Pavel Malý

Pavel Malý
Charles University in Prague | CUNI · Faculty of Mathematics and Physics

Doctor of Philosophy

About

37
Publications
7,491
Reads
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403
Citations
Introduction
Using ultrafast nonlinear and single-molecule spectroscopy in combination with theoretical description, I study photoinduced energy and charge transfer in molecular systems such as natural photosynthetic complexes or conjugated polymers. Currently I am interested in fluorescence-detected coherent spectroscopy. I believe that such technique can measure slow variations of ultrafast kinetics in individual molecular complexes.
Additional affiliations
November 2018 - August 2020
University of Wuerzburg
Position
  • PostDoc Position
Description
  • Alexander von Humboldt research fellow
Education
November 2014 - October 2018
Vrije Universiteit Amsterdam
Field of study
  • Biophysics
October 2014 - October 2018
Charles University in Prague
Field of study
  • Biophysics
September 2012 - June 2014
Charles University in Prague
Field of study
  • Optics

Publications

Publications (37)
Article
Full-text available
Energy relaxation in light-harvesting complexes has been extensively studied by various ultrafast spectroscopic techniques, the fastest processes being in the sub–100-fs range. At the same time, much slower dynamics have been observed in individual complexes by single-molecule fluorescence spectroscopy (SMS). In this work, we use a pump–probe-type...
Article
Full-text available
Nuclear vibrations play a prominent role in the spectroscopy and dynamics of electronic systems. As recent experimental and theoretical studies suggest, this may be even more so when vibrational frequencies are resonant with transitions between the electronic states. Here we present a vibronic multilevel Redfield model for excitonically coupled ele...
Article
Full-text available
Exciton transport and exciton–exciton interactions in molecular aggregates and polymers are of great importance in natural photosynthesis, organic electronics, and related areas of research. Both the experimental observation and theoretical description of these processes across time and length scales, including the transition from the initial wavel...
Article
Optical two-dimensional electronic spectroscopy (2DES) is now widely utilized to study excitonic structure and dynamics of a broad range of systems, from molecules to solid state. Besides the traditional experimental implementation using phase matching and coherent signal field detection, action-based approaches that detect incoherent signals such...
Article
Full-text available
Time-resolved pump–probe (PP) spectroscopy has revolutionized mechanistic investigations in chemistry. In the present work, we introduce a new approach, fluorescence-detected pump–probe (F-PP) spectroscopy, that overcomes several limitations of traditional PP. F-PP suppresses excited-state absorption, provides background-free detection, removes art...
Article
Although azulene's anomalous fluorescence originating from S 2 rather than from S 1 is the textbook example for the violation of Kasha's rule, the understanding of the underlying processes is still a subject of investigation. Here, we use action-based coherent two-dimensional electronic spectroscopy (2DES) to measure a single Liouville-space respon...
Article
Despite the disordered and dynamic environment in which it occurs, photosynthetic light harvesting is highly efficient. Now, measurements of energy transfer in single photosynthetic antennae show how these structures deal with protein fluctuations, robustly transferring the energy before it is lost.
Article
The influence of oligosquaraine chain length on the energies and shape of absorption and emission bands and the exciton coherence length is studied in CHCl3 where the oligomers adopt a random coil structure. From the observed fluorescence band narrowing an effective coherence length of Ncoh = 2.5 was estimated for the nonamer. Applying a theoretica...
Article
Full-text available
Eine ultraschnelle Pump-Probe-Spektroskopie mit Fluoreszenzdetektion wurde entwickelt. Durch die Kombination von empfindlicher Fluoreszenzdetektion mit ultraschneller pulsbegrenzter Zeitauflösung bietet dieser Ansatz eine komplementäre Technik zum Standard der transienten Absorption. Abstract Fluoreszenzdetektierte Pump-Probe-(F-PP-)Spektroskopie...
Article
Exciton–exciton-interaction two-dimensional (EEI2D) spectroscopy is a fifth-order variant of 2D electronic spectroscopy. It can be used to probe biexciton dynamics in molecular systems and to observe exciton diffusion in extended systems such as polymers or light-harvesting complexes. The exciton transport strongly depends on the geometrical and en...
Article
Full-text available
Correction for ‘From wavelike to sub-diffusive motion: exciton dynamics and interaction in squaraine copolymers of varying length’ by Pavel Malý et al. , Chem. Sci. , 2020, 11 , 456–466, DOI: 10.1039/C9SC04367E.
Article
Two-dimensional electronic spectroscopy (2DES) can be realized in increasing nonlinear orders of interaction with the electric field, bringing new information about single- and multi-particle properties and dynamics. Furthermore, signals can be detected both coherently (C-2DES) and by fluorescence (F-2DES), with fundamental and practical difference...
Article
Full-text available
Intramolecular charge transfer processes play an important role in many biological, chemical and physical processes including photosynthesis, redox chemical reactions and electron transfer in molecular electronics. These charge transfer processes are frequently influenced by the dynamics of their molecular or atomic environments, and they are accom...
Article
Full-text available
Coherent two-dimensional spectroscopy is a powerful tool for probing ultrafast quantum dynamics in complex systems. Several variants offer different types of information but typically require distinct beam geometries. Here we introduce population-based three-dimensional (3D) electronic spectroscopy and demonstrate the extraction of all fourth- and...
Article
Full-text available
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 identifi...
Article
