Coherent two-dimensional photocurrent spectroscopy in a PbS quantum dot photocell

Karki, Khadga Jung; Widom, Julia R.; Seibt, Joachim; Moody, Ian; Lonergan, Mark C.; Pullerits, Tõnu; Marcus, Andrew H.

doi:10.1038/ncomms6869

Cited by 164 publications

(223 citation statements)

References 32 publications

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“…17,18 The action-based ansatz employs the detection of incoherent signals, e.g., fluorescence 16,17 (see also Fig. 1(a)), (photo)-electrons, 10,11,13,14 or (photo)-ions. 19 One advantage of detecting incoherent signals is that it permits the study of lowdensity samples, even down to the single-molecule limit.…”

Section: Introductionmentioning

confidence: 99%

“…Coherent two-dimensional (2D) electronic spectroscopy [1][2][3][4][5] has become an established method to study, among others, energy transfer in light harvesting complexes, [6][7][8] electronic dynamics in semiconductors, [9][10][11][12][13] plasmonic coherences, 14 and photochemical reactions. 15 Most of the experimental realizations rely on the non-collinear box geometry and heterodyned detection of a coherent optical signal.…”

Section: Introductionmentioning

confidence: 99%

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Optimizing sparse sampling for 2D electronic spectroscopy

Roeding

Klimovich

Brixner

2017

The Journal of Chemical Physics

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We present a new data acquisition concept using optimized non-uniform sampling and compressed sensing reconstruction in order to substantially decrease the acquisition times in action-based multidimensional electronic spectroscopy. For this we acquire a regularly sampled reference data set at a fixed population time and use a genetic algorithm to optimize a reduced non-uniform sampling pattern. We then apply the optimal sampling for data acquisition at all other population times. Furthermore, we show how to transform two-dimensional (2D) spectra into a joint 4D time-frequency von Neumann representation. This leads to increased sparsity compared to the Fourier domain and to improved reconstruction. We demonstrate this approach by recovering transient dynamics in the 2D spectrum of a cresyl violet sample using just 25% of the originally sampled data points.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Optimizing sparse sampling for 2D electronic spectroscopy

Roeding

Klimovich

Brixner

2017

The Journal of Chemical Physics

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“…Usual implementations of 2D ES rely upon optical wavevector matching to measure a thirdorder mesoscopic polarization response [2].In this work, we focus upon the two-dimensional photoexcitation spectroscopy (2D PES), as a variant of 2D ES techniques, in which the detected nonlinear optical signals rely on the fourth-order excited-state population. According to the final population of interest, one can probe the excitation spectral signals in forms of photoluminescence (PL) [6][7][8] or photocurrent (PC) [9][10][11], for example. Indeed, this implementation of 2D coherent spectroscopy has the formidable advantage that it can exploit photocurrent detection as an extraordinarily sensitive population probe [12].…”

Section: Introductionmentioning

confidence: 99%

Probing polaron excitation spectra in organic semiconductors by photoinduced-absorption-detected two-dimensional coherent spectroscopy

Gauthier-Houle

Grégoire

et al. 2016

Chemical Physics

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We report a theoretical description and experimental implementation of a novel two-dimensional coherent excitation spectroscopy based on quasi-steady-state photoinduced absorption measurement of a long-lived nonlinear population. We have studied a semiconductor-polymer:fullerene-derivative distributed heterostructure by measuring the 2D excitation spectrum by means of photoluminescence, photocurrent and photoinduced absorption from metastable polaronic products. We conclude that the photoinduced absorption probe is a viable and valuable probe in this family of 2D coherent spectroscopies.

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“…They are possible in the IR region [23] and in the visible range. At visible wavelengths, they can be detected by photon echo [22], by fluorescence [42,43], by photocurrent [43] or by photoelectrons [44]. To each one of these methods corresponds a family of mesoscopic systems that may exhibit Fano profiles and that can be studied.…”

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confidence: 99%

Coherent two-dimensional spectroscopy of a Fano model

Finkelstein-Shapiro¹,

Poulsen²,

Pullerits³

et al. 2016

Phys. Rev. B

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The Fano lineshape arises from the interference of two excitation pathways to reach a continuum. Its generality has resulted in a tremendous success in explaining the lineshapes of many one-dimensional spectroscopies -absorption, emission, scattering, conductance, photofragmentation -applied to very varied systems -atoms, molecules, semiconductors and metals. Unravelling a spectroscopy into a second dimension reveals the relationship between states in addition to decongesting the spectra. Femtosecond-resolved two-dimensional electronic spectroscopy (2DES) is a four-wave mixing technique that measures the time-evolution of the populations, and coherences of excited states. It has been applied extensively to the dynamics of photosynthetic units, and more recently to materials with extended band-structures. In this letter, we solve the full time-dependent third-order response, measured in 2DES, of a Fano model and give the new system parameters that become accessible.Whenever a discrete state and a continuum state interact and radiative transitions are allowed from the ground state to both, an interference occurs that gives rise to the Fano lineshape [1][2][3][4]. In the presence of dissipative processes, it has been shown that the generalized Fano equation consisting of a standard Fano plus a Lorentzian term is [1, 2, 5-9]:where q = µ e /nπV µ c and = (ω L − ω e )/γ e , µ e is the transition dipole moment to the discrete excited state, µ c the transition dipole moment to the continuum, V the coupling of the discrete excited state to the continuum, n the density of states of the continuum, ω e is the energy of the discrete state relative to the ground state, ω L is the radiation field frequency, and γ e = nπV 2 is the linewidth of the excited state, induced by its coupling nV 2 to the continuum set of states. C is the weight of the Lorentzian term and is related to the dissipative processes [6][7][8][9][10]. Since its original inception, the 1961 paper has resulted in more than 8,000 citations testifying to its ubiquity in physics, chemistry and materials science. The first Fano profiles were observed more than 80 years ago in atomic spectra, including photoionization of atoms and photodissociation of small molecules [3,4]. The field of study was established around scattering processes where the phenomena of coupling to a thermal bath resulting in dissipation or decoherence is not important, except in a few cases, notably pressure broadening [11][12][13].The synthesis and control of matter at the nanoscale opened up the observation of Fano profiles to dissipative systems [14][15][16][17][18] which in turn spurred a renewed interest in theoretical descriptions that would solve the problem in open quantum systems [8][9][10][19][20][21], and correctly account for the relaxation. Consequent with this desire to measure dissipation, more sophisticated spectroscopies are to be invoked. 2D electronic spectroscopy (2DES) is arguably one of the best spectroscopies to measure decoherence and relaxation between states [22][23]...

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Coherent two-dimensional photocurrent spectroscopy in a PbS quantum dot photocell

Cited by 164 publications

References 32 publications

Optimizing sparse sampling for 2D electronic spectroscopy

Optimizing sparse sampling for 2D electronic spectroscopy

Probing polaron excitation spectra in organic semiconductors by photoinduced-absorption-detected two-dimensional coherent spectroscopy

Coherent two-dimensional spectroscopy of a Fano model

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