Mapping of quantum phases by two-dimensional vibronic spectroscopy of wave-packet revivals

Schubert, Alexander; Renziehausen, Klaus; Engel, Volker

doi:10.1103/physreva.82.013419

Cited by 14 publications

(9 citation statements)

References 58 publications

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“…4(b), the cross section at ω τ = 1.42 eV is plotted as a function of T and clearly depicts the phase oscillations of the cross-peak at ω t = 1.38 eV. This type of line shape modulation was observed in simulations previously, 36,37 and attributed to vibrational coupling. The results presented here show that this need not be the case and that line shape oscillations can be seen, and should be expected, for any pair of coupled transitions evolving as exp (±iω 23 T ).…”

Section: A Simulating the 3d Experimentssupporting

confidence: 62%

Three-dimensional electronic spectroscopy of excitons in asymmetric double quantum wells

Davis

Hall

Dao

et al. 2011

The Journal of Chemical Physics

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We demonstrate three-dimensional (3D) electronic spectroscopy of excitons in a double quantum well system using a three-dimensional phase retrieval algorithm to obtain the phase information that is lost in the measurement of intensities. By extending the analysis of two-dimensional spectroscopy to three dimensions, contributions from different quantum mechanical pathways can be further separated allowing greater insight into the mechanisms responsible for the observed peaks. By examining different slices of the complete three-dimensional spectrum, not only can the relative amplitudes be determined, but the peak shapes can also be analysed to reveal further details of the interactions with the environment and inhomogeneous broadening. We apply this technique to study the coupling between two coupled quantum wells, 5.7 nm and 8 nm wide, separated by a 4 nm barrier. Coupling between the heavy-hole excitons of each well results in a circular cross-peak indicating no correlation of the inhomogeneous broadening. An additional cross-peak is isolated in the 3D spectrum which is elongated in the diagonal direction indicating correlated inhomogeneous broadening. This is attributed to coupling of the excitons involving the two delocalised light-hole states and the electron state localised on the wide well. The attribution of this peak and the analysis of the peak shapes is supported by numerical simulations of the electron and hole wavefunctions and the three-dimensional spectrum based on a density matrix approach. An additional benefit of extending the phase retrieval algorithm from two to three dimensions is that it becomes substantially more reliable and less susceptible to noise as a result of the more extensive use of a priori information.

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Section: A Simulating the 3d Experimentssupporting

confidence: 62%

Three-dimensional electronic spectroscopy of excitons in asymmetric double quantum wells

Davis

Hall

Dao

et al. 2011

The Journal of Chemical Physics

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“…Molecular-beam 2D electronic spectroscopy permits, for example, the experimental investigation of revivals in coherent wave-packet motion 63 , 64 and enables to follow the evolution of coherences during bond breakage or isomerization. It further facilitates comparison with complementary liquid-phase 2D spectroscopy based on fluorescence detection 65 by investigating the same molecule in different environments within one experiment, rendering it possible to study in detail the role of the environment during primary steps of photochemistry.…”

Section: Discussionmentioning

confidence: 99%

Coherent two-dimensional electronic mass spectrometry

Roeding

Brixner

2018

Nat Commun

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Coherent two-dimensional (2D) optical spectroscopy has revolutionized our ability to probe many types of couplings and ultrafast dynamics in complex quantum systems. The dynamics and function of any quantum system strongly depend on couplings to the environment. Thus, studying coherent interactions for different environments remains a topic of tremendous interest. Here we introduce coherent 2D electronic mass spectrometry that allows 2D measurements on effusive molecular beams and thus on quantum systems with minimum system–bath interaction and employ this to identify the major ionization pathway of 3d Rydberg states in NO2. Furthermore, we present 2D spectra of multiphoton ionization, disclosing distinct differences in the nonlinear response functions leading to the ionization products. We also realize the equivalent of spectrally resolved transient-absorption measurements without the necessity for acquiring weak absorption changes. Using time-of-flight detection introduces cations as an observable, enabling the 2D spectroscopic study on isolated systems of photophysical and photochemical reactions.

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“…The multiple interferences of the WP components lead also to the so-called fractional revivals at divisors of the revival time, which have been predicted [18,19] and observed in Rydberg WPs [20] or photon bouncing balls [21]. Fractional revivals can retrieve information about the system even if it decays before the first revival [22]. They can be used for mapping the quantum phase of a molecular nuclear WP in two-dimensional spectroscopy [23], or even to factorize prime numbers [24].…”

Section: Introductionmentioning

confidence: 99%

Quantum Carpets: a Probe to Identify Wave-Packet Fractional Revivals

Yousaf

Iqbal

2016

J Russ Laser Res

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Quantum carpets− in position and momentum space− woven by the self-interference of de Broglie wave of an atom or an electron, trapped in an infinitely deep potential well, are explained. The recurrence of self-similar structures in designs of these carpets mimics the phenomena of quantum revivals and fractional revivals. We identify fractional revivals of various order by means of these space-time and momentum-time interference patterns.2

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Mapping of quantum phases by two-dimensional vibronic spectroscopy of wave-packet revivals

Cited by 14 publications

References 58 publications

Three-dimensional electronic spectroscopy of excitons in asymmetric double quantum wells

Three-dimensional electronic spectroscopy of excitons in asymmetric double quantum wells

Coherent two-dimensional electronic mass spectrometry

Quantum Carpets: a Probe to Identify Wave-Packet Fractional Revivals

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