Simulating action-2D electronic spectroscopy of quantum dots: insights on the exciton and biexciton interplay from detection-mode and time-gating

Abstract

Action-2D Electronic Spectroscopy is emerging as a powerful technique to investigate exciton dynamics in molecular aggregates and nanostructures. While maintaining the power of highlighting coherent evolution between the laser pulses,...

Direct time-frequency response of electronic coherences in assemblies of colloidal CdSe quantum dot dimers probed at room temperature by 2-dimensional electronic spectroscopy

“…2DES action-based fluorescence and photocurrent measurements [20][21][22][23][24][25][26][27]39 are a practical alternative to the polarization BOXCARS ones because they can be implemented with a much simpler collinear set-up. 5 In addition, photocurrent is a more appropriate choice of observable for quantum technology applications as photocurrent measurements can be directly interfaced with classical electronics.…”

“…The ability to measure electronic coherences in the directly measured data, without the need to compute full frequency maps, greatly enhances the potential for use of electronic coherences of QDs in room temperature quantum technologies. Towards applications to quantum information processing, a photocurrent action set-up [20][21][22][23][24][25][26][27] presents several advantages over the BOXCARS one for 2DES: it is a collinear set-up, easier to operate and the output is a photocurrent that can be easier processed and integrated with a classical computer. It is therefore of interest to investigate how electronic coherences are probed in the photocurrent response.…”

Unifying Nonlinear Response and Incoherent Mixing in Action-2D Electronic Spectroscopy

“…Contrary to C-2DES, , the presence of cross-peaks at early waiting times does not represent a univocal signature of excitonic delocalization in A-2DES, , having been reported even in the case of weakly interacting systems. , By analyzing the different contributions to the response function for a molecular dimer, Malý and Mančal demonstrated that cross-peaks can emerge from the incomplete cancellation of different pathways as a consequence of exciton–exciton annihilation during the detection time . Following the same line, several other contributions highlighted the importance of two-exciton manifold dynamics in determining spectral features. − …”

“…This procedure can be numerically implemented in close analogy with the experiment. By employing a non-perturbative treatment of the light–matter interaction, the dynamics of the system is modeled using the Lindblad quantum master equation. ,, Details of the computational procedure and the parameters used for the simulations are reported in the Supporting Information.…”

Time-frequency signatures of electronic coherence of colloidal CdSe quantum dot dimer assemblies probed at room temperature by 2-dimensional electronic spectroscopy

“…The ability to measure electronic coherences in the directly measured data, without the need to compute full frequency maps, greatly enhances the potential for the use of electronic coherences of QDs in room temperature quantum technologies. Towards applications to quantum information processing, the recently proposed photocurrent action-based set-up [20][21][22][23][24][25][26][27] presents several advantages over the BOXCARS one for 2DES: it is a collinear set-up, easier to operate and the output is a photocurrent that can be easier processed and integrated with a classical computer. It is therefore of interest to investigate how electronic coherences are probed in the photocurrent response.…”