Multi-dimensional coherent optical spectroscopy of semiconductor nanostructures: Collinear and non-collinear approaches

Nardin, Gaël; Autry, Travis M.; Singh, Rohan; Li, Hebin; Cundiff, Steven T.

doi:10.1063/1.4913830

Cited by 21 publications

(18 citation statements)

References 50 publications

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“…In a more recent development, various incoherent action signals have been applied to measure coherent spectra. Photocurrent detected 2D spectroscopy has provided valuable information about photoinduced processes in quantum well and quantum dot based materials 17,18. Photo-electron detection has been used to achieve spatial resolution beyond the diffraction limit of the optical beams in 2D spectroscopy 19.…”

Section: Introductionmentioning

confidence: 99%

Before Förster. Initial excitation in photosynthetic light harvesting

et al. 2019

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Electronic 2D spectroscopy allows nontrivial quantum effects in chemistry and biology to be explored in unprecedented detail. Here, we apply recently developed fluorescence detected coherent 2D spectroscopy to study the light harvesting antenna 2 (LH2) of photosynthetic purple bacteria. The method utilizes the destructive interference between two signal components thereby uncovering cross peaks which are not visible in conventional photon-echo based 2D and transient absorption measurements. Analyses of signal generating quantum pathways leads to the conclusion that, contrary to the currently prevailing physical picture, the two weakly-coupled pigment rings of LH2 share the initial electronic excitation leading to quantum mechanical correlation between the two clearly separate bands. These results are general and have consequences for the interpretation of excited states not only in photosynthesis but in all light absorbing systems. The initial delocalization could be the key for enhancing the light harvesting efficiency via biased motion towards the energy funnel.The primary processes in photosynthesis run with nearly 100 % quantum efficiency -almost every absorbed photon leads to a charge separation event. How such high efficiency is achieved and the possible role of quantum processes in it, is currently at the center of active scientific research (1-4). One of the possible functional elements of such quantum behavior and optimization in photosynthesis is delocalization -the spatial domain coherently covered by the excited state after light absorption (5).

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Section: Introductionmentioning

confidence: 99%

Before Förster. Initial excitation in photosynthetic light harvesting

et al. 2019

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“…This includes standard two-pulse pump-probe signals where k S = k i − k i + k 3 and i = 1, 2, as well as non-rephasing (NR) k S = k 1 − k 2 + k 3 and rephasing (R) k S = − k 1 + k 2 + k 3 three-pulse signals. As indicated by figure 1(c), the NR signal is emitted into the fourth quadrant of the box geometry when assuming logical pulse ordering #1-#2-#3, and becomes the R signal for a #2-#1-#3 pulse ordering [22]. This signal emission can be equivalently explained as probe pulse diffraction from a transient grating created by the spatiotemporal interference of two pump pulses.…”

Section: Creation and Detection Of Four Pulse Replicas In A Box Geometrymentioning

confidence: 96%

Ultrafast multidimensional spectroscopy with field resolution and noncollinear geometry at mid-infrared frequencies

et al. 2022

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Energetic correlations and their dynamics govern the fundamental properties of condensed matter materials. Ultrafast multidimensional spectroscopy in the mid infrared is an advanced technique to study such coherent low-energy dynamics. The intrinsic many-body phenomena in functional solid-state materials, in particular few-layer samples, remain widely unexplored to this date, because complex and weak sample responses demand versatile and sensitive detection. Here, we present a novel setup for ultrafast multidimensional spectroscopy with noncollinear geometry and complete field resolution in the 15-40 THz range. Electric fields up to few-100 kV cm-1 drive coherent dynamics in a perturbative regime, and an advanced modulation scheme allows to detect nonlinear signals down to a few tens of V cm-1 entirely background-free with high sensitivity and full control over the geometric phase-matching conditions. Our system aims at the investigation of correlations and many-body interactions in condensed matter systems at low energy. Benchmark measurements on bulk indium antimonide (InSb) reveal a strong six-wave mixing signal and map ultrafast changes of the band structure with access to amplitude and phase information. Our results pave the way towards the investigation of functional thin film materials and few-layer samples.

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“…Pulse sequence (1,2,3), with inter-pulse delays τ and T . t is the real time during which the radiation of the FWM signal occurs.…”

Section: Double-sided Feynman Diagrams and Types Of Multidimensional mentioning

confidence: 99%

“…It will be shown how MDCS enables separation and ‡ Selected contributions from the author's own group were recently reviewed in Ref. [3] measurement of homogeneous and inhomogeneous linewidths in disordered quantum wells, large ensemble of quantum dots and emerging semiconductor materials, and how this can be useful for measuring biexciton binding energies. I also focus on one of the major advantages of MDCS, which is the ability to study coupling between separate resonances.…”

Section: Introductionmentioning

confidence: 99%

Multidimensional coherent optical spectroscopy of semiconductor nanostructures: a review

Nardin

2015

Semicond. Sci. Technol.

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Abstract. Multidimensional Coherent optical Spectroscopy (MDCS) is an elegant and versatile tool to measure the ultrafast nonlinear optical response of materials. Of particular interest for semiconductor nanostructures, MDCS enables the separation of homogeneous and inhomogeneous linewidths, reveals the nature of coupling between resonances, and is able to identify the signatures of many-body interactions. As an extension of transient Four-Wave Mixing (FWM) experiments, MDCS can be implemented in various geometries, in which different strategies can be used to isolate the FWM signal and measure its phase. I review and compare different practical implementations of MDCS experiments adapted to the study of semiconductor materials. The power of MDCS is illustrated by discussing experimental results obtained on semiconductor nanostructures such as quantum dots, quantum wells, microcavities, and layered semiconductors.

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Multi-dimensional coherent optical spectroscopy of semiconductor nanostructures: Collinear and non-collinear approaches

Cited by 21 publications

References 50 publications

Before Förster. Initial excitation in photosynthetic light harvesting

Before Förster. Initial excitation in photosynthetic light harvesting

Ultrafast multidimensional spectroscopy with field resolution and noncollinear geometry at mid-infrared frequencies

Multidimensional coherent optical spectroscopy of semiconductor nanostructures: a review

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