Multidimensional Coherent Spectroscopy of Semiconductors

Smallwood, Christopher L.; Cundiff, Steven T.

doi:10.1002/lpor.201800171

Cited by 59 publications

(39 citation statements)

References 147 publications

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“…In turns out that 3ω m is the first frequency for which P (3) contributes to all terms with no background from P (1) , so I(3ω m , τ ) is used to monitor the nonlinear response. Similar techniques have been used for pump probe experiments in collinear geometry [29,[46][47][48]. Data availability.…”

Section: Methodsmentioning

confidence: 99%

“…The experiments we report here reveal a hitherto unexplored mechanism for optical nonlinearity emerging for polaritonic excitations out of a two dimensional electron system (2DES) in the fractional quantum Hall (FQHE) regime. More specifically, using time resolved four-wave mixing (FWM) experiments [28,29], we find that polariton-polariton interactions U can be enhanced by more than an order of magnitude around the fractional state at filling factor ν = 2/5 as compared to other neighboring compressible states. The interplay between photonic excitations and a 2DES is an exciting field [30][31][32][33][34] with open problems, among others, concerning the relation between transport and optics [35][36][37] and the description of exciton-electron interactions in a magnetic field [10].We study a semiconductor heterostructure that features, at the center of an optical microcavity, a GaAs QW containing an electron system of density n e = 3 × 10 10 cm −2 (see Methods).…”

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confidence: 99%

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Nonlinear optics in the fractional quantum Hall regime

Knüppel

Ravets

Kroner

et al. 2019

Nature

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These authors contributed equally to this work.Engineering strong interactions between optical photons is a great challenge for quantum science. Envisioned applications range from the realization of photonic gates for quantum information processing [1] to synthesis of photonic quantum materials for investigation of strongly-correlated drivendissipative systems [2]. Polaritonics, based on the strong coupling of photons to atomic or electronic excitations in an optical resonator, has emerged as a promising approach to implement those tasks [3]. Recent experiments demonstrated the onset of quantum correlations in the exciton-polariton system [4,5], showing that strong polariton blockade [6] could be achieved if interactions were an order of magnitude stronger. Here, we report time resolved four-wave mixing experiments on a two-dimensional electron system embedded in an optical cavity [7], demonstrating that polariton-polariton interactions are strongly enhanced when the electrons are initially in a fractional quantum Hall state. Our experiments indicate that in addition to strong correlations in the electronic ground state, exciton-electron interactions leading to the formation of polaron polaritons [8-11] play a key role in enhancing the nonlinear optical response. Besides potential applications in realization of strongly interacting photonic systems, our findings suggest that nonlinear optical measurements could provide information about fractional quantum Hall states that is not accessible in linear optical response.Polaritons have recently attracted considerable interest, motivated by the fact that their interactions can be engineered almost at will through the tunability of their matter component. For example, strongly interacting Rydberg polaritons have recently been obtained using the nonlinear behavior of Rydberg excitations in an ensemble of atoms [12], which led to the demonstration of Rydberg polariton blockade [13] where the presence of a single polariton in a well-delimited region of space prevents the resonant injection of other polaritons. In parallel, efforts are being made to realize polariton blockade in condensed matter systems that hold great potential for realizing compact and integrated synthetic quantum materials [3]. Exciton polaritons in semiconductor materials are part light part matter particles that arise from the strong coupling of a quantum well exciton and a cavity photon [14]. These photonic particles inherit a nonlinear behavior from exciton-exciton interactions [2,15,16]. For efficient blockade to be obtained, the nonlinearity U needs to be greater than the inverse lifetime γ of the polaritons [6]. Recent state-of-the art experiments based on photon correlation measurements in semi-integrated microcavities attained optimized values of the ratio U/γ 0.1 in a photonic dot with about 3 µm 2 area [4,5]. These experiments represent the culmination of decade long technological developments aimed at increasing U/γ through reducing the photonic mode area [17][18][19] as well as increasing t...

