Soroush Khosravi Dehaghi,
Department of Physics,
University of Connecticut

Femtosecond Laser Transient Spectroscopy of Carotenoids and Carbon Nanotubes

Carotenoids and semiconducting single-wall carbon nanotubes, which are both nanoscale carbon-based quantum mechanical systems, were studied using different optical spectroscopy techniques.

The lifetime of the S\(_2\) excited state of the carotenoids were estimated using a model-based lifetime analysis routine. It was found that the addition of a conjugated carbonyl group to the carotenoid has several crucial effects on the optical response due to the alteration of the delocalized conjugated \(\pi\) molecular orbital of the molecule. These effects include the shortening of the lifetimes of the excited states, the change in the decay mechanism from the S\(_2\) excited state to the S\(_1\) excited state, and the unresolved vibrational peaks in the steady-state absorption spectrum.

The decay of the E\(_{22}\) excited state of (6,5) semiconducting carbon nanotube dispersed in flavin mononucleotide with water was observed using transient grating spectroscopy. The lifetime of this excited state was estimated to be 450 ± 50 fs. A very strong single-frequency oscillatory component was observed in the transient grating decay profile.

Electric Form Factor of the Neutron from Asymmetry Measurements

Field of Study: Physics

Jonathan Kwolek,
Department of Physics,
University of Connecticut

Studying Charge Exchange in a Hybrid Ion-neutral Trap


Interactions between neutral and ionized atoms are medium-range, and the spiraling nature of these collisions can lead to long interaction times and large cross sections. The field of ion-neutral interactions is bolstered by methods from atomic physics, which allow us to accurately control and determine the quantum-states of the reactants. Atomic physics opens the door to studying these interactions over a large range of energies, in order to observe interesting effects from the ultracold to hot temperature regimes.

The hybrid-trap enables the concentric trapping of a sample of cold atoms and ions. The dissertation discusses our exploration into the controlled reactions in the Na+Ca^+ system, including measurements of sympathetic cooling and a charge-exchange rate which changes as a function of energy and atomic state. The quantum-state distributions of Na in our magneto-optical trap is also explored, as well as its agreement and subsequent deviation based on a predictive model. The measurements of reaction rates indicate a reaction-energy threshold in two different reaction channels, which can be corroborated by theoretical investigation.

Dale L Smith, Department of Physics, University of Connecticut

Velocity Map Imaging of the Single Ionization of
Molecular Iodine

Single ionization in molecules is a critical first step in many higher order process such as high harmonic generation. However, single ionization remains poorly understood even in simple diatomic systems. We have found that molecular iodine, I2, has a complicated ionization processes which does not originate from valance orbitals, as would be expected, but from more tightly bound inner orbitals comprised of 5s electrons. I will discuss two experiments which use ultrafast lasers to investigate the ionization of diatomic I2. Ultrafast laser pulses have a duration in the tens of femtoseconds (fs). Since the vibrational period of I2 is ≈180 fs, we are able to ionize the molecule before it dissociates. Velocity map imaging allows us to observe the kinetic energy release (KER) of charged fragments from dissociation after single ionization. In the first experiment, we have performed a wavelength study from 800 to 400 nm. We have found in the I + I+ dissociation channel (which we denote as the (1,0)) the KER of the fragments was mostly inconsistent with ionization to the X-, A-, or B-states of I2+ which implies ionization through deeper orbitals. A pump-probe Fourier technique also showed that modulation in the cation products only occurs below 0.2 eV, which is consistent with dissociation through the B-state and ionization of high-lying molecular orbitals. This rules out a two-step process through the X- and A-states for much of the observed KER. Employing intensity-, polarization-, and wavelength-dependent experiments we were able to eliminate bond softening, electron rescattering, and photon mediation through the X- or A-states. In the second experiment, we performed a detailed wavelength analysis of I2 around its one-photon B-state resonance at 530 nm where we have identified a strong enhancement in the (1,0) channel. The resonance enhancement is found in both ionization from outer orbitals through the B-state as well as ionization from inner orbitals. Interestingly, the branching ratio for inner orbital ionization reaches over 98% at 519 nm and the peaks in the branching ratios of the two channels occur at slightly different wavelengths. For double ionization into an excited state of I2+ we find that the branching ratio closely follows the branching ratio of the single ionization of deeply bound inner orbitals. This implies that excitation of molecules comes about through inner orbital ionization. The finding of these experiments are inconsistent with current tunneling ionization theory which postulates that ionization arises through the least bound, outer orbital electrons.