Filter-free spectral tunable photodetectors (PDs) are critical for a plethora of applications in imaging, indoor light fidelity (Li-Fi), and light communications. The present band-selective light detection is realized by incorporating different optical filters with broadband inorganic semiconductor-based PDs. However, the use of the optical filters reduces the overall performance of these PDs and is not appliable in the emerging flexible and wearable applications. The rapid advancement of the organic semiconductors offers an exciting opportunity for the development of high-performance filter-free spectral tunable organic photodetectors (OPDs). The development of OPDs has attracted tremendous interests because of the tailored optoelectronic properties of the π-conjugated organic semiconductors and the solution fabrication process of the OPDs. Apart from the rapid progresses made in improving the responsivity and detectivity of OPDs, the spectral properties of OPDs also receive intense attention. This Ph.D. research work has been focused on developing a universal strategy to achieve high-performance filter-free band-selective and spectral tunable OPDs. The correlation between the optical profile and responsivity spectrum of the novel OPDs with a bilayer photoactive layer has been investigated. It suggests that the responsivity spectrum of the OPDs can be effectively modulated by managing the optical profile in the bilayer and multilayer photoactive layer. A filter-free band-selective OPD model, comprising a bilayer shorter-wavelength light depletion layer/longer-wavelength light-absorbing layer architecture photoactive layer, has been developed. The depletion layer in the filter-free OPDs has a dual-function serving as a shorter-wavelength light-absorbing layer and a hole-transporting layer. The photodetection spectrum window of the filter-free band-selective OPDs, defined by the difference in wavelengths between the transmission cutoff of the shorter-wavelength light depletion layer and the absorption edge of the longer-wavelength light-absorbing layer, can then be tuned over the different wavelength ranges by using an appropriate combination of the shorter-wavelength light depletion layer and the longer-wavelength light-absorbing layer. A dual-mode OPD, having a trilayer visible light absorber/optical spacer/near-infrared (NIR) light absorber configuration photoactive layer, has been proposed. The dual-mode OPD exhibits electrically switchable NIR response operated under a reverse bias and visible light response operated under a forward bias. In the presence of NIR light, the trap-assisted charge-injection behavior at the organic/cathode interface in the OPDs operated under a reverse bias. The photocurrent is produced in the visible light-absorbing layer, enabled by the trap-assisted charge injection at the anode/organic interface under a forward bias. The developed filter-free band-selective OPDs and electrically switchable dual-mode OPDs provided an attractive alternative optical detection technology to the conventional panchromatic and single-mode OPDs. The spectral tunable photodetection thus demonstrated offers a promising option for new OPD applications.

Solar energy is a viable alternative to traditional fossil fuel sources. However, single junction silicon solar cells can only efficiently absorb ~30% of available sunlight. A portion of sunlight is too low in energy to be absorbed by the solar cell while another portion of sunlight is too high in energy to be absorbed without losses due to thermalization. Singlet fission, a process that converts a high energy singlet exciton into two lower energy triplet excitons, can be used to convert high energy light into lower energy light that can be absorbed efficiently by silicon. Singlet fission materials that undergo fast singlet fission, have long lived triplets, and have long triplet diffusion lengths show the greatest potential to increase the efficiency of solar cells. This thesis describes the design and singlet fission behavior of norbornene based polymers with pendent acene chromophores. The first chapter highlights other supramolecular singlet fission materials that have been studied to date that served as inspiration for this work. The second chapter demonstrates the efficient singlet fission and the slow, molecular weight dependent triplet recombination that occurs in pendent pentacene polymers. The third chapter outlines how the tunability of the polymer can be used to control singlet fission dynamics. In the fourth chapter, the singlet fission dynamics are shown to be largely unaffected by solvent composition and by casting into thin films. The fifth and final chapter explores exciton migration in pendent tetracene and pentacene block copolymers. This thesis illustrates a new, high tunable platform for studying inter-chromophore singlet fission, which shows promise for use in solar cells.

Filter-free spectral tunable photodetectors (PDs) are critical for a plethora of applications in imaging, indoor light fidelity (Li-Fi), and light communications. The present band-selective light detection is realized by incorporating different optical filters with broadband inorganic semiconductor-based PDs. However, the use of the optical filters reduces the overall performance of these PDs and is not appliable in the emerging flexible and wearable applications. The rapid advancement of the organic semiconductors offers an exciting opportunity for the development of high-performance filter-free spectral tunable organic photodetectors (OPDs). The development of OPDs has attracted tremendous interests because of the tailored optoelectronic properties of the π-conjugated organic semiconductors and the solution fabrication process of the OPDs. Apart from the rapid progresses made in improving the responsivity and detectivity of OPDs, the spectral properties of OPDs also receive intense attention. This Ph.D. research work has been focused on developing a universal strategy to achieve high-performance filter-free band-selective and spectral tunable OPDs. The correlation between the optical profile and responsivity spectrum of the novel OPDs with a bilayer photoactive layer has been investigated. It suggests that the responsivity spectrum of the OPDs can be effectively modulated by managing the optical profile in the bilayer and multilayer photoactive layer. A filter-free band-selective OPD model, comprising a bilayer shorter-wavelength light depletion layer/longer-wavelength light-absorbing layer architecture photoactive layer, has been developed. The depletion layer in the filter-free OPDs has a dual-function serving as a shorter-wavelength light-absorbing layer and a hole-transporting layer. The photodetection spectrum window of the filter-free band-selective OPDs, defined by the difference in wavelengths between the transmission cutoff of the shorter-wavelength light depletion layer and the absorption edge of the longer-wavelength light-absorbing layer, can then be tuned over the different wavelength ranges by using an appropriate combination of the shorter-wavelength light depletion layer and the longer-wavelength light-absorbing layer. A dual-mode OPD, having a trilayer visible light absorber/optical spacer/near-infrared (NIR) light absorber configuration photoactive layer, has been proposed. The dual-mode OPD exhibits electrically switchable NIR response operated under a reverse bias and visible light response operated under a forward bias. In the presence of NIR light, the trap-assisted charge-injection behavior at the organic/cathode interface in the OPDs operated under a reverse bias. The photocurrent is produced in the visible light-absorbing layer, enabled by the trap-assisted charge injection at the anode/organic interface under a forward bias. The developed filter-free band-selective OPDs and electrically switchable dual-mode OPDs provided an attractive alternative optical detection technology to the conventional panchromatic and single-mode OPDs. The spectral tunable photodetection thus demonstrated offers a promising option for new OPD applications.

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