PHOTOINDUCED QUANTUM TRANSPORT

Jeyson P. Alomoto (1), Daniel Gonzalez (1), Duncan J. Mowbray (1), Vito Despoja (2).

(1)1School of Physical Sciences and Nanotechnology, Yachay Tech University, Urcuqu ́ı 100119, Ecuador.
(2)Institute of Physics, 10000 Zagreb, Croatia

Creating organic photovoltaics that are both cost-effective and environmentally friendly is a current goal in the
field of physical and nanotechnology scientific research. To achieve this, it is needed to explore the use of
computational methods to design the next generation of OPVs. However, accurately describing the way large
molecules within these systems undergo excitation processes requires the development of advanced
computational techniques. Once it is constructed a stable computational model, it is possible to effectively
describe the physical properties of interest of our system and then contribute to the efforts of getting novel
materials to the society. Specifically, our point of interest is the External Quantum Efficiency (EQE) of a
photovoltaic device, which determines how much a device is capable of converting incident photons into
electrons. In order to develop new and better OPVs materials, modeling the EQE of a solar cell using ab initio
methods to accurately describe their efficiency is necessary. To address this problem, we must include the optical
absorption process at the independent particle approximation level as a coupling between two leads of the
conducting circuit (FIG. 1). At the quantum regime, it is possible to use the non-equilibrium Green’s function
formalism to determine the EQE of these types of systems. By the implementation of a python code based on
GPAW, it is possible to achieve the computational calculations to obtain the observables of interest in this
system. Particularly, different models were used for constructions of SWCNT with different chiralities. The
difference in the chiralities characterize if the SWCNT is metallic or semiconducting. The optical absorption,
charge carrier generation and the charge transport of low dimensional organic photovoltaic systems such as a
carbon chain and single-walled carbon nanotubes (SWCNTs) have been analyzed. Particularly, the SWCNTs
were modeled using this computational structure. Taking into account the region of available allowed states for
absorption to occur, the absorption and transmission probability T is calculated as a function of the initial energy.
The absorption, transmission, overlapping and Kohn Sham Hamiltonian matrices are represented using a linear
combination of atomic orbitals (LCAO). To test our method for calculating the EQE of a system, we first apply it
to a simple two-level four site tight-binding (TB) toy-model system consisting of an occupied and unoccupied
band coupled via an external electromagnetic field (FIG. 2). The absorption and transmission probability and its
behavior is shown as a function of initial energy and excitation energy (FIG. 3). We find a four atom periodic
carbon chain aligned in the x-direction has a relaxed carbon-carbon bond length of dC−C ≈1.39 Å. Finally,
contributing to the computational design of novel low-dimensional organic photovoltaic systems could enhance
research and development in this important area of physics.

REFERENCES
[1] Glowacki, J. Jung, J. Ulanski, and A. Rybak, 2.33 - Conductivity Measurements, in Polymer Science: A Comprehensive
Reference, edited by K. Matyjaszewski and M. Möller (Elsevier, Amsterdam, 2012) pp. 847–877.
[2] Y. Meir and N. S. Wingreen, Landauer formula for the current through an interacting electron region, Phys. Rev. Lett 68,
2512 (1992).
[3] S. Datta, Electronic Transport in Mesoscopic Systems, Cambridge Studies in Semiconductor Physics and
Microelectronic Engineering (Cambridge University Press, Cambridge, 1995).
[4] C. Meis and P. R. Dahoo, Vector potential quantization and the photon wave-particle representation, J. Phys. Conf. 738,
012099

ACKNOWLEDGMENTS

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 Daniel Gonzalez & Jeison Alomoto Acta Microscopica Vol. 32, Supp. 1, 2023, pp. xx
PROCEEDINGS NSSY 2023- Galapagos 23th-29th April 2023
I would like to express our deep gratitude to our thesis advisor, Duncan Mowbray, for their exceptional guidance, support,
and mentorship. Their unwavering dedication to excellence and their ability to challenge us intellectually have been
instrumental in our academic and personal growth. We extend our gratitude to the School of Physical Science and
Nanotechnology for providing the resources and infrastructure necessary for the successful completion of this research.
Finally, we would like to thank our families and friends for their love, encouragement, and support throughout our academic
journey. Their unwavering belief in us has been a constant source of motivation, and we are deeply grateful for their
presence in our lives.

FIGURES

Figure 1: Schematic of an excitation process across a donor–acceptor interface from an occupied initial state with energy εi
in the input lead to an unoccupied intermediate state with energy εi + ħω via the interaction between an external
electromagnetic field with vector potential  and momenta p̂, 𝑒/2𝑚𝑐〈𝜓𝑓|· 𝑝̂|𝜓𝑖〉 and via coupling to a 2mc phonon mode
of energy hν to an unoccupied final state with energy εf = εi + ħω − hν in the output lead.

Figure 2: (a) Schematic depicting a two level four site tight-binding (TB) model |φ±𝑖〉 with onsite energies ±ε (black
lines), interatomic coupling γ (red arrows), and occupied to unoccupied coupling via the external electromagnetic field
−iα/(ħω)^1/2 (magenta arrows) and (b) calculated density of states (DOS) showing energy gap Egap , band widths 4γ, and
occupation (gray filling).

Figure 3: Absorption and transmission probability T as a function of initial energy εi and excitation energy ħω in eV for a
two-level four-site toy model with Egap = 1 eV, γ = 0.25 eV, ε = 1.5 eV, α = 1 eV3 ⁄2 and εf = εi + ħω. The parallelogram
(white dashed lines) marks the region of available allowed states for absorption to occur.

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