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Section: Methodsmentioning

confidence: 99%

mentioning

confidence: 99%

Nonlinear optics in the fractional quantum Hall regime

Knüppel

Ravets

Kroner

et al. 2019

Nature

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“…This material class, in particular, is very interesting due to the large exciton binding energies up to hundreds of meV, 53,54 making excitonic effects dominant over the semiconductor's response. 55 We photoexcite the sample with 700 nm (1.77 eV) visible pulses from the 1 NOPA output above the A-exciton absorption energy and probe the excited-state population via PEEM with timedelayed 290 nm (4.28 eV) UV pulses, delivered from the 2 NOPA and SHG. The normalincidence excitation scheme with inter-pulse delay T is indicated in Fig.…”

Section: E Two-color Experimentsmentioning

confidence: 99%

Space- and time-resolved UV-to-NIR surface spectroscopy and 2D nanoscopy at 1 MHz repetition rate

Huber

Pres

Wittmann

et al. 2019

Review of Scientific Instruments

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We describe a setup for time-resolved photoemission electron microscopy (TR-PEEM) with aberration correction enabling 3 nm spatial resolution and sub-20 fs temporal resolution. The latter is realized by our development of a widely tunable (215-970 nm) noncollinear optical parametric amplifier (NOPA) at 1 MHz repetition rate. We discuss several exemplary applications. Efficient photoemission from plasmonic Au nanoresonators is investigated with phase-coherent pulse pairs from an actively stabilized interferometer. More complex excitation fields are created with a liquid-crystal-based pulse shaper enabling amplitude and phase shaping of NOPA pulses with spectral components from 600 to 800 nm. With this system we demonstrate spectroscopy within a single plasmonic nanoslit resonator by spectral amplitude shaping and investigate the local field dynamics with coherent two-dimensional (2D) spectroscopy at the nanometer length scale ("2D nanoscopy"). We show that the local response varies across a distance as small as 33 nm in our sample. Further, we report two-color pump-probe experiments using two independent NOPA beamlines. We extract local variations of the excitedstate dynamics of a monolayered 2D material (WSe2) that we correlate with low-energy electron microscopy (LEEM) and reflectivity (LEER) measurements. Finally, we demonstrate the in-situ sample preparation capabilities for organic thin films and their characterization via spatially resolved electron diffraction and dark-field LEEM.

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“…The past few decades have witnessed the birth of multi-dimensional multi-pulse techniques, which allow one to study elementary molecular events such as energy and charge transfer processes, formation and evolution of vibrational and electronic coherences, conformational and solvent dynamics and even to study the evolution of a system simultaneously in time and space (4D spectroscopy). [1][2][3][4][5][6][7][8] In combination with ultra-short laser pulses with high phase stability, these novel techniques have equipped researchers with the necessary tools to unravel gas-and condensed-phase dynamics in the sub-femtosecond (fs, 10 −15 s) and even in the attosecond (as, i.e., 10 −18 s) 9,10 regimes with an unprecedented level of detail. Nonetheless, connecting the optical response of the system to the underlying quantum-chemical structure and vibronic…”

Section: Introductionmentioning

confidence: 99%

iSPECTRON: A simulation interface for linear and nonlinear spectra with ab‐initio quantum chemistry software

et al. 2021

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We introduce iSPECTRON, a program that parses data from common quantum chemistry software (NWChem, OpenMolcas, Gaussian, Cobramm, etc.), produces the input files for the simulation of linear and nonlinear spectroscopy of molecules with the Spectron code, and analyzes the spectra with a broad range of tools. Vibronic spectra are expressed in term of the electronic eigenstates, obtained from quantum chemistry computations, and vibrational/bath effects are incorporated in the framework of the displaced harmonic oscillator model, where all required quantities are computed at the Franck-Condon point. The program capabilities are illustrated by simulating linear absorption, transient absorption and two dimensional electronic spectra of the pyrene molecule. Calculations at two levels of electronic structure theory, time-dependent density functional theory (with NWChem) and RASSCF/ RASPT2 (with OpenMolcas) are presented and compared where possible. The iSPECTRON program is available online at https://github.com/ispectrongit/ iSPECTRON/ and distributed open source under the terms of the Educational Community License version 2.0 (ECL 2.0).

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Multidimensional Coherent Spectroscopy of Semiconductors

Cited by 59 publications

References 147 publications

Nonlinear optics in the fractional quantum Hall regime

Nonlinear optics in the fractional quantum Hall regime

Space- and time-resolved UV-to-NIR surface spectroscopy and 2D nanoscopy at 1 MHz repetition rate

iSPECTRON: A simulation interface for linear and nonlinear spectra with ab‐initio quantum chemistry software

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