Plasmonic coupling of metallic nanoparticles and adjacent pigments can dramatically increase the brightness of the pigments due to the enhanced local electric field. Here, we demonstrate that the fluorescence brightness of a single plant light-harvesting complex (LHCII) can be significantly enhanced when coupled to a gold nanorod (AuNR). The AuNRs...
Preprint
Full-text available
Unravelling 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 remarkable exciton diffusivities. The unam...
Preprint
Plasmonic coupling of metallic nanoparticles and adjacent pigments can dramatically increase the brightness of the pigments due to the enhanced local electric field. Here, we demonstrate that the fluorescence brightness of a single plant light-harvesting complex (LHCII) can be significantly enhanced when coupled to single gold nanorods (AuNRs). The...
Article
Incoherently detected coherent multidimensional spectroscopy is rapidly gaining popularity, promising a different application range and sensitivity than its traditional counterpart. While measuring the same response, the two methods are not equivalent. We present calculations of the fluorescence-detected coherent two-dimensional (F-2DES) spectra of...
Preprint
We present calculations of the fluorescence-detected coherent two-dimensional (F-2DES) spectra of a molecular heterodimer. We compare how the F-2DES technique differs from the standard coherently detected two-dimensional (2DES) spectroscopy in measuring exciton delocalization. We analyze which processes contribute to cross-peaks in the zero-waiting...
Preprint
Full-text available
We present calculations of the fluorescence-detected coherent two-dimensional (F-2DES) spectra of a molecular heterodimer. We compare how the F-2DES technique differs from the standard coherently detected two-dimensional (2DES) spectroscopy in measuring exciton delocalization. We analyze which processes contribute to cross-peaks in the zero-waiting...
Article
Photosystems, the machines of photosynthesis, are highly complex and energetically disordered pigment-protein structures. Yet, they perform their function, be it highly efficient energy transfer and charge separation or the ability to switch between light-harvesting and photoprotective states, extremely well. In this opinioned review we describe th...
Article
Full-text available
Following the observation of coherent oscillations in non-linear spectra of photosynthetic pigment protein complexes, particularly phycobilliprotein such as PC645, coherent vibronic transport has been suggested as a design principle for novel light harvesting materials operating at room temperature. Vibronic transport between energetically remote p...
Article
Full-text available
Photosynthetic light harvesting can be very efficient in solar energy conversion while taking place in a highly disordered and noisy physiological environment. This efficiency is achieved by the ultrafast speed of the primary photosynthetic processes, which is enabled by a delicate interplay of quantum effects, thermodynamics and environmental nois...
Article
Full-text available
The conversion of solar radiation to chemical energy in plants and green algae takes place in the thylakoid membrane. This amphiphilic environment hosts a complex arrangement of light-harvesting pigment-protein complexes that absorb light and transfer the excitation energy to photochemically active reaction centers. This efficient light-harvesting...
Article
Full-text available
Strong excitonic interactions are a key design strategy in photosynthetic light harvesting, expanding the spectral cross-section for light absorption and creating considerably faster and more robust excitation energy transfer. These molecular excitons are a direct result of exceptionally densely packed pigments in photosynthetic proteins. The main...
Article
Full-text available
Ultrafast transient absorption spectroscopy is a powerful technique to study fast photo-induced processes, such as electron, proton and energy transfer, isomerization and molecular dynamics, in a diverse range of samples, including solid state materials and proteins. Many such experiments suffer from signal distortion by scattered excitation light,...
Article
Full-text available
When exciting a complex molecular system with a short optical pulse, all chromophores present in the system can be excited. The resulting superposition of electronically and vibrationally excited states evolves in time, which is monitored with transient absorption spectroscopy. We present a methodology to resolve simultaneously the contributions of...
Article
Full-text available
We derive approximate equations of motion for excited state dynamics of a multilevel open quantum system weakly interacting with light to describe fluorescence detected single molecule spectra. Based on the Frenkel exciton theory, we construct a model for the chlorophyll part of the LHCII complex of higher plants and its interaction with previously...
Article
In the major peripheral plant light-harvesting complex LHCII, excitation energy is transferred between chlorophylls along an energetic cascade before it is transmitted further into the photosynthetic assembly to be converted into chemical energy. The efficiency of these energy transfer processes involves a complicated interplay of pigment-protein s...
Article
We investigate the relevance of dynamic quantum coherence in the energy transfer efficiency of molecular aggregates. We contrast the dynamics after excitation of a quantum mechanical system with that of a classical system. We demonstrate how a classical description of an ensemble average can be satisfactorily interpreted either as a single system d...

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Project (1)
Project
Investigating the Biophysical Mechanisms of Photosynthesis using Stark Spectroscopy (in Collaboration with Professor Rienk van Grondelle of VU University Amsterdam). Examining the spectroscopic properties of organic conjugated polymers important for making light emitting diodes (in Collaboration with Professor Linda Peteanu of Carnegie Mellon University). Laser Induced Break Down Spectroscopy on different Natural Samples such as air, ground water, River Bed Soil in quest of different deleterious heavy metals (at University of Dhaka). Laser Raman Spectroscopy on different (organic, inorganic and biological samples) (at the University of Dhaka). Fabrication of Nanoparticles using Laser Ablation Technique (at the University of Dhaka)