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1.
J Phys Chem Lett ; : 5265-5270, 2019 Aug 27.
Artigo em Inglês | MEDLINE | ID: mdl-31434481

RESUMO

Time-resolved pump-probe photoemission spectroscopy has been used to study the dynamics of charge-carrier recombination and trapping on hydroxylated rutile TiO2(110). Two types of pump excitation were employed, one in the infrared (IR) (0.95 eV) and the other in the ultraviolet (UV) (3.5 eV) region. With IR excitation, electrons associated with defects are excited into the bottom of the conduction band from the polaronic states within the band gap, which are retrapped within 45 ± 10 fs. Under UV excitation, the electrons in these band-gap states (BGSs) and valence-band electrons are excited into the conduction band. In addition to the fast polaron trapping observed with IR excitation, we also observe a long lifetime (∼1 ps) component for both the depletion of hot electrons at the bottom of the conduction band and the refilling of the BGS. This points to a BGS-mediated recombination process with a picosecond lifetime.

2.
Phys Chem Chem Phys ; 21(21): 11142-11149, 2019 Jun 07.
Artigo em Inglês | MEDLINE | ID: mdl-31094379

RESUMO

The dissociation dynamics of CH3I is investigated on the red (269 nm) and blue (255 nm) side of the absorption maximum of the A-band. Using a multiphoton ionisation probe in a time-resolved photoelectron imaging experiment we observe very different dynamics at the two wavelengths, with significant differences in the measured lifetime and dynamic structure. The differences are explained in terms of changes in excitation cross-sections of the accessible 3Q0 and 1Q1 states and the subsequent dynamics upon each of them. The measurements support the existing literature on the rapid dissociation dynamics on the red side of the absorption maximum at 269 nm which is dominated by the dynamics along the 3Q0 state. At 255 nm we observe similar dynamics along the 3Q0 state but also a significant contribution from the 1Q1 state. The dynamics along the 1Q1 potential show a more complex structure in the photoelectron spectrum and a significantly increased lifetime, indicative of a more complex reaction pathway.

3.
Phys Rev Lett ; 120(18): 183003, 2018 May 04.
Artigo em Inglês | MEDLINE | ID: mdl-29775354

RESUMO

We probe the dynamics of dissociating CS_{2} molecules across the entire reaction pathway upon excitation. Photoelectron spectroscopy measurements using laboratory-generated femtosecond extreme ultraviolet pulses monitor the competing dissociation, internal conversion, and intersystem crossing dynamics. Dissociation occurs either in the initially excited singlet manifold or, via intersystem crossing, in the triplet manifold. Both product channels are monitored and show that, despite being more rapid, the singlet dissociation is the minor product and that triplet state products dominate the final yield. We explain this by a consideration of accurate potential energy curves for both the singlet and triplet states. We propose that rapid internal conversion stabilizes the singlet population dynamically, allowing for singlet-triplet relaxation via intersystem crossing and the efficient formation of spin-forbidden dissociation products on longer timescales. The study demonstrates the importance of measuring the full reaction pathway for defining accurate reaction mechanisms.

4.
Phys Chem Chem Phys ; 18(40): 28150-28156, 2016 Oct 12.
Artigo em Inglês | MEDLINE | ID: mdl-27722319

RESUMO

The dissociation dynamics of the Ã-state of ammonia have been studied using a resonant multiphoton ionisation probe in a photoelectron spectroscopy experiment. The use of a resonant intermediate in the multiphoton ionisation process changes the ionisation propensity, allowing access to different ion states when compared with equivalent single photon ionisation experiments. Ionisation through the E' 1A1' Rydberg intermediate means we maintain overlap with the ion state for an extended period, allowing us to monitor the excited state population for several hundred femtoseconds. The vibrational states in the photoelectron spectrum show two distinct timescales, 200 fs and 320 fs, that we assign to the non-adiabatic and adiabatic dissociation processes respectively. The different timescales derive from differences in the wavepacket trajectories for the two dissociation pathways that resonantly excite different vibrational states in the intermediate Rydberg state. The timescales are similar to those obtained from time resolved ion kinetic energy release measurements, suggesting we can measure the different trajectories taken out to the region of conical intersection.

5.
ACS Nano ; 10(6): 6315-22, 2016 06 28.
Artigo em Inglês | MEDLINE | ID: mdl-27267820

RESUMO

The electronic structure of two-dimensional (2D) semiconductors can be significantly altered by screening effects, either from free charge carriers in the material or by environmental screening from the surrounding medium. The physical properties of 2D semiconductors placed in a heterostructure with other 2D materials are therefore governed by a complex interplay of both intra- and interlayer interactions. Here, using time- and angle-resolved photoemission, we are able to isolate both the layer-resolved band structure and, more importantly, the transient band structure evolution of a model 2D heterostructure formed of a single layer of MoS2 on graphene. Our results reveal a pronounced renormalization of the quasiparticle gap of the MoS2 layer. Following optical excitation, the band gap is reduced by up to ∼400 meV on femtosecond time scales due to a persistence of strong electronic interactions despite the environmental screening by the n-doped graphene. This points to a large degree of tunability of both the electronic structure and the electron dynamics for 2D semiconductors embedded in a van der Waals-bonded heterostructure.

6.
Nano Lett ; 15(9): 5883-7, 2015 Sep 09.
Artigo em Inglês | MEDLINE | ID: mdl-26315566

RESUMO

The dynamics of excited electrons and holes in single layer (SL) MoS2 have so far been difficult to disentangle from the excitons that dominate the optical response of this material. Here, we use time- and angle-resolved photoemission spectroscopy for a SL of MoS2 on a metallic substrate to directly measure the excited free carriers. This allows us to ascertain a direct quasiparticle band gap of 1.95 eV and determine an ultrafast (50 fs) extraction of excited free carriers via the metal in contact with the SL MoS2. This process is of key importance for optoelectronic applications that rely on separated free carriers rather than excitons.

