arXiv subjects

John A. McGuire

Publications and source records attributed to John A. McGuire.

6 recordsLinked to original sources

arXiv2025

Orientation- and pressure-dependence of the vibrational response of a monolayer crystal on a vicinal diamond surface

We systematically investigate polarization-dependent Raman spectra of a monolayer crystal of WS2 on the (100) and (230) surfaces of diamond. At ambient pressure, identical polarization dependence of the Raman spectra is observed on the different surfaces, independent of the orientation of the monolayer crystal relative to the diamond crystal. However, when monolayer WS2 is compressed to about 4 GPa, an abrupt drop of the intensity of the 2LA mode relative to the A' mode occurs on the (100) surface and the (230) surface with the zigzag direction along the atomic step edges of the (230) surface. In contrast, no such drop is observed when the armchair direction is along or at 15° to the atomic steps of the (230) surface. We also observe a shift of the polarization angle of the intensity maxima of the 2LA and A' modes on (230) surface during compression. These results demonstrate that the atomic steps of a vicinal surface strongly modify the vibrational response under high pressure.

cond-mat.mtrl-sci↗

arXiv2017

Optical Stark metrology of CdSe quantum dots: Reconciling the size-dependent oscillator strength with theory

The $k\cdot p$ effective mass approximation (EMA) predicts large, nearly size-independent exciton oscillator strengths in quantum confined semiconductors. Yet, experimental reports have concluded that the total oscillator strength of the lowest-energy (1S$_{3/2}$1S$_{\text{e}}$) excitons in strongly confined CdSe NQDs is small and strongly size-dependent. Using the optical Stark effect, we show that the oscillator strength of the 1S$_{3/2}$1S$_{\text{e}}$ excitonic absorption peak in CdSe NQDs follows the predictions of the EMA. These oscillator strengths enable helicity-selective unsaturated Stark shifts corresponding to femtosecond pseudo-magnetic fields exceeding 100 T.

cond-mat.mes-hall↗

arXiv2016

Layer- and Frequency-Dependent Second Harmonic Generation in Reflection from GaSe Atomic Crystals

We report optical second-harmonic generation (SHG) in reflection from GaSe crystals of 1 to more than 100 layers using a fundamental picosecond pulsed pump at 1.58 eV and a supercontinuum white light pulsed laser with energies ranging from 0.85 to 1.4 eV. The measured reflected SHG signal is maximal in samples of $\sim$20 layers, decreasing in thicker samples as a result of interference. The thickness- and frequency-dependence of the SHG response of samples thicker than $\sim$7 layers can be reproduced by a second-order optical susceptibility that is the same as in bulk samples. For samples $\lesssim$7 layers, the second-order optical susceptibility is reduced compared to that in thicker samples, which is attributed to the expected bandgap increase in mono- and few-layer GaSe.

cond-mat.mes-hall↗

arXiv2015

Exciton spin dynamics in GaSe

We analyze exciton spin dynamics in GaSe under nonresonant circularly polarized optical pumping with an exciton spin-flip rate-equation model. The model reproduces polarized time-dependent photoluminescence measurements in which the initial circular polarization approaches unity even when pumping with 0.15 eV excess energy. At T = 10 K, the exciton spin relaxation exhibits a biexponential decay with a sub-20 ps and a >500 ps time constants, which are also reproduced by the rate-equation model assuming distinct spin-relaxation rates for hot (nonequilibrium) and cold band-edge excitons.

cond-mat.mes-hall↗

arXiv2015

Linearly polarized remote-edge luminescence in GaSe nanoslabs

We report highly linearly polarized remote luminescence that emerges at the cleaved edges of nanoscale gallium selenide slabs tens of micrometers away from the optical excitation spot. The remote-edge luminescence (REL) measured in the reflection geometry has a degree of linear polarization above 0.90, with polarization orientation pointing toward the photoexcitation spot. The REL is dominated by an index-guided optical mode that is linearly polarized along the crystalline $c$-axis. This luminescence is from out-of-plane dipoles that are converted from in-plane dipoles through a spin-flip process at the excitation spot.

cond-mat.mes-hall↗

arXiv2014

Near Unity Optical Spin Polarization in GaSe Nanoslabs

We report nearly complete preservation of "spin memory" between optical absorption and photoluminescence (PL) in nanometer slabs of GaSe pumped with 0.2 eV excess energy. At cryogenic temperatures, the initial degree of circular polarization ($ρ_0$) of PL approaches unity, with the major fraction of the spin polarization decaying with a time constant $>$500 ps in sub-100-nm GaSe nanoslabs. Even at room temperature, $ρ_0$ as large as 0.7 is observed, while pumping 1 eV above the band edge yields $ρ_0$ = 0.15. Angular momentum preservation for both electrons and holes is due to the separation of the non-degenerate conduction and valence bands from other bands. In contrast to valley polarization in atomically thin TMDs, here optical spin polarization is preserved in nanoslabs of 100 layers or more of GaSe.

cond-mat.mes-hall↗