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1.
Nanoscale ; 12(45): 22904-22916, 2020 Nov 26.
Artigo em Inglês | MEDLINE | ID: mdl-33185228

RESUMO

Among the layered two dimensional semiconductors, molybdenum disulfide (MoS2) is considered to be an excellent candidate for applications in optoelectronics and integrated circuits due to its layer-dependent tunable bandgap in the visible region, high ON/OFF current ratio in field-effect transistors (FET) and strong light-matter interaction properties. In this study, using multi-terminal measurements, we report high broadband photocurrent response (R) and external quantum efficiency (EQE) of few-atomic layered MoS2 phototransistors fabricated on a SiO2 dielectric substrate and encapsulated with a thin transparent polymer film of Cytop. The photocurrent response was measured using a white light source as well as a monochromatic light of wavelength λ = 400 nm-900 nm. We measured responsivity using a 2-terminal configuration as high as R = 1 × 103 A W-1 under white light illumination with an optical power Popt = 0.02 nW. The R value increased to 3.5 × 103 A W-1 when measured using a 4-terminal configuration. Using monochromatic light on the same device, the measured values of R were 103 and 6 × 103 A W-1 under illumination of λ = 400 nm when measured using 2- and 4-terminal methods, respectively. The highest EQE values obtained using λ = 400 nm were 105% and 106% measured using 2- and 4-terminal configurations, respectively. The wavelength dependent responsivity decreased from 400 nm to the near-IR region at 900 nm. The observed photoresponse, photocurrent-dark current ratio (PDCR), detectivity as a function of applied gate voltage, optical power, contact resistances and wavelength were measured and are discussed in detail. The observed responsivity is also thoroughly studied as a function of contact resistance of the device.

2.
Rev Sci Instrum ; 90(6): 063901, 2019 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-31255018

RESUMO

We performed nonlinear optical two-dimensional Fourier transform spectroscopy measurements using an optical resistive high-field magnet on GaAs quantum wells. Magnetic fields up to 25 T can be achieved using the split helix resistive magnet. Two-dimensional spectroscopy measurements based on the coherent four-wave mixing signal require phase stability. Therefore, these measurements are difficult to perform in environments prone to mechanical vibrations. Large resistive magnets use extensive quantities of cooling water, which causes mechanical vibrations, making two-dimensional Fourier transform spectroscopy very challenging. Here, we report on the strategies we used to overcome these challenges and maintain the required phase-stability throughout the measurement. A self-contained portable platform was used to set up the experiments within the time frame provided by a user facility. Furthermore, this platform was floated above the optical table in order to isolate it from vibrations originating from the resistive magnet. Finally, we present two-dimensional Fourier transform spectra obtained from GaAs quantum wells at magnetic fields up to 25 T and demonstrate the utility of this technique in providing important details, which are obscured in one dimensional spectroscopy.

3.
Nat Commun ; 9(1): 3720, 2018 09 13.
Artigo em Inglês | MEDLINE | ID: mdl-30213976

RESUMO

We present time-integrated four-wave mixing measurements on monolayer MoSe2 in magnetic fields up to 25 T. The experimental data together with time-dependent density function theory calculations provide interesting insights into the biexciton formation and dynamics. In the presence of magnetic fields the coherence at negative and positive time delays is dominated by intervalley biexcitons. We demonstrate that magnetic fields can serve as a control to enhance the biexciton formation and help search for more exotic states of matter, including the creation of multiple exciton complexes and excitonic condensates.

4.
Rev Sci Instrum ; 89(7): 073901, 2018 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-30068119

RESUMO

We describe the development of a broadband (0.3-10 THz) optical pump-terahertz probe spectrometer with an unprecedented combination of temporal resolution (≤200 fs) operating in external magnetic fields as high as 25 T using the new Split Florida-Helix magnet system. Using this new instrument, we measure the transient dynamics in a gallium arsenide four-quantum well sample after photoexcitation at 800 nm.

5.
Phys Rev Lett ; 104(11): 117401, 2010 Mar 19.
Artigo em Inglês | MEDLINE | ID: mdl-20366499

RESUMO

We present experimental coherent two-dimensional Fourier-transform spectra of Wannier exciton resonances in semiconductor quantum wells generated by a pulse sequence that isolates two-quantum coherences. By measuring the real part of the signals, we determine that the spectra are dominated by two-quantum coherences due to mean-field many-body interactions, rather than bound biexcitons. Simulations performed using dynamics controlled truncation agree with the experiments.

