculations also corroborate these findings.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2019

Bond rearrangement during Coulomb explosion of water molecules

Bond rearrangement, namely the dissociation of water ions into H 2 + + (q – 1)+ (q = 1–4) following fast ion-impact ionization, unexpectedly occurs following multiple ionization of water in spite of the presumably fast “Coulomb explosion” of the transient molecular ion. Furthermore, the branching ratio of bond rearrangement is found to be nearly equal for each level of ionization, q. In addition, formation of H 2 + is more than twice as likely to occur from the lighter water isotopologue H 2 O + than D 2 + from D 2 O + . Furthermore, these findings are consistent with the ground state dissociation mechanism in which a fast projection of the ground state nuclear wave function onto the vibrational continuum of the cation potential energy surface is sometimes followed by H 2 + formation.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2018

Nonunique and nonuniform mapping in few-body Coulomb-explosion imaging

Much of our knowledge of molecular geometry and interaction dynamics comes from indirect measurements of the molecular fragments following breakup. This technique—Coulomb-explosion imaging (CEI), i.e., determining the initial molecular configuration of a system from the momenta of the resulting fragments using knowledge of the particle interactions—is one of the fundamental tools of molecular physics. Moreover, CEI has been a staple of molecular studies for decades. Here we show that one often cannot assign a unique initial configuration to the few-body breakup of a polyatomic molecule given the measurement of the resulting fragments' momenta. Specifically, multiple initial configurations can result in identical momenta for a molecule breaking into three or more parts. Finally, the nonunique and nonuniform mapping from the initial configuration to the measured momenta also significantly complicates the determination of molecular alignment at the time of breakup.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2017

Using the carrier-envelope phase to control strong-field dissociation of $\mathrm{HeH^+}$ at midinfrared wavelengths

We study the response of HeH + to an intense, few-cycle laser pulse. Specifically, we present the carrier-envelope phase (CEP) dependence of the kinetic-energy-release spectrum, the spatial asymmetry, and the total dissociation probability in two-cycle pulses with an intensity of 10 14 W/cm 2 and wavelengths of 3200 and 4000 nm. Strong spatial asymmetries are found in spite of the fact that the electron always becomes localized as He+H + , demonstrating that control of such asymmetries can be obtained via control of the nuclear degrees of freedom—as opposed to its usual interpretation as control over the electronic degrees of freedom. Finally, we explain these CEP effects in terms of our photon-phase representation.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2011

Frustrated tunneling ionization during laser-induced D{sub 2} fragmentation: Detection of excited metastable D{sup *} atoms

In a recent Letter, Manschwetus et al.[Phys. Rev. Lett. 102, 113002 (2009)] reported evidence of electron recapture during strong-field fragmentation of H{sub 2}--explained using a frustrated tunneling ionization model. Unusually, the signature of this process was detection of excited H{sup *} atoms. We report here an extensive study of this process in D{sub 2}. Our measurements encompass a study of the pulse duration, intensity, ellipticity, and angular distribution dependence of D{sup *} formation. While we find that the mechanism suggested by Manschwetus et al. is consistent with our experimental data, our theoretical work shows that electron recollision excitation cannot be completely ruled out as an alternative mechanism for D{sup *} production.

74 ATOMIC AND MOLECULAR PHYSICS↗