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Register a new userUltrahigh-density spin-polarized H and D observed via magnetization quantum beats
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We measure nuclear and electron spin-polarized H and D densities of at least 10$^{19}, cm^{-3}$ with $sim$10 ns lifetimes, from the photodissociation of HBr and DI with circularly-polarized UV light pulses. This density is $sim$6 orders of magnitude higher than that produced by conventional continuous-production methods, and, surprisingly, at least 100 times higher than expected densities for this photodissociation method. We observe the hyperfine quantum beating of the H and D magnetization with a pick-up coil, i.e., the respective 0.7 and 3 ns periodic transfer of polarization from the electrons to the nuclei and back. The $rm{10^{19},cm^{-3}}$ spin-polarized H and D density is sufficient for laser-driven ion acceleration of spin polarized electrons, protons, or deuterons, the preparation of nuclear-spin-polarized molecules, and for the demonstration of spin-polarized D-T or D-$rm{{^3He}}$ laser fusion, for which a reactivity enhancement of $rm{sim50%}$ is expected.
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Recently, the production of ultrahigh-density (~10^{19}cm^{-3}) spin-polarized deuterium (SPD) atoms was demonstrated, from the photodissociation of deuterium iodide, but the upper density limit was not determined. Here, we present studies of spin-polarized hydrogen (SPH) densities up to 10^{20} cm^{-3}, by photodissociating 5 bar of hydrogen chloride with a focused 213 nm, 150 ps laser pulse. We extract the depolarization cross-section of hydrogen and chlorine atom collisions, which is the main depolarization mechanism at this high-density regime, to be {sigma}_{HCl} = 7(2) x 10^{-17}cm^2. We discuss the conditions under which the ultrahigh SPH and SPD densities can be reached, and the potential applications to ultrafast magnetometry, laser-ion acceleration, and tests of polarized nuclear fusion.
We present state-selective measurements on the NH$_2^{+}$ + H$^{+}$ and NH$^{+}$ + H$^{+}$ + H dissociation channels following single-photon double ionization at 61.5 eV of neutral NH$_{3}$, where the two photoelectrons and two cations are measured in coincidence using 3-D momentum imaging. Three dication electronic states are identified to contribute to the NH$_2^{+}$ + H$^{+}$ dissociation channel, where the excitation in one of the three states undergoes intersystem crossing prior to dissociation, producing a cold NH$_2^+$ fragment. In contrast, the other two states directly dissociate, producing a ro-vibrationally excited NH$_2^+$ fragment with roughly 1 eV of internal energy. The NH$^{+}$ + H$^{+}$ + H channel is fed by direct dissociation from three intermediate dication states, one of which is shared with the NH$_2^{+}$ + H$^{+}$ channel. We find evidence of autoionization contributing to each of the double ionization channels. The distributions of the relative emission angle between the two photoelectrons, as well as the relative angle between the recoil axis of the molecular breakup and the polarization vector of the ionizing field, are also presented to provide insight on both the photoionization and photodissociation mechanisms for the different dication states.
We present a detailed study of the nuclear quantum effects in H/D sticking to graphene, comparing classical, quantum and mixed quantum/classical simulations to results of scattering experiments. Agreement with experimentally derived sticking probabilities is improved when nuclear quantum effects are included using ring polymer molecular dynamics. Specifically, the quantum motion of the carbon atoms enhances sticking, showing that an accurate description of graphene phonons is important to capturing the adsorption dynamics. We also find an inverse H/D isotope effect arising from Newtonian mechanics.
We report measurements on the H$^{+}$ + H$^{+}$ fragmentation channel following direct single-photon double ionization of neutral NH$_{3}$ at 61.5 eV, where the two photoelectrons and two protons are measured in coincidence using 3-D momentum imaging. We identify four dication electronic states that contribute to H$^{+}$ + H$^{+}$ dissociation, based on our multireference configuration-interaction calculations of the dication potential energy surfaces. The extracted branching ratios between these four dication electronic states are presented. Of the four dication electronic states, three dissociate in a concerted process, while the fourth undergoes a sequential fragmentation mechanism. We find evidence that the neutral NH fragment or intermediate NH$^+$ ion is markedly ro-vibrationally excited. We also identify differences in the relative emission angle between the two photoelectrons as a function of their energy sharing for the four different dication states, which bare some similarities to previous observations made on atomic targets.
Quantum beats in nonlinear spectroscopy of molecular aggregates are often attributed to electronic phenomena of excitonic systems, while nuclear degrees of freedom are commonly included into models as overdamped oscillations of bath constituents responsible for dephasing. However, molecular systems are coupled to various high-frequency molecular vibrations, which can cause the spectral beats hardly distinguishable from those created by purely electronic coherences. Models containing damped, undamped and overdamped vibrational modes coupled to an electronic molecular transition are discussed in this paper in context of linear absorption and two-dimensional electronic spectroscopy. Analysis of different types of bath models demonstrates how do vibrations map onto two-dimensional spectra and how the damping strength of the coherent vibrational modes can be resolved from spectroscopic signals.
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