7.
J Phys Condens Matter ; 27(16): 164206, 2015 Apr 29.
Artigo em Inglês | MEDLINE | ID: mdl-25835249

RESUMO

In order to exploit the intriguing optical properties of graphene it is essential to gain a better understanding of the light-matter interaction in the material on ultrashort timescales. Exciting the Dirac fermions with intense ultrafast laser pulses triggers a series of processes involving interactions between electrons, phonons and impurities. Here we study these interactions in epitaxial graphene supported on silicon carbide (semiconducting) and iridium (metallic) substrates using ultrafast time- and angle-resolved photoemission spectroscopy (TR-ARPES) based on high harmonic generation. For the semiconducting substrate we reveal a complex hot carrier dynamics that manifests itself in an elevated electronic temperature and an increase in linewidth of the π band. By analyzing these effects we are able to disentangle electron relaxation channels in graphene. On the metal substrate this hot carrier dynamics is found to be severely perturbed by the presence of the metal, and we find that the electronic system is much harder to heat up than on the semiconductor due to screening of the laser field by the metal.

8.
Chem Sci ; 6(3): 1614-1629, 2015 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-29308130

RESUMO

Electronic Laboratory Notebooks (ELNs) are progressively replacing traditional paper books in both commercial research establishments and academic institutions. University researchers require specific features from ELNs, given the need to promote cross-institutional collaborative working, to enable the sharing of procedures and results, and to facilitate publication. The LabTrove ELN, which we use as our exemplar, was designed to be researcher-centric (i.e., not only aimed at the individual researcher's basic needs rather than to a specific institutional or subject or disciplinary agenda, but also able to be tailored because it is open source). LabTrove is being used in a heterogeneous set of academic laboratories, for a range of purposes, including analytical chemistry, X-ray studies, drug discovery and a biomaterials project. Researchers use the ELN for recording experiments, preserving data collected, and for project coordination. This perspective article describes the experiences of those researchers from several viewpoints, demonstrating how a web-based open source electronic notebook can meet the diverse needs of academic researchers.

9.
Nano Lett ; 15(1): 326-31, 2015 Jan 14.
Artigo em Inglês | MEDLINE | ID: mdl-25458168

RESUMO

Time- and angle-resolved photoemission measurements on two doped graphene samples displaying different doping levels reveal remarkable differences in the ultrafast dynamics of the hot carriers in the Dirac cone. In the more strongly (n-)doped graphene, we observe larger carrier multiplication factors (>3) and a significantly faster phonon-mediated cooling of the carriers back to equilibrium compared to in the less (p-)doped graphene. These results suggest that a careful tuning of the doping level allows for an effective manipulation of graphene's dynamical response to a photoexcitation.

10.
Faraday Discuss ; 171: 195-218, 2014.
Artigo em Inglês | MEDLINE | ID: mdl-25415646

RESUMO

We show that rotational line spectra of molecular clusters with near zero permanent dipole moments can be observed using impulsive alignment. Aligned rotational wavepackets were generated by non-resonant interaction with intense femtosecond laser pump pulses and then probed using Coulomb explosion by a second, time-delayed femtosecond laser pulse. By means of a Fourier transform a rich spectrum of rotational eigenstates was derived. For the smallest cluster, C(2)H(2)-He, we were able to establish essentially all rotational eigenstates up to the dissociation threshold on the basis of theoretical level predictions. The C(2)H(2)-He complex is found to exhibit distinct features of large amplitude motion and very early onset of free internal rotor energy level structure.

11.
Phys Rev Lett ; 113(4): 043004, 2014 Jul 25.
Artigo em Inglês | MEDLINE | ID: mdl-25105616

RESUMO

Rotational wave packets of the weakly bound C(2)H(2)-He complex have been created using impulsive alignment. The coherent rotational dynamics were monitored for 600 ps enabling extraction of a frequency spectrum showing multiple rotational energy levels up to J = 4. spectrum has been combined with ab initio calculations to show that the complex has a highly delocalized structure and is bound only by ca. 7 cm(-1). The experiments demonstrate how highly featured rotational spectra can be obtained from an extremely cold environment where only the lowest rotational energy states are initially populated.

12.
Opt Express ; 19(10): 9801-6, 2011 May 09.
Artigo em Inglês | MEDLINE | ID: mdl-21643236

RESUMO

Gas jets used as sources for high harmonic generation (HHG) have a complex three-dimensional density and velocity profile. This paper describes how the profile influences the generation of extreme-UV light. As the position of the laser focus is varied along the jet flow axis, we show that the intensity of the output radiation varies by approximately three times, with the highest flux being observed when the laser is focused into the Mach disc. The work demonstrated here will aid in the optimization of HHG flux from gas jet sources. The flux increase is attributed to a density increase within the structure of the jet, which is confirmed by simultaneous imaging of atom and ion fluorescence from the jet.

13.
Opt Express ; 18(12): 13279-84, 2010 Jun 07.
Artigo em Inglês | MEDLINE | ID: mdl-20588457

RESUMO

Accurate three-dimensional modelling of nonlinear pulse propagation within a gas-filled capillary is essential for understanding and improving the XUV yield in high harmonic generation. We introduce both a new model based on a multimode generalized nonlinear Schrödinger equation and a novel spatio-spectral measurement technique to which the model can be compared. The theory shows excellent agreement with the measured output spectrum and the spatio-spectral measurement reveals that the model correctly predicts higher order mode contributions to spectral broadening of the pulse. Fluorescence from the excited argon is used to verify the predicted ion distribution along the capillary.

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