A microfluidic flow-cell for the study of the ultrafast dynamics of biological systems

Chauvet, Adrien; Tibiletti, Tania; Caffarri, Stefano; Chergui, Majed

doi:10.1063/1.4899120

Cited by 11 publications

(6 citation statements)

References 25 publications

(21 reference statements)

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“…20,21 For instance, it has been used for real time monitoring [22][23][24] and control 25,26 of chemical reactions, following mixing reactions, 27,28 steer molecular self-assembly 29,30 and study (out-of-equilibrium) reactions in biological systems. [31][32][33] In this paper, we use a lab-on-a-chip approach as a means to achieve out-of-equilibrium control over the structural hierarchy of an artificial light-harvesting complex: double-walled molecular nanotubes. Structural simplification of such nanotubes has previously been demonstrated in bulk solution by dissolving the outer tube via flash-dilution thereby exposing the bare inner tube for linear absorption spectroscopy.…”

Section: Introductionmentioning

confidence: 99%

Microfluidic out-of-equilibrium control of molecular nanotubes

Kriete

Feenstra

Pshenichnikov

2020

Phys. Chem. Chem. Phys.

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The bottom-up fabrication of functional nanosystems for light-harvesting applications and excitonic devices often relies on molecular self-assembly. Gaining access to the intermediate species involved in self-assembly would provide valuable insights into the pathways via which the final architecture has evolved, yet difficult to achieve due to their intrinsically short-lived nature. Here, we employ a lab-on-a-chip approach as a means to obtain in situ control of the structural complexity of an artificial light-harvesting complex: molecular double-walled nanotubes. Rapid and stable dissolution of the outer wall was realized via microfluidic mixing thereby rendering the thermodynamically unstable inner tubes accessible to spectroscopy. By measurement of the linear dichroism and time-resolved photoluminescence of both double-walled nanotubes and isolated inner tubes we show that the optical (excitonic) properties of the inner tube are remarkably robust to such drastic perturbation of the system's supramolecular structure as removal of the outer wall. The developed platform is readily extendable to a broad range of practical applications such as e.g. self-assembling systems and molecular photonics devices.

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Section: Introductionmentioning

confidence: 99%

Microfluidic out-of-equilibrium control of molecular nanotubes

Kriete

Feenstra

Pshenichnikov

2020

Phys. Chem. Chem. Phys.

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“…A strategy that is capable to alleviate these limitations relies on microfluidics 19 , which in recent years has successfully been implemented to manipulate chemical reactions in real time 20 or to steer self-assembly dynamics 21,22 . In particular, combinations of microfluidics and spectroscopy including steady-state absorption 23 , time-resolved spectroscopy 24,25 , and coherent two-dimensional (2D) infrared spectroscopy 26 have received considerable attention. In this framework, microfluidics bridges the gap between controlled modifications of the sample on timescales of microseconds to minutes with ultrafast processes on timescales down to femtoseconds.…”

Section: Introductionmentioning

confidence: 99%

Interplay between structural hierarchy and exciton diffusion in artificial light harvesting

et al. 2019

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Unraveling the nature of energy transport in multi-chromophoric photosynthetic complexes is essential to extract valuable design blueprints for light-harvesting applications. Long-range exciton transport in such systems is facilitated by a combination of delocalized excitation wavefunctions (excitons) and exciton diffusion. The unambiguous identification of the exciton transport is intrinsically challenging due to the system’s sheer complexity. Here we address this challenge by employing a spectroscopic lab-on-a-chip approach: ultrafast coherent two-dimensional spectroscopy and microfluidics working in tandem with theoretical modeling. We show that at low excitation fluences, the outer layer acts as an exciton antenna supplying excitons to the inner tube, while under high excitation fluences the former converts its functionality into an exciton annihilator which depletes the exciton population prior to any exciton transfer. Our findings shed light on the excitonic trajectories across different sub-units of a multi-layered artificial light-harvesting complex and underpin their great potential for directional excitation energy transport.

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“…The microfluidic flow-cell, [19] as illustrated in Figure 6, is composed of three main elements that are connected via flexible tubing of 1-mm diameter:…”

Section: The Microfluidic Flow-cellmentioning

confidence: 99%

Microfluidics for Ultrafast Spectroscopy

Chauvet¹

2016

Advances in Microfluidics - New Applications in Biology, Energy, and Materials Sciences

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Ultrafast laser technologies became one of the essential tool in the characterization of molecular compounds. Being comprised of spectroscopists, laser scientists, chemists and biologists, the "ultrafast community" is often disconnected and consequently unaware of the developments in microfluidic systems. The challenges of studying limited amount of precious liquid sample by means of ultrafast spectroscopy remains silent and, while no commercial systems are available, each research group is developing its own "homemade" options. This chapter will therefore contribute in filling up the gap that exist between the two communities, that of the ultrafast spectroscopy and that of microfluidics by revealing the importance of this analytical tool as well as the advantages of applying microfluidic technics to it. In this goal, the chapter will focus of the recently developed microfluidic flow-cell. With a minimal volume of about 250 µL, the flow-cell enables the study of precious protein complexes that are simply not available in larger quantities. The multiple advantages of the microfluidic flow-cell will be illustrated by the analysis of the cytochrome bc 1 . In particular, the study will describe how the capabilities of the microfluidic flow-cell enabled the resolution of the ultrafast electronic and nuclear dynamics of specific embedded chromophores.

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A microfluidic flow-cell for the study of the ultrafast dynamics of biological systems

Cited by 11 publications

References 25 publications

Microfluidic out-of-equilibrium control of molecular nanotubes

Microfluidic out-of-equilibrium control of molecular nanotubes

Interplay between structural hierarchy and exciton diffusion in artificial light harvesting

Microfluidics for Ultrafast Spectroscopy

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