6.
Acc Chem Res ; 42(9): 1423-32, 2009 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-19555068

RESUMO

Coherent light-matter interactions of direct-gap semiconductor nanostructures provide a great test system for fundamental research into quantum electronics and many-body physics. The understanding gained from studying these interactions can facilitate the design of optoelectronic devices. Recently, we have used optical two-dimensional Fourier-transform spectroscopy to explore coherent light-matter interactions in semiconductor quantum wells. Using three laser pulses to generate a four-wave-mixing signal, we acquire spectra by tracking the phase of the signal with respect to two time axes and then Fourier transforming them. In this Account, we show several two-dimensional projections and demonstrate techniques to isolate different contributions to the coherent response of semiconductors. The low-temperature spectrum of semiconductor quantum wells is dominated by excitons, which are electron-hole pairs bound through Coulombic interactions. Excitons are sensitive to their electronic and structural environment, which influences their optical resonance energies and line widths. In near perfect quantum wells, a small fluctuation of the quantum well thickness leads to spatial localization of the center-of-mass wave function of the excitons and inhomogeneous broadening of the optical resonance. The inhomogeneous broadening often masks the homogeneous line widths associated with the scattering of the excitons. In addition to forming excitons, Coulombic correlations also form excitonic molecules, called biexcitons. Therefore, the coherent response of the quantum wells encompasses the intra-action and interaction of both excitons and biexcitons in the presence of inhomogeneous broadening. Transient four-wave-mixing studies combined with microscopic theories have determined that many-body interactions dominate the strong coherent response from quantum wells. Although the numerous competing interactions cannot be easily separated in either the spectral or temporal domains, they can be separated using two-dimensional Fourier transform spectroscopy. The most common two-dimensional Fourier spectra are S(I)(omega(tau),T,omega(t)) in which the second time period is held fixed. The result is a spectrum that unfolds congested one-dimensional spectra, separates excitonic pathways, and shows which excitons are coherently coupled. This method also separates the biexciton contributions and isolates the homogeneous and inhomogeneous line widths. For semiconductor excitons, the line shape in the real part of the spectrum is sensitive to the many-body interactions, which we can suppress by exploiting polarization selection rules. In an alternative two-dimensional projection, S(I)(tau,omega(Tau),omega(t)), the nonradiative Raman coherent interactions are isolated. Finally, we show S(III)(tau,omega(Tau),omega(t)) spectra that isolate the two-quantum coherences associated with the biexciton. These spectra reveal previously unobserved many-body correlations.

7.
Opt Express ; 16(22): 18017-27, 2008 Oct 27.
Artigo em Inglês | MEDLINE | ID: mdl-18958080

RESUMO

A combination of spatial interference patterns and spectral interferometry are used to find the global phase for non-collinear two-dimensional Fourier-transform (2DFT) spectra. Results are compared with those using the spectrally resolved transient absorption (STRA) method to find the global phase when excitation is with co-linear polarization. Additionally cross-linear polarized 2DFT spectra are correctly "phased" using the all-optical technique, where the SRTA is not applicable.

8.
J Phys Chem B ; 110(40): 19891-905, 2006 Oct 12.
Artigo em Inglês | MEDLINE | ID: mdl-17020375

RESUMO

Femtosecond two-dimensional infrared (2D IR) spectroscopy has been applied to study the conformations of a model dipeptide, N-acetyl-L-prolinamide (AcProNH2) in deuterated chloroform (CDCl3). Spectral features in the amide-I and -II regions are obtained by rephasing (R), nonrephasing (NR), and reverse photon echo (RPE) pulse sequences with two polarization conditions. The 2D spectra obtained by the RPE and NR sequences with (0, 0, 0, 0) polarization reveal new spectral features associated with the multiple conformers of AcProNH2 that are difficult to discern using R sequence and linear-IR spectroscopy. The high resolving power of the RPE sequence comes from destructive interference between the positive and negative peaks of nearby vibrators, similar to the NR sequence. The RPE response functions that are useful for 2D spectral simulations are evaluated, including the effects of vibrational frequency correlations. The 2D spectra obtained with (45, -45, 90, 0) polarization exhibit clear cross-peak patterns in the off-diagonal region for the R and RPE sequences but in the diagonal region for the NR sequence. These patterns, free from strong diagonal contributions, are crucial for structure determination. DFT calculations, normal-mode analysis, Hessian matrix reconstruction, and vibrational exciton Hamiltonian diagonalization yield molecular parameters needed for quantitative simulations of 2D spectra: angles between transition dipoles, coupling constants, and off-diagonal anharmonicities of the amide-I and -II modes are obtained for solvated trans-C7 and cis structures and for gas-phase trans conformers in the region of phi = -120 degrees to 0 degrees and psi = -100 degrees to 180 degrees in the Ramachandran space. Systematic simulations based on a 4:1 population ratio of the solvated trans-C7 and cis structures reproduce well the 2D spectral features obtained at both polarization conditions. However, better agreement between the experimental and simulated cross-peak patterns can be reached if the dihedral angles of the major trans conformer are close to (phi, psi) = (-80 degrees , 100 degrees ). Our results suggest that the major conformer of AcProNH2 in CDCl3 deviates from the gas-phase global minimum, the trans-C7 form, to an extended intermediate between the C7 and polyproline-II structure. These results are discussed in relationship with earlier findings obtained by NMR, transient IR studies, and MD simulations.


Assuntos
Modelos Moleculares , Conformação Molecular , Prolina/análogos & derivados , Espectrofotometria Infravermelho/métodos , Algoritmos , Clorofórmio/química , Simulação por Computador , Prolina/química , Vibração
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